Data for Spatially-anisotropic S = 1 square-lattice antiferromagnet with single-ion anisotropy realized in a Ni(II) Pyrazine-N,N’-dioxide (pyzdo) coordination polymer

This conclusion is based upon considering in concert the experimental probes X-ray diffraction, magnetic susceptibility, magnetic-field-dependent heat capacity, muon-spin relaxation, neutron diffraction, neutron spectroscopy, and pulsed field magnetization. Long range antiferromagnetic order develops at TN = 18.5 K. Although the samples are polycrystalline, there is an observable spin-flop transition and saturation of the magnetization at ≈80 T. Linear spin-wave theory yields spatially-anisotropic exchanges within an antiferromagnetic square lattice, Jx = 0.235 meV, Jy = 2.014 meV, and an easy-axis single-ion anisotropy D = −1.622 meV (after renormalization).

The anisotropy of the exchanges is supported by density functional theory.<br><br>Dataset to support a paper accepted in Physical Review B.