Time-resolved photoelectron imaging is demonstrated using the third harmonic of a 400-nm femtosecond laser pulse as the ionization source. The resulting 133-nm pulses are combined with 266-nm pulses to study the excited-state dynamics in the A/B- and F-band regions of SO2. The photoelectron signal from the molecules excited to the A/B-band does not decay for at least several picoseconds, reflecting the population of bound states. The temporal variation of the photoelectron angular distribution (PAD) reflects the creation of a rotational wave packet in the excited state. In contrast, the photoelectron signal from molecules excited to the F-band decays with a time constant of 80 fs. This time constant is attributed to the motion of the excited-state wave packet out of the ionization window. The observed time-dependent PADs are consistent with the F band corresponding to a Rydberg state of dominant s character. These results establish low-order harmonic generation as a promising tool for time-resolved photoelectron imaging of the excited-state dynamics of molecules, simultaneously giving access to low-lying electronic states, as well as Rydberg states, and avoiding the ionization of unexcited molecules.

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