Strain-mediated phase crossover in Ruddlesden–Popper nickelates

Recent progress on the signatures of pressure-induced high-temperature superconductivity in Ruddlesden–Popper (RP) nickelates (La n +1 Ni n O 3 n +1 ) has attracted growing interest in both theoretical calculations and experimental efforts. The fabrication of high-quality single-crystalline RP nickelate thin films is critical for possible reducing the superconducting transition pressure and advancing applications in microelectronics in the future. In this study, we report the observations of an active phase transition in RP nickelate films induced by misfit strain. We found that RP nickelate films favor the perovskite structure ( n = ∞) under tensile strains, while compressive strains stabilize the La 3 Ni 2 O 7 ( n = 2) phase. The selection of distinct phases is governed by the strain dependent formation energy and electronic configuration. In compressively strained La 3 Ni 2 O 7 , we experimentally determined the e g splitting energy is ~0.2 eV and electrons prefer to occupy in-plane orbitals. First-principles calculations unveil a robust coupling between strain effects and the valence state of Ni ions in RP nickelates, suggesting a dual driving force for the inevitable phase co-existence transition in RP nickelates. Our work underscores the sensitivity of RP nickelate formation to epitaxial strain, presenting a significant challenge in fabricating pure-phase RP nickelate films. Therefore, special attention to stacking defects and grain boundaries between different RP phases is essential when discussing the pressure-induced superconductivity in RP nickelates.