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

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 $χ$. This so-called $K$$-$$χ$ anomaly occurs in close proximity to the broad peak in $χ(T)$, 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$$-$$χ$ 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.