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Distinct orbital contributions to electronic and magnetic structures in
Phys. Rev. Research 8, 023119 – Published 4 May, 2026
DOI: https://doi.org/10.1103/7ds6-z5w8
Abstract
High- superconductivity has recently been discovered in Ruddlesden-Popper (RP)-phase nickelates under pressure, where the low-energy electronic structure is dominated by Ni and orbitals. However, the respective roles of these orbitals in superconductivity remain unclear. Here, by combining x-ray absorption, electron energy loss spectroscopy, and density functional theory calculations on single crystals, we identify ligand holes in the orbitals of planar oxygen and the orbitals of apical oxygen, which hybridize with the Ni and orbitals, respectively. These ligand holes enable orbital-selective O -edge resonant inelastic x-ray scattering (RIXS) study, which reveals that states dominate the low-energy charge excitations and are more itinerant. We also observe an bimagnon through RIXS and Raman spectroscopy. Our results reveal distinct contributions of Ni and orbitals to the electronic and magnetic structure and provide direct experimental insights to understand the RP-phase nickelate superconductors.
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References (58)
- H. Sun, M. Huo, X. Hu, J. Li, Z. Liu, Y. Han, L. Tang, Z. Mao, P. Yang, B. Wang, J. Cheng, D.-X. Yao, G.-M. Zhang, and M. Wang, Signatures of superconductivity near 80 K in a nickelate under high pressure, Nature (London) 621, 493 (2023).
- N. Wang, G. Wang, X. Shen, J. Hou, J. Luo, X. Ma, H. Yang, L. Shi, J. Dou, J. Feng, et al., Bulk high-temperature superconductivity in pressurized tetragonal , Nature (London) 634, 579 (2024).
- G. Wang, N. N. Wang, X. L. Shen, J. Hou, L. Ma, L. F. Shi, Z. A. Ren, Y. D. Gu, H. M. Ma, P. T. Yang, Z. Y. Liu, H. Z. Guo, J. P. Sun, G. M. Zhang, S. Calder, J. Q. Yan, B. S. Wang, Y. Uwatoko, and J. G. Cheng, Pressure-induced superconductivity in polycrystalline , Phys. Rev. X 14, 011040 (2024).
- Y. Zhu, D. Peng, E. Zhang, B. Pan, X. Chen, L. Chen, H. Ren, F. Liu, Y. Hao, N. Li, et al., Superconductivity in pressurized trilayer single crystals, Nature (London) 631, 531 (2024).
- X. Huang, H. Zhang, J. Li, M. Huo, J. Chen, Z. Qiu, P. Ma, C. Huang, H. Sun, and M. Wang, Signature of superconductivity in pressurized trilayer-nickelate , Chin. Phys. Lett. 41, 127403 (2024).
- Q. Li, Y.-J. Zhang, Z.-N. Xiang, Y. Zhang, X. Zhu, and H.-H. Wen, Signature of superconductivity in pressurized , Chin. Phys. Lett. 41, 017401 (2024).
- H. Nagata, H. Sakurai, Y. Ueki, K. Yamane, R. Matsumoto, K. Terashima, K. Hirose, H. Ohta, M. Kato, and Y. Takano, Pressure-induced superconductivity in ( = 0.04 and −0.01), J. Phys. Soc. Jpn. 93, 095003 (2024).
- E. K. Ko, Y. Yu, Y. Liu, L. Bhatt, J. Li, V. Thampy, C.-T. Kuo, B. Y. Wang, Y. Lee, K. Lee, J.-S. Lee, B. H. Goodge, D. A. Muller, and H. Y. Hwang, Signatures of ambient pressure superconductivity in thin film , Nature (London) 638, 935 (2025).
- G. Zhou, W. Lv, H. Wang, Z. Nie, Y. Chen, Y. Li, H. Huang, W.-Q. Chen, Y.-J. Sun, Q.-K. Xue, and Z. Chen, Ambient-pressure superconductivity onset above 40 K in films, Nature (London) 640, 641 (2025).
- D. Li, K. Lee, B. Y. Wang, M. Osada, S. Crossley, H. R. Lee, Y. Cui, Y. Hikita, and H. Y. Hwang, Superconductivity in an infinite-layer nickelate, Nature (London) 572, 624 (2019).
