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At least 145 records · Page 8

Coupled Nd-142, Nd-143 and Hf-176 Isotopic Data from 3.6-3.9 Ga Rocks: New Constraints on the Timing of Early Terrestrial Chemical Reservoirs

Increasingly precise data from a range of isotopic decay schemes, including now extinct parent isotopes, from samples of the Earth, Mars, Moon and meteorites are rapidly revising our views of early planetary differentiation. Recognising Nd-142 isotopic variations in terrestrial rocks (which can only arise from events occurring during the lifetime of now extinct Sm-146 [t(sub 1/2)=103 myr]) has been an on-going quest starting with Harper and Jacobsen. The significance of Nd-142 variations is that they unequivocally reflect early silicate differentiation processes operating in the first 500 myr of Earth history, the key time period between accretion and the beginning of the rock record. The recent establishment of the existence of Nd-142 variations in ancient Earth materials has opened a new range of questions including, how widespread is the evidence of early differentiation, how do Nd-142 compositions vary with time, rock type and geographic setting, and, combined with other types of isotopic and geochemical data, what can Nd-142 isotopic variations reveal about the timing and mechanisms of early terrestrial differentiation? To explore these questions we are determining high precision Nd-142, Nd-143 and Hf-176 isotopic compositions from the oldest well preserved (3.63- 3.87 Ga), rock suites from the extensive early Archean terranes of southwest Greenland and western Australia.

Bennett, Vickie C.↗

Position-specific kinetic isotope effects for nitrous oxide: a new expansion of the Rayleigh model

Nitrous oxide (N 2 O) is a potent greenhouse gas and the most significant anthropogenic ozone-depleting substance currently being emitted. A major source of anthropogenic N 2 O emissions is the microbial conversion of fixed nitrogen species from fertilizers in agricultural soils. Thus, understanding the enzymatic mechanisms by which microbes produce N 2 O has environmental significance. Measurement of the 15 N/ 14 N isotope ratios of N 2 O produced by purified enzymes or axenic microbial cultures is a promising technique for studying N 2 O biosynthesis. Typically, N 2 O-producing enzymes combine nitrogen atoms from two identical substrate molecules (NO or NH 2 OH). Position-specific isotope analysis of the central (N α ) and outer (N β ) nitrogen atoms in N 2 O enables the determination of the individual kinetic isotope effects (KIEs) for N α and N β , providing mechanistic insight into the incorporation of each nitrogen atom. Previously, position-specific KIEs (and fractionation factors) were quantified using the Rayleigh distillation equation, i.e., via linear regression of δ 15 N α or δ 15 N β against [–f In f / (1 – f)], where f is the fraction of substrate remaining in a closed system. This approach, however, is inaccurate for N α and N β because it does not account for fractionation at N α affecting the isotopic composition of substrate available for incorporation into the β position (and vice versa). Therefore, we developed a new expansion of the Rayleigh model that includes specific terms for fractionation at the individual N 2 O nitrogen atoms. By applying this Expanded Rayleigh model to a variety of simulated N 2 O synthesis reactions with different combinations of normal, inverse, and/or no KIEs at N α and N β , we demonstrate that our new model is both accurate and robust. We also applied this new model to two previously published datasets describing N 2 O production from NH 2 OH oxidation in a methanotroph culture (Methylosinus trichosporium) and N 2 O production from NO by a purified Histoplasma capsulatum (fungal) P450 NOR, demonstrating that the Expanded Rayleigh model is a useful tool in calculating position-specific fractionation for N 2 O synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Collapse of Nuclear Collectivity along the 𝑁 = 𝑍 Line

The lifetime of the 𝐽 𝜋 = 2 + state in the self-conjugate 88 Ru nucleus has been determined in an experiment performed using rare-isotope beams provided by the new Facility for Rare Isotope Beams. This is the heaviest 𝑁 = 𝑍 nucleus for which such a measurement has been achieved. 88 Ru was populated by both one-neutron knockout and charge-exchange reactions, and the lifetime of 14.3$^{+2.5}_{−3.4}$ ps was determined using the triple-foil plunger technique. The extracted electromagnetic transition strength shows that the quadrupole collectivity has dropped significantly compared with the highly deformed 𝑁 = 𝑍 region around 𝐴 ∼ 80. These results are compared with state-of-the-art large-scale shell-model and discrete nonorthogonal shell-model calculations. The theoretical calculations indicate a moderate triaxial deformation and suggest that low-lying states in this nucleus are no longer dominated by strong many-particle many-hole excitations, unlike the lighter, highly deformed 𝑁 = 𝑍 nuclei nearby.

