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At least 19 records

Benchmark of the Chlorine Worth Study Experiments in Support of Chlorine Nuclear Data Validation for Nuclear Criticality Safety

The Chlorine Worth Study (CWS) was a critical experiment to address an urgent need for thermal chlorine nuclear data validation in plutonium systems. This urgent need is tied directly to plutonium recycle and recovery operations in the plutonium facility at Los Alamos National Laboratory, where exceptionally conservative criticality safety limits are used because no credit is taken for the neutron capture by chlorine. The experiment used weapons-grade plutonium metal plates clad in stainless steel, known as the PANN (plutonium aluminum no nickel) ZPPR (zero power physics reactor) plates. The plutonium was reflected and moderated by high-density polyethylene and included combinations of polyvinyl chloride (PVC) and chlorinated polyvinyl chloride (CPVC) as absorbers. The experiment and benchmark included three configurations mimicking 30 g 239 Pu/L plutonium, 300 g 239 Pu/L plutonium, and 600 g 239 Pu/L plutonium in an aqueous chloride solution. Uncertainties in the benchmark included five broad categories: (1) criticality measurement, (2) mass and density, (3) dimensions, (4) material compositions, and (5) positioning. The largest contribution to the overall uncertainties for all three cases came from the material compositions, in particular the PVC and CPVC absorber compositions. A detailed model was created to be a near match (that is within expectations of transport code users) and a simplified model was created to minimize offset dimensions and expedite modeling for code validation. Sample calculations were completed in MCNP6.3 with ENDF/B-VIII.0 and ENDF/B-VII.1 nuclear data. For the detailed and simplified models, the average difference between the computed and experimental k eff was 951 pcm. CWS will serve as the key validation experiment for nuclear criticality safety in support of aqueous chloride operations. The sensitivity to the chlorine capture cross section is orders of magnitude greater than other existing benchmarks. The current limits, as defined by nuclear criticality safety, are 520 g Pu per batch, i.e. the minimum critical mass of the Pu solution infinitely reflected by water [Criticality Handbook: Volume II, (1969)]. This extremely conservative critical mass limit does not credit any neutron capture by chlorine (in particular neutron capture by 35 Cl) and greatly impedes the throughput required for current and future operations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Outcomes of WPEC SG47 on "Use of Shielding Integral Benchmark Archive and Database for Nuclear Data Validation"

The Working Party on International Nuclear Data Evaluation Co-operation Subgroup 47 (WPECSG47) entitled "Use of Shielding Integral Benchmark Archive and Database for Nuclear Data Validation" was organised from 2019 and 2022 with the objectives to promote more systematic and wider use of shielding benchmark experiments in nuclear data (ND) and transport code validation and development, to provide feedback on the Shielding Integral Benchmark Archive and Database (SINBAD), and to promote its further development in coordination with the Expert Group on Physics of Reactor Systems (EGPRS). Altogether 9 meetings, the large majority (8) held remotely, were organised during the past 3 years to discuss the experience on the use of SINBAD, evaluation of new benchmarks and improvements to be contributed to the database which was severely neglected and lacking maintenance over the past ← 10+ years. Several proposals for new or updated benchmark evaluation were presented and discussed, such as FNG copper, LLNL pulsed spheres, CIAE iron sphere, KFK 1977 gamma measurements, Rez Fe sphere, ASPIS, ORNL Oxygen broomstick, TIARA and others. Complementing the database with new features was also discussed, for example providing the nuclear data sensitivity profiles more systematically would facilitate and better guide the use of data. Information on the geometry, (radiation source) and materials available in CAD format is expected to allow an easier and less error prone reference for computational model preparation and a potential input to CAD based workflows. Inputs for various transport codes and other benchmark data from participants have been shared via the NEA GitLab which could hopefully in the future evolve and form a bases for critically checked and validated benchmark data. Future development of SINBAD will be monitored by EGPRS and the newly created SINBAD Task Force.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

An Alternative to Solution Experiments for Nuclear Data Validation: Reflection and Interaction of Juxtaposed Uranium (RAIJU) Experiment Design

