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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Rotational excitations in rare-earth nuclei: A comparative study within three cranking models with different mean fields and treatments of pairing correlations

High-spin rotational bands in rare-earth Er (Z = 68), Tm (Z = 69), and Yb (Z = 70) isotopes are investigated by three different nuclear models. These are (i) the cranked relativistic Hartree-Bogoliubov (CRHB) approach with approximate particle number projection by means of the Lipkin-Nogami (LN) method, (ii) the cranking covariant density functional theory (CDFT) with pairing correlations treated by a shell-model-like approach (SLAP) or the so-called particle-number conserving (PNC) method, and (iii) cranked shell model (CSM) based on the Nilsson potential with pairing correlations treated by the PNC method. A detailed comparison between these three models in the description of the ground-state rotational bands of even-even Er and Yb isotopes is performed. The similarities and differences between these models in the description of the moments of inertia, the features of band crossings, and equilibrium deformations and pairing energies of the even-even nuclei under study are discussed. These quantities are considered as a function of rotational frequency and proton and neutron numbers. The changes in the properties of the first band crossings with increasing neutron number in this mass region are investigated. On average, a comparable accuracy of the description of available experimental data is achieved in these models. However, the differences between model predictions become larger above the first band crossings. Because of the time-consuming nature of numerical calculations in the CDFT-based models, a systematic study of the rotational properties of both ground-state and excited-state bands in odd-mass Tm nuclei is carried out only by the PNC-SCM. With few exceptions, the rotational properties of experimental 1-quasiparticle and 3-quasiparticle bands in 165,167,169,171 Tm are reproduced reasonably well. As a result, the appearance of backbendings or upbendings in these nuclei is well understood from the analysis of the variations of the occupation probabilities of the single-particle states and their contributions to total angular momentum alignment with rotational frequency.

150 ≤ A ≤ 189↗
DOE OSTI2021

Three-Dimensional Network Adjustment of Laser Tracker Measurements for Large-Scale Metrology Applications

The adjustment of laser tracker network measurements for large-scale metrology applications has unique considerations not commonly encountered in the network adjustment approaches generally used in either standard metrology or in traditional geodetic surveying. Many applications that require the measurement accuracy of a laser tracker are confined to small working areas to measure the dimensional quality of manufactured parts. Large-scale metrology applications require the same high measurement accuracy, but over a comparatively larger working area. This paper describes a unified least-squares approach to adjust three-dimensional survey network measurements that takes into account the unique considerations of large-scale metrology networks. The impetus for these unique considerations arises from an application that falls neatly between the disciplines of metrology and geodesy—resembling a mixture of the conditions and requirements from both. In conclusion, this paper will also describe a case study of a large-scale metrology survey network used to align the particle accelerator at Michigan State University’s Facility for Rare Isotope Beams (FRIB).

42 ENGINEERING↗
DOE OSTI2025

Glass-Bonded Monazite Waste Forms for Lanthanide and Actinide Immobilization: From Theoretical Design to Scale-Up Production and Characterization

The development of nuclear waste forms for both existing and future nuclear wastes is critical to ensuring global environmental safety. This study focuses on waste management from molten salt reactors, where fuel exists in a salt form and could be processed in real time for the removal of neutron poisons such as xenon isotopes (e.g., 135 Xe) and rare earth elements (REEs, e.g., 149 Sm). To ensure safe, stable, and long-term disposal in geological repositories, REEs must be incorporated into a durable waste form. Iron-phosphate glasses are a promising candidate due to their low melting points, high chemical durability, and their ability to incorporate high concentrations of REEs. In this study, we successfully prepared iron-phosphate glass waste forms with high Nd loadings (up to 37 mass %) in batch sizes ranging from small (23 g) to large (1600 g). The resulting materials contained up to 75 mass % NdPO 4 , contributing to their mechanical resilience and exceptional chemical durability. These findings highlight the potential of iron-phosphate glasses as high-efficiency, chemically durable waste forms and demonstrate the successful transition from theoretical design to scaled-up production.

amorphous materials↗
NASA NTRSDate not supplied

Mineralogical and Oxygen Isotopic Study of Grossite-Bearing Refractory Inclusions From Reduced CV Chondrites

