Manipulating electronic couplings and nonadiabatic nuclear dynamicswith strong laser pulses

摘要

We demonstrate the possibility of manipulating the coupling between two (optically bright andoptically dark) excited electronic states and of controlling the ensuing nuclear wave packetdynamics via a strong laser pulse, which couples the ground and the bright electronic state. Thecontrol of the wave packet dynamics is implemented through the creation of a highlynonequilibrium distribution in the bright-dark vibronic manifold. The distribution is produced dueto the combined effect of the external pulse (through Rabi cycling) and the system itself (through theelectronic interstate coupling). The induced wave packet dynamics persists long after the pulse isover, both in the isolated and in the dissipative system. The effects are robust and are achieved byvarying the strength and duration of a Gaussian pulse, that is, no careful tuning of the pulse shapeis required. Possible applications of our results include the strong-pulse control of electron transferas well as the enhancement and detection of intramolecular electronic coupling via strong-pulsespectroscopy.