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At least 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
NASA NTRS2011

Hydrogen Isotope Measurements of Organic Acids and Alcohols by Pyrolysis-GC-MS-TC-IRMS

One possible process responsible for methane generation on Mars is abiotic formation by Fischer-Tropsch-type (FTT) synthesis during serpentinization reactions. Measurement of carbon and hydrogen isotopes of intermediary organic compounds can help constrain the origin of this methane by tracing the geochemical pathway during formation. Of particular interest within the context of this work is the isotopic composition of organic intermediaries produced on the surfaces of mineral catalysts (i.e. magnetite) during hydrothermal experiments, and the ability to make meaningful and reproducible hydrogen isotope measurements. Reported here are results of experiments to characterize the hydrogen isotope composition of low molecular weight organic acids and alcohols. The presence of these organic compounds has been suggested by others as intermeadiary products made during mineral surface catalyzed reactions. This work compliments our previous study characterizing the carbon isotope composition of similar low molecular weight intermediary organic compounds (Socki, et al, American Geophysical Union Fall meeting, Abstr. #V51B-2189, Dec., 2010). Our hydrogen isotope measurements utilize a unique analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-High Temperature Conversion-Isotope Ratio Mass Spectrometry (Py-GC-MS-TC-IRMS). Our technique is unique in that it carries a split of the pyrolyzed GC-separated product to a Thermo DSQ-II? quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of separated organic compounds, therefore both chemical and isotopic measurements can be carried out simultaneously on the same sample.

Socki, Richard A.↗
NASA NTRS2012

Hydrogen Isotope Measurements of Organic Acids and Alcohols by Pyrolysis-GC-MS-TC-IRMS: Application to Analysis of Experimentally Derived Hydrothermal Mineral-Catalyzed Organic Products

We report results of experiments to measure the H isotope composition of organic acids and alcohols. These experiments make use of a pyroprobe interfaced with a GC and high temperature extraction furnace to make quantitative H isotope measurements. This work compliments our previous work that focused on the extraction and analysis of C isotopes from the same compounds [1]. Together with our carbon isotope analyses our experiments serve as a "proof of concept" for making C and H isotope measurements on more complex mixtures of organic compounds on mineral surfaces in abiotic hydrocarbon formation processes at elevated temperatures and pressures. Our motivation for undertaking this work stems from observations of methane detected within the Martian atmosphere [2-5], coupled with evidence showing extensive water-rock interaction during Mars history [6-8]. Methane production on Mars could be the result of synthesis by mineral surface-catalyzed reduction of CO2 and/or CO by Fischer-Tropsch Type (FTT) reactions during serpentization [9,10]. Others have conducted experimental studies to show that FTT reactions are plausible mechanisms for low-molecular weight hydrocarbon formation in hydrothermal systems at mid-ocean ridges [11-13]. Our H isotope measurements utilize an analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-High Temperature Conversion-Isotope Ratio Mass Spectrometry (Py-GC-MS-TC-IRMS). This technique is designed to carry a split of the pyrolyzed GC-separated product to a Thermo DSQII quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of separated organic compounds, therefore both chemical and isotopic measurements can be carried out simultaneously on the same sample.

Socki, Richard A.↗
NASA NTRS2013

Potassium Isotopic Compositions of NIST Potassium Standards and 40Ar/39Ar Mineral Standards

Knowledge of the isotopic ratios of standards, spikes, and reference materials is fundamental to the accuracy of many geochronological methods. For example, the 238U/235U ratio relevant to U-Pb geochronology was recently re-determined [1] and shown to differ significantly from the previously accepted value employed during age determinations. These underlying values are fundamental to accurate age calculations in many isotopic systems, and uncertainty in these values can represent a significant (and often unrecognized) portion of the uncertainty budget for determined ages. The potassium isotopic composition of mineral standards, or neutron flux monitors, is a critical, but often overlooked component in the calculation of K-Ar and 40Ar/39Ar ages. It is currently assumed that all terrestrial materials have abundances indistinguishable from that of NIST SRM 985 [2]; this is apparently a reasonable assumption at the 0.25per mille level (1σ) [3]. The 40Ar/39Ar method further relies on the assumption that standards and samples (including primary and secondary standards) have indistinguishable 40K/39K values. We will present data establishing the potassium isotopic compositions of NIST isotopic K SRM 985, elemental K SRM 999b, and 40Ar/39Ar biotite mineral standard GA1550 (sample MD-2). Stable isotopic compositions (41K/39K) were measured by the peak shoulder method with high resolution MC-ICP-MS (Thermo Scientific NEPTUNE Plus), using the accepted value of NIST isotopic SRM 985 [2] for fractionation [4] corrections [5]. 40K abundances were measured by TIMS (Thermo Scientific TRITON), using 41K/39K values from ICP-MS measurements (or, for SRM 985, values from [2]) for internal fractionation corrections. Collectively these data represent an important step towards a metrologically traceable calibration of 40K concentrations in primary 40Ar/39Ar mineral standards and improve uncertainties by ca. an order of magnitude in the potassium isotopic compositions of standards.

