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DOE OSTI2023

Short-lived noble gas effluent trends from a research reactor

An understanding of anthropogenic sources of radioactive noble gases in the atmosphere is needed to enhance the discrimination ability of the International Monitoring System's sensors. These sources include commercial and research nuclear reactors and medical isotope production facilities. While abiding by local environmental ordinances these facilities all emit noble gas radioisotopes through normal operation. Here, this research presents measurements and analysis of noble gas isotopes ( 41 Ar, 135 Xe, 135m Xe, 137 Xe, 138 Xe, 87 Kr, 88 Kr, and 89 Kr) made directly at the stack of the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory. The Xe and Kr noble gases are concurrently observed with 41 Ar, a neutron activation product, when the reactor is operational. The magnitude of the Xe and Kr noble gases released is not constant over the HFIR cycle, but they temporally match the 41 Ar trend. An isotope activity ratio analysis of these shorter lived isotopes combined with the observation of the cycle's temporal trend helps understand the noble gas production mechanism at the HFIR. Isotopes with short half-lives are not useful for long-range environmental monitoring. However, these measurements could potentially be combined with atmospheric modeling to predict the background source term of the longer-lived Xe ratios at a monitoring station.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2025

The lessons learned from ephemeral nuclei

Recent experimental analyses of fleeting clusters of protons and neutrons put the very notion of the atomic nucleus in a new light.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Molecular Dynamics Simulations of Helium Bubble Formation in Palladium Tritides [Slides]

Pd readily absorbs hydrogen and its isotopes, and can be used to purify gas mixtures involving tritium. Tritium decays to He, forming He bubbles. Bubbles causes possible PCT effects swelling, He release, all leading to failures. Radioactive decay experiments take many years. Molecular dynamics (MD) studies can be quickly done. No previous MD methods can simulate He bubble nucleation and growth.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2020

Molecular Dynamics Simulations of Helium Bubble Formation in Palladium Tritides [Slides]

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

Laser spectroscopy for the study of exotic nuclei

Investigation into the properties and structure of unstable nuclei far from stability is a key avenue of research in modern nuclear physics. These efforts are motivated by the continual observation of unexpected structure phenomena in nuclei with unusual proton-to-neutron ratios. In recent decades, laser spectroscopy techniques have made significant contributions in our understanding of exotic nuclei in different mass regions encompassing almost the entire nuclear chart. This is achieved through determining multiple fundamental properties of nuclear ground and isomeric states, such as nuclear spins, magnetic dipole and electric quadrupole moments and charge radii, via the measurement of hyperfine structures and isotope shifts in the atomic or ionic spectra of the nuclei of interest. These properties offer prominent tests of recently developed state-of-the-art nuclear theory and help to stimulate new developments in improving the many-body methods and nucleon–nucleon interactions at the core of these models. With the aim of exploring more exotic short-lived nuclei located ever closer to the proton and neutron driplines, laser spectroscopy techniques, with their continuous technological developments towards higher resolution and higher sensitivity, are extensively employed at current- and next-generation radioactive ion beam facilities worldwide. Ongoing efforts in parallel promise to improve the availability of these even more exotic species at next-generation facilities. Very recently, an innovative application of laser spectroscopy on molecules containing short-lived nuclei has been demonstrated offering additional opportunities for several fields of research, e.g. fundamental symmetry studies and astrophysics. Here, in this review, the basic nuclear properties measurable with laser spectroscopy will be introduced. How these observables are associated with nuclear structure and nucleon–nucleon interactions will be discussed. Following this, a general overview of different laser spectroscopy methods will be given with particular emphasis on technical advancements reported in recent years. The main focus of this article is to review the numerous highlights that have resulted from studying exotic nuclei in different mass regions with laser spectroscopy techniques since the last edition in this series. Finally, the challenges facing the field in addition to future opportunities will be discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NASA NTRS1993

