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Physical Review Letters

Nonlinear Spectroscopy of Biexcitons in CuCl by Resonant Coherent Scattering

Alain D. Maruani, J. L. Oudar, Edmond Batifol, D. S. Chemla

Published Nov 13, 1978• 73 citations
Publisher

Abstract

A new method of nonlinear spectroscopy aiming to probe solids in the highly dispersive and absorbing region is presented. It requires only one laser and uses wave-vector rather than frequency discrimination of the nonlinear signal from the input beams. Application is made to the study of the ${\ensuremath{\Gamma}}_{1}$ biexciton level in CuCl.

DOI
10.1103/physrevlett.41.1372

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A new method of nonlinear spectroscopy aiming to probe solids in the highly dispersive and absorbing region is presented. It requires only one laser and uses wave-vector rather than frequency discrimination of the nonlinear signal from the input beams. Application is made to the study of the \ensuremathΓ1{\ensuremath{\Gamma}}_{1}\ensuremathΓ1​ biexciton level in CuCl.
We present a thorough investigation of the different relaxation channels opened in a strongly interacting system of excitonic quasiparticles in CuCl for density regimes ranging up to 50 MW/cm2{\mathrm{cm}}^{2}cm2. A spectrally narrow pump beam consisting of 30-ps pulses is tuned around one-half the biexciton energy. It creates an initial distribution of biexcitons through resonant two-photon absorption. A spectrally broad probe beam made of pulses that also have 30-ps duration monitors the excitation-induced variation of the transmission spectrum of CuCl samples near the Z3{\mathit{Z}}_{3}Z3​ exciton resonance. Coherent processes corresponding to parametric emissions of various orders are observed. Absorption and gain bands that reflect the evolution of biexciton and exciton populations on their respective dispersion curves are followed as functions of the time delay between pump and probe pulses.
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.
A coherently driven exciton–biexciton transition in CuCl enables one to propagate a probe light beam within the exciton-polariton stop-band where radiation is otherwise completely reflected. The stop-band transparency window can be controlled via the pump beam frequency and intensity. The phenomenon is reminiscent of quantum coherence effects occurring in three-level atomic systems, except that it here involves delocalized electronic excitations in a crystal via a frequency and wave-vector selective polaritonic mechanism. Both a free standing slab and a microcavity configuration are theoretically studied. (© 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)