TaCr3(CuS4)2 crystallizes in the orthorhombic Pmn2_1 space group. Ta(1) is bonded to one S(2), one S(3), two equivalent S(4), and two equivalent S(7) atoms to form TaS6 octahedra that share corners with two equivalent Cr(2)S6 octahedra, corners with two equivalent Cr(3)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with two equivalent Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-54°. There are three inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to one S(1), one S(4), two equivalent S(3), and two equivalent S(8) atoms to form distorted CrS6 octahedra that share corners with two equivalent Cr(2)S6 octahedra, corners with two equivalent Cr(3)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with two equivalent Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 52-58°. In the second Cr site, Cr(2) is bonded to one S(6), one S(7), two equivalent S(1), and two equivalent S(5) atoms to form CrS6 octahedra that share corners with two equivalent Ta(1)S6 octahedra, corners with two equivalent Cr(1)S6 octahedra, edges with two equivalent Cr(2)S6 octahedra, and edges with two equivalent Cr(3)S6 octahedra. The corner-sharing octahedral tilt angles range from 52-54°. In the third Cr site, Cr(3) is bonded to one S(5), one S(8), two equivalent S(2), and two equivalent S(6) atoms to form CrS6 octahedra that share corners with two equivalent Ta(1)S6 octahedra, corners with two equivalent Cr(1)S6 octahedra, edges with two equivalent Cr(2)S6 octahedra, and edges with two equivalent Cr(3)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-58°. There are two inequivalent Cu sites. In the first Cu site, Cu(1) is bonded in a 5-coordinate geometry to one S(1), two equivalent S(3), and two equivalent S(5) atoms. In the second Cu site, Cu(2) is bonded in a 5-coordinate geometry to one S(2), two equivalent S(6), and two equivalent S(8) atoms. There are eight inequivalent S sites. In the first S site, S(1) is bonded in a 4-coordinate geometry to one Cr(1), two equivalent Cr(2), and one Cu(1) atom. In the second S site, S(2) is bonded to one Ta(1), two equivalent Cr(3), and one Cu(2) atom to form distorted STaCr2Cu trigonal pyramids that share corners with four equivalent S(6)Cr3Cu2 square pyramids,  a cornercorner with one S(3)TaCr2Cu2 trigonal bipyramid, corners with two equivalent S(5)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(2)TaCr2Cu trigonal pyramids, and  an edgeedge with one S(6)Cr3Cu2 square pyramid. In the third S site, S(3) is bonded to one Ta(1), two equivalent Cr(1), and two equivalent Cu(1) atoms to form distorted STaCr2Cu2 trigonal bipyramids that share corners with two equivalent S(5)Cr3Cu2 trigonal bipyramids,  a cornercorner with one S(2)TaCr2Cu trigonal pyramid,  an edgeedge with one S(5)Cr3Cu2 trigonal bipyramid, and edges with two equivalent S(3)TaCr2Cu2 trigonal bipyramids. In the fourth S site, S(4) is bonded in a distorted T-shaped geometry to two equivalent Ta(1) and one Cr(1) atom. In the fifth S site, S(5) is bonded to one Cr(3), two equivalent Cr(2), and two equivalent Cu(1) atoms to form distorted SCr3Cu2 trigonal bipyramids that share corners with two equivalent S(3)TaCr2Cu2 trigonal bipyramids, corners with two equivalent S(2)TaCr2Cu trigonal pyramids, edges with two equivalent S(6)Cr3Cu2 square pyramids,  an edgeedge with one S(3)TaCr2Cu2 trigonal bipyramid, and edges with two equivalent S(5)Cr3Cu2 trigonal bipyramids. In the sixth S site, S(6) is bonded to one Cr(2), two equivalent Cr(3), and two equivalent Cu(2) atoms to form distorted SCr3Cu2 square pyramids that share corners with four equivalent S(2)TaCr2Cu trigonal pyramids, edges with two equivalent S(6)Cr3Cu2 square pyramids, edges with two equivalent S(5)Cr3Cu2 trigonal bipyramids, and  an edgeedge with one S(2)TaCr2Cu trigonal pyramid. In the seventh S site, S(7) is bonded in a distorted trigonal planar geometry to two equivalent Ta(1) and one Cr(2) atom. In the eighth S site, S(8) is bonded in a 5-coordinate geometry to one Cr(3), two equivalent Cr(1), and two equivalent Cu(2) atoms.
