Search NASA⌕ Search

SEARCH · Search NASA

Results for “isotopic discrimination”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

The effects of low- Z shielding on uranium isotope discrimination using the time-emission profiles of long-lived delayed neutrons

Characteristic radiation signals can often be obscured or distorted by relatively small amounts of shielding, as is the case for highly-enriched uranium (HEU). Methods that can detect and identify special nuclear material (SNM) even in the presence of shielding are therefore of high value in many nuclear security and nonproliferation applications. It has been previously shown that the buildup and decay time profiles of long-lived delayed neutron emission from induced fission are unique and can be used to successfully discriminate between uranium isotopes and infer enrichment without the need for a calibration standard. Because the long-lived delayed neutron precursors exhibit decay times on the order of tens of seconds, their time profiles are not sensitive to the delays associated with scattering or diffusion in shielding materials, which occur on much shorter time scales. The use of capture-based neutron detectors can also mitigate the effects of shielding, because unlike recoil-based detectors, they do not have a low-energy detection threshold, so that neutrons that lose their energy in the shielding are still detectable. In this work, the effects of low-Z shielding on the discrimination of uranium isotopes using delayed neutron time profile measurements are investigated for the first time. Furthermore, the delayed neutron buildup and decay time profiles of polyethylene-shielded HEU and depleted uranium objects are measured using two different capture-gated detector designs. The recorded profiles show good agreement with the shapes predicted from six-group delayed neutron models even with the shielding in place, and the enrichment of the HEU and DU objects was estimated accurately to within 5%. While this method shows potential for discriminating and characterizing extreme cases of enrichment when a moderate amount of shielding is present, simulation results suggest that significant limitations exist for intermediate enrichment levels due to distortions to the delayed neutron time profile caused by neutron reflection in the shielding.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Isotopic discrimination of natural and anthropogenic perchlorate sources in groundwater in a semi-arid region of northeastern Oregon (USA)

Perchlorate (ClO 4 - ) has synthetic and natural sources. Synthetic ClO 4 - is released to the environment from its use as an oxidant in military and aerospace applications, and from its presence in a variety of common commercial products, such as safety flares, chlorate herbicides, and fireworks. Natural sources of ClO 4 - in the environment include imported nitrate fertilizers derived from salt deposits in the Atacama Desert of Chile and indigenous natural ClO 4 - that accumulates in unsaturated soils and groundwaters in other arid and semi-arid environments, largely from atmospheric deposition. The stable isotope ratios of chlorine ( 37 Cl/ 35 Cl) and oxygen ( 18 O/ 16 O, 17 O/ 16 O) and the isotopic abundance of radioactive 36 Cl in ClO 4 - can be used to discriminate these different sources. Perchlorate was previously detected at relatively high concentrations (3.8–34.7 μg/L) in groundwater from many wells in the Boardman-Umatilla area near the Columbia River in northeastern Oregon, which is a semi-arid, highly agricultural, heavily irrigated area that includes several past and current military installations. Eight representative groundwater wells were sampled throughout this region and isotopic characteristics of ClO 4 - collected from each well were measured along with other chemical and isotopic parameters including tritium and other groundwater age indicators. We report isotopic data indicate that indigenous natural ClO 4 - was present in groundwater from all sampled wells and was the predominant source in five of the wells. Synthetic ClO 4 - was present in the three remaining wells with natural ClO 4 - , and a minor fraction of Atacama-fertilizer-derived ClO4- was indicated in one of the wells. Data from this study expand the geographic area of the USA in which indigenous natural ClO 4 - has been detected to include the semi-arid northwest. This study also illustrates the role of irrigation recharge as a mechanism for producing relatively high concentrations of indigenous natural ClO 4 - in groundwater by flushing accumulated salts from the unsaturated zone.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2003

