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We developed the first covalent organic frameworks (COFs) for efficient solid-state triplet-triplet annihilation upconversion (TTA-UC). These materials enable low-power light management for applications like bioimaging and solar energy harvesting.

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aminal‐linked COFscovalent organic frameworksphoton upconversiontriplet migrationtriplet‐triplet annihilation

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Area of Science:

  • Materials Science
  • Photochemistry
  • Polymer Chemistry

Background:

  • Photon upconversion (UC) is crucial for bioimaging and solar energy.
  • Solution-phase triplet-triplet annihilation upconversion (TTA-UC) faces challenges in solid-state applications.
  • Developing robust solid-state TTA-UC platforms is a key research goal.

Purpose of the Study:

  • To engineer covalent organic frameworks (COFs) for efficient sensitized triplet-triplet annihilation upconversion (TTA-UC).
  • To investigate the performance of aminal-linked COFs integrating anthracene chromophores as solid-state upconverters.
  • To establish design principles for improved solid-state TTA-UC materials.

Main Methods:

  • Synthesis and structural characterization of aminal-linked anthracene-based COFs (Ant-COF-H and Ant-COF-OH).
  • Photoluminescence quantum yield (ΦF) and upconversion quantum yield (UCQY) measurements.
  • Time-resolved emission spectroscopy to study energy transfer dynamics.
  • Correlation of framework structure with energy loss mechanisms.

Main Results:

  • Synthesized highly crystalline COFs with strong photoluminescence (ΦF ≈ 40%).
  • Achieved upconverted emission with quantum yields up to 1.8% using a palladium porphyrin sensitizer.
  • Demonstrated efficient TTA-UC at low excitation power densities (onset of saturation at 100 mW cm-2).
  • Identified intra-framework triplet migration as the dominant energy transfer mechanism.

Conclusions:

  • Aminal-linked COFs can serve as effective solid-state platforms for sensitized TTA-UC.
  • Engineered COFs surpass the performance of conventional solution-phase systems.
  • This work provides a foundation for practical, low-power light management using crystalline polymers.