It is known that α-RuCl3 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-RuCl3 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 temperature T N, the pure magnetic continuous excitations around the Γ point are robust against temperature. Furthermore, by calculating the dynamical spin-spin correlation function using the cluster perturbation theory, we derive magnetic dispersion spectra based on the K–Γ model, which involves with a ferromagnetic Kitaev interaction of –7.2 meV and an off-diagonal interaction of 5.6 meV. We find this model can reproduce not only the spin-wave excitation spectra around the M point, but also the non-spin-wave continuous magnetic excitations around the Γ point. These results provide evidence for the existence of fractional excitations around the Γ point originating from the Kitaev QSL state, and further support the validity of the K–Γ model as the effective minimal spin model to describe α-RuCl3.
We study the spin excitation spectra in magnetically ordered phases proximate to the Kitaev quantum spin liquid (KQSL). Although the low-energy universal features should be governed by the magnetic orders, the
non-universal high-energy features of the KQSL and adjacent phases can be remarkably similar. Therefore, we study the extended Kitaev model within a Stoner-like theory using Majorana partons, and compute the inelastic neutron scattering (INS) intensities in the random phase approximation. First, we benchmark against the antiferromagnetic (AFM) Heisenberg model and recover the AFM order with linear Goldstone modes. We then explore the phase diagram which agrees qualitatively with previous numerical results. In particular, the Majorana parton theory accurately captures Order-by-Disorder effects in the Kitaev-Heisenberg limit. We also find large INS intensities near the associated high-symmetry Brillouin zone (BZ) points of the magnetic orders. At intermediate and high energies, broad multi-spinon continua emerge across the BZ, providing a distinct mechanism for magnon decay and spectral broadening beyond the conventional multi-magnon decay scenario. Finally, we study the model Hamiltonian of candidate Kitaev material
α-RuCl
3. The zigzag ground state agrees qualitatively with experiments, its stability under external magnetic field also exhibits strong anisotropy in the field directions, and broad scattering continua are recovered similar to those observed experimentally.
Abstract What is the correct low-energy spin Hamiltonian description of
α α -RuCl
3 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 using a thermal pure quantum states method. We find that no single current model satisfactorily explains all observed phenomena of
α α -RuCl
3 3 . In particular, we find that Hamiltonians derived from first principles can capture the experimentally observed high-temperature peak in the magnetic specific heat, while overestimating the magnon energy at the zone center. In contrast, other models reproduce important features of the INS data, but do not adequately describe the magnetic specific heat. To address this discrepancy we propose a modified ab initio model that is consistent with both magnetic specific heat and low-energy features of INS data.
Kitaev quantum spin liquids (KQSLs) host fractionalized excitations described by itinerant Majorana quasiparticles and gapped
Z2 fluxes (visons), providing a platform for emergent topological matter. Whether such a state survives under strong magnetic fields, however, remains an open question. The layered honeycomb magnet
α-RuCl
3 is a leading candidate material: an in-plane field of
∼ 7 T suppresses antiferromagnetic order and induces a quantum-disordered phase exhibiting signatures consistent with Majorana excitations, including an anomalous thermal Hall effect and field-angle-dependent specific heat. At higher fields, the magnetization approaches saturation, suggesting a transition to a spin-polarized state, yet the microscopic evolution between these limits remains unresolved. Here we report high-field specific heat measurements up to 24 T that reveal a distinct crossover at $μ_0H^*\approx$15 T, beyond which the perturbative Kitaev description breaks down. Above
H∗, the characteristic six-fold angular modulation of the specific heat collapses and the excitation gap deviates from the predicted
H3 scaling. Meanwhile, the gap decreases with increasing field and the in-plane magnetization anisotropy persists up to
∼ 24 T, both in sharp contrast to a trivial spin-polarized state, indicating that KQSL signatures are preserved even at
∼ 90 % of magnetization saturation. These results reveal that the KQSL in
α-RuCl
3 extends well beyond the perturbative window, persisting as a nonperturbative regime in which the Majorana and vison energy scales merge, before eventually giving way to spin polarization. This thermodynamic roadmap provides a basis for understanding how fractionalized phases evolve under strong magnetic fields.
Motivated by recent synthesis of the hyperhoneycomb material $\ensuremath{\beta}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$, we study the dynamical structure factor (DSF) of the corresponding 3D Kitaev quantum spin-liquid (QSL), whose fractionalized degrees of freedom are Majorana fermions and emergent flux loops. The properties of this 3D model are known to differ in important ways from those of its 2D counterpart---it has a finite-temperature phase transition, as well as distinct features in the Raman response. We show, however, that the qualitative behavior of the DSF is broadly dimension-independent. Characteristics of the 3D DSF include a response gap even in the gapless QSL phase and an energy dependence deriving from the Majorana fermion density of states. Since the majority of the response is from states containing a single Majorana excitation, our results suggest inelastic neutron scattering as the spectroscopy of choice to illuminate the physics of Majorana fermions in Kitaev QSLs.
Abstract Large anisotropic exchange in 5 d and 4 d oxides and halides open the door to new types of magnetic ground states and excitations, inconceivable a decade ago. A prominent case is the Kitaev spin liquid, host of remarkable properties such as protection of quantum information and the emergence of Majorana fermions. Here we discuss the promise for spin-liquid behavior in the 4 d 5 honeycomb halide α -RuCl 3 . From advanced electronic-structure calculations, we find that the Kitaev interaction is ferromagnetic, as in 5 d 5 iridium honeycomb oxides, and indeed defines the largest superexchange energy scale. A ferromagnetic Kitaev coupling is also supported by a detailed analysis of the field-dependent magnetization. Using exact diagonalization and density-matrix renormalization group techniques for extended Kitaev-Heisenberg spin Hamiltonians, we find indications for a transition from zigzag order to a gapped spin liquid when applying magnetic field. Our results offer a unified picture on recent magnetic and spectroscopic measurements on this material and open new perspectives on the prospect of realizing quantum spin liquids in d 5 halides and oxides in general.