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- W4247366887 abstract "<strong class=journal-contentHeaderColor>Abstract.</strong> Dimethyl sulfide (DMS) is the dominant biogenic sulfur compound in the ambient marine atmosphere. Low-volatility acids from DMS oxidation promote the formation and growth of sulfur aerosols and ultimately alter cloud properties and Earth's climate. We studied the OH-initiated oxidation of DMS in the Aarhus University Research on Aerosol (AURA) smog chamber and the marine boundary layer (MBL) with the aerosol dynamics and gas- and particle-phase chemistry kinetic multilayer model ADCHAM. Our work involved the development of a revised and comprehensive multiphase DMS oxidation mechanism, capable of both reproducing smog chamber and atmospheric relevant conditions. The secondary aerosol mass yield in the AURA chamber was found to have a strong dependence on the reaction of methyl sulfinic acid (MSIA) and OH, causing a 82.8â% increase in the total PM at low relative humidity (RH), while the autoxidation of the intermediate radical <span class=inline-formula>CH<sub>3</sub>SCH<sub>2</sub>OO</span> forming hydroperoxymethyl thioformate (HPMTF) proved important at high temperature and RH, decreasing the total PM by 55.8â%. The observations and modelling strongly support the finding that a liquid water film existed on the Teflon surface of the chamber bag, which enhanced the wall loss of water-soluble intermediates and oxidants dimethyl sulfoxide (DMSO), <span class=inline-formula>MSIA</span>, <span class=inline-formula>HPMTF</span>, <span class=inline-formula>SO<sub>2</sub></span>, methanesulfonic acid (<span class=inline-formula>MSA</span>), sulfuric acid (<span class=inline-formula>SA</span>) and <span class=inline-formula>H<sub>2</sub>O<sub>2</sub></span>. The effect caused a 64.8â% and 91.7â% decrease in the secondary aerosol mass yield obtained at both dry (0â%âRHâ12â%âRH) and humid (50â%âRHâ80â%âRH) conditions, respectively. Model runs reproducing the ambient marine atmosphere indicate that OH comprises a strong sink of DMS in the MBL (accounting for 31.1â% of the total sink flux of DMS) although less important than the combined effect of halogen species <span class=inline-formula>Cl</span> and <span class=inline-formula>BrO</span> (accounting for 24.3â% and 38.7â%, respectively). Cloudy conditions promote the production of <span class=inline-formula><math xmlns=http://www.w3.org/1998/Math/MathML id=M10 display=inline overflow=scroll dspmath=mathml><mrow class=chem><msubsup><mi mathvariant=normal>SO</mi><mn mathvariant=normal>4</mn><mrow><mn mathvariant=normal>2</mn><mo>-</mo></mrow></msubsup></mrow></math><span><svg:svg xmlns:svg=http://www.w3.org/2000/svg width=29pt height=17pt class=svg-formula dspmath=mathimg md5hash=8c898138530c760447165fe6cdc920bb><svg:image xmlns:xlink=http://www.w3.org/1999/xlink xlink:href=acp-21-9955-2021-ie00001.svg width=29pt height=17pt src=acp-21-9955-2021-ie00001.png/></svg:svg></span></span> particular mass (PM) from <span class=inline-formula>SO<sub>2</sub></span> accumulated in the gas phase, while cloud-free periods facilitate MSA formation in the deliquesced particles. The exclusion of aqueous-phase chemistry lowers the DMS sink as no halogens are activated in the sea spray particles and underestimates the secondary aerosol mass yield by neglecting <span class=inline-formula><math xmlns=http://www.w3.org/1998/Math/MathML id=M12 display=inline overflow=scroll dspmath=mathml><mrow class=chem><msubsup><mi mathvariant=normal>SO</mi><mn mathvariant=normal>4</mn><mrow><mn mathvariant=normal>2</mn><mo>-</mo></mrow></msubsup></mrow></math><span><svg:svg xmlns:svg=http://www.w3.org/2000/svg width=29pt height=17pt class=svg-formula dspmath=mathimg md5hash=97cb19aa5ca8b26a6d7fd7d4bad307d2><svg:image xmlns:xlink=http://www.w3.org/1999/xlink xlink:href=acp-21-9955-2021-ie00002.svg width=29pt height=17pt src=acp-21-9955-2021-ie00002.png/></svg:svg></span></span> and MSA PM production in the particle phase. Overall, this study demonstrated that the current DMS oxidation mechanisms reported in literature are inadequate in reproducing the results obtained in the AURA chamber, whereas the revised chemistry captured the formation, growth and chemical composition of the formed aerosol particles well. Furthermore, we emphasize the importance of OH-initiated oxidation of DMS in the ambient marine atmosphere during conditions with low sea spray emissions." @default.
- W4247366887 created "2022-05-12" @default.
- W4247366887 date "2021-04-02" @default.
- W4247366887 modified "2023-10-16" @default.
- W4247366887 title "Comment on acp-2020-1324" @default.
- W4247366887 doi "https://doi.org/10.5194/acp-2020-1324-rc1" @default.
- W4247366887 hasPublicationYear "2021" @default.
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