Strain-Driven Oxygen Vacancy Ordering in LaNiO₃ Thin Films Revealed by Integrated Differential Phase Contrast Imaging in Scanning Transmission Electron Microscopy

Abstract

Rare-earth nickelates, such as LaNiO3 (LNO), exhibit complex electronic properties, with ordered oxygen vacancies (OOV) influencing conductivity and magnetic behavior. We investigate the structural stability of strain-induced OOV phase in LNO thin film grown on SrTiO3 substrate and impact of Ruddlesden-Popper (RP) faults. Using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and integrated differential phase contrast (iDPC) STEM imaging, we conducted atomic-scale structural and compositional analyses of OOV. Geometric phase analysis (GPA) was employed to measure the strain in fault-free and RP fault regions, while density functional theory (DFT) calculations explored different OOV arrangements in the LNO phase. Simulated iDPC-STEM imaging of energy-stabilized structures was performed to correlate with experimental results. Our findings reveal superstructure modulation in the chemical composition and atomic-scale lattice structure in LNO, primarily due to the formation of the OOV in Ni-O layers of the LaNiO2.5 phase. The out-of-plane compressive strain of about 2 % stabilizes this phase, reducing the strain, diminishing OOV, and transforming them into LNO.