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At least 775 records · Page 43

Short-lived noble gas effluent trends from a research reactor

An understanding of anthropogenic sources of radioactive noble gases in the atmosphere is needed to enhance the discrimination ability of the International Monitoring System's sensors. These sources include commercial and research nuclear reactors and medical isotope production facilities. While abiding by local environmental ordinances these facilities all emit noble gas radioisotopes through normal operation. Here, this research presents measurements and analysis of noble gas isotopes ( 41 Ar, 135 Xe, 135m Xe, 137 Xe, 138 Xe, 87 Kr, 88 Kr, and 89 Kr) made directly at the stack of the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory. The Xe and Kr noble gases are concurrently observed with 41 Ar, a neutron activation product, when the reactor is operational. The magnitude of the Xe and Kr noble gases released is not constant over the HFIR cycle, but they temporally match the 41 Ar trend. An isotope activity ratio analysis of these shorter lived isotopes combined with the observation of the cycle's temporal trend helps understand the noble gas production mechanism at the HFIR. Isotopes with short half-lives are not useful for long-range environmental monitoring. However, these measurements could potentially be combined with atmospheric modeling to predict the background source term of the longer-lived Xe ratios at a monitoring station.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Determination of the isotopic composition of atmospheric methane and its application in the Antarctic

A procedure for establishing the C-13/C-12 ratio and the C-14 abundance in the atmospheric methane is discussed. The method involves air sample collection, measurement of the methane mixing ratio by gas chromotography followed by quantitative conversion of the methane in the air samples to CO2 and H2O, and analysis of the resulting CO2 for the C-13/C-12 ratio by stable isotope ratio mass spectrometry and measurement of C-14 content by accelerator mass spectrometry. The carbon isotropic composition of methane in air collected at Baring Head, New Zealand, and in air collected on aircraft flights between New Zealand and Antarctica is determined by the method, and no gradient in the composition between Baring Head and the South Pole station is found. As the technique is refined, and more data is gathered, small seasonal and long-term variations in C-13 are expected to be resolved.

Lowe, David C.↗

Isotopes of titanium in cool stars

A program of stellar Ti isotopic-abundance determinations is described and related to changes that may have occurred in the Ti isotopic abundance ratios during the chemical evolution of the Galaxy, and to whether the abundance ratios are perturbed in the S and MS stars having atmospheres with enhanced abundances of s-process nuclei resulting from convective mixing after internal exposure to neutrons. High-resolution (0.07 A) Reticon spectra of portions of the TiO gamma (0,0), gamma (0,1), and delta (0,0) bands were the source material, and particular emphasis was placed on the definition of the continuum level. The isotopic abundance ratios are terrestrial in all of the sample, and errors in the (Ti-i)/(Ti-48) ratio are typically plus or minus 25% for the dwarfs and plus or minus 50% for the giants. The observations show that the magic nucleus Ti-50 is not enhanced in S and MS stars.

Clegg, R. E. S.↗

The C-12/C-13 ratio in stellar atmospheres. II - CN and CO in alpha Orionis

The isotopic abundance ratio C-12/C-13 for the M supergiant alpha Orionis is derived from photoelectric high-resolution scans of the CN 2-0 red system and high-resolution interferometric spectra of the CO second-overtone bands. The two molecules yield consistent results and the final value for the C-12/C-13 ratio is 7.0 plus or minus 1.5. Rationale is offered for the causes contributing to an earlier suggestion that C-12/C-13 ratios from CO and CN were in disagreement.

