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.
The Kitaev model on a honeycomb lattice with bond-dependent Ising interactions offers an exactly solvable model of a quantum spin liquid (QSL) with fractionalized excitations: gapped
Z2 fluxes and gapless linearly dispersing Majorana fermions in the isotropic limit (
Kx=Ky=Kz). We explore the phase diagram along two axes, an external magnetic field
h, applied out of plane of the honeycomb, and anisotropic interactions
Kz larger than the other two (${K}_{x}={K}_{y}\ensuremath{\equiv}K$). For ${K}_{z}/K\ensuremath{\gg}2$ and
h=0, the matter Majorana fermions have the largest gap, and the system is described by a gapped
Z2 toric code. One of the central questions we address is whether the fractionalized excitations in the different phases have sharp signatures that can be detected in experiments. We show that while the response to single-spin excitations is broad, the spectral function corresponding to two-spin excitations across a bond has sharp signatures that can be attributed to specific anyons. In the toric code regime, the $\ensuremath{\epsilon}=e\ifmmode\times\else\texttimes\fi{}m$ fermion, formed from the bosonic Ising electric (
e) and magnetic (
m) charges, disperses along a specific one-dimensional direction that provides a fingerprint of fractionalization. At lower
Kz in the center of the Abelian phase, in a regime we dub the primordial fractionalized regime, the field generates a hybridization between the $\ensuremath{\epsilon}$ fermion and the Majorana matter fermion, resulting in a $\ensuremath{\psi}$ fermion which too has a distinct quasi-one-dimensional dispersion. All the other phases in the field-anisotropy plane are naturally obtained from this primordial soup. These highly constrained fractonlike dispersions can be observable by inelastic light and neutron scattering, thereby providing ``smoking gun'' signatures of fractionalization in the QSL phase. Our analysis is based on calculations of susceptibilities, topological entanglement entropy, and excitation dynamics, obtained using exact diagonalization and density matrix renormalization group, and supported by perturbation theory.
A prominent feature of quantum spin liquids is fractionalization of the spin degree of freedom. Fractionalized excitations have their own dynamics in different energy scales, and hence, affect finite-temperature (
T) properties in a peculiar manner even in the paramagnetic state harboring the quantum spin liquid state. We here present a comprehensive theoretical study of the spin dynamics in a wide
T range for the Kitaev model on a honeycomb lattice, whose ground state is a quantum spin liquid. In this model, the fractionalization occurs to break up quantum spins into itinerant matter fermions and localized
Z2 fluxes, which results in two crossovers at very different
T scales. Extending the previous study for the isotropic coupling case [J. Yoshitake, J. Nasu, and Y. Motome, Phys. Rev. Lett. 117, 157203 (2016)], we calculate the dynamical spin structure factor $S(\mathbf{q},\ensuremath{\omega})$, the NMR relaxation rate
1/T1, and the magnetic susceptibility $\ensuremath{\chi}$ while changing the anisotropy in the exchange coupling constants, by using the dynamical mean-field theory based on a Majorana fermion representation. We describe the details of the methodology including the continuous-time quantum Monte Carlo method for computing dynamical spin correlations and the maximum entropy method for analytic continuation. We confirm that the combined method provides accurate results in a wide
T range including the region where the spins are fractionalized. We find that also in the anisotropic cases the system exhibits peculiar behaviors below the high-
T crossover whose temperature is comparable to the average of the exchange constants: $S(\mathbf{q},\ensuremath{\omega})$ shows an inelastic response at the energy scale of the averaged exchange constant,
1/T1 continues to grow even though the equal-time spin correlations are saturated and almost
T independent, and $\ensuremath{\chi}$ deviates from the Curie-Weiss behavior. In particular, when the exchange interaction in one direction is stronger than the other two, the dynamical quantities exhibit qualitatively different
T dependences from the isotropic case at low
T, reflecting the opposite parity between the flux-free ground state and the flux-excited state, and a larger energy cost for flipping a spin in the strong interaction direction. On the other hand, when the exchange anisotropy is in the opposite way, the results are qualitatively similar to those in the isotropic case. All these behaviors manifest the spin fractionalization in the paramagnetic region. Among them, the dichotomy between the static and dynamical spin correlations is unusual behavior hardly seen in conventional magnets. We discuss the relation between the dichotomy and the spatial configuration of the
Z2 gauge fields. Our results could stimulate further experimental and theoretical analyses of candidate materials for the Kitaev quantum spin liquids.
In Kitaev spin liquids,
S = \textonehalf{} quantum spins on a honeycomb lattice with bond-dependent interactions fractionalize into Majorana fermions. Fingerprints of these fractionalized excitations can be detected via thermodynamic measurements. Here, the authors perform detailed heat capacity experiments on the spin-liquid candidate $\ensuremath{\alpha}$-RuCl
3 as function of temperature and magnetic field. To estimate the intrinsic phonon contribution, they measure the nonmagnetic reference compound RhCl
3 and perform $a\phantom{\rule{0}{0ex}}b$ $i\phantom{\rule{0}{0ex}}n\phantom{\rule{0}{0ex}}i\phantom{\rule{0}{0ex}}t\phantom{\rule{0}{0ex}}i\phantom{\rule{0}{0ex}}o$ phonon calculations. Measurements and analysis provide experimental evidence of fractionalized excitations in good agreement with theoretical predictions.
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.
Temperature evolution of the spin correlation and excitation spectrum is investigated for the Kitaev model defined on a decorated honeycomb lattice by using the quantum Monte Carlo simulation in the Majorana fermion representation. The ground state of this quantum spin model is given by two kinds of chiral spin liquids: one is topologically trivial with Abelian anyon excitations, and the other is topologically nontrivial with non-Abelian anyon excitations. While lowering temperature, the model exhibits several crossovers in the paramagnetic state, which originate from the fractionalization of quantum spins into Majorana fermions, in addition to a phase transition associated with time reversal symmetry breaking. We show that the spin correlation develops around the crossover temperatures, whereas it shows a slight change at the critical temperature, as in other Kitaev-type models. We also calculate the excitation spectrum in terms of Majorana fermions, and find that the excitation gap in the non-Abelian phase is fragile against thermal fluctuations of the Z 2 fluxes, while that in the Abelian phase remains open.