Journal
SCIENCE
Volume 345, Issue 6204, Pages 1596-1598Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1257158
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Funding
- NSF [CHE-1112016, CHE-1362835, CHE-1213347]
- Dreyfus Postdoctoral Program in Environmental Chemistry [EP-12-025]
- American Chemical Society Petroleum Research Fund [ACS PRF 53320-ND6]
- U.S. Air Force Office of Scientific Research (USAFOSR) PECASE award under AFOSR [FA9950-13-1-0157]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1362835, 1213347] Funding Source: National Science Foundation
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Ozonolysis of alkenes, an important nonphotolytic source of hydroxyl (OH) radicals in the troposphere, proceeds through energized Criegee intermediates that undergo unimolecular decay to produce OH radicals. Here, we used infrared (IR) activation of cold CH3CHOO Criegee intermediates to drive hydrogen transfer from the methyl group to the terminal oxygen, followed by dissociation to OH radicals. State-selective excitation of CH3CHOO in the CH stretch overtone region combined with sensitive OH detection revealed the IR spectrum of CH3CHOO, effective barrier height for the critical hydrogen transfer step, and rapid decay dynamics to OH products. Complementary theory provides insights on the IR overtone spectrum, as well as vibrational excitations, structural changes, and energy required to move from the minimum-energy configuration of CH3CHOO to the transition state for the hydrogen transfer reaction.
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