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arXiv:1605.03272 · Physical Review Letters

Resonant Inelastic X-Ray Scattering Response of the Kitaev Honeycomb Model

Gábor B. Halász, Natalia Borisovna Perkins, Jeroen van den Brink

Published Sep 16, 2016• 68 citations
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Abstract

We calculate the resonant inelastic x-ray scattering (RIXS) response of the Kitaev honeycomb model, an exactly solvable quantum-spin-liquid model with fractionalized Majorana and flux excitations. We find that the fundamental RIXS channels, the spin-conserving (SC) and the non-spin-conserving (NSC) ones, do not interfere and give completely different responses. SC RIXS picks up exclusively the Majorana sector with a pronounced momentum dispersion, whereas NSC RIXS also creates immobile fluxes, thereby rendering the response only weakly momentum dependent, as in the spin structure factor measured by inelastic neutron scattering. RIXS can, therefore, pick up the fractionalized excitations of the Kitaev spin liquid separately, making it a sensitive probe to detect spin-liquid character in potential material incarnations of the Kitaev honeycomb model.

DOI
10.1103/physrevlett.117.127203

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We calculate the resonant inelastic x-ray scattering (RIXS) response of the Kitaev honeycomb model, an exactly solvable quantum-spin-liquid model with fractionalized Majorana and flux excitations. We find that the fundamental RIXS channels, the spin-conserving (SC) and the non-spin-conserving (NSC) ones, do not interfere and give completely different responses. SC RIXS picks up exclusively the Majorana sector with a pronounced momentum dispersion, whereas NSC RIXS also creates immobile fluxes, thereby rendering the response only weakly momentum dependent, as in the spin structure factor measured by inelastic neutron scattering. RIXS can, therefore, pick up the fractionalized excitations of the Kitaev spin liquid separately, making it a sensitive probe to detect spin-liquid character in potential material incarnations of the Kitaev honeycomb model.
We propose that resonant inelastic x-ray scattering (RIXS) is an effective probe of the fractionalized excitations in three-dimensional (3D) Kitaev spin liquids. While the non-spin-conserving RIXS responses are dominated by the gauge-flux excitations and reproduce the inelastic-neutron-scattering response, the spin-conserving (SC) RIXS response picks up the Majorana-fermion excitations and detects whether they are gapless at Weyl points, nodal lines, or Fermi surfaces. As a signature of symmetry fractionalization, the SC RIXS response is suppressed around the Γ point. On a technical level, we calculate the exact SC RIXS responses of the Kitaev models on the hyperhoneycomb, stripyhoneycomb, hyperhexagon, and hyperoctagon lattices, arguing that our main results also apply to generic 3D Kitaev spin liquids beyond these exactly solvable models.
Motivated by the ongoing effort to search for high-resolution signatures of quantum spin liquids, we investigate the temperature dependence of the indirect resonant inelastic x-ray scattering (RIXS) response for the Kitaev honeycomb model. We find that, as a result of spin fractionalization, the RIXS response changes qualitatively at two well-separated temperature scales, TL{T}_{L}TL​ and TH{T}_{H}TH​, which correspond to the characteristic energies of the two kinds of fractionalized excitations, Z2{\mathbb{Z}}_{2}Z2​ gauge fluxes and Majorana fermions, respectively. While thermally excited Z2{\mathbb{Z}}_{2}Z2​ gauge fluxes at temperature TL{T}_{L}TL​ lead to a general broadening and softening of the response, the thermal proliferation of Majorana fermions at temperature ${T}_{H}\ensuremath{\sim}10\phantom{\rule{0.16em}{0ex}}{T}_{L}$ results in a significant shift of the spectral weight, both in terms of energy and momentum. Due to its exclusively indirect nature, the RIXS process we consider gives rise to a universal magnetic response and, from an experimental perspective, it directly corresponds to the KKK-edge of Ru3+{\mathrm{Ru}}^{3+}Ru3+ in the Kitaev candidate material $\ensuremath{\alpha}\ensuremath{-}{\mathrm{RuCl}}_{3}$.
We provide an exact study of dynamical correlations for the quantum spin-orbital liquid phases of an SU(2)-symmetric Kitaev honeycomb lattice model. We show that the spin dynamics in this Kugel-Khomskii type model is exactly the density-density correlation function of S=1 fermionic magnons, which could be probed in resonant inelastic x-ray scattering experiments. We predict the characteristic signatures of spin-orbital fractionalization in inelastic scattering experiments and compare them to the ones of the spin-anisotropic Kitaev honeycomb spin liquid. In particular, the resonant inelastic x-ray scattering response shows a characteristic momentum dependence directly related to the dispersion of fermionic excitations. The neutron scattering cross section displays a mixed response of fermionic magnons as well as spin-orbital excitations. The latter has a bandwidth of broad excitations and a vison gap that is three times larger than that of the spin-1=2 Kitaev model.
We consider the question of whether resonant inelastic x-ray scattering (RIXS) can be used to detect many-body excitations that are coupled to the spin-chirality terms ${\mathbf{S}}_{i}\ifmmode\cdot\else\textperiodcentered\fi{}({\mathbf{S}}_{j}\ifmmode\times\else\texttimes\fi{}{\mathbf{S}}_{k})$ in a Mott insulator. We find that while the spin-chirality terms are in general absent in the usual experimental setups of RIXS, there are prospects of realizing such terms if one considers instead the scattering near a pre-edge. We then perform detailed analyses for the square and the kagome lattices, and brief analyses for the triangular and the honeycomb lattices, in which we show that the spin-chirality terms are indeed present in all the above lattices, but that they occur at a higher order in our expansion for the kagome and the honeycomb lattices. The merit of using RIXS in addition to Raman spectroscopy to detect excitations that are coupled to the spin-chirality terms is also briefly discussed in the context of the emergent gauge boson in the U(1)\text{U}(1)U(1) Dirac spin liquid.
We consider the question of whether resonant inelastic x-ray scattering (RIXS) can be used to detect many-body excitations that are coupled to the spin-chirality terms S[subscript i]·(S[subscript j]×S[subscript k]) in a Mott insulator. We find that while the spin-chirality terms are in general absent in the usual experimental setups of RIXS, there are prospects of realizing such terms if one considers instead the scattering near a pre-edge. We then perform detailed analyses for the square and the kagome lattices, and brief analyses for the triangular and the honeycomb lattices, in which we show that the spin-chirality terms are indeed present in all the above lattices, but that they occur at a higher order in our expansion for the kagome and the honeycomb lattices. The merit of using RIXS in addition to Raman spectroscopy to detect excitations that are coupled to the spin-chirality terms is also briefly discussed in the context of the emergent gauge boson in the U(1) Dirac spin liquid.
We determine the spin-exchange dynamical structure factor of the Heisenberg spin chain, as is measured by indirect resonant inelastic x-ray scattering (RIXS). We find that two-spin RIXS excitations nearly entirely fractionalize into two-spinon states. These share the same continuum lower bound as single-spin neutron scattering excitations, even if the relevant final states belong to orthogonal symmetry sectors. The RIXS spectral weight is mainly carried by higher-energy excitations, and is beyond the reach of the low-energy effective theories of Luttinger liquid type.