Observation of a Half-Metallic Interface State for Pyridine-Adsorbed H/Fe₃O₄(100)

Organic molecule/half-metallic oxide interfaces play essential roles in recent molecular spintronics devices, yet factors governing the spin polarization of the hybridized interface state (HIS) formed there remain unclear because of the lack of direct spectroscopic evidence for it. Here, we present a spin-polarized metastable deexcitation spectroscopy (SPMDS) experiment, which is sensitive to the topmost surface, showing that the adsorption of pyridine on H-terminated Fe₃O₄(100) at 100 K produces a highly spin-polarized HIS, while no such HIS forms on a bare Fe₃O₄(100) surface. A density functional theory calculation has predicted the formation of half-metallic HIS, which is consistent with the SPMDS results. This can be understood on the basis of the interface chemical bonding formed by the coordination of the nitrogen end of pyridine to the surface Fe atom where half-metallic conduction electrons are distributed.