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At least 73 records · Page 4

Management of Legacy Enriched Uranium and Transuranic Materials at ORNL

The DOE manages an inventory of materials that contains a range of long-lived radioactive isotopes that were produced from the 1960s through the 1980s. These materials were made by irradiating targets in production reactors to produce special heavy isotopes for DOE programmatic use, scientific research, and industrial and medical applications. ORNL uses these materials in DOE’s center for production, storage, and distribution of transuranium isotopes (plutonium through californium) for the heavy-element research program and has used them as feedstock in the Calutron Electromagnetic Isotope Enrichment Facility, one of only two facilities in the world with capabilities to enrich radioisotopes in multigram quantities. Both the production reactors and enrichment facilities have been shut down, and many of these unique materials will not be produced again in the foreseeable future [1, 2]. As a result, ORNL has an inventory of radioisotopes that are being held for reuse because their potential intrinsic value to DOE, but many of these materials have no currently defined use. ORNL is undertaking an initiative to more actively manage these materials by reviewing the existing inventory to determine if the contents have programmatic use. Steps are being taken to process, repackage, and stage the materials for distribution to programmatic users or for waste disposal, primarily at WIPP. This paper describes the approach that ORNL has taken to determine whether the inventory of materials should be kept or disposed and the processes that are being used to manage or disposition the materials.

Patton, Bradley↗

Finalizing the 63 Cu and 65 Cu Resonance Evaluations for the ENDF/B-VIII Release

The resolved resonance region evaluation for the only two natural isotopes of copper ( 63 Cu and 65 Cu) was carried out at the Oak Ridge National Laboratory (ORNL) in support of the US Department of Energy (DOE) Nuclear Criticality Safety Program (NCSP). The particular interest in the isotope of copper arose because it was linked with poor performance of the Zeus series of integral benchmarks from the International Criticality Safety Benchmark Evaluation Project (ICSBEP). Good agreement between the calculated and experimentally measured values for the ICSBEP benchmarks is essential to the NCSP because the ICSBEP benchmarks are used for validation purposes of criticality safety calculations.

07 ISOTOPE AND RADIATION SOURCES↗

NSUF BOILER Pre-Irradiation Characterization and High Flux Isotope Reactor Experiment Design

Alumina-forming austenitic (AFA) stainless steels have emerged as a candidate alloy because of their high-temperature strength, formability, cost, and compatibility with primary coolants for lead-cooled fast reactors (LFRs). This class of steels has exceptional high-temperature oxidation performance; however, a high concentration of Ni is required to stabilize the austenite phase and to provide sufficient creep strength. AFA stainless steels are also susceptible to liquid metal embrittlement (LME). Additionally, under neutron irradiation, Ni will enrich at grain boundaries due to radiation-induced segregation (RIS). Nickel RIS can increase the LME under these coupled effects. Oak Ridge National Laboratory (ORNL) and the NSUF program have leveraged its High Flux Isotope Reactor (HFIR) and experience with complex irradiation experiments to design experiment capsules that test the aforementioned coupled effects. These capsules are designed for insertion in the central flux trap, the highest flux region, of HFIR. The experiment capsules will be filled with Pb, designed to passively melt from the gamma heating in HFIR. The specimens were fabricated into miniature tensile specimens from two different alloys, GA05-25Ni and GA05-20Ni, varying Ni concentrations. The experiment capsules are designed to achieve target temperatures of 400 °C and 650 °C with accumulated dosage of 3 dpa. This report documents the specimen alloy characterization, experimental design, and expected performance of the capsules.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

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↗

Conifer water use patterns in the East River Watershed, Colorado US, based on stable water isotopes and cellulose isotopes

