DOE Office of Scientific and Technical Information (OSTI.GOV)

Mace, Emily; Aalseth, Craig; Alexander, Tom

Use of ultra-low-background capabilities at Pacific Northwest National Laboratory provide enhanced sensitivity for measurement of low-activity sources of tritium and radiocarbon using proportional counters. Tritium levels are nearly back to pre-nuclear test backgrounds (~2-8 TU in rainwater), which can complicate their dual measurement with radiocarbon due to overlap in the isotope’s respective energy spectra. This activity makes direct dual-isotope measurements challenging without additional chemistry to concentrate the tritium in a sample. We present results of single-isotope proportional counter measurements used to analyze a dual-isotope methane sample synthesized from ~120 mg of H2O and present sensitivity results.

Isotopic composition (oxygen and hydrogen) of groundwater in Norway - a review of current knowledge and future perspectives

NASA Astrophysics Data System (ADS)

Kracht, O.

2012-04-01

A review of current knowledge and available data covering the stable isotope composition of groundwater in Norway is presented. Furthermore, the future challenge of obtaining systematic background datasets and of integrating isotopes into the mainstream of hydrogeological observation programmes is discussed. I will summarize our experiences gained from different preliminary studies and will try to identify relationships to existing datasets, historical registrations, and networks on precipitation data. The study of transient effects in hydrological cycles is highly topical as these are supposed to provide means for investigating the effects of climate change and increasing human activities. From a hydrogeological point of view, is critical to establish suitable tools for the large scale observation of changes in groundwater recharge and depletion, their likely controls, and the expected nature of responses to changing climate, urbanization and other human activities. In this context, stable isotopes (δ18O and δ2H of water) can provide an expedient instrument to investigate the general hydrological setting, connections, and pathways of various scale aquifer systems. However, we are up to now missing an expedient background dataset on hydrogeological and hydrological stable isotopes observations for mainland Norway. Against this background, during years 2010 and 2011 the Geological Survey of Norway (NGU) organized two nation-wide sampling campaigns on the stable isotope composition of modern groundwater. These pilot studies aimed to obtain a first overview about the data ranges and natural variations to be expected. We used stations from the existing Norwegian Groundwater Monitoring Network (Landsomfattende Grunnvannsnett, LGN) to collect samples of groundwater at 55 different locations throughout Norway. As a main characteristic of these two datasets, all δ18O and δ2H values of the "LGN series" were well correlated and plotted close to the global meteoric water line. This essentially documents the in principal exclusively meteoric origin of these waters, and indicates that the LGN groundwaters investigated shared the same type of origin: (i) evaporation from the ocean, and (ii) isotopic enrichment by rainout (continental effect). Conversely this also indicates that other processes (re-evaporation, admixture of water with a different genesis, etc.) did not have significant influence in this dataset. In parallel, two more detailed local application studies have been conducted in unconsolidated glaciofluvial aquifers in S-Norway (eastern part of the Gardermoen / Øvre Romerike Aquifer in Akershus county, and glaciofluvial deposits at the Granli waterworks of Kongsvinger in Hedmark county). In these investigations, detailed vertical profiles obtained with multi level sampling devices displayed systematic vertical evolution of groundwater isotopic composition, and it is demonstrated how an extended local dataset can enable to discuss the discrimination between different groundwater / surface water influences, and supports the planning of groundwater exploitations and groundwater water resources management.

Modeling of proton-induced radioactivation background in hard X-ray telescopes: Geant4-based simulation and its demonstration by Hitomi's measurement in a low Earth orbit

NASA Astrophysics Data System (ADS)

Odaka, Hirokazu; Asai, Makoto; Hagino, Kouichi; Koi, Tatsumi; Madejski, Greg; Mizuno, Tsunefumi; Ohno, Masanori; Saito, Shinya; Sato, Tamotsu; Wright, Dennis H.; Enoto, Teruaki; Fukazawa, Yasushi; Hayashi, Katsuhiro; Kataoka, Jun; Katsuta, Junichiro; Kawaharada, Madoka; Kobayashi, Shogo B.; Kokubun, Motohide; Laurent, Philippe; Lebrun, Francois; Limousin, Olivier; Maier, Daniel; Makishima, Kazuo; Mimura, Taketo; Miyake, Katsuma; Mori, Kunishiro; Murakami, Hiroaki; Nakamori, Takeshi; Nakano, Toshio; Nakazawa, Kazuhiro; Noda, Hirofumi; Ohta, Masayuki; Ozaki, Masanobu; Sato, Goro; Sato, Rie; Tajima, Hiroyasu; Takahashi, Hiromitsu; Takahashi, Tadayuki; Takeda, Shin'ichiro; Tanaka, Takaaki; Tanaka, Yasuyuki; Terada, Yukikatsu; Uchiyama, Hideki; Uchiyama, Yasunobu; Watanabe, Shin; Yamaoka, Kazutaka; Yasuda, Tetsuya; Yatsu, Yoichi; Yuasa, Takayuki; Zoglauer, Andreas

2018-05-01

Hard X-ray astronomical observatories in orbit suffer from a significant amount of background due to radioactivation induced by cosmic-ray protons and/or geomagnetically trapped protons. Within the framework of a full Monte Carlo simulation, we present modeling of in-orbit instrumental background which is dominated by radioactivation. To reduce the computation time required by straightforward simulations of delayed emissions from activated isotopes, we insert a semi-analytical calculation that converts production probabilities of radioactive isotopes by interaction of the primary protons into decay rates at measurement time of all secondary isotopes. Therefore, our simulation method is separated into three steps: (1) simulation of isotope production, (2) semi-analytical conversion to decay rates, and (3) simulation of decays of the isotopes at measurement time. This method is verified by a simple setup that has a CdTe semiconductor detector, and shows a 100-fold improvement in efficiency over the straightforward simulation. To demonstrate its experimental performance, the simulation framework was tested against data measured with a CdTe sensor in the Hard X-ray Imager onboard the Hitomi X-ray Astronomy Satellite, which was put into a low Earth orbit with an altitude of 570 km and an inclination of 31°, and thus experienced a large amount of irradiation from geomagnetically trapped protons during its passages through the South Atlantic Anomaly. The simulation is able to treat full histories of the proton irradiation and multiple measurement windows. The simulation results agree very well with the measured data, showing that the measured background is well described by the combination of proton-induced radioactivation of the CdTe detector itself and thick Bi4Ge3O12 scintillator shields, leakage of cosmic X-ray background and albedo gamma-ray radiation, and emissions from naturally contaminated isotopes in the detector system.

Modeling of proton-induced radioactivation background in hard X-ray telescopes: Geant4-based simulation and its demonstration by Hitomi ’s measurement in a low Earth orbit

DOE Office of Scientific and Technical Information (OSTI.GOV)

Odaka, Hirokazu; Asai, Makoto; Hagino, Kouichi

Hard X-ray astronomical observatories in orbit suffer from a significant amount of background due to radioactivation induced by cosmic-ray protons and/or geomagnetically trapped protons. Within the framework of a full Monte Carlo simulation, we present modeling of in-orbit instrumental background which is dominated by radioactivation. To reduce the computation time required by straightforward simulations of delayed emissions from activated isotopes, we insert a semi-analytical calculation that converts production probabilities of radioactive isotopes by interaction of the primary protons into decay rates at measurement time of all secondary isotopes. Therefore, our simulation method is separated into three steps: (1) simulation ofmore » isotope production, (2) semi-analytical conversion to decay rates, and (3) simulation of decays of the isotopes at measurement time. This method is verified by a simple setup that has a CdTe semiconductor detector, and shows a 100-fold improvement in efficiency over the straightforward simulation. To demonstrate its experimental performance, the simulation framework was tested against data measured with a CdTe sensor in the Hard X-ray Imager onboard the Hitomi X-ray Astronomy Satellite, which was put into a low Earth orbit with an altitude of 570 km and an inclination of 31°, and thus experienced a large amount of irradiation from geomagnetically trapped protons during its passages through the South Atlantic Anomaly. The simulation is able to treat full histories of the proton irradiation and multiple measurement windows. As a result, the simulation results agree very well with the measured data, showing that the measured background is well described by the combination of proton-induced radioactivation of the CdTe detector itself and thick Bi 4Ge 3O 12 scintillator shields, leakage of cosmic X-ray background and albedo gamma-ray radiation, and emissions from naturally contaminated isotopes in the detector system.« less

Modeling of proton-induced radioactivation background in hard X-ray telescopes: Geant4-based simulation and its demonstration by Hitomi ’s measurement in a low Earth orbit

DOE PAGES

Odaka, Hirokazu; Asai, Makoto; Hagino, Kouichi; ...

2018-02-19

Hard X-ray astronomical observatories in orbit suffer from a significant amount of background due to radioactivation induced by cosmic-ray protons and/or geomagnetically trapped protons. Within the framework of a full Monte Carlo simulation, we present modeling of in-orbit instrumental background which is dominated by radioactivation. To reduce the computation time required by straightforward simulations of delayed emissions from activated isotopes, we insert a semi-analytical calculation that converts production probabilities of radioactive isotopes by interaction of the primary protons into decay rates at measurement time of all secondary isotopes. Therefore, our simulation method is separated into three steps: (1) simulation ofmore » isotope production, (2) semi-analytical conversion to decay rates, and (3) simulation of decays of the isotopes at measurement time. This method is verified by a simple setup that has a CdTe semiconductor detector, and shows a 100-fold improvement in efficiency over the straightforward simulation. To demonstrate its experimental performance, the simulation framework was tested against data measured with a CdTe sensor in the Hard X-ray Imager onboard the Hitomi X-ray Astronomy Satellite, which was put into a low Earth orbit with an altitude of 570 km and an inclination of 31°, and thus experienced a large amount of irradiation from geomagnetically trapped protons during its passages through the South Atlantic Anomaly. The simulation is able to treat full histories of the proton irradiation and multiple measurement windows. As a result, the simulation results agree very well with the measured data, showing that the measured background is well described by the combination of proton-induced radioactivation of the CdTe detector itself and thick Bi 4Ge 3O 12 scintillator shields, leakage of cosmic X-ray background and albedo gamma-ray radiation, and emissions from naturally contaminated isotopes in the detector system.« less

Simultaneous measurement of tritium and radiocarbon by ultra-low-background proportional counting

DOE PAGES

Mace, Emily; Aalseth, Craig; Alexander, Tom; ...

2016-12-21

Use of ultra-low-background capabilities at Pacific Northwest National Laboratory provide enhanced sensitivity for measurement of low-activity sources of tritium and radiocarbon using proportional counters. Tritium levels are nearly back to pre-nuclear test backgrounds (~2-8 TU in rainwater), which can complicate their dual measurement with radiocarbon due to overlap in the beta decay spectra. In this paper, we present results of single-isotope proportional counter measurements used to analyze a dual-isotope methane sample synthesized from ~120 mg of H 2O and present sensitivity results.

Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hartig, Kyle C.; Ghebregziabher, Isaac; Jovanovic, Igor

The ability to perform not only elementally but also isotopically sensitive detection and analysis at standoff distances is important 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 emission exhibitsmore » 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. Lastly, 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.« less

Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry

PubMed Central

Hartig, Kyle C.; Ghebregziabher, Isaac; Jovanovic, Igor

2017-01-01

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. PMID:28272450

Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry

DOE PAGES

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 important 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 emission exhibitsmore » 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. Lastly, 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.« less

Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry

NASA Astrophysics Data System (ADS)

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.

Study of the cosmogenic activation in NaI(Tl) crystals within the ANAIS experiment

NASA Astrophysics Data System (ADS)

Villar, P.; Amaré, J.; Cebrián, S.; Coarasa, I.; García, E.; Martínez, M.; Oliván, M. A.; Ortigoza, Y.; Ortiz de Solórzano, A.; Puimedón, J.; Sarsa, M. L.; Villar, J. A.

2018-03-01

The direct detection of galactic dark matter particles requires ultra-low background conditions. NaI(Tl) crystals are applied in the search for these dark matter particles through their interactions in the detector by measuring the scintillation signal produced. The production of long-lived isotopes in materials due to the exposure to cosmic rays on Earth’s surface can be an hazard for these ultra-low background demanding experiments, typically performed underground. Therefore, production rates of cosmogenic isotopes in all the materials present in the experimental set-up, as well as the corresponding cosmic rays exposure history, must be both well-known in order to assess the relevance of this effect in the achievable sensitivity of a given experiment. Here, analysis of the cosmogenic studies developed from the ANAIS experiment NaI(Tl) detectors are presented. Installed inside a convenient shielding at the Canfranc Underground Laboratory just after finishing surface exposure to cosmic rays and thanks to the prompt data taking developed, identification and quantification of isotopes with half-lives of the order of tens of days were allowed, and thanks to the long-term operation of the detectors long-lived isotopes have been also identified and quantified. Main results for the activation yields of iodine and tellurium isotopes, 22Na, 113Sn, 109Cd, and tritium are presented in this work, together with the estimate of the production rates for their activation by cosmic nucleons while on Earth’s surface based on a selection of excitation functions over the entire energy range of cosmic nucleons.

Mercury Stable Isotopes Discriminate Different Populations of European Seabass and Trace Potential Hg Sources around Europe.

PubMed

Cransveld, Alice; Amouroux, David; Tessier, Emmanuel; Koutrakis, Emmanuil; Ozturk, Ayaka A; Bettoso, Nicola; Mieiro, Cláudia L; Bérail, Sylvain; Barre, Julien P G; Sturaro, Nicolas; Schnitzler, Joseph; Das, Krishna

2017-11-07

Our study reports the first data on mercury (Hg) isotope composition in marine European fish, for seven distinct populations of the European seabass, Dicentrarchus labrax. The use of δ 202 Hg and Δ 199 Hg values in SIBER enabled us to estimate Hg isotopic niches, successfully discriminating several populations. Recursive-partitioning analyses demonstrated the relevance of Hg stable isotopes as discriminating tools. Hg isotopic values also provided insight on Hg contamination sources for biota in coastal environment. The overall narrow range of δ 202 Hg around Europe was suggested to be related to a global atmospheric contamination while δ 202 Hg at some sites was linked either to background contamination, or with local contamination sources. Δ 199 Hg was related to Hg levels of fish but we also suggest a relation with ecological conditions. Throughout this study, results from the Black Sea population stood out, displaying a Hg cycling similar to fresh water lakes. Our findings bring out the possibility to use Hg isotopes in order to discriminate distinct populations, to explore the Hg cycle on a large scale (Europe) and to distinguish sites contaminated by global versus local Hg source. The interest of using Hg sable isotopes to investigate the whole European Hg cycle is clearly highlighted.

Simultaneous measurement of tritium and radiocarbon by ultra-low-background proportional counting.

PubMed

Mace, Emily; Aalseth, Craig; Alexander, Tom; Back, Henning; Day, Anthony; Hoppe, Eric; Keillor, Martin; Moran, Jim; Overman, Cory; Panisko, Mark; Seifert, Allen

2017-08-01

Use of ultra-low-background capabilities at Pacific Northwest National Laboratory provide enhanced sensitivity for measurement of low-activity sources of tritium and radiocarbon using proportional counters. Tritium levels are nearly back to pre-nuclear test backgrounds (~2-8 TU in rainwater), which can complicate their dual measurement with radiocarbon due to overlap in the beta decay spectra. We present results of single-isotope proportional counter measurements used to analyze a dual-isotope methane sample synthesized from ~120mg of H 2 O and present sensitivity results. Copyright © 2017 Elsevier Ltd. All rights reserved.

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

NASA Astrophysics Data System (ADS)

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.

Distribution of radioactive isotopes in rock and ore of Arkhangelskaya pipe from the Arkhangelsk diamond province

NASA Astrophysics Data System (ADS)

Kiselev, G. P.; Yakovlev, E. Yu.; Druzhinin, S. V.; Galkin, A. S.

2017-09-01

The contents of radioactive elements and the uranium isotopic composition of kimberlite in the Arkhangelskaya pipe at the M.V. Lomonosov deposit and of nearby country rocks have been studied. A surplus of 234U isotope has been established in rocks from the near-pipe space. The high γ = 234U/238U ratio is controlled by the geological structure of the near-pipe space. A nonequilibrium uranium halo reaches two pipe diameters in size and can be regarded as a local ore guide for kimberlite discovery. The rocks in the nearpipe space are also characterized by elevated or anomalous U, Th, and K contents with respect to the background.

Carbon-13 Isotopic Abundance and Concentration of Atmospheric Methane for Background Air in the Southern and Northern Hemispheres from 1978 to 1989 (NDP-049)

DOE Data Explorer

Stevens, C. M. [Chemical Technology Division, Argonne National Laboratory, Argonne, Illinois (USA)

2012-01-01

This data package presents atmospheric CH4 concentration and 13C isotopic abundance data derived from air samples collected over the period 1978-1989 at globally distributed clean-air sites. The data set comprises 201 records, 166 from the Northern Hemisphere and 35 from the Southern Hemisphere. The air samples were collected mostly in rural or marine locations remote from large sources of CH4 and are considered representative of tropospheric background conditions. The air samples were processed by isolation of CH4 from air and conversion to CO2 for isotopic analysis by isotope ratio mass spectrometry. These data represent one of the earliest records of 13C isotopic yy!measurements for atmospheric methane and have been used to refine estimates of CH4 emissions, calculate annual growth rates of emissions from changing sources, and provide evidence for changes in the rate of atmospheric removal of CH4. The data records consist of sample collection date; number of samples combined for analysis; sampling location; analysis date; CH4 concentration; 13C isotopic abundance; and flag codes to indicate outliers, repeated analyses, and other information.

The Doubly Labeled Water Method for Measuring Human Energy Expenditure: Adaptations for Spaceflight

NASA Technical Reports Server (NTRS)

Schulz, Leslie O.

1991-01-01

It is essential to determine human energy requirements in space, and the doubly labeled water method has been identified as the most appropriate means of indirect calorimetry to meet this need. The method employs naturally occurring, stable isotopes of hydrogen (H-2, deuterium) and oxygen (O-18) which, after dosing, mix with body water. The deuterium is lost from the body as water while the O-18 is eliminated as both water and CO2. The difference between the two isotope elimination rates is therefore a measure of CO2 production and hence energy expenditure. Spaceflight will present a unique challenge to the application of the doubly labeled water method. Specifically, interpretation of doubly labeled water results assumes that the natural abundance or 'background' levels of the isotopes remain constant during the measurement interval. To address this issue, an equilibration model will be developed in an ongoing ground-based study. As energy requirements of women matched to counterparts in the Astronauts Corps are being determined by doubly labeled water, the baseline isotope concentration will be changed by consumption of 'simulated Shuttle water' which is artificially enriched. One group of subjects will be equilibrated on simulated Shuttle water prior to energy determinations by doubly labeled water while the others will consume simulated Shuttle water after dosing. This process will allow us to derive a prediction equation to mathematically model the effect of changing background isotope concentrations.

Enrichment and geochemical mobility of heavy metals in bottom sediment of the Hoedong reservoir, Korea and their source apportionment.

PubMed

Lee, Pyeong-Koo; Kang, Min-Ju; Yu, Soonyoung; Ko, Kyung-Seok; Ha, Kyoochul; Shin, Seong-Cheon; Park, Jung Han

2017-10-01

Physicochemical characteristics of bottom sediment in the Hoedong reservoir were studied to evaluate the effectiveness of the reservoir as traps for trace metals. Roadside soil, stream sediment and background soil were also studied for comparison. Sequential extractions were carried out, and lead isotopic compositions of each extraction were determined to apportion Pb sources. Besides, particle size distribution of roadside soil, and metal concentrations and Pb isotopes of each size group were determined to characterize metal contamination. In result, Zn and Cu were enriched in sediment through roadside soil. The data on metal partitioning implied that Zn posed potential hazards for water quality. Meanwhile, the noticeable reduction of the 206 Pb/ 207 Pb isotopic ratio in the acid-soluble fraction in the size group 200 μm - 2 mm of national roadside soil indicated that this size group was highly contaminated by automotive emission with precipitation of acid-soluble secondary minerals during evaporation. Based on the Pb isotopic ratios, the dry deposition of Asian dust (AD) and non-Asian dust (NAD) affected roadside soil, while the effects of AD and NAD on bottom sediment appeared to be low given the low metal concentrations in sediment. Metal concentrations and Pb isotopic compositions indicated that sediments were a mixture of background and roadside soil. Source apportionment calculations showed that the average proportion of traffic Pb in bottom and stream sediments was respectively 34 and 31% in non-residual fractions, and 26 and 28% in residual fraction. The residual fraction of sediments appeared to be as contaminated as the non-residual fractions. Copyright © 2017 Elsevier Ltd. All rights reserved.

Measuring 226Ra/228Ra in Oceanic Lavas by MC-ICPMS

NASA Astrophysics Data System (ADS)

Standish, J. J.; Sims, K.; Ball, L.; Blusztajn, J.

2007-12-01

238U-230Th-226Ra disequilibrium in volcanic rocks provides an important and unique tool to evaluate timescales of recent magmatic processes. Determination of 230Th-226Ra disequilibria requires measurement of U and Th isotopes and concentrations as well as measurement of 226Ra. While measurement of U and Th by ICPMS is now well established, few published studies documenting 226Ra measurement via ICPMS exist. Using 228Ra as an isotope spike we have investigated two ion-counting methods; a 'peak-hopping' routine, where 226Ra and 228Ra are measured in sequence on the central discrete dynode ETP secondary electron multiplier (SEM), and simultaneous measurement of 226Ra and 228Ra on two multiple ion-counter system (MICS) channeltron type detectors mounted on the low end of the collector block. Here we present 226Ra measurement by isotope dilution using the Thermo Fisher NEPTUNE MC-ICPMS. Analysis of external rock standards TML and AThO along with mid-ocean ridge basalt (MORB) and ocean island basalt (OIB) samples show three issues that need to be considered when making precise and accurate Ra measurements: 1) mass bias, 2) background, and 3) relative efficiencies of the detectors when measuring in MICS mode. Due to the absence of an established 226Ra/228Ra standard, we have used U reference material NBL-112A to monitor mass bias. Although Ball et. al., (in press) have shown that U does not serve as an adequate proxy for Th (and thus not likely for Ra either), measurements of rock standards TML and AThO are repeatedly in equilibrium within the uncertainty of the measurements (where total uncertainty includes propagation of the uncertainty in the 226Ra standard used for calibrating the 228Ra spike). For this application, U is an adequate proxy for Ra mass bias at the 1% uncertainly level. The more important issue is the background correction. Because of the extensive chemistry required to separate and purify Ra (typically fg/g level in volcanic rocks), we observe large ambient backgrounds using both ion-counting techniques, which can significantly influence the measured 226Ra/228Ra ratio. Ra off-peak backgrounds need to be measured explicitly and quantitatively corrected. One advantage of using a 'peak-hopping' routine on the central SEM is the optional use of the high abundance sensitivity lens or repelling potential quadrapole (RPQ). This lens virtually eliminates the ambient background and significantly enhances the signal to noise ratio with only a small decrease in Ra ion transmission. Even with the diminished background levels observed using 'peak-hopping' on the SEM with the RPQ, accurate measurement of Ra isotopes requires off-peak background measurement. Finally, when using MICS it is important to account for the relative efficiency of the detectors. Multiple ion counting is, in principle, preferable to 'peak-hopping' because more time is spent counting each individual isotope. However, our results illustrate that proper calibration of detector yields requires dynamic switching of 226Ra between the two ion counters. This negates the inherent advantage of multiple ion counting. Therefore, when considering mass bias, background correction, and detector gain calibration, we conclude that 'peak-hopping' on the central SEM with the RPQ abundance filter is the preferred technique for 226Ra/228Ra isotopic measurement on the Neptune MC-ICPMS.

Constraining the cause of the end-Guadalupian extinction with coupled records of carbon and calcium isotopes

NASA Astrophysics Data System (ADS)

Jost, A. B.; Mundil, R.; He, B.; Brown, S. T.; Altiner, D.; Sun, Y.; DePaolo, D. J.; Payne, J.

2013-12-01

A negative δ13C excursion in carbonate sediments from Guadalupian (Middle Permian) and Lopingian (Late Permian) stratigraphic sections has been interpreted to result from a large carbon cycle disturbance during end-Guadalupian extinction event (ca. 260 Ma). However, the carbon isotope data alone are insufficient to uniquely determine the type and magnitude of perturbations to the global carbon cycle. The carbon and calcium cycles are coupled via CaCO3 burial, so changes in calcium isotopes can be used to constrain the cause of a carbon isotope excursion. In this study, we present coupled carbon and calcium isotope records from three Guadalupian-Lopingian (G/L) sections in China and Turkey. Isotope records among our studied sections are inconsistent in both their δ13C and δ44/40Ca records. Similar inconsistencies in δ13C among sections occur across previously published datasets. Sections with large (>3‰) changes in δ13C either show evidence for diagenetic alteration or do not show δ13C and δ44/40Ca changes consistent with severe volcanic degassing from Emeishan or methane clathrate destabilization. We conclude that the large isotopic changes are more likely the result of local burial conditions or diagenetic effects, rather than a large carbon cycle disturbance. Perturbations to the global carbon and calcium cycles appear to have been much smaller across the G/L transition than across the subsequent Permian-Triassic boundary. This finding is consistent with recent paleobiological data showing that the end-Guadalupian extinction was much less severe than previously believed, and was indistinguishable in magnitude from background intervals. However, selective extinction of marine animals with passive respiratory physiology indicates that the G/L extinction cannot simply be due to background extinction or sampling failure, and that it was triggered by some environmental event. Therefore, any environmental event must have been small enough to not generate large changes in δ13C and δ44/40Ca. A small acidification or warming event is therefore plausible, but difficult to confirm. Loss of marine habitat by way of sea-level change also remains a possible extinction trigger.

MixSIAR: advanced stable isotope mixing models in R

EPA Science Inventory

Background/Question/Methods The development of stable isotope mixing models has coincided with modeling products (e.g. IsoSource, MixSIR, SIAR), where methodological advances are published in parity with software packages. However, while mixing model theory has recently been ex...

Fully convolutional neural network for removing background in noisy images of uranium bearing particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tarolli, Jay G.; Naes, Benjamin E.; Butler, Lamar

A fully convolutional neural network (FCN) was developed to supersede automatic or manual thresholding algorithms used for tabulating SIMS particle search data. The FCN was designed to perform a binary classification of pixels in each image belonging to a particle or not, thereby effectively removing background signal without manually or automatically determining an intensity threshold. Using 8,000 images from 28 different particle screening analyses, the FCN was trained to accurately predict pixels belonging to a particle with near 99% accuracy. Background eliminated images were then segmented using a watershed technique in order to determine isotopic ratios of particles. A comparisonmore » of the isotopic distributions of an independent data set segmented using the neural network, compared to a commercially available automated particle measurement (APM) program developed by CAMECA, highlighted the necessity for effective background removal to ensure that resulting particle identification is not only accurate, but preserves valuable signal that could be lost due to improper segmentation. The FCN approach improves the robustness of current state-of-the-art particle searching algorithms by reducing user input biases, resulting in an improved absolute signal per particle and decreased uncertainty of the determined isotope ratios.« less

Abatement of Xenon and Iodine Emissions from Medical Isotope Production Facilities

DOE Office of Scientific and Technical Information (OSTI.GOV)

Doll, Charles G.; Sorensen, Christina M.; Bowyer, Ted W.

2014-04-01

The capability of the International Monitoring System (IMS) to detect xenon from underground nuclear explosions is dependent on the radioactive xenon background. Adding to the background, medical isotope production (MIP) by fission releases several important xenon isotopes including xenon-133 and iodine-133 that decays to xenon-133. The amount of xenon released from these facilities may be equivalent to or exceed that released from an underground nuclear explosion. Thus the release of gaseous fission products within days of irradiation makes it difficult to distinguish MIP emissions from a nuclear explosion. In addition, recent shortages in molybdenum-99 have created interest and investment opportunitiesmore » to design and build new MIP facilities in the United States and throughout the world. Due to the potential increase in the number of MIP facilities, a discussion of abatement technologies provides insight into how the problem of emission control from MIP facilities can be tackled. A review of practices is provided to delineate methods useful for abatement of medical isotopes.« less

Potential impact of releases from a new Molybdenum-99 production facility on regional measurements of airborne xenon isotopes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bowyer, Ted W.; Eslinger, Paul W.; Cameron, Ian M.

2014-03-01

The monitoring of the radioactive xenon isotopes 131mXe, 133Xe, 133mXe, and 135Xe is important for the detection of nuclear explosions. While backgrounds of the xenon isotopes are short-lived, they are constantly replenished from activities dominated by the fission-based production of 99Mo used for medical procedures. One of the most critical locations on earth for the monitoring of nuclear explosions is the Korean peninsula, where the Democratic Republic of North Korea (DPRK) has announced that it had conducted three nuclear tests between 2009 and 2013. This paper explores the backgrounds that would be caused by the medium to large scale productionmore » of 99Mo in the region of the Korean peninsula.« less

Determination of the sulfur isotope ratio in carbonyl sulfide using gas chromatography/isotope ratio mass spectrometry on fragment ions 32S+, 33S+, and 34S+.

PubMed

Hattori, Shohei; Toyoda, Akari; Toyoda, Sakae; Ishino, Sakiko; Ueno, Yuichiro; Yoshida, Naohiro

2015-01-06

Little is known about the sulfur isotopic composition of carbonyl sulfide (OCS), the most abundant atmospheric sulfur species. We present a promising new analytical method for measuring the stable sulfur isotopic compositions (δ(33)S, δ(34)S, and Δ(33)S) of OCS using nanomole level samples. The direct isotopic analytical technique consists of two parts: a concentration line and online gas chromatography-isotope ratio mass spectrometry (GC-IRMS) using fragmentation ions (32)S(+), (33)S(+), and (34)S(+). The current levels of measurement precision for OCS samples greater than 8 nmol are 0.42‰, 0.62‰, and 0.23‰ for δ(33)S, δ(34)S, and Δ(33)S, respectively. These δ and Δ values show a slight dependence on the amount of injected OCS for volumes smaller than 8 nmol. The isotope values obtained from the GC-IRMS method were calibrated against those measured by a conventional SF6 method. We report the first measurement of the sulfur isotopic composition of OCS in air collected at Kawasaki, Kanagawa, Japan. The δ(34)S value obtained for OCS (4.9 ± 0.3‰) was lower than the previous estimate of 11‰. When the δ(34)S value for OCS from the atmospheric sample is postulated as the global signal, this finding, coupled with isotopic fractionation for OCS sink reactions in the stratosphere, explains the reported δ(34)S for background stratospheric sulfate. This suggests that OCS is a potentially important source for background (nonepisodic or nonvolcanic) stratospheric sulfate aerosols.

Using Isotopes to Reconstruct Mammalian Diet, Migration and Paleoenvironment for Hominin Sites in Indonesia

NASA Astrophysics Data System (ADS)

Wershow, H.; Janssen, R.; Vonhof, H.; Lubbe, J. V. D.; Joordens, J. J.; Koutamanis, D. S.; Puspaningrum, M. R.; de Vos, J.; Reijmer, J.

2015-12-01

Climate plays a prominent role in ecosystem development in the biodiversity hotspot Sundaland (Malaysia and western Indonesia) throughout the Quaternary. Recurrent isolation and connection of the islands to mainland Asia due to sea level fluctuations has enabled repeated biotic migrations and encouraged genetic speciation. These migration waves also brought Homo erectus to Java. Together with extensive and well-documented collections of other terrestrial species, these hominin fossils form faunal assemblages of which the paleoenvironmental and paleogeographical background is poorly known. Using carbon, oxygen and strontium isotopes, we have reconstructed the paleoenvironmental and paleoecological conditions of several Holocene and Pleistocene fossil sites on Sumatra and Java, Indonesia. Carbon (∂13C) and oxygen (∂18O) isotope analysis of well-preserved herbivore teeth enamel reveals a marked contrast between C3-dominated diets in warmer periods, and C4-dominated diets in cooler periods, reflecting the distinct changes in Sundaland vegetation cover between glacials and interglacials. These isotope patterns allow us to assign the appropriate climatic background to some of the older fossil assemblages from Java, for which dating uncertainty does not allow direct assignment to glacial or interglacial conditions. The stable isotope signatures of herbivores from Trinil and Sangiran, sites well-known for the fossil occurrence of Homo erectus, indicate glacial conditions. The isotope data of several H. erectus fossils from these sites seem to be in line with such an interpretation. Furthermore, we applied strontium (87Sr/86Sr) isotope analyses to a sample subset. The preliminary data show distinct Sr-isotope ratios for different sites, providing clues for the applicability of this isotope technique in detecting climate-related mobility of Sundaland fossil faunas.

ISOTOPIC EVALUATION OF PB OCCURRENCES IN THE RIVERINE ECOSYSTEMS OF THE KANKAKEE WATERSHED, ILLINOIS-INDIANA.

EPA Science Inventory

Environmental background levels of Pb were measured in ponds, river waters, sediments, suspended sediments, rocks, and air particulates within the Kankakee watershed during the period of 1995 to 1999. Stable isotopic Pb distinguised airborne Pb and its incorporation into riverin...

ICC-CLASS: isotopically-coded cleavable crosslinking analysis software suite

PubMed Central

2010-01-01

Background Successful application of crosslinking combined with mass spectrometry for studying proteins and protein complexes requires specifically-designed crosslinking reagents, experimental techniques, and data analysis software. Using isotopically-coded ("heavy and light") versions of the crosslinker and cleavable crosslinking reagents is analytically advantageous for mass spectrometric applications and provides a "handle" that can be used to distinguish crosslinked peptides of different types, and to increase the confidence of the identification of the crosslinks. Results Here, we describe a program suite designed for the analysis of mass spectrometric data obtained with isotopically-coded cleavable crosslinkers. The suite contains three programs called: DX, DXDX, and DXMSMS. DX searches the mass spectra for the presence of ion signal doublets resulting from the light and heavy isotopic forms of the isotopically-coded crosslinking reagent used. DXDX searches for possible mass matches between cleaved and uncleaved isotopically-coded crosslinks based on the established chemistry of the cleavage reaction for a given crosslinking reagent. DXMSMS assigns the crosslinks to the known protein sequences, based on the isotopically-coded and un-coded MS/MS fragmentation data of uncleaved and cleaved peptide crosslinks. Conclusion The combination of these three programs, which are tailored to the analytical features of the specific isotopically-coded cleavable crosslinking reagents used, represents a powerful software tool for automated high-accuracy peptide crosslink identification. See: http://www.creativemolecules.com/CM_Software.htm PMID:20109223

Preparation and characterisation of isotopically enriched Ta2O5 targets for nuclear astrophysics studies

NASA Astrophysics Data System (ADS)

Caciolli, A.; Scott, D. A.; Di Leva, A.; Formicola, A.; Aliotta, M.; Anders, M.; Bellini, A.; Bemmerer, D.; Broggini, C.; Campeggio, M.; Corvisiero, P.; Depalo, R.; Elekes, Z.; Fülöp, Zs.; Gervino, G.; Guglielmetti, A.; Gustavino, C.; Gyürky, Gy.; Imbriani, G.; Junker, M.; Marta, M.; Menegazzo, R.; Napolitani, E.; Prati, P.; Rigato, V.; Roca, V.; Rolfs, C.; Rossi Alvarez, C.; Somorjai, E.; Salvo, C.; Straniero, O.; Strieder, F.; Szücs, T.; Terrasi, F.; Trautvetter, H. P.; Trezzi, D.

2012-10-01

The direct measurement of reaction cross-sections at astrophysical energies often requires the use of solid targets of known thickness, isotopic composition, and stoichiometry that are able to withstand high beam currents for extended periods of time. Here, we report on the production and characterisation of isotopically enriched Ta2O5 targets for the study of proton-induced reactions at the Laboratory for Underground Nuclear Astrophysics facility of the Laboratori Nazionali del Gran Sasso. The targets were prepared by anodisation of tantalum backings in enriched water (up to 66% in 17O and up to 96% in 18O. Special care was devoted to minimising the presence of any contaminants that could induce unwanted background reactions with the beam in the energy region of astrophysical interest. Results from target characterisation measurements are reported, and the conclusions for proton capture measurements with these targets are drawn.

Maximum reasonable radioxenon releases from medical isotope production facilities and their effect on monitoring nuclear explosions.

PubMed

Bowyer, Theodore W; Kephart, Rosara; Eslinger, Paul W; Friese, Judah I; Miley, Harry S; Saey, Paul R J

2013-01-01

Fission gases such as (133)Xe are used extensively for monitoring the world for signs of nuclear testing in systems such as the International Monitoring System (IMS). These gases are also produced by nuclear reactors and by fission production of (99)Mo for medical use. Recently, medical isotope production facilities have been identified as the major contributor to the background of radioactive xenon isotopes (radioxenon) in the atmosphere (Stocki et al., 2005; Saey, 2009). These releases pose a potential future problem for monitoring nuclear explosions if not addressed. As a starting point, a maximum acceptable daily xenon emission rate was calculated, that is both scientifically defendable as not adversely affecting the IMS, but also consistent with what is possible to achieve in an operational environment. This study concludes that an emission of 5 × 10(9) Bq/day from a medical isotope production facility would be both an acceptable upper limit from the perspective of minimal impact to monitoring stations, but also appears to be an achievable limit for large isotope producers. Copyright © 2012 Elsevier Ltd. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Douglas, Matthew; Bernacki, Bruce E.; Erchinger, Jennifer L.

Liquid scintillation counting (LSC) is a versatile and commonplace method for radiometric measurement of charged particle emitting radionuclides. The LSC method provides utility in a range of environmental science applications including hydrological studies of water transport, anthropogenic releases of radionuclides into the environment, and vertical mixing rates within oceans. Instrumental measurement background is one limiting factor of radiometric measurement sensitivity. As part of the development of a custom low background LSC system located in a shallow underground laboratory at Pacific Northwest National Laboratory, a number of measurement applications of LSC have been considered and are summarized here. The focus ismore » on determining which aspects of such measurements would gain the greatest benefit from the reduction of LSC backgrounds by a factor of 10-100 relative to values reported in the literature. Examples of benefits include lowering the minimum detectable activity, reducing the sample size required, and shortening the elapsed timeline of the processing and analysis sequence. In particular tritium, strontium, and actinium isotopes are examined as these isotopes cover a range of requirements related to the LSC measurement method (e.g., 3H: low energy; Sr: spectral deconvolution; Ac: alpha/beta discrimination).« less

Spallation backgrounds in Super-Kamiokande are made in muon-induced showers

NASA Astrophysics Data System (ADS)

Li, Shirley Weishi; Beacom, John F.

2015-05-01

Crucial questions about solar and supernova neutrinos remain unanswered. Super-Kamiokande has the exposure needed for progress, but detector backgrounds are a limiting factor. A leading component is the beta decays of isotopes produced by cosmic-ray muons and their secondaries, which initiate nuclear spallation reactions. Cuts of events after and surrounding muon tracks reduce this spallation decay background by ≃ 90 % (at a cost of ≃ 20 % deadtime), but its rate at 6-18 MeV is still dominant. A better way to cut this background was suggested in a Super-Kamiokande paper by Bays et al. [Phys. Rev. D 85, 052007 (2012)] on a search for the diffuse supernova neutrino background. They found that spallation decays above 16 MeV were preceded near the same location by a peak in the apparent Cherenkov light profile from the muon; a more aggressive cut was applied to a limited section of the muon track, leading to decreased background without increased deadtime. We put their empirical discovery on a firm theoretical foundation. We show that almost all spallation decay isotopes are produced by muon-induced showers and that these showers are rare enough and energetic enough to be identifiable. This is the first such demonstration for any detector. We detail how the physics of showers explains the peak in the muon Cherenkov light profile and other Super-K observations. Our results provide a physical basis for practical improvements in background rejection that will benefit multiple studies. For solar neutrinos, in particular, it should be possible to dramatically reduce backgrounds at energies as low as 6 MeV.

MixSIAR: A Bayesian stable isotope mixing model for characterizing intrapopulation niche variation

EPA Science Inventory

Background/Question/Methods The science of stable isotope mixing models has tended towards the development of modeling products (e.g. IsoSource, MixSIR, SIAR), where methodological advances or syntheses of the current state of the art are published in parity with software packa...

Operating manual for the High Flux Isotope Reactor. Volume I. Description of the facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1982-09-01

This volume contains a comprehensive description of the High Flux Isotope Reactor Facility. Its primary purpose is to supplement the detailed operating procedures, providing the reactor operators with background information on the various HFIR systems. The detailed operating procdures are presented in another report.

Boeing Michigan Aeronautical Research Center (BOMARC) Missile Shelters and Bunkers Scoping Survey Workplan

DTIC Science & Technology

2007-08-01

Characterization (OHM 1998). From the plot, it is clear that the HEU dominates DU in the overall isotopic characteristic. Among the three uranium ... isotopes , 234U comprised about 90 % of the total activity, including naturally-occurring background sources. However, in comparison to the WGP, uranium ...listed for a few sampling locations that had isotopic plutonium analysis of wipe samples. Figure A-19 contains a scatterplot of the paired Table 4-13

Combined use of 15N and 18O of nitrate and 11B to evaluate nitrate contamination in groundwater

USGS Publications Warehouse

Seiler, R.L.

2005-01-01

Isotopic composition of NO3 (??15NNO3 and ??18ONO3) and B (??11B) were used to evaluate NO3 contamination and identify geochemical processes occurring in a hydrologically complex Basin and Range valley in northern Nevada with multiple potential sources of NO3. Combined use of these isotopes may be a useful tool in identifying NO3 sources because NO3 and B co-migrate in many environmental settings, their isotopes are fractionated by different environmental processes, and because wastewater and fertilizers may have distinct isotopic signatures for N and B. The principal cause of elevated NO3 concentrations in residential parts of the study area is wastewater and not natural NO3 or fertilizers. This is indicated by some samples with elevated NO3 concentrations plotting along ??15NNO3 and NO3 mixing lines between natural NO3 from the study area and theoretical septic-system effluent. This conclusion is supported by the presence of caffeine in one sample and the absence of samples with elevated NO3 concentrations that fall along mixing lines between natural NO3 and theoretical percolate below fertilized lawns. Nitrogen isotopes alone could not be used to determine NO3 sources in several wells because denitrification blurred the original isotopic signatures. The range of ??11B values in native ground water in the study area (-8.2??? to +21.2???) is large. The samples with the low ??11B values have a geochemical signature characteristic of hydrothermal systems. Physical and chemical data suggest B is not being strongly fractionated by adsorption onto clays. ??11B values from local STP effluent (-2.7???) and wash water from a domestic washing machine (-5.7???) were used to plot mixing lines between wastewater and native ground water. In general, wells with elevated NO3 concentrations fell along mixing lines between wastewater and background water on plots of ??11B against 1/B and Cl/B. Combined use of ??15N and ??11B in the study area was generally successful in identifying contaminant sources and processes that are occurring, however, it is likely to be more successful in simpler settings with a well-characterized ??11B value for background wells.

Evaluation of perchlorate sources in the Rialto-Colton and Chino California subbasins using chlorine and oxygen isotope ratio analysis

USGS Publications Warehouse

Hatzinger, Paul B.; Böhlke, John Karl; Izbicki, John; Teague, Nicholas F.; Sturchio, Neil C.

2015-01-01

Perchlorate (ClO4-) in groundwater can be from synthetic or natural sources, the latter of which include both historical application of imported nitrate fertilizers from the Atacama Desert of Chile and naturally deposited ClO4- that forms atmospherically and accumulates in arid regions such as the southwestern US. The objective of this study was to evaluate the use of isotopic data to distinguish sources of ClO4- in groundwater in a specific region of the Rialto-Colton and Chino, CA groundwater subbasins (Study Area). This region includes two groundwater ClO4- plumes emanating from known military/industrial source areas, and a larger area outside of these plumes having measurable ClO4-. Perchlorate extracted from wells in this region was analyzed for chlorine and oxygen stable isotope ratios (δ37Cl, δ18O, δ17O) and radioactive chlorine-36 (36Cl) isotopic abundance, along with other geochemical, isotopic, and hydrogeologic data. Isotope data indicate synthetic, Atacama, and indigenous natural ClO4- were present in the Study Area. Stable isotope data from nearly all sampled wells within the contours of the two characterized plumes, including those located in a perched zone and within the regional groundwater aquifer, were consistent with a dominant synthetic ClO4- source. In wells downgradient from the synthetic plumes and in the Chino subbasin to the southwest, isotopic data indicate the dominant source of ClO4- largely was Atacama, presumably from historical application of nitrate fertilizer in this region. Past agricultural land use and historical records are consistent with this source being present in groundwater. The 36Cl and δ18O data indicate that wells having predominantly synthetic or Atacama ClO4- also commonly contained small fractions of indigenous natural ClO4-. The indigenous ClO4- was most evident isotopically in wells having the lowest overall ClO4- concentrations (< 1 μg/L), consistent with its occurrence as a low-level background constituent in the region. A small subset of wells outside the contours of the two synthetic plumes, including an upgradient well, had characteristics indicating small amounts of synthetic ClO4- mixed with one or both of the natural source types. Hydrogeologic data indicate synthetic ClO4- in the upgradient well may be from a source other than the identified plume sources, but it is not known whether this source might also be present in other wells at low concentrations. The stable isotope and 36Cl data provided relatively unambiguous discrimination of synthetic and Atacama ClO4- sources in most wells having relatively high concentrations, providing regional perspective on anthropogenic ClO4- contamination in the Rialto-Colton and Chino subbasins. Where indigenous natural ClO4- was indicated as a substantial component, total ClO4- concentrations were low and concentrations of anthropogenic components were near background levels.

Isotope effects in the evaporation of water: a status report of the Craig-Gordon model.

PubMed

Horita, Juske; Rozanski, Kazimierz; Cohen, Shabtai

2008-03-01

The Craig-Gordon model (C-G 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 Paleotemperatures, E. Tongiorgi (Ed.), pp. 9-130, Laboratorio di Geologia Nucleare, Pisa (1965).] has been synonymous with the isotope effects associated with the evaporation of water from surface waters, soils, and vegetations, which in turn constitutes a critical component of the global water cycle. On the occasion of the four decades of its successful applications to isotope geochemistry and hydrology, an attempt is made to: (a) examine its physical background within the framework of modern evaporation models, (b) evaluate our current knowledge of the environmental parameters of the C-G model, and (c) comment on a general strategy for the use of these parameters in field applications. Despite its simplistic representation of evaporation processes at the water-air interface, the C-G model appears to be adequate to provide the isotopic composition of the evaporation flux. This is largely due to its nature for representing isotopic compositions (a ratio of two fluxes of different isotopic water molecules) under the same environmental conditions. Among many environmental parameters that are included in the C-G model, accurate description and calculations are still problematic of the kinetic isotope effects that occur in a diffusion-dominated thin layer of air next to the water-air interface. In field applications, it is of importance to accurately evaluate several environmental parameters, particularly the relative humidity and isotopic compositions of the 'free-atmosphere', for a system under investigation over a given time-scale of interest (e.g., hourly to daily to seasonally). With a growing interest in the studies of water cycles of different spatial and temporal scales, including paleoclimate and water resource studies, the importance and utility of the C-G model is also likely to grow in the future.

Multi-Isotope Secondary Ion Mass Spectrometry Combining Heavy Water 2H with 15N Labeling As Complementary Tracers for Metabolic Heterogeneity at the Single-Cell Level

NASA Astrophysics Data System (ADS)

Kopf, S.; McGlynn, S.; Cowley, E.; Green, A.; Newman, D. K.; Orphan, V. J.

2014-12-01

Metabolic rates of microbial communities constitute a key physiological parameter for understanding the in situ growth constraints for life in any environment. Isotope labeling techniques provide a powerful approach for measuring such biological activity, due to the use of isotopically enriched substrate tracers whose incorporation into biological materials can be detected with high sensitivity by isotope-ratio mass spectrometry. Nano-meter scale secondary ion mass spectrometry (NanoSIMS) combined with stable isotope labeling provides a unique tool for studying the spatiometabolic activity of microbial populations at the single cell level in order to assess both community structure and population diversity. However, assessing the distribution and range of microbial activity in complex environmental systems with slow-growing organisms, diverse carbon and nitrogen sources, or heterotrophic subpopulations poses a tremendous technical challenge because the introduction of isotopically labeled substrates frequently changes the nutrient availability and can inflate or bias measures of activity. Here, we present the use of hydrogen isotope labeling with deuterated water as an important new addition to the isotopic toolkit and apply it for the determination of single cell microbial activities by NanoSIMS imaging. This tool provides a labeling technique that minimally alters any aquatic chemical environment, can be administered with strong labels even in minimal addition (natural background is very low), is an equally universal substrate for all forms of life even in complex, carbon and nitrogen saturated systems, and can be combined with other isotopic tracers. The combination of heavy water labeling with the most commonly used NanoSIMS tracer, 15N, is technically challenging but opens up a powerful new set of multi-tracer experiments for the study of microbial activity in complex communities. We present the first truly simultaneous single cell triple isotope system measurements of 2H/1H, 13C/12C and 15N/14N and apply it to study of microbial metabolic heterogeneity and nitrogen metabolism in a continuous culture case study. Our data provide insight into both the diversity of microbial activity rates, as well as patterns of ammonium utilization at the single cell level.

Determination of the origin of groundwater nitrate at an air weapons range using the dual isotope approach.

PubMed

Bordeleau, Geneviève; Savard, Martine M; Martel, Richard; Ampleman, Guy; Thiboutot, Sonia

2008-06-06

Nitrate is one of the most common contaminants in shallow groundwater, and many sources may contribute to the nitrate load within an aquifer. Groundwater nitrate plumes have been detected at several ammunition production sites. However, the presence of multiple potential sources and the lack of existing isotopic data concerning explosive degradation-induced nitrate constitute a limitation when it comes to linking both types of contaminants. On military training ranges, high nitrate concentrations in groundwater were reported for the first time as part of the hydrogeological characterization of the Cold Lake Air Weapons Range (CLAWR), Alberta, Canada. Explosives degradation is thought to be the main source of nitrate contamination at CLAWR, as no other major source is present. Isotopic analyses of N and O in nitrate were performed on groundwater samples from the unconfined and confined aquifers; the dual isotopic analysis approach was used in order to increase the chances of identifying the source of nitrate. The isotopic ratios for the groundwater samples with low nitrate concentration suggested a natural origin with a strong contribution of anthropogenic atmospheric NOx. For the samples with nitrate concentration above the expected background level the isotopic ratios did not correspond to any source documented in the literature. Dissolved RDX samples were degraded in the laboratory and results showed that all reproduced degradation processes released nitrate with a strong fractionation. Laboratory isotopic values for RDX-derived NO(3)(-) produced a trend of high delta(18)O-low delta(15)N to low delta(18)O-high delta(15)N, and groundwater samples with nitrate concentrations above the expected background level appeared along this trend. Our results thus point toward a characteristic field of isotopic ratios for nitrate being derived from the degradation of RDX.

Synthesis of isotopically modified ZnO nanoparticles and their potential as nanotoxicity tracers

USGS Publications Warehouse

Dybowska, A.D.; Croteau, M.-N.; Misra, S.K.; Berhanu, D.; Luoma, S.N.; Christian, P.; O'Brien, P.; Valsami-Jones, E.

2011-01-01

Understanding the behavior of engineered nanoparticles in the environment and within organisms is perhaps the biggest obstacle to the safe development of nanotechnologies. Reliable tracing is a particular issue for nanoparticles such as ZnO, because Zn is an essential element and a common pollutant thus present at elevated background concentrations. We synthesized isotopically enriched (89.6%) with a rare isotope of Zn (67Zn) ZnO nanoparticles and measured the uptake of 67Zn by L. stagnalis exposed to diatoms amended with the particles. Stable isotope technique is sufficiently sensitive to determine the uptake of Zn at an exposure equivalent to lower concentration range (<15 ??g g-1). Without a tracer, detection of newly accumulated Zn is significant at Zn exposure concentration only above 5000 ??g g-1 which represents some of the most contaminated Zn conditions. Only by using a tracer we can study Zn uptake at a range of environmentally realistic exposure conditions. ?? 2010 Elsevier Ltd. All rights reserved.

Plant protein-based feeds and commercial feed enable isotopic tracking of aquaculture emissions into marine macrozoobenthic bioindicator species.

PubMed

Kusche, Henrik; Hillgruber, Nicola; Rößner, Yvonne; Focken, Ulfert

2017-06-01

Brittle stars (Ophiura spp.) and other benthic macrofauna were collected in a prospective mariculture area in the North Sea to determine if these taxa could be used as indicator species to track nutrients released from future offshore aquaculture sites. We analysed natural carbon and nitrogen stable isotopic signatures in tissues from macrofauna and compared these to six feed ingredients and four experimental diets made thereof, as well as to a commercial feed with and without lipid and carbonate removal. Our data suggest practicability of using isotopic signatures of Ophiura spp. to track aquaculture-derived organic material if plant-based fish diet ingredients and commercial feed were used for fish farming in the German Exclusive Economic Zone. Diets with high fish meal content would not be detected in Ophiura spp. using isotopic measures due to the similarity with the marine background. Our data provide valuable baseline information for studies on the impact of offshore aquaculture on the marine environment.

Understanding the role of fog in forest hydrology: Stable isotopes as tools for determining input and partitioning of cloud water in montane forests

USGS Publications Warehouse

Scholl, M.; Eugster, W.; Burkard, R.

2011-01-01

Understanding the hydrology of tropical montane cloud forests (TMCF) has become essential as deforestation of mountain areas proceeds at an increased rate worldwide. Passive and active cloud-water collectors, throughfall and stemflow collectors, visibility or droplet size measurements, and micrometeorological sensors are typically used to measure the fog water inputs to ecosystems. In addition, stable isotopes may be used as a natural tracer for fog and rain. Previous studies have shown that the isotopic signature of fog tends to be more enriched in the heavier isotopes 2H and 18O than that of rain, due to differences in condensation temperature and history. Differences between fog and rain isotopes are largest when rain is from synoptic-scale storms, and fog or orographic cloud water is generated locally. Smaller isotopic differences have been observed between rain and fog on mountains with orographic clouds, but only a few studies have been conducted. Quantifying fog deposition using isotope methods is more difficult in forests receiving mixed precipitation, because of limitations in the ability of sampling equipment to separate fog from rain, and because fog and rain may, under some conditions, have similar isotopic composition. This article describes the various types of fog most relevant to montane cloud forests and the importance of fog water deposition in the hydrologic budget. A brief overview of isotope hydrology provides the background needed to understand isotope applications in cloud forests. A summary of previous work explains isotopic differences between rain and fog in different environments, and how monitoring the isotopic signature of surface water, soil water and tree xylem water can yield estimates of the contribution of fog water to streamflow, groundwater recharge and transpiration. Next, instrumentation to measure fog and rain, and methods to determine isotopic concentrations in plant and soil water are discussed. The article concludes with the identification of some of the more pressing research questions in this field and offers various suggestions for future research. ?? 2010 This article is a US Government work and is in the public domain in the USA.

Full-Spectrum-Analysis Isotope ID

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mitchell, Dean J.; Harding, Lee; Thoreson, Gregory G.

2017-06-28

FSAIsotopeID analyzes gamma ray spectra to identify radioactive isotopes (radionuclides). The algorithm fits the entire spectrum with combinations of pre-computed templates for a comprehensive set of radionuclides with varying thicknesses and compositions of shielding materials. The isotope identification algorithm is suitable for the analysis of spectra collected by gamma-ray sensors ranging from medium-resolution detectors, such a NaI, to high-resolution detectors, such as HPGe. In addition to analyzing static measurements, the isotope identification algorithm is applied for the radiation search applications. The search subroutine maintains a running background spectrum that is passed to the isotope identification algorithm, and it also selectsmore » temporal integration periods that optimize the responsiveness and sensitivity. Gain stabilization is supported for both types of applications.« less

The Determination of the Natural Abundance of the Isotopes of Chlorine: An Introductory Experiment in Mass Spectrometry.

ERIC Educational Resources Information Center

O'Malley, Rebecca M.

1982-01-01

Describes a laboratory experiment which introduces basic principles and experimental techniques of mass spectrometry for fourth year undergraduate (B.Sc.) students. Laboratory procedures, background information, and discussion of results are provided for the experiment in which the natural isotopic abundance of chlorine is determined. (Author/JN)

Acquisition and processing of data for isotope-ratio-monitoring mass spectrometry

NASA Technical Reports Server (NTRS)

Ricci, M. P.; Merritt, D. A.; Freeman, K. H.; Hayes, J. M.

1994-01-01

Methods are described for continuous monitoring of signals required for precise analyses of 13C, 18O, and 15N in gas streams containing varying quantities of CO2 and N2. The quantitative resolution (i.e. maximum performance in the absence of random errors) of these methods is adequate for determination of isotope ratios with an uncertainty of one part in 10(5); the precision actually obtained is often better than one part in 10(4). This report describes data-processing operations including definition of beginning and ending points of chromatographic peaks and quantitation of background levels, allowance for effects of chromatographic separation of isotopically substituted species, integration of signals related to specific masses, correction for effects of mass discrimination, recognition of drifts in mass spectrometer performance, and calculation of isotopic delta values. Characteristics of a system allowing off-line revision of parameters used in data reduction are described and an algorithm for identification of background levels in complex chromatograms is outlined. Effects of imperfect chromatographic resolution are demonstrated and discussed and an approach to deconvolution of signals from coeluting substances described.

Simultaneous 99mtc/111in spect reconstruction using accelerated convolution-based forced detection monte carlo

NASA Astrophysics Data System (ADS)

Karamat, Muhammad I.; Farncombe, Troy H.

2015-10-01

Simultaneous multi-isotope Single Photon Emission Computed Tomography (SPECT) imaging has a number of applications in cardiac, brain, and cancer imaging. The major concern however, is the significant crosstalk contamination due to photon scatter between the different isotopes. The current study focuses on a method of crosstalk compensation between two isotopes in simultaneous dual isotope SPECT acquisition applied to cancer imaging using 99mTc and 111In. We have developed an iterative image reconstruction technique that simulates the photon down-scatter from one isotope into the acquisition window of a second isotope. Our approach uses an accelerated Monte Carlo (MC) technique for the forward projection step in an iterative reconstruction algorithm. The MC estimated scatter contamination of a radionuclide contained in a given projection view is then used to compensate for the photon contamination in the acquisition window of other nuclide. We use a modified ordered subset-expectation maximization (OS-EM) algorithm named simultaneous ordered subset-expectation maximization (Sim-OSEM), to perform this step. We have undertaken a number of simulation tests and phantom studies to verify this approach. The proposed reconstruction technique was also evaluated by reconstruction of experimentally acquired phantom data. Reconstruction using Sim-OSEM showed very promising results in terms of contrast recovery and uniformity of object background compared to alternative reconstruction methods implementing alternative scatter correction schemes (i.e., triple energy window or separately acquired projection data). In this study the evaluation is based on the quality of reconstructed images and activity estimated using Sim-OSEM. In order to quantitate the possible improvement in spatial resolution and signal to noise ratio (SNR) observed in this study, further simulation and experimental studies are required.

The IRHUM database - bioavailable strontium isotope ratios of France for geochemical fingerprinting

NASA Astrophysics Data System (ADS)

Willmes, Malte; Moffat, Ian; Grün, Rainer; Armstrong, Richard; Kinsley, Les; McMorrow, Linda

2013-04-01

Strontium isotope ratios (87Sr/86Sr) are used as a geochemical tracer in a wide range of fields including archaeology, ecology, soil, food and forensic sciences. These applications are based on the principle that strontium isotopic ratios of materials reflect the geological sources of the strontium, which were available during its formation. Geologic regions with distinct strontium isotope ranges, which depend on their age and composition, can be differentiated. A major constraint for current studies is the lack of robust reference maps to evaluate the strontium isotope ratios measured in the samples. The aim of the IRHUM (isotopic reconstruction of human migration) database is to provide a reference map of bioavailable strontium isotope ratios for continental France. The current dataset contains 400 sample locations covering the major geologic units of the Paris and Aquitaine Basin, the Massif Central, and the Pyrenees. At each site soil and plant samples have been collected to cover the whole range of strontium ratios at a specific location. The database is available online at www.rses.anu.edu.au/research-areas/archaeogeochemistry and contains the bioavailable strontium isotope data as well as major and trace element concentrations for soil and plant samples. Strontium isotopes were analysed using a Neptune multi-collector inductively-coupled plasma mass spectrometer (MC-ICP-MS) and elemental concentrations with a Varian Vista Pro Axial ICP-AES (inductively-coupled plasma atomic emission spectrometer). In addition, IRHUM provides spatial context for each sample, including background geology, field observations and soil descriptions. This metadata allows users to evaluate the suitability of a specific data point for their study. The IRHUM database fills an important gap between high resolution studies from specific sites (e.g. archaeological sites), to the very broad geochemical mapping of Europe. Thus it provides an excellent tool to evaluate the regional context of a sample and complement more closed spaced studies. New results will be added to the database continuously with the aim of covering all major geologic units of France within the next year.

Fast-Neutron Activation of Long-Lived Isotopes in Enriched Ge

DOE Office of Scientific and Technical Information (OSTI.GOV)

Elliott, Steven R.; Guiseppe, Vincente; LaRoque, B. H.

2010-11-16

We measured the production of 57Co, 54Mn, 68Ge, 65Zn, and 60Co in an sample of Ge enriched in isotope 76 due to high-energy neutron interactions. These isotopes are critical in understanding background in Ge detectors used for double-beta decay experiments. These isotopes are produced by cosmogenic-neutron interactions in the detectors while they reside on the Earth's surface. We compared the measured production to that predicted by cross-section calculations based on CEM03.02. The cross section calculations over-predict our measurements by approximately a factor of 2-3 depending on isotope. We then use the measured cosmic-ray neutron ux and our results to predictmore » the cosmogenic production rate with an accuracy near 15%.« less

Exploiting Stable Mercury Isotopic Analysis to Differentiate between Mercury Sources: Gold Mining vs. Land-Use Change (Invited)

NASA Astrophysics Data System (ADS)

Bergquist, B. A.; Adler Miserendino, R. A.; Guimarães, J. R.; Veiga, M.; Velasquez-López, P.; Lees, P. S.; Thibodeau, A. M.; Fernandez, L. E.

2013-12-01

In parts of the developing world, mercury (Hg) is used to extract gold by amalgamation during artisanal and small-scale gold mining (ASGM) and this can lead to contamination of downstream aquatic ecosystems. Differentiation between Hg from ASGM and from other sources of Hg, such as increased erosion from land cover and land use change (LCLUC), is challenging and has lead to heated debates over the dominant sources of elevated Hg in some ecosystems. Here, stable Hg isotopic analysis was applied in two aquatic ecosystems in South America: (1) the Amazonian aquatic ecosystem of Amapá, Brazil downstream of artisanal gold mining (AGM) and (2) the Puyango-Tumbes River ecosystem downstream of Portovelo-Zaruma, Ecuador, a large mining area where both AGM and small-scale gold mining (SGM) are in operation. The Hg isotopic analyses from Amapá, Brazil, do not support AGM as the source of elevated Hg in the downstream aquatic ecosystem. Instead, Hg isotopes are most consistent with the elevated Hg being from preferential migration of Hg from soil erosion, which is likely associated with land use change. Although soils are regarded as Hg sinks in the global Hg cycle, this work suggests that LCLUC can disrupt Hg stores with significant ecological consequences. In contrast in the Southwestern Andean region of Ecuador and Peru, analysis of Hg isotopes and other toxic metals (i.e., Pb, Zn, Cu), which are associated with the larger scale mining and cyanide used during SGM, demonstrate Hg used during gold mining is the predominant source of Hg downstream and can be traced far from the dominant mining area. Although it has been speculated that Hg from SGM in Ecuador was not that mobile or that Hg far downstream of SGM processing plants was from erosion due to LCLUC or from AGM taking place downstream, the isotopically heavy signature of Hg used during gold mining and elevated other metal concentrations were observed ~120 km downstream of Portovelo-Zaruma. Mercury isotopes appear able to differentiate mining Hg from the non-mining background, which includes runoff from soils and atmospheric deposition, but they cannot distinguish between Hg used during mining from different mining regions or Hg used during AGM versus SGM. Thus, other toxic metals were measured that are more likely to be associated with SGM as opposed to AGM. Together, these studies demonstrate that variations in stable Hg isotopes are a viable tool to differentiate between Hg sources. Although there are unconstrained or unknown aspects of the stable Hg isotope cycle, the isotopic differences between Hg used during ASGM and from background soil, sediment and atmospheric deposition are large enough not to be obscured by changes in isotopic distributions that may be induced as Hg is transported through the environment. This is likely because most of the Hg in the above aquatic ecosystems is bound to particles and colloids and transported such that most of the Hg does not undergo transformations that fractionate Hg isotopes. For example, in the Puyango-Tumbes River, greater than 95% of the Hg is transported in the particulate phase. Thus, in areas where Hg is transported primarily in the particulate or colloidal form, it can be traced if Hg sources are isotopically distinct. Additionally, the contrasting results in our two studies show that scale and processing differences between AGM and SGM influence the extent of Hg contamination.

β-decay spectroscopy of r-process nuclei with N = 126 at KISS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hirayama, Y.; Watanabe, Y. X.; Imai, N.

2014-05-02

The β-decay properties of nuclei with N = 126, which are believed to act as progenitors in the rapid neutron capture (r-) process path forming the third peak (A ∼ 195) in the observed r-abundance element distribution, are considered critical for understanding the production of heavy elements such as gold and platinum at astrophysical sites. We have constructed the KEK Isotope Separation System (KISS), which consists of a gas cell based laser ion source (atomic number selection) and an isotope separation on-line (ISOL) (mass number selection), to produce pure low-energy beams of neutron-rich isotopes around N = 126 and tomore » study their β-decay properties, which are also of interest for astrophysics. The isotopes of interest will be produced by multi-nucleon transfer reactions in heavy ion collisions (e.g. {sup 136}Xe projectile on {sup 198}Pt target). KISS will allow us to study unknown isotopes produced in weak reaction channels under low background conditions. We successfully extracted the stable {sup 56}Fe beam from KISS at the last commissioning on-line experiment with the extraction efficiency of 0.25% and beam purity of more than 98%. We can access the nuclei with N = 126 and measure their half-lives using the KISS in the case of the extraction efficiency of 0.1%.« less

Study of 236U/238U ratio at CIRCE using a 16-strip silicon detector with a TOF system

NASA Astrophysics Data System (ADS)

De Cesare, M.; De Cesare, N.; D'Onofrio, A.; Gialanella, L.; Terrasi, F.

2015-04-01

Accelerator Mass Spectrometry (AMS) is presently the most sensitive technique for the measurement of long-lived actinides, e.g. 236U and xPu isotopes. A new actinide AMS system, based on a 3-MV pelletron tandem accelerator, is operated at the Center for Isotopic Research on Cultural and Environmental Heritage (CIRCE) in Caserta, Italy. In this paper we report on the procedure adopted to increase the 236U abundance sensitivity as low as possible. The energy and position determinations of the 236U ions, using a 16-strip silicon detector have been obtained. A 236U/238U isotopic ratio background level of about 2.9×10-11 was obtained, summing over all the strips, using a Time of Flight-Energy (TOF-E) system with a 16-strip silicon detector (4.9×10-12 just with one strip).

Spurious and functional correlates of the isotopic composition of a generalist across a tropical rainforest landscape

PubMed Central

2009-01-01

Background The isotopic composition of generalist consumers may be expected to vary in space as a consequence of spatial heterogeneity in isotope ratios, the abundance of resources, and competition. We aim to account for the spatial variation in the carbon and nitrogen isotopic composition of a generalized predatory species across a 500 ha. tropical rain forest landscape. We test competing models to account for relative influence of resources and competitors to the carbon and nitrogen isotopic enrichment of gypsy ants (Aphaenogaster araneoides), taking into account site-specific differences in baseline isotope ratios. Results We found that 75% of the variance in the fraction of 15N in the tissue of A. araneoides was accounted by one environmental parameter, the concentration of soil phosphorus. After taking into account landscape-scale variation in baseline resources, the most parsimonious model indicated that colony growth and leaf litter biomass accounted for nearly all of the variance in the δ15N discrimination factor, whereas the δ13C discrimination factor was most parsimoniously associated with colony size and the rate of leaf litter decomposition. There was no indication that competitor density or diversity accounted for spatial differences in the isotopic composition of gypsy ants. Conclusion Across a 500 ha. landscape, soil phosphorus accounted for spatial variation in baseline nitrogen isotope ratios. The δ15N discrimination factor of a higher order consumer in this food web was structured by bottom-up influences - the quantity and decomposition rate of leaf litter. Stable isotope studies on the trophic biology of consumers may benefit from explicit spatial design to account for edaphic properties that alter the baseline at fine spatial grains. PMID:19930701

Effects of variation in background mixing ratios of N2, O2, and Ar on the measurement of δ18O-H2O and δ2H-H2O values by cavity ring-down spectroscopy

NASA Astrophysics Data System (ADS)

Johnson, Jennifer E.; Rella, Chris W.

2017-08-01

Cavity ring-down spectrometers have generally been designed to operate under conditions in which the background gas has a constant composition. However, there are a number of observational and experimental situations of interest in which the background gas has a variable composition. In this study, we examine the effect of background gas composition on a cavity ring-down spectrometer that measures δ18O-H2O and δ2H-H2O values based on the amplitude of water isotopologue absorption features around 7184 cm-1 (L2120-i, Picarro, Inc.). For background mixtures balanced with N2, the apparent δ18O values deviate from true values by -0.50 ± 0.001 ‰ O2 %-1 and -0.57 ± 0.001 ‰ Ar %-1, and apparent δ2H values deviate from true values by 0.26 ± 0.004 ‰ O2 %-1 and 0.42 ± 0.004 ‰ Ar %-1. The artifacts are the result of broadening, narrowing, and shifting of both the target absorption lines and strong neighboring lines. While the background-induced isotopic artifacts can largely be corrected with simple empirical or semi-mechanistic models, neither type of model is capable of completely correcting the isotopic artifacts to within the inherent instrument precision. The development of strategies for dynamically detecting and accommodating background variation in N2, O2, and/or Ar would facilitate the application of cavity ring-down spectrometers to a new class of observations and experiments.

Charge state breeding experiences and plans at TRIUMF

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ames, F., E-mail: ames@triumf.ca; Marchetto, M.; Mjøs, A.

At the Isotope Separation and ACceleration (ISAC) facility at TRIUMF, an electron cyclotron resonance ion source (ECRIS) has been set up for the charge state breeding of radioactive ions. In order to reduce background from stable ions generated in the ECRIS, several measures, including changing materials for the plasma chamber and the surrounding components, have been implemented. Further reduction has been achieved by using the post-accelerator chain as a mass filter. Since the implementation of those measures in 2013, physics experiments with accelerated radioactive isotopes of Rb, Sr, K, and Mg have been performed. In most cases, a charge breedingmore » efficiency of several percent has been achieved. With the planned expansion of the isotope production capabilities at TRIUMF within the Advanced Rare IsotopE Laboratory project, two new target stations, one using photo-fission induced by a high-power electron beam at 50 MeV and the other one using 480 MeV protons as at ISAC, will be put into operation within the next 5 yr. Additionally, a new electron beam ion source (EBIS) based charge state breeding system will be installed. Background from such a source is expected to be much lower. The drawback is that for the efficient operation of such a system, pulsed beam operation is required, which makes the installation of an additional ion buncher in front of the EBIS necessary.« less

Tracking Urban Air Deterioration in San Francisco: Carbon and Nitrogen Isotope Study of Weedy Plants.

NASA Astrophysics Data System (ADS)

Colman, A. S.; Wessells, A.; Swaine, M. E.; Fogel, M. L.

2003-12-01

Stable isotopes of carbon and nitrogen have long been used as indicators of ecosystem structure and nutrient cycling in natural and anthropogenically disturbed terrestrial ecosytems. However, relatively few of these studies have targeted urban environments, where nitrogen and CO2 emissions dramatically impact atmospheric composition. Here we present the results of carbon and nitrogen isotope analyses of herbaceous plants growing in and around San Francisco. These plants were collected mainly as part of a public outreach walking tour of San Francisco ("The Weed Walk - Concrete Jungle") sponsored by the San Francisco Exploratorium. In all cases, the plants were sampled in areas with negligible forest canopy. A consortium of species was collected at each of several distinct sites to examine the localized and regional impact of automobile traffic and proximity to the ocean on isotopic compositions of carbon and nitrogen. δ 13C measurements trend towards relatively light values in the range of --26 to --36 permil. In comparison, the leaves from similar types of herbaceous species in relatively unpolluted and unforested environments typically have δ 13C values in the range of --22 to --28 permil. The observed light carbon isotopic compositions potentially reflect input of isotopically light CO2 emissions from fossil fuel burning, boosting atmospheric CO2 concentrations to >10 % above background. δ 15N values range from +4 to +9 permil. This is substantially offset from the --4 to +1 permil values that typify vegetation in regions where nitrogen oxides from fossil fuel combustion dominate the nitrogen inputs. The nitrogen isotope compositions might suggest nitrogen contributions from a marine source (typically +6 permil).

Calibration and field testing of cavity ring-down laser spectrometers measuring CH4, CO2, and δ13CH4 deployed on towers in the Marcellus Shale region

NASA Astrophysics Data System (ADS)

Miles, Natasha L.; Martins, Douglas K.; Richardson, Scott J.; Rella, Christopher W.; Arata, Caleb; Lauvaux, Thomas; Davis, Kenneth J.; Barkley, Zachary R.; McKain, Kathryn; Sweeney, Colm

2018-03-01

Four in situ cavity ring-down spectrometers (G2132-i, Picarro, Inc.) measuring methane dry mole fraction (CH4), carbon dioxide dry mole fraction (CO2), and the isotopic ratio of methane (δ13CH4) were deployed at four towers in the Marcellus Shale natural gas extraction region of Pennsylvania. In this paper, we describe laboratory and field calibration of the analyzers for tower-based applications and characterize their performance in the field for the period January-December 2016. Prior to deployment, each analyzer was tested using bottles with various isotopic ratios, from biogenic to thermogenic source values, which were diluted to varying degrees in zero air, and an initial calibration was performed. Furthermore, at each tower location, three field tanks were employed, from ambient to high mole fractions, with various isotopic ratios. Two of these tanks were used to adjust the calibration of the analyzers on a daily basis. We also corrected for the cross-interference from ethane on the isotopic ratio of methane. Using an independent field tank for evaluation, the standard deviation of 4 h means of the isotopic ratio of methane difference from the known value was found to be 0.26 ‰ δ13CH4. Following improvements in the field tank testing scheme, the standard deviation of 4 h means was 0.11 ‰, well within the target compatibility of 0.2 ‰. Round-robin style testing using tanks with near-ambient isotopic ratios indicated mean errors of -0.14 to 0.03 ‰ for each of the analyzers. Flask to in situ comparisons showed mean differences over the year of 0.02 and 0.08 ‰, for the east and south towers, respectively. Regional sources in this region were difficult to differentiate from strong perturbations in the background. During the afternoon hours, the median differences of the isotopic ratio measured at three of the towers, compared to the background tower, were &minus0.15 to 0.12 ‰ with standard deviations of the 10 min isotopic ratio differences of 0.8 ‰. In terms of source attribution, analyzer compatibility of 0.2 ‰ δ13CH4 affords the ability to distinguish a 50 ppb CH4 peak from a biogenic source (at -60 ‰, for example) from one originating from a thermogenic source (-35 ‰), with the exact value dependent upon the source isotopic ratios. Using a Keeling plot approach for the non-afternoon data at a tower in the center of the study region, we determined the source isotopic signature to be -31.2 ± 1.9 ‰, within the wide range of values consistent with a deep-layer Marcellus natural gas source.

Field isotopic study of lead fate and compartmentalization in earthworm-soil-metal particle systems for highly polluted soil near Pb recycling factory.

PubMed

Goix, Sylvaine; Mombo, Stéphane; Schreck, Eva; Pierart, Antoine; Lévêque, Thibaut; Deola, Frédéric; Dumat, Camille

2015-11-01

Earthworms are important organisms in soil macrofauna and play a key role in soil functionality, and consequently in terrestrial ecotoxicological risk assessments. Because they are frequently observed in soils strongly polluted by metals, the influence of earthworm bioturbation on Pb fate could therefore be studied through the use of Pb isotopes. Total Pb concentrations and isotopic composition ((206)Pb, (207)Pb and (208)Pb) were then measured in earthworms, casts and bulk soils sampled at different distance from a lead recycling factory. Results showed decreasing Pb concentrations with the distance from the factory whatever the considered matrix (bulk soils, earthworm bodies or cast samples) with higher concentrations in bulk soils than in cast samples. The bivariate plot (208)Pb/(206)Pb ratios versus (206)Pb/(207)Pb ratios showed that all samples can be considered as a linear mixing between metallic process particulate matter (PM) and geochemical Pb background. Calculated anthropogenic fraction of Pb varied between approximately 84% and 100%. Based on Pb isotopic signatures, the comparison between casts, earthworms and bulk soils allowed to conclude that earthworms preferentially ingest the anthropogenic lead fraction associated with coarse soil organic matter. Actually, soil organic matter was better correlated with Pb isotopic ratios than with Pb content in soils. The proposed hypothesis is therefore a decrease of soil organic matter turnover due to Pb pollution with consequences on Pb distribution in soils and earthworm exposure. Finally, Pb isotopes analysis constitutes an efficient tool to study the influence of earthworm bioturbation on Pb cycle in polluted soils. Copyright © 2015 Elsevier Ltd. All rights reserved.

Natural calcium isotonic composition of urine as a marker of bone mineral balance

USGS Publications Warehouse

Skulan, J.; Bullen, T.; Anbar, A.D.; Puzas, J.E.; Shackelford, L.; LeBlanc, A.; Smith, S.M.

2007-01-01

Background: We investigated whether changes in the natural isotopic composition of calcium in human urine track changes in net bone mineral balance, as predicted by a model of calcium isotopic behavior in vertebrates. If so, isotopic analysis of natural urine or blood calcium could be used to monitor short-term changes in bone mineral balance that cannot be detected with other techniques. Methods: Calcium isotopic compositions are expressed as ??44Ca, or the difference in parts per thousand between the 44Ca/40Ca of a sample and the 44Ca/ 40Ca of a standard reference material. ??44Ca was measured in urine samples from 10 persons who participated in a study of the effectiveness of countermeasures to bone loss in spaceflight, in which 17 weeks of bed rest was used to induce bone loss. Study participants were assigned to 1 of 3 treatment groups: controls received no treatment, one treatment group received alendronate, and another group performed resistive exercise. Measurements were made on urine samples collected before, at 2 or 3 points during, and after bed rest. Results: Urine ??44Ca values during bed rest were lower in controls than in individuals treated with alendronate (P <0.05, ANOVA) or exercise (P <0.05), and lower than the control group baseline (P <0.05, Mest). Results were consistent with the model and with biochemical and bone mineral density data. Conclusion: Results confirm the predicted relationship between bone mineral balance and calcium isotopes, suggesting that calcium isotopic analysis of urine might be refined into a clinical and research tool. ?? 2007 American Association for Clinical Chemistry.

Nature and origin of the sedimentary pile subducting in the Nankai Through

NASA Astrophysics Data System (ADS)

Chauvel, C.; Garcon, M.; Yobregat, E.; Chipoulet, C.; Labanieh, S.

2013-12-01

Nd-Hf isotopes and trace and major element concentrations were measured on bulk sediments recovered at Site C0012 during IODP Expedition 322 and 333 in the Shikoku basin. We analyzed the composition of different lithologies such as clay, claystone, sand, sandstone, and ash layers, all through the sedimentary pile, from the surface to the sediment-basalt interface, in order to identify compositional trends and source variations with depth. Major and trace element contents of the background sediments (hemipelagic mudstone) are very homogenous and span a relatively small range of values throughout the entire sedimentary pile. Their composition resembles that of the average upper continental crust of Rudnick and Gao (2003, Treatise on Geochemistry, Vol.3, p. 1-64). Nd and Hf isotopes are more variable, relatively unradiogenic (-8 < ɛNd < -3 ; -4 < ɛHf < +5) but display no systematic variations with depth (Fig. 1). Such isotopic compositions indicate that the background sedimentation of the Shikoku basin may consist of volcaniclastic material from the Izu-Bonin and/or Ryukyu arcs, detrital material eroded from SW Japan and relatively high amount of an evolved continental-derived component, probably Chinese loess as already suggested by Mahomet (2005, Sediment. Geol., 182, p.183-199). Compared to the background sedimentation, volcanic ash layers and volcaniclastic sandstones have very different trace element patterns and more radiogenic Nd-Hf isotopic signature (Fig. 1). Our results allow us to distinguish at least two different volcanic sources for these deposits. At the bottom of the sedimentary pile, siliciclastic sandstones with a mid-Miocene age are present; they have remarkably low ɛNd and ɛHf values (i.e. ɛNd < -8 and ɛHf < -5). Such isotopic compositions clearly demonstrate that their source cannot be the Japanese mainland, as suggested by previous studies (e.g. Underwood et al, 2009, Exp.322 PR ; Fergusson, 2003, Proc. ODP, Sci. Results 190/196). These sandstones are also too coarse to result from an accumulation of Chinese loess transported by wind (particles usually finer than 40 μm). Given the location of the Shikoku basin at 15Ma, we suggest that the siliciclastic sandstones mainly consists of detrital materials transported by Chinese rivers up to the sea in the Shikoku basin. Variations of ɛNd as a function of depth. Potential sediment sources are indicated by color bands

Paleoceanographic Inferences from Carbon and Nitrogen Isotopic Compositions of Cenomanian Black Shales from DSDP/ODP Sites 367, 530, 603, 641, 1257-1261, and 1276 in the Atlantic Ocean

NASA Astrophysics Data System (ADS)

Yum, J.; Meyers, P. A.; Bernasconi, S. M.; Arnaboldi, M.

2005-12-01

The mid-Cretaceous (Cenomanian- Turonian) was characterized as a peak global greenhouse period with highest sea level, highest CO2 concentration in atmosphere and low thermal gradients from the poles to the equator. The depositional environment of the organic-carbon-rich black shales that typify this period remains an open question. A total of 180 Cenomanian- Turonian core samples were selected from multiple ODP and DSDP sites in the Atlantic Ocean: 530 (Cape Basin), 603 (Hatteras Rise), 641 (Galicia Bank), 1257-1261 (Demerara Rise), 1276 (Newfoundland Basin). Total organic carbon and nitrogen concentrations and isotopic compositions were measured to investigate variations in the proto-Atlantic Ocean paleoceanographic conditions that contributed to the origin of the black shales for this period. These new data were combined with existing data from Sites 367 (Senegal Rise), 530, and 603. Both the black shales and the organic-carbon-poor background sediments (less than 1 percent) have carbon isotope values between -29 to -22 permil. The C/N ratios of the background sediments are low (less than 20) compared to those of the black shales (20-40). Nitrogen isotope values range from 0 to 4 permil in the background samples. All black shales have similarly low nitrogen isotope values that range between -4 to 0 permil. These exceptionally low values are inferred to reflect the productivity of blue green algae and cyanobacteria under strongly surface stratified oceanic conditions. Although carbon isotope and C/N values of black shales show almost similar patterns at each location, there are site-specific shifts in these data that could be related to the amount of continental run off and/or the effect of latitude. Our multi-site comparison suggests that specially stratified depositional environments that could produce and accumulate the abnormally high carbon concentrations in sediments occurred throughout the proto-Atlantic ocean during the mid-Cretaceous. However, regional factors affected the amount and origin of organic matter delivered to each location.

Isotopic Characterization of Mercury Downstream of Historic Industrial Contamination in the South River, Virginia.

PubMed

Washburn, Spencer J; Blum, Joel D; Demers, Jason D; Kurz, Aaron Y; Landis, Richard C

2017-10-03

Historic point source mercury (Hg) contamination from industrial processes on the South River (Waynesboro, Virginia) ended decades ago, but elevated Hg concentrations persist in the river system. In an effort to better understand Hg sources, mobility, and transport in the South River, we analyzed total Hg (THg) concentrations and Hg stable isotope compositions of streambed sediments, stream bank soils, suspended particles, and filtered surface waters. Samples were collected along a longitudinal transect of the South River, starting upstream of the historic Hg contamination point-source and extending downstream to the confluence with the South Fork Shenandoah River. Analysis of the THg concentration and Hg isotopic composition of these environmental samples indicates that the regional background Hg source is isotopically distinct in both Δ 199 Hg and δ 202 Hg from Hg derived from the original source of contamination, allowing the tracing of contamination-sourced Hg throughout the study reach. Three distinct end-members are required to explain the Hg isotopic and concentration variation observed in the South River. A consistent negative offset in δ 202 Hg values (∼0.28‰) was observed between Hg in the suspended particulate and dissolved phases, and this fractionation provides insight into the processes governing partitioning and transport of Hg in this contaminated river system.

Diode-laser-based RIMS measurements of strontium-90

NASA Astrophysics Data System (ADS)

Bushaw, B. A.; Cannon, B. D.

1998-12-01

Double- and triple-resonance excitation schemes for the ionization of strontium are presented. Use of single-mode diode lasers for the resonance excitations provides a high degree of optical isotopic selectivity: with double-resonance, selectivity of >104 for 90Sr against the stable Sr isotopes has been demonstrated. Measurement of lineshapes and stable isotope shifts in the triple-resonance process indicate that optical selectivity should increase to ˜109. When combined with mass spectrometer selectivity this is sufficient for measurement of 90Sr at background environmental levels. Additionally, autoionizing resonances have been investigated for improving ionization efficiency with lower power lasers.

Real-time Stack Monitoring at the BaTek Medical Isotope Production Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

McIntyre, Justin I.; Agusbudiman, A.; Cameron, Ian M.

2016-04-01

Radioxenon emissions from radiopharmaceutical production are a major source of background concentrations affecting the radioxenon detection systems of the International Monitoring System (IMS). Collection of real-time emissions data from production facilities makes it possible to screen out some medical isotope signatures from the IMS radioxenon data sets. This paper describes an effort to obtain and analyze real-time stack emissions data with the design, construction and installation of a small stack monitoring system developed by a joint CTBTO-IDC, BATAN, and PNNL team at the BaTek medical isotope production facility near Jakarta, Indonesia.

Existing and emerging technologies for measuring stable isotope labelled retinol in biological samples: isotope dilution analysis of body retinol stores.

PubMed

Preston, Tom

2014-01-01

This paper discusses some of the recent improvements in instrumentation used for stable isotope tracer measurements in the context of measuring retinol stores, in vivo. Tracer costs, together with concerns that larger tracer doses may perturb the parameter under study, demand that ever more sensitive mass spectrometric techniques are developed. GCMS is the most widely used technique. It has high sensitivity in terms of sample amount and uses high resolution GC, yet its ability to detect low isotope ratios is limited by background noise. LCMSMS may become more accessible for tracer studies. Its ability to measure low level stable isotope tracers may prove superior to GCMS, but it is isotope ratio MS (IRMS) that has been designed specifically for low level stable isotope analysis through accurate analysis of tracer:tracee ratios (the tracee being the unlabelled species). Compound-specific isotope analysis, where GC is interfaced to IRMS, is gaining popularity. Here, individual 13C-labelled compounds are separated by GC, combusted to CO2 and transferred on-line for ratiometric analysis by IRMS at the ppm level. However, commercially-available 13C-labelled retinol tracers are 2 - 4 times more expensive than deuterated tracers. For 2H-labelled compounds, GC-pyrolysis-IRMS has now become more generally available as an operating mode on the same IRMS instrument. Here, individual compounds are separated by GC and pyrolysed to H2 at high temperature for analysis by IRMS. It is predicted that GC-pyrolysis-IRMS will facilitate low level tracer procedures to measure body retinol stores, as has been accomplished in the case of fatty acids and amino acids. Sample size requirements for GC-P-IRMS may exceed those of GCMS, but this paper discusses sample preparation procedures and predicts improvements, particularly in the efficiency of sample introduction.

The MAJORANA Demonstrator Radioassay Program

DOE Office of Scientific and Technical Information (OSTI.GOV)

Abgrall, N.; Arnquist, Isaac J.; Avignone, F. T.

