Prehistoric Mining and Metallurgy in South West Iberian Peninsula 9781841715544, 9781407325958

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l na tio ne di nli ad l o ith ria W ate m

Mark A. Hunt Ortiz

BAR  S1188  2003   HUNT ORTIZ   PREHISTORIC MINING AND METALLURGY IN SOUTH WEST IBERIAN

2003 B A R

Prehistoric Mining and Metallurgy in South West Iberian Peninsula

BAR International Series 1188

Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Mark A. Hunt Ortiz

BAR International Series 1188 2003

ISBN 9781841715544 paperback ISBN 9781407325958 e-format DOI https://doi.org/10.30861/9781841715544 A catalogue record for this book is available from the British Library

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PUBLISHING

To Coral and Coral-Ivy, to John and María Teresa

CONTENTS List of Maps........................................................................................................................................................................vi List of Figures.....................................................................................................................................................................vi List of Photographs............................................................................................................................................................ix List of Lead Isotope Plots..................................................................................................................................................ix ACKNOWLEDGEMENTS...............................................................................................................................................xi CHAPTER I. INTRODUCTION ..............................................................................................................................1 CHAPTER II. METHODOLOGY............................................................................................................................8 II.1. MINING-METALLURGICAL SURVEYS ....................................................................................................8 II.1.1. Documentation ..................................................................................................................................................8 II.1.1.1. Geological and Metallogenetic Maps ...........................................................................................................8 II.1.1.2. Topographical Plans: Symbols and Toponymy ............................................................................................9 II.1.1.3. Written Sources ............................................................................................................................................10 II.1.1.4. Unwritten Sources .........................................................................................................................................10 II.1.2. Location of Mines...............................................................................................................................................10 II.1.3. Study of the Mining Works ................................................................................................................................12 II.2. ANALYTICAL METHODS...................................................................................................................................12 II.2.1. Methods for Determining Elemental Composition ............................................................................................14 II.2.1.1. Atomic Absorption (AA)..............................................................................................................................14 II.2.1.2. X-Ray Fluorescence (XRF)...........................................................................................................................14 II.2.1.3. Electron Microprobe Analysis (EMA)..........................................................................................................15 II.2.1.4. Scanning Electron Microscope (SEM)..........................................................................................................15 II.2.1.5. Proton Induced X-Ray Emission (PIXE) ......................................................................................................15 II.2.2. Methods for Determining Phases and Microstructures......................................................................................16 II.2.2.1. X-Ray Diffraction (XRD)..............................................................................................................................16 II.2.2.2. Metallography................................................................................................................................................16 II.2.2.2.1. Sample preparation...................................................................................................................................17 II.2.2.2.2. The Internal Structure and the Fabrication Processes..............................................................................17 II.2.3. Lead Isotopes......................................................................................................................................................18 II.2.3.1. Theoretical Principles....................................................................................................................................19 II.2.3.2. Lead Isotopes and Geology ...........................................................................................................................20 II.2.3.3. Lead Isotopes and Archaeology ....................................................................................................................21 II.2.3.3.1. Theoretical Bases......................................................................................................................................21 II.2.3.3.2. Elemental Analyses and Archaeological Non-metallurgical Application of Lead Isotope Analysis ......23 II.2.3.3.3. Lead Isotopes Analysis Applied to Archaeometallurgy...........................................................................24 II.2.3.3.3.1. Extractive Metallurgy..........................................................................................................................24 II.2.3.3.3.2. Alloys...................................................................................................................................................25 II.2.3.3.3.3. Recycling .............................................................................................................................................26 II.2.3.4. Analytical Procedure ...................................................................................................................................26 II.2.3.5. Presentation of the Lead Isotope data .........................................................................................................26 CHAPTER III. GEOLOGICAL BACKGROUND AND MINERAL RESOURCES...............................................27 III.1. GEOLOGICAL BACKGROUND .................................................................................................................27 III.1.1. Hesperian Massif...............................................................................................................................................27 III.1.1.1. Ossa-Morena Zone .......................................................................................................................................27 III.1.1.2. South Portuguese Zone ................................................................................................................................30 III.1.2. Eastern Area ......................................................................................................................................................31 III.1.2.1. Tertiary Basin of the Guadalquivir ..............................................................................................................31 III.1.2.2. Sub-Betic Zone of the Alpine Domain ........................................................................................................31 III.2. MINERAL RESOURCES .....................................................................................................................................31 III.2.1. Hesperian Massif...............................................................................................................................................32 III.2.1.1. Ossa-Morena Zone .......................................................................................................................................32 III.2.1.1.1. Sierra Albarrana Domain ........................................................................................................................32

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III.2.1.1.2. Zafra-Alanís Domain...............................................................................................................................33 III.2.1.1.3. Olivenza-Monesterio Domain.................................................................................................................33 III.2.1.1.4. Elvas-Cumbres Mayores Domain ...........................................................................................................34 III.2.1.1.5. Barrancos-Hinojales Syncline................................................................................................................34 III.2.1.1.6. Evora-Beja-Aracena Domain..................................................................................................................34 III.2.1.2. South Portuguese Zone ................................................................................................................................35 III.2.1.2.1. Pulo de Lobo Formation .........................................................................................................................35 III.2.1.2.2. Pyritic Belt...............................................................................................................................................35 III.2.1.2.2.1. Volcanic-Sedimentary Complex ........................................................................................................35 III.2.1.2.2.1.1. Rio Tinto Mineral Deposit............................................................................................................35 III.2.1.2.2.2. Phyllitic-Quartzitic Formation ...........................................................................................................40 III.2.1.2.3. Bajo Alentejo Flych Group.....................................................................................................................40 III.2.1.2.3.1. Mértola Formation .............................................................................................................................40 III.2.1.2.3.2. Mira Formation ..................................................................................................................................40 III.2.1.2.3.3. Bejeira Formation ..............................................................................................................................41 III.2.2. Eastern Area ......................................................................................................................................................41 III.2.2.1. Guadalquivir Depression..............................................................................................................................41 III.2.2.2. Alpine Domain ..............................................................................................................................................41 III.2.3. Synopsis of Silver Mineral Resources in the South West Iberian Pensinsula...................................................41 CHAPTER IV. ARCHAEOLOGICAL REGISTER AND ANALYSIS: BASES FOR THE ARCHAEO-METALLURGICAL INVESTIGATION ....................................................................................................44 IV.1. MINING ACTIVITY ............................................................................................................................................44 IV.1.1. Surveyed Areas .................................................................................................................................................44 IV.1.1.1. Sierra de Aracena-Northern Sierra de Sevilla .............................................................................................45 IV.1.1.2. Aznalcóllar-Rio Corumbel-Madroño-El Castillo de las Guardas ...............................................................67 IV.1.1.3. Other Surveyed Mines in the South Portuguese Zone.................................................................................108 IV.1.1.4. Sub-Betic Area.............................................................................................................................................111 IV.1.2. Catalogue of the Mineral Deposits with Evidence of Prehistoric Exploitation in the South West Iberian Peninsula ..........................................................................................................................111 IV.2. METALLURGICAL ACTIVITY ..........................................................................................................................143 IV.2.1. Chalcolithic .......................................................................................................................................................143 IV.2.2. Middle Bronze Age...........................................................................................................................................173 IV.2.3. Pre-Orientalizing Late Bronze Age ..................................................................................................................194 IV.2.4. Orientalizing Period ..........................................................................................................................................194 CHAPTER V. ISOTOPIC CHARACTERISATION OF THE SOUTH WEST IBERIAN PENINSULA......................................................................................................................................................................218 V.1. ISOTOPIC CHARACTERISATION OF THE OREBODIES OF THE SOUTH WEST IBERIAN PENINSULA ..............................................................................................................218 V.1.1. Levels of Internal and Regional Comparison: Mineral Deposits of the South West Iberian Peninsula ...........218 V.1.2. Level of General Comparison: Mineral Deposits of the South-Central and the South-East of the Iberian Peninsula and of the Mediterranean ...........................................................................................................221 V.2. ISOTOPIC STUDY OF THE ARCHAEOMETALLURGICAL SAMPLES FROM THE SOUTH WEST OF THE IBERIAN PENINSULA....................................................................239 V.2.1. Chalcolithic ................................................................................................................................................239 V.2.2. Middle Bronze Age ....................................................................................................................................242 V.2.3. Pre-Orientalizing Late Bronze Age ............................................................................................................249 V.2.4. Orientalizing Period ...........................................................................................................................................250 CHAPTER VI. MINING AND METALLURGICAL TECHNOLOGY VI.1. MINING TECHNOLOGY....................................................................................................................................259 VI.1.1. Formation of the Mineral Deposits...................................................................................................................259 VI.1.2. The Non-metallurgical Use of Minerals ...........................................................................................................260 VI.1.3. The Technological Basis: Antecedents of Metallic Mining .............................................................................262 VI.1.4. Non-metallic Mining in the Iberian Peninsula..................................................................................................264 VI.1.5. Metallic Mining in Europe and the Near East ..................................................................................................266 VI.1.6. Metallic Mining in the Iberian Peninsula..........................................................................................................272 VI.1.7. Metallic Mining in the South West of the Iberian Peninsula............................................................................274 VI.1.7.1. Prehistoric Ore Deposits Surveying.............................................................................................................274 iii

VI.1.7.2. Mineral Species Exploited ...........................................................................................................................276 VI.1.7.3. Mining Tools................................................................................................................................................281 VI.1.7.3.1. Stone Hammers.......................................................................................................................................281 VI.1.7.3.1.1. Typology of the Stone Mining Hammers in the South West Iberian Peninsula ...............................284 VI.1.7.3.2. Stone Axes ..............................................................................................................................................286 VI.1.7.3.3. Metallic Mining Tools ............................................................................................................................286 VI.1.7.3.4. Other Mining Tools ................................................................................................................................287 VI.1.7.4. Typology of Mine Workings .......................................................................................................................287 VI.1.7.5. Mining Accidents.........................................................................................................................................291 VI.2. METALLURGICAL TECHNOLOGY..................................................................................................................291 VI.2.1. Chalcolithic .......................................................................................................................................................292 VI.2.1.1. Ore Concentration.................................................................................................................................292 VI.2.1.1.1. Mortars: Chronology and Typology ......................................................................................................292 VI.2.1.1.2. Ore Concentration in the Chalcolithic ...................................................................................................293 VI.2.1.2. Transformation and Production Activities..................................................................................................294 VI.2.1.2.1. Furnaces, Vase-oven and Crucibles .......................................................................................................294 VI.2.1.2.2. Tuyeres...................................................................................................................................................302 VI.2.1.2.3. Slags .......................................................................................................................................................304 VI.2.1.2.4. Moulds ...................................................................................................................................................306 VI.2.1.3. Metal objects...............................................................................................................................................307 VI.2.1.3.1. Copper-Base Objects ......................................................................................................................307 VI.2.1.3.1.1. Arrowheads ................................................................................................................................308 VI.2.1.3.1.2. Javelins..............................................................................................................................................311 VI.2.1.3.1.3. Axes...................................................................................................................................................313 VI.2.1.3.1.4. Daggers and Knives ..........................................................................................................................315 VI.2.1.3.1.5. Awls, Spatulas and Chisels ...............................................................................................................318 VI.2.1.3.1.6. Saws and Sickles...............................................................................................................................320 VI.2.1.3.1.7. Halberds ............................................................................................................................................320 VI.2.1.3.1.8. Various..............................................................................................................................................321 VI.2.1.3.2. Native Copper .........................................................................................................................................321 VI. 2.1.3.3. Arsenical Copper ...................................................................................................................................323 VI.2.1.3.4. Iron in Copper Artefacts .........................................................................................................................324 VI.2.1.3.5. Gold Objects ............................................................................................................................................324 VI.2.1.3.6. Iron in the Chalcolithic?..........................................................................................................................327 VI.2.2. Middle Bronze Age...........................................................................................................................................329 VI.2.2.1. Ore Concentration................................................................................................................................329 VI.2.2.2. Transformation and Production Activities ...........................................................................................329 VI.2.2.2.1. Furnaces, Vase-oven and Crucibles.................................................................................................329 VI.2.2.2.2. Tuyeres....................................................................................................................................................332 VI.2.2.2.3. Slags ........................................................................................................................................................332 VI.2.2.2.4. Moulds ....................................................................................................................................................333 VI.2.2.3. Metal objects................................................................................................................................................333 VI.2.2.3.1. Copper-Base Metal objects .............................................................................................................333 VI.2.2.3.1.1. Arrowheads ................................................................................................................................333 VI.2.2.3.1.2. Axes ..........................................................................................................................................334 VI.2.2.3.1.3. Daggers, Knives and Rapiers/Swords .......................................................................................336 VI.2.2.3.1.4. Awls and Chisels........................................................................................................................339 VI.2.2.3.1.5. Saws ..........................................................................................................................................341 VI.2.2.3.1.6. Halberds....................................................................................................................................341 VI.2.2.3.1.7. Various......................................................................................................................................342 VI.2.2.3.2. Gold Objects ..................................................................................................................................343 VI.2.2.3.3. Iron in the Middle Bronze Age? ....................................................................................................344 VI.2.2.3.4. Silver in the Middle Bronze Age ...................................................................................................345 VI.2.2.3.4.1. Silver Metallurgy: General Considerations ...............................................................................345 VI.2.2.3.4.2. Distinction between Cupelled and Non-Cupelled Silver...........................................................346 VI.2.2.3.4.3. Middle Bronze Age Silver Metallurgy in South West Iberian Peninsula.................................346 VI.2.2.3.4.4. Silver Objects............................................................................................................................347 VI.2.3. Pre-Orientalizing Late Bronze Age...........................................................................................................349 VI.2.3.1. Ore Concentration........................................................................................................................................349 VI.2.3.2. Transformation and Production Activities...................................................................................................350 VI.2.3.2.1. Furnaces, Vase-ovens and Crucibles ......................................................................................................351

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VI.2.3.2.2. Tuyeres....................................................................................................................................................352 VI.2.3.2.3. Slags ........................................................................................................................................................352 VI.2.3.3. Metal objects................................................................................................................................................353 VI.2.3.3.1. Copper-Base Objects ..............................................................................................................................353 VI.2.3.3.2. Gold Objects ...........................................................................................................................................356 VI.2.3.3.3. Iron objects .............................................................................................................................................356 VI.2.4. Orientalizing Period ..................................................................................................................................356 VI.2.4.1. Copper Metallurgy ...............................................................................................................................356 VI.2.4.1.1. Transformation and Production Activities .....................................................................................356 VI.2.4.1.2. Copper-Base Objects ......................................................................................................................357 VI.2.4.2. Silver Metallurgy .................................................................................................................................358 VI.2.4.2.1. Ore Concentration ...........................................................................................................................358 VI.2.4.2.2. Transformation and Production Activities .....................................................................................359 VI.2.4.2.2.1. Furnaces .....................................................................................................................................359 VI.2.4.2.2.2. Tuyeres.......................................................................................................................................360 VI.2.4.2.2.3. Silver Slags ...............................................................................................................................362 VI.2.4.2.2.3.1. Tapped Slags.........................................................................................................................362 VI.2.4.2.2.3.2. “ Free Silica” Slags ...............................................................................................................362 VI.2.4.2.2.4. Slagged Pottery ..........................................................................................................................366 VI.2.4.2.2.5. Colanders ..................................................................................................................................366 VI.2.4.2.2.6. Cupels .......................................................................................................................................368 VI.2.4.2.2.7. Litharge .....................................................................................................................................369 VI.2.4.2.2.8. Lead Drops........................................................................................................................................369 VI.2.4.2.2.9. Lime ..........................................................................................................................................369 VI.2.4.2.3. Silver Objects..................................................................................................................................370 VI.2.4.3. Gold Objects ......................................................................................................................................370 VI.2.4.4. Iron in the Orientalizing Period ..........................................................................................................370 CHAPTER VII. EVALUATION AND DYNAMICS OF MINING AND METALLURGY DURING THE RECENT PREHISTORY IN THE SOUTH WEST IBERIAN PENINSULA ......................................372 VII.1. VII.2. VII.3. VII.4. VII.5. VII.6. VII.7.

MINERAL RESOURCES ...................................................................................................................................372 ISOTOPIC CHARACTERISATION OF ORE DEPOSITS...............................................................................373 NEOLITHIC-CHALCOLITHIC TRANSITION ................................................................................................374 CHALCOLITHIC MINING AND METALLURGICAL TECHNOLOGY .....................................................376 MIDDLE BRONZE AGE MINING AND METALLURGICAL TECHNOLOGY .........................................383 PRE-ORIENTALIZING LATE BRONZE AGE MINING AND METALLURGICAL TECHNOLOGY......387 ORIENTALIZING PERIOD MINING AND METALLURGICAL TECHNOLOGY ....................................391

CHAPTER VIII. BIBLIOGRAPHY .................................................................................................................................396

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List of Maps Map 1. Main mineral deposits in South West Iberian Peninsula. .............................................................................32 Map 2. Location of North of Chorrito group of mines. ............................................................................................80 Map 3. Mines with evidence of prehistoric exploitation in South West Iberian Peninsula. ............................................112 Map 4. South West Iberian Peninsula Chalcolithic sites with evidence of metallurgical activity...................................294 Map 5. South West Iberian Peninsula Middle Bronze Age sites with evidence of metallurgical activity. ...............330 Map 6. South West Iberian Peninsula Pre-Orientalizing and Orientalizing sites with evidence of metallurgical. .........350

List of Figures Figure 1. Iberian Peninsula Geological Units (after Vázquez Guzmán, 1983)..........................................................28 Figure 2. SW Iberian Peninsula Geological Domains (after Libro Blanco de la Minería, 1986). .............................28 Figure 3. Ossa-Morena Geological Zone (after Locuruta et al., 1990)......................................................................29 Figure 4. South Portuguese Geological Zone (after Oliveira & Oliveira, 1996). . ....................................................30 Figure 5. Geological plan of Rio Tinto (after Baumann, 1976). ...............................................................................36 Figure 6. Geological section of Filón Sur-Cerro Colorado-Filón Norte lodes, Río Tinto (after García Palomero, 1990). .......................................................................................................................................36 Figure 7. Zoning of sulphide deposits (after Fernández & Requena, 1992). ............................................................37 Figure 8. Cala ancient mine workings (after Domergue, 1987).................................................................................47 Figure 9. Stone tool from Cala mine (after Domergue, 1987). ........................................................................................47 Figure 10. Location of La Sultana-San Rafael group (after Palacios & Prieto, 1921-modified-). ............................48 Figure 11. Stone hammers from La Sultana. .............................................................................................................50 Figure 12. San Rafael mine workings. ......................................................................................................................51 Figure 13. Stone mortar from San Rafael mine. .......................................................................................................51 Figure 14. Stone tool from Teuler mine (after Domergue, 1987)..............................................................................52 Figure 15. Draft of Los Paredones mine workings. ...................................................................................................53 Figure 16. Stone hammers from Los Paredones mine. ..............................................................................................54 Figure 17. Sketch of Pozo Rico (after IGME, 1987-modified-). ..............................................................................55 Figure 18. Plan and sections of Potosí mine workings. ...........................................................................................57 Figure 19. Stone hammers from Potosí mine. ...........................................................................................................58 Figure 20. Plan of La Redondilla mining works (after IGME, 1980-modified-).......................................................59 Figure 21. Sections of works M and J from La Redondilla mine. .............................................................................60 Figure 22. Stone hammers from La Redondilla mine. ..............................................................................................61 Figure 23. Stone hammers from Juan Teniente mine. ...............................................................................................63 Figure 24. Plan of works of San Enrique mine (after Pinedo, 1963). .......................................................................63 Figure 25. Stone mining tools from San Enrique mine..............................................................................................65 Figure 26. Finds from the interior of Peñaflor mine (after Cañal, 1894)...................................................................66 Figure 27. Grooved stone hammer from Peñaflor mine. ...........................................................................................67 Figure 28. La Ratera mineralized area (after Pinedo, 1963). ....................................................................................68 Figure 29. Mansegoso (Site 27) mining works (after Blanco & Rothenberg, 1981). ...............................................69 Figure 30. Mansegoso (Site 28) mining works (after Blanco & Rothenberg, 1981). ...............................................69 Figure 31. Chinflón mines. General plan (after Rothenberg & Andrews, 1996). .....................................................70 Figure 32. Chinflón Mine-3. Plan and section (after Rothenberg & Andrews, 1996). ..............................................72 Figure 33. Chinflón mining camp. Plan and archaeological section (after Rothenberg & Andrews, 1996). ............75 Figure 34. Plan of Las Navas mine (after García González, 1988-modified-). .........................................................77 Figure 35. Grooved stone hammer from Las Navas mine. ........................................................................................78 Figure 36. Plan of Cueva del Monge mines (after Blanco & Rothenberg, 1981)......................................................79 Figure 37. North of Chorrito: Mine-1. Plan and section............................................................................................81 Figure 38. Stone tools from North of Chorrito Mine-1. ............................................................................................81 Figure 39. North of Chorrito: Mine-2. Plan. .............................................................................................................82 Figure 40. Stone tools from North of Chorrito Mine-2. ............................................................................................82 Figure 41. North of Chorrito: Mine-3. Plan. .............................................................................................................83 Figure 42. Stone tools from North of Chorrito Mine-3. ............................................................................................83 Figure 43. North of Chorrito: Mine-4. Plan. .............................................................................................................84 Figure 44. Stone tools from North of Chorrito Mine-4. ............................................................................................84 Figure 45. Stone tools from North of Chorrito Mine-6. ............................................................................................85 Figure 46. Stone tools from North of Chorrito Mine-7, Zone A. ..............................................................................85 Figure 47. North of Chorrito: Mine-8. Plan and section. ..........................................................................................86 Figure 48. Stone tools from North of Chorrito Mine-8. ............................................................................................87 vi

Figure 49. North of Chorrito: Mine-9. Plan. .............................................................................................................87 Figure 50. Stone tools from North of Chorrito Mine-9. ............................................................................................88 Figure 51. XRD of crucible fragment from North of Chorrito Mine-9. ....................................................................89 Figure 52. North of Chorrito: Mine-9B. Plan. ..........................................................................................................89 Figure 53. Stone tools from North of Chorrito Mine-9B. .........................................................................................90 Figure 54. Stone tools from North of Chorrito Mine-10. ..........................................................................................90 Figure 55. North of Chorrito: Mine-11. Plan. ...........................................................................................................91 Figure 56. Stone tools from North of Chorrito Mine-11. ..........................................................................................91 Figure 57. Stone tools from North of Chorrito Mine-11B. .......................................................................................91 Figure 58. North of Chorrito: Mine-12. Plan. ...........................................................................................................92 Figure 59. Stone tools from North of Chorrito Mine-12. ..........................................................................................92 Figure 60. North of Chorrito: Mine-13. Plan. ...........................................................................................................92 Figure 61. Stone tools from North of Chorrito Mine-13. ..........................................................................................93 Figure 62. North of Chorrito: Mine-14. Plan. ..........................................................................................................93 Figure 63. Stone tools from North of Chorrito Mine-14. ..........................................................................................93 Figure 64. North of Chorrito: Mine-15. Plan. ..........................................................................................................94 Figure 65. Stone tools from North of Chorrito Mine-15. ..........................................................................................94 Figure 66. North of Chorrito: Mine-16. Plan and section..........................................................................................95 Figure 67. Stone tools from North of Chorrito Mine-16. ..........................................................................................96 Figure 68. Trinidad mining works. Plan and sections. ..............................................................................................97 Figure 69. Hondurillas mine. General plan. ..............................................................................................................98 Figure 70. Grooved stone hammers from Hondurillas mine......................................................................................99 Figure 71. El Tintillo South mine. Plan and sections. ...............................................................................................101 Figure 72. Stone tools from El Tintillo South mine. .................................................................................................101 Figure 73. Coral Group of mines. Plan and sections. ................................................................................................102 Figure 74. Stone tools from Coral Group of mines. ..................................................................................................103 Figure 75. Grooved stone hammer from La Zarcita mine. ........................................................................................104 Figure 76. Aznalcóllar opencast. Ancient Mining Zone: Plan and Sections. ............................................................106 Figure 77. Tharsis mineralized area. Plan of orebodies (after Strauss & Gray, 1986-modified-). ...........................108 Figure 78. Cabezo Hueca mine. Plan of mining works (after Pinedo, 1963-modified-)............................................109 Figure 79. Grooved stone hammer from Cabezo Hueca mine...................................................................................109 Figure 80. Sierrecilla mine. Plan of mining works (after Pinedo, 1963-modified-). ................................................110 Figure 81. Grooved stone hammer from Sierrecilla mine. ........................................................................................111 Figure 82. Grooved stone hammer from Monte Romero mine..................................................................................113 Figure 83. Grooved stone hammer from San Miguel mine. ......................................................................................114 Figure 84. Grooved stone hammer from Sotiel Coronada mine. ...............................................................................118 Figure 85. Stone tools from Cuchillares mine (after Blanco & Rothenberg, 1981). .................................................119 Figure 86. Grooved stone hammer from La Joya mine. ............................................................................................120 Figure 87. Grooved stone hammer from Confesionarios mine. ................................................................................121 Figure 88. Los Guijarros mine. Plan and section (after Pinedo, 1963)......................................................................122 Figure 89. Lomo de Perro area. Plan of mineralizations (after Domergue, 1987).....................................................130 Figure 90. Grooved stone hammer from Los Jarales mine. ......................................................................................132 Figure 91. El Piconcillo area. Plan of mineralizations (after Domergue, 1987). ......................................................134 Figure 92. Almadenes de Bembézar mining works. Plan and sections (after Domergue, 1987). ..............................135 Figure 93. Cerro Muriano mining works. Plan and sections of A) Mine 1-B and B) Mine 2. ..................................138 Figure 94. Stone tools from Cerro Muriano mine. ....................................................................................................139 Figure 95. Metal objects from Chalcolithic sites in the Huelva province: A. Awl from El Tejar (Gibraleón) (after Belén & Del Amo, 1985). B. Axe from La Zarcita grave (San Bartolomé). C. Fragment from El Pozuelo Dolmen-4 (Zalamea la Real) (after Cerdán et al., 1975). D. Fragment from Los Gabrieles Dolmen-4 (Valverde) (after Cabrero, 1978). E. Dagger and F. Axe from El Castañuelo (Aracena). G. Palmela arrowhead from Gil Marquez (Almonaster) (after Perez & Ruiz, 1986)................................144 Figure 96. Metal objects from Valencina: Roquetito (RQ1, RQ2 RQ3) and El Algarrobillo (RQ4, RQ5). .............147 Figure 97. Metal objects from Amarguillo-II. ...........................................................................................................155 Figure 98. Palmela arrowheads from the province of Sevilla. ..................................................................................161 Figure 99. Metal objects from La Pijotilla. ..............................................................................................................165 Figure 100. Dagger (T-3) and halberd (CD13) from La Pijotilla. ............................................................................166 Figure 101. Metal objects from La Pijotilla. .............................................................................................................167 Figure 102. El Trastejón. General plan (after Hurtado, 1990-modified-). ................................................................172 Figure 103. Grooved stone hammer from El Trastejón. ...........................................................................................173 Figure 104. Stratigraphic sequence of El Trastejón Square F-22 (after Hurtado & García, 1994). .........................173 Figure 105. Metallurgical elements from El Trastejón. ............................................................................................176 Figure 106. Silver objects from Middle Bronze Age sites: 1. El Becerrero (Almonaster). 2. Calañas. vii

3. Dolmen del Carnerín (Alcalá del Valle). 4. Valdearenas (Iznajar). ...................................................182 Figure 107. Middle Bronze Age halberds: A. Écija. B. Montejícar. C. El Argar. D. Campina. E. Monte do Castelo. F. La Traviesa (Almadén de la Plata). ...........................................................................................................186 Figure 108. Sample TH-3. PIXE: external elemental distribution.............................................................................190 Figure 109. Sample TH-3. PIXE: complete section elemental distribution...............................................................191 Figure 110. Sample TH-3. PIXE: surface section elemental distribution..................................................................192 Figure 111. Casetillas site: Furnace remains. ............................................................................................................196 Figure 112. Stone mortars from Castrejones site.......................................................................................................203 Figure 113. Stone mortar from Castrejones site. .......................................................................................................204 Figure 114. Stone pounders from Castrejones site. ...................................................................................................205 Figure 115. Stone hammers from Castrejones site. ...................................................................................................206 Figure 116. Metal objects from Castrejones site. ......................................................................................................207 Figure 117. Castrejones site. Mineral sample AZ-20: XRD result. ..........................................................................217 Figure 118. Castillo de Doña Blanca site. Sample TDB-18: XRD result..................................................................217 Figure 119. A. Limonite Palaeolithic mine of Lovas (Hungary). B. Flint mine of Obourg and C. of Spiennes (Belgium) (after Shepherd, 1980). D. Flint mine of Grimes’ Grave (England) (after Forbes, 1966). ...263 Figure 120. Can Tintorer (Gavá) Mine-7: Plan and sections (after Villalba et al., 1986). ........................................265 Figure 121. Stone and bone mining tools from Can Tintorer (Gavá) (after Villalba et al., 1986).............................266 Figure 122. Prehistoric mining systems and stone tools from Fenan (after Weisgerber & Hauptmann, 1988). .......269 Figure 123. Prehistoric mining tools from Cantabrian mines: 1. El Milagro. 2. Aramo. 3. La Profunda (after De Blas, 1989)..............................................................................................................................273 Figure 124. Typology of stone mining hammers from South West Iberian Peninsula. .............................................285 Figure 125. Hafting of stone mining hammers (after Craddock, 1990).....................................................................286 Figure 126. Possible Chalcolithic crucibles from: 1. Castelo Velho de Safara. 2. Porto Mourao. 3. & 4. Tres Moinhos. 5. Sao Bras-1 (after Monge Soares et al., 1994). 6. Valencina. 7. Universidad Laboral (after Fernández & Sierra, 1985). 8. & 9. La Pijotilla. 10. El Acebuchal (after Harrison et al., 1976). ..........297 Figure 127. Slagged pottery ( 1 & 2) and crucibles from Joao Marques (after Gonçalves, 1989). ..........................298 Figure 128. Hypothetical reconstruction of Structure-I.25 from Santa Justa (after Gonçalves, 1989). .....................299 Figure 129. Crucibles and possible clay mould (1) from Santa Justa (after Gonçalves, 1989). ................................300 Figure 130. Nozzle from Pedra do Ouro (1) (after Gómez Ramos, 1966) and possible uses (after Tylecote, 1981).302 Figure 131. Fragments considered possible tuyeres from: 2. Tres Moinhos and 3. Sao Bras-I (after Monge Soares et al., 1994). ......................................................................................................................................303 Figure 132. Moulds from: 1. Joao Marques and 2. Santa Justa (after Gonçalves, 1989). .........................................307 Figure 133. Chalcolithic arrowheads from: 1. & 2. La Palma del Condado. 3. -9. Acebuchal. 10. Estepa. 11. & 12. Villaverde del Río. 13. Torre del Moro (Baena). 14. Alcantarilla (Priego). 15. Cerro Cebero (Priego). 16. Badajoz....................................................................................................................................309 Figure 134. Javelins from La Pastora (Valencina) (after Almagro, 1962) and (1) La Pijotilla (after Hurtado, 1984)....312 Figure 135. Chalcolithic axes from: 1. Huelva. 2. Moguer. 5. Acebuchal. 6. El Coronil. 7. Fuente Tójar. 8. Porto Mourao. 9. Tres Moinhos. 10. Santa Justa. ...................................................................................314 Figure 136. Chalcolithic daggers and knives from: 1. La Palma del Condado. 2. Sotiel Coronada. 3. Zufre. 4. Montilla. 5. Badajoz. 6. Vejer de la Frontera. 7. -9. Acebuchal. 10. Valencina. 11. Palacio Quemado. ....................316 Figure 137. Chalcolithic awls from: 1. & 2. Acebuchal. 3. Cerro Jesús (Baena). ...........................................................319 Figure 138. Halberd from Cerro de San Benito (Lebrija). ........................................................................................320 Figure 139. Middle Bronze Age (except Keos) metallurgical elements: 1. Crucible from Puerto Moral (after Pérez, 1996). 2. Crucible from Keos (after Tylecote, 1987). 3. Crucible fragment from La Barranquera Cist-6 (after Pérez, 1997). A. Moulds from Cerro de las Tres Aguilas (after Pérez, 1996). B. Clay mould from Las Minitas (after Pavón, 1995)....................................................................................................................331 Figure 140. Middle Bronze Age axes from: 1. Aracena. 2. Sierra de Baños. 3. Rio Tinto. 4. Manzanilla. 5. Cádiz. 6. Sevilla. 7. Priego. 8. Km. 125.3 (Priego). 9. Sierra Leones......................................................................335 Figure 141. Middle Bronze Age daggers/knives and rapiers/swords from: 1. & 2. Setefilla. 3. Fuente Tójar. 4. Itálica. 5. Sevilla. 6. Cueva Huerta Anguita. 7. Torrevuelo. 8. Torre Alta. 9. Priego. 10. Camino Tarajal. 11. Fuente Morellana. 12. El Canuto. 13. El Berrueco. .................................................................337 Figure 142. Middle Bronze Age A. Awls from 1. Las Minitas and 2. Alange; B. Saw from Niebla; C. Halberds from 1. Setefilla. and 2. Aguilar de la Frontera. ...........................................................................................340 Figure 143. Halberd from La Traviesa, Cist-5..................................................................................................................341 Figure 144. Metallurgical elements from Setefilla (after Aubet et al., 1983): Stratum XIIa: 1. Crucible. 2. Tuyere. Stratum VIII: 3. Tuyere. ................................................................................................................................351 Figure 145. Pre-Orientalizing Late Bronze Age objects from: 1. Huelva. 2. Río Guadalquivir (Sevilla). 3. Carabuey (Córdoba). 4. Mérida. ..................................................................................................................................354 Figure 146. Orientalizing Period tuyeres. Type A: A1. Monte Romero. A2. San Bartolomé de Almonte. Type B: B1. San Bartolomé de Almonte. B2. Monte Romero. Type C: C. Cerro Salomón. ...................................361 Figure 147. Orientalizing Period colanders: A. Related to silver metalurgy (after Fernández Jurado , 1988-1989). viii

B. From Setefilla (after Aubet et al., 1983). C. From Montilla (Cádiz) (after Schubart, 1987). ................367 Figure 148. Orientalizing Period cupels from Monte Romero (after Kassianidou, 1992 -1-; Pérez, 1991 -2 to 5-). 368

List of Photographs Photo 1. Metallography of chisel RQ-4 (Etched, x500). ...........................................................................................148 Photo 2. Metallography of sheet RQ-5 (x125). ........................................................................................................149 Photo 3. Metallography of sheet RQ-5 (Etched, x125).....................................................................................................149 Photo 4. Metallography of sheet RQ-5 (Etched, x500). ............................................................................................150 Photo 5. Metallography of slag RQ-6 (x500). ...........................................................................................................150 Photo 6. Metallography of axe RQ-1 (Etched, x1250). .............................................................................................152 Photo 7. Metallography of axe RQ-2 (Etched, x500). ...............................................................................................152 Photo 8. Metallography of blade RQ-3 (Etched, x500). ............................................................................................153 Photo 9. Metallography of awl AG-a (Etched, x125). ...............................................................................................158 Photo 10. Metallography of awl AG-a (Etched, x1250). ...........................................................................................158 Photo 11. Metallography of axe AG-b (Etched, x500)..............................................................................................159 Photo 12. Metallography of spatula AG-c (Etched, x125). .......................................................................................159 Photo 13. Metallography of spatula AG-d (Etched, x500). .......................................................................................160 Photo 14. Metallography of slag AG-5 (Etched, x500). ............................................................................................160 Photo 15. Metallography of arrowhead PS-1 (Etched, x125). ..................................................................................162 Photo 16. Metallography of arrowhead PS-2 (x125). ...............................................................................................163 Photo 17. Metallography of arrowhead PS-3 (x125). ...............................................................................................163 Photo 18. Metallography of axe CD-17 (Etched, x500). ...........................................................................................169 Photo 19. Metallography of saw CD-20 (Etched, x500)............................................................................................170 Photo 20. Metallography of saw CD-23 (Etched, x1250)..........................................................................................170 Photo 21. Metallography of arrowhead CD-24 (Etched, x500).................................................................................171 Photo 22. Metallography of fragment CD-29 (Etched, x500). ..................................................................................171 Photo 23. Metallography of awl TR-30 (Etched, x500). ...........................................................................................178 Photo 24. Metallography of handle TR-31 (Etched, x500). ......................................................................................178 Photo 25. Metallography of axe TR-33 (x125). ........................................................................................................179 Photo 26. Metallography of axe TR-33 (x500). ........................................................................................................179 Photo 27. Metallography of axe TR-33 (Etched, x500). ...........................................................................................180 Photo 28. Metallography of slag TR-26 (x500).........................................................................................................180 Photo 29. Metallography of La Traviesa halberd (Etched, x100)..............................................................................186 Photo 30. Metallography of La Traviesa halberd´s rivet (x50)..................................................................................187 Photo 31. Metallography of La Traviesa halberd´s rivet (Etched, x400). .................................................................187 Photo 32. Metallography of wire TH-3 (x500)..........................................................................................................193 Photo 33. Metallography of fragment TH-8 (Etched, x125)......................................................................................194 Photo 34. Section of a slag of the free silica type.....................................................................................................202 Photo 35. Metallography of sword AZ-10 (Etched, x400). ..............................................................................................209 Photo 36. Metallography of arrowhead AZ-14 (Etched, x400). ................................................................................210 Photo 37. Metallography of arrowhead AZ-15 (Etched, x200). ................................................................................210 Photo 38. Metallography of silver ingot fragment AZ-1 (Etched, x100)...................................................................211 Photo 39. Metallography of silver ingot fragment AZ-PAC (Etched, x200). ............................................................211 Photo 40. Metallography of silver earring AZ-2 (Etched, x200)...............................................................................212 Photo 41. Metallography of litharge TDB-12 (x400). ...............................................................................................215

List of Lead Isotope Plots Plot 1. Isotopic fields and samples of South Portuguese geological zone..................................................................219 Plot 2. Isotopic results of Ossa-Morena deposits of Cala,Teuler and La Sultana. .....................................................220 Plot 3. Isotopic results of South Portuguese deposits and Alanís & Posadas samples. ....................................................221 Plot 4. Isotopic results of SW mineral deposits & La Dehesa samples. ...........................................................................221 Plot 5. Isotopic results of South-Central Iberian Peninsula deposits. ........................................................................223 Plot 6. Isotopic results of SW mineral deposits & Linares samples...........................................................................223 Plot 7. Isotopic results of South-East Iberian Peninsula deposits. ............................................................................225 Plot 8. Isotopic results of S. Alhamilla, Linares, La Carolina & Berlanga (La Dehesa). ..........................................226

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Plot 9. Isotopic fields of South-East & Paterna & La Sultana. .................................................................................226 Plot 10. Isotopic fields of South-East & Teuler & Cala.............................................................................................227 Plot 11. Isotopic fields of Sardinian mineral deposits................................................................................................229 Plot 12. Isotopic results of Italian peninsular mineral deposits..................................................................................230 Plot 13. Isotopic results of Italian peninsular mineral deposits (without Montecatini). .............................................232 Plot 14. Isotopic fields of Sardinian and Italian peninsular mineral deposits. ...........................................................232 Plot 15. Isotopic fields of Italian mineral deposits (without Montecatini) & S. Almagrera.......................................233 Plot 16. Isotopic fields of part of Sardinian & Italian mineral deposits & La Carolina. ............................................233 Plot 17. Isotopic fields of Sardinian & Italian (grouped) mineral deposits & Cala. ..................................................234 Plot 18. Isotopic fields of Sardinian Rosas mineral deposit & SW (without Aznalcóllar).........................................234 Plot 19. Isotopic fields of Sardinian (without Sa Duchessa) mineral deposits & Aznalcóllar. ..................................235 Plot 20. Isotopic fields of Sardinian Sa Marchessa mineral deposit & SW (without Aznalcóllar). ...........................235 Plot 21. Isotopic fields of Crete & Cyprus mineral deposits & Cala & La Sultana. .................................................237 Plot 22. Isotopic fields of Laurion,Thera & Siphnos mineral deposits & Cala & La Sultana...................................238 Plot 23. Isotopic results of Valencina samples & Paterna, Aznalcóllar & Río Tinto mineral deposits......................239 Plot 24. Isotopic results of Valencina samples & La Sultana & Cala mineral deposits. ............................................240 Plot 25. Isotopic results of Amarguillo-II samples. ...................................................................................................240 Plot 26. Isotopic results of Amarguillo-II samples & Aznalcóllar, Río Tinto, La Sultana & Cala deposits. .............241 Plot 27. Isotopic results of Amarguillo-II samples & La Sultana & Crete mineral deposits......................................241 Plot 28. Isotopic results of La Pijotilla samples & Aznalcóllar, Río Tinto, Monte Romero, Paterna & La Sultana mineral deposits. ..........................................................................................................................................242 Plot 29. Isotopic results of La Pijotilla samples & La Sultana & Cala mineral deposits. ..........................................242 Plot 30. Isotopic results of El Trastejón samples & La Sultana, Cala & Teuler mineral deposits. ............................244 Plot 31. Isotopic results of El Trastejón samples (T31,T32,T33) & Paterna, Aznalcóllar, Monte Romero & La Sultana mineral deposits...............................................................................................................................244 Plot 32. Isotopic results of Hipogeum-I samples & La Sultana & Cala mineral deposits. .........................................245 Plot 33. Isotopic results of Hipogeum-I samples & Crete & Cyprus mineral deposits. .............................................245 Plot 34. Isotopic results of Hipogeum-I samples (L3,L5,L6) & Linares & La Carolina mineral deposits.................246 Plot 35. Isotopic results of Hipogeum-I samples & Aznalcóllar, Río Tinto, Monte Romero & Paterna mineral deposits. .......................................................................................................................................................246 Plot 36. Isotopic results of Hipogeum-I samples & Sardinian Rosas & Sa Marchessa mineral deposits...................247 Plot 37. Isotopic results of La Papúa samples & Paterna, Aznalcóllar, Linares & La Carolina mineral deposits......247 Plot 38. Isotopic results of La Papúa samples & Sardinian Sa Marchessa, Rosas & Pranu mineral deposits............248 Plot 39. Isotopic results of Peñalosa (Jaén) samples & Linares & La Carolina mineral deposits. .............................248 Plot 40. Isotopic results of Huelva Hoard/El Trastejón (T30,T31) samples & Mediterranean Sa Duchessa, Sa Marchessa & Cyprus mineral deposits. ...................................................................................................249 Plot 41. Isotopic results of Huelva Hoard samples (RH3,RH5) & Cala, La Sultana, Crete & Cyprus mineral deposits. .......................................................................................................................................................249 Plot 42. Isotopic results of Castillo de Doña Blanca samples & Aznalcóllar & Río Tinto mineral deposits. ............251 Plot 43. Isotopic results of Castillo de Doña Blanca samples & Linares, S. Alhamilla, Montecatini & Pranu mineral deposits. ..........................................................................................................................................251 Plot 44. Isotopic results of San Bartolomé de Almonte samples & Aznalcóllar, Río Tinto & Monte Romero mineral deposits. ..........................................................................................................................................252 Plot 45. Isotopic results of San Bartolomé de Almonte samples & Paterna, La Dehesa (Berlanga), Linares-La Carolina (Jaén) & Rosas mineral deposits. ...............................................................................252 Plot 46. Isotopic results of Peñalosa samples & Paterna, La Dehesa (Berlanga) & Linares-La Carolina (Jaén) mineral deposits. ..........................................................................................................................................253 Plot 47. Isotopic results of Tejada la Vieja samples & Paterna, La Dehesa (Berlanga) & Linares-La Carolina (Jaén) mineral deposits.................................................................................................................................253 Plot 48. Isotopic results of Torre del Viento samples & Linares-La Carolina (Jaén), Gador, S. Alhamilla & Pranu mineral deposits. ............................................................................................................................254 Plot 49. Isotopic results of Castillo samples & Aznalcóllar, Río Tinto & Paterna mineral deposits. ........................254 Plot 50. Isotopic results of Castrejones samples & Aznalcóllar, Paterna & Linares mineral deposits.......................255 Plot 51. Isotopic results of Castrejones samples & La Carolina, S. Alhamilla & Sardinian (without Sa Duchessa) mineral deposits. ..........................................................................................................................................255 Plot 52. Isotopic results of Cortijo José Fernández samples & Aznalcóllar, Paterna, Linares-La Carolina (Jaén) & Pranu mineral deposits. ................................................................................................................................256 Plot 53. Isotopic results of Cerro de las Tres Águilas samples & Río Tinto, Aznalcóllar & Paterna mineral deposits. .......................................................................................................................................................257 Plot 54. Isotopic results of Cerro de las Tres Águilas samples & Linares-La Carolina (Jaén) & S. Alhamilla mineral deposits. ..........................................................................................................................................257 Plot 55. Isotopic results of Huelva samples & Aznalcóllar, Río Tinto & Pranu mineral deposits. ............................258 x

ACKNOWLEDGEMENTS The research study “Prehistoric Mining and Metallurgy in South-West Iberian Peninsula”, presented herewith and that was my Doctorate Thesis presented at the Department of Prehistory and Archaeology, University of Sevilla -Spain- (awarded with maximum qualifications, the European Doctorate and the Doctoral Extraordinary Award), is the fruit of a lengthy period of investigation in greatly differing environments. This would not have been possible but for the participation of many sorts of individuals: from the personnel of laboratories specialising in nuclear analysis techniques to the anonymous shepherds of the Andalusian countryside. I was extremely fortunate in my introduction to the field of Archaeometallurgy by having magnificent teachers whose advice and encouragement were never lacking. Among these I would like to make special mention of Prof. Beno Rothenberg, director of the Institute of Archaeo-Metallurgical Studies (IAMS) of London University. Through his good offices I was given a grant which allowed me to initiate my specialisation at the Institute of Archaeology, University College, London University. Dr. Paul Craddock of the British Museum Research Laboratory directed my first investigation work in this field and since then I have always been able to count on his comments and suggestions. My thanks also to the late Professor R. Tylecote from whom I learnt the basic principles, which he set out so clearly in the seminars held at the Institute of Archaeology and in his house in Oxfordshire. Ascribed as a Research Visitor to the Isotrace Laboratory, which then formed part of the Department of Nuclear Physics, University of Oxford, for an academic year, I carried out there the analyses for lead isotopes of the selected samples from the South West area of the Iberian Peninsula. I must thank Prof. Nöel H. Gale and Dr. Zofia Stos-Gale as well as Dr. Brenda Rohl and all the other members of the Isotrace Laboratory for their interest and helpfulness in achieving my rapid integration in the Laboratory routine and the understanding of the complex processes involved in isotopic studies. My belonging to the Isotrace Laboratory also gave me easy access to the technical and archaeological bibliography in the different Oxford libraries, as well as the possibility of using the analytical facilities of other Departments of the University. For the help given me in the Research Laboratory for Archaeology and the History of Art (RLAHA) I must thank its director, Prof. M. Tite as well as Dr. Chris Salter and Mrs. Helen Hatcher. My thanks, too, for the collaboration of Dr. P. Northover of the Material Sciences Department, of Dr. Raik Jarjis of the Scanning Proton Microscope Unit of the Nuclear Physics Department and of Mr. C. Fagg of the Earth Sciences Department which was of inestimable value. The time spent at the Isotrace Laboratory of the University of Oxford, as well as the later work of study and investigation of the analytical results, was made possible by Research Grants awarded by the Dirección General de Bienes Culturales, Consejería de Cultura, Junta de Andalucía (Andalusian Government). To this same Dirección General my thanks for the funding which allowed the carrying out of some of the Archaeological Surveys, partly within the framework of the Research Project “Analysis and Definition of the Cultural Processes of the 2nd. Millennium B.C. in the S.-W. Iberian Peninsula”, directed by Prof. Victor Hurtado. The collection of the isotopic data was completed by a “Short Visit” to the Smithsonian Institution (Washington, D.C.) and to the NIST (Virginia). This visit was made possible through a grant from the Smithsonian Institution given at the suggestion of Mrs. Jacqueline S. Olin of the S.I. Analytical Laboratory and I offer my thanks for her interest, as well as permission to use unpublished isotopic data obtained for her own projects. Prof. Ingo Keesmann of Mainz University, Germany, was kind enough to give a grant to visit the “Arbeitsgruppe Archaometallurgie” of which he is the director and also to carry out the study requested on samples from El Trastejón site. My thanks, too, to Prof. Vagn F. Buchwald of the Technical University of Denmark and Dr. Salvador Rovira of the Museo Arqueológico Nacional, Madrid, and Dr. Pablo Gómez Ramos of the Universidad Autónoma, Madrid, who made studies of other samples from the same site. I extend my thanks to Dr. Rovira to include his help in obtaining some of the archaeological samples. Also, both he and Dr. Ignacio Montero, C.S.I.C., have always been ready to collaborate. They have carried out the analyses that I have requested and, moreover, they have allowed me to use analytical data, as yet unpublished, obtained from the “ Iberian Peninsula Archaeometallurgy Project” which they, together with Miss Susana Consuegra have been working on. My sincere thanks for the collaboration given by the Departamento de Física Atómica Nuclear y Molécular of Sevilla University, especially that of Prof. Miguel Angel Respaldiza, Prof. Blanca Gómez Tubío and D. Mario Fernández and also

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that given by the Departamento de Materiales, Escuela Técnica Superior de Ingenieros Industriales, Sevilla University and its director, Prof. Enrique Herrera García and also Mr. Jesús Pinto and, especially, Prof. José María Gallardo who allowed me the use of the Metallographic Laboratory, participated actively in the development of the experiments and was my guide in the study by SEM of the archaeometallurgical samples. I am also thankful for the help given by Prof. Angel Polvorinos del Río of the Departmento de Química Inorgánica, Sevilla University as well as that of the members of the Department of Material Sciences of the Consejo Superior de Investigaciones Científicas (C.S.I.C.), Sevilla, especially the director, Dr. José Luis Pérez Rodríguez, Dr. Angel Justo and the late D. Eduardo Gómez and that of Dr. José Manuel Murillo, biologist, also of the C.S.I.C. Dr. Craig Merideth, of the Institute of Archaeology, London University, was always most willing to collaborate in many aspects on which I requested his help, especially with the analyses of the SEM. Dr. Merideth also allowed me to use data from his thesis, not yet published, as did Dr. Vassiliki Kassianidou, Dr. B. Rohl, Dr. Leonardo García Sanjuan and Dr. Ignacio Pavón Soldevilla. I was also allowed the unrestricted use of their Degree Theses by Mr. Miguel A. Vargas Durán, Prof. Pedro Sáez Fernández and Dr. Blanca Gómez Tubío. Prof. B. Rothenberg gave me his last work, carried out in collaboration with Mr. P. Andrews, on the Chiflón Mines. My sincere thanks to Dr. F.J. Sarabia, and to Dr. Honorio Quintana for their collaboration regarding questions of bibliographical searching. It would have been impossible to carry out this investigation as planned without the collaboration of members of various mining companies, who gave me mineral samples and allowed access to their archives. In Rio Tinto Mines Dr. Felix García Palomero supplied the mineral samples necessary for the carrying out of the isotopic analyses. In Cala Mines I was able to count on the help of Dr. José Luis Cantos, mining engineer, Dr. Manuel García Sánchez, Chief Geologist, and Dr. Angel Canales, Head of Exploration, all belonging to the PRESUR company. In Aznalcollar Mines there existed a special relation with many of the members of the mining company Boliden-Aspirsa, S.L., who financed the survey work in the area. Particularly involved in the proper development of the archaeometallurgical research which was carried out there were: Mr. Christer Walsten, Dr. Juan Contreras, Mr. José Antonio Rufo, in charge of the Chemical Laboratory who carried out the analyses by the AA method, Mrs. Agneta Wengelin-Díaz, Mr. Enrique Guerrero, the geologists Mr. José Ramón López and Mr. José Manuel Pons, Mr. Pedro Sánchez Cazcarro, Head of Topography, Mr. Aquilino García, Mr. Antonio Ruiz Castell and Dr. Angel Maestre, as well as Mr. Pedro Cruz, who also had a thorough knowledge of María Luisa Mine where he held a directive post for many years. My grateful thanks to the members of the IGME in Sevilla for their kindness and collaboration when consulted on unpublished geological reports, especially Dr. José Luis Baeza-Rojano. Dr. Federico Sobol who has studied the mineralisations of the South-West over a considerable number of years was kind enough to revise the chapter on Geology, particularly complex in this geographical area. D. Manuel Gonzalez García, an expert mineralogist, provided me with both bibliography and indications from his profound knowledge of the mineralisations of the region. I owe a special debt of gratitude to the archaeologists who, either giving samples from their excavations or allowing these to be studied have made this archaeometallurgical research possible. Dr. Fernández Jurado, director of the Archaeological Department of the Huelva Diputación, gave samples from his excavations in Huelva city, Peñalosa, Tejada and San Bartolomé de Almonte. Prof. Diego Ruiz Mata and Dr. Carmen Pérez Pérez, from Cádiz University, supplied me with samples of Las Cumbres necropolis (Hipogeo I) and from Doña Blanca. Mrs. Isabel Santana Falcón gave permission for the study of samples obtained from the excavation, which she carried out at El Algarrobillo, in Valencina. Mrs. Teresa Murillo authorized the inspection of the finds of La Emisora excavation, also located in Valencina, as well as giving samples from the excavation carried out together with the members of the Department of Prehistory and Archaeology of Seville University, Dr. Victor Hurtado and Dr. Rosario Cruz-Auñón, of the burial site of El Roquetito. Prof. Rosario Cabrero, from this same Department, supplied samples from the Amarguillo site, which she herself excavated as well as allowing me to use information not yet published on this important prehistoric site. xii

Prof. V. Hurtado encouraged me and gave me all kinds of facilities to study the remains of metallurgical character from his excavations at El Trastejón (Zufre, Huelva) and La Pijotilla (Badajoz). His intervention gave me access to samples from the “Colección Domínguez”, property of D. Joaquín Domínguez, to whom I offer my grateful thanks. Dr. Leonardo García Sanjuan and Mr. Miguel A. Vargas Durán allowed me to study the metallic samples of their excavation at La Traviesa. Also, Mr. Vargas gave me some unpublished data collected from his survey of the Almadén de la Plata and El Real de la Jara (Sevilla) districts, guiding my steps in the surveys which I made in that area. My colleagues, Mr. Antonio de Padua Díaz, Mrs. Mercedes Rueda and Mrs. Pina López, accompanied me on some of the surveys, thus making the work more effective. The preparation of the topographical plans of some sites of the Aznalcóllar mining zone was carried out by the archaeologist Mrs. Carmen Franco, together with Mrs. Lola Salido and Mrs. Silvana Rodrigues. In the area of Aracena the work of another colleague, Mr. Eduardo Romero, led me to important discoveries. In the Constantina area the help given by Dr. José Juan Fernández in order to visit the mineralisation of San Enrique proved to be indispensable. I should also like to thank Dr. Luis Tomás for his confidence in counting on me to carry out the survey in the Cerro Muriano (Córdoba) mining area and his help in consulting the archives of official institutions. The problems of adapting the computer programmes used were resolved to a great extent by the knowledge and interest of Mr. Lorenzo Dastis and Dr. L. García Sanjuan. I have also been fortunate in counting on the collaboration of friends and thank them for their willingness and availability: the help of Prof. Luisa Garía García helped me overcome my problems with the German language. I have always been able to count on Mr. Francisco José Sánchez Díaz, geographer, as well as the help of Mr. Antonio Muñoz and Mr. Juan Tirado Morueta, Mr. Juan del Valle, Mr. Francisco Garrido, and Mr. Pablo Morilla. It would be unjust not to mention the constant help of my family, especially that of my wife, Coral and my daughter CoralIvy, who adapted themselves to my “necessities” to the extent of renouncing their own. My brothers (John and Javier) and sisters (María Teresa and Anne Mary) have always been willing to help whenever necessary. My parents, John and María Teresa, have given me their unceasing help and collaboration (in a great variety of aspects) from the beginning to the very end of this research. The translation of this work into English (it was originally written in Spanish) has only been possible due to the enormous help and interest of my father, John P. Hunt. Finally, I should like to express my sincere gratitude to Prof. Victor Hurtado, director of my PhD Thesis, who has never ceased to encourage me to continue with this research study and with whose help I have always had in the task of finding the means to complete it.

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Chapter I INTRODUCTION province where, based on little previous information but which began to show a clear contradiction between the mineral wealth and the prehistoric remains discovered (CERDAN et al., 1952), the first archaeometallurgical project in the Southwest Iberian Peninsula was initiated in the 1970’s by IAMS.

The richness in all types of metals of the Iberian Peninsula was praised by classical authors, such as Strabo in his Geography (STRABO, 1969), in which, specifically, the mountains which extend to the North and parallel to the river Guadalquivir are mentioned. The fact that in the Roman period advantage was taken of those riches was clearly shown, among other numerous remains, by the millions of tons of slag which was spread over all the mining districts of the Southwest of the Iberian Peninsula, from the province of Córdoba to the most western deposits of Portugal (DAVIES, 1935; DE ALMEIDA, 1970; PINEDO, 1962, etc.).

Archaeometallurgy already constituted a new discipline developed from a long tradition of the History of Technology, and was at that time consolidated as a field of independent research within Archaeology (TYLECOTE, 1962), with specific research teams such as IAMS in London (BLANCO & ROTHENBERG, 1981) and the German SAM (JUNGHANS et al., 1960; JUNGHANS et al., 1968).

From the more recent exploitations the mythical names of Guadalcanal still echo or, with regard to contemporary times, the enormous sulphide deposits of the Iberian Pyritic Belt, worked for the exportation of their ores.

The interest in this discipline was considerably increased by the controversy on the diffusion or not of the metal production technologies (autoctonism versus colonialism, with the explicit proposition of an independent development in the Iberian Peninsula) and the special consideration given to metallurgy in the evolution of the social structures (RENFREW, 1976; 1978).

The volume and importance of contemporary mining, still in progress, with deposits of the size of Tharsis, Aznalcóllar or Rio Tinto, seem to have produced a tendency to what has been defined as “transtemporal identification of the present environment and its economic implications” (NOCETE et al., 1993).

So, as has been defined, “Renfrew style” (NOCETE et al., 1993), the IAMS project (The Huelva ArchaeoMetallurgical Project) was initiated: if metallurgy could have been discovered independently in the Iberian Peninsula, what place would have be more appropriate for this to have happened than the area of the largest orebodies of Europe, the Southwest of the Iberian Peninsula and fundamentally Huelva, the nucleus of that mineralized zone?

This identification seemed to be backed by the finds belonging to the Orientalizing period which began to be archaeologically documented in the sixties and seventies of the 20th century (GARRIDO ROIZ, 1968; BLANCO & LUZON, 1969; BLANCO et al., 1970) and evidenced a mining activity from prehistoric times. This circumstance was also confirmed by the finding of stone tools proven to be used in mine workings (BLAZQUEZ, 1923), which had been recovered in many mineral deposits from the 19th century onwards by geologists and miners (GONZALO Y TARIN, 1887; CANDAU, 1894; HERNANDEZ PACHECO, 1907; SERRA I RAFOLS, 1924;PINEDO, 1962; DOMERGUE, 1987), continually paying great attention to ancient workings, considered by them as an indication which could lead to the discovery of economically interesting orebodies (MONCADA Y FERRO, 1912).