This data package contains a series of datasets aimed at understanding the seasonal origins of water used by the dominant conifer species, Abies lasiocarpa and Picea engelmannii, in the East River Watershed. There is a distinct difference in the stable isotopic ratio of summer rain and snowpack and thus by tracking the isotopic ratio of the xylem water in trees, it is possible to separate when a tree is using snow vs. summer rain. Following typical protocols, we sampled and extracted water from soils in the "Research Meadow" near Gothic, CO within the East River Watershed through the 2016 growing season. The stable isotopic ratio of these waters were then measured. Using values of the isotopic ratio of precipitation and snowpack from that season, we develop a mixing model to show how the trees transitioned from use of snowpack to summer in late July. We extended the information on the seasonal origins of water from 2016 back until 1980 by using measurements of the isotopic ratio of cellulose from trees in the Research Meadow. The isotopic ratio of tree ring cellulose records a signal both of the Vapor Pressure Deficit at the leaf-atmosphere boundary and also the source water for the trees. We concluded from this extended analysis that the trees underwent transitions between periods where snow was the dominant water source and summer rain was the dominant water source. More details on this analysis can be found in the publication: Persistence and Plasticity in Conifer Water Use Strategies. JGR Biogeoscience. DOI 10.1029/2018JG004845. The dataset specifically includes stable isotope measurements of xylem and soil water for Spruce and Fir trees at the Rocky Mountain Biological Lab's Research Meadow as well as snowpack and precipitation stable isotopes from nearby National Atmospheric Deposition Program sites. Associated meteorological data is included, which is needed to understand the source water for the trees based on the cellulose measurements.This dataset was updated in June 2021 also include intra-ring measurements of the d18O and d13C of cellulose these same species of trees at the Ziegler Reservoir site in Snowmass, CO. These are listed as files: "Interglaciald18OCellulose.csv", "Interglaciald13OCellulose.csv" and "Modernd13CCellulose.csv". The intent of these measurements was to assess whether common conifers (abies and picea) had undergone ecophysiological or ecohydrological changes during the last period in Earth's history was warmer than today, i.e. the last Interglacial (116,000 to 130,000 years ago). This site was chosen because it is a location where subfossil wood from this critical warm period was discovered. We measured the d18O and d13C of the subfossil trees following the same protocol as the modern samples which included chemical extraction of cellulose and isotope ratio mass spectrometry. We found that the trees showed little difference in water use efficiency but utilized more summer rain during the interglacial period. This analysis and detailed methods are provided in the following manuscript: Wetter summers mitigated temperature stress on Rocky Mountain forests during the last interglacial warm period which is in revision at GRL but is available as a preprint here: 10.1002/essoar.10506740.2

54 ENVIRONMENTAL SCIENCES↗

Measurements and modeling of CO 2 concentration and isotopes to improve process-level understanding of Arctic and boreal carbon cycling. Final Report

The major goal of this project was to improve understanding of processes that control the exchanges of CO 2 between the atmosphere and the land biosphere on decadal and longer time scales. The approach involves measuring the changes in atmospheric CO 2 concentration and the isotopes of CO 2 ( 13 C/ 12 C and 18 O/ 16 O) at background stations and uses these and other datasets to challenge and improve numerical models of the earth system. The project particularly emphasized the use of these data to improve understanding of changes occurring in boreal and arctic ecosystems over the past 50 years and to seek from these data improved understanding of large-scale processes impacting carbon cycling, such as the responses to warming, CO 2 fertilization, and disturbance. The project also led to advances in the understanding of changes in water-use efficiency of land ecosystems globally based on trends in 13 C/ 12 C. The core element of this project was providing partial support for continuing measurements of CO 2 concentrations and isotopes from the Scripps CO 2 program, initiated by C. D. Keeling in the 1960s. The measurements included analysis of flasks collected at an array of ten stations distributed from the Arctic to the Antarctic. The project also supported modeling studies and interpretive work to help understand the origins of the large ~50% increase in the amplitude of the atmospheric CO 2 cycle detected at high northern latitudes between 1960 and present and to understand the long-term trend in carbon 13 C/ 12 C of CO 2 . The seasonal cycle work was advanced through collaborations with colleagues at MPI Jena and Imperial College

