Exercise Celestial Skónis: Part 1 – History, purpose, design and results of traditional forensic examinations of the 6th Collaborative materials exercise of the nuclear forensics International Technical Working Group

Schwantes, Jon M.; Corbey, Jordan F.; Marsden, Olivia J.

doi:10.1016/j.forc.2022.100424

Cited by 3 publications

(1 citation statement)

References 6 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Given the small quantities of material analyzed in this work, the ability to discern between similar but distinct chemical species at the micrometer scale is an ideal application of Raman spectroscopy. This optical vibrational spectroscopic technique is widely employed in analysis of materials encountered in the nuclear fuel cycle − and is used here to qualitatively examine chemical species resulting from calcination of UO 2 F 2 . Spectroscopic features of uranyl fluoride and its hydrolysis products are well documented, ,, likewise, the polymorphs of uranium oxides have been extensively examined in recent years due to their relevance in the nuclear fuel cycle. ,− …”

Section: Resultsmentioning

confidence: 99%

Uranium Single Particle Analysis for Simultaneous Fluorine and Uranium Isotopic Determinations via Laser-Induced Breakdown Spectroscopy/Laser Ablation–Multicollector–Inductively Coupled Plasma–Mass Spectrometry

Manard,

Quarles,

Bradley

et al. 2024

J. Am. Chem. Soc.

View full text Add to dashboard Cite

Uranyl fluoride (UO 2 F 2 ) particles (<20 μm) were subjected to first-of-its-kind analysis via simultaneous laser-induced breakdown spectroscopy (LIBS) and laser ablation multi-collector inductively coupled plasma−mass spectrometry (LA−MC−ICP− MS). Briefly, a nanosecond pulsed high-energy laser was focused onto the sample (particle) surface. In a single laser pulse, the UO 2 F 2 particle was excited/ionized within the microplasma volume, and the emission of light was collected via fiber optics such that emission spectroscopy could be employed for the detection of uranium (U) and fluorine (F). The ablated particle was simultaneously transported into the MC−ICP−MS for high precision isotopic (i.e., 234 U, 235 U, and 238 U) analysis. This method, LIBS/LA−MC−ICP−MS was optimized and employed to rapidly measure 80+ UO 2 F 2 particles, which were subjected to different calcination processes, which results in varying degrees of F loss from the individual particles. In measuring the particles, the average F/U ratios for the populations treated at 100 and 500 °C were 2.78 ± 1.28 and 1.01 ± 0.50, respectively, confirming loss of F through the calcination process. The average 235 U/ 238 U on the particle populations for the 100 and 500 °C were 0.007262 (22) and 0.007231 (23), which was determined to be <0.2% from the expected value. The 234 U/ 238 U ratios on the same particles were 0.000053 (11) and 0.000050 (10) for the 100 and 500 °C, respectively, <10% from the expected value. Notably, each population was analyzed in under 5 min, demonstrating the truly rapid analysis technique presented here.

show abstract

Section: Resultsmentioning

confidence: 99%

Uranium Single Particle Analysis for Simultaneous Fluorine and Uranium Isotopic Determinations via Laser-Induced Breakdown Spectroscopy/Laser Ablation–Multicollector–Inductively Coupled Plasma–Mass Spectrometry

Manard,

Quarles,

Bradley

et al. 2024

J. Am. Chem. Soc.

View full text Add to dashboard Cite

show abstract

Spatially Resolved Raman Spectroscopic Investigation of Uranyl Fluoride: A Case Study in the Importance of Instrument Optimization

Spano,

Andrews,

Miskowiec

et al. 2024

Appl Spectrosc

View full text Add to dashboard Cite

Raman spectroscopy is an emerging technique for rapid and nondestructive analysis of nuclear materials for forensic and nonproliferation applications as it is a powerful tool for distinguishing multiple chemical forms of materials with similar stoichiometries. Recent developments in spectroscopic software have enabled rapid data collection with high-speed Raman spectroscopic mapping capabilities. However, some uranium-rich materials are susceptible to degradation in humid air and/or laser-induced phase transformations. To mitigate environmental or measurement-related sample degradation of potential samples of interest, we have taken a systematic approach to define optimized data collection parameters for high-throughput measurements of uranyl fluoride (UO2F2), which is an important intermediate material in the nuclear fuel cycle. First, we systematically describe the influence of optical magnification (5× to 100×), laser power, and exposure time on obtained signal for identical particles of UO2F2 and find that at low laser power and exposure times, comparable signal is obtained regardless of optical magnification. Second, we ensure sample integrity during data collection, and third, collect spectroscopic maps that employ optimized parameters to reduce the time required to obtain spatially resolved spectroscopic information. Reductions of 90% and 99% in measurement times are discussed as they relate to differences in resolving spectroscopic features of particles in identical mapping areas. During this work, we found that additional data processing options were needed and thus developed a customized Python script for importing, processing, analyzing, and visualizing Raman spectroscopic map data.

show abstract

The Auger parameter and plutonium

Roussel

2024

MRS Bulletin

View full text Add to dashboard Cite

Exercise Celestial Skónis: Part 1 – History, purpose, design and results of traditional forensic examinations of the 6th Collaborative materials exercise of the nuclear forensics International Technical Working Group

Cited by 3 publications

References 6 publications

Uranium Single Particle Analysis for Simultaneous Fluorine and Uranium Isotopic Determinations via Laser-Induced Breakdown Spectroscopy/Laser Ablation–Multicollector–Inductively Coupled Plasma–Mass Spectrometry

Uranium Single Particle Analysis for Simultaneous Fluorine and Uranium Isotopic Determinations via Laser-Induced Breakdown Spectroscopy/Laser Ablation–Multicollector–Inductively Coupled Plasma–Mass Spectrometry

Spatially Resolved Raman Spectroscopic Investigation of Uranyl Fluoride: A Case Study in the Importance of Instrument Optimization

The Auger parameter and plutonium

Contact Info

Product

Resources

About