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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Verifying MCNP Models of the TEX High 240 Plutonium Benchmark

Computational modeling programs are invaluable tools that allow us to understand systems, safely develop new processes, and make reliable predictions about future designs. However, the effectiveness of these codes is limited by the degree to which their parameters match the real world. In the field of nuclear engineering, cross section data is one of these vital parameters. Accurate cross section data on important fissile and fissionable isotopes promotes the design of safer and more efficient fabrication, transportation, storage, and stockpiling of nuclear fuel. Unfortunately, there are knowledge gaps in data on key isotopes. In 2011, a multinational meeting hosted by the US Department of Energy Nuclear Criticality Safety Program ranked the priority of certain cross section data needs. In response, Lawrence Livermore National Lab (LLNL) designed the Thermal and Epithermal eXperiment (TEX) series of benchmark experiments. Benchmark experiments are used to validate current cross section data. They validate data by comparing the results of an actual experiment to the predicted results from a computational model. The data a benchmark applies to depends on the isotope and energy range the experiment’s neutron multiplication factor ( k eff ) is most sensitive to. The development and testing of the TEX High 240 Plutonium Benchmark will help validate 240 Pu cross section data. The configuration and materials of this benchmark are designed to be most sensitive to 240 Pu's intermediate energy range (from 0.625 ev to 100 keV ). MCNP® models of the assembly have been developed by LLNL and the results have been written in the final design report. In order for the discrepancies between benchmark models and experiments to be attributed to cross section inaccuracies, the accuracy of the models needs to be verified. The goal of this project is to verify of the results of LLNL's modeling by creating a new set of MCNP models and comparing the results.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Radiolytic degradation of 240 Plutonium and 242 Plutonium oxalates

Raman, FTIR, and diffuse reflectance spectroscopy were used to study the auto-radiolytic degradation of 240 Pu and 242 Pu oxalates. The significant differences in the lifetimes of 240 Pu and 242 Pu enabled the differentiation between environmental and radiolytic mechanisms. 240 Pu oxalates were observed to decompose to PuOCO 3 at intermediate times (~ 20 weeks) followed by partial conversion to PuO 2 at times greater than one year. Atmospheric oxidation was shown to be the primary decomposition mechanism for 242 Pu(IV) oxalate, and the alpha radiolysis of aquo and oxalate ligands serves as a secondary decomposition mechanism. In conclusion, this study offers a fresh perspective on radiolytic aging, which is crucial for long-term storage applications.

Analytical Techniques in Art Conservation↗
DOE OSTI2016

Surrogate Measurements of Actinide (n,2n) Cross Sections with NeutronSTARS

Directly measuring (n,2n) cross sections on short-lived actinides presents a number of experimental challenges. The surrogate reaction technique is an experimental method for measuring cross sections on short-­lived isotopes, and it provides a unique solution for measuring (n,2n) cross sections. This technique involves measuring a charged-­particle reaction cross section, where the reaction populates the same compound nucleus as the reaction of interest. To perform these surrogate (n,2n) cross section measurements, a silicon telescope array has been placed along a beam line at the Texas A&M University Cyclotron Institute, which is surrounded by a large tank of gadolinium-doped liquid scintillator, which acts as a neutron detector. The combination of the charge-particle and neutron-detector arrays is referred to as NeutronSTARS. In the analysis procedure for calculating the (n,2n) cross section, the neutron detection efficiency and time structure plays an important role. Due to the lack of availability of isotropic, mono-energetic neutron sources, modeling is an important component in establishing this efficiency and time structure. This report describes the NeutronSTARS array, which was designed and commissioned during this project. It also describes the surrogate reaction technique, specifically referencing a 235 U(n,2n) commissioning measurement that was fielded during the past year. Advanced multiplicity analysis techniques have been developed for this work, which should allow for efficient analysis of 241 Pu(n,2n) and 239 Pu(n,2n) cross section measurements

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Validation of MCNP6 Version 1.0 with the ENDF/B-VII.1 Cross Section Library for Plutonium Metals, Oxides, and Solutions on the High Performance Computing Platform Moonlight

