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At least 1,369 records · Page 76

Fission TPC cross section ratio results [Abstract]

The fission TPC was designed for precision fission cross section ratio measurements. The high-fidelity 3D particle tracking data is used to conduct a detailed analysis of the uncertainty contributions. In this contribution a brief overview of the instrument was presented. The results of the 238 U(n,f)/ 235 U(n,f) cross section ratio measurement published in [Phys. Rev C 97, 034618 (2018)] were reviewed and the preliminary status of the 239 Pu(n,f)/ 235 U(n,f) cross section ratio measurement was shown.

238U(n,f)/235U(n,f) cross section ratio↗

Constrained Bayesian Optimization of Criticality Experiments [Slides]

The design of criticality experiments is typically an iterative process that employs a Monte Carlo transport code. The goal is to find a design that optimizes some variable, like the sensitivity of a response to a cross section, while simultaneously ensuring criticality. The high fidelity of the Monte Carlo code is a great asset, but it makes exploring the design space computationally expensive. Herein, we present how a constrained Bayesian optimization algorithm can be used to efficiently design a criticality experiment. It uses Gaussian processes as a surrogate model to probe the design space and to reduce the number of code executions that are needed to find the optimum. We demonstrate constrained Bayesian optimization with a Pu-239/polyethylene solution system and a TEX experiment that is designed for criticality safety validation of a nuclear waste model at the Hanford Site. For both systems, a global optimum was found within 75 Monte Carlo simulations.

42 ENGINEERING↗

Constrained Bayesian Optimization of Criticality Experiments at LLNL [Slides]

The design of criticality experiments is typically an iterative process that employs a Monte Carlo transport code. The goal is to find a design that optimizes some variable, like the sensitivity of a response to a cross section, while simultaneously ensuring criticality. The high fidelity of the Monte Carlo code is a great asset, but it makes exploring the design space computationally expensive. Herein, we present how a constrained Bayesian optimization algorithm can be used to efficiently design a criticality experiment. It uses Gaussian processes as a surrogate model to probe the design space and to reduce the number of code executions that are needed to find the optimum. We demonstrate constrained Bayesian optimization with a Pu-239/polyethylene solution system and a TEX experiment that is designed for critical ity safety validation of a nuclear waste model at the Hanford Site. For both systems, a global optimum was found within 75 Monte Carlo simulations.

42 ENGINEERING↗

Nuclear Reaction Data Evaluations for Nuclear Applications Physics and modeling [Slides]

This presentation provides an evaluation workflow scheme for the project. It also discusses nuclear data libraries, including an overview of worldwide nuclear data libraries and current funding agencies. The presentation also discusses the theoretical framework commonly used in the evaluated work, including the R-matrix theory (≈ up to a few keVs for heavy nuclei) as well as pre-equilibrium (PE) and Hauser-Feshbach (HF) theory (⪆1 MeV for medium/heavy nuclei). Inclusion of experimental effects are also discussed. Examples of evaluated work, including theory, experiments, and applications are discussed, specifically n+ 28,29,30 Si evaluation (direct capture component), n+ 53 Cr evaluation (strong multiple scattering effects), n+ 239 Pu(n,γf) reaction (fluctuations in neutron multiplicities), and α+ 17,18 O evaluations (emerging neutron spectra).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

On the Uranium and Plutonium Nuclear Data Evaluations [Slides]

This presentation provides overviews of uraniums, 233 U and 235 U, plutonium research including motivations, current status in ENDF/B-VIII.0, the inclusion of sub-thermal data, and the inclusion of LANL ratio capture-to-fission data. Additionally, the preliminary fit of Mosby’s data as reported, fluctuating neutron multiplicities, uncertainty in evaluated libraries, and experimental effects are also presented. The presentation concludes by providing a summary of plans for the U and Pu evaluation work.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Options for the Removal of Cesium and Strontium from Acidic Uranyl Sulfate Solutions from Molybdenum-99 Production: Part II The Effect of Sodium Carbonate Adjustment to pH 9 on Strontium Removal

