Mott insulators with strong spin-orbit coupling display a strongly anisotropic response to applied magnetic fields. This applies in particular to Kitaev materials, with $α$-RuCl$_3$ and Na$_2$IrO$_3$ representing two important examples. Both show a magnetically ordered zigzag state at low temperatures, and considerable effort has been devoted to properly modeling these systems in order to identify routes towards realizing a quantum spin liquid. Here, we investigate the relevant Heisenberg-Kitaev-$Γ$ model primarily at elevated temperatures, focusing on the characteristic anisotropy between the in-plane and out-of-plane uniform susceptibility. For $α$-RuCl$_3$, we find that the experimentally observed anisotropy, including its temperature dependence, can be reproduced by combining a large off-diagonal $Γ_1$ coupling with a moderate $g$-factor anisotropy. Moreover, we study in detail the effect of magnetic dilution and provide predictions for the doping evolution of the temperature-dependent susceptibilities.
We study the reduced fidelity and reduced fidelity susceptibility in the Kitaev honeycomb model. It is shown that the reduced fidelity susceptibility of two nearest site manifest itself a peak at the quantum phase transition point, although the one-site reduced fidelity susceptibility vanishes. Our results directly reveal that the reduced fidelity susceptibility can be used to characterize the quantum phase transition in the Kitaev honeycomb model, and thus suggest that the reduced fidelity susceptibility is an accurate marker of the topological phase transition when it is properly chosen, des…
We study exactly both the ground-state fidelity susceptibility and bond-bond correlation function in the Kitaev honeycomb model. Our results show that the fidelity susceptibility can be used to identify the topological phase transition from a gapped A phase with Abelian anyon excitations to a gapless B phase with non-Abelian anyon excitations. We also find that the bond-bond correlation function decays exponentially in the gapped phase, but algebraically in the gapless phase. For the former case, the correlation length is found to be $1/ξ=2\sinh^{-1}[\sqrt{2J_z -1}/(1-J_z)]$, which diverges ar…
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…
$α$-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 investigate the impact of two types of disorder, bond randomness and site dilution, on the spin dynamics in the Kitaev model on a honeycomb lattice. The ground state of this model is a canonical quantum spin liquid with spin fractionalization into two types of quasiparticles, itinerant Majorana fermions and localized fluxes. Using unbiased quantum Monte Carlo simulations, we calculate the temperature evolution of the dynamical spin structure factor, the magnetic susceptibility, and the NMR relaxation rate. In the dynamical spin structure factor, we find that the two types of disorder affect…
We study the ordered moment direction in the extended Kitaev-Heisenberg model relevant to honeycomb lattice magnets with strong spin-orbit coupling. We utilize numerical diagonalization and analyze the exact cluster groundstates using a particular set of spin coherent states, obtaining thereby quantum corrections to the magnetic anisotropy beyond conventional perturbative methods. It is found that the quantum fluctuations strongly modify the moment direction obtained at a classical level, and are thus crucial for a precise quantification of the interactions. The results show that the moment di…
The honeycomb $K-Γ$ model is known to have both deconfined spin liquid and confined phases. We study here a confinement transition between the Kitaev spin liquid and a dimerized phase in the limit of strong bond anisotropy. By partially projecting out Majorana states we are able to map the model onto a model of weakly coupled Ising chains in a transverse field. Within this mapping the ordered Ising phase corresponds to the condensation of $Z_2$ fluxes, or confinement. Our results may improve our understanding of the extensively studied spin liquid candidate material $α$-RuCl$_3$, where $K-Γ$ i…
We develop high temperature series expansions for the thermodynamic properties of the honeycomb-lattice Kitaev-Heisenberg model. Numerical results for uniform susceptibility, heat capacity and entropy as a function of temperature for different values of the Kitaev coupling $K$ and Heisenberg exachange coupling $J$ (with $|J|\le |K|$) are presented. These expansions show good convergence down to a temperature of a fraction of $K$ and in some cases down to $T=K/10$. In the Kitaev exchange dominated regime, the inverse susceptibility has a nearly linear temperature dependence over a wide temperat…
