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At least 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Berkelium–carbon bonding in a tetravalent berkelocene

Interest in actinide–carbon bonds has persisted since actinide organometallics were first investigated for applications in isotope separation during the Manhattan Project. Transplutonium organometallics are rarely isolated and structurally characterized, likely owing to limited isotope inventories, a scarcity of suitable laboratory infrastructure, and intrinsic difficulties with the anaerobic conditions required. In this paper, we report the discovery of an organometallic “berkelocene” complex prepared from 0.3 milligrams of berkelium-249. Single-crystal x-ray diffraction shows a tetravalent berkelium ion between two substituted cyclooctatetraene ligands, resulting in the formation of berkelium–carbon bonds. The coordination in berkelocene resembles that of uranocene, and calculations show that the berkelium 5f orbitals engage in covalent overlap with the δ-symmetry orbitals of the cyclooctatetraenide ligand π system. Charge transfer from the ligands is diminished relative to uranocene and other actinocenes, which maximizes contributions from the stable, half-filled 5f 7 configuration of tetravalent berkelium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1987

Rare earth element transport in the western North Atlantic inferred from Nd isotopic observations

The relationship between the Nd isotopic composition in the Atlantic waters and the origin and circulation of the water masses was investigated. Samples were collected in the western North Atlantic between 7 and 54 deg N. The isotopic composition (Nd-143/Nd-144 ratios) showed extensive vertical structure at all locations. In regions where a thermocline was well-developed, large isotopic shifts were observed across the base of the thermocline, while regions without a thermocline were characterized by much more gradual shifts in isotopic composition with depth. The data reveal an excellent correlation between the Nd isotopic distribution in the western North Atlantic water column and the distribution of water masses identified from temperature and salinity measurements.

Piepgras, D. J.↗
DOE OSTI2021

A novel experimental system for the KDK measurement of the 40 K decay scheme relevant for rare event searches

Potassium-40 ( 40 K) is a long-lived, naturally occurring radioactive isotope. The decay products are prominent backgrounds for many rare event searches, including those involving NaI-based scintillators. 40 K also plays a role in geochronological dating techniques. The branching ratio of the electron capture directly to the ground state of argon-40 has never been measured, which can cause difficulty in interpretingcertain results or can lead to lack of precision depending on the field and analysis technique. Additionally, the KDK (Potassium (K) Decay (DK)) collaboration is measuring this decay. A composite method has a silicon drift detector with an enriched, thermally deposited 40 K source inside the Modular Total Absorption Spectrometer. This setup has been characterized in terms of energy calibration, gamma tagging efficiency, live time and false negatives and positives. A complementary, homogeneous, method is also discussed; it employs a KSr 2 I 5 :Eu scintillator as source and detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS1998

Development of a High Resolution-High Sensitivity Ion Microprobe Facility for Cosmochemical Applications

NASA NAGW-4112 has supported development of the CAMECA ims 1270 ion microprobe at UCLA for applications in cosmochemistry. The instrument has been brought to an operational status and techniques developed for accurate, precise microbeam analysis of oxygen isotope ratios in polished thin-sections. We made the first oxygen isotopic (delta(18)O and delta(17)O) measurements of rare mafic silicates in the most chemically primitive meteorites, the a chondrites (Leshin et al., 1997). The results have implications for both high temperature processing in the nebula and low-T aqueous alteration on the CI asteroid. We have performed measurements of oxygen isotopic compositions of magnetite and co-existing olivine from carbonaceous (Choi et al., 1997) and unequilibrated ordinary chondrites (Choi et al., in press). This work has identified a significant new oxygen isotope reservoir in the early solar system: water characterized by a very high Delta(17)) value of approx. 5 % per thousand. We have determined the spatial distributions of oxygen isotopic anomalies in all major mineral phases of a type B CAI from Allende. We have also studied an unusual fractionated CAI from Leoville and made the first oxygen isotopic measurements in rare CAIs from ordinary chondrites.

