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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Investigation of the ground-state spin inversion in the neutron-rich Cl 47 , 49 isotopes

A first γ -ray study of Cl 47 , 49 spectroscopy was performed at the Radioactive Isotope Beam Factory with Ar 50 projectiles at 217 MeV/nucleon, impinging on the liquid hydrogen target of the MINOS device. Prompt deexcitation γ rays were measured with the NaI(Tl) array DALI2 + . Through the one-proton knockout reaction Ar 50 ( p , 2 p ) , a spin assignment could be determined for the low-lying states of Cl 49 from the momentum distribution obtained with the SAMURAI spectrometer. A spin-parity J π = 3 / 2 + is deduced for the ground state of Cl 49 , similar to the recently studied N = 32 isotope K 51 . The evolution of the energy difference E ( 1 / 2 1 + ) - E ( 3 / 2 1 + ) is compared to state-of-the-art theoretical predictions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

The Status and Ambitions of the US Heavy Element Program

The aim of this whitepaper is to highlight the current capabilities and priorities of the US Heavy Element community and to provide the framework for a coordinated advancement of nuclear science from these studies. This is an organized effort to reflect on what has been achieved in the field given the recommendations and initiatives of the 2015 NSAC Long Range Plan, and on what can be realized in the next decade given current and possibly expanded investments. Current investments have positioned the US community to be among the world leaders in studies of the nuclear and chemical properties of the heaviest elements. These include studies of reaction mechanisms, moving us ever closer to the “island of stability”, in spectroscopy, allowing us to better understand nuclear structure at these extreme proton numbers, in chemical behavior, looking to determine how these elements should be placed on the Periodic Table, in performing the first measurements where isotopes are directly identified by their mass numbers, and in laying the foundation for a potential US-led new element discovery experiment. At present, the highest priority of the US Heavy Element community is to capitalize on the current investments by supporting the operations of US facilities at optimal values. These facilities include the Argonne Tandem Linac Accelerator System at Argonne National Laboratory and other Department of Energy facilities such as the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory, which has a dedicated superheavy element program, as well as university laboratories, including Texas A&M University. The High Flux Isotope Reactor at Oak Ridge National Laboratory is crucial to providing the radioactive isotopes required for heavy element science targets. This facility should be supported to provide the actinide materials that are essential for US-based science. Production of stable, rare isotopes for beam material, including 48 Ca, 50 Ti, 54 Cr and 58 Fe, at the Stable Isotope Production and Research Center is critical to continued research in heavy element science and should be a priority. The continued development of targets for heavy element science and retaining US-based expertise is critical for the heavy element community. This is an area that is currently under pressure. For example, the target laboratory at Argonne National Laboratory serves a broad community and is currently under threat due to loss of critical personnel. The skills needed to make targets for nuclear science and develop new targetry methods need to be supported long term at Argonne, Oak Ridge and Lawrence Livermore National Laboratories as well as maintaining the programs at Oregon State University and San José State University as vital pipelines for training students. Advances in theory are the foundation to understand how nuclei behave and to predict those behaviors in new circumstances. Progress in these studies will necessitate continued and new investment and access to high-performance computing. The future health of the heavy element field is dependent on the continuous support of talented early-career professionals at all levels. It is critical that opportunities continue to be created for the next generation to become established in heavy element research so that we can ensure the field is attracting and retaining the best minds for continued success. It is also clear that to ensure diversity of ideas, perspectives and techniques, we need to recruit diverse personnel that are trained at the best facilities. The heavy element community is in support of continued investment to programs with initiatives in diversity, equity, and inclusion. Looking to the next decade of research, support needs to maintain and grow US leadership in heavy element science. Specifically, new investments in state-of-the-art instrumentation will be essential to scientific development of the field and in expanding scientific knowledge. Advances in the next generation of electron cyclotron resonance ion sources, multi-reflection time-of-flight devices, laser spectroscopy, trapping methods and next generation alpha and gamma spectroscopy systems should be prioritized.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

How Rains and Floods Become Groundwater: Understanding Recharge Pathways With Stable and Cosmogenic Isotopes

