How Do Molecular Motions Affect Structures and Properties at Molecule and Aggregate Levels?,Journal of the American Chemical Society

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How Do Molecular Motions Affect Structures and Properties at Molecule and Aggregate Levels?
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-07-22 , DOI: 10.1021/jacs.1c05647
Deshuang Tu ₁ , Jianyu Zhang ₁ , Yunxiao Zhang ₁ , Herman H Y Sung ₁ , Lijie Liu ₁ , Ryan T K Kwok ₁ , Jacky W Y Lam ₁ , Ian D Williams ₁ , Hong Yan ₂ , Ben Zhong Tang _{1,

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Affiliation

Molecular motions are essential natures of matter and play important roles in their structures and properties. However, owing to the diversity and complexity of structures and behaviors, the study of motion–structure–property relationships remains a challenge, especially at all levels of structural hierarchy from molecules to macro-objects. Herein, luminogens showing aggregation-induced emission (AIE), namely, 9-(pyrimidin-2-yl)-carbazole (PyCz) and 9-(5-R-pyrimidin-2-yl)-carbazole [R = Cl (ClPyCz), Br (BrPyCz), and CN (CyPyCz)], were designed and synthesized, to decipher the dependence of materials’ structures and properties on molecular motions at the molecule and aggregate levels. Experimental and theoretical analysis demonstrated that the active intramolecular motions in the excited state of all molecules at the single-molecule level endowed them with more twisted structural conformations and weak emission. However, owing to the restriction of intramolecular motions in the nano/macroaggregate state, all the molecules assumed less twisted conformations with bright emission. Unexpectedly, intermolecular motions could be activated in the macrocrystals of ClPyCz, BrPyCz, and CyPyCz through the introduction of external perturbations, and synergic strong and weak intermolecular interactions allowed their crystals to undergo reversible deformation, which effectively solved the problem of the brittleness of organic crystals, while endowing them with excellent elastic performance. Thus, the present study provided insights on the motion–structure–property relationship at each level of structural hierarchy and offered a paradigm to rationally design multifunctional AIE-based materials.

中文翻译：

分子运动如何影响分子和聚集体水平的结构和性质？

分子运动是物质的基本性质，在其结构和性质中起着重要作用。然而，由于结构和行为的多样性和复杂性，运动-结构-性质关系的研究仍然是一个挑战，特别是在从分子到宏观物体的结构层次的各个层次上。在此，发光体显示聚集诱导发射 (AIE)，即 9-(pyrimidin-2-yl)-carbazole (PyCz) 和 9-(5-R-pyrimidin-2-yl)-carbazole [R = Cl (ClPyCz )、Br (BrPyCz) 和 CN (CyPyCz)] 被设计和合成，以破译材料的结构和性质对分子和聚集体水平上分子运动的依赖性。实验和理论分析表明，所有分子在单分子水平上处于激发态的活跃分子内运动赋予它们更多扭曲的结构构象和弱发射。然而，由于纳米/大聚集体状态下分子内运动的限制，所有分子都呈现出较少扭曲的构象，并具有明亮的发射。出乎意料的是，ClPyCz、BrPyCz和CyPyCz的大晶体可以通过引入外部扰动激活分子间运动，强弱分子间协同作用使其晶体发生可逆变形，有效解决了有机晶体脆性问题，同时赋予它们优良的弹性性能。因此，

更新日期：2021-08-04

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