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Fundamental Spin Interactions Underlying the Magnetic Anisotropy in the Kitaev Ferromagnet CrI$_3$

We lay the foundation for determining the microscopic spin interactions in two-dimensional (2D) ferromagnets by combining angle-dependent ferromagnetic resonance (FMR) experiments on high quality CrI$_3$ single crystals with theoretical modeling based on symmetries. We discover that the Kitaev interaction is the strongest in this material with $K \sim -5.2$ meV, 25 times larger than the Heisenberg exchange $J \sim -0.2$ meV, and responsible for opening the $\sim$5 meV gap at the Dirac points in the spin-wave dispersion. Furthermore, we find that the symmetric off-diagonal anisotropy $Γ\sim -67.5$ $μ$eV, though small, is crucial for opening a $\sim$0.3 meV gap in the magnon spectrum at the zone center and stabilizing ferromagnetism in the 2D limit. The high resolution of the FMR data further reveals a $μ$eV-scale quadrupolar contribution to the $S=3/2$ magnetism. Our identification of the underlying exchange anisotropies opens paths toward 2D ferromagnets with higher $T_\text{C}$ as well as magnetically frustrated quantum spin liquids based on Kitaev physics.