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Temperature dependence of the IR driven cis-trans isomerization of nitrous acid (HONO)


Botan, V; Hamm, P (2008). Temperature dependence of the IR driven cis-trans isomerization of nitrous acid (HONO). Journal of Chemical Physics, 129(11):114510.

Abstract

With the help of ultrafast time-resolved infrared spectroscopy, we investigate the temperature dependence of the IR driven cis->trans isomerization of nitrous acid (HONO) in solid Kr. We find that the lifetime of the OH-stretch vibration, as well as the final cooling into the matrix, is affected only minimally (if at all) by temperature. Nevertheless, the quantum yield of the cis-> trans isomerization reaction increases by approximate to 30% to a total of 50%-70% when lowering the temperature from 30 to 15 K, whereas the trans->cis back yield is reduced by approximate to 40%. The results are discussed in analogy to Marcus theory of nonadiabatic electron transfer for the essentially barrierless case. We present a unified view of this important prototype proton transfer reaction that can explain the high cis->trans quantum yield of close to one.

Abstract

With the help of ultrafast time-resolved infrared spectroscopy, we investigate the temperature dependence of the IR driven cis->trans isomerization of nitrous acid (HONO) in solid Kr. We find that the lifetime of the OH-stretch vibration, as well as the final cooling into the matrix, is affected only minimally (if at all) by temperature. Nevertheless, the quantum yield of the cis-> trans isomerization reaction increases by approximate to 30% to a total of 50%-70% when lowering the temperature from 30 to 15 K, whereas the trans->cis back yield is reduced by approximate to 40%. The results are discussed in analogy to Marcus theory of nonadiabatic electron transfer for the essentially barrierless case. We present a unified view of this important prototype proton transfer reaction that can explain the high cis->trans quantum yield of close to one.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:21 September 2008
Deposited On:14 Jan 2009 15:30
Last Modified:02 Jun 2016 08:13
Publisher:American Institute of Physics
ISSN:0021-9606
Additional Information:Copyright 2008 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in Journal of Chemical Physics 2008, 129(11) and may be found at http://link.aip.org/link/?JCPSA6/129/114510/1
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1063/1.2978386
PubMed ID:19044972

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