Retracing Magna Graecia's Silver: Coupling Lead Isotopes with a Multi‐Standard Trace Element Procedure

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Archaeometry 62, 1 (2020) 81–108 doi: 10.1111/arcm.12499

RETRACING MAGNA GRAECIA’ S SILVER: COUPLING LEAD ISOTOPES WITH A MULTI-STANDARD TRACE ELEMENT PROCEDURE*

T. BIRCH†

Centre for Urban Network Evolutions (UrbNet), Aarhus University, Moesgård Allé 20, 4230 DK-8270 Højbjerg, Denmark

K. J. WESTNER

Institut für Archäologische Wissenschaften, Goethe-Universität Frankfurt, Abt. II. Norbert-Wollheim-Platz 1 D-60621 Frankfurt am Main, Germany

F. KEMMERS

Institut für Archäologische Wissenschaften, Goethe-Universität Frankfurt, Abt. II. Norbert-Wollheim-Platz 1 D-60621 Frankfurt am Main, Germany

S. KLEIN

Deutsches Bergbau-Museum, Archäometallurgie, Am Bergbaumuseum 31 D-44791 Bochum, Germany and Frankfurt Isotope and Element Research Center (FIERCE), Goethe-Universität Frankfurt, Frankfurt am Main, Germany

H. E. HÖFER

Institut für Geowissenschaften, Facheinheit Mineralogie, Goethe-Universität Frankfurt, Altenhöferallee 1 D-60438 Frankfurt am Main, Germany

and H.-M. SEITZ

Institut für Geowissenschaften, Facheinheit Mineralogie, Goethe-Universität Frankfurt, Altenhöferallee 1 D-60438 Frankfurt am Main, Germany and Frankfurt Isotope and Element Research Center (FIERCE), Goethe-Universität Frankfurt, Frankfurt am Main, Germany

This study presents the results of compositional and lead isotopic analysis of coinage issued by the Greek colonies of Syracuse, Metapontum, Taras and Thurium in the fifth to third centuries BCE. The data suggest that each colony in Magna Graecia, regardless of its motherland roots and despite ongoing conflicts between the cities, had access to the same silver, and that this supply was stable overall throughout their period of minting and issuing coinage. The paper retraces the silver sources of the colonies and points out a potential supply route for the metal. It includes a method development for a multi-standard quantification approach for laser ablation-inductively coupled-mass spectrometry (LA-ICP-MS) analysis of silver.

KEYWORDS: MAGNA GRAECIA, SILVER COINAGE, WESTERN MEDITERRANEAN, LEAD ISOTOPES, TRACE ELEMENTS, SOUTHERN ITALY, GREEK

*Received 3 December 2018; accepted 16 August 2019 †Corresponding author: email [email protected] © 2019 The Authors. Archaeometry published by John Wiley & Sons Ltd on behalf of University of Oxford This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modiﬁcations or adaptations are made. 82 T. Birch et al.

INTRODUCTION Literary sources and archaeological evidence confirm that Greek communities began to appear c.750–725 BCE on the coast of southern Italy and the island of Sicily, with the colloquial term Magna Graecia used to describe these colonies (Fischer-Hansen et al. 2004, 250–251). These Greek poleis minted their own coinage, initially in silver, starting from as early as the mid-sixth century BCE. By the end of the third century BCE, Rome had become an important and powerful enterprise that dominated the coinage of southern Italy, putting an end to Greek issues (Rutter 1997, 99–100). The Greek colonies could have tapped into several different silver sources. All silver derives initially from an ore body, which has to be considered as the first potential source. Silver could have been extracted directly from surficial oxidized ores, but most would have derived from the cupellation of argentiferous Pb from smelting of sulphide ores, typically comprising mainly Pb sulphide (galena) besides complex silver-rich phases, for example, fahlore. Once mined, this silver may have travelled in trade form. This movement of silver across the Mediterranean and within the Aegean is well attested by numerous regionally widely spread ingot finds. Four stamped silver ingots from Selinus (Sicily) show the circulation of silver provenanced to Aegean sources, including Laurion, as well as potentially a Spanish silver source (Arnold Biucci 1988; Beer-Tobey et al. 1998). Pb isotope studies of Archaic eastern Greek coinage reveal that silver was mainly derived from the districts of Laurion and Siphnos and a third source with intermediate Pb isotope signatures, hypothesized to be located in Macedonia or Lydia (Gale et al. 1980).

Figure 1 Locations of the four mints (cities) under investigation. [Colour ﬁgure can be viewed at wileyonlinelibrary. com]

Once in circulation, silver may also have been acquired through war booty, gifts and the recycling of existing objects, including the remelting of old or foreign coinage (Howgego 1995, 24). This plethora of metal sources, from mine to existing metals, is well documented in classical works such as those by Livy, Pliny the Elder and Strabo, to name a few (cf. Rowan 2013a). The aim of this paper is to go beyond the historical and archaeological accounts alone and re- trace empirically the metal sources being used to mint the silver coinages of Magna Graecia. We studied the mints of Taras, Metapontum, Thurium and Syracuse in southern Italy (Fig. 1), all with a large and continuous production of silver coinage from the ﬁfth to the third centuries BCE, and sampled coins spanning their complete chronology.

MATERIALS A total of 70 coins minted at Taras, Metapontum, Thurium and Syracuse (Table 1) was sampled and analysed. A previous paper (Birch et al. in press) has already presented 17 further coins that were issued by various mints in Magna Graecia (Metapontum, Syracuse, Taras, Caulonia, Himera, Selinus and Sybaris/Thurium) in the Archaic period. What is interesting about investigat- ing these four poleis is that despite being located in quite close vicinity to one another, and all being Greek colonies, they were divided by territorial tensions, changing strategic partnerships and enemies, and their differential ‘motherland’ roots (Achaean, Corinthian and Spartan). As such, this presents an opportunity to identify whether such political–historical differences between these Greek colonies are also reflected in their access to silver. Taras was founded by the Spartans in the late eighth century BCE, whilst Metapontum was founded by Greeks from Achaea (northern Peloponnese) in the mid- to late seventh century BCE (Fischer-Hansen et al. 2004, 251–252, 279). Thurium was the refoundation of the Achaean colony of Sybaris, a city that was destroyed or captured and refounded several times over in the sixth and fifth centuries BCE. Around 440 BCE, the city, by now dominated by settlers from the Peloponnese and Athens, renamed itself Thurium (Fischer-Hansen et al. 2004, 295–298, 304– 305). Between 280 and 272 BCE, all three cities came under the control of Rome (Rutter et al. 2001). Metapontum began minting coinage c.550 BCE, issuing silver staters based on the Achaean standard until c.280 BCE. Taras started its coin production c.510–500 BCE based on the nomos (comparable with Achaean staters), ending c.228 BCE. Thurium’s silver coinage, based on the Achaean weight standard as well, set off immediately after its foundation around the mid- fifth century BCE and continued until shortly after 280 BCE (Rutter et al. 2001). In antiquity, the Greek colony of Syracuse was the largest city on Sicily. It was founded in the second half of the eighth century BCE by colonists from Corinth. Syracuse began minting silver coins in the late sixth century BCE, based on the Attic standard, and continued to do so until its capture by Rome during the Second Punic War in 212 BCE (Fischer-Hansen et al. 2004, 225– 228; Fischer-Bossert 2012, 142–152).

ANALYTICAL PROTOCOL Each coin was sampled threefold via drilling. Chips from the upper ﬁrst millimetre were discarded and only fresh unadulterated metal was used for subsequent analysis. A part of the drillings from each coin was prepared as standard metallographic blocks (epoxy resin, ground and ﬂatly polished), which were analysed for bulk major and minor elemental composition with an

Sample Mint Denomination HN reference Date FB date Ag Cu Pb Total 53Cr 55Mn 59 Co 60Ni ID (years BCE) (years BCE)

GE033 Metapontum Stater HN 1484-1486 470–440 – 96.87 0.05 2.94 99.86 1.2 0.8 bdl 0.3 GE036 Metapontum Stater HN 1507 430–400 – 96.00 1.49 2.29 99.78 0.5 2.0 0.2 1.5 Archaeometry GE037 Metapontum Stater HN 1526 400–340 – 94.68 4.32 0.50 99.49 0.3 0.7 2.5 10.4 GE041 Metapontum Stater HN 1528 400–340 – 97.31 1.79 0.11 99.21 0.6 1.0 3.0 5.6 GE042 Metapontum Stater HN 1534 400–340 – 94.10 5.05 0.09 99.24 0.3 1.3 8.3 29 GE045 Metapontum Stater HN 1525 400–340 – 96.84 2.69 0.12 99.64 0.3 bdl 2.2 4.3

