CrFe3As2 crystallizes in the tetragonal P-4m2 space group. Cr(1) is bonded to four equivalent Fe(1), four equivalent Fe(2), and four equivalent As(1) atoms to form CrFe8As4 cuboctahedra that share corners with four equivalent Cr(1)Fe8As4 cuboctahedra, faces with four equivalent Cr(1)Fe8As4 cuboctahedra, and faces with four equivalent Fe(1)Cr4Fe4As4 cuboctahedra. There are two inequivalent Fe sites. In the first Fe site, Fe(1) is bonded to four equivalent Cr(1), four equivalent Fe(2), and four equivalent As(1) atoms to form distorted FeCr4Fe4As4 cuboctahedra that share corners with four equivalent Fe(1)Cr4Fe4As4 cuboctahedra, faces with four equivalent Cr(1)Fe8As4 cuboctahedra, and faces with four equivalent Fe(1)Cr4Fe4As4 cuboctahedra. In the second Fe site, Fe(2) is bonded in a 5-coordinate geometry to two equivalent Cr(1), two equivalent Fe(1), and five equivalent As(1) atoms. As(1) is bonded in a 9-coordinate geometry to two equivalent Cr(1), two equivalent Fe(1), and five equivalent Fe(2) atoms.
CrFe3As2 crystallizes in the tetragonal P-4m2 space group. Cr(1) is bonded to four equivalent Fe(1), four equivalent Fe(2), and four equivalent As(1) atoms to form CrFe8As4 cuboctahedra that share corners with four equivalent Cr(1)Fe8As4 cuboctahedra, faces with four equivalent Cr(1)Fe8As4 cuboctahedra, and faces with four equivalent Fe(1)Cr4Fe4As4 cuboctahedra. All Cr(1)-Fe(1) bond lengths are 2.59 Å. All Cr(1)-Fe(2) bond lengths are 2.69 Å. All Cr(1)-As(1) bond lengths are 2.47 Å. There are two inequivalent Fe sites. In the first Fe site, Fe(1) is bonded to four equivalent Cr(1), four equivalent Fe(2), and four equivalent As(1) atoms to form distorted FeCr4Fe4As4 cuboctahedra that share corners with four equivalent Fe(1)Cr4Fe4As4 cuboctahedra, faces with four equivalent Cr(1)Fe8As4 cuboctahedra, and faces with four equivalent Fe(1)Cr4Fe4As4 cuboctahedra. All Fe(1)-Fe(2) bond lengths are 2.69 Å. All Fe(1)-As(1) bond lengths are 2.47 Å. In the second Fe site, Fe(2) is bonded in a 5-coordinate geometry to two equivalent Cr(1), two equivalent Fe(1), and five equivalent As(1) atoms. There is one shorter (2.44 Å) and four longer (2.61 Å) Fe(2)-As(1) bond lengths. As(1) is bonded in a 9-coordinate geometry to two equivalent Cr(1), two equivalent Fe(1), and five equivalent Fe(2) atoms.