arXivDaily arXiv每日学术速递 周一至周五更新
arXiv 2210.08396cond-mat.softcond-mat.mtrl-scicond-mat.stat-mech
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非欧几里得带状结构的构建基块:通过离散的、受挫颗粒实现尺寸可控的自组装

Building blocks of non-Euclidean ribbons: Size-controlled self-assembly via discrete, frustrated particles

Douglas M. Hall, Mark J. Stevens, Gregory M. Grason

AI总结:

研究通过颗粒模型分析负曲率带状组装中微观形状与介观行为的联系,发现自限制依赖有限内聚相互作用范围且离散非线性可引发多畴组装,为尺寸可编程胶体颗粒设计提供指导。

摘要:

几何受挫为具有可控有限尺寸的软物质自组装提供了一条途径。尽管对软物质组装中受挫的理解几乎完全源自连续介质弹性描述,但当前的挑战是理解不匹配“构建基块”的微观物理性质与介观尺度上涌现的组装行为之间的联系。我们提出并分析了一种基于颗粒的描述,针对可以说是受挫软物质组装中研究最充分的例子——负曲率带状组装,该现象在手性表面活性剂和形状受挫纳米颗粒的组装中均被观察到。基于我们的颗粒模型(即鞍形楔形单体),我们在数值上测试了不匹配亚基的微观形状和相互作用与超颗粒尺度上涌现行为之间的联系,特别关注颗粒间应变的传播与弛豫、外在形状对受挫带状结构的涌现作用以及有限宽度选择的平衡区域。除了形状不匹配的直观作用外,我们表明自限制关键依赖于内聚相互作用的有限范围,更大尺寸的有限组装需要逐渐增强的短程颗粒间作用力。此外,我们证明由离散颗粒相互作用引起的非线性改变了自限制行为,这既源于形状扁平化组装中的应变软化,也源于高应变键的部分屈服,这反过来可能引发分层、多畴组装状态。将受挫限制组装的区域追溯到不匹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挫胶体颗粒的设计提供了必要指导。

英文摘要:

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 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 {\it 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 focusing 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.

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