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Title: 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:
 [1]
  1. 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. doi: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. doi: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 = {2013},
month = {5}
}

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Cited by: 4 works
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