From Fe3O4/NiO bilayers to NiFe2O4-like thin films through Ni interdiffusion

Ferrites with (inverse) spinel structure display a large variety of electronic and magnetic properties, making some of them interesting for potential applications in spintronics. We investigate the thermally induced interdiffusion of Ni$^{2+}$ ions out of NiO into Fe$_3$O$_4$ ultrathin films, resulting in off-stoichiometric nickel ferrite–like thin layers. We synthesized epitaxial Fe$_3$O$_4$ bilayers on Nb-doped SrTiO$_3$(001) substrates by means of reactive molecular beam epitaxy. Subsequently, we performed an annealing cycle comprising three steps at temperatures of 400$^\circ$C, 600$^\circ$C, and 800$^\circ$C under an oxygen background atmosphere. We studied the changes of the chemical and electronic properties as result of each annealing step with help of hard x-ray photoelectron spectroscopy and found a rather homogeneous distribution of Ni and Fe cations throughout the entire film after the overall annealing cycle. For one sample we observed a cationic distribution close to that of the spinel ferrite NiFe$_2$O$_4$. Further evidence comes from low-energy electron diffraction patterns indicating a spinel-type structure at the surface after annealing. Site- and element-specific hysteresis loops performed by x-ray magnetic circular dichroism uncovered the antiferrimagnetic alignment between the octahedral coordinated Ni$^{2+}$ and Fe$^{3+}$ ions and the Fe$^{3+}$ ion in tetrahedral coordination. We find a quite low coercive field of 0.02 T, indicating a rather low defect concentration within the thin ferrite films