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At least 55 records · Page 3

Absolute mass calibration of fission product distributions measured with the E-$v$ method

The mass calibration of fission product distributions measured with the energy–velocity (E-v) method constitutes a technical challenge. The energy loss of the fission fragments in the various dead layers of the spectrometer and other sources of pulse-height defects of the energy detectors are a significant source of systematic uncertainty in the mass calculations used to determine the measured fission product yields. Here, in this study, the absolute calibration of the fission mass distributions is accomplished by measuring prompt γ-rays in coincidence with the fission fragments. This allows for the direct calibration of the mass spectra and eliminates any dependence on potentially complicated energy corrections. The first test measurement was performed at the Los Alamos Neutron Science Center employing the SPectrometer for Ion DEtermination in fission Research (SPIDER). SPIDER is a 2E-2v spectrometer designed for measuring independent fission product yields from neutron-induced fission. In this test, the single-arm SPIDER (E-v) system and an array of 252 Cf sources were used. The single-arm system consisted of two time pick-off detectors for measuring the time-of-flight of the fission fragments and a double-sided silicon strip detector (DSSD) for measuring the kinetic energy. Characteristic γ-rays from fission fragments were detected using three high-purity germanium (HPGe) detectors. For the mass calibration, γ–mass coincidence events from twelve product isotopes were used. The measured FPYs from 252 Cf spontaneous fission were found to be in excellent agreement with the evaluated data after applying the absolute mass calibration. From the γ–mass coincidence events, the mass resolution of the system was also extracted. An average mass resolution of ~1.4 AMU (FWHM) for the light fragments and ~2.4 AMU (FWHM) for the heavy fragments were found. This was the first in-situ calibration and characterization of the SPIDER spectrometer, which paves the way for high-quality FPY measurements with this instrument.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Simple separation of technetium from molybdenum for tracer isotope production

A procedure for the separation of technetium isotopes from bulk molybdenum was developed in nitric acid media. After irradiation of nat Mo foils, and dissolution in H 2 O 2 , the solution is acidified to 2 M HNO 3 , and anion exchange resin is used to separate technetium from molybdenum. The procedure is simple, requiring only basic laboratory equipment and, with a two-column separation, the technetium yield is high (~ 85%) with extremely high purity (< 0.1 ppm nat Mo). In conclusion, this is ideally suited for laboratory production of technetium tracer isotopes, particularly 95m Tc.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Improvements to the 115g/115m Cd Nuclear Data

Repeated measurements of the isotope 115m Cd by Los Alamos National Laboratory (LANL), Pacific Northwest National Laboratory (PNNL), and Atomic Weapons Establishment (AWE) have revealed a consistent discrepancy between beta and gamma counting. This suggests that a significant disparity exists between the true value of the isotope’s gamma-ray branching ratios and the values reported by the National Nuclear Data Center (NNDC). Enriched 114 Cd was irradiated using thermal neutrons to produce a high-purity 115m/g Cd source for counting and analysis using traditional singles gamma-ray spectroscopy, liquid scintillation counting, gas-proportional counting, and analysis using the new Gamma-Alpha-Beta-Gamma (GABγ) and Gamma-Alpha-Beta Radio-Isotope EvaLuator (GABRIEL) coincidence detection systems. Using the D-T fusion generated neutrons, reduces the wait time required to let the short-lived 115Cd ground state decay away by leveraging the 1:1 production ratio of the ground and metastable state of 115 Cd from the 115 In (n,p) reaction relative to the 10:1 production ratio of the ground and metastable isotopes of 115 Cd by thermal neutron capture on 114 Cd. However, the much higher flux in from the Washington State University TRIGA reactor is a more rapid method of production of 115m/gCd but requires access to enriched 114 Cd. High purity 115m/g Cd samples were analyzed on regular intervals over a period of 140-days. The activity of 115m Cd measured by beta and gamma show a clear discrepancy using the current best known gamma-ray decay branching ratios. Based on these observations and measurements, a set of new branching ratio recommendations have been produced using conventional counting techniques and the advanced GAB? and GABRIEL instruments.

