Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Letter
  • Open Access

Effect of Pr-doping and oxygen vacancies on spin density wave in La3Ni2O7−δ: A µSR investigation

Kaiwen Chen1,*, Xiangqi Liu2,*, Ying Wang1,*, Jiyuan Han1, Ziyi Zhu3, Jiachen Jiao1, Chengyu Jiang1, Yanfeng Guo2,4, Changlin Zheng1 et al.

Lei Shu1,5,†

  • 1State Key Laboratory of Surface Physics, Department of Physics, Fudan University, Shanghai 200438, China
  • 2School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
  • 3School of Materials, Zhengzhou University of Aeronautics, Zhengzhou 450046, China
  • 4ShanghaiTech Laboratory for Topological Physics, Shanghai 201210, China
  • 5Shanghai Research Center for Quantum Sciences, Shanghai 201315, China

  • *These authors contributed equally to this work.
  • †Contact author: leishu@fudan.edu.cn

Phys. Rev. Research 7, L032014 – Published 15 July, 2025

DOI: https://doi.org/10.1103/blkt-x2ps

Abstract

Here we report the positive muon spin relaxation study on Pr-doped La1.9Pr1.1Ni2O6.97 and oxygen-deficient La3Ni2O6.63 polycrystalline under ambient pressure. Zero-field μ+SR experiments reveal the existence of bulk long-range magnetic order in La1.9Pr1.1Ni2O6.97 with TN=161K, while La3Ni2O6.63 exhibits a short-range magnetic ground state with TN=15K. The microscopic magnetism of La1.9Pr1.1Ni2O6.97 is similar to the La3Ni2O7 with ideal stoichiometry. A comparison with lightly oxygen-deficient La3Ni2O6.92 reveals a crossover in magnetic dimensionality from three dimensional in La1.9Pr1.1Ni2O6.97 to two dimensional in La3Ni2O6.92. Our μ+SR experimental results reveal the destructive effect of apical-oxygen deficiencies on both intraplane and interplane magnetic correlation. On the other hand, Pr doping does not significantly alter the microscopic magnetism of La3Ni2O7.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (51)

