Spin-orbit coupling controlled two-dimensional magnetism in chromium trihalides

CrX_3 (X = Cl, Br, I) have the same crystal structure and Hamiltonian but different ligand spin-orbit coupling (SOC) constant λ_X, providing excellent material platform exploring for exotic two-dimensional (2D) spin orders. Their microscopic mechanism underlying 2D spin physics and Hamiltonian remain unestablished, along with experimental corroboration of Kitaev exchange interaction, central to realizing topological quantum spin liquids. We report Kitaev interaction signature in magnetic anisotropy measured by ferromagnetic resonance (FMR) spectroscopy. We present measured values of Heisenberg J, Kitaev K, and off-diagonal symmetric Γ exchange interactions in CrX_3 determined using FMR and exact diagonalization. K and Γ exhibit dominant quadratic dependencies on λ_X, indicating its central role in 2D magnetism. Our study provides foundation for exploring exotic 2D magnetic topologies by tuning intrinsic material parameters such as SOC.