Quasi-two-dimensional magnetic correlations in<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi>Ni</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">P</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">S</mml:mi><mml:mn>6</mml:mn></mml:msub></mml:mrow></mml:math>probed by<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mmultiscripts><mml:mi mathvariant="normal">P</mml:mi><mml:mprescripts/><mml:none/><mml:mn>31</mml:mn></mml:mmultiscripts></mml:math>NMR
A. P. Dioguardi, S. Selter, U. Peeck, Saicharan Aswartham, Mihai Sturza, Ramasamy Murugesan, Mohamed S. Eldeeb, Liviu Hozoi, B. Büchner, H.‐J. Grafe
Abstract
Detailed $^{31}\mathrm{P}$ nuclear magnetic resonance (NMR) measurements are presented on well-characterized single-crystals of antiferromagnetic van der Waals ${\mathrm{Ni}}_{2}{\mathrm{P}}_{2}{\mathrm{S}}_{6}$. An anomalous breakdown is observed in the proportionality of the NMR shift $K$ with the bulk susceptibility $\ensuremath{\chi}$. This so-called $K$--$\ensuremath{\chi}$ anomaly occurs in close proximity to the broad peak in $\ensuremath{\chi}(T)$, thereby implying a connection to quasi-two-dimensional (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 $K$--$\ensuremath{\chi}$ anomaly. Appreciable 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 (${T}_{1}^{\ensuremath{-}1}$) measurements indicate little to no magnetic field dependence of the N\'eel temperature. Finally, ${T}_{1}^{\ensuremath{-}1}(T)$ evidences relaxation driven by three-magnon scattering in the antiferromagnetic state.