Kitaev Materials Research Articles

SmI3:4f5 honeycomb magnet with spin-orbital entangled Γ7 Kramers doublet

We report magnetic properties of a 4f-honeycomb iodide SmI3 made up of edge-shared network of SmI6 octahedra. High temperature magnetic susceptibility indicates {\Gamma}7 Kramers doublet ground state of Sm3+ (4f5) ions stabilized by the spin-orbit coupling and octahedral crystal electric field, which interact with Sm-I-Sm bond angle nearly 90 degree. Magnetization measurements down to 0.1 K detected antiferromagnetic correlations and an anomaly in the magnetization curve before saturation without a sign of long-range order. Relevance between SmI3 and the antiferromagnetic Kitaev material proposed in the 4f-electron system is discussed.

Interplay of magnetic field and trigonal distortion in the honeycomb Γ model: Occurrence of a spin-flop phase

In candidate Kitaev materials, the off-diagonal $\Gamma$ and $\Gamma'$ interactions are identified to come from the spin-orbit coupling and trigonal distortion, respectively. They have generated intense research efforts because of their intimate relation to the field-induced magnetically disordered state reported in $\alpha$-RuCl$_3$. Theoretically, while a plethora of field-induced phases has been proposed in the honeycomb lattice, a stable intermediate phase that can survive in a wide parameter region regardless of the underlying phases is still lacking. Here we focus on the interplay of an out-of-plane magnetic field and a symmetry-allowed $\Gamma'$ term due to trigonal distortion in the dominant antiferromagnetic $\Gamma$ region. By using multifaceted approaches ranging from classical Monte Carlo and semiclassical spin-wave theory to density-matrix renormalization group, we identify an intriguing spin-flop phase in the presence of magnetic field and antiferromagnetic $\Gamma'$ interaction, before it eventually enters into a fully polarized state. As the $\Gamma'$ interaction approaches the size of $\Gamma$ one, the $\Gamma$-$\Gamma'$ model maps to the easy-axis XXZ antiferromagnet, where the spin-flop phase can be understood as a superfluid phase in the extended Bose-Hubbard model. Our finding thus demonstrates an exciting path from the honeycomb $\Gamma$ model towards a $U(1)$-symmetric XXZ antiferromagnet in a magnetic field.

Strategy to extract Kitaev interaction using symmetry in honeycomb Mott insulators

The Kitaev spin liquid, a ground state of the bond-dependent Kitaev model in a honeycomb lattice has been a center 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 magnetic field directions related by a two-fold rotational symmetry generate distinct spin excitations originated from a specific combination of the Kitaev and Gamma interactions. Together with the in- and out-of-plane magnetic anisotropy, one can determine the Kitaev and Gamma interactions separately. Dynamic spin structure factors are presented to motivate future experiments. The proposed setups will advance the search for Kitaev materials.

Dissipationless spin current generation in a Kitaev chiral spin liquid

$\alpha$-RuCl$_3$ is a promising candidate material for the Kitaev spin liquid state where the half quantization of the thermal Hall effect, suggesting a topological character, has been observed. However, its relation to the existence of chiral Majorana fermions, which is predicted from the theory of the Kitaev model, is still under debate. Here we propose a more direct signature of a chiral Majorana edge mode which emerges in a universal scaling of the Drude weight of the edge spin Seebeck effect in the Kitaev model. Moreover, the absence of backscatterings in the chiral edge mode results in the generation of a dissipationless spin current in spite of an extremely short spin correlation length close to a lattice constant in the bulk. This result is not only experimentally observable, but also opens a way towards spintronics application of Kitaev materials. In contrast to magnetically ordered systems, a Kitaev spin liquid state is stable even in the atomic scale and makes it possible to fabricate a highly integrated device with substantial efficiency to generate a spin current. This proposal for using $\alpha$-RuCl$_3$ as a nano-scale device will pioneer Kitaev spintronics.

