Understanding energy transfer at the molecular scale is both essential for the design of novel molecular level devices and vital for uncovering the fundamental properties of non-equilibrium open quantum systems. In this thesis, we first establish the connection between molecular scale devices -- molecular electronics and phononics -- and open quantum system models. We then develop theoretical tools to study various properties of these models. We extend the standard master equation method to calculate the steady state thermal current and conductance coefficients. We then study the scaling laws of the thermal current with molecular chain size and energy, and apply this tool to investigate the onset of nonlinear thermal current - temperature characteristics, thermal rectification and negative differential conductance. Our master equation technique is valid in the ``on-resonance" regime, referring to the situation in which bath modes in resonance with the subsystem modes are thermally populated. In the opposite ``off-resonance" limit, we develop the Energy Transfer Born-Oppenheimer method to obtain the thermal current scaling without the need to solve for the subsystem dynamics. Finally, we develop a mapping scheme that allows the dynamics of a class of open quantum systems containing coupled subsystems to be treated by considering the separate dynamics in different subsections of the Hilbert space. We combine this mapping scheme with path integral numerical simulations to explore the rich phenomenon of entanglement dynamics within a dissipative two-qubit model. The formalisms developed in this thesis could be applied for the study of energy transfer in different realizations, including molecular electronic junctions, donor-acceptor molecules, artificial solid state qubits and cold-atom lattices.

Este projeto se destina ao estudo de sistemas quânticos não relativísticos de dois, quatro e oito níveis de energia que descrevem partículas com spin s=1/2 sujeitas à ação de campos externos e interagentes entre si. São apresentadas soluções exatas para as equações que regem esses sistemas. Tais sistemas possuem uma vasta aplicação em diversas áreas da física, dentre as quais é possível destacar a computação quântica. Possíveis aplicações dos resultados são a construção de portas lógicas quânticas universais. Estas portas lógicas quânticas representam um elemento essencial no desenvolvimento dos chamados computadores quânticos. A análise e a implementação destes computadores quânticos exige a manipulação de sistemas de vários níveis, sujeitos a campos externos dependentes do tempo. Neste trabalho é apresentada a solução para o assim chamado Problema de Rabi, um particular problema de dois níveis. Um exemplo de solução para o sistema de quatro níveis, aqui relativo a um problema de dois spins também é discutido. Foram obtidas soluções exatas para sistemas de oito níveis cuja possível aplicação é a Correção Quântica de Erros. / This project aims to study the non-relativistic quantum systems of two, four and eight energy levels that describe particles with spin s=1/2 in external .elds and interacting with each other. We find exact analitical solutions for these systems. Such systems have extensive applications in various areas of physics, among which its possible to highlight quantum computing. Possible applications of the results are the construction of quantum universal logic gates.These quantum logic gates are an essential element in the development of so-called quantum computers. The analysis and implementation of quantum computers requires handling systems of various levels, subject to time-dependent external fields. This work presents a solution to the so-called Rabi problem, a particular problem at two levels. An example of a solution to the system of four levels, related to two spins problem is also investigated. We obtained exact solutions for systems of eight levels with possible application to the Quantum Error Correction.

