State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, iChEM and Key Laboratory of Chemical Biology of Fujian Province, Xiamen University, Xiamen, 361005, China.
Institute for Complex Molecular Systems and Computational Biology Group, Eindhoven University of Technology, PO Box 513, 5600 MB, Eindhoven, The Netherlands.
Nat Commun. 2018 Feb 5;9(1):488. doi: 10.1038/s41467-017-02605-x.
Chiral amplification in molecular self-assembly has profound impact on the recognition and separation of chiroptical materials, biomolecules, and pharmaceuticals. An understanding of how to control this phenomenon is nonetheless restricted by the structural complexity in multicomponent self-assembling systems. Here, we create chiral octahedra incorporating a combination of chiral and achiral vertices and show that their discrete nature makes these octahedra an ideal platform for in-depth investigation of chiral transfer. Through the construction of dynamic combinatorial libraries, the unique possibility to separate and characterise each individual assembly type, density functional theory calculations, and a theoretical equilibrium model, we elucidate that a single chiral unit suffices to control all other units in an octahedron and how this local amplification combined with the distribution of distinct assembly types culminates in the observed overall chiral amplification in the system. Our combined experimental and theoretical strategy can be applied generally to quantify discrete multi-component self-assembling systems.
手性分子自组装中的手性放大对手性材料、生物分子和药物的识别和分离有深远的影响。然而，对手性放大的控制理解受到多组分自组装体系结构复杂性的限制。在这里，我们构建了包含手性和非手性顶点的手性八面体，并表明它们的离散性质使这些八面体成为深入研究手性转移的理想平台。通过构建动态组合库，独特的分离和表征每个单体组装类型的可能性、密度泛函理论计算和理论平衡模型，我们阐明了一个手性单元足以控制八面体中的所有其他单元，以及这种局部放大如何与不同组装类型的分布相结合，在手性放大系统中观察到整体手性放大。我们的组合实验和理论策略可以普遍应用于量化离散的多组分自组装体系。