This report documents a validation of the MCNP6 Version 1.0 computer code on the high performance computing platform Moonlight, for operations at Los Alamos National Laboratory (LANL) that involve plutonium metals, oxides, and solutions. The validation is conducted using the ENDF/B-VII.1 continuous energy group cross section library at room temperature. The results are for use by nuclear criticality safety personnel in performing analysis and evaluation of various facility activities involving plutonium materials.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2018

Formation of Superheavy Elements: Study Based on Dynamical Approach

Using multi-dimensional Langevin equations for the probability distribution of the distance between the surfaces of two approaching nuclei, we have studied the formation of superheavy elements via calculation of evaporation and fission cross sections of these elements. Evaporation residue cross sections have been calculated for the 1n, 2n, 3n, 4n, and 5n evaporation channels using one and four dimensional Langevin equations for the {sup 48}Ca+{sup 226}Ra, {sup 232}Th, {sup 238}U, {sup 237}Np, {sup 239,240,242,244}Pu, {sup 243}Am, {sup 245,248}Cm, {sup 249}Bk, and {sup 249}Cf reactions. Our results show that with increasing dimension of Langevin equations the evaporation residue cross section is increased. Also, obtained results based on fourdimensional Langevin are in better agreement with experimental data in comparison with one-dimensional model.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2015

Model development and data uncertainty integration

The effect of data uncertainties is discussed, with the epithermal neutron multiplicity counter as an illustrative example. Simulation using MCNP6, cross section perturbations and correlations are addressed, along with the effect of the 240 Pu spontaneous fission neutron spectrum, the effect of P(ν) for 240 Pu spontaneous fission, and the effect of spontaneous fission and (α,n) intensity. The effect of nuclear data is the product of the initial uncertainty and the sensitivity -- both need to be estimated. In conclusion, a multi-parameter variation method has been demonstrated, the most significant parameters are the basic emission rates of spontaneous fission and (α,n) processes, and uncertainties and important data depend on the analysis technique chosen.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Multiplicity Counting

This set of slides begins by giving background and a review of neutron counting; three attributes of a verification item are discussed: 240 Pu eff mass; α, the ratio of (α,n) neutrons to spontaneous fission neutrons; and leakage multiplication. It then takes up neutron detector systems – theory & concepts (coincidence counting, moderation, die-away time); detector systems – some important details (deadtime, corrections); introduction to multiplicity counting; multiplicity electronics and example distributions; singles, doubles, and triples from measured multiplicity distributions; and the point model: multiplicity mathematics.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2018

NPP Radwaste Activity Determination by the Correlation Method

A radwaste radiation-monitoring methodology based on correlations established between the activity of radionuclides and making it possible to determine the activity of hard-to-detect radionuclides ({sup 3}H, {sup 14}C, {sup 63}Ni, {sup 90}Sr, {sup 238}U, {sup 238,} {sup 239,} {sup 240}Pu, and others) in waste lots was investigated. An algorithm for compiling a list of radionuclides monitored during certification of the wastes, which is based on criteria for the wastes being radioactive and their classification, and requirements for the intermediate storage time and the half-life of radionuclides, and an algorithm for establishing the correlations between the specific activity of the reference and hard-to-detect radionuclides were developed in order to implement the methodology. The application of the criterion and algorithm to the wastes at the Novovoronezh NPP made it possible to compile a list of monitored radionuclides that agrees with the national operator in terms of handling radwastes and to establish the correlations between the activity of individual radionuclides and confirm the applicability of the methodology to radwaste from NPPs.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Excess Lead-210 and Plutonium-239+240: Two suitable radiogenic soil erosion tracers for mountain grassland sites

