TaCr3(CuS4)2 crystallizes in the orthorhombic Pmn2_1 space group. Ta(1) is bonded to one S(5), one S(8), two equivalent S(2), and two equivalent S(6) atoms to form TaS6 octahedra that share corners with two equivalent Cr(1)S6 octahedra, corners with two 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 47-58°. 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 CrS6 octahedra that share corners with two equivalent Ta(1)S6 octahedra, corners with two equivalent Cr(3)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 47-59°. 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 two equivalent Ta(1)S6 octahedra, corners with two equivalent Cr(3)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 49-58°. In the third Cr site, Cr(3) 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 Cr(1)S6 octahedra, corners with two 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 49-59°. There are two inequivalent Cu sites. In the first Cu site, Cu(1) is bonded in a 7-coordinate geometry to one S(1), two equivalent S(3), two equivalent S(5), and two equivalent S(7) atoms. In the second Cu site, Cu(2) is bonded in a 5-coordinate geometry to one S(2), two equivalent S(4), and two equivalent S(6) atoms. There are eight inequivalent S sites. In the first S site, S(1) is bonded to one Cr(2), two equivalent Cr(3), and one Cu(1) atom to form distorted SCr3Cu tetrahedra that share corners with two equivalent S(1)Cr3Cu tetrahedra,  a cornercorner with one S(4)Cr3Cu2 trigonal bipyramid, corners with two equivalent S(6)Ta2CrCu2 trigonal bipyramids, and edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids. In the second S site, S(2) is bonded to two equivalent Ta(1), one Cr(1), and one Cu(2) atom to form distorted STa2CrCu tetrahedra that share corners with two equivalent S(2)Ta2CrCu tetrahedra,  a cornercorner with one S(3)Cr3Cu2 trigonal bipyramid, corners with four equivalent S(6)Ta2CrCu2 trigonal bipyramids,  an edgeedge with one S(6)Ta2CrCu2 trigonal bipyramid, and edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids. In the third S site, S(3) is bonded to one Cr(1), two equivalent Cr(2), and two equivalent Cu(1) atoms to form distorted SCr3Cu2 trigonal bipyramids that share  a cornercorner with one S(2)Ta2CrCu tetrahedra, edges with two equivalent S(1)Cr3Cu tetrahedra, 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(2) atoms to form distorted SCr3Cu2 trigonal bipyramids that share  a cornercorner with one S(1)Cr3Cu tetrahedra, corners with two equivalent S(6)Ta2CrCu2 trigonal bipyramids, edges with two equivalent S(2)Ta2CrCu tetrahedra,  an edgeedge with one S(6)Ta2CrCu2 trigonal bipyramid, edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids. In the fifth S site, S(5) is bonded in a 3-coordinate geometry to one Ta(1), two equivalent Cr(3), and two equivalent Cu(1) atoms. In the sixth S site, S(6) is bonded to two equivalent Ta(1), one Cr(3), and two equivalent Cu(2) atoms to form distorted STa2CrCu2 trigonal bipyramids that share corners with two equivalent S(1)Cr3Cu tetrahedra, corners with four equivalent S(2)Ta2CrCu tetrahedra, corners with two equivalent S(4)Cr3Cu2 trigonal bipyramids,  an edgeedge with one S(2)Ta2CrCu tetrahedra,  an edgeedge with one S(4)Cr3Cu2 trigonal bipyramid, and edges with two equivalent S(6)Ta2CrCu2 trigonal bipyramids. In the seventh S site, S(7) is bonded in a 5-coordinate geometry to one Cr(3), two equivalent Cr(1), and two equivalent Cu(1) atoms. 