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Existing theoretical formulations for the size-resolved scavenging coefficient &Lambda;(d) for atmospheric aerosol particles scavenged by rain predict values lower by one to two orders of magnitude than those estimated from field measurements of particle-concentration changes for particles smaller than 3 μm in diameter. Vertical turbulence is not accounted for in the theoretical formulations of &Lambda;(d) but does contribute to the field-derived estimates of &Lambda;(d) due to its influence on the overall concentration changes of aerosol particles in the layers undergoing impaction scavenging. A detailed one-dimensional cloud microphysics model has been used to simulate rain production and below-cloud particle scavenging, and to quantify the contribution of turbulent diffusion to the overall &Lambda;(d) values calculated from particle concentration changes. The relative contribution of vertical diffusion to below-cloud scavenging is found to be largest for submicron particles under weak precipitation conditions. The discrepancies between theoretical and field-derived &Lambda;(d) values can largely be explained by the contribution of vertical diffusion to below-cloud particle scavenging for all particles larger than 0.01 μm in diameter for which field data are available. The results presented here suggest that the current theoretical framework for &Lambda;(d) can provide a reasonable approximation of below-cloud aerosol particle scavenging by rain in size-resolved aerosol transport models if vertical diffusion is also considered by the models

atmospheric chemistry and physics

On the discrepancies between theoretical and measured below-cloud particle scavenging coefficients for rain – a numerical investigation using a detailed one-dimensional cloud microphysics model