论文标题
通过可编程折叠进行自组装
Self-assembly Through Programmable Folding
论文作者
论文摘要
在材料科学的最前沿,物质旨在自组织成各种功能的结构。在过去的二十年中,在构建基块的多功能性方面见证了重大创新,从纳米级的DNA到宏观上的握手材料。就像拼图拼图一样,如果所有碎片都不同,则可以可靠地自组装任意结构,但是到目前为止,构建块的风味较少的系统仅限于外来晶体的组装。受到自然将生物聚合物折叠成特定RNA和蛋白质结构的策略的启发,我们在这里引入了具有可编程DNA相互作用的胶体聚合物的最小模型系统,该模型将其下坡折叠成二维几何形状。结合了实验,模拟和理论,我们表明,设计相互作用的顺序直接折叠为称为foldamers的唯一几何形状。多达13滴的最简单的交替序列($ abab $ ...)产生了11个折叠剂,同时设计序列并添加了额外的风味,唯一地编码了619个可能的几何形状中的一半以上。这些折叠剂可以进一步相互作用,以制造复杂的上乳状结构,从而播种下一代生物启发的材料。我们的结果与动力学无关,因此适用于在各个长度上具有分层相互作用的聚合物材料,从有机分子一直到Rubik的蛇。
At the cutting edge of materials science, matter is designed to self-organize into structures that perform a wide range of functions. The past two decades have witnessed major innovations in the versatility of building blocks, ranging from DNA on the nanoscale to handshaking materials on the macroscale. Like a jigsaw puzzle, one can reliably self-assemble arbitrary structures if all the pieces are distinct, but systems with fewer flavors of building blocks have so far been limited to the assembly of exotic crystals. Inspired by Nature's strategy of folding biopolymers into specific RNA and protein structures, here we introduce a minimal model system of colloidal polymers with programmable DNA interactions that guide their downhill folding into two-dimensional geometries. Combining experiments, simulations, and theory, we show that designing the order in which interactions are switched on directs folding into unique geometries called foldamers. The simplest alternating sequences ($ABAB$...) of up to 13 droplets yield eleven foldamers, while designing the sequence and adding an extra flavor uniquely encodes more than half of the 619 possible geometries. These foldamers can further interact to make complex supracolloidal architectures, seeding a next generation of bio-inspired materials. Our results are independent of the dynamics and therefore apply to polymeric materials with hierarchical interactions on all length scales, from organic molecules all the way to Rubik's snakes.