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Atmos Chem Phys
| Title: | Constraining remote oxidation capacity with ATom observations |
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| Author(s): | Travis KR; Heald CL; Allen HM; Apel EC; Arnold SR; Blake DR; Brune WH; Chen X; Commane R; Crounse JD; Daube BC; Diskin GS; Elkins JW; Evans MJ; Hall SR; Hintsa EJ; Hornbrook RS; Kasibhatla PS; Kim MJ; Luo G; McKain K; Millet DB; Moore FL; Peischl J; Ryerson TB; Sherwen T; Thames AB; Ullmann K; Wang X; Wennberg PO; Wolfe GM; Yu F; |
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| Address: | "Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA. Department of Earth, Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA, USA. Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA, USA. Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA. Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK. Department of Chemistry, University of California Irvine, Irvine, CA, USA. Department of Meteorology, Pennsylvania State University, University Park, PA, USA. University of Minnesota, Department of Soil, Water and Climate, St. Paul, MN, USA. Dept. of Earth & Environmental Sciences of Lamont-Doherty Earth Observatory and Columbia University, Palisades, NY, USA. Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA. Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA. NASA Langley Research Center, Hampton, VA, USA. Global Monitoring Division, NOAA Earth System Research Laboratory, Boulder, CO, USA. Wolfson Atmospheric Chemistry Laboratories (WACL), Department of Chemistry, University of York, York, UK. National Centre for Atmospheric Science (NCAS), University of York, York, UK. Cooperative Institute for Research in Environmental Science, University of Colorado, CO, USA. Nicholas School of the Environment, Duke University, Durham, NC, USA. Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA, USA. Atmospheric Sciences Research Center, University of Albany, Albany, NY, USA. Chemical Sciences Division, NOAA Earth System Research Laboratory, Boulder, CO, USA. School of Energy and Environment, City University of Hong Kong, Hong Kong, China. Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, MD, USA" |
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| Journal Title: | Atmos Chem Phys |
| Year: | 2020 |
| Volume: | 20200703 |
| Issue: | 13 |
| Page Number: | 7753 - 7781 |
| DOI: | 10.5194/acp-20-7753-2020 |
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| ISSN/ISBN: | 1680-7316 (Print) 1680-7324 (Electronic) 1680-7316 (Linking) |
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| Abstract: | "The global oxidation capacity, defined as the tropospheric mean concentration of the hydroxyl radical (OH), controls the lifetime of reactive trace gases in the atmosphere such as methane and carbon monoxide (CO). Models tend to underestimate the methane lifetime and CO concentrations throughout the troposphere, which is consistent with excessive OH. Approximately half of the oxidation of methane and non-methane volatile organic compounds (VOCs) is thought to occur over the oceans where oxidant chemistry has received little validation due to a lack of observational constraints. We use observations from the first two deployments of the NASA ATom aircraft campaign during July-August 2016 and January-February 2017 to evaluate the oxidation capacity over the remote oceans and its representation by the GEOS-Chem chemical transport model. The model successfully simulates the magnitude and vertical profile of remote OH within the measurement uncertainties. Comparisons against the drivers of OH production (water vapor, ozone, and NO (y) concentrations, ozone photolysis frequencies) also show minimal bias, with the exception of wintertime NO (y) . The severe model overestimate of NO (y) during this period may indicate insufficient wet scavenging and/or missing loss on sea-salt aerosols. Large uncertainties in these processes require further study to improve simulated NO (y) partitioning and removal in the troposphere, but preliminary tests suggest that their overall impact could marginally reduce the model bias in tropospheric OH. During the ATom-1 deployment, OH reactivity (OHR) below 3 km is significantly enhanced, and this is not captured by the sum of its measured components (cOHR(obs)) or by the model (cOHR(mod)). This enhancement could suggest missing reactive VOCs but cannot be explained by a comprehensive simulation of both biotic and abiotic ocean sources of VOCs. Additional sources of VOC reactivity in this region are difficult to reconcile with the full suite of ATom measurement constraints. The model generally reproduces the magnitude and seasonality of cOHR(obs) but underestimates the contribution of oxygenated VOCs, mainly acetaldehyde, which is severely underestimated throughout the troposphere despite its calculated lifetime of less than a day. Missing model acetaldehyde in previous studies was attributed to measurement uncertainties that have been largely resolved. Observations of peroxyacetic acid (PAA) provide new support for remote levels of acetaldehyde. The underestimate in both model acetaldehyde and PAA is present throughout the year in both hemispheres and peaks during Northern Hemisphere summer. The addition of ocean sources of VOCs in the model increases cOHR(mod) by 3% to 9% and improves model-measurement agreement for acetaldehyde, particularly in winter, but cannot resolve the model summertime bias. Doing so would require 100 Tg yr(-1) of a long-lived unknown precursor throughout the year with significant additional emissions in the Northern Hemisphere summer. Improving the model bias for remote acetaldehyde and PAA is unlikely to fully resolve previously reported model global biases in OH and methane lifetime, suggesting that future work should examine the sources and sinks of OH over land" |
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| Notes: | "PubMed-not-MEDLINETravis, Katherine R Heald, Colette L Allen, Hannah M Apel, Eric C Arnold, Stephen R Blake, Donald R Brune, William H Chen, Xin Commane, Roisin Crounse, John D Daube, Bruce C Diskin, Glenn S Elkins, James W Evans, Mathew J Hall, Samuel R Hintsa, Eric J Hornbrook, Rebecca S Kasibhatla, Prasad S Kim, Michelle J Luo, Gan McKain, Kathryn Millet, Dylan B Moore, Fred L Peischl, Jeffrey Ryerson, Thomas B Sherwen, Tomas Thames, Alexander B Ullmann, Kirk Wang, Xuan Wennberg, Paul O Wolfe, Glenn M Yu, Fangqun eng NNX14AP89G/NASA/NASA/ Germany 2021/03/11 Atmos Chem Phys. 2020 Jul; 20(13):7753-7781. doi: 10.5194/acp-20-7753-2020. Epub 2020 Jul 3" |
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