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Review of capture cross sections relevant for intentional nuclear forensics

The NA-22 Intentional Forensics Venture is developing a system for tagging nuclear fuel using various methods of information encoding. One of the main methods under development is the insertion of isotopically enriched tracers into the fuel. In order to aid in the understanding of the neutronic performance of these taggants, we assess the quality of the nuclear data underpinning simulations, which are driven by the neutron-capture cross sections. We present these cross sections of naturally occurring isotopes of the elements provided in the neutron sublibrary of the planned ENDF/B-VIII.1 Feb. 2023 library release. We make this assessment using a rubric designed for this effort, which quantifies orthogonal features related to the overall quality. The quality metric highlights 6 aspects: experimental data, resonance evaluations, integral metrics, covariances, fission products, and documentation. We focus on energy ranges relevant for reactor applications. We also discuss additional sources for new, high-quality cross-section data that may be utilized on the time scale of the venture, including existing global data, new experiments, and computational methods. Finally, overall outlook is presented with conclusions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

β- and γ-Counting for Pre-detonation Nuclear Forensics on Eu-155

Post-detonation nuclear forensics was performed at Los Alamos National Laboratory (LANL) on 155Eu, a fission product on the wing of the fission product production curve whose yield is sensitive to fission fuel and neutron energy. With a half-life of 4.753 years, 155Eu provides a longer-lived option for these measurements than other fission products with similar mass numbers. The Chemistry Division Group - Nuclear and Radiochemistry, at LANL routinely measures a suite of fission products from 235U fissions in thermal neutron flux experiments known as thermal calibration exercises, using a mixture of gas proportional β-decay counting and γ-spectrometry on HPGe detectors. The fission products of interest are reported relative to a high-yield reference fission product from the same sample to create a running average ratio specific to neutron energy and fuel type; Equation 1 below shows the ratio-of-ratios R-value measured fission products are reported in: R i x = [A( i X)/A( 99 Mo)] unknown [A( i X)/A( 99 Mo)] 235 U n,th where A denotes activity, i X is the nuclide of interest, and 235 U n,th denotes irradiations of 235 U with thermal neutrons. Measurements of unknown fission spectra are ratioed to a running-average of thermal calibration results, and the resulting R-value can be referred to as against a library of irradiation conditions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Assessment of the quality of nuclear data for stable oxygen isotopes for Intentional Forensics applications

The Intentional Forensics (IF) project seeks to design a suite of tagging materials that can be used to unobtrusively “barcode” nuclear fuel. The idea being that, if the fuel leaves institutional controls and is later recovered, the “barcode” can be used to determine the provenance of the fuel. The IF project is investigating several schemes for this “barcode” and taggants with tailored isotopic compositions are once leading concept. Recently 18 O was suggested as a potential taggant [IF2023]. This report assesses the quality of 16,17,18 O evaluations in the ENDF/B-VIII.0 library [ENDF8.0]. In a neutron-rich environment such as a nuclear reactor, we are interested in two main processes – neutron scattering and neutron absorption (or capture). For the typical neutron energies encountered in a reactor, absorption is determined exclusively by the neutron radiative capture cross section (in which a neutron is absorbed, and the residual nucleus emits one or more gamma rays). The capture cross sections are described by and can be completely determined from R-matrix parameters in the ENDF evaluations. Therefore, it is sufficient to consider the quality of the neutron resonance part of these evaluations. Neutron scattering is determined mainly by the elastic scattering cross section which is very similar for all oxygen isotopes and is essentially constant until around 100 keV. The cross section varies from 3-4 barns, depending on the isotope, and 16 O has the largest elastic cross section of all isotopes. Therefore, we expect that significant amounts of 17 O and 18 O could diminish the moderating role of oxygen in fuel. We note that, in traditional power reactor, the hydrogen in the coolant water provides the vast majority of the moderation in the reactor, so the impact of 17 O and 18 O in any taggant would be minimal. At higher energies, neutron resonances start to play a role and the R-matrix parameters determine the cross sections. Fig. 1 shows the mass region near stable oxygen isotopes. As nuclei capture neutrons, they transmute into a different isotope, one unit to the right. In particular, 16 O transmutes to 17 O, 17 O transmutes to 18 O and 18 O transmutes to 19 O. 19 O, being unstable, beta decays in 27 s to 19 F. So, even if the 18 O neutron capture data is good, the fact that it transmutes into 19 F may be problematic and needs investigation. Fig. 2 from [NuDat] shows the thermal neutron capture cross sections for all nuclei in the ENDF/B-VII.1 library [ENDF7.1]. Clearly oxygen thermal capture values are quite small compared to other nuclei. Note, there is no 18 O evaluation in the ENDF/B-VII.1 library. In any event, given that neutron capture events lower the reactor reactivity and potentially induce chemical changes in the fuel, we will focus our attention on the capture part of the neutron resonances.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

OPCW Twining Project Visit by the National Laboratory of Scientific and Technical Police (LNPST) to Lawrence Livermore National Laboratory Forensic Science Center (LLNL)

PURPOSE FOR TRIP Through the Organisation for Prohibition of Chemical Weapons (OPCW) Twinning and Assistance Program, Lawrence Livermore National Laboratory, Forensic Science Center (LLNL) has been paired with Morocco’s National Laboratory of Scientific and Technical Police (LNPST), with the goal of mentoring LNPST to become an OPCW Designated Laboratory. The purpose of this visit was for LLNL staff to mentor staff from LNPST as they participated in hands-on, laboratory-based exercises to analyze proficiency test samples prepared by LLNL. This visit was designed to help LNPST scientists strengthen their skills in OPCW proficiency testing.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Creation of Speed-of-Sound Inject Data for Technical Nuclear Forensics

Technical Nuclear Forensics (TNF) exercises simulate a detonation of a nuclear device within the United States, usually in a city. Speed-of-sound (SOS) phenomenology are the atmospheric overpressure and ground shock mechanical motions that are observed at over-pressure (air-blast and infrasound) and seismic sensors, respectively (Figure 1). Amplitudes of SOS data are related to the explosive yield (Kinney and Graham, 1985; Koper et al., 2002; Bonner et al., 2013ab; Ford et al., 2014, 2021; Templeton et al., 2018; Schnurr et al., 2020). Within the country, the United States Prompt Diagnostics System (USPDS) includes a network of geophysical sensors to capture such SOS signals. During the TNF exercise, the event data will be analyzed by the players who know nothing about the technical details of the source (e.g. location, yield, explosive). Specifically, they will use the Integrated Yield Determination Tool (IYDT) to estimate the yield and height-of-burst or depth-of-burial (HOB/DOB). The IYDT allows the user to measure features on the overpressure and seismic channels, evaluate the consistency of features and jointly estimate yield and HOB/DOB. For these exercises, SOS data are simulated for the location, emplacement and yield of the device and signals are propagated to the observing stations. This document describes the steps undertaken in the simulation, validation, preparation and verification of SOS signals for TNF exercises.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Measuring Very Low Radiation Doses in PTFE for Nuclear Forensic Enrichment Reconstruction

Every country that has made nuclear weapons has used uranium enrichment. Despite the centrality of this technology to international security, there is still no reliable physical marker of past enrichment that can be used to perform forensic verification of historically produced weapons. We show that the extremely low radioactivity from uranium alpha emissions during enrichment leaves detectable and irreversible calorimetric signatures in the common enrichment gasket material PTFE, allowing for historical reconstruction of past enrichment activities at a sensitivity better than one weapon's quantity of highly enriched uranium. Fast scanning calorimetry also enables the measurement of recrystallization enthalpies of sequentially microtomed slices, confirming the magnitude and the type of radiation exposure while also providing a detection of tampering and a method for analyzing field samples useful for treaty verification. This work opens the door for common items to be turned into precise dosimeters to detect the past presence of radioactivity, nuclear materials, and related activities with high confidence.

Connick, Rachel↗

Thermoluminescence: Potential Applications in Forensic Science

In crime laboratories one of the most difficult operations is to determine unequivocally whether or not two samples of evidence of the same type were originally part of the same thing or were from the same source. It has been found that high temperature thermoluminescence (room temperature to 723 K) can be used for comparisons of this type, although work to date indicates that there is generally a finite probability for coincidental matching of glass or soil samples. Further work is required to determine and attempt to minimize these probabilities for different types of materials, and to define more clearly the scope of applicability of thermoluminescence to actual forensic situations.

Ingham, J. D.↗

Relevant capture cross sections for intentional nuclear forensics, table summary

This summary provides a brief list of capture cross section metrics for naturally occurring isotopes for review by the Intentional Forensics Venture. This introduction is a companion to the column tabulated data, available in pdf and spreadsheet form. Cross section values for this summary list are taken from ENDF/B-VIII.0 and the development library for ENDF/B-VIII.1, with abundances taken from Nuclear Wallet Cards abundance tables. The cross section metrics are thermal cross section, resonance integral (RI), Maxwellian averaged cross section at 30 keV, and 252 Cf spontaneous fission spectrum averaged cross section. The isotopes are listed in order of Z, then A, with the elemental symbol also reported. This memo gives a brief introduction and overview of the data presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Gamma-ray spectrometry analysis methods for radioisotope dissolution and mixing for nuclear forensics applications

We report the production of surrogate nuclear explosive debris involves the dissolution of irradiated fissile material, elemental isolation, and recombination based on required fission product ratios. Gamma-ray spectrometry is used following each step to assess the radioactive fission product inventory. A high-purity germanium detector is used to measure each sample, and the detector efficiencies are determined prior to sample measurements. Through radiochemical techniques, elements are isolated and recombined into samples with specific fission product ratios. As a result, a matrix-based approach can account for imperfect chemical separations to calculate the proper mixture volumes to obtain intended volatile-to-refractory fission product ratios, or R-values.