Comparing the influence of Floquet dynamics in various Kitaev-Heisenberg materials

In this paper we examine the possibility of Floquet engineering in the three candidate Kitaev materials ${\mathrm{Na}}_{2}{\mathrm{IrO}}_{3}$, $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$, and $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$. We derive an effective Floquet Hamiltonian and give an approximation for heating processes arising from doublon holon propagation. This suggests that compounds with stronger Hund's rule coupling are less prone to heating. We then investigate the impact of light frequency and amplitude on magnetic interaction terms up to third nearest neighbor and find that third neighbor Heisenberg coupling ${J}_{3}$ is very susceptible to tuning by circularly polarized light. Finally, we discuss uses of linear polarized light in selectively tuning single bond directions.

Pressure-induced dimerization and collapse of antiferromagnetism in the Kitaev material α−Li2IrO3

We present magnetization measurements carried out on polycrystalline and single-crystalline samples of $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ under hydrostatic pressures up to 2 GPa and establish the temperature-pressure phase diagram of this material. The N\'eel temperature (${T}_{\mathrm{N}}$) of $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ is slightly enhanced upon compression with $d{T}_{\mathrm{N}}/dp$ = 1.5 K/GPa. Above 1.2 GPa, $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ undergoes a first-order phase transition toward a nonmagnetic dimerized phase, with no traces of the magnetic phase observed above 1.8 GPa at low temperatures. The critical pressure of the structural dimerization is strongly temperature dependent. This temperature dependence is well reproduced on the ab initio level by taking into account lower phonon entropy in the nonmagnetic phase. We further show that the initial increase in ${T}_{\mathrm{N}}$ of the magnetic phase is due to a weakening of the Kitaev interaction $K$ along with the enhancement of the Heisenberg term $J$ and off-diagonal anisotropy $\mathrm{\ensuremath{\Gamma}}$. Our study reveals a common thread in the interplay of magnetism and dimerization in pressured Kitaev materials.

Metastable Kitaev Magnets.

Nearly two decades ago, Alexei Kitaev proposed a model for spin- particles with bond-directional interactions on a two-dimensional honeycomb lattice which had the potential to host a quantum spin-liquid ground state. This work initiated numerous investigations to design and synthesize materials that would physically realize the Kitaev Hamiltonian. The first generation of such materials, such as NaIrO, -LiIrO, and -RuCl, revealed the presence of non-Kitaev interactions such as the Heisenberg and off-diagonal exchange. Both physical pressure and chemical doping were used to tune the relative strength of the Kitaev and competing interactions; however, little progress was made towards achieving a purely Kitaev system. Here, we review the recent breakthrough in modifying Kitaev magnets via topochemical methods that has led to the second generation of Kitaev materials. We show how structural modifications due to the topotactic exchange reactions can alter the magnetic interactions in favor of a quantum spin-liquid phase.

Gapless excitations in non-Abelian Kitaev spin liquids with line defects

We show that line defects in a non-Abelian Kitaev spin liquid harbor gapless one-dimensional Majorana modes if the interaction across the defect falls below a critical value. Treating the weak interaction at the line defect within a mean-field approximation, we determine the critical interaction strength as a function of the external magnetic field. In the gapless regime, we use the low-energy effective field theory to calculate the spin-lattice relaxation rate for a nuclear spin near the defect and find a cubic temperature dependence that agrees with experiments in the Kitaev material $\alpha\text{-RuCl}_3$.

Magnetotropic Response in Ruthenium Chloride

We consider the exchange couplings present in an effective Hamiltonian of $\alpha$-RuCl$_3$, known as the K-$\Gamma$ model. This material has a honeycomb lattice, and is expected to be a representative of the Kitaev materials (which can realize the 2d Kitaev model). However, the behaviour of RuCl$_3$ shows that the exchange interactions of the material are not purely Kitaev-like, especially because it has an antiferromagnetic ordering at low temperatures and under low strengths of an externally applied magnetic field. Fitting the data obtained from the measurements of the magnetotropic coefficient (the thermodynamic coefficient associated with magnetic anisotropy), reported in Nature Physics 17, 240-244 (2020), we estimate the values of the exchange couplings of the effective Hamiltonian. The fits indicate that the Kitaev couplings are subdominant to the other exchange couplings.

