Issue 18, 2019

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

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

Supplementary files

Article information

Article type
Paper
Submitted
14 feb. 2019
Accepted
21 mar. 2019
First published
22 mar. 2019

Phys. Chem. Chem. Phys., 2019,21, 9013-9025

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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