Rapid cloud removal of dimethyl sulfide oxidation products limits SO2 and cloud condensation nuclei production in the marine boundary layer

Novak, Gordon A.; Fite, Charles H.; Holmes, Christopher D.; Veres, Patrick R.; Neuman, J. Andrew; Faloona, Ian; Thornton, Joel A.; Wolfe, Glenn M.; Vermeuel, Michael P.; Jernigan, Christopher M.; Peischl, Jeff; Ryerson, Thomas B.; Thompson, Chelsea R.; Bourgeois, Ilann; Warneke, Carsten; Gkatzelis, Georgios I.; Coggon, Mathew M.; Sekimoto, Kanako; Bui, T. Paul; Dean-Day, Jonathan; Diskin, Glenn S.; DiGangi, Joshua P.; Nowak, John B.; Moore, Richard H.; Wiggins, Elizabeth B.; Winstead, Edward L.; Robinson, Claire; Thornhill, K. Lee; Sanchez, Kevin J.; Hall, Samuel R.; Ullmann, Kirk; Dollner, Maximilian; Weinzierl, Bernadett; Blake, Donald R.; Bertram, Timothy H.

doi:10.1073/pnas.2110472118

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Rapid cloud removal of dimethyl sulfide oxidation products limits SO2 and cloud condensation nuclei production in the marine boundary layer

2021
By Novak, Gordon A. ; Fite, Charles H. ; Holmes, Christopher D. ; ...
Source: PNAS, 118(42): e2110472118

[PDF-1.18 MB]

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Proceedings of the National Academy of Sciences
Personal Author:

Novak, Gordon A. ; Fite, Charles H. ; Holmes, Christopher D. ; Veres, Patrick R. ; Neuman, J. Andrew ; ... More +

Novak, Gordon A. ; Fite, Charles H. ; Holmes, Christopher D. ; Veres, Patrick R. ; Neuman, J. Andrew ; Faloona, Ian ; Thornton, Joel A. ; Wolfe, Glenn M. ; Vermeuel, Michael P. ; Jernigan, Christopher M. ; Peischl, Jeff ; Ryerson, Thomas B. ; Thompson, Chelsea R. ; Bourgeois, Ilann ; Warneke, Carsten ; Gkatzelis, Georgios I. ; Coggon, Mathew M. ; Sekimoto, Kanako ; Bui, T. Paul ; Dean-Day, Jonathan ; Diskin, Glenn S. ; DiGangi, Joshua P. ; Nowak, John B. ; Moore, Richard H. ; Wiggins, Elizabeth B. ; Winstead, Edward L. ; Robinson, Claire ; Thornhill, K. Lee ; Sanchez, Kevin J. ; Hall, Samuel R. ; Ullmann, Kirk ; Dollner, Maximilian ; Weinzierl, Bernadett ; Blake, Donald R. ; Bertram, Timothy H. Less -
NOAA Program & Office:

OAR (Oceanic and Atmospheric Research) ; CSL (Chemical Sciences Laboratory) ; CIRES (Cooperative Institute for Research in Environmental Sciences)

OAR (Oceanic and Atmospheric Research) ; CSL (Chemical Sciences Laboratory) ; CIRES (Cooperative Institute for Research in Environmental Sciences) Less -
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Oceans emit large quantities of dimethyl sulfide (DMS) to the marine atmosphere. The oxidation of DMS leads to the formation and growth of cloud condensation nuclei (CCN) with consequent effects on Earth's radiation balance and climate. The quantitative assessment of the impact of DMS emissions on CCN concentrations necessitates a detailed description of the oxidation of DMS in the presence of existing aerosol particles and clouds. In the unpolluted marine atmosphere, DMS is efficiently oxidized to hydroperoxymethyl thioformate (HPMTF), a stable intermediate in the chemical trajectory toward sulfur dioxide (SO2) and ultimately sulfate aerosol. Using direct airborne flux measurements, we demonstrate that the irreversible loss of HPMTF to clouds in the marine boundary layer determines the HPMTF lifetime (tau(HPMTF) < 2 h) and terminates DMS oxidation to SO2. When accounting for HPMTF cloud loss in a global chemical transport model, we show that SO2 production from DMS is reduced by 35% globally and near-surface (0 to 3 km) SO2 concentrations over the ocean are lowered by 24%. This large, previously unconsidered loss process for volatile sulfur accelerates the timescale for the conversion of DMS to sulfate while limiting new particle formation in the marine atmosphere and changing the dynamics of aerosol growth. This loss process potentially reduces the spatial scale over which DMS emissions contribute to aerosol production and growth and weakens the link between DMS emission and marine CCN production with subsequent implications for cloud formation, radiative forcing, and climate.
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Aerosols Clouds Dimethyl Sulfide Cloud Processing Marine Sulfur Sulfate Aerosol
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PNAS, 118(42): e2110472118
DOI:

https://doi.org/10.1073/pnas.2110472118
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Journal Article
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urn:sha256:57dc0aa280f0477a21cc1855c4cedab6139abe1ae7fbd344d932b56d6f0f64cf
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Rapid cloud removal of dimethyl sulfide oxidation products limits SO2 and cloud condensation nuclei production in the marine boundary layer

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