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Physical Review Letters

Instantaneous frequency dynamics of coherent wave mixing in semiconductor quantum wells

J.‐Y. Bigot, Mary‐Ann Mycek, Shimon Weiss, Rainer G. Ulbrich, D. S. Chemla

Published May 24, 1993• 88 citations
Publisher

Abstract

Using a combination of interferometric-correlation and time-resolved intensity measurement techniques, we characterize the phase and amplitude of the coherent emission of semiconductor quantum wells resonantly excited by ultrashort optical pulses. We demonstrate that exciton-exciton interaction produces nonlinear phase shifts of the instantaneous frequency relative to the incident laser.

DOI
10.1103/physrevlett.70.3307

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Using a combination of interferometric-correlation and time-resolved intensity measurement techniques, we characterize the phase and amplitude of the coherent emission of semiconductor quantum wells resonantly excited by ultrashort optical pulses. We demonstrate that exciton-exciton interaction produces nonlinear phase shifts of the instantaneous frequency relative to the incident laser.
We investigate the temporal evolution of the instantaneous frequency of ultrashort-pulse four-wave mixing in GaAs/Gax{\mathrm{Ga}}_{\mathit{x}}Gax​${\mathrm{Al}}_{1\mathrm{\ensuremath{-}}\mathit{x}}$As quantum-well structures. We find that the coherent light emitted by excitons exhibits a complex phase behavior which depends critically on the density of excitons and the central frequency of the exciting pulses. Depending on the excitation conditions, we observe nonlinear shifts of the instantaneous frequency within one ultrashort pulsed emission or quantum beats. In the latter case we determine that the beat \ensuremath{\pi}-phase shift is very fast, only 40% above the fundamental quantum limit. We also present elaborate numerical simulations of the experiments based on a six-band generalization of the semiconductor Bloch equations. This formalism takes into account Coulomb many-body interactions and Pauli exclusion. It reproduces the salient features of the experimental data. It fails to account for important details revealed by the very sensitive phase measurements. The discrepancies can be traced back to two approximations in the theory: the statical treatment of screening, and the Lorentzian description of dephasing. In both cases, this indicates the need for theoretical refinements requiring a microscopic description of Coulomb scattering and dephasing processes in a non-Markovian theory.
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.
The coherent emission from excitons corresponding to different subband transitions in a 500 Åbroad GaAs/AlGaAs quantum well is studied by spectrally resolved transient four-wave mixing (FWM). For the simultaneous excitation of several subband transitions, the dephasing times of the lowest exciton and higher- order exciton transitions are determined from the width of the resonances in the FWM spectrum. The decay of the spectrally integrated FWM signal as a function of the time delay between the excitation laser pulses does not reflect the dephasing times but is determined by the laser pulse width for multi-subband excitation. This is indicative of quantum interference between exciton and continuum transitions. Many-body Coulomb effects have to be included in a theoretical treatment of these experimental observations.
Coherently controlled four-wave-mixing (FWM) measurements have turned out to be a very sensitive tool to investigate the microscopic origin of the nonlinear optical response of semiconductor quantum-well structures, in particular if excitons are excited [1-3]. The measured signal oscillates as a function of the phase difference of the two interferometric pulses and is modulated additionally by contributions that oscillate with integer multiples of the excitonic resonance frequency. The influence of these harmonics can be measured in background free directions, i.e., the first (FWM) or second (six-wave mixing, SWM) diffracted order in direction 2k2-k1 or 3k2-2k1, respectively. Their intensity is easily quantified by inspecting the corresponding Fourier transforms (FT). Here, we report on transient interferometric SWM measurements and the influence of biexcitons on the signal.
A dual-channel version of spectral interferometry is used to completely characterize the extremely weak ultrashort coherent four wave mixing (FWM) emission from multiple quantum wells (MQWs) by time resolving the polarization state, as well as the scalar amplitude and phase. The amplitudes and the phases of the x and y components of the coherent FWM emission are found to exhibit systematic (but distinct) variations with excitation fluence, time delay between the two incident pulses, detuning of the laser wavelength from the heavy hole (hh) exciton, and the orientation of the input polarizations. From these, a self consistent picture of the temporal dynamics of the amplitude, phase and polarization state is obtained that delineates the roles of many body effects, such as local field corrections, excitation-induced dephasing and biexcitons, in determining the excitonic dynamics.