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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Krypton-85 chronometry of spent nuclear fuel

We describe the use of the radionuclide 85 Kr, which is produced by nuclear fission and has a half-life of 10.76 years, to determine the age of spent nuclear fuel. The method is based on mass-spectrometric measurement of the relative abundance of fissiogenic Kr isotopes extracted from a fuel sample, and we show that it can be applied to micron-scale particles of spent fuel that are analogous to particles that have been released into the environment from various nuclear facilities in the past. 85 Kr chronometry is potentially valuable for identifying and attributing nuclear materials, grouping samples into collections of common origin that can be used to reconstruct the origin and irradiation history of the material, and verifying declared nuclear activities in the context of international monitoring programs.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

First experimental determination of the ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar reaction cross section and ³⁹Ar production in Earth’s atmosphere

The cosmogenic ³⁹Ar(t1∕2 = 268 years) isotope of argon is used for geophysical dating and tracing of underground and ocean water, as well as ice owing to its appropriate half-life and chemical inertness as a noble gas; ³⁹Ar serves also in nuclear weapon test monitoring. We measured for the first time the total cross section of the main ³⁹Ar cosmogenic production reaction in the atmosphere, namely ⁴⁰Ar(𝑛, 2𝑛)39 Ar, using 14.8 ± 0.3 MeV neutrons. The neutrons, produced by a deuterium-tritium generator, impinged on a stainless steel sphere filled with Ar gas highly enriched in the ⁴⁰Ar isotope and were monitored by a stack of fast-neutron activation foils. The reaction yield was measured by atom counting of long-lived ³⁹Ar with noble gas accelerator mass spectrometry and, independently, by decay counting relative to atmospheric argon (³⁹Ar/Ar= 8.12 × 10−16 ). A total ⁴⁰Ar(𝑛, 2𝑛)39 Ar cross section of 610 ± 100 mb was determined at 14.8 ± 0.3 MeV incident neutron energy. This result serves as a benchmark for recent theoretical calculations and evaluations, found to reproduce well the experimental total cross section. We use these energy-dependent theoretical cross sections together with experimental spectra of cosmogenic neutrons at different altitudes to calculate the global average rate of neutron-induced ³⁹Ar atmospheric production, resulting in 770 ± 240 39 Ar atoms/cm²/day. The secular equilibrium between the ³⁹Ar calculated production rate and radioactive decay rate leads to a partial isotopic abundance ³⁹Ar/Ar = (5.9 ± 1.8) × 10−16 , showing that ≈73% of atmospheric ³⁹Ar is produced by cosmogenic neutrons, the remaining part believed to be induced by muons and high-energy 𝛾 rays. The ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar cross section at 14 MeV is also a key parameter for quantifying the anthropogenic contribution to atmospheric 39 Ar produced during the thermonuclear tests of the 1960s. We estimate that anthropogenic ³⁹Ar accounts for roughly 20% of the present atmospheric inventory.

39 Ar atmospheric production↗
DOE OSTI2024

Development of CD46 targeted alpha theranostics in prostate cancer using 134 Ce/ 225 Ac-Macropa-PEG 4 -YS5

