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Title: Domain of validity of the perturbative approach to femtosecond optical spectroscopy

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.
Authors:
; ; ;  [1]
  1. Department of Chemistry, Technische Universit√§t M√ľnchen, D-85747 Garching (Germany)
Publication Date:
OSTI Identifier:
22253843
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 139; Journal Issue: 22; Other Information: (c) 2013 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ABSORPTION; MOLECULAR MODELS; RESPONSE FUNCTIONS; SIMULATION; SPECTROSCOPY