Quantum information processing (QIP), which inherently utilizes quantum mechanical phenomena to perform information processing, may outperform its classical counterpart at certain tasks. As one of the physical implementations of QIP, the electron-spin based architecture has recently attracted great interests. Endohedral fullerenes with unpaired electrons, such as N@C₆₀, are promising candidates to embody the qubits because of their long spin decoherence time. This thesis addresses several fundamental aspects of the strategy of engineering the N@C₆₀ molecules for applications in QIP. Chemical functionalization of N@C₆₀ is investigated and several different derivatives of N@C₆₀ are synthesized. These N@C₆₀ derivatives exhibit different stability when they are exposed to ambient light in a degassed solution. The cyclopropane derivative of N@C60 shows comparable stability to pristine N@C₆₀, whereas the pyrrolidine derivatives demonstrate much lower stability. To elucidate the effect of the functional groups on the stability, an escape mechanism of the encapsulated nitrogen atom is proposed based on DFT calculations. The escape of nitrogen is facilitated by a 6-membered ring formed in the decomposition of the pyrrolidine derivatives of N@C₆₀. In contrast, the 4-membered ring formed in the cyclopropane derivative of N@C₆₀ prohibits such an escape through the addends. Two N@C₆₀-porphyrin dyads are synthesized. The dyad with free base porphyrin exhibits typical zero-field splitting (ZFS) features due to functionalization in the solid-state electron spin resonance (ESR) spectrum. However, the nitrogen ESR signal in the second dyad of N@C₆₀ and copper porphyrin is completely suppressed at a wide range of sample concentrations. The dipolar coupling between the copper spin and the nitrogen spins is calculated to be 27.0 MHz. To prove the presence of the encapsulated nitrogen atom in the second dyad, demetallation of the copper porphyrin moiety is carried out. The recovery of approximately 82% of the signal intensity confirms that the dipolar coupling suppresses the ESR signal of N@C₆₀. To prepare ordered structure of N@C₆₀, the nematic matrix MBBA is employed to align the pyrrolidine derivatives of N@C₆₀. Orientations of these derivatives are investigated through simulation of their ESR spectra. The derivatives with a –CH3 or phenyl group derived straightforward from the N-substituent of the pyrrolidine ring are preferentially oriented based on their powder-like ESR spectra in the MBBA matrix. An angle of about is also found between the directors of fullerene derivatives and MBBA. In contrast, the derivatives with a –CH₂ group inserted between the phenyl group and the pyrrolidine ring are nearly randomly distributed in MBBA. These results illustrate the applicability of liquid crystal as a matrix to align N@C₆₀ derivatives for QIP applications.

Neste trabalho exploramos o emaranhamento em sistemas de muitos férmions. Para o estudo de sistemas inomogêneos, propusemos uma aproximação de densidade local (LDA) para a entropia de emaranhamento de um único sítio com o restante do sistema e uma LDA para o emaranhamento entre blocos de sítios. Analisamos as contribuições universal e não-universal do emaranhamento entre blocos e obtivemos uma expressão para o termo não-universal. Usando o modelo de Hubbard unidimensional, investigamos o emaranhamento em nanoestruturas eletrônicas, quantificando o emaranhamento de um único sítio com relação ao restante da cadeia via entropia de emaranhamento. Para o modelo de Hubbard homogêneo estudamos o comportamento do emaranhamento em função da densidade, da magnetização, da interação eletrônica e de campos magnéticos externos. Encontramos que o emaranhamento é sensível às fases metálica, isolante e supercondutora. Observamos um platô de emaranhamento na região do gap de spin e verificamos que susceptibilidade magnética e emaranhamento estão intrinsecamente relacionados. Obtendo as energias e densidades do modelo de Hubbard inomogêneo através da Teoria do Funcional da Densidade e usando nossa proposta LDA para a entropia de emaranhamento, exploramos o comportamento do emaranhamento na presença de diversas inomogeneidades: superredes, impurezas e confinamento harmônico. Verificamos que o emaranhamento sempre diminui com a inomogeneidade, embora os efeitos de cada inomogeneidade sejam completamente diferentes. Encontramos uma relação entre energias de troca e correlação, de Hartree e cinética, capaz de prever quantitativamente o emaranhamento em função de qualquer das inomogeneidades. / In this work we investigated entanglement in many-fermions systems. To explore inhomogeneous systems we proposed a local density approximation (LDA) for the single-site entanglement entropy. We analysed the universal and nonuniversal contributions to block-block entanglement and obtained an expression for the nonuniversal term. We employ a description in terms of the one-dimensional Hubbard model to investigate the entanglement in electronic nanostructures and to quantify the single-site entanglement with respect to the rest of the chain by means of the entanglement entropy. For the homogeneous Hubbard model we studied the entanglement behavior as a function of density, magnetization, electronic interaction and external magnetic fields. We found that the entanglement is sensitive to the metallic, insulating and superconducting phases. We observed an entanglement plateau in the region of the spin gap and verified that magnetic susceptibility and entanglement are intrinsically related. Energies and densities of the inhomogeneous Hubbard model, obtained from Density Functional Theory, combined with our proposal of an LDA for the entanglement entropy, were used to explore the behavior of the entanglement entropy in the presence of several inhomogeneities: superlattices, impurities and harmonic confinement. We verified that entanglement always decreases with the inhomogeneity, although the effect of each inhomogeneity is completely different. For the same model we found a relation of exchange-correlation, Hartree and kinetic energies, able to predict quantitatively the entanglement as a function of any inhomogeneity.

