Analysis of the Greenland ice core covering the period from 3000 to 500 years ago-the Greek, Roman, Medieval and Renaissance times-shows that lead is present at concentrations four times as great as natural values from about 2500 to 1700 years ago (500 B.C. to 300 A.D.). These results show that Greek and Roman lead and silver mining and smelting activities polluted the middle troposphere of the Northern Hemisphere on a hemispheric scale two millennia ago, long before the Industrial Revolution. Cumulative lead fallout to the Greenland Ice Sheet during these eight centuries was as high as 15 percent of that caused by the massive use of lead alkyl additives in gasoline since the 1930s. Pronounced lead pollution is also observed during Medieval and Renaissance times.

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.

An iridium anomaly at the Cretaceous/Tertiary boundary layer has been attributed to an extraterrestrial body that struck the Earth some 65 million years ago. It has been suggested that, during this event, the carrier of iridium was probably a micrometre-sized silicate-enclosed aggregate or the nanophase material of the vaporized impactor. But the fate of platinum-group elements (such as iridium) that regularly enter the atmosphere via ablating meteoroids remains largely unknown. Here we report a record of iridium and platinum fluxes on a climatic-cycle timescale, back to 128,000 years ago, from a Greenland ice core. We find that unexpectedly constant fallout of extraterrestrial matter to Greenland occurred during the Holocene, whereas a greatly enhanced input of terrestrial iridium and platinum masked the cosmic flux in the dust-laden atmosphere of the last glacial age. We suggest that nanometre-sized meteoric smoke particles, formed from the recondensation of ablated meteoroids in the atmosphere at altitudes >70 kilometres, are transported into the winter polar vortices by the mesospheric meridional circulation and are preferentially deposited in the polar ice caps. This implies an average global fallout of 14 +/- 5 kilotons per year of meteoric smoke during the Holocene.

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Pb, Zn, Cd and Cu have been measured using ultraclean procedures in various sections of a 70.3‐m snow/ice core covering the past 220 years (including the Industrial Revolution) drilled at Summit, central Greenland. These time series are the first reliable ones ever published for Zn, Cd, and Cu; for Pb they are the first verification of the pioneering data published more than two decades ago by C. Patterson and his coworkers [Murozumi et al., 1969]. For all four heavy metals, concentrations are found to have markedly increased up until the 1960s and 1970s before decreasing significantly during the following few decades. The timing and the amplitude of the observed changes differ significantly however from one metal to another. Comparison with concentration values obtained by analyzing ancient Holocene ice dated 7760 years B.P., that is, before humans started to impact on the atmosphere, show that no detectable increase occurred for Zn, Cd, and Cu before the Industrial Revolution. On the other hand, Pb concentrations were already one order of magnitude above natural values in late 18th century ice. Cumulative deposition of heavy metals to the whole Greenland ice cap since the Industrial Revolution ranges from 3200 t for Pb to 60 t for Cd.

Determination of copper concentrations in Greenland ice dated from seven millennia ago to the present showed values exceeding natural levels, beginning about 2500 years ago. This early large-scale pollution of the atmosphere of the Northern Hemisphere is attributed to emissions from the crude, highly polluting smelting technologies used for copper production during Roman and medieval times, especially in Europe and China. This study opens the way to a quantitative assessment of the history of early metal production, which was instrumental in the development of human cultures during ancient eras.

The Northern Hemisphere experienced dramatic changes during the last glacial, featuring vast ice sheets and abrupt climate events, while high northern latitudes during the last interglacial (Eemian) were warmer than today. Here we use high-resolution aerosol records from the Greenland NEEM ice core to reconstruct the environmental alterations in aerosol source regions accompanying these changes. Separating source and transport effects, we find strongly reduced terrestrial biogenic emissions during glacial times reflecting net loss of vegetated area in North America. Rapid climate changes during the glacial have little effect on terrestrial biogenic aerosol emissions. A strong increase in terrestrial dust emissions during the coldest intervals indicates higher aridity and dust storm activity in East Asian deserts. Glacial sea salt aerosol emissions in the North Atlantic region increase only moderately (50%), likely due to sea ice expansion. Lower aerosol concentrations in Eemian ice compared to the Holocene are mainly due to shortened atmospheric residence time, while emissions changed little.

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