07 ISOTOPE AND RADIATION SOURCES↗

Monitoring Methods for Early Detection of Inadvertent Fission Product Release at the Advanced Test Reactor

Isotope effluent data obtained during three instances of experiment failures at the Advanced Test Reactor (ATR) are analyzed to provide an overview of the methods used to detect initial signs of unintended fission product release. The data is contextualized with the operational experience, including means of identification and subsequent mitigation strategies, gained during these events. General trends as well as variations in isotopic behavior between the three failures are explored. Background on the Real Time Monitor, a High Purity Germanium detector, and other fission product monitoring systems utilized at the Advanced Test Reactor is also provided. The presented analysis was used to establish administrative action levels which are currently utilized by ATR for early detection of experiment fission product release. Early identification provides time to make programmatic decisions before approaching safety and environmental limits.

21 - SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLAN↗

Stellar s-process neutron capture cross sections on 78,80,84,86 Kr determined via activation, atom trap trace analysis and decay counting

We present a detailed account of neutron capture experiments of astrophysical relevance on 78,80,84,86 Kr (n, γ) reactions at the border between weak and main s process. The experiments were performed with quasi-Maxwellian neutrons from the Liquid-Lithium Target (LiLiT) and the mA-proton beam at 1.93 MeV (2-3 kW) of the Soreq Applied Research Accelerator Facility (SARAF). The setup yields high-intensity approximate to 40 keV quasi-Maxwellian neutrons (3-5 x10 10 n/s) closely reproducing the conditions of s-process stellar nucleosynthesis. A sample of 100 mg of atmospheric, pre-nuclear-age Kr gas contained in a Ti spherical shell was activated in the LiLiT neutron field. The abundances of long-lived Kr isotopes ( 81,85g Kr) were measured by atom counting via atom trap trace analysis (ATTA) at Argonne National Laboratory and low-level counting (LLC) at University of Bern. This work is the first measurement of a nuclear cross section using atom counting via ATTA. The activities of short-lived Kr isotopes ( 79,85m,87 Kr) were measured by gamma-decay counting with a high-purity germanium detector. Maxwellian-averaged cross sections for s-process thermal energies are extracted. By comparison to reference values, our nucleosynthesis network calculations show that the experimental cross sections have a strong impact on calculated abundances of krypton and neighboring nuclides, in some cases improving agreement between theory and observations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Effects of gas purity on backgrounds of collision reaction cell-equipped MC-ICP-MS

The advent of multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) instruments equipped with collision reaction cells (CRCs) facilitates interference removal/mitigation via online gas phase separations. This approach has proven effective for high intensity ion beams measured on Faraday collectors; however, it has been observed that introduction of gas in the CRC can result in significant background signals relative to the more sensitive ion counters. These backgrounds hinder use of these instruments for low level concentration and isotopic ratio measurements when employing a reaction gas. Here, this work directly evaluates the effect of gas purity on backgrounds of CRC-MC-ICP-MS instruments. Introducing high-purity research grade O 2 (99.999%) into the CRC produces complex background spectra with intensities >10 4 cps observed at most masses across the measured mass range (7-300 m / z ). Some features of the observed spectra (i.e., positive mass defects) can be attributed to molecular compounds comprised of significant hydrogen. Additionally, some specific molecular species can be identified (i.e., MoO x H y + ) and appear to be derived from molybdenum rods comprising the CRC. Further purifying the gas reduces the intensity of these backgrounds by several orders of magnitude, to <10 2 cps in many cases, and reduces complexity of the resulting spectra. This reduction in background appears to be in part driven by removal of impurities (i.e., H 2 O) from the gas. This work demonstrates that additional purification of reaction gases prior to introduction into the CRC significantly reduces backgrounds detected, potentially expanding the utility of CRC-MC-ICP-MS for making low level measurements using inline gas phase ion separations.

Schlieder, Tyler D. [Pacific Northwest National La↗

New approach to precisely measure γ-ray intensities for long-lived fission products, with results for the decay of 95 Zr

