Precision mass determinations with the electric mass filter
Mass determinations of medium weight elements with electric mass filter, and mass ratios of xenon isotopes
Von Zahn, U.↗
SEARCH · Engineering Papers
Results for “ISOTOPE RATIO”
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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The abundances of the elements.
For the immediate cosmic environs, there are three traditional sources of element abundance data, including chondritic meteorites, the solar atmosphere, and a certain type of average of stars near the sun. Cosmic ray material, or at least the particles that were accelerated to very high energies, includes contributions from great distances in the Galaxy, and perhaps from outside the Milky Way system itself. Problems in the determination of solar system abundances are discussed together with some factors affecting the profiles of spectral lines, the abundances of some elements in the solar atmosphere, young stars and the interstellar medium, the helium to hydrogen ratio, the helium isotopes, and abundances of light elements in the Galaxy and in neighboring galaxies.
Aller, L. H.↗
Is lunar bulk material similar to earth's mantle?
In an attempt to ascertain whether or not lunar bulk material is similar to the earth's mantle, consideration is given to the following parameters of both planetary bodies: oxygen isotopic composition, metal/silicate ratio, siderophile trace element concentrations, refractory lithophile trace element concentrations, volatile element ratios and volatile/refractory element ratios, bulk Mg /(Mg + Fe) ratio, Fe/Mn ratios, and redox state. The values of these parameters are estimated and various hypotheses for lunar origin are examined in their light.
Drake, Michael J.↗
Constraints on Galactic Cosmic-Ray Origins from Elemental and Isotopic Composition Measurements
The most recent measurements by the Cosmic Ray Isotope Spectrometer (CRIS) aboard the Advanced Composition Explorer (ACE) satellite of ultra-heavy cosmic ray isotopic and elemental abundances will be presented. A range of isotope and element ratios, most importantly Ne-22/Ne-20, Fe-58/Fe-56, and Ga-31/Ge -32 show that the composition is consistent with source material that is a mix of approx 80% ISM (with Solar System abundances) and 20% outflow/ejecta from massive stars. In addition, our data show that the ordering of refractory and volatile elements with atomic mass is greatly improved when compared to an approx 80%/20% mix rather than pure ISM, that the refractory and volatile elements have similar slopes, and that refractory elements are preferentially accelerated by a factor of approx 4. We conclude that these data are consistent with an OB association origin of GCRs.
Galactic Cosmic Rays↗
The Connected Isotopic Water Cycle in the Community Earth System Model Version 1
Because of the pervasive role of water in the Earth system, the relative abundances of stable isotopologues of water are valuable for understanding atmospheric, oceanic, and biospheric processes, and for interpreting paleoclimate proxy reconstructions. Isotopologues are transported by both largescale and turbulent flows, and the ratio of heavy to light isotopologues changes due to fractionation that can accompany condensation and evaporation processes. Correctly predicting the isotopic distributions requires resolving the relationships between largescale ocean and atmospheric circulation and smallerscale hydrological processes, which can be accomplished within a coupled climate modeling framework. Here we present the water isotopeenabled version of the Community Earth System Model version 1 (iCESM1), which simulates global variations in water isotopic ratios in the atmosphere, land, ocean, and sea ice. In a transient Last Millennium simulation covering the 850-2005 period, iCESM1 correctly captures the latetwentiethcentury structure of δ(exp 18)O and δD over the global oceans, with more limited accuracy over land. The relationship between salinity and seawater δ(exp 18)O is also well represented over the observational period, including interbasin variations. We illustrate the utility of coupled, isotopeenabled simulations using both Last Millennium simulations and freshwater hosing experiments with iCESM1. Closing the isotopic mass balance between all components of the coupled model provides new confidence in the underlying depiction of the water cycle in CESM, while also highlighting areas where the underlying hydrologic balance can be improved. The iCESM1 is poised to be a vital community resource for ongoing model development with both modern and paleoclimate applications.
