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Detailed ${}^{31}$P nuclear magnetic resonance (NMR) measurements arepresented on well-characterized single crystals of antiferromagnetic van derWaals Ni$_2$P$_2$S$_6$. An anomalous breakdown is observed in theproportionality of the NMR shift $K$ with the bulk susceptibility $\chi$. Thisso-called $K$$-$$\chi$ anomaly occurs in close proximity to the broad peak in$\chi(T)$, thereby implying a connection to quasi-2D magnetic correlationsknown to be responsible for this maximum. Quantum chemistry calculations showthat crystal field energy level depopulation effects cannot be responsible forthe $K$$-$$\chi$ anomaly. Appreciable in-plane transferred hyperfine couplingis observed, which is consistent with the proposed Ni$-$S$-$Ni super- andNi$-$S$-$S$-$Ni super-super-exchange coupling mechanisms. Magnetization andspin$-$lattice relaxation rate ($T_1^{-1}$) measurements indicate little to nomagnetic field dependence of the N\'eel temperature. Finally, $T_1^{-1}(T)$evidences relaxation driven by three-magnon scattering in the antiferromagneticstate.

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