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Metal-Based Linear Light Upconversion Implemented in Molecular Complexes: Challenges and Perspectives.

Hélène Bolvin1, Alexandre Fürstenberg2,3, Bahman Golesorkhi2

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Summary
This summary is machine-generated.

Researchers achieved molecular light upconversion by designing CrErCr complexes. This breakthrough enables efficient near-infrared to green light conversion within a single molecule, overcoming previous limitations in coordination chemistry.

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Area of Science:

  • Nonlinear Optics
  • Photochemistry
  • Materials Science

Background:

  • Light upconversion, the process of converting low-energy photons to higher energies, was theorized in the 1930s and demonstrated with lasers in the 1960s.
  • Early methods relied on successive photon absorption in materials with long-lived excited states, such as lanthanide ions or polyaromatic molecules, to enhance efficiency.
  • Energy Transfer Upconversion (ETU) using intermolecular sensitization significantly improved overall efficiency over decades.

Purpose of the Study:

  • To achieve light upconversion at the molecular level within a single discrete entity, overcoming challenges associated with coordination complexes.
  • To explore intramolecular energy transfer processes for tunable light upconversion, contrasting with intermolecular methods in doped solids.
  • To demonstrate the feasibility of molecular light upconversion using a trinuclear CrErCr complex.

Main Methods:

  • Design and synthesis of molecular complexes incorporating sensitizer and activator units for intramolecular energy transfer.
  • Utilizing coordination complexes with specific electronic properties to facilitate excited-state absorption (ESA) and energy transfer upconversion (ETU).
  • Investigating mechanisms including ESA, ETU, cooperative luminescence (CL), and cooperative upconversion (CU) in molecular systems.

Main Results:

  • Demonstrated the first detectable near-infrared to green light upconversion in a molecular unit (trinuclear CrErCr complex) under moderate excitation intensity.
  • Established intramolecular energy transfer as a viable and tunable mechanism for molecular light upconversion, governed by first-order kinetics.
  • Showcased advancements in modeling and understanding factors controlling metal-based light upconversion in molecular complexes.

Conclusions:

  • Molecular light upconversion is achievable, offering advantages in tunability and kinetic control over traditional intermolecular methods.
  • The development of specific molecular designs, like the CrErCr complex, is crucial for efficient light upconversion in single entities.
  • Further research into various mechanisms (ESA, ETU, CL, CU) promises expanded applications of molecular light upconversion.