A Termodinâmica foi concebida através da observação da eficiência no funcionamento mecânico de máquinas que dependiam da troca de temperatura e calor com meio. O paradigma de modelo nesses estudos foram máquinas idealizadas que operavam em ciclos tais como o ciclo de Carnot (o mais eficiente possível) e o ciclo de Otto. Esses ciclos de operação das máquinas ditas térmicas podem ser decompostos em trechos em que processos termodinâmicos, tais como adiabático e isotérmico, atuam. Contudo, embora a compreensão da eficiência no funcionamento dessas máquinas tenha sido o primeiro passo, esta teoria não ficou limitada a tal, se desenvolvendo ao ponto de ser considerada um dos pilares da Física moderna. Atualmente tem-se visto um crescimento substancial dos estudos da Termodinâmica considerando sistemas pequenos e/ou fora do equilíbrio termodinâmico. Resultados curiosos têm sido obtidos quando considerados sistemas pequenos tais que efeitos quânticos têm grande relevância. Nesta situação surge o que tem sido chamado de Termodinâmica quântica: as leis da Termodinâmica sendo obtidas a partir de flutuações descritas pela Mecânica Quântica. Naturalmente, um dos primeiros problemas a ser tratado nesta nova circunstância foi a eficiência de máquinas térmicas. Para a descrição dessas máquinas quânticas foi-se primeiro construído o que seriam os diferentes processos termodinâmicos que guiam o funcionamento da mesma. Baseado nesses resultados, as versões quânticas dos ciclos de Carnot e Otto, através dos quais essas máquinas operavam, foram também determinados e as propriedades das máquinas térmicas puderam ser exploradas e comparadas com seu análogo clássico. Nesta dissertação estudaremos diferentes tipos de máquinas térmicas operando no ciclo de Otto. Essas máquinas são descritas por Hamiltonianos de dois spins 1/2 que apresentam interação. Algumas características desses Hamiltonianos são exploradas e o papel das mesmas sobre a eficiência da máquina foram determinado. Comparamos também esta eficiência com os limites dados pelo ciclo de Carnot e o limite dado pela situação em que o acoplamento entre os spins é nulo. Diferentes situações físicas são exploradas e suas consequências determinadas. Por fim, proporemos algumas discussões sobre o papel da Mecânica Quântica no funcionamento destas máquinas. / Thermodynamics was conceived by observing the efficiency of the mechanical operation of machines that depended on the temperature and heat exchange with the surroundings. The paradigm model in these studies were idealized machines operating in cycles such as the Carnot cycle (the most efficient one) and the Otto cycle. These thermal operating cycles of the machines can be decomposed into parts that thermodynamic processes, such as isothermal and adiabatic, act. However, while the understanding of efficiency in the functioning of these machines has been the first step, this theory was not limited to this, being developed the point of being considered one of the pillars of modern Physics. Currently, it has seen a substantial growth of Thermodynamics studies considering small systems and / or out of equilibrium thermodynamical systems. Curious results have been obtained when considered small systems such that quantum effects are highly relevant. In this situation arises what has been called quantum thermodynamics: the laws of thermodynamics being derived from fluctuations described by Quantum Mechanics. Of course, one of the problems to be addressed in the new condition was the efficiency of heat engines. For a description of these quantum machines first was built what would be the different thermodynamical processes that guide the operation. Based on these results, the quantum versions of Carnot and Otto cycles, through which these machines operate, were also determined and the properties of thermal machines could be explored and compared with its classical analog. This thesis will study different types of heat engines operating in Otto cycle. Such machines are described by two spin 1/2 Hamiltonian presenting interaction. Some characteristics of these Hamiltonians are explored and the role of them on the machine efficiency were determined. We also compared this efficiency with the limits given by the Carnot cycle and the limit given by the situation which the coupling between the spins is zero. Different physical situations are explored and its consequences determined. Finally, we propose some discussions about the role of quantum mechanics in the operation of these machines.

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第21585号 / 理博第4492号 / 新制||理||1645(附属図書館) / 京都大学大学院理学研究科化学専攻 / (主査)教授 谷村 吉隆, 教授 林 重彦, 教授 寺嶋 正秀 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DGAM

In this thesis, we discuss correlations arising between a system and its environment that lead to errors in an open quantum system. Detecting those correlations would be valuable for avoiding and/or correcting those errors. It was studied previously that we can detect correlations by only measuring the system itself if we know the cause of interaction between the two, for example in the case of a dipole-dipole interaction for a spin 1/2-spin 1/2 interaction Hamiltonian. We investigate the unitary, U which is associated with the exchange Hamiltonian and examine the ability to detect initial correlations between a system and its environment for a spin-1/2(qubit) system interacting with a larger higher dimensional environment. We provide bounds for when we can state with certainty that there are initial system-environment correlations given experimental data.