Insights into the Processing of Carbon by Early Microbial Ecosystems

Interactions between Earth and the biosphere that were crucial for early biological evolution also influenced substantially the processes that circulate C between its reservoirs in the atmosphere, ocean, crust and mantle. The C-13 C-12 values of crustal carbonates and organics have recorded changes both in biological discrimination and in the relative rates of burial of organics and carbonates. A full interpretation of these patterns needs further isotopic studies of microbial ecosystems and individual anaerobes. Thus we measured carbon isotope discrimination during autotrophic and heterotrophic growth of pure cultures of sulfate-reducing bacteria and archaea (SRB and SRA). Discrimination during CO2 assimilation is significantly larger than during heterotrophic growth on lactate or acetate. SRB grown lithoautotrophically consumed less than 3% of available CO2 and exhibited substantial discrimination, as follows: Desulfobacterium autotrophicum (alpha 1.0100 to 1.0123), Desulfobacter hydrogenophilus (alpha = 0.0138), and Desulfotomuculum acetoxidans (alpha = 1.0310). Mixotrophic growth of Desulfovibrio desulfuricans on acetate and CO2 resulted in biomass with delta C-13 composition intermediate to that of the substrates. We have recently extended these experiments to include the thermophilic SRA Archeoglobus spp. Ecological forces also influence isotopic discrimination. Accordingly, we quantified the flow of C and other constituents in modern marine cyanobacterial mats, whose ancestry extends back billions of years. Such ecosystem processes shaped the biosignatures that entered sediments and atmospheres. At Guerrero Negro, BCS, Mexico, we examined mats dominated by Microcoleus (subtidal) and Lyngbya (intertidal to supratidal) cyanobacteria. During 24 hour cycles, we observed the exchange of O2 and dissolved inorganic C (DIC) between mats and the overlying water. Microcoleus mats assimilated near-equal amounts of DIC during the day as they released at night, but Lyngbya mats typically showed net uptake of DIC over the diel cycle. Patterns of O2 daytime release and nighttime uptake mirrored these DIC trends in both mat types. Nighttime DIC effluxes from Microcoleus mats were equivalent in the presence versus absence of O2, whereas nighttime DIC effluxes from Lyngbya mats dropped markedly in the absence of O2. Thus aerobic diagenesis was more important in Lyngbya mats than in Microcoleus mats, perhaps because trapped O2 bubbles persist only in Lyngbya mats at night and thus sustain populations of aerbes. In both mat types, effluxes of H2, CH4 and short-chain fatty acids were much greater at night in the absence of 02, emphasizing the importance of fermentation. Differences observed between Microcoleus versus Lyngbya mats forecast differences in their microbial populations and in their patterns of gene expression.

DesMarais, D.↗
DOE OSTI2021

Leaf 13 C data constrain the uncertainty of the carbon dynamics of temperate forest ecosystems

Stable carbon isotope discrimination occurred in plant biophysical and biogeochemical processes can help understand plant physiology and soil biogeochemistry with respect to carbon cycling. Here, we incorporated the photosynthetic carbon isotope discrimination into a process-based land surface model (iTEM) to test if stable carbon isotope composition (δ 13 C) can impose additional constraint on model parameters. Sequential data assimilation was implemented at six eddy covariance flux tower sites using carbon flux observations including gross primary productivity (GPP) and net ecosystem exchange (NEE) with and without considering foliar δ 13 C (δ 13 C f ) measurement constraints, respectively. Our model-data fusion showed that δ 13 C f can provide useful constraint on photosynthetic (V cmax25 , the maximum rate of carboxylation at 25°C) and stomatal (g1, the slope of stomatal function) parameters as well as the posterior carbon fluxes. When including δ 13 C f measurement, g1 spatially varies among the six sites and is significantly correlated with annual precipitation. We incorporated the statistical relationship between g1 and annual precipitation into iTEM, which is then used to quantify the regional carbon dynamic in temperate forest ecosystems of the Northern Hemisphere. Compared with the simulation only conditioned on carbon flux observations, regional carbon flux estimations performed slightly better against the FLUXCOM products and the uncertainties of modeled carbon fluxes were reduced by 27%. Our study demonstrated that δ 13 C f data constrains carbon flux uncertainties across space.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2003

Stable carbon isotope fractionation by sulfate-reducing bacteria

Biogeochemical transformations occurring in the anoxic zones of stratified sedimentary microbial communities can profoundly influence the isotopic and organic signatures preserved in the fossil record. Accordingly, we have determined carbon isotope discrimination that is associated with both heterotrophic and lithotrophic growth of pure cultures of sulfate-reducing bacteria (SRB). For heterotrophic-growth experiments, substrate consumption was monitored to completion. Sealed vessels containing SRB cultures were harvested at different time intervals, and delta(13)C values were determined for gaseous CO(2), organic substrates, and products such as biomass. For three of the four SRB, carbon isotope effects between the substrates, acetate or lactate and CO(2), and the cell biomass were small, ranging from 0 to 2 per thousand. However, for Desulfotomaculum acetoxidans, the carbon incorporated into biomass was isotopically heavier than the available substrates by 8 to 9 per thousand. SRB grown lithoautotrophically consumed less than 3% of the available CO(2) and exhibited substantial discrimination (calculated as isotope fractionation factors [alpha]), as follows: for Desulfobacterium autotrophicum, alpha values ranged from 1.0100 to 1.0123; for Desulfobacter hydrogenophilus, the alpha value was 0.0138, and for Desulfotomaculum acetoxidans, the alpha value was 1.0310. Mixotrophic growth of Desulfovibrio desulfuricans on acetate and CO(2) resulted in biomass with a delta(13)C composition intermediate to that of the substrates. The extent of fractionation depended on which enzymatic pathways were used, the direction in which the pathways operated, and the growth rate, but fractionation was not dependent on the growth phase. To the extent that environmental conditions affect the availability of organic substrates (e.g., acetate) and reducing power (e.g., H(2)), ecological forces can also influence carbon isotope discrimination by SRB.

