arXivDaily arXiv每日学术速递 周一至周五更新
arXiv 2103.14526cond-mat.softcond-mat.mtrl-scicond-mat.stat-mechphysics.chem-ph
收藏

球形禁闭中胶体团簇的自由能谱

Free Energy Landscape of Colloidal Clusters in Spherical Confinement

Junwei Wang, Chrameh Fru Mbah, Thomas Przybilla, Silvan Englisch, Erdmann Spiecker, Michael Engel, Nicolas Vogel

摘要:

有限自组装系统的结构敏感地依赖于组成构件的数量。近年来研究表明,硬球胶体粒子在球形乳液液滴中表现出幻数效应。几何构造规则允许几十个幻数对应于一系列离散的完全填充的同心二十面体壳。在这里,我们调查的自由能景观的这些胶体集群作为一个功能的组成模块的系统大小高达几千个粒子的数量。我们发现,最小的自由能景观,所产生的填充,同心壳的存在下,显着扩大。与它们的原子类似物相比,球形限制中的胶体团簇可以通过在团簇中心有序化二十面体同时改变团簇表面附近的结构来灵活地容纳多余的胶体。在这些幻数区域之间,构建块不能排列成填充壳。相反,我们观察到,缺陷积累在一个单一的楔形,因此只影响少数四面体晶粒的集群。我们预测这个楔形的存在,通过模拟和确认它的存在,在实验中使用电子断层扫描。楔形的引入通过将缺陷限制在簇内的小区域来最小化自由能惩罚。此外,剩余的有序四面体晶粒可以通过破坏二十面体对称性来松弛内部应变。我们的研究结果表明,多种缺陷机制如何相互勾结,形成复杂的自由能景观硬球状胶体集群。

英文摘要:

The structure of finite self-assembling systems depends sensitively on the number of constituent building blocks. Recently, it was demonstrated that hard sphere-like colloidal particles show a magic number effect when confined in spherical emulsion droplets. Geometric construction rules permit a few dozen magic numbers that correspond to a discrete series of completely filled concentric icosahedral shells. Here, we investigate the free energy landscape of these colloidal clusters as a function of the number of their constituent building blocks for system sizes up to several thousand particles. We find that minima in the free energy landscape, arising from the presence of filled, concentric shells, are significantly broadened. In contrast to their atomic analogues, colloidal clusters in spherical confinement can flexibly accommodate excess colloids by ordering icosahedrally in the cluster center while changing the structure near the cluster surface. In-between these magic number regions, the building blocks cannot arrange into filled shells. Instead, we observe that defects accumulate in a single wedge and therefore only affect a few tetrahedral grains of the cluster. We predict the existence of this wedge by simulation and confirm its presence in experiment using electron tomography. The introduction of the wedge minimizes the free energy penalty by confining defects to small regions within the cluster. In addition, the remaining ordered tetrahedral grains can relax internal strain by breaking icosahedral symmetry. Our findings demonstrate how multiple defect mechanisms collude to form the complex free energy landscape of hard sphere-like colloidal clusters.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

↑