We argue that several empirical constraints strongly restrict parameters of the effective microscopic spin model describing $α$-RuCl$_3$. In particular, such constraints dictate a substantial \emph{positive} off-diagonal anisotropic coupling, $Γ^\prime\!>\!0$, not anticipated previously. The renormalization by quantum fluctuations allows to reconcile larger values of the advocated bare parameters with their earlier assessments and provides a consistent description of the field evolution of spin excitations in the paramagnetic phase. We assert that large anisotropic terms inevitably result in strong anharmonic coupling of magnons, necessarily leading to broad features in their spectra due to decays, in accord with the observations in $α$-RuCl$_3$. Using duality transformations, we explain the origin of the pseudo-Goldstone mode that is ubiquitous to the studied parameter space and is present in $α$-RuCl$_3$. Our analysis offers a description of $α$-RuCl$_3$ as an easy-plane ferromagnet with antiferromagnetic further-neighbor and strong off-diagonal couplings, which is in a fluctuating zigzag ground state proximate to an incommensurate phase that is continuously connected to a ferromagnetic one.
Motivated by the recent experimental observation of the half-quantized thermal Hall conductivity for the candidate material of the Kitaev spin liquid, $α$-RuCl$_3$[ Y. Kasahara et al., Nature 559, 227 (2018)], we investigate effects of non-Kitaev exchange interactions, which exist in the real material, on the gapped chiral spin liquid state realized in the case with an applied magnetic field. It is found that off-diagonal exchange interactions enhance significantly the mass gap of Majorana fermions. This result provides a possible explanation for robust quantization of the thermal Hall conduct…
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…
We study the field-induced magnetization processes of extended Heisenberg-Kitaev models on the honeycomb lattice, taking into account off-diagonal and longer-range exchange interactions, using a combination of Monte-Carlo simulations, classical energy minimization, and spin-wave theory. We consider a number of different parameter sets, previously proposed to describe the magnetic behavior of $α$-RuCl$_3$ and Na$_2$IrO$_3$ with their antiferromagnetic zigzag ground states. By classifying these parameter sets, we reveal the existence of three distinct mechanisms to stabilize zigzag states, which…
We study the extended Kitaev model called the K$Γ$ model, using a perturbative expansion combined with a well-controlled mean-field approximation and a cutting-edge exact diagonalization. In the phase diagram, we discover a nematic Kitaev spin liquid and a Kekulé Kitaev spin liquid. The former potentially explains the high-field nematic state with zero Chern number experimentally observed in $α$-RuCl$_3$, even for sufficiently small values of $Γ/|K|$. The latter has a Majorana zero mode in its $Z_3$ vortex core, which can be potentially controlled by the domain wall motion. This opens a possib…
Using quantum chemistry calculations we shed fresh light on the electronic structure and magnetic properties of RuCl3, a proposed realization of the honeycomb Kitaev spin model. It is found that the nearest-neighbor Kitaev exchange K is weaker than in 5d5 Ir oxides but still larger than other effective spin couplings. The electronic-structure computations also indicate a ferromagnetic K in the halide, which is supported by a detailed analysis of the field-dependent magnetization. From exact-diagonalization calculations for extended Kitaev-Heisenberg Hamiltonians we additionally find that a tra…
We present first-principles results on the magnetoelastic coupling in $α$-RuCl$_3$ and uncover a striking dependence of the magnetic coupling constants on strain effects. Different magnetic interactions are found to respond very unequally to variations in the lattice, with the Kitaev interaction being the most sensitive. Exact diagonalization results on our magnetoelastic model reproduce recent measurements of the structural Grüneisen parameter and explain the origin of the negative magnetostriction of $α$-RuCl$_3$, disentangling contributions related to different anisotropic interactions and …
We study the spin-wave excitations in $α$-RuCl$_3$ by the spin-wave theory. Starting from the five-orbital Hubbard model and the perturbation theory, we derive an effective isospin-$1/2$ model in the large Hubbard ($U$) limit. Based on the energy-band structure calculated from the first-principle method, we find that the effective model can be further reduced to the $K$-$Γ$ model containing a ferromagnetic nearest-neighbor (NN) Kitaev interaction ($K$) and a NN off-diagonal exchange interaction ($Γ$). With the spin-wave theory, we find that the $K$-$Γ$ model can give magnetic excitations which…
Kitaev interactions underlying a quantum spin liquid have been long sought, but experimental data from which their strengths can be determined directly is still lacking. Here, by carrying out inelastic neutron scattering measurements on high-quality single crystals of $α$-RuCl$_3$, we observe spin-wave spectra with a gap of $\sim$2 meV around the M point of the two-dimensional Brillouin zone. We derive an effective-spin model in the strong-coupling limit based on energy bands obtained from first-principle calculations, and find that the anisotropic Kitaev interaction $K$ term and the isotropic…
Recent studies have brought $α$-RuCl$_3$ to the forefront of experimental searches for materials realizing Kitaev spin-liquid physics. This material exhibits strongly anisotropic exchange interactions afforded by the spin-orbit coupling of the 4d Ru centers. We investigate the dynamical response at finite temperature and magnetic field for a realistic model of the magnetic interactions in $α$-RuCl$_3$. These regimes are thought to host unconventional paramagnetic states that emerge from the suppression of magnetic order. Using exact diagonalization calculations of the quantum model complemente…
