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Journal of Physics Condensed Matter

Dynamical Stark effect in an exciton-biexciton system

Tohya Hiroshima

Published Apr 6, 1992• 1 citation
Publisher

Abstract

A coherently excited exciton-biexciton system under the action of a non-resonant pump field is analysed within the framework of the Hartree-Fock-Bogolyubov theory. The excitation spectra, which consist of optical absorption and gain, are determined. It is pointed out that the optical gain is greatly enhanced through the giant oscillator strength effect of biexcitonic molecules. Numerical examples for CuCl are also presented.

DOI
10.1088/0953-8984/4/14/015

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A coherently excited exciton-biexciton system under the action of a non-resonant pump field is analysed within the framework of the Hartree-Fock-Bogolyubov theory. The excitation spectra, which consist of optical absorption and gain, are determined. It is pointed out that the optical gain is greatly enhanced through the giant oscillator strength effect of biexcitonic molecules. Numerical examples for CuCl are also presented.
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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.
We measured the transient reflection spectra induced by infrared light for a CuCl single crystal using pump-probe spectroscopy. A Stark shift of the 1 s exciton was observed using light with a near resonant energy between the 1 s and 2 p exciton levels. The amount of energy shift due to the Stark effect was obtained from the absorption spectra calculated using the Kramers–Kronig transform. We investigated the energy shift of 1 s excitons with respect to the excitation density. This is the first published report on the Stark effect of 1 s exciton associated with the internal energy levels of the excitons in CuCl crystal.
Large, nonlinear-optical phenomena are shown theoretically to be observable under nearly two-photon resonant pumping of the excitonic molecule (EM), e.g., in a CuCl crystal. When the exciton polariton (EP) is resonantly pumped into the EM, they are hybridized with each other and show optical Stark splitting. These splittings can be observed, respectively, as a sharp dip in the reflection spectrum and two-photon absorption spectrum due to the EM. We can also clarify how these splittings change into the blueshifts and redshifts of the EP and the EM as functions of the pump frequency and power. The generation of the phase-conjugated wave is shown also to be enhanced under two-photon resonant pumping of the EM. Some characteristics about pump-probe frequency and polarization dependences are also clarified. We have also derived the effective Hamiltonian of the exciton and the EM from the first-principles equation of motion for the exciton coupled with that of the EM. This Hamiltonian has made possible the theoretical analysis of these nonlinear-optical phenomena.
The optical properties of a semiconductor pumped near the 1s exciton resonance are studied. The equation of motion for the density matrix in the Hartree-Fock approximation is traced back to the Bloch equation, well known from two-level systems. The essential difference, however, is the coupling of different wave vectors via the Coulomb potential. Principal features of the different stationary solutions are discussed. For a closer inspection of stability, we calculate the response to a smooth switchon of the pump field. For pump frequencies above the 1s exciton, the system follows first adiabatically the pulse shape, showing a blueshift and a slight increase of the oscillator strength as in the off-resonant case. The system jumps later into a second solution characterized by optical gain below the pump frequency, related to complete saturation (excitonic insulator). The major objective of our paper is to provide a numerical solution to the equation of motion in the Hartree-Fock approximation and to compare the results to those obtained by stationary considerations.
Abstract In CuCl at 1.7 K optical gain/absorption spectra are recorded in the spectral range of bound exciton and biexciton emission. Energy, effective temperature, and oscillator strength of biexcitons are determined. The observed kinetics indicates that the total pair density in the exciton‐biexciton system is pinned at about 1.6 × 1016 cm−3 for all excitation densities above 10 kW/cm2. At intense excitation, a Fano‐interference is observed between a discrete impurity absorption line and a continuum absorption tail. The latter is followed by a band of positive gain towards lower photon energies.