Theory of femtosecond pump-probe spectroscopy of ultrafast internal conversion processes in polyatomic molecules

G. Stock, W. Domcke

Research output: Contribution to journalArticlepeer-review

42 Scopus citations

Abstract

A theoretical description of stimulated-emission pumping with femtosecond laser pulses on complex absorption bands of polyatomic molecules is developed. The strong non-Born-Oppenheimer coupling associated with conical intersections of multidimensional excited-state potential-energy surfaces is included in a fully microscopic manner for appropriate model systems. Additional relaxation effects in the excited-state manifold (lifetime broadening and pure dephasing) are included in the usual phenomenological manner by using the densitymatrix formalism. The calculation of the stimulated-emission pump-probe signalby means of density-matrix perturbation theory is briefly discussed and numerically realized using a time-dependent eigenstate-free treatment of the intramolecular dynamics. Someresults obtained for a simple model of the SI-S2 conical intersection in pyrazine are presented.

Original languageEnglish
Pages (from-to)1970-1980
Number of pages11
JournalJournal of the Optical Society of America B: Optical Physics
Volume7
Issue number9
DOIs
StatePublished - Sep 1990

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