59 ≤ A ≤ 89↗

Isotopic analysis of sub-nanogram neodymium loads using new ATONA™ amplifiers

The long-term gains of the ATONA™ amplifiers are shown to have less than 1 ppm variability. Repeat measurements of the JNdi-1 reference material demonstrate the ability of the ATONA™ amplification technology to make measurements of 143 Nd/ 144 Nd ratios with 23 ppm external reproducibility on 100-pg loads. The effect of increasing integration time on analytical reproducibility is also displayed as increasing integration time from 10 to 30s reduced the external measurement uncertainty from 37 to 23 ppm. These measurements represent an improvement of more than a factor of 3 in external measurement reproducibility relative to previously published 143 Nd/ 144 Nd measurements of 100-pg loads. Furthermore, this new technology will allow for the measurement of smaller samples for precise isotope ratios and open new avenues of research in the geological and nuclear forensic communities.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Ag Isotopic Evolution of the Mantle During Accretion: New Constraints from Pd and Ag Metal-Silicate Partitioning

Decay of (sup 107) Pd to (sup 107) Ag has a half-life of 6.5 times 10 (sup 6) mega-annums. Because these elements are siderophile but also volatile, they offer potential constraints on the timing of core formation as well as volatile addition. Initial modelling has shown that the Ag isotopic composition of the bulk silicate Earth (BSE) can be explained if accretion occurs with late volatile addition. These arguments were tested for sensitivity for pre-cursor Pd/Ag contents, and for a fixed Pd/Ag ratio of the BSE of 0.1. New Ag and Pd partitioning data has allowed a better understanding of the partitioning behavior of Pd and Ag during core formation. The effects of S, C and Si, and the effect of high temperature and pressure has been evaluated. We can now calculate D(Ag) and D(Pd) over the wide range of PT conditions and variable metallic liquid compositions that are known during accretion. We then use this new partitioning information to revisit the Ag isotopic composition of the BSE during accretion.

Righter, K.↗

Isotopically anomalous xenon in meteorites - A new clue to its origin

The CCF xenon component in primitive meteorites, which has been attributed either to fission of a superheavy element or to nucleosynthesis in a supernova, does not show the large enrichment in Xe-129 (from decay of 16 Myr I-129) expected for supernova ejecta. Although this problem can be circumvented by ad hoc assumptions, a fission origin of CCFXe seems more likely.

Lewis, R. S.↗

A Plan to Qualify New Fuel for the High Flux Isotope Reactor for Material Minimization

