In this doctoral thesis, we theoretically investigate the propagation of sound waves in dilute Bose gases, in both the collisionless and hydrodynamic regimes. The study of sound wave is a topic of high relevance for the understanding of dynamical properties of any fluid, classical or quantum, and further provides insightful information about the equation of state of the system. In our work, we focus in particular on the two-dimensional (2D) Bose gas, in which the sound wave is predicted to give useful information about the nature of the superfluid phase transition. Recently, experimental measurement of sound wave in a uniform 2D Bose gas has become available, and we show that the measured data are quantitatively well explained by our collisionless theory. Finally, we study the mixtures of weakly interacting Bose gases, by developing a beyond mean-field theory, which includes the effects of thermal and quantum fluctuations in both the density and spin channels. Our new theory allows for the investigation of sound dynamics, as well as the fundamental problem of phase- separation.

Strongly correlated systems have been a major challenge for a long time in the field of theoretical chemistry. For such systems, the relevant portion of the Hilbert space scales exponentially, preventing efficient simulation on large systems. However, in many cases, the Hilbert space can be partitioned into clusters on the basis of strong and weak interactions. In this work, we mainly focus on an approach where we partition the system into smaller orbital clusters in which we can define many-particle cluster states and use traditional many-body methods to capture the rest of the inter-cluster correlations. This dissertation can be mainly divided into two parts. In the first part of this dissertation, the clustered ansatz, termed as tensor product states (TPS), is used to study large strongly correlated systems. In the second part, we study a particular type of strongly correlated system, correlated triplet pair states that arise in singlet fission. The many-body expansion (MBE) is an efficient tool that has a long history of use for calculating interaction energies, binding energies, lattice energies, and so on. We extend the incremental full configuration interaction originally proposed for a Slater determinant to a tensor product state (TPS) based wavefunction. By partitioning the active space into smaller orbital clusters, our approach starts from a cluster mean-field reference TPS configuration and includes the correlation contribution of the excited TPSs using a many-body expansion. This method, named cluster many-body expansion (cMBE), improves the convergence of MBE at lower orders compared to directly doing a block-based MBE from an RHF reference. The performance of the cMBE method is also tested on a graphene nano-sheet with a very large active space of 114 electrons in 114 orbitals, which would require 1066 determinants for the exact FCI solution. Selected CI (SCI) using determinants becomes intractable for large systems with strong correlation. We introduce a method for SCI algorithms using tensor product states which exploits local molecular structure to significantly reduce the number of SCI variables. We demonstrate the potential of this method, called tensor product selected configuration interaction (TPSCI), using a few model Hamiltonians and molecular examples. These numerical results show that TPSCI can be used to significantly reduce the number of SCI variables in the variational space, and thus paving a path for extending these deterministic and variational SCI approaches to a wider range of physical systems. The extension of the TPSCI algorithm for excited states is also investigated. TPSCI with perturbative corrections provides accurate excitation energies for low-lying triplet states with respect to extrapolated results. In the case of traditional SCI methods, accurate excitation energies are obtained only after extrapolating calculations with large variational dimensions compared to TPSCI. We provide an intuitive connection between lower triplet energy mani- folds with Hückel molecular orbital theory, providing a many-body version of Hückel theory for excited triplet states. The n-body Tucker ansatz (which is a truncated TPS wavefunction) developed in our group provides a good approximation to the low-lying states of a clusterable spin system. In this approach, a Tucker decomposition is used to obtain local cluster states which can be truncated to prune the full Hilbert space of the system. As a truncated variational approach, it has been observed that the self-consistently optimized n-body Tucker method is not size- extensive, a property important for many-body methods. We explore the use of perturbation theory and linearized coupled-cluster methods to obtain a robust yet efficient approximation. Perturbative corrections to the n-body Tucker method have been implemented for the Heisenberg Hamiltonian and numerical data for various lattices and molecular systems has been presented to show the applicability of the method. In the second part of this dissertation, we focus on studying a particular type of strongly correlated states that occurs in singlet fission material. The correlated triplet pair state 1(TT) is a key intermediate in the singlet fission process, and understanding the mechanism by which it separates into two independent triplet states is critical for leveraging singlet fission for improving solar cell efficiency. This separation mechanism is dominated by two key interactions: (i) the exchange interaction (K) between the triplets which leads to the spin splitting of the biexciton state into 1(TT),3(TT) and 5(TT) states, and (ii) the triplet-triplet energy