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<p>The subject of this work is the theoretical analysis of the mean-field and many-body properties of an impurity in a Bose-Einstein condensate in a double well potential. By investigating the stationary mean-field properties we show that a critical value of the boson-impurity interaction energy, W_c, corresponds to a pitchfork bifurcation in the number difference variable in the mean-field theory. Comparing W_c to the value of W where the many-body ground state wave function begins to split shows a direct correlation signaling a connection between the many-body and mean-field theories. Investigation of the mean-field dynamics shows that chaos emerges for W > W_c in the vicinity of an unstable equilibrium point generated by the pitchfork bifurcation. An entropy is defined to quantify the chaos and compared to the entanglement entropy between the BEC and the impurity. The mean-field entropy shows a large gradient at W_c whereas the entanglement entropy shows no apparent features around the same value of W. An increase in correlations between nearest neighbour many-body eigenvalues is seen as W is increased providing evidence for ``quantum chaos''.</p> / Master of Science (MSc)

The field of organic electronics has received considerable attention over the past several years due to the promise of novel electronic materials that are cheap, flexible and light weight. While some devices based on organic materials have already emerged on the market (e.g. organic light emitting diodes), a deeper understanding of the excited states within the condensed phase is necessary both to improve current commercial products and to develop new materials for applications that are currently in the commercial pipeline (e.g. organic photovoltaics, wearable displays, and field effect transistors). To this end, a model for pi-conjugated molecular aggregates and crystals is developed and analyzed. The model considers two types of electronic excitations, namely Frenkel and charge-transfer excitons, both of which play a prominent role in determining the nature of the excited states within tightly-packed organic systems. The former consist of an electron-hole pair bound to the same molecule while in the later the electron and hole are located on different molecules. The model also considers the important nuclear reorganization that occurs when the system switches between electronic states. This is achieved using a Holstein-style Hamiltonian that includes linear vibronic coupling of the electronic states to the nuclear motion associated with the high frequency vinyl-stretching and ring-breathing modes. Analysis of the model reveals spectroscopic signatures of charge-transfer mediated J- and H-aggregation in systems where the photophysical properties are determined primarily by charge-transfer interactions. Importantly, such signatures are found to be sensitive to the relative phase of the intermolecular electron and hole transfer integrals, and the relative energy of the Frenkel and charge-transfer states. When the charge-transfer integrals are in phase and the energy of the charge-transfer state is higher than the Frenkel state, the system exhibits J-aggregate characteristics including a positive band curvature, a red shifted main absorption peak, and an increase in the ratio of the first two vibronic peaks relative to the monomer. On the other hand, when the charge-transfer integrals are out of phase and the energy of the charge-transfer state is higher than the Frenkel state, the system exhibits H-aggregate characteristics including a negative band curvature, a blue shifted main absorption peak, and a decrease in the ratio of the first two vibronic peaks relative to the monomer. Notably, these signatures are consistent with those exhibited by Coulombically coupled J- and H-aggregates. Additional signatures of charge-transfer J- and H-aggregation are also discovered, the most notable of which is the appearance of a second absorption band when the charge-transfer integrals are in phase and the charge-transfer and Frenkel excitons are near resonance. In such instances, the peak-to-peak spacing is found to be proportional to the sum of the electron and hole transfer integrals. Further analysis of the charge-transfer interactions within the context of an effective Frenkel exciton coupling reveals that the charge-transfer interactions interfere directly with the intermolecular Coulombic coupling. The interference can be either constructive or destructive resulting in either enhanced or suppressed J- or H- aggregate behavior relative to what is expected based on Coulombic coupling alone. Such interferences result in four new aggregate types, namely HH-, HJ-, JH-, and JJ-aggregates, where the first letter indicates the nature of the Coulombic coupling and the second indicates the nature of the charge-transfer coupling. Vibronic signatures of such aggregates are developed and provide a means by which to rapidly screen materials for certain electronic characteristics. Notably, a large total (Coulombic plus charge-transfer) exciton coupling is associated with an absorption spectrum in which the ratio of the first two vibronic peaks deviates significantly from that of the unaggregated monomer. Hence, strongly coupled, high exciton mobility aggregates can be readily distinguished from low mobility aggregates by the ratio of their first two vibronic peaks. Analysis of the spatial dependence of the intermolecular interactions reveals that all four aggregate types (HH-, HJ-, JH-, JJ-) can be achieved by enforcing the appropriate crystalline packing arrangement. Such tunability is possible due of the different length scales over which the natures of the two coupling sources interconvert from J-like to H-like; whereas the nature of the Coulombic coupling is known to be sensitive to displacements on the order of half the molecular length, the nature of the charge-transfer mediated exciton coupling is sensitive to geometric displacements of approximately a carbon-carbon bond length. It is proposed that such sensitivity should allow for fine tuning of the total excitonic coupling via modifications in the packing structure, as determined, for example, by the side chains. Several examples of the different aggregate types are provided throughout this dissertation as the model is used to probe the excited state character of several relevant conjugated organic systems. Such examples include pentacene and 7,8,15,16-tetraazaterrylene (TAT) along with several derivatives from the perylene family. / Chemistry