Grossite (CaAl4O7) is predicted to condense as the third major phase, after corundum and hibonite, from a cooling gas of solar composition. Thus, this refractory phase likely preserves a crucial record of high-temperature conditions in the early solar nebula. However, grossite is relatively rare in CAIs from most carbonaceous chondrite groups, except for CH chondrites. Only six grossite-bearing CAIs were reported and studied from CV chondrites, and most of them were coarse-grained Type A inclusions. Our previous study reported the occurrence of six grossite-bearing, fine-grained Ca-Al-rich inclusions (FGIs) from reduced CV chondrites Efremovka, Thiel Mountains (TIL) 07003, and TIL 07007. Here we present oxygen isotopic data of grossite-bearing FGIs from reduced CV chondrites to determine if any oxygen isotopic heterogeneity occurs within and among these inclusions. This isotopic study was coordinated with a FIB/TEM study to examine the formation and alteration history of grossite-bearing FGIs in the early solar nebula and on the asteroidal parent body.

J. Han↗
NASA NTRS1987

Boundary conditions for the paleoenvironment: Chemical and physical processes in the pre-solar nebula

Detailed study of the first interstellar hydrocarbon ring, cyclopropenylidene (C3H2), is continuing. The singly deuterated isotope of this molecule, C3HD, was observed in several cold interstellar clouds. The results of a large survey for C3H2 in galactic sources of various types will soon be completed. It appears that cyclopropenylidene is present in virtually all interstellar clouds of at least moderate density. In order to make the first determinations of the CO2/CO abundance ratio in interstellar sources, observations of protonated CO2 were pursued. The spectrum from 18.5 to 22 GHz for several interstellar clouds is being systematically measured. Particular attention is being given to the cold, dark clouds TMC-1 and L124N, which may be formation sites for solar mass stars. The phenomena of maser emission from molecules of methanol is being studied in certain interstellar clouds. A comparison of 1 millimeter continuum emission from dust with the column density of carbon monoxide as determined from the rare C(18)O isotope for 4 molecular clouds in the Galaxy is nearing completion. Papers published during the period of this report are listed.

Irvine, William M.↗
DOE OSTI2025

Comparing field and lab quantitative stable isotope probing for nitrogen assimilation in soil microbes

ABSTRACT Soil microbial communities play crucial roles in nutrient cycling and can help retain nitrogen in agricultural soils. Quantitative stable isotope probing (qSIP) is a useful method for investigating taxon-specific microbial growth and utilization of specific nutrients, such as nitrogen (N). Typically, qSIP is performed in a highly controlled lab setting, so the field relevance of lab qSIP studies remains unknown. We conducted and compared tandem lab and field qSIP to quantify the assimilation of 15 N by maize-associated soil prokaryotic communities at two agricultural sites. Here, we show that field qSIP with 15 N can be used to measure taxon-specific microbial N assimilation. Relative 15 N assimilation rates were generally lower in the field, and the magnitude of this difference varied by site. Rates differed by method (lab vs field) for 19% of the top N assimilating genera. The field and lab measures were more comparable when relative assimilation rates were weighted by relative abundance to estimate the proportion of N assimilated by each genus with only ~10% of taxa differing by method. Of those that differed, the taxa consistently higher in the lab were inclined to have opportunistic lifestyle strategies, whereas those higher in the field had niches reliant on plant roots or in-tact soil structure (biofilms, mycelia). This study demonstrates that 15 N-qSIP can be successfully performed using field-incubated soils to identify microbial allies in N retention and highlights the strengths and limitations of field and lab qSIP approaches. IMPORTANCE Soil microbes are responsible for critical biogeochemical processes in natural and agricultural ecosystems. Despite their importance, the functional traits of most soil organisms remain woefully under-characterized, limiting our ability to understand how microbial populations influence the transformation of elements such as nitrogen (N) in soil. Quantitative stable isotope probing (qSIP) is a powerful tool to measure the traits of individual taxa. This method has rarely been applied in the field or with 15 N to measure nitrogen assimilation. In this study, we measured genus-specific microbial nitrogen assimilation in two agricultural soils and compared field and lab 15 N qSIP methods. Our results identify taxa important for nitrogen assimilation in agricultural soils, shed light on the field relevance of lab qSIP studies, and provide guidance for the future application of qSIP to measure microbial traits in the field.

