Transient Nonadiabatic Charge Redistribution in Molecules and its Effects on Nuclear Frame

Transient nonadiabatic charge redistribution (TNCR) in a molecule or molecular ion is caused by the strong oscillating electric field of a linearly polarized femtosecond laser pulse and can be maintained throughout a major part of the pulse duration. It directly affects the motion of light components of the nuclear frame (protons) during the pulse and it is imprinted in the evolution of nuclear degrees of freedom after the pulse, most notably, in the impulsive alignment in the molecular ensemble. Prolong charge localization and sequential ionization in polyatomic molecules affects the ensuing fragmentation pattern and charge distribution among the fragments. Our model calculations of the relative yield of ionized fragments and the kinetic energy distributions of the released protons agree quantitatively with the experimental data.The TNCR-mediated interaction of the laser field with molecular rotational degree of freedom results in a characteristic composition of the rotational wavepacket that is formed by this impulseve torque and that determines the subsequent molecular alignment dynamics.TNCR and its consequences are critically influenced by many-body effects. We investigate the interplay of the charge localization and inter-electronic repulsion and the resulting modifications of the angular dependence patterns in the cumulative impulsive torque.