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Issue 18, 2019
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Dynamic exciton localisation in a pyrene–BODIPY–pyrene dye conjugate

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Abstract

The photophysics of a molecular triad consisting of a BODIPY dye and two pyrene chromophores attached in 2-position are investigated by steady state and fs-time resolved transient absorption spectroscopy as well as by field induced surface hopping (FISH) simulations. While the steady state measurements indicate moderate chromophore interactions within the triad, the time resolved measurements show upon pyrene excitation a delocalised excited state which localises onto the BODIPY chromophore with a time constant of 0.12 ps. This could either be interpreted as an internal conversion process within the excitonically coupled chromophores or as an energy transfer from the pyrenes to the BODIPY dye. The analysis of FISH-trajectories reveals an oscillatory behaviour where the excitation hops between the pyrene units and the BODIPY dye several times until finally they become localised on the BODIPY chromophore within 100 fs. This is accompanied by an ultrafast nonradiative relaxation within the excitonic manifold mediated by the nonadiabatic coupling. Averaging over an ensemble of trajectories allowed us to simulate the electronic state population dynamics and determine the time constants for the nonradiative transitions that mediate the ultrafast energy transfer and exciton localisation on BODIPY.

Graphical abstract: Dynamic exciton localisation in a pyrene–BODIPY–pyrene dye conjugate

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Publication details

The article was received on 14 Feb 2019, accepted on 21 Mar 2019 and first published on 22 Mar 2019


Article type: Paper
DOI: 10.1039/C9CP00908F
Phys. Chem. Chem. Phys., 2019,21, 9013-9025

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    Dynamic exciton localisation in a pyrene–BODIPY–pyrene dye conjugate

    N. Auerhammer, A. Schulz, A. Schmiedel, M. Holzapfel, J. Hoche, M. I. S. Röhr, R. Mitric and C. Lambert, Phys. Chem. Chem. Phys., 2019, 21, 9013
    DOI: 10.1039/C9CP00908F

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