The Bose condensation of many exciton system is observed experimentally for the first time. It is found that excitonic molecules in CdSe exhibit the Bose condensation when the excitation is given at 1.8∼4.2 K by pico-second light pulses from a model-locked neodymium glass laser. This is concluded from the experimental facts that (1) an extremely sharp luminescence line attributed to originate from the k =0 condensed excitonic molecules is observed, (2) this sharp line is accompanied by the side-band on the low energy side and the spectrum is well understood by the theory developed by one of the authors, and (3) this line is produced within a limited range of excitation density which is wider at 1.8 K than at 4.2 K. Some arguments are presented on the importance of the use of the picosecond pulse excitation for the realization of the condensation.
The Bose condensation of many exciton system is observed experimentally for the first time. It is found that excitonic molecules in CdSe exhibit the Bose condensation when the excitation is given at 1.8∼4.2 K by pico-second light pulses from a model-locked neodymium glass laser. This is concluded from the experimental facts that (1) an extremely sharp luminescence line attributed to originate from the k =0 condensed excitonic molecules is observed, (2) this sharp line is accompanied by the side-band on the low energy side and the spectrum is well understood by the theory developed by one of the authors, and (3) this line is produced within a limited range of excitation density which is wider at 1.8 K than at 4.2 K. Some arguments are presented on the importance of the use of the picosecond pulse excitation for the realization of the condensation.
To study the dynamical processes of high density single excitons and excitonic molecules in CdSe, the time dependences of M, P M and P luminescence lines and the time-resolved absorption spectra of A excitons are measured in the pico-second region at 4.2 K. The exciton absorption peak shifts to the high energy side due to the high density effect, the shift reaching the maximum at 20 ps after the pulse excitation. M line reaches the maximum at 100 ps, P M line at 200 ps and P line at 300∼350 ps. The decay constants are 100, 100 and 350 ps, respectively. The dynamical aspects of the formation of A excitons, the formation of excitonic molecules and the inelastic collisions of single excitons and excitonic molecules are discussed. It is interpreted why the use of the pico-second pulse excitation is essentially important for the realization of the Bose condensation of excitonic molecules.
In a first part, a brief review of some excitonic properties is presented, with the accent put on their relevance with respect to the possibility of Bose-Einstein condensation. In a second part, recent experimental evidence is described, which supports the idea that excitonic particles may form a highly quantum fluid. In Cu20, the analysis of the exciton decay spectrum shows a gradual evolution of the gas from a classical regime at low densities up to a strongly degenerate one at high densities, with a chemical potential µ ~ 0. In CuCl excitons are unstable against formation of molecules (biexcitons). It is possible to generate directly a high density gas of biexcitons with momentum K ~ 0 by giant two-photon absorption. At low excitation, the observed molecular emission is in agreement with Maxwell -Boltzmann statistics. At high densities, strong deviations occur. In particular, the appearance of a sharp emission line is attributed to the presence of a Bose-Einstein condensate of excitonic molecules.
The case of excitons as candidates for Bose–Einstein condensation is discussed, and experimental results in CuCl and Cu 2 O are presented. In CuCl, spectral analysis of the luminescence from biexcitons as a function of their density reveals a gradual evolution from classical statistics towards a quantum degenerate regime. The appearance of a sharp emission line below a critical temperature and above a critical density is attributed to the presence of a laser-induced Bose–Einstein condensate of excitonic molecules. This interpretation is supported by pump-probe experiments which show that additional particles injected in the presence of a biexciton condensate are drawn into it. In Cu 2 O, free exciton luminescence spectral analysis of ortho- and paraexcitons reveals a gradual evolution from a classical to a Bose quantum degenerate regime with increasing particle densities. Orthoexciton densities close to the critical density for condensation are obtained at high incoherent excitation. Under similar pumping, paraexciton densities exceeding the critical value are inferred from luminescence intensity ratios. Anomalous transport properties of paraexcitons, such as ballistic propagation over macroscopic distances and formation of soliton-like excitonic packets are discussed as evidence for excitonic superfluidity. Introduction Excitons The lowest electronically excited state of a non-metallic crystal corresponds to the promotion of one electron from the top of the highest fully occupied valence band to the bottom of the next empty conduction band. A correct evaluation of the required energy must include the Coulomb correlation between the promoted electron and all other electrons left behind in the valence band.
