3dz2 orbital delocalization and magnetic collapse in superconducting (La,Pr)3Ni2O7-δ films
10 affiliations
- 1Diamond Light Source, Harwell Campus, Didcot OX11 0DE, UK.
- 2National Synchrotron Radiation Laboratory and School of Nuclear Science and Technology, University of Science and Technology of China, Hefei 230026, China.
- 3State Key Laboratory of Quantum Functional Materials, Department of Physics, Guangdong Provincial Key Laboratory of Topological Matter, and Guangdong Basic Research Center of Excellence for Quantum Science, Southern University of Science and Technology, Shenzhen 518055, China.
- 4Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
- 5Department of Physics & Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.
- 6Quantum Science Center of Guangdong-Hong Kong-Macao Greater Bay Area, Shenzhen 518045, China.
- 7Department of Physics, University of Oxford, Clarendon Laboratory, Parks Road, Oxford OX1 3PU, UK.
- 8National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University, Nanjing 210093, China.
- 9Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, China.
- 10New Cornerstone Laboratory, Hefei National Laboratory, Hefei 230088, China.
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)\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 3\end{document}Ni\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 2\end{document}O\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 7−δ \end{document} thin films. We uncover a remarkable two-step narrative. First, signatures of delocalization emerge: spectral weight transfers from an ‘Upper Hubbard’-like peak to the hole-like peak associated with O \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 2pz\end{document} state, and in parallel, the initially localized Ni \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 3dz2\end{document} orbital becomes more itinerant followed by the broadening and weakening of d–d 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 toward the superconducting instability, where the O \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 2pz\end{document} and Ni \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 3dz2\end{document} 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 \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 3dz2\end{document}–\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 2pz\end{document}–\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 3dz2\end{document} 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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BibTeX
@article{chen20263dz2,
title = {{3dz2 orbital delocalization and magnetic collapse in superconducting (La,Pr)3Ni2O7-δ films}},
author = {Xiaoyang Chen and Wenliang Zhang and Fei Peng and Ting Cui and Guangdi Zhou and Zezhong Li and Jaewon Choi and Lizhi Xu and Yiu-Fung Chiu and Stefano Agrestini and Sahil Tippireddy and Haoliang Huang and Heng Wang and Xianfeng Wu and Peng Li and Jin-Feng Jia and Mirian Garcia-Fernandez and Yi Lu and Er-Jia Guo and Qi-Kun Xue and Zhuoyu Chen and Donglai Feng and Ke-Jin Zhou},
journal = {National science review},
year = {2026},
month = aug,
doi = {10.1093/nsr/nwag518},
url = {https://europepmc.org/article/PMC/PMC13725838},
note = {CC BY},
}
RIS
TY - JOUR
TI - 3dz2 orbital delocalization and magnetic collapse in superconducting (La,Pr)3Ni2O7-δ films
AU - Xiaoyang Chen
AU - Wenliang Zhang
AU - Fei Peng
AU - Ting Cui
AU - Guangdi Zhou
AU - Zezhong Li
AU - Jaewon Choi
AU - Lizhi Xu
AU - Yiu-Fung Chiu
AU - Stefano Agrestini
AU - Sahil Tippireddy
AU - Haoliang Huang
AU - Heng Wang
AU - Xianfeng Wu
AU - Peng Li
AU - Jin-Feng Jia
AU - Mirian Garcia-Fernandez
AU - Yi Lu
AU - Er-Jia Guo
AU - Qi-Kun Xue
AU - Zhuoyu Chen
AU - Donglai Feng
AU - Ke-Jin Zhou
PY - 2026
DA - 2026/08/25
JO - National science review
DO - 10.1093/nsr/nwag518
UR - https://europepmc.org/article/PMC/PMC13725838
AB - 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)\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} _3\end{document}Ni\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} _2\end{document}O\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} _7−δ \end{document} thin films. We uncover a remarkable two-step narrative. First, signatures of delocalization emerge: spectral weight transfers from an ‘Upper Hubbard’-like peak to the hole-like peak associated with O \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 2p_z\end{document} state, and in parallel, the initially localized Ni \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 3d_z^2\end{document} orbital becomes more itinerant followed by the broadening and weakening of d–d 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 toward the superconducting instability, where the O \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 2p_z\end{document} and Ni \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 3d_z^2\end{document} 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 \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 3d_z^2\end{document}–\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 2p_z\end{document}–\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{upgreek} \usepackage{mathrsfs} \setlength{\oddsidemargin}{-69pt} \begin{document} 3d_z^2\end{document} 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.
SN - 2095-5138
SN - 2053-714X
ER -