WorldWideScience

Sample records for sas2h isotopic predictions

  1. SAS2H Generated Isotopic Concentrations For B&W 15X15 PWR Assembly (SCPB:N/A)

    Energy Technology Data Exchange (ETDEWEB)

    J.W. Davis

    1996-08-29

    This analysis is prepared by the Mined Geologic Disposal System (MGDS) Waste Package Development Department (WPDD) to provide pressurized water reactor (PWR) isotopic composition data as a function of time for use in criticality analyses. The objectives of this evaluation are to generate burnup and decay dependant isotopic inventories and to provide these inventories in a form which can easily be utilized in subsequent criticality calculations.

  2. Validation of the scale system for PWR spent fuel isotopic composition analyses

    Energy Technology Data Exchange (ETDEWEB)

    Hermann, O.W.; Bowman, S.M.; Parks, C.V. [Oak Ridge National Lab., TN (United States); Brady, M.C. [Sandia National Laboratories, Las Vegas, NV (United States)

    1995-03-01

    The validity of the computation of pressurized-water-reactor (PWR) spent fuel isotopic composition by the SCALE system depletion analysis was assessed using data presented in the report. Radiochemical measurements and SCALE/SAS2H computations of depleted fuel isotopics were compared with 19 benchmark-problem samples from Calvert Cliffs Unit 1, H. B. Robinson Unit 2, and Obrigheim PWRs. Even though not exhaustive in scope, the validation included comparison of predicted and measured concentrations for 14 actinides and 37 fission and activation products. The basic method by which the SAS2H control module applies the neutron transport treatment and point-depletion methods of SCALE functional modules (XSDRNPM-S, NITAWL-II, BONAMI, and ORIGEN-S) is described in the report. Also, the reactor fuel design data, the operating histories, and the isotopic measurements for all cases are included in detail. The underlying radiochemical assays were conducted by the Materials Characterization. Center at Pacific Northwest Laboratory as part of the Approved Testing Material program and by four different laboratories in Europe on samples processed at the Karlsruhe Reprocessing Plant.

  3. RCWIM - an improved global water isotope pattern prediction model using fuzzy climatic clustering regionalization

    Science.gov (United States)

    Terzer, Stefan; Araguás-Araguás, Luis; Wassenaar, Leonard I.; Aggarwal, Pradeep K.

    2013-04-01

    Prediction of geospatial H and O isotopic patterns in precipitation has become increasingly important to diverse disciplines beyond hydrology, such as climatology, ecology, food authenticity, and criminal forensics, because these two isotopes of rainwater often control the terrestrial isotopic spatial patterns that facilitate the linkage of products (food, wildlife, water) to origin or movement (food, criminalistics). Currently, spatial water isotopic pattern prediction relies on combined regression and interpolation techniques to create gridded datasets by using data obtained from the Global Network of Isotopes In Precipitation (GNIP). However, current models suffer from two shortcomings: (a) models may have limited covariates and/or parameterization fitted to a global domain, which results in poor predictive outcomes at regional scales, or (b) the spatial domain is intentionally restricted to regional settings, and thereby of little use in providing information at global geospatial scales. Here we present a new global climatically regionalized isotope prediction model which overcomes these limitations through the use of fuzzy clustering of climatic data subsets, allowing us to better identify and customize appropriate covariates and their multiple regression coefficients instead of aiming for a one-size-fits-all global fit (RCWIM - Regionalized Climate Cluster Water Isotope Model). The new model significantly reduces the point-based regression residuals and results in much lower overall isotopic prediction uncertainty, since residuals are interpolated onto the regression surface. The new precipitation δ2H and δ18O isoscape model is available on a global scale at 10 arc-minutes spatial and at monthly, seasonal and annual temporal resolution, and will provide improved predicted stable isotope values used for a growing number of applications. The model further provides a flexible framework for future improvements using regional climatic clustering.

  4. A Triple-Isotope Approach to Predict the Breeding Origins of European Bats

    Science.gov (United States)

    Popa-Lisseanu, Ana G.; Sörgel, Karin; Luckner, Anja; Wassenaar, Leonard I.; Ibáñez, Carlos; Kramer-Schadt, Stephanie; Ciechanowski, Mateusz; Görföl, Tamás; Niermann, Ivo; Beuneux, Grégory; Mysłajek, Robert W.; Juste, Javier; Fonderflick, Jocelyn; Kelm, Detlev H.; Voigt, Christian C.

    2012-01-01

    Despite a commitment by the European Union to protect its migratory bat populations, conservation efforts are hindered by a poor understanding of bat migratory strategies and connectivity between breeding and wintering grounds. Traditional methods like mark-recapture are ineffective to study broad-scale bat migratory patterns. Stable hydrogen isotopes (δD) have been proven useful in establishing spatial migratory connectivity of animal populations. Before applying this tool, the method was calibrated using bat samples of known origin. Here we established the potential of δD as a robust geographical tracer of breeding origins of European bats by measuring δD in hair of five sedentary bat species from 45 locations throughout Europe. The δD of bat hair strongly correlated with well-established spatial isotopic patterns in mean annual precipitation in Europe, and therefore was highly correlated with latitude. We calculated a linear mixed-effects model, with species as random effect, linking δD of bat hair to precipitation δD of the areas of hair growth. This model can be used to predict breeding origins of European migrating bats. We used δ13C and δ15N to discriminate among potential origins of bats, and found that these isotopes can be used as variables to further refine origin predictions. A triple-isotope approach could thereby pinpoint populations or subpopulations that have distinct origins. Our results further corroborated stable isotope analysis as a powerful method to delineate animal migrations in Europe. PMID:22291947

  5. Zinc Isotope Variability in Three Coal-Fired Power Plants: A Predictive Model for Determining Isotopic Fractionation during Combustion.

    Science.gov (United States)

    Ochoa Gonzalez, R; Weiss, D

    2015-10-20

    The zinc (Zn) isotope compositions of feed materials and combustion byproducts were investigated in three different coal-fired power plants, and the results were used to develop a generalized model that can account for Zn isotopic fractionation during coal combustion. The isotope signatures in the coal (δ(66)ZnIRMM) ranged between +0.73 and +1.18‰, values that fall well within those previously determined for peat (+0.6 ±2.0‰). We therefore propose that the speciation of Zn in peat determines the isotope fingerprint in coal. All of the bottom ashes collected in these power plants were isotopically depleted in the heavy isotopes relative to the coals, with δ(66)ZnIRMM values ranging between +0.26‰ and +0.64‰. This suggests that the heavy isotopes, possibly associated with the organic matter of the coal, may be preferentially released into the vapor phase. The fly ash in all of these power plants was, in contrast, enriched in the heavy isotopes relative to coal. The signatures in the fly ash can be accounted for using a simple unidirectional fractionation model with isotope fractionation factors (αsolid-vapor) ranging between 1.0003 and 1.0007, and we suggest that condensation is the controlling process. The model proposed allows, once the isotope composition of the feed coal is known, the constraining of the Zn signatures in the byproducts. This will now enable the integration of Zn isotopes as a quantitative tool for the source apportionment of this metal from coal combustion in the atmosphere.

  6. Toward Predictive Theories of Nuclear Reactions Across the Isotopic Chart: Web Report

    Energy Technology Data Exchange (ETDEWEB)

    Escher, J. E. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Blackmon, J. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Elster, C. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Launey, K. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Lee, D. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Scielzo, N. D. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2017-05-12

    Recent years have seen exciting new developments and progress in nuclear structure theory, reaction theory, and experimental techniques, that allow us to move towards a description of exotic systems and environments, setting the stage for new discoveries. The purpose of the 5-week program was to bring together physicists from the low-energy nuclear structure and reaction communities to identify avenues for achieving reliable and predictive descriptions of reactions involving nuclei across the isotopic chart. The 4-day embedded workshop focused on connecting theory developments to experimental advances and data needs for astrophysics and other applications. Nuclear theory must address phenomena from laboratory experiments to stellar environments, from stable nuclei to weakly-bound and exotic isotopes. Expanding the reach of theory to these regimes requires a comprehensive understanding of the reaction mechanisms involved as well as detailed knowledge of nuclear structure. A recurring theme throughout the program was the desire to produce reliable predictions rooted in either ab initio or microscopic approaches. At the same time it was recognized that some applications involving heavy nuclei away from stability, e.g. those involving fi ssion fragments, may need to rely on simple parameterizations of incomplete data for the foreseeable future. The goal here, however, is to subsequently improve and refine the descriptions, moving to phenomenological, then microscopic approaches. There was overarching consensus that future work should also focus on reliable estimates of errors in theoretical descriptions.

  7. An Approach for Validating Actinide and Fission Product Burnup Credit Criticality Safety Analyses-Isotopic Composition Predictions

    Energy Technology Data Exchange (ETDEWEB)

    Radulescu, Georgeta [ORNL; Gauld, Ian C [ORNL; Ilas, Germina [ORNL; Wagner, John C [ORNL

    2011-01-01

    The expanded use of burnup credit in the United States (U.S.) for storage and transport casks, particularly in the acceptance of credit for fission products, has been constrained by the availability of experimental fission product data to support code validation. The U.S. Nuclear Regulatory Commission (NRC) staff has noted that the rationale for restricting the Interim Staff Guidance on burnup credit for storage and transportation casks (ISG-8) to actinide-only is based largely on the lack of clear, definitive experiments that can be used to estimate the bias and uncertainty for computational analyses associated with using burnup credit. To address the issues of burnup credit criticality validation, the NRC initiated a project with the Oak Ridge National Laboratory to (1) develop and establish a technically sound validation approach for commercial spent nuclear fuel (SNF) criticality safety evaluations based on best-available data and methods and (2) apply the approach for representative SNF storage and transport configurations/conditions to demonstrate its usage and applicability, as well as to provide reference bias results. The purpose of this paper is to describe the isotopic composition (depletion) validation approach and resulting observations and recommendations. Validation of the criticality calculations is addressed in a companion paper at this conference. For isotopic composition validation, the approach is to determine burnup-dependent bias and uncertainty in the effective neutron multiplication factor (keff) due to bias and uncertainty in isotopic predictions, via comparisons of isotopic composition predictions (calculated) and measured isotopic compositions from destructive radiochemical assay utilizing as much assay data as is available, and a best-estimate Monte Carlo based method. This paper (1) provides a detailed description of the burnup credit isotopic validation approach and its technical bases, (2) describes the application of the approach for

  8. SCALE 5.1 Predictions of PWR Spent Nuclear Fuel Isotopic Compositions

    Energy Technology Data Exchange (ETDEWEB)

    Radulescu, Georgeta [ORNL; Gauld, Ian C [ORNL; Ilas, Germina [ORNL

    2010-03-01

    The purpose of this calculation report is to document the comparison to measurement of the isotopic concentrations for pressurized water reactor (PWR) spent nuclear fuel determined with the Standardized Computer Analysis for Licensing Evaluation (SCALE) 5.1 (Ref. ) epletion calculation method. Specifically, the depletion computer code and the cross-section library being evaluated are the twodimensional (2-D) transport and depletion module, TRITON/NEWT,2, 3 and the 44GROUPNDF5 (Ref. 4) cross-section library, respectively, in the SCALE .1 code system.

  9. Oxygen and hydrogen isotope ratios in tree rings: how well do models predict observed values?

    CSIR Research Space (South Africa)

    Waterhouse, JS

    2002-07-30

    Full Text Available Science Letters 201 (2002) 421^430 www.elsevier.com/locate/epsl environmental data, such as ice cores and lake sediments, owing to unambiguous dating of tree rings to precise years. Ring widths and X-ray ab- sorption measurements have been very success...-7-02 J.S. Waterhouse et al. / Earth and Planetary Science Letters 201 (2002) 421^430 tionship is given by Eq. 1: Nl ? Ns ??Oe ? Ok??13h??1? In this model it is assumed that an isotopic steady state has been reached in the leaf and that source water...

  10. Prediction of equilibrium Li isotope fractionation between minerals and aqueous solutions at high P and T: An efficient ab initio approach

    Science.gov (United States)

    Kowalski, Piotr M.; Jahn, Sandro

    2011-10-01

    The mass-dependent equilibrium stable isotope fractionation between different materials is an important geochemical process. Here we present an efficient method to compute the isotope fractionation between complex minerals and fluids at high pressure, P, and temperature, T, representative for the Earth's crust and mantle. The method is tested by computation of the equilibrium fractionation of lithium isotopes between aqueous fluids and various Li bearing minerals such as staurolite, spodumene and mica. We are able to correctly predict the direction of the isotope fractionation as observed in the experiments. On the quantitative level the computed fractionation factors agree within 1.0‰ with the experimental values indicating predictive power of ab initio methods. We show that with ab initio methods we are able to investigate the underlying mechanisms driving the equilibrium isotope fractionation process, such as coordination of the fractionating elements, their bond strengths to the neighboring atoms, compression of fluids and thermal expansion of solids. This gives valuable insight into the processes governing the isotope fractionation mechanisms on the atomic scale. The method is applicable to any state and does not require different treatment of crystals and fluids.

  11. International challenge to predict the impact of radioxenon releases from medical isotope production on a comprehensive nuclear test ban treaty sampling station.

    Science.gov (United States)

    Eslinger, Paul W; Bowyer, Ted W; Achim, Pascal; Chai, Tianfeng; Deconninck, Benoit; Freeman, Katie; Generoso, Sylvia; Hayes, Philip; Heidmann, Verena; Hoffman, Ian; Kijima, Yuichi; Krysta, Monika; Malo, Alain; Maurer, Christian; Ngan, Fantine; Robins, Peter; Ross, J Ole; Saunier, Olivier; Schlosser, Clemens; Schöppner, Michael; Schrom, Brian T; Seibert, Petra; Stein, Ariel F; Ungar, Kurt; Yi, Jing

    2016-06-01

    The International Monitoring System (IMS) is part of the verification regime for the Comprehensive Nuclear-Test-Ban-Treaty Organization (CTBTO). At entry-into-force, half of the 80 radionuclide stations will be able to measure concentrations of several radioactive xenon isotopes produced in nuclear explosions, and then the full network may be populated with xenon monitoring afterward. An understanding of natural and man-made radionuclide backgrounds can be used in accordance with the provisions of the treaty (such as event screening criteria in Annex 2 to the Protocol of the Treaty) for the effective implementation of the verification regime. Fission-based production of (99)Mo for medical purposes also generates nuisance radioxenon isotopes that are usually vented to the atmosphere. One of the ways to account for the effect emissions from medical isotope production has on radionuclide samples from the IMS is to use stack monitoring data, if they are available, and atmospheric transport modeling. Recently, individuals from seven nations participated in a challenge exercise that used atmospheric transport modeling to predict the time-history of (133)Xe concentration measurements at the IMS radionuclide station in Germany using stack monitoring data from a medical isotope production facility in Belgium. Participants received only stack monitoring data and used the atmospheric transport model and meteorological data of their choice. Some of the models predicted the highest measured concentrations quite well. A model comparison rank and ensemble analysis suggests that combining multiple models may provide more accurate predicted concentrations than any single model. None of the submissions based only on the stack monitoring data predicted the small measured concentrations very well. Modeling of sources by other nuclear facilities with smaller releases than medical isotope production facilities may be important in understanding how to discriminate those releases from

  12. Stable isotope models of sugar intake using hair, red blood cells, and plasma, but not fasting plasma glucose, predict sugar intake in a Yup'ik study population.

    Science.gov (United States)

    Nash, Sarah H; Kristal, Alan R; Hopkins, Scarlett E; Boyer, Bert B; O'Brien, Diane M

    2014-01-01

    Objectively measured biomarkers will help to resolve the controversial role of sugar intake in the etiology of obesity and related chronic diseases. We recently validated a dual-isotope model based on RBC carbon (δ(13)C) and nitrogen (δ(15)N) isotope ratios that explained a large percentage of the variation in self-reported sugar intake in a Yup'ik study population. Stable isotope ratios can easily be measured from many tissues, including RBCs, plasma, and hair; however, it is not known how isotopic models of sugar intake compare among these tissues. Here, we compared self-reported sugar intake with models based on RBCs, plasma, and hair δ(13)C and δ(15)N in Yup'ik people. We also evaluated associations of sugar intake with fasting plasma glucose δ(13)C. Finally, we evaluated relations between δ(13)C and δ(15)N values in hair, plasma, RBCs, and fasting plasma glucose to allow comparison of isotope ratios across tissue types. Models using RBCs, plasma, or hair isotope ratios explained similar amounts of variance in total sugar, added sugar, and sugar-sweetened beverage intake (∼53%, 48%, and 34%, respectively); however, the association with δ(13)C was strongest for models based on RBCs and hair. There were no associations with fasting plasma glucose δ(13)C (R(2) = 0.03). The δ(13)C and δ(15)N values of RBCs, plasma, and hair showed strong, positive correlations; the slopes of these relations did not differ from 1. This study demonstrates that RBC, plasma, and hair isotope ratios predict sugar intake and provides data that will allow comparison of studies using different sample types.

  13. Predicted bounds on peak global mean sea level during marine isotope stages 5a and 5c

    Science.gov (United States)

    Creveling, Jessica R.; Mitrovica, Jerry X.; Clark, Peter U.; Waelbroeck, Claire; Pico, Tamara

    2017-05-01

    Estimates of marine isotope stage (MIS) 5c and 5a global mean sea level (GMSL) based on marine terraces and coastal indicators range from 15-37 m and 9-30 m below present, respectively. Tectonic displacement and glacial isostatic adjustment (GIA) complicate efforts to refine this range. We revisit this issue using numerical predictions of post-glacial sea-level change and updated estimates of site-specific tectonic signals based upon these predictions. Laurentide and Cordilleran peripheral bulge dynamics and variations in the gravitational effect of these ice masses dominate the GIA signal along the east and west coasts of North America. Published compilations suggest that MIS 5 sea-level indicators extending from Virginia to the Caribbean lie on the outer flank of the peripheral bulge, while those along a transect from Oregon to Baja California sit on the inner flank of the bulge. Our GIA modeling reconciles these data by adopting a significantly weaker (i.e., lower viscosity) upper mantle in analyzing data on the Pacific coast relative to the Atlantic, an inference supported by seismic tomography. We present a sensitivity analysis that compares the observed elevation of globally distributed high stand markers to a suite of GIA simulations that vary the Earth model and GMSL from the Last Interglaciation (MIS 5e, ∼130-115 ka) to 70 ka. We conclude that GMSL peaked at -8.5 ± 4.6 m (1σ) during MIS 5a and -9.4 ± 5.3 m during MIS 5c. A more restrictive analysis yields slightly wider bounds corresponding to -10.5 ± 5.5 m and -11.1 ± 6.6 m, respectively.

  14. International challenge to predict the impact of radioxenon releases from medical isotope production on a comprehensive nuclear test ban treaty sampling station

    Energy Technology Data Exchange (ETDEWEB)

    Eslinger, Paul W.; Bowyer, Ted W.; Achim, Pascal; Chai, Tianfeng; Deconninck, Benoit; Freeman, Katie; Generoso, Sylvia; Hayes, Philip; Heidmann, Verena; Hoffman, Ian; Kijima, Yuichi; Krysta, Monika; Malo, Alain; Maurer, Christian; Ngan, Fantine; Robins, Peter; Ross, J. Ole; Saunier, Olivier; Schlosser, Clemens; Schöppner, Michael; Schrom, Brian T.; Seibert, Petra; Stein, Ariel F.; Ungar, Kurt; Yi, Jing

    2016-06-01

    Abstract The International Monitoring System (IMS) is part of the verification regime for the Comprehensive Nuclear-Test-Ban-Treaty Organization (CTBTO). At entry-into-force, half of the 80 radionuclide stations will be able to measure concentrations of several radioactive xenon isotopes produced in nuclear explosions, and then the full network may be populated with xenon monitoring afterward (Bowyer et al., 2013). Fission-based production of 99Mo for medical purposes also releases radioxenon isotopes to the atmosphere (Saey, 2009). One of the ways to mitigate the effect of emissions from medical isotope production is the use of stack monitoring data, if it were available, so that the effect of radioactive xenon emissions could be subtracted from the effect from a presumed nuclear explosion, when detected at an IMS station location. To date, no studies have addressed the impacts the time resolution or data accuracy of stack monitoring data have on predicted concentrations at an IMS station location. Recently, participants from seven nations used atmospheric transport modeling to predict the time-history of 133Xe concentration measurements at an IMS station in Germany using stack monitoring data from a medical isotope production facility in Belgium. Participants received only stack monitoring data and used the atmospheric transport model and meteorological data of their choice. Some of the models predicted the highest measured concentrations quite well (a high composite statistical model comparison rank or a small mean square error with the measured values). The results suggest release data on a 15 min time spacing is best. The model comparison rank and ensemble analysis suggests that combining multiple models may provide more accurate predicted concentrations than any single model. Further research is needed to identify optimal methods for selecting ensemble members and those methods may depend on the specific transport problem. None of the submissions based only

  15. Vibrational Spectroscopy of the CCl[subscript 4] v[subscript 1] Mode: Theoretical Prediction of Isotopic Effects

    Science.gov (United States)

    Gaynor, James D.; Wetterer, Anna M.; Cochran, Rea M.; Valente, Edward J.; Mayer, Steven G.

    2015-01-01

    Raman spectroscopy is a powerful experimental technique, yet it is often missing from the undergraduate physical chemistry laboratory curriculum. Tetrachloromethane (CCl[subscript 4]) is the ideal molecule for an introductory vibrational spectroscopy experiment and the symmetric stretch vibration contains fine structure due to isotopic variations…

  16. Carbon Isotope Composition of Carbohydrates and Polyols in Leaf and Phloem Sap of Phaseolus vulgaris L. Influences Predictions of Plant Water Use Efficiency.

    Science.gov (United States)

    Smith, Millicent; Wild, Birgit; Richter, Andreas; Simonin, Kevin; Merchant, Andrew

    2016-08-01

    The use of carbon isotope abundance (δ(13)C) to assess plant carbon acquisition and water use has significant potential for use in crop management and plant improvement programs. Utilizing Phaseolus vulgaris L. as a model system, this study demonstrates the occurrence and sensitivity of carbon isotope fractionation during the onset of abiotic stresses between leaf and phloem carbon pools. In addition to gas exchange data, compound-specific measures of carbon isotope abundance and concentrations of soluble components of phloem sap were compared with major carbohydrate and sugar alcohol pools in leaf tissue. Differences in both δ(13)C and concentration of metabolites were found in leaf and phloem tissues, the magnitude of which responded to changing environmental conditions. These changes have inplications for the modeling of leaf-level gas exchange based upon δ(13)C natural abundance. Estimates of δ(13)C of low molecular weight carbohydrates and polyols increased the precision of predictions of water use efficiency compared with those based on bulk soluble carbon. The use of this technique requires consideration of the dynamics of the δ(13)C pool under investigation. Understanding the dynamics of changes in δ(13)C during movement and incorporation into heterotrophic tissues is vital for the continued development of tools that provide information on plant physiological performance relating to water use. © The Author 2016. Published by Oxford University Press on behalf of Japanese Society of Plant Physiologists. All rights reserved. For permissions, please email: journals.permissions@oup.com.

  17. Vitamin A isotope dilution predicts liver stores in line with long-term vitamin A intake above the current Recommended Dietary Allowance for young adult women.

    Science.gov (United States)

    Valentine, Ashley R; Davis, Christopher R; Tanumihardjo, Sherry A

    2013-11-01

    The Estimated Average Requirement (EAR) and Recommended Dietary Allowance (RDA) for vitamin A are 1.7 and 2.4 μmol/d (500 and 700 μg retinol activity equivalents/d), respectively, for nonpregnant, nonlactating women aged >19 y. This intake is presumed to maintain a minimally acceptable liver concentration of 0.07 μmol (20 μg) retinol/g; however, liver reserves have not been evaluated with respect to vitamin A intake in women of any age group defined in the Dietary Reference Intakes. This cross-sectional study examined vitamin A intake and liver reserves estimated by stable-isotope dilution testing. Forty nonpregnant, nonlactating women (mean ± SD age: 22.4 ± 2.3 y) completed a Harvard food-frequency questionnaire (FFQ) and 3-d diet record (3DDR) before undergoing vitamin A status assessment by using a [(13)C2]retinol stable-isotope dilution test. Vitamin A intake was 70% higher than the RDA by both dietary-assessment methods (P < 0.001). The mean (±SD) liver concentration of vitamin A was 0.45 ± 0.31 μmol/g (129 ± 89 μg/g) and ranged from 0.09 (26 μg/g) to 1.79 μmol/g (513 μg/g). Liver and total-body vitamin A were highly correlated with intake measured by FFQ (P ≤ 0.009), but 3DDR was not (P ≥ 0.22). Prediction equations were developed for 3- and 7-d data. In this well-nourished population, vitamin A consumption was considerably higher than recommended, and liver reserves were consistent with intake. Because of their sensitivity, stable-isotope techniques can help to describe the vitamin A status and better characterize the intake needs of all groups defined in the Dietary Reference Intakes. Registration was not required for this trial.

  18. Technetium-99m pyrophosphate/thallium-201 dual-isotope SPECT imaging predicts reperfusion injury in patients with acute myocardial infarction after reperfusion

    Energy Technology Data Exchange (ETDEWEB)

    Akutsu, Yasushi; Kaneko, Kyouichi; Kodama, Yusuke; Li, Hui-Ling; Nishimura, Hideki; Hamazaki, Yuji; Kobayashi, Youichi [Showa University School of Medicine, Division of Cardiology, Department of Medicine, Tokyo (Japan); Suyama, Jumpei; Shinozuka, Akira; Gokan, Takehiko [Showa University School of Medicine, Department of Radiology, Tokyo (Japan)

    2009-02-15

    Microcirculatory failure after reperfusion is clinically indicated to cause reperfusion injury whereas excessive intracellular calcium ion overload is experimentally proved as a key mechanism of reperfusion injury. We hypothesized that technetium-99m ({sup 99m}Tc) pyrophosphate (Tc-PYP) uptake in injured but viable infarct-related myocardium with preserved myocardial perfusion after reperfusion estimated by thallium-201 ({sup 201}Tl) uptake would be associated with final functional recovery. Dual-isotope Tc-PYP/{sup 201}Tl single-photon emission computed tomography (SPECT) was performed 2 days after successful reperfusion therapy in patients with first acute myocardial infarction, and 50 patients (63 {+-} 13 years old, female 22%) with preserved {sup 201}Tl uptakes of {>=}50% in reperfused myocardium was followed for 1 month. Tc-PYP uptake was assessed as the heart-to-sternum (H/S) ratio. Two-dimensional echocardiography was also performed 2 days and 1 month after reperfusion to evaluate functional recovery. High Tc-PYP uptake, defined as the H/S ratio {>=}0.81, was predictive of chronic phase no functional recovery (73.7% in 14 of 19 patients with high uptake vs 16.1% in five of 31 patients without those, p < 0.0001). After adjustment for potential confounding variables, including electrocardiographic persistent ST segment elevation at 1 h after reperfusion, high Tc-PYP uptake remained independently predictive of no functional recovery with odds ratio of 8.7 (95% confidential interval = 2 to 38.7; p = 0.005). High Tc-PYP uptake in reperfused but viable infarct-related myocardium was a powerful predictor of no functional recovery, which may reflect excessive intracellular calcium ion overload caused by reperfusion injury. Tc-PYP/{sup 201}Tl dual-isotope SPECT imaging can provide prognostic information after reperfusion. (orig.)

  19. Vitamin A isotope dilution predicts liver stores in line with long-term vitamin A intake above the current Recommended Dietary Allowance for young adult women123

    Science.gov (United States)

    Valentine, Ashley R; Davis, Christopher R

    2013-01-01

    Background: The Estimated Average Requirement (EAR) and Recommended Dietary Allowance (RDA) for vitamin A are 1.7 and 2.4 μmol/d (500 and 700 μg retinol activity equivalents/d), respectively, for nonpregnant, nonlactating women aged >19 y. This intake is presumed to maintain a minimally acceptable liver concentration of 0.07 μmol (20 μg) retinol/g; however, liver reserves have not been evaluated with respect to vitamin A intake in women of any age group defined in the Dietary Reference Intakes. Objective: This cross-sectional study examined vitamin A intake and liver reserves estimated by stable-isotope dilution testing. Design: Forty nonpregnant, nonlactating women (mean ± SD age: 22.4 ± 2.3 y) completed a Harvard food-frequency questionnaire (FFQ) and 3-d diet record (3DDR) before undergoing vitamin A status assessment by using a [13C2]retinol stable-isotope dilution test. Results: Vitamin A intake was 70% higher than the RDA by both dietary-assessment methods (P < 0.001). The mean (±SD) liver concentration of vitamin A was 0.45 ± 0.31 μmol/g (129 ± 89 μg/g) and ranged from 0.09 (26 μg/g) to 1.79 μmol/g (513 μg/g). Liver and total-body vitamin A were highly correlated with intake measured by FFQ (P ≤ 0.009), but 3DDR was not (P ≥ 0.22). Prediction equations were developed for 3- and 7-d data. Conclusions: In this well-nourished population, vitamin A consumption was considerably higher than recommended, and liver reserves were consistent with intake. Because of their sensitivity, stable-isotope techniques can help to describe the vitamin A status and better characterize the intake needs of all groups defined in the Dietary Reference Intakes. Registration was not required for this trial. PMID:24047915

  20. Isotope separation

    Science.gov (United States)

    Bartlett, Rodney J.; Morrey, John R.

    1978-01-01

    A method and apparatus is described for separating gas molecules containing one isotope of an element from gas molecules containing other isotopes of the same element in which all of the molecules of the gas are at the same electronic state in their ground state. Gas molecules in a gas stream containing one of the isotopes are selectively excited to a different electronic state while leaving the other gas molecules in their original ground state. Gas molecules containing one of the isotopes are then deflected from the other gas molecules in the stream and thus physically separated.

  1. Leatherback Isotopes

    Data.gov (United States)

    National Oceanic and Atmospheric Administration, Department of Commerce — SWFSC is currently working on a project identifying global marine isotopes using leatherback turtles (Dermochelys coriacea) as the indicator species. We currently...

  2. Isotope Identification

    Energy Technology Data Exchange (ETDEWEB)

    Karpius, Peter Joseph [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2017-09-18

    The objective of this training modules is to examine the process of using gamma spectroscopy for radionuclide identification; apply pattern recognition to gamma spectra; identify methods of verifying energy calibration; and discuss potential causes of isotope misidentification.

  3. Predicting origins of passerines migrating through Canadian migration monitoring stations using stable-hydrogen isotope analyses of feathers: a new tool for bird conservation

    Directory of Open Access Journals (Sweden)

    Keith A. Hobson

    2015-06-01

    Full Text Available The Canadian Migration Monitoring Network (CMMN consists of standardized observation and migration count stations located largely along Canada's southern border. A major purpose of CMMN is to detect population trends of migratory passerines that breed primarily in the boreal forest and are otherwise poorly monitored by the North American Breeding Bird Survey (BBS. A primary limitation of this approach to monitoring is that it is currently not clear which geographic regions of the boreal forest are represented by the trends generated for each bird species at each station or group of stations. Such information on "catchment areas" for CMMN will greatly enhance their value in contributing to understanding causes of population trends, as well as facilitating joint trend analysis for stations with similar catchments. It is now well established that naturally occurring concentrations of deuterium in feathers grown in North America can provide information on their approximate geographic origins, especially latitude. We used stable hydrogen isotope analyses of feathers (δ²Hf from 15 species intercepted at 22 CMMN stations to assign approximate origins to populations moving through stations or groups of stations. We further constrained the potential catchment areas using prior information on potential longitudinal origins based upon bird migration trajectories predicted from band recovery data and known breeding distributions. We detected several cases of differences in catchment area of species passing through sites, and between seasons within species. We discuss the importance of our findings, and future directions for using this approach to assist conservation of migratory birds at continental scales.

  4. In vivo prediction of goat kids body composition from the deuterium oxide dilution space determined by isotope-ratio mass spectrometry.

    Science.gov (United States)

    Lerch, S; Lastel, M L; Grandclaudon, C; Brechet, C; Rychen, G; Feidt, C

    2015-09-01

    Deuterium oxide dilution space (DOS) determination is one of the most accurate methods for in vivo estimation of ruminant body composition. However, the time-consuming vacuum sublimation of blood preceding infrared spectroscopy analysis, which is traditionally used to determine deuterium oxide (DO) concentration, limits its current use. The use of isotope-ratio mass spectrometry (IRMS) to determine the deuterium enrichment and thus quantify DO in plasma could counteract this limitation by reducing the sample preparation for plasma deproteinisation through centrifugal filters. The aim of this study was to validate the DOS technique using IRMS in growing goat kids to establish in vivo prediction equations of body composition. Seventeen weaned male Alpine goat kids (8.6 wk old) received a hay-based diet supplemented with 2 types of concentrates providing medium ( = 9) or high ( = 8) energy levels. Kids were slaughtered at 14.0 ( = 1, medium-energy diet), 17.2 ( = 4, medium-energy diet, and = 4, high-energy diet), or 21.2 wk of age ( = 4, medium-energy diet, and = 4, high-energy diet). Two days before slaughter, DOS was determined after an intravenous injection of 0.2 g DO/kg body mass (BM) and the resulting study of DO dilution kinetics from 4 plasma samples (+5, +7, +29, and +31 h after injection). The deuterium enrichment was analyzed by IRMS. After slaughter, the gut contents were discarded, the empty body (EB) was minced, and EB water, lipid, protein, ash, and energy contents were measured by chemical analyses. Prediction equations for body components measured postmortem were computed from in vivo BM and DOS. The lack of postmortem variation of fat-free EB composition was confirmed (mean of 75.3% [SD 0.6] of water), and the proportion of lipids in the EB tended ( = 0.06) to be greater for the high-energy diet (13.1%) than for the medium-energy diet (11.1%). There was a close negative relationship (residual CV [rCV] = 3.9%, = 0.957) between EB water and lipid

  5. ISOTOPE SEPARATORS

    Science.gov (United States)

    Bacon, C.G.

    1958-08-26

    An improvement is presented in the structure of an isotope separation apparatus and, in particular, is concerned with a magnetically operated shutter associated with a window which is provided for the purpose of enabling the operator to view the processes going on within the interior of the apparatus. The shutier is mounted to close under the force of gravity in the absence of any other force. By closing an electrical circuit to a coil mouated on the shutter the magnetic field of the isotope separating apparatus coacts with the magnetic field of the coil to force the shutter to the open position.

  6. Stable isotope

    African Journals Online (AJOL)

    Results of the study suggest that there are two main carbon pathways for plankton and nekton in the Kariega estuary, carbon derived from the eelgrass and its associated epiphytes and carbon which has its origins in the salt marsh riparian vegetation and zooplankton. Keywords: stable isotope analysis; temperate estuary; ...

  7. Microbes: Agents of Isotopic Change

    Science.gov (United States)

    Fogel, M. L.

    2012-12-01

    Microbes drive many of the important oxidation and reduction reactions on Earth; digest almost all forms of organic matter; and can serve as both primary and secondary producers. Because of their versatile biochemistry and physiology, they impart unique isotopic signatures to organic and inorganic materials, which have proven to be key measurements for understanding elemental cycling now and throughout Earth's history. Understanding microbial isotope fractionations in laboratory experiments has been important for interpreting isotopic patterns measured in natural settings. In fact, the pairing of simple experiment with natural observation has been the pathway for interpreting the fingerprint of microbial processes in ancient sediments and rocks. Examples of how key experiments have explained stable isotope fractionations by microbes and advanced the field of microbial ecology will be presented. Learning the isotopic signatures of Earth's microbes is a valuable exercise for predicting what isotopic signatures could be displayed by possible extant or extinct extraterrestrial life. Given the potential for discovery on Mars, Enceladus, and other solar system bodies, new methods and techniques for pinpointing what is unique about microbial isotope signatures is particularly relevant.

  8. Crystal chemical constraints on inter-mineral Fe isotope fractionation and implications for Fe isotope disequilibrium in San Carlos mantle xenoliths

    OpenAIRE

    Macris, Catherine A.; Manning, Craig E.; Young, Edward D.

    2015-01-01

    The origin of variations in iron isotope compositions of mantle minerals is uncertain, and predictions of equilibrium inter-mineral iron isotope fractionation conflict. This hinders interpretation of the petrologic and geochemical implications of Fe isotope data from mantle lithologies. To address this, we present a revised ionic model for predicting equilibrium iron isotope fractionation between mantle minerals and use it to interpret measured inter-mineral iron isotopic fractionation from f...

  9. Using stable isotopes of albacore tuna and predictive models to characterize bioregions and examine ecological change in the SW Pacific Ocean

    Science.gov (United States)

    Pethybridge, Heidi R.; Young, Jock W.; Kuhnert, Petra M.; Farley, Jessica H.

    2015-05-01

    Broad-scale food web inferences of 534 albacore tuna, Thunnus alalunga, in the south-west Pacific Ocean in 2009 and 2010 were made using bulk nitrogen (δ15N) and carbon (δ13C) stable isotopes. Condition was also examined for the same fish using C:N ratios. A Generalized Additive Modeling (GAM) approach was used to analyze spatio-temporal, biological and environmental drivers that impact the distribution of tuna isotopes and to create oceanographic maps. Based on model formulations, five bioregions with distinct isotopic signatures were identified and were related to known biological, nutrient cycling and oceanographic (temperature, primary productivity and eddy) features associated with the East Australian Current. δ15N values showed a large-scale, uniform latitudinal gradient decreasing from the south to north, in a region encompassing oligotrophic waters in the Coral Sea. In contrast, δ13C values were lower in the nutrient rich Tasman Sea waters and offshore East Australia. C:N ratios suggested that albacore occupying southern and offshore waters were in better condition. Ontogenetic trends in all three biochemical parameters were identified and related to differences in size distribution. Regional-specific temporal variations were detected including similar monthly changes for both isotopes and significantly less enriched δ13C (by 1.9‰) than in previous work undertaken in 2006, potentially signifying a substantial shift in the carbon cycle that supports food webs off central east Australia. Our results showed that isotopic measurements in tuna and the GAM framework provide powerful tools to assess ecosystem functioning and change by linking sources of nutrients and organic matter to local food web assembly. Such knowledge is vital to support an ecosystem based approach to fisheries management including biogeochemical whole-of-ecosystem models and monitoring programs at regional and landscape-scales.

  10. New Isotope 263Hs

    Energy Technology Data Exchange (ETDEWEB)

    Dragojevic, I.; Gregorich, K.E.; Dullmann, Ch.E.; Dvorak, J.; Ellison, P.A.; Gates, J.M.; Nelson, S.L.; Stavsetra, L.; Nitsche, H.

    2010-03-16

    A new isotope of Hs was produced in the reaction 208Pb(56Fe, n)263Hs at the 88-Inch Cyclotron of the Lawrence Berkeley National Laboratory. Six genetically correlated nuclear decay chains have been observed and assigned to the new isotope 263Hs. The measured cross section was 21+13-8.4 pb at 276.4 MeV lab-frame center-of-target beam energy. 263Hs decays with a half-life of 0.74 ms by alpha-decay and the measured alpha-particle energies are 10.57 +- 0.06, 10.72 +- 0.06, and 10.89 +- 0.06 MeV. The experimental cross section is compared to a theoretical prediction based on the Fusion by Diffusion model [W. J. Swiatecki et al., Phys. Rev. C 71, 014602 (2005)].

  11. Fragmentation of exotic oxygen isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Leistenschneider, A.; Elze, Th.W.; Gruenschloss, A.; Palit, R. [Johann Wolfgang Goethe-Univ., Frankfurt (Germany). Inst. fuer Kernphysik; Aumann, T.; Cortina, D.; Datta Pramanik, U.; Emling, H.; Geissel, H.; Helariutta, K.; Hellstroem, M.; Ilievski, S.; Jones, K.; Muenzenberg, G.; Scheidenberger, C.; Schmidt, K.-H.; Suemmerer, K. [Gesellschaft fuer Schwerionenforschung (GSI), Darmstadt (Germany); Boretzky, K.; Kratz, J.V.; Le Hong, Khiem [Johannes Gutenberg-Univ., Mainz (Germany). Inst. fue Kernchemie; Canto, L.F. [Universidade Federal, Rio de Janeiro, RJ (Brazil). Inst. de Fisica; Carlson, B.V. [Centro Tecnico Aeroespacial (CTA), Sao Jose dos Campos, SP (Brazil). Inst. Tecnologico de Aeronautica (ITA). Dept. de Fisica; Hussein, M.S. [Sao Paulo Univ. (USP), SP (Brazil). Inst. de Fisica; Kulessa, R.; Lubkiewicz, E.; Wajda, E.; Walus, W. [Uniwersytet Jagellonski, Krakow (Poland). Instytut Fizyki; Reiter, P. [Ludwig-Maximilians-Univ., Garching (Germany). Sektion Physik; Simon, H. [Technische Univ., Darmstadt (Germany). Inst. fuer Kernphysik

    2003-06-01

    Abrasion-ablation models and the empirical EPAX parametrization of projectile fragmentation are described. Their cross section predictions are compared to recent data of the fragmentation of secondary beams of neutron-rich, unstable {sup 19,20,21} O isotopes at beam energies near 600 MeV/nucleon as well as data for stable {sup 17,18} O beams. (author)

  12. Modeling equilibrium Fe isotope fractionation

    Science.gov (United States)

    Anbar, A.; Jarzecki, A.; Spiro, T.

    2003-04-01

    Research into the stable isotope biogeochemistry of Fe and other transition metals has been driven primarily by analytical innovations which have revealed significant isotope effects in nature and the laboratory. Further development of these new isotope systems requires complementary theoretical research to guide analytical efforts. The results of the first such studies show some discrepancies with experiments. For example, Johnson et al. (2002) report an experimentally-determined 56Fe/54Fe equilibrium fractionation factor between Fe(II) and Fe(III) aquo complexes of ˜1.0025. This effect is ˜50% smaller than predicted theoretically by Schauble et al. (2001). It is important to resolve such discrepancies. Equilibrium isotope fractionation factors can be predicted from vibrational spectroscopic data of isotopically-substituted complexes, or from theoretical predictions of some or all of these frequencies obtained using force field models. The pioneering work of Schauble et al. (2001) utilized a modified Urey-Bradley force field (MUBFF) model. This approach is limiting in at least three ways: First, it is not ab initio, requiring as input some measured vibrational frequencies. Such data are not always available, or may have significant uncertainties. Second, the MUBFF does not include potentially important effects of solvent interaction. Third, because it makes certain assumptions about molecular symmetry, the MUBFF-based approach is not able to model the spectra of mixed-ligand complexes. To address these limitations, we are evaluating the use of density functional theory (DFT) as an ab initio method to predict vibrational frequencies of isotopically-substituted complexes and, hence, equilibrium fractionation factors. In a preliminary examination of the frequency shift upon isotope substitution of the bending and asymmetric stretching modes of the tetrahedral FeCl_42- complex, we find substantial differences between MUBFF and DFT predictions. Results for other Fe

  13. Stable isotope analysis in primatology: a critical review.

    Science.gov (United States)

    Sandberg, Paul A; Loudon, James E; Sponheimer, Matt

    2012-11-01

    Stable isotope analysis has become an important tool in ecology over the last 25 years. A wealth of ecological information is stored in animal tissues in the relative abundances of the stable isotopes of several elements, particularly carbon and nitrogen, because these isotopes navigate through ecological processes in predictable ways. Stable carbon and nitrogen isotopes have been measured in most primate taxonomic groups and have yielded information about dietary content, dietary variability, and habitat use. Stable isotopes have recently proven useful for addressing more fine-grained questions about niche dynamics and anthropogenic effects on feeding ecology. Here, we discuss stable carbon and nitrogen isotope systematics and critically review the published stable carbon and nitrogen isotope data for modern primates with a focus on the problems and prospects for future stable isotope applications in primatology. © 2012 Wiley Periodicals, Inc.

  14. Oxygen isotope fractionation in stratospheric CO2

    Science.gov (United States)

    Thiemens, M. H.; Jackson, T.; Mauersberger, K.; Schueler, B.; Morton, J.

    1991-01-01

    A new cryogenic collection system has been flown on board a balloon gondola to obtain separate samples of ozone and carbon dioxide without entrapping major atmospheric gases. Precision laboratory isotopic analysis of CO2 samples collected between 26 and 35.5 km show a mass-independent enrichment in both O-17 and O-18 of about 11 per mil above tropospheric values. Ozone enrichment in its heavy isotopes was 9 to 16 percent in O3-50 and 8 to 11 percent in O3-49, respectively (Schueler et al., 1990). A mechanism to explain the isotope enrichment in CO2 has been recently proposed by Yung et al. (1991). The model is based on the isotope exchange between CO2 and O3 via O(1D), resulting in a transfer of the ozone isotope enrichment to carbon dioxide. Predicted enrichment and measured values agree well.

  15. Prediction

    CERN Document Server

    Sornette, Didier

    2010-01-01

    This chapter first presents a rather personal view of some different aspects of predictability, going in crescendo from simple linear systems to high-dimensional nonlinear systems with stochastic forcing, which exhibit emergent properties such as phase transitions and regime shifts. Then, a detailed correspondence between the phenomenology of earthquakes, financial crashes and epileptic seizures is offered. The presented statistical evidence provides the substance of a general phase diagram for understanding the many facets of the spatio-temporal organization of these systems. A key insight is to organize the evidence and mechanisms in terms of two summarizing measures: (i) amplitude of disorder or heterogeneity in the system and (ii) level of coupling or interaction strength among the system's components. On the basis of the recently identified remarkable correspondence between earthquakes and seizures, we present detailed information on a class of stochastic point processes that has been found to be particu...

  16. Platinum isotopes in iron meteorites: Galactic cosmic ray effects and nucleosynthetic homogeneity in the p-process isotope 190Pt and the other platinum isotopes

    Science.gov (United States)

    Hunt, Alison C.; Ek, Mattias; Schönbächler, Maria

    2017-11-01

    Platinum isotopes are sensitive to the effects of galactic cosmic rays (GCR), which can alter isotope ratios and mask nucleosynthetic isotope variations. Platinum also features one p-process isotope, 190Pt, which is very low abundance and therefore challenging to analyse. Platinum-190 is relevant for early solar-system chronology because of its decay to 186Os. Here, we present new Pt isotope data for five iron meteorite groups (IAB, IIAB, IID, IIIAB and IVA), including high-precision measurements of 190Pt for the IAB, IIAB and IIIAB irons, determined by multi-collector ICPMS. New data are in good agreement with previous studies and display correlations between different Pt isotopes. The slopes of these correlations are well-reproduced by the available GCR models. We report Pt isotope ratios for the IID meteorite Carbo that are consistently higher than the predicted effects from the GCR model. This suggests that the model predictions do not fully account for all the GCR effects on Pt isotopes, but also that the pre-atmospheric radii and exposure times calculated for Carbo may be incorrect. Despite this, the good agreement of relative effects in Pt isotopes with the predicted GCR trends confirms that Pt isotopes are a useful in-situ neutron dosimeter. Once GCR effects are accounted for, our new dataset reveals s- and r-process homogeneity between the iron meteorite groups studied here and the Earth. New 190Pt data for the IAB, IIAB and IIIAB iron meteorites indicate the absence of GCR effects and homogeneity in the p-process isotope between these groups and the Earth. This corresponds well with results from other heavy p-process isotopes and suggests their homogenous distribution in the inner solar system, although it does not exclude that potential p-process isotope variations are too diluted to be currently detectable.

  17. METHOD OF ISOTOPE CONCENTRATION

    Science.gov (United States)

    Spevack, J.S.

    1957-04-01

    An isotope concentration process is described which consists of exchanging, at two or more different temperature stages, two isotopes of an element between substances that are physically separate from each other and each of which is capable of containing either of the isotopes, and withdrawing from a point between at least two of the temperatare stages one of the substances containing an increased concentration of the desired isotope.

  18. Statistical clumped isotope signatures

    NARCIS (Netherlands)

    Röckmann, T.; Popa, M.E.; Krol, M.C.; Hofmann, M.E.G.

    2016-01-01

    High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of

  19. Statistical clumped isotope signatures

    NARCIS (Netherlands)

    Röckmann, T.|info:eu-repo/dai/nl/304838233; Popa, M. E.|info:eu-repo/dai/nl/375806407; Krol, M. C.|info:eu-repo/dai/nl/078760410; Hofmann, M. E. G.|info:eu-repo/dai/nl/374642907

    2016-01-01

    High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of a

  20. Statistical clumped isotope signatures

    Science.gov (United States)

    Röckmann, T.; Popa, M. E.; Krol, M. C.; Hofmann, M. E. G.

    2016-01-01

    High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of a molecule, which is the conventional reference. When multiple indistinguishable atoms of the same element are present in a molecule, this reference is calculated from the bulk (≈average) isotopic composition of the involved atoms. We show here that this referencing convention leads to apparent negative clumped isotope anomalies (anti-clumping) when the indistinguishable atoms originate from isotopically different populations. Such statistical clumped isotope anomalies must occur in any system where two or more indistinguishable atoms of the same element, but with different isotopic composition, combine in a molecule. The size of the anti-clumping signal is closely related to the difference of the initial isotope ratios of the indistinguishable atoms that have combined. Therefore, a measured statistical clumped isotope anomaly, relative to an expected (e.g. thermodynamical) clumped isotope composition, may allow assessment of the heterogeneity of the isotopic pools of atoms that are the substrate for formation of molecules. PMID:27535168

  1. Isotopes in heterogeneous catalysis

    CERN Document Server

    Hargreaves, Justin SJ

    2006-01-01

    The purpose of this book is to review the current, state-of-the-art application of isotopic methods to the field of heterogeneous catalysis. Isotopic studies are arguably the ultimate technique in in situ methods for heterogeneous catalysis. In this review volume, chapters have been contributed by experts in the field and the coverage includes both the application of specific isotopes - Deuterium, Tritium, Carbon-14, Sulfur-35 and Oxygen-18 - as well as isotopic techniques - determination of surface mobility, steady state transient isotope kinetic analysis, and positron emission profiling.

  2. Hydrogen and oxygen isotope ratios in body water and hair: modeling isotope dynamics in nonhuman primates.

    Science.gov (United States)

    O'Grady, Shannon P; Valenzuela, Luciano O; Remien, Christopher H; Enright, Lindsey E; Jorgensen, Matthew J; Kaplan, Jay R; Wagner, Janice D; Cerling, Thure E; Ehleringer, James R

    2012-07-01

    The stable isotopic composition of drinking water, diet, and atmospheric oxygen influence the isotopic composition of body water ((2)H/(1)H, (18)O/(16)O expressed as δ(2) H and δ(18)O). In turn, body water influences the isotopic composition of organic matter in tissues, such as hair and teeth, which are often used to reconstruct historical dietary and movement patterns of animals and humans. Here, we used a nonhuman primate system (Macaca fascicularis) to test the robustness of two different mechanistic stable isotope models: a model to predict the δ(2)H and δ(18)O values of body water and a second model to predict the δ(2)H and δ(18)O values of hair. In contrast to previous human-based studies, use of nonhuman primates fed controlled diets allowed us to further constrain model parameter values and evaluate model predictions. Both models reliably predicted the δ(2)H and δ(18)O values of body water and of hair. Moreover, the isotope data allowed us to better quantify values for two critical variables in the models: the δ(2)H and δ(18)O values of gut water and the (18)O isotope fractionation associated with a carbonyl oxygen-water interaction in the gut (α(ow)). Our modeling efforts indicated that better predictions for body water and hair isotope values were achieved by making the isotopic composition of gut water approached that of body water. Additionally, the value of α(ow) was 1.0164, in close agreement with the only other previously measured observation (microbial spore cell walls), suggesting robustness of this fractionation factor across different biological systems. © 2012 Wiley Periodicals, Inc.

  3. Chromium isotope variations

    DEFF Research Database (Denmark)

    D'Arcy, Joan Mary

    Chromium (Cr) stable isotopes are a useful tracer of changes in redox conditions because changes in its oxidation state are accompanied by an isotopic fractionation. For this reason the Cr isotope system is being developed as a potential tool for paleo-redox reconstruction. Dissolved Cr in seawater...... is incorporated into carbonates. Hence, ancient carbonates can potentially record the Cr isotopic composition (δ53Cr ‰) of seawater in the geological past. Reliable application and interpretation of this proxy requires a detailed knowledge about processes that fractionate Cr on the Earth’s surface......, and the quantification the Cr isotope composition of major Cr fluxes into and out of ocean. This thesis adds to the current knowledge of the Cr isotope system and is divided into two studies. The focus of the first study was to determine what processes control the Cr isotopic compositionof river water and to quantify...

  4. Deformation properties of lead isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Tolokonnikov, S. V.; Borzov, I. N.; Lutostansky, Yu. S.; Saperstein, E. E., E-mail: saper43-7@mail.ru [National Research Center Kurchatov Institute (Russian Federation)

    2016-01-15

    The deformation properties of a long lead isotopic chain up to the neutron drip line are analyzed on the basis of the energy density functional (EDF) in the FaNDF{sup 0} Fayans form. The question of whether the ground state of neutron-deficient lead isotopes can have a stable deformation is studied in detail. The prediction of this deformation is contained in the results obtained on the basis of the HFB-17 and HFB-27 Skyrme EDF versions and reported on Internet. The present analysis reveals that this is at odds with experimental data on charge radii and magnetic moments of odd lead isotopes. The Fayans EDF version predicts a spherical ground state for all light lead isotopes, but some of them (for example, {sup 180}Pb and {sup 184}Pb) prove to be very soft—that is, close to the point of a phase transition to a deformed state. Also, the results obtained in our present study are compared with the predictions of some other Skyrme EDF versions, including SKM*, SLy4, SLy6, and UNE1. By and large, their predictions are closer to the results arising upon the application of the Fayans functional. For example, the SLy4 functional predicts, in just the same way as the FaNDF{sup 0} functional, a spherical shape for all nuclei of this region. The remaining three Skyrme EDF versions lead to a deformation of some light lead isotopes, but their number is substantially smaller than that in the case of the HFB-17 and HFB-27 functionals. Moreover, the respective deformation energy is substantially lower, which gives grounds to hope for the restoration of a spherical shape upon going beyond the mean-field approximation, which we use here. Also, the deformation properties of neutron-rich lead isotopes are studied up to the neutron drip line. Here, the results obtained with the FaNDF{sup 0} functional are compared with the predictions of the HFB-17, HFB-27, SKM*, and SLy4 Skyrme EDF versions. All of the EDF versions considered here predict the existence of a region where neutron

  5. Isotopic dependence of the caloric curve

    Science.gov (United States)

    Trautmann, W.; Adrich, P.; Aumann, T.; Bacri, C. O.; Barczyk, T.; Bassini, R.; Bianchin, S.; Boiano, C.; Botvina, A. S.; Boudard, A.; Brzychczyk, J.; Chbihi, A.; Cibor, J.; Czech, B.; De Napoli, M.; Ducret, J.-É.; Emling, H.; Frankland, J. D.; Hellström, M.; Henzlova, D.; Immè, G.; Iori, I.; Johansson, H.; Kezzar, K.; Lafriakh, A.; Le Fèvre, A.; Le Gentil, E.; Leifels, Y.; Lühning, J.; Łukasik, J.; Lynch, W. G.; Lynen, U.; Majka, Z.; Mocko, M.; Müller, W. F. J.; Mykulyak, A.; Orth, H.; Otte, A. N.; Palit, R.; Pawłowski, P.; Pullia, A.; Raciti, G.; Rapisarda, E.; Sann, H.; Schwarz, C.; Sfienti, C.; Simon, H.; Sümmerer, K.; Tsang, M. B.; Verde, G.; Volant, C.; Wallace, M.; Weick, H.; Wiechula, J.; Wieloch, A.; Zwiegliński, B.

    2009-04-01

    Isotopic effects in projectile fragmentation at relativistic energies have been studied with the ALADIN forward spectrometer at SIS. Stable and radioactive Sn and La beams with an incident energy of 600 MeV per nucleon have been used in order to explore a wide range of isotopic compositions. Chemical freeze-out temperatures are found to be nearly invariant with respect to the A/Z ratio of the produced spectator sources, consistent with predictions for expanded systems. Consequences for the proposed interpretation of chemical breakup temperatures as representing the limiting temperatures predicted by microscopic models are discussed.

  6. Chlorine isotope fractionation between chloride (Cl-) and dichlorine (Cl2)

    Science.gov (United States)

    Giunta, Thomas; Labidi, Jabrane; Eggenkamp, Hans G. M.

    2017-09-01

    The use of chlorine stable isotopes (35Cl and 37Cl) can help to constrain natural processes that involve chlorine species with different oxidation states. Theoretical studies based on thermodynamic and quantum mechanical approaches predict large isotope fractionation during redox reactions but to date, these reactions have not been studied experimentally.

  7. Redefining the utility of the three-isotope method

    Science.gov (United States)

    Cao, Xiaobin; Bao, Huiming

    2017-09-01

    The equilibrium isotope fractionation factor αeq is a fundamental parameter in the study of stable isotope effects. Experimentally, it has been difficult to establish that a system has attained equilibrium. The three-isotope method, using the initial trajectory of changing isotope ratios (e.g. 16O, 17O, and 18O) to deduce the final equilibrium point of isotope exchange, has long been hailed as the most rigorous experimental approach. However, over the years some researchers have cautioned on the limitations of this method, but the foundation of three-isotope method has not been properly examined and the method is still widely used in calibrating αeq for both traditional and increasingly non-traditional isotope systems today. Here, using water-water and dissolved CO2-water oxygen exchange as model systems, we conduct an isotopologues-specific kinetic analysis of the exchange processes and explore the underlying assumptions and validity of the three-isotope method. We demonstrate that without knowing the detailed exchange kinetics a priori the three-isotope method cannot lead to a reliable αeq. For a two-reservoir exchanging system, α determined by this method may be αeq, kinetic isotope effect, or apparent kinetic isotope effect, which can all bear different values. When multiple reservoirs exist during exchange, the evolving trajectory can be complex and hard to predict. Instead of being a tool for αeq determination, three-isotope method should be used as a tool for studying kinetic isotope effect, apparent kinetic isotope effect, and detailed exchange kinetics in diverse systems.

  8. Heavy Stable Isotopes: From Exceptional to Expected

    Science.gov (United States)

    Anbar, A.

    2006-12-01

    effect unrelated to Mo redox chemistry. Because the extent of Mn-oxide deposition on the seafloor is a function of ocean oxygenation, Mo isotopes are nevertheless emerging as a powerful ocean redox proxy (Arnold et al., 2004). Collectively, these and other findings demonstrate that MC-ICP-MS analyses open the door to rich new research areas, particularly when analyses of natural samples are combined with laboratory experiments and computational predictions to gain insight into fractionation mechanisms.

  9. Identifying migrations in marine fishes through stable-isotope analysis.

    Science.gov (United States)

    Trueman, C N; MacKenzie, K M; Palmer, M R

    2012-07-01

    The isotopic composition of many elements varies across both land and ocean surfaces in a predictable fashion. These stable-isotope ratios are transferred into animal tissues, potentially providing a powerful natural geospatial tag. To date, most studies using stable isotopes as geolocators in marine settings have focussed on mammals and seabirds conducting large ocean-basin scale migrations. An increasing understanding of isotopic variation in the marine environment, and improved sampling and analytical techniques, however, means that stable isotopes now hold genuine promise as a natural geolocation tag in marine fishes. Here, the theoretical background underpinning the use of stable isotopes of C, N and O in otolith, scale and muscle tissues as geolocation tools in the marine environment is reviewed, and examples of their applications are provided. © 2012 The Authors. Journal of Fish Biology © 2012 The Fisheries Society of the British Isles.

  10. Diffusional exchange of isotopes in a metal hydride sphere.

    Energy Technology Data Exchange (ETDEWEB)

    Wolfer, Wilhelm G.; Hamilton, John C.; James, Scott Carlton

    2011-04-01

    This report describes the Spherical Particle Exchange Model (SPEM), which simulates exchange of one hydrogen isotope by another hydrogen isotope in a spherical metal hydride particle. This is one of the fundamental physical processes during isotope exchange in a bed of spherical metal particles and is thus one of the key components in any comprehensive physics-based model of exchange. There are two important physical processes in the model. One is the entropy of mixing between the two isotopes; the entropy of mixing is increased by having both isotopes randomly placed at interstitial sites on the lattice and thus impedes the exchange process. The other physical process is the elastic interaction between isotope atoms on the lattice. The elastic interaction is the cause for {beta}-phase formation and is independent of the isotope species. In this report the coupled diffusion equations for two isotopes in the {beta}-phase hydride are solved. A key concept is that the diffusion of one isotope depends not only on its concentration gradient, but also on the concentration gradient of the other isotope. Diffusion rate constants and the chemical potentials for deuterium and hydrogen in the {beta}-phase hydride are reviewed because these quantities are essential for an accurate model of the diffusion process. Finally, a summary of some of the predictions from the SPEM model are provided.

  11. Uniform Silicon Isotope Ratios Across the Milky Way Galaxy

    Science.gov (United States)

    Monson, Nathaniel N.; Morris, Mark R.; Young, Edward D.

    2017-04-01

    We report the relative abundances of the three stable isotopes of silicon, 28Si, 29Si, and 30Si, across the Galaxy using the v=0,J=1\\to 0 transition of silicon monoxide. The chosen sources represent a range in Galactocentric radii ({R}{GC}) from 0 to 9.8 kpc. The high spectral resolution and sensitivity afforded by the Green Bank Telescope permit isotope ratios to be corrected for optical depths. The optical-depth-corrected data indicate that the secondary-to-primary silicon isotope ratios {}29{Si}{/}28{Si} and {}30{Si}{/}28{Si} vary much less than predicted on the basis of other stable isotope ratio gradients across the Galaxy. Indeed, there is no detectable variation in Si isotope ratios with {R}{GC}. This lack of an isotope ratio gradient stands in stark contrast to the monotonically decreasing trend with {R}{GC} exhibited by published secondary-to-primary oxygen isotope ratios. These results, when considered in the context of the expectations for chemical evolution, suggest that the reported oxygen isotope ratio trends, and perhaps those for carbon as well, require further investigation. The methods developed in this study for SiO isotopologue ratio measurements are equally applicable to Galactic oxygen, carbon, and nitrogen isotope ratio measurements, and should prove useful for future observations of these isotope systems.

  12. Discovery of the Indium Isotopes

    CERN Document Server

    Amos, S

    2010-01-01

    Thirty-eight indium isotopes (A = 98-135) have so far been observed; the discovery of these isotopes is discussed. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  13. Nickel isotopic composition of the mantle

    Science.gov (United States)

    Gall, Louise; Williams, Helen M.; Halliday, Alex N.; Kerr, Andrew C.

    2017-02-01

    This paper presents a detailed high-precision study of Ni isotope variations in mantle peridotites and their minerals, komatiites as well as chondritic and iron meteorites. Ultramafic rocks display a relatively large range in δ60 Ni (permil deviation in 60 Ni /58 Ni relative to the NIST SRM 986 Ni isotope standard) for this environment, from 0.15 ± 0.07‰ to 0.36 ± 0.08‰, with olivine-rich rocks such as dunite and olivine cumulates showing lighter isotope compositions than komatiite, lherzolite and pyroxenite samples. The data for the mineral separates shed light on the origin of these variations. Olivine and orthopyroxene display light δ60 Ni whereas clinopyroxene and garnet are isotopically heavy. This indicates that peridotite whole-rock δ60 Ni may be controlled by variations in modal mineralogy, with the prediction that mantle melts will display variable δ60 Ni values due to variations in residual mantle and cumulate mineralogy. Based on fertile peridotite xenoliths and Phanerozoic komatiite samples it is concluded that the upper mantle has a relatively homogeneous Ni isotope composition, with the best estimate of δ60Nimantle being 0.23 ± 0.06‰ (2 s.d.). Given that >99% of the Ni in the silicate Earth is located in the mantle, this also defines the Ni isotope composition of the Bulk Silicate Earth (BSE). This value is nearly identical to the results obtained for a suite of chondrites and iron meteorites (mean δ60 Ni 0.26 ± 0.12‰ and 0.29 ± 0.10‰, respectively) showing that the BSE is chondritic with respect to its Ni isotope composition, with little to no Ni mass-dependent isotope fractionation resulting from core formation.

  14. Linking hydrogen (δ2H) isotopes in feathers and precipitation: sources of variance and consequences for assignment to isoscapes

    National Research Council Canada - National Science Library

    Hobson, Keith A; Van Wilgenburg, Steven L; Wassenaar, Leonard I; Larson, Keith

    2012-01-01

    .... Naturally occurring stable isotopes of H (δ(2)H) in feathers provide an alternative intrinsic marker of animal origin due to the predictable spatial linkage to underlying hydrologically driven flow of H isotopes into foodwebs...

  15. SHELL ISOTOPE GEOCHEMISTRY

    African Journals Online (AJOL)

    Valley. Although fossil specimens of this subspecies have been used in palaeoclimatic reconstruction, there have been no previous reports of living examples. Here We describe the local habitat, climate and some aspects of ecology and isotopic variation within the snail shell. If isotope data can be obtained for fossil shells, ...

  16. ICT: isotope correction toolbox.

    Science.gov (United States)

    Jungreuthmayer, Christian; Neubauer, Stefan; Mairinger, Teresa; Zanghellini, Jürgen; Hann, Stephan

    2016-01-01

    Isotope tracer experiments are an invaluable technique to analyze and study the metabolism of biological systems. However, isotope labeling experiments are often affected by naturally abundant isotopes especially in cases where mass spectrometric methods make use of derivatization. The correction of these additive interferences--in particular for complex isotopic systems--is numerically challenging and still an emerging field of research. When positional information is generated via collision-induced dissociation, even more complex calculations for isotopic interference correction are necessary. So far, no freely available tools can handle tandem mass spectrometry data. We present isotope correction toolbox, a program that corrects tandem mass isotopomer data from tandem mass spectrometry experiments. Isotope correction toolbox is written in the multi-platform programming language Perl and, therefore, can be used on all commonly available computer platforms. Source code and documentation can be freely obtained under the Artistic License or the GNU General Public License from: https://github.com/jungreuc/isotope_correction_toolbox/ {christian.jungreuthmayer@boku.ac.at,juergen.zanghellini@boku.ac.at} Supplementary data are available at Bioinformatics online. © The Author 2015. Published by Oxford University Press. All rights reserved. For Permissions, please e-mail: journals.permissions@oup.com.

  17. Water isotope systematics: Improving our palaeoclimate interpretations

    Science.gov (United States)

    Jones, M. D.; Dee, S.; Anderson, L.; Baker, A.; Bowen, G.; Noone, D.

    2016-01-01

    The stable isotopes of oxygen and hydrogen, measured in a variety of archives, are widely used proxies in Quaternary Science. Understanding the processes that control δ18O change have long been a focus of research (e.g. Shackleton and Opdyke, 1973; Talbot, 1990 ; Leng, 2006). Both the dynamics of water isotope cycling and the appropriate interpretation of geological water-isotope proxy time series remain subjects of active research and debate. It is clear that achieving a complete understanding of the isotope systematics for any given archive type, and ideally each individual archive, is vital if these palaeo-data are to be used to their full potential, including comparison with climate model experiments of the past. Combining information from modern monitoring and process studies, climate models, and proxy data is crucial for improving our statistical constraints on reconstructions of past climate variability.As climate models increasingly incorporate stable water isotope physics, this common language should aid quantitative comparisons between proxy data and climate model output. Water-isotope palaeoclimate data provide crucial metrics for validating GCMs, whereas GCMs provide a tool for exploring the climate variability dominating signals in the proxy data. Several of the studies in this set of papers highlight how collaborations between palaeoclimate experimentalists and modelers may serve to expand the usefulness of palaeoclimate data for climate prediction in future work.This collection of papers follows the session on Water Isotope Systematics held at the 2013 AGU Fall Meeting in San Francisco. Papers in that session, the breadth of which are represented here, discussed such issues as; understanding sub-GNIP scale (Global Network for Isotopes in Precipitation, (IAEA/WMO, 2006)) variability in isotopes in precipitation from different regions, detailed examination of the transfer of isotope signals from precipitation to geological archives, and the

  18. Site-Specific Carbon Isotopes in Organics

    Science.gov (United States)

    Piasecki, A.; Eiler, J. M.

    2012-12-01

    propane and labeled propane (13CH3-12CH2-12CH3). Results are consistent with the expected relative fractionations between the two fragments, indicating limited 'scrambling' of carbon positions of less than 2% in the source. The limits of precision of this method are currently ~0.5 ‰, sufficient to resolve known or suspected position-specific isotope effects in propane. We have explored the expected temperature-dependent equilibrium isotopic distributions of propane using density functional theory and quantum mechanical models of vibrational isotope effects. These models predict the homogeneous isotope exchange equilibria among the various isotopologues of propane, which include several of a wide range of effects that should be measurable by our methods. At 300 K we predict that the central carbon site is 15‰ higher in δ13C and 95 ‰ higher in δD than the terminal carbon site; similarly the molecule containing both a 13C and D in the central site is enriched by ~120 ‰ relative to a random isotopic distribution at 300 K. These predictions present targets for future experimental and empirical studies of the temperature dependence of isotopic ordering in propane. More generally, the methods we are developing for the study of intramolecular isotopic distributions in propane will serve as a model for future study of similar effects in other organic compounds. [1]DeNiro, Epstein (1977) Science Volume 197, 261-263.

  19. Carbon Isotopes in an Earth System Model

    Science.gov (United States)

    Cuntz, M.; Reick, C. H.; Maier-Reimer, E.; Heimann, M.; Scholze, M.; Naegler, T.

    2009-04-01

    We present first calculations of the carbon isotopic composition of carbon dioxide in the Earth System Model (ESM) COSMOS. Earth System models consist of coupled models of the ocean, the atmosphere, the land surface, the biosphere (marine and terrestrial, plants and soils), and the cryosphere (snow and ice). In COSMOS from the Max Planck Institute for Meteorology, Hamburg, Germany, these components are the model of the atmospheric circulation ECHAM, the physical ocean model MPI-OM, the land surface parameterisation JSBACH and the oceanic carbon cycle model HAMOCC. The ESM COSMOS therefore calculates its own climate and CO2 concentrations during the diel course with a few degrees resolution, driven only by solar activity and human perturbations. The new model version now computes the multiple fractionation processes occurring during uptake of CO2 from the atmosphere by the terrestrial and marine biosphere. The model then redistributes the isotopic compositions in the land and ocean biospheres, including respiration, phenology, fire, land-use change and carbon export. This means that it includes a full isotopic carbon cycle, in the atmosphere, the ocean and on land. The model calculates not only the stable carbon isotope signatures but also radiocarbon activities in the Earth System. It will include in future the radiocarbon perturbation due to nuclear bomb tests. We compare first results of the ESM with other global estimates of terrestrial discrimination. We also compare predicted zonal and seasonal variations of isotope ratios in atmospheric CO2 with measurements from the GLOBALVIEW flask network. The stable and radioactive carbon isotopes are excellent tests for the overall model performance but also for individual model components. For example radiocarbon will be used to test stratosphere-troposphere exchange, ocean circulation and air-sea gas exchange. The isotope-enabled model can be used in future for example to predict carbon isotope ratios of terrestrial

  20. Chemical stability of levoglucosan: an isotopic perspective

    Science.gov (United States)

    Sang, Xuefang; Gensch, Iulia; Schlag, Patrick; Wildt, Juergen; Laumer, Werner; Kammer, Beatrix; Tillmann, Ralf; Chitwan, Ojha; Heinichen, Gesa; Kiendler-scharr, Astrid

    2014-05-01

    Levoglucosan, used in receptor models as a specific tracer of biomass burning aerosols, has long been considered chemically stable in the atmosphere. Recent laboratory investigations found significant chemical degradation of levoglucosan when exposed to OH radicals (Hennigan et al., 2010). Stable carbon isotopic analyses, complementarily to concentration measurements, can provide additional evidence for physical and chemical processing in the atmosphere, since chemical processing causes changes in the relative abundance between heavy and light isotopes due to kinetic isotope effect (KIE). In this study, the chemical stability of levoglucosan was studied by exploring the isotopic fractionation of the reactant during the oxidation by OH. Mixed particles with levoglucosan and ammonium sulfate were generated in a continuous-stirred flow reactor and exposed to different levels of OH. Levoglucosan chemical degradation as function of OH exposure was derived from the decrease of levoglucosan/(NH4)2SO4 concentration ratios using aerosol mass spectrometry (AMS). Filter samples were collected for off-line isotopic analyses. Liquid extraction - Gas Chromatography - Isotope Ratio Mass Spectrometry (LE-GC-IRMS) was applied to measure stable carbon isotope ratios of levoglucosan. The observed d13C became more positive with increasing OH exposure, showing isotopic fractionations up to 3 ‰ at a reactant conversion of 45%. From the dependence of levoglucosan d13C on the OH exposure, a KIE of 1.00451 was derived, being within the range of predicted values for alkanes and alkenes with the same number of carbon atoms. With known source isotopic composition of levoglucosan in biomass burning aerosol (Sang et al., 2012), ambient measurements of levoglucosan d13C composition can therefore be used to determine the extent of chemical processing at the observation site. Reference: Hennigan, C. J., et al. 2010. Levoglucosan stability in biomass burning particles exposed to hydroxyl radicals

  1. Modeling nuclear volume isotope effects in crystals

    Science.gov (United States)

    Schauble, Edwin A.

    2013-01-01

    Mass-independent isotope fractionations driven by differences in volumes and shapes of nuclei (the field shift effect) are known in several elements and are likely to be found in more. All-electron relativistic electronic structure calculations can predict this effect but at present are computationally intensive and limited to modeling small gas phase molecules and clusters. Density functional theory, using the projector augmented wave method (DFT-PAW), has advantages in greater speed and compatibility with a three-dimensional periodic boundary condition while preserving information about the effects of chemistry on electron densities within nuclei. These electron density variations determine the volume component of the field shift effect. In this study, DFT-PAW calculations are calibrated against all-electron, relativistic Dirac–Hartree–Fock, and coupled-cluster with single, double (triple) excitation methods for estimating nuclear volume isotope effects. DFT-PAW calculations accurately reproduce changes in electron densities within nuclei in typical molecules, when PAW datasets constructed with finite nuclei are used. Nuclear volume contributions to vapor–crystal isotope fractionation are calculated for elemental cadmium and mercury, showing good agreement with experiments. The nuclear-volume component of mercury and cadmium isotope fractionations between atomic vapor and montroydite (HgO), cinnabar (HgS), calomel (Hg2Cl2), monteponite (CdO), and the CdS polymorphs hawleyite and greenockite are calculated, indicating preferential incorporation of neutron-rich isotopes in more oxidized, ionically bonded phases. Finally, field shift energies are related to Mössbauer isomer shifts, and equilibrium mass-independent fractionations for several tin-bearing crystals are calculated from 119Sn spectra. Isomer shift data should simplify calculations of mass-independent isotope fractionations in other elements with Mössbauer isotopes, such as platinum and uranium

  2. Modeling nuclear volume isotope effects in crystals.

    Science.gov (United States)

    Schauble, Edwin A

    2013-10-29

    Mass-independent isotope fractionations driven by differences in volumes and shapes of nuclei (the field shift effect) are known in several elements and are likely to be found in more. All-electron relativistic electronic structure calculations can predict this effect but at present are computationally intensive and limited to modeling small gas phase molecules and clusters. Density functional theory, using the projector augmented wave method (DFT-PAW), has advantages in greater speed and compatibility with a three-dimensional periodic boundary condition while preserving information about the effects of chemistry on electron densities within nuclei. These electron density variations determine the volume component of the field shift effect. In this study, DFT-PAW calculations are calibrated against all-electron, relativistic Dirac-Hartree-Fock, and coupled-cluster with single, double (triple) excitation methods for estimating nuclear volume isotope effects. DFT-PAW calculations accurately reproduce changes in electron densities within nuclei in typical molecules, when PAW datasets constructed with finite nuclei are used. Nuclear volume contributions to vapor-crystal isotope fractionation are calculated for elemental cadmium and mercury, showing good agreement with experiments. The nuclear-volume component of mercury and cadmium isotope fractionations between atomic vapor and montroydite (HgO), cinnabar (HgS), calomel (Hg2Cl2), monteponite (CdO), and the CdS polymorphs hawleyite and greenockite are calculated, indicating preferential incorporation of neutron-rich isotopes in more oxidized, ionically bonded phases. Finally, field shift energies are related to Mössbauer isomer shifts, and equilibrium mass-independent fractionations for several tin-bearing crystals are calculated from (119)Sn spectra. Isomer shift data should simplify calculations of mass-independent isotope fractionations in other elements with Mössbauer isotopes, such as platinum and uranium.

  3. Oxygen isotope fractionation in double carbonates.

    Science.gov (United States)

    Zheng, Yong-Fei; Böttcher, Michael E

    2016-01-01

    Oxygen isotope fractionations in double carbonates of different crystal structures were calculated by the increment method. Synthesis experiments were performed at 60 °C and 100 °C to determine oxygen and carbon isotope fractionations involving PbMg[CO3]2. The calculations suggest that the double carbonates of calcite structure are systematically enriched in (18)O relative to those of aragonite and mixture structures. Internally consistent oxygen isotope fractionation factors are obtained for these minerals with respect to quartz, calcite and water at a temperature range of 0-1200 °C. The calculated fractionation factors for double carbonate-water systems are generally consistent with the data available from laboratory experiments. The experimentally determined fractionation factors for PbMg[CO3]2, BaMg[CO3]2 and CaMg[CO3]2 against H2O not only fall between fractionation factors involving pure carbonate end-members but are also close to the calculated fractionation factors. In contrast, experimentally determined carbon isotope fractionation factors between PbMg[CO3]2 and CO2 are much closer to theoretical predictions for the cerussite-CO2 system than for the magnesite-CO2 system, similar to the fractionation behavior for BaMg[CO3]2. Therefore, the combined theoretical and experimental results provide insights into the effects of crystal structure and exchange kinetics on oxygen isotope partitioning in double carbonates.

  4. Isotopes through the looking glass

    Science.gov (United States)

    Mårtensson Pendrill, Ann Marie

    2000-08-01

    Nuclear distributions affect many aspects of atomic spectra. As an example, recent experimental results for the hyperfine anomaly in Fr isotopes are considered. These depend on nuclear charge and magnetization distributions. The variations in charge radii for these isotopes were studied earlier by measuring optical isotope shifts. The hyperfine anomalies for the odd-odd isotopes involve the neutron distributions, of interest for studies of parity nonconserving effects along a chain of isotopes.

  5. Calcium stable isotope geochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Gausonne, Nikolaus [Muenster Univ. (Germany). Inst. fuer Mineralogie; Schmitt, Anne-Desiree [Strasbourg Univ. (France). LHyGeS/EOST; Heuser, Alexander [Bonn Univ. (Germany). Steinmann-Inst. fuer Geologie, Mineralogie und Palaeontologie; Wombacher, Frank [Koeln Univ. (Germany). Inst. fuer Geologie und Mineralogie; Dietzel, Martin [Technische Univ. Graz (Austria). Inst. fuer Angewandte Geowissenschaften; Tipper, Edward [Cambridge Univ. (United Kingdom). Dept. of Earth Sciences; Schiller, Martin [Copenhagen Univ. (Denmark). Natural History Museum of Denmark

    2016-08-01

    This book provides an overview of the fundamentals and reference values for Ca stable isotope research, as well as current analytical methodologies including detailed instructions for sample preparation and isotope analysis. As such, it introduces readers to the different fields of application, including low-temperature mineral precipitation and biomineralisation, Earth surface processes and global cycling, high-temperature processes and cosmochemistry, and lastly human studies and biomedical applications. The current state of the art in these major areas is discussed, and open questions and possible future directions are identified. In terms of its depth and coverage, the current work extends and complements the previous reviews of Ca stable isotope geochemistry, addressing the needs of graduate students and advanced researchers who want to familiarize themselves with Ca stable isotope research.

  6. Isotope Production Facility (IPF)

    Data.gov (United States)

    Federal Laboratory Consortium — The Los Alamos National Laboratory has produced radioactive isotopes for medicine and research since the mid 1970s, when targets were first irradiated using the 800...

  7. Isotopes in Greenland Precipitation

    DEFF Research Database (Denmark)

    Faber, Anne-Katrine

    ) Constructing a new Greenland database of observations and present-day ice core measurements, and (3) Performance test of isotope-enabled CAM5 for Greenland. The recent decades of rapid Arctic sea ice decline are used as a basis for an observational-based model experiment using the isotope-enabled CAM model 3....... The simulation of Greenland isotopes is tested for the isotope-enabled model CAM5. Here the importance of model resolution is investigated. A positive bias of 6-10 ‰ is found for the annual mean δ18O on the central part of the Greenland Ice Sheet. The amplitude of the seasonal cycle of Greenland δ18O is highly...

  8. Oxygen isotope geochemistry of the amphiboles: Isotope effects of cation substitutions in minerals

    Energy Technology Data Exchange (ETDEWEB)

    Kohn, M.J. [Lawrence Livermore National Lab., CA (United States); Valley, J.W. [Univ. of Wisconsin, Madison, WI (United States). Dept. of Geology and Geophysics

    1998-06-01

    The occurrence of coexisting amphiboles in rocks and the likelihood of concurrent isotope closure allows equilibrium oxygen isotope fractionations among the amphiboles to be recovered from natural samples. Oxygen isotope analyses of mineral separates using laser fluorination show that coexisting amphiboles increasingly partition {sup 18}O in the order: hornblende {much_lt} gedrite < cummingtonite {le} anthophyllite. The observed fractionations at {approximately}575 C are: {Delta}(Ged-Hbl) = 0.8%, {Delta}(Cum-Hbl) = 0.9, {Delta}(Cum-Ged) = 0.2, {Delta}(Ath-Ged) = 0.3, and {Delta}(Ath-Hbl) > 0.9. Previously published data for hornblende, actinolite, glaucophane, and garnet show that {Delta}(Act-Hbl) {approximately} 0.2, {Delta}(Gin-Grt) {much_gt} 1, and {Delta}(Hbl-Grt) {approximately} 0. Thus, glaucophane strongly partitions {sup 18}O relative to the calcic amphiboles. The fractionation between two amphiboles of arbitrary composition can be predicted from the known fractionations for mica endmembers, pyroxene endmembers, and exchange components. Applications of the exchange component method reproduce measured amphibole fractionations to within {+-}0.1 to {+-}0.2%, whereas other predictive methods cause misfit for typical metamorphic hornblende of {ge}0.5% at 575 C. Although the isotope effects of cation exchanges may be small at high-T, they magnify dramatically for minerals formed in surficial, diagenetic, and low-T metamorphic environments. Different composition clays are predicted to have equilibrium {delta}{sup 18}O differences of 2--9%. If the isotope fractionation can be determined for one mineral endmember, then calibrated exchanges allow accurate prediction of the isotope fractionations for intermediate compositions of most ortho-, ring-, chain-, and sheet-silicates.

  9. Isotope toolbox turns 10

    DEFF Research Database (Denmark)

    Wenander, Fredrik; Riisager, Karsten

    2012-01-01

    REX-ISOLDE, one of CERN’s most compact accelerators, has just celebrated its 10th anniversary. The machine’s versatility provides radioactive ion beams across the range of nuclear isotopes.......REX-ISOLDE, one of CERN’s most compact accelerators, has just celebrated its 10th anniversary. The machine’s versatility provides radioactive ion beams across the range of nuclear isotopes....

  10. Isotope research materials

    Energy Technology Data Exchange (ETDEWEB)

    Wilkinson, M. K.; Young, Jr, F. W.

    1977-10-01

    Preparation of research isotope materials is described. Topics covered include: separation of tritium from aqueous effluents by bipolar electrolysis; stable isotope targets and research materials; radioisotope targets and research materials; preparation of an 241Am metallurgical specimen; reactor dosimeters; ceramic and cermet development; fission-fragment-generating targets of 235UO2; and wire dosimeters for Westinghouse--Bettis. (GHT)

  11. Spatial distribution of stable water isotopes in alpine snow cover

    Directory of Open Access Journals (Sweden)

    N. Dietermann

    2013-07-01

    Full Text Available The aim of this study was to analyse and predict the mean stable water isotopic composition of the snow cover at specific geographic locations and altitudes. In addition, the dependence of the isotopic composition of the entire snow cover on altitude was analysed. Snow in four Swiss catchments was sampled at the end of the accumulation period in April 2010 and a second time during snowmelt in May 2010 and analysed for stable isotope composition of 2H and 18O. The sampling was conducted at both south-facing and north-facing slopes at elevation differences of 100 m, for a total altitude difference of approximately 1000 m. The observed variability of isotopic composition of the snow cover was analysed with stepwise multiple linear regression models. The analysis indicated that there is only a limited altitude effect on the isotopic composition when considering all samples. This is due to the high variability of the isotopic composition of the precipitation during the winter months and, in particular in the case of south-facing slopes, an enrichment of heavy isotopes due to intermittent melting processes. This enrichment effect could clearly be observed in the samples which were taken later in the year. A small altitudinal gradient of the isotopic composition could only be observed at some north-facing slopes. However, the dependence of snow depth and the day of the year were significant predictor variables in all models. This study indicates the necessity to further study the variability of water isotopes in the snow cover to increase prediction for isotopic composition of snowmelt and hence increase model performance of residence time models for alpine areas in order to better understand the accumulation processes and the sources of water in the snow cover of high mountains.

  12. Spatial distribution of stable water isotopes in alpine snow cover

    Science.gov (United States)

    Dietermann, N.; Weiler, M.

    2013-07-01

    The aim of this study was to analyse and predict the mean stable water isotopic composition of the snow cover at specific geographic locations and altitudes. In addition, the dependence of the isotopic composition of the entire snow cover on altitude was analysed. Snow in four Swiss catchments was sampled at the end of the accumulation period in April 2010 and a second time during snowmelt in May 2010 and analysed for stable isotope composition of 2H and 18O. The sampling was conducted at both south-facing and north-facing slopes at elevation differences of 100 m, for a total altitude difference of approximately 1000 m. The observed variability of isotopic composition of the snow cover was analysed with stepwise multiple linear regression models. The analysis indicated that there is only a limited altitude effect on the isotopic composition when considering all samples. This is due to the high variability of the isotopic composition of the precipitation during the winter months and, in particular in the case of south-facing slopes, an enrichment of heavy isotopes due to intermittent melting processes. This enrichment effect could clearly be observed in the samples which were taken later in the year. A small altitudinal gradient of the isotopic composition could only be observed at some north-facing slopes. However, the dependence of snow depth and the day of the year were significant predictor variables in all models. This study indicates the necessity to further study the variability of water isotopes in the snow cover to increase prediction for isotopic composition of snowmelt and hence increase model performance of residence time models for alpine areas in order to better understand the accumulation processes and the sources of water in the snow cover of high mountains.

  13. Shifts in rotifer life history in response to stable isotope enrichment: testing theories of isotope effects on organismal growth.

    Science.gov (United States)

    Gorokhova, Elena

    2017-03-01

    In ecology, stable isotope labelling is commonly used for tracing material transfer in trophic interactions, nutrient budgets and biogeochemical processes. The main assumption in this approach is that the enrichment with a heavy isotope has no effect on the organism growth and metabolism. This assumption is, however, challenged by theoretical considerations and experimental studies on kinetic isotope effects in vivo. Here, I demonstrate profound changes in life histories of the rotifer Brachionus plicatilis fed 15N-enriched algae (0.4-5.0 at%); i.e. at the enrichment levels commonly used in ecological studies. These findings support theoretically predicted effects of heavy isotope enrichment on growth, metabolism and ageing in biological systems and underline the importance of accounting for such effects when using stable isotope labelling in experimental studies.

  14. Measurements of Isotopic Composition of Vapour on the Antarctic Plateau

    Science.gov (United States)

    Casado, M.; Landais, A.; Masson-Delmotte, V.; Genthon, C.; Prie, F.; Kerstel, E.; Kassi, S.; Arnaud, L.; Steen-Larsen, H. C.; Vignon, E.

    2015-12-01

    The oldest ice core records are obtained on the East Antarctic plateau. The composition in stable isotopes of water (δ18O, δD, δ17O) permits to reconstruct the past climatic conditions over the ice sheet and also at the evaporation source. Paleothermometer accuracy relies on good knowledge of processes affecting the isotopic composition of surface snow in Polar Regions. Both simple models such as Rayleigh distillation and global atmospheric models with isotopes provide good prediction of precipitation isotopic composition in East Antarctica but post deposition processes can alter isotopic composition on site, in particular exchanges with local vapour. To quantitatively interpret the isotopic composition of water archived in ice cores, it is thus essential to study the continuum water vapour - precipitation - surface snow - buried snow. While precipitation and snow sampling are routinely performed in Antarctica, climatic conditions in Concordia, very cold (-55°C in average) and very dry (less than 1000ppmv), impose difficult conditions to measure the water vapour isotopic composition. New developments in infrared spectroscopy enable now the measurement of isotopic composition in water vapour traces (down to 20ppmv). Here we present the results of a campaign of measurement of isotopic composition in Concordia in 2014/2015. Two infrared spectrometers have been deployed or the first time on top of the East Antarctic Plateau allowing a continuous vapour measurement for a month. Comparison of the results from infrared spectroscopy with cryogenic trapping validates the relevance of the method to measure isotopic composition in dry conditions. Identification of different behaviour of isotopic composition in the water vapour associated to turbulent or stratified regime indicates a strong impact of meteorological processes in local vapour/snow interaction.

  15. Use of Stable Isotopes in Forensic Analysis of Microorganisms

    Energy Technology Data Exchange (ETDEWEB)

    Kreuzer-Martin, Helen W.; Hegg, Eric L.

    2012-01-18

    The use of isotopic signatures for forensic analysis of biological materials is well-established, and the same general principles that apply to interpretation of stable isotope content of C, N, O, and H apply to the analysis of microorganisms. Heterotrophic microorganisms derive their isotopic content from their growth substrates, which are largely plant and animal products, and the water in their culture medium. Thus the isotope signatures of microbes are tied to their growth environment. The C, N, O, and H isotope ratios of spores have been demonstrated to constitute highly discriminating signatures for sample matching. They can rule out specific samples of media and/or water as possible production media, and can predict isotope ratio ranges of the culture media and water used to produce a given sample. These applications have been developed and tested through analyses of approximately 250 samples of Bacillus subtilis spores and over 500 samples of culture media, providing a strong statistical basis for data interpretation. A Bayesian statistical framework for integrating stable isotope data with other types of signatures derived from microorganisms has been able to characterize the culture medium used to produce spores of various Bacillus species, leveraging isotopic differences in different medium types and demonstrating the power of data integration for forensic investigations.

  16. Transportation of medical isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Nielsen, D.L.

    1997-11-19

    A Draft Technical Information Document (HNF-1855) is being prepared to evaluate proposed interim tritium and medical isotope production at the Fast Flux Test Facility (FFTF). This assessment examines the potential health and safety impacts of transportation operations associated with the production of medical isotopes. Incident-free and accidental impacts are assessed using bounding source terms for the shipment of nonradiological target materials to the Hanford Site, the shipment of irradiated targets from the FFTF to the 325 Building, and the shipment of medical isotope products from the 325 Building to medical distributors. The health and safety consequences to workers and the public from the incident-free transportation of targets and isotope products would be within acceptable levels. For transportation accidents, risks to works and the public also would be within acceptable levels. This assessment is based on best information available at this time. As the medical isotope program matures, this analysis will be revised, if necessary, to support development of a final revision to the Technical Information Document.

  17. Isotope geochemistry. Biological signatures in clumped isotopes of O₂.

    Science.gov (United States)

    Yeung, Laurence Y; Ash, Jeanine L; Young, Edward D

    2015-04-24

    The abundances of molecules containing more than one rare isotope have been applied broadly to determine formation temperatures of natural materials. These applications of "clumped" isotopes rely on the assumption that isotope-exchange equilibrium is reached, or at least approached, during the formation of those materials. In a closed-system terrarium experiment, we demonstrate that biological oxygen (O2) cycling drives the clumped-isotope composition of O2 away from isotopic equilibrium. Our model of the system suggests that unique biological signatures are present in clumped isotopes of O2—and not formation temperatures. Photosynthetic O2 is depleted in (18)O(18)O and (17)O(18)O relative to a stochastic distribution of isotopes, unlike at equilibrium, where heavy-isotope pairs are enriched. Similar signatures may be widespread in nature, offering new tracers of biological and geochemical cycling. Copyright © 2015, American Association for the Advancement of Science.

  18. Influence of entrance channel on the production of hassium isotopes

    Science.gov (United States)

    Hong, Juhee; Adamian, G. G.; Antonenko, N. V.

    2015-07-01

    The production of hassium isotopes Hs-271266 in various reactions 22Ne+249Cf,Mg,2625+248Cm,30Si+244Pu,S,3634+238U,40Ar+232Th , and 48Ca+226Ra is studied within the dinuclear system model. The experimental excitation functions of the isotopes 266 -271Hs are well described and predictions are made for future experiments.

  19. Iron and nickel isotope compositions of presolar silicon carbide grains from supernovae

    Science.gov (United States)

    Kodolányi, János; Stephan, Thomas; Trappitsch, Reto; Hoppe, Peter; Pignatari, Marco; Davis, Andrew M.; Pellin, Michael J.

    2018-01-01

    We report the carbon, silicon, iron, and nickel isotope compositions of twenty-five presolar SiC grains of mostly supernova (SN) origin. The iron and nickel isotope compositions were measured with the new Chicago Instrument for Laser Ionization, CHILI, which allows the analysis of all iron and nickel isotopes without the isobaric interferences that plagued previous measurements with the NanoSIMS. Despite terrestrial iron and nickel contamination, significant isotopic anomalies in 54Fe/56Fe, 57Fe/56Fe, 60Ni/58Ni, 61Ni/58Ni, 62Ni/58Ni, and 64Ni/58Ni were detected in nine SN grains (of type X). Combined multi-isotope data of three grains with the largest nickel isotope anomalies (>100‰ or isotope ratio, when expressed as deviation from the solar value) are compared with the predictions of two SN models, one with and one without hydrogen ingestion in the He shell prior to SN explosion. One grain's carbon-silicon-iron-nickel isotope composition is consistent with the prediction of the model without hydrogen ingestion, whereas the other two grains' isotope anomalies could not be reproduced using either SN models. The discrepancies between the measured isotope compositions and model predictions may indicate element fractionation in the SN ejecta prior to or during grain condensation, and reiterate the need for three-dimensional SN models.

  20. Isotopes in Condensed Matter

    CERN Document Server

    G Plekhanov, Vladimir

    2013-01-01

    This book provides a concise introduction to the newly created sub-discipline of solid state physics isotopetronics. The role of isotopes in materials and their properties are describe  in this book. The problem of the enigma of the atomic mass in microphysics is briefly discussed.  The range of the applications of isotopes is wide: from biochemical process in living organisms to modern technical applications in quantum information. Isotopetronics promises to improve nanoelectronic and optoelectronic devices. With numerous illustrations this book is useful to researchers, engineers and graduate students.

  1. Fundamental studies on kinetic isotope effect (KIE) of hydrogen isotope fractionation in natural gas systems

    Science.gov (United States)

    Ni, Y.; Ma, Q.; Ellis, G.S.; Dai, J.; Katz, B.; Zhang, S.; Tang, Y.

    2011-01-01

    Based on quantum chemistry calculations for normal octane homolytic cracking, a kinetic hydrogen isotope fractionation model for methane, ethane, and propane formation is proposed. The activation energy differences between D-substitute and non-substituted methane, ethane, and propane are 318.6, 281.7, and 280.2cal/mol, respectively. In order to determine the effect of the entropy contribution for hydrogen isotopic substitution, a transition state for ethane bond rupture was determined based on density function theory (DFT) calculations. The kinetic isotope effect (KIE) associated with bond rupture in D and H substituted ethane results in a frequency factor ratio of 1.07. Based on the proposed mathematical model of hydrogen isotope fractionation, one can potentially quantify natural gas thermal maturity from measured hydrogen isotope values. Calculated gas maturity values determined by the proposed mathematical model using ??D values in ethane from several basins in the world are in close agreement with similar predictions based on the ??13C composition of ethane. However, gas maturity values calculated from field data of methane and propane using both hydrogen and carbon kinetic isotopic models do not agree as closely. It is possible that ??D values in methane may be affected by microbial mixing and that propane values might be more susceptible to hydrogen exchange with water or to analytical errors. Although the model used in this study is quite preliminary, the results demonstrate that kinetic isotope fractionation effects in hydrogen may be useful in quantitative models of natural gas generation, and that ??D values in ethane might be more suitable for modeling than comparable values in methane and propane. ?? 2011 Elsevier Ltd.

  2. Discoveries of isotopes by fission

    Indian Academy of Sciences (India)

    About 3000 different isotopes have been discovered until now. A recent compilation sum- marized details of the discovery of all isotopes [1–4] including the year, laboratory and country of discovery as well as the production mechanism used to produce the isotopes. Fission, one of the largest contributing production ...

  3. Kinetic 15N-isotope effects on algal growth

    Science.gov (United States)

    Andriukonis, Eivydas; Gorokhova, Elena

    2017-03-01

    Stable isotope labeling is a standard technique for tracing material transfer in molecular, ecological and biogeochemical studies. The main assumption in this approach is that the enrichment with a heavy isotope has no effect on the organism metabolism and growth, which is not consistent with current theoretical and empirical knowledge on kinetic isotope effects. Here, we demonstrate profound changes in growth dynamics of the green alga Raphidocelis subcapitata grown in 15N-enriched media. With increasing 15N concentration (0.37 to 50 at%), the lag phase increased, whereas maximal growth rate and total yield decreased; moreover, there was a negative relationship between the growth and the lag phase across the treatments. The latter suggests that a trade-off between growth rate and the ability to adapt to the high 15N environment may exist. Remarkably, the lag-phase response at 3.5 at% 15N was the shortest and deviated from the overall trend, thus providing partial support to the recently proposed Isotopic Resonance hypothesis, which predicts that certain isotopic composition is particularly favorable for living organisms. These findings confirm the occurrence of KIE in isotopically enriched algae and underline the importance of considering these effects when using stable isotope labeling in field and experimental studies.

  4. Modeled and measured stable isotope data in Siberian tree rings

    Science.gov (United States)

    Sidorova, Olga; Siegwolf, Rolf; Kupzova, Anna; Launois, Thomas; Peylin, Philippe; Spahni, Renato; Bryukhanova, Marina; Roden, John; Saurer, Matthias; Shashkin, Aleksander

    2013-04-01

    Stable isotopes in tree-rings are widely used for the reconstruction of environmental conditions, but more information could be extracted when using mechanistic models for their interpretation. Tree-ring width, cell wall structure and stable carbon as well as oxygen isotope analyses in tree wood and cellulose were carried out for four larch trees (Larix cajanderi Mayr) from northeastern Yakutia (69°N, 148°E) during the period from 1945 to 2004 and these data compared with several models. Based on a biochemical model of photosynthesis and modified model of stomatal conductance our work provides intra-annual dynamics of carbon content in photoassimilates and isotope composition in tree-rings depending on climatic factors. The mechanistic Roden-Lin-Ehleringer model was used to quantify both the physical and biochemical fractionation events associated with hydrogen and oxygen isotope ratios in tree-ring cellulose. Simulation results were compared with measured data. Predictions of carbon isotope ratios from Fritts, ORCHIDEE and LPX models were consistent with measured data. The Roden-Lin-Ehleringer oxygen model allowed the prediction of humidity and source water enrichment as well as oxygen isotope effects associated with leaf water enrichment. This work was supported by Marie Curie Fellowships (EU-ISOTREC 235122; 909122) awarded to Sidorova Olga and a grant of Russian Scientific School 5327.2012.4.

  5. Radiochemical studies of neutron deficient actinide isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Williams, K.E.

    1978-04-01

    The production of neutron deficient actinide isotopes in heavy ion reactions was studied using alpha, gamma, x-ray, and spontaneous fission detection systems. A new isotope of berkelium, /sup 242/Bk, was produced with a cross-section of approximately 10 ..mu..b in reactions of boron on uranium and nitrogen on thorium. It decays by electron capture with a half-life of 7.0 +- 1.3 minutes. The alpha-branching ratio for this isotope is less than 1% and the spontaneous fission ratio is less than 0.03%. Studies of (Heavy Ion, pxn) and (Heavy Ion, ..cap alpha..xn) transfer reactions in comparison with (Heavy ion, xn) compound nucleus reactions revealed transfer reaction cross-sections equal to or greater than the compound nucleus yields. The data show that in some cases the yield of an isotope produced via a (H.I.,pxn) or (H.I.,..cap alpha..xn) reaction may be higher than its production via an xn compound nucleus reaction. These results have dire consequences for proponents of the ''Z/sub 1/ + Z/sub 2/ = Z/sub 1+2/'' philosophy. It is no longer acceptable to assume that (H.I.,pxn) and (H.I.,..cap alpha..xn) product yields are of no consequence when studying compound nucleus reactions. No evidence for spontaneous fission decay of /sup 228/Pu, /sup 230/Pu, /sup 232/Cm, or /sup 238/Cf was observed indicating that strictly empirical extrapolations of spontaneous fission half-life data is inadequate for predictions of half-lives for unknown neutron deficient actinide isotopes.

  6. New isotopes of interest to astrophysics

    CERN Document Server

    Davids, C N; Pardo, R C; Parks, L A

    1976-01-01

    The beta decays of the new isotopes /sup 53/Ti and /sup 59/Mn have been studied. These neutron-rich isotopes have half-lives of 32.7+or-0.9 s and 4.75+or-0.14 s, respectively. They were produced via the /sup 48/Ca(/sup 7/Li, pn)/sup 53/Ti and /sup 48/Ca(/sup 13/C, pn) /sup 59/Mn reactions using beams from the Argonne National Laboratory FN Tandem Van de Graaff accelerator. Measurement of gamma singles, gamma - gamma coincidences, and beta - gamma coincidences were facilitated by a pneumatic target-transfer system ('rabbit'). Decay schemes are presented, and the measured masses compared with various predictions. The relevance to astrophysics will be discussed. In addition, a new 8-target multiple rabbit system will be described. (7 refs).

  7. NOx cycle and tropospheric ozone isotope anomaly: an experimental investigation

    Science.gov (United States)

    Michalski, G.; Bhattacharya, S. K.; Girsch, G.

    2013-04-01

    The oxygen isotope composition of nitrogen oxides (NOx) in the atmosphere may be a useful tool for understanding the oxidation of NOx into nitric acid/nitrate in the atmosphere. A set of experiments were conducted to examine changes in isotopic composition of NOx due to O3-NOx photochemical cycling. At low NO2/O2 mixing ratios, NO2 becomes progressively and nearly equally enriched in 17O and 18O over time until it reaches a steady state with Δ17O values of 40.6 ± 1.9‰ and δ18O values of 84.2 ± 4‰, relative to the isotopic composition of the O2 gas. As the mixing ratio increases, isotopic exchange between O atoms and O2 and NOx suppresses the isotopic enrichments. A kinetic model simulating the observed data shows that the isotope effects during ozone formation play a more dominant role compared to kinetic isotope effects during NO oxidation or exchange of NO2. The model results are consistent with the data when the NO + O3 reaction occurs mainly via the transfer of the terminal atom of O3. The model predicts that under tropospheric concentrations of the three reactants, the timescale of NOx isotopic equilibrium ranges from hours (ppbv mixing ratios) to days/weeks (pptv) and yields steady state Δ17O and δ18O values of 46‰ and 115‰ respectively with respect to Vienna Standard Mean Ocean Water. Interpretation of tropospheric nitrate isotope data can now be done with the derived rate coefficients of the major isotopologue reactions at various pressures.

  8. ISOTOPE METHODS IN HOMOGENEOUS CATALYSIS.

    Energy Technology Data Exchange (ETDEWEB)

    BULLOCK,R.M.; BENDER,B.R.

    2000-12-01

    The use of isotope labels has had a fundamentally important role in the determination of mechanisms of homogeneously catalyzed reactions. Mechanistic data is valuable since it can assist in the design and rational improvement of homogeneous catalysts. There are several ways to use isotopes in mechanistic chemistry. Isotopes can be introduced into controlled experiments and followed where they go or don't go; in this way, Libby, Calvin, Taube and others used isotopes to elucidate mechanistic pathways for very different, yet important chemistries. Another important isotope method is the study of kinetic isotope effects (KIEs) and equilibrium isotope effect (EIEs). Here the mere observation of where a label winds up is no longer enough - what matters is how much slower (or faster) a labeled molecule reacts than the unlabeled material. The most careti studies essentially involve the measurement of isotope fractionation between a reference ground state and the transition state. Thus kinetic isotope effects provide unique data unavailable from other methods, since information about the transition state of a reaction is obtained. Because getting an experimental glimpse of transition states is really tantamount to understanding catalysis, kinetic isotope effects are very powerful.

  9. Quantifying dispersal rates and distances in North American martens: a test of enriched isotope labeling

    Science.gov (United States)

    Jonathan N. Pauli; Winston P. Smith; Merav. Ben-David

    2012-01-01

    Advances in the application of stable isotopes have allowed the quantitative evaluation of previously cryptic ecological processes. In particular, researchers have utilized the predictable spatial patterning in natural abundance of isotopes to better understand animal dispersal and migration. However, quantifying dispersal via natural abundance alone has proven to be...

  10. Equilibrium and kinetic Si isotope fractionation factors and their implications on Si isotope distributions in the Earth's surface environments

    Science.gov (United States)

    Tang, M.; Zhang, S.; Liu, Y.

    2015-12-01

    Several important equilibrium Si isotope fractionation factors among minerals, organic molecules and the H4SiO4 solution are complemented to facilitate explanation of distributions of Si isotope in the Earth's surface environments. The results reveal that heavy Si isotopes will be significantly enriched in the secondary silicate minerals in comparison to aqueous H4SiO4. On the contrary, quadra-coordinated organosilicon complexes are enriched in light silicon isotope relative to the solution. The extent of 28Si-enrichment in hyper-coordinated organosilicon complexes is found the largest. In addition, the large kinetic isotope effect associated with the polymerization of monosilicic acid and dimer is calculated and the result supports previous statement that highly 28Si-enrichment in the formation of amorphous quartz precursor contributes to the discrepancy between theoretical calculations and field observations. With equilibrium Si isotope fractionation factors provided here, Si isotope distributions in many surface systems of the Earth can be explained. For example, the change of bulk soil δ30Si can be predicted as a concave pattern with respect to weathering degree, with the minimum value where allophane completely dissolves and the total amount of sesqui-oxides and poorly crystalline minerals reaches its maximum. When well-crystallized clays start to precipitate from pore solutions under equilibrium conditions, the bulk soil δ30Si will increase again and reach a constant value. Similarly, the precipitation of crystalline smectite and the dissolution of poorly crystalline kaolinite may explain δ30Si variations in the ground water profile. Equilibrium Si isotope fractionations among quadra-coordinated organosilicon complexes and the H4SiO4 solution may also shed the light on the Si isotope distributions in Si-accumulating plants.

  11. Therapeutic use of radioactive isotopes

    CERN Multimedia

    Caroline Duc

    2013-01-01

    In December, researchers from ISOLDE-CERN, the Paul Scherrer Institute (PSI) and the Institut Laue-Langevin (ILL) published the results of an in vivo study which successfully proved the effectiveness of four terbium isotopes for diagnosing and treating cancerous tumours.   Four terbium isotopes suitable for clinical purposes. “ISOLDE is the only installation capable of supplying terbium isotopes of such purity and intensity in the case of three out of the four types used in this study,” explains Karl Johnson, a physicist at ISOLDE.  “Producing over a thousand different isotopes, our equipment offers the widest choice of isotopes in the world!” Initially intended for fundamental physics research, ISOLDE has diversified its activities over time to invest in various projects in the materials science, biochemistry and nuclear medicine fields. The proof-of-concept study has confirmed that the four terbium isotopes 149Tb, 152Tb, 155Tb produ...

  12. Evolution of triaxial shapes at large isospin: Rh isotopes

    Directory of Open Access Journals (Sweden)

    A. Navin

    2017-04-01

    Full Text Available The rotational response as a function of neutron–proton asymmetry for the very neutron-rich isotopes of Rh (116–119Rh has been obtained from the measurement of prompt γ rays from isotopically identified fragments, produced in fission reactions at energies around the Coulomb barrier. The measured energy “signature” splitting of the yrast bands, when compared with the Triaxial Projected Shell Model (TPSM calculations, shows the need for large, nearly constant, triaxial deformations. The present results are compared with global predictions for the existence of non axial shapes in the periodic table in the case of very neutron-rich nuclei Rh isotopes. The predicted trend of a second local maximum for a triaxial shape around N∼74 is not found.

  13. The molecular mechanism of Mo isotope fractionation during adsorption to birnessite

    Science.gov (United States)

    Wasylenki, L.E.; Weeks, C.L.; Bargar, J.R.; Spiro, T.G.; Hein, J.R.; Anbar, A.D.

    2011-01-01

    Fractionation of Mo isotopes during adsorption to manganese oxides is a primary control on the global ocean Mo isotope budget. Previous attempts to explain what drives the surprisingly large isotope effect ??97/95Modissolved-??97/95Moadsorbed=1.8??? have not successfully resolved the fractionation mechanism. New evidence from extended X-ray absorption fine structure analysis and density functional theory suggests that Mo forms a polymolybdate complex on the surfaces of experimental and natural samples. Mo in this polynuclear structure is in distorted octahedral coordination, while Mo remaining in solution is predominantly in tetrahedral coordination as MoO42- Our results indicate that the difference in coordination environment between dissolved Mo and adsorbed Mo is the cause of isotope fractionation. The molecular mechanism of metal isotope fractionation in this system should enable us to explain and possibly predict metal isotope effects in other systems where transition metals adsorb to mineral surfaces. ?? 2011 Elsevier Ltd.

  14. Experimental investigation of mass-dependent and mass-independent fractionation of mercury isotopes

    Science.gov (United States)

    Bergquist, B. A.; Blum, J. D.; Marcus, J. W.; Biswas, A.

    2006-12-01

    Mercury is a globally distributed and highly toxic pollutant, the mobility and bioaccumulation of which is highly dependent on its redox cycling. With seven isotopes (including two odd-mass isotopes) and a relative mass difference of 4%, stable isotope fractionation of Hg could be a powerful tool to track and understand Hg cycling in the environment. Ongoing studies of natural mercury isotope variations in ore deposits, hydrothermal fluids, sediments, soils, fish tissues and bacterial cultures have documented a measurable range in Hg isotopes of up to ~5‰ in the ^{202}Hg/^{198}Hg ratio with most samples displaying mass-dependent fractionation. A small, but growing, body of data also suggests that natural samples display mass-independent fractionation of Hg isotopes. In this study, we explore mechanisms that lead to both mass- dependent and mass-independent fractionation of Hg isotopes. Isotope ratios were measured by continuous- flow cold-vapor generation coupled to MC-ICPMS with an external precision of ±0.1‰ (2SD). We observe three distinct types of isotope fractionation for Hg: (1) mass-dependent fractionation, (2) mass- independent fractionation of odd isotopes concurrent with mass-dependent fractionation of even isotopes, and (3) mass-independent fractionation of all Hg isotopes. Reduction of Hg species to Hg(0) vapor is an important mechanism for removal of Hg from aqueous systems into the atmosphere. Reduction of Hg occurs through numerous pathways including photoreduction, abiotic organic reduction, and biological reduction. We find that photoreduction of Hg(II) by natural sunlight leads to mass-independent fractionation of the odd isotopes (^{201}Hg, ^{199}Hg) with several permil deviations from predicted mass dependence, and mass- dependent fractionation of the even isotopes. In contrast, both biological reduction (Kritee et al., 2006) and dark abiotic organically mediated reduction follow mass-dependent fractionation of even and odd isotopes

  15. Isotopic characteristics of canopies in simulated leaf assemblages

    Science.gov (United States)

    Graham, Heather V.; Patzkowsky, Mark E.; Wing, Scott L.; Parker, Geoffrey G.; Fogel, Marilyn L.; Freeman, Katherine H.

    2014-11-01

    site where leaves were sampled. The model predicts a persistent ∼1‰ difference in δ13Clitter for the two sites which is consistent with higher water availability in the tropical forests. This work provides a new framework for linking contemporary ecological observations to the geochemical record using flux-weighted isotope data and lends insights to the effect of forest architecture on organic and isotopic records of ancient terrestrial ecosystems. How many leaves from a litter assemblage are necessary to distinguish the isotopic gradient characteristics of canopy closure? Are mean δ13Cleaf values for a litter assemblage diagnostic of a forest biome? Can we predict the δ13C values of cumulative litter, soil organic matter, and organic carbon in sedimentary archives using litter flux and isotope patterns in canopies? We determined the δ13C range and mean for different sized assemblages of leaves sampled from data for each forest. We re-sampled very high numbers of leaves in order to estimate the isotopic composition of cumulative carbon delivered to soils as litter, and compared these results to available data from forest soils. Modeled leaf and soil organic carbon isotope patterns in this study offer insights to how forest structure can be derived from carbon isotope measurements of fossil leaves, as well as secondary material - such as teeth, hair, paleosol carbonates, or organic soil carbon (van der Merwe and Medina, 1989; Koch, 1998; Secord et al., 2008; Levin et al., 2011).Distinct climate and seasonal difference in the Panamá and Maryland, USA forests are reflected in their canopy isotope gradients. In the tropical forest of Panamá, leaves are produced throughout the year within a canopy that is both extensively and persistently closed (Leigh, 1975; Lowman and Wittman, 1996). In the temperate forest of Maryland leaves are produced during the spring when canopy conditions are relatively open (Korner and Basler, 2010).

  16. Chromatographic hydrogen isotope separation

    Science.gov (United States)

    Aldridge, Frederick T.

    1981-01-01

    Intermetallic compounds with the CaCu.sub.5 type of crystal structure, particularly LaNiCo.sub.4 and CaNi.sub.5, exhibit high separation factors and fast equilibrium times and therefore are useful for packing a chromatographic hydrogen isotope separation colum. The addition of an inert metal to dilute the hydride improves performance of the column. A large scale mutli-stage chromatographic separation process run as a secondary process off a hydrogen feedstream from an industrial plant which uses large volumes of hydrogen can produce large quantities of heavy water at an effective cost for use in heavy water reactors.

  17. Cold regions isotope applications

    Energy Technology Data Exchange (ETDEWEB)

    Perrigo, L.D.; Divine, T.E.

    1976-04-01

    Pacific Northwest Laboratories (PNL) started the Cold Regions Isotope Applications Program in FY-1975 to identify special conditions in the Arctic and similar geographic areas (Cold Regions) where radioisotope power, heater, or sterilization systems would be desirable and economically viable. Significant progress was made in the first year of this program and all objectives for this initial 12-month period were achieved. The major conclusions and recommendations resulting for this effort are described below. The areas of interest covered include: radiosterilization of sewage; heating of septic tanks; and radioisotope thermoelectric generators as power sources for meteorological instruments and navigational aids. (TFD)

  18. ISOTOPE FRACTIONATION PROCESS

    Science.gov (United States)

    Clewett, G.H.; Lee, DeW.A.

    1958-05-20

    A new method is described for isotopic enrichment of uranium. It has been found that when an aqueous acidic solution of ionic tetravalent uraniunn is contacted with chelate complexed tetravalent uranium, the U/sup 238/ preferentially concentrates in the complexed phase while U/sup 235/ concentrates in the ionic phase. The effect is enhanced when the chelate compound is water insoluble and is dissolved in a water-immiscible organic solvent. Cupferron is one of a number of sultable complexing agents, and chloroform is a suitable organic solvent.

  19. Cluster emission in superdeformed Sr isotopes in the ground state ...

    Indian Academy of Sciences (India)

    2017-01-03

    Jan 3, 2017 ... Abstract. Cluster decay of superdeformed 76,78,80Sr isotopes in their ground state are studied taking the Coulomb and proximity potential as the interacting barrier for the post-scission region. The predicted T1/2 values are found to be in close agreement with those values reported by the preformed cluster ...

  20. Relationships between tree height and carbon isotope discrimination

    Science.gov (United States)

    Nate G. McDowell; Barbara J. Bond; Lee T. Dickman; Michael G. Ryan; David Whitehead

    2011-01-01

    Understanding how tree size impacts leaf- and crown-level gas exchange is essential to predicting forest yields and carbon and water budgets. The stable carbon isotope ratio of organic matter has been used to examine the relationship of gas exchange to tree size for a host of species because it carries a temporally integrated signature of foliar photosynthesis and...

  1. Zinc isotope fractionation during adsorption on calcite

    Science.gov (United States)

    Dong, S.; Wasylenki, L. E.

    2013-12-01

    difference in coordination number between dissolved Zn and adsorbed Zn is drives the observed fractionation. Elzinga and Reeder[5] determined using EXAFS (Extended X-ray Absorption Fine Structure) that Zn adsorbed to calcite surfaces is tetrahedrally coordinated, sharing three oxygens with the calcite surface. Meanwhile density functional theory calculations[6] predicted that tetrahedral Zn-O species should be heavier than octahedral Zn-O species. Thus we infer that equilibrium between octahedrally coordinated, dissolved Zn and tetrahedrally coordinated, adsorbed Zn is the mechanism of fractionation in our experiments. Our further studies will determine whether the isotopically heavy pool of adsorbed Zn becomes the Zn incorporated within carbonates; if so, then we are closer to understanding the mechanism by which carbonate rocks in nature are enriched in heavier isotopes of zinc. [1] Bermin et al., 2006, Chem. Geol. 226, 280. [2] Maréchal et al., 2000, Geochem. Geophys. Geosyst. 1, 1999GC-000029. [3] Dong et al., 2013, Talanta 114, 103-109. [4] Pichat et al., 2003, Earth Planet. Sci. Lett. 210, 167-178. [5] Elzinga and Reeder, 2002, Geochim. Cosmochim. Acta 66, 3943-3954. [6] Schauble, 2003, EOS, Trans. AGU, Fall Meet. Suppl. 84(46), B12B-0781.

  2. Uranium Isotope Systematic in Saanich Inlet

    Science.gov (United States)

    Amini, M.; Holmden, C.; Francois, R.

    2008-12-01

    As a redox-sensitive element Uranium has become the focus of stable isotope studies. Based on the nuclear field shift effect [1], U isotope fractionation was predicted as a function of U(IV)-U(VI) exchange reactions with the insoluble reduced U(IV) species being heavier than the soluble oxidized U(VI) species. Recently, variations in 238U/235U were reported in low temperature aqueous and sedimentary environments [2,3] indicating that U deposited in well-oxygenated environments is characterized by light isotopic composition, whereas suboxic and anoxic deposits tend towards a heavy isotopic signature. U isotope fractionation has been hence proposed as a promising new paleo-redox proxy. In order to test the efficacy of U isotope fractionation to record oxidation states in marine systems, we are investigating sediment samples deposited over a range of redox conditions in the seasonally anoxic Saanich Inlet, on the east coast of Vancouver Island. We have also made δ238U measurements for water samples from above and below the redoxcline. The measurements were carried out by MC-ICPMS using 233U/236U-double spike technique. The data are reported as δ238U relative to NBL 112a with a 238U/235U ratio of 137.88 (2sd). External precision is better than 0.10 permil (2sd). Eleven analyses of seawater performed over the course of this work yielded δ238U of -0.41±0.07 permil (2sd). No clear difference in δ238U values has been found, thus far, in water samples collected at 10m (O2~380μM) and 200m (O2~1μM) depths from a single location in the middle of the inlet. The mean of two measurements of the deepwater sample yielded -0.43±0.01 permil (2sd). Two measurements of the shallow water sample yielded a mean value of -0.38±0.03 permil (2sd). The δ238U values for HF-HNO3 digestions of the organic rich sediments, one taken in the middle of the basin (3.11% organic carbon) below seasonally anoxic bottom waters (-0.22±0.01 permil, n=2), and the other taken from the sill (1

  3. Isotopic Dependence of the Nuclear Caloric Curve

    Science.gov (United States)

    Sfienti, C.; Adrich, P.; Aumann, T.; Bacri, C. O.; Barczyk, T.; Bassini, R.; Bianchin, S.; Boiano, C.; Botvina, A. S.; Boudard, A.; Brzychczyk, J.; Chbihi, A.; Cibor, J.; Czech, B.; de Napoli, M.; Ducret, J.-É.; Emling, H.; Frankland, J. D.; Hellström, M.; Henzlova, D.; Immè, G.; Iori, I.; Johansson, H.; Kezzar, K.; Lafriakh, A.; Le Fèvre, A.; Le Gentil, E.; Leifels, Y.; Lühning, J.; Łukasik, J.; Lynch, W. G.; Lynen, U.; Majka, Z.; Mocko, M.; Müller, W. F. J.; Mykulyak, A.; Orth, H.; Otte, A. N.; Palit, R.; Pawłowski, P.; Pullia, A.; Raciti, G.; Rapisarda, E.; Sann, H.; Schwarz, C.; Simon, H.; Sümmerer, K.; Trautmann, W.; Tsang, M. B.; Verde, G.; Volant, C.; Wallace, M.; Weick, H.; Wiechula, J.; Wieloch, A.; Zwiegliński, B.

    2009-04-01

    The A/Z dependence of projectile fragmentation at relativistic energies has been studied with the ALADIN forward spectrometer at SIS. A stable beam of Sn124 and radioactive beams of La124 and Sn107 at 600 MeV per nucleon have been used in order to explore a wide range of isotopic compositions. Chemical freeze-out temperatures are found to be nearly invariant with respect to the A/Z of the produced spectator sources, consistent with predictions for expanded systems. Small Coulomb effects (ΔT≈0.6MeV) appear for residue production near the onset of multifragmentation.

  4. Isotopic incorporation rates and discrimination factors in mantis shrimp crustaceans.

    Directory of Open Access Journals (Sweden)

    Maya S deVries

    Full Text Available Stable isotope analysis has provided insights into the trophic ecology of a wide diversity of animals. Knowledge about isotopic incorporation rates and isotopic discrimination between the consumer and its diet for different tissue types is essential for interpreting stable isotope data, but these parameters remain understudied in many animal taxa and particularly in aquatic invertebrates. We performed a 292-day diet shift experiment on 92 individuals of the predatory mantis shrimp, Neogonodactylus bredini, to quantify carbon and nitrogen incorporation rates and isotope discrimination factors in muscle and hemolymph tissues. Average isotopic discrimination factors between mantis shrimp muscle and the new diet were 3.0 ± 0.6 ‰ and 0.9 ± 0.3 ‰ for carbon and nitrogen, respectively, which is contrary to what is seen in many other animals (e.g. C and N discrimination is generally 0-1 ‰ and 3-4 ‰, respectively. Surprisingly, the average residence time of nitrogen in hemolymph (28.9 ± 8.3 days was over 8 times longer than that of carbon (3.4 ± 1.4 days. In muscle, the average residence times of carbon and nitrogen were of the same magnitude (89.3 ± 44.4 and 72.8 ± 18.8 days, respectively. We compared the mantis shrimps' incorporation rates, along with rates from four other invertebrate taxa from the literature, to those predicted by an allometric equation relating carbon incorporation rate to body mass that was developed for teleost fishes and sharks. The rate of carbon incorporation into muscle was consistent with rates predicted by this equation. Our findings provide new insight into isotopic discrimination factors and incorporation rates in invertebrates with the former showing a different trend than what is commonly observed in other animals.

  5. Possibilities of synthesis of unknown isotopes of superheavy nuclei with charge numbers Z > 108 in asymmetric actinide-based complete fusion reactions

    Energy Technology Data Exchange (ETDEWEB)

    Hong, Juhee [Institute for Basic Science, Rare Isotope Science Project, Daejeon (Korea, Republic of); Adamian, G.G. [Joint Institute for Nuclear Research, Dubna (Russian Federation); Antonenko, N.V. [Joint Institute for Nuclear Research, Dubna (Russian Federation); Tomsk Polytechnic University, Mathematical Physics Department, Tomsk (Russian Federation)

    2016-10-15

    The possibilities of production of new isotopes of superheavy nuclei with charge numbers Z = 109-114 in various asymmetric hot fusion reactions are studied for the first time. The excitation functions of the formation of these isotopes in the xn evaporation channels are predicted and the optimal conditions for the synthesis are proposed. The products of the suggested reactions can fill a gap of unknown isotopes between the isotopes of the heaviest nuclei obtained in cold and hot complete fusion reactions. (orig.)

  6. Chlorine Isotope Ratios in M Giants and S Stars

    Science.gov (United States)

    Maas, Zachary; Pilachowski, C. A.

    2018-01-01

    Chlorine is an odd-Z, light element that has been poorly studied in stars. Recently, the first stellar abundance measurements of the isotopologue 35Cl were made and the 35Cl/37Cl ratio was derived in RZ Ari (Maas et al. 2016). Additional abundance measurements are necessary to understand the Galactic chemical evolution and complex nucleosynthesis of Cl. The Cl isotope ratio in particular is important in distinguishing contributions from different nucleosynthesis sites to the surface abundances of stars. For example, current nucloesynthesis models predict that both isotopes of Cl are produced primarily during core collapse supernovae (CCSNe) with the energy and progenitor mass impacting the isotopic ratio of the ejected material. In addition to CCSNe, 37Cl is formed by the s-process both in massive stars and in AGB stars, and 35Cl may be produced from neutrino spallation. Understanding the formation of the Cl isotopes is also important to studies of the interstellar medium (ISM). A range of Cl isotope ratios mainly between 2 - 3.5 have been measured in star forming regions, in the circumstellar envelopes of evolved stars, and in proto-stellar cores using Cl bearing molecules. Additional measurements of the Cl isotope ratio in nearby stars will test nucleosynthesis models and allow comparisons with the range of isotope ratios observed in the ISM.We build on the results of Maas et al. (2016) by measuring the Cl isotope ratio in six M giants and four S stars using R~50,000 resolution spectra from Phoenix on Gemini South. We find no significant difference between the average Cl isotope ratios in the M stars and S stars and our measurements are consistent with the range of values seen in the ISM. We also find the average Cl ratio to be larger than the predicted isotope ratio of 1.8 for the solar neighborhood. Finally, two S stars, GG Pup and WY Pyx, show anomalously strong HCl features with equivalent widths ~3-5 times larger than the HCl features of other stars of

  7. Method of separating boron isotopes

    Science.gov (United States)

    Jensen, Reed J.; Thorne, James M.; Cluff, Coran L.; Hayes, John K.

    1984-01-01

    A method of boron isotope enrichment involving the isotope preferential photolysis of (2-chloroethenyl)dichloroborane as the feed material. The photolysis can readily be achieved with CO.sub.2 laser radiation and using fluences significantly below those required to dissociate BCl.sub.3.

  8. Chromium isotope uptake in carbonates

    DEFF Research Database (Denmark)

    Rodler, Alexandra

    retain an isotopically light Cr signature. Cr(VI) enriched in heavy Cr isotopes is then transported via river waters to the oceans and sequestered into marine sediments. Marine chemical sediments such asbanded iron formations and modern marine carbonates have proven useful in recording the Cr isotope...... with calcium carbonate in order to test the reliability of the Cr carbonate compositions. Several experimental approaches have been employed to elucidate the fractionation behavior of Cr isotopes when Cr(VI) is incorporated into calcium carbonate phases. These results indicate that at lower Cr concentrations......Chromium (Cr) is a redox sensitive element potentially capable of tracing fine-scale fluctuations of the oxygenation of Earth’s early surface environments and seawater. The Cr isotope composition of carbonates could perhaps be used as paleo-redox proxy to elucidate changes in the geological past...

  9. Hydrogen and oxygen isotope ratios in human hair are related to geography.

    Science.gov (United States)

    Ehleringer, James R; Bowen, Gabriel J; Chesson, Lesley A; West, Adam G; Podlesak, David W; Cerling, Thure E

    2008-02-26

    We develop and test a model to predict the geographic region-of-origin of humans based on the stable isotope composition of their scalp hair. This model incorporates exchangeable and nonexchangeable hydrogen and oxygen atoms in amino acids to predict the delta(2)H and delta(18)O values of scalp hair (primarily keratin). We evaluated model predictions with stable isotope analyses of human hair from 65 cities across the United States. The model, which predicts hair isotopic composition as a function of drinking water, bulk diet, and dietary protein isotope ratios, explains >85% of the observed variation and reproduces the observed slopes relating the isotopic composition of hair samples to that of local drinking water. Based on the geographical distributions of the isotope ratios of tap waters and the assumption of a "continental supermarket" dietary input, we constructed maps of the expected average H and O isotope ratios in human hair across the contiguous 48 states. Applications of this model and these observations are extensive and include detection of dietary information, reconstruction of historic movements of individuals, and provision of region-of-origin information for unidentified human remains.

  10. Diffusion of multi-isotopic chemical species in molten silicates

    Science.gov (United States)

    Watkins, James M.; Liang, Yan; Richter, Frank; Ryerson, Frederick J.; DePaolo, Donald J.

    2014-08-01

    Diffusion experiments in a simplified Na2O-CaO-SiO2 liquid system are used to develop a general formulation for the fractionation of Ca isotopes during liquid-phase diffusion. Although chemical diffusion is a well-studied process, the mathematical description of the effects of diffusion on the separate isotopes of a chemical element is surprisingly underdeveloped and uncertain. Kinetic theory predicts a mass dependence on isotopic mobility, but it is unknown how this translates into a mass dependence on effective binary diffusion coefficients, or more generally, the chemical diffusion coefficients that are housed in a multicomponent diffusion matrix. Our experiments are designed to measure Ca mobility, effective binary diffusion coefficients, the multicomponent diffusion matrix, and the effects of chemical diffusion on Ca isotopes in a liquid of single composition. We carried out two chemical diffusion experiments and one self-diffusion experiment, all at 1250 °C and 0.7 GPa and using a bulk composition for which other information is available from the literature. The self-diffusion experiment is used to determine the mobility of Ca in the absence of diffusive fluxes of other liquid components. The chemical diffusion experiments are designed to determine the effect on Ca isotope fractionation of changing the counter-diffusing component from fast-diffusing Na2O to slow-diffusing SiO2. When Na2O is the main counter-diffusing species, CaO diffusion is fast and larger Ca isotopic effects are generated. When SiO2 is the main counter-diffusing species, CaO diffusion is slow and smaller Ca isotopic effects are observed. In both experiments, the liquid is initially isotopically homogeneous, and during the experiment Ca isotopes become fractionated by diffusion. The results are used as a test of a new general expression for the diffusion of isotopes in a multicomponent liquid system that accounts for both self diffusion and the effects of counter-diffusing species. Our

  11. Collinear Resonance Ionization Spectroscopy of Neutron-Deficient Francium Isotopes

    CERN Document Server

    Flanagan, K T; Ruiz, R F Garcia; Budincevic, I; Procter, T J; Fedosseev, V N; Lynch, K M; Cocolios, T E; Marsh, B A; Neyens, G; Strashnov, I; Stroke, H H; Rossel, R E; Heylen, H; Billowes, J; Rothe, S; Bissell, M L; Wendt, K D A; de Groote, R P; De Schepper, S

    2013-01-01

    The magnetic moments and isotope shifts of the neutron-deficient francium isotopes Fr202-205 were measured at ISOLDE-CERN with use of collinear resonance ionization spectroscopy. A production-to-detection efficiency of 1\\% was measured for Fr-202. The background from nonresonant and collisional ionization was maintained below one ion in 10(5) beam particles. Through a comparison of the measured charge radii with predictions from the spherical droplet model, it is concluded that the ground-state wave function remains spherical down to Fr-205, with a departure observed in Fr-203 (N = 116).

  12. Collinear Resonance Ionization Spectroscopy of Neutron-Deficient Francium Isotopes

    Science.gov (United States)

    Flanagan, K. T.; Lynch, K. M.; Billowes, J.; Bissell, M. L.; Budinčević, I.; Cocolios, T. E.; de Groote, R. P.; De Schepper, S.; Fedosseev, V. N.; Franchoo, S.; Garcia Ruiz, R. F.; Heylen, H.; Marsh, B. A.; Neyens, G.; Procter, T. J.; Rossel, R. E.; Rothe, S.; Strashnov, I.; Stroke, H. H.; Wendt, K. D. A.

    2013-11-01

    The magnetic moments and isotope shifts of the neutron-deficient francium isotopes Fr202-205 were measured at ISOLDE-CERN with use of collinear resonance ionization spectroscopy. A production-to-detection efficiency of 1% was measured for Fr202. The background from nonresonant and collisional ionization was maintained below one ion in 105 beam particles. Through a comparison of the measured charge radii with predictions from the spherical droplet model, it is concluded that the ground-state wave function remains spherical down to Fr205, with a departure observed in Fr203 (N=116).

  13. Phase Transitions in Even-Even Palladium Isotopes

    Directory of Open Access Journals (Sweden)

    Diab S. M.

    2009-01-01

    Full Text Available The positive and negative parity states of the even-even palladium isotopes were stud- ied within the frame work of the interacting boson approximation model (IBA-1. The energy spectra, potential energy surfaces, electromagnetic transition probabilities, back bending and staggering effect have been calculated. The potential energy surfaces show smooth transition from vibrational-like to gamma-soft and finally to rotational-like nu- clei. Staggering effectle, has been observed between the positive and negative parity states in palladium isotopes. The agreement between theoretical predictions and exper- imental values are fairly good.

  14. Competition from Isotopic Modelling

    Directory of Open Access Journals (Sweden)

    Virginie Fabre

    2011-01-01

    Full Text Available During later MOIS3, in Europe two populations were present, autochthonous Neanderthals and modern humans. Ecological competition between these two populations has often been evoked but never demonstrated. Our aim is to establish whether resource competition occurred. In this paper, in order to examine the possibility of ecological competition between these two populations, 599 isotopic data were subjected to rigorous statistical treatment and analysis through mixing models. The aim of this paper was to compare dietary strategies of Neanderthals and modern humans over time. Our conclusions suggest that Neanderthals and modern humans shared dietary habits in the particular environmental context of MOIS3 characterised in Europe by climatic deterioration. In this environmental context, the resource competition between Neanderthals and modern humans may have accelerated the disappearance of the Neanderthal population.

  15. Compelling Research Opportunities using Isotopes

    Energy Technology Data Exchange (ETDEWEB)

    None

    2009-04-23

    Isotopes are vital to the science and technology base of the US economy. Isotopes, both stable and radioactive, are essential tools in the growing science, technology, engineering, and health enterprises of the 21st century. The scientific discoveries and associated advances made as a result of the availability of isotopes today span widely from medicine to biology, physics, chemistry, and a broad range of applications in environmental and material sciences. Isotope issues have become crucial aspects of homeland security. Isotopes are utilized in new resource development, in energy from bio-fuels, petrochemical and nuclear fuels, in drug discovery, health care therapies and diagnostics, in nutrition, in agriculture, and in many other areas. The development and production of isotope products unavailable or difficult to get commercially have been most recently the responsibility of the Department of Energy's Nuclear Energy program. The President's FY09 Budget request proposed the transfer of the Isotope Production program to the Department of Energy's Office of Science in Nuclear Physics and to rename it the National Isotope Production and Application program (NIPA). The transfer has now taken place with the signing of the 2009 appropriations bill. In preparation for this, the Nuclear Science Advisory Committee (NSAC) was requested to establish a standing subcommittee, the NSAC Isotope Subcommittee (NSACI), to advise the DOE Office of Nuclear Physics. The request came in the form of two charges: one, on setting research priorities in the short term for the most compelling opportunities from the vast array of disciplines that develop and use isotopes and two, on making a long term strategic plan for the NIPA program. This is the final report to address charge 1. NSACI membership is comprised of experts from the diverse research communities, industry, production, and homeland security. NSACI discussed research opportunities divided into three areas: (1

  16. Gallium isotope fractionation during Ga adsorption on calcite and goethite

    Science.gov (United States)

    Yuan, Wei; Saldi, Giuseppe D.; Chen, JiuBin; Vetuschi Zuccolini, Marino; Birck, Jean-Louis; Liu, Yujie; Schott, Jacques

    2018-02-01

    Gallium (Ga) isotopic fractionation during its adsorption on calcite and goethite was investigated at 20 °C as a function of the solution pH, Ga aqueous concentration and speciation, and the solid to solution ratio. In all experiments Ga was found to be enriched in light isotopes at the solid surface with isotope fractionation △71Gasolid-solution up to -1.27‰ and -0.89‰ for calcite and goethite, respectively. Comparison of Ga isotopic data of this study with predictions for 'closed system' equilibrium and 'Rayleigh fractionation' models indicates that the experimental data are consistent with a 'closed system' equilibrium exchange between the fluid and the solid. The results of this study can be interpreted based on Ga aqueous speciation and the structure of Ga complexes formed at the solid surfaces. For calcite, Ga isotope fractionation is mainly triggered by increased Ga coordination and Ga-O bond length, which vary respectively from 4 and 1.84 Å in Ga(OH)4- to 6 and 1.94 Å in the >Ca-O-GaOH(OH2)4+ surface complex. For goethite, despite the formation of Ga hexa-coordinated >FeOGa(OH)20 surface complexes (Ga-O distances of 1.96-1.98 Å) both at acid and alkaline pH, a similar extent of isotope fractionation was found at acid and alkaline pH, suggesting that Ga(OH)4- is preferentially adsorbed on goethite for all investigated pH conditions. In addition, the observed decrease of Ga isotope fractionation magnitude observed with increasing Ga surface coverage for both calcite and goethite is likely related to the formation of Ga surface polymers and/or hydroxides with reduced Ga-O distances. This first study of Ga isotope fractionation during solid-fluid interactions suggests that the adsorption of Ga by oxides, carbonates or clay minerals could yield significant Ga isotope fractionation between secondary minerals and surficial fluids including seawater. Ga isotopes thus should help to better characterize the surficial biogeochemical cycles of gallium and its

  17. Zinc isotopic evidence for the origin of the Moon.

    Science.gov (United States)

    Paniello, Randal C; Day, James M D; Moynier, Frédéric

    2012-10-18

    Volatile elements have a fundamental role in the evolution of planets. But how budgets of volatiles were set in planets, and the nature and extent of volatile-depletion of planetary bodies during the earliest stages of Solar System formation remain poorly understood. The Moon is considered to be volatile-depleted and so it has been predicted that volatile loss should have fractionated stable isotopes of moderately volatile elements. One such element, zinc, exhibits strong isotopic fractionation during volatilization in planetary rocks, but is hardly fractionated during terrestrial igneous processes, making it a powerful tracer of the volatile histories of planets. Here we present high-precision zinc isotopic and abundance data which show that lunar magmatic rocks are enriched in the heavy isotopes of zinc and have lower zinc concentrations than terrestrial or Martian igneous rocks. Conversely, Earth and Mars have broadly chondritic zinc isotopic compositions. We show that these variations represent large-scale evaporation of zinc, most probably in the aftermath of the Moon-forming event, rather than small-scale evaporation processes during volcanism. Our results therefore represent evidence for volatile depletion of the Moon through evaporation, and are consistent with a giant impact origin for the Earth and Moon.

  18. Stable Isotope Systematics of Coalbed Gas during Desorption and Production

    Directory of Open Access Journals (Sweden)

    Martin Niemann

    2017-06-01

    Full Text Available The stable carbon isotope ratios of coalbed methane (CBM demonstrate diagnostic changes that systematically vary with production and desorption times. These shifts can provide decisive, predictive information on the behaviour and potential performance of CBM operations. Samples from producing CBM wells show a general depletion in 13C-methane with increasing production times and corresponding shifts in δ13C-CH4 up to 35.8‰. Samples from canister desorption experiments show mostly enrichment in 13C for methane with increasing desorption time and isotope shifts of up to 43.4‰. Also, 13C-depletion was observed in some samples with isotope shifts of up to 32.1‰. Overall, the magnitudes of the observed isotope shifts vary considerably between different sample sets, but also within samples from the same source. The δ13C-CH4 values do not have the anticipated signature of methane generated from coal. This indicates that secondary processes, including desorption and diffusion, can influence the values. It is also challenging to deconvolute these various secondary processes because their molecular and isotope effects can have similar directions and/or magnitudes. In some instances, significant alteration of CBM gases has to be considered as a combination of secondary alteration effects.

  19. Isotope composition and volume of Earth's early oceans.

    Science.gov (United States)

    Pope, Emily C; Bird, Dennis K; Rosing, Minik T

    2012-03-20

    Oxygen and hydrogen isotope compositions of Earth's seawater are controlled by volatile fluxes among mantle, lithospheric (oceanic and continental crust), and atmospheric reservoirs. Throughout geologic time the oxygen mass budget was likely conserved within these Earth system reservoirs, but hydrogen's was not, as it can escape to space. Isotopic properties of serpentine from the approximately 3.8 Ga Isua Supracrustal Belt in West Greenland are used to characterize hydrogen and oxygen isotope compositions of ancient seawater. Archaean oceans were depleted in deuterium [expressed as δD relative to Vienna standard mean ocean water (VSMOW)] by at most 25 ± 5‰, but oxygen isotope ratios were comparable to modern oceans. Mass balance of the global hydrogen budget constrains the contribution of continental growth and planetary hydrogen loss to the secular evolution of hydrogen isotope ratios in Earth's oceans. Our calculations predict that the oceans of early Earth were up to 26% more voluminous, and atmospheric CH(4) and CO(2) concentrations determined from limits on hydrogen escape to space are consistent with clement conditions on Archaean Earth.

  20. Isotope-based quantum information

    CERN Document Server

    G Plekhanov, Vladimir

    2012-01-01

    The present book provides to the main ideas and techniques of the rapid progressing field of quantum information and quantum computation using isotope - mixed materials. It starts with an introduction to the isotope physics and then describes of the isotope - based quantum information and quantum computation. The ability to manipulate and control electron and/or nucleus spin in semiconductor devices provides a new route to expand the capabilities of inorganic semiconductor-based electronics and to design innovative devices with potential application in quantum computing. One of the major challenges towards these objectives is to develop semiconductor-based systems and architectures in which the spatial distribution of spins and their properties can be controlled. For instance, to eliminate electron spin decoherence resulting from hyperfine interaction due to nuclear spin background, isotopically controlled devices are needed (i.e., nuclear spin-depleted). In other emerging concepts, the control of the spatial...

  1. Isotope Geochronology: Models Versus Reality

    National Research Council Canada - National Science Library

    Jan Burchart

    2015-01-01

    Majority of the papers on isotopic dating of minerals and rocks have been devoted to some new geochronological data important for geology or to developments of apparatus and improvements of laboratory...

  2. Analysis of the site-specific carbon isotope composition of propane by gas source isotope ratio mass spectrometer

    Science.gov (United States)

    Piasecki, Alison; Sessions, Alex; Lawson, Michael; Ferreira, A. A.; Neto, E. V. Santos; Eiler, John M.

    2016-09-01

    Site-specific isotope ratio measurements potentially provide valuable information about the formation and degradation of complex molecules-information that is lost in conventional bulk isotopic measurements. Here we discuss the background and possible applications of such measurements, and present a technique for studying the site-specific carbon isotope composition of propane at natural abundance based on mass spectrometric analysis of the intact propane molecule and its fragment ions. We demonstrate the feasibility of this approach through measurements of mixtures of natural propane and propane synthesized with site-specific 13C enrichment, and we document the limits of precision of our technique. We show that mass balance calculations of the bulk δ13C of propane based on our site-specific measurements is generally consistent with independent constraints on bulk δ13C. We further demonstrate the accuracy of the technique, and illustrate one of its simpler applications by documenting the site-specific carbon isotope signature associated with gas phase diffusion of propane, confirming that our measurements conform to the predictions of the kinetic theory of gases. This method can be applied to propane samples of moderate size (tens of micromoles) isolated from natural gases. Thus, it provides a means of studying the site-specific stable isotope systematics of propane at natural isotope abundances on sample sizes that are readily recovered from many natural environments. This method may also serve as a model for future techniques that apply high-resolution mass spectrometry to study the site-specific isotopic distributions of larger organic molecules, with potential applications to biosynthesis, forensics and other geochemical subjects.

  3. Stable Chlorine Isotope Fractionation

    Science.gov (United States)

    Sharp, Z.

    2006-12-01

    Chlorine isotope partitioning between different phases is not well understood. Pore fluids can have δ37Cl values as low as -8‰, with neoform sediments having strongly positive values. Most strikingly, volcanic gases have δ37Cl values that cover a range in excess of 14‰ (Barnes et al., this meeting). The large range is difficult to explain in terms of equilibrium fractionation, which, although calculated to be very large for Cl in different oxidation states, should be less than 2‰ between chloride species (Schauble et al., 2003, GCA). To address the discrepancy between Nature and theory, we have measured Cl isotope fractionation for selected equilibrium and disequilibrium experiments in order to identify mechanisms that might lead to large fractionations. 1) NaCl (s,l) NaCl (v): NaCl was sealed in an evacuated silica tube and heated at one end, causing vaporization and reprecipitation of NaCl (v) at the cool end of the tube. The fractionation is 0.2‰ at 700°C (halite-vapor) and 0.7‰ at 800°C (liquid-vapor), respectively. The larger fractionation at higher temperature may be related to equilibrium fractionation between liquid and gas vs. `stripping' of the solid in the lower T experiments. 2) Sodalite NaCl(l): Nepheline and excess NaCl were sealed in a Pt crucible at 825°C for 48 hrs producing sodalite. The measured newly-formed sodalite-NaCl fractionation is -0.2‰. 3) Volatilization of HCl: Dry inert gas was bubbled through HCl solutions and the vapor was collected in a downstream water trap. There was no fractionation for 12.4M HCl (HCl fuming) vapor at 25°C. For a 1 M boiling HCl solution, the HCl-vapor fractionation was ~9‰. The difference is probably related to the degree of dissociation in the acid, with HCl dissolved in water for the highly acidic solutions, and dissociated H3O+ and Cl- for lower concentrations. The HCl volatilization experiments are in contrast to earlier vapor-liquid experiments in NaCl-H2O system, where fractionation was

  4. Electron linac for medical isotope production with improved energy efficiency and isotope recovery

    Science.gov (United States)

    Noonan, John; Walters, Dean; Virgo, Matt; Lewellen, John

    2015-09-08

    A method and isotope linac system are provided for producing radio-isotopes and for recovering isotopes. The isotope linac is an energy recovery linac (ERL) with an electron beam being transmitted through an isotope-producing target. The electron beam energy is recollected and re-injected into an accelerating structure. The ERL provides improved efficiency with reduced power requirements and provides improved thermal management of an isotope target and an electron-to-x-ray converter.

  5. A Stochastic Method for Estimating the Effect of Isotopic Uncertainties in Spent Nuclear Fuel

    Energy Technology Data Exchange (ETDEWEB)

    DeHart, M.D.

    2001-08-24

    This report describes a novel approach developed at the Oak Ridge National Laboratory (ORNL) for the estimation of the uncertainty in the prediction of the neutron multiplication factor for spent nuclear fuel. This technique focuses on burnup credit, where credit is taken in criticality safety analysis for the reduced reactivity of fuel irradiated in and discharged from a reactor. Validation methods for burnup credit have attempted to separate the uncertainty associated with isotopic prediction methods from that of criticality eigenvalue calculations. Biases and uncertainties obtained in each step are combined additively. This approach, while conservative, can be excessive because of a physical assumptions employed. This report describes a statistical approach based on Monte Carlo sampling to directly estimate the total uncertainty in eigenvalue calculations resulting from uncertainties in isotopic predictions. The results can also be used to demonstrate the relative conservatism and statistical confidence associated with the method of additively combining uncertainties. This report does not make definitive conclusions on the magnitude of biases and uncertainties associated with isotopic predictions in a burnup credit analysis. These terms will vary depending on system design and the set of isotopic measurements used as a basis for estimating isotopic variances. Instead, the report describes a method that can be applied with a given design and set of isotopic data for estimating design-specific biases and uncertainties.

  6. Prospects for improved understanding of isotopic reactor antineutrino fluxes

    Science.gov (United States)

    Gebre, Y.; Littlejohn, B. R.; Surukuchi, P. T.

    2018-01-01

    Predictions of antineutrino fluxes produced by fission isotopes in a nuclear reactor have recently received increased scrutiny due to observed differences in predicted and measured inverse beta decay (IBD) yields, referred to as the "reactor antineutrino flux anomaly." In this paper, global fits are applied to existing IBD yield measurements to produce constraints on antineutrino production by individual plutonium and uranium fission isotopes. We find that fits including measurements from highly U 235 -enriched cores and fits including Daya Bay's new fuel evolution result produce discrepant best-fit IBD yields for U 235 and Pu 239 . This discrepancy can be alleviated in a global analysis of all data sets through simultaneous fitting of Pu 239 , U 235 , and U 238 yields. The measured IBD yield of U 238 in this analysis is (7.02 ±1.65 )×10-43 cm2/fission , nearly two standard deviations below existing predictions. Future hypothetical IBD yield measurements by short-baseline reactor experiments are examined to determine their possible impact on the global understanding of isotopic IBD yields. It is found that future improved short-baseline IBD yield measurements at both high-enriched and low-enriched cores can significantly improve constraints for U 235 , U 238 , and Pu 239 , providing comparable or superior precision to existing conversion- and summation-based antineutrino flux predictions. Systematic and experimental requirements for these future measurements are also investigated.

  7. Nitrogen Isotope Evidence for a Shift in Eastern Beringian Nitrogen Cycle after the Terminal Pleistocene

    Science.gov (United States)

    Tahmasebi, F.; Longstaffe, F. J.; Zazula, G.