The need for solution experiments was thoroughly discussed at the recent NCERC (National Criticality Experiments Research Center) Futures Meeting in September 2022 for multiple applications including criticality safety, training, and nuclear data. However, this capability does not exist anywhere in the United States. NCERC, located at the Nevada National Security Site and operated by LANL (Los Alamos National Laboratory) is the only general-purpose critical experiments laboratory in the United States. However, solution experiments are not authorized at NCERC, and obtaining that authorization would be too time consuming and costly to happen in the foreseeable future. An alternative is needed – an experimental configuration with the homogeneity of liquid experiments, but without being a liquid. This project, Reflection and Interaction of Juxtaposed Uranium (RAIJU) will fill the gap in capability within LANL, the U.S. Department of Energy, and the international community and will support current and future nuclear material processing needs.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Why Lady Godiva Should be Replaced as the Default Validation Experiment for U-235 Nuclear Data

For the past seven decades the Lady Godiva benchmark (HEU-MET-FAST-001) has been the primary experiment used for 235 U nuclear data validation. The papers associated with large nuclear data library releases such as ENDF/B-VII.1 and ENDF/B-VIII.0 refer to it frequently. The reasons why HEU-MET-FAST-001 has been used as the primary validation experiment for 235 U nuclear data validation will be discussed in the following section. However, as discussed among the benchmark community, the standards associated with International Criticality Safety Benchmark Evaluation Project (ICSBEP) evaluations have changed throughout time; this is subject of the OECD/NEA WPEC (Working Party on Nuclear Criticality Safety) Subgroup 8. HEU-MET-FAST-001 is an older benchmark (issued during the inaugural year of ICSBEP in 1996 with only minor revisions occurring since then) and (along with many of the other benchmarks from this era) does not meet the standards for a modern benchmark. This work explores why HEU-MET-FAST-001 is useful for 235 U nuclear data validation and discusses other alternative validation experiments.

07 ISOTOPE AND RADIATION SOURCES↗

IER-517: Molybdenum Optimized Benchmark System Demonstrating Integral Correlations (MOBY DICK)

Nuclear criticality experiments are essential to the validation of nuclear data used in simulation software. The quality of nuclear data becomes paramount as simulation software becomes more relied upon for criticality safety studies and designs of nuclear systems. To improve the quality of nuclear data, experimenters can design critical experiments that are sensitive to isotope reaction pairs in materials of interest. The efforts conducted by the Organisation for Economic Co-operation and Development - Nuclear Energy Agency (OECD-NEA) Working Party on Nuclear Criticality Safety (WPNCS) Subgroup 8: Preservation of Expert Knowledge and Judgement Applied to Criticality Benchmarks (SG8) to categorize benchmarks according to their usefulness for nuclear data validation have been of great importance. Based on the OECD studies benchmark experiments included in the International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook are concisely used by nuclear data evaluators, criticality safety engineers and others to validate nuclear data and simulation results. A lack of benchmarks sensitive to molybdenum in the (ICSBEP), particularly in the intermediate range, was noted by Los Alamos National Laboratory (LANL), the French Institut de Radioprotection et de Sûreté Nucléaire (IRSN), and Y-12 National Security Site prompting them to submit a joint integral experiment request to the Nuclear Criticality Safety Program (NCSP) in 2019. The request included both HEU and Plutonium systems in order to validate differential nuclear data focusing on the intermediate energy range but also includes thermal and fast configurations. This document represents the preliminary design work for a series of molybdenum integral experiments known as Molybdenum Optimized Benchmark System Demonstrating Integral Correlations (MOBY DICK).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Reaction Rate Ratios for Recent Fast Metal Experiments with Large Plutonium Masses

Reaction rate ratios are integral responses that are used within the criticality experiments field because they contain spectral information. While these types of measurements have been utilized for nuclear data validation with historic experiments, few experiments of this type have been utilized for recent experiments, as few exist. This work focuses on measured reaction rate ratios for two nearly bare plutonium critical assemblies with different geometries: one that is cube like (with a Pu mass of 40 kg) and one that is slab like (with a Pu mass of 109 kg). Irradiations were performed with both configurations in which foils were placed near the center of the assembly. Plutonium, highly enriched uranium, depleted uranium, and Au foils were included in the irradiation and counted via high-purity germanium detectors. From these measurements, reaction rate ratios were calculated. Measured and simulated values and uncertainties are presented for the reaction rate ratios. Ratios utilizing the following reactions are given in this work: 197 Au(n, γ), 197 Au(n,2n), 235 U(n,fission), 238 U(n, fission), 238 U(n,2n), 238 U(n,γ), and 239 Pu(n,fission). Uncertainties for the measured reaction rate ratios ranged from 4% to 7%, and the contribution of various parameters to this uncertainty was investigated. The results are compared to historical experiments and should be used for nuclear data validation for future nuclear data library releases. These measurements are part of the EUCLID (Experiments Underpinned by Computational Learning for Improvements in Nuclear Data) project, which utilizes measurement responses in addition to k eff (such as these reaction rate ratios) to help reduce uncertainties in 239 Pu nuclear data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Neutron Leakage Spectra of the EUCLID Experiment [Abstract]

