Control theory of nonadiabatic electron dynamics of aromatic molecules induced by ultrashort laser pulses

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The control theory of nonadiabatically coupled pi-electron rotation (ring current) and molecular vibration in aromatic molecules irradiated by ultrashort laser pulses has been established. Theoretical and numerical analyses have revealed that it is possible to manipulate the interference between nuclear wave packets created on excited-state potential energy surfaces by a laser pulse of arbitrary polarization. In principle, the angular momentum (magnetic field) of pi electrons circulating along an aromatic ring and the amplitude of molecular vibration can be controlled as desired by means of ultrashort laser pulses. In addition, the frequency spectrum of photo-excited aromatic molecules depends significantly on laser polarization. This finding serves as a basis for rapid identification of molecular chirality.