论文标题

接口处的微凝胶作为具有重入动力学的2D弹性粒子的表现

Microgels at interfaces behave as 2D elastic particles featuring reentrant dynamics

论文作者

Camerin, Fabrizio, Gnan, Nicoletta, Ruiz-Franco, José, Ninarello, Andrea, Rovigatti, Lorenzo, Zaccarelli, Emanuela

论文摘要

软胶体越来越多地用作模型系统,以解决诸如结晶以及玻璃和干扰过渡之类的基本问题。在可用的软胶体类别中,微凝胶正在成为黄金标准。由于它们的内部复杂性使他们的理论表征非常困难,因此在线性弹性理论的简单框架内,至少在小型形式的制度中,通常对微凝胶进行建模。在这里,我们表明存在可以大大扩展其有效性范围的条件,提供了有力的数值证据,表明在界面上吸附的微凝胶遵循二维的赫兹理论,因此与在散装条件下发现的鲜明对比的是2D弹性颗粒,直到2D弹性颗粒。我们还能够估算幼体的单个颗粒模量,并通过将其与较大条件下的对应物进行比较,我们证明了界面处的聚合物网络的显着僵硬。最后,通过分析动力学特性,我们预测了多种重新入侵现象:通过颗粒密度的连续增加,微凝胶首先停止,然后由于其延伸的冠状运动的高渗透性而重新燃料。我们观察到这种异常行为在一系列实验可访问的条件下,对于小而松散的交联微凝胶。因此,目前的工作将微凝胶建立在界面上,作为一种新的模型系统,用于基础研究,为实验合成和研究独特的高密度液体状状态的研究铺平了道路。此外,这些结果可以指导在表面上开发新颖的组装和图案策略,并设计具有所需界面行为的新型材料。

Soft colloids are increasingly used as model systems to address fundamental issues such as crystallisation and the glass and jamming transitions. Among the available classes of soft colloids, microgels are emerging as the gold standard. Since their great internal complexity makes their theoretical characterization very hard, microgels are commonly modelled, at least in the small-deformation regime, within the simple framework of linear elasticity theory. Here we show that there exist conditions where its range of validity can be greatly extended, providing strong numerical evidence that microgels adsorbed at an interface follow the two-dimensional Hertzian theory, and hence behave like 2D elastic particles, up to very large deformations, in stark contrast to what found in bulk conditions. We are also able to estimate the Young's modulus of the individual particles and, by comparing it with its counterpart in bulk conditions, we demonstrate a significant stiffening of the polymer network at the interface. Finally, by analyzing dynamical properties, we predict multiple reentrant phenomena: by a continuous increase of particle density, microgels first arrest and then re-fluidify due to the high penetrability of their extended coronas. We observe this anomalous behavior in a range of experimentally accessible conditions for small and loosely crosslinked microgels. The present work thus establishes microgels at interfaces as a new model system for fundamental investigations, paving the way for the experimental synthesis and research on unique high-density liquidlike states. In addition, these results can guide the development of novel assembly and patterning strategies on surfaces and the design of novel materials with desired interfacial behavior.

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