Projective symmetry groups are applied to Raman observations of the Kitaev quantum spin liquids in spherical lattice geometries realized by Platonic and Archimedean polyhedra. Parton single excitations in Kitaev spin polyhedra are characterized by double-valued irreducible representations of their belonging projective symmetry groups, whereas parton geminate excitations relevant to Raman scattering are decomposed into single-valued irreducible representations of the corresponding point symmetry groups. We combine a standard point-symmetry-group analysis of the Loudon-Fleury vertices and an elaborate projective-symmetry-group analysis of itinerant spinons against the ground gauge fields to reveal $hidden$ $selection$ $rules$ for Raman scattering in $\mathbb{Z}_2$ spin liquids.
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…
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…
Inelastic neutron scattering of the layered Kitaev ferromagnet Li$_3$Co$_2$SbO$_6$
University of Melbourne（墨尔本大学）；Australian Nuclear Science and Technology Organisation (ANSTO)（澳大利亚核科学与技术组织）；The University of Sydney（悉尼大学）；University of Warwick（华威大学）；DESY（德国电子同步加速器研究所）
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…
Recently, Co-based honeycomb magnets have been proposed as promising candidate materials to host the Kitaev spin liquid state. One of the front-runners is BaCo$_2$(AsO$_4$)$_2$ (BCAO), where it was suggested that the exchange processes between Co$^{2+}$ ions via the surrounding edge-sharing oxygen octahedra could give rise to bond-dependent Kitaev interactions. In this work, we present and analyze comprehensive inelastic neutron scattering studies of BCAO with fields in the honeycomb plane. Combining the constraints from the magnon excitations in the high-field polarized state and the inelasti…
Cobaltates with 3$d$ based layered honeycomb structure were recently proposed as Kitaev magnets and putative candidates to host the long-sought Kitaev spin liquid. Here we present inelastic neutron scattering results down to 50 mK for powder samples of Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$, with high resolution in regions of low momentum and energy transfers. We compare the experimental data below the antiferromagnetic zigzag ordering temperature with dynamical structure factors obtained within spin wave theory. We search the wide parameter range of a $K$-$J_1$-$Γ$-$Γ^{\prime}$-$J_3$ spi…
We provide an exact study of dynamical correlations for the quantum spin-orbital liquid phases of an SU(2)-symmetric Kitaev honeycomb lattice model. We show that the spin dynamics in this Kugel-Khomskii type model is exactly the density-density correlation function of S=1 fermionic magnons, which could be probed in resonant inelastic x-ray scattering experiments. We predict the characteristic signatures of spin-orbital fractionalization in inelastic scattering experiments and compare them to the ones of the spin-anisotropic Kitaev honeycomb spin liquid. In particular, the resonant inelastic x-…
In the quest for realizations of quantum spin liquids, the exploration of Kitaev materials - spin-orbit entangled Mott insulators with strong bond-directional exchanges - has taken center stage. However, in these materials the local spin-orbital j=1/2 moments typically show long-range magnetic order at low temperature, thus defying the formation of a spin-liquid ground state. Using resonant inelastic x-ray scattering (RIXS), we here report on a proximate spin liquid regime with clear fingerprints of Kitaev physics in the magnetic excitations of the honeycomb iridates alpha-Li2IrO3 and Na2IrO3.…
Motivated by recent reports of a field-induced intermediate phase (IP) in the antiferromagnetic honeycomb Kitaev model that may be a spin liquid whose nature is distinct from the Kitaev Z2 phase, we present a detailed numerical study on the nature and dynamical response (such as dynamical spin-structure factors and resonant inelastic x-ray scattering intensities) of this field-induced IP and neighboring phases in a family of Kitaev-based models related by hidden symmetries and duality transformations. We further show that the same field-induced IP can appear in models relevant for $α$-RuCl${_3…
We have performed inelastic neutron scattering experiments to investigate the magnetic excitations in the quasi-face-centered-cubic (fcc) iridate double perovskites La2ZnIrO6 and La2MgIrO6, which are characterized by A-type antiferromagnetic ground states. The neutron scattering data, which reveal gapped spin wave excitations with a very weak dispersion, are shown to be well-described by theoretical calculations on a model Hamiltonian with dominant Kitaev interactions. Our surprising finding shows that in contrast to honeycomb materials, where the Kitaev interaction manifests itself via comple…
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 …
