Gd2Cr2O5 crystallizes in the tetragonal P4/mmm space group. There are two inequivalent Gd sites. In the first Gd site, Gd(1) is bonded in a body-centered cubic geometry to eight equivalent O(1) atoms. In the second Gd site, Gd(2) is bonded to four equivalent O(2) and eight equivalent O(1) atoms to form GdO12 cuboctahedra that share corners with four equivalent Gd(2)O12 cuboctahedra, faces with four equivalent Gd(2)O12 cuboctahedra, and faces with eight equivalent Cr(1)O5 square pyramids. Cr(1) is bonded to one O(2) and four equivalent O(1) atoms to form CrO5 square pyramids that share corners with five equivalent Cr(1)O5 square pyramids and faces with four equivalent Gd(2)O12 cuboctahedra. There are two inequivalent O sites. In the first O site, O(1) is bonded to two equivalent Gd(1), two equivalent Gd(2), and two equivalent Cr(1) atoms to form a mixture of distorted edge, face, and corner-sharing OGd4Cr2 octahedra. The corner-sharing octahedral tilt angles range from 0-66°. In the second O site, O(2) is bonded to four equivalent Gd(2) and two equivalent Cr(1) atoms to form a mixture of distorted edge, face, and corner-sharing OGd4Cr2 octahedra. The corner-sharing octahedral tilt angles range from 0-60°.
Gd2Cr2O5 crystallizes in the tetragonal P4/mmm space group. There are two inequivalent Gd sites. In the first Gd site, Gd(1) is bonded in a body-centered cubic geometry to eight equivalent O(1) atoms. All Gd(1)-O(1) bond lengths are 2.53 Å. In the second Gd site, Gd(2) is bonded to four equivalent O(2) and eight equivalent O(1) atoms to form GdO12 cuboctahedra that share corners with four equivalent Gd(2)O12 cuboctahedra, faces with four equivalent Gd(2)O12 cuboctahedra, and faces with eight equivalent Cr(1)O5 square pyramids. All Gd(2)-O(2) bond lengths are 2.77 Å. All Gd(2)-O(1) bond lengths are 2.78 Å. Cr(1) is bonded to one O(2) and four equivalent O(1) atoms to form CrO5 square pyramids that share corners with five equivalent Cr(1)O5 square pyramids and faces with four equivalent Gd(2)O12 cuboctahedra. The Cr(1)-O(2) bond length is 2.01 Å. All Cr(1)-O(1) bond lengths are 1.96 Å. There are two inequivalent O sites. In the first O site, O(1) is bonded to two equivalent Gd(1), two equivalent Gd(2), and two equivalent Cr(1) atoms to form a mixture of distorted edge, face, and corner-sharing OGd4Cr2 octahedra. The corner-sharing octahedral tilt angles range from 0-66°. In the second O site, O(2) is bonded to four equivalent Gd(2) and two equivalent Cr(1) atoms to form a mixture of distorted edge, face, and corner-sharing OGd4Cr2 octahedra. The corner-sharing octahedral tilt angles range from 0-60°.