The pollution history of the atmosphere of the Northern Hemisphere is recorded in the levels of heavy metal impurities in Greenland ice. The possibility also exists of using natural variations in the abundances of lead isotopes to trace the source of this pollution. Lead isotopes have now been measured in ancient Greenland ice with a lead concentration as low as 0.9 pg/g. The results show a depression in the 206 Pb/ 207 Pb ratio between 600 B.C. and 300 A.D., giving unequivocal evidence of early large-scale atmospheric pollution by this toxic metal. This ratio changes from ∼1.201 in ∼8-kyr-old ice to ∼1.183 about 2 kyr ago. Isotopic systematics point to the mining districts in southwest and southeast Spain as the dominant sources of this lead, giving quantitative evidence of the importance of these mining districts to the Carthaginian and Roman civilizations. Lead with a Rio Tinto-type signature represents ∼70% of the lead found in Greenland ice between ∼150 B.C. and 50 A.D. after correcting for the contribution from rock dust indexed to aluminium concentrations. MethodsSample Preparation. We have measured the isotopic composition and concentration of the lead in 26 sections of a 3029 m long ice core from Summit, Greenland (72°34′ N; 37°37′ W; elevation 3238 m), drilled during 1990-1992 for the † This paper is dedicated to the memory of Professor Clair C. Patterson, geochemist at the California Institute of Technology, whose pioneering work on environmental lead has provided the scientific foundation for this study.

IN 1969, Murozumi et al. demonstrated that the concentration of lead in Greenland snow had increased by a factor of 200 since ancient times, and concluded that most of this increase was a result of the use of alkyl-leaded petrol. Partly because of these findings, the United States and other western countries limited the use of lead additives in petrol from about 1970. Recently, Boutron et al. showed that the lead concentration in Greenland snow had decreased by a factor of ∼7.5 over the past 20 years, and suggested that this was a result of the decline in use of leaded petrol. We present here measurements of the Pb/Pb ratio of the lead contained in the samples studied by Boutron et al. Because aerosols from the atmosphere above the United States are more radiogenic than those from Eurasia, we can trace the relative contributions of these two sources in the Greenland lead over the period analysed by Boutron et al.We find that the United States was a significant source of lead in the 1970s, but it has since declined considerably in relative importance. This decline mirrors the decrease in use of leaded petrol in the United States, confirming the earlier hypothesis.

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