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1 Effects of Aqueous Organo-Sulfur Chemistry on Particulate MS-to-NSS Ratios in the Marine Atmosphere

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The oxidation of Dimethyl Sulfide (CH3SCH3, DMS) in the atmosphere could influence climate by affecting cloud condensation nuclei (CCN) concentrations and cloud properties. This work focuses on elucidating the importance of DMS-cloud interactions, especially the poorly understood aqueous phase chemical transformations of DMS oxidation products. For this purpose, we incorporate an oxidation mechanism of atmospheric DMS and its products within the modeling framework of a Trajectory Ensemble Model (TEM). Both marine cumulus and stratocumulus clouds are considered. It is found that the aqueous phase reactions of sulfur compounds contribute>97 % of MS (methanesulfonate, CH3(O)S(O)O−) and>80 % of NSS (non-seasalt sulfate) production in particles, and that about 30 % of total MS and NSS production is from the aqueous phase oxidation of the organo-sulfur compounds. The aqueous phase MSI (methanesulfinate, CH3S(O)O−) + Cl2 − reaction is found to be more important than MSI + OH as

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The oxidation of Dimethyl Sulfide (CH3SCH3, DMS) in the atmosphere could influence climate by affecting cloud condensation nuclei (CCN) concentrations and cloud properties. This work focuses on elucidating the importance of DMS-cloud interactions, especially the poorly understood aqueous phase chemical transformations of DMS oxidation products. For this purpose, we incorporate an oxidation mechanism of atmospheric DMS and its products within the modeling framework of a Trajectory Ensemble Model (TEM). Both marine cumulus and stratocumulus clouds are considered. It is found that the aqueous phase reactions of sulfur compounds contribute>97 % of MS (methanesulfonate, CH3(O)S(O)O−) and>80 % of NSS (non-seasalt sulfate) production in particles, and that about 30 % of total MS and NSS production is from the aqueous phase oxidation of the organo-sulfur compounds. The aqueous phase MSI (methanesulfinate, CH3S(O)O−) + Cl2 − reaction is found to be more important than MSI + OH as

Keywords

Atmosphere (unit)ChemistryParticulatesAqueous solutionSulfurEnvironmental chemistrySulfur dioxideAtmospheric chemistry

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