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NaTl2In crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two NaTl2In 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 3.13 Å. Tl is bonded in a linear geometry to one Na and one In atom. The Tl–In bond length is 2.86 Å. In is bonded in a linear geometry to two equivalent Tl atoms.
NaTl2In 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 3.31 Å. Tl is bonded in a body-centered cubic geometry to four equivalent Na and four equivalent In atoms. All Tl–In bond lengths are 3.31 Å. In is bonded in a body-centered cubic geometry to eight equivalent Tl atoms.