Ta2V3Si crystallizes in the hexagonal P6_3/mmc space group. Ta(1) is bonded in a 16-coordinate geometry to four equivalent Ta(1), nine equivalent V(1), and three equivalent Si(1) atoms. V(1) is bonded to six equivalent Ta(1), four equivalent V(1), and two equivalent Si(1) atoms to form distorted VTa6V4Si2 cuboctahedra that share corners with four equivalent Si(1)Ta6V6 cuboctahedra, corners with fourteen equivalent V(1)Ta6V4Si2 cuboctahedra, edges with six equivalent V(1)Ta6V4Si2 cuboctahedra, faces with six equivalent Si(1)Ta6V6 cuboctahedra, and faces with twelve equivalent V(1)Ta6V4Si2 cuboctahedra. Si(1) is bonded to six equivalent Ta(1) and six equivalent V(1) atoms to form SiTa6V6 cuboctahedra that share corners with twelve equivalent V(1)Ta6V4Si2 cuboctahedra, edges with six equivalent Si(1)Ta6V6 cuboctahedra, faces with two equivalent Si(1)Ta6V6 cuboctahedra, and faces with eighteen equivalent V(1)Ta6V4Si2 cuboctahedra.
Ta2V3Si crystallizes in the hexagonal P6_3/mmc space group. Ta(1) is bonded in a 16-coordinate geometry to four equivalent Ta(1), nine equivalent V(1), and three equivalent Si(1) atoms. There are three shorter (3.02 Å) and one longer (3.15 Å) Ta(1)-Ta(1) bond length. There are six shorter (2.92 Å) and three longer (2.95 Å) Ta(1)-V(1) bond lengths. All Ta(1)-Si(1) bond lengths are 2.88 Å. V(1) is bonded to six equivalent Ta(1), four equivalent V(1), and two equivalent Si(1) atoms to form distorted VTa6V4Si2 cuboctahedra that share corners with four equivalent Si(1)Ta6V6 cuboctahedra, corners with fourteen equivalent V(1)Ta6V4Si2 cuboctahedra, edges with six equivalent V(1)Ta6V4Si2 cuboctahedra, faces with six equivalent Si(1)Ta6V6 cuboctahedra, and faces with twelve equivalent V(1)Ta6V4Si2 cuboctahedra. There are two shorter (2.40 Å) and two longer (2.52 Å) V(1)-V(1) bond lengths. Both V(1)-Si(1) bond lengths are 2.55 Å. Si(1) is bonded to six equivalent Ta(1) and six equivalent V(1) atoms to form SiTa6V6 cuboctahedra that share corners with twelve equivalent V(1)Ta6V4Si2 cuboctahedra, edges with six equivalent Si(1)Ta6V6 cuboctahedra, faces with two equivalent Si(1)Ta6V6 cuboctahedra, and faces with eighteen equivalent V(1)Ta6V4Si2 cuboctahedra.