In the search for experimental realizations of bond-anisotropic Kitaev interactions and resulting spin-liquid phases, the layered magnet $α$-RuCl$_3$ is a prime candidate. Its modelling typically involves Heisenberg, Kitaev, and symmetric off-diagonal $Γ$ interactions on the two-dimensional honeycomb lattice. However, recent neutron-scattering experiments point towards a sizeable magnetic interlayer coupling. Here we study three-dimensional exchange models for $α$-RuCl$_3$, for both possible $R\bar{3}$ and $C2/m$ crystal structures. We discuss the symmetry constraints on the interlayer couplin…
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…
The magnetic orders in Na$_2$IrO$_3$ and $α-$RuCl$_3$, honeycomb systems with strong spin-orbit coupling and correlations, have been recently described by models with the dominant Kitaev interactions. In this work we discuss how the orientation of magnetic order parameter is selected in this class of models. We show that while the order-by-disorder mechanism in the models with solely Kitaev anisotropies always select cubic axes as easy axes for magnetic ordering, the additional effect of other small bond-dependent anisotropies, such as, e.g., $Γ$-terms, lead to a deviation of the order paramet…
What is the correct low-energy spin Hamiltonian description of $α$-RuCl$_3$? The material is a promising Kitaev spin liquid candidate, but is also known to order magnetically, the description of which necessitates additional interaction terms. The nature of these interactions, their magnitudes and even signs, remain an open question. In this work we systematically investigate dynamical and thermodynamic magnetic properties of proposed effective Hamiltonians. We calculate zero-temperature inelastic neutron scattering (INS) intensities using exact diagonalization, and magnetic specific heat usin…
We use an exact numerical diagonalization method to calculate the dynamical spin structure factors (DSFs) of three ab-initio models and one ab-initio-guided model for a honeycomb-lattice magnet $α$-RuCl$_3$. We also use thermal pure quantum states to calculate the temperature dependence of the heat capacity, the nearest-neighbor (NN) spin-spin correlation function, and the static spin structure factor. From the results obtained from these four effective models, we find that, even when the magnetic order is stabilized at low temperature, the intensity at the $Γ$ point in the DSFs increases with…
We present an analytical study of the exchange interactions between pseudospin one-half $d^{5}$ ions in honeycomb lattices with edge-shared octahedra. Various exchange channels involving Hubbard U, charge-transfer excitations, and cyclic exchange are considered. Hoppings within $t_{2g}$ orbitals as well as between $t_{2g}$ and $e_g$ orbitals are included. Special attention is paid to the trigonal crystal field $Δ$ effects on the exchange parameters. The obtained exchange Hamiltonian is dominated by ferromagnetic Kitaev interaction K within a wide range of $Δ$. It is found that a parameter regi…
$α$-RuCl$_3$ has been studied extensively because of its proximity to the Kitaev quantum-spin-liquid (QSL) phase and the possibility of approaching it by tuning the competing interactions. Here we present the first polarized inelastic neutron scattering study on $α$-RuCl$_3$ single crystals to explore the scattering continuum around the $Γ$ point at the Brillouin zone center, which was hypothesized to be resulting from the Kitaev QSL state but without concrete evidence. With polarization analyses, we find that while the spin-wave excitations around the M point vanish above the transition tempe…
Single crystal inelastic neutron scattering data contain rich information about the structure and dynamics of a material. Yet the challenge of matching sophisticated theoretical models with large data volumes is compounded by computational complexity and the ill-posed nature of the inverse scattering problem. Here we utilize a novel machine-learning-assisted framework featuring multiple neural network architectures to address this via high-dimensional modeling and numerical methods. A comprehensive data set of diffraction and inelastic neutron scattering measured on the Kitaev material $α-$RuC…
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…
Motivated by recent terahertz (THz) spectroscopy measurements in $α$-RuCl$_3$, we develop a theory for magnetoelectric (ME) effects in Mott insulators of $d^5$ transition metal ions in an octahedral crystal field. For $4d$ and $5d$ compounds, the relatively wide-spread orbitals favor charge fluctuations of localized electrons to neighboring ions and a significant ME effect from electronic mechanisms is expected. From a three-orbital Hubbard model with strong spin-orbit coupling, we derive the mechanisms for the electric polarization originating from virtual hopping of the localized holes carry…
In this study, we reanalyze the magnetic interactions in the Kitaev spin liquid candidate materials Na$_2$IrO$_3$, $α$-RuCl$_3$, and $α$-Li$_2$IrO$_3$ using nonperturbative exact diagonalization methods. These methods are more appropriate given the relatively itinerant nature of the systems suggested in previous works. We treat all interactions up to third neighbours on equal footing. The computed terms reveal significant long range coupling, bond-anisotropy, and/or off-diagonal couplings which we argue naturally explain the observed ordered phases in these systems. Given these observations, t…
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…
Revisiting spin Hamiltonian parameters in a Kitaev material via Bayesian optimization of magnetization curves
Institute for Solid State Physics, University of Tokyo（东京大学固体物理研究所）；Center for Basic Research on Materials, National Institute for Materials Science（国立物质材料研究所基础材料研究中心）；Graduate School of Frontier Sciences, The University of Tokyo（东京大学前沿科学研究生院）；Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science（国立物质材料研究所材料纳米结构研究中心）
We calculate magnon dispersions and damping in the Kitaev-Heisenberg model with an off-diagonal exchange $Γ$ and isotropic third-nearest-neighbor interaction $J_3$ on a honeycomb lattice. This model is relevant to a description of the magnetic properties of iridium oxides $α$-Li$_2$IrO$_3$ and Na$_2$IrO$_3$, and Ru-based materials such as $α$-RuCl$_3$. We use an unconventional parametrization of the spin-wave expansion, in which each Holstein-Primakoff boson is represented by two conjugate hermitian operators. This approach gives us an advantage over the conventional one in identifying paramet…
