Ta6Cr(CS2)3 crystallizes in the monoclinic C2/m space group. There are two inequivalent Ta sites. In the first Ta site, Ta(1) is bonded to one C(1), two equivalent C(2), one S(2), and two equivalent S(1) atoms to form TaC3S3 octahedra that share  a cornercorner with one Ta(2)C3S3 octahedra, corners with two equivalent Ta(1)C3S3 octahedra, corners with three equivalent Cr(1)S6 octahedra, edges with four equivalent Ta(2)C3S3 octahedra, and edges with five equivalent Ta(1)C3S3 octahedra. The corner-sharing octahedral tilt angles range from 0-46°. In the second Ta site, Ta(2) is bonded to one C(1), two equivalent C(2), one S(2), and two equivalent S(1) atoms to form TaC3S3 octahedra that share  a cornercorner with one Ta(2)C3S3 octahedra, corners with two equivalent Ta(1)C3S3 octahedra,  an edgeedge with one Ta(2)C3S3 octahedra, edges with eight equivalent Ta(1)C3S3 octahedra, and  a faceface with one Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 0-1°. Cr(1) is bonded to two equivalent S(2) and four equivalent S(1) atoms to form CrS6 octahedra that share corners with twelve equivalent Ta(1)C3S3 octahedra and faces with two equivalent Ta(2)C3S3 octahedra. The corner-sharing octahedral tilt angles are 46°. There are two inequivalent C sites. In the first C site, C(1) is bonded to two equivalent Ta(2) and four equivalent Ta(1) atoms to form CTa6 octahedra that share corners with two equivalent S(2)Ta3Cr trigonal pyramids, corners with four equivalent S(1)Ta3Cr trigonal pyramids, edges with six equivalent C(2)Ta6 octahedra, edges with two equivalent S(2)Ta3Cr trigonal pyramids, and edges with four equivalent S(1)Ta3Cr trigonal pyramids. In the second C site, C(2) is bonded to two equivalent Ta(2) and four equivalent Ta(1) atoms to form CTa6 octahedra that share corners with two equivalent S(2)Ta3Cr trigonal pyramids, corners with four equivalent S(1)Ta3Cr trigonal pyramids, edges with three equivalent C(1)Ta6 octahedra, edges with three equivalent C(2)Ta6 octahedra, edges with two equivalent S(2)Ta3Cr trigonal pyramids, and edges with four equivalent S(1)Ta3Cr trigonal pyramids. There are two inequivalent S sites. In the first S site, S(1) is bonded to one Ta(2), two equivalent Ta(1), and one Cr(1) atom to form distorted STa3Cr trigonal pyramids that share  a cornercorner with one C(1)Ta6 octahedra, corners with two equivalent C(2)Ta6 octahedra, corners with three equivalent S(2)Ta3Cr trigonal pyramids, corners with four equivalent S(1)Ta3Cr trigonal pyramids,  an edgeedge with one C(1)Ta6 octahedra, edges with two equivalent C(2)Ta6 octahedra,  an edgeedge with one S(1)Ta3Cr trigonal pyramid, and  an edgeedge with one S(2)Ta3Cr trigonal pyramid. The corner-sharing octahedral tilt angles range from 10-11°. In the second S site, S(2) is bonded to one Ta(2), two equivalent Ta(1), and one Cr(1) atom to form distorted STa3Cr trigonal pyramids that share  a cornercorner with one C(1)Ta6 octahedra, corners with two equivalent C(2)Ta6 octahedra,  a cornercorner with one S(2)Ta3Cr trigonal pyramid, corners with six equivalent S(1)Ta3Cr trigonal pyramids,  an edgeedge with one C(1)Ta6 octahedra, edges with two equivalent C(2)Ta6 octahedra, and edges with two equivalent S(1)Ta3Cr trigonal pyramids. The corner-sharing octahedral tilt angles range from 10-11°.