62 TB014 Metapontum Stater HN 1540 350–340 – 92.87 5.79 0.80 99.47 0.4 0.4 6.2 12 22)81 (2020) 1 , TB015 Metapontum Stater HN 1537 350–340 – 89.55 9.82 0.26 99.62 0.6 bdl 3.5 22 GE035 Metapontum Stater HN 1575 340–330 – 92.55 6.54 0.62 99.71 0.3 0.3 1.1 9.9 GE038 Metapontum Stater HN 1575 340–330 – 94.50 4.91 0.44 99.85 0.3 0.1 0.9 7.3 GE039 Metapontum Stater HN 1575 340–330 – 93.39 5.99 0.49 99.87 0.7 0.3 0.9 7.3 Birch T. – 108 GE044 Metapontum Stater HN 1575 340–330 – 92.95 6.23 0.66 99.84 0.4 0.6 1.8 13 TB016 Metapontum Stater HN 1575 340–330 – 93.06 6.15 0.62 99.83 0.5 1.0 1.7 17

TB017 Metapontum Stater HN 1575 340–330 – 93.31 6.09 0.48 99.88 bdl 0.2 1.8 10 al. et TB018 Metapontum Stater HN 1575 340–330 – 92.75 6.59 0.52 99.86 0.6 0.6 0.8 12 GE034 Metapontum Stater HN 1589 330–290 – 95.72 3.18 0.56 99.45 0.4 3.2 7.3 10.2 GE040 Metapontum Stater HN 1589 330–290 – 95.03 3.74 0.60 99.38 1.2 0.9 0.9 5.9 TB019 Metapontum Stater HN 1582 330–290 – 96.00 3.22 0.47 99.69 1.0 2.4 3.5 7.8 TB020 Metapontum Stater HN 1587 330–290 – 90.55 8.72 0.45 99.72 0.6 0.9 4.1 18 TB021 Metapontum Stater HN 1589 330–290 – 95.29 3.93 0.41 99.63 0.6 3.1 1.1 19 GE005 Syracuse Tetradrachm Boehringer series 14 466–405 – 97.99 1.16 0.71 99.86 0.5 19.0 0.2 1.0 HE003 Syracuse Tetradrachm Boehringer series 22, 440–430 – 98.59 0.43 0.8 99.81 0.4 0.5 0.1 0.4 684 TB034 Syracuse Tetradrachm Boehringer series 22/ 430–430 – 83.23 16.36 0.24 99.83 1.0 1.2 2.2 115 Cop 660–662 TB035 Syracuse Stater SNG Cop 711f 345–317 – 96.70 2.52 0.50 99.72 0.5 0.8 0.1 0.6 GE008 Syracuse Tetradrachm SNG ANS 672–677 313–304 – 96.11 2.53 1.36 100.00 0.5 bdl 0.2 1.7 TB036 Syracuse Tetradrachm SNG Cop 766 305–289 – 77.85 21.51 0.32 99.67 1.4 bdl 9.3 62 GE006 Syracuse Tetradrachm Caccamo Caltabiano 218–214 – 98.09 0.76 0.80 99.64 0.3 bdl 0.1 0.2 146–179

(Continues) Table 1 (Continued)

Sample ID 66Zn 75 As 77 Se 106 Pd 111 Cd 118 Sn 121 Sb 128 Te 130 Te 194 Pt 195 Pt 197 Au 208 Pb 209 Bi

GE033 2.5 2.3 bdl 6.8 4.2 0.1 0.3 bdl 0.4 0.3 0.2 174 29266 515 GE036 2.2 3.3 0.5 8.5 5.1 4.8 3.3 2.4 2.3 1.0 1.0 1023 21066 1020 GE037 2.5 59 1.3 6.9 3.9 417 7.8 2.4 2.5 1.3 1.3 1867 4429 2158 GE041 19 11 0.4 7.7 4.6 62 2.1 3.1 3.2 0.3 0.3 2707 1066 5444 GE042 8 169 1.4 8.9 5.3 5.0 14 2.3 2.3 0.5 0.6 5842 1070 3104 GE045 1.2 6.7 2.1 7.6 5.8 0.9 2.0 2.7 2.7 0.4 0.4 2683 1221 4067

TB014 2.1 43 3.7 4.2 3.1 95 7.7 2.4 2.3 4.3 4.5 2418 7794 4634 Graecia Magna Retracing TB015 1.1 54 4.7 4.9 2.4 162 10 2.6 2.4 6.6 6.4 3349 2526 1162 GE035 1.0 14 2.5 7.3 4.1 4.1 7.6 3.0 3.0 0.6 0.6 2630 6190 844 GE038 1.7 148 0.9 7.1 4.0 8.0 14 1.5 1.6 0.5 0.5 961 4238 663 GE039 1.3 42 1.8 6.8 3.8 7.5 7.2 2.1 2.2 0.7 0.7 1516 4730 728 GE044 1.7 25 2.2 7.4 5.2 19 9.8 2.7 2.7 1.0 0.9 2465 6421 955 TB016 1.8 23 6.4 4.4 3.1 23 11 1.5 1.9 2.7 2.4 1870 6186 866 TB017 1.6 49 5.3 4.1 2.9 7.5 5.0 2.3 2.3 1.8 1.9 1050 4816 706

09Uiest fOxford, of University 2019 © TB018 0.9 23 5.9 4.4 2.9 14 9.6 1.5 1.6 2.8 2.8 1216 5363 877 GE034 0.8 46 1.4 8.3 4.6 12 8.5 7.4 7.6 2.5 2.6 5105 5695 642 GE040 0.9 48 1.1 6.7 3.9 34 6.4 5.1 4.9 0.8 0.8 4308 6049 905 ’ TB019 1.6 24 2.6 4.4 2.7 22 6.5 2.4 2.0. 2.4 2.4 2522 4660 728 silver s TB020 1.0 43 6.1 3.9 2.4 29 12 4.2 4.0 2.7 2.9 2597 4386 754 TB021 1.2 116 2.1 4.4 2.6 10 9.9 3.3 3.3 2.9 2.8 3196 4033 413 GE005 2.1 12 0.5 8.1 6.7 31 5.7 0.7 0.6 1.6 1.6 1475 7032 1948 HE003 1.2 1.4 0.2 6.5 3.9 6.3 0.8 0.8 0.9 0.4 0.4 650 7528 2161 TB034 240 289 12 3.7 2.1 537 210 3.1 3.7 3.4 3.2 470 2391 223 Archaeometry TB035 0.9 0.6 1.2 5.8 2.3 14 0.9 1.0 0.9 4.8 4.9 2730 5032 900 GE008 2.5 4.4 0.9 6.8 5.9 14 4.2 0.5 0.5 1.1 1.1 791 12547 523 TB036 5.2 162 11 3.6 1.5 112 111 4.5 4.6 4.0 4.0 3266 2979 568 GE006 1.8 2.9 0.5 7.7 6.6 30 1.0 2.2 2.1 3.0. 3.0 4267 7516 431 62 GE013 4.7 281 4.6 6.4 5.4 312 39 6.5 6.6 1.5 1.5 3552 5939 640 22)81 (2020) 1 , GE020 0.6 3.4 1.1 11 7.0 0.2 0.1 3.5 3.7 3.7 3.6 2942 2290 1790 GE029 3.3 26 1.4 6.5 4.2 42 10 3.1 3.0 1.6 1.6 2844 15607 2335 TB001 bdl bdl 0.3 3.5 2.8 0 0.1 0.9 1.2 1.9 1.9 2627 6136 2641 – 108 85 (Continues) 86 09Uiest fOxford, of University 2019 © Table 1 (Continued)

Sample Mint Denomination HN reference Date FB date Ag Cu Pb Total 53Cr 55Mn 59 Co 60Ni ID (years BCE) (years BCE)

GE013 Taras Didrachm HN 844 470–425 430–425 86.82 12.28 0.60 99.7 0.5 2.8 38 53 GE020 Taras Didrachm HN 844 470–425 430–425 97.93 1.65 0.23 99.8 0.5 0.5 bdl bdl Archaeometry GE029 Taras Didrachm HN 871 380–340 340–335 93.57 4.51 1.56 99.64 0.8 bdl 0.2 7.2 TB001 Taras Didrachm HN 876 380–340 380–370 98.36 0.46 0.59 99.4 bdl bdl bdl 0.1 TB002 Taras Didrachm HN 876 380–340 344–340 96.91 2.37 0.46 99.74 0.4 1.3 0.1 0.9 GE024 Taras Didrachm HN 889 340–332 344–340 93.87 4.54 1.50 99.91 0.7 bdl 3.8 8.8

62 GE025 Taras Didrachm HN 887 340–332 344–340 95.46 3.51 0.70 99.67 0.7 bdl bdl 3.6 22)81 (2020) 1 , GE027 Taras Didrachm HN 888 340–332 340–335 93.71 4.41 1.32 99.44 0.5 0.1 1.5 76 GE015 Taras Didrachm HN 935 332–302 302–290 94.89 4.26 0.63 99.78 2.2 2.3 10.1 46 GE016 Taras Didrachm HN 935 332–302 302–290 93.57 5.44 0.73 99.75 0.8 0.6 2.2 13 GE022 Taras Didrachm HN 934 var 2 332–302 290–281 93.16 6.07 0.59 99.81 1.4 0.9 6.5 34 Birch T. – 108 GE023 Taras Didrachm HN 934 332–302 290–281 93.37 5.64 0.72 99.73 0.4 0.8 3.3 17 GE030 Taras Didrachm HN 933 332–302 290–281 92.18 6.99 0.58 99.74 0.4 2.0 5.8 17

