Sulfate and nitrate firn concentrations on the Greenland ice sheet: 2. Temporal anthropogenic deposition changes

Intercomparison of three new chemical ice core records from northern Greenland (covering the time span from approximately 1500 A.D. to present) with previously published records for southern and central Greenland reveals a uniform timing of anthropogenic changes in sulfate and nitrate firn concentrations over the entire ice sheet. The anthropogenic sulfate increase started around 1890, was interrupted by a transient decrease in the 1930s, and has resumed a major increase since 1950. Since the late 1970s though, a significant 30% decline in Greenland sulfate firn levels can be documented. The maximum anthropogenic increase in northern Greenland sulfate firn concentrations (up to 200–230 ppb) is 2–3 times larger than in southern and central Greenland. Nitrate records show an essentially steady increase since 1950 and, documented for the first time, a slight reduction during most recent years. Maximum nitrate firn levels of 100–130 ppb exceed the preindustrial background by 100% all over the Greenland ice sheet. Comparison with anthropogenic SO2 and NOx emission records indicates that the major increase in sulfate firn concentrations since 1950 can be attributed to Eurasian sources, while firn levels during the first half of this century appear to be dominated by North American emissions. A stronger North American source contribution is indicated over the entire 20th century in the case of nitrate. Applying a macroscopic deposition model separate time series for wet and dry deposition were derived which revealed a close correspondence of wet deposited sulfate with the timing of U.S. emissions, while the temporal evolution of Eurasian emissions is mainly reflected in the dry sulfate deposition record. During this century wet sulfate deposition increased by a factor of two while the total dry sulfate deposition flux increased by more than 500%. Wet and dry nitrate deposition both increased by 100% during the same period.