Lambert, D. L.↗

Origin of Plutonium-244 in the Early Solar System

We investigate the origin in the early Solar System of the short-lived radionuclide 244 Pu (with a half life of 80 Myr) produced by the rapid (r) neutron-capture process. We consider two large sets of r-process nucleosynthesis models and analyse if the origin of 244 Pu in the ESS is consistent with that of the other r and slow (s) neutron-capture process radioactive nuclei. Uncertainties on the r-process models come from both the nuclear physics input and the astrophysical site. The former strongly affects the ratios of isotopes of close mass ( 129 I/ 127 I, 244 Pu/ 238 U, and 247 Pu/ 235 U). The 129 I/ 247 Cm ratio, instead, which involves isotopes of a very different mass, is much more variable than those listed above and is more affected by the physics of the astrophysical site. We consider possible scenarios for the evolution of the abundances of these radioactive nuclei in the galactic interstellar medium and verify under which scenarios and conditions solutions can be found for the origin of 244 Pu that are consistent with the origin of the other isotopes. Solutions are generally found for all the possible different regimes controlled by the interval (δ) between additions from the source to the parcel of interstellar medium gas that ended up in the Solar System, relative to decay timescales. If r-process ejecta in interstellar medium are mixed within a relatively small area (leading to a long δ), we derive that the last event that explains the 129 I and 247 Cm abundances in the early Solar System can also account for the abundance of 244 Pu. Due to its longer half life, however, 244 Pu may have originated from a few events instead of one only. If r-process ejecta in interstellar medium are mixed within a relatively large area (leading to a short δ), we derive that the time elapsed from the formation of the molecular cloud to the formation of the Sun was 9-16 Myr.

79 ASTRONOMY AND ASTROPHYSICS↗

Identification of Martian Regolith Sulfur Components in Shergottites Using Sulfur K Xanes and Fe/S Ratios

Based on isotopic anomalies in Kr and Sm, Sr-isotopes, S-isotopes, XANES results on S-speciation, Fe/S ratios in sulfide immiscible melts [5], and major element correlations with S determined in impact glasses in EET79001 Lith A & Lith B and Tissint, we have provided very strong evidence for the occurrence of a Martian regolith component in some impact melt glasses in shergottites. Using REE measurements by LA-ICP-MS in shergottite impact glasses, Barrat and co-workers have recently reported conflicting conclusions about the occurrence of Martian regolith components: (a) Positive evidence was reported for a Tissint impact melt, but (b) Negative evidence for impact melt in EET79001 and another impact melt in Tissint. Here, we address some specific issues related to sulfur speciation and their relevance to identifying Martian regolith components in impact glasses in EET79001 and Tissint using sulfur K XANES and Fe/S ratios in sulfide immiscible melts. XANES and FE-SEM measurements in approx. 5 micron size individual sulfur blebs in EET79001 and Tissint glasses are carried out by us using sub-micron size beams, whereas Barrat and coworkers used approx. 90 micron size laser spots for LA- ICP-MS to determine REE abundances in bulk samples of the impact melt glasses. We contend that Martian regolith components in some shergottite impact glasses are present locally, and that studying impact melts in various shergottites can give evidence both for and against regolith components because of sample heterogeneity.

Sutton, S. R.↗

Organosulfur Aerosols Likely Carried Sulfur MIF Signatures in the Early Earth’s Atmosphere

Signatures of mass-independent fractionation (MIF) of sulfur in Archean sulfide and sulfate minerals are widely thought to record an anoxic early Earth’s atmosphere. While experiments of ultraviolet irradiation of SO 2 produce significant sulfur mass-independent fractionation (S-MIF) in reaction products (elemental sulfur and residual sulfur dioxide), they have not been able to reproduce the isotope patterns, in particular Δ 36 S/Δ 33 S ratios, observed in the geologic rock record. Studies that focused on organic sulfur gases and hazes in Archean did not report organosulfur aerosol photoproducts as major contributors to Archean S-MIF chemistry. Here we show, for the first time, that photochemical reactions of SO 2 in the presence of gaseous hydrocarbons (CH 4 , C 2 H 2 , and C 2 H 4 ) produce haze-like organosulfur aerosols bearing S-MIF with variable Δ 36 S/Δ 33 S ratios. The isotope trends for the organosulfur photoproducts produced in our experiments suggest that in addition to elemental sulfur, organosulfur compounds—in particular methanesulfonic acid—are a key component of S-MIF signals from the atmosphere to the ocean and sediments with possible links to Archean atmosphere warmed by a methane greenhouse.

