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An explanation for the quantum-to-classical transition has long been sought after since the haydays of the field. Decoherence theory and open quantum system dynamics have paved the way, showing how a system can become correlated with, and so lose information into the environment. Quantum Darwinism, and its more stringent cousins Strong Quantum Darwinism and Spectrum Broadcast Structures, seek to explain how this information loss is achieved in such a way as to be objective, classical and redundant. However there remains questions as to how the structure of the environment, states and types of interactions can give rise to this redundant encoding. In this thesis, we collect the work of 3 of our papers, exploring these questions. First, we show how information from one environment can spread to another. Then we show how commutativity can play a role in the emergence of objectivity. Lastly, we move beyond a single, pure system to a more realistic bipartite one, with both classical and quantum correlations between the subsystems. We shall show how interactions between only these subsystems can mediate the redundancy of others, and how these can lower bound and upper bound other forms of interactions between said subsystems and the environment.

It is widely accepted that the most emblematic quantity of quantum mechanics, the wavefunction, is the successful tool for making accurate predictions about experimental results. However, the physical meaning of the wavefunction has been a subject of debates since the birth of the theory. A popular dilemma has to do with the question of whether a pure quantum state is an observer-dependent-quantity/a state-of-knowledge, such as probabilities and density operators, or otherwise if it is something (characterised as) real. Reasons why this debate is important include resolutions of the wavefunction collapse mechanism as well as of potential conflicts between quantum mechanics and special relativity. Physicists have had opinions on this dilemma based on intuitions, interpretations or philosophy. But in the recent years, the community of quantum foundations has been equipped with theorems -known as ψ-ontology theorems- that answer this dilemma rigorously. As always, the "advantage" of a theorem is that it comes with a proof and the "disadvantage" that it comes with assumptions. The common ground among all ψ-ontology theorems is that they work within the framework of underlying models. In a previous work R. Colbeck and R. Renner constructed a theorem concluded that a quantum state is not a state-of-knowledge about an underlying physical state. A core assumption behind their proof was that the inputs used for a chained Bell test were uncorrelated with all the variables of the setup that are not caused by them. This free-choice definition of them implies no-conspiracy and parameter-independence (in Bell's theorem terms), and actually, the two latter were the strictly necessary for their proof. At the first part of this thesis we relax these assumptions and we test the robustness of the theorem's conclusion. First, regarding no-conspiracy relaxation, we allow the inputs to be correlated with the underlying variables and through a randomness amplification technique we show that there exist conditions under which the original theorem's conclusion still holds. The situation is different regarding parameter-dependence embedding, since their proof turns out to be unreceptive to it. Under this evidence, we discuss a particular toy underlying model as a counterexample explaining at least why our intended parameter-independence relaxation would be impossible to reach the maximum parameter-dependence strength. Non-signalling correlations play a central role in the next parts of the thesis. The realisation by the community that correlations stronger than any quantum ones, can still be non-signalling, created two -among plenty- broad research programs. Since the non-signalling principle cannot single out quantum correlations, is there any other physical axiom managing so? And, when it comes to performing information-processing tasks, how quantum theory competes with other possible non-signalling theories? Nonlocality distillation, that covers the second part of the thesis, is an absolute "ally" of the earliest aforementioned axiomatization realm. This is because there are correlations that do not violate "at first sight" information-theoretic axioms (such as non-trivial communication complexity, information-causality etc), but they do so after they undergo a distillation process. In a nonlocality distillation situation, we are given a number of nonlocal resources (boxes) characterised by weak nonlocality (according to some measure), and we apply to them operations regarded as free in order to create a final box having stronger nonlocality. However, even in the simplest distillation scenario, that uses two copies of a resource taken from the simplest Bell scenario, there are 82^4 candidate distillation protocols to computationally search over. This fact has been responsible for the extremely slow progress in the whole field. In this work, we initially tackle this chronic obstacle by developing techniques based on Linear Programming and on convex geometry, that significantly speed the search for protocols up. Then, we applied those techniques to construct Serially-Adaptive-Algorithms, algorithms that find out effective ways (in terms of highly amplifying the CHSH measure of nonlocality) to iterate protocols and to combine boxes in a two-by-two manner. After that, we study the almost unexplored so far territory of three-copy CHSH distillation protocols. Overall, four such protocols have been invented in this thesis, that outperform previously known protocols in certain aspects. Three of them are genuine in the sense that they are not reducible to iterations of lower scale (i.e. two-copy) protocols. Our genuine protocols unlock the distillability within sets of quantum correlations as well, that were not known to be distillable before. Every nonlocality distillation scheme developed in this thesis broadens the known set of post-quantum correlations that trivialize communication complexity. Through this prism, each one contributes on ruling out more post-quantum correlations. The third part of the thesis concerns the generalised probabilistic theory involving the full non-signalling state space (termed boxworld). It was known that while the states of boxworld can be richer, "more entangled" than quantum ones, its measurements are much poorer, following a regime of a "trade-off the measurements for the states". In this part we shift the attention towards boxworld measurements, and we are asking, even if they are not as elaborate as quantum ones can be, what is the most interesting set of measurements boxworld gives rise to? To this purpose, we characterise the deterministic effects in a certain boxworld scenario, by a method introduced here as an alternative to vertex-enumeration. We distinguish the couplers, the effects that cannot be expressed as trivial operations connecting inputs and outputs between boxes (the latter are wirings). Finally, having those couplers characterised, we spark-off the research field of finding information-processing tasks that benefit from them and indeed, we show that boxworld state-discrimination and nonlocality-distillation are among such tasks.

In the first half of this thesis, we present two models of ancilla-based quantum computation (ABQC). Computation in the ABQC models is based on effecting changes on a register through the interaction with and manipulation of an ancillary system. The two models presented enable quantum computation through only unitary control of the ancilla - the ancilla-controlled model (ACQC) - or supplemented by measurements on the ancilla which drive the register transfor- mations - the ancilla-driven model (ADQC). For each of the models, we work on systems which couple two continuous variables (CV) or which are hybrid: the register is formed by two-level systems while the ancilla is a CV degree of freedom. The initial models are presented using eigenstates of momentum as the ancillas. We move to a more realistic scenario by modelling the ancillas as finitely squeezed states. We find that the completely unitary ACQC contains persistent entanglement between register and ancilla in the finite-squeezing scenario. In the ancilla-driven model, the effect of finite squeezing is to scale the register state by a real exponential which is inversely proportional to the squeezing in the ancilla. In the second part, we cover work on Genuine Gaussian Multipartite Entanglement (Gaussian GME). We present an algorithm for finding Gaussian states that have GME despite having all two-state reductions separable. This touches on the idea of entanglement as an emergent phenomenon. We determine GME via witnesses which probe only a subset of the state. We therefore referred to them as partially blind witnesses. The algorithm is based on semi-definite programs (SDPs). Such optimisation schemes can be used to efficiently find an optimal, partially blind, GME witness for a given CM and vice versa. We then present results of multipartite states of up to six parties. For the tripartite example, we present two experimental schemes to produce the state using a circuit of beam-splitters and squeezers.

Shannon's theory of information laid the groundwork for the rapid developments in information and communications technologies over the last century. Yet, it assumed that information carriers were described by the laws of classical physics, whilst at the most fundamental level, nature obeys the laws of quantum physics. Quantum Shannon theory, which describes information carriers as quantum states, has led to a new era of possibilities, such as perfectly secure cryptography without pre-established keys. Yet, there is a sense in which this transition from classical to quantum is incomplete. Traditionally, quantum Shannon theory has focused on scenarios where the internal states of information carriers are quantum, whilst their trajectories in spacetime have still been assumed to be classical. This work presents a second level of quantisation where both the information itself and its propagation in spacetime are treated in a quantum fashion. The second-quantised Shannon theory describes the possibility of a single particle being simultaneously transmitted through multiple communication channels in a quantum superposition. The framework is developed using the tools of higher-order transformations and quantum resource theories, formally quantifying the resources required for communication between a sender and receiver in this setting. The advantages of the second-quantised theory are illustrated in a series of examples, showcasing various counterintuitive phenomena that occur when information is simultaneously transmitted through multiple communication channels. In particular, when a single particle travels in a quantum superposition through two alternative transmission lines, the noisy processes in the two lines can destructively interfere, leading to a cleaner communication channel overall. Various different scenarios are encompassed in the framework, including transmission through a superposition of both independent and correlated channels, as well as through large-scale communication networks. This work concludes with a study of the robustness of these protocols to errors and a discussion of recent experimental demonstrations of their associated communication advantages.

Superconducting circuits form one of the most promising hardware platforms for building a quantum computer. As the quantum computing system gets more complex as we increase the size, employing simple circuit designs and control strategies can make the task of building a large scale quantum computer easier. This thesis describes a novel control strategy that utilises spin-echo techniques and native interaction in superconducting circuits, which reduces the cost of calibrating pulsed two-qubit gates. Spin-echo pulses are used to rescale the always-on Hamiltonian, and the timings of spin-echo pulses encode the effective coupling strengths. In collaboration with the NMR group in Oxford, two methods for scaling this technique to large numbers of qubits were explored. In the first approach, pulse sequences for an all-to-all coupled system are obtained numerically using linear programming, and it finds the time-optimal solution for up to twenty qubits and the near time-optimal solution for up to hundreds of qubits. Another approach based on graph colouring finds the near time-optimal pulse sequence analytically, allowing pulse sequences for any number of qubits. An idea based on the Hamiltonian rescaling technique was applied to implementing the variational quantum eigensolver algorithm and error mitigation on two superconducting qubits. In contrast to previous studies, the residual dispersive coupling between qubits was used for computation instead of regarding it as a source of error. Lastly, the detailed dynamics of the residual dispersive coupling in superconducting circuits were investigated to predict the practicality of spin-echo-based quantum computing on superconducting circuits. The Hamiltonian rescaling protocol assumes the always-on coupling to be diagonal, such as Ising Hamiltonian, but deviation from the pure Ising interaction was observed in the strongly coupled superconducting qubits. The origin of the deviation was identified analytically, and the circuit design criteria to suppress the deviation are presented.

