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Journal of the Optical Society of America B

Optical phase conjugation near resonance with biexciton two-photon absorption in CuCl (A)

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

Published Jan 1, 1984• 0 citations
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Abstract

Measurements have been made of phas conjugation from degenerate four-wav mixing (DFWM) based on the large nonlinear susceptibility resulting from the two-photo absorption (TPA) resonance of the excitoni molecule state in CuCl. The excitonic molecule in CuCl is a bound state of two exciton that is responsible for a very strong two-photon absorption resonance at a photo energy of 3.186 eV at T ~ 4.2 K.1

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Phase-Conjugation by Four-Wave Mixing in CuCl: Resonance Enhancement by Exciton and Excitonic Molecule and Its Polarization Dependence

Goro Mizutani, N. Nagasawa

The phase-conjugation in crystalline CuCl has been studied at 1.6 K. It has been found that the two-photon resonance of the \(\varGamma_{1}\)-excitonic molecule and the one-photon resonance of the \(\varGamma_{5}\)-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.

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Optical phase conjugation via degenerate four-wave mixing in copper chloride

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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.

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Direct Two-Photon Creation of Excitonic Molecule in CuCl

W. Ungier, P. Janiszewski, Maciej Suffczynski

The probability of direct excitation of excitonic molecule in the two-photon absorption process is calculated with an Hylleraas-Ore type biexciton envelope, which is variationally optimized.In the second order of perturbation, because of the resonance effect, only the exciton .r5intermediate state is taken into account.The band structure at band extrema due to spin-orbit interaction is assumed.The transition probability of two-photon absorption is expressed by matrix element between the free exciton and the biexciton envelopes.The obtained probability of two-photon absorption in CuCl is about three orders of magnitude smaller when compared to that obtained by Hauamura.

Acta Physica Polonica A•Oct 1, 2000•1 citation
Measurements have been made of phas conjugation from degenerate four-wav mixing (DFWM) based on the large nonlinear susceptibility resulting from the two-photo absorption (TPA) resonance of the excitoni molecule state in CuCl. The excitonic molecule in CuCl is a bound state of two exciton that is responsible for a very strong two-photon absorption resonance at a photo energy of 3.186 eV at T ~ 4.2 K.1
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.
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.
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 probability of direct excitation of excitonic molecule in the two-photon absorption process is calculated with an Hylleraas-Ore type biexciton envelope, which is variationally optimized.In the second order of perturbation, because of the resonance effect, only the exciton .r5intermediate state is taken into account.The band structure at band extrema due to spin-orbit interaction is assumed.The transition probability of two-photon absorption is expressed by matrix element between the free exciton and the biexciton envelopes.The obtained probability of two-photon absorption in CuCl is about three orders of magnitude smaller when compared to that obtained by Hauamura.