TY - JOUR
T1 - Global airborne sampling reveals a previously unobserved dimethyl sulfide oxidation mechanism in the marine atmosphere
AU - Veres, Patrick R.
AU - Andrew Neuman, J.
AU - Bertram, Timothy H.
AU - Assaf, Emmanuel
AU - Wolfe, Glenn M.
AU - Williamson, Christina J.
AU - Weinzierl, Bernadett
AU - Tilmes, Simone
AU - Thompson, Chelsea R.
AU - Thames, Alexander B.
AU - Schroder, Jason C.
AU - Saiz-Lopez, Alfonso
AU - Rollins, Andrew W.
AU - Roberts, James M.
AU - Price, Derek
AU - Peischl, Jeff
AU - Nault, Benjamin A.
AU - Møller, Kristian H.
AU - Miller, David O.
AU - Meinardi, Simone
AU - Li, Qinyi
AU - Lamarque, Jean François
AU - Kupc, Agnieszka
AU - Kjaergaard, Henrik G.
AU - Kinnison, Douglas
AU - Jimenez, Jose L.
AU - Jernigan, Christopher M.
AU - Hornbrook, Rebecca S.
AU - Hills, Alan
AU - Dollner, Maximilian
AU - Day, Douglas A.
AU - Cuevas, Carlos A.
AU - Campuzano-Jost, Pedro
AU - Burkholder, James
AU - Paul Bui, T.
AU - Brune, William H.
AU - Brown, Steven S.
AU - Brock, Charles A.
AU - Bourgeois, Ilann
AU - Blake, Donald R.
AU - Apel, Eric C.
AU - Ryerson, Thomas B.
N1 - Publisher Copyright:
© 2020 National Academy of Sciences. All rights reserved.
PY - 2020/3/3
Y1 - 2020/3/3
N2 - 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.
AB - 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.
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U2 - 10.1073/pnas.1919344117
DO - 10.1073/pnas.1919344117
M3 - Article
C2 - 32071211
AN - SCOPUS:85081150573
SN - 0027-8424
VL - 117
SP - 4505
EP - 4510
JO - Proceedings of the National Academy of Sciences of the United States of America
JF - Proceedings of the National Academy of Sciences of the United States of America
IS - 9
ER -