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NASA NTRS1984

Rare gases in cyclosilicates and cogenetic minerals

The cyclosilicate minerals, beryl, tourmaline, and cordierite, typically contain large amounts of He-4 and Ar-40 which are not in situ radiogenic products. In the study of excess rare gases in cyclosilicates, one of the most enigmatic observations is the age effect, a qualitative tendency for geologically older samples to contain more excess He-4 and Ar-40 than younger samples. The present investigation is concerned with measurements regarding the abundance and isotopic composition of all five rare gases in a number of cyclosilicates as well as in their cogenetic minerals. The significance of the obtained data is discussed. The data indicate that cyclosilicates sample the rare gases present in the environment in which they crystallize. This 'sampling' involves major elemental fractionations which are variable but mineral specific. Cyclosilicates can, therefore, be used to probe the isotopic ratios and elemental compositions.

Saito, K.↗

NASA NTRS1983

The isotopic composition and concentration of Ag in iron meteorites and the origin of exotic silver

The isotopic composition of Ag and the concentration of Ag and Pd in Canyon Diablo (IA), Grant (IIIB), Santa Clara, Tlacotepec and Warburton Range (IVB), Pinon and Deep Springs (anom) were analyzed. Troilite from Santa Clara and from Grant was also studied. With the exception of IA, all the meteorites were enriched in Ag-107 by about 2%-212% and the ratio of Ag-107/Ag-109 in the metal phase was found to be greater than the terrestrial value. Ag of anomalous isotopic composition was found to be common in all IVB and anomalous meteorites. A correlation of Ag-107/Ag-109 with Pd/Ag was established except for the iron meteorite of Santa Clara. The excess Ag-107 is thought to result from the decay of Pd-107. The Grant data appear to represent a Pd-107-Ag-107 isochron and indicate that the cooling rate at elevated temperatures was rapid enough to preserve the isotopic differences between metal and troilite. The data suggest that Ag in Santa Clara is made up of almost pure Ag-107 produced from Pd-107 decay and Ag-109 produced by nuclear reactions with only a small amount of 'normal' Ag. This indicates an intense energetic particle bombardment history in the early solar system which occurred after the formation of small planetary bodies.

Kaiser, T.↗

DOE OSTI2023

Engineering a modular 44 Ti/ 44 Sc generator: eluate evaluation in preclinical models and estimation of human radiation dosimetry

Background: 44 Sc/ 47 Sc is an attractive theranostic pair for targeted in vivo positron emission tomographic (PET) imaging and beta-particle treatment of cancer. The 44 Ti/ 44 Sc generator allows daily onsite production of this diagnostic isotope, which may provide an attractive alternative for PET facilities that lack in-house irradiation capabilities. Early animal and patient studies have demonstrated the utility of 44 Sc. In our current study, we built and evaluated a novel clinical-scale 44 Ti/ 44 Sc generator, explored the pharmacokinetic profiles of 44 ScCl 3 , [ 44 Sc]-citrate and [ 44 Sc]-NODAGA (1,4,7-triazacyclononane,1-glutaric acid-4,7-acetic acid) in naïve mice, and estimated the radiation burden of 44 ScCl 3 in humans. Methods: 44 Ti/ 44 Sc (101.2 MBq) in 6 M HCl solution was utilized to assemble a modular ZR resin containing generator. After assembly, 44 Sc was eluted with 0.05 M HCl for further PET imaging and biodistribution studies in female Swiss Webster mice. Based on the biodistribution data, absorbed doses of 44 / 47 ScCl 3 in human adults were calculated for 18 organs and tissues using the IDAC-Dose software. Results: 44 Ti in 6 M HCl was loaded onto the organic resin generator with a yield of 99.97%. After loading and initial stabilization, 44 ScCl 3 was eluted with 0.05 M HCl in typical yields of 82.9 ± 5.3% (N = 16), which was normalized to the estimated generator capacity. Estimated generator capacity was computed based on elution time interval and the total amount of 44 Ti loaded on the generator. Run in forward and reverse directions, the 44 Sc/ 44 Ti ratio from a primary column was significantly improved from 1038 ± 440 to 3557 ± 680 (Bq/Bq) when a secondary, replaceable, ZR resin cartridge was employed at the flow outlet. In vivo imaging and ex vivo distribution studies of the reversible modular generator for 44 ScCl 3 , [ 44 Sc]-citrate and [ 44 Sc]-NODAGA show that free 44 Sc remained in the circulation significantly longer than the chelated 44 Sc. The dose estimation of 44 ScCl 3 reveals that the radiation burden is 0.146 mSv/MBq for a 70 kg adult male and 0.179 mSv/MBq for a 57 kg adult female. Liver, spleen and heart wall will receive the highest absorbed dose: 0.524, 0.502, and 0.303 mGy/MBq, respectively, for the adult male. Conclusions: A clinical-scale 44 Ti/ 44 Sc generator system with a modular design was developed to supply 44 ScCl 3 in 0.05 M HCl, which is suitable for further radiolabeling and in vivo use. Our data demonstrated that free 44 ScCl 3 remained in the circulation for extended periods, which resulted in approximately 10 times greater radiation burden than stably chelated 44 Sc. Stable 44 Sc/ 47 Sc-complexation will be more favorable for in vivo use and for clinical utility.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

