Nesta dissertação estudamos uma probabilidade obtida a partir de conceitos da Mecânica Estatística Quântica do ponto de vista da Teoria Ergódica. A probabilidade é obtida a partir de um estado KMS sobre um lattice unidimensional de spins quânticos. Mostramos que esta probabilidade é mixing para o shift. Além disso, mostramos que vale um princípio dos grandes desvios para uma certa classe de funções e exploramos algumas propriedades do Jacobiano. Iremos considerar o estado KMS associado a um certo Hamiltoniano específico agindo sobre o lattice de spins quânticos. Nas seções iniciais vamos apresentar alguns conceitos e prerequisitos básicos (como operadores densidade, produto tensorial, C*-algebras e estados KMS) para o entendimento do resultado principal / In this dissertation we study a probability derived from Quantum Statistical Mechanics through the viewpoint of Ergodic Theory. The probability is obtained from a KMS state acting on a one dimensional lattice of quantum spins. We show that this probability is mixing for the shift map. Moreover, we show that a large deviation principle is true for a certain class of functions and we explore some properties of the Jacobian. We will consider the KMS state associated to a certain specific Hamiltonian acting on the quantum spin lattice. In the initial sections we will present some concepts and prerequisites (such as density operators, tensor product, C*-algebras and KMS states) for the understanding of our main results.

Nesta dissertação estudamos uma probabilidade obtida a partir de conceitos da Mecânica Estatística Quântica do ponto de vista da Teoria Ergódica. A probabilidade é obtida a partir de um estado KMS sobre um lattice unidimensional de spins quânticos. Mostramos que esta probabilidade é mixing para o shift. Além disso, mostramos que vale um princípio dos grandes desvios para uma certa classe de funções e exploramos algumas propriedades do Jacobiano. Iremos considerar o estado KMS associado a um certo Hamiltoniano específico agindo sobre o lattice de spins quânticos. Nas seções iniciais vamos apresentar alguns conceitos e prerequisitos básicos (como operadores densidade, produto tensorial, C*-algebras e estados KMS) para o entendimento do resultado principal / In this dissertation we study a probability derived from Quantum Statistical Mechanics through the viewpoint of Ergodic Theory. The probability is obtained from a KMS state acting on a one dimensional lattice of quantum spins. We show that this probability is mixing for the shift map. Moreover, we show that a large deviation principle is true for a certain class of functions and we explore some properties of the Jacobian. We will consider the KMS state associated to a certain specific Hamiltonian acting on the quantum spin lattice. In the initial sections we will present some concepts and prerequisites (such as density operators, tensor product, C*-algebras and KMS states) for the understanding of our main results.

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第22685号 / 理博第4626号 / 新制||理||1665(附属図書館) / 京都大学大学院理学研究科化学専攻 / (主査)准教授 前里 光彦, 教授 吉村 一良, 教授 有賀 哲也 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DGAM

Strongly correlated low-dimensional quantum spin models provide a well-established frame- work to study magnetic properties of insulators, and are of great theoretical interest and experimental relevance in condensed-matter physics. In this thesis, I use quantum Monte Carlo methods to numerically study quantum critical behavior in low-dimensional quantum spin models and wavefunctions. First, I study spinons &ndash emergent spin-1/2 bosonic excitations &ndash at certain one- and two-dimensional quantum phase transitions (QPTs) in spin models, by characterizing their size and confinement length quantitatively. In particular, I focus on the QPT from an antiferromagnetic (AFM) phase into a valence-bond solid (VBS) phase, which is an example of a violation of the standard Landau-Ginzburg-Wilson paradigm for phase transitions. This transition in two dimensions (2D) is instead likely described by a novel theory called "deconfined quantum criticality" (DQC). According to the theory, spinons should be deconfined. The degree of deconfinement is quantified in my calculations. Second, I present a comprehensive study of so-called short-bond resonating-valence-bond (RVB) spin liquids in 2D, which have been suggested as a good starting point for understanding the spin physics of high-temperature cuprates. I find that these RVB states can also be classified as quantum-critical VBS states, which indicates that RVB is less disordered than expected. This work suggests a possible mapping from the quantum RVB states to classical dimer models via a classical continuum field theory--the height model. This map explicitly bridges well-established classical results to future quantum studies. Third, I consider 1D amplitude product (AP) states, which are generalized versions of RVB states, with different wavefunction weightings of bonds according to their lengths. AP states constitute a good ansatz for certain Hamiltonians and are of broad interest in quantum magnetism. I study phase transitions from AFM-VBS phases in AP states by tuning their amplitudes, and obtain continuously varying critical exponents. In addition, I classify the 1D AP states through entanglement entropy calculations of the central charge in (1+1)D conformal field theory. This new classification could serve as guide for AP states as trial wavefunctions to search for ground states of corresponding quantum spin models.

