Liao Can, Zhu Manzhou, Jiang De-En, Li Xiaosong
Department of Chemistry, University of Washington Seattle WA 98195 USA
Department of Chemistry and Center for Atomic Engineering of Advanced Materials, Anhui University China
Chem Sci. 2023 Apr 11;14(18):4666-4671. doi: 10.1039/d3sc00944k. eCollection 2023 May 10.
Atomically precise nanoclusters play an important role in nanoscale catalysis, photonics, and quantum information science. Their nanochemical properties arise from their unique superatomic electronic structures. As the flagship of atomically precise nanochemistry, the Au(SR) nanocluster exhibits tunable spectroscopic signatures that are sensitive to the oxidation state. This work aims to unravel the physical underpinnings of the spectral progression of Au(SR) nanocluster using variational relativistic time-dependent density functional theory. The investigation will focus on the effects of superatomic spin-orbit coupling, its interplay with Jahn-Teller distortion, and their manifestations in the absorption spectra of Au(SR) nanoclusters of different oxidation states.
原子精确的纳米团簇在纳米尺度催化、光子学和量子信息科学中发挥着重要作用。它们的纳米化学性质源于其独特的超原子电子结构。作为原子精确纳米化学的旗舰，Au(SR)纳米团簇表现出对氧化态敏感的可调谐光谱特征。这项工作旨在利用变分相对论含时密度泛函理论揭示Au(SR)纳米团簇光谱进展的物理基础。研究将聚焦于超原子自旋-轨道耦合的影响、其与 Jahn-Teller 畸变的相互作用，以及它们在不同氧化态的 Au(SR)纳米团簇吸收光谱中的表现。
