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Lead Isotopes and Archaeometallurgy

Lead Isotopes and Archaeometallurgy

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Lead isotopes and archaeometallurgy
F. Cattin
B. Guénette-Beck 
M. Besse
V. Serneels
Published online: 16 September 2009
Springer-Verlag 2009
This special issue presents several studies applying leadisotope analysis (LIA) to address archaeological questionsin the field of ancient mining and metallurgy. They were presented during an international workshop, held inFribourg (Switzerland), June 19
20, 2008, organised incollaboration between the Geosciences Department of theUniversity of Fribourg and the Laboratory of PrehistoricArchaeology and Human Peopling (Department of Anthro- pology and Ecology) of the University of Geneva with thefinancial support of the Swiss National Science Foundation.Dr. F. Cattin and Dr. B. Guénette-Beck were in charge of the scientific organization. More than 30 scientists fromBelgium, France, Germany, Italy and Switzerland attendedthe sessions with the seven key lectures dedicated todifferent aspects of actual research in the field of LIA.Over the last few years, several studies of archaeologicalartefacts using lead isotope analysis have shown a renewedinterest in this technique. The workshop aimed to bringtogether experienced senior researchers and young scien-tists active in the field to promote contacts and discussions.The idea was to address research questions on four general points:1. Analytical considerations: possibilities, advantages andshortcomings of various methods like TIMS, ICP-MSand LA-ICP-MSSince the first application of Pb isotopic data inarchaeology, its acquisition has relied on different analyticalmethods. From this concern, it is legitimate to ask if onelead isotope analysis is equivalent to another lead isotopeanalysis. First of all, thermal ionisation mass spectrometry(TIMS) was the only method used in Pb isotope measure-ment until the introduction of high precision multi-collector inductively coupled plasma mass spectrometer, as detailedin the LIA historical perspective of Stos-Gale and Gale. Themore recent development of mass spectrometry with laser ablation reduced the sample size and therefore widenednew perspectives of applications, with the opportunity toinvestigate small or precious artefacts and micro-scalesampling in a heterogeneous matrix. The methodological paper of Villa discusses the protocols of all thesetechniques, with a focus on the one processed at theLaboratory of Isotope Geology at the University of Berne(Switzerland). What comes out of this contribution is that accuracy should concentrate our full attention whenacquiring new data and that precision, whatever high or not, may allow distinction between what needs to bedifferentiated regarding specific archaeological questions.
F. Cattin (
M. BesseDépartement d
anthropologie et d
écologie,Université de Genève,12 rue Gustave-Revilliod,1211 Geneva, Switzerlande-mail: mail@florencecattin.comM. Bessee-mail: marie.besse@unige.chB. Guénette-Beck
V. SerneelsDepartment of Geosciences, University of Fribourg,Chemin du Musée 6,1700 Fribourg, SwitzerlandB. Guénette-Becke-mail: barbara.guenette-beck@unifr.chV. Serneelse-mail: vincent.serneels@unifr.chF. CattinDépartement d
anthropologie, Université de Montrèal,C. P. 6128, succursale Centre-Ville,Montrèal, QC H3C 3J7, CanadaArchaeol Anthropol Sci (2009) 1:137
148DOI 10.1007/s12520-009-0013-4
2. LIA in regard with the materials studied, namely what are the specificities of applying LIA to metals such aslead/silver, copper and iron, to natural ores as well as tometallurgy-related traces of Pb in sediments?From the beginning, the determination of the provenanceof metal artefacts, based on comparison between metallic products and natural ores, has been one of the mainquestions addressed by LIA and a major expectancy fromarchaeologists. The technique was first applied to lead andsilver ores and metals and then to copper and only veryrecently to iron. Despite significant success, it became clear that several pitfalls do exist and that LIA interpretationmust be made carefully with a good background for themineral resources, the history of their exploitation and thetechnology involved.Regarding the chaîne opératoire of silver, Guénette-Beck et al. highlights the problem of re-melted silver inthe case of coin minting. Actually, the control of the silver content in coins requires its purification by cupellation,leading to lead contamination. Lead artefact studies basedon lead isotope analysis have also a specificity in theinterpretation of the data. As described in Bode et al.,when the mixing of two sources of lead is ascertained bya mixing line in binary diagrams, the mixture ratio can becalculated.Within the chaîne opératoire of copper, the lead isotopecomposition may be a concern