Angle-resolved photoemission spectroscopy of superconducting (La,Pr)3Ni2O7/SrLaAlO4 heterostructures

Ruddlesden-Popper bilayer nickelate thin film superconductors discovered under ambient pressure enable great possibilities for investigating electronic structures of the superconducting state. Here, we report angle-resolved photoemission spectroscopy (ARPES) measurements of 1, 2, and 3 unit-cell epitaxial La_2.85Pr_0.15Ni₂O₇ films grown on SrLaAlO₄ substrates, through pure-oxygen in situ sample transportation. Evidence obtained using photons with distinct probing depths shows that conduction is localized primarily at the first unit cell near the interface. Scanning transmission electron microscopy (STEM), together with energy-dispersive X-ray spectroscopy (EDS) and electron energy loss spectroscopy (EELS), indicates that interfacial Sr diffusion and pronounced p-d hybridization gradient may collectively account for the interfacial confinement of conduction. Fermi surface maps reveal hole doping compared to non-superconducting ambient-pressure bulk crystals. Measurements of dispersive band structures suggest contributions from both Ni d _{x ²-y ²} and d _{z ²} orbitals at the Fermi level. Density functional theory (DFT) + U calculations capture qualitative features of the ARPES results, consistent with a hole-doped scenario. These findings constrain theoretical models of the superconducting mechanism and suggest potential for enhancing superconductivity in nickelates under ambient pressure.