LiTaS2 is Caswellsilverite-like structured and crystallizes in the hexagonal P6_3/mmc space group. Li(1) is bonded to six equivalent S(1) atoms to form LiS6 octahedra that share corners with twelve equivalent Ta(1)S6 pentagonal pyramids, edges with six equivalent Li(1)S6 octahedra, and faces with two equivalent Ta(1)S6 pentagonal pyramids. Ta(1) is bonded to six equivalent S(1) atoms to form distorted TaS6 pentagonal pyramids that share corners with twelve equivalent Li(1)S6 octahedra, edges with six equivalent Ta(1)S6 pentagonal pyramids, and faces with two equivalent Li(1)S6 octahedra. The corner-sharing octahedral tilt angles are 45°. S(1) is bonded to three equivalent Li(1) and three equivalent Ta(1) atoms to form a mixture of distorted edge, face, and corner-sharing SLi3Ta3 pentagonal pyramids.
LiTaS2 is Caswellsilverite-like structured and crystallizes in the hexagonal P6_3/mmc space group. Li(1) is bonded to six equivalent S(1) atoms to form LiS6 octahedra that share corners with twelve equivalent Ta(1)S6 pentagonal pyramids, edges with six equivalent Li(1)S6 octahedra, and faces with two equivalent Ta(1)S6 pentagonal pyramids. All Li(1)-S(1) bond lengths are 2.54 Å. Ta(1) is bonded to six equivalent S(1) atoms to form distorted TaS6 pentagonal pyramids that share corners with twelve equivalent Li(1)S6 octahedra, edges with six equivalent Ta(1)S6 pentagonal pyramids, and faces with two equivalent Li(1)S6 octahedra. The corner-sharing octahedral tilt angles are 45°. All Ta(1)-S(1) bond lengths are 2.49 Å. S(1) is bonded to three equivalent Li(1) and three equivalent Ta(1) atoms to form a mixture of distorted edge, face, and corner-sharing SLi3Ta3 pentagonal pyramids.