Brady, E.↗
LLNL International Working Group on Gamma Spectrometry - Preparation of IDB Dataset
The spectral information and associated metadata, including source information, detector setup, and shielding configuration is described in human readable, comma-separated text files (csv). Five csv files are associated with each material type and include the following information (where [Isotope] is U, Pu, and MOX): [Isotope]_measurement_metadata - Metadata of the measurement configuration, including material composition at time of acquisition (decay corrected from certificate date). Data that is unique to a measurement configuration e.g. detector geometry, source-detector distance, analyzer and other electronics used, attenuating materials are provided in this file. [Isotope]_spectrum_metadata - The information that is unique to the spectrum. This includes detector specifications (e.g. date of acquisition, number of channels, gain (keV/channel), energy range, real and live time, full width half-maximum (FWHM) of the 186 or 208 peak for uranium or plutonium measurements, respectively. [Isotope]_source_metadata - The source material used for the measurement, this includes the ratio and uncertainties of isotopes present and processing information of the material. In addition, the certificate information for the source material is listed. [Isotope]_spectrum_counts_metadata - The counts per channel for each spectrum. This data is linked via the UID.spectrum index to the measurement_metadata file. [Isotope]_spectrum_checksum_metadata The MD5 checksum for the original spectrum file. This data is linked via the UID.spectrum index to the measurement_metadata file. This information is provided to prevent duplication of entries in the database.
42 ENGINEERING↗
LLNL International Working Group on Gamma Spectrometry - Preparation of IDB Dataset [Slides]
The spectral information and associated metadata, including source information, detector setup, and shielding configuration is described in human readable, comma-separated text files (csv). Six csv files are associated with each material type and include the following information (where [Isotope] is U, Pu, and MOX): [Isotope]_measurement_metadata Metadata of the measurement configuration, including material composition at time of acquisition (decay corrected from certificate date). Data that is unique to a measurement configuration e.g. detector geometry, source-detector distance, analyzer and other electronics used, attenuating materials are provided in this file. [Isotope]_spectrum_metadata The information that is unique to the spectrum. This includes detector specifications (e.g. date of acquisition, number of channels, gain (keV/channel), energy range, real and live time, full width half-maximum (FWHM) of the 186 or 208 peak for uranium or plutonium measurements, respectively. [Isotope]_source_metadata The source material used for the measurement, this includes the ratio and uncertainties of isotopes present and processing information of the material. In addition, the certificate information for the source material is listed. [Isotope]_spectrum_counts_metadata The counts per channel for each spectrum. This data is linked via the UID.spectrum index to the measurement_metadata file. [Isotope]_spectrum_checksum_metadata The MD5 checksum for the original spectrum file. This data is linked via the UID.spectrum index to the measurement_metadata file. This information is provided to prevent duplication of entries in the database. [Isotope]_provenance Details on the csv data provider, including laboratory and contract information.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Relative abundance of the helium isotopes He-3 and He-4 in the cosmic radiation
The geomagnetic field near the equator is used to measure the He-3/He-4 abundance ratio near 6 GeV/nucleon. This ratio is found to be 0.24 + or - 0.05, under the assumption that the helium rigidity spectrum has the form dI/dR = about R exp(-2.65). If all He-3 is of secondary origin, this implies an interstellar mean escape-path length of about 15 g/sq cm, a value considerably larger than that determined from observations of heavier elements but compatible with measurements of the helium isotopic ratio at lower energies.
