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Title: X-ray excited Auger transitions of Pu compounds

Abstract

X-ray excited Pu core–valence–valence and core–core–valence Auger line-shapes were used in combination with the Pu 4f photoelectron peaks to characterize differences in the oxidation state and local electronic structure for Pu compounds. The evolution of the Pu 4f core-level chemical shift as a function of sputtering depth profiling and hydrogen exposure at ambient temperature was quantified. The combination of the core–valence–valence Auger peak energies with the associated chemical shift of the Pu 4f photoelectron line defines the Auger parameter and results in a reliable method for definitively determining oxidation states independent of binding energy calibration. Results show that PuO{sub 2}, Pu{sub 2}O{sub 3}, PuH{sub 2.7}, and Pu have definitive Auger line-shapes. These data were used to produce a chemical state (Wagner) plot for select plutonium oxides. This Wagner plot allowed us to distinguish between the trivalent hydride and the trivalent oxide, which cannot be differentiated by the Pu 4f binding energy alone.

Authors:
; ; ; ; ;  [1]
  1. Lawrence Livermore National Laboratory, Physical and Life Sciences Directorate, P.O. Box 808, Livermore, California 94550 (United States)
Publication Date:
OSTI Identifier:
22392172
Resource Type:
Journal Article
Journal Name:
Journal of Vacuum Science and Technology. A, Vacuum, Surfaces and Films
Additional Journal Information:
Journal Volume: 33; Journal Issue: 3; Other Information: (c) 2015 U.S. Government; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0734-2101
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; AMBIENT TEMPERATURE; BINDING ENERGY; CALIBRATION; CHEMICAL SHIFT; CHEMICAL STATE; DEPTH; ELECTRONIC STRUCTURE; HYDROGEN; PEAKS; PLUTONIUM HYDRIDES; PLUTONIUM OXIDES; SPUTTERING; VALENCE; X RADIATION

Citation Formats

Nelson, Art J., E-mail: nelson63@llnl.gov, Grant, William K., Stanford, Jeff A., Siekhaus, Wigbert J., Allen, Patrick G., and McLean, William. X-ray excited Auger transitions of Pu compounds. United States: N. p., 2015. Web. doi:10.1116/1.4913886.
Nelson, Art J., E-mail: nelson63@llnl.gov, Grant, William K., Stanford, Jeff A., Siekhaus, Wigbert J., Allen, Patrick G., & McLean, William. X-ray excited Auger transitions of Pu compounds. United States. doi:10.1116/1.4913886.
Nelson, Art J., E-mail: nelson63@llnl.gov, Grant, William K., Stanford, Jeff A., Siekhaus, Wigbert J., Allen, Patrick G., and McLean, William. Fri . "X-ray excited Auger transitions of Pu compounds". United States. doi:10.1116/1.4913886.
@article{osti_22392172,
title = {X-ray excited Auger transitions of Pu compounds},
author = {Nelson, Art J., E-mail: nelson63@llnl.gov and Grant, William K. and Stanford, Jeff A. and Siekhaus, Wigbert J. and Allen, Patrick G. and McLean, William},
abstractNote = {X-ray excited Pu core–valence–valence and core–core–valence Auger line-shapes were used in combination with the Pu 4f photoelectron peaks to characterize differences in the oxidation state and local electronic structure for Pu compounds. The evolution of the Pu 4f core-level chemical shift as a function of sputtering depth profiling and hydrogen exposure at ambient temperature was quantified. The combination of the core–valence–valence Auger peak energies with the associated chemical shift of the Pu 4f photoelectron line defines the Auger parameter and results in a reliable method for definitively determining oxidation states independent of binding energy calibration. Results show that PuO{sub 2}, Pu{sub 2}O{sub 3}, PuH{sub 2.7}, and Pu have definitive Auger line-shapes. These data were used to produce a chemical state (Wagner) plot for select plutonium oxides. This Wagner plot allowed us to distinguish between the trivalent hydride and the trivalent oxide, which cannot be differentiated by the Pu 4f binding energy alone.},
doi = {10.1116/1.4913886},
journal = {Journal of Vacuum Science and Technology. A, Vacuum, Surfaces and Films},
issn = {0734-2101},
number = 3,
volume = 33,
place = {United States},
year = {2015},
month = {5}
}