Morgan, Leah↗
NASA NTRS2016

How Will Sea Ice Loss Affect the Greenland Ice Sheet? On the Puzzling Features of Greenland Ice-Core Isotopic Composition

The modern cryosphere, Earth's frozen water regime, is in fast transition. Greenland ice cores show how fast theses changes can be, presenting evidence of up to 15 C warming events over timescales of less than a decade. These events, called Dansgaard/Oeschger (D/O) events, are believed to be associated with rapid changes in Arctic sea ice, although the underlying mechanisms are still unclear. The modern demise of Arctic sea ice may, in turn, instigate abrupt changes on the Greenland Ice Sheet. The Arctic Sea Ice and Greenland Ice Sheet Sensitivity (Ice2Ice Chttps://ice2ice.b.uib.noD) initiative, sponsored by the European Research Council, seeks to quantify these past rapid changes to improve our understanding of what the future may hold for the Arctic. Twenty scientists gathered in Copenhagen as part of this initiative to discuss the most recent observational, technological, and model developments toward quantifying the mechanisms behind past climate changes in Greenland. Much of the discussion focused on the causes behind the changes in stable water isotopes recorded in ice cores. The participants discussed sources of variability for stable water isotopes and framed ways that new studies could improve understanding of modern climate. The participants also discussed how climate models could provide insights into the relative roles of local and nonlocal processes in affecting stable water isotopes within the Greenland Ice Sheet. Presentations of modeling results showed how a change in the source or seasonality of precipitation could occur not only between glacial and modern climates but also between abrupt events. Recent fieldwork campaigns illustrate an important role of stable isotopes in atmospheric vapor and diffusion in the final stable isotope signal in ice. Further, indications from recent fieldwork campaigns illustrate an important role of stable isotopes in atmospheric vapor and diffusion in the final stable isotope signal in ice. This feature complicates the quantitative interpretation of ice core signals but also makes the stable ice isotope signal a more robust regional indicator of climate, speakers noted. Meeting participants agreed that to further our understanding of these relationships, we need more process-focused field and laboratory campaigns.

Greenland↗
NASA NTRS2017

Ti Isotopes: Echoes of Grain-Scale Heterogenaity in the Protoplanetary Disk

Calcium-aluminum-rich inclusions (CAIs) are the oldest surviving solids to have formed in the Solar System. Their chemical and isotopic compositions provide a record of the conditions present in the protoplanetary disk where they formed and can aid our understanding of how solids formed in the solar nebula, an important step in the eventual process of planet building. The isotopic compositions of CAIs are primarily controlled by volatility. Evaporation/sublimation are well understood through both theory and experimental work to produce an enrichment in the heavy isotopes of an element, but less is understood about the effects of condensation. Mass-dependent fractionation can potentially provide a record of nebular condensation. Ti is not likely to experience evaporation due to its refractory nature, making it a useful tool for assessing the effects of condensation. We have undertaken a study of the stable isotope fractionation of Ti isotopes as a tracer of processes that predate the last evaporation events affecting CAIs. We compare the 49Ti/47Ti stable isotope ratio with excess 50Ti common in CAIs. We have collected Ti, Mg, Si, and Ca isotope data for a suite of CAIs in order to search for heterogeneity in each of these isotope systems, and for potential correlations among them. We compare our results to expectations for condensation.