Quantum computers are thought to be the future of computation, using the properties of quantum mechanics to solve problems intractable to classical computers. Quantum computing leverages non-classical properties, such as entanglement, to achieve an exponential improvement in computational power. A quantum computer would enable us to address many real-world problems, such as how to synthesize fertilizers more efficiently; how to combat global warming; or to simulate protein folding in biological systems. Although much work has been done to describe the use and implementation of entanglement generation theoretically, it is still a challenge to develop such protocols experimentally. The bulk of this work is focused on creating Graphics Processing Unit (GPU)-accelerated computer simulations of quantum systems with advanced numerical and analytical techniques. Simulations can guide experiments attempting to create building blocks of quantum computers - qubits and their control devices. However, simulation of more realistic device setups in two dimensional systems has been facing problems owing to the space and time domain scaling associated with the solutions of the many-particle time dependent Schrodinger equation (TDSE). Nevertheless, recent advances in computer hardware performance has made previously intractable two-particle problems readily solvable. I have developed custom GPU-accelerated software based on a staggered-leapfrog algorithm that opens up new possibilities of simulating two-dimensional two-particle systems accurately. I focus on three research projects. Firstly, optimally defining a charge-based solid state qubit, and controlling it in a simple and experimentally achievable way, while accounting for imperfections of the waveform generators. I simulate the physical qubit on a fine-grained lattice, and propose an innovative control scheme that accounts for finite rise/fall time of the experimental apparatus, while being relatively fast and resulting in very high operation fidelity. An optimal pulsing scheme with rise time-dependent parameters is found, and shown to be able to achieve an arbitrary qubit rotation. Since the proposed pulse sequence reduces to sine waves to minimize total pulse duration, it is straightforward to implement experimentally, and easily generalisable to different systems. I also show how the fidelity remains sufficiently high independently of the initial qubit state. The proposed sequence can even reduce errors caused by charge noise under certain conditions. Readout techniques are discussed as well, and found to not present significant issues. Secondly, I aid the effort to create a Surface Acoustic Wave quantum computer prototype by describing how to produce an universal quantum gate set with a Root-of-SWAP operation used as a physical two-qubit gate. Using realistic parameters, it is shown how this operation can be performed with high fidelity. Previous work has been done to simulate a proposed Root-of-SWAP method in one dimension - this work focuses on extending this to two dimensions. We find that the method of generating Root-of-SWAP mentioned above breaks down in two dimensions- unwanted excitations are introduced in the extra dimension, causing a phase difference to appear, and thus ruining coherence of the state. I propose to implement the Root-of-SWAP operation via a tunneling interaction across the effective double dot instead. This was previously considered, however was thought to be unstable against variations in tunnel barrier height, which has exponential impact on the speed of the quantum operation. Using newly available computing power, we were able to run detailed two dimensional simulations investigating this method and its robustness against variations in the double dot potential. We find that the method produces high fidelity Root-of-SWAP states, and is robust against small variations in the tunnel barrier. Additionally, we find a relation between the tunnel barrier height and spin measurement probability, providing a way for experimentalists to estimate an actual device barrier indirectly. Finally, I theoretically model and simulate transport through a single electron transistor (SET) device. It is shown that a single donor structure can reliably be engineered from doped quantum dots by taking advantage of the tunability of the electron tunneling rates as well as the interplay, at low temperatures, between disorder conferred by randomness in dopant distribution and electron-electron interaction originating from the high doping concentration. It is possible to electrostatically isolate a single donor from the large ensemble of dopants. I investigate how such a complex system is expected to conduct, and verify a hypothesis that two donors take part in the transport by numerically reproducing the experimental measurements. Finally, it is shown that this device can be used as a single atom detector of the charge occupancy of a nearby capacitively coupled double quantum dot. While this final part does not make use of the GPU-accelerated software, it is still closely related to the rest of this work, and the theme of modeling realistic quantum devices.

In this thesis, we discuss aspects of the simulation, characterisation, and control of the dynamics of open quantum systems. The latter are systems governed by quantum mechanical laws and interacting with an environment, which is typically much larger than the system itself. According to the standard approach, one is usually able to perform a suitable average over the environmental degrees of freedom, resulting in an effective description of the main system dynamics, which accounts for the effects of the interaction with the surroundings. In standard scenarios, usually studied within the so-called Born-Markov approximation, the system-environment coupling is weak and such that we can perform a neat separation of timescales: the environmental dynamics is assumed to be fast compared to the typical evolution timescale of the system of interest. However, nowadays we are able to inspect physical scenarios where the usual Born-Markov approximation breaks down: the interaction between system and environment can be strong, likely leading to non-negligible memory (non-Markovian) effects. In this work, we discuss some instances in which we cannot work in the standard Born-Markov regime. We introduce and analyse some numerical and analytical techniques to characterise and simulate non-standard scenarios. We show that, even in the Markovian regime, the traditional formulation of thermodynamic irreversibility shows flaws and inconsistencies. We thus use phase-space methods to assess the role of initial correlations shared by the two parties of a bipartite harmonic system in the entropy production rate, including non-Markovian effects. Furthermore, we show that certain interactions enable to redraw the boundaries between the system and the environment in an effective manner, resulting in a new picture where the system degrees of freedom are augmented, while the residual environment is rearranged in such a way that the Born-Markov approximation is recovered. This analytical technique, known as reaction coordinate mapping approach, is employed in this work to show that, upon an accurate choice of the parameter regime, a spin-boson model can serve as a quantum analogue simulator of non-Markovian multiphoton Jaynes-Cummings models. These systematic studies shed light on the thermodynamic characterisation of open quantum systems, as well as on their numerical simulation.

Quantum computers are on the verge of revolutionising modern technology by providing scientists with unparalleled computational resources. With quantum-mechanical phenomena such as the superposition principle and entanglement, these computers could solve certain computational problems that are otherwise impossible for even the most powerful classical supercomputers. One of the major challenges standing in the way of this computing revolution is the accurate control of quantum bits. Quantum systems are extremely fragile and, by their nature, cannot be measured without destroying their quantum state. I wrote a numerical program to solve the time-dependent Schrödinger equation, the differential equation that describes the evolution of wave functions. The advantage of my code over other solvers is its speed. I used graphics processing units (GPUs), a technology that has only recently matured, to accelerate high-performance computing. Hardware- acceleration allows me to solve complex time-evolution problems within days rather than years. Such an exceptional speedup has enabled me to calculate the behaviour of single electrons in semiconductor devices. Electrons are particularly interesting because they are ubiquitous in modern technology, as well as being fundamental quantum particles. Using the simulations produced by my code, I track the time evolution of an electron wave function as it propagates along quantum circuits. By animating the evolution of the wave function, I am able to visualise the wave function of electrons propagating in space and time. This is a remarkable tool for studying the behaviour of quantum particles in nanodevices. I focused my thesis on the realistic modelling of devices that are readily available in a laboratory or on designs that could be fabricated in the near future. I began by modelling single electrons as quantum bits. I provide a definition for an optimal qubit and lay out the set of operations required to manipulate the quantum information carried by the electron. In all my simulations, I aim to model experimentally realistic devices. I calculated the electrostatic potential of a real nanodevice and simulated the time-evolution of a single electron. I show that it is possible to create a single-electron beam splitter by tuning the voltages applied to various parts of the device and I calculate the range of voltages in which quantum information is preserved and manipulated accurately. These results were verified experimentally by collaborators at the Institut Néel and were published in Nature Communications 10, 4557 (2019). Using my code, I developed a framework for general measurements of electron qubits and provided a design for a semiconductor device capable of performing positive-operator valued measures (POVMs). A POVM is a powerful measurement technique in quantum mechanics that allows quantum information to be manipulated in interesting ways. The proposed setup is suggested as an implementation of entanglement distillation, which is a useful error correction tool that transforms an arbitrary entangled state into a pure Bell pair. Entanglement is one of the most fascinating aspects of quantum mechanics and it remains a challenge to generate perfectly entangled particle pairs. An experimentally viable method for distilling - or perfecting - entanglement is crucial for the design of quantum computers or quantum communication systems. Using this design, I introduced a protocol to use electrons, rather than photons, in quantum-optics-like systems. These results were published in Phys. Rev. A 96, 052305 (2017). Going beyond single-particle behaviour, I compare different methods for generating entanglement between electron-spin qubits using the power-of-SWAP operation. By using realistic experimental parameters in my simulations, I demonstrate that generating entan- glement via electron-electron collisions in a harmonic channel cannot be implemented for multidimensional systems. These findings go against what researchers thought was possible and put forward the need for new solutions to particle entanglement. I provide an alternative by demonstrating that a method based on the exchange energy is more viable than previously thought. I present a semiconductor device structure and an electrostatic potential that experi- mental groups can use in order to obtain the most efficient entangling quantum logic gates. These findings were published in Phys. Rev. A 101, 022329 (2020). The results presented in this thesis provide a comprehensive description of the control of single electrons in a surface-acoustic-wave-based quantum circuit. However, work in this field is far from over. I present various research paths for future projects. These include going beyond the time-dependent Schrödinger equation to capture more complicated dynamics, using different hardware solutions to further accelerate numerical problem solving, and studying new systems of interest to extend this project beyond semiconductor physics.In all my simulations, I aim to model experimentally realistic devices. I calculated the electrostatic potential of a real nanodevice and simulated the time-evolution of a single electron. I show that it is possible to create a single-electron beam splitter by tuning the voltages applied to various parts of the device and I calculate the range of voltages in which quantum information is preserved and manipulated accurately. These results were verified experimentally by collaborators at the Institut Néel and were published in Nature Communications 10, 4557 (2019). Using my code, I developed a framework for general measurements of electron qubits and provided a design for a semiconductor device capable of performing positive-operator valued measures (POVMs). A POVM is a powerful measurement technique in quantum mechanics that allows quantum information to be manipulated in interesting ways. The proposed setup is suggested as an implementation of entanglement distillation, which is a useful error correction tool that transforms an arbitrary entangled state into a pure Bell pair. Entanglement is one of the most fascinating aspects of quantum mechanics and it remains a challenge to generate perfectly entangled particle pairs. An experimentally viable method for distilling - or perfecting - entanglement is crucial for the design of quantum computers or quantum communication systems. Using this design, I introduced a protocol to use electrons, rather than photons, in quantum-optics-like systems. These results were published in Phys. Rev. A 96, 052305 (2017). Going beyond single-particle behaviour, I compare different methods for generating entanglement between electron-spin qubits using the power-of-SWAP operation. By using realistic experimental parameters in my simulations, I demonstrate that generating entan- glement via electron-electron collisions in a harmonic channel cannot be implemented for multidimensional systems. These findings go against what researchers thought was possible and put forward the need for new solutions to particle entanglement. I provide an alternative by demonstrating that a method based on the exchange energy is more viable than previously thought. I present a semiconductor device structure and an electrostatic potential that experi- mental groups can use in order to obtain the most efficient entangling quantum logic gates. These findings were published in Phys. Rev. A 101, 022329 (2020). The results presented in this thesis provide a comprehensive description of the control of single electrons in a surface-acoustic-wave-based quantum circuit. However, work in this field is far from over. I present various research paths for future projects. These include going beyond the time-dependent Schrödinger equation to capture more complicated dynamics, using different hardware solutions to further accelerate numerical problem solving, and studying new systems of interest to extend this project beyond semiconductor physics.

An exquisite control over the dynamics of a quantum system is essential for realizing any quantum technology. This thesis presents some practical and efficient strategies for coherent quantum control: a paradigm for controlling quantum dynamics using electromagnetic fields. Coherent control is a common framework for describing the physical implementation of quantum logic gates in several quantum information processing platforms including superconducting qubits and trapped ions. For the purpose of demonstration, however, liquid-state Nuclear Magnetic Resonance (NMR) is used in this thesis as it is an ideal test-bed for developing, testing and benchmarking coherent control tools and techniques. Coherent control was revitalised in 2005 by the development of Gradient Ascent Pulse Engineering (GRAPE), a powerful optimal control technique that is widely used for designing shaped pulses for a variety of tasks. GRAPE, like any other closed-loop optimal control algorithm, requires multiple evaluations of the computationally expensive matrix exponential and the full time-evolution propagator. To this end, I present strategies to sidestep the explicit evaluation of matrix exponentials, thereby offering substantial speed-ups over conventional implementations of the GRAPE algorithm. The results are demonstrated experimentally in NMR, but also in simulations of ultracold molecules and superconducting qubits. Beyond GRAPE, this thesis also considers methods for designing spin-echo sequences for implementing any arbitrary network of controlled-Z gates in a system of qubits with zz-couplings. First, a method based on linear-programming provides near time-optimal sequences in fully-coupled systems having up to a few hundred qubits. Further, an analytic method based on graph colouring finds near time-optimal spin echo sequences in engineered systems with any number of qubits having only nearest and next-nearest neighbour-couplings.

