Complex perovskite oxides exhibit a rich spectrum of functional responses, including magnetism, ferroelectricity, highly correlated electron behavior, superconductivity, etc. There exists a small set of materials which exhibit multiple order parameters; these are known as multiferroics. Using our work in the field of ferroelectrics and ferromagnetics as the background, we are now exploring such materials, as epitaxial thin films as well as nanostructures. Specifically, we are studying the role of thin film growth, heteroepitaxy and processing on the basic properties as well as magnitude of the coupling between the order parameters. In single phase multiferroic perovskites, such as BiFeO₃, we have found significant enhancements in magnetism and ferroelectricity compared to bulk. Detailed measurements indicate that the enhancement in magnetism is due to a mixed Fe+2/Fe+3 state in the films, while the ferroelectric polarization is reasonably commensurate with that predicted from first principles theory. A very exciting new development has been the discovery of the formation of spontaneously assembled nanostructures consisting of a ferromagnetic phase embedded in a ferroelectric matrix that exhibit very strong coupling between the two order parameters. This involves 3-dimensional heteroepitaxy between the substrate, the matrix perovskite phase and spinel phase that is embedded as single crystalline pillars in this matrix. This epitaxial coupling is critical and is responsible for the significantly higher magnetoelectric coupling and magnetic anisotropy in such vertical heterostructures compared to a conventional heterostructure.

This work is supported by the ONR under a MURI program.