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Orbital-Selective Coexistence of Interlayer Spin-Singlet Formation and SDW Order with Anomalous Spin Reconfiguration in Bilayer Nickelate La3Ni2O7 Revealed by 17O-NMR

Abstract

The spin structure of the spin density wave (SDW) order in the bilayer nickelate La3Ni2O7 has been investigated using site-selective 17O-NMR measurements on the inner apical O(1), outer apical O(2), and planar O(3,4) sites. Below TSDW (= 150 K), the peak of all planar O(3,4) sites significantly broadens due to the emergence of a finite internal magnetic field, whereas O(2) sites remain with no (or a negligibly small) internal field. These results are consistent with commensurate SDW order with a single spin-spinless (or large-tiny spin) stripe. As for the O(1) sites that bridge the NiO2 planes, the internal field is nearly canceled below TSDW, indicating an antiparallel spin configuration between adjacent planes. However, below TA (∼ 115 K), the spectrum of the O(1) site disappears even though the in-plane SDW order remains robust, implying that the antiparallel spin configuration through the Ni--O(1)--Ni bond is not particularly stable below TA, despite the expected strong interlayer spin coupling between the NiO2 planes. Above all, we emphasize that the local spin susceptibility is extremely small at the O(2) site that has a strong covalency with the d3z2−r2 orbital, indicating a well-developed interlayer spin-singlet formation in the Ni-d3z2−r2 orbitals bridging the NiO2 planes. These findings shed new light on the interlayer spin-singlet formation and the anomalous spin reconfiguration through the Ni−−O(1)−−Ni bonding orbitals connecting the NiO2 planes, which characterize the orbital-selective nature of the bilayer nickelate La3Ni2O7.

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BibTeX
@misc{lee2026orbitalselective,
  title = {{Orbital-Selective Coexistence of Interlayer Spin-Singlet Formation and SDW Order with Anomalous Spin Reconfiguration in Bilayer Nickelate La$_3$Ni$_2$O$_7$ Revealed by $^17$O-NMR}},
  author = {H. Lee and M. Yashima and M. Kakoi and T. Ino and Y. Arai and K. Kitagawa and H. Sakurai and Y. Takano and K. Kuroki and H. Mukuda},
  howpublished = {arXiv},
  year = {2026},
  month = aug,
  doi = {10.48550/arxiv.2608.27917},
  eprint = {2608.27917},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2608.27917},
}
RIS
TY  - UNPB
TI  - Orbital-Selective Coexistence of Interlayer Spin-Singlet Formation and SDW Order with Anomalous Spin Reconfiguration in Bilayer Nickelate La_3Ni_2O_7 Revealed by ^17O-NMR
AU  - H. Lee
AU  - M. Yashima
AU  - M. Kakoi
AU  - T. Ino
AU  - Y. Arai
AU  - K. Kitagawa
AU  - H. Sakurai
AU  - Y. Takano
AU  - K. Kuroki
AU  - H. Mukuda
PY  - 2026
DA  - 2026/08/28
PB  - arXiv
DO  - 10.48550/arxiv.2608.27917
UR  - https://arxiv.org/abs/2608.27917
AB  - The spin structure of the spin density wave (SDW) order in the bilayer nickelate La_3Ni_2O_7 has been investigated using site-selective ^17O-NMR measurements on the inner apical O(1), outer apical O(2), and planar O(3,4) sites. Below T_SDW (= 150 K), the peak of all planar O(3,4) sites significantly broadens due to the emergence of a finite internal magnetic field, whereas O(2) sites remain with no (or a negligibly small) internal field. These results are consistent with commensurate SDW order with a single spin-spinless (or large-tiny spin) stripe. As for the O(1) sites that bridge the NiO_2 planes, the internal field is nearly canceled below T_SDW, indicating an antiparallel spin configuration between adjacent planes. However, below T_A (∼ 115 K), the spectrum of the O(1) site disappears even though the in-plane SDW order remains robust, implying that the antiparallel spin configuration through the Ni--O(1)--Ni bond is not particularly stable below T_A, despite the expected strong interlayer spin coupling between the NiO_2 planes. Above all, we emphasize that the local spin susceptibility is extremely small at the O(2) site that has a strong covalency with the d_3z^2−r^2 orbital, indicating a well-developed interlayer spin-singlet formation in the Ni-d_3z^2−r^2 orbitals bridging the NiO_2 planes. These findings shed new light on the interlayer spin-singlet formation and the anomalous spin reconfiguration through the Ni−−O(1)−−Ni bonding orbitals connecting the NiO_2 planes, which characterize the orbital-selective nature of the bilayer nickelate La_3Ni_2O_7.
ER  -