Cluster embedding of ionic systems: Point charges and extended ions
Abstract
The embedding of cluster models of oxides with point charges and with extensions of the embedding which take into account the spatial extent of the cations is examined with an emphasis on the consequences of this embedding for the relative ionization and excitation energies that are measured in core-level spectroscopies. It is found that the dependence of the electronic structure of the oxides and the relative energies of different levels depend only weakly on the embedding and that relatively simple embeddings may be sufficient to provide an adequate model for determining core-level spectra. This is different from absolute values of the ionizations which, as expected, depend strongly on the details of the extended crystal; however, relative values of binding energies, as measured in photoemission, are of greater interest than the absolute values
- Authors:
-
[1];
[2];
[2]
- Univ. of North Texas, Denton, TX (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1605894
- Alternate Identifier(s):
- OSTI ID: 1808060
- Report Number(s):
- PNNL-SA-147745
Journal ID: ISSN 0021-9606; TRN: US2104711
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 151; Journal Issue: 4; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Angular momentum coupling; Relativistic effects; Spin-orbit interactions; Chemical bonding; Core level spectroscopy; Excitation energies; Transition metal oxides; Ions and properties; Ligand fields
Citation Formats
Bagus, Paul S., Sassi, Michel J., and Rosso, Kevin M. Cluster embedding of ionic systems: Point charges and extended ions. United States: N. p., 2019.
Web. doi:10.1063/1.5108728.
Bagus, Paul S., Sassi, Michel J., & Rosso, Kevin M. Cluster embedding of ionic systems: Point charges and extended ions. United States. https://doi.org/10.1063/1.5108728
Bagus, Paul S., Sassi, Michel J., and Rosso, Kevin M. Mon .
"Cluster embedding of ionic systems: Point charges and extended ions". United States. https://doi.org/10.1063/1.5108728. https://www.osti.gov/servlets/purl/1605894.
@article{osti_1605894,
title = {Cluster embedding of ionic systems: Point charges and extended ions},
author = {Bagus, Paul S. and Sassi, Michel J. and Rosso, Kevin M.},
abstractNote = {The embedding of cluster models of oxides with point charges and with extensions of the embedding which take into account the spatial extent of the cations is examined with an emphasis on the consequences of this embedding for the relative ionization and excitation energies that are measured in core-level spectroscopies. It is found that the dependence of the electronic structure of the oxides and the relative energies of different levels depend only weakly on the embedding and that relatively simple embeddings may be sufficient to provide an adequate model for determining core-level spectra. This is different from absolute values of the ionizations which, as expected, depend strongly on the details of the extended crystal; however, relative values of binding energies, as measured in photoemission, are of greater interest than the absolute values},
doi = {10.1063/1.5108728},
journal = {Journal of Chemical Physics},
number = 4,
volume = 151,
place = {United States},
year = {Mon Jul 29 00:00:00 EDT 2019},
month = {Mon Jul 29 00:00:00 EDT 2019}
}
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Cited by: 13 works
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Figures / Tables:
Fig. 1: The FeO6Mg18 PC embedded cluster. The anions and cations explicitly included are shown as large spheres and representative PCs as small spheres.
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Works referencing / citing this record:
Analysis of the Fe 2p XPS for hematite α Fe 2 O 3 : Consequences of covalent bonding and orbital splittings on multiplet splittings
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Figures / Tables found in this record:
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.