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Programming the Excited-State Landscape Via Carborane Count for Dual TADF/RTP.

Yangtao Shao1, Xubin Wang1, Hexi Wei1

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This summary is machine-generated.

Concurrent thermally activated delayed fluorescence (TADF) and room-temperature phosphorescence (RTP) were achieved in carborane-based molecules. This engineering approach enables dual-channel emission with ultralong TADF lifetimes, offering a new design for light-emitting materials.

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Area of Science:

  • Materials Science
  • Organic Chemistry
  • Photophysics

Background:

  • Concurrent thermally activated delayed fluorescence (TADF) and room-temperature phosphorescence (RTP) in a single molecular system are challenging to achieve.
  • Developing novel luminophores with dual emission capabilities is crucial for advanced optical applications.

Purpose of the Study:

  • To engineer carborane-functionalized triphenylamines (TPA-1Cb/2Cb/3Cb) for concurrent TADF and RTP emission.
  • To investigate the effect of carborane count on the photophysical properties and emission mechanisms.

Main Methods:

  • Synthesis of carborane-functionalized triphenylamines.
  • Spectroscopic analysis (UV-Vis absorption, emission spectra, transient absorption).
  • Time-dependent density functional theory (TD-DFT) calculations based on crystal structures.

Main Results:

  • Carborane-number engineering successfully programmed the excited state landscape (S1-Tn) and facilitated dual emission.
  • TPA-2Cb and TPA-3Cb exhibited solution-phase TADF, and solid-state TADF/RTP coexistence under ambient conditions.
  • Ultralong TADF lifetimes of 67.4 ms (TPA-2Cb) and 105.3 ms (TPA-3Cb) were recorded.
  • Carborane-count-dependent tuning of energy gaps (ΔE(S1-Tn)) and spin-orbit coupling (SOC) were identified as key factors.

Conclusions:

  • A compact and generalizable strategy for creating concurrent TADF/RTP luminophores using carborane-based materials was established.
  • This approach enables time-programmable dual emission, expanding possibilities for optoelectronic devices.
  • The study provides a design principle for future development of advanced luminescent materials.