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Modification of aerosol mass and size distribution due to aqueous-phase SO₂ oxidation in clouds: Comparisons of several models

Kreidenweis, Sonia M. and Walcek, Chris J. and Feingold, Graham and Gong, Wanmin and Jacobson, Mark Z. and Kim, Cheol-Hee and Liu, Xiaohong and Penner, Joyce E. and Nenes, Athanasios and Seinfeld, John H. (2003) Modification of aerosol mass and size distribution due to aqueous-phase SO₂ oxidation in clouds: Comparisons of several models. Journal of Geophysical Research. Atmospheres, 108 (D7). Art. No. 4213. ISSN 2169-897X. doi:10.1029/2002jd002697.

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Models of aerosol scavenging and aqueous-phase oxidation of SO₂ by H₂O₂ and O₃ in a cloud updraft are compared. Bulk models considering only a single droplet size are compared with size-resolved models that explicitly simulate multiple aerosol and drop sizes. All models simulate growth of cloud drops on a lognormal ammonium bisulfate aerosol distribution, and subsequent aqueous-phase chemistry during adiabatic ascent. In agreement with earlier published studies, it is found that relative to bulk models, the size-resolved cloud chemical models consistently calculate 2–3 times more oxidation via the SO₂ + O₃ pathway, due to calculated variability of cloud water pH among cloud drops. All models calculate high scavenging of the input dry aerosol mass, but the calculated number of cloud drops formed varies from 275–358 drops cm⁻³. Differences in the calculated number of cloud drops formed result from the treatment of gaseous species uptake, solution thermodynamics, applied water condensation mass accommodation coefficient, and bin size range definitions over which the input aerosol distribution is numerically approximated. The difference in calculated cloud drop number can under many conditions propagate to appreciable variations in cloud albedo. It is found that the modifications to the aerosol size and mass spectrum are sensitive to the number of cloud drops formed, and differences in the processed aerosol spectra were found to induce up to 13% differences in calculated light extinction properties of the modified particle distributions. These significant discrepancies among cloud aerosol chemistry interaction models, even when used to simulate relatively simple conditions, suggest that parameterizations of these processes used in larger-scale cloud, regional and longer-term climate models can contain high levels of uncertainty.

Item Type:Article
Related URLs:
URLURL TypeDescription
Kreidenweis, Sonia M.0000-0002-2561-2914
Feingold, Graham0000-0002-0774-2926
Gong, Wanmin0000-0003-3635-0857
Jacobson, Mark Z.0000-0002-4315-4128
Kim, Cheol-Hee0000-0002-2967-4987
Liu, Xiaohong0000-0002-3994-5955
Penner, Joyce E.0000-0001-5577-452X
Nenes, Athanasios0000-0003-3873-9970
Seinfeld, John H.0000-0003-1344-4068
Additional Information:The authors thank two anonymous reviewers for helpful comments which greatly improved the manuscript. S. K. and G. F. acknowledge support of NOAA Office of Global Programs grants NA67RJ0152 and NA17RJ1228. A. N. acknowledges the support of Office of Naval Research grant N00014-96-1-0119. C. W. acknowledges the U.S. Environmental Protection Agency (EPA) for support under grant R82792901. M. J. acknowledges support from the National Science Foundation (grant ATM 0101596), National Aeronautics and Space Administration (grant NAG5-8645) and the EPA.
Funding AgencyGrant Number
National Oceanic and Atmospheric Administration (NOAA)NA67RJ0152
National Oceanic and Atmospheric Administration (NOAA)NA17RJ1228
Office of Naval Research (ONR)N00014-96-1-0119
Environmental Protection Agency (EPA)R82792901
Issue or Number:D7
Record Number:CaltechAUTHORS:20230221-180045100.1
Persistent URL:
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:119338
Deposited By: Tony Diaz
Deposited On:21 Feb 2023 22:02
Last Modified:21 Feb 2023 22:02

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