Unified description of sequential and coherent contributions to time-resolved spontaneous emission signals: generalized doorway-window approach

M.F. Gelin; D. Egorova; A.V. Pisliakov; W. Domcke

doi:10.1016/j.cplett.2004.05.018

Unified description of sequential and coherent contributions to time-resolved spontaneous emission signals: generalized doorway-window approach

M.F. Gelin (Lead / Corresponding author), D. Egorova (Lead / Corresponding author), A.V. Pisliakov, W. Domcke

Physics

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

18 Citations (Scopus)

Abstract

The doorway-window approach for the description of time- and frequency-gated spontaneous emission is extended to the case of overlapping pump and gate pulses, provided one can neglect the transient terms decaying with the characteristic time of the gate pulse. All the transient terms decaying with the characteristic time of the pump pulse, on the other hand, are taken into account. Both the sequential and the coherent contributions to the signal are considered. The comparison of the standard doorway-window approximation with the present more general formulation for a curve-crossing model system reveals that the former is valid for pump-pulse durations up to the order of the vibrational period and becomes qualitatively incorrect for longer pump pulses.

Original language	English
Pages (from-to)	234-242
Number of pages	9
Journal	Chemical Physics Letters
Volume	391
Issue number	4-6
DOIs	https://doi.org/10.1016/j.cplett.2004.05.018
Publication status	Published - 21 Jun 2004

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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10.1016/j.cplett.2004.05.018

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abstract = "The doorway-window approach for the description of time- and frequency-gated spontaneous emission is extended to the case of overlapping pump and gate pulses, provided one can neglect the transient terms decaying with the characteristic time of the gate pulse. All the transient terms decaying with the characteristic time of the pump pulse, on the other hand, are taken into account. Both the sequential and the coherent contributions to the signal are considered. The comparison of the standard doorway-window approximation with the present more general formulation for a curve-crossing model system reveals that the former is valid for pump-pulse durations up to the order of the vibrational period and becomes qualitatively incorrect for longer pump pulses.",

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Unified description of sequential and coherent contributions to time-resolved spontaneous emission signals: generalized doorway-window approach. / Gelin, M.F. (Lead / Corresponding author); Egorova, D. (Lead / Corresponding author); Pisliakov, A.V. et al.
In: Chemical Physics Letters, Vol. 391, No. 4-6, 21.06.2004, p. 234-242.

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

TY - JOUR

T1 - Unified description of sequential and coherent contributions to time-resolved spontaneous emission signals

T2 - generalized doorway-window approach

AU - Gelin, M.F.

AU - Egorova, D.

AU - Pisliakov, A.V.

AU - Domcke, W.

PY - 2004/6/21

Y1 - 2004/6/21

N2 - The doorway-window approach for the description of time- and frequency-gated spontaneous emission is extended to the case of overlapping pump and gate pulses, provided one can neglect the transient terms decaying with the characteristic time of the gate pulse. All the transient terms decaying with the characteristic time of the pump pulse, on the other hand, are taken into account. Both the sequential and the coherent contributions to the signal are considered. The comparison of the standard doorway-window approximation with the present more general formulation for a curve-crossing model system reveals that the former is valid for pump-pulse durations up to the order of the vibrational period and becomes qualitatively incorrect for longer pump pulses.

AB - The doorway-window approach for the description of time- and frequency-gated spontaneous emission is extended to the case of overlapping pump and gate pulses, provided one can neglect the transient terms decaying with the characteristic time of the gate pulse. All the transient terms decaying with the characteristic time of the pump pulse, on the other hand, are taken into account. Both the sequential and the coherent contributions to the signal are considered. The comparison of the standard doorway-window approximation with the present more general formulation for a curve-crossing model system reveals that the former is valid for pump-pulse durations up to the order of the vibrational period and becomes qualitatively incorrect for longer pump pulses.

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JO - Chemical Physics Letters

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Unified description of sequential and coherent contributions to time-resolved spontaneous emission signals: generalized doorway-window approach

Abstract

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