Quantum information processing (QIP) has the potential to reduce the complexity of many classically ‘hard’ computational problems. To implement quantum information algorithms, a suitable physical quantum computer architecture must be identified. One approach is to store quantum information in the electron spins of an array of paramagnetic N@C₆₀ endohedral fullerene molecules, using the electron-electron dipolar interaction to permit the formation of the entangled quantum states needed to implement QIP. This thesis explores two different chemical methods to create two-spin centre arrays that contain N@C₆₀. The first method uses a double 2,3 dipolar cycloaddition reaction to a dibenzaldehyde-terminated oligo-p-phenylene polyethynylene (OPE) unit , to create an (S_3/2, S_3/2) N@C₆₀-N@C₆₀ dimer with a fixed spin centre separation of 2.7 nm. The second approach is via a self-assembly scheme in which a Lewis base functionalised N@C₆₀ molecule coordinates to an antiferromagnetic metallic ring magnet to form a (S_3/2, S_3/2) two-spin centre N@C₆₀-Cr₇Ni system with an inter-spin separation of 1.4 nm. In both systems, a significant perturbation of the electron spin transition energies is observed using CW ESR, this perturbation is shown to be well accounted for by the inclusion of an electron-electron dipolar coupling term in the electron spin Hamiltonians. To create entanglement in an ensemble of two-spin centre molecules, the dipolar coupling interaction must lie within a narrow distribution. To achieve this not only the separation but also the orientation of the inter-spin axis with respect to the applied magnetic field must be controlled for which a method of macroscopic alignment is required. The potential of using a uniaxially drawn liquid crystal elastomer to exert uniaxial order on fullerene dimers is tested, finding that the degree of alignment is insufficient, possibly a result of the propensity for the fullerene molecules to phase separate from the elastomer. This phase separation is shown to restrict N@C₆₀ phase coherence lifetime to 1.4 µs at 40 K due to instantaneous spin diffusion. The electron spin environment of both N@C₆₀ and an N@C₆₀-C₆₀ dimer in a polymer matrix is examined using polystyrene as the host matrix. By deuteration of the polystyrene matrix, a maximum phase coherence lifetimes of 48 µs and 21 µs are measured for the N@C₆₀ and N@C₆₀-C₆₀ dimer, respectively. The concept of reading out the electron spin state of N@C₆₀ molecules by coupling it to a spin system that can be probed using optically detected magnetic resonance (ODMR) such as an NV- centre has been previously suggested. To this end, the photostability of N@C₆₀ under 637 nm laser illumination has been examined in solution. The effect of the presence of an atmospheric concentration of oxygen is striking, affording a 57-fold retardation in the photodecomposition of N@C₆₀ compared to a degassed solution. When ambient oxygen is present, the average number of excitations that are required to cause decomposition is ≈60000. Finally, for future UV photophysics experiments involving N@C₆₀, the best solvent to use was found to be decalin, finding that it significantly slowed decomposition of N@C₆₀ in both ambient and degassed solutions. The conclusions of this work make a significant contribution to the field of QIP with N@C₆₀, showing that there is a bright future for N@C₆₀.

In this thesis I discuss the nature of ‘measurement’ in quantum theory. ‘Measurement’ is associated with several different processes: the gradual imprinting of information about one system onto another, which is well understood; the collapse of the wavefunction, which is ill-defined and troublesome; and finally, the means by which inferences about unknown experimental parameters are made. I present a theoretical extension to an experimental proposal from Leggett and Garg, who suggested that the quantum-or-classical reality of a macroscopic system may be probed with successive measurements arrayed in time. The extension allows for a finite level of imperfection in the protocol, and makes use of Leggett’s ‘null result’ measurement scheme. I present the results of an experiment conducted in Oxford that, up to certain loopholes, defies a non-quantum interpretation of the dynamics of phosphorous nuclei embedded in silicon. I also present the theory of statistical parameter estimation, and discover that a recent trend to employ time symmetric ‘postselected’ measurements offers no true advantage over standard methods. The technique, known as weak-value amplification, combines a weak transfer of quantum information from system to meter with conditional data rejection, to surprising effect. The Fisher information is a powerful tool for evaluating the performance of any parameter estimation model, and it reveals the technique to be worse than ordinary, preselected only measurements. That this is true despite the presence of noise (including magnetic field fluctuations causing deco- herence, poor resolution detection, and random displacements), casts serious doubt on the utility of the method.

