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At least 109 records · Page 6

Additively Manufactured Pressure Limiting Irradiation Capsule for the High Flux Isotope Reactor

The Advanced Materials and Manufacturing Technologies (AMMT) program previously demonstrated an additively manufactured (AM) irradiation capsule (commonly referred to as a “rabbit”) from 316H stainless steel (SS) for insertion into the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL)1. This report details efforts to design and fabricate an AM pressure limiting structure (PLS) into one of the end caps of a rabbit capsule and qualify it for insertion into HFIR. The PLS includes a thin cylindrical rupture wall, a shield, and internal supports to facilitate printing and ensure mechanical integrity. Its overall dimensions are 9-mm tall and 10-mm in diameter— equivalent to about one-fourth of the size of a AAA battery. The PLS maintains safe internal operating pressures for a rabbit capsule while in the reactor. Although this application is specific to HFIR, the approach lends itself to further applications in industrial, aeronautical, advanced space and power generation environments. Several PLS rabbits capsules have been successfully designed, fabricated, pressure tested, and qualified for future insertion into the HFIR for irradiation and post-irradiation evaluation.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Electrochemical Kinetics of Stable Isotopes (Final Report)

Stable isotopes are sensitive indicators to the mass transport and chemical reactions that occur during potentiostat-controlled electroplating of metals from aqueous (and some non-aqueous) metal-salt solutions. The goal of this research program is to measure the stable isotope fractionation during electrochemical processes, how the isotope-dependent rates are sensitive to chemistry, temperature, and electrochemical kinetics, and to use these measurements to develop a theoretical framework for a kinetic isotope effect that is able to predict kinetic isotope fractionation factors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atomic Beam Laser Spectrometer for In-field Isotopic Analysis

This is a powerpoint presentation for the DTRA quarterly program review that goes into detail about the atomic beam laser spectrometer for in-field isotopic analysis. The project goals are the following: analysis of post-detonation debris, determination of U and Pu isotopic composition, and fieldable prototype: < 2ft 3 , < 1000W.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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↗

Beam dynamics simulations of post low energy beam transport section in RAON heavy ion accelerator

RAON (Rare isotope Accelerator Of Newness) heavy ion accelerator of the rare isotope science project in Daejeon, Korea, has been designed to accelerate multiple-charge-state beams to be used for various science programs. In the RAON accelerator, the rare isotope beams which are generated by an isotope separation on-line system with a wide range of nuclei and charges will be transported through the post Low Energy Beam Transport (LEBT) section to the Radio Frequency Quadrupole (RFQ). In order to transport many kinds of rare isotope beams stably to the RFQ, the post LEBT should be devised to satisfy the requirement of the RFQ at the end of post LEBT, simultaneously with the twiss parameters small. We will present the recent lattice design of the post LEBT in the RAON accelerator and the results of the beam dynamics simulations from it. In addition, the error analysis and correction in the post LEBT will be also described.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Recent activities for β-decay half-lives and β-delayed neutron emission of very neutron-rich isotopes

Beta-delayed neutron (βn) emitters play an important, two-fold role in the stellar nucleosynthesis of heavy elements in the 'rapid neutron-capture process' (r process). On one hand they lead to a detour of the material β-decaying back to stability. On the other hand, the released neutrons increase the neutron-to-seed ratio, and are re-captured during the freeze-out phase and thus influence the final solar r-abundance curve. A large fraction of the isotopes inside the r-process reaction path are not yet experimentally accessible and are located in the (experimental) 'Terra Incognita'. With the next generation of fragmentation and ISOL facilities presently being built or already in operation, one of the main motivation of all projects is the investigation of these very neutron-rich isotopes. A short overview of one of the planned programs to measure βn-emitters at the limits of the presently know isotopes, the BRIKEN campaign (Beta delayed neutron emission measurements at RIKEN) will be given. Presently, about 600 β-delayed one-neutron emitters are accessible, but only for a third of them experimental data are available. Reaching more neutron-rich isotopes means also that multiple neutron-emission becomes the dominant decay mechanism. About 460 β-delayed two-, three-or four-neutron emitters are identified up to now but for only 30 of them experimental data about the neutron branching ratios are available, most of them in the light mass region below A=30. The International Atomic and Energy Agency (IAEA) has identified the urgency and picked up this topic recently in a 'Coordinated Research Project' on a 'Reference Database for Beta-Delayed Neutron Emission Data'. This project will review, compile, and evaluate the existing data for neutron-branching ratios and half-lives of β-delayed neutron emitters and help to ensure a reliable database for the future discoveries of new isotopes and help to constrain astrophysical and theoretical models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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↗

