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

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 conden...

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Bibliographic Details
Published in:	Proceedings of the National Academy of Sciences - PNAS 2020-03, Vol.117 (9), p.4505-4510
Main Authors:	Veres, Patrick R., Neuman, J. Andrew, Bertram, Timothy H., Assaf, Emmanuel, Wolfe, Glenn M., Williamson, Christina J., Weinzierl, Bernadett, Tilmes, Simone, Thompson, Chelsea R., Thames, Alexander B., Schroder, Jason C., Saiz-Lopez, Alfonso, Rollins, Andrew W., Roberts, James M., Price, Derek, Peischl, Jeff, Nault, Benjamin A., Møller, Kristian H., Miller, David O., Meinardi, Simone, Li, Qinyi, Lamarque, Jean-Francois, Kupc, Agnieszka, Kjaergaard, Henrik G., Kinnison, Douglas, Jimenez, Jose L., Jernigan, Christopher M., Hornbrook, Rebecca S., Hills, Alan, Dollner, Maximilian, Day, Douglas A., Cuevas, Carlos A., Campuzano-Jost, Pedro, Burkholder, James, Bui, T. Paul, Brune, William H., Brown, Steven S., Brock, Charles A., Bourgeois, Ilann, Blake, Donald R., Apel, Eric C., Ryerson, Thomas B.
Format:	Article
Language:	eng
Subjects:	Airborne observation Atmosphere Atmospheric models Biogeochemistry Climate effects Condensates Condensation nuclei Dimethyl sulfide Earth Resources And Remote Sensing Oceans Oxidation Physical Sciences Solar radiation Sulfides Sulfur
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Summary:	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.
ISSN:	0027-8424 1091-6490