Prompt release of O 1D products upon UV excitation of CH2OO Criegee intermediates

Vansco, Michael F.; Li, Hongwei; Lester, Marsha I.

doi:10.1063/1.4977987

Prompt release of O ¹D products upon UV excitation of CH₂OO Criegee intermediates

Journal Article · Mon Mar 13 00:00:00 EDT 2017 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4977987· OSTI ID:1465943

Vansco, Michael F. ^[1]; Li, Hongwei ^[2]; ^[2]

Univ. of Pennsylvania, Philadelphia, PA (United States). Department of Chemistry; Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104-6323, USA
Univ. of Pennsylvania, Philadelphia, PA (United States). Department of Chemistry

We report that velocity map imaging has been used to characterize the angular and velocity distributions of O ¹D photofragments arising from UV excitation of the simplest Criegee intermediate CH₂OO in the long wavelength tail region (364 to 417 nm) of the B¹A'–X¹A' spectrum. The O ¹D images exhibit anisotropic angular distributions indicative of rapid dissociation to H₂CO X¹A₁ + O ¹D products, which occurs faster than the rotational period (ps) of CH₂OO. As a result, the broad oscillatory structure reported previously in the long wavelength region of the UV absorption spectrum is attributed to short-lived resonances associated with the excited B¹A' state of CH₂OO, which decay by nonadiabatic coupling to repulsive singlet states. The total kinetic energy distributions show that nearly half of the available energy, on average, is partitioned to product translation. The balance results in significant internal excitation of the H₂CO co-fragments. In conclusion, the product anisotropy and energy partitioning are unchanged across the UV spectrum and consistent with previously reported experimental and theoretical findings of the CH₂OO B-X transition moment and dissociation energy to H₂CO X¹A₁ + O ¹D products.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Pennsylvania, Philadelphia, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: FG02-87ER13792

OSTI ID:: 1465943

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 1 Vol. 147; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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