Highlights: • First application of excess Lead-210 as soil tracer in alpine grasslands. • {sup 239+240}Pu/{sup 137}Cs ratios indicated 75% Chernobyl contribution to {sup 137}Cs inventory. • {sup 239+240}Pu is compared to more mature radioisotopic tracers (i.e. {sup 210}Pb{sub ex} and {sup 137}Cs). • {sup 210}Pb{sub ex}, {sup 137}Cs and {sup 239+240}Pu yielded comparable estimates of soil redistribution. The expected growing population and challenges associated with globalisation will increase local food and feed demands and enhance the pressure on local and regional upland soil resources. In light of these potential future developments it is necessary to define sustainable land use and tolerable soil loss rates with methods applicable and adapted to mountainous areas. Fallout-radionuclides (FRNs) are proven techniques to increase our knowledge about the status and resilience of agro-ecosystems. However, the use of the Caesium-137 ({sup 137}Cs) method is complicated in the European Alps due to its heterogeneous input and the timing of the Chernobyl fallout, which occurred during a few single rain events on partly snow covered ground. Other radioisotopic techniques have been proposed to overcome these limitations. The objective of this study is to evaluate the suitability of excess Lead-210 ({sup 210}Pb{sub ex}) and Plutonium-239+240 ({sup 239+240}Pu) as soil erosion tracers for three different grassland management types at the steep slopes (slope angles between 35 and 38°) located in the Central Swiss Alps. All three FRNs identified pastures as having the highest mean (± standard deviation) net soil loss of −6.7 ± 1.1, −9.8 ± 6.8 and −7.0 ± 5.2 Mg ha{sup -1} yr{sup -1} for {sup 137}Cs, {sup 210}Pb{sub ex} and {sup 239+240}Pu, respectively. A mean soil loss of −5.7 ± 1.5, −5.2 ± 1.5 and-5.6 ± 2.1 was assessed for hayfields and the lowest rates were established for pastures with dwarf-shrubs (−5.2 ± 2.5, −4.5 ± 2.5 and −3.3 ± 2.4 Mg ha{sup -1} yr{sup -1} for {sup 137}Cs, {sup 210}Pb{sub ex} and {sup 239+240}Pu, respectively). These rates, evaluated at sites with an elevated soil erosion risk exceed the respective soil production rates. Among the three FRN methods used, {sup 239+240}Pu appears as the most promising tracer in terms of measurement uncertainty and reduced small scale variability (CV of 13%). Despite a higher level of uncertainty, {sup 210}Pb{sub ex} produced comparable results, with a wide range of erosion rates sensitive to changes in grassland management. {sup 210}Pb{sub ex} can then be as well considered as a suitable soil tracer to investigate alpine agroecosystems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

K West Basin Sand Filter Backwash Sample Analysis

A sand filter is used to help maintain water clarity at the K West Basin where highly radioactive sludge is stored. Eventually that sand filter will require disposal. The radionuclide content of the solids trapped in the sand filter will affect the selection of the sand filter disposal pathway. The Pacific Northwest National Laboratory (PNNL) was contracted by the K Basin Operations & Plateau Remediation Project (operations contractor CH2M Hill) to analyze the radionuclide content of the solids collected from the backwash of the K West Basin sand filter. The radionuclide composition in the sand filter backwash solids will be used by CH2M Hill to determine if the sand filter media and retained sludge solids will be designated as transuranic waste for disposal purposes or can be processed through less expensive means. On October 19, 2015, K Basin Operations & Plateau Remediation Project staff backwashed the sand filter into the North Load-Out Pit (NLOP) and immediately collected sample slurry from a sampling tube positioned 24 in. above the NLOP floor. The 764 g sand filter backwash slurry sample, KW-105 SFBW-001, was submitted to PNNL for analysis on October 20, 2015. Solids from the slurry sample were consolidated into two samples (i.e., a primary and a duplicate sample) by centrifuging and measured for mass (0.82 g combined – wet centrifuged solids basis) and volume (0.80 mL combined). The solids were a dark brown/orange color, consistent with iron oxide/hydroxide. The solids were dried; the combined dry solids mass was 0.1113 g, corresponding to 0.0146 weight percent (wt%) solids in the original submitted sample slurry. The solids were acid-digested using nitric and hydrochloric acids. Insoluble solids developed upon dilution with 0.5 M HNO 3 , corresponding to an average 6.5 wt% of the initial dry solids content. The acid digestate and insoluble solids were analyzed separately by gamma spectrometry. Nominally, 7.7% of the 60 Co was present in the insoluble solids; less than 1% of other gamma-emitters (i.e., 137 Cs, 154/155 Eu, and 241 Am) were present in the insoluble solids. Aliquots of the acid digestate were analyzed directly using gamma energy analysis (GEA) and after separations for 238 Pu, 239+240 Pu, 237 Np, and 241 Am radioisotopes using alpha energy analysis (AEA). The 90 Sr was measured by liquid scintillation counting (LSC) on the Sr-separated fraction. The plutonium isotopic distribution of the acid digestate was analyzed following Pu separations by thermal ionization mass spectrometry (TIMS). A table summarizes the results for the primary and duplicate samples. The 239+240 Pu concentration (µCi/g dry) relative to 90 Sr and to 137 Cs concentrations (µCi/g dry) was examined. The K West Basin sludge has a 239+240 Pu/ 90 Sr ranging from 0.1 to 1.2 and the 239+240 Pu/ 137 Cs ratio ranging from 0.10 to 0.47. In contrast, the sand filter backwash solids 239+240 Pu/ 90 Sr ratio was 10.6 and the 239+240 Pu/ 137 Cs ratio was 2.0. The ratio differences indicate a relative enhancement of the Pu concentration in the sand filter solids relative to the 137 Cs and 90 Sr sludge concentrations currently in the K West Basin. A dose-to-curie radioisotope evaluation of the sand filter waste form may need to consider this dissimilarity.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Analytic computation of average energy of neutrons inducing fission

