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HfNi crystallizes in the orthorhombic Cmcm space group. The structure is three-dimensional. Hf is bonded in a 7-coordinate geometry to seven equivalent Ni atoms. There are a spread of Hf–Ni bond distances ranging from 2.66–2.72 Å. Ni is bonded in a 7-coordinate geometry to seven equivalent Hf atoms.
HfNI crystallizes in the trigonal R-3m space group. The structure is two-dimensional and consists of three HfNI sheets oriented in the (0, 0, 1) direction. Hf4+ is bonded in a 4-coordinate geometry to four equivalent N3- and three equivalent I1- atoms. There are one shorter (2.13 Å) and three longer (2.18 Å) Hf–N bond lengths. All Hf–I bond lengths are 3.07 Å. N3- is bonded to four equivalent Hf4+ atoms to form a mixture of distorted corner and edge-sharing NHf4 trigonal pyramids. I1- is bonded in a 12-coordinate geometry to three equivalent Hf4+ atoms.