Jordan, S. P.↗
The gallium isotopic composition of the Moon
Here, in this study, we present new Ga isotope data from a suite of 28 mare basalts and lunar highland rocks. The δ 71 Ga values of these samples range from -0.10 to +0.66‰ (where δ 71 Ga is the relative difference between the 71 Ga/ 69 Ga ratio of a sample and the Ga-IPGP standard), which is an order of magnitude more heterogeneous than δ 71 Ga values in terrestrial magmatic rocks. The cause of this isotopic heterogeneity must be established to estimate the bulk δ 71 Ga value of the Moon. In general, low-Ti basalts and ferroan anorthosite suite (FAS) rocks have δ 71 Ga values that are lower than high-Ti basalts and KREEP-rich rocks. The observation that rocks derived from later forming LMO cumulates have higher δ 71 Ga values suggests that Ga isotopes are fractionated by processes that operate within the chemically evolving LMO, rather than localized degassing or volatile redistribution. Correlations between indices of plagioclase removal from the LMO (e.g. Eu/Eu*) with Ga isotope ratios suggest that a Δ 71 Ga plagioclase-melt of -0.3‰, (where Δ 71 Ga plagioclase-melt is the isotopic fractionation associated with crystallization of plagioclase from a melt), could drive the observed isotopic fractionation in high-Ti mare basalts and KREEP-rich rocks. This would be consistent with the observation that FAS rocks have δ 71 Ga values that are lower than mare basalts. However, the addition of KREEP-like material into the mare basalt source regions would not contribute enough Ga to perturb the isotopic composition outside of analytical uncertainty. Thus, basalts derived from early formed LMO cumulates such as those from Apollo 15, would preserve light Ga isotopic compositions despite containing modest amounts of urKREEP. We estimate that the δ 71 Ga value of the LMO was ~0.14‰ prior to the onset of plagioclase crystallization and extraction. Whether this δ 71 Ga value is representative of the initial BSM cannot be ascertained from the current dataset. It remains plausible that the Moon accreted with a heavier Ga isotopic composition than the Earth. Alternatively, the Moon and Earth could have accreted with similar isotopic compositions (BSE = 0.00 ± 0.06‰, Kato et al., 2017) and volatile loss drove the LMO to higher δ 71 Ga values prior to formation of the lunar crust.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Microextraction–TQ–ICP–MS for the Direct Analysis of U and Pu from Cotton Swipes
Here, the microextraction sampling technique was integrated with triple quadrupole–inductively coupled plasma–mass spectrometry (TQ–ICP–MS) to directly sample and measure the isotopic compositions of uranium (U) and plutonium (Pu) from cotton swipes. Once extracted, the U/Pu were directed into the TQ–ICP–MS instrument for isotopic determination. Carbon dioxide (CO 2 ) and helium (He) gases were delivered to a collision reaction cell within the ICP–MS system for ion separation. The CO 2 reacts with the U + forming UO + which is ultimately separated from the Pu + ions of interest in the third quadrupole. This study demonstrates direct liquid extraction of U/Pu from a solid surface and subsequent measurement by TQ–ICP–MS in <60 s. Flow rates were optimized (0.3 mL min –1 CO 2 and 5 mL min –1 He) in the reaction cell of the ICP–MS system to maximize the Pu signal while minimizing U interferences (i.e., 238 U + tail and 238 UH + ) at m/z 239. Low levels of Pu (~2 pg) were deposited on a cotton swipe along with U at concentrations ranging from 20 to 200 ng. The 240 Pu/ 239 Pu ratio was measured with <7% relative difference from the certified value at all U concentrations. Major and minor U isotope ratios were also measured with <4% relative difference. This highlights that the microextraction–TQ–ICP–MS method can extract a mixed U/Pu sample directly from a cotton swipe and measure both isotopic systems without chemical separation.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
On the provenance of GEMS, a quarter century post discovery
The provenance of GEMS (glass with embedded metal and sulfides) in cometary type interplanetary dust particles is investigated using analytical scanning transmission electron microscopy and secondary ion mass spectrometry. We review the current state of knowledge and closely examine the densities, elemental compositions and distributions, iron oxidation states, and isotopic compositions of a subset of GEMS in chondritic porous interplanetary dust. We find that GEMS are underdense with estimated densities that are 35–65% of compositionally equivalent crystalline aggregates. GEMS low densities result in a lower contribution to the bulk compositions of IDPs than has been assumed based on their volume fraction. We also find that element/Si ratios, assumed to be primary (indigenous), are instead perturbed by contamination and secondary alteration, including pulse heating during atmospheric entry. Fe in pyrrhotite inclusions was oxidized and Mg, S, Ca, and Fe were depleted relative to lithophile Al and Si, resulting in reduction in element/Si ratios. Because they trap outgassing elements, Fe-rich oxide rims that formed on the surface of GEMS are serendipitous “witness plates” to the changes in composition that accompany atmospheric entry. As a result of alteration, GEMS elemental compositions cannot reliably inform about their provenance. Except for highly anomalous oxygen isotope ratios measured in some large GEMS grains that indicate a contribution from circumstellar dust, oxygen isotope compositions are generally poor indicators of provenance. Prior work indicates that most GEMS fall close to the terrestrial oxygen isotope composition, which, however, does not exclude a presolar interstellar origin. Nitrogen isotopic compositions are more diagnostic. Elevated 15 N/ 14 N ratios indicate that GEMS accreted in conjunction with formation of organic matter by ion–molecule reactions in a cold (<50 K) presolar environment like the extreme outer nebula or interstellar medium. Considering all observations, we conclude that GEMS are most likely processed interstellar silicates.
79 ASTRONOMY AND ASTROPHYSICS↗
Carbon, nitrogen and oxygen isotopes in the low energy galactic cosmic rays
The isotopes of C, N, and O in the galactic cosmic rays were measured in the 45-106 Mev/nucleon range with data collected during 1973-77 by the cosmic-ray telescope onboard the IMP-7 spacecraft. The ratios of (N-15)/N, (C-13)/C, and ((O-18)/O agreed with previous measurements. Cosmic ray propagation and solar modulation indicate that the measured N isotopic ratio is in agreement with a source ratio of (N-14)/O = 0.03, which is much lower than the solar system abundance ratio.
Guzik, T. G.↗
Isotopic Signature of Organic Molecules from Beyond the Solar System: An Enriched Methane D/H Ratio in the Interstellar Object 3I/ATLAS
Interstellar objects are interlopers from other planetary systems, and their volatile compositions provide a glimpse into planet formation around their host star. We present near-infrared spectra of the coma of interstellar object 3I/ATLAS measured with the James Webb Space Telescope. Our results demonstrate an unexpectedly high D/H = (3.31 ± 0.34)% for methane and represent an exceedingly rare detection of deuterated organic molecules in an interstellar object. This D/H ratio is a factor of 14 ± 2 higher than that measured in comet 67P/Churyumov-Gerasimenko by the Rosetta spacecraft, the only other comet for which CH3D has been detected, yet the ratio of deuteration in methane compared with water is consistent for both comets within 1.2σ. The D/H ratio in methane is observationally unconstrained in extrasolar sources to date, but the enriched ratio in 3I/ATLAS is most similar to those measured in other organic molecules toward primitive environments. The high D/H ratios of water and methane in 3I/ATLAS are a natural consequence of formation in a high D/H elemental ratio environment as a result of locally cold conditions in the protoplanetary disk and prior interstellar cloud. Thus, 3I/ATLAS formed in an environment very different from that in which our Sun and planets originated.
Interstellar Object 3I/ATLAS↗
Plutonium Signatures in Molten-Salt Reactor Off-Gas Tank and Safeguards Considerations
Fluid-fueled molten-salt reactors (MSRs) are actively being developed by several companies, with plans to deploy them internationally. The current IAEA inspection tools are largely incompatible with the unique design features of liquid fuel MSRs (e.g., the complex fuel chemistry, circulating fuel inventory, bulk accountancy, and high radiation environment). For these reasons, safeguards for MSRs are seen as challenging and require the development of new techniques. This paper proposes one such technique through the observation of the reactor’s off-gas. Any reactor design using low-enriched uranium will build up plutonium as the fuel undergoes burnup. Plutonium has different fission product yields than uranium. Therefore, a shift in fission product production is expected with fuel evolution. The passive removal of certain gaseous fission products to the off-gas tank of an MSR provides a valuable opportunity for analysis without significant modifications to the design of the system. Uniquely, due to the gaseous nature of the isotopes, beta particle emissions are available for observation. The ratios of these fission product isotopes can, thus, be traced back to the relative amount and types of fissile isotopes in the core. This proposed technique represents an effective safeguards tool for bulk accountancy which, while avoiding being onerous, could be used in concert with other techniques to meet the IAEA’s timeliness goals for the detection of a diversion.