NASA NTRS2001

In Situ Measurements of Meteoric Ions

Extraterrestrial material is the source of metal ions in the Earth's atmosphere, Each year approx. 10(exp 8) kg of material is intercepted by the Earth. The origin of this material is predominantly solar orbiting interplanetary debris from comets or asteroids that crosses the Earth's orbit. It contains a very small amount of interstellar material. On occasion the Earth passes through enhanced amounts of debris associated with the orbit of a decaying comet. This leads to enhanced meteor shower displays for up to several days. The number flux of shower material is typically several times the average sporadic background influx of material. Meteoric material is some of the earliest material formed in the solar system. By studying the relative elemental abundances of atmospheric metal ions, information can be gained on the chemical composition of cometary debris and the chemical makeup of the early solar system. Using in situ sampling with rocket-borne ion mass spectrometers; there have been approximately 50 flights that made measurements of the metal ion abundances at attitudes between 80 and 130 km. It is this altitude range where incoming meteoric particles am ablated, the larger ones giving rise to visible meteor. displays. In several rocket measurements isotopic ratios of different atomic ion mass components and metal molecular ion concentrations have been determined and used to identify unambiguously the measured species and to investigate the processes controlling the metal ion distributions The composition of the Earth's ionosphere was first sampled by an ion mass spectrometer flown an a rocket in 1956. In 1958 a rocket-borne ion spectrometer identified, fbr the first time, a layer of metal ions near 95 km. These data were interpreted as evidence of an extraterrestrial rather than a terrestrial source. Istomin predicted: "It seems probable that with some improvement in the method that analysis of the ion composition in the E-region may be used for determining the chemical composition of those meteors which do not reach the ground. Particularly, we hope to get information about the composition difference between particles of different meteor showers and also sporadic and shower meteoroids". These visions categorized the aims of many subsequent rocket-borne ion mass spectrometer experiments in the lower ionosphere, Although the use such measurements to deduce the composition of different classes of meteoroids has not been successful, the past four decades of rocket observations have provided po%erful sets of data for advancing our understanding of meteor ablation, meteoric composition, metal neutral and ion chemistry as well as ionospheric dynamics.

Grebowsky, Joseph M.↗

NASA NTRS1978

Chemical and Sr-isotopic characteristics of the Luna 24 samples

The chemical and Sr isotopic characteristics of Luna 24 bulk soil samples are determined and interpreted within the framework of lunar mare basalt evolution. Major and trace element compositions lead to the suggestion of candidate rock types consisting of a basalt/gabbro with very low TiO2 and MgO content (52%), a very low TiO2 basalt with 10% MgO (23%), olivine vitrophyre (20%), low K Fra Mauro basalt (4%) and anorthositic gabbro (1%). The proposed compositions are supported by the agreement of mixing models based on the proposed compositions with observed soil compositions. Sr ratios for plagioclase samples imply a lower Sr-87/Sr-86 value for low Mg soils than for other mare basalts and higher Rb/Sr and a more evolved Sr ratio in high Mg basalts. Rb, Sr and rare earth element compositions for low Mg basalts fit a model of partial remelting of cumulates containing small amounts of plagioclase.

