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. The oxidation of dimethyl sulfide (DMS) in the troposphere and subsequentchemical conversion into sulfur dioxide (SO2) and methane sulfonicacid (MSA) are key processes for the formation and growth ofsulfur-containing aerosol and cloud condensation nuclei (CCN), but are highlysimplified in large-scale models of the atmosphere. In this study, weimplement a series of gas-phase and multiphase sulfur oxidation mechanismsinto the Goddard Earth Observing System-Chemistry (GEOS-Chem) global chemical transport model – including two importantintermediates, dimethyl sulfoxide (DMSO) and methane sulphinic acid (MSIA) – toinvestigate the sulfur cycle in the global marine troposphere. We found thatDMS is mainly oxidized in the gas phase by OH (66 %), NO3(16 %) and BrO (12 %) globally. DMS + BrO is important for themodel's ability to reproduce the observed seasonality of surface DMS mixingratio in the Southern Hemisphere. MSA is mainly produced from multiphaseoxidation of MSIA by OH(aq) (66 %) and O3(aq) (30 %)in cloud droplets and aerosols. Aqueous-phase reaction with OH accounts foronly 12 % of MSA removal globally, and a higher MSA removal rate is neededto reproduce observations of the MSA ∕ nssSO42- ratio. Themodeled conversion yield of DMS into SO2 and MSA is 75 % and15 %, respectively, compared to 91 % and 9 % in the standard model runthat includes only gas-phase oxidation of DMS by OH and NO3. Theremaining 10 % of DMS is lost via deposition of intermediates DMSO andMSIA. The largest uncertainties for modeling sulfur chemistry in the marineboundary layer (MBL) are unknown concentrations of reactive halogens (BrO andCl) and OH(aq) concentrations in cloud droplets and aerosols. Toreduce uncertainties in MBL sulfur chemistry, we should prioritizeobservations of reactive halogens and OH(aq).

DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry