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• W4220797144 abstract "<strong class=journal-contentHeaderColor>Abstract.</strong> The OH-initiated oxidation of SO<span class=inline-formula>₂</span> is the dominant, first step in the transformation of this atmospherically important trace gas to particulate sulfate, and accurate rate coefficients for the title reaction under all atmospheric conditions (pressures, temperatures, and humidity) are required to assess its role in, for example, new particle formation. Prior to this study, no temperature-dependent data were available in the fall-off regime for atmospherically relevant bath gases. We thus address an important omission in the kinetic database for this reaction and highlight significant discrepancies in recommended parameterizations. In this work, generation of OH via pulsed laser photolysis at 248 and 351 nm was coupled to its detection by laser-induced fluorescence to obtain rate coefficients (<span class=inline-formula><i>k</i>₁</span>) for the title reaction at pressures of 14–742 Torr (1 Torr <span class=inline-formula>=</span> 1.333 hPa) and temperatures of 220–333 K in N<span class=inline-formula>₂</span> bath gas. In situ SO<span class=inline-formula>₂</span> concentrations, central to accurate kinetic measurements under pseudo-first-order conditions, were measured by optical absorption. Under the conditions of the present study, the termolecular reaction between OH and SO<span class=inline-formula>₂</span> is in the fall-off regime, and we parameterized the rate coefficients in N<span class=inline-formula>₂</span> in terms of low- (<span class=inline-formula><i>k</i>_1,0</span>) and high-pressure (<span class=inline-formula><i>k</i>_1,∞</span>) limiting rate coefficients and a broadening factor (<span class=inline-formula><i>F</i>_C</span>) to obtain <span class=inline-formula><math xmlns=http://www.w3.org/1998/Math/MathML id=M17 display=inline overflow=scroll dspmath=mathml><mrow><msubsup><mi>k</mi><mrow><mn mathvariant=normal>1</mn><mo>,</mo><mn mathvariant=normal>0</mn></mrow><mrow><msub><mi mathvariant=normal>N</mi><mn mathvariant=normal>2</mn></msub></mrow></msubsup><mo>=</mo><mn mathvariant=normal>3.03</mn><mo>×</mo><msup><mn mathvariant=normal>10</mn><mrow><mo>-</mo><mn mathvariant=normal>31</mn></mrow></msup></mrow></math><span><svg:svg xmlns:svg=http://www.w3.org/2000/svg width=92pt height=20pt class=svg-formula dspmath=mathimg md5hash=121727b6745b64381ab66e1fff8a77dd><svg:image xmlns:xlink=http://www.w3.org/1999/xlink xlink:href=acp-22-4969-2022-ie00001.svg width=92pt height=20pt src=acp-22-4969-2022-ie00001.png/></svg:svg></span></span> (<span class=inline-formula><math xmlns=http://www.w3.org/1998/Math/MathML id=M18 display=inline overflow=scroll dspmath=mathml><mrow><mi>T</mi><mo>/</mo><mn mathvariant=normal>300</mn></mrow></math><span><svg:svg xmlns:svg=http://www.w3.org/2000/svg width=33pt height=14pt class=svg-formula dspmath=mathimg md5hash=03aac18976628b7ce0ab3760291c3cce><svg:image xmlns:xlink=http://www.w3.org/1999/xlink xlink:href=acp-22-4969-2022-ie00002.svg width=33pt height=14pt src=acp-22-4969-2022-ie00002.png/></svg:svg></span></span> K)<span class=inline-formula>^−4.10</span> cm<span class=inline-formula>⁶</span> molecule<span class=inline-formula>^−2</span> s<span class=inline-formula>^−1</span>, <span class=inline-formula><math xmlns=http://www.w3.org/1998/Math/MathML id=M23 display=inline overflow=scroll dspmath=mathml><mrow><msub><mi>k</mi><mrow><mn mathvariant=normal>1</mn><mo>,</mo><mi mathvariant=normal>∞</mi></mrow></msub><mo>=</mo><mn mathvariant=normal>2.00</mn><mo>×</mo><msup><mn mathvariant=normal>10</mn><mrow><mo>-</mo><mn mathvariant=normal>12</mn></mrow></msup></mrow></math><span><svg:svg xmlns:svg=http://www.w3.org/2000/svg width=96pt height=17pt class=svg-formula dspmath=mathimg md5hash=adfde75fba13ac778d72c37b36cfdc56><svg:image xmlns:xlink=http://www.w3.org/1999/xlink