    2016-12-01

    The loess deposits of eastern Beringia, a region in North America between 60° and 70°N latitude and bounded by Chukchi Sea to the west and the Mackenzie River to the east, are a magnificent repository of Late Pleistocene megafauna fossils. The stable carbon and nitrogen isotope compositions of these fossils are measured to determine the paleodiet of these animals, and hence the paleoenvironment of this ecosystem during the Quaternary. For this approach to be most successful, however, requires consideration of possible changes in nutrient cycling and hence the carbon and nitrogen isotopic compositions of vegetation in this ecosystem. To test for such a shift following the terminal Pleistocene, we analyzed the stable carbon and nitrogen isotope compositions of modern plants and bone collagen of Arctic ground squirrels from Yukon Territory, and fossil plants and bones recovered from Late Pleistocene fossil Arctic ground squirrel nests. The data for modern samples provided a measure of the isotopic fractionation between ground squirrel bone collagen and their diet. The over-wintering isotopic effect of decay on typical forage grasses was also measured to evaluate its role in determining fossil plant isotopic compositions. The grasses showed only a minor change ( 0-1 ‰) in carbon isotope composition, but a major change ( 2-10 ‰) in nitrogen isotope composition over the 317-day experiment. Based on the modern carbon isotope fractionation between ground squirrel bone collagen and their diet, the modern vegetation carbon isotopic baseline provides a suitable proxy for the Late Pleistocene of eastern Beringia, after accounting for the Suess effect. However, the predicted nitrogen isotope composition of vegetation comprising the diet of fossil ground squirrels remains 2.5 ‰ higher than modern grasslands in this area, even after accounting for possible N-15 enrichment during decay. This result suggests a change in N cycling in this region since the Late Pleistocene.

  8. Titanium stable isotopic variations in chondrites, achondrites and lunar rocks

    Science.gov (United States)

    Greber, Nicolas D.; Dauphas, Nicolas; Puchtel, Igor S.; Hofmann, Beda A.; Arndt, Nicholas T.

    2017-09-01

    SaU 169 exhibits a heavy δ49Ti value of +0.330 ± 0.034‰ which is interpreted to result from Ti isotopic fractionation during ilmenite precipitation in the late stages of lunar magma ocean crystallization. A Rayleigh distillation calculation predicts that a δ49Ti value of +0.330‰ is achieved after removal of 94% of Ti in ilmenite.

  9. Iron isotope characteristics of Hot Springs at Chocolate Pots, Yellowstone National Park.

    Science.gov (United States)

    Wu, Lingling; Brucker, Rebecca Poulson; Beard, Brian L; Roden, Eric E; Johnson, Clark M

    2013-11-01

    Chocolate Pots Hot Springs in Yellowstone National Park is a hydrothermal system that contains high aqueous ferrous iron [∼0.1 mM Fe(II)] at circumneutral pH conditions. This site provides an ideal field environment in which to test our understanding of Fe isotope fractionations derived from laboratory experiments. The Fe(III) oxides, mainly produced through Fe(II) oxidation by oxygen in the atmosphere, have high ⁵⁶Fe/⁵⁴Fe ratios compared with the aqueous Fe(II). However, the degree of fractionation is less than that expected in a closed system at isotopic equilibrium. We suggest two explanations for the observed Fe isotope compositions. One is that light Fe isotopes partition into a sorbed component and precipitate out on the Fe(III) oxide surfaces in the presence of silica. The other explanation is internal regeneration of isotopically heavy Fe(II) via dissimilatory Fe(III) reduction farther down the flow path as well as deeper within the mat materials. These findings provide evidence that silica plays an important role in governing Fe isotope fractionation factors between reduced and oxidized Fe. Under conditions of low ambient oxygen, such as may be found on early Earth or Mars, significantly larger Fe isotope variations are predicted, reflecting the more likely attainment of Fe isotope equilibrium associated with slower oxidation rates under low-O₂ conditions.

  10. Bayesian Integration of Isotope Ratios for Geographic Sourcing of Castor Beans

    Energy Technology Data Exchange (ETDEWEB)

    Webb-Robertson, Bobbie-Jo M.; Kreuzer, Helen W.; Hart, Garret L.; Ehleringer, James; West, Jason B.; Gill, Gary A.; Duckworth, Douglas C.

    2012-08-15

    Recent years have seen an increase in the forensic interest associated with the poison ricin, which is extracted from the seeds of the Ricinus communis plant. Both light element (C, N, O, and H) and strontium (Sr) isotope ratios have previously been used to associate organic material with geographic regions of origin. We present a Bayesian integration methodology that can more accurately predict the region of origin for a castor bean than individual models developed independently for light element stable isotopes or Sr isotope ratios. Our results demonstrate a clear improvement in the ability to correctly classify regions based on the integrated model with a class accuracy of 6 0 . 9 {+-} 2 . 1 % versus 5 5 . 9 {+-} 2 . 1 % and 4 0 . 2 {+-} 1 . 8 % for the light element and strontium (Sr) isotope ratios, respectively. In addition, we show graphically the strengths and weaknesses of each dataset in respect to class prediction and how the integration of these datasets strengthens the overall model.

  11. Integrating stomach content and stable isotope analyses to quantify the diets of pygoscelid penguins.

    Directory of Open Access Journals (Sweden)

    Michael J Polito

    Full Text Available Stomach content analysis (SCA and more recently stable isotope analysis (SIA integrated with isotopic mixing models have become common methods for dietary studies and provide insight into the foraging ecology of seabirds. However, both methods have drawbacks and biases that may result in difficulties in quantifying inter-annual and species-specific differences in diets. We used these two methods to simultaneously quantify the chick-rearing diet of Chinstrap (Pygoscelis antarctica and Gentoo (P. papua penguins and highlight methods of integrating SCA data to increase accuracy of diet composition estimates using SIA. SCA biomass estimates were highly variable and underestimated the importance of soft-bodied prey such as fish. Two-source, isotopic mixing model predictions were less variable and identified inter-annual and species-specific differences in the relative amounts of fish and krill in penguin diets not readily apparent using SCA. In contrast, multi-source isotopic mixing models had difficulty estimating the dietary contribution of fish species occupying similar trophic levels without refinement using SCA-derived otolith data. Overall, our ability to track inter-annual and species-specific differences in penguin diets using SIA was enhanced by integrating SCA data to isotopic mixing modes in three ways: 1 selecting appropriate prey sources, 2 weighting combinations of isotopically similar prey in two-source mixing models and 3 refining predicted contributions of isotopically similar prey in multi-source models.

  12. Isotope shifts in francium isotopes Fr-213206 and 221Fr

    Science.gov (United States)

    Collister, R.; Gwinner, G.; Tandecki, M.; Behr, J. A.; Pearson, M. R.; Zhang, J.; Orozco, L. A.; Aubin, S.; Gomez, E.; FrPNC Collaboration

    2014-11-01

    We present the isotope shifts of the 7 s1 /2 to 7 p1 /2 transition for francium isotopes 206 -213Fr with reference to 221Fr collected from two experimental periods. The shifts are measured on a sample of atoms prepared within a magneto-optical trap by a fast sweep of radio-frequency sidebands applied to a carrier laser. King plot analysis, which includes literature values for 7 s1 /2 to 7 p3 /2 isotope shifts, provides a field shift constant ratio of 1.0520(10) and a difference between the specific mass shift constants of 170(100) GHz amu between the D1 and D2 transitions, of sufficient precision to differentiate between ab initio calculations.

  13. Molecular isotopic engineering (MIE): industrial manufacture of naproxen of predetermined stable carbon-isotopic compositions for authenticity and security protection and intellectual property considerations

    Science.gov (United States)

    Jasper, J. P.; Farina, P.; Pearson, A.; Mezes, P. S.; Sabatelli, A. D.

    2016-05-01

    Molecular Isotopic Engineering (MIE) is the directed stable-isotopic synthesis of chemical products for reasons of product identification and of product security, and also for intellectual property considerations. We report here a generally excellent correspondence between the observed and predicted stable carbon-isotopic (δ13C) results for a successful directed synthesis of racemic mixture from its immediate precursors. The observed results are readily explained by the laws of mass balance and isotope mass balance. Oxygen- and hydrogen isotopic results which require an additional assessment of the effects of O and H exchange, presumably due to interaction with water in the reaction solution, are addressed elsewhere. A previous, cooperative study with the US FDA-DPA showed that individual manufacturers of naproxen could readily be differentiated by their stable-isotopic provenance (δ13C, δ18O, and δD ref. 1). We suggest that MIE can be readily employed in the bio/pharmaceutical industry without alteration of present manufacturing processes other than isotopically selecting and/or monitoring reactants and products.

  14. Isotopes a very short introduction

    CERN Document Server

    Ellam, Rob

    2016-01-01

    An isotope is a variant form of a chemical element, containing a different number of neutrons in its nucleus. Most elements exist as several isotopes. Many are stable while others are radioactive, and some may only exist fleetingly before decaying into other elements. In this Very Short Introduction, Rob Ellam explains how isotopes have proved enormously important across all the sciences and in archaeology. Radioactive isotopes may be familiar from their use in nuclear weapons, nuclear power, and in medicine, as well as in carbon dating. They have been central to establishing the age of the Earth and the origins of the solar system. Combining previous and new research, Ellam provides an overview of the nature of stable and radioactive isotopes, and considers their wide range of modern applications. ABOUT THE SERIES: The Very Short Introductions series from Oxford University Press contains hundreds of titles in almost every subject area. These pocket-sized books are the perfect way to get ahead in a new subjec...

  15. Reactor Fuel Isotopics and Code Validation for Nuclear Applications

    Energy Technology Data Exchange (ETDEWEB)

    Francis, Matthew W. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Weber, Charles F. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pigni, Marco T. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Gauld, Ian C. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2015-02-01

    Experimentally measured isotopic concentrations of well characterized spent nuclear fuel (SNF) samples have been collected and analyzed by previous researchers. These sets of experimental data have been used extensively to validate the accuracy of depletion code predictions for given sets of burnups, initial enrichments, and varying power histories for different reactor types. The purpose of this report is to present the diversity of data in a concise manner and summarize the current accuracy of depletion modeling. All calculations performed for this report were done using the Oak Ridge Isotope GENeration (ORIGEN) code, an internationally used irradiation and decay code solver within the SCALE comprehensive modeling and simulation code. The diversity of data given in this report includes key actinides, stable fission products, and radioactive fission products. In general, when using the current ENDF/B-VII.0 nuclear data libraries in SCALE, the major actinides are predicted to within 5% of the measured values. Large improvements were seen for several of the curium isotopes when using improved cross section data found in evaluated nuclear data file ENDF/B-VII.0 as compared to ENDF/B-V-based results. The impact of the flux spectrum on the plutonium isotope concentrations as a function of burnup was also shown. The general accuracy noted for the actinide samples for reactor types with burnups greater than 5,000 MWd/MTU was not observed for the low-burnup Hanford B samples. More work is needed in understanding these large discrepancies. The stable neodymium and samarium isotopes were predicted to within a few percent of the measured values. Large improvements were seen in prediction for a few of the samarium isotopes when using the ENDF/B-VII.0 libraries compared to results obtained with ENDF/B-V libraries. Very accurate predictions were obtained for 133Cs and 153Eu. However, the predicted values for the stable ruthenium and rhodium isotopes varied

  16. Stirling Isotope Power System Program. Final report, January 1978-December 1980

    Energy Technology Data Exchange (ETDEWEB)

    1980-12-01

    The Stirling Isotope Power System (SIPS) design is discussed, including the control system and engine starter. The development, of fabrication, and testing of the SIPS converter are presented. The work performed on the Isotope Heat Source Assembly is described. The ancillary equipment, system integration and qualification, and safety are discussed. The safety discussion consists primarily of prediction of dose rates around the IHS and the influence on handling equipment design. Reliability and quality assurance are included. (MHR)

  17. Descriptive study of the even-even actinide nuclei 230 - 234Th isotopes using IBM-1

    Science.gov (United States)

    Al-Dahan, N.

    2017-06-01

    The nuclear structure of the actinide even-even thorium isotopes from A=230-234 have been investigated within the framework of the Interacting Boson Model (IBM-1). Predictions are given for the excited state energies for the ground state, β and γ-bands, the transition probabilities between these states, the rotational moment of inertia, and the energy staggering in the γ-band energies. The results of these calculations are compared with the experimental data on these isotopes.

  18. Non-linear Isotope Effects

    DEFF Research Database (Denmark)

    Schmidt, Johan Albrecht

    The isotopic fractionation associated with photodissociation of N2O, OCS and CO2, at different altitudes in Earth’s atmosphere, is investigated theoretically using constructed quantum mechanical models of the dissociation processes (i.e. potential energy surfaces and relevant coupling elements......’s stratosphere is nearly mass dependent, and only a small fraction of the observed anomalous oxygen-17 excess can be attributed to N2O photolysis. In contrast, stratospheric photolysis produces a significant inverse clumped isotope effect.(ii) Stratospheric OCS photolysis significantly enrich the remaining OCS...... in heavy carbon. The sulfur fractionation is weak and photolysis of OCS in the stratosphere produces only a small and mass dependent enrichment of heavy sulfur isotopes in the remaining OCS. Sulfur fractionation from the two remaining chemical sinks (oxidation by O(3P) and OH, respectively) is weak...

  19. Isotope specific arbitrary material sorter

    Science.gov (United States)

    Barty, Christopher P.J.

    2015-12-08

    A laser-based mono-energetic gamma-ray source is used to provide a rapid and unique, isotope specific method for sorting materials. The objects to be sorted are passed on a conveyor in front of a MEGa-ray beam which has been tuned to the nuclear resonance fluorescence transition of the desired material. As the material containing the desired isotope traverses the beam, a reduction in the transmitted MEGa-ray beam occurs. Alternately, the laser-based mono-energetic gamma-ray source is used to provide non-destructive and non-intrusive, quantitative determination of the absolute amount of a specific isotope contained within pipe as part of a moving fluid or quasi-fluid material stream.

  20. Progress update on IUPAC Project 2009-046-2-200: Terminology and definition of quantities related to the isotope distribution in elements with more than two stable isotopes

    Science.gov (United States)

    Kaiser, Jan; Angert, Alon; Bergquist, Bridget; Brand, Willi; Ono, Shuhei; Röckmann, Thomas; Savarino, Joël

    2014-05-01

    The objective of IUPAC Project 2009-046-2-200 (http://www.iupac.org/web/ins/2009-046-2-200) is to define terminology and to identify the most suitable definitions of quantities that characterise the isotope distribution in elements with more than two stable isotopes, including so-called mass-independent fractionation, non-mass dependent fractionation, isotope anomaly, 17O excess, etc. Most atmospheric oxygen-bearing species show deviations in their triple oxygen isotope ratios from mass-dependent fractionation (MDF) relationships predicted by the theories of Urey, Bigeleisen and Mayer. Similar deviations have also been found in sulphur and other elements with more than two stables isotopes (e.g. Hg, Cd, Zn), often preserved in non-atmospheric reservoirs, including rocks, minerals, soils, ice and waters. Despite the ubiquity of this type of isotope anomaly, there has never been an attempt to clearly define the terminology and physical quantities used to measure these anomalies and the processes that lead to their formation. Terms like mass-independent fractionation, non-mass dependent fractionation, isotope anomaly, isotope excess etc. have been used in the historic and recent literature, but are often not carefully distinguished. The realisation that MDF comprises a range of possible relationships between the isotopes of one element led to further complications because it meant that apparent isotope anomalies could be created by a combination of different MDF processes. At the moment, at least four different definitions to quantify isotope anomalies are being used. Furthermore, coefficients used in these definitions vary, which makes the comparison of data from different sources very difficult, even for experts. A consistent set of recommendations on how to express and quantify the isotope distribution in elements with more than two stable isotopes is highly warranted. From our experience as academic teachers, we are woefully aware how impenetrable the field is for

  1. Isotope Fractionation in the Interstellar Medium

    Science.gov (United States)

    Charnley, Steven

    2011-01-01

    Anomalously fractionated isotopic material is found in many primitive Solar System objects, such as meteorites and comets. It is thought, in some cases, to trace interstellar matter that was incorporated into the Solar Nebula without undergoing significant processing. We will present the results of models of the nitrogen, oxygen, and carbon fractionation chemistry in dense molecular clouds, particularly in cores where substantial freeze-out of molecules on to dust has occurred. The range of fractionation ratios expected in different interstellar molecules will be discussed and compared to the ratios measured in molecular clouds, comets and meteoritic material. These models make several predictions that can be tested in the near future by molecular line observations, particularly with ALMA.

  2. Catalytic-site design for inverse heavy-enzyme isotope effects in human purine nucleoside phosphorylase.

    Science.gov (United States)

    Harijan, Rajesh K; Zoi, Ioanna; Antoniou, Dimitri; Schwartz, Steven D; Schramm, Vern L

    2017-06-20

    Heavy-enzyme isotope effects (15N-, 13C-, and 2H-labeled protein) explore mass-dependent vibrational modes linked to catalysis. Transition path-sampling (TPS) calculations have predicted femtosecond dynamic coupling at the catalytic site of human purine nucleoside phosphorylase (PNP). Coupling is observed in heavy PNPs, where slowed barrier crossing caused a normal heavy-enzyme isotope effect (kchemlight/kchemheavy > 1.0). We used TPS to design mutant F159Y PNP, predicted to improve barrier crossing for heavy F159Y PNP, an attempt to generate a rare inverse heavy-enzyme isotope effect (kchemlight/kchemheavy effect of 1.31 for native PNP and an inverse effect of 0.75 for F159Y PNP. Increased isotopic mass in F159Y PNP causes more efficient transition state formation. Independent validation of the inverse isotope effect for heavy F159Y PNP came from commitment to catalysis experiments. Most heavy enzymes demonstrate normal heavy-enzyme isotope effects, and F159Y PNP is a rare example of an inverse effect. Crystal structures and TPS dynamics of native and F159Y PNPs explore the catalytic-site geometry associated with these catalytic changes. Experimental validation of TPS predictions for barrier crossing establishes the connection of rapid protein dynamics and vibrational coupling to enzymatic transition state passage.

  3. Cosmology: Rare isotopic insight into the Universe

    Science.gov (United States)

    Prantzos, Nikos

    2016-01-01

    Light isotopes of hydrogen and helium formed minutes after the Big Bang. The study of one of these primordial isotopes, helium-3, has now been proposed as a useful strategy for constraining the physics of the standard cosmological model.

  4. α -decay chains of superheavy Mt-279265 isotopes

    Science.gov (United States)

    Santhosh, K. P.; Nithya, C.

    2017-10-01

    The α -decay chains of the isotopes Mt-279265 are predicted by comparing the α half-lives calculated within the Coulomb and proximity potential model for deformed nuclei of Santhosh et al. [Nucl. Phys. A 850, 34 (2011)], 10.1016/j.nuclphysa.2010.12.002 with the spontaneous fission half-lives using the shell-effect-dependent formula of Santhosh and Nithya [Phys. Rev. C 94, 054621 (2016)], 10.1103/PhysRevC.94.054621. α half-lives also are calculated using different theoretical formalisms for comparison. The predicted half-lives and decay modes match well with the experimental results. The use of four different mass tables for calculating the α - decay energies indicates that the mass table of Wang et al. [Chin. Phys. C 41, 030003 (2017)], 10.1088/1674-1137/41/3/030003, which is based on the AME2016 atomic mass evaluation, is in better agreement with experimental results. The paper predicts long α chains from 265,267-269,271-273MT with half-lives within experimental limits. The isotopes 274-276,278Mt exhibit 2α chains followed by spontaneous fission. The 2α chain of 266Mt and the 4α chain of 270Mt end with electron capture. The isotopes Mt,279277 decay via spontaneous fission. We hope that the paper will open up new areas in this field.

  5. Developmentand Application of Accelerator Isotopes in China

    OpenAIRE

    YANG Yuan-you; LI Fei-ze; LIAO Jia-li; Liu, Ning

    2015-01-01

    Compared with the isotopes generated by nuclear reactor, the isotopes prepared by accelerator always show high specific activity and short half-life period. And most of such isotopes always were neutron-deficient nuclides, giving β+ or single energy γ ray. As one of the most important methods preparing radionuclides, the preparation of isotopes by accelerator has attracted more and more attention from the beginning of 21th century. The development of the preparation and application of the acc...

  6. Neon Isotope Fractionation in Ice Cores at Close-Off Depth

    Science.gov (United States)

    Liang, C.; Severinghaus, J. P.

    2015-12-01

    Analyzing trapped air bubbles in glacial ice is a well-established and useful method to reconstruct past atmospheric gas concentrations. However, trapped gas composition can be affected by fractionation during the closure of the air bubbles, complicating the reconstruction. Gases such as dioxygen (O2) and dihydrogen (H2) are known to leak out of the bubbles by permeation through the ice lattice at the close-off depth,where firn turns into ice. This process also can cause isotope fractionation, which obscures the past atmospheric isotope ratios in air bubbles in glacial ice. In order to establish the most accurate measurements of past atmospheric content, we need very detailed understanding of the permeation leakage mechanism in order to establish possible corrections. In this study, we propose the use of neon stable isotopes (neon-22 and neon-20) to place constraints on the mechanism of permeation leakage. Neon isotopes are an ideal system to explore because neon has a constant atmospheric isotope ratio, and thus only is affected by close-off fractionation. Neon permeation occurs via velocity-dependent hopping between sites within the ice lattice, because the neon atom is smaller than the critical size (3.6 Å) of the opening in the lattice. Theory predicts that neon isotope fractionation will occur due to the lower velocity of the heavier isotope, but this has never been experimentally verified and the theory is unable to quantitatively predict the magnitude of the fractionation. We will present the first results of high-precision neon isotope (22Ne/20Ne) measurements made in air pumped from the firm-to-ice transition in the Greenland Ice Sheet, where actively closing air bubbles drive permeation leakage. By measuring this natural neon isotope fractionation, we hope to learn about the mass dependence of the leakage mechanism and develop a more quantitative theory that is generalizable to biogeochemically- and climatically-active gases.

  7. Experimental calibration of Mg isotope fractionation between aragonite and seawater

    Science.gov (United States)

    Wang, Zhengrong; Hu, Ping; Gaetani, Glenn; Liu, Chao; Saenger, Casey; Cohen, Anne; Hart, Stanley

    2013-02-01

    The detectable magnesium (Mg) isotope fractionation between biogenic aragonite (including aragonitic corals, bivalves, scaphopod, and sclerosponges) and seawater can potentially be applied to reconstruct sea surface temperature (SST) in the past. To calibrate this thermometer, eight sets of inorganic precipitation experiments ('free-drift') in seawater (Mg/Ca = 5 or 10) have been carried out at 25-55 °C over a range of degassing rate. A cleaning procedure was adopted to remove Mg contamination by sea salt, surface absorbed Mg and silicate dust as nucleation centers. The Mg isotope fractionation between cleaned aragonite and seawater-like aqueous solution varies insignificantly with Mg/Ca ratios and Mg isotope compositions of the initial solution, and the CO2-degassing rate (0-75 cc/min), but decreases noticeably with increasing temperatures having a temperature sensitivity of ˜0.008-0.01‰/°C in the following form: Δ≈1000lnα=1.67(±0.36)-0.82(±0.11)×{1000}/{T} where αaragonite-seawater is the fractionation factor, and T is the absolute temperature in Kelvin. It is consistent with equilibrium fractionation between Mg2+ aquo-complex and magnesite predicted by one theoretical calculation. Qualitative comparison among Mg-bearing carbonates based on Mg-O bond strengths show the relative sequence of 26Mg enrichment is aragonite > dolomite > magnesite > calcite. Thus, the surprising agreement indicates either the calculation overestimated Mg fractionation between magnesite and fluid, or both theoretical calculation and our calibration represent Mg isotope fractionation between MgCO30-H2O cluster and Mg2+ aquo complexes. Comparison of our calibration with the Mg isotope fractionation between biogenic aragonite and seawater suggests Mg and oxygen isotope fractionations of some biogenic aragonites (e.g., Porites sp. corals) agree with our calibration within analytical uncertainty, whereas others deviate significantly, indicating biological and/or kinetic isotope

  8. [Lipid metabolism and lipogenesis: application of stable isotopes].

    Science.gov (United States)

    Martínez, J A; Martí, A

    1998-01-01

    Fat metabolism is regulated by several neuroendocrine and nutritional factors, which affect equilibrium between lipogenesis and lipolysis. Lipid utilization and fate in the organism can be assessed by in vivo and in vitro methods by measuring the rate of the different metabolic pathways (dynamic aspects), but also the net balance which may lead to fat accumulation or loss (static aspects). The quantitation of synthesis and breakdown reactions can be performed by using different tracers such as radioactive and stable isotopes. Fatty acid synthesis can be independently measured by the intravenous infusion of 13C acetate and application of the MIDA technique. In brief, this method uses probability analysis to measure the synthesis of biological polymers. It is based on the mathematical principle that the labeling pattern of a polymer synthesized from a stable-isotopically labeled precursor will conform to a predicted binomial or multinomial expansion. Thus, the isotopic enrichment of the precursor pool is calculated from measurements on the product alone. In the case of fatty acid synthesis, the proportions of excess (above natural background abundance) of single-labeled and double labeled (EM1 and EM2 species respectively) are a function of the probability (p) that the precursor subunits were isotopically labeled. Using this value of P for the isotopic enrichment of the acetylCoA pool, the theoretical 13C enrichment in the fatty acid if 100% were newly formed from this acetate pool is calculated. The actual isotopic enrichment is measured by gas chromatography-mass spectrometry (GCMS). This value divided by the theoretical maximum value equals the fraction of the fatty acid that is newly formed (f). The value for f represents dilution of de novo synthesized fatty acid by non-de novo sources. This method requires that newly synthesized (labeled) and preformed (unlabeled) mix in the liver and communicate with plasma VLDL over the period of the isotope infusion. It also

  9. Stable isotopes and biomarkers in microbial ecology

    NARCIS (Netherlands)

    Boschker, H.T.S.; Middelburg, J.J.

    2002-01-01

    The use of biomarkers in combination with stable isotope analysis is a new approach in microbial ecology and a number of papers on a variety of subjects have appeared. We will first discuss the techniques for analysing stable isotopes in biomarkers, primarily gas chromatography-combustion-isotope

  10. Use of Isotopes for Studying Reaction Mechanisms

    Indian Academy of Sciences (India)

    In the first part of this series, we discussed how isotopes can be used as markers to determine the nature of intermediates in chemical reactions. The second part covered the effect of isotopes on equilibria and reactions, in processes where the bond to the isotopic a tom is broken. We showed with specific examples how.

  11. Mercury isotope fractionation during precipitation of metacinnabar (β-HgS) and montroydite (HgO).

    Science.gov (United States)

    Smith, Robin S; Wiederhold, Jan G; Kretzschmar, Ruben

    2015-04-07

    To utilize stable Hg isotopes as a tracer for Hg cycling and pollution sources in the environment, it is imperative that fractionation factors for important biogeochemical processes involving Hg are determined. Here, we report experimental results on Hg isotope fractionation during precipitation of metacinnabar (β-HgS) and montroydite (HgO). In both systems, we observed mass-dependent enrichments of light Hg isotopes in the precipitates relative to the dissolved Hg. Precipitation of β-HgS appeared to follow equilibrium isotope fractionation with an enrichment factor ε(202)Hg(precipitate-supernatant) of -0.63‰. Precipitation of HgO resulted in kinetic isotope fractionation, which was described by a Rayleigh model with an enrichment factor of -0.32‰. Small mass-independent fractionation was observed in the HgS system, presumably related to nuclear volume fractionation. We propose that Hg isotope fractionation in the HgS system occurred in solution during the transition of O- to S-coordination of Hg(II), consistent with theoretical predictions. In the HgO system, fractionation was presumably caused by the faster precipitation of light Hg isotopes, and no isotopic exchange between solid and solution was observed on the timescale investigated. The results of this work emphasize the importance of Hg solution speciation and suggest that bonding partners of Hg in solution complexes may control the overall isotope fractionation. The determined fractionation factor and mechanistic insights will have implications for the interpretation of Hg isotope signatures and their use as an environmental tracer.

  12. Crystal chemical constraints on inter-mineral Fe isotope fractionation and implications for Fe isotope disequilibrium in San Carlos mantle xenoliths

    Science.gov (United States)

    Macris, Catherine A.; Manning, Craig E.; Young, Edward D.

    2015-04-01

    The origin of variations in iron isotope compositions of mantle minerals is uncertain, and predictions of equilibrium inter-mineral iron isotope fractionation conflict. This hinders interpretation of the petrologic and geochemical implications of Fe isotope data from mantle lithologies. To address this, we present a revised ionic model for predicting equilibrium iron isotope fractionation between mantle minerals and use it to interpret measured inter-mineral iron isotopic fractionation from five distinct mantle xenolith lithologies from San Carlos, Arizona. The samples represent a broad range of modal abundances and include lherzolite, harzburgite, dunite, clinopyroxenite, and websterite. The xenoliths exhibit Fe-isotopic variation between minerals in a single sample, and between samples. In all cases where spinel and olivine coexist, the 57Fe/54Fe of spinel is greater than that of the corresponding olivine, agreeing with expectations for equilibrium fractionation from theory (ionic model), but disagreeing with predictions based on Mössbauer data. The 57Fe/54Fe values of clinopyroxenes from the xenoliths show no clear systematic differences. We interpret this to be a result of varying degrees of metasomatism, perhaps involving interaction with a melt. The spinel peridotite samples (lherzolite, harzburgite, and dunite) are partially melted residual mantle that exhibit a decrease in whole-rock 57Fe/54Fe with increasing olivine abundance. This is consistent with progressive extraction of a 57Fe-rich partial melt. The clinopyroxenite has the highest whole-rock 57Fe/54Fe, consistent with its origin as a cumulate from an unrelated magma possessing elevated 57Fe/54Fe. The websterite sample is transitional to Group II type xenoliths, has the lowest whole-rock 57Fe/54Fe of the investigated samples, and likely experienced a more complex metasomatic history. This study demonstrates that the Fe isotope compositions of San Carlos xenoliths and their component minerals record

  13. Masses of exotic calcium isotopes pin down nuclear forces.

    Science.gov (United States)

    Wienholtz, F; Beck, D; Blaum, K; Borgmann, Ch; Breitenfeldt, M; Cakirli, R B; George, S; Herfurth, F; Holt, J D; Kowalska, M; Kreim, S; Lunney, D; Manea, V; Menéndez, J; Neidherr, D; Rosenbusch, M; Schweikhard, L; Schwenk, A; Simonis, J; Stanja, J; Wolf, R N; Zuber, K

    2013-06-20

    The properties of exotic nuclei on the verge of existence play a fundamental part in our understanding of nuclear interactions. Exceedingly neutron-rich nuclei become sensitive to new aspects of nuclear forces. Calcium, with its doubly magic isotopes (40)Ca and (48)Ca, is an ideal test for nuclear shell evolution, from the valley of stability to the limits of existence. With a closed proton shell, the calcium isotopes mark the frontier for calculations with three-nucleon forces from chiral effective field theory. Whereas predictions for the masses of (51)Ca and (52)Ca have been validated by direct measurements, it is an open question as to how nuclear masses evolve for heavier calcium isotopes. Here we report the mass determination of the exotic calcium isotopes (53)Ca and (54)Ca, using the multi-reflection time-of-flight mass spectrometer of ISOLTRAP at CERN. The measured masses unambiguously establish a prominent shell closure at neutron number N = 32, in excellent agreement with our theoretical calculations. These results increase our understanding of neutron-rich matter and pin down the subtle components of nuclear forces that are at the forefront of theoretical developments constrained by quantum chromodynamics.

  14. Masses of exotic calcium isotopes pin down nuclear forces

    CERN Document Server

    Wienholtz, F; Blaum, K; Borgmann, Ch; Breitenfeldt, M; Cakirli, R B; George, S; Herfurth, F; Holt, J D; Kowalska, M; Kreim, S; Lunney, D; Manea, V; Menéndez, J; Neidherr, D; Rosenbusch, M; Schweikhard, L; Schwenk, A; Simonis, J; Stanja, J; Wolf, R N; Zuber, K

    2013-01-01

    The properties of exotic nuclei on the verge of existence play a fundamental part in our understanding of nuclear interactions. Exceedingly neutron-rich nuclei become sensitive to new aspects of nuclear forces. Calcium, with its doubly magic isotopes $^{40}$Ca and $^{48}$Ca, is an ideal test for nuclear shell evolution, from the valley of stability to the limits of existence. With a closed proton shell, the calcium isotopes mark the frontier for calculations with three-nucleon forces from chiral effective field theory. Whereas predictions for the masses of $^{51}$Ca and $^{52}$Ca have been validated by direct measurements$^4$, it is an open question as to how nuclear masses evolve for heavier calcium isotopes. Here we report the mass determination of the exotic calcium isotopes $^{53}$Ca and $^{54}$Ca, using the multi-reflection time-of-flight mass spectrometer of ISOLTRAP at CERN. The measured masses unambiguously establish a prominent shell closure at neutron number N = 32, in excellent agreement with our t...

  15. Isotope Harvesting Opportunities at FRIB

    Science.gov (United States)

    Morrissey, David

    2017-01-01

    The fragmentation of fast heavy ion beams now at the National Superconducting Cyclotron Laboratory (NSCL) and in the future at the Facility for Rare Isotope Beams (FRIB) under construction produce an unprecedentedly broad spectrum of radionuclides but only a small fraction are used in the on-line rare-isotope program. Projectile fragmentation facilities provide an electromagnetically purified beam of a single projectile fragment for nuclear physics experiments ranging from low energy astrophysics, through nuclear structure studies, to probing fundamental symmetries. By augmenting the NSCL and FRIB production facilities with complimentary collection and purification of discarded ions, called isotope harvesting with chemical purification, many other nuclides will become available for off-line experiments in parallel with the primary experiment. A growing user community has established a list of key target isotopes and is working with the FRIB design team to allow inclusion of necessary equipment in the future. An overview of the possibilities and the techniques will be presented in this talk. Supported by Office of Science, US DOE and Michigan State University.

  16. Charge radii of radium isotopes

    NARCIS (Netherlands)

    Wansbeek, L. W.; Schlesser, S.; Sahoo, B. K.; Dieperink, A. E. L.; Onderwater, C. J. G.; Timmermans, R. G. E.

    2012-01-01

    We present a combined analysis of the available isotope-shift data from the optical spectra of Ra atoms and Ra+ ions. Atomic structure calculations of the field-shift and specific mass-shift constants of the low-lying levels in Ra+ are used. The nuclear radial differences delta for the radium

  17. Surface area dependence of calcium isotopic reequilibration in carbonates: Implications for isotopic signatures in the weathering zone

    Science.gov (United States)

    Fernandez, N. M.; Druhan, J. L.; Potrel, A.; Jacobson, A. D.

    2016-12-01

    The concept of dynamic equilibrium carries the implicit assumption of continued isotopic exchange between a mineral and the surrounding fluid. While this effect has received much attention in the marine paleoproxy literature, it has been relatively overlooked in application to the terrestrial environment. In weathering systems, a potential consequence is that rapid reequilibration may alter or erase isotopic signatures generated during secondary mineral formation. The extent and timescale over which isotopic signatures are reset in these hydrologic systems is unknown. Using reactive transport modeling, we show isotopic reequilibration under conditions reflecting terrestrial hydrologic settings to be significant and dependent on the reactive surface area of the solid. In particular, we suggest that the non-traditional stable isotopes commonly used in application to carbonates (e.g., Ca, Mg, Sr) are sensitive to these effects due to their rapid reaction rates. We aim to characterize the dependence of Ca isotopic reequilibration on surface area during calcite precipitation via batch experiments conducted at ambient temperature over 48-hour time periods. Calcite precipitation was performed in a closed batch reactor utilizing a controlled free-drift method. The batch reactors contained mixed supersaturated solutions of CaCl2 and NaHCO3 at an initial pH of 8.54. Precipitation was initiated by seed inoculation of calcite crystals with two distinct, pre-constrained surface areas. All experiments achieved the same final state of chemical equilibrium, but as expected, the fastest approach to equilibrium occurred for experiments employing calcite seeds with the highest surface area. This implies that differences in equilibrated Ca isotope ratios (δ44/40Ca) should reflect differences in surface area. This prediction is upheld by models of the experiments, indicating a measureable difference in δ44Ca during calcite precipitation where the higher surface area corresponds to

  18. The isotopic contamination in electromagnetic isotope separators; La contagion isotopique dans les separateurs electromagnetiques d'isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Cassignol, Ch. [Commissariat a l' Energie Atomique, Saclay (France).Centre d' Etudes Nucleaires

    1959-07-01

    In the early years of isotope separation, and in particular electromagnetic isotope separation, needs for rapid results have conducted to empiric research. This paper describes fundamental research on the electromagnetic isotope separation to a better understanding of isotope separators as well as improving the performances. Focus has been made on the study of the principle of isotope contamination and the remedial action on the separator to improve the isotope separation ratio. In a first part, the author come back to the functioning of an electromagnetic separator and generalities on isotope contamination. Secondly, it describes the two stages separation method with two dispersive apparatus, an electromagnetic separation stage followed by an electrostatic separation stage, both separated by a diaphragm. The specifications of the electrostatic stage are given and its different settings and their consequences on isotope separation are investigated. In a third part, mechanisms and contamination factors in the isotope separation are discussed: natural isotope contamination, contamination by rebounding on the collector, contamination because of a low resolution, contamination by chromatism and diffusion effect, breakdown of condenser voltage. Analysis of experimental results shows the diffusion as the most important contamination factor in electromagnetic isotope separation. As contamination factors are dependent on geometric parameters, sector angle, radius of curvature in the magnetic field and clearance height are discussed in a fourth part. The better understanding of the mechanism of the different contamination factors and the study of influential parameters as pressure and geometric parameters lead to define a global scheme of isotope contamination and determinate optima separator design and experimental parameters. Finally, the global scheme of isotope contamination and hypothesis on optima specifications and experimental parameters has been checked during a

  19. An isotopic model for basal freeze-on associated with subglacial upward flow of pore water

    Science.gov (United States)

    Souchez, R.; Samyn, D.; Lorrain, R.; Pattyn, F.; Fitzsimons, S.

    2004-01-01

    Subglacial freezing in polar glaciers can have a significant dynamical effect. Recent studies have shown that freezing of pore water flowing upward through subglacial fine-grained sediments at the freezing interface and progression of this freezing front downward are responsible for fast ice flow stoppage in ice streams. The upward pore water flow leads to the formation of debris-bearing basal ice layers. A model for stable isotope composition, both in δD and δ18O, is developed for predicting the isotopic composition of the ice segregated by such a mechanism. The development of this isotopic model for water films present along the grains of the subglacial sediment predicts the absence of apparent fractionation for the ice formed. This prediction is tested against two East Antarctic outlet glaciers by studying the δD-δ18O relationships in the basal ice layers of these glaciers.

  20. Isotopic Compositions of the Elements 1989

    Science.gov (United States)

    De Laeter, J. R.; Heumann, K. G.; Rosman, K. J. R.

    1991-11-01

    The Subcommittee for Isotopic Abundance Measurements (SIAM) of the IUPAC Commission on Atomic Weights and Isotopic Abundances has carried out its biennial review of isotopic compositions, as determined by mass spectrometry and other relevant methods. The Subcommittee's critical evaluation of the published literature element by element forms the basis of the Table of Isotopic Compositions of the Elements as Determined by Mass Spectrometry 1989, which is presented in this Report. Atomic Weights calculated from the tabulated isotopic abundances are consistent with Ar(E) values listed in the Table of Standard Atomic Weights 1989.

  1. Stable isotope compounds - production, detection, and application.

    Science.gov (United States)

    Zachleder, Vilém; Vítová, Milada; Hlavová, Monika; Moudříková, Šárka; Mojzeš, Peter; Heumann, Hermann; Becher, Johannes R; Bišová, Kateřina

    2018-01-19

    Stable isotopes are used in wide fields of application from natural tracers in biology, geology and archeology through studies of metabolic fluxes to their application as tracers in quantitative proteomics and structural biology. We review the use of stable isotopes of biogenic elements (H, C, N, O, S, Mg, Se) with the emphasis on hydrogen and its heavy isotope deuterium. We will discuss the limitations of enriching various compounds in stable isotopes when produced in living organisms. Finally, we overview methods for measuring stable isotopes, focusing on methods for detection in single cells in situ and their exploitation in modern biotechnologies. Copyright © 2018. Published by Elsevier Inc.

  2. Modelling stable water isotopes: Status and perspectives

    Directory of Open Access Journals (Sweden)

    Werner M.

    2010-12-01

    Full Text Available Modelling of stable water isotopes H2 18O and HDO within various parts of the Earth’s hydrological cycle has clearly improved our understanding of the interplay between climatic variations and related isotope fractionation processes. In this article key principles and major research results of stable water isotope modelling studies are described. Emphasis is put on research work using explicit isotope diagnostics within general circulation models as this highly complex model setup bears many resemblances with studies using simpler isotope modelling approaches.

  3. Joint interpretation of enantiomer and stable isotope fractionation for chiral pesticides degradation.

    Science.gov (United States)

    Jin, Biao; Rolle, Massimo

    2016-11-15

    Chiral pesticides are important contaminants affecting the health and functioning of aquatic systems. The combination of stable isotope and enantiomer analysis techniques has been recently proposed to better characterize the fate of these contaminants in natural and engineered settings. We introduce a modeling approach with the aim of unifying and integrating the interpretation of isotopic and enantiomeric fractionation. The model is based on the definition of enantiomer-specific isotopologues and jointly predicts the evolution of concentration, enantiomer fractionation, as well as changes in stable isotope ratios of different elements. The method allows evaluating different transformation pathways and was applied to investigate enzymatic degradation of dichlorprop (DCPP), enzymatic degradation of mecoprop methyl ester (MCPPM), and microbial degradation of α-hexachlorocyclohexane (α-HCH) by different bacterial strains and under different redox conditions. The model accurately reproduces the isotopic and enantiomeric data observed in previous experimental studies and precisely captures the dual-dimensional trends characterizing different reaction pathways. Furthermore, the model allows testing possible combinations of enantiomer analysis (EA), compound specific isotope analysis (CSIA), and enantiomer specific isotope analysis (ESIA) to identify and assess isotope and enantiomer selective reaction mechanisms. Copyright © 2016 Elsevier Ltd. All rights reserved.

  4. Hydrogen isotope adsorption on nano-carbons

    Energy Technology Data Exchange (ETDEWEB)

    Hideki, Tanaka; Daisuke, Noguchi [Chiba Univ., Diversity and Fractal Science, Graduate School of Science and Technology, (Japan); Hirofumi, Kanoh; Katsumi, Kaneko [Chiba Univ., Dept. of Chemistry, Faculty of Science (Japan)

    2005-07-01

    Hydrogen adsorption on carbonaceous materials has received considerable attention in recent decades, because physisorption of hydrogen was considered to be the most promising hydrogen storage technology to achieve the US Department of Energy (DOE) target for fuel cell powered vehicles. Many simulation studies of hydrogen adsorption on single-wall carbon nano-tubes (SWNTs) and graphitic slit pores have been performed by assuming that hydrogen can be modeled as a classical fluid above 77 K, to predict their hydrogen storage capacities; however, Wang et al. recently developed path integral grand canonical Monte Carlo (PI-GCMC) technique to explore statistical properties of quantum fluids [1] and then they applied the PI-GCMC simulation to a study of hydrogen adsorption on SWNTs including quantum effects [2]. Surprisingly, they showed that quantum effects are very important even at 298 K for adsorption in interstices of SWNT bundles: the interstitial adsorption of hydrogen from the quantum simulations is quite smaller than that from classical simulations. Recently, we also showed that quantum effects on adsorption of hydrogen isotopes on single-wall carbon nano-horn (SWNH) are significant at 77 K by comparing experiment and simulations [3]. We have thus measured adsorption isotherms of H{sub 2} and D{sub 2} on nano-carbons [activated carbon fibers (ACFs) and single-wall carbon nano-tubes (SWNTs)] to evaluate quantum effects on adsorption at low temperatures, and found that, for example, adsorption of H{sub 2} on ACFs are about 10% larger than D{sub 2} at 77 K and 0.1 MPa. We have also performed grand canonical Monte Carlo (GCMC) simulations for hydrogen isotope adsorption on graphitic slit pore, SWNT and SWNT bundle models. Quantum effects were incorporated in the simulations through the Feynman-Hibbs (FH) effective potential based on the classical Lennard-Jones (LJ) potential. Fig. 1 shows simulated hydrogen isotope adsorption isotherms on the (10,10) nano-tube bundle

  5. Hydrogen isotope adsorption on nano-carbons

    Energy Technology Data Exchange (ETDEWEB)

    Hideki Tanaka; Daisuke Noguchi [Diversity and Fractal Science, Graduate School of Science and Technology, Chiba University 1-33 Yayoi, Inage, Chiba 263-8522, (Japan); Hirofumi Kanoh; Katsumi Kaneko [Department of Chemistry, Faculty of Science, Chiba University, 1-33 Yayoi, Inage, Chiba 263-8522, (Japan)

    2005-07-01

    Hydrogen adsorption on carbonaceous materials has received considerable attention in recent decades, because physi-sorption of hydrogen was considered to be the most promising hydrogen storage technology to achieve the US Department of Energy (DOE) target for fuel cell powered vehicles. Many simulation studies of hydrogen adsorption on single-wall carbon nano-tubes (SWNTs) and graphitic slit pores have been performed by assuming that hydrogen can be modeled as a classical fluid above 77 K, to predict their hydrogen storage capacities; however, Wang et al. recently developed path integral grand canonical Monte Carlo (PI-GCMC) technique to explore statistical properties of quantum fluids and then they applied the PI-GCMC simulation to a study of hydrogen adsorption on SWNTs including quantum effects. Surprisingly, they showed that quantum effects are very important even at 298 K for adsorption in interstices of SWNT bundles: the interstitial adsorption of hydrogen from the quantum simulations is quite smaller than that from classical simulations. Recently, we also showed that quantum effects on adsorption of hydrogen isotopes on single-wall carbon nano-horn (SWNH) are significant at 77 K by comparing experiment and simulations. We have thus measured adsorption isotherms of H{sub 2} and D{sub 2} on nano-carbons [activated carbon fibers (ACFs) and single-wall carbon nano-tubes (SWNTs)] to evaluate quantum effects on adsorption at low temperatures, and found that, for example, adsorption of H{sub 2} on ACFs are about 10% larger than D{sub 2} at 77 K and 0.1 MPa. We have also performed grand canonical Monte Carlo (GCMC) simulations for hydrogen isotope adsorption on graphitic slit pore, SWNT and SWNT bundle models. Quantum effects were incorporated in the simulations through the Feynman-Hibbs (FH) effective potential based on the classical Lennard-Jones (LJ) potential. Fig. 1 shows simulated hydrogen isotope adsorption isotherms on the (10,10) nano-tube bundle at 77 K

  6. Zinc isotopic compositions of breast cancer tissue.

    Science.gov (United States)

    Larner, Fiona; Woodley, Laura N; Shousha, Sami; Moyes, Ashley; Humphreys-Williams, Emma; Strekopytov, Stanislav; Halliday, Alex N; Rehkämper, Mark; Coombes, R Charles

    2015-01-01

    An early diagnostic biomarker for breast cancer is essential to improve outcome. High precision isotopic analysis, originating in Earth sciences, can detect very small shifts in metal pathways. For the first time, the natural intrinsic Zn isotopic compositions of various tissues in breast cancer patients and controls were determined. Breast cancer tumours were found to have a significantly lighter Zn isotopic composition than the blood, serum and healthy breast tissue in both groups. The Zn isotopic lightness in tumours suggests that sulphur rich metallothionein dominates the isotopic selectivity of a breast tissue cell, rather than Zn-specific proteins. This reveals a possible mechanism of Zn delivery to Zn-sequestering vesicles by metallothionein, and is supported by a similar signature observed in the copper isotopic compositions of one breast cancer patient. This change in intrinsic isotopic compositions due to cancer has the potential to provide a novel early biomarker for breast cancer.

  7. Measuring SNM Isotopic Distributions using FRAM

    Energy Technology Data Exchange (ETDEWEB)

    Geist, William H. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2015-12-02

    The first group of slides provides background information on the isotopic composition of plutonium. It is shown that 240Pu is the critical isotope in neutron coincidence/multiplicity counting. Next, response function analysis to determine isotopic composition is discussed. The isotopic composition can be determined by measuring the net peak counts from each isotope and then taking the ratio of the counts for each isotope relative to the total counts for the element. Then FRAM (Fixed energy Response function Analysis with Multiple efficiencies) is explained. FRAM can control data acquisition, automatically analyze newly acquired data, analyze previously acquired data, provide information on the quality of the analysis, and facilitate analysis in unusual situations (non-standard energy calibrations, gamma rays from non-SNM isotopes, poor spectra (within limits)).

  8. Stable carbon isotope ratios of ambient secondary organic aerosols in Toronto

    Science.gov (United States)

    Saccon, M.; Kornilova, A.; Huang, L.; Moukhtar, S.; Rudolph, J.

    2015-09-01

    A method to quantify concentrations and stable carbon isotope ratios of secondary organic aerosols has been applied to study atmospheric nitrophenols in Toronto, Canada. The sampling of five nitrophenols, all with substantial secondary formation from the photooxidation of aromatic volatile organic compounds (VOCs), was conducted in the gas phase and particulate matter (PM) together and in PM alone. Their concentrations in the atmosphere are in the low ng m-3 range and, consequently, a large volume of air (> 1000 m3) is needed to analyze samples for stable carbon isotope ratios, resulting in sampling periods of typically 24 h. While this extended sampling period increases the representativeness of average values, it at the same time reduces possibilities to identify meteorological conditions or atmospheric pollution levels determining nitrophenol concentrations and isotope ratios. Average measured carbon isotope ratios of the different nitrophenols are between -34 and -33 ‰, which is well within the range predicted by mass balance. However, the observed carbon isotope ratios cover a range of nearly 9 ‰ and approximately 20 % of the isotope ratios of the products have isotope ratios lower than predicted from the kinetic isotope effect of the first step of the reaction mechanism and the isotope ratio of the precursor. This can be explained by isotope fractionation during reaction steps following the initial reaction of the precursor VOCs with the OH radical. Limited evidence for local production of nitrophenols is observed since sampling was done in the Toronto area, an urban center with significant anthropogenic emission sources. Strong evidence for significant local formation of nitrophenols is only found for samples collected in summer. On average, the difference in carbon isotope ratios between nitrophenols in the particle phase and in the gas phase is insignificant, but for a limited number of observations in summer, a substantial difference is observed. This

  9. Isotope hydrology of catchment basins: lithogenic and cosmogenic isotopic systems

    Energy Technology Data Exchange (ETDEWEB)

    Nimz, G. J., LLNL

    1998-06-01

    A variety of physical processes affect solute concentrations within catchment waters. The isotopic compositions of the solutes can indicate which processes have determined the observed concentrations. These processes together constitute the physical history of the water. Many solutes in natural waters are derived from the interaction between the water and the rock and/or soil within the system - these are termed `lithogenic` solutes. The isotopic compositions of these solutes provide information regarding rock-water interactions. Many other solutes have their isotopic compositions determined both within and outside of the catchment - i.e., in addition to being derived from catchment rock and soil, they are solutes that are also transported into the catchment. Important members of this group include solutes that have isotopic compositions produced by atomic particle interactions with other nuclides. The source of the atomic particles can be cosmic radiation (producing `cosmogenic` nuclides in the atmosphere and land surface), anthropogenic nuclear reactions (producing `thermonuclear` nuclides), or radioactive and fission decay of naturally-occurring elements, principally {sup 238}U (producing `in-situ` lithogenic nuclides in the deep subsurface). Current language usage often combines all of the atomic particle-produced nuclides under the heading `cosmogenic nuclides`, and for simplicity we will often follow that usage here, although always indicating which variety is being discussed. This paper addresses the processes that affect the lithogenic and cosmogenic solute concentrations in catchment waters, and how the isotopic compositions of the solutes can be used in integrative ways to identify these processes, thereby revealing the physical history of the water within a catchment system. The concept of a `system` is important in catchment hydrology. A catchment is the smallest landscape unit that can both participate in all of the aspects of the hydrologic cycle and

  10. Methane clumped isotopes: Progress and potential for a new isotopic tracer

    Energy Technology Data Exchange (ETDEWEB)

    Douglas, Peter M. J.; Stolper, Daniel A.; Eiler, John M.; Sessions, Alex L.; Lawson, Michael; Shuai, Yanhua; Bishop, Andrew; Podlaha, Olaf G.; Ferreira, Alexandre A.; Santos Neto, Eugenio V.; Niemann, Martin; Steen, Arne S.; Huang, Ling; Chimiak, Laura; Valentine, David L.; Fiebig, Jens; Luhmann, Andrew J.; Seyfried, William E.; Etiope, Giuseppe; Schoell, Martin; Inskeep, William P.; Moran, James J.; Kitchen, Nami

    2017-11-01

    The isotopic composition of methane is of longstanding geochemical interest, with important implications for understanding hydrocarbon systems, atmospheric greenhouse gas concentrations, the global carbon cycle, and life in extreme environments. Recent analytical developments focusing on multiply substituted isotopologues (‘clumped isotopes’) are opening a potentially valuable new window into methane geochemistry. When methane forms in internal isotopic equilibrium, clumped isotopes can provide a direct record of formation temperature, making this property particularly valuable for identifying different methane origins. However, it has also become clear that in certain settings methane clumped isotope measurements record kinetic rather than equilibrium isotope effects. Here we present a substantially expanded dataset of methane clumped isotope analyses, and provide a synthesis of the current interpretive framework for this parameter. We review different processes affecting methane clumped isotope compositions, describe the relationships between conventional isotope and clumped isotope data, and summarize the types of information that this measurement can provide in different Earth and planetary environments.

  11. C-isotope composition of fossil sedges and grasses

    Science.gov (United States)

    Kurschner, Wolfram M.

    2010-05-01

    C4 plants differ from C3 plants regarding their anatomy and their C-isotope composition. Both features can be used in the geological record to determine the presence of C4 plants. Yet, the evolution of the C4 pathway in the fossil record is enigmatic as palaeobotanical and geological evidence for C4 plants is sparse. The oldest structural evidence for Kranz anatomy has been found in Late Miocene permineralized grass leaf remains. But studies on the C-isotope composition of sedimentary organic matter indicate that abundant C4 biomass was present in N-America and Asia throughout the Miocene in expanding savannahs and grasslands. The success of C4 plants appears to be related also to an increasing seasonal aridity in the tropical climate belts and the co-evolution of grazers. However, C- isotope composition of palaeosols or vertebrate teeth only allows to estimate the abundance of C4 plant biomass in the vegetation or in the diet without further taxonomical specification which plant groups would have had C4 metabolism. In this contribution the first extensive C-isotope analysis of fossil seeds of sedges and a few grasses are presented. The age of the carpological material ranges from Late Eocene to Pliocene and was collected from several central European brown coal deposits. The 52 different taxa studied include several species of Carex, Cladiocarya, Eriopherum, Eleocharis, Scirpus, Sparganium. Most of them representing herbaceous elements of a (sub)tropical vegetation growing near the edge of a lake. The C-isotope composition of the fossil seeds varies between -30 and -23 o/oo indicating C3 photosynthesis. This first systematic inventory shows that C4 plants were absent in the European (sub)tropical brown coal forming wetland vegetation during the Tertiary. These preliminary data are in agreement with phylogenetic studies which predict the origin of C4 plants outside the European realm.

  12. Early inner solar system origin for anomalous sulfur isotopes in differentiated protoplanets.

    Science.gov (United States)

    Antonelli, Michael A; Kim, Sang-Tae; Peters, Marc; Labidi, Jabrane; Cartigny, Pierre; Walker, Richard J; Lyons, James R; Hoek, Joost; Farquhar, James

    2014-12-16

    Achondrite meteorites have anomalous enrichments in (33)S, relative to chondrites, which have been attributed to photochemistry in the solar nebula. However, the putative photochemical reactions remain elusive, and predicted accompanying (33)S depletions have not previously been found, which could indicate an erroneous assumption regarding the origins of the (33)S anomalies, or of the bulk solar system S-isotope composition. Here, we report well-resolved anomalous (33)S depletions in IIIF iron meteorites (inner solar system (inner solar system S-isotope composition was chondritic (consistent with IAB iron meteorites, Earth, Moon, and Mars). The range of mass-independent sulfur isotope compositions may reflect spatial or temporal changes influenced by photochemical processes. A tentative correlation between S isotopes and Hf-W core segregation ages suggests that the two systems may be influenced by common factors, such as nebular location and volatile content.

  13. Study of shape evolution and electromagnetic properties in neutron-rich Zr and Sr isotopes

    Science.gov (United States)

    Chaudhary, R.; Devi, R.; Khosa, S. K.

    2017-09-01

    The projected shell model calculations have been carried out in neutron-rich 100-108Zr and 98-102Sr isotopes. The shape evolution and electromagnetic properties have been examined in neutron-rich Zr and Sr isotopes around N = 60. The structure of yrast states, backbending phenomena, g-factors and B(E2) transition probabilities are calculated and compared with corresponding observable quantities. The present calculations predict the occurrence of coexistence of prolate-oblate shapes at 0+ state in 100,102Zr and 98,100Sr. Nuclei beyond N = 62 are predicted to have prolate deformation in the ground-state.

  14. Temperature limits for preservation of primary calcite clumped isotope paleotemperatures

    Science.gov (United States)

    Henkes, Gregory A.; Passey, Benjamin H.; Grossman, Ethan L.; Shenton, Brock J.; Pérez-Huerta, Alberto; Yancey, Thomas E.

    2014-08-01

    Solid-state reordering of C-O bonds in the calcite lattice can alter the clumped isotope composition of paleotemperature archives such as fossil brachiopod shells without inducing significant changes in shell microstructure and trace element concentrations, metrics commonly used to gauge preservation quality. To correctly interpret the paleoenvironmental significance of clumped isotope-derived paleotemperatures, it is necessary to understand the temperature-time domain in which solid-state C-O bond reordering is important. We address this question using a combination of laboratory and natural geological experiments on Paleozoic brachiopod shells. The laboratory experiments involve heating fossil brachiopod calcite at different temperatures and times to directly observe rates of 13C-18O bond reordering. The resulting Arrhenius parameters are indistinguishable from values previously determined for an optical calcite with similar trace element compositions. We develop an alternative kinetic model for reordering that accounts for non-first-order reaction progress observed during the initial several hundred minutes of laboratory heating experiments, and show that the simplified first-order approximation model (Passey and Henkes, 2012) predicts reaction progress equally well for temperatures and timescales relevant to sedimentary basins. We evaluate our laboratory-based rate predictions by studying brachiopod calcite from several sedimentary basins with independently constrained burial temperature histories. Specifically, we use the laboratory-derived Arrhenius parameters to predict the evolution of brachiopod calcite clumped isotope compositions during successive one million-year time steps reflecting the burial and exhumation temperature paths of each basin. While this exercise is limited by the relatively large uncertainties in the temperature histories of these basins, we find general correspondence, within error, between predicted and observed clumped isotope values

  15. Can stable isotopes ride out the storms? The role of convection for water isotopes in models, records, and paleoaltimetry studies in the central Andes

    Science.gov (United States)

    Rohrmann, Alexander; Strecker, Manfred R.; Bookhagen, Bodo; Mulch, Andreas; Sachse, Dirk; Pingel, Heiko; Alonso, Ricardo N.; Schilgen, Taylor F.; Montero, Carolina

    2015-04-01

    Globally, changes in stable isotope ratios of oxygen and hydrogen (δ18O and δD) in the meteoric water cycle result from distillation and evaporation processes. Isotope fractionation occurs when air masses rise in elevation, cool, and reduce their water-vapor holding capacity with decreasing temperature. As such, d18O and dD values from a variety of sedimentary archives are often used to reconstruct changes in continental paleohydrology as well as paleoaltimetry of mountain ranges. Based on 234 stream-water samples, we demonstrate that areas experiencing deep convective storms in the eastern south-central Andes (22 - 28° S) do not show the commonly observed relationship between δ18O and δD with elevation. These convective storms arise from intermontane basins, where diurnal heating forces warm air masses upward, resulting in cloudbursts and raindrop evaporation. Especially at the boundary between the tropical and extra-tropical atmospheric circulation regimes where deep-convective storms are very common (~ 26° to 32° N and S), the impact of such storms may yield non-systematic stable isotope-elevation relationships as convection dominates over adiabatic lifting of air masses. Because convective storms can reduce or mask the depletion of heavy isotopes in precipitation as a function of elevation, linking modern or past topography to patterns of stable isotope proxy records can be compromised in mountainous regions, and atmospheric circulation models attempting to predict stable isotope patterns must have sufficiently high spatial resolution to capture the fractionation dynamics of convective cells. Rohrmann, A. et al. Can stable isotopes ride out the storms? The role of convection for water isotopes in models, records, and paleoaltimetry studies in the central Andes. Earth Planet. Sci. Lett. 407, 187-195 (2014).

  16. Clumped isotope effects during OH and Cl oxidation of methane

    Science.gov (United States)

    Whitehill, Andrew R.; Joelsson, Lars Magnus T.; Schmidt, Johan A.; Wang, David T.; Johnson, Matthew S.; Ono, Shuhei

    2017-01-01

    A series of experiments were carried out to determine the clumped (13CH3D) methane kinetic isotope effects during oxidation of methane by OH and Cl radicals, the major sink reactions for atmospheric methane. Experiments were performed in a 100 L quartz photochemical reactor, in which OH was produced from the reaction of O(1D) (from O3 photolysis) with H2O, and Cl was from photolysis of Cl2. Samples were taken from the reaction cell and analyzed for methane (12CH4, 12CH3D, 13CH4, 13CH3D) isotopologue ratios using tunable infrared laser direct absorption spectroscopy. Measured kinetic isotope effects for singly substituted species were consistent with previous experimental studies. For doubly substituted methane, 13CH3D, the observed kinetic isotope effects closely follow the product of the kinetic isotope effects for the 13C and deuterium substituted species (i.e., 13,2KIE = 13KIE × 2KIE). The deviation from this relationship is 0.3‰ ± 1.2‰ and 3.5‰ ± 0.7‰ for OH and Cl oxidation, respectively. This is consistent with model calculations performed using quantum chemistry and transition state theory. The OH and Cl reactions enrich the residual methane in the clumped isotopologue in open system reactions. In a closed system, however, this effect is overtaken by the large D/H isotope effect, which causes the residual methane to become anti-clumped relative to the initial methane. Based on these results, we demonstrate that oxidation of methane by OH, the predominant oxidant for tropospheric methane, will only have a minor (∼0.3‰) impact on the clumped isotope signature (Δ13CH3D, measured as a deviation from a stochastic distribution of isotopes) of tropospheric methane. This paper shows that Δ13CH3D will provide constraints on methane source strengths, and predicts that Δ12CH2D2 can provide information on methane sink strengths.

  17. Anthropogenic lead isotopes in Antarctica

    Science.gov (United States)

    Rosman, K. J. R.; Chisholm, W.; Boutron, C. F.; Candelone, J.-P.; Patterson, C. C.

    1994-12-01

    We report the first measurements of Pb isotopes in Antarctic snow, which show that even recent snow containing 2.3 pg/g is highly polluted with anthropogenic Pb. This follows from a comparison of isotope abundances of Pb in surface snow and terrestrial dust extracted from ancient Antarctic ice (Dome C, depth 308 m, approximate age 7,500 a BP), the latter being distinctly more radiogenic. This result is dependent of geochemical arguments based on measurements of Al, Na and SO4. South America is suggested as a likely source of this anthropogenic Pb. The presence of significantly less radiogenic Pb in the snow adjacent to two Antarctic base stations indicates that there is contamination from station emissions, although emission from Australia is an alternative explanation for a site 33 km from Dumont d'Urville.

  18. Isotope fractionation of cadmium in lunar material

    Science.gov (United States)

    Schediwy, S.; Rosman, K. J. R.; de Laeter, J. R.

    2006-03-01

    The double spike technique has been used to measure the isotope fractionation and elemental abundance of Cd in nine lunar samples, the Brownfield meteorite and the Columbia River Basalt BCR-1, by thermal ionisation mass spectrometry. Lunar soil samples give a tightly grouped set of positive isotope fractionation values of between + 0.42% and + 0.50% per mass unit. Positive isotope fractionation implies that the heavy isotopes are enhanced with respect to those of the Laboratory Standard. A vesicular mare basalt gave zero isotope fractionation, indicating that the Cd isotopic composition of the Moon is identical to that of the Earth. A sample of orange glass from the Taurus-Littrow region gave a negative isotope fractionation of - 0.23 ± 0.06% per mass unit, presumably as a result of redeposition of Cd from the Cd-rich vapour cloud associated with volcanism. Cadmium is by far the heaviest element to show isotope fractionation effects in lunar samples. The volatile nature of Cd is of importance in explaining these isotope fractionation results. Although a number of mechanisms have been postulated to be the cause of isotope fractionation of certain elements in lunar soils, we believe that the most likely mechanisms are ion and particle bombardment of the lunar surface.

  19. Anthropogenic lead isotopes in Antarctica

    Energy Technology Data Exchange (ETDEWEB)

    Rosman, K.J.R.; Chisholm, W. [Curtin Univ. of Technology, Bentley (Australia); Boutron, C.F. [Laboratoire de Glaciologie et Geophysique de l`Environnement du CNRS, St. Martin d`Heres (France)]|[Domaine Universitaire, Grenoble (France); Candelone, J.P. [Laboratoire de Glaciologie et Geophysique de l`Environnement du CNRS, St. Martin d`Heres (France); Patterson, C.C. [California Institute of Technology, Pasadena, CA (United States)

    1994-12-01

    The authors present results from the first Pb isotopic study of the sources of lead in snow samples from the Antarctic. Samples of recent snow fields were compared with measurements of samples taken from deep cores, and they reveal that recent snows show pronounced influence of anthropogenic sources. These results are independent of geochemical arguments based on influences of Al, Na, or SO{sub 4}.

  20. Comparative isotope ecology of African great apes.

    Science.gov (United States)

    Oelze, Vicky M; Fahy, Geraldine; Hohmann, Gottfried; Robbins, Martha M; Leinert, Vera; Lee, Kevin; Eshuis, Henk; Seiler, Nicole; Wessling, Erin G; Head, Josephine; Boesch, Christophe; Kühl, Hjalmar S

    2016-12-01

    The isotope ecology of great apes is a useful reference for palaeodietary reconstructions in fossil hominins. As extant apes live in C3-dominated habitats, variation in isotope signatures is assumed to be low compared to hominoids exploiting C4-plant resources. However, isotopic differences between sites and between and within individuals are poorly understood due to the lack of vegetation baseline data. In this comparative study, we included all species of free-ranging African great apes (Pan troglodytes, Pan paniscus, Gorilla sp.). First, we explore differences in isotope baselines across different habitats and whether isotopic signatures in apes can be related to feeding niches (faunivory and folivory). Secondly, we illustrate how stable isotopic variations within African ape populations compare to other extant and extinct primates and discuss possible implications for dietary flexibility. Using 701 carbon and nitrogen isotope data points resulting from 148 sectioned hair samples and an additional collection of 189 fruit samples, we compare six different great ape sites. We investigate the relationship between vegetation baselines and climatic variables, and subsequently correct great ape isotope data to a standardized plant baseline from the respective sites. We obtained temporal isotopic profiles of individual animals by sectioning hair along its growth trajectory. Isotopic signatures of great apes differed between sites, mainly as vegetation isotope baselines were correlated with site-specific climatic conditions. We show that controlling for plant isotopic characteristics at a given site is essential for faunal data interpretation. While accounting for plant baseline effects, we found distinct isotopic profiles for each great ape population. Based on evidence from habituated groups and sympatric great ape species, these differences could possibly be related to faunivory and folivory. Dietary flexibility in apes varied, but temporal variation was overall

  1. ISODEP, A Fuel Depletion Analysis Code for Predicting Isotopic ...

    African Journals Online (AJOL)

    The code ISODEP is developed to compute the rate of production of nuclides in different homogeneous zones of a research reactor. An exponential method proposed by Hansen is the basis for the numerical solution of non-homogeneous simultaneous equations which describe the rate of production and decay of nuclides.

  2. WWW Table of Radioactive Isotopes

    Science.gov (United States)

    Firestone, R. B.; Ekstrom, L. P.; Chu, S. Y. F.

    1999-10-01

    An electronic sequel to the Table of Radioactive Isotopes (John Wiley, 1986) is being developed for use on the WWW. Updated adopted and decay data from the Evaluated Nuclear Structure Decay File (ENSDF) and other sources have been combined and edited. Decay scheme normalizations are revised when necessary. Gamma-ray and alpha-particle energies can be searched interactively by energy or parent half-life, mass, and atomic or neutron number. Summary data including half-lives, Q-values, production mode(s), genetic feedings, and a list of references published since the last full evaluation are available. Users can display energy or intensity ordered tables of gamma-rays, K and L x-rays, alpha-particles, and beta endpoints. Spectra of betas and bremsstrahlung, and Auger/conversion electrons can be viewed with an interactive JAVA applet. Decay schemes can be displayed with the JAVA version of Isotope Explorer 3.0. The URL for the Table of Radioactive Isotopes is http://nucleardata.nuclear.lu.se/nucleardata/toi/.

  3. Isotope Geochemistry for Comparative Planetology of Exoplanets

    Science.gov (United States)

    Mandt, K. E.; Atreya, S.; Luspay-Kuti, A.; Mousis, O.; Simon, A.; Hofstadter, M. D.

    2017-01-01

    Isotope geochemistry has played a critical role in understanding processes at work in and the history of solar system bodies. Application of these techniques to exoplanets would be revolutionary and would allow comparative planetology with the formation and evolution of exoplanet systems. The roadmap for comparative planetology of the origins and workings of exoplanets involves isotopic geochemistry efforts in three areas: (1) technology development to expand observations of the isotopic composition of solar system bodies and expand observations to isotopic composition of exoplanet atmospheres; (2) theoretical modeling of how isotopes fractionate and the role they play in evolution of exoplanetary systems, atmospheres, surfaces and interiors; and (3) laboratory studies to constrain isotopic fractionation due to processes at work throughout the solar system.

  4. Isotopic dependence of the giant monopole resonance in the even-A ^{112-124}Sn isotopes and the asymmetry term in nuclear incompressibility

    CERN Document Server

    Li, T; Liu, Y; Marks, R; Nayak, B K; Rao, P V Madhusudhana; Fujiwara, M; Hashimoto, H; Kawase, K; Nakanishi, K; Okumura, S; Yosoi, M; Itoh, M; Ichikawa, M; Matsuo, R; Terazano, T; Uchida, M; Kawabata, T; Akimune, H; Iwao, Y; Murakami, T; Sakaguchi, H; Terashima, S; Yasuda, Y; Zenihiro, J; Harakeh, M N

    2007-01-01

    The strength distributions of the giant monopole resonance (GMR) have been measured in the even-A Sn isotopes (A=112--124) with inelastic scattering of 400-MeV $\\alpha$ particles in the angular range $0^\\circ$--$8.5^\\circ$. We find that the experimentally-observed GMR energies of the Sn isotopes are lower than the values predicted by theoretical calculations that reproduce the GMR energies in $^{208}$Pb and $^{90}$Zr very well. From the GMR data, a value of $K_{\\tau} = -550 \\pm 100$ MeV is obtained for the asymmetry-term in the nuclear incompressibility.

  5. Toward Closing the Water Cycle over the ARM/CART Region: Implementation of Stable Water Isotope Physics in MM5

    Science.gov (United States)

    Kemball-Cook, S. R.; Miller, N. L.; DePaolo, D. J.

    2001-12-01

    To date, atmospheric water isotope modeling has been performed on a global scale. The development of a stable water isotope scheme in a mesoscale model will lead to a simulated spatial distribution that will improve our understanding of present day climate variability, as well as historical climate patterns. The purpose of this study was to add water isotope tracers to the regional atmospheric model MM5 (NCAR's Mesoscale Model 5) in order to link existing global and basin-scale isotope models, and to work toward an improved knowledge of the water budget over the ARM site. In order to include isotopic processes in MM5, eight new prognostic variables were added to the model's dynamical core. These are the isotopic mixing ratios for water vapor, cloud liquid water, cloud ice, and rain for the stable isotopes O18 and deuterium. The isotopes are treated in a manner similar to the natural water vapor, cloud liquid water, etc. in terms of diffusion, advection, nudging, and filtering. Isotope fractionation and diffusion are handled using the approach of Gedzelman and Arnold (1994). Processes treated in this model are fractionation during deposition of water vapor onto cloud ice and condensation of water vapor onto cloud water, and also diffusive exchange of isotopes between vapor and falling rain drops. The bulk flux model of Hoffman et al. (1998) is used here as a first order approximation for isotopic evaporative processes. For the runs to be discussed here, lateral boundary conditions were generated by the Melbourne University General Circulation Model. This GCM runs at a resolution of R21, and predicts values of the O18 and deuterium mixing ratios at each grid point. Results of preliminary model runs will be discussed.

  6. Isotopic Compositions of the Elements 1997

    Science.gov (United States)

    Rosman, K. J. R.; Taylor, P. D. P.

    1998-11-01

    The Commission's Subcommittee for the Isotopic Composition of the Elements has carried out its biennial review of isotopic compositions, as determined by mass spectrometry and other relevant methods. This involves a critical evaluation of the published literature, element by element, and forms the basis of the Table of Isotopic Compositions of the Elements as Determined by Mass Spectrometry presented here. New guidelines have been used to arrive at the uncertainties on the isotopic abundances and there are numerous changes to the table since it was last published in 1991. Atomic Weights calculated from this table are consistent with Ar(E) values listed in the Table of Standard Atomic Weights 1997.

  7. Stable isotope labeling methods for DNA.

    Science.gov (United States)

    Nelissen, Frank H T; Tessari, Marco; Wijmenga, Sybren S; Heus, Hans A

    2016-08-01

    NMR is a powerful method for studying proteins and nucleic acids in solution. The study of nucleic acids by NMR is far more challenging than for proteins, which is mainly due to the limited number of building blocks and unfavorable spectral properties. For NMR studies of DNA molecules, (site specific) isotope enrichment is required to facilitate specific NMR experiments and applications. Here, we provide a comprehensive review of isotope-labeling strategies for obtaining stable isotope labeled DNA as well as specifically stable isotope labeled building blocks required for enzymatic DNA synthesis. Copyright © 2016 Elsevier B.V. All rights reserved.

  8. Isotopic investigation of an Australian island environment

    Energy Technology Data Exchange (ETDEWEB)

    Groecke, D.R. [Australian National Univ., Canberra, ACT (Australia). Research School of Earth Sciences; Bocherens, H. [Paris-6 Univ., 75 (France)

    1996-12-31

    Collagen has been extracted from fossil bones of mega-fauna herbivores from Kangaroo Island, South Australia (Australia). Carbon and nitrogen stable isotope analyses of collagen have provided an insight into the palaeo-ecology of these late Pleistocene herbivores. In comparison with continental fossil localities in South Australia, the island herbivores have elevated nitrogen isotopic abundances. Carbon isotopic abundances suggest that browsing species had a mixed diet of grasses and leaves on the island, in contrast to the specimens from mainland Australia. Possible causes regarding elevated nitrogen isotope abundances and dietary shifts in this palaeo-ecology are discussed. (authors). 24 refs., 2 figs., 1 tab.

