A unified theory of time-domain and frequency-domain four-wave mixing processes, which is based on the nonlinear response function R(t3, t2, t1), is developed. The response function is expressed in terms of the four-point correlation function of the dipole operator F(τ1, τ2, τ3, τ4) and is evaluated explicitly for a stochastic model of line broadening that holds for any correlation time of the bath. Our results interpolate between the fast-modulation limit, in which the optical Bloch equations are valid, and the static limit of inhomogeneous line broadening. As an example of the relationship between time-domain and frequency-domain four-wave mixing, we compare the capabilities of steady-state and transient coherent anti-Stokes Raman spectroscopy experiments to probe the vibrational dynamics in ground and excited electronic states.
© 1986 Optical Society of America
Original Manuscript: September 20, 1985
Manuscript Accepted: November 19, 1985
Published: April 1, 1986
Shaul Mukamel and Roger F. Loring, "Nonlinear response function for time-domain and frequency-domain four-wave mixing," J. Opt. Soc. Am. B 3, 595-606 (1986)