Jordan, M. K.↗
NASA NTRS2014

A Novel Framework for Quantifying past Methane Recycling by Sphagnum-Methanotroph Symbiosis Using Carbon and Hydrogen Isotope Ratios of Leaf Wax Biomarkers

The concentration of atmospheric methane is strongly linked to variations in Earth's climate. Currently, we can directly reconstruct the total atmospheric concentration of methane, but not individual terms of the methane cycle. Northern wetlands, dominated by Sphagnum, are an important contributor of atmospheric methane, and we seek to understand the methane cycle in these systems. We present a novel method for quantifying the proportion of carbon Sphagnum assimilates from its methanotrophic symbionts using stable isotope ratios of leaf-wax biomarkers. Carbon isotope ratios of Sphagnum compounds are determined by two competing influences, water content and the isotope ratio of source carbon. We disentangled these effects using a combined hydrogen and carbon isotope approach. We constrained Sphagnum water content using the contrast between the hydrogen isotope ratios of Sphagnum and vascular plant biomarkers. We then used Sphagnum water content to calculate the carbon isotope ratio of Sphagnum's carbon pool. Using a mass balance equation, we calculated the proportion of recycled methane contributed to the Sphagnum carbon pool, 'PRM.' We quantified PRM in peat monoliths from three microhabitats in the Mer Bleue peatland complex. Modern studies have shown that water table depth and vegetation have strong influences on the peatland methane cycle on instrumental time scales. With this new approach, delta C-13 of Sphagnum compounds are now a useful tool for investigating the relationships among hydrology, vegetation, and methanotrophy in Sphagnum peatlands over the time scales of entire peatland sediment records, vital to our understanding of the global carbon cycle through the Late Glacial and Holocene.

air pollution↗
NASA NTRS1987

Isotope separation using tuned laser and electron beam

The apparatus comprises means for producing an atomic beam containing the isotope of interest and other isotopes. Means are provided for producing a magnetic field traversing the path of the atomic beam of an intensity sufficient to broaden the energy domain of the various individual magnetic sublevels of the isotope of interest and having the atomic beam passing therethrough. A laser beam is produced of a frequency and polarization selected to maximize the activation of only individual magnetic sublevels of the isotope of interest with the portion of its broadened energy domain most removed from other isotopes with the stream. The laser beam is directed so as to strike the atomic beam within the magnetic field and traverse the path of the atomic beam whereby only the isotope of interest is activated by the laser beam. The apparatus further includes means for producing a collimated and high intensity beam of electrons of narrow energy distribution within the magnetic field which is aimed so as to strike the atomic beam while the atomic beam is simultaneously struck by the laser beam and at an energy level selected to ionize the activated isotope of interest but not ground state species included therewith. Deflection means are disposed in the usual manner to collect the ions.

Trajmar, Sandor↗
NASA NTRS1989

Isotope Ratio Monitoring Gas Chromatography Mass Spectrometry (IRM-GCMS)

On Earth, the C-13 content of organic compounds is depleted by roughly 13 to 23 permil from atmospheric carbon dioxide. This difference is largely due to isotope effects associated with the fixation of inorganic carbon by photosynthetic organisms. If life once existed on Mars, then it is reasonable to expect to observe a similar fractionation. Although the strongly oxidizing conditions on the surface of Mars make preservation of ancient organic material unlikely, carbon-isotope evidence for the existence of life on Mars may still be preserved. Carbon depleted in C-13 could be preserved either in organic compounds within buried sediments, or in carbonate minerals produced by the oxidation of organic material. A technique is introduced for rapid and precise measurement of the C-13 contents of individual organic compounds. A gas chromatograph is coupled to an isotope-ratio mass spectrometer through a combustion interface, enabling on-line isotopic analysis of isolated compounds. The isotope ratios are determined by integration of ion currents over the course of each chromatographic peak. Software incorporates automatic peak determination, corrections for background, and deconvolution of overlapped peaks. Overall performance of the instrument was evaluated by the analysis of a mixture of high purity n-alkanes of know isotopic composition. Isotopic values measured via IRM-GCMS averaged withing 0.55 permil of their conventionally measured values.

