Orbital engineering of nickelates in three-component heterostructures

The orbital configuration of complex oxides dictates the emergence of a wide range of properties, including metal-insulator transitions, interfacial magnetism, and high-temperature superconductivity. In this work, we experimentally demonstrate a novel method for achieving large and tunable orbital polarizations in nickelates. The technique is based on leveraging three-component, atomically layered superlattices to yield a combination of inversion symmetry breaking, charge transfer, and polar distortions. In the system we studied, composed of LaTiO$_3$/LaNiO$_3$/LaAlO$_3$, we use synchrotron x-ray diffraction and spectroscopy to characterize these properties and show that they lead to fully broken orbital degeneracy in the nickelate layer consistent with a single-band Fermi surface. Furthermore, we show that this system is widely tunable and enables quasi-continuous orbital control unachievable by conventional strain and confinement-based approaches. This technique provides an experimentally realizable route for accessing and studying novel orbitally dependent quantum phenomena.