Mechanism and molecular design of nonlinear optical properties originating in the flexibility of complex electronic systems

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We clarified the mechanism of generating nonlinear optical (NLO) phenomena of open-shell systems. The present study first elucidated a close connection between the magnetic interaction and third-order NLO properties, and then constructed novel control guidelines for NLO properties by tuning the diradical character and spin states. Several calculation methods for real open-shell molecules were proposed, and a new class of open-shell NLO molecules was designed. We also developed a quantum master equation approach based on the ab initio MO method, and succeeded in calculating dynamic NLO responses.