2016-05-03

The Majorana collaboration is constructing the Majorana Demonstrator at the Sanford Underground Research Facility at the Homestake gold mine, in Lead, SD. The apparatus will use Ge detectors, enriched in isotope 76Ge, to demonstrate the feasibility of a large-scale Ge detector experiment to search for neutrinoless double beta decay. The long half-life of this postulated process requires that the apparatus be extremely low in radioactive isotopes whose decays may produce backgrounds to the search. The radioassay program conducted by the collaboration to ensure that the materials comprising the apparatus are suffciently pure is described. The resulting measurements of the radioactiveisotopemore » contamination for a number of materials studied for use in the detector are reported.« less

Stable isotope and DNA evidence for ritual sequences in Inca child sacrifice

PubMed Central

Wilson, Andrew S.; Taylor, Timothy; Ceruti, Maria Constanza; Chavez, Jose Antonio; Reinhard, Johan; Grimes, Vaughan; Meier-Augenstein, Wolfram; Cartmell, Larry; Stern, Ben; Richards, Michael P.; Worobey, Michael; Barnes, Ian; Gilbert, M. Thomas P.

2007-01-01

Four recently discovered frozen child mummies from two of the highest peaks in the south central Andes now yield tantalizing evidence of the preparatory stages leading to Inca ritual killing as represented by the unique capacocha rite. Our interdisciplinary study examined hair from the mummies to obtain detailed genetic and diachronic isotopic information. This approach has allowed us to reconstruct aspects of individual identity and diet, make inferences concerning social background, and gain insight on the hitherto unknown processes by which victims were selected, elevated in social status, prepared for a high-altitude pilgrimage, and killed. Such direct information amplifies, yet also partly contrasts with, Spanish historical accounts. PMID:17923675

Background modeling for the GERDA experiment

NASA Astrophysics Data System (ADS)

Becerici-Schmidt, N.; Gerda Collaboration

2013-08-01

The neutrinoless double beta (0νββ) decay experiment GERDA at the LNGS of INFN has started physics data taking in November 2011. This paper presents an analysis aimed at understanding and modeling the observed background energy spectrum, which plays an essential role in searches for a rare signal like 0νββ decay. A very promising preliminary model has been obtained, with the systematic uncertainties still under study. Important information can be deduced from the model such as the expected background and its decomposition in the signal region. According to the model the main background contributions around Qββ come from 214Bi, 228Th, 42K, 60Co and α emitting isotopes in the 226Ra decay chain, with a fraction depending on the assumed source positions.

Uranium Isotopic Ratio Measurements of U3O8 Reference Materials by Atom Probe Tomography

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fahey, Albert J.; Perea, Daniel E.; Bartrand, Jonah AG

2016-01-01

We report results of measurements of isotopic ratios obtained with atom probe tomography on U3O8 reference materials certified for their isotopic abundances of uranium. The results show good agreement with the certified values. High backgrounds due to tails from adjacent peaks complicate the measurement of the integrated peak areas as well as the fact that only oxides of uranium appear in the spectrum, the most intense of which is doubly charged. In addition, lack of knowledge of other instrumental parameters, such as the dead time, may bias the results. Isotopic ratio measurements can be performed at the nanometer-scale with themore » expectation of sensible results. The abundance sensitivity and mass resolving power of the mass spectrometer are not sufficient to compete with magnetic-sector instruments but are not far from measurements made by ToF-SIMS of other isotopic systems. The agreement of the major isotope ratios is more than sufficient to distinguish most anthropogenic compositions from natural.« less

Long-term fate of depleted uranium at Aberdeen and Yuma Proving Grounds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ebinger, M.H.; Essington, E.H.; Gladney, E.S.

1990-06-01

The environmental fate of fragments of depleted uranium (DU) penetrators in soils and waters at Aberdeen Proving Ground (APG) and Yuma Proving Ground (YPG) is a concern to the Testing and Evaluation Command (TECOM) of the US Army. This report presents the information from preliminary soil and water samples that were collected from the humid woodlands of APG and the arid Sonoran Desert of YPG. Soil samples collected beneath a penetrator fragment of the firing range at APG showed approximately 12% DU by weight in the surface horizon and DU significantly above background to a depth of about 20 cm.more » Samples of surface water at APG showed U only at background levels, and bottom sediments showed background U levels but with isotopic ratios of DU instead of natural U. Soil samples beneath a penetrator fragment at YPG showed about 0.5% by weight U in the surface horizon, but only background concentrations and isotopic ratios of U between 8 and 20 cm depth. Results from this preliminary study indicate that DU at APG was redistributed primarily be dissolution and transport with water and possibly by migration of DU colloids or DU attached to small particles. Redistribution at YPG, however, was mainly due to erosion of DU fragments from the impact area and redeposition in washes that drain the area. Proposed work for FY90-FY92 includes additional field sampling, laboratory column studies, and the development of a computer model of DU redistribution at both sites. 39 refs., 11 figs., 5 tabs.« less

Employing extant stable carbon isotope data in Gulf of Mexico sedimentary organic matter for oil spill studies

NASA Astrophysics Data System (ADS)

Rosenheim, Brad E.; Pendergraft, Matthew A.; Flowers, George C.; Carney, Robert; Sericano, José L.; Amer, Reda M.; Chanton, Jeff; Dincer, Zeynep; Wade, Terry L.

2016-07-01

We have compiled and mapped available carbon isotope data from sedimentary organic material sampled from the Gulf of Mexico prior to 2010. These data provide a baseline to which any changes in the Gulf of Mexico after the 2010 Deepwater Horizon oil spill can be compared. The mean (±1σ) δ13C values, relative to PDB, are -21.4±1.9‰ (entire Gulf of Mexico), -21.7±1.2‰ (shelf sediments), -20.4±1.6‰ (deepwater sediments), and -25.2±4.1‰ (seep-affected sediments). We compare pre-spill mean δ13C values to carbon isotope measurements of sedimentary organic material from coretop samples collected after the 2010 Deepwater Horizon oil spill. The differences between the mean compiled δ13C values and the post-spill δ13C values are corroborated by qualitative relationships with the concentration of polycyclic aromatic hydrocarbons (PAHs), a proxy for oil contamination, in the sediment. The relationships between δ13C of the sedimentary organic material and PAH concentrations allow estimation of background levels of PAHs on the shelf and in the deep Gulf of Mexico. Higher background levels of PAH on the shelf likely relate to Mississippi River outflow and its deposition of petrogenic PAH in riverine sediments.

First assessment on NOx sources for a regional background site of North China using isotopic analysis linked with modelling

NASA Astrophysics Data System (ADS)

Zong, Zheng; Wang, Xiaoping; Tian, Chongguo

2017-04-01

Nitrogen oxides (NOx, including NO and NO2) play an important role in the formation of new particles. Thus NOx emission reduction is one of the most critical steps to improve the air quality, especially in severe air-polluted areas (e.g. the North China). In this study, the sources and conversion mechanisms of NOx were explored at Beihuangcheng Island (BH), a regional background site in North China. Results showed humidity and oxidants were important promoters for the conversion of NOx to nitrate (NO3-) in the atmosphere. Based on nitrogen isotope and an improved Bayesian mixing model, 61.85 ± 2.50%, 24.46 ± 4.02% and 13.69 ± 3.18% of NOx could be attributed to mobile source, coal combustion and biomass burning, respectively, which indicated that mobile source was the primary source for NOx on BH. Seasonally, mobile source was dominant contributor in summer (75.24 ± 5.29%), spring (61.53 ± 4.66%) and autumn (58.72 ± 4.17%). While residential coal combustion confirmed by Mann-Kendall test and moving simulation contributed a main portion of 71.75 ± 11.35% in winter. This work indicated that isotope-modelling is a promising tool for partitioning NOx sources, and provided policy maker with the valuable insight into the NOx reduction in North China.

Measuring the radium quartet (228Ra, 226Ra, 224Ra, 223Ra) in seawater samples using gamma spectrometry.

PubMed

van Beek, P; Souhaut, M; Reyss, J-L

2010-07-01

Radium isotopes are widely used in marine studies (eg. to trace water masses, to quantify mixing processes or to study submarine groundwater discharge). While 228Ra and 226Ra are usually measured using gamma spectrometry, short-lived Ra isotopes (224Ra and 223Ra) are usually measured using a Radium Delayed Coincidence Counter (RaDeCC). Here we show that the four radium isotopes can be analyzed using gamma spectrometry. We report 226Ra, 228Ra, 224Ra, 223Ra activities measured using low-background gamma spectrometry in standard samples, in water samples collected in the vicinity of our laboratory (La Palme and Vaccarès lagoons, France) but also in seawater samples collected in the plume of the Amazon river, off French Guyana (AMANDES project). The 223Ra and 224Ra activities determined in these samples using gamma spectrometry were compared to the activities determined using RaDeCC. Activities determined using the two techniques are in good agreement. Uncertainties associated with the 224Ra activities are similar for the two techniques. RaDeCC is more sensitive for the detection of low 223Ra activities. Gamma spectrometry thus constitutes an alternate method for the determination of short-lived Ra isotopes. 2009 Elsevier Ltd. All rights reserved.

24-Hour protein, arginine and citrulline metabolism in fed critically ill children – a stable isotope tracer study

PubMed Central

de Betue, Carlijn T.I.; Garcia Casal, Xiomara C.; van Waardenburg, Dick A.; Schexnayder, Stephen M.; Joosten, Koen F.M.; Deutz, Nicolaas E.P.; Engelen, Marielle P.K.J.

2017-01-01

Background & aims The reference method to study protein and arginine metabolism in critically ill children is measuring plasma amino acid appearances with stable isotopes during a short (4–8h) time period and extrapolate results to 24-hour. However, 24-hour measurements may be variable due to critical illness related factors and a circadian rhythm could be present. Since only short duration stable isotope studies in critically ill children have been conducted before, the aim of this study was to investigate 24-hour appearance of specific amino acids representing protein and arginine metabolism, with stable isotope techniques in continuously fed critically ill children. Methods In eight critically ill children, admitted to the pediatric (n=4) or cardiovascular (n=4) intensive care unit, aged 0–10 years, receiving continuous (par)enteral nutrition with protein intake 1.0–3.7 g/kg/day, a 24-hour stable isotope tracer protocol was carried out. L-[ring-2H5]-phenylalanine, L-[3,3-2H2]-tyrosine, L-[5,5,5-2H3]-leucine, L-[guanido-15N2]-arginine and L-[5-13C-3,3,4,4-2H4]-citrulline were infused intravenously and L-[15N]-phenylalanine and L-[1-13C]leucine enterally. Arterial blood was sampled every hour. Results Coefficients of variation, representing intra-individual variability, of the amino acid appearances of phenylalanine, tyrosine, leucine, arginine and citrulline were high, on average 14–19% for intravenous tracers and 23–26% for enteral tracers. No evident circadian rhythm was present. The pattern and overall 24-hour level of whole body protein balance differed per individual. Conclusions In continuously fed stable critically ill children, the amino acid appearances of phenylalanine, tyrosine, leucine, arginine and citrulline show high variability. This should be kept in mind when performing stable isotope studies in this population. There was no apparent circadian rhythm. PMID:28089618

Heterogeneous distribution of Zn stable isotopes in mice and applications to medical sciences

NASA Astrophysics Data System (ADS)

Moynier, F.; Fujii, T.; Shaw, A.; Le Borgne, M.

2013-12-01

Zinc is required for the function of more than 300 enzymes involved in many metabolic pathways, and is a vital micronutrient for living organisms. To investigate if Zn isotopes could be used to better understand metal homeostasis, as well as a biomarker for diseases, we assessed the distribution of natural Zn isotopes in various mouse tissues. We found that, with respect to Zn isotopes, most mouse organs are isotopically distinct and that the total range of variation within one mouse encompasses the variations observed in the Earth's crust. Therefore, biological activity must have a major impact on the distribution of Zn isotopes in inorganic materials. The most striking aspect of the data is that red blood cells and bones are enriched by ~0.5 per mil in 66Zn relative to 64Zn when compared to serum, and up to ~1 per mil when compared to the brain and liver. This fractionation is well explained by the equilibrium distribution of isotopes between different bonding environments of Zn in different organs. Differences in gender and genetic background did not appear to affect the isotopic distribution of Zn. Together, these results suggest that potential use of Zn isotopes as a tracer for dietary Zn, and for detecting disturbances in Zn metabolism due to pathological conditions.

Lead Contamination and Source Characterization in Soils Around a Lead-Zinc Smelting Plant in a Near-Urban Environment in Baoji, China.

PubMed

Deng, Wenbo; Li, Xuxiang; An, Zhisheng; Yang, Liu

2016-11-01

Economic reforms in China since 1978 have promoted nationwide socioeconomic advancement but led to a considerable amount of environmental pollution. The distribution and sources of Pb in a typical peri-urban industrial part of Baoji, China, were assessed by determining the Pb contents and isotopic compositions in 52 topsoil samples from the study area. The topsoil samples were polluted averagely with 40.88 mg Pb kg -1 , was 1.86 times higher than the Pb content of local background soil (22.04 mg kg -1 ). Pb isotopic compositions were determined by analyzing samples prepared using total digestion and acid extraction methods. Radiogenic isotopes contributed more to the Pb concentrations in the acid extracts than in the total digests. This was shown by the 207/206 Pb and 208/206 Pb ratios, which were 0.845-0.88 and 2.088-2.128, respectively, in the acid extracts and 0.841-0.875 and 2.086-2.125, respectively, in the total digests. This indicates that anthropogenic sources of Pb could be identified more sensitively in acid extracts than in total digests. The Pb isotope ratios showed that burning coal and smelting ore are the predominant anthropogenic sources of Pb in the study area, i.e., a lead-zinc smelter and a coking plant are major sources of Pb in the study area.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mitchell, Dean J.; Harding, Lee T.

Isotope identification algorithms that are contained in the Gamma Detector Response and Analysis Software (GADRAS) can be used for real-time stationary measurement and search applications on platforms operating under Linux or Android operating sys-tems. Since the background radiation can vary considerably due to variations in natu-rally-occurring radioactive materials (NORM), spectral algorithms can be substantial-ly more sensitive to threat materials than search algorithms based strictly on count rate. Specific isotopes or interest can be designated for the search algorithm, which permits suppression of alarms for non-threatening sources, such as such as medical radionuclides. The same isotope identification algorithms that are usedmore » for search ap-plications can also be used to process static measurements. The isotope identification algorithms follow the same protocols as those used by the Windows version of GADRAS, so files that are created under the Windows interface can be copied direct-ly to processors on fielded sensors. The analysis algorithms contain provisions for gain adjustment and energy lineariza-tion, which enables direct processing of spectra as they are recorded by multichannel analyzers. Gain compensation is performed by utilizing photopeaks in background spectra. Incorporation of this energy calibration tasks into the analysis algorithm also eliminates one of the more difficult challenges associated with development of radia-tion detection equipment.« less

Estimates of Radioxenon Released from Southern Hemisphere Medical isotope Production Facilities Using Measured Air Concentrations and Atmospheric Transport Modeling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Eslinger, Paul W.; Friese, Judah I.; Lowrey, Justin D.

2014-09-01

Abstract The International Monitoring System (IMS) of the Comprehensive-Nuclear-Test-Ban-Treaty monitors the atmosphere for radioactive xenon leaking from underground nuclear explosions. Emissions from medical isotope production represent a challenging background signal when determining whether measured radioxenon in the atmosphere is associated with a nuclear explosion prohibited by the treaty. The Australian Nuclear Science and Technology Organisation (ANSTO) operates a reactor and medical isotope production facility in Lucas Heights, Australia. This study uses two years of release data from the ANSTO medical isotope production facility and Xe-133 data from three IMS sampling locations to estimate the annual releases of Xe-133 from medicalmore » isotope production facilities in Argentina, South Africa, and Indonesia. Atmospheric dilution factors derived from a global atmospheric transport model were used in an optimization scheme to estimate annual release values by facility. The annual releases of about 6.8×1014 Bq from the ANSTO medical isotope production facility are in good agreement with the sampled concentrations at these three IMS sampling locations. Annual release estimates for the facility in South Africa vary from 1.2×1016 to 2.5×1016 Bq and estimates for the facility in Indonesia vary from 6.1×1013 to 3.6×1014 Bq. Although some releases from the facility in Argentina may reach these IMS sampling locations, the solution to the objective function is insensitive to the magnitude of those releases.« less

Osmium uptake, distribution, and 187Os/188Os and 187Re/188Os compositions in Phaeophyceae macroalgae, Fucus vesiculosus: Implications for determining the 187Os/188Os composition of seawater

NASA Astrophysics Data System (ADS)

Racionero-Gómez, B.; Sproson, A. D.; Selby, D.; Gannoun, A.; Gröcke, D. R.; Greenwell, H. C.; Burton, K. W.

2017-02-01

The osmium isotopic composition (187Os/188Os) of seawater reflects the balance of input from mantle-, continental- and anthropogenic-derived sources. This study utilizes the Phaeophyceae, Fucus vesiculosus, to analyse its Os abundance and uptake, as well as to assess if macroalgae records the Os isotope composition of the seawater in which it lives. The data demonstrates that Os is not located in one specific biological structure within macroalgae, but is found throughout the organism. Osmium uptake was measured by culturing F. vesiculosus non-fertile tips with different concentrations of Os with a known 187Os/188Os composition (∼0.16), which is significantly different from the background isotopic composition of local seawater (∼0.94). The Os abundance of cultured non-fertile tips show a positive correlation to the concentration of the Os doped seawater. Moreover, the 187Os/188Os composition of the seaweed equalled that of the culture medium, strongly confirming the possible use of macroalgae as a biological proxy for the Os isotopic composition of the seawater.

An optimized method for measuring fatty acids and cholesterol in stable isotope-labeled cells

PubMed Central

Argus, Joseph P.; Yu, Amy K.; Wang, Eric S.; Williams, Kevin J.; Bensinger, Steven J.

2017-01-01

Stable isotope labeling has become an important methodology for determining lipid metabolic parameters of normal and neoplastic cells. Conventional methods for fatty acid and cholesterol analysis have one or more issues that limit their utility for in vitro stable isotope-labeling studies. To address this, we developed a method optimized for measuring both fatty acids and cholesterol from small numbers of stable isotope-labeled cultured cells. We demonstrate quantitative derivatization and extraction of fatty acids from a wide range of lipid classes using this approach. Importantly, cholesterol is also recovered, albeit at a modestly lower yield, affording the opportunity to quantitate both cholesterol and fatty acids from the same sample. Although we find that background contamination can interfere with quantitation of certain fatty acids in low amounts of starting material, our data indicate that this optimized method can be used to accurately measure mass isotopomer distributions for cholesterol and many fatty acids isolated from small numbers of cultured cells. Application of this method will facilitate acquisition of lipid parameters required for quantifying flux and provide a better understanding of how lipid metabolism influences cellular function. PMID:27974366

Ultra low-level measurements of actinides by sector field ICP-MS.

PubMed

Pointurier, F; Baglan, N; Hémet, P

2004-01-01

In the present work, a double-focusing sector field inductively coupled plasma-mass spectrometer was optimised for ultra trace and isotopic analyses of actinide long-lived isotopes in low concentration solutions of the fgml(-1) to the ngml(-1) range. Sensitivities of about 3GHz/(microgml(-1)), with as low a background as 0.1cps, were obtained for U using a conventional concentric pneumatic nebuliser. Detection limits are below the fg range for 239Pu and 240Pu. With natural U, a precision lower than 0.5% RSD is currently obtained for 235U/238U isotopic ratio at the 200pgml(-1) level.

Laboratory studies on the removal of radon-born lead from KamLAND's organic liquid scintillator

NASA Astrophysics Data System (ADS)

Keefer, G.; Grant, C.; Piepke, A.; Ebihara, T.; Ikeda, H.; Kishimoto, Y.; Kibe, Y.; Koseki, Y.; Ogawa, M.; Shirai, J.; Takeuchi, S.; Mauger, C.; Zhang, C.; Schweitzer, G.; Berger, B. E.; Dazeley, S.; Decowski, M. P.; Detwiler, J. A.; Djurcic, Z.; Dwyer, D. A.; Efremenko, Y.; Enomoto, S.; Freedman, S. J.; Fujikawa, B. K.; Furuno, K.; Gando, A.; Gando, Y.; Gratta, G.; Hatakeyama, S.; Heeger, K. M.; Hsu, L.; Ichimura, K.; Inoue, K.; Iwamoto, T.; Kamyshkov, Y.; Karwowski, H. J.; Koga, M.; Kozlov, A.; Lane, C. E.; Learned, J. G.; Maricic, J.; Markoff, D. M.; Matsuno, S.; McKee, D.; McKeown, R. D.; Miletic, T.; Mitsui, T.; Motoki, M.; Nakajima, Kyo; Nakajima, Kyohei; Nakamura, K.; O`Donnell, T.; Ogawa, H.; Piquemal, F.; Ricol, J.-S.; Shimizu, I.; Suekane, F.; Suzuki, A.; Svoboda, R.; Tajima, O.; Takemoto, Y.; Tamae, K.; Tolich, K.; Tornow, W.; Watanabe, Hideki; Watanabe, Hiroko; Winslow, L. A.; Yoshida, S.

2015-01-01

The removal of radioactivity from liquid scintillator has been studied in preparation of a low background phase of KamLAND. This paper describes the methods and techniques developed to measure and efficiently extract radon decay products from liquid scintillator. We report the radio-isotope reduction factors obtained when applying various extraction methods. During this study, distillation was identified as the most efficient method for removing radon-born lead from liquid scintillator.

Laboratory studies on the removal of radon-born lead from KamLAND׳s organic liquid scintillator

DOE Office of Scientific and Technical Information (OSTI.GOV)

Keefer, G.; Grant, C.; Piepke, A.

We studied the removal of radioactivity from liquid scintillator in preparation of a low background phase of KamLAND. We describe the methods and techniques developed to measure and efficiently extract radon decay products from liquid scintillator. Lastly, we report the radio-isotope reduction factors obtained when applying various extraction methods. During this study, distillation was identified as the most efficient method for removing radon daughters from liquid scintillator.

Laboratory studies on the removal of radon-born lead from KamLAND׳s organic liquid scintillator

DOE PAGES

Keefer, G.; Grant, C.; Piepke, A.; ...

2014-09-28

We studied the removal of radioactivity from liquid scintillator in preparation of a low background phase of KamLAND. We describe the methods and techniques developed to measure and efficiently extract radon decay products from liquid scintillator. Lastly, we report the radio-isotope reduction factors obtained when applying various extraction methods. During this study, distillation was identified as the most efficient method for removing radon daughters from liquid scintillator.

Factors controlling precision and accuracy in isotope-ratio-monitoring mass spectrometry

NASA Technical Reports Server (NTRS)

Merritt, D. A.; Hayes, J. M.

1994-01-01

The performance of systems in which picomole quantities of sample are mixed with a carrier gas and passed through an isotope-ratio mass spectrometer system was examined experimentally and theoretically. Two different mass spectrometers were used, both having electron-impact ion sources and Faraday cup collector systems. One had an accelerating potential of 10kV and accepted 0.2 mL of He/min, producing, under those conditions, a maximum efficiency of 1 CO2 molecular ion collected per 700 molecules introduced. Comparable figures for the second instrument were 3 kV, 0.5 mL of He/min, and 14000 molecules/ion. Signal pathways were adjusted so that response times were <200 ms. Sample-related ion currents appeared as peaks with widths of 3-30 s. Isotope ratios were determined by comparison to signals produced by standard gases. In spite of rapid variations in signals, observed levels of performance were within a factor of 2 of shot-noise limits. For the 10-kV instrument, sample requirements for standard deviations of 0.1 and 0.5% were 45 and 1.7 pmol, respectively. Comparable requirements for the 3-kV instrument were 900 and 36 pmol. Drifts in instrumental characteristics were adequately neutralized when standards were observed at 20-min intervals. For the 10-kV instrument, computed isotopic compositions were independent of sample size and signal strength over the ranges examined. Nonlinearities of <0.04%/V were observed for the 3-kV system. Procedures for observation and subtraction of background ion currents were examined experimentally and theoretically. For sample/ background ratios varying from >10 to 0.3, precision is expected and observed to decrease approximately 2-fold and to depend only weakly on the precision with which background ion currents have been measured.

Stable Isotope Biogeochemistry of Seabird Guano Fertilization: Results from Growth Chamber Studies with Maize (Zea Mays)

PubMed Central

Szpak, Paul; Longstaffe, Fred J.; Millaire, Jean-François; White, Christine D.

2012-01-01

Background Stable isotope analysis is being utilized with increasing regularity to examine a wide range of issues (diet, habitat use, migration) in ecology, geology, archaeology, and related disciplines. A crucial component to these studies is a thorough understanding of the range and causes of baseline isotopic variation, which is relatively poorly understood for nitrogen (δ15N). Animal excrement is known to impact plant δ15N values, but the effects of seabird guano have not been systematically studied from an agricultural or horticultural standpoint. Methodology/Principal Findings This paper presents isotopic (δ13C and δ15N) and vital data for maize (Zea mays) fertilized with Peruvian seabird guano under controlled conditions. The level of 15N enrichment in fertilized plants is very large, with δ15N values ranging between 25.5 and 44.7‰ depending on the tissue and amount of fertilizer applied; comparatively, control plant δ15N values ranged between −0.3 and 5.7‰. Intraplant and temporal variability in δ15N values were large, particularly for the guano-fertilized plants, which can be attributed to changes in the availability of guano-derived N over time, and the reliance of stored vs. absorbed N. Plant δ13C values were not significantly impacted by guano fertilization. High concentrations of seabird guano inhibited maize germination and maize growth. Moreover, high levels of seabird guano greatly impacted the N metabolism of the plants, resulting in significantly higher tissue N content, particularly in the stalk. Conclusions/Significance The results presented in this study demonstrate the very large impact of seabird guano on maize δ15N values. The use of seabird guano as a fertilizer can thus be traced using stable isotope analysis in food chemistry applications (certification of organic inputs). Furthermore, the fertilization of maize with seabird guano creates an isotopic signature very similar to a high-trophic level marine resource, which must be considered when interpreting isotopic data from archaeological material. PMID:22479435

New on-line method for water isotope analysis of speleothem fluid inclusions using laser absorption spectroscopy (WS-CRDS)

NASA Astrophysics Data System (ADS)

Affolter, S.; Fleitmann, D.; Leuenberger, M.

2014-01-01

A new online method to analyse water isotopes of speleothem fluid inclusions using a wavelength scanned cavity ring down spectroscopy (WS-CRDS) instrument is presented. This novel technique allows us to simultaneously measure hydrogen and oxygen isotopes for a released aliquot of water. To do so, we designed a new simple line that allows the on-line water extraction and isotope analysis of speleothem samples. The specificity of the method lies in the fact that fluid inclusions release is made on a standard water background, which mainly improves the δD reliability. To saturate the line, a peristaltic pump continuously injects standard water into the line that is permanently heated to 140 °C and flushed with dry nitrogen gas. This permits instantaneous and complete vaporisation of the standard water resulting in an artificial water background with well-known δD and δ18O values. The speleothem sample is placed into a copper tube, attached to the line and after system stabilisation is crushed using a simple hydraulic device to liberate speleothem fluid inclusions water. The released water is carried by the nitrogen/standard water gas stream directly to a Picarro L1102-i for isotope determination. To test the accuracy and reproducibility of the line and to measure standard water during speleothem measurements a syringe injection unit was added to the line. Peak evaluation is done similarly as in gas chromatography to obtain δD and δ18O isotopic composition of measured water aliquots. Precision is better than 1.5‰ for δD and 0.4‰ for δ18O for water measurement for an extended range (-210 to 0‰ for δD and -27 to 0‰ for δ18O) primarily dependent on the amount of water released from speleothem fluid inclusions and secondarily on the isotopic composition of the sample. The results show that WS-CRDS technology is suitable for speleothem fluid inclusion measurements and gives results that are comparable to Isotope Ratio Mass Spectrometry (IRMS) technique.

New online method for water isotope analysis of speleothem fluid inclusions using laser absorption spectroscopy (WS-CRDS)

NASA Astrophysics Data System (ADS)

Affolter, S.; Fleitmann, D.; Leuenberger, M.

2014-07-01

A new online method to analyse water isotopes of speleothem fluid inclusions using a wavelength scanned cavity ring down spectroscopy (WS-CRDS) instrument is presented. This novel technique allows us simultaneously to measure hydrogen and oxygen isotopes for a released aliquot of water. To do so, we designed a new simple line that allows the online water extraction and isotope analysis of speleothem samples. The specificity of the method lies in the fact that fluid inclusions release is made on a standard water background, which mainly improves the δ D robustness. To saturate the line, a peristaltic pump continuously injects standard water into the line that is permanently heated to 140 °C and flushed with dry nitrogen gas. This permits instantaneous and complete vaporisation of the standard water, resulting in an artificial water background with well-known δ D and δ18O values. The speleothem sample is placed in a copper tube, attached to the line, and after system stabilisation it is crushed using a simple hydraulic device to liberate speleothem fluid inclusions water. The released water is carried by the nitrogen/standard water gas stream directly to a Picarro L1102-i for isotope determination. To test the accuracy and reproducibility of the line and to measure standard water during speleothem measurements, a syringe injection unit was added to the line. Peak evaluation is done similarly as in gas chromatography to obtain &delta D; and δ18O isotopic compositions of measured water aliquots. Precision is better than 1.5 ‰ for δ D and 0.4 ‰ for δ18O for water measurements for an extended range (-210 to 0 ‰ for δ D and -27 to 0 ‰ for δ18O) primarily dependent on the amount of water released from speleothem fluid inclusions and secondarily on the isotopic composition of the sample. The results show that WS-CRDS technology is suitable for speleothem fluid inclusion measurements and gives results that are comparable to the isotope ratio mass spectrometry (IRMS) technique.

Wavelet signatures of K-splitting of the Isoscalar Giant Quadrupole Resonance in deformed nuclei from high-resolution (p,p‧) scattering off 146, 148, 150Nd

NASA Astrophysics Data System (ADS)

Kureba, C. O.; Buthelezi, Z.; Carter, J.; Cooper, G. R. J.; Fearick, R. W.; Förtsch, S. V.; Jingo, M.; Kleinig, W.; Krugmann, A.; Krumbolz, A. M.; Kvasil, J.; Mabiala, J.; Mira, J. P.; Nesterenko, V. O.; von Neumann-Cosel, P.; Neveling, R.; Papka, P.; Reinhard, P.-G.; Richter, A.; Sideras-Haddad, E.; Smit, F. D.; Steyn, G. F.; Swartz, J. A.; Tamii, A.; Usman, I. T.

2018-04-01

The phenomenon of fine structure of the Isoscalar Giant Quadrupole Resonance (ISGQR) has been studied with high energy-resolution proton inelastic scattering at iThemba LABS in the chain of stable even-mass Nd isotopes covering the transition from spherical to deformed ground states. A wavelet analysis of the background-subtracted spectra in the deformed 146, 148, 150Nd isotopes reveals characteristic scales in correspondence with scales obtained from a Skyrme RPA calculation using the SVmas10 parameterization. A semblance analysis shows that these scales arise from the energy shift between the main fragments of the K = 0 , 1 and K = 2 components.

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

NASA Technical Reports Server (NTRS)

Freeman, K. H.; Ricci, S. A.; Studley, A.; Hayes, J. M.

1989-01-01

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

High-precision gamma-ray spectroscopy of 82Rb and 72As, two important medical isotopes used in positron emission tomography

NASA Astrophysics Data System (ADS)

Nino, Michael; McCutchan, E.; Smith, S.; Sonzogni, A.; Muench, L.; Greene, J.; Carpenter, M.; Zhu, S.; Lister, C.

2015-10-01

Both 82Rb and 72As are very important medical isotopes used in imaging procedures, yet their full decay schemes were last studied decades ago using low-sensitivity detection systems; high quality decay data is necessary to determine the total dose received by the patient, the background in imaging technologies, and shielding requirements in production facilities. To improve the decay data of these two isotopes, sources were produced at the Brookhaven Linac Isotope Producer (BLIP) and then the Gammasphere array, consisting of 89 Compton-suppressed HPGe detectors, at Argonne National Laboratory was used to analyze the gamma-ray emissions from the daughter nuclei 82 Kr and 72 Ge. Gamma-ray singles and coincidence information were recorded and analyzed using Radware Gf3m software. Significant revisions were made to the level schemes including the observation of many new transitions and levels as well as a reduction in uncertainty on measured γ-ray intensities and deduced β-feedings. The new decay schemes as well as their impact on dose calculations will be presented. DOE Isotope Program is acknowledged for funding ST5001030. Work supported by the U.S. DOE under Grant No. DE-FG02-94ER40848 and Contract Nos. DE-AC02-98CH10946 and DE-AC02-06CH11357 and by the Science Undergraduate Laboratory Internships Program (SULI).

Application Of Stable Isotope Analysis To Study Temporal Changes In Foraging Ecology In A Highly Endangered Amphibian

PubMed Central

Gillespie, J. Hayley

2013-01-01

Background Understanding dietary trends for endangered species may be essential to assessing the effects of ecological disturbances such as habitat modification, species introductions or global climate change. Documenting temporal variation in prey selection may also be crucial for understanding population dynamics. However, the rarity, secretive behaviours and obscure microhabitats of some endangered species can make direct foraging observations difficult or impossible. Furthermore, the lethality or invasiveness of some traditional methods of dietary analysis (e.g. gut contents analysis, gastric lavage) makes them inappropriate for such species. Stable isotope analysis facilitates non-lethal, indirect analysis of animal diet that has unrealized potential in the conservation of endangered organisms, particularly amphibians. Methodology/findings I determined proportional contributions of aquatic macroinvertebrate prey to the diet of an endangered aquatic salamander Eurycea sosorum over a two-year period using stable isotope analysis of 13/12C and 15/14N and the Bayesian stable isotope mixing model SIAR. I calculated Strauss’ dietary electivity indices by comparing these proportions with changing relative abundance of potential prey species through time. Stable isotope analyses revealed that a previously unknown prey item (soft-bodied planarian flatworms in the genus Dugesia) made up the majority of E. sosorum diet. Results also demonstrate that E. sosorum is an opportunistic forager capable of diet switching to include a greater proportion of alternative prey when Dugesia populations decline. There is also evidence of intra-population dietary variation. Conclusions/significance Effective application of stable isotope analysis can help circumvent two key limitations commonly experienced by researchers of endangered species: the inability to directly observe these species in nature and the invasiveness or lethality of traditional methods of dietary analysis. This study illustrates the feasibility of stable isotope analysis in identifying preferred prey species that can be used to guide conservation management of both wild and captive food sources for endangered species. PMID:23341920

A 220Rn source for the calibration of low-background experiments

NASA Astrophysics Data System (ADS)

Lang, R. F.; Brown, A.; Brown, E.; Cervantes, M.; Macmullin, S.; Masson, D.; Schreiner, J.; Simgen, H.

2016-04-01

We characterize two 40 kBq sources of electrodeposited 228Th for use in low-background experiments. The sources efficiently emanate 220Rn, a noble gas that can diffuse in a detector volume. 220Rn and its daughter isotopes produce α-, β-, and γ-radiation, which may used to calibrate a variety of detector responses and features, before decaying completely in only a few days. We perform various tests to place limits on the release of other long-lived isotopes. In particular, we find an emanation of < 0.008 atoms/min/kBq (90% CL) for 228Th and (1.53 ± 0.04) atoms/min/kBq for 224Ra. The sources lend themselves in particular to the calibration of detectors employing liquid noble elements such as argon and xenon. With the source mounted in a noble gas system, we demonstrate that filters are highly efficient in reducing the activity of these longer-lived isotopes further. We thus confirm the suitability of these sources even for use in next-generation experiments, such as XENON1T/XENONnT, LZ, and nEXO.

Reliable determination of oxygen and hydrogen isotope ratios in atmospheric water vapour adsorbed on 3A molecular sieve.

PubMed

Han, Liang-Feng; Gröning, Manfred; Aggarwal, Pradeep; Helliker, Brent R

2006-01-01

The isotope ratio of atmospheric water vapour is determined by wide-ranging feedback effects from the isotope ratio of water in biological water pools, soil surface horizons, open water bodies and precipitation. Accurate determination of atmospheric water vapour isotope ratios is important for a broad range of research areas from leaf-scale to global-scale isotope studies. In spite of the importance of stable isotopic measurements of atmospheric water vapour, there is a paucity of published data available, largely because of the requirement for liquid nitrogen or dry ice for quantitative trapping of water vapour. We report results from a non-cryogenic method for quantitatively trapping atmospheric water vapour using 3A molecular sieve, although water is removed from the column using standard cryogenic methods. The molecular sieve column was conditioned with water of a known isotope ratio to 'set' the background signature of the molecular sieve. Two separate prototypes were developed, one for large collection volumes (3 mL) and one for small collection volumes (90 microL). Atmospheric water vapour was adsorbed to the column by pulling air through the column for several days to reach the desired final volume. Water was recovered from the column by baking at 250 degrees C in a dry helium or nitrogen air stream and cryogenically trapped. For the large-volume apparatus, the recovered water differed from water that was simultaneously trapped by liquid nitrogen (the experimental control) by 2.6 per thousand with a standard deviation (SD) of 1.5 per thousand for delta(2)H and by 0.3 per thousand with a SD of 0.2 per thousand for delta(18)O. Water-vapour recovery was not satisfactory for the small volume apparatus. Copyright (c) 2006 John Wiley & Sons, Ltd.

ForCent model development and testing using the Enriched Background Isotope Study experiment

Treesearch

William J. Parton; Paul J. Hanson; Chris Swanston; Margaret Torn; Susan E. Trumbore; William Riley; Robin Kelly

2010-01-01

The ForCent forest ecosystem model was developed by making major revisions to the DayCent model including: (1) adding a humus organic pool, (2) incorporating a detailed root growth model, and (3) including plant phenological growth patterns. Observed plant production and soil respiration data from 1993 to 2000 were used to demonstrate that the ForCent model could...

River recharge sources and the partitioning of catchment evapotranspiration fluxes as revealed by stable isotope signals in a typical high-elevation arid catchment

NASA Astrophysics Data System (ADS)

Guo, Xiaoyu; Tian, Lide; Wang, Lei; Yu, Wusheng; Qu, Dongmei

2017-06-01

Catchment-scale hydrological cycles are expected to suffer more extremes under a background of climate change. Quantifying hydrological changes in high and remote areas is practically challenging. However, stable isotopes in river water can be seen to vary, dependent upon the combined influence exerted by recharge sources and local climatic conditions; the study of river water stable isotopes can therefore provide a meaningful method for delineating catchment-scale hydrological studies. In this study, we present high-resolution time series of river δ18O and d-excess values; additionally, we identify the seasonal dynamics of river recharge sources and major components of the catchment-scale water balance, together with precipitation and groundwater isotopes, and concurrent meteorological data recorded in Magazangbu catchment on the northwestern Tibetan Plateau (TP). Using isotopic analysis, and within a proportional framework, we partitioned the isotopic fractionation (E1) or non-fractionation (E2) from soil evaporation fluxes (Esoil) apparent in different processes, using NDVI (Normal Differential Vegetation Index) data collected by MODIS satellites to calculate the vegetation fractional coverage (VFC), and Global Land Data Assimilation System (GLDAS) records to determine evapotranspiration data (ET). Finally, the contributions made by each ET component (Esoil and plant transpiration) to total catchment ET were computed for the high and remote northwestern TP. Our results show that: (1) river δ18O values were high in summer and low in winter, while d-excess values displayed a contrary seasonal cycle; (2) for the monsoon period, precipitation contributed 60.6% to Magazangbu catchment runoff. Deeper groundwater was the main water source for the winter low base flow, and shallow groundwater or high elevation snowmelt was the principal component of the spring thaw and autumn freezing periods; and (3) a substantial proportion of Esoil (96.4% annually; 92.2% during monsoon) was consumed without isotopic fractionation (E2); plant transpiration (T) constituted less than half of total ET (41% annually, 29% during monsoon) in Magazangbu catchment. This calculation of river recharge sources and partitioning of catchment ET components using isotopic signals and MODIS NDVI data or GLDAS ET data provide new methods for hydrological studies in high and remote areas. These results provide important catchment-scale water-balance information which is very useful to climate models conducted in a high-elevation arid environment.

Isotopic reconstruction of ancient human migrations: A comprehensive Sr isotope reference database for France and the first case study at Tumulus de Sables, south-western France

NASA Astrophysics Data System (ADS)

Willmes, M.; Boel, C.; Grün, R.; Armstrong, R.; Chancerel, A.; Maureille, B.; Courtaud, P.

2012-04-01

Strontium isotope ratios (87Sr/86Sr) can be used for the reconstruction of human and animal migrations across geologically different terrains. Sr isotope ratios in rocks are a product of age and composition and thus vary between geologic units. From the eroding environment Sr is transported into the soils, plants and rivers of a region. Humans and animals incorporate Sr from their diet into their bones and teeth, where it substitutes for calcium. Tooth enamel contains Sr isotope signatures acquired during childhood and is most resistant to weathering and overprinting, while the dentine is often diagenetically altered towards the local Sr signature. For the reconstruction of human and animal migrations the tooth enamel 87Sr/86Sr ratio is compared to the Sr isotope signature in the vicinity of the burial site and the surrounding area. This study focuses on the establishment of a comprehensive reference map of bioavailable 87Sr/86Sr ratios for France. In a next step we will compare human and animal teeth from key archaeological sites to this reference map to investigate mobility. So far, we have analysed plant and soil samples from ~200 locations across France including the Aquitaine basin, the western and northern parts of the Paris basin, as well as three transects through the Pyrenees Mountains. The isotope data, geologic background information (BRGM 1:1M), field images, and detailed method descriptions are available through our online database iRhum (http://rses.anu.edu.au/research/ee). This database can also be used in forensic studies and food sciences. As an archaeological case study teeth from 16 adult and 8 juvenile individuals were investigated from an early Bell Beaker (2500-2000 BC) site at Le Tumulus des Sables, south-west France (Gironde). The teeth were analysed for Sr isotope ratios using laser ablation ICP-MS. Four teeth were also analysed using solution ICP-MS, which showed a significant offset to the laser ablation results. This requires further detailed investigation. Nevertheless, the teeth showed clear differences between enamel and diagenetically overprinted dentine, which suggests mobility. Unfortunately, the sandy sediment units in the close vicinity of Le Tumulus des Sables show large variations in their 87Sr/86Sr ratios so it is currently not possible to distinguish between migration from outside of the Médoc region from mobility within the region based solely on Sr isotope ratios. The case study illustrates the importance of detailed reference maps, which are required for any isotope studies used for the reconstruction of migrations. Other isotope data, such as O and Pb, will complement the investigation at Tumulus de Sables and may enable us to tie down the range of mobility of the humans that were buried at Le Tumulus des Sables.

Background reduction in 236U/238U measurements

NASA Astrophysics Data System (ADS)

Buompane, Raffaele; De Cesare, Mario; De Cesare, Nicola; Di Leva, Antonino; D'Onofrio, Antonio; Fifield, L. Keith; Fröhlich, Michaela; Gialanella, Lucio; Marzaioli, Fabio; Sabbarese, Carlo; Terrasi, Filippo; Tims, Stephen; Wallner, Anton

2015-10-01

The measurements of actinide isotopic ratios, in particular 236U/238U, in environmental samples requires high sensitivity. In particular, special effort must be devoted to the suppression of interfering nuclides, such as 235,238U, when measuring 236U. At the AMS facility of CIRCE, isotopic ratios down to ∼10-10 are currently measured using a gas E - ΔE detector. In order to push this limit lower towards natural levels, a time-of-flight system is used, featuring a micro-channel plate start detector and a Si stop detector. As the mass resolution of the latter is limited by the layout, an attempt to reduce the abundant isotope interference by other means has been undertaken. In this study, we report preliminary results on the characterization of the presence of molecular interferences when using UO-, UC- and UC2- as injected molecular ions. In particular the possibility to stabilize the current yield from carbide cathodes has been investigated: it was found that the best cathode preparation procedure is obtained pressing U salts baked at 800 °C mixed with graphite and Al powder. Moreover, the 238U background in 236U measurements is strongly reduced injecting UC- ions, as verified using a time-of-flight detection system. On the other hand, 235U interference is larger with respect to UO- injection, but this increase is smaller than expected on the basis of abundances of 13C and 17O in UC and UC2 molecules on one side and UO, on the other.

Analysis of a global database containing tritium in precipitation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Buckley, R. L.; Rabun, R. L.; Heath, M.

The International Atomic Energy Agency (IAEA) directed the collection of tritium in water samples from the mid-1950s to 2009. The Global Network of Isotopes in Precipitation (GNIP) data examined the airborne movement of isotope releases to the environment, with an objective of collecting spatial data on the isotope content of precipitation across the globe. The initial motivation was to monitor atmospheric thermonuclear test fallout through tritium, deuterium, and oxygen isotope concentrations, but after the 1970s the focus changed to being an observation network of stable hydrogen and oxygen isotope data for hydrologic studies. The GNIP database provides a wealth ofmore » tritium data collections over a long period of time. The work performed here primarily examined data features in the past 30 years (after much of the effects of above-ground nuclear testing in the late 1950s to early 1960s decayed away), revealing potentially unknown tritium sources. The available data at GNIP were reorganized to allow for evaluation of trends in the data both temporally and spatially. Several interesting cases were revealed, including relatively high measured concentrations in the Atlantic and Indian Oceans, Russia, Norway, as well as an increase in background concentration at a collector in South Korea after 2004. Recent data from stations in the southeastern United States nearest to the Savannah River Site do not indicate any high values. Meteorological impacts have not been considered in this study. Further research to assess the likely source location of interesting cases using transport simulations and/or literature searches is warranted.« less

Concomitant Ion Effects on Isotope Ratio Measurements with Liquid Sampling – Atmospheric Pressure Glow Discharge Ion Source Orbitrap Mass Spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoegg, Edward D.; Marcus, R. Kenneth; Hager, Georg

2018-02-28

In an effort to understand and improve the accuracy and precision of the liquid sampling- atmospheric pressure glow discharge (LS-APGD)/Orbitrap system, effects of concomitant ions on the acquired mass spectra are examined and presented. The LS-APGD/ Orbitrap instrument system is capable of high quality isotope ratio measurements, which are of high analytical interest for nuclear non-proliferation detection applications. The presence of background and concomitant ions (water clusters, matrix, and other analytes) has presented limitations in earlier studies. In order to mitigate these effects, an alternative quadrupole-Orbitrap hybrid mass spectrometer was employed in this study. This instrument configuration has a quadrupolemore » mass filter preceding the Orbitrap to filter-out undesired non-analyte ions. Results are presented for the analysis of U in the presence of Rb, Ag, Ba, and Pb as concomitants, each present at 5 µg/mL concentration. Progressive filtering of each concomitant ion shows steadily improved U isotope ratio performance. Ultimately, a 235U/238U ratio of 0.007133, with a relative accuracy of -2.1% and a relative standard deviation of 0.087% was achieved using this system, along with improved calibration linearity and lowered limits of detection. The resultant performance compares very favorably with other commonly accepted isotope ratio measurement platforms - surprisingly so for an ion trap type mass spectrometry instrument.« less

Study of medical isotope production facility stack emissions and noble gas isotopic signature using automatic gamma-spectra analysis platform

NASA Astrophysics Data System (ADS)

Zhang, Weihua; Hoffmann, Emmy; Ungar, Kurt; Dolinar, George; Miley, Harry; Mekarski, Pawel; Schrom, Brian; Hoffman, Ian; Lawrie, Ryan; Loosz, Tom

2013-04-01

The nuclear industry emissions of the four CTBT (Comprehensive Nuclear-Test-Ban Treaty) relevant radioxenon isotopes are unavoidably detected by the IMS along with possible treaty violations. Another civil source of radioxenon emissions which contributes to the global background is radiopharmaceutical production companies. To better understand the source terms of these background emissions, a joint project between HC, ANSTO, PNNL and CRL was formed to install real-time detection systems to support 135Xe, 133Xe, 131mXe and 133mXe measurements at the ANSTO and CRL 99Mo production facility stacks as well as the CANDU (CANada Deuterium Uranium) primary coolant monitoring system at CRL. At each site, high resolution gamma spectra were collected every 15 minutes using a HPGe detector to continuously monitor a bypass feed from the stack or CANDU primary coolant system as it passed through a sampling cell. HC also conducted atmospheric monitoring for radioxenon at approximately 200 km distant from CRL. A program was written to transfer each spectrum into a text file format suitable for the automatic gamma-spectra analysis platform and then email the file to a server. Once the email was received by the server, it was automatically analysed with the gamma-spectrum software UniSampo/Shaman to perform radionuclide identification and activity calculation for a large number of gamma-spectra in a short period of time (less than 10 seconds per spectrum). The results of nuclide activity together with other spectrum parameters were saved into the Linssi database. This database contains a large amount of radionuclide information which is a valuable resource for the analysis of radionuclide distribution within the noble gas fission product emissions. The results could be useful to identify the specific mechanisms of the activity release. The isotopic signatures of the various radioxenon species can be determined as a function of release time. Comparison of 133mXe and 133Xe activity ratios showed distinct differences between the closed CANDU primary coolant system and radiopharmaceutical production releases. According to the concept proposed by Kalinowski and Pistner (2006), the relationship between different isotopic activity ratios based on three or four radioxenon isotopes was plotted in a log-log diagram for source characterisation (civil vs. nuclear test). The multiple isotopic activity ratios were distributed in three distinct areas: HC atmospheric monitoring ratios extended to far left; the CANDU primary coolant system ratios lay in the middle; and 99Mo stack monitoring ratios for ANSTO and CRL were located on the right. The closed CANDU primary coolant has the lowest logarithmic mean ratio that represents the nuclear power reactor operation. The HC atmospheric monitoring exhibited a broad range of ratios spreading over several orders of magnitude. In contrast, the ANSTO and CRL stack emissions showed the smallest range of ratios but the results indicate at least two processes involved in the 99Mo productions. Overall, most measurements were found to be shifted towards the reactor domain. The hypothesis is that this is due to an accumulation of the isotope 131mXe in the stack or atmospheric background as it has the longest half-life and extra 131mXe emissions from the decay of 131I. The contribution of older 131mXe to a fresh release shifts the ratio of 133mXe/131mXe to the left. It was also very interesting to note that there were some situations where isotopic ratios from 99Mo production emissions fell within the nuclear test domain. This is due to operational variability, such as shorter target irradiation times. Martin B. Kalinowski and Christoph Pistner, (2006), Isotopic signature of atmospheric xenon released from light water reactors, Journal of Environmental Radioactivity, 88, 215-235.

Passive sampling for the isotopic fingerprinting of atmospheric mercury

NASA Astrophysics Data System (ADS)

Bergquist, B. A.; MacLagan, D.; Spoznar, N.; Kaplan, R.; Chandan, P.; Stupple, G.; Zimmerman, L.; Wania, F.; Mitchell, C. P. J.; Steffen, A.; Monaci, F.; Derry, L. A.

2017-12-01

Recent studies show that there are variations in the mercury (Hg) isotopic signature of atmospheric Hg, which demonstrates the potential for source tracing and improved understanding of atmospheric cycling of Hg. However, current methods for both measuring atmospheric Hg and collecting enough atmospheric Hg for isotopic analyses require expensive instruments that need power and expertise. Additionally, methods for collecting enough atmospheric Hg for isotopic analysis require pumping air through traps for long periods (weeks and longer). Combining a new passive atmospheric sampler for mercury (Hg) with novel Hg isotopic analyses will allow for the application of stable Hg isotopes to atmospheric studies of Hg. Our group has been testing a new passive sampler for gaseous Hg that relies on the diffusion of Hg through a diffusive barrier and adsorption onto a sulphur-impregnated activated carbon sorbent. The benefit of this passive sampler is that it is low cost, requires no power, and collects gaseous Hg for up to one year with linear, well-defined uptake, which allows for reproducible and accurate measurements of atmospheric gaseous Hg concentrations ( 8% uncertainty). As little as one month of sampling is often adequate to collect sufficient Hg for isotopic analysis at typical background concentrations. Experiments comparing the isotopic Hg signature in activated carbon samples using different approaches (i.e. by passive diffusion, by passive diffusion through diffusive barriers of different thickness, by active pumping) and at different temperatures confirm that the sampling process itself does not impose mass-independent fractionation (MIF). However, sampling does result in a consistent and thus correctable mass-dependent fractionation (MDF) effect. Therefore, the sampler preserves Hg MIF with very high accuracy and precision, which is necessary for atmospheric source tracing, and reasonable MDF can be estimated with some increase in error. In addition to experimental work, initial field data will be presented including a transect of increasing distance from a known strong source of Hg (Mt. Amiata mine, Italy), downwind of Kilauea volcano in Hawaii, and several other locales including the Arctic station Alert and various sites across Ontario, Canada.

Preferential flow pathways revealed by field based stable isotope analysis of CO2 by mid-infrared laser spectroscopy

NASA Astrophysics Data System (ADS)

van Geldern, Robert; Nowak, Martin; Zimmer, Martin; Szizybalski, Alexandra; Myrttinen, Anssi; Barth, Johannes A. C.; Jost, Hj

2016-04-01

A newly developed and commercially available isotope ratio laser spectrometer for CO2 analyses has been tested during a 10-day field monitoring campaign at the Ketzin pilot site for CO2 storage in northern Germany. The laser instrument is based on tunable laser direct absorption in the mid-infrared. The instrument recorded a continuous 10-day carbon stable isotope data set with 30 minutes resolution directly on-site in a field-based laboratory container during a tracer experiment. To test the instruments performance and accuracy the monitoring campaign was accompanied by daily CO2 sampling for laboratory analyses with isotope ratio mass spectrometry (IRMS). The carbon stable isotope ratios measured by conventional IRMS technique and by the new mid-infrared laser spectrometer agree remarkably well within 2σ analytical precision (<0.3 ‰). This proves the capability of the new mid-infrared direct absorption technique to measure high precision and accurate real-time table isotope data directly in the field. The injected CO2 tracer had a distinct δ13C value that was largely different from the reservoir background value. The laser spectroscopy data revealed a prior to this study unknown, intensive dynamic with fast changing δ13C values. The arrival pattern of the tracer suggest that the observed fluctuations were probably caused by migration along separate and distinct preferential flow paths between injection well and observation well. The new technique might contribute to a better tracing of the migration of the underground CO2 plume and help to ensure the long-term integrity of the reservoir.

Shielding concepts for low-background proportional counter arrays in surface laboratories

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aalseth, Craig E.; Humble, Paul H.; Mace, Emily K.

2016-02-01

Development of ultra low background gas proportional counters has made the contribution from naturally occurring radioactive isotopes – primarily and activity in the uranium and thorium decay chains – inconsequential to instrumental sensitivity levels when measurements are performed in above ground surface laboratories. Simple lead shielding is enough to mitigate against gamma rays as gas proportional counters are already relatively insensitive to naturally occurring gamma radiation. The dominant background in these surface laboratory measurements using ultra low background gas proportional counters is due to cosmic ray generated muons, neutrons, and protons. Studies of measurements with ultra low background gas proportionalmore » counters in surface and underground laboratories as well as radiation transport Monte Carlo simulations suggest a preferred conceptual design to achieve the highest possible sensitivity from an array of low background gas proportional counters when operated in a surface laboratory. The basis for a low background gas proportional counter array and the preferred shielding configuration is reported, especially in relation to measurements of radioactive gases having low energy decays such as 37Ar.« less

Ammunition is the principal source of lead accumulated by California condors re-introduced to the wild.

PubMed

Church, Molly E; Gwiazda, Roberto; Risebrough, Robert W; Sorenson, Kelly; Chamberlain, C Page; Farry, Sean; Heinrich, William; Rideout, Bruce A; Smith, Donald R

2006-10-01

The endangered California Condor (Gymnogyps californianus) was reduced to a total population of 22 birds by the end of 1982. Their captive-bred descendants are now being released back into the wild in California, Arizona, and Baja California, where monitoring indicates they may accumulate lead to toxic levels. Fragments of ammunition in the carcasses of game animals such as deer, elk, and feral pigs not retrieved by hunters or in gut piles left in the field have been considered a plausible source of the lead, though little direct evidence is available to support this hypothesis. Here, we measured lead concentrations and isotope ratios in blood from 18 condors living in the wild in central California, in 8 pre-release birds, and in diet and ammunition samples to determine the importance of ammunition as a source of exposure. Blood lead levels in pre-release condors were low (average 27.7 ng/mL, SD 4.9 ng/ mL) and isotopically similar to dietary and background environmental lead in California. In contrast, blood lead levels in free-flying condors were substantially higher (average 246 ng/mL, SD 229 ng/mL) with lead isotopic compositions that approached or matched those of the lead ammunition. A two-endmember mixing model defined by the background 207Pb/206Pb ratio of representative condor diet samples (0.8346) and the upper 207Pb/206Pb ratio of the ammunition samples (0.8184) was able to account for the blood lead isotopic compositions in 20 out of the 26 live condors sampled in this study (i.e., 77%). Finally, lead in tissues and in a serially sampled growing feather recovered postmortem from a lead-poisoned condor in Arizona evidence acute exposure from an isotopically distinct lead source. Together, these data indicate that incidental ingestion of ammunition in carcasses of animals killed by hunters is the principal source of elevated lead exposure that threatens the recovery in the wild of this endangered species.

Evidencing lead deposition at the urban scale using "short-lived" isotopic signatures of the source term (Pb-Zn refinery)

NASA Astrophysics Data System (ADS)

Franssens, Matthias; Flament, Pascal; Deboudt, Karine; Weis, Dominique; Perdrix, Espéranza

2004-09-01

To demonstrate the ability of the lead isotope signature technique to evidence the spatial extent of an industrial Pb deposition plume at a local scale, dry deposition of lead in the urban environment of a Pb-Zn refinery was investigated, as a study case, using transient ("short-lived") isotopic signatures of the industrial source. Sampling campaigns were achieved in representative weather conditions, on an 8-h basis. Dry deposition rates measured downwind from refinery emissions (≈102-103 μg Pb m-2 h-1), cross-sectionally in a 3-5 km radius area around the plant, represent 10-100 times the urban background dry fallout, measured upwind, as well as fallout measured near other potential sources of anthropogenic Pb. The Pb-Zn refinery isotopic signature (approx. 1.100<206Pb/207Pb<1.135) is made identifiable, using the same set of Pb and Zn ores for 2 days before sampling and during field experiments, by agreement with the executive staff of the plant. This source signature is less radiogenic than signatures of urban background Pb aerosols (1.155<206Pb/207Pb<1.165) and minor sources of Pb aerosols (1.147<206Pb/207Pb<1.165). By a simple binary mixing model calculation, we established the extension of the industrial Pb deposition plume. Fifty to eighty percents of total lead settled by the dry deposition mode, 3-4 km away from the refinery, still have an industrial origin. That represents from 40 to 80 μg Pb m-2 h-1, in an area where the blood lead level exceeds 100 μg Pb l-1 for 30% of men and 12% of women living there. We demonstrate here that stable Pb isotope analysis is able to evidence the Pb dry deposition plume in stabilised aerodynamic conditions, using a short-lived source term, suggesting that this methodology is able to furnish valuable data to validate industrial Pb aerosols dispersion models, at the urban scale.

Field-based stable isotope analysis of carbon dioxide by mid-infrared laser spectroscopy for carbon capture and storage monitoring.

PubMed

van Geldern, Robert; Nowak, Martin E; Zimmer, Martin; Szizybalski, Alexandra; Myrttinen, Anssi; Barth, Johannes A C; Jost, Hans-Jürg

2014-12-16

A newly developed isotope ratio laser spectrometer for CO2 analyses has been tested during a tracer experiment at the Ketzin pilot site (northern Germany) for CO2 storage. For the experiment, 500 tons of CO2 from a natural CO2 reservoir was injected in supercritical state into the reservoir. The carbon stable isotope value (δ(13)C) of injected CO2 was significantly different from background values. In order to observe the breakthrough of the isotope tracer continuously, the new instruments were connected to a stainless steel riser tube that was installed in an observation well. The laser instrument is based on tunable laser direct absorption in the mid-infrared. The instrument recorded a continuous 10 day carbon stable isotope data set with 30 min resolution directly on-site in a field-based laboratory container during a tracer experiment. To test the instruments performance and accuracy the monitoring campaign was accompanied by daily CO2 sampling for laboratory analyses with isotope ratio mass spectrometry (IRMS). The carbon stable isotope ratios measured by conventional IRMS technique and by the new mid-infrared laser spectrometer agree remarkably well within analytical precision. This proves the capability of the new mid-infrared direct absorption technique to measure high precision and accurate real-time stable isotope data directly in the field. The laser spectroscopy data revealed for the first time a prior to this experiment unknown, intensive dynamic with fast changing δ(13)C values. The arrival pattern of the tracer suggest that the observed fluctuations were probably caused by migration along separate and distinct preferential flow paths between injection well and observation well. The short-term variances as observed in this study might have been missed during previous works that applied laboratory-based IRMS analysis. The new technique could contribute to a better tracing of the migration of the underground CO2 plume and help to ensure the long-term integrity of the reservoir.

Shell model description of heavy nuclei and abnormal collective motions

NASA Astrophysics Data System (ADS)

Qi, Chong

2018-05-01

In this contribution I present systematic calculations on the spectroscopy and electromagnetic transition properties of intermediate-mass and heavy nuclei around 100Sn and 208Pb. We employed the large-scale configuration interaction shell model approach with realistic interactions. Those nuclei are the longest isotopic chains that can be studied by the nuclear shell model. I will show that the yrast spectra of Te isotopes show a vibrational-like equally spaced pattern but the few known E2 transitions show rotational-like behaviour. These kinds of abnormal collective behaviors cannot be reproduced by standard collective models and provide excellent background to study the competition of single-particle and various collective degrees of freedom. Moreover, the calculated B(E2) values for neutron-deficient and heavier Te isotopes show contrasting different behaviours along the yrast line, which may be related to the enhanced neutron-proton correlation when approaching N=50. The deviations between theory and experiment concerning the energies and E2 transition properties of low-lying 0+ and 2+ excited states and isomeric states in those nuclei may provide a constraint on our understanding of nuclear deformation and intruder configuration in that region.

Joint Application of Concentrations and Isotopic Signatures to Investigate the Global Atmospheric Carbon Monoxide Budget: Inverse Modeling Approach

NASA Astrophysics Data System (ADS)

Park, K.; Emmons, L. K.; Mak, J. E.

2007-12-01

Carbon monoxide is not only an important component for determining the atmospheric oxidizing capacity but also a key trace gas in the atmospheric chemistry of the Earth's background environment. The global CO cycle and its change are closely related to both the change of CO mixing ratio and the change of source strength. Previously, to estimate the global CO budget, most top-down estimation techniques have been applied the concentrations of CO solely. Since CO from certain sources has a unique isotopic signature, its isotopes provide additional information to constrain its sources. Thus, coupling the concentration and isotope fraction information enables to tightly constrain CO flux by its sources and allows better estimations on the global CO budget. MOZART4 (Model for Ozone And Related chemical Tracers), a 3-D global chemical transport model developed at NCAR, MPI for meteorology and NOAA/GFDL and is used to simulate the global CO concentration and its isotopic signature. Also, a tracer version of MOZART4 which tagged for C16O and C18O from each region and each source was developed to see their contributions to the atmosphere efficiently. Based on the nine-year- simulation results we analyze the influences of each source of CO to the isotopic signature and the concentration. Especially, the evaluations are focused on the oxygen isotope of CO (δ18O), which has not been extensively studied yet. To validate the model performance, CO concentrations and isotopic signatures measured from MPI, NIWA and our lab are compared to the modeled results. The MOZART4 reproduced observational data fairly well; especially in mid to high latitude northern hemisphere. Bayesian inversion techniques have been used to estimate the global CO budget with combining observed and modeled CO concentration. However, previous studies show significant differences in their estimations on CO source strengths. Because, in addition to the CO mixing ratio, isotopic signatures are independent tracers that contain the source information, jointly applying the isotope and the concentration information is expected to provide more precise optimization results in CO budget estimation. Our accumulated long-term CO isotope measurement data contribute to having more confidence of the inversions as well. Besides the benefit of adding isotope data on the inverse modeling, a trait of each isotope of CO (oxygen and carbon isotope) contains another advantageous use in the top-down estimation of the CO budget. δ18O and δ13C has a distinctive isotopic signature on a specific source; combustion sources such as a fossil fuel use show clearly different values from other natural sources in the δ18O signatures and the methane source can be easily separated by using δ13C information. Therefore, inversions of the two major sources of CO respond with different sensitivity for the different isotopes. To maximize the strengths of using isotope data in the inverse modeling analysis, various coupling schemes combining [CO], δ18O and δ13C have been investigated to enhance the credibility of the CO budget optimization.

Joint Application of Concentrations and Isotopic Signatures to Investigate the Global Atmospheric Carbon Monoxide Budget: Inverse Modeling Approach

NASA Astrophysics Data System (ADS)

Park, K.; Mak, J. E.; Emmons, L. K.

2008-12-01

Carbon monoxide is not only an important component for determining the atmospheric oxidizing capacity but also a key trace gas in the atmospheric chemistry of the Earth's background environment. The global CO cycle and its change are closely related to both the change of CO mixing ratio and the change of source strength. Previously, to estimate the global CO budget, most top-down estimation techniques have been applied the concentrations of CO solely. Since CO from certain sources has a unique isotopic signature, its isotopes provide additional information to constrain its sources. Thus, coupling the concentration and isotope fraction information enables to tightly constrain CO flux by its sources and allows better estimations on the global CO budget. MOZART4 (Model for Ozone And Related chemical Tracers), a 3-D global chemical transport model developed at NCAR, MPI for meteorology and NOAA/GFDL and is used to simulate the global CO concentration and its isotopic signature. Also, a tracer version of MOZART4 which tagged for C16O and C18O from each region and each source was developed to see their contributions to the atmosphere efficiently. Based on the nine-year-simulation results we analyze the influences of each source of CO to the isotopic signature and the concentration. Especially, the evaluations are focused on the oxygen isotope of CO (δ18O), which has not been extensively studied yet. To validate the model performance, CO concentrations and isotopic signatures measured from MPI, NIWA and our lab are compared to the modeled results. The MOZART4 reproduced observational data fairly well; especially in mid to high latitude northern hemisphere. Bayesian inversion techniques have been used to estimate the global CO budget with combining observed and modeled CO concentration. However, previous studies show significant differences in their estimations on CO source strengths. Because, in addition to the CO mixing ratio, isotopic signatures are independent tracers that contain the source information, jointly applying the isotope and the concentration information is expected to provide more precise optimization results in CO budget estimation. Our accumulated long-term CO isotope measurement data contribute to having more confidence of the inversions as well. Besides the benefit of adding isotope data on the inverse modeling, a trait of each isotope of CO (oxygen and carbon isotope) contains another advantageous use in the top-down estimation of the CO budget. δ18O and δ13C has a distinctive isotopic signature on a specific source; combustion sources such as a fossil fuel use show clearly different values from other natural sources in the δ18O signatures and the methane source can be easily separated by using δ13C information. Therefore, inversions of the two major sources of CO respond with different sensitivity for the different isotopes. To maximize the strengths of using isotope data in the inverse modeling analysis, various coupling schemes combining [CO], δ18O and δ13C have been investigated to enhance the credibility of the CO budget optimization.

Identifying the origins of local atmospheric deposition in the steel industry basin of Luxembourg using the chemical and isotopic composition of the lichen Xanthoria parietina.

PubMed

Hissler, Christophe; Stille, Peter; Krein, Andreas; Geagea, Majdi Lahd; Perrone, Thierry; Probst, Jean-Luc; Hoffmann, Lucien

2008-11-01

Trace metal atmospheric contamination was assessed in one of the oldest European industrial sites of steel production situated in the southern part of the Grand-Duchy of Luxembourg. Using elemental ratios as well as Pb, Sr, and Nd isotopic compositions as tracers, we found preliminary results concerning the trace metal enrichment and the chemical/isotopic signatures of the most important emission sources using the lichen Xanthoria parietina sampled at 15 sites along a SW-NE transect. The concentrations of these elements decreased with increasing distance from the historical and actual steel-work areas. The combination of the different tracers (major elements, Rare Earth Element ratios, Pb, Sr and Nd isotopes) enabled us to distinguish between three principal sources: the historical steel production (old tailings corresponding to blast-furnace residues), the present steel production (industrial sites with arc electric furnace units) and the regional background (baseline) components. Other anthropogenic sources including a waste incinerator and major roads had only weak impacts on lichen chemistry and isotopic ratios. The correlation between the Sr and Nd isotope ratios indicated that the Sr-Nd isotope systems represented useful tools to trace atmospheric emissions of factories using scrap metal for steel production.

Isotopically constrained lead sources in fugitive dust from unsurfaced roads in the southeast Missouri mining district.

PubMed

Witt, Emitt C; Pribil, Michael J; Hogan, John P; Wronkiewicz, David J

2016-09-01

The isotopic composition of lead (Pb) in fugitive dust suspended by a vehicle from 13 unsurfaced roads in Missouri was measured to identify the source of Pb within an established long-term mining area. A three end-member model using (207)Pb/(206)Pb and concentration as tracers resulted in fugitive dust samples plotting in the mixing field of well characterized heterogeneous end members. End members selected for this investigation include the (207)Pb/(206)Pb for 1) a Pb-mixture representing mine tailings, 2) aerosol Pb-impacted soils within close proximity to the Buick secondary recycling smelter, and 3) an average of soils, rock cores and drill cuttings representing the background conditions. Aqua regia total concentrations and (207)Pb/(206)Pb of mining area dust suggest that 35.4-84.3% of the source Pb in dust is associated with the mine tailings mixture, 9.1-52.7% is associated with the smelter mixture, and 0-21.6% is associated with background materials. Isotope ratios varied minimally within the operational phases of sequential extraction suggesting that mixing of all three Pb mixtures occurs throughout. Labile forms of Pb were attributed to all three end members. The extractable carbonate phase had as much as 96.6% of the total concentration associated with mine tailings, 51.8% associated with smelter deposition, and 34.2% with background. The next most labile geochemical phase (Fe + Mn Oxides) showed similar results with as much as 85.3% associated with mine tailings, 56.8% associated with smelter deposition, and 4.2% associated with the background soil. Published by Elsevier Ltd.

Isotopically constrained lead sources in fugitive dust from unsurfaced roads in the southeast Missouri mining district

USGS Publications Warehouse

Witt, Emitt C.; Pribil, Michael; Hogan, John P; Wronkiewicz, David

2016-01-01

The isotopic composition of lead (Pb) in fugitive dust suspended by a vehicle from 13 unsurfaced roads in Missouri was measured to identify the source of Pb within an established long-term mining area. A three end-member model using 207Pb/206Pb and concentration as tracers resulted in fugitive dust samples plotting in the mixing field of well characterized heterogeneous end members. End members selected for this investigation include the 207Pb/206Pb for 1) a Pb-mixture representing mine tailings, 2) aerosol Pb-impacted soils within close proximity to the Buick secondary recycling smelter, and 3) an average of soils, rock cores and drill cuttings representing the background conditions. Aqua regia total concentrations and 207Pb/206Pb of mining area dust suggest that 35.4–84.3% of the source Pb in dust is associated with the mine tailings mixture, 9.1–52.7% is associated with the smelter mixture, and 0–21.6% is associated with background materials. Isotope ratios varied minimally within the operational phases of sequential extraction suggesting that mixing of all three Pb mixtures occurs throughout. Labile forms of Pb were attributed to all three end members. The extractable carbonate phase had as much as 96.6% of the total concentration associated with mine tailings, 51.8% associated with smelter deposition, and 34.2% with background. The next most labile geochemical phase (Fe + Mn Oxides) showed similar results with as much as 85.3% associated with mine tailings, 56.8% associated with smelter deposition, and 4.2% associated with the background soil.

Applications of the low-background gamma spectroscopy to the geographical origin of marine salts and prunes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Perrot, F.

The low background gamma spectroscopy has been applied to try to sign the geographical origin of the French atlantic marine salts and of the prunes from Agen. Most of the activity measurements have been done using low background Ge spectrometers located in Bordeaux. Results have shown that a clear signature exists in the case of the French atlantic salts using the 40K, 137Cs and 226Ra isotopes but not in the case of the prunes.

Novel and non-traditional use of stable isotope tracers to study metal bioavailability from natural particles

USGS Publications Warehouse

Croteau, Marie-Noële; Cain, Daniel J.; Fuller, Christopher C.

2013-01-01

We devised a novel tracing approach that involves enriching test organisms with a stable metal isotope of low natural abundance prior to characterizing metal bioavailability from natural inorganic particles. In addition to circumventing uncertainties associated with labeling natural particles and distinguishing background metals, the proposed "reverse labeling" technique overcomes many drawbacks inherent to using radioisotope tracers. Specifically, we chronically exposed freshwater snails (Lymnaea stagnalis) to synthetic water spiked with Cu that was 99.4% 65Cu to increase the relative abundance of 65Cu in the snail’s tissues from 32% to >80%. The isotopically enriched snails were then exposed to benthic algae mixed with Cu-bearing Fe–Al particles collected from the Animas River (Colorado), an acid mine drainage impacted river. We used 63Cu to trace Cu uptake from the natural particles and inferred their bioavailability from calculation of Cu assimilation into tissues. Cu assimilation from these particles was 44%, indicating that 44% of the particulate Cu was absorbed by the invertebrate. This demonstrates that inorganic particulate Cu can be bioavailable. The reverse labeling approach shows great potential in various scientific areas such as environmental contamination and nutrition for addressing questions involving uptake of an element that naturally has multiple isotopes.

Characteristics of Heavy Metals and Pb Isotopic Composition in Sediments Collected from the Tributaries in Three Gorges Reservoir, China

PubMed Central

Gao, Bo; Zhou, Huaidong; Huang, Yong; Wang, Yuchun; Gao, Jijun; Liu, Xiaobo

2014-01-01

The concentrations, distribution, accumulation, and potential ecological risk of heavy metals (Cr, Cu, Zn, Ni, As, Pb, Cd, and Hg) in sediments from the Three Gorges Reservoir (TGR) tributaries were determined and studied. Pb isotopic compositions in sediments were also measured to effectively identify the potential Pb sources. The results showed that the average concentrations of heavy metals in sediment of TGR tributaries were higher than the local background values of soils and sediments in China. The assessment by Geoaccumulation Index indicated that Cu, Ni, and Hg were at the “slightly polluted” level and Cd was ranked as the “moderately polluted” level in tributary sediments of TGR. The assessment by Potential Ecological Risk Index showed that Hg and Cd were the predominant elements in tributary sediments in TGR. The Pb isotopic ratios in sediments varied from 1.171 to 1.202 for 206Pb/207Pb and from 2.459 to 2.482 for 208Pb/207Pb in TGR. All Pb isotopic ratios in sediments were similar to those from coal combustion, lead ores (the mining activities and smelting process), and cement material, indicating that these anthropogenic inputs may be the main sources for Pb pollution in sediments of TGR tributaries. PMID:24624045

A new method and application for determining the nitrogen isotopic composition of NOx

NASA Astrophysics Data System (ADS)

Hastings, M. G.; Miller, D. J.; Wojtal, P.; O'Connor, M.

2015-12-01

Atmospheric nitrogen oxides (NOx = NO + NO2) play key roles in atmospheric chemistry, air quality, and radiative forcing, and contribute to nitric acid deposition. Sources of NOx include both natural and anthropogenic emissions, which vary significantly in space and time. NOx isotopic signatures offer a potentially valuable tool to trace source impacts on atmospheric chemistry and regional acid deposition. Previous work on NOx isotopic signatures suggests large ranges in values, even from the same emission source, as well as overlapping ranges amongst different sources, making it difficult to use the isotopic composition as a quantitative tracer of source influences. These prior measurements have utilized a variety of methods for collecting the NOx as nitrate or nitrite for isotopic analysis, and testing of some of these methods (including active and passive collections) reveal inconsistencies in efficiency of collection, as well as issues related to changes in conditions such as humidity, temperature, and NOx fluxes. A recently developed method allows for accurately measuring the nitrogen isotopic composition of NOx (NOx = NO + NO2) after capturing the NOx in a potassium permanganate/sodium hydroxide solution as nitrate (Fibiger et al., Anal. Chem., 2014). The method has been thoroughly tested in the laboratory and field, and efficiently collects NO and NO2 under a variety of conditions. There are several advantages to collecting NOx actively, including the ability to collect over minutes to hourly time scales, and the ability to collect in environments with highly variable NOx sources and concentrations. Challenges include a nitrate background present in potassium permanganate (solid and liquid forms), accurately deriving ambient NOx concentrations based upon flow rate and solution concentrations above this variable background, and potential interferences from other nitrogen species. This method was designed to collect NOx in environments with very different emission source loadings in an effort to isotopically characterize NOx sources. Results to date suggest very different values, and less variability than previous work, particularly for vehicle emissions. Ultimately, we aim to determine whether the influence of NOx sources can be quantitatively tracked in the environment.

Non-Destructive X-ray Computed Tomography (XCT) of Gas Hydrate Bearing Fractures in Marine Sediment

NASA Astrophysics Data System (ADS)

Oti, E.; Buchwalter, E.; Cook, A.; Crandall, D.

2017-12-01

Hydrate-filled fractures are found in many environments, both related to methane vents and constrained to lithologic layers; how hydrate filled fractures form in layered environments is not well understood. We focus on understanding hydrate origins and fracture formation by examining hydrate-bearing fractures in conventional cores taken from Gulf of Mexico sites from JIP Leg 1 and UT-GOM, Keathley Canyon 151. There are two main methane sources available for hydrate formation. The first is the hydrocarbon reservoir underlying the Gulf sediments. This reservoir formed when deeply buried organic matter of high molecular weight was exposed to high temperature and pressures and degraded. A second source is the biogenesis of organic material, which occurs when microbial activity breaks down organic materials. Biogenic methane is more enriched in lighter carbon isotopes as the reduction or fermentation reactions preferentially consume lighter carbon isotopes. As a result, we hypothesize that sediment surrounding biogenically derived methane will have heavier carbon isotopes when compared to non-host sediment, due to the consumption of the lighter carbon isotopes during methanogenesis. We use non-destructive X-ray Computed Tomography (XCT) scanning to visualize and identify hydrate-bearing fractures. The presence of hydrate fractures is further confirmed with a salinity analysis, as hydrate dissociation freshens the pore water and lowers the salinity. After hydrate fracture location is inferred, carbon isotope analysis is used to identify hydrocarbon source. XCT scans of Keathley Canyon core JIP-1 17H-4 revealed 10 total fractures, five of which XCT and salinity analysis indicated as formerly containing hydrate. All ten fractures, in addition to background sediment, underwent a carbon isotope analysis in which organic isotopes were measured. In the background sediment and the non hydrate-bearing fractures, DOC values were relatively light, with dC13 percentages ranging from -27.8% to -30.8%. In the five hydrate fracture regions, DOC was comparatively heavy, with DOC dC13 values ranging from -23.2% to -30.3%. These values suggest that biogenic methane was formed adjacent to the fracture and likely migrated into the hydrate filled fracture.

133 Ba+: a new ion qubit

NASA Astrophysics Data System (ADS)

Christensen, Justin; Hucul, David; Campbell, Wesley; Hudson, Eric

2017-04-01

133 Ba+ combines many of the advantages of commonly used trapped ion qubits. 133Ba+ has a nuclear spin 1/2, allowing for a robust hyperfine qubit with simple state preparation and readout. The existence of long-lived metastable D-states and a lack of low-lying F-states simplifies shelving, which will allow high fidelity state detection. The visible wavelength optical transitions enable the use of high-power lasers, low-loss fibers, high quantum efficiency detectors, and other optical technologies developed for visible wavelength light. Furthermore, background-free qubit readout, where the readout is insensitive to laser scatter, is possible in 133Ba+, and simplifies its use in small ion traps and the study of ions near surfaces. We report progress on realizing this qubit. We load barium ions into an ion trap using thermal ionization from a platinum ribbon. We experimentally demonstrate the isotopic purification of large numbers of barium ions using laser heating and cooling along with mass filtering to produce isotopically pure chains of any naturally-occurring barium isotope. This purification process has allowed us to laser cool rare, naturally-occurring barium isotopes 132Ba+and130Ba+, and we report the isotope shifts from 138Ba+ of the P1/2 to D3/2 transitions near 650 nm for the first time. In addition, we have developed an ion gun to produce high luminosity ion beams with adjustable mean kinetic energy by combining a surface ionization source and ion optics.

The O and H stable isotope composition of freshwaters in the British Isles. 2. Surface waters and groundwater

NASA Astrophysics Data System (ADS)

Darling, W. G.; Bath, A. H.; Talbot, J. C.

The utility of stable isotopes as tracers of the water molecule has a long pedigree. The study reported here is part of an attempt to establish a comprehensive isotopic "baseline" for the British Isles as background data for a range of applications. Part 1 of this study (Darling and Talbot, 2003) considered the isotopic composition of rainfall in Britain and Ireland. The present paper is concerned with the composition of surface waters and groundwater. In isotopic terms, surface waters (other than some upland streams) are poorly characterised in the British Isles; their potential variability has yet to be widely used as an aid in hydrological research. In what may be the first study of a major British river, a monthly isotopic record of the upper River Thames during 1998 was obtained. This shows high damping of the isotopic variation compared to that in rainfall over most of the year, though significant fluctuations were seen for the autumn months. Smaller rivers such as the Stour and Darent show a more subdued response to the balance between runoff and baseflow. The relationship between the isotopic composition of rainfall and groundwater is also considered. From a limited database, it appears that whereas Chalk groundwater is a representative mixture of weighted average annual rainfall, for Triassic sandstone groundwater there is a seasonal selection of rainfall biased towards isotopically-depleted winter recharge. This may be primarily the result of physical differences between the infiltration characteristics of rock types, though other factors (vegetation, glacial history) could be involved. In the main, however, groundwaters appear to be representative of bulk rainfall within an error band of 0.5‰ δ18O. Contour maps of the δ18O and δ2H content of recent groundwaters in the British Isles show a fundamental SW-NE depletion effect modified by topography. The range of measured values, while much smaller than those for rainfall, still covers some ‰ for δ18O and 30‰ for δ2H. Over lowland areas the "altitude effect" is of little significance, but in upland areas is consistent with a range of -0.2 to -0.3‰ per 100 m increase in altitude. Groundwaters dating from the late Pleistocene are usually modified in δ18O and δ2H owing to the effects of climate change on the isotopic composition of rainfall and thus of recharge. Contour maps of isotopic variability prior to 10 ka BP, based on the relatively limited information available from the British Isles, allow a first comparison between groundwaters now and at the end of the last Ice Age. The position of the British Isles in the context of the stable isotope systematics of NW Europe is reviewed briefly.

Neutron capture cross-section studies of Tellurium isotopes for neutrinoless double beta decay applications

NASA Astrophysics Data System (ADS)

Bhike, Megha; Tornow, Werner

2014-09-01

The CUORE detector at Gran Sasso, aimed at searching for neutrinoless double-beta decay of 130Te, employs an array of TeO2 bolometer modules. To understand and identify the contribution of muon and (α,n) induced neutrons to the CUORE background, fast neutron cature cross-section data of the tellurium isotopes 126Te, 128Te and 130Te have been measured with the activation method at eight different energies in the neutron energy range 0.5-7.5 MeV. Plastic pill boxes of diameter 1.6 cm and width 1 cm containing Te were irradiated with mono-energetic neutrons produced via the 3H(p,n)3He and 2H(d,n)3He reactions. The cross-sections were determined relative to the 197Au(n, γ)198Au and 115In(n,n')115m In standard cross sections. The activities of the products were measured using 60% lead-shielded HPGe detectors at TUNL's low background counting facility. The present results are compared with the evaluated data from TENDL-2012, ENDF/B-VII.1, JEFF-3.2 and JENDL-4.0, as well as with literature data.

Cosmogenic activation of materials

NASA Astrophysics Data System (ADS)

Cebrián, Susana

2017-10-01

Experiments looking for rare events like the direct detection of dark matter particles, neutrino interactions or the nuclear double beta decay are operated deep underground to suppress the effect of cosmic rays. But, the production of radioactive isotopes in materials due to previous exposure to cosmic rays is a hazard when ultra-low background conditions are required. In this context, the generation of long-lived products by cosmic nucleons has been studied for many detector media and for other materials commonly used. Here, the main results obtained on the quantification of activation yields on the Earth’s surface will be summarized, considering both measurements and calculations following different approaches. The isotope production cross-sections and the cosmic ray spectrum are the two main ingredients when calculating this cosmogenic activation; the different alternatives for implementing them will be discussed. Activation that can take place deep underground mainly due to cosmic muons will be briefly commented too. Presently, the experimental results for the cosmogenic production of radioisotopes are scarce and discrepancies between different calculations are important in many cases, but the increasing interest on this background source which is becoming more and more relevant can help to change this situation.

Isotopic evidence of spatial magnitude of the Pb deposition near a lead smelter

NASA Astrophysics Data System (ADS)

Flament, P.; Franssens, M.; Debout, K.; Weis, D.

2003-05-01

In order to détermine the dry deposition of lead around a Pb-Zn refinery, two cross-sectional sampling experiments, using deposition plates, have been performed on a daiiy basis, ucder representative meteorological situations (north-easterly and south-westerly winds). The amount of lead deposited as well as its isotopic composition (expressed by the ^{206}Pb/^{207}Pb ratio) are systematically measured. For a daily production of approximately 670 metric tons of (Pb+Zn) the dry fallout, greater than 1000 μg Pb.h^{-1}.m^{-2} on the edge of the plant, falls to about 100 μg Pb.h^{-1}.m^{-2}, four kilometres away from the refinery. This value is still ten times higher than th urban background (<10 μg Pb.h^{-1}.m^{-2}). The spatial extension of the dry deposition plume is evidenced by the evolution of the isotopic signature of the refinery (1.10<^{206}Pb/^{207}), clearly distinct from the urban backgrounde signature (1.15<^{206}Pb/^{207}Pb<1.16). As a first estimate, the extension of the deposition plume seems not to be linked to the wind speed. At the opposite, diffuse emissions from slag heaps are related to this parameter.

Monitoring CO2 concentration and δ13C in an underground cavity using a commercial isotope ratio infrared spectrometer

NASA Astrophysics Data System (ADS)

Guillon, Sophie; Agrinier, Pierre; Pili, Éric

2015-04-01

CO2 stable carbon isotopes are very attractive in environmental research to investigate both natural and anthropogenic carbon sources. Laser-based isotope ratio infrared spectrometers (IRIS) allow in situ continuous monitoring of CO2 isotopes, and therefore they have a potential for unprecedented understanding of carbon sources and dynamics with a high temporal resolution. Here we present the performance assessment of a commercial IRIS analyzer, including the measurement setup and the data processing scheme that we used. Even if the analyzer performs 1-Hz measurements, an integration time of the order of 1 h is commonly needed to obtain acceptable precision for δ13C. The main sources of uncertainty on δ13C come from the concentration dependence and from the temporal instability of the analyzer. The method is applied to the in situ monitoring of the CO2 carbon isotopes in an underground cavity (Roselend Natural Laboratory, France) during several months. On a weekly timescale, the temporal variability of CO2 is dominated by transient contamination by human breath. Discarding these anthropogenic contaminations, CO2 and δ13C backgrounds do not show diurnal or seasonal fluctuations. A CO2 flux released into the tunnel by the surrounding rocks is measured. The carbon isotope composition of this CO2, identified with a Keeling plot, is consistent with a main production by microbial respiration and a minor production from weathering of carbonate minerals. The presented instrument and application study are relevant to cave monitoring, whether to understand CO2 dynamics in visited and/or painted caves for preservation purposes or to understand paleoclimate recording in speleothems.

Sulphur isotopes as tracers of the influence of a coal-fired power plant on a Scots pine forest in Catalonia (NE Spain)

NASA Astrophysics Data System (ADS)

Puig, R.; Àvila, A.; Soler, A.

