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physica status solidi (b)

Exciton‐Grating Induced Light Mixing at the Giant Two‐Photon Resonances of Excitonic Molecules in CuBr

Goro Mizutani, N. Nagasawa

Published Feb 1, 1989• 3 citations
Publisher

Abstract

Abstract It is shown that in CuBr crystals a coherent scattering process where the exciton population grating and the excitonic molecule are involved is present, from the experiment of a three beam non‐degenerate optical mixing. This process cannot be described by the 3rd order optical nonlinearity but at least a 5th order non‐linearity is necessary.

DOI
10.1002/pssb.2221510219

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physica status solidi (b)•Apr 1, 1985•13 citations
Abstract It is shown that in CuBr crystals a coherent scattering process where the exciton population grating and the excitonic molecule are involved is present, from the experiment of a three beam non‐degenerate optical mixing. This process cannot be described by the 3rd order optical nonlinearity but at least a 5th order non‐linearity is necessary.
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.
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.
Giant two-photon absorption for the direct generation of excitonic molecue is measured. Three absorption peaks are found at 2.9540, 2.9561 and 2.9576 eV, which are responsible for the two-photon transitions to the Γ1(J=0)\varGamma_{1}(J{=}0)Γ1​(J=0), Γ 5 ( J =2) and Γ3(J=2)\varGamma_{3}(J{=}2)Γ3​(J=2) states, respectively, of the excitonic molecule.
Abstract Transient light‐induced gratings due to free carriers and excitons are created in CdSe in a medium density range of 1015 to 1017 cm−3 by two coherent intense (ns) IR‐pump beams. Detailed investigations of probe‐beam diffraction due to thin excitonic gratings in the spectral region just below the An = 1 ‐exciton line at 85 K and its dependence on sample temperature and on the excitation level are presented. First‐order diffraction efficiences up to 5% and a nonlinear dependence of diffraction on the excitation level can be observed. For the first time numerical calculations of probe‐beam diffraction due to excitonic phase and amplitude gratings are presented. The comparison with the experiment shows, that the damping of a dense exciton gas increases proportional to the excitation intensity in the case of two‐photon interband excitation, and that the light‐induced absorptive changes Δ due to dense excitons dominate over the dispersive changes Δn in the spectral region under consideration.