Atmos. Chem. Phys. Discuss., 11, 24191-24231, 2011
www.atmos-chem-phys-discuss.net/11/24191/2011/
doi:10.5194/acpd-11-24191-2011
© Author(s) 2011. This work is distributed
under the Creative Commons Attribution 3.0 License.
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Combining Bayesian methods and aircraft observations to constrain the HO. + NO2 reaction rate
B. H. Henderson1,2, R. W. Pinder2, J. Crooks3, R. C. Cohen4, A. G. Carlton5, H. O. T. Pye2, and W. Vizuete1
1Department of Environmental Science and Engineering, University of North Carolina, Chapel Hill, NC, USA
2National Exposure Research Laboratory, US Environmental Protection Agency (USEPA), RTP, NC, USA
3National Health and Environmental Effects Research Laboratory, US Environmental Protection Agency (USEPA), RTP, NC, USA
4Departments of Chemistry and Earth and Planetary Sciences, University of California, Berkeley, CA, USA
5Department of Environmental Sciences, Rutgers, New Brunswick, NJ, USA

Abstract. Tropospheric ozone is the third strongest greenhouse gas, and has the highest uncertainty in radiative forcing of the top five greenhouse gases. Throughout the troposphere, ozone is produced by radical oxidation of nitrogen oxides (NOx = NO + NO2). In the upper troposphere (8–10 km), current chemical transport models under-estimate nitrogen dioxide (NO2) observations. Improvements to simulated NOx emissions from lightning have increased NO2 predictions, but the predictions in the upper troposphere remain biased low. The upper troposphere has low temperatures (T < 250 K) that increase the uncertainty of many important chemical reaction rates. This study constrains uncertain reaction rates by combining model predictions with measurements from the Intercontinental Chemical Transport Experiment-North America observational campaign. The results show that the nitric acid formation rate, which is the dominant sink of NO2 and radicals, is currently over-estimated by 22 % in the upper troposphere. The results from this study suggest that the temperature sensitivity of nitric acid formation is lower than currently recommended. Since the formation of nitric acid removes nitrogen dioxide and radicals that drive the production of ozone, the revised reaction rate will affect ozone concentrations in upper troposphere impacting climate and air quality in the lower troposphere.

Citation: Henderson, B. H., Pinder, R. W., Crooks, J., Cohen, R. C., Carlton, A. G., Pye, H. O. T., and Vizuete, W.: Combining Bayesian methods and aircraft observations to constrain the HO. + NO2 reaction rate, Atmos. Chem. Phys. Discuss., 11, 24191-24231, doi:10.5194/acpd-11-24191-2011, 2011.
 
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