The appearance of nontrivial phases in Kitaev materials exposed to an external magnetic field has recently been a subject of intensive studies. Here, we elucidate the relation between the field-induced ground states of the classical and quantum spin models proposed for such materials, by using the infinite density matrix renormalization group (iDMRG) and the linear spin wave theory (LSWT). We consider the $K ΓΓ'$ model, where $Γ$ and $Γ'$ are off-diagonal spin exchanges on top of the dominant Kitaev interaction $K$. Focusing on the magnetic field along the $[111]$ direction, we explain the origin of the nematic paramagnet, which breaks the lattice-rotational symmetry and exists in an extended window of magnetic field, in the quantum model. This phenomenon can be understood as the effect of quantum order-by-disorder in the frustrated ferromagnet with a continuous manifold of degenerate ground states discovered in the corresponding classical model. We compute the dynamical spin structure factors using a matrix operator based time evolution and compare them with the predictions from LSWT. We, thus, provide predictions for future inelastic neutron scattering experiments on Kitaev materials in an external magnetic field along the $[111]$ direction. In particular, the nematic paramagnet exhibits a characteristic pseudo-Goldstone mode which results from the lifting of a continuous degeneracy via quantum fluctuations.
A polycrystalline sample of the hyperhoneycomb iridate $β$-ZnIrO$_3$ was synthesized via a topochemical reaction, and its structural, magnetic, and thermodynamic properties were investigated. The magnetization and heat capacity data show the absence of long-range magnetic order at least down to 2 K. A positive Curie-Weiss temperature $θ_W \sim 45$ K probed by the temperature dependence of magnetic susceptibility indicates that a Kitaev interaction is dominant. These observations suggest that a quantum spin liquid may have been realized. Furthermore, the observation of linear temperature-depend…
We study the Kitaev-Heisenberg-$Γ$-$Γ'$ model that describes the magnetism in strong spin-orbit coupled honeycomb lattice Mott insulators. In strong $[111]$ magnetic fields that bring the system into the fully polarized paramagnetic phase, we find that the spin wave bands carry nontrivial Chern numbers over large regions of the phase diagram implying the presence of chiral magnon edge states. In contrast to other topological magnon systems, the topological nontriviality of these systems results from the presence of magnon number non-conserving terms in the Hamiltonian. Since the effects of int…
We study the spin-$1/2$ ferromagnetic Heisenberg-Kitaev-$Γ$ model in the anisotropic (Toric code) limit to reveal the nature of the quantum phase transition between the gapped $Z_2$ quantum spin liquid and a spin ordered phase (driven by Heisenberg interactions) as well as a trivial paramagnet (driven by pseudo-dipolar interactions, $Γ$). The transitions are obtained by a simultaneous condensation of the Ising electric and magnetic charges-- the fractionalized excitations of the $Z_2$ quantum spin liquid. Both these transitions can be continuous and are examples of deconfined quantum critical …
Paramagnetic impurities in a quantum spin-liquid can result in Kondo effects with highly unusual properties. We have studied the effect of locally exchange-coupling a paramagnetic impurity with the spin-1/2 honeycomb Kitaev model in its gapless spin-liquid phase. The (impurity) scaling equations are found to be insensitive to the sign of the coupling. The weak and strong coupling fixed points are stable, with the latter corresponding to a noninteracting vacancy and an interacting, spin-1 defect for the antiferromagnetic and ferromagnetic cases respectively. The ground state in the strong coupl…
$α$-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.…
We show that the mesoscopic incommensurate $\mathbb{Z}_2$ vortex crystals proposed for layered triangular anisotropic magnets can be most saliently identified by two distinctive signatures in dynamical spin response experiments: The presence of pseudo-Goldstone `phonon' modes at low frequencies $ω$, associated with the collective vibrations of the vortex cores, and a characteristic multi-scattered intensity profile at higher $ω$, arising from a large number of Bragg reflections and magnon bandgaps. These are direct fingerprints of the large vortex sizes and magnetic unit cells and the solitoni…
