Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
Nat Nanotechnol. 2010 Feb;5(2):116-20. doi: 10.1038/nnano.2009.378. Epub 2009 Dec 20.
Nanoscale components can be self-assembled into static three-dimensional structures, arrays and clusters using biomolecular motifs. The structural plasticity of biomolecules and the reversibility of their interactions can also be used to make nanostructures that are dynamic, reconfigurable and responsive. DNA has emerged as an ideal biomolecular motif for making such nanostructures, partly because its versatile morphology permits in situ conformational changes using molecular stimuli. This has allowed DNA nanostructures to exhibit reconfigurable topologies and mechanical movement. Recently, researchers have begun to translate this approach to nanoparticle interfaces, where, for example, the distances between nanoparticles can be modulated, resulting in a distance-dependent plasmonic response. Here, we report the assembly of nanoparticles into three-dimensional superlattices and dimer clusters, using a reconfigurable DNA device that acts as an interparticle linkage. The interparticle distances in the superlattices and clusters can be modified, while preserving structural integrity, by adding molecular stimuli (simple DNA strands) after the self-assembly processes has been completed. Both systems were found to switch between two distinct rigid states, but a transition to a flexible device configuration within a superlattice showed a significant hysteresis.
纳米级组件可以使用生物分子基元自组装成静态的三维结构、阵列和团簇。生物分子的结构可塑性及其相互作用的可逆性也可用于制造动态、可重构和响应的纳米结构。DNA 已成为制造此类纳米结构的理想生物分子基元，部分原因是其多功能的形态允许使用分子刺激原位进行构象变化。这使得 DNA 纳米结构能够表现出可重构的拓扑结构和机械运动。最近，研究人员开始将这种方法转化为纳米粒子界面，例如，可以调节纳米粒子之间的距离，从而导致依赖于距离的等离子体响应。在这里，我们报告了使用可重构 DNA 器件（作为粒子间连接）将纳米粒子组装成三维超晶格和二聚体簇。通过在自组装过程完成后添加分子刺激（简单的 DNA 链），可以在不破坏结构完整性的情况下，修改超晶格和簇中的粒子间距离。这两个系统都被发现可以在两种不同的刚性状态之间切换，但是在超晶格中向柔性器件配置的转变显示出明显的滞后。
