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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Anomalous photon echoes and Rabi oscillations of quantum dot excitons

Yasuyoshi Mitsumori, Atsushi Hasegawa, Masahide Sasaki, F. Minami

Published Feb 9, 2006• 0 citations
Publisher

Abstract

Optical coherence time and nonlinear optical response of excitons localized to quantum dots in a GaAs/AlGaAs single quantum well are investigated by the three-pulse photon echo technique. At low temperature, the optical coherence time is estimated to be 1.8 ns from the decay curve of the photon echo signal. The decay profile for short time delay shows the strong dependence on the input pulse area of the third pulse. Rabi oscillations are also observed. The oscillations exhibit nonlinear behavior, which is affected by the pre-excited polarization. Such behavior can be qualitatively explained by the local field effect due to the exciton-exciton interaction between the excitons.

DOI
10.1117/12.661395

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Optical coherence time and nonlinear optical response of excitons localized to quantum dots in a GaAs/AlGaAs single quantum well are investigated by the three-pulse photon echo technique. At low temperature, the optical coherence time is estimated to be 1.8 ns from the decay curve of the photon echo signal. The decay profile for short time delay shows the strong dependence on the input pulse area of the third pulse. Rabi oscillations are also observed. The oscillations exhibit nonlinear behavior, which is affected by the pre-excited polarization. Such behavior can be qualitatively explained by the local field effect due to the exciton-exciton interaction between the excitons.
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Nonlinear optical response and optical coherence time of excitons localized to quantum islands in a GaAs∕AlGaAs\mathrm{Ga}\mathrm{As}∕\mathrm{Al}\mathrm{Ga}\mathrm{As}GaAs∕AlGaAs single quantum well are studied by the three-pulse photon echo technique. At low temperature, the optical coherence time is estimated to be 1.8ns1.8\phantom{\rule{0.3em}{0ex}}\mathrm{ns}1.8ns from the decay of the photon echo signal. The decay profile for short time delay shows the strong dependence on the input pulse area of the third pulse. Rabi oscillations are also observed. The oscillations show nonlinear behavior affected by the pre-excited polarization. Such behavior can be qualitatively explained by the local field effect due to the exciton-exciton interaction between the localized excitons.
We experimentally studied the excitonic Rabi oscillations in self-assembled semiconductor quantum dots using two-pulse photon echo spectroscopy. We observed the change in the shape of the Rabi oscillations by the second pulse intensity. Our experimental results were systematically reproduced by numerical calculations taking into account the local field effect arising from the Coulomb interaction between photoinduced charge densities in a quantum dot. Our experimental findings indicated that the local field effect contributes considerably to the coherent optical responses of the excitons in quantum dots.
The polarization dependence of the ultrafast nonlinear response of localized excitons in GaAs/AlGaAs quantum wells has been investigated by spectrally resolved, transient four-wave mixing. The role of the excitation-induced dephasing in the delay dependence of the signal is discussed in detail. In particular, we show experimentally that the excitation-induced dephasing gives rise to a photon echo in inhomogeneous systems. We develop a simple analytical model for the delay dependence of the signal, which enables us to deduce the dephasing time from the four-wave mixing decay.
This work presents new results of experimental studies of exciton relaxation in GaAs/AlGaAs multiple quantum well materials, using transient nonlinear laser spectroscopy techniques. In the low excitation regime, effective optical Bloch equations similar to the density matrix formalism of a two-level system describe the response. Solutions of these equations appropriate for three-pulse scattering studies are presented, along with a discussion of new experimental techniques used in this work. Non-ideal conditions present in the molecular beam epitaxy growth process introduce monolayer fluctuations in the quantum well thickness, leading to inhomogeneous broadening and exciton localization at sites of minimum energy. Localized excitons are separated in energy from extended, quasi-delocalized states by the mobility edge. Studies of localized exciton relaxation indicate that these excitons relax on a much slower timescale than delocalized excitons. The temperature dependence of the localized exciton relaxation rate shows that above 15K, the excitons are thermally activated to extended states above the mobility edge. Below 15K the excitons relax by phonon assisted migration between localization sites. For temperatures above 5K, and for exciton energies greater than 1 meV below line center, an extra dephasing mechanism characterizes the exciton relaxation. The inhomogeneous broadening of the exciton leads to the emission of stimulated photon echoes in the experimental geometry used in this work. The time-resolved emission demonstrates the stimulated photon echo nature at low excitation densities. At higher excitation densities, the decay dynamics is more complex. The time-resolved emission shows the presence of a stimulated photon echo and a free polarization decay. This unusual result suggests that both a homogeneous and an inhomogeneous exciton distribution comprise the exciton resonance. Exciton relaxation at low excitation densities represents the interaction of the exciton with the lattice. At higher excitation densities, exciton-exciton and exciton-free carrier interactions modify the relaxation rates. The dependence of the exciton relaxation rate on excitation density shows that many-body effects play an important role in the exciton physics. Free carrier interactions are more efficient at increasing the exciton relaxation rate; both types of interactions are more important in quantum well systems than in bulk materials.
The nonlinear response of single GaAs quantum dots is studied in femtosecond near-field pump-probe experiments. At negative time delays, transient reflectivity spectra show pronounced oscillatory structure around the quantum dot exciton line, providing the first evidence for a perturbed free induction decay of the excitonic polarization. Phase-disturbing Coulomb interactions between the excitonic polarization and continuum excitations dominate the optical nonlinearity on ultrafast time scales. A theoretical analysis based on the semiconductor Bloch equations accounts for this behavior.