The ability of the nucleic acids to absorb ultraviolet light and remain relatively photostable is a property upon which life depends. The nucleobases, which are the primary chromophores, when irradiated display rapid radiationless decay back to the ground state, in general faster than is needed for photoreaction. Fluorescent analogs of these bases have structures similar to the nucleic acid bases, but display much longer excited state lifetimes. Theoretical investigations using quantum mechanical methods can provide insight into the precise mechanisms of these decay processes, and to the molecular specifics that contribute to them. The results of multi-reference configuration interaction (MRCI) ab initio investigations into these mechanisms are presented, with emphasis on cytosine and its fluorescent analog 5-methyl-2-pyrimidinone (5M2P). A comprehensive picture of the potential energy surfaces of these two bases is given, including stationary points and conical intersections, where radiationless transitions are promoted, between up to three state surfaces, as well as pathways connecting these points for each base. Cytosine is shown to have two different energetically accessible radiationless decay channels. The fluorescence of 5M2P is also demonstrated theoretically, with mechanism proposed. The potential energy surfaces of the two bases have many close similarities, with the different photophysical properties being attributed to subtle energetic differences between the two bases. Nonadiabatic coupling and the geometric phase effect are analyzed in detail near conical intersections in cytosine, including in a region close to a three-state conical intersection. A substituent effect study on the 2-pyrimidinone ring system shows that the presence, position and orientation of the amino group in cytosine is central to its photophysical properties, particularly its high absorption energy, and can be explained with a simple Frontier Molecular Orbital model. The effects of water solvent on the excitation energies of cytosine and uracil are theoretically investigated using two multi-reference ab initio methods, a quantum mechanical molecular mechanics method using MRCI (MRCI-QM/MM), and the fragment molecular orbital multiconfiguration self-consistent field method (FMO-MCSCF). The solvatochromic shifts calculated from both methods agree well with other more expensive methods and experimental data. The effects of water on the photophysical pathways of cytosine is also investigated using MRCI-QM/MM, including considerations of solvent reorganization. Results show that the overall effect of water on the decay mechanisms is small, with neither decay channel being significantly blocked or favored. / Chemistry

Quantum walks have been utilized by many quantum algorithms which provide improved performance over their classical counterparts. Quantum search algorithms, the quantum analogues of spatial search algorithms, have been studied on a wide variety of structures. We study quantum walks and searches on the Cayley graphs of finitely-generated free groups. Return properties are analyzed via Green’s functions, and quantum searches are examined. Additionally, the stopping times and success rates of quantum searches on random networks are experimentally estimated. / Mathematics

