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arXiv:cond-mat/9910157 · Physical Review Letters

Collective Oscillations Driven by Correlation in the Nonlinear Optical Regime

Th. Östreich, Lu Jeu Sham

Published Oct 25, 1999• 31 citations
arXivHTMLPDF

Abstract

We present an analytical and numerical study of the coherent exciton polarization including exciton-exciton correlation. The time evolution after excitation with ultrashort optical pulses can be divided into a slowly varying polarization component and novel ultrafast collective modes. The frequency and damping of the collective modes are determined by the high-frequency properties of the retarded two-exciton correlation function, which includes Coulomb effects beyond the mean-field approximation. The overall time evolution depends on the low-frequency spectral behavior. The collective mode, well separated from the slower coherent density evolution, manifests itself in the coherent emission of a resonantly excited excitonic system, as demonstrated numerically.

DOI
10.1103/physrevlett.83.3510

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We present an analytical and numerical study of the coherent exciton polarization including exciton-exciton correlation. The time evolution after excitation with ultrashort optical pulses can be divided into a slowly varying polarization component and novel ultrafast collective modes. The frequency and damping of the collective modes are determined by the high-frequency properties of the retarded two-exciton correlation function, which includes Coulomb effects beyond the mean-field approximation. The overall time evolution depends on the low-frequency spectral behavior. The collective mode, well separated from the slower coherent density evolution, manifests itself in the coherent emission of a resonantly excited excitonic system, as demonstrated numerically.
The paper presents a description of two-pair correlations in an electron-hole system in laser-excited direct-gap semiconductors in terms of the exciton-boson formalism. The dependence of the states of quasi-particles on their angular momentum orientation is properly taken into account following group theory rules. It is shown for the example of heavy hole excitons in GaAs quantum wells that Coulomb two-exciton correlations include effective repulsion between excitons with nonzero total momenta and effective attraction between excitons with zero total momenta. They generate exciton and biexciton nonlinearities, respectively, in the exciton-biexciton system. The Heisenberg equations of motion derived are applied to four-wave mixing in the coherent mode. Two components of Coulomb two-exciton correlations were found to generate coherent four-wave mixing either separately, one at the cocircular and the other at the perpendicular-linear polarization of applied pulses, or jointly at parallel-linear polarization. General equations are obtained for the amplitude of four-wave mixing signals with time resolution in these polarization configurations, which, in the limit of ultranarrow pulses, reduce to analytic functions of time and excitation and sample parameters. These equations are used to analyze signal characteristics in every polarization configuration. The results give a correct picture of biexciton effects and the polarization dependence of coherent four-wave mixing in GaAs quantum wells.
Summary form only given. Large-radius excitons in semiconductors suffer strong Coulomb interaction on close approach. This is a distinctive difference in comparison with two-level systems in quantum optics. A mean field theory of interacting excitons in semiconductors leads to purely repulsive interaction, and does not account for spin-dependent polarization mixing and the formation of excitonic molecules (biexcitons). We have developed a theory for the nonlinear optical response, which can account for both. The coherent polarization is driven by exciton-exciton correlation, which can be expressed in terms of spin-dependent retarded memory functions. The effective equation is a generalized Gross-Pitaevskii equation.
We report on the observation of coherent secondary emission from resonantly excited bound and unbound two-exciton states in quantum wells. The emission is intrinsic, in contrast to the well-known Rayleigh scattering from excitons that requires disorder. We measure the spectral amplitude and the phase (and, hence, the femtosecond dynamics) of this coherent emission using ultrafast spectral interferometry, and obtain direct information on the contributions to the nonlinear susceptibility from exciton-exciton correlations beyond the mean-field approximation.
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.
We study the time evolution of excitonic states after photoexcitation in the one-dimensional spinless extended Falicov-Kimball model. Several numerical methods are employed and benchmarked against each other: time-dependent mean-field simulations, the second-Born approximation (2BA) within the Kadanoff-Baym formalism, the generalized Kadanoff-Baym ansatz (GKBA) implemented with the 2BA, and the infinite time-evolving block decimation (iTEBD) method. It is found that the GKBA gives the best agreement with iTEBD and captures the relevant physics. Excitations to the particle-hole continuum and resonant excitations of the equilibrium exciton result in a qualitatively different dynamics. In the former case, the exciton binding energy remains positive and the frequency of the corresponding coherent oscillations is smaller than the band gap. On the other hand, resonant excitations trigger a collective mode whose frequency is larger than the band gap. We discuss the origin of these different behaviors by evaluating the nonequilibrium susceptibility using the nonthermal distribution and a random phase approximation. The peculiar mode with frequency larger than the band gap is associated with a partial population inversion with a sharp energy cutoff. We also discuss the effects of the cooling by a phonon bath. We demonstrate the real-time development of coherence in the polarization, which indicates excitonic condensation out of equilibrium.
We demonstrate the presence of strong exciton-exciton correlations in GaAs-AlGaAs multiple quantum wells by using the polarization selection rules for four-wave mixing and a test that was originally designed to distinguish between quantum beats and polarization interference. We show that, when the four-wave-mixing signal is produced by two pulses that have the same circular polarization, dynamic beating behavior is observed at the heavy-hole-light-hole frequency that provides evidence of Coulomb-induced correlations that go beyond those expected from the semiconductor Bloch equations in the Hartree-Fock approximation and beyond the local field corrections used in simple phenomenological models. Moreover, this behavior cannot be explained by invoking biexcitonic effects. We demonstrate that this dynamic excitonic coupling can be explained in terms of a competition between quantum-beat-like and polarization-interference-like behavior, and we show that such behavior can be used to place quantitative limits on the coupling strength. In addition, we use a simple phenomenological model to show that excitation-induced-dephasing can produce such correlations.