几何受挫组装的分散、凝聚与自限制状态
Dispersed, condensed and self-limiting states of geometrically frustrated assembly
AI总结：
该研究提出一个通用的最小化几何受挫组装模型，通过模拟和连续介质理论分析其热力学，发现有限温度下自限制状态在中等受挫时稳定，且其相边界受温度控制，凸显了平移熵和构象熵的关键作用。
摘要：
在自组装系统中，几何受挫会导致以形状错配的内部梯度为特征的复杂状态。受挫组装近期引起了关注，因为其热力学有可能感知并选择远大于组成构件或其相互作用的组装体有限尺寸。目前，自限制主要被理解为源于零温条件，具体是内聚力与受挫的尺度依赖弹性成本之间的竞争。尽管熵和有限温度涨落效应必然对自组装系统具有重要意义，但它们对受挫组装的自限制状态的影响尚不明确。我们引入了一个通用的、最小化的受挫组装模型，并通过模拟和连续介质理论确立了其依赖于有限温度和浓度的热力学。相图表现为三种不同的平移有序状态：分散气相；充满缺陷的凝聚体；以及自限制聚集态。我们证明，在有限温度下，自限制状态在中等程度的受挫下是稳定的。此外，与主流观点相反，其与宏观分散态和体相态之间的热力学边界受温度控制，这表明平移熵和构象熵在其形成中具有至关重要的作用。
英文摘要：
In self-assembling systems, geometric frustration leads to complex states characterized by internal gradients of shape misfit. Frustrated assemblies have drawn recent interest due to the unique possibility that their thermodynamics can sense and select the finite size of assembly at length scales much larger than constituent building blocks or their interactions. At present, self-limitation is chiefly understood to derive from zero-temperature considerations, specifically the competition between cohesion and scale-dependent elastic costs of frustration. While effects of entropy and finite temperature fluctuations are necessarily significant for self-assembling systems, their impact on the self-limiting states of frustrated assemblies is not known. We introduce a generic, minimal model of frustrated assembly, and establish its finite-temperature and concentration dependent thermodynamics by way of simulation and continuum theory. The phase diagram is marked by three distinct states of translation order: a dispersed vapor; a defect-riddled condensate; and the self-limiting aggregate state. We show that, at finite temperature, the self-limiting state is stable at intermediate frustration. Further, in contrast to the prevailing picture, its thermodynamic boundaries with the macroscopic disperse and bulk states are temperature controlled, pointing to the essential importance of translational and conformational entropy in their formation.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
