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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Effect of Plutonium on Uranium Oxide Microstructural Fingerprint

The analysis of particulates from environmental sampling is routinely performed for nuclear forensics applications. In order to increase the tools available for nuclear forensics applications, capability development materials (CDMs), or reference particulates, are necessary for developing and benchmarking new analytical methods. Historically, these CDM particulates have been produced with highly controlled and characterized isotopic and size parameters for applications in developing and benchmarking particle sizers and mass spectrometry analytical methods [1- 4]. However, the development of CDMs with highly characterized particle morphology and phase of the particles is vital for aiding in the development and benchmarking of particle analytical methods for those parameters. In many cases, key properties such as crystallographic phase, morphology, and microstructure, may be correlated to processing history of environmental sampling particulates [5]. To that end, this work investigates determining the structural fingerprint of produced Pu-doped uranium oxide CDMs using transmission electron microscopy (TEM). The particulates, one of which shown in Figure 1, were synthesized to Fig. 1. Single particulate of uranium oxide fabricated using the THESEUS technique. develop capabilities for environmental sampling investigations. These particles are monodisperse at diameter of 1 μm and a range of plutonium concentrations from 0- 1,000 ppm. Given their small diameter, TEM analysis was ideal for studying the particulate structural fingerprint in detail. Previous investigations confirmed the external homogeneity of the particulates at different plutonium concentrations, however this analysis focuses on determining the grain structure, phase distribution, and porosity of the particulates.

Mayer, Jack [Univ. of Florida, Gainesville, FL (Un↗
DOE OSTI2022

Evaluated 238 U(n,f) Average Prompt Fission Neutron Multiplicities Including the CGMF Model

This report documents an evaluation of the average prompt fission neutron multiplicity, $\overline{v}_p$, of 238 U from 800 keV to MeV. This evaluation had to be re-done from “scratch” as the input to previous $\overline{v}_p$ evaluations, specifically ENDF/B-VIII.0, was not found. That means that all available experimental data were re-analyzed and uncertainties were re-estimated. The new evaluated 238 U $\overline{v}_p$ based on only experimental data differs distinctly from ENDF/B-VIII.0 $\overline{v}_p$ from 2 to 4.5 MeV, and from 6 to 7 MeV, and is otherwise similar. The difference from 2 to 4.5 MeV stems from the fact that ENDF/B-VIII.0 was tweaked in this energy range to data of Frehaut, while two other, equally trustworthy, data sets would indicate an evaluated 238 U $\overline{v}_p$ that is up to 2% higher. Also, second chance fission in ENDF/B-VIII.0 was smoothed over from 6–7 MeV. Another major difference to ENDF/B-VIII.0 is that one of the evaluations presented here includes model information from the Hauser-Feshbach fission fragment decay code CGMF, while ENDF/B-VIII.0 is based purely on experimental data. CGMF links several fission quantities with each other; $\overline{v}_p$ is predicted by assumptions made on, e.g., pre-neutron emission yields as a function of mass, the total kinetic energy, or spin and parity of fission fragments. This allows to validate the new 238 U $\overline{v}_p$ by using CGMF parameters obtained from fitting to experimental 238 U $\overline{v}_p$ to predict yields as a function of mass, the average total kinetic energy, or the mean energy of the prompt fission neutron spectrum. These model-predicted values can then be compared to experimental and evaluated data. The model-predicted fission-observable values using evaluated parameters obtained here are reasonably close to experimental data for some observables, but are farther away from experimental data related to TKE observables. In addition to that, the evaluated 238 U(n,f) $\overline{v}_p$ shows similar deviations from ENDF/B-VIII.0 as for the evaluation with only experimental data. This difference is expected to lead to changes in simulated effective neutron multiplication factor, $k_{eff}$ of ICSBEP critical assemblies that are sensitive to 238 U in the fast range (BigTen, Flattop, Flattop-Pu). These changes in $k_{eff}$ need to be counter-balanced. Chi-Nu PFNS experimental data are expected to be released in the next few months that might lead to the needed changes in the PFNS. Until then, we hold off in benchmarking the new 238 U(n,f) $\overline{v}_p$ as well as submitting it to ENDF/B-VIII.1. Also, new high-precision 238 U $\overline{v}_p$ are expected to be measured by the CEA in the next two years that will shed further light on question on 238 U $\overline{v}_p$ from 2–4.5 and 6–7 MeV.

