Magnetic frustrations are the fundamental cause of many interesting phenomena in materials that have been intensely studied since the middle of the 20th century. Magnetic systems with competing interactions, ranging from insulating antiferromagnets to arrays of superconducting qubits, exhibit nontrivial quantum e ects that arise from the need to satisfy a jagged free energy landscape. The search for and characterization of quantum spin liquids, nontrivial topological phases, and quantum phase transitions is conducted through investigations of such frustrated models. Within the large umbrella of frustrated magnetism I have studied some speci c models with the purpose of answering the following questions: (1) What are the interesting phases and less-interesting phases, and how do they fall in the phase diagram relative to one another? (2) What properties do the phases have, and how can we characterize what happens when one phase transitions to another? Armed with the answers to these questions, researchers can further explore these interesting phenomena and apply them towards new materials and devices. In this thesis, I rst develop a computational methodology for studying both classical and quantum spin models using various forms of Monte Carlo simulation. I use classical Monte Carlo to study highly-frustrated models of Ising spins both at nite temperatures and in the T = 0 limit, to map the phase diagram and determine the universality class of phase transitions. Using these methods, I show that in a dissipative chain of qubits, bath-induced qubit-qubit interactions lead to collective decoherence above a critical dissipation strength. This causes the qubits to lose all stored information and become fully correlated with one another, an e ect that one would need to mitigate in order to perform quantum computation. In another study, I show that in antiferromagnetic insulators with anisotropic interactions, frustration can cause an intermediate paramagnetic phase with oblong \droplets" of correlated spins. This phenomenon is quite general and the presence of these droplets can help explain experimental signatures that occur at unexpected temperatures in such materials. In addition to the classical simulations, I develop a variational Monte Carlo (VMC) technique to search for ground states in Heisenberg-type models, speci cally for spins S = 1. The case of S = 1 is more complicated than the case for S = 1=2 due to an additional local degree of freedom, which has interesting implications for the possible states that can be realized. Using semiclassical energy minimization as well as VMC, I show that spin S = 1 diamond-lattice antiferromagnets experience higher-order spinspin interactions that destroy previously theorized liquid-like spiral spin orderings. However, the presence of these higher-order interactions can also potentially allow other phases such as quantum spin liquids and topological paramagnets. Such results can provide an avenue for explaining anomalous phenomena like low-temperature paramagnetism in future experimental materials.
Magnetic frustrations are the fundamental cause of many interesting phenomena in materials that have been intensely studied since the middle of the 20th century. Magnetic systems with competing interactions, ranging from insulating antiferromagnets to arrays of superconducting qubits, exhibit nontrivial quantum e ects that arise from the need to satisfy a jagged free energy landscape. The search for and characterization of quantum spin liquids, nontrivial topological phases, and quantum phase transitions is conducted through investigations of such frustrated models. Within the large umbrella of frustrated magnetism I have studied some speci c models with the purpose of answering the following questions: (1) What are the interesting phases and less-interesting phases, and how do they fall in the phase diagram relative to one another? (2) What properties do the phases have, and how can we characterize what happens when one phase transitions to another? Armed with the answers to these questions, researchers can further explore these interesting phenomena and apply them towards new materials and devices. In this thesis, I rst develop a computational methodology for studying both classical and quantum spin models using various forms of Monte Carlo simulation. I use classical Monte Carlo to study highly-frustrated models of Ising spins both at nite temperatures and in the T = 0 limit, to map the phase diagram and determine the universality class of phase transitions. Using these methods, I show that in a dissipative chain of qubits, bath-induced qubit-qubit interactions lead to collective decoherence above a critical dissipation strength. This causes the qubits to lose all stored information and become fully correlated with one another, an e ect that one would need to mitigate in order to perform quantum computation. In another study, I show that in antiferromagnetic insulators with anisotropic interactions, frustration can cause an intermediate paramagnetic phase with oblong \droplets" of correlated spins. This phenomenon is quite general and the presence of these droplets can help explain experimental signatures that occur at unexpected temperatures in such materials. In addition to the classical simulations, I develop a variational Monte Carlo (VMC) technique to search for ground states in Heisenberg-type models, speci cally for spins S = 1. The case of S = 1 is more complicated than the case for S = 1=2 due to an additional local degree of freedom, which has interesting implications for the possible states that can be realized. Using semiclassical energy minimization as well as VMC, I show that spin S = 1 diamond-lattice antiferromagnets experience higher-order spinspin interactions that destroy previously theorized liquid-like spiral spin orderings. However, the presence of these higher-order interactions can also potentially allow other phases such as quantum spin liquids and topological paramagnets. Such results can provide an avenue for explaining anomalous phenomena like low-temperature paramagnetism in future experimental materials.