47 OTHER INSTRUMENTATION↗

Analytical Radiochemical Method Development for Mark 18A Program

The Savannah River National Laboratory Nuclear Measurements Group was tasked by the Mark 18A Program team with developing three analytical characterization methods. These methods will support process and waste characterization of the Mark 18A program material. While methods already existed for most analytes of interest to the Mark 18A program team, the Nuclear Measurements Group developed and refined methods to quantify the Cf isotopes, 107 Pd, and 121m Sn. The results of that effort are presented in this work. Methods were successfully developed to characterize the Mark 18A samples for the needed isotopes and the NMG is ready to receive Mark 18A program samples.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

R -Matrix Analysis and Statistical Properties of Dysprosium Isotopes in the Neutron Energy Ranges Up To A Few Kev

In support of the Nuclear Criticality Safety Program, a set of evaluated resonance parameters was generated for seven dysprosium isotopes in the neutron energy range from thermal up to a few keV. The evaluation methodology used the Reich-Moore approximation to fit, with the R-matrix code SAMMY, the high-resolution capture and transmission measurements on natural and enriched samples recently performed at the Rensselaer Polytechnic Institute Gaerttner LINear ACcelerator facility. Additional transmission data measured on enriched samples by Liou at the Columbia University Nevis synchrocyclotron in the mid-seventies were used to gauge the neutron widths above 15 eV. Thermal constants such as absorption and (in)coherent scattering cross sections and corresponding scattering lengths were calibrated to the National Institute of Standards and Technology’s compilation except for 161,164 Dy isotopes.

07 ISOTOPE AND RADIATION SOURCES↗

Mo-99 Concentration and processing by Solvent Extraction and Ion Exchange

Normally derived from its transient-equilibrium parent molybdenum-99 ( 99 Mo) (t½ = 66 h), the short-lived isotope technetium-99m ( 99m Tc) (t ½ = 6.0 h) is the most widely used medical isotope in diagnostic imaging today. The National Nuclear Security Administration’s (NNSA’s) Material Management and Minimization (M3) program—established under the auspices of the American Medical Isotope Production Act—has been tasked with facilitating the work of domestic 99 Mo suppliers that do not use highly enriched uranium (HEU). Superconducting electron linear accelerators that employ high-Z converter targets can generate bremsstrahlung photons and neutron fluxes that can induce photonuclear reactions and uranium (U) fission. Argonne, in collaboration with industrial partners, has been developing the process chemistry for superconducting linear accelerator (LINAC)-irradiated triuranium octoxide (U 3 O 8 ) targets to produce 99 Mo. In short, the process involves dissolving the irradiated targets in nitric acid, which simultaneously releases valuable fission products (xenon and iodine). After adjusting the acid concentration, producers process the feed using tri-n-butyl phosphate (TBP), then mix the raffinate derived from this extraction cycle with a phosphinic acid such as Cyanex 272 or di(2-ethylhexyl) phosphoric acid (HDEHP), which is selective for Mo (molybdenum liquid liquid extraction [MoLLE]). In the next step, a concentration column comprising an anion exchange platform is used to decontaminate the remaining fission products, generating a pure 99 Mo stream in sodium hydroxide (NaOH)/sodium chloride (NaCl).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Analysis Report for Hydrolyzed UF 6 Samples

Under the auspices of the US Department of Energy/National Nuclear Security Agency’s Nuclear Reference Material Program (NRMP), the Material Signatures and Isotopic Standards (MSIS) group of Oak Ridge National Laboratory was tasked with analyzing two UF6 filled hoke tubes for uranium isotopic composition. This report documents the results of the measurements performed by the MSIS group’s International Organization for Standardization/International Electrotechnical Commission 17025:2017 accredited operating procedure CSD-AM-CIMS-IN20, Determination of Uranium and Plutonium Isotopic Composition using Thermal Ionization Mass Spectrometry, and in accordance with the quality assurance plan as described in QAP-X-96-CSD/RML-001, Nuclear Analytical Chemistry Laboratory Section Quality Assurance Plan.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

ORNL Report for Hydrolyzed UF 6 Samples 439451, 438792, 439144, 439616, and 439617

Under the auspices of the US Department of Energy/National Nuclear Security Agency’s Nuclear Reference Material Program (NRMP), the Material Signatures and Isotopic Standards (MSIS) group of Oak Ridge National Laboratory was tasked with analyzing five UF 6 filled P-10 tubes for uranium isotopic composition. This report documents the results of the measurements performed by the MSIS group’s International Organization for Standardization/International Electrotechnical Commission 17025:2017 accredited operating procedure CSD-AM-CIMS-IN20, Determination of Uranium and Plutonium Isotopic Composition using Thermal Ionization Mass Spectrometry, and in accordance with the quality assurance plan as described in QAP-X-96-CSD/RML-001, Nuclear Analytical Chemistry Laboratory Section Quality Assurance Plan.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

ORNL Report of Analysis for the Verification of NRMP CRM U030A

In support of the Certified Reference Material (CRM) program managed by the Nuclear Reference Material Program (NRMP), the Material Signatures and Isotopic Standards (MSIS) group of Oak Ridge National Laboratory (ORNL) was asked to prepare a set of CRM U030A units for use as standards for isotopic analysis using multicollector thermal ionization mass spectrometry (TIMS) and inductively coupled plasma mass spectrometry (ICP-MS) instruments. This report documents the results of the verification measurements performed on three randomly selected units by the MSIS group’s ISO/IEC 17025:2017 accredited operating procedure CSD-AM-CIMS-IN20, Determination of Uranium and Plutonium Isotopic Composition using Thermal Ionization Mass Spectrometry [1], and in accordance with the quality assurance plan as described in QAP-X-96-CSD/RML-001, Nuclear Analytical Chemistry Laboratory Section Quality Assurance Plan [2].

Mathew, Kattathu [Oak Ridge National Laboratory (O↗

Offsite Source Recovery Program; High Activity Beta Gamma Removal, Transport and Disposition - 19663

The Department of Energy's (DOE) National Nuclear Security Administration's (NNSA) Office of Radiological Security's (ORS) Off-Site Source Recovery Program (OSRP) has been tasked with the removal and disposition of radioactive sealed sources in the interest of national security and public health and safety. It is the mission of the program to recover radioactive sources to prevent them from falling into the hands of individuals who would use this material for malicious intent. OSRP is a collaborative effort involving Los Alamos National Laboratory (LANL), Idaho National Laboratory (INL), and Lawrence Livermore National Laboratory (LLNL). At the inception of the program, Pu-239 was the only isotope acceptable for recovery. As a wider security scope developed, OSRP expanded its mission to include the recovery of other sources that posed a potential risk to national security, health, and safety. Starting in 2004, OSRP began recovering cesium and cobalt devices, largely from medical, research, and industrial facilities. These disused higher-activity devices present a burden to licensees in terms of security, and demand for OSRP's assistance in removing them has been high. Today, OSRP removes around 40 high-activity devices per year in support of domestic demand as well as ORS's Cesium Irradiator Replacement Project (CIRP). This represents an average of over 50,000 Ci of Cs-137 and Co-60 removed from the private sector each year for permanent disposition. A major component of this effort is the use of the proper shipping container to transport the devices. As a way to increase transportation capabilities ORS has developed two new Type B containers. The most recently completed of these containers, the 435-B, is currently certified to transport Gammators and Gammacell-1000, -3000, and -40 irradiators in an overpack configuration. This provides greater capacity and flexibility to safely and effectively transport these devices, for which acceptable shipping configurations had been previously limited. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Development of eXternal Nuclear Reaction Analysis (XNRA) Detection Technique for Quantifying Light Isotope Concentrations

