Domain of validity of the perturbative approach to femtosecond optical spectroscopy

Maxim F. Gelin, B. Jayachander Rao, Mathias Nest, Wolfgang Domcke

Research output: Contribution to journalArticlepeer-review

14 Scopus citations

Abstract

We have performed numerical nonperturbative simulations of transient absorption pump-probe responses for a series of molecular model systems. The resulting signals as a function of the laser field strength and the pump-probe delay time are compared with those obtained in the perturbative response function formalism. The simulations and their theoretical analysis indicate that the perturbative description remains valid up to moderately strong laser pulses, corresponding to a rather substantial depopulation (population) of the initial (final) electronic states.

Original languageEnglish
Article number224107
JournalJournal of Chemical Physics
Volume139
Issue number22
DOIs
StatePublished - 14 Dec 2013

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