Ultrafast population relaxation by time-resolved degenerate four-wave mixing with incoherent light and analysis under breakdown of the two-level approximation

Abstract

Time-resolved three-beam degenerate four-wave mixing with incoherent light for observation of population relaxation, originally proposed by Morita et al.. [ J. Opt. Soc. Am. B 4, 1269 ( 1987)] is examined both theoretically and experimentally. Theoretical calculation shows that a large part of the decaying signal in the time-resolved profile originates from the ground-state relaxation if the excited-state relaxation is faster than the ground-state relaxation. It is also shown that the use of a nonzero delay time between the k₂ and k₁ beams, in addition to that between the k₃ and k₁ beams (k_s = k₁ − k₂ + k₃, where k_1–3 and k_s are the wave vectors for the incident and the scattered beams, respectively), provides information on population relaxation, especially when the population-relaxation time is far longer than the correlation time of the incoherent light. These theoretical considerations are verified experimentally with the use of a triphenylmethane dye in solution.

© 1993 Optical Society of America

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