This thesis investigates exotic phases of matter in magnetic materials that present anisotropic properties in two dimensions. Using the microscopic spin Hamiltonians, the study addresses two problems: (i) the appearance of a novel class of magnetic excitations in the spectra of anisotropic magnets at zero temperature, and (ii) the quantum-to-classical correspondence of spins for the description of magnetic solids in the disordered phase above the critical temperature. Different analytical and numerical means are used to this purpose.In the first part, motivated by experimental observations of multipolar excitations in afamily of strongly-anisotropic van der Waals antiferromagnets, we have developed ageneral theory for these excitations as a distinct type of quasi-particles. We called themlongitudinal magnons. They appear in easy-axis magnetic materials, and are characterized by the quantum number Sz = ±2S. They can exist as coherent long-lived excitations for D ≥ |J|, where D and J are the typical single-ion and exchange coupling constants, respectively. Starting with the strong-coupling limit, this work presented different approaches to compute the dispersion of longitudinal magnons. First, a mapping to an effective spin-1/2 model was performed and illustrated for several lattice spin models: the honeycomb-lattice zigzag antiferromagnet and the square-lattice ferro- and antiferromagnet. The excitation energy was derived for different spin values S = 1, 3/2, 2and 5/2. Second, a thorough study explored the S = 1 anisotropic square-lattice, wherethe analytical results of the effective model are compared to the multi-boson spin-wavetheory, the linked-cluster calculations in antiferromagnetic coupling J > 0, and the exactsolution of the two-magnon problem in ferromagnetic coupling J < 0. In the limit of largeJ/D, the longitudinal magnons start to overlap with the multi-magnon continuum, andtheir finite lifetime can be computed using the multi-boson theory, which is specificallyshown for two-magnon decay processes in S = 1. Moreover, critical values of J/D forthe stability of longitudinal magnons are obtained along high-symmetry lines of the Brillouin zone. Third, we investigated the appearance and condensation of the longitudinal magnons in triangular S = 1 antiferromagnets under high magnetic field. As suggested by recent experiments on a candidate material, a spin nematic phase may appear upon condensation of the multipolar excitations, opening the way for realizations of new phases of matter in classically-ordered magnets.In the second part, the correspondence between quantum and classical spins is investigated for spin Hamiltonians at finite temperature. Given a model of quantum spins, it is useful to determine the classical model that best describes its thermodynamics, which is of interest for semi-classical analyses, e.g. by classical Monte Carlo methods. Based on high-temperature series expansions, we established the scaling laws of the different microscopic constants in a quantum spin model, involving quadratic and biquadratic exchange interactions, single-ion anisotropy and the Zeeman energy. We showed that quantum corrections to the thermodynamic quantities are power series in S(S + 1). Subsequently, the findings were applied to numerically determine the phase transition temperature in several ferro- and antiferromagnetic compounds, using classical Monte Carlo simulations. To this aim, the lattice spin models were constructed with microscopic coupling constants from the literature, and the transition temperatures were compared to the experimental values.This illuminates complex collective magnetic behaviors in different models and materials.
