ArticleChemical science2019
Quantitative insights into charge-separated states from one- and two-pulse laser experiments relevant for artificial photosynthesis.
Article in Chemical science, 2019. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 15 papers.
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Who cites it
15 citing papers in PubMed, 27 citations in OpenAlex.
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- Cage escape governs photoredox reaction rates and quantum yields.Nature chemistry · 2024Article
- Better Covalent Connection in a Molecular Triad Enables More Efficient Photochemical Energy Storage.Inorganic chemistry · 2023Article
- Unravelling Dynamics Involving Multiple Charge Carriers in Semiconductor Nanocrystals.Nanomaterials (Basel, Switzerland) · 2023Review
- Selective population of triplet excited states in heavy-atom-free BODIPY-CPhotochemical & photobiological sciences : Official journal of the European Photochemistry Association and the European Society for Photobiology · 2022Article
- Shedding Light on the Oxidizing Properties of Spin-Flip Excited States in a CrJournal of the American Chemical Society · 2022Article
- Red Light-Based Dual Photoredox Strategy Resembling the Z-Scheme of Natural Photosynthesis.JACS Au · 2022Article
- Cobalt(III) Carbene Complex with an Electronic Excited-State Structure Similar to Cyclometalated Iridium(III) Compounds.Journal of the American Chemical Society · 2022Article
- Recent Advances and Perspectives in Photodriven Charge Accumulation in Molecular Compounds: A Mini Review.Energy & fuels : an American Chemical Society journal · 2021Review
- Controlling Spin-Correlated Radical Pairs with Donor-Acceptor Dyads: A New Concept to Generate Reduced Metal Complexes for More Efficient Photocatalysis.Chemistry (Weinheim an der Bergstrasse, Germany) · 2021Article
- Yield-not only Lifetime-of the Photoinduced Charge-Separated State in Iridium Complex-Polyoxometalate Dyads Impact Their Hydrogen Evolution Reactivity.Chemistry (Weinheim an der Bergstrasse, Germany) · 2020Article
- Reactivity control of a photocatalytic system by changing the light intensity.Chemical science · 2019Article
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Authors and funding
3 authors at 1 institution in 1 country.
Funding
No grant is acknowledged in the PubMed record.
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.
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