Role of Hydration in Photoexcited Electron Transfer between a Gold Nanocluster and a Water Molecule
Role of Hydration in Photoexcited Electron Transfer between a Gold Nanocluster and a Water Molecule
复制标题
DOI：
10.1021/acs.jpcc.1c10756
复制
发表时间：
2022-04
期刊：
影响因子：
--
通讯作者：
K. Iida
中科院分区：
文献类型：
--
作者：
K. Iida
贵金属纳米粒子的光激发在相邻分子中引起各种电化学现象。为了理解这些现象，需要获得原子和电子尺度的见解，以了解贵金属纳米颗粒和分子之间的界面在光化学过程中的作用。此外，质子溶剂广泛应用于光电系统，并具有局部分子间相互作用，如氢键，可以在确定电子和光学性质中发挥重要作用。在这项研究中，我们调查的电子结构和Au 147/H2O配合物在水溶液中的光激发电子转移，使用原始的理论方法，这是一个混合公式的量子力学方法的纳米材料的光激发和分子液体的统计力学理论。的溶剂化结构的分析表明，金表面不包括在附近的吸附的H2O氧的水分子。因此，水合增加了吸附的H2O的轨道能量，并增强了从H2O到Au 147的光激发电子转移。
The photoexcitation of noble metal nanoparticles causes various electrochemical phenomena in the neighboring molecules. To understand these phenomena, it is required to obtain atomic and electronic scale insights into the role of the interface between a noble metal nanoparticle and molecules in photochemical processes. In addition, protic solvents are widely employed in photoelectronic systems and have local intermolecular interactions such as hydrogen bonding that could play an important role in determining the electronic and optical properties. In this study, we investigate the electronic structure and the photoexcited electron transfer of a Au147/H2O complex in aqueous solution using an original theoretical approach that is a hybrid formula of the quantum mechanical method for photoexcitation of nanomaterials and a statistical mechanical theory for molecular liquids. The analysis of the solvation structure reveals that the gold surface excludes the water molecules within the proximity of the adsorbed H2O oxygen. Therefore, the hydration increases the orbital energy of the adsorbed H2O and enhances the photoexcited electron transfer from H2O to Au147.