Nonadiabatic response model of laser-induced ultrafast pi-electron rotations in chiral aromatic molecules.

We theoretically investigated the nonadiabatic couplings between optically induced pi-electron rotations and molecular vibrations in a chiral aromatic molecule irradiated by a nonhelical, linearly polarized laser pulse. The results of wave packet dynamics simulation show that the vibrational amplitudes strongly depend on the initial rotation direction, clockwise or counterclockwise, which is controlled by the polarization direction of the incident pulse. This suggests that attosecond pi-electron rotations can be observed by spectroscopic detection of femtosecond molecular vibrations.