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The recent observation of superconductivity in N d 0.8 S r 0.2 N i O 2 has raised fundamental questions about the hierarchy of the underlying electronic structure. Calculations suggest that this system falls in the Mott–Hubbard regime, rather than the charge-transfer configuration of other nickel oxides and the superconducting cuprates. Here, we use state-of-the-art, locally resolved electron energy-loss spectroscopy to directly probe the Mott–Hubbard character of N d 1 − x S r x N i O 2 . Upon doping, we observe emergent hybridization reminiscent of the Zhang–Rice singlet via the oxygen-projected states, modification of the Nd 5d states, and the systematic evolution of Ni 3d hybridization and filling. These experimental data provide direct evidence for the multiband electronic structure of the superconducting infinite-layer nickelates, particularly via the effects of hole doping on not only the oxygen but also nickel and rare-earth bands. 

Abstract The occurrence of unconventional superconductivity in cuprates has long motivated the search for manifestations in other layered transition metal oxides. Recently, superconductivity is found in infinite‐layer nickelate (Nd,Sr)NiO₂and (Pr,Sr)NiO₂thin films, formed by topotactic reduction from the perovskite precursor phase. A topic of much current interest is whether rare‐earth moments are essential for superconductivity in this system. In this study, it is found that with significant materials optimization, substantial portions of the La_1−xSr_xNiO₂phase diagram can enter the regime of coherent low‐temperature transport (x = 0.14 ‐ 0.20), with subsequent superconducting transitions and a maximum onset of ≈9 K atx = 0.20. Additionally, the unexpected indication of a superconducting ground state in undoped LaNiO₂is observed, which likely reflects the self‐doped nature of the electronic structure. Combining the results of (La/Pr/Nd)_1−xSr_xNiO₂reveals a generalized superconducting dome, characterized by systematic shifts in the unit cell volume and in the relative electron‐hole populations across the lanthanides.