Anthracene Diphosphate Ligands for CdSe Quantum Dots; Molecular Design for Efficient Upconversion

De Roo, Jonathan and Huang, Zhiyuan and Schuster, Nathaniel J. and Hamachi, Leslie S. and Congreve, Daniel N. and Xu, Zihao and Xia, Pan and Fishman, Dmitry A. and Lian, Tianquan and Owen, Jonathan S. and Tang, Ming Lee. (2020) Anthracene Diphosphate Ligands for CdSe Quantum Dots; Molecular Design for Efficient Upconversion. Chemistry of Materials, 32 (4). pp. 1461-1466.

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Official URL: https://edoc.unibas.ch/75759/

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Quantum dot (QD)-sensitized photon upconversion follows a multi-step energy transfer process from the QD to transmitter ligand to a soluble annihilator. Using a novel 10-R-anthracene-1,8-diphosphoric acid (R = octyl, 2-hexyldecyl, phenyl) ligand with high binding affinity for CdSe QD surfaces, we demonstrate a photon upconversion process that is limited by the transmitter to annihilator transfer efficiency. Using 1H NMR spectroscopy, we demonstrate that these bidentate diphosphate ligands rapidly and irreversibly displace two carboxylate ligands. These ligands mediate energy transfer from the photoexcited QDs to a triplet annihilator (1,10-diphenylanthracene), producing overall photon upconversion quantum efficiencies as high as 17%, the highest for QDs with no shells. Transient absorption spectroscopy shows that the anthracene dihydrogen phosphate (ADP) ligand supports a 3.4 fold longer triplet state lifetime compared to 9-anthracene carboxylic acid (299.9 ± 9.5 vs 88.2 ± 2.1 μs), increasing the probability of energy transfer.
Faculties and Departments:05 Faculty of Science > Departement Chemie > Chemie > Nanomaterials (De Roo)
UniBasel Contributors:De Roo, Jonathan
Item Type:Article, refereed
Article Subtype:Research Article
Publisher:American Chemical Society
Note:Publication type according to Uni Basel Research Database: Journal article
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Last Modified:25 Feb 2021 02:30
Deposited On:11 Mar 2020 09:17

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