Recent discovery of the half quantized thermal Hall conductivity in $α$-RuCl$_3$, a candidate material for the Kitaev spin liquid, suggests the presence of a highly entangled quantum state in external magnetic fields. This field induced phase appears between the low field zig-zag magnetic order and the high field polarized state. Motivated by this experiment, we study possible field induced quantum phases in theoretical models of the Kitaev magnets, using the two dimensional tensor network approach or infinite tensor product states. We find various quantum ground states in addition to the chiral Kitaev spin liquid occupying a small area in the phase diagram. They form a band of emergent quantum phases in an intermediate window of external magnetic fields, somewhat reminiscent of the experiment. We discuss the implications of these results in view of the experiment and previous theoretical studies.
We study the 3D Kitaev and Kitaev-Heisenberg models respectively on the hyperhoneycomb and hyperoctagon lattices, both at zero and finite-temperature, in the thermodynamic limit. Our analysis relies on advanced tensor network (TN) simulations based on graph Projected Entangled-Pair States (gPEPS). We map out the TN phase diagrams of the models and characterize their underlying gapped and gapless phases both at zero and finite temperature. In particular, we demonstrate how cooling down the hyperhoneycomb system from high-temperature leads to fractionalization of spins to itinerant Majorana ferm…
We investigate the Kitaev-Heisenberg (KH) model at finite temperature using the exact environment full update (eeFU), introduced in Phys. Rev. B 99, 035115 (2019), which represents the purification of a thermal density matrix on an infinite hexagonal lattice by an infinite projected entangled pair state (iPEPS). We show that thanks to a dynamical mapping from a hexagonal to a rhombic lattice, the eeFU on the hexagonal lattice is as efficient as the simple full update (FU) algorithm. Critical temperatures for coupling constants in the stripy and the antiferromagnetic phase are estimated. They a…
Contrasting ground states of quantum magnets with the integer and half-integer spin moments are the manifestation of many-body quantum interference effects. In this work, we investigate the distinct nature of the integer and half-integer spin quantum spin liquids in the framework of the Kitaev's model on the honeycomb lattice. The models with arbitrary spin quantum numbers are not exactly solvable in contrast to the well-known quantum spin liquid solution of the spin-1/2 system. We use the tensor network wavefunctions for the integer and half-integer spin quantum spin liquid states to unveil t…
By using the variational Monte Carlo method, we study the magnetization process of the Kitaev honeycomb model in a magnetic field. Our trial wavefunction is a generalized Bardeen-Cooper-Schrieffer wave function with the Jastrow correlation factor, which exactly describes the ground state of the Kitaev model at zero magnetic field using the Jordan-Wigner (JW) transformation. We find that two phase transitions occur for the antiferromagnetic Kitaev coupling, while only one phase transition occurs for the ferromagnetic Kitaev coupling. For the antiferromagnetic Kitaev coupling, we also find that …
We study the extent of the spin liquid phases in the Kitaev-Heisenberg model using infinite Projected Entangled-Pair States tensor network ansatz wave functions directly in the thermodynamic limit. To assess the accuracy of the ansatz wave functions we perform benchmarks against exact results for the Kitaev model and find very good agreement for various observables. In the case of the Kitaev-Heisenberg model we confirm the existence of 6 different phases: Néel, stripy, ferromagnetic, zigzag and two spin liquid phases. We find finite extents for both spin liquid phases and discontinuous phase t…
Materials that realize Kitaev spin models with bond-dependent anisotropic interactions have long been searched for, as the resulting frustration effects are predicted to stabilize novel forms of magnetic order or quantum spin liquids. Here we explore the magnetism of $γ$-Li$_2$IrO$_3$, which has the topology of a 3D Kitaev lattice of inter-connected Ir honeycombs. Using resonant magnetic x-ray diffraction we find a complex, yet highly-symmetric incommensurate magnetic structure with non-coplanar and counter-rotating Ir moments. We propose a minimal Kitaev-Heisenberg Hamiltonian that naturally …
