Design of novel nonlinear optical substances based on the controlling parameters of open-shell character, charge and spin states

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The strong correlation between experimental and theoretical diradical characters (y) is observed for several real molecular systems. As a novel class of open-shell third-order nonlinear optical (NLO) molecules, we investigate(1) polycyclic aromatic hydrocarbons including graphenes, and(2) transition-metal-metal compounds in order to clarify the relationship between open-shell character and molecular structures as well as the effects of external field, donor/acceptor substituents and spin states on the NLO properties. In(1), the relationship between the molecular architecture and open-shell character is clarified, and in(2) the effects of atom species and dσ-dσ contributions to NLO properties are revealed. In collaboration with experimentalists, we measured the two photon absorption cross sections of zethrenes and confirmed our theoretical prediction.