Abstract: Here, we have shown the reaction of [Cr(ArN(CH2)3NAr)2Cl2] (1) where (Ar = 2,6-Pri
2C6H3) and in presence of NaCp (2) (Cp= C5H5 = cyclopentadien), with a center
coordination η5 interaction between Cp as co-ligand and chromium
metal center, for optimization we used density functional theory
(DFT), under methods, explicitly including electrons correlations, for
the final calculations as MB3LYP (Becke) (Lee–Yang–Parr) level of
theory we used to obtain more exact results. This complex was
calculated as electronic energy for molecular system, because the
calculation accounting all electrons correlations interactions. The
optimised of [Cr(ArN(CH2)3NAr)2(η5-Cp)] (Ar = 2,6-Pri2C6H3 and Cp = C5H5) was found to be thermally stable. By using Dewar-Chatt-Duncanson model, as a basis of the molecular orbital (MO) analysis
and showed the highest occupied molecular orbital (HOMO) and
lowest occupied molecular orbital LUMO.