Noncoplanar and Counterrotating Incommensurate Magnetic Order Stabilized by Kitaev Interactions in γ-Li2IrO3

Materials that realize Kitaev spin models with bond-dependent anisotropic interactions have long been searched for, as the resulting frustration effects are predicted to stabilize novel forms of magnetic order or quantum spin liquids. Here, we explore the magnetism of gamma-Li2IrO3, which has the topology of a three-dimensional Kitaev lattice of interconnected Ir honeycombs. Using magnetic resonant x-ray diffraction, we find a complex, yet highly symmetric incommensurate magnetic structure with noncoplanar and counterrotating Ir moments. We propose a minimal Kitaev-Heisenberg Hamiltonian that naturally accounts for all key features of the observed magnetic structure. Our results provide strong evidence that gamma-Li2IrO3 realizes a spin Hamiltonian with dominant Kitaev interactions.