chemistry of hydrogen oxide radicals (hox) in the arctic troposphere in spring

chemistry of hydrogen oxide radicals (hox) in the arctic troposphere in spring

;L. Jaeglé;C. McNaughton;A. D. Clarke;J. H. Crawford;G. Chen;R. C. Cohen;A. J. Weinheimer;S. R. Hall;J. G. Walega;P. Weibring;A. Fried;J. L. Jimenez;M. J. Cubison;P. O. Wennberg;M. R. Beaver;K. M. Spencer;J. D. Crounse;J. M. St. Clair;W. H. Brune;X. Ren;J. R. Olson;M. J. Evans;D. J. Jacob;J. Mao;J. A. Fisher;R. M. Yantosca;P. Le Sager;C. Carouge
Journal of agricultural and food chemistry 2010 Vol. 10 pp. 5823-5838
142
jaegl2010atmosphericchemistry

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 (HOx≡H+OH+peroxy radicals) and their reservoirs (HOy≡HOx+peroxides) in the springtime Arctic atmosphere. We find that a standard gas-phase chemical mechanism overestimates the observed HO2 and H2O2 concentrations. Computation of HOx and HOy 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 HO2 uptake by aerosols, favored by low temperatures and relatively high aerosol loadings, through a mechanism that does not produce H2O2. We implemented such an uptake of HO2 by aerosol in the model using a standard reactive uptake coefficient parameterization with γ(HO2) 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 HOx species and HOy reservoirs. HO2 uptake by aerosol is then a major HOx and HOy sink, decreasing mean OH and HO2 concentrations in the Arctic troposphere by 32% and 31% respectively. Better rate and product data for HO2 uptake by aerosol are needed to understand this role of aerosols in limiting the oxidizing power of the Arctic atmosphere.

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151950
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10.5194/acp-10-5823-2010
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