54 ENVIRONMENTAL SCIENCES↗

Observation of J = 1-0 emission from H/N-15/C

Emission from the J = 1-0 transition of H(N-15)C has been detected in the direction of DR21(OH). The transition frequency of 88,865.69 MHz was measured in the laboratory by microwave absorption spectroscopy. The computed N-15/C-13 isotopic abundance ratio of 1.01 for DR21(OH) is larger than those calculated from isotopes of HCN in other interstellar clouds, perhaps implying a localized enrichment in N-15 in DR21(OH).

Brown, R. D.↗

A new HALEU isotopic certified reference material

Candidate certified reference material (CRM) U196 was prepared by gravimetrically mixing and dissolving NNSA NRMP CRM 112-A (natural uranium metal) and CRM 116-A (highly enriched 93.2% 235 U metal) to achieve a high-assay low-enriched uranium (HALEU) isotopic abundance reference material. CRM U196 will be certified for the 233 U/ 238 U, 234 U/ 238 U, 235 U/ 238 U, and 236 U/ 238 U ratios. Gravimetrically determined uranium isotope amount ratios and values derived from the isotope data were calculated from the buoyancy corrected mass data and from certified values for the metal CRMs used to create the solution. The 235 U isotope amount fraction (·100) and expanded uncertainty is 19.5846 ± 0.0028. For attribute verification, total evaporation and modified total evaporation isotope ratio measurements were performed. In conclusion, the reference material is to be distributed as a unit containing 5 mg uranium as dry uranyl nitrate.

High-assay low-enriched uranium↗

An investigation of techniques for the measurement and interpretation of cosmic ray isotopic abundances

An instrument, the Caltech High Energy Isotope Spectrometer Telescope was developed to measure isotopic abundances of cosmic ray nuclei by employing an energy loss - residual energy technique. A detailed analysis was made of the mass resolution capabilities of this instrument. A formalism, based on the leaky box model of cosmic ray propagation, was developed for obtaining isotopic abundance ratios at the cosmic ray sources from abundances measured in local interstellar space for elements having three or more stable isotopes, one of which is believed to be absent at the cosmic ray sources. It was shown that the dominant sources of uncertainty in the derived source ratios are uncorrelated errors in the fragmentation cross sections and statistical uncertainties in measuring local interstellar abundances. These results were applied to estimate the extent to which uncertainties must be reduced in order to distinguish between cosmic ray production in a solar-like environment and in various environments with greater neutron enrichments.

Wiedenbeck, M. E.↗

Lower limit to the interstellar C 12/C 13 ratio in the direction of 20 Tauri.

Results of photoelectric scanning of the spectrum of 20 Tau in the vicinity of 4232 A of interstellar CH(+). From the observed absence of the isotopically shifted line of super 13CH(+) it is deduced that the C 12/C 13 isotopic abundance ratio in this direction is greater than 33, and hence consistent with the terrestrial value.

