Designing Morphotropic Phase Composition in BiFeO3.

In classical morphotropic piezoelectric materials, rhombohedral and tetragonal phase variants can energetically compete to form a mixed phase regime with improved functional properties. While the discovery of morphotropic-like phases in multiferroic BiFeO3 films has broadened this definition, accessing these phase spaces is still typically accomplished through isovalent substitution or heteroepitaxial strain which do not allow for continuous modification of phase composition postsynthesis. Here, we show that it is possible to use low-energy helium implantation to tailor morphotropic phases of epitaxial BiFeO3 films postsynthesis in a continuous and iterative manner. Applying this strain doping approach to morphotropic films creates a new phase space based on internal and external lattice stress that can be seen as an analogue to temperature-composition phase diagrams of classical morphotropic ferroelectric systems.

Designing Magnetic Anisotropy through Strain Doping.

The coupling between a material's lattice and its underlying spin state links structural deformation to magnetic properties; however, traditional strain engineering does not allow the continuous, post-synthesis control of lattice symmetry needed to fully utilize this fundamental coupling in device design. Uniaxial lattice expansion induced by post-synthesis low energy helium ion implantation is shown to provide a means of bypassing these limitations. Magnetocrystalline energy calculations can be used a priori to estimate the predictive design of a material's preferred magnetic spin orientation. The efficacy of this approach is experimentally confirmed in a spinel CoFe2O4 model system where the epitaxial film's magnetic easy axis is continuously manipulated between the out-of-plane (oop) and in-plane (ip) directions as lattice tetragonality moves from ip to oop with increasing strain doping. Macroscopically gradual and microscopically abrupt changes to preferential spin orientation are demonstrated by combining ion irradiation with simple beam masking and lithographic procedures. The ability to design magnetic spin orientations across multiple length scales in a single crystal wafer using only crystal symmetry considerations provides a clear path toward the rational design of spin transfer, magnetoelectric, and skyrmion-based applications where magnetocrystalline energy must be dictated across multiple length scales.