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Issue 21, 2019
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Quantitative insights into charge-separated states from one- and two-pulse laser experiments relevant for artificial photosynthesis

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Abstract

Charge-separated states (CSSs) are key intermediates in photosynthesis and solar energy conversion. However, the factors governing the formation efficiencies of CSSs are still poorly understood, and light-induced electron–hole recombinations as deactivation pathways competing with desired charge accumulations are largely unexplored. This greatly limits the possibility to perform efficient multi-electron transfer, which is essential for artificial photosynthesis. We present a systematic investigation of two donor–sensitizer–acceptor triads (with different donor–acceptor distances) capable of storing as much as 2.0 eV in their CSSs upon the absorption of a visible photon. Using quantitative one- and two-pulse laser flash photolysis, we provide deep insights into both the CSS formation quantum yield, which can reach up to 80%, and the fate of the CSS upon further (secondary) excitation with green photons. The triad with shorter intramolecular distances shows a remarkable excitation wavelength dependence of the CSS formation quantum yield, and the CSS of this triad undergoes more efficient light-induced charge recombination than the longer equivalent by about one order of magnitude, whilst thermal charge recombination shows the exact opposite behavior. The unexpected results of our detailed photophysical study can be rationalized by detrimental singlet charge transfer states or structural considerations, and could significantly contribute to the future design of CSS precursors for accumulative multi-electron transfer and artificial photosynthesis.

Graphical abstract: Quantitative insights into charge-separated states from one- and two-pulse laser experiments relevant for artificial photosynthesis

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Supplementary files

Article information


Submitted
20 Mar 2019
Accepted
01 May 2019
First published
09 May 2019

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2019,10, 5624-5633
Article type
Edge Article

Quantitative insights into charge-separated states from one- and two-pulse laser experiments relevant for artificial photosynthesis

S. Neumann, C. Kerzig and O. S. Wenger, Chem. Sci., 2019, 10, 5624
DOI: 10.1039/C9SC01381D

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material and it is not used for commercial purposes.

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    [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
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    [Original citation] - Published by The Royal Society of Chemistry.

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