Mg(CrS2)4 crystallizes in the monoclinic Cm space group. Mg(1) is bonded to one S(2), one S(5), and two equivalent S(3) atoms to form MgS4 tetrahedra that share corners with three equivalent Cr(1)S6 octahedra, corners with three equivalent Cr(2)S6 octahedra, and corners with six equivalent Cr(3)S6 octahedra. The corner-sharing octahedral tilt angles range from 61-62°. There are three inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to one S(2), one S(6), two equivalent S(3), and two equivalent S(4) atoms to form CrS6 octahedra that share corners with three equivalent Mg(1)S4 tetrahedra, edges with two equivalent Cr(2)S6 octahedra, and edges with four equivalent Cr(3)S6 octahedra. In the second Cr site, Cr(2) is bonded to one S(1), one S(5), two equivalent S(3), and two equivalent S(4) atoms to form CrS6 octahedra that share corners with three equivalent Mg(1)S4 tetrahedra, edges with two equivalent Cr(1)S6 octahedra, and edges with four equivalent Cr(3)S6 octahedra. In the third Cr site, Cr(3) is bonded to one S(1), one S(2), one S(3), one S(4), one S(5), and one S(6) atom to form CrS6 octahedra that share corners with three equivalent Mg(1)S4 tetrahedra, edges with two equivalent Cr(1)S6 octahedra, edges with two equivalent Cr(2)S6 octahedra, and edges with two equivalent Cr(3)S6 octahedra. There are six inequivalent S sites. In the first S site, S(1) is bonded in a distorted T-shaped geometry to one Cr(2) and two equivalent Cr(3) atoms. In the second S site, S(2) is bonded to one Mg(1), one Cr(1), and two equivalent Cr(3) atoms to form a mixture of distorted edge and corner-sharing SMgCr3 tetrahedra. In the third S site, S(3) is bonded to one Mg(1), one Cr(1), one Cr(2), and one Cr(3) atom to form a mixture of distorted edge and corner-sharing SMgCr3 tetrahedra. In the fourth S site, S(4) is bonded in a distorted T-shaped geometry to one Cr(1), one Cr(2), and one Cr(3) atom. In the fifth S site, S(5) is bonded to one Mg(1), one Cr(2), and two equivalent Cr(3) atoms to form a mixture of distorted edge and corner-sharing SMgCr3 tetrahedra. In the sixth S site, S(6) is bonded in a distorted T-shaped geometry to one Cr(1) and two equivalent Cr(3) atoms.
Mg(CrS2)4 crystallizes in the monoclinic Cm space group. Mg(1) is bonded to one S(2), one S(5), and two equivalent S(3) atoms to form MgS4 tetrahedra that share corners with three equivalent Cr(1)S6 octahedra, corners with three equivalent Cr(2)S6 octahedra, and corners with six equivalent Cr(3)S6 octahedra. The corner-sharing octahedral tilt angles range from 61-62°. The Mg(1)-S(2) bond length is 2.38 Å. The Mg(1)-S(5) bond length is 2.38 Å. Both Mg(1)-S(3) bond lengths are 2.38 Å. There are three inequivalent Cr sites. In the first Cr site, Cr(1) is bonded to one S(2), one S(6), two equivalent S(3), and two equivalent S(4) atoms to form CrS6 octahedra that share corners with three equivalent Mg(1)S4 tetrahedra, edges with two equivalent Cr(2)S6 octahedra, and edges with four equivalent Cr(3)S6 octahedra. The Cr(1)-S(2) bond length is 2.43 Å. The Cr(1)-S(6) bond length is 2.36 Å. Both Cr(1)-S(3) bond lengths are 2.43 Å. Both Cr(1)-S(4) bond lengths are 2.36 Å. In the second Cr site, Cr(2) is bonded to one S(1), one S(5), two equivalent S(3), and two equivalent S(4) atoms to form CrS6 octahedra that share corners with three equivalent Mg(1)S4 tetrahedra, edges with two equivalent Cr(1)S6 octahedra, and edges with four equivalent Cr(3)S6 octahedra. The Cr(2)-S(1) bond length is 2.36 Å. The Cr(2)-S(5) bond length is 2.43 Å. Both Cr(2)-S(3) bond lengths are 2.43 Å. Both Cr(2)-S(4) bond lengths are 2.36 Å. In the third Cr site, Cr(3) is bonded to one S(1), one S(2), one S(3), one S(4), one S(5), and one S(6) atom to form CrS6 octahedra that share corners with three equivalent Mg(1)S4 tetrahedra, edges 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 Cr(3)-S(1) bond length is 2.36 Å. The Cr(3)-S(2) bond length is 2.43 Å. The Cr(3)-S(3) bond length is 2.43 Å. The Cr(3)-S(4) bond length is 2.36 Å. The Cr(3)-S(5) bond length is 2.43 Å. The Cr(3)-S(6) bond length is 2.36 Å. There are six inequivalent S sites. In the first S site, S(1) is bonded in a distorted T-shaped geometry to one Cr(2) and two equivalent Cr(3) atoms. In the second S site, S(2) is bonded to one Mg(1), one Cr(1), and two equivalent Cr(3) atoms to form a mixture of distorted edge and corner-sharing SMgCr3 tetrahedra. In the third S site, S(3) is bonded to one Mg(1), one Cr(1), one Cr(2), and one Cr(3) atom to form a mixture of distorted edge and corner-sharing SMgCr3 tetrahedra. In the fourth S site, S(4) is bonded in a distorted T-shaped geometry to one Cr(1), one Cr(2), and one Cr(3) atom. In the fifth S site, S(5) is bonded to one Mg(1), one Cr(2), and two equivalent Cr(3) atoms to form a mixture of distorted edge and corner-sharing SMgCr3 tetrahedra. In the sixth S site, S(6) is bonded in a distorted T-shaped geometry to one Cr(1) and two equivalent Cr(3) atoms.