Exploring wavepacket dynamics behind strong-field momentum-dependent photodissociation in CH(2)BrI(+).
The ultrafast photodissociation dynamics of CH(2)BrI(+) into CH(2)Br(+) + I is studied using high level ab initio electronic structure calculations in conjunction with integration of the time-dependent Schrödinger equation and compared with measured pump-probe signals. These pump-probe measurements provide evidence for momentum-dependent dissociation, which is interpreted using two theoretical models. The first is based on DFT and TD-DFT calculations neglecting spin-orbit coupling, while the other, more rigorous model employs a larger number of coupled multi-configurational potentials obtained by means of CASSCF calculations. The latter model highlights the role of spin-orbit coupling between ionic electronic states as well as the effect of strong fields in the quantum dynamics including Stark-shifts and multi-photon excitation.
González-Vázquez
Jesús
J
Institut für Physikalische Chemie, Friedrich-Schiller Universität Jena, Helmholzweg 4, 07743 Jena, Germany.
González
Leticia
L
Nichols
Sarah R
SR
Weinacht
Thomas C
TC
Rozgonyi
Tamás
T