Magnetic anisotropy is crucially important for the stabilization of two-dimensional (2D) magnetism, which is rare in nature but highly desirable in spintronics and for advancing fundamental knowledge. Recent works on CrI$_3$ and CrGeTe$_3$ monolayers not only led to observations of the long-time-sought 2D ferromagnetism, but also revealed distinct magnetic anisotropy in the two systems, namely Ising behavior for CrI$_3$ versus Heisenberg behavior for CrGeTe$_3$. Such magnetic difference strongly contrasts with structural and electronic similarities of these two materials, and understanding it …
Searching for an ideal Kitaev spin liquid candidate with anyonic excitations and long-range entanglement has motivated the synthesis of a new family of intercalated Kitaev magnets such as H$_{3}$LiIr$_{2}$O$_{6}$, Cu$_{2}$IrO$_{3}$, and Ag$_{3}$LiIr$_{2}$O$_{6}$. The absence of a susceptibility peak and a two-step release of the magnetic entropy in these materials has been proposed as evidence of proximity to the Kitaev spin liquid. Here we present a comparative study of the magnetic susceptibility, heat capacity, and muon spin relaxation ($μ$SR) between two samples of Ag$_{3}$LiIr$_{2}$O$_{6}…
The magnetic field response of the Mott-insulating honeycomb iridate Na$_{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…
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 study a quantum spin Kitaev model with zigzag edges to clarify the effects of anisotropy in the exchange couplings on the spin propagation. We simulate the spin and Majorana dynamics triggered by a magnetic pulse, using the real-space time-dependent Majorana mean-field theory. When the anisotropy is small, the dispersion of the itinerant Majorana fermions remains gapless, where the velocity of the spin propagation matches the group velocity of the itinerant Majorana fermions at the nodal points. On the other hand, in the gapped system with a large anisotropy, the spin propagation is strongl…
The layered honeycomb lattice iridate Cu$_2$IrO$_3$ is the closest realization of the Kitaev quantum spin liquid, primarily due to the enhanced interlayer separation and nearly ideal honeycomb lattice. We report pressure-induced structural evolution of Cu$_2$IrO$_3$ by powder x-ray diffraction (PXRD) up to $\sim$17 GPa and Raman scattering measurements up to $\sim$25 GPa. A structural phase transition (monoclinic $C2/c \: \rightarrow$ triclinic $P\bar{1}$) is observed with a broad mixed phase pressure range ($\sim$4 to 15 GPa). The triclinic phase consists of heavily distorted honeycomb lattic…
The Kitaev material $α$-RuCl$_3$ is among the most prominent candidates to host a quantum spin-liquid state endowed with fractionalized excitations. Recent experimental and theoretical investigations have separately revealed the importance of both the magnetoelastic coupling and the magnetic anisotropy, in dependence of the applied magnetic field direction. In this combined theoretical and experimental research, we investigate the anisotropic magnetic and magnetoelastic properties for magnetic fields applied along the main crystallographic axes as well as for fields canted out of the honeycomb…
In the Kitaev honeycomb model, the quantum spin fractionalizes into itinerant Majorana and gauge flux spontaneously upon cooling, leading to rich experimental ramifications at finite temperature and an upsurge of research interest. In this work, we employ the exponential tensor renormalization group approach to explore the Kitaev model under various perturbations, including the external fields, Heisenberg, and the off-diagonal couplings that are common in the Kitaev materials. Through large-scale manybody calculations, we find a Kitaev fractional liquid at intermediate temperature that is robu…
The leading order nonlinear (NL) susceptibility, $χ_3$, in a paramagnet is negative and diverges as $T \rightarrow 0$. This divergence is destroyed when spins correlate and the NL response provides unique insights into magnetic order. Dimensionality, exchange interaction, and preponderance of quantum effects all imprint their signatures in the NL magnetic response. Here, we study the NL susceptibilities in the proximate Kitaev magnet $α$-RuCl$_3$ which differs from the expected antiferromagnetic behavior. For $T< T_c$ = 7.5 K and field $B$ in the ab-plane, we obtain contrasting NL responses in…
Crossover and Changeover in Spin-1 Kitaev-$Γ$ Chain with Uniaxial Single-ion Anisotropy
Nanjing University of Aeronautics and Astronautics（南京航空航天大学）；Beijing Computational Science Research Center（北京计算科学研究中心）；Nankai University（南开大学）；Beijing University of Posts and Telecommunications（北京邮电大学）；Lanzhou University（兰州大学）；Zhejiang University（浙江大学）
