Anion photoelectron spectroscopy and chemical bonding of ThO2- and ThO3-
文献类型：期刊论文
| 作者 | Li, YL; Zou, JH; Xiong, XG; Xie, H; Tang, ZC; Ge, M; Zhao, YF; Liu, HT |
| 刊名 | JOURNAL OF CHEMICAL PHYSICS
 |
| 出版日期 | 2018 |
| 卷号 | 148期号:24页码:- |
| 关键词 | 2-ELECTRON VALENCE INDEXES ELECTRONIC-STRUCTURE INFRARED-SPECTRA ROTATIONAL ANALYSIS ACTINIDE COMPLEXES URANIUM-OXIDES BAND SYSTEMS BASIS-SETS MATRIX UO2 |
| ISSN号 | 0021-9606 |
| DOI | 10.1063/1.5030142 |
| 文献子类 | 期刊论文 |
| 英文摘要 | We conducted a study of electronic structures and chemical bonding of gaseous ThO2- and ThO3- using velocity-map imaging and ab initio calculations. The electron affinity of neutral ThO2- molecule is reported for the first time with the value of 1.21(5) eV. We obtained a vibrationally resolved photoelectron spectroscopy of ThO2- and observed the symmetric stretching frequency of 824(40) cm(-1) for neutral molecules. One hot band transition is observed in the spectrum of ThO2-, which allows the measurement of symmetric stretching mode for ThO2-. The ground state of ThO2- is (2)A(1) with C-2v symmetry: the detachment of an electron from the singly occupied molecular orbital (SOMO) results in the ground state of ThO2. Kohn-Sham molecular orbital analyses reveal an sigma and two weak pi bonds for Th-O multiple bonds in ThO2. Global minimum search methodology combined with quantum chemical calculations are used to find the minima of ThO3 and ThO3-, and the adiabatic detachment energy of ThO3- is calculated to be 3.26 eV at the coupled cluster with singles and doubles plus perturbative triples level. Our theoretical calculations suggest that the ground state of ThO3- is (1)A' with a symmetry of C-s, while the most stable ThO3- is (2)A(1) with C-2v symmetry; thus, the transition from ThO3- to ThO3 undergoes a significant geometry reorganization. Molecular orbital analyses suggest that the SOMO of ThO3- is mainly participated by O 2p and O to Th back donation was found in HOMO-2 molecular orbital. This investigation will shed some light on the understanding of covalent bonding in Th-contained molecules. Published by AIP Publishing. |
| 语种 | 英语 |
| 源URL | [http://ir.sinap.ac.cn/handle/331007/30843]  |
| 专题 | 上海应用物理研究所_中科院上海应用物理研究所2011-2017年 |
| 作者单位 | 1.Inst Appl Phys & Computat Math, Beijing 10088, Peoples R China 2.Nagoya Univ, Inst Transformat Biomol WPI ITbM, Chikusa Ku, Nagoya, Aichi 4648602, Japan 3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China 4.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 5.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China 6.Xiamen Univ, State Key Lab Phys Chem Solid Surfaces, Dept Chem, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China |
| 推荐引用方式 GB/T 7714 | Li, YL,Zou, JH,Xiong, XG,et al. Anion photoelectron spectroscopy and chemical bonding of ThO2- and ThO3-[J]. JOURNAL OF CHEMICAL PHYSICS,2018,148(24):-. |
| APA | Li, YL.,Zou, JH.,Xiong, XG.,Xie, H.,Tang, ZC.,...&Liu, HT.(2018).Anion photoelectron spectroscopy and chemical bonding of ThO2- and ThO3-.JOURNAL OF CHEMICAL PHYSICS,148(24),-. |
| MLA | Li, YL,et al."Anion photoelectron spectroscopy and chemical bonding of ThO2- and ThO3-".JOURNAL OF CHEMICAL PHYSICS 148.24(2018):-. |
入库方式： OAI收割
来源：上海应用物理研究所
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