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Li2TlIn crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Li2TlIn ribbons oriented in the (1, 0, 0) direction. Li is bonded in a linear geometry to one Tl and one In atom. The Li–Tl bond length is 2.91 Å. The Li–In bond length is 2.90 Å. Tl is bonded in a linear geometry to two equivalent Li atoms. In is bonded in a linear geometry to two equivalent Li atoms.
Li2TlIn is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Li is bonded in a body-centered cubic geometry to four equivalent Tl and four equivalent In atoms. All Li–Tl bond lengths are 2.97 Å. All Li–In bond lengths are 2.97 Å. Tl is bonded in a body-centered cubic geometry to eight equivalent Li atoms. In is bonded in a body-centered cubic geometry to eight equivalent Li atoms.