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).

The provision of compositionality in distributional models of meaning, where a word is represented as a vector of co-occurrence counts with every other word in the vocabulary, offers a solution to the fact that no text corpus, regardless of its size, is capable of providing reliable co-occurrence statistics for anything but very short text constituents. The purpose of a compositional distributional model is to provide a function that composes the vectors for the words within a sentence, in order to create a vectorial representation that re ects its meaning. Using the abstract mathematical framework of category theory, Coecke, Sadrzadeh and Clark showed that this function can directly depend on the grammatical structure of the sentence, providing an elegant mathematical counterpart of the formal semantics view. The framework is general and compositional but stays abstract to a large extent. This thesis contributes to ongoing research related to the above categorical model in three ways: Firstly, I propose a concrete instantiation of the abstract framework based on Frobenius algebras (joint work with Sadrzadeh). The theory improves shortcomings of previous proposals, extends the coverage of the language, and is supported by experimental work that improves existing results. The proposed framework describes a new class of compositional models thatfind intuitive interpretations for a number of linguistic phenomena. Secondly, I propose and evaluate in practice a new compositional methodology which explicitly deals with the different levels of lexical ambiguity (joint work with Pulman). A concrete algorithm is presented, based on the separation of vector disambiguation from composition in an explicit prior step. Extensive experimental work shows that the proposed methodology indeed results in more accurate composite representations for the framework of Coecke et al. in particular and every other class of compositional models in general. As a last contribution, I formalize the explicit treatment of lexical ambiguity in the context of the categorical framework by resorting to categorical quantum mechanics (joint work with Coecke). In the proposed extension, the concept of a distributional vector is replaced with that of a density matrix, which compactly represents a probability distribution over the potential different meanings of the specific word. Composition takes the form of quantum measurements, leading to interesting analogies between quantum physics and linguistics.

The progess in NMRQIP can be outlined in to four parts.1) Implementation of theoretical protocols on small number of qubits. 2) Demonstration of QIP on various NMR systems. 3) Designing and implementing the algorithms for mixed initial states. 4) Developing the techniques for coherent and decoherent control on higher number(up to 15) of qubits. This thesis contains some efforts in the direction of first three points. Quantum-state discrimination has important applications in the context of quantum communication and quantum cryptography. One of the characteristic features of quantum mechanics is that it is impossible to devise a measurement that can distinguish nonorthogonal states perfectly. However, one can distinguish them with a finite probability by an appropriate measurement strategy. In Chapter 2, we describe the implementation of a theoretical protocol of programmable quantum-state discriminator, on a two-qubit NMR System. The projective measurement is simulated by adding two experiments. This device does the unambiguous discrimination of a pair of states of the data qubit that are symmetrically located about a fixed state. The device is used to discriminate both linearly polarized states and eillipitically polarized states. The maximum probability of successful discrimination is achieved by suitably preparing the ancilla quubit. The last step of any QIP protocol is the readout. In NMR-QIP the readout is done by using density matrix tomography. It was first proposed by Ernst and co-workers that a two-dimensional method can be used to correlate input and output states. This method uses an extra (aniclla) qubit, whose transitions indicate the quantum states of the remaining qubits. The 2D spectrum of ancilla qubit represent the input and output states along F1 and F2 dimensions respectively. However the 2D method requires several t1 increments to achieve the required spectral width and resolution in the indirect dimension, hence leads to large experimental time. In chapter 3, the conventional 2D NMRQIP method is speeded-up by using Hadamard spectroscopy. The Hadamard method is used to implement various two-, three-qubit gates and qutrit gates. We also use Hadamard spectroscopy for information storage under spatial encoding and to implement a parallel search algorithm. Various slices of water sample can be spatially encoded by using a multi-frequency pulse under the field gradient. Thus the information of each slice is projected to the frequency space. Each slice represents a classical bit, where excitation and no excitation corresponds to the binary values 0 and 1 respectively. However one has to do the experiment for each binary information, by synthesizing a suitable multi-frequency pulse. In this work we show that by recording the data obtained by various Hadamard encoded multi-frequency pulses, one can suitably decode it to obtain any birnary information, without doing further experiments. Geometric phases depend only on the geometry of the path executed in the projective Hilbert space, and are therefore resilient to certain types of errors. This leads to the possibility of an intrinsically fault-tolerant quantum computation. In liquid state NMRQIP. Controlled phase shift gates are achieved by using qubit selective pulses and J evolutions, and also by using geometir phases. In order to achieve higher number of qubits in NMR, one explores dipolar couplings which are larger in magnitude, yielding strongly coupled spectra. In such systems since the Hamiltonian consists of terms, it is difficult to apply qubit selective pulses. However such systems have been used for NMRQIP by considering 2n eigen states as basis states of an n-qubit system. In chapter 4, it is shown that non-adiabatic geometric phases can be used to implement controlled phase shift gates in strongly dipolar coupled systems. A detailed theoretical explanation of non-adiabatic geometric phases in NMR is given, by using single transition operators. Using such controlled phase shift gates, the implementation of Deutsch-Jozsa and parity algorithms are demonstrated. Search algorithms play an important role in the filed of information processing. Grovers quantum search algorithm achieves polynomial speed-up over the classical search algorithm. Bruschweiler proposed a Liouville space search algorithm which achieve polymonial speed-up. This algorithm requires a weakly coupled system with a mixed initial state. In chapter 5 we modified the Bruschweiler’s algorithm, so that it can be implemented on a weakly as well as strongly coupled system. The experiments are performed on a strongly dipolar coupled four-qubit system. The experiments from four spin-1/2 nuclei of a molecule oriented in a liquid crystal matrix. Chapter 6 describes the implementation of controlled phase shift gates on a quadrupolar spin-7/2 nucleus, using non-adiabatic geometric phases. The eight energy levels of spin-7/2 nucleus, form a three qubit system. A general procedure is given, for implementing a controlled phase shift gate on a system consisting of any number of energy levels. Finally Collin’s version of three-qubit DJ algorithm using multi-frequency pulses, is implemented in the spin-7/2 system.