GE031 Taras Didrachm HN 961 302–280 281–276 95.31 3.55 0.68 99.54 0.4 3.1 1.1 5.6 al. et HE006 Taras Didrachm HN 968 302–280 281–276 94.98 4.04 0.66 99.68 0.7 4.9 2.1 6.2 GE011 Taras Didrachm HN 1006 280–272 276–272 94.25 4.90 0.58 99.73 0.4 2.1 2.4 9.0 GE019 Taras Didrachm HN 1006 280–272 276–272 94.20 4.55 1.04 99.79 0.8 0.7 1.4 7.5 GE028 Taras Didrachm HN 1001 280–272 276–272 91.47 7.39 0.82 99.67 0.9 2.6 4.8 21 TB004 Taras Didrachm HN 1003 280–272 276–272 92.07 7.18 0.47 99.71 0.5 3.2 29 21 TB005 Taras Didrachm HN 1001 280–272 276–272 92.54 6.61 0.58 99.73 0.5 2.7 12 22 TB006 Taras Didrachm HN 1006 280–272 276–272 93.28 5.83 0.59 99.69 0.9 1.6 3.3 12 TB007 Taras Didrachm HN 1011 280–272 276–272 94.21 4.96 0.50 99.67 0.3 0.5 1.2 3.6 GE009 Taras Didrachm HN 1025 272–240 272–240 84.36 13.56 0.38 98.30 1.5 bdl 16 24 GE014 Taras Didrachm HN 1041 272–240 272–240 95.39 4.09 0.29 99.76 0.7 0.3 5.2 20 GE021 Taras Didrachm HN 1043 272–240 272–240 91.36 7.82 0.61 99.79 0.5 1.7 5.8 26 TB008 Taras Didrachm HN 1025 272–240 272–240 89.03 10.12 0.51 99.66 0.6 0.4 7.6 30 TB009 Taras Didrachm HN 1040 272–240 272–240 86.59 12.54 0.60 99.72 0.9 4.7 26 46 TB010 Taras Didrachm HN 1041 272–240 272–240 86.68 12.37 0.53 99.57 0.5 0.7 19 32 TB011 Taras Didrachm HN 1043 272–240 272–240 89.36 9.79 0.54 99.69 2.7 0.6 14 34 GE017 Taras Didrachm HN 1055 240–228 240–228 89.26 9.78 0.51 99.54 0.6 bdl 2.6 26

(Continues) Table 1 (Continued)

Sample ID 66Zn 75As 77 Se 106 Pd 111 Cd 118 Sn 121 Sb 128 Te 130 Te 194 Pt 195 Pt 197 Au 208 Pb 209 Bi

TB002 0.6 2.2 1.2 5.0 3.0 22 1.3 1.2 0.9 3.8 3.8 2560 4671 1600 GE024 5.1 14 1.4 6.2 4.5 20 5.9 2.3 2.3 0.8 0.8 1139 14789 1204 GE025 1.5 4.2 2.3 6.6 4.6 4.8 1.6 1.4 1.4 1.3 1.3 3266 6721 2900 GE027 1.7 8.4 13 13 4.5 80 8.4 4.9 5.0 9.6 9.7 3394 12994 3188 GE015 14 62 6.2 31 25.5 64 25 6.2 6.0 3.9 4.0 5638 23502 3483 GE016 2.0 16 2.1 7.7 6.2 16 7.6 2.6 2.7 1.4 1.4 2679 7426 1274

GE022 6.6 55 6.7 19 14.1 49 22 6.7 7.1 3.7 3.8 6023 19323 3387 Graecia Magna Retracing GE023 2.2 34 2.1 6.7 4.7 29 11 2.9 3.0 1.2 1.2 2889 7110 1015 GE030 2.6 49 2.5 7.2 4.0 25 15 3.7 3.9 0.9 1.0 2553 5937 992 GE031 1.6 14 1.4 9.1 4.4 83 6.8 2.0 2.1 2.2 2.2 2722 7098 1773 HE006 1.7 40 1.0 6.7 3.9 98 6.6 4.5 4.4 1.0. 1.0 3597 6493 808 GE011 1.4 23 1.6 6.9 5.7 108 8.4 2.8 2.8 1.5 1.5 2912 5787 1218 GE019 1.5 18 1.7 7.5 5.3 97 6.5 2.7 2.8 1.8 1.8 3155 10407 1260 GE028 2.0. 66 2.2 6.5 4.2 160 16 5.2 5.1 1.7 1.7 3294 7988 968

09Uiest fOxford, of University 2019 © TB004 3.3 73 5.4 3.8 2.8 226 22 3.4 3.6 3.1 3.0 2566 4604 1490 TB005 2.6 56 4.7 4.4 3.0 170 13 4.1 4.3 4.0 3.8 3462 5769 849 TB006 2.3 22 3.4 4.2 2.8 54 8.8 2.3 2.2 2.3 2.3 2584 5828 876 ’ TB007 3.1 6.7 2.2 3.5 2.2 119 3.0 1.8 1.6 2.5 2.3 2532 4477 319 silver s GE009 4.7 124 5.0 7.2 5.2 13 384 104 4.3 4.2 2.4 2.4 5254 3758 833 GE014 2.5 121 1.7 11 7.9 297 11 2.8 2.8 3.6 3.6 2814 4027 1073 GE021 2.3 74 3.7 7.1 5.1 108 34 3.9 4.1 1.5 1.5 3346 5931 1299 TB008 1.2 108 6.0 4.3 2.6 200 28 4.5 4.1 3.7 3.6 3311 5079 656 TB009 2.7 167 7.0 4.5 2.6 284 31 5.5 5.1 4.0. 4.0 3331 5780 1391

Archaeometry TB010 2.8 125 9.2 3.8 2.7 225 25 4.3 3.9 3.7 3.8 2672 5138 821 TB011 2.1 112 9.5 4.1 2.9 152 22 4.6 4.3 4.0 4.0 2983 5384 660 GE017 1.5 65 4.8 7.6 6.0 58 28 6.8 6.7 2.1 2.1 4534 5654 622 HE004 7.6 2.4 bdl 6.3 3.9 1.4 0.3 0.1 0.2 0.2 0.2 116 24369 692

62 HE005 1.6 23 1.2 7.7 4.0 87 6.1 2.3 2.4 1.5 1.5 1432 10417 1194 22)81 (2020) 1 , TB023 2.2 32 1.4 4.1 2.7 1.8 5.4 2.1 2.1 0.7 0.7 1303 544 4878 TB024 1.2 1.3 1.6 7.9 4.1 19 7.2 1.4 1.3 2.8 2.8 1741 12352 3340 GE048 4.1 43 1.2 7.3 4.5 431 7.9 2.0 2.1 1.7 1.7 2601 6221 2094 – 108 87 (Continues) 88 09Uiest fOxford, of University 2019 ©

Table 1 (Continued) Archaeometry

Sample Mint Denomination HN reference Date FB date Ag Cu Pb Total 53Cr 55Mn 59 Co 60Ni ID (years BCE) (years BCE) 62 22)81 (2020) 1 , HE004 Thurium Stater HN 1760 443–400 – 97.45 0.08 2.36 99.89 0.9 bdl bdl 0.2 HE005 Thurium Stater HN 1772 443–400 – 95.52 3.31 1.05 99.88 0.7 4.5 0.5 4.8 TB023 Thurium Stater HN 1757–1769 440–430 – 96.89 2.55 bdl 99.44 0.8 bdl 2.6 7.0 – – Birch T. – TB024 Thurium Stater HN 1773 430 420 98.04 1.30 0.48 99.82 0.9 0.5 0.1 2.5 108 GE048 Thurium Stater HN 1791c 400–350 – 94.84 4.29 0.62 99.75 0.5 0.5 4.1 11 GE050 Thurium Stater HN 1790 400–350 – 96.72 2.48 0.65 99.85 0.3 2.0 bdl 1.9

GE054 Thurium Stater HN 1784 400–350 – 97.36 1.84 0.41 99.61 0.8 13 0.2 1.0. al. et TB025 Thurium Stater HN 1791c 400–350 – 95.64 3.42 0.75 99.81 0.4 0.7 6.5 6.7 GE046 Thurium Stater HN 1811 350–300 – 93.50 5.02 0.78 99.30 0.4 0.1 19.7 15 GE049 Thurium Stater HN 1818 350–300 – 94.75 3.85 0.84 99.43 0.7 bdl 2.4 3.5 GE051 Thurium Stater HN 1860 350–300 – 90.68 7.91 1.25 99.84 0.8 1.7 3.0 20 GE053 Thurium Stater HN 1820 350–300 – 93.80 4.93 1.10 99.83 0.3 0.2 2.6 12 GE047 Thurium Stater HN 1872 300–280 – 92.74 6.42 0.48 99.63 0.5 0.4 1.0. 11 Table 1 (Continued) ercn an Graecia Magna Retracing

