【摘要】 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~1Σ~+态和a~3Π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~1Σ~+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~3Π态的Cu-O键则表现为典型的离子键特征.更多还原

【Abstract】 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~1Σ~+ state can be characterized by mixed ionic and covalent interactions,with the ionic character being more dominant,while the a~3Π state 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.更多还原