in the case of alloying.Actually, the signature would no longer reflect that of copper, but an intermediate solution of lead issued from thecopper and the admixed lead. It is generally considered that lead in tin to produce bronze does not significantly affect the lead signature of the copper.Moving on to the analytical methods, as described byDegryse et al., LIA of iron artefacts requires a huge amount of sample material (up to several milligrams). This is far more than for lead, silver and copper sampling, with theexception of native copper, for which lead content isgenerally inferior to 1 ppm. The complementary use of Sr isotopes by Degryse et al., for which TIMS measurementsare more precise than Pb isotopes, is a very interesting wayto narrow down the possible sources. In the future, thisapproach that holds simultaneously elements coming fromvarious elements might be pursued, extended to otheisotope systems and applied to different metals. At the sametime, the influence of the process on these other elementsdeserves to be understood.3. LIA with regard to archaeology, to what kind of archaeological questions can LIA offer new elementsfor our understanding of the past? How can geo-scientists aid in solving archaeological problems andwhat are the expectations of the archaeologists in thisrespect?Archaeology seeks to understand human populations of the past. Nowadays, there is a panel of related disciplinesthat can be applied to resolve archaeological problems. At  present, the use of LIA remains most often restricted tospecific fields in the framework of research programs. It has been fieldwork, however, that has been the most productivein terms of archaeological finds and publications. Despitethis, we note a scarcity of site monographs that include leadisotope analysis as part of the interpretation of metallicdata. Perhaps the lack of knowledge or understandingregarding the potential of the method and the lack of  publications in general archaeological journals are to betaken into account. In our opinion, lead isotope analysisshould not be restricted to academic research or specifictopics as ingots or coins. Indeed, the interpretation of collected data can provide fieldwork archaeology withvaluable information. As shown by Cattin et al., thismethod improves understanding of a settlement and itscultural background within the final Neolithic of westernSwitzerland. Guénette-Beck et al. relate the exploitationhistory of Ag/Pb ore bodies for the production of silver objects in the metallogenic region of the Valais region,Switzerland, from the Late Iron Age to the Late MediaevalPeriod. Degryse et al. contribute new elements related toiron trade routes in Sagalassos (Turkey) from the earlyRoman period to the early Byzantine period. Bode et al.question the motives of the conquest of Germania by theRoman Empire. They seek to demonstrate Roman-relatedlead mining east of the Rhine river and then to quantify itseconomic importance.4. Methods of establishing databases and their practicaluseThe paper of Stos-Gale and Gale discusses the databasesin LIA. The long developments on methodology andhistory of data acquisition that it contains highlight theheterogeneity of the data within only the Oxford laboratory.In that sense, the wish to merge into a unique database allavailable Pb isotope data for ores and artefacts
and relatedinformation on the analytical process, the precision andaccuracy, the site coordinates, the geology of the ore body,the mining evidences, the artefacts period of usage, etc.
cannot be accomplished without a time-consuming, difficult and multidisciplinary approach. Nevertheless, to give a basis for future research in LIA, a non-exhaustive collectionof published papers with lead isotope data for ores andartefacts is presented in the
. It remains animportant concern to make the huge amount of existingdata available for all.Even if this special issue presents only selected LIAapproaches, this volume, through the diversity of the papers, already shows a heterogeneous panel in theacquisition and the interpretation of the Pb isotope data.
138 Archaeol Anthropol Sci (2009) 1:137
From these approaches, we conclude that a lead isotopeanalysis cannot be separated from those technical parameters,since they aimed at answering specific questions with the best appropriate tools for it. In the future, hopefully, the develop-ment of analytical methods will help improve protocolstowards a less and less destructive Pb isotope acquisition.Simultaneously, analysts, archaeologists and archaeometristsshould keep working together on new and complementaryways of research in the quest for material provenances.As a final remark, we would like to thank the Swiss National Science Foundation for their financial supporregarding the organisation of the workshop and for the twodoctoral grants that made our research possible.