238U↗
DOE OSTI2023

Nuclear Criticality Experiments Research Center Futures: A Report of a Workshop held September 6-9, 2022, Los Alamos, NM, November, 2022

Experiments and training with critical assemblies and fissionable material (at or near the critical state) that explore reactivity phenomena are central to a number of national security challenges. From fission energy to nuclear weapons to a broad suite of scientific challenges, it is clear that additional capacity and capability are needed. The National Criticality Experiments Research Center (NCERC) marked 10 years of operations in 2021. This anniversary was an opportune time to celebrate our successes and progress, and to evaluate the remaining and emergent challenges. Against this backdrop, a workshop of approximately 140 national and international leaders in nuclear research was convened in Los Alamos, New Mexico to explore “NCERC Futures.” Therefore, the present workshop focused specifically on needed capabilities and tools to meet the research challenges in eight topical mission areas served by NCERC. As each Topical Group summarized their discussions in the out brief, it was recognized that key challenges could be met through enabling infrastructure investments and new critical assemblies. Enabling infrastructure includes staffing, additional space/buildings, developing an agile bounding safety basis, the ability to keep pace with technological advances in detectors and data acquisition systems (allowing use of those with Bluetooth™ and similar technologies), an expanded set of materials options (especially plutonium), a “Plug and Play” design and implementation mindset, and a facility that enabled free-field measurements. The new critical assemblies that were identified as having the most impact were a bare plutonium (Pu) Critical Assembly, a Horizontal Split Table (HST), a Super Comet, and a Uranium Solution Burst Assembly. NECRC is a unique, one-of-a-kind facility in the United States. If all the improvements were to be made, NCERC would enable the United States and its partners to address many important research questions related to criticality. These include but are not limited to: (1) Covering the entire neutron energy spectrum for both highly enriched uranium (HEU) and Pu in configurations for virtually all conceivable applications; (2) Performing multi-physics solution experiments and irradiations with a Uranium Solution Burst Assembly, which more closely resembles actual criticality accidents; (3) Conducting free-field experiments to make basic fission physics measurements and much cleaner benchmarks with various experimental observables; and (4) Providing more training classes and more experiments annually at greater cost efficiency enabled by additional buildings and machines and an agile, bounding, risk-balanced Safety Basis. In the end, workshop attendees enthusiastically concluded that NCERC Futures are bright and the workshop helped to identify a roadmap of capability gaps that need to be addressed. This report documents the results of those efforts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

NCSP Outlook and Interest for Collaboration on HST Experiments [Slides]

The majority of the NCSP budget goes to Integral Experiments. The goal is to produce needed integral data for criticality safety needs in DOE, largely resulting in ICSBEP benchmarks. NCSP has a well defined process for allocating funding through proposals and expert review. NCSP is a fairly small program and funding is prioritized for experiments that would address DOE criticality safety needs. The majority of the currently identified DOE criticality safety needs are HEU and Pu systems. NCSP has a formal mechanism to ensure quality and benefit through the phase gates and approvals within the CED process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Modeling and evaluating 239 Pu and 235 U PFNS and average prompt-neutron multiplicity [Slides]

The following are currently in VIII.1 LANL and IAEA test files: 239 Pu nu-bar including CGMF modeling and CEA data, 239 Pu PFNS including Chi-Nu & CEA data, 239 Pu(n,f) cross section including fission TPC data. The following are currently being tested: 235 U nu-bar including CGMF modeling and 235 U PFNS including Chi-Nu data. Upcoming tasks include the correction of 235 U Chi-Nu PFNS at higher E inc , benchmarking 235 U PFNS and nu-bar evaluations, and getting 238 U nu-bar.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Metallic Fuel Benchmark Simulations Based on the X430 Experiments

