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physica status solidi (b)

Two‐photon resonant Raman scattering via biexcitons

Vu Duy Phach, Albert Bivas, B. Hönerlage, J. B. Grün

Published Mar 1, 1978• 58 citations
Publisher

Abstract

Abstract Two‐photon resonant Raman scattering processes are studied in different scattering configurations in CuCl. Observation of Raman lines from the front face of the crystal (backward scattering) yields new information on the energy of the transverse T5 exciton and on the biexciton damping. In transmission (forward scattering), two new emission lines can be identified as due to the Raman effect. They show a strong angular dependence because of the polariton nature of the particles involved. Their characteristic features contradict an interpretation in terms of Bose‐Einstein condensed biexcitons.

DOI
10.1002/pssb.2220860118

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physica status solidi (b)•May 1, 1979•1 citation

Biexciton Two‐Photon Absorption and Raman Scattering in CuBr

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Abstract The probabilities of the two‐photon absorption by a biexciton in the ground and the first vibrational states in CuBr and the probability of the two‐photon Raman scattering with the participation of the ground and the first vibrational states of the biexciton as intermediate states are calculated by perturbation theory method. Supposing that a Lorentzian distribution of frequencies ωi of the exciting light and a Lorentzian shape of the emission lines of the excition occur, the shape of the emission line at different values of the biexciton half‐width Γm is calculated. The dependence of the Raman scattering maximum position on ωi is obtained. At the condition 2Γ ≧ Γm; Γ Γm ≦ Γf the experimentally observed deviation of the Raman scattering maximum shifting from 2Δωi, is explained. The polarizational properties of the Raman scattering probability are obtained including the case when the intermediate states are the biexcitons Γ1, Γ5, Γ3.

physica status solidi (b)•May 1, 1984•1 citation
Abstract Two‐photon resonant Raman scattering processes are studied in different scattering configurations in CuCl. Observation of Raman lines from the front face of the crystal (backward scattering) yields new information on the energy of the transverse T5 exciton and on the biexciton damping. In transmission (forward scattering), two new emission lines can be identified as due to the Raman effect. They show a strong angular dependence because of the polariton nature of the particles involved. Their characteristic features contradict an interpretation in terms of Bose‐Einstein condensed biexcitons.
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.
Giant two-photon absorption spectrum for the direct generation of excitonic molecules is measured with using a frequency tunable dye laser, and absorption peak is found at 3.1870 eV. Emission spectrum with excitation at the giant two-photon absorption band depends on the spectral width, ΔΩ1\varDelta\varOmega_{1}ΔΩ1​, of excitation light. In the case of ΔΩ1=0.25\varDelta\varOmega_{1}{=}0.25ΔΩ1​=0.25 meV, the two-photon resonance Raman scattering is found to be predominant. The Raman process involves an excitonic molecule and a longitudinal exciton as the intermediate and final states, respectively. On the other hand, for the case of ΔΩ1=2.3\varDelta\varOmega_{1}{=}2.3ΔΩ1​=2.3 meV, the emission spectrum shows a very sharp line at 3.1649 eV, which has been previously ascribed to be due to the Bose-Einstein condensation of excitonic molecules. Discussions are made on the dependence of emission spectrum upon the energy band-width of excitation light.
Various optical spectra such as time-resolved luminescence spectra are studied for excitonic molecules in CuCl under two-photon resonance excitation by using picosecond and nanosecond frequency-tunable laser pulses. Two sharp emission lines observed under resonance excitation are ascribed to the radiative decay of “cold” excitonic molecules created directly at k ∼2 k 0 , while the broad emission band on the low energy side of the sharp line to the luminescence of “hot” molecules created through single excitons. The stimulated emission process gives a considerable influence on both the sharp luminescence lines and the hot molecule band, and further on two-photon resonant excitonic Raman lines as well. Discussions are made on the Bose condensation of the excitonic molecules and also on whether the emission under just-resonance excitation is due to Raman scattering or luminescence.
Abstract Phonon‐assisted two‐photon absorption of biexcitonic levels in CuCl is considered including damping of the nearly resonant excitonic intermediate state. A pronounced structure of the line shape due to resonance effects, threshold effects, and structure in the Fourier transform of the envelope of the excitonic molecule is predicted. A detailed discussion of both temperature and damping effects is given. Large cross sections are predicted. The most favourable energetic range to observe the effects derived here is the low energy tail of the line, on the left of the Γ⅕ exeiton.
Abstract The probabilities of the two‐photon absorption by a biexciton in the ground and the first vibrational states in CuBr and the probability of the two‐photon Raman scattering with the participation of the ground and the first vibrational states of the biexciton as intermediate states are calculated by perturbation theory method. Supposing that a Lorentzian distribution of frequencies ωi of the exciting light and a Lorentzian shape of the emission lines of the excition occur, the shape of the emission line at different values of the biexciton half‐width Γm is calculated. The dependence of the Raman scattering maximum position on ωi is obtained. At the condition 2Γ ≧ Γm; Γ Γm ≦ Γf the experimentally observed deviation of the Raman scattering maximum shifting from 2Δωi, is explained. The polarizational properties of the Raman scattering probability are obtained including the case when the intermediate states are the biexcitons Γ1, Γ5, Γ3.