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physica status solidi (a)

Coulomb Memory Effects and Higher-Order Coulomb Correlations in the Excitonic Optical Stark Effect

Peter Brick, Claudia Ell, Matthias Hübner, John P. Prineas, G. Khitrova, H. M. Gibbs, C. Sieh, T. Meier, F. Jahnke, A. Knorr, S. W. Koch

Published Mar 1, 2000• 4 citations
Publisher

Abstract

Differential absorption spectra of high quality InGaAs quantum wells were measured by means of pump–probe spectroscopy as a function of pump–probe delay, for different polarizations of the pulses, and different spectral detunings of the pump beam with respect to the 1s heavy-hole exciton. A clear redshift of the heavy-hole resonance is observed for large detunings and opposite circularly polarized pulses. Microscopic calculations that include not only the Hartree-Fock contribution but also higher-order Coulomb correlations reproduce the experimental findings very well. It is shown that the redshift is caused by Coulomb memory effects and is further enhanced due to the presence of the bound biexciton.

DOI
10.1002/1521-396x(200003)178:1<459::aid-pssa459>3.0.co;2-2

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Differential absorption spectra of high-quality InGaAs quantum wells are presented for various pump detunings and polarization configurations. For low intensity pump pulses tuned well below the exciton a redshift is observed for opposite circularly polarized probe pulses. Microscopic calculations show that this redshift originates from memory effects in the Coulomb-induced excitonic correlations.

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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.

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Signatures of correlations in intensity-dependent excitonic absorption changes

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The intensity dependence of pump-induced excitonic absorption changes is studied in high-quality ${\mathrm{In}}_{0.04}{\mathrm{Ga}}_{0.96}\mathrm{As}$ quantum wells for different detunings and polarization configurations. For resonant excitation with increasing pump intensity a saturation of both the exciton bleaching and the induced absorption due to two-exciton resonances is observed, whereas for pumping below the exciton a characteristic polarization dependence of higher-order contributions to the optical Stark effect is found. Microscopic calculations including Coulomb correlations show that the experimental observations can be described by the coherent dynamics of single- and two-exciton resonances up to fifth order in the optical field.

Physical review. B, Condensed matter•Aug 15, 2000•45 citations
Differential absorption spectra of high quality InGaAs quantum wells were measured by means of pump–probe spectroscopy as a function of pump–probe delay, for different polarizations of the pulses, and different spectral detunings of the pump beam with respect to the 1s heavy-hole exciton. A clear redshift of the heavy-hole resonance is observed for large detunings and opposite circularly polarized pulses. Microscopic calculations that include not only the Hartree-Fock contribution but also higher-order Coulomb correlations reproduce the experimental findings very well. It is shown that the redshift is caused by Coulomb memory effects and is further enhanced due to the presence of the bound biexciton.
Pump-probe experiments on high-quality ${\mathrm{In}}_{x}{\mathrm{Ga}}_{1\ensuremath{-}x}\mathrm{As}$ quantum wells are used to investigate the influence of light-hole excitons on the optical Stark effect. For anticircular polarization of pump and probe pulses and a moderate negative detuning of the pump energy, a redshift of the heavy-hole resonance is observed. However, with increasingly negative detuning a transition from this redshift to a blueshift is found. Microscopic calculations that include both heavy holes and light holes reproduce the experimental results. The theoretical analysis shows that the observation of the redshift depends very sensitively on the detuning of the pump pulses and the heavy-hole to light-hole splitting.
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.
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.
Summary form only given. Recently a lot of interest has been focused on higher-order Coulomb correlations. It was shown, that even in the /spl chi//sup (3)/-limit higher-order excitonic correlations, i.e., bound and unbound two exciton states, influence the coherent optical response. While /spl chi//sup (3)/-contributions to the excitonic Stark effect are well understood, very little is known about the influence of /spl chi//sup (5)/-contributions. Here we investigate the dependence of coherent pump-induced excitonic absorption changes on the pump intensity and relate our results to fifth-order contributions. Pump-probe experiments are performed on high-quality InGaAs quantum wells dominated by a heavy-hole exciton resonance.
The intensity dependence of pump-induced excitonic absorption changes is studied in high-quality In0.04Ga0.96As{\mathrm{In}}_{0.04}{\mathrm{Ga}}_{0.96}\mathrm{As}In0.04​Ga0.96​As quantum wells for different detunings and polarization configurations. For resonant excitation with increasing pump intensity a saturation of both the exciton bleaching and the induced absorption due to two-exciton resonances is observed, whereas for pumping below the exciton a characteristic polarization dependence of higher-order contributions to the optical Stark effect is found. Microscopic calculations including Coulomb correlations show that the experimental observations can be described by the coherent dynamics of single- and two-exciton resonances up to fifth order in the optical field.