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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Atomically precise gold nanocrystal molecules with surface plasmon resonance
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Atomically precise gold nanocrystal molecules with surface plasmon resonance

机译：具有表面等离子体共振的原子精确的金纳米晶体分子

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Since Faraday's pioneering work on gold colloids, tremendous scientific research on plasmonic gold nanoparticles has been carried out, but no atomically precise Au nanocrystals have been achieved. This work reports the first example of gold nanocrystal molecules. Mass spectrometry analysis has determined its formula to be Au_(333)(SR)_(79) (R = CH_2CH_2Ph). This magic sized nanocrystal molecule exhibits fcc-crystallinity and surface plasmon resonance at approximately 520 nm, hence, a metallic nanomolecule. Simulations have revealed that atomic shell closing largely contributes to the particular robustness of Au33_3(SR)_(79), albeit the number of free electrons (i.e., 333 - 79 = 254) is also consistent with electron shell closing based on calculations using a confined free electron model. Guided by the atomic shell closing growth mode, we have also found the next larger size of extraordinarily stability to be Au_(~530)(SR)_(~100) after a size-focusing selection—which selects the robust size available in the starting polydisperse nanoparticles. This work clearly demonstrates that atomically precise nanocrystal molecules are achievable and that the factor of atomic shell closing contributes to their extraordinary stability compared to other sizes. Overall, this work opens up new opportunities for investigating many fundamental issues of nanocrystals, such as the formation of metallic state, and will have potential impact on condensed matter physics, nanochemistry, and catalysis as well.
机译：自从法拉第（Faraday）在金胶体方面的开创性工作以来，已经对等离激元金纳米粒子进行了大量科学研究，但没有获得原子上精确的金纳米晶体。这项工作报告了金纳米晶体分子的第一个例子。质谱分析已确定其公式为Au_（333）（SR）_（79）（R = CH_2CH_2Ph）。这种神奇大小的纳米晶体分子在大约520 nm处显示出fcc结晶度和表面等离振子共振，因此是金属纳米分子。模拟表明，原子壳的闭合在很大程度上有助于Au33_3（SR）_（79）的特定鲁棒性，尽管自由电子的数量（即333-79 = 254）也与基于使用a的计算得出的电子壳的闭合一致受限自由电子模型。在原子壳闭合增长模式的指导下，我们还发现在进行尺寸聚焦选择后，下一个更大的异常稳定尺寸将为Au_（〜530）（SR）_（〜100），该尺寸选择了起始多分散纳米粒子。这项工作清楚地证明了原子精确的纳米晶体分子是可以实现的，并且与其他尺寸相比，原子壳封闭的因素有助于其非凡的稳定性。总的来说，这项工作为研究纳米晶体的许多基本问题（例如金属态的形成）开辟了新的机会，并将对凝聚态物理，纳米化学和催化产生潜在影响。

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