The objective of this report is to describe how I analytically computed the average energy of neutrons that induce fission in the bare BeRP ball. The motivation of this report is to resolve a discrepancy between the average energy computed via the FMULT and F4/FM cards in MCNP6 by comparison to the analytic results.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2019

Spatiotemporal Distribution of {sup 241}Am in the Vicinity of the Waste Isolation Pilot Plant - 19543

Environmental monitoring around nuclear facilities is essential for characterizing the baseline conditions that are critical for identifying releases and quantifying their effects, should they occur, and for assessing post-closure performance. The spatiotemporal distribution and transport behavior of {sup 241}Am in the vicinity of a deep geologic repository for transuranic waste were assessed using data spanning the pre-operational phase to the present, including an accidental radionuclide release in 2014. The {sup 241}Am background values of 0.027±0.109 μBq/m{sup 3} (aerosols), and 0.061±0.065 Bq/kg (soil), as well as the {sup 241}Am/{sup 239+240}Pu ratios of 0.41±0.06 (aerosols) and 0.38±0.04 (soil), are similar to global fallout values. Pre-operations concentrations of {sup 241}Am show a strong seasonal dependence, attributed to resuspension of soils contaminated by global fallout, with no contribution from the upwind Project Gnome site ({sup 241}Am/{sup 239+240}Pu =0.24±0.08). During the 2014 accidental release, aerosol concentrations of {sup 241}Am briefly increased to 115.2 μBq/m{sup 3} at an onsite monitoring station, and 81.4 μBq/m{sup 3} at a station ∼1 km downwind of the exhaust shaft, changing the {sup 241}Am/{sup 239+240}Pu from ∼0.37 to ∼10. However, some four years later, conditions have returned to background. Almost 90% of the {sup 241}Am inventory is the 0-5 cm soil layer and there is no evidence of concentrations above regulatory standards, or that can be attributed to waste disposal operations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

A Rapid Sequential Separation Method for Determination of Actinides and TENORM in Fracking Wastes - 20223

