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| 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 | |
| Source Publication | JOURNAL OF PHYSICAL CHEMISTRY A
 |
| ISSN | 1089-5639 |
| Volume | 120Issue:7Pages:1084—1096 |
| Subtype | 期刊文献 |
| Abstract | 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. |
| Keyword | 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 |
| Indexed By | SCI |
| Language | 英语 |
| WOS ID | WOS:000371103000015 |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.sinap.ac.cn/handle/331007/25813 |
| Collection | 中科院上海应用物理研究所2011-2019年 |
| Corresponding Author | 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. |
| Recommended Citation GB/T 7714 | 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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| Probing the Electron（1723KB） | 期刊论文 | 作者接受稿 | 开放获取 | CC BY-NC-SA | View Download | |
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