Long-range antiferromagnetic (AFM) order occurs below 1.5 (Cl), 1.9 (Br and NCS), and 2.5 K more » (I) as determined by heat capacity and muon-spin relaxation. In contrast, terminal X ligands occupy axial positions in 1-4 and cause a staggered packing of adjacent layers. The 2D layered motifs displayed by 1-4 are relevant to bifluoride-bridged EF6 (E = P, Sb), which also possess the same 2D layers. All four compounds consist of two-dimensional (2D) square arrays self-assembled from octahedral NiN4X2 units that are bridged by pyz ligands. The crystal structures of NiX2(pyz)(2) (X = Cl (1), Br (2), I (3), and NCS (4)) were determined by synchrotron X-ray powder diffraction.
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