Deciphering and quantifying linear light upconversion in molecular erbium complexes

Chemical Science
Bahman GolesorkhiClaude Piguet

Abstract

Single-center light upconversion corresponds to the piling up of low-energy photons via successive linear absorptions: a phenomenon commonly observed in lanthanide-doped low-phonon ionic solids or nanoparticles. Its ultimate miniaturization in molecular complexes opens challenging perspectives in terms of improved reproducibility, chemical control and optical programming. However, high-energy vibrations inherent in coordination complexes severely limit the efficiency of successive excited-state absorptions (ESAs) responsible for the gain in photon energy. By carefully wrapping three polyaromatic ligand strands around trivalent erbium, we managed to induce low-power room temperature near-infrared (λexc = 801 nm or 966 nm) to visible green (λem = 522 nm and 545 nm) light upconversion within mononuclear coordination complexes [Er(Lk )3]3+ operating either in the solid state or in non-deuterated solution. The calculated upconversion quantum yields set the zero-level of an elemental erbium-centered molecular ESA mechanism, a value which favorably compares with cooperative upconversion (CU) previously implemented in sophisticated multisite Yb2Tb supramolecular assemblies. The various dependences of the upconverted emission on the inc...Continue Reading

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Citations

Feb 27, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Guoying HanPengfei Yan
May 6, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Jorge H S K Monteiro
Jun 20, 2020·Angewandte Chemie·Jens KalmbachMichael Seitz
Dec 18, 2020·Chemical Communications : Chem Comm·Richard C KnightonLoïc J Charbonnière
Jan 26, 2021·Inorganic Chemistry·Gwladys NizouRaphaël Tripier
May 1, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Bahman GolesorkhiClaude Piguet
Sep 10, 2021·Journal of the American Chemical Society·Bahman GolesorkhiClaude Piguet
Nov 9, 2021·Angewandte Chemie·Richard C KnightonLoïc J Charbonnière

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Methods Mentioned

BETA
X-ray

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