Moreover, the same mining companies which were still exploiting those deposits, in actual fact those of Rio Tinto, financed the project (BLANCO & ROTHENBERG, 1981). Perhaps, this led to the exclusion of other mines worked by “rival companies”, such as Tharsis, which was studied almost at the same time by C. Domergue, and published in his “Catalogue des Mines et des Fonderies Antiques de la Péninsule Ibérique” (DOMERGUE, 1987), an impressive work not only, although to a great extent, of a summary character which was the first archaeometallurgical study covering the whole of the Iberian Peninsula.

With that viewpoint, the finding of Huelva Hoard was taken as proof of the metallurgical importance of Huelva in ancient times, with an organisation which showed similar characteristics to the mineral exploitation being carried out at the time when the hoard was recovered, significantly when the Tharsis mineral ore pier (one of the several which were built in the Huelva estuary) was being dredged (ALMAGRO BASCH, 1975; PINEDO, 1962).

In any case, The Huelva Archaeo-Metallurgical Project explained that its object was not “a complete survey of the Huelva province, but an endeavour to form a representative profile of the ancient extractive metallurgy of Huelva from its earliest primitive beginnings to the full development of industrial metal production in the Roman era” (ROTHENBERG & BLANCO, 1981: 34).

Although the finding of the remains supporting prehistoric mining were not restricted to Huelva (HERNANDEZ PACHECO, 1907; SERRA I RAFOLS, 1924), it is in that

The basic hypothesis, perfectly logical and based, perhaps, on models from the Near East, more precisely Timna

1

Mark A. Hunt Ortiz VALSERO, 1987), even before checking adequately the available mineral resources of the settlement areas (CHAPMAN, 1991).

(ROTHENBERG, 1972; 1978), was that once located the orebodies, there would be the ancient mines and next to them, also, the remains related to the transformation of ore, and the settlements.

That conclusion, of the importance of metal in the Chalcolithic period, was only arrived at based on the consideration of (again following parallels from the Near East) grooved stone hammers as being used exclusively in that period, with Chinflón taken as the model of mining and metallurgical technology of that moment, connected with the nearby dolmenic graves (BLANCO & ROTHENBERG, 1981), although other investigators directly involved in the Huelva Project, right from the very moment of the excavation, gave, both to the mine workings and to the adjacent settlement, a much later chronology (PELLICER & HURTADO, 1980).

But the first surveys carried out showed the inadequacy of the previously established hypotheses: in the area there were very few habitation sites. Because of this, it became necessary to “extend the Huelva Archaeo-Metallurgical Survey to the coastal areas, including the lower reaches and estuaries of Huelva’s rivers” (ROTHENBERG & BLANCO, 1981:35), but this resulted in a study with no connections whatever. It began to be evident that there was a lack of connection between the location of the mineral resources and that of the prehistoric settlements, at least until the end of the Late Bronze Age.

Today, although in some publications a Chalcolithic date is still given to Chinflon and to the more than 70 mines in which stone hammers appeared (MOHEN, 1992: 88), the date of Late Bronze is accepted for Chinflón (CHAPMAN, 1991; ROTHENBERG & ANDREWS, 1996), although it is also considered that Chinflón, which is the only mine excavated, would be a singular case and would not invalidate the possible relation between megalithism and copper mining, nor the mining exploitation in this zone in the 3rd millennium B.C. (PIÑON VALERA, 1990; NOCETE et al., 1993).

This, which could be considered as one of the most interesting conclusions of the Huelva Project, was not properly valued, insisting with little evidence and using Peninsular parallels (Millares site) in a local indigenous development, perhaps even from an autonomous invention, of metallurgy, which would be the motor of the social transformation (BLANCO & ROTHENBERG, 1981). In this sense, it has been affirmed that the Huelva Project was a failure as far as the articulation of the mine workingssettlements-necropolis is concerned (NOCETE et al., 1993), or to say it in another more technological way, the articulation between mining, the transformation of minerals and the production and use of metal.

The grooved stone hammers could be considered as being used during the whole of the Bronze Age (DOMERGUE, 1987), although there are authors who appear to defend the idea that they were not used until the Middle Bronze Age, following their use in the Argaric period in the Southeast and of their non-existence, it is said, (which is not correct) in the Copper Age and the beginning of the Bronze Age in European mines such as the Balkan mines of Ai Bunar and Rudna Glava, the French Cabrieres and the Irish Mount Gabriel (PEREZ MACIAS, 1996).

But, rather than the actual interpretations made by the Huelva Archaeo-Metallurgical Project which now, after more than 20 years’ research, are considered erroneous (although some did not have to wait long for its invalidation (PELLICER & HURTADO, 1980; DOMERGUE, 1987; CHAPMAN, 1991), it would be convenient to remark that the Huelva Project showed the importance of the archaeometallurgical research in order to gain knowledge of ancient societies, bringing up a series of questions, still not completely answered, which later works have tried and are still trying to resolve with new approaches and taking into account or searching for the data that Archaeology is supplying with regard to the different cultural periods.

Whatever that may be, the interpretation changed regarding Chalcolithic metallurgy from considering it as a fundamental activity which would produce fundamental social changes (BLANCO & ROTHENBERG, 1981) to the opposite extreme: an economic activity almost absent in the archaeological register which showed the insignificant role played by mining and metallurgy in the economy of those times (PEREZ MACIAS, 1996:183).

According to the interpretation of the results, the Huelva Survey considered that “the overwhelming importance of metal in the history of the province can be appreciated by the very scale and extent of the remains of extractive metallurgy in Huelva since early Chalcolithic times” (ROTHENBERG & BLANCO, 1981:163).

In any case, this new interpretation was made from the same approach as that which had been used to defend the contrary, without solving the mentioned disarticulation. This articulation is now trying to be reached through a North-South design, using the Odiel river as the axis (NOCETE et al., 1993), but this has been absent in the research due, partly, to the design of the research projects, both specific or general, in a East-West axis or, in the case of the general ones, without giving metallurgy much importance (CAMPOS CARRASCO et al., 1992; 1995).

This interpretation may have been the base, together with the already mentioned “transtemporal identification”, of an extended vision which has considered the large ore deposits in the province of Huelva as suppliers of raw material to the prehistoric sites some distance away, such as Setefilla (AUBET et al., 1987) or Ardales (Málaga) (DURAN

In the case of the project “Análisis y Definición de los 2

Prehistoric Mining and Metallurgy in South West Iberian Peninsula However, a preliminary bibliographical revision carried out showed clearly that where the information on Chalcolithic metallurgical activities has been concentrated (not only metal objects) is within the projects in which that aspect is not fundamental and which operated in zones far away, to a greater or lesser extent, from the known mineralized areas.

Procesos Culturales en el II milenio B.C.” which began with the object of articulating culturally the South West, different circumstances caused it to remain centred fundamentally in the Sierra de Huelva (HURTADO PEREZ, 1992a). The excavation, within this project, of the site of El Trastejón (Zufre, Huelva) (HURTADO PEREZ, 1990; 1991; 1992; HURTADO PEREZ et al., 1993; HURTADO PEREZ & GARCIA SANJUAN, 1994), has given an archaeometallurgical sequence which has allowed the study of the characteristics and evolution of metal production in the Middle Bronze and Late Bronze Ages, as dealt with later.

This is the case of the Chalcolithic settlements in the southern coastal zone of Portugal (ALARÇAO, 1990; MARTIN DE LA CRUZ, 1994), or the basin of the river Guadiana (GONÇALVES, 1989; MONGE SOARES et al., 1994), some of which such as Sao Bras I, are giving (apart from the proposed copper production in the Southeast Neolithic in Cerro Virtud, province of Almería, see MONTERO RUIZ & RUIZ TABOADA, 1996), the earliest radiocarbon dates for metallurgical activities in the Iberian Peninsula (CASTRO MARTINEZ et al., 1996).

The period in which the archaeological register has clearly shown the complementary nature between areas with mineral resources and zones which lack them is the Orientalizing period, whose archaeometallurgical aspects have been studied, including earlier investigations (GARRIDO ROIZ, 1968; GARRIDO & ORTA, 1978), fundamentally by the research projects under the auspices of the Archaeology Department of the Diputación de Huelva, directed by Dr. Fernández Jurado, both in the town of Huelva (FERNANDEZ JURADO, 1988-1989) and in other areas in this province (RUIZ MATA & FERNANDEZ JURADO, 1986; FERNANDEZ JURADO, 1987b; FERNANDEZ JURADO et al., 1992).

In the same way, similar archaeometallurgical remains appear in the Guadalquivir Valley, in sites such as Valencina (Valencina de la Concepción, Sevilla) (FERNANDEZ GOMEZ & OLIVA ALONSO, 1985; MURILLO DIAZ, 1991; MARTIN ESPINOSA & RUIZ MORENO, 1992; SANTANA FALCON, 1993), Acebuchal (Carmona,Sevilla) (HARRISON, 1977), Amarguillo II (Los Molares, Sevilla) (CABRERO GARCIA, 1987; 1990) and a long list of sites in the agricultural area of the Córdoba province around Castro del Río (CARRILLERO et al., 1982; CARRILLERO MILLAN & MARTINEZ FERNANDEZ, 1985).

This line of investigation is complementary to the studies carried out earlier in the mineralized zones, such as Rio Tinto (BLANCO & LUZON, 1969; BLANCO et al., 1970; BLANCO & ROTHENBERG, 1981), Aznalcóllar (HUNT ORTIZ, 1995), Tharsis (DOMERGUE, 1987) and others (PEREZ MACIAS, 1996).

This also occurs in the alluvial plains in the Badajoz province, as in the case of the sites of La Pijotilla (Badajoz) (HURTADO PEREZ, 1980; 1984; 1988; 1991a) and Castillo de Alange (Alange) (PAVON SOLDEVILLA, 1994; 1995).

Recently the excavations in the Castillo de Doña Blanca (Puerto de Santa María, Cádiz) have widened the geographical limits of the orientalizing metallurgical activity to the ancient coast of the bay of Cádiz (RUIZ MATA, 1992; HUNT ORTIZ, 1995; ROVIRA, 1995a), of which the study is dealt with later.

Most of the archaeometallurgical remains, with few exceptions (for example GONÇALVES, 1989; MONGE SOARES et al., 1994), have not been submitted to a specific study, offering on most cases only a more or less short description.

Returning to more ancient cultural times, with the exception of Cuchillares mine site, of uncertain date (CASTIÑEIRA et al., 1988), the Chalcolithic mining, and to some extent also metallurgy, is found to be in a state of complete indefiniteness in the mineralized zones: the archaeometallurgical projects have been incapable of defining their characteristics, having only, as a base, vague data from casual finds recorded in the bibliography and some others from field surveys in “marginal zones” with regard to the “nucleus” of the orebodies (DOMERGUE, 1987; MERIDETH, 1996).

In actual fact, if something was characteristic of the South West, up to very recent times, it has been the lack of analyses, especially of metal pieces, partly due to the fact that the archaeometallurgical projects, centred on the mineralized zones, did not find them and, on the other hand, the archaeological projects of a non-metallurgical nature, had not programmed the need to do them. So, for example, the idea of an initial metallurgy producing pure copper objects (BLANCO & ROTHENBERG, 1981) was refuted recently by using data from other regions (PEREZ MACIAS, 1996).

This quite obscure mining panorama continues into the Middle Bronze Age, while in the Late Bronze Age the excavated Chinflón mine would be the example of the mining and technological methods of this moment, which, as has already been seen, allow some confusion regarding those -supposedly- existing in the Chalcolithic period (BLANCO & ROTHENBERG, 1981).

This situation, a factor which prevented the global study of archaeometallurgy, is thus consistent with the lack of specialised laboratories in the region and, perhaps, with the impression which can be drawn from the Huelva ArchaeoMetallurgical Project, that it is possible to investigate archaeometallurgy, almost exclusively, through the by3

Mark A. Hunt Ortiz The very complexity of the metallurgical interpretation, especially in the moments when innovations are introduced (FERNANDEZ-MIRANDA et al., 1995) and the lack of global archaeological projects, has been increased by the scarcity of analytical results (in turn, partly due to the lack of specialised laboratories) of objects from the South West. These circumstances, as mentioned before, have made it very difficult to develop complete evolutionary syntheses which, when completed, covered wide regions such as the South of the Iberian Peninsula (HARRISON & CRADDOCK, 1981) or were based on very limited evidence (MONGE SOARES et al., 1994).

products of extractive metallurgy. Of the Chalcolithic and Middle Bronze periods, in the South West, for example, until recently very few elemental analyses were available: from the SAM (JUNGHANS et al., 1960; 1968), the British Museum (HARRISON & CRADDOCK, 1981), most of which came from unclear archaeological contexts, and also from rare analysed objects from specific excavations (for example, FERNANDEZ GOMEZ et al., 1976; RIVERO GALAN & VAZQUEZ RUIZ, 1988) or exceptional metal finds (ALMAGRO, 1962; AUBET et al., 1983).

In the first case, there has been proposed for the South West, considered as a part of the Iberian Peninsula, a sequence which starts with the production of pure copper, in the Millarian period, a sign of primitive technology and evidence of an indigenous development independent of the East Mediterranean. Pure copper was followed by the use of arsenical copper, intentional alloying which would be typical of the Beaker period and would have continued into the Argaric period.

For other periods, such as the Late Bronze Age, and especially the Orientalizing, a larger number of elemental analyses were available, coming from specific sites, such as the Huelva Hoard (ALMAGRO BASCH, 1975) or La Joya necropolis (ESCALERA UREÑA, 1978). The analytical panorama has changed in the last few years, although centred fundamentally on the silver production and leaving copper metallurgy research somewhat relegated, despite having been considered, with all its implications, the Huelva Hoard as the production of a local metal industry (ALMAGRO BASCH, 1975) and having been detected a certain lack of connection between the local production from the mining zones and that of the coastal settlements (BLANCO & ROTHENBERG, 1981).

In the South West the first bronze is detected in the late Beaker period, a single object that is considered to be an intentional alloy, but the question of its possible origin was not treated. So, although rare, bronze appears in Chalcolithic contexts, as would be the case of some Palmela type arrowheads.

Recent archaeometallurgical research has certainly centred a large part of its interest on silver, having been proposed the existence of a local silver production since the Middle Bronze Age, suggested by the finds in La Parrita site (ANONYMOUS, 1981; 1984; BLANCO & ROTHENBERG, 1981; HUNT ORTIZ, 1986; PEREZ MACIAS & FRIAS, 1990) and other sites, such as Cerro de las Tres Aguilas, San Platón and Pozancón (PEREZ MACIAS, 1996), in a way that it is considered by some authors as a technology with knowledge of cupellation and a direct antecedent of the silver metallurgy technology practised in the Orientalizing period. The foreign influences would only suppose, it has been defended, an increase in production, but no mining technology innovation (BLANCO & ROTHENBERG, 1981) nor either a metallurgical one (PEREZ MACIAS, 1995; 1996). However, other authors consider that the use of that silver production technology in the Middle Bronze Age is not in accordance with the data provided by the silver metal objects of this period, and consider, rather, that it indicates the use of native silver or silver ores (ROVIRA, 1995a).

Bronze is also considered to be scarce in the ArgaricMiddle Bronze Age, noting a series of characteristics such as maintaining the arsenical copper and the use of the monovalve moulds, when in other regions it was already out of date. The hypothesis is also suggested of the continuity of the earlier industry because of the lack of means for producing bronze (HARRISON & CRADDOCK, 1981), which implied, in some way, its importation. The introduction of the first bronze objects in the South East, which occurred during the Argaric period, is an aspect difficult to interpret (MONTERO, 1994). On the other hand, based on the study of the metallurgical remains of some sites in the Portuguese basin of the Guadiana, a similar sequence was proposed, with native copper as the first production, followed by intentional arsenical copper and, in the Late Bronze Age, the introduction of bronze (MONGE SOARES et al., 1994).

The same hypotheses have been suggested for the South East of the Iberian Peninsula for the Argaric silver, although with certain differences since the question arose, due to the presence or absence of lead in the metal silver, of the simultaneous use of native silver and silver obtained from argentiferous lead ores (HOOK et al., 1987). The latest interpretations have defended the use of native silver or silver ores; the presence of lead would only signify contamination (MONTERO, 1994).

A recent synthesis of archaeometallurgical character in this zone (PEREZ MACIAS, 1996), which can be considered as a general revision of the Huelva Archaeo-Metallurgical Project, showed well the state of research in the province of Huelva. From a wider knowledge of the area from the data supplied by different archaeological projects carried out in the last few years, it establishes a series of possibilities and conclusions regarding the metallurgical activities from the Chalcolithic to the Late Bronze Age, to many of which 4

Prehistoric Mining and Metallurgy in South West Iberian Peninsula be connected with the appearance of bronzes and which would also be present, although they were not identified as such, in other contemporary sites of the region (MARTIN DE LA CRUZ, 1989).

alternative interpretations are offered in this research study. The need of a global archaeometallurgical vision, which starts from the consideration of the mineral resources, revises the transformation and production and recognises the characteristics of the metal objects used, can be confirmed in projects as that recently published on the South East of the Iberian Peninsula (MONTERO, 1994). But this project could not have been carried out without the backing of a permanent analytical programme, which in this case was the “Proyecto Arqueometalúrgico de la Península Ibérica” (PA) which, from an analytical approach similar to that developed by the SAM, but conscious of the deficiencies of this German project, pursues new objectives, which now began with the study of the mineral resources (MONTERO, 1994).

Considered globally, a rather disjointed archaeometallurgical panorama is seen in the South West Iberian Peninsula, with an unknown metallurgy in Chalcolithic Huelva, which area, however, is surrounded by sites in which pertinent metallurgical activities have been described: South Portugal, Guadalquivir valley, the Badajoz plain, but for which, except for a few exceptions, no references are available other than, at most, the composition of the objects. The proposed evolutionary sequences do not appear to be agreed upon among the different investigators. So, that sequence, as had been traditionally established for a local metallurgy (RENFREW, 1976), would begin according to some, with the use of pure, native copper (MONGE SOARES et al., 1994) or produced from copper carbonates with no impurities (HARRISON & CRADDOCK, 1981; BLANCO & ROTHENBERG, 1981), although other authors consider that the alloys with arsenic are those first used, which, in any case, could be not unintentional (ROVIRA & MONTERO, 1994a), or due to the use of arsenical ores but not intentional (PEREZ MACIAS, 1996) or intentional (HARRISON & CRADDOCK, 1981).

This permanent project, the PA, backed by a competent archaeological team, has concentrated fundamentally on the elemental analysis, using XRF, of metal objects, accompanied by metallographic studies, together with ores and by-products. As far as South West Spain is concerned, the work of the PA has supposed an important quantitative change regarding the knowledge of the prehistoric metal production, especially concerning the manufactured objects. Recently, a monograph has been published containing all the analytical results (ROVIRA et al., 1997), although some of these from South West Spain were published before by the members of the PA or other investigators, for whom the analyses were carried out, centred in concrete areas or definite cultural periods and specific excavations. Among the published works the most important are, those on the Palmela arrowheads in the Guadalquivir Valley (ROVIRA et al., 1992), the prehistoric metal production in the provinces of Cádiz (ROVIRA & MONTERO, 1994), Córdoba (LOPEZ REY, 1994), Sevilla (MONTERO RUIZ & TENEISHVILI, 1996), Huelva (ROVIRA et al., 1987; ROVIRA, 1995; 1995a; GOMEZ RAMOS et al., 1999) and Badajoz (PAVON SOLDEVILLA, 1995).

Also, in the Chalcolithic period, according to some authors, the introduction of the first bronze alloys would occur (HARRISON & CRADDOCK, 1981), which for others only appear from the Middle Bronze Age (GOMEZ RAMOS et al, 1999) or even no earlier than the Late Bronze (BLANCO & ROTHENBERG, 1981; MONGE SOARES et al., 1994), with a local production of arsenical copper during the Middle Bronze, which in some cases is just supposition, as in Setefilla (AUBET et al., 1983), or with data which appear to support it, as in El Trastejón (HURTADO PEREZ & GARCIA SANJUAN, 1994) or in the nearby site of Puerto Moral (PEREZ MACIAS, 1996).

Among the not yet completely published works of the PA, of special interest is that containing data from the site Llanete de los Moros (Montoro, Córdoba) with a cultural sequence starting in the Early Chalcolithic and covering the Bronze Age, although it is still not possible to count on a structured archaeometallurgical evolution and it will be necessary to wait for these analytical data to be integrated in the correct archaeological context (ROVIRA, 1995a) by the investigators of the site (MARTIN DE LA CRUZ, 1987).

Silver, since its appearance in the South West during the Middle Bronze, is considered by some authors as produced locally by cupellation from jarositic type ores (PEREZ MACIAS, 1996) and by others as not cupelled and related, in any case, to other different mineral sources, native silver or silver ores (ROVIRA, 1995a). The mining technology of the Middle Bronze is, as happens with the Chalcolithic, practically unknown.

It is notable that the dynamic of occupation and exploitation (reconstructed through pollen, fauna...analysis) of Llanete de los Moros is found to be more related to the use of the resources of the agricultural land than to those of the mountains (MARTIN DE LA CRUZ, 1993).

The Late Bronze is a period which is archaeologically badly defined, with no precise limits (BELEN DEAMO & ESCACENA CARRASCO, 1995), but with a mining activity characterised through the Chinflón excavation (ROTHENBERG & BLANCO, 1980; 1981).

This site also has an additional interest, apart from the continuous sequence which it appears to present, namely, the evidence of Mycenaean imports (pottery fragments) from as early as the 14th-13th century B.C. that appears to

Certainly it is known how the mining was but not if it was exclusively representative of that period. It is a mining activity considered as very widespread in pre-Orientalizing 5

Mark A. Hunt Ortiz geological and edaphological characteristics, mineralogically sterile, but which on the other hand allow other types of economic activities.

moments but which contrasts with a scarce local copper production which, as well, does not seem to agree with the abundance of bronze objects which could be either of local manufacture (ALMAGRO BASCH, 1975; ROVIRA, 1995) or imported (see RUIZ GALVEZ, 1995), at a time when tin is appearing as part of shipwrecks in the Western Mediterranean (PENHALLURICK, 1986) and, perhaps, a little later, in workshops on some points along the Levantine coast (GONZALEZ PRATS, 1992).

As far as the circumstances have permitted, a whole series of specific analytical techniques have been used in relation with the concrete questions to be answered. In this way, an effort has been made, after its definition, to articulate and, at the same time, to effect contrasts between mining, the transformation of metal and its production and use in the South West of the Iberian Peninsula, for which samples from archaeological sites belonging to different geographical areas and cultural periods have been made available.

In the Orientalizing period, the ceasing of copper mining activity has been defended (PEREZ MACIAS, 1996) although the use of copper as an alloy is widespread, while the interest was concentrated on silver production, about which, as mentioned already, there is no unanimity on its being considered as imported technology or an indigenous technology expanded because of an external demand, centred on coastal points such as Huelva or Castillo de Doña Blanca.

Geographically, the chosen area corresponds -centrally- to a large part of Western Andalusia, which would coincide, according to present-day administrative division, with the provinces of Huelva, Sevilla, Northwest Cádiz and West Córdoba. At the same time, non-Andalusian zones have been studied, either directly, as the South of Badajoz province, or exclusively through the published data, as is the case of the South of Portugal.

It is in this period, either sooner or later, when it is considered that iron was introduced as a foreign innovation (PELLICER, 1989; ALMAGRO-GORBEA, 1993; ROVIRA, 1995), with no question of its earlier local production, although in some cases the analytical evidence, as in the Trastejón site, according to the published data (PEREZ MACIAS, 1996), was interpreted as evidence of iron local production.

The ample size permits a comparative, or rather complementary, study of the different zones (mineralized and non-mineralized) during the whole of the Recent Prehistory. Also, it allows all the types of relations proposed for the different periods to be covered, from a local production to cover a merely local demand, proposed not only for the Chalcolithic period (GARCIA SANJUAN, 1994), to a mining-metallurgical activity of Colonial type organised and directed towards the exportation of metals to extra-Peninsular areas (GALE et al., 1980:49).

With regard to the use of analytical techniques in the study of the prehistoric archaeometallurgy in the South West, despite the development which these techniques have had in the last few years in their application on the most varied aspects of archaeometallurgy (BACHMANN, 1982; PARKES, 1986; LEUTE, 1987; GALE, 1989), in this zone it has been traditionally restricted to elemental analyses, first by chemical methods and then physical.

Chronologically, this study has been confined, for practical reasons fundamentally, to the division of the large cultural periods in which Prehistory is divided in the area, although in this respect there is no unanimity (MARTIN DE LA CRUZ, 1989): Chalcolithic, Middle Bronze and Late Bronze, with a calibrated chronology extending from the end of the 4th-beginning 3rd millennium BC to the first centuries of the 1st. millennium BC (CASTRO MARTINEZ et al, 1996).

Until recently, when the PA has used it frequently, metallography was only used on specific occasions, as with the material from La Joya (ESCALERA UREÑA, 1978) and in some weapons from the Guadalquivir (RUIZ DELGADO & HUNT ORTIZ, 1989). In this panorama, there are rare exceptions. In this geographical area and with regard to the Protohistoric metal production, the study of the metallurgical materials excavated in Monte Romero has to be noted (KASSIANIDOU, 1992), with the object of not only determining the elemental composition, but also the mineralogical phases and even the lead isotopic characteristics of the finds.

In the last period, the Late Bronze, to study with more detail the possible technological innovations that might have taken place, it has been subdivided into two different periods: Pre-Orientalizing Late Bronze and Orientalizing Late Bronze. The establishing of precise limits between periods, and their chronologies, is always very problematic, especially for periods of transition. For example, for the South West various authors have noted the lengthy continuity of the Beaker period (MARTIN DE LA CRUZ, 1989), producing a negation of the Middle Bronze or, rather, accepting the contemporaneity of different cultural manifestations, as would be the late Beaker Horizon of Acebuchal (HARRISON, 1977) and the Middle Bronze levels of

Based on the results of the research projects described, in this study a new diachronic approach to the prehistoric archaeometallurgy of the South West Iberian Peninsula is designed. This approach is basically technological and of a wide geographical area, not reduced to those mineralized zones in which the metallurgical research had concentrated nor to the areas considered today of great mining significance, but rather including other areas with 6

Prehistoric Mining and Metallurgy in South West Iberian Peninsula and differentiated lead isotopic composition of each mineralization and the permanent nature of that composition through the whole of the different metallurgical processes. This allows, theoretically, the establishing of the source of specific metal objects. But, rather than arrive at determining that origin, which is also an aim, the principal objective of the use of the lead isotopes analyses has been to establish its degree of application in this area through, in the first place, the setting up of a data bank, even though limited, of the mineralizations of the different geological domains of the South West in order to, later, be able to compare them with other mineralizations already characterised, and with the metallurgical by-products and the metal objects.

Setefilla (AUBET et al., 1983), which have been related, in turn, to the cist-burial culture of Huelva and other sites such as El Trastejón (HURTADO, 1989), dated as belonging to the first half of the 2nd. millennium BC (non calibrated). A particular problem is caused when establishing valid archaeological criteria, apart from wheel-made pottery, to decide whether a site is either Pre- or Orientalizing (BELEN DEAMO & ESCACENA CARRASCO, 1995). On the other hand, new archaeological excavations seem to be supplying evidence of earlier dates for the arrival of the Semitic influences, which would have preceded the permanent settlements (LOPEZ AMADOR et al., 1996). Generally speaking, the placing of a particular site in a precise period has been established, and even more so if it has been published, according to the criteria of the investigator who studied it, although possible alternative dating is pointed out when it has been suggested by other investigators or when relevant indications exist, also of a metallurgical order.

Thus, the choice of a wide geographical framework was also conditioned by the convenience in regard to the study of lead isotopes to include, to a lesser or greater degree, various geological regions, which have been the Hercynian, subdivided into the Ossa-Morena and South-Portuguese Zones, with their respective domains, the Tertiary Depression of the Guadalquivir, and also, though tangentially, the Subbetic Zone.

To develop this investigation it has been considered imperative to know the potential of the mineral resources of the whole of this area. The defining of the characteristics of the mineral resources, their distribution and abundance is fundamental when arriving at an archaeological interpretation with regard to their relation with settlement location, the later metallurgical phases, and their consideration as a critical and controllable resource or as a resource of limited interest (MUHLY, 1989; MONTERO, 1994).

Another fundamental field of action is the compiling of the data referring to metallurgical activities, both from bibliography and from direct study, and, when possible, analyses of samples coming from different archaeological surveys and excavations. As for manufactured objects, all the analytical results from the bibliography have been considered. To them a large number of analyses carried out by the PA, which have been made available for this study before being published, must be added. These, together with the results of the different analytical techniques applied in this project, have allowed a new approach to be made to prehistoric metallurgy in the South West Iberian Peninsula, which is now to be presented.

For the explanation of local metallurgy development, first of all the natural resources that could be available must be studied. To suggest an autonomous production in areas without resources can only be done in terms of commerce or exchange, which also has social and economic consequences. On the other hand, in these commercial networks metallurgical sites have been set up which, after a study of the neighbouring areas, have shown that they had mineral resources to hand (CHAPMAN, 1991). The study of the mineralizations has been carried out by extracting data from bibliographical sources as well as by surveys of certain areas with a specific methodology, with the aim of, on the one hand, the study of mining technology and its development in the different cultural periods and, on the other hand, the selection of samples to be studied using different analytical methods. The elemental analyses of the ores give fundamental data regarding their relation with later metallurgical phases and the production, intended or not, of metals and metal alloys. However, the use of these results to establish the original connection between a mineralization and the metal object has been, generally, of little use. On the contrary, that relation could be established by means of lead isotope analysis, an analytical method of which the use in the field of archaeometallurgy is based on the typical 7

Chapter II METHODOLOGY orebodies in the Huelva and Sevilla provinces, exploited to the present day, had already been worked by the ancient peoples” (FRITSCHI Y FITZ, 1892:58).

II.1.MINING-METALLURGICAL SURVEYS The surveys carried out in the different zones of the geographical area covered have always had an archaeometallurgical character, centred on the different mineralized zones and with two fundamental objectives: the recording and study of prehistoric mining and whenever necessary, metallurgical activities, and also, the collecting of mining and metallurgical samples for analysis by the different methods employed.

This connection was considered of importance up to the present century, so that it was affirmed in mining manuals that “mine workings carried out in more or less remote eras whose remains might be recognised...can constitute... the basis of an important discovery” (MONCADA Y FERRO, 1912:30). This practice was so extended in the 19th Century AD (for the ease in locating an exploited orebody rather than an unexploited one) that even its use was denounced to be abusive and almost exclusive (FRITSCHI Y FITZ, 1892:59).

To carry out these surveys (which generally had an extensive character conditioned by the resources, especially human, available) a specific methodology has been followed, composed of different phases and in which, for its design, various factors have been considered, some of them hypothetical.

This means that, taking into account the mineral substances exploited in antiquity, the knowledge of the chronology of the modern exploitation of an orebody may be a very important factor when considering if it could have been exploited in ancient times.

Similar methodologies have been put into operation in other geographical contexts, with good results (LARRAZABAL GALARZA, 1995). II.1.1. Documentation

Here can be seen the contradictory character of mineral exploitation: while on the one hand later exploitation can facilitate the locating of previous workings, on the other hand, the very nature of mining activity and its technological evolution tends, inevitably, to destroy completely the remains of earlier times. Paradigmatic cases can be found throughout the Volcanic-Sedimentary Complex, in which, since the 19th century AD to the present day, opencast workings and the use, as ballast or as ore, of the slags have produced tremendous losses in prehistoric and later remains, of which only the minimum of information is available.

As in any archaeological survey, the study of the chosen areas began with the compilation of existing data. For archaeometallurgical surveys this data is particularly dispersed since the investigation must cover areas of diverse specialities such as Geology, Mining, Mineralogy, Archaeology, History, Biology... The mining activity in the South West Iberian Peninsula has a very long tradition. It is a zone in which, during the last centuries many efforts have been made, with an economic purpose, to detect, study and exploit the mineral deposits. For this reason, the compilation of documents of different characteristics has been considered the first action to be taken after the selection of the specific geographical areas. As a starting hypothesis, it has been considered that the systems of modern mine surveying have not changed substantially until a few decades ago, when geophysical methods of mineral deposit detection were developed. Until then, only external signs of the mineralization (of different types, such as outcropping, colouring, differential growth of vegetation...) would permit its location.

II.1.1.1. Geological and Metallogenetic Maps As primary information sources, the study of the geological and metallogenetic maps have been considered a fundamental first approach to the area. The geological maps (MAPA GEOLOGICO DE ESPAÑA, Scale 1:50.000, Instituto Geológico y Minero de España. Edition 1982) (abbreviated MGE), are accompanied by a geological introduction to the zone they cover, a chapter on metallogenesis and, in the Economic Geology section, a brief reference to the main exploitations. Also, the bibliographical references which appear are of interest as the starting point in the search for new data.

Moreover, it was thought that during the technological evolution which has occurred in the different cultural phases until the present day, the remains of earlier mining activities have been a reference when prospecting for mines during later times, in which technological advances permitted orebodies, which had been considered uneconomic, to be put into operation again.

Even more interesting are the metallogenetic maps as an introductory source, although by now they are more than 25 years old (MAPA METALOGENETICO DE ESPAÑA, Scale 1:200.000, IGME, Edition c.1973) (abbreviated MME). In these, the mineral indications are located in a synthesised geological background. Generally, it is

So, with regard to the zone to be studied, it was said, at the end of the 19th Century AD, that “all iron/copper pyrites 81

Prehistoric Mining and Metallurgy in South West Iberian Peninsula or which can lead to their detection. The most usual are:

necessary to establish a relation between the geological substratum and the mineralization, a point which is also dealt with in the geological map. That is, to put aside, to begin with, the non-mineralized geological zones and to concentrate the investigation on geological domains associated with particular types of mineral deposits.

*Mina (mine) and its derivatives (minilla...) and compounds (Casamina, Cortijo de la Mina...), as well as the word of Arab origin almadén (mine) (COROMINAS, 1990). While almadén, of which there are not many examples, appears to refer exclusively to mine workings, the word mina sometimes refers to, although not often in the zone under study, shafts and galleries for collecting water.

In the metallogenetic maps it must be borne in mind that sometimes the data are from drills or other types of modern detection methods, and refer to mineral deposits that do not outcrop and are of no interest for this research study.

*Quite often the toponymy does not refer to mine workings in general (like mina and almadén) but to concrete mining works, as is the case of toponymies such as socavón (trench), pozo (shaft), hondo, hueco, silo and even caño and their derivatives and compounds.

The characteristics of the mineral deposits are treated individually in the metallogenetic maps, specifying their geological origin and the type of ores, although, frequently, not all the minerals are mentioned. For example, in mines considered as pyritic deposits in metallogenetic maps, the archaeological investigation has shown that they were exploited for silver ores in a particular period. So, the paragenesis of the ore deposits can only be considered as a reference in the MME maps.

*Occasionally there are names which give a more natural origin to mine workings: the word cueva (cave) is unusually applied to mining galleries, either large or small. Examples in the zone under study are plentiful: Cueva del Monje, in the Paterna area, and Cueva del Tabaco in Río Tinto (BLANCO & ROTHENBERG, 1981), Cueva de Cuchichón in Aznalcóllar, Cueva de San Francisco in Guadalcanal...

In any case, the MME maps constitute a first class source, determining and delimiting the mineral zones as well as pointing out the location of the deposits or traces of the deposits.

*There are also place names which refer to the metals exploited or treated: plata (silver) (Molino de la Plata...), hierro (iron) (Cerro del Hierro...), etc.. For modern times the word martinete designated the place where copper (and iron) was beaten and, sometimes, also smelted. Thus, the metallurgical slags that can be found in these areas would correspond to modern production.

The sources for the making of these MME maps, on the other hand, are very diverse and, as is noted in the publication itself, are based on “confidential” reports and documents, publications, administrative files for exploitation permits, and special investigations in certain zones and surveys by the IGME’s own teams (MME, 1973:10). These maps also set out the bibliography used to make them.

When taking into account this type of place name it must be remembered that those referring to noble metals are, nearly always, the result of traditions or legends (Fuente del Oro, Arroyo de la Plata...).

II.1.1.2. Topographical Plans: Symbols and Toponymy Once the area limits are chosen and the information on mineral deposits from the MGE and MME maps is collected, since, in these maps, by no means all the existing mines are registered, it is convenient to study the topographical maps. Of these, two series have been very useful: the Servicio Geográfico del Ejército (1:50.000) and the Instituto Geográfico Nacional (IGN) (1:50.000). Mine workings are shown with their corresponding symbol, although this has not always been done in a regular way and sometimes mine workings perfectly visible, and of some importance, are not shown, while smaller ones, which may only be a small trench, are registered. In general, few mine workings are shown in the topographical maps compared with the number which are known to exist through archaeometallurgical surveys.

*The colouring of waters or outcroppings is one of the most well known signs of mineralization (FRITSCHI Y FITZ, 1892:59), which can give place names that refer to the colour, normally reddish tones, due to gossans (iron hats of oxidised iron ore) which are formed on the surface. The names are colorado and tinto (Cerro Colorado in Río Tinto /red river, Los Coloradillos), almagrera or bermejo and their derivatives and compounds. The reliability of these names is not high in some areas, since in certain geological contexts (such as Morón de la Frontera, Sevilla) the red colouring is very extensive without forming real ore concentrations. In any case, bearing this in mind, it is a toponymy to be considered since in other contexts, Palaeozoic, it is almost always related to mineral outcrops.

Consulting both map series is advisable due to the fact that the information they contain is not the same and mines that do not appear in one of the series could appear in the other. When mine workings do not appear as such with the corresponding symbol (which is the same for quarries) one may deduce its existence through toponymy. There are many place names which refer to the existence of workings

* One of the place names which has been of great use and is quite trustworthy is escoria (slag) and its derivatives. Normally, what is easily detected and is clearly visible are the heaps of slags and the usual term is escorial (slag heap). This name rarely errs and is normally found near mining 9

Mark A. Hunt Ortiz works (such as Cortijo Los Escoriales in Constantina, Sevilla). Sometimes the existence of slags is also shown by the toponymy herrerías (smithy area), and a lot less by the term fundición (smelting place). Large slag heaps are normally from the Roman era or later, although, as mentioned before, this is an indication of the possible earlier exploitation of the related mine.

the documents in these archives should be inventoried, as otherwise it would be impossible to carry out the task involved. Luckily, there are occasions when this has already been done (as in the case of GONZALEZ, 1832) although, sometimes, the location of the described mining works, perhaps defined only by long-forgotten place names, has been impossible.

Before passing on to the following phase, all the data collected has to be placed as exactly as possible on the survey map. Often, the name of mining works had changed and various names may have been used, over different periods, for the same workings.

Similarly, the historical-economic works which are based on documents taken from archives must be mentioned. A magnificent example of this is the work of Dr. Sánchez (SANCHEZ GOMEZ, 1989), which offers data which can be related, even, to the prehistoric exploitation of certain mines.

In this sense, the sources studied, until now, allow the more or less exact location of the exploitation, with, in any case, acceptable errors, which still permit the location. This does not happen with all the sources that are going to be mentioned below.

Archaeological works, as well as those on excavations in sites with mining and metallurgical evidence, are fundamental. A general work of great interest, covering the area under study, is that of Oliver Davies (1935) and on the Iberian Peninsula the impressive work of Claude Domergue (DOMERGUE, 1987). For the specific South West zone, that with the results of the Huelva Archaeo-Metallurgical Survey (BLANCO & ROTHENBERG, 1981), a pioneer in Spain on this type of approach.

II.1.1.3. Written Sources Within this section two different types are considered: *Publications and documents of geological, mining and mineralogical character.

II.1.1.4. Unwritten Sources This type of source consists, fundamentally, of the items to be found in different museums and private collections. Not only in reference to archaeological museums but others of a different nature, such as the recent and inexplicably scattered Museum of Natural Sciences of the University of Sevilla, with objects collected from the 19th century AD, including prehistoric mining tools and a magnificent collection of minerals (GALAN HUERTOS, 1993).

This group is formed by national or international periodicals (Studia Geologica, Revista Minera, Mining Magazine, Transactions of the Institute of Mining and Metallurgy...) and monographs, some of them especially useful (GONZALO TARIN, 1888; CALDERON, 1910; PINEDO VARA, 1963...). They are publications that offer data on geological areas or specific mines and which, especially the older ones, frequently give a small historical account or mention the most important archaeometallurgical finds (such as Libro Blanco de la Minería Andaluza, 1986).

It is worthwhile bearing in mind the origin and/or nationality of the companies which, before the creation of the Spanish Historical Heritage legislation, exploited the mines: sometimes the remains located are found in museums of the regions or the countries of origin of those companies.

Although not published, this section includes the technical archives. The most important of these is that of the IGME (Madrid), containing sometimes superb works, with a detailed survey, good plans of workings and mineralogical studies on concrete mineralized zones.

It must be also mentioned that occasionally mining companies created archaeological collections at the mines with the finds discovered during exploitation, as happened with Tharsis, Rio Tinto (Huelva) and San Enrique (Sevilla). These should be studied carefully.

For the area covered, files and reports kept in the archives of the provincial offices of the Consejería de Industria (Industrial Dept.) of the Junta de Andalucía, (Andalusian Government) have been useful. In some cases, apart from the difficulty in obtaining access to them, the older files are badly catalogued and in some disorder. * Publications and documents archaeological character.

of

historical

II.1.2. Location of Mines In general, mine workings can be divided into two large groups: opencast and underground mines.

and The first type, for the size of the workings and waste heaps, is easy to find.

Historical descriptions of villages or concrete areas can be very useful (CANDAU, 1894; LOPEZ, 1989; MADOZ, 1845-1850). Historical archives can also be of great use, both local as well as on a wider scale and even, also, the “public notaries” protocols. Naturally, it is imperative that

Underground mines, of quite different types and scale, are more difficult to detect, although the associated dumps and heaps, normally consisting of waste rock, mineralized to some extent, which impede or prevent the growth of 10

Prehistoric Mining and Metallurgy in South West Iberian Peninsula The possible identification of mine exploitations through the lack of vegetation has already been mentioned. Besides this negative value, in the surveys carried out for this project, the relation between a specific vegetal species and, in principle, slag heaps has been noted.

vegetation, help in their recognition. *Aerial Survey. The use of the different series of vertical commercial aerial photos for the detection and study of mining works has been helpful on certain occasions. The case of the Roman gold mines, exploited by the “arrugiae” method (PLINY, 1984: XXXIII, 70...) in the Northwest of the Iberian Peninsula, is a notable example. The same method was used to detect possible similar workings in the gold fields of the Peñaflor area (Sevilla), but with negative results (DOMERGUE, 1987:471).

This plant has been identified as “Rumex Bucephalophorus”. The studies carried out consider it to prefer sandy soil and showing a distribution over Western Andalusia. It is a small reddish plant with a recognisable ochre-ish coloured floration (VALDES et al., 1987:292).

For the surveys carried out within the South West, the use of commercial aerial photos, taken on a large scale, for the identification of small mine workings has been of very limited relevance.

No reference was found regarding the tolerance of the Rumex Bucephalophorus to metal elements, and not even regarding its tendency to appear more abundantly in mineralized areas.

On the other hand, in the extensive areas of reforestation in the geographical zone studied where eucalyptus and bushes predominate, the visibility during ground surveys is very limited, making the complicated orography an additional negative factor.

Only one mention, rather romantic but interesting, was found referring to “small reddish flowers” growing on the slag heaps around the Poderosa mine (PINEDO, 1963:440). The same association was found in several slag heaps, such as that on the hill of the old explosive store in Cala mines. Thus, it was considered that, through taking advantage of the reddish colour which makes it perfectly discernible at a distance, the Rumex Bucephalophorus should be taken as another indication for the detection of slag heaps. In actual fact this has been the only plant to show a practical use in the detection of archaeometallurgical sites and, even, in some surveyed areas, the Rumex Bucephalophorus appeared, alone, not only on slag heaps but also in mineralized areas.

To resolve these limitations, aerial surveys have been made in specific sectors (limited because of high financial costs) using a Zessna 172 plane, maintaining a height of between 300 y 900 feet above the surface to be surveyed. Once a possible mine had been detected it was photographed in such a way that topographical references were also included, allowing its later location on the ground. The most distinct signs of the small mining works were their associated dumps: areas of little or no vegetation, frequently forming a crescent shape.

In the Paterna (Huelva) zone, for example, this plant was used for the detection of mine workings, mineralizations with no mining activity and slag concentrations, appearing only in these places, not any others.

The study, on the ground, of the possible mines detected by aerial survey, confirmed the trustworthiness of the method, which has been shown to be the most effective for the particular sectors where it was applied.

In La Sierrecilla mine area (Paymogo, Huelva), to mention another example, the slag, sometimes scattered without forming heaps, was detected by the presence of this plant, which formed reddish patches which showed up among the rest of the vegetation.

* Phytoarchaelogy. The use of the vegetation for archaeological ends is today an established field of research (BROOKS & JOHANNES, 1990), but the geobotanical methods of mine surveying have been used for centuries. In the 16th century AD, the difference in growth of vegetation was considered to be an indication for detecting mineralizations (AGRICOLA, 1950). Much more recently, geobotanical studies have established the systematic relation between certain vegetal species and mineralized zones of zinc, copper, nickel...due to the tolerance of these species to concrete metal elements (BROOKS & JOHANNES, 1990:16 ).

The scientific study of the connection of the Rumex Bucephalophorus and highly mineralized soils is still to be done, and the metal element or elements which this plant tolerates is still not defined. This study, which has both archaeological and environmental implications, should be the direct object of botanical research. * Local Enquiries. Enquiring among people who know the ground, individuals who live or work in the zone to be surveyed (forest guards, hunters, shepherds, geologists...) have facilitated the location of archaeometallurgical sites being looked for and the discovery of unknown ones, frequently near known exploitations. Sometimes, because of the characteristics of the orography or vegetation of the area, it is practically impossible to detect a mine, although clearly situated on the survey map, unless directed by a person knowing its exact position.

This is a line of investigation to which, lately, Biology is paying special attention in the South West of the Iberian Peninsula, due to the interest in correcting the enormous environmental impact produced in the mining areas (opencasts, waste heaps, residual dumps...) by mining and mineral treatment (BERMUDEZ DE CASTRO et al., 1988; SOLDEVILLA et al., 1992).

11

Mark A. Hunt Ortiz more often and which can give an approximate idea of the period or periods during which the mining work was carried out. There are three basic types.

II.1.3. Study of the Mining Works Once the mineral exploitations have been located, previous field experience, the type of the outcropping and the mineralogical characteristics of the ore indicate whether it could have been exploited in Prehistory, what type of remains could still exist and where these are to be looked for.

- Typology of the mine. The characteristics of the workings can indicate the date, in a wide sense, of the mine. Thus, superficial works in the form of trenches or “rafas” in copper mineral deposits are in all probability and in a general sense, prehistoric.

Open cast exploitations have to be surveyed as an enormous archaeological site. Apart from surveying the mineralized zone not affected by the opencast, where metallurgical byproducts are often found, it is essential to survey the opencast itself, especially the upper benches. For example, the Aznalcóllar opencast sectioned and exposed three levels where diverse ores had been mined, using methods of different typology and chronology (HUNT ORTIZ, 1994).

It is also quite frequent, practically the rule, to find mixed typological workings in the same mine. The identification of the wood used as pit props can also be a pointer to dating, although in the present state of the investigation, applicable only to recent times (DIAZ QUETCUTY & BLANCO MORENO, 1970). - Tool marks. These marks usually coincide with defined typologies: those mines of trench type present rounded tool marks from the use of blunt stone tools. From, fundamentally, the Roman period, marks of metal picks, chisels and awls appear. The difference between Roman tools and those of earlier or later times is still not well established. A mark that is definitely contemporary is the drill, related to the use of explosives, which was applied commonly to mining from the second half of the 18th century AD (HOLLISTER-SHORT, 1994).

Even in the ore deposits worked in recent times or still in exploitation, and despite the capacity of opencast mining for destruction of previous mining works, the presence of remains of earlier mining activity has been documented. In the few cases in which previous mine workings have not been detected, the use of the sources of information mentioned may allow, although not in detail, the archaeological evolution to be established. Depending on the exploitation, it is well to bear in mind that there are some mining companies which have historical material in their own archives. If this should be the case, its revision is recommended, especially old mining plans, which in many cases included the earlier mining works detected. One must remember that, in mine management it is fundamental to record the mining works which have been previously carried out for two important reasons: one, economic, is the exact cubication of the available ore, and the other, for security, to “avoid to direct the work to places which could break into sunken mines, full of water or invaded by gases” (MONCADA Y FERRO, 1912:321).

It must be borne in mind that, sometimes, because of the nature of the host rock, no marks appear or they must be looked for very thoroughly. And also, it is possible to find types of tool marks mixed together, if the mine has been exploited in different periods. - Stone Tools. One of the archaeological items which appear most frequently in prehistoric mines is the stone mining hammer. These hammers, either clearly grooved, or just with notches or without them, appear outside the workings and are easily detected, not only by their form but also because they are normally made from rocks, often from pebbles, mostly volcanic and geologically distinctive from the rocks of the outcrop. The chronology of these lithic tools is still not fixed but they were certainly in use during the whole of the Bronze Age and also part of the 1st. millennium BC.

Apart from those mentioned, there are other ways of collecting information, in the mining exploitations themselves. In a large number of present mines which treated the mineral at the mine, electro-magnets are usually installed which separate all the metal objects from the ore so that the belts and industrial installations are not damaged. It was not unusual to recover in such a way old mining tools, mainly Roman in some of the mines.

Sometimes, as mentioned before, slags are found in the vicinity of the mines. This type of remains may also, for its typology, be used as an indication of the date of the mining and metallurgical activities (BACHMANN, 1982). In any case, fundamental typological aspects (from the actual mine works to the tools used) have still to be subjected to a more exhaustive study. To define them correctly would certainly be a great help for archaeometallurgical investigation, but it is an impossible task without archaeological excavations.

*Dating of mine works: The extremely few mines that have been excavated in this geographical area have supplied pottery and organic remains in their interior which have allowed dating, although controversial, such as in Chinflón (ROTHENBERG & BLANCO, 1980). Normally, in the surveys of small prehistoric exploitations, no pottery remains are found outside the mine, although fragments occasionally appear. In Roman mines pottery is much more abundant. In any case, there are other remains, directly connected with mining technology which appear

II.2. ANALYTICAL METHODS An important part of the archaeometallurgical investigation 12

Prehistoric Mining and Metallurgy in South West Iberian Peninsula possible at a particular moment.

carried out in this project in the South West of the Iberian Peninsula has been based on the application of different analytical methods to samples from the region, both from the surveys as well as from diverse excavated sites.

In other cases, where “partial access” existed, only a limited number of analyses were able to be carried out, very often because of lack of funding.

With respect to the methodological design, the selected samples, once described after a visual inspection, have to go to the laboratory for a first basic approach, the defining of its elemental composition. This is followed, when considered necessary, by the determination of other characteristics which define it: mineral phases, microstructure, distribution of elements, etc.

The lack of availability of permanent analytical facilities has meant for this project, as pointed out, a serious inconvenience, since the samples could not be requested from investigators and institutions in a systematic way, having in mind the uncertainty of being able to comply with any agreements reached and promises made. In any case, the general helpful attitude of the research centres must be pointed out. They shared their resources between their own lines of investigation and the analytical needs of this project, which were in many cases somewhat of a novelty for them.

As will be seen from the explanation of the different methods employed, it is most important to establish the objectives which are aimed at, for each sample, bearing in mind the characteristics of the sample itself, as well as the analytical methods available, the experience and degree of specialisation of the laboratory, the requisites of each method and the information which it is possible to obtain from them. Also, if the method is or is not destructive, which elements are to be analysed and what are their detection limits...

To these restrictive factors must be added others related to the samples themselves and the analytical requirements. While for certain type of products, such as slags, it is easy to obtain a sample, there are other types, especially metal, for which the mere transportation supposes a risk and the extraction of a sample is always problematic. To each analytical method specific sampling requisites are necessary and will be set out in the corresponding sections.

One fundamental aspect for obtaining proper results from the analytical techniques is the calibration through standards or reference parameters. The quality of these calibrations is basic for obtaining appropriate quantitative results (LEUTE, 1987:154). In actual fact, as proved in practice, in many cases the theoretical capacity is limited by the design and configuration of the quantification systems.

There are cases, normally minerals, slags and other byproducts, in which the samples were taken by cutting them using a diamond disk. When possible metallographical samples have also been obtained from the metal objects in this way. The position of the extracted sample is shown in the corresponding figures of the objects.

In this project, the application of the analytical methods has been subjected to important restrictive factors. Firstly, the scarcity or lack of centres for specialised analyses on a national scale, which has meant that to carry out analyses using specific methods foreign research laboratories have had to be approached. The lead isotope analyses, for example, were done in the Isotrace Laboratory of Oxford University, in which the whole of the analytical process was completed, personally, over the period of one academic year.

With other metal objects, the metallographic study was done directly, without sampling, just by preparing a specific zone of the surface. A special case was that of the so-called “free silica slags”, which showed, on visual inspection, such a heterogeneity that it was considered convenient to carry out, in some samples, a previous treatment to give them homogeneity and a global character to the analyses (FERNANDEZ et al., 1999; 1999a).

Secondly, access to research centres with available analytical methods has always been restricted to their own lines of investigation, with the added inconvenience of their not being specialised in archaeometallurgical investigation, which meant a long period of adapting beforehand.

The analytical methods employed have been classified in three large groups, although some of those of the first two share common characteristics:

One exception has proved to be the “Proyecto Arqueometalúrgico de la Península Ibérica” (PA), centred on the XRF analyses of archaemetallurgical samples, whose members, despite having their own lines of interest, have always been prepared to collaborate.

-Methods for determining elemental composition: 1. Atomic Absorption (AA) 2. X-Ray Fluorescence (XRF) 3. Electron Microprobe Analysis (EMA) 4. Scanning Electron Microscopy (SEM) 5. Proton (or Particle) Induced X-Ray Emission (PIXE) -Methods for defining mineral phases and microstructures 1. X-Ray Diffraction (XRD) 2. Metallography -Lead Isotopes

Another restrictive factor has been the difficult access to the diverse analytical methods. Sometimes, mainly regarding elemental analyses, less appropriate methods have had to be used, as for example, destructive, when the sample was suitable, as those were the only ones to which access was 13

Mark A. Hunt Ortiz II.2.1. Methods for Determining Elemental Composition

1987:142).

In this group all the analytical methods used which provide the elemental composition (presence and proportion) of the samples have been included, together with those that, together with the elemental composition, give microscopic data or other types of details that will be specified in the individual description.

The concentration of the element is calculated later according to the concentration of the light. By repeating the process, using different sources of light appropriate to each element, it is possible to determine more than 40 elements, the majority metal (for a detailed explanation of AA, see PRICE, 1978).

The elemental analyses, which cannot be considered absolute (MONTERO, 1994:32...), only provide incomplete, although fundamental, information on the artefact being studied: exclusively the elements present and their proportion.

Due to the requisites noted, this analytical method is destructive and, as the elements have to be analysed individually, these are selected according to the problem to be investigated, which is another negative aspect of this method, since if an unforeseen element is present it would not be detected (PARKES, 1986:150). Also, it could happen that the laboratory, because of its own interests, lack the light sources, the “lamps”, corresponding to all the elements of interest for the archaeological investigation.

The elements present, according to their proportions, can be classified in three general groups (PARKES, 1986:144): Major Elements: > 2% Minor Elements: between 2% and 0.1 % Trace Elements: < 0.1 %, which is sometimes expressed in parts per million (ppm).

With this method, the presence of elements can be detected within limits ranging from 1 ppm to 100%, with a degree of confidence of between ± 1% for the major components and ± 15% for trace elements.

In any case, these limits are just for reference, and no general agreement has been reached. Thus, some authors consider Major Elements those present in proportions of >1%, Minor Elements when between 1% and 0.01%, and Trace Elements when < 0.01% (MONTERO, 1994:31).

This method is considered particularly interesting for the analysis of low atomic number elements, which cannot be easily determined by XRF. Another aspect, already mentioned, is that the results of the analysis using AA refer to the bulk of the samples.

Traditionally, to determine the elemental composition, wet techniques of chemical analyses have been used, and are still being used in certain laboratories, normally related to industry (BLANCO & ROTHENBERG, 1981), although, since some years ago, they have been substituted in most of them by physical analytical methods based on spectrometry (PARKES, 1986:144).

All the AA analyses of this project were carried out in the Laboratory of Apirsa-Boliden at Aznalcóllar mine (Sevilla). II.2.1.2. X-Ray Fluorescence (XRF) This method consists of irradiating the sample with an Xray beam produced by an X-ray tube or a radioactive source. These X-rays excite the electrons of the atomic layers K and L to higher energetic levels. The electrons return again, with the emission of secondary, fluorescent, X-rays, to the original layers.

All the elemental analytical methods used in this project are classifiable within this group. The analytical techniques by spectrometry are based on the study of the radiation emitted or absorbed by an atom when the electrons or the neutrons or protons of the nucleus move between different energetic levels. Studying the energy that is generated, it can be deduced both the type and the quantity of atoms present (LEUTE, 1987; RESPALDIZA & GOMEZ, 1997).

These fluorescent X-rays possess energies (and wavelengths) characteristic of the elements which have emitted them, so that, by measuring those waves it is possible to determine the concentration of the different elements present in the sample (PARKES, 1986:151-152). X-Ray can be used to determine elemental concentrations ranging between 10 ppm and 100 %, with a confidence of ± 2 to 5 % in the readings.

II.2.1.1. Atomic Absorption (AA) For this technique, it is necessary to obtain a sample of the object to be analysed (using a drill, for example) of a weight of between 10 mg and 1 g, according to the elements which are to be analysed and their proportion.

This technique can be carried out in a perfectly nondestructive manner, since the artefact can be analysed directly, with no previous extraction of samples. Surface irregularities, however, can complicate the calibration of the intensities, a not so serious problem when using nondispersive systems.

The sample is dissolved in an acid and diluted in a suitable proportion. The analytical procedure consists of nebulizing part of the solution and heating it with a flame sufficient to atomise the sample. The flame is lit in a chamber, with a lamp that produces a light of a determined wavelength, which can be absorbed by the element to be analysed (LEUTE,

Also, it must be taken into account that the X-ray of elements with an atomic number lower than 22 (Ti) are absorbed by the air. To analyse these elements the 14

Prehistoric Mining and Metallurgy in South West Iberian Peninsula illuminate the object, uses a beam of electrons, reaching much higher magnifications, in the region of x 50.000.

measuring must be done in a vacuum, and even under these conditions, it frequently happens that elements with an atomic number lower than 12 (Mg) cannot be properly analysed by XRF (PARKES, 1986:151-152).