Recent experimental evidence for a field-induced quantum spin liquid (QSL) in $α$-RuCl$_3$ calls for an understanding for the ground state of honeycomb Kitaev model under a magnetic field. In this work we address the nature of an enigmatic gapless paramagnetic phase in the antiferromagnetic Kitave model, under an intermediate magnetic field perpendicular to the plane. Combining theoretical and numerical efforts, we identify this gapless phase as a $U(1)$ QSL with spinon Fermi surfaces. We also reveal the nature of continuous quantum phase transitions involving this $U(1)$ QSL, and obtain a pha…
We study the Kitaev-Heisenberg-$Γ$ model with antiferromagnetic Kitaev exchanges in the strong anisotropic (toric code) limit to understand the phases and the intervening phase transitions between the gapped $Z_2$ quantum spin liquid and the spin-ordered (in the Heisenberg limit) as well as paramagnetic phases (in the pseudo-dipolar, $Γ$, limit). We find that the paramagnetic phase obtained in the large $Γ$ limit has no topological entanglement entropy and is proximate to a gapless critical point of a system described by an equal superposition of differently oriented stacked one-dimensional $Z…
We investigate possible topological superconductivity in the Kondo-Kitaev model on the honeycomb lattice, where the Kitaev spin liquid is coupled to conduction electrons via the Kondo coupling. We use the self-consistent Abrikosov-fermion mean-field theory to map out the phase diagram. Upon increasing the Kondo coupling, a first order transition occurs from the decoupled phase of spin liquid and conduction electrons to a ferromagnetic topological superconductor of Class D with a single chiral Majorana edge mode. This is followed by a second order transition into a paramagnetic topological supe…
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 …
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…
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…
Quantum spin liquid is an exotic quantum state of matter in magnets. This state is a spin analogue of the liquid helium which does not solidify down to the lowest temperature due to strong quantum fluctuations. In conventional fluids, liquid and gas possess the same symmetry and adiabatically connect to each other by bypassing the critical end point. We find that the situation is qualitatively different in quantum spin liquids realizing in a three-dimensional Kitaev model; both gapless and gapped quantum spin liquid phases at low temperatures are always distinguished from the high-temperature …
We present numerical evidence for the presence of a finite-temperature ($T$) phase transition separating paramagnet and quantum spin liquid in a three-dimensional variant of the Kitaev model defined on a hyperhoneycomb lattice in the limit of strong anisotropy; the model is mapped onto an effective Ising-type model, where elementary excitations consist of closed loops of flipped Ising-type variables. Analyzing this effective model by Monte Carlo simulation, we find a phase transition from quantum spin liquid to paramagnet at a finite critical temperature $T_c$. We also compute the magnetic pro…
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…
A prominent feature of quantum spin liquids is fractionalization of the spin degree of freedom. Fractionalized excitations have their own dynamics in different energy scales, and hence, affect finite-temperature ($T$) properties in a peculiar manner even in the paramagnetic state harboring the quantum spin liquid state. We here present a comprehensive theoretical study of the spin dynamics in a wide $T$ range for the Kitaev model on a honeycomb lattice, whose ground state is such a quantum spin liquid. In this model, the fractionalization occurs to break up quantum spins into itinerant matter …
We study numerically a bosonic analog of the Kitaev honeycomb model, which is a minimal model for $4d^4/5d^4$ quantum magnets with honeycomb lattice geometry. We construct its phase diagram by a combination of Landau theory analysis and quantum Monte Carlo simulations. In particular, we show that the phase boundaries between the paramagnetic state and magnetically ordered states are generically fluctuation-induced first order phase transitions. Our results are potentially applicable to Ru$^{4+}$- and Ir$^{5+}$-based honeycomb magnets.
