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GEOPHYSICAL RESEARCH LETTERS, VOL. 25, NO. 1, PAGES 59–62, 1998

Direct Observation of OH Production from the Ozonolysis of Olefins

Neil M. Donahue

Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts

Jesse H. Kroll

Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts

James G. Anderson

Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts

Kenneth L. Demerjian

Department of Earth and Atmospheric Sciences, and Atmospheric Sciences Research Center, SUNY, Albany

Abstract

Ozone olefin reactions may be a significant source of OH in the urban atmosphere, but current evidence for OH production is indirect and contested. We report the first direct observation of OH radicals from the reaction of ozone with a series of olefins (ethene, isoprene, trans-2-butene and 2,3 dimethyl-2-butene) in 4-6 torr of nitrogen. Using LIF to directly observe the steady-state of OH produced by the initial ozone-olefin reaction and subsequently destroyed by the OH-olefin reaction, we are able to establish OH yields broadly consistent with indirect values. The identification of the OH is unequivocal, and there is no indication that it is produced by a secondary process. To support these observations, we present a complete ab-initio potential energy surface for the O₃-ethene reaction, extending from the reactants to available products.

Received 29 July 1996; accepted 24 November 1996.

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Citation: Donahue, N. M., J. H. Kroll, J. G. Anderson, and K. L. Demerjian (1998), Direct Observation of OH Production from the Ozonolysis of Olefins, Geophys. Res. Lett., 25(1), 59–62.

Copyright 1998 by the American Geophysical Union.