This thesis consists of six chapters. The first chapter gives an introduction to the field of low-dimensional magnetic and electronic systems and relevant numerical techniques. The recent developments in molecular magnets are highlighted. The numerical techniques are reviewed along with their advantages and disadvantages from the present perspective. Study of entanglement of a system can give a great insight into the system. At the last part of this chapter a general overview is given regarding entanglement, its measures and its significance in studying many-body systems.
Chapter 2 deals with the technique that has been developed by us for the full symmetry adaptation of non-relativistic Hamiltonians. It is advantageous both computationally and physically/chemically to exploit both spin and spatial symmetries of a system. It has been a long-standing problem to target a state which has definite total spin and also belongs to a definite irreducible representation of a point group, particularly for non-Abelian point groups. A very general technique is discussed in this chapter which is a hybrid method based on valence-bond basis and the basis of the z-component of the total spin. This technique is not only applicable to a system with arbitrary site spins and belonging to any point group symmetry, it is also quite easy to implement computationally. To demonstrate the power of the method, it is applied to the molecular magnetic system, Cu6Fe8, with cubic symmetry.
In chapter 3, the extension of the previous hybrid technique to electronic systems is discussed. The power of the method is illustrated by applying it to a model icosahedral half-filled electronic system. This model spans a huge Hilbert space (dimension 1,778,966) and is in the largest non-Abelian point group. All the eigenstates of the model are obtained using our technique.
Chapter 4 deals with the thermodynamic properties of an important class of single-chain magnets (SCMs). This class of SCMs has alternate isotropic spin-1/2 units and anisotropic high spin units with the anisotropy axes being non-collinear. Here anisotropy is assumed to be large and negative, as a result, anisotropic units behave like canted spins at low temperatures; but even then simple Ising-type model does not capture the essential physics of the system due to quantum mechanical nature of the isotropic units. A transfer matrix (TM) method is developed to study statistical behavior of this class of SCMs. For the first time, it is also discussed in detail that how weak inter-chain interactions can be treated by a TM method. The finite size effect is also discussed which becomes important for low temperature dynamics. This technique is applied to a real helical chain magnet, which has been studied experimentally.
In the fifth chapter a bipartite entanglement entropy of finite systems is studied using exact diagonalization techniques to examine how the entanglement changes in the presence of long-range interactions. The PariserParrPople model with long-range interactions is used for this…
This thesis consists of six chapters. The first chapter gives an introduction to the field of low-dimensional magnetic and electronic systems and relevant numerical techniques. The recent developments in molecular magnets are highlighted. The numerical techniques are reviewed along with their advantages and disadvantages from the present perspective. Study of entanglement of a system can give a great insight into the system. At the last part of this chapter a general overview is given regarding entanglement, its measures and its significance in studying many-body systems.
Chapter 2 deals with the technique that has been developed by us for the full symmetry adaptation of non-relativistic Hamiltonians. It is advantageous both computationally and physically/chemically to exploit both spin and spatial symmetries of a system. It has been a long-standing problem to target a state which has definite total spin and also belongs to a definite irreducible representation of a point group, particularly for non-Abelian point groups. A very general technique is discussed in this chapter which is a hybrid method based on valence-bond basis and the basis of the z-component of the total spin. This technique is not only applicable to a system with arbitrary site spins and belonging to any point group symmetry, it is also quite easy to implement computationally. To demonstrate the power of the method, it is applied to the molecular magnetic system, Cu6Fe8, with cubic symmetry.
In chapter 3, the extension of the previous hybrid technique to electronic systems is discussed. The power of the method is illustrated by applying it to a model icosahedral half-filled electronic system. This model spans a huge Hilbert space (dimension 1,778,966) and is in the largest non-Abelian point group. All the eigenstates of the model are obtained using our technique.
Chapter 4 deals with the thermodynamic properties of an important class of single-chain magnets (SCMs). This class of SCMs has alternate isotropic spin-1/2 units and anisotropic high spin units with the anisotropy axes being non-collinear. Here anisotropy is assumed to be large and negative, as a result, anisotropic units behave like canted spins at low temperatures; but even then simple Ising-type model does not capture the essential physics of the system due to quantum mechanical nature of the isotropic units. A transfer matrix (TM) method is developed to study statistical behavior of this class of SCMs. For the first time, it is also discussed in detail that how weak inter-chain interactions can be treated by a TM method. The finite size effect is also discussed which becomes important for low temperature dynamics. This technique is applied to a real helical chain magnet, which has been studied experimentally.