  1. 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).
  2. Y. Zhu, D. Peng, E. Zhang, B. Pan, X. Chen, L. Chen, H. Ren, F. Liu, Y. Hao, N. Li, Z. Xing, F. Lan, J. Han, J. Wang, D. Jia, H. Wo, Y. Gu, Y. Gu, L. Ji, W. Wang, H. Gou, Y. Shen, T. Ying, X. Chen, W. Yang, H. Cao, C. Zheng, Q. Zeng, J.-g. Guo, and J. Zhao, Superconductivity in pressurized trilayer La4Ni3O10−δ single crystals, Nature (London) 631, 531 (2024).
  3. Q. Li, Y.-J. Zhang, Z.-N. Xiang, Y. Zhang, X. Zhu, and H.-H. Wen, Signature of superconductivity in pressurized La4Ni3O10, Chin. Phys. Lett. 41, 017401 (2024).
  4. H. Sakakibara, M. Ochi, H. Nagata, Y. Ueki, H. Sakurai, R. Matsumoto, K. Terashima, K. Hirose, H. Ohta, M. Kato, Y. Takano, and K. Kuroki, Theoretical analysis on the possibility of superconductivity in the trilayer Ruddlesden-Popper nickelate La4Ni3O10 under pressure and its experimental examination: Comparison with La3Ni2O7, Phys. Rev. B 109, 144511 (2024).
  5. M. Zhang, C. Pei, D. Peng, X. Du, W. Hu, Y. Cao, Q. Wang, J. Wu, Y. Li, H. Liu, C. Wen, J. Song, Y. Zhao, C. Li, W. Cao, S. Zhu, Q. Zhang, N. Yu, P. Cheng, L. Zhang, Z. Li, J. Zhao, Y. Chen, C. Jin, H. Guo, C. Wu, F. Yang, Q. Zeng, S. Yan, L. Yang, and Y. Qi, Superconductivity in trilayer nickelate La4Ni3O10 under pressure, Phys. Rev. X 15, 021005 (2025).
  6. 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 La4Ni3O10, Sci. China: Phys. Mech. Astron. 67, 117403 (2024).
  7. 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 Pr4Ni3O10−δ, Chin. Phys. Lett. 41, 127403 (2024).
  8. M. Wang, H.-H. Wen, T. Wu, D.-X. Yao, and T. Xiang, Normal and superconducting properties of La3Ni2O7, Chin. Phys. Lett. 41, 077402 (2024).
  9. 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 La3Ni2O7, Nat. Commun. 15, 9597 (2024).
  10. R. Khasanov, T. J. Hicken, D. J. Gawryluk, V. Sazgari, I. Plokhikh, L. P. Sorel, M. Bartkowiak, S. Bötzel, F. Lechermann, I. M. Eremin, H. Luetkens, and Z. Guguchia, Pressure-enhanced splitting of density wave transitions in La3Ni2O7−δ, Nat. Phys. 21, 430 (2025).
  11. K. Chen, X. Liu, J. Jiao, M. Zou, C. Jiang, X. Li, Y. Luo, Q. Wu, N. Zhang, Y. Guo, and L. Shu, Evidence of spin density waves in La3Ni2O7−δ, Phys. Rev. Lett. 132, 256503 (2024).
  12. D. Zhao, Y. Zhou, M. Huo, Y. Wang, L. Nie, Y. Yang, J. Ying, M. Wang, T. Wu, and X. Chen, Pressure-enhanced spin-density-wave transition in double-layer nickelate La3Ni2O7−δ, Sci. Bull. 70, 1239 (2025).
  13. 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 La3Ni2O7−δ revealed by inelastic neutron scattering, Sci. Bull. 69, 3221 (2024).
  14. C. D. Ling, D. N. Argyriou, G. Wu, and J. J. Neumeier, Neutron diffraction study of La3Ni2O7: Structural relationships among n = 1, 2, and 3 phases Lan+1NinO3n+1, J. Solid State Chem. 152, 517 (2000).
  15. I. Plokhikh, T. J. Hicken, L. Keller, V. Pomjakushin, S. H. Moody, P. Foury-Leylekian, J. J. Krieger, H. Luetkens, Z. Guguchia, R. Khasanov, and D. J. Gawryluk, Unraveling spin density wave order in layered nickelates La3Ni2O7 and La2PrNi2O7 via neutron diffraction, arXiv:2503.05287.
  16. N. Wang, G. Wang, X. Shen, J. Hou, J. Luo, X. Ma, H. Yang, L. Shi, J. Dou, J. Feng, J. Yang, Y. Shi, Z. Ren, H. Ma, P. Yang, Z. Liu, Y. Liu, H. Zhang, X. Dong, Y. Wang, K. Jiang, J. Hu, S. Nagasaki, K. Kitagawa, S. Calder, J. Yan, J. Sun, B. Wang, R. Zhou, Y. Uwatoko, and J. Cheng, Bulk high-temperature superconductivity in pressurized tetragonal La2PrNi2O7, Nature (London) 634, 579 (2024).
