A major problem facing the realisation of scalable solid-state quantum computing is that of overcoming decoherence - the process whereby phase information encoded in a qubit is lost as the qubit interacts with its environment. Due to the vast number of environmental degrees of freedom, it is challenging to accurately calculate decoherence times T2, especially when the qubit and environment are highly correlated. Hybrid or mixed electron-nuclear spin qubits, such as donors in silicon, possess 'optimal working points' (OWPs) which are sweet-spots for reduced decoherence in magnetic fields. Analysis of sharp variations of T2 near OWPs was previously based on insensitivity to classical noise, even though hybrid qubits are situated in highly correlated quantum environments, such as the nuclear spin bath of 29Si impurities. This presented limited understanding of the decoherence mechanism and gave unreliable predictions for T2. I present quantum many-body calculations of the qubit-bath dynamics, which (i) yield T2 for hybrid qubits in excellent agreement with experiments in multiple regimes, (ii) elucidate the many-body nature of the nuclear spin bath and (iii) expose significant differences between quantum-bath and classical-field decoherence. To achieve these, the cluster correlation expansion was adapted to include electron-nuclear state mixing. In addition, an analysis supported by experiment was carried out to characterise the nuclear spin bath for a bismuth donor as the hybrid qubit, a simple analytical formula for T2 was derived with predictions in agreement with experiment, and the established method of dynamical decoupling was combined with operating near OWPs in order to maximise T2. Finally, the decoherence of a 29Si spin in proximity to the hybrid qubit was studied, in order to establish the feasibility for its use as a quantum register.
A promising platform for quantum information processing is that of silicon impurities, where the quantum states are manipulated by magnetic resonance. Such systems, in abstraction, can be considered as a nucleus of arbitrary spin coupled to an electron of spin one-half via an isotropic hyperfine interaction. We therefore refer to them as "nuclear-electronic spin systems". The traditional example, being subject to intensive experimental studies, is that of phosphorus doped silicon (Si:P) which couples a spin one-half electron to a nucleus of the same spin, with a hyperfine strength of 117.5 MHz. More recently, bismuth doped silicon (Si:Bi) has been suggested as an alternative instantiation of nuclear-electronic spin systems, differing from Si:P by its larger nuclear spin and hyperfine strength of 9/2 and 1.4754 GHz respectively. The aim of this thesis has been to develop a model that is capable of predicting the magnetic resonance properties of nuclear-electronic spin systems. The theoretical predictions of this model have been tested against experimental data collected on Si:Bi at 4.044 GHz, and have proven quite successful. Furthermore, the larger nuclear spin and hyperfine strength of Si:Bi, compared with that of Si:P, are predicted to offer advantages for quantum information processing. Most notable amongst these is that magnetic field-dependent two-dimensional decoherence free subspaces, called optimal working points, have been identified to exist in Si:Bi, but not Si:P.
Conventional computing faces a huge technical challenge as traditional transistors will soon reach their size limitations. This will halt progress in reaching faster processing speeds and to overcome this problem, require an entirely new approach. Quantum computing (QC) is a natural solution offering a route to miniaturisation by, for example, storing information in electron or nuclear spin states, whilst harnessing the power of quantum physics to perform certain calculations exponentially faster than its classical counterpart. However, QCs face many difficulties, such as, protecting the quantum-bit (qubit) from the environment and its irreversible loss through the process of decoherence.Hybrid systems provide a route to harnessing the benefits of multiple degrees of freedom through the coherent transfer of quantum information between them. In this thesis I show coherent qubit transfer between electron and nuclear spin states in a 15N@C60 molecular system (comprising a nitrogen atom encapsulated in a carbon cage) and a solid state system, using phosphorous donors in silicon (Si:P). The propagation uses a series of resonant mi- crowave and radiofrequency pulses and is shown with a two-way fidelity of around 90% for an arbitrary qubit state. The transfer allows quantum information to be held in the nuclear spin for up to 3 orders of magnitude longer than in the electron spin, producing a 15N@C60 and Si:P ‘quantum memory’ of up to 130 ms and 1.75 s, respectively. I show electron and nuclear spin relaxation (T1), in both systems, is dominated by a two-phonon process resonant with an excited state, with a constant electron/nuclear T1 ratio. The thesis further investigates the decoherence and relaxation properties of metal atoms encapsulated in a carbon cage, termed metallofullerenes, discovering that exceptionally long electron spin decoherence times are possible, such that these can be considered a viable QC candidate.