In the fifth chapter a bipartite entanglement entropy of finite systems is studied using exact diagonalization techniques to examine how the entanglement changes in the presence of long-range interactions. The PariserParrPople model with long-range interactions is used for this…
The first part of the thesis deals with so called numerical renormalization group methods, and in particular the density-matrix renormalization group (DMRG). This method performs extremely well for large one-dimensional quantum systems like spin-chains and Hubbard models. We discuss general features of the quantum states obtained by using this method for large systems. One finds that the method works better, i.e. faster convergence and higher accuracy, when applied to systems having an energy gap between the ground state and the first excited state. An investigation of the behavior of the DMRG for a simple gapless system is done, mainly focusing on the properties of correlation functions. The second part of the thesis deals with topics related to superconductivity. It starts with a discussion of magnetic Josephson junctions and the physical processes governing the behavior of such a system. We also introduce and discuss models of high-temperature superconductors, in particular the t-J model and its relation to stripes. Starting from the t-J model on a two dimensional square lattice, we discuss an approximation where the spin-configuration is assumed static. We discuss the properties of the fictitious magnetic field experienced by the electrons due to the static spin-configuration. Configurations being close to ferromagnetic and antiferromagnetic turn out to have very different properties. Furthermore, we derive an effective model for this system and look for different phases of this model. In particular we investigate whether the system takes advantage of a spin-generated fictitious flux. Uniform phases are discussed in a Hartree-Fock approximation and we also consider stripes between antiferromagnetically ordered regions, these being modeled in a self-consistent Hartree approximation. Finally, and inspired by the fictitious fluxes, there is a chapter discussing the statistics of particles living on a circle. It is shown that there are two free parameters in the quantization of such a system and we also sort out the relation between fermions and hard-core bosons in one dimension.
Spins models, despite their simplicity, are known to describe with great precision physical properties of the materials. Of particular interest are the one-dimensional models that present an exact analytical solution, which can be obtained by the transfer matrix method and the decoration-iteration transformation technique. In this thesis, we studied a spin-electron model and two Ising-Heisenberg spin models, where all models are exactly soluble. The first model we investigate concerns a spin-electron diamond chain with Ising spins located on the local sites and mobile electrons dislocated in the interstitial sites under the external magnetic field action. We analyzed the ground states and the correlation between the spins. We show that thermal fluctuations can lead to the emergence of quantum entanglement above the unfrustrated ground states. We also analyze this same model but for different Landé g-factors. We investigated the phase diagrams at zero temperature. We also analyze the magnetization and we show that the magnetic field can cause the emergence of quantum entanglement in some conditions above the non-entanglement ground states. In this same context, we studied the Ising-XYZ diamond model of spin-1/2, with interaction between the second neighbours of the nodal Ising spins, and an external magnetic field applied to the z-axis. We investigate the phase diagram at zero temperature and the quantum entanglement. We notice that the bipartite entanglement between the pairs of Heisenberg interstitial spins in the natural mineral azurite is insensitive to the external magnetic field applied up to approximately 30 K. The third model we studied is a classical-quantum chain consisting of regularly alternating Ising and Heisenberg spins and with two different local anisotropy axes, subject to an applied external magnetic field. We studied the ground states, the magnetization and the susceptibility. It is evidenced that the investigated spin model reproduces magnetic characteristics of the heterobimetallic coordination compound Dy(NO)3(DMSO)2Cu(opba)(DMSO)2. In this thesis we show that the exact soluble spin models can describe with good precision a class of real magnetic materials, which can present interesting magnetic and thermodynamic properties, and quantum entanglement.
In this thesis we present the results of calculations of the properties of quantum spin systems. \nThe majority of the work is concerned with one dimensional spin chains and the particular \neffects that reduced dimensionality produce. The final chapter describes some earlier work on \nmixed valence manganite compounds. \nWe demonstrate one derivation of the Heisenberg Hamiltonian and discuss its applicability to \nmodelling magnetic systems both in three and one dimension. We discuss systems that are \nexactly soluble and the failure of spin wave theory in I-D. The Density-Matrix \nRenormalisation Group (DMRG) method is discussed in detail as is the extension to finite \ntemperature (TMRG). \nWe show results of calculations on a number of S=1/2 and S=l models and fundamental \ndifferences in their excitation spectra is observed. The thermodynamics of these systems have \nbeen obtained over a wide temperature range. In addition, excellent agreement with \nexperiment is shown for a number of quasi one dimensional compounds. The DMRG and \nTMRG are shown to be very competitive and accurate methods of studying such systems, \nespecially in the case of gapped systems. \nThe final chapter discusses the role of correlated magnetic clusters in determining the magnetic \nproperties of mixed valence manganites at temperatures near the Curie temperature. Our \nresults are supported by recent direct experimental observation of the formation of these \nclusters. We also briefly discuss some preliminary results regarding the effect of an interface \non the electronic and magnetic properties of these compounds.