On etudie la contrôlabilité des systèmes quantiques dans deux contextes différents: le cadre standard fermé, dans lequel un système quantique est considéré comme isolé et le problème de contrôle est formulé sur l'équation de Schrödinger; le cadre ouvert qui décrit un système quantique en interaction avec un plus grand, dont seuls les paramètres qualitatifs sont connus, au moyen de l'équation de Lindblad sur les états.Dans le contexte des systèmes fermés on se focalise sur la classe intéressante des systèmes spin-boson, qui décrivent l'interaction entre un système quantique à deux niveaux et un nombre fini de modes distingués d'un champ bosonique. On considère deux exemples prototypiques, le modèle de Rabi et le modèle de Jaynes-Cummings qui sont encore très populaires dans plusieurs domaines de la physique quantique. Notamment, dans le contexte de la Cavity Quantum Electro Dynamics (C-QED), ils fournissent une description précise de la dynamique d'un atome à deux niveaux dans une cavité micro-onde en résonance, comme dans les expériences récentes de S. Haroche. Nous étudions les propriétés de contrôlabilité de ces modèles avec deux types différents d'opérateurs de contrôle agissant sur la partie bosonique, correspondant respectivement – dans l'application à la C-QED – à un champ électrique et magnétique externe. On passe en revue quelques résultats récents et prouvons la contrôlabilité approximative du modèle de Jaynes-Cummings avec ces contrôles. Ce résultat est basé sur une analyse spectrale exploitant les non-résonances du spectre. En ce qui concerne la relation entre l'Hamiltonien de Rabi et Jaynes-Cummings nous traitons dans un cadre rigoureux l'approximation appelée d'onde tournante. On formule le problème comme une limite adiabatique dans lequel la fréquence de detuning et le paramètre de force d'interaction tombent à zero, ce cas est connu sous le nom de régime de weak-coupling. On prouve que, sous certaines hypothèses sur le rapport entre le detuning et le couplage, la dynamique de Jaynes-Cumming et Rabi montrent le même comportement, plus précisément les opérateurs d'évolution qu'ils génèrent sont proches à la norme.Dans le cadre des systèmes quantiques ouverts nous étudions la contrôlabilité de l'équation de Lindblad. Nous considérons un contrôle agissant adiabatiquement sur la partie interne du système, que nous voyons comme un degré de liberté qui peut être utilisé pour contraster l'action de l'environnement. L'action adiabatique du contrôle est choisie pour produire une transition robuste. On prouve, dans le cas prototype d'un système à deux niveaux, que le système approche un ensemble de points d'équilibre déterminés par l'environnement, plus précisément les paramètres qui spécifient l'opérateur de Lindblad. Sur cet ensemble, le système peut être piloté adiabatiquement en choisissant un contrôle approprié. L'analyse est fondée sur l'application de méthodes de perturbation géométrique singulière. / We investigate the controllability of quantum systems in two differentsettings: the standard 'closed' setting, in which a quantum system is seen as isolated, the control problem is formulated on the Schroedinger equation; the open setting that describes a quantum system in interaction with a larger one, of which just qualitative parameters are known, by means of the Lindblad equation on states.In the context of closed systems we focus our attention to an interesting class ofmodels, namely the spin-boson models. The latter describe the interaction between a 2-level quantum system and finitely many distinguished modes of a bosonic field. We discuss two prototypical examples, the Rabi model and the Jaynes-Cummings model, which despite their age are still very popular in several fields of quantum physics. Notably, in the context of cavity Quantum Electro Dynamics (C-QED) they provide an approximate yet accurate description of the dynamics of a 2-level atom in a resonant microwave cavity, as in recent experiments of S. Haroche. We investigate the controllability properties of these models, analyzing two different types of control operators acting on the bosonic part, corresponding -in the application to cavity QED- to an external electric and magnetic field, respectively. We review some recent results and prove the approximate controllability of the Jaynes-Cummings model with these controls. This result is based on a spectral analysis exploiting the non-resonances of the spectrum. As far as the relation between the Rabi andthe Jaynes-Cummings Hamiltonians concerns, we treat the so called rotating waveapproximation in a rigorous framework. We formulate the problem as an adiabaticlimit in which the detuning frequency and the interaction strength parameter goes to zero, known as the weak-coupling regime. We prove that, under certain hypothesis on the ratio between the detuning and the coupling, the Jaynes-Cumming and the Rabi dynamics exhibit the same behaviour, more precisely the evolution operators they generate are close in norm.In the framework of open quantum systems we investigate the controllability ofthe Lindblad equation. We consider a control acting adiabatically on the internal part of the system, which we see as a degree of freedom that can be used to contrast the action of the environment. The adiabatic action of the control is chosen to produce a robust transition. We prove, in the prototype case of a two-level system, that the system approach a set of equilibrium points determined by the environment, i.e. the parameters that specify the Lindblad operator. On that set the system can be adiabatically steered choosing a suitable control. The analysis is based on the application of geometrical singular perturbation methods.

