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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Coherence and relaxation of excitons in transform-limited time-resolved resonant light-scattering

H. Stolz

Published May 6, 1994• 1 citation
Publisher

Abstract

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.

DOI
10.1117/12.175887

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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.
Summary form only given. After the first observation of resonance scattering from excitons in quantum wells about 1980, this topic has received much interest and has given rise to a hot debate on the origin of this scattering process. Recently, the determination of the temporal behaviour and the coherence properties of this scattering has initiated revival of interferometric techniques in semiconductor optics. Finally, the observation of speckles in the angular distribution proved that this scattering indeed originates from exciton states localized by disorder. However, complementary information on the nature of the excitons and the interplay between scattering and luminescence can be obtained from high resolution cw spectroscopy, having the advantage that only a small fraction of the states within the homogeneous linewidth is excited. However yhe polarization behaviour is quite different for the coherent Rayleigh component and the luminescence, depending on the orientation, splitting and relaxation of the localized states. The experimental results for a 20 nm wide GaAs quantum well clearly confirm this prediction.
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.
The three-dimensional confinement created by the ultrasmall semiconductor structures known as quantum dots greatly modifies the optical properties of the spatially localized carriers. These systems are presently of great interest to the research community, both for the improved understanding of the physics of confined structures, and for the potential applications of these systems to areas such as optoelectronics and quantum computing. Here, the techniques of transient coherent nonlinear optical spectroscopy are applied to the investigation of excitons confined within InAs/GaAs self-assembled quantum dots. These methods provide a powerful tool for the study of dynamic processes in these novel materials. The nonlinear measurements are based on the differential transmission experimental geometry, and utilize ultrafast pulsed lasers in order to temporally resolve the carrier dynamics after excitation. The experiments performed here are resonant with the ground state absorption of the quantum dots, as evidenced by comparison with the photoluminescence measurements which are used to characterize the sample. The incoherent relaxation dynamics of the population of photoexcited excitons are examined, allowing for a determination of both the lifetime of the excitons and the time scale for relaxation between the two polarization eigenstates of the system. The three-dimensional quantum confinement results in the suppression of these relaxation processes, as predicted. The use of coherent spectroscopic techniques allows for the first unambiguous demonstration of an optically-induced nonradiative Raman coherence in these quantum dots. Simultaneous excitation of both polarization states of the exciton results in a coherent superposition state, whose temporal evolution is observed through the homodyne-detection scheme. In these transient experiments, this is manifested as a beating in the nonlinear response, which allows us to directly measure the fine-structure splitting between the polarization states. Utilizing optical pulse shaping techniques, transient spectral hole burning is performed, which allows for the nonlinear response to be spectrally resolved. As expected for the strongly confined quantum dot excitons, the results show that diffusion among the localized states is not a significant effect. Temperature dependent measurements show that at elevated temperatures, extra dephasing processes, potentially related to acoustic phonon scattering, become important. Finally, this technique allows for the first direct observation of the induced absorption from the exciton to biexciton transition in these InAs quantum dots, and a measurement of the associated binding energy. These results lay the foundation for future studies in this material system, and for the possible development of quantum logic devices utilizing quantum dots.
Using laser pulses of duration comparable to semiconductor relaxation and dephasing times, the coherent phenomena common to two-level systems have been demonstrated in II-VI and III-V semiconductors. These light-matter interactions are characterized by electrons and holes in their initially excited states and/or a macroscopic polarization that persists after the excitation. A nonthermal carrier distribution was observed in bulk CdSe, demonstrating the extremely fast energy relaxation possible when carrier-LO-phonon scattering is included. Quantum-confined CdSe microcrystallites were then employed to limit the available decay avenues. The one and two-pair transitions were characterized, and using spectral hole-burning, energy relaxation was shown to be substantially slower than in bulk. Dipole dephasing remained very rapid. Persistent macroscopic polarization was demonstrated in semiconductors through pump and probe experiments conducted on time scales faster than the inverse linewidth of the exciton. In the first set of experiments, it was found that the exciton optical Stark shift deviates from that predicted by a steady-state theory. The shift is smaller than expected and lasts longer than the pump pulse. Both effects are explained by free evolution of the exciton's polarization. Transient exciton bleaching is observed and shown to be a result of adiabatic following. In a second study of coherent polarization, spectral oscillations at negative delay times were studied. Oscillations were measured in a wide variety of semiconductors, temporally preceding several different pump-probe phenomena. By comparison with a semiclassical theory, it was shown that spectral oscillations in the spectral region of the exciton are evidence of persistent exciton polarization. Oscillations in the band are due to four wave mixing of the pump and probe beams.