Laser-polarization effects on coherent vibronic excitation of molecules with quasi-degenerate electronic states.

摘要: The laser-polarization effects on nonadiabatically coupled π-electron rotation (ring current) and molecular vibration have been theoretically analyzed for aromatic molecules with quasi-degenerate excited states irradiated by an ultrashort laser pulse of arbitrary polarization. We first derived general formulations the coherent electronic wave packet expectation value angular momentum within a frozen-nuclei model. relative quantum phase superposed states, which determines oscillating behavior momentum, can be manipulated ellipticity orientation incident laser. Nuclear simulations model molecule confirmed controllability rotation, although is gradually reduced nonadiabatic couplings. amplitude depends prominently linear polarization vectors rather than helicity circular characteristic feature i...