This thesis investigates exotic phases of matter in magnetic materials that present anisotropic properties in two dimensions. Using the microscopic spin Hamiltonians, the study addresses two problems: (i) the appearance of a novel class of magnetic excitations in the spectra of anisotropic magnets at zero temperature, and (ii) the quantum-to-classical correspondence of spins for the description of magnetic solids in the disordered phase above the critical temperature. Different analytical and numerical means are used to this purpose.In the first part, motivated by experimental observations of multipolar excitations in afamily of strongly-anisotropic van der Waals antiferromagnets, we have developed ageneral theory for these excitations as a distinct type of quasi-particles. We called themlongitudinal magnons. They appear in easy-axis magnetic materials, and are characterized by the quantum number Sz = ±2S. They can exist as coherent long-lived excitations for D ≥ |J|, where D and J are the typical single-ion and exchange coupling constants, respectively. Starting with the strong-coupling limit, this work presented different approaches to compute the dispersion of longitudinal magnons. First, a mapping to an effective spin-1/2 model was performed and illustrated for several lattice spin models: the honeycomb-lattice zigzag antiferromagnet and the square-lattice ferro- and antiferromagnet. The excitation energy was derived for different spin values S = 1, 3/2, 2and 5/2. Second, a thorough study explored the S = 1 anisotropic square-lattice, wherethe analytical results of the effective model are compared to the multi-boson spin-wavetheory, the linked-cluster calculations in antiferromagnetic coupling J > 0, and the exactsolution of the two-magnon problem in ferromagnetic coupling J < 0. In the limit of largeJ/D, the longitudinal magnons start to overlap with the multi-magnon continuum, andtheir finite lifetime can be computed using the multi-boson theory, which is specificallyshown for two-magnon decay processes in S = 1. Moreover, critical values of J/D forthe stability of longitudinal magnons are obtained along high-symmetry lines of the Brillouin zone. Third, we investigated the appearance and condensation of the longitudinal magnons in triangular S = 1 antiferromagnets under high magnetic field. As suggested by recent experiments on a candidate material, a spin nematic phase may appear upon condensation of the multipolar excitations, opening the way for realizations of new phases of matter in classically-ordered magnets.In the second part, the correspondence between quantum and classical spins is investigated for spin Hamiltonians at finite temperature. Given a model of quantum spins, it is useful to determine the classical model that best describes its thermodynamics, which is of interest for semi-classical analyses, e.g. by classical Monte Carlo methods. Based on high-temperature series expansions, we established the scaling laws of the different microscopic constants in a quantum spin model, involving quadratic and biquadratic exchange interactions, single-ion anisotropy and the Zeeman energy. We showed that quantum corrections to the thermodynamic quantities are power series in S(S + 1). Subsequently, the findings were applied to numerically determine the phase transition temperature in several ferro- and antiferromagnetic compounds, using classical Monte Carlo simulations. To this aim, the lattice spin models were constructed with microscopic coupling constants from the literature, and the transition temperatures were compared to the experimental values.This illuminates complex collective magnetic behaviors in different models and materials.
This thesis investigates two-dimensional quantum antiferromagnets, with a focus on the spin-21 antiferromagnetic easy-axis XXZ model on a square and a honeycomb lattice. Describing the excitations and interactions of magnons in these models is of substantial interest, as magnons are the fundamental quasiparticles and can thus explain experimental observations. Already for the paradigmatic antiferromagnetic spin-21 Heisenberg model on the square lattice, high-energy features of the magnon dispersion are understood via strong magnon-magnon interactions. Besides that, interesting high-energy features were recently observed in the honeycomb lattice, including a possible decay of the single-magnon mode. The goal of this thesis is to obtain effective descriptions of the aforementioned systems that capture the relevant features of the magnon excitations and their interactions. To study these features, this thesis employs continuous similarity transformations (CSTs), which enables a systematic derivation of an effective quasiparticle picture via so-called flow equations. The approach enables decoupling different magnon sectors and thus for investigating ground-state properties, single-magnon excitations, and multi-magnon bound states. The magnon description is derived from the non-Hermitian Dyson-Maleev representation, which describes fluctuations around a long-range magnetically ordered ground state. The