This appendix presents a non-exhaustive collection of  published papers with lead isotope data for Cu, Pb/Agand Fe ores, as much as copper, silver, lead and ironartefacts. The scope region is Europe and the Mediterra-nean World. It has been constructed based on Guénette-Beck (2005) and Cattin (2008) and significantly increased by M. Bode
s, P. Degryse
s, N. Gale
s and S. Stos
suggestions.Amov B (1999) Lead isotope data for ore deposits fromBulgaria and the possibility for their use in archaeometry.Berlin Beitr Archäom 16:5
19Arias D, Corretgé LG, Suárez O, Villa L, Cuesta A,Gallastegui G (1996) Lead and sulphur isotope composi-tions of the Ibias gold vein system (NW Spain): geneticimplications. Econ Geol 91:1292-1297Arribas A, Tosdal RM (1994) Isotopic composition of Pb in ore deposits of the Betic Cordillera, Spain: origin andrelationship to other European deposits. Econ Geol89:1074
1093Artioli G, Baumgarten B, Marelli M, Giussani B,Recchia S, Nimis P, Giunti I, Angelini I, Omenetto P(2008) Chemical and isotopic tracers in alpine copper deposits: geochemical links between mines and metal. GeoAlp 5:139
148Attanasio D, Bultrini G, Ingo M (2001) The possibilityof provenancing a series of bronze punic coins found at Tharros (western Sardinia) using the literature lead isotopedatabase. Archaeometry 43(4):529
547Baker J, Stos S, Waight T (2006) Lead isotope analysisof archaeological metals by multiple-collector inductivelycoupled plasma mass spectrometry. Archaeometry 48(1):45
56Balassone G, Boni M, Di Maio G, Villa IM (2009)Characterisation of metallic artefacts from the Iron Ageculture in Campania (Italy): a multi-analytical study. PeriodMineral 78(I):45
63Barnes IL, Shields WR, Murphy TJ, Brill RH (1974)Isotopic analysis of Laurion lead ores. Archaeol Chem138:1
10Baron S, Carigna J, Laurent S, Ploquin A (2006)Medieval lead making on Mont-Lozère Massif (Cévennes,France): tracing ore sources using Pb isotopes. ApplGeochem 21:241
252Baudo F, Mozzocchin GA, Cairns W (2007) A pilgrim
sampulla from San Giacomo in Paludo (Venice): provenancehypothesis through lead isotope ratio analysis. J CulHeritage 8:284
288Beer-Tobey L, Gale NH, Kim H, Stos-Gale ZA (1998)Lead isotope analyses of four late archaic silver ingots fromthe Selinus hoard. In: Oddy A, Cowell M (eds) Metallurgyin Numismatics 4. Royal Numismatic Society, SpecialPublication 30. London, pp 385
393Begemann F, Hauptmann A, Palmieri A, Schmitt-Strecker S (2002) Chemical composition and lead isotopyof metal objects from the
tomb and other relatedfinds at Arslantepe, Eastern Anatolia. Paorient 28(2):43
69Begemann F, Schmitt-Strecker S (1994) Das Blei vonSchiff und Ladung: Seine Isotopie und mögliche Herkunft.In: Hellenkemper-Salies G (ed) Das Wrack. Der antikeSchiffsfund von Mahdia, Cologne, pp 1073
1076Begemann F, Schmitt-Strecker S, Pernicka E, LoSchiavo F (2001) Chemical composition and lead isotopyof copper and bronze from nuragic Sardinia. Eur J Archaeol4:43
85Begemann F, Schmitt-Strecker S (2008) Bleiisotopie unddie Provenienz von Metallen. In: Yalçin Ü (ed) AnatolianMetal IV, Der Anschnitt, Beih 21, Deutsches Bergbau-Museum Bochum, Bochum, pp 125
134Bendall Ch (2003) The application of trace element andisotopic analyses to the study of Celtic gold coins and their metal sources. Dissertation, Universität Frankfurt Bendall C, Wigg-Wolf D, Lahaye Y, Von Kaenel H-M,Brey GP (2009) Detecting changes of Celtic gold sourcesthrough the application of trace element and Pb isotopelaser ablation analysis of Celtic gold coins. Archaeometry51:598
625Bielicki KH, Tischendorf G (1990) Lead isotope andPb
Pb model age determinations of ores from centralEurope and their metallogenetic interpretation. ContribMineral Petrol 106:440
461Bode M (2008) Archäometallurgische Untersuchungenzur Blei-/Silbergewinnung im Germanien der frühen Römi-schen Kaiserzeit. Dissertation, University of Münster (URN: urn:nbn:de:hbz:6-22579580819. URL:http://nbn-resolving.de/urn:nbn:de:hbz:6-22579580819)Boni M, Di Maio G, Frei R, Villa IM (2000) Leadisotopic evidence for a mixed provenance for Roman water  pipes from Pompeii. Archaeometry 42:201
Archaeol Anthropol Sci (2009) 1:137
148 139

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