Stable sulphur isotopes and major ionic composition were analysed in precipitation and throughfall samples from a Scots pine ( Pinus sylvestris, L.) forest near the Cercs coal-fired power plant (Catalonia, NE Spain). The purpose of the study was to determine the main sources of sulphur deposition on this pine forest. Sulphur isotope measurements from the SO 2 power plant stack emissions were used to identify the isotopic signature of this source. Net throughfall fluxes of sulphur (26.1 kg S ha 1 yr -1) and nitrogen (16.3 kg N ha -1 yr -1) were higher—5-25 times higher for S and 5-15 times for N—at this site than in other forests in Catalonia. Sulphur isotope analysis confirmed that the net throughfall fluxes of sulphur were mostly due to the dry deposition of the SO 2 power plant emissions onto the pine canopies. Two potential atmospheric end-members were distinguished: regional background rainwater (δ 34S=+7.2‰) and power plant emissions (δ 34S=-2.8‰). By applying a two-component sulphur isotope mixing model, we found that during periods of low power plant activity (⩽10 emission h day -1), 62% of the throughfall sulphate could be attributed to the power plant emissions. At higher activity periods (⩾14 emission h day -1), this contribution rose to 73%. Although power plant contribution to bulk deposition was lower in both cases (34% and 45%), the possible influence of sulphate coming with long-range transport events from the polluted areas in the Mediterranean basin (δ 34S≈0‰) was not discarded.

Isotope-coded ESI-enhancing derivatization reagents for differential analysis, quantification and profiling of metabolites in biological samples by LC/MS: A review.

PubMed

Higashi, Tatsuya; Ogawa, Shoujiro

2016-10-25

The analysis of the qualitative and quantitative changes of metabolites in body fluids and tissues yields valuable information for the diagnosis, pathological analysis and treatment of many diseases. Recently, liquid chromatography/electrospray ionization-(tandem) mass spectrometry [LC/ESI-MS(/MS)] has been widely used for these purposes due to the high separation capability of LC, broad coverage of ESI for various compounds and high specificity of MS(/MS). However, there are still two major problems to be solved regarding the biological sample analysis; lack of sensitivity and limited availability of stable isotope-labeled analogues (internal standards, ISs) for most metabolites. Stable isotope-coded derivatization (ICD) can be the answer for these problems. By the ICD, different isotope-coded moieties are introduced to the metabolites and one of the resulting derivatives can serve as the IS, which minimize the matrix effects. Furthermore, the derivatization can improve the ESI efficiency, fragmentation property in the MS/MS and chromatographic behavior of the metabolites, which lead to a high sensitivity and specificity in the various detection modes. Based on this background, this article reviews the recently-reported isotope-coded ESI-enhancing derivatization (ICEED) reagents, which are key components for the ICD-based LC/MS(/MS) studies, and their applications to the detection, identification, quantification and profiling of metabolites in human and animal samples. The LC/MS(/MS) using the ICEED reagents is the powerful method especially for the differential analysis (relative quantification) of metabolites in two comparative samples, simultaneous quantification of multiple metabolites whose stable isotope-labeled ISs are not available, and submetabolome profiling. Copyright © 2016 Elsevier B.V. All rights reserved.

First results of a simultaneous measurement of tritium and 14C in an ultra-low-background proportional counter for environmental sources of methane

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mace, Emily K.; Aalseth, Craig E.; Day, Anthony R.

Abstract Simultaneous measurement of tritium and 14C would provide an added tool for tracing organic compounds through environmental systems and is possible via beta energy spectroscopy of sample-derived methane in internal-source gas proportional counters. Since the mid-1960’s atmospheric tritium and 14C have fallen dramatically as the isotopic injections from above-ground nuclear testing have been diluted into the ocean and biosphere. In this work, the feasibility of simultaneous tritium and 14C measurements via proportional counters is revisited in light of significant changes in both the atmospheric and biosphere isotopics and the development of new ultra-low-background gas proportional counting capabilities for smallmore » samples (roughly 50 cc methane). A Geant4 Monte Carlo model of a Pacific Northwest National Laboratory (PNNL) proportional counter response to tritium and 14C is used to analyze small samples of two different methane sources to illustrate the range of applicability of contemporary simultaneous measurements and their limitations. Because the two methane sources examined were not sample size limited, we could compare the small-sample measurements performed at PNNL with analysis of larger samples performed at a commercial laboratory. The dual-isotope simultaneous measurement is well matched for methane samples that are atmospheric or have an elevated source of tritium (i.e. landfill gas). For samples with low/modern tritium isotopics (rainwater), commercial separation and counting is a better fit.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Park, HyangKyu

The AMoRE (Advanced Mo based Rare process Experiment) collaboration is going to use calcium molybdate crystals to search for neutrinoless double beta decay of {sup 100}Mo isotope. In order to make the crystal, we use calcium carbonate and molybdenum oxide powders as raw materials. Therefore it is highly necessary to reduce potential sources for radioactive backgrounds such as U and Th in the powders. In this talk, we will present our studies for purification of calcium carbonate and molybdenum oxide powders.

Contaminated lead environments of man: reviewing the lead isotopic evidence in sediments, peat, and soils for the temporal and spatial patterns of atmospheric lead pollution in Sweden.

PubMed

Bindler, Richard

2011-08-01

Clair Patterson and colleagues demonstrated already four decades ago that the lead cycle was greatly altered on a global scale by humans. Moreover, this change occurred long before the implementation of monitoring programs designed to study lead and other trace metals. Patterson and colleagues also developed stable lead isotope analyses as a tool to differentiate between natural and pollution-derived lead. Since then, stable isotope analyses of sediment, peat, herbaria collections, soils, and forest plants have given us new insights into lead biogeochemical cycling in space and time. Three important conclusions from our studies of lead in the Swedish environment conducted over the past 15 years, which are well supported by extensive results from elsewhere in Europe and in North America, are: (1) lead deposition rates at sites removed from major point sources during the twentieth century were about 1,000 times higher than natural background deposition rates a few thousand years ago (~10 mg Pb m(-2) year(-1) vs. 0.01 mg Pb m(-2) year(-1)), and even today (~1 mg Pb m(-2) year(-1)) are still almost 100 times greater than natural rates. This increase from natural background to maximum fluxes is similar to estimated changes in body burdens of lead from ancient times to the twentieth century. (2) Stable lead isotopes ((206)Pb/(207)Pb ratios shown in this paper) are an effective tool to distinguish anthropogenic lead from the natural lead present in sediments, peat, and soils for both the majority of sites receiving diffuse inputs from long range and regional sources and for sites in close proximity to point sources. In sediments >3,500 years and in the parent soil material of the C-horizon, (206)Pb/(207)Pb ratios are higher, 1.3 to >2.0, whereas pollution sources and surface soils and peat have lower ratios that have been in the range 1.14-1.18. (3) Using stable lead isotopes, we have estimated that in southern Sweden the cumulative anthropogenic burden of atmospherically deposited lead is ~2-5 g Pb m(-2) and ~1 g Pb m(-2) in the "pristine" north. Half of this cumulative total was deposited before industrialization. (4) In the vicinity of the Rönnskär smelter in northern Sweden, a major point source during the twentieth century, there is an isotopic pattern that deviates from the general trends elsewhere, reflecting the particular history of ore usage at Rönnskär, which further demonstrates the chronological record of lead loading recorded in peat and in soil mor horizons.

Gamma-Ray Background Variability in Mobile Detectors

NASA Astrophysics Data System (ADS)

Aucott, Timothy John

Gamma-ray background radiation significantly reduces detection sensitivity when searching for radioactive sources in the field, such as in wide-area searches for homeland security applications. Mobile detector systems in particular must contend with a variable background that is not necessarily known or even measurable a priori. This work will present measurements of the spatial and temporal variability of the background, with the goal of merging gamma-ray detection, spectroscopy, and imaging with contextual information--a "nuclear street view" of the ubiquitous background radiation. The gamma-ray background originates from a variety of sources, both natural and anthropogenic. The dominant sources in the field are the primordial isotopes potassium-40, uranium-238, and thorium-232, as well as their decay daughters. In addition to the natural background, many artificially-created isotopes are used for industrial or medical purposes, and contamination from fission products can be found in many environments. Regardless of origin, these backgrounds will reduce detection sensitivity by adding both statistical as well as systematic uncertainty. In particular, large detector arrays will be limited by the systematic uncertainty in the background and will suffer from a high rate of false alarms. The goal of this work is to provide a comprehensive characterization of the gamma-ray background and its variability in order to improve detection sensitivity and evaluate the performance of mobile detectors in the field. Large quantities of data are measured in order to study their performance at very low false alarm rates. Two different approaches, spectroscopy and imaging, are compared in a controlled study in the presence of this measured background. Furthermore, there is additional information that can be gained by correlating the gamma-ray data with contextual data streams (such as cameras and global positioning systems) in order to reduce the variability in the background. This is accomplished by making many hours of background measurements with a truck-mounted system, which utilizes high-purity germanium detectors for spectroscopy and sodium iodide detectors for coded aperture imaging. This system also utilizes various peripheral sensors, such as panoramic cameras, laser ranging systems, global positioning systems, and a weather station to provide context for the gamma-ray data. About three hundred hours of data were taken in the San Francisco Bay Area, covering a wide variety of environments that might be encountered in operational scenarios. These measurements were used in a source injection study to evaluate the sensitivity of different algorithms (imaging and spectroscopy) and hardware (sodium iodide and high-purity germanium detectors). These measurements confirm that background distributions in large, mobile detector systems are dominated by systematic, not statistical variations, and both spectroscopy and imaging were found to substantially reduce this variability. Spectroscopy performed better than the coded aperture for the given scintillator array (one square meter of sodium iodide) for a variety of sources and geometries. By modeling the statistical and systematic uncertainties of the background, the data can be sampled to simulate the performance of a detector array of arbitrary size and resolution. With a larger array or lower resolution detectors, however imaging was better able to compensate for background variability.

PeakWorks

DOE Office of Scientific and Technical Information (OSTI.GOV)

2016-11-30

The PeakWorks software is designed to assist in the quantitative analysis of atom probe tomography (APT) generated mass spectra. Specifically, through an interactive user interface, mass peaks can be identified automatically (defined by a threshold) and/or identified manually. The software then provides a means to assign specific elemental isotopes (including more than one) to each peak. The software also provides a means for the user to choose background subtraction of each peak based on background fitting functions, the choice of which is left to the users discretion. Peak ranging (the mass range over which peaks are integrated) is also automatedmore » allowing the user to chose a quantitative range (e.g. full-widthhalf- maximum). The software then integrates all identified peaks, providing a background-subtracted composition, which also includes the deconvolution of peaks (i.e. those peaks that happen to have overlapping isotopic masses). The software is also able to output a 'range file' that can be used in other software packages, such as within IVAS. A range file lists the peak identities, the mass range of each identified peak, and a color code for the peak. The software is also able to generate 'dummy' peak ranges within an outputted range file that can be used within IVAS to provide a means for background subtracted proximity histogram analysis.« less

Atmospheric Trace Gas Abundances and Stable Isotope Ratios via IR-LIF

NASA Technical Reports Server (NTRS)

Blake, Geoffrey A.

2004-01-01

We propose to develop new technologies with support provided by PIDDP that will enable the in situ measurements of abundances and stable isotope ratios in important radiatively and biogenically active gases such as carbon dioxide, carbon monoxide, water, methane, nitrous oxide, and hydrogen sulfide to very high precision (0.1 per mil or better for the isotopic ratios, for example). Such measurements, impossible at present, could provide pivotal new constraints on the global (bio)geochemical budgets of these critical species, and could also be used to examine the dynamics of atmospheric transport on Mars, Titan, and other solar system bodies. We believe the combination of solid state light sources with imaging of the IR laser induced fluorescence (IR-LIF) via newly available detector arrays will make such in situ measurements possible for the first time. Even under ambient terrestrial conditions, the LIF yield from vibrational excitation of species such as water and carbon dioxide should produce emission measures well in excess of ten billion photons/sec from samples volumes of order 1 c.c. These count rates can, in principle, yield detection limits into the sub-ppt range that are required for the in situ isotopic study of atmospheric trace gases. While promising, such technologies are relatively immature, but developing rapidly, and there are a great many uncertainties regarding their applicability to in situ IR-LIF planetary studies. We therefore feel PIDDP support will be critical to developing these new tools, and propose a three-year program to combine microchip near-IR lasers with low background detection axes and state-of-the-art HgCdTe detectors developed for astronomical spectroscopy to investigate the sensitivity of IR-LIF under realistic planetary conditions, to optimize the optical pumping and filtering schemes for important species, and to apply the spectrometer to the non-destructive measurement of stable isotopes in a variety of test samples. These studies form the necessary precursors to the development of compact, lightweight stable isotope/trace gas sensors for future planetary missions.

A Carbonate Li Isotope Record Through Earth's History

NASA Astrophysics Data System (ADS)

Asael, D.; Kalderon-Asael, B.; Planavsky, N.

2016-12-01

Lithium (Li) isotopes emerge as a powerful geochemical proxy for tracking continental weathering through time. Extensive work on Li fractionation in modern systems has brought to a profound understanding of the modern Li budget as well as to a consensus that marine carbonates faithfully record seawater Li isotope signature. As such record is essential in order to track global-scale changes in weathering processes and intensity through Earth's history, we have generated Li isotope data from marine carbonates from over 40 units, ranging in age from 3.0 Ga to modern. Preliminary results provide evidence for strongly inhibited weathering-mediated clay formation prior to the Paleozoic, which we attribute to the pre-Paleozoic lack of land plants. The initial rise in the Li isotope values is observed during the Ordovician, which is followed by a subsequent drop to background values and then begins the generally increasing trend that is already well reported. These findings are open for interpretation but they still support the view that the emergence of land plants dramatically changed the process of weathering and it seems that biomass has a potentially significant role in mineral breakdown in soils. Li isotopes provide a novel perspective on weathering and the impact on the Earth system of the rise of land plants - one of the most significant transitions in Earth's history.

Isotopic composition analysis and age dating of uranium samples by high resolution gamma ray spectrometry

NASA Astrophysics Data System (ADS)

Apostol, A. I.; Pantelica, A.; Sima, O.; Fugaru, V.

2016-09-01

Non-destructive methods were applied to determine the isotopic composition and the time elapsed since last chemical purification of nine uranium samples. The applied methods are based on measuring gamma and X radiations of uranium samples by high resolution low energy gamma spectrometric system with planar high purity germanium detector and low background gamma spectrometric system with coaxial high purity germanium detector. The ;Multigroup γ-ray Analysis Method for Uranium; (MGAU) code was used for the precise determination of samples' isotopic composition. The age of the samples was determined from the isotopic ratio 214Bi/234U. This ratio was calculated from the analyzed spectra of each uranium sample, using relative detection efficiency. Special attention is paid to the coincidence summing corrections that have to be taken into account when performing this type of analysis. In addition, an alternative approach for the age determination using full energy peak efficiencies obtained by Monte Carlo simulations with the GESPECOR code is described.

Determination of Mo- and Ca-isotope ratios in Ca100MoO4 crystal for AMoRE-I experiment

NASA Astrophysics Data System (ADS)

Karki, S.; Aryal, P.; Kim, H. J.; Kim, Y. D.; Park, H. K.

2018-01-01

The first phase of the AMoRE (Advanced Mo-based Rare process Experiment) is to search for neutrinoless double-beta decay of 100Mo with calcium molybdate (Ca100MoO4) crystals enriched in 100Mo and depleted in 48Ca using a cryogenic technique at Yangyang underground laboratory in Korea. It is important to know 100Mo- and 48Ca-isotope ratios in Ca100MoO4 crystal to estimate half-life of 100Mo decays and to 2 νββ background from 48Ca. We employed the ICP-MS (Inductive Coupled Plasma Mass Spectrometer) to measure 100Mo- and 48Ca-isotope ratios in Ca100MoO4 crystal. The measured results for 100Mo- and 48Ca-isotope ratios in the crystal are (94 . 6 ± 2 . 8) % and (0 . 00211 ± 0 . 00006) %, respectively, where errors are included both statistical and systematic uncertainties.

Quantitative trace analysis of polyfluorinated alkyl substances (PFAS) in ambient air samples from Mace Head (Ireland): A method intercomparison

NASA Astrophysics Data System (ADS)

Jahnke, Annika; Barber, Jonathan L.; Jones, Kevin C.; Temme, Christian

A method intercomparison study of analytical methods for the determination of neutral, volatile polyfluorinated alkyl substances (PFAS) was carried out in March, 2006. Environmental air samples were collected in triplicate at the European background site Mace Head on the west coast of Ireland, a site dominated by 'clean' westerly winds coming across the Atlantic. Extraction and analysis were performed at two laboratories active in PFAS research using their in-house methods. Airborne polyfluorinated telomer alcohols (FTOHs), fluorooctane sulfonamides and sulfonamidoethanols (FOSAs/FOSEs) as well as additional polyfluorinated compounds were investigated. Different native and isotope-labelled internal standards (IS) were applied at various steps in the analytical procedure to evaluate the different quantification strategies. Field blanks revealed no major blank problems. European background concentrations observed at Mace Head were found to be in a similar range to Arctic data reported in the literature. Due to trace-levels at the remote site, only FTOH data sets were complete and could therefore be compared between the laboratories. Additionally, FOSEs could partly be included. Data comparison revealed that despite the challenges inherent in analysis of airborne PFAS and the low concentrations, all methods applied in this study obtained similar results. However, application of isotope-labelled IS early in the analytical procedure leads to more precise results and is therefore recommended.

Multiple sources supply eolian mineral dust to the Atlantic sector of coastal Antarctica: Evidence from recent snow layers at the top of Berkner Island ice sheet

NASA Astrophysics Data System (ADS)

Bory, Aloys; Wolff, Eric; Mulvaney, Robert; Jagoutz, Emil; Wegner, Anna; Ruth, Urs; Elderfield, Harry

2010-03-01

The Sr and Nd isotopic composition of dust extracted from recent snow layers at the top of Berkner Island ice sheet (located within the Filchner-Ronne Ice Shelf at the southern end of the Weddell Sea) enables us, for the first time, to document dust provenance in Antarctica outside the East Antarctic Plateau (EAP) where all previous studies based on isotopic fingerprinting were carried out. Berkner dust displays an overall crust-like isotopic signature, characterized by more radiogenic 87Sr/ 86Sr and much less radiogenic 143Nd/ 144Nd compared to dust deposited on the EAP during glacial periods. Differences with EAP interglacial dust are not as marked but still significant, indicating that present-day Berkner dust provenance is distinct, at least to some extent, from that of the dust reaching the EAP. The fourteen snow-pit sub-seasonal samples that were obtained span a two-year period (2002-2003) and their dust Sr and Nd isotopic composition reveals that multiple sources are at play over a yearly time period. Southern South America, Patagonia in particular, likely accounts for part of the observed spring/summer dust deposition maxima, when isotopic composition is shifted towards "younger" isotopic signatures. In the spring, possible additional inputs from Australian sources would also be supported by the data. Most of the year, however, the measured isotopic signatures would be best explained by a sustained background supply from putative local sources in East Antarctica, which carry old-crust-like isotopic fingerprints. Whether the restricted East Antarctic ice-free areas produce sufficient eolian material has yet to be substantiated however. The fact that large (> 5 μm) particles represent a significant fraction of the samples throughout the entire time-series supports scenarios that involve contributions from proximal sources, either in Patagonia and/or Antarctica (possibly including snow-free areas in the Antarctic Peninsula and other areas as well). This also indicates that additional dust transport, which does not reach the EAP, must occur at low-tropospheric levels to this coastal sector of Antarctica.

Using Pb isotopes in surface media to distinguish anthropogenic sources from undercover uranium sources

NASA Astrophysics Data System (ADS)

Kyser, Kurt; Lahusen, Larry; Drever, Garth; Dunn, Colin; Leduc, Evelyne; Chipley, Don

2015-09-01

The response in elemental concentrations and Pb isotopes in various surface media from the Cigar West unconformity-type uranium deposit located at a depth of 450 m were measured to ascertain if element migration from the deposit can be detected at the surface. The media included clay-size fractions separated from the A2, B and C soil horizons, and tree cores and twigs from black spruce (Picea mariana) and jack pine (Pinus banksiana) trees. Lead isotopes were used to trace any effect on the surface media from the deposit at depth because the 207Pb/206Pb ratios in the ore are < 0.1, whereas the background values in the basin are > 0.7 and modern anthropogenic Pb from aerosols are near 0.9. The tree cores record their lowest and therefore most radiogenic 207Pb/206Pb ratios of < 0.7 near the surface projection of the deposit and associated structures, particularly in tree rings that predate any exploration and drilling activity in the area. The median 207Pb/206Pb ratios increase in the order C, B soil horizon clays, tree cores, A2 soil clays and twigs because of the increasing contribution of common Pb with high ratios from anthropogenic sources that affect the shallowest media the most. Although this anthropogenic Pb as well as that from the background dominates the composition of all media at the surface and the contribution from the deposit at depth is diminished toward the surface, ore-related Pb is still present as a few percent of the composition of pathfinder elements and Pb isotopes.

Production of beta-gamma coincidence spectra of individual radioxenon isotopes for improved analysis of nuclear explosion monitoring data

NASA Astrophysics Data System (ADS)

Haas, Derek Anderson

Radioactive xenon gas is a fission product released in the detonation of nuclear devices that can be detected in atmospheric samples far from the detonation site. In order to improve the capabilities of radioxenon detection systems, this work produces beta-gamma coincidence spectra of individual isotopes of radioxenon. Previous methods of radioxenon production consisted of the removal of mixed isotope samples of radioxenon gas released from fission of contained fissile materials such as 235U. In order to produce individual samples of the gas, isotopically enriched stable xenon gas is irradiated with neutrons. The detection of the individual isotopes is also modeled using Monte Carlo simulations to produce spectra. The experiment shows that samples of 131mXe, 133 Xe, and 135Xe with a purity greater than 99% can be produced, and that a sample of 133mXe can be produced with a relatively low amount of 133Xe background. These spectra are compared to models and used as essential library data for the Spectral Deconvolution Analysis Tool (SDAT) to analyze atmospheric samples of radioxenon for evidence of nuclear events.

Use and abuse of mixing models (MixSIAR)

EPA Science Inventory

Background/Question/MethodsCharacterizing trophic links in food webs is a fundamental ecological question. In our efforts to quantify energy flow through food webs, ecologists have increasingly used mixing models to analyze biological tracer data, often from stable isotopes. Whil...

Improving estimation of phytoplankton isotopic values from bulk POM samples in rivers

EPA Science Inventory

Background/Questions/MethodsResponses of phytoplankton to excessive nutrients in rivers cause many ecological problems, including harmful algal blooms, hypoxia and even food web collapse, posing serious risks to fish and human health. Successful remediation requires identificati...

Radioactivity of peat mud used in therapy.

PubMed

Karpińska, Maria; Mnich, Krystian; Kapała, Jacek; Bielawska, Agnieszka; Kulesza, Grzegorz; Mnich, Stanisław

2016-02-01

The aim of the study was to determine the contents of natural and artificial isotopes in peat mud and to estimate the radiation dose absorbed via skin in patients during standard peat mud treatment. The analysis included 37 samples collected from 8 spas in Poland. The measurements of isotope concentration activity were conducted with the use of gamma spectrometry methods. The skin dose in a standard peat mud bath therapy is approximately 300 nSv. The effective dose of such therapy is considered to be 22 nSv. The doses absorbed during peat mud therapy are 5 orders of magnitude lower than effective annual dose absorbed from the natural radiation background by a statistical Pole (3.5 mSv). Neither therapeutic nor harmful effect is probable in case of such a small dose of ionising radiation. Copyright © 2015 Elsevier Ltd. All rights reserved.

Optical Design Considerations for Efficient Light Collection from Liquid Scintillation Counters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bernacki, Bruce E.; Douglas, Matthew; Erchinger, Jennifer L.

2015-01-01

Liquid scintillation counters measure charged particle-emitting radioactive isotopes and are used for environmental studies, nuclear chemistry, and life science. Alpha and beta emissions arising from the material under study interact with the scintillation cocktail to produce light. The prototypical liquid scintillation counter employs low-level photon-counting detectors to measure the arrival of the scintillation light produced as a result of the dissolved material under study interacting with the scintillation cocktail. For reliable operation the counting instrument must convey the scintillation light to the detectors efficiently and predictably. Current best practices employ the use of two or more detectors for coincidence processingmore » to discriminate true scintillation events from background events due to instrumental effects such as photomultiplier tube dark rates, tube flashing, or other light emission not generated in the scintillation cocktail vial. In low background liquid scintillation counters additional attention is paid to shielding the scintillation cocktail from naturally occurring radioactive material (NORM) present in the laboratory and within the instruments construction materials. Low background design is generally at odds with optimal light collection. This study presents the evolution of a light collection design for liquid scintillation counting in a low background shield. The basic approach to achieve both good light collection and a low background measurement is described. The baseline signals arising from the scintillation vial are modeled and methods to efficiently collect scintillation light are presented as part of the development of a customized low-background, high sensitivity liquid scintillation counting system.« less

Consistent relationship between global climate and surface nitrate utilization in the western subarctic Pacific throughout the last 500 ka

NASA Astrophysics Data System (ADS)

Galbraith, Eric D.; Kienast, Markus; Jaccard, Samuel L.; Pedersen, Thomas F.; Brunelle, Brigitte G.; Sigman, Daniel M.; Kiefer, Thorsten

2008-06-01

The open subarctic Pacific is, at present, a high nitrate low chlorophyll (HNLC) region, where nitrate is perennially abundant at the surface. Theoretically, the HNLC status of this region is subject to modification by ocean circulation and/or micronutrient supply, with implications for the effectiveness of the biological pump and hence carbon sequestration in the ocean interior. Records of biogenic detritus in sediments from throughout the subarctic Pacific indicate that export production was generally lower during glacial maxima, while nitrogen isotope measurements from the Bering Sea have shown that nitrate consumption there was more complete during the last glacial period than it is today. Here, nitrogen isotopic analyses of bulk sediments (δ15Nbulk) from three deep water sites in the open subarctic Pacific are evaluated in terms of regional nitrate isotopic composition and local relative nitrate utilization. The eastern subarctic Pacific δ15Nbulk record bears great similarity to δ15Nbulk records from the western margin of North America over the last glacial cycle, suggesting that variability in the isotopic composition of subeuphotic zone nitrate, the growth substrate, is reasonably coherent throughout the northeast Pacific and dominates at these sites. However, the two western subarctic Pacific records, which lie at the heart of the HNLC region, display a different pattern, implying that significant changes in local relative nitrate utilization overlie the regional background variability. After a novel correction intended to remove the background signal associated with denitrification in the eastern tropical North Pacific, these nitrate utilization records are correlated with a benthic oxygen isotope stack reflecting global deep ocean temperature and ice volume (r2 = 0.65). The correlation implies a strong link between global climate and subarctic Pacific nitrate utilization, with nearly complete nitrate consumption during glacial periods when export production was low.

Radon background in liquid xenon detectors

NASA Astrophysics Data System (ADS)

Rupp, N.

2018-02-01

The radioactive daughters isotope of 222Rn are one of the highest risk contaminants in liquid xenon detectors aiming for a small signal rate. The noble gas is permanently emanated from the detector surfaces and mixed with the xenon target. Because of its long half-life 222Rn is homogeneously distributed in the target and its subsequent decays can mimic signal events. Since no shielding is possible this background source can be the dominant one in future large scale experiments. This article provides an overview of strategies used to mitigate this source of background by means of material selection and on-line radon removal techniques.

Central Irish geology/metallogeny: A lower Carboniferous rifting-related exhalative catastrophy?

NASA Astrophysics Data System (ADS)

Deeny, D. E.

1987-04-01

The geological background and development of a recently presented Irish Carboniferous metallogenic model is outlined. A new (exhalative-based) interpretation of existing central Irish tectonic, stratigraphic, sedimentological and sulphur isotopic data is shown to be consistent with the model, which suggests that stratiform sulphide metallogeny and the central Irish Waulsortian mudbank complex may be the manifestation of a rifting-related exhalative catastrophy. In this view sulphur isotope age curves of the whole world ocean may indicate that phases of globally synchronous (in the relative sense) rifting may have been a feature of the Phanerozoic record.

Global Xenon-133 Emission Inventory Caused by Medical Isotope Production and Derived from the Worldwide Technetium-99m Demand

NASA Astrophysics Data System (ADS)

Kalinowski, Martin B.; Grosch, Martina; Hebel, Simon

2014-03-01

Emissions from medical isotope production are the most important source of background for atmospheric radioxenon measurements, which are an essential part of nuclear explosion monitoring. This article presents a new approach for estimating the global annual radioxenon emission inventory caused by medical isotope production using the amount of Tc-99m applications in hospitals as the basis. Tc-99m is the most commonly used isotope in radiology and dominates the medical isotope production. This paper presents the first estimate of the global production of Tc-99m. Depending on the production and transport scenario, global xenon emissions of 11-45 PBq/year can be derived from the global isotope demand. The lower end of this estimate is in good agreement with other estimations which are making use of reported releases and realistic process simulations. This proves the validity of the complementary assessment method proposed in this paper. It may be of relevance for future emission scenarios and for estimating the contribution to the global source term from countries and operators that do not make sufficient radioxenon release information available. It depends on sound data on medical treatments with radio-pharmaceuticals and on technical information on the production process of the supplier. This might help in understanding the apparent underestimation of the global emission inventory that has been found by atmospheric transport modelling.

Detection of testosterone administration based on the carbon isotope ratio profiling of endogenous steroids: international reference populations of professional soccer players

PubMed Central

Strahm, E; Emery, C; Saugy, M; Dvorak, J; Saudan, C

2009-01-01

Background and objectives: The determination of the carbon isotope ratio in androgen metabolites has been previously shown to be a reliable, direct method to detect testosterone misuse in the context of antidoping testing. Here, the variability in the 13C/12C ratios in urinary steroids in a widely heterogeneous cohort of professional soccer players residing in different countries (Argentina, Italy, Japan, South Africa, Switzerland and Uganda) is examined. Methods: Carbon isotope ratios of selected androgens in urine specimens were determined using gas chromatography/combustion/isotope ratio mass spectrometry (GC-C-IRMS). Results: Urinary steroids in Italian and Swiss populations were found to be enriched in 13C relative to other groups, reflecting higher consumption of C3 plants in these two countries. Importantly, detection criteria based on the difference in the carbon isotope ratio of androsterone and pregnanediol for each population were found to be well below the established threshold value for positive cases. Conclusions: The results obtained with the tested diet groups highlight the importance of adapting the criteria if one wishes to increase the sensitivity of exogenous testosterone detection. In addition, confirmatory tests might be rendered more efficient by combining isotope ratio mass spectrometry with refined interpretation criteria for positivity and subject-based profiling of steroids. PMID:19549614

Production and relevance of cosmogenic radionuclides in NaI(Tl) crystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Amaré, J.; Cebrián, S.; Cuesta, C.

2015-08-17

The cosmogenic production of long-lived radioactive isotopes in materials is an hazard for experiments demanding ultra-low background conditions. Although NaI(Tl) scintillators have been used in this context for a long time, very few activation data were available. We present results from two 12.5 kg NaI(Tl) detectors, developed within the ANAIS project and installed at the Canfranc Underground Laboratory. The prompt data taking starting made possible a reliable quantification of production of some I, Te and Na isotopes with half-lives larger than ten days. Tnitial activities underground were measured and then production rates at sea level were estimated following the history ofmore » detectors; a comparison of these rates with calculations using typical cosmic neutron flux at sea level and a selected description of excitation functions was also carried out. After including the contribution from the identified cosmogenic products in the detector background model, we found that the presence of {sup 3}H in the crystal bulk would help to fit much better our background model and experimental data. We have analyzed the cosmogenic production of {sup 3}H in NaI, and although precise quantification has not been attempted, we can conclude that it could imply a very relevant contribution to the total background below 15 ke in NaI detectors.« less

Stable isotope reactive transport modeling in water-rock interactions during CO2 injection

NASA Astrophysics Data System (ADS)

Hidalgo, Juan J.; Lagneau, Vincent; Agrinier, Pierre

2010-05-01

Stable isotopes can be of great usefulness in the characterization and monitoring of CO2 sequestration sites. Stable isotopes can be used to track the migration of the CO2 plume and identify leakage sources. Moreover, they provide unique information about the chemical reactions that take place on the CO2-water-rock system. However, there is a lack of appropriate tools that help modelers to incorporate stable isotope information into the flow and transport models used in CO2 sequestration problems. In this work, we present a numerical tool for modeling the transport of stable isotopes in groundwater reactive systems. The code is an extension of the groundwater single-phase flow and reactive transport code HYTEC [2]. HYTEC's transport module was modified to include element isotopes as separate species. This way, it is able to track isotope composition of the system by computing the mixing between the background water and the injected solution accounting for the dependency of diffusion on the isotope mass. The chemical module and database have been expanded to included isotopic exchange with minerals and the isotope fractionation associated with chemical reactions and mineral dissolution or precipitation. The performance of the code is illustrated through a series of column synthetic models. The code is also used to model the aqueous phase CO2 injection test carried out at the Lamont-Doherty Earth Observatory site (Palisades, New York, USA) [1]. References [1] N. Assayag, J. Matter, M. Ader, D. Goldberg, and P. Agrinier. Water-rock interactions during a CO2 injection field-test: Implications on host rock dissolution and alteration effects. Chemical Geology, 265(1-2):227-235, July 2009. [2] Jan van der Lee, Laurent De Windt, Vincent Lagneau, and Patrick Goblet. Module-oriented modeling of reactive transport with HYTEC. Computers & Geosciences, 29(3):265-275, April 2003.

Intra-seasonal dynamics in metabolic processes of 13C/12C and 18O/16O in components of Scots pine twigs from southern Siberia interpreted with a conceptual framework based on the Carbon Metabolism Oscillatory Model

PubMed Central

2012-01-01

Background Carbon isotope data from conifer trees play an important role in research on the boreal forest carbon reservoir in the global carbon cycle. Carbon isotopes are routinely used to study interactions between the environment and tree growth. Moreover, carbon isotopes became an essential tool for the evaluation of carbon assimilation and transport from needles into reserve pools, as well as the allocation of stored assimilates within a tree. The successful application and interpretation of carbon isotopes rely on the coherence of isotopic fractionation modeling. This study employs a new Carbon Metabolism Oscillatory Model (CMOM) to interpret the experimental data sets on metabolic seasonal dynamics of 13C/12 C and 18O/16O ratios measured in twig components of Scots pine growing in southern Siberia (Russia). Results The dynamics of carbon isotopic variables were studied in components of Pinus sylvestris L. in light and in dark chambers during the vegetation period from 14 June to 28 July 2006. At the beginning of this period water-soluble organic matter, mostly labile sugars (including sucrose as the main component) and newly formed bulk needle material, displayed relatively “light” δ13C values (depletion in 13 C). Then, 13 C content increased again with noticeable “depletion” events in the middle of the growth period. A gradual 13 C accumulation took place in the second half of the vegetation period. Similar effects were observed both in the light and in the dark with some temporal shifts. Environmental factors did not influence the δ13C values. A gradual 12C-depletion effect was noticed in needles of the previous year. The δ13C values of sucrose and proteins from needle biomass altered independently from each other in the light chamber. A distinct negative correlation between δ13C and δ18O values was revealed for all studied variables. Conclusions The abrupt 13C depletion recorded by all tested trees for the period from June to July provides clear evidence of the transition from the dominant role of reserve carbohydrate pool (RCP) during the first half of the growth season to the preferable current year carbohydrate pool (CCP) consumption by new needles during its second half. The investigation of the isotopic signatures of Pinus sylvestris L. emphasizes the pivotal role of the intra-seasonal dynamics in carbon metabolism through the transport of assimilates from autotrophic (needles) to heterotrophic (twigs) organs of the studied trees. This provides an explanation for changes of carbon isotopic values observed within the growth season. The CMOM-based results support the hypothesis of the integration of three carbohydrate pools by photosynthesizing cells. The fluctuations of the carbon isotope ratios in different carbohydrate pools underlie various physiological processes in the tree metabolism. The possible mechanisms and pathways of formation of these carbohydrate pools are further discussed. Hence, CMOM provides a reasonable explanation for the absence of the impact of environmental conditions on the needle isotopic variables, the 12C-depletion effects and the use of RCP in needles. The model explains the negative connections between δ13C and δ18O values in all studied variables. PMID:22646756

Natural abundance deuterium and 18-oxygen effects on the precision of the doubly labeled water method

NASA Technical Reports Server (NTRS)

Horvitz, M. A.; Schoeller, D. A.

2001-01-01

The doubly labeled water method for measuring total energy expenditure is subject to error from natural variations in the background 2H and 18O in body water. There is disagreement as to whether the variations in background abundances of the two stable isotopes covary and what relative doses of 2H and 18O minimize the impact of variation on the precision of the method. We have performed two studies to investigate the amount and covariance of the background variations. These were a study of urine collected weekly from eight subjects who remained in the Madison, WI locale for 6 wk and frequent urine samples from 14 subjects during round-trip travel to a locale > or = 500 miles from Madison, WI. Background variation in excess of analytical error was detected in six of the eight nontravelers, and covariance was demonstrated in four subjects. Background variation was detected in all 14 travelers, and covariance was demonstrated in 11 subjects. The median slopes of the regression lines of delta2H vs. delta18O were 6 and 7, respectively. Modeling indicated that 2H and 18O doses yielding a 6:1 ratio of final enrichments should minimize this error introduced to the doubly labeled water method.

Natural abundance deuterium and 18-oxygen effects on the precision of the doubly labeled water method.

PubMed

Horvitz, M A; Schoeller, D A

2001-06-01

The doubly labeled water method for measuring total energy expenditure is subject to error from natural variations in the background 2H and 18O in body water. There is disagreement as to whether the variations in background abundances of the two stable isotopes covary and what relative doses of 2H and 18O minimize the impact of variation on the precision of the method. We have performed two studies to investigate the amount and covariance of the background variations. These were a study of urine collected weekly from eight subjects who remained in the Madison, WI locale for 6 wk and frequent urine samples from 14 subjects during round-trip travel to a locale > or = 500 miles from Madison, WI. Background variation in excess of analytical error was detected in six of the eight nontravelers, and covariance was demonstrated in four subjects. Background variation was detected in all 14 travelers, and covariance was demonstrated in 11 subjects. The median slopes of the regression lines of delta2H vs. delta18O were 6 and 7, respectively. Modeling indicated that 2H and 18O doses yielding a 6:1 ratio of final enrichments should minimize this error introduced to the doubly labeled water method.

Differentiation among Multiple Sources of Anthropogenic Nitrate in a Complex Groundwater System using Dual Isotope Systematics: A case study from Mortandad Canyon, New Mexico

NASA Astrophysics Data System (ADS)

Larson, T. E.; Perkins, G.; Longmire, P.; Heikoop, J. M.; Fessenden, J. E.; Rearick, M.; Fabyrka-Martin, J.; Chrystal, A. E.; Dale, M.; Simmons, A. M.

2009-12-01

The groundwater system beneath Los Alamos National Laboratory has been affected by multiple sources of anthropogenic nitrate contamination. Average NO3-N concentrations of up to 18.2±1.7 mg/L have been found in wells in the perched intermediate aquifer beneath one of the more affected sites within Mortandad Canyon. Sources of nitrate potentially reaching the alluvial and intermediate aquifers include: (1) sewage effluent, (2) neutralized nitric acid, (3) neutralized 15N-depleted nitric acid (treated waste from an experiment enriching nitric acid in 15N), and (4) natural background nitrate. Each of these sources is unique in δ18O and δ15N space. Using nitrate stable isotope ratios, a mixing model for the three anthropogenic sources of nitrate was established, after applying a linear subtraction of the background component. The spatial and temporal variability in nitrate contaminant sources through Mortandad Canyon is clearly shown in ternary plots. While microbial denitrification has been shown to change groundwater nitrate stable isotope ratios in other settings, the redox potential, relatively high dissolved oxygen content, increasing nitrate concentrations over time, and lack of observed NO2 in these wells suggest minimal changes to the stable isotope ratios have occurred. Temporal trends indicate that the earliest form of anthropogenic nitrate in this watershed was neutralized nitric acid. Alluvial wells preserve a trend of decreasing nitrate concentrations and mixing models show decreasing contributions of 15N-depleted nitric acid. Nearby intermediate wells show increasing nitrate concentrations and mixing models indicate a larger component derived from 15N-depleted nitric acid. These data indicate that the pulse of neutralized 15N-depleted nitric acid that was released into Mortandad Canyon between 1986 and 1989 has infiltrated through the alluvial aquifer and is currently affecting two intermediate wells. This hypothesis is consistent with previous research suggesting that the perched intermediate aquifers in the Mortandad Canyon watershed are recharged locally from the overlying alluvial aquifers.

Mixing ratio and carbon isotopic composition investigation of atmospheric CO2 in Beijing, China.

PubMed

Pang, Jiaping; Wen, Xuefa; Sun, Xiaomin

2016-01-01

The stable isotope composition of atmospheric CO2 can be used as a tracer in the study of urban carbon cycles, which are affected by anthropogenic and biogenic CO2 components. Continuous measurements of the mixing ratio and δ(13)C of atmospheric CO2 were conducted in Beijing from Nov. 15, 2012 to Mar. 8, 2014 including two heating seasons and a vegetative season. Both δ(13)C and the isotopic composition of source CO2 (δ(13)CS) were depleted in the heating seasons and enriched in the vegetative season. The diurnal variations in the CO2 mixing ratio and δ(13)C contained two peaks in the heating season, which are due to the effects of morning rush hour traffic. Seasonal and diurnal patterns of the CO2 mixing ratio and δ(13)C were affected by anthropogenic emissions and biogenic activity. Assuming that the primary CO2 sources at night (22:00-04:00) were coal and natural gas combustion during heating seasons I and II, an isotopic mass balance analysis indicated that coal combustion had average contributions of 83.83±14.11% and 86.84±12.27% and that natural gas had average contributions of 16.17±14.11% and 13.16±12.27%, respectively. The δ(13)C of background CO2 in air was the main error source in the isotopic mass balance model. Both the mixing ratio and δ(13)C of atmospheric CO2 had significant linear relationships with the air quality index (AQI) and can be used to indicate local air pollution conditions. Energy structure optimization, for example, reducing coal consumption, will improve the local air conditions in Beijing. Copyright © 2015 Elsevier B.V. All rights reserved.

Mixing ratio and carbon isotopic composition investigation of atmospheric CO2 in Beijing, China

NASA Astrophysics Data System (ADS)

Pang, J.; Wen, X.; Sun, X.

2016-12-01

The stable isotope composition of atmospheric CO2 can be used as a tracer in the study of urban carbon cycles, which are affected by anthropogenic and biogenic CO2 components. Continuous measurements of the mixing ratio and δ13C of atmospheric CO2 were conducted in Beijing from Nov. 15, 2012 to Mar. 8, 2014 including two heating seasons and a vegetative season. Both δ13C and the isotopic composition of source CO2 (δ13CS) were depleted in the heating seasons and enriched in the vegetative season. The diurnal variations in the CO2 mixing ratio and δ13C contained two peaks in the heating season, which are due to the effects of morning rush hour traffic. Seasonal and diurnal patterns of the CO2 mixing ratio and δ13C were affected by anthropogenic emissions and biogenic activity. Assuming that the primary CO2 sources at night (22:00-04:00) were coal and natural gas combustion during heating seasons I and II, an isotopic mass balance analysis indicated that coal combustion had average contributions of 83.83 ± 14.11% and 86.84 ± 12.27% and that natural gas had average contributions of 16.17 ± 14.11% and 13.16 ± 12.27%, respectively. The δ13C of background CO2 in air was the main error source in the isotopic mass balance model. Both the mixing ratio and δ13C of atmospheric CO2 had significant linear relationships with the air quality index (AQI) and can be used to indicate local air pollution conditions. Energy structure optimization, for example, reducing coal consumption, will improve the local air conditions in Beijing.

SO2 photoexcitation mechanism links mass-independent sulfur isotopic fractionation in cryospheric sulfate to climate impacting volcanism

PubMed Central

Hattori, Shohei; Schmidt, Johan A.; Johnson, Matthew S.; Danielache, Sebastian O.; Yamada, Akinori; Ueno, Yuichiro; Yoshida, Naohiro

2013-01-01

Natural climate variation, such as that caused by volcanoes, is the basis for identifying anthropogenic climate change. However, knowledge of the history of volcanic activity is inadequate, particularly concerning the explosivity of specific events. Some material is deposited in ice cores, but the concentration of glacial sulfate does not distinguish between tropospheric and stratospheric eruptions. Stable sulfur isotope abundances contain additional information, and recent studies show a correlation between volcanic plumes that reach the stratosphere and mass-independent anomalies in sulfur isotopes in glacial sulfate. We describe a mechanism, photoexcitation of SO2, that links the two, yielding a useful metric of the explosivity of historic volcanic events. A plume model of S(IV) to S(VI) conversion was constructed including photochemistry, entrainment of background air, and sulfate deposition. Isotopologue-specific photoexcitation rates were calculated based on the UV absorption cross-sections of 32SO2, 33SO2, 34SO2, and 36SO2 from 250 to 320 nm. The model shows that UV photoexcitation is enhanced with altitude, whereas mass-dependent oxidation, such as SO2 + OH, is suppressed by in situ plume chemistry, allowing the production and preservation of a mass-independent sulfur isotope anomaly in the sulfate product. The model accounts for the amplitude, phases, and time development of Δ33S/δ34S and Δ36S/Δ33S found in glacial samples. We are able to identify the process controlling mass-independent sulfur isotope anomalies in the modern atmosphere. This mechanism is the basis of identifying the magnitude of historic volcanic events. PMID:23417298

Atmospheric pCO2 reconstructed across five early Eocene global warming events

NASA Astrophysics Data System (ADS)

Cui, Ying; Schubert, Brian A.

2017-11-01

Multiple short-lived global warming events, known as hyperthermals, occurred during the early Eocene (56-52 Ma). Five of these events - the Paleocene-Eocene Thermal Maximum (PETM or ETM1), H1 (or ETM2), H2, I1, and I2 - are marked by a carbon isotope excursion (CIE) within both marine and terrestrial sediments. The magnitude of CIE, which is a function of the amount and isotopic composition of carbon added to the ocean-atmosphere system, varies significantly between marine versus terrestrial substrates. Here we use the increase in carbon isotope fractionation by C3 land plants in response to increased pCO2 to reconcile this difference and reconstruct a range of background pCO2 and peak pCO2 for each CIE, provided two potential carbon sources: methane hydrate destabilization and permafrost-thawing/organic matter oxidation. Although the uncertainty on each pCO2 estimate using this approach is low (e.g., median uncertainty = + 23% / - 18%), this work highlights the potential for significant systematic bias in the pCO2 estimate resulting from sampling resolution, substrate type, diagenesis, and environmental change. Careful consideration of each of these factors is required especially when applying this approach to a single marine-terrestrial CIE pair. Given these limitations, we provide an upper estimate for background early Eocene pCO2 of 463 +248/-131 ppmv (methane hydrate scenario) to 806 +127/-104 ppmv (permafrost-thawing/organic matter oxidation scenario). These results, which represent the first pCO2 proxy estimates directly tied to the Eocene hyperthermals, demonstrate that early Eocene warmth was supported by background pCO2 less than ∼3.5× preindustrial levels and that pCO2 > 1000 ppmv may have occurred only briefly, during hyperthermal events.

Sulfur isotopic analysis of carbonyl sulfide and its application for biogeochemical cycles

NASA Astrophysics Data System (ADS)

Hattori, Shohei; Kamezaki, Kazuki; Ogawa, Takahiro; Toyoda, Sakae; Katayama, Yoko; Yoshida, Naohiro

2016-04-01

Carbonyl sulfide (OCS or COS) is the most abundant gas containing sulfur in the atmosphere, with an average mixing ratio of 500 p.p.t.v. in the troposphere. OCS is suggested as a sulfur source of the stratospheric sulfate aerosols (SSA) which plays an important role in Earth's radiation budget and ozone depletion. Therefore, OCS budget should be validated for prediction of climate change, but the global OCS budget is imbalance. Recently we developed a promising new analytical method for measuring the stable sulfur isotopic compositions of OCS using nanomole level samples: the direct isotopic analytical technique of on-line gas chromatography-isotope ratio mass spectrometry (GC-IRMS) using fragmentation ions S+ (Hattori et al., 2015). The first measurement of the δ34S value for atmospheric OCS coupled with isotopic fractionation for OCS sink reactions in the stratosphere (Hattori et al., 2011; Schmidt et al., 2012; Hattori et al., 2012) explains the reported δ34S value for background stratospheric sulfate, suggesting that OCS is a potentially important source for background (nonepisodic or nonvolcanic) stratospheric sulfate aerosols. This new method measuring δ34S values of OCS can be used to investigate OCS sources and sinks in the troposphere to better understand its cycle. It is known that some microorganisms in soil can degrade OCS, but the mechanism and the contribution to the OCS in the air are still uncertain. In order to determine sulfur isotopic enrichment factor of OCS during degradation via microorganisms, incubation experiments were conducted using strains belonging to the genera Mycobacterium, Williamsia and Cupriavidus, isolated from natural soil environments (Kato et al., 2008). As a result, sulfur isotope ratios of OCS were increased during degradation of OCS, indicating that reaction for OC32S is faster than that for OC33S and OC34S. OCS degradation via microorganisms is not mass-independent fractionation (MIF) process, suggesting that this reaction does not contribute to the MIF signatures observed in sulfate aerosol samples and/or Archaean rock records. At the presentation, we report the comparison of 34ɛ values determined using some strains and the atmospheric implications for the OCS degradation in the present atmosphere are discussed. Hattori, S., Danielache, S. O., Johnson, M. S., Schmidt, J. A., Kjaergaard, H. G., Toyoda, S., Ueno, Y., Yoshida, N. Ultraviolet absorption cross sections of carbonyl sulfide isotopologues OC32S, OC33S, OC34S and O13CS: isotopic fractionation in photolysis and atmospheric implications, Atmos. Chem. Phys., 11, 10293-10303, 2011. Schmidt, J. A., Johnson, M. S., Jung, Y., Danielache, S. O., Hattori, S., Yoshida, N., Predictions of the sulfur and carbon kinetic isotope effects in the OH + OCS reaction, Chem. Phys. Lett., 531, 64-69, 2012. Hattori, S., Schmidt J. A., Mahler D., Danielache, S. O., Johnson M. S., Yoshida N. Isotope Effect in the Carbonyl Sulfide Reaction with O(3P), J. Phys. Chem. A, 116, 3521-3526, 2012. Hattori, S., Toyoda, A., Toyoda, S., Ishino S., Ueno, Y., Yoshida, N.: Determination of the Sulfur Isotope Ratio in Carbonyl Sulfide using Gas Chromatography/Isotope Ratio Mass Spectrometry on Fragment Ions 32S+, 33S+, and 34S+, Anal. Chem., 87, 477-484, 2015. Kato, H., Saito, M., Nagahata, Y., Katayama, Y.: Degradation of ambient carbonyl sulfide by Mycobacterium spp. in soil. Microbiol., 154(1), 249-255, 2008.

The detailed analysis of natural radionuclides dissolved in spa waters of the Kłodzko Valley, Sudety Mountains, Poland.

PubMed

Walencik-Łata, A; Kozłowska, B; Dorda, J; Przylibski, T A

2016-11-01

A survey was conducted to measure natural radioactivity in spa waters from the Kłodzko Valley. The main goal of this study was to determine the activity concentration of uranium, radium and radon isotopes in the investigated groundwaters. Samples were collected several times from 35 water intakes from 5 spas and 2 mineral water bottling plants. The authors examined whether the increased gamma radiation background, as well as the elevated values of radium and uranium content in reservoir rocks, have a significant impact on the natural radioactivity of these waters. The second objective of this research was to provide information about geochemistry of U, Ra, Rn radionuclides and the radiological and chemical risks incurred by ingestion of isotopes with drinking water. On the basis of results obtained, it is feasible to assess the health hazard posed by ingestion of natural radioactivity with drinking waters. Moreover, the data yielded by this research may be helpful in the process of verification of the application of these waters in balneotherapy. In addition, annual effective radiation doses resulting from the isotopes consumption were calculated on the basis of the evaluated activity concentrations. In dose assessment for uranium and radium isotopes, the authors provided values for different human age groups. The obtained uranium content in the investigated waters was compared with the currently valid regulations concerning the quality of drinking water. Based on the activity concentrations data, the activity isotopic ratios (234)U/(238)U, (226)Ra/(238)U, (222)Rn/(238)U, (222)Rn/(226)Ra and the correlations between radionuclides content were then examined. In brief, it may be concluded on the basis of the obtained results that radon solubility is inversely proportional to radium and uranium dissolution in environmental water circulation. The presented study allows conclusions to be drawn on the radionuclide circulation among different environmental biota: from lithosphere through hydrosphere to biosphere. Copyright © 2016 Elsevier B.V. All rights reserved.

Hydrogen stable isotopic constraints on methane emissions from oil and gas extraction in the Colorado Front Range, USA

NASA Astrophysics Data System (ADS)

Townsend-Small, A.; Botner, E. C.; Jimenez, K.; Blake, N. J.; Schroeder, J.; Meinardi, S.; Barletta, B.; Simpson, I. J.; Blake, D. R.; Flocke, F. M.; Pfister, G.; Bon, D.; Crawford, J. H.

2015-12-01

The climatic implications of a shift from oil and coal to natural gas depend on the magnitude of fugitive emissions of methane from the natural gas supply chain. Attempts to constrain methane emissions from natural gas production regions can be confounded by other sources of methane. Here we demonstrate the utility of stable isotopes, particularly hydrogen isotopes, for source apportionment of methane emissions. The Denver, Colorado area is home to a large oil and gas field with both conventional oil and gas wells and newer hydraulic fracturing wells. The region also has a large metropolitan area with several landfills and a sizable cattle population. As part of the DISCOVER-AQ and FRAPPE field campaigns in summer 2014, we collected three types of canister samples for analysis of stable isotopic composition of methane: 1), samples from methane sources; 2), samples from two stationary ground sites, one in the Denver foothills, and one in an oil and gas field; and 3), from the NCAR C-130 aircraft in samples upwind and downwind of the region. Our results indicate that hydrogen isotope ratios are excellent tracers of sources of methane in the region, as we have shown previously in California and Texas. Use of carbon isotope ratios is complicated by the similarity of natural gas isotope ratios to that of background methane. Our results indicate that, despite the large amount of natural gas production in the region, biological sources such as cattle feedlots and landfills account for at least 50% of total methane emissions in the Front Range. Future work includes comparison of isotopes and alkane ratios as tracers of methane sources, and calculation of total methane fluxes in the region using continuous measurements of methane concentrations during aircraft flights.

Radiogenic isotopic approaches for quantifying radionuclide transport (Invited)

NASA Astrophysics Data System (ADS)

Maher, K.; Depaolo, D. J.; Singleton, M. J.; Christensen, J. N.; Conrad, M. E.

2009-12-01

Naturally occurring variations in the isotopic compositions of U and Sr provide unique opportunities for assessing the fate and transport of radionuclides at field-scale conditions. When coupled with reactive transport models, U and Sr isotopes may also provide additional constraints on the rates of sediment-fluid or sediment-waste interactions. Such isotopic approaches can be useful for sites where subsurface characterization is complicated by a lack of accessibility or the presence of substantial heterogeneity. In addition, a variety of quantitative modeling approaches of different complexity can be used to evaluate experimentally determined parameters for radionuclide mobility at the field-scale. At the Hanford Site in eastern Washington, 87Sr/86Sr and 234U/238U ratios have been used to quantify the residence time of Sr and U in the unsaturated zone, the long-term background infiltration rate through the unsaturated zone, and to assess the influence of enhanced wastewater discharge on the regional unconfined aquifer. As a result of different processing techniques or due to interactions between caustic waste and the natural sediment, waste plumes may also inherit isotopic fingerprints (e.g. 234U/238U, 235U/238U, 236U/238U; δ15N & δ18O of nitrate) that can be used to resolve multiple sources of contamination. Finally, enriched isotopic tracers can be applied to experimental manipulations to assess the retardation of a variety of contaminants. Collectively this isotopic data contributes unique perspectives on both the hydrologic conditions across the site and the mobility of key radionuclides. Predicting the long-term fate and transport of radionuclides in the environment is often challenging due to natural heterogeneity and incomplete characterization of the subsurface, however detailed analysis of isotopic variations can provide one additional means of characterizing the subsurface.

The Cd and Zn Isotope Compositions of PM10 in the Atmosphere of Paris: New Tools for Discrimination and Tracking of the Origin of Metallic Pollution

NASA Astrophysics Data System (ADS)

Petelet-Giraud, E.; Widory, D.; Innocent, C.; Quetel, C.; Le Bihan, O.; Fraboulet, I.; Forti, L.; Joos, E.; Goupil, G.; Canard, E.

2008-12-01

Due to their relatively high concentration in urban environments (from 10 to more than 50 μg.m-3), atmospheric particles (PM10) have potential damaging effects on the Public Health. Hence, the development of measures dealing with fine particulate matter is considered a priority by the EU Clean Air For Europe (CAFE) Program. Still, the origin of these airborne particles is subject to debate, as classical chemical methods showed their limitations. Recent studies have shown that stable isotopes of elements such as carbon, nitrogen or lead could be of great help in the search of new particle air pollution tracking tools. We will present here preliminary results on the pioneer use of stable isotope compositions of cadmium, zinc and mercury to help decipher the different possible origins of PM10 pollution in the atmosphere of Paris (France). Main potential sources were characterized: (1) waste incineration, (2) road traffic, (3) central heating and (4) coal-fired power plants. Results show that the use of cadmium (d114Cd) and zinc (d66Zn) isotopes, and the combination of both provides a reliable and precise tool for discriminating the different families of particle vectors. The isotope systematic of mercury (d200Hg) is more difficult to apprehend due to the low levels encountered (mercury is mainly present under gaseous form, but is still observed at low concentrations in particles), but does show significant variations between the different sources. Daily cumulative air samples were taken on three different locations, covering different scenarios in Paris city: 1) background pollution in Paris, 2) under the plume of a major pollution source and 3) Paris vicinity. Corresponding chemical and isotope analyses help identify the main vectors for the three elements (Cd, Zn and Hg) considered as well as assess their respective contributions to the levels of pollution observed.

Interrogating Host-virus Interactions and Elemental Transfer Using NanoSIMS

NASA Astrophysics Data System (ADS)

Pasulka, A.; Thamatrakoln, K.; Poulos, B.; Bidle, K. D.; Sullivan, M. B.; Orphan, V. J.

2016-02-01

Marine viruses (bacteriophage and eukaryotic viruses) impact microbial food webs by influencing microbial community structure, carbon and nutrient flow, and serving as agents of gene transfer. While the collective impact of viral activity has become more apparent over the last decade, there is a growing need for single-cell and single-virus level measurements of the associated carbon and nitrogen transfer, which ultimately shape the biogeochemical impact of viruses in the upper ocean. Stable isotopes have been used extensively for understanding trophic relationships and elemental cycling in marine food webs. While single-cell isotope approaches such as nanoscale secondary ion mass spectrometry (nanoSIMS) have been more readily used to study trophic interactions between microorganisms, isotopic enrichment in viruses has not been described. Here we used nanoSIMS to quantify the transfer of stable isotopes (13C and 15N) from host to individual viral particles in two distinct unicellular algal-virus model systems. These model systems represent a eukaryotic phytoplankton (Emiliania huxleyi strain CCMP374) and its 200nm coccolithovirus (EhV207), as well as a cyanobacterial phytoplankton (Synechococcus WH8101) and its 80nm virus (Syn1). Host cells were grown on labeled media for multiple generations, subjected to viral infection, and then viruses were harvested after lysis. In both cases, nanoSIMS measurements were able to detect 13C and 15N in the resulting viral particles significantly above the background noise. The isotopic enrichment in the viral particles mirrored that of the host. Through use of these laboratory model systems, we quantified the sensitivity (ion counts), spatial resolution, and reproducibility, including sources of methodological and biological variability, in stable isotope incorporation into viral particles. Our findings suggest that nanoSIMS can be successfully employed to directly probe virus-host interactions at the resolution of individual viral particles and quantify the amount of carbon and nitrogen transferred into viruses during infection of autotrophic phytoplankton.

Isotope dilution inductively coupled plasma quadrupole mass spectrometry in connection with a chromatographic separation for ultra trace determinations of platinum group elements (Pt, Pd, Ru, Ir) in environmental samples.

PubMed

Müller, M; Heumann, K G

2000-09-01

An isotope dilution inductively coupled plasma quadrupole mass spectrometric (ID-ICP-QMS) method was developed for the simultaneous determination of the platinum group elements Pt, Pd, Ru, and Ir in environmental samples. Spike solutions, enriched with the isotopes 194Pt, 108Pd, 99Ru, and 191Ir, were used for the isotope dilution step. Interfering elements were eliminated by chromatographic separation using an anion-exchange resin. Samples were dissolved with aqua regia in a high pressure asher. Additional dissolution of possible silicate portions by hydrofluoric acid was usually not necessary. Detection limits of 0.15 ng x g(-1), 0.075 ng x g(-1), and 0.015 ng x g(-1) were achieved for Pt, Pd, Ru, and Ir, respectively, using sample weights of only 0.2 g. The reliability of the ID-ICP-QMS method was demonstrated by analyzing a Canadian geological reference material and by participating in an interlaboratory study for the determination of platinum and palladium in a homogenized road dust sample. Surface soil, sampled at different distances from a highway, showed concentrations in the range of 0.1-87 ng x g(-1). An exponential decrease of the platinum and palladium concentration with increasing distance and a small anthropogenic contribution to the natural background concentration of ruthenium and iridium was found in these samples.

Tracing Waste Water with Li isotopes

NASA Astrophysics Data System (ADS)

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.

Microscopic description of triaxiality in Ru isotopes with covariant energy density functional theory

NASA Astrophysics Data System (ADS)

Shi, Z.; Li, Z. P.

2018-03-01

Background: Triaxiality in nuclear low-lying states has attracted great interest for many years. Recently, reduced transition probabilities for levels near the ground state in 110Ru have been measured and provided strong evidence of a triaxial shape of this nucleus. Purpose: The aim of this work is to provide a microscopic study of low-lying states for Ru isotopes with A ≈100 and to examine in detail the role of triaxiality and the evolution of quadrupole shapes with the isospin and spin degrees of freedom. Method: Low-lying excitation spectra and transition probabilities of even-even Ru isotopes are described at the beyond-mean-field level by solving a five-dimensional collective Hamiltonian with parameters determined by constrained self-consistent mean-field calculations based on the relativistic energy density functional PC-PK1. Results: The calculated energy surfaces, low-energy spectra, and intraband and interband transition rates, as well as some characteristic collective observables, such as E (4g.s . +) /E (2g.s . +) ,E (2γ+) /E (4g.s . +) , and B (E 2 ;2g.s . +→0g.s . +) and γ -band staggerings, are in good agreement with the available experimental data. Conclusions: The main features of the experimental low-lying excitation spectra and electric transition rates are well reproduced and, thus, strongly support the onset of triaxiality in the low-lying excited states of Ru isotopes around 110Ru.

Heavy metals pollution and pb isotopic signatures in surface sediments collected from Bohai Bay, North China.

PubMed

Gao, Bo; Lu, Jin; Hao, Hong; Yin, Shuhua; Yu, Xiao; Wang, Qiwen; Sun, Ke

2014-01-01

To investigate the characteristics and potential sources of heavy metals pollution, surface sediments collected from Bohai Bay, North China, were analyzed for the selected metals (Cd, Cr, Cu, Ni, Pb, and Zn). The Geoaccumulation Index was used to assess the level of heavy metal pollution. Pb isotopic compositions in sediments were also measured to effectively identify the potential Pb sources. The results showed that the average concentrations of Cd, Cr, Cu, Ni, Pb, and Zn were 0.15, 79.73, 28.70, 36.56, 25.63, and 72.83 mg/kg, respectively. The mean concentrations of the studied metals were slightly higher than the background values. However, the heavy metals concentrations in surface sediments in Bohai Bay were below the other important bays or estuaries in China. The assessment by Geoaccumulation Index indicated that Cr, Zn, and Cd were classified as "the unpolluted" level, while Ni, Cu, and Pb were ranked as "unpolluted to moderately polluted" level. The order of pollution level of heavy metals was: Pb > Ni > Cu > Cr > Zn > Cd. The Pb isotopic ratios in surface sediments varied from 1.159 to 1.185 for (206)Pb/(207)Pb and from 2.456 to 2.482 for (208)Pb/(207)Pb. Compared with Pb isotopic radios in other sources, Pb contaminations in the surface sediments of Bohai Bay may be controlled by the mix process of coal combustion, aerosol particles deposition, and natural sources.

Metal enrichment and lead isotope analysis for source apportionment in the urban dust and rural surface soil.

PubMed

Yu, Yang; Li, Yingxia; Li, Ben; Shen, Zhenyao; Stenstrom, Michael K

2016-09-01

To understand the metal accumulation in the environment and identify its sources, 29 different metal contents and lead (Pb) isotope ratios were determined for 40 urban dust samples, 36 surface soil samples, and one river sediment sample collected in the municipality of Beijing, China. Results showed that cadmium, copper (Cu), mercury, Pb, antimony (Sb), and zinc demonstrated to be the typical urban contaminants and mostly influenced by the adjacent human activities with higher content to background ratios and SD values. Among the 29 metal elements investigated, Cu and Sb were found to be the most distinct elements that were highly affected by the developing level and congestion status of the cities with much higher contents in dust in more developed and congested cities. There was a relatively wider range of Pb isotope ratios of country surface soil than those of urban dust. The results of source identification based on Pb isotope ratios showed that coal combustion was the first largest Pb source and vehicle exhaust was the second largest source. The sum of them accounted for 74.6% mass proportion of overall Pb pollution on average. The surface soil sample collected at an iron mine had the highest (204)Pb/(206)Pb, (207)Pb/(206)Pb, and (208)Pb/(206)Pb ratios indicating ore had much higher ratios than other sources. The fine particle subsamples had higher (204)Pb/(206)Pb, (207)Pb/(206)Pb, and (208)Pb/(206)Pb ratios than the coarse particle subsamples indicating more anthropogenic sources of coal combustion and vehicle exhaust for fine particles and more background influence for coarse particles. These results help with pinpointing the major Pb sources and applying suitable measures for the target sources. Copyright © 2016 Elsevier Ltd. All rights reserved.

Springtime carbon emission episodes at the Gosan background site revealed by total carbon, stable carbon isotopic composition, and thermal characteristics of carbonaceous particles

NASA Astrophysics Data System (ADS)

Jung, J.; Kawamura, K.

2011-11-01

In order to investigate the emission of carbonaceous aerosols at the Gosan background super-site (33.17° N, 126.10° E) in East Asia, total suspended particles (TSP) were collected during spring of 2007 and 2008 and analyzed for particulate organic carbon, elemental carbon, total carbon (TC), total nitrogen (TN), and stable carbon isotopic composition (δ13C) of TC. The stable carbon isotopic composition of TC (δ13CTC) was found to be lowest during pollen emission episodes (range: -26.2‰ to -23.5‰, avg. -25.2 ± 0.9‰), approaching those of the airborne pollen (-28.0‰) collected at the Gosan site. Based on a carbon isotope mass balance equation, we found that ~42% of TC in the TSP samples during the pollen episodes was attributed to airborne pollen from Japanese cedar trees planted around tangerine farms in Jeju Island. A negative correlation between the citric acid-carbon/TC ratios and δ13CTC was obtained during the pollen episodes. These results suggest that citric acid emitted from tangerine fruit may be adsorbed on the airborne pollen and then transported to the Gosan site. Thermal evolution patterns of organic carbon during the pollen episodes were characterized by high OC evolution in the OC2 temperature step (450 °C). Since thermal evolution patterns of organic aerosols are highly influenced by their molecular weight, they can be used as additional information on the formation of secondary organic aerosols and the effect of aging of organic aerosols during the long-range atmospheric transport and sources of organic aerosols.

Monitoring steel bridge renovation using lead isotopic tracing.

PubMed

Salome, Fred; Gulson, Brian; Chiaradia, Massimo; Davis, Jeffrey; Morris, Howard

2017-05-01

Monitoring removal of lead (Pb) paint from steel structures usually involves analysis of environmental samples for total lead and determination of blood Pb levels of employees involved in the Pb paint removal. We used high precision Pb isotopic tracing for a bridge undergoing Pb paint removal to determine if Pb in the environmental and blood samples originated from the bridge paint. The paint system on the bridge consisted of an anti-corrosive red Pb primer top-coated with a Micaceous Iron Oxide (MIO) alkyd. Analysis of the red Pb primer gave uniform isotopic ratios indicative of Pb from the geologically-ancient Broken Hill mines in western New South Wales, Australia. Likewise waste abrasive material, as anticipated, had the same isotopic composition as the paint. The isotopic ratios for other samples lay on 2 separate linear arrays on a 207 Pb/ 204 Pb versus 206 Pb/ 204 Pb diagram, one largely defined by gasoline and the majority of the ambient air data, and the other by data for one sample each of gasoline and ambient air and underwater sediments. Isotopic ratios in background ambient air samples for the project were characteristic of leaded gasoline. Air sampling during paint removal showed a contribution of paint Pb ranging from about 20 to 40%. Isotopic ratios in the blood of 8 employees prior to the commencement of work showed that 6 of these had been previously exposed to the Broken Hill Pb possibly from earlier bridge paint removal projects. One subject appeared to have increased exposure to Pb probably from the paint renovations. Copyright © 2017 Elsevier Ltd. All rights reserved.

A European lead isotope signal recorded from 6000 to 300 years BP in coastal marshes (SW France)

NASA Astrophysics Data System (ADS)

Alfonso, S.; Grousset, F.; Massé, L.; Tastet, J.-P.

Cores covering the last 6000 years were recovered from two marshes from south-western France. They were studied in an attempt to build a reliable regional record of heavy metal pollution. The cores were dated using 14C and historical data. Both Pb concentrations and Pb isotopic composition ( 206Pb/ 207Pb and 208Pb/ 206Pb) were measured in bulk sediment samples using the inductively coupled plasma-mass spectrometer technique. The evolution of the 206Pb/ 207Pb ratio recorded in both marshes reveals a good correlation with the worldwide Pb production during the last 5000 years. The lead isotopic records reveal some general trends, along with a few typical events such as the imprints of the pre-anthropogenic background between 6000 and 2300 years BP, the mining activity during the Roman and Greek periods from 2300 to 1700 years BP, the fall of the Roman Empire and the mining activity in Central Europe since the 11th century AD. These results are also consistent with records obtained in other European environments. Consequently, the European atmospheric signal is recorded in these marshes, hiding expected local riverine contributions. Thus, such records may contribute to the construction of a chronological standard curve for continental environments. However, it will be necessary to study other records more accurately dated to obtain an adequate precision before such a reference curve can be set-up.

Conditional CO2 flux analysis of a managed grassland with the aid of stable isotopes

NASA Astrophysics Data System (ADS)

Zeeman, M. J.; Tuzson, B.; Emmenegger, L.; Knohl, A.; Buchmann, N.; Eugster, W.

2009-04-01

Short statured managed ecosystems, such as agricultural grasslands, exhibit high temporal changes in carbon dioxide assimilation and respiration fluxes for which measurements of the net CO2 flux, e.g. by using the eddy covariance (EC) method, give only limited insight. We have therefore adopted a recently proposed concept for conditional EC flux analysis of forest to grasslands, in order to identify and quantify daytime sub-canopy respiration fluxes. To validate the concept, high frequency (≈5 Hz) stable carbon isotope analyis of CO2 was used. We made eddy covariance measurements of CO2 and its isotopologues during four days in August 2007, using a novel quantum cascade laser absorption spectrometer, capable of high time resolution stable isotope analysis. The effects of a grass cut during the measurement period could be detected and resulted in a sub-canopy source conditional flux classification, for which the isotope composition of the CO2 could be confirmed to be of a respiration source. However, the conditional flux method did not work for an undisturbed grassland canopy. We attribute this to the flux measurement height that was chosen well above the roughness sublayer, where the natural isotopic tracer (δ13C) of respiration was too well mixed with background air.

Lead isotope ratios in tree bark pockets: an indicator of past air pollution in the Czech Republic.

PubMed

Conkova, M; Kubiznakova, J

2008-10-15

Tree bark pockets were collected at four sites in the Czech Republic with differing levels of lead (Pb) pollution. The samples, spanning 1923-2005, were separated from beech (Fagus sylvatica) and spruce (Picea abies). Elevated Pb content (0.1-42.4 microg g(-1)) reflected air pollution in the city of Prague. The lowest Pb content (0.3-2.6 microg g(-1)) was found at the Kosetice EMEP "background pollution" site. Changes in (206)Pb/(207)Pb and (208)Pb/(206)Pb isotope ratios were in agreement with operation times of the Czech main anthropogenic Pb sources. Shortly after the Second World War, the (206)Pb/(207)Pb isotope ratio in bark pockets decreased from 1.17 to 1.14 and the (208)Pb/(206)Pb isotope ratio increased from 2.12 to 2.16. Two dominant emission sources responsible for these changes, lignite and leaded petrol combustion, contributed to the shifts in Pb isotope ratios. Low-radiogenic petrol Pb ((206)Pb/(207)Pb of 1.11) lead to lower (206)Pb/(207)Pb in bark pockets over time. High-radiogenic lignite-derived Pb ((206)Pb/(207)Pb of 1.18 to 1.19) was detected in areas affected by coal combustion rather than by traffic.

Validation of a single biopsy approach and bolus protein feeding to determine myofibrillar protein synthesis in stable isotope tracer studies in humans

PubMed Central

2011-01-01

Background Minimizing the number of muscle biopsies has important methodological implications and minimizes subject discomfort during a stable isotope amino acid infusion. We aimed to determine the reliability of obtaining a single muscle biopsy for the calculation of muscle protein fractional synthetic rate (FSR) as well as the amount of incorporation time necessary to obtain that biopsy after initiating a stable isotope infusion (Study 1). The calculation of muscle protein FSR requires tracer steady-state during the stable isotope infusion. Therefore, a second aim was to examine if steady-state conditions are compromised in the precursor pools (plasma free or muscle intracellular [IC]) after ingestion of a tracer enriched protein drink and after resistance exercise (Study 2). Methods Sixteen men (23 ± 3 years; BMI = 23.8 ± 2.2 kg/m2, means ± SD) were randomized to perform Study 1 or Study 2 (n = 8, per study). Subjects received a primed, constant infusion of L-[ring-13C6]phenylalanine coupled with muscle biopsies of the vastus lateralis to measure rates of myofibrillar protein synthesis (MPS). Subjects in Study 2 were fed 25 g of whey protein immediately after an acute bout of unilateral resistance exercise. Results There was no difference (P = 0.3) in rates of MPS determined using the steady-state precursor-product equation and determination of tracer incorporation between sequential biopsies 150 min apart or using plasma protein as the baseline enrichment, provided the infusion length was sufficient (230 ± 0.3 min). We also found that adding a modest amount of tracer (4% enriched), calculated based on the measured phenylalanine content of the protein (3.5%) in the drink, did not compromise steady-state conditions (slope of the enrichment curve not different from zero) in the plasma free or, more importantly, the IC pool (both P > 0.05). Conclusions These data demonstrate that the single biopsy approach yields comparable rates of muscle protein synthesis, provided a longer incorporation time is utilized, to that seen with a traditional two biopsy approach. In addition, we demonstrate that enriching protein-containing drinks with tracer does not disturb isotopic steady-state and thus both are reliable techniques to determine rates of MPS in humans. PMID:21388545

Stable isotope distribution in precipitation in Romania and its relevance for palaeoclimatic studies

NASA Astrophysics Data System (ADS)

Perşoiu, Aurel; Nagavciuc, Viorica; Bădăluţă, Carmen

2014-05-01

A surge of recent studies in Romania have targeted various aspects of palaeoclimate (based on stable isotopes in ice, speleothems, tree rings), mineral water origin, wine and other juices provenance. However, while much needed, these studies lack a stable isotope in precipitation background, with only two LMWL's being published so far. In this paper we discuss the links between the stable isotopic composition of precipitation (δ18O and δ2H), climate (air temperature, precipitation amount and large scale circulation) and their relevance for the palaeocllimatic interpretation of stable isotope values in cave ice, cryogenic calcite and tree rings from different sites in Romania. Most of the precipitation in Romania is delivered by the Westerlies, bringing moisture from the North Atlantic; however, their influence is greatly reduced in the eastern half of the country where local evaporative sources play an important role in the precipitation balance. The SW is dominated by water masses from the Mediterranean Sea, while the SE corner clearly draws most of the moisture from the Black Sea and strongly depleted North Atlantic vapor masses. In 2012, Romania experienced the worst draught in 60 years, possibly due to a northward shift of the jest stream associated to blocking conditions in summer, which led to a more northern penetration of the Mediterranean-derived air masses, as well increased precipitation of re-evaporated waters. We have further analyzed cave drip water (δ18O and δ2H), cryogenic cave calcite (δ18O and δ13C) and tree rings (δ18O and δ13C) from selected sites across NW Romania, where the water isotopes in precipitation showed the best (and easiest to understand, given the climatic conditions in 2012) correlation with climatic parameters. Our results that 1) δ18O and δ2H in cave ice are a good proxy for late summer through early winter air temperature; 2) δ13C in cryogenic cave calcite are possible indicators of soil humidity and 3) δ18O in pine tree rings is a good proxy for air temperature during the growing season. Acknowledgements: RO-2013-0014, LP2012-27/2012, PN-II-RU-TE-2011-3-0235.

Combining XAS speciation and Zn isotopes to track past eutrophication in lake sediments : The example of Baldeggersee (Switzerland)

NASA Astrophysics Data System (ADS)

Noël, V. S.; Voegelin, A.; Jouvin, D.; Louvat, P.; gelabert, A.; Mueller, B.; Benedetti, M. F.; Juillot, F.

2011-12-01

Among transition elements, Zn has attracted a great deal of interest because it is an essential nutrient at low concentrations, but it can also be toxic when present at high concentrations in ecosystems (Morel et al., 2003). In the present study, the isotopic signature and crystal-chemical of Zn were followed along a sediment core from a prealpine lake that experienced a marked eutrophication in order to explore the potential of this approach at tracking past environmental conditions of continental lake-catchment systems. Lake Baldeggersee (Luzern, Switzerland) is located at an elevation of 900 m in the Swiss Prealps. It experienced a period of strong eutrophication due to intensive farming in its catchment (Lotter et al., 1997). These led to the formation of varved sediments over one century prior to artificial lake aeration (Wehrli et al., 1997). This enabled us to correlate Zn speciation and isotopic signatures to the history of the water column. Results indicate that both Zn speciation and isotopes are distinct between sediments deposited during mesotrophic and eutrophic conditions in the water column: During the mesotrophic period, sedimentation was mainly detrital and Zn is mainly found associated with clay minerals in the sediments. During the eutrophic period, sedimentation was dominated by biological activity in the lake and Zn mainly occurs as ZnS in the sediments. Zn isotopes recorded these changes in the sedimentation regime, with δ66ZnJMC values around +0.2 % for the sediments of the mesotrophic period and δ66ZnJMC values around 0 % for the sediments of the eutrophic period. Comparison with the results from a study on the seasonal variation of the isotope signature of Zn in settling sediment of another prealpine lake (Peel et al., 2010) suggests that the enrichment in light Zn isotopes in the eutrophic sediments is in line with predominant Zn input with settling biomass (algae). Since lake eutrophication is mainly related to hydrological conditions and occupancy of the related catchment, these results emphasize the great potential of such a combination of molecular level speciation and Zn isotopes in lake sediments cores to track paleo-climatic or paleo-environmental conditions in lake catchments. Lotter A.F., Sturm M., Teranes J.L. and Wehrli B. (1997) Varve fromation since 1885 and high-resolution varve analyses in hypertrophic Baldeggersee (Switzerland) Aquatic Sciences 59, 304-325. Morel F. M. M. and Price N. M. (2003) The biogeochemical cycles of trace metals in the oceans. Science 300, 944-947. Peel K., Weiss D., Sigg L. (2010) Zinc isotope composition of settling particles as a proxy for biogeochemical processes in lakes: Insights from the eutrophic Lake Greifen, Switzerland. Limnol. Oceanogr., 54(5), 1699-1708. Wehrli, B.; Lotter, A.F.; Schaller, T.; Sturm, M. (1997) High-resolution varve studies in Baldeggersee (Switzerland): Project overview and limnological background data. Aquatic Sciences 59, 285-294).

Measurement of picosecond lifetimes in neutron-rich Xe isotopes

NASA Astrophysics Data System (ADS)

Ilieva, S.; Kröll, Th.; Régis, J.-M.; Saed-Samii, N.; Blanc, A.; Bruce, A. M.; Fraile, L. M.; de France, G.; Hartig, A.-L.; Henrich, C.; Ignatov, A.; Jentschel, M.; Jolie, J.; Korten, W.; Köster, U.; Lalkovski, S.; Lozeva, R.; Mach, H.; Mǎrginean, N.; Mutti, P.; Paziy, V.; Regan, P. H.; Simpson, G. S.; Soldner, T.; Thürauf, M.; Ur, C. A.; Urban, W.; Warr, N.

2016-09-01

Background: Lifetimes of nuclear excited states in fission fragments have been studied in the past following isotope separation, thus giving access mainly to the fragments' daughters and only to long-lived isomeric states in the primary fragments. For the first time now, short-lived excited states in the primary fragments, produced in neutron-induced prompt fission of 235U and 241Pu, were studied within the EXILL&FATIMA campaign at the intense neutron-beam facility of the Institute Laue-Langevin in Grenoble. Purpose: We aim to investigate the quadrupole collective properties of neutron-rich even-even 138,140,142Xe isotopes lying between the double shell closure N =82 and Z =50 and a deformed region with octupole collectivity. Method: The γ rays emitted from the excited fragments were detected with a mixed array consisting of 8 HPGe EXOGAM Clover detectors (EXILL) and 16 LaBr3(Ce) fast scintillators (FATIMA). The detector system has the unique ability to select the interesting fragment making use of the high resolution of the HPGe detectors and determine subnanosecond lifetimes using the fast scintillators. For the analysis the generalized centroid difference method was used. Results: We show that quadrupole collectivity increases smoothly with increasing neutron number above the closed N =82 neutron shell. Our measurements are complemented by state-of-the-art theory calculations based on shell-model descriptions. Conclusions: The observed smooth increase in quadrupole collectivity is similar to the evolution seen in the measured masses of the xenon isotopic chain and is well reproduced by theory. This behavior is in contrast to higher Z even-even nuclei where abrupt change in deformation occurs around N =90 .

Chromium Isotope Behaviour During Aerobic Microbial Reduction Activities

NASA Astrophysics Data System (ADS)

Zhang, Q.; Amor, K.; Porcelli, D.; Thompson, I.

2014-12-01

Microbial activity is a very important, and possibly even the dominant, reduction mechanism for many metals in natural water systems. Isotope fractionations during microbial metal reduction can reflect one major mechanism in metal cycling in the environment, and isotopic signatures can be used to identify and quantify reduction processes during biogeochemical cycling in the present environment as well as in the past. There are many Cr (VI)-reducing bacteria that have been discovered and isolated from the environment, and Cr isotopes were found to be fractionated during microbial reduction processes. In this study, Cr reduction experiments have been undertaken to determine the conditions under which Cr is reduced and the corresponding isotope signals that are generated. The experiments have been done with a facultative bacteria Pseudomonas fluorescens LB 300, and several parameters that have potential impact on reduction mechanisms have been investigated. Electron donors are important for bacteria growth and metabolism. One factor that can control the rate of Cr reduction is the nature of the electron donor. The results show that using citrate as an electron donor can stimulate bacteria reduction activity to a large extent; the reduction rate is much higher (15.10 mgˑL-1hour-1) compared with experiments using glucose (6.65 mgˑL-1ˑhour-1), acetate (4.88 mgˑL-1hour-1) or propionate (4.85 mgˑL-1hour-1) as electron donors. Groups with higher electron donor concentrations have higher reduction rates. Chromium is toxic, and when increasing Cr concentrations in the medium, the bacteria reduction rate is also higher, which reflects bacteria adapting to the toxic environment. In the natural environment, under different pH conditions, bacteria may metabolise in different ways. In our experiments with pH, bacteria performed better in reducing Cr (VI) when pH = 8, and there are no significant differences between groups with pH = 4 or pH = 6. To investigate this further, Cr isotope determinations will be presented, which are essential in better understanding bacterial reducing activities under different environmental conditions and can also provide important background information for interpreting Cr isotope fractionations in natural environment, and using Cr isotopes to identify reduction by microbial activity.

Tracking Cats: Problems with Placing Feline Carnivores on δ18O, δD Isoscapes

PubMed Central

Pietsch, Stephanie J.; Hobson, Keith A.; Wassenaar, Leonard I.; Tütken, Thomas

2011-01-01

Background Several felids are endangered and threatened by the illegal wildlife trade. Establishing geographic origin of tissues of endangered species is thus crucial for wildlife crime investigations and effective conservation strategies. As shown in other species, stable isotope analysis of hydrogen and oxygen in hair (δDh, δ18Oh) can be used as a tool for provenance determination. However, reliably predicting the spatial distribution of δDh and δ18Oh requires confirmation from animal tissues of known origin and a detailed understanding of the isotopic routing of dietary nutrients into felid hair. Methodology/Findings We used coupled δDh and δ18Oh measurements from the North American bobcat (Lynx rufus) and puma (Puma concolor) with precipitation-based assignment isoscapes to test the feasibility of isotopic geo-location of felidae. Hairs of felid and rabbit museum specimens from 75 sites across the United States and Canada were analyzed. Bobcat and puma lacked a significant correlation between H/O isotopes in hair and local waters, and also exhibited an isotopic decoupling of δ18Oh and δDh. Conversely, strong δD and δ18O coupling was found for key prey, eastern cottontail rabbit (Sylvilagus floridanus; hair) and white-tailed deer (Odocoileus virginianus; collagen, bone phosphate). Conclusions/Significance Puma and bobcat hairs do not adhere to expected pattern of H and O isotopic variation predicted by precipitation isoscapes for North America. Thus, using bulk hair, felids cannot be placed on δ18O and δD isoscapes for use in forensic investigations. The effective application of isotopes to trace the provenance of feline carnivores is likely compromised by major controls of their diet, physiology and metabolism on hair δ18O and δD related to body water budgets. Controlled feeding experiments, combined with single amino acid isotope analysis of diets and hair, are needed to reveal mechanisms and physiological traits explaining why felid hair does not follow isotopic patterns demonstrated in many other taxa. PMID:21931770

Metastable Radioxenon Verification Laboratory (MRVL) Year-End Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cooper, Matthew W.; Hayes, James C.; Lidey, Lance S.

2014-11-07

This is the year end report that is due to the client. The MRVL system is designed to measure multiple radioxenon isotopes ( 135Xe, 133Xe, 133mXe and 133mXe) simultaneously. The system has 12 channels to load samples and make nuclear measurements. Although the MRVL system has demonstrated excellent stability in measurements of Xe-133 and Xe-135 over the year of evaluation prior to delivery, there has been concern about system stability over measurements performed on samples with orders of magnitude different radioactivity, and samples containing multiple isotopes. To address these concerns, a series of evaluation test have been performed at themore » end-user laboratory. The evaluation was performed in two separate phases. Phase 1 made measurements on isotopically pure Xe-133 from high radioactivity down to the system background levels of activity, addressing the potential count rate dependencies when activities change from extreme high to very low. The second phase performed measurements on samples containing multiple isotopes (Xe-135, Xe-133 and Xe-133m), and addressed concerns about the dependence of isotopic concentrations on the presence of additional isotopes. The MRVL showed a concentration dependence on the Xe-133 due to the amount of Xe-133m that was in the sample. The dependency is due to the decay of Xe-133m into Xe-133. This document focuses on the second phase and will address the analysis used to account for ingrowth of Xe-133 from Xe-133m.« less

ICPD-A New Peak Detection Algorithm for LC/MS

PubMed Central

2010-01-01

Background The identification and quantification of proteins using label-free Liquid Chromatography/Mass Spectrometry (LC/MS) play crucial roles in biological and biomedical research. Increasing evidence has shown that biomarkers are often low abundance proteins. However, LC/MS systems are subject to considerable noise and sample variability, whose statistical characteristics are still elusive, making computational identification of low abundance proteins extremely challenging. As a result, the inability of identifying low abundance proteins in a proteomic study is the main bottleneck in protein biomarker discovery. Results In this paper, we propose a new peak detection method called Information Combining Peak Detection (ICPD ) for high resolution LC/MS. In LC/MS, peptides elute during a certain time period and as a result, peptide isotope patterns are registered in multiple MS scans. The key feature of the new algorithm is that the observed isotope patterns registered in multiple scans are combined together for estimating the likelihood of the peptide existence. An isotope pattern matching score based on the likelihood probability is provided and utilized for peak detection. Conclusions The performance of the new algorithm is evaluated based on protein standards with 48 known proteins. The evaluation shows better peak detection accuracy for low abundance proteins than other LC/MS peak detection methods. PMID:21143790

An Isotopic view of water and nitrogen transport through the vadose zone in Oregon's southern Willamette Valley's Groundwater Management Area

EPA Science Inventory

Background/Question/MethodsGroundwater nitrate contamination affects thousands of households in Oregon's southern Willamette Valley and many more across the Pacific Northwest. The southern Willamette Valley Groundwater Management Area (SWV GWMA) was established in 2004 due to nit...

