We have undertaken an extensive study of the spectroscopy and dynamics
of the S1-S0 transition in jet-cooled 1-methylindole and 1-methyl(d3)
indole. The energy-resolved fluorescence decays resulting from picosec
ond excitation of S1 vibrational modes display unusual quantum interfe
rence effects which have been attributed to the excitation of a large
number of quaside-generate states even at relatively low levels of vib
rational excitation. This has been attributed to rovibrational couplin
g in which the selection rules are much less restrictive than is norma
lly the case with rigid planar molecules. A significant rotational tem
perature dependence of the vibrational dynamics has been measured whic
h serves to corroborate this model.