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Journal of Experimental and Theoretical Physics Letters

Inelastic light scattering by dipolar excitons

V. M. Kovalev, Alexander V. Chaplik

Published Oct 1, 2011• 0 citations
Publisher

Abstract

The cross section for inelastic light scattering by a system of spatially indirect excitons is calculated. It is shown that there are two resonant scattering channels, one related to the transitions via the vacuum and the other via the two-exciton states of the crystal, and their contributions to the scattering amplitude cancel each other. As a result, there is no resonance enhancement of light scattering by excitons for photon energies in the vicinity of the band gap.

DOI
10.1134/s0021364011160107

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The cross section for inelastic light scattering by a system of spatially indirect excitons is calculated. It is shown that there are two resonant scattering channels, one related to the transitions via the vacuum and the other via the two-exciton states of the crystal, and their contributions to the scattering amplitude cancel each other. As a result, there is no resonance enhancement of light scattering by excitons for photon energies in the vicinity of the band gap.
We use dynamical mean field theory to find an exact solution for inelastic light scattering in strongly correlated materials such as those near a quantum-critical metal-insulator transition. We evaluate the results for q=0 (Raman) scattering and find that resonant effects can be quite large, and yield a double resonance, a significant enhancement of nonresonant scattering peaks, a joint resonance of both peaks when the incident photon frequency is on the order of U, and the appearance of an isosbestic point in all symmetry channels for an intermediate range of incident photon frequencies.
We study the resonance Raman scattering of light from a three-level atom embedded in a photonic band-gap material or in a frequency dispersive medium whose photon spectrum exhibits a gap due to photon coupling to medium excitations such as excitons and optical phonons. We demonstrate that the one-particle spectrum of the system consists of either a continuous part with energy lying outside the gap or a single discrete mode with energy lying inside the gap. The discrete mode, which occurs when both of the allowed atomic transitions of the $\ensuremath{\Lambda}$ configuration lie inside the gap, can be treated as a photon-atom bound state in which the radiation is localized in the vicinity of the atom. In the case of the continuous spectrum, the Rayleigh and Stokes lines are shifted as well as narrowed (or broadened) as the corresponding transition frequencies are shifted relative to the upper band edge, providing a distinctive experimental signature of atom-photon interactions near a photonic band edge.
Great progress has been made in recent years in experimental studies of excitonic molecules, both in direct-band and indirect-band semiconductors. The exciton systems in these semiconductors differ substantially. In direct-band semiconductors with dipole-allowed optical transitions, the direct-recombination times are extremely small. Consequently the processes of binding of excitons into excitonic molecules and their decay occur under strongly nonequilibrium conditions. Hence one can obtain the fundamental information on biexcitons in these semiconductors by nonlinear optical methods. This review discusses the processes on which the various methods are based: two-photon resonance excitation of biexcitons, induced one-photon conversion of an exciton into a biexciton, two-photon resonance Raman scattering involving biexciton states, etc., and their application to studying biexcitons with the example of CdS. Problems of bistability involving biexcitons are also briefly discussed. In indirect semiconductors, where recombination occurs with the emission of a phonon, the lifetimes of excitons are large, and quasiequilibrium can be established in the exciton system. Under these conditions the information on the properties of the molecules is obtained by analyzing their radiative-decay spectra. The problem of detecting biexcitons in indirect semiconductors, radiative decay of molecules, and the effect on their stability of external electric, strain, and magnetic fields are discussed in detail with the examples of Si and Ge. Also the results of investigating the quantum statistical behavior of a dense gas of spin-oriented excitons (in a magnetic field under conditions in which the biexcitons are destabilized) are briefly presented (using the example of uniaxially compressed germanium), and the question of the possibility of their Bose condensation is discussed.
A theory of resonant Raman scattering spectroscopy of one-dimensional electronic systems is developed on the assumptions that (i) the excitations of the one-dimensional electronic system are described by the Luttinger-liquid model, (ii) Raman processes involve virtual excitations from a filled valence band to an empty state of the one-dimensional electronic system, and (iii) excitonic interactions between the valence and conduction bands may be neglected. Closed form analytic expressions are obtained for the Raman scattering cross sections, and are evaluated analytically and numerically for scattering in the polarized channel, revealing a ``double-peak'' structure with the lower peak involving multispinon excitations with total spin S=0S=0S=0 and the higher peak being the conventional plasmon. A key feature of our results is a nontrivial power-law dependence, involving the Luttinger-liquid exponents, of the dependence of the Raman cross sections on the difference of the laser frequency from resonance. We find that near resonance the calculated ratio of intensity in the lower energy feature to the intensity in the higher energy feature saturates at a value of the order of unity (times a factor of the ratio of the velocities of the two modes). We explicate the differences between the ``Luttinger-liquid'' and ``Fermi-liquid'' calculations of resonant Raman spectroscopy (RRS) spectra and argue that excitonic effects, neglected in all treatments so far, are essential for explaining the intensity ratios observed in quantum wires. We also discuss other Luttinger-liquid features which may be observed in future RRS experiments.
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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.