Al-26-Mg-26 ages of iron meteorites

An exposure age for an iron meteorite can be calculated from measurements of a radioactive nuclide and a stable nuclide that are produced by similar sets of nuclear reactions, provided that the stable nuclide is present with low initial abundance. The standard methods rely on either K-40 (t(sub 1/2) = 1.26 Gy), K-39, and K-41 or on a shorter-lived radionuclide and a stable, noble gas isotope. Widely used pairs of this type include Cl-36/Ar-36 and Al-26/Ne-21. Other pairs that may serve the purpose for iron meteorites contain many stable isotopes besides those of K and the noble gases that are produced partly by cosmic rays. We consider here the calculation of exposure ages, t(sub 26), from measurements of Al-26 (t(sub 1/2) = 0.7 My) and (stable) Mg-26. Ages based on Al-26/Mg-26 ratios, like those based on Cl-36/Ar-36 ratios, are 'buffered' against changes in relative production rates due to shielding because decay of the radioactive nuclide accounts for a good part of the inventory of the stable nuclide.

Herzog, G. F.↗

DOE OSTI2025

Angular Correlations of Gamma Rays from Fission Product Solution

Fission products from photon-induced fission are routinely used at Idaho National Laboratory as part of nuclear forensics activities. Typically, the focus is on fission products with relatively large fission yields (Ba-140, Mo-99, etc.). The nuclear data associated with the well-known isotopes have small uncertainties, and many have well-known angular correlations between emitted gamma-rays, if applicable. However, for isotopes with smaller fission yields or less intense gamma-ray emission intensities, the nuclear decay schemes and gamma-ray emission intensities may be less well-known. The Germanium Rotational Measurements for Angular Correlation (GeRMAC) system was designed to use two high-purity germanium (HPGe) detectors in a coincidence counting set-up but allows one of the HPGe detectors to rotate at a constant distance from a radioactive source, changing the relative angle between the two HPGe detectors. Angular correlations can then be determined from the relative photopeak areas between two gamma-rays emitted as part of the same nuclear decay. By recording the HPGe spectra in list mode, the angular correlations of gamma-rays emitted from complex sources, consisting of multiple isotopes, can be measured simultaneously and the individual isotope emissions can be isolated. Using the GeRMAC system, a multi-isotope fission product source, produced with photon-induced fission of U-238, was measured using a single rotational arc (180 degrees) to obtain the angular correlation between gamma-rays emitted by the large number of fission products contained in the solution with an angular accuracy of 1 degree. In particular, La-140 (38 gamma rays) and Nd-147 (26 gamma rays) are of interest to the nuclear forensics community.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

DOE OSTI2022

Options for the Removal of Cesium and Strontium from Acidic Uranyl Sulfate Solutions from Molybdenum-99 Production

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 R91290-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, but CST should be investigated at a higher pH. Limited removal of transuranic species and almost no removal of uranium was observed in this testing. 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 the range of 0.2 to 5 mg Cs per gram of absorbent appears to be achievable.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Evaluation of SNOLAB background mitigation procedures through the use of an ICP-MS based dust monitoring methodology

Dust particulate fallout on materials in use for rare-event searches is a concerning source of radioactive backgrounds due to the presence of the naturally occurring radionuclides 40 K, 232 Th, 238 U, and their progeny in dust. Much effort is dedicated to inform radioactive backgrounds from dust and evaluate the efficacy of mitigation procedures. A great portion of such effort relies on fallout models and assumed dust composition. Here, in this work, an ICP-MS based methodology was employed for a direct determination of fallout rates of radionuclides and stable isotopes of interest from dust particulate at the SNOLAB facility. Hosted in an active mine, the SNOLAB underground laboratory strives to maintain experimental areas at class 2000 cleanroom level. This work validates the mitigation procedures in place at SNOLAB and informs dust backgrounds during laboratory activities. Fallout rates of major constituents of the local rock were measured two to three orders of magnitude lower in the clean experimental areas compared to non-clean transition areas from the mine to the laboratory. An increase of approximately two orders of magnitude in the fallout rate of stable Pb isotopes was determined in an experimental area during activities involving handling of Pb bricks. Increased 40 K, 232 Th, and 238 U fallout rates were measured in clean experimental areas during activities generating particulate.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Production of Precursor Materials for the Development of Iron-Based Superconductor (IBS) Wire