flow equations are set up in momentum space, truncated by the scaling dimension, retaining only operators up to scaling dimension of two, and solved numerically. For the square lattice, a magnon-conserving effective Hamiltonian is obtained across the full anisotropy range by interpolating between the Ising limit and the Heisenberg limit. The ground-state energy, staggered magnetization, dispersion, and critical exponents are in excellent agreement with the literature, supporting the validity of CST also for gapped phases. Two-magnon excitations in the Sz=0 subspace comprise four bound states, which are tracked across the anisotropy range. Their successive decay into the two-magnon continuum is determined by using the inverse participation ratio. For the honeycomb lattice, the magnon-conserving CST is reliable only up to λ≲0.57; an adapted CST scheme that decouples only the ground state while preserving couplings between different higher-magnon sectors yields effective descriptions for all λ and confirms stable long-range order. The low-energy properties determined in this way match the literature values. However, in the Heisenberg limit, the adapted approach fails to capture high-energy features, such as the experimentally observed decay into the multi-particle continuum at corners of the Brillouin zone. A termination of the magnon-conserving flow equations at a finite flow parameter before the divergence reveals a single-magnon decay at high energies, which is connected to a crossing of a two-magnon bound state with the single-magnon mode. The observed energy dip qualitatively agrees with Quantum Monte Carlo results, but magnon–magnon interactions are overestimated, hindering a fully quantitative characterization of the single-magnon dispersion. Analyzing multi-magnon bound states over the anisotropy range unveils that the crossing of a three-magnon bound state with the single-magnon mode accounts for the breakdown of the magnon-conserving CST at higher λ. This work demonstrates that CST with scaling-dimension truncation provides a powerful framework for studying two-dimensional quantum magnets, capturing low-energy properties and bound states. Nevertheless, challenges remain in accurately describing high-energy features arising from a persistent overlap of magnon sectors due to strong binding effects.
We investigate the quantum dynamics of the spins on different Heisenberg antiferromagnetic spin lattice systems. Firstly, we applied the coupled-cluster method to the spin-1/2 antiferromagnetic \emph{XXZ} model on a square lattice by employing an approximation which contains two-body long-range correlations and high-order four-body local correlations. Improvement is found for the ground-state energy, sublattice magnetization, and the critical anisotropy when comparing with the approximation including the two-body correlations alone. We also obtain the full excitation spectrum which is in good agreement with the quantum Monte Carlo results and the high-order spin-wave theory.Secondly, we study the longitudinal excitations of quantum antiferromagnets on a triangular lattice by a recently proposed microscopic many-body approach based on magnon-density waves. We calculate the full longitudinal excitation spectra of the antiferromagnetic Heisenberg model for a general spin quantum number in the isotropic limit. Similar to the square lattice model, we find that, at the center of the first hexagonal Brillouin zone Γ(q=0) and at the magnetic ordering wavevectors ±[Q=(4π/3,0)], the excitation spectra become gapless in the thermodynamic limit, due to the slow, logarithmic divergence of the structure factor. However, these longitudinal modes on two-dimensional models may be considered as quasi-gapped, as any finite-size effect or small anisotropy will induce a large energy gap, when compared with the counterpart of the transverse spin-wave excitations. We have also investigated the excited states of the quasi-one-dimensional quantum antiferromagnets on hexagonal lattices, including the longitudinal modes based on the magnon-density waves. A model Hamiltonian with a uniaxial single-ion anisotropy is first studied by a spin-wave theory based on the one-boson method; the ground state thus obtained is employed for the study of the longitudinal modes. The full energy spectra of both the transverse modes (i.e., magnons) and the longitudinal modes are obtained as functions of the nearest-neighbor coupling and the anisotropy constants. We have found two longitudinal modes due to the non-collinear nature of the triangular antiferromagnetic order, similar to that of the phenomenological field theory approach by Affleck. The excitation energy gaps due to the anisotropy and the energy gaps of the longitudinal modes without anisotropy are then investigated. We then compares our results for the longitudinal energy gaps at the magnetic wavevectors with the experimental results for several antiferromagnetic compounds with both integer and non-integer spin quantum numbers, and we find good agreements after the higher-order contributions are included in our calculations.