- K. Lee, B. Y. Wang, M. Osada, B. H. Goodge, T. C. Wang, Y. Lee, S. Harvey, W. J. Kim, Y. Yu, C. Murthy, et al., Linear-in-temperature resistivity for optimally superconducting (Nd, Sr), Nature (London) 619, 288 (2023).
- C. T. Parzyck, Y. Wu, L. Bhatt, M. Kang, Z. Arthur, T. M. Pedersen, R. Sutarto, S. Fan, J. Pelliciari, V. Bisogni, G. Herranz, A. B. Georgescu, D. G. Hawthorn, L. F. Kourkoutis, D. A. Muller, D. G. Schlom, and K. M. Shen, Superconductivity in the parent infinite-layer nickelate , Phys. Rev. X 15, 021048 (2025).
- S. Zeng, C. S. Tang, X. Yin, C. Li, M. Li, Z. Huang, J. Hu, W. Liu, G. J. Omar, H. Jani, Z. S. Lim, K. Han, D. Wan, P. Yang, S. J. Pennycook, A. T. S. Wee, and A. Ariando, Phase diagram and superconducting dome of infinite-layer thin films, Phys. Rev. Lett. 125, 147003 (2020).
- J. Yang, H. Sun, X. Hu, Y. Xie, T. Miao, H. Luo, H. Chen, B. Liang, W. Zhu, G. Qu, et al., Orbital-dependent electron correlation in double-layer nickelate , Nat. Commun. 15, 4373 (2024).
- H. Li, X. Zhou, T. Nummy, J. Zhang, V. Pardo, W. E. Pickett, J. F. Mitchell, and D. S. Dessau, Fermiology and electron dynamics of trilayer nickelate , Nat. Commun. 8, 704 (2017).
- F. Lechermann, J. Gondolf, S. Bötzel, and I. M. Eremin, Electronic correlations and superconducting instability in under high pressure, Phys. Rev. B 108, L201121 (2023).
- X. Chen, J. Choi, Z. Jiang, J. Mei, K. Jiang, J. Li, S. Agrestini, M. Garcia-Fernandez, H. Sun, X. Huang, D. Shen, M. Wang, J. Hu, Y. Lu, K.-J. Zhou, and D. Feng, Electronic and magnetic excitations in , Nat. Commun. 15, 9597 (2024).
- J. Zhang, D. Phelan, A. S. Botana, Y. S. Chen, H. Zheng, M. Krogstad, S. G. Wang, Y. Qiu, J. A. Rodriguez-Rivera, R. Osborn, S. Rosenkranz, M. R. Norman, and J. F. Mitchell, Intertwined density waves in a metallic nickelate, Nat. Commun. 11, 6003 (2020).
- M. Kakoi, T. Oi, Y. Ohshita, M. Yashima, K. Kuroki, T. Kato, H. Takahashi, S. Ishiwata, Y. Adachi, N. Hatada, T. Uda, and H. Mukuda, Multiband metallic ground state in multilayered nickelates and probed by at ambient pressure, J. Phys. Soc. Jpn. 93, 053702 (2024).
- Y. Meng, Y. Yang, H. Sun, S. Zhang, J. Luo, L. Chen, X. Ma, M. Wang, F. Hong, X. Wang, and X. Yu, Density-wave-like gap evolution in under high pressure revealed by ultrafast optical spectroscopy, Nat. Commun. 15, 10408 (2024).
- Z. Liu, H. Sun, M. Huo, X. Ma, Y. Ji, E. Yi, L. Li, H. Liu, J. Yu, Z. Zhang, et al., Evidence for charge and spin density waves in single crystals of and , Sci. China Phys. Mech. Astron. 66, 217411 (2023).
- S. F. R. TenHuisen, G. A. Pan, Q. Song, D. R. Baykusheva, D. Ferenc Segedin, B. H. Goodge, H. Paik, J. Pelliciari, V. Bisogni, Y. Gu, S. Agrestini, A. Nag, M. García-Fernández, K.-J. Zhou, L. F. Kourkoutis, C. M. Brooks, J. A. Mundy, M. P. M. Dean, and M. Mitrano, Magnetic excitations in Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering, Phys. Rev. B 111, 165145 (2025).