Superconducting qubits are a promising technology for building a scalable quantum computer. An important architecture employed in the field is called Circuit Quantum Electrodynamics (circuit QED), where such qubits are combined with high quality microwave cavities to study the interaction between artificial atoms and single microwave photons. The ultra-strong coupling achieved in these systems allows for control and readout of the quantum state of qubits to perform quantum information processing. The work on circuit QED performed in this thesis consisted of realizing an experimental setup for qubit experiments in a new laboratory, investigating the coherence and decay of higher energy levels of superconducting transmon qubits and finally demonstrating a novel coaxial form of circuit QED. Designing and building a 3D circuit QED setup involved the following main accomplishments: producing high quality 3D cavities; designing and installing the cryogenic microwave setup as well as the room temperature amplification and data acquisition circuitry; successfully developing a recipe for the fabrication of Josephson junctions; controlling and measuring superconducting 3D transmon qubits at 10mK. Several qubits were fully characterised and have shown coherence times of several microseconds and relaxation times up to 25μs. Superconducting qubits in fact possess higher energy levels that can provide significant computational advantages in quantum information applications. In experiments performed at MIT, preparation and control of the five lowest states of a transmon qubit was demonstrated, followed by an investigation of the phase coherence and decay dynamics of these higher energy levels. The decay was found to proceed mainly sequentially with relaxation times in excess of 20μs for all transitions. A direct measurement of the charge dispersion of these levels was performed to explore their characteristics of dephasing. This experiment was also reproduced on a 3D transmon fabricated and measured in Oxford, where due to a higher effective qubit temperature a multi-level decay model including thermal excitations was developed to explain the observed relaxation dynamics. Finally, a coaxial transmon, which we name the coaxmon, is presented and measured with a coaxial LC readout resonator and input/output coupling ports placed inline along the third dimension. This novel coaxial circuit QED architecture holds great promise for developing a scalable planar grid of qubits to build a quantum computer.

