Zhang Ying, Zhang Wei, Zhang Tai-Song, Ge Chao, Tao Yang, Fei Wenwen, Fan Weigang, Zhou Meng, Li Man-Bo
Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Institutes of Physical Science and Information Technology, Anhui University, Hefei 230601, P. R. China.
Department of Chemical Physics, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, P. R. China.
J Am Chem Soc. 2024 Apr 10;146(14):9631-9639. doi: 10.1021/jacs.3c12982. Epub 2024 Mar 26.
The induced structural transformation provides an efficient way to precisely modulate the fine structures and the corresponding performance of gold nanoclusters, thus constituting one of the important research topics in cluster chemistry. However, the driving forces and mechanisms of these processes are still ambiguous in many cases, limiting further applications. In this work, based on the unique coordination mode of the pincer ligand-stabilized gold nanocluster Au(PNP), we revealed the site-recognition mechanism for induced transformations of gold nanoclusters. The "open nitrogen sites" on the surface of the nanocluster interact with different inducers including organic compounds and metals and trigger the conversion of Au(PNP) to Au and AuAg nanoclusters, respectively. Control experiments verified the site-recognition mechanism, and the femtosecond and nanosecond transient absorption spectroscopy revealed the electronic and photoluminescent evolution accompanied by the structural transformation.
诱导结构转变提供了一种精确调节金纳米团簇精细结构及其相应性能的有效方法，从而构成了团簇化学中的重要研究课题之一。然而，在许多情况下，这些过程的驱动力和机制仍然不明确，限制了进一步的应用。在这项工作中，基于钳形配体稳定的金纳米团簇Au(PNP)独特的配位模式，我们揭示了金纳米团簇诱导转变的位点识别机制。纳米团簇表面的“开放氮位点”与包括有机化合物和金属在内的不同诱导剂相互作用，分别触发Au(PNP)向Au和AuAg纳米团簇的转变。对照实验验证了位点识别机制，飞秒和纳秒瞬态吸收光谱揭示了伴随结构转变的电子和光致发光演化。
