Abstract
Laser ablated Be atoms have been reacted with acetonitrile molecules in 4 K solid neon matrix. The diberyllium products BeBeNCCH(3) and CNBeBeCH(3) have been identified by D and (13)C isotopic substitutions and quantum chemical calculations. The stabilization of the diberyllium species is rationalized from the formation of the real Be-Be single bonds with bond distances as 2.077 and 2.058 Å and binding energies as -27.1 and -77.2 kcal/mol calculated at CCSD (T)/aug-cc-pVTZ level of theory for BeBeNCCH(3) and CNBeBeCH(3), respectively. EDA-NOCV analysis described the interaction between Be(2) and NC···CH(3) fragments as Lewis "acid-base" interactions. In the complexes, the Be(2) moiety carries positive charges which transfer from antibonding orbital of Be(2) to the bonding fragments significantly strengthen the Be-Be bonds that are corroborated by AIM, LOL and NBO analyses. In addition, mono beryllium products BeNCCH(3), CNBeCH(3), HBeCH(2)CN and HBeNCCH(2) have also been observed in our experiments.