Sample ID 66Zn 75As 77 Se 106 Pd 111 Cd 118 Sn 121 Sb 128 Te 130 Te 194 Pt 195 Pt 197 Au 208 Pb 209 Bi

GE050 0.9 3.8 0.9 8.1 4.7 58 3.5 1.3 1.4 2.4 2.3 2481 6420 1648 GE054 0.8 2.5 0.8 10 4.6 46 1.3 1.8 1.9 3.5 3.6 3717 4626 2606 TB025 2.2 18 2.9 5.6 2.4 39 4.7 1.7 1.9 4.3 4.3 2176 7349 1705 GE046 4.5 89 1.6 6.7 4.9 19 9.1 2.1 2.2 0.3 0.3 2258 7859 6754

09Uiest fOxford, of University 2019 © GE049 1.7 9.6 0.6 8.2 4.4 134 1.8 1.2 1.2 3.4 3.4 4407 8474 682 GE051 2.0 45 2.5 7.1 3.9 24 14 2.7 2.6 1.0 1.0 1965 12418 1015 GE053 2.7 21 1.8 7.2 4.0 23 5.7 1.6 1.6 1.0 0.9 1417 11058 1014 ’ GE047 1.4 13 2.1 7.1 4.6 127 5.3 2.6 2.7 1.3 1.4 2609 4914 1189 silver s

HN reference refers to the coin identification as per Rutter et al. (2001), the same work from which the dating also derives. FB date refers to the alternative chronology offered for Taras by Fischer- Bossert (2012); for the nomenclature for the other coins, see Boehringer (1993), Caccamo Caltabiano et al. (1997) and the Syllogue Nummorum Graecorum (Danish National Museum 1981; American Numismatic Society 1988). For major, minor and trace element composition of the coins, Ag, Pb and Cu contents (derived from EPMA, normalized, with new calculated total of the three main elements provided) are given in wt%; all other values (derived from LA-ICP-MS) are in ppm. For errors and full results, see additional supporting information S2. bdl, Below detection limits. Archaeometry 62 22)81 (2020) 1 , – 108 89 90 T. Birch et al. electron probe microanalyser (EPMA). The same blocks were analysed in order to quantify the trace elemental composition via laser ablation-inductively coupled-mass spectrometry (LA- ICP-MS) using Pb and Cu values as internal standards. Three new silver alloy reference materials (MBH Analytical) were specially commissioned by a consortium of institutions led by Goethe- Universität Frankfurt am Main (University of Leicester, University of Liverpool, Metropolitan Museum, University College London (UCL), UCL Qatar) for quantification purposes of LA- ICP-MS data and measuring instrument performance. They were also prepared as standard metallographic blocks. Using these reference materials, a multi-standard quantification procedure was developed for accurately determining the trace element composition of silver. The Pb isotopic signature was determined from digested drillings using a multi-collector-inductively coupled plasma-mass spectrometer (MC-ICP-MS). Samples were chromatographically separated according to procedures reported by Klein et al. (2009). The precision and accuracy of the measure- ments were continuously checked by repeatedly analysing the NIST SRM 981 standard. For a detailed description of the sampling protocol, analytical methods, and their accuracy and precision, see additional supporting information S1. Euclidean distances of the measured Pb isotope values were calculated to determine the nearest neighbours (of reference data points) to samples according to the following formula: sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 2 2 2 206Pb 206Pb 207Pb 207Pb 208Pb 208Pb d ¼ þ þ 204Pbr 204Pbm 204Pbr 204Pbm 204Pbr 204Pbm where r is the literature reference data; and m is the measured Pb isotope ratios. The method is similar to Stos-Gale’s TestEuclid method, but without normalizing to analytical measurement errors (cf. Stos-Gale and Gale 2009; Ling et al. 2014), and to calculations described by Delile et al. (2014). Pb isotope data are unconstrained and normally represented in the form of three isotope ratios normalized to either 204Pb or 206Pb, though 204Pb is more informative on ore genesis. The three-dimensionality of Pb isotope data is suited to the Euclidean space, where the distance between two points is measurable. The Pb isotope database compiled for this project was orientated to the reference data set from Blichert-Toft et al. (2016), using the same data for interpretation. Four coins were found to be ancient forgeries upon drilling with a Cu (-alloy) core and were excluded from the present results (DE001, DE002, GE026 and GE052), but for their silver sur- face composition, see additional supporting information S2.

RESULTS

Chemical composition The silver content of the coins ranged between 77.9 and 98.6 wt%, with Cu as the second major element (0.05–21.5 wt%). Between 0.1 and 2.9 wt% Pb were detected (median = 0.59 wt%; Table 1). The range of Cu and Pb abundances of the coins from the four different mints (Fig. 2) largely overlaps and is comparable with data from Burnett and Hook (1989). For Taras, Thurium and Metapontum, a general trend towards higher Cu contents for coins with a younger dating is discernible. The coins from Syracuse are marked by highly ﬂuctuating compositions. Coins from the same mint with an identical dating range typically have a rather homogeneous composition with a relative standard deviation (RSD, %) of silver abundances typically < 5%. Exceptions are coins from Syracuse (83.23 and 98.56 wt%) and Taras (86.82 and 97.93 wt%)

Figure 2 Cu and Pb contents of the investigated coins. Data from this study are shown as circles, literature values (Burnett and Hook 1989) as diamonds. The filling of the symbols corresponds to the dating of the coins: (a) Metapontum, (b) Taras, (c) Thurium and (d) Syracuse. [Colour figure can be viewed at wileyonlinelibrary.com] dating between 440 and 430 BCE and between 470 and 425 BCE, respectively. Overall, the fineness of single issues hence appears to be quite constant. The investigated coins contain variable amounts of minor and trace elements (Table 1). Sn, As, Ni, Sb, Cd, Te, Co, Se and Zn all show median abundances > 1 ppm. Positive correlations (r ≥ 0.70, checked also as log-transformed values) between Cu and Ni (r = 0.74) as well as of Cu with As (r = 0.73), Se (0.74) and Sb (0.75) can be observed. Cu and Sn are not correlated (r = 0.29). The Au contents of the coins range from 0.01 to 0.6 wt% (median = 0.27 wt%). Corresponding Au/Ag ratios scatter between 0.1 × 103 and 6.5 × 103, a typical range for common styles of silver mineralizations such as base metal veins and carbonate replacement deposits comprising accessory Au (Boyle 1968; Sillitoe and Hedenquist 2003), which occur in the broader Mediterra- nean area. Bi is the second most abundant minor element besides Au with contents between 0.02 and 0.70 wt% (median = 0.1 wt%).

Pb isotopes The individual mints show comparable Pb isotope patterns (Fig. 3 and Table 2). With the exception of two coins (TB034, 146 Ma; GE046, 118 Ma), the Pb isotope values represent a geological reservoir with a relatively homogeneous ore formation age corresponding to the Alpine period (i.

Figure 3 Pb isotope diagrams of the investigated coins in comparison with literature data of Archaic silver ingots from the Selinus hoard (Beer-Tobey et al. 1998), Archaic and Classical eastern Greek silver coinage (Gale et al. 1980; Hardwick et al. 1998; Stos-Gale and Gale 2009) and Archaic western Greek coinage (Gale et al. 1980; Birch et al. in press): (a) 207Pb/204Pb-206Pb/204Pb diagram; and (b) 208Pb/204Pb-206Pb/204Pb diagram.

e., ≤ 100 Ma). Differences in the three 204Pb-based isotope ratios reﬂect variations of the Th/U ratios of the raw material sources of the coins (cf. Albarède et al. 2012; Pernicka 2017). Variation of 238U/204Pb and 232Th/204Pb ratios (with 238U and 232Th being the parent isotopes of 206Pb and 208Pb while 204Pb is primordial) as markers of the crustal evolution was shown to extend over the typically well-deﬁned Pb model age provinces within Europe (Blichert-Toft et al. 2016) and hence establishes distinct isotopic characteristics within broadly geologically simultaneous ore- forming events. The coin data compare favourably with Pb isotope values of Archaic coins from the Greek mainland (Gale et al. 1980; Hardwick et al. 1998). This corresponds to an overlap with ores from Attica, Macedonia, the Cyclades, the Biga Peninsula in north-western Anatolia and the Rhodope Massif as well as with metal production residues from these districts (Stos-Gale and Gale 2009). Altogether, the Pb isotope signatures thus are highly suggestive of an overall Aegean provenance

Sample Model age 206 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ Broad Euclidean ID (Ma) 204 Pb 204 Pb 204 Pb 206 Pb 206 Pb neighbours

GE033* 27 18.838 0.014 15.689 0.010 38.860 0.029 0.83284 0.00015 2.06293 0.00040 Aegean Attica (Lavrion) GE036* 17 18.843 0.014 15.685 0.011 38.856 0.030 0.83243 0.00012 2.06215 0.00035 Aegean Attica (Lavrion) GE037 22 18.828 0.006 15.682 0.006 38.857 0.018 0.83298 0.00007 2.06389 0.00032 Aegean Attica (Lavrion) GE041 46 18.751 0.010 15.667 0.009 38.816 0.023 0.83553 0.00012 2.07003 0.00041 Aegean E. Rhodopes, Macedonia (Chalkidiki), W. Rhodopes

