2017
DOI: 10.1021/acs.jpclett.7b02864
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Time-Resolved Kinetic Chirped-Pulse Rotational Spectroscopy in a Room-Temperature Flow Reactor

Abstract: Chirped-pulse Fourier transform millimeter-wave spectroscopy is a potentially powerful tool for studying chemical reaction dynamics and kinetics. Branching ratios of multiple reaction products and intermediates can be measured with unprecedented chemical specificity; molecular isomers, conformers, and vibrational states have distinct rotational spectra. Here we demonstrate chirped-pulse spectroscopy of vinyl cyanide photoproducts in a flow tube reactor at ambient temperature of 295 K and pressures of 1-10 μbar… Show more

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Cited by 22 publications
(22 citation statements)
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“…Using the ATcT results from the SI appendix, table S5 of ref. 43, we find that this reaction is slightly endothermic: Δ r H°(0K) = 5.01 kcal/mol. According to the photofragment translational spectroscopy study of Hall and coworkers (12), the average kinetic energy release in the CH 2 CHCN → CH 2 CCN + H reaction is near 4 kcal/mol, with its distribution extending to 10 kcal/mol.…”
Section: Significancementioning
confidence: 72%
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“…Using the ATcT results from the SI appendix, table S5 of ref. 43, we find that this reaction is slightly endothermic: Δ r H°(0K) = 5.01 kcal/mol. According to the photofragment translational spectroscopy study of Hall and coworkers (12), the average kinetic energy release in the CH 2 CHCN → CH 2 CCN + H reaction is near 4 kcal/mol, with its distribution extending to 10 kcal/mol.…”
Section: Significancementioning
confidence: 72%
“…A fundamental difficulty in the use of CPmmW spectroscopy is understanding how the observed intensity of only one rotational transition relates to a vibrational population. The relevant equations require the existence and knowledge of the rotational temperature (43). The contribution to our measured VPD from TSs that release products with very high rotational excitation (23,24,26,54), which are not thermalized to the ambient temperature in the detection volume, will be underestimated relative to nascent product populations in the low-J states (43).…”
Section: Significancementioning
confidence: 99%
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