transfer integral (t) which enables the formation of the spatially separated (but still spin entangled) state 1(T...T). We develop a simple ab initio technique to compute both the triplet-triplet exchange (K) and triplet-triplet energy transfer coupling (t). Our key findings reveal new conditions for successful correlated triplet pair state dissociation. The biexciton exchange interaction needs to be ferromagnetic or negligible compared to the triplet energy transfer for favorable dissociation. We also explore the effect of chromophore packing to reveal geometries where these conditions are achieved for tetracene. We also provide a simple connectivity rule to predict whether the through-bond coupling will be stabilizing or destabilizing for the (TT) state in covalently linked singlet fission chromophores. By drawing an analogy between the chemical system and a simple spin-lattice, one is able to determine the ordering of the multi-exciton spin state via a generalized usage of Ovchinnikov's rule. In the case of meta connectivity, we predict 5(TT) to be formed and this is later confirmed by experimental techniques like time-resolved electron spin resonance (TR-ESR). / Doctor of Philosophy / The study of the correlated motion of electrons in molecules and materials allows scientists to gain useful insights into many physical processes like photosynthesis, enzyme catalysis, superconductivity, chemical reactions and so on. Theoretical quantum chemistry tries to study the electronic properties of chemical species. The exact solution of the electron correlation problem is exponentially complex and can only be computed for small systems. Therefore, approximations are introduced for practical calculations that provide good results for ground state properties like energy, dipole moment, etc. Sometimes, more accurate calculations are required to study the properties of a system, because the system may not adhere to the as- sumptions that are made in the methods used. One such case arises in the study of strongly correlated molecules. In this dissertation, we present methods which can handle strongly correlated cases. We partition the system into smaller parts, then solve the problem in the basis of these smaller parts. We refer to this block-based wavefunction as tensor product states and they provide accurate results while avoiding the exponential scaling of the full solution. We present accurate energies for a wide variety of challenging cases, including bond breaking, excited states and π conjugated molecules. Additionally, we also investigate molecular systems that can be used to increase the efficiency of solar cells. We predict improved solar efficiency for a chromophore dimer, a result which is later experimentally verified.

As a degree project in Theoretical Physics, the variational MCMC-scheme aided by neural network quantum states was examined for the purpose ofsolving the nuclear pairing model. The method entailed minimization of the local energy sampled via the Born distribution obtained through the neural network output.Both the ground and excited states' energies were computed, where the latter case used an extended loss function which included the overlap to the former.The NNQS-ansatz worked well when emulating the ground state, in which case the Stochastic Reconfiguration optimization method was particularly effective. This optimization method resulted in relative fast convergence to low variance states, and did not require a large number of hyperparameter modifications. Ultimately, all resulting energy intervals encompassed the exact ground state solutions, and had relative errors equal to or near zero.For the excited states, the VMC-NNQS was less effective, as each individual occupation number state investigated required considerable hyperparameter testing before reasonably low lying energy eigenstates could be obtained. Moreover, the convergence properties were less distinguished than for the ground state, as the optimization struggled to maintain orthogonality to the ground state. Nonetheless, the final results included the nearest solutions of the first excited states for several systems and indicated correlation energies similar to those of the ground state. / Som examensarbete inom teoretisk fysik undersöktes den variationella MCMC-metoden tillsammans med neurala nätverk i syfte att lösa kärnparsmodellen. Metoden innebar minimering av den lokala energin som samplades via Born-fördelningen erhållen genom utdata från neurala nätverksapproximationer. Både grundtillståndets och exciterade tillstånds energier beräknades, där det senare fallet använde en utökad kostnadsfunktion som inkluderade överlappet med det förnämnda. NNQS-ansatsen fungerade väl vid emulering av grundtillståndet, i vilket fall optimeringsmethoden stokastisk omkonfigurering (Stochastic Reconfiguration) var särskilt effektivt. Denna optimeringsmetod resulterade i relativt snabb konvergens till lågvarianstillstånd och krävde inte ett stort antal hyperparametriska modifieringar. De slutliga energiintervallen innefattade de exakta lösningarna för grundtillstånden med en relativ felmarginal lika med eller nära noll. För exciterade tillstånd var VMC-NNQS mindre effektivt, eftersom varje enskilt ockupationstillstånd som undersöktes krävde en ansenlig mängd hyperparametrisk testning innan rimligt låga egentillstånd kunde erhållas. Dessutom var konvergensensegenskaperna mycket mindre särspäglade än för grundtillståndet, eftersom optimeringen inte fullt kunde upprätthålla ortogonaliteten mot grundtillståndet. Likväl inkluderade de slutliga resultaten de närmaste lösningarna av de första exciterade energierna för ett flertal system, och visade på korrelationsenergier liknande de för grundtillståndet.

