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Physical Review Letters

Observation of quantum beats in the resonance fluorescence of free excitons

V. Langer, H. Stolz, Wolf von der Osten

Published Feb 19, 1990• 109 citations
Publisher

Abstract

The occurrence of quantum beats for an extended exciton state in a solid is demonstrated for the first time. They are observed as oscillations in the two-phonon resonance fluorescence decay of the indirect free exciton states in AgBr split in magnetic fields up to 1 T after excitation by picosecond laser pulses. The results are in agreement with calculations by a density-matrix formalism. From the beating frequencies the splitting of the exciton states can be obtained with high accuracy. Quantum dephasing times of several hundred picosecond are determined comparable to the energy relaxation time.

DOI
10.1103/physrevlett.64.854

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Summary form only given. The optical properties of semiconductor quantum wells (QW) and, in particular, the coherent dynamics of excitons following resonant excitation with ultrafast laser pulses have attracted much attention in recent years. It is generally accepted that there is a transfer of coherence between the optical field and the QW that disappears in a characteristic time T/sub 2/ (picoseconds for GaAs) after the laser is turned off. However, the questions as to how the coherence is actually induced and that of the nature of the coherent state of the solid are poorly understood. In this work we address these points by re-examining the longstanding problem of the (classical vs. quantum) nature of the ubiquitous beats associated with the light-hole (LX) heavy-hole (HX) excitons, which are observed in transient optical experiments on QW. To this end, we consider the coherent behavior of excitons using the simplest albeit non-trivial model where they are treated as non-interacting bosons. Our results bear directly on studies for which nonlinear effects are not important and are not aimed directly at explaining the fourwave-mixing (FWM) experiments that dominate the field. Nevertheless, since nonlinear effects are, typically, weak compared with harmonic contributions, the free boson picture provides in all cases the correct lowest order wavefunction of the photoexcited solid.