Le formalisme des états graphes consiste à modéliser des états quantiques par des graphes. Ce formalisme permet l'utilisation des notions et des outils de théorie des graphes (e.g. flot, domination, méthodes probabilistes) dans le domaine du traitement de l'information quantique. Ces dernières années, cette modélisation combinatoire a permis plusieurs avancées décisives, notamment (i) dans la compréhension des propriétés de l'intrication quantique (ii) dans l'étude des modèles de calcul particulièrement prometteurs en terme d'implémentation physique, et (iii) dans l'analyse et la construction de protocoles de cryptographie quantique. L'objectif de cette thèse est d'étudier les propriétés graphiques émergeant des problématiques d'informatique quantique, notamment pour la simulation quantique. En particulier, l'étude des propriétés de causalité et de localité des états graphes, en étendant par exemple la notion existante de flot de causalité à une notion intégrant des contraintes de localité, permettrait d'ouvrir de nouvelles perspectives pour la simulation de systèmes quantiques à l'aide d'états graphes. Des connections formelles avec les automates cellulaires quantiques bruités pourront également émerger de cette étude. / Graph States formalism consist in using graphs to model quantum states. This formalism allows us to use notion and tools of graph theory (e.g. flow, domination, probabilistic methods) in quantum information processing. Last years, this combinatorial modelisation had lead to many decisiv breakthroughs, in particular (i) in the comprehension of the quantum entranglement properties (ii) in very promising in term of physical implementation quantum calculus model, and (iii) in the analysis and construction of quantum cryptography protocols. The goal of this thesis is to study the graphic properties emerging of those quantum information processing problematics, especially for quantum simulation. In particular, the properties of causality and locality in graph states, by extanding for exemple the existing notion of causality flows to a notion integring the locality constraints, would allow new perspectives for the quantum system simulation using graphs states. Formal connections with noisy quantum cellular automata would emerge from this study.

Quantum simulations, where controllable quantum systems are used to simulate other quantum systems, originally proposed by Richard Feynman, are one of the most remarkable applications of quantum information science. Compared to computation, quantum simulations require much less number of qubits for the m to be practical. In the work described in this thesis, we have performed a few quantum simulations of small quantum systems using Nuclear Magnetic Resonance(NMR) techniques. These simulations have been used to experimentally demonstrate the underlying interesting quantum protocols. All the experiments presented have been carried out using liquid-state or liquid crystal NMR. Numerical pulse optimization techniques have been utilized in some of the experiments, to achieve better control over the spin systems. The first chapter contains “Introduction” to quantum information processing, NMR, and numerical pulse optimization techniques. In chapter 2, we describe quantum simulation of a 3-spin Heisenberg-XY spin chain having only nearest neighbour interactions. Recently, spin chains having pre-engineered short-range interactions have been proposed to efficiently transfer quantum information between different parts of a quantum information processor. Other important proposals involving these spin chains include generating entangled states and universal quantum computation. However, such engineered interactions do not occur naturally in any system. In such a scenario, the experimental viability of these proposals can be tested by simulating the spin chains in other controllable quantum systems. In this work, we first theoretically study the time evolution of bipartite and tripartite entanglement measures for a 3-spin open ended XY spin chain. Then, by simulating the XY interactions in a 3-spin nuclear spin system, we experimentally generate, (i)a bipartite maximally(pseudo-)entangled state(Bell state) between end qubits, and(ii) multipartite(pseudo-)entangled states(Wand GHZ states),starting from separable pseudo-pure states. Bell state has been generated by using only the natural unitary evolution of the XY spin chain. W-state and GHZ-state have been generated by applying a single-qubit rotation to the second qubit, and a global rotation of all the three qubits respectively after the unitary evolution of the spin chain. In chapter 3, we simulate a 3-spin quantum transverse Ising spin system in a triangular configuration, and show that multipartite quantum correlations can be used to distinguish between the frustrated and non-frustrated regimes in the ground state of this spin system. The ground state of the spin system has been prepared by using adiabatic state preparation method. Gradient ascent pulse engineering technique has been utilized to efficiently realize the adiabatic evolution of the spin system. To analyse the experimental ground state of the system, we employ two different multipartite quantum correlation measures, generated from monogamy studies of bipartite quantum correlations. Chapter 4 contains a digital quantum simulation of the mirror inversion propagator corresponding to the time evolution of an XY spin chain. This simulation has been used to experimentally demonstrate the mirror inversion of quantum states, proposed by Albanese et al.[Phys.Rev.Lett.93,230502(2004)], by which entangled states can be transferred from one end of the chain to the other end. The experiments have been performed in a 5-qubit dipolar coupled nuclear spin system. For simulation, we make use of the recently proposed unitary operator decomposition algorithm along with the numerical pulse optimization techniques, which assisted in achieving high experimental fidelities. Chapter 5 contains a digital quantum simulation of the unitary propagator of a transverse Ising spin chain, which has been used to experimentally demonstrate the perfect state transfer protocol of Di Franco et al. [Phys.Rev.Lett.101,230502(2008)]. The importance of this protocol arises due to the fact that it achieves perfect state transfer from one end of the chain to the other end without the necessity of initializing the intermediate spins of the chain, whereas most of the previously proposed protocols require initialization. The experiments have been performed in a 3-spin nuclear spin system. The simulation has also been used to demonstrate the generation of a GHZ state.

