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Quantum Electronics and Laser Science Conference

The excitonic Stark effect: absorption splitting and the influence of the light-hole exciton

Sangam Chatterjee, Peter Brick, Claudia Ell, H. M. Gibbs, G. Khitrova, T. Meier, C. Sieh, S. W. Koch

Published Nov 13, 2002• 0 citations
Publisher

Abstract

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.

DOI
10.1109/qels.2001.962058

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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.

•Jan 1, 2001•0 citations
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.
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.
Summary form only given. In the excitonic ac Stark shift in quantum wells the excitonic absorption line is blueshifted by shining on the sample an intense laser pulse, whose frequency is lower than the exciton transition frequency. The effect is bigger when the laser spectrum approaches the resonance with the excitonic absorption. But if the laser and excitonic absorption spectra sensibly overlap, a great amount of electronic population is excited and consequently the Coulomb nonlinearities due to the interaction between excited carries or excitons dramatically increase. One prominent effect under these conditions is the excitation- induced dephasing which can destroy the coherence of the electronic system and therefore the coupling between excitons and light, which is inherently coherent. Some evidence for the resonant Stark effect was already reported, but the direct observation of the spectral splitting was still missing. This observation demonstrates that the coherent exciton light coupling in semiconductors can be strong enough to survive the fast dephasing, and that therefore an efficient ultrafast manipulation of the exciton absorption in the coherent transient is possible. In order to magnify the ac Stark effect and its visibility a special sample was designed: a single In/sub 0.04/Ga/sub 0.96/As quantum well is grown on the top of an AlAs/AlGaAs distributed Bragg reflector; two /spl lambda//2 spacers separate the quantum well from the mirror and from the air. In this configuration the light field incident on the sample and the one reflected by the mirror constructively interfere at the quantum well position, giving a high effective absorption.
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.
We show that a laser beam, tuned in the transparency region of a direct-gap semiconductor, not only shifts but also splits the exciton levels. This splitting originates from the degeneracy of the valence band as the (${\ensuremath{\sigma}}_{+},{\ensuremath{\sigma}}_{\ensuremath{-}}$) parts of the light are not similarly coupled to the various exciton components. In the case of a fourfold-degenerate valence band, we find that, at large detuning, the shifts of the (2\ifmmode\times\else\texttimes\fi{}4) eightfold exciton are exactly the shifts of a (2+4) six-level atom. This is just the generalization of the simple band-structure case with one electron and one hole band in which the large detuning excitonic shift has the same value as that of the two-level (dressed) atom. We give the selection rules to observe the various shifted lines for typical pump-probe experiments. We also discuss the experimental conditions necessary to see an exciton red shift at the two-photon absorption threshold, when the molecular biexciton is stable.
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.
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.