Triplet-Fusion Upconversion Using a Rigid Tetracene Homodimer
Triplet-Fusion Upconversion Using a Rigid Tetracene Homodimer
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DOI：
10.1021/acs.jpclett.9b03115
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发表时间：
2019-12-05
影响因子：
5.7
通讯作者：
Wilson, Mark W. B.
中科院分区：
文献类型：
--
作者：
Imperiale, Christian J.;Green, Philippe B.;Wilson, Mark W. B.
通过观察在波长为730 nm的三重态敏化剂激发下，降冰片桥联的四苯均二聚体发射的光子(波长=540 nm)，证明了结构刚性、弱耦合的分子二聚体可以取代传统的单体湮没分子用于溶液中的三重态聚变上转换(TUC)。有趣的是，稳态光谱、动力学模拟和Stern-Volmer猝灭实验表明，二聚体表现出与母体单体本质上不同的光物理：它在扩散介导的三重态激子转移方面效率较低，但它更有效地融合了提取的三重态。我们的结果支持开发超越扩散介导的三联体提取的复合三联体融合平台，最终绕过溶液相TUC的浓度依赖。
We demonstrate that a structurally rigid, weakly coupled molecular dimer can replace traditional monomeric annihilators for triplet fusion upconversion (TUC) in solution by observing emitted photons (lambda = 540 nm) from a norbornyl-bridged tetracene homodimer following excitation of a triplet sensitizer at lambda = 730 nm. Intriguingly, steady-state spectroscopy, kinetic simulations, and Stern-Volmer quenching experiments show that the dimer exhibits qualitatively different photophysics than its parent monomer: it is less effective at diffusion-mediated triplet exciton transfer, but it fuses extracted triplets more efficiently. Our results support the development of composite triplet-fusion platforms that go beyond diffusion-mediated triplet extraction, ultimately circumventing the concentration dependence of solution-phase TUC.