Ultrafast dynamics and dissociative ionization of CS2 molecules studied via the femtosecond pump-probe method

The ultrafast dynamics and dissociative ionization of CS2 were studied using the pump-probe method with time-of-flight mass spectroscopy. The transient behavior of both parent ion (CS2 (+)) and fragment ions (S+ and CS+) was observed. It was found that all the ionic signals decay exponentially with lifetimes that were different for delay times, t > 0 and t < 0, which can be attributed to the evolution of different Rydberg states pumped by 267-nm and 400-nm laser pulses. The lifetimes of two Rydberg states were obtained simultaneously from one fitting of the transients. The fragment ions were produced by the dissociation of CS2 (+), and it is suggested that the final ionic state is the (CI)-I-2 (g) pound (+) state of CS2 (+) based on the measured S+/CS+ branching ratio. The S+/CS+ ratio is dependent on the delay time of the two lasers, indicating that the dissociation process of CS2 (+) is related to the evolution of the intermediate Rydberg state.