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At least 307 records · Page 17

The Mineralogy and Petrology of Anomalous Eucrite Emmaville

It has long been known that certain basaltic achondrites share similarities with eucrites. These eucrite-like achondrites have distinct isotopic compositions and petrologic characteristics indicative of formation on a separate parent body from the howardite-eucrite-diogenite (HED) clan (e.g., Ibitira, Northwest Africa (NWA) 011). Others show smaller isotopic variations but are otherwise petrologically and compositionally indistinguishable from basaltic eucrites (e.g., Pasamonte, Pecora Escarpment (PCA) 91007). The Emmaville eucrite has a delta O-17 value of -0.137 plus or minus 0.024 per mille (1 sigma), which is substantially different from the eucrite mean of -0.246 plus or minus 0.014 per mille (2 sigma), but similar to those of A-881394 and Bunburra Rockhole (BR). Currently little data exist for Emmaville in terms of petrology or bulk composition. Studying anomalous eucrites allows us to more completely understand the numbers of asteroids represented by eucrite- like basalts and thus constrain the heterogeneity of the HED suite. In this study, we present our preliminary petrological and mineral composition results for Emmaville.

Barrett, T. J.↗

Metal Organic Frameworks for Noble Gas Isotope Harvesting at FRIB (Final Technical Report)

This project was a collaborative effort between Lawrence Livermore National Laboratory (LLNL) and Michigan State University (MSU) to investigate the use of promising metal organic frameworks (MOFs) for radioactive noble gas capture, with a focus on harvesting exotic radiokryptons from FRIB. After screening several candidate materials, two MOFs were selected for testing: SIFSIX-3Cu and SBMOF-1. Further evaluation showed that although SIFSIX-3Cu has a high selectivity for Kr, SBMOF-1 is less sensitive to the humidity that is present in the FRIB harvesting system and is more readily integrated into the harvesting infrastructure. SBMOF-1 was then evaluated for temperature-dependent Kr and Xe uptake in order to determine the sorption enthalpy. The SBMOF-1 data led to the design of a noble gas capture system that will be fabricated and put into service for isotope harvesting at FRIB as part of a separate project.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

RF deflecting cavity for fast radioactive ion beams

Abstract The Facility for Rare Isotope Beams (FRIB) will be a new scientific user facility that produces rare-isotope beams for experiments from the fragmentation of heavy ions at energies of 100–200 MeV/u. During the projectile fragmentation, the rare isotope of interest is produced along with many contaminants that need to be removed before the beam reaches detectors. At FRIB, this is accomplished with a magnetic projectile fragment separator. However, to achieve higher beam purity, in particular for proton-rich rare isotopes, additional purification is necessary. RadiaBeam in collaboration with Michigan State University (MSU) has designed a 20.125 MHz radiofrequency (RF) fragment separator capable of producing a 4 MV kick with 18 cm aperture in order to remove contaminant isotopes based on their time of flight. In this paper, we will discuss the RF and engineering design considerations of this separator cavity.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Measurements of pressure-induced shifts in the 1-0 and 2-0 bands of HF and in the 2-0 bands of HCl-35 and HCl-37

Fourier absorption spectra of HCl and HF measured at room temperature and low pressures were found to indicate pressure-induced shifts of the spectral lines at gas pressures of only 10 torr. Self-induced shifts were determined for the HF 2-0 band and for the HCl-35 and HCl-37 2-0 bands, and shift oscillations in the 2-0 bands due to near-resonant dipole-dipole interactions between the two gases were also evaluated. Separate measurements of pressure-induced shifts in the HF 1-0 and 2-0 bands and in both isotopic HCl bands were obtained using argon, neon, nitrogen, and CO2 separately as the perturbing gases.

Guelachvili, G.↗

Composition of solar wind noble gases released by surface oxidation of a metal separate from the Weston meteorite

The paper reports on a set of experiments intended to test the feasibility of determining elemental and isotopic ratios of the noble gases and nitrogen in the solar wind in metal separates from gas-rich ordinary chondrites. Helium, neon, and argon show clear evidence of a solar wind signature, while no solar component could be identified for xenon and nitrogen. Helium, neon, and argon elemental isotopic ratios appear to depend on depth within the metal grains. The ratios derived indicate that the Weston meteorite did not acquire its solar wind gases from a recent exposure to solar wind, but more probably at a time in the past similar to or even earlier than the exposure time of Apollo 17 breccias. The Ar-36/Ar-38 ratio, in tandem with other recent determinations of this value, indicates that the solar and terrestrial values can no longer be assumed to be equivalent.

Becker, R. H.↗

Innovative high-temperature ammonium bifluoride fusion and rapid analysis of elements with nuclear forensic value

High-temperature ammonium bifluoride (ABF) fusions were evaluated for potential use in rapid dissolution of post-detonation nuclear debris. The ABF fusion was carried out in a Pt crucible which allowed evaluation of higher fusion and evaporation temperatures. The high-temperature ABF fusion dissolution method was evaluated using geological reference materials: USGS QLO-1a Quartz Latite, USGS SDC-1 Mica Schist, and NIST 278 Obsidian Rock. The optimized dissolution method involved a 10 min fusion at 540 °C, a 5 min reflux in 8 M HNO 3 , an evaporation at 300 °C and final dilution into 45 mL of 2% (v/v) HNO3. The final solution was filtered after heating at 105 °C using a hotblock. This dissolution method was simple, requiring only a hotplate or hotblock, filtered samples were available for ICP-MS analysis or radiochemical separation within 150 min, and was found to have high (>90%) recovery for many isotopes of interest in nuclear forensics applications. U and Pu in the dissolved material was separated using TEVA and UTEVA extraction chromatography columns, a process which resulted in >90% recovery. An irradiated U tracer was spiked into the material prior to dissolution and analyzed for recovery of major fission products and 239Np. The monitored radionuclides had recoveries of greater than 90%, except for the volatile radioiodine isotopes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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↗

Progress towards the FRIB-EDM 3 -Frontend: A tool to provide radioactive molecules from isotope harvesting for fundamental symmetry studies

The under-construction FRIB-EDM 3 -instrument was designed to study polar radioactive molecules (such as RaF) in transparent cryogenic solids by laser spectroscopy. The instrument is divided into a frontend- and a backend section. The frontend accepts an aqueous sample from isotope harvesting and provides a mass-separated molecular ion beam in an ultra-high vacuum environment. In the backend, the ions are guided into alkali-metal vapor and the resulting neutrals are co-deposited in a solid argon matrix to perform laser spectroscopy. Here, this work addresses the frontend of the instrument. The efficient ionization of harvested radioisotopes from aqueous samples is achieved with a spray-ionization method. Subsequently, the molecular ion beam is analyzed by mass-to-charge ratio by a quadrupole mass filter. To verify the feasibility of the approach, numerical simulations with the COMSOL and SIMION packages have been conducted. While the former was applied to study transport in ion funnels, the latter was used to investigate ion beam transmission through the lower pressure sections. Following promising simulation results, a first experimental setup is under construction.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Actinide in Air (Rn-Progeny Rejected) Alpha Spectroscopy With Tensioned Metastable Fluid Detectors

Here, this article discusses outcome of research for deriving a methodology and apparatus for ascertaining for the presence of ultratrace-level actinides in air from their alpha emission signatures, while remaining blind to the relatively large (1000× higher activity) alpha emissions from Rn-progeny. Apparatus and techniques were developed to collect and characterize alpha-emitting nuclides of Rn-progeny and actinides in air on a polycarbonate 3 μm pore size continuous air monitor (CAM) filter. A wet-chemistry approach was developed and validated for successfully separating the Rn-progeny alpha emitting isotopes of Po-214 and Po-218, while extracting the actinides (U, Pu, Am) in a fluid mixture that is suitable for conduct of alpha spectroscopy with a centrifugally tensioned metastable fluid detector (CTMFD). The resulting α-TMFD technology was compared against the state-of-art “Alpha-Sentry™” Continuous Air Monitor (CAM) system commonly utilized world-wide. Results indicate that the α-TMFD technology can potentially offer complementary and superior performance in multiple performance categories, and ∼18× improvement in the time to detect (e.g., at 0.02 derived air concentration (DAC) within ∼3 h, versus ∼70 h for Alpha-Sentry) for actinides of interest while also remaining ∼100% blind to ∼10 3 × higher Rn-progeny background—with the added potential for offering few keV scale energy resolution without resorting to peak shape fitting, versus ∼300–400 keV for existing CAM systems.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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 ↗

Upper Limit for the 248 Cm( 50 Ti, x n) 298− x Og Reaction Cross Section

After the synthesis of element 113, nihonium (Nh) via the 209 Bi( 70 Zn,n) 278 Nh cold fusion reaction using the RIKEN heavy-ion Linear ACcelerator (RILAC) and the GAs-filled Recoil Ion Separator (GARIS), the search for the heaviest isotopes of oganesson was initiated with GARIS-II by means of the 248 Cm( 50 Ti,xn) 298−x Og fusion evaporation reaction. The optimal bombarding energy for the 50 Ti + 248 Cm reaction was determined from the quasielastic barrier distribution extracted from the excitation function of quasielastic backscattering. Here, this method optimizes the compound nucleus formation. The search for Og was conducted for 39 days on the basis of the experimentally derived 50 Ti beam energy of 227.9(5) MeV at the middle of 248 Cm target. A precise analysis of the dataset based on multiple event search strategies revealed no decay chains with a total dose on 248 Cm target of 4.93 × 10 18 50 Ti projectiles, reaching a sensitivity of 0.27 pb and a 1σ upper cross section limit of 0.50 pb.

Gall, Benoît Jean-Paul [University of Strasbourg (↗

Zirconium, hafnium, and rare earth element partition coefficients for ilmenite and other minerals in high-Ti lunar mare basalts - An experimental study

Partition coefficients were determined for Gd, Lu, Hf and Zr among ilmenite, armalcolite, and synthetic high-Ti mare basaltic melts at temperatures from 1122 deg to 1150 deg, and at oxygen fugacities of IW x 10 exp 0.5, by in situ analysis with an electron microprobe, using samples doped to present concentration levels. Coefficients for Zr were also measured for samples containing 600-1600 ppm Zr using this microprobe. In addition, coefficients were determined for Hf and Zr between chromian ulvospinel and melt, for Hf between pigeonite and melt, and for Lu between olivine and melt by microprobe analysis of samples doped to present levels. Values measured using the microprobe were in agreement with the values measured by analyzing mineral separates from the same run products by isotope dilution. Coefficient values for ilmenite are less than 0.01 for the LREE, are around 0.1 for the HREE, and are several times greater than this for Zr and Hf.

Mckay, G.↗

Cosmic-ray lifetime in the Galaxy - Experimental results and models

The separation of the cosmic-ray Be isotopes achieved by two satellite experiments is discussed. From the measured isotopic ratio between the radioactive Be-10 (half-life = 1,500,000 years) and the stable Be-9, it is deduced that the cosmic rays propagate through matter with an average density of 0.24 = or - 0.07 atoms/ cu cm. The implications of this result for the cosmic-ray age is reviewed in the context of two models of confinement and propagation: the homogeneous model, normally identified with confinement ot the galactic gaseous disk, and a diffusion model in which the cosmic rays extend into a galactic halo. A newly deduced cosmic-ray pathlength distribution, a self-consistent model of solar modulation, and a set of fragmentation cross sections are calculated. It is concluded that in a homogeneous model, the cosmic-ray age is 15 (+7, -4) million years, about a factor longer than early estimates based on the abundances of the light nuclei Li, Be, and B and a nominal interstellar density of 1 atom/ cu cm.

Simpson, J. A.↗

Oxygen isotope fractionation in stratospheric CO2

A new cryogenic collection system has been flown on board a balloon gondola to obtain separate samples of ozone and carbon dioxide without entrapping major atmospheric gases. Precision laboratory isotopic analysis of CO2 samples collected between 26 and 35.5 km show a mass-independent enrichment in both O-17 and O-18 of about 11 per mil above tropospheric values. Ozone enrichment in its heavy isotopes was 9 to 16 percent in O3-50 and 8 to 11 percent in O3-49, respectively (Schueler et al., 1990). A mechanism to explain the isotope enrichment in CO2 has been recently proposed by Yung et al. (1991). The model is based on the isotope exchange between CO2 and O3 via O(1D), resulting in a transfer of the ozone isotope enrichment to carbon dioxide. Predicted enrichment and measured values agree well.

Thiemens, M. H.↗

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↗

Identification of Presolar Spinel Grains from a Murray Residue by Multi-Detection Raster Imaging

Grain size separate CG from the Murray CM2 carbonaceous chondrite contains mostly spinel grains of average diameter 0.5 m. Zinner et al. found that approximately 1% of these spinel grains are of presolar origin as determined by their large O isotopic anomalies. These O isotopic measurements were made with the NanoSIMS on individual grains that were well separated from one another on a gold foil. The grains were selected for analysis from secondary electron and secondary O-16(-) images. The primary beam was then successively deflected onto these single grains for O isotopic analysis. While single grain analysis on dispersed samples is effective for finding relatively abundant anomalous grains, ion imaging in a raster mode on tightly packed grains might be more efficient for locating few anomalous grains among predominantly isotopically normal grains. In fact, this was the analysis mode used by Messenger et al. to discover presolar silicates in interplanetary dust particles. In an exploratory effort that is also geared toward establishing the optimum isotopic imaging technique in the search for presolar silicate grains in primitive meteorites, we measured O isotopic ratios in spinel grains from the Murray CG separate by raster imaging of areas with more or less tightly packed grains.

Nguyen, A.↗

Cadmium isotope systematics in sedimentary carbonate: Extending the utility of the cadmium isotope palaeo-productivity proxy

The cadmium (Cd) isotope compositions of seven Holocene (<11.7 ka) carbonate sediments, including the bulk carbonate, as well as the > 140 μm (zooplankton), <63 μm and < 20 μm (phytoplankton) fractions, and individual species of foraminifera isolated from the bulk carbonate were obtained for sub-samples processed using the Cd-cleaning and Mg/Ca cleaning methods. The respective Cd isotope systematics of each carbonate archive were then compared with the Cd isotope signature within the ocean using modern seawater data. We show that a constant Cd isotope fractionation factor of -0.25 ± 0.03 ‰ (2SE, n = 4) describes the partitioning of Cd from seawater into the carbonate phase ($Δ^{114}Cd_{CdC O_3 - seawater}$), allowing for accurate reconstructions of the past seawater nutrient regime. The Cd isotope signature of the < 63 µm and < 20 µm (phytoplankton) fractions can display comparable values to those recorded in the modern surface ocean, and can be used to model the magnitude of Cd uptake and utilisation in the past ocean. Individual species of planktic and benthic foraminifera, which inhabit different depths of the water column, can provide a full surface to deep water column reconstruction of the Cd nutrient regime, while infaunal benthic foraminifera can be used to interrogate the Cd isotope systematics of sediment porewaters. Bulk sediment and the > 140 µm (zooplankton) fraction also retain important information relating to the overlying water column Cd isotope systematics and can serve as essential archives for palaeo-productivity reconstructions where the separation of individual components from the bulk sediment is not possible. This new Cd isotope palaeo-productivity toolkit can considerably aid reconstruction efforts and vastly improves the ability to quantify the role of phytoplankton in modulating carbon sequestration through transitions in Earth’s climate evolution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NanoSIMS Determination of Carbon and Oxygen Isotopic Compositions of Presolar Graphites from the Murchison Meteorite

Graphite from the Murchison density separate KFC1 (2.15 - 2.20 g/cu cm) has previously been studied by combined SEM/EDX and ion microprobe analysis. These studies found several distinct morphological types of graphites and C isotopic compositions that vary over more than 3 orders of magnitude, clearly establishing their presolar origin. Subsequent TEM measurements of a subset of these particles found abundant embedded crystals of metal (Zr, Mo, Ti, Ru) carbides which were incorporated during the growth of the graphites. A new TEM study of a large set of KFC1 graphites led to the discovery of another type of presolar material, Ru-Fe metal. Here we report results of the C and O isotopic measurements in the same graphite sections, which makes it possible for the first time to directly correlate isotopic and TEM data of KFC1 grains.

Stadermann, F. J.↗