Resonant Rayleigh-Type Mixing Spectroscopy Using a Picosecond Dye Laser System
Resonant Rayleigh-type optical mixing [1–5] has recently been used as a useful method to determine the ultrashort relaxation times of far below 1 psec associated, for example, with electronic transitions of dye solutions. In this frequency-domain method both the longitudinal and transverse relaxation times can be determined from the dispersive characteristics of the third-order nonlinear susceptibility, χ(3)(ω3 = 2ω1-ω2), as a function of |ω1-ω2 } under the conditions of Rayleigh-type resonance (|ω1-ω2} ≃ γ) and near one-photon resonance ω1, ω2 ≃ ω0. Here, ω1 and ω2 are the frequencies of two incident light waves, γ is the relaxation rate of various kind, and ω0 is the frequency of a material transition which is usually inhomogeneously broadened.
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