The High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL) is one of five high power research reactors the Office of Material Management and Minimization (M3) Program, Office of Conversion is working to convert from using highly enriched uranium (HEU) fuel to using low-enriched uranium (LEU) fuel. This effort stems from the primary objective within the U.S. Department of Energy (DOE) National Nuclear Security Administration (NNSA) to achieve permanent threat reduction by minimizing, and when possible, eliminating weapon-usable nuclear material around the world. Under M3’s Office of Conversion, the U.S. High Performance Research Reactor (USHPRR) Project is pursuing fuel qualification and licensing of LEU fuels to support the high-performance reactors. All high-performance reactors except HFIR will be converted to LEU monolithic uranium-molybdenum alloy fuel. HFIR will be evaluated for conversion to LEU using a uranium silicide fuel, namely, U3Si2-Al dispersion fuel. The mission of the USHPRR Project is to develop the technology needed to reduce, and eventually eliminate, worldwide use of HEU in civilian applications. The goal is to develop the technical means needed to use low enriched uranium (LEU) instead of HEU fuel in research and test reactors without significant penalties in performance, economics, or safety of the reactors. The USHPRR Project has four major elements, called Pillars: Fuel Qualification (FQ) managed at Idaho National Laboratory (INL), Fuel Fabrication (FF) managed at Pacific Northwest National Laboratory (PNNL), Reactor Conversion (RC) managed at Argonne National Laboratory (Argonne), and Cross-Cutting (CC) managed at Savannah River National Laboratory (SRNL). FQ is responsible for the qualification of the fuel type. RC is responsible for supporting reactor conversion analysis and overseeing licensing submittals leading to conversions of domestic reactors to LEU fuel. For the FQ effort, FQ (INL) worked in collaboration with RC (Argonne) and ORNL to develop the plan for the uranium silicide fuel qualification for HFIR. The resulting HFIR Fuel Qualification Plan provides the general approach for the USHPRR team to move the selected uranium silicide fuel design for HFIR conversion through qualification. Authorization and use in HFIR will be approved through the DOE’s Office of Science. Uranium silicide fuel was previously qualified in NUREG-1313 at an approximate maximum heat flux of 1.4 MW/m2 and a maximum fuel section temperature of about 130°C. In addition to the different regulator process utilized by DOE, these upper limits will be exceeded in HFIR; therefore, further testing will be necessary to ensure the fuel can meet HFIR qualification requirements. The HFIR fuel loading may exceed 4.8 gU/cm3 which was determined in the NUREG-1313 safety evaluation to be acceptable for use in non-power NRC-licensed reactors provided there exist no other safety considerations. In addition, the uranium silicide fuel will need to be qualified in a HFIR-specific design. This plan includes the currently available information from the USHPRR Project Functions and Requirements document and expands these requirements to ensure that planned tests have traceable results providing evidence that the requirements have been met. Data collection methods are discussed as well as the process to show that the requirements have been met. This document is designed to provide a pathway for researchers to obtain data necessary and at the appropriate quality level for HFIR fuel qualification

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A Plan to Qualify New Fuel for the High Flux Isotope Reactor for Material Minimization

The High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL) is one of five high power research reactors the Office of Material Management and Minimization (M3) Program, Office of Conversion is working to convert from using highly enriched uranium (HEU) fuel to using low-enriched uranium (LEU) fuel. This effort stems from the primary objective within the U.S. Department of Energy (DOE) National Nuclear Security Administration (NNSA) to achieve permanent threat reduction by minimizing, and when possible, eliminating weapon-usable nuclear material around the world. Under M3’s Office of Conversion, the U.S. High Performance Research Reactor (USHPRR) Project is pursuing fuel qualification and licensing of the high-performance reactors to operate with LEU fuels. All high-performance reactors except HFIR will be converted to LEU monolithic uranium-molybdenum alloy fuel. HFIR will be evaluated for conversion to LEU using a uranium silicide fuel, namely, U3Si2-Al dispersion fuel.The mission of the USHPRR Project is to develop the technology needed to reduce, and eventually eliminate, worldwide use of HEU in civilian applications. The goal is to develop the technical means needed to use low enriched uranium (LEU) instead of HEU fuel in research and test reactors without significant penalties in performance, economics, or safety of the reactors. The USHPRR Project has four major elements, called Pillars: Fuel Qualification (FQ) managed at Idaho National Laboratory (INL), Fuel Fabrication (FF) managed at Pacific Northwest National Laboratory (PNNL), Reactor Conversion (RC) managed at Argonne National Laboratory (Argonne), and Cross-Cutting (CC) managed at Savannah River National Laboratory (SRNL). FQ is responsible for the qualification of the fuel type. RC is responsible for supporting reactor conversion analysis and overseeing licensing submittals leading to conversions of domestic reactors to LEU fuel. For the FQ effort, FQ (INL) worked in collaboration with RC (Argonne) and ORNL to develop the plan for the uranium silicide fuel qualification for HFIR.The resulting HFIR Fuel Qualification Plan provides the general approach for the USHPRR team to move the selected uranium silicide fuel design for HFIR conversion through qualification. Authorization and use in HFIR will be approved through the DOE’s Office of Science. Uranium silicide fuel was previously qualified in NUREG-1313 at an approximate maximum heat flux of 1.4 MW/m2 and a maximum fuel section temperature of about 130°C. In addition to the different regulator process utilized by DOE, these upper limits will be exceeded in HFIR; therefore, further testing will be necessary to ensure the fuel can meet HFIR qualification requirements. The HFIR fuel loading may exceed 4.8 gU/cm3 which was determined in the NUREG-1313 safety evaluation to be acceptable for use in non-power NRC-regulated reactors provided there exist no other safety considerations. In addition, the uranium silicide fuel will need to be qualified in a HFIR-specific design. This plan includes the currently available information from the USHPRR Project Functions and Requirements document and expands these requirements to ensure that planned tests have traceable results providing evidence that the requirements have been met. Data collection methods are discussed as well as the process to show that the requirements have been met. This document is designed to provide a pathway for researchers to obtain data necessary and at the appropriate quality level for HFIR fuel qualification.

