Hole-transfer induced energy transfer in perylene diimide dyads with a donor-spacer-acceptor motif

Physical Chemistry Chemical Physics : PCCP
Patrick KölleEberhard Riedle

Abstract

We investigate the photoinduced dynamics of perylene diimide dyads based on a donor-spacer-acceptor motif with polyyne spacers of varying length by pump-probe spectroscopy, time resolved fluorescence, chemical variation and quantum chemistry. While the dyads with pyridine based polyyne spacers undergo energy transfer with near-unity quantum efficiency, in the dyads with phenyl based polyyne spacers the energy transfer efficiency drops below 50%. This suggests the presence of a competing electron transfer process from the spacer to the energy donor as the excitation sink. Transient absorption spectra, however, reveal that the spacer actually mediates the energy transfer dynamics. The ground state bleach features of the polyyne spacers appear due to the electron transfer decay with the same time constant present in the rise of the ground state bleach and stimulated emission of the perylene energy acceptor. Although the electron transfer process initially quenches the fluorescence of the donor it does not inhibit energy transfer to the perylene energy acceptor. The transient signatures reveal that electron and energy transfer processes are sequential and indicate that the donor-spacer electron transfer state itself is responsible ...Continue Reading

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Citations

May 19, 2017·Physical Chemistry Chemical Physics : PCCP·Francesco NastasiMaurizio Prato
Nov 30, 2018·Physical Chemistry Chemical Physics : PCCP·Romain LetrunEric Vauthey
Aug 27, 2018·Journal of Fluorescence·Hoa T HoangMichael U Kumke
Jun 25, 2021·Chemical Science·Raphael LauensteinCorinna R Hess

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