Anthropogenic climate change leads to increased precipitation intensity and exacerbated droughts in California, challenging the reliability and drought resiliency of water supply. Storing floodwater underground via managed aquifer recharge can mitigate these effects through direct infiltration or streambed infiltration. Seasonally dry streams (arroyos) already play an important part in managing groundwater recharge to the Livermore basin (CA). Understanding how, when and where stormwater and arroyo water infiltrate is critical to effectively utilise this strategy. To track water from recent storms (water year 2022–2023, WY23) into the Livermore Valley Groundwater Basin, we analysed stable water isotopes (δ 18 O and δ 2 H) in combination with naturally occurring radioactive isotopic tracers, sulphur-35 ( 35 S, t ½ = 87 days) and tritium ( 3 H, t ½ = 12.3 years). By comparing measurements of δ 18 O, 35 S and 3 H in arroyos to precipitation and groundwater, we classified the relative age and identified source of recharge to 16 wells near two arroyos. Two wells contained water with recent recharge (from WY23) from local precipitation. One well had recent recharge from variable (precipitation and imported water) sources. One well contained imported water recharge. Three wells contained water from mixed recent and older (pre-WY23) waters, from local precipitation sources. Two wells contained recent recharge from local mine settling ponds. Seven wells had older recharge from local precipitation sources. This combination of isotopes allows us to delineate where local and imported water recharges in this highly managed basin and identify locations where managed aquifer recharge is contributing to rapid groundwater infiltration. Our combined interpretation of isotopic water ages and sources in the context of land use shows that local infiltration of precipitation in open spaces is an important recharge mechanism, in addition to the managed arroyo recharge. Finally, a broader familiarity with 35 S will enable more extensive research on the infiltration of urban floodwaters.

58 GEOSCIENCES↗
DOE OSTI2025

Comparison of microprecipitation methods for polonium source preparation for alpha spectrometry

Detection of radioactive isotopes of polonium is important for understanding natural processes, management and assessment of radioactive waste, and nuclear forensics applications. Further, the most common methods for preparation of polonium samples for alpha spectrometry are electrodeposition and spontaneous deposition which are time consuming. Here, we compare three approaches utilizing rapid microprecipitation from bismuth phosphate, copper sulfide, or tellurium alongside traditional spontaneous deposition methods. From these experiments, results show that copper sulfide microprecipitation recoveries are similar to spontaneous deposition on silver and less time consuming with an approximate five-fold decrease in preparation time, including in the presence of complex matrices like seawater.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

The ENDF/B-VIII.0 Compendium Volume IV: Radioactive Decay Rank-Order Analyses

Version 8 of the Evaluated Nuclear Data File (ENDF/B-VIII.0) contains a wealth of nuclear data representing the most recent collection of evaluated neutron cross section measurements, isotopic radioactive decay, and much more. This Compendium has been prepared as a easily-navigable reference of the contents of the ENDF/B-VIII.0 library, while making no statement regarding the accuracy of those contents. The Compendium is split into four volumes. In Volume IV, radioactive decay properties are presented in tabular form, sorted by isotope, energy, element-then- energy, and probability of emission.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2021

Neutron Irradiation Induced Changes in Isotopic Abundance of 6Li and 3D Nanoscale Distribution of Tritium in LiAlO2 Pellets Analyzed by Atom Probe Tomography

Tritium, a radioactive isotope of hydrogen is produced by neutron irradiation of 6Li enriched LiAlO2 pellets in Tritium producing burnable absorber rods (TPBARs). Three-dimensional nanoscale mapping of Tritium in irradiated pellets is critical to understand its spatial variation and its association with various microstructural features in the pellets. Spatially resolved analysis of 6Li isotopic enrichment in such ceramic pellets before and after irradiation can provide insights to heterogeneities in Li isotopic distribution. However, Li being a light isotope, its spatially resolved compositional or isotopic analysis is a challenging task to most analytical methods. Here we used atom probe tomography, to evaluate the Li isotopic enrichment in both the LiAlO¬2 matrix and the Li deficient secondary phase LiAl5O8 before irradiation. These results were then compared with 6Li isotopic ratio measured by APT analysis of neutron irradiated pellets to clearly demonstrate the unique capability of APT to quantitatively analyze the isotopic enrichment of 6Li as well as for other light elements present in these materials. Evidence for heterogenous nanoscale distribution of 3H and O3H within irradiated pellet microstructure is also provided, which is attributed to 3H trapping in irradiation induced vacancy clusters or voids within the LiAlO2 matrix. The characterization results given here, now prove the feasibility for using APT for analyzing nanoscale spatially resolved isotopic enrichment of Li as well as other light elements such as Tritium in TPBARs. This work also paves way to adopt APT for analyzing light elements such as Li and tritium in materials used for nuclear fusion reactor applications, geochemistry, astrophysics as well as for energy storage applications.

