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Chemical Physics Letters

Quantum stochastic theory of exchange dephasing model for a vibrating molecule in dense medium

Eiko Hiroike

Published Mar 1, 1981• 11 citations
Publisher
DOI
10.1016/0009-2614(81)80025-5

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The dephasing of a high-frequency intramolecular vibrational mode in a molecular crystal is successively investigated by the cumulant perturbation expansion method as in the preceding papers in this series, I and II. The dephasing of the high-frequency mode is brought on by the thermal excitation of a low-frequency mode in the same molecule as in I and II. In this paper, however, the intramolecular vibrational modes are expressed by the bands of the exciton waves traveling through the crystal (in I and II, the intramolecular vibrational modes are expressed by the localized excitation in one molecule). The calculation shows that the spectrum becomes considerably broad as the temperature increases, while the narrowing is observed as the band widths of the exciton waves increases.

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Quantum Dephasing in Mesoscopic Systems

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Elsevier eBooks•Jan 1, 1999•0 citations
The indirect dephasing model for a vibrating molecule in a dense medium is investigated by using the cumulant perturbation expansion method. The perturbation is taken as a sum of the anharmonic coupling between the high- and low-frequency modes and the interaction between the low-frequency mode and molecular surrounding. All the states of the low-frequency mode is taken into account in the calculation. Our model is available, only when the dephasing time of the high-frequency mode is shorter than the life-time of the low-frequency mode. This condition is satisfied in usual organic molecular crystals.
The dephasing of a high-frequency intramolecular vibrational mode in a molecular crystal is successively investigated by the cumulant perturbation expansion method as in the preceding papers in this series, I and II. The dephasing of the high-frequency mode is brought on by the thermal excitation of a low-frequency mode in the same molecule as in I and II. In this paper, however, the intramolecular vibrational modes are expressed by the bands of the exciton waves traveling through the crystal (in I and II, the intramolecular vibrational modes are expressed by the localized excitation in one molecule). The calculation shows that the spectrum becomes considerably broad as the temperature increases, while the narrowing is observed as the band widths of the exciton waves increases.