Quantum spin liquid is a disordered but highly entangled magnetic state with fractional spin excitations1. The ground state of an exactly solved Kitaev honeycomb model is perhaps its clearest example2. Under a magnetic field, a spin flip in this model fractionalizes into two types of anyon, a quasiparticle with more complex exchange statistics than standard fermions or bosons: a pair of gauge fluxes and a Majorana fermion2,3. Here, we demonstrate this kind of fractionalization in the Kitaev paramagnetic state of the honeycomb magnet α-RuCl3. The spin excitation gap determined by nuclear magnetic resonance consists of the predicted Majorana fermion contribution following the cube of the applied magnetic field2,4,5, and a finite zero-field contribution matching the predicted size of the gauge flux gap2,6. The observed fractionalization into gapped anyons survives in a broad range of temperatures and magnetic fields, which establishes α-RuCl3 as a unique platform for future investigations of anyons.
The pursuit of quantum spin liquid (QSL) in the Kitaev honeycomb magnets has drawn intensive attention recently. In particular, $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$ has been widely recognized as a promising candidate for the Kitaev QSL. Although the compound exhibits an antiferromagnetic order under zero field, it is believed to be endowed with fractionalized excitations and can be driven to the QSL phase by magnetic fields. Here, based on a realistic $K\text{\ensuremath{-}}J\text{\ensuremath{-}}\mathrm{\ensuremath{\Gamma}}\text{\ensuremath{-}}{\mathrm{\ensuremath{\Gamma}}}^{\ensuremath{'}}$ model for $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$, we exploit the exponential tensor renormalization group approach to explore the phase diagram of the compound under magnetic fields. We calculate the thermodynamic quantities, including the specific heat, Gr\"uneisen parameter, magnetic torque, magnetotropic susceptibility, and so on, under a magnetic field with a tilting angle $\ensuremath{\theta}$ to the
c∗-axis perpendicular to the honeycomb plane. We find an extended QSL in the angle-field phase diagram determined with thermodynamic responses. The gapless nature of such field-induced QSL is identified from the specific heat and entropy data computed down to very low temperatures. The present study provides guidance for future high-field experiments for the QSL in $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$ and other candidate Kitaev magnets.
Abstract Significant efforts have focused on the magnetic excitations of relativistic Mott insulators, predicted to realize the Kitaev quantum spin liquid (QSL). This exactly solvable model involves a highly entangled state resulting from bond-dependent Ising interactions that produce excitations which are non-local in terms of spin flips. A key challenge in real materials is identifying the relative size of the non-Kitaev terms and their role in the emergence or suppression of fractional excitations. Here, we identify the energy and temperature boundaries of non-Kitaev interactions by direct comparison of the Raman susceptibility of α -RuCl 3 with quantum Monte Carlo (QMC) results for the Kitaev QSL. Moreover, we further confirm the fractional nature of the magnetic excitations, which is given by creating a pair of fermionic quasiparticles. Interestingly, this fermionic response remains valid in the non-Kitaev range. Our results and focus on the use of the Raman susceptibility provide a stringent new test for future theoretical and experimental studies of QSLs.
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.
Long-range entanglement in quantum spin liquids (QSLs) leads to novel low-energy excitations with fractionalized quantum numbers and (in two dimensions) statistics. Experimental detection and manipulation of these excitations present a challenge particularly in view of diverse candidate magnets. A promising probe of fractionalization is their coupling to phonons. Here, we present Raman scattering results for the
S=1/2 honeycomb iridate
Cu2IrO3, a candidate Kitaev QSL with fractionalized Majorana fermions and Ising flux excitations. We observe anomalous low-temperature frequency shift and linewidth broadening of the Raman intensities in addition to a broad magnetic continuum, both of which, as we derive, are naturally attributed to the phonon decaying into itinerant Majoranas. The dynamic Raman susceptibility marks a crossover from the QSL to a thermal paramagnet at $\ensuremath{\sim}120$ K. The phonon anomalies below this temperature demonstrate a strong phonon-Majorana coupling. These results provide evidence of spin fractionalization in
Cu2IrO3.
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.