超小尺寸银团簇:类分子结构模拟与吸收光谱计算  

Ultrasmall Size Silver Clusters:Molecular-like Structural Simulation and Absorption Spectra Calculation

作　　者：陈伟林[1] 黄谊平 陈晓桐 乔旭升[1,2,3] 樊先平 CHEN Weilin;HUANG Yiping;CHEN Xiaotong;QIAO Xusheng;FAN Xianping(School of Material Science and Engineering,Zhejiang University,Hangzhou 310058,China;State Key Laboratory of Silicon and Advanced Semiconductor Materials,Zhejiang University,Hangzhou 310058,China;Longmen Laboratory of Luoyang,Luoyang 471000,China)

机构地区：[1]浙江大学材料科学与工程学院,浙江杭州310058 [2]浙江大学硅及先进半导体全国重点实验室,浙江杭州310058 [3]龙门实验室,河南洛阳471000

出　　处：《发光学报》2024年第8期1380-1390,共11页Chinese Journal of Luminescence

基　　金：国家自然科学基金(52172008)。

摘　　要：基于密度泛函理论和含时密度泛函理论研究了多种带中性和正电荷的超小尺寸银团簇([Ag_(m)]^(n+),m=2~8,n=0~2)的几何结构、电子结构和吸收光谱特征。研究结果表明,超小尺寸银团簇的电子能级结构和吸收光谱受到团簇尺寸、对称性、开闭壳层以及电荷等多种因素的共同影响。平均结合能计算结果表明,中性超小尺寸银团簇尺寸的增大使其稳定性逐渐增强。但带正电荷的超小尺寸银团簇由于奇偶振荡现象的影响,使其在阴离子多面体网络中优势构型不一定为最低能量构型。该研究为辨认荧光玻璃中特定构型的银团簇的特征发光,构建了超小尺寸银团簇的几何结构、电子结构和吸收光谱数据集,也能为拓展超小尺寸银团簇在其他各类无机以及有机配体中的结构与光谱研究提供理论数据支撑。In this work,the geometric structures,electronic structures,and absorption spectra of various neutral and positively charged ultrasmall size silver clusters([Ag_(m)]^(n+),m=2-8,n=0-2),have been investigated using density functional theory and time-dependent density functional theory.The simulation results demonstrate that the electronic energy level structures and absorption spectra of the ultrasmall size silver clusters are influenced by multiple factors,including size,symmetry,open-shell and closed-shell systems,and electric charges of clusters.Furthermore,average binding energy calculations indicate that an increase in the size of neutral ultrasmall size silver clusters results in a gradual enhancement in their stability.However,positively charged ultrasmall size silver clusters are subject to the parity oscillations phenomenon,which means that the dominant configuration in the anionic polyhedral network is not necessarily the lowest-energy configuration.This study has led to the construction of a database of the geometrical structures,electronic structures,and absorption spectra of ultrasmall size silver clusters.This dataset has been created to identify the characteristic luminescence of ultrasmall size silver clusters in specific configurations in fluorescent glasses.Furthermore,the database will provide theoretical support data for expanding the structural and spectroscopic studies of ultrasmall size silver clusters in other types of inorganic as well as organic ligands.

关 键 词：银团簇 密度泛函理论 含时密度泛函理论 吸收光谱 

分 类 号：O482.31[理学—固体物理]