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Physical Review A

Interference between four-wave and six-wave mixing in resonant coherent scattering from biexcitons in CuCl

D. S. Chemla, Alain D. Maruani, F. Bonnouvrier

Published Nov 1, 1982• 17 citations
Publisher

Abstract

We present the first evidence of interference between four- and six-wave mixing in multiple coherent scattering near the two-photon resonance of biexcitons in CuCl. The experimental data are quantitatively explained by taking proper account of propagation effects and by a model for ${\ensuremath{\chi}}^{(5)}$ involving no adjustable parameters.

DOI
10.1103/physreva.26.3026

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Physical Review Letters•Nov 13, 1978•73 citations
We present the first evidence of interference between four- and six-wave mixing in multiple coherent scattering near the two-photon resonance of biexcitons in CuCl. The experimental data are quantitatively explained by taking proper account of propagation effects and by a model for \ensuremathχ(5){\ensuremath{\chi}}^{(5)}\ensuremathχ(5) involving no adjustable parameters.
We propose an experimental scheme to evaluate the intrinsic anharmonicity of the biexciton ensemble by extending the conventional four-wave mixing technique to coherent biexciton waves, which can be prepared by two-photon absorption of ultrashort optical pulses. The anharmonicity originates from the two-body interaction of the bosonic quasi-particles at low densities and leads to Kerr-type nonlinearity for the coherent biexcitonic waves generated in the crystal. We discuss the feasibility of determining the two-body biexciton interaction energy in CuCl by measuring the anharmonicity of the biexcitonic ensemble.
Coherently controlled four-wave-mixing (FWM) measurements have turned out to be a very sensitive tool to investigate the microscopic origin of the nonlinear optical response of semiconductor quantum-well structures, in particular if excitons are excited [1-3]. The measured signal oscillates as a function of the phase difference of the two interferometric pulses and is modulated additionally by contributions that oscillate with integer multiples of the excitonic resonance frequency. The influence of these harmonics can be measured in background free directions, i.e., the first (FWM) or second (six-wave mixing, SWM) diffracted order in direction 2k2-k1 or 3k2-2k1, respectively. Their intensity is easily quantified by inspecting the corresponding Fourier transforms (FT). Here, we report on transient interferometric SWM measurements and the influence of biexcitons on the signal.
Experimental evidence for the occurrence of optical bistability using the biexciton two-photon resonance in CuCl is presented. These observations agree with recent theoretical predictions that require an intensity of 10 MW/cm2{\mathrm{cm}}^{2}cm2 and 10-\ensuremath{\mu}m-thick etalons with 90% reflective coatings. Earlier much less demanding predictions neglected two important physical effects: unsaturable background absorption at the biexciton from the tail of the exciton resonance and broadening of the biexciton resonance with intensity.