Department of Chemical Engineering, University of New Hamphire, Durham, New Hampshire03824, United States.
ACS Appl Bio Mater. 2024 Feb 19;7(2):535-542. doi: 10.1021/acsabm.2c00910. Epub 2023 Jan 25.
Colloids with lobed architectures have been shown to self-assemble into promising porous structures with potential biomedical applications. The synthesis of these colloids via experiments can be tuned to vary the number and the position of the lobes. However, the polydispersity involving the numbers, sizes, and the dispositions of lobes, that is often observed in particle designs, can significantly affect their self-assembled structures. In this work, we go beyond the uniform lobe size conditions commonly considered in molecular simulations, and probe the effect of polydispersity due to non-uniform lobe sizes by studying self-assembly in three experimentally observable designs of lobed particles (dumbbell, two lobes; trigonal planar, three lobes; and tetrahedral, four lobes), using coarse-grained Langevin dynamics simulations in the NVT ensemble. With increasing polydispersity, we observed the formation of a crystalline structure from a disordered state for the dumbbell system, and a loss of order in the crystalline structures for the trigonal planar system. The tetrahedral system retained a crystalline structure with only a minor loss in compactness. We observed that the effect of polydispersity on the self-assembled morphology of a given system can be minimized by increasing the number of lobes. The polydispersity in the lobe size may also be useful in tuning self-assemblies toward desired structures.
具有叶状结构的胶体已被证明可以自组装成具有潜在生物医学应用的有前途的多孔结构。这些胶体可以通过实验合成来调节叶的数量和位置。然而,在粒子设计中经常观察到的涉及叶的数量、大小和分布的多分散性会显著影响它们的自组装结构。在这项工作中,我们超越了分子模拟中通常考虑的均匀叶大小条件,并通过研究三个实验可观察到的叶状粒子设计(哑铃形,两个叶;三角平面形,三个叶;和四面体形,四个叶)的自组装,来探测由于叶大小不均匀而导致的多分散性的影响,使用 NVT 系综中的粗粒朗之万动力学模拟。随着多分散性的增加,我们观察到哑铃系统从无序状态形成结晶结构,而三角平面系统的结晶结构失去有序。四面体系统仅在紧凑性上略有损失,保留了结晶结构。我们观察到,通过增加叶的数量,可以最小化多分散性对给定系统自组装形态的影响。叶大小的多分散性也可用于调整自组装以获得所需的结构。