Conformation and dynamics of the ligand shell of a water-soluble Au102 nanoparticle.
Conformation and dynamics of the ligand shell of a water-soluble Au102 nanoparticle.
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DOI：
10.1038/ncomms10401
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发表时间：
2016-01-21
影响因子：
16.6
通讯作者：
Häkkinen H
中科院分区：
文献类型：
--
作者：
Salorinne K;Malola S;Wong OA;Rithner CD;Chen X;Ackerson CJ;Häkkinen H
由有机分子钝化层稳定的无机纳米粒子形成一类多功能纳米结构材料，在材料化学、纳米物理、纳米医学和结构生物学方面具有潜在应用。虽然纳米粒子核心的结构通常以原子精度已知，但获得有机层的精确结构和动力学信息构成了重大挑战。在这里，我们通过结合多维 NMR 方法、密度泛函理论计算和分子动力学模拟，报告了由溶液中的 44 个对巯基苯甲酸配体稳定的水溶性、原子级精确、102 原子金纳米颗粒的所有配体的 1H 和 13C NMR 位移的完整分配。分子动力学模拟通过提供有关配体无序的信息以及最动态配体的可能不同配体构象的可视化来增强数据。这里演示的方法为应用中连接纳米颗粒功能化的可控策略开辟了一条途径。 由有机分子钝化层稳定的无机纳米颗粒的核心结构通常是已知的，但有关有机层的信息很难获得。在这里，作者使用核磁共振和计算方法来探测配体无序并可视化可能的配体构象。
Inorganic nanoparticles, stabilized by a passivating layer of organic molecules, form a versatile class of nanostructured materials with potential applications in material chemistry, nanoscale physics, nanomedicine and structural biology. While the structure of the nanoparticle core is often known to atomic precision, gaining precise structural and dynamical information on the organic layer poses a major challenge. Here we report a full assignment of 1H and 13C NMR shifts to all ligands of a water-soluble, atomically precise, 102-atom gold nanoparticle stabilized by 44 para-mercaptobenzoic acid ligands in solution, by using a combination of multidimensional NMR methods, density functional theory calculations and molecular dynamics simulations. Molecular dynamics simulations augment the data by giving information about the ligand disorder and visualization of possible distinct ligand conformations of the most dynamic ligands. The method demonstrated here opens a way to controllable strategies for functionalization of ligated nanoparticles for applications. The core structure of inorganic nanoparticles, stabilized by a passivating layer of organic molecules, is often known but information about the organic layer is tougher to derive. Here, the authors use NMR and computational methods to probe the ligand disorder and visualize possible ligand conformations.