In the Kitaev honeycomb model, the quantum spin fractionalizes into itinerant Majorana and gauge flux spontaneously upon cooling, leading to rich experimental ramifications at finite temperature and an upsurge of research interest. In this work, we employ the exponential tensor renormalization group approach to explore the Kitaev model under various perturbations, including the external fields, Heisenberg, and the off-diagonal couplings that are common in the Kitaev materials. Through large-scale manybody calculations, we find a Kitaev fractional liquid at intermediate temperature that is robust against perturbations. The fractional liquid exhibits universal thermodynamic behaviors, including the fractional thermal entropy, metallic specific heat, and an intermediate-temperature Curie law of magnetic susceptibility. The emergent universal susceptibility behavior, with a modified Curie constant, can be ascribed to the strongly fluctuating $\mathbb{Z}_2$ fluxes as well as the extremely short-ranged and bond-directional spin correlations. With this insight, we revisit the susceptibility measurements of Na$_2$IrO$_3$ and $α$-RuCl$_3$, and find evident signatures of finite-temperature fractionalization and ferromagnetic Kitaev couplings. Moreover, the peculiar spin correlation in the fractional liquid corresponds to a stripy structure factor which rotates in the extended Brillouin zone as the spin component changes. Therefore, our findings encourage future experimental exploration of fractional liquid in the Kitaev materials by thermodynamic measurements and spin-resolved structure factor probes.
Fractionalization is a hallmark of spin-liquid behavior; it typically leads to response functions consisting of continua instead of sharp modes. However, microscopic processes can enable the formation of short-distance bound states of fractionalized excitations, despite asymptotic deconfinement. Here we study such bound-state formation for the $Z_2$ spin liquid realized in Kitaev's honeycomb compass model, supplemented by a kekule distortion of the lattice. Bound states between flux pairs and Majorana fermions form in the Majorana band gaps. We calculate the dynamic spin susceptibility and sho…
While phase transitions between magnetic analogs of three states of matter --- a long-range ordered state, paramagnet, and spin liquid --- have been extensively studied, the possibility of "liquid-liquid" transitions, namely, between different spin liquids, remains elusive. By introducing the additional Ising coupling into the honeycomb Kitaev model with bond asymmetry, we discover that the Kitaev spin liquid turns into a spin-nematic quantum paramagnet before a magnetic order is established by the Ising coupling. The quantum phase transition between the two liquid states accompanies a topolog…
The quest for Kitaev spin liquids in particular three dimensional solids is long sought goal in condensed matter physics, as these states may give rise to exotic new types of quasi-particle excitations carrying fractional quantum numbers namely Majorana Fermionic excitations. Here we report the experimental signature of this characteristic feature of the Kitaev spin liquid via Raman measurements. Sm2ZnIrO6 is a strongly spin orbit coupled Mott insulator, where Jeff = 1/2 controls the physics, which provide striking evidence for this characteristic feature of the Kitaev spin liquid. As the temp…
We investigate the real-time spin response of the $S=1$ Kitaev model upon stimuli of a pulsed magnetic field in one of the edges using the exact diagonalization method. It is found that the pulsed magnetic field has no effect on the appearance of the spin moments in the quantum spin liquid region, but induces the spin oscillations in the other edge region with a small magnetic field. This is understood by the existence of the itinerant quasiparticles, which carry the spin excitations without the spin polarization in the quantum spin liquid state. This suggests that the spin fractionalizations …
Quantum spin liquids have fascinated condensed matter physicists for decades because of their unusual properties such as spin fractionalization and long-range entanglement. Unlike conventional symmetry breaking the topological order underlying quantum spin liquids is hard to detect experimentally. Even theoretical models are scarce for which the ground state is established to be a quantum spin liquid. The Kitaev honeycomb model and its generalizations to other tri-coordinated lattices are chief counterexamples --- they are exactly solvable, harbor a variety of quantum spin liquid phases, and a…
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…
Fractionalized Fermi liquids (FL$^\ast$) have been introduced as non-Fermi-liquid metallic phases, characterized by coexisting electron-like charge carriers and local moments which itself form a fractionalized spin liquid. Here we investigate a Kondo lattice model on the honeycomb lattice with compass interactions among the local moments, a concrete model hosting FL$^\ast$ phases based on Kitaev's $\mathbb{Z}_2$ spin liquid. We characterize the FL$^\ast$ phases via perturbation theory, and we employ a Majorana-fermion mean-field theory to map out the full phase diagram. Most remarkably we find…
We investigate ground-state and finite temperature properties of the mixed-spin $(s, S)$ Kitaev model. When one of spins is half-integer and the other is integer, we introduce two kinds of local symmetries, which results in a macroscopic degeneracy in each energy level. Applying the exact diagonalization to several clusters with $(s, S)=(1/2, 1)$, we confirm the presence of this large degeneracy in the ground states, in contrast to the conventional Kitaev models. By means of the thermal pure quantum state technique, we calculate the specific heat, entropy, and spin-spin correlations in the sys…
We study ground-state and thermodynamic properties of an $S=1$ Kitaev model. We first clarify the existence of global parity symmetry in addition to the local symmetry on each plaquette, which enables us to perform the large scale calculations up to 24 sites. It is found that the ground state should be singlet and its energy is estimated as $E/N\sim -0.65J$, where $J$ is the Kitaev exchange coupling. We find that a lowest excited state belongs to the same subspace as the ground state and the gap monotonically decreases with increasing system size, which suggests that the ground state of the $S…
The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z2 gauge flux. Detection of these excitations remains challenging, because of their fractional quantum numbers and non-locality. It was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we uncover this effect in $α$-RuCl3 using inelastic X-ray scattering with meV resolut…
Significant efforts have focused on the magnetic excitations of relativistic Mott insulators, predicted to realize the Kitaev quantum spin liquid (QSL). This exactly solvable model involves a highly entangled state resulting from bond-dependent Ising interactions that produce excitations which are non-local in terms of spin flips. A key challenge in real materials is identifying the relative size of the non-Kitaev terms and their role in the emergence or suppression of fractional excitations. Here, we identify the energy and temperature boundaries of non-Kitaev interactions by direct compariso…
Motivated by the ongoing effort to search for high-resolution signatures of quantum spin liquids, we investigate the temperature dependence of the indirect resonant inelastic x-ray scattering (RIXS) response for the Kitaev honeycomb model. We find that, as a result of spin fractionalization, the RIXS response changes qualitatively at two well-separated temperature scales, $T_L$ and $T_H$, which correspond to the characteristic energies of the two kinds of fractionalized excitations, $\mathbb{Z}_2$ gauge fluxes and Majorana fermions, respectively. While thermally excited $\mathbb{Z}_2$ gauge fl…
Experimental identification of quantum spin liquids remains a challenge, as the pristine nature is to be seen in asymptotically low temperatures. We here theoretically show that the precursor of quantum spin liquids appears in the spin dynamics in the paramagnetic state over a wide temperature range. Using the cluster dynamical mean-field theory and the continuous-time quantum Monte Carlo method, which are newly developed in the Majorana fermion representation, we calculate the dynamical spin structure factor, relaxation rate in nuclear magnetic resonance, and magnetic susceptibility for the h…
Kitaev quantum spin liquid is a topological magnetic quantum state characterized by Majorana fermions of fractionalized spin excitations, which are identical to their own antiparticles. Here, we demonstrate emergence of Majorana fermions thermally fractionalized in the Kitaev honeycomb spin lattice α-RuCl3. The specific heat data unveil the characteristic two-stage release of magnetic entropy involving localized and itinerant Majorana fermions. The inelastic neutron scattering results further corroborate these two distinct fermions by exhibiting quasielastic excitations at low energies around …
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 3D Kitaev and Kitaev-Heisenberg models respectively on the hyperhoneycomb and hyperoctagon lattices, both at zero and finite-temperature, in the thermodynamic limit. Our analysis relies on advanced tensor network (TN) simulations based on graph Projected Entangled-Pair States (gPEPS). We map out the TN phase diagrams of the models and characterize their underlying gapped and gapless phases both at zero and finite temperature. In particular, we demonstrate how cooling down the hyperhoneycomb system from high-temperature leads to fractionalization of spins to itinerant Majorana ferm…
Finite-temperature ($T$) properties of a Kitaev model defined on a honeycomb lattice are investigated by a quantum Monte Carlo simulation, from the viewpoint of fractionalization of quantum $S=1/2$ spins into two types of Majorana fermions, itinerant and localized. In this system, the entropy is released successively at two well-separated $T$ scales, as a clear indication of the thermal fractionalization. We show that the high-$T$ crossover, which is driven by itinerant Majorana fermions, is closely related with the development of nearest-neighbor spin correlations. On the other hand, the low-…
Kitaev quantum spin liquids host Majorana fermions via the fractionalization of spins. In a magnetic field, the Majorana fermions were predicted to comprise a topological state, which has attracted great attention by the discovery of the half-quantized thermal Hall conductivity. Nevertheless, a reliable theory remains elusive for the field effect, especially at finite temperature. Here we present unbiased large-scale numerical results for the Kitaev model in a wide range of magnetic field and temperature. We find that the unconventional paramagnetic region showing fractional spin dynamics exte…
