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Physical review. B, Condensed matter

Optical coherent control in semiconductors: Fringe contrast and inhomogeneous broadening

John Erland, Vadim G. Lyssenko, J. M. Hvam

Published Mar 30, 2001• 27 citations
Publisher

Abstract

Optical coherent control experiments in semiconductors reveal how inhomogeneous broadening must be taken into account in contrast to previous coherent control experiments in atomic and molecular systems. With spectral resolution of the coherent control signal, the optical phases involved in the interplay between the homogeneous and inhomogeneous broadenings are measured. Based on these experiments, a coherent control model describing the optical fringe contrast using different detection schemes, such as photoluminescence or four-wave mixing, is established. Significant spectral modulation is observed in the four-wave mixing spectra as a function of phase-delay representing coherent control in the spectral domain. The spectral phase change of this modulation provides a spectroscopic tool to analyze contributions of inhomogeneous broadening to electronic resonances in semiconductor structures.

DOI
10.1103/physrevb.63.155317

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Optical coherent control experiments in semiconductors reveal how inhomogeneous broadening must be taken into account in contrast to previous coherent control experiments in atomic and molecular systems. With spectral resolution of the coherent control signal, the optical phases involved in the interplay between the homogeneous and inhomogeneous broadenings are measured. Based on these experiments, a coherent control model describing the optical fringe contrast using different detection schemes, such as photoluminescence or four-wave mixing, is established. Significant spectral modulation is observed in the four-wave mixing spectra as a function of phase-delay representing coherent control in the spectral domain. The spectral phase change of this modulation provides a spectroscopic tool to analyze contributions of inhomogeneous broadening to electronic resonances in semiconductor structures.
Summary form only given. The developments with coherent control (CC) techniques in optical spectroscopy have recently demonstrated population control and coherence manipulations when the induced optical phase is explored with phase-locked laser pulses. These and other developments have been guiding the new research field of quantum control including the recent applications to semiconductors and nanostructures. We study the influence of inhomogeneous broadening in semiconductors on CC results. Photoluminescence (PL) and the coherent emission in four-wave mixing (FWM) is recorded after resonant excitation with phase-locked laser pulses. The sample is a narrow GaAs single quantum well.
Abstract The influence of inhomogeneous broadening on results obtained from spectrally resolved transient four‐wave mixing in semiconductors is studied and the homogeneous and inhomogeneous linewidths are simultaneously deduced. Experimental results obtained from the impuritybound exciton I1 in CdSe and the heavy‐hole and light‐hole excitons in GaAs multiple quantum well structures are presented. Furthermore, the case is investigated when more resonances are coherently excited leading to quantum beats.
A new optical effect, the coherent control of spontaneous secondary emission with the participation of optical phonons in systems with discrete spectra of electronic transitions, is studied theoretically. Analytical formulas are obtained that describe the time-integrated signals of secondary emission excited resonantly by a pair of phase-locked pulses in the homogeneously and inhomogeneously broadened systems of semiconductor quantum dots. It is shown that coherent control is a promising method for measuring the total dephasing rates of a resonance optical transition. A physically justified criterion for discriminating between scattering and luminescence in the secondary emission is found. The role of spectral filtering of the signal in the measurements of phase and energy relaxation parameters is elucidated.
Current issues in the study of light-matter interactions are coherence and quantum interference. With ultrafast nonlinear spectroscopy such as transient four-wave mixing (TFWM) the imposed coherence on the optical excitations in e.g. GaAs multiple quantum wells has been studied. In this contribution, we study the influence of inhomogeneous broadening on quantum beats observed by spectrally resolved TFWM. In artificially grown semiconductor structures as e.g. quantum wells, inhomogeneities due to interface-disorder has, up till now, been inevitable. In the experiments, the light-hole exciton (lhx) and the heavy-hole exciton (hhx) in a 100 Å GaAs multiple quantum well are excited simultaneously with 150 fs pulses from a self mode-locked Ti:sapphire laser. The spectral profile is shown in the inset of Fig. 1.
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 detailed theoretical study of the time-integrated signal of spontaneous quasi-elastic secondary emission excited by a pair of phase-locked pulses has shown that coherent control is a promising method for measuring the total dephasing rate of a resonant optical transition. This method may be used to study both the homogeneously and inhomogeneously broadened systems, which is highly important in studies of semiconductor quantum dots. Analysis of components of the secondary emission in the framework of the developed theory has allowed us to find a physically justified criterion for separating the scattering and luminescence signals. The role of spectral filtering of the measured signal in determination of the phase and energy relaxation parameters is elucidated.