Thèse numérisée par la Division de la gestion de documents et des archives de l'Université de Montréal.

In dieser Doktorarbeit werden zwei Konzepte der Quanteninformationsverarbeitung realisiert. Der Quantenschlüsselaustausch ist revolutionär, weil er perfekte Sicherheit gewährleistet. Zahlreiche Quantenkryptografieprotokolle wurden schon untersucht. Zwei Probleme bestehen. Zum einen ist es sehr schwer, die Bedingungen herzustellen, die in den Annahmen für perfekte Sicherheit impliziert sind. Zum anderen sind die Reichweiten auf momentan etwa 200 km begrenzt, aufgrund des abnehmenden Signals gegenüber des konstanten Rauschens. Ein Experiment dieser Doktorarbeit beschäftigt sich mit dem ersten Problem. Insbesondere der übertragene Quantenzustands ist kritisch für die Sicherheit des Verfahrens. Es werden Einzelphotonen von Stickstoff- Fehlstellen-Zentren und zum ersten Mal von Silizium-Fehlstellen-Zentren für einen Quantenschlüsselaustausch mit Hilfe des BB84-Protokolls benutzt. Die Abweichung von idealen Einzelphotonenzuständen sowie deren Bedeutung für die Sicherheit werden analysiert. Die Übertragung von Quantenzuständen via Satellit könnte das Problem der begrenzten Reichweite lösen. Das neue Frequenz-Zeit- Protokoll eignet sich dafür besonders gut. Es wird während dieser Arbeit zum ersten Mal überhaupt implementiert. Umfangreiche Untersuchungen inklusive der Variation wesentlicher experimenteller Parameter geben Aufschluss über die Leistungsfähigkeit und Sicherheit des Protokolls. Außerdem werden elementare Bestandteile eines vollautomatischen Experiments zum Quantenschlüsselaustausch über Glasfasern in der sogenannten Time-bin-Implementierung mit autonomem Sender und Empfänger realisiert. Ein anderes Konzept der Quanteninformationsverarbeitung ist die Herstellung zufälliger Bitfolgen durch den Quantenzufall. Zufällige Bitfolgen haben zahlreiche Anwendungsgebiete in der Kryptografie und der Informatik. Die Realisierung eines Quantenzufallszahlengenerators mit mathematisch beschreibbarer und getesteter Zufälligkeit und hoher Bitrate wird ebenfalls beschrieben. / In this thesis, photonic quantum states are used for experimental realisations of two different concepts of quantum information processing. Quantum key distribution (QKD) is revolutionary because it is the only cryptographic scheme offering unconditional security. Two major problems prevail: Firstly, matching the conditions for unconditional security is challenging, secondly, long distance communication beyond 200 km is very demanding because an increasingly attenuated quantum state starts to fail the competition with constant noise. One experiment accomplished in this thesis is concerned with the first problem. The realisation of the actual quantum state is critical. Single photon states from nitrogen and for the first time also silicon vacancy defect centres are used for a QKD transmission under the BB84 (Bennett and Brassard 1984). The deviation of the used single photon states from the ideal state is thoroughly investigated and the information an eavesdropper obtains due to this deviation is analysed. Transmitting quantum states via satellites is a potential solution to the limited achievable distances in QKD. A novel protocol particularly suited for this is implemented for the first time in this thesis, the frequency-time (FT) protocol. The protocol is thoroughly investigated by varying the experimental parameters over a wide range and by evaluating the impact on the performance and the security. Finally, big steps towards a fully automated fibre-based BB84 QKD experiment in the time-bin implementation with autonomous sender and receiver units are accomplished. Another important concept using quantum mechanical properties as a resource is a quantum random number generator (QRNG). Random numbers are used for various applications in computing and cryptography. A QRNG supplying bits with high and quantifiable randomness at a record-breaking rate is reported and the statistical properties of the random output is thoroughly tested.