title: Vibronic transitions and quantum dynamics in molecular oligomers: a theoretical analysis with an application to aggregates of perylene bisimides.
abstract: Vibronic absorption spectra of molecular aggregates consisting of up to N = 9 monomer units are calculated employing methods of time-dependent quantum mechanics. Taking one vibrational degree of freedom for each monomer into account and treating one-exciton excited electronic states leads to a problem with N vibrations and N electronically coupled states. The demanding quantum propagation is carried out within the multiconfiguration time-depended Hartree method (MCTDH). Spectral features of and population transfer in the aggregates are analyzed as a function of the aggregate size and the strength of the electronic coupling. With a model for oligomers of perylene bisimides, it is shown how measured temperature-dependent absorption spectra correlate with the aggregate size. Furthermore, the exciton localization and dynamics in these aggregates are investigated.
authors.affiliation: Institut für Physikalische Chemie, Universität Würzburg Am Hubland, Germany.
authors.forename: J
authors.initials: J
authors.lastname: Seibt
authors.forename: T
authors.initials: T
authors.lastname: Winkler
authors.forename: K
authors.initials: K
authors.lastname: Renziehausen
authors.forename: V
authors.initials: V
authors.lastname: Dehm
authors.forename: F
authors.initials: F
authors.lastname: Würthner
authors.forename: H-D
authors.initials: HD
authors.lastname: Meyer
authors.forename: V
authors.initials: V
authors.lastname: Engel