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Issue 27, 2010

Superexchange-mediated electronic energy transfer in a model dyad

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Abstract

On the basis of time-dependent density functional theory (TD-DFT) calculations coupled to the polarizable continuum model (PCM) and single molecule spectroscopic studies, we provide a detailed investigation of excitation energy transfer within a model bi-chromophoric system where a perylene monoimide (PMI) donor is bridged to a terrylene diimide (TDI) acceptor through a ladder-type pentaphenylene (pPh) spacer. We find that the electronic excitation on the PMI donor significantly extends over the bridge giving rise to a partial charge transfer character and inducing a ∼3-fold increase in the electronic interaction between the chromophores, which explains the failure of the Förster model in reproducing the observed energy migration rates when treating PMI as the donor. However, despite an increased charge transfer contribution in the effective donor state, the increase in solvent polarity is not accompanied by an enhancement in the electronic coupling between the subunits, which is rationalized from a detailed analysis of the excited-state wavefunctions.

Graphical abstract: Superexchange-mediated electronic energy transfer in a model dyad

Article information


Submitted
23 Feb 2010
Accepted
24 May 2010
First published
12 Jun 2010

Phys. Chem. Chem. Phys., 2010,12, 7378-7385
Article type
Paper

Superexchange-mediated electronic energy transfer in a model dyad

C. Curutchet, F. A. Feist, B. V. Averbeke, B. Mennucci, J. Jacob, K. Müllen, T. Basché and D. Beljonne, Phys. Chem. Chem. Phys., 2010, 12, 7378 DOI: 10.1039/C003496G

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