The absolute/relative debate on the nature of space and time is ongoing for thousands of years. Here we attempt to investigate space and time from the information theoretic point of view to understand spatial and temporal correlations under the relative assumption. Correlations, as a measure of relationship between two quantities, do not distinguish space and time in classical probability theory; quantum correlations in space are well-studied but temporal correlations are not well understood. The thesis investigates quantum correlations in space-time, by treating temporal correlations equally in form as spatial correlations and unifying quantum correlations in space and time. In particular, we follow the pseudo-density matrix formalism in which quantum states in spacetime are properly defined by correlations from measurements. We first review classical correlations, quantum correlations in space and time, to motivate the pseudo-density matrix formalism in finite dimensions. Next we generalise the pseudo-density matrix formulation to continuous variables and general measurements. Specifically, we define Gaussian spacetime states by the first two statistical moments, and for general continuous variables spacetime states are defined via the Wigner function representation. We also define spacetime quantum states in position measurements and weak measurements for general measurement processes. Then we compare the pseudo-density matrix formalism with other spacetime formulations: indefinite causal structures, consistent histories, generalised non-local games, out-of-time-order correlation functions, and path integrals. We argue that in non-relativistic quantum mechanics, different spacetime formulations are closely related and almost equivalent via quantum correlations, except path integrals. Finally, we apply the pseudo-density matrix formulation to time crystals. By defining time crystals as long-range order in time, we analyse continuous and discrete time translation symmetry as well as discuss the existence of time crystals from an algebraic point of view. Finally, we summarise our work and provide the outlook for future directions.

Quantum technologies, able to manipulate the individual quantum states of single particles, have the potential to revolutionise science and engineering. The possible applications of these technologies are remarkably broad, ranging from the simulation of the underlying physics that governs our universe, to securing the worlds information, and even to improving health-care through quantum metrology. Though there are many competing quantum technology platforms, quantum platforms based on light are uniquely fascinating due to their low noise and suitability for communications. Modern fabrication methods allow for the production of chip-scale devices that can trap and manipulate single particles of light (photons) to produce complex quantum states on chip. In particular, silicon photonic devices are of interest due to the abundance and supply chains of silicon in the microelectronics industry. Theoretically, these supply chains could be leveraged to mass produce high performance quantum technologies built from silicon photonic components at scale and low cost. In this thesis we explore current silicon quantum photonic technologies and their applications. In particular, we asses how they can be leveraged to generate pure single photons and how multiple photons can be reliably interfered on a chip. In addition, we introduce many key integrated quantum optic components and explain how, when combined with high quality single photon sources, they can be used to encode quantum information in silicon chips. Several of the fundamental protocols of quantum information theory are benchmarked on state-of-the-art silicon photonic chips and methods for chip-to-chip demonstrations are proposed and verified. Finally, we discuss the scalability of these devices and outline the technologies that are required in order to advance the field of integrated quantum photonic technologies.

In this thesis, we discuss applications of machine learning to quantum information science. The interface between these two fields has been the subject of much research, recently, driven by the many successes of machine learning for diverse pattern recognition tasks. The work reported in this Thesis addresses precisely the potential of such an interdisciplinary line of research and illustrates how machine learning provides a valuable add-on to standard techniques used in the context of quantum technologies. Specifically, we will first study the problem of devising time-independent dynamics implementing target quantum operations. This involves a challenging optimisation task, which is hard to tackle with standard numerical tools. We demonstrate how the use of supervised learning algorithms can dramatically speed-up this task. We then consider the tasks of engineering and characterising quantum states in large Hilbert spaces. Motivated by strong experimental reasons, we consider explicitly the embodiment of such multi-dimensional quantum systems provided by the orbital angular momentum and polarisation degrees of freedom of light. We devise a protocol involving quantum walks to implement arbitrary states by only making use of the possibility to couple polarisation and orbital angular momentum through relatively recent technological advances in the field of linear optics. This protocol relies solely on the properties of quantum walk dynamics, and is therefore applicable to different types of architectures. We then present an experimental demonstration of this engineering strategy, and consider the issue of assessing the quality of the states thus generated. We show how different machine learning algorithms, including supervised and unsupervised learning ones, are able to tackle this problem and provide useful information in realistic experimental conditions.

Since its introduction in the 1930s by Wigner, and its generalisations by Moyal and Weyl, the ability to associate an operator on Hilbert space by a quasi-probability distribution function on phase space has found extensive use in the physics of con- tinuous variable systems. Lacking, however, is finite system applications; to date, such functions have taken a back seat to state vector, path integration, and Heisen- berg representations. In recent work, this lack of application has been addressed by giving a general framework to generate phase-space distribution functions for any system. Where the Wigner function for any system can be expressed in displaced parity form. This construction of a general framework for treating quantum mechanics in phase space will be presented in full in this thesis. Demonstrating a general approach to quantum mechanics as a statistical theory. Using this work, it will be shown how varied quantum systems can be easily represented in phase space as well as visualise certain quantum properties, such as entanglement, within these systems. In particular, formalism is applied to directly measure phase space coordinates of multiple qubit states, including a five-qubit GHZ state, on IBM's Quantum Experience. Further, how these methods can be extended for use in general composite quantum systems, such as hybrid atom-cavity systems, will be presented, demonstrating how these phase-space methods are an optimal method for quantum state analysis, entanglement testing, and state characterisations.

Over the last few decades there has been strong interest in quantum information systems based on photonic qubits. Devices able to emit pure single-photon states on demand and detect incoming single photons in the system are fundamental building blocks for the realisation of a quantum photonic scheme. Advances in controlling single carriers have made it possible to transport single electrons using surface acoustic waves (SAWs). In a lateral n-i-p junction SAW-driven single-electron transport can be exploited to pump single electrons across the junction and generate single photons. In this work, devices have been developed in which both electrons and holes can be induced in an undoped GaAs/AlGaAs 15nm quantum well by gates to form a lateral n-i-p junction. The junction is confined into a quasi-1D channel laterally by etching and side gates. Light emission is observed when a 1 or 3 GHz SAW drives a current, by pumping electrons over the potential hill in the intrinsic region. SAW-driven electroluminescence has been characterised in the regime where less than one electron is transported per cycle on average. Time-resolved electroluminescence has been used to extract the electron recombination time and to quantify the contributions from electromagnetic crosstalk and the SAW. In a device without significant crosstalk, the degree of second-order coherence, g(2)(0) , shows the signature of antibunching. Hole SAW-pumping has been investigated as an alternative to electron pumping, showing a shorter recombination time. The dynamics has been further investigated with time-resolved and energy measurements at the junction, using a sub-micron positioner with lens assembly to scan along the pumping direction. A key requirement for practical quantum devices is the scalable integration of single-photon sources, detectors and linear optical elements on a common platform. Using the same type of heterostructure, photons are detected by collecting and measuring the photo-generated carriers. An external light source sends photons into the system, and when they are absorbed in the quantum well, they create electron-hole pairs. The photo-generated carriers are separated and transported by a SAW together with an electric field applied by gates on the surface. The carriers are then collected by ohmic contacts, in order to extract information about the number of photons absorbed. Using the same 15nm GaAs/AlGaAs quantum well as for the single- photon source, an acousto-electric photon detector has been realised and characterised. Single-photon sensitivity can be achieved by measuring the photo-generated charges at single-particle level. The possibility to include single-electron and single-hole charge readout using quantum dots and quantum point contacts has been investigated.

Technology founded in quantum phenomena is set to revolutionise computation, sensing and communication. With an entirely different method of manipulating information, quantum computers in particular are able to offer significant advances when compared to their classical counterparts. Unrelenting research throughout the world implies that such machines are set to be the demise of public-key cryptography that is critical to modern society. Quantum key distribution (QKD) offers a method to securely distribute randomness between distant parties using the fundamental nature of the universe. Protocols do not depend on assumed hard problems and so the security of the key does not decrease as computing power increases. However, QKD systems have been susceptible to information leakage or hacks which compromises their security at the time of key exchange. As research demonstrations evolve into commercial systems, the security of a physical implementations must be addressed. Device-independent protocols have since been introduced to relieve the possibility of secret information falling into the hands of an adversary. Using correlations between random events, the physical system does not contain any information about the key. Therefore, it is not susceptible to attacks or able to reveal the secret key. This simplifies the task of characterising a system to guarantee a secure key exchange. Before QKD can be widely adopted, a cost-effective and scalable platform must be developed. In the last decade, photonic integration has been refined to facilitate circuit complexity simply not possible with bulk alternatives. The inherent robustness and phase-stability make it an excellent candidate for future quantum-secured networks. This thesis will explore how integrated photonics can be deployed in device-independent QKD protocols to both ensure practical security and enhance network accessibility. We will show how integrated components can be used to generate quantum states with high fidelity and demonstrate quantum interference. The complexity of photonic integration will be explored to demonstrate new circuits for QKD that will eventually form the backbone of quantum-secured networks.

A central theme of this thesis is the quantization and generalization of objects from areas of mathematics such as set theory and combinatorics with application to quantum information. We represent mathematical objects such as Latin squares or functions as string diagrams over the category of finite-dimensional Hilbert spaces obeying various diagrammatic axioms. This leads to a direct understanding of how these objects arise in quantum mechanics and gives insight into how quantum analogues can be defined. In Part I of this thesis we introduce quantum Latin squares (QLS), quantum objects which generalize the classical Latin squares from combinatorics. We present a new method for constructing a unitary error basis (UEB) from a quantum Latin square equipped with extra data, which we show simultaneously generalizes the existing shift-and-multiply and Hadamard methods. We introduce two different notions of orthogonality for QLS which we use to construct families of mutually unbiased bases and perfect tensors respectively. We also introduce a further generalization of Latin squares called quantum Latin isometry squares. We use these to produce quantum error codes and to give a new way of characterizing UEBs. In Part II we show that maximal families of mutually unbiased bases (MUBs) are characterized in all dimensions by partitioned UEBs, up to a choice of a family of Hadamards. Furthermore, we give a new construction of partitioned UEBs, and thus maximal families of MUBs, from a finite field, which is simpler and more direct than previous proposals. We introduce new tensor diagrammatic characterizations of maximal families of MUBs, partitioned UEBs, and finite fields as algebraic structures defined over Hilbert spaces. In Part III we introduce quantum functions and quantum sets, which quantize the classical notions. We show that these structures form a 2-category 'QSet'. We extend this framework to introduce quantum graphs and quantum homomorphisms which form a 2-category 'QGraph'. We show that these 2-categories capture several different notions of quantum morphism and noncommutative graph from various previous papers in noncommutative topology, quantum non-local games and quantum information. We later use the correspondence between our quantum graph morphisms and those from quantum non-local games to show that pairs of quantum isomorphic graphs with multiple connected components are built up of quantum isomorphisms on those components.