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.
Strongly correlated systems, i.e., quantum materials for which the interactions between its constituents are strong, are good candidates for the development of applications based on quantum-mechanical principles, such as quantum computers. Two paradigmatic models of strongly correlated systems are heavy-fermionic systems and one-dimensional spin-12 systems, with and without quenched disorder. In the past decade, improvement in computational methods and a vast enhancement in computational power has made it possible to study these systems in a a non-perturbative manner. In this thesis we present state-of-the-art numerical methods to investigate the properties of strongly correlated systems, and we apply these methods to solve a couple of selected problems in quantum condensed matter theory. We start by revisiting the phase diagram of the Falicov-Kimball model on the square lattice which can be considered as a heavy-fermionic systems. This model describes an interplay between conduction electrons and heavy electrons and reveals several distinct metal-insulator phase transitions. Using a lattice Monte-Carlo method, we study the transport properties of the model. Our analysis describes the role of temperature and interaction strength on the metal-insulator phase transitions in the Falicov-Kimball model. The second part of the thesis investigate the spatial structure of the entanglement in ground and thermal statesof the transverse-field Ising chain. We use the logarithmic negativity as a measure for the entanglement between two disjoint blocks. We investigate how logarithmic negativity depends on the spatial separation between two blocks, which can be viewed as the entanglement analog of a spatial correlation function. We find sharp entanglement thresholds at a critical distance beyond which the logarithmic negativity vanishes exactly and thus the two blocks become unentangled. Our results hold even in the presence of long-ranged quantum correlations, i.e., at the system’s quantum critical point. Using Time-Evolving Block Decimation (TEBD), we explore this feature as a function of temperature and size of the two blocks. We present a simple model to describe our numerical observations. In the last part of this thesis, we introduce an order parameter for a many-body localized spin-glass (MBL-SG) phase. We show that many-body localized spin-glass order can also be detected from two-site reduced density matrices, which we use to construct an eigenstate spin-glass order parameter. We find that this eigenstate spin-glass order parameter captures spin-glass phases in random Ising chains, both in many-body eigenstates as well as in the nonequilibrium dynamics, from a local in time measurement. We discuss how our results can be used to observe MBL-SG order within current experiments in Rydberg atoms and trapped ion systems.
In this thesis I present a theoretical study of three different\nstrongly correlated systems: Luttinger liquids, spin-1 chains and\nthe two-dimensional spin-1/2 Heisenberg model.\n\nFor every sub-field of our research I summarize the background and\nprovide further details to the work presented in the appended\npapers. Chapter 1 corresponds to paper I, Chapter 2 to paper II,\nChapter 3 and 4 to paper III and IV.\n\nIn paper I, we calculate with bosonization techniques the local\ndensity of states of a finite segment of Luttinger liquid. Besides of\nbeing of experimental relevance for Scanning Tunneling Microscopy\nexperiments on carbon nanotubes and cleaved overgrowth wires, the\nwave functions of a "Luttinger liquid in a box" very nicely\nvisualize the fundamental bosonic nature of the low energy\nexcitations.\n\nIn paper II, we analyze with field theory methods how the presence\nof a single-ion anisotropy affects the behavior of a spin-1 chain.\nWe determine in the framework of the Non Linear Sigma Model how the gaps\nof the anisotropic chain depend on an applied staggered magnetic\nfield. Our theoretical analysis is meant to model compounds like\nrmR2BaNiO5 that show coexistence of Haldane phase and\nlong-range order.\n\nIn paper III, we compute with quantum Monte Carlo simulations the\nlocal response to a uniform magnetic field around vacancies in the\ntwo-dimensional Heisenberg model. From the full understanding of the\nnumerical results, we can make quantitative predictions of relevance\nfor Nuclear Magnetic Resonance and susceptibility experiments. In\nparticular, we expect, even in the thermodynamic limit, a finite\nCurie contribution to the total susceptibility arising from the\nimpurities.\n\nFinally in paper IV, we consider interaction effects among\nimpurities. We compute the potential between static vacancies in\nseveral low-dimensional spin-1/2 antiferromagnets comparing\nthe numerics with exact results from conformal field theory and\nlinear spin wave theory. The potential is directly related to the\nlocal valence bond order and its magnitude is a loyal measure of the\namount of quantum correlations present into the system.