Ta6Cr(CS2)3 crystallizes in the monoclinic C2/m space group. There are two inequivalent Ta sites. In the first Ta site, Ta(1) is bonded to one C(1), two equivalent C(2), one S(2), and two equivalent S(1) atoms to form TaC3S3 octahedra that share  a cornercorner with one Ta(2)C3S3 octahedra, corners with two equivalent Ta(1)C3S3 octahedra, corners with three equivalent Cr(1)S6 octahedra, edges with four equivalent Ta(2)C3S3 octahedra, and edges with five equivalent Ta(1)C3S3 octahedra. The corner-sharing octahedral tilt angles range from 0-46°. The Ta(1)-C(1) bond length is 2.23 Å. There is one shorter (2.22 Å) and one longer (2.23 Å) Ta(1)-C(2) bond length. The Ta(1)-S(2) bond length is 2.53 Å. Both Ta(1)-S(1) bond lengths are 2.52 Å. In the second Ta site, Ta(2) is bonded to one C(1), two equivalent C(2), one S(2), and two equivalent S(1) atoms to form TaC3S3 octahedra that share  a cornercorner with one Ta(2)C3S3 octahedra, corners with two equivalent Ta(1)C3S3 octahedra,  an edgeedge with one Ta(2)C3S3 octahedra, edges with eight equivalent Ta(1)C3S3 octahedra, and  a faceface with one Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 0-1°. The Ta(2)-C(1) bond length is 2.22 Å. Both Ta(2)-C(2) bond lengths are 2.23 Å. The Ta(2)-S(2) bond length is 2.56 Å. Both Ta(2)-S(1) bond lengths are 2.56 Å. Cr(1) is bonded to two equivalent S(2) and four equivalent S(1) atoms to form CrS6 octahedra that share corners with twelve equivalent Ta(1)C3S3 octahedra and faces with two equivalent Ta(2)C3S3 octahedra. The corner-sharing octahedral tilt angles are 46°. Both Cr(1)-S(2) bond lengths are 2.41 Å. All Cr(1)-S(1) bond lengths are 2.42 Å. There are two inequivalent C sites. In the first C site, C(1) is bonded to two equivalent Ta(2) and four equivalent Ta(1) atoms to form CTa6 octahedra that share corners with two equivalent S(2)Ta3Cr trigonal pyramids, corners with four equivalent S(1)Ta3Cr trigonal pyramids, edges with six equivalent C(2)Ta6 octahedra, edges with two equivalent S(2)Ta3Cr trigonal pyramids, and edges with four equivalent S(1)Ta3Cr trigonal pyramids. In the second C site, C(2) is bonded to two equivalent Ta(2) and four equivalent Ta(1) atoms to form CTa6 octahedra that share corners with two equivalent S(2)Ta3Cr trigonal pyramids, corners with four equivalent S(1)Ta3Cr trigonal pyramids, edges with three equivalent C(1)Ta6 octahedra, edges with three equivalent C(2)Ta6 octahedra, edges with two equivalent S(2)Ta3Cr trigonal pyramids, and edges with four equivalent S(1)Ta3Cr trigonal pyramids. There are two inequivalent S sites. In the first S site, S(1) is bonded to one Ta(2), two equivalent Ta(1), and one Cr(1) atom to form distorted STa3Cr trigonal pyramids that share  a cornercorner with one C(1)Ta6 octahedra, corners with two equivalent C(2)Ta6 octahedra, corners with three equivalent S(2)Ta3Cr trigonal pyramids, corners with four equivalent S(1)Ta3Cr trigonal pyramids,  an edgeedge with one C(1)Ta6 octahedra, edges with two equivalent C(2)Ta6 octahedra,  an edgeedge with one S(1)Ta3Cr trigonal pyramid, and  an edgeedge with one S(2)Ta3Cr trigonal pyramid. The corner-sharing octahedral tilt angles range from 10-11°. In the second S site, S(2) is bonded to one Ta(2), two equivalent Ta(1), and one Cr(1) atom to form distorted STa3Cr trigonal pyramids that share  a cornercorner with one C(1)Ta6 octahedra, corners with two equivalent C(2)Ta6 octahedra,  a cornercorner with one S(2)Ta3Cr trigonal pyramid, corners with six equivalent S(1)Ta3Cr trigonal pyramids,  an edgeedge with one C(1)Ta6 octahedra, edges with two equivalent C(2)Ta6 octahedra, and edges with two equivalent S(1)Ta3Cr trigonal pyramids. The corner-sharing octahedral tilt angles range from 10-11°.