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At least 559 records · Page 31

r-Process Radioisotopes from Near-Earth Supernovae and Kilonovae

The astrophysical sites where r-process elements are synthesized remain mysterious: it is clear that neutron star mergers (kilonovae (KNe)) contribute, and some classes of core-collapse supernovae (SNe) are also possible sources of at least the lighter r-process species. The discovery of 60Fe on the Earth and Moon implies that one or more astrophysical explosions have occurred near the Earth within the last few million years, probably SNe. Intriguingly, 244 Pu has now been detected, mostly overlapping with 60 Fe pulses. However, the 244 Pu flux may extend to before 12 Myr ago, pointing to a different origin. Here, motivated by these observations and difficulties for r-process nucleosynthesis in SN models, we propose that ejecta from a KN enriched the giant molecular cloud that gave rise to the Local Bubble, where the Sun resides. Accelerator mass spectrometry (AMS) measurements of 244 Pu and searches for other live isotopes could probe the origins of the r-process and the history of the solar neighborhood, including triggers for mass extinctions, e.g., that at the end of the Devonian epoch, motivating the calculations of the abundances of live r-process radioisotopes produced in SNe and KNe that we present here. Given the presence of 244 Pu, other r-process species such as 93 Zr, 107 Pd, 129 I, 135 Cs, 182 Hf, 236 U, 237 Np, and 247 Cm should be present. Their abundances and well-resolved time histories could distinguish between the SN and KN scenarios, and we discuss prospects for their detection in deep-ocean deposits and the lunar regolith. We show that AMS 129 I measurements in Fe–Mn crusts already constrain a possible nearby KN scenario.

79 ASTRONOMY AND ASTROPHYSICS↗

Status of the RRR evaluations for 233,235 U and 239 Pu [Slides]

The presentation discusses the R -Matrix Analysis of 233 U, 235 U, and 239 Pu and how their interplay among PFNS, TNC, RRR, and neutron multiplicities has a significant impact on benchmarks. The presentation also discusses the 233 U improved agreement on benchmarks, an additional investigation on the thickness of beryllium reflectors, work on URR (up to 40 keV) and/or extension of RRR (600 eV to 2 keV). Also discussed is how the 235 U progresses on understanding reactivity rates related to depletion calculations, improved agreement with measured (capture) data is quite insensitive to resolve the negative slope, and how the 239 Pu negative slope as a function of the temperature is not understood yet (bias over 2σ lower than measured).

07 ISOTOPE AND RADIATION SOURCES↗

Record of fluid-rock interactions on Mars from the meteorite ALH84001

Allan Hills (ALH) 84001 is the most recently recognized member of a suite of meteorites--the SNCs--that almost certainly originated on Mars. Several factors distinguish ALH84001 from the other SNC meteorites. Preliminary studies suggest that it may be older than other martian meteorites. Moreover, it contains abundant, zoned domains of calcium-iron-magnesium carbonate that are indigenous to the sample and thus may hold important clues regarding near-surface processes on Mars and the evolution of the martian atmosphere. We report here analyses of the carbon and oxygen stable-isotope compositions of the carbonates that place constraints on their formation conditions. Our results imply the presence of at least two chemically distinct carbonates--one Ca,Fe-rich, the other Mg-rich--that are enriched in 13C relative to terrestrial carbonates (delta 13C approximately +41/1000), consistent with martian atmospheric CO2 as the carbon source. The oxygen isotope compositions of the carbonates indicate that they precipitated from a low-temperature fluid in the martian crust. Combined with textural and bulk geochemical considerations, the isotope data suggest that carbonate deposition took place in an open-system environment in which the ambient temperature fluctuated.