McKeegan, Kevin D.↗
DOE OSTI2022

Defining the Sphagnum Core Microbiome across the North American Continent Reveals a Central Role for Diazotrophic Methanotrophs in the Nitrogen and Carbon Cycles of Boreal Peatland Ecosystems

Peat mosses of the genus Sphagnum are ecosystem engineers that frequently predominate over photosynthetic production in boreal peatlands. Sphagnum spp. host diverse microbial communities capable of nitrogen fixation (diazotrophy) and methane oxidation (methanotrophy), thereby potentially supporting plant growth under severely nutrient-limited conditions. Moreover, diazotrophic methanotrophs represent a possible “missing link” between the carbon and nitrogen cycles, but the functional contributions of the Sphagnum-associated microbiome remain in question. A combination of metagenomics, metatranscriptomics, and dual-isotope incorporation assays was applied to investigate Sphagnum microbiome community composition across the North American continent and provide empirical evidence for diazotrophic methanotrophy in Sphagnum-dominated ecosystems. Remarkably consistent prokaryotic communities were detected in over 250 Sphagnum SSU rRNA libraries from peatlands across the United States (5 states, 17 bog/fen sites, 18 Sphagnum species), with 12 genera of the core microbiome comprising 60% of the relative microbial abundance. Additionally, nitrogenase (nifH) and SSU rRNA gene amplicon analysis revealed that nitrogen-fixing populations made up nearly 15% of the prokaryotic communities, predominated by Nostocales cyanobacteria and Rhizobiales methanotrophs. While cyanobacteria comprised the vast majority (>95%) of diazotrophs detected in amplicon and metagenome analyses, obligate methanotrophs of the genus Methyloferula (order Rhizobiales) accounted for one-quarter of transcribed nifH genes. Furthermore, in dual-isotope tracer experiments, members of the Rhizobiales showed substantial incorporation of 13 CH 4 and 15 N 2 isotopes into their rRNA. Our study characterizes the core Sphagnum microbiome across large spatial scales and indicates that diazotrophic methanotrophs, here defined as obligate methanotrophs of the rare biosphere (Methyloferula spp. of the Rhizobiales) that also carry out diazotrophy, play a keystone role in coupling of the carbon and nitrogen cycles in nutrient-poor peatlands.

54 ENVIRONMENTAL SCIENCES↗
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 NTRS1978

Rare-earth abundances in chondritic meteorites

Fifteen chondrites, including eight carbonaceous chondrites, were analyzed for rare earth element abundances by isotope dilution. Examination of REE for a large number of individual chondrites shows that only a small proportion of the analyses have flat unfractionated REE patterns within experimental error. While some of the remaining analyses are consistent with magmatic fractionation, many patterns, in particular those with positive Ce anomalies, can not be explained by known magmatic processes. Elemental abundance anomalies are found in all major chondrite classes. The persistence of anomalies in chondritic materials relatively removed from direct condensational processes implies that anomalous components are resistant to equilibrium or were introduced at a late stage of chondrite formation. Large-scale segregation of gas and condensate is implied, and bulk variations in REE abundances between planetary bodies is possible.

Evensen, N. M.↗
NASA NTRS1991

He-3 and other lunar volatiles

Constraints are considered and estimates are given for the abundances of He-3, other noble gases, and chemically reactive volatiles (e.g., H, C, N, S, F, Cl) on the Moon. For the case of surface inventories, solar wind particles implanted into grains on the surface of the Moon provide an accessible, though not necessarily abundant, source of H, C, N and the noble gases. Solar wind implanted species are concentrated in the infest grain sized, and are only found in the upper few meters of the regolith, where there are grains that have been directly exposed to the Sun. Elemental abundances in surface soils are typically 10s of mg/g, and vary according to the exposure history of the soil. The abundance of the rare, but possibly economically important, isotope He-3 is typically a few mg/g. The largest uncertainty in estimates of the total lunar abundance of solar wind implanted species comes from the lack of knowledge of their distribution with depth below the upper meter or two. For the case of bulk inventories, constraints resulting from lunar sample analyses and from physical chemical models of volatile behavior during the hypothesized giant impact origin of the Moon is used to give estimated abundances.

Fegley, B., Jr.↗
NASA NTRS2019

A Re-Investigation of a Chondritic Xenolith in the Murchsion (CM2) Chondrite: Formation by Fluid-Assisted Percolation During Metamorphism

The CM chondrites are generally complex impact breccias, in which lithic clasts and mineral fragments showing various degrees of aqueous alteration and possibly originating from different parent bodies are mixed together. The occurrence of CM-like clasts in other chondritic and achondritic meteorite breccias is also well-documented, however, reports on the occurrence of foreign clasts in CM chondrites are rare. In this study, we reinvestigated the white clast in the Murchison CM chondrite and demonstrate that the clast is not related to R chondrites as earlier suggested. In addition to the classification we discuss the origin and the history of its formation by studying several aspects like mineralogy, bulk chemistry, Rare Earth Elements (REE), oxygen isotopes, and the soluble organic compounds.