We develop high temperature series expansions for the thermodynamic properties of the honeycomb-lattice Kitaev-Heisenberg model. Numerical results for uniform susceptibility, heat capacity and entropy as a function of temperature for different values of the Kitaev coupling $K$ and Heisenberg exachange coupling $J$ (with $|J|\le |K|$) are presented. These expansions show good convergence down to a temperature of a fraction of $K$ and in some cases down to $T=K/10$. In the Kitaev exchange dominated regime, the inverse susceptibility has a nearly linear temperature dependence over a wide temperat…
The topological non-triviality of insulating phases of matter is by now well understood through topological K-theory where the indices of the Dirac operators are assembled into topological classes. We consider in the context of the Kitaev chain a notion of a generalized Dirac operator where the associated Clifford algebra is centrally extended. We demonstrate that the central extension is achieved via taking rational operator powers of Pauli matrices that appear in the corresponding BdG Hamiltonian. Doing so introduces a pseudo-metallic component to the topological phase diagram within which t…
We describe a mechanism for order fractionalization in a two-dimensional Kondo lattice model, in which electrons interact with a gapless spin liquid of Majorana fermions described by the Yao-Lee (YL) model. When the Kondo coupling to the conduction electrons exceeds a critical value, the model develops a superconducting instability into a state where the spinor order parameter carries charge $e$ and spin $S=1/2$. The broken symmetry state develops a gapless Majorana Dirac cone in the bulk. By including an appropriate gauge string, we can show that the charge $e$, spinorial order develops off-d…
A Majorana fermion is a fermionic particle that is its own antiparticle. Since the theoretical discovery in 1937, the exotic particle has long been searched in particle physics. In the last few decades, however, it has attracted renewed interest in condensed matter physics, where it can be realized as an elementary excitation (quasiparticle) in quantum states of matter. In this review, we discuss another platform for Majorana fermions, the quantum spin liquid, in which interacting magnetic moments remain disordered down to the lowest temperature under strong quantum fluctuations. They are char…
We compute the low-energy excitation spectrum and the dynamical spin structure factor of the Kitaev-Heisenberg-Gamma model through a variational approach based on the exact fractionalized excitations of the pure Kitaev honeycomb model. This novel approach reveals the physical reason for the asymmetric stability of the Kitaev spin liquid phases around the ferromagnetic and antiferromagnetic Kitaev limits. Moreover, we demonstrate that the fractionalized excitations form bound states in specific regions of each Kitaev spin liquid phase and that certain phase transitions induced by Heisenberg and…
Two- and three-dimensional Kitaev magnets are prototypical frustrated quantum spin systems, in which the original spin degrees of freedom fractionalize into Majorana fermions and a $\mathbb{Z}_2$ gauge field -- a purely local phenomenon that reveals itself as a thermodynamic crossover at a temperature scale set by the strength of the bond-directional interactions. For conventional Kitaev magnets, the low-temperature thermodynamics reveals a second transition at which the $\mathbb{Z}_2$ gauge field orders and the system enters a spin liquid ground state. Here we discuss an explicit example that…
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…
In the field of frustrated magnetism, Kitaev models provide a unique framework to study the phenomena of spin fractionalization and emergent lattice gauge theories in two and three spatial dimensions. Their ground states are quantum spin liquids, which can typically be described in terms of a Majorana band structure and an ordering of the underlying $\mathbb{Z}_2$ gauge structure. Here we provide a comprehensive classification of the "gauge physics" of a family of elementary three-dimensional Kitaev models, discussing how their thermodynamics and ground state order depends on the underlying la…
The pursuit of quantum spin liquid (QSL) in the Kitaev honeycomb magnets has drawn intensive attention recently. In particular, $α$-RuCl$_3$ has been widely recognized as a promising candidate for the Kitaev QSL. Although the compound exhibits an antiferromagnetic order under zero field, it is believed to be endowed with fractionalized excitations, and can be driven to the QSL phase by magnetic fields. Here, based on a realistic $K$-$J$-$Γ$-$Γ'$ model for $α$-RuCl$_3$ [1], we exploit the exponential tensor renormalization group approach to explore the phase diagram of the compound under magnet…