A small laboratory-scale column process aimed at removing fission products from prototypical acidic sulfate solution wastes from a prototypical Mo-99 recovery process has been operated in a radioactive materials hood at Savannah River National Laboratory. This equipment has been operated with realistic concentrations of uranium (0.4 wt % 235 U), plutonium ( 239 Pu), neptunium ( 237 Np), non-radioactive surrogates of common fission products (including Cs and Sr) and two promising absorbents – AMP-PAN and CST R9120-B. The goal of this work was to demonstrate the removal and concentration of high specific activity isotopes which are expected to dominate the classification of the low-level waste from the production of 99 Mo. Both AMP-PAN and CST R9120-B are attractive absorbents for the removal of 137 Cs from an acidic sulfate waste stream. They do not provide a solution for the removal of 90 Sr from the acidic solutions. CST was shown to be useful at removing both Cs and Sr after adjustment of the acidic sulfate solution with sodium carbonate to pH 9. Limited removal of transuranic species and almost no removal of uranium was observed for CST R9120B absorbent. This could be important due to the relatively large amount of uranium expected to be present in such waste streams. The capacity of these absorbents for 137 Cs will likely be dependent on the Cs concentration in the solutions processed but loading in excess of 0.7 mg Cs per gram of CST absorbent while loading 0.14 mg Sr per gram of CST absorbent appears to be achievable from pH 9 carbonate solution.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Probing f-orbital covalency through the fold angles of transuranium dithiolene complexes

The ability of the actinide elements to covalently bond to ligands is not well understood. A computational effort for compounds of the formula [Cp 2 AnS 2 C 2 H 2 ] -1,0,+1 where An = U, Np, or Pu has shown that the angle between the plane formed by the two sulfurs and the plane formed by the two sulfur atoms and the two carbons converges to 70 – 75° when the ligand is in the dithiolate state (-2 charge on the ligand). Upon oxidation of [Cp 2 NpS 2 C 2 H 2 ] 0 or [Cp 2 PuS 2 C 2 H 2 ] 0 the electron is removed from the dithiolate rather than the actinide and the dihedral angle is reduced to planarity. The reaction of NpCl 4 DME 2 with deprotonated benzene dithiol shows an intense color change suggestive of a charge transfer complex. The binding of the benzene dithiol as the dithiolate to the neptunium metal center is supported by visible, infrared and NMR spectroscopies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Alternative Power and Propulsion for Space Systems

What are the main sources of power and propulsion for space systems and what are their advantages, disadvantages, how do they work, and what are the politics behind them? The following topics will be analyzed solar panels, batteries, radioisotope thermoelectric generator (RTG), advanced Stirling radioscopic generator (ASRG), reactors, nuclear thermal rockets (NTP), thermionic experiment with conversion (TOPAZ), electrothermal plasma thruster (VASIMR), ion propulsion, and finally nuclear pulse propulsion. The production of Pu-238 is extremely controversial but a vital source of fuel for many of these space systems. Soral and Batteries are the most common and the least controversial forms of power used in space systems today. However, is ineffective for deep space exploration as they only function for up to four years without needing to be recharged. This is where nuclear systems come into play. Nuclear systems such as an RTG will “live” up to 88 years. For example, Voyager 1 is powered by an RTG It has been traveling since 1977 and has left out solar system in 2012 and has yet to run out of power. However, this type of technology (nuclear) has many hurtles it needs to jump through before advancements in can go much further.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Packaging Plan for Mark-18A Plutonium Oxide

