Abstract
Rydberg excitations in the vacuum ultraviolet spectral range may open up molecular photoreaction pathways not accessible from lower-lying valence states. Here, single-shot UV/VUV pump-probe spectroscopy was used to study the photodissociation dynamics of iodomethane after 268 nm excitation in the A-band and excitation of the 6p (2 E3/2) Rydberg state at 161 nm. By combining weak-field VUV single-photon ionization with sub-10 fs temporal resolution and the superior statistical accuracy of the single-shot technique, sub-30 fs wave packet dynamics upon excitation in the A-band by a UV pump pulse were disclosed. Population transfer from the Rydberg state to the 2 1 A1 valence state leading to 100 fs dissociation dynamics was observed by utilizing the same methodology in a VUV-pump/UV-probe scheme.
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