Emergent Ferromagnetism at LaFeO3/SrTiO3 Interface Arising from Strain-induced Spin-State Transition

Abstract: Creating new interfacial magnetic states with desired functionalities is attractive for fundamental studies and spintronics applications. The emergence of interfacial magnetic phases demands the fabrication of pristine interfaces and the characterization and understanding of atomic structure as well as electronic, magnetic, and orbital degrees of freedom at the interface. Here, we report a novel interfacial insulating ferromagnetic order in antiferromagnetic LaFeO3 grown on SrTiO3, characterized by a combination of electron microscopy and spectroscopy, magnetometry, and density functional theory. The epitaxial strain drives a spin-state disproportionation in the interfacial layer of LaFeO3, which leads to a checkerboard arrangement of low- and high-spin Fe3+ ions inside smaller and larger FeO6 octahedra, respectively. Ferromagnetism at the interface arises from superexchange interactions between the low- and high-spin Fe3+. The detailed understanding of creation of emergent magnetism illustrates the potential of designing and controlling orbital degrees of freedom at the interface to realize novel phases and functionalities for future spin-electronic applications.