Materials potentially hosting Kitaev spin-liquid states are considered crucial for realizing topological quantum computing. However, the intricate nature of spin interactions within these materials complicates the precise measurement of low-energy spin excitations indicative of fractionalized excitations. Using Na$_{2}$Co$_2$TeO$_{6}$ as an example, we study these low-energy spin excitations using the time-resolved resonant elastic x-ray scattering (tr-REXS). Our observations unveil remarkably slow spin dynamics at the magnetic peak, whose recovery timescale is several nanoseconds. This timescale aligns with the extrapolated spin gap of $\sim$ 1 $μ$eV, obtained by density matrix renormalization group (DMRG) simulations in the thermodynamic limit. The consistency demonstrates the efficacy of tr-REXS in discerning low-energy spin gaps inaccessible to conventional spectroscopic techniques.
The Kitaev quantum spin liquid displays the fractionalization of quantum spins into Majorana fermions. The emergent Majorana edge current is predicted to manifest itself in the form of a finite thermal Hall effect, a feature commonly discussed in topological superconductors. Here we report on thermal Hall conductivity $κ_{xy}$ measurements in $α$-RuCl$_3$, a candidate Kitaev magnet with the two-dimensional honeycomb lattice. In a spin-liquid (Kitaev paramagnetic) state below the temperature characterized by the Kitaev interaction $J_K/k_B \sim 80$ K, positive $κ_{xy}$ develops gradually upon c…
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…
The insulating honeycomb magnet $α$-RuCl$_{3}$ exhibits fractionalized excitiations that signal its proximity to a Kitaev quantum spin liquid (QSL) state, however, at $T=0$, fragile long-range magnetic order arises from non-Kitaev terms in the Hamiltonian. Spin vacancies in the form of Ir$^{3+}$ substituted for Ru are found to destabilize this long-range order. Neutron diffraction and bulk characterization of Ru$_{1-x}$Ir$_{x}$Cl$_{3}$ show that the magnetic ordering temperature is suppressed with increasing $x$ and evidence of zizag magnetic order is absent for $x>0.3$. Inelastic neutron scat…
Proposed effective Hamiltonians from the literature for the material $α$-RuCl${}_3$ are used to compute the magnon thermal Hall conductivity, $κ_{xy}$, using linear spin wave theory for the magnetically ordered state. No model previously proposed that was tested explains published experimental data. Models with Kitaev interaction $K>0$ are seen to predict $κ_{xy}\gtrsim 0$, which is inconsistent with the data. Fluctuations toward a Kitaev-type spin liquid would have the wrong sign to explain the data. However, a slight variant of a previously proposed model predicts a large $κ_{xy}$, demonstra…
We use the constrained random phase approximation (cRPA) to derive from first principles the Ru-$t_{2g}$ Wannier function based model for the Kitaev spin-liquid candidate material $α$-RuCl$_3$. We find the non-local Coulomb repulsion to be sizable compared to the local one. In addition we obtain the contribution to the Hamiltonian from the spin-orbit coupling and find it to also contain non-negligible non-local terms. We invoke strong coupling perturbation theory to investigate the influence of these non-local elements of the Coulomb repulsion and the spin-orbit coupling on the magnetic intera…
We have investigated the sample dependence of the half-integer thermal Hall effect in $α$-RuCl$_3$ under a magnetic field tilted 45 degree from the $c$ axis to the $a$ axis. We find that the sample with the largest longitudinal thermal conductivity ($κ_{xx}$) shows the half-integer quantized thermal Hall effect expected in the Kitaev model. On the other hand, the quantized thermal Hall effect was not observed in the samples with smaller $κ_{xx}$. We suggest that suppressing the magnetic scattering effects on the phonon thermal conduction, which broaden the field-induced gap protecting the chir…
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…
Despite extensive investigations, a topological state that hosts Majorana edge modes in the magnetic field-induced quantum disordered state of the Kitaev candidate material $α$-RuCl$_3$ has been hotly debated. To gain more insight into this issue, we measured the thermal Hall conductivity $κ_{xy}$ of various samples grown by the Bridgman method. The results show that the half-integer quantum thermal Hall effect is intimately related to the magnitude of longitudinal thermal conductivity and the Néel temperature at zero field, both of which are sample dependent. Samples exhibiting the half-integ…
