论文标题
水二聚体驱动的DNA碱基上层建筑,氢键不匹配
Water dimer driven DNA base superstructure with mismatched hydrogen-bonding
论文作者
论文摘要
最近的研究表明,在室温下及其异常特性在平衡水蒸气中存在水二聚体,这表明水二聚体在实验和理论中的基准作用。但是,由于单分子水平的水分离和产生的挑战,人们对单个水二聚体的观察有限。在这里,我们实现了嵌入DNA碱(腺嘌呤的自组装层)内的单个限制水二聚体的真实空间成像(111)。这些水二聚体对腺嘌呤层的水合会导致局部表面手性反转,以使水合后相邻的同型腺嘌呤分子在邻近腺嘌呤分子之间导致不匹配的氢键模式。此外,理论模拟和计算证实了腺嘌呤上层建筑与这些动态约束水二聚体之间的相互影响。对单一狭窄水二聚体的观察提供了一种前所未有的方法,用于研究水簇的基本形式及其与当地化学环境的相互作用。
The existence of water dimers in equilibrium water vapor at room temperature and their anomalous properties revealed by recent studies suggest the benchmark role of water dimer in both experiment and theory. However, there has been a limited observation of individual water dimers due to the challenge of water separation and generation at the single-molecule level. Here, we achieve real-space imaging of individual confined water dimers embedded inside self-assembled layer of a DNA base, adenine, on Ag(111). The hydration of the adenine layers by these water dimers causes a local surface chiral inversion in a way that the neighboring homochiral adenine molecules become heterochiral after hydration, resulting in a mismatched hydrogen-bond pattern between neighboring adenine molecules. Furthermore, the mutual influence between the adenine superstructure and these dynamic confined water dimers is corroborated by theoretical simulation and calculations. The observation of single confined water dimers offers an unprecedented approach to studying the fundamental forms of water clusters and their interaction with the local chemical environment.