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LiLaTl2 crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two LiLaTl2 ribbons oriented in the (1, 0, 0) direction. Li is bonded in a linear geometry to two equivalent Tl atoms. Both Li–Tl bond lengths are 2.78 Å. La is bonded in a linear geometry to two equivalent Tl atoms. Both La–Tl bond lengths are 3.16 Å. Tl is bonded in a linear geometry to one Li and one La atom.
LiLaTl2 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 eight equivalent Tl atoms. All Li–Tl bond lengths are 3.29 Å. La is bonded in a body-centered cubic geometry to eight equivalent Tl atoms. All La–Tl bond lengths are 3.29 Å. Tl is bonded in a body-centered cubic geometry to four equivalent Li and four equivalent La atoms.