Correlating nanoscale secondary ion mass spectrometry and atom probe tomography analysis of uranium enrichment in metallic nuclear fuel.

Accurate measurements of 235U enrichment within metallic nuclear fuels are essential for understanding material performance in a neutron irradiation environment, and the origin of secondary phases (e.g. uranium carbides). In this work, we analyse 235U enrichment in matrix and carbide phases in low enriched uranium alloyed with 10 wt% Mo via two chemical imaging modalities-nanoscale secondary ion mass spectrometry (NanoSIMS) and atom probe tomography (APT). Results from NanoSIMS and APT are compared to understand accuracy and utility of both approaches across length scales. NanoSIMS and APT provide consistent results, with no statistically significant difference between nominal enrichment (19.95 ± 0.14 at% 235U) and that measured for metal matrix and carbide inclusions.

[1]  M. Wallenius,et al.  Assessment of uranium inhomogeneity and isotope imaging for nuclear forensics , 2020 .

[2]  E. Steel,et al.  Atom Probe Mass Spectrometry of Uranium Isotopic Reference Materials , 2020, Analytical chemistry.

[3]  Dallas D. Reilly,et al.  Focused ion beam for improved spatially-resolved mass spectrometry and analysis of radioactive materials for uranium isotopic analysis. , 2020, Talanta.

[4]  D. Keiser,et al.  A novel approach to determine the local burnup in irradiated fuels using Atom Probe Tomography (APT) , 2020 .

[5]  Dallas D. Reilly,et al.  Characterization of slag and metal from uranium bomb reduction: Morphology, speciation, and the search for thorium , 2019 .

[6]  A. Devaraj,et al.  Nanoscale Spatially Resolved Mapping of Uranium Enrichment , 2019, Scientific Reports.

[7]  P. Weber,et al.  Microscale Isotopic Variation observed in Uranium Fuel Pellets with implications for Nuclear Forensics. , 2019, Analytical chemistry.

[8]  J. D. Fassett,et al.  Advances in age-dating of individual uranium particles by large geometry secondary ion mass spectrometry. , 2019, The Analyst.

[9]  A. Devaraj,et al.  Discontinuous Precipitation in U-10 wt.%Mo Alloy: Reaction Kinetics, Effect of Prior γ-UMo Microstructure, the Role of Grain-Boundary Misorientation, and the Effect of Ternary Alloying Addition , 2019, JOM.

[10]  L. Kovarik,et al.  Crystallographic and compositional analysis of impurity phase U2MoSi2C in UMo alloys , 2019, Journal of Nuclear Materials.

[11]  L. Kovarik,et al.  Phase transformation of metastable discontinuous precipitation products to equilibrium phases in U10Mo alloys , 2018, Scripta Materialia.

[12]  N. LaHaye,et al.  Optical spectroscopy of laser-produced plasmas for standoff isotopic analysis , 2018, Applied Physics Reviews.

[13]  V. Joshi,et al.  The effect of thermomechanical processing on second phase particle redistribution in U-10 wt%Mo , 2018 .

[14]  Ying Shirley Meng,et al.  Three-dimensional nanoscale characterisation of materials by atom probe tomography , 2018 .

[15]  T. P. Forbes,et al.  Considerations for uranium isotope ratio analysis by atmospheric pressure ionization mass spectrometry. , 2018, The Analyst.

[16]  C. D. Quarles,et al.  Laser ablation – inductively couple plasma – mass spectrometry/laser induced break down spectroscopy: a tandem technique for uranium particle characterization , 2017 .

[17]  C. Lavender,et al.  Evaluation of Uranium-235 Measurement Techniques , 2017 .

[18]  W. Setyawan,et al.  Formation mechanism of gas bubble superlattice in UMo metal fuels: Phase-field modeling investigation , 2016 .

[19]  Jay G. Tarolli,et al.  High resolution isotopic analysis of U-bearing particles via fusion of SIMS and EDS images , 2016 .

[20]  Shi-lun Guo,et al.  Studies on analyzing single uranium-bearing particle by FT-TIMS , 2013 .

[21]  D. Newbury,et al.  Postdetonation nuclear debris for attribution , 2010, Proceedings of the National Academy of Sciences.

[22]  D Lawrence,et al.  In situ site-specific specimen preparation for atom probe tomography. , 2007, Ultramicroscopy.

[23]  J. Becker Inductively coupled plasma mass spectrometry (ICP-MS) and laser ablation ICP-MS for isotope analysis of long-lived radionuclides , 2005 .