京都大学 / 新制・課程博士 / 博士(理学) / 甲第25111号 / 理博第5018号 / 新制||理||1715(附属図書館) / 京都大学大学院理学研究科物理学・宇宙物理学専攻 / (主査)准教授 福間 將文, 教授 杉本 茂樹, 教授 橋本 幸士 / 学位規則第4条第1項該当 / Doctor of Agricultural Science / Kyoto University / DFAM

Ce travail de maîtrise a mené à la rédaction d'un article (Physical Review A 80, 062319 (2009)). / L'informatique quantique, brièvement introduite au chapitre 1, exploite les corrélations quantiques et en particulier l'intrication. Ces corrélations sont difficiles à maintenir car un système quantique n'est habituellement pas fermé, mais en interaction avec son environnement. Le traitement formel d'un système quantique ouvert requiert des outils spécifiques, introduits au chapitre 2. En utilisant ces notions, nous montrerons au chapitre 3 que l'interaction entre le système et son environnement aura pour effet de privilégier certains états, qualifiés de quasi-classiques, suggérant ainsi l'émergence d'un monde classique à partir d'un monde quantique. De plus, l'intrication qui se crée entre le système et son environnement détruira la cohérence d'une superposition d'états quasi-classiques. Il s'agit du phénomène de décohérence dont les mécanismes seront mis en évidence dans notre étude originale d'un gyroscope quantique au chapitre 4. Nous montrerons qu'une particule de grand spin servant à mesurer le moment angulaire d'électrons perd sa cohérence en un temps très court par rapport au temps caractéristique de relaxation. Afin de protéger la cohérence d'un système, essentielle pour l'informatique quantique, plusieurs techniques de protection ont été développées. Nous les rappelerons brièvement en début de chapitre 5, avant d'introduire une approche originale qui consiste à préparer l'environnement. Notre étude nous permet de caractériser l'existence d'états initiaux de l'environnement permettant une évolution sans décohérence du système dans une gamme de modèles où le système interagit avec un environnement présentant une dynamique propre. / Quantum information processing, briefly introduced in Chapter 1, relies on quantum correlations, namely on entanglement. Those correlations are difficult to maintain since a typical quantum system is not closed, but interacting with its environment. The analysis of an open quantum system requires specific tools which we introduce in Chapter 2. Using these concepts, we show in Chapter 3 that the interaction between the system and its environment will distinguish certain quasi-classical states, suggesting the emergence of a classical world from a quantum one. Furthermore, the entanglement created between the system and its environment will destroy the coherence of a superposition of such quasi-classical states. This phenomenon of decoherence exhibits mechanisms which we highlight in our original study of a quantum gyroscope in chapter 4. We demonstrate that a particle with large spin, used to measure the angular momentum of electrons, loses its coherence on a timescale much shorter than the characteristic timescale of relaxation. To protect the coherence of a system, essential to quantum information processing, several techniques have been developed. We briefly review them at the beginning of Chapter 5, before introducing a novel approach based on the preparation of the environment. Our analysis characterizes the existence of initial states of the environment allowing for decoherence-free evolution of the system in a large class of models in which the system interacts with a dynamical environment.

