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.
Using quantum chemistry calculations we shed fresh light on the electronic structure and magnetic properties of RuCl3, a proposed realization of the honeycomb Kitaev spin model. It is found that the nearest-neighbor Kitaev exchange K is weaker than in 5d5 Ir oxides but still larger than other effective spin couplings. The electronic-structure computations also indicate a ferromagnetic K in the halide, which is supported by a detailed analysis of the field-dependent magnetization. From exact-diagonalization calculations for extended Kitaev-Heisenberg Hamiltonians we additionally find that a transition from zigzag order to a spin-liquid ground state can be induced in RuCl3 with external magnetic field.
Motivated by the recent experimental observation of the half-quantized thermal Hall conductivity for the candidate material of the Kitaev spin liquid, $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$ [Y. Kasahara et al., Nature 559, 227 (2018)], we investigate effects of non-Kitaev exchange interactions, which exist in the real material, on the gapped chiral spin-liquid state realized in the case with an applied magnetic field. It is found that off-diagonal exchange interactions enhance significantly the mass gap of Majorana fermions. This result provides a possible explanation for robust quantization of the thermal Hall conductivity observed in the above-mentioned experiment. Furthermore, we demonstrate that if the Kitaev spin-liquid state and the zigzag antiferromagnetic order coexist around the border of these two phases, off-diagonal exchange interactions can induce Fermi surfaces of Majorana fermions, leading to a state similar to the U(1) spin liquid.
Recent studies have brought α-RuCl_{3} to the forefront of experimental searches for materials realizing Kitaev spin-liquid physics. This material exhibits strongly anisotropic exchange interactions afforded by the spin-orbit coupling of the 4d Ru centers. We investigate the dynamical response at finite temperature and magnetic field for a realistic model of the magnetic interactions in α-RuCl_{3}. These regimes are thought to host unconventional paramagnetic states that emerge from the suppression of magnetic order. Using exact diagonalization calculations of the quantum model complemented by semiclassical analysis, we find a very rich evolution of the spin dynamics as the applied field suppresses the zigzag order and stabilizes a quantum paramagnetic state that is adiabatically connected to the fully polarized state at high fields. At finite temperature, we observe large redistributions of spectral weight that can be attributed to the anisotropic frustration of the model. These results are compared to recent experiments and provide a road map for further studies of these regimes.
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.
A Kitaev quantum spin liquid involves fractionalized quasiparticles called itinerant Majorana fermions and localized gauge fluxes. The topological character with chiral excitations under a magnetic field is currently in an active debate. For a candidate spin liquid $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$, we report low-energy spin excitations through nuclear magnetic and quadrupole resonance measurements down to temperatures three orders of magnitude lower than the exchange energy. In a field-driven disordered state, we found the evolution of two kinds of gapped spin excitations with distinct field dependences. The result is indicative of a field-induced hybridization between fractionalized quasiparticles, as inferred by the perturbation theory for the Kitaev model. The detailed field dependence of spin dynamics across the quantum critical region shows the emergence of a gapless intermediate phase between the gapped zigzag order phase and spin-disordered phases.
Abstract Elementary excitations in entangled states such as quantum spin liquids may exhibit exotic statistics different from those obeyed by fundamental bosons and fermions. Non-Abelian anyons exist in a Kitaev spin liquid—the ground state of an exactly solvable model. A smoking-gun signature of these excitations, namely a half-integer quantized thermal Hall conductivity, was recently reported in α-RuCl3. While fascinating, a microscopic theory for this phenomenon remains elusive because the pure Kitaev model cannot display this effect in an intermediate magnetic field. Here we present a microscopic theory of the Kitaev spin liquid emerging between the low- and high-field states. Essential to this result is an antiferromagnetic off-diagonal symmetric interaction which allows the Kitaev spin liquid to protrude from the ferromagnetic Kitaev limit under a magnetic field. This generic model displays a strong field anisotropy, and we predict a wide spin liquid regime when the field is perpendicular to the honeycomb plane.