Electronic correlation and electron–molecular vibration coupling effects on non-linear optical properties of molecular dimer

Molecular dimer with two radical electrons is considered as a model system to study the effects of electronic correlation and electron–intramolecular vibration coupling on the non-linear optical properties. The static polarizability α and the static second hyperpolarizability γ are calculated and their dependencies on the model parameters are analyzed. The ion–radical compounds with large and unsymmetrical molecules are shown to have a potential for a high non-linearity.