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Title: Simulating Cl K-edge X-ray absorption spectroscopy in MCl62- (M= U, Np, Pu) complexes and UOCl5- using time-dependent density functional theory

We report simulations of the X-ray absorption near edge structure (XANES) at the Cl K-edge of actinide hexahalides MCl62- (M = U, Np, Pu) and the UOCl5- complex using linear-response time-dependent density functional theory (LR-TDDFT) extended for core excitations. To the best of our knowledge, these are the first calculations of the Cl K-edge spectra of NpCl62- and PuCl62-. In addition, the spectra are simulated with and without the environmental effects of the host crystal as well as ab initio molecular dynamics (AIMD) to capture the dynamical effects due to atomic motion. The calculated spectra are compared with experimental results, where available and the observed trends are discussed.
Publication Date:
OSTI Identifier:
Report Number(s):
47703; KC0302030
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: Theoretical Chemistry Accounts, 133(4):1-7
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org:
Country of Publication:
United States
X-ray; absorption; spectroscopy; Time-Dependent Density Functional Theory; XANES; actinide; excitation; ab initio molecular dynamics; Environmental Molecular Sciences Laboratory