Competition between Carrier Injection and Structural Distortions in Electron-Doped Perovskite Nickelate Thin Films

The discovery of superconductivity in doped infinite-layer nickelate thin films has brought increased attention to the behavior of the doped perovskite phase. Despite this interest, the majority of existing studies pertain to hole-doped perovskite rare-earth nickelate thin films, while most electron-doping studies have been performed on bulk materials so far. To tackle this imbalance, a detailed study that addresses doping of NdNiO3 thin films using A-site substitution is presented, using Pb as a dopant and taking advantage of its valence-skipping nature. Through a combination of complementary techniques including X-ray diffraction, transport measurements, X-ray absorption spectroscopy, electron energy-loss spectroscopy and scanning transmission electron microscopy, the valence of Pb in the Nd1-xPbxNiO3 structure is confirmed to be 4+, and the behavior of the doped thin films is found to be controlled by a competition between carrier injection and structural distortions, which respectively reduce and increase the metal-to-insulator transition temperature. This work provides a systematic study of electron doping in NdNiO3, demonstrating that A-site substitution with Pb is an appropriate method for such doping in perovskite rare-earth nickelate systems.