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At least 433 records · Page 24

Volatile element depletion and K-39/K-41 fractionation in lunar soils

Evidence for selective loss and isotopic fractionation (in the case of K) of volatile elements during formation of agglutinates by micrometeoritic bombardment of lunar soils is presented. Concentrations and isotopic compositions of volatile elements (K, Rb, Pb) and nonvolatile elements (U, Th, Ba, Sr, rare earths) in separates taken from soils 14163, 14259, 15041, 68501, and 71500 are examined. Rayleigh fractionation calculations applied to K-39/K-41 isotopic data indicate ten-fold recycling of bulk soil, to account for observed isotopic anomalies. The lunar soil fines fraction seems to be a site of deposition for volatile or labile Pb produced during agglutination. Local fines (below 75 microns) are viewed as representative of the parent material for agglutinates formed in situ by micrometeoritic impact. Magnetic separation of agglutinates from soil 68501 revealed a bimodal population, with one class comprising welded blocky magnetic glasses.

Church, S. E.↗

Evidence for ground-state electron capture of K 40

Potassium-40 is a widespread, naturally occurring isotope whose radioactivity impacts estimated geological ages spanning billions of years, nuclear structure theory, and subatomic rare-event searches—including those for dark matter and neutrinoless double-beta decay. The decays of this long-lived isotope must be precisely known for its use as a geochronometer, and to account for its presence in low-background experiments. There are several known decay modes for potassium-40, but a predicted electron-capture decay directly to the ground state of argon-40 has never been observed. The existence of this decay mode impacts several fields, while theoretical predictions span an order of magnitude. Here we report on the first, successful observation of this rare decay mode, obtained by the KDK (potassium decay) Collaboration using a novel combination of a low-threshold x-ray detector surrounded by a tonne-scale, high-efficiency γ -ray tagger at Oak Ridge National Laboratory. A blinded analysis reveals a distinctly nonzero ratio of intensities of ground-state electron-captures ( I EC 0 ) over excited-state ones ( I EC * ) of I EC 0 / I EC * = 0.0095 ± stat 0.0022 ± sys 0.0010 (68% CL), with the null hypothesis rejected at 4 σ [Stukel et al. , Phys. Rev. Lett. 131 , 052503 (2023) ]. In terms of branching ratio, this unambiguous signal yields I EC 0 = 0.098 % ± stat 0.023 % ± sys 0.010 % , roughly half of the commonly used prediction. This first observation of a third-forbidden unique electron capture improves our understanding of low-energy backgrounds in dark-matter searches and has implications for nuclear-structure calculations. For example, a shell-model based theoretical estimate for the neutrinoless double-beta decay half-life of calcium-48 is increased by a factor of 7 - 2 + 3 . Our nonzero measurement shifts geochronological ages by up to a percent; implications are illustrated for Earth and solar system chronologies.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NdPO 4 solubility and aqueous Neodymium speciation in supercritical fluids: An experimental study at 500–700 °C and 1.7 kbar

A key aspect in the formation of rare earth elements (REE) deposits is the role of REE transport as aqueous REE complexes in supercritical hydrothermal solutions, where the nature of the aqueous complex is controlled by solution composition, temperature and pressure. Despite chloride being considered as one of the most abundant transporting ligands in magmatic-hydrothermal fluids, experimental investigations on the stability of aqueous REE chloride complexes are scarce above 300 °C. In this study, synthetic NdPO 4 crystals were reacted with non-saline and saline (0, 0.05 and 0.5 mNaCl), acidic (0.01 mHCl) aqueous solutions in a series of solubility experiments conducted at 500–700 °C and 1.7 kbar, where the solubilities were determined using a stable Nd isotope ( 145 Nd isotope spike) dilution technique. NdPO 4 solubility ranges between 28 ppm and 10,858 ppm, where solubility increases with both temperature and salinity. At 500 °C, log mNdPO 4 increases from –3.93 to –1.60 and there is a strong correlation between NdPO 4 solubility and NaCl concentrations (slope of 1.2 ± 0.3), indicating stabilization of the Nd chloride aqueous complexes with a stoichiometry corresponding to NdCl 2+ . At 600 °C, this correlation is weaker (slope of 0.4, log mNdPO 4 increases from –2.63 to –1.88) indicating the stabilization of both Nd chloride and hydroxyl species controlling solubility. At 700 °C, NdPO 4 solubility is largely independent of NaCl concentration indicating that solubility is controlled by Nd hydroxyl complexes, where stoichiometry suggests the neutral Nd(OH) 3 0 species is dominant. The solubility product (Ksp) of NdPO4 is derived from experimental data with the relation: log K sp = -41.81 – 0.057T – 20987/T, with T temperature in Kelvin. Comparison of the measured Nd phosphate solubility to thermodynamic predictions using the available Helgeson-Kirkham-Flowers equation of state parameters for aqueous Nd complexes indicate that predictions are up to three orders of magnitude lower compared to experimental observations. This discrepancy is most pronounced in saline solutions, suggesting that thermodynamic properties of the REE chloride species in supercritical fluids require revision. Numerical simulations of fluid-rock interaction between acidic, saline fluids and a Strange Lake felsic mineral assemblage demonstrates that NdPO 4 solubility predictions from models are four to six orders of magnitude lower than those calculated based on empirical fits from experiments, which suggests that acidic, saline fluids may play an important role in mobilizing large amounts of light REE from 450 to 700 °C.

58 GEOSCIENCES↗

Development of Chemical Procedures for Isotope Harvesting: Separation of Trace Hafnium from Tungsten

The separation of trace hafnium from bulk tungsten alloys is of interest for isotope harvesting at the National Superconducting Cyclotron Laboratory and the Facility for Rare Ion Beams because 172 Hf, the parent of 172 Lu, accumulates in tungsten alloy beam blockers at these facilities. In this work, a procedure for the separation of trace hafnium from a bulk tungsten alloy (454 g) was established using tracer isotopes ( 175 Hf, 88 Zr, 173 Lu, and 88 Y). Here, the procedure employed dissolution in an HF–HNO 3 solution followed by a calcium fluoride precipitation, and then extraction chromatography was used for more selective separation steps. Two stages of column separations using LN resin (HDEHP based) and TRU resin (CMPO based) were performed. Gamma-ray spectroscopy and mass spectrometry were used to analyze the final hafnium sample and follow the steps in the chemical processing. Furthermore, the final recovery of hafnium was high (90 ± 8)%, and the mass of tungsten and other transition metals was reduced to near background levels (as determined by ICP-MS of the blank acid solutions). Zirconium follows hafnium quantitatively in this procedure; there was no detectable 173 Lu in the final hafnium sample.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Evidence for extreme mantle fractionation in early Archaean ultramafic rocks from northern Labrador

Samarium-neodymium isotope data for tectonically interleaved fragments of lithospheric mantle and meta-komatiite from the North Atlantic craton provide the first direct record of mantle differentiation before 3,800 Myr ago. The results confirm the magnitude of light-rare-earth-element depletion in the early mantle, and also its depleted neodymium isotope composition. The mantle fragments were able to retain these ancient geochemical signatures by virtue of having been tectonically incorporated in buoyant felsic crust, thus escaping recycling and homogenization by mantle convection.

Collerson, Kenneth D.↗

Enantiomeric and Isotopic Analysis of Sugar Derivatives in Carbonaceous Meteorites

Several classes of organic compounds are found in carbonaceous meteorites including amino acids, carboxylic acids, hydroxy acids, purines, and pyrimidines. Such compounds are thought to have been delivered to the early Earth in asteroids and comets and may have played a role in the origin of life. Likewise, sugar derivatives are critical to all known lifeforms. Recent analyses of the Murchison and Murray carbonaceous meteorites revealed a diverse suite of such derivatives, i.e., sugar alcohols, and sugar acids. This presentation will focus primarily on the analysis of individual sugar acids - their enantiomeric and isotopic composition. Analysis of these compounds may reveal the nature of past (or present) meteoritic sugars themselves. For example, if parent sugars decomposed (by well-known mechanisms) to give the present acids, were their enantiomeric ratios preserved? Combined with other evidence, the enantiomeric composition of such compounds as glyceric acid and (especially) rare acids may help to answer such questions. C-13 and D isotope analysis of meteoritic sugar alcohols (glycerol, threitol, ribitol, etc.) as a group revealed that they were indigenous to the meteorite. Preliminary C-13 analysis of glyceric acid shows that it is also extraterrestrial.

Cooper, George↗

Chemistry of the thermal water samples of the Camas Prairie area in Idaho, USA

This dataset includes chemistry of geothermal water samples of the Camas Prairie area in Idaho. The samples included in this dataset were collected over the period of 2016-2019. Collection/analysis of new water samples and compilation of existing water chemistry database were conducted for Snake River Play Fairway Project. All chemical analysis of the samples were conducted in the Analytical Laboratory at the Center of Advanced Energy Studies (unless otherwise indicated) in Idaho Falls, Idaho. Isotope analysis were conducted in analytical/isotope measurement labs at Lawrence Berkeley National Laboratory, Utah State University, and University of Utah.

15 GEOTHERMAL ENERGY↗

Sm-Nd Isotopic Studies of Ureilite Novo Urei

Ureilites are ultramafic (harzburgitic) achondrites composed predominantly of olivine and pyroxenes, abundant carbon (graphites and shock-produced diamonds), some metal and sulfides. These rocks probably represent ultramafic mantles of differentiated parent asteroidal bodies. Age determinations of these rocks by Rb-Sr and Sm-Nd methods have been difficult because of their extremely low abundances of these parent-daughter elements. Nevertheless, Sm-Nd isochron ages were reported for Kenna, Goalpara, MET 78008 and PCA 82506 yielding ages of 3.74+/-0.02 Ga, approx.3.7 Ga, 4.09+/-0.08 Ga, 4.23+/-0.06 Ga, respectively [1-4]. These "young" Sm-Nd ages may represent secondary metasomatism events [1] related to impacts [5], as indicated by the similarly young Ar-39-Ar-40 degassing ages of 3.3-4.1 Ga for ureilites Kenna, Novo Urei and Havero [6]. Alternatively, it has been suggested that these rocks may have been contaminated with terrestrial crustal materials and the isochrons do not have any age significance [2,7]. Indications of old approx.4.56 Ga ages for ureilites were reported from the U-Pb and Sm-Nd model ages for MET 78008 [8]. More reliable evidences for old formation ages of ureilites were reported recently using the short-lived chronometers Hf-182-W-182, Al-26-Mg-26 and Mn-53-Cr-53. The deficits of 182W in ureilites suggest the metal-silicate segregation occurred very early, approx.1-2 Ma after CAI [9]. The Al-26-Mg-26 and Mn-53-Cr-53 studies for a feldspathic lithology [10] and the Mn-53-Cr-53 for olivine- and pyroxene-dominant lithologies [11] in ureilites revealed that they crystallized approx.5.4 Ma after CAI, i.e., at 4563.8+/-0.5 Ma relative to D.Orbigny. In this report, we present Sm-Nd isotopic data for a relatively fresh ureilite, Novo Urei, a rare ureilite fall (1886). We compare these data to Sm-Nd data for other ureilites, and discuss Novo Urei's petrogenesis

Shih, C.-Y.↗

On Infrared Excesses Associated with Li-Rich K Giants

Infrared (IR) excesses around K-type red giants (RGs) have previously been discovered using Infrared Astronomy Satellite (IRAS) data, and past studies have suggested a link between RGs with overabundant lithium and IR excesses, implying the ejection of circumstellar shells or disks. We revisit the question of IR excesses around RGs using higher spatial resolution IR data, primarily from the Wide-field Infrared Survey Explorer. Our goal was to elucidate the link between three unusual RG properties: fast rotation, enriched lithium, and IR excess. Our sample of RGs includes those with previous IR detections, a sample with well-defined rotation and lithium abundance measurements with no previous IR measurements, and a large sample of RGs asserted to be lithium-rich in the literature; we have 316 targets thought to be K giants, about 40% of which we take to be Li-rich. In 24 cases with previous detections of IR excess at low spatial resolution, we believe that source confusion is playing a role, in that either (a) the source that is bright in the optical is not responsible for the IR flux, or (b) there is more than one source responsible for the IR flux as measured in IRAS. We looked for IR excesses in the remaining sources, identifying 28 that have significant IR excesses by approximately 20 micrometers (with possible excesses for 2 additional sources). There appears to be an intriguing correlation in that the largest IR excesses are all in Li-rich K giants, though very few lithium-rich K giants have IR excesses (large or small). These largest IR excesses also tend to be found in the fastest rotators. There is no correlation of IR excess with the carbon isotopic ratio, 12C/13C. IR excesses by 20 micrometers, though relatively rare, are at least twice as common among our sample of lithium-rich K giants. If dust shell production is a common by-product of Li enrichment mechanisms, these observations suggest that the IR excess stage is very short-lived, which is supported by theoretical calculations. Conversely, the lithium-enrichment mechanism may only occasionally produce dust, and an additional parameter (e.g., rotation) may control whether or not a shell is ejected.

Li-rich↗

Magnesian anorthosites from the western highlands of the Moon: Isotope geochemistry and petrogenesis

Breccias from the Apollo 14 landing site have provided a wealth of information on the genesis of the lunar highlands. Various pristine rock-types have been discovered in relative abundance including rare ferroan anorthosites and alkali-suite and magnesian-suite rocks. Mineral-chemical and radiogenic isotopic data are reported here for a newly discovered Mg-suite anorthosite from Apollo 14, sample 14303,347. Meyer et al. reported U-Pb zircon analyses of Mg-suite highlands rocks from the western limb of the Moon. We have compiled these ages and generated a weighted average age of 4211 = 6 Ma; some 200 Ma younger than ferroan anorthosites. Utilizing this age for Mg-anorthosite 14303,347, our data results in an initial epsilon(sub Nd) value of -1.0 and initial Sr-87/Sr-86 of 0.69915. Based on trace-element, isotopic, and mineral-chemical data, the western highlands Mg-suite is interpreted to be crustal precipitates of a picritic magma, which assimilated KREEPy trapped liquid from upper-mantle cumulates during its transport to the crust.

Snyder, Gregory A.↗

The Sr and Nd isotopic record of Apollo 12 basalts - Implications for lunar geochemical evolution

Alkali, alkaline earth, and rare earth element data are reported for several Apollo 12 basalts which are representative of the four Apollo 12 magma types. Results confirm the heterogeneity of the lunar mantle and show that the Sm/Nd ratio of at least the Apollo 12 ilmenite basalts was decreased by 13-24% during magma genesis. In addition, whole mare basalt Sm-Nd data are not collinear on an isochron diagram; thus it is no longer possible to explain these data via mixing of 'primitive material' and 'early differentiates' as in the hybridization and assimilation models.

Nyquist, L. E.↗

Assessment of rare earth element fractionation in NIF implosions with radiochemically doped capsules

An ongoing experimental campaign at the National Ignition Facility (NIF) aims to measure neutron induced nuclear reaction cross–sections using radiochemically doped target capsules. Critical to this campaign is the ability to collect a representative sample of the reaction products using Solid Radiochemical Collectors (SRCs) fielded around the NIF chamber. The shot presented in this paper used a doped target capsule with a neopentane gas fill was to investigate the ratio of isotopes collected at three chamber angles. It was found that SRC samples of rare earth elements collected from NIF are representative of the ingoing dopant mix, thereby concluding that fractionation does not occur during a NIF implosion. This validates the doped capsule method for use in measuring neutron induced reaction cross-sections.

Capsule Doping↗

Lithium isotopic analysis in depleted lithium salts

Lithium isotope separation processes require characterization of the isotopic compositions of the different output phases of the process. While considerable effort to develop isotope separation methods has been ongoing for decades, the analytical methods associated with these analyses are rarely provided. Here, in this work three types of mass spectrometers (Q-ICP-MS, MC-ICP-MS, TIMS) were tested for the ability to measure depleted lithium salts that are relevant materials for isotopic separations. Results indicate that, once stabilized, the Q-ICP-MS can provide equal precision for Li isotopic samples compared to TIMS or MC-ICP-MS. However, MC-ICP-MS consistently provides the highest precision for salts across both depleted and natural isotopic abundances. These data demonstrate that Q-ICP-MS is an appropriate choice for analysis of depleted lithium salts, especially when rapid analyses are desired for online process monitoring.

07 ISOTOPE AND RADIATION SOURCES↗

Results of the LEGEND-200 experiment in the search for $0νββ$ decay

The LEGEND experiment is looking for the extremely rare neutrinoless double beta (0νββ) decay of 76 Ge using isotopically-enriched high-purity germanium (HPGe) detectors. The detection of this process would imply that the neutrino is a Majorana particle and the total lepton number would not be conserved, which could be related to the cosmological asymmetry between matter and antimatter through leptogenesis. The long-term goal of the collaboration is LEGEND-1000: a 1-ton detector array planned to run for 10 years, with a projected half-life sensitivity exceeding 10 28 years, fully covering the inverted neutrino mass hierarchy. A first search for the 0νββ decay has been carried out by LEGEND-200 building on the experience gained from GERDA and the MAJORANA DEMONSTRATOR. The experiment has been collecting physics data for a year at the Gran Sasso National Laboratory in Italy with 140 kg of HPGe detectors. With a total exposure of 61 kg yr, LEGEND-200 has achieved a background index of $5_{−2}^{+3}$ × 10 −4 counts/(keV kg yr) in the 0νββ decay signal region from the highest performing detectors. After combining the results from GERDA, the MAJORANA Demonstrator and LEGEND-200, an exclusion sensitivity > 2.8 × 10 26 yr has been obtained at 90% confidence level for the 0νββ decay half-life, with no evidence for a signal. A new observed lower limit of $T_{1/2}^{0v} >$ 1.9 × 10 26 yr at 90% confidence level has been established.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Energy resolution of the LZ detector for high-energy electronic recoils

The LUX-ZEPLIN (LZ) detector is a dual-phase liquid xenon time projection chamber (TPC) installed at the Sanford Underground Research Facility (Lead, South Dakota) at a depth of 1478 meters. Although the main objective of LZ is the direct detection of dark matter, its low background environment allows for the search of other rare processes, such as the neutrinoless double beta decay of xenon isotopes 134 Xe and 136 Xe with the respective Q-values of 826 keV and 2458 keV. The sensitivity of the detector to these decays is directly determined by the energy resolution, which, in turn, is degraded by non-uniformities in detector response. In this work, we present a novel method to correct, in the data, the non-uniformity of the light collected by an array of photosensors in a scintillation detector. This method is based on the knowledge of the light response functions of individual photosensors. With these techniques, we report, at a very early phase of the detector operations, a state-of-the-art energy resolution (σ/μ) of (0.67 ± 0.01)% at 2614 keV for the fiducial volume of 5.6 tonnes of liquid xenon.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

On the origins of trapped helium, neon and argon isotopic variations in meteorites. I - Gas-rich meteorites, lunar soil and breccia. II - Carbonaceous meteorites.

Data are presented from stepwise heating experiments and total extractions on five meteorites: Kapoeta, Fayetteville, Holman Island, Cee Vee, and Pultusk. These data reveal the presence of four isotopically distinct trapped neon components. A comparison of trapped neon with trapped helium and argon in bulk analyses indicates the existence of correlated helium, neon and argon isotopic structures. Component B is attributed primarily to direct implantation of rare gas ions by the present day solar wind. Component C is identified with directly implanted low energy (1-10 Mev/n) solar flare rare gases. Component D is associated with rare gas ions implanted in meteoritic material by the primitive, pre-main sequence, solar wind. A fourth component, observed only in Kapoeta and the lunar fines and breccia, is tentatively attributed to parent body 'atmospheric' ions implanted in surface material by a solar wind induced electric field.

Black, D. C.↗

Partitioning of Eu and Sr between coexisting plagioclase and K-feldspar.

Minerals were separated by an EM approach and with the aid of liquids of great density. An analysis of K, Rb, Ca, Sr, Ha, and rare earth elements was conducted by means of a mass spectrometer isotope dilution technique. The behavior of the divalent europium ions during the partition process was found to be very similar to that of divalent strontium ions, taking into consideration data of the partition coefficients between coexisting feldspars in acidic rocks.

Nagasawa, H.↗