Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Journal of the Physical Society of Japan

Two-Photon Resonant, Coherent Raman Scattering via Excitonic Molecules in CuCl

Yasuaki Masumoto, Shigeo Shionoya

Published Dec 1, 1980• 23 citations
Publisher

Abstract

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.

DOI
10.1143/jpsj.49.2236

Related papers

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

N. Nagasawa, Tsuneyoshi Mita, Masayasu Ueta

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.

Journal of the Physical Society of Japan•Sep 15, 1976•96 citations

Phase-Conjugation by Four-Wave Mixing in CuCl: Resonance Enhancement by Exciton and Excitonic Molecule and Its Polarization Dependence

Goro Mizutani, N. Nagasawa

The phase-conjugation in crystalline CuCl has been studied at 1.6 K. It has been found that the two-photon resonance of the \(\varGamma_{1}\)-excitonic molecule and the one-photon resonance of the \(\varGamma_{5}\)-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.

Journal of the Physical Society of Japan•Jun 1, 1983•27 citations

Optical Nonlinearity Due to the Excitonic System in CuCl

N. Nagasawa

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.

physica status solidi (b)•Dec 1, 1988•2 citations

Relaxation of Excitonic Molecules Generated by the Giant Two-Photon Laser Excitation in CuCl

N. Nagasawa, Tsuneyoshi Mita, Tadashi Itoh +1 more

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.

Journal of the Physical Society of Japan•Oct 1, 1977•6 citations

Resonance Raman Scattering and Luminescence from Highly Excited States

T. Takagahara

Resonance Raman scattering and luminescence under an intense excitation field are studied for both stationary and transient excitation regimes. By means of the Green function theory of resonance Raman scattering and luminescence we explain the characteristic features of the recent experiments on two-photon resonance Raman scattering via excitonic molecule in CuCl where the resonance dip and the asymmetry of the Raman yield around the resonance were observed. We ascribe the origin of the resonance dip of the Raman yield to the resonance enhancement of collisional damping of excitonic molecule and exciton states. The asymmetry of the Raman yield can be naturally understood in terms of the frequency and wave-vector dependent relaxation constants. Furthermore an approach is proposed which incorporates the coherence and correlation among excitonic molecules and excitons in their non-equilibrium state and clarifies their effects on the optical spectra.

Progress of Theoretical Physics Supplement•May 14, 2013•0 citations

Two‐photon resonant Raman scattering via biexcitons

Vu Duy Phach, Albert Bivas, B. Hönerlage +1 more

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.

physica status solidi (b)•Mar 1, 1978•58 citations
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.
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.
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.
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.
Resonance Raman scattering and luminescence under an intense excitation field are studied for both stationary and transient excitation regimes. By means of the Green function theory of resonance Raman scattering and luminescence we explain the characteristic features of the recent experiments on two-photon resonance Raman scattering via excitonic molecule in CuCl where the resonance dip and the asymmetry of the Raman yield around the resonance were observed. We ascribe the origin of the resonance dip of the Raman yield to the resonance enhancement of collisional damping of excitonic molecule and exciton states. The asymmetry of the Raman yield can be naturally understood in terms of the frequency and wave-vector dependent relaxation constants. Furthermore an approach is proposed which incorporates the coherence and correlation among excitonic molecules and excitons in their non-equilibrium state and clarifies their effects on the optical spectra.
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.