Ba3Mo3N5 crystallizes in the triclinic P-1 space group. There are three inequivalent Ba sites. In the first Ba site, Ba(1) is bonded in a 6-coordinate geometry to one N(1), one N(3), one N(4), one N(5), and two equivalent N(2) atoms. In the second Ba site, Ba(2) is bonded in a 6-coordinate geometry to one N(1), one N(3), one N(4), and three equivalent N(5) atoms. In the third Ba site, Ba(3) is bonded in a 5-coordinate geometry to one N(1), one N(2), one N(4), and two equivalent N(3) atoms. There are three inequivalent Mo sites. In the first Mo site, Mo(1) is bonded to one N(1), one N(5), and two equivalent N(3) atoms to form a mixture of corner and edge-sharing MoN4 tetrahedra. In the second Mo site, Mo(2) is bonded to one N(1), one N(2), and two equivalent N(4) atoms to form a mixture of distorted corner and edge-sharing MoN4 tetrahedra. In the third Mo site, Mo(3) is bonded to one N(1), one N(2), one N(4), and one N(5) atom to form a mixture of corner and edge-sharing MoN4 tetrahedra. There are five inequivalent N sites. In the first N site, N(1) is bonded in a 6-coordinate geometry to one Ba(1), one Ba(2), one Ba(3), one Mo(1), one Mo(2), and one Mo(3) atom. In the second N site, N(2) is bonded to one Ba(3), two equivalent Ba(1), one Mo(2), and one Mo(3) atom to form distorted NBa3Mo2 trigonal bipyramids that share corners with four equivalent N(3)Ba4Mo2 octahedra and  an edgeedge with one N(2)Ba3Mo2 trigonal bipyramid. The corner-sharing octahedral tilt angles range from 46-71°. In the third N site, N(3) is bonded to one Ba(1), one Ba(2), two equivalent Ba(3), and two equivalent Mo(1) atoms to form NBa4Mo2 octahedra that share corners with four equivalent N(2)Ba3Mo2 trigonal bipyramids and edges with two equivalent N(3)Ba4Mo2 octahedra. In the fourth N site, N(4) is bonded in a 6-coordinate geometry to one Ba(1), one Ba(2), one Ba(3), one Mo(3), and two equivalent Mo(2) atoms. In the fifth N site, N(5) is bonded in a 2-coordinate geometry to one Ba(1), three equivalent Ba(2), one Mo(1), and one Mo(3) atom.
Ba3Mo3N5 crystallizes in the triclinic P-1 space group. There are three inequivalent Ba sites. In the first Ba site, Ba(1) is bonded in a 6-coordinate geometry to one N(1), one N(3), one N(4), one N(5), and two equivalent N(2) atoms. The Ba(1)-N(1) bond length is 3.17 Å. The Ba(1)-N(3) bond length is 2.91 Å. The Ba(1)-N(4) bond length is 2.96 Å. The Ba(1)-N(5) bond length is 3.29 Å. There is one shorter (2.76 Å) and one longer (2.79 Å) Ba(1)-N(2) bond length. In the second Ba site, Ba(2) is bonded in a 6-coordinate geometry to one N(1), one N(3), one N(4), and three equivalent N(5) atoms. The Ba(2)-N(1) bond length is 2.94 Å. The Ba(2)-N(3) bond length is 2.81 Å. The Ba(2)-N(4) bond length is 2.92 Å. There are a spread of Ba(2)-N(5) bond distances ranging from 2.90-3.25 Å. In the third Ba site, Ba(3) is bonded in a 5-coordinate geometry to one N(1), one N(2), one N(4), and two equivalent N(3) atoms. The Ba(3)-N(1) bond length is 3.06 Å. The Ba(3)-N(2) bond length is 2.79 Å. The Ba(3)-N(4) bond length is 3.01 Å. There is one shorter (2.76 Å) and one longer (2.79 Å) Ba(3)-N(3) bond length. There are three inequivalent Mo sites. In the first Mo site, Mo(1) is bonded to one N(1), one N(5), and two equivalent N(3) atoms to form a mixture of corner and edge-sharing MoN4 tetrahedra. The Mo(1)-N(1) bond length is 1.99 Å. The Mo(1)-N(5) bond length is 1.98 Å. There is one shorter (2.01 Å) and one longer (2.02 Å) Mo(1)-N(3) bond length. In the second Mo site, Mo(2) is bonded to one N(1), one N(2), and two equivalent N(4) atoms to form a mixture of distorted corner and edge-sharing MoN4 tetrahedra. The Mo(2)-N(1) bond length is 2.08 Å. The Mo(2)-N(2) bond length is 1.99 Å. Both Mo(2)-N(4) bond lengths are 2.09 Å. In the third Mo site, Mo(3) is bonded to one N(1), one N(2), one N(4), and one N(5) atom to form a mixture of corner and edge-sharing MoN4 tetrahedra. The Mo(3)-N(1) bond length is 2.14 Å. The Mo(3)-N(2) bond length is 2.00 Å. The Mo(3)-N(4) bond length is 2.03 Å. The Mo(3)-N(5) bond length is 1.96 Å. There are five inequivalent N sites. In the first N site, N(1) is bonded in a 6-coordinate geometry to one Ba(1), one Ba(2), one Ba(3), one Mo(1), one Mo(2), and one Mo(3) atom. In the second N site, N(2) is bonded to one Ba(3), two equivalent Ba(1), one Mo(2), and one Mo(3) atom to form distorted NBa3Mo2 trigonal bipyramids that share corners with four equivalent N(3)Ba4Mo2 octahedra and  an edgeedge with one N(2)Ba3Mo2 trigonal bipyramid. The corner-sharing octahedral tilt angles range from 46-71°. In the third N site, N(3) is bonded to one Ba(1), one Ba(2), two equivalent Ba(3), and two equivalent Mo(1) atoms to form NBa4Mo2 octahedra that share corners with four equivalent N(2)Ba3Mo2 trigonal bipyramids and edges with two equivalent N(3)Ba4Mo2 octahedra. In the fourth N site, N(4) is bonded in a 6-coordinate geometry to one Ba(1), one Ba(2), one Ba(3), one Mo(3), and two equivalent Mo(2) atoms. In the fifth N site, N(5) is bonded in a 2-coordinate geometry to one Ba(1), three equivalent Ba(2), one Mo(1), and one Mo(3) atom.