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.
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.
The density matrix renormalization group (DMRG) is a numerical method for studying low dimensional strongly correlated models. The study of these models is one of the most active areas of condensed matter physics today and has been spurred not only by the discovery of high temperature superconductivity but also by experiments on new compounds. In this thesis we study fundamentals of the density matrix renormalization group method as well as applications of the method to Heisenberg spin chains. The introductory text is meant as a brief overview of the DMRG as well as Heisenberg spin systems and provides an introduction to the papers. In papers I and II we investigate the density matrix renormalization group with the aim to better understand the underlying structure of the method. We find that if the renormalization converges to a fixed point in the thermodynamic limit, the resulting basis states can be written as a matrix product form. We also show an explicit relation of the DMRG to variational calculations using the fact that the matrix product states can be rederived through a variational ansatz without any reference to the DMRG calculation. It is then shown how the matrix product states can be used to define a set of Bloch waves for describing elementary excitations of the Heisenberg spin-1 chain. The low lying energy spectrum is calculated. In papers III and IV we investigate the thermodynamics of impurities in a spin-1/2 chain. For this purpose we have shown that a recently developed transfer matrix DMRG method can be used to calculate impurity properties. Both impurity corrections to thermodynamic properties and local properties at finite temperature can be obtained. The method gives quicker and more accurate results than quantum Monte Carlo. The numerical results show good agreement with field theory calculations for a number of impurity configurations and the cross-over function for the magnetic susceptibility from high- to low-temperature behavior shows the expected data collapse. Our results also give quantitative predictions for experiments on doped spin-1/2 chains.
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…
Quantum magnetism in low dimensions has been one of the central areas of theoretical research for many decades now. One of the key reasons for the long standing interest in this field has been the existence of simplified models, which serve as paradigms for understanding the role of strong interactions in many-electron systems. Although simple, these models quite often can not be solved exactly. In this review, we discuss a variety of analytical and numerical methods, which treat the system in a systematic and controlled manner. The central method employed in all the studies is the density matrix renormalization group (DMRG) method. This is supported by small scale numerical exact calculations, and by analytical methods using field theoretic techniques. We have considered a number of magnetic systems, from magnetic clusters to extended lattices, and have found some novel quantum ground states and low-energy elementary excitations. In some cases, we have also employed the finite-temperature DMRG method to accurately compute the low-temperature thermodynamic properties such as specific heat and magnetic susceptibility.
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.
This thesis is concerned with the numerical study of one-dimensional (1D) spin-1/2 quantum magnets and related method development. Its focus is on the calculation of dynamical spin correlation functions both at zero and finite temperature. This is motivated by the accessibility of dynamical quantities in experiments such as inelastic neutron scattering (INS) and electron spin resonance (ESR). The numerical methods used in this thesis are based on extensions of the density-matrix renormalization group (DMRG) and are formulated in the framework of matrix product states (MPS). While zero-temperature dynamical correlation functions are computed with existing MPS frequency-domain methods, an MPS frequency-domain approach for their calculation at finite temperature is developed in this thesis. The new method combines the Liouville-space formulation of the dynamics with a moment expansion of the dynamical correlation function. The majority of the results are obtained via MPS-based Chebyshev expansions. These numerical techniques are applied to two different model systems describing real materials. The first one is the material copper pyrimidine dinitrate (Cu-PM) which is modeled by a 1D spin-1/2 Heisenberg antiferromagnet with Dzyaloshinskii-Moriya interactions. The spin dynamics of this model is studied in an applied magnetic field and compared to ESR experiments. Zero-temperature calculations for momentum- and