3 years ago

Controlling Lanthanide Exchange in Triple-Stranded Helicates: A Way to Optimize Molecular Light-Upconversion

Controlling Lanthanide Exchange in Triple-Stranded Helicates: A Way to Optimize Molecular Light-Upconversion
Yan Suffren, Claude Piguet, Andreas Hauser, Homayoun Nozary, Davood Zare
The kinetic lability of hexadentate gallium-based tripods is sufficient to ensure thermodynamic self-assembly of luminescent heterodimetallic [GaLn(L3)3]6+ helicates on the hour time scale, where Ln is a trivalent 4f-block cation. The inertness is, however, large enough for preserving the triple-helical structure when [GaLn(L3)3]6+ is exposed to lanthanide exchange. The connection of a second gallium-based tripod further slows down the exchange processes to such an extent that spectroscopically active [CrErCr(L4)3]9+ can be diluted into closed-shell [GaYGa(L4)3]9+ matrices without metal scrambling. This feature is exploited for pushing molecular-based energy-transfer upconversion (ETU) at room temperature. Inert noncovalent [GaL3]3+ ions promote an unprecedented keystone mechanism for the capture/release of labile trivalent lanthanides on hour time scales. The cooperative operation of two [GaL3]3+ tripods pushes the limit of inertness to over months, which makes these new materials compatible with the preparation of solid-state solutions displaying molecular-based energy-transfer upconversion at room temperature.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201709156

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