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 ( TV) 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.
Keywords: Fe3−δO4; Magnetite; Verwey transition; heterointerfaces; spin moment; spintronics.