First-Principles Computational Visualization of Localized Surface Plasmon Resonance in Gold Nanoclusters
First-Principles Computational Visualization of Localized Surface Plasmon Resonance in Gold Nanoclusters
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DOI：
10.1021/jp5088042
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发表时间：
2014-11-27
影响因子：
2.9
通讯作者：
Nobusada, Katsuyuki
中科院分区：
文献类型：
--
作者：
Iida, Kenji;Noda, Masashi;Nobusada, Katsuyuki
利用我们最近开发的纳米结构中光致电子动力学的第一性原理计算程序，研究了Aun纳米团簇（n = 54，146，308，560，922，1414）的局域表面等离子体共振（LSPR）随尺寸的变化. Au-1414的尺寸（直径3.9 nm）与先前纳米团簇中光学响应的第一性原理计算中所解决的尺寸相比是空前大的。这些计算使我们能够清楚地看到，LSPR逐渐增长和LSPR峰红移随着集群大小的增加。在真实的空间中观察到了LSPR的生长，表明电子电荷分布在团簇的最外表面区域以集体的方式振荡。我们进一步说明，核心d电子屏蔽集体振荡的导电类s电子。
Cluster-size dependence of localized surface plasmon resonance (LSPR) for Aun nanoclusters (n = 54, 146, 308, 560, 922, 1414) is investigated by using our recently developed computational program of first-principles calculations for photoinduced electron dynamics in nanostructures. The size of Au-1414 (3.9 nm in diameter) is unprecedentedly large in comparison with those addressed in previous first-principles calculations of optical response in nanoclusters. These computations enable us to clearly see that LSPR gradually grows and the LSPR peaks red shift with increasing cluster size. The growth of LSPR is visualized in real space, demonstrating that electron charge distributions oscillate in a collective manner around the outermost surface region of the clusters. We further illustrate that the core d electrons screen the collective oscillation of the conduction-like s electrons.