Department of Bioengineering, California Institute of Technology, Pasadena, California 91125, USA.
Department of Biology, California Institute of Technology, Pasadena, California 91125, USA.
Nat Nanotechnol. 2017 Mar;12(3):251-259. doi: 10.1038/nnano.2016.256. Epub 2016 Nov 28.
Scaling up the complexity and diversity of synthetic molecular structures will require strategies that exploit the inherent stochasticity of molecular systems in a controlled fashion. Here we demonstrate a framework for programming random DNA tilings and show how to control the properties of global patterns through simple, local rules. We constructed three general forms of planar network-random loops, mazes and trees-on the surface of self-assembled DNA origami arrays on the micrometre scale with nanometre resolution. Using simple molecular building blocks and robust experimental conditions, we demonstrate control of a wide range of properties of the random networks, including the branching rules, the growth directions, the proximity between adjacent networks and the size distribution. Much as combinatorial approaches for generating random one-dimensional chains of polymers have been used to revolutionize chemical synthesis and the selection of functional nucleic acids, our strategy extends these principles to random two-dimensional networks of molecules and creates new opportunities for fabricating more complex molecular devices that are organized by DNA nanostructures.
要提高合成分子结构的复杂性和多样性，就需要采用能够以可控方式利用分子系统固有随机性的策略。在这里，我们展示了一种用于对随机 DNA 平铺结构进行编程的框架，并展示了如何通过简单的局部规则来控制全局图案的属性。我们在微尺度的自组装 DNA 折纸阵列表面构建了三种通用形式的平面网络——随机环、迷宫和树，其分辨率达到纳米级。使用简单的分子构建模块和稳健的实验条件，我们证明了对随机网络的广泛性质的控制，包括分支规则、生长方向、相邻网络之间的接近程度和尺寸分布。就像用于彻底改变化学合成和功能性核酸选择的用于生成聚合物随机一维链的组合方法一样，我们的策略将这些原理扩展到了分子的二维随机网络，并为制造由 DNA 纳米结构组织的更复杂的分子器件创造了新的机会。
