Experimental and theoretical studies of the doubly substituted methyl-ethyl Criegee intermediate: Infrared action spectroscopy and unimolecular decay to OH radical products

Barber, Victoria P.; Hansen, Anne S.; Georgievskii, Yuri; Klippenstein, Stephen J.; Lester, Marsha I.

doi:10.1063/5.0002422

Title: Experimental and theoretical studies of the doubly substituted methyl-ethyl Criegee intermediate: Infrared action spectroscopy and unimolecular decay to OH radical products

Journal Article · Mon Mar 02 00:00:00 EST 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0002422· OSTI ID:1632301

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^[2]; Georgievskii, Yuri ^[3];

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Univ. of Pennsylvania, Philadelphia, PA (United States)
Univ. of Pennsylvania, Philadelphia, PA (United States
Argonne National Lab. (ANL), Lemont, IL (United States)

In this work the infrared (IR) action spectrum of the doubly substituted methyl-ethyl Criegee intermediate (MECI) is observed in the CH stretch overtone region with detection of OH products. The MECI exhibits four conformers, all of which undergo unimolecular decay via a 1,4 H-atom transfer mechanism, followed by the rapid release of OH products. Conformers with different orientations of the carbonyl oxide group with respect to the methyl and ethyl substituents (i.e., anti and syn) decay via distinct transition state barriers (16.1 kcal mol^–1 and 15.4 kcal mol^–1, respectively). The observed IR action spectrum is in good agreement with the predicted anharmonic IR absorption spectrum, but exhibits significant congestion, which is attributed to couplings between spectroscopic bright states and nearby dark states. Energy-dependent OH appearance rates are measured upon IR excitation of the strongest features in the IR action spectrum and are found to be on the order of 10⁶–10⁷ s^–1. The experimental rates are in good agreement with computed Rice–Ramsperger–Kassel–Marcus rates for the unimolecular decay of MECI at these energies, which incorporate quantum mechanical tunneling and sophisticated hindered rotor treatments, as well as high-level theoretical calculations of the TS barrier heights, rovibrational properties, and torsional barriers associated with the MECI conformers. Master equation modeling is used to predict thermal rates for the unimolecular decay of anti- and syn-MECI of 473 s^–1 and 660 s^–1, respectively. Comparison with other previously studied Criegee intermediate systems provides insights into substituent effects on unimolecular decay under both energy-dependent and thermal conditions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Carlsberg Foundation; Independent Research Fund Denmark; Julie von Müllens Fond

Grant/Contract Number:: AC02-06CH11357; CHE-1664572; ACI-1548562; CF18-0614; 9036-00016B

OSTI ID:: 1632301

Alternate ID(s):: OSTI ID: 1602341

Journal Information:: Journal of Chemical Physics, Vol. 152, Issue 9; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Cited by: 12 works

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