Quantum Electronics and Laser Science Conference•Jan 20, 2003•0 citations
The occurrence of quantum beats for an extended exciton state in a solid is demonstrated for the first time. They are observed as oscillations in the two-phonon resonance fluorescence decay of the indirect free exciton states in AgBr split in magnetic fields up to 1 T after excitation by picosecond laser pulses. The results are in agreement with calculations by a density-matrix formalism. From the beating frequencies the splitting of the exciton states can be obtained with high accuracy. Quantum dephasing times of several hundred picosecond are determined comparable to the energy relaxation time.
We report the first observation of quantum beats in the resonance fluorescence of a bound exciton in a semiconductor, the ionized-donor exciton complex in CdS. Measurements of the polarization behavior and magnetic-field dependence of the beats permitted a detailed investigation of strain effects and magneto-optical parameters of the states. From the damping of the beats, coherence times of the order of several hundreds of picoseconds are deduced. For the neutral-donor and -acceptor bound exciton states, very rapid dephasing with coherence times of the order of 20 ps is found.
Utilizing transform-limited time-resolved light scattering with simultaneously optimum temporal and spectral resolution, it is possible to investigate on a picosecond time scale energy and phase relaxation processes of excitons in semiconductors. Thereby quantum-beating as a measure of exciton coherence allows us to discriminate Raman scattering from hot luminescence as exemplified for indirect free excitons in AgBr. In order to distinguish resonant Rayleigh scattering occurring in disordered systems from ordinary fluorescence, the experimental setup has to be fully included in the theoretical description of the light scattering process. Experiments at the (n equals 1, e-hh) exciton in GaAs/AlGaAs quantum well structures confirm the predicted finite decay of this process and allow us to measure the exciton relaxation dynamics.
Multiple frequency quantum beats of a system of the coherently excited quantum confined exciton states in a high-quality semiconductor structure containing a wide InGaAs/GaAs quantum well are experimentally detected by the spectrally resolved pump-probe method. The beat signal is observed both at positive and at negative delays between the pump and probe pulses. Several quantum beat (QB) frequencies are observed in the experiments, which coincide with the interlevel spacings in the exciton system. A theoretical model is developed, which allows one to attribute the QBs at negative delay to the four-wave mixing (FWM) signal detected at the nonstandard direction. The beat signal is strongly enhanced by the interference of the FWM signal with the secondary emission induced by the probe pulse. At positive delays, the QBs are due to the interference of the quantum confined exciton states. The decay time for QBs is of the order of several picoseconds both at positive and negative delays. This is close to the relaxation time of the exciton population that allows one to consider the exciton depopulation as the main mechanism of the coherence relaxation in the system under study.
This work presents new results of experimental studies of exciton relaxation in GaAs/AlGaAs multiple quantum well materials, using transient nonlinear laser spectroscopy techniques. In the low excitation regime, effective optical Bloch equations similar to the density matrix formalism of a two-level system describe the response. Solutions of these equations appropriate for three-pulse scattering studies are presented, along with a discussion of new experimental techniques used in this work. Non-ideal conditions present in the molecular beam epitaxy growth process introduce monolayer fluctuations in the quantum well thickness, leading to inhomogeneous broadening and exciton localization at sites of minimum energy. Localized excitons are separated in energy from extended, quasi-delocalized states by the mobility edge. Studies of localized exciton relaxation indicate that these excitons relax on a much slower timescale than delocalized excitons. The temperature dependence of the localized exciton relaxation rate shows that above 15K, the excitons are thermally activated to extended states above the mobility edge. Below 15K the excitons relax by phonon assisted migration between localization sites. For temperatures above 5K, and for exciton energies greater than 1 meV below line center, an extra dephasing mechanism characterizes the exciton relaxation. The inhomogeneous broadening of the exciton leads to the emission of stimulated photon echoes in the experimental geometry used in this work. The time-resolved emission demonstrates the stimulated photon echo nature at low excitation densities. At higher excitation densities, the decay dynamics is more complex. The time-resolved emission shows the presence of a stimulated photon echo and a free polarization decay. This unusual result suggests that both a homogeneous and an inhomogeneous exciton distribution comprise the exciton resonance. Exciton relaxation at low excitation densities represents the interaction of the exciton with the lattice. At higher excitation densities, exciton-exciton and exciton-free carrier interactions modify the relaxation rates. The dependence of the exciton relaxation rate on excitation density shows that many-body effects play an important role in the exciton physics. Free carrier interactions are more efficient at increasing the exciton relaxation rate; both types of interactions are more important in quantum well systems than in bulk materials.
Picosecond relaxation processes of excitons, including dephasing processes, are systematically studied in CuCl, CdSe and GaAs/AlAs MQW (multi-quantum well structures) by observing time-resolved induced absorption, luminescence and non-degenerate four-wave mixing. By studying the transient induced absorption from the exciton (polariton) state to the excitonic molecule state, time-resolved energy distribution of excitons in CuCl is determined (Fig.1).1) Another technique, i.e. time-resolved luminescence measurement, is applied to excitons in CdSe and GaAs/AlAs MQW (Figs.2 and 3).2,3) By analyzing the above-mentioned experiments the distribution of excitons in the two-dimensional energy-time coordinates is successfully determined. Thus, energy relaxation processes of excitons are clearly visualized. Prior to energy relaxation, coherently generated excitons are considered to be dephased. Phase relaxation of excitons in CuCl is directly measured for the first time in the picosecond time domain by means of time-resolved non-degenerate four-wave mixing (Fig.4).4) These new techniques will be demonstrated and the dephasing as well as energy relaxation mechanism of excitons and excitonic polaritons will be discussed. In the above experiments characteristics of a picosecond tunable optical parametric oscillator pumped by a mode-locked Nd3+:YAG laser as well as a picosecond tunable dye laser synchronously pumped by a mode-locked ion laser are complementarily utilized.
Summary form only given. The optical properties of semiconductor quantum wells (QW) and, in particular, the coherent dynamics of excitons following resonant excitation with ultrafast laser pulses have attracted much attention in recent years. It is generally accepted that there is a transfer of coherence between the optical field and the QW that disappears in a characteristic time T/sub 2/ (picoseconds for GaAs) after the laser is turned off. However, the questions as to how the coherence is actually induced and that of the nature of the coherent state of the solid are poorly understood. In this work we address these points by re-examining the longstanding problem of the (classical vs. quantum) nature of the ubiquitous beats associated with the light-hole (LX) heavy-hole (HX) excitons, which are observed in transient optical experiments on QW. To this end, we consider the coherent behavior of excitons using the simplest albeit non-trivial model where they are treated as non-interacting bosons. Our results bear directly on studies for which nonlinear effects are not important and are not aimed directly at explaining the fourwave-mixing (FWM) experiments that dominate the field. Nevertheless, since nonlinear effects are, typically, weak compared with harmonic contributions, the free boson picture provides in all cases the correct lowest order wavefunction of the photoexcited solid.