Ca3(OsN2)2 crystallizes in the orthorhombic Pnna space group. There are two inequivalent Ca sites. In the first Ca site, Ca(1) is bonded in a 5-coordinate geometry to two equivalent N(1) and three equivalent N(2) atoms. In the second Ca site, Ca(2) is bonded in a 6-coordinate geometry to two equivalent N(2) and four equivalent N(1) atoms. There are two inequivalent Os sites. In the first Os site, Os(1) is bonded in a 4-coordinate geometry to two equivalent N(1) and two equivalent N(2) atoms. In the second Os site, Os(2) is bonded in a 4-coordinate geometry to two equivalent N(1) and two equivalent N(2) atoms. There are two inequivalent N sites. In the first N site, N(1) is bonded to two equivalent Ca(1), two equivalent Ca(2), one Os(1), and one Os(2) atom to form a mixture of distorted corner, face, and edge-sharing NCa4Os2 octahedra. The corner-sharing octahedral tilt angles range from 10-82°. In the second N site, N(2) is bonded to one Ca(2), three equivalent Ca(1), one Os(1), and one Os(2) atom to form a mixture of distorted corner, face, and edge-sharing NCa4Os2 octahedra. The corner-sharing octahedral tilt angles range from 10-82°.
Ca3(OsN2)2 crystallizes in the orthorhombic Pnna space group. There are two inequivalent Ca sites. In the first Ca site, Ca(1) is bonded in a 5-coordinate geometry to two equivalent N(1) and three equivalent N(2) atoms. There is one shorter (2.45 Å) and one longer (2.63 Å) Ca(1)-N(1) bond length. There are a spread of Ca(1)-N(2) bond distances ranging from 2.36-2.80 Å. In the second Ca site, Ca(2) is bonded in a 6-coordinate geometry to two equivalent N(2) and four equivalent N(1) atoms. Both Ca(2)-N(2) bond lengths are 2.53 Å. There are two shorter (2.43 Å) and two longer (2.82 Å) Ca(2)-N(1) bond lengths. There are two inequivalent Os sites. In the first Os site, Os(1) is bonded in a 4-coordinate geometry to two equivalent N(1) and two equivalent N(2) atoms. Both Os(1)-N(1) bond lengths are 2.02 Å. Both Os(1)-N(2) bond lengths are 2.05 Å. In the second Os site, Os(2) is bonded in a 4-coordinate geometry to two equivalent N(1) and two equivalent N(2) atoms. Both Os(2)-N(1) bond lengths are 2.01 Å. Both Os(2)-N(2) bond lengths are 2.11 Å. There are two inequivalent N sites. In the first N site, N(1) is bonded to two equivalent Ca(1), two equivalent Ca(2), one Os(1), and one Os(2) atom to form a mixture of distorted corner, face, and edge-sharing NCa4Os2 octahedra. The corner-sharing octahedral tilt angles range from 10-82°. In the second N site, N(2) is bonded to one Ca(2), three equivalent Ca(1), one Os(1), and one Os(2) atom to form a mixture of distorted corner, face, and edge-sharing NCa4Os2 octahedra. The corner-sharing octahedral tilt angles range from 10-82°.