Ca3Os3N5 is Orthorhombic Perovskite-like structured and crystallizes in the triclinic P-1 space group. There are three inequivalent Ca sites. In the first Ca site, Ca(1) is bonded in a 5-coordinate geometry to one N(3), two equivalent N(2), and two equivalent N(4) atoms. In the second Ca site, Ca(2) is bonded in a 6-coordinate geometry to one N(3), one N(4), two equivalent N(1), and two equivalent N(5) atoms. In the third Ca site, Ca(3) is bonded in a 5-coordinate geometry to one N(1), one N(2), one N(4), two equivalent N(3), and two equivalent N(5) atoms. There are three inequivalent Os sites. In the first Os site, Os(1) is bonded in a 4-coordinate geometry to one N(1), one N(5), and two equivalent N(3) atoms. In the second Os site, Os(2) is bonded in a distorted rectangular see-saw-like geometry to two equivalent N(2) and two equivalent N(4) atoms. In the third Os site, Os(3) is bonded in a 3-coordinate geometry to one N(1), one N(2), and one N(5) atom. There are five inequivalent N sites. In the first N site, N(1) is bonded to one Ca(3), two equivalent Ca(2), one Os(1), and one Os(3) atom to form distorted NCa3Os2 trigonal bipyramids that share corners with three equivalent N(3)Ca4Os2 octahedra, corners with two equivalent N(2)Ca3Os3 pentagonal pyramids,  an edgeedge with one N(1)Ca3Os2 trigonal bipyramid, and  a faceface with one N(3)Ca4Os2 octahedra. The corner-sharing octahedral tilt angles range from 24-71°. In the second N site, N(2) is bonded to one Ca(3), two equivalent Ca(1), one Os(3), and two equivalent Os(2) atoms to form distorted NCa3Os3 pentagonal pyramids that share corners with four equivalent N(3)Ca4Os2 octahedra, corners with two equivalent N(1)Ca3Os2 trigonal bipyramids, and edges with two equivalent N(2)Ca3Os3 pentagonal pyramids. The corner-sharing octahedral tilt angles range from 50-58°. In the third N site, N(3) is bonded to one Ca(1), one Ca(2), two equivalent Ca(3), and two equivalent Os(1) atoms to form distorted NCa4Os2 octahedra that share corners with four equivalent N(2)Ca3Os3 pentagonal pyramids, corners with three equivalent N(1)Ca3Os2 trigonal bipyramids, edges with two equivalent N(3)Ca4Os2 octahedra, and  a faceface with one N(1)Ca3Os2 trigonal bipyramid. In the fourth N site, N(4) is bonded in a 6-coordinate geometry to one Ca(2), one Ca(3), two equivalent Ca(1), and two equivalent Os(2) atoms. In the fifth N site, N(5) is bonded in a 6-coordinate geometry to two equivalent Ca(2), two equivalent Ca(3), one Os(1), and one Os(3) atom.
Ca3Os3N5 is Orthorhombic Perovskite-like structured and crystallizes in the triclinic P-1 space group. There are three inequivalent Ca sites. In the first Ca site, Ca(1) is bonded in a 5-coordinate geometry to one N(3), two equivalent N(2), and two equivalent N(4) atoms. The Ca(1)-N(3) bond length is 2.42 Å. There is one shorter (2.52 Å) and one longer (2.71 Å) Ca(1)-N(2) bond length. There is one shorter (2.39 Å) and one longer (2.66 Å) Ca(1)-N(4) bond length. In the second Ca site, Ca(2) is bonded in a 6-coordinate geometry to one N(3), one N(4), two equivalent N(1), and two equivalent N(5) atoms. The Ca(2)-N(3) bond length is 2.58 Å. The Ca(2)-N(4) bond length is 2.57 Å. There is one shorter (2.45 Å) and one longer (2.71 Å) Ca(2)-N(1) bond length. There is one shorter (2.32 Å) and one longer (2.56 Å) Ca(2)-N(5) bond length. In the third Ca site, Ca(3) is bonded in a 5-coordinate geometry to one N(1), one N(2), one N(4), two equivalent N(3), and two equivalent N(5) atoms. The Ca(3)-N(1) bond length is 2.66 Å. The Ca(3)-N(2) bond length is 2.84 Å. The Ca(3)-N(4) bond length is 3.07 Å. There is one shorter (2.42 Å) and one longer (2.64 Å) Ca(3)-N(3) bond length. There is one shorter (2.47 Å) and one longer (3.03 Å) Ca(3)-N(5) bond length. There are three inequivalent Os sites. In the first Os site, Os(1) is bonded in a 4-coordinate geometry to one N(1), one N(5), and two equivalent N(3) atoms. The Os(1)-N(1) bond length is 1.86 Å. The Os(1)-N(5) bond length is 1.95 Å. There is one shorter (2.01 Å) and one longer (2.12 Å) Os(1)-N(3) bond length. In the second Os site, Os(2) is bonded in a distorted rectangular see-saw-like geometry to two equivalent N(2) and two equivalent N(4) atoms. There is one shorter (2.22 Å) and one longer (2.29 Å) Os(2)-N(2) bond length. There is one shorter (1.98 Å) and one longer (2.00 Å) Os(2)-N(4) bond length. In the third Os site, Os(3) is bonded in a 3-coordinate geometry to one N(1), one N(2), and one N(5) atom. The Os(3)-N(1) bond length is 1.83 Å. The Os(3)-N(2) bond length is 1.99 Å. The Os(3)-N(5) bond length is 2.03 Å. There are five inequivalent N sites. In the first N site, N(1) is bonded to one Ca(3), two equivalent Ca(2), one Os(1), and one Os(3) atom to form distorted NCa3Os2 trigonal bipyramids that share corners with three equivalent N(3)Ca4Os2 octahedra, corners with two equivalent N(2)Ca3Os3 pentagonal pyramids,  an edgeedge with one N(1)Ca3Os2 trigonal bipyramid, and  a faceface with one N(3)Ca4Os2 octahedra. The corner-sharing octahedral tilt angles range from 24-71°. In the second N site, N(2) is bonded to one Ca(3), two equivalent Ca(1), one Os(3), and two equivalent Os(2) atoms to form distorted NCa3Os3 pentagonal pyramids that share corners with four equivalent N(3)Ca4Os2 octahedra, corners with two equivalent N(1)Ca3Os2 trigonal bipyramids, and edges with two equivalent N(2)Ca3Os3 pentagonal pyramids. The corner-sharing octahedral tilt angles range from 50-58°. In the third N site, N(3) is bonded to one Ca(1), one Ca(2), two equivalent Ca(3), and two equivalent Os(1) atoms to form distorted NCa4Os2 octahedra that share corners with four equivalent N(2)Ca3Os3 pentagonal pyramids, corners with three equivalent N(1)Ca3Os2 trigonal bipyramids, edges with two equivalent N(3)Ca4Os2 octahedra, and  a faceface with one N(1)Ca3Os2 trigonal bipyramid. In the fourth N site, N(4) is bonded in a 6-coordinate geometry to one Ca(2), one Ca(3), two equivalent Ca(1), and two equivalent Os(2) atoms. In the fifth N site, N(5) is bonded in a 6-coordinate geometry to two equivalent Ca(2), two equivalent Ca(3), one Os(1), and one Os(3) atom.