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A hybrid molecular sensitizer for triplet fusion upconversion
School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150090, China.
School of Astronautics, Harbin Institute of Technology, Harbin 150001, China.
Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. University of Helsinki, Department of Chemistry, P.O. Box 55 (A.I. Virtanens Plats 1), IN-00014 University of Helsinki, Finland.ORCID iD: 0000-0002-0716-3385
University of Helsinki, Department of Chemistry, P.O. Box 55 (A.I. Virtanens Plats 1), IN-00014 University of Helsinki, Finland; Tomsk State University, 36 Lenin Avenue, Tomsk, Russia.
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2021 (English)In: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 426, article id 131282Article in journal (Refereed) Published
Abstract [en]

Triplet fusion upconversion is useful for a broad spectrum of applications ranging from solar cells, photoredox catalysis, to biophotonics applications, especially in the near-infrared (NIR, >700 nm) range. This upconverting system typically demands efficient conversion of spin-singlet harvested energy through intersystem crossing to spin-triplet states, accessible only in rare metallic-coordinating macrocycle compounds or heavy-metal-containing semiconductor quantum dots for triplet sensitization. Herein, we describe an organic–inorganic system for NIR-to-visible triplet fusion upconversion, interfacing commonly-seen, non-metallic, infrared dyes (IR806, IR780, indyocynine green, and CarCl) and lanthanide nanocrystal (sodium ytterbium fluoride) as a hybrid molecular sensitizer, which extracts molecular spin-singlet energy to nanocrystal-enriched ytterbium dopants at 48% efficiency (IR806, photoexciation at 808 nm). Moreover, ytterbium sub-lattice energy migration increases the interaction possibility between the nanocrystal and the freely-diffusing rubrenes in solution, resulting in 24-fold (IR806) to 1740-fold (indocyanine green) upconversion (600 nm) increase, depending on the IR dye type, as compared to the one without ytterbium nanotransducers. Ab initio quantum chemistry calculations identify enhanced spin-orbital coupling in the ytterbium-IR806 complex and high energy transfer rate in the ytterbium-rubrene interaction (1010 s−1). Employing inorganic lanthanide nanocrystals as nanotransducers unleashes the potential use of non-metallic infrared organic dyes for triplet fusion upconversion.

Place, publisher, year, edition, pages
Elsevier, 2021. Vol. 426, article id 131282
Keywords [en]
Triplet fusion upconversion, Lanthanide, Nanocrystals, NIR dyes
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-178599DOI: 10.1016/j.cej.2021.131282ISI: 000724579200003Scopus ID: 2-s2.0-85110734023OAI: oai:DiVA.org:liu-178599DiVA, id: diva2:1587206
Note

Funding: National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [51972084, 51672061]; State Key Laboratory of Urban Water Resource and Environment (Harbin Institute of Technology)Harbin Institute of Technology [2020DX10]; Fundamental Research Funds for the Central Universities, ChinaFundamental Research Funds for the Central Universities [AUGA5710052614]; Swedish Research CouncilSwedish Research CouncilEuropean Commission [2020-04600, 2018-05973, SNIC 2020-3-29]; Academy of FinlandAcademy of FinlandEuropean Commission [1325369, 1315600]; Russian Science FoundationRussian Science Foundation (RSF) [17-73-20012]

Available from: 2021-08-24 Created: 2021-08-24 Last updated: 2026-03-06Bibliographically approved

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