Shokes, Tamara↗

Production of NBL PO plutonium isotopic standards CRM 136A, CRM 137A, and CRM 138A

Lawrence Livermore National Laboratory (LLNL) produced approximately 1 mg units of purified Pu from the parent New Brunswick Laboratory (NBL) certified reference materials (CRM) 137, 136 and 138 isotopic standards for the NBL Program Office (NBL PO) as detailed in the revised project plan. As stated in the plan, three representative units of each material were dispensed at the same time to be characterized at LLNL and provide informational values for the quantity of Pu and progeny nuclides in each unit. NBL PO intends to collect and evaluate isotopic measurement data from multiple laboratories and certify these materials as new isotopic standards C137A, C136A, and C138A, respectively. Soon after production eleven units of each analytical standard were shipped to other analytical laboratories for the certification effort, and 121, 119, and 119 units of C137A, C136A and C138A, respectively were shipped to Mickey Finch at Y12 NBL distribution center in November 2024 (30-gallon drum, TID 003777 PRL 7000005043). Residual purified Pu from the effort is being stored indefinitely in B332 at LLNL. Detailed methods can be found in the production plan, and this report describes and documents aspects of the production effort that are not in or were modified from the original production plan.

and nuclear chemistry↗

Time-of-flight experiments for nuclear structure and astrophysics

Neutron-rich isotopes are atomic nuclei with a large neutron excess compared to their stable counter parts. Their study provides essential information to understand the properties of the nuclear interaction, and to model nuclear processes in extreme astrophysical environments where neutron-rich isotopes drive the chains of nuclear reactions. Experimentally, these unstable isotopes are difficult to study because of their short half-lives and low production yields at particle accelerator laboratories. The TOF-Bρ technique is a mass measurement technique specialized for experiments with fast beams of short-lived radioactive isotopes. In this project we used the technique for two experiments performed at the National Superconducting Cyclotron Laboratory to measure new masses of isotopes in the region of 112 Mo and 46 S. The experiments at the NSCL were complemented by the development of new timing radiation detectors and experimental techniques to improve the performance and reach of mass measurements on neutron-rich isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Stable isotope analysis at the molecular level: A new approach for determining the origins of amino acids in the Murchison meteorite

A combined gas chromatography/isotope ratio mass spectrometry (GC/IRMS) method has been developed that permits the direct stable carbon isotope analysis of N(O)-trifluoroacetyl-isopropyl esters of individual amino acids and their respective enantiomers at nanomole abundances. Calculation of the original delta C-13 values of the amino acids is accomplished via a correction for the carbon introduced during the derivatization process. Previous GC/IRMS analyses of individual amino acids in the non-hydrolyzed water extract of an interior sample of a Murchison meteorite stone revealed an enrichment in C-13 relative to terrestrial organic matter, in agreement with previous findings for bulk extracts. The range of amino acid delta C-13 values (+5 to +30 per mill, PDB) suggests possible kinetic effects during synthesis. In this study, an apparent kinetic isotope effect was also observed for the amino acid products of a spark discharge experiment. These preliminary resutls are supportive of a similar mechanism for the abiotic synthesis of amino acids in the Murchison meteorite.

Engel, M. H.↗

Nd and Sr isotopic evidence for the origin of tektite material from DSDP site 612 off the New Jersey coast

The Sr and Nd isotopic composition was analyzed for samples from the Late Eocene tektite material from DSDP site 612 off the New Jersey coast, to determine whether these tektites may be assigned to the North-American-tektite group. It was found that the ranges of the Sr-87/Sr-86 and the Nd-143/Nd-144 ratios were much wider than in the 612-tectite material than in the tightly constrained group of North American tektites and microtektites and were significantly different from ratios in other groups of tektites. Results indicate that the DSDP tektites were formed from a chemically and isotopically heterogeneous material, in a regime that was different from that of other groups of tektites. It is suggested that the 612-tectites and the North American tektites were either formed by impacts of several bolides in the same general area or by a single impact event that sampled different layers.

