Kitaev Spin Model Research Articles

Finite-momentum energy dynamics in a Kitaev magnet

We study the energy-density dynamics at finite momentum of the two-dimensional Kitaev spin-model on the honeycomb lattice. Due to fractionalization of magnetic moments, the energy relaxation occurs through mobile Majorana matter, coupled to a static $\mathbb{Z}_2$ gauge field. At finite temperatures, the $\mathbb{Z}_2$ flux excitations act as an emergent disorder, which strongly affects the energy dynamics. We show that sufficiently far above the flux proliferation temperature, but not yet in the classical regime, gauge disorder modifies the coherent low-temperature energy-density dynamics into a form which is almost diffusive, with hydrodynamic momentum scaling of a diffusion-kernel, which however remains retarded, primarily due to the presence of two distinct relaxation channels of particle-hole and particle-particle nature. Relations to thermal conductivity are clarified. Our analysis is based on complementary calculations in the low-temperature homogeneous gauge and a mean-field treatment of thermal gauge fluctuations, valid at intermediate and high temperatures.

Temperature evolution of the phonon dynamics in the Kitaev spin liquid

Here we present a study of the phonon dynamics in the honeycomb Kitaev spin model at finite temperatures. We show that the fractionalized spin excitations of the Kitaev spin liquid, the itinerant Majorana fermions, and static ${Z}_{2}$ fluxes have distinct effects on the phonon dynamics, which makes the phonon dynamics a promising tool for exploring the Kitaev spin liquid candidate materials. In particular, we focus on the signature of the fractionalized excitations in the thermodynamic behavior of the sound attenuation and the phonon Hall viscosity: the former describes the phonon decay into the fractionalized excitations, and the latter is the leading order time-reversal symmetry breaking effect on the acoustic phonon. We find that the angular dependence of the attenuation coefficient and its magnitude is modified by the thermal excitation of the ${Z}_{2}$ fluxes. The strength of this effect strongly depends on the relative magnitude of the sound velocity and the Fermi velocity characterizing the low-energy Majorana fermions. We also show that the Hall viscosity is strongly suppressed by the increase of the density of the ${Z}_{2}$ fluxes at finite temperatures. All these observations reflect the effects of the emergent disorder on the Majorana fermions introduced by the ${Z}_{2}$ fluxes. Our analysis is based on the complementary analytical calculations in the low-temperature zero-flux sector, and numerical calculations in the inhomogeneous flux sectors at intermediate and high temperatures with stratified Monte Carlo (strMC) method.

Computational design of f -electron Kitaev magnets: Honeycomb and hyperhoneycomb compounds A2PrO3 ( A= alkali metals)

The Kitaev spin model offers an exact quantum spin liquid in the ground state, which has stimulated exploration of its material realization over the last decade. Thus far, most of the candidates are found in $4d$- and $5d$-electron compounds, in which the low-spin $d^5$ electron configuration subject to strong spin-orbit coupling comprises a Kramers doublet with the effective angular momentum $j_{\rm eff}=1/2$ and gives rise to the bond-dependent anisotropic interactions in the Kitaev model. Here we theoretically investigate other candidates in $4f$-electron compounds with the $f^1$ electron configuration on both quasi-two-dimensional honeycomb and three-dimensional hyperhoneycomb structures, $A_2$PrO$_3$ with $A$=Li, Na, K, Rb, and Cs. Based on {\it ab initio} calculations, we show that the electronic structures of these compounds host a spin-orbital entangled Kramers doublet with $j_{\rm eff}=1/2$ in the $\Gamma_7$ state. By constructing the tight-binding Hamiltonian and performing a perturbation expansion, we find that the low-energy magnetic properties of $A_2$PrO$_3$ are well described by an effective spin model with the $J$-$K$-$\Gamma'$ model. The most remarkable feature is that the Kitaev interaction $K$ is antiferromagnetic, in contrast to the ferromagnetic one in the $d^5$ candidates at hand. The exchange interactions are systematically modulated by changing the $A$-site cations. As a consequence, the compounds with $A$=Li and Na may have a dominant antiferromagnetic $K$, but $J$ dominates $K$ and $\Gamma'$ in the cases with $A$=Rb and Cs. Also, by computing the ground states of the $J$-$K$-$\Gamma'$ model by using the exact diagonalization, we map out the systematic evolution of the model parameters in the phase diagram. Our results will stimulate material exploration of the antiferromagnetic Kitaev interaction in $f$-electron compounds.

