The workings of a molecular thermometer: the vibrational excitation of carbon tetrachloride by a solvent

The Journal of Chemical Physics
Polly B GrahamRichard M Stratt

Abstract

An intriguing energy-transfer experiment was recently carried out in methanol/carbon tetrachloride solutions. It turned out to be possible to watch vibrational energy accumulating in three of carbon tetrachloride's modes following initial excitation of O-H and C-H stretches in methanol, in effect making those CCl(4) modes "molecular thermometers" reporting on methanol's relaxation. In this paper, we use the example of a CCl(4) molecule dissolved in liquid argon to examine, on a microscopic level, just how this kind of thermal activation occurs in liquid solutions. The fact that even the lowest CCl(4) mode has a relatively high frequency compared to the intermolecular vibrational band of the solvent means that the only solute-solvent dynamics relevant to the vibrational energy transfer will be extraordinarily local, so much so that it is only the force between the instantaneously most prominent Cl and solvent atoms that will significantly contribute to the vibrational friction. We use this observation, within the context of a classical instantaneous-pair Landau-Teller calculation, to show that energy flows into CCl(4) primarily via one component of the nominally degenerate, lowest frequency, E mode and does so fast enough to mak...Continue Reading

Citations

Jul 11, 2006·The Journal of Chemical Physics·Sai G Ramesh, Edwin L Sibert
Jan 4, 2007·The Journal of Chemical Physics·Shuzhou LiJ L Skinner
Jul 19, 2012·The Journal of Chemical Physics·Baofeng Zhang, Richard M Stratt
Jun 1, 2016·Physical Chemistry Chemical Physics : PCCP·Jadwiga KonarskaTomasz M Kardaś
Mar 31, 2007·Physical Chemistry Chemical Physics : PCCP·Alexander KandratsenkaVyacheslav S Vikhrenko
Oct 2, 2008·The Journal of Physical Chemistry. B·Benjamin H Savitzky, Richard M Stratt
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Oct 16, 2008·The Journal of Physical Chemistry. a·Edwin L SibertTolga S Gulmen
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Mar 29, 2007·The Journal of Physical Chemistry. B·George A Marcus, H Alan Schwettman
Sep 25, 2004·Science·John C DeàkDana D Dlott

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