Blake, Geoffrey A. and Liang, Mao-Chang and Morgan, Crristopher G. and Yung, Yuk L. (2003) A Born-Oppenheimer photolysis model of N_2O fractionation. Geophysical Research Letters, 30 (12). Art. No. 1656. ISSN 0094-8276 http://resolver.caltech.edu/CaltechAUTHORS:20120919-090835144
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The isotopically light N_2O produced by microbial activity is thought to be balanced by the return of heavy stratospheric nitrous oxide. The Yung and Miller  method that first explained these trends yields photolytic fractionation factors ∼half those observed by experiment or predicted quantum mechanically, however. To address these issues, we present here a Born-Oppenheimer photolysis model that uses only commonly available spectroscopic data. The predicted fractionations quantitatively reproduce laboratory data, and have been incorporated into zonally averaged atmospheric simulations. Like McLinden et al.  , who employ a three-dimensional chemical transport model with cross sections scaled to match laboratory data, we find excellent agreement between predictions and stratospheric measurements; additional processes that contribute to the mass independent anomaly in N_2O can only account for a fraction of its global budget.
|Additional Information:||© 2003 American Geophysical Union. Received 15 January 2003; revised 21 March 2003; accepted 9 April 2003; published 28 June 2003. This work was supported by the Atmospheric Chemistry program of the NSF (ATM99-03790; YLY, PI). Additional NASA support to GAB is gratefully acknowledged.|
|Subject Keywords:||0317 Atmospheric Composition and Structure: Chemical kinetic and photochemical properties; 0322 Atmospheric Composition and Structure: Constituent sources and sinks.|
|Official Citation:||Blake, G. A., M.-C. Liang, C. G. Morgan, and Y. L. Yung, A Born-Oppenheimer photolysis model of N2O fractionation, Geophys. Res. Lett., 30(12), 1656, doi:10.1029/ 2003GL016932, 2003|
|Usage Policy:||No commercial reproduction, distribution, display or performance rights in this work are provided.|
|Deposited By:||Ruth Sustaita|
|Deposited On:||19 Sep 2012 16:52|
|Last Modified:||26 Dec 2012 16:12|
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