Quantum simulations of vibrational dephasing of molecules in a cryogenic environment

HArF in an argon cluster

Pavel Jungwirth, R. Benny Gerber, Mark A. Ratner

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

The Classical Separable Potential (CSP) method, which is a meanfield approximation to multidimensional quantum dynamics, is applied to the dephasing process of a vibrationally excited HArF molecule in an argon cluster at low temperatures. Dephasing timescales of the order of 1 ps are estimated for dynamics following fundamental excitation of either the H-Ar or the Ar-F stretching mode of HArF. The CSP approach is valid over such timescales, and it is thus a viable approach to quantum simulations of dephasing at low temperatures. Vibrational relaxation is much slower: Quasi-classical molecular dynamics simulations yield a relaxation time around 100 ps for the initial v = 1 Ar-F stretching excitation. Such timescales are beyond the validity range of CSP; therefore, this or similar separable methods are inapplicable for vibrational energy decay.

Original languageEnglish
Pages (from-to)157-162
Number of pages6
JournalIsrael Journal of Chemistry
Volume42
Issue number2-3
Publication statusPublished - 2002

Fingerprint

Argon
Cryogenics
Stretching
Molecules
Relaxation time
Molecular dynamics
Temperature
Computer simulation

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

Quantum simulations of vibrational dephasing of molecules in a cryogenic environment : HArF in an argon cluster. / Jungwirth, Pavel; Gerber, R. Benny; Ratner, Mark A.

In: Israel Journal of Chemistry, Vol. 42, No. 2-3, 2002, p. 157-162.

Research output: Contribution to journalArticle

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