Interplay of magnetism and dimerization in the pressurized Kitaev material β−Li2IrO3

We present magnetization measurements on polycrystalline $\beta$-Li$_2$IrO$_3$ under hydrostatic pressures up to 3~GPa and construct the temperature-pressure phase diagram of this material. Our data confirm that magnetic order breaks down in a first-order phase transition at $p_{\rm{c}}$ $\approx$ 1.4~GPa and additionally reveal a step-like feature -- magnetic signature of structural dimerization -- that appears at $p_{\rm{c}}$ and shifts to higher temperatures upon further compression. Following the structural study by L. S. I. Veiga et al. [Phys. Rev. B 100, 064104 (2019)], we suggest that a partially dimerized phase with a mixture of magnetic and non-magnetic Ir$^{4+}$ sites develops above $p_{\rm{c}}$. This phase is thermodynamically stable between 1.7 and 2.7~GPa according to our ab initio calculations. It confines the magnetic Ir$^{4+}$ sites to weakly coupled tetramers with a singlet ground state and no long-range magnetic order. Our results rule out the formation of a pressure-induced spin-liquid phase in $\beta$-Li$_2$IrO$_3$ and reveal peculiarities of the magnetism collapse transition in a Kitaev material. We also show that a compressive strain imposed by the pressure treatment of $\beta$-Li$_2$IrO$_3$ enhances signatures of the 100~K magnetic anomaly at ambient pressure.

Nesting instability of gapless U(1) spin liquids with spinon Fermi pockets in two dimensions

Quantum spin liquids are exotic states of matter that may be realized in frustrated quantum magnets and feature fractionalized excitations and emergent gauge fields. Here, we consider a gapless U(1) spin liquid with spinon Fermi pockets in two spatial dimensions. Such a state appears to be the most promising candidate to describe the exotic field-induced behavior observed in numerical simulations of the antiferromagnetic Kitaev honeycomb model. A similar such state may also be responsible for the recently-reported quantum oscillations of the thermal conductivity in the field-induced quantum paramagnetic phase of $\alpha$-RuCl$_3$. We consider the regime close to a Lifshitz transition, at which the spinon Fermi pockets shrink to small circles around high-symmetry points in the Brillouin zone. By employing renormalization group and mean-field arguments, we demonstrate that interactions lead to a gap opening in the spinon spectrum at low temperatures, which can be understood as a nesting instability of the spinon Fermi surface. This leads to proliferation of monopole operators of the emergent U(1) gauge field and confinement of spinons. While signatures of fractionalization may be observable at finite temperatures, the gapless U(1) spin liquid state with nested spinon Fermi pockets is ultimately unstable at low temperatures towards a conventional long-range-ordered ground state, such as a valence bond solid. Implications for Kitaev materials in external magnetic fields are discussed.

Non-Loudon-Fleury Raman scattering in spin-orbit coupled Mott insulators

We revisit the theory of magnetic Raman scattering in Mott insulators with strong spin-orbit coupling, with a major focus on Kitaev materials. We show that Kitaev materials with bond-anisotropic interactions are generally expected to show both one- and two-magnon responses. It is further shown that, in order to obtain the correct leading contributions to the Raman vertex operator $\mc{R}$, one must take into account the precise, photon-assisted microscopic hopping processes of the electrons and that, in systems with multiple hopping paths, $\mc{R}$ contains terms beyond those appearing in the traditional Loudon-Fleury theory. Most saliently, a numerical implementation of the revised formalism to the case of the three-dimensional hyperhoneycomb Kitaev material $\beta$-Li$_2$IrO$_3$ reveals that the non-Loudon-Fleury scattering terms actually dominate the Raman intensity. In addition, they induce a qualitative modification of the polarization dependence, including, e.g., the emergence of a sharp one-magnon peak at low energies which is not expected in the traditional Loudon-Fleury theory. This peak is shown to arise from microscopic photon-assisted tunneling processes that are of similar type with the ones leading to the symmetric off-diagonal interaction $\Gamma$ (known to be present in many Kitaev materials), but take the form of a bond-directional magnetic dipole term in the Raman vertex. These results are expected to apply across all Kitaev materials and mark a drastic change of paradigm for the understanding of Raman scattering in materials with strong spin-orbit coupling and multiple exchange paths.

