U2Cr3Si crystallizes in the hexagonal P6_3/mmc space group. U(1) is bonded in a 13-coordinate geometry to one U(1), nine equivalent Cr(1), and three equivalent Si(1) atoms. Cr(1) is bonded to six equivalent U(1), four equivalent Cr(1), and two equivalent Si(1) atoms to form distorted CrU6Cr4Si2 cuboctahedra that share corners with four equivalent Si(1)U6Cr6 cuboctahedra, corners with fourteen equivalent Cr(1)U6Cr4Si2 cuboctahedra, edges with six equivalent Cr(1)U6Cr4Si2 cuboctahedra, faces with six equivalent Si(1)U6Cr6 cuboctahedra, and faces with twelve equivalent Cr(1)U6Cr4Si2 cuboctahedra. Si(1) is bonded to six equivalent U(1) and six equivalent Cr(1) atoms to form SiU6Cr6 cuboctahedra that share corners with twelve equivalent Cr(1)U6Cr4Si2 cuboctahedra, edges with six equivalent Si(1)U6Cr6 cuboctahedra, faces with two equivalent Si(1)U6Cr6 cuboctahedra, and faces with eighteen equivalent Cr(1)U6Cr4Si2 cuboctahedra.
U2Cr3Si crystallizes in the hexagonal P6_3/mmc space group. U(1) is bonded in a 13-coordinate geometry to one U(1), nine equivalent Cr(1), and three equivalent Si(1) atoms. The U(1)-U(1) bond length is 2.65 Å. There are six shorter (2.88 Å) and three longer (3.06 Å) U(1)-Cr(1) bond lengths. All U(1)-Si(1) bond lengths are 3.04 Å. Cr(1) is bonded to six equivalent U(1), four equivalent Cr(1), and two equivalent Si(1) atoms to form distorted CrU6Cr4Si2 cuboctahedra that share corners with four equivalent Si(1)U6Cr6 cuboctahedra, corners with fourteen equivalent Cr(1)U6Cr4Si2 cuboctahedra, edges with six equivalent Cr(1)U6Cr4Si2 cuboctahedra, faces with six equivalent Si(1)U6Cr6 cuboctahedra, and faces with twelve equivalent Cr(1)U6Cr4Si2 cuboctahedra. There are two shorter (2.47 Å) and two longer (2.65 Å) Cr(1)-Cr(1) bond lengths. Both Cr(1)-Si(1) bond lengths are 2.53 Å. Si(1) is bonded to six equivalent U(1) and six equivalent Cr(1) atoms to form SiU6Cr6 cuboctahedra that share corners with twelve equivalent Cr(1)U6Cr4Si2 cuboctahedra, edges with six equivalent Si(1)U6Cr6 cuboctahedra, faces with two equivalent Si(1)U6Cr6 cuboctahedra, and faces with eighteen equivalent Cr(1)U6Cr4Si2 cuboctahedra.