Probing the Electronic Structure and Chemical Bonding of Mono-Uranium Oxides with Different Oxidation States: UOx- and UOx (x=3-5)
Su, J; Li, WL; Lopez, GV; Jian, T; Cao, GJ; Li, WL; Schwarz, WHE; Wang, LS; Li, J; Li, J (reprint author), Tsinghua Univ, Dept Chem, Minist Educ, Beijing 100084, Peoples R China.; 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.
2016
发表期刊JOURNAL OF PHYSICAL CHEMISTRY A
ISSN1089-5639
卷号120期号:7页码:1084—1096
文章类型期刊文献
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.
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
DOI10.1021/acs.jpca.5b11354
收录类别SCI
语种英语
WOS记录号WOS:000371103000015
引用统计
文献类型期刊论文
条目标识符http://ir.sinap.ac.cn/handle/331007/25813
专题中科院上海应用物理研究所2011-2018年
通讯作者Schwarz, WHE; Li, J (reprint author), Tsinghua Univ, Dept Chem, Minist Educ, Beijing 100084, Peoples R China.; 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.
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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,2016,120(7):1084—1096.
APA Su, J.,Li, WL.,Lopez, GV.,Jian, T.,Cao, GJ.,...&Schwarz, WHE .(2016).Probing the Electronic Structure and Chemical Bonding of Mono-Uranium Oxides with Different Oxidation States: UOx- and UOx (x=3-5).JOURNAL OF PHYSICAL CHEMISTRY A,120(7),1084—1096.
MLA Su, J,et al."Probing the Electronic Structure and Chemical Bonding of Mono-Uranium Oxides with Different Oxidation States: UOx- and UOx (x=3-5)".JOURNAL OF PHYSICAL CHEMISTRY A 120.7(2016):1084—1096.
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