Carbonates/analysis↗

Enhanced sensitivity for electron affinity measurements of rare elements

The electron affinity (EA), the energy released when a neutral atom binds an additional electron, is a fundamental property of atoms that is governed by electron-electron correlations and is strongly related to an element’s chemical reactivity. However, conventional techniques for EA determination lack the experimental sensitivity to probe very scarce samples. As a result, the EA for the heaviest elements of the periodic table is entirely uncharted. Here, we present a novel technique to determine EAs through Laser Photodetachment Threshold Spectroscopy, performed in an electrostatic ion beam trap to increase the samples’ exposure to laser photons and, thus, improve the experimental signal sensitivity by three orders of magnitude. Moreover, the additional exposure time allows the use of lower-power continuous-wave narrow-band lasers that reduce uncertainties associated with broadening effects induced by the laser bandwidth. By applying this technique, we measure the EA of 35 Cl to be 3.612720(44) eV, achieving state-of-the-art precision while employing five orders of magnitude fewer anions. The demonstrated sensitivity paves the way for systematic EA measurements across isotopic chains - including isotope shifts and hyperfine splittings - and ultimately for the first direct determination of electron affinities in superheavy elements.

Maier, F. M. [Univ. of Greifswald (Germany); Europ↗

High Flux Isotope Reactor Low-Enriched Uranium High Density Silicide Fuel Preliminary Design Update: System Transient Analysis

As a part of conversion efforts from highly enriched uranium (HEU) to low-enriched uranium (LEU) fuel under direction of the National Nuclear Security Administration of the U.S. Department of Energy, multiple proposed designs of the High Flux Isotope Reactor (HFIR) have been created and assessed regarding reactor physics performance metrics, including designs utilizing uranium silicide dispersion fuel (U3Si2-Al). This report updates the previous analyses that evaluated the nuclear safety performance of LEU fuel designs with respect to selected accident events from the HFIR Safety Analysis Report (SAR). Both the Low Density (LD) and High Density (HD) Optimized designs’ reactivity initiated accident fuel performance improved relative to the HEU fuel, attributed to greater 238 U negative Doppler feedback. However, the thermal margins for primary coolant system accidents were reduced with some acceptance criteria unable to be met. The need to resolve reduced thermal margin, open modeling items, and unresolved assumptions was identified.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fuel Fabrication Specification Impact Analysis for NBSR LEU Conversion

As part of a national initiative to enhance nuclear security and reduce proliferation risks, significant efforts have been undertaken by the National Nuclear Security Administration Material Management and Minimization Office of Reactor Conversion Program to convert U.S. high performance research reactors (USHPRRs) from the use of highly enriched uranium (HEU) to low-enriched uranium (LEU), including the National Bureau of Standards Reactor (NBSR). The current plan is to procure LEU fuel assemblies from commercial fabricators according to fuel specifications tailored for each USHPRR. The analysis conducted at Brookhaven National Laboratory was part of an effort to identify the sources of uncertainty in the fuel specifications that may impact the performance of the NBSR core after its conversion and, in particular, to assess the range of acceptable tolerance limits from the perspective of core safety and reactor performance. Using the stochastic neutronics code MCNP 6.2, the variations in important NBSR neutronics characteristics were analyzed as a function of the specification parameters independently and in combination. The important NBSR specification parameters analyzed were the fuel isotopic composition, the amount of impurity content in cladding, the fuel plate thickness, and the fuel element 235U mass loading. The range of variation of each specification parameter was based on the technical specification limit or available as-fabricated assay data and uncertainties. The NBSR neutronics characteristics selected for analysis were the reactor reactivity characteristics at equilibrium and the equilibrium fuel cycle length. Results show that with variations in the fabrication parameters of the as-fabricated U-10Mo fuel within the specification limitations, the excess reactivity of the NBSR LEU core remains well below the 15% Δk/k technical specification limit, and the shutdown margin is always significantly greater than the required 0.68% Δk/k. This ensures that the NBSR can be operated safely and reliably shut down for all analyzed cases within the specified fabrication limits after the LEU conversion. In the prototypic case, the fuel cycle length was 1.5 days longer than the targeted 38.5 days. In a credible worst-case scenario, where all low-reactivity parameters were combined, the fuel cycle length was reduced to 35.5 days, which is still considered manageable for reactor operations. Variations in cycle length are primarily driven by changes in 235U loading, with other parameters having secondary effects.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurable radiation levels around individuals externally contaminated by nuclear fallout

During the early response to large-scale radioactive contamination events, people who are potentially affected need to be screened for radioactive contamination and public health staff need to triage individuals who may need immediate decontamination. This is typically done by screening individuals for external contamination using ionising radiation detection equipment. In this study, spatially and temporally dependent isotopic compositions from a simulated nuclear detonation and Monte Carlo methods were used to relate contamination activity levels to the measurable radiation levels at select distances away from an individual with whole-body contamination. Radionuclide-specific air kerma rate coefficients and Geiger–Mueller instrument response coefficients at five select distances from contaminated individuals are presented for 662 radionuclides. Temporally and spatially dependent incident-specific coefficients are presented for a hypothetical surface detonation of a 235 U-fueled device.