Defect production and quench dynamics in the three-dimensional Kitaev model

We study the quench dynamics of the three-dimensional Kitaev (spin) model under a linear drive using both exact numerical calculations and analytical "independent crossing approximation". Unlike the two-dimensional Kitaev model, the three-dimensional Kitaev model reduces to a multilevel Landau-Zener problem for each momentum. We show that for the slow quench, the defect density is proportional to the quench rate $1/\tau$. We find that the zeros of the relevant coupling between the levels determine the non-adiabatic condition for the production of defects. The contour on which the energy spectrum becomes gapless does not play an active role. The asymptotic behavior of the defect density crucially depends on the way the system reaches the non-adiabatic regime during the quenching process. We analytically show that defect correlation varies as $\tau^{-1} e^{-A/\tau}$, where $A$ is a constant independent of $\tau$. For the slow quench, the qualitative dependence of the entropy (produced during the quenching process) on the quench time is the same as that of the defect correlation, indicating a close connection between the defect correlation and the entropy content of the final state. Possible experimental realization of such quench dynamics is also described briefly.

Materials design of Kitaev spin liquids beyond the Jackeli–Khaliullin mechanism

The Kitaev spin liquid provides a rare example of well-established quantum spin liquids in more than one dimension. It is obtained as the exact ground state of the Kitaev spin model with bond-dependent anisotropic interactions. The peculiar interactions can be yielded by the synergy of spin-orbit coupling and electron correlations for specific electron configuration and lattice geometry, which is known as the Jackeli–Khaliullin mechanism. Based on this mechanism, there has been a fierce race for the materialization of the Kitaev spin liquid over the last decade, but the candidates have been still limited mostly to 4d- and 5d-electron compounds including cations with the low-spin d5 electron configuration, such as Ir4+ and Ru3+. Here we discuss recent efforts to extend the material perspective beyond the Jackeli–Khaliullin mechanism, by carefully reexamining the two requisites, formation of the jeff = 1/2 doublet and quantum interference between the exchange processes, for not only d- but also f-electron systems. We present three examples: the systems including Co2+ and Ni3+ with the high-spin d7 electron configuration, Pr4+ with the f1-electron configuration, and polar asymmetry in the lattice structure. In particular, the latter two are intriguing since they may realize the antiferromagnetic Kitaev interactions, in contrast to the ferromagnetic ones in the existing candidates. This partial overview would stimulate further material exploration of the Kitaev spin liquids and its topological properties due to fractional excitations.

Phonon renormalization in the Kitaev quantum spin liquid

We study the self-energy of phonons, magnetoelastically coupled to the two-dimensional Kitaev spin-model on the honeycomb lattice. Fractionalization of magnetic moments into mobile Majorana matter and a static $\mathbb{Z}_{2}$ gauge field lead to a continuum of relaxation processes comprising two channels. Thermal flux excitations, which act as an emergent disorder, strongly affect the phonon renormalization. Above the flux proliferation temperature, the dispersion of a narrow quasiparticle-hole channel is suppressed in favor of broad and only weakly momentum dependent features, covering large spectral ranges. Our analysis is based on complementary calculations in the low-temperature homogeneous gauge and a mean-field treatment of thermal gauge fluctuations, valid at intermediate and high temperatures.

Valence bond fluctuations in the Kitaev spin model

We introduce valence bond fluctuations, or bipartite fluctuations associated to bond-bond correlation functions, to characterize quantum spin liquids and their entanglement properties. Using analytical and numerical approaches, we find an identical scaling law between valence bond fluctuations and entanglement entropy in the two-dimensional Kitaev spin model and in one-dimensional chain analogues. We also show how these valence bond fluctuations can locate quantum phase transitions between the three gapped and the gapless Majorana semi-metal phases in the honeycomb model. We then study the effect of a uniform magnetic field along the 111 direction opening a gap in the intermediate phase which becomes topological. We still obtain a robust signal to characterize the transitions towards the three gapped phases. The linear scaling behavior of such bipartite fluctuations in two dimensions is also distinguishable from the one in the Neel magnetic state.

