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Resonantly enhanced multiphoton ionization (REMPI) spectra of jet-cooled Xe2 are presented, covering the spectral region between ≊74 627 and 80 849 cm−1. Dimer ions produced by (2+1) REMPI excitation were mass selected in a linear time-of-flight (TOF) mass spectrometer. The vibrational and isotopic structure of several band systems dissociating to Xe* 5p56p and 5p55d asymptotes have been analyzed, many unambiguously for the first time, and molecular constants derived. Equilibrium bond lengths were estimated from Franck–Condon calculations. Insight into excited state predissociation was also obtained by recording atomic TOF excitation spectra.

(2+1) resonantly enhanced multiphoton ionization spectra of jet-cooled Kr2 between ≊91 800 and 94 100 cm−1 have been recorded. Single isotopomer excitation spectra were obtained using time-of-flight mass detection. Vibronic structure for several Rydberg ← ground state transitions involving excited gerade states which dissociate to Kr+Kr* (4p55p) have been unambiguously analyzed for the first time, and molecular constants derived. Bond lengths were estimated from Franck–Condon calculations. These results compare favorably with recent ab initio calculations. Excited state predissociation effects were inferred from excitation spectra obtained by monitoring atomic daughter fragment ions in TOF.

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