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The (2+1) resonance‐enhanced multiphoton ionization (REMPI) spectrum of Cl2 has been recorded between 76 000 and 90 000 cm−1. The origins of twenty Rydberg states are located, with the s series (4s−8s) generally exhibiting four Ω components and the d series (3d−5d) two components for each value of n. Vibronic coupling between the β(1g) ion‐pair state and the 3d and 4d (Ω=1) states is pronounced, necessitating the use of mass‐resolved REMPI for the analysis of these vibronically mixed states.

Mass-resolved multiphoton ionization spectroscopy of jet-cooled Cl2. II. The (2+1) REMPI spectrum between 76 000 and 90 000 cm−1