To gauge the accuracy of current BISON metallic fuel performance models and identify models that require further development, Oak Ridge National Laboratory has developed benchmark problems based on two pins of the X430 experiment. These benchmarks recreate the experimental conditions of the X430 series of experiments with as much accuracy as possible given the available data. The benchmarks were implemented in the BISON nuclear fuel performance code and the simulation results were compared with the experimental results to quantify the simulation accuracy. Findings in this work were consistent with previous benchmark problems. The temperature profiles, burnup, and fission gas behavior were all as accurate as can reasonably be expected. The cladding radial growth was accurate enough to not affect the results of other measurements. The fuel axial growth was accurate for U-Zr fuel but not for U-Pu-Zr fuel, which appears to be caused by a lack of U-Pu-Zr data. Swelling correlations have not been developed for U-Pu-Zr fuel because there were not enough data on this fuel type, so BISON used the U-Zr correlations. Finally, recommendations were made for near-term BISON development.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Which nuclear data can be validated with LLNL pulsed-sphere experiments? [Slides]

LLNL pulsed sphere are a very valuable experiment series to validate scattering and fission nuclear data. It would be great if they could be evaluated as benchmarks and make it into SINBAD! We see potential issues in ENDF/B-VIII.0 6 Li, 12 C, 16 O, 24- 26 Mg, 27 Al, 48 Ti, 56 Fe, and 208 Pb nuclear data. Good agreement is found with 1,2 H, 7 Li, 9 Be, 14 N, 235,238 U, and 239 Pu nuclear data.

16O and 12C Spheres↗
DOE OSTI2022

Pulsed Sphere Time of Flight Neutron Spectrum Measurements: Blank Run and 1.8 Mean-Free-Path thick Polyethylene Moderating Sphere

From the late 1960s to 1985, Lawrence Livermore National Laboratory (LLNL) undertook a series of ‘pulsed sphere’ experiments for 32 materials involving 148 different experiments using 75 different spheres to measure the neutron leakage spectra for different materials from 14-MeV neutrons generated by 3 H(d, n) 4 He reactions induced by an incident D+ beam from the Insulated Core Transformer (ICT) accelerator at LLNL. This deuteron beam was focused to impinge on tritium loaded onto a titanium substrate within a low mass target assembly placed within the center of a spherical shell constructed from the material of interest. The neutron time of flight was measured at a detector outside a collimator. The program was intended to be comprehensive with numerous targets of various thicknesses spanning the periodic table from H to 239 Pu. Five different neutron detectors were utilized to avoid possible systematic errors due to differences in detector responses. Further, these measurements were designed with the aim that the simple geometry of the measurements could be easily simulated to validate Monte Carlo transport codes and nuclear data libraries. As a result, these benchmarks have been extensively used in the validation of ENDL, ENDF and other libraries. Two experiments selected as benchmark cases in this evaluation are: 1) target assembly without material sphere (blank run), and 2) target assembly with a hollow polyethylene sphere, 1.8 mean free path (mfp) or 16.56 cm thick.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Consistent Nuclear Data Evaluations for Criticality Safety

Evaluations of nuclear data are based on statistical analysis of available experimental data and their uncertainties plus model calculations and their uncertainties. As the models are currently rather limited, the evaluations are heavily biassed toward experimental data, with the caveat that a thorough analysis is also required to understand possible discrepancies between data sets. Hence, as new experimental data become available, they are incorporated into the evaluation procedure. Recent measurements of the 233 U capture to fission cross section ratio at the Los Alamos Neutron Science Center have prompted a re-evaluation of the capture cross section in the resonance and fast regions up to 250 keV. We will discuss the challenges of including the new fast neutron experimental data in an evaluation that is consistent with the resonance region. We will also discuss our consistent evaluation procedure based on the Hauser-Feshbach statistical model for nuclear reactions and its application to the evaluations of 239 Pu and 139 La neutron-induced reactions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

