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Upconversion in a d-f [RuYb3] Supramolecular Assembly.

Richard C Knighton1, Lohona K Soro1, Waygen Thor1,2

  • 1Equipe de Synthèse Pour L'Analyse (SynPA), Institut Pluridisciplinaire Hubert Curien (IPHC), UMR 7178, CNRS, Université de Strasbourg, ECPM, 25 rue Becquerel, 67087 Strasbourg Cedex, France.

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Researchers developed a novel hetero-tetrametallic assembly for molecular upconversion. This system demonstrates the first f → d molecular upconversion, emitting light via a cooperative photosensitization mechanism.

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Area of Science:

  • Inorganic Chemistry
  • Photochemistry
  • Materials Science

Background:

  • Lanthanide ions, particularly ytterbium, are known for their near-infrared absorption properties.
  • Ruthenium polypyridyl complexes, such as [Ru(bpm)3]2+, exhibit rich photophysical behavior.
  • Molecular upconversion (UC) is a process where lower-energy photons are converted into higher-energy photons.

Purpose of the Study:

  • To synthesize and characterize a novel hetero-tetrametallic assembly.
  • To demonstrate and investigate the first instance of f → d molecular upconversion.
  • To elucidate the mechanism behind the observed upconversion process.

Main Methods:

  • Preparation of a hetero-tetrametallic assembly containing ytterbium and ruthenium ions.
  • Photophysical characterization including irradiation at 980 nm and emission spectroscopy at 636 nm.
  • Time-resolved measurements and kinetic modeling to understand the upconversion mechanism.

Main Results:

  • Successful synthesis of a hetero-tetrametallic assembly with three ytterbium ions and a central [Ru(bpm)3]2+ core.
  • Demonstration of f → d molecular upconversion, evidenced by 980 nm excitation leading to 636 nm emission.
  • Time-resolved studies indicated a slow rise in upconversion emission, consistent with a cooperative photosensitization mechanism.

Conclusions:

  • The study presents the first example of f → d molecular upconversion.
  • A cooperative photosensitization mechanism involving a virtual ytterbium-centered doubly excited state and energy transfer to the ruthenium complex is proposed.
  • This work opens new avenues for designing light-harvesting and energy-transfer systems.