In this thesis, we will concentrate on the numerical study of classical and quantum frustrated magnets. If we focus on the full set of problems which are contained in the class of quantum spin systems, we see that the techniques which can deal with them are plenty, but that the presence of frustration introduces several methodological hindrances. Whether it is the presence of a sign problem, or the extensive resources needed to perform the computation, many of these methods are efficient only on a reduced subset of frustrated systems. We will employ the pseudofermion-Functional Renormalization Group (pfFRG) method as our method of choice to tackle two dimensional frustrated quantum magnets, all of them modeled via a Heisenberg Hamiltonian. We will extend the pfFRG formalism to include spin systems where the spin length is unrestricted, S≥1/2. With this extension we are able to study in detail what the effect of quantum fluctuations are on the system. From the extreme quantum limit (S=1/2) to the classical limit (S→∞), the large-S extension of pfFRG allows us to manipulate the strength of the quantum fluctuations and study in detail how the quantum to classical transition happens. We apply this method to the study of incommensurate phases in the Heisenberg honeycomb model. We map the phase diagram for different values of the spin length and analyze how this length, and subsequently quantum fluctuations, affect the phases found in the classical limit. Furthermore, we prove that in the classical limit, pfFRG reduces to the Luttinger-Tisza formalism. When quantum fluctuations can be neglected, we model our frustrated magnet as a classical spin system. While this limit can easily be obtained from the large-S extension of pfFRG, this methodology is constrained to the study of two point correlators at zero temperature. To collect information regarding the behavior of our classical magnet beyond the two point correlators we study classical spin systems via Monte Carlo simulations. In this case we show how the method can be applied to continuous spin systems with strong anisotropic interaction. Furthermore, we employ this technique to numerically study α-Li2IrO3, a material which exhibits an incommensurate ground state but for which a minimal model has not been determined. We study and compare the possible minimal models that have been proposed. We reduce the number of minimal models by showing that many of those that have been proposed do not reproduce the full set of experimental results. Furthermore, we predict the magnetic behavior (for those models which reproduce the experimental results) in the presence of an external magnetic field. With this study we obtain magnetization processes and propose experiments which can confirm if one of the studied models is the correct minimal model for α-Li2IrO3.
This thesis is devoted to the numerical investigation of quantum spin models which describe the low-energy physics of frustrated magnets. At extremely low temperatures, these systems can host the so-called spin liquid phase, an unconventional state of matter characterized by a high degree of quantum entanglement and the absence of magnetic order. The experimental identification of the spin liquid phase in actual materials relies on the detection of its distinctive excitations (named spinons), which possess fractional quantum numbers and can be probed by inelastic neutron scattering experiments. From the theoretical point of view, variational methods have been largely employed to tackle ground state properties of frustrated spin models. In particular, variational Monte Carlo techniques based on Gutzwiller-projected fermionic wave functions have been shown to provide accurate results for several frustrated systems. In this thesis, we pursue an extension of this variational scheme to target dynamical spectra, which are directly measured by inelastic neutron scattering experiments. Specifically, we compute the dynamical structure factor by constructing approximate excited states, which are obtained by applying two-spinon operators to the ground state wave function. Our results prove that this variational method can accurately describe the spectral features of different spin systems. Focusing on prototypical frustrated models on the square and triangular lattices, we observe how the dynamical structure factor reflects the phase transition between a magnetically ordered phase with spin wave excitations, to a spin liquid state with fractional degrees of freedom. In addition to spectral properties, we also explore new directions to improve the accuracy of Gutzwiller-projected states by the application of a neural network correlator, in the form of a restricted Boltzmann machine. While this hybrid variational scheme provides a considerable improvement of the variational energy in the case of unfrustrated spin models, less satisfactory results are obtained for frustrated systems, which call for further refinements of the neural network variational Ansätze.
