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

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ID: 326367
2026
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Abstract
Abstract 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 $3d_{z^2}$ 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 $3d_{z^2}$ 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 $3d_{z^2}$-2pz-$3d_{z^2}$ 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.
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Authors Xiaoyang Chen, Wenliang Zhang, Fei Peng, Ting Cui, Guangdi Zhou, Zezhong Li, Jaewon Choi, Lizhi Xu, Yiu-Fung Chiu, Stefano Agrestini, Sahil Tippireddy, Haoliang Huang, Heng Wang, Xianfeng Wu, Peng Li, Jinfeng Jia, Mirian Garcia-Fernandez, Yi Lu, Er‐Jia Guo, Qi-Kun Xue, Zhuoyu Chen, Donglai Feng, Ke-Jin Zhou
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Journal national science review
Year 2026
DOI
10.1093/nsr/nwag518
URL
https://doi.org/10.1093/nsr/nwag518
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