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Journal of the Physical Society of Japan

Radiative and Two-Photon Resonance Raman Processes Associated with Excitonic Molecules in CuCl

N. Nagasawa, Tsuneyoshi Mita, Masayasu Ueta

Published Sep 15, 1976• 96 citations
Publisher

Abstract

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, \(\varDelta\varOmega_{1}\), of excitation light. In the case of \(\varDelta\varOmega_{1}{=}0.25\) 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 \(\varDelta\varOmega_{1}{=}2.3\) 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.

DOI
10.1143/jpsj.41.929

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Journal of the Physical Society of Japan•Aug 1, 1978•15 citations
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, (\varDelta\varOmega_{1}), of excitation light. In the case of (\varDelta\varOmega_{1}{=}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 (\varDelta\varOmega_{1}{=}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.
Through the studies of excitation spectra of emissions in CuCl crystals by a frequency tunable dye laser, excitonic molecules have been found to be generated directly by the giant two-photon absorption at the photon energy of 3.187 eV, as suggested by Hanamura. Two-photon excitation of crystals at 1.6 K enhanced very narrow emission bands at 3.1647 eV and at 3.1709 eV. These photon energies coincide with those of the high energy edges of the M L and M T bands due to the radiative annihilation of excitonic molecules having K =0. From these facts the Bose condensation of excitonic molecules at K ∼0 has been suggested.
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.
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.
Excitonic molecule state in CuCl has been resonantly excited by the combination of two circularly polarized laser beams of slightly different energies and of the opposite propagation vectors. The secondary emissions associated with the excitonic molecule state of a quite small momentum have been investigated by changing the spectral width of the incident laser light. With the increase of the band width of excitation laser, the luminescence becomes dominant and the Raman component is suppressed. An emission line at 3.1869 eV is assigned to the luminescence due to the decomposition of excitonic molecules, distributed in a region of ±0.022 k 0 around 0.050 k 0 , into a pair of polaritons, where k 0 is the wave vector of the photon of 3.1861 eV. The relaxation of the excitonic molecule system really generated at the small momentum region has been discussed.
The Γ1\varGamma_{1}Γ1​-symmetry of the lowest excitonic molecule state of CuCl has been confirmed experimentally from the measurements of the giant two-photon absorption and resonance Raman scattering by using circularly polarized dye laser light. The giant two-photon transition is found to be forbidden for single beam of circularly polarized light while it is allowed for two beams of circularly polarized lights impinging in crystals from directly opposite directions. It has been verified that the lowest excitonic molecule state is composed of two-electron- and two-hole-states both of the composite spin angular momentum zero.