The quantum spin liquid is an enigmatic quantum state in insulating magnets, in which conventional long-range order is suppressed by strong quantum fluctuations. Recently, an unconventional phase transition was reported between the low-temperature quantum spin liquid and the high-temperature paramagnet in the Kitaev model on a three-dimensional hyperhoneycomb lattice. Here, we show that a similar "liquid-gas" transition takes place in another three-dimensional lattice, the hyperoctagon lattice. We investigate the critical phenomena by adopting the Green-function based Monte Carlo technique wit…
In extended Kitaev models on the honeycomb lattice, off-diagonal interactions (e.g. the $Γ, Γ^{'}$ terms) give rise to non-Kitaev quantum spin liquid (QSL) and several magnetically ordered phases. In the present work, we dope holes to the system and study the resultant $t$-$K$-$Γ$-$Γ^{'}$ model by mean field theory. The interplay between the charge and spin degrees of freedom results in a rich phase diagram. Similar to doped cuprates, superconductors, pseudogap phases, fermi liquid, strange metal and paramagnetic phase are generated. What is different is that, more than one superconducting pha…
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…
Temperature evolution of the spin correlation and excitation spectrum is investigated for a Kitaev model defined on a decorated honeycomb lattice by using the quantum Monte Carlo simulation in the Majorana fermion representation. The ground state of this quantum spin model is given by two kinds of chiral spin liquids: one is topologically trivial with Abelian anyon excitations, and the other is topologically nontrivial with non-Abelian anyon excitations. While lowering temperature, the model exhibits several crossovers in the paramagnetic state, which originate from the fractionalization of qu…
Chiral spin liquids (CSLs) in three dimensions and thermal phase transitions to paramagnet are studied by unbiased Monte Carlo simulations. For an extension of the Kitaev model to a three-dimensional tricoordinate network dubbed the hypernonagon lattice, we derive low-energy effective models in two different anisotropic limits. We show that the effective interactions between the emergent $Z_2$ degrees of freedom called fluxes are unfrustrated in one limit, while highly frustrated in the other. In both cases, we find a first-order phase transition to the CSL, where both time-reversal and parity…
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…
We propose the $π$ flux triangular lattice Hubbard model ($π$-THM) as a prototypical setup to stabilize magnetically disordered quantum states of matter in the presence of charge fluctuations. The quantum paramagnetic domain of the $π$-THM which we identify for intermediate Hubbard U is framed by a Dirac semi-metal for weak coupling and by 120${}^{\circ}$ Néel order for strong coupling. Generalizing the Klein duality from spin Hamiltonians to tight-binding models, the $π$-THM maps to a Hubbard model which corresponds to the $(J_H, J_K)=(-1,2)$ Heisenberg-Kitaev model in its strong coupling lim…
We investigate the non-Abelian topological chiral spin liquid phase in the two-dimensional (2D) Kitaev honeycomb model subject to a magnetic field. By combining density matrix renormalization group (DMRG) and exact diagonalization (ED) we study the energy spectra, entanglement, topological degeneracy, and expectation values of Wilson loop operators, allowing for robust characterization. While the ferromagnetic (FM) Kitaev spin liquid is already destroyed by a weak magnetic field with Zeeman energy $H_*^\text{FM} \approx 0.02$, the antiferromagnetic (AFM) spin liquid remains robust up to a magn…
$α$-RuCl$_{3}$ is a major candidate for the realization of the Kitaev quantum spin liquid, but its zigzag antiferromagnetic order at low temperatures indicates deviations from the Kitaev model. We have quantified the spin Hamiltonian of $α$-RuCl$_{3}$ by a resonant inelastic x-ray scattering study at the Ru $L_{3}$ absorption edge. In the paramagnetic state, the quasi-elastic intensity of magnetic excitations has a broad maximum around the zone center without any local maxima at the zigzag magnetic Bragg wavevectors. This finding implies that the zigzag order is fragile and readily destabilize…
A three-dimensional Kitaev model on a hyperhoneycomb lattice is investigated numerically at finite temperature. The Kitaev model is one of the solvable quantum spin models, where the ground state is given by gapped and gapless spin liquids, depending on the anisotropy of the interactions. This model can be rewritten as a free Majorana fermion system coupled with $Z_2$ variables. The density of states of Majorana fermions shows an excitation gap in the gapped region, while it is semimetallic in the gapless region reflecting the Dirac node. Performing the Monte Carlo simulation, we calculate the…
