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Intramolecular vibrational energy relaxation in nitrous acid (HONO)


Botan, V; Hamm, P (2008). Intramolecular vibrational energy relaxation in nitrous acid (HONO). Journal of Chemical Physics, 129(16):164506.

Abstract

Intramolecular vibrational energy relaxation (IVR) in nitrous acid (HONO) is studied with the help of ultrafast two-color pump-probe spectroscopy. In a previous paper [V. Botan et al., J. Chem. Phys. 124, 234511 (2006)], it has been observed that trans-HONO cools through a cascade of overtones of one specific mode after pumping the OH stretch vibration. We had suggested that this cooling mode is the ONO bend vibration. Furthermore, molecules that have initially been excited by the OH stretch vibration of cis-HONO and then underwent isomerization follow the same relaxation pathway. In the present study, we extend the investigation of IVR of cis- and trans-HONO to the N=O stretch and HON bend spectral regions, finding further evidence that the bottleneck of trans cooling is indeed the ONO bend vibration. In combination with information on the anharmonic coupling constants of different modes, the energy relaxation dynamics preceding this cooling cascade can also be followed in unprecedented detail.

Intramolecular vibrational energy relaxation (IVR) in nitrous acid (HONO) is studied with the help of ultrafast two-color pump-probe spectroscopy. In a previous paper [V. Botan et al., J. Chem. Phys. 124, 234511 (2006)], it has been observed that trans-HONO cools through a cascade of overtones of one specific mode after pumping the OH stretch vibration. We had suggested that this cooling mode is the ONO bend vibration. Furthermore, molecules that have initially been excited by the OH stretch vibration of cis-HONO and then underwent isomerization follow the same relaxation pathway. In the present study, we extend the investigation of IVR of cis- and trans-HONO to the N=O stretch and HON bend spectral regions, finding further evidence that the bottleneck of trans cooling is indeed the ONO bend vibration. In combination with information on the anharmonic coupling constants of different modes, the energy relaxation dynamics preceding this cooling cascade can also be followed in unprecedented detail.

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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:28 October 2008
Deposited On:14 Jan 2009 14:27
Last Modified:03 Jun 2016 07:23
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(16) and may be found at http://link.aip.org/link/?JCPSA6/129/164506/1
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:10.1063/1.2996355
PubMed ID:19045283
Permanent URL: http://doi.org/10.5167/uzh-8695

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