Aerosols in polluted versus nonpolluted air masses Long-range transport and effects on clouds

To assess the influence of anthropogenic aerosols on the physics and chemistry of clouds in the northeastern United States, aerosol and cloud-drop size distributions, elemental composition of aerosols as a function of size, and ionic content of cloud water were measured on Whiteface Mountain, NY, during the summers of 1981 and 1982. In several case studies, the data were cross-correlated with different air mass types - background continental, polluted continental, and maritime - that were advected to the sampling site. The results are the following: (1) Anthropogenic sources hundreds of kilometers upwind cause the small-particle (accumulation) mode number to increase from hundreds of thousands per cubic centimeter and the mass loading to increase from a few to several tens of micrograms per cubic meter, mostly in the form of sulfur aerosols. (2) A significant fraction of anthropogenic sulfur appears to act as cloud condensation nuclei (CCN) to affect the cloud drop concentration. (3) Clouds in Atlantic maritime air masses have cloud drop spectra that are markedly different from those measured in continental clouds. The drop concentration is significantly lower, and the drop size spectra are heavily skewed toward large drops. (4) Effects of anthropogenic pollutants on cloud water ionic composition are an increase of nitrate by a factor of 50, an increase of sulfate by more than one order of magnitude, and an increase of ammonium ion by a factor of 7. The net effect of the changes in ionic concentrations is an increase in cloud water acidity. An anion deficit even in maritime clouds suggests an unknown, possibly biogenic, source that could be responsible for a pH below neutral, which is frequently observed in nonpolluted clouds.