Reed, Kinsey (ORCID:0000000155178664)↗
NASA NTRSDate not supplied

Coordinated analyses of hydrated Kuiper Belt dust

We report on coordinated mineralogical, chemical, and isotopic analyses of hydrated carbon-rich interplanetary dust particles (IDPs). We focus on hydrated IDPs that contain high solar flare track densities consistent with an origin in outer Solar System bodies such as Edgeworth-Kuiper belt objects (EKBOs) [1]. We are searching for evidence of the heavy water reservoir predicted by self-shielding models [2]. The IDPs were embedded in sulfur and microtome thin sections were obtained for Fourier-transform infrared (FTIR), transmission electron microscopy (TEM), and nanoSIMS analyses. The IDPs were only partly microtomed and the remainder was extracted from the sulfur and pressed into In or Au for high precision O isotopic analyses. The hydrated IDPs in this study are compact low-porosity objects with a mineralogy dominated by fine-grained saponite and lesser serpentine, Fe-Ni sulfides, Mg-Fe carbonates, rare crystaline silicates, and abundant organic matter. The C in the IDPs is abundant (typically >4X CI) and occurs as isolated nanoglobules and finely disseminated within the phyllosilicate matrix of the IDPs. TEM analyses of the nanoglobules show O-rich, S-depleted rims with higher carbonyl functionality than their cores. FTIR spectra show strong aliphatic C-H stretches consistent with the presence of short-chain aliphatic hydrocarbons in these IDPs. The oxygen isotopic compositions measured in 6 IDPs all plot within error of the CCAM line [3]. For several of the IDPs we were able to obtain multiple analyses. The ∆^(17)O values range from -23‰ up to +3.4‰ with most analyses clustering above the terrestrial fractionation line. The O isotopic compositions and the high C contents of these IDPs are distinct from known hydrated carbonaceous chondrites. The track-rich hydrated IDPs record parent body aqueous alteration effects through interactions with 16O-poor H2O on a EKBO parent body. The aqueous alteration activity likely resulted from the heat generated by collisional processes among EKBOs given that these objects are believed to have accreted late after the decay of 26Al [4].

Lindsay P. Keller↗
NASA NTRS2021

The effects of terrestrial weathering on samarium-neodymium isotopic composition of ordinary chondrites

Following their fall to Earth, meteorites experience weathering. In this systematic study, we evaluate the trace element composition of ordinary chondrites from the Antarctic cold desert, and Atacama (Chile) and Lut (Iran) hot deserts, with an emphasis on rare earth elements (REE). Our data confirms that terrestrial weathering of meteorites in hot deserts changes their trace element (Sr, Ba, REE, Hf, Th, and U) concentrations. However, weathering effects in majority of Antarctic samples are limited to slight Ba, REE, Hf, and Th depletions and in some case to U enrichment. In comparison to the Antarctic meteorites, hot desert samples show greater disturbances and REE fractionation relative to the average fall values. We measured the Sm-Nd isotopic composition of the hot desert meteorites that have heavily affected REE compositions. Our Sm-Nd isotopic data show a significant effect of terrestrial weathering evidenced by non-CHUR (147)Sm/(144)Nd and (143)Nd/(144)Nd ratios. Measurements show a higher variation and lower values of (147)Sm/(144)Nd for the Atacama samples than those from the Lut Desert. Deviations from CHUR (147)Sm/(144)Nd value are in positive accordance with the degree of La/Lu fractionation caused by weathering. The ɛNd values of Atacama and Lut deserts meteorites range from −2.20 to +1.61, which is wider than the −1.07 to +0.64 range for falls. We suggest that disturbance of primary Sm/Nd ratios resulting from mixing with terrestrial components originating from soil during weathering is responsible for lower (147)Sm/(144)Nd ratio in these meteorites. The majority of the Atacama meteorites regardless of their weathering degrees have their REE compositions and ɛNd affected by terrestrial contamination. Both (147)Sm/(144)Nd ratio and ɛNd values show no straightforward relationship with weathering degree. However, in both cases the samples with the highest negative isotopic disturbances are H chondrites from the Atacama and Lut deserts. In addition, Ba concentration shows a negative correlation with (147)Sm/(144)Nd ratio. Care must be taken into account while dealing with samples collected from hot deserts, even fresh-looking ones.

