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Japanese Journal of Applied Physics

Numerical Analysis of Femtosecond Time-Resolved Degenerate Four-Wave Mixing Signal including Group-Velocity Dispersion Effect

Yoshihisa Yamaoka, Ryuji Morita, Mikio Yamashita

Published Mar 1, 2000• 2 citations
Publisher

Abstract

We numerically analyze the group-velocity dispersion (GVD) effect of the nonlinear medium on the femtosecond time-resolved degenerate four-wave mixing (DFWM) signal with the third-order nonlinear delayed response. As a result, we find that material GVD greatly influences not only the magnitude but also the temporal profile of the DFWM signal.

DOI
10.1143/jjap.39.1170

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We numerically analyze the group-velocity dispersion (GVD) effect of the nonlinear medium on the femtosecond time-resolved degenerate four-wave mixing (DFWM) signal with the third-order nonlinear delayed response. As a result, we find that material GVD greatly influences not only the magnitude but also the temporal profile of the DFWM signal.
A set of coupled equations is derived and used to analyze transient coherent degenerate four-wave mixing (DFWM) in a two-level system. The numerical results show that in the case of near-resonance, intense pumping, and short pulses, the properties of degenerate four-wave mixing have interesting coherent interaction characteristics, such as quasi-periodicity in the pump pulse area, probe pulse areas, and energy reflectivity, oscillatory behavior of the DFWM pulse, and generation of a DFWM signal in the case of delayed incidence, where the three incident pulses do not overlap in the medium.>
Degenerate four-wave mixing (DFWM) is a simple method to achieve phase conjugation. It uses the third-order nonlinearity of the electric susceptibility to produce changes in the optical properties of materials. A dynamic grating is then induced. Such gratings might be used as fast optical memories in optical computing. Our aim is to find media with large nonlinear susceptibilities and fast response time. We report phase conjugation of 532-nm laser radiation by DFWM in dye solutions. The time dependence of the conjugated wave is investigated experimentally and compared to theoretical predictions. We have also studied the influence of the solvents, dye concentration, and pump intensity on the phase conjugated signal. The results are compared with those predicted by three nonlinear mechanisms. Thermally induced refractive-index changes, Kerr effect, and saturable absorption are considered.
The use of picosecond lasers for degenerate four-wave mixing (DFWM) diagnostics of atmospheric pressure flames has been suggested as a means of overcoming the complicated collision-rate dependence of the DFWM signal in the nanosecond-laser pulse-length regime. In this paper DFWM spectroscopy in the regime in which the laser pulse length (τL) is less than the characteristic collisional time (τC) is investigated theoretically. DFWM signal levels for the phase-conjugate geometry (counterpropagating pump beams) are calculated by integration of the time-dependent density-matrix equations at numerous grid points along the phase-matching axis and by summing of the polarization contribution from each of these grid points. Both purely homogeneously broadened resonances and resonances that are both collision broadened and Doppler broadened are considered. DFWM signal generation for these two types of resonances in the fully transient regime (τL≪τC) is strikingly different. For a homogeneously broadened resonance, the DFWM signal persists long after the laser beam has passed through the medium. The decay rate of the DFWM signal is determined by the collision rate in the medium, and the integrated DFWM signal is still dependent on the collision rate even in this fully transient regime. However, when the Doppler broadening of the resonance is much greater than the collisional broadening, the DFWM signal decays with a fall time close to that of the laser pulse. For τL≪τC, we find that it is the laser spectral width, rather than the collisional width, that dictates the range of velocity groups with which the pulses effectively interact. The signal decays with a fall time close to that of the laser pulse because the excited velocity groups radiate out of phase with one another. In a medium in which the Doppler width is much greater than the collisional width, the DFWM reflectivity is independent of collision rate for τL≪τC, but the signal level is dependent on the Doppler width. Finally, we investigate the effect of different laser pulse lengths on reflectivity saturation curves for resonances with different levels of Doppler broadening.
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.