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          Institute: MPI für Polymerforschung     Collection: MPI Polymerforschung     Display Documents

ID: 28333.0, MPI für Polymerforschung / MPI Polymerforschung
Interchain vs. intrachain energy transfer in acceptor-capped conjugated polymers
Authors:Beljonne, D.; Pourtois, G.; Silva, C.; Hennebicq, E.; Herz, L. M.; Friend, R. H.; Scholes, G. D.; Setayesh, S.; Müllen, Klaus; Bredas, J. L.
Date of Publication (YYYY-MM-DD):2002-08-20
Title of Journal:Proceedings of the National Academy of Sciences of the United States of America
Journal Abbrev.:Proc. Natl. Acad. Sci. U. S. A.
Issue / Number:17
Start Page:10982
End Page:10987
Review Status:No review
Audience:Not Specified
Abstract / Description:The energy-transfer processes taking place in conjugated polymers are investigated by means of ultrafast spectroscopy and correlated quantum-chemical calculations applied to polyindenofluorenes end-capped with a perylene derivative. Comparison between the time-integrated luminescence and transient absorption spectra measured in solution and in films allows disentangling of the contributions arising from intrachain and from interchain energy-migration phenomena. Intrachain processes dominate in solution where photoexcitation of the polyindenofluorene units induces a rather slow energy transfer to the perylene end moieties. In films, close contacts between chains favors interchain transport of the excited singlet species (from the conjugated bridge of one chain to the perylene unit of a neighboring one); this process is characterized by a 1-order-of-magnitude increase in transfer rate with respect to solution. This description is supported fully by the results of quantum-chemical calculations that go beyond the usual point-dipole model approximation and account for geometric relaxation phenomena in the excited state before energy migration. The calculations indicate a two-step mechanism for intrachain energy transfer with hopping along the conjugated chains as the rate-limiting step; the higher efficiency of the interchain transfer process is mainly due to larger electronic coupling matrix elements between closely lying chains.
Comment of the Author/Creator:Date: 2002, AUG 20
External Publication Status:published
Document Type:Article
Affiliations:MPI für Polymerforschung
External Affiliations:Univ Arizona, Dept Chem, POB 210041, Tucson, AZ 85721 USA; Univ Mons, B-7000 Mons, Belgium; Univ Cambridge, Cavendish Lab, Cambridge CB3 0HE, England; Univ Toronto, Lash Miller Chem Labs, Toronto, ON M5S 3H6, Canada
Identifiers:ISI:000177606900009 [ID No:1]
ISSN:0027-8424 [ID No:2]
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