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Sending Laurion Back to the Future: Bronze Age Silver and the Source of Confusion

Jonathan R. Wood, Yi-Ting Hsu and Carol Bell

Cite this as: Wood J. R., Hsu, Y-T and Bell, C. 2021 Sending Laurion Back to the Future: Bronze Age Silver and the Source of Confusion, Internet Archaeology 56.


Figure 20: Stag Rhyton (SG388) in the National Museum of Athens (NMA388). Photo Zde (CC-BY-SA-3.0)
Silver stag rhyton (SG388) from Mycenae in the National Museum of Athens (NMA388). Photo by Zde (CC-BY-SA-3.0)

Silver-bearing lead ores at Laurion in Attica were considered to have been first exploited with the introduction of coinage sometime around the birth of Classical Greece. However, in the late 20th century this chronology was radically revised earlier, to the Bronze Age, largely supported by lead isotope analyses (LIA). Here, we acknowledge that lead and silver metallurgy emerged from the earliest times but we propose that any correlation between these metals in the archaeological record is not a consequence of a geological association between lead and silver in ores such as galena until the middle of the first millennium BCE. We suggest that ancient metallurgists recognised that silver minerals (such as horn silver) dispersed in host rocks could be concentrated in molten lead and that LIA signatures of Bronze Age silver artefacts reflect the use of exogenous lead to extract silver, perhaps applying processes similar to those used to acquire silver in Bronze Age Siphnos. We further propose that lead from Laurion used for silver extraction resulted in the inadvertent transfer of its LIA signature (probably aided by roving silver prospectors) to silver objects and metallurgical debris recovered around the Aegean. New compositional analyses for the Mycenaean shaft-grave silver (c. 1600 BCE) support these conclusions. We believe that reverting to the mid-first millennium BCE for the first exploitation of silver from argentiferous lead ores is consistent with the absence of archaeological evidence for centralised control over Laurion until the Archaic period, the paucity of lead slag associated with silver-processing debris at Bronze Age sites, the scarcity of silver artefacts recovered in post-shaft grave contexts at Mycenae and throughout the Early Iron Age Aegean, the few Attic silver coins with LIA signatures consistent with Laurion until after 500 BCE and a single unambiguous mention of silver in the Linear B texts.

Corresponding author: Jonathan R. WoodORCID logo
Institute of Archaeology, UCL

Yi-Ting Hsu
Department of Archaeology, University of Cambridge

Carol Bell
Institute of Archaeology, UCL

Full text

Figure 1 : Schematic of the cupellation process. Argentiferous lead, derived from either smelting argentiferous lead ores (such as cerussite or galena), or by smelting an argentiferous ore (such as jarosite) with exogenous lead, is oxidised under a stream of air at a temperature of about 1000°C. The molten litharge can be absorbed (possibly by bone ash), along with any other metal impurities which oxidise (e.g. copper), leaving the silver and any inert impurities (such as gold) as a separate phase (adapted from Moureau and Thomas 2016 )

Figure 2 : Visual representation of Meyers' model ( 2003 , 271-88) for the exploitation of silver. Note the late application of galena as a silver source in Anatolia and Iran/Afghanistan

Figure 3: Map of the Cycladic islands and other sites mentioned in the text

Figure 4 : LIA plot of Laurion ores (OXALID 2020), Wappenmünzen coins (c. 545-510 BCE) and Athenian owls (5th-4th centuries BCE) (Gale et al. 1980 , table 6). The Athenian coins are consistent with Laurion ores. Six of the Wappenmünzen coins are not consistent with the Laurion ore field. Apart from two of the Wappenmünzen coins (including one that appears to be consistent with the Laurion ore LIA field), the others have Au/Ag x100 levels greater than 0.1 (see Table 5; Gale et al. 1980 , table 10), suggesting that the majority of the Wappenmünzen silver coins were not made from silver that derived from argentiferous lead ores

Figure 5: Native silver dispersed in a host rock. The surface has been coarsely polished to make the silver visible