With the advance in nanotechnology, we are more interested in the "smaller worlds". One of the practical applications of this is to measure a very small displacement or the mass of a nano-mechanical object. To measure such properties, one needs a very sensitive detector. A quantum point contact (QPC) is one of the most sensitive detectors. In a QPC, electrons tunnel one by one through a tunnel junction (a "hole"). The tunnel junction in a QPC consists of a narrow constriction (nm-wide) between two conductors. To measure the properties of a nano-mechanical object (which acts as a harmonic oscillator), we couple it to a QPC. This coupling effects the electrons tunneling through the QPC junction. By measuring the transport properties of the tunneling electrons, we can infer the properties of the oscillator (i.e. the nano-mechanical object). However, this coupling introduces noise, which reduces the measurement precision. Thus, it is very important to understand this source of noise and to study how it effects the measurement process. We theoretically study the transport properties of electrons through a QPC junction, weakly coupled to a vibration mode of a nano-mechanical oscillator via both the position and the momentum of the oscillator. %We study both the position and momentum based coupling. The transport properties that we study consist of the average flow of current through the junction, given by the one-time correlation of the electron tunneling event, and the current noise given by the two-time correlation of the average current, i.e, the variance. The first comprehensive experimental study of the noise spectrum of a detector coupled to a QPC was performed by the group of Stettenheim et al. Their observed spectral features had two pronounced peaks which depict the noise produced due to the coupling of the QPC with the oscillator and in turn provide evidence of the induced feedback loop (back-action). Benatov and Blencowe theoretically studied these spectral features using the Born approximation and the Markovian approximation. In this case the Born approximation refers to second order perturbation of the interaction Hamiltonian. In this approximation, the electrons tunnel independently, i.e., one by one only, and co-tunneling is disregarded. The Markovian approximation does not take into account the past behavior of the system under time evolution. These two approximations also enable one to study the system analytically, and the noise is calculated using the MacDonald formula. Our main aim for this thesis is to find a suitable theoretical model that would replicate the experimental plots from the work of Stettenheim et al. Our work does not use the Markovian approximation. However, we do use the Born approximation. This is justified as long as the coupling between the oscillator and QPC is weak. We first obtain the non-Markovian unconditional master equation for the reduced density matrix of the system. Non-Markovian dynamics enables us to study, in principle, the full memory effects of the system. From the master equation, we then derive analytical results for the current and the current noise. Due to the non-Markovian nature of our system, the electron tunneling parameters are time-dependent. Therefore, we cannot study the system analytically. We thus numerically solve the current noise expression to obtain the noise spectrum. We then compare our noise spectrum with the experimental noise spectrum. We show that our spectral noise results agree better with the experimental evidence compared to the results obtained using the Markovian approximation. We thus conclude that one needs non-Markovian dynamics to understand the experimental noise spectrum of a QPC coupled to a nano-mechanical oscillator. / Physics

No / We present a demonstrative application of the nonholonomic control method to a real physical system composed of two cold Cesium atoms. In particular, we show how to implement a CNOT quantum gate in this system by means of a controlled Stark field.

A philosophic account of quantum physics. The thesis is divided into two parts. Part I is dedicated to laying the groundwork of quantum physics, and explaining some of the primary difficulties. Subjects of interest will include the principle of locality, the quantum uncertainty principle, and Einstein's criterion for reality. Quantum dilemmas discussed include the double-slit experiment, observations of spin and polarization, EPR, and Bell's theorem. The first part will argue that mathematical-physical descriptions of the world fall short of explaining the experimental observations of quantum phenomenon. The problem, as will be argued, is framework of the physical descriptive schema. Part I includes in-depth discussions of mathematical principles. Part II will discuss the Copenhagen interpretation as put forth by its founders. The Copenhagen interpretation will be expressed as a paradox: The classical physical language cannot describe quantum phenomenon completely and with certainty, yet this language is the only possible method of articulating the physical world. The paradox of Copenhagen will segway into Kant's critique of metaphysics. Kant's understanding of causality, things-in-themselves, and a priori synthetic metaphysics. The thesis will end with a conclusion of the quantum paradox by juxtaposing anti-materialist Martin Heidegger with quantum founder Werner Heisenberg. Our conclusion will be primarily a discussion of how we understand the world, and specifically how our understanding of the world creates potential for truth.

Cette thèse est consacrée au contrôle de la dynamique de systèmes quantiques par interaction avec des impulsions laser. Ces impulsions laser sont déterminées par la méthode du contrôle optimale qui peut être formulé dans l'espace de Hilbert pour les fonction d'ondes et dans l'espace de Liouville pour les matrices densité. Cette dernière approche est nécessaire pour étudier la dissipation et la décohérence. La première application concerne la localisation d'un paquet d'ondes dans l'un ou l'autre des puits d'une surface de potentiel à deux dimensions où trois bassins sont connectés par une région de biffurcation. Le modèle moléculaire correspond à l'isomérisation de H3CO en H2COH. La seconde application porte sur un modèle d'isomérisation du rétinal où seul la coordonnée de torsion est prise en compte. Les applications sur la portes logiques ont été réalisées en encodant l'information dans des niveaux vibrationnels d'un double puits à deux dimensions. Des champs permettant de simuler des transformations unitaires telles que la porte NOT, la porte CNOT et la porte HADAMARD ont été optimisés. Ces champs ont été concaténés pour simuler les quatre étapes de l'algorithme de Deutsch sur un système à deux qubits. L'influence de l'environnement a été prise en compte. Ces simulations montrent qu'il est concevable d'utiliser des degrés de liberté moléculaires avec des impulsions laser optimisées pour aller vers la calcul quantique.