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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Photoelectron Spectroscopy and Electronic Structure of ScO_n~- (n = 1 - 4) and YO_n~- (n = 1 - 5): Strong Electron Correlation Effects in ScO~- and YO~-
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Photoelectron Spectroscopy and Electronic Structure of ScO_n~- (n = 1 - 4) and YO_n~- (n = 1 - 5): Strong Electron Correlation Effects in ScO~- and YO~-

机译：ScO_n〜-（n = 1-4）和YO_n〜-（n = 1-5）的光电子能谱和电子结构：ScO〜-和YO〜-的强电子相关效应

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摘要

A photoelectron spectroscopic study of ScO_n~- (n = 1 - 4) and YO_n~- (n = 1 - 5) was carried out at three photon energies: 532, 355, and 266 nm. Vibrationally resolved photoelectron spectra were obtained for ScO~- and YO~-. The electron affinities of both ScO and YO were measured to be identical (1.35 eV) within the experimental accuracy (± 0.02 eV). Three low-lying excited states were observed for the monoxides, A~('2)Δ, A~2Π, and B~2∑~+. The latter two excited states resulted from two-electron detachment, suggesting unusually strong electron correlation (configuration interaction) effects in the ground state of the anions. The excitation energies of the low-lying states were also found to be similar for the two monoxides except that YO has a smaller vibrational frequency and larger spin-orbit splitting. The A~('2)Δ states of both ScO and YO show very strong photon energy-dependent detachment cross sections. Four similar photoelectron features were observed for the dioxides with those of YO_2~- having lower binding energies. A second isomer due to an O_2 complex was also observed for Sc and Y. Broad and featureless spectra were observed for the higher oxides. At least two isomers were present for the higher oxides, one with low and one with high binding energies.
机译：ScO_n〜-（n = 1-4）和YO_n〜-（n = 1-5）的光电子光谱研究是在三种光子能量：532、355和266 nm下进行的。获得了ScO〜-和YO〜-的振动分辨光电子能谱。在实验精度（±0.02 eV）范围内，ScO和YO的电子亲和力均相同（1.35 eV）。一氧化氮的三个低位激发态分别为A〜（'2）Δ，A〜2Π和B〜2∑〜+。后两个激发态是由于两个电子的脱离而产生的，这表明在阴离子的基态中异常强的电子相关（构型相互作用）效应。还发现低态的激发能与两种一氧化物相似，除了YO的振动频率较小，自旋轨道分裂较大。 ScO和YO的A〜（'2）Δ态都显示出非常强的光子能量依赖性脱离截面。观察到四个相似的光电子特征，其中二价氧化物具有较低的结合能。对于Sc和Y，还观察到由于O_2络合物而形成的第二个异构体。对于较高的氧化物，观察到宽光谱和无特征光谱。对于高级氧化物，存在至少两种异构体，一种具有低结合能，一种具有高结合能。

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