xlink:href=acp-22-4969-2022-ie00003.svg width=96pt height=17pt src=acp-22-4969-2022-ie00003.png/></svg:svg></span></span> cm<span class=inline-formula>³</span> molecule<span class=inline-formula>^−1</span> s<span class=inline-formula>^−1</span>, and <span class=inline-formula><i>F</i>_C=0.58</span>. The effects of water vapour on the title reaction were explored through measurements in N<span class=inline-formula>₂</span>–H<span class=inline-formula>₂</span>O mixtures at 273, 298, and 333 K using the same experimental methods. The rate coefficients are significantly enhanced by the presence of water vapour with <span class=inline-formula><math xmlns=http://www.w3.org/1998/Math/MathML id=M30 display=inline overflow=scroll dspmath=mathml><mrow><msubsup><mi>k</mi><mrow><mn mathvariant=normal>1</mn><mo>,</mo><mn mathvariant=normal>0</mn></mrow><mrow><msub><mi mathvariant=normal>H</mi><mn mathvariant=normal>2</mn></msub><mi mathvariant=normal>O</mi></mrow></msubsup><mo>=</mo><mn mathvariant=normal>1.65</mn><mo>×</mo><msup><mn mathvariant=normal>10</mn><mrow><mo>-</mo><mn mathvariant=normal>30</mn></mrow></msup></mrow></math><span><svg:svg xmlns:svg=http://www.w3.org/2000/svg width=97pt height=20pt class=svg-formula dspmath=mathimg md5hash=8c7cfb6e7c7c2e3330fe6eaa443240b3><svg:image xmlns:xlink=http://www.w3.org/1999/xlink xlink:href=acp-22-4969-2022-ie00004.svg width=97pt height=20pt src=acp-22-4969-2022-ie00004.png/></svg:svg></span></span> (<span class=inline-formula><math xmlns=http://www.w3.org/1998/Math/MathML id=M31 display=inline overflow=scroll dspmath=mathml><mrow><mi>T</mi><mo>/</mo><mn mathvariant=normal>300</mn></mrow></math><span><svg:svg xmlns:svg=http://www.w3.org/2000/svg width=33pt height=14pt class=svg-formula dspmath=mathimg md5hash=971389f1e3bf9def6da596ccae29aaed><svg:image xmlns:xlink=http://www.w3.org/1999/xlink xlink:href=acp-22-4969-2022-ie00005.svg width=33pt height=14pt src=acp-22-4969-2022-ie00005.png/></svg:svg></span></span> K)<span class=inline-formula>^−4.90</span> cm<span class=inline-formula>⁶</span> molecule<span class=inline-formula>^−2</span> s<span class=inline-formula>^−1</span>, which indicates that H<span class=inline-formula>₂</span>O is a factor <span class=inline-formula><i>></i>5</span> more efficient in quenching the HOSO<span class=inline-formula>₂</span>* association complex than N<span class=inline-formula>₂</span>. A model-based comparison of our rate coefficients and parameterization with previous literature measurements and recommendations of evaluation panels are presented and discussed. The use of the new parameterization instead of the IUPAC or NASA evaluations, particularly after including H<span class=inline-formula>₂</span>O as a third-body quencher, leads to a significant (10 %–30 %) reduction in the lifetime of SO<span class=inline-formula>₂</span> in some parts of the atmosphere and increases the <span class=inline-formula><math xmlns=http://www.w3.org/1998/Math/MathML id=M42 display=inline overflow=scroll dspmath=mathml><mrow class=chem><msub><mi mathvariant=normal>H</mi><mn mathvariant=normal>2</mn></msub><msub><mi mathvariant=normal>SO</mi><mn mathvariant=normal>4</mn></msub><mo>/</mo><msub><mi mathvariant=normal>SO</mi><mn mathvariant=normal>2</mn></msub></mrow></math><span><svg:svg xmlns:svg=http://www.w3.org/2000/svg width=62pt height=14pt class=svg-formula dspmath=mathimg md5hash=82297e285d180984b5a1a526d0b74899><svg:image xmlns:xlink=http://www.w3.org/1999/xlink xlink:href=acp-22-4969-2022-ie00006.svg width=62pt height=14pt src=acp-22-4969-2022-ie00006.png/></svg:svg></span></span> ratio concomitantly." @default.
• W4220797144 created "2022-04-03" @default.
• W4220797144 creator A5081117962 @default.
• W4220797144 date "2022-03-22" @default.
• W4220797144 modified "2023-10-14" @default.
• W4220797144 title "Reply to RC2" @default.
• W4220797144 doi "https://doi.org/10.5194/acp-2021-1074-ac2" @default.
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