  9. Biogeochemical cycling in an organic-rich coastal marine basin. 8. A sulfur isotopic budget balanced by differential diffusion across the sediment-water interface

    Science.gov (United States)

    Chanton, J.P.; Martens, C.S.; Goldhaber, M.B.

    1987-01-01

    The sulfur isotopic composition of the sulfur fluxes occurring in the anoxic marine sediments of Cape Lookout Bight, N.C., U.S.A., was determined, and the result of isotopic mass balance was obtained via the differential diffusion model. Seasonal pore water sulfate ??34S measurements yielded a calculated sulfate input of 0.6%.. Sulfate transported into the sediments via diffusion appeared to be enriched in the lighter isotope because its concentration gradient was steeper, due to the increase in the measured isotopic composition of sulfate with depth. Similarly, the back diffusion of dissolved sulfide towards the sediment-water interface appeared enriched in the heavier isotope. The isotopic composition of this flux was calculated from measurements of the ??34S of dissolved sulfide and was determined to be 15.9%.. The isotopic composition of buried sulfide was determined to be -5.2%. and the detrital sulfur input was estimated to be -6.2%.. An isotope mass balance equation based upon the fluxes at the sediment-water interface successfully predicted the isotopic composition of the buried sulfur flux within 0.5%., thus confirming that isotopes diffuse in response to their individual concentration gradients. ?? 1987.

  10. Laboratory studies of carbon kinetic isotope effects on the production mechanism of particulate phenolic compounds formed by toluene photooxidation: a tool to constrain reaction pathways.

    Science.gov (United States)

    Irei, Satoshi; Rudolph, Jochen; Huang, Lin; Auld, Janeen; Collin, Fabrice; Hastie, Donald

    2015-01-08

    In this study, we examined compound-specific stable carbon isotope ratios for phenolic compounds in secondary organic aerosol (SOA) formed by photooxidation of isotope-label-free toluene. SOA generated by photooxidation of toluene using a continuous-flow reactor and an 8 m(3) indoor smog chamber was collected on filters, which were extracted with acetonitrile for compound-specific analysis. Eight phenolic compounds were identified in the extracts using a gas chromatograph coupled with a mass spectrometer, and their compound-specific stable carbon isotope ratios were determined using a gas chromatograph coupled with a combustion furnace followed by an isotope ratio mass spectrometer. The majority of products, including methylnitrophenols and methylnitrocatechols, were isotopically depleted by 5-6‰ compared to the initial isotope ratio of toluene, whereas the isotope ratio for 4-nitrophenol remained identical to that of toluene. On the basis of the reaction mechanisms proposed in previous reports, stable carbon isotope ratios of these products were calculated. By comparing the observed isotope ratios with the predicted isotope ratios, we explored possible production pathways for the particulate phenolic compounds.

  11. Excitation functions and isotopic effects in (n, p) reactions for stable nickel isotopes from reaction threshold to 20 MeV

    Energy Technology Data Exchange (ETDEWEB)

    Lalremruata, B. [Department of Physics, University of Pune, Ganeshkhind, Pune-411007, Maharashtra (India)], E-mail: marema@physics.unipune.ernet.in; Ganesan, S. [Reactor Physics Design Division, BARC, Mumbai 58 (India); Bhoraskar, V.N. [Department of Physics, University of Pune, Ganeshkhind, Pune-411007, Maharashtra (India)], E-mail: vnb@physics.unipune.ernet; Dhole, S.D. [Department of Physics, University of Pune, Ganeshkhind, Pune-411007, Maharashtra (India)], E-mail: sanjay@physics.unipune.ernet.in

    2009-05-01

    The excitation function for (n, p) reactions from reaction threshold to 20 MeV on five nickel isotopes viz; {sup 58}Ni, {sup 60}Ni, {sup 61}Ni, {sup 62}Ni and {sup 64}Ni were calculated using Talys-1.0 nuclear model code involving the fixed set of global parameters. A good agreement between the calculated and measured data is obtained with minimum effort on parameter fitting and only one free parameter called 'Shell damping factor'. This is of importance to the validation of nuclear model approaches with increased predictive power. The systematic decrease in (n, p) cross-sections with increasing neutron number in reactions induced by neutrons on isotopes of nickel is explained in terms of the proton separation energy and the pre-equilibrium model. The compound nucleus and pre-equilibrium reaction mechanism as well as the isotopic effects were also studied.

  12. Hydrogen and oxygen isotope values in hydrogen peroxide.

    Science.gov (United States)

    Barnette, Janet E; Lott, Michael J; Howa, John D; Podlesak, David W; Ehleringer, James R

    2011-05-30

    Hydrogen peroxide (H(2)O(2)) is a widely used oxidizer with many commercial applications; unfortunately, it also has terrorist-related uses. We analyzed 97 hydrogen peroxide solutions representing four grades purchased across the United States and in Mexico. As expected, the range of hydrogen (δ(2)H, 230‰) and oxygen (δ(18)O, 24‰) isotope values of the H(2)O(2) solutions was large, reflecting the broad isotopic range of dilution waters. This resulted in predictable linear relationships of δ(2)H and δ(18)O values of H(2)O(2) solutions that were near parallel to the Meteoric Water Line (MWL), offset by the concentration of H(2)O(2) in the solution. By grade, dilute (3 to 35%) H(2)O(2) solutions were not statistically different in slope. Although the δ(2)H values of manufactured H(2)O(2) could be different from those of water, rapid H(2)O(2)-H(2)O exchange of H atoms eliminated any distinct isotope signal. We developed a method to measure the δ(18)O value of H(2)O(2) independent of dilution water by directly measuring O(2) gas generated from a catalase-induced disproportionation reaction. We predicted that the δ(18)O values of H(2)O(2) would be similar to that of atmospheric oxygen (+23.5‰), the predominant source of oxygen in the most common H(2)O(2) manufacturing process (median disproportionated δ(18)O=23.8‰). The predictable H-O relationships in H(2)O(2) solutions make it possible to distinguish commercial dilutions from clandestine concentration practices. Future applications of this work include synthesis studies that investigate the chemical link between H(2)O(2) reagents and peroxide-based explosive products, which may assist law enforcement in criminal investigations. Copyright © 2011 John Wiley & Sons, Ltd.

  13. Unexpectedly large charge radii of neutron-rich calcium isotopes

    CERN Document Server

    Garcia Ruiz, R F; Blaum, K; Ekström, A; Frömmgen, N; Hagen, G; Hammen, M; Hebeler, K; Holt, J D; Jansen, G R; Kowalska, M; Kreim, K; Nazarewicz, W; Neugart, R; Neyens, G; Nörtershäuser, W; Papenbrock, T; Papuga, J; Schwenk, A; Simonis, J; Wendt, K A; Yordanov, D T

    2016-01-01

    Despite being a complex many-body system, the atomic nucleus exhibits simple structures for certain ‘magic’ numbers of protons and neutrons. The calcium chain in particular is both unique and puzzling: evidence of doubly magic features are known in 40,48Ca, and recently suggested in two radioactive isotopes, 52,54Ca. Although many properties of experimentally known calcium isotopes have been successfully described by nuclear theory, it is still a challenge to predict the evolution of their charge radii. Here we present the first measurements of the charge radii of 49,51,52Ca, obtained from laser spectroscopy experiments at ISOLDE, CERN. The experimental results are complemented by state-of-the-art theoretical calculations. The large and unexpected increase of the size of the neutron-rich calcium isotopes beyond N = 28 challenges the doubly magic nature of 52Ca and opens new intriguing questions on the evolution of nuclear sizes away from stability, which are of importance for our understanding of neutron-...

  14. Experimental verification of hydrogen isotope separation by pressure swing adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Kotoh, K. [Faculty of Eng., Kyushu Univ., 744 Moto-oka, Nishi-ku, Fukuoka 819-0395 (Japan); Tanaka, M. [National Inst. for Fusion Science, 322-6 Oroshi-cho, Toki-shi, Gifu 509-5292 (Japan); Nakamura, Y.; Sakamoto, T. [Faculty of Eng., Kyushu Univ., 744 Moto-oka, Nishi-ku, Fukuoka 819-0395 (Japan); Asakura, Y.; Uda, T. [National Inst. for Fusion Science, 322-6 Oroshi-cho, Toki-shi, Gifu 509-5292 (Japan); Sugiyama, T. [Faculty of Eng., Nagoya Univ., Furo-cho, Chikusa-ku, Nagoya 464-8603 (Japan)

    2008-07-15

    Focusing on synthetic zeolites that adsorb hydrogen isotopes at liquid N{sub 2} temperature with priority in the order of T{sub 2}, DT, D{sub 2}, HT, HD and H{sub 2}, we have been developing a pressure swing adsorption process system for hydrogen isotope separation. For this purpose, we carried out fundamental experiments of adsorption and desorption of a tracer D{sub 2} in bulk H{sub 2} with zeolite packed-bed columns. In this paper, the results are reported that D{sub 2} is enriched in the adsorbed phase at separation factors near 2.0, flowing through zeolite 5A and 13X packed-beds at 77.4 K. These are in agreement with values predicted from the multi-component equilibrium characteristics. In the gas samples recovered by evacuating the packed-beds, however, D{sub 2} was detected at a relative concentration of 1.20 or 1.32 to that in the feed gas. This lower range results from the isotopic mass effect in kinetic process. That suggests a highly D{sub 2}-enriched residual left during evacuation. This is verified with an unusually high enrichment factor of 6.68 or 9.21 for zeolite 5A or 13X measured in the residual sample desorbed from the packed-bed by heating up to room temperature. (authors)

  15. Exploring the isotopic niche: isotopic variance, physiological incorporation, and the temporal dynamics of foraging

    Directory of Open Access Journals (Sweden)

    Justin Douglas Yeakel

    2016-01-01

    Full Text Available Consumer foraging behaviors are dynamic, changing in response to prey availability, seasonality, competition, and even the consumer's physiological state. The isotopic composition of a consumer is a product of these factors as well as the isotopic `landscape' of its prey, i.e. the isotopic mixing space. Stable isotope mixing models are used to back-calculate the most likely proportional contribution of a set of prey to a consumer's diet based on their respective isotopic distributions, however they are disconnected from ecological process. Here we build a mechanistic framework that links the ecological and physiological processes of an individual consumer to the isotopic distribution that describes its diet, and ultimately to the isotopic composition of its own tissues, defined as its `isotopic niche’. By coupling these processes, we systematically investigate under what conditions the isotopic niche of a consumer changes as a function of both the geometric properties of its mixing space and foraging strategies that may be static or dynamic over time. Results of our derivations reveal general insight into the conditions impacting isotopic niche width as a function of consumer specialization on prey, as well as the consumer's ability to transition between diets over time. We show analytically that moderate specialization on isotopically unique prey can serve to maximize a consumer's isotopic niche width, while temporally dynamic diets will tend to result in peak isotopic variance during dietary transitions. We demonstrate the relevance of our theoretical findings by examining a marine system composed of nine invertebrate species commonly consumed by sea otters. In general, our analytical framework highlights the complex interplay of mixing space geometry and consumer dietary behavior in driving expansion and contraction of the isotopic niche. Because this approach is established on ecological mechanism, it is well-suited for enhancing the

  16. SWING - The Stable Water Isotope Intercomparison Group

    Science.gov (United States)

    Werner, M.; Barras, V.; Brown, J.; Gourcy, L.; Henderson-Sellers, A.; Hoffmann, G.; Ichiyanagi, K.; Kelley, M.; Noone, D.; Roads, J.; Schmidt, G.; Sturm, K.; Tindall, J.; Valdes, P.; Yoshimura, K.; Zakharov, V.

    2004-12-01

    For more than four decades the isotopic composition of water stored in various archives (e.g. ice cores, ground water) has been used to study changes in the hydrological cycle on timescales from glacial-interglacial to short term variations. However, the interpretation of isotopic variations in terms of climate change is often handicapped by a lack of other relevant observational climate parameters (e.g. temperature, relative humidity, precipitation) both in space and time. Modeling the isotopic composition of water within the hydrological cycle of general circulation models (GCM) may help to overcome this deficit on available climate data. Isotope GCMs simulate the 18O/16O (and/or 2H/1H) relation as an independent quantity within a closed "model world" where all other relevant climate parameters are known, too. This enables an improved analysis of (simulated) isotope variability in terms of climate change and during the last decade several state-of-the-art GCM models (GISS, ECHAM, LMD, GENESIS and others) have been enhanced by the capability to simulate the atmospheric and/or ocean cycle of H218O and 1H2H16O. To ensure isotope GCM reliability, any isotope GCM simulation must pass a rigorous comparison of simulated versus observed isotope data (model-data-intercomparison). In addition, artifacts in isotope simulations based on a specific GCM model parameterization or set-up have to be identified by comparing simulation results of several different isotope GCMs (model-model intercomparison). In our presentation we will give an overview and first results of the SWING project, founded in 2004. This initiative serves as a community platform for experts from the various isotope research groups and has the following objectives: (1) enable an overview about ongoing isotope GCM modeling capabilities; (2) define and perform future common GCM isotope simulation experiments of the various research groups; (3) identify the most important need of new observational isotope data

  17. Testing the Late-Veneer hypothesis with selenium isotopes

    Science.gov (United States)

    Labidi, J.; Koenig, S.; Bennett, N.; Kurzawa, T.; Aierken, E.; Shahar, A.; Schoenberg, R.

    2016-12-01

    Selenium (Se) is a siderophile element displaying an excess abundance in Earth's mantle compared to experimental predictions [1], which may be attributed to the Late-Veneer. As Se is also volatile, testing the late-veneer addition of Se can constrain the origin of other volatile elements on Earth. Here we combine high-precision Se isotope measurements of metal-silicate partitioning experiments and chondrites to assess whether planetary differentiation could leave a measurable Se isotopic signature on planetary mantles. We performed Se isotopic measurements of 5 metal-silicate partitioning experiments and 20 chondrites of all major classes. Experiments were conducted at 1 GPa and 1650 C for 1 to 4 hours using the piston-cylinder apparatus at Carnegie's Geophysical Laboratory. After wet chemistry, data were obtained on a ThermoFisher Scientific™ NeptunePlus MC-ICP-MS at the University of Tübingen with a 74Se/77Se double spike technique. δ82/76Se values are given relative to NIST SRM-3149 and the external reproducibility calculated from duplicate meteorite analyses is ≤ 0.1‰ (2 s.d.). Chondrites vary over a 0.8‰ range of δ82/76Se values. CIs and CMs show evidence for heavier 82Se/76Se ratios, likely due to mixing processes in the proto-planetary nebula. When these isotopically heavier meteorites are excluded, remaining chondrites have δ82/76Se values varying over a 0.3‰ range, within uncertainty of previous results [2]. We suggest that these chondrites may be used to estimate a δ82/76Se value of bulk planets. At the conditions of our experiments, the partition coefficients for Se log Dmetal-silicate range from 0.7±0.1 to 1.9±0.1, consistent with previous work [1]. A small but resolvable Se isotopic fractionation was observed: 82Se/76Se ratios were enriched by ≤ 0.5‰ in the silicates relative to the metals. Thus, given current uncertainties for Se isotopic measurements, marginal differences between planetary mantles and chondrites may be resolved

  18. Joint interpretation of enantiomer and stable isotope fractionation for chiral pesticides degradation

    DEFF Research Database (Denmark)

    Jin, Biao; Rolle, Massimo

    2016-01-01

    introduce a modeling approach with the aim of unifying and integrating the interpretation of isotopic and enantiomeric fractionation. The model is based on the definition of enantiomer-specific isotopologues and jointly predicts the evolution of concentration, enantiomer fractionation, as well as changes...

  19. Intrinsic gK factors of odd-mass 167−179Lu isotopes

    Indian Academy of Sciences (India)

    Phys. J. A3, 225 (1998)) using the spin matrix elements. The theoretical predictions for the gK factors exhibit good agreement with the experimental gK factors with increasing mass number A of the lutetium isotopes. The strongest influence of the neutron–proton spin interaction occurs at q = −1. Sufficient agreement between.

  20. Stable carbon and hydrogen isotope fractionation of dissolved organic groundwater pollutants by equilibrium sorption.

    Science.gov (United States)

    Höhener, Patrick; Yu, Xianjing

    2012-03-15

    Linear free energy relationships (LFERs) were established which relate equilibrium vapor-liquid isotope effects to stable carbon and hydrogen isotope enrichment factors for equilibrium sorption to geosorbents. The LFERs were established for normal, cyclic or branched alkanes, monoaromatic hydrocarbons, and chloroethenes. These LFERs predict that isotopic light compounds sorb more strongly than their heavy counterparts. Defining fractionation as in classical literature by "heavy divided by light", carbon enrichment factors for equilibrium sorption were derived which ranged from -0.13±0.04‰ (benzene) to -0.52±0.19‰ (trichloroethene at 5-15 °C). Hydrogen enrichment factors for sorption of 14 different compounds were between -2.4 and -9.2‰. For perdeuterated hydrocarbons the predicted enrichment factors ranged from -19±5.4‰ (benzene) to -64±30‰ (cyclohexane). Equilibrium sorption experiments with a soil and activated carbon as sorbents were performed in the laboratory for perdeuterocyclohexane and perdeuterotoluene. The measured D/H enrichments agreed with the LFER prediction for both compounds and both sorbents within the uncertainty estimate of the prediction. The results of this work suggest that equilibrium sorption does create only very small isotope shifts for (13)C in groundwater pollutants in aquifers. It is also suggested that deuterium shifts are expected to be higher, especially for strongly sorbing pollutants. Copyright © 2011 Elsevier B.V. All rights reserved.

  1. What is the Role of the Transition State in Soret and Chemical Diffusion Induced Isotopic Fractionation?

    Science.gov (United States)

    Dominguez, G.

    2013-12-01

    For over six decades, Urey's (1) statistical mechanical model of isotopic fractionation based on partition functions with quantized energy levels have enjoyed enormous success in quantitatively explaining equilibrium isotopic fractionation in a wide variety of geochemical systems For example, the interpretation of oxygen isotopic variations in carbonate systems (e.g. foraminiferas), in terms of partition functions with quantized energy levels, forms the basis for paleothermometry (2). Recent observations of isotopic fractionation from chemical and thermal (Soret) diffusion (3-7) appear to challenge our theoretical understanding of mass-transport and isotopic fractionation (8, 9). For example, a recently proposed quantum mechanical model of Soret diffusion, which correctly predicts the isotopic fractionation in thermal gradients for isotopes of Mg, Ca, Fe, Si, and possibly oxygen, was critiqued as being unphysical. First, it was argued that the zero point energies needed to explain the magnitude of isotopic fractionation in basalt melts were unrealistically high based on infrared spectra of these melts. Second, it was argued that the chemical diffusion isotopic fractionation (beta) factors expected from these zero-point energies were also unphysical (10). A recently proposed collision-momentum transfer model partially explains observed fractionation factors, although it fails miserably (by a factor of 3) to account for the isotopic fractionation of Mg isotopes (11). In this presentation, I will review recent observations and models of isotopic fractionation in geochemical melts with thermal gradients and expand upon previous work (8, 12) to show how transition state theory can simultaneously explain mass-transport induced isotopic fractionation, including kinetic, equilibrium, and Soret isotopic fractionation. I show this by providing a few example calculations of the kinetic fractionation factors (a.k.a. beta factors) expected in chemical diffusion as well as

  2. Selected scientific topics of the 11th International Isotope Symposium on the Synthesis and Applications of Isotopes and Isotopically Labeled Compounds.

    Science.gov (United States)

    Atzrodt, Jens; Derdau, Volker

    2013-01-01

    This micro-review describes hot topics and new trends in isotope science discussed at the 11th International Isotope Symposium on the Synthesis and Applications of Isotopes and Isotopically Labeled Compounds from a personal perspective. Copyright © 2013 John Wiley & Sons, Ltd.

  3. ISOTOPIC EFFECTS IN PARTIALLY DEUTERATED PIEZOELECTRIC CRYSTALS OF ROCHELLE SALT

    Directory of Open Access Journals (Sweden)

    R.R.Levitskii

    2004-01-01

    Full Text Available We develop a theory for dielectric, piezoelectric, and elastic properties of partially deuterated (quenched disorder crystals of Rochelle salt with taking into account the piezoelectric coupling. Results of numerical calculations are presented for a completely deuterated Rochelle salt and compared with available experimental data. Isotopic effect is explored within the mean crystal approximation, as well as within the developed theory using different trial sets of the fitting parameters. Theory predictions are given for the temperature and composition dependences of the calculated characteristics for partially deuterated crystals.

  4. On the origin and evolution of isotopes of carbon, nitrogen, and oxygen

    Science.gov (United States)

    Dearborn, D.; Schramm, D. N.; Tinsley, B. M.

    1978-01-01

    Calculations of CNO processing in stellar envelopes, based on theoretical nucleosynthesis rather than empirical abundances in evolving stars, are presented and used in two models for the chemical evolution of the solar neighborhood. Seven stable isotopes are considered: C-12, C-13, N-14, N-15, O-16, O-17, and O-18. The two models ('infall' and 'initial-burst') represent extremes of types consistent with general constraints and include theoretical estimates of other nucleosynthesis sites and yields for CNO isotopes. The results obtained are found to predict that all CNO isotopes are produced mainly by stars with lifetimes much less than the age of the Galaxy (even at the present time when low-mass stars have the greatest death rate), so that isotopic ratios evolve very slowly after the first few billion years. Consequences of these slow changes are that the isotopic ratios cannot be employed to test between alternative hypotheses and that galactic evolution does not seem to be able to account for the apparent difference between the C-13/C-12 ratio in the solar system and in molecular clouds. The predicted envelope processing is shown to lead to approximately the solar-system values for the C-13/C-12 and O-17/O-16 abundance ratios but to a N-14/C-12 ratio that is too small by at least a factor of 2.

  5. Evaluating O, C, and N isotopes in human hair as a forensic tool to reconstruct travel

    Science.gov (United States)

    Ehleringer, Jim; Chesson, Lesley; Cerling, Thure; Valenzuela, Luciano

    2014-05-01

    Oxygen isotope ratios in the proteins of human scalp hair have been proposed and modeled as a tool for reconstructing the movements of humans and evaluating the likelihood that an individual is a resident or non-resident of a particular geographic region. Carbon and nitrogen isotope ratios reflect dietary input and complement oxygen isotope data interpretation when it is necessary to distinguish potential location overlap among continents. The combination of a time sequence analysis in hair segments and spatial models that describe predicted geographic variation in hair isotope values represents a potentially powerful tool for forensic investigations. The applications of this technique have thus far been to provide assistance to law enforcement with information on the predicted geographical travel histories of unidentified murder victims. Here we review multiple homicide cases from the USA where stable isotope analysis of hair has been applied and for which we now know the travel histories of the murder victims. Here we provide information on the robustness of the original data sets used to test these models by evaluating the travel histories of randomly collected hair discarded in Utah barbershops.

  6. Unexpected hydrogen isotope variation in oceanic pelagic seabirds

    Science.gov (United States)

    Ostrom, Peggy H.; Wiley, Anne E.; Rossman, Sam; Stricker, Craig A.; James, Helen F.

    2014-01-01

    Hydrogen isotopes have significantly enhanced our understanding of the biogeography of migratory animals. The basis for this methodology lies in predictable, continental patterns of precipitation δD values that are often reflected in an organism's tissues. δD variation is not expected for oceanic pelagic organisms whose dietary hydrogen (water and organic hydrogen in prey) is transferred up the food web from an isotopically homogeneous water source. We report a 142% range in the δD values of flight feathers from the Hawaiian petrel (Pterodroma sandwichensis), an oceanic pelagic North Pacific species, and inquire about the source of that variation. We show δD variation between and within four other oceanic pelagic species: Newell's shearwater (Puffinus auricularis newellii), Black-footed albatross (Phoebastria nigripes), Laysan albatross (Phoebastria immutabilis) and Buller's shearwater (Puffinus bulleri). The similarity between muscle δD values of hatch-year Hawaiian petrels and their prey suggests that trophic fractionation does not influence δD values of muscle. We hypothesize that isotopic discrimination is associated with water loss during salt excretion through salt glands. Salt load differs between seabirds that consume isosmotic squid and crustaceans and those that feed on hyposmotic teleost fish. In support of the salt gland hypothesis, we show an inverse relationship between δD and percent teleost fish in diet for three seabird species. Our results demonstrate the utility of δD in the study of oceanic consumers, while also contributing to a better understanding of δD systematics, the basis for one of the most commonly utilized isotope tools in avian ecology.

  7. physico-chemical and stable isotopes

    African Journals Online (AJOL)

    This paper details the mineralogical, chemical and stable isotope abundances of calcrete in the Letlhakeng fossil valley. The stable isotope abundances (O and C) of calcretes yielded some values which were tested against the nature of the calcretes – pedogenic or groundwater type. The Kgalagadi (Kalahari) is a vast ...

  8. Advanced Mass Spectrometers for Hydrogen Isotope Analyses

    Energy Technology Data Exchange (ETDEWEB)

    Chastagner, P.

    2001-08-01

    This report is a summary of the results of a joint Savannah River Laboratory (SRL) - Savannah River Plant (SRP) ''Hydrogen Isotope Mass Spectrometer Evaluation Program''. The program was undertaken to evaluate two prototype hydrogen isotope mass spectrometers and obtain sufficient data to permit SRP personnel to specify the mass spectrometers to replace obsolete instruments.

  9. Dual Carbon and Nitrogen Isotope Analysis

    African Journals Online (AJOL)

    According to Hemminga & Mateo. (1996), values of carbon and nitrogen isotope ratios vary considerably between seagrass species. It might also be expected that the remaining seagrass species could have some influence on the shrimp carbon signal. Isotopic evidence for mangroves being a carbon source for shrimps ...

  10. Isotopic niches support the resource breadth hypothesis.

    Science.gov (United States)

    Rader, Jonathan A; Newsome, Seth D; Sabat, Pablo; Chesser, R Terry; Dillon, Michael E; Martínez Del Rio, Carlos

    2017-03-01

    Because a broad spectrum of resource use allows species to persist in a wide range of habitat types, and thus permits them to occupy large geographical areas, and because broadly distributed species have access to more diverse resource bases, the resource breadth hypothesis posits that the diversity of resources used by organisms should be positively related with the extent of their geographic ranges. We investigated isotopic niche width in a small radiation of South American birds in the genus Cinclodes. We analysed feathers of 12 species of Cinclodes to test the isotopic version of the resource breadth hypothesis and to examine the correlation between isotopic niche breadth and morphology. We found a positive correlation between the widths of hydrogen and oxygen isotopic niches (which estimate breadth of elevational range) and widths of the carbon and nitrogen isotopic niches (which estimates the diversity of resources consumed, and hence of habitats used). We also found a positive correlation between broad isotopic niches and wing morphology. Our study not only supports the resource breadth hypothesis but it also highlights the usefulness of stable isotope analyses as tools in the exploration of ecological niches. It is an example of a macroecological application of stable isotopes. It also illustrates the importance of scientific collections in ecological studies. © 2016 The Authors. Journal of Animal Ecology © 2016 British Ecological Society.

  11. Isotopic niches support the resource breadth hypothesis

    Science.gov (United States)

    Rader, Jonathan A.; Newsome, Seth D.; Sabat, Pablo; Chesser, R. Terry; Dillon, Michael E.; Martinez del Rio, Carlos

    2017-01-01

    Because a broad spectrum of resource use allows species to persist in a wide range of habitat types, and thus permits them to occupy large geographical areas, and because broadly distributed species have access to more diverse resource bases, the resource breadth hypothesis posits that the diversity of resources used by organisms should be positively related with the extent of their geographic ranges.We investigated isotopic niche width in a small radiation of South American birds in the genus Cinclodes. We analysed feathers of 12 species of Cinclodes to test the isotopic version of the resource breadth hypothesis and to examine the correlation between isotopic niche breadth and morphology.We found a positive correlation between the widths of hydrogen and oxygen isotopic niches (which estimate breadth of elevational range) and widths of the carbon and nitrogen isotopic niches (which estimates the diversity of resources consumed, and hence of habitats used). We also found a positive correlation between broad isotopic niches and wing morphology.Our study not only supports the resource breadth hypothesis but it also highlights the usefulness of stable isotope analyses as tools in the exploration of ecological niches. It is an example of a macroecological application of stable isotopes. It also illustrates the importance of scientific collections in ecological studies.

  12. Atomic lithium vapor laser isotope separation

    CERN Document Server

    Olivares, I E

    2002-01-01

    An atomic vapor laser isotope separation in lithium was performed using tunable diode lasers. The method permits also the separation of the isotopes between the sup 6 LiD sub 2 and the sup 7 LiD sub 1 lines using a self-made mass separator which includes a magnetic sector and an ion beam designed for lithium. (Author)

  13. The isotopic dipole moment of HDO

    Energy Technology Data Exchange (ETDEWEB)

    Assafrao, Denise; Mohallem, Jose R [Laboratorio de Atomos e Moleculas Especiais, Departamento de Fisica, ICEx, Universidade Federal de Minas Gerais, CP 702, 30123-970, Belo Horizonte, MG (Brazil)

    2007-03-14

    An adiabatic variational approximation is used to study the monodeuterated water molecule, HDO, accounting for the isotopic effect. The isotopic dipole moment, pointing from D to H, is then calculated for the first time, yielding (1.5 {+-} 0.1) x 10{sup -3} Debye, being helpful in the interpretation of experiments. (fast track communication)

  14. Environmental isotopes investigation in groundwater of Challaghatta ...

    African Journals Online (AJOL)

    Radiogenic isotopes (3H and 14C) and stable isotope (18O) together with TDS, EC and salinity of water were used to discriminate qualitative and quantitative groundwater age, probable recharge time, flow respectively in groundwater of Challaghatta valley, Bangalore. The variations between TDS and EC values of sewage ...

  15. Isotope Program Report June FY2016

    Energy Technology Data Exchange (ETDEWEB)

    Lewis, Jr, Benjamin E. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Egle, Brian [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2016-09-01

    Isotope Program Monthly Highlights are briefly described. These include data on isotopes shipped, updates on equipment fabrication and testing, a potential new approach for nondestructive measurement of the amount of Cf-252 deposited on a surface, and efforts to recover and purify uranium-234 obtained from old PuBe sources.

  16. Use of Isotopes for Studying Reaction Mechanisms

    Indian Academy of Sciences (India)

    Home; Journals; Resonance – Journal of Science Education; Volume 2; Issue 8. Use of Isotopes for Studying Reaction Mechanisms-Secondary Kinetic Isotope Effect. Uday Maitra J Chandrasekhar. Series Article Volume 2 Issue 8 August 1997 pp 18-25 ...

  17. Tracing thallium contamination in soils using isotopes

    Science.gov (United States)

    Vaněk, Aleš; Grösslová, Zuzana; Mihaljevič, Martin; Ettler, Vojtěch; Trubač, Jakub; Teper, Leslaw; Cabala, Jerzy; Rohovec, Jan; Penížek, Vít; Zádorová, Tereza; Pavlů, Lenka; Holubík, Ondřej; Drábek, Ondřej; Němeček, Karel; Houška, Jakub; Ash, Christopher

    2017-04-01

    We report the thallium (Tl) isotope record in moderately contaminated soils, which have been historically affected by emissions from coal-fired power plants. Our findings clearly demonstrate that Tl of anthropogenic (high-temperature) origin with light isotope composition was deposited onto the studied soils, where heavier Tl (ɛ205Tl -1) naturally occurs. The results show a positive linear relationship (R2 = 0.71) between 1/Tl and the isotope record, as determined for all the soils and bedrocks, also indicative of binary Tl mixing between two dominant reservoirs. We also identified significant Tl isotope variations within the products from coal combustion and thermo-desorption experiments with local Tl-rich coal pyrite. Bottom ash exhibited the heaviest Tl isotope composition (ɛ205Tl 0), followed by fly ash (ɛ205Tl between -2.5 and -2.8) and volatile Tl fractions (ɛ205Tl between -6.2 and -10.3), suggesting partial Tl isotope fractionations. Despite the evident role of soil processes in the isotope redistribution, we demonstrate that Tl contamination can be traced in soils, and propose that the isotope data represent a possible tool to aid our understanding of post-depositional Tl dynamics in surface environments for the future. This research was supported by the Czech Science Foundation (grant no. 14-01866S and 17-03211S).

  18. Correction of MS data for naturally occurring isotopes in isotope labelling experiments.

    Science.gov (United States)

    Millard, Pierre; Letisse, Fabien; Sokol, Serguei; Portais, Jean-Charles

    2014-01-01

    Mass spectrometry (MS) in combination with isotope labelling experiments is widely used for investigations of metabolism and other biological processes. Quantitative applications-e.g., (13)C metabolic flux analysis-require correction of raw MS data (isotopic clusters) for the contribution of all naturally abundant isotopes. This chapter describes how to perform such correction using the software IsoCor. This flexible, user-friendly software can be used to exploit any isotopic tracer, from well-known ((13)C, (15)N, (18)O, etc.) to unusual ((57)Fe, (77)Se, etc.) isotopes. It also provides options-e.g., correction for the isotopic purity of the tracer-to improve the accuracy of quantitative isotopic studies, and allows automated correction of large datasets that can be collected with modern MS methods.

  19. NOx cycle and the tropospheric ozone isotope anomaly: an experimental investigation

    Science.gov (United States)

    Michalski, G.; Bhattacharya, S. K.; Girsch, G.

    2014-05-01

    The oxygen isotope composition of nitrogen oxides (NOx) in the atmosphere is a useful tool for understanding the oxidation of NOx into nitric acid / nitrate in the atmosphere. A set of experiments was conducted to examine change in isotopic composition of NOx due to NOx-O2-O3 photochemical cycling. At low NOx / O2 mixing ratios, NOx became progressively and nearly equally enriched in 17O and 18O over time until it reached a steady state with Δ17O values of 39.3 ± 1.9‰ and δ18O values of 84.2 ± 4‰, relative to the isotopic composition of the initial O2 gas. As the mixing ratios were increased, the isotopic enrichments were suppressed by isotopic exchange between O atoms, O2, and NOx. A kinetic model was developed to simulate the observed data and it showed that the isotope effects occurring during O3 formation play a dominant role in controlling NOx isotopes and, in addition, secondary kinetic isotope effects or isotope exchange reactions are also important during NOx cycling. The data and model were consistent with previous studies which showed that the NO + O3 reactions occur mainly via the transfer of the terminal atoms of O3. The model predicts that under tropospheric concentrations of NOx and O3, the timescale of NOx-O3 isotopic equilibrium ranges from hours (for ppbv NOx / O2 mixing ratios) to days (for pptv mixing ratios) and yields steady state Δ17O and δ18O values of 45‰ and 117‰ respectively (relative to Vienna Standard Mean Ocean Water (VSMOW)) in both cases. Under atmospheric conditions when O3 has high concentrations, the equilibrium between NOx and O3 should occur rapidly (h) but this equilibrium cannot be reached during polar winters and/or nights if the NOx conversion to HNO3 is faster. The experimentally derived rate coefficients can be used to model the major NOx-O3 isotopologue reactions at various pressures and in isotope modeling of tropospheric nitrate.

  20. The Influence of Kinetic Growth Factors on the Clumped Isotope Composition of Calcite

    Science.gov (United States)

    Hunt, J. D.; Watkins, J. M.; Tripati, A.; Ryerson, F. J.; DePaolo, D. J.

    2014-12-01

    Clumped isotope paleothermometry is based on the association of 13C and 18O within carbonate minerals. Although the influence of temperature on equilibrium 13C-18O bond ordering has been studied, recent oxygen isotope studies of inorganic calcite demonstrate that calcite grown in laboratory experiments and in many natural settings does not form in equilibrium with water. It is therefore likely that the carbon and clumped isotope composition of these calcite crystals are not representative of true thermodynamic equilibrium. To isolate kinetic clumped isotope effects that arise at the mineral-solution interface, clumped isotopic equilibrium of DIC species must be maintained. This can be accomplished by dissolving the enzyme carbonic anhydrase (CA) into the solution, thereby reducing the time required for isotopic equilibration of DIC species by approximately two orders of magnitude between pH 7.7 and 9.3. We conduct calcite growth experiments aimed specifically at measuring the pH-dependence of kinetic clumped isotope effects during non-equilibrium precipitation of calcite. We precipitated calcite from aqueous solution at a constant pH and controlled supersaturation over the pH range 7.7-9.3 in the presence of CA. For each experiment, a gas mixture of N2 and CO2 is bubbled through a beaker of solution without seed crystals. As CO2 from the gas dissolves into solution, calcite crystals grow on the beaker walls. The pH of the solution is maintained by use of an autotitrator with NaOH as the titrant. We control the temperature, pH, the pCO2 of the gas inflow, and the gas inflow rate, and monitor the total alkalinity, the pCO2 of the gas outflow, and the amount of NaOH added. A constant crystal growth rate of ~1.6 mmol/m2/hr is maintained over all experiments. Results from these experiments are compared to predictions from a recently-developed isotopic ion-by-ion growth model of calcite. The model describes the rate, temperature and pH dependence of oxygen isotope uptake

  1. Second international conference on isotopes. Conference proceedings

    Energy Technology Data Exchange (ETDEWEB)

    Hardy, C.J. [ed.

    1997-10-01

    The Second International Conference on Isotopes (2ICI) was hosted by the Australian Nuclear Association in Sydney, NSW, Australia. The Theme of the Second Conference: Isotopes for Industry, Health and a Better Environment recognizes that isotopes have been used in these fields successfully for many years and offer prospects for increasing use in the future. The worldwide interest in the use of research reactors and accelerators and in applications of stable and radioactive isotopes, isotopic techniques and radiation in industry, agriculture, medicine, environmental studies and research in general, was considered. Other radiation issues including radiation protection and safety were also addressed. International and national overviews and subject reviews invited from leading experts were included to introduce the program of technical sessions. The invited papers were supported by contributions accepted from participants for oral and poster presentation. A Technical Exhibition was held in association with the Conference. This volume contains the full text or extended abstracts of papers number 61- to number 114

  2. Selected Isotopes for Optimized Fuel Assembly Tags

    Energy Technology Data Exchange (ETDEWEB)

    Gerlach, David C.; Mitchell, Mark R.; Reid, Bruce D.; Gesh, Christopher J.; Hurley, David E.

    2008-10-01

    In support of our ongoing signatures project we present information on 3 isotopes selected for possible application in optimized tags that could be applied to fuel assemblies to provide an objective measure of burnup. 1. Important factors for an optimized tag are compatibility with the reactor environment (corrosion resistance), low radioactive activation, at least 2 stable isotopes, moderate neutron absorption cross-section, which gives significant changes in isotope ratios over typical fuel assembly irradiation levels, and ease of measurement in the SIMS machine 2. From the candidate isotopes presented in the 3rd FY 08 Quarterly Report, the most promising appear to be Titanium, Hafnium, and Platinum. The other candidate isotopes (Iron, Tungsten, exhibited inadequate corrosion resistance and/or had neutron capture cross-sections either too high or too low for the burnup range of interest.

  3. FRIGA, a new approach to identify isotopes and hypernuclei in n -body transport models

    Science.gov (United States)

    Le Fèvre, A.; Leifels, Y.; Aichelin, J.; Hartnack, Ch.; Kireyev, V.; Bratkovskaya, E.

    2017-11-01

    We present a new algorithm to identify fragments in computer simulations of relativistic heavy-ion collisions. It is based on the simulated annealing technique and can be applied to n -body transport models like the Quantum Molecular Dynamics. This new approach is able to predict isotope yields as well as hypernucleus production. In order to illustrate its predicting power, we confront this new method to experimental data, and show the sensitivity on the parameters which govern the cluster formation.

  4. Biomarker and molecular isotope approaches to deconvolve the terrestrial carbon isotope record: modern and Eocene calibrations

    Science.gov (United States)

    Diefendorf, A. F.; Freeman, K. H.; Wing, S.; Currano, E. D.

    2010-12-01

    Climate, biome, and plant community are important predictors of carbon isotope patterns recorded in leaves and leaf waxes. However, signatures recorded by terrestrial organic carbon and lipids that have mixed floral sources (e.g., n-alkanes) potentially reflect both plant community changes and climate. More taxonomically specific proxies for plants (i.e., di- and tri-terpenoids for conifers and angiosperms, respectively), can help to resolve the relative influences of changing community and climate, provided differences in biomarker production and lipid biosynthetic fractionation among plants can be better constrained. We present biomarker abundance and carbon isotope values for lipids from leaves, branches and bark of 44 tree species, representing 21 families including deciduous and evergreen conifers and angiosperms. n-alkane production differs greatly between conifer and angiosperm leaves. Both deciduous and evergreen angiosperms make significantly more n-alkanes than conifers, with n-alkanes not detected in over half of the conifers in our study. Terpenoid abundances scale strongly with leaf habit: evergreen species have significantly higher abundances. We combine these relative differences in lipid production with published estimates of fluxes for leaf litter from conifer and angiosperm trees to develop a new proxy approach for estimating paleo plant community inputs to ancient soils and sediments. To test our modern calibration results, we have evaluated n-alkanes and terpenoids from laterally extensive (~18 km) carbonaceous shales and mudstones in Eocene sediments (52.6 Ma) at Fifteenmile Creek in the Bighorn Basin (WY, USA). Our terpenoid-based proxy predicts on average a 40% conifer community, which is remarkably close in agreement with a fossil-based estimate of 36%. n-alkane carbon isotope fractionation (leaf-lipid) differs among plant types, with conifer n-alkanes about 2-3‰ 13C enriched relative to those in angiosperms. Since conifer leaves are

  5. Manus Water Isotope Investigation Field Campaign Report

    Energy Technology Data Exchange (ETDEWEB)

    Conroy, Jessica L [University of Illinois, Urbana-Champaign; Cobb, Kim M [Georgia Institute of Technology; Noone, David [University of Colorado, Boulder

    2016-03-01

    The objective of this field campaign was to investigate climatic controls on the stable isotopic composition of water vapor, precipitation, and seawater in the western tropical Pacific. Simultaneous measurements of the stable isotopic composition of vapor and precipitation from April 28 to May 8, 2013, at the Manus Tropical Western Pacific Atmospheric Radiation Measurement site, provided several key insights into the nature of the climate signal archived in precipitation and vapor isotope ratios. We observed a large shift from lower to higher isotopic values in vapor and precipitation because of the passage of a mesoscale convective system west of the site and a transition from a regional stormy period into a more quiescent period. During the quiescent period, the stable isotopic composition of vapor and precipitation indicated the predominance of oceanic evaporation in determining the isotopic composition of boundary-layer vapor and local precipitation. There was not a consistent relationship between intra-event precipitation amount at the site and the stable isotopic composition of precipitation, thus challenging simplified assumptions about the isotopic “amount effect” in the tropics on the time scale of individual storms. However, some storms did show an amount effect, and deuterium excess values in precipitation had a significant relationship with several meteorological variables, including precipitation, temperature, relative humidity, and cloud base height across all measured storms. The direction of these relationships points to condensation controls on precipitation deuterium excess values on intra-event time scales. The relationship between simultaneous measurements of vapor and precipitation isotope ratios during precipitation events indicates the ratio of precipitation-to-vapor isotope ratios can diagnose precipitation originating from a vapor source unique from boundary-layer vapor and rain re-evaporation.

  6. Microscopic Observation of Kinetic Molecular Sieving of Hydrogen Isotopes in a Nanoporous Material

    Science.gov (United States)

    Nguyen, T. X.; Jobic, H.; Bhatia, S. K.

    2010-08-01

    We report quasielastic neutron scattering studies of H2-D2 diffusion in a carbon molecular sieve, demonstrating remarkable quantum effects, with the heavier isotope diffusing faster below 100 K, confirming our recent predictions. Our transition state theory and molecular dynamics calculations show that while it is critical for this effect to have narrow windows of size comparable to the de Broglie wavelength, high flux requires that the energy barrier be reduced through small cages. Such materials will enable novel processes for kinetic molecular sieving of hydrogen isotopes.

  7. Production of neutron-rich isotopes by one- and two-step processes in ISOL targets

    CERN Document Server

    Portillo, M; Gomes, I; Panteleev, V N; Fedorov, D V; Barzakh, A E; Beznosjuk, V I; Moroz, F V; Orlov, S Y; Volkov, Y M

    2002-01-01

    The results are presented for an experiment that compares the difference between a one- and two-step reaction setup using 1 GeV protons. The rates of production from an on-line isotope separator target containing UCx are measured for isotopes in the neutron mass region of Rb and Cs. Some details about the measured results and predictions by the Monte Carlo models are discussed. The effects of the delayed release on the extracted efficiency are generalized using analytical models for application to a wide range of nuclear decay lifetimes.

  8. A carbon isotope mass balance for an anoxic marine sediment: Isotopic signatures of diagenesis

    Science.gov (United States)

    Boehme, Susan E.

    1993-01-01

    A carbon isotope mass balance was determined for the sediments of Cape Lookout Bight, NC to constrain the carbon budgets published previously. The diffusive, ebullitive and burial fluxes of sigma CO2 and CH4, as well as the carbon isotope signatures of these fluxes, were measured. The flux-weighted isotopic signature of the remineralized carbon (-18.9 plus or minus 2.7 per mil) agreed with the isotopic composition of the remineralized organic carbon determined from the particulate organic carbon (POC) delta(C-13) profiles (-19.2 plus or minus 0.2), verifying the flux and isotopic signature estimates. The measured delta(C-13) values of the sigma CO2 and CH4 diffusive fluxes were significantly different from those calculated from porewater gradients. The differences appear to be influenced by methane oxidation at the sediment-water interface, although other potential processes cannot be excluded. The isotope mass balance provides important information concerning the locations of potential diagenetic isotope effects. Specifically, the absence of downcore change in the delta(C-13) value of the POC fraction and the identical isotopic composition of the POC and the products of remineralization indicate that no isotopic fractionation is expressed during the initial breakdown of the POC, despite its isotopically heterogeneous composition.

  9. Measurement of isotope abundance variations in nature by gravimetric spiking isotope dilution analysis (GS-IDA).

    Science.gov (United States)

    Chew, Gina; Walczyk, Thomas

    2013-04-02

    Subtle variations in the isotopic composition of elements carry unique information about physical and chemical processes in nature and are now exploited widely in diverse areas of research. Reliable measurement of natural isotope abundance variations is among the biggest challenges in inorganic mass spectrometry as they are highly sensitive to methodological bias. For decades, double spiking of the sample with a mix of two stable isotopes has been considered the reference technique for measuring such variations both by multicollector-inductively coupled plasma mass spectrometry (MC-ICPMS) and multicollector-thermal ionization mass spectrometry (MC-TIMS). However, this technique can only be applied to elements having at least four stable isotopes. Here we present a novel approach that requires measurement of three isotope signals only and which is more robust than the conventional double spiking technique. This became possible by gravimetric mixing of the sample with an isotopic spike in different proportions and by applying principles of isotope dilution for data analysis (GS-IDA). The potential and principle use of the technique is demonstrated for Mg in human urine using MC-TIMS for isotopic analysis. Mg is an element inaccessible to double spiking methods as it consists of three stable isotopes only and shows great potential for metabolically induced isotope effects waiting to be explored.

  10. Nitrogen isotope fractionation during archaeal ammonia oxidation: Coupled estimates from isotopic measurements of ammonium and nitrite

    Science.gov (United States)

    Mooshammer, Maria; Stieglmeier, Michaela; Bayer, Barbara; Jochum, Lara; Melcher, Michael; Wanek, Wolfgang

    2014-05-01

    Ammonia-oxidizing archaea (AOA) are ubiquitous in marine and terrestrial environments and knowledge about the nitrogen (N) isotope effect associated with their ammonia oxidation activity will allow a better understanding of natural abundance isotope ratios, and therefore N transformation processes, in the environment. Here we examine the kinetic isotope effect for ammonia oxidation in a pure soil AOA culture (Ca. Nitrososphaera viennensis) and a marine AOA enrichment culture. We estimated the isotope effect from both isotopic signatures of ammonium and nitrite over the course of ammonia oxidation. Estimates of the isotope effect based on the change in the isotopic signature of ammonium give valuable insight, because these estimates are not subject to the same concerns (e.g., accumulation of an intermediate) as estimates based on isotopic measurements of nitrite. Our results show that both the pure soil AOA culture and a marine AOA enrichment culture have similar but substantial isotope effect during ammonia consumption (31-34 per mill; based on ammonium) and nitrite production (43-45 per mill; based on nitrite). The 15N fractionation factors of both cultures tested fell in the upper range of the reported isotope effects for archaeal and bacterial ammonia oxidation (10-41 per mill) or were even higher than those. The isotope fractionation for nitrite production was significantly larger than for ammonium consumption, indicating that (1) some intermediate (e.g., hydroxylamine) of ammonia oxidation accumulates, allowing for a second 15N fractionation step to be expressed, (2) a fraction of ammonia oxidized is lost via gaseous N forms (e.g., NO or N2O), which is 15N-enriched or (3) a fraction of ammonium is assimilated into AOA biomass, biomass becoming 15N-enriched. The significance of these mechanisms will be explored in more detail for the soil AOA culture, based on isotope modeling and isotopic measurements of biomass and N2O.

  11. Quantification of Labile Soil Mercury by Stable Isotope Dilution Techniques

    Science.gov (United States)

    Shetaya, Waleed; Huang, Jen-How; Osterwalder, Stefan; Alewell, Christine

    2016-04-01

    Mercury (Hg) is a toxic element that can cause severe health problems to humans. Mercury is emitted to the atmosphere from both natural and anthropogenic sources and can be transported over long distances before it is deposited to aquatic and terrestrial environments. Aside from accumulation in soil solid phases, Hg deposited in soils may migrate to surface- and ground-water or enter the food chain, depending on its lability. There are many operationally-defined extraction methods proposed to quantify soil labile metals. However, these methods are by definition prone to inaccuracies such as non-selectivity, underestimation or overestimation of the labile metal pool. The isotopic dilution technique (ID) is currently the most promising method for discrimination between labile and non-labile metal fractions in soil with a minimum disturbance to soil-solid phases. ID assesses the reactive metal pool in soil by defining the fraction of metal both in solid and solution phases that is isotopically-exchangeable known as the 'E-value'. The 'E-value' represents the metal fraction in a dynamic equilibrium with the solution phase and is potentially accessible to plants. This is carried out by addition of an enriched metal isotope to soil suspensions and quantifying the fraction of metal that is able to freely exchange with the added isotope by measuring the equilibrium isotopic ratio by ICP-MS. E-value (mg kg-1) is then calculated as follows: E-Value = (Msoil/ W) (CspikeVspike/ Mspike) (Iso1IAspike -Iso2IAspikeRss / Iso2IAsoil Rss - Iso1IAsoil) where M is the average atomic mass of the metal in the soil or the spike, W is the mass of soil (kg), Cspike is the concentration of the metal in the spike (mg L-1), Vspike is the volume of spike (L), IA is isotopic abundance, and Rss is the equilibrium ratio of isotopic abundances (Iso1:Iso2). Isotopic dilution has been successfully applied to determine E-values for several elements. However, to our knowledge, this method has not yet

  12. Isotopic geochemistry of Panama rivers

    Science.gov (United States)

    Harmon, Russell S.; Worner, Gerhard; Pribil, Michael; Kern, Zoltan; Forizs, Istvan; Lyons, W. Berry; Gardner, Christopher B.; Goldsmith, Steven T.

    2015-01-01

    River water samples collected from 78 watersheds rivers along a 500-km transect across a Late Cretaceous-Tertiary andesitic volcanic arc terrane in west-central Panama provide a synoptic overview of riverine geochemistry, chemical denudation, and CO2 consumption in the tropics. D/H and 18O/16O relationships indicate that bedrock dissolution of andesitic arc crust in Panama is driven by water-rock interaction with meteoric precipitation as it passes through the critical zone, with no evidence of a geothermal or hydrothermal input. Sr-isotope relationships suggest a geochemical evolution for Panama riverine waters that involves mixing of bedrock pore water with water having 87Sr/86Sr ratios between 0.7037-0.7043 and relatively high Sr-contents with waters of low Sr content that enriched in radiogenic Sr that are diluted by infiltrating rainfall to variable extents.

  13. Nuclear structure of light Ca and heavy Cr isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Buerger, A.

    2007-07-01

    In the present thesis, the shell structure in exotic nuclei has been investigated. The focus of the work was on finding new experimental data in neutron-rich Cr and proton-rich Ca isotopes. The investigation of light Ca isotopes concentrated on the nucleus {sup 36}Ca which was produced in a knockout reaction from a radioactive {sup 37}Ca beam. For {sup 36}Ca, the excitation energy of the first 2{sup +} state has been measured for the first time. Furthermore, momentum distributions were analyzed using a Monte-Carlo simulation of the knockout reaction. This analysis yielded the contributions of neutrons from individual orbitals to the total knockout cross section. In principle, these may be used to calculate spectroscopic factors, but such a calculation is hampered by difficulties of present knockout-reaction models in predicting precise single-particle cross sections. The measured branching ratio to the ground and excited states, on the other hand, is close to the predicted value. A remaining difference might be due to emission of protons which cannot be detected with the present experimental setup. Both the branching ratio and the large excitation energy are compatible with a large N=16 gap in {sup 36}Ca that leads to relatively pure configurations both in the ground state and the excited 2{sup +} state. As a by-product of the experiment, two excitation energies in the T=2 nuclei {sup 32}Ar and {sup 28}S have been confirmed, and two {gamma}-ray transitions have been observed for the first time in {sup 37}Ca. While the mirror energy differences in the T=2 pairs {sup 36}Ca-{sup 36}S, {sup 32}Ar-{sup 32}Si, and {sup 28}S-{sup 28}Mg can be reproduced in shell model calculations using a modified USD interaction, these modifications are not sufficient to explain the mirror energy differences for the pair {sup 37}Ca-{sup 37}Cl. In the heavy Cr isotopes, new experimental evidence for a sub-shell closure at N=32 was found in a measurement of B(E2) values using high

  14. Studies of control materials of isotope transformation

    Energy Technology Data Exchange (ETDEWEB)

    Noda, Tetsuji; Suzuki, Hiroshi; Araki, Hiroshi; Fujita, Mitsutane; Hirano, Toshiyuki; Abe, Fujio; Numazawa, Takenori [National Research Inst. for Metals, Tsukuba, Ibaraki (Japan)

    1999-02-01

    To control wavelength of laser, the physical properties of control materials of molecular excitation and isotope should be studied. We carried out isotopic enrichment, Si thin film growth, and preparation of boron isotope crystal and to make a calculation code of nuclear transmutation simulation. A gas circulation system for developing isotope laser was produced in order to control of molecular vibration excitation. We developed a single straight system of silicon isotope enrichment and silicon thin film preparation by infrared laser. When laser irradiated Si{sub 2}F{sub 6}, unreacted Si{sub 2}F{sub 6} contained 99.72% of {sup 28}Si at about 956 cm{sup -1} wavelength. When SiF{sub 4} or Si{sub 2}F{sub 6} with enriched isotope were directly decomposed by the plasma CVD method at about from 350 to 450degC, the yield of silicon crystal was about 28%. A homogeneous crystal with 10 mm diameter was obtained as the control material of boron isotope. The computer code for simulation of nuclear transmutation was improved to calculate the displacement damage, change of composition, induced radioactivity and decay heat. (S.Y.)

  15. Si isotope homogeneity of the solar nebula

    Energy Technology Data Exchange (ETDEWEB)

    Pringle, Emily A.; Savage, Paul S.; Moynier, Frédéric [Department of Earth and Planetary Sciences and McDonnell Center for the Space Sciences, Washington University in St. Louis, One Brookings Drive, St. Louis, MO 63130 (United States); Jackson, Matthew G. [Department of Earth Science, University of California, Santa Barbara, CA 93109 (United States); Barrat, Jean-Alix, E-mail: eapringle@wustl.edu, E-mail: savage@levee.wustl.edu, E-mail: pringle@ipgp.fr, E-mail: moynier@ipgp.fr, E-mail: jackson@geol.ucsb.edu, E-mail: Jean-Alix.Barrat@univ-brest.fr [Université Européenne de Bretagne, Université de Brest, CNRS UMR 6538 (Domaines Océaniques), I.U.E.M., Place Nicolas Copernic, F-29280 Plouzané Cedex (France)

    2013-12-20

    The presence or absence of variations in the mass-independent abundances of Si isotopes in bulk meteorites provides important clues concerning the evolution of the early solar system. No Si isotopic anomalies have been found within the level of analytical precision of 15 ppm in {sup 29}Si/{sup 28}Si across a wide range of inner solar system materials, including terrestrial basalts, chondrites, and achondrites. A possible exception is the angrites, which may exhibit small excesses of {sup 29}Si. However, the general absence of anomalies suggests that primitive meteorites and differentiated planetesimals formed in a reservoir that was isotopically homogenous with respect to Si. Furthermore, the lack of resolvable anomalies in the calcium-aluminum-rich inclusion measured here suggests that any nucleosynthetic anomalies in Si isotopes were erased through mixing in the solar nebula prior to the formation of refractory solids. The homogeneity exhibited by Si isotopes may have implications for the distribution of Mg isotopes in the solar nebula. Based on supernova nucleosynthetic yield calculations, the expected magnitude of heavy-isotope overabundance is larger for Si than for Mg, suggesting that any potential Mg heterogeneity, if present, exists below the 15 ppm level.

  16. Seafloor alteration, oxygen isotopes and climate

    Science.gov (United States)

    Kanzaki, Y.; Kump, L. R.; Kasting, J. F.

    2016-12-01

    Seafloor alteration can be related to climate in two ways: through storage of carbon dioxide as carbonates and indirectly through its influence on the oxygen isotopic composition of seawater. Low temperature alteration of the seafloor, or seafloor weathering, can store carbon dioxide as carbonates formed as the result of dissolution of cations from silicate rocks, and since this process is temperature dependent, can serve as a climate regulator. On the other hand, the oxygen isotopic composition of seawater is determined by the balance between low temperature crustal alteration (including continental weathering) and high temperature seafloor alteration, because the heavy isotope is depleted from and added to seawater in low and high temperature alteration, respectively. The oxygen isotopic composition of seawater is a parameter necessary to estimate surface temperature of the Earth from the oxygen isotopic composition of authigenic sedimentary rocks. Thus seafloor alteration is related to reconstruction of Earth's climate. We have developed a comprehensive model of seafloor alteration that captures both seafloor weathering and oxygen isotope exchange, and use it to reconcile observations of long-term stability in both climate and altered ocean crust δ18O with secular changes in the oxygen isotopic composition of marine sediments.

  17. Isotopic tracing of perchlorate in the environment

    Science.gov (United States)

    Sturchio, Neil C.; Böhlke, John Karl; Gu, Baohua; Hatzinger, Paul B.; Jackson, W. Andrew; Baskaran, Mark

    2012-01-01

    Isotopic measurements can be used for tracing the sources and behavior of environmental contaminants. Perchlorate (ClO 4 − ) has been detected widely in groundwater, soils, fertilizers, plants, milk, and human urine since 1997, when improved analytical methods for analyzing ClO 4 −concentration became available for routine use. Perchlorate ingestion poses a risk to human health because of its interference with thyroidal hormone production. Consequently, methods for isotopic analysis of ClO 4 − have been developed and applied to assist evaluation of the origin and migration of this common contaminant. Isotopic data are now available for stable isotopes of oxygen and chlorine, as well as 36Cl isotopic abundances, in ClO 4 − samples from a variety of natural and synthetic sources. These isotopic data provide a basis for distinguishing sources of ClO 4 − found in the environment, and for understanding the origin of natural ClO 4 − . In addition, the isotope effects of microbial ClO 4 − reduction have been measured in laboratory and field experiments, providing a tool for assessing ClO 4 − attenuation in the environment. Isotopic data have been used successfully in some areas for identifying major sources of ClO 4 − contamination in drinking water supplies. Questions about the origin and global biogeochemical cycle of natural ClO 4 − remain to be addressed; such work would benefit from the development of methods for preparation and isotopic analysis of ClO 4 − in samples with low concentrations and complex matrices.

  18. Intramolecular Isotopic Studies: Chemical Enhancements and Alternatives

    Science.gov (United States)

    Hayes, J. M.

    2016-12-01

    As mass spectroscopic and NMR-based methods now appropriately flourish, chemical techniques should not be forgotten. First, the methods developed by pioneering intramolecular analysts can be reapplied to new samples. Second, they can be extended. The synthesis of intramolecular isotopic standards is particularly important and straightforward. It requires only that a chemical reaction has no secondary products. An example is provided by the addition of carbon dioxide to a Grignard reagent. The reaction proceeds with an isotope effect. The isotopic composition of the carboxyl group in the acid which is produced is thus not equal to that of the starting carbon dioxide but the unconsumed CO2 can be recovered and analyzed. A simple titration can show that all the rest of the CO2 is in the product acid. The isotopic composition of the carboxyl group can then be calculated by difference. The product is an intramolecular isotopic standard, an organic molecule in which the isotopic composition of a specific carbon position is known accurately. Both analysts and reviewers can thus gain invaluable confidence in the accuracy of instrumental results. A second example: the haloform reaction quantitatively degrades methyl ketones, producing a carboxylic acid which can be decarboxylated to determine the isotopic composition of the parent carbonyl and a haloform (CHI3, for example) that can be combusted to determine the isotopic composition of the methyl group. Ketones thus analyzed can be combined with Grignard reagents to yield carbon skeletons in which the isotopic compositions of internal and terminal -CH2- and -CH3 groups are known accurately. In general, analysts accustomed to demanding quantitative reactions should remember the power of mass balances and recognize that many organic-chemical reactions, while not quantitative, lack side products and can be driven to the total consumption of at least one reactant.

  19. Ab initio calculation of the Zn isotope effect in phosphates, citrates, and malates and applications to plants and soil.

    Directory of Open Access Journals (Sweden)

    Toshiyuki Fujii

    Full Text Available Stable Zn isotopes are fractionated in roots and leaves of plants. Analyses demonstrate that the heavy Zn isotopes are enriched in the root system of plants with respect to shoots and leaves as well as the host soil, but the fractionation mechanisms remain unclear. Here we show that the origin of this isotope fractionation is due to a chemical isotope effect upon complexation by Zn malates and citrates in the aerial parts and by phosphates in the roots. We calculated the Zn isotope effect in aqueous citrates, malates, and phosphates by ab initio methods. For pH<5, the Zn isotopic compositions of the various parts of the plants are expected to be similar to those of groundwater. In the neutral to alkaline region, the calculations correctly predict that (66Zn is enriched over (64Zn in roots, which concentrate phosphates, with respect to leaves, which concentrate malates and citrates, by about one permil. It is proposed that Zn isotope fractionation represents a useful tracer of Zn availability and mobility in soils.

  20. Hafnium isotope stratigraphy of ferromanganese crusts

    Science.gov (United States)

    Lee, D.-C.; Halliday, A.N.; Hein, J.R.; Burton, K.W.; Christensen, J.N.; Gunther, D.

    1999-01-01

    A Cenozoic record of hafnium isotopic compositions of central Pacific deep water has been obtained from two ferromanganese crusts. The crusts are separated by more than 3000 kilometers but display similar secular variations. Significant fluctuations in hafnium isotopic composition occurred in the Eocene and Oligocene, possibly related to direct advection from the Indian and Atlantic oceans. Hafnium isotopic compositions have remained approximately uniform for the past 20 million years, probably reflecting increased isolation of the central Pacific. The mechanisms responsible for the increase in 87Sr/86Sr in seawater through the Cenozoic apparently had no effect on central Pacific deep-water hafnium.

  1. The Facility for Rare Isotope Beams

    Directory of Open Access Journals (Sweden)

    Wrede C.

    2015-01-01

    Full Text Available The Facility for Rare Isotope Beams (FRIB is a United States Department of Energy user facility currently under construction on the campus of Michigan State University. Based on a 400 kW, 200 MeV/u heavy-ion driver linac, FRIB will deliver high-quality fast, thermalized, and re-accelerated beams of rare isotopes with unprecedented intensities to a variety of experimental areas and equipment. New science opportunities at the frontiers of nuclear structure, nuclear astrophysics, fundamental symmetries, and societal applications will be enabled by this future world-leading rare-isotope beam facility.

  2. The Facility for Rare Isotope Beams

    Science.gov (United States)

    Wrede, C.

    2015-05-01

    The Facility for Rare Isotope Beams (FRIB) is a United States Department of Energy user facility currently under construction on the campus of Michigan State University. Based on a 400 kW, 200 MeV/u heavy-ion driver linac, FRIB will deliver high-quality fast, thermalized, and re-accelerated beams of rare isotopes with unprecedented intensities to a variety of experimental areas and equipment. New science opportunities at the frontiers of nuclear structure, nuclear astrophysics, fundamental symmetries, and societal applications will be enabled by this future world-leading rare-isotope beam facility.

  3. Titanium Isotopes Provide Clues to Lunar Origin

    Science.gov (United States)

    Taylor, G. J.

    2012-05-01

    The idea that the Moon formed as the result of the giant impact of a Mars-sized impactor with the still-growing Earth explains two central facts about the Earth-Moon system: its total angular momentum (Earth's spin and the Moon's orbital motion), and the sizes of the metallic cores of the Earth (large) and Moon (tiny). This gives cosmochemists some confidence in the hypothesis, but they would greatly appreciate additional compositional tests. One undisputed point is the identical abundance of the three oxygen isotopes in Earth and Moon. Junjun Zhang and colleagues at the University of Chicago (USA) and the University of Bern (Switzerland) have added another isotopic system to the cosmochemical testing tool kit, titanium isotopes. They find that the ratio of titanium-50 to titanium-47 is identical in Earth and Moon to within four parts per million. In contrast, other solar system materials, such as carbonaceous chondrites, vary by considerably more than this-- up to 150 times as much. The identical oxygen and titanium isotopic compositions in Earth and Moon are surprising in light of what we think we know about planet formation and formation of the Moon after a giant impact. The variations in oxygen and titanium isotopes among meteorite types suggest that it is unlikely that the Moon-forming giant impactor would have had the same isotopic composition as the Earth. Simulations show that the Moon ends up constructed mostly (40-75%) from the impactor materials. Thus, the Moon ought to have different isotopic composition than does Earth. The isotopes might have exchanged in the complicated, messy proto-lunar disk (as has been suggested for oxygen isotopes), making them the same. However, Zhang and colleagues suggest that this exchange is unlikely for a refractory element like titanium. Could the impact simulations be greatly overestimating the contributions from the impactor? Was the mixing of building-block materials throughout the inner solar system much less than

  4. Beneficial uses and production of isotopes

    CERN Document Server

    2001-01-01

    Isotopes, radioactive and stable, are used worldwide in various applications related to medical diagnosis or care, industry and scientific research. More than fifty countries have isotope production or separation facilities operated for domestic supply, and sometimes for international markets. This publication provides up-to-date information on the current status of, and trends in, isotope uses and production. It also presents key issues, conclusions and recommendations, which will be of interest to policy makers in governmental bodies, scientists and industrial actors in the field.

  5. Hafnium isotope stratigraphy of ferromanganese crusts

    Science.gov (United States)

    Lee; Halliday; Hein; Burton; Christensen; Gunther

    1999-08-13

    A Cenozoic record of hafnium isotopic compositions of central Pacific deep water has been obtained from two ferromanganese crusts. The crusts are separated by more than 3000 kilometers but display similar secular variations. Significant fluctuations in hafnium isotopic composition occurred in the Eocene and Oligocene, possibly related to direct advection from the Indian and Atlantic oceans. Hafnium isotopic compositions have remained approximately uniform for the past 20 million years, probably reflecting increased isolation of the central Pacific. The mechanisms responsible for the increase in (87)Sr/(86)Sr in seawater through the Cenozoic apparently had no effect on central Pacific deep-water hafnium.

  6. New Isotopic Tracers for Shale Gas and Hydraulic Fracturing Fluids

    Science.gov (United States)

    The combined application of geochemistry, stable isotopes (δ18O, δ2H), strontium isotopes (87Sr/86Sr), boron isotopes (δ11B), and radium isotopes (228Ra/226Ra) provides a unique methodology for tracing and monitoring shale gas and fracking fluids in the environment.

  7. Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO2 nuclear fuel

    Science.gov (United States)

    Piro, M. H. A.; Banfield, J.; Clarno, K. T.; Simunovic, S.; Besmann, T. M.; Lewis, B. J.; Thompson, W. T.

    2013-10-01

    Predictive capabilities for simulating irradiated nuclear fuel behavior are enhanced in the current work by coupling thermochemistry, isotopic evolution and heat transfer. Thermodynamic models that are incorporated into this framework not only predict the departure from stoichiometry of UO2, but also consider dissolved fission and activation products in the fluorite oxide phase, noble metal inclusions, secondary oxides including uranates, zirconates, molybdates and the gas phase. Thermochemical computations utilize the spatial and temporal evolution of the fission and activation product inventory in the pellet, which is typically neglected in nuclear fuel performance simulations. Isotopic computations encompass the depletion, decay and transmutation of more than 2000 isotopes that are calculated at every point in space and time. These computations take into consideration neutron flux depression and the increased production of fissile plutonium near the fuel pellet periphery (i.e., the so-called “rim effect”). Thermochemical and isotopic predictions are in very good agreement with reported experimental measurements of highly irradiated UO2 fuel with an average burnup of 102 GW d t(U)-1. Simulation results demonstrate that predictions are considerably enhanced when coupling thermochemical and isotopic computations in comparison to empirical correlations. Notice: This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes.

  8. Tungsten isotopes and the origin of the Moon

    Energy Technology Data Exchange (ETDEWEB)

    Kruijer, Thomas S.; Kleine, Thorsten

    2017-10-01

    The giant impact model of lunar origin predicts that the Moon mainly consists of impactor material. As a result, the Moon is expected to be isotopically distinct from the Earth, but it is not. To account for this unexpected isotopic similarity of the Earth and Moon, several solutions have been proposed, including (i) post-giant impact Earth–Moon equilibration, (ii) alternative models that make the Moon predominantly out of proto-Earth mantle, and (iii) formation of the Earth and Moon from an isotopically homogeneous disk reservoir. Here we use W isotope systematics of lunar samples to distinguish between these scenarios. We report high-precision 182W data for several low-Ti and high-Ti mare basalts, as well as for Mg-suite sample 77215, and lunar meteorite Kalahari 009, which complement data previously obtained for KREEP-rich samples. In addition, we utilize high-precision Hf isotope and Ta/W ratio measurements to empirically quantify the superimposed effects of secondary neutron capture on measured 182W compositions. Our results demonstrate that there are no resolvable radiogenic 182W variations within the Moon, implying that the Moon differentiated later than 70 Ma after Solar System formation. In addition, we find that samples derived from different lunar sources have indistinguishable 182W excesses, confirming that the Moon is characterized by a small, uniform ~+26 parts-per-million excess in 182W over the present-day bulk silicate Earth. This 182W excess is most likely caused by disproportional late accretion to the Earth and Moon, and after considering this effect, the pre-late veneer bulk silicate Earth and the Moon have indistinguishable 182W compositions. Mixing calculations demonstrate that this Earth–Moon 182W similarity is an unlikely outcome of the giant impact, which regardless of the amount of impactor material incorporated into the Moon should have generated a significant 182W excess in the Moon. Consequently, our results imply that post

  9. Recent insights into intramolecular 13C isotope composition of biomolecules

    Science.gov (United States)

    Gilbert, A.; Yamada, K.; Julien, M.; Yoshida, N.; Remaud, G.; Robins, R.

    2016-12-01

    In 1961 Abelson & Hoering shown that the intramolecular 13C distribution in amino acids was not homogeneous, namely the carboxylic acid positions were 13C-enriched compared with the mean of the remaining C-atoms in the molecule [1]. Nearly 20 years later, Monson & Hayes were able to demonstrate that even and odd positions in acetogenic fatty acids also showed non-statistical 13C isotope distributions, and that the pattern varied depending on the organism [2]. It took a further decade for the intramolecular 13C distribution in the key metabolite, glucose, to be defined [3]. Although informative, much of this work was incomplete, a number of positions having to be deduced by difference. This limitation arose mainly due to the lack of techniques enabling the separation and quantification of 13C isotopomers of the target molecule. In the past decade, quantitative 13C NMR has been developed for the determination of the intramolecular isotope composition of a given molecule with a precision of 1‰ or better [4]. This breakthrough has made possible a comprehensive view of the determinants governing intramolecular isotope composition of biological molecules. In particular, it can be shown that intramolecular pattern in sugars is influenced by the C-assimilation pathway and by post-photosynthetic fractionation associated with carbohydrate metabolism [5]. In addition, analysis by NMR of the alkyl chain of acetogenic lipids (fatty acids, n-alkanes) shows an alternation between odd and even C-atom positions, as observed by Monson& Hayes [2], throughout the molecule [6]. Overall, it is becoming apparent that this pattern is influenced by two principal metabolic factors: (i) the 13C pattern extant in the starting compounds; (ii) isotope fractionation associated with the enzymes involved in the biosynthetic pathway. On the whole, the determination of intramolecular isotope patterns in biomolecules allows better insights into the conditions and pathways by which they are formed

  10. Modeling position-specific isotope fractionation of organic micropollutants degradation via different reaction pathways

    DEFF Research Database (Denmark)

    Jin, Biao; Rolle, Massimo

    contaminants [2,3] are still lacking. In this study we propose an integrated modeling approach to simultaneously predict concentration as well as bulk and position-specific multi-element isotope evolution during the transformation of organic micropollutants [4]. The model simulates position......Organic compounds are produced in vast quantities for industrial and agricultural use, as well as for human and animal healthcare [1]. These chemicals and their metabolites are frequently detected at trace levels in fresh water environments, such as groundwater systems, and are referred......: dichlorobenzamide (BAM), isoproturon (IPU) and diclofenac (DCF). The model successfully reproduces the multi-element isotope data, and precisely captures the dual element isotope trends, characterizing the different degradation pathways. Besides illustrating the model capability of mechanistic evaluation...