With recent advances in unconventional drilling technology in the US and around the world, the risks of environmental contamination and exposure due to technologically enhanced naturally occurring radioactive materials (TENORM) from fracking wastes have also surfaced. Although the Permian Basin (southeastern New Mexico, western Texas) has long been a modest producer of oil, the advent of fracking technology a decade ago turned it into hot property for producers. A 2018 assessment of undiscovered, technically recoverable continuous oil and gas resources by the U.S. Geological Survey estimates an average 46.3 billion barrels of oil and 281 trillion cubic feet of gas. This is likely to increase the use of unconventional drilling and TENORM generation. TENORM concentrations in oil and gas exploration and production waste can be several hundred to several thousand times higher than background TENORM concentrations. Both the thorium and uranium decay chains contribute to airborne radionuclides arising from the radon gas escaping the ground and subsequently decaying as airborne particulates. Additionally, radon decay products {sup 210}Pb and {sup 210}Po can build up in scale on the internal surfaces of oil and gas handling pipes and in sludge in refineries, becoming potential inhalation and ingestion hazards for workers. Furthermore, southeastern NM is also home to world's only licensed and operating transuranic nuclear waste repository, the DoE's Waste Isolation Pilot Plant (WIPP). Plutonium isotopes ({sup 239+240}Pu) and {sup 241}Am, are expected to account for more than 99% of the total radioactivity scheduled for disposal in the WIPP repository. Thus, an improved understanding of the environmental fate and transport of TENORM, liberated by unconventional drilling, is essential to assess how best to protect individuals and the environment. In this context, accurate measurement of TENORM and actinides in environmental and biological samples is essential. In this presentation, a new sequential method for the separation and pre-concentration of actinides (Pu, Am, Np) and TENORM (Po, U and Th) derived from oil and gas exploration is proposed. The TEVA method involves a rapid co-precipitation step to remove matrix interferences from the samples, followed by plutonium oxidation state adjustment to Pu (IV) and an incubation period of ∼ 1 hour at 50-60 deg. C to allow the resultant Po (II) to oxidize into Po(IV). The polonium, neptunium, thorium and plutonium are then separated on a TEVA column, while americium and uranium are separated on a TRU column. After separation, the alpha counting source was prepared by micro-precipitation with copper sulfide (CuS) for polonium and neodymium fluoride (NdF{sub 3}) for actinides. The efficiency and reliability of the procedures were tested by analyzing filter, drinking water and frack sand samples. The method is simple, robust and can be performed quickly with excellent removal of interferences, high chemical recovery and very good alpha peak resolution. (authors)

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2016

MC{sup 2}-3/DIF3D Analysis of the ZPPR-15 Axial Expansion Experiments

The Zero Power Physics Reactor (ZPPR) fast critical facility at the Argonne National Laboratory-West (ANLW) site in Idaho was built in 1969 to obtain neutron physics information necessary for the design of fast breeder reactors. The ZPPR-15 phases A through D were part of a series of cores intended to model a 330 MWt Integral Fast Reactor (IFR) concept. The ZPPR-15 assembly consisted of an inner core zone, an outer core zone of higher fissile content, a thin radial blanket and a thick steel reflector. The inner and outer core zones were of approximately equal volumes. The core zones simulated a sodium-cooled, metal-fueled fast reactor with approximately 10 wt.% zirconium in the target fuel composition. Phases A and B simulated an equilibrium cycle UPu-Zr fuel core where plutonium created in the blankets was sufficient to negate the need for enriched {sup 235}U feedstock. Phase D simulated a beginning of life U-Zr fuel core with enriched uranium fuel although approximately 10% of the fuel in the outer zone of the Phase D core was plutonium because {sup 240}Pu was required to provide a neutron source for the modified source multiplication technique used for many reactivity worth measurements such as sodium void worth in ZPPR. Phase C simulated the intermediate state between beginning of life and equilibrium cycle conditions with 50% enriched uranium fuel and 50% plutonium fuel in the inner and outer core zones. These configurations represent the various stages of reactor operating conditions. Phase A did not contain zirconium (metal fuel is typically alloyed with Zr) while Phases B, C and D did contain zirconium although the limited plate inventory restricted the zirconium zone to the inner core zone. This set of experiments was performed between April 1985 and July 1986 and focused on validation of both the concept and modeling. In each phase, there were multiple loadings for sub-critical, critical, and with regard to this manuscript, axial expansion worth measurements. Combined, these cores can be used to assess the accuracy of physics codes and evaluated cross section data for IFR concept reactors. This paper presents a recent effort that was made on retrieving validation data from the ZPPR-15 experiments and on deterministic modeling and analysis using MC{sup 2}-3/DIF3D for code validation. Axial expansion experiments and ZPPR-15D loading 206 were selected for this analysis. An explicit modeling of the axial expansion (introduction of gaps between sections of drawer) of ZPPR-15D loading 206 yielded a 32% over-prediction in the worth of the axial expansion with the MC2-3/DIF3D models. This indicates a consistent bias between ZPPR-15B and ZPPR-15D with regard to the deterministic modeling of the experiments. As part of future work, we intend on investigating whether the cross section processing or homogenization model is to blame, but we note with such small changes in k-effective in a large model, it is rather difficult to obtain zero errors as is typical for other worth measurements. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2017