For many fission products, the rays emitted following decay provide an easily-detectable signature that can be used to identify their quantities and distributions in a sample. As a result, γ-ray spectroscopy is often exploited to study fission-product yields, provided sufficiently accurate information on the γ-ray intensity is available. However, in many cases, the uncertainties in the existing nuclear data are large enough that they compromise the precision achievable for modern experiments and applications. To address this need, we have developed a new experimental method that is well suited to precisely measure absolute γ-ray intensities in the β decay of long-lived fission products. The approach involves the production of a radiopure sample by implantation of a mass-separated ion beam from the CAlifornium Rare Isotope Breeder Upgrade (CARIBU) facility on a thin carbon foil. The emitted β-decay radiation is detected with a 4π gas proportional counter and a meticulously efficiency-calibrated high-purity germanium (HPGe) detector. As a first measurement to demonstrate the approach, we studied the absolute γ-ray intensities of the strongest transitions following the β decay of 95 Zr and its decay-daughter 95 Nb, and determined them to fractional precisions of better than 1–2%. In addition, with a larger sample of activity produced through neutron irradiation of an isotopically-enriched Zr foil, we performed a high-precision measurement of the relative γ-ray intensities following the decay of 95 Zr with just the HPGe detector. Here, the sample-production method at CARIBU and the coincidence detection approach demonstrated here can be applied to study fission products with half-lives longer than a day, which includes isotopes important not only for nuclear-energy and national-security applications, but also for medical-isotope research and environmental monitoring.

4π↗

Precise half-life determination of 131 Ba and 125 Xe

Barium-131 and Xenon-125 are valuable radioisotopes with numerous scientific and medical applications. Here, we produced both isotopes via proton irradiation of a cesium iodide (CsI) target at the Brookhaven Tandem Van de Graaff accelerator (BTVG). Following irradiation, we conducted systematic γ-ray spectroscopy measurements at the National Nuclear Data Center (NNDC) decay station using a calibrated High-Purity Germanium (HPGe) detector, collecting data over a 2-month period (spanning approximately 4.5 half-lives for 131 Ba). Through careful analysis of the characteristic γ-ray emissions from both isotopes, we determined the half-life of 131 Ba to be 11.55(6) days, which agrees with the previously evaluated value. For 125 Xe, we measured a half-life of 16.56(8) hours, slightly lower than the evaluated value.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Determination of neutron irradiation temperatures of SiC using electrical resistivity method

The irradiation temperature of silicon carbide (SiC) was determined post-irradiation by examination of the recovery of the electrical resistivity due to thermal annealing in a rapid heating/cooling optical furnace. High-purity, high-resistivity grade SiC is routinely used as a passive temperature monitor in neutron irradiation studies at the High Flux Isotope Reactor (HFIR), and this paper presents an alternative automated technique for determination of the irradiation temperature the SiC experienced. Neutron collisions with the atoms results in displaced lattice atoms (interstitials) that act as electron donors yielding a significant decrease in electrical resistivity. The irradiation defects become thermodynamically unstable and start to recombine, when annealed above the irradiation temperature, resulting in a recovery of the electrical resistivity. The resistivity is measured at a fixed elevated temperature above ambient, which is below the target irradiation temperature. When the resistivity is plotted as a function of annealing temperatures, a clear increase is observed due to the recovery of irradiation defects. We have demonstrated that this electrical resistivity measurement of SiC is effective to determine irradiation temperature of SiC. In conclusion, energy levels of various defects in SiC were calculated from Arrhenius plots of electrical conductivity versus inverse temperature.

36 MATERIALS SCIENCE↗

Quantitative Long-Term Monitoring of the Circulating Gases in the KATRIN Experiment Using Raman Spectroscopy

The Karlsruhe Tritium Neutrino (KATRIN) experiment aims at measuring the effective electron neutrino mass with a sensitivity of 0.2 eV/c2, i.e., improving on previous measurements by an order of magnitude. Neutrino mass data taking with KATRIN commenced in early 2019, and after only a few weeks of data recording, analysis of these data showed the success of KATRIN, improving on the known neutrino mass limit by a factor of about two. This success very much could be ascribed to the fact that most of the system components met, or even surpassed, the required specifications during long-term operation. Here, we report on the performance of the laser Raman (LARA) monitoring system which provides continuous high-precision information on the gas composition injected into the experiment’s windowless gaseous tritium source (WGTS), specifically on its isotopic purity of tritium—one of the key parameters required in the derivation of the electron neutrino mass. The concentrations cx for all six hydrogen isotopologues were monitored simultaneously, with a measurement precision for individual components of the order 10−3 or better throughout the complete KATRIN data taking campaigns to date. From these, the tritium purity, εT, is derived with precision of <10−3 and trueness of <3 × 10−3, being within and surpassing the actual requirements for KATRIN, respectively.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