Deltaproteobacteria/growth & development/metabolis↗
NASA NTRS1995

Global Analysis, Interpretation, and Modelling: First Science Conference

Topics considered include: Biomass of termites and their emissions of methane and carbon dioxide - A global database; Carbon isotope discrimination during photosynthesis and the isotope ratio of respired CO2 in boreal forest ecosystems; Estimation of methane emission from rice paddies in mainland China; Climate and nitrogen controls on the geography and timescales of terrestrial biogeochemical cycling; Potential role of vegetation feedback in the climate sensitivity of high-latitude regions - A case study at 6000 years B.P.; Interannual variation of carbon exchange fluxes in terrestrial ecosystems; and Variations in modeled atmospheric transport of carbon dioxide and the consequences for CO2 inversions.

Sahagian, Dork↗
NASA NTRS2006

Compound-specific Isotope Analysis of Cyanobacterial Pure cultures and Microbial Mats: Effects of Photorespiration?

Microbial mats are considered modern homologs of Precambrian stromatolites. The carbon isotopic compositions of organic matter and biomarker lipids provide clues to the depositional environments of ancient mat ecosystems. As the source of primary carbon fixation for over two billion years, an understanding of cyanobacterial lipid biosynthesis, associated isotopic discriminations, and the influence of physiological factors on growth and isotope expression is essential to help us compare modern microbial ecosystems to their ancient counterparts. Here, we report on the effects of photorespiration (PR) on the isotopic composition of cyanobacteria and biomarker lipids, and on potential PR effects associated with the composition of various microbial mats. The high light, high O2 and limiting CO2 conditions often present at the surface of microbial mats are known to support PR in cyanobacteria. The oxygenase function of ribulose bisphosphate carboxylase/oxygenase can result in photoexcretion of glycolate and subsequent degration by heterotrophic bacteria. We have found evidence which supports an isotopic depletion (increased apparent E) scaled to O2 level associated with growth of Phormidium luridum at low CO2 concentrations (less than 0.04%). Similar to previous studies, isotopic differences between biomass and lipid biomarkers, and between lipid classes were positively correlated with overall fractionation, and should provide a means of estimating the influence of PR on overall isotopic composition of microbial mats. Several examples of microbial mats growing in the hydrothermal waters of Yellowstone National Park and the hypersaline marine evaporation ponds at Guerrero Negro, Baja Sur Mexico will be compared with a view to PR as a possible explanation of the relatively heavy C-isotope composition of hypersaline mats.

Jahnke, L. L.↗
DOE OSTI2026

First field test of a novel optical gas analyser in the exhaust of Wendelstein 7-X

A novel optical gas analyser, designed for isotope-resolved exhaust composition measurement, was field-tested at Wendelstein 7-X (W7-X) to validate its laboratory-proven concept under operational fusion experiment conditions. The system, Optix, comprises a cold cathode remote plasma generator and a high-resolution Fabry–Perot spectrometer and was deployed in the exhaust line of W7-X during the OP2.3 campaign. The injection of 3 He and 4 He for minority ion-cyclotron heating provided a test case for helium isotope discrimination. Despite limitations due to background gas and low partial pressures of the target species, isotope-resolved spectral signatures were successfully observed, demonstrating the fundamental viability of the Optix approach. Additionally, the spectrometer was evaluated for plasma emission measurements from both core and edge sightlines. While helium line emission was detectable, interpretation was hindered by complex background signals, highlighting the benefits of controlled remote plasma generators for spectroscopy. This first deployment provides critical insight into pressure requirements, spectral resolution, and operational constraints, informing future applications of optical exhaust diagnostics in fusion devices.