We present a thorough experimental study of the three-dimensional hyperhoneycomb Kitaev magnet $β$-Li$_2$IrO$_3$, using a combination of inelastic neutron scattering (INS), time-domain THz spectroscopy, and heat capacity measurements. The main results include a massive low-temperature reorganization of the INS spectral weight that evolves into a broad peak centered around 12 meV, and a distinctive peak in the THz data at 2.8(1) meV. A detailed comparison to powder-averaged spin-wave theory calculations reveals that the positions of these two features are controlled by the anisotropic $Γ$ coupl…
We introduce a matrix-product state based method to efficiently obtain dynamical response functions for two-dimensional microscopic Hamiltonians, which we apply to different phases of the Kitaev-Heisenberg model. We find significant broad high energy features beyond spin-wave theory even in the ordered phases proximate to spin liquids. This includes the phase with zig-zag order of the type observed in $α$-RuCl$_3$, where we find high energy features like those seen in inelastic neutron scattering experiments. Our results provide an example of a natural path for proximate spin liquid features t…
Perfect deporalization of the Loudon-Fleury inelastic visible-light scattering in the Kitaev honeycomb model is well known. Though it happens in Heisenberg Kagome and triangular antiferromagnets as well, yet we prove it to be of geometric origin rather than peculiar to quantum spin liquids. A Kitaev spin liquid in the square planar geometry indeed exhibits polarized Raman spectra containing defferent symmetry species, each brought by symmetry-compatible spinon geminate excitations, i.e. arising from symmetry-compatible direct-product representations made of double-valued irreducible representa…
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…
Motivated by recent synthesis of the hyper-honeycomb material $β$-$\mathrm{Li_2 Ir O_3}$, we study the dynamical structure factor (DSF) of the corresponding 3D Kitaev quantum spin-liquid (QSL), whose fractionalised degrees of freedom are Majorana fermions and emergent flux-loops. Properties of this 3D model are known to differ in important ways from those of its 2D counterpart -- it has finite-temperature phase transition, as well as distinct features in Raman response. We show, however, that the qualitative behaviour of the DSF is broadly dimension-independent. Characteristics of the 3D DSF i…
Co$^{2+}$ ions in an octahedral crystal field, stabilise a j$_{eff}$ = 1/2 ground state with an orbital degree of freedom and have been recently put forward for realising Kitaev interactions, a prediction we have tested by investigating spin dynamics in two cobalt honeycomb lattice compounds, Na$_2$Co$_2$TeO$_6$ and Na$_3$Co$_2$SbO$_6$, using inelastic neutron scattering. We used linear spin wave theory to show that the magnetic spectra can be reproduced with a spin Hamiltonian including a dominant Kitaev nearest-neighbour interaction, weaker Heisenberg interactions up to the third neighbour a…
$α$-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…
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…
We study the inelastic light scattering response in two- (2D) and three-dimensional (3D) Kitaev spin-liquid models with \ms band structures in the symmetry classes BDI and D leading to protected gapless surface modes. We present a detailed calculation of the resonant Raman/Brillouin scattering vertex relevant to iridate and ruthenate compounds whose low-energy physics is believed to be proximate to these spin-liquid phases. In the symmetry class BDI, we find that while the resonant scattering on thin films can detect the gapless boundary modes of spin liquids, the non-resonant processes do not…
Finding new materials with antiferromagnetic (AFM) Kitaev interaction is an urgent issue to broaden and enrich the quantum magnetism research significantly. By carrying out inelastic neutron scattering experiments and subsequent analysis, we conclude that Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$ are new honeycomb cobalt-based AFM Kitaev systems. The spin-orbit excitons at 20-28~meV in both compounds strongly supports the idea that Co$^{2+}$ ions of both compounds have a spin-orbital entangled $J_\rm{eff}=1/2$ state. Furthermore, we found that a generalized Kitaev-Heisenberg Hamiltonian can …
We examine recent magnetic torque measurements in two compounds, $γ$-Li$_2$IrO$_3$ and RuCl$_3$, which have been discussed as possible realizations of the Kitaev model. The analysis of the reported discontinuity in torque, as an external magnetic field is rotated across the $c-$axis in both crystals, suggests that they have a translationally-invariant chiral spin-order of the from $<{\bf S}_i. ({\bf S}_j ~\times ~ {\bf S}_k)> \ne 0$ in the ground state and persisting over a very wide range of magnetic field and temperature. An extra-ordinary $|B|B^2$ dependence of the torque for small fields, …
