Glyoxal yield from isoprene oxidation and relation to formaldehyde: chemical mechanism, constraints from SENEX aircraft observations, and interpretation of OMI satellite data

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dc.contributor.authorMiller, Christopher Chan
dc.contributor.authorJacob, Daniel J.
dc.contributor.authorMarais, Eloise A.
dc.contributor.authorYu, Karen
dc.contributor.authorTravis, Katherine R.
dc.contributor.authorKim, Patrick S.
dc.contributor.authorFisher, Jenny A.
dc.contributor.authorZhu, Lei
dc.contributor.authorWolfe, Glenn M.
dc.contributor.authorHanisco, Thomas F.
dc.contributor.authorKeutsch, Frank N.
dc.contributor.authorKaiser, Jennifer
dc.contributor.authorMin, Kyung-Eun
dc.contributor.authorBrown, Steven S.
dc.contributor.authorWashenfelder, Rebecca A.
dc.contributor.authorAbad, Gonzalo González
dc.contributor.authorChance, Kelly
dc.date.accessioned2020-09-17T17:25:58Z
dc.date.available2020-09-17T17:25:58Z
dc.date.issued2017-07-18
dc.description.abstractGlyoxal (CHOCHO) is produced in the atmosphere by the oxidation of volatile organic compounds (VOCs). Like formaldehyde (HCHO), another VOC oxidation product, it is measurable from space by solar backscatter. Isoprene emitted by vegetation is the dominant source of CHOCHO and HCHO in most of the world. We use aircraft observations of CHOCHO and HCHO from the SENEX campaign over the southeast US in summer 2013 to better understand the CHOCHO time-dependent yield from isoprene oxidation, its dependence on nitrogen oxides (NOx  ≡  NO + NO₂), the behavior of the CHOCHO–HCHO relationship, the quality of OMI CHOCHO satellite observations, and the implications for using CHOCHO observations from space as constraints on isoprene emissions. We simulate the SENEX and OMI observations with the Goddard Earth Observing System chemical transport model (GEOS-Chem) featuring a new chemical mechanism for CHOCHO formation from isoprene. The mechanism includes prompt CHOCHO formation under low-NOx conditions following the isomerization of the isoprene peroxy radical (ISOPO₂). The SENEX observations provide support for this prompt CHOCHO formation pathway, and are generally consistent with the GEOS-Chem mechanism. Boundary layer CHOCHO and HCHO are strongly correlated in the observations and the model, with some departure under low-NOx conditions due to prompt CHOCHO formation. SENEX vertical profiles indicate a free-tropospheric CHOCHO background that is absent from the model. The OMI CHOCHO data provide some support for this free-tropospheric background and show southeast US enhancements consistent with the isoprene source but a factor of 2 too low. Part of this OMI bias is due to excessive surface reflectivities assumed in the retrieval. The OMI CHOCHO and HCHO seasonal data over the southeast US are tightly correlated and provide redundant proxies of isoprene emissions. Higher temporal resolution in future geostationary satellite observations may enable detection of the prompt CHOCHO production under low-NOx conditions apparent in the SENEX data.en_US
dc.description.sponsorshipThis work was funded by NASA ACMAP and ACCDAM and is a contribution to the NASA Aura Science Team. This research was undertaken with the assistance of resources provided at the NCI National Facility systems at the Australian National University through the National Computational Merit Allocation Scheme supported by the Australian Government. Jennifer Kaiser, Frank N. Keutsch, Glenn M. Wolfe, and Thomas F. Hanisco acknowledge support from the US EPA Science to Achieve Results (STAR) program (grant 83540601).en_US
dc.description.urihttps://acp.copernicus.org/articles/17/8725/2017/en_US
dc.format.extent14 pagesen_US
dc.genrejournal articlesen_US
dc.identifierdoi:10.13016/m2ueic-iq02
dc.identifier.citationChan Miller, C., Jacob, D. J., Marais, E. A., Yu, K., Travis, K. R., Kim, P. S., Fisher, J. A., Zhu, L., Wolfe, G. M., Hanisco, T. F., Keutsch, F. N., Kaiser, J., Min, K.-E., Brown, S. S., Washenfelder, R. A., González Abad, G., and Chance, K.: Glyoxal yield from isoprene oxidation and relation to formaldehyde: chemical mechanism, constraints from SENEX aircraft observations, and interpretation of OMI satellite data, Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, 2017.en_US
dc.identifier.urihttps://doi.org/10.5194/acp-17-8725-2017
dc.identifier.urihttp://hdl.handle.net/11603/19677
dc.language.isoen_USen_US
dc.publisherCopernicus Publicationsen_US
dc.relation.isAvailableAtThe University of Maryland, Baltimore County (UMBC)
dc.relation.isformatofUMBC Physics Department
dc.relation.isformatofUMBC Faculty Collection
dc.relation.ispartofUMBC Joint Center for Earth Systems Technology
dc.rightsThis item is likely protected under Title 17 of the U.S. Copyright Law. Unless on a Creative Commons license, for uses protected by Copyright Law, contact the copyright holder or the author.
dc.rightsPublic Domain Mark 1.0*
dc.rightsThis work was written as part of one of the author's official duties as an Employee of the United States Government and is therefore a work of the United States Government. In accordance with 17 U.S.C. 105, no copyright protection is available for such works under U.S. Law.
dc.rights.urihttp://creativecommons.org/publicdomain/mark/1.0/*
dc.titleGlyoxal yield from isoprene oxidation and relation to formaldehyde: chemical mechanism, constraints from SENEX aircraft observations, and interpretation of OMI satellite dataen_US
dc.typeTexten_US

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