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.
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.
We study electric-field-induced second harmonic generation (SHG) in the Kitaev model. This frustrated magnet hosts a quantum spin liquid, featuring fractionalization in terms of mobile Majorana fermion and static
Z2 flux-vison elementary excitations. We show that finite-temperature SHG allows to probe characteristic features of both fractional quasiparticle types. In the homogeneous flux state at low temperatures, the SHG susceptibility displays an oscillatory spectrum, which is set by only the fermionic excitations and is subject to temperature-induced Fermi blocking, generic to all higher harmonic generation (HHG). In the intermediate to high-temperature range, intrinsic randomness, which emerges from thermally excited visons leads to drastic changes of the SHG susceptibility, resulting from resonance decoupling over a wide range of energies. At the flux proliferation crossover, we suggest an interpolation between these two temperature regimes. Our results satisfy previously established symmetries for electric-field-induced SHG in Kitaev magnets.
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.
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.
In recent years, techniques of intense THz laser have enabled us to experimentally observe nonlinear spin dynamics in antiferromagnets since the elementary excitations such as magnons reside on a THz to GHz range in antiferromagnets and THz laser thus can directly excite them. We numerically and theoretically investigate THz-laser or GHz-wave driven harmonic generations in typical ordered phases of antiferromagnets: Néel, canted and weak ferromagnetic phases. The radiation waves (harmonic generations) are created by the incident-wave driven magnon dynamics. We point out that magnetic orders and phase transitions can change the spectra of harmonic generations, differently from those of metallic, semiconductor, or atomic-gas systems without (spontaneous) symmetry breakings. We consider both the magnon harmonic generation driven by standard single-color laser and that by two-color laser in the antiferromagnets, and find several dynamical symmetries and the corresponding selection rules of the harmonic generations. These results indicate that the magnon harmonic generation spectra provide new information about symmetry or symmetry breaking of antiferromagnets.