TEX-HEU: Integral Experiments with Highly Enriched Uranium and Polyethylene [Slides]

This presentation discusses Thermal/Epithermal eXperiments (TEX) in relation to integral experiments spanning a wide range of fission energy spectra utilizing existing NCSP fissile material assets, TEX-Pu for plutonium, and TEX-HEU highly enriched uranium (HEU) for highly enriched uranium. It also discusses the TEX-HEU design, the use of HEU fuel, and polyethylene parts. The experiment, executed in the Nuclear Criticality Experiment Research Center of the Nevada National Security Site is discussed, specifically how it was assembled on the Comet Universal Critical Assembly Machine. Measured quantities and various critical configurations are listed. In conclusion, the presentation states that they successfully assembled and documented the baseline TEX-HEU experiments, that six critical configurations and one reproducibility measurement were produced, and that they are compiling results to submit to the International Criticality Safety Benchmark Evaluation Project. A future experiment campaign is planned in 2021 with Hafnium as a diluent.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Criticality Experiments to Reduce Compensating Errors in Plutonium Nuclear Data

Compensating errors between nuclear data observables in a library can adversely impact application simulations. The primary goal of the EUCLID project (Experiments Underpinned by Computational Learning for Improvements in Nuclear Data) is to reduce compensating errors in nuclear data. A new criticality experiment, described in this work, was designed with the specific target nuclear data of 239 Pu fission, inelastic scattering, elastic scattering, capture, nu-bar, and prompt fission neutron spectrum (PFNS). This work will focus on the design and execution of the EUCLID experiment, performed on the Planet vertical lift critical assembly machine at the National Criticality Experiments Research Center (NCERC). The criticality experiment includes two different configurations with very different geometries: one is cube-like to minimize neutron leakage while the other is slab-like to maximize leakage. Having these two widely varying configurations allows the scattering sensitivities of 239 Pu to the neutron multiplication factor to be greatly changed while minimally impacting the other cross section sensitivities. Both configurations utilize the Pu ZPPR (Zero Power Physics Reactor) plates as fuel. The experiments were designed using a D-Optimality criteria, which is an optimization method minimizing the log-determinant of the adjusted nuclear data covariance for the target reactions. These experiments include not only inference of k eff , as done in all critical benchmark experiments, but several other responses as well, such as neutron multiplication measurements and reaction rate ratios. After analysis of the measured data is complete, adjustment of nuclear data will be performed to assess whether the new experimental data successfully reduced compensating errors.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2022

239 Pu R -matrix Analysis and Neutron Multiplicities in the Neutron Energy Region up to a few keVs [Abstract]

The evaluation of 239 Pu neutron resonance parameters coupled to neutron multiplicities $\overline{v}_p$ is of particular importance to investigate the ($\mathcal{n, γf}$) reaction in which a $\mathcal{γ}$-ray emission occurs before the scission of the compound nuclear. This reaction has offered one explanation for the fluctuations in the measured values of $\overline{v}_p$ In this regard, the competition between ($\mathcal{n, γf}$) reaction and the direct fission process can be also included in the R matrix analysis of fission and capture measured data. The goal of this work is the coupled evaluation of the $\mathcal{n}$+ 239 Pu resonance parameters and related neutron multiplicities by ensuring the adoption of thermal neutron constants recently evaluated at the International Atomic Nuclear Energy as well as the recommended (thermal-neutron) induced prompt neutron fission spectrum (PFNS). Moreover, this new set of physical evaluated quantities should also guarantee the agreement for high-leakage solution benchmarks while keeping the good performance of large thermal solution assemblies.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2026

Synthesis and Characterization of Layered Actinide (U, Np, Pu) Oxide and Hydroxide Phases