Classical and quantum spin systems are widely used models in both experimental and theoretical condensed matter physics. In many materials, the electronic interactions can be difficult to model exactly. However, in some insulators (Mott insulators), the magnetic (spin) interactions can be captured well with spin-only models. Several models are studied in this thesis. First, I report the solution of a long-standing issue in a classical frustrated spin model (i.e., where the quantum effects are neglected and the complexity is due to competing interactions): the nature of the thermal phase transition to a stripe state in the two dimensional (2D) J1-J2 model. Here J1 and J2 are nearest- and next-nearest-neighbor couplings. Monte Carlo simulations with single-spin updates are used for the calculations, and an extended-ensemble method, a generalization of the Wang-Landau algorithm, is also developed and tested. I focus on the study of "weak universality" behavior (continuously varying critical exponents, with one of the exponents staying fixed), for which I show a correspondence with a known class of conformal field theories with charge c = 1. Next, moving to quantum spins, to shed light on magnetic systems studied experimentally and to investigate new types of quantum states of interest in developing theories of quantum magnetism, I study the S = 1/2 Heisenberg model on the 2D square lattice with added six-spin interactions (the so-called J-Q3 model) as well as a set of 3D quantum antiferromagnets on dimerized lattices. Here I use the stochastic series expansion quantum Monte Carlo method. In the study of the J-Q3 model, I report on a similar weak-universality behavior as in the classical J1-J2 model, but with a mapping to a different known class of c = 1 conformal field theories. The critical behavior of the system again shows continuously changing exponents, in a way which corresponds to a gradual weakening of Z4 symmetry-breaking to an emergent U(1) symmetry. In the study of dimerized antiferromagnets, I report on a universal behavior of the Néel temperature TN, which can be related to ground state parameters independently of the microscopic interaction details in several different models.
Materials with strongly correlated electrons show a multitude of unconventional phenomena, such as superconductivity or magnetism, that cannot be explained in a single-particle picture and necessitate to take many-body effects into account. A route to explain the origin of these phenomena consists in constructing effective models for these materials that are then solved, often using numerical techniques. Paradigmatic models for two different classes of strongly correlated electron systems are investigated in this thesis: The Hubbard model is a paradigmatic model to describe the Mott metal-insulator transition (MIT) and the Kondo lattice model describes the low-energy physics in heavy fermion compounds. Both models are analyzed numerically using different variations of a quantum cluster technique, the variational cluster approximation (VCA). The first part focuses on the MIT, as it is investigated experimentally in quasi-two-dimensional charge-transfer salts. Its nature and associated universality class are still heavily discussed and both experiments and theoretical approaches come to different conclusions. In this thesis, the Mott transition is investigated on an anisotropic two-dimensional Hubbard model at half-filling. By using a control parameter, which induces this anisotropy, strong evidence for Mott quantum criticality is found in weakly coupled Hubbard chains. The results at zero temperature show that the second-order critical end point Tc of the interaction-driven metal-insulator transition can be tuned down to zero at strong anisotropy. Further results for the antiferromagnetic phase suggest a similar picture and motivate adding the anisotropy as a new axis in the phase diagram to account for a low-temperature critical end point of the Mott transition. The second part of this thesis focuses on unconventional phases that emerge in a paradigmatic model for heavy fermion systems, the Kondo lattice model. Using the VCA, the two-dimensional Kondo lattice model is investigated in the paramagnetic phase as well as in phases with broken symmetry. An antiferromagnetic phase at weak coupling and a phase with Kondo-singlet formation at strong coupling are analyzed. Within the antiferromagnetically ordered region, two phases with different Fermi-surface topology, which are separated by a discontinuous transition, are identified. The model is also tested for s-wave superconductivity as found recently using dynamical mean-field theory, but no indications for robust local pairing are seen within VCA. Instead, nodal d-wave superconductivity is found and analyzed in a large range of couplings and electron fillings, and its interplay with antiferromagnetic order at weak coupling is discussed. This motivates further studies on extended models that might allow for a close comparison with experiments on heavy fermion systems. Understanding the formation of unconventional phases in strongly correlated electron systems is not only of fundamental interest, but it is also essential for designing new functional materials. Although the results of approximate cluster techniques have to be handled with care, the new aspects presented in this thesis pave the way for further investigations in this direction.