Rationale: 225 Ac, a long-lived α-emitter with a half-life of 9.92 days, has garnered significant attention as a therapeutic radionuclide when coupled with monoclonal antibodies and other targeting vectors. Nevertheless, its clinical utility has been hampered by potential off-target toxicity, a lack of optimized chelators for 225 Ac, and limitations in radiolabeling methods. In a prior study evaluating the effectiveness of CD46-targeted radioimmunotherapy, we found great therapeutic efficacy but also significant toxicity at higher doses. To address these challenges, we have developed a radioimmunoconjugate called 225 Ac-Macropa-PEG 4 -YS5, incorporating a stable PEGylated linker to maximize tumoral uptake and increase tumor-to-background ratios. Our research demonstrates that this conjugate exhibits greater anti-tumor efficacy while minimizing toxicity in prostate cancer 22Rv1 tumors. Methods: We synthesized Macropa.NCS and Macropa-PEG 4/8 -TFP esters and prepared Macropa-PEG 0/4/8 -YS5 (with nearly ~1:1 ratio of macropa chelator to antibody YS5) as well as DOTA-YS5 conjugates. These conjugates were then radiolabeled with 225 Ac in a 2 M NH 4 OAc solution at 30 °C, followed by purification using YM30K centrifugal purification. Subsequently, we conducted biodistribution studies and evaluated antitumor activity in nude mice (nu/nu) bearing prostate 22Rv1 xenografts in both single-dose and fractionated dosing studies. Micro-PET imaging studies were performed with 134 Ce-Macropa-PEG 0/4/8 -YS5 in 22Rv1 xenografts for 7 days. Toxicity studies were also performed in healthy athymic nude mice. Results: As expected, we achieved a >95% radiochemical yield when labeling Macropa-PEG 0/4/8 -YS5 with 225 Ac, regardless of the chelator ratios (ranging from 1 to 7.76 per YS5 antibody). The isolated yield exceeded 60% after purification. Such high conversions were not observed with the DOTA-YS5 conjugate, even at a higher ratio of 8.5 chelators per antibody (RCY of 83%, an isolated yield of 40%). Biodistribution analysis at 7 days post-injection revealed higher tumor uptake for the 225 Ac-Macropa-PEG 4 -YS5 (82.82 ± 38.27 %ID/g) compared to other conjugates, namely 225 Ac-Macropa-PEG 0/8 -YS5 (38.2 ± 14.4/36.39 ± 12.4 %ID/g) and 225 Ac-DOTA-YS5 (29.35 ± 7.76 %ID/g). The PET Imaging of 134 Ce-Macropa-PEG 0/4/8 -YS5 conjugates resulted in a high tumor uptake, and tumor to background ratios. In terms of antitumor activity, 225 Ac-Macropa-PEG 4 -YS5 exhibited a substantial response, leading to prolonged survival compared to 225 Ac-DOTA-YS5, particularly when administered at 4.625 kBq doses, in single or fractionated dose regimens. Chronic toxicity studies observed mild to moderate renal toxicity at 4.625 and 9.25 kBq doses. Conclusions: Our study highlights the promise of 225 Ac-Macropa-PEG 4 -YS5 for targeted alpha particle therapy. The 225 Ac-Macropa-PEG 4 -YS5 conjugate demonstrates improved biodistribution, reduced off-target binding, and enhanced therapeutic efficacy, particularly at lower doses, compared to 225 Ac-DOTA-YS5. Incorporating theranostic 134 Ce PET imaging further enhances the versatility of macropa-PEG conjugates, offering a more effective and safer approach to cancer treatment. Overall, this methodology has a high potential for broader clinical applications.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2020

Mitigation of Backgrounds from Cosmogenic $^{137}$Xe in Xenon Gas Experiments using $^{3}$He Neutron Capture

\Xe{136} is used as the target medium for many experiments searching for \bbnonu. Despite underground operation, cosmic muons that reach the laboratory can produce spallation neutrons causing activation of detector materials. A potential background that is difficult to veto using muon tagging comes in the form of \Xe{137} created by the capture of neutrons on \Xe{136}. This isotope decays via beta decay with a half-life of 3.8 minutes and a \Qb\ of $\sim$4.16 MeV. This work proposes and explores the concept of adding a small percentage of \He{3} to xenon as a means to capture thermal neutrons and reduce the number of activations in the detector volume. When using this technique we find the contamination from \Xe{137} activation can be reduced to negligible levels in tonne and multi-tonne scale high pressure gas xenon neutrinoless double beta decay experiments running at any depth in an underground laboratory.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

High Temperature Stability of Aqueous Foams for Potential Application in Enhanced Geothermal System (EGS)

Enhanced Geothermal Systems (EGS) are typically constructed by injecting high-pressure water into the deep hot dry rocks (HDR) under carefully controlled conditions to create new or re-open existing fractures, which usually utilizes an immense quantity of water. Alternatively, aqueous foam-based fracturing fluids may offer potential advantages over conventional water-based fracturing fluid, including reduced consumption of water and environmental impact. Although foam-based fracturing has shown promising results in oil and gas industries, its applicability to EGS is unknown. Foams are complex mixtures of liquids with gaseous phases that are thermodynamically unstable. Their stability will decrease over time due to liquid drainage, bubble coarsening, and coalescence. Therefore, it is essential to stabilize foam fluids at high temperatures for EGS related applications such as fracking of HDRs.This paper is focused on investigating high-temperature stability of N2-in-water or N2 foams containing different surfactants and stabilizing agents. Foam stability was characterized by the half-life, which is defined as the time a foam decreases to 50% of its original height due to drainage. Surfactants with various concentrations dissolved in deionized water were investigated, including alfa olefin sulfonate (AOS), sodium dodecyl sulfonate (SDS), TergitolTM (NP – 40), and cetyltrimethylammonium chloride (CTAC). Also, the effects of other stabilizing agents, including guar gum, bentonite clay, crosslinker, graphene oxide (GO) dispersion on foam stability were tested. Initial results showed that foam stability decreased dramatically as temperature increased. On the other hand, foams became relatively more stable as pressure increased. Certain stabilizing agents, such as guar gum and crosslinker, can enhance foam stability at a wide range of temperatures. Our results indicate that it may be possible to obtain stable foams at high-temperature, high-pressure conditions with appropriate stabilizing agents.

