Direct Frequency Comb Measurement of OD + CO -> DOCO Kinetics

The kinetics of the OH + CO reaction, fundamental to both atmospheric and combustion chemistry, are complex due to the formation of the HOCO intermediate. Despite extensive studies on this reaction, HOCO has not been observed at thermal reaction conditions. Exploiting the sensitive, broadband, and h...

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Veröffentlicht in:arXiv.org 2016-08
Hauptverfasser: Bjork, Bryce J, Bui, Thinh Q, Heckl, Oliver H, Changala, P Bryan, Spaun, Ben, Heu, Paula, Follman, David, Deutsch, Christoph, Cole, Garrett D, Aspelmeyer, Markus, Okumura, Mitchio, Ye, Jun
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creator Bjork, Bryce J
Bui, Thinh Q
Heckl, Oliver H
Changala, P Bryan
Spaun, Ben
Heu, Paula
Follman, David
Deutsch, Christoph
Cole, Garrett D
Aspelmeyer, Markus
Okumura, Mitchio
Ye, Jun
description The kinetics of the OH + CO reaction, fundamental to both atmospheric and combustion chemistry, are complex due to the formation of the HOCO intermediate. Despite extensive studies on this reaction, HOCO has not been observed at thermal reaction conditions. Exploiting the sensitive, broadband, and high-resolution capabilities of time-resolved cavity-enhanced direct frequency comb spectroscopy, we observe OD + CO reaction kinetics with the detection of stabilized trans-DOCO, the deuterated analogue of trans-HOCO, and its yield. By simultaneously measuring the time-dependent concentrations of both trans-DOCO and OD species, we observe unambiguous low-pressure termolecular dependence on the reaction rate coefficients for both N2 and CO bath gases. These results confirm the HOCO formation mechanism and quantify its yield.
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subjects Broadband
Combustion chemistry
Deuteration
Low pressure
Organic chemistry
Physics - Atomic Physics
Physics - Chemical Physics
Physics - Optics
Pressure dependence
Reaction kinetics
Time dependence
title Direct Frequency Comb Measurement of OD + CO -> DOCO Kinetics
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