Devaraj, Arun↗
DOE OSTI2025

The FRIB Decay Station: New Horizons with Rare Isotopes

In May 2022, the Facility for Rare Isotope Beams (FRIB), located on the campus of Michigan State University (MSU), began delivering exotic isotopes to an international community of scientists. New discoveries are now being reported from radioactive decay of neutron-rich nuclei near N = 20 and N = 28.FRIB is expected to produce roughly 80% of the unstable or radioactive isotopes predicted to exist up to uranium (Z = 92). The new user facility is supported by the U.S. Department of Energy, and it is operated by MSU. A high-power superconducting linear accelerator, shaped like a paper-clip, drives the production of these rare isotopes by colliding stable nuclei moving at half the speed of light with a rotating, water-cooled graphite tar-get. These collisions cause the primary stable beam to fragment into a wide variety of unstable nuclei, which can be subsequently filtered through a multistage magnetic separator, the Advanced Rare Isotope Separator, and transported to one of several experimental stations. The FRIB Decay Station initiator (FDSi) (see Figure 1) was developed to enable comprehensive radio-active decay studies of the exotic nuclei produced by FRIB and it was used in the first two experiments in 2022. Further, the FDSi is a highly reconfigurable multidetector system with two focal planes (FP1 for discrete spectroscopy and FP2 for total absorption spectroscopy) that can be optimized for the specific science goals of each experiment. It is designed, built, and operated by a community of users with the sup-port of U.S. funding agencies, including the Department of Energy and National Science Foundation.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2021

Tritiated Sulfur Hexafluoride Disposition Strategies

Tritium (T 2 ) is a radioactive isotope of hydrogen that is produced in nuclear fission reactions and is often used in nuclear fusion reactions and accelerator-based applications for medical isotope production. As a hydrogen isotope, tritium can readily bind to hydroxyl radicals (OH), forming tritiated water (HTO or T 2 0), and to carbon atoms. Tritium decays to helium-3 ( 3 He) via beta-decay with max decay energy of 18.6 keV. While it is not an external radiation hazard, it can be an internal radiation hazard if tritium is inhaled, ingested, or absorbed through the skin. In applications where tritium is handled, tritium confinement is performed using different barriers to minimize releases to the environment. For gaseous (elemental), liquid (oxide), and metal (hydride) tritium, process piping and components provide the primary confinement function. Secondary tritium confinement is typically provided by inert (i.e. non-flammable gases such as nitrogen, argon, or helium) gloveboxes which are connected to a tritium stripper system. Primary tritium confinement barriers typically produce low volumes of high tritium concentrations of tritiated methane from carbon in steels or organic materials along with tritiated water/tritium oxide (e.g. HTO) and tritiated ammonia from reactions with oxygen and nitrogen. Tritium escaping primary confinement into secondary confinement atmospheres (e.g. gloveboxes) produce higher volumes of lower activity contamination than found in process piping. Tritium contamination also occurs by leaks or tritium permeation/diffusion through confinement materials. Tritium from inside primary confinement barriers will diffuse or leak out of the primary confinement barrier and usually into the air, if the system is inside an air hood or ventilated hot cell, or into the secondary confinement (e.g. glovebox) atmosphere which is either exhausted or stripped based on the function of the secondary confinement (glovebox) system. Accelerator based processes for medical isotope production represent an atypical tritium contamination challenge. In medical isotope production, deuterium supply gas is ionized and accelerated to a tritium gas target to produce neutrons that are then used to produce the medical isotopes through additional nuclear fission reactions. To create large voltage differentials for accelerator operations, an electrical insulation medium is needed to prevent or rapidly quench electric discharges. A common electrical insulation medium utilized in accelerator applications is sulfur hexafluoride (SF 6 ) gas. SF 6 has a high dielectric strength and allows for the construction of smaller accelerator systems compared to other electrical insulation mediums such as air or dry nitrogen. Due to tritium permeation/diffusion through accelerator process and confinement materials, there is the possibility that tritium can contaminate the electrical insulation medium of the accelerator. Tritium contaminated SF 6 creates a material without any obvious processes for managing the contamination, reuse, or disposal of the used SF 6 . This document will discuss possible management strategies for tritium contaminated SF 6 for accelerator-based processes for Molybdenum-99 (Mo-99) production.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2025

