Ni-O hybridization-driven electronic reconstruction across the superconducting dome in an infinite-layer nickelate

Abstract

Superconductivity in infinite-layer nickelates has drawn wide interest as a cuprate analogue, yet how the electronic structure evolves with hole doping remains unsettled. Here we map the doping- and temperature-dependent unoccupied states of the La-based infinite-layer nickelate La1-xCaxNiO2 using O K-edge and Ni L-edge x-ray absorption spectroscopy. Superconductivity occurs for 0.18<=x<=0.27. Near x~0.20-0.23, low-energy spectral weight redistributes: Ni3d-dominated states decrease while O2p-hybridized states increase, indicating an orbital-selective crossover in Ni-O covalency. This crossover coincides with a sign reversal of the Hall coefficient and precedes the reduction of the superconducting critical temperature at higher doping. By directly linking transport anomalies and the superconducting dome to a measurable Ni-O orbital reorganization, our results provide a key step toward a unified, orbital-resolved phase diagram for infinite-layer nickelates and a practical route to engineer superconductivity via hybridization control.