Isotope geochemistry↗
NASA NTRS1981

Isotopic and REE studies of lunar basalt 12038 - Implications for petrogenesis of aluminous mare basalts

Sr, Nd, and Sm isotopic studies of lunar basalt 12038, one of the so-called aluminous mare basalts, are reported. The evolution of the Sr and Nd isotopic compositions and the rare earth element (REE) abundances is successfully modeled within the framework of the model developed by Nyquist et al. (1977, 1979) for Apollo 12 olivine-pigeonite and ilmenite basalts. It is pointed out that the isotopic and trace element features of 12038 can by modeled as produced by partial melting of a cumulate mantle source which crystallized from a lunar magma ocean with a chondrite-normalized REE pattern of constant negative slope. Chondrite-normalized La/Yb is equal to 2.2 for this hypothetical magma ocean pattern.

Nyquist, L. E.↗
DOE OSTI2022

Density matrix renormalization group description of the island of inversion isotopes F 28 – 33

Recent experiments have confirmed that the neutron-rich isotopes 28,29 F belong to the so-called island of inversion (IOI), a region of the nuclear chart around Z = 10 and N = 20 where nuclear structure deviates from the standard shell model predictions due to deformation and continuum effects. However, while the general principles leading to the IOI are relatively well understood, the details of the low-lying structure of the exotic fluorine isotopes 28–33 F are basically unknown. In this study, we perform large-scale shell model calculations including continuum states to investigate the properties of the neutron-rich isotopes 25–33 F, from a core of 24 O and using an effective two-body interaction with a small number of adjustable parameters in the central and tensor channels. We develop two models adjusted on experimentally confirmed states in 25,26 O and 25–27 F based on different assumptions concerning the positions of the neutron 0d 3/2 and 1p 3/2 shells, and solve the many-body problem using the density matrix renormalization group (DMRG) method for open quantum systems in an sd–fp model space. We obtain the first detailed spectroscopy of 25–33F in the continuum and show how the interplay between continuum effects and deformation explains the recent data on 28,29 F. Several deformed one- and two-neutron halo states are predicted in 29,31 F, and we provide some information about the possible structure of the heaviest fluorine isotopes. We also suggest several experimental studies of interest to constraint models and test the present predictions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Gas Stopper Developments for Improved Purity and Intensity of Low-Energy, Rare Isotope Ion Beams (Final Technical Report)

