Coulomb interactions for mediator-enhanced sensitized triplet-triplet annihilation upconversion in solution
- Publikationstyp:
- Zeitschriftenaufsatz
- Metadaten:
-
- Autoren
- Felix Glaser
- Matthias Schmitz
- Christoph Kerzig
- Autoren-URL
- https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:001114472500001&DestLinkType=FullRecord&DestApp=WOS_CPL
- DOI
- 10.1039/d3nr05265f
- eISSN
- 2040-3372
- Externe Identifier
- Clarivate Analytics Document Solution ID: CL4U4
- PubMed Identifier: 38054748
- ISSN
- 2040-3364
- Ausgabe der Veröffentlichung
- 1
- Zeitschrift
- NANOSCALE
- Paginierung
- 123 - 137
- Datum der Veröffentlichung
- 2023
- Status
- Published
- Titel
- Coulomb interactions for mediator-enhanced sensitized triplet-triplet annihilation upconversion in solution
- Sub types
- Article
- Ausgabe der Zeitschrift
- 16
Datenquelle: Web of Science (Lite)
- Andere Metadatenquellen:
-
- Abstract
- <jats:p>An energy transfer cascade in a three-component upconversion system improves the emission quantum yield and reduces intrinsic filter effects. Investigations of molecular interactions are combined with lab-scale applications in photocatalysis.</jats:p>
- Autoren
- Felix Glaser
- Matthias Schmitz
- Christoph Kerzig
- DOI
- 10.1039/d3nr05265f
- eISSN
- 2040-3372
- ISSN
- 2040-3364
- Ausgabe der Veröffentlichung
- 1
- Zeitschrift
- Nanoscale
- Sprache
- en
- Online publication date
- 2024
- Paginierung
- 123 - 137
- Status
- Published online
- Herausgeber
- Royal Society of Chemistry (RSC)
- Herausgeber URL
- http://dx.doi.org/10.1039/d3nr05265f
- Datum der Datenerfassung
- 2024
- Titel
- Coulomb interactions for mediator-enhanced sensitized triplet–triplet annihilation upconversion in solution
- Ausgabe der Zeitschrift
- 16
Datenquelle: Crossref
- 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 <i>via</i> 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.
- Addresses
- Department of Chemistry, Johannes Gutenberg University Mainz, Duesbergweg 10-14, 55128 Mainz, Germany. ckerzig@uni-mainz.de.
- Autoren
- Felix Glaser
- Matthias Schmitz
- Christoph Kerzig
- DOI
- 10.1039/d3nr05265f
- eISSN
- 2040-3372
- Externe Identifier
- PubMed Identifier: 38054748
- Funding acknowledgements
- Johannes Gutenberg-Universität Mainz:
- Deutsche Forschungsgemeinschaft: KE 2313/7-1
- Open access
- false
- ISSN
- 2040-3364
- Ausgabe der Veröffentlichung
- 1
- Zeitschrift
- Nanoscale
- Sprache
- eng
- Medium
- Electronic
- Online publication date
- 2023
- Paginierung
- 123 - 137
- Datum der Veröffentlichung
- 2023
- Status
- Published
- Datum der Datenerfassung
- 2023
- Titel
- Coulomb interactions for mediator-enhanced sensitized triplet-triplet annihilation upconversion in solution.
- Sub types
- Journal Article
- Ausgabe der Zeitschrift
- 16
Datenquelle: Europe PubMed Central
- 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.
- Autoren
- Felix Glaser
- Matthias Schmitz
- Christoph Kerzig
- Autoren-URL
- https://www.ncbi.nlm.nih.gov/pubmed/38054748
- DOI
- 10.1039/d3nr05265f
- eISSN
- 2040-3372
- Ausgabe der Veröffentlichung
- 1
- Zeitschrift
- Nanoscale
- Sprache
- eng
- Country
- England
- Paginierung
- 123 - 137
- Datum der Veröffentlichung
- 2023
- Status
- Published online
- Titel
- Coulomb interactions for mediator-enhanced sensitized triplet-triplet annihilation upconversion in solution.
- Sub types
- Journal Article
- Ausgabe der Zeitschrift
- 16
Datenquelle: PubMed
- Beziehungen:
- Eigentum von