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Updated: Aug 5, 2026

Thermochemical Studies of Ni(II) and Zn(II) Ternary Complexes Using Ion Mobility-Mass Spectrometry
Published on: June 8, 2022
Microscopic Evidence for a Zhang-Rice Triplet State in the van der Waals Antiferromagnet, NiPS_{3}
Beom Hyun Kim1,2, Youjin Lee1,2, Junik Hwang3
1Seoul National University, Center for Quantum Materials, Seoul 08826, Republic of Korea.
Abstract:
Quantum-entangled states underpin many emergent phenomena in quantum materials, yet their direct experimental identification remains a challenge. NiPS_{3}, a van der Waals antiferromagnet exhibiting a resolution-limited magnetic exciton in its ordered phase, has been proposed to host a many-body entangled Zhang-Rice triplet state. Here, using ^{33}S nuclear magnetic resonance (NMR) on ^{33}S-enriched NiPS_{3} single crystals, we provide microscopic evidence for this charge-transfer state. The ^{33}S and ^{31}P Knight shifts as a function of temperature reveal a unified spin-triplet configuration arising from strong hybridization between a self-doped hole in the S 3p orbitals and a hole in Ni 3d orbitals. Furthermore, the ^{33}S nuclear spin-lattice relaxation rate exhibits a power-law divergence as it approaches the Néel temperature T_{N}=155 K, indicating critical slowing down of collective charge fluctuations consistent with spin-nematic correlations. These results reveal a spin-charge-intertwined ground state and establish the microscopic foundation for the exceptional coherence of the magnetic exciton in NiPS_{3}.
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