The objective of the activities under this Annex is to address the extrinsic Jc limitations uncovered in pioneering work. In order to engineer the defects pinning landscape charged particle irradiations experiments on bulk samples, different doping and chemical additions will be performed at different National facilities (Test Beam Facility at Fermilab; Linac Isotope Producer at Brookhaven National Laboratory; Integrated Biology Laboratory at University of Wisconsin-Madison; Facility for Rare Isotope Beams at Michigan State University). The samples will be produced at ENEA by different techniques. Magnetization and advanced microscopy measures will be performed at Fermilab. After irradiation, depending on the level of radioactivity, the samples will be tested at Fermilab or where it is possible to measure radioactive materials as University of Wisconsin-Madison.

43 PARTICLE ACCELERATORS↗

NASA NTRS1965

Chromium isotopes in meteorites.

Isotopic composition of Cr in meteorites indicates lack of high energy proton irradiation in early solar system

RADIOACTIVE DATING↗

DOE OSTI2023

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↗

NASA NTRS1993

Radioactivities induced in some LDEF samples

Radioactivities induced in several Long Duration Exposure Facilities (LDEF) samples were measured by low-level counting at Los Alamos and elsewhere. These radionuclides have activities similar to those observed in meteorites and lunar samples. Some trends were observed in these measurements in terms of profiles in trunnion layers and as a function of radionuclide half-life. Several existing computer codes were used to model the production by the protons trapped in the Earth's radiation belts and by the galactic cosmic rays of some of these radionuclides, Mn-54 and Co-57 in steel, Sc-46 in titanium, and Na-22 in alloys of titanium and aluminum. Production rates were also calculated for radionuclides possibly implanted in LDEF, Be-7, Be-10, and C-14. Enhanced concentrations of induced isotopes in the surfaces of trunnion sections relative to their concentrations in the center are caused by the lower-energy protons in the trapped radiation. Secondary neutrons made by high-energy trapped protons and by galactic cosmic rays produce much of the observed radioactivities, especially deep in an object. Comparisons of the observed to calculated activities of several radionuclides with different half-lives indicate that the flux of trapped protons at LDEF decreased significantly at the end of the mission.

Reedy, Robert C.↗

DOE OSTI2020

Full-Scale Implementation of Propane Biosparge System for In-Situ Remediation of 1,4-Dioxane - 20174

1,4-Dioxane is a common co-contaminant with chlorinated solvents but is not readily remediated via similar treatment approaches (e.g., sorption, reductive dechlorination). However, 1,4-dioxane can be cometabolically biodegraded in the presence of alkane gases and oxygen. At Vandenberg Air Force Base in California, USA, historical use of chlorinated solvents resulted in 1,4-dioxane in groundwater across three vertical groundwater zones. Between April 2013 and December 2016, laboratory testing and various field demonstrations were conducted by us, and others. The results from these tests showed in-situ propane biosparging as a promising technology for reduction of both chlorinated solvent and 1,4-dioxane concentrations, with up to 99 percent reduction in groundwater concentrations. Stable isotope probing (SIP) was also used in 2015 to verify that biodegradation was a (destructive) mechanism occurring in the subsurface.). The success of the propane biosparge demonstrations, and confirmation of the biodegradation mechanism via SIP, has led to the full-scale implementation of a propane biosparge treatment system at Site 24 at Vandenberg Air Force Base. The treatment area is a relatively small footprint (e.g., less than 61 meters (200 feet) long), with 83 new wells installed simultaneously across the three groundwater zones. Ultimately 93 wells will be connected to an above-ground treatment system the includes an air compressor, a propane tank, controls to ensure safe operating conditions, and nutrient amendment elements. This full-scale system is currently known to be among the first of its kind. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Applications of Hyporheic Zone Sampling for Assessing VOC Plume Engineered Remediation and Natural Attenuation Effectiveness - 20414