SEM is a type of electron microscope adapted so that (thus its name) the electron beam can be used as a scanner over the whole of the sample surface.

Another of the limitations of the XRF method is the low penetrability of the analysis, which would only include the superficial part of the sample, with the inconveniences which this causes (e.g. variation for selective corrosion) (BUI et al., 1986:204…). This has tried to be compensated, by using PIXE, with the complementary use of other analytical techniques of greater penetration capacity (RESPALDIZA et al., 1990). In the case of the analyses carried out in the Nuclear Physics Department of the University of Sevilla, this method was used to complement the results and to improve that of some elements, especially silver (FERNANDEZ et al., 1999; 1999a).

When the primary electron beam hits the sample a series of reactions are produced, corresponding to diverse processes of excitation and de-excitation of the particles, namely: emission of secondary electrons, emission of backscattered electrons and emission of characteristic X-Rays. The detection of secondary electrons is the basic feature of this method, since the emission is more intense and, consequently, more easily detected (LEUTE, 1987:123). These signals supply information regarding the topography of the sample. The connecting up with an analyser also allows a phase study, which has been applied both to metal objects and slags (MOHEN, 1992:33), a field in which its application, for the correct interpretation of visible phases, is considered fundamental (PHOTOS & SALTER, 1986:259).

A considerable number of XRF analyses have been done by the PA (MONTERO, 1994:38-39) as well as in the Research Laboratory for Archaeology and the History of Art (RLAHA) at Oxford. Although in this latter centre the quantification systems were not quite reliable, same samples analysed by the PA and in the RLAHA, gave homogeneous results.

The backscattered electrons (BSE) also provide information on the surface topography and on the kind of atoms that provoke that backscattering (FELIU ORTEGA & MARTIN CALLEJA, 1994:232-234).

II.2.1.3. Electron Microprobe Analysis (EMA) This method also implies the detection and measuring of XRays. A high-energy beam of particles, in this case, electrons, is used to excite the electrons of the inner layers (K and L) towards layers of higher energy. These electrons emit X-rays and return to their original positions, which are, as happens with the XRF, similarly quantified.

In actual fact, SEM is closely related to the EMA. The main difference is that with SEM the backscattered electrons and the secondary electrons are the ones detected, while in the EMA it is the X-Rays that are measured (PARKES, 1986:185-186). The sample preparation requirements are the same as with the EMA and, although they may restrict the application with regard to the size of the sample, it is only limited by the capacity of the vacuum chamber (LEUTE, 1987:123, 148).

The major difference with XRF is that the beam can be focussed, so that a very minute part of the sample (1 µm2) can be analysed. In this way the characterisation of individual phases is possible with the aid of a microscope, which is also used to carry out the metallographic study (MOHEN, 1992:31). The possibility of scanning, using the beam on the surface also allows the study of the distribution of the elements.

The analyses using this method have been carried out in the Archaeometry Laboratory of the Institute of Archaeology, University College, University of London, and in the Physics Faculty, University of Sevilla.

For this method, vacuum conditions are needed and also, for the preparation of the samples, if not electrical conductive, the application of a carbon or metal coating to make them conductive (PARKES, 1986:153-154). Due to the necessity of a flat surface, the samples are normally mounted and polished, as in the case of the SEM.

II.2.1.5. Proton Induced X-Ray Emission (PIXE) With PIXE the two restrictive aspects explained regarding the analytical methods of SEM and EMA (conductivity and dispersion of electrons), are resolved by using, instead of electrons, heavier particles, with more inertia and not so easily deflected as the electrons. The mass of the protons is 200 times more than that of the electrons. With PIXE a vacuum is not needed and the samples have not to be conductors. Another advantage is that the detection limit is lower (LEUTE, 1987:148).

The analyses using this analytical method were carried out at the Department of Materials of the University of Oxford. II.2.1.4. Scanning Electron Microscope (SEM) SEM has been defined as a technique which allows the simultaneous morphological study of surfaces and the determination of its elemental composition (FELIU ORTEGA & MARTIN CALLEJA, 1994:231). It is similar to an optical microscope, with the difference that SEM, to

PIXE is, then, a multi-elemental non-destructive analytical method, which does not require any previous guessing as to which elements are present. 15

Mark A. Hunt Ortiz indicates the combination of an element as oxide, etc., but also the phase in which it is presented.

The technical procedure consists of using a Van de Graaff accelerator and electrostatic fields of millions of volts to send a beam of protons focussed on the sample, provoking the emission of X-rays. The analysis of the spectrum of the emitted X-rays allows the identification of the elements (Z >12) present in the sample and their concentration (FERNANDEZ et al., 1995). It is even possible for the sample to be scanned by the beam, producing distribution maps of the elements across the sample or to concentrate the analysis on very reduced areas (GOMEZ TUBIO, 1992:15).

The identification of these compounds is of great interest not only for the metallurgical samples (e.g. identification of litharge or specific ores) but also in the pottery connected with them, as for example, the determination of the working temperature from the presence of certain compounds only formed above concrete temperatures. The XRD analyses are usually employed using the process of powder diffraction, which is destructive. Using this process, a sample is taken and crushed into a powder. It is introduced into a chamber and illuminated by monochromatic X-rays (with just one wavelength). The crystals present act as a mirror, reflecting the X-rays, and the sample is rotated so that all the crystals are hit and reflect the X-rays.

Also, the protons of the beam, colliding with the nucleus, are backscattered and, following the principles of the Rutherford Back-Scattering Spectrometry (RBS), provide an alternative and independent method of analysis of the elements in the sample. In practice, RBS is a very good complement to PIXE since the latter is better adapted, as said before, to analysing elements in the region of sodium (Z:11) or heavier, while RBS can be used for those of less mass (GRIME et al., 1991:1-2).

The spectrum or film will pick up the reflected lines of light, lines of diffraction with values which are characteristic of the specific compounds, just as fingerprints are of human beings (ZUSSMANN, 1967:286).

One of the advantages of PIXE is that it can analyse, as a routine, the concentration of elements, with only ppm, in quite different types of samples. This high sensibility is due to the reduced background noise as compared with that produced when using electrons to induce the X-ray emissions (GRIME et al., 1991:1-2).

If there is more than one compound, the relative intensity permits an estimation of their concentration. The minimum concentration that can be detected varies between 1 to 10%, depending on the state of the crystallisation (PARKES, 1986:188-191).

In brief, the analytical characteristics of PIXE have been described as (GRIME, 1997):

The XRD analyses were carried out in two research centres: the Earth Sciences Department, University of Oxford, and the Instituto de Ciencias Materiales, C.S.I.C., of Sevilla. At Oxford the apparatus was not connected to computerised systems, and the identification of the spectrum was done “manually”, using the Diffraction Tables and the reference data (FANG & BLOSS, 1966; MINERAL POWDER DIFFRACTION FILE, 1980). In the case of the C.S.I.C., the identification is done directly through a computer program.

-Sensitive to ppm levels. -Rapid. -Multielemental, analyses all elements Z>11 (Na) and those of less mass can be analysed using RBS. -It allows quantitative analyses. Absolute concentrations can be determined without the need to use referential standards (BARRANDON, 1986:66). -Allows the spatial concentration of the analysis as well as the scanning of the sample.

II.2.2.2. Metallography Among the disadvantages of this method, its low penetration capacity has been noted, so that the analysis would only be made on the 10 µm of the surface of the sample (BARRANDON, 1986:66). For a detailed explanation of the method see KATSANOS (1986).

The metallographic analysis technique is usually applied to metal objects, although for this study it has also been applied to litharge and slag samples. Using the metallographic microscope it is possible to study the internal structure of the metal archaeological objects, deducing from the results the processes to which they were subjected during their manufacture, and, consequently, the technology employed (ROVIRA et al., 1988:9; ROVIRA, 1994:49).

The analyses by PIXE for this project, which were very restricted, have been done at the Instituto do Tecnología Nuclear do Sacavem, Lisboa (FERNANDEZ et al., 1999) and in the University of Oxford, where all the possibilities of this method are being developed (GRIME, 1997; 1997a). II.2.2. Methods Microstructures

for

Determining

Phases

Thus, the metallographic study is based on the fact that each internal structure present in a sample is related to a specific type of treatment to which it has been submitted.

and

II.2.2.1. X-Ray Diffraction (XRD)

Metallography is an analytical technique which has been applied in industry for many decades. It was developed to study the equilibrium diagrams, where it represented the

The principal use of the XRD is the identification of crystalline compounds present in the sample. It not only 16

Prehistoric Mining and Metallurgy in South West Iberian Peninsula variation of the nature and state of the phases in relation to temperature and composition of metal (in experimental conditions) (CALVO, 1971:3-5). Metallography has also been used, traditionally, in the field of Archaeology, although in the South West of the Iberian Peninsula it has not been used until recently, except in a few specific cases (GARRIDO & ORTA, 1978).

treatment.

II.2.2.2.1. Sample preparation

a) Cast structures Bearing in mind that the majority of the ancient metals are not pure or have some type of alloying, either intentional or not, the most frequent casting microstructure is the dendritic. Most of the ancient objects in the cast state present this dendritic structure, formed by “branches” which are classified as primary, secondary or tertiary. The size of the dendrites depends on the cooling rates and sometimes it is possible that they may not be well-defined (SCOTT, 1987:8).

The characteristics of the internal structures, depending on the composition of metals and the fabrication processes applied, as far as those which interest the archaeological interpretation and using the two group classification, would be the following:

Ideally, the preparation of the sample would include the extraction of a section of the object of the most interesting parts, avoiding in this way the possibility of reaching partial interpretations should there exist phenomena such as corrosion, segregation, mechanical deformation...(ALLEN et al., 1970:27). In practice, and generally speaking, efforts are made to spoil the object as little as possible, restricting the cutting of the object and preparing directly that part of its surface to be studied. In this way metallography could be practically nondestructive, since only the treatment of a small area of the surface of the object would be needed.

The dendritic structure is caused by the differentiated segregation of the components of the metal: one of the components, cooling from the liquid state, starts to solidify first (in a Cu-Sn alloy, dendrites have a higher Cu content in the internal part, while the external would be higher in Sn). This produces a segregation structure, which is characteristic, for example, of arsenical copper and bronze (SCOTT, 1987:9).

Consequently, the preparation of the sample includes the extraction of a section or the cleaning of the selected surface area. In the first case, the sample extracted is mounted on resin in order to achieve a horizontal plane. Later, and in both cases, the sample is ground and polished, using micrometric preparation.

A clear dendritic structure indicates that the object has received no treatment after casting, at least, not enough to change it (ALLEN et al., 1970:28).

The microscopic study is divided into two parts, firstly the examination of the sample in its polished state, and later, after being treated with specific chemical agents. These chemical agents are quite varied and specific for each metal and alloy. The details regarding these aspects can be obtained from any manual on metallography (e.g. CALVO, 1971), although it is better to use those specifically for archaeological metals (SCOTT, 1987; 1991).

It must be mentioned that there can be other types of segregation apart from the dendritic (SCOTT, 1987:11): -Normal segregation: in which the constituent with the lowest melting point is concentrated in the internal part of the mould. -Inverse segregation: (some times associated with alloys of Cu with As, Ag and even Sn) in which the constituent with the lowest melting point is pushed toward the outside part of the mould. This case can be seen in the sample LM48113 from Los Millares site, which showed a superficial layer of As (MORENO ONORATO et al., 1995:50, Lám. X).

II.2.2.2.2. The Internal Structure and the Fabrication Processes It has been already mentioned that the internal structure of metals is related to the fabrication processes to which it has been submitted. The possible fabrication processes of an object have been classified in three fundamental types (ROVIRA, 1994:44-45):

In very pure metals (for example Cu, Pb, Au), it could also happen that the slow cooling of the molten metal may not produce a dendritic structure but an equiaxial grain structure.

1- Those which cause a change in state: smelting and melting/casting. 2- Those which imply a mechanical deformation: plastic nature of the metals which permits a change in shape. 3- Those which imply the use of heat treatment: submitting the metal to specific high temperatures produces changes in the internal structure.

Finally, there may appear, though this is not frequent, another type of crystalline structure from casting, which is known as columnar structure, constituted by long grains which are formed by selective growth towards the interior of the mould (SCOTT, 1987:11). b) Worked Structures The crystalline structure is in a thermodynamic equilibrium while the dendritic structure is not. For this reason it is possible to obtain an equiaxial grain structure by sufficient

These processes have been joined (SCOTT, 1987:8) to form two larger groups, since the heat treatment is generally associated with the mechanical work: Cast and Worked, which would cover both mechanical deformation and heat 17

Mark A. Hunt Ortiz There exist microstructures in the metals studied, of Cu and Ag, which reflect the annealing done after cold-working. Thus, after being cold worked and annealed, the recrystallisation of the metal is produced with the formation of the so-called twin lines, straight parallel lines visible in the affected section, crossing, in part or totally, the interior of the individual grains.

annealing of the metal object which presents an original dendritic structure (SCOTT, 1987:11). The crystalline structure supposes, not only a thermodynamic equilibrium, but also causes homogeneity of the composition, which would suppose an improvement of the mechanical properties of the piece with regard to the dendritic structure. It has been suggested that from the Middle Bronze Age the swords, daggers and axes usually present recrystallised structures, from which it can be deduced a technological improvement compared with earlier periods (ROVIRA, 1994:47).

A characteristic of these twin lines formed on annealing after cold-working is that they are perfectly straight. If the object is subjected to cold-working later on, with the consequent grain deformation, this distortion will also affect the twinned grains, which would appear with their limits distorted (SCOTT, 1987:15).

An important property of metal is that it has plastic deformation when it is worked, due to the fact that the atoms can be slipped in what are defined as “slip planes”. This deformation has a limit, which is reached when the slip planes become thicker and immobile. At that point, in order to continue the deformation it is necessary for the metal to be annealed, for it to recrystallise (SCOTT, 1987:5-6), for the atoms to be “reorganised”.

With regard to metals intensively worked, there appear what is defined as slip bands or strain lines, which can be seen in some of the individual grains of the affected sample as fine parallel lines (SCOTT, 1987:15), sometimes forming a reticule.

The plastic deformation of a metal object in a solid state is an operation that can be carried out by different means: hammering, doubling, laminating...(SCOTT, 1987:12).

The strain lines can be masked by the general deformation of the grain, which is compressed in the direction of the work, while the twin lines would appear deformed (ALLEN et al., 1970:29).

If only cold-worked, the effect of the compression produced makes the metal harder but at the cost of increasing internal tensions, which causes greater fragility. Cold working is considered one of the most ancient forms of metal work, used since the Chalcolithic period (ROVIRA, 1994:47).

Another structure which could appear, and which would be evidence of severe working, is the fibrous structure formed when the grains have been mechanically flattened to such a point that a new fibrous elongated structure is produced (SCOTT, 1987:15).

Cold- working is an operation which can be detected, shown by the deformation, in different degrees, of the dendritic structure, the grains and also the inclusions.

Deformed non-metal inclusions, as well as the metal ones, and porosity are also interesting for determining the direction and amount of work carried out on the object (ALLEN et al., 1970:30).

As mentioned before, the initial structure on being coldworked reaches a point when it is too fragile to continue to be worked: if more deformation of the object is wanted, then it is necessary to anneal it, an operation which can be repeated as many times as needed.

Cold-working followed by annealing and hot-working produce essentially the same microstructure (SCOTT, 1987:15). The metallographic analyses carried out for this research project were done at the Departments of Materials of the Universities of Oxford and Sevilla and also, some of them, at the Institute of Archaeology, London University.

By means of annealing, the recrystallisation of the structure is achieved, both from the original dendritic structure and from the deformed cold-worked structure. Both the temperature of recrystallisation and the size of the final grain depend on the degree of deformation: the larger the degree, the smaller the final grain (CALVO, 1971:88). The temperature of recrystallisation goes down to considerably lower temperatures in direct relation to the amount of cold-working to which it has been submitted (SCOTT, 1991:9).

II.2.3. Lead Isotopes The analytical method known as Lead Isotopes, is quite complex with numerous factors of different kinds which must be taken into consideration. It is, also, a little known analytical method in the Iberian Peninsula and which is being applied for the first time, in an ample form, to the archaeological investigation of the South West, intending to assess now its applicability in the field of Archaeology in this particular region of the Iberian Peninsula.

Typically, the annealing temperature is between 500ºC and 800ºC, although time is an important factor: excessive time would produce negative effects in the compactness of the object connected with grain size and an insufficient time would not eliminate the unstable equilibrium and the heterogeneity of the object (SCOTT, 1987:12).

18

Prehistoric Mining and Metallurgy in South West Iberian Peninsula The other three stable lead isotopes, 206Pb, 207Pb and 208Pb, are of radiogenic origin. They are the final stable product of the radiogenic decay of the radioactive isotopes 238U, 235U and 232Th, respectively (HAMILTON, 1965:174-5; RUSSELL & FARQUHAR, 1960:2-3).

II.2.3.1. Theoretical Principles -Isotopes: Definition A stable atom of any element is composed, fundamentally, of two parts (ILLINGWORTH, 1991):

The half-life of the parental isotopes differs considerably: a) Nucleus, formed by: 1. Protons (p), with electric positive charge. 2. Neutrons (n), with no electric charge.

Parental Isotope 238 U 235 U 232 Th

Protons and neutrons concentrate the mass of the atom. b) Electrons, which: - Constitute the extranuclear part of the atom. - Have a negative electric charge, and consequently different polarity, of equal magnitude to the protons. - Their mass is practically nil. - Their number and distribution determine the chemical properties of the atom.

Half-life Stable Product 206 4.47x109 Pb 9 207 0.70x10 Pb 208 14.01x109 Pb

Thus, for example, since the formation of the Earth, only half of the 238U has decayed to 206Pb, while around 90% of the 235U has decayed to 207Pb (HAMILTON, 1965:175). The lead which today is found on Earth (or “common lead”) is a mixture of the lead which was present when the Earth was formed (or “primeval lead”) and the lead produced since then by the radioactive decay of uranium and thorium (or “radiogenic lead”).

The composition of the atom is described according to its number of protons, which is that defined as Atomic Number (Z) and the number of neutrons, which is defined as Neutronic Number (N). Both determine the Atomic Mass (A): (Z+N= A).

So, the common lead is formed by the four stable isotopes of lead, but with the characteristic, which is what defines the common lead, that it does not contain U or Th in significant amounts, through which its composition remains constant (FAURE, 1986: 309).

The element is presented thus: AChemical Symbol. In the case of lead, for example: 207Pb.

Lead is an element that is distributed in quite a large amount over the planet, appearing both of radiogenic origin or forming its own minerals, of which U and Th are excluded. So the isotopic composition of lead varies between quite wide limits, from the highly radiogenic lead of the very ancient deposits with U and Th ores, to the common lead in the lead minerals with low ratios of U/Pb and Th/Pb.

The Atomic Number, as it is always the same in each of the different elements, is not usually specified. The investigations developed in the field of Physics since the end of the 19th century, showed that there are many elements which present stable atoms with different masses, in the case of lead they are 204Pb, 206Pb, 207Pb and 208Pb. That is to say, their neutronic numbers are different. Following the equation mentioned (Z+N=A), these are respectively: 122, 124, 125 and 126.

The main common lead mineral is galena (PbS). Secondary lead minerals such as cerussite (PbCO3) or anglesite (PbSO4) have the same isotopic composition as that of the galena from which they were formed (FAURE, 1986: 309). As Faure states (1986:309), as a result of the geological evolution, with many factors which can intervene, the isotopic compositions of the lead in the rocks and in the mineral deposits show a complex range of variations that reflects their particular geological histories.

These have been named as isotopes (from the Greek ισο, equal, and τοροσ, place): atoms which have the same Atomic Number but different mass, due to the fact that their nuclei contain a different number of neutrons. As has been mentioned before, the number of protons determines the number of extranuclear electrons, and this, in turn, determines the chemical properties of the atom. The isotopes would be atoms of the same element which (FAURE, 1986:13):

-Isotopic formation of the deposits As has been already mentioned, at the formation of the mineral deposits, the common lead would be composed of the mixture of primeval lead and radiogenic lead, which would have been separated from the U and Th as a result of the different geochemical behaviour of those elements. The formation process of the deposit would have, thus, brought about a stable isotopic composition, which would reflect the moment of the formation of the deposit, and, consequently, this could have a particular position within the “lead growth curve”. This lead, thus originated, has been known as

-Have different atomic mass (A) -Have the same characteristics and chemical behaviour (PUTMAN, 1965:51-52). -Isotopic composition of terrestrial lead Of the stable lead isotopes, only the 204Pb is natural, and the quantity of this isotope has been the same since the formation of the Earth (c. 4.500 million years).

19

Mark A. Hunt Ortiz allowed the fact to be demonstrated that, in the mineral samples analysed, there existed clear differences in their lead isotope composition, and a relation was established between the proportions of 206Pb, 207Pb and 208Pb in the samples and the probable geological age of the deposition of the ore: the relative quantities of these radiogenic deposits decreased with regard to the 204Pb when the age of the mineral deposit increased.

“single-stage lead” (HAMILTON, 1965:176). One of the first theories on the evolution of lead is the model known as Holmes-Houtermans, formulated in 1946, which is based on a series of theoretical principles: a) Originally the Earth was fluid and homogeneous. b) In that moment, uranium (U) and thorium (Th) and lead (Pb) were uniformly distributed. c) The isotopic composition of the primeval lead was identical everywhere. d) Later, when the Earth became rigid, small regional differences began to occur in the isotopic proportions of U/Th with regard to Pb. e) In these regions, the proportion of U/Th with regard to Pb changed only as result of the radioactive decay of the U/Th to Pb. f) In the moment of the formation of a common lead mineral, such as galena, the lead was separated from the U and Th and its isotopic composition has remained constant ever since that moment.

The ratios that present the lowest proportions of radiogenic lead have been found on Earth in certain classes of meteorites with no U nor Th. There is unanimity on the place of origin of these meteorites within the Solar System and also their formation is considered to have occurred simultaneously to that of the Earth. Thus, the age of the meteorites is relevant to Earth (DALRYMPLE, 1991:276,401). The results of the lead isotope analyses carried out in 1955 on samples from the Canyon Diablo meteorite (Arizona, U.S.A), in the U and Th free phase troilite (FeS) (HAMILTON, 1965:216), showed the lowest lead isotopes radiogenic ratios which is accepted to be also the composition of the primeval lead (DALRYMPLE, 1991:323): 206Pb/204Pb: 9.307; 207Pb/204Pb:10.294.

The Holmes-Houtermans model, on the one hand, considers the composition of any sample of common lead to be the result of a process of “single-stage history”, and on the other, assumes that the radiogenic lead was produced by the disintegration of the U y Th in the regions of origin and that the result, primeval + radiogenic, was separated from them and incorporated into the mineral deposit as galena or some other lead ore. The isotopic composition of the lead in these ores did not change from that moment due to the absence of the parental nuclei of 238U, 235U and 232Th.

Once the original composition of lead and the half-life of the radiogenic were established, it was not difficult, based on the different evolution models, to determine, although indirectly, the age of the formation of the Earth (which was calculated as 4.57x109 years) and that of the different mineral deposits. That is to say, knowing, together with the composition of the primeval lead, the half-life of the U and Th isotopes in their decay to stable lead isotopes, it is possible to calculate the time passed since the formation of the Earth and that of a mineral deposit, by determining the quantity of radiogenic lead formed.

On the other hand, other types of mineral deposits have been detected which do not fit into the model described and which have been defined as “Anomalous Leads”, due to the unusually high content of radiogenic Pb (HAMILTON, 1965:177; RUSSELL & FARQUHAR, 1960:11) .The explanation of this proved to be incompatible with the evolution model proposed by Holmes-Houtermans (FAURE, 1986:316).

In any case, the theory is based on the consideration of the evolution of lead and the mineral deposit formation in a closed system (ROHL, 1995:5). All these investigations have given rise to a wide interest in the field of Geochronology based on the isotopic composition of the lead. This is a field of Geology that is being fully developed and that also has obvious implications for its application in Archaeology, since the data banks that are providing the geological studies are perfectly applicable to archaeological ones, as has been proved in this study on the South West Iberian Peninsula.

For the integration of the data of these anomalous deposits, new models were proposed which included new phases, adding more possible alternative sequences in the evolution of lead minerals (RUSSELL & FARQUHAR, 1960:62). In short, while most of the lead deposits are explained by simple models of evolution, other deposits have received additions of radiogenic lead, at some period of their evolution: these are the leads which are considered anomalous (RUSSELL & FARQUHAR, 1960:70).

However, although it is only mentioned and does not present any problem, it must be pointed out that the results from Geochronological research are normally presented in the ratios (MARCOUX et al., 1992:1474): 206Pb/204Pb; 207 Pb/204Pb and 208Pb/204Pb.

II.2.3.2. Lead Isotopes and Geology The use of the Lead Isotope analysis for Geochronology has been well established for some decades (HAMILTON, 1965:168...), preceding and serving as a basis for its application in the field of Archaeology.

So that, for their use in archaeological research, which conventionally used other ratios to minimise errors (as will be seen later), a conversion is needed, by a simple mathematical operation, of the ratios employed in Geology.

The advances of Mass Spectrometry from the 1930’s 20

Prehistoric Mining and Metallurgy in South West Iberian Peninsula the method to establish definitive conclusions on the origin of a given sample from a mining area (BRILL & WAMPLER, 1965:163; BEGEMANN et al., 1989:276; PERNICKA el al., 1990:278). It has been said that, apart from noting the enormous potential of the method (GALE, 1989: 498; PERNICKA el al., 1990:287), the most powerful application of lead isotope analysis is that it can establish a negative conclusion with absolute certainty (GALE & STOS-GALE, 1986:87).

II.2.3.3. Lead Isotopes and Archaeology As has been explained, the lead isotope analysis is an analytical technique which comes from the field of Geochronology, where it was well established (HAMILTON, 1965; FAURE, 1986) before being applied, in the 1960’s, to Archaeology. The results of the application of this method to Geochronology suggested that there were significant differences in the isotopic composition of the mineral deposits due to their diverse age of formation and geological evolution and that, consequently, the possibility was proposed of relating the isotopic composition of archaeological objects with the possible ore deposits exploited to obtain the mineral (BRILL & WAMPLER, 1965:155).

In consequence and strictly speaking, it should be affirmed that, should the lead isotopic composition of an object be included within the isotopic field of a particular mineral deposit, the metal of the object is “consistent” with the composition of the deposit (GALE & STOS-GALE, 1986:87; GALE, 1989:489). Contrariwise, if the isotopic composition of an object does not agree, the affirmation would be absolute: that object could not be made of mineral from this particular deposit (GALE, 1989: 489).

That is to say, the principle on which this method is based is that different orebodies can have different lead isotopic compositions (different relative proportions of the 4 stable lead isotopes 204Pb, 206Pb, 207Pb and 208Pb) and consequently, it is possible to determine the isotopic composition of an archaeological sample and study its relation with that of the ore deposits (BRILL et al., 1973:73).

Another fundamental point is the consistency of the results of the different laboratories, essential to maintain the trust in a common data bank, an aspect which has been mentioned by BEGEMANN et al. (1989:273) and also confirmed in the South West, where the isotopic compositions of the ore deposits, obtained from different laboratories, as in the case of Aznalcóllar, are homogeneous.

So, in brief, from the first moment that an attempt was made to apply this method to Archaeology, it was based on two fundamental principles (BRILL & WAMPLER, 1965):

II.2.3.3.1. Theoretical Bases -The value of the stability of the lead isotopes in their application to Archaeology

a) That leads from different deposits have different isotopic compositions. b) That such a characteristic composition of a mineral deposit continues unchangeable throughout all the processes to which the ore could be submitted. From the very beginning, the possible limitations of this method applied to Archaeology were also noted. These would be:

The lead isotope method would have no archaeological value if it were not for the fact that the original isotopic ratios of the raw material used remain constant, independently of any physical-chemical changes, natural or artificial, that the sample might suffer, such as smelting, casting, oxidation, corrosion, etc. (BRILL & WAMPLER, 1965:163).

-The mixing of lead from different origins (BRILL et al. 1973:37). -There could exist mineral deposits situated in a different geographical location with indistinguishable isotopic compositions and also, the results would always be limited by the data bank information available (PERNICKA et al., 1990:287). A weak point which has been mentioned regarding provenance studies is due to the fact that the more numerous the sources of a certain raw material, more difficulties exist to make sure that the data bank is sufficiently ample, as in the case of copper, for which it would be quite possible not to include sources, some of which could have been important in prehistoric times (CATLING, 1991:7). -There are lead deposits defined as “anomalous”, with a wide isotopic field, which can cause difficulties of interpretation although, for example, in the Mediterranean area, this type of deposit has not been detected (GALE, 1989:472).

As for natural changes, the variations produced by chemical, physical or biochemical processes are restricted to elements with reduced mass, such as S, C or O, while the lead isotopes are only subjected to a change of their ratios by radiogenesis (RUSSELL & FARQUHAR, 1960:1-2). A very important fact, as indicated, for the application of lead isotopes method, is that the lead ores only rarely contain U and Th in a sufficient concentration to alter, significantly, the isotopic composition of the lead (RUSSELL & FARQUHAR, 1960:10). With regard to artificial processes, the isotopic ratios do not change during the different transformations to which an ore is submitted (smelting, refining...) until its conversion into a final object, whether the lead be the main component or only present at trace level, as has been demonstrated empirically in different, and sometimes quite complex, processes (GALE, 1989:476-477; BEGEMANN et al., 1989:269).

Where unanimity does seem to exist is on the capacity of 21

Mark A. Hunt Ortiz galena, or else, at the other extreme, as a trace element in the diverse ore species of other metals. In any of these cases, the lead isotope ratios would be homogeneous.

-Isotopic composition of mineral deposits As has been explained, a factor that must be present for the applicability of the lead isotope method is that the individual mineral deposits have a more or less homogeneous isotopic composition, and that this composition should be distinguishable from the other mineral deposits.

The practical aspect of this circumstance in its archaeological application is that, although the lead minerals are used to determine the origin of archaeological lead objects and those of copper to determine the origin of copper objects, it is possible to use, for example, galena ores of a complex deposit to investigate the source of copper ores (ROHL, 1995: 9).

It is fundamental to know up to which point, and to what degree, a mineral deposit can be characterised within itself and individualised, according to such a characterisation, from the rest of the deposits.

This fact is particularly interesting in the case of the presence of polymetallic orebodies, in which various types of ores appear and have been exploited in ancient times, such as copper or lead/silver, a case which is frequent in the complex sulphide deposits of the South West of the Iberian Peninsula, the area which is the object of this investigation. However, it must always be borne in mind, as mentioned before, that in some, though rare, occasions much greater isotopic variations have been found in an ore deposit. This is shown in the isotopic diagrams as a line of points and in a very wide isotopic field (a wide range of isotopic ratios). These anomalous deposits can cause problems of interpretation in archaeological provenance studies.

In this sense, a transcendental aspect to remember is the fact that the isotopic composition of a deposit is determined, in the first place, by its geological age, which means that deposits of different ages would have, in principle, different isotopic compositions. But another important fact to remember is that the intervention of complex secondary factors before, during and after the formation of mineral deposits, causes the opposite not to occur necessarily (STOS-GALE & GALE, 1992:324).

There are different causes, related to the geological origin and evolution, to explain the possible isotopic heterogeneity of a mineral deposit. A deposit can have suffered movements and post-deposition chemical processes, which give them a heterogeneity shown in the wide range of isotopic ratios.

In fact, the possibility of deposits of similar geological ages having completely overlapping lead isotope compositions does not seem to occur and no distant mineral deposits, with equal or similar geological characteristics, have been detected with the same lead isotope compositions (STOSGALE, 1992: 2), and even those isotopic compositions can be quite different (GALE, 1989:471).

In a similar way, there may have occurred, during geological times, two mineral deposition in the same place or even one within the other, each of them with their own geochemical history, so that in that case the lead isotopes ratios would not be the same (ROHL, 1995:10). This seems to be the case, as will be seen later, of the Minas de Cala orebody.

With regard to internal homogeneity, it has been shown that the majority of the mineral deposits have a lead isotope composition that varies very little, independently of the type of mineral analysed or its topographical location within the orebody. In some cases the variation is ± 0.1% (Bleiberg in Austria) and normally less than ± 0.3 % (GALE & STOSGALE, 1986:87; GALE, 1989:471).

Also, the presence of the parental U and Th isotopes in deposits with lead at trace level can give abnormal lead isotope ratios. These ratios depend on the quantity of radioactive elements and are distinguished, in the case of U, generally, by a higher proportion of the isotope 206Pb and a wide range of isotopic compositions throughout the deposit. Unusual high ratios of 208Pb/204Pb indicate the presence of Th (ROHL, 1995:10).

The doubts that were expressed, at the beginning, regarding the homogeneity of isotopic ratios of different ores in the same deposit, especially of the primary sulphides and the oxidised minerals, have been disproved by different research studies, such as the ones carried out in the mines of Laurion (Greece), with a variation of 0.28%, in two Australian deposits (GALE, 1989:478) and, also, in Anatolian mines (BEGEMANN et al., 1989:274).

Mention must also be made of the fact that in the South West of the Iberian Peninsula there exist mining districts (sometimes of enormous proportions, such as the VolcanicSedimentary Complex, and integrated by a large number of deposits) in which the individual deposits present very similar geological histories.

In the South West of the Iberian Peninsula, in general, the results of the lead isotope analyses lead to the same conclusion. In Aznalcóllar mine, during this project, different types of minerals were analysed from the wall and roof of the orebody, and both primary complex sulphides located at depth and copper carbonates in the oxidised, outcropping zones of the orebody.

The establishment of the degree of possibility of individualised distinguishing of the deposits in the South West of the Iberian Peninsula was one of the objectives set when the application of the lead isotope method was

It can be deduced from these facts that lead can appear in a mineral deposit both as a main component, as in the case of 22

Prehistoric Mining and Metallurgy in South West Iberian Peninsula In past decades, many research projects have been dedicated to determine the provenance of the copper used in Prehistory using elemental analyses, with the idea of establishing chemical groups that could be related to sources. Despite the great number of analyses carried out, the results do not seem to have justified the effort, while some investigators consider that the elemental-analytical provenance projects carried out in metal products in the European Bronze Age is, perhaps, the major disaster of all contemporary studies, giving very few answers and creating enormous confusion (GALE & STOS-GALE, 1986:14).

decided upon. The results will be given later, as well as those referring to the comparison of the isotopic composition of these deposits with others from different geographical areas, both Peninsular as well as from the Mediterranean. In this sense, there are investigators who consider that the important point is to characterise, isotopically, the mining districts and not the individual deposits. In some cases, the impossibility to characterise deposits in a small regional scale has been defended, not because of a question of analytical procedure but because of an inherent property of the deposits, so that the provenance studies in that small regional scale, based only on lead isotope analysis, would be impossible (BEGEMANN et al., 1989:275).

Lead isotope composition, on the contrary, does not depend on the distribution of lead in the different phases of the sample; the heterogeneity of the sample, which is important when applying elemental analysis, is of no relevance to isotopic composition (BEGEMANN et al., 1989:269). It is known, for example, that lead has little solubility in copper and for this reason is segregated. In any case, as lead isotopes do not fractionate, even if the presence of lead is of a different proportion in different parts of the object, its isotopic composition will remain the same. For this reason, just a single analysis will provide the isotopic composition of the object (RHOL, 1995:14), an aspect which has been demonstrated experimentally (GALE, 1989:487).

That affirmation is somewhat ambiguous, since in Sardinia, an island of various mining districts, it has been possible to differentiate, apart from mining districts, the individual deposits forming the districts, assigning specific lead isotope composition of objects to specific isotopically defined deposits (GALE & STOS-GALE, 1987). On of the reasons for a negative “a priori” attitude which some investigators show is due to the view they take that the isotopic composition of a deposit depends exclusively on the geological age of genesis, without secondary factors being taken into account (N.H.GALE, personal communication).

However, not everything is negative with regard to the results of the elemental provenance projects. On the one hand, although they did not achieve the original objective (provenance through elemental composition), the analyses made served to characterise elementally the objects and, on the other hand, the application of elemental analyses, especially of certain elements, to resolve the question of provenance, is considered interesting as a help when interpreting the lead isotope results (GALE y STOSGALE, 1986:87).

For the determination of provenance it is essential to analyse sufficient samples to obtain the proper lead isotopic characterisation first, of the mineral deposits, and then, of a mining region. The quantity of samples needed will vary according to particular features, but to obtain a reliable isotopic definition of a mineral deposit a number of between 12 and 20 has been suggested. (ROLH, 1995:10). In practice, mineral deposits not properly characterised, even with just 1 or 2 samples analysed, are used in provenance studies, following the principle that to have a reference, even if not fully precise, is better than having none at all.

Even more, in certain specific cases, it has been shown that the presence of certain elements in determined proportions in the metal objects can possibly be connected with specific mineral deposits (MONTERO, 1986). The fields of application of lead isotopes analysis to Archaeology are numerous, since it can be used on all objects which contain lead in the minimum amounts which the analytical process needs.

This is the case which also occurs for the South West of the Iberian Peninsula, which has experimental characteristics, since many of the mineral deposits are only isotopically characterised by a small number of samples.

With the present methods of mass spectrometry, these minimum lead contents are so small that samples with only 0.5 µg Pb can be analysed, which would allow the analysis, for example, of minerals of copper, iron, etc. (GALE et al., 1990:189).

II.2.3.3.2. Elemental Analyses and Archaeological Nonmetallurgical Application of Lead Isotopes Analysis The invariability of isotopic ratios during the metallurgical production processes, contrasts with the difficulty caused by the determining of the origin of the metals using elemental analyses, where the elements, apart from being heterogeneously distributed in the deposits themselves, may suffer a great many variations during the processes to which the ores are submitted until transformed into usable objects (GALE, 1989:476).

That is to say, it is not only applicable to lead, but to any archaeological element which may contain it in nanogramic quantities (BEGEMANN et al., 1989:269), a fact which has allowed its application to samples of objects such as glass, glazed pottery, slags, coins and metals such as silver, copper, bronze, iron...(STOS-GALE, 1993:599) or 23

Mark A. Hunt Ortiz by-products and objects).

painter’s pigments (KEISCH, 1970:4), among others. II.2.3.3.3. Lead Isotopes Archaeometallurgy

Analysis

Applied

The efforts in collecting the samples from the mineral deposits have been concentrated on those with some kind of evidence of ancient exploitation, taking into account, also, their mineralogical characteristics for later comparison, so that, for example, only the copper based objects would be compared with copper mineral deposits which could have been exploited in prehistoric periods (GALE, 1989:489).

to

Perhaps where the application of the studies of lead isotopes has had, and still has, more importance is in the field of Archaeometallurgy (STOS-GALE, 1993: 600), which is the field in which this project on the South West of the Iberian Peninsula has applied it.

Archaeometallurgy is a discipline which covers multiple processes, with a great diversity of possibilities, some of which can affect the isotopic signature of the objects, so that it is necessary to keep this in consideration in order that the analytical results can be correctly interpreted.

A proof of the value of the method are the numerous publications on lead isotope analysis being applied to diverse metal-related archaeological problems in different geographical areas and cultural periods, as in the Eastern Mediterranean (GALE et al., 1984; GALE et al., 1985; GALE & STOS-GALE, 1986) and Central Mediterranean (GALE, 1989a), Egypt (HASSAN & HASSAN, 1981), North of Africa (FARQUHAR & VITALY, 1989), Bulgaria (GALE et al., 1991), America (JOEL et al., 1988), Great Britain (ROHL & NEEDHAM, 1998), etc.

Thus, the fact must be taken into account that, during the smelting of the metal, or during the fabrication of the object, other products containing lead may be added or mixed (furnace charges, fluxes, alloys, recycling...) which would suppose the alteration of the original mineral isotopic signature (BEGEMANN et al., 1989:269). The most important processes in which this alteration could take place are studied below, in order to try to evaluate their possible incidence, the possibility of their being detected and their correct interpretation.

In the Iberian Peninsula some steps have been taken to carry out projects, still in an embryonic stage, based on lead isotope analysis, as for instance, in the South East, within the Gatas Project (BUIKSTRA et al., 1991; STOS-GALE et al., 1999).

II.2.3.3.3.1. Extractive Metallurgy In the zone covered directly by this study, the South West of the Iberian Peninsula, only two projects have been carried out which include lead isotope analysis. They are very restricted, and centred on archaeological samples from two sites in the province of Huelva, Rio Tinto (CRADDOCK et al., 1985) and Monte Romero (KASSIANIDOU, 1992).

It seems that only native metals and some very pure mineral species do not need the use of flux for smelting and would not produce slags (CRADDOCK, 1993:326). But with the majority of ores, that do contain a large variety of additional gangue elements, it would be necessary, in order to obtain the metal, to submit the ore to a series of processes to, first of all, reduce the mineral and, secondly, to separate it from the unwanted elements. To carry out these processes it is necessary to introduce into the furnace charge other elements as well as the ore, which could cause changes in the lead isotope signature of the original ore.

Thus, with regard to the South West, on initiating this research study, the fundamental and basic aspects which would allow the application of the lead isotope method, such as the isotopic composition of the mineral deposits, were unknown.

The principal components which intervene in smelting are ore with gangue, fluxes and fuel.

For this reason, it was considered of the greatest importance, on starting the project, to experiment on the applicability of the method in the zone to be studied. To do this, levels of comparison were designed, based on the theoretical principles of the method:

The great majority of slags produced in ancient times are iron silicates (BACHMAN, 1982). Thus, to produce slag (which separates the gangue), if the gangue has a high silica content, a charge of flux of iron ore would be added, normally iron oxides such as hematite or limonite.

-Internal comparison: to determine the possibility of defining isotopically the mineral deposits. -Regional comparison: to determine the possibility of being able to distinguish deposits from the same or similar geological zones. -General comparison: to determine the possibility of being able to distinguish the isotopic signature of deposits from different geological areas, in two geographical areas: Peninsular and Mediterranean.

In this sense, in the South West of the Iberian Peninsula, an important situation occurs, and it is that, in mineral deposits there are ore-gangue combinations that are self-fluxing, exemplified by mineral deposits such as Cuchillares or Chinflón (BLANCO & ROTHENBERG, 1981:39,82). A common feature, especially among the outcropping copper deposits of the South West, with evidence of prehistoric exploitation, usually with quartz (silica oxide) as the main gangue, is the presence in their upper parts of abundant iron oxides.

Once these aspects were determined the final step would be to study the relation between the mineral deposits and the archaeometallurgical samples analysed (including minerals, 24

Prehistoric Mining and Metallurgy in South West Iberian Peninsula -Mixture of ores of different origins during smelting. -Addition of ores or metals to the copper during smelting. -Mixture of different metals to make a single casting.

Even in the minerals mixed with iron oxides of the gossanized zones of the complex sulphide deposits, in which it might appear, at first, that they are scarce, silica compounds are present in large quantities, for example in the analysed ores from the mine of Aznalcóllar.

With regard to arsenical coppers, it is important to determine if the alloying was intentional or not. If the arsenical copper were produced intentionally (GALE & STOS-GALE, 1989; BUDD, 1993), then the use of arsenical minerals of an origin different to those of copper would have altered the lead isotope composition of the copper.

In these cases it is clear that, if necessary, the flux would be taken from the same deposit, so that the isotopic signature would not be varied. Even if silica compounds were added to the charge of the furnace, because of the gangue being high in iron oxides, the isotopic composition of the metal would suffer no variations since the silica compounds do not usually contain significant quantities of lead (GALE, 1989:480).

There are authors, on the other hand, who consider that, based on the analytical data, the Cu-As alloy is due to the smelting of copper ores with arsenical content (GALE, 1989:487). This hypothesis has been defended with regard to the production of arsenical coppers in the South East of the Peninsula, both in the Chalcolithic and Argaric periods (MONTERO RUIZ, 1994:260).

An indispensable component in the furnace charge is the fuel, which normally also acts as a reducing agent. The type of fuel seems to have been limited to wood, or to charcoal, which has such a low lead content (RHOL, 1995:12) that it would not affect the isotopic composition of the ore.

Then, if the Cu-As alloying is to be considered as a product of smelting copper ores with arsenic content, the isotopic composition of the objects would only reflect the composition of the copper ores used.

Thus, in the case of the prehistoric copper production of the South West Iberian Peninsula, in principle, the metal produced would have the same isotopic composition as the ore used.

This aspect is important for the South West of the Iberian Peninsula, in which arsenical coppers have been in use during most of its recent Prehistory (a very long chronological period), when the isotopic results are being interpreted.

It will only be noted that, with regard to some metallurgical centres outside the mineralized areas, although samples came from surface collection, the elemental analyses of the copper minerals (as in La Pijotilla site), seem to indicate the use of different mineral sources (see below), although their temporal simultaneity or otherwise, is an unknown aspect. On the other hand, in the Amarguillo site, the copper ore excavated in Chalcolithic contexts would be from a single ore deposit.

From a certain moment in Prehistory, the addition of tin to copper became frequent. The most common tin ore is cassiterite, which is found in Nature in a fairly pure state. The addition of tin would, very rarely, cause the introduction of sufficient lead to alter the composition of the lead in the copper ore used. For example, a 10% Sn addition would only introduce non-significant lead quantities compared with the lead present in copper ores.

With regard to silver metallurgy, in periods when lead was not used as a collector, what has been explained would be applicable. Other very different circumstances could occur from the moment that lead is introduced in the extractive metallurgy of silver, with the possibility, already suggested for the Orientalizing period (FERNANDEZ JURADO, 1994), of the importation of foreign lead. In this case, the metal produced should be considered as an alloy as far as its isotopic composition is concerned.

For this reason, the addition of tin is not considered a factor of contamination to be taken into account with regard to the isotopic analyses (GALE, 1989; ROHL & NEEDHAM, 1998). This statement agrees with the results of the elemental analyses carried out in Peninsular samples of tin minerals (MERIDETH, 1998). Leaded bronzes is quite another matter. Leaded bronzes are considered those containing lead in proportions of more than 1%.

II.2.3.3.3.2. Alloys One circumstance, which can certainly change the isotopic signature, is the mixture of metals of different origins. This fact is considered as a serious inconvenience to the applicability of the lead isotope method, using as an example the case of bronzes, which contain high proportions of tin (Sn) mixed with copper (Cu) (CATLING, 1991:7).

In the case of bronzes with discreet Pb levels (from ppm to c. 2%), for which lead alloying is considered not intentional, the isotopic composition would reflect that of the original high lead copper ore used. In some cases, it has been shown, experimentally, that copper ores relatively rich in lead can produce high lead alloys directly, of about 4-5% Pb, and in some cases with much higher lead values (more than 20% Pb) (GALE, 1989:487). In these cases, despite the

With regard to copper, for example, different forms and degrees of mixing and alloying can be considered: 25

Mark A. Hunt Ortiz differences or similarities among the group of objects, extremely useful for interpreting the possible relations or mineral resources of supply (ROLH, 1995:18).

high lead contents, the isotopic composition would reflect, as it is the same, that of the copper source, as well. In the case of intentional alloys of copper and lead, only if the lead and the copper come from the same deposit, will the isotopic composition reflect the origin of the copper (RHOL, 1995:14). It is obvious that the isotopic composition of intentional copper leaded alloys (of, let us say, more than 8% Pb) will basically determine the origin of the added lead (GALE, 1989:487).

II.2.3.4. Analytical Procedure

The recycling of broken or used metals can produce results difficult to interpret as regards the study of the provenance of the original mineral ore.

The analytical procedure of lead isotopes requires a series of complex processes, which have been recently described (ROHL & NEEDHAM, 1998), including the sample extraction and lead separation (anodic deposition alone or together with the columnar exchange method) and preparation, the charge in the renium filaments, and the analysis through, in the case of the Isotrace Laboratory, a Solid Source Thermal Ionisation Mass Spectrometer (VG38-54) connected with the electronic and computing devices.

The melting of objects coming from different mineral sources with diverse lead isotope compositions would produce a diffuse dispersion in the isotopic compositions of the new objects.

For samples with low lead, all the sequential operations had to be carried out in clean rooms, “low lead” conditions, or ultra clean laboratories, to avoid environmental contamination.

In any case, care must be taken when interpreting the results, since groups of objects which would appear to have come from the mixture of differentiated origin metals, can belong, in actual fact, to different mineral deposits. This has been the case of the EBA objects of Troy, Troas and Yortan, firstly considered as an example of the mixture of metals from various sources (mineral deposits), especially for their distribution when plotted in the diagrams, which was similar to that which could be expected for mixed metals. A more detailed study showed that the individual compositions could be grouped in defined isotopic fields, characteristic of different mineral deposits (GALE, 1989:483-4).

II.2.3.5. Presentation of the Lead Isotope data

II.2.3.3.3.3. Recycling

In its application to Archaeology the data referring to lead isotopes, is presented, not in relative abundance but in isotopic proportions, normally in the ratios 208Pb/206Pb, 207 Pb/206Pb and 206Pb/204Pb. As has been pointed out, while the lead isotope composition in an object is homogeneous and a single analysis is representative, in a mineral deposit the analysis of various samples are necessary to obtain a good characterisation. That is, for a mineral deposit, the isotopic characterisation would be carried out through a range of ratios, which together form its isotopic field.

The question of metal recycling has already been mentioned as complicated, although there are circumstances during many phases of Prehistory, such as the metal objects deposited in funerary contexts, which have been interpreted (GALE, 1989:481-482; GALE, 1991) as proof of the absence of recycling, although it is true that the metallurgical history of those objects before passing on to form part of the grave goods is not known.

For the graphic presentation, the lead isotope data are plotted in two-dimensional bivariable graphs: 208Pb/206Pb versus 207Pb/206Pb and 206Pb/204Pb versus 207Pb/206Pb. In such a way, the variations of the four lead isotopes are represented and also the location of the sample composition in a three-dimensional space.

It is the archaeological register which must be considered in order to value the possible recycling activity of a given society, although it has been noted that the recycling economies, when they are efficient, are not easily detectable in archaeological terms (RHOL, 1995:14-15). In this sense, for the hoards of metal objects, quite usual in the Late Bronze, as is the case of that found in the Huelva estuary, several hypothetical interpretations have been proposed, which go from its consideration as a sunken boat carrying scrap metal, to its formation due to continued ritual offerings (RUIZ-GALVEZ PRIEGO, 1995). For closed archaeological groups, such as hoards and funerary offerings, the lead isotopic compositions are not only useful for provenance studies, but they may also reveal 26

Chapter III GEOLOGICAL BACKGROUND AND MINERAL RESOURCES III.1. GEOLOGICAL BACKGROUND

In general terms, the Hesperian Massif is divided (MGMA, 1985:7) into the Inner and Outer Zones. The Inner Zone includes the Astur-Leonese, Centre-Iberian and OssaMorena geological regions, with earlier materials (from Early Palaeozoic to Pre-Cambrian). The Outer Zone is formed by the Cantabrian and South Portuguese geological regions (Fig. 1), with materials of more recent date. The southern limit of the Hercynian Massif is represented, in almost all its length, by the Tertiary Depression of the Guadalquivir (VAZQUEZ GUZMAN, 1983:15-16).

Geologically, the terrains of the Iberian Peninsula are grouped into two large areas: the Eastern and the Western (Fig. 1). The, more or less, western half of the Peninsula is occupied by the Hesperian or Iberian Massif, also known as the Iberian Plateau, an area of Palaeozoic basement deformed by the Hercynian orogeny. The eastern half is occupied by Mesozoic and Tertiary sediments, which cover the Palaeozoic basement. These large geological areas are subdivided into different domains, of which only some are of interest in this work.

As mentioned, in all the geographical areas covered by this research project only the two most southern zones of the Hesperian Massif are included, the inner geological region of Ossa Morena and the outer South Portuguese.

In the zone covered by this research study, various types of geological terrains exist, of different ages, which, generally speaking, are grouped in large geotectonic blocks. These blocks are, from north to south (Fig. 2):

III.1.1.1. Ossa-Morena Zone The Ossa- Morena zone is limited to the north by the Central Iberian Zone, from which it is separated by the different individual plutons which constitute Los Pedroches Batholith and its prolongation to the NW (LME, 1996:325) as far as the sedimentary terrains of Badajoz (Fig. 3).

A. Hercynian Domain (Hesperian Massif), which is divided in the zone under consideration into: * Ossa-Morena Zone * South Portuguese Zone B. Tertiary Depression of the Guadalquivir, that separates the Hesperian Massif from the Alpine Domain (Betic Range).

The Ossa-Morena, thus named from the Portuguese Ossa and the Spanish Sierra Morena hills, is the most complex zone of the Hesperian Massif, both stratigraphically as well as tectonically and petrologically (FERNANDEZ & REQUENA, 1933:24). This is shown by its division into different domains and structural units separated by important fractures and igneous intrusions (MGMA, 1985:8). The discussion on its differences with other zones of the Hesperian Massif, its limits, internal division and its correlations still continue (QUESADA, 1990:249).

C. Alpine Domain, in which only one of its formations, the Sub-Betic, is within the geological area covered. The Guadalquivir Depression and the Alpine Domain are part of the Eastern Area. III.1.1. Hesperian Massif The Hesperian or Iberian Massif is formed, fundamentally, by ancient materials, Precambrian and Palaeozoic, which cover the western Iberian Peninsula. According to its different geological characteristics and general tectonical evolution, the Hesperian Massif has been divided into five large zones in almost parallel bands disposed in an approximately NW-SE direction.

So, although there does not seem to be general agreement on this geological area, for the explanation of the OssaMorena Zone one of the recent proposals is followed (MGMA, 1985:9-12). This specifies eight domains, all lying in a NW-SE direction and of which the first two are outside the geographical area investigated:

The Hesperian Massif constituted an area, during the whole of the Mesozoic period, with a tendency to elevation, surrounded by zones of marine sedimentation. In general it had no later cover either through lack of later sedimentation or because of surface erosion. The whole of the Massif, including mineralizations and host rocks (GARCIA PALOMERO, 1980:29), is affected by the polyphasical Hercynian orogeny and others which altered, deforming and fracturing, the ancient materiales (Precambrian and Palaeozoic) (FERNANDEZ & REQUENA, 1993:28; LME, 1993:41).

1. Obejo-Valsequillo, limited to the N by the Pedroches batholith and to the South by the Guadiato-Peñarroya carboniferous basin. 2. Valencia de las Torres-Cerro Muriano, which, to the S, reaches the Azuaga Fault. 3. Sierra Albarrana, whose southern limits reach the Malcocinado Fault, and extend from the sedimentary terrain to the S of Badajoz to the N of the city of Córdoba. 4. The Zafra-Alanis domain (also called Córdoba-Alanis) has its southern limit at the outcrop of Precambrian materials of the great Olivenza-Monesterio syncline with extensive Precambrian outcrops on its NE flank and Palaeozoic (from Early Cambrian to Devonian) in the 1 27

Mark A. Hunt Ortiz

Figure 1. Iberian Peninsula Geological Units (after Vázquez Guzmán,1983).

Figure 2. SW Iberian Peninsula Geological Domains (after Libro Blanco de la Minería,1986). 28

Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Figure 3. Ossa-Morena Geological Zone (after Locuruta et al.,1990). authors to be part of the domain which also includes the Aracena Massif (FERNANDEZ & REQUENA, 1993), while others tend to consider it as an independent domain (LOCUTURA et al., 1990). Consequently, for the explanation of the mineral resources of the zone investigated, the Barranco-Hinojales Syncline has been studied independently of the other zones of the Evora-BejaAracena domain. This zone occupies a band which, starting from the SW of Portalegre and narrowing gradually, reaches the sedimentary terrains of the Guadalquivir Basin. Geologically, it consists of Palaeozoic materials: Ordovic slates and schists, black Silurian slates and quartzite and of

centre. It appears to the S of the Badajoz sedimentary basin and is limited to the SE by the Guadalquivir basin. 5. The Olivenza-Monesterio domain includes Precambrian and early Cambrian material, and extends to the SE from the S of Badajoz to the Lora del Río area. 6. The Elvas-Cumbres Mayores domain is limited to the S by the Juromenha folding. The materials are Precambrian and Cambrian. Its limits are, also, in the form of a narrow ridge in a NW-SE direction, to the S of Badajoz, although it extends into Portugal to the W of Portalegre and, to the SE, to the Guadalquivir Basin. 7. The Barrancos-Hinojales Syncline is considered by some 29

Mark A. Hunt Ortiz

Figure 4. South Portuguese Geological Zone (after Oliveira & Oliveira,1996). southern defined by the Tertiary and Quaternary sediments of the Guadalquivir basin (Fig. 4).

a rhythmic alternation of Devonian slates and grauwacks. 8. The Sierra de Aracena domain forms part of a wider archaeological area including those of Evora-Beja in Portugal. It forms a metamorphic band situated in the southernmost part of the Ossa-Morena Zone, limited to the S by the South Portuguese Zone. This domain, although it has been studied as a whole, contains greatly differing structural units (FERNANDEZ & REQUENA, 1993:2425).

Geologically, the South Portuguese Zone is divided into bands of different characteristics, best represented in the part of this Zone in Portugal (FERNANDEZ & REQUENA, 1993:26), and for that reason the Portuguese names have been maintained, although they can be applied to the whole group (OLIVEIRA & OLIVEIRA, 1996). So, the South Portuguese Zone is divided, from S to N in (OLIVEIRA & OLIVEIRA, 1996:11-16) the following:

III.1.1.2. South Portuguese Zone The South Portuguese Zone (MGMA, 1985:12) corresponds to the southernmost outcrops of the Hesperian Massif and is formed by materials later than the Middle Devonian. The biggest difference between the Ossa-Morena Zone and the South Portuguese is, stratigraphically, that the former consists, basically, of Early Palaeozoic rocks, while in the South Portuguese Zone there are Devonian and Carboniferous rocks.

1. The Flych Group of Bajo Alentejo, with formations dating from Early to Middle Carboniferous, and which includes three main units: a) The Brejeira formation, occupying the extreme SW and consisting of the Sierras of Brejeira, Monchique and Carapinha. b) The Mira formation, with slates and grauwacks which extend in a wide band from S of the Grândola Sierra to the river Guadiana, with some little presence in the Villablanca zone of the Huelva province.

Some authors consider the northern limit of the South Portuguese Zone to be the Pulo de Lobo formation and the 30

Prehistoric Mining and Metallurgy in South West Iberian Peninsula with clays (MGMA, 1985:28).

c) The Mértola formation, predominantly grauwack, extends in a wide band to the N of the Mira Formation and to the S of the Pyritic Belt, crossing the river Guadiana and extending eastwards to the S of Valverde del Camino.

III.1.2.2. Sub-Betic Zone of the Alpine Domain The Alpine Domain, situated to the S and SE of the Guadalquivir Basin, consists of the Betic Mountain Range which forms a large structural unit extending from the coasts of Cadiz to those of Valencia, divided geologically into three main units (VAZQUEZ GUZMAN, 1983:17) of which the only one included in this study is the Sub-Betic Zone.

2. The Pyritic Belt, which constitutes the central part of the South Portuguese Zone, extends from the Caveira deposits, close to the Atlantic coast, in the Portuguese district of Grândola, to Aznalcóllar and Castillo de las Guardas, in the western part of Sevilla Province. It occupies an extension of 230 kilometres long by 30 kilometres wide (STRAUSS, 1970:18) and includes, as shall be specified later on, important pyrites and polymetallic sulphide deposits (LME, 1996:15).

