Correlation of Interface Impurities and Chemical Gradients with High Magnetoelectric Coupling Strength in Multiferroic BiFeO₃–BaTiO₃ Superlattices

The detailed understanding of magnetoelectric (ME) coupling in multiferroic oxide heterostructures is still a challenge. In particular, very little is known to date concerning the impact of the chemical interface structure and unwanted impurities that may be buried within short-period multiferroic BiFeO₃–BaTiO₃ superlattices during growth. Here, we demonstrate how trace impurities and elemental concentration gradients contribute to high ME voltage coefficients in thin-film superlattices, which are built from 15 double layers of BiFeO₃–BaTiO₃. Surprisingly, the highest ME voltage coefficient of 55 V cm^–1 Oe^–1 at 300 K was measured for a superlattice with a few atomic percent of Ba and Ti that diffused into the nominally 5 nm thin BiFeO₃ layers, according to analytical transmission electron microscopy. In addition, highly sensitive enhancements of the cation signals were observed in depth profiles by secondary ion mass spectrometry at the interfaces of BaTiO₃ and BiFeO₃. As these interface features correlate with the ME performance of the samples, they point to the importance of charge effects at the interfaces, that is, to a possible charge mediation of ME coupling in oxide superlattices. The challenge is to provide cleaner materials and processes, as well as a well-defined control of the chemical interface structure, to push forward the application of oxide superlattices in multiferroic ME devices