Lanthanoid/Alkali Metal ß-Triketonate Assemblies: A Robust Platform for Efficient NIR Emitters.
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This is the peer reviewed version of the following article: Reid, B. and Stagni, S. and Malicka, J. and Cocchi, M. and Sobolev, A. and Skelton, B. and Moore, E. et al. 2015. Lanthanoid/Alkali Metal ß-Triketonate Assemblies: A Robust Platform for Efficient NIR Emitters. Chemistry. 21 (50): pp. 18354-18363., which has been published in final form at http://doi.org/10.1002/chem.201502536This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving at http://olabout.wiley.com/WileyCDA/Section/id-828039.html#terms
The reaction of hydrated lanthanoid chlorides with tribenzoylmethane and an alkali metal hydroxide consistently resulted in the crystallization of neutral tetranuclear assemblies with the general formula [Ln(Ae⋅HOEt)(L)4]2 (Ln=Eu3+, Er3+, Yb3+; Ae=Na+, K+, Rb+). Analysis of the crystal structures of these species revealed a coordination geometry that varied from a slightly distorted square antiprism to a slightly distorted triangular dodecahedron, with the specific geometrical shape being dependent on the degree of lattice solvation and identity of the alkali metal. The near-infrared (NIR)-emitting assemblies of Yb3+ and Er3+ showed remarkably efficient emission, characterized by significantly longer excited-state lifetimes (τobs≈37–47 μs for Yb3+ and τobs≈4–6 μs for Er3+) when compared with the broader family of lanthanoid β-diketonate species, even in the case of perfluorination of the ligands. The Eu3+ assemblies show bright red emission and a luminescence performance (τobs≈0.5 ms, equation image≈35–37 %, ηsens≈68–70 %) more akin to the β-diketonate species. The results highlight that the β-triketonate ligand offers a tunable and facile system for the preparation of efficient NIR emitters without the need for more complicated perfluorination or deuteration synthetic strategies.
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