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Singlet exciton fission via an intermolecular charge transfer state in coevaporated pentacene-perfluoropentacene thin films
Author(s) -
Vincent Kim,
Katharina Broch,
Valentina Belova,
Y. S. Chen,
Alexander Gerlach,
Frank Schreiber,
Hiroyuki Tamura,
Raffaele Guido Della Valle,
Gabriele D’Avino,
Ingo Salzmann,
David Beljonne,
Akshay Rao,
Richard H. Friend
Publication year - 2019
Publication title -
the journal of chemical physics
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.071
H-Index - 357
eISSN - 1089-7690
pISSN - 0021-9606
DOI - 10.1063/1.5130400
Subject(s) - singlet fission , pentacene , exciton , intermolecular force , singlet state , organic semiconductor , fission , ultrafast laser spectroscopy , biexciton , excitation , intramolecular force , materials science , spectroscopy , chemical physics , semiconductor , atomic physics , molecular physics , chemistry , condensed matter physics , excited state , physics , optoelectronics , nanotechnology , molecule , nuclear physics , quantum mechanics , stereochemistry , layer (electronics) , organic chemistry , neutron , thin film transistor
Singlet exciton fission is a spin-allowed process in organic semiconductors by which one absorbed photon generates two triplet excitons. Theory predicts that singlet fission is mediated by intermolecular charge-transfer states in solid-state materials with appropriate singlet-triplet energy spacing, but direct evidence for the involvement of such states in the process has not been provided yet. Here, we report on the observation of subpicosecond singlet fission in mixed films of pentacene and perfluoropentacene. By combining transient spectroscopy measurements to nonadiabatic quantum-dynamics simulations, we show that direct excitation in the charge-transfer absorption band of the mixed films leads to the formation of triplet excitons, unambiguously proving that they act as intermediate states in the fission process.

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