CsTlBr4 crystallizes in the orthorhombic P2_12_12_1 space group. Cs(1) is bonded in a 11-coordinate geometry to two equivalent Br(1), three equivalent Br(2), three equivalent Br(3), and three equivalent Br(4) atoms. Tl(1) is bonded in a tetrahedral geometry to one Br(1), one Br(2), one Br(3), and one Br(4) atom. There are four inequivalent Br sites. In the first Br site, Br(1) is bonded in a distorted single-bond geometry to two equivalent Cs(1) and one Tl(1) atom. In the second Br site, Br(2) is bonded in a distorted single-bond geometry to three equivalent Cs(1) and one Tl(1) atom. In the third Br site, Br(3) is bonded in a distorted single-bond geometry to three equivalent Cs(1) and one Tl(1) atom. In the fourth Br site, Br(4) is bonded in a 4-coordinate geometry to three equivalent Cs(1) and one Tl(1) atom.
CsTlBr4 crystallizes in the orthorhombic P2_12_12_1 space group. Cs(1) is bonded in a 11-coordinate geometry to two equivalent Br(1), three equivalent Br(2), three equivalent Br(3), and three equivalent Br(4) atoms. There is one shorter (3.80 Å) and one longer (3.82 Å) Cs(1)-Br(1) bond length. There are a spread of Cs(1)-Br(2) bond distances ranging from 3.84-3.99 Å. There are a spread of Cs(1)-Br(3) bond distances ranging from 4.04-4.28 Å. There are a spread of Cs(1)-Br(4) bond distances ranging from 3.77-4.02 Å. Tl(1) is bonded in a tetrahedral geometry to one Br(1), one Br(2), one Br(3), and one Br(4) atom. The Tl(1)-Br(1) bond length is 2.58 Å. The Tl(1)-Br(2) bond length is 2.62 Å. The Tl(1)-Br(3) bond length is 2.59 Å. The Tl(1)-Br(4) bond length is 2.62 Å. There are four inequivalent Br sites. In the first Br site, Br(1) is bonded in a distorted single-bond geometry to two equivalent Cs(1) and one Tl(1) atom. In the second Br site, Br(2) is bonded in a distorted single-bond geometry to three equivalent Cs(1) and one Tl(1) atom. In the third Br site, Br(3) is bonded in a distorted single-bond geometry to three equivalent Cs(1) and one Tl(1) atom. In the fourth Br site, Br(4) is bonded in a 4-coordinate geometry to three equivalent Cs(1) and one Tl(1) atom.