magnetic confinement fusion↗
NASA NTRS1987

Natural abundances of carbon isotopes in acetate from a coastal marine sediment

Measurements of the natural abundances of carbon isotopes were made in acetate samples isolated from the anoxic marine sediment of Cape Lookout Bight, North Carolina. The typical value of the total acetate carbon isotope ratio (delta 13C) was -16.1 +/- 0.2 per mil. The methyl and carboxyl groups were determined to be -26.4 +/- 0.3 and -6.0 +/- 0.3 per mil, respectively, for one sample. The isotopic composition of the acetate is thought to have resulted from isotopic discriminations that occurred during the cycling of that molecule. Measurements of this type, which have not been made previously in the natural environment, may provide information about the dominant microbial pathways in anoxic sediments as well as the processes that influence the carbon isotopic composition of biogenic methane from many sources.

NASA Discipline Exobiology↗
DOE OSTI2021

Rubisco production in maize mesophyll cells through ectopic expression of subunits and chaperones

Abstract C4 plants, such as maize, strictly compartmentalize Rubisco to bundle sheath chloroplasts. The molecular basis for the restriction of Rubisco from the more abundant mesophyll chloroplasts is not fully understood. Mesophyll chloroplasts transcribe the Rubisco large subunit gene and, when normally quiescent transcription of the nuclear Rubisco small subunit gene family is overcome by ectopic expression, mesophyll chloroplasts still do not accumulate measurable Rubisco. Here we show that a combination of five ubiquitin promoter-driven nuclear transgenes expressed in maize leads to mesophyll accumulation of assembled Rubisco. These encode the Rubisco large and small subunits, Rubisco assembly factors 1 and 2, and the assembly factor Bundle sheath defective 2. In these plants, Rubisco large subunit accumulates in mesophyll cells, and appears to be assembled into a holoenzyme capable of binding the substrate analog CABP (carboxyarabinitol bisphosphate). Isotope discrimination assays suggest, however, that mesophyll Rubisco is not participating in carbon assimilation in these plants, most probably due to a lack of the substrate ribulose 1,5-bisphosphate and/or Rubisco activase. Overall, this work defines a minimal set of Rubisco assembly factors in planta and may help lead to methods of regulating the C4 pathway.

Plant Sciences↗
NASA NTRS2022

Estimating Emissions of Methane Consistent with Atmospheric Measurements of Methane and δC-13 of Methane

We have constructed an atmospheric inversion framework based on TM5-4DVAR to jointly assimilate measurements of methane and δC-13 of methane in order to estimate source-specific methane emissions. Here we present global emission estimates from this framework for the period 1999–2016. We assimilate a newly constructed, multi-agency database of CH4 and δC-13 measurements. We find that traditional CH4-only atmospheric inversions are unlikely to estimate emissions consistent with atmospheric δC-13 data and assimilating δC-13 data is necessary to derive emissions consistent with both measurements. Our framework attributes ca. 85% of the post-2007 growth in atmospheric methane to microbial sources, with about half of that coming from the tropics between 23.5° N and 23.5° S. This contradicts the attribution of the recent growth in the methane budget of the Global Carbon Project (GCP). We find that the GCP attribution is only consistent with our top-down estimate in the absence of δC-13 data. We find that at global and continental scales, δC-13 data can separate microbial from fossil methane emissions much better than CH4 data alone, and at smaller scales this ability is limited by the current δC-13 measurement coverage. Finally, we find that the largest uncertainty in using δC-13 data to separate different methane source types comes from our knowledge of atmospheric chemistry, specifically the distribution of tropospheric chlorine and the isotopic discrimination of the methane sink.

Methane↗
DOE OSTI2025

Photon counting with intensified charge coupled device (ICCD) – II. Laser induced breakdown spectroscopy (LIBS) spectral measurement

This study explores the application of photon counting (PC) to enhance the resolution of spectra acquired by an intensified charge-coupled device (ICCD) detector, with a focus on analytical atomic emission spectrometry using laser-induced breakdown spectroscopy (LIBS) as a use-case example. It demonstrates that, for spectra obtained with the same spectrometer–ICCD system, PC provides higher spectral resolution compared to conventional analog detector readout. This enhancement is particularly evident in the line wings of spectral peaks, facilitating better discrimination of isotopic peaks in the measured spectra. Although PC does not improve the resolution of an optical spectrometer directly, it rectifies the resolution lost caused by signal spreading in conventional ICCD analog measurement. However, similar to other counting techniques, excessive photons compromise detector linearity due to signal pileup. A correction model is proposed to mitigate the pileup effect, resulting in improved linearity and dynamic range in PC measurements. Additionally, the study reveals unexpected periodic structures in the flatfield image of the ICCD, which cause non-uniform detector gain in conventional analog as well as PC measurement modes and must be addressed for high-precision measurements.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Increased bundle‐sheath leakiness of CO 2 during photosynthetic induction shows a lack of coordination between the C 4 and C 3 cycles

