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Applied Physics Letters

Nonlinear optical absorption and dynamics in quantum wells

Min Jiang, Hailin Wang, Duncan G. Steel

Published Sep 14, 1992• 6 citations
Publisher

Abstract

We present measurements of differential transmission and four-wave mixing in GaAs quantum well structures at 1.8 K near the inhomogeneously broadened lowest heavy-hole (hh1) exciton resonance using narrow band cw excitation. The data show an increase in absorption and an excitation lifetime of order 1–10 μs outside the spectral hole produced by the pump. The long lifetime and the experimentally determined absence of excitation spatial diffusion in this region suggests that optical absorption produces electron-hole pairs that are correlated but separately localized due to disorder. A phenomenological model is proposed to explain the nonlinear response based on two-photon absorption.

DOI
10.1063/1.107572

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We present measurements of differential transmission and four-wave mixing in GaAs quantum well structures at 1.8 K near the inhomogeneously broadened lowest heavy-hole (hh1) exciton resonance using narrow band cw excitation. The data show an increase in absorption and an excitation lifetime of order 1–10 μs outside the spectral hole produced by the pump. The long lifetime and the experimentally determined absence of excitation spatial diffusion in this region suggests that optical absorption produces electron-hole pairs that are correlated but separately localized due to disorder. A phenomenological model is proposed to explain the nonlinear response based on two-photon absorption.
We report high-resolution nonlinear laser-spectroscopy studies of the n=1 heavy-hole exciton in GaAs multiple quantum wells. Using a new method of cw frequency-domain four-wave mixing, we first show that the excitation relaxation consists of both fast and slow components. We then show that the contribution of well-width fluctuations to inhomogeneous broadening can be elimiated enabling us to obtain a direct measure of the intrinsic exciton line shape. Under certain conditions, this line shape is non-Lorentzian and cannot be explained on the basis of simple excited-state relaxation dynamics.
We investigate the spectral properties of the excitonic nonlinear response in a GaAs quantum-well sample containing wells of different thicknesses. We observe both the heavy-hole biexciton and the light-hole biexciton in the transient four-wave mixing spectrum and estimate their binding energy dependence on well width. For moderate excitation densities the signal for negative delay at the heavy-hole exciton and biexciton resonances is due to two-photon transitions to the biexciton states through the exciton states. The temporal behavior of the transient four-wave mixing signal from the heavy-hole exciton resonance is strongly dependent on the spectral position of the laser. We show that this effect is due to interference phenomena and to excitation-induced dephasing.
Recent experimental and theoretical work suggests that excitons in GaAs/AlGaAs multiple quantum wells may be localized by disorder, or delocalized with Bloch-type wavefunctions1. At low temperature, localized excitons are expected to be characterized by spectral diffusion and by long optical coherence times, while delocalized excitons have short coherence times and exhibit spatial mobility2. The short optical coherence time associated with delocalized excitons results in a linear absorption profile that is primarily homogeneously broadened, while the disorder associated with localized excitons leads to an inhomogeneously broadened profile. In this work, we investigate the energy and phase relaxation of HH1 excitons in GaAs/AlGaAs MQW's at low temperature, and provide evidence that, dependent on the exciton density, both localized and delocalized excitons contribute to the nonlinear optical response.
We report high resolution nonlinear laser spectroscopy studies of excitation relaxation associated with the excitonic optical nonlinearity at room temperature and low temperature in GaAs/AlGaAs multiple quantum wells. Using a new method of cw frequency domain four wave mixing, we show that relaxation of the room temperature nonlinear optical response is characterized by free carrier recombination and ambipolar diffusion. At low temperature, the excitation relaxation for localized excitons is dominated by phonon assisted tunneling. In addition, we use four wave mixing methods to eliminate contributions to the excitation line shape from inhomogeneous broadening. The observed line shape is highly asymmetric and shows the presence of spectral diffusion due to the phonon assisted tunneling associated with the excitation relaxation.
Correlated electron-hole pairs, or excitons, in semiconductor nanostructures have been studied extensively over the past few decades. The optical response of excitons is complicated due to inhomogeneous broadening, presence of multiple states, and exciton-exciton interactions. In this work we bring new perspectives to exciton physics in semiconductor quantum wells (QWs) through two-dimensional coherent spectroscopy (2DCS).\nThe effect of QW growth direction on the optical properties of excitons is explored by studying (110)-oriented GaAs QWs. The homogeneous and inhomogeneous linewidths of the heavy-hole exciton resonance are measured. By probing the optical nonlinear response for polarization along the in-plane crystal axes [1-10] and [001], we measure different homogeneous linewidths for the two orthogonal directions. This difference is found to be due to anisotropic excitation-induced dephasing, caused by a crystal-axis-dependent absorption coefficient. The extrapolated zero-excitation density homogeneous linewidth exhibits an activation-like temperature dependence.\nSpectral diffusion of excitons in (001)-oriented QWs has been studied. We show that the spectral diffusion characteristics depend strongly on the sample temperature. Spectral diffusion is generally assumed to follow the strong-redistribution approximation, partly because of lack of any evidence to the contrary. We find that this assumption is violated at low sample temperatures for excitons in QWs; high-energy excitons preferentially relax due to a negligible phonon population at low temperatures. The frequency-frequency correlation function is measured through a numerical fitting procedure to quantify spectral diffusion for sample temperatures >20>20>20 K.\nExciton-exciton interactions affect the light-matter interactions in QWs significantly. We present an intuitive and simple model for these interactions by treating excitons as interacting bosons. We show that the polarization-dependent exciton dephasing rate in GaAs quantum wells is due to the bosonic character of excitons. We fit slices from simulated spectra to those from the experimentally measured spectra and show that interference between two different quantum mechanical pathways results in a slower dephasing rate for co-circular and co-linear polarization of optical excitation pulses. This interference does not exist for cross-linearly polarized excitation pulses resulting in a faster dephasing rate. Additionally, we were able to separately quantify inter- and intra-mode interactions between excitons through exciton-density-dependent measurements.
The nonlinear optical response of quantum well excitons is investigated experimentally using polarization resolved four wave mixing, optical-pump optical-probe, and optical-pump Terahertz-probe spectroscopy. The four-wave mixing data reveal clear signatures of coherent biexcitons which concur with straight-forward polarization selection rules at the Γ point. The type-I samples show the well-established time-domain beating signatures in the transients as well as the corresponding spectral signatures clearly. The latter are also present in type-II samples; however, the smaller exciton and biexciton binding energies in these structures infer longer beating times which, in turn, are accompanied by faster dephasing of the type-II exciton coherences. Furthermore, the THz absorption following spectrally narrow, picosecond excitation at energies in the vicinity of the 1s exciton resonance are discussed. Here, the optical signatures yield the well-established redshifts and blueshifts for the appropriate polarization geometries in type-I quantum well samples also termed “AC Stark Effect”. The THz probe reveals intriguing spectral features which can be ascribed to coherent negative absorption following an excitation into a virtual state for an excitation below the 1s exciton resonance. Furthermore, the scattering and ionization of excitons is discussed for several excitation geometries yielding control rules for elastic and inelastic quasiparticle collisions.