A range of honeycomb-lattice compounds has been proposed and investigated in the search for a topological Kitaev spin liquid. However, sizable Heisenberg interactions and additional symmetry-allowed exchange anisotropies in the magnetic Hamiltonian of these potential Kitaev materials push them away from the pure Kitaev spin-liquid state. Particularly the Kitaev-to-Heisenberg coupling ratio is essential in this respect. With the help of advanced quantum-chemistry methods, we explore how the magnetic coupling ratios depend on pressure in several honeycomb compounds (Na$_2$IrO$_3$, $β$-Li$_2$IrO$…
We investigate the ground state properties of the spin S=1 Kitaev honeycomb model under a magnetic field based on the density matrix renormalization group (DMRG) calculation. With the time reversal symmetry breaking due to the magnetic field, a gapped Kitaev spin liquid is identified for both ferromagnetic (FM) and antiferromagnetic (AFM) Kitaev couplings. The topological nature of such Kitaev spin liquid is manifested by the nearly quantized Wilson loop, degeneracy in the entanglement spectra and existence of edge modes. While the FM Kitaev spin liquid is destroyed by a weaker magnetic field …
We study the effects of static magnetic and electric fields on Kitaev's honeycomb model. Using the electric polarization operator appropriate for Kitaev materials, we derive the effective Hamiltonian for the emergent Majorana fermions to second-order in both the electric and magnetic fields. We find that while individually each perturbation does not qualitatively alter Kitaev spin liquid, the cross-term induces a finite chemical potential at each Dirac node, giving rise to a Majorana-Fermi surface. We argue this gapless phase is stable and exhibits typical metallic phenomenology, such as linea…
We investigate magnetic properties in the $S=1$ Kitaev model in the anisotropic limit. Performing the fourth-order perturbation expansion with respect to the $x$-bonds, $y$-bonds, and magnetic field, we derive the effective Hamiltonian, where the low-energy physics should be described by the free spins with an effective magnetic field. Making use of the exact diagonalization method for small clusters, we discuss ground-state properties in the system complementary.
The magnetic field response of the Mott-insulating honeycomb iridate Na$_{2}$IrO$_{3}$ is investigated using torque magnetometry measurements in magnetic fields up to 60 tesla. A peak-dip structure is observed in the torque response at magnetic fields corresponding to an energy scale close to the zigzag ordering ($\approx 15~K$) temperature. Using exact diagonalization calculations, we show that such a distinctive signature in the torque response constrains the effective spin models for these classes of Kitaev materials to ones with dominant ferromagnetic Kitaev interactions, while alternative…
In recent years, there has been an intense search for materials realizing the Kitaev quantum spin liquid model. A number of edge-shared compounds with strong spin-orbit coupling, such as RuCl$_3$ and iridates, have been proposed to realize this model. Nevertheless, an effective spin Hamiltonian derived from the microscopic model relevant to these compounds generally contains terms that are antagonistic toward the quantum spin liquid. This is consistent with the fact the zero magnetic field ground state of these materials is generally magnetically ordered. It is a pressing issue to identify pro…
Topological and Trivial Valence-Bond Orders in Higher-Spin Kitaev Models
Ghent University（根特大学）；University of Amsterdam（阿姆斯特丹大学）；Rudolf Peierls Centre for Theoretical Physics, Clarendon Laboratory, Parks Road, Oxford OX1 3PU, United Kingdom（鲁道夫·皮尔斯理论物理中心，克拉伦登实验室，英国牛津公园路）
We study periodically driven pure Kitaev model and ferromagnetic phase of the Kitaev-Heisenberg model on the honeycomb lattice by off-resonant linearly and circularly-polarized lights at zero magnetic field. Using a combination of linear spin wave and Floquet theories, we show that the effective time-independent Hamiltonians in the off-resonant regime map onto the corresponding anisotropic static spin model, plus a tunable photoinduced magnetic field along the $[111]$ direction, which precipitates Floquet topological magnons and chiral magnon edge modes. They are tunable by the light amplitude…