(Thasos), W. Anatolia Graecia Magna Retracing (Balikesir) GE042 17 18.815 0.007 15.676 0.006 38.819 0.017 0.83311 0.00011 2.06315 0.00035 Aegean Attica (Lavrion) GE045 16 18.750 0.019 15.652 0.014 38.737 0.039 0.8348 0.00019 2.06603 0.00042 Aegean E. Rhodopes, Macedonia (Chalkidiki), W. Rhodopes (Thasos), W. Anatolia (Canakkale) TB014* 54 18.756 0.010 15.672 0.008 38.816 0.022 0.83557 0.00011 2.06949 0.00038 Aegean E. Rhodopes, Macedonia

09Uiest fOxford, of University 2019 © (Chalkidiki), W. Rhodopes (Thasos), W. Anatolia (Balikesir) ’ TB015* 25 18.816 0.010 15.680 0.008 38.847 0.022 0.83335 0.00012 2.06455 0.00038 Aegean Attica (Lavrion) silver s GE035 30 18.801 0.022 15.677 0.015 38.834 0.040 0.83394 0.00019 2.06585 0.00049 Aegean Attica (Lavrion), W. Anatolia (Canakkale), E. Rhodopes, Macedonia (Chalkidiki) GE038 20 18.834 0.018 15.684 0.013 38.852 0.036 0.83272 0.00022 2.06284 0.00039 Aegean Attica (Lavrion) Archaeometry GE039 27 18.814 0.020 15.680 0.015 38.840 0.041 0.8334 0.00018 2.06441 0.00040 Aegean Attica (Lavrion) GE044 30 18.812 0.025 15.681 0.018 38.845 0.049 0.83349 0.00022 2.06465 0.00037 Aegean Attica (Lavrion) TB016* 26 18.820 0.010 15.682 0.009 38.848 0.026 0.83325 0.00014 2.06420 0.00052 Aegean Attica (Lavrion) TB017* 28 18.834 0.010 15.688 0.009 38.865 0.028 0.83298 0.00013 2.06357 0.00055 Aegean Attica (Lavrion) 62 TB018* 21 18.836 0.007 15.685 0.006 38.857 0.017 0.83271 0.00010 2.06299 0.00038 Aegean Attica (Lavrion) 22)81 (2020) 1 , GE034 43 18.766 0.025 15.671 0.019 38.830 0.048 0.83506 0.00021 2.06921 0.00038 Aegean E. Rhodopes, W. Rhodopes (Thasos), Macedonia (Chalkidiki) – 108 (Continues) 93 94 09Uiest fOxford, of University 2019 © Table 2 (Continued)

Sample Model age 206 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ Broad Euclidean ID (Ma) 204 Pb 204 Pb 204 Pb 206 Pb 206 Pb neighbours

GE040 34 18.772 0.022 15.668 0.016 38.834 0.044 0.83466 0.00018 2.06876 0.00041 Aegean W. Rhodopes (Thasos), Macedonia (Chalkidiki), E. Archaeometry Rhodopes TB019* 30 18.808 0.008 15.679 0.007 38.844 0.019 0.83369 0.00011 2.06536 0.00036 Aegean Attica (Lavrion), W. Anatolia (Canakkale) TB020* 34 18.802 0.008 15.679 0.007 38.844 0.020 0.83390 0.00009 2.06600 0.00037 Aegean Attica (Lavrion), W.

62 Anatolia (Canakkale) 22)81 (2020) 1 , TB021* 35 18.789 0.008 15.675 0.006 38.837 0.019 0.83427 0.00010 2.06702 0.00040 Aegean Macedonia (Chalkidiki), Attica (Lavrion), W. Anatolia (Canakkale), W. Rhodopes (Thasos) Birch T. – 108 GE005 28 18.804 0.007 15.677 0.007 38.850 0.018 0.83372 0.00011 2.06613 0.00037 Aegean Attica (Lavrion), W. Anatolia (Canakkale)

HE003 14 18.836 0.008 15.682 0.007 38.867 0.022 0.83257 0.00011 2.06342 0.00037 Aegean Attica (Lavrion) al. et TB034* 146 18.559 0.010 15.646 0.009 38.596 0.025 0.84304 0.00011 2.07960 0.00044 Unknown Cyclades (Siphnos), Massif Central, Cantabrian Mountains TB035* 17 18.838 0.008 15.684 0.007 38.851 0.019 0.83256 0.00010 2.06233 0.00036 Aegean Attica (Lavrion) GE008 91 18.734 0.007 15.682 0.006 38.881 0.017 0.83707 0.00009 2.07545 0.00040 Aegean E. Rhodopes, C Rhodopes TB036* 97 18.734 0.009 15.685 0.008 38.901 0.022 0.83727 0.00012 2.07650 0.00034 Aegean E. Rhodopes, W. Anatolia, Cyclades (Siphnos), C Rhodopes GE006 18 18.828 0.007 15.681 0.006 38.852 0.019 0.83285 0.00012 2.06355 0.00042 Aegean Attica (Lavrion) GE013 38 18.820 0.006 15.687 0.005 38.858 0.015 0.83352 0.00009 2.06474 0.00039 Aegean Attica (Lavrion) GE020 20 18.807 0.007 15.674 0.007 38.825 0.017 0.83345 0.00010 2.06450 0.00036 Aegean Attica (Lavrion) GE029 10 18.830 0.009 15.677 0.007 38.847 0.021 0.83260 0.00011 2.06311 0.00040 Aegean Attica (Lavrion) TB001* 18 18.832 0.012 15.682 0.010 38.835 0.029 0.83272 0.00012 2.06215 0.00055 Aegean Attica (Lavrion) TB002* 20 18.832 0.014 15.683 0.011 38.849 0.031 0.83279 0.00013 2.06298 0.00034 Aegean Attica (Lavrion) GE024 10 18.839 0.020 15.681 0.014 38.855 0.039 0.83238 0.00017 2.06258 0.00041 Aegean Attica (Lavrion) GE025 27 18.800 0.007 15.675 0.006 38.829 0.018 0.83381 0.00011 2.06543 0.00032 Aegean Attica (Lavrion)

(Continues) Table 2 (Continued)

Sample Model age 206 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ Broad Euclidean ID (Ma) 204 Pb 204 Pb 204 Pb 206 Pb 206 Pb neighbours

GE027 56 18.744 0.007 15.669 0.006 38.846 0.018 0.83595 0.00010 2.07239 0.00039 Unknown W. Anatolia (Canakkale), E. Rhodopes, Betic Cordillera (Sierra del Cabo de Gata) GE015 17 18.828 0.017 15.681 0.013 38.842 0.036 0.83281 0.00014 2.06290 0.00038 Aegean Attica (Lavrion) GE016 26 18.802 0.015 15.675 0.011 38.831 0.030 0.83371 0.00012 2.06525 0.00031 Aegean Attica (Lavrion), E.

Rhodopes, Macedonia Graecia Magna Retracing (Chalkidiki), W. Anatolia (Canakkale), W. Rhodopes (Thasos) GE022 27 18.818 0.026 15.681 0.018 38.846 0.053 0.83325 0.00021 2.06431 0.00041 Aegean Attica (Lavrion) GE023 34 18.807 0.007 15.681 0.007 38.849 0.019 0.83380 0.00012 2.06570 0.00043 Aegean Attica (Lavrion), W. Anatolia (Canakkale) GE030 32 18.812 0.007 15.682 0.007 38.850 0.019 0.83360 0.00011 2.06518 0.00039 Aegean Attica (Lavrion), W.

