Global airborne sampling reveals a previously unobserved dimethyl sulfide oxidation mechanism in the marine atmosphere

Patrick R. Veres, J. Andrew Neuman, Timothy H. Bertram, Emmanuel Assaf, Glenn M. Wolfe, Christina J. Williamson, Bernadett Weinzierl, Simone Tilmes, Chelsea R. Thompson, Alexander B. Thames, Jason C. Schroder, Alfonso Saiz-Lopez, Andrew W. Rollins, James M. Roberts, Derek Price, Jeff Peischl, Benjamin A. Nault, Kristian H. Møller, David O. Miller, Simone MeinardiQinyi Li, Jean François Lamarque, Agnieszka Kupc, Henrik G. Kjaergaard, Douglas Kinnison, Jose L. Jimenez, Christopher M. Jernigan, Rebecca S. Hornbrook, Alan Hills, Maximilian Dollner, Douglas A. Day, Carlos A. Cuevas, Pedro Campuzano-Jost, James Burkholder, T. Paul Bui, William H. Brune, Steven S. Brown, Charles A. Brock, Ilann Bourgeois, Donald R. Blake, Eric C. Apel, Thomas B. Ryerson

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Abstract

Dimethyl sulfide (DMS), emitted from the oceans, is the most abundant biological source of sulfur to the marine atmosphere. Atmospheric DMS is oxidized to condensable products that form secondary aerosols that affect Earth's radiative balance by scattering solar radiation and serving as cloud condensation nuclei. We report the atmospheric discovery of a previously unquantified DMS oxidation product, hydroperoxymethyl thioformate (HPMTF, HOOCH2SCHO), identified through global-scale airborne observations that demonstrate it to be a major reservoir of marine sulfur. Observationally constrained model results show that more than 30% of oceanic DMS emitted to the atmosphere forms HPMTF. Coincident particle measurements suggest a strong link between HPMTF concentration and new particle formation and growth. Analyses of these observations show that HPMTF chemistry must be included in atmospheric models to improve representation of key linkages between the biogeochemistry of the ocean, marine aerosol formation and growth, and their combined effects on climate.

Original languageEnglish (US)
Pages (from-to)4505-4510
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume117
Issue number9
DOIs
StatePublished - Mar 3 2020

All Science Journal Classification (ASJC) codes

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    Veres, P. R., Andrew Neuman, J., Bertram, T. H., Assaf, E., Wolfe, G. M., Williamson, C. J., Weinzierl, B., Tilmes, S., Thompson, C. R., Thames, A. B., Schroder, J. C., Saiz-Lopez, A., Rollins, A. W., Roberts, J. M., Price, D., Peischl, J., Nault, B. A., Møller, K. H., Miller, D. O., ... Ryerson, T. B. (2020). Global airborne sampling reveals a previously unobserved dimethyl sulfide oxidation mechanism in the marine atmosphere. Proceedings of the National Academy of Sciences of the United States of America, 117(9), 4505-4510. https://doi.org/10.1073/pnas.1919344117