An Isotopic Dilution Experiment Using Liquid Scintillation: A Simple Two-System, Two-Phase Analysis.

ERIC Educational Resources Information Center

Moehs, Peter J.; Levine, Samuel

1982-01-01

A simple isotonic, dilution analysis whose principles apply to methods of more complex radioanalyses is described. Suitable for clinical and instrumental analysis chemistry students, experimental manipulations are kept to a minimum involving only aqueous extraction before counting. Background information, procedures, and results are discussed.…

Guide to the expression of uncertainty in measurements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mathew, Kattathu Joseph

The enabling objectives of this presentation are to: Provide a working knowledge of the ISO GUM method to estimation of uncertainties in safeguards measurements; Introduce GUM terminology; Provide brief historical background of the GUM methodology; Introduce GUM Workbench software; Isotope ratio measurements by MS will be discussed in the next session.

ICP MS selection of radiopure materials for the GERDA experiment

NASA Astrophysics Data System (ADS)

di Vacri, M. L.; Nisi, S.; Cattadori, C.; Janicsko, J.; Lubashevskiy, A.; Smolnikov, A.; Walter, M.

2015-08-01

The GERDA (GERmanium Detector Array) experiment, located in the Gran Sasso Underground Laboratory (LNGS, Italy) aims to search for neutrinoless double beta (0νββ) decay of the 76Ge isotope. Both an ultra-low radioactivity background environment and active techniques to abate the residual background are required to reach the background index (of 10-3 counts/keV kg y) at the Qββ. In order to veto and suppress those events that partially deposit energy in Ge detectors, the readout of liquid argon (LAr) scintillation light (SL) has been implemented for the second GERDA experimental Phase. A double veto system has been designed and constructed using highly radiopure materials (scintillating fibers, wavelength shifters, polymeric foils, reflective foils). This work describes the study of lead, thorium and uranium ultra-trace content, performed at the LNGS Chemistry Laboratory by High Resolution Mass Spectrometry (HR ICP MS), for the selection of all materials involved in the construction of the veto system

ICP MS selection of radiopure materials for the GERDA experiment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Di Vacri, M. L., E-mail: divacrim@lngs.infn.it; Dipartimento di Scienze Fisiche e Chimiche, University of L’Aquila, via Vetoio, 67100 L’Aquila; Nisi, S., E-mail: nisi@lngs.infn.it

2015-08-17

The GERDA (GERmanium Detector Array) experiment, located in the Gran Sasso Underground Laboratory (LNGS, Italy) aims to search for neutrinoless double beta (0νββ) decay of the {sup 76}Ge isotope. Both an ultra-low radioactivity background environment and active techniques to abate the residual background are required to reach the background index (of 10{sup −3} counts/keV kg y) at the Q{sub ββ}. In order to veto and suppress those events that partially deposit energy in Ge detectors, the readout of liquid argon (LAr) scintillation light (SL) has been implemented for the second GERDA experimental Phase. A double veto system has been designedmore » and constructed using highly radiopure materials (scintillating fibers, wavelength shifters, polymeric foils, reflective foils). This work describes the study of lead, thorium and uranium ultra-trace content, performed at the LNGS Chemistry Laboratory by High Resolution Mass Spectrometry (HR ICP MS), for the selection of all materials involved in the construction of the veto system.« less

A protocol to correct for intra- and interspecific variation in tail hair growth to align isotope signatures of segmentally cut tail hair to a common time line.

PubMed

Burnik Šturm, Martina; Pukazhenthi, Budhan; Reed, Dolores; Ganbaatar, Oyunsaikhan; Sušnik, Stane; Haymerle, Agnes; Voigt, Christian C; Kaczensky, Petra

2015-06-15

In recent years, segmental stable isotope analysis of hair has been a focus of research in animal dietary ecology and migration. To correctly assign tail hair segments to seasons or even Julian dates, information on tail hair growth rates is a key parameter, but is lacking for most species. We (a) reviewed the literature on tail hair growth rates in mammals; b) made own measurements of three captive equid species; (c) measured δ(2)H, δ(13)C and δ(15)N values in sequentially cut tail hairs of three sympatric, free-ranging equids from the Mongolian Gobi, using isotope ratio mass spectrometry (IRMS); and (d) collected environmental background data on seasonal variation by measuring δ(2)H values in precipitation by IRMS and by compiling pasture productivity measured by remote sensing via the normalized difference vegetation index (NDVI). Tail hair growth rates showed significant inter- and intra-specific variation making temporal alignment problematic. In the Mongolian Gobi, high seasonal variation of δ(2)H values in precipitation results in winter lows and summer highs of δ(2)H values of available water sources. In water-dependent equids, this seasonality is reflected in the isotope signatures of sequentially cut tails hairs. In regions which are subject to strong seasonal patterns we suggest identifying key isotopes which show strong seasonal variation in the environment and can be expected to be reflected in the animal tissue. The known interval between the maxima and minima of these isotope values can then be used to correctly temporally align the segmental stable isotope signature for each individual animal. © 2015 The Authors. Rapid Communications in Mass Spectrometry published by John Wiley & Sons Ltd.

A protocol to correct for intra- and interspecific variation in tail hair growth to align isotope signatures of segmentally cut tail hair to a common time line

PubMed Central

Burnik Šturm, Martina; Pukazhenthi, Budhan; Reed, Dolores; Ganbaatar, Oyunsaikhan; Sušnik, Stane; Haymerle, Agnes; Voigt, Christian C; Kaczensky, Petra

2015-01-01

Rationale In recent years, segmental stable isotope analysis of hair has been a focus of research in animal dietary ecology and migration. To correctly assign tail hair segments to seasons or even Julian dates, information on tail hair growth rates is a key parameter, but is lacking for most species. Methods We (a) reviewed the literature on tail hair growth rates in mammals; b) made own measurements of three captive equid species; (c) measured δ2H, δ13C and δ15N values in sequentially cut tail hairs of three sympatric, free-ranging equids from the Mongolian Gobi, using isotope ratio mass spectrometry (IRMS); and (d) collected environmental background data on seasonal variation by measuring δ2H values in precipitation by IRMS and by compiling pasture productivity measured by remote sensing via the normalized difference vegetation index (NDVI). Results Tail hair growth rates showed significant inter- and intra-specific variation making temporal alignment problematic. In the Mongolian Gobi, high seasonal variation of δ2H values in precipitation results in winter lows and summer highs of δ2H values of available water sources. In water-dependent equids, this seasonality is reflected in the isotope signatures of sequentially cut tails hairs. Conclusions In regions which are subject to strong seasonal patterns we suggest identifying key isotopes which show strong seasonal variation in the environment and can be expected to be reflected in the animal tissue. The known interval between the maxima and minima of these isotope values can then be used to correctly temporally align the segmental stable isotope signature for each individual animal. © 2015 The Authors. Rapid Communications in Mass Spectrometry published by John Wiley & Sons Ltd. PMID:26044272

Plant family identity distinguishes patterns of carbon and nitrogen stable isotope abundance and nitrogen concentration in mycoheterotrophic plants associated with ectomycorrhizal fungi

PubMed Central

Hynson, Nicole A.; Schiebold, Julienne M.-I.; Gebauer, Gerhard

2016-01-01

Background and Aims Mycoheterotrophy entails plants meeting all or a portion of their carbon (C) demands via symbiotic interactions with root-inhabiting mycorrhizal fungi. Ecophysiological traits of mycoheterotrophs, such as their C stable isotope abundances, strongly correlate with the degree of species’ dependency on fungal C gains relative to C gains via photosynthesis. Less explored is the relationship between plant evolutionary history and mycoheterotrophic plant ecophysiology. We hypothesized that the C and nitrogen (N) stable isotope compositions, and N concentrations of fully and partially mycoheterotrophic species differentiate them from autotrophs, and that plant family identity would be an additional and significant explanatory factor for differences in these traits among species. We focused on mycoheterotrophic species that associate with ectomycorrhizal fungi from plant families Ericaceae and Orchidaceae. Methods Published and unpublished data were compiled on the N concentrations, C and N stable isotope abundances (δ13C and δ15N) of fully (n = 18) and partially (n = 22) mycoheterotrophic species from each plant family as well as corresponding autotrophic reference species (n = 156). These data were used to calculate site-independent C and N stable isotope enrichment factors (ε). Then we tested for differences in N concentration, 13C and 15N enrichment among plant families and trophic strategies. Key Results We found that in addition to differentiating partially and fully mycoheterotrophic species from each other and from autotrophs, C and N stable isotope enrichment also differentiates plant species based on familial identity. Differences in N concentrations clustered at the plant family level rather than the degree of dependency on mycoheterotrophy. Conclusions We posit that differences in stable isotope composition and N concentrations are related to plant family-specific physiological interactions with fungi and their environments. PMID:27451987

Identification of Anthropogenic CO2 Using Triple Oxygen and Clumped Isotopes.

PubMed

Laskar, Amzad H; Mahata, Sasadhar; Liang, Mao-Chang

2016-11-01

Quantification of contributions from various sources of CO 2 is important for understanding the atmospheric CO 2 budget. Considering the number and diversity of sources and sinks, the widely used proxies such as concentration and conventional isotopic compositions (δ 13 C and δ 18 O) are not always sufficient to fully constrain the CO 2 budget. Additional constraints may help in understanding the mechanisms of CO 2 production and consumption. The anomaly in triple oxygen isotopes or 17 O excess (denoted by Δ 17 O) and molecules containing two rare isotopes, called clumped isotopes, are two recently developed tracers with potentials to independently constrain some important processes that regulate CO 2 in the atmosphere. The clumped isotope for CO 2 , denoted by Δ 47 , is the excess of 13 C 16 O 18 O over a random distribution of isotopes in a CO 2 molecule. We measured the concentrations of δ 13 C, δ 18 O, Δ 17 O, and Δ 47 in air CO 2 samples collected from the Hsuehshan tunnel (length: 12.9 km), and applied linear and polynomial regressions to obtain the fossil fuel end-members for all these isotope proxies. The other end-members, the values of all these proxies for background air CO 2 , are either assumed or taken as the values obtained over the tunnel and ocean. The fossil fuel (anthropogenic) CO 2 end-member values for δ 13 C, δ 18 O, Δ 17 O, and Δ 47 are estimated using the two component mixing approach: the derived values are -26.76 ± 0.25‰, 24.57 ± 0.33‰, -0.219 ± 0.021‰, and 0.267 ± 0.036‰, respectively. These four major CO 2 isotope tracers along with the concentration were used to estimate the anthropogenic contribution in the atmospheric CO 2 in urban and suburban locations. We demonstrate that Δ 17 O and Δ 47 have the potential to independently estimate anthropogenic contribution, and the advantages of these two over the conventional isotope proxies are discussed.

An ultra-low background PMT for liquid xenon detectors

DOE PAGES

Akerib, D. S.; Bai, X.; Bernard, E.; ...

2012-11-15

Results are presented from radioactivity screening of two models of photomultiplier tubes designed for use in current and future liquid xenon experiments. The Hamamatsu 5.6 cm diameter R8778 PMT, used in the LUX dark matter experiment, has yielded a positive detection of four common radioactive isotopes: 238U, 232Th, 40K, and 60Co. Screening of LUX materials has rendered backgrounds from other detector materials subdominant to the R8778 contribution. A prototype Hamamatsu 7.6 cm diameter R11410 MOD PMT has also been screened, with benchmark isotope counts measured at <0.4 238U / <0.3 232Th / < 8.3 40K / 2.0+-0.2 60Co mBq/PMT. This represents a large reduction, equal to a change of xmore » $$\\frac{1}{24}$$ 238U / x $$\\frac{1}{9}$$ 232Th / x $$\\frac{1}{8}$$ 40K per PMT, between R8778 and R11410 MOD, concurrent with a doubling of the photocathode surface area (4.5 cm to 6.4 cm diameter). 60Co measurements are comparable between the PMTs, but can be significantly reduced in future R11410 MOD units through further material selection. Assuming PMT activity equal to the measured 90% upper limits, Monte Carlo estimates indicate that replacement of R8778 PMTs with R11410 MOD PMTs will change LUX PMT electron recoil background contributions by a factor of x $$\\frac{1}{25}$$ after further material selection for 60Co reduction, and nuclear recoil backgrounds by a factor of \\times $$\\frac{1}{36}$$. The strong reduction in backgrounds below the measured R8778 levels makes the R11410 MOD a very competitive technology for use in large-scale liquid xenon detectors.« less

Multivariate statistical and lead isotopic analyses approach to identify heavy metal sources in topsoil from the industrial zone of Beijing Capital Iron and Steel Factory.

PubMed

Zhu, Guangxu; Guo, Qingjun; Xiao, Huayun; Chen, Tongbin; Yang, Jun

2017-06-01

Heavy metals are considered toxic to humans and ecosystems. In the present study, heavy metal concentration in soil was investigated using the single pollution index (PIi), the integrated Nemerow pollution index (PIN), and the geoaccumulation index (Igeo) to determine metal accumulation and its pollution status at the abandoned site of the Capital Iron and Steel Factory in Beijing and its surrounding area. Multivariate statistical (principal component analysis and correlation analysis), geostatistical analysis (ArcGIS tool), combined with stable Pb isotopic ratios, were applied to explore the characteristics of heavy metal pollution and the possible sources of pollutants. The results indicated that heavy metal elements show different degrees of accumulation in the study area, the observed trend of the enrichment factors, and the geoaccumulation index was Hg > Cd > Zn > Cr > Pb > Cu ≈ As > Ni. Hg, Cd, Zn, and Cr were the dominant elements that influenced soil quality in the study area. The Nemerow index method indicated that all of the heavy metals caused serious pollution except Ni. Multivariate statistical analysis indicated that Cd, Zn, Cu, and Pb show obvious correlation and have higher loads on the same principal component, suggesting that they had the same sources, which are related to industrial activities and vehicle emissions. The spatial distribution maps based on ordinary kriging showed that high concentrations of heavy metals were located in the local factory area and in the southeast-northwest part of the study region, corresponding with the predominant wind directions. Analyses of lead isotopes confirmed that Pb in the study soils is predominantly derived from three Pb sources: dust generated during steel production, coal combustion, and the natural background. Moreover, the ternary mixture model based on lead isotope analysis indicates that lead in the study soils originates mainly from anthropogenic sources, which contribute much more than the natural sources. Our study could not only reveal the overall situation of heavy metal contamination, but also identify the specific pollution sources.

Delayed signatures of underground nuclear explosions

PubMed Central

Carrigan, Charles R.; Sun, Yunwei; Hunter, Steven L.; Ruddle, David G.; Wagoner, Jeffrey L.; Myers, Katherine B. L.; Emer, Dudley F.; Drellack, Sigmund L.; Chipman, Veraun D.

2016-01-01

Radionuclide signals from underground nuclear explosions (UNEs) are strongly influenced by the surrounding hydrogeologic regime. One effect of containment is delay of detonation-produced radioxenon reaching the surface as well as lengthening of its period of detectability compared to uncontained explosions. Using a field-scale tracer experiment, we evaluate important transport properties of a former UNE site. We observe the character of signals at the surface due to the migration of gases from the post-detonation chimney under realistic transport conditions. Background radon signals are found to be highly responsive to cavity pressurization suggesting that large local radon anomalies may be an indicator of a clandestine UNE. Computer simulations, using transport properties obtained from the experiment, track radioxenon isotopes in the chimney and their migration to the surface. They show that the chimney surrounded by a fractured containment regime behaves as a leaky chemical reactor regarding its effect on isotopic evolution introducing a dependence on nuclear yield not previously considered. This evolutionary model for radioxenon isotopes is validated by atmospheric observations of radioxenon from a 2013 UNE in the Democratic People’s Republic of Korea (DPRK). Our model produces results similar to isotopic observations with nuclear yields being comparable to seismic estimates. PMID:26979288

Delayed signatures of underground nuclear explosions

NASA Astrophysics Data System (ADS)

Carrigan, Charles R.; Sun, Yunwei; Hunter, Steven L.; Ruddle, David G.; Wagoner, Jeffrey L.; Myers, Katherine B. L.; Emer, Dudley F.; Drellack, Sigmund L.; Chipman, Veraun D.

2016-03-01

Radionuclide signals from underground nuclear explosions (UNEs) are strongly influenced by the surrounding hydrogeologic regime. One effect of containment is delay of detonation-produced radioxenon reaching the surface as well as lengthening of its period of detectability compared to uncontained explosions. Using a field-scale tracer experiment, we evaluate important transport properties of a former UNE site. We observe the character of signals at the surface due to the migration of gases from the post-detonation chimney under realistic transport conditions. Background radon signals are found to be highly responsive to cavity pressurization suggesting that large local radon anomalies may be an indicator of a clandestine UNE. Computer simulations, using transport properties obtained from the experiment, track radioxenon isotopes in the chimney and their migration to the surface. They show that the chimney surrounded by a fractured containment regime behaves as a leaky chemical reactor regarding its effect on isotopic evolution introducing a dependence on nuclear yield not previously considered. This evolutionary model for radioxenon isotopes is validated by atmospheric observations of radioxenon from a 2013 UNE in the Democratic People’s Republic of Korea (DPRK). Our model produces results similar to isotopic observations with nuclear yields being comparable to seismic estimates.

Delayed signatures of underground nuclear explosions.

PubMed

Carrigan, Charles R; Sun, Yunwei; Hunter, Steven L; Ruddle, David G; Wagoner, Jeffrey L; Myers, Katherine B L; Emer, Dudley F; Drellack, Sigmund L; Chipman, Veraun D

2016-03-16

Radionuclide signals from underground nuclear explosions (UNEs) are strongly influenced by the surrounding hydrogeologic regime. One effect of containment is delay of detonation-produced radioxenon reaching the surface as well as lengthening of its period of detectability compared to uncontained explosions. Using a field-scale tracer experiment, we evaluate important transport properties of a former UNE site. We observe the character of signals at the surface due to the migration of gases from the post-detonation chimney under realistic transport conditions. Background radon signals are found to be highly responsive to cavity pressurization suggesting that large local radon anomalies may be an indicator of a clandestine UNE. Computer simulations, using transport properties obtained from the experiment, track radioxenon isotopes in the chimney and their migration to the surface. They show that the chimney surrounded by a fractured containment regime behaves as a leaky chemical reactor regarding its effect on isotopic evolution introducing a dependence on nuclear yield not previously considered. This evolutionary model for radioxenon isotopes is validated by atmospheric observations of radioxenon from a 2013 UNE in the Democratic People's Republic of Korea (DPRK). Our model produces results similar to isotopic observations with nuclear yields being comparable to seismic estimates.

Historic and Industrial Lead within the Northwest Pacific Ocean Evidenced by Lead Isotopes in Seawater.

PubMed

Zurbrick, Cheryl M; Gallon, Céline; Flegal, A Russell

2017-02-07

We report the continued lead (Pb) contamination of the Northwest Pacific Ocean in 2002 and present the first comprehensive Pb isotope data set for that region. In the upper ocean, a Pb concentration maxima (64-113 pmol kg -1 ) extended throughout the entire North Pacific Subtropical Gyre (NPSG). We determined most of the Pb in this feature was from industrial emissions by many nations in the 1980s and 1990s, with the largest contributions from leaded gasoline emissions. In contrast, the deep water (>1000 m) Pb concentrations were lower (6-37 pmol kg -1 ), and constituted a mix of background (natural) Pb and anthropogenic Pb inputs from preceding decades. Deep water below the Western Subarctic Gyre (WSAG) contained more industrial Pb than below the NPSG, which was attributed to a calculated 60-fold greater flux of particulate Pb to abyssal waters near the Asian continent. Assuming Pb isotope compositions in the North Pacific Ocean were homogeneous prior to large-scale 20th century anthropogenic inputs, this evidence suggests a relatively faster change in Pb isotope ratios of North Pacific deep water below the WSAG versus the NPSG.

Instrumental and atmospheric background lines observed by the SMM gamma-ray spectrometer

NASA Technical Reports Server (NTRS)

Share, G. H.; Kinzer, R. L.; Strickman, M. S.; Letaw, J. R.; Chupp, E. L.

1989-01-01

Preliminary identifications of instrumental and atmospheric background lines detected by the gamma-ray spectrometer on NASA's Solar Maximum Mission satellite (SMM) are presented. The long-term and stable operation of this experiment has provided data of high quality for use in this analysis. Methods are described for identifying radioactive isotopes which use their different decay times. Temporal evolution of the features are revealed by spectral comparisons, subtractions, and fits. An understanding of these temporal variations has enabled the data to be used for detecting celestial gamma-ray sources.

Uranium beam characterization at CIRCE for background and contamination determinations.

PubMed

De Cesare, M; De Cesare, N; D'Onofrio, A; Fifield, L K; Gialanella, L; Terrasi, F

2015-09-01

The Accelerator Mass Spectrometry (AMS) is the most sensitive technique, compared either to the Inductively Coupled Plasma (ICP-MS) or Thermal Ionization (TI-MS) mass spectrometer, for the actinide (e.g. (236)U, (x)Pu isotopes) measurements. They are present in environmental samples at the ultra trace level since atmospheric tests of Nuclear Weapons (NWs) performed in the past, deliberate dumping of nuclear waste, nuclear fuel reprocessing, on a large scale, and operation of Nuclear Power Plants (NPPs), on a small scale, have led to the release of a wide range of radioactive nuclides in the environment. At the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy, an upgraded actinide AMS system, based on a 3-MV pelletron tandem accelerator, has been developed and routinely operated. At CIRCE a charge state distribution as a function of terminal voltage, the beam emittance, measured in the 20° actinides dedicated beam line, as well as the energy and position validation of the U ions were performed in order to determine the best measurement conditions. A (236)U/(238)U isotopic ratio background level of about 5×10(-12) or 3×10(-13), depending on the Time of Flight-Energy (TOF-E) configurations, as well as the spatial distribution of the (235)U, (238)U interferences ions and a (236)U contamination mass of about 0.5 fg have been determined. Copyright © 2015 Elsevier Ltd. All rights reserved.

Environmental forcing of terrestrial carbon isotope excursion amplification across five Eocene hyperthermals

NASA Astrophysics Data System (ADS)

Bowen, G. J.; Abels, H.

2015-12-01

Abrupt changes in the isotope composition of exogenic carbon pools accompany many major episodes of global change in the geologic record. The global expression of this change in substrates that reflect multiple carbon pools provides important evidence that many events reflect persistent, global redistribution of carbon between reduced and oxidized stocks. As the diversity of records documenting any event grows, however, discrepancies in the expression of carbon isotope change among substrates are almost always revealed. These differences in magnitude, pace, and pattern of change can complicate interpretations of global carbon redistribution, but under ideal circumstances can also provide additional information on changes in specific environmental and biogeochemical systems that accompanied the global events. Here we evaluate possible environmental influences on new terrestrial records of the negative carbon isotope excursions (CIEs) associated with multiple hyperthermals of the Early Eocene, which show a common pattern of amplified carbon isotope change in terrestrial paleosol carbonate records relative to that recorded in marine substrates. Scaling relationships between climate and carbon-cycle proxies suggest that that the climatic (temperature) impact of each event scaled proportionally with the magnitude of its marine CIE, likely implying that all events involved release of reduced carbon with a similar isotopic composition. Amplification of the terrestrial CIEs, however, does not scale with event magnitude, being proportionally less for the first, largest event (the PETM). We conduct a sensitivity test of a coupled plant-soil carbon isotope model to identify conditions that could account for the observed CIE scaling. At least two possibilities consistent with independent lines of evidence emerge: first, varying effects of pCO2 change on photosynthetic carbon isotope discrimination under changing background pCO2, and second, contrasting changes in regional hydroclimate during the PETM and subsequent hyperthermals. These mechanisms have very different implications for the reconstruction of environmental conditions, and resolving the correct interpretation will require new, complimentary records of plant and soil conditions associated with the Early Eocene hyperthermals.

Evidence of the exploitation of marine resource by the terrestrial insect Scapteriscus didactylus through stable isotope analyzes of its cuticle

PubMed Central

Maros, Alexandra; Louveaux, Alain; Lelarge, Caroline; Girondot, Marc

2006-01-01

Background About 4 × 105 eggs in more than 5000 marine turtle nests are deposited every year on a 3.6 km long beach in French Guiana (South America). The dry biomass of eggs is estimated to be 5 × 103 kg, yet only 25% of this organic matter will return to the ocean in the form of hatchlings. Such amounts of organic matter are supposed to drive the functioning of the beach ecosystem. Previous studies have shown that egg predators and detritivorous organisms dominate the trophic relationships and the dynamics of the system. The role of a terrestrial insect Scapteriscus didactylus (Latreille), which damages up to 40% of the eggs of the marine turtle (Dermochelys coriacea), was unexpected. However it was impossible from direct observations to prove that the mole cricket consumed a significant amount of these eggs. Therefore, the precise place of the mole cricket in the nitrogen and carbon cycles of the beach ecosystem could not be determined. In order to answer this question, we looked for a marine signature of carbon and nitrogen source metabolized by the mole cricket. Results This study estimated the individual variability of δ13C and δ15N in the cuticle of Scapteriscus didactylus. The isotopic signature was compared between individuals collected at two sites: a village where mole crickets fed on human food scraps and the nearby Awala-Yalimapo beach, where food availability depends seasonally on the nesting sea turtles. The mole crickets collected near the habitations garbage showed no significant variations in the stable isotopic signature, within-and between age groups. On the contrary, isotopic values shifted from a signature of a terrestrial herbivorous diet in the mole crickets during early developmental stages, to isotopic values in adults in accordance with the exploitation of marine animal resources. Conclusion The heterogeneity of individual signatures during the year is due to a selective exploitation of the food sources, differing in space and time. Some individuals, from the beach sample consumed a sufficient quantity of turtle eggs to induce the increase of isotopic enrichment observed in the cuticle. Scapteriscus didactylus is an opportunist feeder and plays a role in the turn over of the beach organic matter. PMID:16681850

Overview of SIMS-Based Experimental Studies of Tracer Diffusion in Solids and Application to Mg Self-Diffusion

DOE PAGES

Kulkarni, Nagraj S.; Bruce Warmack, Robert J.; Radhakrishnan, Bala; ...

2014-09-23

Tracer diffusivities provide the most fundamental information on diffusion in materials and are the foundation of robust diffusion databases. Compared to traditional radiotracer techniques that utilize radioactive isotopes, the secondary ion mass spectrometry (SIMS) based thin-film technique for tracer diffusion is based on the use of enriched stable isotopes that can be accurately profiled using SIMS. Experimental procedures & techniques that are utilized for the measurement of tracer diffusion coefficients are presented for pure magnesium, which presents some unique challenges due to the ease of oxidation. The development of a modified Shewmon-Rhines diffusion capsule for annealing Mg and an ultra-highmore » vacuum (UHV) system for sputter deposition of Mg isotopes are discussed. Optimized conditions for accurate SIMS depth profiling in polycrystalline Mg are provided. An automated procedure for the correction of heat-up and cool-down times during tracer diffusion annealing is discussed. The non-linear fitting of a SIMS depth profile data using the thin film Gaussian solution to obtain the tracer diffusivity along with the background tracer concentration and tracer film thickness is discussed. An Arrhenius fit of the Mg self-diffusion data obtained using the low-temperature SIMS measurements from this study and the high-temperature radiotracer measurements of Shewmon and Rhines (1954) was found to be a good representation of both types of diffusion data that cover a broad range of temperatures between 250 - 627° C (523 900 K).« less

Quantitative Thermochronology

NASA Astrophysics Data System (ADS)

Braun, Jean; van der Beek, Peter; Batt, Geoffrey

2006-05-01

Thermochronology, the study of the thermal history of rocks, enables us to quantify the nature and timing of tectonic processes. Quantitative Thermochronology is a robust review of isotopic ages, and presents a range of numerical modeling techniques to allow the physical implications of isotopic age data to be explored. The authors provide analytical, semi-analytical, and numerical solutions to the heat transfer equation in a range of tectonic settings and under varying boundary conditions. They then illustrate their modeling approach built around a large number of case studies. The benefits of different thermochronological techniques are also described. Computer programs on an accompanying website at www.cambridge.org/9780521830577 are introduced through the text and provide a means of solving the heat transport equation in the deforming Earth to predict the ages of rocks and compare them directly to geological and geochronological data. Several short tutorials, with hints and solutions, are also included. Numerous case studies help geologists to interpret age data and relate it to Earth processes Essential background material to aid understanding and using thermochronological data Provides a thorough treatise on numerical modeling of heat transport in the Earth's crust Supported by a website hosting relevant computer programs and colour slides of figures from the book for use in teaching

Isotopic analysis of uranium in natural waters by alpha spectrometry

USGS Publications Warehouse

Edwards, K.W.

1968-01-01

A method is described for the determination of U234/U238 activity ratios for uranium present in natural waters. The uranium is coprecipitated from solution with aluminum phosphate, extracted into ethyl acetate, further purified by ion exchange, and finally electroplated on a titanium disc for counting. The individual isotopes are determined by measurement of the alpha-particle energy spectrum using a high resolution low-background alpha spectrometer. Overall chemical recovery of about 90 percent and a counting efficiency of 25 percent allow analyses of water samples containing as little as 0.10 ?g/l of uranium. The accuracy of the method is limited, on most samples, primarily by counting statistics.

Method for correcting for isotope burn-in effects in fission neutron dosimeters

DOEpatents

Gold, Raymond; McElroy, William N.

1988-01-01

A method is described for correcting for effect of isotope burn-in in fission neutron dosimeters. Two quantities are measured in order to quantify the "burn-in" contribution, namely P.sub.Z',A', the amount of (Z', A') isotope that is burned-in, and F.sub.Z', A', the fissions per unit volume produced in the (Z', A') isotope. To measure P.sub.Z', A', two solid state track recorder fission deposits are prepared from the very same material that comprises the fission neutron dosimeter, and the mass and mass density are measured. One of these deposits is exposed along with the fission neutron dosimeter, whereas the second deposit is subsequently used for observation of background. P.sub.Z', A' is then determined by conducting a second irradiation, wherein both the irradiated and unirradiated fission deposits are used in solid state track recorder dosimeters for observation of the absolute number of fissions per unit volume. The difference between the latter determines P.sub.Z', A' since the thermal neutron cross section is known. F.sub.Z', A' is obtained by using a fission neutron dosimeter for this specific isotope, which is exposed along with the original threshold fission neutron dosimeter to experience the same neutron flux-time history at the same location. In order to determine the fissions per unit volume produced in the isotope (Z', A') as it ingrows during the irradiation, B.sub.Z', A', from these observations, the neutron field must generally be either time independent or a separable function of time t and neutron energy E.

Simultaneous determination of the quantity and isotopic signature of dissolved organic matter from soil water using high-performance liquid chromatography/isotope ratio mass spectrometry.

PubMed

Scheibe, Andrea; Krantz, Lars; Gleixner, Gerd

2012-01-30

We assessed the accuracy and utility of a modified high-performance liquid chromatography/isotope ratio mass spectrometry (HPLC/IRMS) system for measuring the amount and stable carbon isotope signature of dissolved organic matter (DOM) <1 µm. Using a range of standard compounds as well as soil solutions sampled in the field, we compared the results of the HPLC/IRMS analysis with those from other methods for determining carbon and (13)C content. The conversion efficiency of the in-line wet oxidation of the HPLC/IRMS averaged 99.3% for a range of standard compounds. The agreement between HPLC/IRMS and other methods in the amount and isotopic signature of both standard compounds and soil water samples was excellent. For DOM concentrations below 10 mg C L(-1) (250 ng C total) pre-concentration or large volume injections are recommended in order to prevent background interferences. We were able to detect large differences in the (13)C signatures of soil solution DOM sampled in 10 cm depth of plots with either C3 or C4 vegetation and in two different parent materials. These measurements also demonstrated changes in the (13)C signature that demonstrate rapid loss of plant-derived C with depth. Overall the modified HLPC/IRMS system has the advantages of rapid sample preparation, small required sample volume and high sample throughput, while showing comparable performance with other methods for measuring the amount and isotopic signature of DOM. Copyright © 2011 John Wiley & Sons, Ltd.

Ultra-Low Background Measurements Of Decayed Aerosol Filters

NASA Astrophysics Data System (ADS)

Miley, H.

2009-04-01

To experimentally evaluate the opportunity to apply ultra-low background measurement methods to samples collected, for instance, by the Comprehensive Test Ban Treaty International Monitoring System (IMS), aerosol samples collected on filter media were measured using HPGe spectrometers of varying low-background technology approaches. In this way, realistic estimates of the impact of low-background methodology can be assessed on the Minimum Detectable Activities obtained in systems such as the IMS. The current measurement requirement of stations in the IMS is 30 microBq per cubic meter of air for 140Ba, or about 106 fissions per daily sample. Importantly, this is for a fresh aerosol filter. Decay varying form 3 days to one week reduce the intrinsic background from radon daughters in the sample. Computational estimates of the improvement factor for these decayed filters for underground-based HPGe in clean shielding materials are orders of magnitude less, even when the decay of the isotopes of interest is included.

Diffusive Fractionation of Lithium Isotopes in Olivine Grain Boundaries

NASA Astrophysics Data System (ADS)

Homolova, V.; Watson, E. B.

2012-12-01

Diffusive fractionation of isotopes has been documented in silicate melts, aqueous fluids, and single crystals. In polycrystalline rocks, the meeting place of two grains, or grain boundaries, may also be a site of diffusive fractionation of isotopes. We have undertaken an experimental and modeling approach to investigate diffusive fractionation of lithium (Li) isotopes by grain boundary diffusion. The experimental procedure consists of packing a Ni metal capsule with predominantly ground San Carlos olivine and subjecting the capsule to 1100C and 1GPa for two days in a piston cylinder apparatus to create a nominally dry, 'dunite rock'. After this synthesis step, the capsule is sectioned and polished. One of the polished faces of the 'dunite rock' is then juxtaposed to a source material of spodumene and this diffusion couple is subject to the same experimental conditions as the synthesis step. Li abundances and isotopic profiles (ratios of count rates) were analyzed using LA-ICP-MS. Li concentrations linearly decrease away from the source from 550ppm to the average concentration of the starting olivine (2.5ppm). As a function of distance from the source, the 7Li/6Li ratio decreases to a minimum before increasing to the background ratio of the 'dunite rock'. The 7Li/6Li ratio minimum coincides with the lowest Li concentrations above average 'dunite rock' abundances. The initial decrease in the 7Li/6Li ratio is similar to that seen in other studies of diffusive fractionation of isotopes and is thought to be caused by the higher diffusivity (D) of the lighter isotope relative to the heavier isotope. The relationship between D and mass (m) is given by (D1/D2) =(m2/m1)^β, where β is an empirical fractionation factor; 1 and 2 denote the lighter and heavier isotope, respectively. A fit to the Li isotopic data reveals an effective DLi of ~1.2x10^-12 m/s^2 and a β of 0.1. Numerical modelling was utilized to elucidate the relationship between diffusive fractionation produced in the grain boundaries versus the lattices of the individual grains of the 'dunite rock'. The model assumes a linear grain boundary juxtaposed to the long side of a rectangular crystal lattice. During a simulation, the diffusant may directly enter the lattice or the grain boundary. Once in the grain boundary, the diffusant may then continue to diffuse away from the source until the end of the simulation or, alternatively, it may be incorporated into the lattice at some point during its travels down the grain boundary. The model system is similar to that considered by Whipple-LeClaire (1963) and our model results agree well with their analytical solution. Preliminary modeling results show that the distinctive minimum in the isotopic ratio is only produced when diffusive fractionation occurs in the grain boundary and not when the fractionation occurs only in the lattice. This suggests that the isotopic profile observed in the experiments may be a product of diffusive fractionation in grain boundaries. Implications of these results extend to the longevity of Li isotopic heterogeneities in the mantle, and suggest that the isotopes of other elements, which have a large relative mass difference, may also be diffusively fractionated by grain boundary diffusion.

New method of 85Kr reduction in a noble gas based low-background detector

NASA Astrophysics Data System (ADS)

Akimov, D. Yu.; Bolozdynya, A. I.; Burenkov, A. A.; Hall, C.; Kovalenko, A. G.; Kuzminov, V. V.; Simakov, G. E.

2017-04-01

Krypton-85 is an anthropogenic beta-decaying isotope which produces low energy backgrounds in dark matter and neutrino experiments, especially those based upon liquid xenon. Several technologies have been developed to reduce the Kr concentration in such experiments. We propose to augment those separation technologies by first adding to the xenon an 85Kr-free sample of krypton in an amount much larger than the natural krypton that is already present. After the purification system reduces the total Kr concentration to the same level, the final 85Kr concentration will be reduced even further by the dilution factor. A test cell for measurement of the activity of various Kr samples has been assembled, and the activity of 25-year-old krypton has been measured. The measured activity agrees well with the expected activity accounting for the 85Kr abundance of the earth's atmosphere in 1990 and the half-life of the isotope. Additional tests with a Kr sample produced in the year 1944 (before the atomic era) have been done in order to demonstrate the sensitivity of the test cell.

Brine Spills Associated with Unconventional Oil Development in North Dakota.

PubMed

Lauer, Nancy E; Harkness, Jennifer S; Vengosh, Avner

2016-05-17

The rapid rise of unconventional oil production during the past decade in the Bakken region of North Dakota raises concerns related to water contamination associated with the accidental release of oil and gas wastewater to the environment. Here, we characterize the major and trace element chemistry and isotopic ratios ((87)Sr/(86)Sr, δ(18)O, δ(2)H) of surface waters (n = 29) in areas impacted by oil and gas wastewater spills in the Bakken region of North Dakota. We establish geochemical and isotopic tracers that can identify Bakken brine spills in the environment. In addition to elevated concentrations of dissolved salts (Na, Cl, Br), spill waters also consisted of elevated concentrations of other contaminants (Se, V, Pb, NH4) compared to background waters, and soil and sediment in spill sites had elevated total radium activities ((228)Ra + (226)Ra) relative to background, indicating accumulation of Ra in impacted soil and sediment. We observed that inorganic contamination associated with brine spills in North Dakota is remarkably persistent, with elevated levels of contaminants observed in spills sites up to 4 years following the spill events.

Iron physiological requirements in Chinese adults assessed by the stable isotope labeling technique.

PubMed

Cai, Jie; Ren, Tongxiang; Zhang, Yuhui; Wang, Zhilin; Gou, Lingyan; Huang, Zhengwu; Wang, Jun; Piao, Jianhua; Yang, Xiaoguang; Yang, Lichen

2018-01-01

Iron is a kind of essential trace mineral in the human body, while the studies on its physiological requirement are very limited recently, especially in China. And most studies were performed with the radioisotope tracer technique, which was harmful to health. This study aimed to first get the value of iron physiological requirements in Chinese adults assessed by the stable isotope labeling technique. Forty-four eligible young Chinese healthy adults were randomly recruited from the Bethune Military Medical College (Shijiazhuang, Hebei, China) between January 2010 and March 2011, and 19 subjects were included in the final data analysis. After adaptive diets and observation, subjects received 58 Fe intravenously. The baseline venous blood sample and general information were collected on day 0. Venous blood samples were also collected on day 14, 30, 60, 100, 120, 150, 240, 330, 425, 515, 605, 767, 1155, respectively. The blood samples were acid digested by a Microwave Digestion System and then analyzed by the MC-ICP-MS and Atomic Absorption Spectroscopy to get the abundance of Fe isotopes and the total iron concentration respectively. The circulation rate (the proportion of blood iron to whole body iron) could be calculated by the intake amount, background content and the peak isotope content. When the abundance changed stably, the iron physiological requirement could be calculated by the iron loss in a period of time. The abundance of 58 Fe reached its peak on day 14, and changed stably from day 425. The average circulation rate was 84%, with no significance difference between the 2 genders. The mean iron requirement in females was 1101.68 μg/d, and the mean requirement adjusted by body weight was 20.69 μg/kg.d. For males, the mean iron requirement was 959.9 μg/d, and the requirement adjusted by body weight was 14.04 μg/kg.d. Our study has obtained the data about the iron physiological requirements of Chinese adults using stable isotope labeling technique, which could provide the basis for adjusting iron DRIs of Chinese people in the future. The trial was registered at the Chinese Clinical Trial Registry (No: ChiCTR-TRC-09000581).

Investigating Western Dead Sea spring systems and their origin by application of hydrogeochemical patterns

NASA Astrophysics Data System (ADS)

Wilske, Cornelia; Siebert, Christian; Geyer, Stefan; Rödiger, Tino; Merkel, Broder

2013-04-01

One of the ecologic and touristic hot spots along the western Dead Sea shore is the spring system of Ein Feshkha (Enot Zukim), which suffers from a changing environment. Its feeding Cretaceous aquifers are hosted in the western Graben flank of the Jordan-Dead Sea Rift. However, the origin of water and the ratio of influence of the unconsolidated Quaternary Graben fill is a controversial issue. The aim of the study is to combine hydrogeochemical information of the spring waters and the potential source aquifers to characterize and differentiate the groundwater origins, groundwater flow paths and eventually groundwater mixtures. Within this case study, which is embedded in the SMART II project (Sustainable Management of Available Water Resources of the Lower Jordan Valley), the investigation area extends in the Judean Mountains from the vicinity of Ramallah down to Hebron and ends along the north-western shoreline of the Dead Sea. The Cretaceous limestone aquifers of Turonian/Upper Cenomanian and Albian age are widely separated by a clayey aquiclude. That so called Judea Group is underlaid by the Kurnub sandstone aquifer. Mainly due to the development of the Rift, the entire area is intensely folded and crossed by faults. Groundwater recharge takes place in the uplands and the groundwater flow gradient is oriented towards the Valley, where it transgresses into the Quaternary Graben fill. Our hypothesis is that Ein Feshkha springs are fed by groundwater originating in general in the mountain range, which also takes a detour through the Graben fill in the north of the Dead Sea. Groundwater from these aquifers emerges along the coast of the Dead Sea through springs. The methodological approach is to use geogenic and anthropogenic hydrochemical parameters like major- and trace elements, stable isotopes like δ2H, δ18O or δ87Sr and heavy metals. Sampling campaigns were and will be carried out quarterly within one hydrological year to uncover possible seasonal variations. Samples are taken from the different aquifers over the whole investigation area. The first results represent the variability of the groundwater chemistry in terms of their TDS contents and their stable isotope signatures. The measured stable isotope ratios of Strontium, which refer to the geological background, show a differentiation between the groundwater of the main Judean aquifers. In combination with stable isotopes the composition of major- and trace elements including heavy metals improve the aquifer differentiation against the background of changes in geological formations.

Carbon isotopes of benthic foraminifera associated with methane seeps in Four-Way Closure Ridge, offshore southwestern Taiwan

NASA Astrophysics Data System (ADS)

Wang, W. R.; Wei, K. Y.; Mii, H. S.; Lin, Y. S.; Huang, J. J.; Wang, P. L.; Lin, A. T.

2015-12-01

Release of large amounts of methane from marine gas hydrate reservoirs has been considered as a possible trigger of climate change, which can be recorded by the variation of carbon isotopes (δ13C) of the benthic foraminifera. In modern analogs, previous studies have suggested that δ13C becomes more negative when influenced by methane seeps. However, values of δ13C of benthic foraminifera might vary with different species and sedimentary settings in different regions. Seismic profiles in offshore southwestern Taiwan show the existence of Bottom Simulating Reflector (BSR) in the region, indicative of gas hydrate reservoirs. Various methane seepages have been found, and they are suspected to be related to the gas hydrates buried underneath. A better understanding of the δ13C signals of benthic foraminifera near the methane seepages can further clarify the origin of the methane and to evaluate it as a proxy of methane release for the geologic past. We have analyzed δ13C of benthic foraminifera Uvigerina proboscidea (150-250 mm) in the topmost 15 cm sediments in five marine cores (OR1-1092-WFWC-1, OR1-1092-WFWC-4, OR1-1092-WFWC-6, OR3-1806-C5-2 and OR3-1806-C10) collected from the Four-Way Closure Ridge in offshore southwestern Taiwan (water depth from 1330 to 1580 m). Our results show that δ13C values of U. proboscidea range from -0.98‰ to -6.21‰ (VPDB) for core OR3-1806-C5-2, which is considered as a seeps-influenced site. On the other hand, δ13C values of U. proboscidea from the background sites range from -0.40‰ to -1.00‰. The difference between the methane seep-affected and the background sites is in the range of 0.00‰ to 5.01‰, comparable to those documented in previous studies in other areas. The significant negative excursion in carbon isotopes in the seep site foraminifera is likely caused by incorporation of light inorganic carbon generated by methanotrophy in the system.

Orbitally Tuned C and N Isotopic Records of Aptian Oceanic Anoxic Event1a in Northeastern Mexico and Deep Sea Drilling Project Site 398, North Atlantic Ocean

NASA Astrophysics Data System (ADS)

Montanez, I. P.; Li, Y.; Osleger, D. A.; Bralower, T. J.

2006-12-01

High-resolution and expanded records of early Aptian Oceanic Anoxic Event (OAE) 1a (120 Ma) were recovered from outer shelf and slope deposits from the Sierra Madre Oriental of northeast Mexico and from hemipelagic deposits at Deep Sea Drilling Project Site 398 on Vigo Seamount in the North Atlantic Ocean. OAE1a is recognized in these deposits by minor increases in organic carbon content (up to 2 wt%) and widely-recognized, characteristic δ13Corg and δ13Ccarb variations that record significant changes in global carbon cycling. Here we present continuous dm-scale records of grain size distributions, wt% TOC and carbonate, C/N ratios, and C and N isotopes for these stratigraphically-expanded sections. Our high-resolution rock magnetic study of the same stratigraphic intervals establishes orbital timescales for OAE1a at these sites. The highly expanded records reveal significantly more structure in isotopic and TOC variation throughout OAE1a than contemporaneous condensed deep-sea records. Our data define an initial prominent negative excursion followed by repeated and short-lived (103 to 104 yr) fluctuations and a final interval of near invariant δ13Ccarb and δ13Corg values. Elevated TOC, a significant increase in C/N ratios from background marine values, rapid shifts in C and N isotopic compositions and sustained decoupling of δ13Corg and δ15Norg occur throughout the interval of short- lived isotopic fluctuations. Anhysteretic remanent magnetization (ARM) measurements were used as proxies for terrigenous influx during OAE1a. Spectral analyses of ARM depth series reveal dominant cycles with wavelength ratios resembling those of modern orbital periodicities, implying that orbital variations may have modulated depositional processes. These orbitally tuned geochemical proxy records indicate that the Aptian deposits from northeastern Mexican and Site 398 on Vigo Seamount hold promise for refining phase relationships between geochemical and isotopic proxies throughout OAE1a, and, in turn, constraining the mechanics of addition of light carbon to the ocean-atmosphere system.

Aircraft profile measurements of 18O/16O and D/H isotope ratios of cloud condensate and water vapor constrain precipitation efficiency and entrainment rates in tropical clouds

NASA Astrophysics Data System (ADS)

Noone, D. C.; Raudzens Bailey, A.; Toohey, D. W.; Twohy, C. H.; Heymsfield, A.; Rella, C.; Van Pelt, A. D.

2011-12-01

Convective clouds play a significant role in the moisture and heat balance of the tropics. The dynamics of organized and isolated convection are a function of the background thermodynamic profile and wind shear, buoyancy sources near the surface and the latent heating inside convective updrafts. The stable oxygen and hydrogen isotope ratios in water vapor and condensate can be used to identify dominant moisture exchanges and aspects of the cloud microphysics that are otherwise difficult to observe. Both the precipitation efficiency and the dilution of cloud updrafts by entrainment can be estimated since the isotopic composition outside the plume is distinct from inside. Measurements of the 18O/16O and D/H isotope ratios were made in July 2011 on 13 research flights of the NCAR C130 aircraft during the ICE-T (Ice in Clouds Experiment - Tropical) field campaign near St Croix. Measurements were made using an instrument based on the Picarro Wave-Length Scanning Cavity Ring Down platform that includes a number of optical, hardware and software modifications to allow measurements to be made at 5 Hz for deployment on aircraft. The measurement system was optimized to make precise measurements of the isotope ratio of liquid and ice cloud condensate by coupling the gas analyzer to the NCAR Counter flow Virtual Impactor inlet. The inlet system provides a particle enhancement while rejecting vapor. Sample air is vigorously heated before flowing into the gas phase analyzer. We present statistics that demonstrate the performance and calibration of the instrument. Measured profiles show that environmental air exhibits significant layering showing controls from boundary layer processes, large scale horizontal advection and regional subsidence. Condensate in clouds is consistent with generally low precipitation efficiency, although there is significant variability in the isotope ratios suggesting heterogeneity within plumes and the stochastic nature of detrainment processes. Entrainment of air into the plume is seen as evaporation of condensate. In the plume between about -7 and -12C, the ice condensate fraction increases with height, and the isotope ratios are used to discern ice formation from deposition from ice formed from in situ freezing of cloud liquid. The observed profiles demonstrate a new capacity for cloud process studies and provide new insight into the water budget of clouds.

Isotopic composition of water vapor near the air-water interface

NASA Astrophysics Data System (ADS)

Zannoni, Daniele; Bergamasco, Andrea; Peschiutta, Mirco; Rampazzo, Giancarlo; Stenni, Barbara

2017-04-01

Evaporation is a key process in water cycle that links liquid water to the atmosphere. In the last fifty years stable isotopes of hydrogen and oxygen have been intensively used to describe climate processes related to evaporation and precipitation, ranging in different spatial and temporal scales. Evaporation introduces large isotopic effects in the phases involved. The well known Craig-Gordon model (Craig & Gordon, 1965) describes those isotopic effects involving several steps and different processes, moving from the air-water interface to the free atmosphere. However, very few works in literature have tested the vertical behavior of the Craig-Gordon model in natural conditions on both fresh and marine waters. In this work we present the results from four field experiments aimed to describe the vertical variability of δ18O and δD in the first few meters over a large water body (the coastal lagoon of Venice, northern Italy) and to test the Craig-Gordon model in such conditions. Each experiment involved cryotrapping of water vapor at different height over the water surface (0.1m, 2m and 4m) and the sampling of the liquid water at two depth (surface and 0.5m). During the experiments, water vapor was also sampled in the nearest mainland (˜2.5 km from gradient measurements) to determine the isotopic composition of background water vapor. Liquid samples were then analyzed with a Picarro L1102-i and Thermo-Fisher Delta Plus Advantage for water vapor and lagoon water, respectively. The last two experiments have also involved simultaneous measurements of relative humidity using commercially-available humidity probes at each height. This approach was used to determine a reference scale in order to compare observations to modeled estimates. Despite the coarse time resolution due to cryotrapping method (measurements are averaged over 1.5 hours), preliminary results show measurable differences in the isotopic composition of water vapor along the vertical gradient and good agreement between observations and predicted values from the model. Even if this work is an exploratory phase it shows an interesting potential to grow our understanding of the processes involved as well as a useful implementation for future studies focused on fractionation of water isotopes due to evaporation in natural conditions. References Craig, H., & Gordon, L. I. (1965). Deuterium and oxygen 18 variations in the ocean and the marine atmosphere.

Influence of West Antarctic Ice Sheet collapse on Antarctic surface climate

NASA Astrophysics Data System (ADS)

Steig, Eric J.; Huybers, Kathleen; Singh, Hansi A.; Steiger, Nathan J.; Ding, Qinghua; Frierson, Dargan M. W.; Popp, Trevor; White, James W. C.

2015-06-01

Climate model simulations are used to examine the impact of a collapse of the West Antarctic Ice Sheet (WAIS) on the surface climate of Antarctica. The lowered topography following WAIS collapse produces anomalous cyclonic circulation with increased flow of warm, maritime air toward the South Pole and cold-air advection from the East Antarctic plateau toward the Ross Sea and Marie Byrd Land, West Antarctica. Relative to the background climate, areas in East Antarctica that are adjacent to the WAIS warm, while substantial cooling (several °C) occurs over parts of West Antarctica. Anomalously low isotope-paleotemperature values at Mount Moulton, West Antarctica, compared with ice core records in East Antarctica, are consistent with collapse of the WAIS during the last interglacial period, Marine Isotope Stage 5e. More definitive evidence might be recoverable from an ice core record at Hercules Dome, East Antarctica, which would experience significant warming and positive oxygen isotope anomalies if the WAIS collapsed.

First application of calorimetric low-temperature detectors in accelerator mass spectrometry

NASA Astrophysics Data System (ADS)

Kraft, S.; Andrianov, V.; Bleile, A.; Egelhof, P.; Golser, R.; Kiseleva, A.; Kiselev, O.; Kutschera, W.; Meier, J. P.; Priller, A.; Shrivastava, A.; Steier, P.; Vockenhuber, C.

2004-03-01

For the first time, calorimetric low-temperature detectors were applied in accelerator mass spectrometry, a well-known method for determination of very small isotope ratios with high sensitivity. The aim of the experiment was to determine with high accuracy the isotope ratio of 236U/238U for several samples of natural uranium, 236U being known as a sensitive monitor for neutron flux. Measurements were performed at the VERA tandem accelerator at Vienna, Austria. The detectors consist of sapphire absorbers and superconducting transition edge thermometers operated at T≈ 1.5 K. The relative energy resolution obtained for 17.39 MeV 238U is ΔE/E=4-9×10-3, depending on the experimental conditions. This performance enabled to substantially reduce background from neighbouring isotopes and to increase the detection efficiency. Due to the high sensitivity achieved, a value of 236U/238U=6.5×10-12 could be obtained, representing the smallest 236U/238U ratio measured until now.

Isotopic Biogeochemistry

NASA Technical Reports Server (NTRS)

Hayes, J. M.

1985-01-01

An overview is provided of the biogeochemical research. The funding, productivity, personnel and facilities are reviewed. Some of the technical areas covered are: carbon isotopic records; isotopic studies of banded iron formations; isotope effects in microbial systems; studies of organic compounds in ancient sediments; and development in isotopic geochemistry and analysis.

Determination of the sources of nitrate contamination in karst springs using isotopic and chemical indicators

USGS Publications Warehouse

Panno, S.V.; Hackley, Keith C.; Hwang, H.-H.; Kelly, W.R.

2001-01-01

The sources of nitrate (NO-3) in groundwater of the shallow karst aquifer in southwestern Illinois' sinkhole plain were investigated using chemical and isotopic techniques. The groundwater in this aquifer is an important source of potable water for about half of the residents of the sinkhole plain area. Previous work has shown that groundwater from approximately 18% of the wells in the sinkhole plain has NO-3 concentrations in excess of the USEPA's drinking water standard of 10 mg N/1. Relative to background levels, the NO-3 concentrations in water from 52% of the wells, and probably all of the springs in the study area, are anomalously high, suggesting that sources other than naturally occurring soil organic matter have contributed additional NO-3 to groundwater in the shallow karst aquifer. This information, and the dominance of agriculture in the study area, suggest that agrichemical contributions may be significant. To test this hypothesis, water samples from 10 relatively large karst springs were collected during four different seasons and analyzed for inorganic constituents, dissolved organic carbon, atrazine, and ??15N and ??18O of the NO-3 ions. The isotopic data were most definitive and suggested that the sources of NO-3 in spring water are dominated by N-fertilizer with some possible influence of atmospheric NO-3 and, to a much lesser extent, human and/or animal waste. Differences in the isotopic composition of NO-3 and some of the chemical characteristics were observed during the four consecutive seasons in which spring water samples were collected. Isotopic values for ??15N and ??18O of the NO-3 ranged from 3.2??? to 19.1??? and from 7.2??? to 18.7???, respectively. The trend of ??15N and ??18O data for NO-3 also indicated that a significant degree of denitrification is occurring in the shallow karst hydrologic system (within the soil zone, the epikarst and the shallow karst aquifer) prior to discharging to springs. ?? 2001 Elsevier Science B.V. All rights reserved.

Contrasting isotopic signatures between anthropogenic and geogenic Zn and evidence for post-depositional fractionation processes in smelter-impacted soils from Northern France

NASA Astrophysics Data System (ADS)

Juillot, Farid; Maréchal, Chloe; Morin, Guillaume; Jouvin, Delphine; Cacaly, Sylvain; Telouk, Philipe; Benedetti, Marc F.; Ildefonse, Philippe; Sutton, Steve; Guyot, François; Brown, Gordon E., Jr.

2011-05-01

Zinc isotopes have been studied along two smelter-impacted soil profiles sampled near one of the largest Pb and Zn processing plants in Europe located in northern France, about 50 km south of Lille. Mean δ 66Zn values along these two soil profiles range from +0.22 ± 0.17‰ (2 σ) to +0.34 ± 0.17‰ (2 σ) at the lowest horizons and from +0.38 ± 0.45‰ (2 σ) to +0.76 ± 0.14‰ (2 σ) near the surface. The δ 66Zn values in the lowest horizons of the soils are interpreted as being representative of the local geochemical background (mean value +0.31 ± 0.38‰), whereas heavier δ 66Zn values near the surface of the two soils are related to anthropogenic Zn. This anthropogenic Zn occurs in the form of franklinite (ZnFe 2O 4)-bearing slag grains originating from processing wastes at the smelter site and exhibiting δ 66Zn values of +0.81 ± 0.20‰ (2 σ). The presence of franklinite is indicated by EXAFS analysis of the topsoil samples from both soil profiles as well as by micro-XANES analysis of the surface horizon of a third smelter-impacted soil from a distant site. These results indicate that naturally occurring Zn and smelter-derived Zn exhibit significantly different δ 66Zn values, which suggests that zinc isotopes can be used to distinguish between geogenic and anthropogenic sources of Zn in smelter-impacted soils. In addition to a possible influence of additional past sources of light Zn (likely Zn-sulfides and Zn-sulfates directly emitted by the smelter), the light δ 66Zn values in the surface horizons compared to smelter-derived slag materials are interpreted as resulting mainly from fractionation processes associated with biotic and/or abiotic pedological processes (Zn-bearing mineral precipitation, Zn complexation by organic matter, and plant uptake of Zn). This conclusion emphasizes the need for additional Zn isotopic studies before being able to use Zn isotopes to trace sources and pathways of this element in surface environments.

Characterizing fallout material using Cs and Pu atom ratios in environmental samples from the FDNPP fallout zone

NASA Astrophysics Data System (ADS)

Richards, David; Dunne, James; Martin, Peter; Scott, Tom; Yamashiki, Yosuke; Coath, Chris; Chen, Hart

2017-04-01

Here we report the use of combined of Cs and Pu isotope measurements to investigate the extensive plumes of radioactive fallout from the disaster at Fukishima Daiichi nuclear power plant (FNDPP) in March 2011. Among the aims of our study are improved assessment of the physico-chemical nature and changing distribution of land-based fallout. 135Cs/137Cs and 134Cs/137Cs atom ratios are indicative of conditions that relate to the nuclear fission reactions responsible for producing the respective radiocaesium isotopes, and offer much more in terms of forensic and chronological analysis than monitoring 137Cs alone. We briefly present methods to quantify the atom ratios of Cs and Pu isotopes in soil, lichen and moss samples from FDNPP catchment using mass spectrometry (ThermoTRITON for Cs and ThermoNEPTUNE for Pu). High precision data from Fukushima are presented (e.g decay corrected 135Cs/137Cs atom ratio = 0.384 ± 0.001 (n = 5) for roadside dust from Iitate region), and these are in agreement with prelimary estimates by others. We also confirm results for IAEA-330, a spinach sample collected from Polesskoe, Ukraine and subject to contamination from the Chernobyl accident. In addition to Cs isotopes, we adopt Pu isotopes to add a further dimension to the forensic analysis. We discuss the corrections required for background levels prior to the disaster, possibility for multiple components of fallout and complicating factors associated with remobilisation during the clean-up operation. In parallel with this work on digests and leaches from bulk environmental samples, we are refining methods for particle identification, isolation and characterisation using a complementary sequence of cutting-edge materials and manipulation techniques, including combined electron microscopy, focused ion beam techniques (Dualbeam), nano/micro manipulators and nano-scale imaging x-ray photoelectron spectroscopy (NanoESCA) and microCT.

Role of Megafauna and Frozen Soil in the Atmospheric CH4 Dynamics

PubMed Central

Zimov, Sergey; Zimov, Nikita

2014-01-01

Modern wetlands are the world’s strongest methane source. But what was the role of this source in the past? An analysis of global 14C data for basal peat combined with modelling of wetland succession allowed us to reconstruct the dynamics of global wetland methane emission through time. These data show that the rise of atmospheric methane concentrations during the Pleistocene-Holocene transition was not connected with wetland expansion, but rather started substantially later, only 9 thousand years ago. Additionally, wetland expansion took place against the background of a decline in atmospheric methane concentration. The isotopic composition of methane varies according to source. Owing to ice sheet drilling programs past dynamics of atmospheric methane isotopic composition is now known. For example over the course of Pleistocene-Holocene transition atmospheric methane became depleted in the deuterium isotope, which indicated that the rise in methane concentrations was not connected with activation of the deuterium-rich gas clathrates. Modelling of the budget of the atmospheric methane and its isotopic composition allowed us to reconstruct the dynamics of all main methane sources. For the late Pleistocene, the largest methane source was megaherbivores, whose total biomass is estimated to have exceeded that of present-day humans and domestic animals. This corresponds with our independent estimates of herbivore density on the pastures of the late Pleistocene based on herbivore skeleton density in the permafrost. During deglaciation, the largest methane emissions originated from degrading frozen soils of the mammoth steppe biome. Methane from this source is unique, as it is depleted of all isotopes. We estimated that over the entire course of deglaciation (15,000 to 6,000 year before present), soils of the mammoth steppe released 300–550 Pg (1015 g) of methane. From current study we conclude that the Late Quaternary Extinction significantly affected the global methane cycle. PMID:24695117

An annually-resolved stalagmite tropical cyclone reconstruction from Belize reveals a northward shift in North Atlantic storm track position since 1550 C.E.

NASA Astrophysics Data System (ADS)

Baldini, Lisa; Baldini, James; McElwaine, Jim; Frappier, Amy; Asmerom, Yemane; Liu, Kam-biu; Prufer, Keith; Ridley, Harriet; Polyak, Victor; Kennett, Douglas; Macpherson, Colin; Aquino, Valorie; Awe, Jaime; Breitenbach, Sebastian

2017-04-01

Hurricanes are large-scale atmospheric phenomena that typically produce high volume, high intensity, and isotopically depleted rainfall. Such storms have the ability to alter the isotopic composition of the groundwater reservoir, imparting a uniquely negative isotopic fingerprint to actively growing stalagmites. In regions influenced by the Intertropical Convergence Zone (ITCZ), large volumes of rainfall delivered during the wet season can obscure the tropical cyclone (TC) rainfall proxy signal. Coupled annually resolved carbon and oxygen isotope ratios were used to isolate the low δ18O TC signal from the isotopically more enriched background rainfall associated with seasonal ITCZ migration. The new composite stalagmite proxy record yielded a 99.7% significant correlation with the western Caribbean-filtered HURDAT2 database over the instrumental record based on a non-parametric bootstrap approach. The new annually-resolved TC reconstruction for the western Caribbean spans the last 450 years and reveals a peak in western Caribbean TCs at 1650 C.E. and a gradual decline until a marked decrease is observed at the start of the Industrial Era. Comparison with documentary records of TC occurrence along the US eastern seaboard reveals a clear pattern of north-eastward TC track migration since peak Little Ice Age cooling. This pattern is consistent with natural warming since the Little Ice Age temperature minimum and with anthropogenic influences after industrialisation. Satellite observations reveal Hadley cell expansion has occurred over the last three decades and modelling studies implicate rising atmospheric greenhouse gas concentrations as the driver. Our results suggest that Hadley cell position and width is a major control on hurricane track position and that future emissions scenarios (continued rising greenhouse gases coupled with decreasing Northern Hemisphere aerosol emissions) are likely to increase storm risk to the north-eastern USA.

Improvements in Precise and Accurate Isotope Ratio Determination via LA-MC-ICP-MS by Application of an Alternative Data Reduction Protocol

NASA Astrophysics Data System (ADS)

Fietzke, J.; Liebetrau, V.; Guenther, D.; Frische, M.; Zumholz, K.; Hansteen, T. H.; Eisenhauer, A.

2008-12-01

An alternative approach for the evaluation of isotope ratio data using LA-MC-ICP-MS will be presented. In contrast to previously applied methods it is based on the simultaneous responses of all analyte isotopes of interest and the relevant interferences without performing a conventional background correction. Significant improvements in precision and accuracy can be achieved when applying this new method and will be discussed based on the results of two first methodical applications: a) radiogenic and stable Sr isotopes in carbonates b) stable chlorine isotopes of pyrohydrolytic extracts. In carbonates an external reproducibility of the 87Sr/86Sr ratios of about 19 ppm (RSD) was achieved, an improvement of about a factor of 5. For recent and sub-recent marine carbonates a mean radiogenic strontium isotope ratio 87Sr/86Sr of 0.709170±0.000007 (2SE) was determined, which agrees well with the value of 0.7091741±0.0000024 (2SE) reported for modern sea water [1,2]. Stable chlorine isotope ratios were determined ablating pyrohydrolytic extracts with a reproducibility of about 0.05‰ (RSD). For basaltic reference material JB1a and JB2 chlorine isotope ratios were determined relative to SMOC (standard mean ocean chlorinity) δ37ClJB-1a = (-0.99±0.06) ‰ and δ37ClJB-1a = (-0.60±0.03) ‰ (SD), respectively, in accordance with published data [3]. The described strategies for data reduction are considered to be generally applicable for all isotope ratio measurements using LA-MC-ICP-MS. [1] J.M. McArthur, D. Rio, F. Massari, D. Castradori, T.R. Bailey, M. Thirlwall, S. Houghton, Palaeogeo. Palaeoclim. Palaeoeco., 2006, 242 (126), doi: 10.1016/j.palaeo.2006.06.004 [2] J. Fietzke, V. Liebetrau, D. Guenther, K. Guers, K. Hametner, K. Zumholz, T.H. Hansteen and A. Eisenhauer, J. Anal. At. Spectrom., 2008, 23, 955-961, doi:10.1039/B717706B [3] J. Fietzke, M. Frische, T.H. Hansteen and A. Eisenhauer, J. Anal. At. Spectrom., 2008, 23, 769-772, doi:10.1039/B718597A

Imprint of CO2 emission in atmosphere and biosphere on the basis of 14C and 13C measurements

NASA Astrophysics Data System (ADS)

Pazdur, Anna; Gabryś, Alicja; Kuc, Tadeusz; Pawełczyk, Sławomira; Piotrowska, Natalia; Rakowski, Andrzej; Różański, Kazimierz; Sensuła, Barbara

2015-04-01

As is shown in the IPCC (Intergovernmental Panel on Climate Change) report, the observed climate changes are caused, among others, by human activity. Mainly emission of CO2 to the atmosphere coming from the burning of fossil fuels, can have dire consequences for life on Earth and development of humankind. The report uses, among others, data obtained from isotopic measurements in the biosphere. Measurements of 14C and 13C concentration in modern atmospheric carbon dioxide and biosphere allow the determination of the decrease of the concentration of this isotope. Furthermore, the magnitude of emission to the atmosphere of carbon dioxide not containing the isotope 14C can be estimated on this basis. Such emission stems from fossil fuel combustion - petroleum, natural gas and black coal. A sensitive bioindicator of the emission are annual tree rings. The measurements of 14C concentration in tree ring material using AMS allow to see its seasonal changes. Trees, treated as an archive of changes in conjunction with information about the isotopic composition of carbon can be used for monitoring of environment as sensitive bioindicators on local, as well as on the global scale. Regular investigations of isotopic composition of carbon in trees have been carried out in the GADAM Centre for the urban areas of both Poland and worldwide. This method can be applied in the study of the emission of CO2 to the atmosphere and its spatial and temporal distribution connected with the production of energy by power plants based on fossil fuel combustion for the area of southern Poland. Modelling of CO2 emission using both 14C and 13C carbon isotopes measured in pine tree rings on the background of climatic changes will be presented. The national ecological policy in the era of global warming requires the manufacturers of energy to get involved in the development of methods suitable for monitoring the state of the environment. Hence, the interest in the area of monitoring the fossil fuel component in CO2 in our region is rising. The measurements of 14C (by AMS method) and 13C isotopes have been carried out in atmospheric CO2 and plants in the Gliwice city centre. A high decrease of both isotopes contents and their short-term seasonal changes during the year caused by human impact during the year are observed.

Modeling calcification periods of Cytheridella ilosvayi from Florida based on isotopic signatures and hydrological data

NASA Astrophysics Data System (ADS)

Meyer, Juliane; Wrozyna, Claudia; Leis, Albrecht; Piller, Werner E.

2017-11-01

The isotopic signatures of ostracod shells are the result of the temperature and composition of their host water and the phenology and ecology of the target species. Investigations addressing the influence of site-specific environmental variations on the isotopic ranges of ostracod shells are still rare but can provide important information on habitat-dependent variations and may signify a seasonally restricted timing of calcification periods. Here we present isotopic signatures (δ18Oostr, δ13Costr) of living Cytheridella ilosvayi (Ostracoda) and physical, chemical, and isotopic (δD, δ18Owater, δ13CDIC) compositions of 14 freshwater habitats (rivers, lakes, canals, marshes, sinkholes) in South Florida from winter 2013 and summer 2014. We also present instrumental data of river temperatures and δ18O of precipitation (δ18Oprec) from this region. The physicochemical and isotopic compositions of the selected sites characterize the different habitats and show the influence of the source water, biological activity, and duration of exposure to the surface. Mean δ18Oostr and δ13Costr signatures of C. ilosvayi shells correlate well with the isotopic composition of their host waters. Within-sample variabilities in repeated isotopic measurements of single ostracod shells reflect habitat-dependent ranges. The similarly high range of ostracod δ18O in rivers and one marsh sample indicates that both temperature and δ18Oprec are responsible for their variation in the whole study area. Rivers and canals, which are predominantly influenced by the input and mixing of inorganic carbon from the catchment, show smaller δ13Costr ranges than the marsh dominated by local fluctuations in biological activities. Based on these observations, background data of water temperatures and δ18Oprec were used to calculate monthly δ18O variations in a theoretical calcite formed in rivers in Florida assuming a direct reaction on precipitation changes. The calculated values showed a high variation coupled with low mean values during the summer wet season, while during the winter dry season the variation remains small and mean values increased. Inferred configurations were used to approximate possible calcification periods of C. ilosvayi. For a plausible calcification period, mean values and ranges of δ18Oostr had to be equal to the theoretical calcite with a slight positive offset (vital effect). The applied model suggests a seasonal calcification period of C. ilosvayi in early spring that is probably coupled to the hydrologic cycle of Florida.

Mass Spectrometric Determination of Uranium and Thorium in High Radiopurity Polymers Using Ultra Low Background Electroformed Copper Crucibles for Dry Ashing.

PubMed

Arnquist, Isaac J; Hoppe, Eric J; Bliss, Mary; Grate, Jay W

2017-03-07

A rapid new method for determining the U and Th mass concentrations in high radiopurity plastics is described, consisting of (1) dry ashing the plastic sample and tracers in low mass crucibles made of ultra low background electroformed copper (ULB EF-Cu) foil cut and folded into boats, (2) dissolving both the ash and the boat in acid, (3) performing a column separation to remove copper, and (4) determining the elements of interest by isotope dilution mass spectrometry. This method was demonstrated on both unfluorinated and fluorinated plastics, demonstrating high tracer recoveries and detection limits to pg/g (i.e., parts per trillion) levels or below, corresponding to μBq/kg of material. Samples of biomedical polyester (Max-Prene 955) and a fluoropolymer (polyvinylidene fluoride, PVDF) were analyzed in powder raw material forms as well as solids in the form of pellets or injection molded parts. The polyester powder contained 6 pg/g and 2 pg/g for 232 Th and 238 U, respectively. These levels correspond to 25 and 25 μBq/kg radioactivity, respectively. Determinations on samples of PVDF powder were typically below 1 pg/g for 232 Th and 2 pg/g for 238 U, corresponding to 4 and 25 μBq/kg radioactivity, respectively. The use of low mass ULB EF-Cu boats for dry ashing successfully overcame the problem of crucible-generated contaminants in the analysis; absolute detection limits, calculated as 3 × standard deviation of the process blanks, were typically 20-100 fg within a sample set. Complete dissolution of the ash and low mass boat provided high tracer recoveries and provides a convincing method to recover both the tracer and sample isotopes when full equilibration of tracer isotopes with sample isotopes is not possible prior to beginning chemical sample processing on solids.

Preliminary assessment of rover power systems for the Mars Rover Sample Return Mission

NASA Technical Reports Server (NTRS)

Bents, David J.

1989-01-01

Four isotope power system concepts were presented and compared on a common basis for application to on-board electrical prime power for an autonomous planetary rover vehicle. A representative design point corresponding to the Mars Rover Sample Return (MRSR) preliminary mission requirements (500 W) was selected for comparison purposes. All systems concepts utilize the General Purpose Heat Source (GPHS) isotope heat source developed by DOE. Two of the concepts employ thermoelectric (TE) conversion: one using the GPHS Radioisotope Thermoelectric Generator (RTG) used as a reference case, the other using an advanced RTG with improved thermoelectric materials. The other two concepts employed are dynamic isotope power systems (DIPS): one using a closed Brayton cycle (CBC) turboalternator, and the other using a free piston Stirling cycle engine/linear alternator (FPSE) with integrated heat source/heater head. Near term technology levels have been assumed for concept characterization using component technology figure-of-merit values taken from the published literature. For example, the CBC characterization draws from the historical test database accumulated from space Brayton cycle subsystems and components from the NASA B engine through the mini-Brayton rotating unit. TE system performance is estimated from Voyager/multihundred Watt (MHW)-RTG flight experience through Mod-RTG performance estimates considering recent advances in TE materials under the DOD/DOE/NASA SP-100 and NASA Committee on Scientific and Technological Information programs. The Stirling DIPS system is characterized from scaled-down Space Power Demonstrator Engine (SPDE) data using the GPHS directly incorporated into the heater head. The characterization/comparison results presented here differ from previous comparison of isotope power (made for Low Earth Orbit (LEO) applications) because of the elevated background temperature on the Martian surface compared to LEO, and the higher sensitivity of dynamic systems to elevated sink temperature. The mass advantage of dynamic systems is significantly reduced for this application due to Mars' elevated background temperature.

Mass Spectrometric Determination of Uranium and Thorium in High Radiopurity Polymers Using Ultra Low Background Electroformed Copper Crucibles for Dry Ashing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arnquist, Isaac J.; Hoppe, Eric J.; Bliss, Mary

A rapid new method for determining the U and Th mass concentrations in high radiopurity plastics is described, consisting of 1) dry ashing the plastic sample and tracers in low mass crucibles made of ultra low background electroformed copper (ULB EF-Cu) foil cut and folded into boats, 2) dissolving both the ash and the boat in acid, 3) performing a column separation to remove copper, and 4) determining the elements of interest by isotope dilution mass spectrometry. This method was demonstrated on both unfluorinated and fluorinated plastics, demonstrating high tracer recoveries and detection limits to pg/g (i.e., parts per trillion)more » levels or below, corresponding to μBq/kg of material. Samples of biomedical polyester (Max-Prene® 955) and a fluoropolymer (polyvinylidene fluoride, PVDF) were analyzed in powder raw material forms as well as solids in the form of pellets or injection molded parts. The polyester powder contained 6 pg/g and 2 pg/g for Th and U respectively. These levels correspond to 25 and 25 μBq/kg radioactivity, respectively. Determinations on samples of PVDF powder were typically below 1 pg/g for Th and 2 pg/g for U, corresponding to 4 and 25 μBq/kg radioactivity, respectively. The use of low mass ULB EF-Cu boats for dry ashing successfully overcame the problem of crucible-generated contaminants in the analysis; absolute detection limits, calculated as 3 × standard deviation of the process blanks, were typically 20-100 fg within a sample set. Complete dissolution of the ash and low mass boat provided high tracer recoveries, and provides a convincing method to recover both the tracer and sample isotopes when full equilibration of tracer isotopes with sample isotopes is not possible prior to beginning chemical sample processing on solids.« less

Stable isotopes of carbon dioxide in soil gas over massive sulfide mineralization at Crandon, Wisconsin

USGS Publications Warehouse

Alpers, Charles N.; Dettman, D.L.; Lohmann, K.C.; Brabec, D.

1990-01-01

Stable isotope ratios of oxygen and carbon were determined for CO2 in soil gas in the vicinity of the massive sulfide deposit at Crandon, Wisconsin with the objective of determining the source of anomalously high CO2 concentrations detected previously by McCarthy et al. (1986). Values of ??13C in soil gas CO2 from depths between 0.5 and 1.0 m were found to range from -12.68??? to -20.03??? (PDB). Organic carbon from the uppermost meter of soil has ??13C between -24.1 and -25.8??? (PDB), indicating derivation from plant species with the C3 (Calvin) type of photosynthetic pathway. Microbial decomposition of the organic carbon and root respiration from C3 and C4 (Hatch-Slack) plants, together with atmospheric CO2 are the likely sources of carbon in soil gas CO2. Values of ??18O in soil-gas CO2 range from 32 to 38??? (SMOW). These ??18O values are intermediate between that calculated for CO2 gas in isotopic equilibrium with local groundwaters and that for atmospheric CO2. The ??18O data indicate that atmospheric CO2 has been incorporated by mixing or diffusion. Any CO2 generated by microbial oxidation of organic matter has equilibrated its oxygen isotopes with the local groundwaters. The isotopic composition of soil-gas CO2 taken from directly above the massive sulfide deposit was not distinguishable from that of background samples taken 1 to 2 km away. No enrichment of the ??13C value of soil-gas CO2 was observed, contrary to what would be expected if the anomalous CO2 were derived from the dissolution of Proterozoic marine limestone country rock or of Paleozoic limestone clasts in glacial till. Therefore, it is inferred that root respiration and decay of C3 plant material were responsible for most CO2 generation both in the vicinity of the massive sulfide and in the "background" area, on the occasion of our sampling. Interpretation of our data is complicated by the effects of rainfall, which significantly reduced the magnitude of the CO2 anomaly. Therefore, we cannot rule out the possible mechanism of carbonate dissolution driven by pyrite oxidation, as proposed by Lovell et al. (1983) and McCarthy et al. (1986). Further work is needed on seasonal and daily variations of CO2 concentrations and stable isotope ratios in various hydrogeologic and ecologic settings so that more effective sampling strategies can be developed for mineral exploration using soil gases. ?? 1990.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Facchetti, S.

Many studies were dedicated to the evaluation of the impact of automotive lead on the environment and to the assessment of its absorption in the human population. They can be subdivided into two groups, those based on changes of air and blood lead concentrations and those based on changes of air and blood lead isotopic compositions. According to various authors, 50-66% of the lead added to petrol is mobilized in the atmosphere, while most of the remainder adheres to the walls of the exhaust system from which it is expelled by mechanical and thermal shocks in the forms of easilymore » sedimented particles. The fraction directly emitted by engine exhaust fumes is found in the form of fine particles, which can be transferred a long way from the emitting sources. However important the contribution of petrol lead to the total airborne lead may be, our knowledge does not permit a straightforward calculation of the percentage of petrol lead in total blood lead, which of course can also originate from other sources (e.g., industrial, natural). To evaluate this percentage in 1973, the idea of the Isotopic Lead Experiment (ILE project) was conceived to label, on a regional scale, petrol with a nonradioactive lead of an isotopic composition sufficiently different from that of background lead and sufficiently stable in time. This Account summarizes the main results obtained by the ILE project.« less

Mobilisation of traffic-derived trace metals from road corridors into coastal stream and estuarine sediments, Cairns, northern Australia

NASA Astrophysics Data System (ADS)

Pratt, C.; Lottermoser, B. G.

2007-04-01

This investigation revealed the presence of traffic-derived metals within road, stream and estuarine sediments collected from a coastal catchment, northern Australia. Studied road sediments displayed variable total metal concentrations (median Cd, Cu, Pb, Pd, Pt, Ni and Zn values: 0.19, 42.6, 67.5, 0.064, 0.104, 36.7 and 698 mg/kg, respectively). The distinctly elevated Zn values are due to abundant tyre rubber shreds (as verified by SEM-EDS and correlation analysis). By comparison to the road sediments, background stream sediments taken upstream from roads have relatively low median Pb, Pd, Pt and Zn concentrations (7.3 mg/kg Pb, 0.01 mg/kg Pd, 0.012 mg/kg Pt, 62 mg/kg Zn). Stream and estuarine sediment samples collected below roads have median values of 21.8 mg/kg Pb, 0.014 mg/kg Pd, 0.021 mg/kg Pt and 71 mg/kg Zn, and exhibit 207Pb/206Pb and 208Pb/206Pb ratios that appear on a mixing line between the isotopically distinct background stream sediments and the road sediments. Thus, mobilisation of dusts and sediments from road surfaces has resulted in relatively elevated Pb, Pd, Pt and Zn concentrations and non-radiogenic Pb isotope ratios in local coastal stream and estuarine sediments. The investigation demonstrates that traffic-derived metals enter coastal stream and estuary sediments at the fringe of the Great Barrier Reef lagoon.

Variability of Fe isotope compositions of hydrothermal sulfides and oxidation products at mid-ocean ridges

NASA Astrophysics Data System (ADS)

Li, Xiaohu; Wang, Jianqiang; Chu, Fengyou; Wang, Hao; Li, Zhenggang; Yu, Xing; Bi, Dongwei; He, Yongsheng

2018-04-01

Significant Fe isotopic fractionation occurs during the precipitation and oxidative weathering of modern seafloor hydrothermal sulfides, which has an important impact on the cycling of Fe isotopes in the ocean. This study reports the Fe-isotope compositions of whole-rock sulfides and single-mineral pyrite collected from hydrothermal fields at the South Mid-Atlantic Ridge (SMAR) and the East Pacific Rise (EPR) and discusses the impacts of precipitation and late-stage oxidative weathering of sulfide minerals on Fe isotopic fractionation. The results show large variation in the Fe-isotope compositions of the sulfides from the different hydrothermal fields on the mid-oceanic ridges, indicating that relatively significant isotope fractionation occurs during the sulfide precipitation and oxidative weathering processes. The Fe-isotope compositions of the sulfides from the study area at the SMAR vary across a relatively small range, with an average value of 0.01‰. This Fe-isotope composition is similar to the Fe-isotope composition of mid-oceanic ridge basalt, which suggests that Fe was mainly leached from basalt. In contrast, the Fe-isotope composition of the sulfides from the study area at the EPR are significantly enriched in light Fe isotopes (average value - 1.63‰), mainly due to the kinetic fractionation during the rapid precipitation process of hydrothermal sulfide. In addition, the pyrite from different hydrothermal fields is enriched in light Fe isotopes, which is consistent with the phenomenon in which light Fe isotopes are preferentially enriched during the precipitation of pyrite. The red oxides have the heaviest Fe-isotope compositions (up to 0.80‰), indicating that heavy Fe isotopes are preferentially enriched in the oxidation product during the late-stage oxidation process. The data obtained from this study and previous studies show a significant difference between the Fe-isotope compositions of the sulfides from the SMAR and EPR. The relatively heavy Fe isotopes compositions of the sulfides from the SMAR may suggest the equilibrium fractionation process under high temperature conditions. The red Fe oxides are enriched in heavy Fe isotopes, indicating that the oxidative weathering processes result in the occurrence of significant Fe-isotope fractionation and the preferential enrichment of heavy Fe isotopes in the oxidation product.

On-line Differential Thermal Isotope Analysis: A New Method for Measuring Oxygen and Hydrogen Isotopes of Hydration Water in Minerals

NASA Astrophysics Data System (ADS)

Bauska, T.; Hodell, D. A.; Walters, G.

2016-12-01

Oxygen (16O,17O,18O) and hydrogen (H,D) isotopes of hydration water in minerals provide a rich source of information about the conditions under which hydrated minerals form on Earth and other planetary bodies (e.g. Mars). We have developed a new method for measuring different types of bonded water (e.g., molecular, hydroxyl) contained in hydrated minerals by coupling a thermal gravimeter (TG) and a cavity ringdown laser spectrometer (CRDS). The method involves step heating a mineral sample, precisely measuring the weight loss and enthalpy as the sample undergoes dehydration and dehydroxylation, whilst simultaneously determining the oxygen and hydrogen isotopes of the water vapor evolved from the mineral sample by cavity ring-down laser spectroscopy (CRDS). Nitrogen carrier gas is used to transfer the sample from the TG to the CRDS via a heated line and interface box. The interface includes the capability of (i) cryogenic trapping discrete types of water for samples containing small amounts of water; (ii) injecting small quantities of water of known isotopic value for calibration; and (iii) converting volatile organic compounds to nascent amounts of water using a catalyst. The CRDS continually measures water vapor concentration in the optical cavity and hydrogen and oxygen isotope ratios. Isotopic values are calculated by integrating the product of the water amount and its isotopic value for the separated peaks after correcting for background. Precision of the method was estimated by comparing isotope results of total water for gypsum measured by DTIA with our conventional method of extraction and analysis (Gázquez et al., 2015. Rapid Communications in Mass Spectrometry, 29, 1997-2006). Errors for the isotopic values of total hydration water vary between ±0.08 and ±0.34 ‰ for δ18O and between ±0.16 and ±0.86 ‰ for δD. We demonstrate the application of the DTIA method to a variety of hydrous minerals and mineraloids including gypsum, clays, and amorphous silica (opal, glass, chert). The DTIA method has wide ranging application for addressing fundamental problems across many disciplines in Earth and Planetary Sciences, including: paleoclimatology, sedimentology, volcanology, water exchange between the solid earth and hydrosphere, and water on Mars and other planetary bodies.

Investigation of off-site airborne transport of lead from a superfund removal action site using lead isotope ratios and concentrations

USGS Publications Warehouse

Pribil, Michael J.; Maddaloni, Mark A.; Staiger, Kimberly; Wilson, Eric; Magriples, Nick; Ali, Mustafa; Santella, Dennis

2014-01-01

Lead (Pb) concentration and Pb isotopic composition of surface and subsurface soil samples were used to investigate the potential for off-site air transport of Pb from a former white Pb processing facility to neighboring residential homes in a six block area on Staten Island, NY. Surface and subsurface soil samples collected on the Jewett White Pb site were found to range from 1.122 to 1.138 for 206Pb/207Pb and 2.393 to 2.411 for 208Pb/207Pb. The off-site surface soil samples collected from residential backyards, train trestle, near site grass patches and background areas varied from 1.144 to 1.196 for 206Pb/207Pb and 2.427 to 2.464 for 208Pb/207Pb. Two soil samples collected along Richmond Terrace, where Jewett site soils accumulated after major rain events, varied from 1.136 to 1.147 for 206Pb/207Pb and 2.407 to 2.419 for 208Pb/207Pb. Lead concentration for on-site surface soil samples ranged from 450 to 8000 ug/g, on-site subsurface soil samples ranged from 90,000 to 240,000 ug/g and off-site samples varied from 380 to 3500 ug/g. Lead concentration and isotopic composition for the Staten Island off-site samples were similar to previously published data for other northeastern US cities and reflect re-suspension and re-mobilization of local accumulated Pb. The considerable differences in both the Pb isotopic composition and Pb concentration of on-site and off-site samples resulted in the ability to geochemically trace the transport of particulate Pb. Data in this study indicate minimal off-site surface transport of Pb from the Jewett site into the neighboring residential area.

Occurrence of selected trace metals and their oral bioaccessibility in urban soils of kindergartens and parks in Bratislava (Slovak Republic) as evaluated by simple in vitro digestion procedure.