Seniority Structure in Neutron-Rich Nucleus 128 Ag : Evidence for Robustness of 𝑁 = 82 Shell Closure in Silver Isotopes

The spectroscopic studies of very neutron-rich nucleus 128 Ag have been performed for the first time at the Radioactive Isotope Beam Factory of RIKEN. A new seniority isomer with a half-life of 1.60(7) μs has been identified and is proposed to have a spin-parity of 16 - with a maximally aligned configuration comprising three proton holes in the g 9/2 orbital and one neutron hole in the h 11/2 orbital. The new level structure in 128 Ag is quite well described by shell model calculations without invoking excitations across the Z = 50 and N = 82 shell gaps, and presents a good case of seniority scheme in odd-odd nuclei in the south vicinity of the double-magic nucleus 132 Sn. With a classification of various components of the proton-neutron interaction, the inversion of lowest-lying 9 - and 10 - states between 128 Ag and its neighboring isotone 130 In is found to be dynamically ascribed to the seniority-nonconserving proton-neutron interaction components. The structure above 10 - up to the 16 - isomer in 128 Ag shows remarkable similarities to seniority structures in the semimagic nuclei 128 Pd and 130 Cd. These spectroscopic features in 128 Ag indicate that the N = 82 shell closure is still robust in silver isotopes.

Luo, D. W. [Peking University, Beijing (China); et↗
NASA NTRS1974

Clues in the rare gas isotopes to early solar system history

Rare gases in meteorites and lunar samples are discussed stimulating the discovery of the solar wind. Radioactive isotopes are examined, making a correlation to the origin of the solar system. It is shown that the heights of the peaks above the horizontal lines represent the spectrum of the fissiogenic sample. Nuclear tracks of iodine, xenon, and plutonium detected in lunar rocks are also explained.

Reynolds, J. H.↗
NASA NTRS1980

A cosmic-ray age based on the abundance of Be-10

The paper discusses a measurement of the isotopic composition of galactic cosmic-ray beryllium made with high resolution aboard the ISEE 3 spacecraft. The isotope fractions of Be-7, Be-9, and Be-10 were determined; the abundance of the radioactive isotope Be-10 is used to deduce the cosmic-ray confinement time of 8,400,000/yr and an interstellar gas density of 0.33 atoms/cu cm in the confinement volume. Errors in the propagation model parameters which result in comparable uncertainties are discussed.

Wiedenbeck, M. E.↗
DOE OSTI2023

Fission with Exotic Nuclei (Full Technical Report)

Despite its importance for stockpile stewardship or nuclear forensics, data on fission is fragmentary: most experiments have only been performed on stable actinide nuclei and are often incomplete, and theoretical simulations often contain many parameters hard to constrain, which results in large uncertainties. Consequently, nuclear libraries have large gaps for important isotopes. The goal of this project was to prepare to take advantage of the unprecedented yields of radioactive isotopes at the upcoming DOE Facility for Rare Ion Beams and to leverage recent progress in the field of machine learning to develop a comprehensive program of fission studies that could address some of the most pressing problems in nuclear fission over the next several decades. Our project leveraged synergies between experimental nuclear physics, nuclear theory, and data science expertise at LLNL. On the experimental front, our main objective was to develop in-house expertise for inverse kinematics reactions with relativistic beams as well as to field and test new detectors to perform correlated measurements of fission properties. On the theoretical side, the objective was to develop a novel, high-fidelity and scalable approach of fissionfragment calculations based on emulating computationally expensive, quantum-mechanical calculations of nuclear properties with deep neural networks.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

