Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing
Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and...
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Online Access: | http://www.osti.gov/servlets/purl/1847069 https://www.osti.gov/biblio/1847069 https://doi.org/10.5194/acp-22-1549-2022 |
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ftosti:oai:osti.gov:1847069 2023-07-30T04:05:38+02:00 Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing Fung, Ka Ming Heald, Colette L. Kroll, Jesse H. Wang, Siyuan Jo, Duseong S. Gettelman, Andrew Lu, Zheng Liu, Xiaohong Zaveri, Rahul A. Apel, Eric C. Blake, Donald R. Jimenez, Jose-Luis Campuzano-Jost, Pedro Veres, Patrick R. Bates, Timothy S. Shilling, John E. Zawadowicz, Maria 2023-02-23 application/pdf http://www.osti.gov/servlets/purl/1847069 https://www.osti.gov/biblio/1847069 https://doi.org/10.5194/acp-22-1549-2022 unknown http://www.osti.gov/servlets/purl/1847069 https://www.osti.gov/biblio/1847069 https://doi.org/10.5194/acp-22-1549-2022 doi:10.5194/acp-22-1549-2022 54 ENVIRONMENTAL SCIENCES 2023 ftosti https://doi.org/10.5194/acp-22-1549-2022 2023-07-11T10:10:22Z Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is -0.11 W m -2 . The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the ... Other/Unknown Material North Atlantic SciTec Connect (Office of Scientific and Technical Information - OSTI, U.S. Department of Energy) Atmospheric Chemistry and Physics 22 2 1549 1573 |
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SciTec Connect (Office of Scientific and Technical Information - OSTI, U.S. Department of Energy) |
op_collection_id |
ftosti |
language |
unknown |
topic |
54 ENVIRONMENTAL SCIENCES |
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54 ENVIRONMENTAL SCIENCES Fung, Ka Ming Heald, Colette L. Kroll, Jesse H. Wang, Siyuan Jo, Duseong S. Gettelman, Andrew Lu, Zheng Liu, Xiaohong Zaveri, Rahul A. Apel, Eric C. Blake, Donald R. Jimenez, Jose-Luis Campuzano-Jost, Pedro Veres, Patrick R. Bates, Timothy S. Shilling, John E. Zawadowicz, Maria Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing |
topic_facet |
54 ENVIRONMENTAL SCIENCES |
description |
Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is -0.11 W m -2 . The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the ... |
author |
Fung, Ka Ming Heald, Colette L. Kroll, Jesse H. Wang, Siyuan Jo, Duseong S. Gettelman, Andrew Lu, Zheng Liu, Xiaohong Zaveri, Rahul A. Apel, Eric C. Blake, Donald R. Jimenez, Jose-Luis Campuzano-Jost, Pedro Veres, Patrick R. Bates, Timothy S. Shilling, John E. Zawadowicz, Maria |
author_facet |
Fung, Ka Ming Heald, Colette L. Kroll, Jesse H. Wang, Siyuan Jo, Duseong S. Gettelman, Andrew Lu, Zheng Liu, Xiaohong Zaveri, Rahul A. Apel, Eric C. Blake, Donald R. Jimenez, Jose-Luis Campuzano-Jost, Pedro Veres, Patrick R. Bates, Timothy S. Shilling, John E. Zawadowicz, Maria |
author_sort |
Fung, Ka Ming |
title |
Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing |
title_short |
Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing |
title_full |
Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing |
title_fullStr |
Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing |
title_full_unstemmed |
Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing |
title_sort |
exploring dimethyl sulfide (dms) oxidation and implications for global aerosol radiative forcing |
publishDate |
2023 |
url |
http://www.osti.gov/servlets/purl/1847069 https://www.osti.gov/biblio/1847069 https://doi.org/10.5194/acp-22-1549-2022 |
genre |
North Atlantic |
genre_facet |
North Atlantic |
op_relation |
http://www.osti.gov/servlets/purl/1847069 https://www.osti.gov/biblio/1847069 https://doi.org/10.5194/acp-22-1549-2022 doi:10.5194/acp-22-1549-2022 |
op_doi |
https://doi.org/10.5194/acp-22-1549-2022 |
container_title |
Atmospheric Chemistry and Physics |
container_volume |
22 |
container_issue |
2 |
container_start_page |
1549 |
op_container_end_page |
1573 |
_version_ |
1772817691300593664 |