Laser-ablated Mo and W atoms react with N-2 in excess nitrogen and argon to form the metal nitrides, MN, and ligated complexes, (NN)(x)MN, the metal dinitrides, NMN, and ligated complexes, (NN)(x)MN2, and several complexes M(NN)(x) leading up to the octahedral species with x = 6. On the basis of the resolution of natural abundance Mo isotopes and N-15 substitution, the open, bent NMoN molecule valence angle is 106 +/- 3 degrees. The dinitride molecules are formed both by direct insertion of metastable metal atoms into dinitrogen and by the addition of atomic nitrogen to the mononitride molecule.