TaCr3(CuS4)2 crystallizes in the orthorhombic Pmc2_1 space group. Ta(1) is bonded to one S(6), one S(8), two equivalent S(1), and two equivalent S(5) atoms to form TaS6 octahedra that share corners with four equivalent Cr(2)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with two equivalent Cr(3)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-59°. There are three inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to one S(2), one S(3), two equivalent S(4), and two equivalent S(7) atoms to form a mixture of edge and corner-sharing CrS6 octahedra. The corner-sharing octahedral tilt angles range from 48-58°. In the second Cr site, Cr(2) is bonded to one S(1), one S(4), two equivalent S(3), and two equivalent S(8) atoms to form CrS6 octahedra that share corners with four equivalent Ta(1)S6 octahedra, edges with two equivalent Cr(1)S6 octahedra, and edges with two equivalent Cr(2)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-59°. In the third Cr site, Cr(3) is bonded to one S(5), one S(7), two equivalent S(2), and two equivalent S(6) atoms to form CrS6 octahedra that share corners with four equivalent Cr(1)S6 octahedra, edges with two equivalent Ta(1)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(2), two equivalent S(4), and two equivalent S(7) atoms. In the second Cu site, Cu(2) is bonded in a 5-coordinate geometry to one S(1), two equivalent S(3), and two equivalent S(6) atoms. There are eight inequivalent S sites. In the first S site, S(1) is bonded to two equivalent Ta(1), one Cr(2), and one Cu(2) atom to form distorted STa2CrCu tetrahedra that share corners with two equivalent S(1)Ta2CrCu tetrahedra,  a cornercorner with one S(4)Cr3Cu2 trigonal bipyramid, corners with four equivalent S(6)TaCr2Cu2 trigonal bipyramids, and edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids. In the second S site, S(2) is bonded to one Cr(1), two equivalent Cr(3), and one Cu(1) atom to form SCr3Cu trigonal pyramids that share  a cornercorner with one S(3)Cr3Cu2 trigonal bipyramid, corners with two equivalent S(7)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(6)TaCr2Cu2 trigonal bipyramids, corners with two equivalent S(2)Cr3Cu trigonal pyramids,  an edgeedge with one S(6)TaCr2Cu2 trigonal bipyramid, edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(7)Cr3Cu2 trigonal bipyramids. In the third S site, S(3) is bonded to one Cr(1), two equivalent Cr(2), and two equivalent Cu(2) atoms to form distorted SCr3Cu2 trigonal bipyramids that share corners with two equivalent S(7)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(6)TaCr2Cu2 trigonal bipyramids,  a cornercorner with one S(2)Cr3Cu trigonal pyramid, edges with two equivalent S(1)Ta2CrCu tetrahedra,  an edgeedge with one S(6)TaCr2Cu2 trigonal bipyramid, edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids. In the fourth S site, S(4) is bonded to one Cr(2), two equivalent Cr(1), and two equivalent Cu(1) atoms to form distorted SCr3Cu2 trigonal bipyramids that share  a cornercorner with one S(1)Ta2CrCu tetrahedra, corners with four equivalent S(7)Cr3Cu2 trigonal bipyramids, edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids, edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids, edges with two equivalent S(7)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(2)Cr3Cu trigonal pyramids. In the fifth S site, S(5) is bonded in a 3-coordinate geometry to two equivalent Ta(1) and one Cr(3) atom. In the sixth S site, S(6) is bonded to one Ta(1), two equivalent Cr(3), and two equivalent Cu(2) atoms to form distorted STaCr2Cu2 trigonal bipyramids that share corners with four equivalent S(1)Ta2CrCu tetrahedra, corners with two equivalent S(3)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(7)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(2)Cr3Cu trigonal pyramids,  an edgeedge with one S(3)Cr3Cu2 trigonal bipyramid, edges with two equivalent S(6)TaCr2Cu2 trigonal bipyramids, and  an edgeedge with one S(2)Cr3Cu trigonal pyramid. In the seventh S site, S(7) is bonded to one Cr(3), two equivalent Cr(1), and two equivalent Cu(1) atoms to form distorted SCr3Cu2 trigonal bipyramids that share corners with two equivalent S(3)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(6)TaCr2Cu2 trigonal bipyramids, corners with four equivalent S(4)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(2)Cr3Cu trigonal pyramids, edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids, edges with two equivalent S(7)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(2)Cr3Cu trigonal pyramids. In the eighth S site, S(8) is bonded in a distorted trigonal planar geometry to one Ta(1) and two equivalent Cr(2) atoms.
