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Physical Review Letters

Coherent Control of the Optical Orientation of Excitons in Quantum Wells

X. Marie, P. Le Jeune, Th. Amand, M. Brousseau, J. Barrau, M. Paillard, Richard Planel

Published Oct 27, 1997• 121 citations
Publisher

Abstract

We demonstrate that the optical orientation of excitons can be coherently controlled and directly observed in a resonant time resolved photoluminescence experiment. The optical dephasing time of excitons, their longitudinal and transverse spin relaxation times, and their radiative lifetime, are measured with strictly the same experimental conditions. The measurements rely on the linear response of the crystal.

DOI
10.1103/physrevlett.79.3222

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We demonstrate that the optical orientation of excitons can be coherently controlled and directly observed in a resonant time resolved photoluminescence experiment. The optical dephasing time of excitons, their longitudinal and transverse spin relaxation times, and their radiative lifetime, are measured with strictly the same experimental conditions. The measurements rely on the linear response of the crystal.
Summary form only given. Ultrafast dephasing of excitons in semiconductor quantum wells is important because it presents insight into fundamental interactions and possible coherent control of optical properties. Standard measurement techniques include time- and frequency-domain four-wave mixing, resonant Rayleigh scattering, and Faraday rotation. We report on a new time-resolved technique based on reflective probing of pump-induced transient linear birefringence. This has various advantages, including sensitivity, applicability to opaque as-grown samples, ease of implementation, and freedom from superimposed signals.
Temporal coherent control experiment have been performed on semiconductor quantum well structures, using a sequence of polarized excitation pulses. The oscillatory behaviour of the populations, spin and alignment of the exciton states are observed through the time resolved secondary emission when the time separation between the two excitation pulses is varied. We show that, in specular detection direction, for bare quantum wells at 10 K and low exciton densities, the oscillations amplitude decay is determined by the exciton inhomogeneous broadening. In non-specular detection directions however, when the SE is dominated by resonant Rayleigh scattering, the decay is longer and becomes temperature dependent, which strongly supports that it is now determined by the exciton dephasing time.
Summary form only given. The coherence decay of optically excited electronic systems provides one of the most powerful tools to investigate interaction processes of excited states. In semiconductors, the optical coherence phenomena are usually investigated by nonlinear techniques such as four wave mixing (FWM), photon echo, or reflectivity experiments. Exciton-phonon, exciton-exciton, or exciton-free carriers scattering processes have been explored in recent years with these techniques. As demonstrated recently, a direct measurement of the optical dephasing time can be obtained through the temporal coherent control of electronic excitations. In these experiments, the emission following the excitation by an ultrashort optical pulse sequence, is detected in a non-specular direction (secondary emission). This provides an alternative approach to FWM techniques, which allows us to analyse the scattering processes either with phonons or due to mutual collisions. Using the coherent control technique monitored through the secondary emission (SE), we report on the coherent dynamics of excitons in bare quantum wells (QW) and compare it to that of exciton-polaritons in microcavity (MC) embedded quantum wells.
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.
Resonant photoexcitation of a predominantly homogeneously broadened exciton line in a GaAs quantum well results in a nonexponential time-resolved photoluminescence decay transient due to the decrease in the exciton-exciton scattering contribution to the homogeneous linewidth, ${\mathrm{\ensuremath{\Gamma}}}_{\mathit{h}}$, as the exciton population decays. This result confirms the theoretically predicted relationship between the exciton radiative recombination lifetime and the homogenous linewidth (and coherence area) of the exciton state.