Drop size-dependent chemical composition of clouds and fogs. Part Ⅱ: Relevance to interpreting the aerosol/trace gas/fog system

摘要

Size-resolved fog drop chemical composition measurements were obtained during a radiation fog campaign near Davis, California in December 1998/January 1999 (reported in Reilly et al., Atmos. Environ. 35(33) (2001) 5717; Moore et al., Atmos. Environ, this issue). Here we explore how knowledge of this size-dependent drop composition―particularly from the newly developed Colorado State University 5-Stage cloud water collector―helps to explain additional observations in the fog environment. Size-resolved aerosol measurements before and after fog events indicate relative depletion of large ( > 2 μm in diameter) particles during fog accompanied by a relative increase in smaller aerosol particle concentrations. Fog equivalent air concentrations suggest that entrainment of additional particles and in-fog sedimentation contributed to observed changes in the aerosol size distribution. Calculated deposition velocities indicate that sedimentation was an important atmospheric removal mechanism for some species. For example, nitrite typically has a larger net deposition velocity than water and its mass is found preferentially in the largest drops most likely to sediment rapidly. Gas-liquid equilibria in fog for NO_3~-/HNO_3, NH_4~+/NH_3, and NO_2~-/HONO were examined. While these systems appear to be close to equilibrium or relative equilibrium during many time periods, divergences are observed, particularly for low liquid water content (<0.1 g m~(-3)) fogs and in different drop sizes. Knowledge of the drop size-dependent composition provided additional data useful to the interpretation of these deviations. The results suggest that data from multi-stage cloud water collectors are useful to understanding fog processes as many depend upon drop size.