Exploring how light interacts with physical systems is an elegant and powerful way to unravel processes occurring at different scales, from bulk materials to single atoms. In this thesis, we employ several microscopy and spectroscopy techniques to investigate the local optoelectronic properties of metal halide perovskites, from thin films to large crystals, as well as to elucidate the physics of single-photon emitters in diamond. First, the influence of the grain size on the low-temperature phase transition in methylammonium lead iodide perovskite polycrystalline thin films is assessed by means of temperature-dependent macro- and micro-photoluminescence measurements coupled with complementary X-ray diffraction and absorption measurements. The results suggest that local strain plays a role in inhibiting thel low-temperature tetragonal-to-orthorhombic phase transition, and in the extreme case of very small grains, can almost entirely suppress it. We then unveil buried charge-carrier recombination pathways in both thin film and micro-crystal methylammonium lead halide perovskite structures through 3D photoluminescence tomography acquired using two-photon confocal microscopy. These measurements reveal that light-induced passivation approaches are primarily surface-sensitive and that even nominal single crystals still contain heterogeneous defects that impact charge-carrier recombination. We build on the two-photon mapping by developing a technique to monitor the carrier diffusion at different depths in a semiconductor by monitoring the photoluminescence as a function of distance from the two-photon-excitation spot. The technique was applied to methylammonium lead bromide crystals, revealing a spatial heterogeneity in diffusion that is not captured in macroscopic diffusion measurements. We outline a model to explain the observations by distinguishing the influences of carrier diffusion and photon reabsorption at different depths in the sample. Finally, a series of optical studies on the Silicon-Vacancy (SiV) colour-centre in diamond are reported. Coherent Population Trapping (CPT) experiments performed using electrically actuated diamond micro-cantilevers show that the ground state splitting, and therefore the strength of the electron-photon coupling limiting the coherence time in this system, depends upon mechanical strain. A route to the all-optical control of such single electron spins in diamond is then outlined. The thesis overall introduces a number of powerful techniques to shed light on the intimate relationships between carrier recombination, defects, strain and other physical properties of novel light absorbing and light emitting materials.

This DPhil thesis presents two key works towards practical applications of quantum optics. Both works are novel and achieve competitive state-of-the-art results. Today's most widely used method of encoding quantum information in optical qubits is the dual-rail basis, often carried out through the polarisation of a single photon. On the other hand, many stationary carriers of quantum information | such as atoms | couple to light via the single-rail encoding in which the qubit is encoded in the number of photons. As such, interconversion between the two encodings is paramount in order to achieve cohesive quantum networks. In the first part of this thesis, we demonstrate this by generating a hybrid entangled resource between the two encodings and using it to teleport a dual-rail qubit onto its singlerail counterpart. Our key results yield an average fidelity of F = (92:8±2:2)% for the teleportation and F = (89:7 ± 2:1)% for entanglement swapping, thus confirming the applicability of this scheme towards a real-world implementation. This work completes the set of tools necessary for the interconversion between the three primary encodings of a qubit in the optical field: single-rail, dual-rail and continuous-variable. A remarkable aspect of quantum theory is that certain measurement outcomes are entirely unpredictable to all possible observers. Such quantum events can be harnessed to generate numbers whose randomness is asserted based upon the underlying physical processes. In the second part of this thesis, we formally introduce and experimentally demonstrate an ultrafast optical quantum randomness generator that uses a totally untrusted photonic source and whose idea we have patented. While considering completely general quantum attacks, we certify randomness at a rate of 1:1 Gbps with a rigorous security parameter of 10-20. Our security proof is entirely composable, thereby allowing the generated randomness to be utilised for arbitrary applications in cryptography and beyond.

Quantum networks lie at the heart of distributed quantum computing and secure quantum communication - research areas that have seen a strong increase of interest over the last decade. Their basic architecture consist of stationary nodes composed of quantum processors which are linked via photonic channels. The key requirement, and at the same time the most demanding challenge, is the efficient distribution of entanglement between distant nodes. The two ground states of single spins confined in self-assembled InGaAs quantum dots provide an effective two-level system for the implementation of quantum bits. Moreover, they offer strong transition dipole moments with outstanding photonic properties allowing for the realisation of close to ideal, high-bandwidth spin-photon interfaces. These properties are combined with the benefits of working in the solid state, such as scalability and integrability of devices, to form a promising candidate for the implementation of fast entanglement distribution. In this dissertation we provide the first implementation of a unit cell of a quantum network based on single electron spins in InGaAs. We use a probabilistic scheme based on spin-photon entanglement and the erasure of which path information to project the two distant spins into a maximally entangled Bell state. The successful generation of entanglement is verified through a reconstruction of the final two-spin state and we achieve an average fidelity of $61.6\pm2.3\%$ at a record-high generation rate of $5.8\,\mathrm{kHz}$. One of the main constraints to the achieved fidelity is the limited coherence of the electron spin. We show that it can be extended by three orders of magnitude through decoupling techniques and develop a new measurement technique, allowing us to investigate the origins of the decoherence which has previously been obscured by nuclear feedback processes. Our results evidence that further extension of coherence is ultimately limited by intrinsic mechanisms closely related to local strain due to the growth method of self-assembled quantum dots. After establishing the intrinsic limits to the electron coherence we investigate the coherence properties of the single hole spin as an alternative two-level system with the potential for higher coherence times. We show that the hole spin coherence is indeed superior to the one of the electron and realise the first successful dynamic decoupling scheme implemented in these systems. We find that the decoherence at low external magnetic fields is still governed by coupling to the nuclear spins whereas it is dominated by electrical noise for fields exceeding a few Tesla. This noise source is extrinsic to the quantum dots and a better understanding offers the potential for further improvement of the coherence time. The findings of this work present a complete study of the coherence of the charge carriers in self-assembled quantum dots and provide the knowledge needed to improve the implementation of a quantum-dot based quantum network. In particular, the combination of spin-spin entanglement and the hole coherence times enable further research towards multidimensional photonic cluster states.

Single-photon sources are essential building blocks in quantum photonic networks, where quantum-mechanical properties of photons are utilised to achieve quantum technologies such as quantum cryptography and quantum computing. In this thesis, a single-photon source driven by a surface acoustic wave (SAW) is developed and characterised. This single-photon source is based on a SAW-driven lateral n-i-p junction in a GaAs quantum-well structure. On this device, the lateral n-i-p junction is formed by gate-induced electrons and holes in two adjacent regions. The SAW potential minima create dynamic quantum dots in a 1D channel between these two regions, and are able to transport single electrons to the region of holes along the channel. Single-photon emission can therefore be generated as these electrons consecutively recombine with holes. After characterisation and optimisation in four batches of devices, clear SAW-driven charge transport and the corresponding electroluminescence (EL) can be observed on an optimised SAW-driven n-i-p junction. Time-resolved measurements have been carried out to study the dynamics of SAW-driven electrons. Time-resolved EL signals indicate that a packet of electrons is transported to the region of holes in each SAW minimum. In addition, the carrier lifetime of SAW-driven electrons in the region of holes is shown to be $\sim 100$ ps, which is much shorter than the SAW period of $860$ ps. Hence, it is promising to observe single-photon emission in the optimised device. In order to test single-photon emission, a Hanbury Brown-Twiss experimental setup has been employed to record an autocorrelation histogram of the SAW-driven EL signal at the single-electron regime. Suppression of autocorrelation coincidences at time delay $\Delta t = 0$ is evidence of photon antibunching. By fitting theoretical functions describing the SAW-driven EL signal, it is found that the second-order correlation function shows $g^{(2)}(0) = 0.39 \pm 0.05$, which is lower than the common criterion for a single-photon source $g^{(2)}(0) < 0.5$. Moreover, theoretical calculation and simulation suggest that, if a constant background signal can be filtered out, $\sim 80 \%$ of the SAW-driven EL is single-photon emission.

The 2-dimensional semiconductor family of materials called transition metal dichalcogenides (2d-TMDs) offers many technological advantages: low power consumption, atomically-precise interfaces, lack of nuclear spins and ease of functional integration with other 2d materials are just a few. In this work we harness the potential of these materials as a platform for quantum devices: develop a method by which we can deterministically create single-photon emitting sites in 2d-TMDs, in large-scale arrays. These we call quantum dots (QDs): quantum confinement potentials within semiconductor materials which can trap single-excitons. The single excitons recombine radiatively to emit single-photons. Single-photon sources are a crucial requirement for many quantum information technology (QIT) applications such as quantum cryptography and quantum communication. The QDs are formed by placing the flakes over substrates nano-patterned with protru- sions which induce local strain and provoke the quantum confinement of excitons at low temperatures. This method has been successfully tested in several TMD materials, hence achieving quantum light at different wavelengths. We present one of the very few systems where quantum confinement sites have been shown to be deterministically engineered in a scalable way. Moreover, we have demonstrated how the 2d-based QDs can be embedded within 2d- heterostructures to form functional quantum devices: we have used TMD monolayers along with other 2d-materials - graphene and hexagonal boron nitride - to create quan- tum light-emitting diodes that produce electrically-driven single-photons. Again, very few single-photon sources can be triggered electrically, and this provides a great ad- vantage when considering on-chip quantum technologies. Finally, we present experimental steps towards using our architecture as quantum bits: capturing single-spins inside the QDs, using field-effect type 2d-heterostructures. We are able to controllably charge the QDs with single-electrons and single-holes – a key breakthrough towards the use of spin and valley pseudospin of confined carriers in 2d-materials as a new kind of optically addressable matter qubit. This work presents the successful marriage of 2d-semiconductor technology with QIT, paving the way for 2-dimensional materials as platforms for scalable, on-chip quantum photonics.

The field of quantum mechanics has revolutionised physics as a subject. Areas such as information theory, computer science and physical sensing have all been affected by the tremendous successes of various quantum protocols. In this thesis I present my contribution to the development of such non-classical protocols. In classical communication theory a message is always carried by physical particles that interact with a transmitter, after which they travel to a receiver. In this thesis I outline a quantum protocol which allows a receiver to obtain a message without receiving any physical object or particles that have interacted with the transmitter-that is, counterfactually. I build my protocol for counterfactual communication on the principles of interaction-free measurements, ensuring that information always propagates in the opposite direction to the protocol particles. The protocol shows how quantum mechanics breaks the previous premise of communication theory. From the perspective of local observers, it is a beautiful manifestation of the non-locality of interaction-free measurements. Furthermore, it is highly robust against experimental errors and external disturbances. The majority of this part of the thesis is based on my published article 'Quantum counterfactual communication without a weak trace' [Phys. Rev. A 94, 062303 (2016)]. Previous to my work, Salih et al. attempted to design a counterfactual communication protocol [Phys. Rev. Lett. 110, 170502 (2013)]. This protocol has been highly controversial. As counterfactual phenomena impose restrictions on the inter-measurement paths of quantum particles, and the physical reality of such paths lacks description in the Copenhagen interpretation of quantum mechanics, an extension of current quantum theory is required to facilitate a discussion. In this thesis I present an operational and interpretation-independent methodology, enabling the discussion of inter-measurement paths of quantum particles. I start by considering the interferometers of counterfactual protocols, making the basic assumption that any quantum evolution naturally involves uncontrolled weak interactions. I then show how the Fisher information of these weak interactions, available at the output of counterfactual experiments, can be used to discuss the pre-measurement past of the particles. Based on this analysis, the protocol developed by Salih et al. is found to strongly violate counterfactuality. However, my protocol is more flexible in that it allows particles to propagate in the opposite direction to the message. This leads to counterfactuality being satisfied-even in the presence of large experimental errors. These results are observed both analytically and numerically. This part of the thesis is based on my article 'Evaluation of counterfactuality in counterfactual communication protocols' [Phys. Rev. A 96, 062316 (2017)]. The numerical methods are inspired by another of my publications: 'Protocol for fermionic positive-operator-valued measures' [Phys. Rev. A 96, 052305 (2017)]. Finally, as the Fisher information measure is found to be useful in evaluating counterfactual protocols, I extend my work by investigating the quantum Fisher information in experiments with general discrete quantum circuits. I prove that the quantum Fisher information of a two-level interaction in a quantum circuit can be expressed by a simple formula. Under certain phase-relations, the formula provides a straightforward connection between the abstract concept of the inter-measurement wavefunction and the quantum Fisher information at the output. With regard to how the information obtained from a certain volume of space influences our perception of classical objects, I argue that the quantum Fisher information measure is highly useful in describing quantum objects. If this measure is applied to observers with a limited set of the experimental measurement outcomes, a quantum object can appear to follow non-classical discontinuous paths. This supports the remarkable conclusion that our perception of the past of a quantum object is subjectively dependent on the measurement we conduct on it.

