Cr3Si5 crystallizes in the tetragonal I4/mcm space group. There are two inequivalent Cr sites. In the first Cr site, Cr(1) is bonded in a 10-coordinate geometry to two equivalent Si(2) and eight equivalent Si(1) atoms. In the second Cr site, Cr(2) is bonded in a 10-coordinate geometry to two equivalent Cr(2) and eight equivalent Si(1) atoms. There are two inequivalent Si sites. In the first Si site, Si(2) is bonded in a 6-coordinate geometry to four equivalent Cr(1), two equivalent Si(2), and eight equivalent Si(1) atoms. In the second Si site, Si(1) is bonded in a 11-coordinate geometry to two equivalent Cr(2), four equivalent Cr(1), two equivalent Si(2), and three equivalent Si(1) atoms.
Cr3Si5 crystallizes in the tetragonal I4/mcm space group. There are two inequivalent Cr sites. In the first Cr site, Cr(1) is bonded in a 10-coordinate geometry to two equivalent Si(2) and eight equivalent Si(1) atoms. Both Cr(1)-Si(2) bond lengths are 2.55 Å. There are a spread of Cr(1)-Si(1) bond distances ranging from 2.41-2.68 Å. In the second Cr site, Cr(2) is bonded in a 10-coordinate geometry to two equivalent Cr(2) and eight equivalent Si(1) atoms. Both Cr(2)-Cr(2) bond lengths are 2.35 Å. All Cr(2)-Si(1) bond lengths are 2.56 Å. There are two inequivalent Si sites. In the first Si site, Si(2) is bonded in a 6-coordinate geometry to four equivalent Cr(1), two equivalent Si(2), and eight equivalent Si(1) atoms. Both Si(2)-Si(2) bond lengths are 2.35 Å. All Si(2)-Si(1) bond lengths are 2.80 Å. In the second Si site, Si(1) is bonded in a 11-coordinate geometry to two equivalent Cr(2), four equivalent Cr(1), two equivalent Si(2), and three equivalent Si(1) atoms. There is one shorter (2.56 Å) and two longer (2.69 Å) Si(1)-Si(1) bond lengths.