Nyquist, L. E.↗

DOE OSTI2022

AGR-5/6/7 Final Release-to-Birth Ratio Data Analysis

AGR-5/6/7 is the last of a series of Advanced Gas Reactor (AGR) experiments conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) in support of development and qualification of tristructural isotropic (TRISO) low-enriched fuel for use in the high-temperature gas cooled reactor (HTGR). AGR configuration and irradiation conditions are based on prismatic HTGR technology that is distinguished primarily through the use of helium coolant, a low-power-density ceramic core capable of withstanding very high temperatures, and TRISO-coated particle fuel. The AGR tests provide valuable irradiation-performance data to support fuel process development, qualify fuel for normal operation and accident conditions, and support development and validation of fuel performance and fission-product (FP) transport models and codes. Each AGR test consists of multiple independently controlled and monitored capsules containing fuel compacts placed in a graphite cylinder shrouded by a steel shell. Release-to-birth ratios (R/B) for fission-gas isotopes released from each capsule are calculated from release rates, measured by germanium detectors in the Fission Product Monitoring System (FPMS) installed downstream from each capsule, and birth rates calculated using numerical models of FG generation. The R/Bs are a critical measure of the ability of the fuel kernel, the particle coating layers, and the compact matrix to retain fission-gas atoms, preventing their release into the sweep-gas flow, and the impact of initially defective particles and/or particle-coating failures that occur during irradiation. For fission-gas isotopes, particle failure is defined as failure of all coating layers, allowing gaseous fission atoms to escape from a particle. During the first five cycles (162B ? 165A), R/Bs were stable in the 10-8?10-6 range, and no in-pile particle failures were observed, based on the gross gamma counts. The maximum R/B value of around 2 ? 10-6 for Kr-85m resulted from the presence of as-fabricated exposed kernels (based on the high exposed kernel fraction), the dispersed uranium, and high fuel particle temperatures in Capsule 1. Comparison of capsule-measured R/Bs from these early cycles to predictions using the previously developed AGR R/B model demonstrated FG release from the AGR-5/6/7 TRISO fuel was comparable to that of previous experiments. In addition, the Kr-85m R/B per-exposed-kernel values are comparable to R/B values obtained in AGR-3/4 irradiation experiment and four irradiation experiments performed during 1980s: (1) HRB-17/18, (2) COMEDIE-BD1, (3) HFR B1, and (4) HRB-21. In contrast, all measured R/B values are lower than predictions by the commonly used Richards and German models, which are intentionally conservative. A large number of in-pile particle failures occurred in Capsule 1 by the end of Cycle 166A. During the final four cycles (166A ? 168A), apparent damage to the Capsule 1 gas line appeared to cause FG leakage from that capsule into the other four capsules, resulting in an increase in fission gas (FG) detected in the effluent for all capsules. Isolation of the Capsule 1 gas line during the last three cycles also prevented measurement of its FG release. Thus, R/Bs in all capsules after Cycle 166A are highly uncertain because of undefined amount of leakage from Capsule 1, especially for long-lived isotopes. A few hundred in-pile particle failures were estimated for Capsule 1 before the end of Cycle 166A, but the total number of failures is unknown due to the lack of FG release data in the later cycles. Based primarily on evidence from the gross gamma counts during Cycle 168A, approximately 15 particles failed in Capsule 3 and four particles failed in Capsule 2. In-pile failures in Capsule 3 were anticipated because this capsule was designed to operate beyond the HTGR normal operating temperature range. In contrast, no in-pile failures were identified in the top two capsules (4 and 5) based on the absence of the typical spikes in gross gamma counts and low failure estimates using the AGR model, developed in INL/EXT-14-32970, for R/B of the short-lived isotopes (Kr-89 and Xe-137) with minimal leakage from Capsule 1.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

The BIRDIES Experiment: Measuring Beryllium Isotopes to Resolve Dynamics in the Stratosphere

Cosmogenic beryllium-10 and beryllium-7, and the ratio of the two (10Be/7Be), are powerful atmospheric tracers of stratosphere–troposphere exchange (STE) processes; however, measurements are sparse for altitudes well above the tropopause. We present a novel high-altitude balloon campaign aimed to measure these isotopes in the mid-stratosphere called Beryllium Isotopes for Resolving Dynamics in the Stratosphere (BIRDIES). BIRDIES targeted gravity waves produced by tropopause-overshooting convection to study their propagation and impact on STE dynamics, including the production of turbulence in the stratosphere. Two custom-designed payloads called FiSH and GASP were flown at altitudes approaching 30 km to measure in situ turbulence and beryllium isotopes (on aerosols), respectively. These were flown on nine high-altitude balloon flights over Kansas, USA, in summer 2022. The atmospheric samples were augmented with a ground-based rainfall collection targeting isotopic signatures of deep convection overshooting. Our GASP samples yielded mostly negligible amounts of both 10Be and 7Be collected in the mid-stratosphere but led to design improvements to increase aerosol capture in low-pressure environments. Observations from FiSH and the precipitation collection were more fruitful. FiSH showed the presence of turbulent velocity, temperature, and acoustic fluctuations in the stratosphere, including length scales in the infra-sonic range and inertial subrange that indicated times of elevated turbulence. The precipitation collection, and subsequent statistical analysis, showed that large spatial datasets of 10Be/7Be can be measured in individual rainfall events with minimum terrestrial contamination. While the spatial patterns in rainfall suggested some evidence for overshooting convection, inter-event temporal variability was clearly observed and predicted with good agreement using the 3D chemical transport model GEOS-CHEM.

