Modulation of magnetoelectric coupling through systematically engineered spin canting in nickel‐zinc ferrite

A nickel-zinc ferrite system, which is one of the well-known versatile soft-ferromagnetic oxides, was investigated in terms of magnetoelectric (ME) coupling at room temperature. Herein, we demonstrated that spin canting is manipulated through a composition-induced structural transition from an inverse to a normal spinel structure, leading to modulation in the ME coupling. The ME coefficient was maximized at 60 at.% Zn substitution with a value of 0.1 mV/(Oe center dot cm), denoting similar to 70% enhancement compared to that of the pure nickel ferrite. It was revealed that the interspin angle is enhanced along the octahedral site at up to similar to 60 at.% Zn substitution, consistent with the composition level at the culmination of the ME coupling, evidenced by X-ray diffraction profiles and magnetic hysteresis loops combined with density functional theory calculations. Given that this approach is based on a tractable fabrication method, this study is expected to be widely used in modulation of the ME coupling in spinel-structured oxides.