Na2Co2TeO6 is a proposed approximate Kitaev magnet, yet its actual magnetic interactions are elusive due to a lack of knowledge on the full excitation spectrum. Here, using inelastic neutron scattering and single crystals, we determine the system's temperature-dependent magnetic excitations over the entire Brillouin zone. Without committing to specific models, we unveil a distinct signature of the third-nearest-neighbor coupling in the spin waves, which signifies the associated distance as an emerging "soft link" in the ordered state. The presence of at least six non-overlapping spin-wave bran…
Kitaev's honeycomb-lattice spin-$1/2$ model has become a paradigmatic example for $\mathbb{Z}_2$ quantum spin liquids, both gapped and gapless. Here we study the fate of these spin-liquid phases in differently stacked bilayer versions of the Kitaev model. Increasing the ratio between the inter-layer Heisenberg coupling $J_\perp$ and the intra-layer Kitaev couplings $K^{x,y,z}$ destroys the topological spin liquid in favor of a paramagnetic dimer phase. We study phase diagrams as a function of $J_\perp/K$ and Kitaev coupling anisotropies using Majorana-fermion mean-field theory, and we employ d…
We study the orbitally frustrated singlet-triplet models that emerge in the context of spin-orbit coupled Mott insulators with $t_{2g}^4$ electronic configuration. In these compounds, low-energy magnetic degrees of freedom can be cast in terms of three-flavor "triplon" operators describing the transitions between spin-orbit entangled $J=0$ ionic ground state and excited $J=1$ levels. In contrast to a conventional, flavor-isotropic O(3) singlet-triplet models, spin-orbit entangled triplon interactions are flavor-and-bond selective and thus highly frustrated. In a honeycomb lattice, we find clos…
The honeycomb Kitaev model in a magnetic field is a source of a topological quantum spin liquid with Majorana fermions and gauge flux excitations as fractional quasiparticles. We present experimental results for the thermal Hall effect of the material $α$-RuCl$_{3}$ which recently emerged as a prime candidate for realizing such physics. At temperatures above long-range magnetic ordering $T\gtrsim T_N\approx8$ K, we observe with an applied magnetic field $B$ perpendicular to the honeycomb layers a sizeable positive transversal heat conductivity $κ_{xy}$ which increases linearly with $B$. Upon r…
An effective field theory is derived that describes the quantum critical behavior of itinerant ferromagnets as the transition is approached from the ferromagnetic phase. This complements a recent study of the critical behavior on the paramagnetic side of the phase transition, and investigates the role of the ferromagnetic Goldstone modes near criticality. We find that the Goldstone modes have no direct impact on the critical behavior, and that the critical exponents are the same as determined by combining results from the paramagnetic phase with scaling arguments.
We have explored the hidden symmetries of a generic four-parameter nearest-neighbor spin model, allowed in honeycomb lattice compounds under trigonal compression. Our method utilizes a systematic algorithm to identify all dual transformations of the model that map the Hamiltonian on itself, changing the parameters and providing exact links between different points in its parameter space. We have found the complete set of points of hidden SU(2) symmetry at which seemingly highly anisotropic model can be mapped back on the Heisenberg model and inherits therefore its properties such as the presen…
The layered honeycomb iridate $α$-Li$_2$IrO$_3$ displays an incommensurate magnetic structure with counterrotating moments on nearest-neighbor sites, proposed to be stabilized by strongly-frustrated anisotropic Kitaev interactions between spin-orbit entangled Ir$^{4+}$ magnetic moments. Here we report powder inelastic neutron scattering measurements that observe sharply dispersive low-energy magnetic excitations centered at the magnetic ordering wavevector, attributed to Goldstone excitations of the incommensurate order, as well as an additional intense mode above a gap $Δ\simeq2.3$ meV. Zero-…
Recent scattering experiments in the 3D Kitaev magnet $β$-Li$_2$IrO$_3$ have shown that a relatively weak magnetic field along the crystallographic ${\bf b}$-axis drives the system from its incommensurate counter-rotating order to a correlated paramagnet, with a significant uniform `zigzag' component superimposing the magnetization along the field. Here it is shown that the zigzag order is not emerging from its linear coupling to the field (via a staggered, off-diagonal element of the ${\bf g}$-tensor), but from its intertwining with the incommensurate order and the longitudinal magnetization.…
An effective model in the isolated dimer limit of the Kitaev-type model on a decorated honeycomb lattice is investigated at finite temperature. The ground state of this model is exactly shown to be a chiral spin liquid with spontaneous breaking of time reversal symmetry. We elaborate the finite-temperature phase diagram by using the mean-field approximation and Monte Carlo simulation. We find that the phase transition between the high-temperature paramagnetic phase and the low-temperature chiral spin liquid phase is always of second order in the Monte Carlo results, although a tricritical poin…
