The physics underlying the technique of degenerate four-wave mixing (DFWM) is presented. Its application to the measurement of energy decay and dephasing rates is considered in the regime of small absorption and coupling coefficients.
Degenerate four-wave mixing (DFWM) spectroscopy is a promising diagnostic technique [1-3], but significant questions remain regarding its application for quantitative concentration measurements in combustion environments with typical laser systems. In this paper we present a summary of two numerical investigations with the goal of quantifying the measurement technique for common experimental situations. Specifically, we investigate both (1) probing a degenerate-level (multistate) resonance with a single-mode laser and (2) probing a two-state resonance with a multimode laser. DFWM signal levels are calculated by solving the time-dependent density matrix equations using direct numerical integration (DNI) [4, 5] for a two or more level system interacting with three laser beams.
The nonlinear response of resonant saturable materials giving rise to degenerate four-wave mixing (DFWM) has been shown both experimentally and theoretically to provide the potential for very large efficiencies for phase conjugation and Doppler-free spectra for high resolution spectroscopy. The geometry for this interaction consists of two counter- propagating pumps (Ef and Ep) and a probe (Ep) intersecting the pumps at some angle θfp. The simultaneous action of one pump and the probe produces spatial hole burning resulting in a spatial modulation of the saturating absorption and dispersion which scatters the remaining pump to produce the signal.
Degenerate four-wave mixing (DFWM) spectroscopy is a potentially powerful technique for quantitative measurement of minor species in gas-phase media [1-3]. In this paper we compare the DFWM signal levels and lineshapes obtained using two different phase-matching geometries: the phase-conjugate geometry and the forward phase-matched geometry. DFWM signal levels are calculated by solving the time-dependent density matrix equations using direct numerical integration (DNI) [4, 5] for a two-level system interacting with three laser beams. This numerical analysis includes the effects of molecular motion, intermolecular collisions, and high laser intensities, all of which have been shown to affect the DFWM signal level.
The steady-state theory of degenerate four-wave mixing (DFWM) with broad-bandwidth lasers is extended to treat the time dependence of the interaction allowing calculation of the intensity dependence and saturation behavior of DFWM with pulsed lasers. An experimental study of this intensity dependence as a function of laser bandwidth is reported, showing qualitative agreement with the theory. The line shape of DFWM induced by broad-bandwidth pump fields, probed by a monochromatic probe, is shown to have a Doppler-broadened profile in agreement with the theoretical predictions.