Control of the photodissociation of CsCl

A femtosecond UV laser pulse is used to resonantly excite CsCl molecules fr om the ionically bound ground state to the first excited repulsive state. T he excitation leads to the dissociation of CsCl. After a certain time delay a visible (VIS) femtosecond laser pulse interrupts the dissociation proces s by resonantly de-exciting the molecule back to the ground state. Accordin g to the Tannor-Rice control scheme, the fraction of dissociated CsCl molec ules is controlled by changing the delay time between the two fs laser puls es. The processes involved are investigated theoretically and experimentall y. Based on the results, a self-learning system has been realized, which is able to control the dissociation without any a priori knowledge of the mol ecule.