09Uiest fOxford, of University 2019 © Anatolia (Canakkale) GE031 28 18.822 0.007 15.683 0.006 38.858 0.017 0.83325 0.00012 2.06452 0.00037 Aegean Attica (Lavrion) HE006 26 18.799 0.006 15.674 0.006 38.843 0.015 0.83377 0.00009 2.06635 0.00036 Aegean Attica (Lavrion), W. ’ Anatolia (Canakkale) silver s GE011 24 18.810 0.020 15.677 0.015 38.843 0.039 0.83347 0.00018 2.06499 0.00039 Aegean Attica (Lavrion), W. Anatolia (Canakkale) GE019 15 18.819 0.023 15.676 0.017 38.834 0.047 0.83299 0.00016 2.06350 0.00030 Aegean Attica (Lavrion) GE028 23 18.813 0.005 15.678 0.005 38.842 0.014 0.83336 0.00008 2.06473 0.00033 Aegean Attica (Lavrion), W. Anatolia (Canakkale) Archaeometry TB004* 38 18.784 0.017 15.675 0.012 38.838 0.034 0.83448 0.00015 2.06766 0.00044 Aegean Attica (Lavrion), Macedonia (Chalkidiki), W. Rhodopes (Thasos), W. Anatolia (Canakkale), E. Rhodopes 62 TB005* 29 18.805 0.008 15.678 0.007 38.844 0.019 0.83373 0.00009 2.06572 0.00035 Aegean Attica (Lavrion), W. 22)81 (2020) 1 , Anatolia (Canakkale) TB006* 28 18.812 0.016 15.680 0.013 38.849 0.034 0.83351 0.00014 2.06516 0.00038 Aegean Attica (Lavrion), W. Anatolia – 108 (Continues) 95 96 09Uiest fOxford, of University 2019 © Table 2 (Continued)

Sample Model age 206 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ Broad Euclidean ID (Ma) 204 Pb 204 Pb 204 Pb 206 Pb 206 Pb neighbours

TB007* 22 18.810 0.019 15.676 0.015 38.834 0.043 0.83341 0.00016 2.06459 0.00057 Aegean Attica (Lavrion), W. Anatolia (Canakkale), E. Archaeometry Rhodopes, Macedonia (Chalkidiki) GE009 30 18.819 0.006 15.683 0.005 38.861 0.015 0.83337 0.00008 2.06505 0.00036 Aegean Attica (Lavrion), W. Anatolia (Canakkale)

62 GE014 21 18.821 0.035 15.680 0.026 38.848 0.073 0.83303 0.00028 2.0639 0.00075 Aegean Attica (Lavrion) 22)81 (2020) 1 , GE021 42 18.788 0.020 15.678 0.015 38.850 0.042 0.83448 0.00018 2.06791 0.00038 Aegean W. Anatolia (Canakkale), E. Rhodopes, W. Rhodopes (Thasos), Attica (Lavrion), Macedonia (Chalkidiki) Birch T. – 108 TB008* 32 18.816 0.008 15.683 0.008 38.869 0.021 0.83351 0.00010 2.06576 0.00039 Aegean Attica (Lavrion), Macedonia (Chalkidiki), W. Anatolia

(Canakkale) al. et TB009* 31 18.804 0.013 15.679 0.010 38.850 0.029 0.83378 0.00013 2.06606 0.00038 Aegean Attica (Lavrion), W. Anatolia TB010* 24 18.811 0.017 15.678 0.013 38.841 0.038 0.83345 0.00019 2.06484 0.00057 Aegean Attica (Lavrion), W. Anatolia (Canakkale) TB011* 20 18.816 0.014 15.677 0.011 38.842 0.031 0.83319 0.00012 2.06431 0.00036 Aegean Attica (Lavrion), W. Anatolia (Canakkale) GE017 18 18.824 0.007 15.679 0.006 38.845 0.018 0.83296 0.00009 2.06369 0.00042 Aegean Attica (Lavrion), W. Anatolia (Canakkale) HE004 13 18.863 0.008 15.690 0.007 38.871 0.019 0.83179 0.00011 2.06060 0.00038 Aegean Attica (Lavrion) HE005 23 18.843 0.010 15.688 0.009 38.872 0.024 0.83259 0.00010 2.06295 0.00040 Aegean Attica (Lavrion) TB023* 77 18.697 0.012 15.662 0.011 38.822 0.031 0.83772 0.00014 2.07638 0.00057 Aegean E. Rhodopes, Cyclades (Siphnos) TB024* 20 18.824 0.008 15.680 0.008 38.854 0.022 0.83299 0.00013 2.06400 0.00047 Aegean Attica (Lavrion), W. Anatolia (Canakkale) GE048 25 18.823 0.009 15.682 0.008 38.856 0.023 0.83311 0.00009 2.06424 0.00039 Aegean Attica (Lavrion), W. Anatolia (Canakkale)

(Continues) Table 2 (Continued)

Sample Model age 206 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ 207 Pb/ 1σ 208 Pb/ 1σ Broad Euclidean 204 204 204 206 206 ID (Ma) Pb Pb Pb Pb Pb neighbours Graecia Magna Retracing

GE050 23 18.832 0.007 15.684 0.006 38.857 0.019 0.83291 0.00010 2.06338 0.00038 Aegean Attica (Lavrion) GE054 35 18.812 0.008 15.683 0.007 38.864 0.019 0.83368 0.00010 2.06589 0.00039 Aegean Attica (Lavrion), Macedonia (Chalkidiki), W. Anatolia TB025* 27 18.832 0.010 15.686 0.008 38.866 0.022 0.83293 0.00011 2.06380 0.00037 Aegean Attica (Lavrion) GE046 118 18.629 0.007 15.658 0.007 38.774 0.017 0.84049 0.00011 2.08121 0.00037 Unknown Basque-Cantabrian Mountains (Legorreta)

09Uiest fOxford, of University 2019 © GE049 8 18.842 0.007 15.681 0.007 38.833 0.018 0.83223 0.00010 2.06083 0.00030 Aegean Attica (Lavrion) GE051 10 18.843 0.007 15.682 0.006 38.849 0.019 0.83228 0.00010 2.06184 0.00042 Aegean Attica (Lavrion) GE053 15 18.830 0.009 15.680 0.008 38.84 0.019 0.83267 0.00012 2.0626 0.00034 Aegean Attica (Lavrion) ’ GE047 31 18.809 0.007 15.680 0.007 38.849 0.018 0.83367 0.00013 2.06544 0.00043 Aegean Attica (Lavrion), W. silver s Anatolia (Canakkale)

Asterisked (*) coins represent averages from multiple analyses (see additional supporting information S1 for all values). Pb isotope provenance interpretation: Broad = approximate geographical area; Euclidean neighbours = nearest reference data points (both ores and metallurgical (by-)products) according to their Euclidean distance. For the nearest Euclidean neighbours for each coin, see addi-

Archaeometry tional supporting information S3. 62 22)81 (2020) 1 , – 108 97 98 T. Birch et al.

(Fig. 3; see also additional supporting information S3 for the nearest Euclidean neighbours for each coin). In a close up, a major share of the samples agrees isotopically with metalliferous remains from Attica, as highlighted by the nearest Euclidean neighbours for 33 of the coins (Taras = 12, Metapontum = 11, Thurium = 7, Syracuse = 3). Of these, the nearest Euclidean neighbours for 18 of the coins are almost—and in some cases are—exclusively ores and metalliferous remains from the Laurion mines. The nearest Euclidean neighbours of two exceptional coins with significantly older Pb-Pb model ages (GE046 = 118 Ma, TB034 = 146 Ma) are ores from the Basque- Cantabrian Basin (Spain) and the Massif Central (France). Their Pb isotope signatures might also have been derived from mixed sources, that is, by addition of geologically older metal won from Variscan deposits to a geologically overall younger bullion. For example, silver from the argentiferous deposits of the Iberian Pyrite Belt—as suggested as provenance for one of the ingots of the Selinus hoard—could have been hypothetically added to predominantly Aegean metal.

DISCUSSION

Relations between elemental composition and Pb isotope data Au and Bi are generally regarded as the most informative trace elements relating to the ore source in ancient silver (Gale et al. 1980, 23; Ponting et al. 2011, 119), since they are commonly present in silver mineralizations and are enriched in argentiferous Pb during primary smelting. Contrary to Au and other precious metals, however, Bi is oxidized in the very last stages of the cupellation process (L’Héritier et al. 2015). Therefore, the Bi abundances in silver artefacts are correlated with the degree of cupellation, but are not directly linked to the geochemical signature of the treated ore. An origin of the silver from Au parting via cementation can be excluded due to the rather low Au contents (< 1 wt%; Pernicka 2017). Low Au contents have typically been associated with silver from Laurion (Ponting et al. 2011, 123), as observed in most Athenian owls (tetradrachms) published (Gale et al. 1980). However, rather low Au contents are not restricted to presumably Laurion silver. Whilst most of the ‘low-gold’ Athenian owls range from 0.02 to 0.05 wt% Au, there are examples lower still (< 0.005 wt%) as well as considerably higher (> 0.2 wt%). Anal- yses of ores from the Laurion district indicate a heterogeneous distribution of the Au content (as has also been hypothesized by Gale et al. 1980) depending on the mineral composition of the ores, which occur in most geological environments as paragenetic mixtures of different phases. In each of these phases, more or less Au is contained and subsequently variable amounts of Au are introduced into the extracted silver. In the investigated coins, the Au contents do not show a relation with the Pb isotope ratios and relatively high Au abundances are also associated with bullion presumably produced from Laurion ores (Fig. 4). Au-rich mineral associations have been described in the Laurion district (Voudouris 2005; Voudouris et al. 2008) and indeed bear the potential for substantial enrichment of Au in the silver metal extracted from such ores. Besides the relatively depleted Au contents, Gale et al. (1980) also observed low abundances of Sn, Sb, Bi and As in coins presumably produced from Laurion silver. The widespread occurrence of Ag-Bi-Sn-As-bearing phases such as sulfosalts in the ores of the Laurion district (Voudouris et al. 2008; Bonsall et al. 2011) rather imply that Laurion silver owes its observed depleted trace element signature (Gale et al. 1980) to a combination of two factors: (1) puriﬁcation of the extracted silver during metallurgical processing and (2) high ﬁneness of the bullion, that is, no introduction of trace elements by debasement with Cu.