Freeman, K. H.↗
NASA NTRS1989

The identification of meteorite inclusions with isotope anomalies

Ca-Al refractory inclusions with characteristic chemical and mineralogical compositions show an enhanced occurrence of 20 pct of isotope anomalies reflecting unknown nucleosynthetic effects for O and Mg. The anomalies are characterized by large isotope fractionation in Mg, apparent deficits in Mg-26/Mg-24, and large correlated effects for isotopes of Ca, Ti, and Cr. These isotope patterns define exotic components depleted in the most neutron-rich isotopes of Ca, Ti, and Cr, or components depleted in isotopes produced in explosive O and Si burning. An opaque assemblage within one of the inclusions yields isotope anomalies in Cr similar to the bulk inclusion and must be intrinsically part of the inclusion and not a trapped, foreign grain aggregate.

Papanastassiou, D. A.↗
NASA NTRS1991

Isotopic constraints on the origin of meteoritic organic matter

Salient features of the isotopic distribution of H, C and N in the organic material found in carbonaceous meteorites are noted. Most organic fractions are strongly enriched in D with respect to the D/H ratio characteristic of H2 in the protosolar system; substantial variations in C-13/C-12 ratio are found among different molecular species, with oxidised species tending to be C-13 enriched relative to reduced species; some homologous series reveal systematic decrease in C-13/C-12 with increasing C number; considerable variation in N-15/N-14 ratio is observed within organic matter, though no systematic pattern to its distribution has yet emerged; no interelement correlations have been observed between isotope enrichments for the different biogenic elements. The isotopic complexity echoes the molecular diversity observed in meteoritic organic matter and suggests that the organic matter was formed by multiple processes and/or from multiple sources. However, existence of a few systematic patterns points towards survival of isotopic signatures characteristic of one or more specific processes. The widespread D enrichment implies either survival of many species of interstellar molecule or synthesis from a reservoir containing a significant interstellar component. Several of the questions raised above can be addressed by more detailed determination of the distribution of the H, C and N isotopes among different well-characterized molecular fractions. Thus, the present study is aimed at discovering whether the different amino acids have comparable D enrichments, which would imply local synthesis from a D-enriched reservoir, or very viable D enrichments, which would imply survival of some interstellar amino acids. The same approach is also being applied to polycyclic aromatic hydrocarbons. Because the analytical technique employed (secondary ion mass spectrometry) can acquire data for all three isotopic systems from each molecular fraction, any presently obscured interelement isotopic correlation should also be revealed, which will aid in identifying pertinent synthetic processes.

Kerridge, J. F.↗
NASA NTRS1993

Variations of the isotopic composition of sulfur in enstatite and ordinary chondrites

High-precision sulfur isotopic analyses (delta S-33, delta S-34, and delta S-36) of bulk ordinary and enstatite chondrites demonstrate that systematic variations exist. The average delta S-34 values are -0.26 +/- 0.07, -0.02 +/- 0.06, and 0.49 +/- 0.16 percent for enstatite and ordinary and carbonaceous chondrites, respectively. Isotopic variations of different sample specimens of primitive meteorites, e.g., Qingzhen and Abee, were observed which may be attributed to heterogeneity in the early solar nebula. Sulfur isotopic fractionations in both bulk samples and mineral separates are mass-dependent, and no nuclear isotopic anomalies were detected. The sulfur isotopic compositions of both mineral and density separates were measured. The sulfur isotopic compositions of separated chondrules from Chainpur and Bjurbole are reported. Significant isotopic difference for the chondrules from the bulk meteorite are noted for both meteorites.

Gao, Xia↗
NASA NTRS1994

Effects of isotope selection on solution convergence in HZE transport

A fragmenting iron ion produces hundreds of isotopes during nuclear reactions. These isotopes are represented in the solution of the transport problem. A reduced set of isotopes is selected to minimize the computational burden but introduces error in the final result. A minimum list of 122 isotopes is required for adequate representation of the mass and charge distributions of the secondary radiation fields. A reduced set of 80 isotopes is sufficient to represent the charge distribution alone and represents reasonably well the linear energy transfer properties of the iron beam. Because iron fragmentation produces nearly every isotope lighter than iron, the resulting 122-isotope list should be adequate for ion beams with charges equal to or less than 26.