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 $α\text…
We have investigated the longitudinal thermal conductivity of $α$-RuCl$_{3}$, the magnetic state of which is considered to be proximate to a Kitaev honeycomb model, along with the spin susceptibility and magnetic specific heat. We found that the temperature dependence of the thermal conductivity exhibits an additional peak around 100 K, which is well above the phonon peak temperature ($\sim$ 50 K). The higher-temperature peak position is comparable to the temperature scale of the Kitaev couplings rather than the Néel temperatures below 15 K. The additional heat conduction was observed for all …
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 investigate the quantum spin liquid (QSL) ground state of anisotropic Kitaev model with antiferromagnetic (AFM) coupling under the $[001]$ magnetic field with the finite-temperature Lanczos method (FTLM). In this anisotropic AFM Kitaev model with $K_{X}=K_{Y}$, $K_{X}+K_{Y}+K_{Z}=-3K$, and $K_{Z}<-K$, with magnetic field increasing, the gapped QSL experiences a transition to a gapless QSL at $h_{c1}=gμ_{B}H_{z1}/K$, to another gapless QSL with $C_{6}$ rotational symmetry at $h_{c2}$, and to a new $U(1)$ gapless QSL between $h_{c3}$ and $h_{c4}$, respectively. These indicate that magnetic fi…
The spin S=$\frac{1}{2}$ Kitaev honeycomb model has attracted significant attention, since emerging candidate materials have provided a playground to test non-Abelian anyons. The Kitaev model with higher spins has also been theoretically studied, as it may offer another path to a quantum spin liquid. However, a microscopic route to achieve higher spin Kitaev models in solid state materials has not been rigorously derived. Here we present a theory of the spin S=1 Kitaev interaction in two-dimensional edge-shared octahedral systems. Essential ingredients are strong spin-orbit coupling in anions …
We study the effects of quantum fluctuations on the dynamical generation of a gap and on the evolution of the spin-wave spectra of a frustrated magnet on a triangular lattice with bond-dependent Ising couplings, analog of the Kitaev honeycomb model. The quantum fluctuations lift the subextensive degeneracy of the classical ground-state manifold by a quantum order-by-disorder mechanism. Nearest-neighbor chains remain decoupled and the surviving discrete degeneracy of the ground state is protected by a hidden model symmetry. We show how the four-spin interaction, emergent from the fluctuations, …
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…
Relationship between doping-induced in-gap states and spin excitations in Kitaev-Hubbard models
Department of Physics, Nanjing University（南京大学物理学院）；Collaborative Innovation Center of Advanced Microstructures, Nanjing University（南京大学先进微结构协同创新中心）；Jiangsu Key Laboratory of Quantum Information Science and Technology, Nanjing University（南京大学江苏省量子信息科学与技术重点实验室）；Department of Applied Physics, Nanjing University of Science and Technology（南京理工大学应用物理系）
$α$-RuCl$_3$ has been hinted as a spin-orbital-assisted Mott insulator in proximity to a Kitaev spin liquid state. Here we present ARPES measurements on single crystal $α$-RuCl$_3$ in both the pristine and electron-doped states, and combine them with LDA+SOC+U calculations performed for the several low-energy competing magnetically ordered states as well as the paramagnetic state. A large Mott gap is found in the measured band structure of the pristine compound that persists to more than 20 times beyond the magnetic ordering temperature, though the paramagnetic calculation shows almost no gap.…
The ruthenium halide $α$-RuCl$_{3}$ is a promising candidate for a Kitaev spin liquid. However, the microscopic model describing $α$-RuCl$_{3}$ is still debated partly because of a lack of analogue materials for $α$-RuCl$_{3}$, which prevents tracking of electronic properties as functions of controlled interaction parameters. Here, we report a successful synthesis of RuBr$_{3}$. The material RuBr$_{3}$~possesses BiI$_3$-type structure (space group: $R\overline{3}$) where Ru$^{3+}$ form an ideal honeycomb lattice. Although RuBr$_{3}$ has a negative Weiss temperature, it undergoes a zigzag antif…
