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Hf2MnOs crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Hf2MnOs ribbons oriented in the (1, 0, 0) direction. Hf is bonded in a linear geometry to one Mn and one Os atom. The Hf–Mn bond length is 2.62 Å. The Hf–Os bond length is 2.30 Å. Mn is bonded in a linear geometry to two equivalent Hf atoms. Os is bonded in a linear geometry to two equivalent Hf atoms.
Hf2MnOs is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Hf is bonded in a body-centered cubic geometry to four equivalent Mn and four equivalent Os atoms. All Hf–Mn bond lengths are 2.78 Å. All Hf–Os bond lengths are 2.78 Å. Mn is bonded in a distorted body-centered cubic geometry to eight equivalent Hf and six equivalent Os atoms. All Mn–Os bond lengths are 3.21 Å. Os is bonded in a body-centered cubic geometry to eight equivalent Hf and six equivalent Mn atoms.