Sizable Ligand-Mediated Bond-Dependent Interactions in a Spin-1 Triangular Antiferromagnet NiI${}_2$

Abstract

The bond-dependent anisotropic Kitaev interactions are the key for the Kitaev model, which has attracted intense interest for its potential to host quantum-spin-liquid states and fractional excitations. However, experimental realizations of such interactions remain scarce. Here, we investigate the magnetic excitations of NiI${}_2$, a van der Waals magnet with spin $S=1$. By combining inelastic neutron scattering, magnetization measurements, magnetic structure analysis, first-principles calculations, and linear-spin-wave simulations, we identify a minimal model that features substantial Kitaev and off-diagonal $\Gamma$ interactions, which together stabilize the canted magnetic ground state and open a gap in the spin-wave spectrum. Notably, these interactions arise from strong spin-orbit coupling on the ligand ions, despite the quenched orbital moment of the magnetic Ni${}^{2+}$ ions. Our results provide compelling experimental evidence for the ligand-driven Kitaev mechanism. This demonstrates a concrete pathway to generating strong bond-dependent anisotropy in systems where the magnetic ions themselves have weak spin-orbit coupling, thereby substantially broadening the range of potential Kitaev materials.

8 pages, 4 figures

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