frequency-resolved dynamical quantities give direct access to the intensity of the elementary excitations and go beyond the low-energy description by the quantum sine-Gordon model. Thus, a deviation from the Lorentz invariant dispersion for the single-soliton resonance is found. The presence of the strongest boundary bound state previously predicted from a boundary sine-Gordon field theory is confirmed, while composite boundary-bulk excitations have too low intensities to be found in the numerical results. At finite temperature, there is a temperature-induced crossover of the soliton. Moreover, additional temperature effects such as interbreather transitions emerge, which is confirmed by accompanying ESR experiments on Cu-PM over a wide range of the applied field strength. The second system studied in this thesis is the compound BaCu2V2O8. It is shown that the magnetic properties of this quasi-1D material can be described by a strongly alternating antiferromagnetic-ferromagnetic spin-1/2 Heisenberg chain. As found for other dimerized systems, the strong correlations in BaCu2V2O8 persist even at elevated temperatures. Moreover, these correlations lead to an asymmetric lineshape broadening of the magnetic excitations at finite temperature. Upon raising the temperature, an increasingly asymmetric lineshape is observed in high-resolution INS experiments for BaCu2V2O8. In this thesis, the lineshape is calculated by the MPS finite-temperature method developed as a part of this work. Comparing these results to the INS data and the lineshape obtained by a diagrammatic approach, excellent agreement is found over a broad temperature range. This demonstrates that coherent quantum behavior persists at elevated temperatures in BaCu2V2O8 and that it can be predicted quantitatively.
Many phenomena in magnetism can be described using classical models, yet magnetism is a quantum mechanical effect. In addition to thermal fluctuations, quantum fluctuations arise due to the quantum uncertainty of the ground state. These fluctuations are enhanced by low dimensionality and low spin. Spin chains show interesting excitations associated with quasiparticles. Model materials for spin chains can be realized in compounds where the interchain interactions are weak enough. This thesis presents neutron scattering studies of two model materials for spin chains with different spin symmetry. The spin2 Heisenberg antiferromagnetic chain CuSO4*5D2O has a main exchange of J ∼ 3 K, which permits to study its excitation spectrum up to temperatures of ten times the exchange. The spin2 Heisenberg magnet has been studied widely both theoretically and experimentally. The excitation spectrum of the spin2 Heisenberg antiferromagnet consists of quasiparticles called spinons, and calculations for it exist for T = 0 and as a function of temperature. A quantitative comparison between experimental data and theoretical models across a range of temperatures is presented. The excitation spectrum of CuSO4*5D2O is excellently described by the excitation spectrum of a spin2 Heisenberg antiferromagnetic chain at finite temperatures. Energy-temperature scaling is observed at temperatures up to 2J . For these temperatures the Luttinger liquid description of the spin2 Heisenberg antiferromagnetic chain is valid. A spinon continuum is confirmed at all measured temperatures. Therefore, even at ten times the main exchange (T ≈ 10 J), CuSO4*5D2O shows the behavior of a quantum magnet, and not of a classical system at infinite temperatures, for which one would expect single spin flips. The Ising chain is one of the most studied models in magnetism, one model compound for it is RbCoCl3. Optical spectroscopy measurements suggest a lower gap than for similar compounds, which makes it better suited for high resolution neutron spectroscopy. Magnetic correlations along the chains arise in RbCoCl3 below 80 K. A gapped continuum is observed, which arises from isolated antiferromagnetic Ising chains. Below the first magnetic ordering temperature TN1 ≈ 28 K bound states are observed, which arise due to correlations which form between the chains. Strong diffuse scattering leads to the conclusion that disorder is still present. At the second magnetic ordering transition, at TN2 ≈ 14 K, the bound states split as the correlations between the chains change. Fits indicate that the correlations change continuously as a function of temperature. Above TN2 the excitation spectrum of RbCoCl3 can be described by a spin1 2 Ising chain with an XY-component which is treated as a perturbation. Below TN2 the main features are reproduced correctly, but deviations from the details indicate that additional terms in the Hamiltonian may be necessary. This thesis was carried out at the Institut Laue-Langevin, the Laboratory for Neutron Scattering and Imaging at the Paul Scherrer Institute and ETH Zurich.