Mahynski Nathan A, Mao Runfang, Pretti Evan, Shen Vincent K, Mittal Jeetain
Chemical Sciences Division, National Institute of Standards and Technology, Gaithersburg, Maryland 20899-8320, USA.
Department of Chemical and Biomolecular Engineering, Lehigh University, 111 Research Dr., Bethlehem, Pennsylvania 18015-4791, USA.
Soft Matter. 2020 Apr 1;16(13):3187-3194. doi: 10.1039/c9sm02426c.
Inverse design methods are powerful computational approaches for creating colloidal systems which self-assemble into a target morphology by reverse engineering the Hamiltonian of the system. Despite this, these optimization procedures tend to yield Hamiltonians which are too complex to be experimentally realized. An alternative route to complex structures involves the use of several different components, however, conventional inverse design methods do not explicitly account for the possibility of phase separation into compositionally distinct structures. Here, we present an inverse design scheme for multicomponent colloidal systems by combining active learning with a method to directly compute their ground state phase diagrams. This explicitly accounts for phase separation and can locate stable regions of Hamiltonian parameter space which grid-based surveys are prone to miss. Using this we design low-density, binary structures with Lennard-Jones-like pairwise interactions that are simpler than in the single component case and potentially realizable in an experimental setting. This reinforces the concept that ground states of simple, multicomponent systems might be rich with previously unappreciated diversity, enabling the assembly of non-trivial structures with only few simple components instead of a single complex one.
逆设计方法是用于创建胶体系统的强大计算方法，该方法通过对系统的哈密顿量进行逆向工程，使胶体系统自组装成目标形态。尽管如此，这些优化程序往往会产生过于复杂而无法通过实验实现的哈密顿量。构建复杂结构的另一种途径涉及使用几种不同的组分，然而，传统的逆设计方法并未明确考虑相分离成组成不同结构的可能性。在此，我们通过将主动学习与直接计算其基态相图的方法相结合，提出了一种用于多组分胶体系统的逆设计方案。这明确考虑了相分离，并能够定位基于网格的调查容易遗漏的哈密顿量参数空间的稳定区域。利用这一方法，我们设计了具有类似 Lennard-Jones 对相互作用的低密度二元结构，这些结构比单一组分情况下的结构更简单，并且有可能在实验环境中实现。这强化了这样一个概念，即简单多组分系统的基态可能具有丰富的、以前未被认识到的多样性，从而能够仅用少数简单组分而非单个复杂组分来组装非平凡结构。
