Size- and Shape-Dependent Photoexcitation Electron Transfer in Metal Nanoclusters

纳米团簇 光激发 电子转移 材料科学 化学物理 电子 结晶学 纳米技术 化学 原子物理学 光化学 物理 激发态 量子力学
作者
Wentao Fan,Ying Yang,Qing You,Jin Li,Haiteng Deng,Nan Yan,Zhikun Wu
出处
期刊:Journal of Physical Chemistry C [American Chemical Society]
卷期号:127 (1): 816-823 被引量:10
标识
DOI:10.1021/acs.jpcc.2c07678
摘要

There are some unresolved fundamental issues for metal nanoclusters; for instance, the close-packed structure transformation from face-centered cubic (fcc) to hexagonal close-packed (hcp) has not yet been reported, and photoexcitation electron transfer is not well understood. Herein, we realized for the first time the fcc-to-hcp structure transformation and revealed the size- and shape-dependent photoexcitation electron transfer for metal nanoclusters. Specifically, a thermally induced ligand exchange method was developed, and a rod-shaped hcp Au42(SCH2Ph)32 (HSCH2Ph: benzyl mercaptan) with the largest aspect ratio was synthesized from fcc Au28(SPh-tBu)20 (HSPh-tBu: p-tert-butylphenol) and structurally resolved, which shows a sharp absorption at 815 nm and dual emission that is well interpreted by time-dependent density functional theory (TD-DFT) calculations. The structure transformation pathway was proposed, and a novel, rod-shaped hcp Au58(SR)40 with larger aspect ratio was predicted. Interestingly, it is found that the kernel-based middle-to-both ends sp ← sp photoexcitation electron transfer can be extended to other rod-like (one-dimensional) gold nanoclusters, and the major photoexcitation turns to the kernel-based sp ← sp transition from the staple-to-kernel sp ← d transition when the spherical gold nanocluster size is increased to Au42 and the Au(6sp) composition increases with increasing size for structure-similar nanoclusters. These findings deepen our understanding of metal nanocluster photoexcitation electron transfer and provide guidance for future nanocluster property tuning aimed at practical applications.
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