Thakore, Virensinh↗
DOE OSTI2021

Integral Measurement of the 237 Np($n$, γ) 238 Np Cross Section with Fast Neutrons

Accurate knowledge of the 237 Np($n$; γ) 238 Np cross section at fast neutron energies is important for applied nuclear science. The presently available experimental data has large disagreements in the fast neutron region. A measurement of the 237 Np($n$; γ) 238 Np cross section was performed using a well characterized fast neutron source and the results was compared with previous measurements and current nuclear data evaluations. This will provide an integral measurement that can be used as a benchmark for current evaluations. Multiple samples of 237 Np were irradiated in the Godiva-IV critical assembly. Following the irradiation, the samples placed in a γ-ray counting setup and the γ-rays emitted from the decay of 238 Np were measured over a time period of approximately 7 days. Multiple γ-ray decay branches of 238 Np were observed. The observed activity of 238 Np was used to calculate the amount of 238 Np produced during the irradiation via the 237 Np($n$; γ) 238 Np and an integral cross section of 359(10) mb was measured. The 238 Np half-life has been measured with a result of 50.34(7) hours. An integral measurement of the 237 Np($n$; γ) 238 Np cross section has been measured. This result has been compared to the calculated integral cross section using the ENDF/BVIII.0 and JENDL-4.0 evaluated cross sections and found to be in good agreement with ENDF/BVIII.0 value of 367 mb. The JENDL-4.0 evaluation yields a value of 312 mb, which is significantly lower than the measured cross section.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Latest results from the CUORE experiment

The CUORE experiment is searching for the neutrinoless double β decay of the 130Te using cryogenic calorimeters. The CUORE detector consists of 988 TeO2 crystals packed in 19 towers and placed in a cryogenic facility with a base temperature of 10 mK. Crystals are enriched in the isotope 130Te which is the candidate for the neutrinoless double β decay. It is taking data since 2017 at the Laboratori Nazionali del Gran Sasso in Italy. Such a long operation of a bolometric experiment in stable condition has no precedent: by reaching 1 tonne-year of exposure CUORE set a fundamental milestone for any future experiment using this technology. The CUORE collaboration investigated the neutrinoless double β decay of 130Te exploiting the updated 1 tonne-year of statistics, setting a limit of 2.2 × 1025 yr at the 90% of credibility interval on the half-life, with a median sensitivity of 2.8 × 1025 yr.

Adams, DQ↗
DOE OSTI2023

High temperature and high beam current compatible targets and methods thereof for generating noble gas/radiohalogen generators for medical isotopes

A method of providing alpha particle emitters and materials suitable for use in generating the alpha particles for medical treatment is disclosed. Metal oxide targets, preferentially Bi 2 O 3 pellets and Bi 2 O 3 coatings on metallic or metal oxide substrates are formed. The targets placed in a heated vacuum chamber subjecting to irradiation using a 6 Li beam at an elevated temperature below the melting point of the target generate a radioactive gas, such as 211 Rn, the radioactive gas is carried by an inert gas which is delivered a carrier for, such as a carbon column or oil for delivery to a treatment facility. The radioactive gas such as 211 Rn generates 211 At, which has a useable half-life of at least about 14 hours, in turn releases alpha particles which are effective for use in medical procedures.

