Field observational constraints on the controllers in glyoxal (CHOCHO) reactive uptake to aerosol

Kim, Dongwook; Cho, Changmin; Jeong, Seokhan; Lee, Soojin; Nault, Benjamin A.; Campuzano-Jost, Pedro; Day, Douglas A.; Schroder, Jason C.; Jimenez, Jose L.; Volkamer, Rainer; Blake, Donald R.; Wisthaler, Armin; Fried, Alan; DiGangi, Joshua P.; Diskin, Glenn S.; Pusede, Sally E.; Hall, Samuel R.; Ullmann, Kirk; Huey, L. Gregory; Tanner, David J.; Dibb, Jack; Knote, Christoph J.; Min, Kyung-Eun

doi:10.5194/acp-22-805-2022

Title: Field observational constraints on the controllers in glyoxal (CHOCHO) reactive uptake to aerosol

Journal Article · 17 January 2022 · Atmospheric Chemistry and Physics (Online)

DOI: https://doi.org/10.5194/acp-22-805-2022 · OSTI ID:1840812

;

; Jeong, Seokhan; Lee, Soojin;

;

; Blake, Donald R.; Wisthaler, Armin; Fried, Alan;

;

; Pusede, Sally E.; Hall, Samuel R.; Ullmann, Kirk;

; Tanner, David J. more »

Abstract. Glyoxal (CHOCHO), the simplest dicarbonyl in the troposphere, is a potential precursor for secondary organic aerosol (SOA) and brown carbon (BrC) affecting air quality and climate. The airborne measurement of CHOCHO concentrations during the KORUS-AQ (KORea–US Air Quality study) campaign in 2016 enables detailed quantification of loss mechanisms pertaining to SOA formation in the real atmosphere. The production of this molecule was mainly from oxidation of aromatics (59 %) initiated by hydroxyl radical (OH). CHOCHO loss to aerosol was found to be the most important removal path (69 %) and contributed to roughly ∼ 20 % (3.7 µg sm−3 ppmv−1 h−1, normalized with excess CO) of SOA growth in the first 6 h in Seoul Metropolitan Area. A reactive uptake coefficient (γ) of ∼ 0.008 best represents the loss of CHOCHO by surface uptake during the campaign. To our knowledge, we show the first field observation of aerosol surface-area-dependent (Asurf) CHOCHO uptake, which diverges from the simple surface uptake assumption as Asurf increases in ambient condition. Specifically, under the low (high) aerosol loading, the CHOCHO effective uptake rate coefficient, keff,uptake, linearly increases (levels off) with Asurf; thus, the irreversible surface uptake is a reasonable (unreasonable) approximation for simulating CHOCHO loss to aerosol. Dependence on photochemical impact and changes in the chemical and physical aerosol properties “free water”, as well as aerosol viscosity, are discussed as other possible factors influencing CHOCHO uptake rate. Our inferred Henry's law coefficient of CHOCHO, 7.0×108 M atm−1, is ∼ 2 orders of magnitude higher than those estimated from salting-in effects constrained by inorganic salts only consistent with laboratory findings that show similar high partitioning into water-soluble organics, which urges more understanding on CHOCHO solubility under real atmospheric conditions.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0018221