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 Pmn2_1 space group. Ta(1) is bonded to one S(5), one S(8), two equivalent S(2), and two equivalent S(6) atoms to form TaS6 octahedra that share corners with two equivalent Cr(1)S6 octahedra, corners with two 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 47-58°. The Ta(1)-S(5) bond length is 2.39 Å. The Ta(1)-S(8) bond length is 2.59 Å. Both Ta(1)-S(2) bond lengths are 2.45 Å. Both Ta(1)-S(6) bond lengths are 2.48 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 CrS6 octahedra that share corners with two equivalent Ta(1)S6 octahedra, corners with two equivalent Cr(3)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 47-59°. The Cr(1)-S(2) bond length is 2.49 Å. The Cr(1)-S(3) bond length is 2.36 Å. Both Cr(1)-S(4) bond lengths are 2.46 Å. Both Cr(1)-S(7) bond lengths are 2.38 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 two equivalent Ta(1)S6 octahedra, corners with two equivalent Cr(3)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 49-58°. The Cr(2)-S(1) bond length is 2.43 Å. The Cr(2)-S(4) bond length is 2.36 Å. Both Cr(2)-S(3) bond lengths are 2.44 Å. Both Cr(2)-S(8) bond lengths are 2.38 Å. In the third Cr site, Cr(3) 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 Cr(1)S6 octahedra, corners with two 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 49-59°. The Cr(3)-S(6) bond length is 2.41 Å. The Cr(3)-S(7) bond length is 2.54 Å. Both Cr(3)-S(1) bond lengths are 2.33 Å. Both Cr(3)-S(5) bond lengths are 2.43 Å. There are two inequivalent Cu sites. In the first Cu site, Cu(1) is bonded in a 7-coordinate geometry to one S(1), two equivalent S(3), two equivalent S(5), and two equivalent S(7) atoms. The Cu(1)-S(1) bond length is 2.28 Å. Both Cu(1)-S(3) bond lengths are 2.51 Å. Both Cu(1)-S(5) bond lengths are 2.99 Å. Both Cu(1)-S(7) bond lengths are 2.83 Å. In the second Cu site, Cu(2) is bonded in a 5-coordinate geometry to one S(2), two equivalent S(4), and two equivalent S(6) atoms. The Cu(2)-S(2) bond length is 2.36 Å. Both Cu(2)-S(4) bond lengths are 2.42 Å. Both Cu(2)-S(6) bond lengths are 2.76 Å. There are eight inequivalent S sites. In the first S site, S(1) is bonded to one Cr(2), two equivalent Cr(3), and one Cu(1) atom to form distorted SCr3Cu tetrahedra that share corners with two equivalent S(1)Cr3Cu tetrahedra,  a cornercorner with one S(4)Cr3Cu2 trigonal bipyramid, corners with two equivalent S(6)Ta2CrCu2 trigonal bipyramids, and edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids. In the second S site, S(2) is bonded to two equivalent Ta(1), one Cr(1), and one Cu(2) atom to form distorted STa2CrCu tetrahedra that share corners with two equivalent S(2)Ta2CrCu tetrahedra,  a cornercorner with one S(3)Cr3Cu2 trigonal bipyramid, corners with four equivalent S(6)Ta2CrCu2 trigonal bipyramids,  an edgeedge with one S(6)Ta2CrCu2 trigonal bipyramid, and edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids. In the third S site, S(3) is bonded to one Cr(1), two equivalent Cr(2), and two equivalent Cu(1) atoms to form distorted SCr3Cu2 trigonal bipyramids that share  a cornercorner with one S(2)Ta2CrCu tetrahedra, edges with two equivalent S(1)Cr3Cu tetrahedra, 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(2) atoms to form distorted SCr3Cu2 trigonal bipyramids that share  a cornercorner with one S(1)Cr3Cu tetrahedra, corners with two equivalent S(6)Ta2CrCu2 trigonal bipyramids, edges with two equivalent S(2)Ta2CrCu tetrahedra,  an edgeedge with one S(6)Ta2CrCu2 trigonal bipyramid, edges with two equivalent S(3)Cr3Cu2 trigonal bipyramids, and edges with two equivalent S(4)Cr3Cu2 trigonal bipyramids. In the fifth S site, S(5) is bonded in a 3-coordinate geometry to one Ta(1), two equivalent Cr(3), and two equivalent Cu(1) atoms. In the sixth S site, S(6) is bonded to two equivalent Ta(1), one Cr(3), and two equivalent Cu(2) atoms to form distorted STa2CrCu2 trigonal bipyramids that share corners with two equivalent S(1)Cr3Cu tetrahedra, corners with four equivalent S(2)Ta2CrCu tetrahedra, corners with two equivalent S(4)Cr3Cu2 trigonal bipyramids,  an edgeedge with one S(2)Ta2CrCu tetrahedra,  an edgeedge with one S(4)Cr3Cu2 trigonal bipyramid, and edges with two equivalent S(6)Ta2CrCu2 trigonal bipyramids. In the seventh S site, S(7) is bonded in a 5-coordinate geometry to one Cr(3), two equivalent Cr(1), and two equivalent Cu(1) atoms. 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.