  11. Non-biological fractionation of stable Ca isotopes in soils of the Atacama Desert, Chile

    Science.gov (United States)

    Ewing, Stephanie A.; Yang, Wenbo; DePaolo, Donald J.; Michalski, Greg; Kendall, Carol; Stewart, Brian W.; Thiemens, Mark; Amundson, Ronald

    2008-02-01

    We measured Ca stable isotope ratios (δ 44/40Ca) in an ancient (2 My), hyperarid soil where the primary source of mobile Ca is atmospheric deposition. Most of the Ca in the upper meter of this soil (3.5 kmol m -2) is present as sulfates (2.5 kmol m -2), and to a lesser extent carbonates (0.4 kmol m -2). In aqueous extracts of variably hydrated calcium sulfate minerals, δ 44/40Ca E values (vs. bulk Earth) increase with depth (1.4 m) from a minimum of -1.91‰ to a maximum of +0.59‰. The trend in carbonate-δ 44/40Ca in the top six horizons resembles that of sulfate-δ 44/40Ca, but with values 0.1-0.6‰ higher. The range of observed Ca isotope values in this soil is about half that of δ 44/40Ca values observed on Earth. Linear correlation among δ 44/40Ca, δ 34S and δ 18O values indicates either (a) a simultaneous change in atmospheric input values for all three elements over time, or (b) isotopic fractionation of all three elements during downward transport. We present evidence that the latter is the primary cause of the isotopic variation that we observe. Sulfate-δ 34S values are positively correlated with sulfate-δ 18O values ( R2 = 0.78) and negatively correlated with sulfate δ 44/40Ca E values ( R2 = 0.70). If constant fractionation and conservation of mass with downward transport are assumed, these relationships indicate a δ 44/40Ca fractionation factor of -0.4‰ in CaSO 4. The overall depth trend in Ca isotopes is reproduced by a model of isotopic fractionation during downward Ca transport that considers small and infrequent but regularly recurring rainfall events. Near surface low Ca isotope values are reproduced by a Rayleigh model derived from measured Ca concentrations and the Ca fractionation factor predicted by the relationship with S isotopes. This indicates that the primary mechanism of stable isotope fractionation in CaSO 4 is incremental and effectively irreversible removal of an isotopically enriched dissolved phase by downward

  12. Theoretical isotopic fractionation between structural boron in carbonates and aqueous boric acid and borate ion

    Science.gov (United States)

    Balan, Etienne; Noireaux, Johanna; Mavromatis, Vasileios; Saldi, Giuseppe D.; Montouillout, Valérie; Blanchard, Marc; Pietrucci, Fabio; Gervais, Christel; Rustad, James R.; Schott, Jacques; Gaillardet, Jérôme

    2018-02-01

    The 11B/10B ratio in calcite and aragonite is an important proxy of oceanic water pH. However, the physico-chemical mechanisms underpinning this approach are still poorly known. In the present study, we theoretically determine the equilibrium isotopic fractionation properties of structural boron species in calcium carbonates, BO33-, BO2(OH)2- and B(OH)4- anions substituted for carbonate groups, as well as those of B(OH)4- and B(OH)3 species in vacuum. Significant variability of equilibrium isotopic fractionation properties is observed among these structural species which is related to their contrasted coordination state, Bsbnd O bond lengths and atomic-scale environment. The isotopic composition of structural boron does not only depend on its coordination number but also on its medium range environment, i.e. farther than its first coordination shell. The isotopic fractionation between aqueous species and their counterparts in vacuum are assessed using previous investigations based on similar quantum-mechanical modeling approaches. At 300 K, the equilibrium isotope composition of structural trigonal species is 7-15‰ lighter than that of aqueous boric acid molecules, whereas substituted tetrahedral borate ions are heavier than their aqueous counterparts by 10-13‰. Although significant uncertainties are known to affect the theoretical prediction of fractionation factors between solids and solutions, the usually assumed lack of isotopic fractionation during borate incorporation in carbonates is challenged by these theoretical results. The present theoretical equilibrium fractionation factors between structural boron and aqueous species differ from those inferred from experiments which may indicate that isotopic equilibrium, unlike chemical equilibrium, was not reached in most experiments. Further research into the isotopic fractionation processes at the interface between calcium carbonates and aqueous solution as well as long duration experiments aimed at

  13. Hydrogen isotope fractionation in lipids of the methane-oxidizing bacterium Methylococcus capsulatus

    Science.gov (United States)

    Sessions, Alex L.; Jahnke, Linda L.; Schimmelmann, Arndt; Hayes, John M.

    2002-11-01

    Hydrogen isotopic compositions of individual lipids from Methylococcus capsulatus, an aerobic, methane-oxidizing bacterium, were analyzed by hydrogen isotope-ratio-monitoring gas chromatography-mass spectrometry (GC-MS). The purposes of the study were to measure isotopic fractionation factors between methane, water, and lipids and to examine the biochemical processes that determine the hydrogen isotopic composition of lipids. M. capsulatus was grown in six replicate cultures in which the δD values of methane and water were varied independently. Measurement of concomitant changes in δD values of lipids allowed estimation of the proportion of hydrogen derived from each source and the isotopic fractionation associated with the utilization of each source. All lipids examined, including fatty acids, sterols, and hopanols, derived 31.4 ± 1.7% of their hydrogen from methane. This was apparently true whether the cultures were harvested during exponential or stationary phase. Examination of the relevant biochemical pathways indicates that no hydrogen is transferred directly (with C-H bonds intact) from methane to lipids. Accordingly, we hypothesize that all methane H is oxidized to H 2O, which then serves as the H source for all biosynthesis, and that a balance between diffusion of oxygen and water across cell membranes controls the concentration of methane-derived H 2O at 31%. Values for α l/ w, the isotopic fractionation between lipids and water, were 0.95 for fatty acids and 0.85 for isoprenoid lipids. These fractionations are significantly smaller than those measured in higher plants and algae. Values for α l/ m, the isotopic fractionation between lipids and methane, were 0.94 for fatty acids and 0.79 for isoprenoid lipids. Based on these results, we predict that methanotrophs living in seawater and consuming methane with typical δD values will produce fatty acids with δD between -50 and -170‰, and sterols and hopanols with δD between -150 and -270‰.

  14. A new feature in the internal heavy isotope distribution in ozone

    Science.gov (United States)

    Bhattacharya, S. K.; Savarino, Joel; Michalski, G.; Liang, Mao-Chang

    2014-10-01

    Ozone produced by discharge or photolysis of oxygen has unusually heavy isotopic composition (18O/16O and 17O/16O ratio) which does not follow normal mass fractionation rule: δ17O ˜ 0.52*δ18O, expressed as an anomaly Δ17O = δ17O - 0.52*δ18O. Ozone molecule being an open isosceles triangle can have the heavy isotope located either in its apex or symmetric (s) position or the base or asymmetric (as) position. Correspondingly, one can define positional isotopic enrichment, written as δ18O (s) or δ18O (as) (and similarly for δ17O) as well as position dependent isotope anomaly Δ17O (s) and Δ17O (as). Marcus and co-workers have proposed a semi-empirical model based in principle on the RRKM model of uni-molecular dissociation but with slight modification (departure from statistical randomness assumption for symmetrical molecules) which explains many features of ozone isotopic enrichment. This model predicts that the bulk isotope anomaly is contained wholly in the asymmetric position and the Δ17O (s) is zero. Consequently, Δ17O (as) = 1.5 * Δ17O (bulk) (named here simply as the "1.5 rule") which has been experimentally confirmed over a range of isotopic enrichment. We now show that a critical re-analysis of the earlier experimental data demonstrates a small but significant departure from this 1.5 rule at the highest and lowest levels of enrichments. This departure provides the first experimental proof that the dynamics of ozone formation differs from a statistical model constrained only by restriction of symmetry. We speculate over some possible causes for the departure.

  15. Novel methods for estimating 3D distributions of radioactive isotopes in materials

    Energy Technology Data Exchange (ETDEWEB)

    Iwamoto, Y., E-mail: y.iwamoto0805@ruri.waseda.jp [Research Institute for Science and Engineering, Waseda University, Shinjuku, Tokyo 169-8555 (Japan); Kataoka, J.; Kishimoto, A.; Nishiyama, T.; Taya, T.; Okochi, H.; Ogata, H. [Research Institute for Science and Engineering, Waseda University, Shinjuku, Tokyo 169-8555 (Japan); Yamamoto, S. [Nagoya University Graduate School of Medicine, 1-1-20, Daikominami, Higashi-ku, Nagoya-shi, Aichi 461-8673 (Japan)

    2016-09-21

    In recent years, various gamma-ray visualization techniques, or gamma cameras, have been proposed. These techniques are extremely effective for identifying “hot spots” or regions where radioactive isotopes are accumulated. Examples of such would be nuclear-disaster-affected areas such as Fukushima or the vicinity of nuclear reactors. However, the images acquired with a gamma camera do not include distance information between radioactive isotopes and the camera, and hence are “degenerated” in the direction of the isotopes. Moreover, depth information in the images is lost when the isotopes are embedded in materials, such as water, sand, and concrete. Here, we propose two methods of obtaining depth information of radioactive isotopes embedded in materials by comparing (1) their spectra and (2) images of incident gamma rays scattered by the materials and direct gamma rays. In the first method, the spectra of radioactive isotopes and the ratios of scattered to direct gamma rays are obtained. We verify experimentally that the ratio increases with increasing depth, as predicted by simulations. Although the method using energy spectra has been studied for a long time, an advantage of our method is the use of low-energy (50–150 keV) photons as scattered gamma rays. In the second method, the spatial extent of images obtained for direct and scattered gamma rays is compared. By performing detailed Monte Carlo simulations using Geant4, we verify that the spatial extent of the position where gamma rays are scattered increases with increasing depth. To demonstrate this, we are developing various gamma cameras to compare low-energy (scattered) gamma-ray images with fully photo-absorbed gamma-ray images. We also demonstrate that the 3D reconstruction of isotopes/hotspots is possible with our proposed methods. These methods have potential applications in the medical fields, and in severe environments such as the nuclear-disaster-affected areas in Fukushima.

  16. Nuclear volume effects in equilibrium stable isotope fractionations of mercury, thallium and lead

    Science.gov (United States)

    Yang, Sha; Liu, Yun

    2015-01-01

    The nuclear volume effects (NVEs) of Hg, Tl and Pb isotope systems are investigated with careful evaluation on quantum relativistic effects via the Dirac’s formalism of full-electron wave function. Equilibrium 202Hg/198Hg, 205Tl/203Tl, 207Pb/206Pb and 208Pb/206Pb isotope fractionations are found can be up to 3.61‰, 2.54‰, 1.48‰ and 3.72‰ at room temperature, respectively, larger than fractionations predicted by classical mass-dependent isotope fractionations theory. Moreover, the NVE can cause mass-independent fractionations (MIF) for odd-mass isotopes and even-mass isotopes. The plot of vs. for Hg-bearing species falls into a straight line with the slope of 1.66, which is close to previous experimental results. For the first time, Pb4+-bearing species are found can enrich heavier Pb isotopes than Pb2+-bearing species to a surprising extent, e.g., the enrichment can be up to 4.34‰ in terms of 208Pb/206Pb at room temperature, due to their NVEs are in opposite directions. In contrast, fractionations among Pb2+-bearing species are trivial. Therefore, the large Pb fractionation changes provide a potential new tracer for redox conditions in young and closed geologic systems. The magnitudes of NVE-driven even-mass MIFs of Pb isotopes (i.e., ) and odd-mass MIFs (i.e., ) are almost the same but with opposite signs. PMID:26224248

  17. Short course on St-02 applications of isotope dilutions and isotopic measurements

    Energy Technology Data Exchange (ETDEWEB)

    Miller, P.

    1998-01-05

    This short course includes information on these topics and subtopics: (I) Nuclear Properties: (A) Historic roots; (B) Nomenclature; (C) Nuclear Stability and abundance; (D) Uses of isotopic techniques; (II) Instrumentation: (A) Sources; (B) Mass resolving elements; (C) Detectors; (III) Making Isotopic Measurements by ICP-MS: (A) Deadtime Correction; (B) Mass Discrimination; (C) Signal /Noise considerations; (IV) Applications and examples: (A) Isotope dilution; (B) Double Spike; (C) Biological Application; (D) Environmental Application; (E) Geological.

  18. Calculation of nucleon densities in calcium, nickel, and molybdenum isotopes on the basis of the dispersive optical model

    Science.gov (United States)

    Bespalova, O. V.; Klimochkina, A. A.

    2017-09-01

    The radial distributions of proton and neutron densities in the even-even isotopes 40-70Ca and 48-78Ni and the analogous distributions of neutron densities in the even-even isotopes 92-138Mo were calculated on the basis of the mean-fieldmodel involving a dispersive optical potential. The respective root-mean-square radii and neutron-skin thicknesses were determined for the nuclei under study. In N > 40 calcium isotopes, the calculated neutron root-mean-square radius exhibits a fast growth with increasing N, and this is consistent with the prediction of the neutron-halo structure in calcium isotopes near the neutron drip line.

  19. Within-population isotopic niche variability in savanna mammals: disparity between carnivores and herbivores

    Directory of Open Access Journals (Sweden)

    Daryl eCodron

    2016-02-01

    Full Text Available Large mammal ecosystems have relatively simple food webs, usually comprising three – and sometimes only two – trophic links. Since many syntopic species from the same trophic level therefore share resources, dietary niche partitioning features prominently within these systems. In African and other subtropical savannas, stable carbon isotopes readily distinguish between herbivore species for which foliage and other parts of dicot plants (13C-depleted C3 vegetation are the primary resource (browsers and those for which grasses (13C-enriched C4 vegetation are staples (grazers. Similarly, carbon isotopes distinguish between carnivore diets that may be richer in either browser, grazer, or intermediate-feeding prey. Here, we investigate levels of carbon and nitrogen isotopic niche variation and niche partitioning within populations (or species of carnivores and herbivores from South African savannas. We emphasize predictable differences in within-population trends across trophic levels: we expect that herbivore populations, which require more foraging effort due to higher intake requirements, are far less likely to display within-population resource partitioning than carnivore populations. Our results reveal generally narrower isotopic niche breadths in herbivore than carnivore populations, but more importantly we find lower levels of isotopic differentiation across individuals within herbivore species. While these results offer some support for our general hypothesis, the current paucity of isotopic data for African carnivores limits our ability to test the complete set of predictions arising from our hypothesis. Nevertheless, given the different ecological and ecophysiological constraints to foraging behaviour within each trophic level, comparisons across carnivores and herbivores, which are possible within such simplified foodwebs, make these systems ideal for developing a process-based understanding of conditions underlying the evolution of

  20. Inferring foraging areas of nesting loggerhead turtles using satellite telemetry and stable isotopes.

    Directory of Open Access Journals (Sweden)

    Simona A Ceriani

    Full Text Available In recent years, the use of intrinsic markers such as stable isotopes to link breeding and foraging grounds of migratory species has increased. Nevertheless, several assumptions still must be tested to interpret isotopic patterns found in the marine realm. We used a combination of satellite telemetry and stable isotope analysis to (i identify key foraging grounds used by female loggerheads nesting in Florida and (ii examine the relationship between stable isotope ratios and post-nesting migration destinations. We collected tissue samples for stable isotope analysis from 14 females equipped with satellite tags and an additional 57 untracked nesting females. Telemetry identified three post-nesting migratory pathways and associated non-breeding foraging grounds: (1 a seasonal continental shelf-constrained migratory pattern along the northeast U.S. coastline, (2 a non-breeding residency in southern foraging areas and (3 a residency in the waters adjacent to the breeding area. Isotopic variability in both δ(13C and δ(15N among individuals allowed identification of three distinct foraging aggregations. We used discriminant function analysis to examine how well δ(13C and δ(15N predict female post-nesting migration destination. The discriminant analysis classified correctly the foraging ground used for all but one individual and was used to predict putative feeding areas of untracked turtles. We provide the first documentation that the continental shelf of the Mid- and South Atlantic Bights are prime foraging areas for a large number (61% of adult female loggerheads from the largest loggerhead nesting population in the western hemisphere and the second largest in the world. Our findings offer insights for future management efforts and suggest that this technique can be used to infer foraging strategies and residence areas in lieu of more expensive satellite telemetry, enabling sample sizes that are more representative at the population level.

  1. Mixing effects on apparent reaction rates and isotope fractionation during denitrification in a heterogeneous aquifer

    Science.gov (United States)

    Green, C.T.; Böhlke, J.K.; Bekins, B.A.; Phillips, S.P.

    2010-01-01

    Gradients in contaminant concentrations and isotopic compositions commonly are used to derive reaction parameters for natural attenuation in aquifers. Differences between field-scale (apparent) estimated reaction rates and isotopic fractionations and local-scale (intrinsic) effects are poorly understood for complex natural systems. For a heterogeneous alluvial fan aquifer, numerical models and field observations were used to study the effects of physical heterogeneity on reaction parameter estimates. Field measurements included major ions, age tracers, stable isotopes, and dissolved gases. Parameters were estimated for the O2 reduction rate, denitrification rate, O 2 threshold for denitrification, and stable N isotope fractionation during denitrification. For multiple geostatistical realizations of the aquifer, inverse modeling was used to establish reactive transport simulations that were consistent with field observations and served as a basis for numerical experiments to compare sample-based estimates of "apparent" parameters with "true" (intrinsic) values. For this aquifer, non-Gaussian dispersion reduced the magnitudes of apparent reaction rates and isotope fractionations to a greater extent than Gaussian mixing alone. Apparent and true rate constants and fractionation parameters can differ by an order of magnitude or more, especially for samples subject to slow transport, long travel times, or rapid reactions. The effect of mixing on apparent N isotope fractionation potentially explains differences between previous laboratory and field estimates. Similarly, predicted effects on apparent O2 threshold values for denitrification are consistent with previous reports of higher values in aquifers than in the laboratory. These results show that hydrogeological complexity substantially influences the interpretation and prediction of reactive transport. ?? 2010 by the American Geophysical Union.

  2. Evaluating chlorine isotope effects from isotope ratios and mass spectra of polychlorinated molecules.

    Science.gov (United States)

    Elsner, Martin; Hunkeler, Daniel

    2008-06-15

    Compound-specific chlorine isotope analysis receives much interest to assess the fate of chlorinated hydrocarbons in contaminated environments. This paper provides a theoretical basis to calculate isotope ratios and quantify isotope fractionation from ion-current ratios of molecular- and fragment-ion multiplets. Because both (35)Cl and (37)Cl are of high abundance, polychlorinated hydrocarbons consist of molecules containing different numbers of (37)Cl denoted as isotopologues. We show that, during reactions, the changes in isotopologue ratios are proportional to changes in the isotope ratio assuming a nonselective isotope distribution in the initial compound. This proportionality extents even to fragments formed in the ion source of a mass spectrometer such as C 2Cl 2 (double dechlorinated fragment of perchloroethylene, PCE). Fractionation factors and kinetic isotope effects (KIE) may, therefore, be evaluated from isotope, isotopologue or even fragment ratios according to conventional simple equations. The proportionality is exact with symmetric molecules such as dichloroethylene (DCE) and PCE, whereas it is approximately true with molecules containing nonreactive positions such as trichloroethylene (TCE). If in the latter case isotope ratios are derived from dechlorinated fragments, e.g., C 2HCl 2, it is important that fragmentation in the ion source affect all molecular positions alike, as otherwise isotopic changes in reactive positions may be underrepresented.

  3. Application of heavy stable isotopes in forensic isotope geochemistry: A review

    Energy Technology Data Exchange (ETDEWEB)

    Aggarwal, Jugdeep [W.M. Keck Isotope Laboratory, Department of Earth Sciences, University of California, Santa Cruz, CA 95064 (United States)], E-mail: jaggarwal@pmc.ucsc.edu; Habicht-Mauche, Judith; Juarez, Chelsey [Department of Anthropology, University of California, Santa Cruz, CA 95064 (United States)

    2008-09-15

    Light stable isotopes have been used for many years to characterize the source and transport of materials. More recently heavy isotope systems such as Sr, Nd and Pb have been added to this list in order to aid source identification. With the advent of multiple collector ICP-MS, the range of isotopic tools now available has increased considerably, however, until the isotope systematics of these new non-traditional isotope systems have become better understood, they will not be as useful in characterizing material source and transportation. Applications using heavy metal stable isotopes (mostly traditional heavy isotopes) have reached most avenues in science, including earth sciences, archaeology, anthropology, animal physiology, ecology and toxicology. This field will continue to grow as new applications are developed and techniques become simpler and quicker. This paper provides a review of how this field has grown and presents two new applications using Pb and Sr isotopes in glazes to determine the source of ore used in glazes, and using Sr isotopes to determine the origin of undocumented deceased Mexican border crossers.

  4. Oxygen isotope fractionation processes in the water-calcite-aragonite system

    Science.gov (United States)

    Fohlmeister, Jens; Spötl, Christoph; Plessen, Birgit; Tjallingii, Rik; Schröder-Ritzrau, Andrea; Frank, Norbert; Arps, Jennifer; Leutz, Kathrin; Vollweiler, Nicole; Trüssel, Martin

    2017-04-01

    The O isotopic composition of speleothems in their pure calcite or pure aragonite polymorphs provides valuable insight into past climate variability. However, robust climatic interpretations become difficult when both polymorphs are present either in different growth layers or as intergrown fabrics. Experimental studies show that the O isotope fractionation between the dissolved carbonate species and CaCO3 is about 0.75‰ (at 10°C) larger for aragonite than for calcite (e.g., Kim et al., 2007, Kim and O'Neil, 1997). The temperature dependence of this offset is negligible for temperature variations typical of most cave systems. However, cave analogue experiments examining this offset are still lacking. Here, we present stable O isotope measurements of a Holocene speleothem from the Swiss Alps, which shows exactly one calcite-aragonite transition along individual growth layers. Oxygen isotope measurements along 'Hendy test'-like traverses across those transitions provide insight into the fractionation behavior of the water-calcite vs. water-aragonite system. We observed a fractionation offset smaller than predicted by laboratory experiments that varies by at least a factor of two. In addition, the observed variations correlate positively with growth rate and negatively with the isotopic composition of the calcite precipitating at the growth axis. The reason for this behavior is still unclear. Trace element analyses across the transitions of growth layers are planned to help understanding this pattern.

  5. Stable Isotope Biogeochemistry of the Centennial Re-survey of the San Jacinto Mountains, CA

    Science.gov (United States)

    Fogel, M. L.; Swarth, E.; Swarth, C.; Smith-Herman, N.; Tremor, S.; Unitt, P.

    2009-12-01

    In 1908, the San Jacinto Mountains were first surveyed for their animal and plant diversity by Joseph Grinnell and Harry Swarth, Museum of Vertebrate Zoology, UC Berkeley. In 2008, continuing until 2011, the ecology and stable isotope biogeochemistry of the plants, insects, birds, and mammals is being re-surveyed. Results of carbon, nitrogen, and hydrogen isotopes in organic matter show the variation in regional climate and trophic structure. For example, δ15N of plants at more arid stations are more positive by 3-5‰. Plants on westward facing slopes have more negative δ15N (to -6‰) possibly indicating N sources from atmospheric N deposition originating from urban Los Angeles. Isotopic analyses of recent collections will be compared with historic, museum archived specimens of plants and resident birds species. Our initial results show that the carbon isotopic compositions of plants collected in 1908 and during the early part of the 20th century are 1.6‰ enriched in δ13C, as predicted with the rise in industrially influenced atmospheric CO2. Isotopic data will be augmented by species diversity to test the hypothesis that 100 years of human influence has affected the ecosystem in this area and in what manner.

  6. An Investigation into the Relationship Between Distillate Yield and Stable Isotope Fractionation

    Science.gov (United States)

    Sowers, T.; Wagner, A. J.

    2016-12-01

    Recent breakthroughs in laser spectrometry have allowed for faster, more efficient analyses of stable isotopic ratios in water samples. Commercially available instruments from Los Gatos Research and Picarro allow users to quickly analyze a wide range of samples, from seawater to groundwater, with accurate isotope ratios of D/H to within ± 0.2 ‰ and 18O/16O to within ± 0.03 ‰. While these instruments have increased the efficiency of stable isotope laboratories, they come with some major limitations, such as not being able to analyze hypersaline waters. The Los Gatos Research Liquid Water Isotope Analyzer (LWIA) can accurately and consistently measure the stable isotope ratios in waters with salinities ranging from 0 to 4 grams per liter (0 to 40 parts per thousand). In order to analyze water samples with salinities greater than 4 grams per liter, however, it was necessary to develop a consistent method through which to reduce salinity while causing as little fractionation as possible. Using a consistent distillation method, predictable fractionation of δ 18O and δ 2 H values was found to occur. This fractionation occurs according to a linear relationship with respect to the percent yield of the water in the sample. Using this method, samples with high salinity can be analyzed using laser spectrometry instruments, thereby enabling laboratories with Los Gatos or Picarro instruments to analyze those samples in house without having to dilute them using labor-intensive in-house standards or expensive premade standards.

  7. Variable Isotopic Compositions of Host Plant Populations Preclude Assessment of Aphid Overwintering Sites

    Directory of Open Access Journals (Sweden)

    Michael S. Crossley

    2017-12-01

    Full Text Available Soybean aphid (Aphis glycines Matsumura is a pest of soybean in the northern Midwest whose migratory patterns have been difficult to quantify. Improved knowledge of soybean aphid overwintering sites could facilitate the development of control efforts with exponential impacts on aphid densities on a regional scale. In this preliminary study, we explored the utility of variation in stable isotopes of carbon and nitrogen to distinguish soybean aphid overwintering origins. We compared variation in bulk 13C and 15N content in buckthorn (Rhamnus cathartica L. and soybean aphids in Wisconsin, among known overwintering locations in the northern Midwest. Specifically, we looked for associations between buckthorn and environmental variables that could aid in identifying overwintering habitats. We detected significant evidence of correlation between the bulk 13C and 15N signals of soybean aphids and buckthorn, despite high variability in stable isotope composition within and among buckthorn plants. Further, the 15N signal in buckthorn varied predictably with soil composition. However, lack of sufficient differentiation of geographic areas along axes of isotopic and environmental variation appears to preclude the use of carbon and nitrogen isotopic signals as effective predictors of likely aphid overwintering sites. These preliminary data suggest the need for future work that can further account for variability in 13C and 15N within/among buckthorn plants, and that explores the utility of other stable isotopes in assessing likely aphid overwintering sites.

  8. CO self-shielding as the origin of oxygen isotope anomalies in the early solar nebula.

    Science.gov (United States)

    Lyons, J R; Young, E D

    2005-05-19

    The abundances of oxygen isotopes in the most refractory mineral phases (calcium-aluminium-rich inclusions, CAIs) in meteorites have hitherto defied explanation. Most processes fractionate isotopes by nuclear mass; that is, 18O is twice as fractionated as 17O, relative to 16O. In CAIs 17O and 18O are nearly equally fractionated, implying a fundamentally different mechanism. The CAI data were originally interpreted as evidence for supernova input of pure 16O into the solar nebula, but the lack of a similar isotope trend in other elements argues against this explanation. A symmetry-dependent fractionation mechanism may have occurred in the inner solar nebula, but experimental evidence is lacking. Isotope-selective photodissociation of CO in the innermost solar nebula might explain the CAI data, but the high temperatures in this region would have rapidly erased the signature. Here we report time-dependent calculations of CO photodissociation in the cooler surface region of a turbulent nebula. If the surface were irradiated by a far-ultraviolet flux approximately 10(3) times that of the local interstellar medium (for example, owing to an O or B star within approximately 1 pc of the protosun), then substantial fractionation of the oxygen isotopes was possible on a timescale of approximately 10(5) years. We predict that similarly irradiated protoplanetary disks will have H2O enriched in 17O and 18O by several tens of per cent relative to CO.

  9. Iron isotope systematics of the Skaergaard intrusion

    DEFF Research Database (Denmark)

    Lesher, Charles; Lundstrom, C.C.; Barfod, Gry

    crystallization on non-traditional stable isotope systems, particularly iron. FeTi oxide minerals (titanomagnetite and ilmenite) appear after ~60% of the magma had solidified. This was a significant event affecting the liquid line of descent and potentially accompanied by iron isotope fractionation. Here we...... report the results of a broad study of the iron isotope compositions of gabbros within the layered and upper border series of the Skaergaard intrusion, pegmatite and granophyre associated with these gabbroic rocks, and the sandwich horizon thought to represent the product of extreme differentiation and....... Forward modeling of closed system fractional crystallization constrained by cumulate volumes, whole rock and mineral compositions, mineral modes and independent constraints on Fe isotope fractionation factors account for the stratigraphic relations, except during the final stages of differentiation...

  10. Quantification of isotopic turnover in agricultural systems

    Science.gov (United States)

    Braun, A.; Auerswald, K.; Schnyder, H.

    2012-04-01

    The isotopic turnover, which is a proxy for the metabolic rate, is gaining scientific importance. It is quantified for an increasing range of organisms, from microorganisms over plants to animals including agricultural livestock. Additionally, the isotopic turnover is analyzed on different scales, from organs to organisms to ecosystems and even to the biosphere. In particular, the quantification of the isotopic turnover of specific tissues within the same organism, e.g. organs like liver and muscle and products like milk and faeces, has brought new insights to improve understanding of nutrient cycles and fluxes, respectively. Thus, the knowledge of isotopic turnover is important in many areas, including physiology, e.g. milk synthesis, ecology, e.g. soil retention time of water, and medical science, e.g. cancer diagnosis. So far, the isotopic turnover is quantified by applying time, cost and expertise intensive tracer experiments. Usually, this comprises two isotopic equilibration periods. A first equilibration period with a constant isotopic input signal is followed by a second equilibration period with a distinct constant isotopic input signal. This yields a smooth signal change from the first to the second signal in the object under consideration. This approach reveals at least three major problems. (i) The input signals must be controlled isotopically, which is almost impossible in many realistic cases like free ranging animals. (ii) Both equilibration periods may be very long, especially when the turnover rate of the object under consideration is very slow, which aggravates the first problem. (iii) The detection of small or slow pools is improved by large isotopic signal changes, but large isotopic changes also involve a considerable change in the input material; e.g. animal studies are usually carried out as diet-switch experiments, where the diet is switched between C3 and C4 plants, since C3 and C4 plants differ strongly in their isotopic signal. The

  11. The Most Useful Actinide Isotope: Americium-241.

    Science.gov (United States)

    Navratil, James D.; And Others

    1990-01-01

    Reviewed is the discovery, nuclear and chemical properties, and uses of an isotope of Americium (Am-241). Production and separation techniques used in industry are emphasized. Processes are illustrated in flow sheets. (CW)

  12. Barium Isotopes in Single Presolar Grains

    Science.gov (United States)

    Pellin, M. J.; Davis, A. M.; Savina, M. R.; Kashiv, Y.; Clayton, R. N.; Lewis, R. S.; Amari, S.

    2001-01-01

    Barium isotopic compositions of single presolar grains were measured by laser ablation laser resonant ionization mass spectrometry and the implications of the data for stellar processes are discussed. Additional information is contained in the original extended abstract.

  13. The production of stable isotopes in Spain

    Energy Technology Data Exchange (ETDEWEB)

    Urgel, M.; Iglesias, J.; Casas, J.; Saviron, J. M.; Quintanilla, M.

    1965-07-01

    The activities developed in the field of the production of stable isotopes by means of ion-exchange chromatography and thermal diffusion techniques are reported. The first method was used to study the separation of the nitrogen and boron isotopes, whereby the separation factor was determined by the break through method. Values ranging from 1,028 to 1,022 were obtained for the separation factor of nitrogen by using ammonium hydroxide solutions while the corresponding values as obtained for boron amounted to 1,035-1,027 using boric acid solutions. Using ammonium chloride or acetate and sodium borate, respectively, resulted in the obtention of values for the separation factor approaching unity. The isotopic separation has been carried out according to the method of development by displacement. The separation of the isotopes of the noble gases, oxygen, nitrogen and carbon has been accomplished resorting to the method of thermal diffusion. (Author) 16 refs.

  14. Neutron Capture Cross Sections of Tellurium Isotopes

    Science.gov (United States)

    Eastman, Micah; Krane, Kenneth

    2006-05-01

    Neutron capture by the stable even-mass Te isotopes (A = 120 to 130) produces in the neighboring odd-neutron isotopes a low-spin ground state (1/2 or 3/2) and a high-spin (11/2) isomeric state. By irradiating samples of natural isotopic Te in our reactor, we have measured the neutron capture cross sections for all of the odd-mass radioactive ground states and isomers produced in the capture process. By using Cd-shielded and unshielded irradiations, we have been able to obtain both the effective thermal cross sections and the resonance integrals. Comparison with similar neutron capture processes in Sn isotopes leads to interesting systematic effects, especially among the thermal cross sections of the low-spin and high-spin states.

  15. Robust optical carbon dioxide isotope analyzer Project

    Data.gov (United States)

    National Aeronautics and Space Administration — Isotopic analysis of carbon dioxide is an important tool for characterization of the exchange and transformation of carbon between the biosphere and the atmosphere....

  16. Benchmarking stable isotope labeling based quantitative proteomics

    NARCIS (Netherlands)

    Altelaar, A.F.M.|info:eu-repo/dai/nl/304833517; Frese, C.K.; Preisinger, C.|info:eu-repo/dai/nl/325801703; Hennrich, M.L.|info:eu-repo/dai/nl/314406778; Schram, A.W.; Timmers, H.T.M.; Heck, A.J.R.|info:eu-repo/dai/nl/105189332; Mohammed, S.|info:eu-repo/dai/nl/30483632X

    Several quantitative mass spectrometry based technologies have recently evolved to interrogate the complexity, interconnectivity and dynamic nature of proteomes. Currently, the most popular methods use either metabolic or chemical isotope labeling with MS based quantification or chemical labeling

  17. Allan Hills Stable Water Isotopes, Version 1

    Data.gov (United States)

    National Aeronautics and Space Administration — This data set includes stable water isotope values at 10 m resolution along an approximately 5 km transect through the main icefield of the Allan Hills Blue Ice...

  18. Predictive Testing

    Science.gov (United States)

    ... you want to learn. Search form Search Predictive testing You are here Home Testing & Services Testing for ... you make the decision. What Is Predictive Genetic Testing Predictive genetic testing searches for genetic changes, or ...

  19. Sulfur Isotope Effects of Dissimilatory Sulfite Reductase

    Directory of Open Access Journals (Sweden)

    William D. Leavitt

    2015-12-01

    Full Text Available The precise interpretation of environmental sulfur isotope records requires a quantitative understanding of the biochemical controls on sulfur isotope fractionation by the principle isotope-fractionating process within the S cycle, microbial sulfate reduction (MSR. Here we provide the only direct observation of the major (34S/32S and minor (33S/32S, 36S/32S sulfur isotope fractionations imparted by a central enzyme in the energy metabolism of sulfate reducers, dissimilatory sulfite reductase (DsrAB. Results from in vitro sulfite reduction experiments allow us to calculate the in vitro DsrAB isotope effect in 34S/32S (hereafter, 34εDsrAB to be 15.3±2‰, 2σ. The accompanying minor isotope effect in 33S, described as 33λDsrAB, is calculated to be 0.5150±0.0012, 2σ. These observations facilitate a rigorous evaluation of the isotopic fractionation associated with the dissimilatory MSR pathway, as well as of the environmental variables that govern the overall magnitude of fractionation by natural communities of sulfate reducers. The isotope effect induced by DsrAB upon sulfite reduction is a factor of 0.3 to 0.6 times prior indirect estimates, which have ranged from 25 to 53‰ in 34εDsrAB. The minor isotope fractionation observed from DsrAB is consistent with a kinetic or equilibrium effect. Our in vitro constraints on the magnitude of 34εDsrAB is similar to the median value of experimental observations compiled from all known published work, where 34εr-p = 16.1‰ (r – p indicates reactant versus product, n = 648. This value closely matches those of MSR operating at high sulfate reduction rates in both laboratory chemostat experiments (34εSO4-H2S = 17.3±1.5‰ and in modern marine sediments (34εSO4-H2S = 17.3±3.8‰. Targeting the direct isotopic consequences of a specific enzymatic processes is a fundamental step toward a biochemical foundation for reinterpreting the biogeochemical and geobiological sulfur isotope records in modern

  20. Diffusive Fractionation of Lithium Isotopes in Olivine

    Science.gov (United States)

    Homolova, V.; Richter, F. M.; Watson, E. B.; Chaussidon, M.

    2014-12-01

    Systematic lithium isotope variations along concentration gradients found in olivine and pyroxene grains from terrestrial, lunar and martian rocks have been attributed to diffusive isotopic fractionation [Beck et al., 2006; Tang et al., 2007]. In some cases, these isotopic excursions are so large that a single grain may display isotopic variability that spans almost the entire range of documented terrestrial values [Jeffcoate et al., 2007]. In this study, we present the results of experiments to examine diffusive isotopic fractionation of lithium in olivine. The experiments comprised crystallographically oriented slabs of San Carlos olivine juxtaposed with either spodumene powder or a lithium rich pyroxene crystal. Experiments were conducted at 1 GPa and 0.1MPa over a temperature range of 1000 to 1125⁰C. Oxygen fugacity in the 0.1MPa experiments was controlled using the wustite-magnetite and nickel-nickel oxide solid buffer assemblages. Lithium concentrations generally decrease smoothly away from the edges of the grains; however, experiments involving diffusion parallel to the a-axis consistently show peculiar wavy or segmented concentration profiles. Lithium diffusivity parallel to the c-axis is on the order of 1E-14m2/s at 1100⁰C. The diffusivity parallel to the c-axis is more than an order of magnitude faster than diffusion parallel to the b-axis and correlates positively with oxygen fugacity. The lithium isotopic composition, δ7Li = 1000‰ * ((δ7Lisample- δ7Ligrain center)/ δ7Ligrain center), shows a decrease away from the edge of the grain to a minimum value (up to 70‰ lighter) and then an abrupt increase back to the initial isotopic composition of the olivine grain. This isotopic profile is similar to those found in natural grains and an experimental study on diffusive fractionation of lithium isotopes in pyroxene [Richter et al., 2014]. Results from the present study are modeled using the approach of Dohmen et al. [2010], which assumes lithium

  1. Isotope analysis in the transmission electron microscope

    OpenAIRE

    Susi, Toma; Hofer, Christoph; Argentero, Giacomo; Leuthner, Gregor T.; Pennycook, Timothy J.; Mangler, Clemens; Meyer, Jannik C.; Kotakoski, Jani

    2016-01-01

    The {\\AA}ngstr\\"om-sized probe of the scanning transmission electron microscope can visualize and collect spectra from single atoms. This can unambiguously resolve the chemical structure of materials, but not their isotopic composition. Here we differentiate between two isotopes of the same element by quantifying how likely the energetic imaging electrons are to eject atoms. First, we measure the displacement probability in graphene grown from either $^{12}$C or $^{13}$C and describe the proc...

  2. Metastasic bone pain management with radioactive isotopes

    OpenAIRE

    Juan Coya Viña

    2005-01-01

    Pain is the commonest clinical manifestation of bone metastases. Its treatment is palliative in nature, and consists of chemotherapy, radiotherapy, hormonotherapy, diphosphonates, and drug therapy (i. e., opiates). Radioactive isotopes represent an appealing alternative to conventional treatment modalities. Among the different types of isotopes, wide clinical experience with 153Sm has been obtained in this laboratory. In the present study, 94 patients (mean age = 65 years), who had been diagn...

  3. IUPAC Periodic Table of the Isotopes

    Science.gov (United States)

    Holden, N.E.; Coplen, T.B.; Böhlke, J.K.; Wieser, M.E.; Singleton, G.; Walczyk, T.; Yoneda, S.; Mahaffy, P.G.; Tarbox, L.V.

    2011-01-01

    For almost 150 years, the Periodic Table of the Elements has served as a guide to the world of elements by highlighting similarities and differences in atomic structure and chemical properties. To introduce students, teachers, and society to the existence and importance of isotopes of the chemical elements, an IUPAC Periodic Table of the Isotopes (IPTI) has been prepared and can be found as a supplement to this issue.

  4. Isotope separation in a "seeded beam%".

    Science.gov (United States)

    Anderson, J B; Davidovits, P

    1975-02-21

    A new method of separating isotopes in a gaseous mixture is described. The method takes advantage of the differences in velocities of isotopic species in a molecular beam formed by expansion of the mixture with a light gas from a nozzle source. For the separation of the hexafluorides of uranium-235 and uranium-238 the technique has an estimated separative work factor about 500 times higher than the gaseous diffusion process and 100 times higher than the curved-jet method.

  5. Laser Spectroscopy of Neutron Rich Bismuth Isotopes

    CERN Multimedia

    2002-01-01

    %IS344 :\\\\ \\\\ The aim of the experiment is to measure the optical isotope shifts and hyperfine structures of bismuth isotopes across the N=126 shell closure in order to extract the change in mean square charge radii ($\\delta\\langle r^{2}\\rangle$) and static moments. These include the first isotones of lead to be measured directly above the shell closure and will provide new information on the systematics of the kink ($\\delta\\langle r^{2}\\rangle)$ seen in the lead isotopic chain. After two very successful runs the programme has been extended to include the neutron deficient isotopes below $^{201}$Bi to study the systematics across the $i_{13/2}$ neutron sub-shell closure at N=118.\\\\ \\\\ During the initial 2 runs (9 shifts) the isotope shifts and hyperfine structures of three new isotopes, $ ^{210,212,213}$Bi and the 9$^{-}$ isomer of $^{210}$Bi have been measured. The accuracy of the previous measurements of $^{205,206,208}$Bi have been greatly improved. The samples of $ ^{208,210,210^{m}}$Bi were prepared by c...

  6. The discovery of isotopes a complete compilation

    CERN Document Server

    Thoennessen, Michael

    2016-01-01

    This book describes the exciting discovery of every isotope observed on earth to date, which currently numbers some 3000. For each isotope a short essay highlights the authors of the first publication for the isotope, the laboratory and year where and when the isotope was discovered, as well as details about the production and detection methods used. In controversial cases previously claims are also discussed. At the end a comprehensive table lists all isotopes sorted by elements and a complete list of references. Preliminary versions of these paragraphs have been published over the last few years as separate articles in the journal "Atomic Data and Nuclear Data Tables". The work re-evaluates all assignments judging them with a uniform set of criteria. In addition, the author includes over 100 new isotopes which have been discovered since the articles published. This book is a source of information for researchers as well as enthusiastic laymen alike. From the prepublication review: “The explanations focus ...

  7. Stable water isotopes in the MITgcm

    Science.gov (United States)

    Völpel, Rike; Paul, André; Krandick, Annegret; Mulitza, Stefan; Schulz, Michael

    2017-08-01

    We present the first results of the implementation of stable water isotopes in the Massachusetts Institute of Technology general circulation model (MITgcm). The model is forced with the isotopic content of precipitation and water vapor from an atmospheric general circulation model (NCAR IsoCAM), while the fractionation during evaporation is treated explicitly in the MITgcm. Results of the equilibrium simulation under pre-industrial conditions are compared to observational data and measurements of plankton tow records (the oxygen isotopic composition of planktic foraminiferal calcite). The broad patterns and magnitude of the stable water isotopes in annual mean seawater are well captured in the model, both at the sea surface as well as in the deep ocean. However, the surface water in the Arctic Ocean is not depleted enough, due to the absence of highly depleted precipitation and snowfall. A model-data mismatch is also recognizable in the isotopic composition of the seawater-salinity relationship in midlatitudes that is mainly caused by the coarse grid resolution. Deep-ocean characteristics of the vertical water mass distribution in the Atlantic Ocean closely resemble observational data. The reconstructed δ18Oc at the sea surface shows a good agreement with measurements. However, the model-data fit is weaker when individual species are considered and deviations are most likely attributable to the habitat depth of the foraminifera. Overall, the newly developed stable water isotope package opens wide prospects for long-term simulations in a paleoclimatic context.

  8. Stable water isotopes in the MITgcm

    Directory of Open Access Journals (Sweden)

    R. Völpel

    2017-08-01

    Full Text Available We present the first results of the implementation of stable water isotopes in the Massachusetts Institute of Technology general circulation model (MITgcm. The model is forced with the isotopic content of precipitation and water vapor from an atmospheric general circulation model (NCAR IsoCAM, while the fractionation during evaporation is treated explicitly in the MITgcm. Results of the equilibrium simulation under pre-industrial conditions are compared to observational data and measurements of plankton tow records (the oxygen isotopic composition of planktic foraminiferal calcite. The broad patterns and magnitude of the stable water isotopes in annual mean seawater are well captured in the model, both at the sea surface as well as in the deep ocean. However, the surface water in the Arctic Ocean is not depleted enough, due to the absence of highly depleted precipitation and snowfall. A model–data mismatch is also recognizable in the isotopic composition of the seawater–salinity relationship in midlatitudes that is mainly caused by the coarse grid resolution. Deep-ocean characteristics of the vertical water mass distribution in the Atlantic Ocean closely resemble observational data. The reconstructed δ18Oc at the sea surface shows a good agreement with measurements. However, the model–data fit is weaker when individual species are considered and deviations are most likely attributable to the habitat depth of the foraminifera. Overall, the newly developed stable water isotope package opens wide prospects for long-term simulations in a paleoclimatic context.

  9. Iron isotopic fractionation during continental weathering

    Energy Technology Data Exchange (ETDEWEB)

    Fantle, Matthew S.; DePaolo, Donald J.

    2003-10-01

    The biological activity on continents and the oxygen content of the atmosphere determine the chemical pathways through which Fe is processed at the Earth's surface. Experiments have shown that the relevant chemical pathways fractionate Fe isotopes. Measurements of soils, streams, and deep-sea clay indicate that the {sup 56}Fe/{sup 54}Fe ratio ({delta}{sup 56}Fe relative to igneous rocks) varies from +1{per_thousand} for weathering residues like soils and clays, to -3{per_thousand} for dissolved Fe in streams. These measurements confirm that weathering processes produce substantial fractionation of Fe isotopes in the modern oxidizing Earth surface environment. The results imply that biologically-mediated processes, which preferentially mobilize light Fe isotopes, are critical to Fe chemistry in weathering environments, and that the {delta}{sup 56}Fe of marine dissolved Fe should be variable and negative. Diagenetic reduction of Fe in marine sediments may also be a significant component of the global Fe isotope cycle. Iron isotopes provide a tracer for the influence of biological activity and oxygen in weathering processes through Earth history. Iron isotopic fractionation during weathering may have been smaller or absent in an oxygen-poor environment such as that of the early Precambrian Earth.

  10. Identification of isotopically primitive interplanetary dust particles: A NanoSIMS isotopic imaging study

    Energy Technology Data Exchange (ETDEWEB)

    Floss, C; Stadermann, F J; Bradley, J P; Dai, Z R; Bajt, S; Graham, G; Lea, A S

    2005-09-02

    We have carried out a comprehensive survey of the isotopic compositions (H, B, C, N, O, S) of a suite of interplanetary dust particles (IDPs), including both cluster and individual particles. Isotopic imaging with the NanoSIMS shows the presence of numerous discrete hotspots that are strongly enriched in {sup 15}N, including the largest {sup 15}N enrichments ({approx}1300 {per_thousand}) observed in IDPs to date. A number of the IDPs also contain larger regions with more modest enrichments in {sup 15}N, leading to average bulk N isotopic compositions that are {sup 15}N-enriched in these IDPs. Although C isotopic compositions are normal in most of the IDPs, two {sup 15}N-rich N-hotspots have correlated {sup 13}C anomalies. CN{sup -}/C{sup -} ratios suggest that most of the {sup 15}N-rich hotspots are associated with relatively N-poor carbonaceous matter, although specific carriers have not been determined. H isotopic distributions are similar to those of N: D anomalies are present both as distinct very D-rich hotspots and as larger regions with more modest enrichments. Nevertheless, H and N isotopic anomalies are not directly correlated, consistent with results from previous studies. Oxygen isotopic imaging shows the presence of abundant presolar silicate grains in the IDPs. The O isotopic compositions of the grains are similar to those found in presolar oxide and silicate grains from primitive meteorites. Most of the silicate grains in the IDPs have isotopic ratios consistent with meteoritic Group 1 oxide grains, indicating origins in oxygen-rich red giant and asymptotic giant branch stars, but several presolar silicates exhibit the {sup 17}O and {sup 18}O enrichments of Group 4 oxide grains, whose origin is less well understood. Based on their N isotopic compositions, the IDPs studied here can be divided into two groups. One group is characterized as being ''isotopically primitive'' and consists of those IDPs that have anomalous bulk N isotopic

  11. Discovery and cross-section measurement of neutron-rich isotopes in the element range from neodymium to platinum with the FRS

    Energy Technology Data Exchange (ETDEWEB)

    Kurcewicz, J., E-mail: j.kurcewicz@gsi.de [GSI Helmholtzzentrum fuer Schwerionenforschung, 64291 Darmstadt (Germany); Farinon, F.; Geissel, H. [GSI Helmholtzzentrum fuer Schwerionenforschung, 64291 Darmstadt (Germany); Justus-Liebig-Universitaet Giessen, 35392 Giessen (Germany); Pietri, S.; Nociforo, C. [GSI Helmholtzzentrum fuer Schwerionenforschung, 64291 Darmstadt (Germany); Prochazka, A. [GSI Helmholtzzentrum fuer Schwerionenforschung, 64291 Darmstadt (Germany); Justus-Liebig-Universitaet Giessen, 35392 Giessen (Germany); Weick, H.; Winfield, J.S. [GSI Helmholtzzentrum fuer Schwerionenforschung, 64291 Darmstadt (Germany); Estrade, A. [GSI Helmholtzzentrum fuer Schwerionenforschung, 64291 Darmstadt (Germany); Astronomy and Physics Department, Saint Mary' s University, Halifax, Nova Scotia B3H 3C3 (Canada); Allegro, P.R.P. [Institute of Physics, Universidade de Sao Paulo, CEP 05508-090 Cidade Universitaria, Sao Paulo (Brazil); Bail, A.; Belier, G. [CEA DAM DiF, 91290 Arpajon Cedex (France); Benlliure, J. [Universidad de Santiago de Compostela, E-15706 Santiago de Compostella (Spain); Benzoni, G. [INFN sezione di Milano, I-20133 Milano (Italy); Bunce, M.; Bowry, M. [Department of Physics, University of Surrey, Guildford, Surrey, GU2 7XH (United Kingdom); Caballero-Folch, R. [Universitat Politecnica de Catalunya, 08034 Barcelona (Spain); and others

    2012-10-31

    Using the high-resolution performance of the fragment separator FRS at GSI we have discovered 60 new neutron-rich isotopes in the atomic number range of 60 Less-Than-Or-Slanted-Equal-To Z Less-Than-Or-Slanted-Equal-To 78. The new isotopes were unambiguously identified in reactions with a {sup 238}U beam impinging on a Be target at 1 GeV/nucleon. The production cross-section for the new isotopes have been measured down to the pico-barn level and compared with predictions of different model calculations. For elements above hafnium fragmentation is the dominant reaction mechanism which creates the new isotopes, whereas fission plays a dominant role for the production of the new isotopes up to thulium.

  12. Discovery and cross-section measurement of neutron-rich isotopes in the element range from neodymium to platinum with the FRS

    Science.gov (United States)

    Kurcewicz, J.; Farinon, F.; Geissel, H.; Pietri, S.; Nociforo, C.; Prochazka, A.; Weick, H.; Winfield, J. S.; Estradé, A.; Allegro, P. R. P.; Bail, A.; Bélier, G.; Benlliure, J.; Benzoni, G.; Bunce, M.; Bowry, M.; Caballero-Folch, R.; Dillmann, I.; Evdokimov, A.; Gerl, J.; Gottardo, A.; Gregor, E.; Janik, R.; Kelić-Heil, A.; Knöbel, R.; Kubo, T.; Litvinov, Yu. A.; Merchan, E.; Mukha, I.; Naqvi, F.; Pfützner, M.; Pomorski, M.; Podolyák, Zs.; Regan, P. H.; Riese, B.; Ricciardi, M. V.; Scheidenberger, C.; Sitar, B.; Spiller, P.; Stadlmann, J.; Strmen, P.; Sun, B.; Szarka, I.; Taïeb, J.; Terashima, S.; Valiente-Dobón, J. J.; Winkler, M.; Woods, Ph.

    2012-10-01

    Using the high-resolution performance of the fragment separator FRS at GSI we have discovered 60 new neutron-rich isotopes in the atomic number range of 60 ⩽ Z ⩽ 78. The new isotopes were unambiguously identified in reactions with a 238U beam impinging on a Be target at 1 GeV/nucleon. The production cross-section for the new isotopes have been measured down to the pico-barn level and compared with predictions of different model calculations. For elements above hafnium fragmentation is the dominant reaction mechanism which creates the new isotopes, whereas fission plays a dominant role for the production of the new isotopes up to thulium.

  13. In-situ Nd isotope measurements on accessory minerals: Insights into isotope equilibration during metamorphism

    Science.gov (United States)

    Hammerli, Johannes; Spandler, Carl; Kemp, Tony; Pirard, Cassian

    2015-04-01

    Understanding isotope equilibration processes during metamorphism has huge implications for a range of geoscience applications, ranging from provenance studies of sedimentary units to the origin of magmas and ore bodies. Furthermore, recent claims of isotope disequilibrium situations during the melting of continental crust have questioned the reliability of using certain isotope systems to track magma sources. Our recent work investigated a prograde sequence of high-temperature, low-pressure (350-650 ˚C, ~3-5 kbar) metasedimentary rocks from the Mt. Lofty Ranges, South Australia that underwent widespread pervasive fluid flow at peak metamorphism. In situ Nd-isotope analyses by LA-MC-ICP-MS found that the detrital signature of apatite survives temperatures of 500 °C. However, the observed isotope equilibration of REE-bearing accessory minerals at ~600 °C, before the onset of partial melting, suggests that isotope disequilibrium is unlikely during high-grade metamorphism of upper crustal rocks where fluid induced melting takes place. Here, we extend our research to metasedimentary rocks from (ultra)-high pressure metamorphic terrains from northern New Caledonia, and Dabieshan, China that represent pressure and temperature conditions found in subduction zones. Our study helps to understand isotope equilibration processes from heterogeneous protoliths as well as the impact of retrogression and the resetting of isotope systems over a pressure-temperature range from ~350 °C to 700 °C and ~15 kbar to 40 kbar. Nd isotope analyses of apatite, allanite, titanite, xenotime, monazite, lawsonite and epidote in pelitic and psammitic samples allow the investigation of isotope equilibration on a mineral and sub-mineral scale, as well as comparison with traditional bulk rock isotope analyses. Our preliminary results show that under high-pressure conditions (~20 to 30 kbar) and temperatures to ~650 °C, REE-bearing phases show variable ɛNd values in some cases. These

  14. KIPS kilowatt isotope power system

    Energy Technology Data Exchange (ETDEWEB)

    1977-01-01

    This Control System topical report covers basic control requirements, selection of control system and a recent review of an electromechanical approach to the flow control valve. Section I covers the basic control requirements for Organic Rankine cycle systems, particular requirements for an isotope fueled space power system, and special requirements imposed by launch, Shuttle deployment and spacecraft requirements. Various control devices which can be used to meet system requirements are discussed. In Section II, various combinations of control functions and devices are presented with comments as to the suitability of each for the intended application. This is essentially a review of the selection process used to pick the present KIPS control system. The formal trade-off matrix, component description, and system selection, as prepared for Design Reviews 2 and 3, is included as Appendix A to the report. Section 3 covers the recently completed design of an electronic-electromechanical flow control valve and compares this approach to the thermal bulb-hydro-mechanical flow control valve baseline. The results of this comparative study indicate that the present configuration is preferable to an electrical valve.

  15. The Incredible, Embryological Egg: Calcium and Strontium Isotopes Recapitulate Ontogeny

    Science.gov (United States)

    Gordon, G. W.; Skulan, J. L.

    2011-12-01

    Embryological development reflects evolutionary history. Understanding the processes of fetal growth is important for curing human birth defects and predicting damage to ecosystems from environmental insults. Tracing enzymatic and hormonal gradients during development, and correlating them to genetic cues dominate modern embryology. Previous work done tracing the mass transfer of elements has generally been limited to isotope spikes in vitro. Natural mass-dependent Ca and Sr isotopic ratios and radiogenic Sr isotopes have the potential to reveal both source and biochemical mechanism information about processes in vivo, but have not previously been extensively explored. The process when a hen lays a fertilized egg that becomes a chick includes formation and dissolution of calcium phosphate (bone) and calcium carbonate (shell). Skulan and DePaolo (1999) showed that chickens have 2% δ44/42Ca between a hen's bones and an egg white; this span represents more than 80% of the entire range of natural Ca isotope variation and illustrates there is significant variation to investigate. A striking feature of archosaurian development that also occurs in many mammals, including humans, is mass transfer of calcium from mother to embryo. The yolk of the domestic hen matures over 7-9 days, but the albumen, shell membranes and shell form in less than 20 hours. Domestic laying hens are at the physiological limit of egg production and selective breeding is no longer an effective method of increasing egg production. 60-75% of the shell's ~1.5 g of calcium comes from dietary sources, while 25-40% comes from the hen's medullary bone. Medullary bone is spicules formed in the marrow of long bones, and is a store of dietary calcium rapidly available for eggshell secretion. During in ovo development, the embryo's skeleton is formed from calcium in the yolk and by bulk dissolution of the eggshell's inner aspect via carbonic anhydrase in a process that has an effect on bone density similar to

  16. Bayesian Integration of Isotope Ratio for Geographic Sourcing of Castor Beans

    Science.gov (United States)

    Webb-Robertson, Bobbie-Jo; Kreuzer, Helen; Hart, Garret; Ehleringer, James; West, Jason; Gill, Gary; Duckworth, Douglas

    2012-01-01

    Recent years have seen an increase in the forensic interest associated with the poison ricin, which is extracted from the seeds of the Ricinus communis plant. Both light element (C, N, O, and H) and strontium (Sr) isotope ratios have previously been used to associate organic material with geographic regions of origin. We present a Bayesian integration methodology that can more accurately predict the region of origin for a castor bean than individual models developed independently for light element stable isotopes or Sr isotope ratios. Our results demonstrate a clear improvement in the ability to correctly classify regions based on the integrated model with a class accuracy of 60.9 ± 2.1% versus 55.9 ± 2.1% and 40.2 ± 1.8% for the light element and strontium (Sr) isotope ratios, respectively. In addition, we show graphically the strengths and weaknesses of each dataset in respect to class prediction and how the integration of these datasets strengthens the overall model. PMID:22919270

  17. Searching for isovector signatures in the neutron-rich oxygen and calcium isotopes

    Directory of Open Access Journals (Sweden)

    Wei-Chia Chen

    2015-09-01

    Full Text Available We search for potential isovector signatures in the neutron-rich oxygen and calcium isotopes within the framework of a relativistic mean-field theory with an exact treatment of pairing correlations. To probe the isovector sector we calibrate a few relativistic density functionals using the same isoscalar constraints but with one differing isovector assumption. It is found that under certain conditions, the isotopic chain in oxygen can be made to terminate at the experimentally observed 24O isotope and in the case of the calcium isotopes at 60Ca. To produce such behavior, the resulting symmetry energy must be soft, with predicted values for the symmetry energy and its slope at saturation density being J=(30.92±0.47 MeV and L=(51.0±1.5 MeV, respectively. As a consequence, the neutron-skin thickness of 208Pb is rather small: Rskin208=(0.161±0.011 fm. This same model—labeled “FSUGarnet”—predicts R1.4=(13.0±0.1 km for the radius of a “canonical” 1.4M⊙ neutron star, yet is also able to support a two-solar-mass neutron star.

  18. Bayesian Integration of Isotope Ratio for Geographic Sourcing of Castor Beans

    Directory of Open Access Journals (Sweden)

    Bobbie-Jo Webb-Robertson

    2012-01-01

    Full Text Available Recent years have seen an increase in the forensic interest associated with the poison ricin, which is extracted from the seeds of the Ricinus communis plant. Both light element (C, N, O, and H and strontium (Sr isotope ratios have previously been used to associate organic material with geographic regions of origin. We present a Bayesian integration methodology that can more accurately predict the region of origin for a castor bean than individual models developed independently for light element stable isotopes or Sr isotope ratios. Our results demonstrate a clear improvement in the ability to correctly classify regions based on the integrated model with a class accuracy of 60.9±2.1% versus 55.9±2.1% and 40.2±1.8% for the light element and strontium (Sr isotope ratios, respectively. In addition, we show graphically the strengths and weaknesses of each dataset in respect to class prediction and how the integration of these datasets strengthens the overall model.

  19. Chromium isotope heterogeneity in the mantle

    Science.gov (United States)

    Xia, Jiuxing; Qin, Liping; Shen, Ji; Carlson, Richard W.; Ionov, Dmitri A.; Mock, Timothy D.

    2017-04-01

    To better constrain the Cr isotopic composition of the silicate Earth and to investigate potential Cr isotopic fractionation during high temperature geological processes, we analyzed the Cr isotopic composition of different types of mantle xenoliths from diverse geologic settings: fertile to refractory off-craton spinel and garnet peridotites, pyroxenite veins, metasomatised spinel lherzolites and associated basalts from central Mongolia, spinel lherzolites and harzburgites from North China, as well as cratonic spinel and garnet peridotites from Siberia and southern Africa. The δ53CrNIST 979 values of the peridotites range from - 0.51 ± 0.04 ‰ (2SD) to + 0.75 ± 0.05 ‰ (2SD). The results show a slight negative correlation between δ53Cr and Al2O3 and CaO contents for most mantle peridotites, which may imply Cr isotopic fractionation during partial melting of mantle peridotites. However, highly variable Cr isotopic compositions measured in Mongolian peridotites cannot be caused by partial melting alone. Instead, the wide range in Cr isotopic composition of these samples most likely reflects kinetic fractionation during melt percolation. Chemical diffusion during melt percolation resulted in light Cr isotopes preferably entering into the melt. Two spinel websterite veins from Mongolia have extremely light δ53Cr values of - 1.36 ± 0.04 ‰ and - 0.77 ± 0.06 ‰, respectively, which are the most negative Cr isotopic compositions yet reported for mantle-derived rocks. These two websterite veins may represent crystallization products from the isotopically light melt that may also metasomatize some peridotites in the area. The δ53Cr values of highly altered garnet peridotites from southern Africa vary from - 0.35 ± 0.04 ‰ (2SD) to + 0.12 ± 0.04 ‰ (2SD) and increase with increasing LOI (Loss on Ignition), reflecting a shift of δ53Cr to more positive values by secondary alteration. The Cr isotopic composition of the pristine, fertile upper mantle is

  20. Magnesium isotope systematics in Martian meteorites

    Science.gov (United States)

    Magna, Tomáš; Hu, Yan; Teng, Fang-Zhen; Mezger, Klaus

    2017-09-01

    Magnesium isotope compositions are reported for a suite of Martian meteorites that span the range of petrological and geochemical types recognized to date for Mars, including crustal breccia Northwest Africa (NWA) 7034. The δ26Mg values (per mil units relative to DSM-3 reference material) range from -0.32 to -0.11‰; basaltic shergottites and nakhlites lie to the heavier end of the Mg isotope range whereas olivine-phyric, olivine-orthopyroxene-phyric and lherzolitic shergottites, and chassignites have slightly lighter Mg isotope compositions, attesting to modest correlation of Mg isotopes and petrology of the samples. Slightly heavier Mg isotope compositions found for surface-related materials (NWA 7034, black glass fraction of the Tissint shergottite fall; δ26Mg > -0.17‰) indicate measurable Mg isotope difference between the Martian mantle and crust but the true extent of Mg isotope fractionation for Martian surface materials remains unconstrained. The range of δ26Mg values from -0.19 to -0.11‰ in nakhlites is most likely due to accumulation of clinopyroxene during petrogenesis rather than garnet fractionation in the source or assimilation of surface material modified at low temperatures. The rather restricted range in Mg isotope compositions between spatially and temporally distinct mantle-derived samples supports the idea of inefficient/absent major tectonic cycles on Mars, which would include plate tectonics and large-scale recycling of isotopically fractionated surface materials back into the Martian mantle. The cumulative δ26Mg value of Martian samples, which are not influenced by late-stage alteration processes and/or crust-mantle interactions, is - 0.271 ± 0.040 ‰ (2SD) and is considered to reflect δ26Mg value of the Bulk Silicate Mars. This value is robust taking into account the range of lithologies involved in this estimate. It also attests to the lack of the Mg isotope variability reported for the inner Solar System bodies at current

  1. Oxygen isotope fractionation between bird bone phosphate and drinking water

    Science.gov (United States)

    Amiot, Romain; Angst, Delphine; Legendre, Serge; Buffetaut, Eric; Fourel, François; Adolfssen, Jan; André, Aurore; Bojar, Ana Voica; Canoville, Aurore; Barral, Abel; Goedert, Jean; Halas, Stanislaw; Kusuhashi, Nao; Pestchevitskaya, Ekaterina; Rey, Kevin; Royer, Aurélien; Saraiva, Antônio Álamo Feitosa; Savary-Sismondini, Bérengère; Siméon, Jean-Luc; Touzeau, Alexandra; Zhou, Zhonghe; Lécuyer, Christophe

    2017-06-01

    Oxygen isotope compositions of bone phosphate (δ18Op) were measured in broiler chickens reared in 21 farms worldwide characterized by contrasted latitudes and local climates. These sedentary birds were raised during an approximately 3 to 4-month period, and local precipitation was the ultimate source of their drinking water. This sampling strategy allowed the relationship to be determined between the bone phosphate δ18Op values (from 9.8 to 22.5‰ V-SMOW) and the local rainfall δ18Ow values estimated from nearby IAEA/WMO stations (from -16.0 to -1.0‰ V-SMOW). Linear least square fitting of data provided the following isotopic fractionation equation: δ18Ow = 1.119 (±0.040) δ18Op - 24.222 (±0.644); R 2 = 0.98. The δ18Op-δ18Ow couples of five extant mallard ducks, a common buzzard, a European herring gull, a common ostrich, and a greater rhea fall within the predicted range of the equation, indicating that the relationship established for extant chickens can also be applied to birds of various ecologies and body masses. Applied to published oxygen isotope compositions of Miocene and Pliocene penguins from Peru, this new equation computes estimates of local seawater similar to those previously calculated. Applied to the basal bird Confuciusornis from the Early Cretaceous of Northeastern China, our equation gives a slightly higher δ18Ow value compared to the previously estimated one, possibly as a result of lower body temperature. These data indicate that caution should be exercised when the relationship estimated for modern birds is applied to their basal counterparts that likely had a metabolism intermediate between that of their theropod dinosaur ancestors and that of advanced ornithurines.

  2. Isotopic inferences of ancient biochemistries - Carbon, sulfur, hydrogen, and nitrogen

    Science.gov (United States)

    Schidlowski, M.; Hayes, J. M.; Kaplan, I. R.

    1983-01-01

    In processes of biological incorporation and subsequent biochemical processing sizable isotope effects occur as a result of both thermodynamic and kinetic fractionations which take place during metabolic and biosynthetic reactions. In this chapter a review is provided of earlier work and recent studies on isotope fractionations in the biogeochemical cycles of carbon, sulfur, hydrogen, and nitrogen. Attention is given to the biochemistry of carbon isotope fractionation, carbon isotope fractionation in extant plants and microorganisms, isotope fractionation in the terrestrial carbon cycle, the effects of diagenesis and metamorphism on the isotopic composition of sedimentary carbon, the isotopic composition of sedimentary carbon through time, implications of the sedimentary carbon isotope record, the biochemistry of sulfur isotope fractionation, pathways of the biogeochemical cycle of nitrogen, and the D/H ratio in naturally occurring materials.

  3. Spatial isotopic heterogeneity during the Guttenberg isotopic carbon excursion: Mechanisms and implications for craton-wide isotope gradients

    Science.gov (United States)

    Metzger, J. G.; Fike, D. A.

    2012-12-01

    The carbon isotopic compositions of carbonate carbon (δ13Ccarb) and organic carbon (δ13Corg) in marine limestones are frequently used as paleoenvironmental proxies and as chemostratigraphic tools for aligning strata. These functions are predicated upon the assumption that isotopic variability in these strata reflects the secular variation in the marine reservoir of dissolved inorganic carbon (DIC). As such, the utility of these isotopic systems largely depends on the assumed spatial homogeneity of marine δ13CDIC. While other isotope systems such as sulfate and strontium have been shown to be extremely well mixed in the modern ocean, a 1-2‰ range in δ13CDIC exists over the entire depth and latitude range of the ocean. This variability in δ13CDIC is largely the result of differences in the local balance of organic carbon fixation and export (increasing δ13CDIC) and/or organic carbon oxidation (decreasing δ13CDIC). The preservation of such isotopic variability in the geologic record has been advocated on several occasions. In particular, previous workers have argued for an ocean-to-interior seaway isotopic gradient in δ13Ccarb, δ13Corg, and ɛNd across Laurentia during the Late Ordovician across the interval that spans the Guttenberg Isotopic Carbon Excursion (GICE). Here we examine two Late Ordovician-aged sections from Missouri, USA that contain the GICE. At first glace, our data showed high degree of stratigraphic and lateral variability. Detailed petrographic and geochemical (e.g., trace element abundance) screening reveals that the majority of the isotopic heterogeneity in our sections is the result of local syndepositional/diagenetic alteration - and not the result of primary gradients in δ13CDIC between the localities examined. Our 'least-altered' δ13Ccarb profile matches closely with previously published records from Iowa; however, sections adjacent both to our locations in Missouri and to the similar δ13Ccarb profile in Iowa are characterized by

  4. Production of noble gas isotopes by proton-induced reactions on lead

    Science.gov (United States)

    Leya, I.; Wieler, R.; David, J.-C.; Leray, S.; Donadille, L.; Cugnon, J.; Michel, R.

    2005-02-01

    We measured integral thin target cross sections for the proton-induced production of He-, Ne-, Ar-, Kr- and Xe-isotopes from lead from the respective reaction threshold up to 2.6 GeV. The production of noble gas isotopes from lead is of special importance for design studies of accelerator driven nuclear reactors and/or energy amplifiers. For all experiments with proton energies above 200 MeV a new mini-stack approach was used instead of the stacked-foil technique in order to minimise the influences of secondary particles on the residual nuclide production. About 420 cross sections for 23 nuclear reactions were determined. The phenomenology of the determined excitation functions enables us to distinguish between the different reaction modes fragmentation, hot and cold symmetric fission, asymmetric fission and deep spallation. Cross sections for the production of 21Ne and 38Ar measured below 100 MeV and 200 MeV, respectively, enable us to study nuclide production below the nominal Coulomb-barrier. The experimental data are compared to results from the theoretical nuclear model code INCL4/ABLA. While the model describes the production of 4He reasonably well, it underestimates the cross sections for Ne- and Ar-isotopes produced via deep spallation and/or multifragmentation by up to two orders of magnitude. For the Kr- and Xe-isotopes the agreement between modelled and measured data strongly depends on the reaction mechanisms. While INCL4/ABLA describes the production of n-poor Kr-isotopes via hot-symmetric fission and the production of Xe-isotopes via asymmetric fission reasonably well, i.e. within a factor of 2, the discrepancies between modelled and measured cross sections for the n-rich Kr-isotopes produced via cold symmetric fission are significantly larger. For the Xe-isotopes produced via spallation, i.e. at energies higher than about 600 MeV, the model completely fails to describe the experimental data. Therefore, the comparison of measured and modelled thin

  5. Using Natural Stable Calcium Isotopes to Rapidly Assess Changes in Bone Mineral Balance Using a Bed Rest Model to Induce Bone Loss

    Science.gov (United States)

    Morgan, J. L. L.; Skulan, J. L.; Gordon, G. E.; Smith, Scott M.; Romaniello, S. J.; Anbar, A. D.

    2012-01-01

    Metabolic bone diseases like osteoporosis result from the disruption of normal bone mineral balance (BMB) resulting in bone loss. During spaceflight astronauts lose substantial bone. Bed rest provides an analog to simulate some of the effects of spaceflight; including bone and calcium loss and provides the opportunity to evaluate new methods to monitor BMB in healthy individuals undergoing environmentally induced-bone loss. Previous research showed that natural variations in the Ca isotope ratio occur because bone formation depletes soft tissue of light Ca isotopes while bone resorption releases that isotopically light Ca back into soft tissue (Skulan et al, 2007). Using a bed rest model, we demonstrate that the Ca isotope ratio of urine shifts in a direction consistent with bone loss after just 7 days of bed rest, long before detectable changes in bone mineral density (BMD) occur. The Ca isotope variations tracks changes observed in urinary N-teleopeptide, a bone resorption biomarker. Bone specific alkaline phosphatase, a bone formation biomarker, is unchanged. The established relationship between Ca isotopes and BMB can be used to quantitatively translate the changes in the Ca isotope ratio to changes in BMD using a simple mathematical model. This model predicts that subjects lost 0.25 0.07% ( SD) of their bone mass from day 7 to day 30 of bed rest. Given the rapid signal observed using Ca isotope measurements and the potential to quantitatively assess bone loss; this technique is well suited to study the short-term dynamics of bone metabolism.

  6. Matching isotopic distributions from metabolically labeled samples.

    Science.gov (United States)

    McIlwain, Sean; Page, David; Huttlin, Edward L; Sussman, Michael R

    2008-07-01

    In recent years stable isotopic labeling has become a standard approach for quantitative proteomic analyses. Among the many available isotopic labeling strategies, metabolic labeling is attractive for the excellent internal control it provides. However, analysis of data from metabolic labeling experiments can be complicated because the spacing between labeled and unlabeled forms of each peptide depends on its sequence, and is thus variable from analyte to analyte. As a result, one generally needs to know the sequence of a peptide to identify its matching isotopic distributions in an automated fashion. In some experimental situations it would be necessary or desirable to match pairs of labeled and unlabeled peaks from peptides of unknown sequence. This article addresses this largely overlooked problem in the analysis of quantitative mass spectrometry data by presenting an algorithm that not only identifies isotopic distributions within a mass spectrum, but also annotates matches between natural abundance light isotopic distributions and their metabolically labeled counterparts. This algorithm is designed in two stages: first we annotate the isotopic peaks using a modified version of the IDM algorithm described last year; then we use a probabilistic classifier that is supplemented by dynamic programming to find the metabolically labeled matched isotopic pairs. Such a method is needed for high-throughput quantitative proteomic metabolomic experiments measured via mass spectrometry. The primary result of this article is that the dynamic programming approach performs well given perfect isotopic distribution annotations. Our algorithm achieves a true positive rate of 99% and a false positive rate of 1% using perfect isotopic distribution annotations. When the isotopic distributions are annotated given 'expert' selected peaks, the same algorithm gets a true positive rate of 77% and a false positive rate of 1%. Finally, when annotating using machine selected peaks, which

  7. Iron isotope biogeochemistry of Neoproterozoic marine shales

    Science.gov (United States)

    Kunzmann, Marcus; Gibson, Timothy M.; Halverson, Galen P.; Hodgskiss, Malcolm S. W.; Bui, Thi Hao; Carozza, David A.; Sperling, Erik A.; Poirier, André; Cox, Grant M.; Wing, Boswell A.