The Sachdev-Ye-Kitaev (SYK) model provides an uncommon example of a chaotic theory that can be analysed analytically. In the deep infrared limit, the original model has an emergent conformal (reparametrisation) symmetry that is broken both spontaneously and explicitly. The explicit breaking of this symmetry comes about due to pseudo-Nambu-Goldstone modes that are not exact zero-modes of the model. In this paper, we study a version of the model which preserves the reparametrisation symmetry at all length scales. We study the heavy-light correlation functions of the operators in the conformal sp…
Chiral spin liquids (CSLs) are time-reversal symmetry breaking ground states of frustrated quantum magnets that show no long-range magnetic ordering, but instead exhibit topological order and fractional excitations. Their realization in simple and tractable microscopic models has, however, remained an open challenge for almost two decades until it was realized that Kitaev models on lattices with odd-length loops are natural hosts for such states, even in the absence of a time-reversal symmetry breaking magnetic field. Here we report on the formation of CSLs in a three-dimensional Kitaev model,…
Frustrated quantum spin systems such as the Heisenberg and Kitaev models on various lattices, have been known to exhibit various exotic properties not only at zero temperature but also for finite temperatures. Inspired by the remarkable development of the quantum frustrated spin systems in recent years, we investigate the finite-temperature properties of the $S=1/2$ Kitaev-Heisenberg models on kagome and triangular lattices by means of finite-temperature Lanczos methods with improved accuracy. In both lattices, multiple peaks are confirmed in the specific heat. To find the origin of the multip…
There have been intensive studies on Kitaev materials for the sake of the realization of exotic states such as quantum spin liquid and topological orders. In realistic materials, the Kitaev interaction may coexist with the Dzyaloshinskii-Moriya interaction (DMI), and it is a challenge to distinguish their magnitudes separately. Here, we study the topological magnon excitations and related thermal Hall conductivity of kagome magnet exhibiting Heisenberg, Kitaev and DM interactions exposed to a magnetic field. In a strong magnetic field perpendicular to the plane of the lattice ([111] direction)…
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…
Motivated by the experiments on the rare-earth double perovskites, we propose a generalized Kitaev-Heisenberg model to describe the generic interaction between the spin-orbit-entangled Kramers' doublets of the rare-earth moments. We carry out a systematic analysis of the mean-field phase diagram of this new model. In the phase diagram, there exist large regions with a continuous U(1) or O(3) degeneracy. Since no symmetry of the model protects such a continuous degeneracy, we predict that the quantum fluctuation lifts the continuous degeneracy and favors various magnetic orders in the phase dia…
The quest for Kitaev quantum spin liquids has led to great interest in honeycomb quantum magnets with strong spin-orbit coupling. It has been recently proposed that even Mott insulators with $3d$ transition metal ions, having nominally weak spin-orbit coupling, can realize such exotic physics. Motivated by this, we study the rhombohedral honeycomb cobaltates CoTiO$_3$, BaCo$_2$(PO$_4$)$_2$, and BaCo$_2$(AsO$_4$)$_2$, using $\textit{ab initio}$ density functional theory, which takes into account realistic crystal field distortions and chemical information, in conjunction with exact diagonalizat…
The honeycomb lattice iridates $A_2$IrO$_3$ ($A =$ Na, Li) are candidates for realization of the Kitaev-Heisenberg model although their proximity to Kitaev's quantum Spin-Liquid (QSL) is still debated. We report on heat capacity $C$ and entropy $S_{mag}$ for $A_2$IrO$_3$ ($A =$ Na, Li) in the temperature range $0.075~{\rm K}\leq T \leq 155$~K\@. We find a well separated two-peak structure for the magnetic heat capacity $C_{mag}$ for both materials and $S_{mag}$ for Na$_2$IrO$_3$ shows a shoulder between the peaks with a value close to ${1\over 2}$Rln$2$. These features signal the fractionaliza…
The long-sought quantum spin liquid is a quantum-entangled magnetic state leading to the fractionalization of spin degrees of freedom. Quasiparticles emergent from the fractionalization affect not only the ground state properties but also thermodynamic behavior in a peculiar manner. We here investigate how the spin dynamics evolves from the high-temperature paramagnet to the quantum spin liquid ground state, for the Kitaev spin model describing the fractionalization into itinerant matter fermions and localized $Z_2$ gauge fluxes. Beyond the previous study [J. Yoshitake, J. Nasu, and Y. Motome,…