The Sub-Betic Zone, or the exterior zone of the Betic Mountain Range, occupies the stretch of land from Cádiz to the SE of Jaén (Fig. 1), and consists of Triassic and Jurassic outcrops of mainly limestone and loams, with major, local intercalations of marine volcanic rocks. These materials were affected by the Alpine orogeny (MGMA, 1985:24,27).

The Pyritic Belt contains two main complexes: a) Volcanic-Sedimentary Complex of Upper Devonian and Lower Carboniferous. b) Phyllitic-Quartzitic Formation of Middle Devonian which corresponds to the substratum of the Pyritic Belt, consisting of slates and quartzites.

III.2. MINERAL RESOURCES The very large-scale exploitation of the mineral resources since the 19th century AD in specific geological zones in the south western part of the Iberian Peninsula (especially the Pyritic Belt) and the present-day economic aspect of mining and geological publications, seem to have, to a great extent, created a myth regarding the role of supplier of certain mines in prehistoric ages.

The close association in which the Volcanic-Sedimentary Complex and the Phyllitic-Quartzite Formation appear has given rise to considering both blocks as a single mineralised zone, except for the area between Valverde del Camino and Aznalcóllar, which will be treated individually.

This has happened without taking into account the possibility of the existence of nearby resources and without considering the difference between the types of ore exploited in modern times and those which were sought after and treated in Prehistory.

3. The Pulo de Lobo anticline of Middle Devonian period, formed by alternating slates and quartzites and also divided into various domains, occupying a line to the N of the Pyritic Belt, from the Portuguese town of Ferreira do Alentejo to the S of Almonester la Real, in the Huelva province.

Having briefly explained the geological background of the SW zone of the Iberian Peninsula included in the study, an important aspect of this investigation is the general quantification of the mineral resources of the extensive zone under consideration. The intention is to determine the existence or not of a possible relation of certain types of minerals with specific geological domains, or in other words, to determine the grade of spatial concentration and type of mineral resources.

III.1.2. Eastern Area The eastern part of the Iberian Peninsula is subdivided as mentioned before, in different domains, of which only those included in the geographical area covered are treated, namely, the Tertiary Basin of the Guadalquivir and the SubBetic Zone of the Alpine Domain. III.1.2.1. Tertiary Basin of the Guadalquivir

The inventory of the mineral resources is presented by following the different geological domains which are studied according to their location from E to W and from N to S (Map 1).

The Hesperian Massif and the Betic Mountain Range are separated by the Guadalquivir Basin, which contains Cenozoic material from the Tertiary and the Quaternary (MGMA, 1985:7).

The basis of this distribution does not pay detailed attention to the specific characteristics of the deposits, although, sometimes, particular mineral deposits are examined as typical examples. The data is based on the GeologicalMining Map of Andalusia (MGMA, 1985) and Extremadura (MGME, 1987), the Mining Map of Portugal (CMP, 1960) as well as Metalogenetic Maps published by the Spanish IGME (Instituto Geotecnológico y Minero) and other more specialised publications which are mentioned at certain points in the explanation.

The sediments of the Guadalquivir Basin may be grouped into two different units: The Aloctonous Unit, with sediments from the Sub-Betic accumulating to form large deposits in the subsident Miocenean basin, and the Autoctonous Zone, composed of Miocenic limestone, sandstone and conglomerates. These are covered by the marine Pliocene and Plioquaternary consisting of sands and slimes interspersed 31

Mark A. Hunt Ortiz

Map 1. Main mineral deposits in South West Iberian Peninsula. mineralization. Immediately to the W of this domain and, consequently, outside the area of study, in the AlangePueblo de la Reina-Hornachos zone, there are also Pb vein mineralizations, and some of Cu and Fe.

III.2.1. Hesperian Massif III.2.1.1. Ossa-Morena Zone The Ossa-Morena Zone is considered, globally, as containing a large number of diverse mineral deposits related to the different stages of its complex geological evolution. For example, copper lodes appear, with irregular development and associated intrusions along the whole of the Ossa-Morena zone (LOCUTURA et al., 1990:321, 327).

From N to S, lead vein mineralizations appear between Ribera del Fresno and Hornachos, and also exist in the zone between Hornachos, Llera and N of the village of Maguila. To the NE of the village of Ahillones there commences the vein mineralized area of Azuaga-Berlanga, with numerous Pb-Zn veins, sometimes associated with other types of minerals such as those of Cu and Ag. Occasionally, Cu vein mineral deposits are also to be found.

III.2.1.1.1. Sierra Albarrana Domain The Azuaga-Berlanga mineralized area is considered the most important for Pb-Zn deposits in Extremadura and was, at the beginning of the 20th century AD, the zone of highest lead production in Spain. The veins, sometimes very long although with discontinuous mineralization, are inserted in the Precambrian Azuaga formation The paragenesis consists of galena, sphalerite, pyrites with occasional

This domain has its name because it covers the Sierra Albarrana (Córdoba province). It also extends from the sedimentary terrain to the S of Badajoz, in the Ribera del Fresno area, to the N of the city of Córdoba. To the N of Puebla del Prior there is a copper

32

Prehistoric Mining and Metallurgy in South West Iberian Peninsula Passing to the province of Sevilla, there appear Fe, Ba, Cu and Pb mineralizations in the zone which extends from Guadalcanal to Malcocinado (veins of Ba and Cu in Malcocinado) and as far N as Alanis. To the W of Guadalcanal there is a Fe mineralization.

tetrahedrite, and their minerals of supergenic formation. The gangue is quartz and calcite with the occasional appearance of barite. This lode area extends E to Granja de Torrehermosa, to the SW to Valverde de Lerena and, to the SE, to Sierra de los Santos (Piconcillo). The lead mineralizations also reach to the S of Piconcillo through the eastern slope of Sierra Albarrana. In the Pb deposits of this area, sometimes, Cu appears, occasionally, in such quantities that it could be considered the main lode. This is the case of the mineral deposits to the S of Granja de Torrehermosa, to the S of Argallón (on the border of the provinces of Córdoba and Badajoz), and in the zones of Piconcillo and to the NE of Posadilla.

There are also mineralizations of Ba to the S of Alanis and of Cu, Ba, Pb and Fe (Cerro del Hierro) to the S of San Nicolás del Puerto. To the N of Cazalla de la Sierra there are two Ag mineralizations marked. To the S of the village of Navas de la Concepción Cu mineralizations appear with other types of minerals associated, which also appear, together with Fe and Ba to the W of this village. In the area between Constantina and Peñaflor, Cu, Pb and Fe deposits appear. In the zone named Peñaflor-Almenara they are predominantly of Cu, while those of Fe are concentrated to the N of Peñaflor.

To the SW of the Azuaga area, there are Pb mineralizations in the River Onza zone. To the S of Villaviciosa, in the Córdoba province, there is a large mineralized zone in which Cu orebodies predominate with some of Pb, with a wide paragenesis (Zn-Cu-Ag), which extends from the Bembezar dam to the N of the town of Córdoba.

In the central-eastern part of the Sevilla Province (MME76) mineralization is concentrated on Puebla de los Infantes, with predominant Pb (Ag) deposits, forming an area known as “Plomo de los Infantes” (PINEDO, 1963), although there are also Cu deposits.

III.2.1.1.2. Zafra-Alanís Domain

From an imaginary line, that joins the villages of Las Navas and Peñaflor, to the E, abundant mineralizations of Cu and especially Pb are to be found, together with Ba and Fe, which extend to the N of the town of Córdoba. The mineralizations of Cu and Ba are more abundant in the area between Las Navas de la Concepción and Hornachuelos, while in the Hornachuelos-Posadas- Almodovar del Rio zone there are many Pb deposits, although those of Cu, especially in the Almodovar area and to the E, are also numerous.

The Zafra-Alanis Domain (also known as Córdoba-Alanís) extends in a NW-SE band from the S of the sedimentary basin of Badajoz (Santa Marta and Villalba de los Barros) to the Guadalquivir basin. In the northern part of this Domain the mineralization is located to the N of Santa Marta, with vein type Pb-Zn mineralizations containing galena, sphalerite, pyrite and chalcopyrite and secondary minerals of iron and copper carbonates. The gangue is quartz and limestone. A stratiform Pb-Zn mineralization exists to the SW of Villafranca de los Barros.

III.2.1.1.3. Olivenza-Monesterio Domain In the northernmost part of this Domain a vein-type Fe deposit is located to the S of the village of Almendral. Another vein deposit, in this case of Cu, is located to the W of the village of La Lapa, in the NE part of the domain.

Further S there are vein mineralizations of Fe, Cu and Pb in the Feria zone as far as Medina de las Torres. To the SE of Feria there is a small series of lodes with a paragenesis consisting of chalcopyrite, pyrite and arsenical pyrite and tetrahedrite, with quartz as gangue, set in between Precambrian slates.

Further to the S (Jerez de los Caballeros) there is an important zone of iron mineralization, with mainly veintype deposits, associated with the pluton of Burguillos del Cerro. The most important iron mineralizations are of the skarn type. Mention must be made that, together with magnetite and Fe sulphides, Cu sulphides also appear, as in the case of the San Guillermo, Colmenar, Santa Justa, Monchi and La Berrona mines, the most important iron mines in the zone.

Towards the SE there is a zone of mineralization with vein deposits of mainly Ba, Cu and Pb from the N of Villagarcía de la Torre (S of Usagre) to the S of Llerena which also appear in the E, to the S of Ahillones. In this zone the Cu ores are set in the Precambrian rocks. The paragenesis consists, fundamentally, of chalcopyrite, pyrite and marcasite with abundant azurite, bornite and covelline appearing locally. The gangue is quartz with occasional barite.

Also, there are deposits, such as the La Bilbaina Mine, in which the magnetite and pyrite are accompanied by chalcopyrite, tetrahedrite, bornite and galena as accessory ores.

To the S of Valverde de Llerena there also exist lodes of Cu set in the Sotillos (Precambrian) Formation with pyrite, chalcopyrite, bornite and secondary copper carbonates, fundamentally malachite.

To the E of the Burguillos pluton, to the N of Atalaya, a Cu 33

Mark A. Hunt Ortiz minerals. The Cu content of Cala Mines reaches 0.4% (LOCUTURA et al., 1990:326).

deposit appears, and another to the E of Fuente de Cantos. In the area between the S of Fuente de Cantos and Montemolin and Monesterio vein-type deposits, both of Pb and Cu are to be found. The most northerly are those of Pb, while the Cu deposits are related, rather, with the Sierra de Tentudía Formation, especially to the E (towards Calera de León) and S. The Tentudía Cu vein deposits are set in Precambrian rocks, and contain pyrite and chalcopyrite with Cu carbonates, both malachite and azurite, as well as other secondary minerals.

Immediately to the NE of Cala there is the La Sultana-San Rafael mineralization, a zone of quartz lodes of little potential, in present geological-economic terms, but of great length, containing, fundamentally, chalcopyrite and its secondary minerals. Other minerals also appear as well as native gold (FERNANDEZ & REQUENA, 1993:52). Further E, in the Sevilla province, Fe deposits exist, some associated with Cu, as for example in the Real de la Jara zone, appearing others, containing Fe, further to the SE.

A little to the E, to the S of Montemolin, La Albuera Mine is located. The mineral deposit, also set in Precambrian rocks, is of vein-type with paragenesis of chalcopyrite, galena and sphalerite, with quartz gangue, accompanied by limestone and siderite. Common secondary Cu minerals are the carbonates (malachite and azurite).

III.2.1.1.5. Barrancos-Hinojales Syncline The zone considered to be included in the BarrancosHinojales Syncline extends, in the form of a curved band, narrower in the SE part, from near the Portuguese village of Redondo and San Benito de la Contienda in the province of Badajoz, to the Guadalquivir Basin in the Lora del Río zone.

In the Sevilla Province, bordering on that of Badajoz, several Pb-Zn (Ag) deposits appear, to the E of the Pintado dam. Immediately to the N of El Pedroso, in the Sierra of that name, massive Fe mineralizations exist, with Cu minerals appearing in the southeastern zone.

The most northerly deposits are to be found on both banks of the river Guadiana, in the Portuguese zone of Rosário and Capelins and to the N of Cheles in the Badajoz province. The most northernmost of these is near the aforementioned village of San Benito de la Contienda. In this zone vein-type deposits of both Fe and Cu appear.

In the southeastern part of the Domain, in the upper reaches of the river Guadalbarcar, there are Cu (Ni,Au) deposits and others of Pb (Zn,Ag) along its tributary, the Tamujoso stream. Finally, to the N of Villanueva del Río y Minas, there exist Fe deposits, especially along the left bank of the river Huesna.

Further S there is a Cu deposit, to the N of Villanueva del Fresno, and still further S another to the NE of Valencia de Mombuey, a zone in which, towards the E of Zahinos, there also appear Fe mineralizations.

III.2.1.1.4. Elvas-Cumbres Mayores Domain

In the area of the rivers Ardila and Múrtiga many vein-type deposits of Cu are located, and extend from Barrancos to the W and SW of Encinasola and the Sierra de la Contienda.

This Domain extends, in the zone under consideration, from the S of Badajoz as far as the NW of Villanueva del Rio y Minas. In the northernmost zone, to the N of Alconchel, a stratiform mineralization of Fe and Cu is located. Rather more to the S, to the S of Táliga, there is a Cu deposit.

Geologically, this sector is made up of schists and quartzites from the Silurian Age, cut across by numerous lodes with chalcopyrite and grey copper, apparently of little depth, which can be located by the surface outcrops of ferruginous quartz, and also gangue of barite, with spots of copper carbonates (GONZALO Y TARIN, 1878:590; DOMERGUE, 1987:226). The veins are mainly composed of Cu sulphide, together with oxides and carbonates, and most unusual, native Cu (GONZALO Y TARIN, 1878:592), creating an important mineralized zone, although today it has no economic interest (LOCUTURA et al, 1990:325).

In the Olivenza-Monesterio Domain, the Burguillos del Cerro Fe deposits were mentioned which in this domain extend to the N of Jerez de los Caballeros-Valle de Santa Ana. To the SW, in Oliva de la Frontera, there exists a mineralized zone with bismuth deposits, with which, in some cases, Cu minerals are associated. In the Higuera la Real area there are Fe mineralizations.

In the Spanish part alone, 932 mining concessions were registered, grouped in 5 large blocks, plus others not integrated in them (GONZALO Y TARIN, 1878:591-594; JUBES & CARBONELL, 1920b).

Between Cumbres Mayores and Hinojales Ba deposits appear, in some cases accompanied by some chalcopyrite and galena (LOCUTURA et al., 1990:324). The Cala Mines, located in the NE of the Huelva Province, the same as the nearby Teuler Mines, are a skarn type mineralization, with iron minerals (magnetite and pyrite) together with accessory copper pyrites and its secondary

The mineralizations are absent, according to the metallogenetic maps, as far as the Santa Olalla del Cala fault, appearing again, in the Almaden de la Plata area, as 34

Prehistoric Mining and Metallurgy in South West Iberian Peninsula to the NW, to Castillo de las Guardas-Aznalcóllar to the SE, and is closely associated with volcanic-sedimentary rocks. Geologically, the deposits which make up this metallogenetic province have a similar origin, all being considered syngenetic, volcanogenetic, exhalativesedimentary and of submarine formation (BARRIGA, 1990:370).

Cu deposits to the NE of that town and also to the SW, in the Ribera de Cala. Fe is found to the NW of Almaden de la Plata. III.2.1.1.6. Evora-Beja-Aracena Domain The zone considered to form this Domain extends from Montemor o Novo and Evora, in the NW, to Zufre in the SE.

The deposits of polymetal sulphides which appear in this domain are large lenticular masses of iron sulphide with chalcopyrite, galena and sphalerite as main components and other minerals in lesser proportions (MGMA, 1985:37), such as the precious metals, Au and Ag, and another series of metals, with contents ranging from ten to thousands of ppm, such as Sn, Cd, Co, Hg, Bi, Se, and others (BARRIGA, 1990: 369).

The northernmost mineralized zone is located precisely to the SW of Montemor o Novo and is made up of Cu veins. From this zone to the N of Viana do Alentejo there are Cu deposits in Santa Ana, to the W, and in Tourega, Alcáçovas and E of Aguiar, those located most to the E. Iron deposits also appear to the W of Santiago do Escoural.

In actual fact, there are hundreds of types of minerals inventoried in these deposits (CRAIG & VAUGHAN, 1990:1), both of primary and secondary formation (e.g., for the Lousal Mine STRAUSS, 1970:138-139).

To the S, more Fe mineralizations appear in Alvito, Cuba, to the E of Beja, Minas da Orada and in Sobral de Adiça (between Moura and Rosal de la Frontera). In this area Cu deposits are only registered to the SE of Moura, to the S of Sao Amador and to the E of Santo Aleixo.

A summary description of the principal mineralized areas of the Pyrites Belt (Fig. 4), shows that to the NW, as already mentioned, the mineral deposits appear to the S of Grândola, in the Sierra de Caveira, separated from the rest of the Belt by the Sado sedimentary basin. The Lousal deposit of complex sulphides is the most important there.

The Sierra de Aracena is a zone of diverse mineralizations, with various Fe deposits between Aroche and Cortegana, as well as to the W of La Nava, S of Jabugo, in the zone of Valdelarco, and in that of Aracena. There are also Cu deposits in the Jabugo-La Nava alignment, of which the most important is the volcanic-sedimentary deposit of María Luisa Mine, with predominantly Zn, Cu, Pb and little Ag, As and Sb (LOCUTURA et al., 1990:324).

To the S there appears, again isolated, the Cercal mineralized zone where numerous deposits, including 60 ferromanganese as well as one of Pb-Zn-Cu (STRAUSS, 1970: 24).

The Pb mineralizations are concentrated in the El RepilaoAracena alignment, with another Pb deposit appearing more to the E, in Higuera de la Sierra.

Towards the E of the Portuguese region the Pyritic Belt develops into two parallel bands: the most southerly extends from the Sado basin to Castro Verde and Neves Corvo (one of the few mines discovered recently) and also outcrops in the Alcoutim zone.

III.2.1.2. South Portuguese Zone III.2.1.2.1. Pulo de Lobo Formation

The most northern band appears in the Aljustrel zone and extends to the Santo Domingo area, reaching to the E the Spanish provinces of Huelva and Sevilla, with such important mineral masses as Tharsis, Sotiel, La Zarza, Rio Tinto and Aznalcóllar, and many others (PINEDO VARA, 1963).

This Formation constitutes a band with an almost W-E direction which goes, narrowing in that direction, from Ferreira do Alemtejo to Almonaster la Real, representing the most northern part of of the South Portuguese Zone. Of the different domains studied, this is the one that has a noticeable sterile mineralogy, with no registered mineralizations within its geographical boundaries.

Bearing in mind that the deposits of the VolcanicSedimentary Complex have very similar characteristics, Rio Tinto has been chosen to describe the mineral deposit type because it is one of the most intensively studied. The specific characteristics of other deposits, which have been exploited in prehistoric times, are set out in the appropriate chapter (Chap. IV).

III.2.1.2.2. Pyritic Belt III.2.1.2.2.1. Volcanic-Sedimentary Complex The Pyrite Belt includes more than 75 polymetal deposits, forming a metallogenetic province (BARRIGA, 1990:369; FERNANDEZ ALVAREZ, 1975:66), that is to say, a group of deposits concentrated in one particular geographical area, usually with geological affinities (ANGUITA & MORENO, 1991:201), considered to be one of the most important in Europe (STRAUSS & GRAY, 1986:304). It extends in a wide W to E band from Grândola

III.2.1.2.2.1.1. Rio Tinto Mineral Deposit The different masses which constitute the Rio Tinto mineralization (Fig. 5) are composed of, due to their genesis and geological evolution, three types of mineralized zones: 35

Mark A. Hunt Ortiz

Figure 5. Geological plan of Rio Tinto (after Baumann,1976).

Figure 6. Geological section of Filón Sur-Cerro Colorado-Filón Norte lodes, Río Tinto (after García Palomero,1990).

36

Prehistoric Mining and Metallurgy in South West Iberian Peninsula residual enrichment of the less soluble elements including Au, Ba, Pb and Sn, some of which are enriched as much as five times when compared with their contents in the massive sulphides (GARCIA PALOMERO, 1990: 26). Looking at the geological evolution of the deposits of massive sulphides which, due to erosion outcropped or remained near the surface, are those exploited since prehistoric Figure 7. Zoning of sulphide deposits (after Fernández & Requena,1992). times (only very recently have any new deposits been discovered due to -Stockwork sulphides in volcanic rocks. modern prospecting methods, such as Los Frailes and Las -Stratiform deposits of massive sulphides over stockwork. Cruces, in the province of Sevilla, or Neves Corvo in -Gossan, formed by the weathering of the outcropping Portugal), it can be seen that they suffered the effect of deposits of stockwork and massive sulphides, restricted to surface waters, producing reactions and originating a series some 70 m from the surface (GARCIA PALOMERO, of zones arranged vertically and with special characteristics, 1990:20). which are the following (according to MARTIN GONZALES, 1981:106-107) (Fig. 7): The Cerro Colorado-North Lode-South Lode deposit, located in the centre of the Rio Tinto anticline, is the most -Zone of Oxidation or Infiltration. extensive mineralization of the area. It consists of small -Secondary Enrichment Area, below the hydrostatic level, remains of massive sulphide, essentially pyrites, more or where enrichment takes place, especially of Cu. less, cupriferous (North Lode-South Lode) in connection -Primary Zone, formed by the original unaltered sulphide with an enormous iron hat (montera) of iron oxides and minerals. hydroxides, also known as “gossan” and an extensive mineralization of stockwork (GARCIA PALOMERO, In the Oxidation Zone, limited in depth by the freatic levels 1990:24) (Fig. 6). of underground waters, a series of processes take place, which bring about the alteration of the original minerals and In these deposits, practically all of the original sulphide the formation of new types (MARTIN GONZALEZ, (between 70% and 90%) has been weathered or altered by 1981:108-113). external agents, which produced the formation of the great gossan capping, which represents, to give an idea of the size The minerals of the different metals have a characteristic of these deposits, a total of between 100-150 million tons, behaviour in the Oxidation Zone: the pyrites, the most formed from some 400-500 million tons of original frequent iron ore, is transformed through chain reactions to sulphides (GARCIA PALOMERO, 1990:26). produce a whole variety of minerals, such as limonite, haematite and goethite, which are very stable and form It is worthwhile mentioning, for its possible connections together the aforementioned gossan. with prehistoric mining, that the gossan has conditions which allow it to be transported during weathering to Chalcopyrite, the main primary copper mineral of these distant locations from the mineral masses where it was deposits, after suffering weathering, is transformed into formed. This is the sedimentary gossan (or Bog-Iron) as in other types of minerals (sulphates, oxides and sulphides Alto de la Mesa (Fig. 5), which has characteristics in its such as chalcocite, bornite, etc.) which tend to concentrate composition and stratigraphy different to those of the in the secondary enrichment zone. In Rio Tinto, the gossan “in situ” (MARTIN GONZALEZ, 1981:135). chalcocite (known as “negrillo”) is the most abundant secondary Cu mineral, followed by covellite. Thus, while in The existence of gossan iron hats is one of the the oxidation zone the Cu content decreases, it increases characteristics of the outcropping masses, in which the considerably in the enrichment zone. atmospheric agents cause the oxidation of the sulphide minerals to form iron oxides and hydroxides, losing certain On the other hand, under certain conditions, the Cu elements, such as practically all the S, Zn and As, and sulphides tend to form “in situ” oxidised compounds, such partial loss of Cu and Ag. At the same time it produces a as malachite, azurite, cuprite and even native copper 37

Mark A. Hunt Ortiz A metal in the complex sulphide deposits which has now great economic importance is gold. In general, it resists dissolution and remains in the oxidation zone, in residualtype concentrations. However it does have a certain degree of mobility as can be deduced from the concentrations detected in the lower limits of the gossan (MARTINEZ GONZALEZ, 1981:122).

(MARTIN GONZALEZ, 1981:116-117). Copper carbonates appear on the surface of different massive sulphide deposits, such as Lousal and Aljustrel, and in Rio Tinto have been found in the contact rocks, especially in the most oxidised parts, although Cu carbonates are considered as a rare mineral type there.

The other noble metal present in these deposits, which also has an economic interest today, is silver. As with Pb, it is not an excessively soluble element, concentrating in the Oxidation Zone, where it is deposited, sometimes as chloride (cerargyrite) (as the small vein found in North Lode: CALDERON, 1919,I:230) and far more frequently in the form of earthy yellow-coloured accumulations of jarosites and argentojarosites (MARTINEZ GONZALEZ, 1981:124-125; PRYOR et al, 1972:A145), which have been subject to a great deal of study in the North Lode of Rio Tinto (WILLIAMS:1934).

Native Cu is also considered a curiosity in Rio Tinto (PINEDO, 1963:155), although in other mines like Monte Romero it was relatively abundant. In the case of Rio Tinto, even though Cu in the oxidation zone, in native form or as carbonates, seems to have been rare (although it is known that they appeared on the surface in Cerro Colorado (AVERY, 1974:413)), other secondary types, such as cuprite and tenorite, appear there in greater amounts (DOMERGUE, 1987:236). Sphalerite is the primary mineral bearer of Zn, which oxidises to form a sulphate. This sulphate is very soluble and travels with the surface waters away, laterally, from the Oxidation Zone without producing large concentrations in the secondary enrichment zone (MARTIN GONZALAEZ, 1981:119).

As for its formation, as mentioned before, the mineral deposits were covered, before being exploited by contemporary mining, by gossan iron hats. The thickness of the gossan varies, generally between 10 and 40 m, with an average of some 30 m. The uniformity of the gossan base is a general characteristic, it being dependent on ancient hydrostatic levels (WILLIAMS, 1934:630).

The primary mineral containing lead is galena, which reacts to form lead sulphate (anglesite). The sulphate, in its turn, reacts very slowly with the surface waters, thus allowing it to remain in the Oxidation Zone, having a marked tendency to turn into a carbonate (cerussite) with a similar degree of insolubility. Also the formation of a surface anglesite or cerussite covering on the galena stops its oxidation process and that is the reason why sometimes this sulphide is found in the Oxidation Zone, even in some concentrations (MARTIN GONZALEZ, 1981:120).

Perhaps the earliest description of this jarositic mineralization is given by Calderón, with regard to Rio Tinto, although in reference to gold, “another class of gold deposit, very different to the former, is constituted by the pyrite masses...between the limonite iron cap and the subjacent sulphides there is a small zone of one or various decimetres, in which the gold and silver content is higher, for which it is now being exploited” (CALDERON, 1910, I: 82).

Mentioned must also be made of the the presence of samples of 10-12% Pb in the walls of the altered porphyry in some areas of South Lode, North Lode and San Dionisio (DOUGLAS, 1924). The assay of a galena sample from North Lode, picked up in the Roman slag heaps, showed an Ag content of 1200 ppm (DOMERGUE, 1987:236).

In Rio Tinto this level appears as a band of up to 1.5 metres wide at the base of the gossans, frequently composed of different coloured strata: yellow, red, grey and black. The disposition of the bands was not always continuous, and could be absent in specific zones. The yellow bands have been considered predominant and on occasions appear alone (WILLIAMS, 1934:631-632; 1950:8).

Barium, an element of great interest in some aspects of ancient metallurgy, has a similar behaviour to lead. Its sulphate, barite, is not very soluble and accumulates in the Oxidation Zone, registering significative content figures there.

These zones of jarositic enrichment, formed by the alteration of massive sulphides and whose mineralogical characteristics will be studied later, would have been exposed, on some occasions, by lateral weathering of the gossan, thereby giving them easy access (DUTRIZAC et al., 1985:80) (Fig. 6), a very important fact when establishing its possible exploitation by ancient mining technologies. For Río Tinto and other mines it has been suggested, even, the existence of concentrations of jarosite on the surface or near it (ALLAN, 1968:48; DUTRIZAC et al., 1985:78).

The arsenopyrite (mispickel), the primary mineral bearing arsenic, is transformed into other species, such as Pb, Cu and Zn arseniates, some of which (although the majority being soluble are dispersed) like Pb (mimetesite) tend, because of their high stability, to concentrate in this zone. There is another series of metals which, in different compounds, are present in the oxidation zone, although in a lesser proportion, such as Sb, Sn, Bi, Co and Ni (MARTINEZ GONZALEZ, 1981:120-121).

As for the mineralogical composition, jarosite is basically an iron sulphate with the general composition XFe3 (SO4)2 (OH)6, where X could be K, Na, Ag, Pb or NH4 38

Prehistoric Mining and Metallurgy in South West Iberian Peninsula (BACHMANN, 1980:3; AMOROS et al., 1981:206). Thus, the group of jarosites includes the isomorphous plumbojarosite, natrojarosite and argentojarosite (FERNANDEZ & REQUENA, 1993:69), types which have been identified by XRD (WILLIAMS, 1950: 8). The yellow jarositic bands, together with the black ones, were those which gave the major concentration in Ag and Au (WILLIAMS, 1934: 631-632; 1950: 8). As well as in these elements, the jarositic bands were also enriched in Pb, Sb, Bi, Se and Ba and normally in silica (SALKIELD, 1970:90) and in As and Sn (JENKIN, 1902:1). On the other hand, they are characterised by their low Cu and Zn content (WILLIAMS, 1934: 632).

Tons 20 915 631 1750

Ag 1650 1787 1628 166

Au 44 36 18 35

Years 1897 to 1910

South Lode (extreme values) Tons Pb% Cu% Ag 3 0.05 118 2452 to to to 32 0.08 2531

Au 1 to 56

Years 1903-6 1908-1

Mineralogically, jarosite contains, as principal oxides, those of iron and quartz, and varying quantities of barite, cerussite and anglesite, and the only arseniate being escorodite. The silver probably appears as argentojarosite, as a sulphate and as cerargyrite (WILLIAMS, 1934:632; ALLAN, 1968:48), although more recently it has been affirmed that in these enrichment bands silver has been deposited mainly as argentojarosite (GARCIA et al., 1985:8-9), estimating that 50-70% of the Ag appears in the different types of jarosites (DURTIZAC et al., 1985:79).

Salomon Lode Pb% Cu% 0.18 28.2 0.07 3.1 2.6 0.02

Year 1893 1896 1900-4 1932

Years 1908-12

Lago Lode Tons Pb% 332 0.39 6257 0.53

Ag 1500 710

Dehesa Lode (highest values) Tons Pb% Ag 46.302 4.08 4665

Au 25 10

Au 67

Also, a shipment of various thousands of tons, analysed in 1895, contained 1.460 ppm Ag, apparently with 34% Pb and 1.22% Sn (SALKIELD, 1987:15). Other records are from 1924, when a silver concentration was detected in nº 2 and nº 3 masses of North Lode, at the point where the pyrites and the gossan met, with a thickness of between 15 and 45 cm. In the case of the nº 3 mass, the samples analysed contained about 2.800 ppm Ag and 30 ppm Au, which was extracted and exported (DOUGLAS, 1924).

This is not incompatible with the opinion of other authors who had suggested that, because of the variation in colouring, composition, and therefor, in density, it would be more adequate to call them jarositic earths, rather than jarosites, since the true jarosites would be present in small quantities (BACHMANN, 1980:3; ALLAN, 1968:50), although they consider jarosite the major fixing agent of silver in the gossan zone (ALLAN, 1968:48).

Their not very specific aspect and the interest concentrated on other types of minerals in these deposits caused the contemporary rediscovery of these enriched jarositic zones to be tardy. In Rio Tinto this did not occur until 1884, and then merely by chance. The discovery was made because of a sample of what was apparently iron oxide, “red iron “ brought from Cueva de la Mora mine to determine its iron content. It turned out that it contained 19.5% Pb and 410 ppm Ag. Immediately the circumstances of the appearance of this ore in Cueva de la Mora must have been studied, since in that same month 20 tons of ore were shipped to Swansea, containing 0.18% Cu, 33% SiO2, 1.650 ppm Ag and 44.4 ppm Au (SALKIELD, 1984:410-415).

Argentojarosites have been identified, as red and yellow earth bands of 1 m thick, above the sterile porphyry in the southern part of Cerro Salomón, with high Au contents, more than 1 oz. per ton -31.1 gr.-, and large quantities of Ag, as well as abundant barite (WILLIAMS, 1934:633). Also, these earthy layers, in which the Roman workings were concentrated, were identified between South Lode and Dehesa Opencast, in North Lode (ALLAN, 1968:48) and to a minor degree, over the sulphide deposits of Lago and Salomon.

This concentration of silver in geologically determined zones is, as mentioned, by no means a phenomenon confined exclusively to the Rio Tinto deposits. The discovery of jarosites in Cueva de la Mora mine has just been described, and doubtless it was exploited in the South and Central Lodes of Tharsis (CHECKLAND, 1967:26,50). From the archaeological work carried out in Aznalcóllar mine (Sevilla), this type of concentration has been detected in exploitations (in the gossans which still remain in the western part of the present opencast) that could be dated as Late Bronze/Phoenician Colonization period. In the case of Aznalcollar, the jarosite was identified in the mineral samples by XRD. In this mine, the jarositic levels are also characterised by their high content in Ag, Pb and Ba, and a very low Cu content (HUNT ORTIZ, 1993). In general, many of the massive complex sulphide deposits of the

It has been estimated that the volume of jarositic earths in Rio Tinto was around 1.000.000 metric tons (ALLAN, 1968:48), although other authors give the higher figure of 3.000.000 tons (DUTRIZAC et al., 1985:78), of which perhaps some 2.000.000 were exploited by the Romans (SALKIELD, 1987:13). From the archives of The Rio Tinto Co. Ltd., partial information of the quantities and composition of this mineral extracted from the different orebodies during the contemporary period is known (SALKIELD, 1984:410415) (Au and Ag in ppm):

39

Mark A. Hunt Ortiz Pb and 0.08% Ag. The mine known as Santa Isabel gave figures of 10% Zn, 4.5% Cu, traces of Pb and 0.012% Ag. However another sample from a nearby place gave 49% As, 1.3% Co and only traces of Cu. A sample from the orebody of the Colón mine gave 49% Cu and 0.11% Ag (GONZALO Y TARIN, 1878:600-2).

Pyritic Belt had mineralogical and geological conditions, which would have produced in them the zoning of jarositic enrichment (HUNT ORTIZ, 1993). III.2.1.2.2.2. Phyllitic-Quartzitic Formation In the Phyllitic-Quartzitic Formation many veins of hydrothermal origin appear, with varying thicknesses, depths and lengths, which have been associated with the Variscan orogeny (STRAUSS, 1970:223).

Thus, the complexity of these mineralizations is clear, and in them, from the analytical results given and as will be explained later, the possibility of the treatment of other metals, as well as Cu can be studied, as for example, the case of Ag.

The paragenesis is of a different type, with veins of chalcopyrite, as the one exploited in la Juliana Mine, to the NE of Aljustrel (OLIVEIRA & OLIVEIRA, 1996:21-22), and of Pb, Zn and others sulphides.

It must be mentioned that to the S of the river Corumbel, in contact with the Tertiary agricultural land, there is a mineralized zone of somewhat different characteristics. It covers, from E to W, the districts of Paterna, Villalba and Palma del Condado, and its difference consists in the predominance of galena, more or less, argentiferous, and blenda (sphalerite) deposits. The orebodies consist of small isolated discontinuous vein-type masses of variable composition, following the strike of the slate rocks, almost E-W (GONZALO Y TARIN, 1878:608).

As mentioned before, this formation is inserted within the Pyritic Belt, so it has not been differentiated except in the East of Valverde-West of Aznalcóllar zone, in which it appears alone. In this area, divided by the river Tinto, which flows from N to S, extensive vein-type mineralizations of hydrothermal origin are located in the Rite and Tejada Sierras.

In this zone, as well, there are vein type chalcopyrite mineralizations in which other different mineral specimens of secondary formation appear (FERNANDEZ & REQUENA, 1993:52).

In the Tejada Sierra, as in that of Rite, the veins are of copper: oxidised carbonates in the upper parts of the orebodies and sulphides at depth, while the gangue is quartz (GONZALO Y TARIN, 1878:240).

To the E of the Pyritic Belt, there are mineralizations of different species in terrains predominantly composed of igneous rocks, as those of the Pb orebodies of Pero Amigo and the Minilla dam, a zone in which some Fe deposits also appear.

In the Rite Sierra, to the W of the river Tinto, there are different deposits, among which the most notable are La Ratera, Segunderalejo and, 6oo metres to the E, the San Fernando group of mines (GONZALO Y TARIN, 1878:597-598). More to the N, near the village of El Pozuelo, the Chinflón mine is located, with quartz outcrops set in slate. The mineralization is principally chalcopyrite, with associated secondary minerals: Fe oxides and Cu carbonates (PINEDO VARA, 1963:488-489).

III.2.1.2.3. Bajo Alentejo Flych Group III.2.1.2.3.1. Mértola Formation The geological zone of the Mértola Formation is situated to the S of the Pyritic Belt. It extends from the Sado basin, to the NW, to the Valverde del Camino area, in the province of Huelva. Its southern limit is, in the Portuguese sector, the Mira Formation, and in the Spanish, the Guadalquivir depression. In this area various Cu mineral deposits are registered, such as those situated to the SE of Castro Verde, to the N of Martin Longo and to the S of Alcoutim, as well as various deposits between the rivers Foupana and Oleite.

In the Tejada Sierra, there have been a great number of mining concessions. A total of 325 have been catalogued according to historical documents referring to the second half of the 19th century and to the early 20th century AD (FERNANDEZ & GARCIA, 1988:24). These concessions have been grouped in 8 mineralized zones, which extend from the river Corumbel to the S, to near Berrocal to the N. From E to W it extends from the river Tinto to the Sevilla province.

III.2.1.2.3.2. Mira Formation As mentioned in general terms, the vein-type mineralisation consists of Fe and Cu oxides, together with carbonates in the upper levels of the orebodies, which are replaced by sulphides, sometimes argentiferous, from a certain depth, although the secondary minerals do not disappear, and also, are sometimes, accompanied by Pb and Zn sulphides.

This formation appears in the Algarve, occupying a range that extends from the Sierra de Mu ou Caldeirao to the NW, as far as Villablanca to the SE. It extends a little to the N, in the western part, beyond the Sierra de Cercal as far as the Sierra de Grândola.

Old analyses of different samples from different lodes indicate the existence of complex minerals at depth. The most southern lodes gave figures of 10% Cu, 20%Pb and 0.14%Ag and a lode next to La Tallisca gave 14% Cu, 14%

The mineralizations are not very abundant. There is one of Cu in the extreme NW, located to the S of Santiago do Cacem. More to the SE there is another of Cu, to the S of Garvao and, also, those of Cu in the zone of Alte, to the S, 40

Prehistoric Mining and Metallurgy in South West Iberian Peninsula centred exclusively on the Morón de la Frontera district, has shown that there definitely do exist some possibilities of mineral exploitation, far more than those which could be deduced from the information shown on the maps mentioned.

and Cachopo to the N. III.2.1.2.3.3. Bejeira Formation In this formation, located in the SW corner of Portugal, there are Cu mineralizations to the E of Aljezur.

Historical documents, studied by D. Pablo Morilla, showed the existence of Cu and Ag mines in Cerro de la Jereza, Cerro del Calvario, Sierra de la Encarnación and Sierra de Ayta (MIÑANO, 1826:110), this last one in the Montellano district.

III.2.2. Eastern Area III.2.2.1. Guadalquivir Depression The Guadalquivir Tertiary Depression can be considered, minerallogically, as a sterile zone with the exception of the detrital tertiary and alluvial deposits containing Au, which are located on the northern border, between Lora del Rio and Almodóvar del Rio. Some attention was given in the 19th century AD to the auriferuous deposits of this zone, especially to those in the Sierra de Peñaflor area (NOGUES, 1885).

Finally, in the zone of the town of Badolatosa, in the area known as Patudo, the existence of Pb and Cu mines is also mentioned (MADOZ, 1845-1850:47). III.2.3. Synopsis of Silver Mineral Resources in the South West Iberian Pensinsula The ubiquity of Cu mineral resources makes no further consideration necessary. Whereas it is certainly necessary to collect the information referring to silver ores and their characteristics to achieve a general vision of its potentiality as regards ancient mining and metallurgy.

III.2.2.2. Alpine Domain Of this Domain, which occupies the area S of the Guadalquivir Depression, only the most northern part, located in the SE of the Sevilla province, has been studied. This zone corresponds to the edges of the Betic Range, known as the Sub-Betic Zone.

The silver minerals have been put into three large groups, all represented in the mineralizations in the South West of the Iberian Peninsula: A. Native silver and silver ores; B. Lead-silver ores; C. Jarosites.

To the S of the river Guadalquivir there are Tertiary and Quaternary terrains which reach, in an almost continuous form, to the line formed by the villages of Coronil-Puebla de Cazalla-Osuna-Badolatosa (MME,82). South of this imaginary line there are the pre-Betic and sub-Betic terrains in which outcroppings of secondary rocks from the Triassic, Jurassic and Cretaceous periods appear.

A. Native silver and silver ores The silver, although not frequently, does appear in its native state, normally in fine veins or dendrites which would necessitate melting for it to be made into an object (GOWLAND, 1912:262; 1920:121; AITCHINSON, 1960,I:45). Exceptionally, native silver appears as nodules, rarely of great size, although sometimes extraordinary samples have been found, such as in a mine in Saxony “so big that it was possible to make a table without further working” (BIRINGUCCIO, 1966:45) and in the Kongsberg Mines in Norway (GOWLAND, 1920:121).

In the chart of the Metallogenetic Map covering the SW part of the Sevilla province (MME, 80-81) there exists only one register (nº 3) of pyrites, surely from a bore, in the middle of the Quaternary alluvial terrains, to the S of La Puebla del Rio. On the chart covering the central-eastern part of the province (MME,76), to the S of the river Guadalquivir, from Peñaflor to Cantillana, with Quaternary terrains apart from some outcropping of the Triassic on the SE border, only one indication (nº 211) of Fe is registered, in El Rubio.

It must be mentioned that in both cases the native silver was mined in underground workings. This circumstance is due to the fact that silver, in its metal state, resists corrosive agents well, except for some such as chlorides which are common, especially in the form of sodium chloride (NaCl) in rain water (GOWLAND, 1920:123-4; 1977:78). For this reason, most of the silver on the surface is converted, more or less rapidly, into its chloride form (AgCl), which means that the native silver would appear, fundamentally, below the hydrostatic level (GOWLAND, 1920:121; TYLECOTE, 1987:87) beyond the reach of primitive man.

In the chart covering the most eastern part of the Sevilla province (MME,82) 12 Fe deposits are registered (nº 1-12). Of these, 5 are in the Morón de la Frontera district (nº 5-9) and 3 in the Los Corrales district (nº 10-12), in all cases in Triassic terrains. So, using the information from the Metallogenetic Maps, the whole southern part, to the S of the river Guadalquivir, could be discarded, as a possible catchment zone of mineral resources in prehistoric times.

Native silver is generally 99% pure, with the principal residue being mercury Hg (PATTERSON, 1971:301). However it appears that in its pure state it is not so frequent, and normally appears associated with other minerals, such

However, a closer study of the zone, which has been 41

Mark A. Hunt Ortiz as cerargyrite.

(CALDERON, 1910,I:175).

Cerargyrite, silver chloride (AgCl) also called horned silver, is, in fact, a common inclusion in native silver. This mineral appears with a soft streaky texture, thick and metal grey in colour. So, it would not be unusual for it to be confused, due to its frequent association and apparent similarity, with the spongy type of native silver (PATTERSON, 1971:303305).

High proportions of Ag content can also be found in the Pb mineralizations S of Badajoz and Córdoba. Cerussite (CO3Pb) is relatively abundant, appearing in the Pb sulphide deposits, especially in their upper parts (TYLECOTE, 1986:54). In many occasions it is argentiferous, as in Linares and Cazalla de la Sierra (CALDERON, 1910, II:102); the general rule being that the silver content in lead ores is higher in the upper levels of the deposits.

Cerargyrite is a mineral which is fairly abundant, appearing in many argentiferous mines as a secondary product, especially in the upper levels of the orebodies (CALDERON, 1910, I:401). When it is pure, it has up to 75% silver (DANA, 1853:323), but normally it appears mixed with the Pb minerals, cerussite, anglesite and contunnite (PbCl2). In the analyses which have been carried out on different samples of native silver, some amounts of Pb appear, of between 3% Pb) and Ag (101150 ppm Ag). Some samples also had a very high Cu content (PH112: 2.16% Cu and PH138: 1.3% Cu).

*Cerro del Calvario Mine (UTM:30STG815105) Municipality of Morón de la Frontera (LOPEZ, 1989:123; MADOZ, 1845-50:115). No mining activity was detected.

Sample PH138 had a more compact character, and over 60 analyses were carried out on this type of slag, containing different proportions of Cu and Fe in a metal state: 91% of these slags had a metallic Cu content of 1.3%, 9.2% metallic Fe, 36.9% silica, 5.4% Pb and 150 ppm Ag.

*El Patudo Mine (UTM:30SUG503278) Municipality of Badolatosa (MADOZ, 1845-50:47). Cu. Contemporary workings.

The authors considered the presence of metallic Cu and Fe of great metallurgical interest. In any case, their conclusion is that the metal produced was silver (BLANCO & ROTHENBERG, 1981:94).

IV.1.2. Catalogue of the Mineral Deposits with Evidence of Prehistoric Exploitation in the South West Iberian Peninsula In this section a catalogue of the mineralizations of which there is evidence of prehistoric exploitation, both of the areas surveyed (which, as they have already been described will only be mentioned), as well as other zones, covering geographically the provinces of Huelva and Sevilla, the western area of Córdoba province, the southern part of Badajoz and southern Portugal is presented.

XRF One of these slags, classified mistakenly as “free silica”, from Sierrecilla was analysed using XRF (PA). The sample (PA7551) showed Cu leaching and fragments of quartz only partially smelted. The result of the analysis (in which the presence of Ba was also detected) was the following (in %): PA7551

Fe 11.89

Cu 12.78

To make the chapter clearer, the listing is by provinces (or districts in Portugal) and municipalities (both in Spain and Portugal). All the mines have been numbered, and this is the denomination with which they appear in Map 3.

Zn Sb Pb 3.15 1.54 69.9

111

Mark A. Hunt Ortiz

Map 3. Mines with evidence of prehistoric exploitation in South West Iberian Peninsula (numbered relation in Chap. IV.1.2). -Mines in the province of Huelva

(DOMERGUE, 1987:195).

Municipality: Almonaster la Real

The mining hammers in the orebody, some of which seem to have been found in gossan dumps, have been related with the expansion of Ag mining in the Orientalizing period (PEREZ MACIAS, 1995:436).

Name: Cueva de la Mora Mine (1) (UTM:29SPB936839) a) Name and Location Cueva de la Mora mine is on the outskirts of the village of that name.

d) Evidence of Metallurgy There are slags, probably from the Roman period (GONZALO Y TARIN, 1887:442) which have been classified for their composition as both Ag and Cu slags (SALKIELD, 1970:88).

b) Mineralization It outcropped as a gossan cap, 400 m long and 30 m wide, which was removed when its exploitation by opencast was initiated (DOMERGUE, 1987:195). The mineralization consists of complex sulphides with average Cu content of about 1% Cu, and sulphides of Pb, Zn, Cu and As (PINEDO, 1963:294), especially in the edges of the mass (RAMBAUD, 1969:152). In this orebody concentrations of argentojarosite have also been detected (SALKIELD, 1984:410).

Municipality: Almonaster la Real Name: Monte Romero (2) (UTM:29SPB947838) a) Name and Location The Monte Romero Mine is located to the E of Cueva de la Mora.

c) Evidence of Mining b) Mineralization The mineralization had numerous narrow shafts and ancient excavations. The clearest evidence is the appearance, quite early on, of grooved hammers of porphyritic rock, some of which were exposed in the Madrid Exhibition of 1885

It is a very irregular mine but with a high production of Cu ores and with concentrations of complex pyrites. In the composition, too, it has been considered heterogeneous. In 112

Prehistoric Mining and Metallurgy in South West Iberian Peninsula some zones native bismuth has been found. In the upper levels considerable amounts of native Cu were found in a quartzitic matrix (RAMBAUD, 1969:152-153), in such a way that it was once considered the main ore, followed by Cu carbonates and chalcopyrite (GONZALO Y TARIN, 1887:596). Up to 5 lodes have been recognised in which chalcocite, chalcopyrite, Cu carbonates and a certain amount of native Cu appeared, and part of the mineral containing Zn blende (sphalerite) and galena (PINEDO, 1963:404) The most recent publications consider the Monte Romero orebody as one more of the 75 masses of polymetallic sulphides of the Pyrite Belt, situated, geologically, on the northern flank of the Riotinto syncline, in the volcanic intermediary formation between the Devonian and the Carboniferous (FERNANDEZ ALVAREZ, 1975:66,79). The orebody would consist of two lenticular masses of FeCu pyrite whose ends extend into blende and galena mineralizations. Primary minerals detected are pyrite, chalcopyrite, blende, galena, freibergite, tetrahedrite, tenantite, native Cu, bournonite and mispickel (arsenopyrite). Secondary minerals are chalcocite, covellite, melanterite, azurite, malachite, haematite, goethite, limonite, cuprite, cerussite and anglesite.

Figure 82. Grooved stone hammer from Monte Romero mine.

Some of the results of the analyses carried out on samples from different parts of the interior of the mine gave the following results, in % (Ag in ppm) (FERNANDEZ ALVAREZ, 1975:82): Sample S Fe Cu Zn Pb As Ag ppm SiO2 Cd

2 37.4 24.6 1.4 17.6 7.4 0.4 147 6.7 0.1

4 29.5 3 1.4 32.9 17.9 0.7 286 13.1 0.1

5 24 8.3 1.3 25.1 7. 2 0.6 642 23.9 0.1

d) Evidence of Metallurgy Despite what has been expressed regarding the possible relation of the hammers with the exploitation of native Cu and Cu carbonates, the only evidence of metallurgical activity that has been detected is in the nearby metallurgical site of Monte Romero, related to the extraction of Ag-Cu from complex ores (BLANCO & ROTHENBERG, 1981; ROTHENBERG et al., 1986; KASSIANIDOU et al., 1995) and dated to the second half of the 7th and beginning of the 6th century BC (PEREZ, 1991).

6 27 5.1 2.2 31.6 21.6 0.5 835 10.3 0.1

The metallurgical samples were subjected to a detailed study (KASSIANIDOU, 1992), which included the lead isotope analysis of numerous samples of different natures, connected, fundamentally, with silver metallurgy.

Sb also has been detected in the complex ores (0.65% Sb in one sample) (PINEDO, 1963:406), but no Ba is mentioned. c) Evidence of Mining

Of those samples, only three are ores (M21, M85, M140), supposed to come from the nearby mine of Monte Romero. The general homogeneity of the results permitted the proposal of the exclusive use of the ores from that mine. In that way, all the metallurgical remains of the excavation have been used for the isotopic characterisation of the mineral deposit of Monte Romero.

Since the 19th century AD, Monte Romero mine has been considered one of the first to be exploited, relating this to the existence of native Cu and Cu ores in the deposit. Already in 1879, when clearing up ancient workings, various hammers of porphyric rock, with a central groove, were found (GONZALO Y TARIN, 1887:19), one of which was preserved in the defunct old Museun of Natural Sciences of Sevilla University (MCNUS) (Fig. 82) and another in the Museo Arqueológico Nacional, in Madrid (DOMERGUE, 1987:195-196). This type of lithic mining instruments were also found at the entrance to the exploitation, where more than 40 of them were collected “in a short time and with no effort” (BLAZQUEZ, 1923:37,fig.; SERRA I RAFOLS, 1924:160).

The isotopic results used from Monte Romero, which are marked with the letter M in the isotopic graphs, are the following:

113

Mark A. Hunt Ortiz MONTE ROMERO (M) (after KASSIANIDOU, 1992) Pb 208/206

Pb 207/206

Pb 206/204

MR-21

2.09735

0.85794

18.224

MR-85

2.09688

0.85770

18.267

MR-140

2.09988

0.85810

18.230

MR-10

2.10023

0.85885

18.208

MR-29

2.10161

0.85849

18.251

MR-53

2.09911

0.85829

18.233

MR-101

2.09924

0.86033

18.233

MR-5

2.09828

0.85814

18.213

MR-129c

2.09857

0.85794

18.226

Figure 83. Grooved stone hammer from San Miguel mine.

Municipality: Almonaster la Real. Name: San Miguel Mine (3) (UTM: 29SPB983819)

Municipality: Almonaster la Real Name: San Platón Mine (4) (UTM: 29SQB048823)

a) Name and Location San Miguel Mine is situated some 5 km. to the E-SE of Cueva de la Mora, on the left bank of the river Escalada.

a) Name and Location San Platón Mine (also called Era del Soldado Mine) is on the right bank of the river Odiel.

b) Mineralization This complex sulphide deposit has an E-W orientation, 700 m long, in a form of discontinuous pockets. One of its characteristics was the large size of its gossan cap (MESEGUER et al., 1945:53), removed when opencast operations were started. The presence of concentrates of secondary Cu ore was considerable in the cementation zone (GONZALO Y TARIN, 1887:441; RAMBAUD, 1969:148). Chalcosite and chalcopyrite were exploited at the end of the 19th century AD in this upper zone of the orebody (DOMERGUE, 1987:196). Veins of very rich complex ores have been detected as well (PINEDO, 1963:304).

b) Mineralization Two lodes are mentioned: the northernmost, with a length of 500 m and the other, divided by the river Odiel, 170 m long on one bank and 250 on the other (MESEGUER et al., 1945:52), with small gossan caps which disappeared during the opencast operations. In the orebody two main types of mineralization have been described: one of pyrites with higher than average Cu content for this type of deposit, and the other of complex ores with the following grades (PINEDO, 1963:419): 6.3% Cu, 14% Zn, 2.8% Pb, 30% S, 0.23% As, 2.5ppm Au and 60ppm Ag.

c) Evidence of Mining There are references to Roman shafts (PINEDO, 1963:305). The ancient workings were concentrated mainly in the gossan cap.

Lead isotopes From this mine there is only one result of lead isotope analysis, from a sample of complex ore:

In this mine grooved stone hammers have been found, one of which, of diabase, was kept in Sevilla University, in the MCNUS (Fig. 83).

SAN PLATÓN MINE (SP) (after MARCOUX et al, 1992)

d) Evidence of Metallurgy The only evidence of metallurgy consists of slag heaps, in which Roman coins have been found (DOMERGUE, 1987:196).

SP6

114

Pb 208/206

Pb 207/206

Pb 206/204

2.09797

0.85820

18.188

Prehistoric Mining and Metallurgy in South West Iberian Peninsula c) Evidence of Mining

explain the slag with high Cu and Ag contents.

As far as the base of the gossan cap, recent mining operations cut through ancient galleries of small dimensions, some following veins of chalcocite (DOMERGUE, 1987:196), probably of Roman times (PINEDO, 1963:418).

Municipality: Almonaster la Real

Grooved stone mining hammers have been found, which have been related to the exploitation of Ag ores in the Orientalizing period (PEREZ MACIAS, 1995:436), although later they were associated with Middle Bronze Age mining of Ag ores (PEREZ MACIAS, 1996:66,72,fig.18).

Concepción Mine is to the N of San Platón mine.

Name: Concepción Mine (4A) a) Name and Location

b) Mineralization The mineral deposit, 400 m long and 20 m wide was set in porphyric rocks to the S and schist to the N, and almost vertical, with an E-W orientation. The outcropping consisted of a shallow iron hat, today disappeared due to exploitation by opencast mining. Mineralogically it was classified as variable in its qualities, with very erratic Cu contents, as well as some Pb and Zn, and very low in As (PINEDO, 1963:307-310; RAMBAUD, 1969:150).

d) Evidence of Metallurgy In a surface survey, an area was detected that was classified as a small metallurgical site, with small Cu slags, undefined hand-made pottery together with stone tools, which were dated to late Copper Age, early Bronze Age. Thus, this mine was considered as having produced one of the earliest evidence of Cu mining (PEREZ MACIAS, 1995:425). But the results of the analysis of that slag caused them to be considered from Ag smelting. This led to the interpretation of the mentioned finds, together with other discoveries, as evidence of the exploitation of argentiferous ores for the production of Ag in the Middle Bronze Age. The finds, dated to that moment, and completing the explanation already mentioned, consisted of a fragment of a grooved stone hammer, a flint lamina of trapezoidal section and hand-made pottery.

Lead Isotopes There is only one result, from a sample of complex mineral: CONCEPCIÓN MINE (CO) (after MARCOUX et al., 1992)

CO 1

Slag A 34.45 26.16 2.78 1.45 105

Slag SL 30.40 19.44 1.02 0.10 16

Pb 207/206

Pb 206/204

2.10035

0.85871

18.176

c) Evidence of Mining

These elements were accompanied by two types of slag and some ore: small nodules of porous slag (Slag A), fragments of gossan, and some fragments of “free silica” slag (Slag SL). The analyses carried out gave the following results, in % (Ag in ppm) (PEREZ MACIAS, 1996:72): Sample Si Fe Cu Pb Ag ppm

Pb 208/206

Remains of workings, defined as Roman, such as shafts (some cleaned up in the 19th century AD) and drainage galleries, have been mentioned (GONZALO Y TARIN, 1887:429,432).

Gossan 15.67 41.51 0.16 0.88 42

There are also unspecified references to its exploitation in earlier periods, Tartessian (PINEDO, 1963:306) or preRoman (DOMERGUE, 1987). d) Evidence of Metallurgy

From the results of the analyses it is difficult to consider this gossan as the ore treated to produce the slag. The two types of slag are considered by-products of processes of Ag production, although in one of the cases, that of “free silica”, its classification as a Cu slag is mentioned (PEREZ MACIAS, 1996:72).

Considerable slag heaps, probably Roman, were found in the surroundings of the mine (GONZALO Y TARIN, 1887:429,432). Municipality: Alosno Name: Cabezo Hueca Mine (5) (UTM:29SPB696625)

The compositions of the “free silica” type of slag will be commented on later and its general characterisitics described, as well as the possible confusion with other types of slags.

Municipality: Alosno. Name: El Lagunazo Mine (6) (UTM:29SPB619664)

As the very person who made the discovery suggested, a major investigation of this site is necessary (PEREZ MACIAS, 1996:66). In any case, the existence of complex ores similar to those of Monte Romero, could very well

a) Name and Location Lagunazo Mine is situated some 8 km. to the N of Tharsis 115

Mark A. Hunt Ortiz 1) North Lode: 800 m long and 30 to 80 m wide. The gossan cap which covered it disappeared due to the opencast operation.

(Fig. 77). b) Mineralization

2) Sierra Bullones: 500 m long and 20 m wide. The gossan cap was also removed by contemporary opencast mining. This deposit continues to the W with that of Poca Pringue Lode, 250 m long and between 30 to 40 m wide.