Stecher, O.↗

Application of Fe Isotopes to the Search for Life and Habitable Planets

The relatively new field of Fe isotope geochemistry can make important contributions to tracing the geochemical cycling of Fe, which bears on issues such as metabolic processing of Fe, surface redox conditions, and development of planetary atmospheres and biospheres. It appears that Fe isotope fractionation in nature and the lab spans about 4 per mil (%) in Fe-56/Fe-54, and although this range is small, our new analytical methods produce a precision of +/- 0.05% on sample sizes as small as 100 ng (10(exp -7) g); this now provides us with a sufficient "signal-to-noise" ratio to make this isotope system useful. We review our work in three areas: 1) the terrestrial and lunar rock record, 2) experiments on inorganic fractionation, and 3) experiments involving biological processing of Fe. Additional information is contained in the original extended abstract.

Johnson, Clark M.↗

The mineralogical, chemical, and chronological characteristics of the crystalline Apollo 16 impact melt rocks

A comparative review of mineralogical, chemical, and chronological data on crystalline Apollo 16 impact melt rocks is presented. The use of such data to identify distinct impact melt complex is discussed, and 22 distinct impact melt bodies are identified. The recently detected group of feldspathic microporphyritic (FM) melt rocks was tested for chemical and isotopic homogeneity; instrumental neutron activation analysis and new Rb-Sr isotopic whole rock data indicate that FMs were probably not derived from a single impact melt sheet, but might be representative of the Descartes basement. Stratigraphical and chronological concepts for the geological development of the landing site are discussed, and a model is presented for the formation of the Cayley Plains and the Descartes formation.

Reimold, W. U.↗

Source term estimation using noble gas and aerosol samples

Algorithms that estimate the location, time, and magnitude of a point-source atmospheric release using remotely sampled air concentrations typically use data for a single chemical or radioactive isotope. Here, a Bayesian algorithm is presented that uses data from multiple radioactive isotopes that are all released in the same short-duration event. Data from noble gas and aerosol samplers can be used simultaneously in the model. Application to a large synthetic data set using four isotopes shows the new algorithm generally gives more accurate location and time estimates than a comparable model using a single isotope.

54 ENVIRONMENTAL SCIENCES↗

A new highly enriched 233 U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples

A highly-enriched 233 U reference material (>0.99987 n( 233 U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity 233 U to further reduce trace amounts of contaminant Pu in the material. The purified 233 U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Furthermore, modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used 233 U certified reference materials.

233U↗

Water isotopes, climate variability, and the hydrological cycle: recent advances and new frontiers

Abstract The hydrologic cycle is a fundamental component of the climate system with critical societal and ecological relevance. Yet gaps persist in our understanding of water fluxes and their response to increased greenhouse gas forcing. The stable isotope ratios of oxygen and hydrogen in water provide a unique opportunity to evaluate hydrological processes and investigate their role in the variability of the climate system and its sensitivity to change. Water isotopes also form the basis of many paleoclimate proxies in a variety of archives, including ice cores, lake and marine sediments, corals, and speleothems. These records hold most of the available information about past hydrologic variability prior to instrumental observations. Water isotopes thus provide a ‘common currency’ that links paleoclimate archives to modern observations, allowing us to evaluate hydrologic processes and their effects on climate variability on a wide range of time and length scales. Building on previous literature summarizing advancements in water isotopic measurements and modeling and describe water isotopic applications for understanding hydrological processes, this topical review reflects on new insights about climate variability from isotopic studies. We highlight new work and opportunities to enhance our understanding and predictive skill and offer a set of recommendations to advance observational and model-based tools for climate research. Finally, we highlight opportunities to better constrain climate sensitivity and identify anthropogenically-driven hydrologic changes within the inherently noisy background of natural climate variability.

Dee, Sylvia (ORCID:000000022140785X)↗