Kerraouch, I.↗
NASA NTRS1971

Geochemical aspects of some Japanese lavas.

K, Rb, Sr, Ba and rare-earth concentrations in some Japanese lavas have been determined by mass-spectrometric stable-isotope dilution. The samples fall into three rare-earth groups corresponding to tholeiitic, high alumina and alkali basalts. Japanese tholeiites have trace element characteristics similar to those of oceanic ridge tholeiites except for distinctly higher relative concentrations of Ba. Japanese lavas may result from various degrees of partial fusion of amphibole eclogite.

Philpotts, J. A.↗
NASA NTRS2017

The Beryllium-10 Abundance in an Unusual Hibonite-Perovskite Refractory Inclusion from Allende: Implications for the Origin of Be-10

Beryllium-10 (decays to B-10, t1/2 = t(sub 1/2) = 1.3 Myr) 1.3 Myr) is a radionuclide that exclusively requires a is a radionuclide that exclusively requires a spallation origin. Therefore, one could obtain important insights into the irradiation environment in the solar nebula by understanding the distribution and abundance of this radionuclide in meteoritic inclusions. Most previous data are derived from B isotopic analysis of coarse-grained CV3 Ca-Al-rich Inclusions (CAIs) that have AL-26.Al-27 Al close to the canonical level of 5 x 10 (exp -5) and inferred Be-10/Be-9 ratios between 4 x 10(exp -4) and 1 x 10 (exp -2=3) [1-5]. Al-26-depleted FUN (Fractionaed and Unknown Nuclear anomalies) CAIs are less studied due to their rarity. FUN CAIs are thought to have formed prior to homogenization of Al-26/Al-27 Al and stable isotope anomalies (e.g., Ti-50) in the solar nebula, and thus represent one of the oldest Solar System solids [6]. So far, only three FUN CAIs (Axtell 2771, KT-1 and HAL) from CV3 chondrites have been measured for Be-10. They are characterized by variable Be-10/Be-9 ratios between (2.7−4.4) × 10(exp -4) [4,7]. Another group of rare, Al-26-free and and isotopically more anomalous inclusions, namely platy hibonite crystals (PLACs) from CM2 chondrites, have well-defined Be-10/Be-9 = (5.3 +/- 1.0) x 10 (exp -4) [9]. Al-26-free CAIs appear to have lower Be-1-/Be-9 than Al-26-bearing CAIs, although large analytical errors associated with some data would allow for an apparent overlap. It has been argued that the observed Be-10 variation resulted from the in-situ production of this radionuclide in CAIs (or their precursors) by irradiation, and the ratio difference simply reflects the fluctuation in projectile fluences [e.g., 9]. Another observation in support of this explanation comes from these CAIs' initial B-10/B-11 ratios, most of which are higher than the chondritic value 0.2478 [10]. This has been interpreted as a result of mixing between spallogenic B (B-10/B-11 = 0.4, co-produced with Be-10 in the irradiated solids) and a chondritic component [5,8]. Alternatively, given that all the inferred ratios, most of which are higher than chondritic value 0.2478 [10]. This has been interpreted as a result of mixing between spallogenic B (B-10/B-11 = 0.4, co-produced with Be-10 in the irradiated solics) and a chondritic component [5,8], Alternatively, given that all the inferred ratios in CAIs never fall below 3x10(exp -4), it has been proposed that the Solar System formed with baseline Be-10/Be-9 at this level, which originated from cosmic ray irradiation of the parental molecular cloud, and any value higher than this is a result of additional in-situ spallation [4,11]. Although not explicitly stated in this model, one would expect that inclusions that incorporated the background Be-10 abundance should form with the chondritic B isotopic ratio. However, the three FUN CAIs all have supra-chondritic B-10/B-11 indicative of the presence of a spallogenic component. To test whether some Be-10 did come into the solar nebula by inheritance,a better understanding of Be-10/Be-9 and initial B-10/B-11 in Al-26-free isotopically anomalous samples is needed. Here we present the result of Be10−B-10 system in an unsual hibonite-perovskite inclusion SHAL (son of HAL) from Allende.