Post-Closure Environmental Sampling and Inspection at the Amchitka Island, Alaska, Site - 17251

In the 1960's and early 1970's, three underground nuclear tests were conducted on Amchitka Island, Alaska. In 1965, the US Department of Defense-in conjunction with the US Atomic Energy Commission (AEC)-conducted the first of these nuclear tests, Long Shot, to provide data that would improve US capabilities for detecting underground nuclear explosions. In 1969, AEC conducted the second test, Milrow, to explore the feasibility of detonating a much larger device. In 1971, AEC conducted the third test, Cannikin, which was the largest underground test ever conducted by the US. The Long-Term Surveillance Plan (LTSP) for the Amchitka, Alaska, Site details how the US Department of Energy Office of Legacy Management (LM) intends to fulfill its mission to protect human health and the environment at and around the Amchitka Island site. The LTSP calls for monitoring to be performed every 5 years, at least during the initial phase of the project. The purpose of the monitoring is to develop a baseline of activity concentrations for selected radionuclides in biota, water, and soil, both on Amchitka Island and at the reference location on Adak Island, approximately 322 kilometers (200 miles) northeast of Amchitka. In addition to the environmental monitoring activities, seven mud pit caps that contain diesel-contaminated soils are inspected. The plan for biological and water sampling (both seawater and freshwater) during the May 2016 sampling event was developed through close coordination with the primary stakeholders, including the Alaska Department of Environmental Conservation, the Aleutian Pribilof Islands Association, and the US Fish and Wildlife Service. The environmental sampling in 2016 is a continuation of LM's evaluation of Amchitka Island's environment. Previous results from similar monitoring programs in 2004 and 2011 indicate that the environment is not being impacted by radionuclide migration and uptake from the underground nuclear testing conducted beneath Amchitka Island; consequently, subsistence and commercial-catch seafood is safe for human consumption. The collection of biota samples (rockfish, Irish lords, greenling, and rockweed) for cesium-134 ({sup 134}Cs), cesium-137 ({sup 137}Cs), plutonium-239 ({sup 239}Pu), plutonium-240 ({sup 240}Pu), and freshwater and seawater samples for {sup 134}Cs, {sup 137}Cs, and tritium ({sup 3}H) was the primary objective of the 2016 sampling effort. Rockfish, Irish lords, and greenling are resident, nonmigratory fish species that spend their entire life cycle in the marine environment, and rockweed is an inter-tidal species that may concentrate cesium. The seawater samples were collected primarily to determine if leakage from the Long Shot detonation could be detected and, secondarily, to compare with the background seawater samples collected from Adak Island. Cesium isotopes are also being analyzed to better understand the potential impact that the Fukushima-Daiichi release might have on the Amchitka and Adak environments. The target detection limits used for the 2016 sampling are lower than those used in previous studies. The lower detection limits make it possible for LM to delineate background activity levels for the radionuclides of interest. Data from the 2016 sampling event go beyond assessing food safety and focus on detecting leakage from the underground nuclear explosions. Additionally, the baseline activity concentrations obtained for the reference area (Adak Island) will enable identification of quantitative statistical trends in the results of future sampling programs. Sampling programs conducted in 2021 and beyond will have an objective to assess the statistical trends of radioactivity levels in the Amchitka Island environment. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Measuring SNM Isotopic Distributions using FRAM

