CAS OpenIR  > 中科院上海应用物理研究所2011-2020年
Strong electron correlation in UO2-: A photoelectron spectroscopy and relativistic quantum chemistry study
Li, WL; Su, J; Jian, T; Lopez, GV; Hu, HS; Cao, GJ; Li, J; Wang, LS; junli@tsinghua.edu.cn; lai-sheng_wang@brown.edu
2014
Source PublicationJOURNAL OF CHEMICAL PHYSICS
ISSN0021-9606
Volume140Issue:9
AbstractThe electronic structures of actinide systems are extremely complicated and pose considerable challenges both experimentally and theoretically because of significant electron correlation and relativistic effects. Here we report an investigation of the electronic structure and chemical bonding of uranium dioxides, UO2- and UO2, using photoelectron spectroscopy and relativistic quantum chemistry. The electron affinity of UO2 is measured to be 1.159(20) eV. Intense detachment bands are observed from the UO2- low-lying (7s sigma(g))(2)(5f phi(u))(1) orbitals and the more deeply bound O2p-based molecular orbitals which are separated by a large energy gap from the U-based orbitals. Surprisingly, numerous weak photodetachment transitions are observed in the gap region due to extensive two-electron transitions, suggesting strong electron correlations among the (7s sigma(g))(2)(5f phi(u))(1) electrons in UO2- and the (7s sigma(g))(1)(5f phi(u))(1) electrons in UO2. These observations are interpreted using multi-reference ab initio calculations with inclusion of spin-orbit coupling. The strong electron correlations and spin-orbit couplings generate orders-of-magnitude more detachment transitions from UO2- than expected on the basis of the Koopmans' theorem. The current experimental data on UO2- provide a long-sought opportunity to arbitrating various relativistic quantum chemistry methods aimed at handling systems with strong electron correlations. (C) 2014 AIP Publishing LLC.
KeywordBasis-sets Infrared-spectra Actinyl Ions Gas-phase Perturbation-theory Spin-orbit Molecules Atoms Complexes Elements
Indexed BySCI
Language英语
WOS IDWOS:000334067400018
Citation statistics
Cited Times:21[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/14414
Collection中科院上海应用物理研究所2011-2020年
Corresponding Authorjunli@tsinghua.edu.cn; lai-sheng_wang@brown.edu
Recommended Citation
GB/T 7714
Li, WL,Su, J,Jian, T,et al. Strong electron correlation in UO2-: A photoelectron spectroscopy and relativistic quantum chemistry study[J]. JOURNAL OF CHEMICAL PHYSICS,2014,140(9).
APA Li, WL.,Su, J.,Jian, T.,Lopez, GV.,Hu, HS.,...&lai-sheng_wang@brown.edu.(2014).Strong electron correlation in UO2-: A photoelectron spectroscopy and relativistic quantum chemistry study.JOURNAL OF CHEMICAL PHYSICS,140(9).
MLA Li, WL,et al."Strong electron correlation in UO2-: A photoelectron spectroscopy and relativistic quantum chemistry study".JOURNAL OF CHEMICAL PHYSICS 140.9(2014).
Files in This Item: Download All
File Name/Size DocType Version Access License
Strong electron corr(841KB) 开放获取CC BY-NC-SAView Download
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[Li, WL]'s Articles
[Su, J]'s Articles
[Jian, T]'s Articles
Baidu academic
Similar articles in Baidu academic
[Li, WL]'s Articles
[Su, J]'s Articles
[Jian, T]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Li, WL]'s Articles
[Su, J]'s Articles
[Jian, T]'s Articles
Terms of Use
No data!
Social Bookmark/Share
File name: Strong electron correlation in UO2-. A photoelectron spectroscopy and relativistic quantum chemistry study.pdf
Format: Adobe PDF
All comments (0)
No comment.
 

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.