New evidence has been found for the participation of the 1La state in the excited-state dynamics of jet-cooled 2,3-dialkylindoles. Excited-state-lifetime measurements of 2,3-dimethylindole, 1,2,3,4-tetrahydrocarbazole, and their deuterated analogues afford a clear view of the 1La-1Lb state coupling in these systems. Polar clusters of 2,3-dimethylindole are shown to exhibit fluorescence that can be attributed to a bound 1La state. The present observations made on clusters have direct parallels to phenomena observed in condensed-phase work and are discussed in terms of a model that unifies the disparate pictures of the excited states of indoles derived from condensed-phase data and previous jet-cooled experiments. © 1990 American Chemical Society.