Muon Spin Relaxation Study of Spin Dynamics on a Kitaev honeycomb material H$_3$LiIr$_2$O$_6$
Yan-Xing Yang, Cheng-Yu Jiang, Liang-Long Huang, Zi-Hao Zhu, Chang-Sheng Chen, Qiong Wu, Zhao-Feng Ding, Cheng Tan, Pabi K. Biswas, Adrian D. Hillier, You-Guo S… 展开作者
Yan-Xing Yang, Cheng-Yu Jiang, Liang-Long Huang, Zi-Hao Zhu, Chang-Sheng Chen, Qiong Wu, Zhao-Feng Ding, Cheng Tan, Pabi K. Biswas, Adrian D. Hillier, You-Guo Shi, Cai Liu, Le Wang, Fei Ye, Jia-Wei Mei, Lei Shu
The vacancy effect in quantum spin liquid (QSL) has been extensively studied. A finite density of random vacancies in the Kitaev model can lead to a pileup of low-energy density of states (DOS), which is generally experimentally determined by a scaling behavior of thermodynamic or magnetization quantities. Here, we report detailed muon spin relaxation ($μ$SR) results of H$_3$LiIr$_2$O$_6$, a Kitaev QSL candidate with vacancies. The absence of magnetic order is confirmed down to 80 mK, and the spin fluctuations are found to be persistent at low temperatures. Intriguingly, the time-field scaling law of longitudinal-field (LF)-$μ$SR polarization is observed down to 0.1 K. This indicates a dynamical scaling, whose critical exponent 0.46 is excellently consistent with the scaling behavior of specific heat and magnetization data. All the observations point to the finite DOS with the form $N(E) \sim E^{-0.5}$ , which is expected for the Kitaev QSL in the presence of vacancies. Our μSR study provides a dynamical fingerprint of the power-law low-energy DOS, and introduces a crucial new insight into the vacancy effect in QSL.
H3LiIr2O6 is the first honeycomb-lattice system without any signs of long-range magnetic order down to the lowest temperatures, raising the hope for the realization of an ideal Kitaev quantum spin liquid. Its honeycomb layers are coupled by interlayer hydrogen bonds. Static or dynamic disorder of these hydrogen bonds was proposed to strongly affect the magnetic exchange and to make Kitaev-type interactions dominant. Using dielectric spectroscopy, here we provide experimental evidence for dipolar relaxations in H3LiIr2O6 and deuterated D3LiIr2O6, which mirror the dynamics of protons and deutero…
Recently H$_3$LiIr$_2$O$_6$ has been reported as a spin-orbital entangled quantum spin liquid (QSL) [K. Kitagawa et al., Nature {\bf 554}, 341 (2018)], albeit its connection to Kitaev QSL has not been yet identified. To unveil the related Kitaev physics, we perform the first Raman spectroscopy studies on single crystalline H$_3$LiIr$_2$O$_6$ samples. We implement a soft chemical replacement of Li$^+$ with H$^+$ from $α$-Li$_2$IrO$_3$ single crystals to synthesize the single crystal samples of the iridate second generation H$_3$LiIr$_2$O$_6$. The Raman spectroscopy can be used to diagnose the Q…
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…
We report low-temperature (down to $\sim$5 K) Raman signatures of the recently discovered intercalated honeycomb magnet Ag$_3$LiIr$_2$O$_6$, a putative Kitaev quantum spin liquid (QSL) candidate. The Kitaev QSL is predicted to host Majorana fermions as its emergent elementary excitations through a thermal fractionalization of entangled spins $S = 1/2$. We observe evidence of this fractionalization in the low-energy magnetic continuum whose temperature evolution harbours signatures of the predicted Fermi statistics obeyed by the itinerant Majorana quasiparticles. The magnetic Raman susceptibili…
The 5d-electron honeycomb compound H$_3$LiIr$_2$O$_3$ [K. Kitagawa $et$ $al.$, Nature 554, 341-345 (2018)] exhibits an apparent quantum spin liquid (QSL) state. In this intercalated spin-orbital compound, a remarkable pile up of low-energy states was experimentally observed in specific heat and nuclear magnetic (NMR) spin relaxation. We show that a bond disordered Kitaev model can naturally account for this phenomenon, suggesting that disorder plays an essential role in its theoretical description. In the exactly soluble Kitaev model, we obtain, via spin fractionalization, a random bipartite h…
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$_{6}…
A new quantum spin liquid (QSL) candidate material H$_{3}$LiIr$_{2}$O$_{6}$ was synthesized recently and was found not to show any magnetic order or phase transition down to low temperatures. In this work, we study the quantum dynamics of the hydrogen ions, i.e., protons, in this material by combining first-principles calculations and theoretical analysis. We show that each proton and its adjacent oxygen ions form an electric dipole. The dipole interactions and the proton tunneling are captured by a transverse-field Ising model with a quantum disordered paraelectric ground state. The dipole ex…
