Sm(GdS2)2 crystallizes in the tetragonal I-42d space group. Gd(1) is bonded to eight equivalent S(1) atoms to form distorted GdS8 hexagonal bipyramids that share corners with four equivalent Gd(1)S8 hexagonal bipyramids, corners with four equivalent Sm(1)S8 hexagonal bipyramids, edges with four equivalent Gd(1)S8 hexagonal bipyramids, faces with four equivalent Gd(1)S8 hexagonal bipyramids, and faces with four equivalent Sm(1)S8 hexagonal bipyramids. Sm(1) is bonded to eight equivalent S(1) atoms to form distorted SmS8 hexagonal bipyramids that share corners with eight equivalent Gd(1)S8 hexagonal bipyramids, edges with four equivalent Sm(1)S8 hexagonal bipyramids, and faces with eight equivalent Gd(1)S8 hexagonal bipyramids. S(1) is bonded to four equivalent Gd(1) and two equivalent Sm(1) atoms to form a mixture of distorted corner, face, and edge-sharing SSm2Gd4 octahedra. The corner-sharing octahedral tilt angles range from 17-50°.
Sm(GdS2)2 crystallizes in the tetragonal I-42d space group. Gd(1) is bonded to eight equivalent S(1) atoms to form distorted GdS8 hexagonal bipyramids that share corners with four equivalent Gd(1)S8 hexagonal bipyramids, corners with four equivalent Sm(1)S8 hexagonal bipyramids, edges with four equivalent Gd(1)S8 hexagonal bipyramids, faces with four equivalent Gd(1)S8 hexagonal bipyramids, and faces with four equivalent Sm(1)S8 hexagonal bipyramids. There are a spread of Gd(1)-S(1) bond distances ranging from 2.83-3.02 Å. Sm(1) is bonded to eight equivalent S(1) atoms to form distorted SmS8 hexagonal bipyramids that share corners with eight equivalent Gd(1)S8 hexagonal bipyramids, edges with four equivalent Sm(1)S8 hexagonal bipyramids, and faces with eight equivalent Gd(1)S8 hexagonal bipyramids. There are four shorter (2.85 Å) and four longer (3.01 Å) Sm(1)-S(1) bond lengths. S(1) is bonded to four equivalent Gd(1) and two equivalent Sm(1) atoms to form a mixture of distorted corner, face, and edge-sharing SSm2Gd4 octahedra. The corner-sharing octahedral tilt angles range from 17-50°.