A comprehensive investigation of the optical properties of excitonic molecules in CuCl films is presented and discussed. The experimental work includes resonant two-photon absorption (TPA), observations of the resonantly excited biexciton emission, and optical pump-and-probe studies. The collision broadening of the TPA implies a collision rate \ensuremath{\sim}${10}^{\ensuremath{-}12}$ sec for the biexcitons, which is sufficiently rapid to establish a quasithermal equilibrium for the particles on a time scale that is short in comparison with the biexciton lifetime and the duration of the laser pump pulse. The biexciton luminescence line shapes obtained with resonant $\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}=0$ two-photon excitation have been fitted using a Bose-Einstein thermal distribution of biexcitons. The chemical potential obtained from the fits goes to zero as the biexciton density is increased at a fixed lattice temperature or if the lattice temperature is decreased at fixed density. The sharp luminescence features that are observed at high densities and low temperatures with single-beam, two-photon excitation are interpreted as resulting from a Bose-Einstein---condensed state of the biexcitons at twice the wave vector of the laser pumping photons. Further evidence for a condensed state is obtained from optical-probe measurements in which a small number of probe biexcitons is injected into the sample, with and without the presence of a condensed state produced by an intense laser pump beam. The luminescence of these injected probe biexcitons is modified in the presence of the pump beam such that it exhibits the sharp features of the emission from the condensed state. Measurements of optical gain and stimulated emission in the presence of the pump beam show that the redistribution of the probe luminescence does not result from those processes, but must involve a preferential redistribution of the probe particles in momentum space via collisions. Such a redistribution is expected when additional particles are added to a condensed system of bosons.
Pulsed-laser excitation of naturally grown crystals of Cu2O produces a dense gas of excitons, which exhibits Bose-Einstein quantum statistics. Both orthoexcitons and paraexcitons, split by a 12-meV electron-hole exchange energy, are formed. At high excitation levels, the time-resolved luminescence of orthoexcitons yields a density-temperature relation that follows the phase boundary for Bose-Einstein condensation, n=CT3/2, but no striking evidence for a condensed fraction is observed. We have now measured the time-resolved spectrum of the lower-lying paraexcitons whose luminescence is 1500 times weaker than the orthoexciton luminescence. At intermediate power levels, the paraexciton distribution is more degenerate than the orthoexcitons. The relative intensities of the two species indicate that at high excitation levels the paraexciton density exceeds the critical density for condensation. At these high densities the paraexciton spectrum develops a structure that cannot be explained in terms of the thermalized Bose-Einstein distribution. Time-resolved spatial measurements of the luminescence indicate a rapid nondiffusive expansion of the gas at supersonic velocities that approach the expected ballistic velocities of the excitons. The rapid transport and the concurrent changes in the spectral distribution of paraexcitons may be the first observation of excitonic Bose-Einstein condensation and superfluidity.
Introduction. Polaritons and Semiconductor Microcavities As we have mentioned previously, BEC of excitons or biexcitons and lasing can be seen as two limits of the same theory. Lasing occurs in the case of strong electron-photon coupling (recombination rate fast compared with interparticle-scattering rate) while excitonic BEC occurs in the case of weak electron-photon coupling (recombination rate slow compared with the interparticle-scattering rate.) A laser can be seen as a Bose condensate in which the long-range phase coherence exists in the photon states [1], while in the exciton condensate the coherence exists in the electronic states. This is one of the reasons for some of the confusing debates in the early history of excitonic Bose condensation – in many systems there is not a sharp distinction between an excitonic condensate and supperradiance, i.e., luminescence with enhanced intensity due to stimulated emission [2-4]. In the previous chapters, we have so far considered a laser light source only as a source of excitons by means of quantum transitions. In Chapter 6, the laser radiation was taken into account as a given external factor. This chapter is dedicated to phenomena related to a strong and noticeable exciton-photon interaction, when the light significantly influences the energy spectrum of the high-density excitons [5-9]. As we will see, this leads to many fascinating effects related to instabilities. A strong exciton-photon interaction implies a strong polariton effect, in which photon and exciton states are mixed (as in Fig. 1.3). When this mixing is strong, it is not obvious how to define the ground state of the system.