Quantitative insights into charge-separated states from one- and two-pulse laser experiments relevant for artificial photosynthesis
- Publikationstyp:
- Zeitschriftenaufsatz
- Metadaten:
-
- Autoren
- Svenja Neumann
- Christoph Kerzig
- Oliver S Wenger
- Autoren-URL
- https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:000474412700020&DestLinkType=FullRecord&DestApp=WOS_CPL
- DOI
- 10.1039/c9sc01381d
- eISSN
- 2041-6539
- Externe Identifier
- Clarivate Analytics Document Solution ID: IH3SN
- PubMed Identifier: 31293747
- ISSN
- 2041-6520
- Ausgabe der Veröffentlichung
- 21
- Zeitschrift
- CHEMICAL SCIENCE
- Paginierung
- 5624 - 5633
- Datum der Veröffentlichung
- 2019
- Status
- Published
- Titel
- Quantitative insights into charge-separated states from one- and two-pulse laser experiments relevant for artificial photosynthesis
- Sub types
- Article
- Ausgabe der Zeitschrift
- 10
Datenquelle: Web of Science (Lite)
- Andere Metadatenquellen:
-
- Abstract
- <p>Quantitative laser flash photolysis experiments with several excitation wavelengths provided unprecedented insights into the charge-separated state photochemistry of molecular triads.</p>
- Autoren
- Svenja Neumann
- Christoph Kerzig
- Oliver S Wenger
- DOI
- 10.1039/c9sc01381d
- eISSN
- 2041-6539
- ISSN
- 2041-6520
- Ausgabe der Veröffentlichung
- 21
- Zeitschrift
- Chemical Science
- Sprache
- en
- Online publication date
- 2019
- Paginierung
- 5624 - 5633
- Status
- Published online
- Herausgeber
- Royal Society of Chemistry (RSC)
- Herausgeber URL
- http://dx.doi.org/10.1039/c9sc01381d
- Datum der Datenerfassung
- 2024
- Titel
- Quantitative insights into charge-separated states from one- and two-pulse laser experiments relevant for artificial photosynthesis
- Ausgabe der Zeitschrift
- 10
Datenquelle: Crossref
- 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.
- Addresses
- Department of Chemistry , University of Basel , St. Johanns-Ring 19 , 4056 Basel , Switzerland . Email: christoph.kerzig@unibas.ch ; Email: oliver.wenger@unibas.ch.
- Autoren
- Svenja Neumann
- Christoph Kerzig
- Oliver S Wenger
- DOI
- 10.1039/c9sc01381d
- eISSN
- 2041-6539
- Externe Identifier
- PubMed Identifier: 31293747
- PubMed Central ID: PMC6553010
- Funding acknowledgements
- Swiss Nanoscience Institute: P1406
- Swiss National Science Foundation: 200021_178760
- Swiss National Science Foundation: 178760
- Swiss National Science Foundation: 200021
- Open access
- true
- ISSN
- 2041-6520
- Ausgabe der Veröffentlichung
- 21
- Zeitschrift
- Chemical science
- Sprache
- eng
- Medium
- Electronic-eCollection
- Online publication date
- 2019
- Open access status
- Open Access
- Paginierung
- 5624 - 5633
- Datum der Veröffentlichung
- 2019
- Status
- Published
- Publisher licence
- CC BY-NC
- Datum der Datenerfassung
- 2019
- Titel
- Quantitative insights into charge-separated states from one- and two-pulse laser experiments relevant for artificial photosynthesis.
- Sub types
- research-article
- Journal Article
- Ausgabe der Zeitschrift
- 10
Files
https://pubs.rsc.org/en/content/articlepdf/2019/sc/c9sc01381d https://europepmc.org/articles/PMC6553010?pdf=render
Datenquelle: Europe PubMed Central
- 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.
- Date of acceptance
- 2019
- Autoren
- Svenja Neumann
- Christoph Kerzig
- Oliver S Wenger
- Autoren-URL
- https://www.ncbi.nlm.nih.gov/pubmed/31293747
- DOI
- 10.1039/c9sc01381d
- Externe Identifier
- PubMed Central ID: PMC6553010
- ISSN
- 2041-6520
- Ausgabe der Veröffentlichung
- 21
- Zeitschrift
- Chem Sci
- Sprache
- eng
- Country
- England
- Paginierung
- 5624 - 5633
- PII
- c9sc01381d
- Datum der Veröffentlichung
- 2019
- Status
- Published online
- Titel
- Quantitative insights into charge-separated states from one- and two-pulse laser experiments relevant for artificial photosynthesis.
- Sub types
- Journal Article
- Ausgabe der Zeitschrift
- 10
Datenquelle: PubMed
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