  17. Y. Zhang, D. Su, Y. Huang, Z. Shan, H. Sun, M. Huo, K. Ye, J. Zhang, Z. Yang, Y. Xu, Y. Su, R. Li, M. Smidman, M. Wang, L. Jiao, and H. Yuan, High-temperature superconductivity with zero resistance and strange-metal behaviour in La3Ni2O7−δ, Nat. Phys. 20, 1269 (2024).
  18. J. Li, D. Peng, P. Ma, H. Zhang, Z. Xing, X. Huang, C. Huang, M. Huo, D. Hu, Z. Dong, X. Chen, T. Xie, H. Dong, H. Sun, Q. Zeng, H.-K. Mao, and M. Wang, Identification of superconductivity in bilayer nickelate La3Ni2O7 under high pressure up to 100 GPa, Natl. Sci. Rev. nwaf220 (2025).
  19. Y.-B. Liu, J.-W. Mei, F. Ye, W.-Q. Chen, and F. Yang, s±-wave pairing and the destructive role of apical-oxygen deficiencies in La3Ni2O7 under pressure, Phys. Rev. Lett. 131, 236002 (2023).
  20. Q. Qin and Y.-f. Yang, High-Tc superconductivity by mobilizing local spin singlets and possible route to higher Tc in pressurized La3Ni2O7, Phys. Rev. B 108, L140504 (2023).
  21. H. Sakakibara, N. Kitamine, M. Ochi, and K. Kuroki, Possible high Tc superconductivity in La3Ni2O7 under high pressure through manifestation of a nearly half-filled bilayer Hubbard model, Phys. Rev. Lett. 132, 106002 (2024).
  22. Y. Shen, M. Qin, and G.-M. Zhang, Effective Bi-layer model Hamiltonian and density-matrix renormalization group study for the high-Tc superconductivity in La3Ni2O7 under high pressure, Chin. Phys. Lett. 40, 127401 (2023).
  23. J.-R. Xue and F. Wang, Magnetism and superconductivity in the t–J model of La3Ni2O7 Under multiband Gutzwiller approximation, Chin. Phys. Lett. 41, 057403 (2024).
  24. Q.-G. Yang, D. Wang, and Q.-H. Wang, Possible s±-wave superconductivity in La3Ni2O7, Phys. Rev. B 108, L140505 (2023).
  25. Y.-f. Yang, G.-M. Zhang, and F.-C. Zhang, Interlayer valence bonds and two-component theory for high-Tc superconductivity of La3Ni2O7 under pressure, Phys. Rev. B 108, L201108 (2023).
  26. Y. Zhang, L.-F. Lin, A. Moreo, T. A. Maier, and E. Dagotto, Trends in electronic structures and s±-wave pairing for the rare-earth series in bilayer nickelate superconductor R3Ni2O7, Phys. Rev. B 108, 165141 (2023).
  27. Z. Luo, B. Lv, M. Wang, W. Wú, and D.-X. Yao, High-Tc superconductivity in La3Ni2O7 based on the bilayer two-orbital t−J model, npj Quantum Mater. 9, 61 (2024).
  28. Z. Fan, J.-F. Zhang, B. Zhan, D. Lv, X.-Y. Jiang, B. Normand, and T. Xiang, Superconductivity in nickelate and cuprate superconductors with strong bilayer coupling, Phys. Rev. B 110, 024514 (2024).
  29. G. Heier, K. Park, and S. Y. Savrasov, Competing dxy and s± pairing symmetries in superconducting La3Ni2O7: LDA+FLEX calculations, Phys. Rev. B 109, 104508 (2024).
  30. K. Jiang, Z. Wang, and F.-C. Zhang, High-temperature superconductivity in La3Ni2O7, Chin. Phys. Lett. 41, 017402 (2024).
  31. C. Xia, H. Liu, S. Zhou, and H. Chen, Sensitive dependence of pairing symmetry on Ni-eg crystal field splitting in the nickelate superconductor La3Ni2O7, Nat. Commun. 16, 1054 (2025).
  32. F. Lechermann, J. Gondolf, S. Bötzel, and I. M. Eremin, Electronic correlations and superconducting instability in La3Ni2O7 under high pressure, Phys. Rev. B 108, L201121 (2023).
  33. 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 La3Ni2O7−δ, Nature (London) 630, 847 (2024).
  34. J. Hou, P.-T. Yang, Z.-Y. Liu, J.-Y. Li, P.-F. Shan, L. Ma, G. Wang, N.-N. Wang, H.-Z. Guo, J.-P. Sun, Y. Uwatoko, M. Wang, G.-M. Zhang, B.-S. Wang, and J.-G. Cheng, Emergence of high-temperature superconducting phase in pressurized La3Ni2O7 crystals, Chin. Phys. Lett. 40, 117302 (2023).
