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Ti2OsFe crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Ti2OsFe ribbons oriented in the (1, 0, 0) direction. Ti is bonded in a linear geometry to one Os and one Fe atom. The Ti–Os bond length is 2.23 Å. The Ti–Fe bond length is 2.30 Å. Os is bonded in a linear geometry to two equivalent Ti atoms. Fe is bonded in a linear geometry to two equivalent Ti atoms.
Ti2OsFe is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ti is bonded in a body-centered cubic geometry to four equivalent Os and four equivalent Fe atoms. All Ti–Os bond lengths are 2.63 Å. All Ti–Fe bond lengths are 2.63 Å. Os is bonded in a body-centered cubic geometry to eight equivalent Ti atoms. Fe is bonded in a distorted body-centered cubic geometry to eight equivalent Ti atoms.