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physica status solidi (b)

Exciton‐grating induced metamorphoses of the degenerate four‐wave mixing spectra in the giant two‐photon resonances of the excitonic molecules in CuBr and CuCl

Goro Mizutani, N. Nagasawa

Published Apr 1, 1989• 4 citations
Publisher

Abstract

Abstract It is demonstrated that the spectral shape of the DFWM generation in CuBr and CuCl show remarkable metamorphoses when the polarization of the incident two beams is set parallel to each other. According to the polarization character of the nonlinear polarization, these phenomena are concluded to be due to higher order non‐linearity than χ(3) where the really populated exciton grating contributes.

DOI
10.1002/pssb.2221520211

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The three-wave mixing process has been studied as functions of incident photon energy and also of the geometrical configuration when incident photon energy lies around the two-photon resonance of excitonic molecule. Experiments indicate that the intensity of the third order nonlinear light beam is enhanced when the phase matching condition derived from the dispersion of excitonic polariton holds or when incident photon energy is equal to the two-photon resonance of excitonic molecule. The relation between this three-wave mixing process and two-photon resonant Raman scattering so far observed is discussed. It is shown that this three-wave mixing process is regarded as the two-photon resonant, coherent Raman scattering via excitonic molecules.

Journal of the Physical Society of Japan•Dec 1, 1980•23 citations
Abstract It is demonstrated that the spectral shape of the DFWM generation in CuBr and CuCl show remarkable metamorphoses when the polarization of the incident two beams is set parallel to each other. According to the polarization character of the nonlinear polarization, these phenomena are concluded to be due to higher order non‐linearity than χ(3) where the really populated exciton grating contributes.
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.
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.
The three-wave mixing process has been studied as functions of incident photon energy and also of the geometrical configuration when incident photon energy lies around the two-photon resonance of excitonic molecule. Experiments indicate that the intensity of the third order nonlinear light beam is enhanced when the phase matching condition derived from the dispersion of excitonic polariton holds or when incident photon energy is equal to the two-photon resonance of excitonic molecule. The relation between this three-wave mixing process and two-photon resonant Raman scattering so far observed is discussed. It is shown that this three-wave mixing process is regarded as the two-photon resonant, coherent Raman scattering via excitonic molecules.