The interactions of atmospheric cosmogenic radionuclides with spacecraft surfaces

The discovery of the cosmogenic radionuclide Be-7 on the front surface (and the front surface only) of the Long Duration Exposure Facility (LDEF) spacecraft has opened opportunities to investigate new phenomena in several disciplines of space science. The experiments performed for this work show that the Be-7 results only if the source of the isotope is the atmosphere through which the spacecraft passed. We should expect that the uptake of beryllium in such circumstances will depend on the chemical form of the Be and the chemical nature of the substrate. It was found that the observed concentration of Be-7 does, in fact, differ between metal surfaces and organic surfaces such as PTFE (teflon). It is noted, however, that: (1) organic surfaces, even PTFE, are etched by the atomic oxygen found under these orbital conditions, and (2) the relative velocity of the species is 8 km(exp -1)s relative to the surface and the interaction chemistry and physics may differ from the norm. The Be-7 is formed by spallation of O and N nuclei under cosmic ray proton bombardment. The principal source region is at altitudes of 12-15 km. While very small quantities are produced above 300 km, the amount measured on the LDEF was 3 to 4 orders of magnitude higher than expected from production at orbital attitude. The most reasonable explanation is that Be-7 is rapidly transported from low altitudes by some unknown mechanism. The process must take place on a time scale similar to the half-life of the isotope (53 days). Many other isotopes are produced by cosmic ray reactions, and some of these are suited to measurement by the extremely sensitive methods of accelerator mass spectrometry. A program was initiated to search for these isotopes and it is hoped that such studies will provide new methods for studying mixing in the upper atmosphere.

Gregory, John C.↗

The interactions of atmospheric cosmogenic radionuclides with spacecraft surfaces

The discovery of the cosmogenic radionuclide Be-7 on the front surface of the Long Duration Exposure Facility (LDEF) spacecraft has opened opportunities to investigate new phenomena in several disciplines of space science. The experiments performed for this work show that the Be-7 results only if the source of the isotope is the atmosphere through which the spacecraft passed. We should expect that the uptake of beryllium in such circumstances will depend on the chemical form of the Be and the chemical nature of the substrate. It was found that the observed concentration of Be-7 does, in fact, differ between metal surfaces and organic surfaces such as PTFE (teflon). It is noted, however, that: (1) organic surfaces, even PTFE, are etched by the atomic oxygen found under these orbital conditions, and (2) the relative velocity of the species is 8 km(exp -1)s relative to the surface and the interaction chemistry and physics may differ from the norm. The Be-7 is formed by spallation of O and N nuclei under cosmic ray proton bombardment. The principal source region is at altitudes of 12-15 km. While very small quantities are produced above 300 km, the amount measured on the LDEF was 3 to 4 orders of magnitude higher than expected from production at orbital altitude. The most reasonable explanation is that Be-7 is rapidly transported from low altitudes by some unknown mechanism. The process must take place on a time scale similar to the half-life of the isotope (53 days). Many other isotopes are produced by cosmic ray reactions, and some of these are suited to measurement by the extremely sensitive methods of accelerator mass spectrometry. A program was initiated to search for these isotopes and it is hoped that such studies will provide new methods for studying mixing in the upper atmosphere.