    2017-07-01

    Iron isotopes have been widely applied to investigate the redox evolution of Earth's surface environments. However, it is still unclear whether iron cycling in the water column or during diagenesis represents the major control on the iron isotope composition of sediments and sedimentary rocks. Interpretation of isotopic data in terms of oceanic redox conditions is only possible if water column processes dominate the isotopic composition, whereas redox interpretations are less straightforward if diagenetic iron cycling controls the isotopic composition. In the latter scenario, iron isotope data is more directly related to microbial processes such as dissimilatory iron reduction. Here we present bulk rock iron isotope data from late Proterozoic marine shales from Svalbard, northwestern Canada, and Siberia, to better understand the controls on iron isotope fractionation in late Proterozoic marine environments. Bulk shales span a δ 56Fe range from -0.45 ‰ to +1.04 ‰ . Although δ 56Fe values show significant variation within individual stratigraphic units, their mean value is closer to that of bulk crust and hydrothermal iron in samples post-dating the ca. 717-660 Ma Sturtian glaciation compared to older samples. After correcting for the highly reactive iron content in our samples based on iron speciation data, more than 90% of the calculated δ 56Fe compositions of highly reactive iron falls in the range from ca. -0.8 ‰ to +3 ‰ . An isotope mass-balance model indicates that diagenetic iron cycling can only change the isotopic composition of highly reactive iron by water column processes, namely the degree of oxidation of the ferrous seawater iron reservoir, control the isotopic composition of highly reactive iron. Considering a long-term decrease in the isotopic composition of the iron source to the dissolved seawater Fe(II) reservoir to be unlikely, we offer two possible explanations for the Neoproterozoic δ 56Fe trend. First, a decreasing supply of Fe

  8. Stable isotopes in Lithuanian bioarcheological material

    Science.gov (United States)

    Skipityte, Raminta; Jankauskas, Rimantas; Remeikis, Vidmantas

    2015-04-01

    Investigation of bioarcheological material of ancient human populations allows us to understand the subsistence behavior associated with various adaptations to the environment. Feeding habits are essential to the survival and growth of ancient populations. Stable isotope analysis is accepted tool in paleodiet (Schutkowski et al, 1999) and paleoenvironmental (Zernitskaya et al, 2014) studies. However, stable isotopes can be useful not only in investigating human feeding habits but also in describing social and cultural structure of the past populations (Le Huray and Schutkowski, 2005). Only few stable isotope investigations have been performed before in Lithuanian region suggesting a quite uniform diet between males and females and protein intake from freshwater fish and animal protein. Previously, stable isotope analysis has only been used to study a Stone Age population however, more recently studies have been conducted on Iron Age and Late medieval samples (Jacobs et al, 2009). Anyway, there was a need for more precise examination. Stable isotope analysis were performed on human bone collagen and apatite samples in this study. Data represented various ages (from 5-7th cent. to 18th cent.). Stable carbon and nitrogen isotope analysis on medieval populations indicated that individuals in studied sites in Lithuania were almost exclusively consuming C3 plants, C3 fed terrestrial animals, and some freshwater resources. Current investigation demonstrated social differences between elites and country people and is promising in paleodietary and daily life reconstruction. Acknowledgement I thank prof. dr. G. Grupe, Director of the Anthropological and Palaeoanatomical State Collection in Munich for providing the opportunity to work in her laboratory. The part of this work was funded by DAAD. Antanaitis-Jacobs, Indre, et al. "Diet in early Lithuanian prehistory and the new stable isotope evidence." Archaeologia Baltica 12 (2009): 12-30. Le Huray, Jonathan D., and Holger

  9. Tungsten Stable Isotope Compositions of Ferromanganese Crusts

    Science.gov (United States)

    Abraham, K.; Barling, J.; Hein, J. R.; Schauble, E. A.; Halliday, A. N.

    2014-12-01

    We report the first accurate and precise data for mass-dependent fractionation of tungsten (W) stable isotopes, using a double spike technique and MC-ICPMS. Results are expressed relative to the NIST 3136 W isotope standard as per mil deviations in 186W/184W (δ186W). Although heavy element mass-dependent fractionations are expected to be small, Tl and U both display significant low temperature isotopic fractionations. Theoretical calculations indicate that W nuclear volume isotopic effects should be smaller than mass-dependent fractionations at low temperatures. Hydrogenetic ferromanganese (Fe-Mn) crusts precipitate directly from seawater and have been used as paleoceanographic recorders of temporal changes in seawater chemistry. Crusts are strongly enriched in W and other metals, and are a promising medium for exploring W isotopic variability. Tungsten has a relatively long residence time in seawater of ~61,000 years, mainly as the tungstate ion (WO42-). Water depth profiles show conservative behaviour. During adsorption on Fe-Mn crusts, W species form inner-sphere complexes in the hexavalent (W6+) state. The major host phase is thought to be Mn oxides and the lighter W isotope is expected to be absorbed preferentially. Surface scrapings of 13 globally distributed hydrogenetic Fe-Mn crusts display δ186W from -0.08 to -0.22‰ (±0.03‰, 2sd). A trend toward lighter W isotope composition exists with increasing water depth (~1500 to ~5200m) and W concentration. One hydrothermal Mn-oxide sample is anomalously light and Mn nodules are both heavy and light relative to Fe-Mn crusts. Tungsten speciation depends on concentration, pH, and time in solution and is not well understood because of the extremely slow kinetics of the reactions. In addition, speciation of aqueous and/or adsorbed species might be sensitive to pressure, showing similar thermodynamic stability but different effective volumes. Thus, W stable isotopes might be used as a water-depth barometer in

  10. Iron Isotope Constraints on Planetesimal Core Formation

    Science.gov (United States)

    Jordan, M.; Young, E. D.

    2016-12-01

    The prevalence of iron in both planetary cores and silicate mantles renders the element a valuable tool for understanding core formation. Magmatic iron meteorites exhibit an enrichment in 57Fe/54Fe relative to chondrites and HED meteorites. This is suggestive of heavy Fe partitioning into the cores of differentiated bodies. If iron isotope fractionation accompanies core formation, we can elucidate details about the history of accretion for planetary bodies as well as their compositions and relative core sizes. The equilibrium 57Fe/54Fe between metal and silicate is necessary for understanding observed iron isotope compositions and placing constraints on core formation. We measure this fractionation in two Aubrite meteorites, Norton County and Mount Egerton, which have known temperatures of equilibration and equilibrated silicon isotopes. Iron was purified using ion-exchange chromatography. Data were collected on a ThermoFinnigan NeptuneTM multiple-collector inductively coupled plasma-source mass spectrometer (MC-ICP-MS) run in wet plasma mode. The measured fractionation Δ57Femetal-silicate is 0.08‰ ± 0.039 (2 SE) for Norton County and 0.09‰ ± 0.019 (2 SE) for Mount Egerton, indicating that the heavy isotopes of Fe partition into the metallic phase. These rocks are in isotopic equilibrium at a temperature of 1130 K and 1200 K ± 80 K, respectively. The concentration of the heavy isotopes of iron in the metallic phase is consistent with recent experimental studies. Using our measured metal-silicate Fe isotope fractionation and the resulting temperature calibration, while taking into account impurities in the metallic phase and temperatures of equilibration, determine that core formation could explain the observed difference between magmatic iron meteorites and chondrites if parent bodies have small cores. In order to verify that Rayleigh distillation during fractional crystallization was not a cause of iron isotope fractionation in iron meteorites, we measured

  11. CERN to start producing medical isotopes

    CERN Multimedia

    Anaïs Schaeffer

    2012-01-01

    A promising project that was hailed at the ICTR-PHE 2012 medical conference (see Bulletin issues 10-11/2012 and 12-13/2012) has seen the light of day at CERN. The project, known by the name of MEDICIS, will make it possible to produce a large variety of radioactive isotopes for medical research.   This image of a brain, superimposed on a drawing by Leonardo da Vinci, was taken by a PET scanner after injecting a molecule containing a positron-emitting isotope. CERN-MEDICIS will produce new isotopes for imaging which will be able to show up cancerous tissues and destroy them by emitting local radiation as the isotopes decay. In the United States, a new radium-based drug which targets bone metastases is about to go on the market. Radium, which can be brought to bear at the cell level, is a potent weapon in the fight against certain types of cancer, and is opening the way to a new form of medicine. This is the direction that CERN has decided to follow through the CERN-MEDICIS* (Medical Isotopes...

  12. Tin isotope fractionation in terrestrial cassiterites

    Energy Technology Data Exchange (ETDEWEB)

    McNaughton, N.J. (Univ. of Western Australia, Nedlands (Australia)); Rosman, K.J.R. (Curtin Univ. of Technology, Bentley (Australia))

    1991-02-01

    The isotopic composition of tin has been measured in a range of cassiterites and pure reagents to assess the extent to which this element is isotopically fractionated in natural processes. Only two samples showed evidence of isotopic fractionation, and it is concluded that natural Sn isotope fractionation is small and uncommon. This feature reflects the world dominance of Sn-oxide ores Sn-sulfide ores, and the highly efficient processes of Sn dissolution and precipitation which negate equilibrium and kinetic fractionation of Sn isotopes, respectively. The two samples which show slight fractionation are a highly purified and cassiterite from the Archaean Greenbushes pegmatite, Western Australia. The latter Sn is 0.15{per thousand} per mass unit heavier than the authors laboratory standard, whereas the former is 0.12{per thousand} per mass unit lighter. Although the cassiterite fractionation is considered to result from natural geological processes, the fractionation of purified Sn may be either natural or relate to the purification process, the fractionation of this magnitude has a negligible effect on the current best estimate of the atomic weight of Sn, but it does place a lower limit on its associated accuracy.

  13. Stable isotope analysis of dynamic lipidomics.

    Science.gov (United States)

    Brandsma, Joost; Bailey, Andrew P; Koster, Grielof; Gould, Alex P; Postle, Anthony D

    2017-08-01

    Metabolic pathway flux is a fundamental element of biological activity, which can be quantified using a variety of mass spectrometric techniques to monitor incorporation of stable isotope-labelled substrates into metabolic products. This article contrasts developments in electrospray ionisation mass spectrometry (ESI-MS) for the measurement of lipid metabolism with more established gas chromatography mass spectrometry and isotope ratio mass spectrometry methodologies. ESI-MS combined with diagnostic tandem MS/MS scans permits the sensitive and specific analysis of stable isotope-labelled substrates into intact lipid molecular species without the requirement for lipid hydrolysis and derivatisation. Such dynamic lipidomic methodologies using non-toxic stable isotopes can be readily applied to quantify lipid metabolic fluxes in clinical and metabolic studies in vivo. However, a significant current limitation is the absence of appropriate software to generate kinetic models of substrate incorporation into multiple products in the time domain. Finally, we discuss the future potential of stable isotope-mass spectrometry imaging to quantify the location as well as the extent of lipid synthesis. This article is part of a Special Issue entitled: BBALIP_Lipidomics Opinion Articles edited by Sepp Kohlwein. Copyright © 2017 Elsevier B.V. All rights reserved.

  14. Second international conference on isotopes. Conference proceedings

    Energy Technology Data Exchange (ETDEWEB)

    Hardy, C.J. [ed.

    1997-10-01

    The Second International Conference on Isotopes (2ICI) was hosted by the Australian Nuclear Association in Sydney, NSW, Australia. The Theme of the Second Conference: Isotopes for Industry, Health and a Better Environment recognizes that isotopes have been used in these fields successfully for many years and offer prospects for increasing use in the future. The worldwide interest in the use of research reactors and accelerators and in applications of stable and radioactive isotopes, isotopic techniques and radiation in industry, agriculture, medicine, environmental studies and research in general, was considered. Other radiation issues including radiation protection and safety were also addressed. International and national overviews and subject reviews invited from leading experts were included to introduce the program of technical sessions. The invited papers were supported by contributions accepted from participants for oral and poster presentation. A Technical Exhibition was held in association with the Conference. This volume contains the foreword, technical program, the author index and of the papers (1-60) presented at the conference.

  15. Stable Isotope Spectroscopy for Diagnostic Medicine

    Science.gov (United States)

    Murnick, D. E.

    2000-06-01

    Isotopic tracers have been used in medical research for more than fifty years. Radioactive isotopes have been most used because of the high detection efficiencies possible. With increased awareness of the effects of low level radiation and radioactive waste management problems, the need for safe non radioactive tracers has become apparent. Rare stable isotopes of biologically active elements can be used for metabolic and pharmacokinetic studies provided that both sufficient detection sensitivity can be achieved and reliable cost effective instruments can be developed. High resolution optical spectroscopic methods which can determine isotopic ratios with high precision and accuracy are viable for research and clinical use. The study of 13C/12C ratios in CO2 for breath test diagnostics will be described in detail. Using the laser optogalvonic effect with isotopic lasers a specific medical diagnostic for h-pylori infection, has recently received FDA approval. Opportunities exist to study D/H ratios in water and 18O/16O ratios in CO2 and water for basic metabolism diagnostics and 15N/14N ratios in urine for liver function and related studies.

  16. Carbon isotopes in mollusk shell carbonates

    Science.gov (United States)

    McConnaughey, Ted A.; Gillikin, David Paul

    2008-10-01

    Mollusk shells contain many isotopic clues about calcification physiology and environmental conditions at the time of shell formation. In this review, we use both published and unpublished data to discuss carbon isotopes in both bivalve and gastropod shell carbonates. Land snails construct their shells mainly from respired CO2, and shell δ13C reflects the local mix of C3 and C4 plants consumed. Shell δ13C is typically >10‰ heavier than diet, probably because respiratory gas exchange discards CO2, and retains the isotopically heavier HCO3 -. Respired CO2 contributes less to the shells of aquatic mollusks, because CO2/O2 ratios are usually higher in water than in air, leading to more replacement of respired CO2 by environmental CO2. Fluid exchange with the environment also brings additional dissolved inorganic carbon (DIC) into the calcification site. Shell δ13C is typically a few ‰ lower than ambient DIC, and often decreases with age. Shell δ13C retains clues about processes such as ecosystem metabolism and estuarine mixing. Ca2+ ATPase-based models of calcification physiology developed for corals and algae likely apply to mollusks, too, but lower pH and carbonic anhydrase at the calcification site probably suppress kinetic isotope effects. Carbon isotopes in biogenic carbonates are clearly complex, but cautious interpretation can provide a wealth of information, especially after vital effects are better understood.

  17. Fusion and the Discovery of Isotopes

    Science.gov (United States)

    Thoennessen, M.

    2017-11-01

    Heavy-ion fusion-evaporation has been the most productive method to form and identify new isotopes. Of the presently known over 3200 isotopes, almost 25% were discovered with heavy-ion induced reactions. Since the development of the first heavy-ion beam at Berkeley in 1950 most of the nuclides on the neutron-deficient side of the line of stability and all isotopes of the superheavy elements were discovered utilizing fusion reactions. In addition, some isotopes were first produced in heavy-ion transfer, charge-exchange, incomplete fusion or deep inelastic reactions. The discovery of isotopes relies on new advances in accelerator and detector technology. The continuous development of pioneering and innovative separation and detection techniques have pushed the limit towards ‒ and in many cases beyond ‒ the proton-dripline. A review of the discovery of neutron-deficient and super-heavy nuclides in heavy-ion induced reactions as well as an outlook for the discovery potential in the future is presented.

  18. A Hydrogen and He Isotope Nanoprobe

    Energy Technology Data Exchange (ETDEWEB)

    Doyle, Barney L. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Van Deusen, Stuart B. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2017-09-01

    Materials that incorporate hydrogen and helium isotopes are of great interest at Sandia and throughout the NNSA and DOE. The Ion Beam Lab at SNL-NM has invented techniques using micron to mm-size MeV ion beams to recoil these light isotopes (Elastic Recoil Detection or ERD) that can very accurately make such measurements. However, there are many measurements that would benefit NW and DOE that require much better resolution, such as the distribution of H isotopes (and 3He) in individual grains of materials relevant to TPBARs, H and He-embrittlement of weapon components important to Tritium Sustainment Programs, issues with GTSs, batteries… Higher resolution would also benefit the field of materials science in general. To address these and many other issues, nm-scale lateral resolution is required. This LDRD demonstrated that neutral H atoms could be recoiled through a thin film by 70 keV electrons and detected with a Channeltron electron multiplier (CEM). The electrons were steered away from the CEM by strong permanent magnets. This proved the feasibility that the high energy electrons from a transmissionelectron- microscope-TEM can potentially be used to recoil and subsequently detect (e-ERD), quantify and map the concentration of H and He isotopes with nm resolution. This discovery could lead to a TEM-based H/He-isotope nanoprobe with 1000x higher resolution than currently available.

  19. Zn Isotope Fractionation during Sorption onto Kaolinite.

    Science.gov (United States)

    Guinoiseau, Damien; Gélabert, Alexandre; Moureau, Julien; Louvat, Pascale; Benedetti, Marc F

    2016-02-16

    In this study, we quantify zinc isotope fractionation during its sorption onto kaolinite, by performing experiments under various pH, ionic strength, and total Zn concentrations. A systematic enrichment in heavy Zn isotopes on the surface of kaolinite was measured, with Δ(66)Znadsorbed-solution ranging from 0.11‰ at low pH and low ionic strength to 0.49‰ at high pH and high ionic strength. Both the measured Zn concentration and its isotopic ratio are correctly described using a thermodynamic sorption model that considers two binding sites: external basal surfaces and edge sites. Based on this modeling approach, two distinct Zn isotopic fractionation factors were calculated: Δ(66)Znadsorbed-solution = 0.18 ± 0.06‰ for ion exchange onto basal sites, and Δ(66)Znadsorbed-solution = 0.49 ± 0.06‰ for specific complexation onto edge sites. These two distinct factors indicate that Zn isotope fractionation is dominantly controlled by the chemical composition of the solution (pH, ionic strength).

  20. Quantifying Uranium Isotope Ratios Using Resonance Ionization Mass Spectrometry: The Influence of Laser Parameters on Relative Ionization Probability

    Energy Technology Data Exchange (ETDEWEB)

    Isselhardt, Brett H. [Univ. of California, Berkeley, CA (United States)

    2011-09-01

    Resonance Ionization Mass Spectrometry (RIMS) has been developed as a method to measure relative uranium isotope abundances. In this approach, RIMS is used as an element-selective ionization process to provide a distinction between uranium atoms and potential isobars without the aid of chemical purification and separation. We explore the laser parameters critical to the ionization process and their effects on the measured isotope ratio. Specifically, the use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of 235U/238U ratios to decrease laser-induced isotopic fractionation. By broadening the bandwidth of the first laser in a 3-color, 3-photon ionization process from a bandwidth of 1.8 GHz to about 10 GHz, the variation in sequential relative isotope abundance measurements decreased from >10% to less than 0.5%. This procedure was demonstrated for the direct interrogation of uranium oxide targets with essentially no sample preparation. A rate equation model for predicting the relative ionization probability has been developed to study the effect of variation in laser parameters on the measured isotope ratio. This work demonstrates that RIMS can be used for the robust measurement of uranium isotope ratios.

  1. An integrated sulfur isotope model for Namibian shelf sediments

    Science.gov (United States)

    Dale, Andrew W.; Brüchert, Volker; Alperin, Marc; Regnier, Pierre

    2009-04-01

    In this study the sulfur cycle in the organic-rich mud belt underlying the highly productive upwelling waters of the Namibian shelf is quantified using a 1D reaction-transport model. The model calculates vertical concentration and reaction rate profiles in the top 500 cm of sediment which are compared to a comprehensive dataset which includes carbon, sulfur, nitrogen and iron compounds as well as sulfate reduction (SR) rates and stable sulfur isotopes ( 32S, 34S). The sulfur dynamics in the well-mixed surface sediments are strongly influenced by the activity of the large sulfur bacteria Thiomargaritanamibiensis which oxidize sulfide (H 2S) to sulfate ( SO42-) using sea water nitrate ( NO3-) as the terminal electron acceptor. Microbial sulfide oxidation (SOx) is highly efficient, and the model predicts intense cycling between SO42- and H 2S driven by coupled SR and SOx at rates exceeding 6.0 mol S m -2 y -1. More than 96% of the SR is supported by SOx, and only 2-3% of the SO42- pool diffuses directly into the sediment from the sea water. A fraction of the SO42- produced by Thiomargarita is drawn down deeper into the sediment where it is used to oxidize methane anaerobically, thus preventing high methane concentrations close to the sediment surface. Only a small fraction of total H 2S production is trapped as sedimentary sulfide, mainly pyrite (FeS 2) and organic sulfur (S org) (˜0.3 wt.%), with a sulfur burial efficiency which is amongst the lowest values reported for marine sediments (<1%). Yet, despite intense SR, FeS 2 and S org show an isotope composition of ˜5 ‰ at 500 cm depth. These heavy values were simulated by assuming that a fraction of the solid phase sulfur exchanges isotopes with the dissolved sulfide pool. An enrichment in H 2S of 34S towards the sediment-water interface suggests that Thiomargarita preferentially remove H 232S from the pore water. A fractionation of 20-30‰ was estimated for SOx (ɛ SOx) with the model, along with a maximum

  2. Influence of liquid structure on diffusive isotope separation in molten silicates and aqueous solutions

    Energy Technology Data Exchange (ETDEWEB)

    Watkins, J.M.; DePaolo, D.J.; Ryerson, F.J.; Peterson, B.

    2011-03-01

    }/D{sub Si}. Cations diffusing in aqueous solutions display a similar relationship between isotopic separation efficiency and D{sub cation} =D{sub H 2 O} , although the efficiencies are smaller than in silicate liquids. Our empirical relationship provides a tool for predicting the magnitude of diffusive isotopic effects in many geologic environments and a basis for a more comprehensive theory of isotope separation in liquid solutions. We present a conceptual model for the relationship between diffusivity and liquid structure that is consistent with available data.

  3. Enhanced understanding of ectoparasite–host trophic linkages on coral reefs through stable isotope analysis

    Directory of Open Access Journals (Sweden)

    Amanda W.J. Demopoulos

    2015-04-01

    Full Text Available Parasitism, although the most common type of ecological interaction, is usually ignored in food web models and studies of trophic connectivity. Stable isotope analysis is widely used in assessing the flow of energy in ecological communities and thus is a potentially valuable tool in understanding the cryptic trophic relationships mediated by parasites. In an effort to assess the utility of stable isotope analysis in understanding the role of parasites in complex coral-reef trophic systems, we performed stable isotope analysis on three common Caribbean reef fish hosts and two kinds of ectoparasitic isopods: temporarily parasitic gnathiids (Gnathia marleyi and permanently parasitic cymothoids (Anilocra. To further track the transfer of fish-derived carbon (energy from parasites to parasite consumers, gnathiids from host fish were also fed to captive Pederson shrimp (Ancylomenes pedersoni for at least 1 month. Parasitic isopods had δ13C and δ15N values similar to their host, comparable with results from the small number of other host–parasite studies that have employed stable isotopes. Adult gnathiids were enriched in 15N and depleted in 13C relative to juvenile gnathiids, providing insights into the potential isotopic fractionation associated with blood-meal assimilation and subsequent metamorphosis. Gnathiid-fed Pedersen shrimp also had δ13C values consistent with their food source and enriched in 15N as predicted due to trophic fractionation. These results further indicate that stable isotopes can be an effective tool in deciphering cryptic feeding relationships involving parasites and their consumers, and the role of parasites and cleaners in carbon transfer in coral-reef ecosystems specifically.

  4. Geographic variation of strontium and hydrogen isotopes in avian tissue: implications for tracking migration and dispersal.

    Directory of Open Access Journals (Sweden)

    Megan J Sellick

    Full Text Available BACKGROUND: Isotopes can provide unique solutions to fundamental problems related to the ecology and evolution of migration and dispersal because prior movements of individuals can theoretically be tracked from tissues collected from a single capture. However, there is still remarkably little information available about how and why isotopes vary in wild animal tissues, especially over large spatial scales. METHODOLOGY/PRINCIPAL FINDINGS: Here, we describe variation in both stable-hydrogen (deltaD(F and strontium ((87Sr/(86Sr(F isotopic compositions in the feathers of a migratory songbird, the Tree Swallow (Tachycineta bicolor, across 18 sampling sites in North America and then examine potential mechanisms driving this variation. We found that deltaD(F was correlated with latitude of the sampling site, whereas (87Sr/(86Sr(F was correlated with longitude. deltaD(F was related to deltaD of meteoric waters where molting occurred and (87Sr/(86Sr(F was influenced primarily by the geology in the area where feathers were grown. Using simulation models, we then assessed the utility of combining both markers to estimate the origin of individuals. Using 13 geographic regions, we found that the number of individuals correctly assigned to their site of origin increased from less than 40% using either deltaD or (87Sr/(86Sr alone to 74% using both isotopes. CONCLUSIONS/SIGNIFICANCE: Our results suggest that these isotopes have the potential to provide predictable and complementary markers for estimating long-distance animal movements. Combining isotopes influenced by different global-scale processes may allow researchers to link the population dynamics of animals across large geographic ranges.

  5. Simultaneous iron and nickel isotopic analyses of presolar silicon carbide grains

    Science.gov (United States)

    Trappitsch, Reto; Stephan, Thomas; Savina, Michael R.; Davis, Andrew M.; Pellin, Michael J.; Rost, Detlef; Gyngard, Frank; Gallino, Roberto; Bisterzo, Sara; Cristallo, Sergio; Dauphas, Nicolas

    2018-01-01

    Aside from recording stellar nucleosynthesis, a few elements in presolar grains can also provide insights into the galactic chemical evolution (GCE) of nuclides. We have studied the carbon, silicon, iron, and nickel isotopic compositions of presolar silicon carbide (SiC) grains from asymptotic giant branch (AGB) stars to better understand GCE. Since only the neutron-rich nuclides in these grains have been heavily influenced by the parent star, the neutron-poor nuclides serve as GCE proxies. Using CHILI, a new resonance ionization mass spectrometry (RIMS) instrument, we measured 74 presolar SiC grains for all iron and nickel isotopes. With the CHARISMA instrument, 13 presolar SiC grains were analyzed for iron isotopes. All grains were also measured by NanoSIMS for their carbon and silicon isotopic compositions. A comparison of the measured neutron-rich isotopes with models for AGB star nucleosynthesis shows that our measurements are consistent with AGB star predictions for low-mass stars between half-solar and solar metallicity. Furthermore, our measurements give an indication on the 22Ne (α,n)25Mg reaction rate. In terms of GCE, we find that the GCE-dominated iron and nickel isotope ratios, 54Fe /56Fe and 60Ni /58Ni , correlate with their GCE-dominated counterpart in silicon, 29Si /28Si . The measured GCE trends include the Solar System composition, showing that the Solar System is not a special case. However, as seen in silicon and titanium, many presolar SiC grains are more evolved for iron and nickel than the Solar System. This confirms prior findings and agrees with observations of large stellar samples that a simple age-metallicity relationship for GCE cannot explain the composition of the solar neighborhood.

  6. Geographic Variation of Strontium and Hydrogen Isotopes in Avian Tissue: Implications for Tracking Migration and Dispersal

    Science.gov (United States)

    Sellick, Megan J.; Kyser, T. Kurt; Wunder, Michael B.; Chipley, Don; Norris, D. Ryan

    2009-01-01

    Background Isotopes can provide unique solutions to fundamental problems related to the ecology and evolution of migration and dispersal because prior movements of individuals can theoretically be tracked from tissues collected from a single capture. However, there is still remarkably little information available about how and why isotopes vary in wild animal tissues, especially over large spatial scales. Methodology/Principal Findings Here, we describe variation in both stable-hydrogen (δDF) and strontium (87Sr/86SrF) isotopic compositions in the feathers of a migratory songbird, the Tree Swallow (Tachycineta bicolor), across 18 sampling sites in North America and then examine potential mechanisms driving this variation. We found that δDF was correlated with latitude of the sampling site, whereas 87Sr/86SrF was correlated with longitude. δDF was related to δD of meteoric waters where molting occurred and 87Sr/86SrF was influenced primarily by the geology in the area where feathers were grown. Using simulation models, we then assessed the utility of combining both markers to estimate the origin of individuals. Using 13 geographic regions, we found that the number of individuals correctly assigned to their site of origin increased from less than 40% using either δD or 87Sr/86Sr alone to 74% using both isotopes. Conclusions/Significance Our results suggest that these isotopes have the potential to provide predictable and complementary markers for estimating long-distance animal movements. Combining isotopes influenced by different global-scale processes may allow researchers to link the population dynamics of animals across large geographic ranges. PMID:19266102

  7. Enhanced understanding of ectoparasite: host trophic linkages on coral reefs through stable isotope analysis

    Science.gov (United States)

    Demopoulos, Amanda W. J.; Sikkel, Paul C.

    2015-01-01

    Parasitism, although the most common type of ecological interaction, is usually ignored in food web models and studies of trophic connectivity. Stable isotope analysis is widely used in assessing the flow of energy in ecological communities and thus is a potentially valuable tool in understanding the cryptic trophic relationships mediated by parasites. In an effort to assess the utility of stable isotope analysis in understanding the role of parasites in complex coral-reef trophic systems, we performed stable isotope analysis on three common Caribbean reef fish hosts and two kinds of ectoparasitic isopods: temporarily parasitic gnathiids (Gnathia marleyi) and permanently parasitic cymothoids (Anilocra). To further track the transfer of fish-derived carbon (energy) from parasites to parasite consumers, gnathiids from host fish were also fed to captive Pederson shrimp (Ancylomenes pedersoni) for at least 1 month. Parasitic isopods had δ13C and δ15N values similar to their host, comparable with results from the small number of other host–parasite studies that have employed stable isotopes. Adult gnathiids were enriched in 15N and depleted in13C relative to juvenile gnathiids, providing insights into the potential isotopic fractionation associated with blood-meal assimilation and subsequent metamorphosis. Gnathiid-fed Pedersen shrimp also had δ13C values consistent with their food source and enriched in 15N as predicted due to trophic fractionation. These results further indicate that stable isotopes can be an effective tool in deciphering cryptic feeding relationships involving parasites and their consumers, and the role of parasites and cleaners in carbon transfer in coral-reef ecosystems specifically.

  8. Stable water isotope variation in a Central Andean watershed dominated by glacier and snowmelt

    Directory of Open Access Journals (Sweden)

    N. Ohlanders

    2013-03-01

    Full Text Available Central Chile is an economically important region for which water supply is dependent on snow- and ice melt. Nevertheless, the relative contribution of water supplied by each of those two sources remains largely unknown. This study represents the first attempt to estimate the region's water balance using stable isotopes of water in streamflow and its sources. Isotopic ratios of both H and O were monitored during one year in a high-altitude basin with a moderate glacier cover (11.5%. We found that the steep altitude gradient of the studied catchment caused a corresponding gradient in snowpack isotopic composition and that this spatial variation had a profound effect on the temporal evolution of streamflow isotopic composition during snowmelt. Glacier melt and snowmelt contributions to streamflow in the studied basin were determined using a quantitative analysis of the isotopic composition of streamflow and its sources, resulting in a glacier melt contribution of 50–90% for the unusually dry melt year of 2011/2012. This suggests that in (La Niña years with little precipitation, glacier melt is an important water source for central Chile. Predicted decreases in glacier melt due to global warming may therefore have a negative long-term impact on water availability in the Central Andes. The pronounced seasonal pattern in streamflow isotope composition and its close relation to the variability in snow cover and discharge presents a potentially powerful tool to relate discharge variability in mountainous, melt-dominated catchments with related factors such as contributions of sources to streamflow and snowmelt transit times.

  9. Combining Solvent Isotope Effects with Substrate Isotope Effects in Mechanistic Studies of Alcohol and Amine Oxidation by Enzymes*

    Science.gov (United States)

    Fitzpatrick, Paul F.

    2014-01-01

    Oxidation of alcohols and amines is catalyzed by multiple families of flavin-and pyridine nucleotide-dependent enzymes. Measurement of solvent isotope effects provides a unique mechanistic probe of the timing of the cleavage of the OH and NH bonds, necessary information for a complete description of the catalytic mechanism. The inherent ambiguities in interpretation of solvent isotope effects can be significantly decreased if isotope effects arising from isotopically labeled substrates are measured in combination with solvent isotope effects. The application of combined solvent and substrate (mainly deuterium) isotope effects to multiple enzymes is described here to illustrate the range of mechanistic insights that such an approach can provide. PMID:25448013

  10. Tissue turnover rates and isotopic trophic discrimination factors in the endothermic teleost, pacific bluefin tuna (Thunnus orientalis.

    Directory of Open Access Journals (Sweden)

    Daniel J Madigan

    Full Text Available Stable isotope analysis (SIA of highly migratory marine pelagic animals can improve understanding of their migratory patterns and trophic ecology. However, accurate interpretation of isotopic analyses relies on knowledge of isotope turnover rates and tissue-diet isotope discrimination factors. Laboratory-derived turnover rates and discrimination factors have been difficult to obtain due to the challenges of maintaining these species in captivity. We conducted a study to determine tissue- (white muscle and liver and isotope- (nitrogen and carbon specific turnover rates and trophic discrimination factors (TDFs using archived tissues from captive Pacific bluefin tuna (PBFT, Thunnus orientalis, 1-2914 days after a diet shift in captivity. Half-life values for (15N turnover in white muscle and liver were 167 and 86 days, and for (13C were 255 and 162 days, respectively. TDFs for white muscle and liver were 1.9 and 1.1‰ for δ(15N and 1.8 and 1.2‰ for δ(13C, respectively. Our results demonstrate that turnover of (15N and (13C in bluefin tuna tissues is well described by a single compartment first-order kinetics model. We report variability in turnover rates between tissue types and their isotope dynamics, and hypothesize that metabolic processes play a large role in turnover of nitrogen and carbon in PBFT white muscle and liver tissues. (15N in white muscle tissue showed the most predictable change with diet over time, suggesting that white muscle δ(15N data may provide the most reliable inferences for diet and migration studies using stable isotopes in wild fish. These results allow more accurate interpretation of field data and dramatically improve our ability to use stable isotope data from wild tunas to better understand their migration patterns and trophic ecology.

  11. Analysis and optimization of gas-centrifugal separation of uranium isotopes by neural networks

    Directory of Open Access Journals (Sweden)

    Migliavacca S.C.P.

    2002-01-01

    Full Text Available Neural networks are an attractive alternative for modeling complex problems with too many difficulties to be solved by a phenomenological model. A feed-forward neural network was used to model a gas-centrifugal separation of uranium isotopes. The prediction showed good agreement with the experimental data. An optimization study was carried out. The optimal operational condition was tested by a new experiment and a difference of less than 1% was found.

  12. Isotopic scaling in strong-field dissociation by few-cycle pulses

    DEFF Research Database (Denmark)

    Madsen, Lars Bojer

    2009-01-01

    Within the Born-Oppenheimer approximation, scaling laws are derived for isotopic homonuclear diatomic molecules interacting with strong few-cycles laser pulses. As a consequence of an approximate scaling of the transition dipole moment function between charge-resonant states, the Schrödinger...... be performed by a channel specific mapping. By comparing the scaling predictions with the results of ab initio calculations, insight is gained into the nature of the highly nonlinear dissociative ionization mechanisms....

  13. Prediction of reaction cross section for p-Cr

    Directory of Open Access Journals (Sweden)

    Hemalatha M.

    2016-01-01

    Full Text Available Nuclear matter densities and charge radii for even 46−62Cr isotopes have been calculated using relativistic Hartree-Bogoliubov model based on density-dependent meson-exchange relativistic energy density functional. The calculated root-mean-square charge radii agree well with corresponding data and the kink at N=28 is reproduced by the calculation. The calculated target matter densities are folded with the Jeukenne, Lejeune, and Mahaux-Bruyéres inter-nucleon interaction to obtain semi-microscopic optical model potentials for incident protons of 65 MeV on even 46−62Cr isotopes. The elastic scattering differential cross sections calculated using the proton optical potentials reproduce corresponding data for stable isotopes. The optical model potential parameters required for prediction of differential and total reaction cross sections for unstable even isotopes have been obtained.

  14. Water Metabolism of Walruses by Isotope Dilution

    DEFF Research Database (Denmark)

    Acquarone, M.; Born, E. W.; Chwalibog, A.

    In August 2000, the hydrogen isotope dilution method was used on 7 adult male Atlantic walruses (Odobenus rosmarus rosmarus) (weight: 1197±148 kg, mean±SD, range 1013-1508 kg) at a terrestrial haul-out in Northeastern Greenland to determine their body water pool sizes and body water turnover rates....... During immobilization by use of etorphine HCl (reversed with diprenorphine HCl), a first blood sample was taken to measure background isotope levels. The animals were then enriched with deuterium oxide by infusion into the epidural vein. During recovery, while the animals were still on the beach, blood...... was sampled via an epidural catheter, at regular intervals, for up to seven hours after the initial enrichment to assess isotope equilibration in the body water pools. Five individuals returned to the haul-out after feeding trips of varying duration (158±86 hr, 44-287 hr) where they were immobilized again...

  15. Laser spectroscopy of neutron deficient Sn isotopes

    CERN Multimedia

    We propose to study the ground state properties of neutron-deficient Sn isotopes towards the doubly-magic nucleus $^{100}$Sn. Nuclear spins, changes in the rms charge radii and electromagnetic moments of $^{101-121}$Sn will be measured by laser spectroscopy using the CRIS experimental beam line. These ground-state properties will help to clarify the evolution of nuclear structure properties approaching the $\\textit{N = Z =}$ 50 shell closures. The Sn isotopic chain is currently the frontier for the application of state-of-the-art ab-initio calculations. Our knowledge of the nuclear structure of the Sn isotopes will set a benchmark for the advances of many-body methods, and will provide an important test for modern descriptions of the nuclear force.

  16. Stable isotope dilution assays in mycotoxin analysis.

    Science.gov (United States)

    Rychlik, Michael; Asam, Stefan

    2008-01-01

    The principle and applications of stable isotope dilution assays (SIDAs) in mycotoxin analysis are critically reviewed. The general section includes historical aspects of SIDAs, the prerequisites and limitations of the use of stable isotopically labelled internal standards, and possible calibration procedures. In the application section actual SIDAs for the analysis of trichothecenes, zearalenone, fumonisins, patulin, and ochratoxin A are presented. The syntheses and availability of labelled mycotoxins for use as internal standards is reviewed and specific advances in food analysis and toxicology are demonstrated. The review indicates that LC-MS applications, in particular, require the use of stable isotopically labelled standards to compensate for losses during clean-up and for discrimination due to ion suppression. As the commercial availability of these compounds continues to increase, SIDAs can be expected to find expanding use in mycotoxin analysis.

  17. Strontium isotope stratigraphy of the Pelotas Basin

    Energy Technology Data Exchange (ETDEWEB)

    Zerfass, Geise de Santana dos Anjos, E-mail: geise.zerfass@petrobras.com.br [Petroleo Brasileiro S.A. (PETROBRAS/CENPES/PDGEO/BPA), Rio de Janeiro, RJ (Brazil). Centro de Pesquisas e Desenvolvimento Leopoldo Americo Miguez de Mello; Chemale Junior, Farid, E-mail: fchemale@unb.br [Universidade de Brasilia (UnB), DF (Brazil). Instituto de Geociencias; Moura, Candido Augusto Veloso, E-mail: candido@ufpa.br [Universidade Federal do Para (UFPA), Belem, PA (Brazil). Centro de Geociencias. Dept. de Geoquimica e Petrologia; Costa, Karen Badaraco, E-mail: karen.costa@usp.br [Instituto Oceanografico, Sao Paulo, SP (Brazil); Kawashita, Koji, E-mail: koji@usp.br [Unversidade de Sao Paulo (USP), SP (Brazil). Centro de Pesquisas Geocronologicas

    2014-07-01

    Strontium isotope data were obtained from foraminifera shells of the Pelotas Basin Tertiary deposits to facilitate the refinement of the chronostratigraphic framework of this section. This represents the first approach to the acquisition of numerical ages for these strata. Strontium isotope stratigraphy allowed the identification of eight depositional hiatuses in the Eocene-Pliocene section, here classified as disconformities and a condensed section. The reconnaissance of depositional gaps based on confident age assignments represents an important advance considering the remarkably low chronostratigraphic resolution in the Cenozoic section of the Pelotas Basin. The recognition of hiatuses that match hiatuses is based on biostratigraphic data, as well as on global events. Furthermore, a substantial increase in the sedimentation rate of the upper Miocene section was identified. Paleotemperature and productivity trends were identified based on oxygen and carbon isotope data from the Oligocene-Miocene section, which are coherent with worldwide events, indicating the environmental conditions during sedimentation. (author)

  18. Stable Oxygen-18 and Deuterium Isotopes

    DEFF Research Database (Denmark)

    Müller, Sascha

    link the observed seasonal regression/transgression pattern to the inland recharge cycle, which is expressed in hydraulic head configuration and submarine groundwater discharge rates at the fieldsite. Nonetheless, those observed dynamics could not be simulated due to numerical limitations. By the use...... the Skjern River catchment, Denmark. The presented applications focused on studying the isotopic 'input signal' to the hydrosphere in the form of precipitation, the isotopic 'output signal' with its related dynamic processes at a coastal saltwater-freshwater interface (groundwater isotopes) and the temporal...... young age. Those results are in contrast to earlier age estimations from groundwater samples just beneath the stream. We therefore suggest the conceptualization of the hydrological conditions at this headwater catchment to be revised....

  19. Sourcing explosives: a multi-isotope approach.

    Science.gov (United States)

    Widory, David; Minet, Jean-Jacques; Barbe-Leborgne, Martine

    2009-06-01

    Although explosives are easily identified with current instrumental techniques, it is generally impossible to distinguish between sources of the same substance. To alleviate this difficulty, we present a multi-stable isotope (delta13C, delta15N, delta18O, deltaD) approach for appraising the possibility of discriminating explosives. The results from 30 distinct PETN, TNT and ANFO samples show that the different families of explosives are clearly differentiated by both their specific isotope signatures and their combination with corresponding element concentrations. Coupling two or more of the studied isotope systematics yields an even more precise differentiation on the basis of their raw-material origin and/or manufacturing process.

  20. Isotope analysis in the transmission electron microscope

    Science.gov (United States)

    Susi, Toma; Hofer, Christoph; Argentero, Giacomo; Leuthner, Gregor T.; Pennycook, Timothy J.; Mangler, Clemens; Meyer, Jannik C.; Kotakoski, Jani

    2016-10-01

    The Ångström-sized probe of the scanning transmission electron microscope can visualize and collect spectra from single atoms. This can unambiguously resolve the chemical structure of materials, but not their isotopic composition. Here we differentiate between two isotopes of the same element by quantifying how likely the energetic imaging electrons are to eject atoms. First, we measure the displacement probability in graphene grown from either 12C or 13C and describe the process using a quantum mechanical model of lattice vibrations coupled with density functional theory simulations. We then test our spatial resolution in a mixed sample by ejecting individual atoms from nanoscale areas spanning an interface region that is far from atomically sharp, mapping the isotope concentration with a precision better than 20%. Although we use a scanning instrument, our method may be applicable to any atomic resolution transmission electron microscope and to other low-dimensional materials.

  1. Stable isotope dilution assays in mycotoxin analysis

    Energy Technology Data Exchange (ETDEWEB)

    Rychlik, Michael; Asam, Stefan [Universitaet Muenchen, Lehrstuhl fuer Lebensmittelchemie der Technischen, Garching (Germany)

    2008-01-15

    The principle and applications of stable isotope dilution assays (SIDAs) in mycotoxin analysis are critically reviewed. The general section includes historical aspects of SIDAs, the prerequisites and limitations of the use of stable isotopically labelled internal standards, and possible calibration procedures. In the application section actual SIDAs for the analysis of trichothecenes, zearalenone, fumonisins, patulin, and ochratoxin A are presented. The syntheses and availability of labelled mycotoxins for use as internal standards is reviewed and specific advances in food analysis and toxicology are demonstrated. The review indicates that LC-MS applications, in particular, require the use of stable isotopically labelled standards to compensate for losses during clean-up and for discrimination due to ion suppression. As the commercial availability of these compounds continues to increase, SIDAs can be expected to find expanding use in mycotoxin analysis. (orig.)

  2. Chromium isotope fractionation in ferruginous sediments

    Science.gov (United States)

    Bauer, Kohen W.; Gueguen, Bleuenn; Cole, Devon B.; Francois, Roger; Kallmeyer, Jens; Planavsky, Noah; Crowe, Sean A.

    2018-02-01

    Ferrous Fe is a potent reductant of Cr(VI), and while a number of laboratory studies have characterized Cr isotope fractionation associated with Cr(VI) reduction by ferrous iron, the expression of this fractionation in real-world ferrous Fe-rich environments remains unconstrained. Here we determine the isotope fractionation associated with Cr(VI) reduction in modern ferrous Fe-rich sediments obtained from the previously well studied Lake Matano, Indonesia. Whole core incubations demonstrate that reduction of Cr(VI) within ferruginous sediments provides a sink for Cr(VI) leading to Cr(VI) concentration gradients and diffusive Cr(VI) fluxes across the sediment water interface. As reduction proceeded, Cr(VI) remaining in the overlying lake water became progressively enriched in the heavy isotope (53Cr), increasing δ53Cr by 2.0 ± 0.1‰ at the end of the incubation. Rayleigh distillation modelling of the evolution of Cr isotope ratios and Cr(VI) concentrations in the overlying water yields an effective isotope fractionation of εeff = 1.1 ± 0.2‰ (53Cr/52Cr), whereas more detailed diagenetic modelling implies an intrinsic isotope fractionation of εint = 1.80 ± 0.04‰. Parallel slurry experiments performed using anoxic ferruginous sediment yield an intrinsic isotope fractionation of εint = 2.2 ± 0.1‰. These modelled isotope fractionations are corroborated by direct measurement of the δ53Cr composition on the upper 0.5 cm of Lake Matano sediment, revealing an isotopic offset from the lake water of Δ53Cr = 0.21-1.81‰. The data and models reveal that effective isotope fractionations depend on the depth at which Cr(VI) reduction takes place below the sediment water interface-the deeper the oxic non-reactive zone, the smaller the effective fractionation relative to the intrinsic fractionation. Based on the geochemistry of the sediment we suggest the electron donors responsible for reduction are a combination of dissolved Fe(II) and 0.5 M HCl extractable (solid

  3. Ca isotope fractionation on the moon

    Science.gov (United States)

    Russell, W. A.; Papanastassiou, D. A.; Tombrello, T. A.; Epstein, S.

    1977-01-01

    Ca has been measured in a lunar soil in order to establish the presence of isotopically mass-fractionated components. Ca was extracted by a series of water leaches after the soils were 'activated' by brief exposures to fluorine gas. The O2 obtained by this fluorination is found to have delta (O-18) of +21 per mil and to be, therefore, significantly mass-fractionated. Ca obtained in the leaches was analyzed using the double-spike technique. Very small Ca isotope fractionation is found in the leaches of this soil of up to 1 per mil per mass unit difference. The small Ca effects are in marked contrast to the measured delta (O-18) for the same sample and to large effects observed in many soils for oxygen, silicon, sulfur, and potassium. The data on Ca provide stringent constraints on models which attempt to explain the isotope mass-fractionation effects in lunar soils.

  4. Guideline on Isotope Dilution Mass Spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Gaffney, Amy [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2017-05-19

    Isotope dilution mass spectrometry is used to determine the concentration of an element of interest in a bulk sample. It is a destructive analysis technique that is applicable to a wide range of analytes and bulk sample types. With this method, a known amount of a rare isotope, or ‘spike’, of the element of interest is added to a known amount of sample. The element of interest is chemically purified from the bulk sample, the isotope ratio of the spiked sample is measured by mass spectrometry, and the concentration of the element of interest is calculated from this result. This method is widely used, although a mass spectrometer required for this analysis may be fairly expensive.

  5. Water balance model for mean annual hydrogen and oxygen isotope distributions in surface waters of the contiguous United States

    Science.gov (United States)

    Bowen, Gabriel J.; Kennedy, Casey D.; Liu, Zhongfang; Stalker, Jeremy

    2011-12-01

    The stable H and O isotope composition of river and stream water records information on runoff sources and land-atmosphere water fluxes within the catchment and is a potentially powerful tool for network-based monitoring of ecohydrological systems. Process-based hydrological models, however, have thus far shown limited power to replicate observed large-scale variation in U.S. surface water isotope ratios. Here we develop a geographic information system-based model to predict long-term annual average surface water isotope ratios across the contiguous United States. We use elevation-explicit, gridded precipitation isotope maps as model input and data from a U.S. Geological Survey monitoring program for validation. We find that models incorporating monthly variation in precipitation-evapotranspiration (P-E) amounts account for the majority (>89%) of isotopic variation and have reduced regional bias relative to models that do not consider intra-annual P-E effects on catchment water balance. Residuals from the water balance model exhibit strong spatial patterning and correlations that suggest model residuals isolate additional hydrological signal. We use interpolated model residuals to generate optimized prediction maps for U.S. surface water δ2H and δ18O values. We show that the modeled surface water values represent a relatively accurate and unbiased proxy for drinking water isotope ratios across the United States, making these data products useful in ecological and criminal forensics applications that require estimates of the local environmental water isotope variation across large geographic regions.

  6. Isotope shift measurements on the D1 line in francium isotopes at TRIUMF

    Science.gov (United States)

    Collister, R.; Tandecki, M.; Gwinner, G.; Behr, J. A.; Pearson, M. R.; Gomez, E.; Aubin, S.; Zhang, J.; Orozco, L. A.

    2013-05-01

    Francium is the heaviest alkali and has no stable isotopes. The longest-lived among them, with half-lives from seconds to a few minutes, are now available in the new Francium Trapping Facility at TRIUMF, Canada, for future weak interaction studies. We present isotope shift measurements on the 7S1 / 2 --> 7P1 / 2 (D 1) transition on three isotopes, 206, 207 and 213 in a magneto-optical trap. The shifts are measured using a c.w. Ti:sapphire laser locked to a stabilized cavity at the mid-point between two hyperfine transitions of the reference isotope 209Fr. Scanning tunable microwave sidebands locate transitions in the other isotopes. In combination with the D 2 isotope shifts, analysis can provide a separation of the field shift, due to a changing nuclear charge radius, and specific mass shift, due to changing electron correlations, in these isotopes. Work supported by NSERC and NRC from Canada, NSF and DOE from USA, CONYACT from Mexico.

  7. Zinc isotope fractionation during magmatic differentiation and the isotopic composition of the bulk Earth

    Science.gov (United States)

    Chen, Heng; Savage, Paul S.; Teng, Fang-Zehn; Helz, Rosalind T.; Moynier, Frédéric

    2013-01-01

    he zinc stable isotope system has been successfully applied to many and varied fields in geochemistry, but to date it is still not completely clear how this isotope system is affected by igneous processes. In order to evaluate the potential application of Zn isotopes as a proxy for planetary differentiation and volatile history, it is important to constrain the magnitude of Zn isotopic fractionation induced by magmatic differentiation. In this study we present high-precision Zn isotope analyses of two sets of chemically diverse, cogenetic samples from Kilauea Iki lava lake, Hawaii, and Hekla volcano, Iceland, which both show clear evidence of having undergone variable and significant degrees of magmatic differentiation. The Kilauea Iki samples display small but resolvable variations in Zn isotope composition (0.26‰66Zn66Zn defined as the per mille deviation of a sample's 66Zn/64Zn compositional ratio from the JMC-Lyon standard), with the most differentiated lithologies exhibiting more positive δ66Zn values. This fractionation is likely a result of the crystallization of olivine and/or Fe–Ti oxides, which can both host Zn in their crystal structures. Samples from Hekla have a similar range of isotopic variation (0.22‰66Zn66Zn=0.28±0.05‰ (2s.d.).

  8. Diffusion in silicon isotope heterostructures

    Energy Technology Data Exchange (ETDEWEB)

    Silvestri, Hughes Howland [Univ. of California, Berkeley, CA (United States)

    2004-01-01

    The simultaneous diffusion of Si and the dopants B, P, and As has been studied by the use of a multilayer structure of isotopically enriched Si. This structure, consisting of 5 pairs of 120 nm thick natural Si and 28Si enriched layers, enables the observation of 30Si self-diffusion from the natural layers into the 28Si enriched layers, as well as dopant diffusion from an implanted source in an amorphous Si cap layer, via Secondary Ion Mass Spectrometry (SIMS). The dopant diffusion created regions of the multilayer structure that were extrinsic at the diffusion temperatures. In these regions, the Fermi level shift due to the extrinsic condition altered the concentration and charge state of the native defects involved in the diffusion process, which affected the dopant and self-diffusion. The simultaneously recorded diffusion profiles enabled the modeling of the coupled dopant and self-diffusion. From the modeling of the simultaneous diffusion, the dopant diffusion mechanisms, the native defect charge states, and the self- and dopant diffusion coefficients can be determined. This information is necessary to enhance the physical modeling of dopant diffusion in Si. It is of particular interest to the modeling of future electronic Si devices, where the nanometer-scale features have created the need for precise physical models of atomic diffusion in Si. The modeling of the experimental profiles of simultaneous diffusion of B and Si under p-type extrinsic conditions revealed that both species are mediated by neutral and singly, positively charged Si self-interstitials. The diffusion of As and Si under extrinsic n-type conditions yielded a model consisting of the interstitialcy and vacancy mechanisms of diffusion via singly negatively charged self-interstitials and neutral vacancies. The simultaneous diffusion of P and Si has been modeled on the basis of neutral and singly negatively charged self-interstitials and neutral and singly

  9. Modeling chlorine isotope trends during sequential transformation of chlorinated ethenes

    NARCIS (Netherlands)

    Hunkeler, D.; van Breukelen, B.M.; Elsner, M.

    2009-01-01

    There is increasing interest in combined carbon-chlorine compound-specific isotope analysis (CSIA) to differentiate between contaminant sources and to assess transformation processes. However, the significant abundance of polychlorinated molecules with several heavy chlorine isotopes complicates the

  10. The Mt Logan Holocene-late Wisconsinan isotope record

    DEFF Research Database (Denmark)

    Dahl-Jensen, Dorthe; Fisher, David; Osterberg, Erich

    2008-01-01

    Mt Logan • stable isotopes • Holocene • ENSO • peat • N Pacific • sudden change Udgivelsesdato: August......Mt Logan • stable isotopes • Holocene • ENSO • peat • N Pacific • sudden change Udgivelsesdato: August...

  11. Isotopic compositions of boron in sediments and their implications

    Digital Repository Service at National Institute of Oceanography (India)

    Shirodkar, P.V.; Yingkai, X.

    The abundance and isotopic compositions of boron in sediments from the salt lakes of Qaidam Basin, China have been determined by thermal ionization mass spectrometry of cesium borate. The results show large variations in the isotopic compositions...

  12. Production of medical 99 m Tc isotope via photonuclear reaction

    Science.gov (United States)

    Fujiwara, M.; Nakai, K.; Takahashi, N.; Hayakawa, T.; Shizuma, T.; Miyamoto, S.; Fan, G. T.; Takemoto, A.; Yamaguchi, M.; Nishimura, M.

    2017-01-01

    99 m Tc with a 6 hour half-life is one of the most important medical isotopes used for the Single-Photon Emission Computed Tomography (SPECT) inspection in hospitals of US, Canada, Europe and Japan. 99 m Tc isotopes are extracted by the milking method from parent 99Mo isotopes with a 66 hour half-life. The supply of 99Mo isotopes now encounters a serious crisis. Hospitals may not suitably receive 99Mo medical isotopes in near future, due to difficulties in production by research nuclear reactors. Many countries are now looking for alternative ways to generate 99Mo isotopes other than those with research reactors. We discuss a sustained availability of 99 m Tc isotopes via the nat Mo(γ, n) photonuclear reaction, and discuss to solve technical problems for extracting pure 99 m Tc isotopes from other output materials of photonuclear reactions.

  13. Chlorine isotopes potential as geo-chemical tracers

    Digital Repository Service at National Institute of Oceanography (India)

    Shirodkar, P.V.; Pradhan, U.K.; Banerjee, R.

    The potential of chlorine isotopes as tracers of geo-chemical processes of earth and the oceans is highlighted based on systematic studies carried out in understanding the chlorine isotope fractionation mechanism, its constancy in seawater and its...

  14. Biological signatures in clumped isotopes of O2

    Science.gov (United States)

    Yeung, Laurence Y.; Ash, Jeanine L.; Young, Edward D.

    2015-04-01

    The abundances of molecules containing more than one rare isotope have been applied broadly to determine formation temperatures of natural materials. These applications of “clumped” isotopes rely on the assumption that isotope-exchange equilibrium is reached, or at least approached, during the formation of those materials. In a closed-system terrarium experiment, we demonstrate that biological oxygen (O2) cycling drives the clumped-isotope composition of O2 away from isotopic equilibrium. Our model of the system suggests that unique biological signatures are present in clumped isotopes of O2—and not formation temperatures. Photosynthetic O2 is depleted in 18O18O and 17O18O relative to a stochastic distribution of isotopes, unlike at equilibrium, where heavy-isotope pairs are enriched. Similar signatures may be widespread in nature, offering new tracers of biological and geochemical cycling.

  15. Assessment of a delta15N isotopic method to indicate anthropogenic eutrophication in aquatic ecosystems.

    Science.gov (United States)

    Cole, Marci L; Valiela, Ivan; Kroeger, Kevin D; Tomasky, Gabrielle L; Cebrian, Just; Wigand, Cathleen; McKinney, Richard A; Grady, Sara P; Carvalho da Silva, Maria Helena

    2004-01-01

    Increased anthropogenic delivery of nutrients to water bodies, both freshwater and estuarine, has caused detrimental changes in habitat, food web structure, and nutrient cycling. Nitrogen-stable isotopes may be suitable indicators of such increased nutrient delivery. In this study, we looked at the differences in response of macrophyte delta15N values to anthropogenic N across different taxonomic groups and geographic regions to test a stable isotopic method for detecting anthropogenic impacts. Macrophyte delta15N values increased with wastewater input and water-column dissolved inorganic nitrogen (DIN) concentration. When macrophytes were divided into macroalgae and plants, they responded similarly to increases in wastewater N, although macroalgae was a more reliable indicator of both wastewater inputs and water-column DIN concentrations. Smooth cordgrass (Spartina alterniflora Loisel.) Delta15N increased uniformly with wastewater inputs across a geographic range. We used the relationship derived between S. alterniflora and relative wastewater load to predict wastewater loads in locations lacking quantitative land use data. The predictions matched well with known qualitative information, proving the use of a stable isotopic method for predicting wastewater input.

  16. Isotopic abundance in atom trap trace analysis

    Science.gov (United States)

    Lu, Zheng-Tian; Hu, Shiu-Ming; Jiang, Wei; Mueller, Peter

    2014-03-18

    A method and system for detecting ratios and amounts of isotopes of noble gases. The method and system is constructed to be able to measure noble gas isotopes in water and ice, which helps reveal the geological age of the samples and understand their movements. The method and system uses a combination of a cooled discharge source, a beam collimator, a beam slower and magneto-optic trap with a laser to apply resonance frequency energy to the noble gas to be quenched and detected.

  17. Precision Mass Measurement of Argon Isotopes

    CERN Multimedia

    Lunney, D

    2002-01-01

    % IS388\\\\ \\\\ A precision mass measurement of the neutron-deficient isotopes $^{32,33,34}$Ar is proposed. Mass values of these isotopes are of importance for: a) a stringent test of the Isobaric-Multiplet- Mass-Equation, b) a verification of the correctness of calculated charge-dependent corrections as used in super-allowed $\\beta$- decay studies aiming at a test of the CVC hypothesis, and c) the determination of the kinematics in electron-neutrino correlation experiments searching for scalar currents in weak interaction. The measurements will be carried out with the ISOLTRAP Penning trap mass spectrometer.

  18. Iron isotopes in an Archean ocean analogue

    Science.gov (United States)

    Busigny, Vincent; Planavsky, Noah J.; Jézéquel, Didier; Crowe, Sean; Louvat, Pascale; Moureau, Julien; Viollier, Eric; Lyons, Timothy W.

    2014-05-01

    Iron isotopes have been extensively used to trace the history of microbial metabolisms and the redox evolution of the oceans. Archean sedimentary rocks display greater variability in iron isotope ratios and more markedly negative values than those deposited in the Proterozoic and Phanerozoic. This increased variability has been linked to changes in either water column iron cycling or the extent of benthic microbial iron reduction through time. We tested these contrasting scenarios through a detailed study of anoxic and ferruginous Lac Pavin (France), which can serve as a modern analogue of the Archean ocean. A depth-profile in the water column of Lac Pavin shows a remarkable increase in dissolved Fe concentration (0.1-1200 μM) and δ56Fe values (-2.14‰ to +0.31‰) across the oxic-anoxic boundary to the lake bottom. The largest Fe isotope variability is found at the redox boundary and is related to partial oxidation of dissolved ferrous iron, leaving the residual Fe enriched in light isotopes. The analysis of four sediment cores collected along a lateral profile (one in the oxic layer, one at the redox boundary, one in the anoxic zone, and one at the bottom of the lake) indicates that bulk sediments, porewaters, and reactive Fe mostly have δ56Fe values near 0.0 ± 0.2‰, similar to detrital iron. In contrast, pyrite δ56Fe values in sub-chemocline cores (60, 65, and 92 m) are highly variable and show significant deviations from the detrital iron isotope composition (δ56Fepyrite between -1.51‰ and +0.09‰; average -0.93‰). Importantly, the pyrite δ56Fe values mirror the δ56Fe of dissolved iron at the redox boundary—where near quantitative sulfate and sulfide drawdown occurs—suggesting limited iron isotope fractionation during iron sulfide formation. This finding has important implications for the Archean environment. Specifically, this work suggests that in a ferruginous system, most of the Fe isotope variability observed in sedimentary pyrites can

  19. Iron isotope fractionation in planetary crusts

    OpenAIRE

    Wang, Kun; Moynier, Frédéric; Dauphas, Nicolas; Barrat, Jean-Alix,; Craddock, Paul; Sio, Corliss,

    2012-01-01

    International audience; We present new high precision iron isotope data (δ56Fe vs. IRMM-014 in per mil) for four groups of achondrites: one lunar meteorite, 11 martian meteorites, 32 howardite-eucrite-diogenite meteorites (HEDs), and eight angrites. Angrite meteorites are the only planetary materials, other than Earth/Moon system, significantly enriched in the heavy isotopes of Fe compared to chondrites (by an average of +0.12‰ in δ56Fe). While the reason for such fractionation is not complet...

  20. Isotope separation and advanced manufacturing technology

    Science.gov (United States)

    Carpenter, J.; Kan, T.

    This is the fourth issue of a semiannual report for the Isotope Separation and Advanced Materials Manufacturing (ISAM) Technology Program at Lawrence Livermore National Laboratory. Primary objectives include: (1) the Uranium Atomic Vapor Laser Isotope Separation (UAVLIS) process, which is being developed and prepared for deployment as an advanced uranium enrichment capability; (2) Advanced manufacturing technologies, which include industrial laser and E-beam material processing and new manufacturing technologies for uranium, plutonium, and other strategically important materials in support of DOE and other national applications. This report features progress in the ISAM Program from October 1993 through March 1994.

  1. Novel PEFC Application for Deuterium Isotope Separation

    Directory of Open Access Journals (Sweden)

    Hisayoshi Matsushima

    2017-03-01

    Full Text Available The use of a polymer electrolyte fuel cell (PEFC with a Nafion membrane for isotopic separation of deuterium (D was investigated. Mass analysis at the cathode side indicated that D diffused through the membrane and participated in an isotope exchange reaction. The exchange of D with protium (H in H2O was facilitated by a Pt catalyst. The anodic data showed that the separation efficiency was dependent on the D concentration in the source gas, whereby the water produced during the operation of the PEFC was more enriched in D as the D concentration of the source gas was increased.

  2. Isotopic effect on thermal physical properties of isotopically modified boron single crystals

    Energy Technology Data Exchange (ETDEWEB)

    Hu, Quanli [Japan Science and Technology Corporation, Kawaguchi, Saitama (Japan); Noda, Tetsuji; Suzuki, Hiroshi; Araki, Hiroshi; Numazawa, Takenori; Hirano, Toshiyuki [National Institute for Materials Science, Tsukuba, Ibaraki (Japan); Nogi, Naoyuki; Tanaka, Satoru [University of Tokyo, Department of Quantum Engineering and Systems Science, Tokyo (Japan)

    2002-04-01

    The measurement of specific heat and thermal conductivity at low temperature for isotopically modified boron single crystals was performed between 0.5 and 100K using relaxation method and steady heat flow method, respectively. The results indicate that the specific heat has obvious divergences at T<5K. At 40K, the thermal conductivity of {sup 10}B-enriched crystal is about 570 W/m{center_dot}K, which is 40% larger than that of natural boron crystal. The influence of lattice vibration modes and the isotopic effect on specific heat and thermal conductivity for isotopically modified boron are discussed. (author)

  3. Determination of fission gas yields from isotope ratios

    DEFF Research Database (Denmark)

    Mogensen, Mogens Bjerg

    1983-01-01

    This paper describes a method of calculating the actual fission yield of Kr and Xe in nuclear fuel including the effect of neutron capture reactions and decay. The bases for this calculation are the cumulative yields (ref. 1) of Kr and Xe isotopes (or pairs of isotopes) which are unaffected...... by neutron capture reactions, and measured Kr and Xe isotope ratios. Also the burnup contribution from the different fissile heavy isotopes must be known in order to get accurate fission gas yields....

  4. Stable isotope deltas: Tiny, yet robust signatures in nature

    Science.gov (United States)

    Brand, Willi A.; Coplen, Tyler B.

    2012-01-01

    Although most of them are relatively small, stable isotope deltas of naturally occurring substances are robust and enable workers in anthropology, atmospheric sciences, biology, chemistry, environmental sciences, food and drug authentication, forensic science, geochemistry, geology, oceanography, and paleoclimatology to study a variety of topics. Two fundamental processes explain the stable isotope deltas measured in most terrestrial systems: isotopic fractionation and isotope mixing. Isotopic fractionation is the result of equilibrium or kinetic physicochemical processes that fractionate isotopes because of small differences in physical or chemical properties of molecular species having different isotopes. It is shown that the mixing of radioactive and stable isotope end members can be modelled to provide information on many natural processes, including 14C abundances in the modern atmosphere and the stable hydrogen and oxygen isotopic compositions of the oceans during glacial and interglacial times. The calculation of mixing fractions using isotope balance equations with isotope deltas can be substantially in error when substances with high concentrations of heavy isotopes (e.g. 13C, 2H, and 18O ) are mixed. In such cases, calculations using mole fractions are preferred as they produce accurate mixing fractions. Isotope deltas are dimensionless quantities. In the International System of Units (SI), these quantities have the unit 1 and the usual list of prefixes is not applicable. To overcome traditional limitations with expressing orders of magnitude differences in isotope deltas, we propose the term urey (symbol Ur), after Harold C. Urey, for the unit 1. In such a manner, an isotope delta value expressed traditionally as−25 per mil can be written as−25 mUr (or−2.5 cUr or−0.25 dUr; the use of any SI prefix is possible). Likewise, very small isotopic differences often expressed in per meg ‘units’ are easily included (e.g. either+0.015 ‰ or+15 per meg

  5. Stable isotope deltas: tiny, yet robust signatures in nature.

    Science.gov (United States)

    Brand, Willi A; Coplen, Tyler B

    2012-09-01

    Although most of them are relatively small, stable isotope deltas of naturally occurring substances are robust and enable workers in anthropology, atmospheric sciences, biology, chemistry, environmental sciences, food and drug authentication, forensic science, geochemistry, geology, oceanography, and paleoclimatology to study a variety of topics. Two fundamental processes explain the stable isotope deltas measured in most terrestrial systems: isotopic fractionation and isotope mixing. Isotopic fractionation is the result of equilibrium or kinetic physicochemical processes that fractionate isotopes because of small differences in physical or chemical properties of molecular species having different isotopes. It is shown that the mixing of radioactive and stable isotope end members can be modelled to provide information on many natural processes, including (14)C abundances in the modern atmosphere and the stable hydrogen and oxygen isotopic compositions of the oceans during glacial and interglacial times. The calculation of mixing fractions using isotope balance equations with isotope deltas can be substantially in error when substances with high concentrations of heavy isotopes (e.g. (13)C, (2)H, and (18)O ) are mixed. In such cases, calculations using mole fractions are preferred as they produce accurate mixing fractions. Isotope deltas are dimensionless quantities. In the International System of Units (SI), these quantities have the unit 1 and the usual list of prefixes is not applicable. To overcome traditional limitations with expressing orders of magnitude differences in isotope deltas, we propose the term urey (symbol Ur), after Harold C. Urey, for the unit 1. In such a manner, an isotope delta value expressed traditionally as-25 per mil can be written as-25 mUr (or-2.5 cUr or-0.25 dUr; the use of any SI prefix is possible). Likewise, very small isotopic differences often expressed in per meg 'units' are easily included (e.g. either+0.015 ‰ or+15 per meg

  6. Theoretical Evaluation of Intermolecular and Intramolecular Isotope Fractionations in Fragmentation

    OpenAIRE

    Tang, Caiming; Peng, Xianzhi

    2017-01-01

    Revelation of the effects of isotope fractionation during fragmentation in electron ionization mass spectrometry (EI-MS) on compound-specific isotope analysis of chlorine and bromine (CSIA-Cl/Br) may be of crucial significance, yet a theoretical basis for elucidating the effects is absent. This study provides a solid theoretical deduction regarding the isotope fractionation taking place during fragmentation in EI-MS. Both intermolecular and intramolecular isotope fractionations present in deh...

  7. Intramolecular stable isotope distributions detect plant metabolic responses on century time scales

    Science.gov (United States)

    Schleucher, Jürgen; Ehlers, Ina; Augusti, Angela; Betson, Tatiana

    2014-05-01

    Plants respond to environmental changes on a vast range of time scales, and plant gas exchanges constitute important feedback mechanisms in the global C cycle. Responses on time scales of decades to centuries are most important for climate models, for prediction of crop productivity, and for adaptation to climate change. Unfortunately, responses on these timescale are least understood. We argue that the knowledge gap on intermediate time scales is due to a lack of adequate methods that can bridge between short-term manipulative experiments (e.g. FACE) and paleo research. Manipulative experiments in plant ecophysiology give information on metabolism on time scales up to years. However, this information cannot be linked to results from retrospective studies in paleo research, because little metabolic information can be derived from paleo archives. Stable isotopes are prominent tools in plant ecophysiology, biogeochemistry and in paleo research, but in all applications to date, isotope ratios of whole molecules are measured. However, it is well established that stable isotope abundance varies among intramolecular groups of biochemical metabolites, that is each so-called "isotopomer" has a distinct abundance. This intramolecular variation carries information on metabolic regulation, which can even be traced to individual enzymes (Schleucher et al., Plant, Cell Environ 1999). Here, we apply intramolecular isotope distributions to study the metabolic response of plants to increasing atmospheric [CO2] during the past century. Greenhouse experiments show that the deuterium abundance among the two positions in the C6H2 group of photosynthetic glucose depends on [CO2] during growth. This is observed for all plants using C3 photosynthesis, and reflects the metabolic flux ratio between photorespiration and photosynthesis. Photorespiration is a major C flux that limits assimilation in C3 plants, which encompass the overwhelming fraction of terrestrial photosynthesis and the

  8. Stable isotope fractionation in response to variable fluid residence time distributions

    Science.gov (United States)

    Druhan, J. L.; Maher, K.

    2013-12-01

    +) both in the fluid and mineral phase. The isotopic composition of the product species may be bounded if the fractionation factor and the rate of precipitation are known, and may be predicted accurately if the structure of the permeability field is also described. Such variability in the final steady state isotopic value and spatial distribution of a secondary mineral phase formed as a result of a fractionating reaction has important consequences for the interpretation of mineral phase isotopic compositions in subsurface environments. Maher, K. (2011) The role of fluid residence time and topographic scales in determining chemical fluxes from landscapes. Earth Planet. Sci. Lett., 312, 48 - 58.

  9. A case study of nitrification and nitrite isotope fractionation in a eutrophic temperate river system

    Science.gov (United States)

    Jacob, Juliane; Dähnke, Kirstin; Sanders, Tina

    2014-05-01

    Stable isotopes of nitrate are often used to assess processing of nitrate in the water column of oceans, estuaries, and rivers. In all these environments, nitrate regeneration via nitrification is an important source of new nitrate. The bulk isotope effect of nitrification is hard to predict: It is a two-step-process by distinct groups of microorganisms oxidizing ammonium to nitrate via nitrite. Both processes have divergent isotope effects, and it is even more difficult to unravel these effects in natural environments, because nitrite usually does not accumulate and isotope analysis is not possible. During our routine sampling scheme at the River Elbe an exceptional flood occurred in June 2013, and nitrite and ammonium accumulated, allowing us to investigate isotope fractionation of nitrification in a natural river system. We measured nutrient concentrations, dual nitrate isotopes, δ15N-NO2, and, where possible, δ15N-NH4. Nitrate leached from catchment area, and δ15N-NO3 and δ18O-NO3 decreased from typical spring bloom values (9.0 o and 3.5 o respectively) to winter nitrate background values (7.4 o and 2.1 o respectively). This indicates that riverine assimilation was minimal during the flood. Ammonium and nitrite concentrations increased to 12.5 μM and 5.7 μM, respectively, which likely was due to remineralization and nitrification in the water column. Ammonium δ15N-NH4 values increased up to 12 o and nitrite δ15N-NO2 values ranged from -4.8 o and -14.2 ‰Nitrite oxidation and decreasing concentrations were coupled with a fractionation factor 15ɛ of -8.6 o following normal, and not inverse, isotope fractionation. This deviates from findings in pure cultures of nitrite-oxidizing bacteria. We assume that the mechanisms responsible for inverse fractionation apply in natural environment as well, but that the resulting trend in δ15N-NO2 is masked by dilution with fresh nitrite stemming from ammonium oxidation. Our data are a first approximation of the

  10. Performance and limits of liquid chromatography isotope ratio mass spectrometry system for halogenated compounds

    Science.gov (United States)

    Gilevska, Tetyana; Gehre, Matthias; Richnow, Hans

    2014-05-01

    in the coil and increase in the concentration of radical but complete combustion of highly chlorinated or fluorinated compounds was not achieved. Due to these findings the limit for a LC-IRMS system for similar structure compounds can be predicted. 1. Elsner, M., et al., Current challenges in compound-specific stable isotope analysis of environmental organic contaminants. Analytical and Bioanalytical Chemistry, 2012. 403(9): p. 2471-2491. 2. Krummen, M., et al., A new concept for isotope ratio monitoring liquid chromatography/mass spectrometry. Rapid Communications in Mass Spectrometry, 2004. 18(19): p. 2260-2266.

  11. An empirical formula for isotopic yield in Fe + p spallation reactions

    Science.gov (United States)

    Ma, Chun-Wang; Xu, Jing-Li

    2017-12-01

    An empirical formula is proposed for predicting the cross sections of fragments in a spallation reaction. The cross sections of fragments measured in the 300, 500, 750, 1000 and 1500 MeV u‑1 56Fe + p spallation reactions are analysed. The mass and incident energy dependence of the isotopic yield have been considered in the empirical formula. The cross sections of fragments predicted by the proposed empirical formula and the spallation residue cross section (spacs) parameterizations have been compared to the experimental results, showing that both of them can predict the results well. The cross sections of fragments in the 1000 MeV u‑1 136Xe + p reactions can also be predicted by the proposed formula, while the spacs parameterizations significantly underestimate the measured results. The empirical formula is useful for predicting the yield of radioactive nuclei produced in proton therapy.

