Deformed spin-$\frac12$ square lattice in antiferromagnetic NaZnVOPO$_4$(HPO$_4$)

Abstract

We report the structural and magnetic properties of a new spin-$\frac12$ antiferromagnet NaZnVOPO$_4$(HPO$_4$) studied via x-ray diffraction, magnetic susceptibility, high-field magnetization, specific heat, and $^{31}$P nuclear magnetic resonance (NMR) measurements, as well as density-functional band-structure calculations. While thermodynamic properties of this compound are well described by the $J_1-J_2$ square-lattice model, \textit{ab initio} calculations suggest a significant deformation of the spin lattice. From fits to the magnetic susceptibility we determine the averaged nearest-neighbor and second-neighbor exchange couplings of $\bar J_1\simeq -1.3$ K and $\bar J_2\simeq 5.6$ K, respectively. Experimental saturation field of 15.3\,T is consistent with these estimates if 20\% spatial anisotropy in $J_1$ is taken into account. Specific heat data signal the onset of a magnetic long-range order at $T_{\rm N} \simeq 2.1$ K, which is further supported by a sharp peak in the NMR spin-lattice relaxation rate. The NMR spectra mark the superposition of two P lines due to two noneqivalent P sites where the broad line with the strong hyperfine coupling and short $T_1$ is identified as the P(1) site located within the magnetic planes, while the narrow line with the weak hyperfine coupling and long $T_1$ is designated as the P(2) site located between the planes.