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Revue de Physique Appliquée

Subpicosecond excitonic optical nonlinearities in quantum wells

M. Joffre, Daniele Hulin, A. Migus, A. Mysyrowicz, A. Antonetti

Published Jan 1, 1987• 8 citations
Publisher

Abstract

Excitonic resonances in semiconductors are very sensitive to applied optical fields. We present here a comparison between the effects of resonant and non resonant optical excitation, creating respectively real or virtual excitons. A blue shift of the exciton line and a reduction of the oscillator strength are simultaneously observed in multiple-quantum-well-structures for the two following cases : presence of a population of real excitons in very thin wells (two-dimensional systems), or presence of an intense offresonance non absorbed optical field (virtual excitons) independently of the well thickness. The latter configuration (optical Stark effect) has been studied as a function of pump intensity, determining in particular how the saturation of the blue shift is related to the exciton bleaching.

DOI
10.1051/rphysap:0198700220120170500

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Excitonic resonances in semiconductors are very sensitive to applied optical fields. We present here a comparison between the effects of resonant and non resonant optical excitation, creating respectively real or virtual excitons. A blue shift of the exciton line and a reduction of the oscillator strength are simultaneously observed in multiple-quantum-well-structures for the two following cases : presence of a population of real excitons in very thin wells (two-dimensional systems), or presence of an intense offresonance non absorbed optical field (virtual excitons) independently of the well thickness. The latter configuration (optical Stark effect) has been studied as a function of pump intensity, determining in particular how the saturation of the blue shift is related to the exciton bleaching.
This dissertation presents investigations of fundamental optical nonlinearities in semi-conductor microstructures. Two distinct effects are studied. In the first part the excitonic optical Stark effect in InGaAs and GaAs multiple quantum-well structures is investigated by means of pump-probe spectroscopy. For nonresonant excitation below the excitonic transition the direction of the shift of the resonance depends on the polarization of the pump and probe pulses. In particular, for anti-circular polarization a surprising red-shift is observed. For resonant excitation, induced absorption energetically above and below the exciton transition and bleaching of the resonance is found. Experiments using both resonant and nonresonant excitation reveal the importance of bound and unbound two-exciton states in absorption changes of the 1s heavy-hole exciton resonance. It is found that higher-order Coulomb contributions determine the intensity as well as the time dependence of the differential excitonic absorption. In addition, the influence of light-hole excitons is analyzed. It is shown that the direction of the optical Stark shift for nonresonant excitation depends also sensitively on the heavy-hole to light-hole splitting and the detuning of the pump pulse. For very high pump intensities and nonresonant excitation the absorption is split when a circularly polarized pump and a linearly polarized probe beam are used. For co-circular excitation traces of hyper-Raman gain are observed. In the second part of this dissertation, the nonlinear optical response of semiconductor microcavities in the nonperturbative regime is studied in resonant single-beam transmission and pump-probe experiments. In both types of experiment, a pronounced third transmission peak lying spectrally between the two normal modes is observed. Its dependence on the probe intensity, pump intensity, pump-probe delay, exciton-cavity detuning and pump detuning is investigated. For single-beam transmission, the energy of the third peak parallels the position of the cavity resonance. It is more pronounced for circularly polarized excitation and lasts longer than the two normal modes. For pump-probe experiments, the third peak increases with decreasing probe intensity and increasing pump intensity. Its energy is close to the low-energy side of the pump spectrum and virtually unaffected by the cavity-exciton detuning. The appearance of the third peak requires temporal overlap of pump and probe pulses. The origin of this complex nonlinearity is the quantum nature of light, which induces intraband polarizations in the presence of a coherent driving field and a finite carrier density. It is found that the coupling of the intraband polarizations via guided modes to the polarization of the fundamental longitudinal mode is responsible for the third transmission peak. A fully quantized theory reproduces the experimental observations.
Recent works in the area of ultrafast nonlinearities due to virtual carriers in semiconductor heterostructures have generated significant interest among researchers. It has been shown that excitons in QW's behave very much like conventional two-level atoms, to the extent that exciton-exciton interaction can be neglected. Therefore, fast coherent phenomena usually associated with two-level system may occur in excitonic QW transitions. Indeed, dynamic (AC) Stark effect in QW's have been demonstrated. When semiconductor QW's were pumped below the absorption edge there were a strong "blue" shift of the exciton resonance, accompanied by a strong bleaching.
Irradiation of a medium with non-resonant light leads to a shift of the energy levels in the system. This optical, or dynamical Stark effect has been studied for many years in atomic gases. It is only recently, however, that it could be detected for excitonic transitions in solids. This development has stirred considerable interest, because the optical Stark effect has inherent features which makes it well suited for applications such as in ultrafast all-optical data processing. Since the pump light beam falls in a transparency region of the medium, it experiences little loss, in contrast to optical non-linearities based on a saturation mechanism. Also, because virtual transitions are involved, the light-induced shift of exciton levels follows closely the pump pulse duration, making it possible to design ultrafast all-optical logic gates with subpicosecond switch-on and -off times.
The optical Stark effect of excitons in semiconductors, where the exciton resonance is blue shifted by an off-resonance light beam, has been actively studied. Here we report on the observation of a very fast recovery of the exciton bleaching for an off-resonance excitation condition in a quantum well sample at room temperature. The good agreement between the experimental results and our numerical calculations of the time-resolved absorption spectra suggests a coherent transient population buildup and decay occurring on the time scale of the pump pulse.
Summary form only given. Since the original discovery of the excitonic optical Stark effect, substantial progress has been made in the understanding of this ultrafast nonlinear optical effect. Recently, a red shift of the excitonic absorption line has been reported using low intensity excitation detuned 4.5 meV below the 1s-heavy-hole (hh) resonance and cross-circularly-polarized pulses. This was attributed to higher-order Coulomb correlations, interpretable as bound and unbound two-exciton states and memory effects. For co-circularly polarized pulses the well-known blue shift was found. Here we present a related effect occurring in the higher-intensity regime. Standard pump-probe experiments were performed on high-quality 8.5 nm-thick In/sub 0.04/Ga/sub 0.96/As multiple quantum well (MQW) samples.