Programmable self-assembly of core-shell ellipsoids at liquid interfaces

Jack Eatson, Susann Bauernfeind, Benjamin Midtvedt, Antonio Ciarlo, Johannes Menath, Giuseppe Pesce, Andrew B. Schofield, Giovanni Volpe, Paul S. Clegg, Nicolas Vogel, D. Martin. A. Buzza, Marcel Rey
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Abstract

Ellipsoidal particles confined at liquid interfaces exhibit complex self-assembly behaviour due to quadrupolar capillary interactions induced by meniscus deformation. These interactions cause particles to attract each other in either tip-to-tip or side-to-side configurations. However, controlling their interfacial self-assembly is challenging because it is difficult to predict which of these two states will be preferred. In this study, we demonstrate that introducing a soft shell around hard ellipsoidal particles provides a means to control the self-assembly process, allowing us to switch the preferred configuration between these states. We study their interfacial self-assembly and find that pure ellipsoids without a shell consistently form a "chain-like" side-to-side assembly, regardless of aspect ratio. In contrast, core-shell ellipsoids transition from "flower-like" tip-to-tip to "chain-like" side-to-side arrangements as their aspect ratios increase. The critical aspect ratio for transitioning between these structures increases with shell-to-core ratios. Our experimental findings are corroborated by theoretical calculations and Monte Carlo simulations, which map out the phase diagram of thermodynamically preferred self-assembly structures for core-shell ellipsoids as a function of aspect ratio and shell-to-core ratios. This study shows how to program the self-assembly of anisotropic particles by tuning their physicochemical properties, allowing the deterministic realization of distinct structural configurations.
液体界面上核-壳椭圆体的可编程自组装
由于四极毛细管的相互作用,被限制在液体界面上的椭圆形颗粒在流体变形的诱导下表现出复杂的自组装行为。这些相互作用导致颗粒在顶端到顶端或侧面到侧面的配置中相互吸引。然而,控制它们的界面自组装具有挑战性,因为很难预测这两种状态中哪一种更受青睐。在本研究中,我们证明了在硬椭圆形粒子周围引入软壳可以控制自组装过程,从而在这两种状态之间切换首选配置。我们对它们的界面自组装进行了研究,发现不带外壳的纯椭圆体无论长宽比如何,都能始终如一地形成 "链状 "侧对侧组装。相反,随着长宽比的增加,有核有壳的椭圆体会从 "花状 "的顶端到顶端排列过渡到 "链状 "的侧面到侧面排列。在这些结构之间过渡的临界长宽比随着壳对壳长宽比的增加而增加。我们的实验结果得到了理论计算和蒙特卡罗模拟的证实,这些计算和模拟绘制出了核壳椭圆体的热力学优选自组装结构相图,它是高宽比和壳核比的函数。这项研究展示了如何通过调整各向异性粒子的物理化学特性来对其自组装进行编程,从而确定性地实现不同的结构构型。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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