Figure 4 Plot of Au/Ag versus 206Pb/204Pb ratios of the investigated coins, Archaic and Classical eastern Greek silver coinage (Gale et al. 1980) and Archaic western Greek coinage (Gale et al. 1980; Birch et al. in press). The range of Au/Ag and 206Pb/204Pb ratios of argentiferous ores and related metallurgical (by-)products from the Laurion district (Gale et al. 1980; Gale and Stos-Gale 1981; Stos-Gale and Gale 2009) is shown for comparison. [Colour ﬁgure can be viewed at wileyonlinelibrary.com]

Apart from Au, the platinum-group elements (i.e., Os, Ir, Ru, Rh, Pt, Pd) with the exception of Os, which easily volatilizes, as precious metals also are relatively enriched in crude Pb during primary smelting. The significance of Ir abundances for provenancing silver artefacts has been discussed controversially (Pernicka 2017; Wood et al. 2017a, 2017b). The Pt and Pd abundances determined in the investigated coins (other platinum-group elements are not certified for the used reference materials (RM)) are not related to the chemical and isotopic composition of the coins. In fact, the determined Pt and Pd values merely seem to reflect the geological background and record neither technological nor provenance information.

Potential chronological variations of the metal supply Overall, all studied mints apparently used very comparable raw material to produce their coinage, which primarily was almost exclusively derived from deposits in the broader Aegean region. As mentioned above, the deposits of Laurion were the single most important silver supplier for the investigated coins. However, production in Laurion was highest in the ﬁfth century BCE with the subsequent decrease in metal output suspended only by an intermittent rise in the mid-fourth century BCE (Meier 1990, passim). It is generally assumed that other districts in the Aegean com- pensated Laurion’s declining relevance. The scale of the workings at the Chalkidiki Peninsula, where numerous presumably antique galleries and shafts were found, are comparable with those of Laurion (Wagner et al. 1986). A major share of the investigated coins indeed clusters between Pb isotope reference data of these two districts (Fig. 5). The few known Pb isotope values of metallurgical debris from sites at the Biga Peninsula in north-western Anatolia overlap with data of smelting remains from Chalkidiki and Attica and consequently also with some of the investigated coins. Hellenistic and potentially earlier mining activities have been documented for several lo- calities there (Pernicka et al. 1984), rendering it a potential metal source as well. The island group of the Cyclades hosts several occurrences of argentiferous ores; only Siphnos, however, is proven to have been an important source of silver in ancient time (Gale and Stos-Gale 1981; Pernicka

Figure 5 208Pb/204Pb-206Pb/204Pb diagrams of the investigated coins in comparison with literature data of Ag-(Pb) ores and metallurgical debris from Ag extraction from the districts of Laurion, Chalkidiki, Biga Peninsula, Rhodopes and Siphnos (Gale et al. 1980; Gale and Stos-Gale 1981; Seeliger et al. 1985; Vavelidis et al. 1985; Wagner et al. 1986; Chalkias et al. 1988; Kalogeropoulos et al. 1989; Wagner et al. 2003; Stos-Gale and Gale 2009). The relatively high variation of 204Pb seen in the reference data might result from comparably lower precision and accuracy when these values were determined. The ﬁlling of the coin symbols (circles) corresponds to the dating of the coins: (a) Metapontum, (b) Taras, (c) Thurium and (d) Syracuse. [Colour ﬁgure can be viewed at wileyonlinelibrary.com]

1987). Datable archaeological material unambiguously revealed that mining in Siphnos ceased c.500 BCE (Pernicka and Wagner 1985). Some of the analysed coin samples from Syracuse and Thurium, though, do agree with reference data from Siphnos, hence suggesting that metal derived from this district decades ago still is present in circulated coins due to recycling. In the southern Rhodopes several precious metal mineralizations are located, of which literature data of ores from the eastern (the district around Essimi and Kirki) and western parts (Thasos) of the mountain range directly overlaps with Pb isotope values of the investigated coins. For Thasos at least, pre-Roman metal production, potentially also of silver besides Pb, has been attested (Pernicka et al. 1981). The other districts still await a systematic archaeometallurgical study. The precious metal mineralizations of the Pangaion Mountains are historically linked with the Macedon King Philip II, who in 356 BCE gained control over this district and allegedly intensiﬁed its metal output considerably (Diodorus Siculus, Bibliotheca Historica, 16, 8, 4). Ore extraction in the Pangaion as well as in the neighbouring Lekani Range around Palaia Kavala dates back already to at least the Classical and Archaic periods (Vavelidis et al. 1985; Pernicka 1987; Unger 1987). Overall, the Pb isotope analyses do not show a clearly deﬁned trend paralleling the changing relevance of Aegean mining districts outlined above (Fig. 5). Particularly Attica besides Chalkidiki (and potentially the Biga Peninsula) remain important silver sources throughout the

© 2019 University of Oxford, Archaeometry 62, 1 (2020) 81–108 Retracing Magna Graecia’s silver 101 dating range of the investigated coins—or rather metal produced from these districts still domi- nates the circulating coin issues without much change of the supply. The recorded intensified metal production from ores of the Rhodopes in northern Greece or specifically the Pangaion Mountains in the Hellenistic period cannot be deduced from our data set. In fact, the Rhodope Mountains were identified as the most likely silver source already for several of the Archaic coins from Magna Graecia (Birch et al. in press) and mainland Greece (Stos-Gale 2017).

Implications for a recycling-based bullion supply and its consequences The Pb isotope data of the investigated coins clearly imply that Magna Graecia did not use local sources, that is, argentiferous mineralizations of the Italian mainland or Sardinia (Swainbank et al. 1982; cf. Boni and Koeppel 1985; Ludwig et al. 1989; Valera et al. 2005; Stos-Gale and Gale 2009). Instead, the colonies relied on imported metal. The position of the settlements would ren- der trade with the eastern and western Mediterranean possible. The Pb isotope signature of one ingot from the Selinus hoard indicates that metal from the Iberian Peninsula, besides sources in the Aegean, was accessed by the colonies. Of the coins investigated, however, only two potentially argue for a contribution of Iberian metal (see above) and hence the Iberian Peninsula does not seem to have been an important metal supplier for Magna Graecia. In fact, the metal sources of the colonial mints apparently were equal to those of mainland Greece (Gale et al. 1980; Stos- Gale 2017), not only in the Classical and Hellenistic periods discussed here but also for the Ar- chaic period (Birch et al. in press). In the archaeological record, metal from mainland Greece is ubiquitously present in Magna Graecia. Coin hoards in Sicily frequently comprise Corinthian staters and Athenian tetradrachms besides other coins from the eastern Greek sphere (Rowan 2013b; Rutter 2016). In the fourth century BCE, coins minted by Corinth even constitute the dominant issues in these hoard ﬁnds (Rowan 2013b). In southern Italy, coinage from Corinth and Athens and overstrikes on coins from these two mints are rarely found. Presumably, this is a consequence of the incompatibility of weight standards common in southern Italy with those employed by Corinth and Athens (see above). The weight standard of Syracuse in contrast is the same as the Athenian and double the Corinthian one, hence permitting direct coining. Owing to the differing weight standards and the difﬁculty to erase completely the imagery on the older coins, overstrikes are altogether a rare phe- nomenon in the Greek world (de Callataÿ 2018) and the mints presumably rather remelted and restruck such coinage. In southern Italy and Sicily, although still rare, it seems to have been a bit more frequent than elsewhere, but largely restricted to brief episodes. Using this evidence and established network connections based on other artefacts (e.g., ce- ramics) and art styles (i.e., cock type on Himera coinage, southern Italy, being inspired by Corin- thian vases), Rowan (2013b) argues that eastern Greek silver coinages can themselves be interpreted as a traded material commodity, a silver bullion source for western Greek coinage. Pb isotope data of Corinthian and Athenian Archaic coinage scatters isotopically between reference data from Laurion, Chalkidiki and Siphnos (Gale et al. 1980; Stos-Gale 2017) and as such fully coincides with the present analyses. The ubiquitous occurrence of metal originally derived from Aegean deposits throughout Magna Graecia also mirrors the observation that colonies, regardless of their different motherland roots (Achaean, Corinthian, etc.), had access to broadly the same metal sources. A likely explanation for the occasional potentially Iberian provenance of bullion can also be found in coin hoards, which partially comprise Carthaginian silver coinage (i.e., IGCH 2144, 2146, 2186, 2187). This might explain the potential Iberian provenance for the coin from

Thurium (GE034) struck in the period 400–350 BCE, as this occurs after the period when Car- thage started to mint silver coins (410 BCE at the earliest). However, for the earlier coin from Syr- acuse (GE046) minted in 440–430 BCE, the possible Iberian provenance cannot relate to Carthaginian coinage, but may relate to Carthaginian influence (such as the Selinus ingots indi- cation of Iberian silver in the sixth century BCE and Sicily’s strong Carthaginian presence/influence on the western part of the island from 500 BCE onwards). For the interpretation of chemical and isotopic signatures, the hypothesis of a largely recycling- based metal supply in which the mints frequently derived bullion from remelting of eastern Greek coinages has a significant impact. Both the Pb isotope signatures and the content of elements, which remain in the silver, are thereby homogenized. As a consequence, the relevance of elemental and isotopic patterns for the provenance of the original metal sources is notably impaired and may even fail to provide detailed information. For the set of coins studied here, it was hence not generally possible to follow the way of silver from the mine(s) to the mints. The essential ques- tions, however, could be answered by overall retracing possible routes of bullion supply and embedding of the findings in the archaeological context.

