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IEEE Journal of Quantum Electronics

Coherent phenomena involved in the time-resolved optical Kerr effect

J. L. Oudar

Published Apr 1, 1983• 47 citations
Publisher

Abstract

The effect of parametric coupling between pump and probe beams in time-resolved optical Kerr effect is theoretically discussed for various experimental configurations. It is shown that with a cicularly polarized pump beam, the polarization changes induced on a nearly collinear probe beam are due to this coherence effect only. In other configurations, this parametric coupling can appear as an additional contribution to the observed signal, especially when pump and probe are derived from the same laser beam. It is pointed out that this coupling can occur not only when the pump and probe beams are at the same wavelength, but also when the difference or the sum of their frequencies can excite a Raman or a two-photon resonance in the medium.

DOI
10.1109/jqe.1983.1071918

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The effect of parametric coupling between pump and probe beams in time-resolved optical Kerr effect is theoretically discussed for various experimental configurations. It is shown that with a cicularly polarized pump beam, the polarization changes induced on a nearly collinear probe beam are due to this coherence effect only. In other configurations, this parametric coupling can appear as an additional contribution to the observed signal, especially when pump and probe are derived from the same laser beam. It is pointed out that this coupling can occur not only when the pump and probe beams are at the same wavelength, but also when the difference or the sum of their frequencies can excite a Raman or a two-photon resonance in the medium.
The noise tenaciously appearing in the optically heterodyne detected (OHD) transient optical Kerr effect (OKE) o f simple molecular liquids is investigated. We show that, for liquid samples of interest to us, coherent coupling does exist and appears as noise when not properly resolved. The strength of coherent coupling relative to the OKE depends critically on the sample position, with respect to the beam waist of the probe laser, as well as the angle subtended by the pump and probe beams. When the optics alignment is optimized for the OKE against coherent coupling the OHD-OKE signal is found to increase linearly with the local oscillator strength; the coherent coupling signal also appears to increase though the trend is not clear-cut. PACS. 42.50.Md- Optical transient phenomena: quantum beats, photon echo, freeinduction decay, dephasings and revivals, optical nutation, and self-induced transparency. PACS. 78.47.+p- Time-resolved optical spectroscopies and other ultrafast optical measurements in condensed matter. I.
We demonstrate the existence of coherent coupling effects in pump-probe measurements with collinear, copropagating beams, despite the absence of any induced spatial gratings in this geometry. The coherent interaction, which is found to be similar but not identical to that for crossed beams, must be taken into account in analyzing relaxation processes occurring on the time scale of the laser pulse. These coherent effects cannot generally be eliminated by detecting the total change in energy in both the pump and probe beams.
Femtosecond two-beam coupling is demonstrated in N,N′-dimethylformamide and dimethyl sulfoxide by using a time-resolved pump-probe system at a wavelength of 800 nm. As the temporal delay between pulses is varied within the coherence time, transient energy transfer from one pulse to another occurs. Because of the asymmetry of the normalized transmittance, two-photon absorption is considered in the two liquids. A theory based on two-beam coupling in perpendicular linear polarization is used to interpret the experimental results. Good agreement is obtained between the theory and experiment. Moreover, by introducing a valuable variable, the ratio of the relaxation times of the two Kerr liquids is directly characterized.
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This paper presents an exact solution to the slowly varying envelope equations for the probe and signal fluxes in degenerate four-wave mixing in Kerr media. The analysis is performed for a noncollinear geometry, and all beams have the same linear polarization in the nonlinear medium. It is assumed that the angle separating the directions of the counterpropagating pumps and probe and signal beams is large enough so that cross-coupled waves do not contribute to the envelope equations describing the spatial evolution of the pump, probe, and signal beams. Multiple values of the transmitted probe are obtained for equal pump fluxes above a threshold determined by the nonlinear phase shift in the medium. Significant pump depletion occurs in this regime, but it can also occur without the appearance of multiple solutions. Since exact optical phase conjugation occurs only in the limit where the pumps are undepleted in Kerr media, this result implies that there are fundamental upper limits on the pump intensity that can be used to increase signal reflectivities in optical phase conjugation.