Vanden Bout, P.↗

Analyzers Measure Greenhouse Gases, Airborne Pollutants

In complete darkness, a NASA observatory waits. When an eruption of boiling water billows from a nearby crack in the ground, the observatory s sensors seek particles in the fluid, measure shifts in carbon isotopes, and analyze samples for biological signatures. NASA has landed the observatory in this remote location, far removed from air and sunlight, to find life unlike any that scientists have ever seen. It might sound like a scene from a distant planet, but this NASA mission is actually exploring an ocean floor right here on Earth. NASA established a formal exobiology program in 1960, which expanded into the present-day Astrobiology Program. The program, which celebrated its 50th anniversary in 2010, not only explores the possibility of life elsewhere in the universe, but also examines how life begins and evolves, and what the future may hold for life on Earth and other planets. Answers to these questions may be found not only by launching rockets skyward, but by sending probes in the opposite direction. Research here on Earth can revise prevailing concepts of life and biochemistry and point to the possibilities for life on other planets, as was demonstrated in December 2010, when NASA researchers discovered microbes in Mono Lake in California that subsist and reproduce using arsenic, a toxic chemical. The Mono Lake discovery may be the first of many that could reveal possible models for extraterrestrial life. One primary area of interest for NASA astrobiologists lies with the hydrothermal vents on the ocean floor. These vents expel jets of water heated and enriched with chemicals from off-gassing magma below the Earth s crust. Also potentially within the vents: microbes that, like the Mono Lake microorganisms, defy the common characteristics of life on Earth. Basically all organisms on our planet generate energy through the Krebs Cycle, explains Mike Flynn, research scientist at NASA s Ames Research Center. This metabolic process breaks down sugars for energy to fuel cellular functions. "We think this chemical process did not exist when life first formed on Earth," he says, "because it is based on oxygen being available, and there was little oxygen available on the early Earth." It is possible that there are anaerobic regions beneath the sea floor in which life forms like those early non-Krebs Cycle microbes may yet exist. To detect and potentially collect samples of life emerging from hydrothermal vents, Flynn and his colleagues created Medusa, a multi-sensor instrument designed for long-term observation of diked vents on the ocean floor. When the vents erupt, Medusa assesses indicators of life within the expelled water. If the results are positive, the observatory collects samples and detaches from the ocean floor, making the long journey to the surface for retrieval by scientists. One of the indicators Medusa measures is the ratio of carbon isotopes in the water, namely carbon-12 and carbon-13. Living organisms preferentially take up carbon-12, Flynn says, so examining the ratio of these isotopes can help to determine the source of carbon in an environment as either biological or non-biological. "On Mars, there is evidence of localized methane in the atmosphere, and that methane could come from biological sources or from geochemical ones," Flynn says. "Determining the background planetary carbon isotope ratios and then evaluating the specific carbon ratios in this methane would help to determine how it was formed." A long-duration observatory similar to Medusa could one day provide essential evidence for or against the presence of life on the Red Planet or beneath the ice-crusted oceans of Europa.

Source record↗

Probing Neodymium Isotopic Variations in the Inner Solar System

One of the key problems in planetary science is the identification of the building blocks of Earth, and whether they exist within our current collection of meteorites. Stable mass independent isotopic anomalies, usually nucleosynthetic in origin, are a key tool in fingerprinting material coming from different accretionary regions within the protoplanetary disk. For a number of isotopic systems such as O, Ni, Ti and Cr, enstatite chondrites (EC) appear to be the strongest candidates for Earth's building blocks, despite their low Mg/Si ratios relative to the bulk Earth. It has been proposed that Earth, the Moon-forming impactor and enstatite chondrites all were originally sourced from the same reservoir in the protoplanetary disk, but subsequently experienced divergent chemical evolution pathways. This was recently challenged by who used the correlation between Mo and Nd isotopes in bulk meteorites to argue that such a reservoir does not exist as the isotopic composition of enstatite chondrites is resolvable from Earth. However, in detail the Nd isotopic ratios of EC ((142)Nd/(144)Nd, (148)Nd/(144)Nd, (150)Nd/(144)Nd) show considerable variability, and overlap significantly with the isotopic composition of both the bulk Earth and ordinary chondrites (OC). previously identified Nd isotopic variability in EC, linking it to the degree of equilibration the meteorite had experienced, however they only focused on collecting high precision (142)Nd/(144)Nd, which also has contributions from the decay of the short-lived Sm-146 nuclide (t(sub 1/2) ~103 Myr), making identification of nucleosynthetic anomalies less clear. While the study of reports all the Nd isotopic ratios measured at high precision, only equilibrated EC were analyzed. Therefore, with the currently published data it is unclear to what extent thermal equilibration in the EC is responsible for the variation observed in the stable Nd isotopic ratios, and whether the EC reservoir can be resolved from Earth. In order to better understand the genetic relationship between enstatite chondrites and the Earth we are carrying out a more systematic study including both equilibrated and unequilibrated enstatite chondrites, focusing on high precision analysis of all the stable Nd isotopic ratios.

