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Ultrafast spectroscopy of single quantum dots

Wolpert, Christian

Published Jan 1, 2012• 0 citations
Publisher

Abstract

In this thesis, the coherent interaction of single semiconductor quantum dots and ultrafast optical pulses is studied. Under certain conditions, localized exciton transitions in quantum dots can be seen as semi-isolated two-level systems. While this description is sufficient for the explanation of some observations in coherent experiments, it is sometimes necessary to explicitly consider coupling of the discreet quantum states confined to the dot with the environment. We start out from simple, classical examples of coherent spectroscopy and then turn towards experiments where the interaction with the vicinity of the dot becomes an important factor. First, a novel method for transient differential reflectivity spectroscopy of single quantum systems is introduced. It is a pure far-field optical technique which does not require any sophisticated sample preparation steps which makes it applicable to a broad range of structures. Pump pulses excite the sample structure and probe pulses read out the pump-induced changes in the system after a variable delay time. In the case of a single dipole, the signal is given in the form of the spectral inteferogram between the backscattered wave from the particle and the probe light which is reflected at the sample surface. This form of homodyne detection amplifies the weak scattered wave from the particle and thus makes this kind of spectroscopy for single quantum dots feasible. In the remainder of this thesis our spectroscopic method is applied to either characterize the coherent properties of single quantum dots, to prepare and read-out a desired quantum state or to deliberately manipulate them. Coherence times and oscillator strengths are determined for localized exciton transitions. Arbitrary population states can be written by driving coherent population oscillations using resonant pulses, while entangled superpositions of two exciton states in a single dot are investigated by quantum beats on transient differential spectra. We finally exploit the interaction between the dot and a nearby absorbing layer to switch the dot's absorption spectrum on ultrafast timescales via light-induced transient electric fields.

