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Published on: August 21, 2018
Programming the Excited-State Landscape Via Carborane Count for Dual TADF/RTP
Yangtao Shao1, Xubin Wang1, Hexi Wei1
1Shaanxi Key Laboratory of New Concept Sensors and Molecular Materials, Key Laboratory of Applied Surface and Colloid Chemistry (Ministry of Education), School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an 710119, P. R. China.
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.
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.
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