PubMed

Hiller, Edgar; Mihaljevič, Martin; Filová, Lenka; Lachká, Lucia; Jurkovič, Ľubomír; Kulikova, Tatsiana; Fajčíková, Katarína; Šimurková, Mária; Tatarková, Veronika

2017-10-01

A total of eighty surface soil samples were collected from public kindergartens and urban parks in the city of Bratislava, and the <150µm soil fraction was evaluated for total concentrations of five metals, Cd, Cu, Hg, Pb and Zn, their oral bioaccessibilities, non-carcinogenic and carcinogenic health risks to children, and lead isotopic composition. The mean metal concentrations in urban soils (0.29, 36.1, 0.13, 30.9 and 113mg/kg for Cd, Cu, Hg, Pb and Zn, respectively) were about two times higher compared with background soil concentrations. The order of bioaccessible metal fractions determined by Simple Bioaccessibility Extraction Test was: Pb (59.9%) > Cu (43.8%) > Cd (40.8%) > Zn (33.6%) > Hg (12.8%). Variations in the bioaccessible metal fractions were mainly related to the total metal concentrations in urban soils. A relatively wide range of lead isotopic ratios in urban soils (1.1598-1.2088 for 206 Pb/ 207 Pb isotopic ratio) indicated a combination of anthropogenic and geogenic sources of metals in the soils. Lower values of 206 Pb/ 207 Pb isotopic ratio in the city centre and similar spatial distribution of total metal concentrations, together with their increasing total concentrations in soils towards the city centre, showed that traffic and coal combustion in former times were likely the major sources of soil contamination. The non-carcinogenic and carcinogenic health risks to children due to exposure to metals in kindergarten and urban park soils were low, with hazard index and cancer risk values below the threshold values at all studied sites. Copyright © 2017 Elsevier Inc. All rights reserved.

An overview of methods using (13)C for improved compound identification in metabolomics and natural products.

PubMed

Clendinen, Chaevien S; Stupp, Gregory S; Ajredini, Ramadan; Lee-McMullen, Brittany; Beecher, Chris; Edison, Arthur S

2015-01-01

Compound identification is a major bottleneck in metabolomics studies. In nuclear magnetic resonance (NMR) investigations, resonance overlap often hinders unambiguous database matching or de novo compound identification. In liquid chromatography-mass spectrometry (LC-MS), discriminating between biological signals and background artifacts and reliable determination of molecular formulae are not always straightforward. We have designed and implemented several NMR and LC-MS approaches that utilize (13)C, either enriched or at natural abundance, in metabolomics applications. For LC-MS applications, we describe a technique called isotopic ratio outlier analysis (IROA), which utilizes samples that are isotopically labeled with 5% (test) and 95% (control) (13)C. This labeling strategy leads to characteristic isotopic patterns that allow the differentiation of biological signals from artifacts and yield the exact number of carbons, significantly reducing possible molecular formulae. The relative abundance between the test and control samples for every IROA feature can be determined simply by integrating the peaks that arise from the 5 and 95% channels. For NMR applications, we describe two (13)C-based approaches. For samples at natural abundance, we have developed a workflow to obtain (13)C-(13)C and (13)C-(1)H statistical correlations using 1D (13)C and (1)H NMR spectra. For samples that can be isotopically labeled, we describe another NMR approach to obtain direct (13)C-(13)C spectroscopic correlations. These methods both provide extensive information about the carbon framework of compounds in the mixture for either database matching or de novo compound identification. We also discuss strategies in which (13)C NMR can be used to identify unknown compounds from IROA experiments. By combining technologies with the same samples, we can identify important biomarkers and corresponding metabolites of interest.

DETERMINATION OF THE BACKGROUND WHILE MEASURING ACTIVITIES OF THE ORDER OF 10$sup -11$ TO 10$sup -13$ CURIE (in Russian)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Artem'ev, V.V.

1962-11-01

Activity measurements must be occasionally carried out in presence of a background radiation with a higher value than the radiation under study. Such cases are encountered in geological prospecting, biological and medical experiments with isotopes having half life periods longer than 10 years, requiring instruments with sensisitivities exceeding the 10/sup -13/ to 10/sup - 14/ curie range. Measurement of activities from 10/sup -11/ to 10/sup -13/ curie with an error of less than 1% requires tens of hours during which the background may vary radically because of the variations of cosmic rays and solar flares. In radiochemical dating studies themore » background usually consists of a constant component due to natural radioactive materials such as KID, and decay products of the U and Th series, and of a variable component primarily controlled by the cosmic radiation. Multiple scattering and absorption events cause a spreading of the spectral lines in neighboring portions of the spectrum of the background radiation; the changes in the second component may be determined by decomposing the count rate. The method was used successfully in mass determinations of C/sup 14/ in geological and archeological samples. The C sample was used to prepare ethyl benzene in which scintillating compounds, such as 2,5 diphenyl oxazol and 1,4-STAdi2,5 phenyl oxazolyl! benzene were dissolved, measuring the activity by means of a scintillation counter and a photomultiplier. (TTT)« less

Improved performance comparisons of radioxenon systems for low level releases in nuclear explosion monitoring.

PubMed

Haas, Derek A; Eslinger, Paul W; Bowyer, Theodore W; Cameron, Ian M; Hayes, James C; Lowrey, Justin D; Miley, Harry S

2017-11-01

The Comprehensive Nuclear-Test-Ban Treaty bans all nuclear tests and mandates development of verification measures to detect treaty violations. One verification measure is detection of radioactive xenon isotopes produced in the fission of actinides. The International Monitoring System (IMS) currently deploys automated radioxenon systems that can detect four radioxenon isotopes. Radioxenon systems with lower detection limits are currently in development. Historically, the sensitivity of radioxenon systems was measured by the minimum detectable concentration for each isotope. In this paper we analyze the response of radioxenon systems using rigorous metrics in conjunction with hypothetical representative releases indicative of an underground nuclear explosion instead of using only minimum detectable concentrations. Our analyses incorporate the impact of potential spectral interferences on detection limits and the importance of measuring isotopic ratios of the relevant radioxenon isotopes in order to improve discrimination from background sources particularly for low-level releases. To provide a sufficient data set for analysis, hypothetical representative releases are simulated every day from the same location for an entire year. The performance of three types of samplers are evaluated assuming they are located at 15 IMS radionuclide stations in the region of the release point. The performance of two IMS-deployed samplers and a next-generation system is compared with proposed metrics for detection and discrimination using representative releases from the nuclear test site used by the Democratic People's Republic of Korea. Copyright © 2017 Elsevier Ltd. All rights reserved.

Enhanced sensitivity of DNA- and rRNA-based stable isotope probing by fractionation and quantitative analysis of isopycnic centrifugation gradients.

PubMed

Lueders, Tillmann; Manefield, Mike; Friedrich, Michael W

2004-01-01

Stable isotope probing (SIP) of nucleic acids allows the detection and identification of active members of natural microbial populations that are involved in the assimilation of an isotopically labelled compound into nucleic acids. SIP is based on the separation of isotopically labelled DNA or rRNA by isopycnic density gradient centrifugation. We have developed a highly sensitive protocol for the detection of 'light' and 'heavy' nucleic acids in fractions of centrifugation gradients. It involves the fluorometric quantification of total DNA or rRNA, and the quantification of either 16S rRNA genes or 16S rRNA in gradient fractions by real-time PCR with domain-specific primers. Using this approach, we found that fully 13C-labelled DNA or rRNA of Methylobacterium extorquens was quantitatively resolved from unlabelled DNA or rRNA of Methanosarcina barkeri by cesium chloride or cesium trifluoroacetate density gradient centrifugation respectively. However, a constant low background of unspecific nucleic acids was detected in all DNA or rRNA gradient fractions, which is important for the interpretation of environmental SIP results. Consequently, quantitative analysis of gradient fractions provides a higher precision and finer resolution for retrieval of isotopically enriched nucleic acids than possible using ethidium bromide or gradient fractionation combined with fingerprinting analyses. This is a prerequisite for the fine-scale tracing of microbial populations metabolizing 13C-labelled compounds in natural ecosystems.

Hydrothermal activity lowers trophic diversity in Antarctic hydrothermal sediments

NASA Astrophysics Data System (ADS)

Bell, James B.; Reid, William D. K.; Pearce, David A.; Glover, Adrian G.; Sweeting, Christopher J.; Newton, Jason; Woulds, Clare

2017-12-01

Hydrothermal sediments are those in which hydrothermal fluid is discharged through sediments and are one of the least studied deep-sea ecosystems. We present a combination of microbial and biochemical data to assess trophodynamics between and within hydrothermal and background areas of the Bransfield Strait (1050-1647 m of depth). Microbial composition, biomass, and fatty acid signatures varied widely between and within hydrothermally active and background sites, providing evidence of diverse metabolic activity. Several species had different feeding strategies and trophic positions between hydrothermally active and inactive areas, and the stable isotope values of consumers were not consistent with feeding morphology. Niche area and the diversity of microbial fatty acids was lowest at the most hydrothermally active site, reflecting trends in species diversity. Faunal uptake of chemosynthetically produced organics was relatively limited but was detected at both hydrothermal and non-hydrothermal sites, potentially suggesting that hydrothermal activity can affect trophodynamics over a much wider area than previously thought.

PANDORA, a large volume low-energy neutron detector with real-time neutron-gamma discrimination

NASA Astrophysics Data System (ADS)

Stuhl, L.; Sasano, M.; Yako, K.; Yasuda, J.; Baba, H.; Ota, S.; Uesaka, T.

2017-09-01

The PANDORA (Particle Analyzer Neutron Detector Of Real-time Acquisition) system, which was developed for use in inverse kinematics experiments with unstable isotope beams, is a neutron detector based on a plastic scintillator coupled to a digital readout. PANDORA can be used for any reaction study involving the emission of low energy neutrons (100 keV-10 MeV) where background suppression and an increased signal-to-noise ratio are crucial. The digital readout system provides an opportunity for pulse shape discrimination (PSD) of the detected particles as well as intelligent triggering based on PSD. The figure of merit results of PANDORA are compared to the data in literature. Using PANDORA, 91 ± 1% of all detected neutrons can be separated, while 91 ± 1% of the detected gamma rays can be excluded, reducing the gamma ray background by one order of magnitude.

Carbon Isotopes of Methane in the Atlantic Realm: Links Between Background Station Data and Emission Source Regions

NASA Astrophysics Data System (ADS)

Lowry, D.; Fisher, R. E.; Lanoisellé, M.; Nisbet, E. G.

2011-12-01

Large networks of cavity ring-down spectroscopy (CRDS) instruments to measure mixing ratios of greenhouse gases are currently being developed in wealthier populated regions. However, many major natural source regions are remote from wealthy nations, and there are often great logistical obstacles to setting up and maintaining continuous monitoring of these sources. Thus flux assessments in many regions of the world rely on a few unequally spaced 'background' stations, plus satellite interpolation. This limited network can be supplemented to great effect by methane isotope data to identify emissions from different sources and their region of emission. Ideally both carbon and hydrogen isotope signatures are needed for maximum separation of source groups. However the more complex analytical procedure and larger sample requirements for D/H measurement mean that resources are currently better utilized for high-precision carbon isotope (δ13C) measurement of methane. In particular, NOAA maintains an invaluable isotopic measurement network. Since 2008 the greenhouse gas group at Royal Holloway and partners have been measuring methane in and around the Atlantic region, currently measuring mixing ratios by CRDS at Barra (Scotland), Ascension, and E. Falklands. In addition, regular flask sampling for δ13C of CH4 is underway at these sites, plus Cape Point, South Africa, and Ny-Alesund, Spitzbergen, supplemented by collection at Sable Island, Canada, and sampling campaigns on-board the British Antarctic Survey ship, RRS James Clark Ross, between 50°S and 80°N. Methane mixing ratio and δ13C, when combined with back trajectory analysis, help to identify sources over which the air masses have passed. While the South Atlantic shows little N-S variation in δ13C (predominantly -47.2 to -46.8%) it is punctuated by emission plumes from sources in South America and Africa, and although infrequently sampled, they can in some instances be compared with the isotopic characteristics from source studies and monthly emission maps from satellite products. North Atlantic sites have a seasonal cycle (up to 0.7 to 0.8%) that increases polewards, reaching -48% in Arctic summer. Emissions contributing to this seasonal cycle and inter-annual anomalies in the cycle are wetlands (-70 to -55%, but generally more 13C-depleted with increasing latitude) and biomass burning (-30 to -25%). Added to these, and mostly with isotopic signatures between those of the two main natural sources, are anthropogenic fossil fuel (gas, coal), landfill, ruminant and vehicle emissions. The δ13C of the source mix that dominated the North Atlantic from 8 to 53°N in late September 2010 was -56.5%. This is lower than expected if anthropogenic emissions were dominant (eg. London -52 to -49%), but corresponds to the period when maximum influence of high latitude wetland (around -68%) is expected. Methane in air leaving the Eastern seaboard of Canada (Sable Island) allows regional contributions to the Atlantic mix to be assessed. These samples indicate a δ13C source mix of -52 ±2% for air leaving the NE USA and -60 ±2% for air leaving Southern Canada during summer 2010. Further north a wetland emission signal (-70 to -66%) has predominated during recent summers.

Using Nitrogen and Oxygen Isotope Compositions of Nitrate to Distinguish Contaminant Sources in Hanford Soil and Groundwater

DOE Office of Scientific and Technical Information (OSTI.GOV)

Conrad, Mark; Bill, Markus

2008-08-01

The nitrogen ({delta}{sup 15}N) and oxygen ({delta}{sup 18}O) isotopic compositions of nitrate in the environment are primarily a function of the source of the nitrate. The ranges of isotopic compositions for nitrate resulting from common sources are outlined in Figure 1 from Kendall (1998). As noted on Figure 1, processes such as microbial metabolism can modify the isotopic compositions of the nitrate, but the effects of these processes are generally predictable. At Hanford, nitrate and other nitrogenous compounds were significant components of most of the chemical processes used at the site. Most of the oxygen in nitrate chemicals (e.g., nitricmore » acid) is derived from atmospheric oxygen, giving it a significantly higher {delta}{sup 18}O value (+23.5{per_thousand}) than naturally occurring nitrate that obtains most of its oxygen from water (the {delta}{sup 18}O of Hanford groundwater ranges from -14{per_thousand} to -18{per_thousand}). This makes it possible to differentiate nitrate from Hanford site activities from background nitrate at the site (including most fertilizers that might have been used prior to the Department of Energy plutonium production activities at the site). In addition, the extreme thermal and chemical conditions that occurred during some of the waste processing procedures and subsequent waste storage in select single-shell tanks resulted in unique nitrate isotopic compositions that can be used to identify those waste streams in soil and groundwater at the site (Singleton et al., 2005; Christensen et al., 2007). This report presents nitrate isotope data for soil and groundwater samples from the Hanford 200 Areas and discusses the implications of that data for potential sources of groundwater contamination.« less

Collectivity of light Ge and As isotopes

NASA Astrophysics Data System (ADS)

Corsi, A.; Delaroche, J.-P.; Obertelli, A.; Baugher, T.; Bazin, D.; Boissinot, S.; Flavigny, F.; Gade, A.; Girod, M.; Glasmacher, T.; Grinyer, G. F.; Korten, W.; Libert, J.; Ljungvall, J.; McDaniel, S.; Ratkiewicz, A.; Signoracci, A.; Stroberg, R.; Sulignano, B.; Weisshaar, D.

2013-10-01

Background: The self-conjugate nuclei of the A˜70 mass region display rapid shape evolution over isotopic or isotonic chains. Shape coexistence has been observed in Se and Kr isotopes reflecting the existence of deformed subshell gaps corresponding to different shell configurations. As and Ge isotopes are located halfway between such deformed nuclei and the Z=28 shell closure.Purpose: The present work aims at clarifying the low-lying spectroscopy of 66Ge and 67As, and providing a better insight into the evolution of collectivity in light even-even Ge and even-odd As isotopes.Methods: We investigate the low-lying levels and collectivity of the neutron deficient 67As and 66Ge through intermediate-energy Coulomb excitation, inelastic scattering, and proton knockout measurements. The experiment was performed using a cocktail beam of 68Se, 67As, and 66Ge nuclei at an energy of 70-80 MeV/nucleon. Spectroscopic properties of the low-lying states are compared to those calculated via shell model with the JUN45 interaction and beyond-mean-field calculations with the five-dimensional collective Hamiltonian method implemented using the Gogny D1S interaction. The structure evolution of the lower-mass Ge and As isotopes is discussed.Results: Reduced electric quadrupole transition probabilities B(E2) have been extracted from the Coulomb-excitation cross sections measured in 66Ge and 67As. The value obtained for the B(E2;01+→21+) in 66Ge is in agreement with a recent measurement, ruling out the existence of a minimum at N=34 in the B(E2) systematics as previously observed. New transitions have been found in 67As and were assigned to the decay of low-lying negative-parity states.

Study report on a double isotope method of calcium absorption

NASA Technical Reports Server (NTRS)

1978-01-01

Some of the pros and cons of three methods to study gastrointestinal calcium absorption are briefly discussed. The methods are: (1) a balance study; (2) a single isotope method; and (3) a double isotope method. A procedure for the double isotope method is also included.

Cosmogenically-produced isotopes in natural and enriched high-purity germanium detectors for the MAJORANA DEMONSTRATOR

NASA Astrophysics Data System (ADS)

Gilliss, Thomas; MAJORANA DEMONSTRATOR Collaboration

2017-01-01

The MAJORANA DEMONSTRATOR advances toward measurements of the neutrinoless double-beta decay of 76Ge. Detectors employed in the DEMONSTRATOR are subject to cosmogenic spallation during production and processing, resulting in activation of certain long-lived radioisotopes. Activation of these cosmogenic isotopes is mitigated by shielded storage of detectors and through underground operation of the DEMONSTRATOR at the 4850 ft level of the Sanford Underground Research Facility. In this work, we explore the appearance and reduction of cosmogenic contributions to the DEMONSTRATOR background spectrum. This work is supported by the U.S. Department of Energy, Office of Science, Office of Nuclear Physics, the Particle Astrophysics and Nuclear Physics Programs of the National Science Foundation, and the Sanford Underground Research Facility.

Separated isotopes: Vital tools for science and medicine

NASA Astrophysics Data System (ADS)

Deliberations and conclusions of a workshop on stable isotopes and derived radioisotopes organized by the Subcommittee on Nuclear and Radiochemistry of the National Research Council's Committee on Chemical Sciences at the request of the Department of Energy (DOE) are summarized. The workshop was jointly supported by the National Institutes of Health and DOE's Office of Basic Energy Sciences. An overview with three recommendations resulting from the workshop is followed by reports of the four workshop panels. Background papers were prepared by individuals on the Steering Committee and made available to all participants prior to the Workshop. They are reproduced as Appendixes 3 to 8. Short reports on alternate separation techniques were presented at the Workshop and are reproduced in Appendixes 9 to 11.

Sulfur biogeochemistry of cold seeps in the Green Canyon region of the Gulf of Mexico

NASA Astrophysics Data System (ADS)

Formolo, Michael J.; Lyons, Timothy W.

2013-10-01

Cold seeps in the Gulf of Mexico provide a natural laboratory to study biogeochemical cycling of sulfur, carbon, and oxygen at hydrate- and hydrocarbon-rich deep marine settings with obvious additional relevance to studies of diverse modern and ancient seeps. Of particular interest are the sulfur isotope signatures of microbial sulfate reduction coupled to anaerobic oxidation of methane and other non-methane liquid and gaseous hydrocarbons. Whereas most of the published sulfur isotope data from cold seep systems pertain to pore-water species, our study integrates both solid and dissolved sulfur: acid-volatile sulfides (SAVS), pyrite (Spy), elemental sulfur (S°), dissolved sulfate and ΣH2S. Modeled and 35SO42- reduction rates and δ13C and δ18O data for authigenic carbonates are integrated within this sulfur framework. Our results indicate extreme variability over narrow spatial and temporal scales within short distances (meters) from active seeps. High rates of microbial sulfate reduction can lead to complete consumption of the sulfate within the upper few centimeters of burial, while meters away the sulfate profile shows little depletion. Such small-scale variability must reflect the structure and temporal dynamics of hydrocarbon migration in the presence of low amounts of background organic matter. Our past work demonstrated that electron donors other than methane drive significant levels of microbial activity at these seeps, and very recent work has demonstrated that oxidation of higher chain volatile hydrocarbons can contribute to the high levels of microbial activity. These findings are consistent with our new results. Elevated concentrations of pyrite and diagenetic carbonate relative to background sediments are diagnostic of active seepage, yet the S isotopes tell more complex stories. Low levels of the transient, 'instantaneous' products of S cycling-AVS and S°-show high δ34S values that increase with depth. Most of the pyrite formation, however, seems to be very early as limited by the availability of reactive Fe phases. As such, δ34S values for pyrite at ancient seeps can show consistently low δ34S values that undersell the full intensity of microbial sulfate reduction. Low sedimentation rates, and the resulting low detrital iron fluxes, may in fact limit our ability to recognize seeps in the geologic record using only δ34S compositions for pyrite.

Delayed signatures of underground nuclear explosions

DOE PAGES

Carrigan, Charles R.; Sun, Yunwei; Hunter, Steven L.; ...

2016-03-16

Radionuclide signals from underground nuclear explosions (UNEs) are strongly influenced by the surrounding hydrogeologic regime. One effect of containment is delay of detonation-produced radioxenon reaching the surface as well as lengthening of its period of detectability compared to uncontained explosions. Using a field-scale tracer experiment, we evaluate important transport properties of a former UNE site. Here, we observe the character of signals at the surface due to the migration of gases from the post-detonation chimney under realistic transport conditions. Background radon signals are found to be highly responsive to cavity pressurization suggesting that large local radon anomalies may be anmore » indicator of a clandestine UNE. Computer simulations, using transport properties obtained from the experiment, track radioxenon isotopes in the chimney and their migration to the surface. They show that the chimney surrounded by a fractured containment regime behaves as a leaky chemical reactor regarding its effect on isotopic evolution introducing a dependence on nuclear yield not previously considered. This evolutionary model for radioxenon isotopes is validated by atmospheric observations of radioxenon from a 2013 UNE in the Democratic People’s Republic of Korea (DPRK). In conclusion, our model produces results similar to isotopic observations with nuclear yields being comparable to seismic estimates.« less

Calibration of Safecast dose rate measurements.

PubMed

Cervone, Guido; Hultquist, Carolynne

2018-10-01

A methodology is presented to calibrate contributed Safecast dose rate measurements acquired between 2011 and 2016 in the Fukushima prefecture of Japan. The Safecast data are calibrated using observations acquired by the U.S. Department of Energy at the time of the 2011 Fukushima Daiichi power plant nuclear accident. The methodology performs a series of interpolations between the U.S. government and contributed datasets at specific temporal windows and at corresponding spatial locations. The coefficients found for all the different temporal windows are aggregated and interpolated using quadratic regressions to generate a time dependent calibration function. Normal background radiation, decay rates, and missing values are taken into account during the analysis. Results show that the standard Safecast static transformation function overestimates the official measurements because it fails to capture the presence of two different Cesium isotopes and their changing magnitudes with time. A model is created to predict the ratio of the isotopes from the time of the accident through 2020. The proposed time dependent calibration takes into account this Cesium isotopes ratio, and it is shown to reduce the error between U.S. government and contributed data. The proposed calibration is needed through 2020, after which date the errors introduced by ignoring the presence of different isotopes will become negligible. Copyright © 2018 Elsevier Ltd. All rights reserved.

Monitoring Energy Calibration Drift Using the Scintillator Background Radiation

NASA Astrophysics Data System (ADS)

Conti, Maurizio; Eriksson, Lars; Hayden, Charles

2011-06-01

Scintillating materials commonly used in nuclear medicine can contain traces of isotopes that naturally emit gamma or beta radiation. Examples of these are 138La contained in LaBr3 and other Lanthanum based scintillators, and 176Lu contained in LSO, LYSO, LuYAP and other Lutetium based scintillators. In particular,176Lu decays into 176Hf and emits a beta particle with maximum energy 589 keV, and a cascade of gamma rays of energies 307 keV, 202 keV and 88 keV. We propose to use the background radiation for monitoring of detector calibration drift and for self-calibration of detectors in complex detector systems. A calibration drift due to random or systematic changes in photomultiplier tube (PMT) gain was studied in a Siemens PET scanner, based on LSO blocks. Both a conventional radioactive source (68Ge, 511 keV photons from electron-positron annihilation) and the LSO background radiation were used for calibration. The difference in the calibration peak shift at 511 keV estimated with the two methods was less than 10%.

Isotope Analysis Reveals Foraging Area Dichotomy for Atlantic Leatherback Turtles

PubMed Central

Angulo, Elena; Das, Krishna; Girondot, Marc

2008-01-01

Background The leatherback turtle (Dermochelys coriacea) has undergone a dramatic decline over the last 25 years, and this is believed to be primarily the result of mortality associated with fisheries bycatch followed by egg and nesting female harvest. Atlantic leatherback turtles undertake long migrations across ocean basins from subtropical and tropical nesting beaches to productive frontal areas. Migration between two nesting seasons can last 2 or 3 years, a time period termed the remigration interval (RI). Recent satellite transmitter data revealed that Atlantic leatherbacks follow two major dispersion patterns after nesting season, through the North Gulf Stream area or more eastward across the North Equatorial Current. However, information on the whole RI is lacking, precluding the accurate identification of feeding areas where conservation measures may need to be applied. Methodology/Principal Findings Using stable isotopes as dietary tracers we determined the characteristics of feeding grounds of leatherback females nesting in French Guiana. During migration, 3-year RI females differed from 2-year RI females in their isotope values, implying differences in their choice of feeding habitats (offshore vs. more coastal) and foraging latitude (North Atlantic vs. West African coasts, respectively). Egg-yolk and blood isotope values are correlated in nesting females, indicating that egg analysis is a useful tool for assessing isotope values in these turtles, including adults when not available. Conclusions/Significance Our results complement previous data on turtle movements during the first year following the nesting season, integrating the diet consumed during the year before nesting. We suggest that the French Guiana leatherback population segregates into two distinct isotopic groupings, and highlight the urgent need to determine the feeding habitats of the turtle in the Atlantic in order to protect this species from incidental take by commercial fisheries. Our results also emphasize the use of eggs, a less-invasive sampling material than blood, to assess isotopic data and feeding habits for adult female leatherbacks. PMID:18365003

Application of stable isotope tools for evaluating natural and stimulated biodegradation of organic pollutants in field studies.

PubMed

Fischer, Anko; Manefield, Mike; Bombach, Petra

2016-10-01

Stable isotope tools are increasingly applied for in-depth evaluation of biodegradation of organic pollutants at contaminated field sites. They can be divided into three methods i) determination of changes in natural abundance of stable isotopes using compound-specific stable isotope analysis (CSIA), ii) detection of incorporation of stable-isotope label from a stable-isotope labelled target compound into degradation and/or mineralisation products and iii) determination of stable-isotope label incorporation into biomarkers using stable isotope probing (SIP). Stable isotope tools have been applied as key monitoring tools for multiple-line-of-evidence-approaches (MLEA) for sensitive evaluation of pollutant biodegradation. This review highlights the application of CSIA, SIP and MLEA including stable isotope tools for assessing natural and stimulated biodegradation of organic pollutants in field studies dealing with soil and groundwater contaminations. Copyright © 2016 Elsevier Ltd. All rights reserved.

Effects of must concentration techniques on wine isotopic parameters.

PubMed

Guyon, Francois; Douet, Christine; Colas, Sebastien; Salagoïty, Marie-Hélène; Medina, Bernard

2006-12-27

Despite the robustness of isotopic methods applied in the field of wine control, isotopic values can be slightly influenced by enological practices. For this reason, must concentration technique effects on wine isotopic parameters were studied. The two studied concentration techniques were reverse osmosis (RO) and high-vacuum evaporation (HVE). Samples (must and extracted water) have been collected in various French vineyards. Musts were microfermented at the laboratory, and isotope parameters were determined on the obtained wine. Deuterium and carbon-13 isotope ratios were studied on distilled ethanol by nuclear magnetic resonance (NMR) and isotope ratio mass spectrometry (IRMS), respectively. The oxygen-18 ratio was determined on extracted and wine water using IRMS apparatus. The study showed that the RO technique has a very low effect on isotopic parameters, indicating that this concentration technique does not create any isotopic fractionation, neither at sugar level nor at water level. The effect is notable for must submitted to HVE concentration: water evaporation leads to a modification of the oxygen-18 ratio of the must and, as a consequence, ethanol deuterium concentration is also modified.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Guinn, I.; Buuck, M.; Cuesta, C.

The MAJORANA Collaboration will seek neutrinoless double beta decay (0νββ) in {sup 76}Ge using isotopically enriched p-type point contact (PPC) high purity Germanium (HPGe) detectors. A tonne-scale array of HPGe detectors would require background levels below 1 count/ROI-tonne-year in the 4 keV region of interest (ROI) around the 2039 keV Q-value of the decay. In order to demonstrate the feasibility of such an experiment, the MAJORANA DEMONSTRATOR, a 40 kg HPGe detector array, is being constructed with a background goal of < 3 count/ROI-tonne-year, which is expected to scale down to < 1 count/ROI-tonne-year for a tonne-scale experiment. The signalmore » readout electronics, which must be placed in close proximity to the detectors, present a challenge toward reaching this background goal. This talk will discuss the materials and design used to construct signal readout electronics with low enough backgrounds for the MAJORANA DEMONSTRATOR.« less

Molybdenum Isotopic Composition of Iron Meteorites, Chondrites and Refractory Inclusions

NASA Technical Reports Server (NTRS)

Becker, H.; Walker, R. J.

2003-01-01

Recent Mo isotopic studies of meteorites reported evidence for differences in isotopic compositions for whole rocks of some primitive and differentiated meteorites relative to terrestrial materials. Enrichments of r- and p-process isotopes of up to 3-4 units (e unit = parts in 10(exp 4) over s-process dominated isotopes are the most prominent features. Certain types of presolar grains show large enrichments in s-process isotopes, however, it was concluded on grounds of mass balance that incomplete digestion of such grains cannot explain the enrichments of r- and p-process isotopes in whole rocks of primitive chondrites. If the reported variability in r- and p-process isotope enrichments reflects the true isotopic characteristics of the whole rocks, the implications are quite profound. It would suggest the presence of large scale Mo isotopic heterogeneity within the solar accretion disk with likely collateral effects for other elements. However, such effects were not found for Ru isotopes, nor for Zr isotopes. Another recent Mo isotopic study by multi collector ICP-MS could not confirm the reported deviations in Allende, Murchison or iron meteorites. Here, we present new results for the Mo isotopic composition of iron meteorites, chondrites and CAIs obtained by negative thermal ionization mass spectrometry (NTIMS). We discuss analytical aspects and the homogeneity of Mo isotopic compositions in solar system materials.

Ultra-Sensitive Elemental Analysis Using Plasmas 4.Application of Inductively Coupled Plasma Mass Spectrometry to the Study of Environmental Radioactivity

NASA Astrophysics Data System (ADS)

Yoshida, Satoshi

Applications of inductively coupled plasma mass spectrometry (ICP-MS) to the determination of long-lived radionuclides in environmental samples were summarized. In order to predict the long-term behavior of the radionuclides, related stable elements were also determined. Compared with radioactivity measurements, the ICP-MS method has advantages in terms of its simple analytical procedures, prompt measurement time, and capability of determining the isotope ratio such as240Pu/239Pu, which can not be separated by radiation. Concentration of U and Th in Japanese surface soils were determined in order to determine the background level of the natural radionuclides. The 235U/238U ratio was successfully used to detect the release of enriched U from reconversion facilities to the environment and to understand the source term. The 240Pu/239Pu ratios in environmental samples varied widely depending on the Pu sources. Applications of ICP-MS to the measurement of I and Tc isotopes were also described. The ratio between radiocesium and stable Cs is useful for judging the equilibrium of deposited radiocesium in a forest ecosystem.

Ages and Growth of the Continental Crust from Radiogenic Isotopes

NASA Astrophysics Data System (ADS)

Patchett, P. J.; Samson, S. D.

2003-12-01

The development and application of radiogenic isotopes to dating of geologic events, and to questions of growth, evolution, and recycling processes in the continental crust are mature areas of scientific inquiry. By this we understand that many of the approaches used to date rocks and constrain the evolution of the continents are well established, even routine, and that the scope of data available on age and evolution of continents is very large. This is not to say that new approaches have not been developed in recent years, or that new approaches and/or insights cannot be developed in the future. However, the science of continental crustal evolution is definitely a domain where many of the problems are well defined, the power of the techniques used to solve them are well known, and the limitations of field and laboratory databases, as well as the preserved geologic record, are understood.From the very early days of crustal evolution studies, it was innovations and improvements in laboratory techniques that drove the pace of discovery (e.g., Holmes, 1911; Nier, 1939). This remained true through all the increments in capability reviewed in this chapter, up to the present day. Thus, continental crustal evolution is an area of Earth science where a species of very laboratory-oriented investigator, the "radiogenic isotope geologist" or "geochronologist," has made major advances, even breakthroughs, in understanding. This is true in spite of the fact that many of the individuals of the species may have lacked field expertise, or even more than a primitive level of geologic background. Because design and building of instruments like radiation detectors or mass spectrometers requires a knowledge of physics, many of the early practitioners of rock dating were physicists, like Alfred Nier (cited above). Since the 1970s, essentially all mass spectrometers have been constructed by specialized commercial firms, and the level of physics expertise among isotope geologists has been lower. These firms, based mainly (but not exclusively) in and around Manchester, England, and Bremen, Germany, have spearheaded technical innovations in mass spectrometry. Isotope geology researchers are one group of consumers for this technology, along with chemists, nuclear-weapon laboratories and nuclear-power generating facilities. Today, the vast majority of isotope geology researchers are derived from geological backgrounds.This chapter will briefly review historical aspects of the development of radiogenic isotope geology as applied to continents. Some details, references and cross-references to other chapters in this volume will be provided for most major radiogenic isotopic methods, and for applications of these. However, this chapter will ultimately concentrate on two major approaches that dominate the research field today: (i) crustal tectonic and magmatic ages from U-Pb dating of accessory minerals like zircon; and (ii) crustal differentiation and growth from neodymium isotopic determinations on total rocks.The sheer amount of data available from continental areas, and the pace of data acquisition today, places any geographically constrained compilation in the impossible category for a chapter like this one. In this chapter, the state of the art in both geochronology and crustal origins will be illustrated by selected examples, not by global compilations or comprehensive discussions of each region that has been studied. Nevertheless, some remarks about the availability of data from different parts of the world need to be made. As with other areas of geology, biology, and botany, the parts of the world that have been longest settled by western civilization have the best data coverage for both ages of continental rocks, and their origins and evolution. Thus, Western Europe, Canada, the USA and Australia have generally somewhat thorough coverage. More limited data have become available from Eastern Europe, Greenland, Central and South America, Africa, Asia, and Antarctica. Some of these data have been produced by groups based in those regions, but much of the data published between 1970 and today have been driven by studies based in, and funded from, western countries. Availability of state-of-the-art results for ages of crust and its evolution are low in Antarctica and Greenland, where climate and ice cover limit work, and in South America, Africa, and parts of Asia, where studies have been sporadic, and are certainly limited in some cases by political instability. This general situation is now changing, however. Two parts of the world where results for ages of orogenic belts and for crustal evolution in general are accumulating more rapidly since about 1990 are China and Russia; this is connected with growth of modern isotope geology facilities in those countries. Understanding of global continent growth and evolution is limited in critical respects by the large regions of the world that are poorly dated. Therefore, gradual improvement of the state of knowledge of less accessible parts of the continents will bring significant benefits, even though the conceptual issues may be understood to a large extent.

The Antarctic ice core chronology (AICC2012): an optimized multi-parameter and multi-site dating approach for the last 120 thousand years

NASA Astrophysics Data System (ADS)

Veres, D.; Bazin, L.; Landais, A.; Toyé Mahamadou Kele, H.; Lemieux-Dudon, B.; Parrenin, F.; Martinerie, P.; Blayo, E.; Blunier, T.; Capron, E.; Chappellaz, J.; Rasmussen, S. O.; Severi, M.; Svensson, A.; Vinther, B.; Wolff, E. W.

2013-08-01

The deep polar ice cores provide reference records commonly employed in global correlation of past climate events. However, temporal divergences reaching up to several thousand years (ka) exist between ice cores over the last climatic cycle. In this context, we are hereby introducing the Antarctic Ice Core Chronology 2012 (AICC2012), a new and coherent timescale developed for four Antarctic ice cores, namely Vostok, EPICA Dome C (EDC), EPICA Dronning Maud Land (EDML) and Talos Dome (TALDICE), alongside the Greenlandic NGRIP record. The AICC2012 timescale has been constructed using the Bayesian tool Datice (Lemieux-Dudon et al., 2010) that combines glaciological inputs and data constraints, including a wide range of relative and absolute gas and ice stratigraphic markers. We focus here on the last 120 ka, whereas the companion paper by Bazin et al. (2013) focuses on the interval 120-800 ka. Compared to previous timescales, AICC2012 presents an improved timing for the last glacial inception, respecting the glaciological constraints of all analyzed records. Moreover, with the addition of numerous new stratigraphic markers and improved calculation of the lock-in depth (LID) based on δ15N data employed as the Datice background scenario, the AICC2012 presents a slightly improved timing for the bipolar sequence of events over Marine Isotope Stage 3 associated with the seesaw mechanism, with maximum differences of about 600 yr with respect to the previous Datice-derived chronology of Lemieux-Dudon et al. (2010), hereafter denoted LD2010. Our improved scenario confirms the regional differences for the millennial scale variability over the last glacial period: while the EDC isotopic record (events of triangular shape) displays peaks roughly at the same time as the NGRIP abrupt isotopic increases, the EDML isotopic record (events characterized by broader peaks or even extended periods of high isotope values) reached the isotopic maximum several centuries before. It is expected that the future contribution of both other long ice core records and other types of chronological constraints to the Datice tool will lead to further refinements in the ice core chronologies beyond the AICC2012 chronology. For the time being however, we recommend that AICC2012 be used as the preferred chronology for the Vostok, EDC, EDML and TALDICE ice core records, both over the last glacial cycle (this study), and beyond (following Bazin et al., 2013). The ages for NGRIP in AICC2012 are virtually identical to those of GICC05 for the last 60.2 ka, whereas the ages beyond are independent of those in GICC05modelext (as in the construction of AICC2012, the GICC05modelext was included only via the background scenarios and not as age markers). As such, where issues of phasing between Antarctic records included in AICC2012 and NGRIP are involved, the NGRIP ages in AICC2012 should therefore be taken to avoid introducing false offsets. However for issues involving only Greenland ice cores, there is not yet a strong basis to recommend superseding GICC05modelext as the recommended age scale for Greenland ice cores.

Simulation of HEAO 3 Background

DTIC Science & Technology

2007-01-01

i i o iipp i i o iinn VdE A NaEEf VdE A NaEEfprod ji ji j R where i is a stable isotope in volume V, ai is its fractional abundance, i the...National Nuclear Data Center (NNDC), Brookhaven National Laboratory, Brookhaven, NY. [10] W. Nelson et al., ”The EGS4 code system ”, SLAC-Report-265

Stable isotopic variation in tropical forest plants for applications in primatology.

PubMed

Blumenthal, Scott A; Rothman, Jessica M; Chritz, Kendra L; Cerling, Thure E

2016-10-01

Stable isotope analysis is a promising tool for investigating primate ecology although nuanced ecological applications remain challenging, in part due to the complex nature of isotopic variability in plant-animal systems. The aim of this study is to investigate sources of carbon and nitrogen isotopic variation at the base of primate food webs that reflect aspects of primate ecology. The majority of primates inhabit tropical forest ecosystems, which are dominated by C3 vegetation. We used stable isotope ratios in plants from Kibale National Park, Uganda, a well-studied closed-canopy tropical forest, to investigate sources of isotopic variation among C3 plants related to canopy stratification, leaf age, and plant part. Unpredictably, our results demonstrate that vertical stratification within the canopy does not explain carbon or nitrogen isotopic variation in leaves. Leaf age can be a significant source of isotopic variation, although the direction and magnitude of this difference is not consistent across tree species. Some plant parts are clearly differentiated in carbon and nitrogen isotopic composition, particularly leaves compared to non-photosynthetic parts such as reproductive parts and woody stem parts. Overall, variation in the isotopic composition of floral communities, plant species, and plant parts demonstrates that stable isotope studies must include analysis of local plant species and parts consumed by the primates under study from within the study area. Am. J. Primatol. 78:1041-1054, 2016. © 2015 Wiley Periodicals, Inc. © 2015 Wiley Periodicals, Inc.

The early bird gets the shrimp: Confronting assumptions of isotopic equilibrium and homogeneity in a wild bird population

USGS Publications Warehouse

Wunder, Michael B.; Jehl, Joseph R.; Stricker, Craig A.

2012-01-01

1. Because stable isotope distributions in organic material vary systematically across energy gradients that exist in ecosystems, community and population structures, and in individual physiological systems, isotope values in animal tissues have helped address a broad range of questions in animal ecology. It follows that every tissue sample provides an isotopic profile that can be used to study dietary or movement histories of individual animals. Interpretations of these profiles depend on the assumption that metabolic pools are isotopically well mixed and in equilibrium with dietary resources prior to tissue synthesis, and they extend to the population level by assuming isotope profiles are identically distributed for animals using the same proximal dietary resource. As these assumptions are never fully met, studying structure in the variance of tissue isotope values from wild populations is informative. 2. We studied variation in δ13C, δ15N, δ2H and δ18O data for feathers from a population of eared grebes (Podiceps nigricollis) that migrate to Great Salt Lake each fall to moult feathers. During this time, they cannot fly and feed almost exclusively on superabundant brine shrimp (Artemia franciscana). The ecological simplicity of this situation minimized the usual spatial and trophic complexities often present in natural studies of feather isotope values. 3. Ranges and variances of isotope values for the feathers were larger than those from previously published studies that report feather isotopic variance, but they were bimodally distributed in all isotope dimensions. Isotope values for proximal dietary resources and local surface water show that some of the feathers we assumed to have been grown locally must have been grown before birds reached isotopic equilibrium with local diet or immediately prior to arrival at Great Salt Lake. 4. Our study provides novel insights about resource use strategies in eared grebes during migration. More generally, it demonstrates the utility of studying variance structures and questioning assumptions implicit in the interpretation of stable isotope data from wild animals.

Uranium and Calcium Isotope Ratio Measurements using the Modified Total Evaporation Method in TIMS

NASA Astrophysics Data System (ADS)

Richter, S.; Kuehn, H.; Berglund, M.; Hennessy, C.

2010-12-01

A new version of the "modified total evaporation" (MTE) method for isotopic analysis by multi-collector thermal ionization mass spectrometry (TIMS), with high analytical performance and designed in a more user-friendly and routinely applicable way, is described in detail. It is mainly being used for nuclear safeguards measurements of U and Pu and nuclear metrology, but can readily be applied to other scientific tasks in geochemistry, e.g. for Sr, Nd and Ca, as well. The development of the MTE method was organized in collaboration of several "key nuclear mass spectrometry laboratories", namely the New Brunswick Laboratory (NBL), the Institute for Transuranium Elements (ITU), the Safeguards Analytical Laboratory (now Safeguards Analytical Services, SGAS) of the International Atomic Energy Agency (IAEA) and the Institute for Reference Materials and Measurements (IRMM), with IRMM taking the leading role. The manufacturer of the TRITON TIMS instrument, Thermo Fisher Scientific, integrated this method into the software of the instrument. The development has now reached its goal to become a user-friendly and routinely useable method for uranium isotope ratio measurements with high precision and accuracy. Due to the use of the “total evaporation” (TE) method the measurement of the "major" uranium isotope ratio 235U/238U is routinely being performed with a precision of 0.01% to 0.02%. The use of a (certified) reference material measured under comparable conditions is emphasized to achieve an accuracy at a level of 0.02% - depending on the stated uncertainty of the certified value of the reference material. In contrast to the total evaporation method (TE), in the MTE method the total evaporation sequence is interrupted on a regular basis to allow for correction for background from peak tailing, internal calibration of a secondary electron multiplier (SEM) detector versus the Faraday cups, and ion source re-focusing. Therefore, the most significant improvement using the MTE method is in the analytical performance achieved for the "minor" ratios 234U/238U and 236U/238U. The MTE method is now routinely used at all collaborating laboratories and possibly more in the future. Additional applications for the MTE method, e.g. to take advantage of the good external precision in combination with the possibilities of internal background and detector calibrations or mass jumps between different cup configurations, are presented as well. One interesting application concerns new absolute isotope ratio measurements for Ca with an unprecedented level of accuracy. This is important because up to now most reported Ca isotope data are only calculated as relative deviations from a standard like NIST-SRM 915. Using the MTE method measurements on new gravimetrically prepared Ca isotope mixtures were performed. A significantly improved level of accuracy at the level of about 0.02% for both the 42Ca/40Ca and 44Ca/40Ca ratios was obtained.

Shape of intrinsic alpha pulse height spectra in lanthanide halide scintillators

NASA Astrophysics Data System (ADS)

Wolszczak, W.; Dorenbos, P.

2017-06-01

Internal contamination with actinium-227 and its daughters is a serious drawback in low-background applications of lanthanide-based scintillators. In this work we showed the important role of nuclear γ de-excitations on the shape of the internal alpha spectrum measured in scintillators. We calculated with Bateman equations the activities of contamination isotopes and the time evolution of actinium-227 and its progenies. Next, we measured the intrinsic background spectra of LaBr3(Ce), LaBr3(Ce,Sr) and CeBr3 with a digital spectroscopy technique, and we analyzed them with a pulse shape discrimination method (PSD) and a time-amplitude analysis. Finally, we simulated the α background spectrum with Geant4 tool-kit, consequently taking into account complex α-γ-electron events, the α / β ratio dependence on the α energy, and the electron/γ nonproportionality. We found that α-γ mixed events have higher light yield than expected for alpha particles alone, which leads to overestimation of the α / β ratio when it is measured with internal 227Th and 223Ra isotopes. The time-amplitude analysis showed that the α peaks of 219Rn and 215Po in LaBr3(Ce) and LaBr3(Ce,Sr) are not symmetric. We compared the simulation results with the measured data and provided further evidence of the important role of mixed α-γ-electron events for understanding the shape of the internal α spectrum in scintillators.

Cosmogenic production of tritium in dark matter detectors

NASA Astrophysics Data System (ADS)

Amaré, J.; Castel, J.; Cebrián, S.; Coarasa, I.; Cuesta, C.; Dafni, T.; Galán, J.; García, E.; Garza, J. G.; Iguaz, F. J.; Irastorza, I. G.; Luzón, G.; Martínez, M.; Mirallas, H.; Oliván, M. A.; Ortigoza, Y.; Ortiz de Solórzano, A.; Puimedón, J.; Ruiz-Chóliz, E.; Sarsa, M. L.; Villar, J. A.; Villar, P.

2018-01-01

The direct detection of dark matter particles requires ultra-low background conditions at energies below a few tens of keV. Radioactive isotopes are produced via cosmogenic activation in detectors and other materials and those isotopes constitute a background source which has to be under control. In particular, tritium is specially relevant due to its decay properties (very low endpoint energy and long half-life) when induced in the detector medium, and because it can be generated in any material as a spallation product. Quantification of cosmogenic production of tritium is not straightforward, neither experimentally nor by calculations. In this work, a method for the calculation of production rates at sea level has been developed and applied to some of the materials typically used as targets in dark matter detectors (germanium, sodium iodide, argon and neon); it is based on a selected description of tritium production cross sections over the entire energy range of cosmic nucleons. Results have been compared to available data in the literature, either based on other calculations or from measurements. The obtained tritium production rates, ranging from a few tens to a few hundreds of nuclei per kg and per day at sea level, point to a significant contribution to the background in dark matter experiments, requiring the application of specific protocols for target material purification, material storing underground and limiting the time the detector is on surface during the building process in order to minimize the exposure to the most dangerous cosmic ray components.

GraXe, graphene and xenon for neutrinoless double beta decay searches

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gómez-Cadenas, J.J.; Martín-Albo, J.; Monrabal, F.

2012-02-01

We propose a new detector concept, GraXe (to be pronounced as grace), to search for neutrinoless double beta decay in {sup 136}XE. GraXe combines a popular detection medium in rare-event searches, liquid xenon, with a new, background-free material, graphene. In our baseline design of GraXe, a sphere made of graphene-coated titanium mesh and filled with liquid xenon (LXe) enriched in the {sup 136}XE isotope is immersed in a large volume of natural LXe instrumented with photodetectors. Liquid xenon is an excellent scintillator, reasonably transparent to its own light. Graphene is transparent over a large frequency range, and impermeable to themore » xenon. Event position could be deduced from the light pattern detected in the photosensors. External backgrounds would be shielded by the buffer of natural LXe, leaving the ultra-radiopure internal volume virtually free of background. Industrial graphene can be manufactured at a competitive cost to produce the sphere. Enriching xenon in the isotope {sup 136}XE is easy and relatively cheap, and there is already near one ton of enriched xenon available in the world (currently being used by the EXO, KamLAND-Zen and NEXT experiments). All the cryogenic know-how is readily available from the numerous experiments using liquid xenon. An experiment using the GraXe concept appears realistic and affordable in a short time scale, and its physics potential is enormous.« less

Atmospheric pCO2 Reconstructed across the Early Eocene Hyperthermals

NASA Astrophysics Data System (ADS)

Cui, Y.; Schubert, B.

2015-12-01

Negative carbon isotope excursions (CIEs) are commonly associated with extreme global warming. The Early Eocene is punctuated by five such CIEs, the Paleocene-Eocene thermal maximum (PETM, ca. 55.8 Ma), H1 (ca. 53.6 Ma), H2 (ca. 53.5 Ma), I1 (ca. 53.3 Ma), and I2 (ca. 53.2 Ma), each characterized by global warming. The negative CIEs are recognized in both marine and terrestrial substrates, but the terrestrial substrates exhibit a larger absolute magnitude CIE than the marine substrates. Here we reconcile the difference in CIE magnitude between the terrestrial and marine substrates for each of these events by accounting for the additional carbon isotope fractionation by C3 land plants in response to increased atmospheric pCO2. Our analysis yields background and peak pCO2 values for each of the events. Assuming a common mechanism for each event, we calculate that background pCO2 was not static across the Early Eocene, with the highest background pCO2 immediately prior to I2, the last of the five CIEs. Background pCO2 is dependent on the source used in our analysis with values ranging from 300 to 720 ppmv provided an injection of 13C-depleted carbon with δ13C value of -60‰ (e.g. biogenic methane). The peak pCO2 during each event scales according to the magnitude of CIE, and is therefore greatest during the PETM and smallest during H2. Both background and peak pCO2 are higher if we assume a mechanism of permafrost thawing (δ13C = -25‰). Our reconstruction of pCO2 across these events is consistent with trends in the δ18O value of deep-sea benthic foraminifera, suggesting a strong link between pCO2 and temperature during the Early Eocene.

Engineered in situ bioremediation of a petroleum hydrocarbon-contaminated aquifer: assessment of mineralization based on alkalinity, inorganic carbon and stable carbon isotope balances

NASA Astrophysics Data System (ADS)

Hunkeler, Daniel; Höhener, Patrick; Bernasconi, Stefano; Zeyer, Josef

1999-04-01

A concept is proposed to assess in situ petroleum hydrocarbon mineralization by combining data on oxidant consumption, production of reduced species, CH 4, alkalinity and dissolved inorganic carbon (DIC) with measurements of stable isotope ratios. The concept was applied to a diesel fuel contaminated aquifer in Menziken, Switzerland, which was treated by engineered in situ bioremediation. In the contaminated aquifer, added oxidants (O 2 and NO 3-) were consumed, elevated concentrations of Fe(II), Mn(II), CH 4, alkalinity and DIC were detected and the DIC was generally depleted in 13C compared to the background. The DIC production was larger than expected based on the consumption of dissolved oxidants and the production of reduced species. Stable carbon isotope balances revealed that the DIC production in the aquifer originated mainly from microbial petroleum hydrocarbon mineralization, and that geochemical reactions such as carbonate dissolution produced little DIC. This suggests that petroleum hydrocarbon mineralization can be underestimated if it is determined based on concentrations of dissolved oxidants and reduced species.

Stable isotopes in yellow-bellied marmot (Marmota flaviventris) fossils reveal environmental stability in the late Quaternary of the Colorado Rocky Mountains

NASA Astrophysics Data System (ADS)

Reynard, Linda M.; Meltzer, David J.; Emslie, Steven D.; Tuross, Noreen

2015-03-01

High elevation plant and animal communities are considered extremely sensitive to environmental change. We investigated an exceptional fossil record of yellow-bellied marmot (Marmota flaviventris) specimens that was recovered from Cement Creek Cave (elev. 2860 m) and ranged in age from radiocarbon background circa 49.8 cal ka BP to ~ 1 cal ka BP. We coupled isotopic and radiocarbon measurements (δ18O, δD, δ15N, δ13C, and 14C) of bone collagen from individually-AMS dated specimens of marmots to assess ecological responses by this species to environmental change over time in a high elevation basin in the Rocky Mountains of southwestern Colorado, USA. We find little change in all four isotope ratios over time, demonstrating considerable environmental stability during periods when the marmots were present. The stable ecology and the apparent persistence of the small mammal community in the cave fauna throughout the late Quaternary are in marked contrast to the changes that occurred in the large mammal community, including local extirpation and extinction, at the end of the Pleistocene.

Development of a detector in order to investigate (n,γ)-cross sections by ToF method with a very short flight path

NASA Astrophysics Data System (ADS)

Wolf, C.; Glorius, J.; Reifarth, R.; Weigand, M.

2018-01-01

The determination of neutron capture cross sections of some radioactive isotopes like 85Kr is very important to improve the knowledge about the s process. Based on its own radioactive decay these isotopes can only be used in small samples inside a TOF facility, which is why the neutron flux of these facilities has to be very high. Unfortunately the neutron flux of the FRANZ setup at Goethe University Frankfurt, which will offer the highest neutron flux in astrophysical energy regions (keV region) [1], is still to low to investigate isotopes like 85Kr. Therefore a new setup called NAUTILUS is under development, which will reduce the flight path from 80 cm to a few centimeter to enhance the angular coverage of the sample and therefore increase the neutron flux by a factor of nearly 100. This implies a higher intensity of the γ-flash energy inside the detector and the neutron induced background. Hence the geometry, the scintillator material and the moderator were optimized by GEANT3 simulations.

Isotope-ratio-monitoring gas chromatography-mass spectrometry: methods for isotopic calibration

NASA Technical Reports Server (NTRS)

Merritt, D. A.; Brand, W. A.; Hayes, J. M.

1994-01-01

In trial analyses of a series of n-alkanes, precise determinations of 13C contents were based on isotopic standards introduced by five different techniques and results were compared. Specifically, organic-compound standards were coinjected with the analytes and carried through chromatography and combustion with them; or CO2 was supplied from a conventional inlet and mixed with the analyte in the ion source, or CO2 was supplied from an auxiliary mixing volume and transmitted to the source without interruption of the analyte stream. Additionally, two techniques were investigated in which the analyte stream was diverted and CO2 standards were placed on a near-zero background. All methods provided accurate results. Where applicable, methods not involving interruption of the analyte stream provided the highest performance (sigma = 0.00006 at.% 13C or 0.06% for 250 pmol C as CO2 reaching the ion source), but great care was required. Techniques involving diversion of the analyte stream were immune to interference from coeluting sample components and still provided high precision (0.0001 < or = sigma < or = 0.0002 at.% or 0.1 < or = sigma < or = 0.2%).

Evaluating Volatility-controlled Isotope Fractionation During Planet Formation: Kinetics versus Equilibrium

NASA Astrophysics Data System (ADS)

Young, E. D.

2017-12-01

Recent advances in our ability to measure stable isotope ratios of light, rock-forming elements, including those for Zn, K, Fe, Si, and Mg, among others, has resulted in an emerging hypothesis that collisions among rocky planetesimals, planetary embryos, and/or proto-planets caused losses of moderately volatile elements (e.g., K) and "common" or moderately refractory elements (e.g., Mg and Si). The primary evidence is in the form of heavy isotope enrichments in rock-forming elements relative to the chondrite groups that are thought to be representative of planetary precursors. Equilibrium volatility-controlled isotope fractionation for planetesimal magma oceans might have occurred for bodies larger than 0.1% of an Earth mass (½ the mass of Pluto) as these bodies had sufficient gravity to overpower the escape velocities of hot gas at 2000K. Both Jean's escape and viscous drag hydrodynamic escape can obviate the escape velocity limit but will fractionate by mass, not by volatility. Equilibrium vapor/melt fractionation is qualitatively consistent with the greater disparity in 29Si/28Si between Earth and chondrites than in 25Mg/24Mg. However, losses of large masses of vapor are required to record the fractionation in the melts. We consider that if Earth was derived from E chondrite-like materials, the bulk composition of the Earth, assuming refractory Ca was retained, requires > 60% loss of Mg. This is a lot of vapor loss for a process relying on at least intermittent equilibrium, although it comports with the isotopic lever-rule requirements. Paradoxically, the alternative of evaporative loss of rock-forming elements requires less total mass loss. For example, the calculated Mg and Si isotopic compositions of residues resulting from evaporation of chondritic melts can fit the Mg and Si isotopic compositions of Earth, Mars, and angrites with varying background pressures and with total mass losses of near 5% or less. These mass losses are closer to, and even lower than, those suggested by Ca concentrations relative to CI chondrite. Equilibrium models achieve greater Si than Mg isotope fractionation by large mass losses while evaporation models produce this effect for small mass losses. Additional constraints involving other isotope systems as well as models for vapor loss can distinguish between the two scenarios.

The Isotopologue Record of Repeat Vital Effect Offenders: Tracking (Dis)equilibrium Effects in Sea Urchins and Nannofossil Using Clumped Isotopes

NASA Astrophysics Data System (ADS)

John, C. M.; Davies, A.; Drury, A. J.

2016-12-01

Vital effects vary between species and affect various isotopic systems in unequal proportion. The magnitude of the response of different isotopic systems might thus be key in understanding biologically-mediated disequilibrium, especially in groups that show a tendency to be "repeat offenders" with regards to vital effects. Here we present carbon, oxygen, and clumped isotope data from echinoderm calcite and nannofossil ooze, both of which exhibit strong vital effects in bulk isotopes. Our study is the first to investigate the clumped isotope (dis)equilibrium of echinoids. Results from two echinoids, three marine gastropods and a bivalve mollusk from modern beach deposits of Bali, Indonesia, highlight a significant offset in clumped isotopes of a regular echinoid test from expected values, interpreted as evidence of a similar "vital effect" as observed in surface corals. This is in contrast to the test of an irregular "sand dollar" echinoid, with clumped isotope values within error of expected sea surface temperature. Furthermore, data on the inter-skeletal variability in the clumped isotopic composition of two regular echinoid species shows that the spines of the echinoids are in equilibrium with seawater with respect to clumped isotopes, but the test is not. For the nannofossil material, no clumped isotope vital effects are observed, consistent with previously published studies but at odds with strong vital effects in carbon and oxygen isotopes, often correlated with cell-size. In addition, we reveal that the <63 micron fraction of deep-sea ooze could constitute useful material for clumped isotope studies. An intriguing result of our study is that vital effects are mostly absent in clumped isotopes, even in phylums known for important isotopic effects. It remains to be explained why some parts of the echinoids show clear vital effects, notably enrichment in clumped isotopes of urchin tests. Mechanisms that could explain this include pH effects during calcification. Rapid precipitation of calcite is however not considered as a likely mechanism as skeletal components with the largest growth rates show no clear clumped isotope vital effects.

Application of 129I/127I Ratios in Groundwater Studies Conducted at Los Alamos National Laboratory, New Mexico

NASA Astrophysics Data System (ADS)

Longmire, P.; Dale, M.; Granzow, K.; Yanicak, S. M.

2014-12-01

Los Alamos National Laboratory (LANL) is an operating nuclear site that has released treated effluents from three plutonium-processing facilities since the mid 1940s. The radioisotope 129I (T1/2 = 15.7 Myrs) derived from235U and 239Pu processing at LANL is locally detected in groundwater above background concentrations. This isotope provides a unique tracer for groundwater investigations conducted at LANL that helps to identify source releases linked to groundwater-flow paths in aquifers subject to binary and ternary mixing of natural- and industrial-derived waters containing chromate and other chemicals. Bromide, chlorate, chloride, nitrate, perchlorate, sulfate, and tritium were associated with multiple outfalls at LANL and, therefore, do not provide unique chemical signatures identifying a specific point of release or source. Natural and anthropogenic ratios of 129I/127I measured in groundwater samples collected at LANL were quantified using accelerator mass spectrometry at Purdue Rare Isotope Measurement Laboratory, Purdue University. Anthropogenic ratios of 129I/127I range from 1,531 X 10-15 to 10,323 X 10-15 within perched-intermediate groundwater present in volcanoclastic and basalt aquifers (210 - 216 m depth). Anthropogenic ratios of 129I/127I range from 359 X 10-15 to 4,350 X 10-15 within the regional aquifer (280 m depth) consisting of volcanoclastic sediments of variable hydraulic properties. Local background ratios of 129I/127I have a narrow range of 171 X 10-15 to 378 X 10-15 in the regional aquifer. Dissolved iodide measured in groundwater at LANL is stable dominantly as iodate. Background concentrations of dissolved iodate (0.1 to 33.2 nM) are less variable compared to anthropogenic iodate (8.0 to 246 nM) in groundwater at the site. Variability in concentrations of anthropogenic iodate is controlled by heterogeneous source releases of iodate over time and non-uniform mixing of groundwater in the different aquifers.

Cleaning and passivation of copper surfaces to remove surface radioactivity and prevent oxide formation

NASA Astrophysics Data System (ADS)

Hoppe, E. W.; Seifert, A.; Aalseth, C. E.; Bachelor, P. P.; Day, A. R.; Edwards, D. J.; Hossbach, T. W.; Litke, K. E.; McIntyre, J. I.; Miley, H. S.; Schulte, S. M.; Smart, J. E.; Warren, G. A.

2007-08-01

High-purity copper is an attractive material for constructing ultra-low-background radiation measurement devices. Many low-background experiments using high-purity copper have indicated surface contamination emerges as the dominant background. Radon daughters plate out on exposed surfaces, leaving a residual 210Pb background that is difficult to avoid. Dust is also a problem; even under cleanroom conditions, the amount of U and Th deposited on surfaces can represent the largest remaining background. To control these backgrounds, a copper cleaning chemistry has been developed. Designed to replace an effective, but overly aggressive concentrated nitric acid etch, this peroxide-based solution allows for a more controlled cleaning of surfaces. The acidified hydrogen peroxide solution will generally target the Cu +/Cu 2+ species which are the predominant surface participants, leaving the bulk of copper metal intact. This preserves the critical tolerances of parts and eliminates significant waste disposal issues. Accompanying passivation chemistry has also been developed that protects copper surfaces from oxidation. Using a high-activity polonium surface spike, the most difficult-to-remove daughter isotope of radon, the performance of these methods are quantified.

Characterization of 176Lu background in LSO-based PET scanners

NASA Astrophysics Data System (ADS)

Conti, Maurizio; Eriksson, Lars; Rothfuss, Harold; Sjoeholm, Therese; Townsend, David; Rosenqvist, Göran; Carlier, Thomas

2017-05-01

LSO and LYSO are today the most common scintillators used in positron emission tomography. Lutetium contains traces of 176Lu, a radioactive isotope that decays β - with a cascade of γ photons in coincidence. Therefore, Lutetium-based scintillators are characterized by a small natural radiation background. In this paper, we investigate and characterize the 176Lu radiation background via experiments performed on LSO-based PET scanners. LSO background was measured at different energy windows and different time coincidence windows, and by using shields to alter the original spectrum. The effect of radiation background in particularly count-starved applications, such as 90Y imaging, is analysed and discussed. Depending on the size of the PET scanner, between 500 and 1000 total random counts per second and between 3 and 5 total true coincidences per second were measured in standard coincidence mode. The LSO background counts in a Siemens mCT in the standard PET energy and time windows are in general negligible in terms of trues, and are comparable to that measured in a BGO scanner of similar size.

Considerations in the development of the utility of stable isotopes in science, medicine, and agriculture, and environmental studies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matwiyoff, N.A.

1976-01-01

The prospects for the broad scale development of the utility of stable isotopes in science, medicine, agriculture, and environmental studies are considered with emphasis on the current status of isotope production, synthesis of isotopically labelled compounds, and analytical techniques.

Fish fins as non-lethal surrogates for muscle tissues in freshwater food web studies using stable isotopes.

PubMed

Hette Tronquart, Nicolas; Mazeas, Laurent; Reuilly-Manenti, Liana; Zahm, Amandine; Belliard, Jérôme

2012-07-30

Dorsal white muscle is the standard tissue analysed in fish trophic studies using stable isotope analyses. However, sampling white muscle often implies the sacrifice of fish. Thus, we examined whether the non-lethal sampling of fin tissue can substitute muscle sampling in food web studies. Analysing muscle and fin δ(15)N and δ(13)C values of 466 European freshwater fish (14 species) with an elemental analyser coupled with an isotope ratio mass spectrometer, we compared the isotope values of the two tissues. Correlations between fin and muscle isotope ratios were examined for all fish together and specifically for 12 species. We further proposed four methods of assessing muscle from fin isotope ratios and estimated the errors made using these muscle surrogates. Despite significant differences between isotope values of the two tissues, fin and muscle isotopic signals are strongly correlated. Muscle values, estimated with raw fin isotope ratios (1st method), induce an error of ca. 1‰ for both isotopes. In comparison, specific (2nd method) or general (3rd method) correlations provide meaningful corrections of fin isotope ratios (errors <0.6‰). On the other hand, relationships, established for Australian tropical fish, only give poor muscle estimates (errors >0.8‰). There is little chance that a global model can be created. However, the 2nd and 3rd methods of estimating muscle values from fin isotope ratios should provide an acceptable level of error for the studies of European freshwater food web. We thus recommend that future studies use fin tissue as a non-lethal surrogate for muscle. Copyright © 2012 John Wiley & Sons, Ltd.

Oxygen and Carbon Isotope Variations in a Modern Rodent Community – Implications for Palaeoenvironmental Reconstructions

PubMed Central

Gehler, Alexander; Tütken, Thomas; Pack, Andreas

2012-01-01

Background The oxygen (δ18O) and carbon (δ13C) isotope compositions of bioapatite from skeletal remains of fossil mammals are well-established proxies for the reconstruction of palaeoenvironmental and palaeoclimatic conditions. Stable isotope studies of modern analogues are an important prerequisite for such reconstructions from fossil mammal remains. While numerous studies have investigated modern large- and medium-sized mammals, comparable studies are rare for small mammals. Due to their high abundance in terrestrial ecosystems, short life spans and small habitat size, small mammals are good recorders of local environments. Methodology/Findings The δ18O and δ13C values of teeth and bones of seven sympatric modern rodent species collected from owl pellets at a single locality were measured, and the inter-specific, intra-specific and intra-individual variations were evaluated. Minimum sample sizes to obtain reproducible population δ18O means within one standard deviation were determined. These parameters are comparable to existing data from large mammals. Additionally, the fractionation between coexisting carbonate (δ18OCO3) and phosphate (δ18OPO4) in rodent bioapatite was determined, and δ18O values were compared to existing calibration equations between the δ18O of rodent bioapatite and local surface water (δ18OLW). Specific calibration equations between δ18OPO4 and δ18OLW may be applicable on a taxonomic level higher than the species. However, a significant bias can occur when bone-based equations are applied to tooth-data and vice versa, which is due to differences in skeletal tissue formation times. δ13C values reflect the rodents’ diet and agree well with field observations of their nutritional behaviour. Conclusions/Significance Rodents have a high potential for the reconstruction of palaeoenvironmental conditions by means of bioapatite δ18O and δ13C analysis. No significant disadvantages compared to larger mammals were observed. However, for refined palaeoenvironmental reconstructions a better understanding of stable isotope signatures in modern analogous communities and potential biases due to seasonality effects, population dynamics and tissue formation rates is necessary. PMID:23226212

Vehicle NOx emission plume isotopic signatures: Spatial variability across the eastern United States

NASA Astrophysics Data System (ADS)

Miller, David J.; Wojtal, Paul K.; Clark, Sydney C.; Hastings, Meredith G.

2017-04-01

On-road vehicle nitrogen oxide (NOx) sources currently dominate the U.S. anthropogenic emission budgets, yet vehicle NOx emissions have uncertain contributions to oxidized nitrogen (N) deposition patterns. Isotopic signatures serve as a potentially valuable observational tool to trace source contributions to NOx chemistry and N deposition, yet in situ emission signatures are underconstrained. We characterize the spatiotemporal variability of vehicle NOx emission isotopic signatures (δ15N-NOx) representative of U.S. vehicle fleet-integrated emission plumes. A novel combination of on-road mobile and stationary urban measurements is performed using a field and laboratory-verified technique for actively capturing NOx in solution to quantify δ15N-NOx at hourly resolution. On-road δ15N-NOx upwind of Providence, RI, ranged from -7 to -3‰. Simultaneous urban background δ15N-NOx observations showed comparable range and variations with on-road measurements, suggesting that vehicles dominate NOx emissions in the Providence area. On-road spatial δ15N-NOx variations of -9 to -2‰ were observed under various driving conditions in six urban metropolitan areas and rural interstate highways during summer and autumn in the U.S. Northeast and Midwest. Although isotopic signatures were insensitive to on-road driving mode variations, statistically significant correlations were found between δ15N-NOx and NOx emission factor extremes associated with heavy diesel emitter contributions. Overall, these results constrain an isotopic signature of fleet-integrated roadway NOx emission plumes, which have important implications for distinguishing vehicle NOx from other sources and tracking emission contributions to NOx chemistry and N deposition.

Separated isotopes: vital tools for science and medicine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1982-01-01

Deliberations and conclusions of a Workshop on Stable Isotopes and Derived Radioisotopes organized by the Subcommittee on Nuclear and Radiochemistry of the National Research Council's Committee on Chemical Sciences at the request of the Department of Energy (DOE) are summarized. The workshop was jointly supported by the National Institutes of Health and DOE's Office of Basic Energy Sciences. An overview with three recommendations resulting from the Workshop is followed by reports of the four Workshop panels. Background papers were prepared by individuals on the Steering Committee and made available to all participants prior to the Workshop. They are reproduced asmore » Appendixes 3 to 8. Short reports on alternate separation techniques were presented at the Workshop and are reproduced in Appendixes 9 to 11.« less

Lifetime measurement of neutron-rich even-even molybdenum isotopes

NASA Astrophysics Data System (ADS)

Ralet, D.; Pietri, S.; Rodríguez, T.; Alaqeel, M.; Alexander, T.; Alkhomashi, N.; Ameil, F.; Arici, T.; Ataç, A.; Avigo, R.; Bäck, T.; Bazzacco, D.; Birkenbach, B.; Boutachkov, P.; Bruyneel, B.; Bruce, A. M.; Camera, F.; Cederwall, B.; Ceruti, S.; Clément, E.; Cortés, M. L.; Curien, D.; De Angelis, G.; Désesquelles, P.; Dewald, M.; Didierjean, F.; Domingo-Pardo, C.; Doncel, M.; Duchêne, G.; Eberth, J.; Gadea, A.; Gerl, J.; Ghazi Moradi, F.; Geissel, H.; Goigoux, T.; Goel, N.; Golubev, P.; González, V.; Górska, M.; Gottardo, A.; Gregor, E.; Guastalla, G.; Givechev, A.; Habermann, T.; Hackstein, M.; Harkness-Brennan, L.; Henning, G.; Hess, H.; Hüyük, T.; Jolie, J.; Judson, D. S.; Jungclaus, A.; Knoebel, R.; Kojouharov, I.; Korichi, A.; Korten, W.; Kurz, N.; Labiche, M.; Lalović, N.; Louchart-Henning, C.; Mengoni, D.; Merchán, E.; Million, B.; Morales, A. I.; Napoli, D.; Naqvi, F.; Nyberg, J.; Pietralla, N.; Podolyák, Zs.; Pullia, A.; Prochazka, A.; Quintana, B.; Rainovski, G.; Reese, M.; Recchia, F.; Reiter, P.; Rudolph, D.; Salsac, M. D.; Sanchis, E.; Sarmiento, L. G.; Schaffner, H.; Scheidenberger, C.; Sengele, L.; Singh, B. S. Nara; Singh, P. P.; Stahl, C.; Stezowski, O.; Thoele, P.; Valiente Dobon, J. J.; Weick, H.; Wendt, A.; Wieland, O.; Winfield, J. S.; Wollersheim, H. J.; Zielinska, M.; PreSPEC Collaboration

2017-03-01

Background: In the neutron-rich A ≈100 mass region, rapid shape changes as a function of nucleon number as well as coexistence of prolate, oblate, and triaxial shapes are predicted by various theoretical models. Lifetime measurements of excited levels in the molybdenum isotopes allow the determination of transitional quadrupole moments, which in turn provides structural information regarding the predicted shape change. Purpose: The present paper reports on the experimental setup, the method that allowed one to measure the lifetimes of excited states in even-even molybdenum isotopes from mass A =100 up to mass A =108 , and the results that were obtained. Method: The isotopes of interest were populated by secondary knock-out reaction of neutron-rich nuclei separated and identified by the GSI fragment separator at relativistic beam energies and detected by the sensitive PreSPEC-AGATA experimental setup. The latter included the Lund-York-Cologne calorimeter for identification, tracking, and velocity measurement of ejectiles, and AGATA, an array of position sensitive segmented HPGe detectors, used to determine the interaction positions of the γ ray enabling a precise Doppler correction. The lifetimes were determined with a relativistic version of the Doppler-shift-attenuation method using the systematic shift of the energy after Doppler correction of a γ -ray transition with a known energy. This relativistic Doppler-shift-attenuation method allowed the determination of mean lifetimes from 2 to 250 ps. Results: Even-even molybdenum isotopes from mass A =100 to A =108 were studied. The decays of the low-lying states in the ground-state band were observed. In particular, two mean lifetimes were measured for the first time: τ =29 .7-9.1+11.3 ps for the 4+ state of 108Mo and τ =3 .2-0.7+0.7 ps for the 6+ state of 102Mo. Conclusions: The reduced transition strengths B (E 2 ) , calculated from lifetimes measured in this experiment, compared to beyond-mean-field calculations, indicate a gradual shape transition in the chain of molybdenum isotopes when going from A =100 to A =108 with a maximum reached at N =64 . The transition probabilities decrease for 108Mo which may be related to its well-pronounced triaxial shape indicated by the calculations.

Geant4 Developments for the Radon Electric Dipole Moment Search at TRIUMF

NASA Astrophysics Data System (ADS)

Rand, E. T.; Bangay, J. C.; Bianco, L.; Dunlop, R.; Finlay, P.; Garrett, P. E.; Leach, K. G.; Phillips, A. A.; Sumithrarachchi, C. S.; Svensson, C. E.; Wong, J.

2011-09-01

An experiment is being developed at TRIUMF to search for a time-reversal violating electric dipole moment (EDM) in odd-A isotopes of Rn. Extensive simulations of the experiment are being performed with GEANT4 to study the backgrounds and sensitivity of the proposed measurement technique involving the detection of γ rays emitted following the β decay of polarized Rn nuclei. GEANT4 developments for the RnEDM experiment include both realistic modelling of the detector geometry and full tracking of the radioactive β, γ, internal conversion, and x-ray processes, including the γ-ray angular distributions essential for measuring an atomic EDM.

Use of Quantity Indicators for Forecasting of Biogeochemical Behavior Sr-90 and Cs-137 in the Conditions of the Combined Pollution of Soils

NASA Astrophysics Data System (ADS)

Lavrentyeva, G. V.; Geshel, I. V.

2012-04-01

From huge number of the radionuclides generated by anthropogenous activity the major value the group of biologically active radionuclides has. First of all, it Sr-90 and Cs-137 which play an important role in various radiological situations. In researches on studying of laws of behavior in environment Sr -90 and Cs-137 the basic attention was given to studying of influence of their chemical analogs Ca and K, instead of stable isotopes Sr and Cs. However, even low concentration of stable isotopes Sr and Cs in soil can influence on biogeochemical behavior of radionuclides. Objects of research: dernovo-podsolic soil, summer barley of grade, stable and radioactive isotopes Sr, Cs. Schemes of experiments provided entering of 8 doses stable Cs and Sr in the range from 0 to 500-750 mg/kg of air-dry weight of soil and 50 kBq of radionuclides on each frequency. Absorption of radionuclides by plants will be defined by two parametres of transport. The first - factor of transition (TF), which characterises level of regulation of process of carrying over of a radionuclide from soil in plants and depends on distribution of an element between the firm and liquid phase, distribution defined in the factor (Kd). The second parametre - factor of concentrating (CF) which characterises biological level of regulation of this process. The increase in quantity of stable Sr in soil leads to an active desorption Sr-90 in a soil solution on all frequency. Kd of Cs-137 on the general background of which decrease in values some increase in factor in the range of 120-225 mg of Cs/kg of soil is observed. Received Kd of radionuclides will well be co-ordinated with the revealed functional dependences between concentration Cs and Sr in soil and specific activity Cs-137 and Sr-90 in a soil solution. Comparison CF of two radionuclides shows that plants absorb Sr-90 from a soil solution actively, than Cs-137. Thus values CF of Sr-90 in the investigated interval of concentration of a stable isotope are in inverse relationship from the element maintenance in a soil solution in all investigated interval of the maintenance of the isotope carrier whereas change similar the indicator for Cs-137 has more difficult dependence. The revealed laws of change of CF studied radionuclides prove to be true the received dependences of accumulation Sr-90 and Cs-137 in barley from specific activity of radionuclides in a soil solution. Values of TF of Sr-90 are in direct dependence on level of the maintenance stable Sr, below similar indicators for Cs-137 in all interval of change of concentration of stable isotopes. It finds reflection in the analysis of functional dependences between concentration of radionuclides in plants and soil. The received values of studied factors completely reflect change of specific activity of radionuclides in a soil solution and their biological availability depending on concentration of their stable isotopes that confirms use possibility in the prognostic purposes of these indicators.

Cryogenic gamma detectors enable direct detection of 236U and minor actinides for non-destructive assay [Cryogenic gamma detectors enable direct detection of minor actinides for non-destructive assay

DOE Office of Scientific and Technical Information (OSTI.GOV)

Velazquez, Miguel; Dreyer, Jonathan; Drury, Owen B.

2015-09-05

Here, we demonstrate the utility of a superconducting transition edge sensor (TES) γ-ray detector with high energy resolution and low Compton background for non-destructive assay (NDA) of a uranium sample from reprocessed nuclear fuel. We show that TES γ-detectors can separate low energy actinide γ-emissions from the background and nearby lines, even from minor isotopes whose signals are often obscured in NDA with conventional Ge detectors. Superconducting γ detectors may therefore bridge the gap between high-accuracy destructive assay (DA) and easier to-use NDA.

Assessing ecosystem effects of reservoir operations using food web-energy transfer and water quality models

USGS Publications Warehouse

Saito, L.; Johnson, B.M.; Bartholow, J.; Hanna, R.B.

2001-01-01

We investigated the effects on the reservoir food web of a new temperature control device (TCD) on the dam at Shasta Lake, California. We followed a linked modeling approach that used a specialized reservoir water quality model to forecast operation-induced changes in phytoplankton production. A food web–energy transfer model was also applied to propagate predicted changes in phytoplankton up through the food web to the predators and sport fishes of interest. The food web–energy transfer model employed a 10% trophic transfer efficiency through a food web that was mapped using carbon and nitrogen stable isotope analysis. Stable isotope analysis provided an efficient and comprehensive means of estimating the structure of the reservoir's food web with minimal sampling and background data. We used an optimization procedure to estimate the diet proportions of all food web components simultaneously from their isotopic signatures. Some consumers were estimated to be much more sensitive than others to perturbations to phytoplankton supply. The linked modeling approach demonstrated that interdisciplinary efforts enhance the value of information obtained from studies of managed ecosystems. The approach exploited the strengths of engineering and ecological modeling methods to address concerns that neither of the models could have addressed alone: (a) the water quality model could not have addressed quantitatively the possible impacts to fish, and (b) the food web model could not have examined how phytoplankton availability might change due to reservoir operations.

Surface dust wipes are the best predictors of blood leads in young children with elevated blood lead levels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gulson, Brian, E-mail: brian.gulson@mq.edu.au; CSIRO Earth Science and Resource Engineering, North Ryde NSW 2113; Anderson, Phil

Background: As part of the only national survey of lead in Australian children, which was undertaken in 1996, lead isotopic and lead concentration measurements were obtained from children from 24 dwellings whose blood lead levels were ≥15 µg/dL in an attempt to determine the source(s) of their elevated blood lead. Comparisons were made with data for six children with lower blood lead levels (<10 µg/dL). Methods: Thermal ionisation and isotope dilution mass spectrometry were used to determine high precision lead isotopic ratios ({sup 208}Pb/{sup 206}Pb, {sup 207}Pb/{sup 206}Pb and {sup 206}Pb/{sup 204}Pb) and lead concentrations in blood, dust from floormore » wipes, soil, drinking water and paint (where available). Evaluation of associations between blood and the environmental samples was based on the analysis of individual cases, and Pearson correlations and multiple regression analyses based on the whole dataset. Results and discussion: The correlations showed an association for isotopic ratios in blood and wipes (r=0.52, 95% CI 0.19–0.74), blood and soil (r=0.33, 95% CI −0.05–0.62), and blood and paint (r=0.56, 95% CI 0.09–0.83). The regression analyses indicated that the only statistically significant relationship for blood isotopic ratios was with dust wipes (B=0.65, 95% CI 0.35–0.95); there were no significant associations for lead concentrations in blood and environmental samples. There is a strong isotopic correlation of soils and house dust (r=0.53, 95% CI 0.20–0.75) indicative of a common source(s) for lead in soil and house dust. In contrast, as with the regression analyses, no such association is present for bulk lead concentrations (r=−0.003, 95% CI −0.37–0.36), the most common approach employed in source investigations. In evaluation of the isotopic results on a case by case basis, the strongest associations were for dust wipes and blood. -- Highlights: • Children with elevated blood lead ≥15 µg/dL compared with a group with <10 µg/dL. • High precision lead isotopic ratios in blood, house dust wipes, soil, water, paint. • Associations for isotopic measures of blood and dust, blood and soil, blood and paint. • Regressions gave significance for isotopic measures of blood/dust and dust/soil.« less

Determination of the isotopic composition of evapotranspiration in a mature oil palm plantation in Jambi province, Indonesia.

NASA Astrophysics Data System (ADS)

Bonazza, Mattia; Meijide, Ana; Knohl, Alexander

2017-04-01

Evapotranspiration (ET) is defined as the sum of the water vapor fluxes from evaporation (E) and transpiration (T). The relative proportion between these two quantities depends on the species, on their age and on the structure of the stand and canopy. Evaporation represents the fraction of water that doesn't contribute to plants growth hence it often considered as "unused" water by the plants root system. For this reason, in a fast changing environment like Indonesia where, since almost 30 years, tropical rainforests are gradually converted into extensive oil palm plantation, it is important to quantify the amount of evaporated water to improve agricultural practices and water quality. As powerful tracers of the hydrological cycle, water stable isotopes represent an important tool to estimate the isotopic composition of the evapotranspiration flux and they can be used as a starting point for the determination of the T/ET ratio, which can be considered as a plant water uptake efficiency indicator. The isotopic composition (δDvand δ18Ov) and the mixing ratio (qv) of water vapor measured in a stand is the result of the isotopic mixing between two members; ecosystem evapotranspiration (δET) and background air (δa). With the implementation of laser-based isotopic analysers we are now able to improve the measurement frequency of δDvand δ18Ov that leads us to an improved estimation of δET. Here we present the results of a measurement campaign, performed with a Picarro L-2120i and conducted in a mature oil palm plantation in the province of Jambi, Indonesia. We measured the atmospheric water vapor mixing ratio and isotopic composition at 5 sampling heights (21 m, 16 m, 9 m, 3.5 and 0.3 m) along a flux tower throughout the oil palm canopy (average height 10 m). The range of the water vapor isotopic composition was between -19 and -11 and -134 and -82 ‰ for δ18Ov and δDvrespectively. A fairly open canopy structure resulted in small mixing ratio gradients along the vertical profile. We collected and analysed all rain event and estimated the variability of the water vapor isotopic composition. Micrometeorological measurements, provided by the tower's sensors, were used to calculate ET using the Bowen ratio energy balance. To determine the isotopic composition of the evapotranspiration flux we used and compared two different methods: Keeling plot and flux gradient approach.

Doubly labelled water assessment of energy expenditure: principle, practice, and promise.

PubMed

Westerterp, Klaas R

2017-07-01

The doubly labelled water method for the assessment of energy expenditure was first published in 1955, application in humans started in 1982, and it has become the gold standard for human energy requirement under daily living conditions. The method involves enriching the body water of a subject with heavy hydrogen ( 2 H) and heavy oxygen ( 18 O), and then determining the difference in washout kinetics between both isotopes, being a function of carbon dioxide production. In practice, subjects get a measured amount of doubly labelled water ( 2 H 2 18 O) to increase background enrichment of body water for 18 O of 2000 ppm with at least 180 ppm and background enrichment of body water for 2 H of 150 ppm with 120 ppm. Subsequently, the difference between the apparent turnover rates of the hydrogen and oxygen of body water is assessed from blood-, saliva-, or urine samples, collected at the start and end of the observation interval of 1-3 weeks. Samples are analyzed for 18 O and 2 H with isotope ratio mass spectrometry. The doubly labelled water method is the indicated method to measure energy expenditure in any environment, especially with regard to activity energy expenditure, without interference with the behavior of the subjects. Applications include the assessment of energy requirement from total energy expenditure, validation of dietary assessment methods and validation of physical activity assessment methods with doubly labelled water measured energy expenditure as reference, and studies on body mass regulation with energy expenditure as a determinant of energy balance.

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

PubMed Central

2017-01-01

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. PMID:28405367

A hydrogen gas-water equilibration method produces accurate and precise stable hydrogen isotope ratio measurements in nutrition studies

USDA-ARS?s Scientific Manuscript database

Stable hydrogen isotope methodology is used in nutrition studies to measure growth, breast milk intake, and energy requirement. Isotope ratio MS is the best instrumentation to measure the stable hydrogen isotope ratios in physiological fluids. Conventional methods to convert physiological fluids to ...

Pollution and Climate Effects on Tree-Ring Nitrogen Isotopes

NASA Astrophysics Data System (ADS)

Savard, M. M.; Bégin, C.; Marion, J.; Smirnoff, A.

2009-04-01

BACKGROUND Monitoring of nitrous oxide concentration only started during the last 30 years in North America, but anthropogenic atmospheric nitrogen has been significantly emitted over the last 150 years. Can geochemical characteristics of tree rings be used to infer past changes in the nitrogen cycle of temperate regions? To address this question we use nitrogen stable isotopes in 125 years-long ring series from beech specimens (Fagus grandifolia) of the Georgian Bay Islands National Park (eastern Ontario), and pine (Pinus strobus) and beech trees of the Arboretum Morgan near Montreal (western Quebec). To evaluate the reliability of the N stable isotopes in wood treated for removal of soluble materials, we tested both tree species from the Montreal area. The reproducibility from tree to tree was excellent for both pine and beech trees, the isotopic trends were strongly concordant, and they were not influenced by the heartwood-sapwood transition zone. The coherence of changes of the isotopic series observed for the two species suggests that their tree-ring N isotopic values can serve as environmental indicator. RESULTS AND INTERPRETATION In Montreal and Georgian Bay, the N isotopes show strong and similar parallel agreement (Gleichlaufigkeit test) with the climatic parameters. So in fact, the short-term isotopic fluctuations correlate directly with summer precipitation and inversely with summer and spring temperature. A long-term decreasing isotope trend in Montreal indicates progressive changes in soil chemistry after 1951. A pedochemical change is also inferred for the Georgian Bay site on the basis of a positive N isotopic trend initiated after 1971. At both sites, the long-term ^15N series correlate with a proxy for NOx emissions (Pearson correlation), and carbon-isotope ring series suggest that the same trees have been impacted by phytotoxic pollutants (Savard et al., 2009a). We propose that the contrasted long-term nitrogen-isotope changes of Montreal and Georgian Bay reflect deposition of NOx emissions from cars and coal-power plants, with higher proportions from coal burning in Georgian Bay (Savard et al., 2009b). This interpretation is conceivable because recent monitoring indicates that coal-power plant NOx emissions play an important role in the annual N budget in Ontario, but they are negligible on the Quebec side. CONCLUSION Interpretations of long tree-ring N isotopic series in terms of effects generated by airborne N-species have been previously advocated. Here we further propose that the contrasted isotopic trends obtained for wood samples from two regions reflect different regional anthropogenic N deposition combined with variations of climatic conditions. This research suggests that nitrogen tree-ring series may record both regional climatic conditions and anthropogenic perturbations of the N cycle. REFERENCES Savard, M.M., Bégin,C., Marion, J., Aznar, J.-C., Smirnoff, A., 2009a. Changes of Air Quality in an urban region as inferred from tree-ring width and stable isotopes. Chapter 9 in "Relating Atmospheric Source Apportionment to Vegetation Effects: Establishing Cause Effect Relationships" (A. Legge ed.). Elsevier, Amsterdam; doi: 10.1016/S1474-8177(08)00209x. Savard, M.M., Bégin, C., Smirnoff, A., Marion, J., Rioux-Paquette, E., 2009b. Tree-ring nitrogen isotopes reflect climatic effects and anthropogenic NOx emissions. Env. Sci. Tech (doi: 10.1021/es802437k).

