Abstract Recently, DNA has emerged as a designer material for the controlled assembly of nanoparticles. The unique programmability of Watson-Crick base pairing offers limitless control over assembly via specific interactions. At the same time, reliance on non-specific interactions, such as layer-by-layer (LbL) assembly offers a simple assembly method, albeit with limited control. Here, by assembling DNA-capped gold nanoparticles in a LbL fashion we combine these two approaches and present a simple and robust method to construct large-scale three-dimensional nanoparticle assemblies with readily tunable plasmonics. Through variation of the DNA ligand and the nanoparticle core size the morphology of the three-dimensional nanoparticle assemblies was carefully adjusted. These morphological changes, confirmed using grazing incidence x-ray scattering, enabled the tuning of the plasmonic behavior of the three-dimensional nanoparticle assemblies. The morphology could also be modified in real-time through water vapor induced swelling enabling dynamic tuning of the optical properties. The introduction of the DNA ligand to the LbL assembly method presented here imparted tunability to the process previously inaccessible with other nanoparticle ligands and presents a platform with which to create optically active materials of various compositions.

中文翻译：

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通过逐层工艺具有可调等离子体的三维纳米粒子组件

摘要 最近，DNA 已成为纳米粒子受控组装的设计材料。Watson-Crick 碱基配对的独特可编程性通过特定交互提供对组装的无限控制。同时，对非特定交互的依赖，例如逐层 (LbL) 组装提供了一种简单的组装方法，尽管控制有限。在这里，通过以 LbL 方式组装 DNA 加帽的金纳米粒子，我们将这两种方法结合起来，并提出了一种简单而可靠的方法来构建具有易于调节的等离子体激元的大规模三维纳米粒子组件。通过改变 DNA 配体和纳米颗粒核心尺寸，仔细调整三维纳米颗粒组件的形态。这些形态变化，使用掠入射 X 射线散射证实，能够调整三维纳米粒子组件的等离子体行为。还可以通过水蒸气诱导的膨胀实时修改形态，从而实现光学特性的动态调整。将 DNA 配体引入这里介绍的 LbL 组装方法，赋予了以前其他纳米粒子配体无法实现的过程的可调性，并提供了一个平台，用于创建各种成分的光学活性材料。