We study the response of the Kitaev spin liquid (KSL) to a local magnetic field perpendicular to the Kitaev honeycomb lattice. The local magnetic field induces a dynamical excitation of a flux pair in the spin liquid and the system can be described by a generally particle-hole asymmetric interacting resonant level model. The dynamical excitation of the flux pair closes the flux gap in the spectrum of the spin correlation function locally for the gapless KSL even from the perturbative response to a weak magnetic field. Beyond the perturbative regime, the p-h asymmetry competes with the magnetic…
The insulating honeycomb magnet $α$-RuCl$_{3}$ exhibits fractionalized excitiations that signal its proximity to a Kitaev quantum spin liquid (QSL) state, however, at $T=0$, fragile long-range magnetic order arises from non-Kitaev terms in the Hamiltonian. Spin vacancies in the form of Ir$^{3+}$ substituted for Ru are found to destabilize this long-range order. Neutron diffraction and bulk characterization of Ru$_{1-x}$Ir$_{x}$Cl$_{3}$ show that the magnetic ordering temperature is suppressed with increasing $x$ and evidence of zizag magnetic order is absent for $x>0.3$. Inelastic neutron scat…
The Kitaev model exhibits a Quantum Spin Liquid hosting emergent fractionalized excitations. We study the Kitaev model on the honeycomb lattice coupled to a magnetic field along the [111] axis. Utilizing large scale matrix product based numerical models, we confirm three phases with transitions at different field strengths depending on the sign of the Kitaev exchange: a non-abelian topological phase at low fields, an enigmatic intermediate regime only present for antiferromagnetic Kitaev exchange, and a field-polarized phase. For the topological phase, we numerically observe the expected cubic…
Recent experiments on Kitaev spin liquid candidate materials reported non-monotonic behavior of thermal conductivity as a function of magnetic field, which lead to conflicting interpretations of its origin. Motivated by this development, we study the magnetic field dependence of thermal conductivity of a generalized Kitaev model, which allows the phase transitions between different flux sectors as a function of the magnetic field. The thermal conductivity due to Majorana fermions shows dip-bump structures as the magnetic field increases, which is caused by either the transitions between differ…
We consider the quasi-two-dimensional pseudo-spin-1/2 Kitaev - Heisenberg model proposed for A2IrO3 (A=Li, Na) compounds. The spin-wave excitation spectrum, the sublattice magnetization, and the transition temperatures are calculated in the random phase approximation (RPA) for four different ordered phases, observed in the parameter space of the model: antiferomagnetic, stripe, ferromagnetic, and zigzag phases. The Néel temperature and temperature dependence of the sublattice magnetization are compared with the experimental data on Na2IrO3.
Relevance of on-site and intersite Coulomb interactions in the Kitaev-Heisenberg magnet Na$_3$Co$_2$SbO$_6$
Institute for Theoretical Solid State Physics, Leibniz IFW Dresden（德累斯顿亥姆霍兹中心莱布尼茨研究所理论固态物理研究所）；Department of Physics, Karpagam Academy of Higher Education（卡尔帕甘高等教育学院物理系）；Centre for Computational Physics, Karpagam Academy of Higher Education（卡尔帕甘高等教育学院计算物理中心）；School of Physics, University of Melbourne（墨尔本大学物理学院）；Department of Physics, Technical University Dresden（德累斯顿工业大学物理系）
The layered honeycomb magnet $α$-Li$_2$IrO$_3$ has been theoretically proposed as a candidate to display novel magnetic behaviour associated with Kitaev interactions between spin-orbit entangled $j_{\rm eff}=1/2$ magnetic moments on a honeycomb lattice. Here we report single crystal magnetic resonant x-ray diffraction combined with powder magnetic neutron diffraction to reveal an incommensurate magnetic order in the honeycomb layers with Ir magnetic moments counter-rotating on nearest-neighbour sites. This type of magnetic structure has not been reported experimentally before in honeycomb magn…
We investigate the quantum spin liquid (QSL) ground state of anisotropic Kitaev model with antiferromagnetic (AFM) coupling under the $[001]$ magnetic field with the finite-temperature Lanczos method (FTLM). In this anisotropic AFM Kitaev model with $K_{X}=K_{Y}$, $K_{X}+K_{Y}+K_{Z}=-3K$, and $K_{Z}<-K$, with magnetic field increasing, the gapped QSL experiences a transition to a gapless QSL at $h_{c1}=gμ_{B}H_{z1}/K$, to another gapless QSL with $C_{6}$ rotational symmetry at $h_{c2}$, and to a new $U(1)$ gapless QSL between $h_{c3}$ and $h_{c4}$, respectively. These indicate that magnetic fi…
