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At least 163 records · Page 9

Nuclear Forensics at Los Alamos National Laboratory

The overview of this presentation is: (1) Introduction to nonproliferation efforts; (2) Scope of activities at Los Alamos National Laboratory; (3) Facilities for radioanalytical work at LANL; (4) Radiochemical characterization capabilities; and (5) Bulk chemical and materials analysis capabilities. Some conclusions are: (1) Analytical chemistry measurements on plutonium and uranium matrices are critical to numerous defense and non-defense programs including safeguards accountancy verification measurements; (2) Los Alamos National Laboratory operates capable actinide analytical chemistry and material science laboratories suitable for nuclear material forensic characterization; (3) Actinide analytical chemistry uses numerous means to validate and independently verify that measurement data quality objectives are met; and (4) Numerous LANL nuclear facilities support the nuclear material handling, preparation, and analysis capabilities necessary to evaluate samples containing nearly any mass of an actinide (attogram to kilogram levels).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Comparing multiple statistical methods for inverse prediction in nuclear forensics applications

Forensic science seeks to predict source characteristics using measured observables. Statistically, this objective can be thought of as an inverse problem where interest is in the unknown source characteristics or factors ( X ) of some underlying causal model producing the observables or responses (Y = g ( X ) + error ). Here, this paper reviews several statistical methods for use in inverse problems and demonstrates that comparing results from multiple methods can be used to assess predictive capability. Motivation for assessing inverse predictions comes from the desired application to historical and future experiments involving nuclear material production for forensics research in which inverse predictions, along with an assessment of predictive capability, are desired.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

A Study of Fission Modes to Improve Nuclear Forensics

Obtain and evaluate charge and mass distributions from various databases and the literature Establish the mathematical formulism to decompose the selected mass distributions into their respective components of the multimodal fission models Compare and evaluate the results with prior work available from the literature Obtain, evaluate/validate experimentally-measured, photofission mass distributions using complementary INL-led research Apply decomposition methods to the photofission mass distributions Evaluate peak-to-valley ratios and specific isotopic ratios as a function of excitation energies Report and publish appropriate findings

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Round-robin 230 Th– 234 U age dating of bulk uranium for nuclear forensics

In an inter-laboratory measurement comparison study, four laboratories determined 230 Th– 234 U model ages of uranium certified reference material NBL U050 using isotope dilution mass spectrometry. The model dates determined by the participating laboratories range from 9 March 1956 to 19 October 1957, and are indistinguishable given the associated measurement uncertainties. As a result, these model ages are concordant with to slightly older than the known production age of NBL U050.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Micro-Analysis of Actinide Minerals for Nuclear Forensics and Treaty Verification

Micro-Raman spectroscopy has been demonstrated to be a viable tool for nondestructive determination of the crystal phase of relevant minerals. Collecting spectra on particles down to 5 microns in size was completed. Some minerals studied were weak scatterers and were better studied with the other techniques. A decent graphical software package should easily be able to compare collected spectra to a spectral library as well as subtract out matrix vibration peaks. Due to the success and unequivocal determination of the most common mineral false positive (zircon), it is clear that Raman has a future for complementary, rapid determination of unknown particulate samples containing actinides.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Nuclear Forensics Analysis with Missing and Uncertain Data

We have applied a new imputation-based method for analyzing incomplete data, called Monte Carlo Bayesian Database Generation (MCBDG), to the Spent Fuel Isotopic Composition (SFCOMPO) database. About 60% of the entries are absent for SFCOMPO. The method estimates missing values of a property from a probability distribution created from the existing data for the property, and then generates multiple instances of the completed database for training a machine learning algorithm. Uncertainty in the data is represented by an empirical or an assumed error distribution. The method makes few assumptions about the underlying data, and compares favorably against results obtained by replacing missing information with constant values.

97 MATHEMATICS AND COMPUTING↗

International cooperation in age-dating uranium standards for nuclear forensics using the 231 Pa/ 235 U radiochronometer

During 2017–2018 Los Alamos National Laboratory, Lawrence Livermore National Laboratory and the China Institute of Atomic Energy collaborated in an interlaboratory 231 Pa/ 235 U radiochronometry exercise. The laboratories used different analytical methods to obtain a consensus model purification date for CRM U010 of December 28, 1958 ± 198 days and for CRM U850 of May 20, 1958 ± 363 days. These results agree with previously reported model dates using the 230 Th/ 234 U radiochronometer as well as the production histories of these materials. The concordance of interlaboratory data here confirms the ability of laboratories to make reproducible radiochronometry measurements using distinct analytical approaches.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Results from a controlled depleted uranium metal casting experiment designed to investigate nuclear Forensic Radiochronometry Signatures

The accurate interpretation of uranium metal 230 Th/ 234 U and 231 Pa/ 235 U radiochronometry model ages requires an understanding of how uranium parent nuclides and decay progeny ( 230 Th and 231 Pa) behave during uranium metal casting. In order to directly measure the spatial distribution of 230 Th and 231 Pa in uranium metal before and after vacuum induction melting (VIM), Los Alamos National Laboratory identified uranium metal feedstock, characterized the metal feedstock, conducted a controlled casting experiment of an approximately 120 kg uranium metal rod, and characterized the cast metal. Herein this study presents radiochronometry results and quantified 230 Th and 231 Pa VIM separation factors from bulk uranium.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Exploring the use of thorium isotope compositions and concentrations as nuclear forensic signatures for uranium ore concentrates

This interlaboratory study measured thorium concentrations and isotope compositions in uranium ore concentrates from different geographical locations to examine whether thorium impurities may be useful forensic signatures for uranium ore concentrates found out of regulatory control. Measured 230 Th/ 232 Th in fifteen uranium ore concentrates record over three orders of magnitude of compositional variation. Results demonstrate that 230 Th/ 232 Th used in combination with U/Th ratios resulted in a unique signature for individual uranium ore concentrates from different processing locations. Data presented here suggest potential for 230 Th/ 232 Th and U/Th to be used as comparative signatures to investigate the provenance of seized uranium ore concentrates.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Age determination of a 75 Se gamma radiography source for nuclear forensics

Here, two methods were used to evaluate the age of 75 Se sealed source material. Both methods utilized gamma spectroscopy to determine the quantity of parent 75 Se present, but they differed in the technique used to determine the quantity of daughter 75 As. In one method, 75 As was quantified using inductively coupled plasma-mass spectrometry (ICP-MS) after using chromatographic techniques to separate the parent and daughter isotopes. In the other method, total As was measured using optical emission spectroscopy (OES), which did not require separation prior to measurement. The OES method was faster and gave slightly lower uncertainties, but required more daughter material to be present because of higher concentration requirements, making it unsuitable for young material. Both methods are hampered by the monoisotopic nature of As, but still gave reasonable model ages that were in agreement with each other.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Post detonation nuclear forensics

The problem of working backwards from the debris of a nuclear explosion to attempt to attribute the event to a particular actor is singularly difficult technically. However, moving from physical information of any certainty through the political steps that would lead to national action presents daunting policy questions as well. This monograph will outline the operational and physical components of this problem and suggest the difficulty of the policy questions that remain.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