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Area of Science:

  • Photochemistry
  • Materials Science
  • Organic Electronics

Background:

  • Triplet-triplet annihilation photon upconversion (TTA-UC) converts two low-energy photons into one high-energy photon.
  • The statistical probability factor (f) is critical for TTA-UC efficiency, representing singlet state formation probability.
  • Experimental f values for acene-based annihilators show significant variations, hindering efficient TTA-UC system design.

Purpose of the Study:

  • To investigate factors causing variations in the statistical probability factor (f) for acene-based annihilators.
  • To determine the experimental f value for perylene, a commonly used annihilator with widely reported f variations.
  • To provide insights for designing more efficient TTA-UC systems.

Main Methods:

  • Systematic investigation of TTA-UC using a palladium tetraphenyl-benzoporphyrin (PdTPBP) sensitizer and perylene annihilator in THF solution.
  • Experimental determination of the statistical probability factor (f) for perylene.
  • Analysis of energy-gap law effects on singlet formation probability and non-radiative losses.

Main Results:

  • An experimental f value of 17.9 ± 2.1% was obtained for perylene, limiting its maximum TTA-UC quantum yield to 9.0%.
  • The low f value for perylene is attributed to the energy-gap law, with significant non-radiative losses due to a small energy gap between 2 × T1 and T2 states.
  • This energy-gap law dependency was observed in other acene-based annihilators emitting from UV to yellow regions.

Conclusions:

  • The energy-gap law significantly influences the statistical probability factor (f) in acene-based TTA-UC systems.
  • Understanding and mitigating non-radiative losses governed by the energy gap is crucial for enhancing TTA-UC efficiency.
  • This study provides a blueprint for designing future TTA-UC systems by considering molecular energy level alignment and minimizing non-radiative decay pathways.