Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing
<jats:p>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...
| Main Authors: | , , , , , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
Copernicus GmbH
2023
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| Online Access: | https://hdl.handle.net/1721.1/148582 |
| _version_ | 1811005578547298304 |
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| 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 |
| author2 | Massachusetts Institute of Technology. Department of Civil and Environmental Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Civil and Environmental Engineering 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 |
| collection | MIT |
| description | <jats:p>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 aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms
the sensitivity of aerosol IRF to the PI aerosol loading and the
need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.
</jats:p> |
| first_indexed | 2024-09-23T16:38:27Z |
| format | Article |
| id | mit-1721.1/148582 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T16:38:27Z |
| publishDate | 2023 |
| publisher | Copernicus GmbH |
| record_format | dspace |
| spelling | mit-1721.1/1485822023-03-17T03:02:15Z 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 Massachusetts Institute of Technology. Department of Civil and Environmental Engineering <jats:p>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 aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading and the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes. </jats:p> 2023-03-16T17:18:41Z 2023-03-16T17:18:41Z 2022 2023-03-16T17:15:01Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/148582 Fung, Ka Ming, Heald, Colette L, Kroll, Jesse H, Wang, Siyuan, Jo, Duseong S et al. 2022. "Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing." Atmospheric Chemistry and Physics, 22 (2). en 10.5194/ACP-22-1549-2022 Atmospheric Chemistry and Physics Creative Commons Attribution 4.0 International license https://creativecommons.org/licenses/by/4.0/ application/pdf Copernicus GmbH Copernicus Publications |
| spellingShingle | 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 |
| title | 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_short | 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 |
| url | https://hdl.handle.net/1721.1/148582 |
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