Mark-18A (Mk-18A) targets were irradiated at the Savannah River Site and have been in wet storage at the site since the 1970s. The Mk-18A Target Material Recovery Program has been established to recover the 244 Pu and heavy curium (≥50% 246 Cm and 248 Cm) in the targets at the Savannah River National Laboratory (SRNL) and ship the materials to Oak Ridge National Laboratory’s (ORNL’s) Radiochemical Engineering Development Center for programmatic use. Two products will be recovered from the Mk- 18A targets for shipment from SRNL to ORNL: a plutonium oxide stream and an oxide material that will contain the americium, curium, and lanthanides. This document presents the plan for packaging of the plutonium oxide material for shipment and storage at ORNL.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Validating ENDF/B-VIII.1beta1 with LLNL Pulsed-Sphere Neutron-Leakage Spectra [Slides]

In this presentation 6 Li Distinct changes are observed. 235 U Discussion shows Improvements (seen in VIII.1beta0) are coming from new PFNS informed by Chi-Nu experimental data. Additionally, 239 Pu large changes coming from inelastic scattering. 9 Be ENDF/B-VIII.0 shows to be better right after elastic peak while 16 O had slight changes. 19 F had small improvements in ENDF/B-VIII.1 and 56 Fe had noticeable changes in thicker spheres. Examples of negligible changes for the sake of completeness are given.

16-Oxygen↗

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

This presentation found validation efforts revealed noticeable differences in c k for light-water and polyethylene moderated systems when compared to PST-002-001. Additionally, although 1 H-H 2 O and 1 H-poly use the same cross section and covariance data, the treatment of TSLs in SCALE lead to no contribution to ck between polyethylene application and benchmark experiment. When H 2 O contribution were removed the difference in c k appears to come from 239 Pu chi. Sensitivity profiles and data-induced uncertainty confirmed that the polyethylene application was more closely resembling the benchmark experiment. Specific differences between similar systems can be accounted for and examined to help understand differences in similarity (c k ) between systems was a conclusion reached by this presentation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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↗

Plutonium Basket Counter Measurement Control Q3-Q4 2023

The Plutonium Basket Counter (PBC) is a spent fuel nuclear safeguards instrument that was developed to measure spent-fuel elements from MAGNOX-type research reactors and determine their plutonium content. The instrument is designed to measure fuel elements in spent fuel cooling pools through underwater operation, but it is also able to measure radiation sources in air. The PBC determines fuel plutonium content by detecting neutrons with an array of Helium-3 detectors. The electronics make use of a JSR-15 shift register for data collection and IAEA Neutron Coincidence Counting (INCC) software for data analysis. The PBC is used to determine the 240 Pu content in spent MAGNOX fuel elements grouped into basket-like bundles, thus the instrument’s name. Reactor burnup calculations can be used in conjunction with the data from the PBC to estimate the total plutonium content in the fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fission with Exotic Nuclei (Abbreviated Report)

Nuclear fission is a key mechanism involved in the synthesis of heavy elements in the Cosmos and is the primary explanation for the stability of superheavy elements. Nevertheless, our knowledge of fission remains extremely fragmented. Most experiments have been conducted only on a tiny number of stable actinide nuclei and are often incomplete, leading to gaps in our basic understanding of the process. For many radioactive isotopes, basic fission data such as the charge or mass distribution of the fragments is unknown. These gaps cannot always be filled by simulation alone. Common fission models contain too many free parameters and lack predictive power. In contrast, the fundamental theory of fission under development at LLNL is much more predictive, but its current computational cost is too high to be used extensively for data evaluations. A unique window of opportunity to resolve these limitations has recently opened: the U.S. nuclear science community is ramping up major experimental programs at the Facility for Rare Isotope Beams (FRIB, the DOE flagship facility in low-energy nuclear science), and techniques from machine learning have shown great potential to simplify the use of a fundamental, quantum-mechanical theory of fission. This project has two components. On the experimental side, we acquired and deployed at the HIGS facility a new dual Frisch-Grid ionization chamber to measure correlated fragment-mass, kinetic energy, and angular distributions of fission fragments from induced fission. This new device was used to perform measurements of charge, mass and total kinetic energy of fission fragments in the photofission of 238 U and eight gamma-ray beam energies between 6.2 and 13 MeV, which allowed extracting high-precision independent yields for this reaction. The device was also used to perform measurements of the same quantities in the neutron-induced fission of 234 U with monoenergetic beams of energy between 5 and 8 MeV. In parallel, we collaborated with a team at Commissariat à l’énergie atomique et aux énergies alternatives (CEA) to perform a series of measurements of fission yields in inverse kinematics for the two isotopes of 236 U and 240 Pu. The experiment took place at the Grand Accélérateur National d’Ions Lourds in France in June 2023. The deployment of the VAMOS spectrometer with a new array called PISTA allowed determining the excitation energy of the fissioning system within 1 Mega-electronvolts. The second component of the project involved using deep neural networks to build fast and reliable emulators of our current fission models. In an invited paper published in Frontier in Physics, we showed that autoencoders could successfully compress nuclear wavefunctions in nuclear density functional theory. We achieved a dimensionality reduction of the order of two orders of magnitude while keeping the error in the total energy to less than 0.01%. In a second paper submitted to Physical Review Letters in June 2023 with our collaborators at CEA, we showed that variational autoencoders can learn the collective degrees of freedom driving the fission process.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Update of the Cesium-136 Cumulative Fission Yields at Multiple Neutron Energies

