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Coherent spectroscopy of single quantum dots

John H. Quilter

Published Dec 4, 2014• 1 citation
OpenAlex

Abstract

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.

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•Aug 18, 2015•0 citations
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.
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.
We demonstrate an approach to realize the population inversion of a single InGaAs/GaAs quantum dot, which is driven by a laser pulse tuned within the neutral exciton phonon sideband. The inversion is achieved by rapid thermalization of the optically dressed states via phonon-assisted relaxation. A maximum exciton population of 0.67 ±\pm± 0.06 is measured for a laser tuned 0.83 meV to higher energy and the phonon sideband is mapped using a two-color pump-probe technique. Our experiments reveal that, in accordance with theory, the phonon-bath provides additional functionality for an optically driven quantum dot qubit.
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.
We demonstrate a new method to realize the population inversion of a single InGaAs=GaAs quantum dot excited by a laser pulse tuned within the neutral exciton phonon sideband.In contrast to the conventional method of inverting a two-level system by performing coherent Rabi oscillation, the inversion is achieved by rapid thermalization of the optically dressed states via incoherent phonon-assisted relaxation.A maximum exciton population of 0.67 Æ 0.06 is measured for a laser tuned 0.83 meV to higher energy.Furthermore, the phonon sideband is mapped using a two-color pump-probe technique, with its spectral form and magnitude in very good agreement with the result of path-integral calculations.
Semiconductor quantum dots have been featured in a number of proposals for quantum computing because of the advantages afforded by confinement on the nanoscale, such as well separated, discrete energy levels and ease of optical manipulation. In addition, they can leverage established semiconductor fabrication techniques and, like the quantum dots used in this work, can be designed to match the telecommunication band, improving the scalability and potential integration of the platform into existing technologies. This thesis work applied optical pulse engineering to manipulate exciton qubits in self-assembled InAs quantum dots. Optimal quantum control theory was used to design pulse shapes that implement high fidelity single-qubit and two-qubit operations, with constraints on the numerical optimization that ensure that the pulses can be accurately implemented using a commercial 4f pulse shaper. In the case of single-qubit operations, the results showed that two uncoupled qubits can be manipulated in parallel using a single phase-shaped laser pulse, provided their optoelectronic properties are sufficiently different. It was demonstrated that targeted differences in inversion and phase between the qubits can be achieved on an ultrafast timescale with high fidelity. In the case of two-qubit operations, the controlled-rotation gate was optimized using amplitude-only and phase-only pulse shaping schemes. The shaped pulses for both schemes were shown to produce higher fidelity operations. The ability to implement robust state inversion on short timescales is particularly useful for technologies such as ultrafast optical switches, single-photon sources, and entangled-photon sources. This work has demonstrated state inversion in a single InAs quantum dot via adiabatic rapid passage using linearly chirped laser pulses. The achieved gate times were an order of magnitude shorter than previous demonstrations. Theoretical predictions of the dependence of the inversion efficiency of the exciton on the sign of the pulse chirp were also verified experimentally, allowing for the identification of phonon-mediated dephasing as the dominant source of decoherence.