Quasi-2D magnetic correlations in Ni${}_2$P${}_2$S${}_6$ probed by ${}^{31}$P NMR

Abstract

Detailed ${}^{31}$P nuclear magnetic resonance (NMR) measurements are presented on well-characterized single crystals of antiferromagnetic van der Waals Ni${}_2$P${}_2$S${}_6$. An anomalous breakdown is observed in the proportionality of the NMR shift $K$ with the bulk susceptibility $\chi$. This so-called $K$$-$$\chi$ anomaly occurs in close proximity to the broad peak in $\chi (T)$, thereby implying a connection to quasi-2D magnetic correlations known to be responsible for this maximum. Quantum chemistry calculations show that crystal field energy level depopulation effects cannot be responsible for the $K$$-$$\chi$ anomaly. Appreciable in-plane transferred hyperfine coupling is observed, which is consistent with the proposed Ni$-$S$-$Ni super- and Ni$-$S$-$S$-$Ni super-super-exchange coupling mechanisms. Magnetization and spin$-$lattice relaxation rate ($T_1^{-1}$) measurements indicate little to no magnetic field dependence of the Néel temperature. Finally, $T_1^{-1}(T)$ evidences relaxation driven by three-magnon scattering in the antiferromagnetic state.

arXiv comment16 pages, 16 figures, submitted to Phys. Rev. B

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• Crystal Growth and Anisotropic Magnetic Properties of Quasi-2D (Fe${}_{1-x}$Ni${}_x$)${}_2$P${}_2$S${}_6$
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• Spin liquid state in a rare-earth hyperkagome lattice
• Low-energy excitations and magnetic anisotropy of the layered van der Waals antiferromagnet Ni${}_2$P${}_2$S${}_6$
• Understanding and tuning magnetism in layered Ising-type antiferromagnet FePSe3 for potential 2D magnet
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