Stable isotope trophic patterns in echinoderm megafauna in close proximity to and remote from Gulf of Mexico lower slope hydrocarbon seeps

NASA Astrophysics Data System (ADS)

Carney, Robert Spencer

2010-11-01

Hydrocarbon-seep communities in the Gulf of Mexico have a high biomass that is exploited as a food source to varying degrees by the photosynthesis-dependent fauna inhabiting the surrounding mud bottom. A decline concurrent with ocean depth in detritus influx to that background habitat results in a much lower background biomass. The biomass contrast between population-rich seeps and depauperate mud bottom leads to the prediction that seep utilization by the background fauna should be extensive at all depths and should increase with depth. Species depth zonation makes like-species comparisons over the full depth of the Gulf of Mexico impossible. Seeps and normal bottom above 1000 m have different fauna from those below 1000 m. Lower slope seeps are surrounded by a fauna rich in echinoderm species, especially asteroids, ophiuroids, and holothuroids. All three taxa have species that are abundant within seeps and are probably endemic to them. They also contain species found only in mud background or within mud and seeps backgrounds. Tissue analyses of δ13C and δ15N of echinoderms collected by ROV within seeps and trawling away from seeps indicate a pattern of utilization similar to that found in upper slope seeps exploited by different taxa. Seastar and ophiuroid species abundant in or endemic to seeps have tissue isotope values reflecting seep chemosynthetic input via a free-living microbial detritus or predation. A single seep-endemic deposit-feeding holothuroid showed distinct seep tissue values. Background deposit-feeding holothuroids collected within seeps showed either no or only minor incorporation of seep carbon, indicating either a lack of access to seep detritus or short feeding times within the seep. A predicted extensive utilization of seep productivity at the deeper seeps was not found. Seeps may be relatively closed systems that require special adaptations of species in order for them to enter, exploit, and survive. Alternately, the surrounding deep benthos may not be as food-poor as assumed from biomass measurements and flux estimates.

Radiocarbon-depleted CO2 evidence for fuel biodegradation at the Naval Air Station North Island (USA) fuel farm site.

PubMed

Boyd, Thomas J; Pound, Michael J; Lohr, Daniel; Coffin, Richard B

2013-05-01

Dissolved CO(2) radiocarbon and stable carbon isotope ratios were measured in groundwater from a fuel contaminated site at the North Island Naval Air Station in San Diego, CA (USA). A background groundwater sampling well and 16 wells in the underground fuel contamination zone were evaluated. For each sample, a two end-member isotopic mixing model was used to determine the fraction of CO(2) derived from fossil fuel. The CO(2) fraction from fossil sources ranged from 8 to 93% at the fuel contaminated site, while stable carbon isotope values ranged from -14 to +5‰VPDB. Wells associated with highest historical and contemporary fuel contamination showed the highest fraction of CO(2) derived from petroleum (fossil) sources. Stable carbon isotope ratios indicated sub-regions on-site with recycled CO(2) (δ(13)CO(2) as high as +5‰VPDB) - most likely resulting from methanogenesis. Ancillary measurements (pH and cations) were used to determine that no fossil CaCO(3), for instance limestone, biased the analytical conclusions. Radiocarbon analysis is verified as a viable and definitive technique for confirming fossil hydrocarbon conversion to CO(2) (complete oxidation) at hydrocarbon-contaminated groundwater sites. The technique should also be very useful for assessing the efficacy of engineered remediation efforts and by using CO(2) production rates, contaminant mass conversion over time and per unit volume.

Hydrogeochemical and Isotopic Indicators of Hydraulic Fracturing Flowback Fluids in Shallow Groundwater and Stream Water, derived from Dameigou Shale Gas Extraction in the Northern Qaidam Basin.

PubMed

Zheng, Zhaoxian; Zhang, Hongda; Chen, Zongyu; Li, Xufeng; Zhu, Pucheng; Cui, Xiaoshun

2017-06-06

Most of the shale gas production in northwest China is from continental shale. Identifying hydrogeochemical and isotopic indicators of toxic hydraulic fracturing flowback fluids (HFFF) has great significance in assessing the safety of drinking water from shallow groundwater and streamwater. Hydrogeochemical and isotopic data for HFFF from the Dameigou shale formations (Cl/Br ratio (1.81 × 10 -4 -6.52 × 10 -4 ), Ba/Sr (>0.2), δ 11 B (-10-1‰), and ε SW Sr (56-65, where ε SW Sr is the deviation of the 87 Sr/ 86 Sr ratio from that of seawater in parts per 10 4 )) were distinct from data for the background saline shallow groundwater and streamwater before fracturing. Mixing models indicated that inorganic elemental signatures (Br/Cl, Ba/Sr) and isotopic fingerprints (δ 11 B, ε SW Sr ) can be used to distinguish between HFFF and conventional oil-field brine in shallow groundwater and streamwater. These diagnostic indicators were applied to identify potential releases of HFFF into shallow groundwater and streamwater during fracturing, flowback and storage. The monitored time series data for shallow groundwater and streamwater exhibit no clear trends along mixing curves toward the HFFF end member, indicating that there is no detectable release occurring at present.

An Isotopic view of water and nitrogen transport through the ...

EPA Pesticide Factsheets

Background/Question/MethodsGroundwater nitrate contamination affects thousands of households in Oregon's southern Willamette Valley and many more across the Pacific Northwest. The southern Willamette Valley Groundwater Management Area (SWV GWMA) was established in 2004 due to nitrate levels in the groundwater exceeding the human health standard of 10 mg nitrate-N L-1. Much of the nitrogen inputs to the GWMA comes from agricultural nitrogen use, and thus efforts to reduce N inputs to groundwater are focused upon improving N management. However, the effectiveness of these improvements on groundwater quality is unclear because of the complexity of nutrient transport through the vadose zone and long groundwater residence times. Our objective was to focus on vadose zone transport and understand the dynamics and timing of N and water movement below the rooting zone in relation to N management and water inputs. Stable isotopes are a powerful tool for tracking water movement, and understanding nitrogen transformations within the vadose zone. In partnership with local farmers, and state agencies, we established lysimeters and groundwater wells in multiple agricultural fields in the GWMA, and have monitored nitrate, nitrate isotopes, and water isotopes weekly for multiple years Results/ConclusionsOur results indicate that vadose zone transport is highly complex, and the residence time of water collected in lysimeters was much longer than expected. While input precipitatio

Metal Chemical and Isotope Characterisation in the Upper Loire River Basin, France

NASA Astrophysics Data System (ADS)

Widory, D.; Nigris, R.; Morard, A.; Gassama, N.; Poirier, A.; Bourrain, X.

2016-12-01

The Water Framework Directive (WFD) elaborated by the European Commission regulates water resources in the EC based on five years management plans. A new management plan that started in 2016 imposes strict water quality criteria to its member states, including good status thresholds for metallic contaminants. The Loire River, the most important river in France, flows through areas with lithologies naturally containing high metal concentrations in the upper part of its basin. Understanding these metal fluxes into the river is thus a prerequisite to understand their potential impact on the quality of its water in regards to the criteria defined by the WFD. The Massif Central, a residue of the Hercynian chain, is composed of granitic and volcanic rocks. Both its upstream position in the Loire basin and its numerous metal mineralizations made this region a good candidate for characterizing the natural metal geochemical background of its surface waters. To fulfill this objective we focused on the Pb, Cd and Zn chemical and isotope characteristics of selected non-anthropized small watersheds. The investigated small watersheds were selected for supposedly draining a single lithology and undergoing (as far as possible) negligible to no anthropogenic pressure. Results showed that although the high metal potential of the upper part of the Loire River basin has been highly exploited by humans for centuries, metal concentrations during the hydrological cycle are still under the guidelines defined by the WFD. Isotope compositions/ratios are strongly related to the corresponding lithologies along the rivers and help precisely define the local geochemical background that can then be used to identify and quantify any anthropogenic inputs downstream.

Detection of counterfeit antiviral drug Heptodin and classification of counterfeits using isotope amount ratio measurements by multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) and isotope ratio mass spectrometry (IRMS).

PubMed

Santamaria-Fernandez, Rebeca; Hearn, Ruth; Wolff, Jean-Claude

2009-06-01

Isotope ratio mass spectrometry (IRMS) and multicollector inductively coupled plasma mass spectrometry (MC-ICP-MS) are highly important techniques that can provide forensic evidence that otherwise would not be available. MC-ICP-MS has proved to be a very powerful tool for measuring high precision and accuracy isotope amount ratios. In this work, the potential of combining isotope amount ratio measurements performed by MC-ICP-MS and IRMS for the detection of counterfeit pharmaceutical tablets has been investigated. An extensive study for the antiviral drug Heptodin has been performed for several isotopic ratios combining MC-ICP-MS and an elemental analyser EA-IRMS for stable isotope amount ratio measurements. The study has been carried out for 139 batches of the antiviral drug and analyses have been performed for C, S, N and Mg isotope ratios. Authenticity ranges have been obtained for each isotopic system and combined to generate a unique multi-isotopic pattern only present in the genuine tablets. Counterfeit tablets have then been identified as those tablets with an isotopic fingerprint outside the genuine isotopic range. The combination of those two techniques has therefore great potential for pharmaceutical counterfeit detection. A much greater power of discrimination is obtained when at least three isotopic systems are combined. The data from these studies could be presented as evidence in court and therefore methods need to be validated to support their credibility. It is also crucial to be able to produce uncertainty values associated to the isotope amount ratio measurements so that significant differences can be identified and the genuineness of a sample can be assessed.

Initial Results: An Ultra-Low-Background Germanium Crystal Array

DTIC Science & Technology

2010-09-01

data (focused on γ -γ coincidence signatures) (Smith et al., 2004) and the Multi- Isotope Coincidence Analysis code (MICA) (Warren et al., 2006). The...The follow-on “CASCADES” project aims to develop a multicoincidence data- analysis package and make robust fission-product demonstration measurements...sensitivity. This effort is focused on improving gamma analysis capabilities for nuclear detonation detection (NDD) applications, e.g., nuclear treaty

Background Perchlorate Source Identification Technical Guidance

DTIC Science & Technology

2013-12-01

Sciences Branch (Code 71752) of the Advanced Systems and Applied Sciences Division (Code 71700), Space and Naval Warfare Systems Center (SSC Pacific), San...Head Advanced Systems & Applied Sciences Division iii EXECUTIVE SUMMARY The objective of this document is to outline the approach, tools, and...Helium HMX Octahydro-1,3,5,7-Tetranitro-1,3,5,7- Tetrazocine IR Installation Restoration IRIS Integrated Risk Information System IR-MS Isotope-Ratio

Changes in vegetation and climate as reflected in tooth enamel isotopes of Quaternary mammalian faunas from Indonesia

NASA Astrophysics Data System (ADS)

Janssen, Renee; Joordens, Josephine; Koutamanis, Dafne; Puspaningrum, Mika; de Vos, John; den Ouden, Natasja; van der Lubbe, Jeroen; Reijmer, John; Hampe, Oliver; Davies, Gareth; Vonhof, Hubert

2017-04-01

Climate and sea level fluctuations play a dominant role in the Quaternary biodiversity dynamics of Indonesia, with glacial-interglacial cycles affecting hydroclimate, vegetation, and animal migrations. We analyzed the carbon (δ13C), oxygen (δ18O), and strontium (87Sr/86Sr) isotopes of bovid, cervid, and suid teeth from several Pleistocene and Holocene sites on Java and Sumatra, in order to refine reconstructions of the paleohabitats of these faunas, gain more insight into their climatic background, and constrain their chronology. Our carbon isotope data indicate that individual sites are strongly dominated by the presence of either C3-browsers or C4-grazers. Herbivores from the Padang Highlands (Sumatra) and Hoekgrot (Java) cave faunas were mainly C3-browsers, while the studied herbivores from Homo erectus-bearing sites Trinil and Sangiran (Java) utilized an almost exclusive C4 diet. The C4 signal of Trinil herbivores confirms that the Hauptknochenschicht (Trinil HK) was deposited during glacial conditions, allowing us to hypothesize that it can be dated to MIS 16, 14 or 12. We propose that the dominant vegetation signals in Indonesian fossil sites, as revealed by δ13C data, reflect a glacial-interglacial contrast. The scarcity of δ13C values typically indicating mixed C3/C4 feeding may indicate that the transition between glacial and interglacial precipitation regimes was relatively abrupt. The observed positive correlation between δ13C and δ18O values can be attributed to the glacial-interglacial contrast between precipitation δ18O values, caused by differences in monsoon intensity. The 87Sr/86Sr data show that the dominant C4 signal observed in the Sangiran and Trinil herbivore faunas corresponds with roaming in a variety of landscape settings, corroborating our hypothesis that the δ13C values are representative of the overall C3/C4vegetation balance in these areas. These results provide a framework that will allow interpretation of future isotope data from these and other fossil sites in this region, including the isotopic composition of Homo erectus fossils.

Cross-Calibration of Secondary Electron Multiplier in Noble Gas Analysis

NASA Astrophysics Data System (ADS)

Santato, Alessandro; Hamilton, Doug; Deerberg, Michael; Wijbrans, Jan; Kuiper, Klaudia; Bouman, Claudia

2015-04-01

The latest generation of multi-collector noble gas mass spectrometers has decisively improved the precision in isotopic ratio analysis [1, 2] and helped the scientific community to address new questions [3]. Measuring numerous isotopes simultaneously has two significant advantages: firstly, any fluctuations in signal intensity have no effect on the isotope ratio and secondly, the analysis time is reduced. This particular point becomes very important in static vacuum mass spectrometry where during the analysis, the signal intensity decays and at the same time the background increases. However, when multi-collector analysis is utilized, it is necessary to pay special attention to the cross calibration of the detectors. This is a key point in order to have accurate and reproducible isotopic ratios. In isotope ratio mass spectrometry, with regard to the type of detector (i.e. Faraday or Secondary Electron Multiplier, SEM), analytical technique (TIMS, MC-ICP-MS or IRMS) and isotope system of interest, several techniques are currently applied to cross-calibrate the detectors. Specifically, the gain of the Faraday cups is generally stable and only the associated amplifier must be calibrated. For example, on the Thermo Scientific instrument control systems, the 1011 and 1012 ohm amplifiers can easily be calibrated through a fully software controlled procedure by inputting a constant electric signal to each amplifier sequentially [4]. On the other hand, the yield of the SEMs can drift up to 0.2% / hour and other techniques such as peak hopping, standard-sample bracketing and multi-dynamic measurement must be used. Peak hopping allows the detectors to be calibrated by measuring an ion beam of constant intensity across the detectors whereas standard-sample bracketing corrects the drift of the detectors through the analysis of a reference standard of a known isotopic ratio. If at least one isotopic pair of the sample is known, multi-dynamic measurement can be used; in this case the known isotopic ratio is measured on different pairs of detectors and the true value of the isotopic ratio of interest can be determined by a specific equation. In noble gas analysis, due to the decay of the ion beam during the measurement as well as the special isotopic systematic of the gases themselves, the cross-calibration of the SEM using these techniques becomes more complex and other methods should be investigated. In this work we present a comparison between different approaches to cross-calibrate multiple SEM's in noble gas analysis in order to evaluate the most suitable and reliable method. References: [1] Mark et al. (2009) Geochem. Geophys. Geosyst. 10, 1-9. [2] Mark et al. (2011) Geochim. Cosmochim. 75, 7494-7501. [3] Phillips and Matchan (2013) Geochimica et Cosmochimica Acta 121, 229-239. [4] Koornneef et al. (2014) Journal of Analytical Atomic Spectrometry 28, 749-754.

QEMSCAN+LAICPMS: a new tool for petrochronology and sedimentary provenance analysis

NASA Astrophysics Data System (ADS)

Vermeesch, Pieter; Rittner, Martin; Omma, Jenny

2017-04-01

Only a relatively small number of rock-forming minerals contain sufficiently high concentrations of naturally occurring radioactive parent isotopes and sufficiently low background concentrations of the corresponding daughter isotopes to be suitable for geochronology. The first step in most geochronological studies is to extract these datable minerals from the host rock using a combination of magnetic and density separation techniques, a process that is tedious and time consuming. We here present a new method to avoid mineral separation by coupling a QEMSCAN electron microscope to an LA-ICP-MS instrument. Given a polished hand specimen, a petrographic thin section, or a grain mount, the QEMSCAN+LAICPMS method produces chemical and mineralogical maps from which the X-Y coordinates of the datable mineral are extracted. These coordinates are subsequently passed on to the laser ablation system for isotopic and, hence, geochronological analysis. QEMSCAN+LAICPMS can be applied to a wide range of problems in igneous, metamorphic and sedimentary geology, as is illustrated with three case studies. In the first case study, a 3 × 4 cm slab of polished granite from the L'Erée pluton in Guernsey is scanned for zircon. This yields 23 U-Pb ages resulting in a concordia age of 615 ± 2 Ma. The second case study re-investigates a paragneiss from an ultra-high pressure terrane in the Qaidam Basin (Qinghai, China) that was previously analysed by conventional petrography, electron microscopy and SIMS zircon U-Pb analysis. In this example, the QEMSCAN revealed 107 small (20 μm) metamorphic zircons that were analysed by LA-ICP-MS to constrain the 430 Ma age of peak metamorphism. The third and final case study investigates the mineralogy and geochronology of sedimentary rocks of the Ordovician Sarah Formation (Saudi Arabia). We analysed 44 outcrop samples and a further 35 subsurface samples, resulting in a dataset comprising 10,000 detrital zircon U-Pb ages and 79 heavy mineral compositions and petrographic analyses. Jointly considering this enormous dataset by 3-way multidimensional scaling paints a remarkably simple picture of sandstone compositions that are determined by a combination of provenance and diagenesis. In conclusion, the QEMSCAN+LAICPMS method represents an efficient and cost effective way to obtain chemical and isotopic compositions on the same sample, which improves both the quantity and quality of geological data.

Oxygen isotopes as a tracer of phosphate sources and cycling in aquatic systems (Invited)

NASA Astrophysics Data System (ADS)

Young, M. B.; Kendall, C.; Paytan, A.

2013-12-01

The oxygen isotopic composition of phosphate can provide valuable information about sources and processes affecting phosphorus as it moves through hydrologic systems. Applications of this technique in soil and water have become more common in recent years due to improvements in extraction methods and instrument capabilities, and studies in multiple aquatic environments have demonstrated that some phosphorus sources may have distinct isotopic compositions within a given system. Under normal environmental conditions, the oxygen-phosphorus bonds in dissolved inorganic phosphate (DIP) can only be broken by enzymatic activity. Biological cycling of DIP will bring the phosphate oxygen into a temperature-dependent equilibrium with the surrounding water, overprinting any existing isotopic source signals. However, studies conducted in a wide range of estuarine, freshwater, and groundwater systems have found that the phosphate oxygen is often out of biological equilibrium with the water, suggesting that it is common for at least a partial isotopic source signal to be retained in aquatic systems. Oxygen isotope analysis on various potential phosphate sources such as synthetic and organic fertilizers, animal waste, detergents, and septic/wastewater treatment plant effluents show that these sources span a wide range of isotopic compositions, and although there is considerable overlap between the source groups, sources may be isotopically distinct within a given study area. Recent soil studies have shown that isotopic analysis of phosphate oxygen is also useful for understanding microbial cycling across different phosphorus pools, and may provide insights into controls on phosphorus leaching. Combining stable isotope information from soil and water studies will greatly improve our understanding of complex phosphate cycling, and the increasing use of this isotopic technique across different environments will provide new information regarding anthropogenic phosphate inputs and controls on biological cycling within hydrologic systems.

Quantification of in Situ Biodegradation Rate Constants Using a Novel Combined Isotope Approach

NASA Astrophysics Data System (ADS)

Blum, P.; Sültenfuß, J.; Martus, P.

2014-12-01

Numerous studies have shown the enormous potential of the compound-specific isotope analysis (CSIA) for studying the biodegradation of organic compounds such as monoaromatic hydrocarbons (BTEX), polyaromatic hydrocarbons (PAH), chlorinated solvents and other organic contaminants and environmental transformation mechanisms in groundwater. In addition, two-dimensional isotope analysis such as carbon and hydrogen have been successfully studied indicating the potential to also investigate site-specific reaction mechanisms. The main objective of the current study however is to quantify real effective in situ biodegradation rate constants in a coal-tar contaminated aquifer by combining compound-specific isotope analysis (CSIA) and tracer-based (3H-3He) ground-water dating (TGD). Hence, groundwater samples are used to determine groundwater residence times, and carbon and hydrogen stable isotopes are analyzed for selected BTEX and PAH. The results of the hydrogen stable isotopes surprisingly indicate no isotope fractionation and therefore no biodegradation. In contrast, for stable carbon isotopes of selected BTEX such as o-xylene and toluene, isotope shifts are detected indicating active biodegradation under sulfate-reducing conditions. These and previous results of stable carbon isotopes show that only for o-xylene a clear evidence for biodegradation is possible for the studied site. Nevertheless, in combining these results with the groundwater residence times, which range between 1 year for the shallow wells (20 m below surface) and 41 years for the deeper wells (40 m below surface), it is feasible to effectively determine in situ biodegradation rate constants for o-xylene. Conversely, the outcome also evidently demonstrate the major limitations of the novel combined isotope approach for a successful implementation of monitored natural attenuation (MNA) at such field sites.

Isotopic insights into biological regulation of zinc in contaminated systems

USGS Publications Warehouse

Wanty, Richard B.; Balistrieri, Laurie S.; Wesner, Jeff S.; Walters, David; Schmidt, Travis S.; Podda, Francesca; De Giudici, G.; Stricker, Craig A.; Kraus, Johanna M.; Lattanzi, Pierfranco; Wolf, Ruth E.; Cidu, R.

2015-01-01

Aquatic organisms use a variety of biogeochemical reactions to regulate essential and non-essential trace metals. Many of these mechanisms can lead to isotopic fractionation, thus measurement of metal isotopes may yield insights into the processes by which organisms respond to metal exposure. We illustrate these concepts with two case studies, one involving an intra- and the other an extra-cellular mechanism of Zn sequestration. In the first study, the mayfly Neocloeon triangulifer was grown in the laboratory, and fed a diet of Zn-doped diatoms at Zn levels exceeding the requirements for normal mayfly life functions. The N. triangulifer larvae consumed the diatoms and retained their Zn isotopic signature. Upon metamorphosis, the subimago life stage lost Zn mass either in the exuvia or by excretion, and the Zn retained was isotopically enriched. Thus, Zn uptake is nonfractionating, but Zn regulation favors the lighter isotope. Thus the Zn remaining in the subimago was isotopically heavier. In the second study, Zn was adsorbed on the cell walls and exopolysaccharide secretions of cyanobacteria, which favored the heavier Zn isotope. Continued adsorption eventually resulted in nucleation and biomineralization of hydrozincite {Zn5(CO3)2(OH)6}. These case studies demonstrate the utility of Zn isotopes to provide insights into how aquatic insects respond to metal exposure.

Hydrological cycle during the early Eocene: What can we learn from leaf waxes?

NASA Astrophysics Data System (ADS)

Krishnan, S.; Pagani, M.; Huber, M.

2012-12-01

Understanding how rapid warming modified global precipitation patterns during periods of global warming is essential to forecasting the impact of future climate change. The early Eocene (~55-52 Ma) represents a period of peak warmth for the past 65 million years with global temperatures ~10 degrees C warmer than present. This period is also known for at least three, greenhouse gas-induced episodes of rapid global warming (hyperthermals: PETM; ~55 Ma, ETM-2; ~53.7 Ma and ETM-3; 52.8 Ma), often considered extreme analogues to modern climate change. Hyperthermals are also characterized by negative carbon isotope excursions (CIE), which reflect the input of isotopically light carbon responsible for observed temperature increases. A novel proxy used for hydrological reconstructions uses the hydrogen isotopic composition of compound-specific biomarkers preserved in the sedimentary record. For terrestrial leaf-wax lipids (e.g., n-alkanes), the hydrogen isotopic composition primarily reflects the isotopic composition of meteoric waters, which is dependent on distance of vapor transport, number of rainout events, precipitation amount, and evapotranspiration. Isotopic compositions of PETM n-alkanes (δDalkanes) recovered from the Arctic Ocean show a substantial deuterium (D)-enrichment at the onset of the CIE which was argued to potentially reflect reduced rainout in the mid-latitudes, resulting in increased precipitation in the Arctic (Pagani et al., 2006). D-depleted values of n-alkanes during peak warmth of the PETM suggest either modification of local precipitation or a global change in the fraction of rainout. In this study, we evaluate the veracity of previous conclusions by compiling existing δDalkanes records (including from Mar-2X, Venezuela; Tawanui, New Zealand; Wilkes Land, Antarctica; and the Lomonsov Ridge, Arctic) with new records from the Pacific and Atlantic oceans and marginal marine sections (including Cicogna, Italy; Giraffe Core, Canadian High Arctic). To determine the background state of the hydrological cycle in a warmer world, we measured early Eocene δDalkanes at these sites. This compilation was then compared against results from the isotope-coupled National Center for Atmospheric Research (NCAR) Community Climate System Model v3.0 (CCSM) global climate model, with Eocene boundary conditions and two different pCO2 levels (2240 and 4480 ppm). Preliminary analyses suggest that the model is able to simulate the equator-pole trends in precipitation δD. However, predicted values are offset from the n-alkane data by up to 40‰. To study changes in the hydrological cycle with rapid warming, we analyze n-alkane δD and δ13C values for the PETM and ETM-2. Leads and lags between the carbon and hydrogen isotopic records help constrain the timing and type of hydrological shifts with respect to carbon input. Preliminary results from the ETM-2 recovered from the Arctic indicate similar hydrological changes during both hyperthermals. A pre-event increase in δD values (of 60‰ during the PETM and 25‰ during ETM-2) is observed, followed by a decrease in δD (~10-15‰ for both the events) during the peak of the CIE. A significant pre-PETM D-enrichment at mid-latitudes is not evident, however, more negative δD values during the CIE is observed in some sites. The reasons for these isotopic shifts and their implication for the local and global water cycles will be discussed.

Modern applications for a total sulfur reduction distillation method - what’s old is new again

PubMed Central

2014-01-01

Background The use of a boiling mixture of hydriodic acid, hypophosphorous acid, and hydrochloric acid to reduce any variety of sulfur compounds has been in use in various applications since the first appearance of this method in the literature in the 1920’s. In the realm of sulfur geochemistry, this method remains a useful, but under-utilized technique. Presented here is a detailed description of the distillation set-up and procedure, as well as an overview of potential applications of this method for marine sulfur biogeochemistry/isotope studies. The presented applications include the sulfur isotope analysis of extremely low amounts of sulfate from saline water, the conversion of radiolabeled sulfate into sulfide, the extraction of refractory sulfur from marine sediments, and the use of this method to assess sulfur cycling in Aarhus Bay sediments. Results The STrongly Reducing hydrIodic/hypoPhosphorous/hydrochloric acid (STRIP) reagent is capable of rapidly reducing a wide range of sulfur compounds, including the most oxidized form, sulfate, to hydrogen sulfide. Conversion of as little as approximately 5 micromole sulfate is possible, with a sulfur isotope composition reproducibility of 0.3 permil. Conclusions Although developed many decades ago, this distillation method remains relevant for many modern applications. The STRIP distillation quickly and quantitatively converts sulfur compounds to hydrogen sulfide which can be readily collected in a silver nitrate trap for further use. An application of this method to a study of sulfur cycling in Aarhus Bay demonstrates that we account for all of the sulfur compounds in pore-water, effectively closing the mass balance of sulfur cycling. PMID:24808759

Source Identification of Zn Contamination around a Zn-smelting Facility in Korea

NASA Astrophysics Data System (ADS)

Lee, S.; Jeon, S. K.

2016-12-01

With massive production of Zn for various industrial purposes, Zn release into the environment becomes highly possible, some of which might require a proper countermeasure depending on the residual concentration in environmental media. In order to set up an effective countermeasure, identification of contaminant source should be essential for determining the target object to be managed, and delineating the extent of necessary remedial work. In this study, we focus on a Zn-smelting facility located in eastern Korea where Zn concentrations in surrounding soils have been reported to exceed the contamination criteria. An abandoned mine which had been explored for Zn ores was located adjacent to the facility, and background concentration of Zn in the area was naturally high. The objective of the present study is to identify the major source of Zn contamination in the area, and to estimate the relative contributions of multiple sources, if so. In order to achieve these goals, we analyzed and compared the stable isotope ratios of Pb in the soil samples collected at different distances from the facility and the Zn concentrates (ZnS, sphalerite) of raw material in the facility. The Pb isotope ratios were further investigated by performing sequential extraction for each sample and comparing the isotopes ratios observed in each fraction of soil. In addition, possible presence of ZnS in the samples, which could be an evidence of Zn contamination by the smelting facility, was estimated by X-ray diffraction (XRD) analysis and scanning electron microscopy equipped with energy dispersive X-ray spectrometry (SEM-EDS) after separating the soil sample into the fractions with different particle sizes

Dike intrusions into bituminous coal, Illinois Basin: H, C, N, O isotopic responses to rapid and brief heating

USGS Publications Warehouse

Schimmelmann, A.; Mastalerz, Maria; Gao, L.; Sauer, P.E.; Topalov, K.

2009-01-01

Unlike long-term heating in subsiding sedimentary basins, the near-instantaneous thermal maturation of sedimentary organic matter near magmatic intrusions is comparable to artificial thermal maturation in the laboratory in terms of short duration and limited extent. This study investigates chemical and H, C, N, O isotopic changes in high volatile bituminous coal near two Illinois dike contacts and compares observed patterns and trends with data from other published studies and from artificial maturation experiments. Our study pioneers in quantifying isotopically exchangeable hydrogen and measuring the D/H (i.e., 2H/1H) ratio of isotopically non-exchangeable organic hydrogen in kerogen near magmatic contacts. Thermal stress in coal caused a reduction of isotopically exchangeable hydrogen in kerogen from 5% to 6% in unaltered coal to 2-3% at contacts, mostly due to elimination of functional groups (e.g., {single bond}OH, {single bond}COOH, {single bond}NH2). In contrast to all previously published data on D/H in thermally matured organic matter, the more mature kerogen near the two dike contacts is D-depleted, which is attributed to (i) thermal elimination of D-enriched functional groups, and (ii) thermal drying of hydrologically isolated coal prior to the onset of cracking reactions, thereby precluding D-transfer from relatively D-enriched water into kerogen. Maxima in organic nitrogen concentration and in the atomic N/C ratio of kerogen at a distance of ???2.5 to ???3.5 m from the thicker dike indicate that reactive N-compounds had been pyrolytically liberated at high temperature closer to the contact, migrated through the coal seam, and recombined with coal kerogen in a zone of lower temperature. The same principle extends to organic carbon, because a strong ??13Ckerogen vs. ??15Nkerogen correlation across 5.5 m of coal adjacent to the thicker dike indicates that coal was functioning as a flow-through reactor along a dynamic thermal gradient facilitating back-reactions between mobile pyrolysis products from the hot zone as they encounter less hot kerogen. Vein and cell filling carbonate is most abundant in highest rank coals where carbonate ??13CVPDB and ??18OVSMOW values are consistent with thermal generation of 13C-depleted and 18O-enriched CO2 from decarboxylation and pyrolysis of organic matter. Lower background concentrations of 13C-enriched carbonate in thermally unaffected coal may be linked to 13C-enrichment in residual CO2 in the process of CO2 reduction via microbial methanogenesis. Our compilation and comparison of available organic H, C, N isotopic findings on magmatic intrusions result in re-assessments of majors factors influencing isotopic shifts in kerogen during magmatic heating. (i) Thermally induced shifts in organic ??D values of kerogen are primarily driven by the availability of water or steam. Hydrologic isolation (e.g., near Illinois dikes) results in organic D-depletion in kerogen, whereas more common hydrologic connectivity results in organic D-enrichment. (ii) Shifts in kerogen (or coal) ??13C and ??15N values are typically small and may follow sinusoidal patterns over short distances from magmatic contacts. Laterally limited sampling strategies may thus result in misleading and non-representative data. (iii) Fluid transport of chemically active, mobile carbon and nitrogen species and recombination reactions with kerogen result in isotopic changes in kerogen that are unrelated to the original, autochthonous part of kerogen. ?? 2009 Elsevier Ltd. All rights reserved.

IsoCor: correcting MS data in isotope labeling experiments.

PubMed

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

2012-05-01

Mass spectrometry (MS) is widely used for isotopic labeling studies of metabolism and other biological processes. Quantitative applications-e.g. metabolic flux analysis-require tools to correct the raw MS data for the contribution of all naturally abundant isotopes. IsoCor is a software that allows such correction to be applied to any chemical species. Hence it 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 new features-e.g. correction for the isotopic purity of the tracer-to improve the accuracy of quantitative isotopic studies, and implements an efficient algorithm to process large datasets. Its user-friendly interface makes isotope labeling experiments more accessible to a wider biological community. IsoCor is distributed under OpenSource license at http://metasys.insa-toulouse.fr/software/isocor/

Carbon Isotopic Measurements and Aerosol Optical Determinations during CARES: Indications of the Importance of Background Biogenic Aerosols

NASA Astrophysics Data System (ADS)

Gaffney, J. S.; Marley, N. A.; Begum, M.; Sturchio, N. C.; Guilderson, T. P.

2011-12-01

High volume size-fractionated aerosol samples were obtained in Cool, CA during the Carbonaceous Aerosol and Radiative Effects Study (CARES) in June of 2010. This site was chosen to study the regional impacts of carbonaceous aerosols originating from the Sacramento area. Samples were collected for 6 to 24 hour time periods on quartz fiber filters by using slotted impactors to allow for collection of sample size cuts above and below one micron. Both total carbon content and carbon isotopic composition, including 13C/12C and 14C, were determined on the samples. In addition, Ångstrom absorption exponents (AAEs) were determined for the region of 300-900 nm on the sub-micron size cut by using state of the art diffuse reflectance UV-visible spectroscopy with integrating sphere technology. The overall carbonaceous aerosol loadings were found to be quite low and relatively constant during the study, suggesting that most of the aerosols at the site were locally formed background aerosols. The 14C data is consistent with a substantial fraction (~80 %) being from modern carbon sources and 13C/12C results indicate that the carbon source was from C-3 plants. This is consistent with a significant fraction of the aerosols in the area arising from secondary formation from biogenic precursor emissions from trees, most likely mono- and sesquiterpenes. These results are compared to past results obtained in Mexico City and discussed in terms of the potential importance of biogenic emissions to UV absorbing aerosols as these are anticipated to increase with climate change. This work was supported by the Office of Science (BER), U.S. Department of Energy, Grant No. DE-FG02-07ER64328 and Grant No. DE-FG02-07-ER64329 as part of the Atmospheric Systems Research program.

Redefining the utility of the three-isotope method

NASA Astrophysics Data System (ADS)

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.

Isotope pattern deconvolution as rising tool for isotope tracer studies in environmental research

NASA Astrophysics Data System (ADS)

Irrgeher, Johanna; Zitek, Andreas; Prohaska, Thomas

2014-05-01

During the last decade stable isotope tracers have emerged as versatile tool in ecological research. Besides 'intrinsic' isotope tracers caused by the natural variation of isotopes, the intentional introduction of 'extrinsic' enriched stable isotope tracers into biological systems has gained significant interest. Hereby the induced change in the natural isotopic composition of an element allows amongst others for studying the fate and fluxes of metals, trace elements and species in organisms or provides an intrinsic marker or tag of particular biological samples. Due to the shoreless potential of this methodology, the number of publications dealing with applications of isotope (double) spikes as tracers to address research questions in 'real world systems' is constantly increasing. However, some isotope systems like the natural Sr isotopic system, although potentially very powerful for this type of application, are still rarely used, mainly because their adequate measurement/determination poses major analytical challenges; as e.g. Sr is available in significant amounts in natural samples. In addition, biological systems underlie complex processes such as metabolism, adsorption/desorption or oxidation/reduction. As a consequence, classic evaluation approaches such as the isotope dilution mass spectrometry equation are often not applicable because of the unknown amount of tracer finally present in the sample. Isotope pattern deconvolution (IPD), based on multiple linear regression, serves as simplified alternative data processing strategy to double spike isotope dilution calculations. The outstanding advantage of this mathematical tool lies in the possibility of deconvolving the isotope pattern in a spiked sample without knowing the quantities of enriched isotope tracer being incorporated into the natural sample matrix as well as the degree of impurities and species-interconversion (e.g. from sample preparation). Here, the potential of IPD for environmental tracer studies is critically discussed, where special emphasis is set on evaluating different data processing strategies on the example of enriched stable Sr isotopes.1 The analytical key parameters such as blank (Kr, Sr and Rb), variation of the natural Sr isotopic composition in the sample, mass bias, interferences (Rb) and total combined uncertainty are considered. A full metrological protocol for data processing using IPD is presented based on data gained during two transgenerational marking studies of fish, where the transfer of a Sr isotope double spike (84Sr and 86Sr) from female spawners of common carp (Cyprinus carpio L.) and brown trout (Salmo trutta f.f.)2 to the centre of the otoliths of their offspring was studied by (LA)-MC-ICP-MS. 1J. Irrgeher, A. Zitek, M. Cervicek and T. Prohaska, J. Anal. At. Spectrom., 2014, 29, 193-200. 2A. Zitek, J. Irrgeher, M. Kletzl, T. Weismann and T. Prohaska, Fish. Manage. Ecol., 2013, 20, 654-361.

Intraspecific carbon and nitrogen isotopic variability in foxtail millet (Setaria italica).

PubMed

Lightfoot, Emma; Przelomska, Natalia; Craven, Martha; O Connell, Tamsin C; He, Lu; Hunt, Harriet V; Jones, Martin K

2016-07-15

Isotopic palaeodietary studies generally focus on bone collagen from human and/or animal remains. While plant remains are rarely analysed, it is known that plant isotope values can vary as a result of numerous factors, including soil conditions, the environment and type of plant. The millets were important food crops in prehistoric Eurasia, yet little is known about the isotopic differences within millet species. Here we compare the stable isotope ratios within and between Setaria italica plants grown in a controlled environment chamber. Using homogenised samples, we compare carbon isotope ratios of leaves and grains, and nitrogen isotope ratios of grains, from 29 accessions of Setaria italica. We find significant isotopic variability within single leaves and panicles, and between leaves and panicles within the same plant, which must be considered when undertaking plant isotope studies. We find that the leaves and grains from the different accessions have a ca 2‰ range in δ(13) C values, while the nitrogen isotope values in the grains have a ca 6‰ range. We also find an average offset of 0.9‰ between leaves and grains in their δ(13) C values. The variation found is large enough to have archaeological implications and within- and between-plant isotope variability should be considered in isotope studies. The range in δ(15) N values is particularly significant as it is larger than the typical values quoted for a trophic level enrichment, and as such may lead to erroneous interpretations of the amount of animal protein in human or animal diets. It is therefore necessary to account for the variability in plant stable isotope values during palaeodietary reconstructions. Copyright © 2016 John Wiley & Sons, Ltd. Copyright © 2016 John Wiley & Sons, Ltd.

A novel methodology to investigate isotopic biosignatures

NASA Astrophysics Data System (ADS)

Horner, T. J.; Lee, R. B. Y.; Henderson, G. M.; Rickaby, R. E. M.

2012-04-01

An enduring goal of trace metal isotopic studies of Earth History is to find isotopic 'fingerprints' of life or of life's individual physiochemical processes. Generally, such signatures are sought by relating an isotopic effect observed in controlled laboratory conditions or a well-characterized environment to a more complex system or the geological record. However, such an approach is ultimately limited because life exerts numerous isotopic fractionations on any one element so it is hard to dissect the resultant net fractionation into its individual components. Further, different organisms, often with the same apparent cellular function, can express different isotopic fractionation factors. We have used a novel method to investigate the isotopic fractionation associated with a single physiological process-enzyme specific isotopic fractionation. We selected Cd isotopes since only one biological use of Cd is known, CdCA (a Cd/Zn carbonic anhydrase from the coastal diatom T. Weissflogii). Thus, our investigation can also inform the long standing mystery as to why this generally toxic element appears to have a nutrient-like dissolved isotopic and concentration profile in the oceans. We used the pET-15b plasmid to insert the CdCA gene into the E. coli genome. There is no known biochemical function for Cd in E. coli, making it an ideal vector for studying distinct physiological processes within a single organism. The uptake of Cd and associated isotopic fractionation was determined for both normal cells and those expressing CdCA. It was found that whole cells always exhibited a preference for the light isotopes of Cd, regardless of the expression of CdCA; adsorption of Cd to cell surfaces was not seen to cause isotopic fractionation. However, the cleaning procedure employed exerted a strong control on the observed isotopic composition of cells. Using existing protein purification techniques, we measured the Cd isotopic composition of different subcellular fractions of E. coli (e.g. membranes, cytosol, etc.), including the catalytic metal atoms within CdCA. These experiments allow isotopic exchange reactions to be observed in biological systems at an unparalleled resolution, demonstrating that isotopic fractionation can occur, in vivo, on length scales as small as a few Å. We will explore future applications of this technique using the marine geochemistry of Cd as a case study. This experimental approach has great promise for studying the individual isotopic biosignatures of other biochemical reactions, in particular those which may have been active during early Earth History.

Calcium isotope analysis by mass spectrometry.

PubMed

Boulyga, Sergei F

2010-01-01

The variations in the isotopic composition of calcium caused by fractionation in heterogeneous systems and by nuclear reactions can provide insight into numerous biological, geological, and cosmic processes, and therefore isotopic analysis finds a wide spectrum of applications in cosmo- and geochemistry, paleoclimatic, nutritional, and biomedical studies. The measurement of calcium isotopic abundances in natural samples has challenged the analysts for more than three decades. Practically all Ca isotopes suffer from significant isobaric interferences, whereas low-abundant isotopes can be particularly affected by neighboring major isotopes. The extent of natural variations of stable isotopes appears to be relatively limited, and highly precise techniques are required to resolve isotopic effects. Isotope fractionation during sample preparation and measurements and instrumental mass bias can significantly exceed small isotope abundance variations in samples, which have to be investigated. Not surprisingly, a TIMS procedure developed by Russell et al. (Russell et al., 1978. Geochim Cosmochim Acta 42: 1075-1090) for Ca isotope measurements was considered as revolutionary for isotopic measurements in general, and that approach is used nowadays (with small modifications) for practically all isotopic systems and with different mass spectrometric techniques. Nevertheless, despite several decades of calcium research and corresponding development of mass spectrometers, the available precision and accuracy is still not always sufficient to achieve the challenging goals. The present article discusses figures of merits of presently used analytical methods and instrumentation, and attempts to critically assess their limitations. In Sections 2 and 3, mass spectrometric methods applied to precise stable isotope analysis and to the determination of (41)Ca are described. Section 4 contains a short summary of selected applications, and includes tracer experiments and the potential use of biological isotope fractionation in medical studies, paleoclimatic and paleoceanographic, and other terrestrial as well as extraterrestrial investigations. 2009 Wiley Periodicals, Inc.

Precise ruthenium fission product isotopic analysis using dynamic reaction cell inductively coupled plasma mass spectrometry (DRC-ICP-MS)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brown, Christopher F.; Dresel, P. Evan; Geiszler, Keith N.

2006-05-09

99Tc is a subsurface contaminant of interest at numerous federal, industrial, and international facilities. However, as a mono-isotopic fission product, 99Tc lacks the ability to be used as a signature to differentiate between the different waste disposal pathways that could have contributed to subsurface contamination at these facilities. Ruthenium fission-product isotopes are attractive analogues for the characterization of 99Tc sources because of their direct similarity to technetium with regard to subsurface mobility, and their large fission yields and low natural background concentrations. We developed an inductively coupled plasma mass spectrometry (ICP-MS) method capable of measuring ruthenium isotopes in groundwater samplesmore » and extracts of vadose zone sediments. Samples were analyzed directly on a Perkin Elmer ELAN DRC II ICP-MS after a single pass through a 1-ml bed volume of Dowex AG 50W-X8 100-200 mesh cation exchange resin. Precise ruthenium isotopic ratio measurements were achieved using a low-flow Meinhard-type nebulizer and long sample acquisition times (150,000 ms). Relative standard deviations of triplicate replicates were maintained at less than 0.5% when the total ruthenium solution concentration was 0.1 ng/ml or higher. Further work was performed to minimize the impact caused by mass interferences using the dynamic reaction cell (DRC) with O2 as the reaction gas. The aqueous concentrations of 96Mo and 96Zr were reduced by more than 99.7% in the reaction cell prior to injection of the sample into the mass analyzer quadrupole. The DRC was used in combination with stable-mass correction to quantitatively analyze samples containing up to 2-orders of magnitude more zirconium and molybdenum than ruthenium. The analytical approach documented herein provides an efficient and cost-effective way to precisely measure ruthenium isotopes and quantitate total ruthenium (natural vs. fission-product) in aqueous matrixes.« less

The Antarctic ice core chronology (AICC2012): an optimized multi-parameter and multi-site dating approach for the last 120 thousand years

NASA Astrophysics Data System (ADS)

Veres, D.; Bazin, L.; Landais, A.; Toyé Mahamadou Kele, H.; Lemieux-Dudon, B.; Parrenin, F.; Martinerie, P.; Blayo, E.; Blunier, T.; Capron, E.; Chappellaz, J.; Rasmussen, S. O.; Severi, M.; Svensson, A.; Vinther, B.; Wolff, E. W.

2012-12-01

The deep polar ice cores provide reference records commonly employed in global correlation of past climate events. However, temporal divergences reaching up to several thousand years (ka) exist between ice cores over the last climatic cycle. In this context, we are hereby introducing the Antarctic Ice Core Chronology 2012 (AICC2012), a new and coherent timescale developed for four Antarctic ice cores, namely Vostok, EPICA Dome C (EDC), EPICA Dronning Maud Land (EDML) and Talos Dome (TALDICE), alongside the Greenlandic NGRIP record. The AICC2012 time scale has been constructed using the Bayesian tool Datice (Lemieux-Dudon et al., 2010) that combines glaciological inputs and data constraints, including a wide range of relative and absolute gas and ice stratigraphic markers. We focus here on the last 120 ka, whereas the companion paper by Bazin et al., (2012) focuses on the interval 120-800 ka. Compared to previous timescales, AICC2012 presents an improved timing for the last glacial inception respecting the glaciological constraints of all analyzed records. Moreover, with the addition of numerous new stratigraphic markers and improved calculation of the lock-in depth (LID) based on δ15N data employed as the Datice background scenario, the AICC2012 presents a new timing for the bipolar sequence of events over Marine Isotope Stage 3 associated with the see-saw mechanism, with maximum differences of about 500 yr with respect to the previous Datice-derived chronology of Lemieux-Dudon et al. (2010), hereafter denoted LD2010. Our improved scenario confirms the regional differences for the millennial scale variability over the last glacial period: while the EDC isotopic record (events of triangular shape) displays peaks roughly at the same time as the NGRIP abrupt isotopic increases, the EDML isotopic record (events characterized by broader peaks or even extended periods of high isotope values) reached the isotopic maximum several centuries before.

Long-Term Species, Sexual and Individual Variations in Foraging Strategies of Fur Seals Revealed by Stable Isotopes in Whiskers

PubMed Central

Kernaléguen, Laëtitia; Cazelles, Bernard; Arnould, John P. Y.; Richard, Pierre; Guinet, Christophe; Cherel, Yves

2012-01-01

Background Individual variations in the use of the species niche are an important component of diversity in trophic interactions. A challenge in testing consistency of individual foraging strategy is the repeated collection of information on the same individuals. Methodology/Principal Findings The foraging strategies of sympatric fur seals (Arctocephalus gazella and A. tropicalis) were examined using the stable isotope signature of serially sampled whiskers. Most whiskers exhibited synchronous δ13C and δ15N oscillations that correspond to the seal annual movements over the long term (up to 8 years). δ13C and δ15N values were spread over large ranges, with differences between species, sexes and individuals. The main segregating mechanism operates at the spatial scale. Most seals favored foraging in subantarctic waters (where the Crozet Islands are located) where they fed on myctophids. However, A. gazella dispersed in the Antarctic Zone and A. tropicalis more in the subtropics. Gender differences in annual time budget shape the seal movements. Males that do not perform any parental care exhibited large isotopic oscillations reflecting broad annual migrations, while isotopic values of females confined to a limited foraging range during lactation exhibited smaller changes. Limited inter-individual isotopic variations occurred in female seals and in male A. tropicalis. In contrast, male A. gazella showed large inter-individual variations, with some males migrating repeatedly to high-Antarctic waters where they fed on krill, thus meaning that individual specialization occurred over years. Conclusions/Significance Whisker isotopic signature yields unique long-term information on individual behaviour that integrates the spatial, trophic and temporal dimensions of the ecological niche. The method allows depicting the entire realized niche of the species, including some of its less well-known components such as age-, sex-, individual- and migration-related changes. It highlights intrapopulation heterogeneity in foraging strategies that could have important implications for likely demographic responses to environmental variability. PMID:22431988

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

PubMed

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 releases from a nuclear explosion. Published by Elsevier Ltd.

Comparison of gas chromatography/isotope ratio mass spectrometry and liquid chromatography/isotope ratio mass spectrometry for carbon stable-isotope analysis of carbohydrates.

PubMed

Moerdijk-Poortvliet, Tanja C W; Schierbeek, Henk; Houtekamer, Marco; van Engeland, Tom; Derrien, Delphine; Stal, Lucas J; Boschker, Henricus T S

2015-07-15

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 LC/IRMS is expected to be more accurate and precise, no direct comparison has been reported. GC/IRMS with the aldonitrile penta-acetate (ANPA) derivatisation method was compared with LC/IRMS without derivatisation. A large number of glucose standards and a variety of natural samples were analysed for five neutral carbohydrates at natural abundance as well as at (13)C-enriched levels. Gas chromatography/chemical ionisation mass spectrometry (GC/CIMS) was applied to check for incomplete derivatisation of the carbohydrate, which would impair the accuracy of the GC/IRMS method. The LC/IRMS technique provided excellent precision (±0.08‰ and ±3.1‰ at natural abundance and enrichment levels, respectively) for the glucose standards and this technique proved to be superior to GC/IRMS (±0.62‰ and ±19.8‰ at natural abundance and enrichment levels, respectively). For GC/IRMS measurements the derivatisation correction and the conversion of carbohydrates into CO2 had a considerable effect on the measured δ(13)C values. However, we did not find any significant differences in the accuracy of the two techniques over the full range of natural δ(13)C abundances and (13)C-labelled glucose. The difference in the performance of GC/IRMS and LC/IRMS diminished when the δ(13)C values were measured in natural samples, because the chromatographic performance and background correction became critical factors, particularly for LC/IRMS. The derivatisation of carbohydrates for the GC/IRMS method was complete. Although both LC/IRMS and GC/IRMS are reliable techniques for compound-specific stable carbon isotope analysis of carbohydrates (provided that derivatisation is complete and the calibration requirements are met), LC/IRMS is the technique of choice. The reasons for this are the improved precision, simpler sample preparation, and straightforward isotopic calibration. Copyright © 2015 John Wiley & Sons, Ltd.

Macrobiotic Communities of Vailulu'u Seamount, Samoan Archipelago

NASA Astrophysics Data System (ADS)

Young, C. M.; Lee, R. W.; Pile, A. J.; Hudson, I. R.; Brooke, S. D.; Ted, P.; Staudigel, H.; Hart, S.; Bailey, B. E.; Haucke, L.; Koppers, A.; Konter, J.; Templeton, A.; Tebo, B.

2005-12-01

Vailulu'u, the active seamount on the hotspot at the Eastern end of the Samoan volcanic chain, was the focus of two research cruises in April and June 2005 using the Pisces V submersible. Warm-water vents on the summit of a newly formed volcanic cone in the crater supported a low-diversity community dominated by thick microbial mats and the synaphobranchid eel Dysommina rugosa. Isotope and gut analyses indicated that the eels feed not on the mats but on planktonic crustaceans imported to the system from the overlying water column. The microbial mat exhibited isotopic signatures consistent with local chemosynthesis, but not methane-based chemosynthesis; A<

Modeling of water isotopes in polar regions and application to ice core studies

NASA Astrophysics Data System (ADS)

Jouzel, J.

2012-04-01

Willi Dansgaard spear-headed the use of the stable isotopes of water in climatology and palaeoclimatology especially as applied to deep ice cores for which measurements of the oxygen and hydrogen isotope ratios remain the key tools for reconstructing continuous palaeotemperature records. In the line of his pioneering work on "Stable isotopes in precipitation" published in Tellus in 1964, I will review how isotopic models, either Rayleigh type or based on the implementation of water isotopes in General Circulation Models, have developed and been used for applications in polar ice core studies. This will include a discussion of the conventional approach for interpreting water isotopes in ice cores and of additional information provided by measurements of the deuterium excess and more recently of the 17O-excess.

Zinc isotope ratio imaging of rat brain thin sections from stable isotope tracer studies by LA-MC-ICP-MS.

PubMed

Urgast, Dagmar S; Hill, Sarah; Kwun, In-Sook; Beattie, John H; Goenaga-Infante, Heidi; Feldmann, Jörg

2012-10-01

Zinc stable isotope tracers (⁶⁷Zn and ⁷⁰Zn) were injected into rats at two different time points to investigate the feasibility of using tracers to study zinc kinetics at the microscale within distinct tissue features. Laser ablation coupled to multi-collector ICP-MS was used to analyse average isotope ratios in liver thin sections and to generate bio-images showing zinc isotope ratio distribution in brain thin sections. Average isotope ratios of all samples from treated animals were found to be statistically different (P < 0.05) from samples from untreated control animals. Furthermore, differing isotope ratios in physiological features of the brain, namely hippocampus, amygdala, cortex and hypothalamus, were identified. This indicates that these regions differ in their zinc metabolism kinetics. While cortex and hypothalamus contain more tracer two days after injection than 14 days after injection, the opposite is true for hippocampus and amygdala. This study showed that stable isotope tracer experiments can be combined with laser ablation MC-ICP-MS to measure trace element kinetics in tissues at a microscale level.

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

NASA Technical Reports Server (NTRS)

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.

Liquid and gas chromatography coupled to isotope ratio mass spectrometry for the determination of 13C-valine isotopic ratios in complex biological samples.

PubMed

Godin, Jean-Philippe; Breuillé, Denis; Obled, Christiane; Papet, Isabelle; Schierbeek, Henk; Hopfgartner, Gérard; Fay, Laurent-Bernard

2008-10-01

On-line gas chromatography-combustion-isotope ratio mass spectrometry (GC-C-IRMS) is commonly used to measure isotopic ratios at natural abundance as well as for tracer studies in nutritional and medical research. However, high-precision (13)C isotopic enrichment can also be measured by liquid chromatography-isotope ratio mass spectrometry (LC-IRMS). Indeed, LC-IRMS can be used, as shown by the new method reported here, to obtain a baseline separation and to measure (13)C isotopic enrichment of underivatised amino acids (Asp, Thr-Ser, Glu, Pro, Gly, Ala, Cys and Val). In case of Val, at natural abundance, the SD(delta(13)C) reported with this method was found to be below 1 per thousand . Another key feature of the new LC-IRMS method reported in this paper is the comparison of the LC-IRMS approach with the conventional GC-C-IRMS determination. To perform this comparative study, isotopic enrichments were measured from underivatised Val and its N(O, S)-ethoxycarbonyl ethyl ester derivative. Between 0.0 and 1.0 molar percent excess (MPE) (delta(13)C= -12.3 to 150.8 per thousand), the calculated root-mean-square (rms) of SD was 0.38 and 0.46 per thousand and the calculated rms of accuracy was 0.023 and 0.005 MPE, respectively, for GC-C-IRMS and LC-IRMS. Both systems measured accurately low isotopic enrichments (0.002 atom percent excess (APE)) with an SD (APE) of 0.0004. To correlate the relative (delta(13)C) and absolute (atom%, APE and MPE) isotopic enrichment of Val measured by the GC-C-IRMS and LC-IRMS devices, mathematical equations showing the slope and intercept of the curves were established and validated with experimental data between 0.0 to 2.3 MPE. Finally, both GC-C-IRMS and LC-IRMS instruments were also used to assess isotopic enrichment of protein-bound (13)C-Val in tibial epiphysis in a tracer study performed in rats. Isotopic enrichments measured by LC-IRMS and GC-C-IRMS were not statistically different (p>0.05). The results of this work indicate that the LC-IRMS was successful for high-precision (13)C isotopic measurements in tracer studies giving (13)C isotopic enrichment similar to the GC-C-IRMS but without the step of GC derivatisation. Therefore, for clinical studies requiring high-precision isotopic measurement, the LC-IRMS is the method of choice to measure the isotopic ratio.

Improving Charging-Breeding Simulations with Space-Charge Effects

NASA Astrophysics Data System (ADS)

Bilek, Ryan; Kwiatkowski, Ania; Steinbrügge, René

2016-09-01

Rare-isotope-beam facilities use Highly Charged Ions (HCI) for accelerators accelerating heavy ions and to improve measurement precision and resolving power of certain experiments. An Electron Beam Ion Trap (EBIT) is able to create HCI through successive electron impact, charge breeding trapped ions into higher charge states. CBSIM was created to calculate successive charge breeding with an EBIT. It was augmented by transferring it into an object-oriented programming language, including additional elements, improving ion-ion collision factors, and exploring the overlap of the electron beam with the ions. The calculation is enhanced with the effects of residual background gas by computing the space charge due to charge breeding. The program assimilates background species, ionizes and charge breeds them alongside the element being studied, and allows them to interact with the desired species through charge exchange, giving fairer overview of realistic charge breeding. Calculations of charge breeding will be shown for realistic experimental conditions. We reexamined the implementation of ionization energies, cross sections, and ion-ion interactions when charge breeding.

Serum apolipoprotein A-1 quantification by LC–MS with a SILAC internal standard reveals reduced levels in smokers

PubMed Central

Wang, Qingqing; Zhang, Suhong; Guo, Lili; Busch, Christine M; Jian, Wenying; Weng, Naidong; Snyder, Nathaniel W; Rangiah, Kannan; Mesaros, Clementina; Blair, Ian A

2015-01-01

Background: Absolute quantification of protein biomarkers such as serum apolipoprotein A1 by both immunoassays and LC–MS can provide misleading results. Results: Recombinant ApoA-1 internal standard was prepared using stable isotope labeling by amino acids in cell culture with [13C615N2]-lysine and [13C915N1]-tyrosine in human cells. A stable isotope dilution LC–MS method for serum ApoA-1 was validated and levels analyzed for 50 nonsmokers and 50 smokers. Conclusion: The concentration of ApoA-1 in nonsmokers was 169.4 mg/dl with an 18.4% reduction to 138.2 mg/dl in smokers. The validated assay will have clinical utility for assessing effects of smoking cessation and therapeutic or dietary interventions in high-risk populations. PMID:26394123

Lead in ancient Rome's city waters.

PubMed

Delile, Hugo; Blichert-Toft, Janne; Goiran, Jean-Philippe; Keay, Simon; Albarède, Francis

2014-05-06

It is now universally accepted that utilization of lead for domestic purposes and water distribution presents a major health hazard. The ancient Roman world was unaware of these risks. How far the gigantic network of lead pipes used in ancient Rome compromised public health in the city is unknown. Lead isotopes in sediments from the harbor of Imperial Rome register the presence of a strong anthropogenic component during the beginning of the Common Era and the Early Middle Ages. They demonstrate that the lead pipes of the water distribution system increased Pb contents in drinking water of the capital city by up to two orders of magnitude over the natural background. The Pb isotope record shows that the discontinuities in the pollution of the Tiber by lead are intimately entwined with the major issues affecting Late Antique Rome and its water distribution system.

Mixing Ratios of CO, CO2, CH4, and Isotope Ratios of Associated 13C, 18O, and 2H in Air Samples from Niwot Ridge, Colorado\\, and Montana de Oro, California, USA (January 2004)

DOE Data Explorer

Tyler, Stanley C. [Department of Earth System Science, University of California, Irvine, CA (USA)

2004-01-01

Air samples from Niwot Ridge, Colorado (41°N, 105°W) and Montaña de Oro, CA (35°N, 121°W) have been collected at approximately semi-monthly to monthly intervals since the mid 1990s. Such time series can provide information about: (1) seasonal cycling of CO, CO2, and CH4 sources and sinks in background air, (2) trends in atmospheric concentrations of CO2 and CH4 and their stable carbon, oxygen, and hydrogen isotopes, (3) the distribution of the hydroxyl (OH) radical in the atmosphere, and (4) the role of the terrestrial biosphere as a source or sink of atmospheric CO2.

Determination of the origin of dissolved inorganic carbon in groundwater around a reclaimed landfill in Otwock using stable carbon isotopes.

PubMed

Porowska, Dorota

2015-05-01

Chemical and isotopic analyses of groundwater from piezometers located around a reclaimed landfill in Otwock (Poland) were performed in order to trace the origin of dissolved inorganic carbon (DIC) in the groundwater. Due to differences in the isotopic composition of carbon from different sources, an analysis of stable carbon isotopes in the groundwater, together with the Keeling plot approach and a two-component mixing model allow us to evaluate the relative contributions of carbon from these sources in the groundwater. In the natural (background) groundwater, DIC concentrations and the isotopic composition of DIC (δ(13)CDIC) comes from two sources: decomposition of organic matter and carbonate dissolution within the aquifer sediments, whereas in the leachate-contaminated groundwater, DIC concentrations and δ(13)CDIC values depend on the degradation of organic matter within the aquifer sediments and biodegradation of organic matter stored in the landfill. From the mixing model, about 4-54% of the DIC pool is derived from organic matter degradation and 96-46% from carbonate dissolution in natural conditions. In the leachate-contaminated groundwater, about 20-53% of the DIC is derived from organic matter degradation of natural origin and 80-47% from biodegradation of organic matter stored in the landfill. Partial pressure of CO2 (P CO2) was generally above the atmospheric, hence atmospheric CO2 as a source of carbon in DIC pool was negligible in the aquifer. P CO2 values in the aquifer in Otwock were always one to two orders of magnitude above the atmospheric P CO2, and thus CO2 escaped directly into the vadose zone. Copyright © 2015 Elsevier Ltd. All rights reserved.

Inside HOLMES experiment: 163Ho metallic target production for the micro-calorimeter absorber

NASA Astrophysics Data System (ADS)

Pizzigoni, G.; Alpert, B.; Balata, M.; Bennett, D.; Biasotti, M.; Boragno, C.; Brofferio, C.; De Gerone, M.; Dressler, R.; Faverazani, M.; Ferri, E.; Folwer, J.; Gatti, F.; Giachero, A.; Heinitz, S.; Hilton, G.; Köster, U.; Lusignoli, M.; Maino, M.; Mates, J.; Nisi, S.; Nizzolo, R.; Nucciotti, A.; Pessina, G.; Puiu, A.; Ragazzi, S.; Reintsema, C.; Ribeiro Gomes, M.; Shmidt, D.; Schumann, D.; Sisti, M.; Swetz, D.; Terranova, F.; Ullom, J.; Day, P. K.

2016-07-01

The main goal in the HOLMES experiment is the neutrino mass measurement using an array of 1000 micro-calorimeters with standard metallic absorber. A good isotope for such measurement is the 163Ho, those isotopes embedded in the metallic absorber will be 1011-1013. Since 163Ho is not available in nature, a dedicated process must be set up to produce the amount needed for this neutrino mass experiment. The process with the highest born-up cross-section is the neutron irradiation of Er2O3 enriched in 162Er: 162Er(n,γ)163Er →163Ho+νe, where the decay is an EC with half-life of about 75 min and the (n,γ) is about 20 barns for thermal neutron. After the neutron irradiation in the oxide powder there are several radioactive isotopes which are potentially disturbing because of the background that they cause below 5 keV. The chemical separation of holmium from the irradiation enriched Er2O3 powder is therefore mandatory and will be performed by means of ion exchange chromatography. On the end of those processes the oxide powder enriched in 162Er will have the 163Ho isotope number required. The holmium chemical state influences the end point of the EC spectrum, in order to avoid such effect it is necessary to embed in the absorber only the metallic isotope. Reduction and distillation technique allowed us to obtain a pure metallic holmium, starting from natural oxide holmium. This technique will be applied on the irradiated oxide powder to obtain the metallic 163Ho, ready to be embedded in the micro-calorimeter absorber.

Unravelling biocultural population structure in 4th/3rd century BC Monterenzio Vecchio (Bologna, Italy) through a comparative analysis of strontium isotopes, non-metric dental evidence, and funerary practices.

PubMed

Sorrentino, Rita; Bortolini, Eugenio; Lugli, Federico; Mancuso, Giuseppe; Buti, Laura; Oxilia, Gregorio; Vazzana, Antonino; Figus, Carla; Serrangeli, Maria Cristina; Margherita, Cristiana; Penzo, Annachiara; Gruppioni, Giorgio; Gottarelli, Antonio; Jochum, Klaus Peter; Belcastro, Maria Giovanna; Cipriani, Anna; Feeney, Robin N M; Benazzi, Stefano

2018-01-01

The 4th century BC marks the main entrance of Celtic populations in northern Italy. Their arrival has been suggested based on the presence of Celtic customs in Etruscan mortuary contexts, yet up to now few bioarchaeological data have been examined to support or reject the arrival of these newcomers. Here we use strontium isotopes, non-metric dental traits and funerary patterns to unravel the biocultural structure of the necropolis of Monterenzio Vecchio (Bologna, Italy). Subsamples of our total sample of 38 individuals were analyzed based on different criteria characterizing the following analyses: 1) strontium isotope analysis to investigate migratory patterns and provenance; 2) non-metric dental traits to establish biological relationships between Monterenzio Vecchio, 13 Italian Iron age necropolises and three continental and non-continental Celtic necropolises; 3) grave goods which were statistically explored to detect possible patterns of cultural variability. The strontium isotopes results indicate the presence of local and non-local individuals, with some revealing patterns of mobility. The dental morphology reveals an affinity between Monterenzio Vecchio and Iron Age Italian samples. However, when the Monterenzio Vecchio sample is separated by isotopic results into locals and non-locals, the latter share affinity with the sample of non-continental Celts from Yorkshire (UK). Moreover, systematic analyses demonstrate that ethnic background does not retain measurable impact on the distribution of funerary elements. Our results confirm the migration of Celtic populations in Monterenzio as archaeologically hypothesized on the basis of the grave goods, followed by a high degree of cultural admixture between exogenous and endogenous traits. This contribution shows that combining different methods offers a more comprehensive perspective for the exploration of biocultural processes in past and present populations.

Temperature dependence of the isotope chemistry of the heavy elements.

PubMed Central

Bigeleisen, J

1996-01-01

The temperature coefficient of equilibrium isotope fractionation in the heavy elements is shown to be larger at high temperatures than that expected from the well-studied vibrational isotope effects. The difference in the isotopic behavior of the heavy elements as compared with the light elements is due to the large nuclear isotope field shifts in the heavy elements. The field shifts introduce new mechanisms for maxima, minima, crossovers, and large mass-independent isotope effects in the isotope chemistry of the heavy elements. The generalizations are illustrated by the temperature dependence of the isotopic fractionation in the redox reaction between U(VI) and U(IV) ions. PMID:8790340

ICP-MS for isotope ratio measurement

USDA-ARS?s Scientific Manuscript database

The use of stable isotopes in mineral nutrition research has become a fundamental aspect of conducting this research. A gradual transition has occurred, now virtually complete, from radioactive isotope studies to those using stable isotopes. Although primarily used in human research, mineral stable ...

Isotopic constraints on global atmospheric methane sources and sinks: a critical assessment of recent findings and new data

NASA Astrophysics Data System (ADS)

Schwietzke, S.; Sherwood, O.; Michel, S. E.; Bruhwiler, L.; Dlugokencky, E. J.; Tans, P. P.

2017-12-01

Methane isotopic data have increasingly been used in recent studies to help constrain global atmospheric methane sources and sinks. The added scientific contributions to this field include (i) careful comparisons and merging of atmospheric isotope measurement datasets to increase spatial coverage, (ii) in-depth analyses of observed isotopic spatial gradients and seasonal patterns, and (iii) improved datasets of isotopic source signatures. Different interpretations have been made regarding the utility of the isotopic data on the diagnosis of methane sources and sinks. Some studies have found isotopic evidence of a largely microbial source causing the renewed growth in global atmospheric methane since 2007, and underestimated global fossil fuel methane emissions compared to most previous studies. However, other studies have challenged these conclusions by pointing out substantial spatial variability in isotopic source signatures as well as open questions in atmospheric sinks and biomass burning trends. This presentation will review and contrast the main arguments and evidence for the different conclusions. The analysis will distinguish among the different research objectives including (i) global methane budget source attribution in steady-state, (ii) source attribution of recent global methane trends, and (iii) identifying specific methane sources in individual plumes during field campaigns. Additional comparisons of model experiments with atmospheric measurements and updates on isotopic source signature data will complement the analysis.

Thermal evolution of old white dwarfs

NASA Astrophysics Data System (ADS)

Kozhberov, Andrew

2017-11-01

This work is devoted to a description of thermodynamic properties of Coulomb crystals which are expected to form in white dwarf interiors. Effects of magnetic field, isotopic impurities, polarization of the electron background and crystal lattice type on the thermal evolution of white dwarfs are discussed. It is shown that the electron polarization could play a noticeable role in the cooling process. While other parameters in concern do not make a significant impact.

Low Background Signal Readout Electronics for the MAJORANA DEMONSTRATOR

DOE Office of Scientific and Technical Information (OSTI.GOV)

Guinn, I.; Abgrall, N.; Arnquist, Isaac J.

2015-03-18

The Majorana Demonstrator (MJD)[1] is an array of p-type point contact (PPC) high purity Germanium (HPGe) detectors intended to search for neutrinoless double beta decay (0vBB decay) in 76Ge. MJD will consist of 40 kg of detectors, 30 kg of which will be isotopically enriched to 87% 76Ge. The array will consist of 14 strings of four or ve detectors placed in two separate cryostats. One of the main goals of the experiment is to demonstrate the feasibility of building a tonne-scale array of detectors to search for 0vBB decay with a much higher sensitivity. This involves acheiving backgrounds inmore » the 4 keV region of interest (ROI) around the 2039 keV Q-value of the BB decay of less than 1 count/ROI-t-y. Because many backgrounds will not directly scale with detector mass, the specific background goal of MJD is less than 3 counts/ROI-t-y.« less

Nucleosynthetic Heterogeneity Controls Vanadium Isotope Variations in Bulk Chondrites

NASA Technical Reports Server (NTRS)

Nielsen, S. G.; Righter, K.; Wu, F.; Owens, J. D.; Prytulak, J.; Burton, K.; Parkinson, I.; Davis, D.

2018-01-01

The vanadium (V) isotope composition of early solar system materials have been hypothesized to be sensitive to high energy irradiation that originated from the young Sun. Vanadium has two isotopes with masses 50 and 51 that have (51)V/(50)V ratio of approximately 410. High energy irradiation produces (50)V from various target isotopes of Ti, Cr and Fe, which would result in light V isotope compositions (expressed as delta (51)V in per mille = 1000 x (((51)V/(50)V(sub sample)/(51)V/(50)V(sub AlfaAesar)) - 1)) relative to a presumably chondritic starting composition. Recently published V isotope data for calcium aluminium inclusions (CAIs) has revealed some very negative values relative to chondrites (by almost -4 per mille) that were indeed interpreted to reflect irradiation processes despite the fact that the studied CAIs all exhibited significant initial abundances of (10)Be, while only a few CAIs displayed light V isotope compositions. It is difficult to relate V isotope variations directly to a singular process because V only possesses two isotopes. Therefore, V isotope variations can principally be produced both mass dependent and independent processes. Mass dependent kinetic stable isotope fractionation is common in CAIs for refractory elements due to partial condensation/evaporation processes. The element strontium (Sr) has an almost identical condensation temperature to V and studies of stable Sr isotope compositions in CAIs reveal both heavy and light values relative to chondrites of several permil. These variations are similar in magnitude to those reported for V isotopes in CAIs, which suggests it is possible that some of the V isotope variation in CAIs could be due to kinetic stable isotope fractionation during condensation/evaporation processes.

How yield relates to ash content, Δ13C and Δ18O in maize grown under different water regimes

PubMed Central

Cabrera-Bosquet, Llorenç; Sánchez, Ciro; Araus, José Luis

2009-01-01

Background and Aims Stable isotopes have proved a valuable phenotyping tool when breeding for yield potential and drought adaptation; however, the cost and technical skills involved in isotope analysis limit its large-scale application in breeding programmes. This is particularly so for Δ18O despite the potential relevance of this trait in C4 crops. The accumulation of minerals (measured as ash content) has been proposed as an inexpensive way to evaluate drought adaptation and yield in C3 cereals, but little is known of the usefulness of this measure in C4 cereals such as maize (Zea mays). The present study investigates how yield relates to ash content, Δ13C and Δ18O, and evaluates the use of ash content as an alternative or complementary criterion to stable isotopes in assessing yield potential and drought resistance in maize. Methods A set of tropical maize hybrids developed by CIMMYT were subjected to different water availabilities, in order to induce water stress during the reproductive stages under field conditions. Ash content and Δ13C were determined in leaves and kernels. In addition, Δ18O was measured in kernels. Key Results Water regime significantly affected yield, ash content and stable isotopes. The results revealed a close relationship between ash content in leaves and the traits informing about plant water status. Ash content in kernels appeared to reflect differences in sink–source balance. Genotypic variation in grain yield was mainly explained by the combination of ash content and Δ18O, whilst Δ13C did not explain a significant percentage of such variation. Conclusions Ash content in leaves and kernels proved a useful alternative or complementary criterion to Δ18O in kernels for assessing yield performance in maize grown under drought conditions. PMID:19773272

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hervey, IV, William Judson; Khalsa-Moyers, Gurusahai K; Lankford, Patricia K

Protein enrichments of engineered, affinity-tagged (or bait ) fusion proteins with interaction partners are often laden with background, non-specific proteins, due to interactions that occur in vitro as an artifact of the technique. Furthermore, the in vivo expression of the bait protein may itself affect physiology or metabolism. In this study, intrinsic affinity purification challenges were investigated in a model protein complex, DNA-dependent RNA polymerase (RNAP), encompassing chromosome- and plasmid-encoding strategies for bait proteins in two different microbial species: Escherichia coli and Rhodopseudomonas palustris. Isotope ratio measurements of bait protein expression strains relative to native, wild-type strains were performed bymore » liquid chromatography tandem mass spectrometry (LC-MS-MS) to assess bait protein expression strategies in each species. Authentic interacting proteins of RNAP were successfully discerned from artifactual co-isolating proteins by the isotopic differentiation of interactions as random or targeted (I-DIRT) method (A. J. Tackett et al. J. Proteome Res. 2005, 4 (5), 1752-1756). To investigate broader effects of bait protein production in the bacteria, we compared proteomes from strains harboring a plasmid that encodes an affinity-tagged subunit (RpoA) of the RNAP complex with the corresponding wild-type strains using stable isotope metabolic labeling. The ratio of RpoA abundance in plasmid strains versus wild type was 0.8 for R. palustris and 1.7 for E. coli. While most other proteins showed no appreciable difference, proteins significantly increased in abundance in plasmid-encoded bait-expressing strains of both species included the plasmid encoded antibiotic resistance protein, GenR and proteins involved in amino acid biosynthesis. Together, these local, complex-specific and more global, whole proteome isotopic abundance ratio measurements provided a tool for evaluating both in vivo and in vitro effects of plasmid-encoding strategies for bait protein expression. This approach has the potential for enabling discovery of protein-protein interactions among the growing number of sequenced microbial species without the need for development of chromosomal insertion systems.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jiang, C. L.; Santiago-Gonzalez, D.; Almaraz-Calderon, S.

Carbon burning is a critical phase for nucleosynthesis in massive stars. The conditions for igniting this burning stage, and the subsequent isotope composition of the resulting ashes, depend strongly on the reaction rate for 12C+ 12C fusion at very low energies. Results for the cross sections for this reaction are influenced by various backgrounds encountered in measurements at such energies. In this paper, we report on a new measurement of 12C+ 12C fusion cross sections where these backgrounds have been minimized. In conclusion, it is found that the astrophysical S factor exhibits a maximum around E cm=3.5–4.0 MeV, which leadsmore » to a reduction of the previously predicted astrophysical reaction rate.« less

Reaction rate for carbon burning in massive stars

NASA Astrophysics Data System (ADS)

Jiang, C. L.; Santiago-Gonzalez, D.; Almaraz-Calderon, S.; Rehm, K. E.; Back, B. B.; Auranen, K.; Avila, M. L.; Ayangeakaa, A. D.; Bottoni, S.; Carpenter, M. P.; Dickerson, C.; DiGiovine, B.; Greene, J. P.; Hoffman, C. R.; Janssens, R. V. F.; Kay, B. P.; Kuvin, S. A.; Lauritsen, T.; Pardo, R. C.; Sethi, J.; Seweryniak, D.; Talwar, R.; Ugalde, C.; Zhu, S.; Bourgin, D.; Courtin, S.; Haas, F.; Heine, M.; Fruet, G.; Montanari, D.; Jenkins, D. G.; Morris, L.; Lefebvre-Schuhl, A.; Alcorta, M.; Fang, X.; Tang, X. D.; Bucher, B.; Deibel, C. M.; Marley, S. T.

2018-01-01

Carbon burning is a critical phase for nucleosynthesis in massive stars. The conditions for igniting this burning stage, and the subsequent isotope composition of the resulting ashes, depend strongly on the reaction rate for 12C+12C fusion at very low energies. Results for the cross sections for this reaction are influenced by various backgrounds encountered in measurements at such energies. In this paper, we report on a new measurement of 12C+12C fusion cross sections where these backgrounds have been minimized. It is found that the astrophysical S factor exhibits a maximum around Ecm=3.5 -4.0 MeV, which leads to a reduction of the previously predicted astrophysical reaction rate.

Atmospheric trace elements and Pb isotopes at an offshore site, Ieodo Ocean Research Station, in the East China Sea from June to October 2015

NASA Astrophysics Data System (ADS)

Lee, S.; Han, C.; Shin, D.; Hur, S. D.; Jun, S. J.; Kim, Y. T.; Hong, S.

2016-12-01

East Asia, especially China, has become a major anthropogenic source region of trace elements due to the rapid industrialization and urbanization in the past decades. Numerous studies reported that anthropogenic pollutants from East Asia are transported by westerly winds during winter to spring across the Pacific to North America and beyond. Here we report elemental concentrations and Pb isotope ratios in airborne particles from Ieodo Ocean Research Station (IORS) located in the middle of the East China Sea (32.07o N, 125.10o E). A total of 30 aerosol samples (PM2.5-10) were collected between 18 June and 30 October 2015 and analyzed for trace elements (Zn, As, Mo, Cd, Sb, Ba, Tl, and Pb) and Pb isotopes using ICP-SFMS and TIMS, respectively. The mean concentrations of trace elements ranged from 0.06 ng m-3 for Tl to 10.1 ng m-3 for Zn. These values are much lower (up to several orders) than those at unban sites in East Asia, confirming a low level of air pollution at IORS due to the remoteness of the site from major sources of anthropogenic pollutants. On the other hand, the mean crustal enrichment factors, calculated using Ba as a conservative crustal element, are much higher than unity (84 for Tl, 100 for Mo, 140 for Pb, 166 for Zn, 262 for As, 526 for Cd, and 570 for Sb, respectively), indicating that these elements are of anthropogenic origin. Combining the Pb isotope ratios and the HYSPLIT model 5-day backward trajectory analysis, we have identified episodic long-range transport of air pollutants from diverse source regions of China, Korea, Japan and Taiwan to the site in summer (June to August). By comparison, an increasing long-range transport of pollution from China was observed in autumn (September and October). Finally, our study shows that IORS is an ideal background site for monitoring levels of concentrations and source origins of atmospheric trace elements in East Asia.

Discrimination factors of carbon and nitrogen stable isotopes from diet to hair and scat in captive tigers (Panthera tigris) and snow leopards (Uncia uncia).

PubMed

Montanari, Shaena; Amato, George

2015-06-15

In order to use stable isotope ratio values obtained from wild animal tissues, we must accurately calculate the differences in isotope ratios between diet and consumer (δtissue - δdiet). These values, called trophic discrimination factors (TDFs, denoted with ∆), are necessary for stable isotope ecology studies and are best calculated in controlled environments. Scat, hair, and diet samples were collected from captive tigers (n = 8) and snow leopards (n = 10) at the Bronx Zoo. The isotope ratios of carbon and nitrogen, the two most commonly used in ecological studies, of the samples were measured by continuous-flow isotope ratio mass spectrometry. The trophic discrimination factors were calculated for both carbon (δ(13)C values) and nitrogen (δ(15)N values). It was found that the only significant TDFs in this study were diet-hair, ∆(13)CHair, for snow leopards (5.97 ± 1.25‰) and tigers (6.45 ± 0.54‰), and diet-scat, ∆(15)NScat, in snow leopards (2.49 ± 1.30‰). The other mean isotope ratios were not significantly different from that of the premixed feline diet. The ∆(15)NHair values for both species were unusually low, potentially due to the protein content and quality of the feline diet. The discrimination factors of the stable isotopes of carbon and nitrogen calculated in this study can be applied to ecological studies of wild, non-captive terrestrial mammals. The effect of protein quality in isotope discrimination is also worthy of further investigation to better understand variation in TDFs. Carnivore scat is shown to be a valuable material for isotopic analysis. Copyright © 2015 John Wiley & Sons, Ltd.

Multiple stable isotope fronts during non-isothermal fluid flow

NASA Astrophysics Data System (ADS)

Fekete, Szandra; Weis, Philipp; Scott, Samuel; Driesner, Thomas

2018-02-01

Stable isotope signatures of oxygen, hydrogen and other elements in minerals from hydrothermal veins and metasomatized host rocks are widely used to investigate fluid sources and paths. Previous theoretical studies mostly focused on analyzing stable isotope fronts developing during single-phase, isothermal fluid flow. In this study, numerical simulations were performed to assess how temperature changes, transport phenomena, kinetic vs. equilibrium isotope exchange, and isotopic source signals determine mineral oxygen isotopic compositions during fluid-rock interaction. The simulations focus on one-dimensional scenarios, with non-isothermal single- and two-phase fluid flow, and include the effects of quartz precipitation and dissolution. If isotope exchange between fluid and mineral is fast, a previously unrecognized, significant enrichment in heavy oxygen isotopes of fluids and minerals occurs at the thermal front. The maximum enrichment depends on the initial isotopic composition of fluid and mineral, the fluid-rock ratio and the maximum change in temperature, but is independent of the isotopic composition of the incoming fluid. This thermally induced isotope front propagates faster than the signal related to the initial isotopic composition of the incoming fluid, which forms a trailing front behind the zone of transient heavy oxygen isotope enrichment. Temperature-dependent kinetic rates of isotope exchange between fluid and rock strongly influence the degree of enrichment at the thermal front. In systems where initial isotope values of fluids and rocks are far from equilibrium and isotope fractionation is controlled by kinetics, the temperature increase accelerates the approach of the fluid to equilibrium conditions with the host rock. Consequently, the increase at the thermal front can be less dominant and can even generate fluid values below the initial isotopic composition of the input fluid. As kinetics limit the degree of isotope exchange, a third front may develop in kinetically limited systems, which propagates with the advection speed of the incoming fluid and is, therefore, traveling fastest. The results show that oxygen isotope signatures at thermal fronts recorded in rocks and veins that experienced isotope exchange with fluids can easily be misinterpreted, namely if bulk analytical techniques are applied. However, stable isotope microanalysis on precipitated minerals may - if later isotope exchange is kinetically limited - provide a valuable archive of the transient thermal and hydrological evolution of a system.

Rapidly Assessing Changes in Bone Mineral Balance Using Natural Stable Calcium Isotopes

NASA Technical Reports Server (NTRS)

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

2011-01-01

We demonstrate that variations in the Ca isotope ratios in urine rapidly and quantitatively reflect changes in bone mineral balance. This variation occurs because bone formation depletes soft tissue of light Ca isotopes, while bone resorption releases that isotopically light Ca back into soft tissue. In a study of 12 individuals confined to bed rest, a condition known to induce bone resorption, we show that Ca isotope ratios shift in a direction consistent with net bone loss after just 7 days, long before detectible changes in bone density occur. Consistent with this interpretation, the Ca isotope variations track changes observed in N-teleopeptide, a bone resorption biomarker, while bone-specific alkaline phosphatase, a bone formation biomarker, is unchanged. Ca isotopes can in principle be used to quantify net changes in bone mass. Ca isotopes indicate an average loss of 0.62 +/- 0.16 % in bone mass over the course of this 30-day study. The Ca isotope technique should accelerate the pace of discovery of new treatments for bone disease and provide novel insights into the dynamics of bone metabolism.

Effects of spin crossover on iron isotope fractionation in Earth's mantle

NASA Astrophysics Data System (ADS)

Qin, T.; Shukla, G.; Wu, Z.; Wentzcovitch, R.

2017-12-01

Recent studies have revealed that the iron isotope composition of mid-ocean ridge basalts (MORBs) is +0.1‰ richer in heavy Fe (56Fe) relative to chondrites, while basalts from Mars and Vesta have similar Fe isotopic composition as chondrites. Several hypotheses could explain these observations. For instance, iron isotope fractionation may have occurred during core formation or Earth may have lost some light Fe isotope during the high temperature event in the early Earth. To better understand what drove these isotopic observations, it is important to obtain accurate Fe isotope fractionation factors among mantle and core phases at the relevant P-T conditions. In bridgmanite, the most voluminous mineral in the lower mantle, Fe can occupy more than one crystalline site, be in ferrous and/or ferric states, and may undergo a spin crossover in the lower mantle. Iron isotopic fractionation properties under spin crossover are poorly constrained, while this may be relevant to differentiation of Earth's magma ocean. In this study we address the effect of these multiple states on the iron isotope fractionation factors between mantle and core phases.

Isotopic Effects in Nuclear Fragmentation and GCR Transport Problems

NASA Technical Reports Server (NTRS)

Cucinotta, Francis A.

2002-01-01

Improving the accuracy of the galactic cosmic ray (GCR) environment and transport models is an important goal in preparing for studies of the projected risks and the efficiency of potential mitigations methods for space exploration. In this paper we consider the effects of the isotopic composition of the primary cosmic rays and the isotopic dependence of nuclear fragmentation cross sections on GCR transport models. Measurements are used to describe the isotopic composition of the GCR including their modulation throughout the solar cycle. The quantum multiple-scattering approach to nuclear fragmentation (QMSFRG) is used as the data base generator in order to accurately describe the odd-even effect in fragment production. Using the Badhwar and O'Neill GCR model, the QMSFRG model and the HZETRN transport code, the effects of the isotopic dependence of the primary GCR composition and on fragment production for transport problems is described for a complete GCR isotopic-grid. The principle finding of this study is that large errors ( 100%) will occur in the mass-flux spectra when comparing the complete isotopic-grid (141 ions) to a reduced isotopic-grid (59 ions), however less significant errors 30%) occur in the elemental-flux spectra. Because the full isotopic-grid is readily handled on small computer work-stations, it is recommended that they be used for future GCR studies.