DOI
10.18419/opus-6798

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In this thesis, the coherent interaction of single semiconductor quantum dots and ultrafast optical pulses is studied. Under certain conditions, localized exciton transitions in quantum dots can be seen as semi-isolated two-level systems. While this description is sufficient for the explanation of some observations in coherent experiments, it is sometimes necessary to explicitly consider coupling of the discreet quantum states confined to the dot with the environment. We start out from simple, classical examples of coherent spectroscopy and then turn towards experiments where the interaction with the vicinity of the dot becomes an important factor. First, a novel method for transient differential reflectivity spectroscopy of single quantum systems is introduced. It is a pure far-field optical technique which does not require any sophisticated sample preparation steps which makes it applicable to a broad range of structures. Pump pulses excite the sample structure and probe pulses read out the pump-induced changes in the system after a variable delay time. In the case of a single dipole, the signal is given in the form of the spectral inteferogram between the backscattered wave from the particle and the probe light which is reflected at the sample surface. This form of homodyne detection amplifies the weak scattered wave from the particle and thus makes this kind of spectroscopy for single quantum dots feasible. In the remainder of this thesis our spectroscopic method is applied to either characterize the coherent properties of single quantum dots, to prepare and read-out a desired quantum state or to deliberately manipulate them. Coherence times and oscillator strengths are determined for localized exciton transitions. Arbitrary population states can be written by driving coherent population oscillations using resonant pulses, while entangled superpositions of two exciton states in a single dot are investigated by quantum beats on transient differential spectra. We finally exploit the interaction between the dot and a nearby absorbing layer to switch the dot's absorption spectrum on ultrafast timescales via light-induced transient electric fields.
The focus of the thesis is nonlinear transient optical properties and coherent control of single interface fluctuation quantum dots (QD's). When single exciton and biexciton resonances were driven by strong resonant laser pulses, Rabi oscillations of these transitions were observed in the differential transmission (DT) geometry. These results extend the concept of coherent control to the limit of single quantum confined systems in solids and have important implications for the feasibility of building quantum information processing devices using semiconductor QD's. Exciton Rabi oscillations are equivalent to arbitrary single-bit operations. The pulsed control of the exciton-biexciton transition is utilized as the optical operation for building a two-bit controlled rotational gates (CROT) in a single QD. A fidelity of 0.79 was obtained from numerical evaluation of the gate operation itself assuming typical decay parameters measured from these dots. Next, the nonradiative quantum coherence between two orthogonally polarized excitons confined in a single QD was studied. By using pulses with large enough bandwidth and the proper polarization, two exciton states are simultaneously excited. The quantum beats between the two exciton states were temporally resolved as the relative phase between the two dipole oscillations changed. It was found that the nonradiative coherence time is limited by the lifetimes of the excitons involved even in the strong field regime. In the basis of the pseudo-spin Bloch vectors of exciton transitions, the total wavefunction following the pulsed excitation is an entangled state, i.e. the wavefunction is non-factorizable. Finally, the quantum coherence between the biexciton, exciton, and the crystal ground states was studied in a novel quantum beat experiment, where the oscillations only existed when the pump and probe pulses overlapped in time. Laser pulses generated after a passive pulse shaper with just enough bandwidth to cover both the exciton and biexciton transitions were used in this experiment. The appearance of the beats is indicative of a reasonably long coherence time between the biexciton and other states even in the presence of strong pulsed excitations.
Excitons in quantum dots represent a remarkably good two-level system with a large optical dipole transition moment. Although most research currently focuses on enhancing their already outstanding properties as single photon emitters they become also increasingly interesting for experimental fundamental research due to their large dipole transition moment. This thesis presents studies which explore fundamental phenomena in quantum dots using coherent spectrocopy methods. First, we will first examine the optical properties of site-controlled quantum dots which were grown using a buried stressor via resonance fluorescence. Subsequently, we will show results that were obtained using photocurrent spectroscopy to study single quantum dots that are embedded in micropillar resonators. This is followed by a study of the Wigner time delay induced by a single quantum dot and which shows that the maximum delay is larger than its dephasing time T2 which is the theoretical limit for coherently scattered fraction. The next section demonstrates that the response of a resonantly driven two-level system which in our case is represented by an exciton in a seminconductor quantum dot depends significantly on the photon statistics of the exciting light field. Most strikingly, the Mollow triplet which we observe under coherent excitation vanishes under thermal excitation. The second part presents results concerned with the resonantly driven biexciton cascade via two- photon excitation. The coherent interaction between light field and excitons gives rise to a complex five-level system. Here, we show for the first time two-photon Rabi oscillations in the temporal domain. Furthermore, we examine the correlations between the different transitions. The measurements show that we can manipulate the time-ordering of the emitted photons by changing for example the laser power. All these studies share the resonant excitation scheme which allows for a coherent manipulation of the states of the quantum dot and grants access to phenomena typical for resonance fluorescence such as the Mollow triplet and Rabi oscillations. In particular the experiments on photon excitation spectroscopy and the studies on the dressed biexciton cascade show that fundamental effects of quantum optics can be explored in a scalable and application oriented setting using quantum dots.
Quantum dots have been the focus of both fundamental and applied research due to their atomic-like properties. The delta-function-like density of states along with strong nonlinear optical properties have made quantum dots the focus of novel opto-electronic devices and of quantum computing proposals. The key issue for implementing quantum dots in devices such as quantum computers is the ability to coherently entangle separately localized quantum dot states. Using continuous wave coherent nonlinear optical spectroscopy techniques, this thesis focuses on creating coherent super-position states built from separately localized quantum dot states. The narrow bandwidths and mutual coherence of the applied laser fields allow for the creation of radiative and nonradiative coherences which can be understood from the coherent nonlinear optical response. The quantum dots under study are formed due to the width fluctuations of a thin quantum well. By applying nondegenerate mutually coherent fields on the sample in the traditional pump and probe geometry and homodyne detecting the nonlinear signal field, nonradiative coherences between two laterally coupled quantum dots are created and the coupling between their states examined. The coherent nonlinear optical response is compared with theoretical predictions based on the density matrix formalism for the interacting two exciton model. From this comparison, binding energies of the two-exciton bound state created with separately localized excitons is found to be on the order of 20 mueV for like-polarized excitons and on the order of 100 mueV for unlike-polarized excitons. A second order coherence between the ground and two-exciton state is also noted in the experimental data after comparison with theory. Further work attempting to study a vertically coupled quantum dot system was unsuccessful. The spectrum of a quantum dot is further understood from the comparison of the linear and nonlinear excited state spectra. Excited states which appear in both spectra imply a Coulomb interaction between them and their respective ground states. Coherent nonlinear optical signatures of excited states correlated with their linear excitation spectra are presented, and the importance of such states for a quantum computer read-out is described.
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.
This thesis presents experiments carried out into the coherent properties of charge carriers confined within a single InGaAs/GaAs quantum dot. Specifically the ground state - single exciton qubit system is controlled with ultrafast optical pulses and then the population of the dot is measured by a high-sensitivity photocurrent detection technique. There are two principal results of these experiments, firstly by modulating the bias applied to the quantum dot diode, the detection efficiency of the photocurrent measurement technique is enhanced. The enhancement is possible as the modulated bias allows fast switching of the voltage-dependent carrier tunneling rates. Secondly, when the transition is addressed by an intense, positively detuned laser, the qubit system can be driven to a population inversion. This occurs due to phonon-assisted relaxation of the optical dressed states of the system. Here, the rapid thermalization due to the exciton-phonon interaction actually enables the population inversion, instead of simply being a source of decoherence.
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.