标题： DNA包覆胶体结晶中非特异性相互作用的被低估的作用 显示英文标题

标题： The underappreciated role of nonspecific interactions in the crystallization of DNA-coated colloids

摘要： 在过去十年中，可编程自组装领域出现了大量可以从DNA涂层的纳米级和微米级胶体粒子中合成的晶体晶格。普遍的观点是，通过设计DNA介导的相互作用来实现特定粒子对之间的结合，并通过粒子直径来控制各种物种的排列，可以针对特定的晶体结构。在本文中，我们表明其他普遍存在的非特异性相互作用在决定不同晶体多形体的相对稳定性方面同样起着重要作用，因此决定了实验中最可能形成的晶体结构。对于一种相同尺寸的DNA涂层胶体微米级粒子的二元混合物，我们展示了改变非特异性立体和范德华相互作用的大小如何产生一系列二元体心四角晶体，包括铯氯化物和铜金晶体。使用考虑这些相互作用的对势进行的模拟定量地再现了我们的实验观察结果，一个理论模型揭示了特异性与非特异性力之间微妙的平衡如何决定平衡晶体结构。这些结果突显了在晶体工程设计过程中考虑非特异性相互作用的重要性。 显示英文摘要

摘要： Over the last decade, the field of programmable self-assembly has seen an explosion in the diversity of crystal lattices that can be synthesized from DNA-coated colloidal nanometer- and micrometer-scale particles. The prevailing wisdom has been that a particular crystal structure can be targeted by designing the DNA-mediated interactions, to enforce binding between specific particle pairs, and the particle diameters, to control the packing of the various species. In this article, we show that other ubiquitous nonspecific interactions can play equally important roles in determining the relative stability of different crystal polymorphs and therefore what crystal structure is most likely to form in an experiment. For a binary mixture of same-sized DNA-coated colloidal micrometer-scale particles, we show how changing the magnitudes of nonspecific steric and van der Waals interactions gives rise to a family of binary body-centered tetragonal crystals, including both cesium-chloride and copper-gold crystals. Simulations using pair potentials that account for these interactions reproduce our experimental observations quantitatively, and a theoretical model reveals how a subtle balance between specific and nonspecific forces determines the equilibrium crystal structure. These results highlight the importance of accounting for nonspecific interactions in the crystal-engineering design process.