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Molecular Upconversion in Water in Heteropolynuclear Supramolecular Tb/Yb Assemblies
- Source :
- Journal of the American Chemical Society, Journal of the American Chemical Society, 2019, 141 (4), pp.1568-1576. ⟨10.1021/jacs.8b10932⟩, Journal of the American Chemical Society, American Chemical Society, 2019, 141 (4), pp.1568-1576. ⟨10.1021/jacs.8b10932⟩
- Publication Year :
- 2019
- Publisher :
- American Chemical Society (ACS), 2019.
-
Abstract
- Piling up excited states to reach upconversion (UC) is severely restricted by vibrational quenching mechanisms, especially when one looks at discrete molecular entities in solution. By carefully controlling the supramolecular assembly processes resulting from the strong electrostatic interactions between negatively charged Yb complexes and Tb3+ cations in aqueous solutions, we engineered the formation of heteropolynuclear complexes of [(YbL)2Tb x] compositions ( x = 1 and 2). These edifices display a phenomenon of cooperative photosensitization UC with green emission of the Tb cations upon NIR excitation at 980 nm in the Yb absorption band. The photophysical properties of the complexes were carefully investigated by steady-state and time-resolved luminescence experiments in D2O, allowing one to quantify the impact of the composition and pD of the solution on the emission intensity as well as clarifying the exact cooperative photosensitization upconversion mechanism. Using optimized conditions, the energy transfer UC process could be observed for the first time in nondeuterated water with discrete molecular compounds.
- Subjects :
- Quenching (fluorescence)
Aqueous solution
Chemistry
Supramolecular chemistry
General Chemistry
010402 general chemistry
Photochemistry
01 natural sciences
Biochemistry
Catalysis
Photon upconversion
0104 chemical sciences
Supramolecular assembly
Colloid and Surface Chemistry
Absorption band
Excited state
[CHIM.COOR]Chemical Sciences/Coordination chemistry
Luminescence
Subjects
Details
- ISSN :
- 15205126 and 00027863
- Volume :
- 141
- Database :
- OpenAIRE
- Journal :
- Journal of the American Chemical Society
- Accession number :
- edsair.doi.dedup.....c7a21bea30c3c7dc6dfc5759a056dca2