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Global airborne sampling reveals a previously unobserved dimethyl sulfide oxidation mechanism in the marine atmosphere.
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-François; 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.
  • Veres PR; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305; patrick.veres@noaa.gov.
  • Neuman JA; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305.
  • Bertram TH; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Assaf E; Department of Chemistry, University of Wisconsin-Madison, Madison, WI 53706.
  • Wolfe GM; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305.
  • Williamson CJ; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Weinzierl B; Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, MD 20771.
  • Tilmes S; Joint Center for Earth Systems Technology, University of Maryland, Baltimore County, Baltimore, MD 21250.
  • Thompson CR; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305.
  • Thames AB; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Schroder JC; Faculty of Physics, Aerosol Physics and Environmental Physics, University of Vienna, 1090 Vienna, Austria.
  • Saiz-Lopez A; Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80301.
  • Rollins AW; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305.
  • Roberts JM; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Price D; Department of Meteorology and Atmospheric Science, Pennsylvania State University, University Park, PA 16801.
  • Peischl J; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Nault BA; Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309.
  • Møller KH; Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, Consejo Superior de Investigaciones Científicas, 28006 Madrid, Spain.
  • Miller DO; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305.
  • Meinardi S; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305.
  • Li Q; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Lamarque JF; Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309.
  • Kupc A; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305.
  • Kjaergaard HG; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Kinnison D; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Jimenez JL; Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309.
  • Jernigan CM; Department of Chemistry, University of Copenhagen, 1165 Copenhagen, Denmark.
  • Hornbrook RS; Department of Meteorology and Atmospheric Science, Pennsylvania State University, University Park, PA 16801.
  • Hills A; School of Physical Science, University of California, Los Angeles, CA 90095.
  • Dollner M; Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, Consejo Superior de Investigaciones Científicas, 28006 Madrid, Spain.
  • Day DA; Climate & Global Dynamics Lab, National Center for Atmospheric Research, Boulder, CO 80301.
  • Cuevas CA; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305.
  • Campuzano-Jost P; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Burkholder J; Faculty of Physics, Aerosol Physics and Environmental Physics, University of Vienna, 1090 Vienna, Austria.
  • Bui TP; Department of Chemistry, University of Copenhagen, 1165 Copenhagen, Denmark.
  • Brune WH; Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80301.
  • Brown SS; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309.
  • Brock CA; Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309.
  • Bourgeois I; Department of Chemistry, University of Wisconsin-Madison, Madison, WI 53706.
  • Blake DR; Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80301.
  • Apel EC; Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80301.
  • Ryerson TB; Faculty of Physics, Aerosol Physics and Environmental Physics, University of Vienna, 1090 Vienna, Austria.
Proc Natl Acad Sci U S A ; 117(9): 4505-4510, 2020 03 03.
Article en En | MEDLINE | ID: mdl-32071211
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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