This thesis is focused on the application and development of numerical methods for studying quantum many- body spin systems. Part I sets the stage for research projects. In chapter 1, I go over major milestones in the field of frustrated magnetism, how it fits into a larger category of condensed matter physics, and recent developments that provide context for the research projects presented in part II. Chapters 2 3 provide the reader with necessary concepts in physics of phase transitions and numerical methods that are often employed when studying ground states of quantum many body systems. Part II focuses on the research projects carried out during my PhD research. In chapter 4 I present a machine-learning inspired method for solving quantum many body problems. This method addresses issues of representation of variational wave functions and their optimization. In chapter 5, I present a numerical study on the embedding of an exactly solvable point in a phase diagram of an extended Heisenberg model on a kagome lattice. Chapter 6 studies a quantum Heisenberg model on the stuffed honeycomb lattice. Phase transitions in quantum many body systems manifest themselves as a reorganization of low energy spectra of the system. They come in a variety of forms ranging from symmetry breaking transitions, where a local order parameter is formed and to topological phase transitions where the change of the ground state can be attributed to non-local changes in the entanglement patterns. In chapter 2, I review classic models studied in the context of frustrated magnetism and briefly go over the formulation of Landau symmetry breaking theory and common order parameters. The breakdown of Landau symmetry-breaking theory for topological phase transition is discussed using the example of Resonance Valence Bond (RVB) state, which serves as a qualitative exemplification of spin liquid phases. I discuss means of detecting phase transitions with a focus on methods that are applicable in a numerical setting. Chapter 3 presents elements of the numerical machinery that the rest of the thesis employs and builds upon. I discuss traditional trade-offs and provide rough metrics used for analysis of strengths and drawbacks of different approaches. Then I focus on Exact Diagonalization (ED) and Variational Monte Carlo (VMC) methods that are used in later chapters. In chapter 4, I describe the application of machine learning techniques to the variational approach to the quantum many body problem. I introduce Computational Graph States (CGS), a new class of variational wave functions based on the dataflow programming paradigm. The use of computational graphs makes composing new wave functions easy due to its modular structure. Automatic differentiation allows us to obtain efficient derivatives with respect to variational parameters automatically. We also develop a novel optimization scheme, Supervised Wave-function Optimization. It combines ideas of supervised learning and imaginary time evolution. Our method resolves a number of technical challenges and allows seamless optimization of complicated variational models. During the exploration process we constructed a new class of system size invariant model wave functions that can be trained on one system size and generalized to other system sizes with high accuracy. In chapter 5, we study the phase diagram of the kagome antiferromagnet in the J2, Jz plane, which corresponds to second nearest neighbor interactions and spin anisotropy. We report an exactly solvable point with macroscopic degeneracy at J2 = 0, Jz = −0.5 and show that many phases emanate from around this point. In addition, we find a previously unknown transition within the spin-liquid region suggesting a possibility of two distinct spin liquids. In chapter 6, we consider a Heisenberg model on the stuffed honeycomb lattice which interpolated between the triangular and honeycomb lattices. Using exact diagonalization we compute the phase diagram of this model. We find that for this model, the triangular lattice J1-J2 spin liquid region is extended to a larger domain that has lower symmetries than that of the triangular lattice. We perform a variational study of projected BCS wave functions which we directly compare to exact ground states on 36 site cluster as well as consider variational energies from larger system sizes. We argue that construction of symmetric states is essential to obtain good variational energies and give evidence that Dirac spin-liquid state is likely to characterize the spin liquid phase.