The project concerns the study of the interplay among quantum mechanics, statistical mechanics and thermodynamics, in isolated quantum systems. The goal of this research is to improve our understanding of the concept of thermal equilibrium in quantum systems. First, I investigated the role played by observables and measurements in the emergence of thermal behaviour. This led to a new notion of thermal equilibrium which is specific for a given observable, rather than for the whole state of the system. The equilibrium picture that emerges is a generalization of statistical mechanics in which we are not interested in the state of the system but only in the outcome of the measurement process. I investigated how this picture relates to one of the most promising approaches for the emergence of thermal behaviour in quantum systems: the Eigenstate Thermalization Hypothesis. Then, I applied the results to study the equilibrium properties of peculiar quantum systems, which are known to escape thermalization: the many-body localised systems. Despite the localization phenomenon, which prevents thermalization of subsystems, I was able to show that we can still use the predictions of statistical mechanics to describe the equilibrium of some observables. Moreover, the intuition developed in the process led me to propose an experimentally accessible way to unravel the interacting nature of many-body localised systems. Then, I exploited the "Concentration of Measure" and the related "Typicality Arguments" to study the macroscopic properties of the basis states in a tentative theory of quantum gravity: Loop Quantum Gravity. These techniques were previously used to explain why the thermal behaviour in quantum systems is such an ubiquitous phenomenon at the macroscopic scale. I focused on the local properties, their thermodynamic behaviour and interplay with the semiclassical limit. The ultimate goal of this line of research is to give a quantum description of a black hole which is consistent with the expected semiclassical behaviour. This was motivated by the necessity to understand, from a quantum gravity perspective, how and why an horizon exhibits thermal properties.

Decoherence is a major barrier to the implementation of quantum technologies. Theoretical techniques for understanding decoherence in composite systems have traditionally been focused on systems with distinguishable emission spectra, where measuring the frequency of an emitted photon allows one to determine which process took place. Here the photon contains information about the state of the system. On the other hand, systems with indistinguishable spectra do not necessarily completely reveal information about the state of the system when a photon is emitted. It can be impossible to say for certain which of two nearly degenerate transitions has occurred just by measuring the photon's frequency. It is then possible to preserve information within the system throughout the decay process. In this Thesis we show that indistinguishable spectra can lead to protected coherences within one part of a coupled quantum system, even as another part decays. We develop a zero-temperature exact approach for modelling such systems, and compare it to the microscopically derived Born-Markov master equation. This comparison helps us to understand the range of validity of the Markovian approximation. We use this understanding to extend the master equation approach to finite temperature within the Markovian regime, and we compare its high temperature results to a semiclassical model. We examine the physical conditions required for coherence protection, and remarkably we find that heating the system can improve coherence protection. Similarly, increasing the decay rate of the unprotected part of the coupled system can also enhance the coherence of the protected part. These effects are the results of linewidth broadening and thus greater spectral indistinguishability. The findings in this Thesis are of interest to both those seeking to engineer hybrid quantum systems and those seeking to develop theoretical techniques for dealing with the decoherence of composite quantum systems.

We investigate the coupling of a single trapped ion to a miniature optical cavity operating in the ultraviolet. Our cavity provides a source of single photons at a high rate into a single spatial mode. Using our apparatus, we have demonstrated the highest atom-cavity coupling rate achieved with a single ion by an order of magnitude. When the ion is continuously excited, we observe phase-sensitive correlations between emission into free-space and into the cavity mode, which can be explained by a cavity induced back-action effect on a driven dipole. We demonstrate coherent manipulation of a hyperfine qubit and ultra-short optical π rotations, which are essential tools for creation and detection of spin-photon entanglement. To this end, we have developed optical fibre-based Fabry-Perot cavities in the ultraviolet spectral range. These cavities operate near the primary dipole transition of Yb at 370 nm, and allow us to couple a pure atomic two-level system offered by a single trapped ion to the cavity mode. A new Paul trap apparatus in an ultra-high vacuum chamber has been built which allows for the integration of these cavities at very small ion-mirror separations. In order for independent operation of the trap, a compact system of diode lasers has been built which are stabilised to low-drift optical reference cavities. Coherent control of the hyperfine qubit in Yb 171 is achieved through application of microwave radiation, and ultra-short optical π rotations are performed with resonant light pulses derived from a frequency-doubled mode-locked titanium-sapphire laser. The experiment is controlled through a system of hardware and software which has been developed in a modular fashion and will allow for efficient control on the nanosecond time-scale when several such systems are interconnected. The success of our system opens the door to future experiments with trapped ions which will reach the strong coupling regime with a single ion. Furthermore, when operated in the fast-cavity regime, systems based on our approach will enable high-efficiency collection of photons from the ion into the single mode of an optical fibre. These systems will allow for the generation of distributed entanglement and will prove ideal as nodes in a larger quantum network of trapped ions.

Electron spins confined to self-assembled quantum dots are considered as nodes for a coherent optical network capable of supporting distributed quantum states. Through a series of experiments, the work contributing to this dissertation examines some of the key criteria for constructing such a network. First, the ability to optically extract a coherent spin state from the quantum dot without perturbing the nuclear environment is explored: nuclear feedback is an issue that has frustrated previous studies into electron spin coherence in these systems. With the novel techniques we develop, we identify and characterise the previously undetermined intrinsic mechanisms that govern the coherence of the central spin. We show how the coherence of the electron spin is intimately related to the growth of these strained nanostructures. Second, a model network is constructed in which two spins confined to separate quantum dots are projected into a highly entangled state. This is the first time electron spins in distant quantum dots have been entangled, and in doing so we demonstrate controllable entanglement generation at the highest rates recorded for optically accessible qubit definitions. We investigate the realisation of a hybrid quantum network by demonstrating the first interconnect between wholly different single quantum systems: a semiconductor quantum dot and a trapped ytterbium ion. In forming an optical link between these two complementary qubit definitions, we show that we can circumvent their intrinsic optical differences through coherent photon generation at the quantum dot. A network built from these diverse constituents could combine the ultrafast operations self-assembled quantum dots enable with the long coherence times states in trapped ions experience. Finally, in a step towards truly scalable entanglement generation between quantum dot spins, we design minimally invasive structures that will funnel large proportions of the optical dipole field from the optically dense material that surrounds the quantum dot. The techniques developed in this work and the knowledge gained from their operation should enable the demonstration the creation of high-order nonlocal states between quantum dot spins, single photons and trapped ions, as well as the development of new optically active systems that will benefit from enhanced spin coherence.

Quantum mechanics, which describes the behaviour of matter and energy on very small scales, is one of the most successful theories in the history of science. Einstein's theory of special relativity, which describes the relationship between space and time, is likewise a highly successful and widely accepted theory. And yet there is a well-documented tension between the two theories, to the extent that it is still not clear that the two can ever be reconciled. This thesis is concerned with furthering the current understanding of the relationship between quantum mechanics and special relativity. In the first part of the thesis we study the behaviour of quantum information in relativistic spacetime. The field of quantum information arose from the realisation that quantum information has a number of crucial properties that distinguish it from classical information, such as the no-cloning property, quantum contextuality, and quantum discord. More recently, it has been realised that placing quantum information under relativistic constraints leads to the emergence of further unique features which are not exhibited by either non-relativistic quantum information or relativistic classical information; as part of this ongoing research programme we develop a new relativistic quantum `paradox' which puts pressure on conventional views about the spatiotemporal persistence of quantum states over time. We then study a new set of relativistic quantum protocols which involve the distribution of entangled states over spacetime, defining one task involving the distribution of the two halves of a known entangled state, and another task involving the distribution of the two halves of an unknown entangled state. The second part of the thesis deals with relativistic quantum cryptography, a field which first began attracting serious attention when it was realised that a cryptographic task known as `bit commitment,' can be implemented with perfect security under relativistic constraints. This result was highly significant, since it is provably impossible to implement bit commitment with perfect security in a purely classical or purely quantum context, and hence bit commitment is an ideal starting point for probing the power of relativistic quantum cryptography. In this thesis we propose several new relativistic quantum bit commitment protocols which have notable advantages over previously known protocols. We then move to a related task, a generalization of zero-knowledge proving which we refer to as knowledge-concealing evidencing of knowledge of a quantum state; we prove no-go theorems concerning the possibility of implementing this task with perfect security, and then set out a relativistic protocol for the task which is asymptotically secure as the dimension of the state in question becomes large. These results have interesting foundational significance above and beyond their applications in the field of cryptography, providing a new perspective on the connections between knowledge, realism and quantum states.

Quantum theory describes our universe incredibly successfully. To our classically-inclined brains, however, it is a bizarre description that requires a reimagining of what fundamental reality, or 'ontology', could look like. This thesis examines different ontological features in light of the success of quantum theory, what it requires, and what it rules out. While these investigations are primarily foundational, they also have relevance to quantum information, quantum communication, and experiments on quantum systems. The way that quantum theory describes the state of a system is one of its most unintuitive features. It is natural, therefore, to ask whether a similarly strange description of states is required on an ontological level. This thesis proves that almost all quantum superposition states for d &GT; 3 dimensions must be real - that is, present in the ontology in a well-defined sense. This is a strong requirement which prevents intuitive explanations of the many quantum phenomena which are based on superpositions. A new theorem is also presented showing that quantum theory is incompatible with macro-realist ontologies, where certain physical quantities must always have definite values. This improves on the Leggett-Garg argument, which also aims to prove incompatibility with macro-realism but contains loopholes. Variations on both of these results that are error-tolerant (and therefore amenable to experimentation) are presented, as well as numerous related theorems showing that the ontology of quantum states must be somewhat similar to the quantum states themselves in various specific ways. Extending these same methods to quantum communication, a simple proof is found showing that an exponential number of classical bits are required to communicate a linear number of qubits. That is, classical systems are exponentially bad at storing quantum data. Causal influences are another part of ontology where quantum theory demands a revision of our classical notions. This follows from the outcomes of Bell experiments, as rigorously shown in recent analyses. Here, the task of constructing a native quantum framework for reasoning about causal influences is tackled. This is done by first analysing the simple example of a common cause, from which a quantum version of Reichenbach's principle is identified. This quantum principle relies on an identification of quantum conditional independence which can be defined in four ways, each naturally generalising a corresponding definition for classical conditional independence. Not only does this allow one to reason about common causes in a quantum experiments, but it can also be generalised to a full framework of quantum causal models (mirroring how classical causal models generalise Reichenbach's principle). This new definition of quantum causal models is illustrated by examples and strengthened by it's foundation on a robust quantum Reichenbach's principle. An unusual, but surprisingly fruitful, setting for considering quantum ontology is found by considering time travel to the past. This provides a testbed for different ontological concepts in quantum theory and new ways to compare classical and quantum frameworks. It is especially useful for comparing computational properties. In particular, time travel introduces non-linearity to quantum theory, which brings (sometimes implicit) ontological assumptions to the fore while introducing strange new abilities. Here, a model for quantum time travel is presented which arguably has fewer objectionable features than previous attempts, while remaining similarly well-motivated. This model is discussed and compared with previous quantum models, as well as with the classical case. Together, these threads of investigation develop a better understanding of how quantum theory affects possible ontologies and how ontological prejudices influence quantum theory.

