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Conference on Lasers and Electro-Optics

Influence of correlations on intensity dependent excitonic absorption changes

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

Published Aug 29, 2005• 0 citations
Publisher

Abstract

Summary form only given. Polarization dependent excitonic absorption changes have been studied recently for excitation with weak pump pulses. It was shown, that for both resonant and off-resonant excitation even in the low-intensity /spl chi//sup (3)/-limit many-body Coulomb correlations strongly contribute to the optical response. We investigate, how the coherent pump-induced absorption changes vary with the pump intensity by analysing the next higher, i.e. the fifth-order contributions.

DOI
10.1109/iqec.2000.908034

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cond-mat.mes-hallCross-listedarXiv:2512.03198•Dec 4, 2025
Summary form only given. Polarization dependent excitonic absorption changes have been studied recently for excitation with weak pump pulses. It was shown, that for both resonant and off-resonant excitation even in the low-intensity /spl chi//sup (3)/-limit many-body Coulomb correlations strongly contribute to the optical response. We investigate, how the coherent pump-induced absorption changes vary with the pump intensity by analysing the next higher, i.e. the fifth-order contributions.
The intensity dependence of pump-induced excitonic absorption changes is studied in high-quality In0.04Ga0.96As{\mathrm{In}}_{0.04}{\mathrm{Ga}}_{0.96}\mathrm{As}In0.04​Ga0.96​As quantum wells for different detunings and polarization configurations. For resonant excitation with increasing pump intensity a saturation of both the exciton bleaching and the induced absorption due to two-exciton resonances is observed, whereas for pumping below the exciton a characteristic polarization dependence of higher-order contributions to the optical Stark effect is found. Microscopic calculations including Coulomb correlations show that the experimental observations can be described by the coherent dynamics of single- and two-exciton resonances up to fifth order in the optical field.
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.
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.
Summary form only given. The nonlinear optics near the fundamental absorption edge is commonly formulated in terms of a limited number of material parameters characterizing the strength of specific nonlinear processes. Once the nonlinear response function underlying these material parameters is known, one can optimize the relevant nonlinear optical effect for specific device applications. This study is focused on optical nonlinearities at quasi-resonant conditions in the picosecond-pulse regime, where excitonic correlations, such as biexcitonic resonances, contribute prominently to the physical processes. Using a microscopic theory, we have calculated systematically the parameter dependencies of some representative figures of merit, nonlinear phase shift /spl Delta//spl phi/ and differential transmissivity AT, which provide complementary information on the nonlinear susceptibility-/spl chi//sup (3)/:/spl Delta//spl phi//spl sim/Re/spl chi//sup (3)/, /spl Delta/T/spl sim/Im/spl chi//sup (3)/, approximately. We will show in detail how the various aspects of excitonic dynamics affect these quantities around the exciton resonance.
A model study of the characteristic signatures of carrier-correlation effects on the excitonic differential absorption spectra in semiconductors is presented. Using an effectively one-dimensional tight-binding system Coulomb-induced carrier-correlations up to third-order in the optical field are treated without additional approximations. To illustrate the influence of the different many-body contributions excitonic differential absorption spectra are computed for various polarizations and pump-probe time delays. The simultaneous influence of energetic disorder and correlations on the differential absorption spectra is discussed. Also presented are numerical results for the case when the semiconductor system is placed inside a microcavity in the strong-coupling regime. It is shown that the correlations induce characteristic signatures in the normal mode spectra.
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.