We investigate the magnetic excitations of the hyperhoneycomb Kitaev magnet $β$-$\text{Li}_2\text{IrO}_3$ by means of inelastic Raman scattering. The spectra exhibits a coexistence of a broad scattering continuum and two sharp low-energy peaks at 2.5 meV and 3 meV, with a distinctive polarization dependence. While the continuum is suggestive of fractional quasi-particles emerging from a proximate quantum spin liquid phase, the sharp peaks provide the first experimental signature of the `non-Loudon-Fleury' one-magnon scattering processes proposed recently [Phys. Rev. B 104, 144412 (2021)]. The …
The low energy excitations in Na2IrO3 have been investigated using resonant inelastic x-ray scattering (RIXS). A magnetic excitation branch can be resolved, whose dispersion reaches a maximum energy of about 35 meV at the Γ-point. The momentum dependence of the excitation energy is much larger along the Γ-X direction compared to that along the Γ-Y direction. The observed dispersion relation is consistent with a recent theoretical prediction based on Heisenberg-Kitaev model. At high temperatures, we find large contributions from lattice vibrational modes to our RIXS spectra, suggesting that a s…
We analyse the dynamical response of a range of 3D Kitaev quantum spin-liquids, using lattice models chosen to explore the different possible low-energy spectra for gapless Majorana fermions, with either Fermi surfaces, nodal lines or Weyl points. We find that the behaviour of the dynamical structure factor is distinct in all three cases, reflecting the quasiparticle density of states in two fundamentally different ways. First, the low-energy response is either straightforwardly related to the power with which the low-energy density of states vanishes; or for a non-vanishing density of states,…
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 ori…
Inelastic light scattering studies on single crystals of (Na$_{1-x}$Li$_x$)$_2$IrO$_3$ ($x = 0, 0.05$ and $0.15$) show a polarization independent broad band at $\sim $~2750 cm$^{-1}$ with a large band-width $\sim 1800$~cm$^{-1}$. For Na$_2$IrO$_3$ the broad band is seen for temperatures $ \leq 200$~K and persists inside the magnetically ordered state. For Li doped samples, the intensity of this mode increases, shifts to lower wave-numbers and persists to higher temperatures. Such a mode has recently been predicted (Knolle et.al.) as a signature of the Kitaev spin liquid. We assign the observat…
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…
Quantum magnets with significant bond-directional Ising interactions, so-called Kitaev materials, have attracted tremendous attention recently in the search for exotic spin liquid states. Here we present a comprehensive set of measurements that enables us to investigate the crystal structures, Ir$^{4+}$ single ion properties, and magnetic ground states of the double perovskite iridates La$_2B$IrO$_6$ ($B$ $=$ Mg, Zn) and $A_2$CeIrO$_6$ ($A$ $=$ Ba, Sr) with a large nearest neighbor distance $>$ 5 Angstroms between Ir$^{4+}$ ions. Our neutron powder diffraction data on Ba$_2$CeIrO$_6$ can be re…
We calculate the dynamical spin structure factor of the generalized spin-$1/2$ compass spin chain using the density matrix renormalization group. The model, also known as the twisted Kitaev spin chain, was recently proposed to be relevant for the description of the spin chain compound CoNb$_2$O$_6$. It features bond-dependent interactions and interpolates between an Ising chain and a one-dimensional variant of Kitaev's honeycomb spin model. The structure factor, in turn, is found to interpolate from gapped and non-dispersive in the Ising limit to gapless with non-trivial continua in the Kitaev…
Proximate quantum spin liquids and Majorana continua in magnetically ordered Kitaev magnets
Technical University of Munich（慕尼黑工业大学）；Max Planck Institute for the Physics of Complex Systems（马克斯·普朗克复杂系统物理研究所）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与工程中心）
Kitaev interactions in the van der Waals antiferromagnet VBr3
Fudan University（复旦大学）；J-PARC Center（日本原子力研究开发机构J-PARC中心）；Shanghai Research Center for Quantum Sciences（上海量子科学研究中心）；Institute of Nanoelectronics and Quantum Computing, Fudan University（复旦大学纳米电子与量子计算研究所）
研究通过非弹性中子散射揭示了van der Waals反铁磁体VBr3中的Kitaev相互作用，并表明配体工程可调节Kitaev相互作用。
The honeycomb magnet $α-$RuCl$_3$ is a prime candidate material for realizing the Kitaev quantum spin liquid (QSL), but it shows long-range magnetic order at low temperature. Nevertheless, its broad inelastic neutron scattering (INS) response at finite frequency has been interpreted as that of a 'proximate QSL'. A moderate in-plane magnetic field indeed melts the residual zigzag order, giving rise to peculiar intermediate field phases before the high-field polarized state. In INS measurements the low-frequency spin waves disappear, leading to a broad scattering continuum in the field-induced i…
