Directing the self-assembly of block copolymers into a metastable complex network phase via a deep and rapid quench.
Directing the self-assembly of block copolymers into a metastable complex network phase via a deep and rapid quench.
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DOI：
10.1103/physrevlett.111.267801
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发表时间：
2013-12
影响因子：
8.6
通讯作者：
M. Müller;De-Wen Sun
中科院分区：
文献类型：
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作者：
M. Müller;De-Wen Sun
自组装嵌段共聚物系统的自由能景观的特点是由大量的亚稳极小值。使用基于粒子的模拟软，粗粒度的模型，我们探索的机会，可重复地直接自发订购这些自组装系统到一个亚稳态复杂的网络形态-特别是，Schoen的I-WP周期性最小表面-从一个高度不稳定的状态，是由快速膨胀产生的。这种过程导向的自组装提供了一种替代微调分子结构或混合制造复杂的网络结构。比较我们的粒子为基础的模拟结果，最近开发的自由能技术，我们严格评估其预测自发形成的能力，并强调在起始状态和局部密度守恒的非平衡分子构象的重要性。
The free-energy landscape of self-assembling block copolymer systems is characterized by a multitude of metastable minima. Using particle-based simulations of a soft, coarse-grained model, we explore opportunities to reproducibly direct the spontaneous ordering of these self-assembling systems into a metastable complex network morphology--specifically, Schoen's I-WP periodic minimal surface--starting from a highly unstable state that is generated by a rapid expansion. This process-directed self-assembly provides an alternative to fine-tuning molecular architecture or blending for fabricating complex network structures. Comparing our particle-based simulation results to recently developed free-energy techniques, we critically assess their ability to predict spontaneous formation and highlight the importance of nonequilibrium molecular conformations in the starting state and the local conservation of density.