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题名:
Probing the Electronic Structure and Chemical Bonding of Mono-Uranium Oxides with Different Oxidation States: UOx- and UOx (x=3-5)
作者: Su, J; Li, WL; Lopez, GV; Jian, T; Cao, GJ; Li, WL; Schwarz, WHE; Wang, LS; Li, J
刊名: JOURNAL OF PHYSICAL CHEMISTRY A
出版日期: 2016
卷号: 120, 期号:7, 页码:1084—1096
关键词: RELATIVISTIC QUANTUM-CHEMISTRY ; KOHN-SHAM ORBITALS ; INFRARED-SPECTRA ; BASIS-SETS ; GAS-PHASE ; VALENCE INDEXES ; WAVE-FUNCTIONS ; PHOTOELECTRON-SPECTROSCOPY ; EXCITATION-ENERGIES ; SPIN-ORBIT
DOI: 10.1021/acs.jpca.5b11354
通讯作者: Schwarz, WHE ; Li, J (reprint author), Tsinghua Univ, Dept Chem, Minist Educ, Beijing 100084, Peoples R China. ; Schwarz, WHE ; Li, J (reprint author), Tsinghua Univ, Minist Educ, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China. ; Wang, LS (reprint author), Brown Univ, Dept Chem, Providence, RI 02912 USA. ; Schwarz, WHE (reprint author), Univ Siegen, Phys & Theoret Chem, D-57068 Siegen, Germany.
文章类型: 期刊文献
英文摘要: Uranium oxide clusters UOx- (x = 3-5) were produced by laser vaporization and characterized by photoelectron spectroscopy and quantum theory. Photoelectron spectra were obtained for UOx- at various photon energies with well-resolved detachment transitions and vibrational resolution for x = 3 and 4. The electron affinities of UOx were measured as 1.12, 3.60, and 4.02 eV for x = 3, 4, and 5, respectively. The geometric and electronic structures of both the anions and the corresponding neutrals were investigated by quasi-relativistic electron-correlation quantum theory to interpret the photoelectron spectra and to provide insight into their chemical bonding. For UOx clusters with x <= 3, the O atoms appear as divalent closed-shell anions around the U atom, which is in various oxidation states from U-II(fds)(4) in UO to U-VI(fds)(0) in UO3. For x > 3, there are no longer sufficient valence electrons from the U atom to fill the O(2p) shell, resulting in fractionally charged and multicenter delocalized valence states for the O ligands as well as eta(1)- or eta(2)-bonded O-2 units, with unusual spin couplings and complicated electron correlations in the unfilled poly oxo shell. The present work expands our understanding of both the bonding capacities of actinide elements with extended spdf valence shells as well as the multitude of oxygen's charge and bonding states.
收录类别: SCI
语种: 英语
WOS记录号: WOS:000371103000015
ISSN号: 1089-5639
Citation statistics:
内容类型: 期刊论文
URI标识: http://ir.sinap.ac.cn/handle/331007/25813
Appears in Collections:中科院上海应用物理研究所2011-2017年_期刊论文

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Recommended Citation:
Su, J,Li, WL,Lopez, GV,et al. Probing the Electronic Structure and Chemical Bonding of Mono-Uranium Oxides with Different Oxidation States: UOx- and UOx (x=3-5)[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2016-01-01,120(7):1084—1096.
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