Summary Use of a complete dynamic model of NADP‐malic enzyme C 4 photosynthesis indicated that, during transitions from dark or shade to high light, induction of the C 4 pathway was more rapid than that of C 3 , resulting in a predicted transient increase in bundle‐sheath CO 2 leakiness ( ϕ ). Previously, ϕ has been measured at steady state; here we developed a new method, coupling a tunable diode laser absorption spectroscope with a gas‐exchange system to track ϕ in sorghum and maize through the nonsteady‐state condition of photosynthetic induction. In both species, ϕ showed a transient increase to > 0.35 before declining to a steady state of 0.2 by 1500 s after illumination. Average ϕ was 60% higher than at steady state over the first 600 s of induction and 30% higher over the first 1500 s. The transient increase in ϕ , which was consistent with model prediction, indicated that capacity to assimilate CO 2 into the C 3 cycle in the bundle sheath failed to keep pace with the rate of dicarboxylate delivery by the C 4 cycle. Because nonsteady‐state light conditions are the norm in field canopies, the results suggest that ϕ in these major crops in the field is significantly higher and energy conversion efficiency lower than previous measured values under steady‐state conditions.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Data for Increased bundle sheath leakiness of CO2 during photosynthetic induction shows a lack of coordination between the C4 and C3 cycles

We developed a new application of isotopic gas exchange which couples a tunable diode laser absorption spectroscope (TDL) with a leaf gas exchange system, analyzing leakiness through induction of C4 photosynthesis on dark to high-light transitions. The youngest fully expanded leaf was measured on 40-45 day-old maize(B73) and sorghum (Tx430). Detail definition of each variable in raw Li-6400XT and Li-6800 (in "Original_data_AND_Data_processing_code.zip") is summarized in: https://www.licor.com/env/support/LI-6800/topics/symbols.html#const

bundle sheath leakage↗
DOE OSTI2023

CO 2 electroreduction favors carbon isotope 12 C over 13 C and facilitates isotope separation

We discovered that CO 2 electroreduction strongly favors the conversion of the dominant isotope of carbon ( 12 C) and discriminates against the less abundant, stable carbon 13 C isotope. Both absorption of CO 2 in the alkaline electrolyte and CO 2 electrochemical reduction favor the lighter isotopologue. As a result, the stream of unreacted CO 2 leaving the electrolyzer has an increased 13 C content, and the depletion of 13 C in the product is several times greater than that of photosynthesis. Using a natural abundance feed, we demonstrate enriching of the 13 C fraction to ~1.3% (i.e., +18%) in a single-pass reactor and propose a scalable and economically attractive process to yield isotopes of a commercial purity. Our finding opens pathways to both cheaper and less energy-intensive production of stable isotopes ( 13 C, 15 N) essential to the healthcare and chemistry research, and to an economically viable, disruptive application of electrolysis technologies developed in the context of sustainability transition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Neutron Coincidence Measurements of Uranium-233 Oxide

Renewed international interest in thorium-fueled advanced reactors has challenged the safeguards community to address future proliferation concerns. Thorium-based technology presents many benefits but does not eliminate the proliferation risks associated with producing and processing fissile material. A byproduct of thorium-fueled reactors is uranium-233, which is classified as a direct-use material. As a result, the development of new or improved methods to characterize and measure materials containing 233U must mirror the pace of development of reactors and facilities that produce such material. Research is underway to assess, develop, and test approaches for safeguarding nuclear materials within the thorium fuel cycle. Neutron signatures from the nondestructive assay (NDA) of materials containing 233U are being quantified to inform the potential characterization of these materials. Using a traditional neutron coincidence counter and a series of well-documented 233U oxide samples, initial measurements have been made to assess the feasibility of 233U characterization and discrimination from other uranium isotopes, primarily 235U, using a combination of measurement techniques and analysis methods. Data acquisition is performed in list mode, allowing for a variety of analyses to be performed on the raw data that is not available using traditional shift register technology. Measurements were performed in passive and active configurations to quantify the strength of signal and to validate simulations in support of this work. This paper presents and discusses the results of the initial measurements of 233U oxide performed at Oak Ridge National Laboratory.

Lockhart, Madeline↗