In spin lattices, frustration happens when there exists a competition between different terms of the Hamiltonian, which cannot be simultaneously minimized in all local physical bases. Frustration can destabilize the bipartite Neel order, which is the conventional groundstate of antiferromagnetic Heisenberg-type models in two dimensions. Hence, the focus of two-dimensional quantum magnetism studies has been directed toward elucidating the zero-temperature properties of Heisenberg-type models on the Archimedean lattices that exhibit geometrical frustration. This type of frustration is of great interest since it can lead to exotic forms of the quantum matter, such as topological spin-liquid (SL) and many-sublattice long-range-ordered phases. The spin-1/2 triangular Heisenberg model (THM) is a prototypical model with geometrical frustration, which has the highest coordination number of all Archimedean lattices. However, there exist two major, distinct difficulties for numerical methods to efficiently determine the groundstate properties of the THM: the immense dimension of the Hilbert space and the geometrical frustration phenomenon. In this thesis, to deal with such difficulties, we employ the state-of-the- art non-Abelian matrix product states (MPS) and density matrix renormalization group (DMRG) methods. We exploit the symmetries of the Hamiltonian to reduce the working dimension of the Hilbert space and, to lessen the effects of the geometrical frustration, we depend on the local entanglement (area-law) nature of the MPS as it scales with the size of a lattice subspace with reduced spatial dimensions. In such a way, we thoroughly examine the phase diagram of the THM with nearest and next-nearest neighbor (NN and NNN) exchange couplings on finite- and infinite-length cylinders of widths up to 12 sites. In addition, we develop new numerical tools to analyze topological and symmetry-broken phases in the context of the SU(2)-symmetric translation-invariant MPS algorithm. We establish that on infinite cylinders, the anyonic sectors of a topological order can be classified through the fractionalization of global symmetries and degeneracy patterns of the entanglement spectrum (ES). On the other hand, we detect symmetry-breaking phase transitions by a combination of the correlation lengths and second and fourth cumulants of the magnetic order parameters, even though symmetry implies that the order parameter itself is strictly zero. Furthermore, the appearance of Nambu-Goldstone modes in the excitation spectrum can be detected using “tower of states” (TOS) levels in the momentum-resolved ES. By applying the new tools to the THM, we discover a variety of exotic groundstates such as a Z2-gauge toric-code-type topological order (with vison and spinon excitations), a NNN Majumdar-Gosh, and a long-range 120◦-ordered state.
In spin lattices, frustration happens when there exists a competition between different terms of the Hamiltonian, which cannot be simultaneously minimized in all local physical bases. Frustration can destabilize the bipartite Neel order, which is the conventional groundstate of antiferromagnetic Heisenberg-type models in two dimensions. Hence, the focus of two-dimensional quantum magnetism studies has been directed toward elucidating the zero-temperature properties of Heisenberg-type models on the Archimedean lattices that exhibit geometrical frustration. This type of frustration is of great interest since it can lead to exotic forms of the quantum matter, such as topological spin-liquid (SL) and many-sublattice long-range-ordered phases. The spin-1/2 triangular Heisenberg model (THM) is a prototypical model with geometrical frustration, which has the highest coordination number of all Archimedean lattices. However, there exist two major, distinct difficulties for numerical methods to efficiently determine the groundstate properties of the THM: the immense dimension of the Hilbert space and the geometrical frustration phenomenon. In this thesis, to deal with such difficulties, we employ the state-of-the- art non-Abelian matrix product states (MPS) and density matrix renormalization group (DMRG) methods. We exploit the symmetries of the Hamiltonian to reduce the working dimension of the Hilbert space and, to lessen the effects of the geometrical frustration, we depend on the local entanglement (area-law) nature of the MPS as it scales with the size of a lattice subspace with reduced spatial dimensions. In such a way, we thoroughly examine the phase diagram of the THM with nearest and next-nearest neighbor (NN and NNN) exchange couplings on finite- and infinite-length cylinders of widths up to 12 sites. In addition, we develop new numerical tools to analyze topological and symmetry-broken phases in the context of the SU(2)-symmetric translation-invariant MPS algorithm. We establish that on infinite cylinders, the anyonic sectors of a topological order can be classified through the fractionalization of global symmetries and degeneracy patterns of the entanglement spectrum (ES). On the other hand, we detect symmetry-breaking phase transitions by a combination of the correlation lengths and second and fourth cumulants of the magnetic order parameters, even though symmetry implies that the order parameter itself is strictly zero. Furthermore, the appearance of Nambu-Goldstone modes in the excitation spectrum can be detected using “tower of states” (TOS) levels in the momentum-resolved ES. By applying the new tools to the THM, we discover a variety of exotic groundstates such as a Z2-gauge toric-code-type topological order (with vison and spinon excitations), a NNN Majumdar-Gosh, and a long-range 120◦-ordered state.