07 ISOTOPE AND RADIATION SOURCES↗

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 ↗

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↗

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↗

Application of HRGS for forensic characterization of uranium oxides, pure uranium metals and uranium alloys

A nondestructive iterative method for uranium-bearing material characterization with HRGS developed earlier in (J. appl. Rad. Isotopes, 166 (2020) 109433) is applied to determine matrix densities and uranium isotope masses of a variety of uranium materials, namely uranium ore, UO 2 and U 3 O 8 powders, fuel elements in the form of UO2 microspheres, uranium metal and uranium alloys. It is shown that U 3 O 8 powders with uranium mass fraction of about 84% can be distinguished from the powders of UO 2 with uranium mass fraction of about 87%; uranium products in the form of liquid or loose powder with matrix density of 0.5-2.0 g/cm 3 can be distinguished from uranium products in the form of compacted fuel elements with matrix density of 6.0-10.0 g/cm 3 and from pure metal uranium and uranium alloys with matrix density of 14.0- 19.0 g/cm 3 . In fuel microspheres based on UO2 the uranium mass fraction 88.02% measured by HRGS is consistent, within the measurement uncertainties, with the results of isotope dilution mass spectrometry 87.76±0.64 % and also is confirmed by X-ray diffraction technique. The uranium mass fraction of the uranium ore estimated as 0.08% by HRGS is consistent, within the measurement uncertainties, with the value 0.09±0.01% determined with WDXRF. Densities of two different uranium metal samples, estimated as 18.42 g/cm 3 and 19.33 g/cm 3 by HRGS are consistent with values 18.24±0.55 g/cm 3 and 18.86±0.59 g/cm 3 , respectively, obtained by the gas pycnometry technique.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Structural features of early fuel cycle taggant incorporation for intentional nuclear forensics

To develop strategies for incorporating transition metal taggants (Fe, Cr, and Ni) into oxide fuels and to understand how these taggant candidates persist through early fuel cycle processes, synthetic procedures are modified from established production routes to yield intentionally tagged early fuel cycle intermediates including uranyl nitrate hexahydrate (UNH, UO 2 (NO 3 ) 2 ·6H 2 O), uranyl peroxide tetrahydrate (studtite, UO 2 O 2 ·4H 2 O), and uranyl peroxide dihydrate (metastudtite, UO 2 O 2 ·2H 2 O). First, Fe, Cr, and Ni nitrate solutions are introduced to an aqueous solution of UNH followed by precipitation to produce tagged UNH. Then, studtite is precipitated from UNH followed by dehydration to metastudtite. Structural influences of taggant incorporation within all synthesized phases are investigated using powder X-ray diffraction (PXRD) and Raman spectroscopy to provide insight into crystallographic modifications resulting from the addition of tags to these early fuel cycle materials and elucidate the chemical form of taggants introduced at these stages. The possibility of segregation of taggant species into discrete phases within U matrices was examined using scanning electron microscopy with energy dispersive X-ray spectroscopy. Taggant concentrations in solid-phase materials were determined using inductively coupled plasma-optical emission spectroscopy. Observations from Raman spectroscopy and PXRD indicate that introducing transition metal tags during uranyl nitrate precipitation results in potential impurity phase segregation in UNH, but transition metal incorporation is suggested by results for tagged uranyl peroxide materials. Further, results from this study will inform strategies for optimizing taggant incorporation in UO 2 .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Utilization of traceable standards to validate plutonium isotopic purification and separation of plutonium progeny using AG MP-1M resin for nuclear forensic investigations

Radio-chronometric studies on plutonium (Pu) materials require independent measurement of the Pu (parent) content and isotopic distribution as well as concentration and isotopic distribution of the plutonium isotopic decay products. We performed a series of experiments to demonstrate the consistency of separations using the Lewatit MP 800 macroporous anion exchange resin and the AG MP-1M resin with traceable Pu isotopic certified reference material (CRM) standards 136, 137, 138, and 126-A. Two different mesh-sizes of the AG MP-1M resin were tested and the 50–100 mesh size resin was found to work more efficiently for the separation task. Both Lewatit and AG MP-1M resins were found to perform satisfactorily for quantitatively extracting the americium (Am) and uranium (U) progeny as well as gallium (Ga) present as a tracer in the Pu material. Both resins were effective in removing isobaric interferences from the Pu fraction used in isotopic measurements by thermal ionization mass spectrometry (TIMS). To address the co-elution of uranium and gallium, Alizarin red S (ARS) was used as a colorimetric dye to determine the behavior of UO 2 2+ and Ga 3+ on AG MP-1M resin with various acidic solutions as eluents using UV–vis spectra. Poor resolution of these peaks complicated quantitative analysis by UV–vis spectroscopy, but these results were informative in planning automated separation experiments by HPLC. LA-UR-24-28919.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