Velocity map imaging of OH radical products from IR activated (CH3)2COO Criegee intermediates

Li, Hongwei; Kidwell, Nathanael M.; Wang, Xiaohong; Bowman, Joel M.; Lester, Marsha I.

doi:10.1063/1.4962361

Title: Velocity map imaging of OH radical products from IR activated (CH₃)₂COO Criegee intermediates

Journal Article · Mon Sep 12 00:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4962361· OSTI ID:1467883

^[1];

^[1]; Wang, Xiaohong ^[2];

^[2]; Lester, Marsha I. ^[1]

Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Chemistry
Emory Univ., Atlanta, GA (United States). Dept. of Chemistry

The unimolecular dissociation dynamics of the dimethyl-substituted Criegee intermediate (CH₃)₂COO is examined experimentally using velocity map imaging to ascertain the translational and internal energy distributions of the OH and H₂CC(CH₃)O radical products. The energy profile of key features along the reaction coordinate is also evaluated theoretically. Unimolecular decay of (CH₃)₂COO is initiated by vibrational activation in the CH stretch overtone region and the resultant OH X²Π_3/2 (v = 0) products are state-selectively ionized and imaged. Analysis reveals an isotropic spatial distribution, indicative of a 3 ps lower limit for the timescale of dissociation, and a broad and unstructured total kinetic energy release distribution. The energy released to products is partitioned principally as internal excitation of the H₂CC(CH₃)O fragments with modest translational excitation of the fragments and a small degree of OH rotational excitation. The total kinetic energy release distribution observed for (CH₃)₂COO is compared with that predicted for statistical partitioning over product quantum states, and contrasted with recent experimental and quasi-classical trajectory results for syn-CH₃CHOO [N. M. Kidwell et al., Nat. Chem. 8, 509 (2016)].

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

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

Grant/Contract Number:: FG02-87ER13792; FG02-97ER14782

OSTI ID:: 1467883

Alternate ID(s):: OSTI ID: 1323993

Journal Information:: Journal of Chemical Physics, Vol. 145, Issue 10; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Cited by: 11 works

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Deep tunneling in the unimolecular decay of CH ₃ CHOO Criegee intermediates to OH radical products Fang, Yi; Liu, Fang; Barber, Victoria P. The Journal of Chemical Physics, Vol. 145, Issue 23 https://doi.org/10.1063/1.4972015	journal	December 2016
Tunneling effects in the unimolecular decay of (CH ₃ ) ₂ COO Criegee intermediates to OH radical products Fang, Yi; Barber, Victoria P.; Klippenstein, Stephen J. The Journal of Chemical Physics, Vol. 146, Issue 13 https://doi.org/10.1063/1.4979297	journal	April 2017
Photodissociation Dynamics of Carbon Dioxide Cation via the Vibrationally Mediated Ã ² Π _u,1/2 State: A Time-Sliced Velocity-Mapped Ion Imaging Study Mao, Rui; He, Chao; Chen, Min Chinese Journal of Chemical Physics, Vol. 30, Issue 2 https://doi.org/10.1063/1674-0068/30/cjcp1611208	journal	April 2017
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