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http://doi.org/10.25358/openscience-9722
Autoren: | Glaser, Felix Schmitz, Matthias Kerzig, Christoph |
Titel: | Raw data for "Coulomb interactions for mediator-enhanced sensitized triplet-triplet annihilation upconversion in solution" |
Online-Publikationsdatum: | 1-Dez-2023 |
Erscheinungsdatum: | 2023 |
Sprache des Dokuments: | Englisch |
Zusammenfassung/Abstract: | Sensitized triplet-triplet annihilation upconversion offers an attractive possibility to replace a high-energy photon by two photons with lower energy through the combination of a light-harvesting triplet sensitizer and an annihilator for the formation of a fluorescent singlet state. Typically, high annihilator concentrations are required to achieve an efficient initial energy transfer and as a direct consequence the most highly energetic emission is often not detectable due to intrinsic reabsorption by the annihilator itself. Herein, we demonstrate that the addition of a charge-adapted mediator drastically improves the energy transfer efficiency at low annihilator concentrations via an energy transfer cascade. Inspired by molecular dyads and recent developments in nanocrystal-sensitized upconversion, our system exploits a concept to minimize intrinsic filter effects, while boosting the upconversion quantum yield in solution. A sensitizer-annihilator combination consisting of a ruthenium-based complex and 9,10-diphenylanthracene (DPA) is explored as model system and a sulfonated pyrene serves as mediator. The impact of opposite charges between sensitizer and mediator – to induce Coulombic attraction and subsequently result in accelerated energy transfer rate constants – is analyzed in detail by different spectroscopic methods. Ion pairing and the resulting static energy transfer in both directions is a minor process, resulting in an improved overall performance. Finally, the more intense upconverted emission in the presence of the mediator is used to drive two catalytic photoreactions in a two-chamber setup, illustrating the advantages of our approach, in particular for photoreactions requiring oxygen that would interfere with the upconversion system. |
DDC-Sachgruppe: | 540 Chemie 540 Chemistry and allied sciences |
Veröffentlichende Institution: | Johannes Gutenberg-Universität Mainz |
Organisationseinheit: | FB 09 Chemie, Pharmazie u. Geowissensch. |
Veröffentlichungsort: | Mainz |
ROR: | https://ror.org/023b0x485 |
DOI: | http://doi.org/10.25358/openscience-9722 |
URN: | urn:nbn:de:hebis:77-openscience-8fd3ff4a-9fe9-4657-ac77-3cae1551c6808 |
Version: | Original work |
Publikationstyp: | Datensammlung |
Nutzungsrechte: | CC BY |
Informationen zu den Nutzungsrechten: | https://creativecommons.org/licenses/by/4.0/ |
Beziehungen: | is source of 10.1039/D3NR05265F |
Enthalten in den Sammlungen: | JGU-Forschungsdaten |
Dateien zu dieser Ressource:
Datei | Beschreibung | Größe | Format | ||
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coulomb_interactions_for_medi-20231129184324929.zip | Raw data for figures in the main manuscript | 3.3 MB | ZIP | Öffnen/Anzeigen |