Sampathkumaran, Uma↗
DOE OSTI2020

The Nature and State of Groundwater Contamination at the Nevada National Security Site: What Have We Learned from Decades of Groundwater Analysis? - 20337

The regulatory framework for remediating radionuclide contamination from underground nuclear testing at the Nevada National Security Site (NNSS) is based on a combination of characterization and modeling studies, monitoring, and institutional controls [1]. Currently, tritium is the largest contributor (∼90%) to the estimated 44.6 million-curie radionuclide inventory resulting from underground testing [2]. Because of its short half-life (12.32 years), its relative contribution reduces below 10% of the total radiologic inventory over the next 120 years as a result of radioactive decay. Although tritium levels are observed well above the Safe Drinking Water Act (SDWA) maximum contaminant levels (MCLs) in groundwater, other radionuclides are well below their MCLs except within the nuclear test near-field (nuclear test cavity and chimney) environment. In fact, most device-derived radionuclides are below their MCL in groundwater even in samples collected from this near-field environment. The distribution of radionuclides following the nuclear detonation greatly influences the availability of potential contaminants for groundwater transport. Tritium is initially distributed in the gas phase, later as tritiated water in steam, and finally as liquid water, and is available to groundwater transport away from the near-field environment. Other radionuclides that are mobile in groundwater are {sup 14}C, {sup 36}Cl, {sup 99}Tc, and {sup 129}I though their radiologic inventory is small when compared to tritium. Many radionuclides (e.g. U, Pu, Am) are incorporated to a significant extent into the melt glass at the bottom of the cavity and are accessible to groundwater primarily through the slow process of glass dissolution. These radionuclides are also adsorbed to the surfaces of the crushed rock within the cavity and chimney which limits their migration in groundwater. Although colloid facilitated transport of radionuclides at the NNSS has been observed [3], radionuclide concentrations decrease with time and migration distances due to desorption and colloid filtration processes. Current studies indicate that radionuclides associated with colloids are unlikely to migrate downgradient from NNSS underground nuclear tests at concentrations above the SDWA MCL [4][5]. The results of over 50 years of sampling, along with an understanding of these post detonation processes, indicate that tritium is the only contaminant of concern downgradient of testing and that even tritium will not exceed its MCL in groundwater after ∼120 years. Although other longer-lived radionuclides may continue to be released slowly from the near-field environment they will likely never reach levels exceeding their MCLs in groundwater downgradient of the NNSS. Groundwater monitoring will continue to verify these observations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Novel Photonuclear Methods to Produce an Argon-37 Standard

The mission of this research is to explore novel photonuclear-based pathways into the production of 37Ar. Above-background detection levels of 37Ar uniquely indicates the occurrence of an underground nuclear explosion, produced from fission neutrons interacting in the surrounding environment through the 40Ca(n,a)37Ar reaction. The half-life of 35 days allows on-site inspectors (OSI) adequate time following the nuclear event to detect 37Ar and verify compliance or defiance of non-proliferation treaties such as the Comprehensive Nuclear-Test-Ban Treaty (CTBT). An 37Ar standard would give OSI the ability to calibrate their detectors and measure detector efficiency allowing for the quantification of detected activity, give OSI authentic samples to test detectors in field exercises, and improve models predicting diffusion pathways of 37Ar through the underground environment.

43 PARTICLE ACCELERATORS↗
DOE OSTI2024

SARS-CoV-2 variant nanobodies and constructs comprising such nanobodies

A large and highly diverse nanobody library was constructed and screened against multiple variants of SARS-COV-2 to find nanobodies with high sensitivity and specificity for the variants. Four rounds of positive selection against a panel of six diverse SARS-COV-2 variant RBDs was performed with our high-diversity. At least 59 of these nanobodies were found to work well against Alpha, Beta, Gamma, Delta, Kappa, Lambda and Mu with some overlap efficacy against other variants. These nanobodies have efficacy as stand-alone nanobodies and as a construct comprising nanobodies linked to the human IgG1 constant fragment (Fc) (nanobody-hFc constructions or nb-hFcs) to make enhanced humanized sdAbs with all the attributes of nanobodies with improved half-life and optimized effector functions. Several promising nanobodies that neutralize the original SARS-COV-2 and several of its variants have been identified, including Delta, with high efficacy. In particular, a subset of these nanobodies bind to the Omicron RBD.