In this thesis the elementary excitations of the spin-1=2 Heisenberg antiferromagnet on the square lattice are studied. This fundamental model is a paradigmatic example for long range ordered quantum phases and the spontaneous breaking of a continuous symmetry in condensed matter. The elementary excitations at long wavelengths are well understood by quantized spin waves, i.e., magnons, which are the gapless Goldstone bosons of the broken SU(2) symmetry. However, recent findings reveal an anomalous energy dip at short wavelengths, which cannot be explained by the conventional spin wave theory. The nature of spin waves at short wavelengths remains unclear to this day. A central aim of this thesis is the derivation of an effective magnon description for the square lattice antiferromagnet which is quantitatively valid for all length scales. For this purpose, the method of continuous unitary transformations (CUT) is extended to its use for gapless excitations. CUT methods provide a powerful tool for the derivation of effective quasi-particle descriptions by means of flow equations. However, typical approaches are truncated in real space restricting their scope of application to gapped quantum phases. In order to circumvent these limitations a CUT approach in momentum space is developed. The scaling dimension of operator terms is established as a suitable truncation criterion for gapless quasi-particles. Moreover, a diagrammatic representation of operator terms is introduced which simplifies the derivation and interpretation of flow equations in momentum space. The developed approach is used to transform the Heisenberg Hamiltonian into an effective Hamiltonian which conserves the number of magnons. In addition, effective observables required for the theoretical description of inelastic neutron scattering are derived. The initial magnon operators before the transformation are defined by the Dyson-Maleev representation which leads to a superficially non-hermitian Hamiltonian. As a result, the transformation constitutes a continuous similarity transformation (CST). This formalism enables the formulation of spin wave interactions by means of quartic boson operators. A crucial step of the transformation is the proper renormalization of the spin wave interaction which is achieved by a selfsimilar CST for scaling dimension d = 2. The resulting effective magnon description is consistent at all length scales. In particular, the magnon dispersion exhibits an energy dip at short wavelengths which is in quantitative agreement with recent numerical and experimental data. Further analysis of the spectral properties indicates a strong attraction between spin waves giving rise to a resonance in the longitudinal two-magnon channel. This resonance can be interpreted as the amplitude or Higgs mode of the continuously broken SU(2) symmetry with finite lifetime. The origin of the anomalous dispersion is ascribed to a scattering between the Higgs resonance and single magnon states. The theoretical results are directly compared with experimental data obtained by inelastic neutron scattering and various numerical results which support this view. The quantitative agreement between the effective spin wave approach and numerous numerical and experimental findings shows that magnons are a valid description of the elementary excitations at all length scales. Therefore, this thesis provides a final settlement of the question about the nature of the elementary excitations in the square lattice quantum antiferromagnet.
Based on our recently proposed magnon-density-waves using the microscopic many- body approach, we investigate the longitudinal excitations in quantum antiferromagnets by including the second order corrections in the large-s expansion. The longitudinal excitation spectra for a general spin quantum number using the antiferromagnetic Heisenberg Hamiltonian are obtained for various spin lattice models. For bipartite lattice models, we find that the numerical results for the energy gaps for the longitudinal modes at q → 0 and the magnetic ordering wavevector Q are reduced by about 40-50 % after including the second order corrections. Thus, our estimate of the energy gaps for the quasi-one-dimensional (quasi- 1D) antiferromagnetic compound KCuF 3 is in better agreement with the experimental result. For the quasi-1D antiferromagnets on hexagonal lattices, the full excitation spectra of both the transverse modes (i.e., magnons) and the longitudinal modes are obtained as functions of the nearest-neighbor coupling and the anisotropy constants. We find two longitudinal modes due to the non-collinear nature of the triangular antiferromagnetic order, similar to that of the phenomenological field theory approach by Affleck. We compare our results for the longitudinal energy gaps at the magnetic wavevectors with the experimental results for several antiferromagnetic compounds with both integer and non-integer spin quantum numbers, and also find good agreement after the higher-order contributions are included in our calculations.