Liu, M-C.↗
DOE OSTI2025

Emulation of the calculations of final r -process abundance patterns with a neural network

This work explores the construction of a fast emulator for the calculation of the final pattern of nucleosynthesis in the rapid neutron capture process (the r-process). An emulator is built using a feed-forward artificial neural network (ANN). We train the ANN with nuclear data and relative abundance patterns. We take as input the β-decay half-lives and the one-neutron separation energy of the nuclei in the rare-earth region. The output is the final isotopic abundance pattern. In this work, we focus on the nuclear data and abundance patterns in the rare-earth region to reduce the dimension of the input and output space. We show that the ANN can capture the effect of the changes in the nuclear physics inputs on the final r-process abundance pattern in the adopted astrophysical conditions. We employ the deep ensemble method to quantify the prediction uncertainty of the neural network emulator. The emulator achieves a speed-up by a factor of about 20 000 in obtaining a final abundance pattern in the rare-earth region. The emulator may be utilized in statistical analyses such as uncertainty quantification, inverse problems, and sensitivity analysis.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS2017

Distinct Chlorine Isotopic Reservoirs on Mars: Implications for Character, Extent and Relative Timing of Crustal Interaction with Mantle-Derived Magmas, Evolution of the Martian Atmosphere, and the Building Blocks of an Early Mars

The style, magnitude, timing, and mixing components involved in the interaction between mantle derived Martian magmas and Martian crust have long been a point of debate. Understanding this process is fundamental to deciphering the composition of the Martian crust and its interaction with the atmosphere, the compositional diversity and oxygen fugacity variations in the Martian mantle, the bulk composition of Mars and the materials from which it accreted, and the noble gas composition of Mars and the Sun. Recent studies of the chlorine isotopic composition of Martian meteorites imply that although the variation in delta (sup 37) Cl is limited (total range of approximately14 per mille), there appears to be distinct signatures for the Martian crust and mantle. However, there are potential issues with this interpretation. New Cl isotope data from the SAM (Sample Analysis at Mars) instrument on the Mars Science Lab indicate a very wide range of Cl isotopic compositions on the Martian surface. Recent measurements by [10] duplicated the results of [7,8], but placed them within the context of SAM surface data. In addition, Martian meteorite Chassigny contains trapped noble gases with isotopic ratios similar to solar abundance, and has long been considered a pristine, mantle derived sample. However, previous studies of apatite in Chassigny indicate that crustal fluids have interacted with regions interstitial to the cumulus olivine. The initial Cl isotope measurements of apatite in Chassigny suggest an addition of crustal component to this lithology, apparently contradicting the rare gas data. Here, we examine the Cl isotopic composition of multiple generations and textures of apatite in Chassigny to extricate the crustal and mantle components in this meteorite and to reveal the style and timing of the addition of crustal components to mantle-derived magmas. These data reveal distinct Martian Cl sources whose signatures have their origins linked to both the early Solar System and the evolving Martian atmosphere.

Shearer, C. K.↗
DOE OSTI2021

Development of a separation method for rare earth elements using LN resin

The lanthanide elements and isotopes are analytes of significant interest for several nuclear-related fields. Chemical separation among these elements is uniquely challenging due to their nearly identical chemical properties. This difficulty in interelement separation can create obstacles for quantitative radiometric analysis, specifically for isotopes without distinct energy emissions easily measured by gamma spectroscopy, for example Tb-161. Presented in this work is an optimized method for the isolation of individual rare earth elements using Eichrom’s LN resin.

Arrigo, Leah M.↗
NASA NTRS2020

Coordinated NanoSIMS and TEM Analysis of a Large 26Mg-Rich AGB Silicate from the Meteorite Hills 00426 CR2 Chondrite

Silicates are one of the most abundant presolar phases around evolved stars, in the inter-stellar medium (ISM), and in our Solar System. These grains afford the opportunity for O, Si, Mg, Fe, and Ca isotopic analyses to constrain stellar nucleosynthetic and mixing processes, and Galactic chemical evolution (GCE). While Mg and Fe isotopic studies have been successfully conducted on presolar silicates, isotopic analyses beyond O and Si are often hampered by the small grain sizes (average ~250 nm). This also makes coordinated mineral and chemical characterization challenging. These studies provide insight into the dust condensation conditions as well as subsequent alteration in the ISM and/or the Solar System. TEM studies of presolar silicates have shown that they are much more mineralogically and chemically diverse than other presolar phases [1 and references therein]. Large (>500nm) presolar silicate grains are rare, but they allow for detailed isotopic, mineral, and chemical characterization. We identified a large presolar silicate grain in the MET 00426 CR2 chondrite and report the O, Si, Mg, and Fe isotopic compositions and TEM study of this grain.