We have investigated the field-angle behaviors of magnetic excitations under an in-plane magnetic field for proximate Kitaev systems. By employing the exact diagonalization method in conjunction with the linear spin wave theory, we have demonstrated that the magnetic excitation gap in the polarized phase is determined by the magnon excitation at $M$ points and has a strong anisotropy with respect to the field direction in the vicinity of the critical field limit. The specific heat from this magnon excitation bears qualitatively the same anisotropic behaviors as expected one for the non-Abelian…
Raman scattering has been employed to investigate lattice and magnetic excitations of the honeycomb Kitaev material $α$-RuCl$_3$ and its Heisenberg counterpart CrCl$_3$. Our phonon Raman spectra give evidence for a first-order structural transition from a monoclinic to a rhombohedral structure for both compounds. Significantly, only $α$-RuCl$_3$ features a large thermal hysteresis, consistent with the formation of a wide phase of coexistence. In the related temperature interval of $70-170$ K, we observe a hysteretic behavior of magnetic excitations as well. The stronger magnetic response in th…
$α$-RuCl$_3$ is drawing much attention as a promising candidate Kitaev quantum spin liquid. However, despite intensive research efforts, controversy remains about the form of the basic interactions governing the physics of this material. Even the sign of the Kitaev interaction (the bond-dependent anisotropic interaction responsible for Kitaev physics) is still under debate, with conflicting results from theoretical and experimental studies. The significance of the symmetric off-diagonal exchange interaction (referred to as the $Γ$ term) is another contentious question. Here, we present resonan…
We have investigated the longitudinal thermal conductivity of $α$-RuCl$_{3}$, the magnetic state of which is considered to be proximate to a Kitaev honeycomb model, along with the spin susceptibility and magnetic specific heat. We found that the temperature dependence of the thermal conductivity exhibits an additional peak around 100 K, which is well above the phonon peak temperature ($\sim$ 50 K). The higher-temperature peak position is comparable to the temperature scale of the Kitaev couplings rather than the Néel temperatures below 15 K. The additional heat conduction was observed for all …
Recently there has been a great interest in understanding quantum spin liquid phases with varying spin magnitude, partly due to possible material realizations. A number of recent numerical computations suggest that the ground state of the S=1 Kitaev model may be a quantum spin liquid in analogy to the renowned $S$=$1/2$ model. On the other hand, the nature of the ground state remains elusive since the $S$=$1$ model is not exactly solvable in contrast to the $S$=$1/2$ model. In this work, we construct a tensor network ground state wavefunction for the S=1 Kitaev model, which is explicitly writt…
There has been a great interest in magnetic field induced quantum spin liquids in Kitaev magnets after the discovery of neutron scattering continuum and half quantized thermal Hall conductivity in the material $α$-RuCl$_3$. In this work, we provide a semiclassical analysis of the relevant theoretical models on large system sizes, and compare the results to previous studies on quantum models with small system sizes. We find a series of competing magnetic orders with fairly large unit cells at intermediate magnetic fields, which are most likely missed by previous approaches. We show that quantum…
The recently-synthesized iridate $β$-Li$_2$IrO$_3$ has been proposed as a candidate to display novel magnetic behavior stabilized by frustration effects from bond-dependent, anisotropic interactions (Kitaev model) on a three-dimensional "hyperhoneycomb" lattice. Here we report a combined study using neutron powder diffraction and magnetic resonant x-ray diffraction to solve the complete magnetic structure. We find a complex, incommensurate magnetic order with non-coplanar and counter-rotating Ir moments, which surprisingly shares many of its features with the related structural polytype "strip…
The combination of strong spin-orbit coupling and correlations, e.g. in ruthenates and iridates, has been proposed as a means to realize quantum materials with nontrivial topological properties. We discuss here Mott insulators where onsite spin-orbit coupling favors a local $J_{\textrm{tot}}=0$ singlet ground state. We investigate excitations into a low-lying triplet, triplons, and find them to acquire nontrivial band topology in a magnetic field. We also comment on magnetic states resulting from triplon condensation, where we find, in addition to the same ordered phases known from the $J_{\te…
