论文标题

功能性胶体组件的非平衡设计策略

Nonequilibrium design strategies for functional colloidal assemblies

论文作者

Das, Avishek, Limmer, David T.

论文摘要

我们使用非平衡变异原理来优化DNA涂层胶体自组装纳米簇的稳态,剪切诱导的互连。在随机优化算法中采用此原理使我们能够发现功能材料的设计策略。我们发现,远离平衡剪切流量可以通过取消稳定性和平衡中系统所需的反应性之间的权衡来显着增强特定胶体状态之间的通量。对于孤立的纳米簇,我们发现通过将给定反应坐标与背景剪切流耦合来扩大过渡速率的非平衡策略。我们还发现,可以通过耦合构象转变的自由度来选择性地打破详细的平衡和最大化概率电流。对于由许多纳米群体组成的微观相,我们研究了簇之间跳跃的胶体的通量。我们发现,剪切流可以放大磁通量,而无需对微相结构的比例折衷。这种方法提供了一种揭示纳米级,自主,功能材料远离平衡的功能材料的一般手段。

We use a nonequilibrium variational principle to optimize the steady-state, shear-induced interconversion of self-assembled nanoclusters of DNA-coated colloids. Employing this principle within a stochastic optimization algorithm allows us to discover design strategies for functional materials. We find that far-from-equilibrium shear flow can significantly enhance the flux between specific colloidal states by decoupling trade-offs between stability and reactivity required by systems in equilibrium. For isolated nanoclusters, we find nonequilibrium strategies for amplifying transition rates by coupling a given reaction coordinate to the background shear flow. We also find that shear flow can be made to selectively break detailed balance and maximize probability currents by coupling orientational degrees of freedom to conformational transitions. For a microphase consisting of many nanoclusters, we study the flux of colloids hopping between clusters. We find that a shear flow can amplify the flux without a proportional compromise on the microphase structure. This approach provides a general means of uncovering design principles for nanoscale, autonomous, functional materials driven far from equilibrium.

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