58 GEOSCIENCES↗

DOE OSTI2023

Light-driven hydrogen evolution via a novel pincer/no pincer mechanism including a possible concerted proton electron transfer

The road to efficient molecular catalysts for artificial photosynthesis requires a great deal of basic research to address the challenges of anthropogenic global warming. An unexpected result of such research is a novel pincer/no pincer mechanism discovered for the DFT-calculated catalytic cycle of PNP-C2 complexes. Structural parameters from theoretical modeling are supported by single crystal X-ray data for the corresponding complexes. Using the examples of [M(II)Cl(PNP-C2-R)] + (M = Pd 2+ , Ni 2+ ; R = CH 3 , H; PNP-C2 = N,N-bis{(di(2-methoxy-phenyl)phosphanyl)ethyl}-N-alkylamine) this pincer/no pincer mechanism is supported by differential pulse voltammetric, cyclic voltammetric, UV-Vis spectroscopic (combined with voltammetry) and 31 P nuclear magnetic resonance spectroscopic studies. The efficiency of hydrogen evolution during artificial photosynthesis depends significantly on the ratio of photosensitiser and water reduction catalysts. At first sight, the results from irradiation experiments (gas chromatography and mass spectrometry) seem obvious, but show a considerable impact of secondary and tertiary amines within the pincer structure. The best result obtained for the palladium pincer complex was with a secondary amine as a proton relay, delivering a turnover number of 2237 after only 2.5 hours. In contrast the analogous water reduction catalyst with a methylated (tertiary) amine instead of a secondary one gives only 972 turnovers under the same experimental conditions, over the same time. For all photocatalytic measurements the amount of hydrogen is approximately 2.5-times higher when a secondary amine is used as the proton relay. The influences of these different amines on the activity of water reduction catalysts during irradiation experiments in H 2 O or D 2 O lead to evidence of a kinetic isotope effect, supporting a possible concerted proton electron transfer. DFT calculations of reaction enthalpies, activation energies and intrinsic reaction coordinates of the catalytic cycle support the high efficiency of the presented catalysts. In particular, results from secondary amines suggest new candidates as examples of the rarely known concerted proton electron transfer.

