ARC Centre of Excellence in Exciton Science and School of Chemistry, Monash University, Clayton, VIC 3800, Australia.
Nanoscale. 2018 Nov 7;10(41):19557-19567. doi: 10.1039/c8nr05509b. Epub 2018 Oct 16.
Developments in DNA nanotechnology offer control of the self-assembly of materials into discrete nanostructures. Within this paradigm, pre-assembled DNA origami with hundreds of DNA strands allows for precise and programmable spatial positioning of functionalised nanoparticles. We propose an alternative approach to construct multiple, structurally different, nanoparticle assemblies from just a few complementary nanoparticle-functionalised DNA strands. The approach exploits local minima in the potential energy landscape of hybridised nanoparticle-DNA structures by employing kinetic control of the assembly. Using a four-strand DNA template, we synthesise five different 3D gold nanoparticle (plasmonic) tetrameric isomers, akin to molecular structural isomers. The number of different structures formed using this approach for a set of DNA strands represents a combinatorial library, which we summarise in a hybridisation pathway tree and use to achieve deposition of tetrahedral assemblies onto substrates in high yield. The ability to program nanoparticle self-assembly pathways gives unprecedented access to unique plasmonic nanostructures.
DNA 纳米技术的发展为控制材料自组装成离散的纳米结构提供了可能。在这个范例中，使用数百条 DNA 链预先组装的 DNA 折纸术可以实现功能化纳米粒子的精确和可编程的空间定位。我们提出了一种替代方法，可以仅使用少数几个互补的纳米粒子功能化 DNA 链来构建多个结构不同的纳米粒子组装体。该方法通过利用杂交纳米粒子-DNA 结构的势能景观中的局部极小值来实现组装的动力学控制。我们使用一个四链 DNA 模板，合成了五个不同的三维金纳米粒子（等离子体）四聚体异构体，类似于分子结构异构体。使用这种方法，一组 DNA 链可以形成的不同结构的数量代表一个组合文库，我们将其总结在一个杂交途径树中，并用于实现四面体组装体在基底上的高产量沉积。对纳米粒子自组装途径进行编程的能力为独特的等离子体纳米结构提供了前所未有的途径。
