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physica status solidi (b)

Anomalously fast decay of the LH–HH exciton Raman coherence

Cecilia Borca, Amelia G. VanEngen Spivey, Steven T. Cundiff

Published Jul 21, 2003• 4 citations
Publisher

Abstract

Abstract We perform 3‐pulse transient four‐wave‐mixing on a GaAs/AlGaAs multiple quantum well. This allows us to measure both the decay of the Raman coherence between the heavy‐hole and light‐hole excitons and the decay of the respective optical coherences. We observe that the decay rate of the Raman coherence is greater than the sum of decay rates of the optical coherences. This cannot happen within a Markov approximation for the scattering processes, as verified by simulations. The simulations show that such behavior can occur only in the presence of anti‐correlated scattering processes in a non‐Markovian regime.

DOI
10.1002/pssb.200303179

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Abstract We perform 3‐pulse transient four‐wave‐mixing on a GaAs/AlGaAs multiple quantum well. This allows us to measure both the decay of the Raman coherence between the heavy‐hole and light‐hole excitons and the decay of the respective optical coherences. We observe that the decay rate of the Raman coherence is greater than the sum of decay rates of the optical coherences. This cannot happen within a Markov approximation for the scattering processes, as verified by simulations. The simulations show that such behavior can occur only in the presence of anti‐correlated scattering processes in a non‐Markovian regime.
Quantum beats involving the light hole (lh) and heavy hole (hh) excitons in GaAs are observed using homodyne detection of the transient four-wave mixing response. Unlike the beats of earlier studies, these beats are detected in a geometry for which the effect would be forbidden in the absence of exciton interactions and arise from coherence induced between the lh and hh excitons. The beats demonstrate the existence of the Raman coherence due to interaction, and the decay of the coherence shows the correlation of exciton dephasing rates to be relatively unaffected by the interaction.
Three-beam time-integrated transient four-wave mixing (TFWM) is used to probe both light-hole (LH) and heavy-hole (HH) exciton coherences in weakly disordered GaAs quantum wells. The period of the quantum beats between the LH and the HH exciton coherences changes as a function of first-second pulse delay. A theoretical model for the TFWM signal, including exciton dephasing rates that vary with frequency across the inhomogeneous linewidth, reproduces the observations. The inclusion of inhomogeneous dephasing also improves the correspondence between theory and experiment when data as a function of both first-second and second-third pulse delays are simultaneously examined.
Abstract The polarization and population dynamics of resonantly generated excitons in GaAs/AlGaAs quantum well structures are investigated using transient three‐pulse four‐wave mixing. The decay dynamics show strongly nonexponential behavior for both variation of the delay between the first two pulses reflecting the polarization dynamics and variation of the delay between the second two pulses, which reflects the population dynamics. A comparison with a theoretical model shows that the dynamics of both polarization and population are mainly determined by frequency fluctuations and not by scattering processes or by recombination. The characteristic time of the fluctuations TC has to be energy‐dependent to fully describe the results.
We have studied the transient behavior of a sharp emission line, which emerges close to the heavy-hole (hh) exciton photoluminescence line in a 1.6-monolayer-thick InAs layer embedded in a GaAs matrix. The sharp emission line appears under resonant excitation of the light-hole (lh) exciton transition, whose energy separation from the hh exciton transition amounts to one GaAs LO phonon. We have measured the decay time of the sharp emission line in addition to the lifetime of the hh and the lh excitons, using time-correlated single-photon counting and two-wavelength picosecond time-resolved pump–probe transmission techniques. We find that the decay time of the sharp emission line is equal to the lh exciton lifetime for excitation on resonance but that it strongly decreases for excitation off resonance. We conclude that, whereas the sharp line originates from doubly resonant Raman scattering for off-resonant excitation, it is predominantly due to resonant luminescence for resonant excitation. We derive a lh exciton dephasing time of 40 ps, which suggests that the length scale of potential fluctuations from disorder is larger than the lh exciton Bohr radius.
Secondary emission from GaAs quantum wells following resonant pulsed excitation is studied in the time domain. Selective excitation of heavy- and light-hole excitons is accomplished in a two-pulse excitation experiment which preserves sub-ps time resolution. After the initial rise the emission decays exponentially at a fast rate and then with another much slower exponential decay at longer times. The variations in the initial decay times with excitation density and sample temperature are similar to the variation in dephasing rates measured in four-wave mixing experiments. The decay in the visibility of heavy- and light-hole exciton beating is consistent with the decay rates measured for both species separately.