This mineralization consists of a complex sulphide deposit with a NW-SE direction and very elongated form, which was visible on the surface through a gossan cap, 500 m long, 25 to 30 m deep and variable in width. In the N zone there were also veins with abundant Zn blende and galena, especially in the central part of the mass, with average grades of 15% Zn and 6% Pb, as well as appreciable contents of silver (160 ppm Ag) (GONZALO Y TARIN, 1887:525).

3) Centre Lode: 300 m long by 40 m wide. Exploited by opencast, the gossan cap was also removed. This lode continued to the E by the Silillos Lode, whose surface showed a gossan cap but beneath which there was no sulphide deposit.

Also, there were zones of concentration of Cu ores, with veins of chalcocite and even arborescent native copper in the roof of the deposit, near the schists (DOMERGUE, 1987:198).

4) South Lode: Covered by an enormous gossan cap with appreciable quantities of Ag and Au, its size caused the assumption of the existence underneath of a large pyrite mineralization despite the fact that the 580 m long Sabina prospection gallery, excavated in the 19th century AD, cut no orebody whatever. Recently, between 1967 and 1971 a relatively small lenticular lode, discovered above that gallery, was exploited by an opencast, removing part of the gossan cap.

c) Evidence of Mining A considerable number of Roman workings have been reported, the most remarkable an adit 800 m long “provided with light shafts”, and the remains of a wooden water wheel, while mention was also made of a possible “Phoenician” exploitation (GONZALO Y TARIN, 1887:518,525; DOMERGUE, 1987:198). However, regarding the prehistoric exploitation of this mine what is known for certain is that grooved stone hammers have been found there (DOMERGUE, 1987:199).

5) Esperanza Lode: located to the E of South Lode, the cupreous schists, also with gossan and quartz outcroppings, of Esperanza Lode were exploited recently by an opencast. Lead Isotopes The results of two lead isotope analyses carried out on two samples of complex pyrites from Tharsis mines are available:

d) Evidence of Metallurgy In the surroundings of the orebody slag, scattered or forming heaps, have been reported (GONZALO Y TARIN, 1887:525), probably of the Roman period, although it is possible that in earlier times metallurgical activities were carried out. The study of these remains will provide the concrete information, which is lacking at the moment.

THARSIS MINES (MT) (after MARCOUX et al., 1992)

Municipality: Alosno Name: Tharsis Mines (7) (UTM:29SPB664618)

Pb 208/206

Pb 207/206

Pb 206/204

Th 17 (1)

2.10366

0.86004

18.135

Th (2)

2.10409

0.86023

18.137

a) Name and Location

c) Evidence of mining

The large mineral mass of Tharsis Mines is located some 5 km. to the N of the village of Alosno, and was named thus in 1863 by Deligny. The co-ordinates of its location are those of South Lode, although there are different separate deposits (Fig. 77).

The intense contemporary mining activity by opencast methods, which are still being carried out in South Lode, have removed the great majority of the remains of ancient exploitations in the different lodes at Tharsis. These workings were massive in Roman times, as described in old publications, and located in North Lode (with water wheels and drainage galleries), Sierra Bullones, Poca Pringue, Centre Lode and South Lode (GONZALO Y TARIN, 1887:347-390).

b) Mineralization There are various deposits of complex pyrites, with different metal grades (average 1% Pb, 1.3-5%Zn, 13.5%Cu (VAZQUEZ GUZMAN, 1983:101), with outcropping gossan caps.

The only remains which, for their typology could be considered prehistoric, were documented as on the upper part of South Lode: a trench-type working which was exploiting a vein of an earthy reddish mineral set in yellow rock. Similar remains, less well defined, also appear nearby.

The different Tharsis mineral deposits are (DOMERGUE, 1987:200-210): 116

Prehistoric Mining and Metallurgy in South West Iberian Peninsula in the previously mentioned Pico del Oro zone, and also with slags (DOMERGUE, 1987:203,211).

The absence of marks of metal tools and the forms of the walls seem to indicate the use of stone tools, such as grooved hammers (PEREZ MACIAS et. al., 1992:236), although none connected with this working have been found.

In 1989 also, some squares were excavated there, of which two (numbers 2 and 3) gave evidence of the establishing on the rock surface, in the Late Bronze/Orientalizing periods, of a small metallurgical installation for Ag production, with hand-made pottery, “paleo-Phoenician” amphorae and, again, “free silica” slags (in the form of flat convex balls), tuyères, cupels and crucibles. Those were considered the most ancient evidence of metal production in Tharsis, over which the Roman slags were deposited (PEREZ MACIAS et al., 1992: 228,234).

However, numerous examples of grooved stone hammers have been reported in Tharsis Mines (DOMERGUE, 1987:203). d) Evidence of Metallurgy The clearest signs of metallurgical activity in Tharsis are the slags. There are various large Roman slag heaps (in Silillos, Huerta Grande, South Lode and Esperanza) calculated as being originally about 3.5 million tons., a great deal of which was used as ballast on the railway lines (PINEDO, 1963:216).

Municipality: Berrocal Name: La Caba Mine (8) (UTM: 29SQB229589) Municipality: Berrocal Name: Las Navas Mines (9) (UTM :29SQB241549)

After being analysed, they were classified as Ag slags (ROMAN PEREZ, 1898) although also Cu slags (1.2% Cu, 0.3% Pb and 3 ppm Ag) have been detected (SALKIELD, 1970:88).

Municipality: Cala Name: Cala Mines (10) (UTM:29SQC325035)

Some data on pre-Roman settlements in Tharsis Mines, connected with mining and metallurgy, is known, concentrated in the area N and NE of South Lode, in the zones denominated Pico del Oro and Campo de Tenis.

Municipality: Cala Name: San Rafael Mine (11) (UTM:29SQC374068)

* In the Pico del Oro zone, in the years 1964-1965, the mining operations brought to light remains of a settlement with hand-made and wheel-made pottery, “free silica” Ag slag (analyses 342 to 349), curved tuyères and stone tools for grinding ores (hammer or crusher, as well as a possible mortar), which was dated to the 8th-7th century BC, comparable to the site of Cerro Salomón at Rio Tinto Mines, dedicated to Ag production and lasting until the 5th century BC (DOMERGUE, 1987:203-209).

Municipality: Cala Name: La Sultana Mine (12) (UTM:29SQC392057)

Perhaps this site was related to a grave found at the beginning of the 20th century near the Esperanza opencast, which contained a “Tartessian” gold necklace, dated between the 7th-6th centuries BC (NIEMEYER, 1977).

San Cristobal Mine is located between the river Odiel and the Zafra-Huelva railway line (km.143), to the S of the Atalaya house.

Municipality: Calañas Name: San Cristobal (13) (UTM:29SPB847573) a) Name and Location

b) Mineralization In this same zone of Pico del Oro, a limited archaeological excavation was made in 1989, with negative results regarding habitat structures and stratigraphy (PEREZ MACIAS et al., 1992: 230: PEREZ MACIAS, 1996:107) but recovering numerous fragments of “free silica” slag, dated in the second half of the 7th century BC, of which an analysis gave: 66.7% Si, 15.2% Fe, 0.02% Cu, 3.2% Pb and 336 ppm Ag (PEREZ MACIAS, 1996:112).

The mineralization is considered cupriferous of the lode type, set in slates, then considered Silurian (PINEDO, 1963:478; DOMERGUE:1987:216-7). Quartz and malachite have been detected in the modern dumps (PEREZ MACIAS, 1996:166). c) Evidence of Mining In the concession two reduced zones of workings have been discerned. In the western one, when clearing the ancient workings, the remains of a Roman water wheel were found, as well as stone hammers (PINEDO, 1963:479). In the eastern part, grooved stone hammers and burnished pottery were also found next to modern waste heaps (PEREZ MACIAS, 1996:166).

*In the Campo de Tenis zone, to the NE of South Lode, in the area occupied by the tennis court, precisely when this was being prepared in the 1960’s, a stratigraphic section of 3.9 m was made which was then inspected. The upper Roman strata (more than 2.5 m) were preceded by strata containing Iberian pottery, while the lower strata corresponded to periods comparable with the remains found

117

Mark A. Hunt Ortiz and others with 5.5% Cu (VAZQUEZ GUZMAN, 1983:41). Specific areas have been found with up to 40% Cu (GONZALO Y TARIN, 1887:509).

Municipality: Calañas Name: La Zarza Mine (14) (UTM:29SQB895759)

Also a mineralized vein with 60% Ag has been described, although doubts have been cast on its existence (DAVIES, 1935:120).

a) Name and Location La Zarza Mine is located in the immediate vicinity of Silos de Calañas, near the road from Calañas to Cerro de Andévalo.

The outcropping of the mineralization was not noticeable for the typical gossan hat but by “parched ferruginous zones” which increased at depth, reaching the level of the sulphides, at depths of 100 m (PINEDO, 1963:383).

b) Mineralization The mineralization consists of two main complex pyrite ore masses: to the W, that of Perrunal and to the E, that of Los Silos. Both are orientated from E to W and practically vertical, covered with a gossan hat, which was more than 70 m thick. The Los Silos orebody is the most important, presenting diverse mineral contents, with zones containing up to 7% Cu and even native Cu in the gallery walls and the edges of the deposit (GONZALO Y TARIN, 1887:401-2). On the eastern end there were veins of chalcopyrite and galena (DOMERGUE, 1987:217-8).

c) Mining Evidence In Roman times, as indicated by the levels of the drainage galleries discovered, the gossan and cementation zones were exploited quite extensively, and in those works the remains of various Archimedes screws were discovered (GONZALO Y TARIN, 1887:502-3; DOMERGUE, 1987:221). Of earlier periods, the finding of stone mining hammers has been pointed out (GONZALO Y TARIN, 1887:21), some of them near a malachite outcropping (SERRA I RAFOLS, 1924:160).

c) Evidence of Mining

Undefined remains of superficial exploitation of Cu carbonates have been noted in the Tiberio opencast zone (PEREZ MACIAS, 1995:422), in whose surroundings grooved stone hammers have appeared (PEREZ MACIAS, 1996:167). Examples of stone hammers, precisely from the Tiberio opencast, are now in the Municipal Museum of Valverde del Camino (Fig. 84). The Tiberio shaft was situated in the most eastern part of the concession (PINEDO, 1963:385).

The remains of ancient mining works that have been described are very numerous and extensive although they all seem to be Roman, both the galleries (la Algaida adit was 1.800 m long with 72 shafts) and twin-shafts, of which up to 800 were counted (GONZALO Y TARIN, 1887:393394). Of earlier mining activities it is only known that in this mine some stone tools have been found (GONZALO Y TARIN, 1887:21) which would be of the grooved type (DOMERGUE, 1987:218). d) Evidence of Metallurgy The slag heaps are only mentioned as existing in the surroundings of the mine (GONZALO Y TARIN, 1887:393) apparently concentrated between the village and the Sierra Cerrejón to the N and dated to the Roman period (DOMERGUE, 1987:218). Municipality: Calañas Name: Sotiel Coronada Mine (15) (UTM:29SPB903639). a) Name and Location

Figure 84. Grooved stone hammer from Sotiel Coronada mine.

The Sotiel Coronada Mine was named Site 32 in the Huelva Survey (BLANCO & ROTHENBERG, 1981:117-122). It is located on the right bank of the river Odiel.

d) Metallurgical Evidence

b) Mineralization

The ancient slags have been calculated at 40.000 tons. and classified in three different types (DOMERGUE, 1987:221):

The mineralization consists of three masses of complex sulphides: North Mass, Centre Mass and South Mass. Today the most interesting is considered to be the Centre Mass which has a thickness of up to 11 m with 15% Pb+Zn

-Black slags, green stained, produced in Cu smelting in the Roman period. 118

Prehistoric Mining and Metallurgy in South West Iberian Peninsula b) Mineralization

-Brown slags, apparently with no Cu content. Roman Fe or Ag minerals smelting.

In the zone, along an E-W line, outcrops of tuff and rhyolite appear, containing blue and green Cu carbonates with Fe oxides and quartz gangue.

-A third type, very scarce and of indeterminate date. There is also a report, of 1885, mentioning other slags “earlier than the Romans”, but with no further details (DOMERGUE, 1987:222).

The “marginal” samples of ore analysed were classified as quartz with Cu carbonates and gossan (PH153: 3.7% Cu, 9.7% Fe, 62% SiO2), malachite (PH152: 8.1% Cu, 13.8% Fe, 58.4% SiO2) and chrysocolla and cuprite (PH131: 4.1% Cu, 11.3% Fe, 53.5% SiO2) (BLANCO & ROTHENBERG, 1981:81-83).

Also in the eastern part of the Tiberio opencast, hand-made pottery has appeared, dated in the Late Bronze Age (which would also date the stone hammers) (PEREZ MACIAS, 1995:428) together with some Cu slags, porous and with some unreacted quartz -8.8% Cu, 0.1% Pb, 11 ppm Ag, 20.8% Fe and 44.3% Si- (PEREZ MACIAS, 1996:167).

c) Mining Evidence In the surveys carried out many workings were discovered which were defined as rough cavities and holes made with stone hammers, as well as narrow fissures, one of them following a 3 cm vein of green minerals between layers of red gossan. In the neighbourhood of these workings a large number of mining stone tools were found, without grooves (Fig. 85).

Municipality: Campofrio Name: Cuchillares Mine (16) (UTM:29SQB158809) a) Name and Location Cuchillares mine is situated to the E of the Campofrio dam. It was named Site 54 by the Huelva Project (BLANCO & ROTHENBERG, 1981) and in this zone the contemporary pyrites mine, exploited by shaft and gallery method, of Cuchillares was located (MESEGUER et al., 1945).

No pottery was found but the mining-metallurgical workings were dated, based on a flint scraper, the mining technology and the type of slag, at the beginning of the Bronze Age (BLANCO & ROTHENBERG, 1981:81-83), i.e., Early Chalcolithic.

Figure 85. Stone tools from Cuchillares mine (after Blanco & Rothenberg,1981). 119

Mark A. Hunt Ortiz of complex compositions:

The study of the quarry and the stone workshop discovered in the vicinity of Cuchillares Mine, as well as the study of the lithic industry of the mine itself, has pointed out the homogeneity of forms of the stone tools of both sites, which were also considered to be of Chalcolithic date, and have been related to the dolmens at the source of the river Tinto (CASTIÑEIRA et al., 1988:37-62) and even with a Chalcolithic settlement still not discovered (PEREZ MACIAS, 1996:44-5).

pyrite

samples,

with

the

following

LA JOYA MINE (JO) (after MARCOUX et al., 1992)

This chronology would set aside another date, that of the beginning of the Middle Bronze Age, proposed for Cuchillares Mine and for the workshop, based on an hypothetical relation with the two cist burials discovered close to the workshop (PEREZ MACIAS, 1995:426). The truth is that the dating of the mine workings is still not clear. The study of the lithic material confirmed, as well as the existence of a varied typology, the presence of mining tools with lateral notches, used for fitting a handle (CASTIÑEIRA et al., 1988:51).

Pb 208/206

Pb 207/206

Pb 206/204

J9 (9)

2.09561

0.85751

18.198

JO11 (1)

2.09863

0.85870

18.168

c) Mining Evidence There are general references to the existence of ancient workings, most probably Roman, shafts and galleries, which were concentrated in the upper part of the orebody, especially to the E (GONZALO Y TARIN, 1887:478). The only clear evidence regarding prehistoric mining is the grooved stone hammer (Fig. 86) which was in the MCNUS (SERRA Y RAFOLS, 1924:160), at present deposited in the Department of Prehistory and Archaeology of Sevilla University, which is considered, in all probability, to come from La Joya Mine (DOMERGUE;1987:224).

Three hammers from Cuchillares Mine, with only lateral notches, catalogued as “hoes or flat axes”, are on exhibition in the Municipal Museum of Valverde del Camino. d) Metallurgical Evidence The only evidence of metallurgical activities consists of fragmented slag, crushed into small pieces to extract the metal globules. The slag is of fayalite type and with a composition of 41.9% Fe and low, 0.3%, Cu content (BLANCO & ROTHENBERG, 1981:81-83). Evidently, a wider archaeological and analytical study of this deposit is necessary to understand its real significance. Municipality: Cerro del Andévalo

Figure 86. Grooved stone hammer from La Joya mine.

Name: La Joya Mine (17) (UTM:29SPB743818)

d) Metallurgical Evidence

a) Name and Location

The existence of fairly widespread slag heaps has been mentioned, though of little thickness, on the banks of the river Oraque (GONZALO Y TARIN, 1887:478) and in La Joya river (DOMERGUE, 1987:224), which would surely be Roman.

La Joya Mine is located more than 8 km. to the W of the village of Cerro del Andévalo. b) Mineralization

Municipality: Cerro del Andévalo/Cortegana

The deposit consists of two masses of complex sulphides set in porphyry rocks. The Levante (East) Mass is the more important, with a length of 320 m. The Poniente (West) Mass is located at a distance of 100 m and is 80 m long. Both outcropped with gossan hats, of a variable thickness, between 9 and 30 m (GONZALO Y TARIN, 1887:480).

Name: Lomero-Poyatos Mine (18) (UTM:29SPB827865) a) Name and Location

Two mineral samples from the Levante Mass contained up to 0.2% Cu, 20.8% Pb, 13.8% Zn, 1.07% As and 41.4% Fe (PINEDO, 1971:7).

The Lomero-Poyatos orebody is composed of two sections. The eastern part, known as Lomeros, is in the municipality of Cerro del Andévalo, while the western, Poyatos, is in the Cortegana municipality.

Lead Isotopes

b) Mineralization

From this mineralization there are two lead isotope analyses

The mineralization, of complex sulphide ore, is united at 120

Prehistoric Mining and Metallurgy in South West Iberian Peninsula depth, as well as the workings of the modern exploitation. The polymetallic ore had varying grades, frequently between 1.5-1.9% Cu and 3% Zn and Pb. In certain zones the Pb-Zn contents were higher, with 0.3% Cu, 8% Zn, 5% Pb and 0.1% As. The deposit outcropped on the surface with a not quite developed gossan hat: in Poyatos with only 2 to 4 m thickness and in Lomero the outcrop was defined as unremarkable and very narrow (PINEDO, 1963:250,260). The high grade of precious metals in the complex sulphides is mentioned (PINEDO, 1971:6). c) Mining Evidence The only evidence consists of the reference to the finding of stone mining hammers, which were related to the expansion of Ag mining in the Orientalizing period (PEREZ MACIAS, 1995:436), although this mine is not included, by the same author, in the list of mines with mining stone hammers (PEREZ MACIAS, 1996:169-170).

Figure 87. Grooved stone hammer from Confesionarios mine. d) Metallurgical Evidence In the surroundings only some slag, considered to be Roman, has been mentioned (GONZALO Y TARIN, 1887:449).

Municipality: Corteconcepción Name: El Madroñal Mine (19) (UTM:29SQB205984) Municipality: Cortegana

Municipality: Cortegana

Name: Confesionarios Mine (20) (UTM:29SPB866848)

Name: San Telmo Mine (21) (UTM:29SPB790858)

a) Name and Location

a) Name and Location

The Confesionarios or Herrerias de los Confesionarios Mine is situated on the hill of the same name, in the vicinity of the village of Valdelamusa.

San Telmo Mine is located to the north of the village of San Telmo. b) Mineralization

b) Mineralization

The mine has three well-differentiated complex sulphide orbodies, which are (PINEDO, 1963:275-283; DOMERGUE, 1987:225):

It is a pyrite deposit with, in general, low Cu grades, which extends along the western flank of the hill mentioned. The outcrop consisted of a gossan cap 400 m long and 16 m thick, the greater part of which was removed at the end of the 19th century AD (GONZALO Y TARIN, 1887:448).

1) San Germán, with a 4º N direction, covered with a gossan hat 400 m long and 10 to 20 m wide but with little depth. An opencast has been made to reach the massive ore, which in the upper zones of the deposit contained 6% Cu. Some complex ores gave up to 9% Pb (PINEDO, 1963:275-283).

c) Evidence of Mining Very few ancient workings existed in the western part, only a gallery with shafts dated in Roman times (GONZALO Y TARIN, 1887:450).

2) Cruzadillo, in a 40º N direction, made up of small masses covered with a compact gossan cap, exploited by an opencast.

The grooved stone hammer which was in the MCNUS (Fig. 87) in all probability came from this mine, from the Valdelamusa area.

3) Santa Bárbara, has an E-W orientation, marked by more discreet gossan outcroppings and with average grades of about 1.2% Cu, 0.4% Pb, 12% Zn and 60ppm Ag (VAZQUEZ GUZMAN, 1983: 42). It is considered, in general terms, that the upper levels are richer in Ag (PINEDO, 1971:7).

Based on non-specified information, a prehistoric exploitation of a mass of “copper sulphates” has been suggested (PEREZ MACIAS, 1995:422) as well as, based on the finding of stone hammers in gossan dumps, an exploitation of Ag ores, already, it seems to be suggested, in a period of Phoenician influence (PEREZ MACIAS, 1995:436).

Lead Isotopes The results of three analyses on samples of complex sulphide from this mine are as follows:

121

Mark A. Hunt Ortiz Municipality: Encinasola SAN TELMO MINE (ST) (after MARCOUX et al., 1992)

Name: Los Guijarros Mine (23) (UTM:29SPC818236)

Pb 208/206

Pb 207/206

Pb 206/204

a) Name and Location

ST 12 (2)

2.09797

0.85820

18.188

ST 13 (3)

2.09465

0.85718

18.192

ST 18 (8)

2.09728

0.85816

18.183

The mineralized zone of Los Guijarros, also known as Diamante orebody and La Lapa, is 3 km. to the E of the Portuguese frontier, on the right bank of a meander of the river Múrtiga.

c) Mining Evidence

b) Mineralization

The Roman workings described consist of numerous shafts and galleries (PINEDO, 1963:278). San Telmo has been also exploited in prehistoric times, but regarding this, the only facts known are that in the 19th century AD in the upper levels of the San Germán orebody stone tools were found (PINEDO, 1963:277).

Los Guijarros Mine (numbered 895-M-3 by PRESUR, 1987) is considered to be a Cu/Pb deposit, although the latter does not seem to be in great quantities. The mineralization is joined to a quartz structure set in slate, in a direction N35ºW in which the workings are aligned (Fig. 88). It presents gossan outcrops with Cu oxides and sulphides. The Cu grade in the samples found in these workings reached 70% (GONZALO Y TARIN, 1878:20,595).

d) Metallurgical Evidence The evidence of metallurgical activity is reduced to the discovery of slag heaps, of the Roman period, in the surroundings (PINEDO, 1963:278). Municipality: El Campillo Name: Poderosa Mine (22) (UTM:29SQB064807) a) Name and Location The Poderosa or La Poderosa Mine, is situated in El Campillo municipality, near, to the SE, of San Platón Mines. b) Mineralization The two complex sulphide masses which formed the original orebody were covered by a gossan cap of between 20 to 60 m thickness. This mine was considered to have been the richest in Cu of this type of deposit, especially in its western part (GONZALO Y TARIN, 1887:423), with a large quantity of disseminated chalcopyrite and a great deal of chalcocite and covelline (PINEDO, 1963:439-441). c) Mining Evidence A few decades ago, it was proposed that the exploitation of this mine was carried out by “Tartessians and Romans” (PINEDO, 1963: 440). The stone hammers that have been found in the mine have been considered as evidence of an expansion of Ag mining in the Orientalizing period (PEREZ MACIAS, 1995:436). d) Metallurgical Evidence The only known evidence are the slag heaps, dated in the Roman period, found in the surrounding area (PINEDO, 1963:440).

Figure 88. Los Guijarros mine. Plan and section (after Pinedo,1963).

122

Prehistoric Mining and Metallurgy in South West Iberian Peninsula c) Mining Evidence

c) Mining evidence

The workings most evident today consist of 3 modern exploration shafts (PRESUR, 1987:372-375). The ancient workings were classified as superficial, shallow and made following the direction and the dip of the lode. In the 19th century AD, around these workings and when reopening them, lots of stone picks and hammers of different sizes were found, some of them so big that it was thought they were employed using both hands (GONZALO Y TARIN, 1878:20,595).

The only evidence of prehistoric mining is that on clearing an ancient working during the 19th century AD, more than 40 grooved stone hammers were found, and two iron wedges (GONZALO Y TARIN, 1878:20,595). So, in these workings exploitations would have been carried out in two very different periods: one, prehistoric and a later one, probably Roman. Municipality: Escacena del Campo Name: Del Carmen Mine (25) (UTM:29SQB321533)

In the Sierra de la Lapa zone, situated some 2 km. to the S of Los Guijarros sector, on the left bank of the river, two workings were discovered: Cueva del Moro, with a large slag heap at its entrance, and another working, by the river, with two galleries. In neither of these workings were stone mining tools discovered (PEREZ MACIAS, 1983:210215).

Municipality: Minas de Rio Tinto Name: Rio Tinto Mines (26) (UTM:29SQB130755) a) Name and Location The Rio Tinto Mines is composed of a group of massive complex sulphide orebodies and other mineralizations situated mainly in the Rio Tinto municipality. The publications of diverse character on these mines are numerous and therefore this explanation will concentrate on the recording of fundamental data, especially as regards its potential and its prehistoric exploitation.

Later, a lode was found in the immediate vicinity of the Casa de la Lapa, almost completely covered by a layer of vegetal growth, where grooved stone hammers and Cu carbonates were recovered on the surface (PEREZ MACIAS, 1996:165-166). d) Metallurgical Evidence

The UTM coordinates referred to are those of South Lode. In Sierra de la Lapa area, a Late Bronze Age settlement, with Tartessian related pottery, was discovered. Although this site, at first, was linked with agriculture and fishing activities, only stating that it was near a mineralization (although it appears that such activities were presupposed), through later investigations the settlement was defined as mining-metallurgical, as “some fragments of broken furnace slag” were discovered. An analysis (3.4% Cu, 39.1% Fe, 21.5% Si, 0.01% Pb and 10ppm Ag) allowed them to be classified as Cu slag (PEREZ MACIAS, 1983: 210-215; 1994: 123; 1996:165-166).

b) Mineralization Following, fundamentally, the description of Pinedo (1963:114-189) and of Martín Gonzalez (1981), the complex sulphide orebodies could be put into two large groups. -North Group, consisting of the mineral masses Lago Lode, Dehesa Lode (named before Balcón del Moro) and North Lode (also called Salomón). In order to give an idea of the size of the orebodies, the Dehesa Lode, one of the most exploited in ancient times, was 720 m long and with a thickness of 80 m.

Municipality: Encinasola Name: El Juncal Mine (24) (UTM:29SPC864194)

-South Group, formed by the well known South Lode (also known as Nerva) and the San Dionisio Lode, which was the largest of all the mineral masses. Both would originally constitute a single mass, but was divided by the so-called Eduardo Fault.

a) Name and Location The Juncal Mine is also known as Victoria Mine, and is situated in La Dehesa del Juncal, on the left bank of the river Múrtiga, 4 km. to the S of the village of Encinasola.

To the SW of these groups there was a small lode known as El Valle, with a small gossan hat.

b) Mineralization

These masses had a W-E direction along the sides of a mountain chain formed by the hills of Atalaya, the most western, San Dionisio, Cerro Colorado, Cerro Salomón and Cerro Quebrantahuesos. Together with these sulphide deposits there were completely gossanized deposits, which are known as Cerro Colorado and La Isla, which connected the North and Lago Lodes and Quebrantahuesos (MARTIN GONZALEZ, 1981:104-105).

The Victoria Mine is located in a lode with similar characteristics as those of Los Guijarros. It is a Cu oxides and sulphides deposit marked on the surface by ferruginous quartz outcrops stained with Cu carbonates, with samples of up to 70% Cu (GONZALO Y TARIN, 1878:20,595; DOMERGUE, 1987:228).

123

Mark A. Hunt Ortiz references to prehistoric mining works are very few.

It is also necessary to mention Mesa de los Pinos (or Alto de la Mesa) which will be referred to later, a large area of iron oxides of sedimentary origin, which is situated to the S of South Lode.

It has been suggested that, although rare, the native Cu and the Cu carbonates formed in the outcrops must have been noticed and exploited by the first prospectors (DOMERGUE, 1987) and it appears that the malachite and azurite, with their attractive colours, were apparent on the surface on Cerro Salomón (AVERY, 1974:413). In the Municipal Museum in Valverde del Camino good examples of azurite and malachite from Cerro Colorado are exhibited. The relatively easy accessibility to the levels of the jarosites has also been noted: from the sides exposed by weathering, thus avoiding the layer of hard gossan cap (BLANCO, 1984:105; JONES, 1980:150) (Fig. 6). The product of these, let us say, lateral workings, would be the so-called caves (SALKIELD, 1984:31).

The composition of the Rio Tinto ores is somewhat complex if one takes into account all the substances which were detected in a rigorous analysis (GONZALO Y TARIN, 1887:317) (already mentioned in Chapter III). A more complicated question is the accessibility of these mineral formations, both regarding primary and secondary Cu and Ag, by means of prehistoric mining technology. Lead Isotopes A number of lead isotope analyses of both primary and secondary ores from the different Rio Tinto deposits are available and the results are as follows :

The finding of stone mining tools would also be evidence of the prehistoric exploitation. There are stone tools which have been related to mining exploitation and considered as belonging to the Chalcolithic Age, as is the case of the socalled “rhyolite scrapers” which would have been used to sharpen the stone axes (DOMERGUE, 1987:247), of the type found in Cala and Teuler mines. This is a possibility that would have to be confirmed by studying these pieces. Also, dated to the 3rd-4th millennium BC, a grooved stone pick was recovered in Rio Tinto Mines, like those of the Late Bonze Age, but with the difference that it was pointed at one end (DOMERGUE, 1987:242).

RIO TINTO MINES (R) (after MARCOUX et al.., 1992) Pb 208/206

Pb 207/206

Pb 206/204

RT1-Dehesa (1)

2.09833

0.85785

18.193

C12-Dehesa (2)

2.09847

0.85840

18.207

RT3-Atalay (3)

2.10089

0.85968

18.188

CA1-Atalay (4)

2.10032

0.85905

18.191

CA2-Atalay (5)

2.10325

0.85965

18.198

329-Alfred (6)

2.10295

0.85971

18.192

338-Alfred (7)

2.09911

0.85891

18.180

It can be seen that the evidence used to propose a mining activity in the Chalcolithic Age at Rio Tinto is weak and open to argument. Naturally, the connection proposed between mining activity and the dolmen found in the municipality of Nerva, sustained, solely on the basis of its proximity (ANONYMOUS, 1984:2) cannot be taken as evidence of an exploitation of that period.

RIO TINTO MINES (R) Pb 208/206

Pb 207/206

Pb 206/204

RT-e

2.10095

.85745

18.254

RT-f

2.10293

.85904

18.215

RT-j

2.10218

.85983

18.172

RT-l

2.10200

.85948

18.205

RT-m

2.10426

.86028

18.197

RT-n

2.10065

.85923

18.196

RT-o

2.10356

.86000

18.186

RT-q

2.10172

.85948

18.198

RT-r

2.10174

.85948

18.197

RT-s

2.10060

.85929

18.188

In the Municipal Museum of Valverde del Camino there is a tool catalogued as an axe which came from the SW of Corta Atalaya. It consists of a fragment of a rounded pebble with a pointed end, which would need to be studied to decide whether it could be considered a mining tool. On the other hand, it is true that grooved stone hammers have appeared in different places in the exploitations (DAVIES, 1935:38; BLANCO & LUZON, 1969:126) and there are even references to their appearance, in this case defined as “handleless pounders”, within the mine workings and associated with skeletons. The absence of groove is considered in this case a sign of degeneration rather than a sign of antiquity (DAVIES 1935: 38). In general, the presence of grooved stone hammers has been related with mine workings of the Bronze Age (DOMERGUE, 1987:240).

c) Mining Evidence

The major concentration of stone tools of this type occurred in the sedimentary Miocene gossan on Alto de la Mesa (Fig. 5). It was there that “in an ancient cave beneath the iron hat known as Alto de la Mesa almost a ton of hammers were found, some with signs of use and others apparently

The evidence of Roman mining works are numerous and even specific studies have been carried out (WILLIES, 1981; PEREZ MACIAS et al., 1991). However the 124

Prehistoric Mining and Metallurgy in South West Iberian Peninsula there must be considered as only partial.

new”, which was interpreted as a kind of storage (KENNEDY, 1984:4). If it is considered that mining exploitation was carried out there, it could be suggested, because of the kind of mineralization, the possibility of an exploitation of Fe ores (DOMERGUE, 1987:242) rather than a prospection in search of Ag ores, which is another of the hypotheses suggested for this activity.

What is interesting to note is that the archaeological finds which appeared there were considered, although this hypothesis will be revised, as representative of the Ag metallurgical technology of the Middle Bronze Age (2nd. millennium BC) (ANONYMOUS, 1981:2; BLANCO & ROTHENBERG, 1981:115; ANONYMOUS, 1984:2), based on the treatment of argentiferous ores by cupellation (PEREZ & FRIAS, 1990).

Exploitation of the Orientalizing Period would be carried out by workings developed in the contact between the kaolinized slate and the gossan hat, penetrating laterally into the Lago Lode and searching horizontally the lower level of the gossan, although there is no certainty regarding their size nor the ore that was being looked for (PEREZ MACIAS, 1996:97-99).

-El Cerro de las Tres Aguilas: will also be studied in more detail later. For the moment it is sufficient to say that it consists of a site with chronological phases that produce a certain controversy (HUNT ORTIZ, 1996). These phases have been established both in the Middle Bronze Age as well as Late Bronze/Orientalizing period. Its excavation produced, among the archaeological material, “free silica” slags, which have been related, both technologically and chronologically, with La Parrita settlement (PEREZ MACIAS, 1995:434).

d) Metallurgical Evidence Crushing stones with several hollows appeared on the surface of Cerro Salomon, but also inside mine workings. When opencast operations started in South Lode one of these stones was found with various hollows and a crusher, 45 feet down. It was found exactly in the contact line between the pyrites and the gossan cap which covered it, and it was also noticed that the gossan was generally composed of compacted iron ore, but the place where this piece was found consisted of an ochre-like earth. This earth was thought to be related to the mining and treatment of pigments (KENNEDY, 1894:4). But, knowing now the appearance of this type of stone on Cerro Salomon and the exploitation of jarositic ores in that period, the find would have to be related to the mining of argentiferous ores in the Orientalizing period; ores which would be submitted to a first selection or concentration in the mining work place.

-Corta Lago: this site was situated in the upper part of the northern edge of the Corta del Lago opencast. The opencast operations, carried out in the 1930’s, brought about the cutting through of the archaeological site, exposing its whole section, composed mainly of metallurgical debris, more than 700 m long and a height, at some places, of more than 8 m. At the moment, as the slag has been recently processed as an Ag ore, only a few m of the original section are left. Regarding the most ancient strata, one of the earliest descriptions of the Corta Lago section, which was then over-dimensioned, mentioned the existence, in the lowest levels, of slags with “the same free silica characteristics as those of Salomón” (ALLAN, 1970:9).

Again, in the Municipal Museum of Valverde del Camino, there is, from Rio Tinto, a stone with 16 hollows in its visible faces, very similar to the one found in the Orientalizing site of Castrejones, in Aznalcóllar.

The first concrete data on the stratigraphy of Corta Lago section, although only partial, referred to the existence at its base, excavated on the porphyric bed rock, of 3 shallow furnaces, numbered 109, 110 and 111, containing slag of type “P” (for Phoenician, another name given-originally by Prof. Tylecote to the “free silica” type of slag) with a high content of quartz visible to the naked eye. These structures were dated around the 7th-6th centuries BC (JONES, 1980:157).

From the Roman period there existed at Rio Tinto millions of tons of slags, the great majority of Ag (ROTHENBERG & GARCIA, 1986), practically all disappeared today through its utilisation in different ways, lastly, systematically, as an ore. However, apart from some metal objects found, presumably, in Rio Tinto, of which their local production is not confirmed, like the Bronze Age axe characteristic of the Alentejo culture (DOMERGUE, 1987:240), there is no evidence for Cu metallurgy nor of Fe either, in Rio Tinto before the Roman period.

The first global reading of the stratigraphy, gave the date for the first metallurgical debris in Corta Lago (Site 44/5) as Late Bronze (12th-9th centuries BC). In level 110, belonging to that period, a tapped slag was analysed which was considered to be a product of Ag metallurgy. These strata were followed by those corresponding to the Phoenician period, in which the continuity of the same previous technology was pointed out (BLANCO & ROTHENBERG, 1981:104-107).

The metallurgical evidence at Rio Tinto, which would indicate, indirectly, that of mining, is greater with respect to Ag ores. Presenting them in a chronological order, they are: -La Parrita: is a cist necropolis, perhaps associated with a settlement, situated in the neighbourhood of the village of Nerva. This site is studied in detail in Chapter IV.2. It has some bibliography but the archaeological work carried out

A later revision of the Corta Lago stratigraphy, based on the materials from the squares numbered T1 and T2 125

Mark A. Hunt Ortiz It is considered a mining-metallurgical settlement, dedicated to Ag production, with “free silica” type of slag scattered even in the habitat areas, but without forming heaps. Consequently the Ag production activity was classified as of a domestic character (BLANCO et. al., 1970: 12-13).

(AMORES, 1986) dated the earliest levels of the Corta Lago section to the 7th century B.C. “...with the association of the initiation of the metallurgical activity with the presence of Phoenician elements, and not the contrary” (AMORES, 1986:751). A new study of this section (named then as RT-24) considered the lowest levels, with only hand-made pottery, of the Initial Late Bronze Age (late 9th/early 8th century BC) although some of the pottery types could correspond to the Orientalizing period (PEREZ MACIAS, 1996:83-93), finally stating that the oldest levels could not be earlier than the 8th century BC (PEREZ MACIAS, 1996:80).

The site was dated, with the fairly homogeneous pottery, around the 8th century BC (BLANCO & LUZON, 1969:126). Together with the slag more evidence related to metallurgy was found: stones with hollows (known as multiple mortars, some even made in the bed rock) pounders, charcoal and drops of lead, scorified pottery, as well as “horn-shaped” type tuyères and others of a square section and double conduit. A fragment of perforated pottery (named “colander” type) also appeared (BLANCO & LUZON, 1969; BLANCO et al., 1970:12-13).

In another part of the same Corta Lago section, in a naturally formed lower area (named RT-26), again the stratigraphy was studied, from the bed rock, (RT-26A). A series of levels were distinguished: the lowest one, Level 16, up to Level 5 were dated to the Initial Late Bronze Age. Of these, only Level 5 produced datable pottery, which places it “during the late 9th or early 8th century BC” very close to the first Orientalizing materials.

No clear evidence of furnaces were excavated but it is thought, due to the remains of House-1 (plate XIII), that primitive furnaces were used: a simple hole in the ground in which the tuyéres would be placed or positioned to receive the wind (BLANCO et al., 1970:14).

It was stated that the large number of strata below Level 5, all with no pottery or undatable fragments, could put back the initial date of the chronology as far as the 2nd. Millennium BC. As the excavator himself noted “a point difficult to prove because of the amorphous nature of the fragments of the handmade pottery” (PEREZ MACIAS: 1996:82).

-Quebrantahuesos: this settlement is considered a prolongation of that of Cerro Salomon. The campaigns carried out in 1975 excavated 100 m2 of the total remaining area, of about 650 m2 .

The characteristics of these strata are not specified, nor their thickness nor the appearance or not of metallurgical remains. Above them, with no hiatus mentioned, was Level 4, with handmade pre-Orientalizing pottery but also with a single fragment of wheel-made pottery, by which this level was dated to the late 8th/early 7th century BC.

In the stratigraphy, of just 0.85 m, 4 levels were distinguished, corresponding to 3 phases (Levels 3 and 2 corresponded to the same phase) (PELLICER, 1983:61-63). In Level 4, the most ancient and dated to the Late Bronze, wheel-made pottery appeared with a chronology of late 8th/early 7th century BC. In this level some slag was recovered, although it was far more abundant in the following Level 3, classified as Phoenician-Punic and dated in the 7th-6th centuries B.C. (PELLICER, 1983:66,69).

In Level 3 only handmade pottery was excavated so it was considered, as it was found between two levels containing wheel-made pottery, to be Orientalizing, of an early phase due to the lack of wheel-made pottery (PEREZ MACIAS, 1996:80-81).

The settlement is defined, in general, as rudimentary, with no planned urbanism and with squared huts of stone walls and mud roofs. Metallurgy was its main productive activity. In relation to this activity, apart from slag, some fragments of tuyéres, crushing stones and charcoal were found. A feature noted on this site was its archaism, which is shown by the maintaining of the use of Late Bronze Age elements, such as the “naviform” querns or the hand-made pottery types. The characteristics of the settlement and the excavated remains led to propose a non-permanent, i.e. seasonal or temporal, occupation during the existence of the settlement (PELLICER, 1983:85-87).

The results of the various studies of the Corta Lago stratigraphy is a clear example of the indefinition of the typology of the pottery in the transition period from Bronze Age to the Iron Age. It was also on one of the edges of the Corta Lago section where the “lateral” mining gallery, already mentioned, was excavated. It was named as the Protohistoric Gallery of Corta Lago and was filled with debris, among which were recovered a large quantity of horn-shaped tuyéres, some tapped Ag slag and pottery, dating the complex to the second half of the 7th century BC (PEREZ MACIAS, 1996:97-99).

The type of slag found is not mentioned, but it must have been mostly of the “free silica” type. More information was given later on this site, including the mentioning of the finding of crucibles and a fragment of litharge. The analysed slag from Level 1 was of Ag (BLANCO & ROTHENBERG, 1981:100-101).

-Cerro Salomón: the settlement was located on the hill of this name, and it extended 900 m to the E as far as Quebrantahuesos Hill (BLANCO & LUZON, 1969:125). 126

Prehistoric Mining and Metallurgy in South West Iberian Peninsula d) Metallurgical Evidence

Municipality: Paterna del Campo Name: Cueva del Monje Mine (27) (UTM:29SQB250549)

In the vicinity there were ancient slag heaps (GONZALO Y TARIN, 1887:538) associated with Roman remains, produced from Cu and also Ag ores smelting (DOMERGUE, 1987:233, analyses 350,351).

Municipality: Paterna del Campo Name: Arroyo Zahorí Mine (28) (UTM:29SQB255539)

Muncipality: Santa Olalla del Cala Name: Teuler Mine (32) (UTM:29SQC388019)

Municipality: Paterna del Campo Name: Norte del Chorrito (15 Mines) (29) (UTM:29SQB253507)

Municipality: Valverde del Camino Name: Mansegoso Mine, Site 27 (33) (UTM:29SQB035621)

Municipality: Puebla de Guzman Name: Sierecilla (30) (UTM:29SPB537717)

Name: Herrerías Mine (31) (UTM:29SPB506649).

Municipality: Valverde del Camino. Name: Mansegoso Mine, Site 28 (34) (UTM:29SQB046619)

a) Name and Location

Municipality: Valverde del Camino

The Herrerías Mine is located to the S of the village of Las Herrerías.

Name: Campanario (35) (UTM: 29SPB923574)

b) Mineralization

a) Name and Location

Set in the slates there are two complex sulphide masses (named Santa Bárbara and Guadiana) with pyrites associated with chalcopyrite, blende and galena. Both were marked on the surface by gossan caps, which contained Cu secondary minerals and also native Cu (GONZALO Y TARIN, 1887:540; PINEDO, 1963:233...; DOMERGUE, 1987:232).

Campanario Mine is some 7 km. S of Valverde del Camino village. This mine is identified by Domergue (1987:249) with those known as De la Corte Mines, described by Gonzalo y Tarín (1887:497-500).

Municipality: Puebla de Guzman

b) Mineralization This mine appears to be a complex sulphide orebody, outcropping in the form of iron oxides, which stain the slates and form masses of little development, with a NWSE direction.

Lead Isotopes Only one lead isotope analysis is available, carried out on a sample of complex sulphide ore, with the following results:

In this mine the abundance of the Cu ore known as “negrillo” (chalcocite, Cu2S) was noted, as well as the high average grades of Ag, of 400 ppm, in some sulphide areas (GONZALO Y TARIN, 1887:497-500).

HERRERÍAS MINE (MH) (after MARCOUX et al., 1992)

H 9 (1)

Pb 208/206

Pb 207/206

Pb 206/204

2.09728

0.85777

18.225

c) Mining Evidence More than 40 shafts were discovered, which, as well as the slag heaps, were considered Roman (GONZALO Y TARIN, 1887:497).

c) Mining Evidence The ancient workings were concentrated at the base of the gossan, especially in the west orebody, Santa Bárbara (DOMERGUE, 1987:232), and were classified as Roman (GONZALO Y TARIN, 1887:538), mentioning also the existence of possibly “Tartessian” mining works (PINEDO, 1963:234).

It is thought that from this mine, from the zone of Rodeo del Madroño, grooved stone hammers could have been collected (DOMERGUE, 1987:250). At this place 20 diorite stone hammers were recovered, and one of them was deposited in the Anthropological Museum in Madrid (SERRA I RAFOLS, 1924:160).

Stone mining hammers have been recovered in Herrerias mine (DOMERGUE, 1987:233), which can be considered the only evidence available regarding its prehistoric exploitation.

d) Metallurgical Evidence The metallurgical evidence is restricted to referring to the fact that in the surroundings some slag heaps were found, which were considered probably Roman (GONZALO Y TARIN, 1887:497). 127

Mark A. Hunt Ortiz grade of less then 1%. However, zones with veins of chalcopyrite were detected and some consignments contained more than 6% copper. In the analyses carried out, the average composition of various lots of sulphides were 38% Fe, 6% SO4Ba, and up to 1.97% Cu, 1.4% Pb, 1% Zn, 0.34%? Ag, and 6% SiO2. It outcropped in a gossan hat (recently mined out) with a depth of up to 90 m (GONZALO Y TARIN, 1887:488;PINEDO, 1963:433439).

Municipality: Villalba del Alcor Name: Undefined (36) Municipality: Zalamea la Real. Name: Chinflon Mine (37) (UTM:29SQB084649). Municipality: Zalamea la Real. Name: Tinto-Santa Rosa Mines (38) (UTM:29SPB941681).

The amount of silver shown in the analysis is surprising, and no comment on it was made nor on the other two with 0.17 and 0.18% Ag. Looking at the results of the analysis of ores from the nearby twin mine of Tinto-Santa Rosa, it is quite possible that it is an error of typing and that the results in percentage refer to As and not to Ag.

a) Name and Location The Tinto-Santa Rosa mineralization is in the SW part of the Zalamea la Real municipality, close to the river Odiel. b) Mineralization

Lead Isotopes Three complex sulphide masses appeared there, set in the schists and with gossan caps marking the outcroppings. They were considered a prolongation of the Castillo de Buitrón orebody from which they were separated by the river Villar. The sulphide grades were similar to those of Castillo de Buitrón (PINEDO, 1963:426-431). Mention has been made of narrow veins of malachite in the surrounding slates, which when analysed gave 4.1% Cu (DAVIES, 1935:46).

The result of a single lead isotope analysis made on a complex sulphide sample was: BUITRON MINE (MB) (after MARCOUX et al., 1992)

BTR 11(1)

Pb 208/206

Pb 207/206

Pb 206/204

2.10198

0.85962

18.159

c) Mining Evidence c) Evidence of Mining

Numerous ancient workings appeared in the North Lode: shafts and galleries, which were destroyed when opencast operations started (DOMERGUE, 1987:250).

Although only evidence of Roman exploitation has been found (DOMERGUE, 1987:250), the isotopic data has been used as evidence of prehistoric mining found in the closely, geologically related mine of Tinto-Santa Rosa.

The only reference to prehistoric mining is the finding of grooved stone hammers, which were related both with the exploitation of Cu ores (PEREZ MACIAS, 1995:422) and with the expansion of Ag mining in the Orientalizing period (PEREZ MACIAS, 1995:436).

-Mines in the province of Sevilla Municipality: Alanis Name: Redondillla Mine (39) (UTM:30STH657183)

d) Metallurgical Evidence

Municipality: Alanis Name: La Onza/ Sepultura de la Reina. Undefined (40)

Davies (1935:46, 52-53) mentioned a metallurgical workshop, containing some kind of metallic Pb sheets, which could be Roman although an earlier date has been proposed (DOMERGUE, 1987:250). This workshop has been related with cupellation or liquation processes.

Municipality: Almadén de la Plata Name: Los Paredones Mine (41) (UTM:29SQB535929) Muncipality: Aznalcóllar Name: Tintillo Mine (42) (UTM:29SQB357666)

Municipality: Zalamea la Real Name: Buitrón Mine (38A) a) Name and Location

Municipality: Aznalcóllar Name: Coral Group (Various mines) (43) (UTM:29SQB382575)

Buitrón (or Castillo de Buitrón) Mine is close, separated by the river Villar, to the Tinto-Santa Rosa mines, which are considered a prolongation of the same orebody.

Municipality: Aznalcóllar Name: La Zarcita Mine (44) (UTM: 29SQB391574)

b) Mineralization

Municipality: Aznalcóllar Name: Aznalcóllar Mines (45) (UTM:29SQB432563)

This deposit had two masses of complex sulphide ore and is considered the poorest in Cu of its type, with an average

Municipality: Constantina 128

Prehistoric Mining and Metallurgy in South West Iberian Peninsula of the place, with no further indications of the type of mineralization nor other circumstances.

Name: San Enrique Mine (46) (UTM:30STG809920) Municipality: El Madroño Name: Hondurillas Mine (47) (UTM:29SQB287683)

The finds were produced in two places in the Cabeza La Vaca municipality: in Cumbres de Valdezurrones and in the mine known as la Herreria. Neither of those places has been, so far, located.

Municipality: El Pedroso Name: Juan Teniente Mine (48) (UTM:30STG583929)

b) Mineralization

Municipality: Guadalcanal Name: Potosí Mine (49) (UTM:30STH519201)

The mining surveys carried out on the mineral reserve “La Monaguera” (PRESUR, 1987), only in the area included in the Sheet 897, registered 12 Cu mines, two of them, in the municipality of Cabeza La Vaca: Del Bujo and La Sierra mines. In La Sierra mine, old workings have been detected, with associated Fe oxides and Cu carbonates.

Municipality: Peñaflor Name: Peñaflor Mine (50) (UTM:30STG938771) Municipality: Puebla de los Infantes Name: Undefined (51)

This list follows, fundamentally, previously published works and so, the geographical co-ordinates are not generally given.

In the municipality of Monesterio, to the E of Cabeza La Vaca, 3 Cu mineralizations were discovered, and in that of Calera de León, another 5 mineralizations exploited for Cu carbonates. It would be convenient to carry out an archaeometallurgical survey of all these workings.

Municipality: Azuaga

c) Mining Evidence

Name: Mesas del Castaño Mine (52)

In the Cumbres de Valdezurrones, the find consisted of a grooved stone hammer of serpentine, which was deposited in the Barcelona Museum. In the same place there were remains of mining, a ruined shaft, and also remains related to metallurgy.

-Mines in the South of the province of Badajoz

a) Name and Location Mesas del Castaño (BA 18) is situated 17 km. to the SE of Azuaga, in what is, today, the San Antonio mining concession.

In Cabeza de Vaca itself, in the mine known as La Herrería, a piece of a stone hammer was found which was also deposited in the Barcelona Museum (SERRA I RAFOLS, 1924:164), although this museum (today the Museo de Cataluña) officially reported that these stone tools were not among the objects in the Museum.

b) Mineralization It is a Cu mineralization consisting of three parallel lodes separated by a distance of 8 m in a N10º direction, set in slate.

d) Metallurgical Evidence c) Mining Evidence The only reference mentioned is the finding, in Cumbres de Valdezurrones, together with the mining remains already mentioned, of a furnace and plenty of slags (SERRA I RAFOLS, 1924:164).

The lodes are marked on the surface by ancient workings for a length of 300 m. In the adjacent waste dumps, apart from Cu mineral samples, grooved stone hammers were found.

Municipality: Castuera d) Metallurgical Evidence Name: Miraflores Mine (54) Not far away, near the river Bembézar, there were scattered Cu slags, although its chronology has not been determined (DOMERGUE, 1987:22).

a) Name and Location Miraflores mine (BA 39) is located 6 km. to the N-NE of the village of Castuera.

Municipality: Cabeza la Vaca

b) Mineralization

Name: Cumbres de Valdezurrones and La Herreria Mines (53)

The mineralization appears as a vein with argentiferous galena as the principal ore, although in the waste heaps adjacent to the mine workings there were also malachite samples.

a) Name and Location Regarding the finding of prehistoric mining tools the references are very scarce, only mentioning the toponymy 129

Mark A. Hunt Ortiz Castuera, with a great deal of activity in the 19th and early 20th century AD in the 30 concessions in which it is divided (DOMERGUE, 1987:33).

To the W, there are other deposits with the same mineralization (DOMERGUE, 1987:32). c) Mining Evidence

b) Mineralization As in the majority of the mineralizations in the area, considerable ancient workings have been discovered, of superficial trench type, which have been covered, to a great extent, by contemporary mining operations.

Set in the Precambrian slates, more than 19 lodes, marked superficially by trench works, have been discovered in the different concessions (Fig. 89).

Municipality: Castuera

The mineralization is, essentially, of argentiferous galena, which in the upper levels was oxidised to lead carbonate, cerussite. Samples of chalcopyrite were also frequent and Cu carbonates, especially malachite.

Name: Lomo de Perro Mines (55)

c) Mining Evidence

a) Name and Location

On exploiting the waste heaps adjacent to the mine workings to extract the ores they still contained, for example in the Peñalobosa zone, many stone tools were

In the waste heaps stone hammers and pounders were found (DOMERGUE, 1987:32).

Lomo de Perro (BA 42), is an extensive zone to the NE of

Figure 89. Lomo de Perro area. Plan of mineralizations (after Domergue,1987) 130

Prehistoric Mining and Metallurgy in South West Iberian Peninsula recovered, such as mortars with hollows with all the faces used, as well as three stone hammers, two of them grooved, and the third re-utilised as a mortar (DOMERGUE, 1987:33).

Municipality: Granja de Torrehermosa Name: Las Minillas Mine (58) a) Name and Location

d) Metallurgical Evidence Las Minillas mine (BA 47) is located 2.5 km. to the S of the village of Granja de Torrehermosa.

In spite of having been treated as ores during the 19th century AD, there are still some scattered slags, probably most of them from the Roman Imperial period (DOMERGUE, 1987:34).

b) Mineralization The mineralization is the lode type, with a N20º direction. The gangue is quartz with a paragenesis of chalcopyrite, bornite, galena and blende, in a smaller proportion. In the upper part of the lode the ore appears in the form of narrow carbonated veins, but at depth the carbonates are substituted by the sulphides. Quartz and malachite were abundant in the waste heaps (DOMERGUE, 1987:38).

Municipality: Garlitos Name: El Borracho Mine (56). a) Name and Location El Borracho mine (BA 46) is 10 km. E of Garlitos village, on the right bank of the river Esteras.

c) Mining evidence Together with a contemporary shaft and building, the lode is marked on the surface by trench works situated to the N and S of the shaft.

b) Mineralization In the Palaeozoic slates various lodes outcrop with a N60º orientation. The ore is argentiferous galena (a sample from one of the ancient dumps gave 2.807 gr. Ag/ton Pb) but the paragenesis of the most southern lodes also included chalcopyrite (DOMERGUE, 1987:37).

In the waste heaps grooved hammers of volcanic stone were found, as well as in mines situated to the S and some 3 km. to the SE (Juanita and Santa Clara mines) (DOMERGUE, 1987:39).

c) Mining Evidence Municipality: Jerez de los Caballeros The mineralization is marked on the surface by trenches aligned along a stretch of 1 km. The only evidence of prehistoric mining consists of the finding, together with Roman materials, of grooved stone hammers (DOMERGUE, 1987:37).

Name: Cerro de las Minas Mines (59) a) Name and Location This exploitation is near the Cerro de las Minas (BA 53), located about 2 km. to the W of Jerez de los Caballeros town.

Municipality: Garlitos Name: Las Minillas Mine (57)

b) Mineralization a) Name and Location The mineralization consists of Cu veins, which outcrop as ferruginous caps.

The exploitation of Las Minillas (BA 45) is situated 7 km. to the SE of Garlitos.

c) Mining Evidence b) Mineralization The mining evidence consisted of trench workings, with the walls fallen in and with grooved stone hammers in the associated waste heaps (DOMERGUE, 1987:40).

The principal ore is highly argentiferous galena (5.500 gr. Ag/ton Pb), reaching a depth of 40 m. The upper part of the outcropping deposit is made up of secondary mineral specimens, mainly lead carbonates. Also the presence of Cu minerals has been noted (DOMERGUE, 1987:36).

Municipality: Jerez de los Caballeros Name: Tort Mine (60)

c) Mining Evidence a) Name and Location The exploitation in Roman and modern times of these mines has been very intense. The evidence of prehistoric mining is the presence of grooved stone hammers (DOMERGUE, 1987:37).

It has been impossible to identify the exact place of the mine, but by its situation in the distribution map, to the W of Los Jarales and near the border of the Huelva province 131

Mark A. Hunt Ortiz (SERRA I RAFOLS, 1924:fig. 62), it is located in the W of the Jerez de los Caballeros municipality.

Municipality: Mérida Name: Berrocal Mine (62)

c) Mining Evidence a) Name and Location The only reference to prehistoric mining is the finding of stone hammers (SERRA I RAFOLS, 1924:164).

The Berrocal mine is situated at km. 5 on the MéridaAlange road, on the left bank of the river Guadiana.

Municipality: Fregenal de la Sierra b) Mineralization Name: Los Jarales Mine (61) The mineralization is set in a granite outcrop, related to the Hercynian Mérida batholith, consisting of quartz veins containing different minerals such as cassiterite and chalcopyrite, with secondary Cu carbonates, azurite and malachite.

a) Name and Location The locating of this mine has been very complicated because of the scarce information available (SERRA I RAFOLS, 1924: fig.62), but finally a reference, found mentioning the fact that Barras collected samples of malachite with quartz “in the granite next to Los Jarales station on the railway line from Huelva to Zafra” (CALDERON, 1910,II:118), permitted its geographical situation to be established, in the vicinity of Los Jarales railway station (UTM:29SQC317168).

c) Mining Evidence In the mineralization scattered superficial workings were found, as well as stone mining tools, hammers without grooves, and pounders.

b) Mineralization

The pottery picked up on the surface during an archaeological survey was dated in the Chalcolithic (MERIDETH, 1996:212-223).

As mentioned before, the mineralization would consist of an outcrop, probably a quartz vein containing Cu carbonates.

-Mines in the West of the province of Córdoba To give an idea of the richness in prehistoric mining remains of the Córdoba province, it will only be necessary to mention that Prof. C. Domergue (1987) in the distribution map of pre-Roman exploitations in this province included more than 60 mines. In any case, the data presented will be centred on the most western zone of the Córdoba province, the geographical area covered by this research study.

c) Mining Evidence The only reference is that in this mine stone hammers were found (SERRA I RAFOLS, 1924:164), one of them was deposited in the old MCNUS (Fig. 90), although the place name is stated, incorrectly, as Sarales. It is made of granite, which agrees with the host rock of the Cu lode.