Kim, Myung-Hee Y.↗
NASA NTRS1994

Search for isotopic anomalies in oldhamite (CaS) from unequilibrated (E3) enstatite chondrites

The Ca isotopic compositions of 32 oldhamite (CaS) grains from the Qingzhen (EH3), MAC88136 (EL3), and Indarch (EH4) enstatite chondrites were determined by ion microprobe mass spectrometry. Also measured were the S isotopic compositions of eight oldhamite, two niningerite (MgS), and seven troilite (FeS) grains. The S isotopic compositions of all minerals are normal, but oldhamite grains of the first two meteorites exhibit apparent small Ca-48 excesses and deficits that are correlated with isotopic mass fractionation as determined from the Ca-40-Ca-44 pair. The interpretation of these results is complicated by the fact that none of the established mass fractionation laws can account for the data in the Norton County oldhamite standard. The method of analysis is carefully scrutinized for experimental artifacts. Neither interferences nor any known mass frationation effect can satisfactorily explain the observed small deviations from normal isotopic composition. If these are truly isotopic anomalies, they are much smaller than those observed in hibonite. The nucleosynthetic origin of Ca isotopes is discussed.

Lundberg, Laura L.↗
NASA NTRS1996

Meteoritic Sulfur Isotopic Analysis

Funds were requested to continue our program in meteoritic sulfur isotopic analysis. We have recently detected a potential nucleosynthetic sulfur isotopic anomaly. We will search for potential carriers. The documentation of bulk systematics and the possible relation to nebular chemistry and oxygen isotopes will be explored. Analytical techniques for delta(sup 33), delta(sup 34)S, delta(sup 36)S isotopic analysis were improved. Analysis of sub milligram samples is now possible. A possible relation between sulfur isotopes and oxygen was detected, with similar group systematics noted, particularly in the case of aubrites, ureilites and entstatite chondrites. A possible nucleosynthetic excess S-33 has been noted in bulk ureilites and an oldhamite separate from Norton County. High energy proton (approximately 1 GeV) bombardments of iron foils were done to experimentally determine S-33, S-36 spallogenic yields for quantitation of isotopic measurements in iron meteorites. Techniques for measurement of mineral separates were perfected and an analysis program initiated. The systematic behavior of bulk sulfur isotopes will continue to be explored.

Thiemens, Mark H.↗
NASA NTRS2003

Physics of the Isotopic Dependence of Galactic Cosmic Ray Fluence Behind Shielding

For over 25 years, NASA has supported the development of space radiation transport models for shielding applications. The NASA space radiation transport model now predicts dose and dose equivalent in Earth and Mars orbit to an accuracy of plus or minus 20%. However, because larger errors may occur in particle fluence predictions, there is interest in further assessments and improvements in NASA's space radiation transport model. In this paper, we consider the effects of the isotopic composition of the primary galactic cosmic rays (GCR) and the isotopic dependence of nuclear fragmentation cross-sections on the solution to transport models used for shielding studies. Satellite measurements are used to describe the isotopic composition of the GCR. Using NASA's quantum multiple-scattering theory of nuclear fragmentation (QMSFRG) and high-charge and energy (HZETRN) transport code, we study the effect of the isotopic dependence of the primary GCR composition and secondary nuclei on shielding calculations. The QMSFRG is shown to accurately describe the iso-spin dependence of nuclear fragmentation. The principal finding of this study is that large errors (plus or minus 100%) will occur in the mass-fluence spectra when comparing transport models that use a complete isotope grid (approximately 170 ions) to ones that use a reduced isotope grid, for example the 59 ion-grid used in the HZETRN code in the past, however less significant errors (less than 20%) occur in the elemental-fluence spectra. Because a complete isotope grid is readily handled on small computer workstations and is needed for several applications studying GCR propagation and scattering, it is recommended that they be used for future GCR studies.

