Photochemical modeling of glyoxal at a rural site: observations and analysis from BEARPEX 2007

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dc.contributor.authorHuisman, A. J.
dc.contributor.authorHottle, J. R.
dc.contributor.authorGalloway, M. M.
dc.contributor.authorDiGangi, J. P.
dc.contributor.authorCoens, K. L.
dc.contributor.authorChoi, W.
dc.contributor.authorFaloona, I. C.
dc.contributor.authorGilman, J. B.
dc.contributor.authorKuster, W. C.
dc.contributor.authorGouw, J. de
dc.contributor.authorBouvier-Brown, N. C.
dc.contributor.authorGoldstein, A. H.
dc.contributor.authorLaFranchi, B. W.
dc.contributor.authorCohen, R. C.
dc.contributor.authorWolfe, G. M.
dc.contributor.authorThornton, J. A.
dc.contributor.authorDocherty, K. S.
dc.contributor.authorFarmer, D. K.
dc.contributor.authorCubison, M. J.
dc.contributor.authorJimenez, J. L.
dc.contributor.authorMao, J.
dc.contributor.authorBrune, W. H.
dc.contributor.authorKeutsch, F. N.
dc.date.accessioned2020-09-17T17:03:23Z
dc.date.available2020-09-17T17:03:23Z
dc.date.issued2011-09-01
dc.description.abstractWe present roughly one month of high time-resolution, direct, in situ measurements of gas-phase glyoxal acquired during the BEARPEX 2007 field campaign. The research site, located on a ponderosa pine plantation in the Sierra Nevada mountains, is strongly influenced by biogenic volatile organic compounds (BVOCs); thus this data adds to the few existing measurements of glyoxal in BVOC-dominated areas. The short lifetime of glyoxal of ~1 h, the fact that glyoxal mixing ratios are much higher during high temperature periods, and the results of a photochemical model demonstrate that glyoxal is strongly influenced by BVOC precursors during high temperature periods. A zero-dimensional box model using near-explicit chemistry from the Leeds Master Chemical Mechanism v3.1 was used to investigate the processes controlling glyoxal chemistry during BEARPEX 2007. The model showed that MBO is the most important glyoxal precursor (~67 %), followed by isoprene (~26 %) and methylchavicol (~6 %), a precursor previously not commonly considered for glyoxal production. The model calculated a noon lifetime for glyoxal of ~0.9 h, making glyoxal well suited as a local tracer of VOC oxidation in a forested rural environment; however, the modeled glyoxal mixing ratios over-predicted measured glyoxal by a factor 2 to 5. Loss of glyoxal to aerosol was not found to be significant, likely as a result of the very dry conditions, and could not explain the over-prediction. Although several parameters, such as an approximation for advection, were found to improve the model measurement discrepancy, reduction in OH was by far the most effective. Reducing model OH concentrations to half the measured values decreased the glyoxal over-prediction from a factor of 2.4 to 1.1, as well as the overprediction of HO2 from a factor of 1.64 to 1.14. Our analysis has shown that glyoxal is particularly sensitive to OH concentration compared to other BVOC oxidation products. This relationship arises from (i) the predominantly secondary- or higher-generation production of glyoxal from (mainly OH-driven, rather than O3-driven) BVOC oxidation at this site and (ii) the relative importance of photolysis in glyoxal loss as compared to reaction with OH. We propose that glyoxal is a useful tracer for OH-driven BVOC oxidation chemistry.en_US
dc.description.sponsorshipThe authors gratefully acknowledge the support of the University of Wisconsin-Madison Department of Chemistry. The authors would like to thank Sierra Pacific Industries for the use of their land and the University of California, Berkeley, Center for Forestry, Blodgett Forest Research Station for cooperation in facilitating this research. This work was supported by the Camille and Henry Dreyfus Foundation, a National Defense Science and Engineering Graduate Fellowship (NDSEG) funded by the Army Research Office (ARO) and NSF ATM 0852406.Development of the Madison-LIP instrument and measurements during BEARPEX 2007 were supported by NSF ATM 0724912, and the NDSEG-ARO. The NOAA GC-MS measurements weresupported by the National Science Foundation, Division of Atmospheric Sciences (grant 0516610). DKF, KSD, MJC and JLJ were supported by NSF ATM 0449815 & ATM 0919189, and a NOAA postdoctoral fellowship to DKF. A. H. G. and N. C. B.-B. weresupported by NSF ATM 0922562.en_US
dc.description.urihttps://acp.copernicus.org/articles/11/8883/2011/en_US
dc.format.extent15 pagesen_US
dc.genrejournal articlesen_US
dc.identifierdoi:10.13016/m2bhaq-znfl
dc.identifier.citationHuisman, A. J., Hottle, J. R., Galloway, M. M., DiGangi, J. P., Coens, K. L., Choi, W., Faloona, I. C., Gilman, J. B., Kuster, W. C., de Gouw, J., Bouvier-Brown, N. C., Goldstein, A. H., LaFranchi, B. W., Cohen, R. C., Wolfe, G. M., Thornton, J. A., Docherty, K. S., Farmer, D. K., Cubison, M. J., Jimenez, J. L., Mao, J., Brune, W. H., and Keutsch, F. N.: Photochemical modeling of glyoxal at a rural site: observations and analysis from BEARPEX 2007, Atmos. Chem. Phys., 11, 8883–8897, https://doi.org/10.5194/acp-11-8883-2011, 2011.en_US
dc.identifier.urihttps://doi.org/10.5194/acp-11-8883-2011
dc.identifier.urihttp://hdl.handle.net/11603/19675
dc.language.isoen_USen_US
dc.publisherCopernicus Publicationsen_US
dc.relation.isAvailableAtThe University of Maryland, Baltimore County (UMBC)
dc.relation.ispartofUMBC Joint Center for Earth Systems Technology
dc.relation.ispartofUMBC Physics Department
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.titlePhotochemical modeling of glyoxal at a rural site: observations and analysis from BEARPEX 2007en_US
dc.typeTexten_US

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