The Origin of the Photoluminescence Enhancement of Gold-Doped Silver Nanoclusters: The Importance of Relativistic Effects and Heteronuclear Gold-Silver Bonds.
The Origin of the Photoluminescence Enhancement of Gold-Doped Silver Nanoclusters: The Importance of Relativistic Effects and Heteronuclear Gold-Silver Bonds.
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DOI：
10.1002/anie.201803683
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发表时间：
2018-07
影响因子：
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通讯作者：
Xiaoxiang Xie;Pin Xiao;Xiaoyan Cao;W. Fang;G. Cui;M. Dolg
中科院分区：
文献类型：
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作者：
Xiaoxiang Xie;Pin Xiao;Xiaoyan Cao;W. Fang;G. Cui;M. Dolg
银纳米团簇的弱光致发光阻碍了其作为发光纳米材料的广泛应用。然而，最近的实验表明，金掺杂可以显着增强Ag 29纳米团簇的光致发光强度，但这种效应的分子和物理起源仍然未知。因此，我们已经计算探索的几何和电子结构的Ag 29和金掺杂的Ag 29-x Aux（x=1-5）纳米团簇在S 0和S1状态。结果表明：1）相对论效应对荧光强度的增强起着重要作用，主要是由于Au原子引起的; 2）异质Au-Ag键的存在可以增加这些金掺杂纳米团簇的稳定性，并调节其同分异构体的荧光强度。这些新的发现有助于设计具有优异发光性能的掺杂银纳米团簇。
The weak photoluminescence of silver nanoclusters prevents their broad application as luminescent nanomaterials. Recent experiments, however, have shown that gold doping can significantly enhance the photoluminescence intensity of Ag29 nanoclusters but the molecular and physical origins of this effect remain unknown. Therefore, we have computationally explored the geometric and electronic structures of Ag29 and gold-doped Ag29-x Aux (x=1-5) nanoclusters in the S0 and S1 states. We found that 1) relativistic effects that are mainly due to the Au atoms play an important role in enhancing the fluorescence intensity, especially for highly doped Ag26 Au3 , Ag25 Au4 , and Ag24 Au5 , and that 2) heteronuclear Au-Ag bonds can increase the stability and regulate the fluorescence intensity of isomers of these gold-doped nanoclusters. These novel findings could help design doped silver nanoclusters with excellent luminescence properties.