Exotic Structure of Carbon Isotopes

NASA Astrophysics Data System (ADS)

Suzuki, Toshio; Sagawa, Hiroyuki; Hagino, Kouichi

2003-12-01

Ground state properties of C isotopes, deformation and elecromagnetic moments, as well as electric dipole transition strength are investigated. We first study the ground state properties of C isotopes using a deformed Hartree-Fock (HF) + BCS model with Skyrme interactions. Isotope dependence of the deformation properties is investigated. Shallow deformation minima are found in several neutron-rich C isotopes. It is also shown that the deformation minima appear in both the oblate and the prolate sides in 17C and 19C having almost the same binding energies. Next, we carry out shell model calculations to study electromagnetic moments and electric dipole transitions of C isotopes. We point out the clear configuration dependence of the quadrupole and magnetic moments in the odd C isotopes, which will be useful to find out the deformation and spin-parities of the ground states of these nuclei. Electric dipole states of C isotopes are studied focusing on the interplay between low energy Pigmy strength and giant dipole resonances. Low peak energies, two-peak structure and large widths of the giant resonances show deformation effects. Calculated transition strength below dipole giant resonance in heavier C isotopes than 15C is found to exhaust 12 ~ 15% of the Thomas-Reiche-Kuhn sum rule value and 50 ~ 80% of the cluster sum rule value.

Cleaning and passivation of copper surfaces to remove surface radioactivity and prevent oxide formation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoppe, Eric W.; Seifert, Allen; Aalseth, Craig E.

High-purity copper is an attractive material for constructing ultra-low-background radiation measurement devices. Many low-background experiments using high-purity copper have indicated surface contamination emerges as the dominant background. Radon daughters plate out on exposed surfaces, leaving a residual 210Pb background that is difficult to avoid. Dust is also a problem; even under cleanroom conditions, the amount of U and Th deposited on surfaces can represent the largest remaining background. To control these backgrounds, a copper cleaning chemistry has been developed. Designed to replace an effective, but overly aggressive concentrated nitric acid etch, this peroxide-based solution allows for a more controlled cleaningmore » of surfaces. The acidified hydrogen peroxide solution will generally target the Cu+/Cu2+ species which are the predominant surface participants, leaving the bulk of copper metal intact. This preserves the critical tolerances of parts and eliminates significant waste disposal issues. Accompanying passivation chemistry has also been developed that protects copper surfaces from oxidation. Using a high-activity polonium surface spike, the most difficult-to-remove daughter isotope of radon, the performance of these methods are quantified. © 2001 Elsevier Science. All rights reserved« less

Asian anthropogenic lead contamination in the North Pacific Ocean as evidenced by stable lead isotopic compositions

NASA Astrophysics Data System (ADS)

Zurbrick, Cheryl M.

This dissertation work determined the changing scope of lead (Pb) contamination in the North Pacific Ocean since the phase-out of leaded gasoline in most of the world. Chapters 1 and 2 consisted of validating our method for determining Pb concentrations and isotopic compositions in seawater. Chapter 3 established a baseline of Pb isotopic compositions (PbICs) in the western and central North Pacific in 2002. This was an ideal time to establish such a baseline because China had recently (mid-2000) ceased their use of leaded gasoline and simultaneously began consuming increasingly large amounts of coal, known to have relatively high Pb concentrations. We found subsurface waters were contaminated with Asian industrial Pb, predominantly Chinese coal emissions. In contrast, the abyssal waters were a mix of Asian industrial Pb and background (i.e., natural) Pb. Chapter 4 revisited the western and central North Pacific in 2009 -- 2011 to determine what, if any, changes had occurred in this short time period. We found that Pb in subsurface and abyssal waters of the western North Pacific were similar to Chinese aerosols. Such a large change in the PbICs of abyssal water in 9 years was unanticipated and attributed to the relatively large flux of particle-bound Pb from the euphotic zone to the deep ocean, which was in isotopic equilibrium with the reservoir of dissolved Pb. In contrast, the central North Pacific abyssal water PbICs were similar to values previously reported because of the relatively lower particulate export. Based on comparisons to baseline PbIC data, we determined that abyssal waters in the western and central North Pacific would be isotopically indistinguishable from surface waters in the next three decades. Sources of Pb to coastal California waters were reevaluated in Chapter 5. Prior studies had found that surface waters of the California Current System (CCS) were isotopically consistent with both Asian industrial Pb and US leaded gasoline, still in use at that point in time. In 2010 and 2011, we found that surface and subsurface waters of the CCS were isotopically similar to Asian industrial emissions. However, remobilized US gasoline Pb from sediments in the San Francisco Bay, California, were accumulating in the "mud belt" on the continental shelf and changing the isotopic composition of overlying waters. During periods of intense upwelling, this historic Pb was brought to the surface of the water. However, the much larger quantity of Pb from Asian industrial emissions made the isotopic composition of Pb from historic US gasoline unidentifiable in off-shore waters. A secondary research focus of this dissertation was to improve my own teaching abilities. Chapter 6 explored the intersection of system thinking and aquatic toxicology in undergraduate education. Among a wealth of information, I found that group concept mapping was no more useful to student learning than the same activity done individually. This was due to poor implementation of team learning strategies by me and inadequate time for students to adjust to non-traditional instruction methodologies.

Shell evolution above Z ,N =50 within Skyrme density functional theory: The impact of deformation and tensor interactions

NASA Astrophysics Data System (ADS)

Shi, Yue

2017-03-01

Background: Recent years have seen considerable effort in associating the shell evolution (SE) for a chain of isotones or isotopes with the underlying nuclear interactions. In particular, it has been fairly well established that the tensor part of the Skyrme interaction is indispensable for understanding certain SE above Z ,N =50 shell closures, as a function of nucleon numbers. Purpose: The purpose of the present work is twofold: (1) to study the effect of deformation due to blocking on the SE above Z ,N =50 shell closures and (2) to examine the optimal parametrizations in the tensor part which gives a proper description of the SE above Z ,N =50 shell closures. Methods: I use the Skyrme-Hartree-Fock-Bogoliubov (SHFB) method to compute the even-even vacua of the Z =50 isotopes and N =50 isotones. For Sb and odd-A Sn isotopes, I perform calculations with a blocking procedure which accounts for the polarization effects, including deformations. Results: The blocking SHFB calculations show that the light odd-A Sb isotopes, with only one valence proton occupying down-sloping Ω =11 /2- and Ω =7 /2+ Nilsson orbits, assume finite oblate deformations. This reduces the energy differences between 11 /2- and 7 /2+ states by about 500 keV for 51Sb56 -66 , bringing the energy-difference curve closer to the experimental one. With une2t1 energy density functional (EDF), which differs from unedf2 parametrization by tensor terms, a better description of the slope of Δ e (π 1 h11 /2-π 1 g7 /2) as a function of neutron number has been obtained. However, the trend of Δ e (π 1 g7 /2-π 2 d5 /2) curve is worse using une2t1 EDF. Δ e (ν 3 s1 /2-ν 2 d5 /2) and Δ e (ν 1 g7 /2-ν 2 d5 /2) curve for N =50 isotones using une2t1 seems to be consistent with experimental data. The neutron SE of Δ e (ν 1 h11 /2-ν 1 g7 /2) and Δ e (ν 1 g7 /2-ν 2 d5 /2) for Sn isotopes are shown to be sensive to αT tensor parameter. Conclusions: Within the Skyrme self-consistent mean-field model, the deformation degree of freedom has to be taken into account for Sb isotopes, N =51 isotones, and odd-A Sn isotopes when discussing variation of quantities like shell gap etc. The tensor terms are important for describing the strong variation of Δ E (Ωπ=11 /2--7 /2+) in Sb isotopes. The SE of 1 /2+ and 7 /2+ states in N =51 isotones may show signature for the existence of tensor interaction. The experimental excitation energies of 11 /2- and 7 /2+ states in odd-A Sn isotopes close to 132Sn give prospects for constraining the αT parameter.

Astrophysical quests for neutron capture data of unstable nuclei

NASA Astrophysics Data System (ADS)

Käppeler, F.

2016-11-01

The abundances of the chemical elements heavier than iron can be attributed in about equal parts to the r and to the s process, which are taking place in supernova explosions and during the He and C burning phases of stellar evolution, respectively. So far, quantitative studies on the extremely short-lived neutron-rich nuclei constituting the ( n, γ) network of the r process are out of reach. On the contrary, the situation for the s -process is far advanced, as the reaction path of the s process from 12C to the Pb/Bi region is located within the valley of stability. Accordingly, a comprehensive database of experimental ( n, γ) cross sections has been established. While for many stable isotopes the necessary accuracy is still to be reached, reliable cross sections for the involved unstable isotopes are almost completely missing. Because of the intrinsic γ background of radioactive samples, successful time-of-flight measurements are depending on intense pulsed neutron sources. Such data are fundamental for our understanding of branchings in the s -process reaction path, which carry important model-independent information on neutron flux and temperature in the deep stellar interior.

Enrichment of 57Fe isotope in neutron flux of nuclear reactors observed by Mössbauer spectroscopy.

PubMed

Sawicki, Jerzy A

2018-02-01

The abundance of 57 Fe isotope in nuclear reactor core materials can be considerably enriched by neutron-capture 56 Fe(n,γ) reactions. This is demonstrated using the sections of Zr-2.5 wt.%Nb pressure tubes removed from two CANDU* reactors. The tubes contained 0.11 and 0.04wt% Fe and were irradiated for about 10 effective full power years (EFPY) up to ~10 26 n/m 2 fast neutron (E > 1MeV) fluencies. The Mössbauer spectra of 57 Fe in irradiated samples indicated up to 10 times larger areas than unirradiated off-cuts from the same pressure tubes. The observed effect is in accord with the values calculated for known thermal neutron-capture cross-sections and resonance capture integrals, neutron flux profiles and spectra, and times of irradiation. The build-up of 57 Fe facilitated recording Mössbauer absorption spectra of alloys with minor amount of Fe down to ~ 400ppm, despite intense background radiation emitted by samples. These findings can open new possibilities in post-irradiation studies of alloys used in nuclear reactors and in other objects subjected to large neutron fluencies. Copyright © 2017 Elsevier Ltd. All rights reserved.

Muon capture on light isotopes in Double Chooz

NASA Astrophysics Data System (ADS)

Strait, M.; Double Chooz Collaboration

2017-09-01

Using the Double Chooz reactor neutrino detector, we have measured the products of µ - capture on 12C, 13C, 14N and 16O. Over a period of 490 days, we collected 2.3 × 106 stopping cosmic µ -, of which 1.8 × 105 captured on these nuclei in the inner detector. The resulting isotopes were tagged using prompt neutron emission (when applicable), the subsequent beta decays, and, in some cases, β-delayed neutrons. Production of these βn isotopes, primarily 9Li, which are {{{ν _e}} \\over {{ν _μ }}} backgrounds, was found at a significance of 5.5σ. The probability of 9Li production per capture on natC is (2.4 ± 0.9(stat) ± 0.1(syst)) × 10-4. We have made the most precise measurement of the rate of 12C(µ -, ν)12B to date, 6.57 - 0.21 + 0.11 × {10^3}{{ }}{{{s}} - 1},{{ or }}≤ft( {17.35 - 0.59 + 0.35} \\right)% of nuclear captures. By tagging excited states emitting gammas, the ground state transition rate to 12B is found to be 5.68 - 0.23 + 0.14 × {10^3}{{ }}{{{s}} - 1}.

Reference measurements for total mercury and methyl mercury content in marine biota samples using direct or species-specific isotope dilution inductively coupled plasma mass spectrometry.

PubMed

Krata, Agnieszka; Vassileva, Emilia; Bulska, Ewa

2016-11-01

The analytical procedures for reference measurements of the total Hg and methyl mercury (MeHg) mass fractions at various concentration levels in marine biota samples, candidates for certified reference materials (oyster and clam Gafrarium tumidum), were evaluated. Two modes of application of isotope dilution inductively coupled plasma mass spectrometry method (ID ICP-MS), namely direct isotope dilution and species-specific isotope dilution analysis with the use of two different quantification mass spectrometry techniques were compared. The entire ID ICP-MS measurement procedure was described by mathematical modelling and the combined uncertainty of measurement results was estimated. All factors influencing the final results as well as isotopic equilibrium were systematically investigated. This included the procedural blank, the moisture content in the biota samples and all factors affecting the blend ratio measurements (instrumental background, spectral interferences, dead time and mass discrimination effects as well as the repeatability of measured isotopic ratios). Modelling of the entire measurement procedures and the use of appropriate certified reference materials enable to assure the traceability of obtained values to the International System of Units (SI): the mole or the kilogram. The total mass fraction of mercury in oyster and clam biota samples, after correction for moisture contents, was found to be: 21.1 (1.1) 10(-9) kg kg(-1) (U =5.1% relative, k=2) and 390.0 (9.4) 10(-9) kg kg(-1) (U=2.4% relative, k=2), respectively. For the determination of mercury being present as methyl mercury, the non-chromatographic separation on anion-exchange resin AG1-X8 of the blended samples was applied. The content of MeHg (as Hg) in oyster sample was found: 4.81 (24) 10(-9)kgkg(-1) (U=5.0%, k=2) and 4.84 (21) 10(-9)kgkg(-1) (U=4.3%, k=2) with the use of quadrupole (ICP QMS) or sector field (ICP SFMS) inductively coupled plasma mass spectrometers, respectively. In the case of clam sample, the concentration of MeHg (as Hg) was found to be: 61.0 (2.3) 10(-)(9)kgkg(-1) (U=3.8%, k=2) and 61.3 (2.2) 10(-)(9)kgkg(-1) (U=3.6%, k=2), respectively. The mass fractions for total Hg and MeHg determined in this study were used as a contribution of the International Atomic Energy Agency (IAEA) Environment Laboratories in the characterisation of the IAEA 461 and IAEA 470 certified reference materials. The obtained good agreement with the reference values further validated the methods developed in this study. Copyright © 2016 Elsevier B.V. All rights reserved.

Li Isotope Studies of Olivine in Mantle Xenoliths by SIMS

NASA Technical Reports Server (NTRS)

Bell, D. R.; Hervig, R. L.; Buseck, P. R.

2005-01-01

Variations in the ratio of the stable isotopes of Li are a potentially powerful tracer of processes in planetary and nebular environments [1]. Large differences in the 7Li/6Li ratio between the terrestrial upper mantle and various crustal materials make Li isotope composition a potentially powerful tracer of crustal recycling processes on Earth [2]. Recent SIMS studies of terrestrial mantle and Martian meteorite samples report intra-mineral Li isotope zoning [3-5]. Substantial Li isotope heterogeneity also exists within and between the components of chondritic meteorites [6,7]. Experimental studies of Li diffusion suggest the potential for rapid isotope exchange at elevated temperatures [8]. Large variations in 7Li, exceeding the range of unaltered basalts, occur in terrestrial mantle-derived xenoliths from individual localities [9]. The origins of these variations are not fully understood.

Iron-Isotopic Fractionation Studies Using Multiple Collector Inductively Coupled Plasma Mass Spectrometry

NASA Technical Reports Server (NTRS)

Anbar, A. D.; Zhang, C.; Barling, J.; Roe, J. E.; Nealson, K. H.

1999-01-01

The importance of Fe biogeochemistry has stimulated interest in Fe isotope fractionation. Recent studies using thermal ionization mass spectrometry (TIMS) and a "double spike" demonstrate the existence of biogenic Fe isotope effects. Here, we assess the utility of multiple-collector inductively-coupled plasma mass spectrometry(MC-ICP-MS) with a desolvating sample introduction system for Fe isotope studies, and present data on Fe biominerals produced by a thermophilic bacterium. Additional information is contained in the original extended abstract.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bushuev, A. V.; Kozhin, A. F., E-mail: alexfkozhin@yandex.ru; Aleeva, T. B.

An active neutron method for measuring the residual mass of {sup 235}U in spent fuel assemblies (FAs) of the IRT MEPhI research reactor is presented. The special measuring stand design and uniform irradiation of the fuel with neutrons along the entire length of the active part of the FA provide high accuracy of determination of the residual {sup 235}U content. AmLi neutron sources yield a higher effect/background ratio than other types of sources and do not induce the fission of {sup 238}U. The proposed method of transfer of the isotope source in accordance with a given algorithm may be usedmore » in experiments where the studied object needs to be irradiated with a uniform fluence.« less

Hydrologic and environmental controls on uranium-series and strontium isotope ratios in a natural weathering environment

NASA Astrophysics Data System (ADS)

White, A. M.; Ma, L.; Moravec, B. G.; McIntosh, J. C.; Chorover, J.

2017-12-01

In a remote, volcanic headwater catchment of the Jemez River Basin Critical Zone Observatory (JRB-CZO) in NM, stable water isotopes and solute chemistry have shown that snowmelt infiltrates and is stored before later discharging into springs and streams via subsurface flowpaths that vary seasonally. Therefore, water-rock reactions are also expected to change with season as hydrologic flowpaths transport water, gases and solutes through different biogeochemical conditions, rock types and fracture networks. Uranium-series isotopes have been shown to be a novel tracer of water-rock reactions and source water contributions while strontium isotopes are frequently used as indicators of chemical weathering and bedrock geology. This study combines both isotopes to understand how U and Sr isotope signatures evolve through the Critical Zone (CZ). More specifically, this work examines the relationship between seasonality, water transit time (WTT), and U-series and Sr isotopes in stream and spring waters from three catchments within the JRB-CZO, as well as lithology, rock type and CZ structure in solid phase cores. Samples from ten springs with known WTTs were analyzed for U and Sr isotopes to determine the effect of WTT on the isotopic composition of natural waters. Results suggest that WTT alone cannot explain the variability of U and Sr isotopes in JRB-CZO springs. Stream samples were also collected across two water years to establish how seasonality controls surface water isotopic composition. U and Sr isotope values vary with season, consistent with a previous study from the La Jara catchment; however, this study revealed that these changes do not show a systematic pattern among the three catchments suggesting that differences in the mineralogy and structure of the deep CZ in individual catchments, and partitioning of water along deep vs surficial and fracture vs matrix flow paths, likely also control isotopic variability. The distribution of U-series and Sr isotopes in core samples with depth shows distinct weathering profiles with variable 234U/238U activity and Sr isotope ratios. Comparison of the isotopic composition of cores and groundwaters from similar depths, as well as surface waters in the JRB-CZO will be vital for the characterization of hydrogeologic controls on isotopic composition in this complex terrain.

Investigating differences in light stable isotopes between Thai jasmine rice and Sungyod rice

NASA Astrophysics Data System (ADS)

Kukusamude, C.; Kongsri, S.

2017-10-01

We report the differences in light stable isotopes between two kinds of Thai rice (Thai jasmine and Sungyod rice). Thai jasmine rice and Sungyod rice were cultivated in the northeast and the south of Thailand. Light isotopes including 13C, 15N and 18O of Thai jasmine rice and Sungyod rice samples were carried out using isotope ratio mass spectrometry (IRMS). Thai jasmine rice (Khao Dawk Mali 105) was cultivated from Thung Kula Rong Hai area, whereas Sungyod rice was cultivated from Phathalung province. Hypothesis testing of difference of each isotope between Thai jasmine rice and Sungyod rice was also studied. The study was the feasibility test whether the light stable isotopes can be the variables to identify Thai jasmine rice and Sungyod rice. The result shows that there was difference in the isotope patterns of Thai jasmine rice and Sungyod rice. Our results may provide the useful information in term of stable isotope profiles of Thai rice.

STABLE ISOTOPES IN ECOLOGICAL STUDIES: NEW DEVELOPMENTS IN MIXING MODELS

EPA Science Inventory

Stable isotopes are increasingly being used as tracers in ecological studies. One application uses isotopic ratios to quantify the proportional contributions of multiple sources to a mixture. Examples include food sources for animals, water sources for plants, pollution sources...

Isotopic composition of atmospheric moisture from pan water evaporation measurements.

PubMed

Devi, Pooja; Jain, Ashok Kumar; Rao, M Someshwer; Kumar, Bhishm

2015-01-01

A continuous and reliable time series data of the stable isotopic composition of atmospheric moisture is an important requirement for the wider applicability of isotope mass balance methods in atmospheric and water balance studies. This requires routine sampling of atmospheric moisture by an appropriate technique and analysis of moisture for its isotopic composition. We have, therefore, used a much simpler method based on an isotope mass balance approach to derive the isotopic composition of atmospheric moisture using a class-A drying evaporation pan. We have carried out the study by collecting water samples from a class-A drying evaporation pan and also by collecting atmospheric moisture using the cryogenic trap method at the National Institute of Hydrology, Roorkee, India, during a pre-monsoon period. We compared the isotopic composition of atmospheric moisture obtained by using the class-A drying evaporation pan method with the cryogenic trap method. The results obtained from the evaporation pan water compare well with the cryogenic based method. Thus, the study establishes a cost-effective means of maintaining time series data of the isotopic composition of atmospheric moisture at meteorological observatories. The conclusions drawn in the present study are based on experiments conducted at Roorkee, India, and may be examined at other regions for its general applicability.

Annual INTEC Groundwater Monitoring Report for Group 5 - Snake River Plain Aquifer (2001)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Roddy, Michael Scott

2002-02-01

This report describes the monitoring activities conducted and presents the results of groundwater sampling and water-level measurements from October 2000 to September 2001. Groundwater samples were initially collected from 41 wells from the Idaho Nuclear Technology and Engineering Center and the Central Facilities Area and analyzed for iodine-129, strontium-90, tritium, gross alpha, gross beta, technetium-99, uranium isotopes, plutonium isotopes, neptunium-237, americium-241, gamma spectrometry, and mercury. Samples from 41 wells were collected in April and May 2001. Additional sampling was conducted in August 2001 and included the two CFA production wells, the CFA point of compliance for the production wells, onemore » well that was previously sampled and five additional monitoring wells. Iodine-129 and strontium-90 were the only analytes above their respective maximum contaminant levels. Iodine-129 was detected just above its maximum contaminant level of 1 pCi/L at two of the Central Facilities Area landfill wells. Iodine-129 was detected in the CFA production wells at 0.35±0.083 pCi/L in CFA-1, but was below detectable activity in CFA-2. Strontium-90 was above its maximum contaminant level of 8 pCi/L in several wells near the Idaho Nuclear Technology and Engineering Center but was below its maximum contaminant level in the downgradient wells at the Central Facilities Area landfills. Sr-90 was not detected in the CFA production wells. Gross beta results generally mirrored the results for strontium-90 and technetium-99. Plutonium isotopes and neptunium-237 were not detected. Uranium-233/234 and uranium-238 isotopes were detected in all samples. Concentrations of background and site wells were similar and are within background limits for total uranium determined by the USGS, suggesting that the concentrations are background. Uranium-235/236 was detected in 11 samples, but all the detected concentrations were similar and near the minimum detectable activity. Americium-241 was detected at three locations near the minimum detectable activity of approximately 0.07 pCi/L. The gamma spectrometry results detected cesium-137 in three samples, potassium-40 at eight locations, and radium-226 at one location. Mercury was below its maximum contaminant level of 2 µg/L in all samples. Gamma spectrometry results for the CFA production wells did not detect any analytes. Water-level measurements were taken from wells in the Idaho Nuclear Technology and Engineering Center, Central Facilities Area, and the area south of Central Facilities Area to evaluate groundwater flow directions. Water-level measurements indicated groundwater flow to the south-southwest from the Idaho Nuclear Technology and Engineering Center.« less

Electrothermal vaporization of mineral acid solutions in inductively coupled plasma mass spectrometry: comparison with sample nebulization

NASA Astrophysics Data System (ADS)

Mora, Juan; Gras, Luis; van Veen, Eric H.; de Loos-Vollebregt, Margaretha T. C.

1999-06-01

The analytical behaviour of an electrothermal vaporization (ETV) device for the introduction of mineral acid solutions in inductively coupled plasma mass spectrometry (ICP-MS) was evaluated. Water, nitric acid, hydrochloric acid, perchloric acid and sulphuric acid in concentrations within the 0.05-1.0 mol l-1 range were studied. For all the acids tested, increasing the acid concentration increases the ion signal and deteriorates the precision. The magnitude of the signal enhancement depends on the analyte and on the acid considered. Acid solutions give rise to ion signals that are between 2 and 10 times higher than those with water. Among the acids tested, sulphuric acid provides the highest signals. The addition of palladium reduces matrix effects due to the acids and increases the signal in ETV ICP-MS. In comparison with conventional sample nebulization (CS), the ETV sample introduction system provides higher sensitivities (between 2 and 20 times higher) at the same acid concentration. The magnitude of this improvement is similar to that obtained with a microwave desolvation system (MWDS). The ETV sample introduction system gives rise to the lowest background signals from matrix-induced species. Due to this fact, the limits of detection (LODs) obtained for the isotopes affected by any interference are lower for ETV sample introduction than those obtained with the CS and the MWDS. For the isotopes that do not suffer from matrix-induced spectral interferences, the ETV gives rise to LODs higher than those obtained with the CS. For these isotopes the lowest LODs are obtained with MWDS.

A practical method for the determination of total selenium in environmental samples using isotope dilution-hydride generation-inductively coupled plasma-mass spectrometry

USGS Publications Warehouse

Kleckner, Amy E.; Kakouros, Evangelos; Stewart, A. Robin

2017-01-01

A safe, practical, and accurate method for the determination of selenium (Se) in range of environmental samples was developed. Small sample masses, 5–20 mg, were amended with 82Se enriched isotope for the isotope dilution (ID), preceding a multi-step wet digestion with nitric acid (HNO3) and hydrogen peroxide (H2O2). Samples were incubated in an autoclave for 3 h at 20 psi and 126°C. Digestates were subsequently reduced with concentrated hydrochloric acid to Se(IV) the most favorable valence for hydride generation (HG). The solutions were then analyzed on an ICP-MS equipped with Flow Injection system (FIAS-400). Polyatomic, isobaric, and background interferences were removed through the use of HG and ID with an 82Se enriched isotope spike. Recoveries for certified reference materials were determined and averaged 96% for biological tissues (NRCC DOLT3, DOLT4, DORM2, TORT2, and TORT3, and NIST 2976) and 108% for estuarine sediment (NRCC PACS2) with an average coefficient of variation for replicate measurements of ∼ 3.5%. Limit of detection was 0.13 ng Se g−1 dry weight or 0.19 ng Se L−1. This method can be broadly applied to biological tissues, sediments, suspended particulates, and water samples with minimal modifications making this method highly useful for assessing the ecotoxicology of total Se in aquatic ecosystems.

Lead isotopes in lichen transplants around a Cu smelter in Russia determined by MC-ICP-MS reveal transient records of multiple sources.

PubMed

Spiro, B; Weiss, D J; Purvis, O W; Mikhailova, I; Williamson, B J; Coles, B J; Udachin, V

2004-12-15

Transplants of the lichen Hypogymnia physodes, which is relatively tolerant to SO2 and heavy metals, were deployed for 3 months over a 60 km long SW-NE transect centered on a highly polluting Cu smelter and its adjoining town of Karabash, southern Urals, Russia. The abundance of 206Pb, 207Pb, 208Pb, and 204Pb were determined by MC-ICP-MS. The measurement of 204Pb revealed critical features, which would otherwise remain concealed: (i) The precise isotope ratios referenced to 204Pb allowed several different sources to be resolved even within the small area covered: (a) the obvious pollutant source of the Karabash Cu smelter; (b) two dispersed sources, likely to include soil with lower and different contributions of thorogenic and uranogenic lead; and (c) one anthropogenic source with higher contribution of 235U derived Pb. (ii) In part of the transect, the Pb isotope composition changed while the Pb concentrations remained the same. This indicates that the Pb content of the transplantation material from the background site was largely replaced and that the transplants provide a transient record reflecting a continuous accumulation and loss of environmental Pb, probably mainly in the form of extracellular particles. Overall, the method of lichen transplantation coupled with Pb isotope ratio determinations proved effective in assessing the usefulness of lichens in biomonitoring and in resolving different sources of atmospheric deposition.

Inferring foliar water uptake using stable isotopes of water.

PubMed

Goldsmith, Gregory R; Lehmann, Marco M; Cernusak, Lucas A; Arend, Matthias; Siegwolf, Rolf T W

2017-08-01

A growing number of studies have described the direct absorption of water into leaves, a phenomenon known as foliar water uptake. The resultant increase in the amount of water in the leaf can be important for plant function. Exposing leaves to isotopically enriched or depleted water sources has become a common method for establishing whether or not a plant is capable of carrying out foliar water uptake. However, a careful inspection of our understanding of the fluxes of water isotopes between leaves and the atmosphere under high humidity conditions shows that there can clearly be isotopic exchange between the two pools even in the absence of a change in the mass of water in the leaf. We provide experimental evidence that while leaf water isotope ratios may change following exposure to a fog event using water with a depleted oxygen isotope ratio, leaf mass only changes when leaves are experiencing a water deficit that creates a driving gradient for the uptake of water by the leaf. Studies that rely on stable isotopes of water as a means of studying plant water use, particularly with respect to foliar water uptake, must consider the effects of these isotopic exchange processes.

Substitution of stable isotopes in Chlorella

NASA Technical Reports Server (NTRS)

Flaumenhaft, E.; Katz, J. J.; Uphaus, R. A.

1969-01-01

Replacement of biologically important isotopes in the alga Chlorella by corresponding heavier stable isotopes produces increasingly greater deviations from the normal cell size and changes the quality and distribution of certain cellular components. The usefulness of isotopically altered organisms increases interest in the study of such permuted organisms.

Preservation of carbonate clumped isotopes in sedimentary paleoclimate archives

NASA Astrophysics Data System (ADS)

Henkes, G. A.; Passey, B. H.; Grossman, E. L.; Shenton, B.; Perez-Huerta, A.

2014-12-01

Carbonate clumped isotope thermometry is increasingly used to reconstruct paleotemperatures of ancient terrestrial environments. One promising application is elucidating paleoelevation from carbonate archives such as paleosols, lacustrine marls, and fossil freshwater shells. Unlike conventional stable isotope approaches (e.g., mineral δ18O or δD), clumped isotope thermometry is independent of the isotopic composition of the precipitating waters and can therefore be used to reconstruct elevation by both the temperature-altitude relationship and the rainfall δ18O-altitude relationship. However, interpretation of clumped isotope data is not without its own complications. Like conventional stable isotopes, clumped isotope paleotemperatures can be effectively reset to warmer values by dissolution/reprecipitation-type diagenesis during sedimentary burial. It is also known that carbonate clumped isotope bonds (i.e., 13C-18O) are susceptible to 'reordering' in the solid mineral lattice at warmer burial temperatures, with laboratory studies of natural carbonates indicating activation of this phenomenon at temperatures as low as 100 °C over geologic timescales. A challenge in applying carbonate clumped isotope thermometry to natural samples is now evaluating terrestrial archives with respect to both types of alteration: 'open-system' alteration and 'closed-system' bond reordering. In this talk we will review our experimental efforts to constrain the kinetics of clumped isotope reordering, with relevance to low-temperature carbonates like fossil shells and early diagenetic minerals, and present new laboratory data that further inform our theoretical framework for the mechanism(s) of 13C-18O bond reordering. Together with traditional analytical and petrographic screening for recrystallization, empirical and laboratory studies of carbonate clumped isotope reordering represent the next steps in evaluating isotopic records of paleoclimate, paleobiology, and paleoelevation that are emerging from clumped isotope analyses.

Isotopy of the hydrosphere

NASA Astrophysics Data System (ADS)

Ferronskii, V. I.; Poliakov, V. A.

This book is concerned with the natural relations regarding the distribution of the stable isotopes of hydrogen and oxygen in the hydrosphere, taking into account the most important problems with respect to the dynamics and the origin of waters. The solution of these problems on an isotopic basis is considered. The physicochemical principles of isotope separation are discussed along with the isotopic composition of atmospheric moisture, the isotopic composition of surface continental waters, the hydrogen and oxygen isotopic composition of minerals of magmatic and metamorphic rocks and fluid inclusions, the isotopic composition of groundwaters of modern volcanic regions, and the origin of the earth's hydrosphere in the light of isotopic, cosmochemical, and theoretical studies. Attention is also given to the separation of hydrogen and oxygen isotopes of waters in the underground cycle, the isotopic composition of the deep-formation waters of sedimentary basins, the relationship between surface and ground waters, and the groundwater residence time in an aquifer.

Isotopic Analysis of Fingernails as a USGS Open House Demonstration of the Use of Stable Isotopes in Foodweb Studies

NASA Astrophysics Data System (ADS)

Silva, S. R.; Kendall, C.; Young, M. B.; Choy, D.

2011-12-01

The USGS Isotope Tracers Project uses stable isotopes and tritium to add a unique dimension of chemical information to a wide range of environmental investigations. The use and application of isotopes is usually an unfamiliar and even esoteric topic to the general public. Therefore during three USGS open house events, as a public outreach effort, we demonstrated the use of stable isotopes by analyzing nitrogen and carbon isotopes from very small fragments of fingernail from willing participants. We titled the exhibit "You Are What You Eat". The results from all participants were plotted on a graph indicating the general influence of different food groups on the composition of body tissues as represented by fingernails. All participants were assigned a number and no personal-identification information was collected. A subset of participants provided us with an estimate of the number of days a week various foods were eaten and if they were vegetarians, vegans or non-vegetarians. Volunteers from our research group were on hand to explain and discuss fundamental concepts such as how foods attain their isotopic composition, the difference between C3 and C4 plants, the effects of assimilation, trophic enrichment, and the various uses of stable isotopes in environmental studies. The results of the fingernail analyses showed the variation of the range of isotopic compositions among about 400 people at each event, the distinct influence of C4 plants (mainly corn and cane sugar) on our carbon isotopic composition, and the isotopic differences between vegetarians and non vegetarians among other details (http://wwwrcamnl.wr.usgs.gov/isoig/projects/fingernails/). A poll of visitors attending the open house event in 2006 indicated that "You Are What You Eat" was among the most popular exhibits. Following the first two open house events we were contacted by a group of researchers from Brazil who had completed a very similar study. Our collaboration resulted in a publication in the American Journal of Physical Anthropology (Nardoto et al., 2006). This study found that despite global trends toward dietary homogenization, regional differences in food resources and dietary preferences were recorded in the carbon and nitrogen isotopic compositions of fingernails.

STABLE ISOTOPES IN ECOLOGICAL STUDIES: NEW DEVELOPMENTS IN MIXING MODELS (URUGUAY)

EPA Science Inventory

Stable isotopes are increasingly being used as tracers in ecological studies. One application uses isotopic ratios to quantify the proportional contributions of multiple sources to a mixture. Examples include pollution sources for air or water bodies, food sources for animals, ...

STABLE ISOTOPES IN ECOLOGICAL STUDIES: NEW DEVELOPMENTS IN MIXING MODELS (BRAZIL)

EPA Science Inventory

Stable isotopes are increasingly being used as tracers in ecological studies. One application uses isotopic ratios to quantify the proportional contributions of multiple sources to a mixture. Examples include pollution sources for air or water bodies, food sources for animals, ...

Concerns about Quadrupole ICP-MS Lead Isotopic Data and Interpretations in the Environment and Health Fields.

PubMed

Gulson, Brian; Kamenov, George D; Manton, William; Rabinowitz, Michael

2018-04-11

There has been a massive increase in recent years of the use of lead (Pb) isotopes in attempts to better understand sources and pathways of Pb in the environment and in man or experimental animals. Unfortunately, there have been many cases where the quality of the isotopic data, especially that obtained by quadrupole inductively coupled plasma mass spectrometry (Q-ICP-MS), are questionable, resulting in questionable identification of potential sources, which, in turn, impacts study interpretation and conclusions. We present several cases where the isotopic data have compromised interpretation because of the use of only the major isotopes 208 Pb/ 206 Pb and 207 Pb/ 206 Pb, or their graphing in other combinations. We also present some examples comparing high precision data from thermal ionization (TIMS) or multi-collector plasma mass spectrometry (MC-ICP-MS) to illustrate the deficiency in the Q-ICP-MS data. In addition, we present cases where Pb isotopic ratios measured on Q-ICP-MS are virtually impossible for terrestrial samples. We also evaluate the Pb isotopic data for rat studies, which had concluded that Pb isotopic fractionation occurs between different organs and suggest that this notion of biological fractionation of Pb as an explanation for isotopic differences is not valid. Overall, the brief review of these case studies shows that Q-ICP-MS as commonly practiced is not a suitable technique for precise and accurate Pb isotopic analysis in the environment and health fields.

Concerns about Quadrupole ICP-MS Lead Isotopic Data and Interpretations in the Environment and Health Fields

PubMed Central

Gulson, Brian; Manton, William; Rabinowitz, Michael

2018-01-01

There has been a massive increase in recent years of the use of lead (Pb) isotopes in attempts to better understand sources and pathways of Pb in the environment and in man or experimental animals. Unfortunately, there have been many cases where the quality of the isotopic data, especially that obtained by quadrupole inductively coupled plasma mass spectrometry (Q-ICP-MS), are questionable, resulting in questionable identification of potential sources, which, in turn, impacts study interpretation and conclusions. We present several cases where the isotopic data have compromised interpretation because of the use of only the major isotopes 208Pb/206Pb and 207Pb/206Pb, or their graphing in other combinations. We also present some examples comparing high precision data from thermal ionization (TIMS) or multi-collector plasma mass spectrometry (MC-ICP-MS) to illustrate the deficiency in the Q-ICP-MS data. In addition, we present cases where Pb isotopic ratios measured on Q-ICP-MS are virtually impossible for terrestrial samples. We also evaluate the Pb isotopic data for rat studies, which had concluded that Pb isotopic fractionation occurs between different organs and suggest that this notion of biological fractionation of Pb as an explanation for isotopic differences is not valid. Overall, the brief review of these case studies shows that Q-ICP-MS as commonly practiced is not a suitable technique for precise and accurate Pb isotopic analysis in the environment and health fields. PMID:29641487

What controls silicon isotope fractionation during dissolution of diatom opal?

NASA Astrophysics Data System (ADS)

Wetzel, F.; de Souza, G. F.; Reynolds, B. C.

2014-04-01

The silicon isotope composition of opal frustules from photosynthesising diatoms is a promising tool for studying past changes in the marine silicon cycle, and indirectly that of carbon. Dissolution of this opal may be accompanied by silicon isotope fractionation that could disturb the pristine silicon isotope composition of diatom opal acquired in the surface ocean. It has previously been shown that dissolution of fresh and sediment trap diatom opal in seawater does fractionate silicon isotopes. However, as the mechanism of silicon isotope fractionation remained elusive, it is uncertain whether opal dissolution in general is associated with silicon isotope fractionation considering that opal chemistry and surface properties are spatially and temporally (i.e. opal of different age) diverse. In this study we dissolved sediment core diatom opal in 5 mM NaOH and found that this process is not associated with significant silicon isotope fractionation. Since no variability of the isotope effect was observed over a wide range of dissolution rates, we can rule out the suggestion that back-reactions had a significant influence on the net isotope effect. Similarly, we did not observe an impact of temperature, specific surface area, or degree of undersaturation on silicon isotope partitioning during dissolution, such that these can most likely also be ruled out as controlling factors. We discuss the potential impacts of the chemical composition of the dissolution medium and age of diatom opal on silicon isotope fractionation during dissolution. It appears most likely that the controlling mechanism of silicon isotope fractionation during dissolution is related to the reactivity, or potentially, aluminium content of the opal. Such a dependency would imply that silicon isotope fractionation during dissolution of diatom opal is spatially and temporally variable. However, since the isotope effects during dissolution are small, the silicon isotope composition of diatom opal appears to be robust against dissolution in the deep sea sedimentary environment.

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

NASA Astrophysics Data System (ADS)

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.

Calcium Isotope Systematics During Development of the Domestic Chicken (Gallus gallus)

NASA Astrophysics Data System (ADS)

Wheatley, P. V.

2003-12-01

Calcium isotope distributions have been recognized as showing systematic and predictable fractionation in nature. However, most of the observed calcium isotope fractionation to date is due to biological processes. The presence of abundant amounts of calcium in mineralized tissues makes the isotopic system of calcium particularly valuable in biological and paleobiological questions involving biomineralization. In order to apply calcium isotope systematics to paleobiological questions the changes in the calcium isotope signatures of mineralized tissue in modern animals should be studied. My study observed the domestic chicken (Gallus gallus) through embryologic ontogeny. This was accomplished by obtaining fertilized eggs staged in a growth series from day 12 to day 20. The eggs were dissected and shell, embryonic bone, albumen, and yolk were analyzed in order to characterize the calcium isotopic composition of the individual components over the course of the growth series. Several systematic changes in the isotopic signatures of various tissues were observed during the course of the development of the embryos. In general, mineralization in biological systems preferentially partitions the lighter isotopes of calcium into hard parts. As a result of this fractionation during mineralization, partitioning of light isotopes of calcium into the mineralized tissues may result in residual tissues being enriched in the heavier isotopes as ontogeny progresses. Better understanding of the behavior of calcium in modern biological systems will improve its application to fossils and expand the number of paleobiological and evolutionary questions that can be addressed using calcium isotopic data.

Pyroxene Homogenization and the Isotopic Systematics of Eucrites

NASA Technical Reports Server (NTRS)

Nyquist, L. E.; Bogard, D. D.

1996-01-01

The original Mg-Fe zoning of eucritic pyroxenes has in nearly all cases been partly homogenized, an observation that has been combined with other petrographic and compositional criteria to establish a scale of thermal "metamorphism" for eucrites. To evaluate hypotheses explaining development of conditions on the HED parent body (Vesta?) leading to pyroxene homogenization against their chronological implications, it is necessary to know whether pyroxene metamorphism was recorded in the isotopic systems. However, identifying the effects of the thermal metamorphism with specific effects in the isotopic systems has been difficult, due in part to a lack of correlated isotopic and mineralogical studies of the same eucrites. Furthermore, isotopic studies often place high demands on analytical capabilities, resulting in slow growth of the isotopic database. Additionally, some isotopic systems would not respond in a direct and sensitive way to pyroxene homogenization. Nevertheless, sufficient data exist to generalize some observations, and to identify directions of potentially fruitful investigations.

Real-time airborne gamma-ray background estimation using NASVD with MLE and radiation transport for calibration

NASA Astrophysics Data System (ADS)

Kulisek, J. A.; Schweppe, J. E.; Stave, S. C.; Bernacki, B. E.; Jordan, D. V.; Stewart, T. N.; Seifert, C. E.; Kernan, W. J.

2015-06-01

Helicopter-mounted gamma-ray detectors can provide law enforcement officials the means to quickly and accurately detect, identify, and locate radiological threats over a wide geographical area. The ability to accurately distinguish radiological threat-generated gamma-ray signatures from background gamma radiation in real time is essential in order to realize this potential. This problem is non-trivial, especially in urban environments for which the background may change very rapidly during flight. This exacerbates the challenge of estimating background due to the poor counting statistics inherent in real-time airborne gamma-ray spectroscopy measurements. To address this challenge, we have developed a new technique for real-time estimation of background gamma radiation from aerial measurements without the need for human analyst intervention. The method can be calibrated using radiation transport simulations along with data from previous flights over areas for which the isotopic composition need not be known. Over the examined measured and simulated data sets, the method generated accurate background estimates even in the presence of a strong, 60Co source. The potential to track large and abrupt changes in background spectral shape and magnitude was demonstrated. The method can be implemented fairly easily in most modern computing languages and environments.

The MAJORANA DEMONSTRATOR for 0νββ: Current Status and Future Plans

NASA Astrophysics Data System (ADS)

Green, M. P.; Abgrall, N.; Aguayo, E.; Avignone, F. T.; Barabash, A. S.; Bertrand, F. E.; Boswell, M.; Brudanin, V.; Busch, M.; Byram, D.; Caldwell, A. S.; Chan, Y.-D.; Christofferson, C. D.; Combs, D. C.; Cuesta, C.; Detwiler, J. A.; Doe, P. J.; Efremenko, Yu.; Egorov, V.; Ejiri, H.; Elliott, S. R.; Fast, J. E.; Finnerty, P.; Fraenkle, F. M.; Galindo-Uribarri, A.; Giovanetti, G. K.; Goett, J.; Gruszko, J.; Guiseppe, V. E.; Gusev, K.; Hallin, A. L.; Hazama, R.; Hegai, A.; Henning, R.; Hoppe, E. W.; Howard, S.; Howe, M. A.; Keeter, K. J.; Kidd, M. F.; Kochetov, O.; Konovalov, S. I.; Kouzes, R. T.; LaFerriere, B. D.; Leon, J.; Leviner, L. E.; Loach, J. C.; MacMullin, J.; MacMullin, S.; Martin, R. D.; Meijer, S.; Mertens, S.; Nomachi, M.; Orrell, J. L.; O'Shaughnessy, C.; Overman, N. R.; Phillips, D. G.; Poon, A. W. P.; Pushkin, K.; Radford, D. C.; Rager, J.; Rielage, K.; Robertson, R. G. H.; Romero-Romero, E.; Ronquest, M. C.; Schubert, A. G.; Shanks, B.; Shima, T.; Shirchenko, M.; Snavely, K. J.; Snyder, N.; Suriano, A. M.; Thompson, J.; Timkin, V.; Tornow, W.; Trimble, J. E.; Varner, R. L.; Vasilyev, S.; Vetter, K.; Vorren, K.; White, B. R.; Wilkerson, J. F.; Wiseman, C.; Xu, W.; Yakushev, E.; Young, A. R.; Yu, C.-H.; Yumatov, V.

The MAJORANA DEMONSTRATOR will search for neutrinoless-double-beta decay (0νββ) in 76Ge, while establishing the feasibility of a future tonne-scale germanium-based 0νββ experiment, and performing searches for new physics beyond the Standard Model. The experiment, currently under construction at the Sanford Underground Research Facility in Lead, SD, will consist of a pair of modular high-purity germanium detector arrays housed inside of a compact copper, lead, and polyethylene shield. Through a combination of strict materials qualifications and assay, low-background design, and powerful background rejection techniques, the Demonstrator aims to achieve a background rate in the 0νββ region of interest (ROI) of no more than 3 counts in the 0νββ-decay ROI per tonne of target isotope per year (cnts/(ROI-t-y)). The current status of the Demonstrator is discussed, as are plans for its completion.

Resetting of Mg isotopes between calcite and dolomite during burial metamorphism: Outlook of Mg isotopes as geothermometer and seawater proxy

NASA Astrophysics Data System (ADS)

Hu, Zhongya; Hu, Wenxuan; Wang, Xiaomin; Lu, Yizhou; Wang, Lichao; Liao, Zhiwei; Li, Weiqiang

2017-07-01

Magnesium isotopes are an emerging tool to study the geological processes recorded in carbonates. Calcite, due to its ubiquitous occurrence and the large Mg isotope fractionation associated with the mineral, has attracted great interests in applications of Mg isotope geochemistry. However, the fidelity of Mg isotopes in geological records of carbonate minerals (e.g., calcite and dolomite) against burial metamorphism remains poorly constrained. Here we report our investigation on the Mg isotope systematics of a dolomitized Middle Triassic Geshan carbonate section in eastern China. Magnesium isotope analysis was complemented by analyses of Sr-C-O isotopic compositions, major and trace element concentrations, and petrographic and mineralogical features. Multiple lines of evidence consistently indicated that post-depositional diagenesis of carbonate minerals occurred to the carbonate rocks. Magnesium isotope compositions of the carbonate rocks closely follow a mixing trend between a high δ26Mg dolomite end member and a low δ26Mg calcite end member, irrespective of sample positions in the section and calcite/dolomite ratio in the samples. By fitting the measured Mg isotope data using a two-end member mixing model, an inter-mineral Δ26Mgdolomite-calcite fractionation of 0.72‰ was obtained. Based on the experimentally derived Mg isotope fractionation factors for dolomite and calcite, a temperature of 150-190 °C was calculated to correspond to the 0.72‰ Δ26Mgdolomite-calcite fractionation. Such temperature range matches with the burial-thermal history of the local strata, making a successful case of Mg isotope geothermometry. Our results indicate that both calcite and dolomite had been re-equilibrated during burial metamorphism, and based on isotope mass balance of Mg, the system was buffered by dolomite in the section. Therefore, burial metamorphism may reset Mg isotope signature of calcite, and Mg isotope compositions in calcite should be dealt with caution in studies of carbonate rocks with thermal history. By contrast, Mg isotopes of dolomite are less prone to post-depositional resetting due to a number of properties including high Mg abundance and high thermodynamic stability, and Mg isotopes in dolomite may be a more robust recorder for original carbonate precipitates.

Migratory orientation in a narrow avian hybrid zone

PubMed Central

Toews, David P.L.; Delmore, Kira E.; Osmond, Matthew M.; Taylor, Philip D.

2017-01-01

Background Zones of contact between closely related taxa with divergent migratory routes, termed migratory divides, have been suggested as areas where hybrid offspring may have intermediate and inferior migratory routes, resulting in low fitness of hybrids and thereby promoting speciation. In the Rocky Mountains of Canada there is a narrow hybrid zone between Audubon’s and myrtle warblers that is likely maintained by selection against hybrids. Band recoveries and isotopic studies indicate that this hybrid zone broadly corresponds to the location of a possible migratory divide, with Audubon’s warblers migrating south-southwest and myrtle warblers migrating southeast. We tested a key prediction of the migratory divide hypothesis: that genetic background would be predictive of migratory orientation among warblers in the center of the hybrid zone. Methods We recorded fall migratory orientation of wild-caught migrating warblers in the center of the hybrid zone as measured by video-based monitoring of migratory restlessness in circular orientation chambers. We then tested whether there was a relationship between migratory orientation and genetic background, as measured using a set of species-specific diagnostic genetic markers. Results We did not detect a significant association between orientation and genetic background. There was large variation among individuals in orientation direction. Mean orientation was towards the NE, surprising for birds on fall migration, but aligned with the mountain valley in which the study took place. Conclusions Only one other study has directly analyzed migratory orientation among naturally-produced hybrids in a migratory divide. While the other study showed an association between genetic background and orientation, we did not observe such an association in yellow-rumped warblers. We discuss possible reasons, including the possibility of a lack of a strong migratory divide in this hybrid zone and/or methodological limitations that may have prevented accurate measurements of long-distance migratory orientation. PMID:28439469

Oxygen and iron isotope studies of magnetite produced by magnetotactic bacteria

USGS Publications Warehouse

Mandernack, K.W.; Bazylinski, D.A.; Shanks, Wayne C.; Bullen, T.D.

1999-01-01

A series of carefully controlled laboratory studies was carried out to investigate oxygen and iron isotope fractionation during the intracellular production of magnetite (Fe3O4) by two different species of magnetotactic bacteria at temperatures between 4??and 35??C under microaerobic and anaerobic conditions. No detectable fractionation of iron isotopes in the bacterial magnetites was observed. However, oxygen isotope measurements indicated a temperature-dependent fractionation for Fe3O4 and water that is consistent with that observed for Fe3O4 produced extracellularly by thermophilic Fe3+-reducing bacteria. These results contrast with established fractionation curves estimated from either high-temperature experiments or theoretical calculations. With the fractionation curve established in this report, oxygen-18 isotope values of bacterial Fe3O4 may be useful in paleoenvironmental studies for determining the oxygen-18 isotope values of formation waters and for inferring paleotemperatures.

Realistic Fasting Does Not Affect Stable Isotope Levels of a Metabolically Efficient Salamander

EPA Science Inventory

Stable isotopes are commonly used to examine various aspects of animal ecology. The use of stable isotopes generally proceeds under the implicit assumption that resource use is the only factor driving variation in stable isotope levels; however, a wealth of studies demonstrate a...

Analysis of stable isotopes in fish to identify habitat use and switching

EPA Science Inventory

In our isotopic studies of fish in Oregon Coast Range streams we have found stable isotopes of carbon, oxygen and sulfur to be surprisingly useful in identifying and discriminating specific habitat or tributary use by a variety of fish species. Stable isotopes of carbon can be u...

Stable isotopes in fish as indicators of habitat use

EPA Science Inventory

In our isotopic studies of fish in Oregon Coast Range streams we have found stable isotopes of carbon, oxygen and sulfur to be surprisingly useful in identifying and discriminating specific habitat or tributary use by a variety of fish species. Stable isotopes of carbon can be u...

Stable isotopes of carbon and nitrogen in the study of avian and mammalian trophic ecology

Treesearch

Jeffrey F. Kelly

2000-01-01

Differential fractionation of stable isotopes of carbon during photosynthesis causes C4 plants and C3 plants to have distinct carbon-isotope signatures. In addition, marine C3 plants have stable-isotope ratios of carbon that are intermediate between C4 and terrestrial C3 plants. The direct incorporation of the carbon-isotope ratio (13C/12C) of plants into consumers...

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

PubMed Central

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

Origin of heavy Fe isotope compositions in high-silica igneous rocks: A rhyolite perspective

NASA Astrophysics Data System (ADS)

Du, De-Hong; Wang, Xiao-Lei; Yang, Tao; Chen, Xin; Li, Jun-Yong; Li, Weiqiang

2017-12-01

The origin of heavy Fe isotope compositions in high-silica (>70 wt% SiO2) igneous rocks remains a highly controversial topic. Considering that fluid exsolution in eruptive rocks is more straight-forward to constrain than in plutonic rocks, this study addresses the problem of Fe isotope fractionation in high-silica igneous rocks by measuring Fe isotope compositions of representative rhyolitic samples from the Neoproterozoic volcanic-sedimentary basins in southern China and the Triassic Tu Le Basin in northern Vietnam. The samples show remarkably varied δ56FeIRMM014 values ranging from 0.05 ± 0.05‰ to 0.55 ± 0.05‰, which is among the highest values reported from felsic rocks. The extensional tectonic setting and short melt residence time in magma chambers for the studied rhyolites rule out Soret diffusion and thermal migration processes as causes of the high δ56Fe values. Effects of volcanic degassing and fluid exsolution on bulk rock δ56Fe values for the rhyolites are also assessed using bulk rock geochemical indicators and Rayleigh fractionation models, and these processes are found to be insufficient to produce resolvable changes in Fe isotope compositions of the residual melt. The most probable mechanism accounting for heavy Fe isotope compositions in the high-silica rhyolites is narrowed down to fractional crystallization processes in the magma before rhyolite eruption. Removal of isotopically light Fe-bearing minerals (i.e. ulvöspinel-rich titanomagnetite, ilmenite and biotite) is proposed as the main cause of Fe isotope variation in silicic melts during magmatic evolution. This study implies that crystal fractionation is the dominant mechanism that controls Fe isotope fractionation in eruptive rocks and Fe isotopes could be used to study magmatic differentiation of high-silica magmas.

Assessing connectivity of estuarine fishes based on stable isotope ratio analysis

NASA Astrophysics Data System (ADS)

Herzka, Sharon Z.

2005-07-01

Assessing connectivity is fundamental to understanding the population dynamics of fishes. I propose that isotopic analyses can greatly contribute to studies of connectivity in estuarine fishes due to the high diversity of isotopic signatures found among estuarine habitats and the fact that variations in isotopic composition at the base of a food web are reflected in the tissues of consumers. Isotopic analysis can be used for identifying nursery habitats and estimating their contribution to adult populations. If movement to a new habitat is accompanied by a shift to foods of distinct isotopic composition, recent immigrants and residents can be distinguished based on their isotopic ratios. Movement patterns thus can be reconstructed based on information obtained from individuals. A key consideration is the rate of isotopic turnover, which determines the length of time that an immigrant to a given habitat will be distinguishable from a longtime resident. A literature survey indicated that few studies have measured turnover rates in fishes and that these have focused on larvae and juveniles. These studies reveal that biomass gain is the primary process driving turnover rates, while metabolic turnover is either minimal or undetectable. Using a simple dilution model and biomass-specific growth rates, I estimated that young fishes with fast growth rates will reflect the isotopic composition of a new diet within days or weeks. Older or slower-growing individuals may take years or never fully equilibrate. Future studies should evaluate the factors that influence turnover rates in fishes during various stages of the life cycle and in different tissues, as well as explore the potential for combining stable isotope and otolith microstructure analyses to examine the relationship between demographic parameters, movement and connectivity.

Tracing subducted crustal materials in the mantle by using magnesium isotopes

NASA Astrophysics Data System (ADS)

Teng, F. Z.

2016-12-01

Recent studies show that some continental basalt, mantle-metasomatised peridotite and cratonic eclogite have heterogeneous Mg isotopic compositions. These isotopically distinct Mg isotopic compositions have been explained by the incorporation of subducted materials in their mantle sources though the detailed mechanisms are still not well understood. In particular, how Mg-poor crustal materials can modify Mg isotopic systematics of Mg-rich mantle is unknown. Subduction zones are the most efficient sites for crust and mantle interactions, hence should be where the most prominent Mg isotopic variation occurs. However, to date, little is known on Mg isotope systematics in the subduction factory. Here I first review and report new Mg isotopic data for arc lava, subarc peridotite and the subducted slab (marine sediment, altered basalt and abyssal peridotite), then use them to constrain the origins of mantle Mg isotopic heterogeneity and lay the foundation for using Mg isotopes as new tools for tracing crust-mantle interactions. The main conclusions are 1) fluid-rock interactions can modify Mg isotopic systematics of abyssal peridotites; 2) island arc lavas have non-MORB Mg isotopic compositions, reflecting distinct surbarc mantle Mg isotopic signature; 3) continental arcs have non-MORB Mg isotopic compositions, likely resulting from crustal contamination and 4) the isotopically heterogeneous continental basalts are mainly produced by mixing of isotopically distinct magmas instead of being partial melting products of metasomatised mantle peridotites.

Speciation and preservation of CrVI and CrIII in finished drinking water matrices using collision cell ion chromatography-inductively coupled plasma-mass spectrometry

EPA Science Inventory

The polyatomic background at the major isotope of Cr was evaluated as a function of collision cell gas flow rate using three different mobile phases. The stability of CrVI was evaluated as a function of solution pH using an enriched 53CrVI. The recovery was ≥ 95% at pH 7.8 but...

Isotopic Dependence of GCR Fluence behind Shielding

NASA Technical Reports Server (NTRS)

Cucinotta, Francis A.; Wilson, John W.; Saganti, Premkumar; Kim, Myung-Hee Y.; Cleghorn, Timothy; Zeitlin, Cary; Tripathi, Ram K.

2006-01-01

In this paper we consider the effects of the isotopic composition of the primary galactic cosmic rays (GCR), nuclear fragmentation cross-sections, and isotopic-grid on the solution to transport models used for shielding studies. Satellite measurements are used to describe the isotopic composition of the GCR. For the nuclear interaction data-base and transport solution, we use the quantum multiple-scattering theory of nuclear fragmentation (QMSFRG) and high-charge and energy (HZETRN) transport code, respectively. The QMSFRG model is shown to accurately describe existing fragmentation data including proper description of the odd-even effects as function of the iso-spin dependence on the projectile nucleus. The principle finding of this study is that large errors (+/-100%) will occur in the mass-fluence spectra when comparing transport models that use a complete isotopic-grid (approx.170 ions) to ones that use a reduced isotopic-grid, for example the 59 ion-grid used in the HZETRN code in the past, however less significant errors (<+/-20%) occur in the elemental-fluence spectra. Because a complete isotopic-grid is readily handled on small computer workstations and is needed for several applications studying GCR propagation and scattering, it is recommended that they be used for future GCR studies.

Weathering and vegetation controls on nickel isotope fractionation in surface ultramafic environments (Albania)

NASA Astrophysics Data System (ADS)

Estrade, Nicolas; Cloquet, Christophe; Echevarria, Guillaume; Sterckeman, Thibault; Deng, Tenghaobo; Tang, YeTao; Morel, Jean-Louis

2015-08-01

The dissolved nickel (Ni) isotopic composition of rivers and oceans presents an apparent paradox. Even though rivers represent a major source of Ni in the oceans, seawater is more enriched in the heavier isotopes than river-water. Additional sources or processes must therefore be invoked to account for the isotopic budget of dissolved Ni in seawater. Weathering of continental rocks is thought to play a major role in determining the magnitude and sign of isotopic fractionation of metals between a rock and the dissolved product. We present a study of Ni isotopes in the rock-soil-plant systems of several ultramafic environments. The results reveal key insights into the magnitude and the control of isotopic fractionation during the weathering of continental ultramafic rocks. This study introduces new constraints on the influence of vegetation during the weathering process, which should be taken into account in interpretations of the variability of Ni isotopes in rivers. The study area is located in a temperate climate zone within the ophiolitic belt area of Albania. The serpentinized peridotites sampled present a narrow range of heavy Ni isotopic compositions (δ60Ni = 0.25 ± 0.16 ‰, 2SD n = 2). At two locations, horizons within two soil profiles affected by different degrees of weathering all presented light isotopic compositions compared to the parent rock (Δ60Nisoil-rock up to - 0.63 ‰). This suggests that the soil pool takes up the light isotopes, while the heavier isotopes remain in the dissolved phase. By combining elemental and mineralogical analyses with the isotope compositions determined for the soils, the extent of fractionation was found to be controlled by the secondary minerals formed in the soil. The types of vegetation growing on ultramafic-derived soils are highly adapted and include both Ni-hyperaccumulating species, which can accumulate several percent per weight of Ni, and non-accumulating species. Whole-plant isotopic compositions were found to be isotopically heavier than the soil (Δ60Niwhole plant-soil up to 0.40‰). Fractions of Ni extracted by DTPA (diethylenetriaminepentaacetic acid) presented isotopically heavy compositions compared to the soil (Δ60NiDTPA-soil up to 0.89‰), supporting the hypothesis that the dissolved Ni fraction controlled by weathering has a heavy isotope signature. The non-hyperaccumulators (n = 2) were inclined to take up and translocate light Ni isotopes with a large degree of fractionation (Δ60Nileaves-roots up to - 0.60 ‰). For Ni-hyperaccumulators (n = 7), significant isotopic fractionation was observed in the plants in their early growth stages, while no fractionation occurred during later growth stages, when plants are fully loaded with Ni. This suggests that (i) the high-efficiency translocation process involved in hyperaccumulators does not fractionate Ni isotopes, and (ii) the root uptake process mainly controls the isotopic composition of the plant. In ultramafic contexts, vegetation composed of hyperaccumulators can significantly influence isotopic compositions through its remobilization in the upper soil horizon, thereby influencing the isotopic balance of Ni exported to rivers.

Characterization of wines according the geographical origin by analysis of isotopes and minerals and the influence of harvest on the isotope values.

PubMed

Dutra, S V; Adami, L; Marcon, A R; Carnieli, G J; Roani, C A; Spinelli, F R; Leonardelli, S; Vanderlinde, R

2013-12-01

We studied Brazilian wines produced by microvinification from Cabernet Sauvignon and Merlot grapes, vintages 2007 and 2008, from the Serra Gaúcha, Campanha and Serra do Sudeste regions, in order to differentiate them according to geographical origin by using isotope and mineral element analyses. In addition, the influence of vintage production in isotope values was verified. Isotope analysis was performed by isotope ratio mass spectrometry (IRMS), and the determination of minerals was by flame atomic absorption (FAA). The best parameters to classify the wines in the 2008 vintage were Rb and Li. The results of the δ(13)C of wine ethanol, Rb and Li showed a significant difference between the varieties regardless of the region studied. The δ(18)O values of water and δ(13)C of ethanol showed significant differences, regardless of the variety. Discriminant analysis of isotope and minerals values allowed to classify approximately 80% of the wines from the three regions studied. Copyright © 2013 Elsevier Ltd. All rights reserved.

Stable isotope methodology in the pharmacokinetic studies of androgenic steroids in humans.

PubMed

Shinohara, Y; Baba, S

1990-04-01

The use of stable isotopically labeled steroids combined with gas chromatography/mass spectrometry (GC/MS) has found a broad application in pharmacologic studies. Initially, stable isotopically labeled steroids served as the ideal analytic internal standard for GC/MS analysis; however, their in vivo use has expanded and has proven to be a powerful pharmacokinetic tool. We have successfully used stable isotope methodology to study the pharmacokinetic/bioavailability of androgens. The primary advantage of the technique is that endogenous and exogenous steroids with the same basic structure can be differentiated by using stable isotopically labeled analogs. The method was used to examine the pharmacokinetics of testosterone and testosterone propionate, and to clarify the influence of endogenous testosterone. Another advantage of the isotope methods is that steroidal drugs can be administered concomitantly in two formulations (e.g., solution and solid dosage). A single set of blood samples serves to describe the time course of the formulations being compared. This stable isotope coadministration technique was used to estimate the relative bioavailability of 17 alpha-methyltestosterone.

A method for screening of plant species for space use

NASA Technical Reports Server (NTRS)

Goeschl, J. D.; Sauer, R. L.; Scheld, H. W.

1986-01-01

A cost-effective methodology which monitors numerous dynamic aspects of carbon assimilation and allocation kinetics in live, intact plants is discussed. Analogous methods can apply to nitrogen uptake and allocation. This methodology capitalizes on the special properties of the short-lived, positron-gamma emitting isotope C-11 especially when applied as CO2-11 in a special extended square wave (ESW) pattern. The 20.4 minute half-life allows for repeated or continuous experiments on the same plant over periods of minutes, hours, days, or weeks. The steady-state isotope equilibrium approached during the ESW experiments, and the parameters which can be analyzed by this technique are also direct results of that short half-life. Additionally, the paired .511 MeV gamma rays penetrate any amount of tissue and their 180 deg opposite orientation provides good collimation and allows coincidence counting which nearly eliminates background.

Geothermal data for 95 thermal and nonthermal waters of the Valles Caldera - southern Jemez Mountains region, New Mexico

DOE Office of Scientific and Technical Information (OSTI.GOV)

Goff, F.; McCormick, Trujillo, P.E. Jr.; Counce, D.

1982-05-01

Field, chemical, and isotopic data for 95 thermal and nonthermal waters of the southern Jemez Mountains, New Mexico are presented. This region includes all thermal and mineral waters associated with Valles Caldera and many of those located near the Nacimiento Uplift, near San Ysidro. Waters of the region can be categorized into five general types: (1) surface and near surface meteoric waters; (2) acid-sulfate waters (Valles Caldera); (3) thermal meteoric waters (Valles Caldera); (4) deep geothermal and derivative waters (Valles Caldera); and (5) mineralized waters near San Ysidro. Some waters display chemical and isotopic characteristics intermediate between the types listed.more » The object of the data is to help interpret geothermal potential of the Jemez Mountains region and to provide background data for investigating problems in hydrology, structural geology, hydrothermal alterations, and hydrothermal solution chemistry.« less

Commissioning of a new photon detection system for charge radii measurements of neutron-deficient Ca

NASA Astrophysics Data System (ADS)

Watkins, J.; Garand, D.; Miller, A. J.; Minamisono, K.; Everett, N.; Powel, R. C.; Maaß, B.; Nörtershäuser, W.; Kalman, C.; Lantis, J.; Kujawa, C.; Mantica, P.

2017-09-01

Calcium is unique for its possession of two stable isotopes of ``doubly magic'' nuclei at proton and neutron numbers (Z , N) = (20 , 20) and (20 , 28) . Recent charge radii measurements of neutron-rich calcium isotopes yielded an upward trend beyond current theoretical predictions. At the BECOLA facility at NSCL/MSU, Ca charge radii measurements will be extended to the neutron-deficient regime using collinear laser spectroscopy. A new photon detection system with an ellipsoidal reflector and a compound parabolic concentrator has been commissioned for the experiment. The system increases the signal-to-noise ratio by reducing background, which is critical for the low production rates of the Ca experiment. Details of the system and results of the characterization tests will be discussed. Work supported in part by NSF Grant PHY-15-65546, U.S. DOE Grant DE-NA0002924 and by the Deutsche Forschungsgemeinschaft Grant SFB 1245.

Bioaccumulation and enantiomeric profiling of organochlorine pesticides and persistent organic pollutants in the killer whale (Orcinus orca) from British and Irish waters.

PubMed

McHugh, Brendan; Law, Robin J; Allchin, Colin R; Rogan, Emer; Murphy, Sinead; Foley, M Barry; Glynn, Denise; McGovern, Evin

2007-11-01

Concentrations and enantiomeric profiles for a range of organochlorine compounds are reported in blubber samples from a number of individual killer whales (Orcinus orca) from British and Irish waters. Elevated contaminant levels and enriched isotopic ratios were determined in one individual whale sampled in the Scottish Western Isles compared to the others suggesting marine mammal based dietary influences. The potential application of isotopic ratios to model contaminant uptake, enantioselective enrichment and accumulation is demonstrated. Data are presented which provide information on enantioselective enrichment factors (EFs) for o,p'-DDT, alpha-HCH and toxaphene congeners CHB26 and CHB 50. This dataset further improves the current database on reported levels of a number of contaminants and provides additional background information on potential metabolic processes in killer whales from British and Irish waters.

Complementary stable carbon isotope ratio and amount of substance measurements in sports anti-doping.

PubMed

Cawley, Adam T; George, Adrian V

2012-12-01

The detection of steroids originating from synthetic precursors against a background of their chemically identical natural analogues has proven to be a significant challenge for doping control laboratories accredited by the World Anti-Doping Agency (WADA). The complementary application of gas chromatography-mass spectrometry (GC-MS) and gas chromatography-combustion-isotope ratio mass spectrometry (GC-C-IRMS) has been demonstrated to provide specific detection of endogenous steroid misuse for improved anti-doping analysis. Markers of synthetically derived steroids are reviewed on the basis of abnormal urinary excretions and low (13)C content. A combinatorial approach is presented for the interpretation of GC-MS and GC-C-IRMS data in the anti-doping context. This methodology can allow all relevant information concerning an individual's metabolism to be assessed in order to make an informed decision with respect to a doping violation. Copyright © 2012 John Wiley & Sons, Ltd.

Chromatographic separation of radioactive noble gases from xenon

NASA Astrophysics Data System (ADS)

Akerib, D. S.; Araújo, H. M.; Bai, X.; Bailey, A. J.; Balajthy, J.; Beltrame, P.; Bernard, E. P.; Bernstein, A.; Biesiadzinski, T. P.; Boulton, E. M.; Bramante, R.; Cahn, S. B.; Carmona-Benitez, M. C.; Chan, C.; Chiller, A. A.; Chiller, C.; Coffey, T.; Currie, A.; Cutter, J. E.; Davison, T. J. R.; Dobi, A.; Dobson, J. E. Y.; Druszkiewicz, E.; Edwards, B. N.; Faham, C. H.; Fiorucci, S.; Gaitskell, R. J.; Gehman, V. M.; Ghag, C.; Gibson, K. R.; Gilchriese, M. G. D.; Hall, C. R.; Hanhardt, M.; Haselschwardt, S. J.; Hertel, S. A.; Hogan, D. P.; Horn, M.; Huang, D. Q.; Ignarra, C. M.; Ihm, M.; Jacobsen, R. G.; Ji, W.; Kamdin, K.; Kazkaz, K.; Khaitan, D.; Knoche, R.; Larsen, N. A.; Lee, C.; Lenardo, B. G.; Lesko, K. T.; Lindote, A.; Lopes, M. I.; Manalaysay, A.; Mannino, R. L.; Marzioni, M. F.; McKinsey, D. N.; Mei, D.-M.; Mock, J.; Moongweluwan, M.; Morad, J. A.; Murphy, A. St. J.; Nehrkorn, C.; Nelson, H. N.; Neves, F.; O'Sullivan, K.; Oliver-Mallory, K. C.; Palladino, K. J.; Pease, E. K.; Pech, K.; Phelps, P.; Reichhart, L.; Rhyne, C.; Shaw, S.; Shutt, T. A.; Silva, C.; Solovov, V. N.; Sorensen, P.; Stephenson, S.; Sumner, T. J.; Szydagis, M.; Taylor, D. J.; Taylor, W.; Tennyson, B. P.; Terman, P. A.; Tiedt, D. R.; To, W. H.; Tripathi, M.; Tvrznikova, L.; Uvarov, S.; Verbus, J. R.; Webb, R. C.; White, J. T.; Whitis, T. J.; Witherell, M. S.; Wolfs, F. L. H.; Yazdani, K.; Young, S. K.; Zhang, C.

2018-01-01

The Large Underground Xenon (LUX) experiment operates at the Sanford Underground Research Facility to detect nuclear recoils from the hypothetical Weakly Interacting Massive Particles (WIMPs) on a liquid xenon target. Liquid xenon typically contains trace amounts of the noble radioactive isotopes 85Kr and 39Ar that are not removed by the in situ gas purification system. The decays of these isotopes at concentrations typical of research-grade xenon would be a dominant background for a WIMP search experiment. To remove these impurities from the liquid xenon, a chromatographic separation system based on adsorption on activated charcoal was built. 400 kg of xenon was processed, reducing the average concentration of krypton from 130 ppb to 3.5 ppt as measured by a cold-trap assisted mass spectroscopy system. A 50 kg batch spiked to 0.001 g/g of krypton was processed twice and reduced to an upper limit of 0.2 ppt.

Area G perimeter surface-soil and single-stage water sampling: Environmental surveillance for fiscal year 95. Progress report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Childs, M.; Conrad, R.

1997-09-01

ESH-19 personnel collected soil and single-stage water samples around the perimeter of Area G at Los Alamos National Laboratory (LANL) during FY 95 to characterize possible radionuclide movement out of Area G through surface water and entrained sediment runoff. Soil samples were analyzed for tritium, total uranium, isotopic plutonium, americium-241, and cesium-137. The single-stage water samples were analyzed for tritium and plutonium isotopes. All radiochemical data was compared with analogous samples collected during FY 93 and 94 and reported in LA-12986 and LA-13165-PR. Six surface soils were also submitted for metal analyses. These data were included with similar data generatedmore » for soil samples collected during FY 94 and compared with metals in background samples collected at the Area G expansion area.« less

Lead in ancient Rome’s city waters

PubMed Central

Delile, Hugo; Blichert-Toft, Janne; Goiran, Jean-Philippe; Keay, Simon; Albarède, Francis

2014-01-01

It is now universally accepted that utilization of lead for domestic purposes and water distribution presents a major health hazard. The ancient Roman world was unaware of these risks. How far the gigantic network of lead pipes used in ancient Rome compromised public health in the city is unknown. Lead isotopes in sediments from the harbor of Imperial Rome register the presence of a strong anthropogenic component during the beginning of the Common Era and the Early Middle Ages. They demonstrate that the lead pipes of the water distribution system increased Pb contents in drinking water of the capital city by up to two orders of magnitude over the natural background. The Pb isotope record shows that the discontinuities in the pollution of the Tiber by lead are intimately entwined with the major issues affecting Late Antique Rome and its water distribution system. PMID:24753588

Nitrogen Isotopic Anomalies in a Hydrous Interplanetary Dust Particle

NASA Technical Reports Server (NTRS)

Smith, J. B.; Dai, Z. R.; Weber, P. K.; Graham, G. A.; Hutcheon, I. D.; Bajt, S.; Ishii, H.; Bradley, J. P.

2005-01-01

Interplanetary dust particles (IDPs) collected in the stratosphere are the fine-grained end member (5 - 50 microns in size) of the meteoritic material available for investigation in the laboratory. IDPs are derived from either cometary or asteroidal sources. Some IDPs contain cosmically primitive materials with isotopic signatures reflecting presolar origins. Recent detailed studies using the NanoSIMS have shown there is a wide variation of isotopic signatures within individual IDPs; grains with a presolar signature have been observed surrounded by material with a solar isotopic composition. The majority of IDPs studied have been anhydrous. We report here results from integrated NanoSIMS/FIB/TEM/Synchrotron IR studies of a hydrous IDP, focused on understanding the correlations between the isotopic, mineralogical and chemical compositions of IDPs.

Stable Chlorine Isotope Study: Application to Early Solar System Materials

NASA Technical Reports Server (NTRS)

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 other [4], some authors have claimed that the 37Cl/35Cl ratio of geological samples obtained by TIMS technique are, in general, misleadingly too high and variable compared to those of IRMS [3]. For eample, 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]. In order to clarify the stable chlorine isotope features of early solar system materials, we have initiated development of the TIMS technique at NASA JSC applicable to analysis of small amounts of meteoritic and planetary materials. We report here the current status of chlorine isotope analysis at NASA JSC.

An experimental study of the isotopic enrichment in Ar, Kr, and Xe when trapped in water ice

NASA Technical Reports Server (NTRS)

Notesco, G.; Laufer, D.; Bar-Nun, A.; Owen, T.

1999-01-01

The isotopic enrichment of argon, krypton, and xenon, when trapped in water ice, was studied experimentally. The isotopes were found to be enriched according to their (m1/m2)1/2 ratio. These enrichment factors could be useful for comparison among the uncertain cosmic or solar isotopic ratios, the hopeful in situ cometary ratio, and those in Earth's atmosphere, in the context of cometary delivery of volatiles to Earth.

Stable water isotope patterns in a climate change hotspot: the isotope hydrology framework of Corsica (western Mediterranean).

PubMed

van Geldern, Robert; Kuhlemann, Joachim; Schiebel, Ralf; Taubald, Heinrich; Barth, Johannes A C

2014-06-01

The Mediterranean is regarded as a region of intense climate change. To better understand future climate change, this area has been the target of several palaeoclimate studies which also studied stable isotope proxies that are directly linked to the stable isotope composition of water, such as tree rings, tooth enamel or speleothems. For such work, it is also essential to establish an isotope hydrology framework of the region of interest. Surface waters from streams and lakes as well as groundwater from springs on the island of Corsica were sampled between 2003 and 2009 for their oxygen and hydrogen isotope compositions. Isotope values from lake waters were enriched in heavier isotopes and define a local evaporation line (LEL). On the other hand, stream and spring waters reflect the isotope composition of local precipitation in the catchment. The intersection of the LEL and the linear fit of the spring and stream waters reflect the mean isotope composition of the annual precipitation (δP) with values of-8.6(± 0.2) ‰ for δ(18)O and-58(± 2) ‰ for δ(2)H. This value is also a good indicator of the average isotope composition of the local groundwater in the island. Surface water samples reflect the altitude isotope effect with a value of-0.17(± 0.02) ‰ per 100 m elevation for oxygen isotopes. At Vizzavona Pass in central Corsica, water samples from two catchments within a lateral distance of only a few hundred metres showed unexpected but systematic differences in their stable isotope composition. At this specific location, the direction of exposure seems to be an important factor. The differences were likely caused by isotopic enrichment during recharge in warm weather conditions in south-exposed valley flanks compared to the opposite, north-exposed valley flanks.

Serum carbon and nitrogen stable isotopes as potential biomarkers of dietary intake and their relation with incident type 2 diabetes: the EPIC-Norfolk study123

PubMed Central

Patel, Pinal S; Cooper, Andrew JM; O'Connell, Tamsin C; Kuhnle, Gunter GC; Kneale, Catherine K; Mulligan, Angela M; Luben, Robert N; Brage, Soren; Khaw, Kay-Tee; Wareham, Nicholas J; Forouhi, Nita G

2014-01-01

Background: Stable-isotope ratios of carbon (13C/12C, expressed as δ13C) and nitrogen (15N/14N, or δ15N) have been proposed as potential nutritional biomarkers to distinguish between meat, fish, and plant-based foods. Objective: The objective was to investigate dietary correlates of δ13C and δ15N and examine the association of these biomarkers with incident type 2 diabetes in a prospective study. Design: Serum δ13C and δ15N (‰) were measured by using isotope ratio mass spectrometry in a case-cohort study (n = 476 diabetes cases; n = 718 subcohort) nested within the European Prospective Investigation into Cancer and Nutrition (EPIC)–Norfolk population-based cohort. We examined dietary (food-frequency questionnaire) correlates of δ13C and δ15N in the subcohort. HRs and 95% CIs were estimated by using Prentice-weighted Cox regression. Results: Mean (±SD) δ13C and δ15N were −22.8 ± 0.4‰ and 10.2 ± 0.4‰, respectively, and δ13C (r = 0.22) and δ15N (r = 0.20) were positively correlated (P < 0.001) with fish protein intake. Animal protein was not correlated with δ13C but was significantly correlated with δ15N (dairy protein: r = 0.11; meat protein: r = 0.09; terrestrial animal protein: r = 0.12, P ≤ 0.013). δ13C was inversely associated with diabetes in adjusted analyses (HR per tertile: 0.74; 95% CI: 0.65, 0.83; P-trend < 0.001], whereas δ15N was positively associated (HR: 1.23; 95% CI: 1.09, 1.38; P-trend = 0.001). Conclusions: The isotope ratios δ13C and δ15N may both serve as potential biomarkers of fish protein intake, whereas only δ15N may reflect broader animal-source protein intake in a European population. The inverse association of δ13C but a positive association of δ15N with incident diabetes should be interpreted in the light of knowledge of dietary intake and may assist in identifying dietary components that are associated with health risks and benefits. PMID:24990425

Revisiting streamside trees that do not use stream water: can the two water worlds hypothesis and snowpack isotopic effects explain a missing water source?: Riparian tree water sources

DOE PAGES

Bowling, David R.; Schulze, Emily S.; Hall, Steven J.

2016-10-14

We revisit a classic ecohydrological study that showed streamside riparian trees in a semiarid mountain catchment did not use perennial stream water. The original study suggested that mature individuals of Acer negundo, Acer grandidentatum, and other species were dependent on water from “deeper strata,” possibly groundwater. We used a dual stable isotope approach (δ 18O and δ 2H) to further examine the water sources of these trees. We tested the hypothesis that groundwater was the main tree water source, but found that neither groundwater nor stream water matched the isotope composition of xylem water during two growing seasons. Soil watermore » (0–1 m depth) was closest to and periodically overlapped with xylem water isotope composition, but overall, xylem water was isotopically enriched compared to all measured water sources. The “two water worlds” hypothesis postulates that soil water comprises isotopically distinct mobile and less mobile pools that do not mix, potentially explaining this disparity. We further hypothesized that isotopic effects during snowpack metamorphosis impart a distinct isotope signature to the less mobile soil water that supplies summer transpiration. Depth trends in water isotopes following snowmelt were consistent with the two water worlds hypothesis, but snow metamorphic isotope effects could not explain the highly enriched xylem water. Thus, the dual isotope approach did not unambiguously determine the water source(s) of these riparian trees. Further exploration of physical, geochemical, and biological mechanisms of water isotope fractionation and partitioning is necessary to resolve these data, highlighting critical challenges in the isotopic determination of plant water sources.« less

Revisiting streamside trees that do not use stream water: can the two water worlds hypothesis and snowpack isotopic effects explain a missing water source?: Riparian tree water sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bowling, David R.; Schulze, Emily S.; Hall, Steven J.

We revisit a classic ecohydrological study that showed streamside riparian trees in a semiarid mountain catchment did not use perennial stream water. The original study suggested that mature individuals of Acer negundo, Acer grandidentatum, and other species were dependent on water from “deeper strata,” possibly groundwater. We used a dual stable isotope approach (δ 18O and δ 2H) to further examine the water sources of these trees. We tested the hypothesis that groundwater was the main tree water source, but found that neither groundwater nor stream water matched the isotope composition of xylem water during two growing seasons. Soil watermore » (0–1 m depth) was closest to and periodically overlapped with xylem water isotope composition, but overall, xylem water was isotopically enriched compared to all measured water sources. The “two water worlds” hypothesis postulates that soil water comprises isotopically distinct mobile and less mobile pools that do not mix, potentially explaining this disparity. We further hypothesized that isotopic effects during snowpack metamorphosis impart a distinct isotope signature to the less mobile soil water that supplies summer transpiration. Depth trends in water isotopes following snowmelt were consistent with the two water worlds hypothesis, but snow metamorphic isotope effects could not explain the highly enriched xylem water. Thus, the dual isotope approach did not unambiguously determine the water source(s) of these riparian trees. Further exploration of physical, geochemical, and biological mechanisms of water isotope fractionation and partitioning is necessary to resolve these data, highlighting critical challenges in the isotopic determination of plant water sources.« less

Tracking natural and anthropogenic origins of dissolved arsenic during surface and groundwater interaction in a post-closure mining context: Isotopic constraints.

PubMed

Khaska, Mahmoud; Le Gal La Salle, Corinne; Verdoux, Patrick; Boutin, René

2015-01-01

Arsenic contamination of stream waters and groundwater is a real issue in Au-As mine environments. At the Salsigne Au-As mine, southern France, arsenic contamination persists after closure and remediation of the site. In this study, natural and anthropogenic arsenic inputs in surface water and groundwater are identified based on (87)Sr/(86)Sr, and δ(18)O and δ(2)H isotopic composition of water. In the wet season, downstream of the remediated zone, the arsenic contents in stream water and alluvial aquifer groundwater are high, with values in the order of 36 μg/L and 40 μg/L respectively, while upstream natural background average concentrations are around 4 μg/L. Locally down-gradient of the reclaimed area, arsenic concentrations in stream water showed 2 peaks, one during an important rainy event (101 mm) in the wet season in May, and a longer one over the dry period, reaching 120 and 110 μg/L respectively. The temporal variations in arsenic content in stream water can be explained i) during the dry season, by release of arsenic stored in the alluvial sediments through increased contribution from base flow and decreased stream flow and ii) during major rainy events, by mobilization of arsenic associated with important surface runoff. The (87)Sr/(86)Sr ratios associated with increasing arsenic content in stream waters downstream of the reclaimed area are significantly lower than that of the natural Sr inherited from Variscan formations. These low (87)Sr/(86)Sr ratios are likely to be associated with the decontaminating water treatment processes, used in the past and still at present, where CaO, produced from marine limestone and therefore showing a low (87)Sr/(86)Sr ratios, is used to precipitate Ca3(AsO4)2. The low Sr isotope signatures will then impact on the Sr isotope ratio of (1) the Ca-arsenate stored in tailing dams, (2) effluent currently produced by water treatment process and (3) groundwater draining from the overall site. Furthermore, Δ(2)H shows that the low (87)Sr/(86)Sr ratio, arsenic rich water is characterized by an evaporated signature suggesting a potential influence of water impacted by evaporation during storage in decantation lagoons. This study shows the suitability of Sr and stable isotopes of water as tracers to differentiate natural and anthropogenic sources of arsenic release or other trace elements from mining context where CaO is used for water treatment. Copyright © 2015 Elsevier B.V. All rights reserved.

Tracking natural and anthropogenic origins of dissolved arsenic during surface and groundwater interaction in a post-closure mining context: Isotopic constraints

NASA Astrophysics Data System (ADS)

Khaska, Mahmoud; Le Gal La Salle, Corinne; Verdoux, Patrick; Boutin, René

2015-06-01

Arsenic contamination of stream waters and groundwater is a real issue in Au-As mine environments. At the Salsigne Au-As mine, southern France, arsenic contamination persists after closure and remediation of the site. In this study, natural and anthropogenic arsenic inputs in surface water and groundwater are identified based on 87Sr/86Sr, and δ18O and δ2H isotopic composition of water. In the wet season, downstream of the remediated zone, the arsenic contents in stream water and alluvial aquifer groundwater are high, with values in the order of 36 μg/L and 40 μg/L respectively, while upstream natural background average concentrations are around 4 μg/L. Locally down-gradient of the reclaimed area, arsenic concentrations in stream water showed 2 peaks, one during an important rainy event (101 mm) in the wet season in May, and a longer one over the dry period, reaching 120 and 110 μg/L respectively. The temporal variations in arsenic content in stream water can be explained i) during the dry season, by release of arsenic stored in the alluvial sediments through increased contribution from base flow and decreased stream flow and ii) during major rainy events, by mobilization of arsenic associated with important surface runoff. The 87Sr/86Sr ratios associated with increasing arsenic content in stream waters downstream of the reclaimed area are significantly lower than that of the natural Sr inherited from Variscan formations. These low 87Sr/86Sr ratios are likely to be associated with the decontaminating water treatment processes, used in the past and still at present, where CaO, produced from marine limestone and therefore showing a low 87Sr/86Sr ratios, is used to precipitate Ca3(AsO4)2. The low Sr isotope signatures will then impact on the Sr isotope ratio of (1) the Ca-arsenate stored in tailing dams, (2) effluent currently produced by water treatment process and (3) groundwater draining from the overall site. Furthermore, Δ2H shows that the low 87Sr/86Sr ratio, arsenic rich water is characterized by an evaporated signature suggesting a potential influence of water impacted by evaporation during storage in decantation lagoons. This study shows the suitability of Sr and stable isotopes of water as tracers to differentiate natural and anthropogenic sources of arsenic release or other trace elements from mining context where CaO is used for water treatment.

