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NaTl2Sn crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two NaTl2Sn ribbons oriented in the (1, 0, 0) direction. Na is bonded in a linear geometry to two equivalent Tl atoms. Both Na–Tl bond lengths are 3.11 Å. Tl is bonded in a linear geometry to one Na and one Sn atom. The Tl–Sn bond length is 2.78 Å. Sn is bonded in a linear geometry to two equivalent Tl atoms.
NaTl2Sn is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Na is bonded in a body-centered cubic geometry to eight equivalent Tl atoms. All Na–Tl bond lengths are 3.37 Å. Tl is bonded in a body-centered cubic geometry to four equivalent Na and four equivalent Sn atoms. All Tl–Sn bond lengths are 3.37 Å. Sn is bonded in a body-centered cubic geometry to eight equivalent Tl atoms.