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 use x-ray spectroscopy at Ir L$_3$/L$_2$ absorption edge to study powder samples of the intercalated honeycomb magnet Ag$_3$LiIr$_2$O$_6$. Based on x-ray absorption and resonant inelastic x-ray scattering measurements, and exact diagonalization calculations including next-neighbour Ir-Ir electron hoping integrals, we argue that the intercalation of Ag atoms results in a nearly itinerant electronic structure with enhanced Ir-O hybridization. As a result of the departure from the local relativistic $j_{\rm eff}\! = \!1/2$ state, we find that the relative orbital contribution to the magnetic m…
We investigate the structural and magnetic properties of a Kitaev spin liquid candidate material Ag$_3$LiIr$_2$O$_6$ based on $^7$Li nuclear magnetic resonance line shape, Knight shift and spin-lattice relaxation rate $1/T_1$. The first sample A shows signatures of magnetically ordered spins, and exhibits one sharp $^7$Li peak with FWHM increasing significantly below 14~K. $1/T_1^{stretch}$ of this sample displays a broad local maximum at 40~K, followed by a very sharp peak at $T_N = 9\pm1$~K due to critical slowing down of Ir spin fluctuations, a typical signature of magnetic long range order…
The Kitaev honeycomb model has attracted significant attention due to its exactly solvable spin-liquid ground state with fractionalized Majorana excitations and its possible materialization in magnetic Mott insulators with strong spin-orbit couplings. Recently, the 5d-electron compound H$_{3}$LiIr$_{2}$O$_{6}$ has shown to be a strong candidate for Kitaev physics considering the absence of any signs of a long-range ordered magnetic state. In this work, we demonstrate that a finite density of random vacancies in the Kitaev model gives rise to a striking pileup of low-energy Majorana eigenmodes …
A decade ago, Alexei Kitaev proposed an exactly solvable $S$ = 1/2 model on a two-dimensional honeycomb lattice, where the spins fractionalize into Majorana fermions and form a topological quantum spin liquid (QSL) in the ground state. It was soon recognized that a family of complex iridium oxides, as well as ruthenium chloride, with honeycomb structure are magnetic insulators and accommodate essential ingredients of the Kitaev model, due to the interplay of electron correlation and spin-orbit coupling. This initiated a race to materialize the Kitaev QSL and to capture the signature of Majoran…
We have investigated experimentally and theoretically the series (Na$_{1-x}$Li$_{x}$)$_{2}$IrO$_{3}$. Contrary to what has been believed so far, only for $x\leq0.25$ the system forms uniform solid solutions. For larger Li content, as evidenced by powder X-ray diffraction, scanning electron microscopy and density functional theory calculations, the system shows a miscibility gap and a phase separation into an ordered Na$_{3}$LiIr$_2$O$_{6}$ phase with alternating Na$_3$ and LiIr$_2$O$_6$ planes, and a Li-rich phase close to pure Li$_{2}$IrO$_{3}$. For $x\leq 0.25$ we observe (1) an increase of …
In this work, we investigate whether the Kitaev honeycomb model can serve as a starting point to realize the intriguing physics of the Sachdev-Ye-Kitaev (SYK) model. The starting point is to strain the system, which leads to flat bands reminiscent of Landau levels, thereby quenching the kinetic energy. The presence of weak residual perturbations, such as Heisenberg interactions and the $γ$-term, creates effective interactions between the Majorana modes when projected into the flux-free sector. We assume the resulting interactions to be effectively random. This leads to a bipartite Sachdev-Ye-K…
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…
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$…
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 $θ_{CW}$ …
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 calculate the resonant inelastic X-ray scattering (RIXS) response of the Kitaev honeycomb model, an exactly solvable quantum-spin-liquid model with fractionalized Majorana and flux excitations. We find that the fundamental RIXS channels, the spin-conserving (SC) and the non-spin-conserving (NSC) ones, do not interfere and give completely different responses. SC-RIXS picks up exclusively the Majorana sector with a pronounced momentum dispersion, whereas NSC-RIXS also creates immobile fluxes, thereby rendering the response only weakly momentum dependent, as in the spin structure factor measur…
Low-energy states of quantum spin liquids are thought to involve partons living in a gauge-field background. We study the spectrum of Majorana fermions of Kitaev's honeycomb model on spherical clusters. The gauge field endows the partons with half-integer orbital angular momenta. As a consequence, the multiplicities reflect not the point-group symmetries of the cluster, but rather its projective symmetries, operations combining physical and gauge transformations. The projective symmetry group of the ground state is the double cover of the point group.
