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MgY2Tl is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Mg is bonded in a body-centered cubic geometry to eight equivalent Y atoms. All Mg–Y bond lengths are 3.28 Å. Y is bonded in a body-centered cubic geometry to four equivalent Mg and four equivalent Tl atoms. All Y–Tl bond lengths are 3.28 Å. Tl is bonded in a body-centered cubic geometry to eight equivalent Y atoms.
MgY2Tl crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two MgY2Tl ribbons oriented in the (1, 0, 0) direction. Mg is bonded in a linear geometry to two equivalent Y atoms. Both Mg–Y bond lengths are 3.38 Å. Y is bonded in a linear geometry to one Mg and one Tl atom. The Y–Tl bond length is 2.90 Å. Tl is bonded in a linear geometry to two equivalent Y atoms.