揭示荧光素衍生物ACQ向AIE转化的机制,The Journal of Physical Chemistry A

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揭示荧光素衍生物ACQ向AIE转化的机制
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2023-06-09 , DOI: 10.1021/acs.jpca.3c02244
Gaoshang Jiang _{1,

2} , Jianyong Liu ₁ , Panwang Zhou _{1,

3}

Affiliation

尽管荧光素衍生物具有优异的性能和较强的实用性，但它们是典型的聚集诱导猝灭（ACQ）分子，不利于在固态下工作。最近，合成了具有聚集诱导发射（AIE）特性的荧光素衍生物Fl-Me，为荧光素基材料的研究和开发带来了新的曙光。本研究基于时间相关密度泛函理论和ONIOM方法研究了Fl-Me的AIE机理。结果表明，有效的暗态失活途径导致 Fl-Me 在溶液环境中荧光猝灭。因此，AIE现象源于暗态猝灭通道的关闭。值得强调的是，我们发现分子Fl-Me的羰基与相邻分子之间存在分子间氢键相互作用，导致晶态暗态能量的增加。此外，旋转运动的限制和π-π堆积相互作用的不存在有利于聚集时荧光的增强。最后，讨论了荧光素衍生物的ACQ到AIE的转化机制。这项工作为具有AIE功能的荧光素衍生物Fl–Me的光物理机制提供了更深入的见解，最终有望帮助研究人员开发更多具有卓越性能的荧光素基AIE材料，应用于各个领域。导致晶态暗态能量的增加。此外，旋转运动的限制和π-π堆积相互作用的不存在有利于聚集时荧光的增强。最后，讨论了荧光素衍生物的ACQ到AIE的转化机制。这项工作为具有AIE功能的荧光素衍生物Fl–Me的光物理机制提供了更深入的见解，最终有望帮助研究人员开发更多具有卓越性能的荧光素基AIE材料，应用于各个领域。导致晶态暗态能量的增加。此外，旋转运动的限制和π-π堆积相互作用的不存在有利于聚集时荧光的增强。最后，讨论了荧光素衍生物的ACQ到AIE的转化机制。这项工作为具有AIE功能的荧光素衍生物Fl–Me的光物理机制提供了更深入的见解，最终有望帮助研究人员开发更多具有卓越性能的荧光素基AIE材料，应用于各个领域。讨论了荧光素衍生物的ACQ到AIE的转化机制。这项工作为具有AIE功能的荧光素衍生物Fl–Me的光物理机制提供了更深入的见解，最终有望帮助研究人员开发更多具有卓越性能的荧光素基AIE材料，应用于各个领域。讨论了荧光素衍生物的ACQ到AIE的转化机制。这项工作为具有AIE功能的荧光素衍生物Fl–Me的光物理机制提供了更深入的见解，最终有望帮助研究人员开发更多具有卓越性能的荧光素基AIE材料，应用于各个领域。

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Unraveling the Mechanism of ACQ-to-AIE Transformation of Fluorescein Derivatives

Although fluorescein derivatives have excellent properties and strong practicability, they are typical aggregation-induced quenching (ACQ) molecules, which are not conducive to working in the solid state. Recently, the fluorescein derivative Fl–Me with aggregation-induced emission (AIE) property was synthesized, which brought a new dawn for the research and development of fluorescein-based materials. In this study, the AIE mechanism of Fl–Me was investigated based on time-dependent density functional theory and the ONIOM method. The results revealed that an effective dark-state deactivation pathway leads to the fluorescence quenching of Fl–Me in a solution environment. Accordingly, the AIE phenomenon originates from the closure of the dark-state quenching channel. It is worth emphasizing that we found that the carbonyl group of molecular Fl–Me has intermolecular hydrogen bonding interaction with the adjacent molecules, which caused the increase of the dark-state energy in the crystalline state. Moreover, the restriction of the rotational motion and the nonexistence of the π–π stacking interaction are beneficial to the enhancement of fluorescence upon aggregation. Finally, the ACQ-to-AIE transformation mechanisms of fluorescein derivatives have been discussed. This work provides deeper insight into the photophysical mechanism for the fluorescein derivatives Fl–Me with AIE feature and eventually is expected to help researchers to develop more fluorescein-based AIE materials with remarkable properties for various fields.

更新日期：2023-06-09

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