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Detailed Reference Information |
Tang, Y., Carmichael, G.R., Uno, I., Woo, J., Kurata, G., Lefer, B., Shetter, R.E., Huang, H., Anderson, B.E., Avery, M.A., Clarke, A.D. and Blake, D.R. (2003). Impacts of aerosols and clouds on photolysis frequencies and photochemistry during TRACE-P: 2. Three-dimensional study using a regional chemical transport model. Journal of Geophysical Research 108: doi: 10.1029/2002JD003100. issn: 0148-0227. |
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A three-dimensional regional chemical transport model, STEM 2K1, coupled with a detailed radiation model is used to study the influences of aerosols and clouds on photolysis rates and photochemical processes over East Asia-Western Pacific during the TRACE-P period. Measured J-values are compared with those calculated using three-dimensional modeled fields of clouds and aerosols. The model is shown to accurately represent observed J-values over a broad range of conditions. Model studies with and without aerosols and clouds are performed and compared with clear-sky conditions to isolate the various influences. Clouds are shown to have a large impact on photolysis rates during the observation periods of TRACE-P, with J2> decreased by 20% below clouds and enhanced by ~30% from 1 km to 8 km. Clouds also exert a dominant influence on short-lived radicals, like OH and HO2. For March, clouds reduce OH by 23% at altitudes below 1 km and increase OH by ~25% above 1 km. Asian aerosols contain large amounts of carbonaceous material, inorganic components such as sulfates, and mineral oxides. These aerosols significantly influence J-values and photochemical processes. When averaged over all TRACE-P DC-8 and P-3 flights, the aerosol influence via affecting J-values reduces OH by ~40% below 1 km, and by ~24% above 1 km. Aerosols have a stronger impact on longer-lived chemical species than clouds do because aerosols tend to be coemitted with precursors and have a longer contact time with the polluted air masses. The accumulated aerosol impact generally is to reduce O3 concentrations by about 6 ppbv in the biomass burning plumes emitted from Southeast Asia. In megacity plumes, aerosols can increase NOx concentration by 40% via reducing its photolytic loss and reduce NOz concentration by a similar amount. A detailed case study of the DC-8 and P-3 flights on 27 March is used to make comparisons for cloud and aerosol influences. During these flights, the cloud impact on J-values is stronger than the aerosol impact, but aerosols are shown to exert a much stronger accumulated influence on O3 production. |
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Abstract |
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Keywords
Atmospheric Composition and Structure, Aerosols and particles (0345, 4801), Atmospheric Composition and Structure, Pollution--urban and regional, Atmospheric Composition and Structure, Troposphere--composition and chemistry, Meteorology and Atmospheric Dynamics, Numerical modeling and data assimilation, Meteorology and Atmospheric Dynamics, Radiative processes |
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Publisher
American Geophysical Union 2000 Florida Avenue N.W. Washington, D.C. 20009-1277 USA 1-202-462-6900 1-202-328-0566 service@agu.org |
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