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Donor Engineering and Solid-State Confinement Enable Switchable RTP and TADF in Saccharin-Based Emitters.

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Summary
This summary is machine-generated.

Understanding triplet exciton conversion is key for controllable thermally activated delayed fluorescence (TADF) and room-temperature phosphorescence (RTP). This study reveals how donor engineering and solid-state effects tune triplet fate in saccharin-based emitters for selective emission pathways.

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Computational Chemistry

Background:

  • Controlling triplet exciton conversion is vital for efficient thermally activated delayed fluorescence (TADF) and room-temperature phosphorescence (RTP) in donor-acceptor (D-A) emitters.
  • Understanding the excited-state dynamics, including intersystem crossing (ISC) and reverse intersystem crossing (RISC), is crucial for optimizing luminescence efficiency.

Purpose of the Study:

  • To elucidate the excited-state dynamics and triplet exciton conversion mechanisms of five saccharin-based D-A emitters.
  • To establish a unified mechanistic picture for TADF and RTP emission based on molecular structure and solid-state effects.
  • To demonstrate how donor engineering and solid-state confinement can selectively control emission pathways.

Main Methods:

  • Multiscale calculation methods were employed to investigate the electronic structure and excited states.
  • Thermal vibration correlation function theory was used to analyze excited-state dynamics and energy transfer processes.
  • Comparative studies were performed in both solution and solid states to understand environmental influences.

Main Results:

  • In solution, all emitters showed limited efficiency due to fast nonradiative decay. Inefficient triplet recycling was observed in 6-Cz-Sac and 5-Cz-Sac.
  • DiCz-Sac demonstrated efficient triplet recycling via a T2-assisted RISC channel, while 5-Sac-Pxz and 5-Sac-Ptz exhibited conventional single-channel TADF.
  • In the solid state, crystal packing and hydrogen bonding suppressed relaxation and reduced nonradiative loss, leading to RTP-dominated (6-Cz-Sac, 5-Cz-Sac), mixed TADF/RTP (DiCz-Sac), or single-channel TADF (5-Sac-Pxz, 5-Sac-Ptz) emission.

Conclusions:

  • Donor structure and solid-state packing critically influence triplet exciton fate and emission properties.
  • A unified mechanism explains the selective access to RTP, mixed TADF/RTP, or conventional TADF within the saccharin-based platform.
  • This work provides insights for designing high-performance organic light-emitting diodes (OLEDs) by controlling TADF and RTP processes.