  12. Use of dual isotope tracers in biomedical research

    NARCIS (Netherlands)

    Stellaard, F

    Biomedical stable isotope studies involve administration of tracer and measurement of isotope enrichment in blood, urine, feces or breath. The aim of the studies is to gather quantitative information about a specific metabolic function. However, the measured isotope enrichment may be affected by

  13. Discovery of palladium, antimony, tellurium, iodine, and xenon isotopes

    CERN Document Server

    Kathawa, J; Thoennessen, M

    2012-01-01

    Currently, thirty-eight palladium, thirty-eight antimony, thirty-nine tellurium, thirty-eight iodine, and forty xenon isotopes have been observed and the discovery of these isotopes is discussed here. For each isotope a brief synopsis of the first refereed publication, including the production and identification method, is presented.

  14. Discovery of the astatine, radon, francium, and radium isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Fry, C.; Thoennessen, M., E-mail: thoennessen@nscl.msu.edu

    2013-09-15

    Thirty-nine astatine, thirty-nine radon, thirty-five francium, and thirty-four radium isotopes have so far been observed; the discovery of these isotopes is described. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  15. Discovery of the astatine, radon, francium, and radium isotopes

    CERN Document Server

    Fry, C

    2012-01-01

    Currently, thirty-nine astatine, thirty-nine radon, thirty-five francium, and thirty-four radium isotopes have so far been observed; the discovery of these isotopes is discussed. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  16. Discovery of the astatine, radon, francium, and radium isotopes

    Science.gov (United States)

    Fry, C.; Thoennessen, M.

    2013-09-01

    Thirty-nine astatine, thirty-nine radon, thirty-five francium, and thirty-four radium isotopes have so far been observed; the discovery of these isotopes is described. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  17. Discovery of Gallium, Germanium, Lutetium, and Hafnium Isotopes

    CERN Document Server

    Gross, J L

    2011-01-01

    Currently, twenty-eight gallium, thirty-one germanium, thirty-five lutetium, and thirty-six hafnium isotopes have been observed and the discovery of these isotopes is discussed here. For each isotope a brief synopsis of the first refereed publication, including the production and identification method, is presented.

  18. Towards a "perfect" Penning trap mass spectrometer for unstable isotopes

    Science.gov (United States)

    Bollen, G.; Hartmann, H.; Kluge, H.-J.; König, M.; Otto, T.; Savard, G.; Stolzenberg, H.; ISOLDE Collaboration

    1992-12-01

    A Penning trap mass spectrometer has been set up at the on-line isotope separator ISOLDE/CERN for the mass determination of unstable heavy isotopes. The spectrometer should fulfil the following requirements: capture of external ions in high efficiency, high resolving power and accuracy, general applicability to all elements and isotopes available at the on-line facility.

  19. 21 CFR 886.1670 - Ophthalmic isotope uptake probe.

    Science.gov (United States)

    2010-04-01

    ... 21 Food and Drugs 8 2010-04-01 2010-04-01 false Ophthalmic isotope uptake probe. 886.1670 Section... (CONTINUED) MEDICAL DEVICES OPHTHALMIC DEVICES Diagnostic Devices § 886.1670 Ophthalmic isotope uptake probe. (a) Identification. An ophthalmic isotope uptake probe is an AC-powered device intended to measure...

  20. Production and application of stable enriched isotopes in the USSR

    Energy Technology Data Exchange (ETDEWEB)

    Kudziev, A.G. (Institute of Stable Isotopes, Tbilisi (USSR))

    1989-10-01

    At present stable enriched isotopes are contributing essentially to the progress in many fields of sciences and national economy. The application of isotopically modified compounds and materials allowed to obtain a number of remarkable scientific results and initiated developments of great applied significance. This presentation will survey status and development activities involving enriched stable isotopes in the USSR. (orig.).

  1. Recent results on neutron rich tin isotopes by laser spectroscopy

    CERN Document Server

    Roussière, B; Crawford, J E; Essabaa, S; Fedosseev, V; Geithner, W; Genevey, J; Girod, M; Huber, G; Horn, R; Kappertz, S; Lassen, J; Le Blanc, F; Lee, J K P; Le Scornet, G; Lettry, Jacques; Mishin, V I; Neugart, R; Obert, J; Oms, J; Ouchrif, A; Peru, S; Pinard, J; Ravn, H L; Sauvage, J; Verney, D

    2001-01-01

    Laser spectroscopy measurements have been performed on neutron rich tin isotopes using the COMPLIS experimental setup. The nuclear charge radii of the even-even isotopes from A=108 to 132 are compared to the results of macroscopic and microscopic calculations. The improvements and optimizations needed to perform the isotope shift measurement on $^{134}$Sn are presented.

  2. Final Report on Isotope Ratio Techniques for Light Water Reactors

    Energy Technology Data Exchange (ETDEWEB)

    Gerlach, David C.; Gesh, Christopher J.; Hurley, David E.; Mitchell, Mark R.; Meriwether, George H.; Reid, Bruce D.

    2009-07-01

    The Isotope Ratio Method (IRM) is a technique for estimating the energy or plutonium production in a fission reactor by measuring isotope ratios in non-fuel reactor components. The isotope ratios in these components can then be directly related to the cumulative energy production with standard reactor modeling methods.

  3. Stable Isotope Characteristics of Akiri Vein Copper Mineralization ...

    African Journals Online (AJOL)

    The Akiri vein copper mineralization was investigated for its carbon and oxygen isotopic composition to determine the characteristics of the mineralizing fluid. Carbon and oxygen isotope analyses of Akiri siderite range between δ13C values (-1.05 to -1.71‰) and δ13O values (-14.94 to -15.18) respectively. δ 13C isotopic ...

  4. Atmospheric Argon Isotope Evolution Informed by MAVEN Results

    Science.gov (United States)

    Slipski, M.; Jakosky, B. M.; Benna, M.; Mahaffy, P.; Elrod, M. K.

    2017-10-01

    Mars' atmosphere is enriched in heavy isotopes of its major species. We have modeled the evolution of Ar isotopes of 4 Gyr due to volcanic outgassing and loss to space, using MAVEN results to constrain how sputtering loss fractionates Ar isotopes.

  5. Assessing the ability of isotope-enabled General Circulation Models to simulate the variability of Iceland water vapor isotopic composition

    Science.gov (United States)

    Erla Sveinbjornsdottir, Arny; Steen-Larsen, Hans Christian; Jonsson, Thorsteinn; Ritter, Francois; Riser, Camilla; Messon-Delmotte, Valerie; Bonne, Jean Louis; Dahl-Jensen, Dorthe

    2014-05-01

    During the fall of 2010 we installed an autonomous water vapor spectroscopy laser (Los Gatos Research analyzer) in a lighthouse on the Southwest coast of Iceland (63.83°N, 21.47°W). Despite initial significant problems with volcanic ash, high wind, and attack of sea gulls, the system has been continuously operational since the end of 2011 with limited down time. The system automatically performs calibration every 2 hours, which results in high accuracy and precision allowing for analysis of the second order parameter, d-excess, in the water vapor. We find a strong linear relationship between d-excess and local relative humidity (RH) when normalized to SST. The observed slope of approximately -45 o/oo/% is similar to theoretical predictions by Merlivat and Jouzel [1979] for smooth surface, but the calculated intercept is significant lower than predicted. Despite this good linear agreement with theoretical calculations, mismatches arise between the simulated seasonal cycle of water vapour isotopic composition using LMDZiso GCM nudged to large-scale winds from atmospheric analyses, and our data. The GCM is not able to capture seasonal variations in local RH, nor seasonal variations in d-excess. Based on daily data, the performance of LMDZiso to resolve day-to-day variability is measured based on the strength of the correlation coefficient between observations and model outputs. This correlation coefficient reaches ~0.8 for surface absolute humidity, but decreases to ~0.6 for δD and ~0.45 d-excess. Moreover, the magnitude of day-to-day humidity variations is also underestimated by LMDZiso, which can explain the underestimated magnitude of isotopic depletion. Finally, the simulated and observed d-excess vs. RH has similar slopes. We conclude that the under-estimation of d-excess variability may partly arise from the poor performance of the humidity simulations.

  6. Tracing increasing tropical Andean glacier melt with stable isotopes in water.

    Science.gov (United States)

    Mark, Bryan G; Mckenzie, Jeffrey M

    2007-10-15

    Glaciers in the tropical Andes are undergoing rapid retreat with potentially devastating consequences for populations who rely on them for water resources. We measured stable water isotope ratios in synoptically sampled streams discharging from glacierized watersheds to associate hydroisotopic variation with relative changes in glacierized area. A total of 73 water samples were collected from hydrological endmembers including streams, glacier meltwater, and groundwater during the dry seasons of 2004-2006 in the Callejon de Huaylas, a 5000 km2 watershed that drains the western side of the Cordillera Blanca in northern Perú. To differentiate the influence of elevation on isotopic values, we use samples from shallow groundwater springs and nonglacierized subcatchments to derive a local meteoric elevation effect. From published historical runoff data and satellite-mapped glacier cover, we estimate an average increase of 1.6 (+/-1.1)% in the specific discharge of the glacierized catchments as a function of isotopic changes from 2004 to 2006. These results confirm predicted short-term increases in discharge as glaciers melt and demonstrate the utility of stable isotopes in water for tracing relative glacier melt water contributions to watersheds.

  7. Arctic cyclone water vapor isotopes support past sea ice retreat recorded in Greenland ice.

    Science.gov (United States)

    Klein, Eric S; Cherry, J E; Young, J; Noone, D; Leffler, A J; Welker, J M

    2015-05-29

    Rapid Arctic warming is associated with important water cycle changes: sea ice loss, increasing atmospheric humidity, permafrost thaw, and water-induced ecosystem changes. Understanding these complex modern processes is critical to interpreting past hydrologic changes preserved in paleoclimate records and predicting future Arctic changes. Cyclones are a prevalent Arctic feature and water vapor isotope ratios during these events provide insights into modern hydrologic processes that help explain past changes to the Arctic water cycle. Here we present continuous measurements of water vapor isotope ratios (δ(18)O, δ(2)H, d-excess) in Arctic Alaska from a 2013 cyclone. This cyclone resulted in a sharp d-excess decrease and disproportional δ(18)O enrichment, indicative of a higher humidity open Arctic Ocean water vapor source. Past transitions to warmer climates inferred from Greenland ice core records also reveal sharp decreases in d-excess, hypothesized to represent reduced sea ice extent and an increase in oceanic moisture source to Greenland Ice Sheet precipitation. Thus, measurements of water vapor isotope ratios during an Arctic cyclone provide a critical processed-based explanation, and the first direct confirmation, of relationships previously assumed to govern water isotope ratios during sea ice retreat and increased input of northern ocean moisture into the Arctic water cycle.

  8. Technical note: A linear model for predicting δ13 Cprotein.

    Science.gov (United States)

    Pestle, William J; Hubbe, Mark; Smith, Erin K; Stevenson, Joseph M

    2015-08-01

    Development of a model for the prediction of δ(13) Cprotein from δ(13) Ccollagen and Δ(13) Cap-co . Model-generated values could, in turn, serve as "consumer" inputs for multisource mixture modeling of paleodiet. Linear regression analysis of previously published controlled diet data facilitated the development of a mathematical model for predicting δ(13) Cprotein (and an experimentally generated error term) from isotopic data routinely generated during the analysis of osseous remains (δ(13) Cco and Δ(13) Cap-co ). Regression analysis resulted in a two-term linear model (δ(13) Cprotein (%) = (0.78 × δ(13) Cco ) - (0.58× Δ(13) Cap-co ) - 4.7), possessing a high R-value of 0.93 (r(2)  = 0.86, P < 0.01), and experimentally generated error terms of ±1.9% for any predicted individual value of δ(13) Cprotein . This model was tested using isotopic data from Formative Period individuals from northern Chile's Atacama Desert. The model presented here appears to hold significant potential for the prediction of the carbon isotope signature of dietary protein using only such data as is routinely generated in the course of stable isotope analysis of human osseous remains. These predicted values are ideal for use in multisource mixture modeling of dietary protein source contribution. © 2015 Wiley Periodicals, Inc.

  9. Isotope fingerprinting of precipitation associated with western ...

    Indian Academy of Sciences (India)

    Ghulam Jeelani

    2017-11-22

    Nov 22, 2017 ... by geographic factors such as altitude, latitude, moisture source, and transport process (e.g., Craig. 1961; Siegenthaler and Oeschger 1980; Gat 1996; ..... cel over the continent, its isotopic composition is expected to change from its initial value due to various processes like picking up of locally recycled.

  10. Isotope specific arbitrary material flow meter

    Science.gov (United States)

    Barty, Christopher P. J.; Post, John C.; Jones, Edwin

    2016-10-25

    A laser-based mono-energetic gamma-ray source is used to provide non-destructive and non-intrusive, quantitative determination of the absolute amount of a specific isotope contained within pipe as part of a moving fluid or quasi-fluid material stream.

  11. Isotope effects on the crotonase reaction

    Energy Technology Data Exchange (ETDEWEB)

    Bahnson, B.J.; Anderson, V.E. (Brown Univ., Providence, RI (USA))

    1989-05-16

    The primary, alpha-secondary, beta-secondary, and beta'-secondary deuterium and primary 18O kinetic isotope effects on V/K for the dehydration of ((3S)-3-hydroxybutyryl)pantetheine by bovine liver crotonase (enoyl-CoA hydratase, EC 4.2.1.17) have been determined by the equilibrium perturbation method. The primary deuterium and 18O kinetic isotope effects are 1.61 and 1.051, respectively. The secondary deuterium effects at C-2, C-3, and C-4 are 1.12, 1.13, and 1.00 per H, respectively. The large 18O isotope effect suggests C-O bond cleavage is largely rate determining but is consistent with either an E1cb or E2 mechanism with a large amount of carbanion character. The beta-secondary effect is a factor of 1.05 greater than the equilibrium isotope effect, indicating that this C-H bond is less stiff in the affected transition state or that its motion is coupled to the reaction coordinate motion. Analytical solutions to the differential equations describing uni-uni equilibrium perturbations are presented.

  12. Seabird modulations of isotopic nitrogen on islands.

    Directory of Open Access Journals (Sweden)

    Stéphane Caut

    Full Text Available The transport of nutrients by migratory animals across ecosystem boundaries can significantly enrich recipient food webs, thereby shaping the ecosystems' structure and function. To illustrate the potential role of islands in enabling the transfer of matter across ecosystem boundaries to be gauged, we investigated the influence of seabirds on nitrogen input on islands. Basing our study on four widely differing islands in terms of their biogeography and ecological characteristics, sampled at different spatial and temporal intervals, we analyzed the nitrogen isotopic values of the main terrestrial ecosystem compartments (vascular plants, arthropods, lizards and rodents and their relationship to seabird values. For each island, the isotopic values of the ecosystem were driven by those of seabirds, which ultimately corresponded to changes in their marine prey. First, terrestrial compartments sampled within seabird colonies were the most enriched in δ(15N compared with those collected at various distances outside colonies. Second, isotopic values of the whole terrestrial ecosystems changed over time, reflecting the values of seabirds and their prey, showing a fast turnover throughout the ecosystems. Our results demonstrate that seabird-derived nutrients not only spread across the terrestrial ecosystems and trophic webs, but also modulate their isotopic values locally and temporally on these islands. The wealth of experimental possibilities in insular ecosystems justifies greater use of these model systems to further our understanding of the modalities of trans-boundary nutrient transfers.

  13. Use of Isotopes for Studying Reaction Mechanisms

    Indian Academy of Sciences (India)

    titative measurements of equilibrium and kinetic isotope effects. In this part, we describe an ingenious way of studying ... is whether the structure obtained is the preferred one or just the superposition of some other equilibrating structures. ... Ammonia is a pyramidal molecule, but it undergoes rapid umbrella inversion. On the ...

  14. Function and application of isotope controlled materials

    Energy Technology Data Exchange (ETDEWEB)

    Yagi, Koichi; Suzuki, Hiroshi; Araki, Hiroshi; Fujita, Mitsutane; Hirano, Toshiyuki; Numazawa, Takenori; Noda, Tetsuji [National Research Inst. for Metals, Tsukuba, Ibaraki (Japan)

    2000-02-01

    As large amounts of silicone isotopes were separated in previous research, we tried to develop function of isotope controlled materials. Molecular vibration excitation control to control laser wavelength, physical properties of isotope control materials and nuclear transformation function were studied. A gas circulation system for isotope laser development was manufactured. When a part of {sup 16}O in CO{sub 2} were changed by {sup 18}O, the stretching mode of CO{sub 2} became unsymmetrical mode. P17 and P19 of laser oscillation were observed. They are odd lines that have never been observed. SiF{sub 4} and Si{sub 2}F{sub 6} were decomposed by plasma CVD method. About 28% Si crystal was obtained by controlling the reaction temperature at about 350 to 450degC. Homogeneous P single crystal(100) with 10 mm diameter was obtained. Thermal conductivity of B single crystal with {sup 10}B showed 1.5 times as much as that of natural components. Calculation of displacement damages, change of components, induced radioactivity and decay heat were improved by arrangement of simulation code. (S.Y.)

  15. Tomographic, hydrochemical and isotopic investigations of the ...

    Indian Academy of Sciences (India)

    An electrical imaging tomography survey was carried out to identify the lateral and vertical salinity distribution in the oasis shallow aquifers of the Nefzaoua region located in southwestern Tunisia. In addition, hydrochemical and isotopic data were examined to determine the main factors and mechanisms controlling the ...

  16. Stable carbon isotope analysis of coprocessing materials

    Energy Technology Data Exchange (ETDEWEB)

    Burke, F. P.; Winschel, R. A.; Lancet, M. S.

    1989-06-01

    The program is designed to address a substantial, demonstrated need of the coprocessing community (both exploratory and development) for a technique to quantitatively distinguish the contributions of the individual coprocessing feedstocks to the various products. The carbon isotope technique is currently in routine use for other applications. Results achieved this quarter include: Feed and product fractions from a Kentucky 9 coal/Kentucky tar sand bitumen coprocessing bench unit run at the Kentucky Center for Applied Energy Research (CAER) were analyzed for carbon isotope ratios. Corrections were made to the coal carbon recoveries and selectivities from the products of HRI Run 227-53. Feeds (Westerholt coal/Cold Lake VSB) and products from two periods of HRI coprocessing Run 238-1 were analyzed. Three petroleum samples and three coal samples were pyrolyzed at 800{degree}F for 30 min to determine the effect of pyrolysis on the isotopic homogeneity of each petroleum and coal sample. Products from each pyrolysis test were separated into five fractions; an additional set of coprocessing samples and a set of two-stage coal liquefaction samples were obtained from HRI for future work; work performed by the Pennsylvania State University show that microscopy is a promising method for distinguishing coal and petroleum products in residual coprocessing materials; and coal and petroleums that have large differences in carbon isotope ratios were identified for Auburn University. 7 refs., 2 figs., 12 tabs.

  17. Geochemistry of the stable isotopes of silicon

    Energy Technology Data Exchange (ETDEWEB)

    Douthitt, C.B. (California Inst. of Tech., Pasadena (USA). Div. of Geological and Planetary Sciences)

    1982-08-01

    One hundred thirty two new measurements of the relative abundances of the stable isotopes of silicon in terrestrial materials are presented. The total variation of delta/sup 30/Si found is 6.2 parts per thousand, centered on the mean of terrestrial mafic and ultramafic igneous rocks, delta/sup 30/Si = -0.4 parts per thousand. Igneous rocks show limited variation; coexisting minerals exhibit small, systematic silicon isotopic fractionations that are roughly 1/3 the magnitude of concomitant oxygen isotopic fractionations at 1150/sup 0/C. In both igneous minerals and rocks, delta/sup 30/Si shows a positive correlation with silicon content, as does delta/sup 18/O. Opal from both sponge spicules and sinters is light, with delta/sup 30/Si = -2.3 and -1.4 parts per thousand respectively. Large delta/sup 30/Si values of both positive and negative sign are reported for the first time from clay minerals, opaline phytoliths, and authigenic quartz. All highly fractionated samples were precipitated from solution at low temperatures; however, aqueous silicon is not measurably fractionated relative to quartz at equilibrium. A kinetic isotope fractionation of approximately 3.5 parts per thousand is postulated to occur during the low temperature precipitation of opal and, possibly, poorly ordered phyllosilicates, with the silicate phase being enriched in /sup 28/Si. This fractionation, coupled with a Rayleigh precipitation model, is capable of explaining most non-magmatic delta/sup 30/Si variations.

  18. Use of Isotopes for Studying Reaction Mechanisms

    Indian Academy of Sciences (India)

    Home; Journals; Resonance – Journal of Science Education; Volume 2; Issue 10. Use of Isotopes for Studying Reaction Mechanisms Distinguishing between Single Minima and Rapidly Equilibrating Structures. Uday Maitra J Chandrasekhar. Series Article Volume 2 Issue 10 October 1997 pp 29-37 ...

  19. Use of Isotopes for Studying Reaction Mechanisms

    Indian Academy of Sciences (India)

    Home; Journals; Resonance – Journal of Science Education; Volume 16; Issue 12. Use of Isotopes for Studying Reaction Mechanisms - Distinguishing between Single Mimima and Rapidly Equilibrating Structures. Uday Maitra J Chandrasekhar. Volume 16 Issue 12 December 2011 pp 1315-1323 ...

  20. Exploring the calcium isotope signature of

    NARCIS (Netherlands)

    Hippler, D.; Witbaard, R.; van Aken, H.M.; Buhl, D.; Immenhauser, A.

    2013-01-01

    The calcium-isotope composition (delta Ca-44/40) of the aragonitic bivalve Arctica islandica grown in laboratory and field cultures was investigated in terms of environmental and biological controls to explore its potential as a palaeoceanographic proxy. While we found no significant effect of

  1. Pb isotopes during mingling and melting

    DEFF Research Database (Denmark)

    Waight, Tod Earle; Lesher, Charles E.

    2010-01-01

    Pb isotopic data are presented for hybrid rocks formed by mingling between mantle-derived tholeiitic magma of the Eocene Miki Fjord macrodike (East Greenland) and melt derived from the adjacent Precambrian basement. Bulk mixing and AFC processes between end-members readily identified in the field...

  2. Methodology for the Validation of Isotopic Analyses by Mass Spectrometry in Stable-Isotope Labeling Experiments.

    Science.gov (United States)

    Heuillet, Maud; Bellvert, Floriant; Cahoreau, Edern; Letisse, Fabien; Millard, Pierre; Portais, Jean-Charles

    2018-02-06

    Stable-isotope labeling experiments (ILEs) are widely used to investigate the topology and operation of metabolic networks. The quality of isotopic data collected in ILEs is of utmost importance to ensure reliable biological interpretations, but current evaluation approaches are limited due to a lack of suitable reference material and relevant evaluation criteria. In this work, we present a complete methodology to evaluate mass spectrometry (MS) methods used for quantitative isotopic studies of metabolic systems. This methodology, based on a biological sample containing metabolites with controlled labeling patterns, exploits different quality metrics specific to isotopic analyses (accuracy and precision of isotopologue masses, abundances, and mass shifts and isotopic working range). We applied this methodology to evaluate a novel LC-MS method for the analysis of amino acids, which was tested on high resolution (Orbitrap operating in full scan mode) and low resolution (triple quadrupole operating in multiple reaction monitoring mode) mass spectrometers. Results show excellent accuracy and precision over a large working range and revealed matrix-specific as well as mode-specific characteristics. The proposed methodology can identify reliable (and unreliable) isotopic data in an easy and straightforward way and efficiently supports the identification of sources of systematic biases as well as of the main factors that influence the overall accuracy and precision of measurements. This approach is generic and can be used to validate isotopic analyses on different matrices, analytical platforms, labeled elements, or classes of metabolites. It is expected to strengthen the reliability of isotopic measurements and thereby the biological value of ILEs.

  3. Mg Isotopes of USGS Igneous Rock Standards

    Science.gov (United States)

    Huang, F.; Glessner, J. J.; Lundstrom, C. C.

    2008-12-01

    Magnesium has three stable isotopes, 24Mg, 25Mg, and 26Mg with abundances of 78.99%, 10.00%, and 11.01%, respectively. It is one of the most abundant elements in the crust and mantle. As advancements of analytical techniques using MC-ICP-MS have dramatically advanced our ability to measure isotope ratios of Mg with greater precision, Mg isotopes can now be applied to study a variety of fundamental geological processes, such as continental crust weathering, chemical diffusion, and chondrule formation. Therefore the need for well characterized Mg isotope ratios for geological materials is increasingly important. Routine measurement of readily-available USGS rock standards is a viable way for inter-lab comparison to show the quality of data. However, the Mg isotope data for USGS standards reported in the literature are limited and inconsistent. USGS standards reported by different MC-ICP-MS labs have a range of Mg isotopic data outside of the normal external error of 0.1‰ (2σ). Mg isotopes of USGS igneous rock standards (dunite, DTS-1; basalts, BCR-1, BCR-2, BHVO-1; and andesite, AGV-1) were measured by a sample-standard bracketing method using a low resolution MC-ICP- MS (Nu-Plasma HR). The method has a large tolerance of matrix bias with Na/Mg and Al/Mg > 100% only changing the δ26Mg by less than 0.1‰. Dilution effects do not cause significant error (99.5%) and acceptable concentrations of matrix (mainly Na, Al, Ca, and Fe) are included in these results. Duplicate analyses of independently processed standards yielded the following results (δ26MgDSM-3 (‰)): BCR-2 (-0.306±0.144, - 0.290±0.116, -0.283±0.048, -0.288±0.057), BCR-1 (-0.399±0.079, -0.346±0.046), AGV-1 (-0.295±0.110, -0.307±0.086, -0.339±0.068), BHVO-1 (-0.308±0.076, - 0.299±0.103), and DTS-1 (-0.299±0.163, -0.368±0.059). δ26MgDSM-3 of measured USGS standards are consistent within error (2σ).

  4. Iron Isotope Fractionation in Artic Weathering Environments

    Science.gov (United States)

    Rouxel, O. J.; Escoube, R.; Pokrovsky, O. S.; Wisch, M.; Miller, C.

    2008-12-01

    While our current knowledge of Fe isotope systematics in rivers is still limited, Fe isotopes provide a new approach to important questions concerning Fe sources, Fe speciation and its bioavailability in the hydrological cycles. Here, we investigated several Arctic rivers for elemental and Fe-isotopic composition with specific emphasis on silicate weathering and organic C content in order to provide new insights into the delivery of trace nutrients, such as Fe, that are important for the biological productivity of the Arctic Ocean. Without such characterization of the present state of the system, future changes in the response of these river systems to global change cannot be properly evaluated. Our Fe isotope systematics results in Siberian rivers, include (1) a time-series of water samples from large rivers (Ob and Lena) focusing on the peak flow that has not yet been investigated despite its critical importance for annual budgets; (2) the colloidal fractions (1 kDa to 0.45 μm) of rivers and their estuaries in the White Sea, including the Severnaya Dvina River to assess the influence of Fe-rich colloids flocculation on the Fe isotopic composition of the estuarine waters. Dissolved iron fractions (ice break-up on the rivers. In contrast, dissolved iron fractions in the Severnaya Dvina River and its tributaries yield more positive δ56Fe values, with values ranging from -0.09 to up to 0.64‰, averaging 0.2‰ (n=19). Small swamp rivers from the South White Sea coast reveal an even higher spread of dissolved δ56Fe values, from -1.1 to +0.8‰ with some clear variations among the various colloidal fractions (1 kDa-10 kDa - 100 kDa). These results, together with the high Fe and DOC concentrations in the water samples, suggest that Fe-redox cycling in soil aquifer, as well as the formation of organic-rich colloids, may impart specific Fe-isotope signatures in dissolved Fe reaching the Artic Ocean. Recent studies (e.g. Fantle and De Paolo, 2004 and Bergquist and

  5. The Valanginian terrestrial carbon-isotope record

    Science.gov (United States)

    Grocke, D. R.; Price, G. D.; Baraboshkin, E.; Mutterlose, J.; Ruffell, A. H.

    2003-04-01

    A stratigraphic, biostratigraphic and isotopic investigation has been performed on a Crimean section located on the Kacha River, Verkhorechie Village, SW Crimea. This clastic-dominated succession consists of a series of bioturbated inter-bedded shallow-marine silty sands, claystones and some oolitic sands. A published detailed study of the ammonite fauna has been undertaken and has revealed that the succession can be compared to standard Tethyan schemes. The lower part of the succession is dated on the basis of the ammonite fauna as Early Valanginian (otopeta-campylotoxus ammonite Zones), although this latter zone is highly condensed. A more expanded Late Valanginian is present (verrucosum, callidiscus and tauricum ammonite Zones), and is overlain by sand-dominated sediments of Early Hauterivian age. Throughout this section woody plant matter ranging in preservation from charcoal to coal has been collected and analyzed for stable carbon-isotope ratios. There is no correlation between state of preservation and carbon-isotope ratios. Carbon-isotope ratios range in the Early Valanginian from -24 ppm to -22 ppm, and in the mid-verrucosum Zone values shift abruptly towards more positive values and peak at -18 ppm in the lower callidiscus Zone. Wood carbon-isotope ratios decrease gradually through the remainder of the callidiscus Zone and return to pre-excursion values in the tauricum Zone. The remaining Hauterivian values fluctuate between -24 ppm to -21 ppm. The structure, magnitude and timing of the terrestrial carbon-isotope curve is very similar to the marine carbonate curve (from +1 ppm to +3 ppm) for the Valanginian. This would indicate, based on a delta-delta relationship between organic matter and carbonate, that there was very little change in atmospheric CO_2 concentrations during the Valanginian, and that the isotopic composition of the global carbon reservoir shifted. Future research on an Early Cretaceous (Valanginian-Hauterivian) interval from the Yatria

  6. Free Air Respiratory Carbon Isotope Enrichment Experiment

    Science.gov (United States)

    Sternberg, L. D.; Greaver, T.; Schaffer, B.; Moreno, T.

    2003-12-01

    Recycling of respiratory carbon in canopies is difficult to measure. Other than a steady state model, there are currently no direct methods of measuring recycling. Respiratory carbon recycling not only will affect the carbon isotope ratio signature of the canopy, but is also important in partitioning gross photosynthesis and respiration from net ecosystem exchange (NEE). In order to better understand recycling, we empirically derived an integrated measure of recycling in a cover crop (Crotalaria juncea L.) and compared it with that derived by the steady state model. A measured dose of nitrogen gas having CO2 with a high Carbon-13 abundance (41%) was applied at ground level ( ˜10 cm above the soil surface) with a system of hoses in a 10 by 10 m plot embedded in a 30 by 30 m plot. We adjusted the flux rate of this enriched gas weekly to correspond to weekly measurements of soil respiration rates. The gas application rates at ground level were sufficiently low so as to not affect the carbon dynamics of the treatment plot relative to that of a control plot with only nitrogen (no CO2) applied. The isotopic composition of the applied gas, however, was high enough to significantly increase the isotopic composition of respired CO2. Using the carbon isotopic composition of respiration and biomass from the control and treatment plots and mass balance principles we calculated that 45% of the total respired CO2 is recycled by this crop, which compares well with that derived by the steady state model (48%). Partitioning of gross photosynthesis and respiration by isotopic methods usually assumes no recycling. Recycling, however, will have an effect on the isotopic composition of respired CO2. After correcting for the recycling effects on the carbon isotope ratios of respired CO2 leaving the canopy, we calculated that the average gross photosynthesis for this crop was 40.4μ moles/m2s and gross respiration was in the order of 17.8 μ moles/m2s. These values are similar to those

  7. Iron isotope systematics in planetary reservoirs

    Science.gov (United States)

    Sossi, Paolo A.; Nebel, Oliver; Foden, John

    2016-10-01

    Iron is the only polyvalent major element, and controls reduction-oxidation (redox) reactions in a host of geologic processes and reservoirs, from the mineral- to planetary-scale, on Earth and in space. Mass transfer of Fe is often accompanied by changes in bonding environment, meaning the resultant variation in bond-strength in crystals, liquids and gases induces stable isotope fractionation, even at high temperatures. In the absence of iron exchange, electron transfer can also affect iron's valence state and calculated oxygen fugacity (fO2), however its isotope composition remains unchanged. Thus, iron isotopes are a powerful tool to investigate processes that involve mass transfer, redox reactions and changes in bonding environment in planetary systems. Primitive chondritic meteorites show remarkable isotopic homogeneity, δ57 Fe = - 0.01 ± 0.01 ‰ (2SE), over a wide range of Fe/Mg vs Ni/Mg, a proxy for fO2 in the solar nebula. In chondrites, there are iron isotope differences between metal and silicates that become more pronounced at higher metamorphic grades. However, on a planetary scale, Mars and Vesta overlap with chondrites, preserving no trace of core formation or volatile depletion on these bodies. Upon assessment of pristine lherzolites, the Bulk Silicate Earth is heavier than chondrites (δ57 Fe = + 0.05 ± 0.01 ‰; 2SE), and similar to or slightly lighter than the Moon. That the mantles of some differentiated inner solar system bodies extend to heavier compositions (+ 0.2 ‰) than chondrites may principally result from volatile depletion either at a nebular or late accretion stage. Within terrestrial silicate reservoirs, iron isotopes provide insight into petrogenetic and geodynamic processes. Partial melting of the upper mantle produces basalts that are heavier than their sources, scaling with degree of melting and driving the increasingly refractory peridotite to lighter compositions. Mid-Ocean Ridge Basalts (MORBs) are homogeneous to δ57 Fe

  8. Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry.

    Science.gov (United States)

    Hartig, Kyle C; Ghebregziabher, Isaac; Jovanovic, Igor

    2017-03-08

    The ability to perform not only elementally but also isotopically sensitive detection and analysis at standoff distances is impor-tant for remote sensing applications in diverse ares, such as nuclear nonproliferation, environmental monitoring, geophysics, and planetary science. We demonstrate isotopically sensitive real-time standoff detection of uranium by the use of femtosecond filament-induced laser ablation molecular isotopic spectrometry. A uranium oxide molecular emission isotope shift of 0.05 ± 0.007 nm is reported at 593.6 nm. We implement both spectroscopic and acoustic diagnostics to characterize the properties of uranium plasma generated at different filament-uranium interaction points. The resulting uranium oxide emis-sion exhibits a nearly constant signal-to-background ratio over the length of the filament, unlike the uranium atomic and ionic emission, for which the signal-to-background ratio varies significantly along the filament propagation. This is explained by the different rates of increase of plasma density and uranium oxide density along the filament length resulting from spectral and temporal evolution of the filament along its propagation. The results provide a basis for the optimal use of filaments for standoff detection and analysis of uranium isotopes and indicate the potential of the technique for a wider range of remote sensing applications that require isotopic sensitivity.

  9. Determination of porphyrin carbon isotopic composition using gas chromatography-isotope ratio monitoring mass spectrometry.

    Science.gov (United States)

    Yu, Z; Sheng, G; Fu, J; Peng, P

    2000-12-01

    Carbon isotopic compositions of aetio I occurring in the form of free-base, nickel, demetallation, dihydroxysilicon(IV) and bis(tert.-butyldimethylsiloxy)silicon(IV) [(tBDMSO)2Si(IV)] have shown that it has experienced no obvious isotope fractionation during the synthesis of [(tBDMSO)2Si(IV)] porphyrin from aetio I. Here, aetio I porphyrin species such as free-base, nickel, demetallated and dihydroxysilicon were analyzed by the conventional method, namely it is combusted in sealed system, and followed by isotope ratio monitoring mass spectrometric analysis. [(tBDMSO)2Si(IV)] aetio I was assayed by gas chromatography-isotope ratio monitoring mass spectrometry (GC-IRMS). A porphyrin mixture of [(tBDMSO)2Si(IV)] aetio I and octaethylporphyrin was also prepared. Their carbon isotopic compositions measured by GC-IRMS indicate that no isotope exchange took place between the porphyrins during the synthesis of [(tBDMSO)2Si(IV)] porphyrins. This method is employed for delta13C determination of geoporphyrins from the Maoming and Jianghan oil shales.

  10. Carbon isotope ratios and isotopic correlations between components in fruit juices

    Science.gov (United States)

    Wierzchnicki, Ryszard

    2013-04-01

    Nowadays food products are defined by geographical origin, method of production and by some regulations concerning terms of their authenticity. Important data for confirm the authenticity of product are providing by isotopic methods of food control. The method checks crucial criteria which characterize the authenticity of inspected product. The European Union Regulations clearly show the tendency for application of the isotopic methods for food authenticity control (wine, honey, juice). The aim of the legislation steps is the protection of European market from possibility of the commercial frauds. Method of isotope ratio mass spectrometry is very effective tool for the use distinguishably the food products of various geographical origin. The basic problem for identification of the sample origin is the lack of databases of isotopic composition of components and information about the correlations of the data. The subject of the work was study the isotopic correlations existing between components of fruits. The chemical and instrumental methods of separation: water, sugars, organic acids and pulp from fruit were implemented. IRMS technique was used to measure isotopic composition of samples. The final results for original samples of fruits (apple, strawberry etc.) will be presented and discussed. Acknowledgement: This work was supported by the Polish Ministry of Science and Higher Education under grant NR12-0043-10/2010.

  11. Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry

    Science.gov (United States)

    Hartig, Kyle C.; Ghebregziabher, Isaac; Jovanovic, Igor

    2017-03-01

    The ability to perform not only elementally but also isotopically sensitive detection and analysis at standoff distances is impor-tant for remote sensing applications in diverse ares, such as nuclear nonproliferation, environmental monitoring, geophysics, and planetary science. We demonstrate isotopically sensitive real-time standoff detection of uranium by the use of femtosecond filament-induced laser ablation molecular isotopic spectrometry. A uranium oxide molecular emission isotope shift of 0.05 ± 0.007 nm is reported at 593.6 nm. We implement both spectroscopic and acoustic diagnostics to characterize the properties of uranium plasma generated at different filament-uranium interaction points. The resulting uranium oxide emis-sion exhibits a nearly constant signal-to-background ratio over the length of the filament, unlike the uranium atomic and ionic emission, for which the signal-to-background ratio varies significantly along the filament propagation. This is explained by the different rates of increase of plasma density and uranium oxide density along the filament length resulting from spectral and temporal evolution of the filament along its propagation. The results provide a basis for the optimal use of filaments for standoff detection and analysis of uranium isotopes and indicate the potential of the technique for a wider range of remote sensing applications that require isotopic sensitivity.

  12. Isotopic evidence of early hominin diets

    Science.gov (United States)

    Sponheimer, Matt; Alemseged, Zeresenay; Cerling, Thure E.; Grine, Frederick E.; Kimbel, William H.; Leakey, Meave G.; Lee-Thorp, Julia A.; Kyalo Manthi, Fredrick; Reed, Kaye E.; Wood, Bernard A.; Wynn, Jonathan G.

    2013-06-01

    Carbon isotope studies of early hominins from southern Africa showed that their diets differed markedly from the diets of extant apes. Only recently, however, has a major influx of isotopic data from eastern Africa allowed for broad taxonomic, temporal, and regional comparisons among hominins. Before 4 Ma, hominins had diets that were dominated by C3 resources and were, in that sense, similar to extant chimpanzees. By about 3.5 Ma, multiple hominin taxa began incorporating 13C-enriched [C4 or crassulacean acid metabolism (CAM)] foods in their diets and had highly variable carbon isotope compositions which are atypical for African mammals. By about 2.5 Ma, Paranthropus in eastern Africa diverged toward C4/CAM specialization and occupied an isotopic niche unknown in catarrhine primates, except in the fossil relations of grass-eating geladas (Theropithecus gelada). At the same time, other taxa (e.g., Australopithecus africanus) continued to have highly mixed and varied C3/C4 diets. Overall, there is a trend toward greater consumption of 13C-enriched foods in early hominins over time, although this trend varies by region. Hominin carbon isotope ratios also increase with postcanine tooth area and mandibular cross-sectional area, which could indicate that these foods played a role in the evolution of australopith masticatory robusticity. The 13C-enriched resources that hominins ate remain unknown and must await additional integration of existing paleodietary proxy data and new research on the distribution, abundance, nutrition, and mechanical properties of C4 (and CAM) plants.

  13. Strontium-isotope stratigraphy of Enewetak Atoll

    Science.gov (United States)

    Ludwig, K. R.; Halley, Robert B.; Simmons, Kathleen R.; Peterman, Zell E.

    1988-01-01

    87Sr/86Sr ratios determined for samples from a 350 m core of Neogene lagoonal, shallow-water limestones from Enewetak Atoll display a remarkably informative trend. Like the recently published data for Deep Sea Drilling Project (DSDP) carbonates, 87Sr/86Sr at Enewetak increases monotonically but not smoothly from the early Miocene to the Pleistocene. The data show intervals of little or no change in 87Sr/86Sr, punctuated by sharp transitions to lower values toward greater core depths. The sharp transitions correlate with observed solution disconformities caused by periods of subaerial erosion, whereas the intervals of little or no change in 87Sr/86Sr correspond to intervals of rapid accumulation of shallow-water carbonate sediments. When converted to numerical ages using the published DSDP 590B trend, the best-resolved time breaks are at 282 m (12.3 to 18.2 Ma missing) and 121.6 m (3.0 to 5.3 Ma missing) below the lagoon floor. At Enewetak, Sr isotopes offer a stratigraphic resolution for these shallow-marine Neogene carbonates comparable to that of nannofossil zonation in deep-sea carbonates (0.3-3 m.y.). In addition, the correlation of times of Sr-isotope breaks at Enewetak with times of rapid Sr-isotope change in the DSDP 590B samples confirms the importance off sea-level changes in the evolution of global-marine Sr isotopes and shows that the Sr-isotope response to sea-level falls is rapid.

  14. Stable isotope customer list and summary of shipments - FY 1983

    Energy Technology Data Exchange (ETDEWEB)

    Davis, W.C. (comp.)

    1983-12-01

    This compilation is published as an aid to those concerned with the separation and sale of stable isotopes. The information is divided into four sections: (1) alphabetical list of domestic and foreign customers, showing the stable isotopes purchased during the fiscal year; (2) alphabetical list of isotopes, cross-referenced to customer numbers and divided into domestic and foreign categories; (3) alphabetical list of states and countries, cross-referenced to customer numbers and indicating geographical concentrations of isotope users; and (4) tabulation of the shipments, quantities, and dollars for domestic, foreign, and project categories for each isotope.

  15. The influence of leaf-atmosphere NH3(g ) exchange on the isotopic composition of nitrogen in plants and the atmosphere.

    Science.gov (United States)

    Johnson, Jennifer E; Berry, Joseph A

    2013-10-01

    The distribution of nitrogen isotopes in the biosphere has the potential to offer insights into the past, present and future of the nitrogen cycle, but it is challenging to unravel the processes controlling patterns of mixing and fractionation. We present a mathematical model describing a previously overlooked process: nitrogen isotope fractionation during leaf-atmosphere NH3(g ) exchange. The model predicts that when leaf-atmosphere exchange of NH3(g ) occurs in a closed system, the atmospheric reservoir of NH3(g ) equilibrates at a concentration equal to the ammonia compensation point and an isotopic composition 8.1‰ lighter than nitrogen in protein. In an open system, when atmospheric concentrations of NH3(g ) fall below or rise above the compensation point, protein can be isotopically enriched by net efflux of NH3(g ) or depleted by net uptake. Comparison of model output with existing measurements in the literature suggests that this process contributes to variation in the isotopic composition of nitrogen in plants as well as NH3(g ) in the atmosphere, and should be considered in future analyses of nitrogen isotope circulation. The matrix-based modelling approach that is introduced may be useful for quantifying isotope dynamics in other complex systems that can be described by first-order kinetics. © 2013 John Wiley & Sons Ltd.

  16. THE ATOMIC WEIGHTS COMMISSION AND ISOTOPIC ABUNDANCE RATIO DETERMINATIONS.

    Energy Technology Data Exchange (ETDEWEB)

    HOLDEN, N.E.

    2005-08-07

    Following Thomson's discovery of stable isotopes in non-radioactive chemical elements, the derivation of atomic weight values from mass spectrometric measurements of isotopic abundance ratios moved very slowly. Forty years later, only 3 1/2 % of the recommended values were based on mass spectrometric measurements and only 38% in the first half century. It might be noted that two chemical elements (tellurium and mercury) are still based on chemical measurements, where the atomic weight value calculated from the relative isotopic abundance measurement either agrees with the value from the chemical measurement or the atomic weight value calculated from the relative isotopic abundance measurement falls within the uncertainty of the chemical measurement of the atomic weight. Of the 19 chemical elements, whose atomic weight is based on non-corrected relative isotopic abundance measurements, five of these are two isotope systems (indium, iridium, lanthanum, lutetium and tantalum) and one is a three-isotope system (oxygen).

  17. Stable isotope analysis of the bioelements: an introduction.

    Science.gov (United States)

    Flenker, Ulrich

    2009-09-01

    The abundances of the stable isotopes of the bioelements are not constant. Subtle, but significant, variations may be induced by physical, physiological and biochemical processes. These variations may be detected and quantified. Often, isotope fingerprints are characteristic of certain processes and may reveal information concerning the sources and origins of compounds of interest. Moreover, natural variabilities of stable isotopes may be exploited in order to perform tracer experiments. The most accurate technology to perform stable isotope analysis is (gas) isotope ratio MS (IRMS). Compound-specific approaches employ hyphenation of GC and LC to IRMS. In these approaches, complete conversion to simple gases prior to MS is required. Analysis by stable isotope ratio spectroscopy currently approaches the accuracy of IRMS. However, for bioanalytical projects, it is still predominantly confined to material synthetically enriched with stable isotopes.

  18. Production Situation and Technology Prospect of Medical Isotopes

    Directory of Open Access Journals (Sweden)

    GAO Feng;LIN Li;LIU Yu-hao;MA Xing-jun

    2016-10-01

    Full Text Available The isotope production technology was overviewed, including traditional and newest technology. The current situation of medical isotope production was introduced. The problems faced by isotope supply and demand were analyzed. The future development trend of medical isotopes and technology prospect were put forward. As the most populous country, nuclear medicine develops rapidly, however, domestic isotope mainly relies on imports. The highly productive and relatively safe MIPR is expected to be an effective way to breakthrough the bottleneck of the development of nuclear medicine. Traditional isotope production technologies with reactor can be improved. It's urgent to research and promote new isotope production technologies with reactor. Those technologies which do not depend on reactor will have a bright market prospects.

  19. Further development of IDGS: Isotope dilution gamma-ray spectrometry

    Science.gov (United States)

    Li, T. K.; Parker, J. L.; Kuno, Y.; Sato, S.; Kamata, M.; Akiyama, T.

    The isotope dilution gamma-ray spectrometry (IDGS) technique for determining the plutonium concentration and isotopic composition of highly radioactive spent-fuel dissolver solutions has been further developed. Both the sample preparation and the analysis have been improved. The plutonium isotopic analysis is based on high-resolution, low-energy gamma-ray spectrometry. The plutonium concentration in the dissolver solutions then is calculated from the measured isotopic differences among the spike, the dissolver solution, and the spiked dissolver solution. Plutonium concentrations and isotopic compositions of dissolver solutions analyzed from this study agree well with those obtained by traditional isotope dilution mass spectrometry (IDMS) and are consistent with the first IDGS experimental result. With the current detector efficiency, sample size, and a 100-min count time, the estimated precision is approximately 0.5 percent for Pu-239 and Pu-240 isotopic analyses and approximately 1 percent for the plutonium concentration analysis.

  20. Large deuterium isotope effects and their use: a historical review.

    Science.gov (United States)

    Krumbiegel, Peter

    2011-03-01

    Isotope effects are differences in the properties of the isotopes of an element resulting in different reaction rates of a corresponding compound, in equilibrium constants and in the spectra. Shortly after the discovery of stable isotopes of hydrogen, oxygen, and carbon, Jacob Bigeleisen formulated a theory of isotope effects and calculated possible maximum values. Large isotope effects of (2)H (deuterium) against (1)H (protium) were seen to possibly influence interpretations of reaction mechanisms if corresponding labelling is used. Much work was invested to ensure the safety of deuterium use in men in spite of the large isotope effect. On the other hand, large deuterium isotope effects gave rise to several practical applications. Examples are the enhancement of the stability of some technical products against oxidative and against hydrolytic degradation (oils, pharmaceuticals) as well as alterations of the detoxification metabolism of pharmaceuticals in vivo.

  1. Modelling non-steady-state isotope enrichment of leaf water in a gas-exchange cuvette environment.

    Science.gov (United States)

    Song, Xin; Simonin, Kevin A; Loucos, Karen E; Barbour, Margaret M

    2015-12-01

    The combined use of a gas-exchange system and laser-based isotope measurement is a tool of growing interest in plant ecophysiological studies, owing to its relevance for assessing isotopic variability in leaf water and/or transpiration under non-steady-state (NSS) conditions. However, the current Farquhar & Cernusak (F&C) NSS leaf water model, originally developed for open-field scenarios, is unsuited for use in a gas-exchange cuvette environment where isotope composition of water vapour (δv ) is intrinsically linked to that of transpiration (δE ). Here, we modified the F&C model to make it directly compatible with the δv -δE dynamic characteristic of a typical cuvette setting. The resultant new model suggests a role of 'net-flux' (rather than 'gross-flux' as suggested by the original F&C model)-based leaf water turnover rate in controlling the time constant (τ) for the approach to steady sate. The validity of the new model was subsequently confirmed in a cuvette experiment involving cotton leaves, for which we demonstrated close agreement between τ values predicted from the model and those measured from NSS variations in isotope enrichment of transpiration. Hence, we recommend that our new model be incorporated into future isotope studies involving a cuvette condition where the transpiration flux directly influences δv . There is an increasing popularity among plant ecophysiologists to use a gas-exchange system coupled to laser-based isotope measurement for investigating non-steady state (NSS) isotopic variability in leaf water (and/or transpiration); however, the current Farquhar & Cernusak (F&C) NSS leaf water model is unsuited for use in a gas-exchange cuvette environment due to its implicit assumption of isotope composition of water vapor (δv ) being constant and independent of that of transpiration (δE ). In the present study, we modified the F&C model to make it compatible with the dynamic relationship between δv and δE as is typically associated

  2. Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO{sub 2} nuclear fuel

    Energy Technology Data Exchange (ETDEWEB)

    Piro, M.H.A., E-mail: markuspiro@gmail.com [Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN (United States); Banfield, J. [Nuclear Engineering Department, University of Tennessee, Knoxville, TN (United States); Clarno, K.T., E-mail: clarnokt@ornl.gov [Reactor and Nuclear Systems Division, Oak Ridge National Laboratory, Oak Ridge, TN (United States); Simunovic, S. [Computer Science and Mathematics Division, Oak Ridge National Laboratory, Oak Ridge, TN (United States); Besmann, T.M. [Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN (United States); Lewis, B.J.; Thompson, W.T. [Department of Chemistry and Chemical Engineering, Royal Military College of Canada, Kingston, ON (Canada)

    2013-10-15

    Predictive capabilities for simulating irradiated nuclear fuel behavior are enhanced in the current work by coupling thermochemistry, isotopic evolution and heat transfer. Thermodynamic models that are incorporated into this framework not only predict the departure from stoichiometry of UO{sub 2}, but also consider dissolved fission and activation products in the fluorite oxide phase, noble metal inclusions, secondary oxides including uranates, zirconates, molybdates and the gas phase. Thermochemical computations utilize the spatial and temporal evolution of the fission and activation product inventory in the pellet, which is typically neglected in nuclear fuel performance simulations. Isotopic computations encompass the depletion, decay and transmutation of more than 2000 isotopes that are calculated at every point in space and time. These computations take into consideration neutron flux depression and the increased production of fissile plutonium near the fuel pellet periphery (i.e., the so-called “rim effect”). Thermochemical and isotopic predictions are in very good agreement with reported experimental measurements of highly irradiated UO{sub 2} fuel with an average burnup of 102 GW d t(U){sup −1}. Simulation results demonstrate that predictions are considerably enhanced when coupling thermochemical and isotopic computations in comparison to empirical correlations. Notice: This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes.

  3. Laser ablation molecular isotopic spectroscopy (LAMIS) towards the determination of multivariate LODs via PLS calibration model of 10B and 11B Boric acid mixtures

    Science.gov (United States)

    Harris, C. D.; Profeta, Luisa T. M.; Akpovo, Codjo A.; Johnson, Lewis; Stowe, Ashley C.

    2017-05-01

    A calibration model was created to illustrate the detection capabilities of laser ablation molecular isotopic spectroscopy (LAMIS) discrimination in isotopic analysis. The sample set contained boric acid pellets that varied in isotopic concentrations of 10B and 11B. Each sample set was interrogated with a Q-switched Nd:YAG ablation laser operating at 532 nm. A minimum of four band heads of the β system B2∑ -> Χ2∑transitions were identified and verified with previous literature on BO molecular emission lines. Isotopic shifts were observed in the spectra for each transition and used as the predictors in the calibration model. The spectra along with their respective 10/11B isotopic ratios were analyzed using Partial Least Squares Regression (PLSR). An IUPAC novel approach for determining a multivariate Limit of Detection (LOD) interval was used to predict the detection of the desired isotopic ratios. The predicted multivariate LOD is dependent on the variation of the instrumental signal and other composites in the calibration model space.

  4. Isotopic ratio correlation for the isotopic composition analysis of plutonium in Am-Pu mixed samples having high americium content.

    Science.gov (United States)

    Patra, Sabyasachi; Agarwal, Chhavi; Chaudhury, Sanhita; Newton Nathaniel, T; Gathibandhe, M; Goswami, A

    2013-08-01

    Interference of high amount of americium in the plutonium isotopic composition analysis has been studied by simulating gamma-ray spectra for Am-Pu samples over a wide composition range (5-97% (241)Am) for both power and research reactor grade plutonium. An alternate way for isotopic composition analysis has been proposed by correlating the isotopic ratios available in our old database with the experimentally obtained (241)Pu/(239)Pu isotopic ratio. The proposed method has been validated using simulated spectra of known isotopic compositions. Copyright © 2013 Elsevier Ltd. All rights reserved.

  5. Pb and Sr isotope measurements by inductively coupled plasma mass spectrometer: efficient time management for precision improvement

    Science.gov (United States)

    Monna, F.; Loizeau, J.-L.; Thomas, B. A.; Guéguen, C.; Favarger, P.-Y.

    1998-08-01

    One of the factors limiting the precision of inductively coupled plasma mass spectrometry is the counting statistics, which depend upon acquisition time and ion fluxes. In the present study, the precision of the isotopic measurements of Pb and Sr is examined. The time of measurement is optimally shared for each isotope, using a mathematical simulation, to provide the lowest theoretical analytical error. Different algorithms of mass bias correction are also taken into account and evaluated in term of improvement of overall precision. Several experiments allow a comparison of real conditions with theory. The present method significantly improves the precision, regardless of the instrument used. However, this benefit is more important for equipment which originally yields a precision close to that predicted by counting statistics. Additionally, the procedure is flexible enough to be easily adapted to other problems, such as isotopic dilution.

  6. Carbonate "clumped" isotope signatures in aragonitic scleractinian and calcitic gorgonian deep-sea corals

    Science.gov (United States)

    Kimball, Justine; Eagle, Robert; Dunbar, Robert

    2016-12-01

    between the corals of different mineralogy is in the same direction as published theoretical predictions for the offset between calcite and aragonite although the magnitude of the offset is different. One possibility is that the deep-sea coral results reflect high-Mg and aragonite crystals attaining nominal mineral equilibrium clumped isotope signatures due to conditions of extremely slow growth. In that case, a possible explanation for the attainment of disequilibrium bulk isotope signatures and equilibrium clumped isotope signatures by deep-sea corals is that extraordinarily slow growth rates can promote the occurrence of isotopic reordering in the interfacial region of growing crystals. We also cannot rule out a component of a biological "vital effect" influencing clumped isotope signatures in one or both orders of coral. Based on published experimental data and theoretical calculations, these biological vital effects could arise from kinetic isotope effects due to the source of carbon used for calcification, temperature- and pH-dependent rates of CO2 hydration and/or hydroxylation, calcifying fluid pH, the activity of carbonic anhydrase, the residence time of dissolved inorganic carbon in the calcifying fluid, and calcification rate. A third possible explanation is the occurrence of variable acid digestion fractionation factors. Although a recent study has suggested that dolomite, calcite, and aragonite may have similar clumped isotope acid digestion fractionation factors, the influence of acid digestion kinetics on Δ47 is a subject that warrants further investigation.

  7. Calculation of individual isotope equilibrium constants for geochemical reactions

    Science.gov (United States)

    Thorstenson, D.C.; Parkhurst, D.L.

    2004-01-01

    Theory is derived from the work of Urey (Urey H. C. [1947] The thermodynamic properties of isotopic substances. J. Chem. Soc. 562-581) to calculate equilibrium constants commonly used in geochemical equilibrium and reaction-transport models for reactions of individual isotopic species. Urey showed that equilibrium constants of isotope exchange reactions for molecules that contain two or more atoms of the same element in equivalent positions are related to isotope fractionation factors by ?? = (Kex)1/n, where n is the number of atoms exchanged. This relation is extended to include species containing multiple isotopes, for example 13C16O18O and 1H2H18O. The equilibrium constants of the isotope exchange reactions can be expressed as ratios of individual isotope equilibrium constants for geochemical reactions. Knowledge of the equilibrium constant for the dominant isotopic species can then be used to calculate the individual isotope equilibrium constants. Individual isotope equilibrium constants are calculated for the reaction CO2g = CO2aq for all species that can be formed from 12C, 13C, 16O, and 18O; for the reaction between 12C18 O2aq and 1H218Ol; and among the various 1H, 2H, 16O, and 18O species of H2O. This is a subset of a larger number of equilibrium constants calculated elsewhere (Thorstenson D. C. and Parkhurst D. L. [2002] Calculation of individual isotope equilibrium constants for implementation in geochemical models. Water-Resources Investigation Report 02-4172. U.S. Geological Survey). Activity coefficients, activity-concentration conventions for the isotopic variants of H2O in the solvent 1H216Ol, and salt effects on isotope fractionation have been included in the derivations. The effects of nonideality are small because of the chemical similarity of different isotopic species of the same molecule or ion. The temperature dependence of the individual isotope equilibrium constants can be calculated from the temperature dependence of the fractionation

  8. Charge state distribution studies of pure and oxygen mixed krypton ECR plasma - signature of isotope anomaly and gas mixing effect.

    Science.gov (United States)

    Kumar, Pravin; Mal, Kedar; Rodrigues, G

    2016-11-01

    We report the charge state distributions of the pure, 25% and 50% oxygen mixed krypton plasma to shed more light on the understanding of the gas mixing and the isotope anomaly [A. G. Drentje, Rev. Sci. Instrum. 63 (1992) 2875 and Y Kawai, D Meyer, A Nadzeyka, U Wolters and K Wiesemann, Plasma Sources Sci. Technol. 10 (2001) 451] in the electron cyclotron resonance (ECR) plasmas. The krypton plasma was produced using a 10 GHz all-permanent-magnet ECR ion source. The intensities of the highly abundant four isotopes, viz. 82 Kr (~11.58%), 83 Kr (~11.49%), 84 Kr (~57%) and 86 Kr (17.3%) up to ~ +14 charge state have been measured by extracting the ions from the plasma and analysing them in the mass and the energy using a large acceptance analyzer-cum-switching dipole magnet. The influence of the oxygen gas mixing on the isotopic krypton ion intensities is clearly evidenced beyond +9 charge state. With and without oxygen mixing, the charge state distribution of the krypton ECR plasma shows the isotope anomaly with unusual trends. The anomaly in the intensities of the isotopes having quite closer natural abundance, viz. 82 Kr, 86 Kr and 83 Kr, 86 Kr is prominent, whereas the intensity ratio of 86 Kr to 84 Kr shows a weak signature of it. The isotope anomaly tends to disappear with increasing oxygen mixing in the plasma. The observed trends in the intensities of the krypton isotopes do not follow the prediction of linear Landau wave damping in the plasma. Copyright © 2016 John Wiley & Sons, Ltd. Copyright © 2016 John Wiley & Sons, Ltd.

  9. Estimating ground-water inflow to lakes in central Florida using the isotope mass-balance approach

    Science.gov (United States)

    Sacks, Laura A.

    2002-01-01

    quantification. The lakes fit into three categories based on their range of ground-water inflow: low (less than 25 percent of total inflows), medium (25-50 percent of inflows), and high (greater than 50 percent of inflows). The majority of lakes in the coastal lowlands had low ground-water inflow, whereas the majority of lakes in the central highlands had medium to high ground-water inflow. Multiple linear regression models were used to predict ground-water inflow to lakes. These models help identify basin characteristics that are important in controlling ground-water inflow to Florida lakes. Significant explanatory variables include: ratio of basin area to lake surface area, depth to the Upper Floridan aquifer, maximum lake depth, and fraction of wetlands in the basin. Models were improved when lake water-quality data (nitrate, sodium, and iron concentrations) were included, illustrating the link between ground-water geochemistry and lake chemistry. Regression models that considered lakes within specific geographic areas were generally poorer than models for the entire study area. Regression results illustrate how more simplified models based on basin and lake characteristics can be used to estimate ground-water inflow. Although the uncertainty in the amount of ground-water inflow to individual lakes is high, the isotope mass-balance approach was useful in comparing the range of ground-water inflow for numerous Florida lakes. Results were also helpful in understanding differences in the geographic distribution of ground-water inflow between the coastal lowlands and central highlands. In order to use the isotope mass-balance approach to estimate inflow for multiple lakes, it is essential that all the lakes are sampled during the same time period and that detailed isotopic, hydrologic, and climatic data are collected over this same period of time. Isotopic data for Florida lakes can change over time, both seasonally and interannually, primarily because of differ

  10. A Simple Approach to Simulate the Complexity of Planktonic Foraminifer Oxygen Isotope Time Series

    Science.gov (United States)

    Waelbroeck, C.; Roche, D. M.; Caley, T.; Kucera, M.; Jonkers, L.; Vazquez Riveiros, N.

    2016-12-01

    Oxygen isotopic curves measured on different planktonic foraminifer species at the same site often exhibit a variable offset. This means that the habitats of the involved species may change through time, which affects the interpretation of the paleoclimatic records. Here we propose to investigate the effect of habitat change by comparing measured and mechanistically computed calcite oxygen isotopic ratios (δ18O) for N. pachyderma left and right coiling, G. bulloides, and G. ruber. To this end we developed the module "Foraminifers as Modeled Entities" (FAME) using species and temperature-dependent growth rates to predict the vertical and seasonal habitat of each species. FAME is forced by hydrography and water δ18O taken from observations or models, and predicts sedimentary average δ18O for each planktonic foraminifer species. FAME yields excellent agreement with MARGO Late Holocene and core top planktonic δ18O data when forced with WOA13 temperature and GISS water δ18O data, in contrast to the calculation of calcite equilibrium δ18O without correction for foraminifer habitat. We explore the applicability of the module to the past by forcing it with vertical temperature and water δ18O profiles computed by the isotope-enabled Earth System Model of Intermediate Complexity iLOVECLIM and compare δ18O simulations with fossil data for the LGM time slice and for the last deglaciation.

  11. Production of noble gas isotopes by proton-induced reactions on lead and bismuth

    Science.gov (United States)

    Leya, I.; Wieler, R.; David, J.-C.; Leray, S.; Donadille, L.; Cugnon, J.; Michel, R.

    2006-06-01

    We measured integral thin target cross-sections for the proton-induced production of He-, Ne-, Ar-, Kr-, and Xe-isotopes from lead and bismuth from the respective reaction threshold up to 2.6 GeV. The production of noble gas isotopes from lead and bismuth is of special importance for design studies of accelerator driven nuclear reactors and/or energy amplifiers. For all experiments with proton energies above 200 MeV a new mini-stack approach was used instead of the stacked-foil technique in order to minimise influences of secondary particles. The phenomenology of the determined excitation functions enables us to distinguish between the different reaction modes fragmentation, hot and cold symmetric fission, asymmetric fission, and deep spallation. For lead more than 420 cross-sections for 23 nuclear reactions have been measured. While the lead data have already been published, here we present first results for the production of noble gas isotopes from bismuth. The experimental data are compared to results from the theoretical nuclear model code INCL4/ABLA. This comparison clearly indicates that experimental data are still needed because the predictive power of nuclear model codes, though permanently improving, does still not allow to reliably predict the cross-sections needed for most applications and irradiation experiments remain indispensable.

  12. Inferring global and regional methane sources and sinks using isotopic observations and atmospheric chemical transport models

    Science.gov (United States)

    Rigby, M. L.; Wenger, A.; O'Doherty, S.; Lunt, M. F.; Ganesan, A.; Manning, A.; Prinn, R. G.

    2015-12-01

    Measurements of the major isotopologues of atmospheric methane have the potential to improve our understanding of the methane budget at the global and regional scale. Using global and regional chemical transport models, we can predict the atmospheric variations in 13C-CH4 and D-CH4, for given assumptions about source isotope ratios and fractionation due to methane sinks. This information can then be used to test the impact that various measurement techniques, technologies and sampling strategies have on our knowledge of the methane budget. We show that, at the global scale, an extensive and accurate network of isotopic measurements can lead to a reduction in the uncertainties in the major global sources. Furthermore, measurements of the D/H ratio in methane may provide some level of uncertainty reduction in the magnitude of the OH sink. Uncertainties can be reduced with improved precision and accuracy of the atmospheric observations. However, to make the most of an atmospheric methane isotope network, we show that the characterisation of source isotope ratios must also be improved. Finally, we put the theory into practice by deriving sector-specific methane sources at the national scale using 13C-CH4 samples collected as part of the Greenhouse gAs Uk and Global Emissions (GAUGE) project. GAUGE measurements are made from a tall tower site to the east of the UK, a background station on the west coast of Ireland and during intensive aircraft sampling campaigns. We will discuss the challenges and benefits associated with adding isotopic information to a national greenhouse gas sampling network and outline a strategy for improvements in the future.

  13. Laser Spectroscopic Measurements of Isotope Shift and Hyperfine Structure in BISMUTH-207 and BISMUTH-208.

    Science.gov (United States)

    Fang, Zuyun

    1988-12-01

    Measurements of the hyperfine spectra of 38-yr ^{207}Bi and 3.7 times 10^5-yr ^{208}Bi in the 6p^3 ^4S_{3/2} - 6p^27s ^4P_{1/2} 306.7-nm resonance line were made using laser spectroscopic methods. The atomic excitation was produced with use of the frequency doubled output of a tunable ring dye laser. Laser absorption spectroscopy was used for the ^ {208}Bi measurement, while fluorescence spectroscopy, with photon counting detection, was used for ^{208}Bi. The experiments of ^{207}Bi were performed in both zero and high (0.7515 T) magnetic fields. The latter also provided a reliable measurement of the nuclear spin of ^{207}Bi. The results obtained from the ^ {208}Bi spectra are: A(^4P _{1/2}) = 4911(17)MHz and B( ^4S_{3/2}) = -314(92)MHz. These give the values: mu = 4.523(16) mu_{N} and Q = - 0.39(12)b. The measured isotope shift is: IS( ^{208}Bi-^{209 }Bi) = 1870(63)MHz. The results for ^{207} Bi are: I = 9/2, A(^4P_{1/2 }) = 4900.0(8.1)MHz, A(^4S_ {1/2}) = -444.6(1.5)MHz and B(^4S_{1/2}) = -443(17)MHz. These give the values: mu = 4.062(8)mu_ {N} and Q = -0.55(2)b. The measured isotope shift is: IS(^{207 }Bi-^{209}Bi) = 2997(10)MHz. The isotope shift odd-even staggering parameter for ^{208}Bi, gamma = 0.752(43), was derived and used for an isotonic comparison. The measured nuclear magnetic moments are in agreement with theoretical predictions. An improved calculation of the isotope shift constant using a diffuse nuclear charge model is given and a weak, but significant, model dependence of the isotope shifts was found.

  14. Isotopic and molecular distributions of biochemicals from fresh and buried Rhizophora mangle leaves†

    Directory of Open Access Journals (Sweden)

    Jacobson Myrna E

    2003-12-01

    Full Text Available Rhizophora mangle L. (red mangrove is the dominant species of mangrove in the Americas. At Twin Cays, Belize (BZ red mangroves are present in a variety of stand structures (tall >5 m in height, transition ~2–4 m and dwarf ~1–1.5 m. These height differences are coupled with very different stable carbon and nitrogen isotopic values1 (mean tall δ13C = -28.3‰, δ15N = 0‰; mean tall δ13C = -25.3‰, δ15N = -10‰. To determine the utility of using these distinct isotopic compositions as 'biomarkers' for paleoenvironmental reconstruction of mangrove ecosystems and nutrient availability, we investigated the distribution and isotopic (δ13C and δ15N composition of different biochemical fractions (water soluble compounds, free lipids, acid hydrolysable compounds, individual amino acids, and the residual un-extractable compounds in fresh and preserved red mangrove leaves from dwarf and tall trees. The distribution of biochemicals are similar in dwarf and tall red mangrove leaves, suggesting that, regardless of stand structure, red mangroves use nutrients for biosynthesis and metabolism in a similar manner. However, the δ13C and δ15N of the bulk leaf, the biochemical fractions, and seven amino acids can be used to distinguish dwarf and tall trees at Twin Cays, BZ. The data support the theory that the fractionation of carbon and nitrogen occurs prior to or during uptake in dwarf and tall red mangrove trees. Stable carbon and nitrogen isotopes could, therefore, be powerful tools for predicting levels of nutrient limitation at Twin Cays. The δ13C and δ15N of biochemical fractions within preserved leaves, reflect sedimentary cycling and nitrogen immobilization. The δ15N of the immobilized fraction reveals the overlying stand structure at the time of leaf deposition. The isotopic composition of preserved mangrove leaves could yield significant information about changes in ecosystem dynamics, nutrient limitation and past stand structure in

  15. Clumped-isotope geochemistry of carbonates: A new tool for the reconstruction of temperature and oxygen isotope composition of seawater

    Energy Technology Data Exchange (ETDEWEB)

    Bernasconi, Stefano M., E-mail: Stefano.bernasconi@erdw.ethz.ch [Geological Institute, ETH Zuerich, Sonneggstrasse 5, 8092 Zuerich (Switzerland); Schmid, Thomas W.; Grauel, Anna-Lena [Geological Institute, ETH Zuerich, Sonneggstrasse 5, 8092 Zuerich (Switzerland); Mutterlose, Joerg [Institut fuer Geologie, Mineralogie und Geophysik, Ruhr Universitaet Bochum, Universitaetsstr. 150, 44801 Bochum (Germany)

    2011-06-15

    Highlights: > Clumped-isotope thermometry of carbonates is discussed. > Clumped isotopes of Belemnites show higher sea surface temperatures than commonly assumed for the lower Cretaceous. > The potential of clumped-isotope measurement on foraminifera is discussed. - Abstract: Clumped-isotope geochemistry deals with State of ordering of rare isotopes in molecules, in particular with their tendency to form bonds with other rare isotopes rather than with the most abundant ones. Among its possible applications, carbonate clumped-isotope thermometry is the one that has gained most attention because of the wide potential of applications in many disciplines of the earth sciences. In particular, it allows reconstructing the temperature of formation of carbonate minerals without knowledge of the isotopic composition of the water from which they were formed. In addition, the O isotope composition of the waters from which they were formed can be calculated using the {delta}{sup 18}O of the same carbonate sample. This feature offers new approaches in paleoclimatology for reconstructing past global geochemical cycles. In this contribution two applications of this method are presented. First the potential of a new analytical method of measurement of clumped isotopes on small samples of foraminifera, for high-resolution SST and seawater {delta}{sup 18}O reconstructions from marine sediments is shown. Furthermore the potential of clumped isotope analysis of belemnites, for reconstructing seawater {delta}{sup 18}O and temperatures in the Cretaceous is shown.

