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Physical Review Letters

Coherent Control of the Exciton-Biexciton System in an InAs Self-Assembled Quantum Dot Ensemble

Takeshi Suzuki, Rohan Singh, M. Bayer, Arne Ludwig, Andreas Dirk Wieck, Steven T. Cundiff

Published Oct 6, 2016• 42 citations
Publisher

Abstract

Coherent control of a strongly inhomogeneously broadened system, namely, InAs self-assembled quantum dots, is demonstrated. To circumvent the deleterious effects of the inhomogeneous broadening, which usually masks the results of coherent manipulation, we use prepulse two-dimensional coherent spectroscopy to provide a size-selective readout of the ground, exciton, and biexciton states. The dependence on the timing of the prepulse is due to the dynamics of the coherently generated populations. To further validate the results, we performed prepulse polarization dependent measurements and confirmed the behavior expected from selection rules. All measured spectra can be excellently reproduced by solving the optical Bloch equations for a 4-level system.

DOI
10.1103/physrevlett.117.157402

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Coherent control of a strongly inhomogeneously broadened system, namely, InAs self-assembled quantum dots, is demonstrated. To circumvent the deleterious effects of the inhomogeneous broadening, which usually masks the results of coherent manipulation, we use prepulse two-dimensional coherent spectroscopy to provide a size-selective readout of the ground, exciton, and biexciton states. The dependence on the timing of the prepulse is due to the dynamics of the coherently generated populations. To further validate the results, we performed prepulse polarization dependent measurements and confirmed the behavior expected from selection rules. All measured spectra can be excellently reproduced by solving the optical Bloch equations for a 4-level system.
Inhomogeneous broadening in ensembles of semiconductor quantum dots (QDs) has hindered coherent operations due to the detuning effects, caused by the large fluctuation in the QD transition energy due to size dispersion. This difficulty is especially evident when using femtosecond laser pulses for excitation. Here, the authors successfully measure detuning-dependent coherent evolution for a QD ensemble by employing prepulse two-dimensional coherent spectroscopy. The dephasing mechanism is found to be significantly different from that observed using picosecond lasers. This work presents a novel method to explore collective phenomena, such as superfluorescence, as well as motivating future studies of coherent interactions in the femtosecond regime.
The strong confinement of semiconductor excitons in a quantum dot gives rise to atomlike behavior. The full benefit of such a structure is best observed in resonant excitation where the excited state can be deterministically populated and coherently manipulated. Because of the large refractive index and device geometry it remains challenging to observe resonantly excited emission that is free from laser scattering in III/V self-assembled quantum dots. Here we exploit the biexciton binding energy to create an extremely clean single photon source via two-photon resonant excitation of an InAs/GaAs quantum dot. We observe complete suppression of the excitation laser and multiphoton emissions. Additionally, we perform full coherent control of the ground-biexciton state qubit and observe an extended coherence time using an all-optical echo technique. The deterministic coherent photon pair creation makes this system suitable for the generation of time-bin entanglement and experiments on the interaction of photons from dissimilar sources.
We developed a high-resolution Michelson interferometer with a He–Ne two-frequency laser positioning system, and measured the coherent carrier dynamics of a single InAs self-assembled quantum dot (SAQD) using a micro-spectroscopy system. The phase-locked double pulses were stabilized, with the maximum deviation being below 10 nm during the long measurement time of 1 h. Using this system, coherent control of an exciton in an InAs SAQD with very fine phase stabilization was demonstrated. The dephasing time of the single quantum dots was 9.5 ps which is close to that estimated from the homogeneous linewidth in the photoluminescence excitation (PLE) spectrum.
The three-dimensional confinement created by the ultrasmall semiconductor structures known as quantum dots greatly modifies the optical properties of the spatially localized carriers. These systems are presently of great interest to the research community, both for the improved understanding of the physics of confined structures, and for the potential applications of these systems to areas such as optoelectronics and quantum computing. Here, the techniques of transient coherent nonlinear optical spectroscopy are applied to the investigation of excitons confined within InAs/GaAs self-assembled quantum dots. These methods provide a powerful tool for the study of dynamic processes in these novel materials. The nonlinear measurements are based on the differential transmission experimental geometry, and utilize ultrafast pulsed lasers in order to temporally resolve the carrier dynamics after excitation. The experiments performed here are resonant with the ground state absorption of the quantum dots, as evidenced by comparison with the photoluminescence measurements which are used to characterize the sample. The incoherent relaxation dynamics of the population of photoexcited excitons are examined, allowing for a determination of both the lifetime of the excitons and the time scale for relaxation between the two polarization eigenstates of the system. The three-dimensional quantum confinement results in the suppression of these relaxation processes, as predicted. The use of coherent spectroscopic techniques allows for the first unambiguous demonstration of an optically-induced nonradiative Raman coherence in these quantum dots. Simultaneous excitation of both polarization states of the exciton results in a coherent superposition state, whose temporal evolution is observed through the homodyne-detection scheme. In these transient experiments, this is manifested as a beating in the nonlinear response, which allows us to directly measure the fine-structure splitting between the polarization states. Utilizing optical pulse shaping techniques, transient spectral hole burning is performed, which allows for the nonlinear response to be spectrally resolved. As expected for the strongly confined quantum dot excitons, the results show that diffusion among the localized states is not a significant effect. Temperature dependent measurements show that at elevated temperatures, extra dephasing processes, potentially related to acoustic phonon scattering, become important. Finally, this technique allows for the first direct observation of the induced absorption from the exciton to biexciton transition in these InAs quantum dots, and a measurement of the associated binding energy. These results lay the foundation for future studies in this material system, and for the possible development of quantum logic devices utilizing quantum dots.
A detailed understanding of the population and coherence dynamics in optically driven individual emitters in solids and their signatures in ultrafast nonlinear-optical signals is of prime importance for their applications in future quantum and optical technologies. In a combined experimental and theoretical study on exciton complexes in single semiconductor quantum dots we reveal a detailed picture of the dynamics employing three-beam polarization-resolved four-wave mixing (FWM) micro-spectroscopy. The oscillatory dynamics of the FWM signals in the exciton-biexciton system is governed by the fine-structure splitting and the biexciton binding energy in an excellent quantitative agreement between measurement and analytical description. The analysis of the excitation conditions exhibits a dependence of the dynamics on the specific choice of polarization configuration, pulse areas and temporal ordering of driving fields. The interplay between the transitions in the four-level exciton system leads to rich evolution of coherence and population. Using two-dimensional FWM spectroscopy we elucidate the exciton-biexciton coupling and identify neutral and charged exciton complexes in a single quantum dot. Our investigations thus clearly reveal that FWM spectroscopy is a powerful tool to characterize spectral and dynamical properties of single quantum structures.