First spectroscopic study of odd-odd Cu 78

Nuclei in the vicinity of 78 Ni are important benchmarks for nuclear structure, which can reveal changes in the shell structure far from stability. Spectroscopy of the odd-odd isotope 78 CU was performed for the first time in an experiment with the EURICA setup at the Radioactive Isotope Beam Factory at RIKEN Nishina Center. Excited states in the neutron-rich isotope were populated following the β decay of 78 Ni produced by in-flight fission and separated by the BigRIPS separator. A level scheme based on the analysis of $\gamma$-$\gamma$ coincidences is presented. Tentative spin and parity assignments were made when possible based on the β -decay feeding intensities and $\gamma$-decay properties of the excited states. Time correlations between β and $\gamma$ decay show clear indications of an isomeric state with a half-life of 3.8(4) ms. Large-scale Monte Carlo shell-model calculations were performed using the A3DA-m interaction and a valence space comprising the full f p shell and the 1⁢g 9/2 and 2⁢d 5/2 orbitals for both protons and neutrons. The comparison of the experimental results with the shell-model calculations allows interpreting the excited states in terms of spin multiplets arising from the proton-neutron interaction. In conclusion, the results provide further insight into the evolution of the proton single-particle orbitals as a function of neutron number, and quantitative information about the proton-neutron interaction outside the doubly magic 78 Ni core.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Summary of Forensic Examinations in Support of Breach Sealed Source Event at Harborview Medical Facility on 2 May 2019

On May 2, 2019, International Isotopes, Inc. (INIS), a subcontractor to Triad National Security, LLC (contractor for Los Alamos National Laboratory) breached a sealed radioactive source containing ~2800 Ci of the radioactive isotope cesium-137 ( 137 Cs) at the University of Washington Harborview Research and Training (HRT) Building in downtown Seattle while attempting to recover the source for the National Nuclear Security Administration’s (NNSA’s) Off-site Source Recovery Program (OSRP). The breach of the source resulted in the contamination of 13 personnel, all 7 floors of the building, and a release of material to the environment. A summary of root and contributing causes of the event was investigated and published by a joint investigation team (JIT) co-led by NNSA and Triad National Security, LLC. That investigation was supported by forensics examinations provided by Pacific Northwest National Laboratory. This report summarizes the results of those forensic examinations.

61 RADIATION PROTECTION AND DOSIMETRY↗
NASA NTRS2007

Processes in Early Planetesimals: Evidence from Ureilite Meteorites

Ureilites are primitive ultramafic achondrites composed largely of olivine and pigeonite, with minor augite, carbon, sulphide and metal. They represent very early material in the history of the Solar System and form a bridge between undifferentiated chondrites and fully differentiated asteroids. They show a mixture of chemical characteristics, some of which are considered to be nebula-derived (e.g. a negative correlation between Mg/Fe and Delta O-17 that resembles that of the ordinary chondrites but at lower Delta O-17 values) whereas others have been imposed by asteroidal differentiation. Carbon isotope data show a striking negative correlation of delta C-13 values with mg# in olivine. delta C-13 also correlates positively with Delta O-17, and therefore this isotopic variation was probably also nebula-derived. Thus, oxygen and carbon isotope compositions and Fe-Mg systematics of each monomict ureilite were established before differentiation processes began. Heated by decay of short-lived radioactive isotopes, the ureilite asteroid started to melt. Metal and sulphide would have melted first, forming a Fe-S eutectic liquid, which removed chalcophile elements and incompatible siderophile elements, and basaltic melts that removed Al, Ca and the LREE. Several elements show different abundances and/or correlations with Fo content in olivine, e.g. carbon shows a positive correlation in ferroan ureilites, and a weak or even negative correlation in more magnesian compositions. HSE such as Os and Ir also show different distributions, i.e. ureilites with Fo < 82 have very scattered Os and Ir concentrations, which reach high values, whereas ureilites with Fo > 82 tend to have much less scattered and overall lower Os and Ir abundances. A similar change in elemental behaviour is shown by the Fe-Mn relations in ureilitic olivines: those with Fo contents < 85 show a good negative correlation, whereas those with Fo > 85 show much greater scatter. This suggests that a major change affected the parent body at a time when melting had reached relatively magnesian bulk compositions. We consider that this event may have been a hit and run collision in which the ureilite parent body collided with a larger object. During the collision, the ureilite mantle broke up catastrophically but re-accreted in a jumbled state around the still-intact core. Mg-rich basaltic melts that were in the process of being formed at the time of break-up were retained in part as melt clasts that re-accreted to the regolith and are found in polymict ureilites.