The aim of this work is to investigate projection operator method of deriva- tion of equations of motion for reduced density matrix and apply it to a model open quantum system. We gradually pass from quantum mechanical model of a molecule with one vibrational degree of freedom to an example of open quantum system relevant in the theory of nonlinear spectroscopy. In the thesis we present results of numerical simulations of the time evolution of the open quantum system performed with a program written for this purpose. We are specially concerned with simulations of the solution of the time-convolutionless generalized master equation up to the a second order of the perturbation expan- sion, and we show that under certain conditions it provides an exact solution of the problem. The text also contains derivation of the recurrence relations for the Franck-Condon factors for the most general case of two quantum harmonic oscillators in one space dimension, i. e. transformation matrix between two bases of the L2 (R) space determined by the solutions of the time-independent Schrödinger equation appropriate for these oscillators. 1

Estudamos o amortecimento radiativo e o ruído de spins de um material magnético acoplado a um circuito ressonante. O amortecimento radiativo em ressonância magnética é um fenômeno de dissipação, na qual a magnetização preparada após um pulso de Rabi sofre um decaimento até seu estado de equilíbrio. O material magnético perde energia através do seu acoplamento com o circuito ressonante, que deve estar sintonizado na freqüência de Larmor dos spins do material. Apesar deste fenômeno ter sido estudado há vários anos, nenhuma descrição quântica completa lhe foi dada. Apresentamos um modelo hamiltoniano quântico que descreve o amortecimento radiativo. Para isto usamos o método de equações de Langevin quânticas. Mostramos que além do amortecimento radiativo do material magnético, se o circuito está em um estado inicial coerente, a magnetização adquire um movimento complicado não-trivial. Usando as mesmas equações de Langevin, estudamos a influência da amostra no ruído do circuito ressonante. Calculamos a densidade espectral da corrente no caso em que todo o sistema está em equilíbrio térmico. Pudemos verifcar a efcácia do método comparando-o com estudos anteriores. Além disso, estudamos as alterações do ruído do circuito quando uma tensão oscilante externa é aplicada. Nesta situação surgem dois outros picos laterais ao pico central do espectro de absorção da amostra magnética. Isso leva a três depressões no espectro da corrente do circuito. Este efeito deve-se à separação dupla dos estados de energia dos spins. Comentamos sobre a analogia deste fenômeno com a fluorescência ressonante observada na Óptica Quântica. / We study the radiation damping and the spin noise of a magnetic material coupled with a resonant circuit. Radiation damping in magnetic resonance is a dissipation phenomenon, where magnetization prepared after a Rabi pulse decays toward its equilibrium state. The magnetic sample loses its energy by the coupling with resonant circuit, that must be tuned in Larmor frequency of the sample spins. Even though this phenomenon had been studied many years ago, no full quantum description was done. We present a quantum Hamiltonian model, that explains the radiation damping. We use quantum Langevin equation method for this task. Beyond radiation damping, we show the magnetization acquires an unusual intrincate motion, if the circuit initial state is coherent. Using the same Langevin equation, we study the sample influence on the resonant circuit noise. We calculate the current spectral density in the case of thermal equilibrium of whole system. We can verify the method efectiveness, comparing former papers. Moreover we study modifcations in the circuit noise, if an external oscillating tension is applied. In this situation, other two peaks emerge in the central peak sidebands of the sample absorption spectrum. It leads to appear three dips in circuit current spectrum. This efect is due to the splitting of the spin energy states. We comment about the analogy between this phenomenon and the resonance fluorescence in Quantum Optics.