Superconductivity and Electronic Structures of Nickelate Thin Film Superstructures

Abstract

Ruddlesden-Popper (RP) nickelates have emerged as a crucial platform for exploring the mechanisms of high-temperature superconductivity. However, the Fermi surface topology required for superconductivity remains elusive. Here, beyond the superconducting pure bilayer (2222) phase, we report the thin film growth and ambient-pressure superconductivity of monolayer-bilayer (1212) and bilayer-trilayer (2323) superstructures, together with the absence of superconductivity in monolayer-trilayer (1313) superstructure, under identical compressive epitaxial strain. The onset superconducting transition temperatures range from 46 to 50 K, exceeding the McMillan limit. Angle-resolved photoemission spectroscopy reveals key Fermi surface differences in these atomically-engineered structures. In superconducting 1212 and 2222 films, a dispersive hole-like band ($γ^{\mathrm{II}}$) forms an underlying Fermi pocket, surrounding the Brillouin zone corner. In contrast, the top of the flat band ($γ^{\mathrm{III}}$) is observed ~70 meV below $E_{\text{F}}$ in the non-superconducting 1313 films. Particularly, the superconducting 2323 films host both $γ^{\mathrm{II}}$ and $γ^{\mathrm{III}}$ bands. The polarization dependence of the ${\hat{I}}^3$ bands reveals their Ni $d_{z^2}$ origin. Our findings expand the family of ambient-pressure nickelate superconductors and establish a connection between structural configuration, electronic structure, and the emergence of superconductivity in nickelates.