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…
The Kitaev-Heisenberg model defined on both honeycomb and triangular lattices has been studied intensively in recent years as a possible model to describe spin-orbital physics in iridium oxides. In the model, there are many phases characteristic for each lattice. However, there is no study how the phases in the two lattices merge each other when geometry changes from honeycomb lattice to triangular lattice. We investigate the ground state of the Kitaev-Heisenberg model defined on the system connecting the honeycomb and triangular lattices, named a honeycomb-triangular lattice. We obtain a grou…
The properties of Kitaev materials are attracting ever increasing attention owing to their exotic properties. In realistic two-dimensional materials, Kitaev interaction is often accompanied by the Dzyloshinskii-Moriya interaction, which poses a challenge of distinguishing their magnitude separately. In this work, we demonstrate that it can be done by accessing magnonic transport properties. By studying honeycomb ferromagnets exhibiting Dzyaloshinskii-Moriya and Kitaev interactions simultaneously, we reveal non-trivial magnonic topological properties accompanied by intricate magnonic transport …
In addition to the Kitaev ($K$) interaction, candidate Kitaev materials also possess Heisenberg ($J$) and off-diagonal symmetric ($Γ$) couplings. We investigate the quantum ($S = 1/2$) $K$-$J$-$Γ$ model on the honeycomb lattice by a variational Monte Carlo (VMC) method. In addition to the "generic" Kitaev spin liquid (KSL), we find that there is just one proximate KSL (PKSL) phase, while the rest of the phase diagram contains different magnetically ordered states. The PKSL is a gapless Z$_2$ state with 14 Majorana cones, which in contrast to the KSL has a gapless spin response. In a magnetic f…
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…
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…
Recent proposals for spin-1 Kitaev materials, such as honeycomb Ni oxides with heavy elements of Bi and Sb, have shown that these compounds naturally give rise to antiferromagnetic (AFM) Kitaev couplings. Conceptual interest in such AFM Kitaev systems has been sparked by the observation of a transition to a gapless $U(1)$ spin liquid at intermediate field strengths in the AFM spin-1/2 Kitaev model. However, all hitherto known spin-1/2 Kitaev materials exhibit ferromagnetic bond-directional exchanges. Here we discuss the physics of the spin-1 Kitaev model in a magnetic field and show, by extens…
University of Toronto（多伦多大学）；Canadian Institute for Advanced Research（加拿大高等研究院）
Recently, honeycomb cobaltates with 3$d^7$ were proposed to display Kitaev physics despite weak spin-orbit coupling. However, other theoretical and experimental works found leading XXZ Heisenberg and negligible Kitaev interactions in BaCo$_2$(AsO$_4$)$_2$ (BCAO), which calls for a further study to clarify the origin of the discrepancies. Here we derive the analytical expressions of the spin model using strong-coupling perturbation theory. With tight binding parameters obtained by {\it ab-initio} calculations for idealized honeycomb BCAO, we find that the largest intraorbital $t_{2g}-t_{2g}$ ex…
We apply the SU(2) slave fermion formalism to the Kitaev honeycomb lattice model. We show that both the Toric Code phase (the A phase) and the gapless phase of this model (the B phase) can be identified with p-wave superconducting phases of the slave fermions, with nodal lines which, respectively, do not or do intersect the Fermi surface. The non-Abelian Ising anyon phase is a $p+ip$ superconducting phase which occurs when the B phase is subjected to a gap-opening magnetic field. We also discuss the transitions between these phases in this language.