FGMS-poster

Idaho National Laboratory (INL) performs post irradiation examination (PIE) of tri-structural isotropic (TRISO)-coated particle fuel to help qualify it for high temperature gas cooled reactors. TRISO fuel compacts are re-irradiated in the Neutron Radiography Reactor (NRAD) to generate the short lived fission products needed for fission product release testing. The Fuel Accident Condition Simulator (FACS) furnace and newly added Screen Neutron Irradiated Fuel for Failure (SNIFF) furnace heat the compacts in helium to temperatures of up to 2,000°C, prompting fission product release—predominantly gaseous xenon and krypton isotopes and condensable products such as cesium—from failed particles. These released isotopes are transported to a fission gas monitoring system (FGMS 1 or FGMS 3), where they accumulate in cryogenic cold traps and are quantified using high-purity germanium (HPGe) detectors. The addition of SNIFF and FGMS 3 increases throughput by enabling simultaneous testing of multiple compacts. Furthermore, automated INL developed software provides continuous, near-real time monitoring of fission product inventories and manages the liquid nitrogen cooling of the traps. These system enhancements improve the efficiency, data quality, and testing capacity of TRISO fuel performance evaluations.

07 - ISOTOPES AND RADIATION SOURCES↗

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↗

Computational Tool for Cosmic Ray Flux and Cosmogenic Activation Production Rates

Silicon charge couple devices (CCDs) are used in direct detection dark matter searches. Silicon can be obtained with very high purity and negligible amounts of radioactive contaminants. However, silicon exposed to cosmic rays can be activated, leading to the buildup of radioactive isotopes such as tritium. The decay of tritium can produce signals that cannot be distinguished from the expected signals of dark matter interactions and tritium produced by cosmic rays is expected as one of the leading sources of background for next-generation experiments. The cosmic ray flux depends on variables such as geomagnetic latitude and longitude, atmospheric depth/altitude, solar activity, and surrounding environment for example. The goal of this work is to create a tool that will evaluate the total cosmic ray exposure and related tritium production rate for any given exposure history of a silicon detector. EXcel-based Program for calculation Atmospheric Cosmic-ray Spectrum (EXPACS) was used to obtain the cosmic ray fluxes. We have worked on creating a 3-dimensional gird that spans latitude, longitude, and altitude, and can be used to interpolate the cosmic ray flux at any given location. This computation tool additionally has use for work requiring knowledge of the cosmic ray flux at multiple locations.

79 ASTRONOMY AND ASTROPHYSICS↗

Fabrication and Testing of Micro Flux Monitors in the High Flux Isotope Reactor

Neutron dosimetry is a critical technique to measure the neutron flux, fluence, and energy spectrum of nuclear reactors and can be used to indicate fuel reloading, high-power operations, or changes in cycle length. This work presents results of a novel device named the micro flux monitor, which is a miniaturized neutron dosimeter made from small quantities (100s of nanograms) of Ti, Al, Ni, and Au metals deposited on Si and high-purity fused silica substrates using standard semiconductor fabrication techniques. Approximately 1,250 of these devices were produced, and 40 were irradiated in the pneumatic tube facility of the Neutron Activation Analysis Laboratory at the High Flux Isotope Reactor. Testing demonstrated that dosimeter metals can be deposited predictably and repeatedly in multiple geometries, including as quick response (QR) codes. Neutron flux measurements with these devices were within 3% of measurements made using standard flux monitors, demonstrating the efficacy of these devices. Devices were also tested at 500°C under a N2 atmosphere and showed minimal degradation, suggesting they could be deployed for neutron dosimetry measurements in high-temperature advanced reactors.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Qualification of Commercially Available Silicon Carbide for Passive Thermometry in Reactor Experiments – FY23 Status Report

Silicon carbide (SiC) is often used as a passive temperature indicator for uninstrumented in-core nuclear experiments. For the past several decades, Oak Ridge National Laboratory has relied primarily on SiC thermometry manufactured by Dow Chemical Company, formerly Rohm and Haas because of the material’s high density and reduced grain boundary elements. Although Dow SiC has performed well in this application, this material is no longer commercially available, and a new supplier is needed for future experiments. To determine a suitable replacement, a study was initiated on five types of SiC from four commercial vendors. Several critical properties, including density, electrical resistivity, chemical purity, grain structure, crystal structure, and strength were measured in samples from each material. Additionally, thermometry specimens were manufactured for irradiation in the High Flux Isotope Reactor at nominal temperatures of 300°C, 600°C, and 900°C, which will be measured using continuous dilatometry at a later date. This report provides an update of commercially available SiC material characterization and the irradiation capsule design.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Sulfur-functionalized solid-phase materials for the selective separation of arsenic and selenium

