[en] The anthropogenic emission and subsequent deposition of heavy metals including mercury (Hg) and lead (Pb) present human health and environmental concerns. Although it is known that local and regional sources of these metals contribute to deposition in the Great Lakes region, it is difficult to trace emissions from point sources to impacted sites. Recent studies suggest that metal isotope ratios may be useful for distinguishing between and tracing source emissions. We measured Pb, strontium (Sr), and Hg isotope ratios in daily precipitation samples that were collected at seven sites across the Great Lakes region between 2003 and 2007. Lead isotope ratios ("2"0"7Pb/"2"0"6Pb = 0.8062 to 0.8554) suggest that Pb deposition was influenced by coal combustion and processing of Mississippi Valley-Type Pb ore deposits. Regional differences in Sr isotope ratios ("8"7Sr/"8"6Sr = 0.70859 to 0.71155) are likely related to coal fly ash and soil dust. Mercury isotope ratios (δ"2"0"2Hg = − 1.13 to 0.13‰) also varied among the sites, likely due to regional differences in coal isotopic composition, and fractionation occurring within industrial facilities and in the atmosphere. These data represent the first combined characterization of Pb, Sr, and Hg isotope ratios in precipitation collected across the Great Lakes region. We demonstrate the utility of multiple metal isotope ratios in parallel with traditional trace element multivariate statistical modeling to enable more complete pollution source attribution. - Highlights: • We measured Pb, Sr, and Hg isotopes in precipitation from the Great Lakes region. • Pb isotopes suggest that deposition was impacted by coal combustion and metal production. • Sr isotope ratios vary regionally, likely due to soil dust and coal fly ash. • Hg isotopes vary due to fractionation occurring within facilities and the atmosphere. • Isotope results support conclusions of previous trace element receptor modeling

[en] Total mercury (Hg) concentrations in hair and urine are often used as biomarkers of exposure to fish-derived methylmercury (MeHg) and gaseous elemental Hg, respectively. We used Hg stable isotopes to assess the validity of these biomarkers among small-scale gold mining populations in Ghana and Indonesia. Urine from Ghanaian miners displayed similar Δ"1"9"9Hg values to Hg derived from ore deposits (mean urine Δ"1"9"9Hg=0.01‰, n=6). This suggests that urine total Hg concentrations accurately reflect exposure to inorganic Hg among this population. Hair samples from Ghanaian miners displayed low positive Δ"1"9"9Hg values (0.23–0.55‰, n=6) and low percentages of total Hg as MeHg (7.6–29%, n=7). These data suggest that the majority of the Hg in these miners' hair samples is exogenously adsorbed inorganic Hg and not fish-derived MeHg. Hair samples from Indonesian gold miners who eat fish daily displayed a wider range of positive Δ"1"9"9Hg values (0.21–1.32‰, n=5) and percentages of total Hg as MeHg (32–72%, n=4). This suggests that total Hg in the hair samples from Indonesian gold miners is likely a mixture of ingested fish MeHg and exogenously adsorbed inorganic Hg. Based on data from both populations, we suggest that total Hg concentrations in hair samples from small-scale gold miners likely overestimate exposure to MeHg from fish consumption. - Highlights: • Mercury isotopes were measured in hair and urine from small-scale gold miners. • Mercury isotopes indicate that Hg in urine comes from mining activity. • Mercury isotopes suggest Hg in hair is a mixture of fish MeHg and inorganic Hg. • A large percentage of Hg in miner’s hair is released during amalgam burning and adsorbed