This thesis studies continuous variable mixed states with the aim of better understanding the fundamental behaviour of quantum correlations in such states, as well as searching for applications of these correlations. I first investigate the interesting phenomenon of discord increase under local loss and explain the behaviour by considering the non-orthogonality of quantum states. I then explore the counter-intuitive result where entanglement can be created by a passive optical beamsplitter, even if the input states are classical, as long as the input states are part of a larger globally nonclassical system. This result emphasises the importance of global correlations in a quantum state, and I propose an application of this protocol in the form of quantum dense coding. Finally, I develop a quantum digital signature protocol that can be described entirely using the continuous variable formalism. Quantum digital signatures provide a method to ensure the integrity and provenance of a message using quantum states. They follow a similar method to quantum key distribution (QKD), but require less post-processing, which means they can sometimes be implemented over channels that are inappropriate for QKD. The method I propose uses homodyne measurement to verify the signature, unlike previous protocols that use single photon detection. The single photon detection of previous methods is designed to give unambiguous results about the signature, but this comes at the cost of getting no information much of the time. Using homodyne detection has the advantage of giving results all the time, but this means that measurement results always have some ambiguity. I show that, even with this ambiguity, the signature protocol based on homodyne measurement outperforms previous protocols, with the advantage enhanced when technical considerations are included. Therefore this represents an interesting new direction in the search for a practical quantum digital signature scheme.

One of today’s challenges to realise computing based on quantum mechanics is to reliably and scalably encode information in quantum systems. Here, we present a photon source to on-demand deliver photonic quantum bits of information based on a strongly coupled atom-cavity system. The source operates intermittently for periods of up to 100 μs, with a single-photon repetition rate of 1 MHz, and an intra-cavity production efficiency of up to 85%. Our ability to arbitrarily control the photons’ wavepackets and phase profiles, together with long coherence times of 500 ns, allows to store time-bin encoded quantum information within a single photon. To do so, the spatio-temporal envelope of a single photon is sub-divided in d time bins which allows for the delivery of arbitrary qu-d-its. This is done with a fidelity of > 95% for qubits, and 94% for qutrits verified using a newly developed time-resolved quantum-homodyne measurement technique. Additionally, we combine two separate fields of quantum physics by using our deterministic single-photon source to seed linear optics quantum computing (LOQC) circuits. As a step towards quantum networking, it is shown that this photon source can be combined with quantum gates, namely a chip-integrated beam splitter, a controlled-NOT (CNOT) gate as well as a CNOT4 gate. We use this CNOT4 gate to entangle photons deterministically emitted from our source and observe non-classical correlations between events separated by periods exceeding the travel time across the chip by three orders of magnitude. Additionally, we use time-bin encoded qubits to systematically study the de- and re-phasing of quantum states as well as the the effects of time-varying internal phases in photonic quantum circuits.

The development of integrated quantum photonics is integral to many areas of quantum information science, in particular linear optical quantum computing. In this context, a diversity of physical systems is being explored and thus versatility and adaptability are important prerequisites for any candidate platform. Silicon oxynitride is a promising material because its refractive index can be varied over a wide range. This dissertation describes the development of silicon oxynitride waveguides for applications in the field of integrated quantum photonics. The project consisted of three stages: design, characterisation, and application. First, the parameter space was studied through simulations. The structures were optimised to achieve low-loss devices with a small footprint at a wavelength of 900 nm. Buried channel waveguides with a cross-section of 1.6 ?m x 1.6 ?m and a core (cladding) refractive index of 1.545 (1.505) were chosen. Second, following their fabrication with plasma-enhanced chemical vapour deposition, electron beam lithography, and reactive ion etching, the waveguides were characterised. The refractive index was shown to be tunable from the silica to the silicon nitride regime. Optimised tapers significantly improved the coupling efficiency. The minimum bend radius was measured to be less than 2 mm. Propagation losses as low as 1.45 dB cm-1 were achieved. Directional couplers with coupling ratios ranging from 0 to 1 were realised. Third, building blocks for linear optical quantum computing were demonstrated. Reconfigurable quantum circuits consisting of Mach-Zehnder interferometers with near perfect visibilities were fabricated along with a four-port switch. The potential of quantum speedup was illustrated by carrying out the Deutsch-Jozsa algorithm with a fidelity of 100 % using on-demand single photons from a quantum dot. This dissertation presents the first implementation of tunable Mach-Zehnder interferometers, which act on single photons, based on silicon oxynitride waveguides. Furthermore, for the first time silicon oxynitride photonic quantum circuits were operated with on-demand single photons. Accordingly, this work has created a platform for the development of integrated quantum photonics.

This thesis probes the usefulness of non-classical correlations within imperfect continuous variable decoherent quantum systems. Although a consistent function and practical usefulness of these correlations is largely unknown, it is important to examine their characteristics in more realistic dissipative systems, to gain further insight into any possible advantageous behaviour. A bipartite separable discordant state under the action of controlled loss on one subsystem was considered. Under these conditions the Gaussian quantum discord not only proved to be robust against loss, but actually improves as loss is intensified. Harmful imperfections which reduce the achievable level of discord can be counteracted by this controlled loss. Through a purification an explanation of this effect was sought by considering system-environment correlations, and found that a flow of system-environment correlations increases the quantumness of the state. Entanglement recovery possibilities were discussed and revealed the importance of hidden quantum correlations along bi-partitions across the discordant state and a classically prepared "demodulating" system, acting in such a way as to partially cancel the entanglement preventing noise. Entanglement distribution by separable states was studied by a similar framework, in an attempt to explain the emergence of quantum entanglement by a specific flow of correlations in the globally pure system. Discord appears to play a less fundamental role compared to the qubit version of the protocol. The strengthening of non-classical correlations can be attributed to a flow of classical and quantum correlations. This work proves that discord can be created in unique ways and, in select circumstances, can act to counteract harmful imperfections in the apparatus. Due to this advantageous behaviour discord indeed may ultimately aid in more applicable "real world" applications, which are by definition decoherent.

Spin properties of donor impurities in silicon have been investigated by electron spin resonance (ESR) techniques for more than sixty years. These studies gave us a contribution towards understanding some of the physics of doped semiconductor materials in general, which is the platform for much of our current technology. Despite the fact that donor electron and nuclear spins have been researched for so long, ESR studies of their properties are still giving us interesting insights. With the introduction of the concept of quantum information in the 1980s, some properties of donor spins in silicon, that were known from the fifties (such as long relaxations), have been reinterpreted for their potential application in this field. Since then, incredible experimental results have been achieved with magnetic resonance control, including manipulation and read-out of individual spins. However, some open questions are still to be answered before the realisation of a spin-based silicon quantum architecture will be achieved. Currently, ESR studies still contribute to help answering some of those questions. In this thesis, we demonstrate electrical and optical methods for donor charge state manipulation measured by ESR. Recent experiments have demonstrated that coherence time of nuclear spins may be enhanced by manipulating the state of donors from neutral to singly charged. We investigate electric field ionisation/neutralisation of arsenic donors in a silicon SOI device measured by ESR. Below ionisation threshold, we also measure the hyperfine Stark shift of arsenic donors spins in silicon. These results have, for instance, implications on how fast individual addressability of donor spins may be achieved in certain quantum computer architectures. Here, we also study optical-driven charge state manipulation of selenium impurities in silicon. Selenium has two additional electrons when it replaces an atom in the silicon crystal (i.e. double donor). The electronic properties of singly-ionised selenium make it potentially advantageous as spin qubit, compared to the more commonly studied group-V donors. For instance, we find here that the electron spin relaxation and coherence times of selenium are up to two orders of magnitude longer than phosphorus at the same temperature. Finally, we demonstrate that it is possible to bring selenium impurity in singly-charged state and subsequently re-neutralise them leaving a potential long-lived 77Se nuclear spin.

Quantum correlations play a fundamental role in quantum information science. The variety of their manifestations has become increasingly apparent following the development of novel light sources, protocols and photodetectors. One broad classification identifies two instances of non-classical correlations: particle and mode entanglement. These categories mirror two coexisting descriptions of quantum systems in terms of discrete and continuous variables of the electromagnetic field. The past decades have generated a number of promising results based on schemes which encompass elements from both frameworks, rather than viewing the two descriptions as mutually exclusive. In this context, it is possible to conceive and realise experiments where either the quantum resource or the detection system is 'hybrid'. Optical weak-field homodyne detectors bring together phase sensitivity and photon counting; as such, they represent a detection scheme which works across continuous and discrete variables of the radiation field. In this thesis we present a two-mode weak-field homodyne detection layout with added photon-number resolution and apply it to the study of a split single-photon state and a squeezed vacuum state. As a first test of the capabilities of this system, we investigate the reconstruction of relevant features of a given quantum resource - such as its photon statistics - with our detection scheme. Further, we experimentally demonstrate the observation of an instance of non-classical optical coherence which combines the continuous- and discrete-variable descriptions explicitly. The ability to probe phenomena at the interface of wave and particle regimes opens the way to novel, improved schemes for quantum information processing. From a more fundamental perspective, such hybrid approaches may shed light on the very roots of quantum enhancement.

Quantum memories are key components in photonics-based quantum information processing networks. Their ability to store and retrieve information on demand makes repeat-until-success strategies scalable. Warm alkali-metal vapours are interesting candidates for the implementation of such memories, thanks to their very long storage times as well as their experimental simplicity and versatility. Operation with the Raman memory protocol enables high time-bandwidth products, which denote the number of possible storage trials within the memory lifetime. Since large time-bandwidth products enable multiple synchronisation trials of probabilistically operating quantum gates via memory-based temporal multiplexing, the Raman memory is a promising tool for such tasks. Particularly, the broad spectral bandwidth allows for direct and technologically simple interfacing with other photonic primitives, such as heralded single photon sources. Here, this kind of light-matter interface is implemented using a warm caesium vapour Raman memory. Firstly, we study the storage of polarisation-encoded quantum information, a common standard in quantum information processing. High quality polarisation preservation for bright coherent state input signals can be achieved, when operating the Raman memory in a dual-rail configuration inside a polarisation interferometer. Secondly, heralded single photons are stored in the memory. To this end, the memory is operated on-demand by feed-forward of source heralding events, which constitutes a key technological capability for applications in temporal multiplexing. Prior to storage, single photons are produced in a waveguide-based spontaneous parametric down conversion source, whose bespoke design spectrally tailors the heralded photons to the memory acceptance bandwidth. The faithful retrieval of stored single photons is found to be currently limited by noise in the memory, with a signal-to-noise ratio of approximately 0.3 in the memory output. Nevertheless, a clear influence of the quantum nature of an input photon is observed in the retrieved light by measuring the read-out signal's photon statistics via the g(2)-autocorrelation function. Here, we find a drop in g(2) by more than three standard deviations, from g(2) ~ 1.69 to g(2) ~ 1.59 upon changing the input signal from coherent states to heralded single photons. Finally, the memory noise processes and their scalings with the experimental parameters are examined in detail. Four-wave-mixing noise is determined as the sole important noise source for the Raman memory. These experimental results and their theoretical description point towards practical solutions for noise-free operation.

