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physica status solidi (b)

Biexciton Two‐Photon Absorption and Raman Scattering in CuBr

A. I. Bobrysheva, V. V. Baltaga, M. V. Grodetskii

Published May 1, 1984• 1 citation
Publisher

Abstract

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.

DOI
10.1002/pssb.2221230119

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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.
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.
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.
Forward Raman scattering of excitonic molecule in CuCl has been studied at the giant two-photon excitation with using laser light having a wave vector K 0 but three different half band-widths, 0.2, 1.4 and 2.5 meV. In cases of laser excitation with broader half band-widths, the Raman and luminescence processes coexist and give emission lines called (LEP) R and (LEP) B , respectively. Both lines show the similar dependence of energy change upon the scattering angle. The (LEP) R and (LEP) B lines show red and blue shift, respectively, with the increase of laser excitation intensity. The excitonic molecule-state generated at K =2 K 0 is responsible for the (LEP) R line, while the (LEP) B line is considered to arise from a state having a certain K value smaller than 2 K 0 . Excitonic molecules generated coherently by the giant two-photon excitation are assumed to relax towards K =0 with keeping their individual momentum at almost the same value.
The biexciton optical Stark-effect under resonant pumping between the exciton and biexciton levels is studied theoretically. The probabilities of biexciton two-photon absorption of a weak probe light and of one-photon biexciton-exciton transition are calculated. The optical Stark splitting manifests itself in two-photon biexciton absorption through two absorption peaks spaced 2 (Omega) apart. Omega is the Raby frequency. In the luminescence spectrum due to biexciton-exciton one-photon transition three luminescence maxima appear which are shifted with respect to the luminescence maximum in the case without pumping.
The review deals with various variants of classification of the types of secondary emission of light by molecules; cases are distinguished in which the secondary emission occurs without additional processes that find their way between photon emission and absorption; the advisability of differentiating between the cases of resonance fluorescence and resonance scattering is noted. Reference is made to papers that have made contributions to the development of quantum-mechanical and classical theory of Raman scattering and to the development of the concepts of the relations between electron-vibrational absorption spectra, fluorescence spectra, and scattering excitation near and near and far resonance. Conditions are considered of excitation of the spectrum at different relations between the electronic-oscillator damping constant, the atom vibration frequency, the rotational frequencies, and the difference between the frequency of the incident light and the frequency of the electronic transition. The conditions for the excitation of typical light scattering, typical resonance fluorescence, and certain intermediate types, in which individual features of scattering are combined with certain features of fluorescence (phenomena of the transition type) are noted. The results of investigations of different models of the scattering centers, their advantages, shortcomings, and limits of applicability are compared. The most interesting results of the experimental investigations of resonant scattering of light by molecules and crystals are noted.