The National Nuclear Security Administration’s Tritium Sustainment Program is responsible for the design, development, demonstration, testing, analysis, and characterization of tritium-producing burnable absorber rods (TPBARs) and their components used to produce tritium for the nation’s strategic stockpile. The FY19 call for proposals included the specific basic science research topic, “Demonstration and evaluation of advanced characterization methods, particularly for quantifying the concentration of light isotopes ( 1 H, 3 H, 3 He, and 4 He, 6 Li and 7 Li) in metal or ceramic matrices”. Last year the same language appeared in the call for proposals, and a project IWO-389859 was awarded to the Ion Beam Lab (IBL) at Sandia-NM which was successful using Elastic Recoil Detection, but in the future could have resulted in tritium contamination that jeopardized other equally important NNSA projects. An alternative approach using deuterium nuclear reaction analysis was proposed and funded in FY2019 which was also successful and eliminated any possibility of contaminating the Ion Beam Laboratory with tritium, and will be described in this report.

61 RADIATION PROTECTION AND DOSIMETRY↗

Perspectives on Few-Body Cluster Structures in Exotic Nuclei

It is a fascinating phenomenon in nuclear physics that states with a pronounced few-body structure can emerge from the complex dynamics of many nucleons. Such halo or cluster states often appear near the boundaries of nuclear stability. As such, they are an important part of the experimental program beginning at the Facility for Rare Isotope Beams (FRIB). A concerted effort of theory and experiment is necessary both to analyze experiments involving effective few-body states, as well as to constrain and refine theories of the nuclear force in light of new data from these experiments. Here, as a contribution to exactly this effort, this paper compiles a collection of “perspectives” that emerged out of the Topical Program “Few-body cluster structures in exotic nuclei and their role in FRIB experiments” that was held at FRIB in August 2022 and brought together theorists and experimentalists working on this topic.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Gas stopping and reacceleration techniques at the Facility for Rare Isotope Beams (FRIB)

The Facility for Rare Isotope Beams (FRIB) at Michigan State University provides a wide range of beams and energies for science with fast, stopped and reaccelerated rare-isotope beams. FRIB was commissioned in 2022 with the science program beginning in May 2022. Here, the combination of fast beams followed by gas stopping of rare-isotope beams together with reacceleration is unique to FRIB. Stopping techniques and beam manipulation at very-low energies are important to slow down fast beams for use in either stopped-beam experimental devices, or subsequent injection in the reaccelerator for experiments at energies ranging from 0.3 MeV/u to 12 MeV/u, depending on the Q/A of the ion. Innovative stopped-beam techniques to optimize the stopping and extraction efficiencies across a wide range of atomic numbers, as well as to reduce contamination and increase extraction speed, were developed. Reacceleration of those beams involve cooling, bunching, charge breeding and acceleration by a state-of-the-art superconducting reaccelerator, ReA. In this contribution we present the latest results of various gas stoppers and techniques to eliminate contaminants after reacceleration by the ReA.

43 PARTICLE ACCELERATORS↗

Minor Actinide Production at Oak Ridge National Laboratory

The U.S. Department of Energy (DOE) manages an inventory of nuclear materials containing a range of long-lived radioactive isotopes. They were produced from the 1960s through the 1980s by irradiating targets in production reactors and in the High Flux Isotope Reactor, a research reactor commissioned at Oak Ridge National Laboratory (ORNL) in 1967, to produce special heavy isotopes for DOE programmatic use, scientific research, and industrial and medical applications. ORNL uses these transuranium isotopes (plutonium through californium) for the heavy-element research program and other R&D needs. As a result, ORNL has extensive experience in the production of transuranium isotopes. An effort is under way to review and document the techniques for the production of minor actinides, which are the actinide elements in used fuels other than uranium and plutonium (e.g., neptunium, americium, curium) at ORNL.

Patton, Bradley↗