Theoretical investigation of the forward phase-matched geometry for degenerate four-wave mixing spectroscopy

Abstract

We examine theoretically the degenerate four-wave mixing (DFWM) signal intensities and line shapes obtained with the forward phase-matched geometry in which all beams propagate in the same direction and compare the results to those of the phase-conjugate geometry with counterpropagating pump beams. To examine the forward phase-matched geometry, we modify a theoretical approach used previously to calculate phase-conjugate DFWM signal intensities. This theoretical approach, which involves numerical integration of the time-dependent density-matrix equations, is validated for the forward phase-matched geometry by comparison of our calculated line shapes to both a perturbative solution and to experimental data. This methodology is then used to compare the signal intensities and line shapes obtained with the forward phase-matched geometry and the phase-conjugate geometry in the perturbative (low laser power) and saturated (high laser power) regimes. In the perturbative regime the forward phase-matched signal exhibits less sensitivity to the Doppler linewidth. At pump laser intensities approximately equal to the saturation intensity the signal for the forward phase-matched geometry is stronger than that for the phase-conjugate geometry for primarily Doppler-broadened resonances, assuming the same probe volume for both geometries. These advantages warrant further investigations employing the forward phase-matched configuration for DFWM measurements of gas-phase species.