We present a theoretical study of the response of $β$-$\text{Li}_2\text{IrO}_3$ under external magnetic fields in the $ab$, $bc$ and $ac$ crystallographic planes. The results are based on the minimal nearest-neighbor $J$-$K$-$Γ$ model and reveal a rich intertwining of field-induced phases and magnetic phase transitions with distinctive signatures that can be probed directly via torque magnetometry. Most saliently, we observe: i) an unusual reentrance of the incommensurate counter-rotating order for fields in the $ab$-plane, and ii) a set of abrupt torque discontinuities which are particularly …
Layered honeycomb magnets are of interest as potential realizations of the Kitaev quantum spin liquid (KQSL), a quantum state with long-range spin entanglement and an exactly solvable Hamiltonian. Conventional magnetically ordered states are present for all currently known candidate materials, however, because non-Kitaev terms in the Hamiltonians obscure the Kitaev physics. Current experimental studies of the KQSL are focused on 4d- or 5d-transition-metal-based honeycombs, in which strong spin-orbit coupling can be expected, yielding Kitaev interaction that dominate in an applied magnetic fiel…
Ground State Properties of the Doped Kitaev-Heisenberg Chain: Topological Superconducting and Mott Insulating Phases Driven by Magnetic Frustration
University of Warsaw（华沙大学）；TU Wien（维也纳工业大学）；Technical University Dresden（德累斯顿工业大学）；Institute for Theoretical Solid State Physics, IFW Dresden（德累斯顿联邦材料研究所理论固态物理研究所）
Very recently a quantum liquid was reported to form in H$_3$LiIr$_2$O$_6$, an iridate proposed to be a close realization of the Kitaev honeycomb model. To test this assertion we perform detailed quantum chemistry calculations to determine the magnetic interactions between Ir moments. We find that weakly bond dependent ferromagnetic Kitaev exchange dominates over other couplings, but still is substantially lower than in Na$_2$IrO$_3$. This reduction is caused by the peculiar position of the inter-layer species: removing hydrogen cations next to a Ir$_2$O$_2$ plaquette increases the Kitaev excha…
The quest for Kitaev spin liquids in particular three dimensional solids is long sought goal in condensed matter physics, as these states may give rise to exotic new types of quasi-particle excitations carrying fractional quantum numbers namely Majorana Fermionic excitations. Here we report the experimental signature of this characteristic feature of the Kitaev spin liquid via Raman measurements. Sm2ZnIrO6 is a strongly spin orbit coupled Mott insulator, where Jeff = 1/2 controls the physics, which provide striking evidence for this characteristic feature of the Kitaev spin liquid. As the temp…
The theoretical inception of the Kitaev honeycomb model has had defining influence on the experimental hunt for quantum spin liquids, bringing unprecedented focus onto the synthesis of materials with bond-directional interactions. Numerous Kitaev materials, which are believed to harbor ground states parametrically close to the Kitaev spin liquid, have been investigated since. Yet, in these materials the Kitaev interaction often comes hand in hand with off-diagonal $Γ$ interactions -- with the competition of the two potentially giving rise to a magnetically ordered ground state. In an attempt t…
Mott insulators under sufficiently strong spin-orbit coupling can display quantum spin liquid phases with topological order and fractional excitations. Quantum magnets with pure Kitaev spin exchange interactions can host a gapped quantum spin liquid with a single Majorana edge mode propagating in the counter-clockwise direction when a small positive magnetic field is applied. Here, we show how under a sufficiently strong positive magnetic field a topological transition into a gapped quantum spin liquid with two Majorana edge modes propagating in the clockwise direction occurs. The Dzyaloshinsk…
Motivated by recent reports of a field-induced intermediate phase (IP) in the antiferromagnetic honeycomb Kitaev model that may be a spin liquid whose nature is distinct from the Kitaev Z2 phase, we present a detailed numerical study on the nature and dynamical response (such as dynamical spin-structure factors and resonant inelastic x-ray scattering intensities) of this field-induced IP and neighboring phases in a family of Kitaev-based models related by hidden symmetries and duality transformations. We further show that the same field-induced IP can appear in models relevant for $α$-RuCl${_3…