SOLAR SYSTEM↗

Isotopic Heterogeneity Imaged in a Uranium Fuel Pellet with Extreme Ultraviolet Laser Ablation and Ionization Time-of-Flight Mass Spectrometry

We use extreme ultraviolet laser ablation and ionization time-of-flight mass spectrometry (EUV TOF) to map uranium isotopic heterogeneity at the nanoscale (=100 nm). Using low-enriched uranium fuel pellets that were made by blending two isotopically distinct feedstocks, we show that EUV TOF can map the 235U/238U content in 100 nm-sized pixels. The two-dimensional (2D) isotope maps reveal U ratio variations in sub-microscale to =1 µm areas of the pellet that had not been fully exposed by microscale or bulk mass spectrometry analyses. Compared to the ratio distribution measured in a homogeneous U reference material, the ratios in the enriched pellet follow a ~3× wider distribution. These results indicate U heterogeneity in the fuel pellet from incomplete blending of the different source materials. EUV TOF results agree well with those obtained on the same enriched pellets by nanoscale secondary ionization mass spectrometry (NanoSIMS), which reveals a comparable U isotope ratio distribution at the same spatial scale. EUV TOF’s ability to assess and map isotopic heterogeneity at the nanoscale makes it a promising tool in fields such as nuclear forensics, geochemistry, and biology that could benefit from uncovering sub-microscale sources of chemical modifications.

Rush, Lydia A.↗

Limits to the fractionation of isotopes in the solar wind as observed with SOHO/CELIAS/MTOF

Observations of isotope fractionation in the solar wind for the Mg and Ne elements are reported on the basis of measurements performed by the mass time of flight (MTOF) sensor of the charge, element, and isotope analysis system (CELIAS) onboard the SOHO spacecraft. Their isotopic abundance ratios are shown to vary by (0.8+/-0.6) amu in the solar wind bulk velocity range from 350 km/s to 650 km/s. A good correlation is noticed between the isotope fractionation and the elemental fractionation 4He/1H in the solar wind. The results were discussed in the context of recent theoretical models, which predict isotope fractionation in the solar wind by variable Coulomb friction in several solar wind regimes.

Kallenbach, R.↗

Solar helium and neon in the Earth

Neon isotopic compositions in mantle-derived samples commonly are enriched in (20)Ne and (21)Ne relative to (22)Ne compared with atmospheric neon ((20)Ne/(22)Ne and (21)Ne/(22)Ne ratios in atmospheric neon are 9.8 and 0.029, respectively), together with significant primordial (3)He. Such results have been obtained on MORB's, intraplate plume-related oceanic island basalts, backarc basin basalts, mantle xenoliths, ancient diamonds and CO2 well gases (e.g., 1 - 8). The highest (20)Ne/(22)Ne ratio observed in MORB glasses (= 13.6 plus or minus 1.3 is close to the solar value (= 13.6, as observed in solar wind). In order to explain the enrichment of (20)Ne and (21)Ne relative to atmospheric neon for samples derived from the mantle, it is necessary to postulate the presence of at least two distinct non-atmospheric components. The two most likely candidates are solar and nucleogenic ((20)Ne/(22)Ne solar = 13.6 (21)Ne/(22)Ne solar = 0.032, (20)Ne/(22)Ne nucleogenic = 2.5 and (21)Ne/(22)Ne nucleogenic = 32). This is because solar neon is the only known component with a (20)Ne/(22)Ne ratio greater than both the atmospheric value and that observed in samples derived from the mantle. Nucleogenic neon is well known to elevate (21)Ne/(22)Ne ratios. Neon isotopic signatures observed in mantle-derived samples can be accounted for by mixing of the three neon end members: solar, nucleogenic and atmospheric.

Honda, M.↗

Solar-type xenon - Isotopic abundances in Pesyanoe

Elemental and isotopic abundances of Ar and Xe were measured in three grain-size separates in the dark phase of the enstatite achondrite Pesyanoe by stepwise heating, using a combination of pyrolysis and combustion steps. The data reveal a low-temperature gas fraction with Ar/Xe ratios close to the solar ratio and isotopically similar to solar-type Ar and Xe observed in lunar samples. The gas released at intermediate temperature steps shows that Ar and Xe are isotopically fractionated, compared to the low-temperature components. Pesyanoe does not have excess Ar-40 and fission Xe, which means its parent body was too small for ion reimplantation. It is concluded that solar-type Xe isotopic abundances can be inferred from the low-temperature component. A comparison of Pesyanoe and lunar data shows that isotopic signatures of solar-wind Xe, as sampled at two different points in solar system space and time, are identical within experimental error.

Kim, J. S.↗