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.