气候变化领域集成服务门户(CCPortal): Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing

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DOI	10.5194/acp-22-1549-2022
	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
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	1549
结束页码	1573
卷号	22 期号:2 页码:25
英文摘要	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 IRE. 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 WM-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.
学科领域	Environmental Sciences; Meteorology & Atmospheric Sciences
语种	英语
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号	WOS:000751425800001
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/273307
作者单位	Massachusetts Institute of Technology (MIT); Massachusetts Institute of Technology (MIT); University of Colorado System; University of Colorado Boulder; National Oceanic Atmospheric Admin (NOAA) - USA; National Center Atmospheric Research (NCAR) - USA; Texas A&M University System; Texas A&M University College Station; United States Department of Energy (DOE); Pacific Northwest National Laboratory; University of California System; University of California Irvine; University of Colorado System; University of Colorado Boulder; University of Washington; University of Washington Seattle; United States Department of Energy (DOE); Brookhaven National Laboratory
推荐引用方式 GB/T 7714	Fung, Ka Ming,Heald, Colette L.,Kroll, Jesse H.,et al. Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing[J],2022,22(2):25.
APA	Fung, Ka Ming.,Heald, Colette L..,Kroll, Jesse H..,Wang, Siyuan.,Jo, Duseong S..,...&Zawadowicz, Maria.(2022).Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(2),25.
MLA	Fung, Ka Ming,et al."Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.2(2022):25.