L’étude de l’état fondamental liquide de spins est un des domaines très actif de la recherche en matière condensée. Le réseau le plus à même de stabiliser un tel état fondamental semble être, à deux dimensions, le réseau kagomé de spins antiferromagnétiques 1/2. Il y a à présent un consensus théorique sur le fait que ce modèle stabilise un état fondamental liquide de spin. Cependant, la nature de cet état est encore inconnue, notamment la nature des corrélations. Nous ne savons toujours pas si ces dernières sont à courte portée avec un gap dans le spectre d’excitations, ou si elles sont à plus longue portée avec un spectre d’excitations sans gap. D’un point de vue expérimental il n’existe que très peu de matériaux et seul l’Herbertsmithite présente un réseau kagomé de spins 1/2 géométriquement parfait. Les différentes études réalisées sur ce composé pointent toutes vers un état liquide de spin sans gap mais révèlent aussi des déviations à l’hamiltonien de Heisenberg qui pourraient être responsables de la fermeture de ce gap.Cette thèse traite de l’étude expérimentale principalement par RMN et µSR de nouveaux composés kagomé à base de vanadium faisant partie d’une famille récemment synthétisée, les vanadates fluorés à géométrie kagomé. Le matériau que nous avons le plus étudié est un composé à réseau kagomé de spins 1/2 à base de V4+, (NH4)2[C7H14N][V7O6F18] (DQVOF). Le modèle magnétique de ce composé peut être décomposé en deux sous systèmes presque indépendants, des plans kagomé trimérisés isolés et des ions V3+ quasi paramagnétiques. Les études de µSR démontrent une absence de gel magnétique jusqu’à 20 mK donc un état liquide de spins dans DQVOF. Les études de chaleur spécifique et de RMN dévoilent un comportement liquide de spin sans gap malgré la trimérisation du réseau et la faible valeur supposée de l’interaction Dzyaloshinskii Moriya. Nos résultats montrent finalement que l’absence de gap, intrinsèque ou due à des déviations à l’hamiltonien idéal, est une caractéristique robuste des matériaux kagomé. Nous avons de plus étudié un second matériau de cette famille, (NH4)2[C2H8N][V3F12] (DDVF), dont le réseau magnétique est formé par des plans kagomé découplés entre eux à base de V3+ (S = 1). Ce réseau présente de fortes distorsions par rapport au réseau idéal et les expériences thermodynamiques et de µSR mettent en évidence une transition magnétique vers un état gelé à 10 K avec une mise en ordre à longue distance qui s’effectue à 6 K uniquement. / The search for quantum liquid state is a very active field in condensed matter research. In two dimensions, the antiferromagnetic spin 1/2 kagome lattice seems to be the most able to stabilize such a ground state. Indeed, from recent theoretical investigations, we are now quite sure that this model has a quantum spin liquid ground state. However, we still do not know its nature, in particular the nature of its correlations. They could be short ranged with a gap in the excitation spectrum, or long ranged with a gapless excitation spectrum. On the experimental side, only few materials exist and only one possesses a geometrically perfect lattice, the Herbertsmithite. All the experiments that have been done on this compound reveal a gapless spin liquid state along with deviations to the spin 1/2 Heisenberg hamiltonian which could be responsible of the gap closure.This thesis deals with the experimental study, mainly by NMR and µSR, of new vanadium based kagomé compounds which are part of a newly synthesized family, the kagome fluoride vanadates. The material that we studied the most is a spin 1/2 kagomé compound based on V4+, (NH4)2[C7H14N][V7O6F18] (DQVOF). The magnetic model of this compound can be decomposed in two rather independent parts, trimerized kagome planes and quasi paramagnetic V3+ ions. The µSR studies, showing the absence of frozen moment down to 20 mK, reveal a spin liquid ground state in DQVOF. The heat capacity and the NMR experiments point out a gapless behavior despite trimerization and likely weak Dzyaloshinskii Moriya interactions. Our results demonstrate that the gapless ground state, whether intrinsic or due to deviation to the ideal hamiltonian, is a rather robust characteristic of kagome materials.Furthermore, we studied another compound of this family, (NH4)2[C2H8N][V3F12] (DDVF), which magnetic lattice is made of uncoupled kagomé planes based on V3+ (S = 1). The lattice shows large deviations to the ideal kagomé and the thermodynamic experiments and the µSR studies reveal a magnetic transition to a frozen state at 10 K with a long distance order which is effective only below 6 K.