Municipality: Belalcázar Name: La Pastora Mine (63) a) Name and Location La Pastora mine (CO25) is 5 km. to the S-SW of the village of Bélmez. b) Mineralization This consists of Cu bearing lodes, which include carbonates, especially malachite, which appears frequently in the waste heaps. c) Mining Evidence The lodes have been exploited by trenches, marked on the surface. The remains of prehistoric mining discovered consisted of grooved stone hammers. Also some Iberian coins heve been found in this mine (DOMERGUE, 1987:109).

Figure 90. Grooved stone hammer from Los Jarales mine.

132

Prehistoric Mining and Metallurgy in South West Iberian Peninsula orebody. That settlement, very much destroyed, would have been unfortified and made up of a group of huts placed, chronologically, in the II millennium BC, the Middle Bronze Age, but with some fragments of Beaker pottery found among the “black and rough hand-made pottery” (BLAZQUEZ, 1988:120).

Municipality: Fuente Obejuna Name: La Loba Mine (64) a) Name and Location La Loba mine (CO 55) is in a small hill some 3 km. from Fuente Obejuna.

The connection of the settlement with the exploitation of the nearby La Loba mine is confirmed by the discovery in it of metal objects and smelting slags (BLAZQUEZ, 19823:32; 1988:120).

b) Mineralization The mineralization appears on the S. side of the hill, marked by parallel lines of trench type works, which show the direction of the various lodes, NE-SW (DOMERGUE, 1987:135).

There is also the reference to mineral treatment/concentration at the mine, as can de deduced by he detection of a number of hollows, that could be used as mortars, in the granite rock that covers the hill (BLAZQUEZ, 1988:120).

The mineral specimens detected, especially in the dumps, are galena and Pb carbonate, as well as Cu ores, also carbonates.

Municipality: Fuente Ovejuna

c) Mining Evidence

Name: Navalespino Mines (65)

The northernmost lode was exploited by trenches, extending for some 500 m. These trenches are very narrow in the upper part (0.3 to 1 m), broadening somewhat in depth (1 to 1.5 m) and reaching, in some points, a depth of up 20 m.

a) Name and Location Navalespino Mines (CO 57) is located 17 km. to the NW of Fuente Ovejuna village. b) Mineralization

The remains found during its excavation permitted the dating of these workings in two main periods: Bronze Age and Roman Republican (2nd. and 1st. centuries BC) (BLAZQUEZ, 1982-3:37). This latter period was of an intense mining activity (DOMERGUE, 1987:137).

The mineralization consists of up to a dozen lodes orientated between N23º and N60º. In the waste heaps quartz and barytes gangue were found, together with galena and chalcopyrite and its secondary minerals cerussite and cuprite, malachite and azurite, as well as iron oxides from the oxidised upper parts of the veins.

Among the finds considered to be of the former period of exploitation is an ore mortar and several grooved stone hammers (DOMERGUE, 1987:137; BLAZQUEZ, 19823:32). The stone mining tools are classified as picks and “are easily distinguished from the Romans” (BLAZQUEZ, 1988:120).

The mineralization is argentiferous, though not of a very high grade, in the lead sulphides and in the associated grey copper, of 200-600 gr.Ag/ton Pb. However, superficial phenomena of secondary enrichment must have been produced, with high Ag content samples. In the modern workings, at a depth of between 125 and 160 m, chalcopyrite was abundant and also native silver was detected (DOMERGUE, 1987:138).

This affirmation seems to be due to the finding of stone tools, the “mallei” (hammers of hard stone, oval in shape and quite heavy) (BLAZQUEZ, 1988:120) of which examples were found, together with iron tools, both in the mine works and in the stores of the Roman period which were excavated (BLAZQUEZ, 1988:125).

c) Mining Evidence All along the length of the lodes there were trench type workings, sometimes discontinuous, as in Lode 10. In Lode 9 the mineralization was worked for a length of 250 m. The ancient workings, most of them Roman, reached depths of 12 m following the narrow ore veins (DOMERGUE, 1987:138).

This mine could be used, for the data it provides, to complete the typological variation of the stone instruments used in mining, but that information has been given in a very general way and detailed specifications would be necessary. From the Buitrón mine in the Huelva province, for example, from the Roman period, came, kept today in a private collection, a grooved hammer of enormous proportions, used, undoubtedly, in a mechanical system since it would be impossible to use it manually.

In the waste heaps associated with the workings, grooved stone hammers have been found, thought to be related to superficial Cu minerals exploitation.

d) Metallurgical Evidence

d) Metallurgical Evidence

In this mine area the remains belonging to a small settlement were found on top of a hill right next to the

Particularly in the zone from Lode 7 to Lode 11, Roman 133

Mark A. Hunt Ortiz of them had depths of up to 11 m. In the associated waste dumps dozens of grooved stone hammers as well as mortars were found, as in Lodes 2 and 7. In these dumps (Lode 2) more recent material was also detected, as slag and Roman Republican pottery (DOMERGUE, 1987:141).

building remains and debris of smelting operations (slags and litharge) of the argentiferous ores were documented (DOMERGUE, 1987:138). Municipality: Fuente Ovejuna

In the East Piconcillo sector, 2 km. to the SE of the North sector, the situation is very similar, with trench type workings marking the veins, some reaching lengths of nearly 2 km. It appears that the Cu content is higher than in the previous zone, with plenty of fragments of malachite appearing in the waste heaps, in which also grooved stone hammers were detected (DOMERGUE, 1987:142).

Name: El Piconcillo Mines (66) a) Name and Location El Piconcillo Mines (CO 60) is composed of a large group of lodes situated to the S of Piconcillo village (DOMERGUE, 1987:141).

In the South Piconcillo sector Lodes 17 to 22 are located. The mining exploitation presented the same characteristics as those described for the other sectors (DOMERGUE, 1987:142).

b) Mineralization In general, it has been divided into sectors, North, South, East and West (Fig. 91) comprising up to 27 veins with complex sulphide ores: blende, pyrite, argentiferous galena and chalcopyrite. The gangue is of quartz and barytes, with some calcite and fluorite. Secondary minerals were abundant in the adjacent dumps and included Cu carbonates, mainly malachite, and Fe oxides (DOMERGUE, 1987:142, 147).

Finally, the West Piconcillo sector, situated 2.5 km. to the NW of the South sector presented 4 lodes, numbered from 24 to 27. Of these, Lodes 26 and 27 showed the most important and continuous mining workings, and there, also, were found grooved stone hammers and various pounders (DOMERGUE, 1987:143).

c) Mining Evidence d) Metallurgical Evidence Most of the lodes are marked on the surface by ancient trench type mine workings.

The scattered slags detected in all the Piconcillo Mines sectors were related to the important Roman exploitation of these mines, also evidenced by the settlements built in the surroundings of the lodes of the different sectors (DOMERGUE, 1987:142).

-The North Piconcillo sector included 10 main lodes. The trench workings extend for a long distance (200-400 m) with an average depth of between 1 and 1.5 m, though some

Figure 91. El Piconcillo area. Plan of mineralizations (after Domergue,1987)

134

Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Figure 92. Almadenes de Bembézar mining works. Plan and sections (after Domergue,1987). later works. In the associated waste heaps, situated on the southern slope, as well as the mineral specimens already mentioned, grooved stone hammers, both complete and fragmented, made of pebbles from the river, were found. The South Lode had a similar exploitation, though less intense. The trench workings were much less numerous and sometimes forming groups of three. The waste heaps had the same content as in the North Lode.

Municipality: Hornachuelos Name: Almadenes del Bembézar Mines (67) a) Name and Location The Almadenes del Bembézar mines (CO 72) are located in the Dehesa de la Aldelfilla area, by the Bembézar river (Fig. 92).

As mentioned before, the state of conservation of the shafts is especially interesting. They are not very deep (maximum depth 8 m) and inclined, sometimes nearly horizontal, adapted to the dip of the lode. The sections of these shafts had an occasional tendency to be circular, of about 0.8 m in diameter, but mostly they were square, more or less narrow (1 x 1 m) occasionally broadening out following the direction of the vein, measuring up to 1.6 x 1 m (DOMERGUE, 1987:149).

b) Mineralization The mineralization, which is set in Cambrian slates, consists of two parallel lodes, 10 m apart, of cupreous quartz, presenting in the outcrops Fe oxides and Cu carbonates (DOMERGUE, 1987:149-150). c) Mining Evidence

Frequently, the trenches were made in pairs, close together, but without communication between them, as in the case of trench 15 (Fig. 92-D) although in some cases they were connected, as in trenches 3-4 (Fig. 92-A), 17-18 and 23-24.

The mineralization was easily discernible on the surface by the superficial mine workings carried out along the whole length of the lodes. In the North Lode (Fig. 92) there was a line of up to 37 small shafts, which have been preserved undisturbed from

With regard to the access system, there was one working 135

Mark A. Hunt Ortiz that had a sort of stair made in the rock, with steps of between 35 and 50 cm high, but the majority of the trenches showed notches in the centre of the walls or in the corners (Fig. 92-A) which gave hand and foot holds.

Municipality: Obejo/Córdoba Name: Cerro Muriano Mines (69) a) Name and Location

In general, the placing of the shafts and their separation would be in relation to the irregularity of the mineralization of the lodes, which would be mined for their superficial Cu oxides and carbonates (DOMERGUE, 1987:150).

The Cerro Muriano Mines are located immediately to the E of the village of Cerro Muriano, extending to the N, in terrains belonging to the municipalities of Obejo and Córdoba.

These mine workings, based on the type of stone tools employed and, especially, on the few pottery fragments found, have been dated, generically, in the Bronze Age (DOMERGUE, 1987:150).

b) Mineralization The Cerro Muriano mineralized area is considered cupriferous, consisting of a group of 6 lodes set in Cambrian rocks (Archives of the Section of Mines in Cordoba. Demarcation File nº11334/1962, henceforward referred to as ASMC.DF). The lodes, with an E -W direction and dipping to the N, are known, from N to S, as: Santa Isabel del Norte, Calavera, San Lorenzo, Excelsior, Cerro Muriano or San Rafael and Santa Isabel del Sur. The Calavera and San Lorenzo lodes are cut transversely by the only lode with a N-S direction, known as La Unión (DOMERGUE, 1987:117).

Municipality: Posadas Name: Santa Bárbara Mine (68) a) Name and Location The Santa Barbara Mine (CO 81), also known as Casiano de Prado Mine, is situated 10 km. to the N-NW of Posadas, on the left bank of the river Guadalvacarejo.

The average thickness of the lodes is about 1 m, and the main ore is chalcopyrite, with an average grade of more than 4% Cu, although there have been zones where the Cu sulphides had grades higher than 14%. In the upper secondary enriched zones, chalcocite was abundant, found together with cuprite and Cu carbonates (SERRA I RAFOLS, 1924:152). Of the latter, a magnificent example was taken to the Madrid Natural Science Museum from the Cerro Muriano Lode (CARBONELL, 1925-1927:37). The lodes outcropped showing accumulations of red and brown Fe oxides (ASMC,DF 11334/1962).

b) Mineralization The Santa Barbara mine has a lode-type mineralization set in Cambrian slates. The lode, oriented in an E-W direction, outcrops for a length of about 2 km., with an average width of 1.7 m. The gangue is quartz and barytes, with a mineralization of B-P-G type (blenda, pyrite and galena), with their secondary minerals, including iron oxides. Lead Isotopes Only one result (from a galena sample) was available regarding lead isotope composition, taken from the publication by BRILL et al. (1987) (which it has not been able to consult despite intensive searching) and given by J. Olin (Smithsonian Institution):

c) Mining Evidence An opportunity occurred to study these mines, which are located partly inside a military restricted area, together with Dr. Luis J. Tomás García and helped by Army personnel from BRIMZ-XXI Base, Cerro Muriano (TOMAS & HUNT, 1990; 1994).

SANTA BARBARA MINE (Pb) (after BRILL et al., 1987) Pb 208/206 BSP0708 (1)

2.09610

Pb 207/206

Pb 206/204

.85610

18.2116

The results obtained from documentation and bibliographical research, as well as archaeological surveying, succeeded in establishing two great exploitation phases:

c) Mining Evidence

1. A Pre-Industrial phase, which was possibly initiated in the Chalcolithic period, with clear evidence of occupation and exploitation of the mineral resources in the Late Bronze Age, which was extensively increased in Roman times, plus some data referring to Mediaeval times and the 16th century AD.

This mine was intensively exploited in Roman times (DOMERGUE, 1987:155-158), and the most remarkable finds from that period were the Archimedes screws (BLAZQUEZ, 1978:152). The only possible evidence of its working in prehistoric times are the two grooved stone hammers found in the Ag mines of Posadas (SERRA I RAFOLS, 1924:163; DAVIES, 1935:37), which might well have come from this mine.

2. An Industrial phase, which started with the reactivation of the Cerro Muriano Mines in the middle of the 19th century AD. At first, in a timid fashion and making use of the slag heaps and the ancient debris and dumps, and 136

Prehistoric Mining and Metallurgy in South West Iberian Peninsula as blue Cu sulphate in the walls.

attaining a great expansion at the beginning of the 20th century, with the intervention of mining companies such as “Cerro Muriano Mines Ltd.” or the “Cordoba Copper Cº. Ltd.”

In the same outcrop, a few metres to the E, another tiny opencast working was found presenting, at its bottom, the entrance to a working, Mine 1-B, (Fig. 93) in the form of an irregular shaped shaft going down for more than 4 m, filled in with water to that depth.

In the bibliography studied there were frequent references to prehistoric workings (e.g. PINEDO, 1963:21). Of possible workings in the Chalcolithic period there are specific references, which are restricted to the appearance of a settlement, dated in that period, on a hill near the Excelsior shaft (DOMERGUE, 1987:118-119). A flint blade from Cerro Muriano could belong to this same period (DAVIES, 1935:119). So, it would be possible to put forward a hypothesis of a Chalcolithic exploitation of the Cerro Muriano lodes, based also on the striking aspect of the outcroppings and the presence of Cu oxides and carbonates. Further investigations are needed in order to give definite support to this hypothesis.

In the vicinity of these two mines, grooved stone hammers were found, as well as abundant samples of Cu carbonates. About 100 m to the E of Mine 1-B, Mine 2 was discovered (UTM:30SUH466079) (Fig. 93). The entrance, excavated in the slate, had a somewhat rectangular form, poorly defined, with the longest part, of 3.5 m, oriented in the direction of the lode. The working continued with the same narrowness and, at little depth, descended to the E with a slight drop. In the E part, to which access was obtained through a narrow cavity (Fig. 93, section B’-B), the ore was also extracted upwards, leaving a narrow vertical working space, inclined to follow the mineralization. In the interior of this mine the signs of the Cu minerals accompanied by Fe oxides were perfectly visible, especially in the walls above the entrance to the eastern part.

Several authors have also pointed out the finding in Cerro Muriano of objects defined, loosely, as pre-Roman, such as hand-made pottery, deposited in the Ashmolean Museum in Oxford (DAVIES, 1935:119), grooved stone mining hammers (SERRA I RAFOLS, 1924), “stone wedges” and mortars with hollows (DAVIES, 1935:35-37,39).

The waste heap of this mine, to the S, contained malachite and also chalcopyrite samples together with grooved stone hammers (Fig. 94) of volcanic rock, deposited, together with the rest of the archaeological remains collected, in the Provincial Archaeological Museum in Córdoba.

Prof. C. Domergue (1987:119) discovered a settlement in the mining area, known as the Cerro del Depósito, in which hand-made pottery datable in the Late Bronze Age and grooved stone hammers were found. The presence, also, of a fragment of scorified pottery led him to propose the metallurgical treatment of Cu minerals in the same place of habitation.

d) Metallurgical Evidence Apart from the mineral samples and slags from the aforementioned Cerro del Depósito, on the Cerro de la Cantina (UTM: 30SUH452078), immediately to the E of the village of Cerro Muriano, extensive remains of Iberian and Roman periods were found, including a tapped slag heap in the northeastern part.

The new survey carried out in the Cerro del Depósito site (UTM:30SUH458077) brought about the finding of more hand-made pottery and also some fragments of wheel-made pottery on the western slope, as well as samples of malachite, some slag on the top of the western slope and grooved stone hammers, both on the top and the slopes. Grain querns were also collected.

It must be mentioned that the ancient slag heaps at Cerro Muriano, characterised by the presence of slag stained with Cu minerals and even containing metallic Cu globules, covering an area of 40.000 m2 and between 1 to 1.5 m thick, were re-smelted at the beginning of the 20th century AD (CARBONELL, 1925-1927; CALDERON, 1910,I:216).

So, it is considered that this site must be chronology situated in the last moments of the Late Bronze Age (even reaching the 7th century BC according to DOMERGUE, 1987:121), dedicated to mining/metallurgical activities and some of an agricultural nature, which must not have been very developed due to the scarcity of arable land in the zone.

Also, large stone blocks with a cube-like tendency and hollows in all their faces were detected in the valley to the S of Cerro de la Cantina, most probably Roman and used as ore crushers. One of them is kept in the private Posada del Moro collection, in the village of Torrecampo.

Datable in this same chronological moment and related, in principle, to the Cerro del Depósito settlement, three mine workings were discovered located in the outcroppings of Fe oxides with Cu carbonates, some 600 m to the E-NE of the settlement.

-Mines in Southern Portugal Following the administrative division in districts, concelhos (municipalities) and parishes established in Portugal and being confined to the regions of Algarve and Alentejo, the evidence of prehistoric mining is found in different mineralized geological areas, both in the mineral deposits of the South Portuguese Zone, and in others situated outside this geological zone. From S to N, are as follows:

The mine marked as Mine 1-A (UTM:30SUH465079) consisted of various small superficial opencast workings, except for one, a trench, shaft-like working opened in the rocky outcrop containing the Cu mineralization, visible now

137

Mark A. Hunt Ortiz

Figure 93. Cerro Muriano mining works. Plan and sections of A) Mine 1-B and B) Mine 2.

138

Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Figure 94. Stone tools from Cerro Muriano mine.

Faro District

Longo.

Concelho: Alcoutim

b) Mineralization

Name: Cerro da Mina Mine (70)

The mineral deposit consists of a quartz lode mineralized with Cu ore, oxidised to malachite in the surface area.

a) Name and Location

c) Mining Evidence

Cerro da Mina (POR 23) (DOMERGUE, 1987:519) is in the Alcoutim municipality, 1.500 m to the NE of Martim

The dumps of the modern exploitation have covered the 139

Mark A. Hunt Ortiz c) Mining Evidence

ancient workings. Despite this, a grooved stone hammer was found in them.

Name: Atalaia de Alte Mine (71)

On that hill there is a mine working that goes down 41 m, which would be of the trench type (DOMERGUE, 1987:520) in which grooved stone hammers were found, as well as Fe tools (EDMONSON, 1987:209).

a) Name and Location

Concelho: Silves

The mine known as Atalaia de Alte (POR 24) (DOMERGUE, 1987:519) is in the municipality of Loule, in the Senhora da Assumpçâo parish.

Name: Santo Estevâo Mine (75)

b) Mineralization The deposit consists of a Cu mineralization.

The Santo Estevâo mine (POR 27) (DOMERGUE, 1987:520-521) is in Sé parish, 5 km. to the N-E of the village of Silves.

c) Mining Evidence

b) Mineralization

The only information known about this exploitation is that many stone and Cu metal tools were found there (SERRA I RAFOLS, 1924:167).

In this area, mineralized lodes were detected, containing Cu oxides, carbonates and native Cu in their superficial zones (SERRA I RAFOLS, 1924:166; DOMERGUE, 1987:520).

Concelho: Loulé

c) Mining Evidence

Name: Vendinha do Esteval Mine (72)

It appears that in the area there are plenty of mine workings with a primitive typology, quite superficial and without order.

Concelho: Loulé

a) Name and Location

a) Name and Location

Many grooved hammers have been found in Santo Estevâo mine, one of them of diorite. Also Cu axes, apparently flat, were found there (SERRA I RAFOLS, 1924:166).

This mine is also in the Senhora da Assumpçâo parish, in the place known as Querença. c) Mining Evidence

Concelho: Aljezur There is only a reference about the finding of stone and Cu “axes” in this mine (SERRA I RAFOLS, 1924:167).

Name: Arregata Mine (76)

Concelho: Silves

a) Name and Location

Name: Picalto Mine (73)

The Arregata mine is in the Aljezur municipality.

a) Name and Location

c) Mining Evidence

The Picalto mine (POR 25) (DOMERGUE, 1987:520) or Pico Alto Mine is in the Picalto parish, 3 km. to the E of Sao Bartolomeu de Messines.

The only information available is the statement that Arregata is a Cu mine worked since prehistoric times (EDMONSON, 1987:208), but with no knowledge of the data on which this affirmation is based.

c) Mining Evidence Concelho: Aljezur There is some evidence of its ancient exploitation, including Cu tools (SERRA I RAFOLS, 1924:166).

Name: Margalho e Penedo Mine (77)

Concelho: Silves

a) Name and Location

Name: Cisterna dos Caes Mine (74)

The Margalho e Penedo mine is in the Senhora da Alva parish, in the place known as Margalhos, close to the sea.

a) Name and Location c) Mining Evidence The Cisterna dos Caes mine (POR 26) (DOMERGUE, 1987:520) is situated on the hill of the Silves castle itself.

The mine workings discovered in this Cu orebody consisted of a shaft 27 m deep with a gallery. 140

Prehistoric Mining and Metallurgy in South West Iberian Peninsula In this site of Mangancha, Late Bronze Age decorated, burnished pottery was recovered, dated between 10th/9th to 7th-6th centuries BC. (MARTINS, 1996:102), and also Phoenician amphorae, showing a situation similar to that of Riotinto and Tharsis (DOMERGUE, 1983:35).

This working, either Roman or later, must have had prehistoric antecedents if one accepts the mining use proposed for the “stone axes” which were found there (SERRA I RAFOLS, 1924:166).

Beja District

d) Metallurgical Evidence

Concelho: Aljustrel

However, despite the finds mentioned and the excavations made in the areas in which Beaker pottery appeared, no metallurgical activity has been detected apart from that of the Roman period, to which the large slag heaps in the area belonged, calculated at 45.000 tons. (DE ALMEIDA, 1970:213).

Name: Aljustrel Mine (78) a) Name and Location The Aljustrel orebody (POR 2) (DOMERGUE, 1987:495499) is located immediately to the SE of the village of Aljustrel.

Concelho: Beja

b) Mineralization

Name: Juliana Mine (79)

The Aljustrel orebody has two main mineralizations of complex sulphides, with Cu carbonate ores and other secondary Cu minerals such as chalcocite.

a) Name and Location The Juliana mine (POR 6) (DOMERGUE, 1987:503) is located some 14 km. to the N-NE of Aljustrel, in the Santa Vitoria parish.

In the gossan cap of Los Algares, as well as in the settlement of Mangancha, samples of Cu carbonates were collected, showing a very low As content (DOMERGUE, 1983:24,571).

b) Mineralization The mineralization worked in this mine consists of a lode of chalcopyrite, with malachite in the upper zones (EDMONSON, 1987:216).

The main orebodies are those known as Sao Joao do Deserto, with a length of 300 m and 40 m wide, and los Algares. Los Algares has two main masses: Centre Lode (100 m long) and East Lode (500 m long). Centre Lode divides into two masses, Tecto and Muro, and is also considered to include the lodes known as Chalco and Poço, at the SE end (PINEDO, 1963:763).

c) Mining Evidence In the workings, stone hammers have been found and also metal axes and a chisel (Cu and bronze) (EDMONSON, 1987:216), even in the interior of the working (SERRA I RAFOLS, 1924:166).

c) Mining Evidence

Concelho: Moura

Evidence directly connected with prehistoric mining is reduced to the finding of a diorite hammer in a small opencast in Los Algares, together with other undefined tools of diorite and flint (MARTINS, 1996:99) and another two grooved stone hammers (WEISGERBER, 1982:Plate IV,2).

Name: Ruy Gomes Mine (80) a) Name and Location The Ruy Gomes Mine (POR 8) (DOMERGUE, 1987:506) is located near, to the SE, of Moura, in the parish of Santo Aleixo.

With regard to more indirect references to the exploitation of these mines, in the hill occupied by the mediaeval castle of Aljustrel a Chalcolithic settlement was detected (MARTINS, 1996:100).

b) Mineralization The orebody consists of a mineralized lode, apparently predominating the Fe oxides but also containing Cu ores (DE ALMEIDA, 1970:214).

From a later age, in the Los Algares outcrop a Beaker pottery fragment was found, that was considered to be related to the exploitation of the Cu minerals and perhaps Au in this mineralization (DOMERGUE, 1983:30). Also, two other fragments of Beaker pottery were found in the site known as Castro de Mangancha, situated near the S. Joao do Deserto Lode.

c) Mining Evidence 5 grooved stone hammers were found in a mine working, of which it is only known that it had an elliptical form and a very primitive aspect (SERRA I RAFOLS, 1924:165). More samples of stone hammers, a total of 22, were found near a shaft of this mine (DE ALMEIDA, 1970:214).

It appears that in the interior of the mine an arrow head was found, of pure or arsenical Cu (SERRA I RAFOLS, 1924:165), dated between 1500-1100 BC. 141

Mark A. Hunt Ortiz Concelho: Moura

b) Mineralization

Name: Monte Judeu (81)

The orebody has three Cu mineralized outcrops. At depth chalcopyrite appears, oxidised in the upper levels into Cu oxides and carbonates. The presence of native Cu is also mentioned (DOMERGUE, 1987:518).

a) Name and Location The Monte Judeu mine (POR 9) (DOMERGUE, 1987:507) or Monte Judem mine, is located to the S of Moura and some km. to the S of the river Toutalga.

In this area of Alandroal, there are two main groups of mineralizations: one to the N of Alandroal, with deposits of Cu and others of Fe and Mn, and a second group to the SE of that same village, on the right bank of the river Guadiana, with the same type of mineral deposits (CMP, 1960).

b) Mineralization The mineralization is of Cu but no further details are known.

c) Mining Evidence c) Mining Evidence In this mine, grooved stone hammers were found (SERRA I RAFOLS, 1924:165; DOMERGUE, 1987:158).

In this mine grooved stone hammers have been found together with other undefined stone objects (SERRA I RAFOLS, 1924:166).

Concelho: Montemor o Novo

Concelho: Barrancos

Name: Nogueirinha Mine (84)

Name: Barrancos Mines (82)

a) Name and Location

a) Name and Location

Mina Nogueirinha (POR 22) (DOMERGUE, 1987:518) is in the Montemor o Novo municipality.

It is known that in the proximity of the village of Barrancos mineralizations exploited in ancient times have been detected, but the exact position was not specified.

b) Mineralization The mineralization is, fundamentally, of Fe, probably with some Cu ores.

b) Mineralization

c) Mining Evidence

The mineralization must have been of the vein type, with characteristics similar to those described in the municipality of Encinasola, of which they are the western prolongation. Some data are available regarding this zone of the mine known as Minancos (DOMERGUE, 1987:503), consisting of a mineralization of Cu ores, among which are chalcopyrite, malachite and even native Cu.

Stone axes were found here and a metal tool of arsenical Cu (DOMERGUE, 1987:518).

Setubal District Concelho: Grándola

c) Mining Evidence

Name: Serra de Caveira Mines (85)

Stone hammers have been found in the mines of the area (SERRA I RAFOLS, 1924:164) as well as, it appears, Cu tools (DAVIES, 1935:117).

a) Name and Location

Evora District

Serra de Caveira (POR 36) (DOMERGUE, 1987:530) is located to the NW of Lousal.

Concelho: Alandroal

b) Mineralization

Name: Do Bugalho Mine (83)

The Caveira mining zone represents the western limit of the Pyritic Belt (STRAUSS, 1970:17). The mineralization is made up of two sulphide orebodies at the ends of a long (12 km.) stretch of porphyry rocks (PINEDO, 1963:765).

a) Name and Location The Mina do Bugalho (POR 21) (DOMERGUE, 1987:518) seems to be the same as the one called Heredade do Bargalho (SERRA I RAFOLS, 1924:165), located in the Sao Bras das Mattas parish.

The paragenesis consists of cupriferous pyrite, outcropping with gossan caps.

142

Prehistoric Mining and Metallurgy in South West Iberian Peninsula grouped into three large distinct cultural phases: Chalcolithic, Middle Bronze and Late Bronze, this last one subdivided into Pre-Orientalizing and Orientalizing periods. The following exposition treats exclusively those sites, which have been studied directly within this study (or with unpublished data). The rest of the sites with available data will be treated in later chapters. In every archaeological site, the debris (and the metal objects) classified as metallurgical are set out and the results of the different analytical methods applied to them listed.

c) Mining Evidence The exploitation of these mines in the Roman period must have been intense, treating, from the results of the analyses of the slags carried out, both Cu and argentiferous ores (DOMERGUE, 1987:530). The processing of these ores left an accumulation of slag calculated to be 300.000 tons (DE ALMEIDA, 1970:213). The only pre-Roman remains consists of a socketed axe with two loops, for which an exploitation in the Bronze Age was suggested (EDMONSON, 1987:217).

IV.2.1. Chalcolithic

Concelho: Grándola

*El Tejar grave (Gibraleón, Huelva)

Name: Lousal Mines (86)

The grave of El Tejar, which must be near the protohistoric site of the same name (GOMEZ et. al., 1994:333) was excavated in a rescue intervention, in which the work was centred on the surviving structure which would form part of a circular chamber with walls lined with slate slabs and with a lintelled roof, perhaps without a passage (BELEN & DEL AMO, 1985: 71).

a) Name and Location The Lousal mineralized area is immediately to the S of that village. b) Mineralization

This grave has been related to the cist-like structures of the Middle Bronze Age, dating them in the last period of collective burials, at the end of the 3rd/early 2nd. millennium BC.

The Lousal mineralization is made up of 14 polymetallic sulphide orebodies, with a total length of 400 m (PINEDO, 1963: 765).

Amongst the grave-goods of El Tejar, a square section metal awl was recovered (Fig. 95-A) (BELEN & DEL AMO, 1985:76).

The mineralization is composed of pyrite with variable proportions of galena, blende and chalcopyrite, together with an ample number of secondary minerals. The outcropping masses presented a sharpish dip, with ferruginous iron hats of red haematite and limonite, over which concentrations of malachite have been detected.

XRF The analysis of the awl by XRF (PA) gave the following results (PA 7347) (with no detected Zn, As, Ag, Sn, Sb, Pb and only traces of Ni) (GOMEZ RAMOS et. al., 1999): 99.9% Cu, 0.08% Fe.

The orebodies were those known as Massa Extreme Sud (100 m long and 14 wide), Massa Sud (55 m long and 10 wide), Massa Central, Massa Norte and Massa Miguel, worked in ancient times (STRAUSS, 1970:126, 137, 170).

* La Zarcita Tholos (Santa Bárbara de Casas, Huelva)

c) Mining Evidence

The necropolis of la Zarcita, of which this tholos-type grave is part, has been related to the nearby fortified settlement of Los Vientos (a citadel, 30 x 20 m with bastions situated at the most vulnerable points), which has been described as situated in a strategic position, dominating communication routes and controlling the exploitation of the territory, including the fertile Raña valley (PIÑON, 1987a:317). The excavation of this site allowed the establishment of two phases: Los Vientos I, preceding the fortification, classified as Late Neolithic or Transitional, and related to Papa Uvas site.

The only information known is that in the Lousal mines stone hammers were found similar to those from Aljustrel (STRAUSS, 1970:19), i.e., with a central groove.

IV.2. METALLURGICAL ACTIVITY Metallurgical remains are relatively frequent, according to the division mining/metallurgy adopted (set out in Chapter IV.1.), in the mineral deposits with evidence of prehistoric exploitation.

Los Vientos II, evolving from the previous habitat, is considered Chalcolithic despite the absence of metal objects or remains related with copper metallurgy (PIÑON, 1987:275).

This part of the study will be centred on the archaeological sites located, to a greater or lesser degree, in a marginal position or outside the zones containing the mineral resources and in which, through surveys or excavations, metallurgical (or even mining related) debris and artefacts have been recovered. These archaeological sites have been

In any case, in the associated Tholos-type (without passage) grave of La Zarcita, together with an ample group of stone items, a flat metal axe was excavated (Reg.M.H: 130) (Fig. 95-B) (CERDAN et al., 1974:82). 143

Mark A. Hunt Ortiz

Figure 95. Metal objects from Chalcolithic sites in the Huelva province: A. Awl from El Tejar (Gibraleón)(after Belén & Del Amo,1985). B. Axe from La Zarcita grave (San Bartolomé). C. Fragment from El Pozuelo Dolmen-4 (Zalamea la Real) (after Cerdán et al.,1975). D. Fragment from Los Gabrieles Dolmen-4 (Valverde) (after Cabrero,1978). E. Dagger and F. Axe from El Castañuelo (Aracena). G. Palmela arrowhead from Gil Marquez (Almonaster) (after Perez & Ruiz,1986).

144

Prehistoric Mining and Metallurgy in South West Iberian Peninsula XRF

AA

The axe from this grave, as mentioned the only metal object found, was analysed by XRF (PA7339) (in %; Ni, Zn, Ag and Pb not detected) (GOMEZ RAMOS et al., 1999):

The only sample analysed from this site was the fragment of slag (AZ-42), with the following results (in %):

PA7339

Cu 99.0

Fe 0.046

As 0.9

Cu Pb Zn Ag Fe Ca Mg Mn SiO2

Sn Sb 0.03 0.02

* Pozuelo Dolmens (Zalamea la Real, Huelva) From the whole megalithic group in Pozuelo, only the Dolmen 4 offered a small fragment of a copper object (Inv. M.H.:805), probably part of an awl or needle with a square section (Fig. 95-C). This discovery led to the idea of these dolmen type graves belonging to a culture already metallurgical, with the general absence of metal objects due more to cultural reasons than chronological (CERDAN et al., 1974:70).

The results of the analysis of this slag fragment, which is described in the Field Notebook as “scorification”, seems to indicate that the sample corresponds to a fragment of quartz greatly affected by heat, although with reduced quantities of metals.

The proximity of Dolmen-4 to Chinflón Mine, exploited at a time that, at first, was dated in the Chalcolithic, caused a relation to be established between the dolmens and the first metallurgical activities (ROTHENBERG & BLANCO, 1980), although this connection, in the specific case of Chinflón, was revised later (ROTHENBERG & ANDREWS, 1996).

* Poblado Las Mesas (Aznalcóllar, Sevilla) It is also worthwhile mentioning the discovery of another Chalcolithic settlement situated on the border of the new Los Frailes opencast, detected during a field survey by the concentration of Chalcolithic material, also similar to that of Valencina (RUIZ MATA, 1983:199), and which can be dated to the middle of the 3rd millennium BC.

XRF

At present there is no information to define more clearly the extension of the site nor its function nor its possible relation with the nearby Aznalcóllar orebody (HUNT ORTIZ, 1993). The later occupations of this same site, which will be explained later, make such definitions difficult without an excavation.

The fragment of the awl, the only metal object found in the Pozuelo group of dolmens, was analysed using XRF (PA7349) (in %; Ni, Zn, Sn and Pb not detected) (GOMEZ RAMOS et. al., 1999): PA7349

Cu Fe As 97.6 0.27 1.8

Ag 0.017

AZ-42 0.01 0.05 0.02 ---0.85 0.29 0.05 0.004 96.3

Sb 0.03

* Valencina (Valencina de la Concepción, Sevilla)

* Los Páramos (Aznalcóllar, Sevilla)

The Valencina site covers an area of 300 hectares including the necropolis, which partially surrounds it. It is situated in the municipality of Valencina de la Concepcion and, to a lesser degree, in that of Castilleja de Gúzman (SANTANA FALCON, 1993:548).

This settlement is located to the SE of Aznalcóllar and is crossed by the road to Gerena. The making of this road, which necessitated the levelling of the slight slope on which the site is located, exposed a section of 60 m, with an E-W orientation and a maximum depth of 1.5 m.

The subsoil of the area is made up of yellowish Miocene loams, in which any structure made on the land remains clearly defined (FERNANDEZ GOMEZ & OLIVA ALONSO, 1985:9).

In the section there appeared a series of 11 structures made in Miocene terrain and covered by a superficial stratum of brown soil. In general, these underground structures are considered grain stores or huts, although in some cases the function of each one of them is not established. Their interiors were filled with earth with an abundance of archaeological material exposed in the section. In the section of Structure 5 a slagged fragment was collected (AZ-42).

As for the chronology of the village of Valencina, three periods or phases have been established: Ia. Early Chalcolithic (Calcolítico Inicial), with the presence of carenated bowls (“cazuelas carenadas”) type of pottery and the absence of thickened rim plates and dishes (“platos de borde engrosado”).

The pottery found (dishes and hemispherical bowls) (HUNT ORTIZ, 1990:289) is similar to that of the nearby site of Valencina, where the same underground structures were excavated (RUIZ MATA, 1983:185) and dated by C14 to the 3rd millennium BC (HURTADO, 1985:43).

Ib. Middle Calcolithic (Calcolítico Pleno), with the presence of the two elements missing in the previous period.

145

Mark A. Hunt Ortiz Also, in the area of the actual village of Valencina, the finding of metal objects has been registered, as well as fragments of a crucible, in Square A in Jacinto Benavente street and also, in Square D, awls, needles, saws and other metal types were collected (FERNANDEZ & OLIVA, 1985:83).

II.Characterised by the presence of Bell-beaker pottery. The central moment of the Valencina site is given by the calibrated C14 dates (FERNANDEZ GOMEZ & OLIVA ALONSO, 1985:117; CASTRO MARTINEZ et. al., 1996): (GIF-4028) 2560-2250 BC and (I-10187) 27502480 BC. The C14 results for the Bell-Beaker period is (UGRA-72)1890-1510 BC.

Also inside the present town, in Duero Street-39, in the so called Structure 3, considered a hut floor with pottery and stone and bone tools dated in the Chalcolithic Horizon of Valencina, no metal tools were discovered although “relatively plenty of slag of a copper material” was found to be present, especially in levels between 1.76 and 2.64 m. (BLANCO RUIZ, 1991:431).

The nucleus of the habitat area is formed by dwelling structures such as huts and others with a less clearly defined function such as “silos” and ditches. The disposition of the tombs that make up the necropolis, occupying the escarpment of the hill to the NE of Valencina (Tholos del Moro) circling round the site on the East side, has been seen as forming a semicircular limit to the river Guadalquivir valley.

In the area of the sports stadium in Valencina, filled-in habitat structures and ditches were excavated, where metal materials, awls and sickle blades, were recovered (MURILLO et al., 1987:313).

This general arrangement of the habitat zone and necropolis is proof, for some authors, of an orientation in search of resources, not towards the Guadalquivir Valley, but rather towards the N and W, for reasons as much agricultural, as connected with hunting and the exploitation of the mineral resources of the Aznalcóllar area and even in relation to trade routes (MURILLO et al., 1990:359).

One of the excavations which seemed most interesting was that carried out in the area of La Emisora, with elements dated in the Early and Middle Chalcolithic, without reaching the Beaker period (MURILLO DIAZ, 1991:560). The published data mentioned the finding, together with metal objects, mainly awls and saws, of other metallurgical items, for example, in Square ES-IV, “some remains of slag and charcoal” (MURILLO DIAZ, 1991:560). The excavation also found, in Squares VIII-IX, a large circular structure, containing a number of “tuyères, most of them burnt”, as well as another clay tuyére in a hut floor in area E-N. (MURILLO DIAZ, 1991:559).

This theory would be supported by the intense Chalcolithic occupation, which the Aznalcóllar area shows and which appears to have lasted until the Bell-beaker period. A Bellbeaker bowl was found in Aznalcóllar, at present exhibited in the Sevilla Archaeological Museum, and also Beaker pottery has been recovered in the practically uninvestigated area of the quarries of Gerena, more to the E.

The director of this excavation, Mrs.Teresa Murillo, allowed an examination of those findings, which, as has been mentioned, appeared to have an exceptional archaeometallurgical interest. However, the examination of the remains of the excavation of La Emisora gave the following perspective: the remains considered to be tuyères in actual fact correspond to cylindrical clay pieces. The only complete one, of 8 cm (C-Sup.ES. Stratum Sup.), presented clear rims at both ends, with an internal diameter of about 6 cm

As for the local economical activities of the Valencina site, the structures that appear there (ditches and silos) have been connected with an intense agricultural activity, complemented with cattle raising. It has been suggested that, supported by those basic activities, the metallurgical production would have been of little importance, limited to the sporadic treatment of the copper ores from nearby zones, like Aznalcóllar, and perhaps functioning as a centre of control and even of trade (FERNANDEZ & OLIVA, 1985:115-116).

In fact, all the remains classified as fragments of tuyères correspond to a pottery type known as support (“soporte”) with a form of a diabolo, or with a tendency to it, which appears in the more ancient levels normally associated with culinary activities (FERNANDEZ GOMEZ & OLIVA ALONSO, 1985:102,57-58,fig.157), thus dismissing its metallurgical function.

However, despite this affirmation, in this site there were plenty of references, although in many cases quite vague, to the appearance of metal objects as well as remains apparently connected with metallurgical activities, in the different excavations carried out.

Of the fragments that were classified as slags, only a very small fragment was found (0.9cms) (C-IV. Testigo B. Silo I, Sector E-Profile S. Level VI-X) similar to a slag, but which belonged to a sheet of mineralized copper, surrounded by an earthy matrix.

In the excavation in the area of “La Gallega”, to the NE of the present village, of the Beaker period, with underground, interconnected structures of a certain complexity, diverse metal objects were found: two knives with notches for the handle, a fragment of a serrated blade, a flat axe and various awls and needles, all of which were classified as made of copper. Also, the discovery of “various fragments of metal slag” was mentioned (MARTIN & RUIZ, 1992:455-457).

The appearance of ochre is also mentioned in the excavation reports of the Valencina site, sometimes in considerable quantities and related to funerary rituals. This 146

Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Figure 96. Metal objects from Valencina: Roquetito (RQ1, RQ2 RQ3) and El Algarrobillo (RQ4, RQ5). Valencina. In that zone various squares were excavated. In Square 7, a circular structure was discovered dug in the loam, 1.35 m deep and with a maximum diameter at its base of 4.6 m. This structure was interpreted as a hut filled in with remains which seem to correspond to a later use as a rubbish dump (SANTANA FALCON, 1993:548-550). Various stratigraphic units were clearly defined throughout the sequence but with the same pottery types, corresponding to Middle Chalcolithic (SANTANA FALCON, 1993:550-551).

is the case of the dolmen with a circular chamber in the area of Castilleja de Guzmán, in which an accumulation of ochre was discovered, 0.45 m in diameter and 20-25 cm thick (SANTANA FALCON, 1991:448-9). This material could have been obtained from the metal mineral deposits of the area. Of all the archaeological interventions carried out in the site of Valencina, there has only been an opportunity to study, analytically, the archaeometallurgical remains of two of them: El Algarrobillo and El Roquetito-I.

The excavated material of an archaeometallurgical character consisted of a fragment of slag and two metal objects (SANTANA FALCON, 1993:550) (Fig. 96), which were studied analytically. The objects were RQ-4: Metal

-El Algarrobillo El Algarrobillo is situated to the SO of the village of 147

Mark A. Hunt Ortiz chisel (32 gr.); RQ-5: Copper sheet (5 gr.) and RQ-6: Slag, which corresponded to a fragment which had a definite aspect of slag, with copper leachings and extensive porosity.

Metallography

XRF

RQ-4

The XRF analysis of the slag sample (PA7233) gave the following result (in %; Pb, Zn, Ag, As, and Ni not detected):

The metallography was carried out on a sample taken from the edge of the chisel (Fig. 96). The study of the section showed an intense corrosion, which penetrated parallel to the main axis of the object. There are numerous inclusions with elliptical forms and deformed remnants of the dendritic structure.

PA7233 Sn Cu Fe Sb

All the samples, including the slag, from the excavation in El Algarrobillo were studied metallographically.

3.63 51.03 45.22 0.11

The etched sample revealed (Photo 1) a structure of recrystallized grains intensely deformed. The deformation by cold working is such (35-45%) that it has extensively distorted the grains.

Microprobe The two metal objects gave the following elemental composition:

The microstructure of this object reveals that it has been submitted to annealing and to an intense cold-working as the last phase of treatment. Being a chisel, it is possible that its use may have also affected the microstructure.

RQ-4 RQ-5 0.01 Tr Fe Co 0.007 0.01 0.08 0.005 Ni Cu 98.71 99.79 -Zn Tr 1.04 0.08 As 0.01 0.02 Sb 0.015 0.01 Sn 0.015 Ag 0.04 0.03 0.03 Bi -0.01 Pb Tr Au 0.02

RQ-5 This metallography was carried out on a section taken from a fragment of the sheet, probably the broken blade of a knife (Fig. 96). The surface of the object shows a layer of corrosion, cuprite, covering a surface considerably perforated (Photo 2). The object was clearly reduced in thickness, with cuprite particles of the original interdendritic Cu-Cu2O forming long parallel lines, increasing in density towards one of the surfaces (Photo 3).

Photo 1. Metallography of chisel RQ-4 (Etched, x500).

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Photo 2. Metallography of sheet RQ-5 (x125).

Photo 3. Metallography of sheet RQ-5 (Etched, x125). The study of enlargements of the etched sample showed a structure of recrystallised equiaxial grains, with twin lines, which are shown with no deformation (Photo 4). There is a marked gradient in the size of the grains, in connection with

the density of the parallel lines, which indicates that the blade was forged, fundamentally, from only one of its sides, resulting, from the major distortion, in a smaller grain size. The state in which the blade was left was annealed.

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Photo 4. Metallography of sheet RQ-5 (Etched, x500).

Photo 5. Metallography of slag RQ-6 (x500). (Photo 5) with phases which seem to correspond to elements partially reduced more than a proper slag. No fayalite phases were found, nor other iron silicates, but, however, a large quantity of metal copper globules appeared all along the section of the sample, although not very developed.

RQ-6 This metallography was carried out on a sample extracted from a fragment of the slag. The sample shows a very heterogeneous internal structure 150

Prehistoric Mining and Metallurgy in South West Iberian Peninsula RQ-1

So, this sample appears more likely to be a mineral (or better a furnace charge) partially reduced rather than a proper slag of the fayalite type (for comparison see BACHMANN, 1982:23).

The metallography corresponds to a section taken from the edge of the axe (Fig. 96). The microstructure is similar to that of RQ-4, in which the arsenic would appear to be infravalued due to its heterogeneity. The corrosion, in this case, too, penetrated to a certain depth.

Lead Isotopes Lead isotope analyses were carried out on the two metal objects, giving the following compositions:

The section showed the remains of a dendritic structure, with numerous particles of Cu3As in the rich interdendritic arsenical material.

El Algarrobillo (Q) Pb 208/206

Pb 207/206

Pb 206/204

RQ4

2.09734

.85836

18.201

RQ5

2.09543

.85708

18.230

The etching of the sample revealed a structure of intense cold working with heavily distorted recrystallised grains (Photo 6). The combination of the As content (nearly 3.5%) and the reduction of about 40-50% by cold-working, would give the blade a hardness of approximately 200HV, which is comparable with that of bronze (Cu+ Sn) although with much greater fragility (communication from Dr. P. Northover).

-El Roquetito In the area of Valencina known as El Roquetito various sectors were excavated in relation with the construction of a new road Camas-Salteras. 5 graves were excavated wholly or partially: the one known as El Roquetito-I consisted of a sepulchre with a more or less circular shaped chamber with passage and antechamber, dug in the Miocene loams.

RQ-2 The metallography was carried out on a sample taken from the extreme edge of this flat axe (Fig. 96).

There, at base level and together with the remains of 31 individuals with stone, bone and pottery objects, 5 metal objects were dug up: a dagger blade, a saw and 3 flat axes (MURILLO DIAZ et al., 1990:354-356).

The section obtained was very affected by corrosion and only a small proportion of the metal remained, all the rest being mineralized. It shows considerable inclusions of mixed oxides of Cu and As. The etching showed (Photo 7) a distorted recrystallized grain structure. The last phase of the shaping of this object consisted of an intense coldworking.

Although all the samples were lent to study, because of the nature of the analysis and the characteristics of the objects (one axe had remains of cloth adhered to it) only three samples from El Roquetito-I grave were studied (Fig. 96): RQ-1: Flat axe (fragmented in two)(235 gr.); RQ-2: Flat axe (275gr.) RQ-3: Fragmented blade of a dagger (25 gr).

RQ-3 The metallography was carried out on a sample taken from the side edge of the dagger blade (Fig. 96). The sample was seriously mineralized and within the metal phase large oxide inclusions were present, sometimes difficult to distinguish from the corrosion products.

Microprobe The 3 objects analysed gave the following results:

The etching (Photo 8) showed a recrystallised grain structure seriously distorted by intense cold working, which would give the blade a very considerable hardness.

RQ-1 RQ-2 RQ-3 0.01 Tr tr Fe 0.005 tr Co 0.01 0.005 0.01 Tr Ni Cu 96.38 98.93 98.32 -0.01 Zn 0.005 3.47 0.83 1.5 As 0.005 -0.005 Sb 0.01 0.01 0.025 Sn 0.075 Ag 0.005 0.04 0.055 0.05 0.04 Bi 0.025 0.05 0.02 Pb -0.05 -Au

Lead Isotopes The three samples from Roquetito-I were analysed by the lead isotope method, with the following results: El Roquetito I (Q)

Metallography Samples from the objects were extracted and studied metallographically.

151

Pb 208/206

Pb 207/206

Pb 206/204

RQ1

2.07943

.84678

18.455

RQ2

2.11175

.86119

18.249

RQ3

2.09211

.85183

18.346

Mark A. Hunt Ortiz

Photo 6. Metallography of axe RQ-1 (Etched, x1250).

Photo 7. Metallography of axe RQ-2 (Etched, x500).

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Photo 8. Metallography of blade RQ-3 (Etched, x500). Bell-beaker vessels of the maritime type and Palmela type arrowheads (CABRERO GARCIA, 1987:181; 1990:276277).

* Amarguillo-II (Los Molares, Sevilla) The site (often known simply as Amarguillo) is situated 2 km. to the NE of the village of los Molares, and the archaeological remains are scattered over an area of some 5 hectares (CABRERO GARCIA, 1987:180).

The sample AG-5, a piece of slag, as will be mentioned later, contained entrapped fragments of charcoal, which was dated by C14 (OxA-3971), giving a calibrated date of 2854-2472 BC.

The site was discovered by late Prof. M.M. Ruiz Delgado, while making an archaeological survey of the area. Its location was connected with the exploitation of agricultural land and the control of water resources and of cattle paths. In this first survey he picked up a copper arrowhead and was informed of the discovery, in the site, of grooved stone hammers (RUIZ DELGADO, 1985:63-66).

With regard to metallurgical evidence, Structure-I was interpreted as a copper furnace “formed by cavities made of low walls of small stones firmly fixed with clay “ similar to “the smelting furnace of site 39 in Timna”. In this context there appeared what was classified as “a probable fragment of a crucible or tuyére” (CABRERO GARCIA, 1987:181, 184).

In general, the site was appraised as an important Chalcolithic settlement, related with the megalithic funerary area of Los Molares (CABRERO GARCIA, 1987:181), with its initiation established in the Middle Chalcolithic and its abandonment with the first Bell-beaker impact (RUIZ DELGADO, 1985:65).

In the vicinity, slags and other remains connected with copper smelting were found, which reinforced the hypothesis of that interpretation (CABRERO GARCIA, 1987:182). In lower levels another structure appeared which was also interpreted as a more rudimentary smelting furnace, corresponding to the first period of the occupation of the village.

At the site of Amarguillo II, Dr. Rosario Cabrero carried out two excavation campaigns, from which came all the elements studied. The stratigraphy of the site indicates the existence of two strata, one on the surface, all mixed up and some 30 to 40 cm thick, while under this there is a conglomeration of up to 1.69 m thick in which three successive levels of occupation were distinguished, all belonging to the same cultural period, (judging from the typology of the pottery and the presence of thickened rim plates). The abandonment, as said, coincided with the appearance of

The structure consisted of “an irregular hollow” made in the ground, with a lime filling, occupying an extension of 0.95 x 0.58 m (CABRERO GARCIA, 1987:182; 1990:277). Also, at a depth of 1.25 to 1.30 m, there was found what was classified as “unsmelted copper”, ore that was thought to be, from a visual inspection, azurite (CABRERO 153

Mark A. Hunt Ortiz AG-e: Slag (Ref: Am II/1987. Sq. 3, Layer V). Fragment of a light scorification. It is very porous and in some places on the outside there is greenish-yellowish glazing.

GARCIA, 1987:182). It is also worthwhile pointing out the abundance of ochre and red and yellow colouring, both in funerary and habitat contexts (CABRERO GARCIA, 1987:182-184).

AG-f: Scorification (Ref: Am II/1987. Sq. 3. Layer IX). Minute fragment of a very light, porous and yellow scorification.

Samples Studied

3-Metals (Fig. 97):

The samples from Amarguillo II which were available for analysis were the following (the abbreviation for this site was both AG and AM):

AG-a: Metal awl/spatula (Fig. 97-A), (Ref: Sq.2,Sec.N), pointed at one end and bevelled at the other. Rectangular section. Weight: 5 gr. AG-b: Fragment of axe (Fig. 97-B) (Ref: Surface). Weight: 44 gr. AG-c: Spatula (Fig. 97-C)(Ref: Surface). Weight: 11 gr. AG-d: Awl/spatula, bent (Fig. 97-D)(Ref: Surface). Weight: 10 gr. AG-4: Metal fragment with no definite shape (Fig. 97-4) (Ref: Sq.1,Layer V). Weight: 5 gr. AM-40: Awl (Fig. 97-40)(Ref: AmII/1987. Sq.3, Sec.SE;Layer 7). Weight 4.5 gr.

1-Minerals: Minerals (AmII/1986. Square 1, Layer XI /base Layer X, sector SE). These samples correspond to an accumulation of small sized ores which, according to their external characteristics, were divided into three groups: Group 1.- The samples AG-g to AG-o, were classified as fragments of very pure malachite, some of them with internal concentric structure and a “kidney-shaped” external aspect. The total weight of this group of ore samples, mainly well-formed malachite, was 95 gr.

XRF XRF- Ores. Various ore samples were analysed using XRF (PA and RLAHA). The legends used in results tables are:

Group 2.- The group of samples AG-p to AG-u all have a brown compact matrix with a greenish tone, with different coloured spots: brown, reddish and yellowish. The group weighed 320 gr.

p: present not quantified// pm: centred on point-brown powder// pn: centred on point/black powder// pr: centred on point/red powder// pv: centred on point/green powder// ca: centred on calcite globule// az: centred on azurite// mq: centred on malachite// mz: centred on the matrix.

Group 3.- The group of samples AG-v to AG-z and AG-I to AG-X and the samples numbered AM-3X, AG-XP and C1/CX all have a matrix with an intense greenish colour with, also, spots in the matrix, especially brown, in greater or lesser proportion. The whole group of these samples weighed 260 gr.

The results were the following (in %): Group 1:

2-Slags: (RLAHA) AG-g/a(mq) AG-g/b(mq) AG-h/a (mq) AG-h /b (pn) AG-h /c (pr) AG-i/a (mq) AG-i /b (mz) AG-i /c (mq) AG-j (mq) AG-k/a (mq) AG-k /b (pm) AG-l/a (mq) AG-l /b (pr) AG-m (mq) AG-n (mq) AG-o/a (mz) AG-o /b (mq)

AG-2: Low-density slag (Ref: Sq.1,Layer IX, Sector SE). Globular fragment, very porous with light scorification. On the outside, with a lot of limestone adhered, some specific points of glazing of reddish-brown colour. AG-3: Catalogued during excavation as slag (Ref: AmII/1986.Sq. 1, Layer XI), it has a scorification with a globular tendency, very light and porous. One side (a) is less glazed than the other (b), more porous and with greenish glazing. AG-5: Heavy slag (Ref: Am II/1986. Sq. 1, Layer VII). Fragment of slag smaller than a fist, with fragments of charcoal adhered to it. Much porosity and Cu leaching could be seen. Both the black matrix (a) as well as a concentration of copper minerals (b) were analysed. This sample was sent to Oxford to be dated by C14, and it had to be crushed to extract the charcoal.

154

Fe 0.23 0.15 0.23 9.8 27 0.2 18 1.2 0.15 0.8 32.6 0.2 4.6 0.23 0.2 0.3 2.3

Cu As 50.9 0.26 53.8 0.26 47.6 0.35 27.3 1 1.7 1.2 46.5 0.35 24.1 3.83 46.4 0.4 52.9 0.18 50.5 0.98 12.5 1.07 51.5 1.25 6.5 0.53 52.4 0.35 50.5 0.17 27.6 13.3 37.7 16.4

Mn

1.7 1.2 0.5

1.6 0.6

0.5

Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Figure 97. Metal objects from Amarguillo-II.

Fe Ni Cu Zn As Ag Sn Sb Pb

AG-m (PA7209) 0.46 Nd 99.05 Nd 0.49 Nd Nd 0.004 Nd

Group 2 (with Zn p in AG-r/b):

AG-i (PA7229) 0.88 Nd 98.04 Nd 1.08 Nd Nd Nd Nd

(RLAHA) AG-p(pr) AG-q(mz) AG-r/a(pv) AG-r/b(pm) AG-s/a(pv) AG-s/b(pm) AG-t/a(mz) AG-t/b(pr) AG-u(mz)

155

Fe 10.73 8.46 1.5 34.03 9.84 19.23 5.42 13.3 13.2

Cu 32.9 34.2 42.9 3.01 33.3 22.15 35.47 2.94 30.37

As 12.7 12.6 16.42 1.96 12.58 8.21 13.39 2.5 12.14

Mn 1 1.7 0.4 1.1 0.6 8.6 1.2 1.5 0.8

Mark A. Hunt Ortiz pottery fragment (personal communication of Dr. R. Cabrero). This sample (Amarguillo II, 1986. Sq. 1, Layer 9. Sector SW) was analysed in the Department of Inorganic Chemistry of Sevilla University (Sample M3) and the results were given by Dr. Cabero herself.

Group 3: AM-3X/a (PA7208a) 4.61 Fe 0.17 Ni 78.7 Cu Nd Zn 16.47 As 0.003 Ag 0.03 Sn 0.007 Sb Nd Pb

AG-XP (PA7234) Exterior 8.7 Fe Nd Ni 78.35 Cu Nd Zn 12.84 As Nd Ag Nd Sn 0.01 Sb Nd Pb

RLAHA AG-v (mz) AG-w (mz) AG-x/a(mz) AG-x/b(mz) AG-y (mz) AG-z (mz) AG-I (mz) AG-II (mz) AG-III(mz) AG-IV (mz) AG-V (mz) AG-VI (mz) AG-VII(mz) AG-VIII(mz) AG-IX (mz) AG-X (mz)

AM-3X/b (PA7208b) 3.15 0.15 79.29 nd 17.22 nd 0.08 0.007 nd

C1/Cxa (PA7235a) Ext. Brown 14.37 nd 74.45 nd 11.09 nd 0.056 0.021 nd

Fe 2.84 2.42 5.2 0.6 2.4 1.3 1.4 1.9 31.07 2.23 2.88 2.03 1.7 4.6 2.84 4.15

The XRD analysis showed that it was made up of “feldspar (60%), quartz (20%) and calcite (20%)”. Also elemental analyses were carried out on sample M3, using A.A.: Fe % Cu ppm Mn ppm Ca % M % Na % K %

C1/CXb C1/CXc (PA7235b) (PA7235c) Section Ext. green 9.5 3.45 nd nd 73.5 74.54 nd nd 16.89 21.90 0.002 nd 0.056 0.063 nd 0.008 nd nd

Cu 45.6 37.5 38.9 14.4 42.7 25.9 31.2 37.13 12 39.8 34.9 38.03 41 44.9 42.5 43.7

As 0.4 12.4 12.05 5.7 0.2 12.1 10.9 12.5 6.07 12.85 17.32 7.67 8.27 0.2 10.2 0.26

In the visual inspection, the sample seemed to be an irregular fragment of pottery, apparently belonging to a globular pot, subjected to intense heat. One of the surfaces was covered with a sort of green vitreous layer. This side was porous, and in the section (1 cm thick) it was noticed that the porosity diminished progressively towards the interior, which had no porosities.

