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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Many-body aspects of excitonic Rabi oscillations in semiconductors

Rolf H. Binder, Maj Lindberg, Axel Schülzgen, M. E. Donavan, Kai Wundke, Hyatt M. Gibbs, G. Khitrova, Nasser N. Peyghambarian

Published Aug 6, 1999• 0 citations
Publisher

Abstract

A theoretical study of excitonic Rabi oscillations in semiconductor quantum wells is presented. Fundamental differences between excitonic Rabi oscillations and optical Rabi oscillations in ideal atomic or molecular 2-level systems are due to the existence of the continuous 1-particle spectrum in solids (energy bands) and the resulting strong effects of the Coulomb interaction, such as the attractive electron-hole interaction and the repulsive exchange interaction. In spite of these fundamental differences, Rabi-like oscillations of the excited electron-hole densities are computed for the case of resonant optical pumping of excitons. We compare our theoretical results with our recent experimental observation of excitonic Rabi oscillations.

DOI
10.1117/12.356946

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An excitonic approach to the ultrafast optical response of confined semiconductors at elevated densities below the Mott transition is presented. The theory is valid from the coherent regime, where coherent excitonic transitions and biexcitons dominate, to the incoherent regime, where excitonic occupations dominate. Numerical simulations of the 1s1s1s exciton dynamics during intense circularly polarized pump pulses in two different Coulomb-interaction regimes are performed for two-dimensional semiconductors: Moderate Coulomb interaction is compared with dominating Coulomb interaction with respect to the light-matter interaction strength. The different many-body contributions are disentangled and it is found, that excitonic Rabi oscillations in the Coulomb-dominated regime are considerably less strong. By also comparing circular and linear excitation in a MoSe2_22​ monolayer, it is found, that linear excitation creates a regime, where excitonic Rabi oscillations are almost completely suppressed.
Data are presented which show eight excitonic density (Rabi) oscillations in an In0.1Ga0.9As/GaAs multiple quantum well at 5 K. Our time resolved, two-color pump-probe experimental technique for observing these oscillations is described. The quantum well sample geometry and linear spectrum are shown along with data characterizing the pump and probe pulses. Experimental data is shown to be in excellent agreement with our theoretical calculation of exciton density versus time, verifying the important affect of the Coulomb interaction between carriers in renormalizing the Rabi frequency. The theoretical calculations include the two-fold degenerate light-hole, heavy-hole, and valence bands in the Hartree-Fock form of the semiconductor Block equations, with all variables selected to conform to the experiment.
We observe multiple excitonic optical Rabi oscillations in a semiconductor quantum well. Up to eight oscillation periods of the heavy-hole exciton density on a subpicosecond time scale are observed. An approximate linear dependence of the oscillation frequency on the light field amplitude is established. The experiment is based on a two-color detection scheme which allows for the observation of the heavy-hole exciton density via transmission changes at the light-hole exciton. The observations are in good agreement with theoretical computations based on multiband semiconductor Bloch equations.
We studied the semiconductor response with respect to high intensity resonant excitation on short-time scale when the contribution of the Fermi statistics of the electrons and holes prevails. We studied both the single- and double-pulse excitations. For the latter case we considered the time evolution of the multiwave mixing exciton polarization. The main difference between the excitation by a single pulse or by two noncollinear pulses is that the Rabi oscillations of the multiwave mixing response are characterized by two harmonics. Analyzing the operator dynamics governed by the external excitation we found that there are three invariant spin classes, which do not mix with the evolution of the system. Two classes correspond to the bright exciton states and one contains all dark states. We found that the dynamics of the classes are described by six frequencies and the Rabi frequencies are only two of them (one for each bright class). We discuss the effect of the dispersion of the electrons and holes and the Coulomb interaction describing the semiconductor by the semiconductor Bloch equation (SBE). We show that if initially the system is in the ground state then the SBE preserves the invariant spin classes, thus proving the absence of the dark excitons in the framework of this description. We found that due to the mass difference between holes of different kind additional Rabi frequencies, two of those present in the operator dynamics should appear in the evolution of the exciton polarization.