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第21548号 / 理博第4455号 / 新制||理||1640(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)教授 川上 則雄, 教授 田中 耕一郎, 教授 前野 悦輝 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DFAM

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第19479号 / 理博第4139号 / 新制||理||1595(附属図書館) / 32515 / 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 戸塚 圭介, 教授 川上 則雄, 教授 石田 憲二 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DFAM

Thesis advisor: Fazel Tafti / The search for an ideal quantum spin-liquid (QSL) material which can host a QSL ground state as well as exotic excitations has been one of the leading research topics in condensed matter physics over the past few decades. Out of all the proposals to realize the physics of a QSL, the Kitaev model is the most promising proposal with a QSL ground state. The Kitaev Hamiltonian is exactly solvable via fractionalization of its spin degrees of freedom into Majorana excitations, and it can be engineered in real materials. Among all the proposed Kitaev candidates, α-Li2IrO3, Na2IrO3, Li2RhO3, and α-RuCl3 are the most promising candidates. During my Ph.D. research I explored new physics related to Kitaev materials via modification of the symmetry and structural properties of these known Kitaev candidates. First, I studied how modification of the inter-layer chemistry can alter the thermodynamic properties of Kitaev candidate α-Li2IrO3 via an enhancement of the spin-orbit coupling (SOC) effect. The light, octahedrally-coordinated inter-layer Li atoms are replaced with heavier, linearly-coordinated Ag atoms to synthesize Ag3LiIr2O6. In addition to these structural modifications to the parent compound α-Li2IrO3, having heavier elements between the honeycomb layers in the Ag compound increased the effect of SOC in the honeycomb layers and led to a decrease in the long-range ordering temperature in Ag3LiIr2O6 compared to its parent compound. Second, I studied the effect of local crystal distortion in the presence of a weak SOC effect to explore a new spin-orbital state different from the Jeff=1/2 state. Based on theoretical predictions, the ground states of Kitaev materials can be tuned to other exotic spin-orbital states such as an Ising spin-1/2 state. To provide the proper conditions for a competition between the trigonal crystal distortion and the SOC effect, I modified the crystal environment around the magnetic elements in the parent compound Li2RhO3 via a topo-chemical method and synthesized Ag3LiRh2O6. An increase in the strength of trigonal distortion in Ag3LiRh2O6, in the presence of weak SOC, led to a transition from the Jeff=1/2 ground state (Kitaev limit) in the parent compound to an Ising spin-1/2 ground state (Ising limit) in the product. This change in spin-orbital state resulted in a dramatic change in magnetic behavior. Whereas Li2RhO3 shows a spin-freezing transition at 6 K, Ag3LiRh2O6 reveals a robust long-range antiferromagnetic transition at 94 K. This is the first realization of a change of ground state between the Kitaev and Ising limits in the same structural family. Lastly, I studied how the crystal symmetry can be an important factor in the physics of Kitaev materials. Honeycomb layered materials can be crystallized in space groups C2/m, C2/c, and P6_322. However, the crystal symmetry of most Kitaev candidates is described by the C2/m space group. We successfully synthesized a polymorph of a 3d Kitaev candidate, hexagonal Na2Co2TeO6 (P6_322 space group) in space group C2/m. The change in crystal symmetry of this cobalt tellurate replaced three anti-ferromagnetic (AFM) orders at 27, 15, 7 K in the hexagonal polymorph by a single AFM peak at 9.6 K in the monoclinic Na2Co2TeO6. / Thesis (PhD) — Boston College, 2023. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.

