Building blocks of non-Euclidean ribbons: size-controlled self-assembly via discrete frustrated particles
Building blocks of non-Euclidean ribbons: size-controlled self-assembly via discrete frustrated particles
复制标题
非欧几里得带的构建块：通过离散受挫粒子进行尺寸控制的自组装
DOI：
10.1039/d2sm01371a
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发表时间：
2023
期刊：
影响因子：
3.4
通讯作者：
Grason, Gregory M.
中科院分区：
文献类型：
--
作者：
Hall, Douglas M.;Stevens, Mark J.;Grason, Gregory M.
几何挫折提供了一种具有可控有限尺寸的软物质自组装途径。虽然对软物质组装挫败的理解几乎完全来自连续弹性描述，但当前的挑战是理解失配“构件”的微观物理特性与中尺度的紧急组装行为之间的联系。我们提出并分析了基于粒子的描述，该描述可以说是受挫软物质组装、负曲率带状组装的最佳研究示例，在手性表面活性剂和形状受挫纳米颗粒的组装中观察到。基于我们的粒子模型（称为鞍楔单体），我们对微观形状和失配亚基相互作用之间的联系以及超粒子尺度的涌现行为进行了数值测试，特别关注粒子间应变的传播和弛豫、受挫带上外在形状的涌现作用以及有限宽度选择的平衡机制。除了形状失配的直观作用之外，我们还表明，自我限制严重依赖于内聚相互作用的有限范围，较大尺寸的有限组件需要增加短程粒子间力。此外，我们证明，由于形状扁平组装中的应变软化和高应变键的部分屈服，离散粒子相互作用产生的非线性会改变自限行为，这反过来可能会引起分层、多域组装的状态。追踪受阻限制组装的机制到失配颗粒形状和相互作用的特定微观特征，为将尺寸可编程组装理论转化为有意受阻胶体颗粒的设计提供了必要的指导。
Geometric frustration offers a pathway to soft matter self-assembly with controllable finite sizes. While the understanding of frustration in soft matter assembly derives almost exclusively from continuum elastic descriptions, a current challenge is to understand the connection between microscopic physical properties of misfitting “building blocks” and emergent assembly behavior at the mesoscale. We present and analyze a particle-based description of what is arguably the best studied example for frustrated soft matter assembly, negative-curvature ribbon assembly, observed in both assemblies of chiral surfactants and shape-frustrated nanoparticles. Based on our particle model, known as saddle wedge monomers, we numerically test the connection between microscopic shape and interactions of the misfitting subunits and the emergent behavior at the supra-particle scale, specifically focussing on the propagation and relaxation of inter-particle strains, the emergent role of extrinsic shape on frustrated ribbons and the equilibrium regime of finite width selection. Beyond the intuitive role of shape misfit, we show that self-limitation is critically dependent on the finite range of cohesive interactions, with larger size finite assemblies requiring increasing short-range interparticle forces. Additionally, we demonstrate that non-linearities arising from discrete particle interactions alter self-limiting behavior due to both strain-softening in shape-flattened assembly and partial yielding of highly strained bonds, which in turn may give rise to states of hierarchical, multidomain assembly. Tracing the regimes of frustration-limited assembly to the specific microscopic features of misfitting particle shapes and interactions provides necessary guidance for translating the theory of size-programmable assembly into design of intentionally-frustrated colloidal particles.