论文标题
非平衡胶体组件的变分设计原理
Variational design principles for nonequilibrium colloidal assembly
论文作者
论文摘要
使用大偏差理论和随机最佳控制的原理，我们表明，稀有的分子动力学轨迹以组装特定的目标结构编码一组相互作用和外部力，从而导致该结构的稳定性增强。这种关系可以被提出为变分原理，为此，我们开发了相关的优化算法，并使用它来确定非平衡稳态内有针对性自组装的最佳力量。我们在线性剪切流中的胶体群集组件模型中说明了有关反设计的这一观点。我们发现，胶体簇可以使用可调复杂性的特定短距离相互作用来组装高产量。剪切可降低刚性簇的产量，而少量剪切值会增加非凝聚簇的产量。通过广义线性响应理论合理化了剪切产量的增强或抑制。通过研究由6、7或8个颗粒制成的21个独特的簇，我们从平衡中发现了针对靶向组装的基本设计原理。
Using large deviation theory and principles of stochastic optimal control, we show that rare molecular dynamics trajectories conditioned on assembling a specific target structure encode a set of interactions and external forces that lead to enhanced stability of that structure. Such a relationship can be formulated into a variational principle, for which we have developed an associated optimization algorithm and have used it to determine optimal forces for targeted self-assembly within nonequilibrium steady-states. We illustrate this perspective on inverse design in a model of colloidal cluster assembly within linear shear flow. We find that colloidal clusters can be assembled with high yield using specific short-range interactions of tunable complexity. Shear decreases the yields of rigid clusters, while small values of shear increase the yields of nonrigid clusters. The enhancement or suppression of the yield due to shear is rationalized with a generalized linear response theory. By studying 21 unique clusters made of 6, 7 or 8 particles, we uncover basic design principles for targeted assembly out of equilibrium.