The experimental quest for a quantum spin-liquid state (QSL) in frustrated magnetic systems addresses fundamental scientific interests, as this intriguing quantum phase provides excellent grounds for discovering exotic collective phenomena. ZnCu3(OH)6Cl2 (herbertsmithite), an S=1/2 kagomé-lattice Heisenberg antiferromagnet, is the most promising candidate for experimentally realizing a QSL. However, despite years of intense research, the nature of its paramagnetic ground state remains highly debated. The root cause of the controversy lies in the difficulty in distinguishing the effects of defects from the intrinsic properties of the kagomé lattice. In this thesis, we present 17-O nuclear magnetic resonance (NMR) measurements of an isotope-enriched ZnCu3(OH)6Cl2 single crystal. We succeeded in distinguishing the intrinsic magnetic behavior of the kagomé lattice from the defect-induced phenomena down to T~0.01J, where J~200K is the Cu-Cu super-exchange interaction. We identify NMR signals arising from the nearest-neighbor 17-O sites of Cu2+ defects occupying the Zn2+ interlayer sites. From the 17-O Knight shift measurements, we show that these Cu2+ defects induce a large Curie-Weiss contribution to the bulk-averaged susceptibility at low temperatures. Moreover, our 17-O single-crystal lineshapes show no signature of nonmagnetic Zn2+ defects within the kagomé lattice, and therefore, we rule out “anti-site disorder” as a cause of the paramagnetic ground state in ZnCu3(OH)6Cl2. Most importantly, we demonstrate that the intrinsic spin susceptibility of the kagome lattice asymptotically tends to zero below T~0.03J, indicating the presence of a finite gap Δ = 0.03~ 0.07J in the spin excitation spectrum; this gap is completely suppressed under the application of a high magnetic field of ~ 9T. The behavior of low-energy spin fluctuations probed by the 17-O nuclear spin-lattice relaxation rate is consistent with the gap signature observed for the 17-O Knight shift. In short, our 17-O NMR results provide the first experimental evidence for a gapped QSL realized in ZnCu3(OH)6Cl2. / Thesis / Doctor of Philosophy (PhD)

