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physica status solidi (b)

Time‐Resolved Four‐Wave Mixing Experiments in CuCl

Maria J. M. Gomes, Bernard J. Kippelen, R. Lévy, J. B. Grün, B. Hönerlage

Published May 1, 1990• 4 citations
Publisher

Abstract

Abstract By a light‐induced grating technique with three degenerate laser beams, the diffusion constants and the decay times of optical nonlinearities in CuCl are determined. By comparison with results from induced absorption, the nonlinearities may be identified as being due to different excitonic populations as well as to thermal effects.

DOI
10.1002/pssb.2221590111

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Abstract By a light‐induced grating technique with three degenerate laser beams, the diffusion constants and the decay times of optical nonlinearities in CuCl are determined. By comparison with results from induced absorption, the nonlinearities may be identified as being due to different excitonic populations as well as to thermal effects.
Abstract Using a picosecond light source and a streak camera as detection system, the temporal evolution of the signal generated throughout degenerate four‐wave mixing (DFWM) experiments is analysed in CuCl at low temperature. The signal emission shows different temporal behaviour depending on whether the test pulse reaches the surface of the sample before, during, or after the pump pulse. This enables one to distinguish the light‐induced grating contribution from the induced decay of quasi‐particles. The latter process can then be used to determine their dephasing time.
Abstract Using nanosecond laser pulses the time behaviour is investigated of degenerate four‐wave mixing close to the biexcitonic resonance in CuCl. The signal emission presents different time evolutions depending on excitation conditions. Its generation rate shows intensity changes and retardation effects. These effects are explained by an attenuation of the pump pulse through a time‐dependent nonlinear absorption and, at the resonance, by a loss of coherence related to collisions with bi‐excitons.
Abstract The optical nonlinearity associated with the giant two‐photon absorption, GTA, of excitonic molecules in CuCl is discussed. The metamorphoses of the four‐wave mixing spectra due to the generation of the exciton grating are demonstrated by the observation of their polarization characteristics. The propagation characteristics of the excitation around the GTA resonance are observed by micro‐Raman spectroscopy. The two‐photon Raman scattering light is used as a probe to monitor the spatial character of the excitation. The propagation characteristics show a drastic change in the very narrow spectral range around the GTA resonance energy.
Abstract We present a study of optical phase conjugation through degenerate four-wave mixing in CuCl, as a function of light frequency, intensity, polarization and sample temperature. The phase-conjugate signal exhibits two maxima at the frequencies of the T5 exciton (one-photon resonance) and of the biexciton (two-photon resonance). By appropriate combinations of the input beam polarizations, it is possible to single out the various terms contributing to the signal (small-spaced, large-spaced population grating and two-photon coherent excitation). The absolute value of X(3) responsible for the two-photon resonance has been determined ( x(3) (-w,w,w, -w) = 3.10-7 e.s.u.). It leads to ‘mirror’ efficiencies of the order of 10% for input pump intensities I0 » 105 W cm -2 and sample thickness d» 10-4 cm. At higher I0, a saturation of the reflection takes place. The variation of the conjugate beam with temperature has been studied in the range 15 K < T <70 K. Finally, the phase-conjugate nature of the signal has been verified by inserting an aberrator in the path of the input probe beam, and by checking the reconstruction of the reflected beam.