- Y.-B. Liu, J.-W. Mei, F. Ye, W.-Q. Chen, and F. Yang, -wave pairing and the destructive role of apical-oxygen deficiencies in under pressure, Phys. Rev. Lett. 131, 236002 (2023).
- Y. Zhang, L. F. Lin, A. Moreo, T. A. Maier, and E. Dagotto, Structural phase transition, -wave pairing, and magnetic stripe order in bilayered superconductor under pressure, Nat. Commun. 15, 2470 (2024).
- Y. Zhang, L.-F. Lin, A. Moreo, and E. Dagotto, Electronic structure, dimer physics, orbital-selective behavior, and magnetic tendencies in the bilayer nickelate superconductor under pressure, Phys. Rev. B 108, L180510 (2023).
- V. Christiansson, F. Petocchi, and P. Werner, Correlated electronic structure of under pressure, Phys. Rev. Lett. 131, 206501 (2023).
- Z. Luo, B. Lv, M. Wang, W. Wú, and D.-X. Yao, High- superconductivity in based on the bilayer two-orbital –J model, npj Quantum Mater. 9, 61 (2024).
- M. Zhang, H. Sun, Y.-B. Liu, Q. Liu, W.-Q. Chen, and F. Yang, -wave superconductivity in pressurized , Phys. Rev. B 110, L180501 (2024).
- C. Lu, Z. Pan, F. Yang, and C. Wu, Superconductivity in under pressure, Phys. Rev. B 111, 134515 (2025).
- J. Huang and T. Zhou, Interlayer pairing-induced partially gapped Fermi surface in trilayer superconductors, Phys. Rev. B 110, L060506 (2024).
- S. Ryee, N. Witt, and T. O. Wehling, Quenched pair breaking by interlayer correlations as a key to superconductivity in , Phys. Rev. Lett. 133, 096002 (2024).
- X.-Z. Qu, D.-W. Qu, J. Chen, C. Wu, F. Yang, W. Li, and G. Su, Bilayer model and magnetically mediated pairing in the pressurized nickelate , Phys. Rev. Lett. 132, 036502 (2024).
- J. Chen, F. Yang, and W. Li, Orbital-selective superconductivity in the pressurized bilayer nickelate : An infinite projected entangled-pair state study, Phys. Rev. B 110, L041111 (2024).
- Q.-G. Yang, K.-Y. Jiang, D. Wang, H.-Y. Lu, and Q.-H. Wang, Effective model and -wave superconductivity in trilayer nickelate , Phys. Rev. B 109, L220506 (2024).
- Q. Qin and Y.-f. Yang, High- superconductivity by mobilizing local spin singlets and possible route to higher in pressurized , Phys. Rev. B 108, L140504 (2023).
- Z. Dong, M. Huo, J. Li, J. Li, P. Li, H. Sun, L. Gu, Y. Lu, M. Wang, Y. Wang, and Z. Chen, Visualization of oxygen vacancies and self-doped ligand holes in , Nature (London) 630, 847 (2024).
- Z. Dong, G. Wang, N. Wang, W.-H. Dong, L. Gu, Y. Xu, J. Cheng, Z. Chen, and Y. Wang, Interstitial oxygen order and its competition with superconductivity in , Nat. Mater. 24, 1927 (2025).
- N. L. Saini, S. Venkatesh, P. Srivastava, B. R. Sekhar, K. B. Garg, L. H. Tjeng, C. T. Chen, A. Menovsky, and J. J. M. Franse, Polarized x-ray absorption spectroscopy study of the symmetry of unoccupied electronic states near the Fermi level in the system, J. Phys.: Condens. Matter 8, 2467 (1996).
- L. J. P. Ament, M. van Veenendaal, T. P. Devereaux, J. P. Hill, and J. van den Brink, Resonant inelastic x-ray scattering studies of elementary excitations, Rev. Mod. Phys. 83, 705 (2011).
- J. Li, C.-Q. Chen, C. Huang, Y. Han, M. Huo, X. Huang, P. Ma, Z. Qiu, J. Chen, X. Hu, L. Chen, T. Xie, B. Shen, H. Sun, D.-X. Yao, and M. Wang, Structural transition, electric transport, and electronic structures in the compressed trilayer nickelate , Sci. China: Phys. Mech. Astron. 67, 117403 (2024).