The overarching theme of this thesis is the question of how constraints influence collective behavior. Constraints are crucial in shaping both static and dynamic properties of systems across diverse areas within condensed matter physics and beyond. For example, the simple geometric constraint that hard particles cannot overlap at high density leads to slow dynamics and jamming in glass formers. Constraints also arise effectively at low temperature as a consequence of strong competing interactions in magnetic materials, where they give rise to emergent gauge theories and unconventional magnetic order. Enforcing constraints artificially in turn can be used to protect otherwise fragile quantum information from external noise. This thesis in particular contains progress on the realization of different unconventional phases of matter in constrained systems. The presentation of individual results is organized by the stage of realization of the respective phase. Novel physical phenomena after conceptualization are often exemplified in simple, heuristic models bearing little resemblance of actual matter, but which are interesting enough to motivate efforts with the final goal of realizing them in some way in the lab. One form of progress is then to devise refined models, which retain a degree of simplification while still realizing the same physics and improving the degree of realism in some direction. Finally, direct efforts in realizing either the original models or some refined version in experiment today are mostly two-fold. One route, having grown in importance rapidly during the last two decades, is via the engineering of artificial systems realizing suitable models. The other, more conventional way is to search for realizations of novel phases in materials. The thesis is divided into three parts, where Part I is devoted to the study of two simple models, while artificial systems and real materials are the subject of Part II and Part III respectively. Below, the content of each part is summarized in more detail. After a general introduction to entropic ordering and slow dynamics we present a family of models devised as a lattice analog of hard spheres. These are often studied to explore whether low-dimensional analogues of mean-field glass- and jamming transitions exist, but also serve as the canonical model systems for slow dynamics in granular materials more generally. Arguably the models in this family do not offer a close resemblance of actual granular materials. However, by studying their behavior far from equilibrium, we observe the onset of slow dynamics and a kinetic arrest for which, importantly, we obtain an essentially complete analytical and numerical understanding. Particularly interesting is the fact that this understanding hinges on the (in-)ability to anneal topological defects in the presence of a hardcore constraints, which resonates with some previous proposals for an understanding of the glass transition. As another example of anomalous dynamics arising in a magnetic system, we also present a detailed study of a two-dimensional fracton spin liquid. The model is an Ising system with an energy function designed to give rise to an emergent higher-rank gauge theory at low energy. We show explicitly that the number of zero-energy states in the model scales exponentially with the system size, establishing a finite residual entropy. A purpose-built cluster Monte-Carlo algorithm makes it possible to study the behavior of the model as a function of temperature. We show evidence for a first order transition from a high-temperature paramagnet to a low-temperature phase where correlations match predictions of a higher-rank coulomb phase. Turning away from heuristic models, the second part of the thesis begins with an introduction to quantum error correction, a scheme where constraints are artificially imposed in a quantum system through measurement and feedback. This is done in order to preserve quantum information in the presence of external noise, and is widely believed to be necessary in order to one day harness the full power of quantum computers. Given a certain error-correcting code as well as a noise model, a particularly interesting quantity is the threshold of the code, that is the critical amount of external noise below which quantum error correction becomes possible. For the toric code under independent bit- and phase-flip noise for example, the threshold is well known to map to the paramagnet to ferromagnet transition of the two-dimensional random-bond Ising model along the Nishimori line. Here, we present the first generalization of this mapping to a family of codes with finite rate, that is a family where the number of encoded logical qubits grows linearly with the number of physical qubits. In particular, we show that the threshold of hyperbolic surface codes maps to a paramagnet to ferromagnet transition in what we call the 'dual'' random-bond Ising model on regular tessellations of compact hyperbolic manifolds. This model is related to the usual random-bond Ising model by the Kramers-Wannier duality but distinct from it even on self-dual tessellations. As a corollary, we clarify long-standing issues regarding self-duality of the Ising model in hyperbolic space. The final part of the thesis is devoted to the study of material candidates of quantum spin ice, a three-dimensional quantum spin liquid. The work presented here was done in close collaboration with experiment and focuses on a particular family of materials called dipolar-octupolar pyrochlores. This family of materials is particularly interesting because they might realize novel exotic quantum states such as octupolar spin liquids, while at the same time being described by a relatively simple model Hamiltonian. This thesis contains a detailed study of ground state selection in dipolar-octupolar pyrochlore magnets and its signatures as observable in neutron scattering. First, we present evidence that the two compounds Ce2Zr2O7 and Ce2Sn2O7 despite their similar chemical composition realize an exotic quantum spin liquid state and an ordered state respectively. Then, we also study the ground-state selection in dipolar-octupolar pyrochlores in a magnetic field. Most importantly, we show that the well-known effective one-dimensional physics -- arising when the field is applied along a certain crystallographic axis -- is expected to be stable at experimentally relevant temperatures. Finally, we make predictions for neutron scattering in the large-field phase and compare these to measurements on Ce2Zr2O7.