61 RADIATION PROTECTION AND DOSIMETRY↗

Lunar Science Conference, 5th, Houston, Tex., March 18-22, 1974, Proceedings. Volume 1 - Mineralogy and petrology. Volume 2 Chemical and isotope analyses. Organic chemistry. Volume 3 - Physical properties

Numerous studies on the properties of the moon based on Apollo findings and samples are presented. Topics treated include ages of the lunar nearside light plains and maria, orange material in the Sulpicius Gallus formation at the southwestern edge of Mare Serenitatis, impact-induced fractionation in the lunar highlands, igneous rocks from Apollo 16 rake samples, experimental liquid line of descent and liquid immiscibility for basalt 70017, ion microprobe mass analysis of plagioclase from 'non-mare' lunar samples, grain size and the evolution of lunar soils, chemical composition of rocks and soils at Taurus-Littrow, the geochemical evolution of the moon, U-Th-Pb systematics of some Apollo 17 lunar samples and implications for a lunar basin excavation chronology, volatile-element systematics and green glass in Apollo 15 lunar soils, solar wind nitrogen and indigenous nitrogen in Apollo 17 lunar samples, lunar trapped xenon, solar flare and lunar surface process characterization at the Apollo 17 site, and the permanent and induced magnetic dipole moment of the moon. Individual items are announced in this issue.

Gose, W. A.↗

Microfossils in cherts from the Mesoproterozoic (Middle Riphean) Debengda Formation, the Olenek Uplift, northeastern Siberia

Silicified shallow-water marine carbonate deposits of the Proterozoic Debengda Formation (the Olenek Uplift, northeastern Siberia) contain well preserved microfossils. One or two distinct assemblages consists only of filamentous Siphonophycus microfossils, which are presumably the extracellular sheaths of hormogonium cyanobacteria. The other is dominated by coccoidal microfossils, first by the entophysalidacean cyanobacterium Eoentophysalis. The coccoidal assemblage was recognized in the layered carbonate precipitate structures of a superficially stromatolite appearance. Despite its simple composition, the microfossil assemblage supports the generally accepted Mesoproterozoic (middle Riphean) age of the Debengda Formation. This conclusion corresponds to the available data on isotopic geochronology, and to the composition of columnar stromatolites from the Dehengda Formation. Both the structural features and carbon isotopic composition of its rocks are comparable to those of rocks of known Mesoproterozoic age, but differ from the characteristics of definitely Neoproterozoic deposits.

Non-NASA Center↗

Biomineralization: Integrating mechanism and evolutionary history

Calcium carbonate (CaCO 3 ) biomineralizing organisms have played major roles in the history of life and the global carbon cycle during the past 541 Ma. Both marine diversification and mass extinctions reflect physiological responses to environmental changes through time. An integrated understanding of carbonate biomineralization is necessary to illuminate this evolutionary record and to understand how modern organisms will respond to 21st century global change. Biomineralization evolved independently but convergently across phyla, suggesting a unity of mechanism that transcends biological differences. In this review, we combine CaCO 3 skeleton formation mechanisms with constraints from evolutionary history, omics, and a meta-analysis of isotopic data to develop a plausible model for CaCO 3 biomineralization applicable to all phyla. The model provides a framework for understanding the environmental sensitivity of marine calcifiers, past mass extinctions, and resilience in 21st century acidifying oceans. Thus, it frames questions about the past, present, and future of CaCO 3 biomineralizing organisms.

60 APPLIED LIFE SCIENCES↗

Status of the RRR evaluations for 233,235 U and 239 Pu [Slides]

The presentation discusses the R -Matrix Analysis of 233 U, 235 U, and 239 Pu and how their interplay among PFNS, TNC, RRR, and neutron multiplicities has a significant impact on the benchmarks. The presentation also discusses the 233 U improved agreement on benchmarks, an additional investigation on the thickness of beryllium reflectors, work on URR (up to 40 keV) and/or extension of RRR (600 eV to 2 keV). Also discussed is how the 235 U progresses on understanding reactivity rates related to depletion calculations, improved agreement with measured (capture) data is quite insensitive to resolve the negative slope, and how the 239 Pu negative slope as a function of the temperature is not understood yet (bias over 2σ lower than measured).

07 ISOTOPE AND RADIATION SOURCES↗

An Automated Ultraclean Ion Exchange Separation Method for the Determinations of 232Th and 238U in Copper using Inductively Coupled Plasma Mass Spectrometry

This work presents a novel automated analytical method developed for high throughput ultrasensitive determinations of Th and U in copper using inductively coupled plasma mass spectrometry (ICP-MS). The method is based on the use of ultra clean sample preparation procedures including the use of a fully automated off-line chromatography system for the extraction and pre-concentration of the analytes prior to ICP-MS analysis. The separation system is equipped with a single reusable chromatographic column that, with the rigorously clean procedures developed herein, provided a low carryover, low background, and reproducible automated separation method. Isotope dilution methods were used for quantitation. Method Detection Limits (MDLs) of 3.7 and 9.4 fg·g-1 were obtained for the quantitation of 232Th and 238U in copper, respectively, corresponding to activities of 0.0148 and 0.116 microBq·kg-1 for 232Th and 238U, respectively. The analytical method provided high and reproducible tracer recoveries. The use of an automated system significantly reduced the extremely tedious active work time required for the chemist (by ca. 80%) relative to manually performing the separation. This method could be adapted to other critical sample matrices requiring the utmost in high throughput clean chemistry procedures for automated ultrasensitive analyses.

Arnquist, Isaac J.↗

Temperature Dependence of Nuclear Quadrupole Resonance and the Observation of Metal–Ligand Covalency in Actinide Complexes: 35 Cl in Cs 2 UO 2 Cl 4

We report a study of the temperature dependence of 35 Cl nuclear quadrupole resonance (NQR) transition energies and spin–lattice relaxation times (T 1 ) for 235 U-depleted dicesium uranyl tetrachloride (Cs 2 UO 2 Cl 4 ) aimed at elucidating electronic interactions between the uranium center and atoms in the equatorial plane of the UO 2 2+ ion. The transition frequency decreases slowly with temperature below 75 K and with a more rapid linear dependence above this temperature. The spin–lattice relaxation time becomes shorter with temperature, and as temperatures increase, the T 1 decrease becomes nearly quadratic. The observed trends are reproduced by a model that assumes phonon-induced fluctuations of the electric field gradient tensor and partial electron delocalization from Cl to U. The fit of the theoretical model to experimental data allows a Debye temperature of 96 K to be estimated. Finally, the generalization of this approach to investigations of covalency in actinide–ligand bonding is examined.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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.↗

Experimental studies of the two-step scheme with an intense radioactive 132 Sn beam for next-generation production of very neutron-rich nuclei

The study of nuclei in the yet-unexplored, very neutron-rich, mid- to heavy-mass region of the nuclear chart, comprising perhaps half of all nuclei predicted to exist, is leading to new and/or upgraded facilities, as well as to research into the underlying production processes. In the present study, the usefulness of the two-step scheme, an alternate method to produce very neutron-rich nuclei, by a combination of an isotope-separation online (ISOL) system as a first step, and in-beam fragmentation of re-accelerated radioactive isotopes (RIs) as a second step, was investigated with a 132 Sn beam. In this work, very neutron-rich RIs around the neutron-rich neutron number N = 82 region were produced from the 278-MeV/nucleon 132 Sn beam impinging on a 5.97-mm Be target, and their production cross sections were measured. Yields were then estimated for the two-step scheme with the 132 Sn beam relative to the ones by a one-step scheme, in-flight fission of a 238 U beam, for 1-MW proton and 238 U beams at respective RI-beam facilities. This comparison suggests that the two-step scheme with the 132 Sn beam provides yields >40-times higher than those with the one-step scheme for the very neutron-rich N = 82 region. Moreover, by using various RI beams over the nuclear chart from ISOL, certain kinds of very neutron-rich RIs around the supernova r-process path can be produced with greater yields than by the one-step approach.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Ground-state and decay properties of neutron-rich 106 Nb

The ground-state properties of neutron-rich 106 Nb and its β decay into 106 Mo have been studied using the CARIBU radioactive-ion-beam facility at Argonne National Laboratory. Niobium-106 ions were extracted from a 252 Cf fission source and mass separated before being delivered as low-energy beams to the Canadian Penning Trap, as well as the X-Array and SATURN β-decay-spectroscopy station. The measured 106 Nb ground-state mass excess of –66202.0(13) keV is consistent with a recent measurement but has three times better precision; this work also rules out the existence of a second long-lived, β-decaying state in 106 Nb above 5 keV in excitation energy. The decay half-life of 106 Nb was measured to be 1.097(21) s, which is 8% longer than the adopted value. Here, the level scheme of the decay progeny, 106 Mo, has been expanded up to ≈ 4 MeV. The distribution of decay strength and considerable population of excited states in 106 Mo of J ≥ 3 emphasizes the need to revise the adopted J π = 1 – ground-state spin-parity assignment of 106 Nb; it is more likely to be J ≥ 3.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Mars Volatiles and Climate Surveyor (MVACS) Integrated Payload for the Mars Polar Lander Mission

The Mars Volatiles and Climate Surveyor (MVACS) integrated payload for the Mars Polar Lander will be launched in January 1999, with a scheduled landing on Mars' south-polar layered deposits in December 1999. Over the course of its 90-day nominal mission during the martian southern spring and summer seasons, it will make in situ measurements that will provide new insights into the behavior and distribution of martian volatiles, MVACS consists of four major instrument systems: a surface stereo imager (SSI), which will acquire multispectral stereo images of the surface and atmosphere; a 2-m robotic arm (RA), which will dig a O.5-m deep trench and acquire surface and subsurface samples that will be imaged by a focusable robotic arm camera (RAC), which will take close-up images of surface and subsurface samples at a spatial resolution of 21 micron; a meteorology package (MET), which will make the first measurements of surface pressure, temperature, and winds in Mars' southern hemisphere and employ a tunable diode laser (TDL) spectrometer to measure the water-vapor concentration and isotopic composition of CO2 in the martian atmosphere; and a thermal and evolved gas analyzer (TEGA), which will use differential scanning calorimetry and TDL-evolved gas analysis to determine the concentrations of ices, adsorbed volatiles, and volatile-bearing minerals in surface and subsurface soil samples. The unique in situ measurements made by MVACS at its high-latitude landing site will define a number of important aspects of the physical, isotopic, and chemical nature of the martian near-surface and subsurface environment that will be valuable in better understanding Mars meteorites and returned samples, as well as in the search for martian resources that could be utilized by humans.

Paige, D. A.↗

Isotopic, Chemical and Mineralogical Investigations of Extraterrestrial Materials

The principal aim of our work was to improve our understanding of the earliest evolutionary period of our solar system (i.e. the first tens of millions of years). We have studied its chronology by using short and long term chronometers (based on extinct and long lived radioactive nuclei), explored the bearing of short lived nuclei on planetary heating and differentiation, and the addition of 'exotic' nuclei to solar system matter to help constrain models of nucleosynthesis. Our basic tool is high precision Thermal Ionization Mass Spectrometry (TIMS). Over the years we have developed clean chemical separation procedures for many elements. The chemical elements most relevant to our investigations are Cr, Ni, Rb, Sr, Sm, Nd, Pb, and U, for which highly efficient measurement techniques by TIMS have been developed and have been in use in our laboratory for many years. We have explored the Mn-53 Cr-53 system (T (Mn-53) = 3.7 Ma) and have found it to be a powerful tool to obtain relative ages of meteorite formation and, more general, of early solar system processes with a time resolution of approx. 1 Ma. By measuring the Mn-Cr system in many meteorite types (chondrites, basaltic achondrites, angrites, pallasites, etc.) we have found that this condition is indeed met for most meteorite families.

Lugmair, Guenter W.↗