Transient phenomena in time- and frequency-gated spontaneous emission

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

Research output: Contribution to journalArticlepeer-review

2 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 languageEnglish
Pages (from-to)3587-3597
Number of pages11
JournalJournal of Physical Chemistry A
Volume109
Issue number16
DOIs
Publication statusPublished - 28 Apr 2005

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