Antiferromagnetism at T > 500 K in the layered hexagonal ruthenate SrRu2O6

We report an experimental and computational study of the magnetic and electronic properties of the layered Ru(V) oxide SrRu2O6 (hexagonal, P ¯31m), which shows antiferromagnetic order with a N´eel temperature of 563(2) K, among the highest for 4d oxides. Magnetic order occurs both within edge-shared octahedral sheets and between layers and is accompanied by anisotropic thermal expansivity that implies strong magnetoelastic coupling of Ru(V) centers. Electrical transport measurements using focused-ion-beam–induced deposited contacts on a micron-scale crystallite as a function of temperature show p-type semiconductivity. The calculated electronic structure using hybrid density functional theory successfully accounts for the experimentally observed magnetic and electronic structure, and Monte Carlo simulations reveal how strong intralayer as well as weaker interlayer interactions are a defining feature of the high-temperature magnetic order in the material