Figure 6 : Simplified phase diagram of lead-silver system. 1. Liquid + solid Pb and 2. Solid + Pb eutectic. Melting point of lead (point A: 327.5°C); melting point of silver (point C: 962°C). The dashed line B-G corresponds to the eutectic composition of 2.5wt%Ag. The solubility of silver in lead is so small that it cannot be drawn on this diagram (i.e. 0.099wt%Ag). The process of heating argentiferous lead containing a very small quantity of silver and cooling to get pure lead and liquid richer in silver is now known as Pattinson's process. This process can be understood by following the phase diagram of the Ag-Pb system. The argentiferous lead is melted and heated to a temperature above the melting point of pure lead. Point a'' represents this system on the diagram. As the system cools slowly and the temperature of the melt decreases along a''-a', the solid lead starts separating at a'. As the system further cools, more and more lead separates and the liquid in equilibrium with the solid lead gets richer in silver. The lead that separates can be continuously removed by ladles. When the temperature of the liquid reaches a on the line DBE (the eutectic temperature), solid lead is in equilibrium with the liquid having the composition B. The liquid is cooled further when it solidifies to give a mixture of lead and silver having the eutectic composition of 2.5 wt% (25000ppm) of silver. This solid mixture of lead and silver can then undergo cupellation to recover the silver. Adapted from Karakaya and Thompson ( 1987)

Figure 7 : (left) Bronze Age slag from Ayios Sostis, Siphnos. (right) Typical large tapping slag from 4th-century BCE lead-smelting furnace installations at Pountazeza, Panormus and Laurion. (adapted from Gale and Stos-Gale 1981a, pl. 40)

Figure 8 : LIA plot of Bronze Age lead objects (OXALID 2020) from Crete, islands in the Cyclades (Amorgos, Antiparos, Despotiko, Kea, Makronisos, Naxos, Syros, Melos, Paros, Thera), the Dodecanese (Rhodes) and the Saronic Gulf (Dokos) and the Greek mainland (Argolid, Messenia, Thebes, Thessaly, Attica, Boeotia) delineated by chronology. The objects fall into two main groups that are consistent with the Laurion and Siphnian ore LIA fields identified by Gale and Stos-Gale ( 1981a ). The lead boat models recovered on Naxos lie within the Siphnian ore LIA field. Some objects from the LBA have higher 207Pb/206Pb values which are not shown due to scale

Figure 9 : LIA mirror plot of silver objects (OXALID 2020) found on the Greek mainland (Laconia, Messenia and the Argolid, in the Peloponnese, and Perati near Laurion) and Crete and other Greek islands (Amorgos and Syros in the Cyclades, Kos in the Dodecanese and Euboea). Note that three silver objects consistent with the Siphnian ore field are from the Early Bronze Age, which could suggest that the silver was extracted using Siphnian lead. Although the silver may have derived from Siphnos, it could have come from silver-bearing ores elsewhere - possibly from the islands on which the objects were recovered, i.e. Amorgos and Syros. Note the spread in the LIA values of silver, which could suggest mixed isotopic signatures, i.e. lead from one source, silver from another

Figure 10 : Histogram of the silver content (ppm) in 267 Bronze Age lead artefacts recovered around the Aegean (data from OXALID 2020). For example, about 70 lead objects have concentrations of silver between 423 and 507ppm in the lead. The distribution shows no evidence of bimodality, which would suggest a remarkably efficient separation process if lead (ores or metal) was being selected for either lead or silver objects on the basis of its silver content. Alternatively, it may suggest that lead ores with higher levels of silver had yet to be discovered and/or exploited

Figure 11 : LIA mirror plots for lead and litharge on Kea and Crete. (left mirror plots) Lead objects and litharge found on Kea are presented with Laurion and Siphnian ores. Lead objects found on Kea are consistent with Laurion and Siphnos. Litharge recovered on Kea appears to be consistent with Laurion. A group of litharge and lead samples may be present at 207Pb/206Pb ≈ 0.833. This could indicate a further source in addition to Siphnos and Laurion signatures, or possibly mixed lead from Laurion and Siphnian sources. (right mirror plots) Litharge and lead objects recovered on Crete are consistent with both Siphnian and Laurion ores. Some lead objects fall between these two ore fields which could suggest mixed LIA signatures, i.e. lead from both sources was mixed together. Alternatively, it could suggest that lead derived from another source, e.g. lead from one of the islands, such as Crete. Data from OXALID ( 2020)

Figure 12: Map of Attica showing Laurion and sites mentioned in the text

Figure 13 : LIA plot for Bronze Age silver analysed by Pernicka et al. ( 1983 ) alongside Laurion ores (OXALID 2020). Ten samples are from the shaft graves at Mycenae. The three outlined yellow points show the Bronze Age silver samples identified by Pernicka as having LIA signatures consistent with Laurion but inconsistent compositional analyses. Beside each of the points are their respective Au/Ag ×100 values

