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Ti2VOs crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Ti2VOs ribbons oriented in the (1, 0, 0) direction. Ti is bonded in a linear geometry to one V and one Os atom. The Ti–V bond length is 2.10 Å. The Ti–Os bond length is 2.21 Å. V is bonded in a linear geometry to two equivalent Ti atoms. Os is bonded in a linear geometry to two equivalent Ti atoms.
Ti2VOs is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ti is bonded in a distorted body-centered cubic geometry to four equivalent V and four equivalent Os atoms. All Ti–V bond lengths are 2.70 Å. All Ti–Os bond lengths are 2.70 Å. V is bonded in a 8-coordinate geometry to eight equivalent Ti and six equivalent Os atoms. All V–Os bond lengths are 3.12 Å. Os is bonded in a distorted body-centered cubic geometry to eight equivalent Ti and six equivalent V atoms.