Integral experiments with sub-critical and critical configurations of special nuclear material are performed in support of nuclear data validation and adjustment. Different nuclear data evaluations may have different values for individual cross sections due to uncertainties in (or lack of) differential experiments, but compensating errors in these data sets can lead to the same k eff results for one application while vastly different for another application. One example of this is 239 Pu, where both ENDF/B-VIII.0 and JEFF-3.3 correctly compute k eff of the Jezebel critical assembly, but the individual contributions from each reaction are vastly different. To help resolve this specific case, the Experiments Underpinned by Computational Learning for Improvements in Nuclear Data (EUCLID) project used machine learning to design a set of experiments to help resolve the compensating errors in 239 Pu. A total of six responses were measured during the experimental campaign, which constrain the data in ways that k eff alone cannot and will be used for adjustment of the nuclear data. One of these responses is the neutron leakage spectrum, which recent work has shown to be useful for constraining the prompt fission neutron spectrum and inelastic scattering. The neutron leakage spectra were measured utilizing a 3 in. right cylinder EJ-301D detector. The measured signal in the detector was deconvoluted using spectrum unfolding techniques, which are presented and compared to simulations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Chlorine Validation through Critical Integral Experiments

An increased interest in the validation of chlorine nuclear data, specifically 35Cl, in recent years has led to the prioritization of conducting chlorine critical experiments for nuclear data validation and criticality safety evaluations. A previous experiment was conducted with PVC and CPVC (chlorinated polyvinyl chloride) to reduce the margin of subcriticality for PF-4 operations with aqueous plutonium chloride solutions. Challenges in determining the composition of specific polymers, namely the CPVC, made it difficult to characterize, and therefore benchmark. Additional materials that were utilizable for chlorine validation were not immediately clear, as form, strength, purity, and composition are all important. A series of possible absorber materials were identified and studied, but ultimately granular sodium chloride was chosen. In addition to the needs of LANL’s PF-4 other industry collaborators have brought attention to the need for chlorine validation. Specifically, the need for HEU electrorefining with LiCl salts at Y-12 was taken into consideration for this experiment, with the experimental configurations being finely tuned to best meet their needs. Needs for validation were also presented by Idaho National Lab (INL) and TerraPower for validation of their Molten Chloride Reactor Experiment (MCRE) and Molten Chloride Fast Reactor (MCFR) and have also been considered.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Why the US Needs an Enduring Plutonium Critical Assembly

Jezebel (operated from 1954-1977) has been the primary experiment for fast 239 Pu nuclear data validation for the last 70 years. Validation has included not only k eff , but also spectral indicies, Rossi-α, reactivity coefficients, and neutron leakage spectra. While this has been incredibly valuable to the community, there are three major issues. The first issue is that documentation on many of these experiments were lacking, leading to large uncertainties or (even worse) incorrect assumptions. The second issue is that while there have been many advances in research, there is no way to test those new advances today. The last issue is that since the assembly only operated for 23 years (and at time when 30 other critical assemblies were operating at the same facility and nuclear weapons testing was occurring), there were limited opportunities to observe how any system parameters changed as a function of time. Note that this work is not suggesting that a "Jezebel re placement" used for a limited experiment campaign would have great value. A new enduring (100 year target) plutonium (Pu) assembly with simple geometry and low uncertainties, however, would be extremely valuable. Such a capability would have a transformative impact on many research areas including nuclear data validation, analytical methods validation, dosimetry, reactor kinetics, and materials. The need for a new plutonium assembly is not new: it has been in the DOE Nuclear Criticality Safety Program (NCSP) Mission and Vision for over 10 years and was also the top priority established at the 2022 National Criticality Experiments Research Center (NCERC) Futures meeting. This work will discuss how such a new capability would help ensure that the US retains international leadership in plutonium research. Last, a brief overview of Lilith, a project aimed to design a new enduring plutonium assembly for operation at the NCERC will be given.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Nuclear Criticality Safety Integral Experiment Covariance Determination