Cucinotta, Francis A.↗
NASA NTRS2004

Evaporation and Accompanying Isotopic Fractionation of Sulfur from FE-S Melt During Shock Wave Heating

Chondrules probably formed by melting and subsequent cooling of solid precursors. Evaporation during chondrule melting may have resulted in depletion of volatile elements in chondrules. It is known that kinetic evaporation, especially evaporation from a melt, often leads to enrichment of heavy isotopes in an evaporation residue. However, no evidence for a large degree of heavy-isotope enrichment has been reported in chondrules for K, Mg, Si, and Fe (as FeO). The lack of isotopic fractionation has also been found for sulfur in troilites (FeS) within Bishunpur (LL3.1) and Semarkona (LL3.0) chondrules by an ion microprobe study. The largest fractionation, found in only one grain, was 2.7 +/- 1.4 %/amu, while all other troilite grains showed isotopic fractionations of <1 %/amu. The suppressed isotopic fractionation has been interpreted as results of (i) rapid heating of precursors at temperatures below the silicate solidus and (ii) diffusion-controlled evaporation through a surrounding silicate melt at temperatures above the silicate solidus. The kinetic evaporation model suggests that a rapid heating rate of >10(exp 4)-10(exp 6) K/h for a temperature range of 1000-1300 C is required to explain observed isotopic fractionations. Such a rapid heating rate seems to be difficult to be achieved in the X-wind model, but can be achieved in shock wave heating models. In this study, we have applied the sulfur evaporation model to the shock wave heating conditions of to evaluate evaporation of sulfur and accompanying isotopic fractionation during shock wave heating at temperatures below the silicate solidus.

Tachibana, S.↗
NASA NTRS2007

Sm-Nd Isotopic Systematics of Troctolite 76335

A study of the Sm-Nd isotopic systematics of lunar Mg-suite troctolite 76335 was undertaken to further establish the early chronology of lunar magmatism. Because the Rb-Sr isotopic systematics of similar sample 76535 yielded an age of 4570 +/- 70 Ma [2, lambda = 1.402 x 10(exp -11)], 76335 was expected to yield an old age. In contrast, the Sm-Nd and K-Ar ages of 76535 indicate that the sample is approximately 4260 Ma old, one of the youngest ages obtained for a Mg-suite rock. This study establishes the age of 76335 and discusses the constraints placed on its petrogenesis by its Sm-Nd isotope systematics. The Sm-Nd isotopic system of lunar Mg-suite troctolite 76335 indicates an age of 4278 +/- 60 Ma with an initial epsilon (sup 143)(sub Nd) value of 0.06 +/- 0.39. These values are consistent with the Sm-Nd isotopic systematics of similar sample 76535. Thus, it appears that a robust Sm-Nd age can be determined from a highly brecciated lunar sample. The Sm-Nd isotopic systematics of troctolites 76335 and 76535 appear to be different from those dominating the Mg-suite norites and KREEP basalts. Further analysis of the Mg-suite must be completed to reveal the isotopic relationships of these early lunar rocks.

Edmunson, J.↗
NASA NTRS2007

Stardust in STARDUST - the C, N, and O Isotopic Compositions of Wild 2 Cometary Matter in Al foil Impacts

In January 2006, the STARDUST mission successfully returned dust samples from the tail of comet 81P/Wild 2 in two principal collection media, low density silica aerogel and Al foil. While hypervelocity impacts at 6.1 km/s, the encounter velocity of STARDUST, into Al foils are generally highly disruptive for natural, silicate-dominated impactors, previous studies have shown that many craters retain sufficient residue to allow a determination of the elemental and isotopic compositions of the original projectile. We have used the NanoSIMS to perform C, N, and O isotope imaging measurements on four large (59-370 microns diameter) and on 47 small (0.32-1.9 microns diameter) Al foil impact craters as part of the STARDUST Preliminary Examination. Most analyzed residues in and around these craters are isotopically normal (solar) in their C, N, and O isotopic compositions. However, the debris in one large crater shows an average 15N enrichment of approx. 450 %, which is similar to the bulk composition of some isotopically primitive interplanetary dust particles. A 250 nm grain in another large crater has an O-17 enrichment with approx. 2.65 times the solar O-17/O-16 ratio. Such an O isotopic composition is typical for circumstellar oxide or silicate grains from red giant or asymptotic giant branch stars. The discovery of this circumstellar grain clearly establishes that there is authentic stardust in the cometary samples returned by the STARDUST mission. However, the low apparent abundance of circumstellar grains in Wild 2 samples and the preponderance of isotopically normal material indicates that the cometary matter is a diverse assemblage of presolar and solar system materials.

Stadermann, Frank J.↗