We present new numerical tools to analyze symmetry-broken phases in the context of SU(2)-symmetric translation-invariant matrix product states (MPS) and density-matrix renormalization-group (DMRG) methods for infinite cylinders, and determine the phase diagram of the geometrically frustrated triangular Heisenberg model with nearest- and next-nearest-neighbor (NN and NNN) interactions. The appearance of Nambu-Goldstone modes in the excitation spectrum is characterized by ``tower of states'' levels in the momentum-resolved entanglement spectrum. Symmetry-breaking phase transitions are detected by a combination of the correlation lengths and second and fourth cumulants of the magnetic order parameters (which we call the Binder ratio), even though symmetry implies that the order parameter itself is strictly zero. Using this approach, we have identified a ${120}^{\ensuremath{\circ}}$ order, a columnar order, and an algebraic spin liquid (specific to width-6 systems), alongside the previously studied topological spin liquid phase. For the latter, we also demonstrate robustness against chiral perturbations.
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.
When sizable quantum fluctuations and strong frustration mechanisms act in concert to repel the formation of conventional long-range order in quantum magnets, they can make way for massively entangled spin liquid phases which may imbue the material with extraordinary properties. \nThe search for such curious phases of matter has proceeded for several decades, gaining extra momentum some fifteen years ago when Kitaev proposed an analytically solvable model for a quantum spin liquid with anyonic excitations on the basis of realistic microscopic spin exchange terms [Kitaev, Annals of Physics 321, 2 (2006)]. Attempts to identify different models or materials which harbor quantum spin liquid ground states have kept researchers -- experimentalists and theorists alike -- in suspense ever since. However, the simulation of quantum many-body systems poses a serious challenge even to modern numerical techniques, particularly in the case of frustrated quantum magnetism in three spatial dimensions. Such models evade tractability by many established approaches, leaving a methodological void. \n \nIn this thesis, we report on recent progress in cutting-edge implementations of the pseudo-fermion functional renormalization group (pf-FRG), which has originally been proposed by Reuther and Wölfle in the context of two-dimensional frustrated quantum magnetism with highly symmetric spin interactions [Reuther and Wölfle, Phys. Rev. B 81, 144410 (2010)]. Reflecting the growing interest in models with SU(2) symmetry-breaking spin exchange terms that has followed the unearthing of Kitaev's honeycomb model, we present a generalized implementation of the pf-FRG which is suited to numerically simulate arbitrary microscopic models with diagonal or off-diagonal two-spin interactions, even in three-dimensional frustrated quantum magnets. We provide insight into the inner workings of the method which has emerged over the course of the last couple of years, arguing that the pf-FRG formalism simultaneously combines aspects of a large-S expansion as well as a large-N expansion on equal footing, thus being able to resolve the subtle interplay between magnetic ordering tendencies and disruptive quantum fluctuations. \n \nMoreover, on a case by case basis we explore the stability of quantum spin liquids in paradigmatic models of frustrated quantum magnetism and elucidate the joint action of geometric frustration, exchange frustration, and quantum fluctuations to inhibit the formation of magnetic long-range order. Examples include: (i) a Heisenberg spin model on the three-dimensional diamond lattice where geometric frustration arises from antiferromagnetic next-nearest neighbor interactions. The additional competition with nearest neighbor interactions leads to an unusually large ground state degeneracy already on classical level. The quantum-to-classical transition is studied by systematically varying the spin length and the different roles of quantum fluctuations and thermal fluctuations are discussed. The theory is applied to interpret experiments on the spin-liquid candidate NiRh2O4; (ii) a Heisenberg antiferromagnet on the face centered cubic lattice which is augmented by competing bond-directional interactions, evolving around the concurrent manifestation of geometric frustration and exchange frustration. A situation is identified where both mechanisms collude to give rise to an unusually large degree of frustration over a wide parameter regime. We discuss related experimental findings on the highly frustrated iridate compound Ba2CeIrO6; (iii) a Heisenberg antiferromagnet on the kagome lattice with additional Dzyaloshinskii-Moriya interactions. The robustness of the unperturbed kagome antiferromagnet's spin liquid ground state against low-symmetry Dzyaloshinskii-Moriya interactions is investigated. Implications for the spin-liquid candidate herbertsmithite are discussed.
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.
