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Tl2Ba crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Ba is bonded in a 12-coordinate geometry to twelve equivalent Tl atoms. There are six shorter (3.57 Å) and six longer (4.03 Å) Ba–Tl bond lengths. Tl is bonded in a 10-coordinate geometry to six equivalent Ba and four equivalent Tl atoms. There are three shorter (3.21 Å) and one longer (3.54 Å) Tl–Tl bond lengths.
BaTl3 crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Ba is bonded to twelve equivalent Tl atoms to form a mixture of distorted face and corner-sharing BaTl12 cuboctahedra. There are six shorter (3.62 Å) and six longer (3.90 Å) Ba–Tl bond lengths. Tl is bonded in a 2-coordinate geometry to four equivalent Ba and six equivalent Tl atoms. There are four shorter (3.32 Å) and two longer (3.50 Å) Tl–Tl bond lengths.