Neste trabalho exploramos o emaranhamento em sistemas de muitos férmions. Para o estudo de sistemas inomogêneos, propusemos uma aproximação de densidade local (LDA) para a entropia de emaranhamento de um único sítio com o restante do sistema e uma LDA para o emaranhamento entre blocos de sítios. Analisamos as contribuições universal e não-universal do emaranhamento entre blocos e obtivemos uma expressão para o termo não-universal. Usando o modelo de Hubbard unidimensional, investigamos o emaranhamento em nanoestruturas eletrônicas, quantificando o emaranhamento de um único sítio com relação ao restante da cadeia via entropia de emaranhamento. Para o modelo de Hubbard homogêneo estudamos o comportamento do emaranhamento em função da densidade, da magnetização, da interação eletrônica e de campos magnéticos externos. Encontramos que o emaranhamento é sensível às fases metálica, isolante e supercondutora. Observamos um platô de emaranhamento na região do gap de spin e verificamos que susceptibilidade magnética e emaranhamento estão intrinsecamente relacionados. Obtendo as energias e densidades do modelo de Hubbard inomogêneo através da Teoria do Funcional da Densidade e usando nossa proposta LDA para a entropia de emaranhamento, exploramos o comportamento do emaranhamento na presença de diversas inomogeneidades: superredes, impurezas e confinamento harmônico. Verificamos que o emaranhamento sempre diminui com a inomogeneidade, embora os efeitos de cada inomogeneidade sejam completamente diferentes. Encontramos uma relação entre energias de troca e correlação, de Hartree e cinética, capaz de prever quantitativamente o emaranhamento em função de qualquer das inomogeneidades. / In this work we investigated entanglement in many-fermions systems. To explore inhomogeneous systems we proposed a local density approximation (LDA) for the single-site entanglement entropy. We analysed the universal and nonuniversal contributions to block-block entanglement and obtained an expression for the nonuniversal term. We employ a description in terms of the one-dimensional Hubbard model to investigate the entanglement in electronic nanostructures and to quantify the single-site entanglement with respect to the rest of the chain by means of the entanglement entropy. For the homogeneous Hubbard model we studied the entanglement behavior as a function of density, magnetization, electronic interaction and external magnetic fields. We found that the entanglement is sensitive to the metallic, insulating and superconducting phases. We observed an entanglement plateau in the region of the spin gap and verified that magnetic susceptibility and entanglement are intrinsically related. Energies and densities of the inhomogeneous Hubbard model, obtained from Density Functional Theory, combined with our proposal of an LDA for the entanglement entropy, were used to explore the behavior of the entanglement entropy in the presence of several inhomogeneities: superlattices, impurities and harmonic confinement. We verified that entanglement always decreases with the inhomogeneity, although the effect of each inhomogeneity is completely different. For the same model we found a relation of exchange-correlation, Hartree and kinetic energies, able to predict quantitatively the entanglement as a function of any inhomogeneity.

<p>Optimization and Machine learning (ML) have emerged as two positively disruptive methodologies and have thus resulted in unprecedented applications in several domains of technology. In recent years, ML has forayed into physical sciences and provided promising outcomes thanks to its ability in representing and generalizing complex functions to reveal underlying relations among variables describing a system. By casting ML as an optimization task, we first focus on its application in solving quantum many-body problems. Leveraging the power of quantum computation, we develop hybrid quantum machine learning protocols and implement benchmark tests to calculate the band structures of two-dimensional materials. We also show how this method can be used to estimate the critical point for a quantum phase transition. One  hurdle in such techniques is related to parameter optimization, wherein to obtain the desired result, the parameters have to be optimized, which can be computationally intensive. For a particular class of problem and a choice of algorithm, we deduce a simple parameter setting rule. This rule is projected as a heuristic and is validated numerically for several problem instances. Finally, by venturing into thermal photonics, a framework that takes advantage of the spectral and spatial information of hyperspectral thermal images to establish a completely passive machine perception, titled HADAR is presented. A conventional deep neural network is developed that utilizes the governing equation of HADAR and its performance in semantic segmentation is demonstrated. Altogether, this report establishes the need for creative algorithms that exploit modern hardware to solve complex problems that were previously deemed unsolvable.</p>

