Summary: | The Ni(NCS)<sub>2</sub> (pyzdo)<sub>2</sub> coordination polymer is found to be an <i>S</i> = 1 spatially anisotropic square lattice with easy-axis single-ion anisotropy. 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 (AFM) order develops at <i>T</i><sub><i>N</i></sub> = 18.5K. 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 AFM square lattice, <i>J</i><sub><i>x</i></sub> =0.235 meV, <i>J</i><sub><i>y</i></sub> =2.014 meV, and an easy-axis single-ion anisotropy <i>D</i> = −1.622 meV (after renormalization). The anisotropy of the exchanges is supported by density functional theory.
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