Influence of nuclear motion on ultrafast electronic dynamics
Irradiation of a molecular system by ultrashort laser pulses very often populates several cationic states launching pure electron dynamics that appear as ultrafast migration of the electronic charge throughout the system. A crucial question in the emerging field of attochemistry is whether these pure electronic coherences last long enough to allow for their efficient observation and eventual manipulation with ultrashort laser pulses.
My researches on this subject are directed on exploring how the nuclear motion affects the ultrafast dynamics of electrons in a molecule. In particular, I develop fully quantum as well as semiclassical methodologies which allow to calculate concerted motion of electrons and nuclei in experimentally interesting systems.
Recently, we demonstrated by fully ab initio simulation that ultrafast oscillations of a positive charge created after ionization of a molecule can last long enough to be observed and controlled. More details can be found in the following paper.
- V. Despré, N. V. Golubev, and A. I. Kuleff
Charge Migration in Propiolic Acid: A Full Quantum Dynamical Study
Phys. Rev. Lett. 121, 203002 (2018)