Three-dimensional (3D) strain induced in self-assembled vertically aligned nanocomposite (VAN) epitaxial films provides an unrivaled method to induce very large strains in thin films. Here, by growing VAN films of EuTiO3 (ETO)-Eu2O3 (EO) with different EO fractions, the vertical strain was systematically increased in ETO, up to 3.15%, and the Eu-Ti-Eu bond angle along ⟨111⟩ decreased by up to 1°, leading to a weakening of the antiferromagnetic interactions and switching from antiferromagnetic to ferromagnetic behavior. Our work has shown for the first time that Eu-Ti-Eu superexchange interactions play a key role in determining the magnetic ground state of ETO. More broadly, our work serves as an exemplar to show that multifunctionalities in strong spin-lattice coupling perovskite oxides can be uniquely tuned at the atomic scale using simple VAN structures.
Keywords: multiferroics; nanocomposite; self-assembled nanostructures; spintronics; thin films.