Dipole switching in large molecules described by explicitly time-dependent configuration interaction.
In this paper, we report laser-driven charge transfer simulations for Li-(Ph)(n)-CN (n=1,2,3) using the time-dependent configuration interaction single approach. These molecules serve as systematically extendable model systems, in order to investigate the selectivity, and thus controllability, of an ultrashort laser-induced electronic excitation as a function of the molecular size. For example, such control would be needed if a small electronic molecular switch is connected to a larger molecular device. We demonstrate that for larger molecules, the selectivity of the electronic transition is considerably reduced even for rather long pulses due to dynamic polarizations of the molecules. We also show that these dynamic polarizations might be substantially underestimated in few state models.
Institut für Chemie, Theoretische Chemie, Universität Potsdam, Germany.
Pascal
P
Krause
Tillmann
T
Klamroth