The role of collective motion in examples of coarsening and self-assembly.

The role of collective motion in examples of coarsening and self-assembly.
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DOI:
10.1039/b810031d
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发表时间:
2009-03-21
期刊:
影响因子:
3.4
通讯作者:
Geissler PL
Geissler PL
中科院分区:
化学2区
文献类型:
--
作者:
Whitelam S;Feng EH;Hagan MF;Geissler PL

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从其组成部分构建图案化结构的最简单处方是将粒子添加到适当的模板中,一次一个。然而,自然界中的自组织分子和胶体系统可以以更加分层的方式进化。具体地,成分(或成分的集群)可以聚集以形成集群(或集群的集群),其用作组装的后续阶段的构建块。在这里,我们评估的性质和后果,这种集体运动在一组原型组装过程。我们这样做使用计算机模拟,其中系统的能力,层次动态可以系统地控制。通过明确地允许或抑制集体运动,我们量化了它的影响。我们发现,二维有吸引力的晶格气(以及类似的三维非晶格模型)内的粗化在很大的温度和密度范围内自然由集体运动主导。在这种情况下,集团的流动性抑制发展的均匀共存相,特别是当宏观偏析是强烈的热力学青睐。相比之下,模型病毒衣壳的组装并没有受到阻碍,而是通过集体移动来促进,这促进了由几个单体组成的中间体的有序结合。
The simplest prescription for building a patterned structure from its constituents is to add particles, one at a time, to an appropriate template. However, self-organizing molecular and colloidal systems in nature can evolve in much more hierarchical ways. Specifically, constituents (or clusters of constituents) may aggregate to form clusters (or clusters of clusters) that serve as building blocks for later stages of assembly. Here we evaluate the character and consequences of such collective motion in a set of prototypical assembly processes. We do so using computer simulations in which a system's capacity for hierarchical dynamics can be controlled systematically. By explicitly allowing or suppressing collective motion, we quantify its effects. We find that coarsening within a two dimensional attractive lattice gas (and an analogous off-lattice model in three dimensions) is naturally dominated by collective motion over a broad range of temperatures and densities. Under such circumstances, cluster mobility inhibits the development of uniform coexisting phases, especially when macroscopic segregation is strongly favored by thermodynamics. By contrast, the assembly of model viral capsids is not frustrated but is instead facilitated by collective moves, which promote the orderly binding of intermediates consisting of several monomers.
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