Waveguide quantum electrodynamics, or wQED in short, has emerged as an exciting platform to explore strong light-matter interactions at the level of single photons and single atoms. The very nature of photons being guided and interacting with atoms residing at specific spots with respect to the waveguide modes offers exciting applications of the wQED platform to communicate and process quantum information over longer distances. With the advancement in optical fiber technologies and atom trapping techniques, it is now possible to experimentally test different theoretical proposals in this single setup. With this motivation, in this thesis, we have studied a few-photon transport, routing, localization, nonlinearity, and band structure in many-atom wQED in one-dimensional architectures and beyond. Our central focus throughout this thesis was to develop novel ways the different types of quantum interference effects can be used to control and engineer the transport of a few photons in this setup. Despite the availability of different theoretical tools to study many-body wQED, we have adopted the real-space formalism of quantum optics as our standard approach. On the application side, quantum networking and long-distance quantum communications are two areas in quantum information science that can find the results reported in this thesis helpful.

Quantum networks play an indispensable role in quantum information tasks such as secure communications, enhanced quantum sensing, and distributed computing. In recent years several platforms are being developed for such tasks, witnessing breakthrough technological advancement in terms of fabrication techniques, precise control methods, and information transfer. Among the most mature and promising platforms are color centers in solids. These systems provide an optically active electronic spin and long-lived nuclear spins for information storage. The first part of this dissertation is concerned with error mechanisms in the control of electronic and nuclear spins. First, I will focus on control protocols for improved electron-spin rotations tailored to specific color centers in diamond. I will then discuss how to manipulate the entanglement between the electron and the always-coupled nuclear spin register. I will describe a general formalism to quantify and control the generation of en- tanglement in an arbitrarily large nuclear spin register. This formalism incorporates exactly the dynamics with unwanted nuclei, and quantifies the performance of entangling gates in the presence of unwanted residual entanglement links. Using experimental parameters from a well-characterized multinuclear spin register, I will show that preparation of multipartite entanglement in a single-shot is possible, which drastically reduces the total gate time of conventional protocols. Then, I will present a new formalism for describing all-way entanglement and show how to design gates that prepare GHZM states. I will show how to incorporate errors such as unwanted correlations, electronic dephasing errors or pulse control errors. The second part of this thesis focuses on the preparation of all-photonic graph states from a few quantum emitters. I will introduce heuristic algorithms that exploit graph theory concepts in order to reduce the entangling gate counts, and also discuss the role of locally equivalent graphs in the optimization of the generation circuits.

Quantum Computation has attracted massive interest because of the recent technological advancement in both hardware and software suggesting the potential of quantum advantage. On the software side, hybrid classical-quantum algorithms are extensively studied as they can be implemented on the current noisy intermediate-scale quantum devices. On the hardware side, researchers are striving for faster and more noise-robustness quantum operations to achieve higher quantum processing power. The dissertation presents two topics in the above-mentioned aspects. The first one is constructing adaptive ans"atze for variational quantum eigensolver, one of the most promising hybrid algorithms. We present how to compress different required quantum resources by designing different ans"atze. The second topic is about designing fast entangling gates with a geometric approach. We show that the geometric approach can improve the existing numerical methods by locating the good initial guesses.

This PhD thesis contains a general introduction and three main chapters. Chapter 2 investigates Bell inequalities that generalize the CHSH and Braunstein-Caves inequalities. Chapter 3 shows a derivation of an upper bound on the success probability of a class of quantum teleportation protocols, denoted as port-based teleportation, from the no-cloning theorem and the no-signalling principle. Chapter 4 introduces the principle of quantum information causality. Chapter 2 considers the predictions of quantum theory and local hidden variable theories (LHVT) for the correlations obtained by measuring a pair of qubits by projections defined by randomly chosen axes separated by a given angle θ. The predictions of LHVT correspond to binary colourings of the Bloch sphere with antipodal points oppositely coloured. We show a Bell inequality for all θ, which generalizes the CHSH and the Braunstein-Caves inequalities in the sense that the measurement choices are not restricted to be in a finite set, but are constrained only by the angle θ. We motivate and explore the hypothesis that for a continuous range of θ > 0, the maximum correlation (anticorrelation) is obtained by assigning to one qubit the colouring with one hemisphere black and the other white, and assigning the same (reverse) colouring to the other qubit. We describe numerical tests that are consistent with this hypothesis and bound the range of θ. Chapter 3 shows a derivation of an upper bound on the success probability of port-based teleportation from the no-cloning theorem and the no-signalling principle. Chapter 4 introduces the principle of quantum information causality, a quantum version of the information causality principle. The quantum information causality principle states the maximum amount of quantum information that a transmitted quantum system can communicate as a function of its dimension, independently of any quantum physical resources previously shared by the communicating parties. These principles reduce to the no-signalling principle if no systems are transmitted. We present a new quantum information task, the quantum information causality game, whose success probability is upper bounded by the new principle, and show that an optimal strategy to perform it combines the quantum teleportation and superdense coding protocols with a task that has classical inputs.

Single atoms are promising candidates for physically implementing quantum bits, the fundamental unit of quantum information. We have built an apparatus for cooling, trapping and imaging single rubidium atoms in microscopic optical tweezers. The traps are formed from a tightly focused off-resonant laser beam, which traps atoms using the optical dipole force. The traps have a diameter of ~1 μm and a depth of ~1 mK. The novelty of our approach is the use a digital mirror device (DMD) to generate multiple independently movable tweezers from a single laser beam. The DMD consists of an array of micro-mirrors that can be switched on and off, thus acting as a binary amplitude modulator. We use the DMD to imprint a computer-generated hologram on the laser beam, which is converted in to the desired arrangement of traps in the focal plane of a lens. We have developed fast algorithms for calculating binary holograms suitable for the DMD. In addition, we use this method to measure and correct for errors in the phase of the wavefront caused by optical aberrations, which is necessary for producing diffraction-limited focal spots. Using this apparatus, we have trapped arrays of up to 20 atoms with arbitrary geometrical arrangements. We exploit light-assisted collisions between atoms to ensure there is at most one atom per trapping site. We measure the temperature of the atoms in the traps to be 12 μK, and their lifetime to be 1.4 s. Finally, we demonstrate the ability to select individual atoms from an array and transport them over a distance of 14μm with laser cooling, and 5 μm without.

Building complex quantum systems has the potential to reveal phenomena that cannot be studied using classical simulation. Photonics has proven to be an effective test-bed for the investigation of such quantum-enhanced technologies, however, the proliferation of bulk optical components is unlikely to be a scalable route towards building more complex devices. Instead, the miniaturisation, inherent phase stability and trivial alignment afforded by integrated photonic systems has been shown to be a promising alternative. In the first half of this thesis, we describe experiments exploiting the quantum interference of three single photons on a reconfigurable integrated photonic chip. We develop a low-loss source of single photons and introduce a low-loss silica-on-silicon waveguide architecture which enables us to show the first genuine quantum interference of three single photons on an integrated platform. A loss-tolerant, element-wise characterisation scheme is developed along with a statistical test to verify that this multi-photon circuit behaves as expected. We then make use of this three-photon interference to detail the first proof-of-principle demonstration of a new intermediate model of quantum computation called boson sampling. Finally, we perform an on-chip demonstration of the quantum teleportation protocol where all key parts --- entanglement preparation, Bell-state analysis and quantum state tomography --- are performed on a reconfigurable photonic chip. The element-wise characterisation scheme developed earlier is shown to be critical to mitigate fabricated component errors. We develop a theoretical model to account for all sources of possible error in the circuit and find good agreement with the measured teleported state fidelities, which exceed the average teleportation fidelity possible with a classical device. We identify the elements of this error budget relevant to scaling and propose improvements to chip characterisation and fabrication in order to achieve high fidelity operation. In the second half, we discuss the use of high efficiency superconducting transition edge sensors in enabling quantum experiments using more photons. We detail the installation and characterisation of these detectors in a new lab in Oxford. We achieve good photon number-resolution and high-efficiency operation. Work to integrate these detectors on the silica-on-silicon waveguide architecture is discussed and we detail the optical and thermal device modelling performed to optimise the on-chip detection efficiency. New, on-chip detectors, fabricated according to this design are shown to operate as expected and achieve high-efficiency and good energy resolution.

The preparation of single photons in a pure quantum state is a subject of great interest in physics, enabling the control of light at an unprecedented level. The ease with which certain degrees of freedom of photon states, such as polarisation, can be manipulated, along with the inherent resilience of photons to decoherence, makes them well suited for use as qubits. Recent rapid developments in the transmission and processing of quantum information, as well as the likely technological impact of potential real-world applications such as quantum cryptography and quantum computation, mean that the demand for high performance single photon sources is likely to increase in the near future. One approach to producing single photon states, which are known to be in a well-defined spatio-temporal mode without destructively measuring them, is to take advantage of nonlinear optics. Nonlinear processes can be used to realise frequency conversion by generating a single, correlated pair of photons from an intense pump laser source. The detection of one of the photons from a pair can then be used to indicate the presence of the other photon in the pair, a procedure known as heralding. This thesis describes the development of a source of heralded single photons at 1550 nm, generated directly in the core of a photonic crystal fibre (PCF). By taking advantage of low loss fibre components for the required spectral filtering of the generated photon state, a heralding fidelity of 52% was achieved. The source was designed to be used with a picosecond pulsed fibre laser, making it relatively low cost and maintenance free. With 148 mW of average pump power a heralded output photon rate of 6.4 × 104 s-1 was observed, demonstrating the brightness of the source. The purity of the generated single photons was established by measuring non-classical interference, with a visibility of 70%, between the photons output from this source and a source based on a PPLN waveguide. The fabrication of a series of birefringent PCFs for the generation of spectrally pure state photons at 1550 nm is also discussed. These PCFs will be useful for incorporation in the next generation of high performance, fibre-based photon sources.

Electrically detected magnetic resonance (EDMR) is a sensitive spectroscopic technique, which can be used to readout few to single electron spins in semiconductor and carbon nanodevices for applications in solid state quantum information processing (QIP). Since only electrically active defects contribute to the EDMR signal, this technique can be used further to investigate defects and impurities in photovoltaic devices, in which they limit the sunlight-to-energy conversion efficiency significantly. Here, I employ X-band EDMR for semiconductor defect analysis and identify the most important recombination centres in Czochralski silicon with oxide precipitates, which can be intentionally grown to confine detrimental metallic impurities to inactive regions of the wafer in order to serve as a defect-free substrate for modern silicon photovoltaic devices. Those experiments show that oxide precipitation is accompanied by the formation of silicon dangling bonds. Furthermore, I describe a very promising route towards the fabrication and readout of few to single electron spins in carbon nanotube devices, which can be characterised structurally via transmission electron microscopy in order to relate their electrical and spin properties with their structure. Finally, I employ EDMR to read out electron spin states in donor-doped silicon field-effect transistors as a prerequisite for their application in QIP. I report on a novel cryogenic probe head for EDMR experiments in resonant microwave cavities operating at 0.35 T (9.7 GHz, X-band) and 3.34 T (94 GHz, W-band). This approach overcomes the inherent limitations of conventional X-band EDMR and permits the investigation of paramagnetic states with a higher spectroscopic resolution and signal intensity. Both advantages are demonstrated and discussed. I further report on a novel mechanism giving rise to the EDMR effect in donor-doped silicon field-effect transistors, which is capable of explaining why the EDMR signal intensities of the conduction electrons are enhanced by a factor of ∼100, while the donor resonance signals increase by a factor of ∼20 from X- to W-band only. The spin-relaxation and dephasing times are extracted from a series of pulsed-EDMR measurements and confirm this model. The author gratefully acknowledges funding from Trinity College Oxford, Department of Materials, EPSRC DTA, and Konrad-Adenauer-Stiftung e.V. (Begabtenförderung).