Highly frustrated magnetism in relativistic d4 Mott insulators: Bosonic analog of the Kitaev honeycomb model

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 close analogies with the Kitaev spin model---an infinite number of conserved quantities, no magnetic condensation, and spin correlations being strictly short-ranged. However, due to the bosonic nature of triplons, there are no emergent gapless excitations within the spin gap, and the ground state is a strongly correlated paramagnet of dense triplon pairs with no long-range entanglement. Using exact diagonalization, we study the bosonic Kitaev model and its various extensions, which break exact symmetries of the model and allow magnetic condensation of triplons. Possible implications for magnetism of ruthenium oxides are discussed.

Nonequilibrium Majorana dynamics by quenching a magnetic field in Kitaev spin liquids

The honeycomb Kitaev spin model provides a quantum spin liquid in the ground state, where the spin excitations are fractionalized into itinerant and localized Majorana fermions; the former spectrum has a broad continuum ranging up to a high energy, while the latter has a sharp peak at a low energy. Despite tremendous efforts, it remains elusive to clearly identify these distinct Majorana excitations in experiments. Here we show their manifestation in the time evolution after quenching the magnetic field, by using the time-dependent Majorana mean-field theory for both the ferromagnetic and antiferromagnetic Kitaev models. We find that the transient spin dynamics from the quantum spin liquid states is qualitatively different from the conventional spin precessions by the quench from the high-field forced-ferromagnetic state. We obtain peculiar time evolutions with distinct time scales, i.e., short-time decay of high-energy components associated with the itinerant Majorana excitations, and long-lived excitations at a low energy by the localized ones. These peculiar behaviors are caused by the energy transfer between the two Majorana quasiparticles after the field quench. Moreover, we find that the Majorana semimetal with the point nodes in equilibrium turns into a Majorana metal with the transient "Fermi surfaces" by the energy transfer. In particular, for the quench from the intermediate-field quantum spin liquid in the antiferromagnetic Kitaev model, the Fermi surfaces change their topology in the time evolution, which is regarded as a dynamical version of the Majorana "Lifshitz transition". Our results unveil that the real-time dynamics provides another route to not only the identification of the fractional Majorana excitations in candidate materials of Kitaev magnets but also unprecedented quantum phases that cannot be stabilized as the equilibrium states.

Topology and localization of a periodically driven Kitaev model

Periodically driven quantum many-body systems support anomalous topological phases of matter, which cannot be realized by static systems. In many cases, these anomalous phases can be many-body localized, which implies that they are stable and do not heat up as a result of the driving. What types of anomalous topological phenomena can be stabilized in driven systems, and in particular, can an anomalous phase exhibiting non-Abelian anyons be stabilized? We address this question using an exactly solvable, stroboscopically driven 2D Kitaev spin model, in which anisotropic exchange couplings are boosted at consecutive time intervals. The model shows a rich phase diagram which contains anomalous topological phases. We characterize these phases using weak and strong scattering-matrix invariants defined for the fermionic degrees of freedom. Of particular importance is an anomalous phase whose zero flux sector exhibits fermionic bands with zero Chern numbers, while a vortex binds a pair of Majorana modes, which as we show support non-Abelian braiding statistics. We further show that upon adding disorder, the zero flux sector of the model becomes localized. However, the model does not remain localized for a finite density of vortices. Hybridization of Majorana modes bound to vortices form ``vortex bands,'' which delocalize by either forming Chern bands or a thermal metal phase. We conclude that while the model cannot be many-body localized, it may still exhibit long thermalization times, owing to the necessity to create a finite density of vortices for delocalization to occur.

Heat transport in the anisotropic Kitaev spin liquid

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 emergent thermal gauge disorder on any finite system, we find that in the thermodynamic limit, gapless and gapful phases both feature normal dissipative transport, with a temperature dependence crossing over from power law to exponentially activated behavior upon gap opening.