Integral benchmarks for criticality safety and nuclear data validation require expensive uncertainty quantification studies. Commonly, the uncertainty quantification ignores correlations between experiments that share components. Experiments such as the TEX (Thermal/Epithermal eXperiments) campaigns consist of many shared parts between experiments, such as fuel, which creates a strong correlation in their errors. While these correlations are known to exist, they are often not estimated due to the complexity of such calculations. This paper describes a software package that uses an intuitive method of determining the covariance for each of the experimental components, providing a correlation matrix for each family of parts across the multiple cases examined within a benchmark. The code uses the TEX-HEU campaign as a proof of concept, and we show that the correlations can be calculated with information commonly found in ICSBEP (International Criticality Safety Benchmark Evaluation Project) benchmarks. The estimated covariances are used in χ 2 trending studies to evaluate their impact on nuclear data validation. The covariance determination code can be easily integrated into current benchmark evaluations as well as reevaluating legacy benchmark uncertainties. Uncertainty correlation calculations should become the baseline for criticality safety integral experiment benchmarks and can now be easily calculated with the described software package.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nuclear Criticality Safety Integral Experiment Covariance Determination

Integral benchmarks for criticality safety and nuclear data validation require expensive uncertainty quantification studies. Commonly, the uncertainty quantification ignores correlations between experiments that share components. Experiments such as the TEX (Thermal/Epithermal eXperiments) campaigns consist of many shared parts, such as fuel, which create a strong correlation in their uncertainties. While these correlations are known to exist, they are often not estimated due to the complexity of such calculations. This paper describes a software package that uses an intuitive method of determining the covariance for each of the experimental components, providing a correlation matrix for each family of parts across the multiple cases examined within a benchmark. The code uses the TEX-HEU campaign as a proof of concept, and we show that the correlations can be calculated with information commonly found in ICSBEP (International Criticality Safety Benchmark Evaluation Project) benchmarks. The estimated covariances are used in χ 2 trending studies to evaluate their impact on nuclear data validation. Without covariances, χ 2 per degree of freedom was calculated as 2.203 and with covariances it was 1.179. The difference shows that omitting covariance information may cause overly pessimistic bias quantifications. The covariance determination code can be easily integrated into current benchmark evaluations as well as reevaluating legacy benchmark uncertainties. Uncertainty correlation calculations should become the baseline for criticality safety integral experiment benchmarks and can now be easily calculated with the described software package.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Experimental Covariance Determination for Critical Integral Experiments

Integral benchmarks for criticality safety and nuclear data validation require expensive uncertainty quantification studies. In general, uncertainty quantification techniques ignore correlations between experiments and shared parts. Experiments, such as the TEX (Thermal/Epithermal eXperiments) campaigns, consist of many shared parts, such as the ‘Jemima’ HEU fuel plates, which create a strong correlation in their uncertainties. While these correlations are known to exist, they are often not estimated due to the complexity of such calculations. This paper describes an intuitive method of determining the covariance for each of the experimental components, providing a correlation for each family of parts across the multiple cases examined within a benchmark. A proof-of-principle study using the TEX-HEU experimental campaign was performed and verified that the correlations can be calculated with information commonly found in the ICSBEP (International Criticality Safety Benchmark Evaluation Project) benchmarks. This study showed that the introduction of model and experimental covariances reduces the χ 2 per degree of freedom from 2.203 to 1.179, indicating that the omission causes overly pessimistic bias quantifications. This technique can be seamlessly integrated to current benchmark evaluations as well as reevaluations of legacy benchmarks.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Jemima Plate Characterization

The HEU Jemima plates have been utilized in numerous International Criticality Safety Benchmark Evaluation Project (ICSBEP) evaluations. ICSBEP evaluations are a vital com ponent of nuclear data validation for applications across the nuclear community. In the past, different combinations of mass, caliper measurements, and drawing dimensions have been used to define the HEU Jemima plates in ICSBEP evaluations. Some of these combinations result in large density ranges (17 g/cm 3 to 19 g/cm 3 ) or unrealistic densities (greater than 19 g/cm 3 ). Additionally, oxidation of the plates has led to questioning the flatness of each plate, which can add additional gaps in experiment configurations. This work proposes a standardized method of defining the commonly used HEU Jemima plates across different experiments.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