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Direct population of triplet excited states through singlet–triplet transition for visible-light excitable organic afterglow

机译:通过单重态-三重态跃迁直接填充三重态激发态以获得可见光可激发的有机余辉

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摘要

Invoking efficient afterglow in metal-free organic molecules represents an important material advancement. However, organic afterglow suffers from low intensity and efficiency and generally needs to be excited by UV light owing to its spin-forbidden phosphorescent nature that essentially requires facile intersystem crossing (ISC). Here, we propose a strategy to bypass the traditional ISC through facilitating singlet–triplet transition to directly populate triplet excited states from the ground state by combining synergetic effects of both heavy/hetero-atom incorporation and aromatic aggregation. Verified by systematic experimental and computational investigations, this unique singlet-to-triplet absorption results in a much improved organic afterglow quantum efficiency up to 9.5% with a prolonged lifetime of 0.25 s under visible-light irradiation. Fundamentally, this work illustrates for the first time the great potential of the direct population method to red-shift the excitation wavelength and improve the afterglow efficiency, offering important clues for the development of triplet-state involved organic optoelectronic technologies.
机译:在不含金属的有机分子中调用有效的余辉代表着重要的材料进展。然而,有机余辉的强度和效率较低,并且由于其自旋禁止的磷光性质而通常需要用紫外光激发,这本质上要求容易的系统间交叉(ISC)。在这里,我们提出了一种策略,通过结合重/杂原子掺入和芳族聚集的协同效应,通过促进单重态-三重态跃迁从基态直接构成三重态激发态来绕过传统的ISC。经过系统的实验和计算研究验证,这种独特的单重态-三重态吸收导致可见光照射下有机余辉量子效率大大提高,高达9.5%,寿命延长0.25 s。从根本上讲,这项工作首次说明了直接填充方法在激发波长红移和提高余辉效率方面的巨大潜力,这为涉及三重态有机光电技术的发展提供了重要线索。

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