Quantum Lifshitz transitions generated by order from quantum disorder in strongly correlated Rashba spin-orbit-coupled systems

We study the system of strongly interacting spinor bosons in a square lattice subject to the isotropic Rashba spin-orbit coupling $\ensuremath{\alpha}=\ensuremath{\beta}$. It supports a collinear spin-bond correlated magnetic Y-x phase, a gapped coplanar in-commensurate (IC) XY-y phase, and a noncoplanar commensurate (C) $3\ifmmode\times\else\texttimes\fi{}3$ Skyrmion crystal phase. The state at the Abelian point $\ensuremath{\alpha}=\ensuremath{\beta}=\ensuremath{\pi}/2$ is just a ferromagnetic state in a rotated basis. Slightly away from the point, we identify a spurious $\text{U}(1)$ symmetry, develop a nonperturbative method to calculate not only the gap but also the excitation spectrum due to the order from quantum disorder (OFQD) mechanism. We construct a symmetry-based effective action to investigate the quantum Lifshitz transition from the Y-x state to the IC XY-y state and establish the connection between the phenomenological parameters in the effective action and those evaluated by the microscopic nonperturbative OFQD analysis in the large $S$ limits. Experimental implications on cold atoms and some $4d$ or $5d$ Kitaev materials are discussed.

Machine-learned phase diagrams of generalized Kitaev honeycomb magnets

We use a recently developed interpretable and unsupervised machine-learning method, the tensorial kernel support vector machine (TK-SVM), to investigate the low-temperature classical phase diagram of a generalized Heisenberg-Kitaev-$\Gamma$ ($J$-$K$-$\Gamma$) model on a honeycomb lattice. Aside from reproducing phases reported by previous quantum and classical studies, our machine finds a hitherto missed nested zigzag-stripy order and establishes the robustness of a recently identified modulated $S_3 \times Z_3$ phase, which emerges through the competition between the Kitaev and $\Gamma$ spin liquids, against Heisenberg interactions. The results imply that, in the restricted parameter space spanned by the three primary exchange interactions -- $J$, $K$, and $\Gamma$, the representative Kitaev material $\alpha$-${\rm RuCl}_3$ lies close to the boundaries of several phases, including a simple ferromagnet, the unconventional $S_3 \times Z_3$ and nested zigzag-stripy magnets. A zigzag order is stabilized by a finite $\Gamma^{\prime}$ and/or $J_3$ term, whereas the four magnetic orders may compete in particular if $\Gamma^{\prime}$ is anti-ferromagnetic.

Electric Probe for the Toric Code Phase in Kitaev Materials through the Hyperfine Interaction.

The Kitaev model is a remarkable spin model with gapped and gapless spin liquid phases, which are potentially realized in iridates and α-RuCl_{3}. In the recent experiment of α-RuCl_{3}, the signature of a nematic transition to the gapped toric code phase, which breaks the C_{3} symmetry of the system, has been observed through the angle dependence of the heat capacity. We here propose a mechanism by which the nematic transition can be detected electrically. This is seemingly impossible because J_{eff}=1/2 spins do not have an electric quadrupole moment (EQM). However, in the second-order perturbation, the virtual state with a nonzero EQM appears, which makes the nematic order parameter detectable by nuclear magnetic resonance and Mössbauer spectroscopy. The purely magnetic origin of the EQM is different from conventional electronic nematic phases, allowing the direct detection of the realization of Kitaev's toric error-correction code.

