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V2MnFe crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two V2MnFe ribbons oriented in the (0, 1, 0) direction. V is bonded in a linear geometry to one Mn and one Fe atom. The V–Mn bond length is 2.74 Å. The V–Fe bond length is 2.48 Å. Mn is bonded in a linear geometry to two equivalent V atoms. Fe is bonded in a linear geometry to two equivalent V atoms.
V2MnFe is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. V is bonded in a body-centered cubic geometry to four equivalent Mn and four equivalent Fe atoms. All V–Mn bond lengths are 2.49 Å. All V–Fe bond lengths are 2.49 Å. Mn is bonded in a distorted body-centered cubic geometry to eight equivalent V and six equivalent Fe atoms. All Mn–Fe bond lengths are 2.88 Å. Fe is bonded in a distorted body-centered cubic geometry to eight equivalent V and six equivalent Mn atoms.