Nguyen, A. N.↗
NASA NTRS1997

Seventh Annual V. M. Goldschmidt Conference

Topics considered include: Subduction of the Aseismic Cocos Ridge Displaced Magma Sources Beneath the Cordillera de Talamanca, Costa Rica; Topography of Transition Zone Discontinuities: A Measure of 'Olivine' Content and Evidence for Deep Cratonic Roots; Uranium Enrichment in Lithospheric Mantle: Case Studies from French Massif Central; Rare-Earth-Element Anomalies in the Decollement Zone of the nankai Accretionary Prism, Japan: Evidence of Fluid Flow?; Rare Earth Elements in Japanese Mudrocks: The Influence of Provenance; The Evolution of Seawater Strontium Isotopes in the Last Hundred Million Years: Reinterpretation and Consequences for Erosion and Climate Models; From Pat to Tats: The Lead Isotope Legacy in the Studies of the Continental Crust-Upper Mantle System; Geochronology of the Jack Hills Detrital Zircons by Precise Uranium-Lead Isotope-Dilution Analysis of Crystal Fragments; Iridium in the Oceans; The Helium-Heat-Lead Paradox; Control of Distribution Patterns of Heavy Metals in Ganga Plain Around Kanpur Region, India, by Fluvial Geomorphic Domains; Geochemical and Isotopic Features of Ferrar Magmatic Provience (Victoria Land, Antarctica); Rare Earth Elements in Marine Fine-Grained Sediments from the Northwestern Portuguese Shelf (Atlantic); Aspects of Arc Fluxes; General Kinetic Model for Dolomite Precipitation Rate with Application to the Secular History of Seawater Composition; High-Precision Uranium-series Chronology from Speleothems; Trace-Element Modeling of Aqueous Fluid-Peridotite Interaction in the Mantle Wedge of Subduction Zones; Rainfall Variations in Southeastern Australia over the Last 500,000 Years from Speleothem Deposition; The Role of Water in High-Pressure Fluids; The Kinetic Conditions of Metamorphic Minearogenesis: Evidence from Minerals and Assemblages.

Source record↗
DOE OSTI2021

Chemical Compositions of Red Giant Stars from Habitable Zone Planet Finder Spectroscopy

We have used the Habitable Zone Planet Finder (HPF) to gather high-resolution, high signal-to-noise near-infrared spectra of 13 field red horizontal branch (RHB) stars, one open cluster giant, and one very metal-poor halo red giant. The HPF spectra cover the 0.81–1.28 μm wavelength range of the zyJ bands, partially filling the gap between the optical (0.4–1.0 μm) and infrared (1.5–2.4 μm) spectra already available for the program stars. We derive abundances of 17 species from LTE-based computations involving equivalent widths and spectrum syntheses, and estimate abundance corrections for the species that are most affected by departures from LTE in RHB stars. Generally good agreement is found between HPF-based metallicities and abundance ratios and those from the optical and infrared spectral regions. Light element transitions dominate the HPF spectra of these red giants, and HPF data can be used to derive abundances from species with poor or no representation in optical spectra (e.g., C i, P i, S i, K i). Attention is drawn to the HPF abundances in two field solar-metallicity RHB stars of special interest: one with an extreme carbon isotope ratio, and one with a rare, very large lithium content. The latter star is unique in our sample in exhibiting very strong He i 10830 Å absorption. The abundances of the open cluster giant concur with those derived from other wavelength regions. Detections of C i and S i in HD 122563 are reported, yielding the lowest metallicity determination of [S/Fe] from more than one multiplet.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Mapping the N = 40 island of inversion: Precision mass measurements of neutron-rich Fe isotopes

Nuclear properties across the chart of nuclides are key to improving and validating our understanding of the strong interaction in nuclear physics. Here we present high-precision mass measurements of neutron-rich Fe isotopes performed at the TITAN facility. The multiple-reflection time-of-flight mass spectrometer (MR-ToF-MS), achieving a resolving power greater than 600000 for the first time, enabled the measurement of 63–70 Fe, including first-time high-precision direct measurements (δm/m ≈ 10 -7 ) of 68–70 Fe, as well as the discovery of a long-lived isomeric state in 69 Fe. These measurements are accompanied by both mean-field and ab initio calculations using the most recent realizations which enable theoretical assignment of the spin-parities of the 69 Fe ground and isomeric states. Together with mean-field calculations of quadrupole deformation parameters for the Fe isotope chain, these results benchmark a maximum of deformation in the N = 40 island of inversion in Fe and shed light on trends in level densities indicated in the newly refined mass surface.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