Systematic structural comparisons across the early actinides remain limited by the scarcity of well-defined transuranic layered oxide and oxyhydroxide phases. Here, we report the synthesis and single-crystal characterization of new layered actinide compounds spanning U, Np, and Pu obtained under mild hydrothermal conditions in concentrated alkali hydroxide media. These include hydrated oxides α-Cs 2 U 2 O 7 •0.5H 2 O and Rb 2 An 2 O 7 •0.5H 2 O (An = Np, Pu), oxy-hydroxides Rb 6 [(AnO 2 ) 6 O 8 (OH) 2 ]•xH 2 O x = 0, 0.5 (An = U, Np) and Rb 4 [(UO 2 ) 5 O 6 (OH) 2 ]•2H 2 O, as well as nitrate-intercalated compounds Cs 6 [(AnO 2 ) 3 O 4 (OH) 2 ](NO 3 ) 2 (An = Np, Pu). Single-crystal X-ray diffraction studies reveal extended two-dimensional architectures constructed from edge- and vertex-sharing actinyl polyhedra, with systematic evolution in equatorial coordination, hydration, and anionic sheet topology across the U–Np–Pu series. Incorporation of nitrate anions within the interlayer region of Cs 6 [(AnO 2 ) 3 O 4 (OH) 2 ](NO 3 ) 2 establishes a previously unobserved structural motif in layered transuranic oxyhydroxides, demonstrating an additional pathway for anion-mediated framework stabilization. Correlation of crystallographic metrics with single-crystal Raman spectroscopy provides new vibrational benchmarks linking differences in An═O yl bond lengths to the equatorial coordination and the interstitial cations. These findings expand the structural hierarchy of layered actinide materials and address clarifying periodic trends governing topology, bonding, and vibrational signatures in high-valent 5ƒ oxide systems.

actinides↗
DOE OSTI2021

Development of a U-19Pu-10Zr fuel performance benchmark case based on the IFR-1 experiment

Metallic nuclear fuels are subject to research and development for use in advanced reactors. Robust, accurate metallic fuel performance models are important for the design, safety analysis, and licensing of these reactors. However, metallic fuel performance models require additional development; they are not as mature as UO 2 fuel performance models. A benchmark case based on the IFR-1 experiment was developed to better gauge the accuracy of existing models, identify models for high-priority development, and potentially quantify any future improvements made by further model development.This work collected publicly available information on the IFR-1 experiment and used it to develop the benchmark case. Fuel behavior during the IFR-1 irradiation was simulated by using the fuel performance code BISON, and the predicted results were compared with postirradiation examination data from the IFR-1 experiment. Furthermore, a sensitivity study and tuning studies were performed as a preliminary investigation into the causes of inaccurate temperature and dimensional change predictions.The benchmark predicted reasonably accurate values for the burnup and fission gas release. There was error in the predicted temperatures, which could be explained by uncertainty in the input parameters and legacy temperatures. BISON over-predicted dimensional changes in the fuel and cladding. The sensitivity study showed that the dimensional changes were most sensitive to the fuel swelling anisotropy and the cladding void swelling model. Future benchmark and model development should focus on cladding swelling behaviors to improve dimensional change predictions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Impact of Thermal Scattering Law on Similarity Assessment in Light-Water or Polyethylene-Moderated Systems