Dunkle, Nicholas (ORCID:000000027323011X)↗
Abundances in red giant stars - Carbon and oxygen isotopes in carbon-rich molecular envelopes
Millimeter-wave observations have been made of isotopically substituted CO toward the envelopes of 11 carbon-rich stars. In every case, C-13O was detected and model calculations were used to estimate the C-12/C-13 abundance ratio. C-17O was detected toward three, and possibly four, envelopes, with sensitive upper limits for two others. The CO-18 variant was detected in two envelopes. New results include determinations of oxygen isotopic ratios in the two carbon-rich protoplanetary nebulae CRL 26688 and CRL 618. As with other classes of red giant stars, the carbon-rich giants seem to be significantly, though variably, enriched in O-17. These results, in combination with observations in interstellar molecular clouds, indicate that current knowledge of stellar production of the CNO nuclides is far from satisfactory.
Wannier, P. G.↗
Abundances in red giant stars - Nitrogen isotopes in carbon-rich molecular envelopes
Results are presented of millimeter- and submillimeter-wave observations of HCN and HCCCN that were made of the circmustellar envelopes of eight carbon stars, including the two protoplanetary nebulae CRL 618 and CRL 2688. The observations yield a measure of the double ratio (N-14)(C-13)/(N-15)(C-12). Measured C-12/C-13 ratios are used to estimate the N-14/N-15 abundance ratio, with the resulting lower limits in all eight envelopes and possible direct determinations in two envelopes. The two determinations and four of the remaining six lower limits are found to be in excess of the terrestrial value of N-14/N-15 = 272, indicating an evolution of the nitrogen isotope ratio, which is consistent with stellar CNO processing. Observations of thermal SiO (v = 0, J = 2-1) emission show that the Si-29/Si-28 ratio can be determined in carbon stars, and further observations are indicated.
Wannier, P. G.↗
Chemical composition measurements of the atmosphere of Jupiter with the Galileo Probe mass spectrometer
The Galileo Probe entered the atmosphere of Jupiter on December 7, 1995. Measurements of the chemical and isotopic composition of the Jovian atmosphere were obtained by the mass spectrometer during the descent over the 0.5 to 21 bar pressure region over a time period of approximately 1 hour. The sampling was either of atmospheric gases directly introduced into the ion source of the mass spectrometer through capillary leaks or of gas, which had been chemically processed to enhance the sensitivity of the measurement to trace species or noble gases. The analysis of this data set continues to be refined based on supporting laboratory studies on an engineering unit. The mixing ratios of the major constituents of the atmosphere hydrogen and helium have been determined as well as mixing ratios or upper limits for several less abundant species including: methane, water, ammonia, ethane, ethylene, propane, hydrogen sulfide, neon, argon, krypton, and xenon. Analysis also suggests the presence of trace levels of other 3 and 4 carbon hydrocarbons, or carbon and nitrogen containing species, phosphine, hydrogen chloride, and of benzene. The data set also allows upper limits to be set for many species of interest which were not detected. Isotope ratios were measured for 3He/4He, D/H, 13C/12C, 20Ne/22Ne, 38Ar/36Ar and for isotopes of both Kr and Xe.
unmanned↗
Nitrogen isotopes in lunar soils as a measure of cosmic-ray exposure and regolith history
Previous studies have shown that the bulk of the nitrogen in soils has been implanted by the solar wind, that the N-15/N-14 ratio of the implanted nitrogen has apparently increased with time, and that both soils and rocks contain a nitrogen component greatly enriched in N-15, relative to natural abundance ratios, due to cosmic-ray spallation. An investigation was, therefore, conducted to test the feasibility of using spallation-produced N-15 for determining cosmic-ray exposure ages. Samples from several depths in the Apollo 15 deep drill core were analyzed. The data obtained have also been evaluated with regard to possible models for the prior history of the material now in the Apollo 15 core. In addition, analyses have been performed of several other soil samples considered for various reasons to be of particular interest, such as orange soil 74220 and its companion 74240, Apollo 16 drill core sample 60002, and the apparently peculiar fillet soil 67461. Wherever possible, analyses were carried out by step-wise heating rather than by total pyrolysis. On the basis of the results of the investigation it is concluded that nitrogen isotope ratio determinations provide a usable method for determining cosmic-ray exposures for soils.
Becker, R. H.↗