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

Abstract: The spin structure of the spin density wave (SDW) order in the bilayer nickelate La$<em>3$Ni$_2$O$_7$ has been investigated using site-selective $<sup>{17}$O-NMR measurements on the inner apical O(1), outer apical O(2), and planar O(3,4) sites. Below $T</em>{\rm SDW}$ (= 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$<em>2$ planes, the internal field is nearly canceled below $T</em>{\rm SDW}$, indicating an antiparallel spin configuration between adjacent planes. However, below $T_\text{A}$ ($\sim$ 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 $T_{\rm A}$, despite the expected strong interlayer spin coupling between the NiO$<em>2$ 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 $d</em>{3z<sup>2-r<sup>2}$ orbital, indicating a well-developed interlayer spin-singlet formation in the Ni-$d_{3z<sup>2-r<sup>2}$ orbitals bridging the NiO$_2$ planes. These findings shed new light on the interlayer spin-singlet formation and the anomalous spin reconfiguration through the $\text{Ni--O(1)--Ni}$ bonding orbitals connecting the NiO$_2$ planes, which characterize the orbital-selective nature of the bilayer nickelate La$_3$Ni$_2$O$_7$.