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Host Surface-Induced Excitation Wavelength-Dependent Organic Afterglow
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-06-08 , DOI: 10.1021/jacs.3c03681
Zhongwei Man 1, 2 , Zheng Lv 3 , Zhenzhen Xu 1 , Jingping He 1 , Qing Liao 1 , Yongan Yang 2 , Jiannian Yao 2, 4 , Hongbing Fu 1, 2
Affiliation  

The design and construction of organic afterglow materials is an attractive but formidably challenging task due to the low intersystem crossing efficiency and nonradiative decay. Here, we developed a host surface-induced strategy to achieve excitation wavelength-dependent (Ex-De) afterglow emission through a facile dropping process. The prepared PCz@dimethyl terephthalate (DTT)@paper system exhibits a room-temperature phosphorescence afterglow, with the lifetime up to 1077.1 ± 15 ms and duration time exceeding 6 s under ambient conditions. Furthermore, we can switch the afterglow emission on and off by adjusting the excitation wavelength below or above 300 nm, showing a remarkable Ex-De behavior. Spectral analysis demonstrated that the afterglow originates from the phosphorescence of PCz@DTT assemblies. The stepwise preparation process and detailed experiments (XRD, 1H NMR, and FT-IR analysis) proved the presence of strong intermolecular interactions between the carbonyl groups on the surface of DTT and the entire frame of PCz, which can inhibit the nonradiative processes of PCz to achieve afterglow emission. Theoretical calculations further manifested that DTT geometry alteration under different excitation beams is the main reason for the Ex-De afterglow. This work discloses an effective strategy for constructing smart Ex-De afterglow systems that can be fully exploited in a range of fields.

中文翻译:

主体表面诱导激发波长相关的有机余辉

由于低系间穿越效率和非辐射衰减,有机余辉材料的设计和构造是一项有吸引力但极具挑战性的任务。在这里,我们开发了一种主体表面诱导策略,通过简单的滴落过程实现激发波长相关(Ex-De)余辉发射。所制备的PCz@对苯二甲酸二甲酯(DTT)@paper体系表现出室温磷光余辉,在环境条件下寿命可达1077.1±15 ms,持续时间超过6 s。此外,我们可以通过调节低于或高于 300 nm 的激发波长来打开和关闭余辉发射,显示出显着的 Ex-De 行为。光谱分析表明余辉源自 PCz@DTT 组件的磷光。1 H NMR和FT-IR分析证明DTT表面的羰基与PCz整个框架之间存在强烈的分子间相互作用,可以抑制PCz的非辐射过程,从而实现余辉发射。理论计算进一步表明,不同激发光束下DTT几何结构的改变是Ex-De余辉产生的主要原因。这项工作揭示了构建智能 Ex-De 余辉系统的有效策略,该系统可以在一系列领域得到充分利用。
更新日期:2023-06-08
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