Electronic structures across superconductor-insulator transition in Ruddlesden-Popper bilayer nickelate films

Abstract

High-transition-temperature ($T_{C}$) superconductivity is recently discovered in Ruddlesden-Popper (RP) nickelate films with extraordinarily strong oxidation. While investigating phase diagrams is essential for uncovering the superconducting mechanism, the oxygen-tuned superconductor-insulator transition (SIT) in RP nickelates differs fundamentally from that in cuprates or iron-based systems. Here, we unveil the evolution of electronic structure in RP bilayer nickelate thin films across the SIT, combining angle-resolved photoemission spectroscopy (ARPES) and X-ray absorption spectroscopy (XAS) for both occupied and unoccupied states. In the superconducting state, a coherent quasiparticle band near Fermi level ($E_{F}$) coexists with an incoherent waterfall feature at high energy, paralleling that in cuprates. Approaching the insulating state with oxygen deficiency, the spectral weight of the occupied coherent quasiparticle band is gradually suppressed, accompanied by pronounced density of states redistribution and orbital reconfiguration in unoccupied states. These results reveal the electronic origin of the SIT in the phase diagram, which transcends carrier doping effects and oxygen vacancy states. Our findings point to a decisive role of oxygen in shaping the essential electronic landscape of RP bilayer nickelates, offering crucial insights into the superconducting mechanism.