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The Lead and Copper Isotopic Composition of Copper Ores from the Sierra Morena (Spain)

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The Lead and Copper Isotopic Composition of Copper Ores from the Sierra Morena (Spain) ISSN (print): 1698-6180. ISSN (online): 1886-7995 www.ucm.es /info/estratig/journal.htm Journal of Iberian Geology 35 (1) 2009: 59-68 The lead and copper isotopic composition of copper ores from the Sierra Morena (Spain) Análisis de los isótopos de plomo y de cobre de los minerales de cobre de Sierra Morena (España) S. Klein1, C. Domergue2, Y. Lahaye3, G.P. Brey1, H.-M. von Kaenel4 1Institut für Geowissenschaften, Facheinheit Mineralogie – Petrologie und Geochemie, J.W. Goethe Universität, Altenhöferallee 1, D-60438 Frankfurt a. M. (Germany) [email protected] 2 T.R.A.C.E.S (UMR 56 08 CNRS), Maison de la Recherche, Université de Toulouse-Le Mirail, 5 allée Antonio-Machado, F-31058 Toulouse Cédex 09 (France) 3 GTK Geological Survey of Finland, Betonimiehenuja 4, 02151 ESPOO (Finland) 4 Institut für Archäologische Wissenschaften, Abt. Archäologie und Geschichte der römischen Provinzen sowie Hilfswissenschaften der Altertumskunde, Grüneburgplatz 1, D-60629 Frankfurt a. M. (Germany) Received: 3/10/07 / Accepted: 18/11/08 Abstract The paper presents lead and copper isotope analyses of 51 copper ore samples from the Sierra Morena, South of Spain. They are from ancient mines of the Iberian Peninsula collected by Claude Domergue during various field campaigns in the central Sierra Morena from 1965 to 1975. Most samples consist of copper oxide minerals such as malachite, azurite and chrysocolla and stem from the surficial sections of the ore deposits. The aim of the study was to supplement the existing reference data bank on lead isotopic compositions of ancient copper mines from the Iberian Peninsula. This is particularly important for the Sierra Morena for which data exist mostly for lead-zinc but not for copper ores. The lead isotope ratios range from 18.165 to 19.712 (206Pb/204Pb), 0.797 to 0.859 (207Pb/206Pb) and 1.955 to 2.108 (208Pb/206Pb). Two separate fields can be distinguished with a major field intermediate between the ore deposits from SW and SE Spain and a second at higher 208Pb/206Pb values. Copper isotopes were analysed additionally to provide further constraints for provenance studies. The copper isotope ratios δ65Cu of the copper oxide samples are mostly positive and higher on average than those of sulphide minerals. They are a potential tool to distinguish between either sulphide ore or oxide ore deposit derived artefacts. Keywords: lead isotopes, copper isotopes, mass spectrometry, Spain, Sierra Morena, copper ores, archaeometry Resumen En este artículo, presentamos los resultados de los análisis isotópicos (plomo y cobre) llevados a cabo sobre 51 muestras de mineral de cobre de Sierra Morena, Sur de España. Las muestras provienen de minas antiguas de la Península Ibérica, que habían sido recogidas por Claude Domergue en el curso de sus prospecciones en Sierra Morena central, entre 1965 y 1975. La mayoría de 35-1.indb 59 08/01/2009 9:20:43 60 Klein et al. / Journal of Iberian Geology 35 (1) 2009: 59-68 las muestras consiste de minerales de óxido de cobre como malaquita, azurita y crisocola que se encuentran en la superficie de los depósitos. El objetivo de este estudio es de contribuir a la base hoy disponible de datos de isótopos de plomo de las antiguas minas de cobre en la Península Ibérica. Este objetivo es particularmente importante puesto que la mayoría de los datos publicados de Sierra Morena se refieren a minerales de plomo-zinc. Las proporciones de isótopos de plomo varían entre 18.165 y 19.713 206Pb/204Pb, de 0.797 a 0.859 207Pb/206Pb, y de 1.955 a 2.108 208Pb/206Pb. Se pueden distinguir dos zonas independientes: una zona principal que se sitúa entre los depósitos de España del sudoeste y sudeste y una segunda zona con las proporciones de isótopos de plomo más altas. Además, los isótopos del cobre fueron analizados para suplir restricciones adicionales en los estudios de proveniencia. Las propor- ciones de isótopos de cobre, δ65Cu/63Cu, fueron analizadas en los óxidos de cobre y son en la mayor parte positivas y mas altas en medio que las proporciones δ65Cu de los sulfuros de cobre. Los resultados presentan un instrumento eficiente para distinguir los artefactos elaborados de minerales de sulfuros de cobre o de minerales de óxido de cobre. Palabras clave: isótopos de plomo, isótopos de cobre, espectrometría de masas, España, Sierra Morena, mineral de cobre, ar- queometría, . 