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Chemistry of hydrogen oxide radicals (HO_x) in the Arctic troposphere in spring

Mao, J. and St. Clair, J. M. and Crounse, J. D. and Spencer, K. M. and Beaver, M. R. and Wennberg, P. O. (2010) Chemistry of hydrogen oxide radicals (HO_x) in the Arctic troposphere in spring. Atmospheric Chemistry and Physics, 10 (13). pp. 5823-5838. ISSN 1680-7316. https://resolver.caltech.edu/CaltechAUTHORS:20100811-084643946

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Abstract

We use observations from the April 2008 NASA ARCTAS aircraft campaign to the North American Arctic, interpreted with a global 3-D chemical transport model (GEOS-Chem), to better understand the sources and cycling of hydrogen oxide radicals (HO_x≡H+OH+peroxy radicals) and their reservoirs (HO_y≡HO_x+peroxides) in the springtime Arctic atmosphere. We find that a standard gas-phase chemical mechanism overestimates the observed HO_2 and H_2O_2 concentrations. Computation of HO_x and HO_y gas-phase chemical budgets on the basis of the aircraft observations also indicates a large missing sink for both. We hypothesize that this could reflect HO_2 uptake by aerosols, favored by low temperatures and relatively high aerosol loadings, through a mechanism that does not produce H_2O_2. We implemented such an uptake of HO_2 by aerosol in the model using a standard reactive uptake coefficient parameterization with γ(HO_2) values ranging from 0.02 at 275 K to 0.5 at 220 K. This successfully reproduces the concentrations and vertical distributions of the different HO_x species and HO_y reservoirs. HO_2 uptake by aerosol is then a major HO_x and HO_y sink, decreasing mean OH and HO_2 concentrations in the Arctic troposphere by 32% and 31% respectively. Better rate and product data for HO_2 uptake by aerosol are needed to understand this role of aerosols in limiting the oxidizing power of the Arctic atmosphere.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.5194/acp-10-5823-2010 DOIArticle
http://www.atmos-chem-phys.net/10/5823/2010/acp-10-5823-2010.htmlPublisherArticle
ORCID:
AuthorORCID
St. Clair, J. M.0000-0002-9367-5749
Crounse, J. D.0000-0001-5443-729X
Wennberg, P. O.0000-0002-6126-3854
Additional Information:© Author(s) 2010. This work is distributed under the Creative Commons Attribution 3.0 License. Received: 3 March 2010 – Published in Atmos. Chem. Phys. Discuss.: 11 March 2010. Revised: 13 June 2010 – Accepted: 21 June 2010 – Published: 1 July 2010. The authors would like to thank Scot T. Martin, Hongyu Liu, Charles E. Miller, Richard A. Ferrare, Karl D. Froyd and Daniel M. Murphy for helpful discussions. We also would like to thank Yuhang Wang for providing the TOPSE dataset, Huisheng Bian for providing Fast-JX updates and Dirk Richter for contributing to the HCHO measurement. J. Mao also thanks David M. Shelow and the NASA DC-8 crew for their generous help with making HOx measurements on the aircraft. This work was supported by the NASA Tropospheric Chemistry Program. Edited by: P. Monks.
Funders:
Funding AgencyGrant Number
NASAUNSPECIFIED
Issue or Number:13
Record Number:CaltechAUTHORS:20100811-084643946
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20100811-084643946
Official Citation:Mao, J., Jacob, D. J., Evans, M. J., Olson, J. R., Ren, X., Brune, W. H., Clair, J. M. St., Crounse, J. D., Spencer, K. M., Beaver, M. R., Wennberg, P. O., Cubison, M. J., Jimenez, J. L., Fried, A., Weibring, P., Walega, J. G., Hall, S. R., Weinheimer, A. J., Cohen, R. C., Chen, G., Crawford, J. H., McNaughton, C., Clarke, A. D., Jaeglé, L., Fisher, J. A., Yantosca, R. M., Le Sager, P., and Carouge, C.: Chemistry of hydrogen oxide radicals (HOx) in the Arctic troposphere in spring, Atmos. Chem. Phys., 10, 5823-5838, doi:10.5194/acp-10-5823-2010, 2010
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:19386
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:13 Aug 2010 17:23
Last Modified:09 Mar 2020 13:19

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