Thermal transport in a two-dimensional Z2 spin liquid

We study the dynamical thermal conductivity of the two-dimensional Kitaev spin-model on the honeycomb lattice. We find a strongly temperature dependent low-frequency spectral intensity as a direct consequence of fractionalization of spins into mobile Majorana matter and a static $\mathbb{Z}_{2}$ gauge field. The latter acts as an emergent thermally activated disorder, leading to the appearance of a pseudogap which partially closes in the thermodynamic limit, indicating a dissipative heat conductor. Our analysis is based on complementary calculations of the current correlation function, comprising exact diagonalization by means of a complete summation over all gauge sectors, as well as a phenomenological mean-field treatment of thermal gauge fluctuations, valid at intermediate and high temperatures. The results will also be contrasted against the conductivity discarding gauge fluctuations.

Temperature evolution of spin dynamics in two- and three-dimensional Kitaev models: Influence of fluctuating Z2 flux

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, Phys. Rev. Lett. $\textbf{117}$, 157203 (2016)], in which the mean-field nature of the cluster dynamical mean-field theory prevented us from studying low-temperature properties, we develop a numerical technique by applying the continuous-time quantum Monte Carlo (CTQMC) method to statistical samples generated by the quantum Monte Carlo (QMC) method in a Majorana fermion representation. This QMC+CTQMC method is fully unbiased and enables us to investigate the low-temperature spin dynamics dominated by thermally excited gauge fluxes, including the unconventional phase transition caused by gauge flux loops in three dimensions, which was unreachable by the previous methods. We apply this technique to the Kitaev model in both two and three dimensions. Our results clearly distinguish two cases: while the dynamics changes smoothly through the crossover in the two-dimensional honeycomb case, it exhibits singular behaviors at the phase transition in the three-dimensional hyperhoneycomb case. We show that the low-temperature spin dynamics is a sensitive probe for thermally fluctuating gauge fluxes that behave very differently between two and three dimensions.

Thermal transport in a one-dimensional Z2 spin liquid

We study the dynamical thermal conductivity of the Kitaev spin model on a two-leg ladder. In contrast to conventional integrable one-dimensional spin systems, we show that heat transport is completely dissipative. This is a direct consequence of fractionalization of spins into mobile Majorana matter and a static $Z_{2}$ gauge field, which acts as an emergent thermally activated disorder. Our finding rests on three complementary calculations of the current correlation function, comprising a phenomenological mean-field treatment of thermal gauge fluctuations, a complete summation over all gauge sectors, as well as exact diagonalization of the original spin model. The results will also be contrasted against the conductivity discarding gauge fluctuations.

Neutron scattering in the proximate quantum spin liquid α-RuCl3.

The Kitaev quantum spin liquid (KQSL) is an exotic emergent state of matter exhibiting Majorana fermion and gauge flux excitations. The magnetic insulator α-RuCl3 is thought to realize a proximate KQSL. We used neutron scattering on single crystals of α-RuCl3 to reconstruct dynamical correlations in energy-momentum space. We discovered highly unusual signals, including a column of scattering over a large energy interval around the Brillouin zone center, which is very stable with temperature. This finding is consistent with scattering from the Majorana excitations of a KQSL. Other, more delicate experimental features can be transparently associated with perturbations to an ideal model. Our results encourage further study of this prototypical material and may open a window into investigating emergent magnetic Majorana fermions in correlated materials.

Monoclinic crystal structure ofα−RuCl3and the zigzag antiferromagnetic ground state