OSTI ID:: 1840812

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 2 Vol. 22; ISSN 1680-7324

Publisher:: Copernicus GmbHCopyright Statement

Country of Publication:: Germany

Language:: English

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Speciation of OH reactivity above the canopy of an isoprene-dominated forest Kaiser, J.; Skog, K. M.; Baumann, K. Atmospheric Chemistry and Physics, Vol. 16, Issue 14 https://doi.org/10.5194/acp-16-9349-2016	journal	January 2016
Modeling biogenic and anthropogenic secondary organic aerosol in China Hu, Jianlin; Wang, Peng; Ying, Qi Atmospheric Chemistry and Physics, Vol. 17, Issue 1 https://doi.org/10.5194/acp-17-77-2017	journal	January 2017
Glyoxal yield from isoprene oxidation and relation to formaldehyde: chemical mechanism, constraints from SENEX aircraft observations, and interpretation of OMI satellite data Chan Miller, Christopher; Jacob, Daniel J.; Marais, Eloise A. Atmospheric Chemistry and Physics, Vol. 17, Issue 14 https://doi.org/10.5194/acp-17-8725-2017	journal	January 2017
Liquid–liquid phase separation in organic particles containing one and two organic species: importance of the average O : C Song, Mijung; Ham, Suhan; Andrews, Ryan J. Atmospheric Chemistry and Physics, Vol. 18, Issue 16 https://doi.org/10.5194/acp-18-12075-2018	journal	January 2018
Atmospheric oxidation in the presence of clouds during the Deep Convective Clouds and Chemistry (DC3) study Brune, William H.; Ren, Xinrong; Zhang, Li Atmospheric Chemistry and Physics, Vol. 18, Issue 19 https://doi.org/10.5194/acp-18-14493-2018	journal	January 2018
Primary emissions of glyoxal and methylglyoxal from laboratory measurements of open biomass burning Zarzana, Kyle J.; Selimovic, Vanessa; Koss, Abigail R. Atmospheric Chemistry and Physics, Vol. 18, Issue 20 https://doi.org/10.5194/acp-18-15451-2018	journal	January 2018
Secondary organic aerosol production from local emissions dominates the organic aerosol budget over Seoul, South Korea, during KORUS-AQ Nault, Benjamin A.; Campuzano-Jost, Pedro; Day, Douglas A. Atmospheric Chemistry and Physics, Vol. 18, Issue 24 https://doi.org/10.5194/acp-18-17769-2018	journal	January 2018
Technical note: Updated parameterization of the reactive uptake of glyoxal and methylglyoxal by atmospheric aerosols and cloud droplets Curry, Leah A.; Tsui, William G.; McNeill, V. Faye Atmospheric Chemistry and Physics, Vol. 18, Issue 13 https://doi.org/10.5194/acp-18-9823-2018	journal	January 2018
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors Song, Mijung; Maclean, Adrian M.; Huang, Yuanzhou Atmospheric Chemistry and Physics, Vol. 19, Issue 19 https://doi.org/10.5194/acp-19-12515-2019	journal	January 2019
A new model mechanism for atmospheric oxidation of isoprene: global effects on oxidants, nitrogen oxides, organic products, and secondary organic aerosol Bates, Kelvin H.; Jacob, Daniel J. Atmospheric Chemistry and Physics, Vol. 19, Issue 14 https://doi.org/10.5194/acp-19-9613-2019	journal	January 2019
Formation and sink of glyoxal and methylglyoxal in a polluted subtropical environment: observation-based photochemical analysis and impact evaluation Ling, Zhenhao; Xie, Qianqian; Shao, Min Atmospheric Chemistry and Physics, Vol. 20, Issue 19 https://doi.org/10.5194/acp-20-11451-2020	journal	January 2020
Glyoxal's impact on dry ammonium salts: fast and reversible surface aerosol browning De Haan, David O.; Hawkins, Lelia N.; Jansen, Kevin Atmospheric Chemistry and Physics, Vol. 20, Issue 16 https://doi.org/10.5194/acp-20-9581-2020	journal	January 2020
Secondary Organic Aerosol Formation from Acetylene (C ₂ H ₂ ): seed effect on SOA yields due to organic photochemistry in the aerosol aqueous phase Volkamer, R.; Ziemann, P. J.; Molina, M. J. Atmospheric Chemistry and Physics, Vol. 9, Issue 6 https://doi.org/10.5194/acp-9-1907-2009	journal	January 2009
Glyoxal uptake on ammonium sulphate seed aerosol: reaction products and reversibility of uptake under dark and irradiated conditions Galloway, M. M.; Chhabra, P. S.; Chan, A. W. H. Atmospheric Chemistry and Physics, Vol. 9, Issue 10 https://doi.org/10.5194/acp-9-3331-2009	journal	January 2009
A compact PTR-ToF-MS instrument for airborne measurements of volatile organic compounds at high spatiotemporal resolution Müller, M.; Mikoviny, T.; Feil, S. Atmospheric Measurement Techniques, Vol. 7, Issue 11 https://doi.org/10.5194/amt-7-3763-2014	journal	January 2014
A broadband cavity enhanced absorption spectrometer for aircraft measurements of glyoxal, methylglyoxal, nitrous acid, nitrogen dioxide, and water vapor Min, K. -E.; Washenfelder, R. A.; Dubé, W. P. Atmospheric Measurement Techniques, Vol. 9, Issue 2 https://doi.org/10.5194/amt-9-423-2016	journal	January 2016
Isoprene-derived secondary organic aerosol in the global aerosol–chemistry–climate model ECHAM6.3.0–HAM2.3–MOZ1.0 Stadtler, Scarlet; Kühn, Thomas; Schröder, Sabine Geoscientific Model Development, Vol. 11, Issue 8 https://doi.org/10.5194/gmd-11-3235-2018	journal	January 2018
The Framework for 0-D Atmospheric Modeling (F0AM) v3.1 Wolfe, Glenn M.; Marvin, Margaret R.; Roberts, Sandra J. Geoscientific Model Development, Vol. 9, Issue 9 https://doi.org/10.5194/gmd-9-3309-2016	journal	January 2016

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