论文标题

通过活动掺杂来普遍重塑被捕的胶体凝胶

Universal reshaping of arrested colloidal gels via active doping

论文作者

Mallory, S. A., Bowers, M. L., Cacciuto, A.

论文摘要

通过短距离吸引力相互作用的胶体是广泛的自组装材料的主要构建块。但是,该策略的众所周知的缺点之一是,这些构件迅速凝结成亚稳态的胶体凝胶。使用计算机模拟,我们说明了一小部分纯粹排斥的自旋转胶体的添加是如何添加称为活动掺杂的一种技术,可以防止形成这种稳态的凝胶状态并将系统驱动到其热力学上偏爱的结晶靶结构。该策略的简单性和鲁棒性具有改善大量复杂胶体结构的自组装的系统和通用途径。我们详细讨论了完成此壮举的过程,并提供了用于利用它来调节自组装的定量指标。我们通过证明在两个和三个维度的许多不同各向异性的短距离相互作用下,它在多个不同的各向异性短距离相互作用下保持稳健,从而为这种方法提供了证据。此外,我们报告了被动和活性胶体混合物中的一种新型显微相。对于广泛的自我推销速度,可以稳定相当单分散的有限大小的晶体的悬架。令人惊讶的是,该微观相对于构建基块之间的基本对相互作用也不敏感。这些中等大小的单分散簇的积极稳定非常出色,在层次结构自组装策略的设计中应该具有很大的实用性。这项工作进一步增强了这样一种观念,即主动力可以在指导胶体自组装中发挥关键作用。

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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