Identifying debased versus cupelled silver The identification of debased silver is highly problematic for several reasons. In cupellation, Pb, Cu (and other minor/trace elements) will be gradually removed from the silver. The fineness of silver, however, is heterogeneous within the cupellation hearth and is higher close to the air inlet where the oxidation effect is most intense (cf. Flament et al. 2017). The fineness of cupelled silver is also related to the number of cupellation steps. Experiments by Pernicka and Bachmann (1983) demonstrate that crude Pb with 4 wt% Cu may yield silver metal still containing up to 2.2 wt% Cu after a one-step cupellation, or produce highly pure silver (< 0.5 wt% Cu) after a two-step cupellation. While Cu abundances of ≥ 10 wt% in the analysed silver coins are surely the result of debasement, defining the lower limits of threshold values for the Cu content of debased silver (and distinguishing it from cupelled silver) is not straightforward. The ultimate fineness of silver de- pends on a multitude of different factors (the Cu content of the ore, cupellation and/or debasement) and therefore it is very difficult to define the lower threshold limits of Cu content for cupelled and debased silver. Some observations in the coin results are suggestive of silver debasement. The positive correlations observed between Cu and other elements (Ni, As and Sb) indicate that these elements are associated and may have been introduced together with the Cu. While the Sn contents of the coins analysed are generally < 100 ppm, they appear to show an increase during the third century BCE (≈100–300 ppm). This is also the case for As (generally < 50 ppm), which shows an increase during the mid-third century BCE (≈ 100–200 ppm). The increase in Sn and As, which are associated with Cu, may relate to Cu additions in debased silver. The lack of correlation between Cu and Sn support the same conclusion made by Gale et al. (1980, 21–22) for Archaic Greek coinage that fresh Cu, rather than Cu-alloy scrap, was being added. Only one of the later coins from Taras (GE009, 272–240 BCE) contains ≈1.3 wt% Sn and 13.5 wt% Cu, indicating the addition of scrap bronze in the order of 9.6 wt% Sn. The decision for or against debasement of the silver is further complicated by the presumably complex history of the coin bullion. The rarity of overstriking (de Callataÿ 2018) is also in favour of the metal being reused. Silver in Magna Graecia is assumed to have arrived as minted coins from the Greek mainland, that is, the metal was obtained through trade and some of it was even- tually used for minting local coinage. Several potential cycles of melting and metal mixing,

Figure 6 Principal components analysis (PCA) biplot of silver coinage trace-element composition (variables = Cr, Co, Ni, Zn, As, Se, Pd, Cd, Sb, Te, Pt, Au and Bi) accounting for 72.1% of the total variance. Robust PCA analysis was per- formed on isometric log ratio (ilr-)transformed compositional data according to the R package ‘robCompositions’ (Templ et al. 2011) on 63 complete cases: (a) cases labelled according to mint; and (b) cases labelled according to Euclidean neighbours (overlapping symbols represents multiple Euclidean neighbour possibilities, i.e., Rhodopes and Anatolia are represented by an open circle with overlapping cross). [Colour ﬁgure can be viewed at wileyonlinelibrary.com]

© 2019 University of Oxford, Archaeometry 62, 1 (2020) 81–108 104 T. Birch et al. including the addition of recycled material, might blur the trace element signatures of the coin bullion on its way from the mines to the mints. Furthermore, coin bullion that was once debased might have been ‘purified’ when producing new coinage by adding silver with a higher fineness to the melting pot. Generally, and in contrast to Cu (alloy) coinage, where ‘fresh’ metal from the mines was coming in at a higher rate and more metal overall was in circulation, silver was exten- sively reused and remelted. Figure 6 shows a principal components analysis (PCA) of a subset of trace elements of the silver coinage analysed, highlighting no correspondence between trace element composition and Pb isotope pattern (Euclidean neighbours) or mint. As a consequence of this presumably complex material history, no significant relation between the trace element signature of the coins and their Pb isotope pattern is discernible.

CONCLUSIONS The elemental and Pb isotopic composition of the investigated coins are overall comparable. The samples from Syracuse are marked by a highly ﬂuctuating composition, which appears to be un- related to their dating. For Metapontum, Taras and Thurium, an increase of the Cu content is generally noted for younger coins. The debasement of the coins also manifests in elevated abundances of Ni, As, Sb and Se, which are introduced together with the Cu. The bullion supply of the mints is assumed to have been largely based on the recycling of coinage from the Greek mainland, as archaeological evidence also indicates (Rowan 2013b). As such, the initial sources of metal are equal to those of eastern Greek coinages (Gale et al. 1980; Hardwick et al. 1998; Stos-Gale 2017) and comprise Laurion as the single most important supplier besides ore deposits in northern Greece (Chalkidiki, Rhodopes) and potentially north-western Anatolia. For some coins, metal apparently was derived from deposits in Siphnos. The hypothesized large-scaled remelting of eastern Greek coinage homogenizes geochemical indices and hence has the potential to obscure direct provenance information.

ACKNOWLEDGEMENTS This work was funded by the Volkswagen Foundation (under the Lichtenberg scheme), whose financial support is thankfully acknowledged. The drafting of this paper was also supported by the Danish National Research Foundation (grant number DNRF119)—Centre of Excellence for Urban Network Evolutions (UrbNet). The work was also supported by the Frankfurt Isotope and Element Research Center (FIERCE), Goethe-Universität Frankfurt, Frankurt am Main, Germany; FIERCE is financially supported by the Wilhelm and Else Heraeus Foundation, which is gratefully acknowledged. This is FIERCE contribution No. 4. The authors are greatly indebted to the curators of the university coin collections of Gießen (Professor A. Klöckner and Dr M. Recke), Heidelberg (Professor C. Witschel and Dr S. Börner) and Tübingen (Professor Th. Schäfer and Dr S. Krmnicek), who generously gave permission to sample their coin collections. M. Bladt and N. Prawitz (Goethe University Frankfurt) and P. Späthe (University Würzburg) are thanked for the preparation of the metallographic blocks. The authors are also grateful to the two reviewers for comments and suggestions. Sampling, method development (LA-ICP-MS multi- standard element quantification), analysis of coins and preliminary draft were undertaken by T. B. Precision and accuracy data gathered reflect the entire analytical duration (30 months) of the project, jointly undertaken by T.B. (30 months) and K.J.W. (six months). S.K., H.-M.S. and H. E.H. set up the analytical protocols for MC-ICP-MS, LA-ICP-MS and EPMA, respectively. The overall project was designed by F.K., who also obtained the funding. K.J.W. and F.K.

© 2019 University of Oxford, Archaeometry 62, 1 (2020) 81–108 Retracing Magna Graecia’s silver 105 significantly improved the manuscript and discussion, embedding the results in a cultural historical context and, most importantly, refined the final interpretation from Aegean silver to remelted archaic coinage. Special credit is due to K.J.W. who played a decisive role in seeing the paper through the final production stages, for which it would otherwise be overly delayed. All authors contributed to and approved the final manuscript.

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SUPPORTING INFORMATION Additional supporting information may be found online in the Supporting Information section at the end of the article. S1. Detailed description of the sampling and analytical protocol with results reported from accuracy and precision testing.

S2. Full results: spreadsheet containing the complete compositional and Pb isotope data of the investigated coins, including Pb-Pb model ages calculated according to Stacey and Kramers (1975). Normalized electron probe microanalyser (EPMA) (wt%) with the raw analytical total provided; laser ablation-inductively coupled-mass spectrometry (LA-ICP-MS) data are expressed in ppm. The analytical error of the respective data is denoted as ‘_err’ and is given as 1σ for EMPA, LA-ICP-MS and Pb isotope data. Note the four forgeries (f). Nomenclature and dating of the coins are from Boehringer (1993), Caccamo Caltabianco et al. (1997), Rutter (2001) and the

Syllogue Nummorum Graecorum (Danish National Museum 1981; American Numismatic Soci- ety 1988).

S3. Euclidean distances: spreadsheet containing the nearest 100 Euclidean neighbours (sorted in ascending order from nearest to farthest) compiled from reference data (ores and metalliferous residues). Those neighbours whose distance (d) is within the largest analytical error (1σ) of a coin (often the 208Pb/204Pb ratio) are highlighted in bold. The literature database comprises ores, metallurgical (by-)products and artefacts from Pb-Ag metallurgy; references are supplied in the spreadsheet. Some neighbours can be excluded immediately based on their archaeological/geographical incongruence (i.e., Tunisia).