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This study reveals how solid-state effects in thermally activated delayed fluorescence (TADF) molecules influence their luminescence. Bending deformation in the amorphous state enhances TADF properties for improved organic light-emitting diodes.

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Area of Science:

  • Materials Science
  • Organic Chemistry
  • Quantum Chemistry

Background:

  • Thermally activated delayed fluorescence (TADF) molecules are crucial for organic light-emitting diodes (OLEDs) due to tunable solid-state luminescence.
  • Limited theoretical studies exist on the solid-state effects influencing the luminescence of organic emitters.

Purpose of the Study:

  • To investigate the photophysical properties of a difluoroboron β-diketonate-based molecule (M1) in various states (liquid, crystal, amorphous).
  • To understand the solid-state effect on TADF mechanisms and guide the design of new TADF emitters.

Main Methods:

  • Multiscale methods combined with the thermal vibration correlation function theory were employed.
  • Geometric structures and electronic properties (S1-T1 energy gap, spin-orbit coupling) were analyzed in different states.

Main Results:

  • M1 adopts a bent structure in the amorphous state due to intramolecular hydrogen bonding and intermolecular interactions.
  • The amorphous state significantly reduces the S1-T1 energy gap and increases spin-orbit coupling, favoring TADF.
  • Solid-state emission exhibits a red shift compared to the liquid state.

Conclusions:

  • The solid-state effect, particularly molecular conformation changes, plays a critical role in enhancing TADF properties.
  • Theoretical design of M2 demonstrates potential for near-infrared emitting TADF materials.
  • This work provides insights into TADF mechanisms and aids in designing novel TADF emitters with tunable solid-state emission.