- M. Hepting, D. Li, C. J. Jia, H. Lu, E. Paris, Y. Tseng, X. Feng, M. Osada, E. Been, Y. Hikita, et al., Electronic structure of the parent compound of superconducting infinite-layer nickelates, Nat. Mater. 19, 381 (2020).
- I. Timrov, P. Agrawal, X. Zhang, S. Erat, R. Liu, A. Braun, M. Cococcioni, M. Calandra, N. Marzari, and D. Passerone, Electronic structure of pristine and Ni-substituted from near edge x-ray absorption fine structure experiments and first-principles simulations, Phys. Rev. Res. 2, 033265 (2020).
- J. Vinson, J. J. Rehr, J. J. Kas, and E. L. Shirley, Bethe-Salpeter equation calculations of core excitation spectra, Phys. Rev. B 83, 115106 (2011).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/7ds6-z5w8 for sample preparation and characterization, data analysis method of RIXS, XAS, Raman, and DFT calculation and some more detailed results, which includes Refs. [47, 48, 49, 50, 51].
- M. W. Haverkort, Theory of resonant inelastic x-ray scattering by collective magnetic excitations, Phys. Rev. Lett. 105, 167404 (2010).
- S. Goldberg, C. Fadley, and S. Kono, Photoionization cross-sections for atomic orbitals with random and fixed spatial orientation, J. Electron Spectrosc. Relat. Phenom. 21, 285 (1981).
- C. D. Ling, D. N. Argyriou, G. Wu, and J. Neumeier, Neutron diffraction study of : Structural relationships among = 1, 2, and 3 phases , J. Solid State Chem. 152, 517 (2000).
- A. Singh, H. Y. Huang, Y. Y. Chu, C. Y. Hua, S. W. Lin, H. S. Fung, H. W. Shiu, J. Chang, J. H. Li, J. Okamoto, et al., Development of the soft x-ray AGM-AGS RIXS beamline at the Taiwan Photon Source, J. Synchrotron Radiat. 28, 977 (2021).
- G. Kresse and J. Furthmüller, Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set, Comput. Mater. Sci. 6, 15 (1996).
- G. Kresse and J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set, Phys. Rev. B 54, 11169 (1996).
- J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
- S. Deswal, D. Kumar, D. Rout, S. Singh, and P. Kumar, Dynamics of electron-electron correlated to electron-phonon coupled phase progression in trilayer nickelate , Appl. Phys. Lett. 127, 071903 (2025).
- L. J. P. Ament, G. Ghiringhelli, M. M. Sala, L. Braicovich, and J. van den Brink, Theoretical demonstration of how the dispersion of magnetic excitations in cuprate compounds can be determined using resonant inelastic x-ray scattering, Phys. Rev. Lett. 103, 117003 (2009).
- V. Bisogni, L. Simonelli, L. J. P. Ament, F. Forte, M. Moretti Sala, M. Minola, S. Huotari, J. van den Brink, G. Ghiringhelli, N. B. Brookes, and L. Braicovich, Bimagnon studies in cuprates with resonant inelastic x-ray scattering at the O K edge. I. Assessment on and comparison with the excitation at Cu and Cu edges, Phys. Rev. B 85, 214527 (2012).
- R. R. P. Singh, P. A. Fleury, K. B. Lyons, and P. E. Sulewski, Quantitative determination of quantum fluctuations in the spin-1/2 planar antiferromagnet, Phys. Rev. Lett. 62, 2736 (1989).
- C.-Q. Chen, Z. Luo, M. Wang, W. Wú, and D.-X. Yao, Trilayer multiorbital models of , Phys. Rev. B 110, 014503 (2024).
- U. Kumar, C. Melnick, and G. Kotliar, Softening of excitation in the resonant inelastic x-ray scattering spectra as a signature of Hund’s coupling in nickelates, Phys. Rev. Res. 7, L012066 (2025).
- T. Xie, M. Huo, X. Ni, F. Shen, X. Huang, H. Sun, H. C. Walker, D. Adroja, D. Yu, B. Shen, L. He, K. Cao, and M. Wang, Strong interlayer magnetic exchange coupling in revealed by inelastic neutron scattering, Sci. Bull. 69, 3221 (2024).