Figure 14: Scanning electron micrographs (SEM) of Mycenaean shaft-grave silver: SG520a (left) and SG520b (right)

Figure 15 : Scanning electron micrographs (SEM) of Mycenaean shaft-grave silver: SG865a (left) and SG865b (right). Note that SG865b is heavily corroded

Figure 16 : Scanning electron micrographs (SEM) of Mycenaean shaft-grave silver: SG479-1 (left) and SG479-2 (right). Note that SG479-1 is heavily corroded

Figure 17 : LIA mirror plots of Mycenaean silver objects presented alongside Laurion ores and silver objects plotted in Figure 9 (see Table 9, Table 11 and Table 12; OXALID 2020). At least two of the Mycenaean objects (SG388 and SG880) are clearly not consistent with Laurion. Data from OXALID (2020), Stos-Gale and MacDonald ( 1991 ) and Stos-Gale ( 2014 )

Figure 18 : Pb crustal ages (Ma) determined from the two-stage evolution model for the 30 Mycenaean shaft-grave silver samples, using LIA values from Stos-Gale and MacDonald ( 1991 ) and Stos-Gale ( 2014 ), and parameters from Desaulty et al. ( 2011 ). The samples are delineated by find location (i.e. Grave Circles A and B, and unknown). Different colours denote the individual shaft graves (see Tables 11 and 12). There is no obvious pattern between the crustal ages and the find locations. As expected from the LIA plots in Figure 17, two samples (SG388 and SG880) have much higher crustal ages than the majority of the Mycenaean silver

Figure 19 : Frequency histogram of the Pb crustal age (Ma) for ores from Laurion, as calculated from the lead isotopes from the Greek ores database (OXALID 2020) using the two-stage evolution model with parameters from Desaulty et al. ( 2011 ). The range of calculated Pb crustal ages for Athenian coins from the Asyut hoard (Gale et al. 1980 ) is also presented and shows that these coins are commensurate with silver mined from Laurion

Figure 20 : Stag Rhyton (SG388) in the National Museum of Athens (NMA388). Potentially of Anatolian origin as it has no Aegean parallels, with possible comparisons from 3rd millennium contexts, mainly in Anatolia, e.g. Kultepe rhyta (Özgüç and Özgüç 1953); Alaca Höyük bronze and silver stags (Arik 1937 ). For this reason, its presence at Mycenae has often been interpreted as an heirloom (Davis 1977). Photo Zde (CC-BY-SA-3.0)

Figure 21 : Plot of Au/Ag x100 against Pb crustal age (Ma) for Mycenaean silver. The ranges of crustal age and their maximum Au/Ag x100 levels are plotted for Laurion ores (Au/Ag x100 = 0.1286) and for Athenian coins (Au/Ag x100 = 0.3438). The three labelled samples (SG66b, SG520b and 3109) are the only pieces with Au/Ag x100 levels below 0.1

Figure 22 : Plot of Pb/Ag ×100 against Pb crustal age (Ma) for Mycenaean silver (Tables 11 and 12). Most samples fall within the crustal ages of Laurion ores (shaded box), which would suggest that Laurion lead was used to extract silver. There are possibly two groups (higher and lower levels of lead in these samples - see Figure 23). The lower lead levels (Pb/Ag ×100 <0.3) could suggest that they had not been cupellated, i.e. silver for these objects came from large silver minerals such as large crystals. These samples also have lower levels of bismuth. The crustal ages of these low-lead samples would also suggest they were from Laurion and older sources

Figure 23 : Histogram of the Pb/Ag x100 in the Mycenaean silver measured in this study by EPMA (Table 11). The shaded areas highlight a possible distribution at low levels of lead, which might reflect the natural distribution of lead found in large silver minerals at Laurion and around the Aegean. Higher lead levels were potentially cupellated with exogenous lead, thereby obliterating the signature associated with this distribution

Table 1: Gale's analysis (Gale 1980 , 161-96; Stos-Gale and Gale 1982) of Buchholz ( 1972, 21-36; Buchholz and Karageorghis 1973, 282) and Branigan's (1974, 155-205) cataloguing of Bronze Age Aegean and Anatolian lead and silver objects. The possible correlation between lead and silver objects recovered in the archaeological record was used to support the exploitation of argentiferous lead ores

