Tunable Magnetic Phases at Fe₃O₄/SrTiO₃ Oxide Interfaces

We demonstrate the emergence and control of magnetic phases between magnetite (Fe₃O₄), a ferrimagnetic halfmetal, and SrTiO₃, a transparent nonmagnetic insulator considered the bedrock of oxide-based electronics. The Verwey transition ( T_V) was detected to persist from bulk-like down to ultrathin Fe₃O₄ films, decreasing from 117 ± 4 K (38 nm) to 25 ± 4 K (2 nm), respectively. Element-selective electronic and magnetic properties of the ultrathin films and buried interfaces are studied by angle-dependent hard X-ray photoelectron spectroscopy and X-ray magnetic circular dichroism techniques. We observe a reduction of Fe²⁺ ions with decreasing film thickness, accompanied by an increase of Fe³⁺ ions in both tetrahedral and octahedral sites and conclude on the formation of a magnetically active ferrimagnetic 2 u.c. γ-Fe₂O₃ intralayer. To manipulate the interfacial magnetic phase, a postannealing process causes the controlled reduction of the γ-Fe₂O₃ that finally leads to stoichiometric and ferrimagnetic Fe₃O₄/SrTiO₃(001) heterointerfaces.