Resource identification and quantification is an essential element of both classical and quantum information theory. Entanglement is one of these resources, arising when quantum communication and nonlocal operations are expensive to perform. In the first part of this thesis we quantify the effective entanglement when operations are additionally restricted to account for both fundamental restrictions on operations, such as those arising from superselection rules, as well as experimental errors arising from the imperfections in the apparatus. For an important class of errors we find a linear relationship between the usual and effective higher dimensional generalization of concurrence, a measure of entanglement. Following the treatment of effective entanglement, we focus on a related concept of nonlocality in the presence of superselection rules (SSR). Here we propose a scheme that may be used to activate nongenuinely multipartite nonlocality, in that a single copy of a state is not multipartite nonlocal, while two or more copies exhibit nongenuinely multipartite nonlocality. The states used exhibit the more powerful genuinely multipartite nonlocality when SSR are not enforced, but not when they are, raising the question of what is needed for genuinely multipartite nonlocality. We show that whenever the number of particles is insufficient, the degrading of genuinely multipartite to nongenuinely multipartite nonlocality is necessary. While in the first few chapters we focus our attention on understanding the resources present in quantum states, in the final part we turn the picture around and instead treat operations themselves as a resource. We provide our observers with free access to classical operations - ie. those that cannot detect or generate quantum coherence. We show that the operation of interest can then be used to either generate or detect quantum coherence if and only if it violates a particular commutation relation. Using the relative entropy, the commutation relation provides us with a measure of nonclassicality of operations. We show that the measure is a sum of two contributions, the generating power and the distinguishing power, each of which is separately an essential ingredient in quantum communication and information processing. The measure also sheds light on the operational meaning of quantum discord - we show it can be interpreted as the difference in superdense coding capacity between a quantum state and a classical state.

Categorical quantum mechanics is a way of formalising the structural features of quantum theory using category theory. It uses compound systems as the primitive notion, which is formalised by using symmetric monoidal categories. This leads to an elegant formalism for describing quantum protocols such as quantum teleportation. In particular, categorical quantum mechanics provides a graphical calculus that exposes the information flow of such protocols in an intuitive way. However, the graphical calculus also reveals surprising features of these protocols; for example, in the quantum teleportation protocol, information appears to flow `backwards-in-time'. This leads to question of how causal structure can be described within categorical quantum mechanics, and how this might lead to insight regarding the structural compatibility between quantum theory and relativity. This thesis is concerned with the project of formalising causal structure in categorical quantum mechanics. We begin by studying an abstract view of Bell-type experiments, as described by `no-signalling boxes', and we show that under time-reversal no-signalling boxes generically become signalling. This conflicts with the underlying symmetry of relativistic causal structure. This leads us to consider the framework of categorical quantum mechanics from the perspective of relativistic causal structure. We derive the properties that a symmetric monoidal category must satisfy in order to describe systems in such a background causal structure. We use these properties to define a new type of category, and this provides a formal framework for describing protocols in spacetime. We explore this new structure, showing how it leads to an understanding of the counter-intuitive information flow of protocols in categorical quantum mechanics. We then find that the formal properties of our new structure are naturally related to axioms for reconstructing quantum theory, and we show how a reconstruction scheme based on purification can be formalised using the structures of categorical quantum mechanics. Finally, we discuss the philosophical aspects of using category theory to describe fundamental physics. We consider a recent argument that category-theoretic formulations of physics, such as categorical quantum mechanics, can be used to support a variant of structural realism. We argue against this claim. The work of this thesis suggests instead that the philosophy of categorical quantum mechanics is subtler than either operationalism or realism.

Optical spin readout (OSR) in fullerene-based systems has the potential to solve the spin readout and scalability challenges in solid-state quantum information processing. While the rich variety of chemical groups that can be linked (covalently or not) to the fullerenes opens the possibility of making large and controlled arrays of qubits, optical methods can be used to measure EPR down to a single spin thanks to the large energy of optical photons compared to the microwave ones. After reviewing the state of the art of OSR, for which the diamond NV cen- ters constitute the benchmark, we undertake the study of fullerene-based species for OSR. An optically detected magnetic resonance (ODMR) setup was imple- mented in a commercial EPR spectrometer for this purpose. Each experimental chapter focuses on one of the molecular systems in question: a functionalised C60 fullerene with a phosphonate group (C60-phosphine), porphyrin-fullerene ar- chitectures (weakly, strongly and moderately coupled) and finally erbium-doped trimetallic nitride template (TNT) fullerenes (focusing on ErSc2N@C80). In the C60-phosphine system, coherent optically detected magnetic resonance (ODMR) in the triplet state has been achieved. Since a large variety of organic and organometallic molecules can be attached to it both via the fullerene cage and the phosponate group, this result makes it a very useful template to study OSR molecules chemically linked to a qubit. In the porphyrin based structures, an intermediate coupling case in the form of a trimer-fullerene host-guest complex is found to allow detection of both the porphyrin and fullerene triplet sates by CW ODMR, which makes organo-metallic complexes a possible coupling route for a qubit to an OSR component. In the TNT fullerene, crystal field mixing makes the Er3+ inaccessible by ODMR. However, optical photons cause a mechanical rearrangement of the en- dohedral cluster which in turns impacts on the observed EPR. In particular, the dynamics of this process have been studied for the first time and hint to- wards diffusion kinetics at low pump power. An orientational selectivity has been discovered by using a polarised pump, and the time dynamics indicate the rearrangement of the matrix via difusion on a free volume around the fullerenes. This shows that the endohedral Er3+ in ErSc2N@C80 can probe the environment outside the cage.

The highly parallel nature of the fundamental principles of quantum mechanics means that certain key resource-intensive tasks --- including searching, code decryption and medical, chemical and material simulations --- can be computed polynomially or even exponentially faster with a quantum computer. In spite of its remarkably fast development, the field of quantum computing is still young, and a large-scale prototype using any one of the candidate quantum bits (or 'qubits') under investigation has yet to be developed. Spin-based qubits in condensed matter systems are excellent candidates. Spins controlled using magnetic resonance have provided the first, most advanced, and highest fidelity experimental demonstrations of quantum algorithms to date. Despite having highly promising control characteristics, most physical ensembles investigated using magnetic resonance are unable to produce entanglement, a critical missing ingredient for a pure-state quantum computer. Quantum objects are said to be entangled if they cannot be described individually: they remain fundamentally linked regardless of their physical separation. Such highly non-classical states can be exploited for a host of quantum technologies including teleportation, metrology, and quantum computation. Here I describe how to experimentally create, control and characterise entangled quantum ensembles using magnetic resonance. I first explore the relationship between entanglement and quantum metrology and demonstrate a sensitivity enhancement over classical resources using molecular sensors controlled with liquid-state nuclear magnetic resonance. I then examine the computational potential of irreversible relaxation processes in combination with traditional reversible magnetic resonance control techniques. I show how irreversible processes can polarise both nuclear and electronic spins, which improves the quality of qubit initialisation. I discuss the process of quantum state tomography, where an arbitrary quantum state can be accurately measured and characterised, including components which go undetected using traditional magnetic resonance techniques. Lastly, I combine the above findings to initialise, create and characterise entanglement between an ensemble of electron and nuclear spin defects in silicon. I further this by generating pseudo-entanglement between an ensemble of nuclear spins mediated by a transient electron spin in a molecular system. These findings help pave the way towards a particular architecture for a scalable, spin-based quantum computer.

This thesis is about the experimental implementation of a high-speed and robust quantum memory for light. A novel far off-resonant Raman approach to ensemble-based quantum memories in a room-temperature environment is developed and demonstrated. Storage and retrieval of sub-nanosecond, weak coherent light pulses at the single-photon-level with total efficiencies exceeding 30% and storage times of up to 4 μs are achieved. The coherence of the memory is shown by directly interfering a copy of the incident signal with the retrieved signal from the memory. The unconditional noise floor of the memory is found to be low enough to operate the memory in the quantum regime at room temperature. Multiple readout of a single stored excitation is demonstrated, suggesting that 100% readout is possible in different temporal modes. Furthermore, first results regarding the storage and retrieval of polarisation encoded qubits are obtained. This and the memory’s ability to operate in the quantum regime at room temperature with a low unconditional noise floor illustrate its potential usefulness for real world applications.

This work is about diagrammatic languages, how they can be represented, and what they in turn can be used to represent. More specifically, it focuses on representations and applications of string diagrams. String diagrams are used to represent a collection of processes, depicted as "boxes" with multiple (typed) inputs and outputs, depicted as "wires". If we allow plugging input and output wires together, we can intuitively represent complex compositions of processes, formalised as morphisms in a monoidal category. While string diagrams are very intuitive, existing methods for defining them rigorously rely on topological notions that do not extend naturally to automated computation. The first major contribution of this dissertation is the introduction of a discretised version of a string diagram called a string graph. String graphs form a partial adhesive category, so they can be manipulated using double-pushout graph rewriting. Furthermore, we show how string graphs modulo a rewrite system can be used to construct free symmetric traced and compact closed categories on a monoidal signature. The second contribution is in the application of graphical languages to quantum information theory. We use a mixture of diagrammatic and algebraic techniques to prove a new classification result for strongly complementary observables. Namely, maximal sets of strongly complementary observables of dimension D must be of size no larger than 2, and are in 1-to-1 correspondence with the Abelian groups of order D. We also introduce a graphical language for multipartite entanglement and illustrate a simple graphical axiom that distinguishes the two maximally-entangled tripartite qubit states: GHZ and W. Notably, we illustrate how the algebraic structures induced by these operations correspond to the (partial) arithmetic operations of addition and multiplication on the complex projective line. The third contribution is a description of two software tools developed in part by the author to implement much of the theoretical content described here. The first tool is Quantomatic, a desktop application for building string graphs and graphical theories, as well as performing automated graph rewriting visually. The second is QuantoCoSy, which performs fully automated, model-driven theory creation using a procedure called conjecture synthesis.

This thesis describes experimental demonstrations of high-fidelity readout of trapped ion quantum bits ("qubits") for quantum information processing. We present direct single-shot measurement of an "optical" qubit stored in a single calcium-40 ion by the process of resonance fluorescence with a fidelity of 99.991(1)% (surpassing the level necessary for fault-tolerant quantum computation). A time-resolved maximum likelihood method is used to discriminate efficiently between the two qubit states based on photon-counting information, even in the presence of qubit decay from one state to the other. It also screens out errors due to cosmic ray events in the detector, a phenomenon investigated in this work. An adaptive method allows the 99.99% level to be reached in 145us average detection time. The readout fidelity is asymmetric: 99.9998% is possible for the "bright" qubit state, while retaining 99.98% for the "dark" state. This asymmetry could be exploited in quantum error correction (by encoding the "no-error" syndrome of the ancilla qubits in the "bright" state), as could the likelihood values computed (which quantify confidence in the measurement outcome). We then extend the work to parallel readout of a four-ion string using a CCD camera and achieve the same 99.99% net fidelity, limited by qubit decay in the 400us exposure time. The behaviour of the camera is characterised by fitting experimental data with a model. The additional readout error due to cross-talk between ion images on the CCD is measured in an experiment designed to remove the effect of qubit decay; a spatial maximum likelihood technique is used to reduce this error to only 0.2(1)x10^{-4} per qubit, despite the presence of ~4% optical cross-talk between neighbouring qubits. Studies of the cross-talk indicate that the readout method would scale with negligible loss of fidelity to parallel readout of ~10,000 qubits with a readout time of ~3us per qubit. Monte-Carlo simulations of the readout process are presented for comparison with experimental data; these are also used to explore the parameter space associated with fluorescence detection and to optimise experimental and analysis parameters. Applications of the analysis methods to readout of other atomic and solid-state qubits are discussed.