This final technical report summarizes the work of the Michigan State University (MSU) team supported by grant # DE-SC0021423 awarded by the Office of Nuclear Physics, Department of Energy. Objectives: The successful fulfillment of the FRIB science mission hinges on ensuring the availability of fast, stopped, and reaccelerated beams consisting of rare isotopes. This project's research and development focus was dedicated to supporting the advancement and creation of a cutting-edge linear gas stopper. The primary aim is to efficiently convert the high-intensity fast beams of rare isotopes provided by FRIB into high-quality, low-energy beams. These beams are essential for conducting stopped beam experiments or for subsequent reacceleration. The overarching goal is to advance technology, aiming to increase the beam rate capability of the linear gas stopper for medium-to-heavy-mass rare isotopes by more than tenfold compared to the currently most effective gas stopper in operation, and to improve the purity of the delivered beams. Project Description: The existing technology employed in gas stopping devices designed for low-energy, rare-isotope beams presents limitations in both the purity of extracted beams and the intensities of injected beams. These limitations are incompatible with the requirements of the recently commissioned rare isotope beam facility, FRIB. Our research and development efforts, aligned with the previously outlined objectives, focused on addressing the most critical aspects for enhancing beam-rate capability and purity. Specifically, advanced particle-in-cell simulations were developed and integrated into a simulation pipeline to explore the efficacy of multi-layer RF carpets on increasing ion transport efficiency with high incoming beam rates that generate space charge fields which can limit it. We also explored the possibility of using a collision-induced-dissociation (CID) gas cell to break up molecular contaminant ions that are generated during the stopping process. A prototype CID gas cell was constructed and tested with beams from an offline ion source, validating the concept with the successful demonstration of breaking of molecular ions. The outcome of this research enabled the formulation a conceptual design for a next-generation linear gas stopping device specifically tailored for FRIB. This device is envisioned to deliver rare-isotope-ion beams at a rate of 10 8 particles per second or higher, accompanied by advancements in purity. Methods employed: This project leverages advancements in technologies initially designed for the Advanced Cryogenic Gas Stopper (ACGS), the current state-of-the-art linear gas stopper, through the use of new simulations and beam purification via collision-induced-dissociation. The methods include: 1. Development of a prototype low-energy, low-pressure CID gas stopper. This prototype features a thin, approximately 20 nm, Si 3 N 4 entrance window designed for dissociating stable and rare-isotope molecular ions. The goal is to enhance beam purification and overall efficiency. 2. Creation of Particle-in-cell (PIC) simulations to assess the advantages of multi-layer RF carpets and multi-point extraction for ion transport efficiency. These simulations rely on the 3DCylPIC package, specifically designed for studying devices of this nature. The goal is to quantify and mitigate ion transport losses due to space charge generated in the stopping process of large numbers of ions. 3. Perform ion transport simulations across an RF carpet using an 8-phase travelling wave and evaluate its performance. Compared to the 4-phase RF carpets used in ACGS, the 8-phase carpets will double the wavelength of the generated traveling wave allowing for larger maximum RF amplitudes that could result in improved ion transport efficiency for high-intensity incoming beams when large space charge fields are present. Impact: Tackling the primary challenges associated with transforming high-energy projectile fragment beams into low-energy beams—specifically, addressing efficiency and purity—holds significant promise for advancing FRIB science. This advancement will particularly impact precision mass measurements, laser spectroscopy of short-lived nuclei, and studies in astrophysics and nuclear reactions using reaccelerated beams. These domains play a crucial role in addressing key questions outlined in the 2023 NSAC long-range plan, spanning nuclear structure, nuclear astrophysics, and fundamental symmetries. Additionally, they contribute to addressing 10 out of the 17 benchmarks identified by the NRC RISAC. The development of a next-generation gas stopping device capable of delivering low-energy, rare-isotope beams at a rate of 10 8 particles per second, or more, with high purity holds the potential to unlock experiments that would otherwise be unfeasible. Furthermore, it is expected to reduce the time required for experiments at FRIB, thereby maximizing scientific output. The research and development activities performed as part of this project bolstered essential competencies at FRIB in beam physics and ion source technologies, provided valuable training opportunities for junior scientists.

43 PARTICLE ACCELERATORS↗
DOE OSTI2026

Investigating trends in actinide covalency and magnetism with 35/37 Cl SSNMR spectroscopy and first-principles calculations

Solid-state NMR (SSNMR) spectroscopy is a powerful technique for studying actinide chemistry but has been significantly limited due to the complex paramagnetism, and radiological hazards presented by these materials. Lanthanide and actinide salts often feature magnetic ordering and can be paramagnetic, ferromagnetic, or antiferromagnetic depending on temperature and electronic structure. Paramagnetic interactions can manifest in SSNMR both as secular spectral shifts and/or couplings as well as contributions from non-secular relaxation. Both effects can be directly measured with NMR and used to extrapolate rich chemical information such as coordination environments, bonding characteristics, local molecular dynamics, and correlation times. Typically, these studies are carried out on high-γ and highly abundant NMR-active isotopes (e.g., 1 H, 6/7 Li, 19 F, 23 Na, etc.) or on enriched rare isotopes (e.g., 2 H and 17 O), which can be expensive. Herein, we present a facile methodology to measure the 35/37 Cl electric-field gradient (EFG) and paramagnetic shift anisotropy (SA) tensor components using static wideline SSNMR measurements of LaCl 3 , NdCl 3 , UCl 3 , and UCl 4 . The static powder spectra were measured with both 35 Cl and 37 Cl SSNMR to increase the fidelity of the extracted tensor parameters. Variable temperature NMR of a select case confirms the Curie–Weiss paramagnetism. Relaxation measurements of both nuclei further corroborate observations owing to the paramagnetic relaxation enhancement and reveal simultaneous quadrupolar relaxation mechanisms. Density functional theory (DFT) calculations using Hubbard U corrections to the uranium valence orbitals show excellent agreement with experimental EFG tensor parameters and help describe the bonding characteristics in these lanthanide and actinide systems.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
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 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↗
NASA NTRS2005