Mott insulators under sufficiently strong spin-orbit coupling can display quantum spin liquid phases with topological order and fractional excitations. Quantum magnets with pure Kitaev spin exchange interactions can host a gapped quantum spin liquid with a single Majorana edge mode propagating in the counter-clockwise direction when a small positive magnetic field is applied. Here, we show how under a sufficiently strong positive magnetic field a topological transition into a gapped quantum spin liquid with two Majorana edge modes propagating in the clockwise direction occurs. The Dzyaloshinsk…
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…
Dominant Kitaev Interaction and Field-induced Quantum Disordered Phase in the Cobaltate Na$_2$Co$_2$TeO$_6$
Institute for Solid State Physics, University of Tokyo（东京大学固体物理研究所）；School of Physics, Southeast University（东南大学物理学院）；Anhui Key Laboratory of Low-Energy Quantum Materials and Devices, High Magnetic Field Laboratory, Hefei Institutes of Physical Science, Chinese Academy of Sciences（中国科学院合肥物质科学研究院强磁场科学中心）；School of Physical Science and Engineering, Beijing Jiaotong University（北京交通大学物理科学与工程学院）；Center for Quantum Materials, Seoul National University（首尔大学量子材料中心）；School of Physics, Georgia Institute of Technology（佐治亚理工学院物理学院）；Institute of Theoretical Physics, Chinese Academy of Sciences（中国科学院理论物理研究所）
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 investigate both the longitudinal thermal conductivity ($κ_{xx}$) and the planar thermal Hall conductivity ($κ_{xy}$) in the Kitaev spin liquid candidate of Co-based honeycomb antiferromagnet Na$_2$Co$_2$TeO$_6$ in a magnetic field ($B$) applied along the $a$ and $a^*$ axes. A finite $κ_{xy}$ is resolved for both field directions in the antiferromagnetic (AFM) phase below the Néel temperature of 27 K. The temperature dependence of $κ_{xy}/T$ shows the emergence of topological bosonic excitations. In addition, the field dependence of $κ_{xy}$ shows sign reversals at the critical fields in th…
We present a study of longitudinal thermal transport in the Kitaev spin model on the honeycomb lattice, focusing on the role of anisotropic exchange to cover both, gapless and gapped phases. Employing a complementary combination of exact diagonalization on small systems and an average gauge configuration approach for up to $\sim O(10^4)$ spinful sites, we report results for the dynamical energy current auto-correlation function as well as the dc thermal conductivity over a wide range of temperatures and exchange anisotropies. Despite a pseudogap in the current correlation spectra, induced by e…
The ruby lattice is a four-valent lattice interpolating between honeycomb and triangular lattices. In this work we investigate the topological spin-liquid phases of a spin Hamiltonian with Kitaev interactions on the ruby lattice using exact diagonalization and perturbative methods. The latter interactions combined with the structure of the lattice yield a model with $\mathbb{Z}_2 \times \mathbb{Z}_2$ gauge symmetry. We mapped out the phase digram of the model and found gapped and gapless spin-liquid phases. While the low energy sector of the gapped phase corresponds to the well-known topologic…
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…
The Kitaev quantum spin liquid (QSL) on the two-dimensional honeycomb lattice epitomizes an entangled topological state, where the spins fractionalize into Majorana fermions. This state has aroused tremendous interest because it harbors non-Abelian anyon excitations. The half-integer quantized thermal Hall (HIQTH) conductance observed in $α$-RuCl$_3$ is a key signature of these excitations. However, the fate of this topologically nontrivial state at intense fields remains largely elusive. Here, we report the thermal conductivity $κ$ and specific heat $C$ of $α$-RuCl$_3$ with in-plane magnetic …
The combination of geometric frustration, extended hopping, spin-orbit coupling, and a disordered magnetic ground state make NaRuO$_{2}$ an attractive Heisenberg-Kitaev candidate material. Historically, NaRuO$_2$ has been a challenging material to produce, even in polycrystalline form. Here we present synthetic efforts that identify a propensity for Na$_\text{Ru}$ defects to form in NaRuO$_2$, revealing a full solid-solution between NaRuO$_{2}$ and disordered Na$_2$RuO$_3$. We report the synthesis of alloys along the Na$_{3+x}$Ru$_{3-x}$O$_6$ solid solution and characterize changes in the bulk…