Harmon, Brooke Nicole↗
DOE OSTI2025

Tritium Breeder Composites for Fusion Applications

Due to the short half-life of tritium, all fusion reactors planned for long-term operation using a deuterium-tritium fuel cycle must produce sufficient tritium from reactions outside the core to maintain reactor operation. Typically, the core is surrounded by a tritium breeder blanket filled with lithium-containing materials which react under a neutron flux to form tritium that can then be collected. Here, reactor designers are forced to choose between using chemically reactive liquid breeders (e.g., Pb-Li, FLiBe, Li) or solid breeders, which often have lower lithium concentrations and questionable mechanical integrity under irradiation (e.g., Li4SiO4, Li2TiO3). To expand this pool of options, this work has sought to produce composite tritium breeder materials using lithium-containing ceramics and metal reinforcements. The resultant composite tritium breeders simultaneously feature higher lithium densities and improved mechanical integrity, including tensile strength and toughness, compared to other tritium breeders previously reported in literature.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Multiscale, mechanistic calculation of the effective silver diffusion coefficient in polycrystalline silicon carbide: application to silver release in AGR-1 TRISO particles

The silicon carbide (SiC) layer in tristructural isotropic (TRISO) fuel particles serves as a barrier to prevent the escape of fission from the fuel kernel. The release of silver (Ag) is a concern due to the long half-life of the 110mAg isotope. In this study, the effective diffusion coefficient of the fission product Ag through the grain boundary (GB) network is calculated using a combination of atomistic and phase-field methods. Atomistic calculations of Ag diffusivity in SiC bulk and GBs are leveraged to develop a mesoscale effective Ag diffusion coefficient (Deff) in SiC. Since GBs serve as pathways for Ag diffusion, Deff is defined as a function of temperature, microstructure variables, and fluence. Deff is implemented in the fuel performance code Bison to predict Ag release from AGR-1 TRISO fuel particles. We hereby quantify the impact of SiC grain size and irradiation on Ag release and improve Bison's predictions.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Understanding the effect of irradiation and silicon carbide microstructure on silver diffusion in TRISO particles

The silicon carbide (SiC) layer in tristructural isotropic (TRISO) fuel particles serves as a barrier to prevent the escape of fission from the fuel kernel. The release of silver (Ag) is a concern due to the long half-life of the 110mAg isotope. In this study, a combination of atomistic and phase-field methods focuses on quantifying the effect of irradiation and SiC microstructure on Ag diffusion. Atomistic calculations provide the Ag diffusivity in SiC bulk and GBs, also providing an estimate of the effect of irradiation defects on Ag diffusivity in bulk SiC. These lower length scale efforts are leveraged to develop a mesoscale effective Ag diffusion coefficient (Deff) in SiC. Deff is defined as a function of temperature, microstructure variables, and fluence. Deff is implemented in the fuel performance code Bison to predict Ag release from AGR-1 and AGR-2 TRISO fuel particles. We hereby quantify the impact of SiC grain size and irradiation on Ag release and improve Bison's predictions.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Absolute decay counting of 146 Sm with 4π cryogenic microcalorimetry

We present a methodology for absolute activity counting of long-lived isotopes based on cryogenic Decay Energy Spectroscopy. A 146 Sm source was produced at the TRIUMF Laboratory and then processed and purified at Lawrence Livermore National Laboratory, yielding a pure sample. The source was embedded within a 4π thermal absorber coupled to a magnetic microcalorimeter achieving nearly 100% counting efficiency. Experimental uncertainties were studied and modeled, including thermal coupling of the source to the absorber, pulse pile-up, trigger, and event selection efficiencies. Here, the absolute activity of the pure 146 Sm source was measured to better than 1% uncertainty.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

FITEVT: A FORTRAN program for arrival-time analysis of nuclear-decay events

FITEVT is a FORTRAN program designed to analyze recorded arrival times of nuclear-decay events affected by dead-time. Here, the primary goal of the program is precise and accurate determination of half-lives. Its method involves imposition of a known sufficiently long extending dead-time to the recorded event sequence, so that the original dead-time effects are completely obliterated and the remaining live-times of the survived events are known exactly. Upon completion of the analysis, the arrival-time spectrum and the live-time spectrum are predicted and compared to those constructed from the survived events.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Branching ratio and γ -ray emission probabilities in the decay of the J π = 13 / 2 + isomer in 197Hg

Gamma rays following the decay of the 197 g Hg and 197 m Hg radionuclides were measured using chemically-purified sources and a planar HPGe detector. In the case of 197 m Hg, precise values of 94.68 (9)% and 5.32 (9)% were confirmed for the IT and EC branches, respectively, the latter discovered to differ significantly from previously published data. The half-lives of 197 g Hg and 197 m Hg were also measured as 64.81 (24) h and 23.82 (4) h.

197𝑔Hg↗