We study the spin-one Kitaev model on the honeycomb lattice in the presence of single-ion anisotropies. We consider two types of single ion anisotropies: A $D_{111}$ anisotropy which preserves the symmetry between $X$, $Y$, and $Z$ bonds but violates flux conservation and a $D_{100}$ anisotropy that breaks the symmetry between $X$, $Y$, and $Z$ bonds but preserves flux conservation. We use series expansion methods, degenerate perturbation theory, and exact diagonalization to study these systems. Large positive $D_{111}$ anisotropy leads to a simple product ground state with conventional magnon…
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…
We lay the foundation for determining the microscopic spin interactions in two-dimensional (2D) ferromagnets by combining angle-dependent ferromagnetic resonance (FMR) experiments on high quality CrI$_3$ single crystals with theoretical modeling based on symmetries. We discover that the Kitaev interaction is the strongest in this material with $K \sim -5.2$ meV, 25 times larger than the Heisenberg exchange $J \sim -0.2$ meV, and responsible for opening the $\sim$5 meV gap at the Dirac points in the spin-wave dispersion. Furthermore, we find that the symmetric off-diagonal anisotropy $Γ\sim -67…
We discuss the finite-temperature phase diagram of the Heisenberg-Kitaev model on the hexagonal lattice, which has been suggested to describe the spin-orbital exchange of the effective spin-1/2 momenta in the Mott insulating Iridate Na2IrO3. At zero-temperature this model exhibits magnetically ordered states well beyond the isotropic Heisenberg limit as well as an extended gapless spin liquid phase around the highly anisotropic Kitaev limit. Using a pseudofermion functional renormalization group (RG) approach, we extract both the Curie-Weiss scale and the critical ordering scale (for the magne…
Dynamical magnetotropic susceptibility as a new probe of Kitaev materials and beyond
Institut für Theoretische Physik und Astrophysik, Universität Würzburg（维尔茨堡大学理论与天体物理研究所）；TU Dresden（德累斯顿工业大学）；Institute of Science and Technology Austria（奥地利科学技术研究院）；Max-Planck-Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Institute of Solid State Physics, TU Wien（维也纳工业大学固体物理研究所）；Würzburg-Dresden Cluster of Excellence ctd.qmat（维尔茨堡-德累斯顿卓越集群ctd.qmat）；Institute for Theoretical Solid State Physics, IFW Dresden（德累斯顿IFW理论固体物理研究所）
We study the effect of site dilution in Kitaev's model. We derive an analytical solution of the dynamical spin correlation functions for arbitrary configurations of $Z_2$ fluxes. By incorporating this solution into classical Monte Carlo scheme, we address how a site vacancy affects the experimental observables, such as the static spin susceptibility and the spin lattice relaxation rate, $1/T_1$. As a result, we found an enhancement of dynamical magnetic response in the vicinity of vacancy, which leads to Friedel-like oscillation in local $1/T_1$, in contrast to limited influences on the static…
The magnetic insulator $α$-RuCl$_{3}$ is a promising candidate to realize Kitaev interactions on a quasi-2D honeycomb lattice. We perform extensive susceptibility measurements on single crystals of $α$-RuCl$_{3}$, including angle-dependence of the in-plane longitudinal and transverse susceptibilities, which reveal a unidirectional anisotropy within the honeycomb plane. By comparing the experimental results to a high-temperature expansion of a Kitaev-Heisenberg-$Γ$ spin Hamiltonian with bond anisotropy, we find excellent agreement with the observed phase shift and periodicity of the angle-resol…
In the pseudospin-$\frac{1}{2}$ honeycomb Mott insulators with strong spin-orbit coupling, there are two types of bond-dependent exchange interactions, named Kitaev ($K$) and $Γ$, leading to strong frustration. While the ground state of the Kitaev model is a quantum spin liquid with fractionalized excitations, the ground state of the $Γ$ model remains controversial. In particular, the phase diagram of the $KΓ$ model with ferromagnetic $K$ and antiferromagnetic $Γ$ interactions has been intensively studied because of its relevance to candidate materials such as $α$-RuCl$_{3}$. Numerical studies…
Significant efforts have focused on the magnetic excitations of relativistic Mott insulators, predicted to realize the Kitaev quantum spin liquid (QSL). This exactly solvable model involves a highly entangled state resulting from bond-dependent Ising interactions that produce excitations which are non-local in terms of spin flips. A key challenge in real materials is identifying the relative size of the non-Kitaev terms and their role in the emergence or suppression of fractional excitations. Here, we identify the energy and temperature boundaries of non-Kitaev interactions by direct compariso…
We present results on entropy and heat-capacity of the spin-S honeycomb-lattice Kitaev models using high-temperature series expansions and thermal pure quantum (TPQ) state methods. We study models with anisotropic couplings $J_z=1\ge J_x=J_y$ for spin values 1/2, 1, 3/2, and 2. We show that for $S>1/2$, any anisotropy leads to well developed plateaus in the entropy function at an entropy value of $\frac{1}{2}\ln{2}$, independent of $S$. However, in the absence of anisotropy, there is an incipient entropy plateau at $S_{max}/2$, where $S_{max}$ is the infinite temperature entropy of the system.…
