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Issue 38, 2013
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Stepwise versus pseudo-concerted two-electron-transfer in a triarylamine–iridium dipyrrin–naphthalene diimide triad

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Abstract

A triad based on triarylamine donors, an iridium dipyrrin sensitiser and a naphthalene diimide acceptor is investigated using fs-pump–probe spectroscopy at two different pump wavelengths. Excitation of the naphthalene diimide induces a stepwise electron transfer process that yields within ca. 100 ps a charge separated state with 50–60% quantum yield in which one triarylamine is oxidised and the imide is reduced. Although being in the Marcus normal region, this state has a lifetime of 580 ns in MeCN. Excitation at the dipyrrin ligand centred absorption directly produces the charge separated state within ca. 1 ns however without formation of an intermediate. This pseudo-concerted two-electron transfer step was analysed with the help of a model dyad and a modified triad and is interpreted to be caused by inverted electron transfer rates. Although being much slower the latter process has a quantum yield of practically 100%.

Graphical abstract: Stepwise versus pseudo-concerted two-electron-transfer in a triarylamine–iridium dipyrrin–naphthalene diimide triad

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Publication details

The article was received on 10 May 2013, accepted on 30 Jul 2013 and first published on 20 Aug 2013


Article type: Paper
DOI: 10.1039/C3CP51981C
Phys. Chem. Chem. Phys., 2013,15, 16024-16030

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    Stepwise versus pseudo-concerted two-electron-transfer in a triarylamine–iridium dipyrrin–naphthalene diimide triad

    J. H. Klein, T. L. Sunderland, C. Kaufmann, M. Holzapfel, A. Schmiedel and C. Lambert, Phys. Chem. Chem. Phys., 2013, 15, 16024
    DOI: 10.1039/C3CP51981C

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