The apparent absence of chemical sensitivity in the 4d and 5d X-ray absorption spectroscopy of uranium compounds
Abstract
X-ray absorption spectroscopy (XAS) and related derivative measurements have been used to demonstrate that the Pu 5f states are strongly relativistic and have a 5f occupation number near 5. Owing to the success in this regime, it has been argued that the XAS measurements should be a powerful tool to probe 5f occupation variation, both as a function of elemental nature (actinide atomic number) and as a function of physical and chemical perturbation, e.g., oxidation state. We show that XAS and its related measurements fail in this latter aspect for a wide variety of uranium compounds and materials. Possible causes will be discussed.
- Authors:
-
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1237532
- Report Number(s):
- LLNL-JRNL-636485
Journal ID: ISSN 0368-2048
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Electron Spectroscopy and Related Phenomena
- Additional Journal Information:
- Journal Volume: 194; Journal ID: ISSN 0368-2048
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; actinides; photoelectron spectroscopy; x-ray absorption spectroscopy
Citation Formats
Tobin, J. G. The apparent absence of chemical sensitivity in the 4d and 5d X-ray absorption spectroscopy of uranium compounds. United States: N. p., 2013.
Web. doi:10.1016/j.elspec.2014.01.020.
Tobin, J. G. The apparent absence of chemical sensitivity in the 4d and 5d X-ray absorption spectroscopy of uranium compounds. United States. https://doi.org/10.1016/j.elspec.2014.01.020
Tobin, J. G. Fri .
"The apparent absence of chemical sensitivity in the 4d and 5d X-ray absorption spectroscopy of uranium compounds". United States. https://doi.org/10.1016/j.elspec.2014.01.020. https://www.osti.gov/servlets/purl/1237532.
@article{osti_1237532,
title = {The apparent absence of chemical sensitivity in the 4d and 5d X-ray absorption spectroscopy of uranium compounds},
author = {Tobin, J. G.},
abstractNote = {X-ray absorption spectroscopy (XAS) and related derivative measurements have been used to demonstrate that the Pu 5f states are strongly relativistic and have a 5f occupation number near 5. Owing to the success in this regime, it has been argued that the XAS measurements should be a powerful tool to probe 5f occupation variation, both as a function of elemental nature (actinide atomic number) and as a function of physical and chemical perturbation, e.g., oxidation state. We show that XAS and its related measurements fail in this latter aspect for a wide variety of uranium compounds and materials. Possible causes will be discussed.},
doi = {10.1016/j.elspec.2014.01.020},
journal = {Journal of Electron Spectroscopy and Related Phenomena},
number = ,
volume = 194,
place = {United States},
year = {Fri May 03 00:00:00 EDT 2013},
month = {Fri May 03 00:00:00 EDT 2013}
}
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Works referenced in this record:
Electronic structure of uranium halides and oxyhalides in the solid state. An x-ray photoelectron spectral study of bonding ionicity
journal, October 1982
- Thibaut, Elisabeth; Boutique, Jean Pol; Verbist, Jacques J.
- Journal of the American Chemical Society, Vol. 104, Issue 20
Splittings, Satellites and Fine Structure in the Soft X-ray Spectroscopy of the Actinides
journal, June 2013
- Tobin, J. G.; Yu, S. -W.; Chung, B. W.
- Topics in Catalysis, Vol. 56, Issue 12
Works referencing / citing this record: