Ultraviolet spectrum and photochemistry of the simplest Criegee intermediate CH2OO

Beames, Joseph M. ORCID: https://orcid.org/0000-0002-5508-8236, Liu, Fang, Lu, Lu and Lester, Marsha I. 2012. Ultraviolet spectrum and photochemistry of the simplest Criegee intermediate CH2OO. Journal of the American Chemical Society 134 (49) , pp. 20045-20048. 10.1021/ja310603j

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Abstract

Ozonolysis of alkenes in the troposphere produces Criegee intermediates, which have eluded detection in the gas phase until very recently. This laboratory has synthesized the simplest Criegee intermediate within a quartz capillary tube affixed to a pulsed valve to cool and isolate CH2OO in a supersonic expansion. UV excitation resonant with the B 1A′ ← X 1A′ transition depletes the ground-state population of CH2OO, which is detected by single-photon ionization at 118 nm. The large UV-induced depletion (approaching 100%) near the peak of the profile at 335 nm is indicative of rapid dissociation, consistent with the repulsive B 1A′ potential along the O–O coordinate computed theoretically. The experimental spectrum is in very good accord with the absorption spectrum calculated using the one-dimensional reflection principle. The B ← X spectrum is combined with the solar actinic flux to estimate an atmospheric lifetime for CH2OO at midday on the order of ∼1 s with respect to photodissociation.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry
Subjects:	Q Science > QD Chemistry
Publisher:	American Chemical Society
ISSN:	0002-7863
Last Modified:	10 Dec 2022 02:22
URI:	https://orca.cardiff.ac.uk/id/eprint/72857

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