Strain engineering of epitaxial oxide heterostructures beyond substrate limitations

The limitation of commercial single-crystal substrates and the lack of continuous strain tunability preclude the ability to take full advantage of strain engineering for further exploring novel properties and exhaustively studying fundamental physics in complex oxides. Here, we report an approach for imposing continuously tunable epitaxial strain in oxide heterostructures beyond substrate limitations by inserting an interface layer through tailoring of its gradual strain relaxation. Taking BiFeO3 as a model system, we demonstrate the introduction of an ultrathin interface layer that allows the creation of desired strain states that can induce phase transition and stabilize a super-tetragonal phase as well as morphotropic phase boundaries, overcoming substrate limitations. Continuously tunable strain from tension to compression can be generated by precisely adjusting the interface layer thickness, enabling the achievement of continuous orthorhombic–rhombohedral-like–tetragonal-like phase transition. This proposed route could be extended to other oxide heterostructures, providing a platform for creating exotic phases and emergent phenomena.