  35. Y. Zhou, J. Guo, S. Cai, H. Sun, C. Li, J. Zhao, P. Wang, J. Han, X. Chen, Y. Chen, Q. Wu, Y. Ding, T. Xiang, H.-K. Mao, and L. Sun, Investigations of key issues on the reproducibility of high-Tc superconductivity emerging from compressed La3Ni2O7, Matter Radiat. Extrem. 10, 027801 (2025).
  36. 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 La3Ni2O7−δ, Phys. Rev. X 14, 011040 (2024).
  37. R. Gao, L. Jin, S. Huyan, D. Ni, H. Wang, X. Xu, S. L. Bud'ko, P. Canfield, W. Xie, and R. J. Cava, Is La3Ni2O6.5 a bulk superconducting nickelate? ACS Appl. Mater. Interfaces 16, 66857 (2024).
  38. A. D. Hillier, S. J. Blundell, I. McKenzie, I. Umegaki, L. Shu, J. A. Wright, T. Prokscha, F. Bert, K. Shimomura, A. Berlie, H. Alberto, and I. Watanabe, Muon spin spectroscopy, Nat. Rev. Methods Primers 2, 4 (2022).
  39. S. J. Blundell, Spin-polarized muons in condensed matter physics, Contemp. Phys. 40, 175 (1999).
  40. A. Yaouanc and P. D. de Réotier, Muon Spin Rotation, Relaxation, and Resonance: Applications to Condensed Matter (Oxford University Press, Oxford, UK, 2011).
  41. R. S. Hayano, Y. J. Uemura, J. Imazato, N. Nishida, T. Yamazaki, and R. Kubo, Zero-and low-field spin relaxation studied by positive muons, Phys. Rev. B 20, 850 (1979).
  42. See Supplemental Material at http://link.aps.org/supplemental/10.1103/blkt-x2ps for more details of sample characterization and analysis of ZF-, wTF- and LF- µSR results.
  43. N. Mott, Conduction in glasses containing transition metal ions, J. Non-Cryst. Solids 1, 1 (1968).
  44. J. Sugiyama, M. Månsson, Y. Ikedo, T. Goko, K. Mukai, D. Andreica, A. Amato, K. Ariyoshi, and T. Ohzuku, μ+SR investigation of local magnetic order in LiCrO2, Phys. Rev. B 79, 184411 (2009).
  45. T. Saito, A. Oosawa, T. Goto, T. Suzuki, and I. Watanabe, Muon spin rotation and relaxation studies on the solid solution of the two spin-gap systems (CH3)2CHNH3−CuCl3 and (CH3)2CHNH3−CuBr3, Phys. Rev. B 74, 134423 (2006).
  46. A. L. Talapov and H. W. J. Blöte, The magnetization of the 3D Ising model, J. Phys. A: Math. Gen. 29, 5727 (1996).
  47. R. Khasanov, I. Plokhikh, T. J. Hicken, H. Luetkens, D. J. Gawryluk, and Z. Guguchia, Pressure effect on the spin density wave transition in La2PrNi2O6.96, Phys. Rev. Res. 7, L022046 (2025).
  48. K. H. Chow, P. A. Pattenden, S. J. Blundell, W. Hayes, F. L. Pratt, T. Jestädt, M. A. Green, J. E. Millburn, M. J. Rosseinsky, B. Hitti, S. R. Dunsiger, R. F. Kiefl, C. Chen, and A. J. S. Chowdhury, Muon-spin-relaxation studies of magnetic order in heavily doped La2−xSrxNiO4+δ, Phys. Rev. B 53, R14725 (1996).
  49. T. Jestädt, K. H. Chow, S. J. Blundell, W. Hayes, F. L. Pratt, B. W. Lovett, M. A. Green, J. E. Millburn, and M. J. Rosseinsky, Temperature and doping-level dependence of magnetic order in La2−xSrxNiO4+δ studied by muon spin rotation, Phys. Rev. B 59, 3775 (1999).
  50. R. Khasanov, T. J. Hicken, I. Plokhikh, V. Sazgari, L. Keller, V. Pomjakushin, M. Bartkowiak, S. Królak, M. J. Winiarski, and J. A. Krieger, Identical suppression of spin and charge density wave transitions in La4Ni3O10 by pressure, arXiv:2503.04400.
  51. X.-S. Ni, Y. Ji, Li. He, T. Xie, D.-X. Yao, M. Wang, and K. Cao, Spin density wave in the bilayered nickelate La3Ni2O7−δ at ambient pressure, npj Quantum Mater. 10, 17 (2025).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation