Combined experimental and theoretical study on low-lying electronic states of CuO^(-)  

CuO^(-)低电子态的实验与理论研究

作　　者：Gaoming Hu Zhen Li Wenli Liu Qiang Zhang Boxing Zhu Yang Chen Dongfeng Zhao 胡高明;李珍;刘文莉;张强;朱波星;陈旸;赵东锋(美国加州大学河滨分校化学系,河滨92521;安徽师范大学物理系,安徽省光电材料科学与技术重点实验室,芜湖241000)

机构地区：[1]Hefei National Research Center for Physical Sciences at the Microscale,Department of Chemical Physics,University of Science and Technology of China,Hefei 230026,China [2]Hefei National Laboratory,University of Science and Technology of China,Hefei 230088,China

出　　处：《Chinese Journal of Chemical Physics》2024年第6期863-868,I0043,共7页化学物理学报(英文)

基　　金：supported by the National Natural Science Foudation of China(No.22173089,and No.22103075);the National Key R&D Program of China(No.2021YFA0716801);Innovation Program for Quantum Science and Technology(2021ZD0300301).

摘　　要：We present a combined experimental and theoretical study on the electronic structure and bonding characteristics of the CuO^(-)anion.On the experimental side,high resolution photoelectron imaging has allowed the detection of new features of the low-lying states of the CuO^(-).Supporting MRCI+Q calculations with inclusion of complex spin-orbit coupling effects have yielded complemented assignments of the photoelectron spectra obtained in the present and previous experiments to low-lying spin-orbit mixed states,which also reveal strong multiconfiguration correlation effects in CuO^(-).Analyses on the experimentally measured photoelectron angular distributions indicate that,the Cu-O bond in the X^(1)Σ^(+)state can be characterized by mixed ionic and covalent interactions,with the ionic character being more dominant,while the a^(3)Пstate can be characterized by a typical ionic bond.Our results provide a renewed understanding in the interplay of ionic-covalent bonding characters in the diatomic CuO^(-)anion.实验与理论相结合研究了CuO^(-)的电子结构和成键特性.实验上利用高分辨光电子成像技术,获得了X^(1)Σ^(+)态和a^(3)∏态振动和电子自旋分裂的能级结构.基于包含自旋-轨道耦合作用的多参考组态相互作用方法的量子化学计算结果,对实验获得的光电子谱精细结构进行了标识,并证实前人文献提出的CuO^(-)分子存在强电子相关作用.进一步结合实验获得光电子角分布,发现X^(1)Σ^(+)态的Cu-O键表现出离子-共价键作用共存的特征,且以离子键作用为主;而a^(3)∏态的Cu-O键则表现为典型的离子键特征.

关 键 词：CuO^(-) Photoelectron imaging Spin-orbit coupling Ionic/covalent bond 

分 类 号：O64[理学—物理化学]