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Issue 3, 2016
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Quantifying highly efficient incoherent energy transfer in perylene-based multichromophore arrays

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Abstract

Multichromophore perylene arrays were designed and synthesized to have extremely efficient resonance energy transfer. Using broadband ultrafast photoluminescence and transient absorption spectroscopies, transfer timescales of approximately 1 picosecond were resolved, corresponding to efficiencies of up to 99.98%. The broadband measurements also revealed spectra corresponding to incoherent transfer between localized states. Polarization resolved spectroscopy was used to measure the dipolar angles between donor and acceptor chromophores, thereby enabling geometric factors to be fixed when assessing the validity of Förster theory in this regime. Förster theory was found to predict the correct magnitude of transfer rates, with measured ∼2-fold deviations consistent with the breakdown of the point-dipole approximation at close approach. The materials presented, along with the novel methods for quantifying ultrahigh energy transfer efficiencies, will be valuable for applications demanding extremely efficient energy transfer, including fluorescent solar concentrators, optical gain, and photonic logic devices.

Graphical abstract: Quantifying highly efficient incoherent energy transfer in perylene-based multichromophore arrays

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Supplementary files

Article information


Submitted
13 Nov 2015
Accepted
04 Dec 2015
First published
10 Dec 2015

Phys. Chem. Chem. Phys., 2016,18, 1712-1719
Article type
Paper
Author version available

Quantifying highly efficient incoherent energy transfer in perylene-based multichromophore arrays

J. E. A. Webb, K. Chen, S. K. K. Prasad, J. P. Wojciechowski, A. Falber, P. Thordarson and J. M. Hodgkiss, Phys. Chem. Chem. Phys., 2016, 18, 1712
DOI: 10.1039/C5CP06953J

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