Mn 0.5 0.7 0.9 -0.4 0.2 0.6 0.7 3.5 0.6 0.6 0.7 0.6 1.2 0.6 1.6

XRF-Metals The samples of metal elements, analysed by XRF, gave the following results (in %): AM-40 (PA7204) 0.11 Fe 0.067 Ni 98.75 Cu Nd Zn 1.026 As 0.004 Ag 0.030 Sn 0.005 Sb Tr Pb

XRF-Slags The samples of slags analysed gave the following results: (RLAHA) AG-2 (int) AG-3/a (ex) AG-3/b(int) AG-3/c (ca) AG-5/a (mq) AG-5/b (az) AG-e/a (ex) AG-e /b (mz) AG-f

Fe 5.8 9.53 10.2 0.7 6.5 5.3 6.03 2.84 4.15

Cu 0.11 0.11 10.2 -36.5 35.7 0.15 0.07 --

M-3 6.37 215 777 3.26 2.04 7.05 1.78

(RLAHA) AG-a/a AG-a/b AG-b/a AG-b/b AG-c/a AG-c/b AG-d/a AG-d/b AG-4

As Ca Mn -5.8 p -7.4 p --p -47.8 -1.33 --1.51 ---14 p -7.4 p -9.8 p

Fe 0.23 0.19 0.15 0.19 0.3 0.17 0.19 0.19 0.19

Cu >90 >90 >90 >90 >90 >90 >90 >90 >90

As --1.96 1.87 --0.27 0.53 --

Microprobe Five of the metal samples were also analysed by microprobe, with the following results (in %):

Mention must be made that the classification of a possible crucible or tuyère, indicated earlier, was made by Dr. Cabrero (CABRERO GARCIA, 1987:184) based on a

156

Prehistoric Mining and Metallurgy in South West Iberian Peninsula Fe Co Ni Cu Zn As Sb Sn Ag Bi Pb

AG-a Tr 0.005 0.01 99.6 0.01 0.2 Tr 0.005 0.035 -0.04

state.

AG-4 AG-b AG-c AG-d 0.04 tr tr 0.01 tr 0.005 0.01 0.005 tr 0.005 0.01 0.015 99.7 96.9 99.4 99.11 tr ---0.08 2.97 0.46 0.74 0.01 -0.01 -0.01 0.007 0.005 Tr 0.025 0.01 0.005 0.04 0.07 0.01 0.03 0.01 0.015 -0.015 0.045

AG-c This metallography was carried out on a section taken from the less marked edge of a spatula (Fig. 97-C). The surface was affected by corrosion, which produced cavities in the metal and developed towards the interior in an intergranular form. The dendritic structure was very distorted, as well as the copper oxide particles, in lines. Superimposed on it (Photo 12) was a recrystallised grain structure with twin lines. The grains and the twin lines showed no distortion, and the large size of the grains (50-60 µm) would indicate a single reheating.

Metallography The same metal objects analysed by microprobe, as well as the slag numbered AG-5, were studied by metallography. AG-a

Consequently, this part of the object was cold-worked and reheated without being subjected to later working.

The metallography corresponds to a section taken from the stem of the awl (Fig. 97-A).

AG-d The metallography was carried out on a sample taken from near the edge of a spatula (Fig. 97-D).

The metallography (Photo 9) showed a severe superficial corrosion which extends to the centre of the object following the disposition of the dendritic structure which was still visible, although very distorted, with a spiral disposition around the main axis of the object.

The section showed a layer of surface corrosion, as well as numerous inclusions of CuO2, As2O3 and a mixture of both, concentrated in the limits of the grains. The etching revealed (Photo 13) a structure of recrystallised grains with twin lines -from annealing-, rather distorted.

Superimposed on this remnant dendritic structure could be seen the structure of grains with twin lines (Photo 10). Both the grain and the twin lines showed severe distortion.

This spatula was cold-worked and annealed and, after the last reheating, was cold-worked, which brought about the grains and twin lines deformation.

So, this object was subjected to an intense cold-working to give it the required shape. It was also annealed which did not succeed in making the dendritic structure disappear completely and then was finally cold worked after the last annealing, which produced the distortion of the twin lines and grains.

AG-4 The metallography corresponds to a section of a metal object with no definite form (Fig.53-4). The study of the sample before etching showed an intense and deep corrosive action.

AG-b The metallography was carried out on a section taken from a fragment of an axe (Fig. 97-B). The surface of the sample, partly covered by cuprite, was greatly affected by corrosion. Some internal cavities were seen to be occupied by corrosion products, which had an inter and intragranular character when extending away from the cavities. Also, in the interior there could be appreciated a few, scarcely developed inclusions of arsenical oxide and also Cu3As.

The etching presented problems but in some zones it could be seen, although with difficulty, a structure of recrystallised grains, with twin lines in some areas. From this sample it can be confirmed that the object was coldworked and annealed. AG-5 This metallography corresponds to a fragment of slag, which was sectioned and submitted to standard metallographical procedures.

Before etching, remnants of dendritic structure could be distinguished but less visible after the etching (Photo 11), with well-developed grains (50 µm), which would indicate a slow cooling in the mould.

The section studied showed a very heterogeneous internal structure, with much porosity and numerous different internal phases, which would need a specific study to make identifications.

Superimposed on the remnants of the dendritic structure, recrystallised grains with undistorted twin lines were visible, with no final cold-working in this area of the sample.

One phase which, however, was visually identified was the fayalite (BACHMANN, 1982: 25, plate XIIa) forming a net of fibrous crystals in the crystalline matrix (Photo 14).

This tool (or rather this part of the tool) once out of the mould was cold-worked and annealed, then left in this latter 157

Mark A. Hunt Ortiz

Photo 9. Metallography of awl AG-a (Etched, x125).

Photo 10. Metallography of awl AG-a (Etched, x1250).

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Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Photo 11. Metallography of axe AG-b (Etched, x500).

Photo 12. Metallography of spatula AG-c (Etched, x125).

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Photo 13. Metallography of spatula AG-d (Etched, x500).

Photo 14. Metallography of slag AG-5 (Etched, x500). There were plenty of metal copper globules in the whole of the sample, especially in the zones without fayalite.

Amarguillo, each one of them coming from one of the different groups of ores established:

XRD

Group 1: AG-g: The only phase detected was malachite (Cu2CO3(OH)2).

Analyses by XRD were also carried out on 3 samples from 160

Prehistoric Mining and Metallurgy in South West Iberian Peninsula * Province of Sevilla It corresponds, as was appreciated visually, to a fairly pure sample of copper carbonate.

Found in the province of Sevilla, three Palmela type arrowheads (Fig. 98) (classified according to the general typology proposed by ROVIRA et al., 1992), were studied analytically: PS-1(type B), PS-2 (type A) and PS-3 (type C).

Group 2: AG-p: The phases detected were pseudomalachite (Cu5(PO4) 2(OH) 4) and goethite (FeO(OH)). Group 3: AG-w: In this sample the mineral compounds pseudo-malachite (Cu5(PO4) 2(OH) 4), muscovite, (KAl2(Si3Al)O10 (OH,F)2) and quartz (SiO2) were detected.

XRF The XRF (RLAHA) analyses carried out gave the following results (in %):

Lead Isotopes On samples from the Amarguillo II site various lead isotope analyses have been carried out, both on metal and ore samples (h,j,l,n). The results are as follows:

(RLAHA) PS-1 PS-2 PS-3

Fe 0.2 0.2 0.1

Cu >90 >90 >90

As 4.7 0.35 0.62

Microprobe

Amargillo –II (AG) Pb 208/206

Pb 207/206

Pb 206/204

AG4

2.08111

.84615

18.498

Aga

2.09951

.85892

18.207

Agb

2.08391

.84370

18.564

Agc

2.07476

.84155

18.626

Agh

2.09064

.85892

18.174

Agj

2.09446

.85129

18.384

Agl

2.10019

.85878

18.240

Agn

2.10122

.86279

18.185

The results of these analyses, done in the metallographic sections, are fairly similar to those obtained by XRF: PS-1 PS-2 PS-3 Tr 0.01 0.01 Fe 0.005 tr Co 0.01 0.02 0.005 0.15 Ni Cu 93.71 99.33 99.28 0.01 Tr Zn 0.02 6.12 0.36 0.53 As 0.03 0.02 0.01 Sb 0.01 0.01 0.01 Sn 0.03 0.08 Ag 0.03 0.03 0.11 tr Bi 0.015 0.05 0.03 Pb -0.04 -Au

Figure 98. Palmela arrowheads from the province of Sevilla. 161

Mark A. Hunt Ortiz the surfaces of the sample. Most of them were associated with cracks, which probably had a mechanical origin, although they were enlarged and extended by the action of the corrosion.

Metallography PS-1 The metallography was carried out on a sample taken from the side of the edge of the arrowhead (Fig. 98, PS1). The section obtained showed a fairly homogeneous metal, with few inclusions. On the surface a layer of corrosion was detected containing a Cu3As precipitate. The etching (Photo 15) showed a homogeneous metal phase, with completely recrystallised equiaxial grains, of variable size, with twin lines.

The etching showed a very distorted structure of recrystallised grains, which would give the arrowhead an appreciable hardness. * La Pijotilla (Badajoz) The study of this site was carried out, at first, through the archaeological remains collected on surface finds. The objects are now kept forming the “Colección Domínguez”, in which the metal industry is represented by a rich variety of tools characteristic of the Chalcolithic Age: axes, awls, sickles, daggers, spatulas and rings (HURTADO, 1988:36). It must be mentioned that at the site of La Pijotilla a number of mineral fragments were also collected, which have also been included in the analytical work.

PS-2 The section studied was taken from the side of the edge of the arrowhead (Fig. 98, PS2). The sample was severely corroded with only a small part remaining of the metal phase (Photo 16). The etching showed a distorted recrystallised grain structure, with twin lines.

Also, the different archaeological excavation campaigns which have been carried out since 1976 have allowed the site to be defined as one with the greatest extensions known, which together with the richness and diversity of the material recovered has succeeded in considering it a centre of considerable importance in its period (HURTADO, 1980:196; 1991:66).

PS-3 The sample was taken from the side edge of the arrowhead (Fig. 98,PS3). The surface showed signs of corrosion (Photo 17), which produced considerable cavities, especially on the edge itself. There were numerous inclusions of cuprite and mixed oxides, located parallel to

Photo 15. Metallography of arrowhead PS-1(Etched, x125)

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Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Photo 16. Metallography of arrowhead PS-2 (x125).

Photo 17. Metallography of arrowhead PS-3 (x125). found were considered to be from an earlier occupation (HURTADO, 1991:66). The only C14 dating available is, calibrated, 2460-2280 BC (GARCIA SANJUAN, 1996; incorrectly catalogued by CASTRO MARTINEZ et al., 1996).

There, structures of huts and “silos” have been documented, as well as ditches and burials of different typology, among which the most remarkable are the Tholoi (the T-3, for example), excavated in the limestone bedrock and covered with a false cupola. In those collective graves, ochre was used in the funerary rites (HURTADO, 1988:46).

A Bell-Beaker phase has also been detected, both in habitation areas and in differentiated burial sites (circular tombs) (HURTADO, 1988:44,52).

As for the chronology, at first it was thought that its origin was in the Middle Chalcolithic, although some remains 163

Mark A. Hunt Ortiz Ochre: (P95,T-3, B/III/1, 19). Excavated in grave T-3.

The Bronze Age was also detected, just from surface materials. The levels corresponding to that period have been considered as washed away (HURTADO & ENRIQUEZ, 1991:71).

Metal Samples (Figs. 99-101) CD-10(A): Fragment of a thick blade slightly curved of a rectangular section (Fig. 99). Fractured at both ends. Weight: 100gr.

Samples studied The samples from La Pijotilla, as the majority came from the Dominguez Collection, were denominated CD, followed by the corresponding number. For the lead isotope analyses the CD was changed to P, followed by the same number.

CD-11(B): Fragment of a chisel with squared section and sharp edge (Fig. 99). CD-12(C): Long chisel with rectangular section and sharp edge (Fig. 101). Weight: 20 gr.

From this site the following samples were studied: Ores:

CD-13(D): Halberd with central rib and trapezoidal, perforated hilt area (Fig. 100). Weight: 275 gr.

CD-1: Nodule of iron ore. It has the appearance of a reddish gossan pebble but, on being fractured, the interior shows specular haematite (oligist).

CD-14(E): Fragment of a flat axe of rectangular section, with protruding edges at the ends and sharpened on double bevel (Fig. 99). Weight: 140 gr.

CD-2: Ore with malachite, in some areas, very pure, and iron oxides.

CD-15(F): Irregular shaped piece of metal, with no clear typology and with flat-convex section. It has been considered a possible ingot (Fig. 99). Weight: 200 gr.

CD-3: Fragment of ore, predominantly chalcopyrite with internal bands. Green copper leachings and yellowish iron oxides were visible.

CD-16: Fragment of awl or punch. CD-17: Metal fragment, probably belonging to the edge of an axe (Fig. 101).

CD-4: Fragment of ore with quartz, iron oxides and leached copper minerals, with a similar interior.

CD-18: Fragment of the blade of a pointed dagger (Fig. 101).

CD-5: Fragment of greenish ore, containing quartz with green copper leaching and yellowish spots of iron oxides.

CD-19: Fragment of a piece of shapeless sheet. CD-6: Fragment of quartz with copper mineralizations in the form of greenish leaching and little iron oxide.

CD-20: Fragment of a curved saw or sickle. The inside edge is serrated (Fig. 101).

CD-7: A fragment of ore which seems to be a fragment of compact slate with brilliant spots which would correspond to pyrites, plus some iron oxides and green copper leaching.

CD-21: Metal fragment of no precise typology. CD-22: Metal fragment of no precise typology.

CD-8: Fragment of pyrite with ferruginous zones in the interior and green copper leaching covering the outside.

CD-23: Fragment of a straight saw or sickle with serrated edge (Fig. 101).

CD-9: Quartz nodule in which malachite and iron oxides were visible.

CD-24: Fragment of a tip (Fig. 101). CD-25: Metal fragment of no precise typology.

Inv. 74: Cuprous ore with a considerable amount of greenish spots in a dark brown matrix.

CD-26: Metal fragment of shapeless sheet. Inv. 75: Cuprous ore, greenish tones in a dark brown matrix CD-27: Metal fragment of no precise typology. Inv. 76: Cuprous ore, greenish spots in a dark brown matrix. CD-28: Fragment of a rod. Ochre CD-29: Fragment of a thin sheet. Ochre: (P95, T-3,C/II/4, 19-ground-). Excavated in grave T-3.

Dagger T-3: Flat dagger with lateral notches (P91, T3, A/III/3, 15, Bag-7) Excavated in T-3 (Fig. 100). Weight: 40 gr.

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Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Figure 99. Metal objects from La Pijotilla.

165

Mark A. Hunt Ortiz

Figure 100. Dagger (T-3) and halberd (CD13) from La Pijotilla.

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Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Figure 101. Metal objects from La Pijotilla. Inv. 71: A rounded metal drop, probably from casting (2.5x2x0.9 cm). Weight: 13 gr.

(RLAHA) CD-1 CD-2 CD-3 CD-4 CD-5 CD-6 CD-7a CD-7b CD-8a CD-8b CD-9

Inv. 72: A rounded metal drop, probably from casting (4x1.5x1cm). Weight: 18 gr. Inv. 73: An irregular metal drop, probably from casting (4x3.5x1.7 cm). Weight: 46 gr. XRF XRF-Ores

Fe 33.34 2.26 4.34 5.6 1.7 0.38 9.6 17.2 1.26 6.15 1.15

Cu 0.11 39.25 33.96 34.3 37.3 46.4 34.3 23.6 45.6 32.18 26.03

As

Pb

Zn

Mn 1.8

1.75 2.6

0.9 0.2

0.27 0.6

XRF(PA) analyses were repeated on ore samples CD-3 and CD-8, in various different points, both on the sectioned interior and on the exterior. The results (PA7236 and PA7275) were as follows (in %; Ni not detected):

The XRF analyses (RLAHA) carried out on the ore samples gave the following results: 167

Mark A. Hunt Ortiz no Ni, Zn and Pb detected) were: CD3a 4.89 Fe Cu 83.12 Zn 4.45 nd As Ag 0.018 tr Sn 0.02 Sb Pb 7.48

CD3b CD3c CD8a 4.48 4.23 12.6 84.11 83.03 87.1 4.65 Nd 4.4 nd 0.24 nd 0.002 0.006 0.03 0.05 nd 0.05 0.33 0.015 0.18 6.89 8.02 Nd

CD8b 8.5 90.9 Nd Tr 0.02 0.03 0.27 0.21

CD8c 12.8 86.01 nd 0.59 0.03 nd 0.5 nd

Inv. 71 PA7089 1.85 Fe Cu 99.7 Tr As Nd Ag Nd Sn Nd Sb

Inv. 75 PA7092B 4.51 76.41 14.7 nd 0.07 0.03 0.03 4.22

Inv. 73 PA7091 0.38 98.94 0.66 0.002 tr 0.009

Microprobe

Other ores from La Pijotilla gave the following results from XRF (PA) analyses (in %; Ni not detected): Inv. 74 PA7092A 6.81 Fe Cu 93.13 Nd Zn Tr As Tr Ag 0.03 Sn 0.02 Sb Nd Pb

Inv. 72 PA7090 0.36 99.39 0.19 0.004 nd 0.003

The metal samples analysed by this method gave the following results (in %):

Inv. 76 PA7092C 3.37 96.56 Nd Nd Nd 0.07 0.003 Nd

Fe Co Ni Cu Zn As Sb Sn Ag Bi Pb Au

XRF-Ochre From the results of the XRF analysis it is only possible to note that the two samples of ochre from Tomb 3 were composed of iron, from which it can be deduced that iron oxide was used for the funeral rites.

CD29 0.01 tr 0.01 98.12 0.01 1.71 0.01 -0.02 0.04 tr 0.04

CD17 Tr 0.01 0.01 98.76 0.01 1.06 0.01 tr 0.02 0.07 tr tr

CD18 0.01 -0.01 98.88 0.02 0.92 tr tr 0.01 0.05 0.03 0.05

CD20 0.01 -0.04 97.67 tr 2.13 0.01 0.01 0.01 0.05 0.04 tr

CD23 CD24 0.005 tr 0.005 -0.01 0.005 97.04 95.16 0.01 0.01 2.68 4.65 0.01 0.01 --0.12 0.11 0.04 0.02 0.05 0.025 tr --

Metallography

XRF-Metals

The same samples analysed by microprobe were also studied metallographically.

The XRF (RLAHA) analyses carried out on the metal objects were (in %):

CD-17

CD-10 CD-11 CD-12 CD-13 CD-14/ext. CD-14/sec. CD-15 CD-16 CD-17 CD-19 CD-20 CD-21 CD-22 CD-23 CD-24 CD-25 CD-26 CD-27 CD-28 CD-29

Cu 95.75 97.42 96.29 95.88 98.68 99.23 95.56 98.34 98.59 96.53 97.47 98.92 97.93 96.63 95.52 99.28 98.98 97.74 98.42 97.72

The metallography was carried out on a sample taken from the edge of this axe fragment (Fig. 101).

As 4.24 2.57 2.94 4.1 1.31 0.75 4.42 1.65 1.4 3.46 2.52 1.07 2.05 3.35 4.46 0.7 1 2.25 1.55 2.27

The surface of the section presented severe corrosion, which developed in depth in the direction of the main axis of the object. There were some rather distorted mixed oxide inclusions, also following the main axis. The etching (Photo 18) showed remnants of the dendritic structure and also an extremely distorted recrystallised granular structure, with strain lines, which indicate a cold reduction of about 30% after the final annealing. CD-18 The section (Fig. 101) was completely corroded and no data could be obtained about its microstructure. CD-20

The XRF (PA7203) analysis of the dagger from Tomb 3 (T-3) gave (without detecting Zn, Sn and Pb) the following results (in %): T-3

The metallography was carried out on the complete transverse section of this saw (Fig. 101) although problems with the mounting only allowed three separate areas to be studied.

Fe Ni Cu As Ag Sb 0.03 0.08 98.5 1.07 0.15 0.1

In sound condition, the metal presented numerous small oxide inclusions. The etching showed the existence of a

The analyses by XRF (PA) of the metal drops (in %; with 168

Prehistoric Mining and Metallurgy in South West Iberian Peninsula CD-29

structure of recrystallised equiaxial grains with twin lines, as well as strain lines, concentrated in some areas (Photo 19), indicating a variable grade of distortion, from the zones not affected to a cold work deformation of more than 40% (Dr. P. Northover, personal communication).

The metallography was carried out on a section of this shapeless fragment. The corrosion has penetrated deeply, with a fissure cutting across it, filled with cuprite. The surface has many hollows made by the corrosion, which penetrated following the grain boundaries. The etching (Photo 22) showed a recrystallised grain structure with twin lines, somewhat distorted.

CD-23 The sample was taken as a complete transverse section of the blade of a saw (Fig. 101).

Lead isotopes On the outside there was a narrow superficial band of cuprite, filling the cavities. The corrosion penetrated into the interior in parallel plains and the oxide inclusions were flattened.

The analyses carried out by lead isotopes were centred on metal samples, and the results were:

The etching (Photo 20) exposed a dendritic structure totally distorted in parallel lines and also a very distorted recrystallised grain structure, produced by severe mechanical work.

La Pijotilla (P)

CD-24 The metallography was carried out on a section of a probable fragment of an arrowhead (Fig. 101). The sample had large superficial cavities full of cuprite and parallel lines of corrosion penetrating to the interior. There were scattered and flattened oxide inclusions. The etching showed the remnant of a very distorted dendritic structure with a clearly defined direction. Superimposed (Photo 21), appeared a completely distorted structure of recrystallised equiaxial grains, with strain lines, characteristic of a last phase of intense cold-working.

Pb 208/206

Pb 207/206

Pb 206/204

P10

2.08963

.85080

18.415

P15

2.08602

.84750

18.474

P19

2.09471

.85299

18.290

P20

2.09544

.85048

18.439

P21

2.03046

.82634

19.008

P25

2.08821

.85063

18.352

P26

2.09851

.85638

18.310

P28

2.10346

.85982

18.225

P29

2.09937

.85672

18.232

Photo 18. Metallography of axe CD-17 (Etched, x500). 169

Mark A. Hunt Ortiz

Photo 19. Metallography of saw CD-20 (Etched, x500).

Photo 20. Metallography of saw CD-23 (Etched, x1250).

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Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Photo 21. Metallography of arrowhead CD-24 (Etched, x500).

Photo 22. Metallography of fragment CD-29 (Etched, x500).

171

Mark A. Hunt Ortiz

Figure 102. El Trastejón. General plan (after Hurtado,1990-modified-).

172

Prehistoric Mining and Metallurgy in South West Iberian Peninsula upper strata belongs to the Late Bronze Age. It was the only zone in which these latter strata were preserved without severe alterations (HURTADO, 1992:179).

IV.2.2. Middle Bronze Age *El Trastejón (Zufre, Huelva)

The stratigraphic sequence of Square F-22, which is the one that will be followed when studying the cultural and chronological context, was defined by a diagram of stratigraphic units (abbreviated as UE or U.E.) (Fig. 104), in which these units have been grouped into two phases: Ancient (1600-1200 BC) and Recent (1200-800 BC), corresponding to the two cultural periods of occupation of the settlement and which serve as reference for the comparison of the productive evolution in their different aspects (HURTADO & GARCIA, 1994:240).

The El Trastejón (or simply Trastejón) archaeological site is located in the municipality of Zufre (Sheet 918, UTM:29SQC298009), on a hill hidden among others much higher, apparently related to the control of communication ways (HURTADO, 1992:176). El Trastejón, and also the Papúa site, are situated in a chain of hills closing to the N the Rivera de Huelva valley, exactly at the points where it is crossed transversely by two rivers, Hierro and Montemayor respectively. These mark natural passes which connect the above-mentioned Rivera de Huelva to the zone more to the N, with the Tierra de Barros (HURTADO & GARCIA, 1994:243). El Trastejón site is encircled by two concentric wall structures (Fig. 102), the upper delimiting an oval plateau (Upper Terrace: Squares C-1 and C-2), in which the excavation of 1988 was centred (HURTADO, 1991:372). The function of the walls would seem to be more in relation with the creating of a slope to sustain more space for habitation rather than with a defence system (HURTADO & GARCIA, 1994:243). Later excavations were centred on the Lower Terrace, where remains of metallurgical activities were documented (HURTADO, 1990:162-164), especially in the SW zone, where plenty of slag was found on the surface, as well as a grooved stone mining hammer (Fig. 103), also with no precise archaeological context (HURTADO, 1991:373).

Figure 104. Stratigraphic sequence of El Trastejón Square F-22 (after Hurtado & García,1994). The extreme radiocarbon calibrated dates obtained are as follows (GARCIA, 1996), although they do not correspond to the final nor initial strata: (RCD-447) 2030-1780 BC/ (RCD-445) 1220-930 BC. The finding of remains related, at least hypothetically, to the early metallurgical activity in El Trastejón was quantified. The slag appeared in the Lower Terrace, in almost insignificant quantities in the most ancient UE, while in the upper UE a great increase was detected, with its highest point in the surface UE of the Square F-22, where almost 23 kg of slags were collected (HURTADO & GARCIA, 1994:250). The ores, which are related in some way with the processes of transformation, were found, fundamentally, on the Lower Terrace and showed little variety: a small quantity of malachite and iron oxide nodules, much more abundant and which appear constantly throughout the whole of the stratigraphy.

Figure 103. Grooved stone hammer from El Trastejón. During the 1990 campaign new squares were dug in this zone. That known as F-22 (Fig. 102) to the SW, had, as one of its objectives, to find out about the metallurgical activity of the site (HURTADO, 1992:178) and it is in this Square F-22 that this study has been centred. It showed a stratigraphy starting in the Middle Bronze Age, while the

The increase of the ores, theoretically related to metallurgical activities, on the Lower Terrace, runs parallel 173

Mark A. Hunt Ortiz together with the slag, plenty of burnt earth, remains of furnaces and fragments of clay baked at high temperatures. The metallurgical activity extended along the whole of the Lower Terrace, which was deduced by the presence in Square 30 (Fig. 102) of furnace remains (HURTADO & GARCIA, 1994:246). Of these, one of the possible structures, containing two fragments of slag and burnt earth, cut through the strata of the Middle Bronze Age (HURTADO, 1992:181).

with that of the slags: in the lower levels they appeared very little and even did not appear at all, and progressively increased on reaching the more recent levels. A considerable increase was produced in the UE 20, the first of those considered to be transitional (HURTADO & GARCIA, 1994:250). In this quantification it must be taken into account the fact that all the few fragments of malachite, the pyrite and also the iron minerals that appeared throughout the stratigraphy, have been considered as ore, even though their final destination could be different to that of extractive metallurgy, as happens, for example, with the pyrite, which as it is in the form of a cylinder and decorated, should not be considered, metallurgically, an ore.

The information obtained from the Late Bronze Age phase is practically reduced to the intense use of the Lower Terrace for metallurgical activities, with metallurgical structures (HURTADO, 1992a: 469). As for the metallurgical function of El Trastejón and its relation with nearby mines, a note has been taken of its possible specialisation, exclusively extractive in the Late Bronze Age, with no dedication to metal production (the manufacture of objects), as there must have been other settlements in the area dedicated to this process (HURTADO, 1992:181), as for example the case of Puerto Moral, a site with melting moulds, while in El Trastejón there were only large quantities of slags (HURTADO, 1992:176).

The lithic material has also been studied in relation to the extractive processes (pounders, crushers,...) although this aspect should be studied more specifically, as well the as the relation of the fragments of adobe (HURTADO & GARCIA, 1994:251) with the metallurgical activities. As for the metal, it was surprising to find no remains connected with copper smelting/casting, and also the scarcity of metal objects, of which only one fragment on the surface, one in UE 4 (Late Bronze) and one in a Middle Bronze Age context were found (HURTADO, 1992:179).

Too, the possibility of a dependent settlement, more or less temporary, has been proposed at the mine of Cala, following the Chinflón model, which would supply the necessary mineral resources to El Trastejón (HURTADO & GARCIA, 1994:242). So, the hypothesis is put forward of a division of productive functions, within the miningmetallurgical activities, of contemporary settlements (HURTADO, 1992:176).

In general, as an evaluation of the site, and based on the first information obtained from the study of the materials from the two excavation campaigns, the following deductions were made (HURTADO et al., 1993:257; HURTADO & GARCIA, 1994:252): -An initial occupation occurred, dated in the first half of the II millennium BC, with little agricultural activity, and dedicated mainly to cattle raising and hunting. At that time the metallurgical activity is characterised by a very restricted production and a very primitive type of slag. The copper objects would be of arsenical copper.

El Trastejón was considered the first site in the Sierra of Huelva to have appeared in a mining context, and for that reason great possibilities of getting to know about the mining-metallurgical activities in the II millennium BC were envisaged (HURTADO, 1991:374). This must serve to contrast the hypothesis of the relation, traditionally used and with very little empirical base in this area, between the pattern of settlements in the II millennium BC and the exploitation of mineral resources (HURTADO & GARCIA, 1994:240).

-In a second phase of occupation, between the end of the second/beginning of the first millennium BC and the middle of the 9th century BC, there was a transformation in the use of the Lower Terrace, a specialisation in the extractive treatment of ore, judging by the remains associated with furnaces and the abundance of slags. This slag, also classified as copper slag, would be tapped. The metal analysed, on a surface level, was bronze. As for the Upper Terrace, it maintained its character as a habitation zone.

After having exposed the general considerations made by those who excavated this site, it is important to remark that during this study, after the detection of a “technological anomaly” and the subsequent revision of the materials from Square F-22, a Medieval/Modern intrusion was detected, reaching, from the surface, the levels of the Ancient Phase, and which was characterised by the presence of black tapped slag, related to iron smelting (which has been studied independently by Dr. Rovira and Dr. Gómez Ramos, Prof. I. Keesmann and Prof. V. F. Buchwald).

In general, the information on the possible smelting structures are very few: the Square F-22 gave most information, offering Middle Bronze Age oval structures containing some slags in their interior and which, although their function was not for habitat, neither did they offer evidence of metallurgical activity (HURTADO & GARCIA, 1994: 245).

Samples studied In the upper strata of Square F-22, belonging to the Recent Phase, there were (always according to the excavators),

As mentioned before, after insulating the strata affected by 174

Prehistoric Mining and Metallurgy in South West Iberian Peninsula Green globules (A) in the slagged walls (B)(Fig. 105). TR-13:(6/48-49-50) Fragments of slagged crucibles. One (nº 48) with a thick wall (2.1cm.) coarse temper-slate and quartz and light grey clay (A) (Fig. 105). Another (nº 49) also with a thick wall and coarse temper in the grey clay (B) (Fig. 105). Also two other pieces were analysed: a fragment of slagged crucible with grey clay (C) and a slagged rock (D).

the Medieval/Modern intrusion, the archaeometallurgical study of El Trastejón was centred on Square F-22: all the stratigraphic units (UE) were checked and all the information from the samples which could have any relation with mining and/or metallurgy was collected. It must be pointed out that the Recent Phase is treated here to give homogeneity to the explanation, although it is considered as belonging to the following stage to be treated, the Late Bronze Age.

TR-14: (9Cleaning7/4) Fragment of crucible. If its orientation corresponds to that of the drawing (Fig. 105) the slagged parts would be on the outside.

Thus, the samples chosen for analysis, marked as TR followed by its respective number, belong to the Square F22, excavated in the 1990 campaign. To each sample a new shortened number was given for its analytical identification. For the isotopic graphs the sign for samples from El Trastejón was reduced to T followed by the corresponding number.

TR-15: (15/15) Dark-red porous iron mineral. TR-25: (10/52) Two fragments of slag weighing 50 gr. When sectioned, showed abundant globular cavities covered with green copper leaching.

Also, in the following list, this identification is completed by the excavation reference (first the stratigraphic unit and then the inventory number) followed by the type of the sample in question. So, the sample TR-1 would correspond to a fragment of malachite from TR-90, F-22, U.E.39, Nº.Inv.7. In the isotopic graphs this sample would appear as T1.

TR-26:(25/7) Fragment of slag weighing 50 gr. Its interior showed porosity with green copper leaching. TR-30:(Surface. Zone SO.) Metal bent copper awl (weight: 15 gr.) (Fig. 105). TR-31:(4/Bag 1) Fragment of a metal object with copper as base metal. Possible handle (weight: 25 gr.) (Fig. 105).

The revision provided the following samples to be analysed, with the UE grouped according to their ascription to the Recent Phase and to the Ancient Phase:

TR-32:(12/46) Carved pyrite. Polished cylinder of pyrite (Fig. 105). Analysed in the interior (A) and on the outside (B).

TR-1:(39/7) Fragment catalogued as copper. In actual fact, the sample consists of very small fragments of malachite, well-formed, very fibrous and green coloured.

TR-33:(23/58) Catalogued as bronze metal. It corresponds to a metal fragment, perhaps part of the edge of an axe (weight: 25 gr.) (Fig. 105).

TR-2:(31/80) Catalogued as copper. They are in fact small fragments of ore with malachite and yellowish iron oxides, limonite type.

XRF The analyses by XRF (RLAHA) were the following (in %), organised by Phases and types (d: detected but not quantified).

TR-3:(23/60) Malachite weighing 25 gr. One single fragment with numerous globules in the upper side, pale green on the outside and the inside a well-formed malachite.

*Recent Phase

TR-5:(31/bolsa 33) Small fragment of malachite, showing iron oxides on the outside although in general it is fairly compact but of a pale green colour.

Metal TR-30.A TR-30.B TR-31.A TR-31.B TR-31.C

TR-6:(10/51) Inventoried as slag (weighing 50 gr.), it was found to be a limonite type iron ore, with the section showing these oxides, yellowish and earthy, with some malachite in the form of spots.

Fe 0.2 -0.2 0.2 0.6

Cu >90 >90 90 90 90

Sn 3.7 5.4 11.1 10 8.7

Mineral

TR-7:(20/6) Nodule of iron ore, similar to gossan. TR-15

TR-11:(7/ 54-55) Two fragments of crucible with an open form. There are slagged concretions in the interior surface. Grey clay and thick slate temper. One (nº 55) is a fragment of a wall (A). The other (nº 54) included part of the rim with a green globule (B) in the slagged wall (C) (Fig. 105).

Fe Cu 38.5 0.4

Crucibles TR-13.A TR-13.B TR-13.C TR-13.D

TR-12:(9/15) Fragments of crucible with part of the rim. 175

Fe Cu As 19.4 18.1 8.5 21.3 0.4 -25.7 7.4 1.9 14.2 0.3 --

Mn 1 0.9 1.8 0.6

Mark A. Hunt Ortiz

Figure 105. Metallurgical elements from El Trastejón.

176

Prehistoric Mining and Metallurgy in South West Iberian Peninsula *Ancient Phase

the central part of the awl (Fig. 105).

Metal

The surface was pitted by corrosion. In the section studied some porosity and numerous oval inclusions appeared, which seemed to be copper sulphides.

TR-33

Fe 0.2

Cu >90

As 3.1

Tin (Sn) has strong deoxidising properties, so that the oxygen associates with it, while the sulphur leaves the solution as particles of copper sulphide (Cu2S). These particles are common to all ancient bronzes.

Slag TR-25.A TR-25.B TR-26.A TR-26.B TR-26.C

Fe 8.8 1.8 5.9 21.9 31.1

Cu 23.6 2.0 22.1 8.0 12.2

As 7.8 1.6 3.1 1.6 0.6

Mn Ca 0.7 0.2 0.5 0.8 0.9 0.6 0.7

When etched (Photo 23) the sample showed a recrystallised grain structure and twin lines, produced in a final annealing, with no evidence of later cold-working. The absence of dendritic structure can be related with the use of a sufficient temperature (about 700º C) and time to achieve a complete homogeneity of this structure.

Mineral TR-1 TR-2 TR-3 TR-5 TR-6 TR-7 TR-32.A TR-32.B

Fe 1.5 12.2 0.5 2.7 16.9 31.9 20.6 39.2

Cu As Mn 51.6 28.9 2.2 48.9 42.9 27.7 0.1 D 18.3 2.4 0.4

Ca

TR-31 The section taken from the object (Fig. 105) showed the surface attacked by corrosion, mainly cuprite, which has an intergranular development, with circular porosity cavities and small inclusions of copper sulphides.

0.6

The etching of the sample (Photo 24) showed a homogenised structure of recrystallised grains with twin lines localised in certain zones, which showed restricted cold working or damage caused mechanically.

Crucibles TR-11.A TR-11.B TR-11.C TR-12.A TR-12.B TR-14

Fe 26.7 0.9 23.4 9.6 8.8 18.8

Cu As Mn 8. 4 1.3 3.0 38.7 2.7 0.3 0.4 D 13.2 5 D 4.0 1 D 10.5 1

Ca D D D

TR-33 The metallography was made on a section taken from this probable edge of an axe (Fig. 105).

D

Microprobe

The surface of the sample (Photo 25) was affected by corrosion with the spaces filled with cuprite. An intergranular extensive network of Cu3As was noted, far more visible with greater enlargement (Photo 26). It is a type of segregation, perhaps, formed by a precipitation at low temperature of the phase from solid solution, supersaturated after being homogenised at temperatures around 700ºC (communication from Dr. P. Northover).

Only the metal elements from El Trastejón were analysed by this method, giving the following results (in %): Recent Ancient Phase Phase TR-30 TR-31 TR-33 0.01 0.01 Tr Fe Tr Co 0.005 0.015 0.06 0.03 0.005 Ni 90.8 94.8 Cu 86.4 0.01 -Zn Tr 0.31 0.6 5.03 As -0.03 0.02 Sb 8.3 Tr Sn 13.05 0.04 Tr Ag 0.04 -0.03 -Bi 0.03 0.06 0.03 Pb 0.02 -Au 0.03

The etching (Photo 27) showed a recrystallised grain structure with twin lines. These grains, rather ellipsoid, showed slip bands, which resulted from a final cold working of 25-30%. TR-26

Metallographic examination has been made of all the metal samples from El Trastejón, as well as the slag sample TR26.

The metallography was carried out on a section of this very heterogeneous slag. Fayalite crystals were found, on a crystalline matrix. It is in this slag sample, of all those studied, where the highest number of metal globules were present (Photo 28), seen as round, brilliant inclusions of different diameters.

TR-30

XRD

The metallography was carried out on a sample taken from

XRD analyses were carried out on two samples from El

Metallography

177

Mark A. Hunt Ortiz

Photo 23. Metallography of awl TR-30 (Etched, x500).

Photo 24. Metallography of handle TR-31 (Etched, x500).

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Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Photo 25. Metallography of axe TR-33 (x125).

Photo 26. Metallography of axe TR-33 (x500).

179

Mark A. Hunt Ortiz

Photo 27. Metallography of axe TR-33 (Etched, x500).

Photo 28. Metallography of slag TR-26 (x500).

180

Prehistoric Mining and Metallurgy in South West Iberian Peninsula * Becerrero IV, Tomb 1: this cist was also undisturbed. The grave furniture, found 42 cm below the surface, consisted of a pottery bowl and a silver spiral, with a square section and thickened at one end (DEL AMO, 1975:142) (Fig. 106-1).

Trastejón, both pottery fabrics catalogued as crucibles, TR11 (Ancient Phase) and TR-13 (Recent Phase). The following compounds were detected: TR-11E: Quartz, Muscovite, Gehlenite (Ca2Al2SiO7) and Anorcite (CaAl2Si2O8).

This is the only silver object from this necropolis, which means that the analysis which is given must belong to it, although the reference in the Huelva Archaeological Museum happens to be El Becerrero I/Tomb 9; especially when this tomb 9 from Becerrero I, corresponding to Sector B, was excavated and did not contain any metal objects (DEL AMO, 1975:127).

TR-13 A: Albite (NaAlSi3O8) and Quartz . Lead isotopes Various lead isotope analyses were carried out on samples from El Trastejón (which in the isotopic plots are identified solely by the letter T, followed by the corresponding number) with the following results:

XRF The analysis of the silver object (PA7359) from El Becerrero gave (GOMEZ RAMOS et al., 1999):

El Trastejón (T) Pb 208/206

Pb 207/206

Pb 206/204

TR1

1.99478

.81133

19.399

TR3

2.04270

.80997

19.344

TR5

2.05342

.83749

18.703

TR32

2.09422

.85414

18.381

TR30

2.08898

.83847

18.667

TR31

2.09949

.85829

18.232

TR33

2.09289

.85263

18.362

El Becerrero (Inv.M.H:6633) 0.995 Cu 99.0 Ag nd Pb nd Au

* Gil Marquez Cist necropolis (Almonaster la Real, Huelva) This necropolis is 300 m to the S of the hamlet of Gil Marquez. Two cists were detected, and in their vicinity a Palmela type arrowhead was found (PEREZ & RUIZ, 1986:77) (Fig. 95), which has been interpreted as belonging to the earliest period of the Middle Bronze Age.

* Becerrero Cist necropolis (Almonaster la Real, Huelva)

XRF

This necropolis of cists was excavated by Mariano del Amo, who placed it in the area known as Coto de la Mora, some 15 km. to the S of the village of Almonaster. The necropolis is formed by various groups of cists, numbered Becerrero I to V (with 11, 18, 1,4 and 6 tombs, respectively).

The arrowhead gave the following composition (PA7345): Gil Marquez (Inv.M.H:6626) Tr Fe 0.09 Ni 98.75 Cu Nd Zn 1.02 As 0.017 Ag Tr Sn 0.055 Sb 0.04 Pb

The information of possible metallurgical interest can be resumed as follows (DEL AMO, 1975): Becerrero I,Sector A,Tomb 3: 2 pieces of slag in an immediate earth heap (from looting) (DEL AMO, 1975:125).

* Valdegalaroza Cist necropolis (La Nava, Huelva)

* Becerrero II,Tomb 10: on the ground in the cist, 3 fragments of slag that were considered to be contemporary with the cist (DEL AMO, 1975:136).

In the place known as Valdegalaroza, apparently in the municipality of La Nava (UTM: 29SQC004023) a necropolis of cists was discovered, of which neither the number nor the condition of the tombs are known, although it is definite that it was excavated by Mariano del Amo.

*Becerrero II, Tomb 12: small pieces of slag from the earth inside the cist (DEL AMO, 1975:137). * Becerrero II, Tomb 13: in the earth from the cist 3 pieces of slag were found (DEL AMO, 1975:137).

A large fragment of slag (about 7 cm), deposited in the Huelva Archaeological Museum (Inv.M.H:4402/7), seems to have come from one of these cists.

* Becerrero II, Tomb 15: this cist was discovered intact. During its excavation two small pieces of slag were found (DEL AMO, 1975:138).

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Mark A. Hunt Ortiz

Figure 106. Silver objects from Middle Bronze Age sites: 1. El Becerrero (Almonaster). 2. Calañas. 3. Dolmen del Carnerín (Alcalá del Valle). 4. Valdearenas (Iznajar). XRF * El Castañuelo Cist necropolis (Aracena, Huelva) The analytical results (PA7360) of the slag fragment were as follows (GOMEZ RAMOS et. al., 1999):

Situated near the small village of Castañuelo, this necropolis of cists was excavated in the 1970’s when two separate zones were established, Castañuelo-I and II. The first has 4 groups of cists with a total of 34 cists identified. In Castañuelo-II, 5 cists were excavated. Of all these, it was considered that more then 90% had been looted (DEL AMO, 1975:160).

Valdegalaroza slag (Inv.M.H:4402/7) Fe Ni Cu Zn As Ag Sn Sb Pb Ba Mn Ca Si

60.7 Nd 8.36 nd tr nd 0.06 0.03 0.34 0.22 1.9 2.1 12.0

Their excavation discovered no object related to metallurgy, nor any metal objects. It seems that, as has been reported textually, in earlier excavations carried out by Cerdán, only the existence of a few objects was confirmed, among which the most remarkable were 2 small gold bells (Inv, M.H.:6636/1 and Inv, M.H.:6636/2) and a small silver triangular dagger ferrule. It seems that these objects would be from the 182

Prehistoric Mining and Metallurgy in South West Iberian Peninsula 1991). The survey of this immediate orebody, which does not present this type of mineralization, together with the absence of both prehistoric metallurgical and mining remains in the site and in the mining area (see Chap. IV.1), leaves this affirmation with no base on which to stand.

necropolis, although its specific origin is unknown (DEL AMO, 1975:158). Also, in connection with the dating of those pieces, it must be mentioned that habitation archaeological remains of more recent date have been detected in the funeral area (DEL AMO, 1975:158).

* La Papua (Zufre/Arroyomolinos de León, Huelva) With the name of La Papua are known both the settlement and the necropolis of cists associated with it.

So, the dating of the gold objects is not at all sure. Their analyses made by XRF (PA) gave the following results (in %; Fe,Ni,As,Sn,Sb and Pb were not detected): El Castañuelo 6636/1 0.155 Cu 7.947 Ag 91.73 Au

The settlement is located on a height, surrounded by a 1 km. long wall, with an area of 14 hectares. A circular enclosure at the highest point appears to indicate the habitat zone. It dominated a fertile valley, today covered by the waters of the Aracena dam, and is considered one of the most important sites in the area of the Huelva Rivera (HURTADO, 1992a:466). The excavation campaigns carried out in 1994 found no evidence of metallurgical activities (HURTADO & GARCIA, 1995:239).

El Castañuelo 6636/2 0.193 10.48 89.33

The habitat site of El Castañuelo was excavated at a later date (DEL AMO, 1978) and was dated between the 4th and the 3th centuries BC, although the possible existence of a Bronze Age settlement has not been dismissed (DEL AMO, 1978:320,327). It will only be mentioned (as it is not within the chronological period being studied) that within this last phase of pre-Roman occupation, the only metallurgical activity in El Castañuelo, classified as silver related, was registered (DEL AMO, 1978:319), although that interpretation, judging by the analyses carried out (DEL AMO, Undated: 5; FLORES, 1981:42) is not appropriate.

In the vicinity of the settlement of La Papua, 11 cist burials were found, grouped in two areas, La Papua-I and II, still unpublished although they were excavated by M. del Amo decades ago. The cists presented a relatively rich and varied grave furniture, which has been related to a high rank sector of the population of the settlement (HURTADO & GARCIA, 1995:239).

An earlier settlement in El Castañuelo has also been defended by other authors, who mention the discovery by Cerdán of another gold button and a flat copper axe (Fig. 95-F) (PEREZ & RUIZ, 1986:73).

The metal samples from the La Papua cist necropolis analysed are: Papua I, (Nº inv. MH: 4398/1): Bracelet (PA7354) (PU1)

In a new survey, on the S side of the zone known as El Santuario, a 3-notched copper dagger was found (Fig. 95E), giving the composition (PEREZ & RUIZ, 1986:73-74; PEREZ, 1996:52):

Cu As Sb Bi Se Fe Pb Ni

Papua II, (Nº Inv.MH: 4398/10)(a): Spiral with three turns (PA7355) Papúa II, (Nº Inv. MH: 4398/10)(b): Spiral with three turns (PA7356) (PU2)

El Castañuelo Dagger 94.7 2.7 0.04 0.05 0.11 0.25 0.05 0.02

Papúa II, (Nº Inv. MH: 4398/10)(c): Spiral (fragment) (PA7357) La Papua, Cist 5. Metal sheet (PA7205) Papúa II, (Nº Inv. MH: 4398/9): Copper dagger (PA7346)

The chronology for the different occupation periods in El Castañuelo is ample, with a proposed first Middle Bronze Age (of Chalcolithic tradition) site, in which both the flat axe and the dagger should be placed. This was followed by other occupation phases in the Late Bronze, Iron-II and the Roman period (PEREZ & RUIZ, 1986:73-76).

XRF The XRF (PA) analyses carried out on various silver metal objects, today deposited in the Huelva Archaeological Museum, gave the following results (some of them published by GOMEZ RAMOS et al., 1999) (in %):

Regarding the Middle Bronze Age settlement, it has been affirmed that it could have been the metallurgical activity that led to the choice of this particular emplacement, due to the existence in the vicinity of an argentiferous lead mineralization known as Casa Santa (PEREZ & BEDIA,

La Papua Bracelet (PA7354) Spiral (PA7355) Spiral (PA7356) Spiral (PA7357) Sheet (PA7205)

183

Cu Ag 0.62 99.3 Tr 99.9 0.58 99.4 Tr 99.9 1.44 98.54

Pb nd nd nd nd nd

Au nd nd nd nd --

Mark A. Hunt Ortiz grave goods to be placed in the cists.

The analysis of the copper dagger gave (in % with no detected Ni, Zn and Sn): Dagger (PA7346)

Fe 0.039

Cu 98.22

As Ag Sb 1.59 0.12 0.003

The metal adhesions inside the cupel, which they analysed, gave the following figures:

Pb 0.025

La Parrita Cupel 613 ppm Pb 273 ppm Ag 204 ppm Cu

Lead isotopes Two samples excavated from La Papua cists (PU in the isotopic graphs) were analysed using lead isotopes:

They considered, doubtless, this cupel as part of the remains of a cupellation process (PEREZ & FRIAS, 1990:14).

La Papua Cist Necropolis (PU) Pb 208/206

Pb 207/206

Pb 206/204

PU1

2.19030

.85868

18.184

PU2

2.10077

.85846

18.222

XRF Some years ago, the occasion arose to study samples collected in La Parrita, which were then deposited in the British Museum. There were 5 samples on which semiquantitative analyses were carried out using XRF (ME, SE and TE= Main, Secondary and Trace Element): HP 515. Surface mineral: ME: Fe; TE: Pb

* La Parrita Cist necropolis (Nerva, Huelva) Another site to be considered is that known as La Parrita (also known as RT-63) in Nerva (Huelva), in the Rio Tinto mining zone.

HP 510. Sq.I, Layer 2. Described as argaric material, “casting slag”, in actual fact it consisted of 2 fragments, one was certainly gossan(a) and the other appeared to be so, too (b): (a) ME: Fe; TE: Pb, As (b) ME: Fe; TE: Ba, Pb.

There, on La Parrita hill, 8 cists were discovered in very bad condition. In the surrounding area stone axes and “Argaric” pottery were found, which were connected with the existence of a possible village on the hill. Afterwards, a small excavation trench was made in the hill, near the cists, where nodular fragments of slag and slagged crucible fragments were found, which were considered to have been used for silver metallurgy in the middle of the II millennium BC. (ANONYMOUS, 1981:2; 1984:2; BLANCO & ROTHENBERG, 1981:115).

HP 525 /Cist 4. Described as crucible. It was a fragment of light, grey pottery, which had some slagging on the inside face (a). Also in the section (c) it showed something which could be scorification (b): (a) ME: Fe; TE: Ba, Mn, Pb (b) ME: Fe; TE: Ba (c) ME: Fe; TE: K. HP 524 (1) Described as a cupel. It was the bottom of a pottery receptacle, of grey clay and very light. The analysis of its interior gave the following results: ME: Fe; TE: K, Ba, Pb, Ag.

More recently, further research was done on this site (PEREZ & FRIAS, 1990) based on samples collected by uncontrolled excavations of the tombs, including a piece of slag from Cist 6.

HP 524 (2) Described as a cupel. It consisted of a pottery rim: ME: Fe; TE: Ba, K. Then it was considered, in the absence of the quantification of the elements, that (although the nodular slag fragments turned out to be gossan), based on the information obtained, especially that from sample 524(1), in La Parrita some type of jarositic ore with appreciable contents of lead and silver could have been treated (HUNT ORTIZ, 1986:42-43).

The analysis of one of the slags, which was considered a prototype (PEREZ & FRIAS, 1990:13) gave the following results: La Parrita Slag Au 0.35 ppm Ag 1775 ppm 0.19 % Cu 0.22 % Pb 42.60 % Fe 22.00 % Si

* Alpizar Cist necropolis (Paterna del Campo, Huelva) In the farm with that name, a group of cists was discovered, of which no details are known except that it appears to have been excavated by Mariano del Amo, with no results published, and that some objects are deposited in the Huelva Archaeological Museum.

They considered that (because of the high percentage of silver and lead, this latter metal being used as a collector) they were silver smelting slags.

XRF

The finding of what they considered a cupel in the vicinity, together with the scarcity of slag fragments, was taken as being related to the specific work of the manufacture of the

Using XRF (PA) an analysis was carried out (PA7353) on a single object from this necropolis, probably an earring (Inv. Nº M.H 4410/1). The composition is (in %): 184

Prehistoric Mining and Metallurgy in South West Iberian Peninsula The halberd found in Cist-5 is typologically unusual among the grave furniture of the South-West. The piece had two perforations to ensure its handle by rivets, and weighed 301 gr. (Fig. 107-F). Only 5 other examples of this typology were known previously in the South of the Iberian Peninsula (SCHUBART, 1973): 2 of them from the cultural area of the Bronze Age in the South-West, from two cist necropolis near Faro (Portugal): Monte de Castelo (Fig. 107-E), with 1.5% As, and Campina (Fig. 107-D).

Alpizar Earring 0.22 Fe Nd Ni Cu 95.8 Nd Zn 2.95 As 0.035 Ag Nd Sn Nd Sb Nd Pb

Within the circle of El Argar, another of these halberds appeared in the “pithos” grave 575 of El Argar (Fig. 107-C) and another in the “marginal area” of Montejicar (Granada) (Fig. 107-B), with 4.3% As. The last known example was found, apparently, in the Ecija (Sevilla) area (SCHUBART, 1973:256) (Fig. 63-A).

Lead Isotopes This same object has been analysed using lead isotopes (denominated AP1 in the isotope graphs) with the following result: Alpizar (AP)

AP1

Pb 208/206

Pb 207/206

Pb 206/204

2.10254

.85499

18.596

AA Atomic Absortion analyses were made on two samples extracted by 2 mm. drilling (Fig. 107-F), one from the blade of the halberd and the other from one of the rivets.

* Huelva Province

La Traviesa Halberd Blade Rivet 97.7 Cu 97.4 0.06 0.07 Sn 0.003 0.003 Pb 2.47 1.88 As 0.03 0.03 Sb 0.007 0.28 Ag 0.01 0.005 Ni 0.007 0.02 Bi 0.03 0.03 Fe

In the Huelva Archaeological Museum there is an armlet whose origin, within the province of Huelva, is unknown (Inv.M.H:6635) of which the XRF analysis (PA7358) gave a 99.9% Ag content (with no Fe, Ni, Zn, As, Sn, Sb, Pb or Au detected). *La Traviesa Cist necropolis (Almadén de la Plata, Sevilla) In 1992 the first excavation campaign was carried out in this necropolis, in which 27 cist structures were detected. 17 were excavated, giving an extremely scarce grave furniture.

Metallography The metallographic study was carried out both on the halberd itself as well as on one of the rivets.

Of the 6 sealed tombs excavated in that campaign, 4 contained only a pottery vase, one contained a coral bead (Cist 13), and another, of those already disturbed, an iron oxide nodule (GARCIA & VARGAS, 1995).

*Halberd The metallography was carried out directly on the blade of the halberd, without extracting a section (Fig. 107-F:2). The halberd (Photo 29) presented a granular microstructure with little porosity. The grains, of a heterogeneous size, showed twin lines, rather distorted, and strain lines. So the halberd was cold-worked and annealed, after which it was again cold-worked, and left in that state. The intensity of the mechanical work could have provoked the fissures or folds detected.

In the 1993 excavation campaign (GARCIA & VARGAS, 1995), the Cist no. 5 was excavated, which was found intact. This grave was considered exceptional as being the only one, which had a ring of slate round it and a tumulus covering it. This grave was also an exception for its grave furniture, consisting of 2 pottery vases and a metal halberd (the only metal object found in the necropolis).

*Rivet of the halberd The metallography was carried out on a transverse section of one of the rivets. The polished section (Photo 30) showed an enormous quantity of porosities, some showing elongation. Also, the original dendritic structure was completely distorted by cold-working, with a very marked orientation.

The necropolis was related with the second phase of occupation of a nearby Copper and Bronze Age site, not yet excavated (GARCIA & VARGAS, 1992). The excavation results have been published in a monograph (GARCIA SANJUAN, 1998) The C14 date obtained for the necropolis was, calibrated, (RCD-2111) 1880-1670 BC (GARCIA, 1996).

Both the directionality observed and the distortion of the porosities are a reflection of the intense mechanical work to 185

Mark A. Hunt Ortiz

Figure 107. Middle Bronze Age halberds: A. Écija. B. Montejícar. C. El Argar. D. Campina. E. Monte do Castelo. F. La Traviesa (Almadén de la Plata).

Photo 29. Metallography of La Traviesa halberd (Etched, x100).

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Prehistoric Mining and Metallurgy in South West Iberian Peninsula

Photo 30. Metallography of La Traviesa halberd´s rivet (x50).

Photo 31. Metallography of La Traviesa halberd´s rivet (Etched, x400). lines. So, the internal structure of the rivet showed that it was subjected to an intense mechanical work by coldworking and annealing. The final process consisted of coldworking, which produced the distortion of the twin lines and the strain lines.

which the rivet was subjected. The etching (Photo 31) showed a recrystallised grain structure of quite an irregular size. Within the limits of the grains there were bent twin lines and, less evident, strain 187

Mark A. Hunt Ortiz burial in an artificial cave, the grave goods recovered suggested a date of the beginning of the Middle Bronze Age.

* El Carnerín dolmen (Alcalá del Valle, Cádiz) The dolmen is located on the plateau of Alcalá del Valle, within the general area of the western Sub-Betic hills. The collective tomb consisted of a stone-built megalithic structure open on one of its sides, defined as a short gallery of 2.4 m long, 1.3 wide, and 1.3 m maximum height. The grave furniture appeared around the bone remains of at least 8 individuals. It is considered a secondary collective burial. Ochre had been applied to the long bones.