Mittlefehldt, David W.↗
NASA NTRS1991

Naturally induced secondary radiation in interplanetary space: Preliminary analyses for gamma radiation and radioisotope production from thermal neutron activation

Thermal neutron activation analyses were carried out for various space systems components to determine gamma radiation dose rates and food radiation contamination levels. The space systems components selected were those for which previous radiation studies existed. These include manned space vehicle radiation shielding, liquid hydrogen propellant tanks for a Mars mission, and a food supply used as space vehicle radiation shielding. The computational method used is based on the fast neutron distribution generated by the BRYNTRN and HZETRN transport codes for Galactic Cosmic Rays (GCR) at solar minimum conditions and intense solar flares in space systems components. The gamma dose rates for soft tissue are calculated for water and aluminum space vehicle slab shields considering volumetric source self-attenuation and exponential buildup factors. In the case of the lunar habitat with regolith shielding, a completely exposed spherical habitat was assumed for mathematical convenience and conservative calculations. Activation analysis of the food supply used as radiation shielding is presented for four selected nutrients: potassium, calcium, sodium, and phosphorus. Radioactive isotopes that could represent a health hazard if ingested are identified and their concentrations are identified. For nutrients soluble in water, it was found that all induced radioactivity was below the accepted maximum permissible concentrations.

Plaza-Rosado, Heriberto↗
DOE OSTI2021

Residual Insoluble Solids Expected from Saltcake Dissolution

A review of previous SRS saltcake dissolution and characterization studies was performed to inform the analysis of the amount of residual insoluble solids that may result from saltcake dissolution. A realistic value covering most cases for the maximum volume of a settled layer of residual insoluble solids that would result from dissolution of a volume of saltcake was calculated as 0.08 mL/mL (8 vol%). Applying factors to account for dissolution test uncertainty and differences between in-tank settling and laboratory testing, the recommended value for a settled layer of residual insoluble solids that would result from dissolution of a volume of saltcake is 0.16 mL/mL (16 vol%). This should apply to dissolution of saltcake with typical minimal amounts of entrained sludge but may not apply to saltcake with significant sludge. As it is composed of primarily non-radioactive isotopes, the precipitated aluminum hydroxide material does not contribute to the heat load.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRSDate not supplied

Development of Radioluminescent Tritium Polymeric Material for High Visibility Applications

The Development of Radioluminescent Tritium Polymeric Material for High Visibility Applications effort investigates the nature and properties of materials consisting of tritium lights combined with various silicone adhesives. Physical, mechanical, and optical properties will be observed/measured, including their durability in the low earth orbit environment. Tritium or hydrogen-three is a radioactive isotope of hydrogen that emits beta particles as it undergoes a process called beta decay. A beta particle is a high-energy, high-speed electron (or positron) emitted from radioactive decay of an atomic nucleus. Because it is a gas, tritium must be bound to a material or encapsulated in a sealed glass container. The gaseous tritium can then be combined with a phosphor source which when struck with beta particles, fluoresces and emits light. Such a light source is referred to as a gaseous tritium light source (GTLS). A self-powered, radioluminescent tritium material capable of surviving multiple space environments has the potential to fulfill visibility requirements levied on space flight hardware and facilitate additional long term internal and external lighting needs such as for imaging, docking, tracking, and xEMU suits for lunar exploration on the moon.

Lauren Fisher↗