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Chemical analysis of surface snows and dated ice core samples from Dye 3, Greenland, suggests that the ammonium cation is a major constituent in all samples and that the annual ammonium levels present in the south Greenland samples have varied from 3.3 to 26.3 μg/kg between the seventeenth century and the present time. The annual range of 1974–1975 surface samples was between 3.8 and 8.8 μg/kg, while the mean was 5.7±1.8 μg/kg. The recent large-scale uses of fixed nitrogen fertilizers and industrial pollution have apparently not affected the levels of ammonia reaching southern Greenland. The sodium and chloride present are predominantly derived from ocean spray, while more than 90% of the calcium is of continental origin. The levels of these three elements have not apparently been affected by human activity since the industrial revolution. Sulfate levels have increased dramatically since the industrial revolution, suggesting that sulfate of anthropogenic origin is the most important source of sulfate in modern snows from southern Greenland. The amount of the sulfuric acid neutralized by the ammonium cations was approximately 100% in the seventeenth and eighteenth centuries, dropping to approximately 20% in the 1974–1975 samples. These figures imply that there has been an increase in the acidity of precipitation in southern Greenland since the end of the eighteenth century.