Controlling the quantum states of charge (excitons) or spin-polarized carriers in semiconductor quantum dots (QDs) has been the focus of a considerable research effort in recent years due to the strong promise of using this approach to develop solid state quantum computing hardware. The long-term scalability of this type of quantum computing architecture is enhanced by the use of QDs emitting in the telecom band, which would exploit the established photonic infrastructure. This thesis reports the use of all optical infrared experimental techniques to control exciton dynamics in two different QD samples consisting of InAs/GaAs QDs and InAs/InP QDs within a planar microcavity. An infrared quantum control apparatus was developed and used to apply optimized shaping masks to ultrafast pulses from an optical parametric oscillator. Pulse shaping protocols designed to execute a two-qubit controlled-rotation operation on an individual semiconductor QD were demonstrated and characterized. The quantum control apparatus was then implemented in simultaneous single qubit rotations using two uncoupled, distant InAs/GaAs QDs. These optimal control experiments demonstrated high fidelity optical manipulation of exciton states in the two QDs using a single broadband laser pulse, representing a step forward on the path to a scalable QD architecture and showcasing the power of pulse shaping techniques for quantum control on solid state qubits. As an alternative to single QDs, which have very low optical signals, subsets of QDs within an ensemble can be used in quantum computing applications. To investigate the mediation of inhomogeneities in a QD ensemble, pump-probe experiments were performed on InAs/InP QDs within a dielectric Bragg stack microcavity. Two different excitation geometries showed that the angle dependence of the microcavity transmission allowed for the spectral selection of QD subsets with transition energies resonant with the cavity mode. The microcavity mitigated inhomogeneities in the ensemble while providing a basis for addressing QD subsets which could be used as distinguishable quantum bits. This thesis work shows significant advances towards an optical computing architecture using quantum states in semiconductor QDs.
Controlling the quantum states of charge (excitons) or spin-polarized carriers in semiconductor quantum dots (QDs) has been the focus of a considerable research effort in recent years due to the strong promise of using this approach to develop solid state quantum computing hardware. The long-term scalability of this type of quantum computing architecture is enhanced by the use of QDs emitting in the telecom band, which would exploit the established photonic infrastructure. This thesis reports the use of all optical infrared experimental techniques to control exciton dynamics in two different QD samples consisting of InAs/GaAs QDs and InAs/InP QDs within a planar microcavity. An infrared quantum control apparatus was developed and used to apply optimized shaping masks to ultrafast pulses from an optical parametric oscillator. Pulse shaping protocols designed to execute a two-qubit controlled-rotation operation on an individual semiconductor QD were demonstrated and characterized. The quantum control apparatus was then implemented in simultaneous single qubit rotations using two uncoupled, distant InAs/GaAs QDs. These optimal control experiments demonstrated high fidelity optical manipulation of exciton states in the two QDs using a single broadband laser pulse, representing a step forward on the path to a scalable QD architecture and showcasing the power of pulse shaping techniques for quantum control on solid state qubits. As an alternative to single QDs, which have very low optical signals, subsets of QDs within an ensemble can be used in quantum computing applications. To investigate the mediation of inhomogeneities in a QD ensemble, pump-probe experiments were performed on InAs/InP QDs within a dielectric Bragg stack microcavity. Two different excitation geometries showed that the angle dependence of the microcavity transmission allowed for the spectral selection of QD subsets with transition energies resonant with the cavity mode. The microcavity mitigated inhomogeneities in the ensemble while providing a basis for addressing QD subsets which could be used as distinguishable quantum bits. This thesis work shows significant advances towards an optical computing architecture using quantum states in semiconductor QDs.
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.
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.
Self-assembled quantum dots (QDs) containing a single electron are one of the leading candidate systems for the realization of a quantum computer. The spin states of charges confined in these dots have been shown to possess a number of qualities that are attractive for use as the quantum bits (qubits) in quantum computing implementations, particularly their long lifetimes and coherence times. In addition, these spin qubits may be controlled optically, offering the prospect of ultrafast qubit gate operations, a crucial necessity for the execution of quantum algorithms. Due to the weak interaction of self-assembled QDs with light, however, the coherent optical control and read-out of the spin states of charged self-assembled QDs has proven to be a considerable challenge. This thesis presents two sets of experiments demonstrating the coherent optical control and read-out of the quantum states of a self-assembled InAs QD containing a single electron. The first utilizes mode-locked picosecond optical pulses to control the optical transitions in the dot and to detect QD level occupations. These capabilities are used to observe transient phenomena in a singly charged InAs QD such as the generation and decay of excited state population and spin precession. Further, Rabi oscillations between the electron and the lowest-lying excited state are observed, demonstrating the ability to coherently control the optical transitions of the QD, a prerequisite for spin control. These results are built upon in the second set of experiments, in which a combination of optical pulses, an externally applied DC magnetic field and a continuous-wave (CW) optical field are employed to initialize and completely control the states of a QD confined electron spin. Spin control by the use of pulse-driven two-photon Raman processes, spin precession about the external magnetic field and geometric phases generated by CW-driven cyclic evolutions in the dot is demonstrated. A number of spin qubit gate operations are shown for these spin control mechanisms, forming a foundational set of single qubit gates required for the implementation of quantum computing with singly charged self-assembled QDs.
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.
Shaped ultrafast pulses designed for controlled-rotation (C-ROT) operations on exciton qubits in semiconductor quantum dots are demonstrated using a quantum control apparatus operating at ∼1 eV. Optimum pulse shapes employing amplitude and phase shaping protocols are implemented using the output of an optical parametric oscillator and a programmable pulse shaping system, and characterized using autocorrelation and multiphoton intrapulse interference phase scan techniques. We apply our pulse characterization results and density matrix simulations to assess the fundamental limits on the fidelity of the C-ROT operation, providing a benchmark for the evaluation of sources of noise in other quantum control experiments. Our results indicate the effectiveness of pulse shaping techniques for achieving high fidelity quantum operations in quantum dots with a gate time below 1 ps.
Coherent optically driven semiconductor quantum dot systems are proposed for the implementation of quantum information processing devices. Fundamental quantum computation units, the quantum bits (qubits), are realized and optically manipulated in the exciton and spin bases. In this thesis, consecutive phase-sensitive rotations of a single qubit and their importance in the measurement of the full physical density matrix have been demonstrated experimentally in the exciton system in neutral GaAs/Al0:3Ga0:7As interface fluctuation quantum dots. The experimental work done on the exciton system serves as a foundation for consequent work on the long coherence lifetime spin-based qubits in charged quantum dots. In the spin-based system in the charged GaAs/Al0:3Ga0:7As interface fluctuation quantum dots, we demonstrate the selective excitation from the two spin ground states to the charged exciton (trion) state through phase sensitive control of the spin coherence in an ensemble of three-level spin-trion Lambda systems. This controlled excitation utilized the optically coupled and decoupled states of the electron spin in the presence of coherent transient excitation of the spin ground states in singly charged quantum dots. This progress lays the ground work for achieving complete ultrafast spin rotations.