Interfacial Strain: The Driving Force for Selective Orbital Occupancy in Manganite Thin Films

Complex oxides with perovskite structure are the ideal arena to study a plethora of physical properties including superconductivity, ferromagnetism, ferroelectricity, piezoelectricity and more. Among them, transition metal oxides are especially relevant since they present large electronic correlations leading to a strong competition between lattice, charge, spin, and orbital degrees of freedom. In particular, manganese perovskites oxides exhibit half‐metallic character and colossal magnetoresistive response rendering them as the ideal materials to develop novel concepts of oxide‐electronic devices and for the study of fundamental physical interactions. Due to the close similarity between kinetic energy of charge carriers and Coulomb repulsion, tiny perturbations caused by small changes in temperature, magnetic or electric fields, strain and so forth may drastically modify the magnetic and transport properties of these materials. In particular clarifying the role of interfacial strain in manganite thin films is interesting not only for device applications but also for basic understanding of physical interactions. A better comprehension of such strongly correlated systems might lead to control the different degrees of freedom in a near future contributing to the development of the so called orbitronics, i.e. controlling and modifying at will the orbital orientation of the 3d levels in transition metals. Here we reveal the importance of interfacial strain in high quality epitaxial thin films of La_2/3Ca_1/3MnO₃ (LCMO), grown on top of SrTiO₃ (STO) and NdGaO₃ (NGO) (001)‐oriented substrates. We show that in such systems interfacial strain due to lattice mismatch lifts the degeneracy of the e_g and t_2g orbitals close to the film/substrate interface inducing Jahn‐Teller like distortions and promoting selective orbital occupancy and the appearance of an orbital glass insulating state in an otherwise ferromagnetic metallic material. These results highlight the role of strain and identify it as a key parameter in orbital control.