A three-dimensional stochastic model is developed for predicting atmospheric aerosol collection and aggregation on the surface of a falling raindrop at its terminal velocity. Potential flow and viscous flow are assumed as the flow fields in the vicinity of the large and the small raindrops, respectively. The results show that hydrophobic coarse mode aerosols collected by either small raindrops (d(c) 100m) or large drops (d(c) 100m) form aggregations on the surfaces of drops, and accumulation mode aerosols tend to be captured by the aggregations or hydrophobic coarse particles which have been collected by the drops, and this may significantly enhance the capability of the raindrop for fine aerosol collection. When the aggregation effect is considered in the calculation, fine aerosol efficiency can be promoted by one to two orders of magnitude. Therefore, fine particle collision efficiency by raindrops is underestimated by employing the classical dynamic theory which neglects the particle aggregation effect. However, the collection efficiency of coarse particles remains almost constant with the increase in the amount of particles collected by large drops, while there is only a slight increase in efficiency by small raindrops upon increasing in particle concentration. This implies that the traditional limiting trajectory method can still be used for the calculation of coarse particle collection efficiencies by either small or large raindrops.Copyright (c) 2018 American Association for Aerosol Research
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