Interactions between the microscopic constituents of a solid---a many-body system--- can lead to novel phases and exotic physical phenomena like fractionalization, topological order, quantum spin liquids, emergent gauge field, etc.. The concept of frustration provides a ground for such exotic phenomena. Frustration can prevent a many-body system from establishing long-range order down to the lowest temperatures due to competing interactions. Instead, competing interactions may result in disordered and liquid-like phases of matter that provide the vacuum for fractional excitations. The absence of any order parameter in strongly frustrated systems---due to not breaking any symmetry spontaneously--- immediately raises the question about possible experimental probes of spin-liquids and their fractional excitations. Dynamic probes, like inelastic neutron scattering or Raman scattering, provide an experimental method to detect signatures of fractionalised quasiparticles. The energy and momentum transferred in a scattering event is split between the fractional quasiparticles. On the theory side, computing such dynamical signatures beyond one spatial dimension is generally a difficult task. In this thesis, numerical methods like density matrix renormalisation group and matrix product states are used to study strongly frustrated magnets and their dynamics in a non-perturbative way. This thesis covers two physical models in the context of frustration and emergent gauge fields. Firstly, the Kitaev model of spin-1/2 degrees of freedom subject to strongly anisotropic spin exchange. The Kitaev model features quantum spin liquid ground states with fractionalization of spins into Majorana fermions and Z_2-fluxes---the visons of an emergent Z_2 gauge theory. The main questions addressed here concern the stability of the quantum spin liquid phase upon adding perturbations relevant in magnetic compounds such as Heisenberg or the symmetric-offdiagonal Gamma exchange. Applying a magnetic field drives the Kitaev model into a topologically ordered phase. The excitations and dynamical signatures within the spin liquid, the topologically ordered phase, and within ordered phases are studied. Secondly, a classical minimal model of the proton configuration in water ice is studied. The ice rules, a local constraint describing the low energy manifold, result in emergent Maxwell's equation. Upon applying an external electric field along certain axis, a polarization plateau occurs in which the remaining degrees of freedom can be described by dimers on two-dimensional lattices.
Frustrated magnetism provides a rich platform for realizing exotic quantum phases in condensed matter systems. Among these, quantum spin liquids (QSLs) are a particularly intriguing class of states that exhibit no magnetic ordering and preserve all symmetries down to zero temperature. Just as conventional magnets can be thought of as spin crystals,QSLs represent their liquid analogs. This thesis explores two broad types of QSLs in two-dimensional magnets, with a focus on their dynamic properties and the nature of transitions from conventional magnetic states into QSL phases. QSLs are topological phases that host fractionalized excitations known as spinons. In these states, mobile spinons are coupled to an emergent gauge field, forming a highly entangled phase of matter. The first part of this thesis focuses on Dirac spin liquids (DSLs), a class of QSLs where spinons exhibit a gapless Dirac dispersion. To study the dynamicsof these spin liquids beyond leading-order mean-field theory, we develop a novel large-N fermionic limit of gapless spinons. In this limit, all gauge excitations are suppressed, and the leading-order corrections instead arise from order parameter fluctuations, which may condense and drive transitions into symmetry-broken phases from the parent DSL. Incorporating random phase approximation (RPA) corrections to the spin susceptibility, we find that sharp, spin-wave–like modes are recovered in the excitation spectrum. This methodology successfully captures characteristic features of the dynamics near phase transitions and in weakly symmetry-broken phases proximate to a DSL. We apply this approach to microscopic models, including the J1-J2 XXZ model on the triangular lattice and the J1-J3 XXZ model on the honeycomb lattice. These models closely represent a wide range of frustrated materials, such as triangular and honeycomb cobaltates and triangular ytterbium compounds. Our theoretical predictions show excellent agreement with experimentally measured inelastic neutron scattering spectra from these materials. Gapless spinons can also sometimes become gapped through chiral symmetry breaking, leading to the formation of a chiral spin liquid (CSL). The CSL is an archetypal bosonic realization of a fractional quantum Hall (FQH) state at half-filling, and has been proposed as a time-reversal–breaking ground state in a variety of frustrated spin models. The second part of this thesis addresses the intriguing possibility of realizing a CSL through the "melting" of a chiral spin crystal—a conventional magnet with non-coplanar ordering. Such a transition offers a physically appealing analogue to the melting of a Wigner crystal into a fermionic FQH liquid. Focusing on the kagome lattice, where chiral interactions are knownto stabilize a CSL ground state, we study the effects of additional long-range Heisenberg interactions and demonstrate a phase transition into a non-coplanar octahedral magnetic order. To describe the universal class of transition between a CSL and a non-coplanar anti-ferromagnetic order, we then develop a novel Chern-Simons–matter field theory framework, constrained by symmetry principles and symmetry fractionalization patterns. This thesis thus provides new insights into the dynamical signatures and phase transitions of quantum spin liquids, offering a bridge between theoretical models and experimental observations in frustrated magnetic systems.