A Kitaev-Heisenberg-J2-J3 model is proposed to describe the Mott-insulating layered iridates A2IrO3 (A=Na,Li). The model is a combination of the Kitaev honeycomb model and the Heisenberg model with all three nearest neighbor couplings J1, J2 and J3. A rich phase diagram is obtained at the classical level, including the experimentally suggested zigzag ordered phase; as well as the stripy phase, which extends from the Kitaev-Heisenberg limit to the J1-J2-J3 one. Combining the experimentally observed spin order with the optimal fitting to the uniform magnetic susceptibility data gives an estimate…
We present a methodology for probing the details of electronic susceptibility through minimally-invasive nuclear magnetic resonance techniques. Specifically, we classify electron-mediated long-range interactions in an ensemble of nuclear spins by revealing their effect on simple spin echo experiments. We find that pulse strength and applied field orientation dependence of these spin echo measurements resolves the spatial extent and anisotropy of electronic spin susceptibility. This work provides an alternate explanation to NMR results in superconducting and magnetically-ordered systems. The me…
Recently, the family of rare-earth chalcohalides were proposed as candidate compounds to realize the Kitaev spin liquid (KSL). In the present work, we firstly propose an effective spin Hamiltonian consistents with the symmetry group of the crystal structure. Then we apply classical Monte Carlo simulations to preliminarily study the model and establish a phase diagram. When approaching to the low temperature limit, several magnetic long range orders are observed, including the stripe, the zigzag, the antiferromagnetic (AFM), the ferromagnetic (FM), the incommensurate spiral (IS), the Multi-$\pm…
A general discussion of the simulation procedure of the full susceptibility tensor and isothermal magnetization pseudovector for compounds comprising weakly-interacting magnetic centers is presented. A single-crystal-sample as well as a powder-sample case are considered. The procedure is used to obtain explicit expressions for the full susceptibility tensor for spins S=1, 3/2, 2, and 5/2 for non-vanishing rhombic local anisotropy and any form of spectroscopic tensor.
The energy-level scheme and wave functions of the titanium ions in LaTiO$_{3}$ are calculated using crystal-field theory and spin-orbit coupling. The theoretically derived temperature dependence and anisotropy of the magnetic susceptibility agree well with experimental data obtained in an untwinned single crystal. The refined fitting procedure reveals an almost isotropic molecular field and a temperature dependence of the van Vleck susceptibility. The charge distribution of the 3d--electron on the Ti positions and the principle values of the quadrupole moments are derived and agree with NMR da…
By using the extraordinary Hall effect in SrRuO3 films we performed sensitive measurements of the paramagnetic susceptibility in this itinerant ferromagnet, from Tc (~ 150 K) to 300 K. These measurements, combined with measurements of magnetoresistance, reveal that the susceptibility, which is almost isotropic at 300 K, becomes highly anisotropic as the temperature is lowered, diverging along a single crystallographic direction in the vicinity of Tc. The results provide a striking manifestation of the effect of exceptionally large magnetocrystalline anisotropy in the paramagnetic state of a 4d…
The spin-1/2 Heisenberg kagome antiferromagnet is one of the paradigmatic playgrounds for frustrated quantum magnetism, with an extensive number of competing resonating valence bond (RVB) states emerging at low energies, including gapped and gapless spin liquids and valence bond crystals. Here we revisit the crossover from this quantum RVB phase to a semiclassical regime brought about by anisotropic Kitaev interactions, and focus on the precise mechanisms underpinning this crossover. To this end, we introduce a simple parametrization of the classical ground states (GSs) in terms of emergent Is…
Kitaev magnets are materials with bond-dependent Ising interactions between localized spins on a honeycomb lattice. Such interactions could lead to a quantum spin-liquid (QSL) ground state at zero temperature. Recent theoretical studies suggest two potential signatures of a QSL at finite temperatures, namely a scaling behavior of thermodynamic quantities in the presence of quenched disorder, and a two-step release of the magnetic entropy. Here, we present both signatures in Ag$_{3}$LiIr$_{2}$O$_{6}$ which is synthesized from $α$-Li$_{2}$IrO$_{3}$ by replacing the inter-layer Li atoms with Ag a…
