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

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4836636· OSTI ID:22253843
; ; ;  [1]
  1. Department of Chemistry, Technische Universität München, D-85747 Garching (Germany)

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.

OSTI ID:
22253843
Journal Information:
Journal of Chemical Physics, Vol. 139, Issue 22; Other Information: (c) 2013 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
Country of Publication:
United States
Language:
English