  16. Isotope systematics of Icelandic thermal fluids

    Science.gov (United States)

    Stefánsson, Andri; Hilton, David R.; Sveinbjörnsdóttir, Árný E.; Torssander, Peter; Heinemeier, Jan; Barnes, Jaime D.; Ono, Shuhei; Halldórsson, Sæmundur Ari; Fiebig, Jens; Arnórsson, Stefán

    2017-05-01

    Thermal fluids in Iceland range in temperature from 440 °C and are dominated by water (> 97 mol%) with a chloride concentration from 20,000 ppm. The isotope systematics of the fluids reveal many important features of the source(s) and transport properties of volatiles at this divergent plate boundary. Studies spanning over four decades have revealed a large range of values for δD (- 131 to + 3.3‰), tritium (- 0.4 to + 13.8 TU), δ18O (- 20.8 to + 2.3‰), 3He/4He (3.1 to 30.4 RA), δ11B (- 6.7 to + 25.0‰), δ13C∑ CO2 (- 27.4 to + 4.6‰), 14C∑ CO2 (+ 0.6 to + 118 pMC), δ13CCH4 (- 52.3 to - 17.8‰), δ15N (- 10.5 to + 3.0‰), δ34S∑ S- II (- 10.9 to + 3.4‰), δ34SSO4 (- 2.0 to + 21.2‰) and δ37Cl (- 1.0 to + 2.1‰) in both liquid and vapor phases. Based on this isotopic dataset, the thermal waters originate from meteoric inputs and/or seawater. For other volatiles, degassing of mantle-derived melts contributes to He, CO2 and possibly also to Cl in the fluids. Water-basalt interaction also contributes to CO2 and is the major source of H2S, SO4, Cl and B in the fluids. Redox reactions additionally influence the composition of the fluids, for example, oxidation of H2S to SO4 and reduction of CO2 to CH4. Air-water interaction mainly controls N2, Ar and Ne concentrations. The large range of many non-reactive volatile isotope ratios, such as δ37Cl and 3He/4He, indicate heterogeneity of the mantle and mantle-derived melts beneath Iceland. In contrast, the large range of many reactive isotopes, such as δ13C∑ CO2 and δ34S∑ S- II, are heavily affected by processes occurring within the geothermal systems, including fluid-rock interaction, depressurization boiling, and isotopic fractionation between secondary minerals and the aqueous and vapor species. Variations due to these geothermal processes may exceed differences observed among various crust and mantle sources, highlighting the importance and effects of chemical reactions on the isotope

  17. Aerosol carbon isotope composition over Baltic Sea

    Science.gov (United States)

    Garbaras, Andrius; Pabedinskas, Algirdas; Masalaite, Agne; Petelski, Tomasz; Gorokhova, Elena; Sapolaite, Justina; Ezerinskis, Zilvinas; Remeikis, Vidmantas

    2017-04-01

    Particulate carbonaceous matter is significant contributor to ambient particulate matter originating from intervening sources which contribution is difficult to quantify due to source diversity, chemical complexity and processes during atmospheric transport. Carbon isotope analysis can be extremely useful in source apportionment of organic matter due to the unique isotopic signatures associated with anthropocentric (fossil fuel), continental (terrestrial plants) and marine sources, and is particularly effective when these sources are mixed (Ceburnis et al., 2011;Ceburnis et al., 2016). We will present the isotope ratio measurement results of aerosol collected during the cruise in the Baltic Sea. Sampling campaign of PM10 and size segregated aerosol particles was performed on the R/V "Oceania" in October 2015. Air mass back trajectories were prevailing both from the continental and marine areas during the sampling period. The total carbon concentration varied from 1 µg/m3 to 8 µg/m3. Two end members (δ13C = -25‰ and δ13C = -28 ‰ ) were established from the total stable carbon isotope analysis in PM10 fraction. δ13C analysis in size segregated aerosol particles revealed δ13C values being highest in the 1 - 2.5 µm range (δ13C = -24.9 ‰ ) during continental transport, while lowest TC δ13C values (δ13C ≈ -27 ‰ ) were detected in the size range D50 matter origin in submicron marine aerosol by 13 C and 14 C isotope analysis, Atmospheric Chemistry and Physics, 11, 8593-8606, 2011. Ceburnis, D., Masalaite, A., Ovadnevaite, J., Garbaras, A., Remeikis, V., Maenhaut, W., Claeys, M., Sciare, J., Baisnée, D., and O'Dowd, C. D.: Stable isotopes measurements reveal dual carbon pools contributing to organic matter enrichment in marine aerosol, Scientific Reports, 6, 2016. Masalaite, A., Remeikis, V., Garbaras, A., Dudoitis, V., Ulevicius, V., and Ceburnis, D.: Elucidating carbonaceous aerosol sources by the stable carbon δ13C TC ratio in size

  18. Oxygen isotope fractionation in phosphates: the role of dissolved complex anions in isotope exchange.

    Science.gov (United States)

    Zheng, Yong-Fei

    2016-01-01

    Oxygen isotope fractionation factors for phosphates were calculated by means of the increment method. The results suggest that Ag3PO4 and BiPO4 are enriched in (18)O relative to AgPO4, and the three phosphates are consistently depleted in (18)O relative to Ba3[PO4]2; fluorapatite and chlorapatite exhibit a similar behaviour of oxygen isotope fractionation with consistent enrichment of (18)O relative to hydroxyapatite. The valence, radii and coordination of metal cations play a quantitative role in dictating the (18)O/(16)O partitioning in these phosphates of different compositions. The calculated fractionation factors for the Ag3PO4-H2O system are in agreement with experimental determinations derived from enzyme-catalysed isotope exchange between dissolved inorganic phosphate and water at the longest reaction durations at low temperatures. This demonstrates that the precipitated Ag3PO4 has completely captured the oxygen isotope fractionation in the dissolved inorganic phosphate. The calculated fractionation factors for the F/Cl-apatite-water systems are in agreement with the enzyme-catalysed experimental fractionations for the dissolved phosphate-water system at the longest reaction durations but larger than fractionations derived from bacteria-facilitated exchange and inorganic precipitation experiments as well as natural observations. For the experimental calibrations of oxygen isotope fractionation involving the precipitation of dissolved phosphate species from aqueous solutions, the fractionation between precipitate and water is primarily dictated by the isotope equilibration between the dissolved complex anions and water prior to the precipitation. Therefore, the present results provide a quantitative means to interpret the temperature dependence of oxygen isotope fractionation in inorganic and biogenic phosphates.

  19. Isotopic analysis of oxidative pollutant degradation pathways exhibiting large H isotope fractionation.

    Science.gov (United States)

    Wijker, Reto S; Adamczyk, Pawel; Bolotin, Jakov; Paneth, Piotr; Hofstetter, Thomas B

    2013-01-01

    Oxidation of aromatic rings and its alkyl substituents are often competing initial steps of organic pollutant transformation. The use of compound-specific isotope analysis (CSIA) to distinguish between these two pathways quantitatively, however, can be hampered by large H isotope fractionation that precludes calculation of apparent (2)H-kinetic isotope effects (KIE) as well as the process identification in multi-element isotope fractionation analysis. Here, we investigated the C and H isotope fractionation associated with the transformation of toluene, nitrobenzene, and four substituted nitrotoluenes by permanganate, MnO4(-), to propose a refined evaluation procedure for the quantitative distinction of CH3-group oxidation and dioxygenation. On the basis of batch experiments, an isotopomer-specific kinetic model, and density functional theory (DFT) calculations, we successfully derived the large apparent (2)H-KIE of 4.033 ± 0.20 for the CH3-group oxidation of toluene from H isotope fractionation exceeding >1300‰ as well as the corresponding (13)C-KIE (1.0324 ± 0.0011). Experiment and theory also agreed well for the dioxygenation of nitrobenzene, which was associated with (2)H- and (13)C-KIEs of 0.9410 ± 0.0030 (0.9228 obtained by DFT) and 1.0289 ± 0.0003 (1.025). Consistent branching ratios for the competing CH3-group oxidation and dioxygenation of nitrotoluenes by MnO4(-) were obtained from the combined modeling of concentration as well as C and H isotope signature trends. Our approach offers improved estimates for the identification of contaminant microbial and abiotic oxidation pathways by CSIA.

  20. Temperature dependence of carbon kinetic isotope effect for the oxidation reaction of ethane by OH radicals under atmospherically relevant conditions

    Science.gov (United States)

    Piansawan, Tammarat; Saccon, Marina; Laumer, Werner; Gensch, Iulia; Kiendler-Scharr, Astrid

    2015-04-01

    Modeling of the global distribution of atmospheric ethane sources and sinks by using the 13C isotopic composition requires accurate knowledge of the carbon kinetic isotope effect (KIE) of its atmospheric removal reactions. The quantum mechanical prediction implies the necessity to elucidate the temperature dependence of KIE within atmospherically relevant temperature range by experiment. In this study, the KIE and its temperature dependence for ethane oxidation by OH radicals was investigated at ambient pressure in a temperature range of 243 K to 303 K. The chemical reactions were carried out in a 15 L PFE reaction chamber, suspended in a thermally controlled oven. The isotope ratios of the gas phase components during the course of the reactions were measured by Thermal Desorption -- Gas Chromatography -- Isotope Ratio Mass Spectrometry (TD-GC-IRMS). For each temperature, the KIE was derived from the temporal evolution of the concentration and stable carbon isotope ratio (δ13C) of ethane using a method adapted from the relative reaction rate concept. The room temperature KIE of the ethane reaction with OH radicals was found to be 6.85 ± 0.32 ‰. This value is in agreement with the previously reported value of 8.57 ± 1.95 ‰ [Anderson et al. 2004] but has a substantially lower uncertainty. The experimental results will be discussed with the KIE temperature dependence predicted by quantum mechanical calculations. Reference: Rebecca S. Anderson, Lin Huang, Richard Iannone, Alexandra E. Thompson, and Jochen Rudolph (2004), Carbon Kinetic Isotope Effects in the Gas Phase Reactions of Light Alkanes and Ethene with the OH Radical at 296 ± 4 K, J. Phys. Chem. A, 108, 11537--11544

  1. Spatial, seasonal, and source variability in the stable oxygen and hydrogen isotopic composition of tap waters throughout the USA

    Science.gov (United States)

    Landwehr, Jurate M.; Coplen, Tyler B.; Stewart, David W.

    2013-01-01

    To assess spatial, seasonal, and source variability in stable isotopic composition of human drinking waters throughout the entire USA, we have constructed a database of δ18O and δ2H of US tap waters. An additional purpose was to create a publicly available dataset useful for evaluating the forensic applicability of these isotopes for human tissue source geolocation. Samples were obtained at 349 sites, from diverse population centres, grouped by surface hydrologic units for regional comparisons. Samples were taken concurrently during two contrasting seasons, summer and winter. Source supply (surface, groundwater, mixed, and cistern) and system (public and private) types were noted. The isotopic composition of tap waters exhibits large spatial and regional variation within each season as well as significant at-site differences between seasons at many locations, consistent with patterns found in environmental (river and precipitation) waters deriving from hydrologic processes influenced by geographic factors. However, anthropogenic factors, such as the population of a tap’s surrounding community and local availability from diverse sources, also influence the isotopic composition of tap waters. Even within a locale as small as a single metropolitan area, tap waters with greatly differing isotopic compositions can be found, so that tap water within a region may not exhibit the spatial or temporal coherence predicted for environmental water. Such heterogeneities can be confounding factors when attempting forensic inference of source water location, and they underscore the necessity of measurements, not just predictions, with which to characterize the isotopic composition of regional tap waters. Published 2013. This article is a U.S. Government work and is in the public domain in the USA.

  2. Ion implantation system and process for ultrasensitive determination of target isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Farmer, III, Orville T.; Liezers, Martin

    2016-09-13

    A system and process are disclosed for ultrasensitive determination of target isotopes of analytical interest in a sample. Target isotopes may be implanted in an implant area on a high-purity substrate to pre-concentrate the target isotopes free of contaminants. A known quantity of a tracer isotope may also be implanted. Target isotopes and tracer isotopes may be determined in a mass spectrometer. The present invention provides ultrasensitive determination of target isotopes in the sample.

  3. Nuclear quantum effects and kinetic isotope effects in enzyme reactions.

    Science.gov (United States)

    Vardi-Kilshtain, Alexandra; Nitoker, Neta; Major, Dan Thomas

    2015-09-15

    Enzymes are extraordinarily effective catalysts evolved to perform well-defined and highly specific chemical transformations. Studying the nature of rate enhancements and the mechanistic strategies in enzymes is very important, both from a basic scientific point of view, as well as in order to improve rational design of biomimetics. Kinetic isotope effect (KIE) is a very important tool in the study of chemical reactions and has been used extensively in the field of enzymology. Theoretically, the prediction of KIEs in condensed phase environments such as enzymes is challenging due to the need to include nuclear quantum effects (NQEs). Herein we describe recent progress in our group in the development of multi-scale simulation methods for the calculation of NQEs and accurate computation of KIEs. We also describe their application to several enzyme systems. In particular we describe the use of combined quantum mechanics/molecular mechanics (QM/MM) methods in classical and quantum simulations. The development of various novel path-integral methods is reviewed. These methods are tailor suited to enzyme systems, where only a few degrees of freedom involved in the chemistry need to be quantized. The application of the hybrid QM/MM quantum-classical simulation approach to three case studies is presented. The first case involves the proton transfer in alanine racemase. The second case presented involves orotidine 5'-monophosphate decarboxylase where multidimensional free energy simulations together with kinetic isotope effects are combined in the study of the reaction mechanism. Finally, we discuss the proton transfer in nitroalkane oxidase, where the enzyme employs tunneling as a catalytic fine-tuning tool. Copyright © 2015 Elsevier Inc. All rights reserved.

  4. Rate equation model of laser induced bias in uranium isotope ratios measured by resonance ionization mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Isselhardt, B. H.; Prussin, S. G.; Savina, M. R.; Willingham, D. G.; Knight, K. B.; Hutcheon, I. D.

    2016-01-01

    Resonance Ionization Mass Spectrometry (RIMS) has been developed as a method to measure uranium isotope abundances. In this approach, RIMS is used as an element-selective ionization process between uranium atoms and potential isobars without the aid of chemical purification and separation. The use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of the U-235/U-238 ratio to decrease laser-induced isotopic fractionation. In application, isotope standards are used to identify and correct bias in measured isotope ratios, but understanding laser-induced bias from first-principles can improve the precision and accuracy of experimental measurements. A rate equation model for predicting the relative ionization probability has been developed to study the effect of variations in laser parameters on the measured isotope ratio. The model uses atomic data and empirical descriptions of laser performance to estimate the laser-induced bias expected in experimental measurements of the U-235/U-238 ratio. Empirical corrections are also included to account for ionization processes that are difficult to calculate from first principles with the available atomic data. Development of this model has highlighted several important considerations for properly interpreting experimental results.

  5. Isotope ratio mass spectrometry in combination with chemometrics for characterization of geographical origin and agronomic practices of table grape.

    Science.gov (United States)

    Longobardi, Francesco; Casiello, Grazia; Centonze, Valentina; Catucci, Lucia; Agostiano, Angela

    2017-08-01

    Although table grape is one of the most cultivated and consumed fruits worldwide, no study has been reported on its geographical origin or agronomic practice based on stable isotope ratios. This study aimed to evaluate the usefulness of isotopic ratios (i.e. (2) H/(1) H, (13) C/(12) C, (15) N/(14) N and (18) O/(16) O) as possible markers to discriminate the agronomic practice (conventional versus organic farming) and provenance of table grape. In order to quantitatively evaluate which of the isotopic variables were more discriminating, a t test was carried out, in light of which only δ(13) C and δ(18) O provided statistically significant differences (P ≤ 0.05) for the discrimination of geographical origin and farming method. Principal component analysis (PCA) showed no good separation of samples differing in geographical area and agronomic practice; thus, for classification purposes, supervised approaches were carried out. In particular, general discriminant analysis (GDA) was used, resulting in prediction abilities of 75.0 and 92.2% for the discrimination of farming method and origin respectively. The present findings suggest that stable isotopes (i.e. δ(18) O, δ(2) H and δ(13) C) combined with chemometrics can be successfully applied to discriminate the provenance of table grape. However, the use of bulk nitrogen isotopes was not effective for farming method discrimination. © 2016 Society of Chemical Industry. © 2016 Society of Chemical Industry.

  6. Estimation of lake water - groundwater interactions in meromictic mining lakes by modelling isotope signatures of lake water.

    Science.gov (United States)

    Seebach, Anne; Dietz, Severine; Lessmann, Dieter; Knoeller, Kay

    2008-03-01

    A method is presented to assess lake water-groundwater interactions by modelling isotope signatures of lake water using meteorological parameters and field data. The modelling of delta(18)O and deltaD variations offers information about the groundwater influx into a meromictic Lusatian mining lake. Therefore, a water balance model is combined with an isotope water balance model to estimate analogies between simulated and measured isotope signatures within the lake water body. The model is operated with different evaporation rates to predict delta(18)O and deltaD values in a lake that is only controlled by weather conditions with neither groundwater inflow nor outflow. Comparisons between modelled and measured isotope values show whether the lake is fed by the groundwater or not. Furthermore, our investigations show that an adaptation of the Craig and Gordon model [H. Craig, L.I. Gordon. Deuterium and oxygen-18 variations in the ocean and the marine atmosphere. In Stable Isotopes in Oceanographic Studies and Paleotemperature, Spoleto, E. Tongiorgi (Ed.), pp. 9-130, Consiglio Nazionale delle Ricerche, Laboratorio di Geologia Nucleare, Pisa (1965).] to specific conditions in temperate regions seems necessary.

  7. Tracing subducted sediment inputs to the Ryukyu arc-Okinawa Trough system: Evidence from thallium isotopes

    Science.gov (United States)

    Shu, Yunchao; Nielsen, Sune G.; Zeng, Zhigang; Shinjo, Ryuichi; Blusztajn, Jerzy; Wang, Xiaoyuan; Chen, Shuai

    2017-11-01

    Sediments are actively subducted in virtually every arc worldwide. However, quantifying their contributions to arc lavas and thereby establishing budgets of how sediments participate in slab-mantle interaction is challenging. In this contribution we use thallium (Tl) abundances and isotopic compositions of lavas from the Ryukyu arc (including south Kyushu) and its back-arc basin, Okinawa Trough, to investigate the influence of sediments from arc to back-arc. We also present extensive geochemical data for sediments and altered oceanic crust (AOC) outboard of the northern (DSDP Sites 296, 442B, 443 and 444) and central (DSDP Sites 294 and 295) part of the Ryukyu arc. The Tl isotopic compositions of sediments change systematically from lighter outboard of northern Ryukyu arc to heavier outboard of central Ryukyu arc. The feature reflects the dominance of terrigenous material and pelagic sedimentation outboard of the northern and central Ryukyu arc, respectively. Central and northern sections of Ryukyu arc and Okinawa Trough display larger range of Tl isotopic variation than southern section, which is consistent with more pelagic provenance for sediments outboard of central and northern Ryukyu arcs than that of expected sediments outboard of southern Ryukyu arc. Identical Tl, Sr, Nd and Pb isotope variations are found when comparing arc and back arc lavas, which indicates that sediments fluxes also account for the Tl isotopic variations in the Okinawa Trough lavas. Two-end-member mixing models of Tl with Pb, Sr and Nd isotopes require sediment inputs ofsediment end members predict very similar sediment fluxes when using Tl, Sr, Nd and Pb isotopes, which indicates that fractionation of these elements must have happened after mixing between mantle and sediments. This conclusion is corroborated by model calculations of mixing between sediment melts with fractionated Sr/Nd ratios and mantle wedge, which show that no arc lava plot on such mixing lines. Thus bulk sediment

  8. CO2-dependent carbon isotope fractionation in the dinoflagellate Alexandrium tamarense

    Science.gov (United States)

    Wilkes, Elise B.; Carter, Susan J.; Pearson, Ann

    2017-09-01

    The carbon isotopic composition of marine sedimentary organic matter is used to resolve long-term histories of pCO2 based on studies indicating a CO2-dependence of photosynthetic carbon isotope fractionation (εP). It recently was proposed that the δ13C values of dinoflagellates, as recorded in fossil dinocysts, might be used as a proxy for pCO2. However, significant questions remain regarding carbon isotope fractionation in dinoflagellates and how such fractionation may impact sedimentary records throughout the Phanerozoic. Here we investigate εP as a function of CO2 concentration and growth rate in the dinoflagellate Alexandrium tamarense. Experiments were conducted in nitrate-limited chemostat cultures. Values of εP were measured on cells having growth rates (μ) of 0.14-0.35 d-1 and aqueous carbon dioxide concentrations of 10.2-63 μmol kg-1 and were found to correlate linearly with μ/[CO2(aq)] (r2 = 0.94) in accord with prior, analogous chemostat investigations with eukaryotic phytoplankton. A maximum fractionation (εf) value of 27‰ was characterized from the intercept of the experiments, representing the first value of εf determined for an algal species employing Form II RubisCO-a structurally and catalytically distinct form of the carbon-fixing enzyme. This value is larger than theoretical predictions for Form II RubisCO and not significantly different from the ∼25‰ εf values observed for taxa employing Form ID RubisCO. We also measured the carbon isotope contents of dinosterol, hexadecanoic acid, and phytol from each experiment, finding that each class of biomarker exhibits different isotopic behavior. The apparent CO2-dependence of εP values in our experiments strengthens the proposal to use dinocyst δ13C values as a pCO2 proxy. Moreover, the similarity between the εf value for A. tamarense and the consensus value of ∼25‰ indicates that the CO2-sensitivity of carbon isotope fractionation saturates at similar CO2 levels across all three

  9. Penning-trap mass measurements of neutron-deficient Rb and Sr isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Otto, T. (Inst. fuer Physik, Univ. Mainz (Germany)); Bollen, G. (Inst. fuer Physik, Univ. Mainz (Germany)); Savard, G. (Inst. fuer Physik, Univ. Mainz (Germany)); Schweikhard, L. (Inst. fuer Physik, Univ. Mainz (Germany)); Stolzenberg, H. (Inst. fuer Physik, Univ. Mainz (Germany)); Audi, G. (CSNSM, IN2P3-CNRS, Lab. Rene Bernas, 91 Orsay (France)); Moore, R.B. (Foster Radiation Lab., McGill Univ., Montreal, PQ (Canada)); Rouleau, G. (Foster Radiation Lab., McGill Univ., Montreal, PQ (Canada)); Szerypo, J. (Inst. of Experimental Physics, Warsaw Univ. (Poland)); Patyk, Z. (Soltan Inst. for Nuclear Studies, Warsaw (Poland)); ISOLDE Collaboration

    1994-01-17

    The Penning-trap mass spectrometer ISOLTRAP installed at the on-line mass separator ISOLDE 2 at CERN has been used for mass determination of [sup 75-87]Rb and [sup 78-83,87]Sr. Ions are captured in a Penning trap and their cyclotron frequency [omega][sub c] =(q/m)B in the trapping field B is measured. Ratios of these frequencies lead to the determination of the atomic mass of these isotopes. A resolving power of typically m/[Delta]m=10[sup 6] and an accuracy y of [delta]m[approx]10 keV is obtained. The mass of [sup 78]Sr is measured for the first time, in most cases, the mass values of the other isotopes are significantly improved. The experimental masses are compared with theoretical predictions. (orig.)

  10. Penning-trap mass measurements of neutron-deficient Rb and Sr isotopes

    Science.gov (United States)

    Otto, T.; Bollen, G.; Savard, G.; Schweikhard, L.; Stolzenberg, H.; Audi, G.; Moore, R. B.; Rouleau, G.; Szerypo, J.; Patyk, Z.; Isolde Collaboration

    1994-01-01

    The Penning-trap mass spectrometer ISOLTRAP installed at the on-line mass separator ISOLDE 2 at CERN has been used for mass determination of 75-87Rb and 78-83,87Sr. Ions are captured in a Penning trap and their cyclotron frequency ω c = ( {q}/{m})B in the trapping field B is measured. Ratios of these frequencies lead to the determination of the atomic mass of these isotopes. A resolving power of typically {m}/{Δm} = 10 6 and an accuracy of δm ≈10 keV is obtained. The mass of 78Sr is measured for the first time and, in most cases, the mass values of the other isotopes are significantly improved. The experimental masses are compared with theoretical predictions.

  11. Mineralogy and Oxygen Isotope Compositions of Two C-Rich Hydrated Interplanetary Dust Particles

    Science.gov (United States)

    Snead, C. J.; McKeegan, K. D.; Messenger, S.; Nakamura-Messenger, K.

    2012-01-01

    Oxygen isotopic compositions of chondrites reflect mixing between a O-16-rich reservoir and a O-17,O-18-rich reservoir produced via mass-independent fractionation. The composition of the O-16-rich reservoir is reasonably well constrained, but material representing the O-17,O-18-rich end-member is rare. Self-shielding models predict that cometary water, presumed to represent this reservoir, should be enriched in O-17 and O-18 18O by > 200%. Hydrated interplanetary dust particles (IDPs) rich in carbonaceous matter may be derived from comets; such particles likely contain the products of reaction between O-16-poor water and anhydrous silicates that formed in the inner solar system. Here we present mineralogy and oxygen isotope compositions of two C-rich hydrated IDPs, L2083E47 and L2071E35.

  12. Shell closures in Fl superheavy isotopes via determination of alpha decay preformation factor

    Science.gov (United States)

    Alsaif, Norah A. M.; Radiman, Shahidan; Saleh Ahmed, Saad M.

    2017-10-01

    Based on the hypothesized cluster-formation model (CFM), the α-decay preformation factors of superheavy isotopes of Flerovium (Fl) with atomic number Z = 114 and neutron numbers 150 ≤ N ≤ 196 were determined. The formula from the CFM used depends on the eigenvalues of the cluster-formation energy of the α particles and the total energy values of the parent nuclei. The binding energy difference was used to determine these values. The results from the calculations for these isotopes reflect some properties of their nuclear structure. Within the CFM, the prediction of the magic nucleus occurs at N = 172 and Z = 114. Our results indicate towards the existence of shell closure of the stabilization superheavy nuclei.

  13. Observations of the Li, Be, and B isotopes and Constraints on Cosmic-ray Propagation

    Energy Technology Data Exchange (ETDEWEB)

    de Nolfo, Georgia A.; Moskalenko, I.V.; Binns, W.R.; Christian, E.R.; Cummings, A.C.; Davis, A.J.; George, J.S.; Hink, P.L.; Israel, M.H.; Leske, R.A.; Lijowski, M.; Mewaldt, R.A.; Stone, E.C.; Strong, A.W.; von Rosenvinge, T.T.; Wiedenbeck, M.E.; Yanasak, N.E.; /NASA, Goddard /Stanford U., HEPL /Washington U., St. Louis /NASA, Headquarters

    2006-11-15

    The abundance of Li, Be, and B isotopes in galactic cosmic rays (GCR) between E=50-200 MeV/nucleon has been observed by the Cosmic Ray Isotope Spectrometer (CRIS) on NASA's ACE mission since 1997 with high statistical accuracy. Precise observations of Li, Be, B can be used to constrain GCR propagation models. We find that a diffusive reacceleration model with parameters that best match CRIS results (e.g. B/C, Li/C, etc) are also consistent with other GCR observations. A {approx}15-20% overproduction of Li and Be in the model predictions is attributed to uncertainties in the production cross-section data. The latter becomes a significant limitation to the study of rare GCR species that are generated predominantly via spallation.

  14. Neutron transfer in the 13C+197Au reaction from gold isotope residuals

    Science.gov (United States)

    Daub, B. H.; Bleuel, D. L.; Wiedeking, M.; Bernstein, L. A.; Brickner, N. M.; Brown, J. A.; Goldblum, B. L.; Holliday, K. S.; Lundgren, J.; Moody, K.

    2017-08-01

    Residual gold nuclei were produced via neutron transfer at multiple energies using a 130-MeV 13C beam incident on a stacked-foil target consisting of alternating layers of 197Au and 27Al. Production cross sections, over an energy range of 56 to 129 MeV, for seven gold isotopes and two gold isomers were determined through activation analysis. By using the Wilczyński binary transfer model with a modified version of the recoil formula and a standard evaporation model, we were able to reproduce the isotopic production cross sections at high beam energy, with some disagreement at lower beam energies. This limiting angular momentum model does not predict the transfer of sufficient angular momentum to reproduce the observed isomeric populations.

  15. Stable Chlorine Isotope Study: Application to Early Solar System Materials

    Science.gov (United States)

    Mala,ira. M/; Nyquist, L. E.; Reese, Y.; Shih, C-Y; Fujitani, T.; Okano, O.

    2010-01-01

    A significantly large mass fractionation between two stable chlorine isotopes is expected during planetary processes In addition, in view of the isotopic heterogeneity of other light elements, the chlorine isotopes can potentially be used as a tracer for the origins and evolutionary processes of early solar system materials. Due to analytical difficulties, however, current chlorine isotope studies on planetary materials are quite controversial among IRMS (gas source mass spectrometry) and/or TIMS (Thermal Ionization Mass Spectrometry) groups [i.e. 1-3]. Although a cross-calibration of IRMS and TIMS indicates that both techniques are sufficiently consistent with each other [4], some authors have claimed that the Cl-37/Cl-35 ratio of geological samples obtained by TIMS technique are, in general, misleadingly too high and variable compared to those of IRMS [3]. For example, almost no differences of Cl isotope composition were observed among mantle materials and carbonaceous meteorites by [3]. On the other hand, according to more recent IRMS work [2], significant Cl isotope variations are confirmed for mantle materials. Therefore, additional careful investigation of Cl isotope analyses are now required to confirm real chlorine isotope variations for planetary materials including carbonaceous chondrites [5]. A significantly large mass fractionation between two stable chlorine isotopes is expected during planetary processes In addition, in view of the isotopic heterogeneity of other light elements, the chlorine isotopes can potentially be used as a tracer for the origins and evolutionary processes of early solar system materials. Due to analytical difficulties, however, current chlorine isotope studies on planetary materials are quite controversial among IRMS (gas source mass spectrometry) and/or TIMS (Thermal Ionization Mass Spectrometry) groups [i.e. 1-3]. Although a cross-calibration of IRMS and TIMS indicates that both techniques are sufficiently consistent with each

  16. Simulating Isotope Enrichment by Gaseous Diffusion

    Science.gov (United States)

    Reed, Cameron

    2015-04-01

    A desktop-computer simulation of isotope enrichment by gaseous diffusion has been developed. The simulation incorporates two non-interacting point-mass species whose members pass through a cascade of cells containing porous membranes and retain constant speeds as they reflect off the walls of the cells and the spaces between holes in the membranes. A particular feature is periodic forward recycling of enriched material to cells further along the cascade along with simultaneous return of depleted material to preceding cells. The number of particles, the mass ratio, the initial fractional abundance of the lighter species, and the time between recycling operations can be chosen by the user. The simulation is simple enough to be understood on the basis of two-dimensional kinematics, and demonstrates that the fractional abundance of the lighter-isotope species increases along the cascade. The logic of the simulation will be described and results of some typical runs will be presented and discussed.

  17. Isotopic And Geochemical Investigations Of Meteorites

    Science.gov (United States)

    Walker, Richard J.

    2005-01-01

    The primary goals of our research over the past four years are to constrain the timing of certain early planetary accretion/differentiation events, and to constrain the proportions and provenance of materials involved in these processes. This work was achieved via the analysis and interpretation of long- and short-lived isotope systems, and the study of certain trace elements. Our research targeted these goals primarily via the application of the Re-187, Os-187, Pt-190 Os-186 Tc-98 Ru-99 and Tc-99 Ru-99 isotopic systems, and the determination/modeling of abundances of the highly siderophile elements (HSE; including Re, Os, Ir, Ru, Pd, Pt, and maybe Tc). The specific events we examined include the segregation and crystallization histories of asteroidal cores, the accretion and metamorphic histories of chondrites and chondrite components, and the accretionary and differentiation histories of Mars and the Moon.

  18. Oxygen Isotope Systematics of Almahata Sitta

    Science.gov (United States)

    Kita, N. T.; Goodrich, C. A.; Herrin, J. S.; Shaddad, M. H.; Jenniskens, P.

    2011-01-01

    The Almahata Sitta (hereafter "AHS") meteorite was derived from an impact of asteroid 2008TC3 on Earth and is classified as an anomalous polymict ureilite. More than 600 meteorite fragments have been recovered from the strewnfield. Previous reports indicate that these fragments consist mainly of ureilitic materials with textures and compositions, while some fragments are found to be chondrites of a wide range of chemical classes. Bulk oxygen three isotope analyses of ureilitic fragments from AHS fall close to the CCAM (Carbonaceous Chondrite Anhydrous Mineral) line similar to ureilites. In order to further compare AHS with known ureilites, we performed high precision SIMS (Secondary Ion Mass Spectrometer) oxygen isotope analyses of some AHS samples

  19. On-line orientation of bromine isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Barham, C.G.; Alghamdi, S.S.; Grant, I.S. (Schuster Lab., Manchester Univ. (United Kingdom)); Bhagwat, A.; Singleton, B.D.D.; Walker, P.M. (Dept. of Physics, Univ. of Surrey, Guildford (United Kingdom)); Booth, M.; Lindroos, M.; Rikovska, J.; Stone, N.J. (Clarendon Lab., Oxford Univ. (United Kingdom))

    1992-11-01

    Assignments for the principal Nilsson configuration in light [beta][sup +]-decaying bromine isotopes were proposed in a contribution to the OLNO-1 conference. These assignments were made on the basis of magnetic moments derived from the temperature dependence of anisotropies in daughter Se isotopes observed in the DOLIS-COLD facility at Daresbury. Anisotropy measurements have since been extended to a lower base temperature in [sup 74m]Br and [sup 72g]Br decay, leading to more stringent limits on the ground state moment of [sup 72]Br. The proposed [pi][312]3/2 configuration for [sup 75]Br has also now been confirmed by a measurement of the sign of its magnetic moment. This was done by observing the [beta]-asymmetry in [sup 75]Br decay using high purity Si detectors mounted within the dilution refrigerator. (orig.).

  20. (n,{gamma}) Experiments on tin isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Baramsai, B.; Mitchell, G. E.; Walker, C. L.; Rusev, G. [North Carolina State University, Raleigh, NC 27695, USA and Triangle Universities Nuclear Laboratory, Durham, NC 27708 (United States); Bredeweg, T. A.; Couture, A.; Haight, R. C.; Jandel, M.; Mosby, S.; O' Donnell, J. M.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J. [Los Alamos National Laboratory, P.O. Box 1663, Los Alamos, NM 87545 (United States); Becvar, F.; Krticka, M.; Kroll, J. [Charles University of Prague, V Holesovickach 2, 180 00 Prague 8 (Czech Republic); Agvaanluvsan, U.; Dashdorj, D.; Erdenehuluun, B.; Tsend-Ayush, T. [MonAme Scientific Research Center, Ulaanbaatar (Mongolia)

    2013-04-19

    Neutron capture experiments on highly enriched {sup 117,119}Sn isotopes were performed with the DANCE detector array located at the Los Alamos Neutron Science Center. The DANCE detector provides detailed information about the multi-step {gamma}-ray cascade following neutron capture. Analysis of the experimental data provides important information to improve understanding of the neutron capture reaction, including a test of the statistical model, the assignment of spins and parities of neutron resonances, and information concerning the Photon Strength Function (PSF) and Level Density (LD) below the neutron separation energy. Preliminary results for the (n,{gamma}) reaction on {sup 117,119}Sn are presented. Resonance spins of the odd-A tin isotopes were almost completely unknown. Resonance spins and parities have been assigned via analysis of the multi-step {gamma}-ray spectra and directional correlations.

  1. The Oxygen Isotopic Composition of the Sun

    Science.gov (United States)

    McKeegan, K. D.; Kallio, A.; Heber, V. S.; Jarzebinski, G.; Mao, P.; Coath, C.; Kunihiro, T.; Wiens, R. C.; Judith, A.; Burnett, D. S.

    2010-12-01

    An accurate and precise determination of the oxygen isotopic composition of the Sun is the highest priority scientific goal of the Genesis Mission [1] as such data would provide a baseline from which one could interpret the oxygen isotopic anomalies found at all spatial scales in inner solar system materials. We have measured oxygen isotope compositions of implanted solar wind in 40 spots along a radial traverse of the Genesis SiC target sample 60001 by depth profiling with the UCLA MegaSIMS [2]. Mass-dependent fractionation induced by the solar wind concentrator [3] ion optics was corrected by comparison of the concentrator 22Ne/20Ne with that measured in a bulk solar wind target (diamond-like carbon on Si, [4]). The solar wind captured at L1 has an isotopic composition of (δ18O, δ17O) ≈ (-99, -79)‰, a value which is far removed from the terrestrial mass fractionation line. Profiles from the central portion of the target, where solar concentrations are highest and background corrections minimal, yield a mean Δ17O = -28.3 ± 1.8 ‰ indicating that the Earth and other planetary materials from the inner solar system are highly depleted in 16O relative to the solar wind. A mass-dependent fractionation of ~ -20%/amu in the acceleration of solar wind is required if we hypothesize that the photospheric oxygen isotope value, which represents the bulk starting composition of the solar system, is on the 16O-mixing line characteristic of refractory phase in primitive meteorites [5]. With this assumption, our preferred value for the bulk solar oxygen isotope composition is δ18O ≈ δ17O ≈ -57‰. A mechanism is required to fractionate oxygen isotopes in a non-mass-dependent manner to deplete 16O by ~6 to 7% in the rocky materials of the solar nebula. As oxygen is the third most abundant element in the solar system, and the most abundant in the terrestrial planets, this mechanism must operate on a large scale. Isotope-selective photochemistry, for example as in

  2. Propagation of Isotopic Bias and Uncertainty to Criticality Safety Analyses of PWR Waste Packages

    Energy Technology Data Exchange (ETDEWEB)

    Radulescu, Georgeta [ORNL

    2010-06-01

    Burnup credit methodology is economically advantageous because significantly higher loading capacity may be achieved for spent nuclear fuel (SNF) casks based on this methodology as compared to the loading capacity based on a fresh fuel assumption. However, the criticality safety analysis for establishing the loading curve based on burnup credit becomes increasingly complex as more parameters accounting for spent fuel isotopic compositions are introduced to the safety analysis. The safety analysis requires validation of both depletion and criticality calculation methods. Validation of a neutronic-depletion code consists of quantifying the bias and the uncertainty associated with the bias in predicted SNF compositions caused by cross-section data uncertainty and by approximations in the calculational method. The validation is based on comparison between radiochemical assay (RCA) data and calculated isotopic concentrations for fuel samples representative of SNF inventory. The criticality analysis methodology for commercial SNF disposal allows burnup credit for 14 actinides and 15 fission product isotopes in SNF compositions. The neutronic-depletion method for disposal criticality analysis employing burnup credit is the two-dimensional (2-D) depletion sequence TRITON (Transport Rigor Implemented with Time-dependent Operation for Neutronic depletion)/NEWT (New ESC-based Weighting Transport code) and the 44GROUPNDF5 crosssection library in the Standardized Computer Analysis for Licensing Evaluation (SCALE 5.1) code system. The SCALE 44GROUPNDF5 cross section library is based on the Evaluated Nuclear Data File/B Version V (ENDF/B-V) library. The criticality calculation code for disposal criticality analysis employing burnup credit is General Monte Carlo N-Particle (MCNP) Transport Code. The purpose of this calculation report is to determine the bias on the calculated effective neutron multiplication factor, k{sub eff}, due to the bias and bias uncertainty associated with

  3. Stable isotope ratios of rain and vapor in 1995 hurricanes

    Science.gov (United States)

    Lawrence, James Robert; Gedzelman, Stanley David; Zhang, Xiaoping; Arnold, Robert

    1998-05-01

    Isotope ratios of rain and vapor samples collected at the surface from four tropical cyclones during the active 1995 Atlantic hurricane season were determined. A two-dimensional bulk microphysics isotope model was applied to steady symmetric tropical cyclones to explain the observed low mean values and inward decrease of isotope ratios of the rain and vapor. The low mean value is caused by the tropical cyclone's relatively large size, longevity, and deep clouds. The inward decrease is due to diffusive isotope exchange between falling rain and converging vapor in the atmospheric boundary layer. Dean, a minimal tropical storm, produced relatively high isotope ratios because of its small size and youth. Rains from the extreme outer edge of Felix, a category 3 hurricane, exhibited high isotope ratios similar to normal summer rain. Isotope ratios of rains and vapors from Hurricane Luis in Puerto Rico decreased as the storm approached. Isotope ratios of rain exhibited an abrupt jump from low values in the eastern half of Puerto Rico to high values farther west which is linked to the storm's rainbands. Isotope ratios of Hurricane Opal's rains reflected the storm's asymmetric structure, with lowest values west of the point of landfall. Record low isotope ratios from a squall line that struck eastern Texas two days before landfall are linked to low-level outflow from Opal and demonstrate that hurricanes can vent enormous quantities of vapor to the surroundings.

  4. Measurement system analysis (MSA) of the isotopic ratio for uranium isotope enrichment process control

    Energy Technology Data Exchange (ETDEWEB)

    Medeiros, Josue C. de; Barbosa, Rodrigo A.; Carnaval, Joao Paulo R., E-mail: josue@inb.gov.br, E-mail: rodrigobarbosa@inb.gov.br, E-mail: joaocarnaval@inb.gov.br [Industrias Nucleares do Brasil (INB), Rezende, RJ (Brazil)

    2013-07-01

    Currently, one of the stages in nuclear fuel cycle development is the process of uranium isotope enrichment, which will provide the amount of low enriched uranium for the nuclear fuel production to supply 100% Angra 1 and 20% Angra 2 demands. Determination of isotopic ration n({sup 235}U)/n({sup 238}U) in uranium hexafluoride (UF{sub 6} - used as process gas) is essential in order to control of enrichment process of isotopic separation by gaseous centrifugation cascades. The uranium hexafluoride process is performed by gas continuous feeding in separation unit which uses the centrifuge force principle, establishing a density gradient in a gas containing components of different molecular weights. The elemental separation effect occurs in a single ultracentrifuge that results in a partial separation of the feed in two fractions: an enriched on (product) and another depleted (waste) in the desired isotope ({sup 235}UF{sub 6}). Industrias Nucleares do Brasil (INB) has used quadrupole mass spectrometry (QMS) by electron impact (EI) to perform isotopic ratio n({sup 235}U)/n({sup 238}U) analysis in the process. The decision of adjustments and change te input variables are based on the results presented in these analysis. A study of stability, bias and linearity determination has been performed in order to evaluate the applied method, variations and systematic errors in the measurement system. The software used to analyze the techniques above was the Minitab 15. (author)

  5. Utilizing Stable Isotopes and Isotopic Anomalies to Study Early Solar System Formation Processes

    Science.gov (United States)

    Simon, Justin

    2017-01-01

    Chondritic meteorites contain a diversity of particle components, i.e., chondrules and calcium-, aluminum-rich refractory inclusions (CAIs), that have survived since the formation of the Solar System. The chemical and isotopic compositions of these materials provide a record of the conditions present in the protoplanetary disk where they formed and can aid our understanding of the processes and reservoirs in which solids formed in the solar nebula, an important step leading to the accretion of planetesimals. Isotopic anomalies associated with nucleosynthetic processes are observed in these discrete materials, and can be compared to astronomical observations and astrophysical formation models of stars and more recently proplyds. The existence and size of these isotopic anomalies are typically thought to reflect a significant state of isotopic heterogeneity in the earliest Solar System, likely left over from molecular cloud heterogeneities on the grain scale, but some could also be due to late stellar injection. The homogenization of these isotopic anomalies towards planetary values can be used to track the efficiency and timescales of disk wide mixing,

  6. Daresbury on-line isotope separator (DOLIS)

    Energy Technology Data Exchange (ETDEWEB)

    Grant, I.S.; Eastham, D.A.; Groves, J.; Tolfree, D.W.L.; Walker, P.M.; Green, V.R.; Rikovska, J.; Stone, N.J.; Hamilton, W.D.

    1987-05-01

    The isotope separator DOLIS, which is on-line to the Daresbury Laboratory's 20-MV tandem accelerator, is used to measure nuclear moments and decay schemes. Separated beams may be collected on a tape and transported to a counting station, implanted directly into a host lattice at on-line temperatures down to less than 10 mK, or allowed to interact with a collinear laser beam. The present status of DOLIS and its ancillary equipment is described.

  7. Graphs for Isotopes of 108-Hs (Hassium)

    Science.gov (United States)

    Sukhoruchkin, S. I.; Soroko, Z. N.

    This document is part of the Supplement containing the complete sets of data of Subvolume B `Nuclei with Z = 55 - 100' of Volume 22 `Nuclear Binding Energies and Atomic Masses' of Landolt-Börnstein - Group I `Elementary Particles, Nuclei and Atoms', and additionally including data for nuclei with Z = 101 - 130. It provides a graphic representation of nucleon separation energies and residual interaction parameters for isotopes of the chemical element 108-Hs (Hassium, atomic number Z = 108).

  8. Groundwater Paleohydrology Using Microsample Sr Isotopic Data

    Science.gov (United States)

    Farmer, G.; Fritz, D. E.

    2003-12-01

    Physical microsampling of silicate alteration phases produced during past episodes of groundwater flow, combined with Sr isotopic data, can be used to determine the age of the alteration phases and to define paleogroundwater flow paths. For example, we have obtained microsamples of secondary adularia present in the K-metasomatized, mid-Tertiary Lemitar Tuff in southern New Mexico. The microsamples (~25 micrograms) yield a Rb-Sr "errochron" (MSWD~29) of 6.3 Ma, and an 87Sr/86Sr (6 Ma)=0.7206. The adularia isotopic compositions are considerably higher than those determined for igneous plagioclase and sanidine phenocrysts in the same tuff (0.710), or for the tuff matrix, and indicate that the radiogenic Sr incorporated into the adularia was introduced to the tuff during alteration. Na-Ca sulfates present in playa deposits in the Tertiary Popotosa Formation have Sr isotopic compositions similar to the unaltered tuffs, and not the adularia, and suggest that the fluids responsible for the K-metasomatism of the Lemitar Tuff were not down-flowing saline fluids originating from playa lakes in the Popotosa Basin. Instead, we argue that the fluids were generated during topographically driven flow of meteoric waters through high 87Sr/86Sr Precambrian basement-cored horsts generated during early Basin and Range extension in this area. These data illustrate the utility of such Sr isotopic information in investigations of paleogroundwater flow and we are currently extending the technique to study the origin of the multiple low-T groundwater flow events recorded in the various secondary silicate, sulfate, and carbonate phases present in the Late Paleozoic Fountain Formation in northern Colorado.

  9. Nuclear sizes and the isotope shift

    OpenAIRE

    Friar, J. L.; Martorell Domenech, Juan; Sprung, Donald W. L.

    1997-01-01

    Darwin-Foldy nuclear-size corrections in electronic atoms and nuclear radii are discussed from the nuclear-physics perspective. The interpretation of precise isotope-shift measurements is formalism dependent, and care must be exercised in interpreting these results and those obtained from relativistic electron scattering from nuclei. We strongly advocate that the entire nuclear-charge operator be used in calculating nuclear-size corrections in atoms rather than relegating portions of it to th...

  10. Oxygen and hydrogen isotope geochemistry of zeolites

    Science.gov (United States)

    Karlsson, Haraldur R.; Clayton, Robert N.

    1990-01-01

    Oxygen and hydrogen isotope ratios for natural samples of the zeolites analcime, chabazite, clinoptilolite, laumontite, mordenite, and natrolite have been obtained. The zeolite samples were classified into sedimentary, hydrothermal, and igneous groups. The ratios for each species of zeolite are reported. The results are used to discuss the origin of channel water, the role of zeolites in water-rock interaction, and the possibility that a calibrated zeolite could be used as a low-temperature geothermometer.

  11. Stable isotopic analyses in paleoclimatic reconstruction

    Energy Technology Data Exchange (ETDEWEB)

    Wigand, P.E. [Univ. and Community College System of Nevada, Reno, NV (United States)

    1995-09-01

    Most traditional paleoclimatic proxy data have inherent time lags between climatic input and system response that constrain their use in accurate reconstruction of paleoclimate chronology, scaling of its variability, and the elucidation of the processes that determine its impact on the biotic and abiotic environment. With the exception of dendroclimatology, and studies of short-lived organisms and pollen recovered from annually varved lacustrine sediments, significant periods of time ranging from years, to centuries, to millennia may intervene between climate change and its first manifestation in paleoclimatic proxy data records. Reconstruction of past climate through changes in plant community composition derived from pollen sequences and plant remains from ancient woodrat middens, wet environments and dry caves all suffer from these lags. However, stable isotopic analyses can provide more immediate indication of biotic response to climate change. Evidence of past physiological response of organisms to changes in effective precipitation as climate varies can be provided by analyses of the stable isotopic content of plant macrofossils from various contexts. These analyses consider variation in the stable isotopic (hydrogen, oxygen and carbon) content of plant tissues as it reflects (1) past global or local temperature through changes in meteoric (rainfall) water chemistry in the case of the first two isotopes, and (2) plant stress through changes in plant respiration/transpiration processes under differing water availability, and varying atmospheric CO, composition (which itself may actually be a net result of biotic response to climate change). Studies currently being conducted in the Intermountain West indicate both long- and short-term responses that when calibrated with modem analogue studies have the potential of revealing not only the timing of climate events, but their direction, magnitude and rapidity.

  12. Iron isotope fractionation in marine invertebrates in near shore environments

    Science.gov (United States)

    Emmanuel, S.; Schuessler, J. A.; Vinther, J.; Matthews, A.; von Blanckenburg, F.

    2014-04-01

    Chitons (Mollusca) are marine invertebrates that produce radula (teeth or rasping tongue) containing high concentrations of biomineralized magnetite and other iron bearing minerals. As Fe isotope signatures are influenced by redox processes and biological fractionation, Fe isotopes in chiton radula might be expected to provide an effective tracer of ambient oceanic conditions and biogeochemical cycling. Here, in a pilot study to measure Fe isotopes in marine invertebrates, we examine Fe isotopes in modern marine chiton radula collected from different locations in the Atlantic and Pacific oceans to assess the range of isotopic values, and to test whether or not the isotopic signatures reflect seawater values. Furthermore, by comparing two species that have very different feeding habits but collected from the same location, we infer a possible link between diet and Fe isotopic signatures. Values of δ56Fe (relative to IRMM-014) in chiton teeth range from -1.90 to 0.00‰ (±0.05‰ (2σ) uncertainty in δ56Fe), probably reflecting a combination of geographical control and biological fractionation processes. Comparison with published local surface seawater Fe isotope data shows a consistent negative offset of chiton teeth Fe isotope compositions relative to seawater. Strikingly, two different species from the same locality in the North Pacific (Puget Sound, Washington, USA) have distinct isotopic signatures. Tonicella lineata, which feeds on red algae, has a mean δ56Fe of -0.65 ± 0.26‰ (2σ, 3 specimens), while Mopalia muscosa, which feeds primarily on green algae, shows lighter isotopic values with a mean δ56Fe of -1.47 ± 0.98‰ (2σ, 5 specimens). Although chitons are not simple recorders of the ambient seawater Fe isotopic signature, these preliminary results suggest that Fe isotopes provide information concerning Fe biogeochemical cycling in near shore environments, and might be used to probe sources of Fe in the diets of different organisms.

  13. Ab initio calculations of Li and B equilibrium isotope fractionation between high -P and -T minerals and aqueous fluids

    Science.gov (United States)

    Kowalski, P.; Jahn, S.; Wunder, B.

    2011-12-01

    Stable isotopes are excellent geochemical tracers widely used in petrology. Among them the isotopes of light elements such as Li or B strongly fractionate between minerals and aqueous fluids during fluid-rock interaction processes, which makes them excellent tracers of mass transfer processes in the subduction cycle. In order to use the full power of isotopes tracing methods the isotope fractionation mechanisms and fractionation factors between minerals and fluids of interest must be well known and characterized. One of the most important mechanisms leading to the formation of isotopic signatures is the equilibrium isotope fractionation, which nowadays can be modeled on the atomic scale by modern computational methods. However, due to high computational requirements the current works have been limited to calculations of simple materials only. In order to overcome these limitations we develop an efficient ab initio based computational approach for prediction of the equilibrium isotope fractionation factors between high pressure and temperature materials, including fluids, which would allow for efficient calculations of the isotope fractionation factors of complex minerals and fluids containing even hundreds of atoms in the supercell. We will show our results for the Li and B stable equilibrium isotope fractionation factors between complex Li/B-bearing crystalline solids (staurolite, spodumene, tourmaline, olenite and micas) and aqueous fluids. The fractionation factors were obtained in an efficient way by simplifying the consideration to calculations of the properties of fractionating atoms only. The comparison of the calculated fractionation factors, on the qualitative and quantitative levels, with the existing experimental data show the comparable to the in situ experimental techniques, predictive power of the computations. We show that with the atomistic scale modelling we are able to reproduce correctly the experimental isotope fractionation sequences

  14. Compositional and stable carbon isotopic fractionation during non-autocatalytic thermochemical sulfate reduction by gaseous hydrocarbons

    Science.gov (United States)

    Xia, Xinyu; Ellis, Geoffrey S.; Ma, Qisheng; Tang, Yongchun

    2014-01-01

    The possibility of autocatalysis during thermochemical sulfate reduction (TSR) by gaseous hydrocarbons was investigated by examination of previously reported laboratory and field data. This reaction was found to be a kinetically controlled non-autocatalytic process, and the apparent lack of autocatalysis is thought to be due to the absence of the required intermediate species. Kinetic parameters for chemical and carbon isotopic fractionations of gaseous hydrocarbons affected by TSR were calculated and found to be consistent with experimentally derived values for TSR involving long-chain hydrocarbons. Model predictions based on these kinetic values indicate that TSR by gaseous hydrocarbon requires high-temperature conditions. The oxidation of C2–5 hydrocarbons by sulfate reduction is accompanied by carbon isotopic fractionation with the residual C2–5 hydrocarbons becoming more enriched in 13C. Kinetic parameters were calculated for the stable carbon isotopic fractionation of gaseous hydrocarbons that have experienced TSR. Model predictions based on these kinetics indicate that it may be difficult to distinguish the effects of TSR from those of thermal maturation at lower levels of hydrocarbon oxidation; however, unusually heavy δ13C2+ values (>−10‰) can be diagnostic of high levels of conversion (>50%). Stoichiometric and stable carbon isotopic data show that methane is stable under the investigated reaction conditions and is likely a product of TSR by other gaseous hydrocarbons rather than a significant reactant. These results indicate that the overall TSR reaction mechanism for oxidation of organic substrates containing long-chain hydrocarbons involves three distinct phases as follows: (1) an initial slow and non-autocatalytic stage characterized by the reduction of reactive sulfate by long-chain saturated hydrocarbons; (2) a second autocatalytic reaction phase dominated by reactions involving reduced sulfur species and partially oxidized hydrocarbons; (3

  15. Radial mixing and Ru-Mo isotope systematics under different accretion scenarios

    Science.gov (United States)

    Fischer, Rebecca A.; Nimmo, Francis; O'Brien, David P.

    2018-01-01

    The Ru-Mo isotopic compositions of inner Solar System bodies may reflect the provenance of accreted material and how it evolved with time, both of which are controlled by the accretion scenario these bodies experienced. Here we use a total of 116 N-body simulations of terrestrial planet accretion, run in the Eccentric Jupiter and Saturn (EJS), Circular Jupiter and Saturn (CJS), and Grand Tack scenarios, to model the Ru-Mo anomalies of Earth, Mars, and Theia analogues. This model starts by applying an initial step function in Ru-Mo isotopic composition, with compositions reflecting those in meteorites, and traces compositional evolution as planets accrete. The mass-weighted provenance of the resulting planets reveals more radial mixing in Grand Tack simulations than in EJS/CJS simulations, and more efficient mixing among late-accreted material than during the main phase of accretion in EJS/CJS simulations. We find that an extensive homogeneous inner disk region is required to reproduce Earth's observed Ru-Mo composition. EJS/CJS simulations require a homogeneous reservoir in the inner disk extending to ≥3-4 AU (≥74-98% of initial mass) to reproduce Earth's composition, while Grand Tack simulations require a homogeneous reservoir extending to ≥3-10 AU (≥97-99% of initial mass), and likely to ≥6-10 AU. In the Grand Tack model, Jupiter's initial location (the most likely location for a discontinuity in isotopic composition) is ∼3.5 AU; however, this step location has only a 33% likelihood of producing an Earth with the correct Ru-Mo isotopic signature for the most plausible model conditions. Our results give the testable predictions that Mars has zero Ru anomaly and small or zero Mo anomaly, and the Moon has zero Mo anomaly. These predictions are insensitive to wide variations in parameter choices.

  16. PREFACE: Processes in Isotopes and Molecules

    Science.gov (United States)

    Bogdan, Diana; Tosa, Valer

    2009-07-01

    These Proceedings present some of the Invited Lectures and Contributed Papers of the International Conference 'Processes in Isotopes and Molecules' (PIM), held in Cluj-Napoca, Romania, 24-26 September 2009. The PIM conference, started in 1999 as a local event, is now an international conference organized every two years by the National Institute for R&D of Isotopic and Molecular Technologies in Cluj-Napoca, the capital city of Transylvania, Romania. The meetings are attended by researchers in the field of atomic and molecular physics as well as those developing new materials and technologies. The scientific subjects are at the cross-roads of three fundamental research areas: physics, chemistry, and biology. The papers here are grouped according to the five conference topics: T1 - Molecular and biomolecular systems T2 - Modern techniques and technologies T3 - Environmental molecular processes T4 - Hydrogen and renewable sources of energy T5 - Nanostructured materials and nanocomposites We gratefully acknowledge the contribution of our colleagues from the Scientific Committee and Program Committee who contributed their time, energy and expertise to the refereeing process. Finally, we would like to thank people from IOP Publishing for their friendly advice and prompt help during the editing process, as well as for their efforts making the Journal of Physics: Conference Series available to the scientific community. Diana Bogdan and Valer Tosa National Institute for R&D Isotopic and Molecular Technologies, Cluj-Napoca

  17. Radium isotopes in the Ulsan Bay

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Jae Seong [Department of Oceanography, Chungnam National University, Gung-dong 220, Yuseong, Daejeon 305-764 (Korea, Republic of)]. E-mail: leejs728@nfrda.re.kr; Kim, Kee Hyun [Department of Oceanography, Chungnam National University, Gung-dong 220, Yuseong, Daejeon 305-764 (Korea, Republic of); Moon, Duck Soo [Department of Oceanography, Chungnam National University, Gung-dong 220, Yuseong, Daejeon 305-764 (Korea, Republic of)

    2005-07-01

    In order to estimate the fluxes of Ra isotopes, we measured {sup 224}Ra, {sup 226}Ra, and {sup 228}Ra activities in the Ulsan Bay mixing zone. The convex upwards curvature of the plot of Ra isotope activities versus salinity for the mixing zone suggests that Ra isotopes are supplied from particles entering the mixing zone from both the river and bottom sediments. This addition increases the estuarine flux of {sup 226}Ra and {sup 228}Ra to the outer sea by factors of 15 and 95 over the flux attributable to Ra dissolved in the riverine water alone. In order to estimate the residence time of the water in Ulsan Bay, we applied a mass balance model to the distribution of {sup 224}Ra and {sup 226}Ra activities in the Ulsan Bay mixing zone with the inflow from the Taehwa River. The obtained residence times of the waters in the Ulsan Bay were estimated to be 6.8-11.4 d. The waters in the upper part of the estuary have long residence times whereas those in the lower part, in contact with the open sea, have shorter residence times. The mean residence time of the water in the Ulsan Bay was estimated to be 9.1 d.

  18. AMS of the Minor Plutonium Isotopes

    Science.gov (United States)

    Steier, P.; Hrnecek, E.; Priller, A.; Quinto, F.; Srncik, M.; Wallner, A.; Wallner, G.; Winkler, S.

    2013-01-01

    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu = (5.7 ± 1.0) × 10−5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method. PMID:23565016

  19. Measuring Isotope Ratios Across the Solar System

    Science.gov (United States)

    Webster, Chris R.; Mahaffy, Paul R.

    2012-01-01

    Stable isotope ratios in C, H, N, O and S are powerful indicators of a wide variety of planetary geophysical processes that can identify origin, transport, temperature history, radiation exposure, atmospheric escape, environmental habitability and biology [1]. For the Allan Hills 84001 meteorite, for example, the (sup 1)(sup 3)C/(sup 1)(sup 2)C ratio identifies it as a Mars (SNC) meteorite; the ??K/??Ar ratio tells us the last time the rock cooled to solid, namely 4 Gya; isotope ratios in (sup 3)He, (sup 2)(sup 1)Ne and (sup 3)?Ar show it was in space (cosmic ray exposure) for 10-20 million years; (sup 1)?C dating that it sat in Antarctica for 13,000 years before discovery; and clumped isotope analysis of (sup 1)?O(sup 1)(sup 3)C(sup 1)?O in its carbonate that it was formed at 18+/-4 ?C in a near-surface aqueous environment [2]. Solar System Formation

  20. Isotopic fractionation of tritium in biological systems.

    Science.gov (United States)

    Le Goff, Pierre; Fromm, Michel; Vichot, Laurent; Badot, Pierre-Marie; Guétat, Philippe

    2014-04-01

    Isotopic fractionation of tritium is a highly relevant issue in radiation protection and requires certain radioecological considerations. Sound evaluation of this factor is indeed necessary to determine whether environmental compartments are enriched/depleted in tritium or if tritium is, on the contrary, isotopically well-distributed in a given system. The ubiquity of tritium and the standard analytical methods used to assay it may induce biases in both the measurement and the signification that is accorded to the so-called fractionation: based on an exhaustive review of the literature, we show how, sometimes large deviations may appear. It is shown that when comparing the non-exchangeable fraction of organically bound tritium (neOBT) to another fraction of tritium (e.g. tritiated water) the preparation of samples and the measurement of neOBT reported frequently led to underestimation of the ratio of tritium to hydrogen (T/H) in the non-exchangeable compartment by a factor of 5% to 50%. In the present study, corrections are proposed for most of the biological matrices studied so far. Nevertheless, the values of isotopic fractionation reported in the literature remain difficult to compare with each other, especially since the physical quantities and units often vary between authors. Some improvements are proposed to better define what should encompass the concepts of exchangeable and non-exchangeable fractions. Copyright © 2014 Elsevier Ltd. All rights reserved.

  1. THE NITROGEN ISOTOPIC COMPOSITION OF METEORITIC HCN

    Energy Technology Data Exchange (ETDEWEB)

    Pizzarello, Sandra, E-mail: pizzar@asu.edu [Department of Chemistry and Biochemistry, Arizona State University, Tempe, AZ 85018-1604 (United States)

    2014-12-01

    HCN is ubiquitous in extraterrestrial environments and is central to current theories on the origin of early solar system organic compounds such as amino acids. These compounds, observed in carbonaceous meteorites, were likely important in the origin and/or evolution of early life. As part of our attempts to understand the origin(s) of meteoritic CN{sup –}, we have analyzed the {sup 15}N/{sup 14}N isotopic composition of HCN gas released from water extracts of the Murchison meteorite and found its value to be near those of the terrestrial atmosphere. The findings, when evaluated viz-a-viz molecular abundances and isotopic data of meteoritic organic compounds, suggest that HCN formation could have occurred during the protracted water alteration processes known to have affected the mineralogy of many asteroidal bodies during their solar residence. This was an active synthetic stage, which likely involved simple gasses, organic molecules, their presolar precursors, as well as mineral catalysts and would have lead to the formation of molecules of differing isotopic composition, including some with solar values.

  2. Hydrogen isotope fractionation in methane plasma

    Science.gov (United States)

    Robert, François; Derenne, Sylvie; Lombardi, Guillaume; Hassouni, Khaled; Michau, Armelle; Reinhardt, Peter; Duhamel, Rémi; Gonzalez, Adriana; Biron, Kasia

    2017-01-01

    The hydrogen isotope ratio (D/H) is commonly used to reconstruct the chemical processes at the origin of water and organic compounds in the early solar system. On the one hand, the large enrichments in deuterium of the insoluble organic matter (IOM) isolated from the carbonaceous meteorites are interpreted as a heritage of the interstellar medium or resulting from ion-molecule reactions taking place in the diffuse part of the protosolar nebula. On the other hand, the molecular structure of this IOM suggests that organic radicals have played a central role in a gas-phase organosynthesis. So as to reproduce this type of chemistry between organic radicals, experiments based on a microwave plasma of CH4 have been performed. They yielded a black organic residue in which ion microprobe analyses revealed hydrogen isotopic anomalies at a submicrometric spatial resolution. They likely reflect differences in the D/H ratios between the various CHx radicals whose polymerization is at the origin of the IOM. These isotopic heterogeneities, usually referred to as hot and cold spots, are commensurable with those observed in meteorite IOM. As a consequence, the appearance of organic radicals in the ionized regions of the disk surrounding the Sun during its formation may have triggered the formation of organic compounds.

  3. AMS of the Minor Plutonium Isotopes

    Science.gov (United States)

    Steier, P.; Hrnecek, E.; Priller, A.; Quinto, F.; Srncik, M.; Wallner, A.; Wallner, G.; Winkler, S.

    2013-01-01

    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu = (5.7 ± 1.0) × 10-5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

  4. Multispectral dual isotope and NMR image analysis

    Energy Technology Data Exchange (ETDEWEB)

    Vannier, M.W.; Beihn, R.M.; Butterfield, R.L.; De Land, F.H.

    1985-05-01

    Dual isotope scintigraphy and nuclear magnetic resonance imaging produce image data that is intrinsically multispectral. That is multiple images of the same anatomic region are generated with different gray scale distribution and morphologic content that is largely redundant. Image processing technology, originally developed by NASA for satellite imaging, is available for multispectral analysis. These methods have been applied to provide tissue characterization. Tissue specific information encoded in the grapy scale data from dual isotope and NMR studies may be extracted using multispectral pattern recognition methods. The authors used table lookup minimum distance, maximum likelihood and cluster analysis techniques with data sets from Ga-67 / Tc-99m, 1-131 labeled antibodies / Tc-99m, Tc-99m perfusion / Xe-133 ventilation, and NMR studies. The results show; tissue characteristic signatures exist in dual isotope and NMR imaging, and these spectral signatures are identifiable using multispectral image analysis and provide tissue classification maps with scatter diagrams that facilitate interpretation and assist in elucidating subtle changes.

  5. Tracing Waste Water with Li isotopes

    Science.gov (United States)

    Millot, R.; Desaulty, A. M.

    2015-12-01

    The contribution of human activities such as industries, agriculture and various domestic inputs, becomes more and more significant in the chemical composition of the dissolved load of rivers. Human factors act as a supplementary key process. Therefore the mass-balance for the budget of catchments and river basins include anthropogenic disturbances. In the present study, we investigate waste water tracing by the use of Li isotopes in a small river basin near Orléans in France (l'Egoutier, 15 km² and 5 km long). It is well known that Li has strategic importance for numerous industrial applications including its use in the production of batteries for both mobile devices (computers, tablets, smartphones, etc.) and electric vehicles, but also in pharmaceutical formulations. In the present work, we collected river waters samples before and after the release from a waste water treatment plant connected to an hospital. Lithium isotopic compositions are rather homogeneous in river waters with δ7Li values around -0.5‰ ± 1 along the main course of the stream (n=7). The waste water sample is very different from the natural background of the river basin with Li concentration being twice of the values without pollution and significant heavy lithium contribution (δ7Li = +4‰). These preliminary results will be discussed in relation with factors controlling the distribution of Li and its isotopes in this specific system and compared with the release of other metals such as Pb or Zn.

  6. Predicting Macrosomia

    National Research Council Canada - National Science Library

    Pates, Jason A; McIntire, Donald D; Casey, Brian M; Leveno, Kenneth J

    2008-01-01

    Objective. The purpose of this study was to evaluate the prediction of fetal macrosomia based on ultrasound estimates of fetal weight and amniotic fluid volume combined with clinical risk factors. Methods...

  7. Strontium isotopes (87Sr/86Sr) in terrestrial ecological and palaeoecological research: empirical efforts and recent advances in continental-scale models.

    Science.gov (United States)

    Crowley, Brooke E; Miller, Joshua H; Bataille, Clément P

    2017-02-01

    Strontium (Sr) isotope analysis can provide detailed biogeographical and ecological information about modern and ancient organisms. Because Sr isotope ratios ( 87 Sr/ 86 Sr) in biologically relevant materials such as water, soil, vegetation, and animal tissues predominantly reflect local geology, they can be used to distinguish geologically distinct regions as well as identify highly mobile individuals or populations. While the application of Sr isotope analysis to biological research has been steadily increasing, high analytical costs have prohibited more widespread use. Additionally, accessibility of this geochemical tool has been hampered due to limited understanding of (i) the degree to which biologically relevant materials differ in their spatial averaging of 87 Sr/ 86 Sr ratios, and (ii) how these differences may be affected by lithologic complexity. A recently developed continental-scale model that accounts for variability in bedrock weathering rates and predicts Sr isotope ratios of surface water could help resolve these questions. In addition, if this 'local water' model can accurately predict 87 Sr/ 86 Sr ratios for other biologically relevant materials, there would be reduced need for researchers to assess regional Sr isotope patterns empirically. Here, we compile 87 Sr/ 86 Sr data for surface water, soil, vegetation, and mammalian and fish skeletal tissues from the literature and compare the accuracy with which the local water model predicts Sr isotope data among these five materials across the contiguous USA. We find that measured Sr isotope ratios for all five materials are generally close to those predicted by the local water model, although not with uniform accuracy. Mammal skeletal tissues are most accurately predicted, particularly in regions with low variability in 87 Sr/ 86 Sr predicted by the local water model. Increasing regional geologic heterogeneity increases both the offset and variance between modelled and empirical Sr isotope ratios, but

  8. Comparison of gas chromatography/isotope ratio mass spectrometry and liquid chromatography/isotope ratio mass spectrometry for carbon stable-isotope analysis of carbohydrates

    NARCIS (Netherlands)

    Moerdijk-Poortvliet, T.C.W.; Schierbeek, H.; Houtekamer, M.; van Engeland, T.; Derrien, D.; Stal, L.J.; Boschker, H.T.S.

    2015-01-01

    We compared gas chromatography/isotope ratio mass spectrometry (GC/IRMS) and liquid chromatography/isotope ratio mass spectrometry (LC/IRMS) for the measurement of d13C values in carbohydrates. Contrary to GC/IRMS, no derivatisation is needed for LC/IRMS analysis of carbohydrates. Hence, although

  9. Comparison of gas chromatography/isotope ratio mass spectrometry and liquid chromatography/isotope ratio mass spectrometry for carbon stable-isotope analysis of carbohydrates

    NARCIS (Netherlands)

    Moerdijk-Poortvliet, Tanja C. W.; Schierbeek, Henk; Houtekamer, Marco; van Engeland, Tom; Derrien, Delphine; Stal, Lucas J.; Boschker, Henricus T. S.

    2015-01-01

    We compared gas chromatography/isotope ratio mass spectrometry (GC/IRMS) and liquid chromatography/isotope ratio mass spectrometry (LC/IRMS) for the measurement of δ(13)C values in carbohydrates. Contrary to GC/IRMS, no derivatisation is needed for LC/IRMS analysis of carbohydrates. Hence, although

  10. Comparison of gas chromatography/isotope ratio mass spectrometry and liquid chromatography/isotope ratio mass spectrometry for carbon stable-isotope analysis of carbohydrates

    NARCIS (Netherlands)

    Moerdijk-Poortvliet, T.C.W.; Schierbeek, H.; Houtekamer, M.; van Engeland, T.; Derrien, D.; Stal, L.J.; Boschker, H.T.S.

    2015-01-01

    Rationale: We compared gas chromatography/isotope ratio mass spectrometry (GC/IRMS) and liquid chromatography/isotope ratio mass spectrometry (LC/IRMS) for the measurement of δ13C values in carbohydrates. Contrary to GC/IRMS, no derivatisation is needed for LC/IRMS analysis of carbohydrates. Hence,

  11. Constraints on post-depositional isotope modifications in East Antarctic firn from analysing temporal changes of isotope profiles

    Science.gov (United States)

    Münch, Thomas; Kipfstuhl, Sepp; Freitag, Johannes; Meyer, Hanno; Laepple, Thomas

    2017-09-01

    The isotopic composition of water in ice sheets is extensively used to infer past climate changes. In low-accumulation regions their interpretation is, however, challenged by poorly constrained effects that may influence the initial isotope signal during and after deposition of the snow. This is reflected in snow-pit isotope data from Kohnen Station, Antarctica, which exhibit a seasonal cycle but also strong interannual variations that contradict local temperature observations. These inconsistencies persist even after averaging many profiles and are thus not explained by local stratigraphic noise. Previous studies have suggested that post-depositional processes may significantly influence the isotopic composition of East Antarctic firn. Here, we investigate the importance of post-depositional processes within the open-porous firn (≳ 10 cm depth) at Kohnen Station by separating spatial from temporal variability. To this end, we analyse 22 isotope profiles obtained from two snow trenches and examine the temporal isotope modifications by comparing the new data with published trench data extracted 2 years earlier. The initial isotope profiles undergo changes over time due to downward advection, firn diffusion and densification in magnitudes consistent with independent estimates. Beyond that, we find further modifications of the original isotope record to be unlikely or small in magnitude (≪ 1 ‰ RMSD). These results show that the discrepancy between local temperatures and isotopes most likely originates from spatially coherent processes prior to or during deposition, such as precipitation intermittency or systematic isotope modifications acting on drifting or loose surface snow.

  12. Isotope-specific and amino acid-specific heavy atom substitutions alter barrier crossing in human purine nucleoside phosphorylase.

    Science.gov (United States)

    Suarez, Javier; Schramm, Vern L

    2015-09-08

    Computational chemistry predicts that atomic motions on the femtosecond timescale are coupled to transition-state formation (barrier-crossing) in human purine nucleoside phosphorylase (PNP). The prediction is experimentally supported by slowed catalytic site chemistry in isotopically labeled PNP (13C, 15N, and 2H). However, other explanations are possible, including altered volume or bond polarization from carbon-deuterium bonds or propagation of the femtosecond bond motions into slower (nanoseconds to milliseconds) motions of the larger protein architecture to alter catalytic site chemistry. We address these possibilities by analysis of chemistry rates in isotope-specific labeled PNPs. Catalytic site chemistry was slowed for both [2H]PNP and [13C, 15N]PNP in proportion to their altered protein masses. Secondary effects emanating from carbon-deuterium bond properties can therefore be eliminated. Heavy-enzyme mass effects were probed for local or global contributions to catalytic site chemistry by generating [15N, 2H]His8-PNP. Of the eight His per subunit, three participate in contacts to the bound reactants and five are remote from the catalytic sites. [15N, 2H]His8-PNP had reduced catalytic site chemistry larger than proportional to the enzymatic mass difference. Altered barrier crossing when only His are heavy supports local catalytic site femtosecond perturbations coupled to transition-state formation. Isotope-specific and amino acid specific labels extend the use of heavy enzyme methods to distinguish global from local isotope effects.

  13. Fishing for isotopes in the Brookhaven Lab Isotope Producer (BLIP) cooling water

    Energy Technology Data Exchange (ETDEWEB)

    Fitzsimmons, Jonathan [Brookhaven National Lab. (BNL), Upton, NY (United States). Collider Accelerator Dept.

    2016-04-29

    Be-7 has been used in environmental studies; the isotope is produced during BLIP irradiations and accumulates in the 320 gallons of cooling water. Be-7 has a 53.24 day half-life, so the optimal production/purification time is at the end of the BLIP run season. To purify Be-7 fifteen to twenty gallons of BLIP cooling water are removed and pumped through ion exchange columns that retain Be-7. This labor intensive approach captures ~15 mCi of Be-7, but the solution requires further purification. The method can lead to increased radiation exposure to staff. The ideal way to capture isotopes from large volumes is to reach in to the solution and selectively pull out the desired isotope. It is a lot like fishing.

  14. Isotope ratio analysis by Orbitrap mass spectrometry

    Science.gov (United States)

    Eiler, J. M.; Chimiak, L. M.; Dallas, B.; Griep-Raming, J.; Juchelka, D.; Makarov, A.; Schwieters, J. B.

    2016-12-01

    Several technologies are being developed to examine the intramolecular isotopic structures of molecules (i.e., site-specific and multiple substitution), but various limitations in sample size and type or (for IRMS) resolution have so far prevented the creation of a truly general technique. We will discuss the initial findings of a technique based on Fourier transform mass spectrometry, using the Thermo Scientific Q Exactive GC — an instrument that contains an Orbitrap mass analyzer. Fourier transform mass spectrometry is marked by exceptionally high mass resolutions (the Orbitrap reaches M/∆M in the range 250,000-1M in the mass range of greatest interest, 50-200 amu). This allows for resolution of a large range of nearly isobaric interferences for isotopologues of volatile and semi-volatile compounds (i.e., involving isotopes of H, C, N, O and S). It also provides potential to solve very challenging mass resolution problems for isotopic analysis of other, heavier elements. Both internal and external experimental reproducibilities of isotope ratio analyses using the Orbitrap typically conform to shot-noise limits down to levels of 0.2 ‰ (1SE), and routinely in the range 0.5-1.0 ‰, with similar accuracy when standardized to concurrently run reference materials. Such measurements can be made without modifications to the ion optics of the Q Exactive GC, but do require specially designed sample introduction devices to permit sample/standard comparison and long integration times. The sensitivity of the Q Exactive GC permits analysis of sub-nanomolar samples and quantification of multiply-substituted species. The site-specific capability of this instrument arises from the fact that mass spectra of molecular analytes commonly contain diverse fragment ion species, each of which samples a specific sub-set of molecular sites. We will present applications of this technique to the biological and abiological chemistry of amino acids, forensic identification of

  15. Stable water isotope patterns i