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Combining Bayesian methods and aircraft observations to constrain the HO. + NO2 reaction rate
Citation:
Henderson, B., R. W. PINDER, J. L. CROOKS, R. COHEN, A. G. CARLTON, H. O. PYE, AND W. Vizuete. Combining Bayesian methods and aircraft observations to constrain the HO. + NO2 reaction rate. Atmospheric Chemistry and Physics. Copernicus Publications, Katlenburg-Lindau, Germany, 12(2):653-667, (2012).
Impact/Purpose:
The National Exposure Research Laboratory′s (NERL′s) Atmospheric Modeling and Analysis Division (AMAD) conducts research in support of EPA′s mission to protect human health and the environment. AMAD′s research program is engaged in developing and evaluating predictive atmospheric models on all spatial and temporal scales for forecasting the Nation′s air quality and for assessing changes in air quality and air pollutant exposures, as affected by changes in ecosystem management and regulatory decisions. AMAD is responsible for providing a sound scientific and technical basis for regulatory policies based on air quality models to improve ambient air quality. The models developed by AMAD are being used by EPA, NOAA, and the air pollution community in understanding and forecasting not only the magnitude of the air pollution problem, but also in developing emission control policies and regulations for air quality improvements.
Description:
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 (NO,x =NO+NO2). In the upper troposphere (8–10 km), current chemical transport models under-estimate nitrogen dioxide (NO2) observations. Improvements to simulated NOx production 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 overestimated 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.
URLs/Downloads:
Combining Bayesian Methods and Aircraft Observations to Constrain the HO + NO2 Reaction Rate (PDF, NA pp, 4749 KB, about PDF)Atmospheric Chemistry and Physics