Gregory, J. C.↗

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↗

The continuous measurement of hydrogen chloride in the ambient atmosphere using the dual isotope infrared absorption technique

The results of a program to develop a prototype gas filter correlation NDIR analyzer capable of providing the required HCl measurement capability, while maintaining an adequate rejection of any other gases anticipated in the atmosphere are presented. Examples of the performance of the prototype analyzer are presented which show an rms noise equivalent concentration of 0.06 ppm of HCl was achieved while maintaining an electronically determined 10% to 90% time response to gas samples of about 2 seconds. No measureable response was observed to CO2, CO, and H2O while maintaining an adequate rejection of the hydrocarbons, for example CH4 and n-hexane. The experiments were performed which demonstrate that the span stability of the HCl gas filter correlation analyzer is unaffected by the presence of water vapor and which support the belief that the incorporation of a relatively open-volume, multiple path sample cell into the instrument would enable ground station as well as airborne measurements of trace quantities of HCl in the ambient atmosphere to be performed.

Williams, K. G.↗

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↗

Implementation of Arizona's nuclear future 153192.doc10 - 15319

The Arizona Energy Education Fund (AEEF), now a 501(c) (3) non-profit entity, is an assembly of stakeholders from the private sector, government, education and energy industries dedicated to supporting K-12 (kindergarten through 12. grade), community colleges and universities through an enhanced program of smart nuclear generator expansion, isotope production, testing of breeder reactor power plants, recycling spent nuclear fuel in power generation facilities, and nuclear fuel cycle support. AEEF priorities are to collaborate with stakeholders in Arizona to develop safe plans that will make Arizona the most nuclear friendly state benefiting all stakeholders. Long-term plans include promoting: - education of K-12 students as well as the general Arizona population so that they fully understand the benefits and safe use of nuclear power; - reliable supply of medical and industrial radioisotopes; - Arizona as host of new reactor concepts which are being developed and demonstrated; - development of nuclear engineering programs in Arizona universities to drive the development of the next generation of nuclear power plants; and - supply of nuclear-generated electricity to California and Sonora, Mexico to power desalinisation plants in exchange for Colorado River water currently allocated to California and Sonora. The development described will generate significant long-term employment for Arizona while delivering a critical service to the nation. Arizona's location advantages include the lack of significant seismic activity, hurricanes, tsunamis, floods or frigid weather. Interstate highways and railroads are well developed and provide good, all-weather access to many potential development sites. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

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

The resolved resonance region evaluation for the only two natural isotopes of copper ({sup 63}Cu and {sup 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. The particular set of four Zeus experiments had a highly-enriched uranium core with a thick copper-reflector resulting in a large sensitivity of the criticality of these systems to the cross section of copper in the intermediate energy range. Sobes et al. presented the effect of the newly resolved resonance region evaluations for the two isotopes of copper on the Zeus integral benchmarks, as well as 23 other benchmarks from the ICSBEP during the 2016 ANS Annual Meeting. The results presented in Ref. were calculated with the ENDF/B-VII.1 cross section libraries used for all other materials. However, it is suggested that the resolved resonance region evaluations for the isotopes of copper should not be judged only on their performance in the integral benchmark calculations especially when the ENDF/B-VII.1 cross sections are used for all of the other isotopes. Three reasons are provided for this. First and foremost, a new evaluation is an assessment of the physics of the nucleus of the particular isotope, and the goal of an application agnostic nuclear data evaluation is to improve evaluation by fitting state-of-the art R-Matrix formalism to highly precise experimental cross section measurements. The improved performance in the integral benchmarks should only come as a consequence of the improvement in the physics of the evaluation. Secondly, there is some uncertainty in the nuclear data evaluation of the cross section of all isotopes, so there could be some error in evaluating another isotope used in calculating the integral benchmark experiment. Such an error may have been having a compensating effect, in combination with the previous evaluations for the isotopes of copper. Thirdly, with the two isotopes of copper proposed for inclusion in the upcoming release of the ENDF/B-VIII library, performance of the new resonance evaluation for copper should be evaluated based on the calculation of the integral benchmarks with all of the evaluations proposed for inclusion in the ENDF/B-VIII release. These benchmarking results using the ENDF/B-VIII evaluations as they converge closer to their final form will be presented at the conference. This summary stresses the importance of the physics of the evaluation and reviews some of the steps taken in finalizing a resolved resonance region evaluation. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

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↗