Cloud processing of dimethyl sulfide (DMS) oxidation products limits sulfur dioxide (SO 2 ) and carbonyl sulfide (OCS) production in the eastern North Atlantic marine boundary layer

Kilgour, Delaney B.; Jernigan, Christopher M.; Garmash, Olga; Aggarwal, Sneha; Zhou, Shengqian; Mohr, Claudia; Salter, Matt E.; Thornton, Joel A.; Wang, Jian; Zieger, Paul; Bertram, Timothy H.

doi:10.5194/acp-25-1931-2025

Title: Cloud processing of dimethyl sulfide (DMS) oxidation products limits sulfur dioxide (SO ₂ ) and carbonyl sulfide (OCS) production in the eastern North Atlantic marine boundary layer

Journal Article · 13 February 2025 · Atmospheric Chemistry and Physics (Online)

DOI: https://doi.org/10.5194/acp-25-1931-2025 · OSTI ID:2516784

;

; Garmash, Olga;

; Zhou, Shengqian;

;

; Thornton, Joel A.;

;

Abstract. Dimethyl sulfide (DMS) is the major sulfur species emitted from the ocean. The gas-phase oxidation of DMS by hydroxyl radicals proceeds through the stable, soluble intermediate hydroperoxymethyl thioformate (HPMTF), eventually forming carbonyl sulfide (OCS) and sulfur dioxide (SO2). Recent work has shown that HPMTF is efficiently lost to marine boundary layer (MBL) clouds, thus arresting OCS and SO2 production and their contributions to new-particle formation and growth events. To date, no long-term field studies exist to assess the extent to which frequent cloud processing impacts the fate of HPMTF. Here, we present 6 weeks of measurements of the cloud fraction and the marine sulfur species methanethiol, DMS, and HPMTF made at the Atmospheric Radiation Measurement (ARM) research facility on Graciosa Island, Azores, Portugal. Using an observationally constrained chemical box model, we determine that cloud loss is the dominant sink of HPMTF in this region of the MBL during the study, accounting for 79 %–91 % of HPMTF loss on average. When accounting for HPMTF uptake to clouds, we calculate campaign average reductions in DMS-derived MBL SO2 and OCS of 52 %–60 % and 80 %–92 % for the study period. Using yearly measurements of the site- and satellite-measured 3D cloud fraction and DMS climatology, we infer that HPMTF cloud loss is the dominant sink of HPMTF in the eastern North Atlantic during all seasons and occurs on timescales faster than what is prescribed in global chemical transport models. Accurately resolving this rapid loss of HPMTF to clouds has important implications for constraining drivers of MBL new-particle formation.

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Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0021985

OSTI ID:: 2516784

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 3 Vol. 25; ISSN 1680-7324

Publisher:: Copernicus GmbHCopyright Statement

Country of Publication:: Germany

Language:: English

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