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Oligomers of the organic semiconductor PTCDA are studied by means of heliumnanodroplet isolation (HENDI) spectroscopy. In contrast to the monomerabsorption spectrum, which exhibits clearly separated, very sharp absorptionlines, it is found that the oligomer spectrum consists of three main peakshaving an apparent width orders of magnitude larger than the width of themonomer lines. Using a simple theoretical model for the oligomer, in which aFrenkel exciton couples to internal vibrational modes of the monomers, theseexperimental findings are nicely reproduced. The three peaks present in theoligomer spectrum can already be obtained taking only one effective vibrationalmode of the PTCDA molecule into account. The inclusion of more vibrationalmodes leads to quasi continuous spectra, resembling the broad oligomer spectra.

Vibronic Lineshapes of PTCDA Oligomers in Helium Nanodroplets