School of Chemistry, University of Birmingham, Edgbaston, Birmingham B15 2TT, UK.
Nanoscale. 2018 Jul 26;10(29):13875-13882. doi: 10.1039/c7nr09258j.
Encoding hierarchical self-assembly in colloidal building blocks is a promising bottom-up route to high-level structural complexity often observed in biological materials. However, harnessing this promise faces the grand challenge of bridging hierarchies of multiple length- and time-scales, associated with structure and dynamics respectively along the self-assembly pathway. Here we report on a case study, which examines the kinetic accessibility of a series of hollow spherical structures with a two-level structural hierarchy self-assembled from charge-stabilized colloidal magnetic particles. By means of a variety of computational methods, we find that for a staged assembly pathway, the structure, which derives the strongest energetic stability from the first stage of assembly and the weakest from the second stage, is most kinetically accessible. Such a striking correspondence between energetics and kinetics for optimal design principles should have general implications for programming hierarchical self-assembly pathways for nano- and micro-particles, while matching stability and accessibility.
编码胶体构建块中的层次自组装是一种很有前途的自下而上的方法，可以实现生物材料中常见的高级结构复杂性。然而，要实现这一目标，面临着一个巨大的挑战，即需要在沿着自组装途径的结构和动力学方面，分别跨越多个长度和时间尺度的层次。在这里，我们报告了一个案例研究，该研究考察了一系列具有两级结构层次的中空球形结构的动力学可及性，这些结构是由带电稳定胶体磁性颗粒自组装而成的。通过各种计算方法，我们发现对于分阶段组装途径，结构从第一阶段组装中获得最强的能量稳定性，而从第二阶段组装中获得最弱的能量稳定性，其动力学可及性最强。这种在最佳设计原则中，能量学和动力学之间的惊人对应关系，对于为纳米和微粒子编程层次自组装途径，同时匹配稳定性和可及性，应该具有普遍的意义。