京都大学 / 新制・課程博士 / 博士(理学) / 甲第25099号 / 理博第5006号 / 新制||理||1714(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)講師 PETERSRobert, 教授 柳瀬 陽一, 教授 田中 耕一郎 / 学位規則第4条第1項該当 / Doctor of Agricultural Science / Kyoto University / DGAM

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Many problems in applied mathematics and physics are formulated most naturally in terms of matrices, and can be solved by computing functions of these matrices. For example, in quantum mechanics, the coherent dynamics of physical systems is described by the matrix exponential of their Hamiltonian. In state of the art experiments, one can now observe such unitary evolution of many-body systems, which is of fundamental interest in the study of many-body quantum phenomena. On the other hand the theoretical simulation of such non-equilibrium many-body dynamics is very challenging. In this thesis, we develop a symbolic approach to matrix functions and quantum dynamics based on a novel algebraic structure we identify for sets of walks on graphs. We begin by establishing the graph theoretic equivalent to the fundamental theorem of arithmetic: all the walks on any finite digraph uniquely factorise into products of prime elements. These are the simple paths and simple cycles, walks forbidden from visiting any vertex more than once. We give an algorithm that efficiently factorises individual walks and obtain a recursive formula to factorise sets of walks. This yields a universal continued fraction representation for the formal series of all walks on digraphs. It only involves simple paths and simple cycles and is thus called a path-sum. In the second part, we recast matrix functions into path-sums. We present explicit results for a matrix raised to a complex power, the matrix exponential, matrix inverse, and matrix logarithm. We introduce generalised matrix powers which extend desirable properties of the Drazin inverse to all powers of a matrix. In the third part, we derive an intermediary form of path-sum, called walk-sum, relying solely on physical considerations. Walk-sum describes the dynamics of a quantum system as resulting from the coherent superposition of its histories, a discrete analogue to the Feynman path-integrals. Using walk-sum we simulate the dynamics of quantum random walks and of Rydberg-excited Mott insulators. Using path-sum, we demonstrate many-body Anderson localisation in an interacting disordered spin system. We give two observable signatures of this phenomenon: localisation of the system magnetisation and of the linear magnetic response function. Lastly we return to the study of sets of walks. We show that one can construct as many representations of series of walks as there are ways to define a walk product such that the factorisation of a walk always exist and is unique. Illustrating this result we briefly present three further methods to evaluate functions of matrices. Regardless of the method used, we show that graphs are uniquely characterised, up to an isomorphism, by the prime walks they sustain.

Au cours de cette thèse, la physique des systèmes en interaction à été étudié expérimentalement à partir de gaz froids d'atomes de Rydberg. Les atomes de Rydberg sont des atomes dans un état fortement excités et ils ont la propriété d'interagir fortement du fait d'interactions électrostatiques à longue portée. Le premier résultat majeur de cette thèse est l'observation expérimentale d'un processus à quatre corps. Ce processus consiste en l'échange d'énergie interne entre quatre atomes de Rydberg induit par leurs interactions mutuelles. Il a été possible, en plus de son observation expérimentale, de décrire théoriquement ce processus, au niveau quantique. L'excitation par laser des gaz d'atomes de Rydberg en forte interaction a aussi été étudiée durant cette thèse. Cette situation donne lieu à de très intéressants comportements à N-corps. Ce sujet d'intérêt fondamental pourrait aussi amener à d'éventuelles applications pour la réalisation de simulateurs quantiques ou de sources de lumière non classiques. Un second résultat majeur de cette thèse est l'observation expérimentale d'une statistique fortement sub-poissonienne, i.e corrélée de l'excitation Rydberg. Ce résultat confirme le caractère à N-corps de tels systèmes. Le troisième résultat majeur de cette thèse est le développement d'un modèle théorique pour l'excitation par laser des gaz d'atomes de Rydberg en forte interaction. En utilisant les états quantiques dit états collectifs de Dicke, il a été possible de mettre au jour de nouveaux mécanismes liés au comportement à N-corps de ces sytèmes atomiques en forte interaction. / Uring this thesis, the Physics of interacting systems has been investigated experimentally using Cold Rydberg gases. Rydberg atoms are highly excited atoms and have the property to interact together through long-range electrostatic interactions.The first highlight of this thesis is the direct experimental observation of a 4-body process. This process consists in the exchange of internal energy between 4 Rydbergs atoms due to their mutual interactions. In addition to its observation, it has been possible to describ this process theoretically at a quantum level.The laser excitation of strongly interacting Rydberg gases has been also investigated during this thesis. In this regime, the interactions between Rydberg atoms give rise to very interesting many-body behaviors. In addition to fundamental interest, such systems could be used to realyze quantum simulators or non-classical light sources.A second highlight of this thesis is the experimental observation of a highly sub-poissonian, i.e correlated, excitation statistics. This result confirms the many-body character of the investigated system.The third highlight of this thesis is the development of a theoretical model to describ the laser excitation of strongly interacting Rydberg gases. Using the so-called Dicke collective states it has been possible to point out new mechanismes related to the many-body character of strongly atomic interacting systems.

