通过活性掺杂的被捕集胶体凝胶的普遍重塑
Universal reshaping of arrested colloidal gels via active doping
摘要:
通过短程吸引相互作用的胶体作为广泛的自组装材料的主要构建块。然而,这种策略的一个众所周知的缺点是,这些结构单元迅速且容易地凝聚成亚稳态胶体凝胶。使用计算机模拟,我们说明了如何添加一小部分的纯排斥性自推进胶体,一种被称为活性掺杂的技术,可以防止这种亚稳凝胶状态的形成,并驱动系统向其结晶有利的目标结构。这种策略的简单性和鲁棒性提供了一种系统和通用的途径来改善大量复杂胶体结构的自组装。我们详细讨论了这一壮举完成的过程,并利用它来调节自组装提供定量指标。我们提供的证据,这种方法的通用性,证明它仍然是强大的下,在二维和三维的一些不同的各向异性短程对相互作用。此外,我们报告了一种新的微相在被动和主动胶体的混合物。对于宽范围的自推进速度,可以稳定相当单分散的有限尺寸微晶的悬浮液。令人惊讶的是,这种微相也对结构单元之间的潜在对相互作用不敏感。这些中等大小的单分散团簇的活性稳定是相当显着的,应该是非常有用的分层自组装策略的设计。这项工作进一步支持了主动力在指导胶体自组装中发挥关键作用的概念。
英文摘要:
Colloids that interact via a short-range attraction serve as the primary building blocks for a broad range of self-assembled materials. However, one of the well-known drawbacks to this strategy is that these building blocks rapidly and readily condense into a metastable colloidal gel. Using computer simulations, we illustrate how the addition of a small fraction of purely repulsive self-propelled colloids, a technique referred to as active doping, can prevent the formation of this metastable gel state and drive the system toward its thermodynamically favored crystalline target structure. The simplicity and robust nature of this strategy offers a systematic and generic pathway to improving the self-assembly of a large number of complex colloidal structures. We discuss in detail the process by which this feat is accomplished and provide quantitative metrics for exploiting it to modulate self-assembly. We provide evidence for the generic nature of this approach by demonstrating that it remains robust under a number of different anisotropic short-ranged pair interactions in both two and three dimensions. In addition, we report on a novel microphase in mixtures of passive and active colloids. For a broad range of self-propelling velocities, it is possible to stabilize a suspension of fairly monodisperse finite-size crystallites. Surprisingly, this microphase is also insensitive to the underlying pair interaction between building blocks. The active stabilization of these moderately-sized monodisperse clusters is quite remarkable and should be of great utility in the design of hierarchical self-assembly strategies. This work further bolsters the notion that active forces can play a pivotal role in directing colloidal self-assembly.
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