Abstract
The dynamic evolution of CS2 4d and 6s Rydberg wave packet components has been experimentally visualized via femtosecond time-resolved photoelectron imaging coupled with time-resolved mass spectroscopy. The temporal evolution of the four components of the prepared Rydberg wave packet is directly observed as time-dependent changes of the intensities of different parts in the main photoelectron peak. Furthermore, time-resolved photoelectron angular distributions (PADs) clearly reflect the different component characters of 4d and 6s molecular orbitals. The lifetime of Rydberg wave packets is determined to be about 830fs and their decay is attributed to predissociation. Our results suggest the possibility of directly visualizing and determining the amplitudes and relative phases of different electronic and vibrational wave packet components in polyatomic molecules.
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