Determining the efficacy of engineered remedial actions and/or natural attenuation as an acceptable EPA Record of Decision (ROD) must address long-term temporal and spatial variability. Since final plume downslope destinations are aquifers and related surface streams and rivers, hyporheic zone sampling is essential. Comprehensive hyporheic sampling documents plume groundwater remediation prior to upwelling into stream benthic strata and natural attenuation within this dynamic zone itself. Our intensive sampling of the Savannah River Site (SRS) Chemical, Metals, and Pesticides (CMP) Pits VOC plume-fringe from 2005 to 2018 documented PCE natural attenuation and effectiveness of In Situ Thermal Treatment (ISTT). Most plume hyporheic upwelling was delimited to a 20 m inflow reach along Pen Branch. Our study utilized corroborative sampling methodologies: ambient hole-water grab samples: passive diffusion bags (PDB); and hole-core sediment samples to confirm station to station spatial and temporal trends. VOC hot spot detections were confirmed from both groundwater and soil core samples. VOC pathways through the Pen Branch hyporheic zone were assessed at hole-installation using sequential soil samples from augered cores and grab-samples of hole-bottom water. Longer term, composite water samples were collected from PDBs deployed for a minimum two-week equilibration period. Soil samples were collected from the 15 and 65 cm core levels in December 2017 and June 2018 at six stations. Additional core depths of 40 and 85 cm were sampled in June 2018 at the highest VOC station (5DB80). All samples were analyzed in an EPA certified lab by purge and trap GC-MS. Effectiveness of previous ISTT and soil vapor extraction (SVE) for this CMP Pits PCE plume, was clearly documented by significant downward trends in VOC at hyporheic zone stations prior to December 2015. Achieving final stage conversions of PCE daughter products to ethene and CO{sub 2} may be limited depending upon suitable interactions between hyporheic zone sediment morphology, hydrology, and redox conditions. Because declines in VOC daughter products at our hyporheic stations may also be caused by physical actions of dilution and dispersion rather than true biochemical dechlorination, full quantification of natural attenuation requires the use of compound-specific isotope ratio analysis (CSIA) and microbial 16S rRNA with qPCR. To assist these next-phase efforts, a natural attenuation index (NAI) was used to help produce quicker, more cost-effective decision making for locating CSIA and microbial sampling efforts. The NAI used natural logarithm transformed GC-MS results for station VOC degradation compounds versus VOC parent compounds. Wide differences were observed between stations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Production of Precursor Materials for the Development of Iron-Based Superconductor (IBS) Wire

The objective of the activities under this Annex is to address the extrinsic Jc limitations uncovered in pioneering work. In order to engineer the defects pinning landscape charged particle irradiations experiments on bulk samples with different doping and chemical additions will be performed at different National facilities (Test Beam Facility at Fermilab; Linac Isotope Producer at Brookhaven National Laboratory; Integrated Biology Laboratory at University of Wisconsin-Madison; Facility for Rare Isotope Beams at Michigan State University). The samples will be produced at TUAT by different synthesis techniques. Magnetization and advanced microscopy measures will be performed at Fermilab. After irradiation, depending on the level of radioactivity, the samples will be tested at Fermilab or where it is possible to measure radioactive materials as University of Wisconsin-Madison. In parallel, the precursor materials produced by TUAT will be used for IBS-wire fabrication at Fermi

