磷光
荧光粉
系统间交叉
合理设计
共发射极
发光
组分(热力学)
光电子学
材料科学
化学
光化学
纳米技术
化学物理
荧光
物理
原子物理学
热力学
激发态
光学
单重态
作者
Cheng‐Wei Ju,Xi–Chao Wang,Bo Li,Qiu-Shi Ma,Yuhao Shi,Jinyu Zhang,Yuzhi Xu,Qian Peng,Dongbing Zhao
标识
DOI:10.1073/pnas.2310883120
摘要
Development of single-component organic phosphor attracts increasing interest due to its wide applications in optoelectronic technologies. Theoretically, activating efficient intersystem crossing (ISC) via 1 (π, π*) to 3 (π, π*) transitions, rather than 1 (n, π*) → 3 (π, π*) transitions, is an alternative access to purely organic phosphors but remains challenging. Herein, we designed and successfully synthesized the sila-8-membered ring fused biaryl benzoskeleton by transition metal catalysis, which served as a new organic phosphor with efficient 1 (π, π*) to 3 (π, π*) ISC. We first found that such a compound exhibits a record-long phosphorescence lifetime of 6.5 s at low temperature for single-component organic systems. Then, we developed two strategies to tune their decay channels to evolve such nonemissive molecules into bright phosphors with elongated lifetimes at room temperature: 1) Physic-based design, where quantitative analyses of electron–phonon coupling led us to reveal and hinder the major nonradiative channels, thus lighted up room temperature phosphorescence (RTP) with a lifetime of 480 ms at 298 K; 2) chemical geometry-driven molecular engineering, where a geometry-based descriptor ΔΘ T1–S0 /Θ S0 was developed for rational screening RTP candidates and further improved the RTP lifetime to 794 ms. This study clearly shows the power of interdiscipline among synthetic methodology, physics-based rational design, and computational modeling, which represents a paradigm for the development of an organic emitter.
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