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We report on quantum dynamical studies of ultrafast photo-induced energy and charge transfer in organic semiconductor materials, complementing time-resolved spectroscopic observations that underscore the coherent nature of the ultrafast elementary transfer events in these molecular aggregate systems. Our approach combines first-principles parametrized Hamiltonians with accurate quantum dynamics simulations using multiconfigurational methods, along with semiclassical approaches. This paper focuses on the elementary mechanism of coherent exciton migration and creation of charge-transfer excitons in polythiophene type materials, representative of the poly(3-hexylthiophene) (P3HT) polymer. Special emphasis is placed on the interplay of trapping due to high-frequency phonon modes, and thermal activation due to low-frequency ”soft” modes which drive a diffusive dynamics.
Robert Binder,Wjatscheslaw Popp,Dominik Brey, andIrene Burghardt
"Coherent carrier and exciton transport in organic semiconductors", Proc. SPIE 11345, Nanophotonics VIII, 113451M (13 April 2020); https://doi.org/10.1117/12.2556073
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Robert Binder, Wjatscheslaw Popp, Dominik Brey, Irene Burghardt, "Coherent carrier and exciton transport in organic semiconductors," Proc. SPIE 11345, Nanophotonics VIII, 113451M (13 April 2020); https://doi.org/10.1117/12.2556073