1. Introduction riano (District de Córdoba), Zumajo (District of Los Pe- droches) and are known to have continuously produced Mining in the South of the Iberian Peninsula has been copper in Roman times. They are presumably the source intensive since the Bronze Age. The Romans maintained of copper for the famous copper production of Córdoba, high mining activities from the end of the second cen- the aes Cordubense, also called aes Marianum (Pliny tury BC to at least the beginning of the III century AD the Elder, Naturalis Historia, 34, 4). Aes Marianum was (Domergue, 1987; Domergue, 1990; Domergue, 1998). named after S. Marius, who was the owner of this mining Rio Tinto within the Pyrite Belt in the Southwest almost estate at the beginning of the Roman Empire (Domergue, appeared to be the unique centre of copper production in 1990). The Sierra Morena deposits produced mainly lead, ancient times within the whole of the Iberian Peninsula, silver and copper. The development of visible gossans on but other mines in this pyritic ensemble (i.e. Tharsis, So- the surface of the copper deposits testifies to their long tiel-Coronada, São Domingos, Aljustrel) have also pro- term exploitation. The remains of ancient mining activi- duced copper and silver. ties can be observed in situ in the form of tailings, mining It is also known that the numerous copper rich vein de- tools, ceramics, etc. posits of the Sierra Morena in Central South Spain have In archaeometallurgy, lead isotopes are applied for been exploited reaching back to the beginning of the provenancing the raw materials of metal objects by com- Bronze Age. The larger copper deposits in this area are paring the lead isotope signatures of ores from known Los Escoriales (District of Andujar-Montoro), Cerro Mu- deposits with those of the metal objects. However, prov- 2.12 Sardinia 2.11 SW-Spain Sardinia 2.10 SW-Spain Pb 2.09 Tuscany 206 SE-Spain Aegaean Pb/ 2.08 Isotope gap: No data 208 Cyprus Sardinia available in literature or lack 2.07 Cyprus of deposits? 2.06 0.83 0.84 0.85 0.86 207Pb/206Pb Fig. 1.- Reference lead isotope diagram 207Pb/206Pb versus 208Pb/206Pb. Lead isotope fields derived from published lead isotope data of ores from the Mediterranean area. Fig.1.- Diagrama mostrando las relaciones de los isótopos de cobre Pb207Pb/206Pb versus 208Pb/206Pb. Los campos de los isóto- pos de cobre provienen de aquellos datos publicados de las menas del área mediterránea. 35-1.indb 60 08/01/2009 9:20:43 Klein et al. / Journal of Iberian Geology 35 (1) 2009: 59-68 61 50 km Fig. 2.- Map of Southern Spain indicating the locations of the ore samples. The sample numbers refer to Table I. Map based on C. Domergue’s Catalogue des mines et des fonderies antiques de la Péninsule Ibérique. Cartes et plans hors texte (1987). (IPB: Iberian Pyrite Belt, OMZ: Ossa Morena zone, CIZ: Central Iberian zone; OVD: Los Pedroches sector, exocontact batholite, PBT: Los Pedroches sector, inner batholite occurences, AAC: Alcudia-Almadén-Castuera). Not referenced in this map is the LMZ (Lusitan-Marianic zone): this northern limit of the OMZ is still continuously under discussion and modification (de San José et al., 2004). Fig. 2.- Mapa del sur de España indicando las localizaciones de las menas de las muestras estudiadas. Los números de las muestras están referidos en la Tabla 1. El mapa está basado en “Catalogue des mines et des fonderies antiques de la Péninsule Ibérique. Cartes et plans hors texte (Domergue, 1987). IPB: Cinturón Pirítico Ibérico, OMZ: Zona de Ossa Morena, CIZ: Zona Centro Ibérica, OVD: Sector de Los Pedroches; contacto exterior batolítico enance studies can only be successful, when the refer- 2. Geological Setting ence data bank is complete. During the accumulation of published lead isotope data of Mediterranean copper The south central Spanish ore deposits are divided east ore deposits a significant lack of data for central Iberian to west into occurrences from the Central Iberian Zone deposits became apparent together with a seeming gap (CIZ), the Ossa Morena Zone (OMZ) and the Iberian in a lead isotope ratio diagram (Fig. 1). Roman copper Pyrite Belt (IBP) (Fig. 2). Our samples were mostly ob- coins analysed by Klein et al. (2004) plotted within this tained from the Central Iberian Zone and a few from the gap of the reference data bank and were interpreted as a Ossa Morena zone. They are the main tectonic units of the mixture of ores from two deposits. Scarce new data from Hercynian Iberian Massif (Gibbons and Moreno, 2002). Los Pedroches (cited in Rico et al., 2005-2006), however, The contact between CIZ and OMZ is a NW-SE trending provided lead isotope data in the vicinity of these coins. feature whose nature is not completely understood (e.g. This prompted us to embark on a more comprehensive Expósito et al., 1999; San José et al., 2004). study of the mines in Central South Spain and especially CIZ consists of three major sub-zones: 1. the central of Sierra Morena. Los Pedroches Batholith complex (PBT), 2. the exo- 35-1.indb 61 08/01/2009 9:20:44 62 Klein et al.
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