A rigorous non-empirical theoretical analysis of the 2p XPS of NiO: Is it necessary to invoke nonlocal screening?

Bagus, Paul S.; Brundle, Christopher R.; Ilton, Eugene S.

doi:10.1016/j.jelechem.2020.114135

A rigorous non-empirical theoretical analysis of the 2p XPS of NiO: Is it necessary to invoke nonlocal screening?

Journal Article · Fri Apr 03 00:00:00 EDT 2020 · Journal of Electroanalytical Chemistry

DOI:https://doi.org/10.1016/j.jelechem.2020.114135· OSTI ID:1762484

Bagus, Paul S. ^[1]; Brundle, Christopher R. ^[2]; Ilton, Eugene S. ^[3]

Univ. of North Texas, Denton, TX (United States)
C. R. Brundle and Associates, Soquel, CA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

The role of ligand field effects and many-body effects arising from angular momentum coupling and shake effects for the XPS of NiO, as a representative transition metal oxide, have been investigated using rigorous, non-empirical wave functions for single site cluster models. Here it is shown that important features of the XPS arise from proper treatment of angular momentum coupling and it is unnecessary to invoke non-local screening to explain the experimental XPS. Contrary to the usual understanding, it is shown that inclusion of shake excitations in the many body wavefunctions is responsible for the high BE satellites that are observed. The contribution of covalent mixing of metal and ligand orbitals in the closed shells to screening of core-holes is demonstrated.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1762484

Alternate ID(s):: OSTI ID: 1734369

Report Number(s):: PNNL--SA-149146

Journal Information:: Journal of Electroanalytical Chemistry, Journal Name: Journal of Electroanalytical Chemistry Vol. 875; ISSN 1572-6657

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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