14 SOLAR ENERGY↗

DOE OSTI2022

Evaluation of the Effect of Burnup Acceleration on UO 2 Microstructure Evolution

Accelerated fuel qualification (AFQ) is a methodology by which new nuclear fuels are developed in an accelerated time frame compared with historical fuel qualification approaches. AFQ generally relies on high-fidelity physics-based modeling and simulation tools to adequately describe fuel performance as well as on revolutionary methods to accelerate burnup accumulation and collect relevant data more quickly. This report summarizes the use of advanced fuel modeling and simulation tools to evaluate microstructures from commercially irradiated fuel and microstructures from proposed MiniFuel irradiations, in which burnup accumulation is accelerated while prototypic temperature conditions are maintained. In this milestone, we used the mesoscale fuel performance code MARMOT to model the evolution of irradiated UO 2 microstructures and their potential restructuring at high burnup. The simulation conditions were informed by BISON models of both commercially irradiated fuel and MiniFuel. A first set of simulations investigated the recrystallization behavior of fully dense microstructures and showed full recrystallization at burnups as low as 52 MWd/kgU at 950°C. However, these simulations did not account for the presence of fission gas bubbles (predicted by BISON). Therefore, a second set of simulations including fission gas bubbles was performed and indicated that at the lowest temperature considered (650°C), the porous UO 2 microstructures have the highest total Gibbs free energies and are likely to recrystallize earlier than higher temperature cases (800 and 950°C), which agrees with high-burnup fuel characterization data. The results also showed that at lower temperature (650°C), the total free energies of the PWR fuel and MiniFuel microstructures are not significantly different. However, at the highest temperature (950°C), MiniFuel microstructures have a lower free energy than that of the PWR fuel microstructure. The competing effects between the temperature-dependent grain nucleation rate and the reduction of the free energy of the microstructure at higher temperature as a result of diffusion indicated that restructuring may occur at even higher temperatures than those considered in this study. In addition to the microstructure evolution modeling efforts, the burnup gradient across a single fuel specimen was also considered. This evaluation was for the VXF-15 position of the High Flux Isotope Reactor (HFIR) using the code suite HFIRCON, which was developed to automate the workflow for evaluating targets and fuel as they are irradiated in HFIR. The burnup gradient evaluation showed a dependence on both the axial and radial locations within the specimen, with a maximum difference of 1.7 between the inner and outermost radial layers. This relationship was further supported by considering the fission product speciation with respect to location within the specimen, which showed a higher concentration of 239 Pu, 240 Pu, and 241 Pu on the outer radial locations of the specimen than the center. The findings of the burnup and speciation evaluation show that some amount of self-shielding is occurring in the specimen when irradiated in the high-flux environment of HFIR; however, this impact is more pronounced for natural uranium when compared to 6% enrichment due to the higher ratio of 238 U in the specimen. Further analyses are required to understand the sensitivity of this gradient to spatial mesh and enrichment of the specimen.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

COMBLE-ISLAS water isotopes in precipitation (COMBLEISLASISO)

During the measurement period, precipitation was sampled on daily to sub-daily basis with a sampling kit consiting of a clear plastic box (60x40x40 cm) mounted to a ground structure. Daily sampling lasted from 22 Feb to 24 Mar 2020. At a fixed time of day (10 UTC), samples were collected and the sampling box cleaned for the next sample. Additionally, during intense observations periods (IOPs) announced by ISLAS, ARMS scientists increased sampling frequency to sub-daily sampling. During the campaign period, 2 IOPs were conducted, with in total 12 samples taken. IOP1 lasted from 27 Feb 10 to 02 Mar 2020, and IOP2 lasted from 12 Mar to 14 Mar 2020. Solid precipitation in the box was then melted, transferred to an 8 ml glass vial, sealed and shipped to FARLAB (University of Bergen, Norway) for stable water isotope analysis. Measured stable isotope composition of precipitation samples will be related to conditions at other sampling locations, and at the evaporation site to inform about conservation of water isotope quantities. In the period from 22 Feb to 24 Mar, 23 daily samples were collected at 10 UTC for stable water isotope analysis. During the entire sampling period, a high variability of precipitation phase was encountered. Most samples were recovered in the form of graupel/snow (12 samples), as rain (7 samples), and the remaining samples fell as graupel, snow, rain or frozen rain. Precipitation amounts varied between <1 mm (26 Feb) and 140 mm (25 Feb) within the sampling box. Furthermore, higher-resolution sampling was conducted during 2 intense observation periods (IOPs). During IOP1, lasting from 27 Feb 10 UTC to 02 Mar 10 UTC, 7 samples were collected, all of them as solid phase precipitation. IOP2 lasted from 12 Mar 10 UTC to 14 Mar 09 UTC, and 5 samples (all as graupel/snow) were collected. Samples were processed according to FARLAB standard measurement procedures. In short, samples were transferred to 1.5 ml glass vials with rubber/PTFE septa (part #548-0907, VWR, USA). An autosampler (A0325, Picarro Inc) transferred ca. 2µl per injection into a high-precision vapourizer (A0211, Picarro Inc, USA) heated to 110°C. After blending with dry N2 (< 5 ppm H2O) the gas mixture was directed into the measurement cavity of a Cavity-Ring Down Spectrometer (L2140-i, Picarro Inc) for about 7 min with a typical water concentration of 20 000 ppm. Memory effects were reduced by two times measuring a vapour mixture at a mixing ratio of 50 000 ppm, obtained from 2 injections of 2 µl for 5 min at the beginning of each new sample vial. Thereafter, another 6 injections of 2 µl per sample were measured individually as described above, and averages of the last 5 injections were used for further processing. Three standards were measured at the beginning and end of each batch, including a drift standard DI2 (δD: -50.72±0.73 permil, δ18O: -7.63±0.10 permil), and for calibration the laboratory standards GLW (δD: -307.79±0.75 permil, δ18O: -40.02±0.07 permil) and EVAP2 (δD: 9.52±0.65 permil, δ18O: 1.81±0.13 permil). A detailed calibration report is included with the final uploaded data set.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRSDate not supplied

