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Optics and Spectroscopy

On the possibility of Raman scattering of light via decay of the incident photon into two photons and a phonon

Vasilij N. Moiseenko, В. С. Горелик, V. Т. Shvets, B. Abusal

Published Jan 1, 1999• 0 citations
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The unusual two-photon emission by Bose-condensed excitons caused by simultaneous recombination of two excitons with opposite momenta leaving the occupation numbers of excitonic states with momenta $\mathbf{p}\ensuremath{\ne}0$ unchanged (below coherent two-exciton recombination) is investigated. Raman scattering accompanied by the analogous two-exciton recombination (or creation) is also analyzed. The excess momentum equal to the change of the electromagnetic field momentum in these processes can be transferred to phonons or impurities. The processes under consideration take place if there is Bose condensation in the interacting exciton system, and, therefore, can be used as a method to reveal exciton Bose condensation. If the frequency of the incident light $\ensuremath{\omega}<2\ensuremath{\Omega}$ $(\ensuremath{\Omega}$ is the frequency corresponding to the recombination of an exciton with p=0), the coherent two-exciton recombination with the excess momentum elastically transferred to impurities leads to the appearance of the spectral line $2\ensuremath{\Omega}\ensuremath{-}\ensuremath{\omega}$ corresponding to the induced two-photon emission. In this case the anti-Stokes line on frequency $\ensuremath{\omega}+2\ensuremath{\Omega}$ also appears in the Raman spectrum. If $\ensuremath{\omega}>2\ensuremath{\Omega},$ there are both Stokes and anti-Stokes lines on frequencies $\ensuremath{\omega}\ifmmode\pm\else\textpm\fi{}2\ensuremath{\Omega}$ in the Raman spectrum. The induced two-photon emission is impossible in this case. The spectral lines mentioned above have phonon replicas on frequencies $|\ensuremath{\omega}\ifmmode\pm\else\textpm\fi{}(2\ensuremath{\Omega}\ensuremath{-}n{\ensuremath{\omega}}_{0}^{s})|$ corresponding to the transmission of the excess momentum (partially or as a whole) to optical phonons of frequency ${\ensuremath{\omega}}_{0}^{s}$ $(n$ is an integer number). The quantitative estimation shows that the light corresponding to the coherent two-exciton recombination can be experimentally observed in ${\mathrm{Cu}}_{2}\mathrm{O}.$

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Optics and Spectroscopy•Nov 1, 1967•1 citation
The unusual two-photon emission by Bose-condensed excitons caused by simultaneous recombination of two excitons with opposite momenta leaving the occupation numbers of excitonic states with momenta $\mathbf{p}\ensuremath{\ne}0$ unchanged (below coherent two-exciton recombination) is investigated. Raman scattering accompanied by the analogous two-exciton recombination (or creation) is also analyzed. The excess momentum equal to the change of the electromagnetic field momentum in these processes can be transferred to phonons or impurities. The processes under consideration take place if there is Bose condensation in the interacting exciton system, and, therefore, can be used as a method to reveal exciton Bose condensation. If the frequency of the incident light $\ensuremath{\omega}<2\ensuremath{\Omega}$ $(\ensuremath{\Omega}$ is the frequency corresponding to the recombination of an exciton with p=0), the coherent two-exciton recombination with the excess momentum elastically transferred to impurities leads to the appearance of the spectral line $2\ensuremath{\Omega}\ensuremath{-}\ensuremath{\omega}$ corresponding to the induced two-photon emission. In this case the anti-Stokes line on frequency $\ensuremath{\omega}+2\ensuremath{\Omega}$ also appears in the Raman spectrum. If $\ensuremath{\omega}>2\ensuremath{\Omega},$ there are both Stokes and anti-Stokes lines on frequencies $\ensuremath{\omega}\ifmmode\pm\else\textpm\fi{}2\ensuremath{\Omega}$ in the Raman spectrum. The induced two-photon emission is impossible in this case. The spectral lines mentioned above have phonon replicas on frequencies $|\ensuremath{\omega}\ifmmode\pm\else\textpm\fi{}(2\ensuremath{\Omega}\ensuremath{-}n{\ensuremath{\omega}}_{0}^{s})|$ corresponding to the transmission of the excess momentum (partially or as a whole) to optical phonons of frequency ${\ensuremath{\omega}}_{0}^{s}$ (n(n(n is an integer number). The quantitative estimation shows that the light corresponding to the coherent two-exciton recombination can be experimentally observed in Cu2O.{\mathrm{Cu}}_{2}\mathrm{O}.Cu2​O.
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.
Using the approximation of small fluctuations around a stationary solution, photon statistics and quadrature variances are derived in stimulated Raman and hyper-Raman scattering including the coupling of pumping, Stokes, anti-Stokes and phonon modes. The depletion of pump light is included. Compared to Raman scattering, additional regimes to generate anti-bunched, sub-Poisson and squeezed light were found caused by self-interaction of the pump mode. It was possible to include effects of nonlinear dynamics, initial squeezing of radiation and phonon system, external noise and losses.