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Numerical Investigation of Gas Scavenging by Weak Precipitation

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Abstract

A one-dimensional cloud model with size-resolved microphysics and size-resolved aqueous-phase chemistry, driven by prescribed dynamics, has been used to study gas scavenging by weak precipitation developed from low-level, warm stratiform clouds. The dependence of the gas removal rate on the physical and chemical properties of precipitation has been explored under controlled initial conditions. It is found that the removal of four gaseous species (SO2, NH3, H2O2 and HNO3) strongly depends on the total droplet surface area, regardless the mean size of droplets. The removal rates also correlate positively with the precipitation rate, especially for precipitation having a mean radius larger than 20 μm. The dependence of the scavenging coefficients on the total droplet surface area is stronger than on the precipitation rate.

The removal rates of SO2, NH3 and H2O2 by precipitation strongly depend on the others' initial concentrations. When NH3 (or H2O2) concentration is much lower than that of SO2, the removal rate of SO2 is then controlled by the concentration of H2O2 (or NH3). The removal of NH3 (or H2O2) also directly depends on the concentration of SO2. NH3 and H2O2 can also indirectly affect each other's removal rate through interaction with SO2. The scavenging coefficient of SO2 increases with the concentration ratio of NH3 to SO2 if the ratio is larger than 0.5, while the scavenging coefficient of NH3 increases with the concentration ratio of SO2 to NH3 when the ratio is smaller than 1. The scavenging coefficient of H2O2 generally increases with the concentration ratio of SO2 to H2O2. Although the Henry's law equilibrium approach seems to be able to simulate gas scavenging by cloud droplets, it causes large errors when used for simulating the scavenging of soluble gas species by droplets of precipitating sizes.

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Authors and Affiliations

  1. Air Quality Research Division, Science and Technology Branch, Environment Canada, 4905 Dufferin Street, Toronto, Ontario, M3H 5T4, Canada

    Leiming Zhang & Robert Vet

  2. Centre for Research in Earth and Space Science, York University, 4700 Keele Street, Toronto, Ontario, M3J 1P3, Canada

    Diane V. Michelangeli

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  1. Leiming Zhang
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  2. Robert Vet
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  3. Diane V. Michelangeli
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Correspondence to Leiming Zhang.

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Zhang, L., Vet, R. & Michelangeli, D.V. Numerical Investigation of Gas Scavenging by Weak Precipitation. J Atmos Chem 54, 203–231 (2006). https://doi.org/10.1007/s10874-005-9010-x

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