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A comprehensive theory of a new type of three-wave optical mixing (₃=2₁-₂) is given for the spectroscopic purpose of determining ultra-short relaxation times (picoseconds or less) associated with excited states of condensed matter. Two incident light frequencies ₁ and ₂ are chosen so that they are both resonant with an inhomogeneously broadened optical transition and |₂-₁| is in the vicinity of inverse relaxation times. The theory is developed for its major application to broad-band electronic transitions. The nonlinear susceptibility ₑ^ (3) for this process (named resonant Rayleigh-type mixing) is calculated by a density-matrix formalism with the model of a two-level atomic system incorporating the distribution of resonance frequencies and longitudinal (T₁) and transverse (T₂) relaxation times. The result shows a frequency characteristic depending only on T₁, T₂, and ₂-₁ in a broad-band limit, which serves for the determination of T₁ and T₂ in the frequency domain. The analysis is further extended to include the various effects as follows. The calculation of the saturation effect in the lowest order reveals that it modifies the shape of the frequency characteristic of the nonlinear susceptibility but does not affect seriously the determination of relaxation times. The effect of spectral cross relaxation within the inhomogeneous broadening is incorporated by a generalized density-matrix formalism. The resultant ₑ^ (3) consists of two terms. The dominant term is the same as before except that T₁ is replaced by a combined relaxation time T₁^'= ({T₁^-1+T₃^-1) }^-1, where T₃ is the cross-relaxation time. The other term originates from the inverse spectral-diffusion process. The effect of other energy levels located between the two levels under study is analyzed with a simple three-level model. The resultant ₑ^ (3) also consists of two terms, the dominant one being the same as that for the two-level model except that T₁^-1 should be interpreted as total population decay rate of the upper level. For accurate derivation of ₑ^ (3) from experiment, we discuss the interference between the resonant and nonresonant susceptibility terms and the light-wave propagation effect. Finally, the close analogy between this type of optical mixing and the photon echo is discussed.
Yajima et al. (Sun,) studied this question.