Yan Chaoqiang, Li Yanshuang, Wang Endong, Xu Wen Wu
Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo 315211, China.
School of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian 116029, China.
J Phys Chem Lett. 2023 Aug 31;14(34):7632-7637. doi: 10.1021/acs.jpclett.3c01731. Epub 2023 Aug 21.
Structural global searches employing highly efficient algorithms have been extensively applied for studying molecules and clusters. However, the code-aided spatial conformational determination of thiolated gold nanoclusters (AuNCs) has not been accomplished because of the complex structural architecture of AuNCs, especially when only the chemical formula of the cluster is known. Experiments have shown that the star [Au(SR)] cluster can transform into the [Au(SR)] cluster. However, the crystal structure of the [Au(SR)] cluster has not been experimentally determined, and theoretical structural predictions for this cluster are challenging because no template cluster presents for [Au(SR)]. Utilizing the grand unified model, this study succeeded in obtaining the structure of the [Au(SR)] cluster by using minimal computations, which was verified to be reasonable through stability analysis and experimental absorption spectrum confirmation. Although the predicted [Au(SR)] cluster has the same number of Au atoms as the [Au(SR)] cluster, the structure is considerably altered, owing to the presence of a face-centered cubic kernel. This study provides insights for decoding the chemical formulas of AuNCs to determine their spatial conformations.
采用高效算法的结构全局搜索已广泛应用于分子和团簇研究。然而，由于硫醇化金纳米团簇（AuNCs）结构复杂，尤其是仅知道团簇化学式时，通过代码辅助确定其空间构象尚未实现。实验表明，星形[Au(SR)]团簇可转化为[Au(SR)]团簇。然而，[Au(SR)]团簇的晶体结构尚未通过实验确定，且由于没有[Au(SR)]的模板团簇，对该团簇进行理论结构预测具有挑战性。本研究利用大统一模型，通过最少计算成功获得了[Au(SR)]团簇的结构，并通过稳定性分析和实验吸收光谱确认验证其合理性。尽管预测的[Au(SR)]团簇与[Au(SR)]团簇的金原子数相同，但由于存在面心立方内核，结构有很大改变。本研究为解读AuNCs化学式以确定其空间构象提供了思路。
