The attosecond time-scale electronic dynamics induced by an ultrashort laser pulse is computed using a multi configuration time dependent approach in ABCU (C10H19N), a medium size polyatomic molecule with a rigid cage geometry. The coupling between the electronic states induced by the strong pulse is included in the many electron Hamiltonian used to compute the electron dynamics. We show that it is possible to implement control of the electron density stereodynamics in this medium size molecule by varying the characteristics of the laser pulse, for example by polarizing the electric field either along the N–C axis of the cage, or in the plane perpendicular to it. The excitation produces an oscillatory, non-stationary, electronic state that exhibits localization of the electron density in different parts of the molecule both during and after the pulse. The coherent oscillations of the non-stationary electronic state are also demonstrated through the alternation of the dipole moment of the molecule.
Phys. Chem. Chem. Phys.

Mignolet, B., Gijsbertsen, A., Vrakking, M. J. J., Levine, R. D., & Remacle, F. (2011). Stereocontrol of attosecond time-scale electron dynamics in ABCU using ultrafast laser pulses: a computational study. Phys. Chem. Chem. Phys., 13(18), 8331–8344. doi:10.1039/C1CP20094A