We propose that resonant inelastic X-ray scattering (RIXS) is an effective probe of the fractionalized excitations in three-dimensional (3D) Kitaev spin liquids. While the non-spin-conserving RIXS responses are dominated by the gauge-flux excitations and reproduce the inelastic-neutron-scattering response, the spin-conserving (SC) RIXS response picks up the Majorana-fermion excitations and detects whether they are gapless at Weyl points, nodal lines, or Fermi surfaces. As a signature of symmetry fractionalization, the SC RIXS response is suppressed around the $Γ$ point. On a technical level, w…
In conventional insulating magnets, heat is carried by magnons and phonons. In contrast, when the magnets harbor a quantum spin liquid state, emergent quasiparticles from the fractionalization of quantum spins can carry heat. Here, we investigate unconventional thermal transport yielded by such exotic carriers, in both longitudinal and transverse components, for the Kitaev model, whose ground state is exactly shown to be a quantum spin liquid with fractional excitations described as itinerant Majorana fermions and localized $Z_2$ fluxes. We find that the longitudinal thermal conductivity exhib…
We study the thermodynamic properties of modified spin-$S$ Kitaev models introduced by Baskaran, Sen and Shankar (Phys. Rev. B 78, 115116 (2008)). These models have the property that for half-odd-integer spins their eigenstates map on to those of spin-1/2 Kitaev models, with well-known highly entangled quantum spin-liquid states and Majorana fermions. For integer spins, the Hamiltonian is made out of commuting local operators. Thus, the eigenstates can be chosen to be completely unentangled between different sites, though with a significant degeneracy for each eigenstate. For half-odd-integer …
The pure Kitaev honeycomb model harbors a quantum spin liquid in zero magnetic fields, while applying finite magnetic fields induces a topological spin liquid with non-Abelian anyonic excitations. This latter phase has been much sought after in Kitaev candidate materials, such as $α$-RuCl$_3$. Currently, two competing scenarios exist for the intermediate field phase of this compound ($B=7-10$ T), based on experimental as well as theoretical results: (i) conventional multiparticle magnetic excitations of integer quantum number vs. (ii) Majorana fermionic excitations of possibly non-Abelian natu…
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…
Quantum spin liquids are highly fascinating quantum liquids in which the spin degrees of freedom fractionalize. An interesting class of spin liquids are the exactly solvable, three-dimensional Kitaev spin liquids. Their fractionalized excitations are Majonara fermions, which may exhibit a variety of topological band structures --- ranging from topologically protected Weyl semi-metals over nodal semi-metals to systems with Majorana Fermi surfaces. We study the entanglement spectrum of such Kitaev spin liquids and verify that it is closely related to the topologically protected edge spectrum. Mo…
Unambiguous identification of fractionalized excitations in quantum spin liquids has been a long-standing issue in correlated topological phases. Conventional spectroscopic probes, such as the dynamical spin structure factor, can only detect composites of fractionalized excitations, leading to a broad continuum in energy. Lacking a clear signature in conventional probes has been the biggest obstacle in the field. In this work, we theoretically investigate what kinds of distinctive signatures of fractionalized excitations can be probed in two-dimensional nonlinear spectroscopy by considering th…
$α$-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…
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…
A key characteristic of quantum spin liquids(QSL) is the presence of fractional excitations related to their entanglement properties, yet experimental verification of their statistics is missing. For example, in the potential Kitaev spin liquid, RuCl3 experiments uncovered signs of fractional particles, though not their Fermi statistics. Here we employ Raman scattering to reveal the true nature of the magnetic excitations, using improved experimental methods and analysis to remove the influence of laser heating and thermal fluctuations. Via the energy loss and gain spectra, we extract the ener…
The exactly-solvable Kitaev model of two-dimensional honeycomb magnet leads to a quantum spin liquid (QSL) characterized by Majorana fermions, relevant for fault-tolerant topological quantum computations. In the high-field paramagnetic state of $α$-RuCl3, half-integer quantization of thermal Hall conductivity has been reported as a signature of edge current, but the bulk nature of this state remains elusive. Here, from high-resolution heat capacity measurements under in-plane field rotation, we find strongly angle-dependent low-energy excitations in bulk $α$-RuCl3. The excitation gap has a sex…
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…
Kitaev's honeycomb-lattice compass model describes a spin liquid with emergent fractionalized excitations. Here we study the physics of isolated magnetic impurities coupled to the Kitaev spin-liquid host. We reformulate this Kondo-type problem in terms of a many-state quantum impurity coupled to a multichannel bath of Majorana fermions and present the numerically exact solution using Wilson's numerical renormalization group technique. Quantum phase transitions occur as a function of Kondo coupling and locally applied field. At zero field, the impurity moment is partially screened only when it …
