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Photoinduced electron transfer in a molecular dyad by nanosecond pump-pump-probe spectroscopy

Abstract

The design of robust inexpensive molecular photocatalysts for conversion of abundant stable molecules like H2O and CO2 into an energetic carrier is one of major fundamental questions for scientists nowadays. The outstanding challenge is to couple single photoinduced charge separation events with the sequential accumulation of redox equivalents at catalytic unit for performing multielectronic catalytic reactions. Herein, a double excitation by nanosecond pump-pump-probe experiment was used to interrogate the photoinduced charge transfer and charge accumulation on a molecular dyad composed of a porphyrin chromophore and a ruthenium-based catalyst in the presence of a reversible electron acceptor. Accumulative charge transfer state is unattainable because of rapid reverse electron transfer to the photosensitizer upon the second excitation and the low driving force of the forward photodriven electron transfer reaction. Such method allows the fundamental understanding of the relaxation mechanism after two sequential photon absorption, deciphering the undesired electron transfer reactions that limit the charge accumulation efficiency. This study is a step toward the improvement of synthetic strategies of molecular photocatalysts for light-induced charge accumulation and more generally, for solar energy conversion.

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Publication details

The article was received on 30 Jan 2018, accepted on 12 May 2018 and first published on 14 May 2018


Article type: Paper
DOI: 10.1039/C8PP00048D
Citation: Photochem. Photobiol. Sci., 2018, Accepted Manuscript
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    Photoinduced electron transfer in a molecular dyad by nanosecond pump-pump-probe spectroscopy

    M. Ha-Thi, V. Pham, T. Pino, M. Valeriia, A. Quaranta, C. Lefumeux, W. Leibl and A. Aukauloo, Photochem. Photobiol. Sci., 2018, Accepted Manuscript , DOI: 10.1039/C8PP00048D

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