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Intrinsic exchange bias up to 12.6 kOe is observed inNixCoyFe3-x-yO4(111)/{\alpha}-Al2O3(0001) (0<=x+y<=3) epitaxial thin filmswhere 0.15<=y<=2. An interfacial layer of rock-salt structure emerges betweenNixCoyFe3-x-yO4 thin films and {\alpha}-Al2O3 substrates and is proposed as theantiferromagnetic layer unidirectionally coupled with ferrimagneticNixCoyFe3-x-yO4. In NiCo2O4(111)/{\alpha}-Al2O3(0001) films, results ofreflection high energy electron diffraction, X-ray photoelectron spectroscopy,X-ray reflectometry, and polarized neutron reflectometry support that theinterfacial layer is antiferromagnetic NixCo1-xO (0.32<=x<=0.49) of rock-saltstructure; the interfacial layer and exchange bias can be controlled by growthoxygen pressure revealing the key role of oxygen in the mechanism of theinterfacial reconstruction. This work establishes a family of intrinsicexchange bias materials with great tunability by stoichiometry and growthparameters and emphasizes the strategy of interface engineering in controllingmaterial functionalities.

Highly Tunable Intrinsic Exchange Bias from Interfacial Reconstruction in Epitaxial NixCoyFe3-x-yO4(111)/{\alpha}-Al2O3(0001) Thin Films