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Titel |
Combining Bayesian methods and aircraft observations to constrain the HO. + NO2 reaction rate |
VerfasserIn |
B. H. Henderson, R. W. Pinder, J. Crooks, R. C. Cohen, A. G. Carlton, H. O. T. Pye, W. Vizuete |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 12, no. 2 ; Nr. 12, no. 2 (2012-01-16), S.653-667 |
Datensatznummer |
250010521
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Publikation (Nr.) |
copernicus.org/acp-12-653-2012.pdf |
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Zusammenfassung |
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 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 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. |
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