Low-energy excitations and magnetic anisotropy of the layered van der Waals antiferromagnet Ni2P2S6

Abstract

The quasi-two-dimensional antiferromagnet Ni$_2$P$_2$S$_6$ belongs to the family of magnetic van der Waals compounds that provides a rich material base for the realization of fundamental models of quantum magnetism in low dimensions. Here, we report high-frequency/high-magnetic field electron spin resonance measurements on single crystals of Ni$_2$P$_2$S$_6$. The results enable to reliably determine the positive, 'easy'-plane type of the single ion anisotropy of the Ni$^{2+}$ ions with the upper limit of its magnitude $\lesssim 0.7$ meV. The resonance response reveals strongly anisotropic spin fluctuations setting in shortly above the N\'eel temperature $T_{\rm N} = 158$ K and extending in the antiferromagnetically ordered state down to low temperatures. There, a new low-energy magnon excitation gapped from the ground state by only $\sim 1$ meV was found. This magnon mode may explain unusual low temperature relaxation processes observed in a latest nuclear magnetic resonance experiments and together with the estimate of the single ion anisotropy they should enable setting up a realistic spin model for an accurate description of magnetic properties of Ni$_2$P$_2$S$_6$.