Charge Transfer and Orbital Reconstruction in Strain-Engineered (La,Sr)MnO₃/LaNiO₃ Heterostructures

We investigate charge transfer, orbital reconstruction, and the emergence of exchange bias in (La,Sr)MnO3/LaNiO3 heterostructures. We demonstrate that charge transfer from Mn(3+) ions to Ni(3+) ions is accompanied by the formation of hybridized Mn/Ni 3z(2) - r(2) orbits at the interface, instead of strain-stabilized Mn and Ni x(2) - y(2) orbits in the bulk films. In the heterostructures with ultrathin LaNiO3, orbital reconstruction induced by charge transfer results in magnetization frustration of (La,Sr)MnO3 at the interface. But the strain effect exerted by the growth of the LaNiO3 top layer plays a dominant role on orbital reconstruction in the heterostructures with thick LaNiO3, stabilizing 3z(2) - r(2) orbits. In this case, robust spin glass, associated with larger magnetization frustration, accounts for the exchange bias effect. Our work builds a bridge between the microscopic electronic structure and the macroscopic magnetic property, providing the possibility of manipulating the exotic states with the aid of strain engineering in oxide-based electronics.