Quantum chemical investigations of the electronic structure of the design carbazole (Cz) containing supermolecules, supramolecules, single charge donor and acceptor molecules were performed in the framework of the semiempirical neglect of differential overlap (MNDO) method. The data obtained show that it is a small charge redistribution in Cz-(CH2)4-1,2,4,5-tetracyanobenzene (TCNB) and Cz::TCNB. These designed derivatives are potential molecular photo-diodes. The sequence of the stability of the Cz containing supramolecules is found. The modeling of the photoinduced charge separation in Cz, TCNB, 2,4,7-trinitro-9-diciano-fluorene (TN9(CN)2F) and 2,4,5,7-tetranitro-9-diciano-fluorene (TeN9(CN)2F) molecules was done.