Silver played a key role in the progressive monetization of early Mediterranean civilizations. We combine Pb and Ag isotopes with volatile trace elements (Bi, Sb, and As) to assess whether, during the Roman occupation of Iberia, galena constituted a significant source of silver. We find that the Pb and Ag isotopic compositions of 47 samples of galena from eight different Iberian mining provinces, many of them exploited during Roman times, are uncorrelated. This indicates that their respective isotopic variabilities depend on different petrogenetic processes. Moreover, the range of Ag isotopic abundances is approximately six times wider than that displayed worldwide by silver coins in general and Roman silver coins in particular. Although galena from the Betics provides the best fit for Pb isotopes with Roman coins, their fit with Ag isotopic compositions is at best sporadic. We suggest that, together with Sb, Bi, and As, silver is primarily derived from fluids boiled off from differentiated mantle-derived magmas. These fluids, in turn, reacted with preexisting galena and functioned as a silver trap. Lead sulfides with ε109Ag of ~0 and unusually rich in Ag, Sb, Bi, and As were the most probable sources of ancient silver, whereas samples with ε109Ag departing significantly from ~0 reflect low-temperature isotopic fractionation processes in the upper crust.

In an attempt to clarify the significance of Pb model ages in Pb-Zn sedimentary deposits, we report high-precision Pb isotopic compositions for 64 galenas and 52 K-feldspars, the former from ores and the latter separated from granites. All samples are from Spain and the French Pyrenees. Lead from galena ores is of unequivocal continental origin. With few exceptions, Pb model ages systematically exceed emplacement ages by up to 400 Ma, a gap which is well outside the uncertainties of ~30 Ma assigned to the model. The histogram of the new high-precision Pb isotope data shows prominent peaks of galena Pb model ages at 94±38 Ma and 392±39 Ma. When the data are consolidated with literature data and examined in 3-dimensional Pb isotope space, cluster analysis identifies five groups. The model ages of the peaks occur, in order of decreasing peak intensity, at 395±40 (Middle Devonian), 90±34 Ma (Middle Cretaceous), and 613±42 Ma (Neoproterozoic), with two minor peaks at 185+26 Ma (Jurassic) and 313±41 (Upper Carboniferous). To a large extent, the model ages centered around these peaks correspond to distinct localities. The ages of the peaks do not coincide with any of the Betic, Variscan, or Pan-African tectonic events, which are the main tectonic episodes that shaped Iberian geology, but rather match well-known global oceanic anoxic events. It is argued that surges of metals weathered from continental surfaces scorched during anoxic events accumulated and combined in anoxic water masses with unoxidized marine sulfide released by submarine hydrothermal activity to precipitate the primary Pb-Zn stock. Frozen Pb isotope compositions require that galenas from black shales are the source of the final ores. The Revised manuscript with no changes marked Click here to view linked References sulfides were later remobilized by large-scale convective circulation of basinal and hydrothermal fluids. The peaks of K-feldspar Pb model ages are distinct from those of galenas and do not correlate with magmatic emplacement ages. It is suggested that they instead reflect local circulation in Paleozoic sediments surrounding individual plutons. While Pbisotopes can be used as a regional provenance tool, such an approach requires that the data are considered in a fully 3-dimensional space.

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