Incommensurate counterrotating magnetic order stabilized by Kitaev interactions in the layered honeycomb [alpha]-Li[subscript 2] IrO[Subscript 3]

Abstract

The layered honeycomb magnet α-Li_{2}IrO_{3} has been theoretically proposed as a candidate to display unconventional magnetic behaviour associated with Kitaev interactions between spin-orbit entangled j_{eff}=1/2 magnetic moments on a honeycomb lattice. Here we report single crystal magnetic resonant x-ray diffraction combined with powder magnetic neutron diffraction to reveal an incommensurate magnetic order in the honeycomb layers with Ir magnetic moments counterrotating on nearest-neighbor sites. This unexpected type of magnetic structure for a honeycomb magnet cannot be explained by a spin Hamiltonian with dominant isotropic (Heisenberg) couplings. The magnetic structure shares many key features with the magnetic order in the structural polytypes β- and γ-Li_{2}IrO_{3}, understood theoretically to be stabilized by dominant Kitaev interactions between Ir moments located on the vertices of three-dimensional hyperhoneycomb and stripyhoneycomb lattices, respectively. Based on this analogy and a theoretical soft-spin analysis of magnetic ground states for candidate spin Hamiltonians, we propose that Kitaev interactions also dominate in α-Li_{2}IrO_{3}, indicative of universal Kitaev physics across all three members of the harmonic honeycomb family of Li_{2}IrO_{3} polytypes.