Frustration in many-body spin systems is a situation where the spins cannot orient themselves to fully minimize the interactions with their neighbors. It is caused, in general, by competing interactions or by the lattice structure, as in the antiferromagnets on non-bipartite lattices. Over the years frustrated systems have been studied substantially, since frustration can destabilize the antiferromagnetic order, lead to different phases of matter and induce various exotic properties. Frustration can be caused also by a choice of boundary conditions, i.e. the lattice topology. For instance, a ring with an odd number of sites is non-bipartite, which makes antiferromagnets in this setting frustrated. The subject of this thesis are zero-temperature one-dimensional quantum systems exactly in this setting. The major content is discussing how such a simple setting can influence the antiferromagnetic order, by studying spin-1/2 chains with discrete symmetries, whose breaking is related to the onset of the order. After reviewing the known results on topological frustration, dealing with non-thermodynamic quantities, we develop an approach for studying symmetry breaking, that is both suitable for exact analytical computations and meaningful for discussing the order also in a finite system. It consists of the realization that many spin-1/2 chains without external magnetic fields, such as the quantum XY chain, possess anticommuting global symmetries when the number of lattice sites is an odd number, implying the ground-state degeneracy already in a finite system. In this framework, we discover that topological frustration, despite being induced only by the choice of boundary conditions and even/odd system size choice, can affect the magnetization in the thermodynamic limit and system's quantum phase transitions. We find that topological frustration can destroy local order, create a site-dependent magnetization that varies in space with an incommensurate pattern, induce a first-order quantum phase transition that is not present without frustration and modify the nature of a second-order transition, by destroying local order at both sides of the transition and preserving only non-local string order parameters. All these results indicate the incompleteness of the approach to quantum many-body systems, based on the Ginzburg-Landau theory, that tries to capture the properties of the system by taking the system size to infinity before computing the observables and neglects the influence of the chain length as a relevant scale. We find that topological frustration can affect also non-equilibrium properties, by considering a local quantum quench setup. Namely, we study the Loschmidt echo and find it displays qualitatively and quantitatively different behavior for antiferromagnetic rings with an even and odd number of sites. Most of all, the differences become clearer for large system sizes, thus allowing to distinguish in a simple out-of-equilibrium experiment a system made by a certain, large, number of spins from the one with a single additional spin. The thesis also contains a mathematical part. In studying order parameters of models mappable to free fermions, Toeplitz determinants with symbols that possess a part proportional to the delta function arise. We derive asymptotic formulas for this type of determinants.
The study of various types of orders and phases of matter in magnetic systems is extremely popular theme in condensed matter physics. Not only frequently applicable in real world, quantum magnetism provides a fruitful and at the same time frequently feasible framework to search for new phases of matter. In this work we study quantum and associated classical phase transitions of spin systems by combinations of numerical and analytical methods.In Chapter 1 we study quantum paramagnets that are a generalization of antiferromagnetic AKLT [2] construction for the spin group SU(N). We map the so called simplex solid state ansatz wavefunction into a partition function of the classical system on the same lattice using coherent state representation. Then we study phase transitions of that classical models via classical Monte Carlo methods to determine properties of the original quantum simplex solid state [3].In Chapter 2 we are interested in the O(2) model in (2+1)-dimensional system with the dilution, i.e. when some sites are removed from the system. This relativistic O(2) model originates from the description of a transition between superfluid and Mott insulator phases. We study critical properties of the transition using a recently invented [4] worm algorithm.In Chapter 3 we are studying large-N expansion for the symplectic spin group Sp(N). When the original SU(2) spin model proves to be too difficult to be solved, for example at low temperatures, one of the alternative ways is to consider a system based on a more general spin group, for example SU(N) or Sp(N). Results often remain relevant for the original SU(2) group. We are using the mean-field theory approach to find phase transitions associated with the cubic Sp(N) system at large N.Another fundamental question of interest is how different systems behave when they are periodically driven by some external field. Such systems are called Floquet systems, and we will study them in Chapter 4. We will consider interacting and non-interacting systems, that might have a non-conventional type of ordering, topological order.
Frustrated quantum magnets may exhibit fascinating collective phenomena. The main goal of this dissertation is to provide conclusive evidence for the emergence of novel phases of matter like quantum spin liquids in local quantum spin models. We develop novel algorithms for large-scale Exact Diagonalization computations. Sublattice coding methods for efficient use of lattice symmetries in the procedure of diagonalizing the Hamiltonian matrix are proposed and suggest a randomized distributed memory parallelization strategy. Benchmarks of computations on various supercomputers with system size up to 50 spin-1/2 particles have been performed. Results concerning the emergence of a chiral spin liquid in a frustrated kagome Heisenberg antiferromagnet are presented. The stability and extent of this phase are discussed. In an extended Heisenberg model on the triangular lattice, we establish another chiral spin liquid phase. We discuss the special case of the Heisenberg J1-J2 model and present a scenario where the critical point of phase transition from the 120-degree Néel to a putative Z2 spin liquid is described by a Dirac spin liquid. A generalization of the SU(2) Heisenberg model with SU(N) degrees of freedom on the triangular lattice with an additional ring-exchange term is discussed. We present our contribution to the project and the final results that suggest a series of chiral spin liquid phases in an extended parameter range. Finally, we present preliminary data from a Quantum Monte Carlo study of an SU(N) version of the J-Q model on a square lattice for N=2,...,10, and multi-column representations. We establish the phase boundary between the Néel ordered phase and the disordered phases. The disordered phase in the four-column representation is expected to be a two-dimensional analog of the Haldane phase for the spin-1 Heisenberg chain.