Isotopic Tracers for CO 2 Produced During A Planetary Impact Into Limestone Target Rocks

Terrestrial meteorite impacts have been directly linked with multiple mass extinction events throughout Earth’s history. Among these impacts, those that land in sedimentary target rocks are thought to generate large quantities of CO 2 via decarbonation. This injection of CO 2 into the atmosphere has the potential to alter the climate and threaten terrestrial habitability. The magnitude of this change depends upon the net amount of CO 2 released, which is controlled by how much CO 2 is produced by the impact, how much CO 2 is removed by back-reactions after the impact, and other post-impact CO 2 sinks. To interrogate the behavior of CO 2 release into the impact atmosphere, we present carbon (δ 13 C), oxygen (δ 18 O), and clumped (Δ 47 ) isotope results from carbonate clasts preserved within the impact breccia of the Steen River Impact Structure (SRIS) in Alberta, Canada. These clasts exhibit a ~65‰ range in δ 13 C and a ~5‰ variation in δ 18 O. However, while δ 13 C and δ 18 O are positively correlated, Δ 47 unexpectedly has a negative relationship with δ 13 C and δ 18 O. Based on prior assumptions, there would either be (1) no relationship with carbonate Δ 47 and the bulk ratios because Δ 47 would be reset at extreme impact temperatures, or (2) Δ 47 would have a positive correlation with the bulk ratios, reflecting gradual Δ 47 ‘resetting.’ To reconcile the SRIS result with these expectations, we conducted a series of in vacuo heating experiments at temperatures above calcite decomposition. As predicted by Rayleigh fractionation, these heating experiments generated depletions in δ 13 C and δ 18 O that increased with reaction time. Mimicking the SRIS results, these experiments also produced concomitant increases in Δ 47 . Using an adaptation of a mechanistic model for decomposition fractionation (Hayles & Killingsworth, 2022) we hypothesize that these exotic isotope trends are caused by Rayleigh fractionation and a Δ 47 kinetic isotope effect that results from the disproportionation of O to CaO and CO 2 during thermal decomposition. This high Δ 47 CO 2 subsequently exchanges with the residual CaCO 3 . This work highlights a potential pathway for identifying and quantifying CO 2 generation by impacts and builds on the relatively limited literature characterizing the behavior of carbonate clumped isotopes at very high geologic temperatures.

Multi-isotope systems↗

NASA NTRS1994

Heating during solar nebula formation and Mg isotopic fractionation in precursor grains of CAIs and chondrules

In some Ca-Al-rich inclusion (CAI) grains, mass-dependent isotopic fractionations of Mg, Si, and O are observed and large Mg isotopic fractionation is interpreted to have been produced by cosmochemical processes such as evaporation and condensation. Mass-dependent Mg isotopic fractionation was found in olivine chondrules of Allende meteorites. Presented is an approximate formula for the temperature of the solar nebula that depends on heliocentric distance and the initial gas distribution. Shock heating during solar nebula formation can cause evaporative fractionation within interstellar grains involved in a gas at the inner zone (a less than 3 AU) of the disk. Alternatively collision of late-accreting gas blobs might cause similar heating if Sigma(sub s) and Sigma are large enough. Since the grain size is small, the solid/gas mass ratio is low and solar (low P(sub O2)), and the ambient gas pressure is low, this heating event could not produce chondrules themselves. Chondrule formation should proceed around the disk midplane after dust grains would grow and sediment to increase the solid/gas ratio there. The heating source there is uncertain, but transient rapid accretion through the disk could release a large amount of heat, which would be observed as FU Orionis events.

Sasaki, S.↗

NASA NTRS1993

Interstellar grains in primitive meteorites - Diamond, silicon carbide, and graphite

Primitive meteorites contain a few parts per million (ppm) of pristine interstellar grains that provide information on nuclear and chemical processes in stars. Their interstellar origin is proven by highly anomalous isotopic ratios, varying more than 1000-fold for elements such as C and N. Most grains isolated thus far are stable only under highly reducing conditions (C/O greater than 1), and apparently are 'stardust' formed in stellar atmospheres. Microdiamonds, of median size about 10 A, are most abundant (about 400-1800 ppm) but least understood. They contain anomalous noble gases including Xe-HL, which shows the signature of the r- and p-processes. Silicon carbide, of grain size 0.2-10 microns and abundance about 6 ppm, shows the signature of the s-process and apparently comes mainly from red giant carbon (AGB) stars of 1-3 solar masses. Some grains appear to be not less than 10 exp 9 a older than the solar system. Graphite spherules of grain size 0.8-7 microns and abundance less than 2 ppm contain highly anomalous C and noble gases, as well as large amounts of fossil Mg-26 from the decay of extinct Al-26. They seem to come from at least three sources, probably AGB stars, novae, and Wolf-Rayet stars.

Anders, Edward↗

NASA NTRS2013

Elemental GCR Observations during the 2009-2010 Solar Minimum Period

Using observations from the Cosmic Ray Isotope Spectrometer (CRIS) onboard the Advanced Composition Explorer (ACE), we present new measurements of the galactic cosmic ray (GCR) elemental composition and energy spectra for the species B through Ni in the energy range approx. 50-550 MeV/nucleon during the record setting 2009-2010 solar minimum period. These data are compared with our observations from the 1997-1998 solar minimum period, when solar modulation in the heliosphere was somewhat higher. For these species, we find that the intensities during the 2009-2010 solar minimum were approx. 20% higher than those in the previous solar minimum, and in fact were the highest GCR intensities recorded during the space age. Relative abundances for these species during the two solar minimum periods differed by small but statistically significant amounts, which are attributed to the combination of spectral shape differences between primary and secondary GCRs in the interstellar medium and differences between the levels of solar modulation in the two solar minima. We also present the secondary-to-primary ratios B/C and (Sc+Ti+V)/Fe for both solar minimum periods, and demonstrate that these ratios are reasonably well fit by a simple "leaky-box" galactic transport model that is combined with a spherically symmetric solar modulation model.

Solar Modulation↗

DOE OSTI2020

The Cost of (In-) Accurate Waste Characterization in the U.S. Nuclear Power Industry - 20066

Proper disposal of waste has never been a human priority. Our history is full of examples of throwing away things with minimal effort or thought to consequence. That is until disease or toxicity become apparent and we realize we need to change. Unfortunately, we almost never have all the information we need at the time we make decisions. In addition to the technical and scientific issues, profits and politics are also factors. Newton's third law also applies to politics and so for every policy (action) put in place, there will be (opposite reaction) forces in play to push back against it. These forces are seldom balanced and so the reaction to the discovery of harm is to over-correct and destroy the benefit to be had. This of course causes those who want the benefit, or profit from it, to work to undermine or repeal those measures put in place to eliminate the harm. The issue is exacerbated when the problem to be solved is highly technical and at the edge of our science so that the harm and benefit cannot be easily or accurately quantified. At these times, reason often goes out the window and our decision makers are influenced by either greed or fear as these emotions are much easier to stoke. Those of us in the middle, with the charge to 'do the right thing for the least cost', are therefore frequently constrained and forced into actions that are neither technically the right thing to do and not cost effective. The cost of radioactive waste disposal is based on the concentrations of various radioisotopes in the waste. Some of these isotopes are relatively easy to quantify and some are not. Most laboratory methods for quantification are limited in the amount of activity that can be present during the measurement process. Current nuclear plants were not designed with the idea that taking truly representative waste samples would be important. The limits used to define waste class and therefore cost are precisely defined but the methods for determining those concentrations are far less precise. Improving the accuracy of radioactivity concentrations in waste and having consistent and reasonable oversight can reduce waste costs through active management of the process. So what can we do about it? Science may provide an answer. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS2007

A Rb-Sr and Sm-Nd Isotope Geochronology and Trace Element Study of Lunar Meteorite LaPaz Icefield 02205

Rubidium-strontium and samarium-neodymium isotopes of lunar meteorite LaPaz Icefield (LAP) 02205 are consistent with derivation of the parent magma from a source region similar to that which produced the Apollo 12 low-Ti olivine basalts followed by mixing of the magma with small amounts (1 to 2 wt%) of trace element-enriched material similar to lunar KREEP-rich sample SaU 169. The crystallization age of LAP 02205 is most precisely dated by an internal Rb-Sr isochron of 2991+/-14 Ma, with an initial Sr-87/Sr-88 at the time of crystallization of 0.699836+/-0.000010. Leachable REE-rich phosphate phases of LAP 02205 do not plot on a Sm-Nd mineral isochron, indicating contamination or open system behavior of the phosphates. Excluding anomalous phases from the calculation of a Sm-Nd isochron yields a crystallization age of 2992+/-85 (initial Epsilon Nd-143 = +2.9+/-0.8) that is within error of the Rb-Sr age, and in agreement with other independent age determinations for LAP 02205 from Ar-Ar and U-Pb methods. The calculated Sm-147/Nd-144 source ratios for LAP 02205, various Apollo 12 and 15 basalts, and samples with strong affinities to KREEP (SaU 169, NWA 773, 15386) are uncorrelated with their crystallization ages. This finding does not support the involvement of a common KREEP component as a heat source for lunar melting events that occurred after crystallization of the lunar magma ocean.

Rankenburg, K.↗

DOE OSTI2022

Implications of the non-observation of 6 Li in halo stars for the primordial 7 Li problem

The primordial Lithium Problem is intimately connected to the assumption that the 7 Li abundance observed in metal-poor halo stars is unchanged from its primordial value, which lies significantly below the predictions of standard big-bang nucleosynthesis. Two key lines of evidence have argued that these stars have not significantly depleted their initial (mostly primordial) 7 Li: i) the lack of dispersion in Li abundance measurements at low metallicity (and high surface temperature); and ii) the detection of the more fragile 6 Li isotope in at least two halo stars. The purported 6 Li detections were in good agreement with predictions from cosmic-ray nucleosynthesis which is responsible for the origin of 6 Li. This concordance left little room for 6 Li depletion, and the apparent 6 Li survival implied that 7 Li largely evaded destruction, because stellar interiors destroy 6 Li more vigorously then than 7 Li. Recent (re)-observations of halo stars challenge the evidence against 7 Li depletion: i) lithium elemental abundances now show significant dispersion, and ii) sensitive 6 Li searches now reveal only upper limits to the 6 Li/ 7 Li ratio. We discuss the consequences of these 6 Li non-detections on the primordial 7 Li Problem, Galactic cosmic-ray nucleosynthesis, and the question of differential depletion of Li in stars. The tight new 6 Li upper limits generally fall far below the predictions of cosmic-ray nucleosynthesis, implying that substantial 6 Li depletion has occurred — by factors up to 50. We show that in stars with 6 Li limits and thus lower bounds on 6 Li depletion, an equal amount of 7 Li depletion is more than sufficient to resolve the primordial 7 Li Problem. This picture is consistent with well-studied stellar models in which 7 Li is less depleted than 6 Li, and strengthen the case that the Lithium Problem has an astrophysical solution. We conclude by suggesting future observations that could test these ideas.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2022

The calculation of light element impurity (α, n) yield curves in a PuO 2 matrix and associated specific yield coefficients: Influence of the reaction cross sections

Most of the Pu separated from irradiated commercial nuclear fuel is stored as PuO 2 . The primary quantitative nondestructive measurement technique used to verify the amount of Pu in storage containers is passive neutron correlation counting. An important physical property of the oxide material is the ratio, α, of the rate of (α, n) neutrons produced inside the item to the rate of neutrons produced by spontaneous fission. This ratio influences the precision of the correlated counting method and affects the interpretation of the data because of how it changes both the primary total neutron production rate and the rate of induced fission events taking place inside the item. In addition to the main O(α, n) contribution, additional contributions come from α-particle interactions with light element impurities that are inevitably present. In this work, we calculate specific (α, n) yield coefficients, expressed in units of neutrons per second per gram of α-emitting nuclide per part per million by mass of the specified impurity element distributed in a pure PuO 2 matrix, for some key α-emitting actinides commonly present in reprocessed Pu ( 238–242 Pu+ 241 Am). These coefficients are directly applicable to nuclear safeguards verification work in which the α ratio is often calculated from the Pu-isotopic composition and chemical information obtained by other means. Further, they also provide a convenient up-to-date reference set against which values generated by other methods can be compared. Results are presented for impurities with atomic number from 3 to 17 inclusive, plus K and Fe. In most cases, these coefficients are not expected to change by more than 5%–10% at any time in the future. However, as new data become available, changes as large as 20% may be needed for some targets (e.g., F). The present yield calculations are limited by the general shortage of quality experimental total (α, n) reaction cross section data, which, together with unexplained variation between determinations, means that an objective and coherent evaluation is not possible. The situation is even less satisfactory for the partial differential cross section needed to calculate neutron spectra.

(𝛼, n) reactions↗