- Accepted Paper
Spectroscopic evidence of competing diagonal spin interactions and spin disproportionation in the bilayer nickelate LaNiO
Phys. Rev. X - Accepted 2 November, 2026
DOI: https://doi.org/10.1103/r4pc-2hrt
Phys. Rev. X - Accepted 2 November, 2026
DOI: https://doi.org/10.1103/r4pc-2hrt
A comprehensive spectroscopic map of the electronic, magnetic, and lattice excitations is presented for the bilayer nickelate LaNiO using Raman scattering at ambient pressure. Upon entering the spin density wave state below 153 K, the channel exhibits an abrupt electronic spectral gap with a clear isosbestic point. In contrast, the and channels are dominated by pronounced two-magnon (2M) excitations, representing a signature of incipient Mottness. These 2M signals in both channels constitute evidence for two distinct in-plane spin exchange interactions along the Ni-O bonding and its diagonal directions. Calculations based on the spin wave theory further reveal that the 2M mode in the channel arises from the competition between two bond-diagonal antiferromagnetic interactions mediated by nickel orbitals. Furthermore, emergent low-energy 2M excitations below 10 meV are found to originate from distinct, weaker spin moments, supporting spin disproportionation. Simultaneously, an anomalous softening of phonons from 280 down to 4.5 K is uncovered, suggesting the presence of an incipient lattice instability leading to checkerboard-type breathing modulations. Collectively, these findings identify a ground state of the bilayer nickelate characterized by competing bond-diagonal interactions, spin disproportionation, and an incipient lattice instability, establishing key ingredients for understanding the mechanism of nickelate superconductivity.
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