Developments in the interdisciplinary field of quantum information open up previously impossible abilities in the realms of information processing and communication. Quantum entanglement has emerged as one property of quantum systems that acts as a resource for quantum information processing and, in particular, enables teleportation and secure cryptography. Therefore, the creation of entangled resources is of key importance for the application of these technologies. Despite a great deal of research the efficient creation of entanglement over long distances is limited by inevitable noise. This problem can be overcome by creating entanglement between nodes in a network and then performing operations to distribute the entanglement over a long distance. This thesis contributes to the field of entanglement distribution within such quantum networks. Entanglement distribution has been extensively studied for one-dimensional networks resulting in "quantum repeater" protocols. However, little work has been done on higher dimensional networks. In these networks a fundamentally different scaling, called "long distance entanglement distribution", can appear between the resources and the distance separating the systems to be entangled. I reveal protocols that enable long distance entanglement distribution for quantum networks composed of mixed state and give a few limitations to the capabilities of entanglement distribution. To aid in the implementation of all entanglement distribution protocols I finish by introducing a new system, composed of an optical nanofibre coupled to a carbon nanotube, that may enable new forms of photo-detectors and quantum memories.

This thesis is concerned with the generation of non-classical quantum states of light, the photon-level manipulation of quantum states and the accurate tomography of both quantum states and quantum processes. In optics, quantum information can be encoded and processed in both discrete and continuous variables. Hybrid approaches combining for example homodyne detection with conditional state preparation and manipulation are gaining increasing prominence. The development and characterization of a time-domain balanced homodyne detector (BHD) is presented. The detector has a bandwidth of 80 MHz, a signal-to-noise ratio of 14.5 dB and an efficiency of 86% making it well-suited to pulse-to-pulse measurement of quantum optical states. The BHD is employed to perform quantum state tomography (QST) of non-classical multi-photon Fock states generated by spontaneous parametric down-conversion. A detailed investigation of the mode-matching between the local oscillator used for homodyne detection and the generated Fock states is presented. The one-, two- and three-photon Fock states are reconstructed with a combined preparation and detection efficiency exceeding 50%. Fock states have a number of applications in quantum state engineering, where non-classical ancilla states and conditional measurements enable photon-level manipulation of quantum states. Fock state filtration (FSF) is investigated - an example of a post-selected beam splitter which is a basic building block for many quantum state engineering protocols. A model is developed incorporating the effect of experimental imperfections. An experimental implementation of a Fock state filter is fully characterized by means of coherent-state quantum process tomography (QPT). The reconstructed process is found to be consistent with the model. The filter preferentially removes the single-photon component from an arbitrary input quantum state. Calibration of optical detectors in the quantum regime is discussed. Quantum detector tomography (QDT) is reviewed and contrasted with a new technique for performing QST with a calibrated detector known as the fitting of data patterns (FDP). The first experimental characterization of a BHD is performed by probing the detector with phase-averaged coherent states. The FDP method is shown to be applicable to the estimation of quantum processes, where a detector response is not assumed - thus demonstrating the versatility of the FDP approach as a new method in the quantum tomography toolbox.

In this thesis, we are concerned with continuous-variable quantum optical state engineering protocols. Such protocols are designed to repair or enhance the nonclassical features of a given state. In particular, we build a weak measurement model of Gaussian entanglement concentration of the two mode squeezed vacuum state. This model allows the simultaneous description of all possible ancilla system variations. In addition, it provides an explanation of the Gaussian-preserving property of these protocols while providing a success criterion which links all of the degrees of freedom on the ancilla. Following this, we demonstrate the wider application of weak measurements to quantum optical state engineering by showing that they allow probabilistic noiseless amplifi cation of photon number. We then establish a connection between weak measurements and entanglement concentration as a fundamental result of weak measurements on entangled probes. After this, we explore the trade-off between Gaussian and non-Gaussian operations in the preparation of non-Gaussian pure states. In particular, we suggest that an operational cost for an arbitrary non-Gaussian pure state is the largest Fock state required for its approximate preparation. We consider the extent to which this non-Gaussian operational cost can be reduced by applying unitary Gaussian operations. This method relies on the identification of a minimal core state for any target non-Gaussian pure state.

La dissertation explore différentes applications des fibres optiques en ingénierie quantique. Deux thématiques sont développées : d'une part l'utilisation des fibres optiques monomodales en silice pour l'implémentation d'algorithmes et de protocoles de communication quantiques et d'autre part l'utilisation de la non-linéarité de ces fibres pour réaliser des sources de paires de photons corrélés. L'étude est à la fois théorique et expérimentale./ The dissertation explores various uses of optical fibers for quantum engineering. Two topics are developed : first the use of single-mode silica fibers for implementing quantum algorithms and communication protocols, second the use of these fibers for generating correlated photon-pairs.

In this paper the features of quantum systems which lay the foundation of quantum entanglement are studied. General properties of entangled states are discussed, including their entropy and relation to Bell's inequality. Applications of entanglement, namely quantum teleportation and quantum cryptography, are also considered.

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.