Magnetoelastic interaction couples spin and lattice degrees of freedom and plays a key role in thermal transport properties of magnetic insulators. In the Kitaev quantum spin liquid, the low energy excitations are charge neutral Majorana fermions, which transform the magnetoelasctic interaction into Majorana-phonon scattering. Motivated by anomalous thermal properties of the Kitaev quantum spin liquid candidate RuCl$_3$, in this letter, we combine meV resolution inelastic x-ray scattering and theoretical calculation to examine the Majorana-phonon scattering. We analytically derive the velocity…
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-…
Spin-orbit coupling locks spin direction and spatial orientation and generates, in semi-classical magnets, a local spin easy-axis and associated ordering. Quantum spin-1/2's defy this fate: rather than spins becoming locally anisotropic, the spin-spin interactions do. Consequently interactions become dependent on the spatial orientation of bonds between spins, prime theoretical examples of which are Kitaev magnets. Bond-directional interactions imply the existence of bond-directional magnetic modes, predicted spin excitations that render crystallographically equivalent bonds magnetically inequ…
We have performed inelastic neutron scattering (INS) experiments to investigate the magnetic excitations in the weakly distorted face-centered-cubic (fcc) iridate double perovskites La$_2$ZnIrO$_6$ and La$_2$MgIrO$_6$, which are characterized by A-type antiferromagnetic ground states. The powder inelastic neutron scattering data on these geometrically frustrated $j_{\rm eff}=1/2$ Mott insulators provide clear evidence for gapped spin wave excitations with very weak dispersion. The INS results and thermodynamic data on these materials can be reproduced by conventional Heisenberg-Ising models wi…
We consider an exact solvable interacting spinful Kitaev chain which is a generalization of the Mattis-Nam model. A nearest-neighbor dimerized interaction favoring the production of disjoint molecules drives the quantum phase into an insulating one. The phases are characterized statically and dynamically in terms of magnetization and spin-singlet correlations by using the exact solution. The model is shown to be exactly solvable also in the presence of boundary interactions which are originated from a spin-singlet superconducting pairing and a magnetic field. We exploit the exact solution to i…
The family of edge-sharing tri-coordinated iridates and ruthenates has emerged in recent years as a major platform for Kitaev spin liquid physics, where spins fractionalize into emergent magnetic fluxes and Majorana fermions with Dirac-like dispersions. While such exotic states are usually pre-empted by long-range magnetic order at low temperatures, signatures of Majorana fermions with long coherent times have been predicted to manifest at intermediate and higher energy scales, similar to the observation of spinons in quasi-1D spin chains. Here we present a Resonant Inelastic X-ray Scattering …
Kitaev interactions underlying a quantum spin liquid have been long sought, but experimental data from which their strengths can be determined directly is still lacking. Here, by carrying out inelastic neutron scattering measurements on high-quality single crystals of $α$-RuCl$_3$, we observe spin-wave spectra with a gap of $\sim$2 meV around the M point of the two-dimensional Brillouin zone. We derive an effective-spin model in the strong-coupling limit based on energy bands obtained from first-principle calculations, and find that the anisotropic Kitaev interaction $K$ term and the isotropic…
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 zig-zag magnetic order. The onset of long-range magnetic order below 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…
Despite the exciting implications of the Kitaev spin-Hamiltonian, finding and confirming the quantum spin liquid state has proven incredibly difficult. Recently the applicability of the model has been expanded through the development of a microscopic description of a spin-1 Kitaev interaction. Here we explore a candidate spin-1 honeycomb system, KNiAsO$_4$ , which meets many of the proposed criteria to generate such an interaction. Bulk measurements reveal an antiferromagnetic transition at $\sim$ 19 K which is generally robust to applied magnetic fields. Neutron diffraction measurements show …
We use an exact numerical diagonalization method to calculate the dynamical spin structure factors (DSFs) of three ab-initio models and one ab-initio-guided model for a honeycomb-lattice magnet $α$-RuCl$_3$. We also use thermal pure quantum states to calculate the temperature dependence of the heat capacity, the nearest-neighbor (NN) spin-spin correlation function, and the static spin structure factor. From the results obtained from these four effective models, we find that, even when the magnetic order is stabilized at low temperature, the intensity at the $Γ$ point in the DSFs increases with…
