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Physical Review A

Optical phase conjugation based on the giant two-photon resonance of the excitonic molecule in CuCl

Lloyd L. Chase, M. L. Claude, Daniele Hulin, A. Mysyrowicz

Published Dec 1, 1983• 25 citations
Publisher

Abstract

Optical phase conjugation resulting from the two-photon coherence due to the excitonic molecule resonance in CuCl has been observed and studied as a function of frequency, polarization, and pump intensity. Reconstruction of the polarization of an aberrated probe beam is demonstrated.
DOI
10.1103/physreva.28.3696

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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.
The phase-conjugation in crystalline CuCl has been studied at 1.6 K. It has been found that the two-photon resonance of the Γ1\varGamma_{1}Γ1​-excitonic molecule and the one-photon resonance of the Γ5\varGamma_{5}Γ5​-exciton contribute to the generation of the phase-conjugated wave. Each contribution has been separated spectroscopically by adjusting the polarization configuration of the incident fields adequately and has been compared qualitatively with the theory. The efficiency of the phase-conjugated reflection has become maximum at around the two-photon resonance of the excitonic molecule, 3.186 eV and has been ∼1% at the maximum.
Large, nonlinear-optical phenomena are shown theoretically to be observable under nearly two-photon resonant pumping of the excitonic molecule (EM), e.g., in a CuCl crystal. When the exciton polariton (EP) is resonantly pumped into the EM, they are hybridized with each other and show optical Stark splitting. These splittings can be observed, respectively, as a sharp dip in the reflection spectrum and two-photon absorption spectrum due to the EM. We can also clarify how these splittings change into the blueshifts and redshifts of the EP and the EM as functions of the pump frequency and power. The generation of the phase-conjugated wave is shown also to be enhanced under two-photon resonant pumping of the EM. Some characteristics about pump-probe frequency and polarization dependences are also clarified. We have also derived the effective Hamiltonian of the exciton and the EM from the first-principles equation of motion for the exciton coupled with that of the EM. This Hamiltonian has made possible the theoretical analysis of these nonlinear-optical phenomena.
The Γ1\varGamma_{1}Γ1​-symmetry of the lowest excitonic molecule state of CuCl has been confirmed experimentally from the measurements of the giant two-photon absorption and resonance Raman scattering by using circularly polarized dye laser light. The giant two-photon transition is found to be forbidden for single beam of circularly polarized light while it is allowed for two beams of circularly polarized lights impinging in crystals from directly opposite directions. It has been verified that the lowest excitonic molecule state is composed of two-electron- and two-hole-states both of the composite spin angular momentum zero.
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.