43 PARTICLE ACCELERATORS↗

DOE OSTI2024

Modeling and Design of Micro Flux Monitors for Neutron Fluence Measurements

Measuring neutron flux is critical to understanding the characteristics of nuclear reactors and can provide information on the energy spectrum, total neutron fluence, and operational history of a facility. Such measurements are typically performed by irradiating high-purity materials in an operating reactor for a known length of time. By measuring and identifying activation products in the irradiated materials and referencing the energy-dependent cross section of each isotope, the neutron energy spectrum and total fluence can be determined. Historical techniques use a variety of small, individually pressed foils or wires for dosimeter devices, which can result in excessively high levels of radioactivity and complications in handling after irradiation. The present work describes a new neutron dosimetry concept, named the micro flux monitor, that uses semiconductor device fabrication processes to deposit thin films of flux monitoring materials in precise geometries onto a SiC wafer. This approach allows multiple dosimetry materials to be located on a single device, simplifying irradiation and subsequent analysis. The geometry, and therefore mass, of each material can be custom-tailored for a specific application—considering the expected neutron flux, duration of irradiation, and device retrieval time of a facility. Additionally, hundreds of identical dosimetry monitors can be produced simultaneously, reducing fabrication costs. Finally, the extremely thin metal dimensions of these devices could improve the fidelity of neutron fluence measurements by reducing neutron self-shielding and gamma self-attenuation effects.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

NASA NTRS2004

Chondrites and the Protoplanetary Disk, Part 3

Contents include the following: Ca-, Al-Rich Inclusions and Ameoboid Olivine Aggregates: What We Know and Don t Know About Their Origin. Aluminium-26 and Oxygen Isotopic Distributions of Ca-Al-rich Inclusions from Acfer 214 CH Chondrite. The Trapping Efficiency of Helium in Fullerene and Its Implicatiion to the Planetary Science. Constraints on the Origin of Chondritic Components from Oxygen Isotopic Compositions. Role of Planetary Impacts in Thermal Processing of Chondrite Materials. Formation of the Melilite Mantle of the Type B1 CAIs: Flash Heating or Transport? The Iodine-Xenon System in Outer and Inner Portions of Chondrules from the Unnamed Antarctic LL3 Chondrite. Nucleosynthesis of Short-lived Radioactivities in Massive Stars. The Two-Fluid Analysis of the Kelvin-Helmholtz Instability in the Dust Layer of a Protoplanetary Disk: A Possible Path to the Planetesimal Formation Through the Gravitational Instability. Shock-Wave Heating Model for Chonodrule Formation: Heating Rate and Cooling Rate Constraints. Glycine Amide Hydrolysis with Water and OH Radical: A Comparative DFT Study. Micron-sized Sample Preparation for AFM and SEM. AFM, FE-SEM and Optical Imaging of a Shocked L/LL Chondrite: Implications for Martensite Formation and Wave Propagation. Infrared Spectroscopy of Chondrites and Their Components: A Link Between Meteoritics and Astronomy? Mid-Infrared Spectroscopy of CAI and Their Mineral Components. The Origin of Iron Isotope Fractionation in Chondrules, CAIs and Matrix from Allende (CV3) and Chainpur (LL3) Chondrites. Protoplanetary Disk Evolution: Early Results from Spitzer. Kinetics of Evaporation-Condensation in a Melt-Solid System and Its Role on the Chemical Composition and Evolution of Chondrules. Oxygen Isotope Exchange Recorded Within Anorthite Single Crystal in Vigarano CAI: Evidence for Remelting by High Temperature Process in the Solar Nebula. Chondrule Forming Shock Waves in Solar Nebula by X-Ray Flares. Organic Globules with Anormalous Nitrogen Isotopic Compositions in the Tagish Lake Meteorite: Products of Primitive Organic Reactions. Yet Another Chondrule Formation Scenario. CAIs are Not Supernova Condensates. Microcrystals and Amorphous Material in Comets and Primitive Meteorites: Keys to Understanding Processes in the Early Solar System. A Nearby Supernova Injected Short-lived Radionuclides into Our Protoplanetary Disk. REE+Y Systematics in CC and UOC Chondrules. Meteoritic Constraints on Temperatures, Pressures, Cooling Rates, Chemical Compositions, and Modes of Condensation in the Solar Nebula. The I-Xe Record of Long Equilibration in Chondrules from the Unnamed Antarctic Meteorite L3/LL3. Early Stellar Evolution.

Source record↗