The first group of slides provides background information on the isotopic composition of plutonium. It is shown that 240 Pu is the critical isotope in neutron coincidence/multiplicity counting. Next, response function analysis to determine isotopic composition is discussed. The isotopic composition can be determined by measuring the net peak counts from each isotope and then taking the ratio of the counts for each isotope relative to the total counts for the element. Then FRAM (Fixed energy Response function Analysis with Multiple efficiencies) is explained. FRAM can control data acquisition, automatically analyze newly acquired data, analyze previously acquired data, provide information on the quality of the analysis, and facilitate analysis in unusual situations (non-standard energy calibrations, gamma rays from non-SNM isotopes, poor spectra (within limits)).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Expanded Intercomparison of Nuclear Data Libraries Using Jupiter and Jupiter High-240 Experiments

There is a limited availability of plutonium experiments with sensitivity to lead in the ICSBEP (International Handbook of Evaluated Criticality Safety Benchmark Experiments) Handbook. The Jupiter and Jupiter High-240 experiments were performed at the National Criticality Experiments Research Center as a collaborative effort between Los Alamos National Laboratory and the Japan Atomic Energy Agency to assess lead void coefficients in a plutonium-lead system containing weapons- and reactor-grade plutonium, respectively. Concurrent with benchmark development, an intercomparison of calculations using different nuclear data libraries has been performed to assess the usability of the experimental data for nuclear data adjustment in a “softer-that-fast” neutron energy spectrum. Eigenvalue calculations using MCNP with the ENDF/B-VIII.0 and TENDL-2021 nuclear data libraries calculate closest to the benchmark values for Jupiter. Calculations using JENDL-5 and ENDF/B-VIII.1 match best with the Jupiter High-240 values. Lead void worth calculations using the various nuclear data libraries are all within 3σ of their respective measured values. Perturbation studies between ENDF/B-VIII.0 and ENDF/B-VIII.1 demonstrate an approximate increase in calculated eigenvalues for the Jupiter series experiments by ~240 pcm for plutonium (mostly 239 Pu) and ~120 pcm for lead accompanied by a decrease contributed by ~113 pcm for copper and ~13 pcm for stainless steel. Nuclear data sensitivities and uncertainties investigated using Whisper show slightly lower sensitivity to scatter than a lead-reflected plutonium sphere but greater sensitivity to neutron capture. The sensitivities between Jupiter and Jupiter High-240 for lead are very similar for both ENDF/B-VIII.0 and ENDF/B-VIII.1 nuclear data. These benchmarks are more sensitive to neutron capture in lead than other plutonium benchmark experiments and would be useful for both lead and 240 Pu validation. In conclusion, with the high degree of compensating effects between copper, lead, and plutonium cross sections, additional isolated Pb-Pu and Cu-Pu benchmarks would be beneficial in improving these nuclear data.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Fissile Material Stockpile Declarations and Cooperative Nuclear Archaeology

With the beginning of the Cold War, the United States and the Soviet Union quickly began to produce fissile material (plutonium and highly enriched uranium, HEU) for military purposes on an industrial scale. By the mid-1950s, both countries were already making ton-quantities of fissile material per year to supply their growing nuclear arsenals. They were soon joined by the United Kingdom (1951), France (1955), China (1964), and Israel (1965)—and later by India, Pakistan, and finally North Korea. By the time most of these production efforts ended in the early 1990s, the global stockpile of military fissile material had reached fantastic levels. While the combined global nuclear weapon inventory had peaked at about 64,000 in 1986,1 the military fissile-material stockpile ultimately reached almost 2200 tons (240 tons of plutonium and 1960 tons of highly enriched uranium), which is sufficient to make about 200,000 simple nuclear weapons.2 Since the end of the Cold War, almost 700 tons of highly enriched uranium have been down-blended and other material is now reserved for naval fuel. Overall, the military material available for weapon purposes today is sufficient for more than 150,000 weapons (Figure 1).

Glaser, Alexander↗