Table 2: X-ray fluorescence (XRF) analyses (in weight per cent) of ores from Ayios Sostis, Siphnos. (s= standard deviation; nd = not determined) (adapted from Gale et al. 1980 , table 2). The final column is misleading, as exemplified by sample TG43-20, i.e. lead cannot dissolve 8.3wt% of silver in the solid state (see Figure 6)

Table 3: Compositional data from neutron activation analysis (NAA) of Laurion ores (from Gale et al. 1980 ); s is the standard deviation. Values in italics are from Gale and Stos-Gale ( 1981a) - not all elements were measured (nm) for these data. We assume here that lead was approximately 86wt%Pb, in accordance with the concentrations found in pure galena ores

Table 4: Silver and gold content of ores from Ayios Sostis, Siphnos (after Muller and Gentner ( 1979 ) published in Gale et al. 1980 ). s is standard deviation. Note that the silver values are slightly different from those in Table 2 because the current table presents the mean values of duplicate runs (adapted from Tylecote 1987, table 3.9b)

Table 5: Au/Ag ×100 of Laurion and Siphnian ores and Athenian and Siphnian coins (for data sources see Table 3 and Table 4 and Figure 4). Values of the mean, standard deviation, median and ranges are shown. n denotes the number of samples measured. Athenian coins generally exhibit lower Au/Ag values than Siphnian coins, in agreement with the Au/Ag values of the ores from which they are considered to have derived. The Au/Ag ×100 of Wappenmünzen coins and the LIA values plotted in Figure 4 support that the silver was not from the galena ores of Laurion

Table 6: Early Bronze Age silver from Anatolia (adapted from Meyers 2003 ). Note that zinc is present in appreciable concentrations and levels of lead are generally in the tenths of per cent. The Au/Ag ratios for this EBA silver are generally much higher than those found in silver derived from galena, which has values of Au/Ag ×100 <0.1

Table 7: Mean and standard deviation of Au/Ag ×100 levels in litharge and lead recovered on Kea. Median values and ranges are also shown. Lead objects found at Perati on Attica and Bronze Age lead objects recovered from around the Aegean are also presented alongside Laurion ores. n denotes the number of samples. The Au/Ag levels in the Kea litharge suggest that another component was present which had higher levels of gold than that found in association with the silver in lead ores or lead objects. Data from OXALID 2020

Table 8: Lead and litharge found at a Bronze Age (Middle Helladic context) site in Thorikos, Acropolis 153cS. Analyses include one of four fragments of melted lead metal and one of the two pieces of litharge. LIA and NAA of Thorikos samples are from Gale et al. ( 1980 ), Gale and Stos-Gale ( 1981a) and OXALID (2020). Pb crustal ages in millions of years (Ma) were calculated from the lead isotope data using the two-stage evolution model with parameters from Desaulty et al. ( 2011 )

Table 9: Lead isotope and compositional values for Aegean silver artefacts from OXALID ( 2020) database delineated by find location, i.e. Greek islands, specifically the island of Crete and the Greek mainland (excluding Mycenae). All compositional data were measured using XRF. Au/Ag ×100 values in bold have been calculated from a detection limit of 0.1wt% Au

Table 10: Compositions of the silver reference materials in weight per cent and limits of detection on the EPMA. Values below these limits were classified as below the detection limit (bdl)

Table 11: Compositional data – EPMA results from the Mycenaean shaft-grave silver. Heavily corroded samples are shaded and have their totals in bold type. Asterisks denote samples with low totals because the EPMA field of view was higher than the sample width. Pernicka et al.'s ( 1983 ) NAA data are presented in blue with the compositional data being measured percentages which had been previously recalculated to yield 100% based on metals. The main metal in the yellow highlighted sample 3109 is not silver

Table 12: Lead isotope analyses from Stos-Gale and MacDonald ( 1991 ) and Stos-Gale ( 2014 ). Pb crustal age calculated from two-stage evolution model using parameters from Desaulty et al. ( 2011 ). Question mark denotes uncertainty with regard to which LIA values correspond to the compositional data. LIA values in blue are from Pernicka et al. ( 1983 ) which do not have 204Pb values (and therefore the Pb crustal age could not be calculated). The main metal in the yellow highlighted sample 3109 may not have been silver (see section 4.1).

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