A collaborative effort between Pacific Northwest National Laboratory (PNNL) and Oak Ridge National Laboratory (ORNL) is underway to provide a technical basis and methodology for the criticality safety community to use the sum of fractions (SoF) method for generating limits for mixtures of “selected actinide nuclides” included in the ANSI/ANS 8.15 standard. The PNNL scope in this project is to define a range of mixtures of 233 U, 235 U, and 239 Pu moderated with either light water or polyethylene and to examine the critical masses for these mixtures. The ORNL scope is primarily to provide validation support for these studies. More complete discussion of the project and its validation aspects will be presented at the upcoming International Conference on Nuclear Criticality Safety (ICNC) this Fall in Sendai, Japan. Clear differences in benchmark similarity to application systems as assessed by the integral parameter ck are noted in the validation studies performed as part of this project as a function of moderator. The c k value is a correlation coefficient that represents that amount of shared uncertainty in k eff due to cross sections between two systems. Individual nuclide-reaction contributions between the two systems can be simply summed to arrive at the total c k value. Specifically, the c k values for light-water–moderated solution experiments are higher for a water-moderated application than for a polyethylene-moderated application. This result is neither totally unexpected nor surprising, but the magnitude of the difference was difficult to anticipate. The TSUNAMI sequence, in the SCALE 6.2.4 code package developed by ORNL, was used to generate eigenvalues and reactivity effects with perturbation-theory based approach through sensitivity coefficients for all nuclides in the system with all reactions and energy groups. The TSUNAMI-Indices and Parameters (IP) sequence then uses the sensitivity data generated through TSUNAMI to generate relational parameters (i.e., c k ) to determine the degree of similarity between systems. One detail of the SCALE material and data implementation must be discussed at this point. Several thermal scattering laws (TSLs) are available for 1 H. SCALE uses a different nuclide ID number for each TSL; essentially, each version of 1 H is treated as a unique nuclide. For example, 1 H bound in water ( 1 H-H2O) is assigned the nuclide ID 1001, whereas 1 H bound in polyethylene (h-poly) is assigned the nuclide ID 9001001. The same cross section data are used for all reactions in 1 H, regardless of TSL, except for scattering below the TSL cutoff energy. TSUNAMI-IP treats different nuclide IDs as different nuclides; thus, no uncertainty is shared between 1 H-H2O and h-poly, despite much of the same data, including covariance data, being used for both nuclides. This presents a question: how much of the difference in assessed similarity between water- and polyethylene-moderated systems is due to the moderators, and how much is caused by the treatment of 1 H-H2O and h poly with cross section and covariance data. The extended edits generated by TSUANMI-IP allow for an investigation of this issue specifically, as well as a demonstration of the general techniques available within TSUNAMI to understand the results of the similarity assessment. This paper presents and analyzes the similarity assessment of both water- and polyethylene-moderated systems for a single benchmark: PST-002-001.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

NCSP supports 240 Pu prompt fission neutron spectrum (PFNS) evaluation

A new 240 Pu PFNS evaluation was recently undertaken at LANL as a strategic priority. It truly is an NCSP end-to-end product. It factors in a new differential experiment funded by NCSP, builds on theoretical work coming out of a previous NCSP nuclear data evaluation milestone and was validated with an NCERC experiment that was recently evaluated as an integral benchmark with NCSP funds.

240Pu↗
DOE OSTI2023

Integral Experiment Final Design for Thermal/Epithermal eXperiments with 233U3O8 ZPR Fuel Elements and Polyethylene (IER-329 CED-2 Report)

This report documents the integral experiment final design for IER-329, Thermal/Epithermal eXperiments (TEX) with 233 U 3 O 8 Zero Power Reactor (ZPR) Fuel Elements and Polyethylene. IER-329 (TEX-23) is the third baseline design in the Thermal/Epithermal eXperiments (TEX) series led by Lawrence Livermore National Laboratory (LLNL) and funded by the DOE’s Nuclear Criticality Safety Program. This experiment was designed to address the existing 233U integral benchmark experiments over prediction in k eff by up to 2% for thermal systems and under-prediction in k eff by up to 4% for intermediate systems. The TEX-23 design utilizes assemblies of 233 U 3 O 8 Zero Power Reactor (ZPR) fuel elements moderated and reflected by high-density polyethylene. This design is similar to the existing TEX-Pu and TEX-HEU designs, utilizing an adjustable moderator to tune the neutron energy spectra and modular layers for the incorporation of diluent materials.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Covariance Testing Progress for ENDF/B-VIII.1β1 at ORNL [Slides]

This presentation touched on how data-induced uncertainty significantly increased for thermal 235 U-fueled systems. And how 239 Pu covariance changes are worrying. Additionally discussed is how 103 Rh is the only significant important fission product change. The Impact of ENDF/B-VIII.1β1 on burnup credit similarity assessments is similar to ENDF/B-VII.1 data.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