CsCrAs2O7 crystallizes in the monoclinic P2_1/c space group. Cs(1) is bonded in a 10-coordinate geometry to one O(1), one O(3), one O(4), one O(5), two equivalent O(2), two equivalent O(6), and two equivalent O(7) atoms. Cr(1) is bonded to one O(1), one O(2), one O(3), one O(5), one O(6), and one O(7) atom to form CrO6 octahedra that share corners with three equivalent As(1)O4 tetrahedra and corners with three equivalent As(2)O4 tetrahedra. There are two inequivalent As sites. In the first As site, As(1) is bonded to one O(1), one O(2), one O(3), and one O(4) atom to form AsO4 tetrahedra that share corners with three equivalent Cr(1)O6 octahedra and  a cornercorner with one As(2)O4 tetrahedra. The corner-sharing octahedral tilt angles range from 28-54°. In the second As site, As(2) is bonded to one O(4), one O(5), one O(6), and one O(7) atom to form AsO4 tetrahedra that share corners with three equivalent Cr(1)O6 octahedra and  a cornercorner with one As(1)O4 tetrahedra. The corner-sharing octahedral tilt angles range from 18-46°. There are seven inequivalent O sites. In the first O site, O(5) is bonded in a distorted bent 150 degrees geometry to one Cs(1), one Cr(1), and one As(2) atom. In the second O site, O(6) is bonded in a 2-coordinate geometry to two equivalent Cs(1), one Cr(1), and one As(2) atom. In the third O site, O(7) is bonded in a 2-coordinate geometry to two equivalent Cs(1), one Cr(1), and one As(2) atom. In the fourth O site, O(1) is bonded in a bent 150 degrees geometry to one Cs(1), one Cr(1), and one As(1) atom. In the fifth O site, O(2) is bonded in a 2-coordinate geometry to two equivalent Cs(1), one Cr(1), and one As(1) atom. In the sixth O site, O(3) is bonded in a distorted bent 120 degrees geometry to one Cs(1), one Cr(1), and one As(1) atom. In the seventh O site, O(4) is bonded in a bent 120 degrees geometry to one Cs(1), one As(1), and one As(2) atom.
CsCrAs2O7 crystallizes in the monoclinic P2_1/c space group. Cs(1) is bonded in a 10-coordinate geometry to one O(1), one O(3), one O(4), one O(5), two equivalent O(2), two equivalent O(6), and two equivalent O(7) atoms. The Cs(1)-O(1) bond length is 3.23 Å. The Cs(1)-O(3) bond length is 3.05 Å. The Cs(1)-O(4) bond length is 3.32 Å. The Cs(1)-O(5) bond length is 3.39 Å. There is one shorter (3.17 Å) and one longer (3.27 Å) Cs(1)-O(2) bond length. There is one shorter (3.11 Å) and one longer (3.13 Å) Cs(1)-O(6) bond length. There is one shorter (2.96 Å) and one longer (3.19 Å) Cs(1)-O(7) bond length. Cr(1) is bonded to one O(1), one O(2), one O(3), one O(5), one O(6), and one O(7) atom to form CrO6 octahedra that share corners with three equivalent As(1)O4 tetrahedra and corners with three equivalent As(2)O4 tetrahedra. The Cr(1)-O(1) bond length is 1.99 Å. The Cr(1)-O(2) bond length is 2.03 Å. The Cr(1)-O(3) bond length is 1.98 Å. The Cr(1)-O(5) bond length is 1.96 Å. The Cr(1)-O(6) bond length is 2.02 Å. The Cr(1)-O(7) bond length is 1.95 Å. There are two inequivalent As sites. In the first As site, As(1) is bonded to one O(1), one O(2), one O(3), and one O(4) atom to form AsO4 tetrahedra that share corners with three equivalent Cr(1)O6 octahedra and  a cornercorner with one As(2)O4 tetrahedra. The corner-sharing octahedral tilt angles range from 28-54°. The As(1)-O(1) bond length is 1.67 Å. The As(1)-O(2) bond length is 1.68 Å. The As(1)-O(3) bond length is 1.69 Å. The As(1)-O(4) bond length is 1.78 Å. In the second As site, As(2) is bonded to one O(4), one O(5), one O(6), and one O(7) atom to form AsO4 tetrahedra that share corners with three equivalent Cr(1)O6 octahedra and  a cornercorner with one As(1)O4 tetrahedra. The corner-sharing octahedral tilt angles range from 18-46°. The As(2)-O(4) bond length is 1.77 Å. The As(2)-O(5) bond length is 1.65 Å. The As(2)-O(6) bond length is 1.68 Å. The As(2)-O(7) bond length is 1.69 Å. There are seven inequivalent O sites. In the first O site, O(5) is bonded in a distorted bent 150 degrees geometry to one Cs(1), one Cr(1), and one As(2) atom. In the second O site, O(6) is bonded in a 2-coordinate geometry to two equivalent Cs(1), one Cr(1), and one As(2) atom. In the third O site, O(7) is bonded in a 2-coordinate geometry to two equivalent Cs(1), one Cr(1), and one As(2) atom. In the fourth O site, O(1) is bonded in a bent 150 degrees geometry to one Cs(1), one Cr(1), and one As(1) atom. In the fifth O site, O(2) is bonded in a 2-coordinate geometry to two equivalent Cs(1), one Cr(1), and one As(1) atom. In the sixth O site, O(3) is bonded in a distorted bent 120 degrees geometry to one Cs(1), one Cr(1), and one As(1) atom. In the seventh O site, O(4) is bonded in a bent 120 degrees geometry to one Cs(1), one As(1), and one As(2) atom.