We study the ground state properties of the Kitaev-Heisenberg model in a magnetic field and explore the evolution of spin correlations in the presence of non-magnetic vacancies. By means of exact diagonalizations, the phase diagram without vacancies is determined as a function of the magnetic field and the ratio between Kitaev and Heisenberg interactions. We show that in the (antiferromagnetic) stripe ordered phase the static susceptibility and its anisotropy can be described by a spin canting mechanism. This accounts as well for the transition to the polarized phase when including quantum flu…
The Kitaev spin liquid, a ground state of the bond-dependent Kitaev model in a honeycomb lattice has been a centre of attraction, since a microscopic theory to realize such an interaction in solid-state materials was discovered. A challenge in real materials though is the presence of the Heisenberg and another bond-dependent Gamma interactions detrimental to the Kitaev spin liquid, and there have been many debates on their relative strengths. Here we offer a strategy to extract the Kitaev interaction out of a full microscopic model by utilizing the symmetries of the Hamiltonian. Two tilted mag…
Kitaev quantum spin liquid, massively quantum entangled states, is so scarce in nature that searching for new candidate systems remains a great challenge. Honeycomb heterostructure could be a promising route to realize and utilize such an exotic quantum phase by providing additional controllability of Hamiltonian and device compatibility, respectively. Here, we provide epitaxial honeycomb oxide thin film Na3Co2SbO6, a candidate of Kitaev quantum spin liquid proposed recently. We found a spin glass and antiferromagnetic ground states depending on Na stoichiometry, signifying not only the import…
We present a study of the magnetic susceptibility in carefully detwinned La_{2-x}Sr_{x}CuO_4 single crystals in the lightly-doped region (x=0-0.03), which demonstrates a remarkable in-plane anisotropy of the spin system. This anisotropy is found to persist after the long-range antiferromagnetic (AF) order is destroyed by hole doping, suggesting that doped holes break the AF order into domains in which the spin alignment is kept essentially intact. It turns out that the freezing of the spins taking place at low temperatures is also notably anisotropic, implying that the "spin-glass" feature is …
We study the fidelity susceptibility in an antiferromagnetic spin-1 XXZ chain numerically. By using the density-matrix renormalization group method, the effects of the alternating single-site anisotropy $D$ on fidelity susceptibility are investigated. Its relation with the quantum phase transition is analyzed. It is found that the quantum phase transition from the Haldane spin liquid to periodic Néel spin solid can be well characterized by the fidelity. Finite size scaling of fidelity susceptibility shows a power-law divergence at criticality, which indicates the quantum phase transition is of…
We measure the magnetic susceptibility of ultrathin Co films with an in-plane uniaxial magnetic anisotropy grown on a vicinal Cu substrate. Above the Curie temperature the influence of the magnetic anisotropy can be investigated by means of the parallel and transverse susceptibilities along the easy and hard axes. By comparison with a theoretical analysis of the susceptibilities we determine the isotropic exchange interaction and the magnetic anisotropy. These calculations are performed in the framework of a Heisenberg model by means of a many-body Green's function method, since collective mag…
The microscopic modeling of spin-orbit entangled $j=1/2$ Mott insulators such as the layered hexagonal Iridates Na$_2$IrO$_3$ and Li$_2$IrO$_3$ has spurred an interest in the physics of Heisenberg-Kitaev models. Here we explore the effect of lattice distortions on the formation of the collective spin-orbital states which include not only conventionally ordered phases but also gapped and gapless spin-orbital liquids. In particular, we demonstrate that in the presence of spatial anisotropies of the exchange couplings conventionally ordered states are formed through an order-by-disorder selection…
Recent experimental evidence for a field-induced quantum spin liquid (QSL) in $α$-RuCl$_3$ calls for an understanding for the ground state of honeycomb Kitaev model under a magnetic field. In this work we address the nature of an enigmatic gapless paramagnetic phase in the antiferromagnetic Kitave model, under an intermediate magnetic field perpendicular to the plane. Combining theoretical and numerical efforts, we identify this gapless phase as a $U(1)$ QSL with spinon Fermi surfaces. We also reveal the nature of continuous quantum phase transitions involving this $U(1)$ QSL, and obtain a pha…
