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Physical Review Letters

Quantum Correlations in the Nonperturbative Regime of Semiconductor Microcavities

Claudia Ell, Peter Brick, Matthias Hübner, E. S. Lee, Ove Lyngnes, John P. Prineas, G. Khitrova, H. M. Gibbs, M. Kira, F. Jahnke, S. W. Koch, DENNIS GLENN DEPPE, Diana L. Huffaker

Published Dec 18, 2000• 35 citations
Publisher

Abstract

The nonlinear optical response of semiconductor microcavities in the nonpertubative regime is studied in resonant single-beam-transmission and pump-probe experiments. In both cases a pronounced third transmission peak lying spectrally between the two normal modes is observed. A fully quantized theory is essential for the agreement with the experimental observations, demonstrating that quantum fluctuations leading to intraband polarizations are responsible for this effect.

DOI
10.1103/physrevlett.85.5392

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Coherent optical nonlinearities in semiconductor microstructures

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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
The nonlinear optical response of semiconductor microcavities in the nonpertubative regime is studied in resonant single-beam-transmission and pump-probe experiments. In both cases a pronounced third transmission peak lying spectrally between the two normal modes is observed. A fully quantized theory is essential for the agreement with the experimental observations, demonstrating that quantum fluctuations leading to intraband polarizations are responsible for this effect.
Summary form only given. The nonlinear optical response of semiconductor microcavities in the nonperturbative regime has been the subject of many recent experiments. Contrary to clear demonstrations of the quantized nature of the vacuum-field Rabi splitting of a single atom, most of the experiments on semi-conductor microcavities could be explained in terms of a classical light field. Only recently, quantized light field effects have been reported in a coherent control experiment (Lee et al, 1999) and theoretically investigated in secondary emission (Kira et al, 1999). Here, results are presented that display a pronounced third transmission maximum lying energetically between the two normal modes. The third peak can be observed in resonant femtosecond single-beam as well as picosecond pump-probe experiments under various excitation conditions.
The normal modes in a nonperturbatively coupled quantum-well semiconductor microcavity are linear superpositions of the QW exciton and cavity mode when the QW exciton transition is resonant with the cavity mode. When the lower normal mode is excited by a phase-locked pair of optical pulses, the nonlinear response of a probe pulse tuned to the upper mode is controlled. Thus the normal modes are coupled in their nonlinear optical response due to the nonlinearity of the exciton underlying the two normal modes. The cavity enhancement of the excitonic nonlinearity gives rise to a large signal; modulating the relative phase of the excitation pulses produces a differential reflectivity of up to 10%. Besides the coherent control of normal modes which is explainable with in the frame of semiclassical models, we observe a purely quantum mechanical phenomenon in our system. The quantum correlations between the field and carrier density lead to intraband coherences which live much longer than the interband dephasing time.
A fully quantized theory of optical interactions with semiconductors reveals quantum correlations between the field and carrier density. These quantum correlations lead to intraband coherences which live much longer than the interband dephasing time; the correlations are observed as oscillations in the time-resolved reflectivity in a pump-probe experiment on a normal-mode microcavity. Coherent control of the microcavity normal modes using phase-locked pump pulses enables considerable enhancement of the intraband oscillations due to quantum interference; the detailed phase dependence is well reproduced by the theory.
Summary form only given. The ultrafast nonlinear optical response of semiconductor-microcavities (SMCs) in the nonperturbative regime is attracting growing interest for exploring fundamental light-matter interactions in many-particle quantum systems, as well as for the future implementations of ultrafast photonic devices. In spite of many investigations, the coherent dynamics of excitonic nonlinear-response in the nonperturbative regime has not been fully understood. Open questions are how strong exciton-cavity coupling affects exciton-exciton (X-X) interactions, and how in turn the X-X correlation influences the nonlinear response of SmCs. We investigate these open questions and show that the nonperturbative regime provides an unprecedented tool for investigating four-particle correlations.We start from the equations for the third order exciton polarization and cavity field describing quantum optical effects and coherent nonlinear optics in SMCs, perform the semiclassical factorization and include multiple scattering processes.
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.