It is now well established that the Kitaev honeycomb model in a magnetic field along the $[111]$-direction harbors an intermediate gapless quantum spin liquid (QSL) phase sandwiched between a gapped non-abelian QSL at low fields $H< H_{c1}$ and a partially polarized phase at high fields $H> H_{c2}$. Here, we analyze the low field and high field phases and phase transitions in terms of single- and two-magnon excitations using exact diagonalization (ED) and density matrix renormalization group (DMRG) methods. We find that the energy to create a bound state of two-magnons $Δ_p$ becomes lower than…
Frustrated quantum magnets can harbor unconventional spin liquid ground states in which the elementary magnetic moments fractionalize into new emergent degrees of freedom. While the fractionalization of quantum numbers is one of the recurring themes in modern condensed matter physics, it often remains a challenge to devise a controlled analytical framework tracking this phenomenon. A notable exception is the exactly solvable Kitaev model, in which spin degrees of freedom fractionalize into Majorana fermions and a Z2 gauge field. Here we discuss the physics of fractionalization in three-dimensi…
We study the effect of adding disorder to the exactly solvable Kitaev model on the hyper-honeycomb lattice, which hosts both gapped and gapless spin liquid phases with an emergent $\mathbb{Z}_2$ gauge field. The latter has an unusual gapless spectrum of Majorana fermion excitations, with a co-dimension-two Fermi ring. We thus address the question of the interplay of topological physics and disorder by considering the properties of isolated single and pair of vacancies. We show that near the vacancies, the local magnetic response to a field $h_z$ is parametrically enhanced in comparison to the …
The Raman scattering with local optical excitation from the Majorana edge modes of Kitaev spin liquids and topological superconductors is studied theoretically. Although the effective one-dimensional model is common between these two cases, the coupling to the electromagnetic field is different. It is found that the Raman spectrum at low energy scales with $ω^3$ in Kitaev spin liquids while it shows the gap in topological superconductors. This is in sharp contrast to the infrared absorption, where the spectrum shows the gap in Kitaev spin liquids, while it behaves as $\sim ω^2$ in topological …
Recent numerical studies indicate that the antiferromagnetic Kitaev honeycomb lattice model undergoes a magnetic-field-induced quantum phase transition into a new spin-liquid phase. This intermediate-field phase has been previously characterized as a gapless spin liquid. By implementing a recently developed variational approach based on the exact fractionalized excitations of the zero-field model, we demonstrate that the field-induced spin liquid is gapped and belongs to Kitaev's 16-fold way. Specifically, the low-field non-Abelian liquid with Chern number $C=\pm 1$ transitions into an Abelian…
Quantum spin liquid involves fractionalized quasipariticles such as spinons and visons. They are expressed as itinerant Majorana fermions and $Z_2$ fluxes in the Kitaev model with bond-dependent exchange interactions on a honeycomb spin lattice. The observation has recently attracted attention for a candidate material $α$-RuCl$_3$, showing spin liquid behaviour induced by a magnetic field. Since the observable spin excitation is inherently composed of the two quasiparticles, which further admix each other by setting in the magnetic field as well as non-Kitaev interactions, their individual ide…
Frustrated magnetic systems exhibit many fascinating phases. Prime among them are quantum spin liquids, where the magnetic moments do not order even at zero temperature. A subclass of quantum spin liquids called Kitaev spin liquids are particularly interesting, because they are exactly solvable, can be realized in certain materials, and show a large variety of gapless and gapped phases. Here, we show that non-symmorphic symmetries can enrich spin liquid phases, such that the low-energy spinon degrees of freedom form three-dimensional Dirac cones or nodal chains. In addition, we suggest how suc…
