Abstract We present comprehensive inelastic neutron spectroscopic maps of the magnetic field-induced disordered phase of the Kitaev quantum spin liquid candidate material α-RuCl 3 . For fields along both in-plane high symmetry directions we observe that the spin excitation spectrum at and above a magnetic field of 8 T is gapped. Excitation modes then sharpen for increasing field but are consistently broader than experimental resolution even at 13.5 T. The out-of-plane dispersion diminishes in the 7-10 T regime, signifying enhanced two-dimensional behavior as the in-plane liquid correlations are established. In this regime, excitations are very broad and largely flat for all accessible energy-momenta, which is kinematically at odds with a magnon-decay picture. By contrast, a continuum of fractionalized excitations naturally yields a broad continuum response, which crucially may be accompanied by sharper modes of bound states of fractionalized excitations. Their damping by the continuum accounts for the observed spectral broadening and field dependence. Our results provide strong evidence for the existence of fractionalized excitations in α-RuCl 3 in a magnetic field.
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.
α-RuCl
3 is a leading material for proximate Kitaev magnetism. We address the origin of the broad,
Γ-point centered excitation continuum observed by inelastic neutron scattering at elevated temperatures in this compound. Using stochastic Landau-Lifshitz dynamics augmented with quantum-equivalent corrections, we reproduce the temperature-dependent dynamical spin structure factor across both the correlated and conventional paramagnetic regimes. A meta-analysis of 38 published exchange parameter sets identifies those most consistent with the full temperature evolution. A Bayesian optimization procedure is used to derive parameters that capture the low-energy star-like momentum dependence and the overall bandwidth of the continuum. Rescaling temperatures by the Curie--Weiss scale produces a collapse of spectral measures, demonstrating that the high-
T dynamics are governed by correlated paramagnetism below
θCW rather than by the Kitaev crossover to fractionalized excitations. Complementary 24-site exact diagonalization clarifies finite-size systematics at low temperature and the proximity to zigzag/incommensurate ordering. Beyond
α-RuCl
3, our simulation pipeline provides a reproducible, data-driven framework to infer effective spin models in magnets that exhibit broad continua.
Low-energy spin excitation can be anisotropic in the Kitaev spin liquid and evolve with magnetic field, as the Majorana fermions acquire the gap.In a candidate material α-RuCl 3 , the spin disordered phase appears under the in-plane magnetic field.We measure the in-plane anisotropy of spin excitation by 35 Cl nuclear magnetic resonance in α-RuCl 3 .The NMR spectrum maintains the three-fold rotational symmetry at low temperatures, as expected for the R 3 lattice.We compare the result with the numerical calculation of the 35 Cl NMR frequency as a function of magnetic field strength and direction.
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.
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.