The vibrationally resolved excitation functions for Cl− formation from jet-cooled HCl and DCl, following photoabsorption in the region 75–86 nm (HCl/DCl+hν→H+/D++Cl−), are reported and compared with ab initio calculations. This completes our understanding of the various possible decay channels available to superexcited states of HCl and DCl that lie above the first ionization limit. Our experimental and theoretical results suggest that the Rydberg states responsible for ion-pair formation in HCl and DCl via predissociation by the V 1Σ+ ion-pair state correspond to 1Σ+ states that are only weakly autoionized. These same Rydberg states appear to act as, at least, one class of precursor states for neutral dissociation to yield excited H* and Cl* atoms.
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