Magnetic Ordering and Structural Phase Transitions in a Strained Ultrathin SrRuO3/SrTiO3 Superlattice

Ruthenium-based perovskite systems are attractive because their structural, electronic, and magnetic properties can be systematically engineered. The SrRuO3/SrTiO3 superlattice, with its period consisting of one unit cell each, is very sensitive to strain change. Our first-principles simulations reveal that, in the high tensile strain region, it transits from a ferromagnetic metal to an antiferromagnetic insulator with clear tilted octahedra, while in the low strain region, it is a ferromagnetic metal without octahedra tilting. Detailed analyses of three spin-down Ru - t(2g) orbitals just below the Fermi level reveal that the splitting of these orbitals underlies these dramatic phase transitions, with the rotational force constant of RuO6 octahedron high up to 16 meV/Deg(2), 4 times larger than that of TiO6. Differently from nearly all the previous studies, these transitions can be probed optically through the diagonal and off-diagonal dielectric tensor elements. For a 1% change in strain, our experimental spin moment change is -0.14 +/- 0.06 (mu B), quantitatively consistent with our theoretical value of -0.1 (mu B).