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…
The main question we address is how to probe the fractionalized excitations of a quantum spin liquid (QSL), for example, in the Kitaev honeycomb model. By analyzing the energy spectrum and entanglement entropy, for antiferromagnetic couplings and a field along either [111] or [001], we find a gapless QSL phase sandwiched between the non-Abelian Kitaev QSL and polarized phases. Increasing the field strength towards the polarized limit destroys this intermediate QSL phase, resulting in a considerable reduction in the number of frequency modes and the emergence of a beating pattern in the local d…
Due to the combination of a substantial spin-orbit coupling and correlation effects, iridium oxides hold a prominent place in the search for novel quantum states of matter, including, e.g., Kitaev spin liquids and topological Weyl states. We establish the promise of the very recently synthesized hyper-honeycomb iridate $β$-Li2IrO3 in this regard. A detailed theoretical analysis reveals the presence of large ferromagnetic first-neighbor Kitaev interactions, while a second-neighbor antiferromagnetic Heisenberg exchange drives the ground state from ferro to zigzag order via a three-dimensional Ki…
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 investigate the generic features of the low energy dynamical spin structure factor of the Kitaev honeycomb quantum spin liquid perturbed away from its exact soluble limit by generic symmetry-allowed exchange couplings. We find that the spin gap persists in the Kitaev-Heisenberg model, but generally vanishes provided more generic symmetry-allowed interactions exist. We formulate the generic expansion of the spin operator in terms of fractionalized Majorana fermion operators according to the symmetry enriched topological order of the Kitaev spin liquid, described by its projective symmetry gr…
We derive and study a spin one-half Hamiltonian on a honeycomb lattice describing the exchange interactions between Ir$^{4+}$ ions in a family of layered iridates $A_2$IrO$_3$ ($A$=Li,Na). Depending on the microscopic parameters, the Hamiltonian interpolates between the Heisenberg and exactly solvable Kitaev models. Exact diagonalization and a complementary spin-wave analysis reveal the presence of an extended spin-liquid phase near the Kitaev limit and a conventional Néel state close to the Heisenberg limit. The two phases are separated by an unusual stripy antiferromagnetic state, which is t…
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 study the gapped phase of Kitaev's honeycomb model (a Z_2 spin liquid) in the presence of lattice defects. We find that some dislocations and bond defects carry unpaired Majorana fermions. Physical excitations associated with these defects are (complex) fermion modes made out of two (real) Majorana fermions connected by a Z_2 gauge string. The quantum state of these modes is robust against local noise and can be changed by winding a Z_2 vortex around a dislocation. The exact solution respects gauge invariance and reveals a crucial role of the gauge field in the physics of Majorana modes.
Intensive studies of the interplay between spin-orbit coupling (SOC) and electronic correlations in transition metal compounds have recently been undertaken. In particular, $j_{\rm eff}$ = 1/2 bands on a honeycomb lattice provide a pathway to realize Kitaev's exactly solvable spin model. However, since current wisdom requires strong atomic SOC to make $j_{\rm eff}=1/2$ bands, studies have been limited to iridium oxides. Contrary to this expectation, we demonstrate how Kitaev interactions arise in 4$d$-orbital honeycomb $α$-RuCl$_3$, despite having significantly weaker SOC than the iridium oxid…
Recently, realizations of Kitaev physics have been sought in the A2IrO3 family of honeycomb iridates, originating from oxygen-mediated exchange through edge-shared octahedra. However, for the j = 1/2 Mott insulator in these materials exchange from direct d-orbital overlap is relevant, and it was proposed that a Heisenberg term should be added to the Kitaev model. Here we provide the generic nearest-neighbour spin Hamiltonian when both oxygen-mediated and direct overlap are present, containing a bond dependent off-diagonal exchange in addition to Heisenberg and Kitaev terms. We analyze this com…
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.
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…
We study the Kitaev-Heisenberg model with spin-1 local degree of freedom on a two-dimensional honeycomb lattice numerically by density matrix renormalization group method. By tuning the relative value of the Kitaev and Heisenberg exchange couplings, we obtain the whole phase diagram with two spin liquid phases and four symmetry broken phases. We identify that the spin liquid phases are gapless by calculating the central charge at the pure Kitaev points without Heisenberg interaction. Comparing to its spin-1/2 counterpart, the position and number of gapless modes of the spin-1 case are quite di…
We study the ground state of the 1D Kitaev-Heisenberg (KH) model using the density-matrix renormalization group and Lanczos exact diagonalization methods. We obtain a rich ground-state phase diagram as a function of the ratio between Heisenberg ($J=\cosϕ)$ and Kitaev ($K=\sinϕ$) interactions. Depending on the ratio, the system exhibits four long-range ordered states: ferromagnetic-$z$ , ferromagnetic-$xy$, staggered-$xy$, Néel-$z$, and two liquid states: Tomonaga-Luttinger liquid and spiral-$xy$. The two Kitaev points $ϕ=\fracπ{2}$ and $ϕ=\frac{3π}{2}$ are singular. The $ϕ$-dependent phase dia…