Ce mémoire présente une étude théorique des propriétés de localisation collective dans les superfluides de Bose désordonnés ou quasipériodiques. S'il est connu depuis Anderson que le désordre peut localiser les particules libres, comprendre ses effets dans les systèmes quantiques en interaction, où il est à l'origine de transitions de phase et d'effets de localisation non-Triviaux, représente aujourd'hui un défi majeur. En nous focalisant sur le cas d'un gaz de Bose dans le régime de faibles interactions, bien décrit par la théorie de Bogoliubov, nous étudions les transitions de localisation de ses excitations collectives dans différents contextes. Dans le cas d'un vrai désordre dans l'espace continu tout d'abord, nous développons un formalisme de désordre fort allant au-Delà des études antérieures, aboutissant à une description complète des propriétés de localisation des excitations en dimension arbitraire. Nous présentons un diagramme de localisation générique, et une interprétation microscopique de la propagation des excitations dans le désordre. Dans un second temps, nous considérons le cas d'un potentiel quasipériodique unidimensionel, aux propriétés intermédiaires entre un vrai désordre et un potentiel périodique. Notre traitement analytique et numérique du problème révèle une transition de localisation collective, que nous caractérisons et interprétons en termes de localisation dans un potentiel effectif multiharmonique. Pour finir, nous considérons le cas d'un gaz de Bose à deux composants. Nous développons le formalisme général pour étudier ces questions et décrivons la physique de base de ces systèmes qui présentent leurs propres spécificités. / In this thesis, we theoretically investigate the collective localization properties of weakly-Interacting Bose superfluids subjected to disordered or quasiperiodic potentials. While disorder has been recognized since Anderson to induce single-Particle localization, the interplay between disorder and interactions in quantum systems is today among the most challenging questions in the field, and underlies fascinating phase transitions and non-Trivial localization effetcs. Focusing on Bose gases in the weakly-Interacting regime for which the Bogoliubov theory proves a successful tool, we study the localization transitions of collective excitations in several contexts. First, in the case of a continuous true disorder, we develop a strong-Disorder formalism going beyond previous studies, providing us with a complete description of the localization behaviour of collective excitations in arbitrary dimension. A generic localization diagram is obtained and the transport of excitations in the disorder is microscopically interpreted. Secondly, we consider the case of one-Dimensional quasiperiodic potentials, which are known to display intermediate properties between periodic and disordered ones. We perform a numerical and analytical treatment of the localization problem of collective excitations, allowing us to quantitatively characterize and interpret the localization transition in terms of an effective multiharmonic problem. Finally, we set up the general inhomogeneous formalism to address such issues in multicomponent Bose gases, and enlighten the basic physic of such systems, which are known to exhibit their own specific features.

