We investigate the nonlinear response of the Kitaev honeycomb lattice model in a weak magnetic field using the theory of two-dimensional (2D) coherent spectroscopy. We observe that at the isotropic point in the non-Abelian phase of this model, the nonlinear spectrum in the 2D frequency domain consists of sharp signals that originate from the flux excitations and Majorana bound states. Signatures of different flux excitations can be clearly observed in this spectrum, such that one can observe evidences of flux states with 4-adjacent, 2-nonadjacent, and 4-far-separated fluxes, which are not visible in linear response spectroscopy such as neutron scattering experiments. Moreover, in the Abelian phase we perceive that the spectrum in the frequency domain is composed of streak signals. These signals, as in the nonlinear response of the pure Kitaev model, represent a distinct signature of itinerant Majorana fermions. However, deep in the Abelian phase whenever a Kitaev exchange coupling is much stronger than the others, the streak signals are weakened and only single sharp spots are seen in the response, which resembles the dispersionless response of the conventional toric code.
Two-dimensional coherent terahertz spectroscopy (2DCS) emerges as a valuable tool to probe the nature, couplings, and lifetimes of excitations in quantum materials. It thus promises to identify unique signatures of spin liquid states in quantum magnets by directly probing properties of their exotic fractionalized excitations. Here, we calculate the second-order 2DCS of the Kitaev honeycomb model and demonstrate that distinct spin liquid fingerprints appear already in this lowest-order nonlinear response
χyzx(2)(ω1,ω2) when using crossed light polarizations. We further relate the off-diagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by
Z2 flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wavefunctions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our work can guide future 2DCS experiments on Kitaev magnets.
The Kekul\'e-Kitaev model, an extension of the Kitaev model, exhibits quantum spin liquid properties, which has an exact solution through Kitaev parton construction. In this study, we calculate the dynamical spin structure factor as a linear response and the third-order magnetic susceptibility as a nonlinear response using two-dimensional coherent spectroscopy for the Kekul\'e-Kitaev model. Our results reveal that the few-matter fermion excitations approximation provides reliable results for both linear and nonlinear responses. Notably, while the Kekul\'e-Kitaev model shows linear and nonlinear responses qualitatively similar to the Kitaev model, it displays distinct behavior under a weak uniform and staggered magnetic field. Specifically, the Kekul\'e-Kitaev model does not present a non-Abelian phase under a uniform magnetic field, while such phase appears in the presence of a staggered magnetic field. Interestingly, within the non-Abelian phase, signals originating from two nonadjacent fluxes in the nonlinear response are stronger than signals from other flux excitations. Furthermore, we demonstrate that the ground state of the Kekul\'e-Kitaev model at isotropic coupling is mapped, through unitary spin rotations, to an excited state of the Kitaev model with a uniform flux configuration.
Two-dimensional coherent terahertz spectroscopy (2DCS) emerges as a valuable tool to probe the nature, couplings, and lifetimes of excitations in quantum materials. It thus promises to identify unique signatures of spin liquid states in quantum magnets by directly probing properties of their exotic fractionalized excitations. Here, we calculate the second-order 2DCS of the Kitaev honeycomb model and demonstrate that distinct spin liquid fingerprints appear already in this lowest-order nonlinear response χ_{yzx}^{(2)}(ω_{1},ω_{2}) when using crossed light polarizations. We further relate the off-diagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by Z_{2} flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wave functions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our Letter can guide future 2DCS experiments on Kitaev magnets.
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.
We study the dynamical response functions relevant for electric field induced two-dimensional (2D) coherent nonlinear optical spectroscopy in a Kitaev magnet at finite temperature. We show that these response functions are susceptible to both types of fractional quasiparticles of this quantum spin-liquid, i.e. fermions and flux visons. Focusing on the second order response, we find a strong antidiagonal feature in the 2D frequency plane, related to the galvanoelectric effect of the fractional fermions. Perpendicular to the antidiagonal, the width of this feature is set by quasiparticle relaxation rates beyond the bare Kitaev magnet, thereby providing access to single-particle characteristics within a multi-particle continuum. While the 2D spectrum of the response is set by the fermionic quasiparticles and displays Fermi blocking versus temperature, the emergent bond randomness which arises due to thermally populated visons strongly modifies the fermionic spectrum. Therefore also the presence of gauge excitations is manifest in the 2D nonlinear response as the temperature is increased beyond the flux proliferation crossover.
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.