Compounds of transition metal ions with strong spin-orbit coupling recently attracted attention due to the possibility to host frustrated bond-dependent anisotropic magnetic interactions. In general, such interactions lead to complex phase diagrams that may include exotic phases, e.g. the Kitaev spin liquid. Here we report on our comprehensive analysis of the global phase diagram of the extended Kitaev-Heisenberg model relevant to honeycomb lattice compounds Na2IrO3 and alpha-RuCl3. We have utilized recently developed method based on spin coherent states that enabled us to resolve arbitrary sp…
Motivated by recent experiments on the Kitaev honeycomb magnet $α\text{-RuCl}_3$, we introduce time-domain probes of the edge and quasiparticle content of non-Abelian spin liquids. Our scheme exploits ancillary quantum spins that communicate via time-dependent tunneling of energy into and out of the spin liquid's chiral Majorana edge state. We show that the ancillary-spin dynamics reveals the edge-state velocity and, in suitable geometries, detects individual non-Abelian anyons and emergent fermions via a time-domain counterpart of quantum-Hall anyon interferometry. We anticipate applications …
An osmium chloride with the chemical formula of OsxCl3 (x = 0.81) was synthesized and its crystal structure and thermodynamic properties were investigated. OsxCl3 crystallizes in a layered CdCl2-type structure with the triangular lattice partially occupied by Os ions on average. However, on microscopic length scales, the triangular lattice is composed of nano-domains with a honeycomb arrangement of Os ions, as observed by electron microscopy and Raman scattering experiments. Magnetization and heat capacity measurements revealed an absence of magnetic long-range order down to 0.08 K, while a br…
We theoretically propose a family of $f$-electron based magnets that realizes Kitaev-type bond-dependent anisotropic interactions. Based on {\it ab initio} calculations, we show that $A_2$PrO$_3$ ($A$: alkali metals) crystalize in a triclinic structure with honeycomb layers of edge-sharing PrO$_6$ octahedra. Each Pr$^{4+}$ cation has a $4f$ electron in the $Γ_7$ doublet, which comprises a spin-orbital entangled Kramers pair with the effective moment $J_{\rm eff}=1/2$. By using the Wannier orbitals from the {\it ab initio} calculations, we find that the effective interactions between the $J_{\r…
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…
We study the extended Kitaev-Heisenberg (EKH) quantum spin model by adding bond-dependent off-diagonal Heisenberg term into the original KH model, which was recently proposed to describe the honeycomb Iridates. A rigorous mathematical mapping of spin operators reveals the intrinsic symmetry of the model Hamiltonian. By employing an unbiased numerical entanglement renormalization method based on tensor network ansatz, we obtain the global phase diagram containing eight distinct quantum phases. By using the dual mapping of spin operators, each of the individual magnetic phase in the global phase…
We compute the quantum Fisher information (QFI) associated with two different local operators in the Kitaev honeycomb model, and find divergent behaviour in the second derivatives of these quantities with respect to the driving parameter at the quantum phase transition between the gapped and gapless phases for both fully anti-ferromagnetic and fully ferromagnetic exchange couplings. The QFI associated with a local magnetization operator behaves differently from that associated with a local bond operator depending on whether the critical point is approached from the gapped or gapless side. We s…
Here we revisit the thermodynamics of the Kitaev quantum spin liquid realized on the honeycomb lattice. We address two main questions: First, we investigate whether there are observable thermodynamic signatures of the topological Majorana boundary modes of the Kitaev honeycomb model. We argue that for the time-reversal invariant case the residual low-temperature entropy is the primary thermodynamic signature of these Majorana edge modes, and verify using large-scale Monte Carlo simulations that this residual entropy is present in the full Kitaev model. When time-reversal symmetry is broken, th…
Based on the Dirac spinor representation of the SO(4) group, we discuss the relationship between three types of representation of spin in terms of Majorana fermions, namely the Kitaev representation, the SO(3) representation and the SO(4) chiral representation. Comparing the three types, we show that the Hilbert space of the SO(3) representation is different from the other two by requiring pairing of sites, but it has the advantage over the other two in that no unphysical states are involved. As an example of its application, we present a new alternative solution of the Kitaev honeycomb model.…
The Kitaev model, characterized by bond-dependent Ising spin interactions among spin-orbit entangled dipole moments in Mott insulators, offered a new approach to quantum spin liquids. Motivated by another type of bond-dependent interaction among quadrupole moments in $5d^2$ Mott insulators, we provide a microscopic route to uncover the Kitaev multipolar liquid, featuring fractionalized excitations out of non-Kramers doublets carrying multipole moments. The key ingredient is the magnetic field that allows for bond-anisotropic quadrupole-octupole interactions via mixing with the excited triplet …
