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Hyomen Kagaku

Ultrafast Nonlinear Spectroscopy of Strain-compensated Quantum Dots

Junko Ishi‐Hayase

Published Jan 1, 2011• 0 citations
Publisher

Abstract

We investigate the dephasing mechanism of optically-induced exciton coherence in an ensemble of InAs self-assembled quantum dots (QDs) using a two-pulse photon-echo (PE) technique. The sample was fabricated on an InP (311)B substrate using strain compensation to control the emission wavelength. This technique also enabled us to fabricate a 150-layer stacked QD structure for enhancing the PE signal intensity. We show the measured decay time of PE signal intensity for resonant excitation of ground-state transition is extremely long, which corresponds to ultralong coherence times of excitons in our QDs. We confirmed that non-radiative population relaxation and pure dephasing are considerably smaller than the radiative relaxation at low temperature. Furthermore, we demonstrate the ultrafast coherent control of QD exciton polarization by changing the pulse areas (Rabi oscillations) in the PE experiment. We also propose a new scheme for implementing QD quantum memory by using the PE technique.

DOI
10.1380/jsssj.32.767

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We investigate the dephasing mechanism of optically-induced exciton coherence in an ensemble of InAs self-assembled quantum dots (QDs) using a two-pulse photon-echo (PE) technique. The sample was fabricated on an InP (311)B substrate using strain compensation to control the emission wavelength. This technique also enabled us to fabricate a 150-layer stacked QD structure for enhancing the PE signal intensity. We show the measured decay time of PE signal intensity for resonant excitation of ground-state transition is extremely long, which corresponds to ultralong coherence times of excitons in our QDs. We confirmed that non-radiative population relaxation and pure dephasing are considerably smaller than the radiative relaxation at low temperature. Furthermore, we demonstrate the ultrafast coherent control of QD exciton polarization by changing the pulse areas (Rabi oscillations) in the PE experiment. We also propose a new scheme for implementing QD quantum memory by using the PE technique.
We investigate the dephasing of excitons in InAs self-assembled quantum dots by using a transient four-wave-mixing technique. A used sample is specially designed to compensate the strain. We observe long-lived coherence of excitons at 5 K which corresponds to the dephasing time longer than a nanosecond, where the photon energy of the excitation pulse is 0.874~eV. We find that a pure dephasing due to exciton-phonon interactions dominates in the exciton dephasing rather than the population decay and the exciton-exciton interaction in the weak excitation region, by analyzing the population lifetime and the polarization-dependent dephasing time.
Semiconductor quantum dots are excellent candidates for ultrafast coherent manipulation of qubits by laser pulses on picosecond timescales or even faster. In inhomogeneous ensembles a macroscopic optical polarization decays rapidly due to dephasing, which, however, is reversible in photon echoes carrying complete information about the coherent ensemble dynamics. Control of the echo emission time is mandatory for applications. Here, we propose a novel concept to reach this goal. In a two-pulse photon echo sequence, we apply an additional resonant control pulse with multiple of 2pi area. Depending on its arrival time, the control slows down dephasing or rephasing of the exciton ensemble during its action. We demonstrate for self-assembled (In,Ga)As quantum dots that the photon echo emission time can be retarded or advanced by 5 ps relative to its nominal appearance time without control. This versatile protocol may be used to obtain significantly longer temporal shifts for suitably tailored control pulses.
Abstract In this work femtosecond spectral hole burning spectroscopy is used to resonantly excite ground state excitons in an ensemble of self‐assembled InAs/GaAs quantum dots with a strong pump pulse. Two fundamental coherent nonlinear effects are observed with the aid of the intrinsic time‐ and frequency resolution of the setup: The low temperature Rabi oscillation of the two‐level system associated with the excitonic ground state transition and the observation of two‐photon absorption in the surrounding GaAs crystal matrix. The emergence of the latter effect also infers the existence of charged excitons in the nominally undoped QD sample, backed up by the observation of additional spectral holes next to the excitonic transitions. (© 2009 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)
Abstract Semiconductor quantum dots are excellent candidates for ultrafast coherent manipulation of qubits by laser pulses on picosecond timescales or even faster. In inhomogeneous ensembles a macroscopic optical polarization decays rapidly due to dephasing, which, however, is reversible in photon echoes carrying complete information about the coherent ensemble dynamics. Control of the echo emission time is mandatory for applications. Here, we propose a concept to reach this goal. In a two-pulse photon echo sequence, we apply an additional resonant control pulse with multiple of 2πarea. Depending on its arrival time, the control slows down dephasing or rephasing of the exciton ensemble during its action. We demonstrate for self-assembled (In,Ga)As quantum dots that the photon echo emission time can be retarded or advanced by up to 5 ps relative to its nominal appearance time without control. This versatile protocol may be used to obtain significantly longer temporal shifts for suitably tailored control pulses.
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.
Two quantum control spectroscopic techniques were applied to study InAs quantum dot (QD) devices, which contain different strain-reducing layers. By adaptively control light matter interaction, a delayed resonant response from the InAs QDs was found to be encoded into the optimal phase profile of ultrafast optical pulse used. We verified the delayed resonant response to originate from excitons coupled to acoustic phonons of InAs QDs with two-dimensional coherent spectroscopy. Our study yields valuable dynamical information that can deepen our understanding of the coherent coupling process of exciton in the quantum-confined systems.