The layered honeycomb magnet alpha-RuCl3 has been proposed as a candidate to realize a Kitaev spin model with strongly frustrated, bond-dependent, anisotropic interactions between spin-orbit entangled jeff=1/2 Ru4+ magnetic moments. Here we report a detailed study of the three-dimensional crystal structure using x-ray diffraction on untwinned crystals combined with structural relaxation calculations. We consider several models for the stacking of honeycomb layers and find evidence for a crystal structure with a monoclinic unit cell corresponding to a stacking of layers with a unidirectional in-plane offset, with occasional in-plane sliding stacking faults, in contrast with the currently-assumed trigonal 3-layer stacking periodicity. We report electronic band structure calculations for the monoclinic structure, which find support for the applicability of the jeff=1/2 picture once spin orbit coupling and electron correlations are included. We propose that differences in the magnitude of anisotropic exchange along symmetry inequivalent bonds in the monoclinic cell could provide a natural mechanism to explain the spin gap observed in powder inelastic neutron scattering, in contrast to spin models based on the three-fold symmetric trigonal structure, which predict a gapless spectrum within linear spin wave theory. Our susceptibility measurements on both powders and stacked crystals, as well as neutron powder diffraction show a single magnetic transition at TN ~ 13K. The analysis of the neutron data provides evidence for zigzag magnetic order in the honeycomb layers with an antiferromagnetic stacking between layers. Magnetization measurements on stacked single crystals in pulsed field up to 60T show a single transition around 8T for in-plane fields followed by a gradual, asymptotic approach to magnetization saturation, as characteristic of strongly anisotropic exchange interactions.

Theory of Raman response in three-dimensional Kitaev spin liquids: Application toβ- andγ−Li2IrO3compounds

We calculate the Raman response for the Kitaev spin model on the $\mathcal{H}$-$0$, $\mathcal{H}$-$1$, and $\mathcal{H}$-$\infty$ harmonic honeycomb lattices. We identify several quantitative features in the Raman spectrum that are characteristic of the spin liquid phase. Unlike the dynamical structure factor, which probes both the Majorana spinons and flux excitations that emerge from spin fractionalization, the Raman spectrum in the Kitaev models directly probes a density of states of pairs of fractional, dispersing Majorana spinons. As a consequence, the Raman spectrum in all these models is gapless for sufficiently isotropic couplings, with a low-energy power law that results from the Fermi lines (or points) of the dispersing Majorana spinons. We show that the polarization dependence of the Raman spectrum contains crucial information about the symmetry of the ground state. We also discuss to what extent the features of the Raman response that we find reflect generic properties of the spin liquid phase, and comment on their possible relevance to $\alpha-$, $\beta-$ and $\gamma-$Li$_2$IrO$_3$ compounds.

Exact chiral spin liquids and mean-field perturbations of gamma matrix models on the ruby lattice

We theoretically studied an exactly solvable gamma matrix generalization of the Kitaev spin model on the ruby lattice, which is a honeycomb lattice with ‘expanded’ vertices and links. We find that this model displays an exceptionally rich phase diagram that includes (i) gapless phases with stable spin Fermi surfaces, (ii) gapless phases with low-energy Dirac cones and quadratic band touching points and (iii) gapped phases with finite Chern numbers possessing the values ±4,±3,±2 and ±1. The model is then generalized to include Ising-like interactions that break the exact solvability of the model in a controlled manner. When these terms are dominant, they lead to a trivial Ising ordered phase which is shown to be adiabatically connected to a large coupling limit of the exactly solvable phase. In the limit where these interactions are weak, we treat them within mean-field theory and present the resulting phase diagrams. We discuss the nature of the transitions between various phases. Our results show the richness of possible ground states in closely related magnetic systems.

Spin Waves and Revised Crystal Structure of Honeycomb IridateNa2IrO3

We report inelastic neutron scattering measurements on Na2IrO3, a candidate for the Kitaev spin model on the honeycomb lattice. We observe spin-wave excitations below 5 meV with a dispersion that can be accounted for by including substantial further-neighbor exchanges that stabilize zigzag magnetic order. The onset of long-range magnetic order below T(N)=15.3 K is confirmed via the observation of oscillations in zero-field muon-spin rotation experiments. Combining single-crystal diffraction and density functional calculations we propose a revised crystal structure model with significant departures from the ideal 90° Ir-O-Ir bonds required for dominant Kitaev exchange.

Exotic phase diagram of a topological quantum system

We study the quantum phase transitions (QPTs) in the Kitaev spin model on a triangle-honeycomb lattice. In addition to the ordinary topological QPTs between Abelian and non-Abelian phases, we find new QPTs which can occur between two phases belonging to the same topological class, namely, either two non-Abelian phases with the same Chern number or two Abelian phases with the same Chern number. Such QPTs result from the singular behaviors of the nonlocal spin-spin correlation functions at the critical points.