3 dz 2 orbital delocalization and magnetic collapse in superconducting (La,Pr)3Ni2O7 − δ films

The recent discovery of Ruddlesden-Popper (RP) nickelate thin-film superconductors has opened a new frontier in unconventional superconductivity. Its realization requires both compressive epitaxial strain and highly oxidative growth conditions, yet the microscopic pathway from the parent phase to the superconducting phase remains elusive. Here, X-ray absorption spectra and resonant inelastic X-ray scattering are employed to track this evolution by independently tuning strain and oxygen content in (La,Pr)3Ni2O7 − δ thin films. We uncover a remarkable two-step narrative. First, signatures of delocalization emerge: Spectral weight transfers from a “Upper Hubbard”-like peak to the hole-like peak associated with O 2pz state, and in parallel, the initially localized Ni 3dz² orbital becomes more itinerant followed by the broadening and weakening of dd orbital excitations. Second, as itinerancy increases, long-range spin-density-wave (SDW) order is suppressed in both intensity and correlation length, indicating direct competition with superconductivity. Yet, short-range magnons persist: they become damped but their bandwidth stays unchanged. Our results paint a coherent picture that both strain and oxygenation drive the RP bilayer nickelates towards the superconducting instability, where the O 2pz and Ni 3dz² orbitals become delocalized. Concomitantly, the long-range magnetic order loses coherence and gets suppressed. These findings establish an orbital-selective route to RP nickelate superconductivity, in which the emergence and progressive delocalization of the interlayer 3dz²-2pz-3dz² channel and the robust short-range magnons upon the melting of SDW order are prerequisites, providing strong constraints for theory and the roadmap for designing nickelate superconductors.