TaCr3(CuS4)2 crystallizes in the orthorhombic Pmn2_1 space group. Ta(1) is bonded to one S(2), one S(3), two equivalent S(4), and two equivalent S(7) atoms to form TaS6 octahedra that share corners with two equivalent Cr(2)S6 octahedra, corners with two equivalent Cr(3)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with two equivalent Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-54°. The Ta(1)-S(2) bond length is 2.37 Å. The Ta(1)-S(3) bond length is 2.49 Å. Both Ta(1)-S(4) bond lengths are 2.47 Å. Both Ta(1)-S(7) bond lengths are 2.45 Å. There are three inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to one S(1), one S(4), two equivalent S(3), and two equivalent S(8) atoms to form distorted CrS6 octahedra that share corners with two equivalent Cr(2)S6 octahedra, corners with two equivalent Cr(3)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with two equivalent Cr(1)S6 octahedra. The corner-sharing octahedral tilt angles range from 52-58°. The Cr(1)-S(1) bond length is 2.39 Å. The Cr(1)-S(4) bond length is 2.38 Å. Both Cr(1)-S(3) bond lengths are 2.43 Å. Both Cr(1)-S(8) bond lengths are 2.43 Å. In the second Cr site, Cr(2) is bonded to one S(6), one S(7), two equivalent S(1), and two equivalent S(5) atoms to form CrS6 octahedra that share corners with two equivalent Ta(1)S6 octahedra, corners with two equivalent Cr(1)S6 octahedra, edges with two equivalent Cr(2)S6 octahedra, and edges with two equivalent Cr(3)S6 octahedra. The corner-sharing octahedral tilt angles range from 52-54°. The Cr(2)-S(6) bond length is 2.37 Å. The Cr(2)-S(7) bond length is 2.54 Å. Both Cr(2)-S(1) bond lengths are 2.35 Å. Both Cr(2)-S(5) bond lengths are 2.47 Å. In the third Cr site, Cr(3) is bonded to one S(5), one S(8), two equivalent S(2), and two equivalent S(6) atoms to form CrS6 octahedra that share corners with two equivalent Ta(1)S6 octahedra, corners with two equivalent Cr(1)S6 octahedra, edges with two equivalent Cr(2)S6 octahedra, and edges with two equivalent Cr(3)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-58°. The Cr(3)-S(5) bond length is 2.40 Å. The Cr(3)-S(8) bond length is 2.54 Å. Both Cr(3)-S(2) bond lengths are 2.40 Å. Both Cr(3)-S(6) bond lengths are 2.41 Å. There are two inequivalent Cu sites. In the first Cu site, Cu(1) is bonded in a 5-coordinate geometry to one S(1), two equivalent S(3), and two equivalent S(5) atoms. The Cu(1)-S(1) bond length is 2.76 Å. Both Cu(1)-S(3) bond lengths are 2.45 Å. Both Cu(1)-S(5) bond lengths are 2.52 Å. In the second Cu site, Cu(2) is bonded in a 5-coordinate geometry to one S(2), two equivalent S(6), and two equivalent S(8) atoms. The Cu(2)-S(2) bond length is 2.74 Å. Both Cu(2)-S(6) bond lengths are 2.78 Å. Both Cu(2)-S(8) bond lengths are 2.38 Å. There are eight inequivalent S sites. In the first S site, S(1) is bonded in a 4-coordinate geometry to one Cr(1), two equivalent Cr(2), and one Cu(1) atom. In the second S site, S(2) is bonded to one Ta(1), two equivalent Cr(3), and one Cu(2) atom to form distorted STaCr2Cu trigonal pyramids that share corners with four equivalent S(6)Cr3Cu2 square pyramids,  a cornercorner with one S(3)TaCr2Cu2 trigonal bipyramid, corners with two equivalent S(5)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(2)TaCr2Cu trigonal pyramids, and  an edgeedge with one S(6)Cr3Cu2 square pyramid. In the third S site, S(3) is bonded to one Ta(1), two equivalent Cr(1), and two equivalent Cu(1) atoms to form distorted STaCr2Cu2 trigonal bipyramids that share corners with two equivalent S(5)Cr3Cu2 trigonal bipyramids,  a cornercorner with one S(2)TaCr2Cu trigonal pyramid,  an edgeedge with one S(5)Cr3Cu2 trigonal bipyramid, and edges with two equivalent S(3)TaCr2Cu2 trigonal bipyramids. In the fourth S site, S(4) is bonded in a distorted T-shaped geometry to two equivalent Ta(1) and one Cr(1) atom. In the fifth S site, S(5) is bonded to one Cr(3), two equivalent Cr(2), and two equivalent Cu(1) atoms to form distorted SCr3Cu2 trigonal bipyramids that share corners with two equivalent S(3)TaCr2Cu2 trigonal bipyramids, corners with two equivalent S(2)TaCr2Cu trigonal pyramids, edges with two equivalent S(6)Cr3Cu2 square pyramids,  an edgeedge with one S(3)TaCr2Cu2 trigonal bipyramid, and edges with two equivalent S(5)Cr3Cu2 trigonal bipyramids. In the sixth S site, S(6) is bonded to one Cr(2), two equivalent Cr(3), and two equivalent Cu(2) atoms to form distorted SCr3Cu2 square pyramids that share corners with four equivalent S(2)TaCr2Cu trigonal pyramids, edges with two equivalent S(6)Cr3Cu2 square pyramids, edges with two equivalent S(5)Cr3Cu2 trigonal bipyramids, and  an edgeedge with one S(2)TaCr2Cu trigonal pyramid. In the seventh S site, S(7) is bonded in a distorted trigonal planar geometry to two equivalent Ta(1) and one Cr(2) atom. In the eighth S site, S(8) is bonded in a 5-coordinate geometry to one Cr(3), two equivalent Cr(1), and two equivalent Cu(2) atoms.