Department of Chemistry and Nanoscience, Ewha Womans University, 52 Ewhayeodae-gil, Seodaemun-gu, Seoul 03760, Korea.
Nano Lett. 2024 Feb 28;24(8):2574-2580. doi: 10.1021/acs.nanolett.3c04637. Epub 2024 Feb 13.
The highly programmable and responsive molecular recognition properties of DNA provide unparalleled opportunities for fabricating dynamic nanostructures capable of structural transformation in response to various external stimuli. However, they typically operate in tightly controlled environments because certain conditions (ionic strength, pH, temperature, etc.) must be met for DNA duplex formation. In this study, we adopted site-specific enzymatic ligation and DNA-based layer-by-layer thin film fabrication to build shape-morphing DNA-linked nanoparticle films operational in a broad range of environments. The ligated films remained intact in unusual conditions such as pure water and high temperature causing dissociation of DNA duplexes and showed predictable and reversible shape morphing in response to various environmental changes and DNA exchange reactions. Furthermore, domain-selective ligation combined with photoinduced interlayer mixing allowed for the fabrication of unusual edge-sealed double-layered films through midlayer etching, which is difficult to realize by other methods.
DNA 具有高度可编程和响应性的分子识别特性，为制造能够响应各种外部刺激进行结构转变的动态纳米结构提供了无与伦比的机会。然而，它们通常在严格控制的环境中运行，因为形成 DNA 双链需要满足某些条件（离子强度、pH 值、温度等）。在这项研究中，我们采用定点酶连接和基于 DNA 的层层薄膜制造技术，构建了在广泛的环境中运行的形态变形 DNA 连接纳米粒子薄膜。在导致 DNA 双链解离的异常条件下（如纯水和高温），连接的薄膜仍然保持完整，并对各种环境变化和 DNA 交换反应表现出可预测和可逆的形态变形。此外，通过层间混合的光诱导，结合域选择性连接，允许通过中层刻蚀制造不常见的边缘密封双层薄膜，这是其他方法难以实现的。