Dans cette thèse nous étudions théoriquement de systèmes dissipatifs pompés,décrits par une équation maîtresse de Lindblad. En particulier, nous adressons les problématiques liés à l’émergence de phénomènes critiques. Nous présentons une théorie générale reliant les transitions de phase du premier et deuxième ordres aux propriétés spectrales du superopérateur liouvillien. Dans la région critique, nous déterminons la forme générale de l’état stationnaire et de la matrice propre du liouvillien associée à son gap spectral. Nous discutons aussi l’utilisation de trajectoires quantiques individuelles afin de révéler l’apparition des transitions de phase. En ayant dérivé une théorie générale, nous étudions le modèle de Kerr en présence de pompage à un photon (cohérent) et à deux photons (paramétrique) ainsi que de dissipation. Nous explorons les propriétés dynamiques d’une transition de phase du premier ordre dans un modèle de Bose-Hubbard dissipatif et d’une de second ordre dans un modèle XYZ dissipatif d’Heisenberg. Enfin, nous avons considéré la physique des cavités soumises à de la dissipation à un et deux photons ainsi qu’un pompage à deux photons, obtenu par ingénierie de réservoirs. Nous avons démontré que l’état stationnaire unique est un mélange statistique de deux états chats de Schrödinger, malgré de fortes pertes à un photon.Nous proposons et étudions un protocole de rétroaction pour la génération d’états chat purs / In this thesis we theoretically study driven-dissipative nonlinear systems, whosedynamics is capture by a Lindblad master equation. In particular, we investigate theemergence of criticality in out-of-equilibrium dissipative systems. We present a generaland model-independent spectral theory relating first- and second-order dissipative phasetransitions to the spectral properties of the Liouvillian superoperator. In the critical region,we determine the general form of the steady-state density matrix and of the Liouvillianeigenmatrix whose eigenvalue defines the Liouvillian spectral gap. We discuss the relevanceof individual quantum trajectories to unveil phase transitions. After these general results,we analyse the inset of criticality in several models. First, a nonlinear Kerr resonator in thepresence of both coherent (one-photon) and parametric (two-photon) driving and dissipation.We then explore the dynamical properties of the coherently-driven Bose-Hubbard and of thedissipative XYZ Heisenberg model presenting a first-order and a second-order dissipativephase transition, respectively. Finally, we investigate the physics of photonic Schrödingercat states in driven-dissipative resonators subject to engineered two-photon processes andone-photon losses. We propose and study a feedback protocol to generate a pure cat-likesteady state

In dieser Dissertation werden Programmtransformationen für die Klasse der regulär-irregulären Schleifenkomplexe, welche typischerweise in komplexen Simulationscodes für Vielteilchensysteme auftreten, betrachtet. Dabei wird die Effizienz der resultierenden Programme auf modernen Multicore-Systemen untersucht. Reguläre Schleifenkomplexe zeichnen sich durch feste Schleifengrenzen und eine regelmäßige Struktur der Abhängigkeiten der Berechnungen aus, bei irregulären Berechnungen sind Abhängigkeiten zwischen Berechnungen erst zur Laufzeit bekannt und stark von den Eingabedaten abhängig. Die hier betrachteten regulären-irregulären Berechnungen koppeln beide Arten von Berechnungen eng. Die Herausforderung der effizienten Realisierung regulär-irregulärer Schleifenkomplexe auf modernen Multicore-Systemen liegt in der Kombination von Transformationstechnicken, die sowohl ein hohes Maß an Parallelität erlauben als auch die Lokalität der Berechnungen berücksichtigen. Moderne Multicore-Systeme bestehen aus einer komplexen Speicherhierachie aus privaten und gemeinsam genutzten Caches, sowie einer gemeinsamen Speicheranbindung. Diese neuen architektonischen Merkmale machen es notwendig Programmtransformationen erneut zu betrachten und die Effizienz der Berechnungen neu zu bewerten. Es werden eine Reihe von Transformationen betrachtet, die sowohl die Reihenfolge der Berechnungen als auch die Reihenfolge der Abspeicherung der Daten im Speicher ändern, um eine erhöhte räumliche und zeitliche Lokalität zu erreichen. Parallelisierung und Lokalität sind eng verknüpft und beeinflussen gemeinsam die Effizienz von parallelen Programmen. Es werden in dieser Arbeit verschiedene Parallelisierungsstrategien für regulär-irreguläre Berechnungen für moderne Multicore-Systeme betrachtet. Einen weiteren Teil der Arbeit bildet die Betrachtung rein irregulärer Berechnungen, wie sie typisch für eine große Anzahl von Vielteilchensimualtionscodes sind. Auch diese Simulationscodes wurden für Multicore-Systeme betrachtet und daraufhin untersucht, inwieweit diese auf modernen Multicore-CPUs skalieren. Die neuartige Architektur von Multicore-System, im besonderen die in hohem Maße geteilte Speicherbandbreite, macht auch hier eine neue Betrachtung solcher rein irregulärer Berechnungen notwendig. Es werden Techniken betrachtet, die die Anzahl der zu ladenden Daten reduzieren und somit die Anforderungen an die gemeinsame Speicherbandbreite reduzieren.