Engineering polar distortions in multiferroic Sr1−xBaxMnO3−δ thin films

The physical properties of perovskite oxide thin films are governed by the subtle interplay between chemical composition and crystal symmetry variations, which can be altered by epitaxial growth. In the case of perovskite-type multiferroic thin films, precise control of stoichiometry and epitaxial strain allows for gaining control over the ferroic properties through selective crystal distortions. Here, we demonstrate the chemical tailoring of the polar atomic displacements by tuning the stoichiometry of multiferroic Sr1−xBaxMnO3−δ (0 ≤ x ≤ 0.5) epitaxial thin films. A combination of x-ray diffraction and aberration-corrected scanning transmission electron microscopy enables unraveling the local polarization orientation at the nanoscale as a function of the film’s composition and induced crystalline structure. We demonstrate experimentally that the orientation of polarization is intimately linked to the Ba doping and O stoichiometry of the films and, with the biaxial strain induced by the substrate, it can be tuned either in-plane or out-of-plane with respect to the substrate by the appropriate choice of the post-growth annealing temperature and O2 atmosphere. This chemistry-mediated engineering of the polarization orientation of oxide thin films opens new venues for the design of functional multiferroic architectures and the exploration of novel physics and applications of ferroelectric textures with exotic topological properties.