Exciton dispersion in para-quaterphenyl: Significant molecular interactions beyond Coulomb coupling
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Contributors
Abstract
We have experimentally determined the momentum dependence of the electronic excitation spectra of para-quaterphenyl single crystals. The parallel arrangement of para-quaterphenyl molecules results in a strong Coulomb coupling of the molecular excitons. Such crystals have been considered to be a very good realization of the Frenkel exciton model, including the formation of H-type aggregates. Our data reveal an unexpected exciton dispersion of the upper Davydov component, which cannot be rationalized in terms of inter-molecular Coulomb coupling of the excitons. A significant reduction of the nearest neighbor coupling due to additional charge-transfer processes is able to provide an explanation of the data. Furthermore, the spectral onset of the excitation spectrum, which represents a heavy exciton resulting from exciton-phonon coupling, also shows a clear dispersion, which had been unknown so far. Finally, an optically forbidden excitation about 1 eV above the excitation onset is observed.
Details
Original language | English |
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Article number | 095313 |
Journal | AIP advances |
Volume | 11 |
Issue number | 9 |
Publication status | Published - 1 Sept 2021 |
Peer-reviewed | Yes |