Radioactive arsenic (As) isotopes are of growing interest for applications in nuclear medicine, national security, and environmental research. Recent efforts at the Facility for Rare Isotope Beams (FRIB) have focused on aqueous harvesting of selenium-72,73 ( 72,73 Se) and their daughter isotopes, arsenic-72,73 ( 72,73 As), which are particularly valuable for medical applications and nuclear data studies, respectively. Both conventional isotope production and harvesting methods require chemical separations to purify radioactive As from parent and co-produced Se radioisotopes. While several solid-phase separation methods for As and Se exist, many depend on complex oxidation state control or highly acidic conditions. This study presents results for sulfur-based solid-phase materials selected to enable uptake at lower acidity and eliminate the need for intricate redox chemistry. Specifically, the performance of three covalently bound sulfur-based ligands were evaluated: (1) thiophenol-polystyrene, (2) propanethiol-silica, and (3) thiourea-silica. Uptake characteristics—including distribution coefficients (Dw), kinetics, and column separation behavior—were assessed using 75 Se and 73 As in hydrochloric (HCl) acid and nitric (HNO 3 ) solutions. The resins demonstrated high-yield (>95%) and high-purity As recovery across a range of HCl concentrations. Comparable results in HNO 3 were achieved when combined with anion exchange chromatography. Furthermore, the potential application of these materials for medical isotope generators was also investigated through ligand stability and repeated elution studies. Overall, sulfur leaching from the resins was negligible at the concentrations relevant for these separations but increased with higher acid concentrations.

Arsenic↗

Hydride Bed Helium-3 Recovery and Partial Regeneration

Savannah River Tritium Enterprise has used LaNi 4.25 Al 0.75 (LANA75) hydride beds to store hydrogen isotopes for over two decades. A benefit of using LANA75 is that the 3He generated from tritium decay is retained in the hydride material, allowing the hydride beds to deliver high-purity product gas. A disadvantage is that the 3He accumulates in the LANA75 material over time, which forms a heel that cannot be removed under normal operating conditions. The heel traps hydrogen in the bed, slowly reducing the operational capacity of the bed as the heel grows. Eventually, the 3 He begins to release from the material, preventing the delivery of high-purity product. The hydride beds are replaced when (1) operational capacity is reduced such that it is impactive to routine operations, and/or (2) product purity is not maintained due to 3 He release.Several beds were operated beyond their design life. One of these beds was selected to undergo heating beyond its normal operating temperature to evaluate the possibility of removing a portion of the hydrogen and helium heel to improve bed function until a replacement could take place. This bake-out removed a portion of the hydrogen and helium heel, and preliminary data indicate that bake-outs may partially regenerate the beds. The bed’s performance will continue to be monitored, and additional bake-outs will likely be performed. Performing bake-outs results in increasing the recovery of 3 He, more efficient end-of-life activities (such as isotopic exchange), and extension of the useful service life of the bed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Maximum Likelihood Spectrum Decomposition for Isotope Identification and Quantification

A spectral decomposition method has been implemented to identify and quantify isotopic source terms in high-resolution gamma-ray spectroscopy in static geometry and shielding scenarios. Monte Carlo simulations were used to build the response matrix of a shielded high-purity germanium detector monitoring an effluent stream with a Marinelli configuration. The decomposition technique was applied to a series of calibration spectra taken with the detector using a multi-nuclide standard. These results are compared with decay-corrected values from the calibration certificate. For most nuclei in the standard ( 241 Am, 109 Cd, 137 Cs, and 60 Co), the deviations from the certificate values were generally no more than 6% with a few outliers as high as 10%. Furthermore, for 57 Co, the radionuclide with the lowest activity, the deviations from the standard reached as high as 25%, driven by the meager statistics in the calibration spectra. In addition, a complete treatment of error propagation for the technique is presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