We analyzed the molecular orbitals for a Al4Cl4(NH3)(4) compound, which is a model of the (AlBr.NEt3)(4) crystal structure recently reported by Schnockel and co-workers. We found that even though Al4Cl4(NH3)(4) contains a planar square Al-4 cluster it is not an aromatic compound. However, the addition of two sodium atoms to Al4Cl4(NH3)(4) yields a new Na2Al4Cl4(NH3)(4) compound which is a pi-aromatic molecule. We hope that prediction of this new compound will facilitate a synthesis of aluminum aromatic solids.