Transient phenomena in time- and frequency-gated spontaneous emission

Maxim F. Gelin; Dassia Egorova; Andrei V. Pisliakov; Wolfgang Domcke

doi:10.1021/jp044463t

Transient phenomena in time- and frequency-gated spontaneous emission

Maxim F. Gelin (Lead / Corresponding author), Dassia Egorova, Andrei V. Pisliakov, Wolfgang Domcke

Physics

Research output: Contribution to journal › Article › peer-review

6 Citations (Scopus)

Abstract

The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.

Original language	English
Pages (from-to)	3587-3597
Number of pages	11
Journal	Journal of Physical Chemistry A
Volume	109
Issue number	16
DOIs	https://doi.org/10.1021/jp044463t
Publication status	Published - 28 Apr 2005

ASJC Scopus subject areas

Physical and Theoretical Chemistry

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10.1021/jp044463t

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title = "Transient phenomena in time- and frequency-gated spontaneous emission",

abstract = "The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.",

author = "Gelin, {Maxim F.} and Dassia Egorova and Pisliakov, {Andrei V.} and Wolfgang Domcke",

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T1 - Transient phenomena in time- and frequency-gated spontaneous emission

AU - Gelin, Maxim F.

AU - Egorova, Dassia

AU - Pisliakov, Andrei V.

AU - Domcke, Wolfgang

PY - 2005/4/28

Y1 - 2005/4/28

N2 - The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.

AB - The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.

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JO - Journal of Physical Chemistry A

JF - Journal of Physical Chemistry A

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Transient phenomena in time- and frequency-gated spontaneous emission

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