This grave was named as Hipogeo-1, and consisted of a tomb excavated in the rock, with a circular chamber of almost 3 m diameter and a flattened roofing supported by a central pillar. The access was by a square shaft with two steps; the entrance opening at the bottom showing a lintel decorated with the symbols of the sun and the moon. The grave was partly looted and the material was broken and scattered, except in certain places. Some pottery types found, including Beaker pots, are related to the Copper Age, but the majority are plain and typologically related to the register of the Middle Bronze Age strata of the site (located in the same area) of El Berrueco (Medina Sidonia). The stone and metal objects found can be classified as impressive: 60 beads of variscite (“calaíta”), alabaster, malachite, bone and bronze; 2 big silver beads; 1 gold 2 and silver ear-rings; 2 riveted bronze knives with a curved blade, various fragments of bronze and silver spirals, 3 bronze awls and some other bronze fragments (RUIZ, 1990:383; 1992a:301).

The excavation recovered, together with a pottery bowl, the following grave-goods (MARTINEZ & PEREDA, 1991:66-69) (Fig. 106-3): -(PA0874) Silver armlet of 63 mm. diameter and 5 mm. thick -(PA0873) Silver armlet of 68 mm. diameter and 3 mms. thick. -(PA0872) Silver wire twisted into a spiral of 3 coils, with an average diameter of 15 mm. and 2 mm. thick. In a general valuation, El Carnerín is considered parallel to the megalithic necropolis of Granada, with grave furniture datable in the Bronze Age. In this case, mainly because of the presence of the silver objects (MARTINEZ & PEREDA, 1991:69). XRF

For the cultural ascription of the grave, it has been suggested the continuation of the Beaker culture up to 1700-1600 BC. (RUIZ, 1994:288), the period in which this hypogeum should be dated, although other authors have proposed a later date (LOPEZ et al., 1996).

The XRF analytical results of the 3 metal objects were already published, first partially (MARTINEZ & PEREZ, 1991:69), and later complete (MONTERO et al., 1995:101). The results are:

The provisional dating of the materials would be around the middle of the 2nd millennium BC. and possessing cultural links with elements of the Aegean Bronze, especially with regard to the metal materials (RUIZ, 1990:383-384).

El Carnerín Wire Spiral Armlet Armlet PA 0872 PA 0873 PA 0874 99.9 99.8 99.9 Ag nd tr nd Cu nd nd nd Pb nd nd nd Au

What is certain is that the silver objects which were analysed during this research are, typologically, completely different to the rest of the silver objects known in the Middle Bronze Age of the South Iberian Peninsula, showing a complexity in their fabrication far removed from the habitual, simple, solid forms (Fig. 106).

* Las Cumbres Necropolis (Puerto de Santa María, Cádiz)

The analysed samples from this grave (provided by Dr. Ruiz Mata) were the following (with the original description and inventory number):

This necropolis is situated in the Sierra de San Cristóbal, and in it more than 100 tumulus-type graves have been detected, presenting three different typologies (RUIZ, 1987:158-160):

TH-1 (B.1-C.1; nº inv. 31) Fragment of amorphous bronze TH-2 (B.1-C.1; nº inv. 32) Fragment of serrated bronze

a) Large-sized tumulus with incineration in pits. The metal grave furniture, including curved iron blades, would be dated in the 2nd. half of the 8th century BC.

TH-3 (B.1-C.1; nº inv. 34) 8 mm. fragment of a silver spiral, consisting of a 1 mm. thick foil forming a tube of 3 mm. diameter

b) Tumulus covering stone-built chambers dated from the 7th to 5th centuries BC.

TH-4 (B.1-C.II; nº inv. 74) Fragment of a silver spiral

c) Hypogeum type

TH-5 (B.1-C.II; nº inv. 75) Fragment of a silver spiral

Although no evidence of occupation has been found in the zone corresponding to Middle Bronze Age, precisely in one of the hypogeum-type graves (Hypogeum nº 1), a collective

TH-6 (B.1-C.II; nº inv. 76) Fragment of a silver spiral TH-7 (B.1-C.II; nº inv. 103-111) Two serrated bronze 188

Prehistoric Mining and Metallurgy in South West Iberian Peninsula Apart from the elemental distribution maps, two sets of quantitative data were obtained from the corrosion zone. The first of these corresponded to the average of compositions all along the length of the corrosion layer scanned. The second data group was obtained from a localised point of the centre of the line of scanning. The results are the following (in %):

fragments TH-8 (A.1-H.1; nº inv. 7) Amorphous edged bronze fragment, probably part of a blade TH-9 (A.1-H.1; nº inv. 8) Amorphous bronze fragment XRF The XRF (RLAHA) analyses gave the following results (with the elements not included, among them Pb, below the limits of detection): TH-1 TH-4 0.11 -Fe 2.4 Cu >90 1.3 -As ->90 Ag -tr Au

TH-5 Tr 0.1 ->90 --

TH-6 -0.2 ->90 --

C O Al P S Cl Ca Cu Br Ag Au

TH-9 tr >90 0.2 ---

Microprobe

Also, using the sectioned sample, the metal core (well away from the corrosion products) was analysed, with the following results (in %):

The analyses on 4 metal samples gave the following results: Fe Co Ni Cu Zn As Sb Sn Ag Bi Pb Au S

TH-2 6% Sn). The smelting of the copper ores with higher Sn contents could give alloys with various percentages of Sn. If they also contained As, part of this element could also pass to form part of the alloy.

It would be possible, rather, to consider the existence of not very reducing smelting conditions, at least in the initial smelting phase, which would produce the loss of large quantities of this element (MCKERRELL & TYLECOTE, 1972:217), but sufficiently reducing to produce FeO, and perhaps free Fe. In this respect, it has been considered that, in the primitive smelting processes, with very poor reducing conditions, the iron ores would not be sufficiently reduced to be incorporated as Fe into the copper being formed (CRADDOCK, 1985:137). But despite this, another deduction which comes from the examination of this slag AG-5 from El Amarguillo, is that the copper has been formed through its migration and aggregation in the scoriaceous and viscuous matrix, being forced to collect certain elements, such as Fe, which would make it necessary, in order to eliminate them, to carry out refining of the metal copper produced.

From the site of Amarguillo a series of samples, generically classified as “slags”, have been studied. Of these, with regard to the porous, light slags, sample AG-f did not present detectable Cu, sample AG-e only minor Cu content (0.15% Cu) as well as AG-2 (0.11% Cu).

This refining could be carried out in the moment that the copper produced, in more or less large globules (since it would not be separated from the slag during smelting), would have to be melted for its aggregation. This operation could be done in the moment that casting had to be carried out. That is to say, the aggregation, refining and casting could be done in one single operation. In any case, this melting or meltings of the metal would bring about a considerable loss of As (TYLECOTE, 1980:7).

However, the sample AG-3, which in its external analysis showed very low Cu content (0.11% Cu), in the internal analysis there were zones with high content in this element (up to 10.2% Cu). This gives an idea of the relativity of the representation of the analyses in specific areas in heterogeneous samples, in which the different elements are unequally distributed and with a tendency to concentrate in certain areas. The sample AG-5, however, is a different case and, as there are not much more analytical data for the South West, exceptional with regard to the Chalcolithic period. Its analysis showed that it contained large quantities of Cu (more than 35% Cu), with appreciable quantities of As (about 1.5%). Its metallographic examination (Photo 14) showed the presence of metal copper globules in a matrix, which included fayalite crystals. It is not a tapped slag, but from the information set out a series of considerations can be put forth.

A different vision, or perhaps rather a complementary one, can be obtained from the examination of the copper drops (“pingos”) from Joao Marques and also, it appears, in Santa Justa: they are rather globular, of about 1 cm and characterised by extensive porosity (GONÇALVES, 1989,II:229). They could correspond to copper formed directly in the furnace, in the least reducing parts where the free Fe is not formed, and so it would not be aggregated to the metal copper, as the analyses seem to indicate (GONÇALVES, 1989,I:481) by the absence of Fe, in contrast to the contents of some of the metal pieces, with abnormally high Fe contents (excluding errors).

The sample AG-5 is really a true smelting slag, although heterogeneous, so that it can be said that the copper ores used were not very pure: they contained elements which can be considered gangue, such as Fe oxides and silica.

VI.2.1.2.4. Moulds On the other hand, in the furnace charge would be the ores containing As, which in this case, from the analyses of the

The presence of moulds in any site is connected with 306

Prehistoric Mining and Metallurgy in South West Iberian Peninsula metallurgical production activities. As has been already mentioned, possible moulds were found in the sites of Valencina, La Pijotilla, Três Moinhos and Joao Marques and were interpreted as, apparently, used for the production of copper masses with a function still not defined. Moulds, which were definitely used for the production of metal artefacts, have been excavated in the sites of Joao Marques and Santa Justa. In Joao Marques a probable mould and another one, that certainly is, were recovered. This last one (AFC-2) is a mould for an awl which was found, together with other metallurgical elements, by the side of what was considered a smelting structure (GONÇALVES, 1989.I:157). It is an open mould made of clay and with negative shapes of awls in various faces (Fig. 132-1). From the Santa Justa excavation two moulds are also mentioned, later reduced to a probable mould of an awl, in grauwacke type rock. Although other functional interpretations have been put forward (GONÇALVES, 1989,I:283), its graphic representation offers no doubt whatever regarding its being considered an open mould (Fig.132-2). In the cases of both sites, the moulds were flat and open and not very clearly defined, so a considerable forging would be necessary to give the cast tool its final shape. From the rest of the geographical area being studied there is only reference to a mould in the Estacada de Alfaro site (Puebla del Río, Sevilla), excavated by Prof. Carriazo in the 1960’s. Its Chalcolithic date has been confirmed by the recent revision of the materials from the excavation (PELLICER, 1986a:246). Among the materials “a mould for casting bronze axes” was found (CARRIAZO, 1980:163,photo 9). It consists, according to the graphic documentation published and the notes which accompanied it, of a multiple, open mould, made of sandstone with a cubic shape, with the negative of a flat axe in the only face shown, although it is known there were others for “other pieces in the other faces”. Figure 132. Moulds from: 1. Joao Marques and 2. Santa Justa (after Gonçalves,1989).

Just as a reference, in the whole South East of the Iberian Peninsula, with many more excavated Chalcolithic sites, only four flat moulds have been found: for awls in Los Millares and for a dagger in Las Anchuras (MONTERO, 1994:231).

VI.2.1.3.1. Copper-Base Objects With regard to objects with a copper base, the principal analytical series carried out in the South West of the Iberian Peninsula, more exactly, in the Spanish provinces, are those of the SAM, those carried out on objects deposited in the British Museum (BM) and, with great quantitative difference, those carried out in the last few years by the Archaeometallurgical Project of the Iberian Peninsula (PA), while there are also some dispersed analyses in monographs and specific publications.

VI.2.1.3. Metal objects Only the use of two metals is well documented in the Chalcolithic period: copper and gold. Just a single and not very clear reference exists regarding the possible existence of an iron object in the final phase of this period.

307

Mark A. Hunt Ortiz It frequently occurs that many of the objects analysed (SAM and BM) lack a precise archaeological context, and only in some cases, with greater or lesser exactitude, their exact geographical origin is known.

As according to SAM but is reduced to 0.5% As in the PA analysis. The content of other elements is also higher in the SAM analysis (as in the case of Ni), while Fe is undervalued in comparison with the PA analytical data.

In the following sections the copper base metal objects, of which some technological data is available are treated, grouped according to their typology.

The study on the arrowheads from the Guadalquivir Valley concluded that the Palmela type arrowheads were made of Cu or Cu-As, and in only one case from Carmona (SAM 803) appreciable contents of Sn were detected, 1.35% Sn, which was considered to be within the limits of a fortuitous alloying (ROVIRA et al., 1992:276). In any case, the PA new XRF analysis of this arrowhead did not, surprisingly, detect any Sn.

VI.2.1.3.1.1. Arrowheads A basic reference for the study of this metal type is a work published on 76 examples from the Guadalquivir Valley (ROVIRA et al., 1992). Following the classification used by the above authors, three basic types are established: A and B (typical Palmela) and C (related), which are usually associated with the Beaker period, although with certain specific chronological prolongations. Type D is considered intermediate between type C and the last type, Type E, which is registered in Middle Bronze contexts and continues its evolution in the Late Bronze Age. Also the possibility is pointed out of a certain degree of coexistence of Palmela arrowheads with these later types (ROVIRA et al., 1992:269-270).

As for the elaboration of the arrowheads, and based on the metallographic studies carrried out, the conclusion were that the Type A arrowheads were cast and then cold worked, to give them their final shape and to harden them. Those of Type B show, in general, the same treatment, although in some cases they were also submitted to annealing. This combination of cold-working and annealing is more frequent in Type C, although cold-working is predominant (ROVIRA et al., 1992:227). The fact that both the arrowheads with As and those without this element received the same treatment, together with the circumstance noted of, in general terms, a progressive diminishing of the quantity of As until the introduction of bronze, lead the authors to suppose that the Cu-As alloying was not intentional.

In general, with regard to the analytical results obtained, an overvaluation of the As content by the SAM analyses has been noted. Since new analyses have been carried out by PA of samples from Acebuchal (Carmona) previusly analysed by SAM, the comparison of the analytical results can be made directly for individual metal objects from the geographical area in which this research study is centred. The results obtained in Palmela type arrowheads are the following (always, as in all the analyses, in % unless another figure is specified):

Since that work on the Palmela arrowheads in the Guadalquivir Valley was completed, some analytical results have been obtained from new samples from the South West of the Iberian Peninsula.

Fe Ni As Ag Sn Sb Pb SAM803 0.07 1.9 1% As. The axe edge fragment 384

Prehistoric Mining and Metallurgy in South West Iberian Peninsula In general, the number of Middle Bronze Age sites with evidence of copper metallurgy (and the volume of production) is considerably restricted in comparison with the Chalcolithic period.

examined metallographically showed and intense cold working in the final phase of the process in which annealing was also used. Also three axes (14% of the total analysed) dated to the Middle Bronze Age were made of bronze (two from the province of Huelva and one from Cadiz, in rather uncertain contexts), both arsenical (Arrabalde) and with low (Almonaster) or no As contents (Arcos de la Frontera). In these bronzes, with about 10% Sn, Pb was a minor or trace element.

The local metallurgical technology seems to be very similar to that practised during the previous period, based on the same ores, using pottery receptacles with similar types of slagging/glazing and a production of objects characterised, regarding their composition, by “erratic” contents of As, although with a general tendency to reduce its presence. The forging treatments continue to be essentially the same. On the other hand, there are certain signs which point to a relative progress and increase in specialisation, as would be the fabrication of specific forms for crucibles and, above all, the intentional appearance of copper alloys, both with silver and, fundamentally, with tin.

The composition of the binary bronze of the axes appears to represent a more advanced stage than that of the arrowheads, with compositions very near the ideal of 10% Sn, which results in an alloy which lowers the melting temperature, minimises the problem of gases and gives greater hardness to metal, without making it brittle.

The bronze objects were a relative minority (some metal types, such as awls and halberds, do not appear in bronze) and present a great heterogeneity in their compositions. The only site in which evidence of the presence of tin in the metallurgical material is recorded is Llanete de los Moros, which would be explained, as mentioned, by the use, since Chalcolithic times, of high tin content copper ores. But, in general, the bronzes of this period, with a very heterogeneous Sn content, even in the same site, must be considered as intentional alloys.

Among the daggers predominate those made of copper with highly varying quantities of As, with this element absent in only one case. Of the daggers analysed, 11% (2, from Alcalá del Río y Luque) were made of binary bronze, with similar Sn contents (11% and 12% Sn). The knives analysed were three examples coming from a single site, Hipogeum-I, and even so, show the diversity peculiar to this period: two examples were bronzes, with different proportions of Sn (14.5 and 7.7% Sn) and without any As. The third example was of copper, with only 0.3% As. Through the metallography carried out on the copper knife, it is known that, in combination with annealing, an intense cold working was employed, with a reduction of the original thickness, a state in which it was left.

In the South East, the appearance of bronze objects in the Argaric period does not seem to show a behaviour which makes it easy to explain its introduction for motives of technology or prestige (MONTERO, 1994:259). An aspect that could throw light on this circumstance would be the determination of the bronze local production or importation. In this respect, in the South West of the Iberian Peninsula (except for the low Sn bronzes which could be produced in Llanete de los Moros) there is no proof today that supports a local production of bronze. In this sense, the existence of placer resources of Sn minerals in the northern part of the Córdoba province cannot be forgotten, as well as in the Spanish provinces of Extremadura and in Portugal, where stone hammers have been discovered in the alluvial tin placers of Colineal, near Belmonte (MOHEN, 1992:110).

The swords/rapiers (4 analysed) were always made of arsenical copper, while in the case of the halberds, in one the As was under 1%. The halberds were also annealed and cold worked, in which state the edge was left. The awls were all made of copper with different As contents, between 0.4% and 4.7%. There is only one exception, an awl from Las Minitas, which contained 10%Ag. The chisels analysed, all from Alcalá del Rio, showed that this type was fabricated both in copper and binary bronze with low Sn contents (6 and 8%). A single saw analysed was of arsenical copper, while the group of various objects were composed of arsenical and non-arsenical copper, and also both of bronze with low Sn contents (5% to 8%) and higher Sn contents (11.8% and 10.3%).

Unfortunately, the isotopic analyses of copper-base objects have not included bronze objects of this period in the South West of the Iberian Peninsula and were centred on the earring from El Alpizar cist necropolis, two copper objects from Hipogeum I (L8 and L9) and one from El Trastejón (T33). Also 4 mineral samples from Ancient Phase layers of this latter site were isotopically analysed.

A new element which appeared in the Middle Bronze Age was the rivets for the handles, which usually have copper compositions (arsenical or not) different to that of the object, and which were in some cases made of silver or a silver alloy. The only one of this latter type analysed had no Pb content.

The earring from El Alpizar showed an isotopic composition that, despite its geographical proximity, is not consistent with the South Portuguese Zone deposits. In fact, it is not consistent with any of the characterised deposits. The two samples from the Hipogeum had isotopic compositions that point to diverse origins. L8 occupies an 385

Mark A. Hunt Ortiz at La Parrita and their qualitative analysis, drew the conclusion that there jarositic type ores could have been treated in some way or other, especially on the basis of traces of Ag and Pb (not quantified) which appeared in the scorifications of a fragment of a pottery receptacle. Later the Ag and Pb contents of the scorifications were analysed quantitatively, and again the production of Ag and cupellation was proposed. However those results did not show the concentration of Pb and Ag which appears, in even considerably larger quantities, in the oxidised surface ores of the nearby and huge Rio Tinto ore deposits. That is to say, no metallurgical concentration of Ag was detected, and there even exists the possibility of the confusion of gossanized ores with true metallurgical slag, which means that a study of the phases of the samples would be necessary.

intermediate position between mineralizations from the South West and the Eastern Mediterranean, without being consistent with either of them. L9, also a low arsenic copper, is consistent with mineralizations from the OssaMorena Zone, particularly with La Sultana, although it is also consistent with some from the Eastern Mediterranean, in this case, Crete. As for El Trastejón, starting with the ore samples, the malachite T5 is consistent with Cala and La Sultana mineralizations, as well as the carved chalcopyrite piece, which is consistent with Cala. The other two malachite samples, T1 and T3, are not consistent with any of the characterised mineralizations of the South West. Again one is reminded of the anomalous character of the ore deposits of this particular zone.

While the minimum quantities of Cu make it difficult to establish the significance of these samples from La Parrita, the trace quantities of Pb will not allow their connection with cupellation. What is evident is that it would be necessary to carry out an integral analytical study, not just elemental, of these adherences and the other remains from La Parrita, in order to succeed in knowing their true nature. So, the data at present available regarding La Parrita (also with dating problems) offer no evidence whatever which supports, neither the use of Pb as a collector nor cupellation. Even, strictly speaking and considering the geological context in which the site is located, there is not even conclusive proof of the metallurgical activity itself, for the production of silver.

The only metal sample from the Ancient Phase of El Trastejón, number T33 (arsencial copper), has an isotopic composition consistent both with Cala and La Sultana mineral deposits. Another important novelty of the Middle Bronze Age is silver. Silver is a metal that appeared for the first time during the Middle Bronze Age in the Southwest of the Iberian Peninsula (as also occurs in the South East, with a function connected with personal prestige, although in some cases, as the rivets, it could be also for functional purposes). In the area under study silver has been registered both as a component metal in objects, always in funeral contexts, as in rivets for copper base weapons. Also, as an exceptional case, silver appeared alloyed with copper in the awl from Las Minitas necropolis.

As has just been mentioned, the composition itself of the silver objects of the Middle Bronze Age in the South West Iberian Peninsula excludes silver elaborated using a metallurgical technology based on the use of lead and cupellation.

In general, silver can be considered a very scarce metal in the South West Iberian Peninsula: less than 30 examples (including the 13 examples from a single grave, Hipogeo I) are known from the southwestern Spanish provinces. This is even more obvious if it is remembered that in the South East more than 460 silver objects (without counting the silver rivets) were registered some years ago.

On the other hand, the argument has been put forward that it is wrong to date in the Middle Bronze Age the metallurgical activity of silver production detected both in Cerro de las Tres Aguilas and in San Platón. Technologically, neither could the remains from La Parrita site be related to those of these two other sites, which, in any case, are to be dated in the later Orientalizing period.

In all the cases analysed in the South West Iberian Peninsula, once having determined that no differentiated loss of Pb has been produced by corrosion, silver is characterised, whether it is alloyed with Cu or not, by the absence of Pb. The absence of this element, lead, would exclude the hypothesis of producing Ag by means of the reduction and cupellation of lead-silver ores. The Cl content detected in the internal metal phase (without corrosion) of the sample TH-3 from the Hipogeo 1, could provide a connection with the use of native silver or silver ores of the cerargyrite type, or both together.

With regard to the ore deposits of the South West in which the existence of native silver or silver ores have been registered, no evidence of their prehistoric exploitation has been found. Thus, the possibility of the importation of silver to the geographical area that is being studied has been considered, backed also by the results of lead isotope analyses of a reduced set of silver metal samples from the Hipogeum-I site (4 samples) and La Papúa (2 samples).

As have been explained, based on analytical results not published, local silver metallurgy was proposed for the 2nd millennium BC in La Parrita (Nerva), a site situated in the Rio Tinto mining area. Without forgetting that no excavations have been made there and that the relation between the metallurgical samples and the cist is “geographical”, a later revision of the metallurgical remains

Regarding the silver samples from the Hipogeum-I, it can be affirmed that the origin is diverse. The comparison with specific mineralizations has proved the isotopic consistence of a sample (L3) with the mineralizations of Linares. Those 386

Prehistoric Mining and Metallurgy in South West Iberian Peninsula peninsular gold deposits, it appears that the gold used was alluvial in origin and would not be alloyed, while the major technological difference with the previous period is considered to be the appearance of cast gold objects.

numbered L4 and L5 are not consistent with any of the mineralizations isotopically characterised. The sample L6 is consistent with the Monte Romero mineralization but also with the Sardinian mineralization of Rosas-Sa Marchessa. From the isotopic results of the two samples from La Papua a similar situation to that of the Hipogeum can be deduced: the two of them have different origins. The sample PU1 is consistent with the mineralization of a La Carolina. The sample PU2, for its part, is consistent with an ore deposit in the South Portuguese geological zone, Aznalcóllar (and Paterna) but also with the same deposit as that of the sample L6 from the Hipogeo, that is, with the Sa Marchessa deposit in Sardinia.

VII.6. PRE-ORIENTALIZING LATE BRONZE AGE MINING AND METALLURGICAL TECHNOLOGY The mining technology of this period appears perfectly reflected by the results of the archaeological excavation in Chinflón mines, characterised by the use of grooved stone hammers, of Type 4a. However, the dating of the majority of mine workings that have any resemblance to Chinflón, is uncertain.

So, the lead isotope compositions of the South West Iberian Peninsula silver samples analysed showed that they have diverse origins, which in some cases seems to suggest relations with other zones of the Iberian Peninsula (the mineralized fields of the province of Jaén) and even of the Mediterranean (Sardinia) which, as has been explained at the beginning of the chapter, showed overlapping isotopic compositions with some mineralizations in the South Portuguese Zone. In this case, rather than the possibility of establishing definite conclusions, the isotopic results clearly indicate the lines of future research.

Summarising and bearing in mind the data from the archaeological register, it is considered that the mining technology documented in Chinflón would not be exclusively of the Late Bronze Age and that similar workings, dated only generically, could have been exploited during earlier, or even later, periods. The types of stone mining tools which appear in workings which are or could be of this period, showed that in the same exploitation various of the types classified were used, related, to a great extent to the characteristics of the material employed. The stone industry, which was studied in San Enrique exploitation for example, has shown the predominance of modified pebbles of volcanic origin, especially those of the andesite group. The modification consists almost exclusively in the making of a simple transversal groove (Type 4a) with only one case of double groove (Type 4b). More than 80% of the examples weighed between 700 and 2500 gr.

Regarding the cases in which iron has been mentioned in connection with Middle Bronze Age contexts, mention has already been made of the possible dating in the late Beaker period of an iron awl, not analysed, described in El Acebuchal. Also, in the excavation in the site of Alange reference has been made to two samples classified as being related to iron production, in Middle Bronze Age layers. For both sites, the possibility was put forward of an intrusion from later levels, as was the case of the iron tapped slags excavated in El Trastejón. In this latter case, they were even interpreted as the result of unsuccessful attempts at silver production (PEREZ MACIAS, 1996:209), this being included as an argument supporting the hypothesis of the local production of silver in the 2nd millennium BC.

The mine workings of Chinflón, although they reach a certain depth (more than 10 m) are restricted to following the mineralised vein, and are narrow and prolonged, without developing into galleries.

Summing up, no clear evidence exists for the production or use of iron in the South West of the Iberian Peninsula.

The depth reached would entail the use of illumination, which would be obtained by the use of small open pottery lamps, and of a system of hoisting the ore, and also the sterile, as well as the miners themselves.

Another metal documented in the South West Iberian Peninsula Middle Bronze Age is gold. From this period gold objects are very scarce and continues, with regard to composition, the Chalcolithic models, although the objects, now, are not exclusively laminar, with also some cast examples appearing. The gold would be coming from placer deposits, with silver contents that can be high and, in some cases (such as that of the earring from Hipogeum), with values of more than 1% Cu, which is considered by some authors as an intentional alloy (an experimental phase previous to its extensive use in the Late Bronze Age (ROVIRA & MONTERO, 1994) although others consider it natural (HARTMANN, 1978).

The tree trunks with notches made in them and the possible wooden crosspieces in Chinflón, as well as the alternating hollows registered in the vertical walls of a number of the shafts would also be used to cover these needs. But the use of more complicated hoisting systems has also been recorded, probably made with tree trunks which would be placed and fixed in the hollows registered on the surface of some of the shafts (as in 3B in Chinflón, or the Mines 6 and 9B of the Sierra de Tejada). This hoisting system would need the use of more perishable materials, which have not survived, such as vegetal ropes or leather. Of the auxiliary tools employed only an oval wooden shovel has been registered in the Mine 3B in Chinflón.

So, without counting on a minimum data bank of the

The waste, which sometimes was accumulated in the parts 387

Mark A. Hunt Ortiz Setefilla, La Saetilla or Cerro Muriano. In El Trastejón very impure copper carbonate was registered (UE3) and in El Llanete de los Moros the ores which have continued to appear since Chalcolithic times, characterised by their Sn content of between 1 and 2%, are still being used during this period.

of the mine already exploited, more for practical than ritual reasons, would be taken to the surface by the hoisting system which would also serve to drain the mine. This waste normally formed heaps at the mine entrance, and should be considered an integral part of the archaeological site. The information they contain, not only of ore and rock remains, but also of mining tools and other types of elements has been confirmed clearly by the excavation of some mines (as is the case of Cwmystwyth, in Wales).

The information available on the use of metallurgical furnaces in the Pre-Orientalizing Late Bronze, although in some cases with chronological uncertainty, has been deduced from the remains registered in the Mansegoso site (nº.27). These would be of the “bowl” type and with characteristics defined as very primitive and associated with furnace viscous slag, of the same type as that found in Chinflón and in the Mansegoso site (nº.28).

There are a great number of workings in the South West of the Iberian Peninsula, which, as has just been mentioned, show similarities to the Chinflón exploitation. In all the cases it appears that they were dedicated to the exploitation of copper ores, oxides and carbonates.

In the case of Chinflón and Mansegoso (nº.28), in which Late Bronze Age dated pottery was also found, that synchronism does occur, but in general it must de borne in mind that this type of fayalitic slag appears since Chalcolithic times in the South West of the Iberian Peninsula. Consequently, this technological criterion, alone, would not be sufficient to establish a precise chronology.

But together with them, another type of working appears, especially in the Sierra de Tejada, more open and less deep, also associated with the same type of stone tools, which had the present-day aspect of a very small opencast mine. While most of the mines are characterised by the lack of development of galleries, there are some examples where the same technology was used that, if they did not develop, strictly speaking, true galleries, used a system of successive shafts opened very close together with galleries communicating them. A good example of this system is Mine 8 in Sierra de Tejada.

The crucible fragments which also appear in the Recent Phase layers of El Trastejón, corresponded to open pottery shapes, with adherences, related with copper smelting or a first refining of the copper nodules, which showed that during the Late Bronze Age, in this site, although in small quantities, arsenical copper was produced. These crucibles showed a greyish paste (as the ones from the Ancient Phase) with a predominance of aluminium compounds, which are also detected in a crucible from Mine 9 in the Sierra de Tejada. These kinds of pastes in the crucibles have appeared from the Chalcolithic period and it would be interesting to find out their true archaeo-metallurgical significance, which, as has been mentioned earlier, would need special research work.

The lack of the practice of shoring up with pit-props would be the reason for the strong tendency, which is notable in prehistoric mining, not to make galleries. The miners would bear in mind very strongly the risks attached to this type of mining (as can be deduced by the human remains found associated with grooved hammers, in Rio Tinto, Peñaflor, Chinflón and perhaps, Potosí, mines). With regard to ore concentration, at this moment, the most reliable information also comes from Chinflón, both from the excavation of the mines and of the settlement connected with the exploitation. There, specific types of tools have been excavated, such as Type A mortars, with a single hollow, and spherical pounders which would be used for the preparation of the ore, and, it has also been suggested, to crush the slags and to recover the copper nuggets trapped in them, something which would be perfectly acceptable. In the experimental test carried out within this research study, the copper globules trapped in the slag were separated mechanically with no difficulty whatever.

There is another small series of sites (Map 6) which have offered crucible remains (some not analysed), connected with copper metallurgy according to the scorifications they had, both with reduction (Cerro del Depósito site) and production (Cerro del Hornito, and from the XIIa stratum in Setefilla, considered by some authors already Orientalizing). As been mentioned before, the Chinflón slags and those from the Mansegoso sites, as well as the fragments from some of the mines in Sierra de Tejada, are fayalitic but not tapped. Neither were the copper slags from the Cerro del Depósito, Sierra de la Lapa and Cerro de San Cristóbal. No details are known, apart from the fact they are classified as slags, about those recovered in the stratum XIIa of Setefilla (IX-VIII centuries BC) and those of the Late Bronze Age strata in Saetilla.

However, the Chinflón model, which is built on the finding of specific tools for ore concentration, has not to be considered unique, since it has been also documented in another series of mines in which, apart from the grooved stone hammers, Type A mortars and pounders also appeared. In Cerro Muriano, with the mining exploitations nearby, the ore dressing would be carried out in the settlement itself, also using specific stone tools.

Of importance to metallurgical production, in that XIIa stratum in Setefilla, in a period immediately before the Phoenician Colonization or, according to other authors, already within that period, and for the first time in the

The copper ores exploited would consist fundamentally of oxides and carbonates, as registered in sites as Chinflón, 388

Prehistoric Mining and Metallurgy in South West Iberian Peninsula the South West Iberian Peninsula. The third example of a chisel from Encinasola is binary bronze (9.7% Sn). In El Trastejón, the only object excavated from the Recent Phase (TR31) is a binary bronze (8.3% Sn) with some As content (0.6%). The metal object (TR30) found on the surface of this same site shows a similar composition, although with higher Sn (13% Sn).

Southwest of the Iberian Peninsula, a tuyere was registered. Summing up, in all the sites with metallurgical activity related to copper, the remains analysed indicate that the production was centred on copper or arsenical copper on a very reduced scale, using a simple technology, similar to that of the earlier periods, without using tuyeres and without producing tapped slag, although it appears that the fayalite slag is a common by-product, which would indicate probably a more systematic adding of suitable fluxes to the furnace charge.

The Portuguese settlement of Sao Bras showed a similar technological succession: copper and arsenical copper in the Chalcolithic period, with the exclusive appearance of these same metal compositions in the Middle Bronze, while in layers of the Late Bronze Age a bronze object was recovered.

In this general technological context, the tuyere from the problematical stratum XIIa of Setefilla, could be considered as one more of the numerous examples which are recorded in the South West of the Iberian Peninsula in relation to the Phoenician influence, already within the Orientalizing period.

The compositions of the local metallurgical productions remains in El Trastejón, of copper/ arsenical copper, and the composition of the metal objects, of bronze, allow the imported character of the latter to be deduced. This is a model of the general situation detected, as has just been mentioned, in the whole of the South West. Even Llanete de los Moros, the only site in which a possible production of Sn (which is started in the Chalcolithic period and which is due to the use of copper ore with a high content of this element) has been detected, showed a similar behaviour: the information available indicates, apart from the fact that production would be on a small scale, that the ores used would not justify the production of bronzes with high Sn contents, which is precisely the composition of the objects corresponding to that period excavated there.

With regard to the Ag/Pb slags which have been considered as belonging to the Pre-Orientalizing Late Bronze Age, the dating has always been based on data collected during field surveys, as those from Sierra de la Corte, with porous furnace slags, or the free silica slags from Pozancón. However, the information supplied by the archaeological excavations show that the Ag/Pb metallurgy is always related to Phoenician influences, even just by a single fragment of orientalizing pottery appearing together with the common hand-made pottery. Even the absence of wheel-made pottery is not a determining factor to consider a specific stratum as not belonging to the Orientalizing period; for example, Level 3 of Corta Lago 26A, has only hand-made pottery, while the previous chronological Level 4, has wheel-made pottery, although only a fragment.

It would be superfluous to set out again the compositions of all the objects, almost all of an absolutely new typology, which appear in the Late Bronze Age, forming, fundamentally, hoards, in which arms predominate, related in many cases to water courses and that have been interpreted in many different ways (RUIZ GALVEZ, 1995).

Thus, it is defended that the slags reflecting an extractive silver technology related to the use of lead as a collector must be considered as belonging to the Orientalizing period. Having treated the raw material used and the by-products which originated from the metallurgical activities during this period in the South West, now what will be considered are the characteristics of the metal objects registered: copper and its alloys, gold and iron, the only three documented metals, although rather scarce with regard to iron, at that period. There is no information of any silver object whatever.

Only it is to be remembered in a general way that the bronzes are mainly binary. Ternary bronzes only appear very occasionally, with about 2% Pb (with the exception of the axe from Mérida containing 25% Pb). The Huelva Hoard gives an idea of the calibre and the impulse with which this new metallurgical reality imposed its methods, producing a definite break with the local metallurgical tradition and inducing the thought of veritable metallurgical standardised production centres, which does not correspond in any way with the panorama of metallurgical production offered by the local archaeological register of the South West of the Iberian Peninsula.

With regard to copper and copper alloys, it is necessary to point out the lack of elemental metal analyses, apart from those objects from the groups known as “deposits” or hoards, which characterise this cultural period and which are considered to give a certain partiality to the general interpretation.

As some authors have pointed out (FERNANDEZMIRANDA et al,. 1995:59) and in view of the absence of the production of bronzes and its regular and permanent appearance, it is thought that, already from that period, the South West Iberian Peninsula would be included within a regular commercial network.

Of the 3 chisels from Encinasola, two are of arsenical copper and follow the models seen in the previous period. These are the only two Pre-Orientalizing Late Bronze objects analysed which are not bronzes, although, as has been seen, the production of copper/arsenical copper (always with the exception of the unintentional production in Llanete de los Moros) is the only one detected locally in

In other geographical zones, technological reasons 389

Mark A. Hunt Ortiz the others in this wide geological zone of the South West under study. This circumstance is in accordance with the archaeo-metallurgical register of the region, set out above.

(improved casting, better quality of the metal produced without the need of forging afterwards) (MCKERRELL & TYLECOTE, 1972:209) and also medical (PATTERSON, 1971) have been used to justify the rapid change from an arsenical copper metalwork to bronze. This latter hypothesis is based on the probable poisoning suffered by the metallurgists connected with the production of arsenical copper (HIEGER, 1949; JHAVERI, 1954; HARPER, 1987). Intoxication by arsenic is a possibility that is not unreasonable to suggest that it could have occurred among the metallurgists of the Chalcolithic and Bronze Age (even when not considering arsenical copper an intentional alloy). Certainly a considerable volatilisation of As would have been produced in the smelting of some high arsencial ores, such as the ones excavated in Amarguillo site, and as also in the later mechanical/heat treatment. However, local production still continued for a long time after the appearance of bronzes.

One of these groups could be related to the mineralizations of the Central Mediterranean, specifically, the Sardinian Sa Duchessa, although only one of them, RH2, is strictly isotopically consistent with it. The second group of compositions, rather more dispersed and formed by RH3 and RH5, has an isotopic composition close to the mineralizations of Cyprus, although strictly they are not consistent with them. As for the two samples from El Trastejón, the surface find T30, occupied a similar, although differentiated, position to that of the second group of the Huelva Hoard. This sample is consistent with the Cala mineralization, although this orebody possesses an isotopic field which can be considered anomalous and needs further investigation.

The metallographies that have been carried out on the objects of the Huelva Hoard, especially on the swords, show a very bad quality of the cast, with many inclusions and bubbles due to the lack of degassing facilities. Besides, the forge treatment, combining cold working and annealing, continued to be used, especially on the cutting edges.

The sample T31, excavated in the UE 4, showed an isotopic composition that is within the area occupied by the South Portuguese Zone orbodies, being consistent with Aznalcóllar, Monte Romero and Paterna. However, this sample is also consistent with another orebody, from Sardinia, Sa Marchessa.

In general, in the case of the South West Iberian Peninsula it does not seem that the arrival and implantation of bronze can be explained exclusively because of technical improvement factors. Quality seems not to be a factor of excessive importance, a circumstance seen in the cast and also in the presence of ternary bronzes (even swords), although rather limited in that area. The addition of lead, precisely with respect to the swords, has led to the proposal that they would be weapons used rather for military parades than for warfare, which could also be extended to at least some of the unleaded swords in the Huelva Hoard. That non-utilitarian function would allow the technical oversight recorded.

Its possible foreign origin, especially bearing in mind the isotopic results of the other samples and the local production, must be considered in future research work. If the bronze objects in the Huelva Hoard are of a foreign origin then, in principle, that same origin must be given to the iron object that appeared there. It seems that, leaving out the doubtful cases from El Acebuchal and Alange, no iron objects are recorded in the South West of the Iberian Peninsula from before the arrival of the Oriental Semitic influences, although it is true that more and more ancient evidence is being recorded of iron objects. From the initial belief of the introduction of iron in the Southwest of the Iberian Peninsula in the 8th century BC by the Phoenician colonisation (PELLICER, 1989), the research today, is presenting proofs of the existence of this metal in periods before that colonisation, although connected with it (ALMAGRO-GORBEA, 1993: RUIZ-GALVEZ PRIEGO, 1995; LOPEZ AMADOR et al., 1996).

The results of the lead isotope analyses, although rather scarce, confirm the foreign character of the bronze production. The only samples that have been analysed are those from two archaeological sites dated in this period: the Huelva Hoard and El Trastejón. From the Huelva Hoard, two spearheads (RH1 and RH2), two ferrules (RH3 and RH4) and a sword (RH5) were isotopically characterised. The first affirmation that can be made is that the samples do not have a single mineralogical origin, being grouped in two different compositive regions, with no relation whatever to the typology of the objects.

The confirmation of the presence of Mycenaean pottery in the archaeological register of the South West of the Iberian Peninsula from the 14th-13th centuries BC, and even earlier (MARTIN DE LA CRUZ, 1992) cannot be forgotten. In the Central Mediterranean, this influence, documented since the 16th-15th centuries BC (VAGNETTI, 1992), has been related with the appearance of iron metallurgy.

Besides, not one of these samples is consistent with the isotopic compositions of the mineralizations of the South Portuguese Zone.

The gold objects detected, apart from their larger size and their being found in treasure hoards, do not seem to show any technological changes with regard to earlier periods.

So, it can be concluded (based on the isotopic data available) that the ore used in the manufacture of these arms did not come from the enormous polymetal orebodies of the massive type, such as Tharsis or Rio Tinto mines, nor from

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Prehistoric Mining and Metallurgy in South West Iberian Peninsula globules. These technical conditions, even worse than some objects studied from hoards, must have made the sword so fragile that it would be no use for practical purposes.

VII.7. ORIENTALIZING PERIOD MINING AND METALLURGICAL TECHNOLOGY The mining tools continue to be the same as in the previous period, with predominance of the Type 4 stone mining hammer, though not exclusive. Perhaps the only new type, accepting its connection with mining and not mineral dressing, such as concentration or preparation, is that represented by a unique example from Los Castrejones (Aznalcóllar) in which the handle is fixed by means of the carefully prepared butt (Fig. 115).

The suggestion could be put forward that the demand for these types, with no great technical requirements, would instigate its being copied in local workshops, a context in which the bivalve mould from Ronda could be situated. With the absolute predominance of bronzes in this period (with some relation in the use of different alloys according to the object to be produced) and without a single evidence of their being produced “locally”, it is in Castillo de Doña Blanca, a colonial site, in which the first metallurgical remains related with the production of bronze in the South West Iberian Peninsula have appeared.

If the tools used were inherited from previous periods, this is not the case with mining where transcendental changes are detected, both in mineralogical orientation and in the type of workings.

The most transcendental change in the Orientalizing period, which embraces all the different ambits of metallurgy and which leads to exercise a direct control of the mineral sources, occurs in relation with silver production.

With regard to copper metallurgy, this continues to be practised in interior sites, which can be considered as exceptional, such as Setefilla, based on specimens of secondary copper ores (cuprite in this case). The bulk of the remains have been found, although badly described and defined, in coastal sites. In general, the use of copper-based objects, recovered from habitation and funeral contexts, can be considered as widespread, with a great variety of types.

Within mining, the surveying of these minerals is the first activity to denote an important qualitative and quantitative change: from searching for ores which were identifiable visually (copper oxides and carbonates, iron oxides) to the surveying of argentiferous ores which can, or cannot be, contained (without, it seems, the possibility of a visual distinction) in ore specimens formed fundamentally by iron oxides, namely, the jarosite ores.

Although there are very few objects (Tejada la Vieja, Castrejones and Huelva) that are not bronzes, bronze is the characteristic composition of the copper-based objects in this period.

The confirmation of the existence of interesting quantities of silver would have to be made by additional methods. The case which shows most clearly the mechanisms used in this new stage is that of the Hondurillas mine. This is a mineralization without Pb, marked on the surface by gossan outcrops. However, at the mine entrance fragments of free silica type slag were collected, which were characterised by high proportions of Pb and the absence of Ag. Given the mineral composition of the orebody there is no doubt that the lead was taken there. Based on this information, it was considered that the slag would correspond to the remains of an assay (using a fairly large ore sample and foreign lead as a collector) of the minerals from Hondurillas to test its silver content.

Those bronzes are both binary and ternary, as occurs in La Joya, Cancho Roano, El Gandul, Tejada la Vieja or Huelva, where in the excavation of Puerto-9, together with other bronze objects (10) both leaded and unleaded, obeloi were recovered, considered commercial products and evidence of the importation of metal to this site. They are low tin bronzes. In Castrejones, of the 9 copper base objects analysed, only one, AZ14 (a socketed arrowhead) was not made of bronze and was submitted, in combination with annealing, to an intense mechanical working, which was the last treatment applied. The binary bronzes (6) from Castrejones show diverse Sn contents: the hilt of the Sa Idda type sword had 10% Sn, a socketed tip, 17% Sn, and the rest of the objects less than 8% Sn.

The question could arise, in view of the scarcity of Cu in this mineralization, of the possibility that the workings detected there correspond to, rather than a mineral exploitation, workings from mine surveys in search of an argentiferous mineralization. With the data available this could only be a hypothesis which would need the excavation of Hondurillas mine to come to more definite conclusions.

The tip (AZ15) studied metallographically, showed a mechanical treatment combined with annealing, whose final phase was light cold-working. The two ternary bronzes, with high lead contents, were a clasp representing a Hathoric head (28% Pb) and a fragment of a sword blade (AZ10). While it is not unusual to find high quantities of lead in the cast clasp, attention is called to the composition of the sword for its high lead content (18.2% Pb and 7.8% Sn) and the bad conditions of the casting, in which state it was left as shown by the metallography, which besides allowed clear confirmation of enormous porosities and considerable segregated lead

If this were so, it would reinforce the idea of a sort of “silver rush” in this period, with prospector/miners capable of dedicating a considerable effort with only the possibility (not the certainty) of finding a rich argentiferous lode. There are data from some other lode type mines in the Sierra de Tejada, which would support the possibility of 391

Mark A. Hunt Ortiz contrast to their scarcity in Tejada la Vieja. This is presumably because of the lesser extension of metallurgical activity and perhaps, also, because of the preparation of the ore at the mines themselves, where the Type A stone mortars, pounders and even hammers reused as mortars, frequently appeared. The structure classified as an ore washer in this Tejada la Vieja cannot be considered as such. The same situation was registered in San Bartolomé de Almonte site and the same interpretation can be put forward, but the preparation of the ores in the mining areas would not always be the case, since in the site of Huelva, Type A mortars have also been recorded.

their having been exploited (or tested) not only as copper mines but also as silver mines. But where mining effort is centred at this period is in the zone of concentration of the argentiferous jarosites of some of the massive sulphide deposits, which characterise the Volcanic-Sedimentary Complex of the South Portuguese geological Zone. This demonstrates knowledge of the formation conditions of that type of mineralization. For their exploitation, mining becomes more horizontal, using the exposed flanks of the geological formation. This would be the case of the mine working system detected in the Ancient Mining Zone of the Aznalcóllar opencast, and also the working, known as the “protohistoric gallery” in Corta Lago.

From the charge of some of the furnaces excavated in Huelva, connected with silver metallurgy, it has been positively confirmed that the ores would be well and extensively crushed before being introduced into the furnace.

In Aznalcóllar, the exploitation system, of which only the most eastern part remains, shows considerable dimensions and complexity. Even bearing in mind the bad state in which they are to be found today, the inspection of their interior gave an opportunity of obtaining a view which has nothing in common with that of mining works of the Chinflón-type mines.

The silver furnaces documented in this period seem to correspond to two types. One would be of a small size, excavated in the ground in the shape of a bowl (as in Cerro Salomon and those from the Corta Lago section). The other type, of which the function is not clearly known, would be circular (Huelva and Casetillas examples) of ample dimensions, with a low wall as a base and probably a dome and a chimney. It appears that it would not be functioning with tuyeres, but probably with a draught system. The existence in them of a system of discharging the metal produced has been also proposed. These large furnaces are always connected with the production of free silica type of slag, which, as seen in Casetillas site, would be formed inside the furnace.

The jarosite ores from these massive sulphide deposits would always be characterised by their fundamentally iron oxide composition and, although they are very heterogeneous and some lots could have a greater content, for their reduced proportion of Pb (the average of the Castrejones ores is 2.7% Pb, in San Bartolomé the highest content is 2.7% Pb and in Tejada 1.4% Pb) and also heterogeneous Ag contents. To extract silver it would be necessary to use lead as a collector and as this element appears in such small quantities in jarosite ore, that lead would have to be imported to the smelting sites, probably already as a metal. On the other hand, while not a single piece of evidence has been found of mining exploitation of deposits containing silver minerals/native silver, the Monte Romero mine and silver smelting workshop show that the polymetal argentiferous ore, with a high Pb content, was used for silver production. In this case, it seems that it would not be necessary to add foreign lead, as would also indicate the results of the lead isotope analyses.

Tuyeres, can be considered an innovation introduced in this period. They became common and present diverse typology, Types A, B and C, of which their different functions have been mentioned. As a reference and an argument for placing the arrival of metallurgical innovations together with the Eastern influence, at the site of Apliki, in the centre of the mining district of Cyprus, twelve tuyeres, dating from the 13th century BC were found mixed amongst copper smelting slag (MUHLY, 1991:183). They corresponded to the three types established in the South West of the Iberian Peninsula (although those of type C had only a single orifice).

It is possible that the free silica type slag from Casetillas might be related to the exploitation of a small silver outcropping in that area, where silver slags have also been detected, as in the Sierra de la Corte site.

The slag connected with silver production in the Orientalizing period is of two types. The tapped slag, which only appears in Corta Lago and Monte Romero, can be considered as exceptional and in the latter of the two sites mentioned it was considered as having been produced by re-smelting the free silica slag.

Regarding ore concentration, it would be carried out, basically and according to archaeological records, using hollowed stone mortars, both Type A, with a varying number of hollows, and Type B. Associated with them are the stone pounders, both spherical and cylindrical. The number and diversity of these that appeared in Castrejones show their frequent use and the amplitude of the metallurgical activities on the site.

It is unfortunate that, despite having been excavated on various occasions, there is not a clear sequence available, supported by analytical studies, of the technical evolution of Corta Lago section. Of what was once a huge and exceptional metallurgical site, now there are only a few

The high number of these stone types in Castrejones is in 392

Prehistoric Mining and Metallurgy in South West Iberian Peninsula 1-That it was recycled, as can be presumed from its storage in Monte Romero.

square metres left, with neither certainty of the origin nor the types and volumes of the slag that existed, nor their metallurgical relation...etc. It is not even known whether the Orientalizing tapped slags appear on their own, in what proportion and with what other remains, for example litharge, they were related. The discussion has been centred on dating rather than the technological evolutionary sequence itself.

2-That it may not have been identified. Its elemental analysis would only show the presence of the element Pb, which means it could have been classified as metal lead. For instance, until its XRD analysis during this research, the litharge fragments from Castillo de Doña Blanca, of considerable size, were considered as lead.

The Orientalizing period habitual silver slag is the furnace slag, both free silica type and, in less numerous sites and in smaller proportion, that which does not contain visible quartz, and which, in any case, usually accompanies the former.

As an alternative interpretation, the hypothesis can be proposed of a division of functions in the sites, at least in a first moment. Cupellation would be carried out, judging by the quantity and size of the litharge found, on a scale that could almost be classified as a real industry, in the Castillo de Doña Blanca site, round about 800 BC, for which it would be necessary to have a solid supply organisation, set up previously. Contrariwise, not one fragment of litharge has been described as coming from sites with great silver metallurgical activity, such as San Bartolomé de Almonte, Tejada, Aznalcóllar or Peñalosa.

Free silica type slag has been recorded in more than 25 Orientalizing sites in the province of Huelva and the western part of the Seville province (Map 6), in geographical relation to the South Portuguese Geological Zone mineral deposits, except in the case of Las Casetillas, for which there is no certainty regarding with which mineral deposit it should be related.

Lead drops are usually habitual, both with high and low Ag contents. The appearance also of perforated lead disks is frequent, as in Cerro de las Tres Aguilas or Cerro Salomon, in Rio Tinto, Aznalcóllar (AZ4 containing 0.36 Ag) or Tejada la Vieja. In the Carambolo site these lead disks have been considered as weights used for fishing nets (CARRIAZO, 1980:292). These lead objects, whatever their function, are assumed to be the first evidence of the use of this metal for making objects in the South West of the Iberian Peninsula.

Apart from the homogeneity of their visual appearance, within a pronounced heterogeneity, they have the same compositive models: they are Ag-Pb slags resulting from the application of a specific extractive technology, based on the application of lead as a collector, of argentiferous ores, fundamentally, but not exclusively, of the jarositic type. This is a governing characteristic of the technology of silver production in the Orientalizing period: the use of lead as a collector.

Metal silver, very scarce in the Middle Bronze Age and that is considered not cupelled, probably imported (the same as would be the fragment of coral from La Traviesa cist grave), is absent during the Pre-Orientalizing Late Bronze period and it is only in the Orientalizing period when it is extensively recorded.

Unlike earlier periods, in which lead does not appear at all in connection with silver (lead is only known as an alloy in the “imported” bronzes), in the Orientalizing period lead becomes ubiquitous and is present in all its forms and at all process levels: metal or as litharge or other oxides, in the ore, in the slags, in the crucibles, in the cupels and also in the metal silver itself.

In this latter period is when the first examples of silver containing significant proportions of lead appear in the South West of the Iberian Peninsula, which is considered evidence of silver production by cupellation. Together with these examples of silver with Pb there also appears a series, which is quite large, of silver with no detectable Pb, which would indicate that silver from a different technical origin is still being used, perhaps from silver ores or native silver.

The most abundant type of pottery related to silver metallurgy is the scorified pottery, which is usually of common open shapes. The composition of the scorifications seem to indicate that they would be used in refining activities, previous to the actual cupellation. The use of these pottery receptacles is also recorded, since the 8th century BC in Castillo de Doña Blanca, always with high Pb content and sometimes high proportions of Ag.

A clear example of the relation Ag-Pb and the application of cupellation comes from Aznalcóllar. The fragment of the ingot (AZ2), with dendritic structure, found there, contained 25% Pb and 1.6% Cu. This is an unrefined silver which would need to be cupelled to obtain a refined metal similar in composition to the earring (AZ2), with a cold-worked structure, found in the same site, with only 180 ppm Pb and 807 ppm Cu.

This duality, which also occurs in the chronologically later site of Monte Romero, where cupels and scorified pottery appeared, would support the function proposed for these latter objects. The only complete cupels recorded are those from Monte Romero, whose original paste had been completely substituted by litharge. In all probability, the scarcity or lack of this synthetic Pb oxide in many sites can be explained by two factors:

The major analytical effort of this research in the field of lead isotopes has been centred on the remains related to silver metallurgy in the sites belonging to the Orientalizing 393

Mark A. Hunt Ortiz

In general, the results obtained are of great interest and reflect the situation with regard to a basic technological point: the necessity of importing lead into the South West Iberian Peninsula in order to carry out the silver metallurgy. This situation is not surprising after knowing the lead content of the jarositic argentiferous ores.

The interpretation of the isotopic composition which the samples analysed present seems to be evident: to the local ores foreign lead would be added, which would produce a silver (and some by-products) with an isotopic composition different both to the local ores and to that of the mineralization of the foreign lead employed, whose origin will have to be studied by future research and for which here possible lines of action have been laid down.

This does not deny that there may be sites, such as Monte Romero, in which the ore composition (polymetal high in Pb) would make unnecessary the addition of foreign lead, and even in the same jarositic mineralizations there would be specific areas with higher Pb contents.

It is a crucial aspect for isotopic studies in the Mediterranean area to know that the silver produced in the South West of the Iberian Peninsula would not have the same composition as that of the ore deposits which were exploited here.

This last possibility would be confirmed by the isotopic composition of the principal group of eight litharge samples from Castillo de Doña Blanca, which were consistent with the Volcanic-Sedimentary ore deposits, namely, those of Aznalcóllar and Rio Tinto.

As for the specific case of the Cerro de las Tres Aguilas, the elemental and isotopic composition of the slag samples place it in this technological context, characteristic of the Orientalizing period; another argument contrary to the proposed, much earlier, date for the production of silver on this site.

period.

From Huelva, only the sample H1 (a litharge) was consistent with the Aznalcóllar and Rio Tinto isotopic fields, while the other two samples (free silica slags) were not consistent and had an isotopic behaviour similar to the metallurgical silver related samples from the other sites. These litharge fragments, isotopically consistent with the local mineralizations, can be connected with a single free silica sample (CS3), from Castillo site, consistent with the Aznalcóllar ore deposit. This sample is, in actual fact, an exception, but shows that, occasionally, silver was produced in Aznalcóllar without the need to recur to foreign lead.

To a hypothetical initial monopoly of the technology of cupellation, would have to be added, as has already been put forward, a control of the indispensable raw materials for the production of silver, in this case, lead. The demand for metal from the coastal centres would be an important factor for the new organisation of the territory and also for a new relation with the mineral resources (WAGNER, 1983:14-15). But that relation, as has been seen, would not be of a single direction (of exportation), being introduced through those commercial centres, together with other products, both raw material (lead) as well as manufactured goods, both in bronze, or in silver itself or in gold, in whose elaboration considerable changes are noted, both in the use of alloys with copper as in the introduction of new “jewellery” techniques (like granulated and filigree work), and whose distribution has been related with highly Orientalized contexts and commercial lines of interchange (PEREA, 1991).

None of the other samples of free silica slag from Aznalcóllar area of this period is isotopically consistent with the mineralization. That situation, the inconsistency of the isotopic compositions of the metallurgical remains with the local mineralizations isotopic field, is repeated in all the sites isotopically examined, such as San Bartolomé de Almonte, Peñalosa, Tejada la Vieja, Cortijo de José Fernandez, Aznalcóllar, and Huelva.

The iron objects, a metal which became common in this period, could also be connected with the commercial activity of the coastal centres, which in other Southern Iberian geographical areas seem to be specialised in their production, as in Toscanos or El Castellar, with a technology characterised by the non-production of tapped slag.

The case of Cerro de las Tres Aguilas is especially significant for the early dating which has been proposed for it. The lead isotope analyses of three free silica slag samples showed, in the first place, their inconsistency with the Rio Tinto mineralization isotopic field. On the other hand, they have a composition similar (although not consistent with any of the mineralizations studied) to the rest of the samples from the other archaeological sites: they are grouped in an isotopic zone in which a lot of mineralizations appear, such as those of Jaén and the Central Mediterranean, especially Sardinia, which with some specific samples are consistent.

The colonial offer, that together with bronze introduced iron tools at an early date, could have led to the stopping of the “traditional” metallurgical production in Chinflón or El Trastejón. It seems, regarding iron, that only from the 8th century BC was a certain local production recorded, as would have occurred in the sites of Setefilla or El Carambolo, although this aspect is uncertain, based solely on the finding of slag (not analysed) classified as iron slag, and some fragments of iron ore, haematite, which in the case of El Carambolo is

The context and location of the Orientalizing silver producing sites makes it absurd to suggest a possible alternative to the use of local argentiferous ores as raw material for the silver metallurgy carried out there. 394

Prehistoric Mining and Metallurgy in South West Iberian Peninsula described as a triangular prism, which, perhaps, indicates it non-metallurgical character. They could be rather forging than reduction slags, as it appears that would be the case of the sample HU3, from Huelva.

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Chapter VIII BIBLIOGRAPHY AMBERT, P. and BERGE-MAHIEU, P. (1991) Les Mines Préhistóriques de Cabriéres (Hérault). En: Découverte du Métal: 259-277. Picard Editeur, Paris.

ACOSTA MARTINEZ, P. (1995) Las culturas del Neolítico y Calcolítico en Andalucía Occidental. Espacio, Tiempo y Forma, Serie I,8: 33-80. Revista de la Facultad de Geografía e Historia. UNED. Madrid.

AMORES CARREDANO, F. (1988) El yacimiento arqueológico de Cortalagos (Riotinto, Huelva): datos para una síntesis. Actas del I Congreso Internacional Cuenca Minera de Río Tinto: 741-753.

AGRICOLA (1556) De Re Metala. H.C. HOOVER & L.M. HOOVER Translation. Dover Publications, New York.

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