Temperature dependent spectral densities and quantum activated rate theory

Dimitri Antoniou, Steven D Schwartz

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

The variability with temperature of spectral densities and rates calculated with quantum activated rate theory is investigated. Classical spectral densities at two temperatures are computed via molecular dynamics for a model of proton transfer in methyl chloride. In addition, quantum dynamics is computed for spectral densities which artificially boost variability at low frequency. We find significant variation in computed spectral densities at moderate frequency. These variations, however, have little effect on overall computed quantum dynamics. In contradistinction, artificial variation in spectral densities at the lowest frequencies can generate fairly significant effects on quantum dynamics. Detailed flux correlation function calculations are presented which illustrate this phenomenon.

Original languageEnglish (US)
Pages (from-to)5487-5492
Number of pages6
JournalThe Journal of Chemical Physics
Volume109
Issue number13
DOIs
StatePublished - 1998
Externally publishedYes

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Spectral density
Temperature
temperature
Methyl Chloride
low frequencies
methyl chloride
Proton transfer
acceleration (physics)
Molecular dynamics
Fluxes
molecular dynamics
protons

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

Cite this

Temperature dependent spectral densities and quantum activated rate theory. / Antoniou, Dimitri; Schwartz, Steven D.

In: The Journal of Chemical Physics, Vol. 109, No. 13, 1998, p. 5487-5492.

Research output: Contribution to journalArticle

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