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Physical review. B, Condensed matter

Coherent dynamics of radiatively coupled quantum-well excitons

T. Stroucken, A. Knorr, P. Thomas, Stefan W. Koch

Published Jan 15, 1996• 197 citations
Publisher

Abstract

The optical response of radiatively coupled semiconductor multiple-quantum-well structures is investigated theoretically. It is shown that the transverse optical field leads to a coupling of exciton states within each well which causes a radiative decay and a mixing of excitonic resonances. Simultaneously, the field-induced long-ranged coupling between different wells leads to collective effects that are very sensitive to the detailed geometry of the structure. For a quantum-well spacing equal to an integer multiple of half the optical wavelength inside the medium, it is predicted that the collective effects cause a stimulated decay of electronic excitations that should be observable in either transmission or reflection geometry. On the other hand, in a quarter wavelength structure, the light-induced coupling causes an interwell energy transport and a splitting of the excitonic resonances, that should be observable as quantum beats in the time-resolved transmitted or reflected signal.

DOI
10.1103/physrevb.53.2026

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The optical response of radiatively coupled semiconductor multiple-quantum-well structures is investigated theoretically. It is shown that the transverse optical field leads to a coupling of exciton states within each well which causes a radiative decay and a mixing of excitonic resonances. Simultaneously, the field-induced long-ranged coupling between different wells leads to collective effects that are very sensitive to the detailed geometry of the structure. For a quantum-well spacing equal to an integer multiple of half the optical wavelength inside the medium, it is predicted that the collective effects cause a stimulated decay of electronic excitations that should be observable in either transmission or reflection geometry. On the other hand, in a quarter wavelength structure, the light-induced coupling causes an interwell energy transport and a splitting of the excitonic resonances, that should be observable as quantum beats in the time-resolved transmitted or reflected signal.
This dissertation addresses both fundamental aspects of the coherent exciton kinetics in single semiconductor quantum wells and more application-oriented aspects of the collective excitonic optical properties in quantum well Bragg structures. We use a bosonic theory to investigate the ultrafast coherent exciton dynamics after an optical excitation in a single semiconductor quantum well. It is shown that, on intermediate time scales, nonlinear mean-field interactions between excitons lead to a coherent, wave-like evolution in the momentum distribution of optically inactive excitons, which can survive for some time before dephasing sets in. Driven by two-exciton correlations, this coherent quantum kinetic effect bridges the well-known kinetics associated with optical excitation on the one hand and incoherent relaxation on the other. We also study more general dynamical properties of bosonic mean field systems with N-species of excitons (in a single semiconductor quantum well). We find that the momentum-conserving exciton mean field equations, including the coupling to external fields and fermionic corrections, have the dynamical structure su(N,N). We show that one can define a non-real generalized "Bloch vector" and a non-hermitian "density matrix" description, which allow us to explicitly obtain all the constants of motion associated with the su(N,N) symmetry. The many-body effects and correlations of excitons in a single quantum well are mainly induced by the Coulomb interactions. In the case of a semiconductor quantum well Bragg structure, the light induced coupling between different quantum wells also dramatically affects the excitons' behavior, especially through the collective excitations of excitons in the whole structure. We investigate the linear excitonic optical properties of the quantum well Bragg structure induced by the collective excitations using the transfer matrix approach. We show that the so called "intermediate band" (IB) created by the exciton resonance, which does not exist in conventional photonic crystals, can be used for the stopping, storing and releasing of light, which is important in information processing devices. We also discuss the compensation of the dispersive distortion in the light delay process through reversing the IB band structure. Other conceptual and practical issues such as the decay rate of the IB modes and the generalized anti-reflection coating are also investigated.
Time- and spectrally resolved reflectivity measurements on multiple-quantum-well structures excited by ultrashort laser pulses are presented. In Bragg structures, where the interwell distance amounts to half the optical wavelength at the exciton resonance, superradiant coupling of the polarization dynamics within different quantum wells leads to an enhancement of the reflectivity strength and linewidth. We show that the superradiance is not limited to the heavy-hole exciton but can be observed even on excited and light-hole exciton states as well as on correlated electron-hole pair states. These coupling effects grow with the number of quantum wells. For our samples containing 60 and 30 quantum wells, pronounced superradiant enhanced reflectivity is present even at high excitation intensities and high temperatures, showing the insensitivity of radiative coupling with respect to incoherent scattering processes. Our findings are in good agreement with solutions of the semiconductor Maxwell-Bloch equations.
Rapid superradiant decay of coherently excited excitons in thin quantum wells (QWs) on a time scale of approximately 10 ps has been theoretically predicted by several groups [1], however, the experimental observation of this ultrafast radiative recombination is still the subject of controversial discussions. A recent theoretical paper [2] concludes, that this radiative decay rate should be strongly enhanced in multiple QW (MQW) Bragg structures due to radiative coupling of excitons excited in different wells via the exchange of transverse photons.
The influence of radiative coupling on the four-wave-mixing signals of multiple-quantum-well structures is investigated theoretically for excitation at the excitonic resonance. It is shown that amplitude and shape of the FWM signals depend strongly on the number of quantum wells N in the sample and on the periodicity of the structure. For a fixed delay time τ12, the signal amplitude of a Bragg structure increases quadratically with N due to constructive interference as long as the radiative decay rate Nγrad is small compared to the inverse delay time τ—112. For large N, if the enhanced radiative decay rate exceeds the inverse delay time, superradiant emission leads to a decrease of the observed signals with increasing N. The signals of anti-Bragg structures with an odd number of quantum wells decrease with increasing N due to destructive interference effects whereas anti-Bragg structures with an even number of quantum wells behave similarly to Bragg structures.
Summary form only given. Optical interactions in semiconductor microcavities embedded with quantum wells enter a nonperturbative regime when the dipole coupling rate between the exciton and the cavity mode exceeds relevant decay rates. In this regime, coherent energy exchange between the exciton and the cavity mode, i.e. normal mode oscillation (NMO), takes place when the cavity mode is excited impulsively by a short laser pulse. Similar coherent oscillations have also been observed in transient four-wave mixing (FWM) responses. In this paper, we present experimental and theoretical studies on the nature of oscillations in these transient FWM responses. We show that, in contrast to earlier beliefs, oscillations in time-integrated transient FWM do not correspond to NMO of the exciton or photon populations. Theoretical studies further reveal that FWM arising from different physical mechanisms including band filling, excitation-induced dephasing, and renormalized electric fields is characterized by highly distinct coherent dynamics. Oscillations in transient FWM reflect interference between these coherent optical processes and can be used as a unique probe for exciton many-body interactions in the nonperturbative regime.