Nuclear data is foundational to several fields, including nuclear forensics. Nuclear forensics investigations of fission events, relies heavily on the cumulative fission yields, however several highly useful fission products suffer from very poor nuclear data including cumulative fission yields or associated uncertainties in that value. Cesium-136 is a highly relevant example of this issue, where the cumulative fission yield may be accurate but its uncertainty high enough to preclude its usefulness. In this work we evaluate and calculate an updated cumulative fission yield for 136 Cs for 235 U, 238 U, and 239 Pu at multiple neutron energies or sources using data obtained from irradiation campaigns. In all cases these newly determined cumulative fission yields provided small changes to the actual fission yields but had dramatic improvements to the uncertainty in those yields. These improvements in uncertainty will enable nuclear forensics end users to use 136 Cs data with more confidence.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Np-237 LoD Measurement by TIMS-Multi-Ion Counting Total Evaporation [Poster]

Requests for ultra-low-level 237 Np analyses highlight the importance of a robust chemical purification and measurement technique for Np. In FY2022, LANL is quantifying the instrumental 237 Np LoD. Need to incorporate a chemical purification procedure for TIMS-MICTE sample preparation. What is the recovery of the chemical purification procedure? What is the ultimate detection limit that can be achieved while incorporating a chemical purification procedure? We have adapted and refined the Pu TIMS-MICTE method for Np analyses. We have determined expected uncertainties for 237 Np TIMS-MICTE measurements. We have increased sensitivity through technique improvements. We have improved method reliability for Np analyses and increased throughput. Apply knowledge gained from progress made in FY2022 to further develop Np sample purification and analyses by TIMSMICTE.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Kinetics and Mechanism of Tetravalent Cerium Extraction by Di-2-Ethylhexyl Isobutyramide (DEHiBA)

DEHiBA is a fully-incinerable, CHON extractant with a high selectivity for hexavalent actinides. However, as a recently-developed ligand, much remains unknown about its physical and chemical properties, including its extraction and phase disengagement rates. Here, we present data on the phase transfer kinetics of Ce(IV) extraction and stripping by both DEHiBA and TBP collected using microfluidic devices. Ce(IV) was selected as a surrogate for Pu(IV) and Np(IV) in the initial tests of the microfluidics system prior to testing with the actinides. Pseudo first-order reaction rate constants are determined for both systems, and the corresponding Damköhler numbers (Da) are calculated to establish whether the extraction and stripping processes are kinetically or diffusion controlled. The stoichiometry of the extracted Ce(IV)-DEHiBA complex is determined, and the phase disengagement properties under extraction conditions are assessed using the dimensionless dispersion number. A possible explanation for the favorable extraction of Ce(IV) by DEHiBA, which is known to poorly extract many tetravalent cations, is presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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↗