Evidence for the random singlet phase in the honeycomb iridate SrIr2O6

Strong spin-orbital-coupling magnetic systems with the honeycomb structure can provide bond-directional interactions which may result in Kitaev quantum spin liquids and exotic anyonic excitations. However, one of the key ingredients in real materials$-$disorders$-$has been much less studied in Kitaev systems. Here we synthesized a trigonal SrIr$_2$O$_{6-\delta}$ with $\delta \approx 0.25$, which consists of two-dimensional honeycomb Ir planes with edge-sharing IrO$_6$ octahedra. First-principles computation and experimental measurements suggest that the electronic system is gapped, and there should be no magnetic moment as the Ir$^{5+}$ ion has no unpaired electrons. However, significant magnetism has been observed in the material, and it can be attributed to disorders that are most likely from oxygen vacancies. No magnetic order is found down to 0.05 K, and the low-temperature magnetic properties exhibit power-law behaviors in magnetic susceptibility and zero-field specific heat, and a single-parameter scaling of the specific heat under magnetic fields. These results provide strong evidence for the existence of the random singlet phase in SrIr$_2$O$_{6-\delta}$, which offers a different member to the family of spin-orbital entangled iridates and Kitaev materials.

Effective model for rare-earth Kitaev materials and its classical Monte Carlo simulation* *Project supported by the National Key Research and Development Program of China (Grant Nos. 2017YFA0302904 and 2016YFA0300504), the National Natural Science Foundation of China (Grant Nos. U1932215, 11774419, 11574392, and 11974421), the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB33010100), the Fundamental Research

Recently, the family of rare-earth chalcohalides were proposed as candidate compounds to realize the Kitaev spin liquid (KSL) [Chin. Phys. Lett. 38 047502 (2021)]. In the present work, we firstly propose an effective spin Hamiltonian consistent 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- Q , and the 120° ones. We further calculate the thermodynamic properties of the system, such as the temperature dependence of the magnetic susceptibility and the heat capacity. The ordering transition temperatures reflected in the two quantities agree with each other. For most interaction regions, the system is magnetically more susceptible in the ab-plane than in the c-direction. The stripe phase is special, where the susceptibility is fairly isotropic in the whole temperature region. These features provide useful information to understand the magnetic properties of related materials.

Disorder upon disorder: Localization effects in the Kitaev spin liquid

In recent years, several magnetic Mott insulators with strong spin–orbit couplings were suggested to be proximate to the Kitaev quantum spin liquid (QSL) whose one of the most exciting features is the fractionalization of spin excitations into itinerant Majorana fermions and static Z2 fluxes. Motivated by the emergence of this plethora of 4d and 5d transition metal Kitaev materials and by the fact that some level of disorder is inevitable in real materials, here we study how the Kitaev QSL responds to various forms of disorder, such as vacancies, impurities, and bond randomness. First, we argue that the presence of the quenched disorder in the Kitaev QSL can lead to the Anderson localization of Majorana fermions and the appearance of Lifshitz tails. We point out that the Anderson localization of low-energy states is particularly strong in the extended Kitaev model with the time reversal symmetry breaking term. Second, we show that the disorder effects on the low-energy Majorana fermion modes can be detected in thermal transport. Third, we show that at finite temperatures the Z2 fluxes become thermally excited and give rise to an additional disorder for the Majorana fermions. This source of the disorder dominates at high temperatures. Fourth, we demonstrate that both the structure of the energy spectrum and the thermal transport properties of the disordered Kitaev QSL depend strongly on the character of disorder. While we find that both the site disorder and the bond randomness suppress the longitudinal thermal conductivity, the low-energy localization is stronger in the case of the site disorder.

Functional renormalization group study of the Kitaev- Γ model on the honeycomb lattice and emergent incommensurate magnetic correlations

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 $\Gamma$ interactions -- with the competition of the two potentially giving rise to a magnetically ordered ground state. In an attempt to aid future material investigations, we study the phase diagram of the spin-1/2 Kitaev-$\Gamma$ model on the honeycomb lattice. Employing a pseudofermion functional renormalization group approach which directly operates in the thermodynamic limit and captures the joint effect of thermal and quantum fluctuations, we unveil the existence of extended parameter regimes with emergent incommensurate magnetic correlations at finite temperature. We supplement our results with additional calculations on a finite cylinder geometry to investigate the impact of periodic boundary conditions on the incommensurate order, thereby providing a perspective on previous numerical studies on finite systems.

Magnetoelectric generation of a Majorana-Fermi surface in Kitaev's honeycomb model

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 linear in temperature heat capacity and finite, but non-quantized, thermal Hall response. Finally, we speculate on the potential for realization of this physics in Kitaev materials.