The Kitaev model is an exactly solvable quantum spin model within the language of the constrained real fermions. In spite of numerous studies along special magnetic-field orientations, there is a limited amount of knowledge on the complete field-angle characterization, which can provide valuable information on the existence of fractionalized excitations. For this purpose, we first extend previous studies on the field-angle response of the ferromagnetic Kitaev model to its antiferromagnetic version. Yet, the realistic description of the candidate Kitaev materials, within the edge-sharing octahe…
Quantum spin liquid is a disordered magnetic state with fractional spin excitations. Its clearest example is found in an exactly solved Kitaev honeycomb model where a spin flip fractionalizes into two types of anyons, quasiparticles that are neither fermions nor bosons: a pair of gauge fluxes and a Majorana fermion. Here we demonstrate this kind of fractionalization in the Kitaev paramagnetic state of the honeycomb magnet $α$-RuCl$_3$. The spin-excitation gap measured by nuclear magnetic resonance consists of the predicted Majorana fermion contribution following the cube of the applied magneti…
Magnetic properties of the substitution series Ru$_{1-x}$Cr$_x$Cl$_3$ were investigated to determine the evolution from the anisotropic Kitaev magnet $α$-RuCl$_3$ with $J_{\rm eff} = 1/2$ magnetic Ru$^{3+}$ ions to the isotropic Heisenberg magnet CrCl$_3$ with $S = 3/2$ magnetic Cr$^{3+}$ ions. Magnetization measurements on single crystals revealed a reversal of the magnetic anisotropy under doping, which we argue to arise from the competition between anisotropic Kitaev and off-diagonal interactions on the Ru-Ru links and approximately isotropic Cr-Ru and isotropic Cr-Cr interactions. In addit…
We provide a framework for understanding the gapless Kitaev spin liquid (KSL) in the language of tensor network(TN). Without introducing Majorana fermion, most of the features of the KSL including the symmetries, gauge structure, criticality and vortex-freeness are explained in a compact TN representation. Our construction reveals a hidden string gas structure of the KSL. With only two variational parameters to adjust, we obtain an accurate KSL ansatz with the bond dimension D = 8 in a compact form, where the energy is about 0.007% higher than the exact one. In addition, the opening of gap and…
Motivated by the magnetic phase transition of a proximate Kitaev system $α$-RuCl$_3$ in the presence of a magnetic field, we study the simplest but essential quantum spin model with the ferromagnetic nearest neighboring (NN) Kitaev interaction and additional antiferromagnetic third NN Heisenberg interaction. Employing both exact diagonalization and density matrix renormalization group methods, we demonstrate that the model shows the magnetic phase transition from the zigzag order phase to the spin polarized phase through an intermediate phase in both cases when an in-plane magnetic field is ap…
We investigate the non-Abelian topological chiral spin liquid phase in the two-dimensional (2D) Kitaev honeycomb model subject to a magnetic field. By combining density matrix renormalization group (DMRG) and exact diagonalization (ED) we study the energy spectra, entanglement, topological degeneracy, and expectation values of Wilson loop operators, allowing for robust characterization. While the ferromagnetic (FM) Kitaev spin liquid is already destroyed by a weak magnetic field with Zeeman energy $H_*^\text{FM} \approx 0.02$, the antiferromagnetic (AFM) spin liquid remains robust up to a magn…
The realization of Kitaev spin liquid, where spins on a honeycomb lattice are coupled ferromagnetically by bond-dependent anisotropic interactions, has been a sought-after dream. 5d iridium oxides $α$-Li2IrO3 and $α$-Na2IrO3 with a honeycomb lattice of Jeff = 1/2 moments recently emerged as a possible materialization. Strong signature of Kitaev physics, however, was not captured. Here we report the discovery of a complex iridium oxide $β$-Li2IrO3 with Jeff = 1/2 moments on "hyper-honeycomb" lattice, a three-dimensional analogue of honeycomb lattice. A positive Curie-Weiss temperature $θ_{CW}$ …
