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Photoelectron spectroscopy and theoretical studies of gaseous uranium hexachlorides in different oxidation states: UCl6q- (q=0-2)
Su, J; Dau, PD; Liu, HT; Huang, DL; Wei, F; Schwarz, WHE; Li, J; Wang, LS
2015
Source PublicationJOURNAL OF CHEMICAL PHYSICS
Volume142Issue:13Pages:
Subtype期刊文献
AbstractUranium chlorides are important in actinide chemistry and nuclear industries, but their chemical bonding and many physical and chemical properties are not well understood yet. Here, we report the first experimental observation of two gaseous uranium hexachloride anions, UCl6- and UCl62-, which are probed by photoelectron spectroscopy in conjunction with quantum chemistry calculations. The electron affinity of UCl6 is measured for the first time as +5.3 eV; its second electron affinity is measured to be +0.60 eV from the photoelectron spectra of UCl62-. We observe that the detachment cross sections of the 5f electrons are extremely weak in the visible and UV energy ranges. It is found that the one-electron one-determinental molecular orbital picture and Koopmans' theorem break down for the strongly internally correlated U-5f(2) valence shell of tetravalent U+4 in UCl62-. The calculated adiabatic and vertical electron detachment energies from ab initio calculations agree well with the experimental observations. Electronic structure and chemical bonding in the uranium hexachloride species UCl62- to UCl6 are discussed as a function of the oxidation state of U. (C) 2015 AIP Publishing LLC.
KeywordMultiply-charged Anions Multireference Perturbation-theory 2-electron Valence Indexes Repulsive Coulomb Barrier Reference Wave-functions Kohn-sham Orbitals Electronic-structure Force-constants Basis-sets Internuclear Distances
Indexed BySCI
Language英语
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/24531
Collection中科院上海应用物理研究所2011-2019年
Recommended Citation
GB/T 7714
Su, J,Dau, PD,Liu, HT,et al. Photoelectron spectroscopy and theoretical studies of gaseous uranium hexachlorides in different oxidation states: UCl6q- (q=0-2)[J]. JOURNAL OF CHEMICAL PHYSICS,2015,142(13):—.
APA Su, J.,Dau, PD.,Liu, HT.,Huang, DL.,Wei, F.,...&Wang, LS.(2015).Photoelectron spectroscopy and theoretical studies of gaseous uranium hexachlorides in different oxidation states: UCl6q- (q=0-2).JOURNAL OF CHEMICAL PHYSICS,142(13),—.
MLA Su, J,et al."Photoelectron spectroscopy and theoretical studies of gaseous uranium hexachlorides in different oxidation states: UCl6q- (q=0-2)".JOURNAL OF CHEMICAL PHYSICS 142.13(2015):—.
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