An Achondritic Micrometeorite from Antarctica: Expanding the Solar System Inventory of Basaltic Asteroids

Micrometeorites with sizes below 1 mm are collected in a diversity of environments such as deep-sea sediments and polar caps. Chemical, mineralogical and isotopic studies indicate that micrometeorites are closely related to primitive carbonaceous chondrites that amount to only approximately 2% of meteorite falls. While thousands of micrometeorites have been studied in detail, no micrometeorite has been found so far with an unambiguous achondritic composition and texture. One melted cosmic spherule has a low Fe/Mn ratio similar to that of eucrites, the most common basaltic meteorite group. Here we report on the texture, mineralogy, Rare Earth Elements (REEs) abundance and oxygen isotopic composition of the unmelted Antarctic micrometeorite 99-21-40 that has an unambiguous basaltic origin.

Gounelle, M.↗
DOE OSTI2020

A Single Small-Scale Plutonium Redox Reaction System Yields Three Crystallographically-Characterizable Organoplutonium Complexes

Here, an approach to obtaining substantial amounts of data from a hazardous starting material that can only be obtained and handled in small quantities is demonstrated by the investigation of a single small-scale reaction of cyclooctatetraene, C 8 H 8 , with a solution obtained from the reduction of Cp' 3 Pu (Cp' = C 5 H 4 SiMe 3 ) with potassium graphite. This one reaction coupled with oxidation of a product has provided single-crystal X-ray structural data on three organoplutonium compounds as well as information on redox chemistry thereby demonstrating an efficient route to new reactivity and structural information on this highly radioactive element. The crystal structures were obtained from the reduction of C 8 H 8 by a putative Pu(II) complex, (Cp' 3 Pu II ) 1– , generated in situ, to form the Pu(III) cyclooctatetraenide complex, [K(crypt)][(C 8 H 8 ) 2 Pu III ], 1-Pu , and the tetra(cyclopentadienyl) Pu(III) complex, [K(crypt)][Cp' 4 Pu III ], 2-Pu . Oxidation of the sample of 1-Pu with Ag(I) afforded a third organoplutonium complex that has been structurally characterized for the first time, (C 8 H 8 ) 2 Pu IV , 3-Pu . Complexes 1-Pu and 3-Pu contain Pu sandwiched between parallel (C 8 H 8 ) 2– rings. The (Cp' 4 Pu III ) – anion in 2-Pu features three η 5 -Cp' rings and one η 1 -Cp' ring, which is a rare example of a formal Pu–C η 1 -bond. In addition, this study addresses the challenge of small-scale synthesis imparted by radiological and material availability of transuranium isotopes, in particular that of pure metal samples. A route to an anhydrous Pu(III) starting material from the more readily available Pu IV O 2 was developed to facilitate reproducible syntheses and allow complete spectroscopic analysis of 1-Pu and 2-Pu . Pu IV O 2 was converted to Pu III Br 3 (DME) 2 (DME = CH 3 OCH 2 CH 2 OCH 3 ) and subsequently Pu III Br 3 (THF) x , which was used to independently synthesize 1-Pu , 2-Pu , and 3-Pu .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Determination of γ-ray branching ratios for ⁹⁵Zr and ¹⁴⁷Nd

For many fission products, the γ 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 (FPYs), provided sufficiently accurate information on the γ-ray branching ratio 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 the γ-ray branching ratios in the 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 γ-ray branching ratios of the strongest transitions following the decay of ⁹⁵Zr and decay-daughter ⁹⁵Nb and determined these branching ratios to fractional precisions of 1%. We then applied this approach to determine the γ-ray branching ratios for the β decay of ¹⁴⁷Nd. The results for the γ-ray branching ratios are presented here and compared to previous results and evaluations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

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↗