Nuclear spins in certain solids couple weakly to their environment, making them attractive candidates for quantum information processing and inertial sensing. When coupled to the spin of an optically active electron, nuclear spins can be rapidly polarized, controlled, and read via lasers and radio-frequency (rf) fields. Possessing typical coherence times of several milliseconds at room temperature, nuclear spins hosted by a nitrogen-vacancy center in diamond are thus intriguing systems to observe how classical physical rotation at quantum timescales affects a quantum system. In this work, we demonstrate optical nuclear-spin polarization and rapid quantum control of nuclear spins in a diamond physically rotating at 1kHz, faster than the nuclear-spin coherence time. Free from the need to maintain strict field alignment, we are able to measure and control nuclear spins in the presence of a large, time-varying magnetic field that makes an angle of more than ${100}^{\ensuremath{\circ}}$ to the nitrogen-lattice vacancy axis. The field induces spin mixing between the electron and nuclear states of the qubits, decoupling them from oscillating rf fields. We are able to demonstrate that coherent spin state control is possible at any point of the rotation. We combine continuous dynamical decoupling with feed-forward control to eliminate decoherence induced by imperfect mechanical rotation. Our work liberates a previously inaccessible degree of freedom of the NV nuclear spin, unlocking new approaches to quantum control and rotation sensing.
The nuclear spin state of a phosphorus donor (31P) in isotopically enriched silicon-28 is an excellent host to store quantum information in the solid state. The spin's insensitivity to electric fields yields a solid-state qubit with record coherence times but also renders coupling to other quantum systems very challenging. Here, we describe how to generate a strong electric dipole (>100 D) at microwave frequencies for the nuclear spin. This is achieved by applying a magnetic drive to the spin of the donor-bound electron while simultaneously controlling its charge state with electric fields. Under certain conditions, the microwave magnetic drive also renders the nuclear spin resonance frequency and electric dipole strongly insensitive to electrical noise, yielding long (>1 ms) dephasing times and robust gate operations. The nuclear spin could then be strongly coupled to microwave resonators, with a vacuum Rabi splitting of the order of 1 MHz, or to other nuclear spins, nearly half a micrometer apart, via strong electric dipole-dipole interaction. This work brings the 31P nuclear qubit into the realm of hybrid quantum systems and opens up new avenues in quantum information processing.
Spins localized in semiconductor nanostructures have been intensively investigated for quantum spintronics. These include the spin of single electron localized by quantum dots or impurities, and spins of the lattice nuclei. These localized spins can be exploited as carriers of quantum information, while in some circumstances they also play the role of deleterious noise sources for other quantum objects through their couplings. Quantum control of the spins in semiconductor nanostructures is therefore of central interest for quantum applications. In this thesis, we address several problems related to the quantum control of electron or hole spin and nuclear spins in semiconductor quantum dots and impurity centers. The first problem studied is the control of nuclear spin bath for a hole spin qubit in III-V semiconductor quantum dot. In quantum dots formed on III-V compounds, the direct band gap of the host material allows ultrafast optical addressability of a single electron or hole spin qubit. However, nonzero nuclear spins of group III and group V elements result in a large statistical fluctuation in the Zeeman splitting of the spin qubit which then dephases in nanosecond time scale. We present a novel feedback scheme to suppress the statistical fluctuation of the nuclear spin field for enhancing the coherence time of the hole spin qubit. We also find positive feedback control which can amplify the magnitude of the nuclear field, so that a bimodal distribution can develop, realizing a quantum environment that can not be described by a single temperature. The second problem addressed here is the control of donor spin qubits in silicon architecture which have ultra-long quantum coherence time. We developed the quantum control scheme to realize the quantum metrology of magnetic field gradient, based on the celebrated Kane’s architecture for quantum computation. The scheme can also be generalized to calibrate the locations of the donors. In the third part of the thesis, we investigate a novel type of quantum dot formed in a new class of two-dimensional semiconductors, monolayer transition metal dichalcogenides (TMDs), which exhibit interesting spin and pseudospin physics. This novel quantum dot system may offer new opportunity for quantum spintronics in the ultimate 2D limit, and we investigate here the valley pseudospin as a possible quantum bit carrier. A main finding is that, contrary to the intuition, the lateral confinement by the quantum dot potential does not lead to noticeable valley hybridization, and therefore the valley pseudospin in monolayer TMDs QD can well inherit the valley physics such as the valley optical selection rules from the 2D bulk which implies a variety of quantum control possibilities.