TaCr3(CuS4)2 crystallizes in the orthorhombic Pmc2_1 space group. Ta(1) is bonded to one S(6), one S(8), two equivalent S(1), and two equivalent S(5) atoms to form TaS6 octahedra that share corners with four equivalent Cr(2)S6 octahedra, edges with two equivalent Ta(1)S6 octahedra, and edges with two equivalent Cr(3)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-59°. The Ta(1)-S(6) bond length is 2.41 Å. The Ta(1)-S(8) bond length is 2.56 Å. Both Ta(1)-S(1) bond lengths are 2.44 Å. Both Ta(1)-S(5) bond lengths are 2.46 Å. There are three inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to one S(2), one S(3), two equivalent S(4), and two equivalent S(7) atoms to form a mixture of edge and corner-sharing CrS6 octahedra. The corner-sharing octahedral tilt angles range from 48-58°. The Cr(1)-S(2) bond length is 2.43 Å. The Cr(1)-S(3) bond length is 2.35 Å. Both Cr(1)-S(4) bond lengths are 2.44 Å. Both Cr(1)-S(7) bond lengths are 2.41 Å. In the second Cr site, Cr(2) is bonded to one S(1), one S(4), two equivalent S(3), and two equivalent S(8) atoms to form CrS6 octahedra that share corners with four equivalent Ta(1)S6 octahedra, edges with two equivalent Cr(1)S6 octahedra, and edges with two equivalent Cr(2)S6 octahedra. The corner-sharing octahedral tilt angles range from 48-59°. The Cr(2)-S(1) bond length is 2.50 Å. The Cr(2)-S(4) bond length is 2.36 Å. Both Cr(2)-S(3) bond lengths are 2.43 Å. Both Cr(2)-S(8) bond lengths are 2.36 Å. In the third Cr site, Cr(3) is bonded to one S(5), one S(7), two equivalent S(2), and two equivalent S(6) atoms to form CrS6 octahedra that share corners with four equivalent Cr(1)S6 octahedra, edges with two equivalent Ta(1)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 2.41 Å. The Cr(3)-S(7) bond length is 2.55 Å. Both Cr(3)-S(2) bond lengths are 2.33 Å. Both Cr(3)-S(6) bond lengths are 2.45 Å. There are two inequivalent Cu sites. In the first Cu site, Cu(1) is bonded in a 5-coordinate geometry to one S(2), two equivalent S(4), and two equivalent S(7) atoms. The Cu(1)-S(2) bond length is 2.27 Å. Both Cu(1)-S(4) bond lengths are 2.63 Å. Both Cu(1)-S(7) bond lengths are 2.61 Å. In the second Cu site, Cu(2) is bonded in a 5-coordinate geometry to one S(1), two equivalent S(3), and two equivalent S(6) atoms. The Cu(2)-S(1) bond length is 2.41 Å. Both Cu(2)-S(3) bond lengths are 2.39 Å. Both Cu(2)-S(6) bond lengths are 2.73 Å. There are eight inequivalent S sites. In the first S site, S(1) is bonded to two equivalent Ta(1), one Cr(2), and one Cu(2) atom to form distorted STa2CrCu tetrahedra that share corners with two equivalent S(1)Ta2CrCu tetrahedra,  a cornercorner with one S(4)Cr3Cu2 trigonal bipyramid, corners with four equivalent S(6)TaCr2Cu2 trigonal bipyramids, and edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids. In the second S site, S(2) is bonded to one Cr(1), two equivalent Cr(3), and one Cu(1) atom to form SCr3Cu trigonal pyramids that share  a cornercorner with one S(3)Cr3Cu2 trigonal bipyramid, corners with two equivalent S(7)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(6)TaCr2Cu2 trigonal bipyramids, corners with two equivalent S(2)Cr3Cu trigonal pyramids,  an edgeedge with one S(6)TaCr2Cu2 trigonal bipyramid, edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(7)Cr3Cu2 trigonal bipyramids. In the third S site, S(3) is bonded to one Cr(1), two equivalent Cr(2), and two equivalent Cu(2) atoms to form distorted SCr3Cu2 trigonal bipyramids that share corners with two equivalent S(7)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(6)TaCr2Cu2 trigonal bipyramids,  a cornercorner with one S(2)Cr3Cu trigonal pyramid, edges with two equivalent S(1)Ta2CrCu tetrahedra,  an edgeedge with one S(6)TaCr2Cu2 trigonal bipyramid, edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids. In the fourth S site, S(4) is bonded to one Cr(2), two equivalent Cr(1), and two equivalent Cu(1) atoms to form distorted SCr3Cu2 trigonal bipyramids that share  a cornercorner with one S(1)Ta2CrCu tetrahedra, corners with four equivalent S(7)Cr3Cu2 trigonal bipyramids, edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids, edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids, edges with two equivalent S(7)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(2)Cr3Cu trigonal pyramids. In the fifth S site, S(5) is bonded in a 3-coordinate geometry to two equivalent Ta(1) and one Cr(3) atom. In the sixth S site, S(6) is bonded to one Ta(1), two equivalent Cr(3), and two equivalent Cu(2) atoms to form distorted STaCr2Cu2 trigonal bipyramids that share corners with four equivalent S(1)Ta2CrCu tetrahedra, corners with two equivalent S(3)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(7)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(2)Cr3Cu trigonal pyramids,  an edgeedge with one S(3)Cr3Cu2 trigonal bipyramid, edges with two equivalent S(6)TaCr2Cu2 trigonal bipyramids, and  an edgeedge with one S(2)Cr3Cu trigonal pyramid. In the seventh S site, S(7) is bonded to one Cr(3), two equivalent Cr(1), and two equivalent Cu(1) atoms to form distorted SCr3Cu2 trigonal bipyramids that share corners with two equivalent S(3)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(6)TaCr2Cu2 trigonal bipyramids, corners with four equivalent S(4)Cr3Cu2 trigonal bipyramids, corners with two equivalent S(2)Cr3Cu trigonal pyramids, edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids, edges with two equivalent S(7)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(2)Cr3Cu trigonal pyramids. In the eighth S site, S(8) is bonded in a distorted trigonal planar geometry to one Ta(1) and two equivalent Cr(2) atoms.