Using semi-continuous, in-situ measurements of nitrous oxide isotopic composition at a suburban site to track emission processes

NASA Astrophysics Data System (ADS)

Harris, Eliza; Henne, Stephan; Christoph, Hüglin; Christoph, Zellweger; Béla, Tuzson; Erkan, Ibraim; Lukas, Emmenegger; Joachim, Mohn

2017-04-01

Nitrous oxide (N2O) is a potent greenhouse gas and the strongest ozone-destroying substance emitted this century. The atmospheric N2O mole fraction has been increasing at a rate of 0.2-0.3% per year over the past decades due to anthropogenic emissions; in addition, recent results suggest that the rate of increase is rising - therefore effective mitigation of N2O emissions is a critical point for environmental policy. However, N2O sources are poorly defined and disperse, complicating the development of targeted mitigation strategies. Online isotopic measurements using preconcentration and laser spectroscopy [1,2,3] have great potential to unravel spatial and temporal variations in sources, sinks and chemistry of trace gases such as N2O. Semi-continuous, real-time measurements of N2O isotopic composition (δ18O, site preference [SP = 14N15N16O - 15N14N16O] and δ15Nbulk) were performed at the suburban site of Dübendorf, Switzerland, for 19 months between July 2014 and February 2016. The data precision reached 0.1‰ in the final months, thus the results could clearly identify nocturnal build-up of N2O, with a corresponding decrease in δ18O, SP and δ15Nbulk due to isotopically depleted anthropogenic sources. Daily mean source isotopic composition was calculated by considering the measured and the background mole fraction and isotopic composition. Delta values of the mean emission source were highest in winter, with a seasonal cycle of 12, 8 and 5‰ for δ18O, SP and δ15Nbulk respectively. The chemical and meteorological parameters controlling source isotopic composition were considered using data from the Swiss National Air Pollution Monitoring Network (NABEL) as well as a transport regime cluster analysis. A clear spatial distribution for source isotopic composition was observed for δ18O, as well as a significant relationship with the level of urban pollution, indicating δ18O may be a strong indicator of combustion/industrial vs. agricultural N2O. In contrast, δ15Nbulk and particularly SP appear to vary too strongly in response to other factors affecting emission processes to provide a useful distinction between source categories on a regional scale - these isotopocules may however be useful to distinguish emission pathways on a local scale. For comparison, FLEXPART-COSMO transport simulations [4] were combined with emissions from the EDGAR inventory and estimates of source isotopic composition from literature, to simulate N2O isotopic composition at the sampling site. The model was able to capture variability in N2O mole fraction adequately (R2 = 0.34; p <<0.01). However, the measured variability in source isotopic composition was 1-2 orders of magnitude larger than simulated, illustrating that our knowledge of isotopic source signatures - in particular technical N2O sources - is still too limited to successfully model variations in ambient N2O isotopic composition. [1] Mohn et al. (2012) Atmospheric Measurement Techniques, doi:10.5194/amt-5-1601-2012 [2] Harris et al. (2014) Analytical Chemistry, doi: 10.1021/ac403606u. [3] Röckmann et al. (2016) Atmospheric Chemistry and Physics, doi:10.5194/acp-16-10469-2016. [4] Henne et al. (2016) Atmospheric Chemistry and Physics, doi:10.5194/acp-16-3683-2016.

A negative excursion at 14-16 Ma in seawater osmium isotope record: Implications for paleoceanographic studies using Fe-Mn crusts

NASA Astrophysics Data System (ADS)

Goto, K. T.; Tejada, M. L. G.; Suzuki, K.

2017-12-01

Osmium isotope stratigraphy is a recently proposed method to determine the depositional age of Fe-Mn crusts [1, 2]. Seawater Os isotope (187Os/188Os) is roughly determined by the balance of riverine Os inputs with radiogenic value (187Os/188Os = 1.4), and mantle-derived and extra-terrestrial Os inputs with non-radiogenic value (187Os/188Os = 0.12) [3]. Secular variation of global seawater Os isotope (seawater Os isotope curve) has been reconstructed by the analysis of pelagic sediments and exhibits large variations ranging from 0.2 to 1.0 with several negative excursions [3]. Hence, the depositional age of Fe-Mn crusts can be approximately estimated by fitting their Os isotope depth profiles to the seawater Os isotope curve (Osmium isotope stratigraphy). However, this method allows multiple interpretations which are partly due to the lack of high-resolution seawater Os isotope curve [1, 2]. For example, the available seawater Os isotope curve does not exhibit negative anomaly during the Miocene, which contrasts with Os isotope records of Fe-Mn crusts [4]. In the present study, we obtained a high-resolution Os isotope record of Miocene seawater using hemipelagic sediments from IODP Expedition 351 SiteU1438. We found a small negative Os isotope anomaly as low as 0.7 from sediments deposited at 14-16 Ma. The magnitude of this anomaly is similar to those reported from Fe-Mn crusts. Although the extrapolation of Be-10 ages for Fe-Mn crust indicate a younger age for the anomaly ( 11 Ma) [4], we could not find any discernable isotope anomaly at 11 Ma. Our finding is consistent with the timing of major eruption of the Columbia River flood basalts (CFRB) which could provide non-radiogenic Os to seawater at 14-16 Ma [5]. Hence, we suggest that the observed isotope anomaly reflect eruption and subsequent weathering of the CFRB. As the similar Os isotope anomaly is commonly found from Fe-Mn crusts, the Os isotope anomaly at 14-16 Ma could be used as a key event to constrain depositional ages of Fe-Mn crusts. In the presentation, we will also discuss the significance of our findings to paleoceanographic studies using Fe-Mn crusts. References: [1] Klemm et al., 2005 EPSL; [2] Nielsen et al., 2009 EPSL; [3] Peucker-Ehrenbrink & Ravizza, 2012 The Geologic Time Scale 2012; [4] Klemm et al., 2008 EPSL; [5] Hopper et al., 2002 GSA Bulletin

Nitrogen isotopic baselines and implications for estimating foraging habitat and trophic position of yellowfin tuna in the Indian and Pacific Oceans

NASA Astrophysics Data System (ADS)

Lorrain, Anne; Graham, Brittany S.; Popp, Brian N.; Allain, Valérie; Olson, Robert J.; Hunt, Brian P. V.; Potier, Michel; Fry, Brian; Galván-Magaña, Felipe; Menkes, Christophe E. R.; Kaehler, Sven; Ménard, Frédéric

2015-03-01

Assessment of isotopic compositions at the base of food webs is a prerequisite for using stable isotope analysis to assess foraging locations and trophic positions of marine organisms. Our study represents a unique application of stable-isotope analyses across multiple trophic levels (primary producer, primary consumer and tertiary consumer) and over a large spatial scale in two pelagic marine ecosystems. We found that δ15N values of particulate organic matter (POM), barnacles and phenylalanine from the muscle tissue of yellowfin tuna all showed similar spatial patterns. This consistency suggests that isotopic analysis of any of these can provide a reasonable proxy for isotopic variability at the base of the food web. Secondly, variations in the δ15N values of yellowfin tuna bulk-muscle tissues paralleled the spatial trends observed in all of these isotopic baseline proxies. Variation in isotopic composition at the base of the food web, rather than differences in tuna diet, explained the 11‰ variability observed in the bulk-tissue δ15N values of yellowfin tuna. Evaluating the trophic position of yellowfin tuna using amino-acid isotopic compositions across the western Indian and equatorial Pacific Oceans strongly suggests these tuna occupy similar trophic positions, albeit absolute trophic positions estimated by this method were lower than expected. This study reinforces the importance of considering isotopic baseline variability for diet studies, and provides new insights into methods that can be applied to generate nitrogen isoscapes for worldwide comparisons of top predators in marine ecosystems.

COMPOUND-SPECIFIC ISOTOPE ANALYSIS OF MTBE AND TBA FOR BIOREMEDIATION STUDIES

EPA Science Inventory

The utility of stable isotope ratios to detect biodegradation for a number of chemical compounds including MTBE and TBA has been demonstrated in a number of laboratory or field studies. Chemical reactions tend to favor molecules with the lighter isotopic species (e.g., 12C, 1H), ...

Isotopic incorporation rates for shark tissues from a long-term captive feeding study.

PubMed

Kim, Sora Lee; del Rio, Carlos Martínez; Casper, Dave; Koch, Paul L

2012-07-15

Stable isotope analysis has provided insight into the dietary and habitat patterns of many birds, mammals and teleost fish. A crucial biological parameter to interpret field stable isotope data is tissue incorporation rate, which has not been well studied in large ectotherms. We report the incorporation of carbon and nitrogen into the tissues of leopard sharks (Triakis semifasciata). Because sharks have relatively slow metabolic rates and are difficult to maintain in captivity, no long-term feeding study has been conducted until the point of isotopic steady state with a diet. We kept six leopard sharks in captivity for 1250 days, measured their growth, and serially sampled plasma, red blood cells and muscle for stable carbon and nitrogen isotope analysis. A single-compartment model with first-order kinetics adequately described the incorporation patterns of carbon and nitrogen isotopes for these three tissues. Both carbon and nitrogen were incorporated faster in plasma than in muscle and red blood cells. The rate of incorporation of carbon into muscle was similar to that predicted by an allometric equation relating isotopic incorporation rate to body mass that was developed previously for teleosts. In spite of their large size and unusual physiology, the rates of isotopic incorporation in sharks seem to follow the same patterns found in other aquatic ectotherms.

Studies on the optogalvanic effect and isotope-selective excitation of ytterbium in a hollow cathode discharge lamp using a pulsed dye laser.

PubMed

Kumar, Pankaj; Kumar, Jitendra; Prakash, Om; Saini, Vinod K; Dixit, Sudhir K; Nakhe, Shankar V

2013-09-01

This paper presents studies on the pulsed optogalvanic effect and isotope-selective excitation of Yb 555.648 nm (0 cm(-1) → 17 992.007 cm(-1)) and 581.067 nm (17 992.007 cm(-1) → 35 196.98 cm(-1)) transitions, in a Yb/Ne hollow cathode lamp. The Yb atoms were excited by narrow linewidth (500-1000 MHz) Rh110 and Rh6G dye based pulsed lasers. Optogalvanic signal inversion for ground state transition at 555.648 nm was observed beyond a hollow cathode discharge current of 8.5 mA, in contrast to normal optogalvanic signal at 581.067 nm up to maximum current of 14 mA. The isotope-selective excitation studies of Yb were carried out by recording Doppler limited optogalvanic signals as a function of dye laser wavelength. For the 581.067 nm transition, three even isotopes, (172)Yb, (174)Yb, and (176)Yb, and one odd isotope, (171)Yb, were clearly resolved. These data were compared with selective isotope excitation by 10 MHz linewidth continuous-wave dye laser. For 555.648 nm transition, isotopes were not clearly resolved, although isotope peaks of low modulation were observed.

Stable Isotope Signatures of Middle Palaeozoic Ahermatypic Rugose Corals - Deciphering Secondary Alteration, Vital Fractionation Effects, and Palaeoecological Implications.

PubMed

Jakubowicz, Michal; Berkowski, Blazej; López Correa, Matthias; Jarochowska, Emilia; Joachimski, Michael; Belka, Zdzislaw

2015-01-01

This study investigates stable isotope signatures of five species of Silurian and Devonian deep-water, ahermatypic rugose corals, providing new insights into isotopic fractionation effects exhibited by Palaeozoic rugosans, and possible role of diagenetic processes in modifying their original isotopic signals. To minimize the influence of intraskeletal cements on the observed signatures, the analysed specimens included unusual species either devoid of large intraskeletal open spaces ('button corals': Microcyclus, Palaeocyclus), or typified by particularly thick corallite walls (Calceola). The corals were collected at four localities in the Holy Cross Mountains (Poland), Mader Basin (Morocco) and on Gotland (Sweden), representing distinct diagenetic histories and different styles of diagenetic alteration. To evaluate the resistance of the corallites to diagenesis, we applied various microscopic and trace element preservation tests. Distinct differences between isotopic compositions of the least-altered and most-altered skeleton portions emphasise a critical role of material selection for geochemical studies of Palaeozoic corals. The least-altered parts of the specimens show marine or near-marine stable isotope signals and lack positive correlation between δ13C and δ18O. In terms of isotopic fractionation mechanisms, Palaeozoic rugosans must have differed considerably from modern deep-water scleractinians, typified by significant depletion in both 18O and 13C, and pronounced δ13C-δ18O co-variance. The fractionation effects exhibited by rugosans seem similar rather to the minor isotopic effects typical of modern non-scleractinian corals (octocorals and hydrocorals). The results of the present study add to growing evidence for significant differences between Scleractinia and Rugosa, and agree with recent studies indicating that calcification mechanisms developed independently in these two groups of cnidarians. Consequently, particular caution is needed in using scleractinians as analogues in isotopic studies of extinct coral lineages. Answering some of the pertinent palaeoecological questions, such as that of the possibility of photosymbiosis in Palaeozoic corals, may not be possible based on stable isotope data.

Do Hf isotopes in magmatic zircons represent those of their host rocks?

NASA Astrophysics Data System (ADS)

Wang, Di; Wang, Xiao-Lei; Cai, Yue; Goldstein, Steven L.; Yang, Tao

2018-04-01

Lu-Hf isotopic system in zircon is a powerful and widely used geochemical tracer in studying petrogenesis of magmatic rocks and crustal evolution, assuming that zircon Hf isotopes can represent initial Hf isotopes of their parental whole rock. However, this assumption may not always be valid. Disequilibrium partial melting of continental crust would preferentially melt out non-zircon minerals with high time-integrated Lu/Hf ratios and generate partial melts with Hf isotope compositions that are more radiogenic than those of its magma source. Dissolution experiments (with hotplate, bomb and sintering procedures) of zircon-bearing samples demonstrate this disequilibrium effect where partial dissolution yielded variable and more radiogenic Hf isotope compositions than fully dissolved samples. A case study from the Neoproterozoic Jiuling batholith in southern China shows that about half of the investigated samples show decoupled Hf isotopes between zircons and the bulk rocks. This decoupling could reflect complex and prolonged magmatic processes, such as crustal assimilation, magma mixing, and disequilibrium melting, which are consistent with the wide temperature spectrum from ∼630 °C to ∼900 °C by Ti-in-zircon thermometer. We suggest that magmatic zircons may only record the Hf isotopic composition of their surrounding melt during crystallization and it is uncertain whether their Hf isotopic compositions can represent the primary Hf isotopic compositions of the bulk magmas. In this regard, using zircon Hf isotopic compositions to trace crustal evolution may be biased since most of these could be originally from disequilibrium partial melts.

Calcium Isotopes in Foraminifera Shells: Evaluation for Paleo-temperature Reconstruction

NASA Astrophysics Data System (ADS)

Paytan, A.; Revello, C. A.; Bullen, T. D.

2002-12-01

The Ca stable isotope ratio of foraminifera shells has been suggested as a potential paleo-temperature proxy and has recently been applied in several studies to reconstruct glacial interglacial fluctuations in seawater temperatures. The major advantage of using Ca isotopes for paleo-temperature reconstruction is the relatively long residence time of Ca in the ocean. Thus, no spatial or temporal change in the Ca isotopic composition of seawater is expected over time scales much shorter than a million years. Moreover, since Ca is a major constituent of carbonate, and an isotopic ratio rather than an element concentration or element-element ratio (e.g. Mg/Ca, Sr/Ca) is measured, the Ca isotope proxy is much less likely to be affected by post depositional diagenetic alteration. However, preliminary results indicate that kinetic effects might largely control the Ca isotope fractionation involved in calcite shell formation. Before this new and exciting proxy can be utilized routinely, a better understanding of the parameters controlling Ca isotope fractionation in carbonate minerals in general and in foraminifera and other carbonate-secreting organisms is required. We have measured the Ca stable isotope ratio of several foraminifera species from core top sediments from two well-studied sites to determine the inter-species and within-species variability in Ca isotopes. We assess the effects of water temperature, calcification rate, and vital effects on the Ca stable isotope ratio of modern foraminifera and evaluate the potential of this proxy for paleo-temperature reconstruction.

Illuminating hydrological processes at the soil-vegetation-atmosphere interface with water stable isotopes

NASA Astrophysics Data System (ADS)

Sprenger, Matthias; Leistert, Hannes; Gimbel, Katharina; Weiler, Markus

2016-09-01

Water stable isotopes (18O and 2H) are widely used as ideal tracers to track water through the soil and to separate evaporation from transpiration. Due to the technical developments in the last two decades, soil water stable isotope data have become easier to collect. Thus, the application of isotope methods in soils is growing rapidly. Studies that make use of soil water stable isotopes often have a multidisciplinary character since an interplay of processes that take place in the vadose zone has to be considered. In this review, we provide an overview of the hydrological processes that alter the soil water stable isotopic composition and present studies utilizing pore water stable isotopes. The processes that are discussed include the water input as precipitation or throughfall, the output as evaporation, transpiration, or recharge, and specific flow and transport processes. Based on the review and supported by additional data and modeling results, we pose a different view on the recently proposed two water world hypothesis. As an alternative to two distinct pools of soil water, where one pool is enriched in heavy isotopes and used by the vegetation and the other pool does not undergo isotopic fractionation and becomes recharge, the water gets successively mixed with newly introduced rainwater during the percolation process. This way, water initially isotopically enriched in the topsoil loses the fractionation signal with increasing infiltration depth, leading to unfractionated isotopic signals in the groundwater.

U/Th series radionuclides as coastal groundwater tracers

USGS Publications Warehouse

Swarzenski, P.W.

2007-01-01

The study of coastal groundwater has recently surfaced as an active interdisciplinary area of research, driven foremost by its importance as a poorly quantified pathway for subsurface material transport into coastal ecosystems. Key issue in coastal groundwater research include a complete geochemical characterization of the groundwater(s); quantification of the kinetics of subsurface transport, including rock-water interactions; determination of groundwater ages; tracing of groundwater discharge into coastal waters using radiochemical fingerprints; and an assessment of the potential ecological impact of such subsurface flow to a reviving water body. For such applications, the isotopic systemics of select naturally occurring radionucludes in the U/Th series has proven to be particularly useful. These radionuclides (e.g., U, Th, Ram and Rn) are ubiquitous in all groundwaters ad are represented by several isotopes with widely different half-lives and chemistries (Figure 1). As a result, varied biogeochemical processes occurring over a broad range of time scales can be studied. In source rock, most U/Th series isotopes in secular equilibrium; that is, the rate of decay of a daughter isotope is equal to that of it radiogenic parent, and so will have equal activities (in this context, the specific activity is simply a measure of the amount of radioactivity per unit amount). In contrast, these nuclides exhibit strong fractionations within the surrounding groundwaters because of their respective physiochemical differences. Disequilibria in U/Th series radionuclides can thus be used to identify distinct water masses, quantify release rates from source rocks, assess groundwater migration rates, and assess groundwater discharge rates in coastal waters., Large isotopic variations also have the potential for providing precise fingerprints for groundwaters from specific aquifers and have been explored as a means for calculating groundwater ages and estuarine water mass transit times. The highly fractionated nature of U/Th series nuclides in groundwater is illustrated by the range in some measured activities. highest activities are typically observed for 222Rn, reflecting the inert nature of this noble gas. Groundwater 222Rn (t1/2=3.8) activities are thus controlled only by rapid in situ decay (Table 1) and production within host rocks, without the added complications of reversible removal via absorption or precipitation. Uranium, which is soluble as U(VI) in oxidizing waters, is present in intermediate activities in groundwaters that are moderated by redox-initiated removal onto aquifer rocks. The alkaline earth Ra and, to a greater extent, the less soluble actinide Th are readily removed from groundwater by water -- rock interactions and so are strongly depleted. Both of these elements have very short-lived as well as longer-lived isotopes, and so isotopes compositions reflect processes over a range of time scales. Many studies have evaluated and behavior of select radionuclides in groundwater and surface water systems. Recent advances in high-=precision mass spectrometry have opted new possibilities for more subtle interpretations in select long-lived U/Th series isotopes, such as U, Ra, Pa, and Th. However, these techniques have yet to be fully developed, ahns as a consequence, such data remain largely scarce and underutilized. Although many different approaches have been developed to study radionucluide behavior in groundwater, all are based on principles of radioactive production and decay and knowledge of source terms from weathering and recoil processes, as well as removal terms from the interaction with aquifer host rock surface by sorption and precipitation. This review is structured to present first a brief description of the background, driving forces, scales, and ecological significance of submarine groundwater discharge. Following this, a description of the geochemistry and behavior of select radionuclides in groundwater will be presented, and their application to tracing submarine groundwater discharge will be discussed.

Evaluation of the plasma hydrogen isotope content by residual gas analysis at JET and AUG

NASA Astrophysics Data System (ADS)

Drenik, A.; Alegre, D.; Brezinsek, S.; De Castro, A.; Kruezi, U.; Oberkofler, M.; Panjan, M.; Primc, G.; Reichbauer, T.; Resnik, M.; Rohde, V.; Seibt, M.; Schneider, P. A.; Wauters, T.; Zaplotnik, R.; ASDEX-Upgrade, the; EUROfusion MST1 Teams; contributors, JET

2017-12-01

The isotope content of the plasma reflects on the dynamics of isotope changeover experiments, efficiency of wall conditioning and the performance of a fusion device in the active phase of operation. The assessment of the isotope ratio of hydrogen and methane molecules is used as a novel method of assessing the plasma isotope ratios at JET and ASDEX-Upgrade (AUG). The isotope ratios of both molecules in general shows similar trends as the isotope ratio detected by other diagnostics. At JET, the absolute values of RGA signals are in relatively good agreement with each other and with spectroscopy data, while at AUG the deviation from neutral particle analyser data are larger, and the results show a consistent spatial distribution of the isotope ratio. It is further shown that the isotope ratio of the hydrogen molecule can be used to study the degree of dissociation of the injected gas during changeover experiments.

A latitudinal study of oxygen isotopes within horsehair

NASA Astrophysics Data System (ADS)

Thompson, E.; Bronk Ramsey, C.; McConnell, J. R.

2016-12-01

This study aims to explore the hypothesis that 'if oxygen isotope ratios deplete with decreasing temperature then a study of oxygen isotope ratios within horsehair from Oxfordshire to Iceland will show a latitudinal depletion gradient'. By looking at oxygen isotope values at different geographical positions, we can track the relationship with latitude and with different regional climate features. This will provide a firmer understanding of how to compare climate records from different locations. Additionally, a comparison of the horse breeds from this study to those analysed within previous studies will create an even better understanding of the intra-species variation within the δ18O values of horsehair. A total of 24 horses were sampled on the 7th March from Thordale Stud in Shetland, the Icelandic Food And Veterinary Authority in Iceland, the Exmoor Pony Centre in Exmoor and the Pigeon House Equestrian Centre in Oxfordshire. By starting the sampling process from the most recent growth at the follicle, the sampling date becomes a chronological marker, temporally fixing the first sample within a sequential set of data points extending for one year or longer, depending on the length of each individual hair. The samples were analysed for oxygen isotope values using an IRMS coupled within a Sercon HTEA. Preliminary results show a latitudinal gradient is evident on comparison between the locations, consistent with the findings of Darling and Talbot's study of fresh water isotopes in the British Isles (2003). These results support the hypothesis, showing that a study of oxygen isotope ratios within horse hair from Oxfordshire to Iceland showing a latitudinal depletion gradient, consistent with a depletion of oxygen isotope ratios due to decreasing temperatures. Darling, W. and Talbot, J. (2003). The O and H stable isotope composition of freshwaters in the British Isles. 1. Rainfall. Hydrol. Earth System Science, 7(2), pp.163-181.

Chemical purification of lanthanides for low-background experiments

NASA Astrophysics Data System (ADS)

Boiko, R. S.

2017-10-01

There are many potentially active isotopes among the lanthanide elements which are possible to use for low-background experiments to search for double β decay, dark matter, to investigate rare α and β decays. These kind of experiments require very low level of radioactive contamination, but commercially available compounds of lanthanides are always contamined by uranium, thorium, radium, potassium, etc. A simple chemical method based on liquid-liquid extraction has been applied for the purification of CeO2, Nd2O3 and Gd˙2O˙3 from radioactive traces. Detailed schemes of purification procedure are described. Measurements by using HPGe spectrometry demonstrate high efficiency in K, Ra, Th, U contaminations reduction on at least one order of magnitude.

Reaction rate for carbon burning in massive stars

DOE PAGES

Jiang, C. L.; Santiago-Gonzalez, D.; Almaraz-Calderon, S.; ...

2018-01-10

Carbon burning is a critical phase for nucleosynthesis in massive stars. The conditions for igniting this burning stage, and the subsequent isotope composition of the resulting ashes, depend strongly on the reaction rate for 12C+ 12C fusion at very low energies. Results for the cross sections for this reaction are influenced by various backgrounds encountered in measurements at such energies. In this paper, we report on a new measurement of 12C+ 12C fusion cross sections where these backgrounds have been minimized. In conclusion, it is found that the astrophysical S factor exhibits a maximum around E cm=3.5–4.0 MeV, which leadsmore » to a reduction of the previously predicted astrophysical reaction rate.« less

Neutrinoless double beta decay with 82SeF6 and direct ion imaging

NASA Astrophysics Data System (ADS)

Nygren, D. R.; Jones, B. J. P.; López-March, N.; Mei, Y.; Psihas, F.; Renner, J.

2018-03-01

We present a new neutrinoless double beta decay concept: the high pressure selenium hexafluoride gas time projection chamber. A promising new detection technique is outlined which combines techniques pioneered in high pressure xenon gas, such as topological discrimination, with the high Q-value afforded by the double beta decay isotope 82Se. The lack of free electrons in SeF6 mandates the use of an ion TPC. The microphysics of ion production and drift, which have many nuances, are explored. Background estimates are presented, suggesting that such a detector may achieve background indices of better than 1 count per ton per year in the region of interest at the 100 kg scale, and still better at the ton-scale.

Mass fractionation processes of transition metal isotopes

NASA Astrophysics Data System (ADS)

Zhu, X. K.; Guo, Y.; Williams, R. J. P.; O'Nions, R. K.; Matthews, A.; Belshaw, N. S.; Canters, G. W.; de Waal, E. C.; Weser, U.; Burgess, B. K.; Salvato, B.

2002-06-01

Recent advances in mass spectrometry make it possible to utilise isotope variations of transition metals to address some important issues in solar system and biological sciences. Realisation of the potential offered by these new isotope systems however requires an adequate understanding of the factors controlling their isotope fractionation. Here we show the results of a broadly based study on copper and iron isotope fractionation during various inorganic and biological processes. These results demonstrate that: (1) naturally occurring inorganic processes can fractionate Fe isotope to a detectable level even at temperature ˜1000°C, which challenges the previous view that Fe isotope variations in natural system are unique biosignatures; (2) multiple-step equilibrium processes at low temperatures may cause large mass fractionation of transition metal isotopes even when the fractionation per single step is small; (3) oxidation-reduction is an importation controlling factor of isotope fractionation of transition metal elements with multiple valences, which opens a wide range of applications of these new isotope systems, ranging from metal-silicate fractionation in the solar system to uptake pathways of these elements in biological systems; (4) organisms incorporate lighter isotopes of transition metals preferentially, and transition metal isotope fractionation occurs stepwise along their pathways within biological systems during their uptake.

Is it really organic?--multi-isotopic analysis as a tool to discriminate between organic and conventional plants.

PubMed

Laursen, K H; Mihailova, A; Kelly, S D; Epov, V N; Bérail, S; Schjoerring, J K; Donard, O F X; Larsen, E H; Pedentchouk, N; Marca-Bell, A D; Halekoh, U; Olesen, J E; Husted, S

2013-12-01

Novel procedures for analytical authentication of organic plant products are urgently needed. Here we present the first study encompassing stable isotopes of hydrogen, carbon, nitrogen, oxygen, magnesium and sulphur as well as compound-specific nitrogen and oxygen isotope analysis of nitrate for discrimination of organically and conventionally grown plants. The study was based on wheat, barley, faba bean and potato produced in rigorously controlled long-term field trials comprising 144 experimental plots. Nitrogen isotope analysis revealed the use of animal manure, but was unable to discriminate between plants that were fertilised with synthetic nitrogen fertilisers or green manures from atmospheric nitrogen fixing legumes. This limitation was bypassed using oxygen isotope analysis of nitrate in potato tubers, while hydrogen isotope analysis allowed complete discrimination of organic and conventional wheat and barley grains. It is concluded, that multi-isotopic analysis has the potential to disclose fraudulent substitutions of organic with conventionally cultivated plants. Copyright © 2013 Elsevier Ltd. All rights reserved.

Chapter 16Tracing Nitrogen Sources and Cycling in Catchments

USGS Publications Warehouse

Kendall, Carol

1998-01-01

This chapter focuses on the uses of isotopes to understand water chemistry.I Isotopic compositions generally cannot be interpreted successfully in the absence of other chemical and hydrologic data. The chapter focusses on uses of isotopes in tracing sources and cycling of nitrogen in the water-component of forested catchment, and on dissolved nitrate in shallow waters, nutrient uptake studies in agricultural areas, large-scale tracer experiments, groundwater contamination studies, food-web investigations, and uses of compound-specific stable isotope techniques. Shallow waters moving along a flowpath through a relatively uniform material and reacting with minerals probably do not achieve equilibrium but gradually approach some steady-state composition. The chapter also discusses the use of isotopic techniques to assess impacts of changes in land-management practices and land use on water quality. The analysis of individual molecular components for isotopic composition has much potential as a method for tracing the source, biogeochemistry, and degradation of organic liquids and gases because different materials have characteristic isotope spectrums or biomarkers.

[Research progress on food sources and food web structure of wetlands based on stable isotopes].

PubMed

Chen, Zhan Yan; Wu, Hai Tao; Wang, Yun Biao; Lyu, Xian Guo

2017-07-18

The trophic dynamics of wetland organisms is the basis of assessing wetland structure and function. Stable isotopes of carbon and nitrogen have been widely applied to identify trophic relationships in food source, food composition and food web transport in wetland ecosystem studies. This paper provided an overall review about the current methodology of isotope mixing model and trophic level in wetland ecosystems, and discussed the standards of trophic fractionation and baseline. Moreover, we characterized the typical food sources and isotopic compositions of wetland ecosystems, summarized the food sources in different trophic levels of herbivores, omnivores and carnivores based on stable isotopic analyses. We also discussed the limitations of stable isotopes in tra-cing food sources and in constructing food webs. Based on the current results, development trends and upcoming requirements, future studies should focus on sample treatment, conservation and trophic enrichment measurement in the wetland food web, as well as on combing a variety of methodologies including traditional stomach stuffing, molecular markers, and multiple isotopes.

Enzymatic Kinetic Isotope Effects from First-Principles Path Sampling Calculations.

PubMed

Varga, Matthew J; Schwartz, Steven D

2016-04-12

In this study, we develop and test a method to determine the rate of particle transfer and kinetic isotope effects in enzymatic reactions, specifically yeast alcohol dehydrogenase (YADH), from first-principles. Transition path sampling (TPS) and normal mode centroid dynamics (CMD) are used to simulate these enzymatic reactions without knowledge of their reaction coordinates and with the inclusion of quantum effects, such as zero-point energy and tunneling, on the transferring particle. Though previous studies have used TPS to calculate reaction rate constants in various model and real systems, it has not been applied to a system as large as YADH. The calculated primary H/D kinetic isotope effect agrees with previously reported experimental results, within experimental error. The kinetic isotope effects calculated with this method correspond to the kinetic isotope effect of the transfer event itself. The results reported here show that the kinetic isotope effects calculated from first-principles, purely for barrier passage, can be used to predict experimental kinetic isotope effects in enzymatic systems.

Isotope pattern deconvolution as a tool to study iron metabolism in plants.

PubMed

Rodríguez-Castrillón, José Angel; Moldovan, Mariella; García Alonso, J Ignacio; Lucena, Juan José; García-Tomé, Maria Luisa; Hernández-Apaolaza, Lourdes

2008-01-01

Isotope pattern deconvolution is a mathematical technique for isolating distinct isotope signatures from mixtures of natural abundance and enriched tracers. In iron metabolism studies measurement of all four isotopes of the element by high-resolution multicollector or collision cell ICP-MS allows the determination of the tracer/tracee ratio with simultaneous internal mass bias correction and lower uncertainties. This technique was applied here for the first time to study iron uptake by cucumber plants using 57Fe-enriched iron chelates of the o,o and o,p isomers of ethylenediaminedi(o-hydroxyphenylacetic) acid (EDDHA) and ethylenediamine tetraacetic acid (EDTA). Samples of root, stem, leaves, and xylem sap, after exposure of the cucumber plants to the mentioned 57Fe chelates, were collected, dried, and digested using nitric acid. The isotopic composition of iron in the samples was measured by ICP-MS using a high-resolution multicollector instrument. Mass bias correction was computed using both a natural abundance iron standard and by internal correction using isotope pattern deconvolution. It was observed that, for plants with low 57Fe enrichment, isotope pattern deconvolution provided lower tracer/tracee ratio uncertainties than the traditional method applying external mass bias correction. The total amount of the element in the plants was determined by isotope dilution analysis, using a collision cell quadrupole ICP-MS instrument, after addition of 57Fe or natural abundance Fe in a known amount which depended on the isotopic composition of the sample.

A Teaching Exercise to Introduce Stable Isotope Fractionation of Metals into Geochemistry Courses

ERIC Educational Resources Information Center

Weiss, Dominik J.; Harris, Caroline; Maher, Kate; Bullen, Thomas

2013-01-01

Variations in the isotopic composition of elements have been widely used to study earth's climate, biosphere, and interior, and more recently to track the fate of contaminants. Within the broad range of elements that exhibit measureable isotopic variations, metal stable isotopes are increasingly applied across the biological, geological,…

Isotope Cancer Treatment Research at LANL

ScienceCinema

Weidner, John; Nortier, Meiring

2018-02-13

Los Alamos National Laboratory has produced medical isotopes for diagnostic and imaging purposes for more than 30 years. Now LANL researchers have branched out into isotope cancer treatment studies. New results show that an accelerator-based approach can produce clinical trial quantities of actinium-225, an isotope that has promise as a way to kill tumors without damaging surrounding healthy cells.

Rate-dependent carbon and nitrogen kinetic isotope fractionation in hydrolysis of isoproturon.

PubMed

Penning, Holger; Cramer, Christopher J; Elsner, Martin

2008-11-01

Stable isotope fractionation permits quantifying contaminant degradation in the field when the transformation reaction is associated with a consistent isotope enrichment factor epsilon. When interpreted in conjunction with dual isotope plots, isotope fractionation is also particularly useful for elucidating reaction mechanisms. To assess the consistency of epsilon and dual isotope slopes in a two-step reaction, we investigated the abiotic hydrolysis of the herbicide isoproturon (3-(4-isopropylphenyl)-1,1-dimethylurea) using a fragmentation method that allows measuring isotope ratios in different parts of the molecule. Carbon and nitrogen position-specific isotope fractionation, as well as slopes in dual isotope plots, varied linearly with rate constants k(obs) depending on the presence of buffers that mediate the initial zwitterion formation. The correlation can be explained by two consecutive reaction steps (zwitterion formation followed by dimethylamine elimination) each of which has a different kinetic isotope effect and may be rate-limiting. Intrinsic isotope effects for both steps, extracted from our kinetic data using a novel theoretical treatment, agree well with values computed from density functional calculations. Our study therefore demonstrates that more variable isotope fractionation may be observed in simple chemical reactions than commonly thought, but that consistent epsilon or dual isotope slopes may nonetheless be encountered in certain molecular fragments.

Integration of stable carbon isotope, microbial community, dissolved hydrogen gas, and 2HH2O tracer data to assess bioaugmentation for chlorinated ethene degradation in fractured rocks

USGS Publications Warehouse

Révész, Kinga M.; Lollar, Barbara Sherwood; Kirshtein, Julie D.; Tiedeman, Claire; Imbrigiotta, Thomas E.; Goode, Daniel J.; Shapiro, Allen M.; Voytek, Mary A.; Lancombe, Pierre J.; Busenberg, Eurybiades

2014-01-01

An in situ bioaugmentation (BA) experiment was conducted to understand processes controlling microbial dechlorination of trichloroethene (TCE) in groundwater at the Naval Air Warfare Center (NAWC), West Trenton, NJ. In the BA experiment, an electron donor (emulsified vegetable oil and sodium lactate) and a chloro-respiring microbial consortium were injected into a well in fractured mudstone of Triassic age. Water enriched in 2H was also injected as a tracer of the BA solution, to monitor advective transport processes. The changes in concentration and the δ13C of TCE, cis-dichloroethene (cis-DCE), and vinyl chloride (VC); the δ2H of water; changes in the abundance of the microbial communities; and the concentration of dissolved H2 gas compared to pre- test conditions, provided multiple lines of evidence that enhanced biodegradation occurred in the injection well and in two downgradient wells. For those wells where the biodegradation was stimulated intensively, the sum of the molar chlorinated ethene (CE) concentrations in post-BA water was higher than that of the sum of the pre-BA background molar CE concentrations. The concentration ratios of TCE/(cis-DCE + VC) indicated that the increase in molar CE concentration may result from additional TCE mobilized from the rock matrix in response to the oil injection or due to desorption/diffusion. The stable carbon isotope mass-balance calculations show that the weighted average 13C isotope of the CEs was enriched for around a year compared to the background value in a two year monitoring period, an effective indication that dechlorination of VC was occurring. Insights gained from this study can be applied to efforts to use BA in other fractured rock systems. The study demonstrates that a BA approach can substantially enhance in situ bioremediation not only in fractures connected to the injection well, but also in the rock matrix around the well due to processes such as diffusion and desorption. Because the effect of the BA was intensive only in wells where an amendment was distributed during injection, it is necessary to adequately distribute the amendments throughout the fractured rock to achieve substantial bioremediation. The slowdown in BA effect after a year is due to some extend to the decrease abundant of appropriate microbes, but more likely the decreased concentration of electron donor.

Integration of stable carbon isotope, microbial community, dissolved hydrogen gas, and ²HH₂O tracer data to assess bioaugmentation for chlorinated ethene degradation in fractured rocks.

PubMed

Révész, Kinga M; Lollar, Barbara Sherwood; Kirshtein, Julie D; Tiedeman, Claire R; Imbrigiotta, Thomas E; Goode, Daniel J; Shapiro, Allen M; Voytek, Mary A; Lacombe, Pierre J; Busenberg, Eurybiades

2014-01-01

An in situ bioaugmentation (BA) experiment was conducted to understand processes controlling microbial dechlorination of trichloroethene (TCE) in groundwater at the Naval Air Warfare Center (NAWC), West Trenton, NJ. In the BA experiment, an electron donor (emulsified vegetable oil and sodium lactate) and a chloro-respiring microbial consortium were injected into a well in fractured mudstone of Triassic age. Water enriched in ²H was also injected as a tracer of the BA solution, to monitor advective transport processes. The changes in concentration and the δ¹³C of TCE, cis-dichloroethene (cis-DCE), and vinyl chloride (VC); the δ²H of water; changes in the abundance of the microbial communities; and the concentration of dissolved H₂ gas compared to pre- test conditions, provided multiple lines of evidence that enhanced biodegradation occurred in the injection well and in two downgradient wells. For those wells where the biodegradation was stimulated intensively, the sum of the molar chlorinated ethene (CE) concentrations in post-BA water was higher than that of the sum of the pre-BA background molar CE concentrations. The concentration ratios of TCE/(cis-DCE+VC) indicated that the increase in molar CE concentration may result from additional TCE mobilized from the rock matrix in response to the oil injection or due to desorption/diffusion. The stable carbon isotope mass-balance calculations show that the weighted average ¹³C isotope of the CEs was enriched for around a year compared to the background value in a two year monitoring period, an effective indication that dechlorination of VC was occurring. Insights gained from this study can be applied to efforts to use BA in other fractured rock systems. The study demonstrates that a BA approach can substantially enhance in situ bioremediation not only in fractures connected to the injection well, but also in the rock matrix around the well due to processes such as diffusion and desorption. Because the effect of the BA was intensive only in wells where an amendment was distributed during injection, it is necessary to adequately distribute the amendments throughout the fractured rock to achieve substantial bioremediation. The slowdown in BA effect after a year is due to some extend to the decrease abundant of appropriate microbes, but more likely the decreased concentration of electron donor. © 2013. Published by Elsevier B.V. All rights reserved.

Multiple sulfur isotopes fractionations associated with abiotic sulfur transformations in Yellowstone National Park geothermal springs

PubMed Central

2014-01-01

Background The paper presents a quantification of main (hydrogen sulfide and sulfate), as well as of intermediate sulfur species (zero-valent sulfur (ZVS), thiosulfate, sulfite, thiocyanate) in the Yellowstone National Park (YNP) hydrothermal springs and pools. We combined these measurements with the measurements of quadruple sulfur isotope composition of sulfate, hydrogen sulfide and zero-valent sulfur. The main goal of this research is to understand multiple sulfur isotope fractionation in the system, which is dominated by complex, mostly abiotic, sulfur cycling. Results Water samples from six springs and pools in the Yellowstone National Park were characterized by pH, chloride to sulfate ratios, sulfide and intermediate sulfur species concentrations. Concentrations of sulfate in pools indicate either oxidation of sulfide by mixing of deep parent water with shallow oxic water, or surface oxidation of sulfide with atmospheric oxygen. Thiosulfate concentrations are low (<6 μmol L-1) in the pools with low pH due to fast disproportionation of thiosulfate. In the pools with higher pH, the concentration of thiosulfate varies, depending on different geochemical pathways of thiosulfate formation. The δ34S values of sulfate in four systems were close to those calculated using a mixing line of the model based on dilution and boiling of a deep hot parent water body. In two pools δ34S values of sulfate varied significantly from the values calculated from this model. Sulfur isotope fractionation between ZVS and hydrogen sulfide was close to zero at pH < 4. At higher pH zero-valent sulfur is slightly heavier than hydrogen sulfide due to equilibration in the rhombic sulfur–polysulfide – hydrogen sulfide system. Triple sulfur isotope (32S, 33S, 34S) fractionation patterns in waters of hydrothermal pools are more consistent with redox processes involving intermediate sulfur species than with bacterial sulfate reduction. Small but resolved differences in ∆33S among species and between pools are observed. Conclusions The variation of sulfate isotopic composition, the origin of differences in isotopic composition of sulfide and zero–valent sulfur, as well as differences in ∆33S of sulfide and sulfate are likely due to a complex network of abiotic redox reactions, including disproportionation pathways. PMID:24959098

The Mantle Isotopic Array: A Tale of Two FOZOs

NASA Astrophysics Data System (ADS)

Apen, F. E.; Mukhopadhyay, S.; Williams, C. D.

2017-12-01

Oceanic basalts display isotopic arrays that suggest mixing between a depleted component, several enriched components, and a primitive component. The topology of the arrays provides information on mantle mixing, the distribution of heterogeneities, and information on mantle structure. Here we use a global compilation of mid-ocean ridge basalt (MORB) and ocean island basalt (OIB) He-Sr-Nd-Pb isotopic data to further analyze the topology of these arrays. Previous work indicated that OIB isotopic arrays converge to a common component [1-3] referred to as the focus zone, or FOZO. Our analyses suggest that while all OIBs do point to a common component with unradiogenic 4He/3He ratios relative to MORBs, this component has to be quite variable in its He, Sr, Nd and Pb isotopic compositions. FOZO cannot be a pure component but must represent a heterogeneous mixture of primitive and recycled material. Our analyses of the MORB and OIB isotopic compositions also indicate that while MORBs and OIBs sample the same components, the topology of their mixing arrays are quite distinct. Different MOR segments show quasi-linear isotopic arrays that all converge to a common component. This component is distinctive from the OIB FOZO being more depleted and more restrictive in its He, Sr, Nd and Pb composition. We suggest two common but distinguishable components are present in the mantle arrays: one common to MORBs and the other to OIBs, and we refer to them as MORB-FOZO and OIB-FOZO, respectively. We interpret the two FOZOs to represent the average composition of small-scale heterogeneities that make up the background matrix in the sources of MORBs and OIBs. The depleted and enriched components that are sampled in MORBs and OIBs reflect relatively large-scale heterogeneities distributed within the matrix, material that have yet to be deformed into the smaller length scales of the matrix material. Differences between the two FOZO compositions reflects the inclusion of a component with primitive He in OIBs along with differences in mixing timescales and mantle processing rates for MORBs and OIBs. The two distinct FOZO compositions must also indicate limited direct mixing between the two over Earth's 4.5 Gyr history. References: [1] Hart et al., Science 1992; [2] Farley et al., EPSL 1992; [3] Hanan and Graham, Science 1996.

Determination of the origin of dissolved inorganic carbon in groundwater around a reclaimed landfill in Otwock using stable carbon isotopes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Porowska, Dorota, E-mail: dorotap@uw.edu.pl

Highlights: • Research showed the origin of DIC in the groundwater around a reclaimed landfill. • Carbon isotope was used to evaluate the contributions of carbon from different sources. • The leachate-contaminated water was isotopically distinct from the natural groundwater. • DIC in the natural groundwater comes from organic matter and dissolution of carbonates. • In the contaminated water, DIC comes from organic matter in the aquifer and landfill. - Abstract: Chemical and isotopic analyses of groundwater from piezometers located around a reclaimed landfill in Otwock (Poland) were performed in order to trace the origin of dissolved inorganic carbon (DIC)more » in the groundwater. Due to differences in the isotopic composition of carbon from different sources, an analysis of stable carbon isotopes in the groundwater, together with the Keeling plot approach and a two-component mixing model allow us to evaluate the relative contributions of carbon from these sources in the groundwater. In the natural (background) groundwater, DIC concentrations and the isotopic composition of DIC (δ{sup 13}C{sub DIC}) comes from two sources: decomposition of organic matter and carbonate dissolution within the aquifer sediments, whereas in the leachate-contaminated groundwater, DIC concentrations and δ{sup 13}C{sub DIC} values depend on the degradation of organic matter within the aquifer sediments and biodegradation of organic matter stored in the landfill. From the mixing model, about 4–54% of the DIC pool is derived from organic matter degradation and 96–46% from carbonate dissolution in natural conditions. In the leachate-contaminated groundwater, about 20–53% of the DIC is derived from organic matter degradation of natural origin and 80–47% from biodegradation of organic matter stored in the landfill. Partial pressure of CO{sub 2} (P CO{sub 2}) was generally above the atmospheric, hence atmospheric CO{sub 2} as a source of carbon in DIC pool was negligible in the aquifer. P CO{sub 2} values in the aquifer in Otwock were always one to two orders of magnitude above the atmospheric P CO{sub 2}, and thus CO{sub 2} escaped directly into the vadose zone.« less

Long-term data set analysis of stable isotopic composition in German rivers

NASA Astrophysics Data System (ADS)

Reckerth, Anne; Stichler, Willibald; Schmidt, Axel; Stumpp, Christine

2017-09-01

Stable isotopes oxygen-18 (18O) and deuterium (2H) are commonly used to investigate hydrological processes in catchments. However, only a few isotope studies have been conducted on a large scale and rarely over long time periods. The objective of this study was to identify the spatial and seasonal variability of isotopic composition in river water and how it is affected by geographical and hydrological factors. The stable isotopic composition of river water has been measured in nine large river catchments in Germany for a time period of 12 years or 26 years. We conducted time series and correlation analyses to identify spatial and temporal patterns of the isotopic composition in the rivers. Further, we compared it to isotopic composition in local precipitation and catchments characteristics. In the majority of the rivers, the spatial and temporal patterns of precipitation were directly reflected in river water. The isotopic signals of the river water were time shifted and show attenuated amplitudes. Further deviations from isotopic compositions in local precipitation were observed in catchments with complex flow systems. These deviations were attributed to catchment processes and influences like evaporation, damming and storage. The seasonality of the isotopic composition was mainly determined by the discharge regimes of the rivers. We found correlations between isotopic long-term averages and catchment altitude as well as latitude and longitude, resulting in a northwest-southeast gradient. Furthermore, it was shown that long-term averages of d-excess were inversely related to flow length and catchment size, which indicates that evaporation enrichment has an impact on the isotopic composition even in catchments of humid climates. This study showed that isotopic composition in rivers can serve as a proxy for the local precipitation and can be utilized as an indicator for hydrological processes even in large river basins. In future, such long time series will help to also understand the impact of changes in the hydrological cycle on the larger scales. They can also be used for calibration and validation of flow and transport models at catchment and sub-catchment scale.

Growth of the European abalone ( Haliotis tuberculata L.) in situ: Seasonality and ageing using stable oxygen isotopes

NASA Astrophysics Data System (ADS)

Roussel, Sabine; Huchette, Sylvain; Clavier, Jacques; Chauvaud, Laurent

2011-02-01

The ormer, Haliotis tuberculata is the only European abalone species commercially exploited. The determination of growth and age in the wild is an important tool for fisheries and aquaculture management. However, the ageing technique used in the past in the field is unreliable. The stable oxygen isotope composition ( 18O/ 16O) of the shell depends on the temperature and oxygen isotope composition of the ambient sea water. The stable oxygen isotope technique, developed to study paleoclimatological changes in shellfish, was applied to three H. tuberculata specimens collected in north-west Brittany. For the specimens collected, the oxygen isotope ratios of the shell reflected the seasonal cycle in the temperature. From winter-to-winter cycles, estimates of the age and the annual growth increment, ranging from 13 to 55 mm per year were obtained. This study shows that stable oxygen isotopes can be a reliable tool for ageing and growth studies of this abalone species in the wild, and for validating other estimates.

Microbially Mediated Kinetic Sulfur Isotope Fractionation: Reactive Transport Modeling Benchmark

NASA Astrophysics Data System (ADS)

Wanner, C.; Druhan, J. L.; Cheng, Y.; Amos, R. T.; Steefel, C. I.; Ajo Franklin, J. B.

2014-12-01

Microbially mediated sulfate reduction is a ubiquitous process in many subsurface systems. Isotopic fractionation is characteristic of this anaerobic process, since sulfate reducing bacteria (SRB) favor the reduction of the lighter sulfate isotopologue (S32O42-) over the heavier isotopologue (S34O42-). Detection of isotopic shifts have been utilized as a proxy for the onset of sulfate reduction in subsurface systems such as oil reservoirs and aquifers undergoing uranium bioremediation. Reactive transport modeling (RTM) of kinetic sulfur isotope fractionation has been applied to field and laboratory studies. These RTM approaches employ different mathematical formulations in the representation of kinetic sulfur isotope fractionation. In order to test the various formulations, we propose a benchmark problem set for the simulation of kinetic sulfur isotope fractionation during microbially mediated sulfate reduction. The benchmark problem set is comprised of four problem levels and is based on a recent laboratory column experimental study of sulfur isotope fractionation. Pertinent processes impacting sulfur isotopic composition such as microbial sulfate reduction and dispersion are included in the problem set. To date, participating RTM codes are: CRUNCHTOPE, TOUGHREACT, MIN3P and THE GEOCHEMIST'S WORKBENCH. Preliminary results from various codes show reasonable agreement for the problem levels simulating sulfur isotope fractionation in 1D.

Do deposit-feeders compete? Isotopic niche analysis of an invasion in a species-poor system

PubMed Central

Karlson, Agnes M. L.; Gorokhova, Elena; Elmgren, Ragnar

2015-01-01

Successful establishment of invasive species is often related to the existence of vacant niches. Competition occurs when invaders use the same limiting resources as members of the recipient community, which will be reflected in some overlap of their trophic niches. The concept of isotopic niche has been used to study trophic niche partitioning among species. Here, we present a two-year field study comparing isotopic niches of the deposit-feeding community in a naturally species-poor system. The isotopic niche analyses showed no overlap between a recent polychaete invader and any of the native species suggesting that it has occupied a vacant niche. Its narrow isotopic niche suggests specialized feeding, however, the high δ15N values compared to natives are most likely due to isotope fractionation effects related to nitrogen recycling and a mismatch between biological stoichiometry of the polychaete and the sediment nitrogen content. Notably, highly overlapping isotopic niches were inferred for the native species, which is surprising in a food-limited system. Therefore, our results demonstrate that invaders may broaden the community trophic diversity and enhance resource utilization, but also raise questions about the congruence between trophic and isotopic niche concepts and call for careful examination of assumptions underlying isotopic niche interpretation. PMID:25988260

Isotopic niches support the resource breadth hypothesis

USGS Publications Warehouse

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.

Deciphering the iron isotope message of the human body

NASA Astrophysics Data System (ADS)

Walczyk, Thomas; von Blanckenburg, Friedhelm

2005-04-01

Mass-dependent variations in isotopic composition are known since decades for the light elements such as hydrogen, carbon or oxygen. Multicollector-inductively coupled plasma mass spectrometry (MC-ICP-MS) and double-spike thermal ionization mass spectrometry (TIMS) permit us now to resolve small variations in isotopic composition even for the heavier elements such as iron. Recent studies on the iron isotopic composition of human blood and dietary iron sources have shown that lighter iron isotopes are enriched along the food chain and that each individual bears a certain iron isotopic signature in blood. To make use of this finding in biomedical research, underlying mechanisms of isotope fractionation by the human body need to be understood. In this paper available iron isotope data for biological samples are discussed within the context of isotope fractionation concepts and fundamental aspects of human iron metabolism. This includes evaluation of new data for body tissues which show that blood and muscle tissue have a similar iron isotopic composition while heavier iron isotopes are concentrated in the liver. This new observation is in agreement with our earlier hypothesis of a preferential absorption of lighter iron isotopes by the human body. Possible mechanisms for inducing an iron isotope effect at the cellular and molecular level during iron uptake are presented and the potential of iron isotope effects in human blood as a long-term measure of dietary iron absorption is discussed.

Final report of the key comparison CCQM-K98: Pb isotope amount ratios in bronze

NASA Astrophysics Data System (ADS)

Vogl, Jochen; Yim, Yong-Hyeon; Lee, Kyoung-Seok; Goenaga-Infante, Heidi; Malinowskiy, Dmitriy; Ren, Tongxiang; Wang, Jun; Vocke, Robert D., Jr.; Murphy, Karen; Nonose, Naoko; Rienitz, Olaf; Noordmann, Janine; Näykki, Teemu; Sara-Aho, Timo; Ari, Betül; Cankur, Oktay

2014-01-01

Isotope amount ratios are proving useful in an ever increasing array of applications that range from studies unravelling transport processes, to pinpointing the provenance of specific samples as well as trace element quantification by using isotope dilution mass spectrometry (IDMS). These expanding applications encompass fields as diverse as archaeology, food chemistry, forensic science, geochemistry, medicine and metrology. However, to be effective tools, the isotope ratio data must be reliable and traceable to enable the comparability of measurement results. The importance of traceability and comparability in isotope ratio analysis has already been recognized by the Inorganic Analysis Working Group (IAWG) within the CCQM. While the requirements for isotope ratio accuracy and precision in the case of IDMS are generally quite modest, 'absolute' Pb isotope ratio measurements for geochemical applications as well as forensic provenance studies require Pb isotope ratio measurements of the highest quality. To support present and future CMCs on isotope ratio determinations, a key comparison was urgently needed and therefore initiated at the IAWG meeting in Paris in April 2011. The analytical task within such a comparison was decided to be the measurement of Pb isotope amount ratios in water and bronze. Measuring Pb isotope amount ratios in an aqueous Pb solution tested the ability of analysts to correct for any instrumental effects on the measured ratios, while the measurement of Pb isotope amount ratios in a metal matrix sample provided a real world test of the whole chemical and instrumental procedure. A suitable bronze material with a Pb mass fraction between 10 and 100 mg•kg-1 and a high purity solution of Pb with a mass fraction of approximately 100 mg•kg-1 was available at the pilot laboratory (BAM), both offering a natural-like Pb isotopic composition. The mandatory measurands, the isotope amount ratios n(206Pb)/n(204Pb), n(207Pb)/n(204Pb) and n(208Pb)/n(204Pb) were selected such that they correspond with those commonly reported in Pb isotopic studies and fully describe the isotopic composition of Pb in the sample. Additionally, the isotope amount ratio n(208Pb)/n(206Pb) was added, as this isotope ratio is typically measured when performing Pb quantitation by IDMS involving a 206Pb spike. Each participant was free to use any method they deemed suitable for measuring the individual isotope ratios. However, the majority of the results were obtained by using muIti-collector ICPMS or TIMS. The key requirements for all analytical procedures were a traceability statement for all results and the establishment of an uncertainty budget meeting a target uncertainty for all ratios of 0.2 %, relative (k=1). Additionally, the use of a Pb-matrix separation procedure was encouraged. The obtained overall result was excellent, demonstrating that the individual results reported by the NMIs/DIs were comparable and compatible for the determination of Pb isotope ratios. MC-ICPMS and MC-TIMS data were consistent with each other and agree to within 0.05 %. The corresponding uncertainties can be considered as realistic uncertainties and mainly range from 0.02 % to 0.08 % (k=1). As stated above isotope ratios are being increasingly used in different fields. Despite the availability and ease of use of new mass spectrometers, the metrology of unbiased isotope ratio measurements remains very challenging. Therefore, further comparisons are urgently needed, and should be designed to also engage scientists outside the NMI/DI community. Possible follow-up studies should focus on isotope ratio and delta measurements important for environmental and technical applications (e.g. B), food traceability and forensics (e.g. H, C, N, O, S and 87Sr/86Sr) or climate change issues (e.g. Li, B, Mg, Ca, Si). Main text. To reach the main text of this paper, click on Final Report. The final report has been peer-reviewed and approved for publication by the CCQM.

Spatial and Temporal Trends in Stable Carbon and Oxygen Isotope Ratios of Juvenile Winter Flounder

EPA Science Inventory

Isotopic ratios of fish otoliths have been used in numerous studies as natural tags or markers to aid the study of connectivity among fish populations. We investigated the use of spatial and temporal changes in the stable carbon and oxygen isotope ratios of otoliths to different...

MAST - A mass spectrometer telescope for studies of the isotopic composition of solar, anomalous, and galactic cosmic ray nuclei

NASA Technical Reports Server (NTRS)

Cook, Walter R.; Cummings, Alan C.; Cummings, Jay R.; Garrard, Thomas L.; Kecman, Branislav; Mewaldt, Richard A.; Selesnick, Richard S.; Stone, Edward C.; Von Rosenvinge, T. T.

1993-01-01

The Mass Spectrometer Telescope (MAST) on SAMPEX is designed to provide high resolution measurements of the isotopic composition of energetic nuclei from He to Ni (Z = 2 to 28) over the energy range from about 10 to several hundred MeV/nuc. During large solar flares MAST will measure the isotopic abundances of solar energetic particles to determine directly the composition of the solar corona, while during solar quiet times MAST will study the isotopic composition of galactic cosmic rays. In addition, MAST will measure the isotopic composition of both interplanetary and trapped fluxes of anomalous cosmic rays, believed to be a sample of the nearby interstellar medium.

Isotope effects on desorption kinetics of hydrogen isotopes implanted into stainless steel by glow discharge

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matsuyama, M.; Kondo, M.; Noda, N.

2015-03-15

In a fusion device the control of fuel particles implies to know the desorption rate of hydrogen isotopes by the plasma-facing materials. In this paper desorption kinetics of hydrogen isotopes implanted into type 316L stainless steel by glow discharge have been studied by experiment and numerical calculation. The temperature of a maximum desorption rate depends on glow discharge time and heating rate. Desorption spectra observed under various experimental conditions have been successfully reproduced by numerical simulations that are based on a diffusion-limited process. It is suggested, therefore, that desorption rate of a hydrogen isotope implanted into the stainless steel ismore » limited by a diffusion process of hydrogen isotope atoms in bulk. Furthermore, small isotope effects were observed for the diffusion process of hydrogen isotope atoms. (authors)« less

Wide Area Recovery and Resiliency Program (WARRP) Integrated Program Plan

DTIC Science & Technology

2011-06-01

Agent YELLOW, which is a mixture of the chemical warfare agents Sulfur Mustard and Lewisite, is a liquid with a garlic-like odor. Sulfur mustard...Radioisotope Background Cesium -137 (137Cs) is a radioactive isotope of cesium . The half-life of cesium -137 is 30.17 years. Because of the chemical...nature of cesium , it moves easily through the environment. This makes the cleanup of cesium - 137 difficult. People may ingest cesium -137 with food

Intracellular Cadmium Isotope Fractionation

NASA Astrophysics Data System (ADS)

Horner, T. J.; Lee, R. B.; Henderson, G. M.; Rickaby, R. E.

2011-12-01

Recent stable isotope studies into the biological utilization of transition metals (e.g. Cu, Fe, Zn, Cd) suggest several stepwise cellular processes can fractionate isotopes in both culture and nature. However, the determination of fractionation factors is often unsatisfactory, as significant variability can exist - even between different organisms with the same cellular functions. Thus, it has not been possible to adequately understand the source and mechanisms of metal isotopic fractionation. In order to address this problem, we investigated the biological fractionation of Cd isotopes within genetically-modified bacteria (E. coli). There is currently only one known biological use or requirement of Cd, a Cd/Zn carbonic anhydrase (CdCA, from the marine diatom T. weissfloggii), which we introduce into the E. coli genome. We have also developed a cleaning procedure that allows for the treating of bacteria so as to study the isotopic composition of different cellular components. We find that whole cells always exhibit a preference for uptake of the lighter isotopes of Cd. Notably, whole cells appear to have a similar Cd isotopic composition regardless of the expression of CdCA within the E. coli. However, isotopic fractionation can occur within the genetically modified E. coli during Cd use, such that Cd bound in CdCA can display a distinct isotopic composition compared to the cell as a whole. Thus, the externally observed fractionation is independent of the internal uses of Cd, with the largest Cd isotope fractionation occurring during cross-membrane transport. A general implication of these experiments is that trace metal isotopic fractionation most likely reflects metal transport into biological cells (either actively or passively), rather than relating to expression of specific physiological function and genetic expression of different metalloenzymes.

Utility of stable isotope analysis in studying foraging ecology of herbivores: Examples from moose and caribou

USGS Publications Warehouse

Ben-David, Merav; Shochat, Einav; Adams, Layne G.

2001-01-01

Recently, researchers emphasized that patterns of stable isotope ratios observed at the individual level are a result of an interaction between ecological, physiological, and biochemical processes. Isotopic models for herbivores provide additional complications because those mammals consume foods that have high variability in nitrogen concentrations. In addition, distribution of amino acids in plants may differ greatly from that required by a herbivore. At northern latitudes, where the growing season of vegetation is short, isotope ratios in herbivore tissues are expected to differ between seasons. Summer ratios likely reflect diet composition, whereas winter ratios would reflect diet and nutrient recycling by the animals. We tested this hypothesis using data collected from blood samples of caribou (Rangifer tarandus) and moose (Alces alces) in Denali National Park and Preserve, Alaska, USA. Stable isotope ratios of moose and caribou were significantly different from each other in late summer-autumn and winter. Also, late summer-autumn and winter ratios differed significantly between seasons in both species. Nonetheless, we were unable to evaluate whether differences in seasonal isotopic ratios were a result of diet selection or a response to nutrient recycling. We believe that additional studies on plant isotopic ratios as related to ecological factors in conjunction with investigations of diet selection by the herbivores will enhance our understanding of those interactions. Also, controlled studies investigating the relation between diet and physiological responses in herbivores will increase the utility of isotopic analysis in studying foraging ecology of herbivores.

Calcium Isotope Analysis by Mass Spectrometry

NASA Astrophysics Data System (ADS)

Boulyga, S.; Richter, S.

2010-12-01

The variations in the isotopic composition of calcium caused by fractionation in heterogeneous systems and by nuclear reactions can provide insight into numerous biological, geological, and cosmic processes, and therefore isotopic analysis finds a wide spectrum of applications in cosmo- and geochemistry, paleoclimatic, nutritional, and biomedical studies. The measurement of calcium isotopic abundances in natural samples has challenged the analysts for more than three decades. Practically all Ca isotopes suffer from significant isobaric interferences, whereas low-abundant isotopes can be particularly affected by neighboring major isotopes. The extent of natural variations of stable isotopes appears to be relatively limited, and highly precise techniques are required to resolve isotopic effects. Isotope fractionation during sample preparation and measurements and instrumental mass bias can significantly exceed small isotope abundance variations in samples, which have to be investigated. Not surprisingly, a TIMS procedure developed by Russell et al. (Russell et al., 1978. Geochim Cosmochim Acta 42: 1075-1090) for Ca isotope measurements was considered as revolutionary for isotopic measurements in general, and that approach is used nowadays (with small modifications) for practically all isotopic systems and with different mass spectrometric techniques. Nevertheless, despite several decades of calcium research and corresponding development of mass spectrometers, the available precision and accuracy is still not always sufficient to achieve the challenging goals. This presentation discusses figures of merits of presently used analytical methods and instrumentation, and attempts to critically assess their limitations. Additionally, the availability of Ca isotope reference materials will be discussed.

"Wave" signal-smoothing and mercury-removing device for laser ablation quadrupole and multiple collector ICPMS analysis: application to lead isotope analysis.

PubMed

Hu, Zhaochu; Zhang, Wen; Liu, Yongsheng; Gao, Shan; Li, Ming; Zong, Keqing; Chen, Haihong; Hu, Shenghong

2015-01-20

A novel "wave" signal-smoothing and mercury-removing device has been developed for laser ablation quadrupole and multiple collector ICPMS analysis. With the wave stabilizer that has been developed, the signal stability was improved by a factor of 6.6-10 and no oscillation of the signal intensity was observed at a repetition rate of 1 Hz. Another advantage of the wave stabilizer is that the signal decay time is similar to that without the signal-smoothing device (increased by only 1-2 s for a signal decay of approximately 4 orders of magnitude). Most of the normalized elemental signals (relative to those without the stabilizer) lie within the range of 0.95-1.0 with the wave stabilizer. Thus, the wave stabilizer device does not significantly affect the aerosol transport efficiency. These findings indicate that this device is well-suited for routine optimization of ICPMS, as well as low repetition rate laser ablation analysis, which provides smaller elemental fractionation and better spatial resolution. With the wave signal-smoothing and mercury-removing device, the mercury gas background is reduced by 1 order of magnitude. More importantly, the (202)Hg signal intensity produced in the sulfide standard MASS-1 by laser ablation is reduced from 256 to 0.7 mV by the use of the wave signal-smoothing and mercury-removing device. This result suggests that the mercury is almost completely removed from the sample aerosol particles produced by laser ablation with the operation of the wave mercury-removing device. The wave mercury-removing device that we have designed is very important for Pb isotope ratio and accessory mineral U-Pb dating analysis, where removal of the mercury from the background gas and sample aerosol particles is highly desired. The wave signal-smoothing and mercury-removing device was applied successfully to the determination of the (206)Pb/(204)Pb isotope ratio in samples with low Pb content and/or high Hg content.

Stretching and smearing of chemical heterogeneity by melting and melt migration beneath mid-ocean ridges

NASA Astrophysics Data System (ADS)

Liu, B.; Liang, Y.

2017-12-01

The size of mantle source heterogeneity is important to the interpretation of isotopic signals observed in residual peridotites and basalts. During concurrent melting and melt migration beneath a mid-ocean ridge, both porosity and melt velocity increase upward, resulting in an upward increase in the effective transport velocity for a trace element. Hence a chemical heterogeneity of finite size will be stretched during its transport in the upwelling mantle. This melt migration induced chemical deformation can be quantified by a simple stretching factor. During equilibrium melting, the isotope signals of Sr, Nd and Hf in a 1 km size enriched mantle will be stretched to 2 6 km at the top of the melting column, depending on the style of melt migration. A finite rate of diffusive exchange between residual minerals and partial melt will result in smearing of chemical heterogeneity during its transport in the upwelling melting column. A Gaussian-shaped enriched source in depleted background mantle would be gradually deformed its transit through the melting column. The width of the enriched signal spreads out between the fronts of melt and solid while its amplitude decreases. This melt migration induced smearing also cause mixing of nearby heterogeneities or absorption of enriched heterogeneity by the ambient mantle. Smaller heterogeneities in the solid is more efficiently mixed or aborted by the background mantle than larger ones. Mixing of heterogeneities in the melt depends on the size in the same sense although the erupted melt is more homogenized due to melt accumulation and magma chamber process. The mapping of chemical heterogeneities observed in residual peridotites and basalts into their source region is therefore highly nonlinear. We will show that the observed variations in Nd and Hf isotopes in the global MORB and abyssal peridotites are consistent with kilometer-scale enriched heterogeneities embedded in depleted MORB mantle.

Natural Ca Isotope Composition of Urine as a Rapid Measure of Bone Mineral Balance

NASA Astrophysics Data System (ADS)

Skulan, J.; Gordon, G. W.; Morgan, J.; Romaniello, S. J.; Smith, S. M.; Anbar, A. D.

2011-12-01

Naturally occurring stable Ca isotope variations in urine are emerging as a powerful tool to detect changes in bone mineral balance. Bone formation depletes soft tissue of light Ca isotopes while bone resorption releases isotopically light Ca into soft tissue. Previously published work found that variations in Ca isotope composition could be detected at 4 weeks of bed rest in a 90-day bed rest study (data collected at 4, 8 and 12 weeks). A new 30-day bed rest study involved 12 patients on a controlled diet, monitored for 7 days prior to bed rest and 7 days post bed rest. Samples of urine, blood and food were collected throughout the study. Four times daily blood samples and per void urine samples were collected to monitor diurnal or high frequency variations. An improved chemical purification protocol, followed by measurement using multiple collector inductively coupled plasma mass spectrometry (MC-ICP-MS) allowed accurate and precise determinations of mass-dependent Ca isotope variations in these biological samples to better than ±0.2% (δ44/42Ca) on <25 μg of Ca. Results from this new study show that Ca isotope ratios shift in a direction consistent with net bone loss after just 7 days, long before detectible changes in bone density by X-ray measurements occur. Consistent with this interpretation, the Ca isotope variations track changes observed in N-teleopeptide, a bone resorption biomarker. Bone-specific alkaline phosphatase, a bone formation biomarker, is unchanged over this period. Ca isotopes can in principle be used to quantify net changes in bone mass. Using a mass-balance model, our results indicate an average loss of 0.62 ± 0.16 % in bone mass over the course of this 30-day study. This is consistent with the rate of bone loss in longer-term studies as seen by X-ray measurements. This Ca isotope technique should accelerate the pace of discovery of new treatments for bone disease and provide novel insights into the dynamics of bone metabolism.

Mobile measurement of methane: plumes, isotopes and inventory verification

NASA Astrophysics Data System (ADS)

Lowry, D.; Zazzeri, G.; Fisher, R. E.; France, J.; Al-Shalaan, A.; Lanoisellé, M.; Nisbet, E. G.

2015-12-01

Since 2013 the RHUL group has been identifying methane plumes from major UK sources using a Picarro 2301 coupled to the A0941 mobile module. Once identified the plumes have been sampled by filling Tedlar or Flexfoil bags for later carbon isotopic analysis by high-precision IRMS. This method has ben successfully deployed to isotopically characterize the main anthropogenic methane emitters in the UK (natural gas, coal, landfill, wastewater treatment, cattle; Zazzeri et al., 2015) and during overseas campaigns in eastern Australia (coal, cattle, legacy gas wells) and Kuwait (landfill, wastewater treatment, oil refineries, cattle, camels). This has identified strong similarities of isotopic signature for some sources (landfill, cattle), but large variations for others (natural gas, coal), which must be isotopically resolved at regional scale. Both landfill and natural gas emissions in SE England have tightly-constrained δ13C signatures, averaging -58 ± 3‰ and -36 ± 2‰, respectively, the latter being characteristic of homogenised North Sea gas supply. In contrast, signatures for coal mines in England and Wales fall in a range of 51.2 ± 0.3‰ to 30.9 ± 1.4‰, but can be tightly constrained by region. On a local scale in west London, repeat surveys in the boroughs of Hounslow and Runnymede have been made for comparison with the latest 1x1 km grid UK inventories for 2009 and 2012, which are subdivided by UNECE categories. An excess methane map can be derived for comparison with inventory emissions maps by identifying daily background and binning the excess values from mobile measurements by grid-square. This shows that the spatial distribution of emissions in the UK 2012 inventory is a big improvement on that of 2009. It also suggests that there is an overestimation of emissions from old landfills (closed before 2000 and reliant on a topsoil cap for oxidation), and an underestimation on emissions from currently active landfill cells. Zazzeri, G. et al. (2015) Plume mapping and isotopic characterization of anthropogenic methane sources, Atmospheric Environment, 110, 151-162.

Variation in the isotopic composition of striped weakfish Cynoscion guatucupa of the Southwest Atlantic Ocean in response to dietary shifts.

PubMed

Viola, M N Paso; Riccialdelli, L; Jaureguizar, A; Panarello, H O; Cappozzo, H L

2018-05-01

The aim of this study was to analyze the isotopic composition in muscle of striped weakfish Cynoscion guatucupa from Southwest Atlantic Ocean in order to evaluate a possible variation in δ13C and δ15N in response to dietary shifts that occur as animals grow. We also explored for isotopic evidence of differences between sample locations. The results showed an agreement between isotope analysis and previous conventional studies. Differences in the isotope composition between sampling location were not observed. A positive relation exists between isotope values and total body length of the animals. The Cluster analysis defined three groups of size classes, validated by the MDS. Differences in the relative consumption of prey species in each size class were also observed performing isotope mixing models (SIAR). Variation in δ15N among size classes would be associated with the consumption of a different type of prey as animals grow. Small striped weakfish feed on small crustaceans and progressively increase their consumption of fish (anchovy, Engraulis anchoita), increasing by this way their isotope values. On the other hand, differences in δ13C values seemed to be related to age-class specific spatial distribution patterns. Therefore, large and small striped weakfish remain specialized but feeding on different prey at different trophic levels. These results contribute to the study of the diet of striped weakfish, improve the isotopic ecology models and highlight on the importance of accounting for variation in the isotopic composition in response to dietary shifts with the size of one of the most important fishery resources in the region.

Carbon isotope ratios of human tooth enamel record the evidence of terrestrial resource consumption during the Jomon period, Japan.

PubMed

Kusaka, Soichiro; Uno, Kevin T; Nakano, Takanori; Nakatsukasa, Masato; Cerling, Thure E

2015-08-17

Archaeological remains strongly suggest that the Holocene Japanese hunter-gatherers, the Jomon people, utilized terrestrial plants as their primary food source. However, carbon and nitrogen isotope analysis of bone collagen indicates that they primarily exploited marine resources. We hypothesize that this inconsistency stems from the route of protein synthesis and the different proportions of protein-derived carbon in tooth enamel versus bone collagen. Carbon isotope ratios from bone collagen reflect that of dietary protein and may provide a biased signal of diet, whereas isotope ratios from tooth enamel reflect the integrated diet from all macronutrients (carbohydrates, lipids, and proteins). In order to evaluate the differences in inferred diet between the archaeological evidence and bone collagen isotope data, this study investigated carbon isotopes in Jomon tooth enamel from four coastal sites of the Middle to Late-Final Jomon period (5,000-2,300 years BP). Carbon isotope ratios of human teeth are as depleted as coeval terrestrial mammals, suggesting that C 3 plants and terrestrial mammals were major dietary resources for the Jomon people. Dietary dependence on marine resources calculated from enamel was significantly lower than that calculated from bone collagen. The discrepancy in isotopic ratios between enamel and collagen and the nitrogen isotope ratio in collagen shows a negative correlation on individual and population levels, suggesting diets with variable proportions of terrestrial and marine resources. This study highlights the usefulness of coupling tooth enamel and bone collagen in carbon isotopic studies to reconstruct prehistoric human diet. Am J Phys Anthropol, 2015. © 2015 Wiley Periodicals, Inc. © 2015 Wiley Periodicals, Inc.

Variations in Urine Calcium Isotope: Composition Reflect Changes in Bone Mineral Balance in Humans

NASA Technical Reports Server (NTRS)

Skulan, Joseph; Anbar, Ariel; Bullen, Thomas; Puzas, J. Edward; Shackelford, Linda; Smith, Scott M.

2004-01-01

Changes in bone mineral balance cause rapid and systematic changes in the calcium isotope composition of human urine. Urine from subjects in a 17 week bed rest study was analyzed for calcium isotopic composition. Comparison of isotopic data with measurements of bone mineral density and metabolic markers of bone metabolism indicates the calcium isotope composition of urine reflects changes in bone mineral balance. Urine calcium isotope composition probably is affected by both bone metabolism and renal processes. Calcium isotope. analysis of urine and other tissues may provide information on bone mineral balance that is in important respects better than that available from other techniques, and illustrates the usefulness of applying geochemical techniques to biomedical problems.

Isotope Geochemistry for Comparative Planetology of Exoplanets

NASA Technical Reports Server (NTRS)

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.

Using Oxygen and Carbon Isotopic Signatures in Order to Infer Climatic and Dietary Information in Roman Edessa, Greece

NASA Astrophysics Data System (ADS)

Michael, Dimitra-Ermioni; Dotsika, Elissavet

2017-12-01

Even though many isotopic studies have been conducted on ancient populations from Greece for the purpose of dietary reconstruction; mostly through carbon and nitrogen isotopic signals of bone collagen, less attention has been given to the utility of apatite signatures (oxygen and carbon) as dietary and palaeoenvironmental tools. Moreover, until recently the isotopic signal of tooth enamel for both the purposes of environmental and dietary reconstructions has been rarely assessed in ancient Greek societies. Therefore, the present study aims to provide with novel isotopic information regarding Edessa; a town in Northern Greece, during the Roman period. The current study primarily aims to explore the possible differentiation between the present climatic conditions in Edessa in relation to those occurring at the Roman period. Secondly, this study aims to reveal the significant utility of enamel isotopic signatures (carbon and oxygen) in palaeoenvironmental and palaeodietary studies regarding ancient human remains. The isotopic analyses have been conducted at the Stable Isotope and Radiocarbon Unit of INN, NCSR “Demokritos”. The population of Roman Edessa (2nd-4th c. AD) consists of 22 individuals, providing with 19 bone samples and 16 enamel ones. The mean enamel oxygen value is at -7.7 ±1.1 %0, the bone apatite mean oxygen value at -9.2 ±1.9 %0, and finally the mean carbon enamel value is at -11.7 ±1.2 %0. Oxygen values probably indicate that Edessa had a cooler climate during the Roman times in relation to present conditions, even though more research should be carried out in order to be more certain. In addition, the possible existence of non-local individuals has been revealed through the oxygen teeth enamel-bone apatite spacing. Finally, the carbon enamel signature has pointed out possible differentiations between the adult and the juvenile diet. Based on Edessa’s findings, the stated study strongly encourages the enamel oxygen and carbon isotopic signals as palaeoclimatological and palaeodietary tools respectively.

Stable isotope turnover and half-life in animal tissues: a literature synthesis.

PubMed

Vander Zanden, M Jake; Clayton, Murray K; Moody, Eric K; Solomon, Christopher T; Weidel, Brian C

2015-01-01

Stable isotopes of carbon, nitrogen, and sulfur are used as ecological tracers for a variety of applications, such as studies of animal migrations, energy sources, and food web pathways. Yet uncertainty relating to the time period integrated by isotopic measurement of animal tissues can confound the interpretation of isotopic data. There have been a large number of experimental isotopic diet shift studies aimed at quantifying animal tissue isotopic turnover rate λ (%·day(-1), often expressed as isotopic half-life, ln(2)/λ, days). Yet no studies have evaluated or summarized the many individual half-life estimates in an effort to both seek broad-scale patterns and characterize the degree of variability. Here, we collect previously published half-life estimates, examine how half-life is related to body size, and test for tissue- and taxa-varying allometric relationships. Half-life generally increases with animal body mass, and is longer in muscle and blood compared to plasma and internal organs. Half-life was longest in ecotherms, followed by mammals, and finally birds. For ectotherms, different taxa-tissue combinations had similar allometric slopes that generally matched predictions of metabolic theory. Half-life for ectotherms can be approximated as: ln (half-life) = 0.22*ln (body mass) + group-specific intercept; n = 261, p<0.0001, r2 = 0.63. For endothermic groups, relationships with body mass were weak and model slopes and intercepts were heterogeneous. While isotopic half-life can be approximated using simple allometric relationships for some taxa and tissue types, there is also a high degree of unexplained variation in our models. Our study highlights several strong and general patterns, though accurate prediction of isotopic half-life from readily available variables such as animal body mass remains elusive.

Calculation and mitigation of isotopic interferences in liquid chromatography-mass spectrometry/mass spectrometry assays and its application in supporting microdose absolute bioavailability studies.

PubMed

Gu, Huidong; Wang, Jian; Aubry, Anne-Françoise; Jiang, Hao; Zeng, Jianing; Easter, John; Wang, Jun-sheng; Dockens, Randy; Bifano, Marc; Burrell, Richard; Arnold, Mark E

2012-06-05

A methodology for the accurate calculation and mitigation of isotopic interferences in liquid chromatography-mass spectrometry/mass spectrometry (LC-MS/MS) assays and its application in supporting microdose absolute bioavailability studies are reported for the first time. For simplicity, this calculation methodology and the strategy to minimize the isotopic interference are demonstrated using a simple molecule entity, then applied to actual development drugs. The exact isotopic interferences calculated with this methodology were often much less than the traditionally used, overestimated isotopic interferences simply based on the molecular isotope abundance. One application of the methodology is the selection of a stable isotopically labeled internal standard (SIL-IS) for an LC-MS/MS bioanalytical assay. The second application is the selection of an SIL analogue for use in intravenous (i.v.) microdosing for the determination of absolute bioavailability. In the case of microdosing, the traditional approach of calculating isotopic interferences can result in selecting a labeling scheme that overlabels the i.v.-dosed drug or leads to incorrect conclusions on the feasibility of using an SIL drug and analysis by LC-MS/MS. The methodology presented here can guide the synthesis by accurately calculating the isotopic interferences when labeling at different positions, using different selective reaction monitoring (SRM) transitions or adding more labeling positions. This methodology has been successfully applied to the selection of the labeled i.v.-dosed drugs for use in two microdose absolute bioavailability studies, before initiating the chemical synthesis. With this methodology, significant time and cost saving can be achieved in supporting microdose absolute bioavailability studies with stable labeled drugs.

Comparison of new and existing algorithms for the analysis of 2D radioxenon beta gamma spectra

DOE PAGES

Deshmukh, Nikhil; Prinke, Amanda; Miller, Brian; ...

2017-01-13

The aim of this study is to compare radioxenon beta–gamma analysis algorithms using simulated spectra with experimentally measured background, where the ground truth of the signal is known. We believe that this is among the largest efforts to date in terms of the number of synthetic spectra generated and number of algorithms compared using identical spectra. We generate an estimate for the minimum detectable counts for each isotope using each algorithm. The paper also points out a conceptual model to put the various algorithms into a continuum. Finally, our results show that existing algorithms can be improved and some newermore » algorithms can be better than the ones currently used.« less

The Search for a Non-Superallowed Branch in the β decay of ^38mK

NASA Astrophysics Data System (ADS)

Leach, Kyle; Bandyopadhyay, D.; Finlay, P.; Garrett, P. E.; Grinyer, G. F.; Phillips, A. A.; Schumaker, M. A.; Svensson, C. E.; Wong, J.; Ball, G. C.; Bassiachvilli, E.; Ettenauer, S.; Hackman, G.; Morton, A. C.; Mythili, S.; Newman, O.; Pearson, C. J.; Pearson, M. R.; Savajols, H.; Leslie, J. R.; Melconian, D.; Austin, R. A. E.; Barton, C.

2007-10-01

The study presented is part of an experimental program exploring the properties of superallowed Fermi β decays conducted at the Isotope Separator and Accelerator (ISAC) facility at TRIUMF in Vancouver, B.C. Canada. Using the 8π γ-ray spectrometer and the Scintillating Electron Positron Tagging Array (SCEPTAR), it was possible to set a new upper limit on an unobserved non-analogue branch in the decay of ^38mK. This branch is expected to be extremely weak, and the removal of contaminant isobaric decays and background radiation in the spectra was thus exceedingly important during the analysis. Our work has reduced the previous upper limit by approximately a factor of two and is approaching the theoretically predicted branching ratio.

Orbital Noise in the Earth System is a Common Cause of Climate and Greenhouse-Gas Fluctuation

NASA Technical Reports Server (NTRS)

Liu, H. S.; Kolenkiewicz, R.; Wade, C., Jr.; Smith, David E. (Technical Monitor)

2002-01-01

The mismatch between fossil isotopic data and climate models known as the cool-tropic paradox implies that either the data are flawed or we understand very little about the climate models of greenhouse warming. Here we question the validity of the climate models on the scientific background of orbital noise in the Earth system. Our study shows that the insolation pulsation induced by orbital noise is the common cause of climate change and atmospheric concentrations of carbon dioxide and methane. In addition, we find that the intensity of the insolation pulses is dependent on the latitude of the Earth. Thus, orbital noise is the key to understanding the troubling paradox in climate models.

Apollo-Soyuz pamphlet no. 2: X-rays, gamma-rays. [experimental design

NASA Technical Reports Server (NTRS)

Page, L. W.; From, T. P.

1977-01-01

The nature of high energy radiation and its penetration through earth's atmosphere is examined with emphasis on X-rays, gamma rays, and cosmic radiation and the instruments used in their detection. The history of radio astronomy and the capabilities of the Uhuru satellite are summarized. The ASTP soft X-ray experiment (MA-048) designed to study the spectra in the range from 0.1 to 10 keV and survey the background over a large section of the sky is described, as well as the determination of SMC C-1 as an X-ray pulsar. The crystal activation experiment (MA-151) used to measure the radioactive isotopes created by cosmic rays in crystals used for gamma ray detectors is also discussed.

A setup for active neutron analysis of the fissile material content in fuel assemblies of nuclear reactors

NASA Astrophysics Data System (ADS)

Bushuev, A. V.; Kozhin, A. F.; Aleeva, T. B.; Zubarev, V. N.; Petrova, E. V.; Smirnov, V. E.

2016-12-01

An active neutron method for measuring the residual mass of 235U in spent fuel assemblies (FAs) of the IRT MEPhI research reactor is presented. The special measuring stand design and uniform irradiation of the fuel with neutrons along the entire length of the active part of the FA provide high accuracy of determination of the residual 235U content. AmLi neutron sources yield a higher effect/background ratio than other types of sources and do not induce the fission of 238U. The proposed method of transfer of the isotope source in accordance with a given algorithm may be used in experiments where the studied object needs to be irradiated with a uniform fluence.

Understanding Copper Isotope Behavior in the High Temperature Magmatic-Hydrothermal Porphyry Environment

NASA Astrophysics Data System (ADS)

Gregory, Melissa J.; Mathur, Ryan

2017-11-01

Copper stable isotope geochemistry has the potential to constrain aspects of ore deposit formation once variations in the isotopic data can be related to the physiochemical conditions during metal deposition. This study presents Cu isotope ratios for samples from the Pebble porphyry Cu-Au-Mo deposit in Alaska. The δ65Cu values for hypogene copper sulfides range from -2.09‰ to 1.11‰ and show linear correlations with the δ18O isotope ratios calculated for the fluid in equilibrium with the hydrothermal alteration minerals in each sample. Samples with sodic-potassic, potassic, and illite alteration display a negative linear correlation between the Cu and O isotope results. This suggests that fractionation of Cu isotopes between the fluid and precipitating chalcopyrite is positive as the hydrothermal fluid is evolving from magmatic to mixed magmatic-meteoric compositions. Samples with advanced argillic alteration display a weak positive linear correlation between Cu and O isotope results consistent with small negative fluid-chalcopyrite Cu isotope fractionation during fluid evolution. The hydrothermal fluids that formed sodic-potassic, potassic, and illite alteration likely transported Cu as CuHS0. Hydrothermal fluids that resulted in advanced argillic alteration likely transport Cu as CuCl2-. The pH conditions also control Cu isotope fractionation, consistent with previous experimental work. Larger fractionation factors were found between fluids and chalcopyrite precipitating under neutral conditions contrasting with small fractionation factors calculated between fluids and chalcopyrite precipitating under acidic conditions. Therefore, this study proposes that hydrothermal fluid compositions and pH conditions are related to Cu isotope variations in high temperature magmatic-hydrothermal deposits.