Power dependence of transient degenerate four-wave mixing in molecular systems

Abstract

The object of this study is to quantitatively elucidate the laser-power dependence in transient degenerate four-wave mixing (DFWM) with an emphasis on the high laser-pump intensity region. We discuss our investigation on the power dependence of transient DFWM by taking gas-phase iodine (${\mathrm{I}}_{2}$) molecules as a testing example. The distinct physical feature is that in the high-power laser pump, where both laser-pulse duration and the inverse of pump rate are much shorter than the molecular population relaxation time, the steady-state DFWM theory of Abrams and Lind [Optical Phase Conjugation, edited by R. A. Fisher (Academic, New York, 1983), Chap. 8, pp. 211--284; Opt. Lett. 2, 94 (1978); 3, 205 (1978)] is not appropriate. The prediction by the steady-state theory has shown the DFWM to decrease with increasing laser-pump intensity as a function of 1/${\mathrm{I}}_{\mathrm{laser}}$, which disagrees with the saturation behavior observed in the experiment. To elucidate the dependence of DFWM on the laser pump intensity, a non-steady-state extension of the nonperturbative theory of Abrams and Lind is required. The non-steady-state theoretical result will be shown to be in good agreement with the experimental power dependence at resonance transient DFWM especially in the high-power pump region.