CsMo3I3Cl4 crystallizes in the trigonal P31c space group. There are two inequivalent Cs sites. In the first Cs site, Cs(1) is bonded to three equivalent I(1) and three equivalent I(2) atoms to form distorted CsI6 octahedra that share corners with three equivalent Mo(1)ICl4 square pyramids and corners with three equivalent Mo(2)ICl4 square pyramids. In the second Cs site, Cs(2) is bonded in a 9-coordinate geometry to three equivalent I(1), three equivalent I(2), and three equivalent Cl(4) atoms. There are two inequivalent Mo sites. In the first Mo site, Mo(1) is bonded to one I(1), one Cl(1), one Cl(3), and two equivalent Cl(4) atoms to form distorted MoICl4 square pyramids that share  a cornercorner with one Cs(1)I6 octahedra, edges with two equivalent Mo(1)ICl4 square pyramids, and edges with two equivalent Mo(2)ICl4 square pyramids. The corner-sharing octahedral tilt angles are 54°. In the second Mo site, Mo(2) is bonded to one I(2), one Cl(2), one Cl(4), and two equivalent Cl(1) atoms to form distorted MoICl4 square pyramids that share  a cornercorner with one Cs(1)I6 octahedra, edges with two equivalent Mo(1)ICl4 square pyramids, and edges with two equivalent Mo(2)ICl4 square pyramids. The corner-sharing octahedral tilt angles are 69°. There are two inequivalent I sites. In the first I site, I(1) is bonded in a 3-coordinate geometry to one Cs(1), one Cs(2), and one Mo(1) atom. In the second I site, I(2) is bonded in a 3-coordinate geometry to one Cs(1), one Cs(2), and one Mo(2) atom. There are four inequivalent Cl sites. In the first Cl site, Cl(2) is bonded in a 3-coordinate geometry to three equivalent Mo(2) atoms. In the second Cl site, Cl(3) is bonded in a 3-coordinate geometry to three equivalent Mo(1) atoms. In the third Cl site, Cl(4) is bonded in a 3-coordinate geometry to one Cs(2), one Mo(2), and two equivalent Mo(1) atoms. In the fourth Cl site, Cl(1) is bonded in a 3-coordinate geometry to one Mo(1) and two equivalent Mo(2) atoms.
CsMo3I3Cl4 crystallizes in the trigonal P31c space group. There are two inequivalent Cs sites. In the first Cs site, Cs(1) is bonded to three equivalent I(1) and three equivalent I(2) atoms to form distorted CsI6 octahedra that share corners with three equivalent Mo(1)ICl4 square pyramids and corners with three equivalent Mo(2)ICl4 square pyramids. All Cs(1)-I(1) bond lengths are 4.03 Å. All Cs(1)-I(2) bond lengths are 3.91 Å. In the second Cs site, Cs(2) is bonded in a 9-coordinate geometry to three equivalent I(1), three equivalent I(2), and three equivalent Cl(4) atoms. All Cs(2)-I(1) bond lengths are 4.29 Å. All Cs(2)-I(2) bond lengths are 4.13 Å. All Cs(2)-Cl(4) bond lengths are 4.05 Å. There are two inequivalent Mo sites. In the first Mo site, Mo(1) is bonded to one I(1), one Cl(1), one Cl(3), and two equivalent Cl(4) atoms to form distorted MoICl4 square pyramids that share  a cornercorner with one Cs(1)I6 octahedra, edges with two equivalent Mo(1)ICl4 square pyramids, and edges with two equivalent Mo(2)ICl4 square pyramids. The corner-sharing octahedral tilt angles are 54°. The Mo(1)-I(1) bond length is 2.82 Å. The Mo(1)-Cl(1) bond length is 2.50 Å. The Mo(1)-Cl(3) bond length is 2.48 Å. There is one shorter (2.48 Å) and one longer (2.49 Å) Mo(1)-Cl(4) bond length. In the second Mo site, Mo(2) is bonded to one I(2), one Cl(2), one Cl(4), and two equivalent Cl(1) atoms to form distorted MoICl4 square pyramids that share  a cornercorner with one Cs(1)I6 octahedra, edges with two equivalent Mo(1)ICl4 square pyramids, and edges with two equivalent Mo(2)ICl4 square pyramids. The corner-sharing octahedral tilt angles are 69°. The Mo(2)-I(2) bond length is 2.82 Å. The Mo(2)-Cl(2) bond length is 2.49 Å. The Mo(2)-Cl(4) bond length is 2.50 Å. There is one shorter (2.48 Å) and one longer (2.49 Å) Mo(2)-Cl(1) bond length. There are two inequivalent I sites. In the first I site, I(1) is bonded in a 3-coordinate geometry to one Cs(1), one Cs(2), and one Mo(1) atom. In the second I site, I(2) is bonded in a 3-coordinate geometry to one Cs(1), one Cs(2), and one Mo(2) atom. There are four inequivalent Cl sites. In the first Cl site, Cl(2) is bonded in a 3-coordinate geometry to three equivalent Mo(2) atoms. In the second Cl site, Cl(3) is bonded in a 3-coordinate geometry to three equivalent Mo(1) atoms. In the third Cl site, Cl(4) is bonded in a 3-coordinate geometry to one Cs(2), one Mo(2), and two equivalent Mo(1) atoms. In the fourth Cl site, Cl(1) is bonded in a 3-coordinate geometry to one Mo(1) and two equivalent Mo(2) atoms.