skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Raman microspectroscopy of PuO 2 particulate aggregates

Abstract

Raman microspectroscopy is a useful technique with the capability to infer local physical properties of materials such as crystalline order. Crystalline order and morphology of plutonium dioxide (PuO 2) grains and aggregates are known to be sensitive to the initial production conditions and represent the baseline for understanding subsequent signatures. PuO 2 samples were synthesized and then characterized by scanning electron microscopy prior to Raman analysis. A total of nine laser excitation wavelengths (785, 633, 561, 514, 488, 457, 405, 325 and 244 nm) were evaluated to maximize signal and minimize fluorescence, with 514 nm selected for most subsequent work. The effect of laser-induced heating and annealing on the Raman spectra were investigated with a 514 nm laser beam. The ratio of the Stokes and anti-Stokes band intensities was used to estimate the temperature during the laser-induced heating process. The band position and the band full-width at half-maximum (FWHM) were used to track the degree of sample annealing at an estimated temperature. The Raman spectra showed that laserinduced annealing resulted in significant enhancement of the intensity for most spectral bands. Similarly, the FWHM of most bands decreased with increasing annealing temperature. The largest Raman shift of the T 2g bandmore » for an annealed sample was measured at 480 cm -1. A new, sharp band at 1047 cm -1 emerged during the material annealing process and the intensity grew proportional to the intensity of the T 2g band. Crystal Field Theory computational analysis suggests the 1047 cm -1 band is the long sought Γ 1 → Γ 4 electronic transition proposed by several researchers. The data acquired in this work helps to explain the variability in band position and FWHM reported in the literature, including the assignment of new weak bands associated with Raman resonance and Raman electronic transitions.« less

Authors:
 [1];  [1];  [1]; ORCiD logo [1]
  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1488665
Alternate Identifier(s):
OSTI ID: 1487370
Report Number(s):
SRNL-STI-2018-00056
Journal ID: ISSN 0022-3115; PII: S0022311518302277
Grant/Contract Number:  
AC09-08SR22470; SR15-Pu_Oxide_Studies-NDD3b
Resource Type:
Published Article
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 515; Journal ID: ISSN 0022-3115
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Villa-Aleman, Eliel, Bridges, Nicholas J., Shehee, Thomas C., and Houk, Amanda L. Raman microspectroscopy of PuO2 particulate aggregates. United States: N. p., 2018. Web. doi:10.1016/j.jnucmat.2018.12.022.
Villa-Aleman, Eliel, Bridges, Nicholas J., Shehee, Thomas C., & Houk, Amanda L. Raman microspectroscopy of PuO2 particulate aggregates. United States. doi:10.1016/j.jnucmat.2018.12.022.
Villa-Aleman, Eliel, Bridges, Nicholas J., Shehee, Thomas C., and Houk, Amanda L. Sat . "Raman microspectroscopy of PuO2 particulate aggregates". United States. doi:10.1016/j.jnucmat.2018.12.022.
@article{osti_1488665,
title = {Raman microspectroscopy of PuO2 particulate aggregates},
author = {Villa-Aleman, Eliel and Bridges, Nicholas J. and Shehee, Thomas C. and Houk, Amanda L.},
abstractNote = {Raman microspectroscopy is a useful technique with the capability to infer local physical properties of materials such as crystalline order. Crystalline order and morphology of plutonium dioxide (PuO2) grains and aggregates are known to be sensitive to the initial production conditions and represent the baseline for understanding subsequent signatures. PuO2 samples were synthesized and then characterized by scanning electron microscopy prior to Raman analysis. A total of nine laser excitation wavelengths (785, 633, 561, 514, 488, 457, 405, 325 and 244 nm) were evaluated to maximize signal and minimize fluorescence, with 514 nm selected for most subsequent work. The effect of laser-induced heating and annealing on the Raman spectra were investigated with a 514 nm laser beam. The ratio of the Stokes and anti-Stokes band intensities was used to estimate the temperature during the laser-induced heating process. The band position and the band full-width at half-maximum (FWHM) were used to track the degree of sample annealing at an estimated temperature. The Raman spectra showed that laserinduced annealing resulted in significant enhancement of the intensity for most spectral bands. Similarly, the FWHM of most bands decreased with increasing annealing temperature. The largest Raman shift of the T2g band for an annealed sample was measured at 480 cm-1. A new, sharp band at 1047 cm-1 emerged during the material annealing process and the intensity grew proportional to the intensity of the T2g band. Crystal Field Theory computational analysis suggests the 1047 cm-1 band is the long sought Γ1 → Γ4 electronic transition proposed by several researchers. The data acquired in this work helps to explain the variability in band position and FWHM reported in the literature, including the assignment of new weak bands associated with Raman resonance and Raman electronic transitions.},
doi = {10.1016/j.jnucmat.2018.12.022},
journal = {Journal of Nuclear Materials},
number = ,
volume = 515,
place = {United States},
year = {2018},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1016/j.jnucmat.2018.12.022

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share: