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Sample records for 234u 235u 232th

  1. IUPAC-IUGS status report on the half-lives of 238U, 235U and 234U

    NASA Astrophysics Data System (ADS)

    Villa, I. M.; Bonardi, M. L.; De Bièvre, P.; Holden, N. E.; Renne, P. R.

    2016-01-01

    The current state of knowledge on the half-lives of the long-lived U radionuclides has been reviewed by the IUPAC-IUGS joint Task Group "Isotopes in Geosciences". 238U is assigned a half-life of (4.4683 ± 0.0096) Ga, i.e. a decay constant λ238 = (0.155125 ± 0.000333) Ga-1. The coverage factor is k = 2 for this and all other estimates presented here. The 238U half-life can be used as a reference for the half-lives/decay constants of all other isotopic geochronometers. A revision of the half-life of 235U based on intercomparison of natural geological samples is premature. The improved repeatability of mass spectrometric measurements has revealed Type B uncertainties that had been dismissed as subordinate in the past. The combined uncertainty of these as yet incompletely charted and quantified sources of Type B uncertainty may be no smaller than the currently accepted uncertainty of the α counting experiments. A provisional value for the 234U half-life can be calculated with the assumption of secular equilibrium in the analyzed natural samples. This assumption has not yet been verified independently and its metrological traceability appears sub-optimum. A Type B evaluation suggests that the ca. 0.17% offset between the N(234U)/N(238U) number-ratios of the natural samples used to estimate the 235U half-life and those of the four samples used to estimate the 234U half-life should be compounded into the standard measurement uncertainty of the latter. The resulting provisional uncertainty interval (k = 2) for the 234U half-life is (244.55-247.77) ka, corresponding to λ234 = (2.8203-2.8344) Ma-1.

  2. 206Pb-230Th-234U-238U and 207Pb-235U geochronology of Quaternary opal, Yucca Mountain, Nevada

    USGS Publications Warehouse

    Neymark, Leonid A.; Amelin, Yuri V.; Paces, James B.

    2000-01-01

    U–Th–Pb isotopic systems have been studied in submillimeter-thick outermost layers of Quaternary opal occurring in calcite–silica fracture and cavity coatings within Tertiary tuffs at Yucca Mountain, Nevada, USA. These coatings preserve a record of paleohydrologic conditions at this site, which is being evaluated as a potential high-level nuclear waste repository. The opal precipitated from groundwater is variably enriched in 234U (measured 234U/238U activity ratio 1.124–6.179) and has high U (30–313 ppm), low Th (0.008–3.7 ppm), and low common Pb concentrations (measured 206Pb/204Pb up to 11,370). It has been demonstrated that the laboratory acid treatment used in this study to clean sample surfaces and to remove adherent calcite, did not disturb U–Th–Pb isotopic systems in opal. The opal ages calculated from 206Pb∗/238U and 207Pb∗/235U ratios display strong reverse discordance because of excess radiogenic 206Pb∗ derived from the elevated initial 234U. The data are best interpreted using projections of a new four-dimensional concordia diagram defined by 206Pb∗/238U, 207Pb∗/235U, 234U/238Uactivity, and 230Th/238Uactivity. Ages and initial 234U/238U activity ratios have been calculated using different projections of this diagram and tested for concordance. The data are discordant, that is observed 207Pb∗/235U ages of 170 ± 32 (2σ) to 1772 ± 40 ka are systematically older than 230Th/U ages of 34.1 ± 0.6 to 452 ± 32 ka. The age discordance is not a result of migration of uranium and its decay products under the open system conditions, but a consequence of noninstantaneous growth of opal. Combined U–Pb and 230Th/U ages support the model of slow mineral deposition at the rates of millimeters per million years resulting in layering on a scale too fine for mechanical sampling. In this case, U–Pb ages provide more accurate estimates of the average age for mixed multiage samples than 230Th/U ages, because ages based on shorter

  3. Resonance Region Covariance Analysis Method and New Covariance Data for {sup 232}Th, {sup 233}U, {sup 235}U, {sup 238}U, and {sup 239}Pu

    SciTech Connect

    Leal, L.C. Arbanas, G.; Wiarda, D.; Derrien, H.

    2008-12-15

    Resonance-parameter covariance matrix (RPCM) evaluations in the resolved resonance region were done for {sup 232}Th, {sup 233}U, {sup 235}U, {sup 238}U, and {sup 239}Pu using the computer code SAMMY. The retroactive approach of the code SAMMY was used to generate the RPCMs for {sup 233}U and {sup 235}U. RPCMs for {sup 232}Th, {sup 238}U and {sup 239}Pu were generated together with the resonance parameter evaluations. The RPCMs were then converted in the ENDF format using the File32 representation. Alternatively, for computer storage reasons, the File32 was converted in the File33 cross section covariance matrix (CSCM). Both representations were processed using the computer code PUFF-IV. This paper describes the procedures used to generate the RPCM with SAMMY.

  4. Comparison of the (p,xn) cross sections from /sup 238/U, /sup 235/U, and /sup 232/Th targets irradiated with 200-MeV protons

    SciTech Connect

    Chu, Y.Y.; Zhou, M.L.

    1982-01-01

    We have measured absolute cross sections for (p,xn) reactions (x ranges from 0 to 8) from /sup 238/U, /sup 235/U, and /sup 232/Th targets irradiated with 200-MeV protons at the Brookhaven AGS Linac injector. Chemical yields were determined by using /sup 239/Np and /sup 233/Pa as tracers. Yield patterns obtained in this work can be compared to the experimental results and theoretical calculations from earlier work, and they are consistent within the framework of intranuclear cascade followed by neutron evaporation and fission competition.

  5. Reliability of using 238U/235U and 234U/238U ratios from alpha spectrometry as qualitative indicators of enriched uranium contamination.

    PubMed

    Minteer, Mark; Winkler, Paul; Wyatt, Bill; Moreland, Scott; Johnson, Jamie; Winters, Tim

    2007-05-01

    Alpha spectrometry is a commonly used technique for the measurement of uranium isotopes in environmental samples because it is widely available at a relatively low cost. For natural uranium the (234)U to (238)U activity ratio should be 1 and the (238)U to (235)U activity ratio should be 21.7. However, a lower (238)U to (235)U ratio is usually observed in alpha spectrometric analysis of environmental soil samples. This observation has led to the conclusion that soils from nuclear weapons facilities were contaminated with highly enriched uranium. This study was undertaken to test the reliability of using activity ratios from alpha spectrometry to infer the presence of highly enriched uranium in soil samples. The results of these experiments indicate that the (238)U to (235)U activity ratio is not a reliable indicator, but that the (234)U to (238)U activity ratio can be used to qualitatively indicate the presence of highly enriched uranium at concentrations near 10 ng g(-1) and above.

  6. Uranium ((234)U, (235)U and (238)U) contamination of the environment surrounding phosphogypsum waste heap in Wiślinka (northern Poland).

    PubMed

    Olszewski, Grzegorz; Boryło, Alicja; Skwarzec, Bogdan

    2015-08-01

    The aim of this work was to determine the uranium concentration ((234)U, (235)U and (238)U) and values of the activity ratio (234)U/(238)U in soil samples collected near phosphogypsum waste heap in Wiślinka (northern Poland). On the basis of the studies it was found that the values of the (234)U/(238)U activity ratio in the analyzed soils collected in the vicinity of phosphogypsum dump in Wiślinka are in most cases close to one and indicate the phosphogypsum origin of the analyzed nuclides. The obtained results of uranium concentrations are however much lower than in previous years before closing of the phosphogypsum stockpile. After this process and covering the phosphogypsum stockpile in Wiślinka with sewage sludge, phosphogypsum particles are successfully immobilized. In the light of the results the use of phosphate fertilizers seems to be a major problem. Prolonged and heavy rains can cause leaching accumulated uranium isotopes in the phosphogypsum stockpile, which will be washed into the Martwa Wisła and on the fields in the immediate vicinity of this storage.

  7. Calibration factors for determination of relativistic particle induced fission rates in natU, 235U, 232Th, natPb and 197Au foils

    NASA Astrophysics Data System (ADS)

    Hashemi-Nezhad, S. R.; Zhuk, Igor; Potapenko, A.; Kievets, M.; Krivopustov, M. I.

    2012-02-01

    Calibration factors w, for determination of fission rate in metallic foils of natU, 235U, 232Th, natPb and 197Au were determined for foils in contact with synthetic mica track detectors. Proton-induced fission at proton energies of 0.7 GeV and 1.5 GeV were used. Using our experimental results as well as those of the other authors, w for different foil-mica systems were determined. Two methods were used to calculate w, relative to the calibration factor for uranium-mica system, which has been obtained in a standard neutron field of energy 14.7 MeV. One of these methods requires the knowledge of the mean range of the fission fragments in the foils of interest and other method needs information on the values of the fission cross-sections at the required energies as well as the density of the tracks recorded in the track detectors in contact with the foil surfaces. The obtained w-values were compared with Monte Carlo calculations and good agreements were found. It is shown that a calibration factor obtained at low energy neutron induced fissions in uranium isotopes deviates only by less than 10% from those obtained at relativistic proton induced fissions.

  8. Ground water contamination with (238)U, (234)U, (235)U, (226)Ra and (210)Pb from past uranium mining: cove wash, Arizona.

    PubMed

    Dias da Cunha, Kenya Moore; Henderson, Helenes; Thomson, Bruce M; Hecht, Adam A

    2014-06-01

    The objectives of the study are to present a critical review of the (238)U, (234)U, (235)U, (226)Ra and (210)Pb levels in water samples from the EPA studies (U.S. EPA in Abandoned uranium mines and the Navajo Nation: Red Valley chapter screening assessment report. Region 9 Superfund Program, San Francisco, 2004, Abandoned uranium mines and the Navajo Nation: Northern aum region screening assessment report. Region 9 Superfund Program, San Francisco, 2006, Health and environmental impacts of uranium contamination, 5-year plan. Region 9 Superfund Program, San Franciso, 2008) and the dose assessment for the population due to ingestion of water containing (238)U and (234)U. The water quality data were taken from Sect. "Data analysis" of the published report, titled Abandoned Uranium Mines Project Arizona, New Mexico, Utah-Navajo Lands 1994-2000, Project Atlas. Total uranium concentration was above the maximum concentration level for drinking water (7.410-1 Bq/L) in 19 % of the water samples, while (238)U and (234)U concentrations were above in 14 and 17 % of the water samples, respectively. (226)Ra and (210)Pb concentrations in water samples were in the range of 3.7 × 10(-1) to 5.55 × 102 Bq/L and 1.11 to 4.33 × 102 Bq/L, respectively. For only two samples, the (226)Ra concentrations exceeded the MCL for total Ra for drinking water (0.185 Bq/L). However, the (210)Pb/(226)Ra ratios varied from 0.11 to 47.00, and ratios above 1.00 were observed in 71 % of the samples. Secular equilibrium of the natural uranium series was not observed in the data record for most of the water samples. Moreover, the (235)U/(total)U mass ratios ranged from 0.06 to 5.9 %, and the natural mass ratio of (235)U to (total)U (0.72 %) was observed in only 16 % of the water samples, ratios above or below the natural ratio could not be explained based on data reported by U.S. EPA. In addition, statistical evaluations showed no correlations among the distribution of the radionuclide concentrations

  9. Investigation of (235)U, (226)Ra, (232)Th, (40)K, (137)Cs, and heavy metal concentrations in Anzali international wetland using high-resolution gamma-ray spectrometry and atomic absorption spectroscopy.

    PubMed

    Zare, Mohammad Reza; Kamali, Mahdi; Fallahi Kapourchali, Maryam; Bagheri, Hashem; Khoram Bagheri, Mahdi; Abedini, Ali; Pakzad, Hamid Reza

    2016-02-01

    Measurements of natural radioactivity levels and heavy metals in sediment and soil samples of the Anzali international wetland were carried out by two HPGe-gamma ray spectrometry and atomic absorption spectroscopy techniques. The concentrations of (235)U, (226)Ra, (232)Th, (40)K, and (137)Cs in sediment samples ranged between 1.05 ± 0.51-5.81 ± 0.61, 18.06 ± 0.63-33.36 ± .0.34, 17.57 ± 0.38-45.84 ± 6.23, 371.88 ± 6.36-652.28 ± 11.60, and 0.43 ± 0.06-63.35 ± 0.94 Bq/kg, while in the soil samples they vary between 2.36-5.97, 22.71-38.37, 29.27-42.89, 472.66-533, and 1.05-9.60 Bq/kg for (235)U, (226)Ra, (232)Th, (40)K, and (137)Cs, respectively. Present results are compared with the available literature data and also with the world average values. The radium equivalent activity was well below the defined limit of 370 Bq/kg. The external hazard indices were found to be less than 1, indicating a low dose. Heavy metal concentrations were found to decrease in order as Fe > Mn > Sr > Zn > Cu > Cr > Ni > Pb > Co > Cd. These measurements will serve as background reference levels for the Anzali wetland.

  10. Decay of {sup 246}Bk* formed in similar entrance channel reactions of {sup 11}B+{sup 235}U and {sup 14}N+{sup 232}Th at low energies using the dynamical cluster-decay model

    SciTech Connect

    Singh, BirBikram; Sharma, Manoj K.; Gupta, Raj K.

    2008-05-15

    The decay of the {sup 246}Bk* nucleus, formed in entrance channel reactions {sup 11}B+{sup 235}U and {sup 14}N+{sup 232}Th at different incident energies, is studied by using the dynamical cluster-decay model (DCM) extended to include the deformations and orientations of nuclei. The main decay mode here is fission. The other (weaker) decay channels are the light particles evaporation (A{<=}4) and intermediate mass fragments (5{<=}A{<=}20). All decay products are calculated as emissions of preformed clusters through the interaction barriers. The calculated fission cross sections {sigma}{sub fiss}, taken as a sum of the energetically favored symmetric and near symmetric fragments (A{sub CN}/2{+-}7 and A=106-110 plus complementary fragments) show an excellent agreement with experimental data at all experimental incident c.m. energies for both reactions, except for the top three energies in the case of the {sup 11}B+{sup 235}U reaction. The disagreement between the DCM calculations and data at higher incident c.m. energies for the {sup 11}B+{sup 235}U entrance channel is associated with the presence of additional effects of noncompound, quasifission (qf) components, in contradiction with the measured anisotropy effects which indicate the other entrance channel {sup 14}N+{sup 232}Th to contain the noncompound nucleus contribution. The prediction of two fission windows, the symmetric fission (SF) and near symmetric or heavy mass fragments (HMFs), suggests the presence of a fine structure of fission fragments, which also need an experimental verification. The only parameter of the model is the neck length parameter {delta}R whose value is shown to depend strongly on limiting angular momentum, which in turn depends on the use of sticking or nonsticking moment of inertia for angular momentum effects.

  11. Preliminary results of calculations for heavy-water nuclear-power-plant reactors employing 235U, 233U, and 232Th as a fuel and meeting requirements of a nonproliferation of nuclear weapons

    NASA Astrophysics Data System (ADS)

    Ioffe, B. L.; Kochurov, B. P.

    2012-02-01

    A physical design is developed for a gas-cooled heavy-water nuclear reactor intended for a project of a nuclear power plant. As a fuel, the reactor would employ thorium with a small admixture of enriched uranium that contains not more than 20% of 235U. It operates in the open-cycle mode involving 233U production from thorium and its subsequent burnup. The reactor meets the conditions of a nonproliferation of nuclear weapons: the content of fissionable isotopes in uranium at all stages of the process, including the final one, is below the threshold for constructing an atomic bomb, the amount of product plutonium being extremely small.

  12. Preliminary results of calculations for heavy-water nuclear-power-plant reactors employing {sup 235}U, {sup 233}U, and {sup 232}Th as a fuel and meeting requirements of a nonproliferation of nuclear weapons

    SciTech Connect

    Ioffe, B. L.; Kochurov, B. P.

    2012-02-15

    A physical design is developed for a gas-cooled heavy-water nuclear reactor intended for a project of a nuclear power plant. As a fuel, the reactor would employ thorium with a small admixture of enriched uranium that contains not more than 20% of {sup 235}U. It operates in the open-cycle mode involving {sup 233}U production from thorium and its subsequent burnup. The reactor meets the conditions of a nonproliferation of nuclear weapons: the content of fissionable isotopes in uranium at all stages of the process, including the final one, is below the threshold for constructing an atomic bomb, the amount of product plutonium being extremely small.

  13. Activity measurements of a suite of radionuclides (241Am, 239,240Pu, 238Pu, 238U, 234U, 235U, 232Th, 230Th, 228Th, 228Ra, 137Cs, 210Pb, 90Sr and 40K) in biota reference material (Ocean Shellfish): CCRI(II)-S3

    NASA Astrophysics Data System (ADS)

    Nour, S.; Karam, L. R.; Inn, K. G. W.

    2012-01-01

    In 2005, the CCRI decided that a comparison undertaken from 2002 to 2008 by the NIST (under the auspices of the Inter-America Metrology System [SIM]) in the development of a new biota (Ocean Shellfish) standard reference material (SRM) was sufficiently well constructed that it could be converted into a supplementary comparison under CCRI(II), with comparison identifier CCRI(II)-S3. This would enable the comparison to be used to support calibration and measurement capability (CMC) claims for radionuclide measurements in reference materials (specifically, animal-based organic materials). Previous comparisons of radionuclides have been of single or multiple nuclides in non-complex matrices and results of such could not be extended to support capabilities to measure the same nuclides in reference materials. The results of this comparison have been used to determine the certified reference value of the SRM. The key comparison working group (KCWG) of the CCRI(II) has approved this approach as a mechanism to link all the results to certified 'reference values' in lieu of the key comparison reference value (KCRV) of these specified radionuclides in this type of matrix (shellfish) so as to support CMCs of similar materials submitted by the present participants. Main text. To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/. The final report has been peer-reviewed and approved for publication by the CCRI, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

  14. SUPPLEMENTARY COMPARISON: Activity measurements of a suite of radionuclides (40K, 137Cs, 210Pb, 210Po, 228Ra, 232Th, 234U, 235U, 238U, 238Pu, 239Pu, 239+240Pu, 241Am) in vegetal reference material (seaweed)

    NASA Astrophysics Data System (ADS)

    Outola, I.; Inn, K. G. W.; Karam, L. R.

    2008-01-01

    In 2005, the CCRI decided that a comparison undertaken from 2002 to 2005 by the NIST (SIM) in the development of a new seaweed standard reference material (SRM) was sufficiently well constructed that it could be converted into a supplementary comparison under CCRI(II), with comparison identifier CCRI(II)-S1, so as to support calibration and measurement capability (CMC) claims for radionuclide measurements in reference material (specifically, plant material). Previous comparisons of radionuclides have been of single or multiple nuclides in non-complex matrices and results of such could not be extended to support capabilities to measure the same nuclides in reference materials. The results of this comparison have been reported to the participants, and were also used to determine the certified reference values of the SRM. The key comparison working group (KCWG) of the CCRI(II) has approved this approach as a mechanism to link all the results to the certified 'reference values' in lieu of the key comparison reference value (KCRV) of these specified radionuclides in this type of matrix (vegetative) so as to support CMCs of similar materials. Main text. To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/. The final report has been peer-reviewed and approved for publication by the CCRI Section II, according to the provisions of the CIPM Mutual Recognition Arrangement (MRA).

  15. Activity ratios of (234)U/(238)U and (226)Ra/(228)Ra for transport mechanisms of elevated uranium in alluvial aquifers of groundwater in south-western (SW) Punjab, India.

    PubMed

    Kumar, A; Karpe, R K; Rout, S; Gautam, Y P; Mishra, M K; Ravi, P M; Tripathi, R M

    2016-01-01

    The concentrations of total dissolved uranium (U), its isotopic composition ((234)U, (235)U, (238)U) and two long lived Ra isotopes ((226)Ra and (228)Ra) in alluvial aquifers of groundwater were determined to investigate the groundwater flow pattern in the south-western (SW) Punjab, India. Particular attention was given to the spatial variability of activity ratios (ARs) of (234)U/(238)U and (226)Ra/(228)Ra to predict the possible sources and supply process of U into the water from the solid phase. The measured groundwater (234)U/(238)U ARs were ∼1 or >1 in the shallow zone (depth < 30 m) with high U concentration and <1 in the deeper zone (depth > 30 m) with relatively low U concentration. The simultaneous elevated U concentration and (234)U/(238)U ARs in waters were possibly due to differences in imprints of rock-water interactions under hydrologic conditions. However, (234)U/(238)U ARs < 1 clearly indicate the lack of recharge from surface water to groundwater leading to (234)U deficit in groundwater. This deficit might be also attributed to alpha recoil processes under strong dissolution. Overall, the decreasing pattern of (234)U/(238)U ARs observed from SE to SW or NW ward clearly indicates a groundwater flow paths from SE to SW/NW. Similarly, (226)Ra/(238)U ARs < 1 for all water samples reflect that the precursor (238)U is fairly mobile relative to (226)Ra. This might be due to unusually high amount of (238)U in groundwaters and subsequently the different geochemistry of the two isotopes. On the other hand, (226)Ra/(228)Ra ARs in groundwaters varied widely and observed about 50-300 times higher than (238)U/(232)Th ARs in granitic rocks or soils. Such elevation in ARs might be attributed to different dissolution properties of their parents during water-rock interactions or lattice damage during decay or local enrichments of uranium in the aquifers.

  16. sup 234 U/ sup 238 U and sup 230 Th/ sup 234 U activity ratios in the collidal phases of aquifers in lateritic weathered zones

    SciTech Connect

    Short, S.A.; Lowson, R.T. ); Ellis, J. )

    1988-11-01

    A procedure was developed for comparing solute and colloid phases of groundwaters in contact with uranium ore bodies at Nabarlek and Koongarra in the Alligator Rivers region, Northern Territory, Australia. Single-pass ultrafiltration of large volumes with cut-offs of 18 nm and 1 {mu}m was used. Colloids were composed of Fe and Si species with sorbed U and U daughters. Uranium isotopes were mostly present as soluble species. Thorium was significantly associated with the colloids. The {sup 234}U/{sup 238}U activity ratios (ARs) were similar in solute and colloid phases close to the ore bodies but further down-gradient colloids were generally more depleted of {sup 234}U than the solute. The {sup 230}Th/{sup 234}U ARs rose from very low values for both solute and colloid phases close to the ore bodies through several orders of magnitude to much higher values further down-gradient. Colloid {sup 230}Th/{sup 234}U ARs were always significantly greater than solute ARs. Results were consistent with a systematic leaching of U from colloids going down-gradient and very little mobilization of ore body. {sup 230}Th relative to U. Ubiquitous complexes {sup 232}Th appeared to suppress the solubility of {sup 230}Th.

  17. 234U /238U and 230Th /234U activity ratios in the colloidal phases of aquifers in lateritic weathered zones

    NASA Astrophysics Data System (ADS)

    Short, Stephen A.; Lowson, Richard T.; Ellis, John

    1988-11-01

    A procedure was developed for comparing solute and colloid phases of groundwaters in contact with uranium ore bodies at Nabarlek and Koongarra in the Alligator Rivers region, Northern Territory, Australia. Single-pass ultrafiltration of large volumes with cut-offs of 18 nm and 1 μm was used. Colloids were composed of Fe and Si species with sorbed U and U daughters. Uranium isotopes were mostly present as soluble species. Thorium was significantly associated with the colloids. The 234U /238U activity ratios (ARs) were similar in solute and colloid phases close to the ore bodies but further down-gradient colloids were generally more depleted of 234U than the solute. The 230Th /234U ARs rose from very low values for both solute and colloid phases close to the ore bodies through several orders of magnitude to much higher values further down-gradient. Colloid 230Th /234U ARs were always significantly greater than solute ARs. Results were consistent with a systematic leaching of U from colloids going down-gradient and very little mobilization of ore-body 230Th relative to U. Ubiquitous complexed 232Th appeared to suppress the solubility of 230Th.

  18. Geochemistry of speleothem records from southern Illinois: Development of (234U)/(238U) as a proxy for paleoprecipitation

    USGS Publications Warehouse

    Zhou, Juanzuo; Lundstrom, C.C.; Fouke, B.; Panno, S.; Hackley, K.; Curry, B.

    2005-01-01

    Natural waters universally show fractionation of uranium series (U-series) parent-daughter pairs, with the disequilibrium between 234U and 238U (234U)/(238U) commonly used as a tracer of groundwater flow. Because speleothems provide a temporal record of geochemical variations in groundwater precipitating calcite, (234U)/(238U) variations in speleothems provide a unique method of investigating water-rock interaction processes over millennium time scales. We present high precision Thermal Ionization Mass Spectrometric (TIMS) U-series analyses of speleothems and drip waters from Fogelpole Cave in southern Illinois. Data from all speleothems from the cave show an inverse correlation between (234U)/(238U) and U concentration, following the pattern observed in groundwaters globally. Within a 65-cm-long stalagmite, concordant 234U-238 U-230Th and 235U-231Pa ages for 5 samples indicate accurate chronology from 78.5 ka to 30 ka. Notably, (234U)/(238U)o which differs from most speleothems by having (234U)/(238U)o <1, positively correlates with speleothem growth rate. We generalize this to the observation that speleothems globally show (234U)/ (238U)o deviating farther from secular equilibrium at lower growth rates and approaching secular equilibrium at higher grow rates. Based on the Fogelpole observations, we suggest that groundwater (234U)/(238U) is controlled by the U oxidation state, the U concentration of the water and the fluid velocity. A transport model whereby U-series nuclides react and exchange with mineral surfaces can reproduce the observed trend between growth rate and (234U)/(238U)o. Based on this result, we suggest that (234U)/(238U)o in speleothems may record changes in hydrologic flux with time and thus could provide a useful proxy for long term records of paleoprecipitation. ?? 2005 Elsevier B.V. All rights reserved.

  19. Feasibility of 99Mo production by proton-induced fission of 232Th

    NASA Astrophysics Data System (ADS)

    Abbas, Kamel; Holzwarth, Uwe; Simonelli, Federica; Kozempel, Jan; Cydzik, Izabela; Bulgheroni, Antonio; Cotogno, Giulio; Apostolidis, Christos; Bruchertseifer, Frank; Morgenstern, Alfred

    2012-05-01

    The current global crisis in supply of the medical isotope generator 99Mo/99mTc has triggered much research into alternative non-reactor based production methods for 99Mo including innovative radionuclide production techniques using ion accelerators. A novel method is presented here that has thus far not been considered: 232Th is used as target material to produce carrier-free 99Mo for 99Mo/99mTc generators by proton-induced fission (232Th (p, f) 99Mo). The thick target yields of 99Mo are estimated as 3.6 MBq/μA·h and 21 MBq/μA·h for proton energies of 22 MeV and 40 MeV, respectively, energies that are available from many cyclotrons. With respect to 99Mo reactor based methods using uranium targets, the presented concept using 232Th does not pose proliferation concerns, transport of highly radioactive target materials can be reduced and unused cyclotron capacities could be exploited. Radiochemical target processing could be based on existing technologies of extraction of 99Mo from reactor irradiated 235U. The presented method could be used for co-production of other radioisotopes of medical interest such as 131I.

  20. Remeasurement of (234)U Half-Life.

    PubMed

    Varga, Zsolt; Nicholl, Adrian; Wallenius, Maria; Mayer, Klaus

    2016-03-01

    The half-life of (234)U has been measured using a novel approach. In this method, a uranium material was chemically purified from its thorium decay product at a well-known time. The ingrowth of the (230)Th daughter product in the material was followed by measuring the accumulated (230)Th daughter product relative to its parent (234)U nuclide using inductively coupled plasma mass spectrometry. Then, the (234)U decay constant and the respective half-life could be calculated using the radioactive decay equations based on the n((230)Th)/n((234)U) amount ratio. The obtained (234)U half-life is 244 900 ± 670 years (k = 1), which is in good agreement with the previously reported results in the literature with comparable uncertainty. The main advantages of the proposed method are that it does not require the assumption of secular equilibrium between (234)U and (238)U. Moreover, the calculation is independent from the (238)U half-life value and its uncertainty. The suggested methodology can also be applied for the remeasurement of the half-lives of several other long-lived radionuclides.

  1. sup 238 U- and sup 232 Th-series chronology of phonolite fractionation at Mount Erebus, Antarctica

    SciTech Connect

    Reagan, M.K. ); Volpe, A.M. ); Cashman, K.V. )

    1992-03-01

    Uranium, thorium, radium, and barium abundances and {sup 234}U/{sup 238}U and {sup 230}Th/{sup 232}Th isotopic ratios determined by thermal ionization mass spectrometry and ({sup 228}Th)/({sup 232}Th) activity ratios determined by alpha spectrometry are used to date anorthoclase growth and infer magma chamber residence times of phonolites erupted in 1984 and 1988 from Mount Erebus, Antarctica. The 1984 and 1988 glasses have slightly different ({sup 230}Th)/({sup 232}Th) ratios but both have a 10% excess of ({sup 230}Th) over ({sup 238}U) and equilibrium ({sup 228}Th) values. By comparing these data and Pb-isotopic data reported in SUN and HANSON (1975) to similar data for oceanic basalts, the duration of differentiation from basanite to phonolite is limited to less than 150,000 years. The anorthoclase separates have ({sup 230}Th)/({sup 238}U) ratios exceeding those of the associated glasses but have ({sup 230}Th)/({sup 232}Th) ratios like those of the glasses. Both glasses are depleted in {sup 226}Ra with respect to {sup 230}Th by about 25%, whereas associated anorthoclase separates have extreme excesses of {sup 226}Ra over {sup 230}Th and ({sup 228}Th)/({sup 232}Th) = 2.2. On a plot of ({sup 226}Ra)/Ba vs. ({sup 230}Th)/BA, the glass-anorthoclase pairs produce isochrons averaging 2,380 y, which represents the average age of anorthoclase growth in the shallow magma system at Erebus. The implied residence time of phonolite magmas in the shallow magma chamber system of Erebus is about 3,000 y. Final crystal growth occurred after intrusion into the convecting lava lake less than decades before eruption.

  2. Fission Product Yields from 232Th, 238U, and 235U Using 14 MeV Neutrons

    NASA Astrophysics Data System (ADS)

    Pierson, B. D.; Greenwood, L. R.; Flaska, M.; Pozzi, S. A.

    2017-01-01

    Neutron-induced fission yield studies using deuterium-tritium fusion-produced 14 MeV neutrons have not yet directly measured fission yields from fission products with half-lives on the order of seconds (far from the line of nuclear stability). Fundamental data of this nature are important for improving and validating the current models of the nuclear fission process. Cyclic neutron activation analysis (CNAA) was performed on three actinide targets-thorium-oxide, depleted uranium metal, and highly enriched uranium metal-at the University of Michigan's Neutron Science Laboratory (UM-NSL) using a pneumatic system and Thermo-Scientific D711 accelerator-based fusion neutron generator. This was done to measure the fission yields of short-lived fission products and to examine the differences between the delayed fission product signatures of the three actinides. The measured data were compared against previously published results for 89Kr, -90, and -92 and 138Xe, -139, and -140. The average percent deviation of the measured values from the Evaluated Nuclear Data Files VII.1 (ENDF/B-VII.1) for thorium, depleted-uranium, and highly-enriched uranium were -10.2%, 4.5%, and -12.9%, respectively. In addition to the measurements of the six known fission products, 23 new fission yield measurements from 84As to 146La are presented.

  3. Dating open systems by the 238U- 234U- 230Th method: application to Quaternary reef terraces

    NASA Astrophysics Data System (ADS)

    Villemant, B.; Feuillet, N.

    2003-05-01

    The sedimentation conditions and diagenetic processes of biogenic and inorganic carbonates are such that the assumptions of a closed system evolution and the absence of initial Th invoked in classical 238U- 234U- 230Th dating methods are very often not fulfilled for such material. This problem is of interest for all studies requiring accurate dating of corals or aragonite-rich sediments as in palaeoclimatology or neotectonics. Extending the approach of Henderson and Slowey [Nature 404 (2000) 61-66], we propose a consistent model that takes into account possible initial 230Th excess and where continuous selective redistribution (gain or loss) of 234U, 234Th and 230Th is controlled by recoil processes. This model applied to Quaternary marine terraces in Barbados, Marie Galante (Lesser Antilles arc) and Pacific islands, is able to explain the large scatter in isotopic compositions observed in the series of cogenetic corals or sediments. We show that recoil processes generally tend to increase the ( 234U/ 238U) and ( 230Th/ 234U) ratios with time, leading to an overestimation of the apparent ages calculated using classical methods. On the basis of simple assumptions (identical 'marine' initial ( 234U/ 238U) 0 and ( 230Th/ 232Th) 0 ratios), we propose a method for calculating a best estimate of the age of cogenetic series. Our model offers an alternative way to date old reef terraces where corals are almost systematically altered and where classical dating methods do not apply. It may also explain the apparent variations of the ( 234U/ 238U) seawater initial ratio estimated from corals formed in the last 300 ka and the apparent uncoupling between sea-level highstands and high-latitude Northern Hemisphere summer insolation. Our set of equations can be applied to all weathering processes where the mobility of U-series isotopes is controlled by recoil.

  4. Resonance Region Covariance Analysis Method and New Covariance Data for Th-232, U-233, U-235, U-238, and Pu-239

    SciTech Connect

    Leal, Luiz C; Arbanas, Goran; Derrien, Herve; Wiarda, Dorothea

    2008-01-01

    Resonance-parameter covariance matrix (RPCM) evaluations in the resolved resonance region were done for 232Th, 233U, 235U, 238U, and 239Pu using the computer code SAMMY. The retroactive approach of the code SAMMY was used to generate the RPCMs for 233U, 235U. RPCMs for 232Th, 238U and 239Pu were generated together with the resonance parameter evaluations. The RPCMs were then converted in the ENDF format using the FILE32 representation. Alternatively, for computer storage reasons, the FILE32 was converted in the FILE33 cross section covariance matrix (CSCM). Both representations were processed using the computer code PUFF-IV. This paper describes the procedures used to generate the RPCM with SAMMY.

  5. Coulomb excitation of states in 232Th

    NASA Astrophysics Data System (ADS)

    McGowan, F. K.; Milner, W. T.

    1993-09-01

    Twenty-five states in 232Th have been observed with 18 MeV 4He ions on a thick target. Eleven 2 + states between 774 and 1554 keV and three 3 - states are populated by direct E2 and E3, respectively. The remaining states are either weakly excited by multiple Coulomb excitation and/or populated by the decay of the directly excited states. Spin assignments are based on γ-ray angular distributions. Reduced transition probabilities have been deduced from the γ-ray yields. The B(E2) values for excitation of the 2 + states range from 0.024 to 3.5 W.u. (222 W.u. for the first 2 + state). For the 3 - states, the B(E3,0 → 3 -) values are 1.7, 11, and 24 W.u. A possible two-phonon state at 1554 keV, which is nearly harmonic, decays to four members of the one-phonon states, to the ground-state band, and to the K = 0 - octupole band. The B(E2) value for excitation of this state is 0.66 ± 0.05 W.u. and the B(E1) values for decay of this state are (2 and 6)×10 -4 W.u. The B(E2) values between two- and one-phonon vibrational states range between 16 and 53 W.u. which are an order of magnitude larger than the B(E2) values between the one- and zero-phonon states. This disagrees with our present understanding of collectivity in nuclei if this 2 + state is considered to be a collective two-phonon excitation. The 2 + states at 1477 and 1387 keV, which are also nearly harmonic, are possible candidates with two-phonon structure. The agreement between the experimental results and the microscopic calculations by Neergård and Vogel of the B(E3,0 → 3) for the 3 - members of the one-phonon octupole quadruplet is satisfactory when the Coriolis coupling between the states with K and K ± 1 is included. The B(E1) branching ratios for transitions from the 3 - and 1 - states to the ground-state band have large deviations from the Alaga-rule predictions. These deviations can be understood by the strong Coriolis coupling between the states of the octupole quadruplet in deformed nuclei.

  6. Evaluation of 235U decay data.

    PubMed

    Xiaolong, Huang; Baosong, Wang

    2009-09-01

    Evaluation of the complete decay scheme and data for (235)U including new measurements are presented in this report; literature data available up to June 2008 are included. The half-life is determined to be (7.04+/-0.01) x 10(8) yr. All known measured gamma-ray absolute intensities have been examined; the gamma-ray emission probability of the reference gamma-ray line of 185.72 keV is recommended to be 57.0+/-0.3%. The calculated internal conversion coefficients and their uncertainties have been used to obtain the complete decay intensity balance. The other decay characteristics are calculated using the ENSDF analysis program. Finally the new decay scheme for (235)U is presented.

  7. 31 CFR 540.315 - Uranium-235 (U235).

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 31 Money and Finance: Treasury 3 2010-07-01 2010-07-01 false Uranium-235 (U235). 540.315 Section... FOREIGN ASSETS CONTROL, DEPARTMENT OF THE TREASURY HIGHLY ENRICHED URANIUM (HEU) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.315 Uranium-235 (U235). The term uranium-235 or U235 means the...

  8. Correction methodology for the spectral interfering γ-rays overlapping to the analytical peaks used in the analysis of 232Th.

    PubMed

    Yücel, H; Köse, E; Esen, A N; Bor, D

    2011-06-01

    In the γ-ray spectrometric analysis of the radionuclides, a correction factor is generally required for the spectral interfering γ-rays in determining the net areas of the analytical peaks because some interfering γ-rays often might contribute to the analytical peaks of interest. In present study, a correction methodology for the spectral interfering γ-rays (CSI) is described. In particular, in the analysis of (232)Th contained in samples, the interfering γ-rays due to (226)Ra, (235)U, (238)U and their decay products often overlap to the peaks of interest from (232)Th decay products, and vise versa. For the validation of the proposed CSI method, several certified reference materials (CRM) containing U and Th were measured by using a 76.5% efficient n-type Ge detector. The required correction factors were quantified for spectral interference, self-absorption and true coincidence summing (TCS) effects for the relevant γ-rays. The measured results indicate that if one ignores the contributions of the interfering γ-rays to the analytical peaks at 583.2 keV of (208)Tl and 727.3 keV of (212)Bi, this leads to a significantly systematic influence on the resulted activities of (232)Th. The correction factors required for spectral interference and TCS effects are estimated to be ∼13.6% and ∼15.4% for 583.2 keV peak. For the 727.3 keV peak, the correction factor is estimated to be ∼15% for spectral interference, and ∼5% for the TCS effects at the presently used detection geometry. On the other hand, the measured results also indicate that ignoring the contribution of the interfering γ-rays to the areas of the analytical peaks at 860.6 keV of (208)Tl, 338.3 and 911.2 keV of (228)Ac does not lead to any significant systematic influence on the (232)Th analysis. Because these factors are remained generally less than ∼5%, i.e., within overall uncertainty limits. The present study also showed that in view of both the spectral interference and TCS effects, the

  9. 238U-234U-230Th disequilibrium in hydrogenous oceanic Fe-Mn crusts: Palaeoceanographic record or diagenetic alteration?

    USGS Publications Warehouse

    Chabaux, F.; O'Nions, R. K.; Cohen, A.S.; Hein, J.R.

    1997-01-01

    A detailed TIMS study of (234Uexc/238U), (230Th/232Th), and Th/U ratios have been performed on the outermost margin of ten hydrogenous Fe-Mn crusts from the equatorial Pacific Ocean and west-central Indian Ocean. Th/U concentration ratios generally decrease from the crust's surface down to 0.5-1 mm depth and growth rates estimated by uranium and thorium isotope ratios are significantly different in Fe-Mn crusts from the Peru Basin and the west-central Indian Ocean. Fe-Mn crusts from the same geographical area define a single trend in plots of Ln (234Uexc/238U) vs. Ln(230Th/232Th) and Th/U ratios vs. age of the analysed fractions. Results suggest that (1) hydrogenous Fe-Mn crusts remain closed-systems after formation, and consequently (2) the discrepancy observed between the 230Th and 234U chronometers in Fe-Mn crusts, and the variations of the Th/U ratios through the margin of Fe-Mn crusts, are not due to redistribution of uranium and thorium isotopes after oxyhydroxide precipitation, but rather to temporal variations of both Th/U and initial thorium activity ratios recorded by the Fe-Mn layers. Implications of these observations for determination of Fe-Mn crust growth-rates are discussed. Variations of both Th/U and initial Th activity ratios in Fe-Mn crusts might be related to changes in particle input to seawater and/or changes in ocean circulation during the last 150 ka. Copyright ?? 1997 Elsevier Science Ltd.

  10. 238U series isotopes and 232Th in carbonates and black shales from the Lesser Himalaya: implications to dissolved uranium abundances in Ganga-Indus source waters.

    PubMed

    Singh, S K; Dalai, Tarun K; Krishnaswami, S

    2003-01-01

    238U and (232)Th concentrations and the extent of (238)U-(234)U-(230)Th radioactive equilibrium have been measured in a suite of Precambrian carbonates and black shales from the Lesser Himalaya. These measurements were made to determine their abundances in these deposits, their contributions to dissolved uranium budget of the headwaters of the Ganga and the Indus in the Himalaya and to assess the impact of weathering on (238)U-(234)U-(230)Th radioactive equilibrium in them. (238)U concentrations in Precambrian carbonates range from 0.06 to 2.07 microg g(-1). The 'mean' U/Ca in these carbonates is 2.9 ng U mg(-1) Ca. This ratio, coupled with the assumption that all Ca in the Ganga-Indus headwaters is of carbonate origin and that U and Ca behave conservatively in rivers after their release from carbonates, provides an upper limit on the U contribution from these carbonates, to be a few percent of dissolved uranium in rivers. There are, however, a few streams with low uranium concentrations, for which the carbonate contribution could be much higher. These results suggest that Precambrian carbonates make only minor contributions to the uranium budget of the Ganga-Indus headwaters in the Himalaya on a basin wide scale, however, they could be important for particular streams. Similar estimates of silicate contribution to uranium budget of these rivers using U/Na in silicates and Na* (Na corrected for cyclic and halite contributions) in river waters show that silicates can contribute significantly (approximately 40% on average) to their U balance. If, however, much of the uranium in these silicates is associated with weathering resistant minerals, then the estimated silicate uranium component would be upper limits. Uranium concentration in black shales averages about 37 microg g(-1). Based on this concentration, supply of U from at least approximately 50 mg of black shales per liter of river water is needed to balance the average river water U concentration, 1.7 microg L

  11. Accurate fast method with high chemical yield for determination of uranium isotopes (234U, 235U, 238U) in granitic samples using alpha spectroscopy

    NASA Astrophysics Data System (ADS)

    Guirguis, Laila A.; Farag, Nagdy M.; Salim, Adham K.

    2015-03-01

    The present study aims to use the α-spectroscopy at Nuclear Materials Authority (NMA) of Egypt. A radiochemical technique for analysis uranium isotopes was carried out for ten mineralized granitic samples together with the International standards RGU-1 (IAEA) and St4 (NMA). Several steps of sample preparation, radiochemical separation and source preparation were performed before analysis. Uranium was separated from sample matrix with 0.2 M TOPO in cyclohexane as an extracting agent with a chemical yield 98.95% then uranium was purified from lanthanides and actinides present with 0.2 M TOA in xylene as an extracting agent. The pure fraction was electrodeposited on a mirror-polished copper disc from buffer solution (NaHSO4+H2SO4+NH4OH). Rectangle pt-electrode with an anode-cathode distance of 2 cm was used. Current was 900 mA and the electrodeposition time reach up to 120 min. The achieved results show that the chemical yield ranged between 87.9±6.8 and 98±8.6.

  12. The applicability of MGA method for depleted and natural uranium isotopic analysis in the presence of actinides (232Th, 237Np, 233Pa and 241Am).

    PubMed

    Yücel, Haluk

    2007-11-01

    The multi-group analysis (MGA) method for the determination of uranium isotopic abundances in depleted uranium (DU) and natural uranium (NU) samples is applied in this study. A set of non-destructive gamma-ray measurements of DU and NU samples were performed using a planar Ge detector. The relative abundances of 235U and 238U isotopes were compared with the declared values of the standards. The relative abundance for 235U obtained by MGA for a "clean" DU or NU sample with a content of uranium>1wt% is determined with an accuracy of about +/-5%. However, when several actinides such as 232Th, 237Np, 233Pa and 241Am are present along with uranium isotopes simulating "dirty" DU or NU, it has been observed that MGA method gives erroneous results. The 235U abundance results for the samples were 6-25 times higher than the declared values in the presence of above-mentioned actinides, since MGA is utilized the X-ray and gamma-ray peaks in the 80-130 keV energy region, covering XKalpha and XKbeta regions. After the least-squares fitting of the spectra, it is found that the increases in the intensities of the X-ray and gamma-ray peaks of uranium are remarkably larger in the complex 80-130 keV region. On the other hand, it is observed that the interferences of the actinide peaks are relatively less dominant in the higher gamma-ray region of 130-300 keV. The results imply the need for dirty DU and NU samples that the MGA method should utilize the higher energy gamma-rays (up to 1001 keV of (234m)Pa) combined with lower energies of the spectra, which may be collected in a two detector mode (a planar Ge and a high efficient coaxial Ge).

  13. Nuclear excitation by electronic transition of 235U

    DOE PAGES

    Chodash, P. A.; Norman, E. B.; Burke, J. T.; ...

    2016-03-11

    Here, nuclear excitation by electronic transition (NEET) is a rare nuclear excitation that can occur in isotopes containing a low-lying nuclear excited state. Over the past 40 yr, several experiments have attempted to measure NEET of 235U and those experiments have yielded conflicting results.

  14. High-Resolution Inductively Coupled Plasma Optical Emission Spectrometry for (234)U/(238)Pu Age Dating of Plutonium Materials and Comparison to Sector Field Inductively Coupled Plasma Mass Spectrometry.

    PubMed

    Krachler, Michael; Alvarez-Sarandes, Rafael; Rasmussen, Gert

    2016-09-06

    Employing a commercial high-resolution inductively coupled plasma optical emission spectrometry (HR-ICP-OES) instrument, an innovative analytical procedure for the accurate determination of the production age of various Pu materials (Pu powder, cardiac pacemaker battery, (242)Cm heat source, etc.) was developed and validated. This undertaking was based on the fact that the α decay of (238)Pu present in the investigated samples produced (234)U and both mother and daughter could be identified unequivocally using HR-ICP-OES. Benefiting from the high spectral resolution of the instrument (<5 pm) and the isotope shift of the emission lines of both nuclides, (234)U and (238)Pu were selectively and directly determined in the dissolved samples, i.e., without a chemical separation of the two analytes from each other. Exact emission wavelengths as well as emission spectra of (234)U centered around λ = 411.590 nm and λ = 424.408 nm are reported here for the first time. Emission spectra of the isotopic standard reference material IRMM-199, comprising about one-third each of (233)U, (235)U, and (238)U, confirmed the presence of (234)U in the investigated samples. For the assessment of the (234)U/(238)Pu amount ratio, the emission signals of (234)U and (238)Pu were quantified at λ = 424.408 nm and λ = 402.148 nm, respectively. The age of the investigated samples (range: 26.7-44.4 years) was subsequently calculated using the (234)U/(238)Pu chronometer. HR-ICP-OES results were crossed-validated through sector field inductively coupled plasma mass spectrometry (SF-ICPMS) analysis of the (234)U/(238)Pu amount ratio of all samples applying isotope dilution combined with chromatographic separation of U and Pu. Available information on the assumed ages of the analyzed samples was consistent with the ages obtained via the HR-ICP-OES approach. Being based on a different physical detection principle, HR-ICP-OES provides an alternative strategy to the well-established mass

  15. Neutron Capture Cross Sections of 236U and 234U

    SciTech Connect

    Rundberg, R. S.; Bredeweg, T. A.; Bond, E. M.; Haight, R. C.; Hunt, L. F.; O'Donnell, J. M.; Schwantes, J. M.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wouters, J. M.; Kronenberg, A.

    2006-03-13

    Accurate neutron capture cross sections of the actinide elements at neutron energies up to 1 MeV are needed to better interpret archived nuclear test data, for post-detonation nuclear attribution, and the Advanced Fuel Cycle Initiative. The Detector for Advance Neutron Capture Experiments, DANCE, has unique capabilities that allow the differentiation of capture gamma rays from fission gamma rays and background gamma rays from scattered neutrons captured by barium isotopes in the barium fluoride scintillators. The DANCE array has a high granularity, 160 scintillators, high efficiency, and nearly 4-{pi} solid angle. Through the use of cuts in cluster multiplicity and calorimetric energy the capture gamma-rays are differentiated from other sources of gamma rays. The preliminary results for the capture cross sections of 236U are in agreement with the ENDF/B-VI evaluation. The preliminary results for 234U lower are than ENDF/B-VI evaluation and are closer to older evaluations.

  16. Impact of the 235U Covariance Data in Benchmark Calculations

    SciTech Connect

    Leal, Luiz C; Mueller, Don; Arbanas, Goran; Wiarda, Dorothea; Derrien, Herve

    2008-01-01

    The error estimation for calculated quantities relies on nuclear data uncertainty information available in the basic nuclear data libraries such as the U.S. Evaluated Nuclear Data File (ENDF/B). The uncertainty files (covariance matrices) in the ENDF/B library are generally obtained from analysis of experimental data. In the resonance region, the computer code SAMMY is used for analyses of experimental data and generation of resonance parameters. In addition to resonance parameters evaluation, SAMMY also generates resonance parameter covariance matrices (RPCM). SAMMY uses the generalized least-squares formalism (Bayes method) together with the resonance formalism (R-matrix theory) for analysis of experimental data. Two approaches are available for creation of resonance-parameter covariance data. (1) During the data-evaluation process, SAMMY generates both a set of resonance parameters that fit the experimental data and the associated resonance-parameter covariance matrix. (2) For existing resonance-parameter evaluations for which no resonance-parameter covariance data are available, SAMMY can retroactively create a resonance-parameter covariance matrix. The retroactive method was used to generate covariance data for 235U. The resulting 235U covariance matrix was then used as input to the PUFF-IV code, which processed the covariance data into multigroup form, and to the TSUNAMI code, which calculated the uncertainty in the multiplication factor due to uncertainty in the experimental cross sections. The objective of this work is to demonstrate the use of the 235U covariance data in calculations of critical benchmark systems.

  17. 234U /238U and 230Th /234U activity ratios in mineral phases of a lateritic weathered zone

    NASA Astrophysics Data System (ADS)

    Lowson, Richard T.; Short, Stephen A.; Davey, Brian G.; Gray, David J.

    1986-08-01

    A selective phase extraction procedure was developed for the identification of the significant phases of a typical deep soil profile sampled in the vicinity of the Ranger No. 1 uranium ore body, Alligator Rivers region, N.T., Australia. The significant phases were identified as amorphous iron oxide, crystalline iron oxide and a clay/quartz resistate. The distribution of 238U, 234U, 230Th and 226Ra between the phases was measured. The results indicated that the amorphous iron oxide phase is in adsorption/desorption equilibrium with the ground water. The crystalline iron oxide phase contains a chemical control, the kinetics of which are commensurate with or less than the half-life of 230Th (7.52 × 10 4 y). The clay/quartz resistate is enriched in 238U descendants in such a way that they are not readily accessible to the ground water.

  18. Concentrations of (226)Ra, (232)Th and (4)(0)K in industrial kaolinized granite.

    PubMed

    Todorović, Nataša; Hansman, Jan; Mrđa, Dušan; Nikolov, Jovana; Kardos, Richárd; Krmar, Miodrag

    2017-03-01

    Activity concentrations of (226)Ra, (232)Th and (4)(0)K in 120 kaolinized granite samples imported in Serbia from the Motajica mine, Bosnia and Herzegovina, were measured. The (226)Ra concentration ranged from 61 to 319 Bq kg(-1), the (232)Th from 44 to 272 Bq kg(-1), and the (4)(0)K from 590 to 1470 Bq kg(-1). The frequency distribution of (4)(0)K concentrations was near-Gaussian, where those of (226)Ra and (232)Th were right-skewed. In 6 samples, the gamma index, I, was higher than 2, which exceeds the exemption dose criterion (0.3 mSv y(-1)). The absorbed dose rate and annual effective doses for workers in the ceramic industries in Serbia who worked with kaolinized granite were below levels of concern.

  19. (234)U/(238)U signatures associated with uranium ore bodies: part 3 Koongarra.

    PubMed

    Lowson, Richard T

    2013-04-01

    The Koongarra ore body is an early Proterozoic U ore body in the Alligator Rivers U province, Northern Territory, Australia. It has surface expression with a redox front located ∼30 m below the surface. The (234)U/(238)U activity ratios (AR) for the ground water and the amorphous phase of the solid have been analysed for the ore zone and dispersion halo as a function of depth. The results display a (234)U/(238)U AR signature with depth which may be common to all U ore bodies. The (234)U/(238)U AR is depressed below secular equilibrium in the weathered material above the redox front; rises significantly above secular equilibrium in the vicinity of the redox front; and is followed by a gradual decrease with depth below the redox front. The amplitude of the profile is a function of local conditions. A model is proposed for the signature in which oxidising waters preferentially leach the (234)U sites at the redox front due to preconditioning of the (234)U sites by α recoil during the decay of (23)(8)U to (23)(4)U. Mass balance requires the solid material left behind the redox front to have a (234)U/(238)U AR reduced below 1. Local second order effects may be superimposed on the signature. The signature may have application to calibrating scenarios for nuclear waste repositories, assisting in understanding historical climates, economic evaluation of U ore bodies and U exploration.

  20. Dating ivory by determination of 14C, 90Sr and 228/232Th.

    PubMed

    Schmied, Stefanie A K; Brunnermeier, Matthias J; Schupfner, Robert; Wolfbeis, Otto S

    2012-09-10

    A method is described to determine the time of death of elephants. This is accomplished by analysis of the radionuclides 14C, 90Sr and 228/232Th in known samples of ivory, and in samples of unknown age. The reliability of this method is considerably increased by multi nuclide analysis.

  1. Evaluation of the thermal-neutron constants for /sup 233/U, /sup 235/U, /sup 239/Pu and /sup 241/Pu

    SciTech Connect

    Stehn, J.R.; Divadeenam, M.; Holden, N.E.

    1982-01-01

    A consistent set of best values of the 2200 meter/second neutron cross sections, Westcott g-factors, and fission neutron yields for /sup 233/U, /sup 235/U, /sup 239/Pu and /sup 241/Pu are presented. A least squares fitting program, LSF, is used to obtain the best fit and to estimate the sensitivity of these fissile parameters to the quoted uncertainties in experimental data. The half-lives of the uranium and plutonium nuclides have been evaluated and these have been used to reassess the significant experimental data. The latest revision of the spontaneous fission neutron yield anti nu, of /sup 252/Cf and the foil thickness corrections to the fission neutron yield ratios of fissile nuclei to /sup 252/Cf are included. These lead to greater consistency in the data used for anti nu (/sup 252/Cf). Similarly, the /sup 234/U half-life as revised leads to improved consistency in the /sup 235/U fission cross section. Comparison is made with the values from ENDF/B-V and other evaluations.

  2. Impact of the 235U series on doses from intakes of natural uranium and decay progeny.

    PubMed

    Lowe, L M

    1997-10-01

    The doses from 235U series radionuclides have often been ignored in dose assessments involving natural uranium and progeny. This is due to the relatively low abundance of 235U in natural uranium (less than 5% on an activity basis). However, inclusion of the 235U series radionuclides, especially 227Ac and 231Pa, in dose calculations can have a substantial impact on estimated inhalation doses.

  3. (234)U/(238)U signatures associated with uranium ore bodies: part 1 Ranger 3.

    PubMed

    Lowson, Richard T; McIntyre, Mark G

    2013-04-01

    The Ranger 3 ore body is an early Proterozoic U ore body in the Alligator Rivers U province, Northern Territory, Australia. It has surface expression with a redox front located between 30 and 50 m below the surface. The ground water U concentration and (234)U/(238)U AR signature in the top 10 m of the weathered zone are reported for 357 samples collected over 4 wet seasons, at 5 depths, along a transect in-line with the hydraulic gradient and along the centre line of the ore body and its associated dispersion halo. The results show that the weathered zone displays a general U isotope feature for this type of ore body with the (234)U/(238)U AR for the ground water and amorphous phase of the solid matrix being less than 1. The ground water (234)U/(238)U AR is independent of the annual monsoonal climate and depth within the range surface to 10 m. In the vicinity of the U ore body the ground water (234)U/(238)U AR is 0.75 and is very similar to the (234)U/(238)U AR of the amorphous phase of the solid (0.76). The (234)U/(238)U ARs of the amorphous phase and ground water rise and separate to values of 0.88 and 1.02 at the end of the transect. The rise and separation in (234)U/(238)U AR are interpreted as evidence that the source of the U in the ground water is from the water-soluble sub-phase of the amorphous phase and that the ground water flow is too fast to allow the processes occurring across the solid-water interface to reach chemical equilibrium. The data set is a robust characterisation of the coarse and fine detail of the (234)U/(238)U AR signature in the weathered zone of U ore bodies.

  4. (234)U/(238)U signatures associated with uranium ore bodies: part 2 Manyingee.

    PubMed

    Lowson, Richard T; McIntyre, Mark G

    2013-04-01

    The Manyingee ore body is a roll-front U ore body located at depth in the Cretaceous sandstone sediments of a Proterozoic palaeo valley. It is located in a confined aquifer. The aquifer is recharged 4 km upstream by the Ashburton River. Groundwater samples were collected at and up to 4.7 km downstream of the ore body. The ground water (234)U/(238)U activity ratios (AR) were elevated to 1.86 in the vicinity of the ore body and then declined to 1.06 over the 4.7 km transect. The elevated (234)U/(238)U ARs are attributed to selective leaching of (234)U sites by oxidising waters, with α recoil as a necessary precursor to produce activated (234)U sites. Direct ejection into another phase following α recoil is considered to be a minor contributor to (234)U -(238)U disequilibrium in this environment. The profile is considered to be typical of the (234)U/(238)U AR profile at and down gradient of the redox front of a U ore body.

  5. Ocean mixing and ice-sheet control of seawater 234U/238U during the last deglaciation

    NASA Astrophysics Data System (ADS)

    Chen, Tianyu; Robinson, Laura F.; Beasley, Matthew P.; Claxton, Louis M.; Andersen, Morten B.; Gregoire, Lauren J.; Wadham, Jemma; Fornari, Daniel J.; Harpp, Karen S.

    2016-11-01

    Seawater 234U/238U provides global-scale information about continental weathering and is vital for marine uranium-series geochronology. Existing evidence supports an increase in 234U/238U since the last glacial period, but the timing and amplitude of its variability has been poorly constrained. Here we report two seawater 234U/238U records based on well-preserved deep-sea corals from the low-latitude Atlantic and Pacific Oceans. The Atlantic 234U/238U started to increase before major sea-level rise and overshot the modern value by 3 per mil during the early deglaciation. Deglacial 234U/238U in the Pacific converged with that in the Atlantic after the abrupt resumption of Atlantic meridional overturning. We suggest that ocean mixing and early deglacial release of excess 234U from enhanced subglacial melting of the Northern Hemisphere ice sheets have driven the observed 234U/238U evolution.

  6. [Cytogenetic effects of separate and combined action of 232Th and Cd nitrates on Allum cepa root meristem cells].

    PubMed

    Evseeva, T I; Geras'kin, S A; Khramova, E S

    2001-01-01

    Effects of separate and combined action of 232Th and Cd on Allium cepa root tip cells were investigated. It has been shown that cytogenetic effects of 232Th results mainly from its ability to induce genome damages. Cadmium in the examined concentration does not induce chromosomal vagrants, and this effect is not intensified by the combined action of 232Th and Cd (with 232Th). Cd induced increased aberrations of chromosome type frequency (1.5 times more than in control group), and fragment frequence, while mitotic index was significantly decreased. While taking into consideration the frequency of anaphase--telophase damages, and the number of aberrations per cell, the combined effects of 232Th and Cd may be considered as synergic. The aberration type ratio, frequencies of bridges and fragments, and also the level of proliferative activity of 232Th and Cd in the presence of both ions were similar with the corresponding parameters obtained when Cd acted alone. Possible mechanisms of formation of 232Th and Cd synergic effects are discussed.

  7. Study of contents of 226Ra, 232Th and 40K in fertilisers.

    PubMed

    Tahir, S N A; Alaamer, A S; Omer, R M

    2009-02-01

    In this study concentrations of naturally occurring radionuclides (226)Ra, (232)Th and (40)K were measured in the fertiliser samples in Pakistan using a high-resolution and high-purity germanium detector. Samples were collected from main fertiliser depots located in 10 big cities in the Punjab province. Gamma spectrometric analysis revealed that concentrations of (226)Ra, (232)Th and (40)K existed in the ranges from 232 to 511 Bq kg(-1), 21 to 58 Bq kg(-1) and 556 to 1302 Bq kg(-1) with average values of 386 +/- 92, 38 +/- 14 and 885 +/- 220 Bq kg(-1), respectively. Average values of the three natural radionuclides measured in this study were within the range of reported values from some of the other countries of the world. Correlations drawn between measured concentrations were not significant.

  8. Ultra Sensitive Neutron Activation Measurements of {sup 232}Th in Copper

    SciTech Connect

    Clemenza, M.; Previtali, E.; Borio di Tigliole, A.; Salvini, A.

    2011-04-27

    Copper, thanks to its low content in radioactive contaminations, is a material widely used for shielding, holders and other objects close to the sensitive parts of the detectors in many experiments in rare event physics. This implies that tools able to reach sensitivity of the order of <10{sup -12} gram of contaminants per gram of copper are of crucial importance. A methodology based in Neutron Activation Analysis (NAA) has been developed to obtain an extremely high sensitivity in the analysis of {sup 232}Th in copper samples. A detection limit of 5x10{sup -13} g {sup 232}Th/g Cu has been achieved through the irradiation of 200 g of copper sample which subsequently was radio-chemically concentrated using nitric acid and then actinide resin from Eichrom Inc. Several elutions were performed with various inorganic acids to concentrate the {sup 232}Th activation product ({sup 233}Pa) from the copper matrix and to also eliminate the radioactive background induced by the neutron bombardment to reach higher sensitivity.

  9. Measurement of (233)U/(234)U ratios in contaminated groundwater using alpha spectrometry.

    PubMed

    Harrison, Jennifer J; Payne, Timothy E; Wilsher, Kerry L; Thiruvoth, Sangeeth; Child, David P; Johansen, Mathew P; Hotchkis, Michael A C

    2016-01-01

    The uranium isotope (233)U is not usually observed in alpha spectra from environmental samples due to its low natural and fallout abundance. It may be present in samples from sites in the vicinity of nuclear operations such as reactors or fuel reprocessing facilities, radioactive waste disposal sites or sites affected by clandestine nuclear operations. On an alpha spectrum, the two most abundant alpha emissions of (233)U (4.784 MeV, 13.2%; and 4.824 MeV, 84.3%) will overlap with the (234)U doublet peak (4.722 MeV, 28.4%; and 4.775 MeV, 71.4%), if present, resulting in a combined (233+234)U multiplet. A technique for quantifying both (233)U and (234)U from alpha spectra was investigated. A series of groundwater samples were measured both by accelerator mass spectrometry (AMS) to determine (233)U/(234)U atom and activity ratios and by alpha spectrometry in order to establish a reliable (233)U estimation technique using alpha spectra. The Genie™ 2000 Alpha Analysis and Interactive Peak Fitting (IPF) software packages were used and it was found that IPF with identification of three peaks ((234)U minor, combined (234)U major and (233)U minor, and (233)U major) followed by interference correction on the combined peak and a weighted average activity calculation gave satisfactory agreement with the AMS data across the (233)U/(234)U activity ratio range (0.1-20) and (233)U activity range (2-300 mBq) investigated. Correlation between the AMS (233)U and alpha spectrometry (233)U was r(2) = 0.996 (n = 10).

  10. Uranium isotope systematics of ferromanganese crusts in the Pacific Ocean: Implications for the marine 238U/235U isotope system

    NASA Astrophysics Data System (ADS)

    Goto, Kosuke T.; Anbar, Ariel D.; Gordon, Gwyneth W.; Romaniello, Stephen J.; Shimoda, Gen; Takaya, Yutaro; Tokumaru, Ayaka; Nozaki, Tatsuo; Suzuki, Katsuhiko; Machida, Shiki; Hanyu, Takeshi; Usui, Akira

    2014-12-01

    Variations of 238U/235U ratio (δ238U) in sedimentary rocks have been proposed as a possible proxy for the paleo-oceanic redox conditions, although the marine δ238U system is not fully understood. Here we investigate the spatial variation of δ238U in modern ferromanganese (Fe-Mn) crusts by analyzing U isotopes in the surface (0-3 mm depth) layer of 19 Fe-Mn crusts collected from 6 seamounts in the Pacific Ocean. δ238U values in the surface layers show little variation and range from -0.59‰ to -0.69‰. The uniformity of δ238U values is consistent with the long residence time of U in modern seawater, although the δ238U values are lighter than that of present-day seawater by ∼0.24‰. The light δ238U values are consistent with the isotope offset observed in previously reported adsorption experiment of U to Mn oxide. These results indicate that removal of U from seawater to Mn oxide is responsible for the second largest U isotope fractionation in the modern marine system, and could contribute to isotopically heavy U to seawater. Depth profiles of U isotopes (δ234U and δ238U) in two Fe-Mn crusts (MR12-03_D06-R01 and MC10_CB07_B), dated by Os isotope stratigraphy, were investigated to reconstruct the evolution of the oceanic redox state during the Cenozoic. The δ238U depth profiles show very limited ranges (-0.57‰ to -0.67‰ for MR12-03_D06-R01 and -0.56‰ to -0.69‰ for MC10_CB07_B), and have values that are similar to those of the surface layers of Fe-Mn crusts. The absence of any resolvable variation in the δ238U depth profiles may suggest that the relative amounts of oxic and reducing U sinks have not varied significantly over the past 45 Myr. However, the δ234U depth profiles of the same samples show evidence for the possible redistribution of 234U after deposition. Therefore, the depth profile of δ238U in Fe-Mn crusts may have been also overprinted by later chemical exchange with pore-water or seawater, and may not reflect the paleo

  11. Determination of 235U/238U Ratio on Urine by ICP-MS

    SciTech Connect

    Collins, L; Gobaleza, A; Langston, R; Radev, R; Than, C; Wong, C; Wood-Zika, A

    2011-10-19

    LLNL Internal Dosimetry Program - The new procedure satisfies the requirement to determine {sup 235}U/{sup 238}U ratio in bioassay urine samples. MDA - The L{sub C} and MDA{sub 95} for {sup 235}U are well below the required detection limit of 0.00035 {mu}g/L. Turn around time - Analysis of 10 samples plus 2 QCs can be completed in one work day (8 hours).

  12. Studies of positron electron pair production in {sup 238}U + {sup 232}Th

    SciTech Connect

    Ahmad, I.; Back, B.B.; Betts, R.R.

    1995-08-01

    Following the non-observation of sharp sum-energy lines in our earlier {sup 238}U + {sup 181}Ta measurements, it was decided to pursue measurements of the {sup 238}U + {sup 232}Th system which, in the previously published work, showed the most striking evidence for near-equal-energy back-to-back pairs leading to sharp sum-energy lines. Following the refurbishing of the APEX silicon arrays and extensive tests of the rotating target wheel assembly, a major positron run took place in November 1994. Rolled 1-mg/cm{sub 2} {sup 232}Th targets were bombarded with 5.95-MeV/u {sup 238}U. The target rotation allowed up to 2 pnA of beam to be used without serious deterioration of the targets. Over 300,000 pairs were accumulated, representing an order-of-magnitude improvement in statistics over the previously published results. Preliminary analysis shows no evidence for the sharp lines at a cross section level orders of magnitude below those previously reported. The analysis of these data is currently being completed in preparation for publication.

  13. The low-energy dipole structure of 232Th , 236U and 238U actinide nuclei

    NASA Astrophysics Data System (ADS)

    Kuliev, A. A.; Guliyev, E.; Ertugral, F.; Özkan, S.

    2010-03-01

    In this study, ensuremath I^{π} = 1+ and ensuremath I^{π} = 1- dipole mode excitations are systematically investigated within the rotational and translational + Galilean invariant quasiparticle random-phase approximation for 232Th , 236U , and 238U actinide nuclei. It is shown that the investigated nuclei reach a B( M1) strength structure, which corresponds to the scissors mode. The calculated mean excitation energies as well as the summed B( M1) value of the scissors mode excitations are consistent with the available experimental data. The results of calculations indicate large differences to the rare-earth nuclei as is the case for the experiment: a doubling of the observed dipole strengths and a shift of the energy centroid to the lower energies by about 800keV. The calculations indicate the presence of a few prominent negative-parity ensuremath K^{π} = 1- states in the 2.0-4.0MeV energy interval. The occurrence of the negative-parity dipole states with the rather high B( E1) value less than 4MeV shows the necessity of explicit parity measurements for the correct determination of the scissors mode strength in 232Th , 236U , and 238U isotopes.

  14. The Application of 238U/235U as a Redox-Proxy for Past Ocean Chemistry

    NASA Astrophysics Data System (ADS)

    Andersen, M. B.; Westermann, S.; Bahniuk, A.; Vasconcelos, C.; McKenzie, J. A.; Föllmi, K. B.; Vance, D.

    2014-12-01

    The recent discovery of significant variation in 238U/235U caused by redox change at the surface Earth has led to its use to extract information on the oxygenation state of ancient oceans from marine sediments [e.g. 1]. Recent studies have focused on improving the understanding of the 238U/235U signature in modern marine carbonates [2] and black shales [3] to improve the robustness of this tracer. To further advance its use we have focused on improving our understanding of 238U/235U systematics in modern dolomite, another commonly occurring rock-type in the geological record, before turning to 238U/235U signatures in ancient sediments. The measured dolomite samples, precipitated in modern environments of coastal hypersaline lagoons in Brazil, all exhibit 238U/235U values that deviate from the seawater composition [3]. Observed values are both lighter (ca. 130 ppm; as also observed in dolomite from tidal-ponds on Bahamas [2]) and heavier (50-180 ppm). These distinct 238U/235U values for different dolomite-precipitates likely attest to the particular formation style, as well as early diagenetic processes. We use such modern settings to discuss the utility of 238U/235U in ancient sediments, the singularity of any observed 238U/235U signal, its relation to global ocean chemistry and potential diagenetic overprinting. These constraints are then used to evaluate a well-preserved marine carbonate section [4] and published black shale 238U/235U data [1], both deposited during the Oceanic Anoxic Event 2 (93 Ma). We discuss the capabilities of both the carbonate and black shale section for retaining information on the 238U/235U composition in the ocean during OAE 2. [1] Montoya-Pino et al. (2010) Geology, 38, 315-318 [2] Romaniello et al. (2013) 362, 305-316 [3] Andersen et al. (2014) EPSL, 400, 184-194 [4] Westermann et al. (2010) Cret. Res., 31, 500-514

  15. 232Th(n,{gamma})233Th Thermal Reaction Cross-Section Measurement

    SciTech Connect

    Maidana, Nora L.; Vanin, Vito R.; Pascholati, Paulo R.; Helene, Otaviano; Castro, Ruy M.; Dias, Mauro S.; Koskinas, Marina F.

    2005-05-24

    The 232Th(n,{gamma})233Th thermal neutron-capture reaction cross section was measured using targets of {approx} 1.5 mg of high-purity metallic thorium irradiated in the IPEN IEA-R1m 5 MW pool research reactor. The 197Au(n,{gamma})198Au reaction was used to monitor the thermal and epithermal neutron fluxes in the irradiation position, which was found using the Westcott formalism. The residual gamma-ray activity was followed with an HPGe detector. The detector efficiency curve was fitted by the least-squares method applying covariance analysis to all uncertainties involved. The experimental result is {sigma}0 =7.20{+-}0.20 b, in agreement with previous published values.

  16. Systematics of the mean energy and the mean multiplicity of prompt neutrons originating from {sup 232}Th fission

    SciTech Connect

    Svirin, M. I.

    2012-12-15

    The cross section for the neutron-induced fission of {sup 232}Th target nuclei, {sigma}{sub f} (E{sub n}), was described within statistical theory. The spectra of the mean multiplicity, v-bar (E{sub n}), and the mean energy, E-bar(E{sub n}), of secondary neutrons accompanying {sup 232}Th fission induced by neutrons of energy extending up to E{sub n} = 20 MeV were analyzed on the basis of the chance structure of the cross section.

  17. Relative {sup 235}U(n,{gamma}) and (n,f) cross sections from {sup 235}U(d,p{gamma}) and (d,pf)

    SciTech Connect

    Allmond, J.M.; Bernstein, L.A.; Beausang, C.W.; Phair, L.; Bleuel, D.L.; Burke, J.T.; Escher, J.E.; Evans, K.E.; Goldblum, B.L.; Hatarik,, R.; Jeppesen, H.B.; Rasmussen, J.O.

    2009-01-01

    The internal surrogate ratio method allows for the determination of an unknown cross section, such as (n,{gamma}), relative to a better-known cross section, such as (n,f), by measuring the relative exit-channel probabilities of a surrogate reaction that proceeds through the same compound nucleus. The validity of the internal surrogate ratio method is tested by comparing the relative gamma and fission exit-channel probabilities of a {sup 236}U* compound nucleus, formed in the {sup 235}U(d,p) reaction, to the known {sup 235}U(n,{gamma}) and (n,f) cross sections. A model-independent method for measuring the gamma-channel yield is presented and used.

  18. Round-robin 230Th–234U age dating of bulk uranium for nuclear forensics

    DOE PAGES

    Gaffney, Amy M.; Hubert, Amélie; Kinman, William S.; ...

    2015-07-30

    In an inter-laboratory measurement comparison study, four laboratories determined 230Th–234U model ages of uranium certified reference material NBL U050 using isotope dilution mass spectrometry. The model dates determined by the participating laboratories range from 9 March 1956 to 19 October 1957, and are indistinguishable given the associated measurement uncertainties. As a result, these model ages are concordant with to slightly older than the known production age of NBL U050.

  19. Isotope ratios of (235)U/(238)U and (137)Cs/(235)U in black rain streaks on plaster wall caused by fallout of the Hiroshima atomic bomb.

    PubMed

    Shizuma, Kiyoshi; Endo, Satoru; Fujikawa, Yoko

    2012-02-01

    Radiological investigations of fallout from the atomic bomb detonated over Hiroshima city on 6 August 1945 are important to estimate doses for inhabitants. The authors have analyzed the concentrations of (137)Cs, (235)U, and (238)U in streaks of black rain caused by the atomic bomb using gamma-ray spectroscopy and the ICP-QMS method. The black rain streaks were deposited on a plaster wall of a house located 3.7 km west of the hypocenter that has been kept in the same condition as after the rainfall. Cesium-137 ((137)Cs) was detected from black streak samples. Concentration of (137)Cs in the black rain streaks is twice as high as fallout deposition on the ground in this area. A (235)U/(238)U atom ratio of 0.00887 was found, which is higher than the natural ratio, reflecting the fact that the atomic bomb "Little Boy" used enriched uranium as fuel. The ratio (137)Cs/(235)U was determined to be 0.0091, which is about eight times higher than the estimated ratio of 0.00113 based on the fission yield.

  20. Precise determination of the 235U reactor antineutrino cross section per fission

    NASA Astrophysics Data System (ADS)

    Giunti, C.

    2017-01-01

    We investigate which among the reactor antineutrino fluxes from the decays of the fission products of 235U, 238U, 239Pu, and 241Pu may be responsible for the reactor antineutrino anomaly if the anomaly is due to a miscalculation of the antineutrino fluxes. We find that it is very likely that at least the calculation of the 235U flux must be revised. From the fit of the data we obtain the precise determination σ235 = (6.33 ± 0.08) ×10-43cm2 /fission of the 235U cross section per fission, which is more precise than the calculated value and differs from it by 2.2σ. The cross sections per fission of the other fluxes have large uncertainties and in practice their values are undetermined by the fit.

  1. Retroactive covariance matrix for {sup 235}U in the resolved-resonance region

    SciTech Connect

    Arbanas, G.; Leal, L. C.; Larson, N. M.; Derrien, H.

    2006-07-01

    For the first time, a resonance-parameter covariance matrix (RPCM) has been generated for {sup 235}U in the resolved resonance region. The method used to produce this RPCM is the retroactive approach of the SAMMY code [1]. As reported elsewhere [2], a Reich-Moore resonance evaluation for {sup 235}U had been performed in the energy range between 0 and 2.25 keV using SAMMY; a total of 3193 resonances, including the external levels, were identified. At the time that the evaluation was performed, the complete RPCM was not generated because of computer memory and storage limitations [3]. Subsequently, a procedure for retroactively creating RPCMs has been developed and implemented in the SAMMY code. This procedure is used to generate the RPCM for the {sup 235}U parameters of the ENDF/B-VI evaluation. (authors)

  2. Distinguishing fissions of ^239Pu and ^235U with low-resolution detectors

    NASA Astrophysics Data System (ADS)

    Swanberg, E.; Norman, E. B.; Prussin, S. G.; Shugart, H.; Browne, E.

    2008-10-01

    When ^239Pu and ^235U undergo thermal neutron-induced fission, both produce significant numbers of β-delayed gamma rays with energies in the several MeV range. Experiments using high energy-resolution germanium detectorsootnotetextR. E. Marrs et al., Nucl. Instr. & Meth. A (in press). have shown that it is possible to distinguish the fission of ^239Pu from that of ^235U. Using differences in the temporal behavior and in the shapes of the gamma-ray energy spectra, we show that these two isotopes can also be differentiated using low-resolution plastic or liquid scintillators. It is likely this method could be extended to homeland security applications, such as screening of cargo containers for ^235U and ^239Pu, using a neutron source and such scintillators.

  3. A contribution to improvement of the nuclear data concerning alpha decay of 235U

    NASA Astrophysics Data System (ADS)

    Dayras, Fatima; Chauvin, Nicolas

    2004-09-01

    Compared to other alpha-particle emitting nuclides, for those with long half-lives (T1/2 > 106 years), there is generally some inconsistency and inaccuracy in the associated nuclear data. However, these radionuclides play a major role in modern society and, for a number of reasons, are the subject of widespread interest. The study of their alpha decay, which is more difficult than in the case of the other nuclides, enables knowledge of their nuclear data to be increased. In the present paper, we accordingly consider one of the most well known ones: 235U. Using a quasi mono-isotopic deposit of 235U obtained by electromagnetic separation, we have studied the alpha-particle decay of 235U using a high-energy resolution spectrometer developed in our laboratory. The stability of the spectrometer made it possible to perform long measurements which is crucial in the case of 235U. The Colégram program, with a new fit criterion to better take into account peaks of low statistical significance, was used to extract the data (alpha-particle emission probabilities and energies). Monte-Carlo simulations carried out in the context of this work were also used to corroborate the data obtained. Finally, thirteen alpha-particle emissions from 235U were measured, from which only ten were previously observed and measured. This work has substantially reduced the uncertainty concerning alpha-particle emission probability and energy values and has resolved some of the ambiguities concerning the 235U disintegration scheme to 231Th.

  4. High precision {sup 230}Th and {sup 232}Th in the Norwegian Sea and Denmark by thermal ionization mass spectrometry

    SciTech Connect

    Moran, S.B.; Hoff, J.A.; Edwards, R.L.

    1995-10-01

    Seawater samples (1-2 liters) were collected from the Norwegian Sea and Denmark Strait and analyzed for {sup 230}Th and {sup 232}Th using highly sensitive thermal ionization mass spectrometry (TIMS). Depth profiles of dissolved {sup 230}Th and {sup 232}Th are characterized by surface water minima (<1 fg/kg, <5 pg/kg), subsurface maxima (12 fg/kg, 134 pg/kg), and intermediate concentrations that progressively decrease toward the bottom ({approximately}5 fg/kg, {approximately}17 pg/kg), respectively. The lack of an increase in {sup 230}Th with depth is suggested to result from the short ventilation age of Norwegian Sea Deep Water combined with enhanced scavenging near the basin margins. The {sup 230}Th maximum is attributed to advection of high {sup 230}Th in the Arctic Intermediate Water, whereas the {sup 232}Th maximum may he related to a particulate source. The low dissolved {sup 230}Th and {sup 232}Th concentrations observed in the NADW formation regions implies a minor advective export of these long-lived Th tracers to the North Atlantic. 24 refs., 1 fig., 1 tab.

  5. Verification of 235U mass content in nuclear fuel plates by an absolute method

    NASA Astrophysics Data System (ADS)

    El-Gammal, W.

    2007-01-01

    Nuclear Safeguards is referred to a verification System by which a State can control all nuclear materials (NM) and nuclear activities under its authority. An effective and efficient Safeguards System must include a system of measurements with capabilities sufficient to verify such NM. Measurements of NM using absolute methods could eliminate the dependency on NM Standards, which are necessary for other relative or semi-absolute methods. In this work, an absolute method has been investigated to verify the 235U mass content in nuclear fuel plates of Material Testing Reactor (MTR) type. The most intense gamma-ray signature at 185.7 keV emitted after α-decay of the 235U nuclei was employed in the method. The measuring system (an HPGe-spectrometer) was mathematically calibrated for efficiency using the general Monte Carlo transport code MCNP-4B. The calibration results and the measured net count rate were used to estimate the 235U mass content in fuel plates at different detector-to-fuel plate distances. Two sets of fuel plates, containing natural and low enriched uranium, were measured at the Fuel Fabrication Facility. Average accuracies for the estimated 235U masses of about 2.62% and 0.3% are obtained for the fuel plates containing natural and low enriched uranium; respectively, with a precision of about 3%.

  6. New evaluation of the{sup 232}Th resonance parameters in the energy range

    SciTech Connect

    Derrien, H.; Leal, L. C.; Larson, N. M.

    2006-07-01

    Neutron resonance parameters of {sup 232}Th were obtained from a Reich-Moore SAMMY analysis of high-resolution neutron transmission measurements performed at the Oak Ridge Linear Accelerator (ORELA) by Olsen et al. in 1981 and of high-resolution neutron capture measurements performed recently at the Geel Linear Accelerator (GELINA (Belgium)) by Schillebeeckx et al. and at n-TOF (CERN (Switzerland)) by Aerts et al. The ORELA data were analyzed previously by Olsen using the Breit-Wigner multilevel code SIOB, and their results were used for the ENDF/B-VI evaluation. In our new analysis of the Olsen neutron transmissions using the modern computer code SAMMY, better accuracy is obtained for the resonance parameters by including recent experimental neutron capture data in the experimental data base. The experimental data base and the method of analysis are described in the report. Neutron transmissions and capture cross sections calculated with the resonance parameters are compared to the experimental values. A description is given of the statistical properties of the resonance parameters. The new evaluation produces a decrease in the capture resonance integral, and improves the prediction of integral thermal benchmarks. (authors)

  7. Retardation of 238U and 232Th decay chain radionuclides in Long Island and Connecticut aquifers

    NASA Astrophysics Data System (ADS)

    Copenhaver, Sally A.; Krishnaswami, S.; Turekian, Karl K.; Epler, Nathan; Cochran, J. K.

    1993-02-01

    Knowledge of the ability of an aquifer to retard the groundwater transport of toxic or radioactive ions can be inferred from the analysis of groundwater for the radionuclides of the 238U- and 232Th-decay chains. Groundwaters of varying chemical composition were analyzed from wells in Long Island, New York, and Connecticut. Aquifer lithologies are arkose, quartz sandstone, granite, and glacial drift. Adsorption ( k1) and desorption ( k2) coefficients for Ra and Pb were calculated using 222Rn activity as a measure of the supply of other α-recoil nuclides. Laboratory tests of the validity of this assumption were made by measuring the flux of 224Ra and 222Rn from aquifer solids. The ratio k 1/k 2 is the distribution coefficient, K, which is effectively equal to R ƒ, the retardation factor. The average value of K for Ra is 6 × 10 2 in Long Island aquifers and 5 × 10 4 in Connecticut. The distribution coefficient for Pb is 10 4 in Long Island and 10 5 in Connecticut. Results from this and other studies reveal a strong dependence of retardation on pH, ƒ O 2, and ionic strength that tends to overwhelm any dependence of retardation on lithology.

  8. Mass distribution and mass resolved angular distribution of fission products in 28Si+232Th

    NASA Astrophysics Data System (ADS)

    Sodaye, Suparna; Tripathi, R.; John, B. V.; Ramachandran, K.; Pujari, P. K.

    2017-01-01

    Background: Fission process with heavier projectiles and actinide targets has contributions from processes, such as compound nucleus fission, transfer-induced fission, and noncompound nucleus fission. Mass distribution and mass-dependent anisotropy can be used to identify and delineate the contributions due to these different processes. Purpose: Mass distribution in 28Si+232Th has been studied at beam energies of 180 and 158 MeV to investigate the nature of mass distribution arising from complete and incomplete momentum-transfer fission events. Mass-dependent angular anisotropy has been measured at 166 MeV to investigate the dominant noncompound nucleus process contributing to the fission. Method: Mass distribution and mass resolved angular distribution of fission products were measured by the recoil catcher method followed by off-line γ -ray spectrometry. Results: Mass distributions for full momentum-transfer fission processes were found to be symmetric, and those for transfer-induced fission were found to be asymmetric at both beam energies. The relative contribution from transfer-induced fission was found to be higher at lower beam energy. The anisotropy of the fission product angular distribution was found to increase with decreasing mass asymmetry. Conclusions: The mass distribution indicates that, apart from the full momentum-transfer fission process, there is a significant contribution due to transfer-induced fission. The mass dependence of angular anisotropy indicated that preequilibrium fission is the dominant noncompound nucleus process in the present reaction system at near barrier energy (Ec .m ./VC=1.06 ) .

  9. Study of 234U(n,f) Resonances Measured at the CERN n_TOF Facility

    NASA Astrophysics Data System (ADS)

    Leal-Cidoncha, E.; Durán, I.; Paradela, C.; Tarrío, D.; Leong, L. S.; Audouin, L.; Tassan-Got, L.; Praena, J.; Berthier, B.; Ferrant, L.; Isaev, S.; Le Naour, C.; Stephan, C.; Trubert, D.; Abbondanno, U.; Aerts, G.; Álvarez, H.; Álvarez-Velarde, F.; Andriamonje, S.; Andrzejewski, J.; Badurek, G.; Baumann, P.; Bečvář, F.; Berthoumieux, E.; Calviño, F.; Calviani, M.; Cano-Ott, D.; Capote, R.; Carrapiço, C.; Cennini, P.; Chepel, V.; Chiaveri, E.; Colonna, N.; Cortes, G.; Couture, A.; Cox, J.; Dahlfors, M.; David, S.; Dillmann, I.; Domingo-Pardo, C.; Dridi, W.; Eleftheriadis, C.; Embid-Segura, M.; Ferrari, A.; Ferreira-Marques, R.; Fujii, K.; Furman, W.; Gonçalves, I.; González-Romero, E.; Gramegna, F.; Guerrero, C.; Gunsing, F.; Haas, B.; Haight, R.; Heil, M.; Herrera-Martinez, A.; Igashira, M.; Jericha, E.; Kadi, Y.; Käppeler, F.; Karadimos, D.; Kerveno, M.; Koehler, P.; Kossionides, E.; Krtička, M.; Lampoudis, C.; Leeb, H.; Lindote, A.; Lopes, I.; Lozano, M.; Lukic, S.; Marganiec, J.; Marrone, S.; Martínez, T.; Massimi, C.; Mastinu, P.; Mengoni, A.; Milazzo, P. M.; Moreau, C.; Mosconi, M.; Neves, F.; Oberhummer, H.; O'Brien, S.; Oshima, M.; Pancin, J.; Papadopoulos, C.; Pavlik, A.; Pavlopoulos, P.; Perrot, L.; Pigni, M. T.; Plag, R.; Plompen, A.; Plukis, A.; Poch, A.; Pretel, C.; Quesada, J.; Rauscher, T.; Reifarth, R.; Rubbia, C.; Rudolf, G.; Rullhusen, P.; Salgado, J.; Santos, C.; Sarchiapone, L.; Savvidis, I.; Tagliente, G.; Tain, J. L.; Tavora, L.; Terlizzi, R.; Vannini, G.; Vaz, P.; Ventura, A.; Villamarin, D.; Vincente, M. C.; Vlachoudis, V.; Vlastou, R.; Voss, F.; Walter, S.; Wiescher, M.; Wisshak, K.

    2014-05-01

    We present the analysis of the resolved resonance region for the 234U(n,f) cross section data measured at the CERN n_TOF facility. The resonance parameters in the energy range from 1 eV to 1500 eV have been obtained with the SAMMY code by using as initial parameters for the fit the resonance parameters of the JENDL-3.3 evaluation. In addition, the statistical analysis has been accomplished, partly with the SAMDIST code, in order to study the level spacing and the Mehta-Dyson correlation.

  10. Study of 232Th(n, γ) and 232Th(n,f) reaction rates in a graphite moderated spallation neutron field produced by 1.6 GeV deuterons on lead target

    NASA Astrophysics Data System (ADS)

    Asquith, N. L.; Hashemi-Nezhad, S. R.; Westmeier, W.; Zhuk, I.; Tyutyunnikov, S.; Adam, J.

    2015-02-01

    The Gamma-3 assembly of the Joint Institute for Nuclear Research (JINR), Dubna, Russia is designed to emulate the neutron spectrum of a thermal Accelerator Driven System (ADS). It consists of a lead spallation target surrounded by reactor grade graphite. The target was irradiated with 1.6 GeV deuterons from the Nuclotron accelerator and the neutron capture and fission rate of 232Th in several locations within the assembly were experimentally measured. 232Th is a proposed fuel for envisaged Accelerator Driven Systems and these two reactions are fundamental to the performance and feasibility of 232Th in an ADS. The irradiation of the Gamma-3 assembly was also simulated using MCNPX 2.7 with the INCL4 intra-nuclear cascade and ABLA fission/evaporation models. Good agreement between the experimentally measured and calculated reaction rates was found. This serves as a good validation for the computational models and cross section data used to simulate neutron production and transport of spallation neutrons within a thermal ADS.

  11. Natural Variation of 238U/235U in Geo- and Cosmochemistry

    NASA Astrophysics Data System (ADS)

    Weyer, S.; Brennecka, G.; Montoya Pino, C.; Noordmann, J.; Schauble, E. A.; Wadhwa, M.; Anbar, A. D.

    2009-12-01

    The ratio of the two primordial U isotopes has long been assumed to be invariant (i.e. 238U/235U = 137.88, [1]) in the Solar [1, 2]. Due to analytical improvements, small (‰-range) U isotope variations can now be detected in both terrestrial [3, 4, 5] and meteoritic materials [6]. Uranium isotope variations on Earth are produced by chemical reactions, analogous to stable isotope fractionation, although U has no stable isotopes. The range of U isotope variations observed thus far on Earth exceeds 1‰ and is mostly driven by nuclear field shift effects, which depend on nuclear volume rather than mass [7]. The strongest isotope fractionation appears to occur between oxidized and reduced U species (UVI and UIV). As a result, oxic environments (e.g., seawater) are enriched in the light U isotope, 235U, while anoxic sediments (e.g., from the Black Sea) are enriched in the heavy U isotope, 238U [4]. This redox-sensitive behavior of U isotope compositions makes the 238U/235U ratio promising for use as a paleo-redox proxy. In paleoceanography, 238U/235U ratios can be used to estimate the extent of seafloor anoxia. During periods of enhanced global ocean anoxia (e.g., during the mid-Cretaceous oceanic anoxic event OAE-2) heavy U was preferentially buried into anoxic sediments. Accordingly, sea water and all oceanic sinks became depleted in heavy U. We used this shift in U isotope compositions to estimate a three times enhancement of anoxic environments in the oceans during OAE-2 compared to today [8]. In meteoritic materials, 238U/235U variations may be produced by (1) chemical reactions (2) nucleosynthetic anomalies and/or (3) decay of the short-lived extant 247Cm (half life = 15.6 Ma) to 235U. We investigated the U isotope composition of calcium aluminum-rich inclusions (CAIs). The Pb-Pb ages of CAIs define the age of the Solar System, as they represent the first solids to condense from the cooling protoplanetary disk. The investigated CAIs from the Allende meteorite

  12. Covariance data for{sup 232}Th in the resolved resonance region from 0 to 4 keV

    SciTech Connect

    Leal, L. C.; Derrien, H.; Arbanas, G.; Larson, N. M.; Wiarda, D.

    2006-07-01

    This paper reports on the generation and testing of the covariance matrix associated with the resonance parameter evaluation for {sup 232}Th up to 4 keV. [1] Covariance data are required to correctly assess uncertainties in design parameters in nuclear applications. The error estimation of calculated quantities relies on the nuclear data uncertainty information available in the basic nuclear data libraries, such as the US Evaluated Nuclear Data Library, ENDF/B. Uncertainty files in the ENDF/B library are obtained from analysis of experimental data and are stored as variance and covariance data. In this paper, we address the generation of covariance data in the resonance region via the computer code SAMMY, which is used in the evaluation of experimental data in the resolved and unresolved resonance energy regions. The resolved resonance parameter covariance matrix for {sup 232}Th, obtained using the retroactive approach, is also presented here. (authors)

  13. The Concentrations of {sup 40}K, {sup 226}Ra and {sup 232}Th in Soil Sample in Osmaniye (Turkey)

    SciTech Connect

    Akkurt, I.; Guenoglu, K.; Kara, A.; Mavi, B.; Karaboerklue, S.

    2011-12-26

    The {sup 40}K, {sup 226}Ra and {sup 232}Th concentration is due to the magmatic structure of the earth and it can be varied from place to place. Osmaniye is located in the Eastern side of Mediteranean Region. It holds the climatic characteristics of the same region and arises with Middle Taurus Mountains from west to North and with Amonos Mounations in East and West-east parts and is situated between 35 deg. .52'-36 deg. .42' east longitudes and 36 deg. .57'-37 deg. .45' north latitudes. In this study, the natural radioactivity concentrations {sup 40}K, {sup 226}Ra and {sup 232}Th in some soil samples collected in Osmaniye have been investigated. The measurements have been performed using 3x3{sup ''} NaI(Tl) detector system.

  14. Radionuclide ((226)Ra, (232)Th, (40)K) accumulation among plant species in mangrove ecosystems of Pattani Bay, Thailand.

    PubMed

    Kaewtubtim, Pungtip; Meeinkuirt, Weeradej; Seepom, Sumalee; Pichtel, John

    2017-02-15

    Little is known regarding phytoremediation of radionuclides from soil; even less is known about radionuclide contamination and removal in tropical ecosystems such as mangrove forests. In mangrove forests in Pattani Bay, Thailand, 18 plant species from 17 genera were evaluated for radionuclide concentrations within selected plant parts. Two shrub species, Avicennia marina and Pluchea indica, accumulated the highest (232)Th (24.6Bqkg(-1)) and (40)K (220.7Bqkg(-1)) activity concentrations in roots, respectively. Furthermore, the aquatic species Typha angustifolia accumulated highest (232)Th, (40)K and (226)Ra activity concentrations (85.2, 363.5, 16.6Bqkg(-1), respectively) with the highest transfer factors (TFs) (3.0, 2.0, 5.9, respectively) in leaves. Leaves of T. angustifolia had an absorbed dose rate in air (D) over the recommended value (74.8nGyh(-1)) that was considered sufficiently high to be of concern for human consumption.

  15. Quasi-elastic scattering and transfer angular distribution for B,1110+232Th systems at near-barrier energies

    NASA Astrophysics Data System (ADS)

    Dubey, Shradha; Biswas, D. C.; Mukherjee, S.; Patel, D.; Gupta, Y. K.; Prajapati, G. K.; Joshi, B. N.; Danu, L. S.; Mukhopadhyay, S.; John, B. V.; Suryanarayana, S. V.; Vind, R. P.

    2016-12-01

    Quasi-elastic scattering and transfer angular distributions for B,1110+232Th reactions have been measured simultaneously in a wide range of bombarding energies around the Coulomb barrier. The quasi-elastic angular distribution data are analyzed using the optical model code ecis with phenomenological Woods-Saxon potentials. The obtained potential parameters suggest the presence of usual threshold anomaly, confirming tightly bound characteristics for both the projectiles. The reaction cross sections are obtained from the fitting of quasi-elastic angular distribution data. The reduced cross sections at sub-barrier energies compared with Li,76+232Th systems show a systematic dependence on projectile breakup energy. The angular distribution of the transfer products show similar behavior for both the systems.

  16. 230Th-234U Model-Ages of Some Uranium Standard Reference Materials

    SciTech Connect

    Williams, R W; Gaffney, A M; Kristo, M J; Hutcheon, I D

    2009-05-28

    The 'age' of a sample of uranium is an important aspect of a nuclear forensic investigation and of the attribution of the material to its source. To the extent that the sample obeys the standard rules of radiochronometry, then the production ages of even very recent material can be determined using the {sup 230}Th-{sup 234}U chronometer. These standard rules may be summarized as (a) the daughter/parent ratio at time=zero must be known, and (b) there has been no daughter/parent fractionation since production. For most samples of uranium, the 'ages' determined using this chronometer are semantically 'model-ages' because (a) some assumption of the initial {sup 230}Th content in the sample is required and (b) closed-system behavior is assumed. The uranium standard reference materials originally prepared and distributed by the former US National Bureau of Standards and now distributed by New Brunswick Laboratory as certified reference materials (NBS SRM = NBL CRM) are good candidates for samples where both rules are met. The U isotopic standards have known purification and production dates, and closed-system behavior in the solid form (U{sub 3}O{sub 8}) may be assumed with confidence. We present here {sup 230}Th-{sup 234}U model-ages for several of these standards, determined by isotope dilution mass spectrometry using a multicollector ICP-MS, and compare these ages with their known production history.

  17. Development of a method for activity measurements of 232Th daughters with a multidetector gamma-ray coincidence spectrometer.

    PubMed

    Antovic, N; Svrkota, N

    2009-06-01

    The method for activity measurements of the (232)Th daughters, developed at the six-crystal gamma-ray coincidence spectrometer PRIPYAT-2M and based on coincidence counting of the 583 and 2615 keV photons from cascade transitions which follow beta(-)-decay of (208)Tl, as well as on counting the 911 keV photons which follow beta(-)-decay of (228)Ac in the integral and non-coincidence mode of counting, is presented.

  18. Solubility assessment of 232Th from various types of soil in Malaysia using USP and DIN In Vitro digestion method

    NASA Astrophysics Data System (ADS)

    Rashid, Nur Shahidah Abdul; Perama, Yasmin Mohd Idris; Salih, Fitri Hakeem Mohd; Sarmani, Sukiman; Majid, Amran Ab.; Siong, Khoo Kok

    2016-11-01

    The overall results of the study showed that the concentrations of 232Th radionuclide using DIN digestion method during gastric phase are 0.0015 mg/kg - 0.0554 mg/kg and 0.0015 mg/kg - 0.0139 mg/kg during intestinal phase, respectively. As for USP digestion method during gastric phase are between 0.0877 mg/kg - 0.4964 mg/kg and 0.0207 mg/kg - 0.2291 mg/kg. The results from the measurements in various types of soils indicates some elevation of 232Th concentration in some types of soil compared to UNSCEAR reference values, in which may be a result from the impact of previous mining activity in the surrounding area and considered to be safe. In general, the results of 232Th concentrations from in vitro extraction technique is considered to be safe. By natural processes, thorium ingestion is getting transferred to living beings through different pathways and need to be monitored in order to assess possible hazards. Environmental studies are generally carried out to trace the pathway of radionuclides/radiotoxic elements to reach living organism. Environmental monitoring and meaningful interpretation of data from man-made pollution are more complicated without adequate knowledge about the natural abundance of radioactive elements in the environment.

  19. [About the contents of 40K, 226Ra and 232Th in forest soils of the Republic of Belarus].

    PubMed

    Perevolotskiĭ, A N; Perevolotskaia, T V

    2014-01-01

    The specific activity of 40K, 232Th and 226Ra in forest soil ecotopes (A2-B2-C2-D2) has been investigated. When the fertility of the soil increases from A2 to D2, then the specific activity of 40K increases in the rooting zone of the soil from 275 ± 6.9 up to 499 ± 11 Bq/kg, 232Th--from 11.8 ± 0.5 to 17.1 ± 1.1 Bq/kg, 226Ra- from 19.2 γ 0.8 to 27.9 ± 1.5 Bq/kg. The calculated capacity of the absorbed dose of γ-radiation conditioned by 40K, 232Th and 226Ra increases from A2 to D2 from 27.5 ± 0.5 to 44.1 ± 1.1 nGy / h at the height of 1 m.

  20. Candidate processes for diluting the {sup 235}U isotope in weapons-capable highly enriched uranium

    SciTech Connect

    Snider, J.D.

    1996-02-01

    The United States Department of Energy (DOE) is evaluating options for rendering its surplus inventories of highly enriched uranium (HEU) incapable of being used to produce nuclear weapons. Weapons-capable HEU was earlier produced by enriching uranium in the fissile {sup 235}U isotope from its natural occurring 0.71 percent isotopic concentration to at least 20 percent isotopic concentration. Now, by diluting its concentration of the fissile {sup 235}U isotope in a uranium blending process, the weapons capability of HEU can be eliminated in a manner that is reversible only through isotope enrichment, and therefore, highly resistant to proliferation. To the extent that can be economically and technically justified, the down-blended uranium product will be made suitable for use as commercial reactor fuel. Such down-blended uranium product can also be disposed of as waste if chemical or isotopic impurities preclude its use as reactor fuel.

  1. Differential Die-Away Analysis for detection of 235U in metallic matrix

    NASA Astrophysics Data System (ADS)

    Kashyap, Yogesh; Agrawal, Ashish; Roy, Tushar; Sarkar, P. S.; Shukla, Mayank; Patel, Tarun; Sinha, Amar

    2016-01-01

    Differential Die-Away Analysis is a powerful tool for detecting small quantity of fissile material even if it is shielded or placed in non-fissile matrix. The technique can be used to monitor and characterize fissile content for nuclear waste assay. In this paper, we have discussed the application of differential die away technique for detection of small quantity of fissile material in nuclear waste assay. Feasibility experiments to optimize various parameters have been carried out for detection of 235U in metallic matrix and reported in this paper. A minimum quantity of 1 g of 235U in 150 kg of metallic matrix has been detected in the experimental configuration being reported.

  2. The 235U Prompt Fission Neutron Spectrum in the BR1 Reactor at SCK•CEN

    NASA Astrophysics Data System (ADS)

    Wagemans, Jan; Malambu, Edouard; Borms, Luc; Fiorito, Luca

    2016-02-01

    The BR1 research reactor at SCK•CEN has a spherical cavity in the graphite above the reactor core. In this cavity an accurately characterised Maxwellian thermal neutron field is present. Different converters can be loaded in the cavity in order to obtain other types of neutron (and gamma) irradiation fields. Inside the so-called MARK III converter a fast 235U(n,f) prompt fission neutron field can be obtained. With the support of MCNP calculations, irradiations in MARK III can be directly related to the pure 235U(n,f) prompt fission neutron spectrum. For this purpose MARK III spectrum averaged cross sections for the most relevant fluence dosimetry reactions have been determined. A calibration factor for absolute measurements has been determined applying activation dosimetry following ISO/IEC 17025 standards.

  3. Critical mass experiment using {sup 235}U foil-SiO{sub 2}-polyethylene plates

    SciTech Connect

    Sanchez, R.; Kimpland, R.; Butterfield, K.; Jaegers, P.; Casson, W.

    1998-12-31

    Fissile material in waste is frequently encountered in decontamination and decommissioning activities. Thousands of drums containing radioactive waste are stored in storage facilities throughout the US Department of Energy (DOE) complex. The amount of fissile material in each drum is generally small because of the criticality safety limits that have been calculated using neutron transport computer codes such as MCNP, KENO, or ONEDANT. No experimental critical data are available to ensure the correctness of the calculations for those systems containing fissile material ({sup 235}U, {sup 233}U, and {sup 239}Pu) in contact with matrix material (Al{sub 2}O{sub 3}, CaO, MgO, and SiO{sub 2}) in the drums. The purpose of the {sup 235}U foil-SiO{sub 2}-polyethylene experiment is to provide experimental data to validate the computer transport codes and the cross-section data.

  4. Isotope fractionation of 238U and 235U during biologically-mediated uranium reduction

    NASA Astrophysics Data System (ADS)

    Stirling, Claudine H.; Andersen, Morten B.; Warthmann, Rolf; Halliday, Alex N.

    2015-08-01

    A series of laboratory-controlled microbial experiments using gram-negative sulphate-reducing bacteria (Desulfovibrio brasiliensis) inoculated with natural uranium were performed to investigate 238U/235U fractionation during bacterially-mediated U reduction. Control experiments, without bacteria to drive U reduction, were conducted in parallel. Paired measurements of 238U/235U and U concentration for both the residual growth medium solution and the accumulated biologically-mediated precipitate were obtained using multiple-collector inductively coupled plasma mass spectrometry (MC-ICPMS). The control experiments show that only minor (<0.1‰), if any 238U/235U fractionation occurs during co-precipitation with calcite. This implies that carbonate sediments are capable of faithfully recording the signature of the global ocean during Earth's major climatic events, including oxygenation and de-oxygenation transitions in the marine environment. The results for the microbial experiments demonstrate that the 238U/235U composition of the unreacted growth medium containing U(VI) is isotopically lighter than the composition of the U(IV)-bearing precipitate as U(VI) is consumed, in agreement with field-based observations of microbially-mediated U reduction. Uranium isotopic shifts of up to 0.8‰ were observed between the liquid and solid phases. These observations can be modelled using a Rayleigh distillation approach describing kinetic uptake in a closed system, which yields a fractionation factor α of 0.99923 ± 0.00004 (ε = -0.77 ± 04‰) for U(VI)-U(IV) reduction mediated by the D. brasiliensis microbe. This fractionation behaviour is consistent with that observed in field-based redox environments, which give rise to similar α values. Competing processes such as U co-precipitation (e.g. adsorption) may act to lower the apparent value for α and possibly play a secondary role both in the microbial experiments of this study and in natural U reduction settings where

  5. Critical mass experiment using {sup 235}U foils and lucite plates

    SciTech Connect

    Sanchez, R.; Butterfield, K.; Kimpland, R.; Jaegers, P.

    1998-09-01

    This experiment demonstrated how the neutron multiplication of a system increases as moderated material is placed between highly enriched uranium foils. In addition, this experiment served to demonstrate the hand-stacking technique and approach to criticality be remote operation. This experiment was designed by McLaughlin in the mid-seventies as part of the criticality safety course that is taught at the Los Alamos Critical Experiments Facility. The H/{sup 235}U ratio for this experiment was 215, which is the ratio at which the minimum critical mass for this configuration occurs.

  6. Collinear cluster tripartition channel in the reaction {sup 235}U(n{sub th}, f)

    SciTech Connect

    Pyatkov, Yu. V.; Kamanin, D. V.; Kopach, Yu. N.; Alexandrov, A. A.; Alexandrova, I. A.; Borzakov, S. B.; Voronov, Yu. N.; Zhuchko, V. E.; Kuznetsova, E. A. Panteleev, Ts.; Tyukavkin, A. N.

    2010-08-15

    Investigation of the {sup 235}U(n{sub th}, f) reaction using the miniFOBOS double-arm time-of-flight spectrometer of fission fragments confirmed manifestations of the earlier unknown many-body, at least ternary, decay involving almost collinear decay-product escape, which were first observed in the spontaneous fission of {sup 252}Cf(sf). The use of variables sensitive to the nuclear charge of fission fragments allowed the reliability of identification of decay events to be increased and new decay modes to be revealed.

  7. Moderation control in low enriched {sup 235}U uranium hexafluoride packaging operations and transportation

    SciTech Connect

    Dyer, R.H.; Kovac, F.M.; Pryor, W.A.

    1993-10-01

    Moderation control is the basic parameter for ensuring nuclear criticality safety during the packaging and transport of low {sup 235}U enriched uranium hexafluoride before its conversion to nuclear power reactor fuel. Moderation control has permitted the shipment of bulk quantities in large cylinders instead of in many smaller cylinders and, therefore, has resulted in economies without compromising safety. Overall safety and uranium accountability have been enhanced through the use of the moderation control. This paper discusses moderation control and the operating procedures to ensure that moderation control is maintained during packaging operations and transportation.

  8. 230Th-234U Age-Dating Uranium by Mass Spectrometry

    SciTech Connect

    Williams, R W; Gaffney, A M

    2012-04-18

    This is the standard operating procedure used by the Isotope Ratio Mass Spectrometry Group of the Chemical Sciences Division at LLNL for the preparation of a sample of uranium oxide or uranium metal for {sup 230}Th-{sup 234}U age-dating. The method described here includes the dissolution of a sample of uranium oxide or uranium metal, preparation of a secondary dilution, spiking of separate aliquots for uranium and thorium isotope dilution measurements, and purification of uranium and thorium aliquots for mass spectrometry. This SOP may be applied to uranium samples of unknown purity as in a nuclear forensic investigation, and also to well-characterized samples such as, for example, U{sub 3}O{sub 8} and U-metal certified reference materials. The sample of uranium is transferred to a quartz or PFA vial, concentrated nitric acid is added and the sample is heated on a hotplate at approximately 100 C for several hours until it dissolves. The sample solution is diluted with water to make the solution approximately 4 M HNO{sub 3} and hydrofluoric acid is added to make it 0.05 M HF. A secondary dilution of the primary uranium solution is prepared. Separate aliquots for uranium and thorium isotope dilution measurements are taken and spiked with {sup 233}U and {sup 229}Th, respectively. The spiked aliquot for uranium isotope dilution analysis is purified using EiChrom UTEVA resin. The spiked aliquot for thorium isotope dilution analysis is purified by, first, a 1.8 mL AG1x8 resin bed in 9 M HCl on which U adsorbs and Th passes through; second, adsorbing Th on a 1 mL AG1x8 resin bed in 8 M HNO{sub 3} and then eluting it with 9 M HCl followed by 0.1 M HCl + 0.005 M HF; and third, by passing the Th through a final 1.0 mL AG1x8 resin bed in 9 M HCl. The mass spectrometry is performed using the procedure 'Th and U Mass Spectrometry for {sup 230}Th-{sup 234}U Age Dating'.

  9. Covariances of Evaluated Nuclear Cross Section Data for (232)Th, (180,182,183,184,186)W and (55)Mn

    SciTech Connect

    Trkov, A.; Capote, R.; Soukhovitskii, E; Leal, Luiz C; Sin, M; Kodeli, I.; Muir, D W

    2011-01-01

    The EMPIRE code system is a versatile package for nuclear model calculations that is often used for nuclear data evaluation. Its capabilities include random sampling of model parameters, which can be utilized to generate a full covariance matrix of all scattering cross sections, including cross-reaction correlations. The EMPIRE system was used to prepare the prior covariance matrices of reaction cross sections of (232)Th, (180,182,183,184,186)W and (55)Mn nuclei for incident neutron energies up to 60 MeV. The obtained modeling prior was fed to the GANDR system, which is a package for a global assessment of nuclear data, based on the Generalized Least-Squares method. By introducing experimental data from the EXFOR database into GANDR, the constrained covariance matrices and cross section adjustment functions were obtained. Applying the correction functions on the cross sections and formatting the covariance matrices, the final evaluations in ENDF-6 format including covariances were derived. In the resonance energy range, separate analyses were performed to determine the resonance parameters with their respective covariances. The data files thus obtained were then subjected to detailed testing and validation. Described evaluations with covariances of (232)Th, (180,182,183,184,186)W and (55)Mn nuclei are included into the ENDF/B-VII.1 library release.

  10. Primordial radioactivity ((238)U, (232)Th and (40)K) measurements for soils of Ludhiana district of Punjab, India.

    PubMed

    Badhan, K; Mehra, R

    2012-11-01

    The aim of the present work was to study the activity concentration and absorbed gamma dose rates due to primordial radionuclides ((238)U, (232)Th and (40)K) for the soil of different villages of Ludhiana district of Punjab, India using a high-purity germanium detector based on high resolution gamma-ray spectrometry. The average activity concentrations of (238)U, (232)Th and (40)K in the soil samples have been found to be 28.58, 50.95 and 569.59 Bq kg(-1), respectively, which gives the total gamma dose rate contribution of 68.50 nGy h(-1). To evaluate the radiological hazard of the natural radioactivity, the radium equivalent activity, the external hazard index, the absorbed dose rate and the effective dose rate have been calculated. The calculated radium equivalent activity values are on the lower side of the recommended safe limit value of 370 Bq kg(-1) by Organization of Economic and Control Department. The calculated value of external health hazard index is lower than unity.

  11. A dispersive optical model potential for nucleon induced reactions on 238U and 232Th nuclei with full coupling

    NASA Astrophysics Data System (ADS)

    Quesada, José Manuel; Soukhovitskiĩ, EfremS.; Capote, Roberto; Chiba, Satoshi

    2013-03-01

    A dispersive coupled-channel optical model potential (DCCOMP) that couples the ground-state rotational and low-lying vibrational bands of 238U and 232Th nuclei is studied. The derived DCCOMP couples almost all excited levels below 1 MeV of excitation energy of the corresponding even-even actinides. The ground state, octupole, beta, gamma, and non-axial bands are coupled. The first two isobar analogue states (IAS) populated in the quasi-elastic (p,n) reaction are also coupled in the proton induced calculation, making the potential approximately Lane consistent. The coupled-channel potential is based on a soft-rotor description of the target nucleus structure, where dynamic vibrations are considered as perturbations of the rigid rotor underlying structure. Matrix elements required to use the proposed structure model in Tamura coupled-channel scheme are derived. Calculated ratio R(U238/Th232) of the total cross-section difference to the averaged σT for 238U and 232Th nuclei is shown to be in excellent agreement with measured data.

  12. Covariances of Evaluated Nuclear Cross Section Data for 232Th, 180,182,183,184,186W and 55Mn

    NASA Astrophysics Data System (ADS)

    Trkov, A.; Capote, R.; Soukhovitskii, E. Sh.; Leal, L. C.; Sin, M.; Kodeli, I.; Muir, D. W.

    2011-12-01

    The EMPIRE code system is a versatile package for nuclear model calculations that is often used for nuclear data evaluation. Its capabilities include random sampling of model parameters, which can be utilised to generate a full covariance matrix of all scattering cross sections, including cross-reaction correlations. The EMPIRE system was used to prepare the prior covariance matrices of reaction cross sections of 232Th, 180,182,183,184,186W and 55Mn nuclei for incident neutron energies up to 60 MeV. The obtained modelling prior was fed to the GANDR system, which is a package for a global assessment of nuclear data, based on the Generalised Least-Squares method. By introducing experimental data from the EXFOR database into GANDR, the constrained covariance matrices and cross section adjustment functions were obtained. Applying the correction functions on the cross sections and formatting the covariance matrices, the final evaluations in ENDF-6 format including covariances were derived. In the resonance energy range, separate analyses were performed to determine the resonance parameters with their respective covariances. The data files thus obtained were then subjected to detailed testing and validation. Described evaluations with covariances of 232Th, 180,182,183,184,186W and 55Mn nuclei are included into the ENDF/B-VII.1 library release.

  13. Total Kinetic Energy Release in the Fast Neutron Induced Fission of 235U

    NASA Astrophysics Data System (ADS)

    Loveland, Walter; Yanez, Ricardo

    2016-09-01

    We have measured the total kinetic energy (TKE) release, its variance and associated fission product mass distributions for the neutron induced fission of 235U for En = 2-90 MeV using the 2E method. The neutron energies were determined,event by event, by time of flight measurements with the white spectrum neutron beam from LANSCE. The TKE decreases with increasing neutron energy. This TKE decrease is due to increasing symmetric fission (and decreasing asymmetric fission)with increasing neutron energy, in accord with Brosa model predictions. Our measurement of the TKE release for 235U(nth,f) is in excellent agreement with the known value, indicating our measurements are absolute measurements. The TKE variances are sensitive indicators of nth chance fission. Due to the occurrence of nth chance fission and pre-fission neutron emission, the average fissioning system and its excitation energy is a complex function of the incident neutron energy. Detailed comparisons of our data with previous measurements will be made. This work was supported, in part, by the Director, Office of Energy Research, Division of Nuclear Physics of the Office of High Energy and Nuclear Physics of the U.S. Department of Energy under Grant DE-SC0014380.

  14. Consistent Data Assimilation of Actinide Isotopes: 235U and 239Pu

    SciTech Connect

    G. Palmiottti; H. Hiruta; M. Salvatores

    2011-09-01

    In this annual report we illustrate the methodology of the consistent data assimilation that allows to use the information coming from integral experiments for improving the basic nuclear parameters used in cross section evaluation. A series of integral experiments were analyzed using the EMPIRE evaluated files for {sup 235}U, {sup 238}U, and {sup 239}Pu. Inmost cases the results have shown quite large worse results with respect to the corresponding existing evaluations available for ENDF/B-VII. The observed discrepancies between calculated and experimental results were used in conjunction with the computed sensitivity coefficients and covariance matrix for nuclear parameters in a consistent data assimilation. Only the GODIVA and JEZEBEL experimental results were used, in order to exploit information relative to the isotope of interest that are, in this particular case: {sup 235}U and {sup 239}Pu. The results obtained by the consistent data assimilation indicate that with reasonable modifications (mostly within the initial standard deviation) it is possible to eliminate the original large discrepancies on the K{sub eff} of the two critical configurations. However, some residual discrepancy remains for a few fission spectral indices that are, most likely, to be attributed to the detector cross sections.

  15. Neutron methods for measuring {sup 235}U content in UF{sub 6} gas

    SciTech Connect

    Stromswold, D.C.; Peurrung, A.J.; Reeder, P.L.; Pappas, R.A.; Sunberg, D.S.

    1996-10-01

    In the United States and Russia, UF{sub 6} gas streams of highly enriched uranium and lower enrichment uranium am being blended to reduce the stockpile of the highly enriched material. The resultant uranium is no longer useful for weapons, but is suitable as fuel for nuclear reactors. A method to verify the blending of high- and low-enrichment uranium was developed at Pacific Northwest National Laboratory (PNNL) for the U.S. Department of Energy, Office of Research and Development (NN-20). In the United States, blending occurs at the U.S. Department of Energy`s Portsmouth Gaseous Diffusion Plant located near Portsmouth, Ohio. In Russia, the blending takes place at Novouralsk. The United States is purchasing the blended product produced in Russia in a program to reduce the availability of enriched uranium that can be used for weapons production. Monitoring the {sup 235}U mass flux of the input stream having the highly enriched uranium will provide confidence that high-enrichment uranium is being consumed in the blending process, and monitoring the output stream will provide an on-line measure of the {sup 235}U in the mixed product. The Portsmouth plant is a potential test facility for non-destructive technology to monitor blending. In addition, monitoring the blending at Portsmouth can support International Atomic Energy Agency activities on controlling and reducing enriched uranium stockpiles.

  16. Photon-induced Fission Product Yield Measurements on 235U, 238U, and 239Pu

    NASA Astrophysics Data System (ADS)

    Krishichayan, Fnu; Bhike, M.; Tonchev, A. P.; Tornow, W.

    2015-10-01

    During the past three years, a TUNL-LANL-LLNL collaboration has provided data on the fission product yields (FPYs) from quasi-monoenergetic neutron-induced fission of 235U, 238U, and 239Pu at TUNL in the 0.5 to 15 MeV energy range. Recently, we have extended these experiments to photo-fission. We measured the yields of fission fragments ranging from 85Kr to 147Nd from the photo-fission of 235U, 238U, and 239Pu using 13-MeV mono-energetic photon beams at the HIGS facility at TUNL. First of its kind, this measurement will provide a unique platform to explore the effect of the incoming probe on the FPYs, i.e., photons vs. neutrons. A dual-fission ionization chamber was used to determine the number of fissions in the targets and these samples (along with Au monitor foils) were gamma-ray counted in the low-background counting facility at TUNL. Details of the experimental set-up and results will be presented and compared to the FPYs obtained from neutron-induced fission at the same excitation energy of the compound nucleus. Work supported in part by the NNSA-SSAA Grant No. DE-NA0001838.

  17. 238,234U contents on Lepomis Cyanellus from San Marcos dam located in a uraniferous area

    NASA Astrophysics Data System (ADS)

    Lares, Magaly Cabral; Luna-Porres, Mayra Y.; Montero-Cabrera, María E.; Renteria-Villalobos, Marusia

    2014-07-01

    Fish species are suitable biomonitors of radioisotopes in aquatic systems. In the present study, it was made the determination of uranium isotopic contents on fish fillet (Lepomis Cyanellus) from San Marcos dam which is located in uranium mineralized zone. Uranium activity concentrations (AC) in fish samples were obtained on wet weight (ww), using liquid scintillation. 238U and 234U AC in fish fillet ranged from 0.0004 to 0.0167 Bq kg-1, and from 0.0013 to 0.0394 Bq kg-1, respectively. The activity ratio (234U/overflow="scroll">238U) in fish fillet ranged from 2.2 to 8.8. Lepomis cyanellus from San Marcos dam shows bioaccumulation factor (FB) of 0.6 L kg-1. The results suggest that the Lepomis Cyanellus in environments with high U contents tends to have a greater bioaccumulation compared to others.

  18. Search for nuclear excitation by electronic transition in {sup 235}U

    SciTech Connect

    Claverie, G.; Aleonard, M.M.; Chemin, J.F.; Gobet, F.; Hannachi, F.; Harston, M.R.; Malka, G.; Scheurer, J.N.; Morel, P.; Meot, V.

    2004-10-01

    We have searched for the nuclear excitation by electronic transition (NEET) of the isomeric level at 76 eV in {sup 235}U in a plasma induced by a YAG laser with an energy of 1 Joule and a full width at half maximum time distribution of 5 ns, operating at an intensity of 10{sup 13} W cm{sup -2}. We present a thorough description of the experimental conditions and analysis of our data. In this experimental situation we do not detect any excitation of the isomeric level, a result that is at variance with a previously reported one. An upper limit of 6x10{sup -6} per atom and per second averaged over the laser-pulse width has been set on the nuclear excitation rate. This value is compared with results obtained in previous experimental and theoretical works.

  19. High accuracy 235U(n,f) data in the resonance energy region

    NASA Astrophysics Data System (ADS)

    Paradela, C.; Duran, I.; Tassan-Got, L.; Audouin, L.; Berthier, B.; Isaev, S.; Le Naour, C.; Stephan, C.; Tarrío, D.; Abbondanno, U.; Aerts, G.; Álvarez-Pol, H.; Álvarez-Velarde, F.; Andriamonje, S.; Andrzejewski, J.; Badurek, G.; Baumann, P.; Becvar, F.; Berthoumieux, E.; Calviño, F.; Calviani, M.; Cano-Ott, D.; Capote, R.; Carrapiço, C.; Cennini, P.; Chepel, V.; Chiaveri, E.; Colonna, N.; Cortes, G.; Couture, A.; Cox, J.; Dahlfors, M.; David, S.; Dillmann, I.; Domingo-Pardo, C.; Dridi, W.; Eleftheriadis, C.; Embid-Segura, M.; Ferrant, L.; Ferrari, A.; Ferreira-Marques, R.; Fujii, K.; Furman, W.; Gonçalves, I. F.; Gonzalez-Romero, E.; Goverdovski, A.; Gramegna, F.; Guerrero, C.; Gunsing, F.; Haight, R.; Heil, M.; Igashira, M.; Jericha, E.; Kadi, Y.; Kaeppeler, F.; Karadimos, D.; Kerveno, M.; Ketlerov, V.; Koehler, P.; Konovalov, V.; Krticka, M.; Lampoudis, C.; Lederer, C.; Leeb, H.; Lindote, A.; Lukic, S.; Marganiec, J.; Martinez, T.; Marrone, S.; Massimi, C.; Mastinu, P.; Mengoni, A.; Milazzo, P. M.; Moreau, C.; Mosconi, M.; Pancin, S., J.; Pavlik, A.; Pavlopoulos, P.; Perrot, L.; Plag, R.; Plompen, A.; Plukis, A.; Poch, A.; Pretel, C.; Praena, J.; Quesada, J.; Rauscher, T.; Reifarth, R.; Rubbia, C.; Rudolf, G.; Rullhusen, P.; Salgado, J.; Santos, C.; Sarchiapone, L.; Savvidis, I.; Tagliente, G.; Tain, J. L.; Tavora, L.; Terlizzi, R.; Vaz, P.; Ventura, A.; Villamarin, D.; Vincente, M. C.; Vlachoudis, V.; Vlastou, R.; Voss, F.; Walter, S.; Weiss, C.; Wiesher, M.; Wisshak, K.

    2016-03-01

    The 235U neutron-induced cross section is widely used as reference cross section for measuring other fission cross sections, but in the resonance region it is not considered as an IAEA standard because of the scarce experimental data covering the full region. In this work, we deal with a new analysis of the experimental data obtained with a detection setup based on parallel plate ionization chambers (PPACs) at the CERN n_TOF facility in the range from 1 eV to 10 keV. The relative cross section has been normalised to the IAEA value in the region between 7.8 and 11 eV, which is claimed as well-known. Comparison with the ENDF/B-VII evaluation and the IAEA reference file from 100 eV to 10 keV are provided.

  20. Evaluation of the 232Th Neutron Cross Sections between 4 keV and 140 keV

    SciTech Connect

    Volev, K.; Koyumdjieva, N.; Brusegan, A.; Borella, A.; Siegler, P.; Schillebeeckx, P.; Janeva, N.; Lukyanov, A.; Leal, L.

    2005-05-24

    An evaluation of the 232Th neutron total and capture cross sections has been performed in the energy region between 4 keV and 140 keV. The evaluation results from a simultaneous analysis of capture, transmission, and self-indication measurement data, including the most recent capture cross-section data obtained at the GELINA facility of the Institute for Reference Materials and Measurements at Geel (B) and at the n-TOF facility at CERN (CH). The experimental data have been analysed in terms of average resonance parameters exploiting two independent theoretical approaches -- the Characteristic Function model and the Hauser-Feshbach-Moldauer theory. The resulting parameters are consistent with the resolved resonance parameters deduced from the transmission measurements of Olsen et al. at the ORELA facility.

  1. Measurement of resolved resonances of 232Th(n,γ) at the n_TOF facility at CERN

    NASA Astrophysics Data System (ADS)

    Gunsing, F.; Berthoumieux, E.; Aerts, G.; Abbondanno, U.; Álvarez, H.; Alvarez-Velarde, F.; Andriamonje, S.; Andrzejewski, J.; Assimakopoulos, P.; Audouin, L.; Badurek, G.; Baumann, P.; Bečvář, F.; Calviño, F.; Cano-Ott, D.; Capote, R.; Carrillo de Albornoz, A.; Cennini, P.; Chepel, V.; Chiaveri, E.; Colonna, N.; Cortes, G.; Couture, A.; Cox, J.; Dahlfors, M.; David, S.; Dillman, I.; Dolfini, R.; Domingo-Pardo, C.; Dridi, W.; Duran, I.; Eleftheriadis, C.; Embid-Segura, M.; Ferrant, L.; Ferrari, A.; Ferreira-Marques, R.; Fitzpatrick, L.; Frais-Koelbl, H.; Fujii, K.; Furman, W.; Goncalves, I.; Gonzalez-Romero, E.; Goverdovski, A.; Gramegna, F.; Griesmayer, E.; Guerrero, C.; Haas, B.; Haight, R.; Heil, M.; Herrera-Martinez, A.; Igashira, M.; Isaev, S.; Jericha, E.; Käppeler, F.; Kadi, Y.; Karadimos, D.; Karamanis, D.; Kerveno, M.; Ketlerov, V.; Koehler, P.; Konovalov, V.; Kossionides, E.; Krtička, M.; Lampoudis, C.; Leeb, H.; Lindote, A.; Lopes, I.; Lozano, M.; Lukic, S.; Marganiec, J.; Marques, L.; Marrone, S.; Mastinu, P.; Mengoni, A.; Milazzo, P. M.; Moreau, C.; Mosconi, M.; Neves, F.; Oberhummer, H.; O'Brien, S.; Oshima, M.; Pancin, J.; Papachristodoulou, C.; Papadopoulos, C.; Paradela, C.; Patronis, N.; Pavlik, A.; Pavlopoulos, P.; Perrot, L.; Pigni, M. T.; Plag, R.; Plompen, A.; Plukis, A.; Poch, A.; Pretel, C.; Quesada, J.; Rauscher, T.; Reifarth, R.; Rosetti, M.; Rubbia, C.; Rudolf, G.; Rullhusen, P.; Salgado, J.; Sarchiapone, L.; Savvidis, I.; Stephan, C.; Tagliente, G.; Tain, J. L.; Tassan-Got, L.; Tavora, L.; Terlizzi, R.; Vannini, G.; Vaz, P.; Ventura, A.; Villamarin, D.; Vincente, M. C.; Vlachoudis, V.; Vlastou, R.; Voss, F.; Walter, S.; Wendler, H.; Wiescher, M.; Wisshak, K.

    2012-06-01

    The yield of the neutron capture reaction 232Th(n,γ) has been measured at the neutron time-of-flight facility n_TOF at CERN in the energy range from 1 eV to 1 MeV. The reduction of the acquired data to the capture yield for resolved resonances from 1 eV to 4 keV is described and compared to a recent evaluated data set. The resonance parameters were used to assign an orbital momentum to each resonance. A missing level estimator was used to extract the s-wave level spacing of D0=17.2±0.9 eV.

  2. Benchmark experiments at ASTRA facility on definition of space distribution of {sup 235}U fission reaction rate

    SciTech Connect

    Bobrov, A. A.; Boyarinov, V. F.; Glushkov, A. E.; Glushkov, E. S.; Kompaniets, G. V.; Moroz, N. P.; Nevinitsa, V. A.; Nosov, V. I.; Smirnov, O. N.; Fomichenko, P. A.; Zimin, A. A.

    2012-07-01

    Results of critical experiments performed at five ASTRA facility configurations modeling the high-temperature helium-cooled graphite-moderated reactors are presented. Results of experiments on definition of space distribution of {sup 235}U fission reaction rate performed at four from these five configurations are presented more detail. Analysis of available information showed that all experiments on criticality at these five configurations are acceptable for use them as critical benchmark experiments. All experiments on definition of space distribution of {sup 235}U fission reaction rate are acceptable for use them as physical benchmark experiments. (authors)

  3. Theoretical Model for Volume Fraction of UC, 235U Enrichment, and Effective Density of Final U 10Mo Alloy

    SciTech Connect

    Devaraj, Arun; Prabhakaran, Ramprashad; Joshi, Vineet V.; Hu, Shenyang Y.; McGarrah, Eric J.; Lavender, Curt A.

    2016-04-12

    The purpose of this document is to provide a theoretical framework for (1) estimating uranium carbide (UC) volume fraction in a final alloy of uranium with 10 weight percent molybdenum (U 10Mo) as a function of final alloy carbon concentration, and (2) estimating effective 235U enrichment in the U 10Mo matrix after accounting for loss of 235U in forming UC. This report will also serve as a theoretical baseline for effective density of as-cast low-enriched U 10Mo alloy. Therefore, this report will serve as the baseline for quality control of final alloy carbon content

  4. 234U/238U evidence for local recharge and patterns of groundwater flow in the vicinity of Yucca Mountain, Nevada, USA

    USGS Publications Warehouse

    Paces, J.B.; Ludwig, K. R.; Peterman, Z.E.; Neymark, L.A.

    2002-01-01

    Uranium concentrations and 234U/238U ratios in saturated-zone and perched ground water were used to investigate hydrologic flow and downgradient dilution and dispersion in the vicinity of Yucca Mountain, a potential high-level radioactive waste disposal site. The U data were obtained by thermal ionization mass spectrometry on more than 280 samples from the Death Valley regional flow system. Large variations in both U concentrations (commonly 0.6-10 ??g 1-1) and 234U/238U activity ratios (commonly 1.5-6) are present on both local and regional scales; however, ground water with 234U/238U activity ratios from 7 up to 8.06 is restricted largely to samples from Yucca Mountain. Data from ground water in the Tertiary volcanic and Quaternary alluvial aquifers at and adjacent to Yucca Mountain plot in 3 distinct fields of reciprocal U concentration versus 234U/238U activity ratio correlated to different geographic areas. Ground water to the west of Yucca Mountain has large U concentrations and moderate 234U/238U whereas ground water to the east in the Fortymile flow system has similar 234U/238U, but distinctly smaller U concentrations. Ground water beneath the central part of Yucca Mountain has intermediate U concentrations but distinctive 234U/238U activity ratios of about 7-8. Perched water from the lower part of the unsaturated zone at Yucca Mountain has similarly large values of 234U/238U. These U data imply that the Tertiary volcanic aquifer beneath the central part of Yucca Mountain is isolated from north-south regional flow. The similarity of 234U/238U in both saturated- and unsaturated-zone ground water at Yucca Mountain further indicates that saturated-zone ground water beneath Yucca Mountain is dominated by local recharge rather than regional flow. The distinctive 234U/238U signatures also provide a natural tracer of downgradient flow. Elevated 234U/238U in ground water from two water-supply wells east of Yucca Mountain are interpreted as the result of induced

  5. Testing the 234U/238U weathering tracer in a tropical granitoid watershed, Luquillo, Puerto Rico

    NASA Astrophysics Data System (ADS)

    Pett-Ridge, J. C.; Derry, L. A.

    2006-12-01

    Recent studies have employed U-series disequilibria as a tracer of both weathering profile development and of timescale of erosion for whole watersheds. We have undertaken a detailed analysis of the behavior of the U- series isotopes in a previously well-characterized watershed in order to test this approach. In the Rio Icacos watershed in the Luquillo Mountains of Puerto Rico, previous studies have determined both the rate of propagation of the chemical weathering front by regolith mass balance analysis, and the surface denudation rate using the cosmogenic 10Be tracer. Our study aims to determine whether the U-series approach provides regolith development and erosion rates in agreement with those previously determined. In order to better constrain interpretations based on U-series data, we have coupled the U-series analysis with analyses of trace element concentrations, δ^{30}Si, Ge/Si, and 87Sr/86Sr ratios. Used together, these geochemical tracers provide a powerful tool for understanding weathering reactions, chemical transfers within and out of the weathering profile, and the timing of these chemical transfers. Analyses of soil, saprolite and pore water samples reveal a complex history of U and Th transformations including mobilization of both U and Th in the soil followed by re-adsorption deeper in the profile. 234U/238U activity ratios in soil and saprolite show significant variability both with depth, and also among individual mineral phases at any particular depth. This variation among mineral phases, combined with the likely physical sorting of these phases during erosional transport, results in an additional isotopic fractionation unrelated to that imparted by the weathering process. This implies that suspended sediment samples taken from streamwater are unlikely to accurately reflect the average disequilibria carried by the secondary minerals phases in the soil and saprolite. Our analyses also reveal a significant contribution of atmospheric mineral

  6. Cross-sections of the reaction 232Th(p,3n)230Pa for production of 230U for targeted alpha therapy.

    PubMed

    Morgenstern, Alfred; Apostolidis, Christos; Bruchertseifer, Frank; Capote, Roberto; Gouder, Thomas; Simonelli, Federica; Sin, Mihaela; Abbas, Kamel

    2008-10-01

    (230)U/(226)Th is a promising novel alpha-emitter system for application in targeted alpha therapy of cancer. The therapeutic nuclides can be produced by proton irradiation of natural (232)Th according to the reaction (232)Th(p,3n)(230)Pa, followed by subsequent beta decay of (230)Pa to (230)U. In this study, the experimental excitation function for the (232)Th(p,3n)(230)Pa reaction up to 34 MeV proton energy has been measured using the stacked-foil technique. The proton energies in the various foils were calculated with the SRIM 2003 code and gamma-ray spectrometry was used to measure the activities of the various radioisotopes produced. The measured cross-sections are in good agreement with selected literature values and with model calculations using the EMPIRE II code. The reaction (232)Th(p,3n)(230)Pa allows the production of carrier-free (230)U in clinically relevant levels.

  7. Combined 238U/235U and Pb Isotopics of Planetary Core Material: The Absolute Age of the IVA Iron Muonionalusta

    NASA Astrophysics Data System (ADS)

    Brennecka, G. A.; Amelin, Y.; Kleine, T.

    2016-08-01

    We report a measured 238U/235U for the IVA iron Muonionalusta. This measured value requires an age correction of ~7 Myr to the previously published Pb-Pb age. This has major implications for our understanding of planetary core formation and cooling.

  8. Uranium stable isotope fractionation in the Black Sea: Modern calibration of the 238U/235U paleo-redox proxy

    NASA Astrophysics Data System (ADS)

    Rolison, John M.; Stirling, Claudine H.; Middag, Rob; Rijkenberg, Micha J. A.

    2017-04-01

    The isotopic compositions of redox-sensitive metals, including uranium (U), in marine sediments have recently emerged as powerful diagnostic tracers of the redox state of the ancient ocean-atmosphere system. Reliable interpretation of sedimentary isotopic information requires a thorough understanding of the environmental controls on isotopic fractionation in modern anoxic environments before being applied to the paleo-record. In this study, the relationship between ocean anoxia and the isotopic fractionation of U was investigated in the water column and sediments of the Black Sea, the world's largest anoxic basin. Paired measurements of 238U/235U and U concentration, supported by other redox parameters, were obtained for water column and sediment samples collected during the 2013 GA04N GEOTRACES expedition to the Black Sea. Removal of U from the water column occurs during the redox transition of soluble U(VI) to relatively insoluble U(IV), resulting in up to 43% of U being removed from solution in euxinic bottom waters. Uranium reduction and removal is accompanied by a progressive shift in 238U/235U towards isotopically light values in the water column as heavier 238U is preferentially exported to sediments over lighter 235U. This gives rise to apparent isotope enrichment factors of ε = -0.63 ± 0.09‰ and ε = -0.84 ± 0.11‰ when U removal is modelled by Rayleigh and closed system equilibrium isotope fractionation, respectively. These ε values fall within the range determined for bacterial U reduction experiments, and together with a striking correlation between the distributions of U and H2S, implicate microbially-mediated U(VI)-U(IV) reduction as the primary mechanism controlling U isotopic shifts in the Black Sea. The 238U/235U of underlying sediments is related to the the 238U/235U of Black Sea bottom waters through the isotope enrichment factor of the U reduction reaction but the relationship between sedimentary and water column 238U/235U is complicated

  9. Determination of 235U enrichment with a large volume CZT detector

    NASA Astrophysics Data System (ADS)

    Mortreau, Patricia; Berndt, Reinhard

    2006-01-01

    Room-temperature CdZnTe and CdTe detectors have been routinely used in the field of Nuclear Safeguards for many years [Ivanov et al., Development of large volume hemispheric CdZnTe detectors for use in safeguards applications, ESARDA European Safeguards Research and Development Association, Le Corum, Montpellier, France, 1997, p. 447; Czock and Arlt, Nucl. Instr. and Meth. A 458 (2001) 175; Arlt et al., Nucl. Instr. and Meth. A 428 (1999) 127; Lebrun et al., Nucl. Instr. and Meth. A 448 (2000) 598; Aparo et al., Development and implementation of compact gamma spectrometers for spent fuel measurements, in: Proceedings, 21st Annual ESARDA, 1999; Arlt and Rudsquist, Nucl. Instr. and Meth. A 380 (1996) 455; Khusainov et al., High resolution pin type CdTe detectors for the verification of nuclear material, in: Proceedings, 17th Annual ESARDA European Safeguards Research and Development Association, 1995; Mortreau and Berndt, Nucl. Instr. and Meth. A 458 (2001) 183; Ruhter et al., UCRL-JC-130548, 1998; Abbas et al., Nucl. Instr. and Meth. A 405 (1998) 153; Ruhter and Gunnink, Nucl. Instr. and Meth. A 353 (1994) 716]. Due to their performance and small size, they are ideal detectors for hand-held applications such as verification of spent and fresh fuel, U/Pu attribute tests as well as for the determination of 235U enrichment. The hemispherical CdZnTe type produced by RITEC (Riga, Latvia) [Ivanov et al., 1997] is the most widely used detector in the field of inspection. With volumes ranging from 2 to 1500 mm 3, their spectral performance is such that the use of electronic processing to correct the pulse shape is not required. This paper reports on the work carried out with a large volume (15×15×7.5 mm 3) and high efficiency hemispherical CdZnTe detector for the determination of 235U enrichment. The measurements were made with certified uranium samples whose enrichment ranging from 0.31% to 92.42%, cover the whole range of in-field measurement conditions. The interposed

  10. Neutron experiments at Portsmouth for measuring flow and {sup 235}U content in UF{sub 6} gas

    SciTech Connect

    Stromswold, D C; Reeder, P L; Peurrung, A J

    1997-04-01

    The Portsmouth Gaseous Diffusion Plant produces enriched uranium for use in commercial power reactors. The plant also aids disposal of excess high-enrichment uranium (HEU) by blending it with lower-enrichment material. Experiments were conducted to test two neutron-based methods for monitoring the down-blending of HEU. Results of the initial experiments showed that gas (on-off) could be detected, but that additional tests and data are needed to quantify the flow velocity and {sup 235}U content. The experiments used a {sup 252}Cf neutron source to induce fission in a small fraction of the {sup 235}U contained in the UF{sub 6} gas. The first method measured the attenuation of neutrons passing through the low-pressure UF{sub 6} gas in a 7.6-cm diameter pipe. The concept was based on the fact that some of the thermal neutrons are absorbed by {sup 235}U, thus changing the observed count rate. The second method, tested on a 20-cm diameter pipe where gas pressure was higher, used a modulated neutron flux to induce fission in the {sup 235}U. Modulation was achieved by moving a neutron source. During both experiments, plant monitoring equipment showed that light gases (freon, oxygen, and nitrogen) were present in widely varying amounts, along with the UF{sub 6} gas. These gases may have affected the experimental results, at least to the extent that they replaced UF{sub 6}. This report also contains results of computer simulations and tests performed on the electronics after the experiments were completed at Portsmouth. Recommendations are made for follow-on work to measure the flow velocity and {sup 235}U content.

  11. Prompt fission neutron spectra of n+235U above the (n,nf) fission threshold

    NASA Astrophysics Data System (ADS)

    Shu, Neng-Chuan; Jia, Min; Chen, Yong-Jing; Liu, Ting-Jin

    2015-05-01

    Calculations of prompt fission neutron spectra (PFNS) from the 235U(n, f) reaction were performed with a semi-empirical method for En = 7.0 and 14.7 MeV neutron energies. The total PFNS were obtained as a superposition of (n,xnf) pre-fission neutron spectra and post-fission spectra of neutrons which were evaporated from fission fragments, and these two kinds of spectra were taken as an expression of the evaporation spectrum. The contributions of (n,xnf) fission neutron spectra on the calculated PFNS were discussed. The results show that emission of one or two neutrons in the (n,nf) or (n,2nf) reactions influences the PFNS shape, and the neutron spectra of the (n,xnf) fission-channel are soft compared with the neutron spectra of the (n,f) fission channel. In addition, analysis of the multiple-chance fission component showed that second-chance fission dominates the PFNS with an incident neutron energy of 14.7 MeV whereas first-chance fission dominates the 7 MeV case. Supported by National Natural Science Foundation of China (11205246, 91126010, U1230127, 91226102), IAEA CRP (15905), and Defense Industrial Technology Development Program (B0120110034)

  12. Diagenesis of fossil coral skeletons: Correlation between trace elements, textures, and [sup 234]U/[sup 238]U

    SciTech Connect

    Bar-Matthews, M.; Wasserburg, G.J.; Chen, J.H. )

    1993-01-01

    A comparative study of Pleistocene fossil coral skeletons and of modern coral skeletons was carried out using petrographic and trace element analyses on a suite of Pleistocene samples that had previously been studied from [sup 234]U, [sup 230]Th, and U-[sup 230]Th ages (Chen et al. 1991). Evidence of a range of diagenetic changes can be recognized by optical (OM) and scanning electron microscopy (SEM). Using an electron microprobe and SEM, concentrations of Na, S, Sr, and Mg were measured. No other trace elements were detected. Na, S, and Mg contents of the matrix, the fibrous micropores, and radiating needles are highly variable and well correlated. High concentrations of Na, S, and Mg were found in modern living corals with lower concentrations in fossil corals and fibrous micropores, and the lowest value in the radiating needles. The reason for the correlations of Na, S, and Mg and crystal chemistry and the response to diagenesis of these trace elements is not understood. The average concentrations of Na, S, and Mg for each sample, when plotted against the whole coral initial [delta][sup 234]U, are generally correlated (Chen et al., 1991). As all these diagenetic changes involve the recystallization and deposition of aragonite, the authors infer that the geologic site of diagenesis both for forming the secondary aragonitic phases and for the enhancement of the [sup 234]U content in the fossil corals was the marine environment. It is possible that the textural and Na, S, and Mg trace element contents of fossil corals be used to ascertain the reliability of fossil coral skeletons for U-[sup 230]Th dating. The basic problem of identifying a priori unaltered coral skeletons for [sup 230]Th dating is not yet resolved. 64 refs., 16 figs., 5 tabs.

  13. Absolute L X-ray intensities in the decays of 230Th, 234U, 238Pu and 244Cm

    NASA Astrophysics Data System (ADS)

    Johnston, Peter N.; Burns, Peter A.

    1995-02-01

    The absolute L X-ray emission rates of 230Th, 234U, 238Pu and 244Cm have been measured. The rates were obtained by an alpha-particle gated photon spectrometry technique involving the use of a highly calibrated Ge(HP) detector in coincidence with a SiSB detector. The directional correlation between L X-rays and alpha-particles has been accounted for. The present results are compared with previous experimental values and theoretical estimates. Agreement with theoretical estimates is good, however few of the previous experimental values agree with the present work. Differences with previous work partly seem to lie with the detector calibration.

  14. Variation of uranium isotopic composition in soil within the JCO grounds from the 30 September 1999 criticality accident at JCO, Tokai-mura, Japan.

    PubMed

    Yamamoto, Masayoshi; Kawabata, Yoshiko; Murata, Yoshimasa; Komura, Kazuhisa

    2002-08-01

    Following the 30 September 1999 criticality accident at JCO, 29 surface and 3 core soil samples were collected inside and outside the JCO grounds to evaluate possible contamination by 235U-enriched uranium (18.8%) being handled at the time of the accident. Uranium (234U, 235U, and 238U) and thorium (228Th, 230Th, and 232Th) isotopes were determined by alpha-spectrometry and ICP-MS after radiochemical separation. Concentrations of 238U and 234U ranged from 11.3 to 63.5 and 11.6 to 360 mBq g(-1), respectively. Higher amounts of 238U and/or 234U were found in the vicinity of the uranium conversion building. The calculated 234U/235U activity ratios ranged from a 1.0 radioactive equilibrium value to an unusually high 5.7 value. Several of the soil samples showed considerably higher 235U/238U atomic ratios (1.06-4.37%) than 0.725% for natural uranium. Based on the assumption that measured U-series nuclides in soil samples taken from the JCO grounds were almost at radioactive equilibrium up to 230Th, excess uranium could be calculated for each sample. The results suggest that the excess uranium in the soils have lower 235U/238U atomic ratios (a few %) than the 18.8% enrichment of the precipitation tank uranium.

  15. Fission fragments mass distributions of nuclei populated by the multinucleon transfer channels of the 18O + 232Th reaction

    NASA Astrophysics Data System (ADS)

    Léguillon, R.; Nishio, K.; Hirose, K.; Makii, H.; Nishinaka, I.; Orlandi, R.; Tsukada, K.; Smallcombe, J.; Chiba, S.; Aritomo, Y.; Ohtsuki, T.; Tatsuzawa, R.; Takaki, N.; Tamura, N.; Goto, S.; Tsekhanovich, I.; Petrache, C. M.; Andreyev, A. N.

    2016-10-01

    It is shown that the multinucleon transfer reactions is a powerful tool to study fission of exotic neutron-rich actinide nuclei, which cannot be accessed by particle-capture or heavy-ion fusion reactions. In this work, multinucleon transfer channels of the 18O + 232Th reaction are used to study fission of fourteen nuclei 231,232,233,234Th, 232,233,234,235,236Pa, and 234,235,236,237,238U. Identification of fissioning nuclei and of their excitation energy is performed on an event-by-event basis, through the measurement of outgoing ejectile particle in coincidence with fission fragments. Fission fragment mass distributions are measured for each transfer channel, in selected bins of excitation energy. In particular, the mass distributions of 231,234Th and 234,235,236Pa are measured for the first time. Predominantly asymmetric fission is observed at low excitation energies for all studied cases, with a gradual increase of the symmetric mode towards higher excitation energy. The experimental distributions are found to be in general agreement with predictions of the fluctuation-dissipation model.

  16. Retardation of [sup 238]U and [sup 232]Th decay chain radionuclides in Long Island and Connecticut aquifers

    SciTech Connect

    Copenhaver, S.A.; Krishnaswami, S.; Turekian, K.K. ); Epler, N.; Cochran, J.K. )

    1993-02-01

    Knowledge of the ability of an aquifer to retard the groundwater transport of toxic or radioactive ions can be inferred from the analysis of groundwater for the radionuclides of the [sup 238]U- and [sup 232]Th-decay chains. Groundwaters of varying chemical composition were analyzed from wells in Long Island, New York, and Connecticut. Aquifer lithologies are arkose, quartz sandstone, granite, and glacial drift. Adsorption (k[sub 1]) and desorption (k[sub 2]) coefficients for Ra and Pb were calculated using [sup 222]Rn activity as a measure of the supply of other [alpha]-recoil nuclides. Laboratory tests of the validity of this assumption were made by measuring the flux of [sup 224]Ra and [sup 222]Rn from aquifer solids. The ratio k[sub 1]/k[sub 2] is the distribution coefficient, K, which is effective equal to R[sub f], the retardation factor. The average value of K for Ra is 6 [times] 10[sup 2] in Long Island aquifers and 5 [times] 10[sup 4] in Connecticut. The distribution coefficient for Pb is 10[sup 4] in Long Island and 10[sup 5] in Connecticut. Results from this and other studies reveal a strong dependence of retardation on pH, f[sub o[sub 2

  17. Non-destructive determination of uranium, thorium and 40K in tobacco and their implication on radiation dose levels to the human body.

    PubMed

    Landsberger, S; Lara, R; Landsberger, S G

    2015-11-01

    The naturally occurring radionuclides of (235)U, (238)U and (232)Th and their daughter products are a potential major source of anthropogenic radiation to tobacco smokers. Often overlooked is the presence of (40)K in tobacco and its implication to radiation dose accumulation in the human body. In this study, these three radiation sources have been determined in four typical US cigarettes using neutron activation analysis (NAA). The NAA reactions of (238)U(n,γ)(239)U, (232)Th(n,γ)(233)Th and (41)K(n,γ)(42)K were used to determine (235)U, (238)U and (232)Th and (40)K, respectively. The activity of (238)U can easily be determined by epithermal NAA of the (238)U(n,γ)(239)U reaction, and the activity of (235, 234)U can easily be deduced. Using isotopic ratios, the activity due to (40)K was found by the determined concentrations of (41)K (also by epithermal neutrons) in the bulk material. Each gram of total potassium yields 30 Bq of (40)K. The annual effective dose for smokers using 20 cigarettes per day was calculate to be 14.6, 137 and 9 μSv y(-1) for (238,235,) (234)U, (232)Th and (40)K, respectively. These values are significantly lower that the dose received from (210)Po except for (232)Th.

  18. A modern framework for the interpretation of 238U/235U in studies of ancient ocean redox

    NASA Astrophysics Data System (ADS)

    Andersen, M. B.; Romaniello, S.; Vance, D.; Little, S. H.; Herdman, R.; Lyons, T. W.

    2014-08-01

    The abundance and isotope composition of redox sensitive elements in ancient sediments are increasingly used to understand the past ocean's geochemical state and the oxygenation history of the Earth. The redox transition of uranium (U) from soluble U+6 to relatively insoluble U+4 and its subsequent incorporation into reduced sediments has been used to deduce the redox state of the oceans in the past. Furthermore, recent analytical improvements have revealed significant 238U/235U fractionation during this redox transition, offering the potential for U isotopes to act as a redox proxy. However, the development of U isotopes as a geochemical tracer requires that U isotope systematics associated with redox changes, are well-characterized. This study focuses on U isotopes in recent sediments from the two largest modern anoxic ocean basins, the Black Sea and the Cariaco Basin, with the aim of advancing our understanding of the U isotope systematics in reducing marine environments. These anoxic sediments have high U accumulation rates and high 238U/235U ratios relative to seawater, in general agreement with a process that accumulates reduced U with a heavy isotopic composition. Using Al and Ca concentrations to correct for detrital and biogenic carbonate-bound U, we estimate the reduced authigenic U accumulated in the sediments and its 238U/235U. These results highlight the importance of isotopic mass balance constraints during diffusive transport and reaction of U from seawater and through pore-water, affecting the observed 238U/235U in sediments. Using these constraints, the average percentages of U depletion from top to bottom of the water column can be estimated, assuming batch-removal of U into anoxic sediments in a restricted basin. Using this framework, 238U/235U in modern anoxic sediments from the Black Sea imply U depletions in the water column of ∼30%, which is close to the observed ∼40% U depletion in the modern Black Sea water column at these depths

  19. Uranium concentrations and 234U/238U activity ratios in fault-associated groundwater as possible earthquake precursors

    NASA Astrophysics Data System (ADS)

    Finkel, R. C.

    In order to assess the utility of uranium isotopes as fluid phase earthquake precursors, uranium concentrations and 234U/238U activity ratios have been monitored on a monthly or bimonthly basis in water from 24 wells and springs associated with Southern California fault zones. Uranium concentrations vary from 0.002 ppb at Indian Canyon Springs on the San Jacinto fault to 8.3 ppb at Lake Hughes well on the San Andreas fault in the Palmdale area. 234U/238U activity ratios vary from 0.88 at Agua Caliente Springs on the Elsinore fault to 5.4 at Niland Slab well on the San Andreas fault in the Imperial Valley. There was one large earthquake in the study area during 1979, the 15 October 1979 M=6.6 Imperial Valley earthquake. Correlated with this event, uranium concentrations varied by a factor of more than 60 and activity ratios by a factor of 3 at the Niland Slab site, about 70 km from the epicenter. At the other sites monitored, uranium concentrations varied in time, but with no apparent pattern, while uranium activity ratios remained essentially constant throughout the monitoring period.

  20. 234U and 238U concentration in brine from geopressured aquifers of the northern Gulf of Mexico basin

    USGS Publications Warehouse

    Kraemer, T.F.

    1981-01-01

    The 234U and 238U concentration in brine from six Gulf Coast geopressured aquifers has been determined. The results reveal very low uranium concentrations (from 0.003 to 0.03 ??g/l) and uranium activity ratios slightly greater than unity (from 1.06 to 1.62). Reducing conditions within the aquifers are responsible for the low uranium concentrations. The uranium activity ratios observed are well below those calculated using theoretical considerations of alpha-particle recoil effects. This can be explained by interference with alpha-recoil nuclides entering the liquid phase as a result of quartz overgrowths on sand grains and high-temperature re-equilibration that tends to minimize the effects of the alpha-recoil process. The fact that the uranium activity ratios of the brines are slightly greater than unity instead of the equilibrium value of 1.000 indicates that either the alpha particle recoil blocking and re-equlibration effects are not complete or that another process is operative that enriches the fluid in excess 234U by selectively removing uranium from radiation induced damage sites in the mineral (sand grain) matrix. ?? 1981.

  1. Crustal subsidence rate off Hawaii determined from sup 234 U/ sup 238 U ages of drowned coral reefs

    SciTech Connect

    Ludwig, K.R.; Szabo, B.J.; Simmons, K.R. ); Moore, J.G. )

    1991-02-01

    A series of submerged coral reefs off northwestern Hawaii was formed during (largely glacial) intervals when the rate of local sea-level rise was less than the maximum upward growth rate of the reefs. Mass-spectrometric {sup 234}U/{sup 238}U ages for samples from six such reefs range from 17 to 475 ka and indicate that this part of the Hawaiian Ridge has been subsiding at a roughly uniform rate of 2.6 mm/yr for the past 475 ka. The {sup 234}U/{sup 238}U ages are in general agreement with model ages of reef drowning (based on estimates of paleo-sea-level stands derived from oxygen-isotope ratios of deep-sea sediments), but there are disagreements in detail. The high attainable precision ({plus minus}10 ka or better on samples younger than {approximately}800 ka), large applicable age range, relative robustness against open-system behavior, and ease of analysis for this technique hold great promise for future applications of dating of 50-1,000 ka coral.

  2. Measurements of /sup 234/U, /sup 238/U and /sup 230/Th in excreta of uranium-mill crushermen

    SciTech Connect

    Fisher, D.R.; Jackson, P.O.; Brodacynski, G.G.; Scherpelz, R.I.

    1982-07-01

    Uranium and thorium levels in excreta of uranium mill crushermen who are routinely exposed to airborne uranium ore dust were measured. The purpose was to determine whether /sup 230/Th was preferentially retained over either /sup 234/U or /sup 238/U in the body. Urine and fecal samples were obtained from fourteen active crushermen with long histories of exposure to uranium ore dust, plus four retired crushermen and three control individuals for comparison. Radiochemical procedures were used to separate out the uranium and thorium fractions, which were then electroplated on stainless steel discs and assayed by alpha spectrometry. Significantly greater activity levels of /sup 234/U and /sup 238/U were measured in both urine and fecal samples obtained from uranium mill crushermen, indicating that uranium in the inhaled ore dust was cleared from the body with a shorter biological half-time than the daughter product /sup 230/Th. The measurements also indicated that uranium and thorium separate in vivo and have distinctly different metabolic pathways and transfer rates in the body. The appropriateness of current ICRP retention and clearance parameters for /sup 230/Th in ore dust is questioned.

  3. 238U and 235U isotope fractionation upon oxidation of uranium-bearing rocks by fracture waters

    NASA Astrophysics Data System (ADS)

    Chernyshev, I. V.; Golubev, V. N.; Chugaev, A. V.; Mandzhieva, G. V.

    2016-10-01

    The variations in 238U/235U values accompanying mobilization of U by fracture waters from uranium-bearing rocks, in which U occurs as a fine impregnation of oxides and silicates, were studied by the high-precision (±0.07‰) MC-ICP-MS method. Transition of U into the aqueous phase in the oxidized state U(VI) is accompanied by its isotope fractionation with enrichment of dissolved U(VI) in the heavy isotope 238U up to 0.32‰ in relation to the composition of the solid phases. According to the sign, this effect is consistent with the tendency of the behavior of 238U and 235U upon interaction of river waters with rocks of the catchment areas [11] and with the effect observed during oxidation of uraninite by the oxygen-bearing NaHCO3 solution [12].

  4. An examination of the potential fission-bomb weaponizability of nuclides other than 235U and 239Pu

    NASA Astrophysics Data System (ADS)

    Reed, B. Cameron

    2017-01-01

    Long-lived fissionable isotopes other than uranium-235 and plutonium-239 are examined for possible use in fission weapons. A few other isotopes are potentially weaponizable and in some cases have been tried or their criticality experimentally demonstrated. In most cases, however, promising isotopes are either extremely rare, difficult to produce in quantity, or hazardous to handle. Some isotopes can serve to boost the yield of fission weapons, but 235U and 239Pu are likely to remain the only practical primary fuels for nuclear weapons. In view of this, and the fact that this analysis gives no engineering details on the design of nuclear weapons, this paper will be of no assistance to putative bomb-makers; rather, my purpose is to clarify the physics similarities between 235U and 239Pu that make them suitable candidates for fission weapons.

  5. A beta-alpha coincidence counting system for measurement of trace quantities of 238U and 232Th in aqueous samples at the Sudbury Neutrino Observatory.

    NASA Astrophysics Data System (ADS)

    Dawson, M.; Doucas, G.; Fergani, H.; Jelley, N. A.; Majerus, S.; O'Keeffe, H. M.; Peeters, S. J. M.; Perry, C.

    2016-08-01

    The Sudbury Neutrino Observatory experiment was built to measure the total flux of 8B solar neutrinos via the neutral current disintegration deuterium nuclei. This process can be mimiced by daughter isotopes of 232Th and 238U which can photodisintegrate the deuterium nucleus. Measurement of the concentration of such radioisotopes in the heavy water was critical to the success of the experiment. A radium assay technique using Hydrous Titanium Oxide coated filters was developed for this purpose and it was used in conjunction with a delayed beta-alpha coincidence counting system. The design, calibration and operation of this counting system are described in this paper. The counting efficiency for 232Th (224Ra) and 238U (226Ra) were measured to be 50 ± 5% and 62 ± 7%

  6. 226Ra, 232Th and 40K contents in water samples in part of central deserts in Iran and their potential radiological risk to human population

    PubMed Central

    2014-01-01

    Background The radiological quality of 226Ra, 232Th and 40K in some samples of water resources collected in Anarak-Khour a desertic area, Iran has been measured by direct gamma ray spectroscopy using high purity germanium detector in this paper. Result The concentration ranged from ≤0.5 to 9701 mBq/L for 226Ra; ≤0.2 to 28215 mBq/L for 232Th and < MDA to 10332 mBq/L for 40K. The radium equivalent activity was well below the defined limit of 370Bq/L. The calculated external hazard indices were found to be less than 1 which shows a low dose. Conclusion These results can be contributed to the database of this area because it may be used as disposal sites of nuclear waste in future. PMID:24883192

  7. Revision and reevaluation of the {sup 235}U cross sections for ENDF/B-VI to address integral data measurements

    SciTech Connect

    Leal, L.C.

    1995-04-01

    The ENDF/B-VI cross-section representation of the {sup 235}U in the resolved energy range is based on the reduced R-matrix Reich-Moore formalism. The evaluation extends the resolved energy range up to 2250 eV to allow better treatment of the energy self-shielding effects on the cross sections. In the ENDF/B-VI library, the Reich-Moore resonance parameters consist of eleven disjoint energy consecutive sets. The intent of this paper is to address the need to reevaluate the {sup 235}U cross sections in the resolved energy range to overcome the deficiencies of the data in reproducing integral benchmark results, in particular, the discrepancy in reproducing the capture-to-fission ratio. The cross-section representation based on the eleven disjoint sets of resonance parameters restricts the use of the ENDF/B-VI {sup 235}U resonance data m applications based on the continuous-energy approach. This limitation is also addressed.

  8. Measurement of 226Ra, 232Th, 137Cs and 40K activities of Wheat and Corn Products in Ilam Province – Iran and Resultant Annual Ingestion Radiation Dose

    PubMed Central

    CHANGIZI, Vahid; SHAFIEI, Elham; ZAREH, Mohammad Reza

    2013-01-01

    Background: Background: Natural background radiation is the main source of human exposure to radioactive material. Soils naturally have radioactive mineral contents. The aim of this study is to determine natural (238 U, 232 Th, 40 K) and artificial (137 Cs) radioactivity levels in wheat and corn fields of Eilam province. Methods: HPGe detector was used to measure the concentration activity of 238 U and 232 Th series, 40 K and 137 Cs in wheat and corn samples taken from different regions of Eilam province, in Iran. Results: In wheat and corn samples, the average activity concentrations of 226 Ra, 232 Th, 40 K and 137 Cs were found to be 1, 67, 0.5, 91.73, 0.01 and 0.81, 0.85, 101.52, 0.07 Bq/kg (dry weight), respectively. H ex and H in in the present work are lower than 1. The average value of H ex was found to be 0.02 and 0.025 and average value of H in to be found 0.025 and 0.027 in wheat fields samples and corn samples in Eilam provinces, respectively. The obtained values of AGDE are 30.49 mSv/yr for wheat filed samples and 37.89 mSv/yr for corn samples; the AEDE rate values are 5.28 mSv/yr in wheat filed samples and this average value was found to be 6.13 mSv/yr in corn samples in Eilam. Transfer factors (TFs) of long lived radionuclide such as 137 Cs, 226 Ra, 232 Th and 40 K from soils to corn and wheat plants have been studied by radiotracer experiments. Conclusion: The natural radioactivity levels in Eilam province are not at the range of high risk of morbidity and are under international standards. PMID:26056646

  9. Comparison of activity concentration of 238U, 232Th and 40K in different Layers of subsurface Structures in Dei-Dei and Kubwa, Abuja, northcentral Nigeria

    NASA Astrophysics Data System (ADS)

    Maxwell, Omeje; Wagiran, Husin; Ibrahim, Noorddin; Lee, Siak Kuan; Sabri, Soheil

    2013-10-01

    The study of activity concentration of 232Th, 238U and 40K of rock samples from site one (S1L1-S1L11, 70 m) and site two (S2L1-S2L9, 60 m) boreholes in Dei-Dei and Kubwa was presented and the first time in the region to be compared. Activity concentrations were analysed using a high resolution co-axial HPGe gamma ray spectrometer system. The activity concentration ranges in site one borehole were from 45±1 to 98±6 Bq kg-1 for 232Th, from 18±2 to 37±4 Bq kg-1 for 238U and from 254 ±32 Bq kg-1 to 1195 ±151 Bq kg-1 for 40K. The activity concentration ranges in site two borehole were from 32±3 to 84±7 Bq kg-1 for 232Th, from 15±2 to 52±5 Bq kg-1 for 238U and from 119±15 to 705±94 for 40K Bq kg-1. Significantly higher concentration of 232Th and 238U occurs in samples collected from S1L7, S1L11 and S2L1 layers. These zones experienced granitic intrusions produced by denudation and tectonism. 40K in rock samples of S1L4 and S2L4 activity concentrations is close; it could be that biotite granitic intrusion that is inferred as the formation in that layer reflects the same activity of potassium in rock's radioactivity measurement. The area requires further investigation of soil geochemistry and activity concentration of radionuclides in groundwater.

  10. Sources of alluvium in a coastal plain stream based on radionuclide signatures from the 238U and 232Th decay series

    NASA Astrophysics Data System (ADS)

    Yeager, Kevin M.; Santschi, Peter H.; Phillips, Jonathan D.; Herbert, Bruce E.

    2002-11-01

    Discerning alluvial sources and their change over time or distance is a fundamental question in hydrology and geology, often critical in identifying impacts of human and natural perturbations on fluvial systems. Surfaces of upland interfluves and subsoils, sources of alluvium in the lower Loco Bayou basin, Texas, were distinguished using the isotope ratios 226Ra/232Th, 226Ra/230Th, and 230Th/232Th. Channel alluvium indicates a transition from interfluve surface to subsoil sources during flood (subsoil ˜34% to ˜91%, over about 8 km) and bank-full stages (subsoil ˜9% to ˜74%, over about 12 km), with distance downstream. These results indicate strong coupling between hillslope and channel processes, reflecting land use change from forested to agricultural, concentrated in lower Loco Bayou. This methodology shows that sediment sources can be differentiated based upon landscape placement where lithologic contrast is absent. The geochemistry, long half-lives, and fractionation of 238U and 232Th decay series radionuclides during pedogenic and fluvial processes in humid climates suggest that these methods are applicable in a wide variety of fluvial systems.

  11. STUDY OF NATURAL RADIOACTIVITY (226Ra, 232Th AND 40K) IN SOIL SAMPLES FOR THE ASSESSMENT OF AVERAGE EFFECTIVE DOSE AND RADIATION HAZARDS.

    PubMed

    Bangotra, Pargin; Mehra, Rohit; Kaur, Kirandeep; Jakhu, Rajan

    2016-10-01

    The activity concentration of (226)Ra (radium), (232)Th (thorium) and (40)K (potassium) has been measured in the soil samples collected from Mansa and Muktsar districts of Punjab (India) using NaI (Tikl) gamma detector. The concentration of three radionuclides ((226)Ra, (232)Th and (40)K) in the studied area has been varied from 18±4 to 46±5, 53±7 to 98±8 and 248±54 to 756±110 Bq kg(-1), respectively. Radium equivalent activities (Raeq) have been calculated in soil samples for the assessment of the radiation hazards arising due to the use of these soil samples. The absorbed dose rate of (226)Ra, (232)Th and (40)K in studied area has been varied from 8 to 21, 33 to 61 and 9 to 25 nGy h(-1), respectively. The corresponding indoor and outdoor annual effective dose in studied area was 0.38 and 0.09 mSv, respectively. The external and internal hazard has been also calculated for the assessment of radiation hazards in the studied area.

  12. Assay Methods for 238U, 232Th, and 210Pb in Lead and Calibration of 210Bi Bremsstrahlung Emission from Lead

    SciTech Connect

    Orrell, John L.; Aalseth, Craig E.; Arnquist, Isaac J.; Eggemeyer, Tere A.; Glasgow, Brian D.; Hoppe, Eric W.; Keillor, Martin E.; Morley, Shannon M.; Myers, Allan W.; Overman, Cory T.; Shaff, Sarah M.; Thommasson, Kimbrelle S.

    2016-02-13

    Assay methods for measuring 238U, 232Th, and 210Pb concentrations in refined lead are presented. The 238U and 232Th concentrations are assayed via inductively coupled plasma mass spectrometry (ICP-MS) after anion exchange column separation on dissolved lead samples. The 210Pb concentration is inferred through α-spectroscopy of a daughter isotope, 210Po, after chemical precipitation separation on dissolved lead samples. Subsequent to the 210Po α-spectroscopy assay, a method for evaluating 210Pb concentrations in solid lead samples was developed via measurement of bremsstrahlung radiation from β-decay of a daughter isotope, 210Bi, by employing a 14-crystal array of high purity germanium (HPGe) detectors. Ten sources of refined lead were assayed. The 238U concentrations were <34 microBq/kg and the 232Th concentrations ranged <0.6 – 15 microBq/kg, as determined by the ICP-MS assay method. The 210Pb concentrations ranged from ~0.1 – 75 Bq/kg, as inferred by the 210Po α-spectroscopy assay method.

  13. Measurement of cross sections for the {sup 232}Th(P,4n){sup 229}Pa reaction at low proton energies

    SciTech Connect

    Jost, C. U.; Griswold, J. R.; Bruffey, S. H.; Mirzadeh, S.; Stracener, D. W.; Williams, C. L.

    2013-04-19

    The alpha-emitters {sup 225}Ac and {sup 213}Bi are of great interest for alpha-radioimmunotherapy which uses radioisotopes attached to cancer-seeking antibodies to efficiently treat various types of cancers. Both radioisotopes are daughters of the long-lived {sup 229}Th(t{sub 1/2} = 7880y). {sup 229}Th can be produced by proton irradiation of {sup 232}Th and {sup 230}Th, either directly or through production of isobars that beta-decay into {sup 229}Th. To obtain excitation functions, {sup 232}Th and {sup 230}Th have been irradiated at the On-Line Test Facility at the Holifield Radioactive Ion Beam Facility at ORNL. Benchmark tests conducted with Cu and Ni foils show very good agreement with literature results. The experiments with thorium targets were focused on the production of {sup 229}Pa and its daughter {sup 225}Ac from both {sup 232}Th and {sup 230}Th. Differential cross-sections for production of {sup 229}Pa and other Pa isotopes have been obtained.

  14. Activity concentration, transfer factors and resultant radiological risk of 226Ra, 232Th, and 40K in soil and some vegetables consumed in Selangor, Malaysia

    NASA Astrophysics Data System (ADS)

    Solehah, A. R.; Yasir, M. S.; Samat, S. B.

    2016-11-01

    The activity concentrations of the natural radionuclides 226Ra, 232Th, and 40K were determined in vegetable crops consumed by Malaysian people in Sungai Besar, Selangor. Sample of vegetables and the soil where the crops were cultivated and collected at five different location. The activity concentrations in Bq/kg of 226Ra, 232Th, and 40K were measured by the gamma-ray spectroscopy using the high purity germanium detector. The range activity concentration in soil is between 51.81 and 71.84 Bq/kg, 64.18 and 78.00 Bq/kg, and 210.49 and 244.29 Bq/kg for 226Ra, 232Th, and 40K, respectively. The activity concentration of 226Ra, 232Th, and 40K in vegetables were found to be in the range of 2.06 to 5.44 Bq/kg, Not Detectable to 0.61 Bq/kg, and 101.00 to 1223.09 Bq/kg, respectively. The activity concentration in both soil and vegetables were all less than lower limit stated by UNSCEAR. The Transfer Factors range value for 226Ra, 232Th, and 40K varied from 0.02 to 0.06, 0.003 to 0.008, and 1.79 to 5.19 respectively. Radium equivalent for soil range from 165.57 to 194.84 Bq/kg. It was within the international accepted value (370 Bq/kg). Absorb dose rate for soil range between 73.5 to 86.40 nGyh-1, in safe range from limit of international accepted value (55nGyh-1). Effective dose rate is found to be in range of 0.09 to 0.11 mSvy-1 for soil which is less than 2.4 mSv/y. External and Internal Hazard indices of soil was all below 1, within agreement of other researcher and UNSCEAR. The estimation of the consequent radiological risk due to the presence of those radionuclides is significantly low.

  15. Coupling groundwater residence time and 234U/238U isotopic ratios in a granitic catchment (Vosges, Eastern France)

    NASA Astrophysics Data System (ADS)

    Viville, Daniel; Aquilina, Luc; Ackerer, Julien; Chatton, Eliot; Labasque, Thierry; Pierret, Marie-Claire; Granet, Mathieu; Perrone, Thierry; Chabaux, François

    2016-04-01

    Weathering processes are active in surface waters but groundwater also represents no neglectable chemical fluxes. As residence-time in groundwater are high, silicate weathering might take place and control Si, Ca and C fluxes. Weathering processes can be deduced from U isotopic ratios but the kinetics of these processes remain relatively poorly constrained. In order to better characterize these processes, we have coupled residence-times deduced from anthropogenic gases (CFC and SF6) analysis and 234U/238U isotopic ratios determination. Samples were collected in the Strengbach catchment (Hydro-geochemical Observatory OHGE, Vosges, eastern France). Two campaigns were carried out in May and August 2015 during two highly contrasted hydro-climatic periods. Both springs and boreholes down to 80 m depth have been sampled. A very clear geochemical distinction is observed between groundwater from surface springs and deeper groundwater from boreholes. Springs show much lower residence-time (few years) and specific chemical composition. Deeper groundwater have residence-time of several decades and different geochemical composition. A clear SF6 production is observed with increasing SF6 concentrations with residence-time. The campaign of May is characterized by highly groundwater levels and spring fluxes. All groundwater show very low residence time, except in the boreholes at depth greater than 40 m. Conversely, during low groundwater-level period in August, the residence times are much higher and CFC concentrations indicate a large mixing process between surface groundwater and deeper levels. The 234U/238U isotopic ratios confirm this vertical zonation in the boreholes, with much higher activity ratios in the deep ground-waters from borehole than in the surface and spring waters; Such high U activity ratios are indicative of long water-rock interactions, which is consistent with the long residence times deducted from the CFC and SF6 data.

  16. Measurements of absolute delayed neutron yield and group constants in the fast fission of {sup 235}U and {sup 237}Np

    SciTech Connect

    Loaiza, D.J.; Brunson, G.; Sanchez, R.; Butterfield, K.

    1998-03-01

    The delayed neutron activity resulting from the fast induced fission of {sup 235}U and {sup 237}Np has been studied. The six-group decay constants, relative abundances, and absolute yield of delayed neutrons from fast fission of {sup 235}U and {sup 237}Np were measured using the Godiva IV fast assembly at the Los Alamos Critical Experiments Facility. The absolute yield measured for {sup 235}U was 0.0163 {+-} 0.0008 neutron/fission. This value compares very well with the well-established Keepin absolute yield of 0.0165 {+-} 0.0005. The absolute yield value measured for {sup 237}Np was 0.0126 {+-} 0.0007. The measured delayed neutron parameters for {sup 235}U are corroborated with period (e-folding time) versus reactivity calculations.

  17. Current Issues in Nuclear Data Evaluation Methodology: {sup 235}U Prompt Fission Neutron Spectra and Multiplicity for Thermal Neutrons

    SciTech Connect

    Trkov, A.; Capote, R.; Pronyaev, V.G.

    2015-01-15

    Issues in evaluation methodology of the prompt fission neutron spectra (PFNS) and neutron multiplicity for the thermal-neutron-induced fission of the {sup 235}U are discussed. The inconsistency between the experimental differential and integral data is addressed. By using differential data as ”shape data” good consistency was achieved between available sets of differential data. Integral dosimetry data have been used to define the PFNS slope at high outgoing neutron energies, where the quality of the differential data is poor. The inclusion into the fit of measured integral (spectrum-averaged) cross sections had a very small impact in the region where differential PFNS data are abundant and accurate, but removed the discrepancy with integral data at higher neutron emission energies. All experimental data are consistently fitted giving a PFNS average energy of 2.008 MeV. The impact on criticality prediction of the newly evaluated PFNS was tested. The highly enriched {sup 235}U solution assemblies with high leakage HEU-SOL-THERM-001 and HEU-SOL-THERM-009 benchmarks are the most sensitive to the PFNS. Criticality calculations for those solutions show a significant increase in reactivity if the average neutron energy of the fission neutrons is reduced from the ENDF/B-VI.5 value of 2.03 MeV. The proposed reduction of the PFNS average energy by 1.1% can be compensated by reducing the average number of neutrons per fission ν{sup ¯} at the thermal energy to the Gwin et al. measured value. The simple least-squares PFNS fit was confirmed by a more sophisticated combined fit of differential PFNS data for {sup 233,235}U, {sup 239}Pu and {sup 252}Cf nuclides with the generalised least-squares method using the GMA and GANDR codes.

  18. Current Issues in Nuclear Data Evaluation Methodology: 235U Prompt Fission Neutron Spectra and Multiplicity for Thermal Neutrons

    NASA Astrophysics Data System (ADS)

    Trkov, A.; Capote, R.; Pronyaev, V. G.

    2015-01-01

    Issues in evaluation methodology of the prompt fission neutron spectra (PFNS) and neutron multiplicity for the thermal-neutron-induced fission of the 235U are discussed. The inconsistency between the experimental differential and integral data is addressed. By using differential data as "shape data" good consistency was achieved between available sets of differential data. Integral dosimetry data have been used to define the PFNS slope at high outgoing neutron energies, where the quality of the differential data is poor. The inclusion into the fit of measured integral (spectrum-averaged) cross sections had a very small impact in the region where differential PFNS data are abundant and accurate, but removed the discrepancy with integral data at higher neutron emission energies. All experimental data are consistently fitted giving a PFNS average energy of 2.008 MeV. The impact on criticality prediction of the newly evaluated PFNS was tested. The highly enriched 235U solution assemblies with high leakage HEU-SOL-THERM-001 and HEU-SOL-THERM-009 benchmarks are the most sensitive to the PFNS. Criticality calculations for those solutions show a significant increase in reactivity if the average neutron energy of the fission neutrons is reduced from the ENDF/B-VI.5 value of 2.03 MeV. The proposed reduction of the PFNS average energy by 1.1% can be compensated by reducing the average number of neutrons per fission νbar at the thermal energy to the Gwin et al. measured value. The simple least-squares PFNS fit was confirmed by a more sophisticated combined fit of differential PFNS data for 233,235U, 239Pu and 252Cf nuclides with the generalised least-squares method using the GMA and GANDR codes.

  19. Energy dependence of mass, charge, isotopic, and energy distributions in neutron-induced fission of 235U and 239Pu

    NASA Astrophysics Data System (ADS)

    Pasca, H.; Andreev, A. V.; Adamian, G. G.; Antonenko, N. V.; Kim, Y.

    2016-05-01

    The mass, charge, isotopic, and kinetic-energy distributions of fission fragments are studied within an improved scission-point statistical model in the reactions 235U+n and 239Pu+n at different energies of the incident neutron. The charge and mass distributions of the electromagnetic- and neutron-induced fission of 214,218Ra, 230,232,238U are also shown. The available experimental data are well reproduced and the energy-dependencies of the observable characteristics of fission are predicted for future experiments.

  20. Neutron multiplicity in the fission of 238U and 235U with neutrons up to 200 MeV.

    PubMed

    Ethvignot, T; Devlin, M; Duarte, H; Granier, T; Haight, R C; Morillon, B; Nelson, R O; O'Donnell, J M; Rochman, D

    2005-02-11

    Prompt-fission-neutron multiplicities were measured for 238U(n,f) and 235U(n,f) from 0.4 to 200 MeV. The data are of great importance in connection with accelerator-coupled nuclear reactor systems incinerating actinides. We report that fission induced by 200 MeV neutrons produces approximately 10 more prompt neutrons than fission induced by reactor neutrons. Most neutrons are evaporated from the fission fragments and the prefission compound nucleus, as the preequilibrium emission of energetic neutrons accounts for a maximum of 15% of the prompt neutrons at 200 MeV.

  1. 234U and 230Th determination by FIA-ICP-MS and application to uranium-series disequilibrium in marine samples.

    PubMed

    Godoy, Maria Luiza D P; Godoy, José Marcus; Kowsmann, Renato; Dos Santos, Guaciara M; Petinatti da Cruz, Rosana

    2006-01-01

    A 234U and 230Th determination method based on an extraction chromatographic separation on a flow injection system coupled to a quadruple ICP-MS was developed. Two-milliliter UTEVA (Eichrom Co.) cartridges were applied as separation tool and 236U and 229Th as spikes. Loading and washing steps were carried out in 3 M HNO3 solution and 0.05 M ammonium oxalate applied to elute both uranium and thorium. The method was applied initially to the IAEA-327 soil reference sample and NIST SRM 4357 ocean sediment reference material, with the obtained 234U and 230Th concentrations in agreement with the reference levels. Samples from a deep-sea sediment core (2450 m water depth) were analyzed and based on 230Th/234U dating, a mean sedimentation rate of 3.3 cm ky(-1) was calculated. Samples from two sediment layers were also dated by 14C-AMS and the observed ages agree with the 230Th/234U results.

  2. 234U/238U isotope data from groundwater and solid-phase leachate samples near Tuba City Open Dump, Tuba City, Arizona

    USGS Publications Warehouse

    Johnson, Raymond H.; Horton, Robert J.; Otton, James K.; Ketterer, Michael K.

    2012-01-01

    This report releases 234U/238U isotope data, expressed as activity ratios, and uranium concentration data from analyses completed at Northern Arizona University for groundwater and solid-phase leachate samples that were collected in and around Tuba City Open Dump, Tuba City, Arizona, in 2008.

  3. Measurement of the Total Kinetic Energy Release (TKE) in 232 Th(n,f) with En = 2.59 - 87.31 MeV

    NASA Astrophysics Data System (ADS)

    King, Jonathan; Yanez, Ricardo; Barrett, Jonathan; Loveland, Walter; Tovesson, Fredrik; Fotiades, Nick; Lee, Hye Young

    2015-04-01

    Experimental results for the Total Kinetic Energy Release (TKE) of 232 Th(n,f) with En = 2.59 - 87.31 MeV will be presented. The experiment was performed at the 15R beamline at the Weapons Neutron Research(WNR) facility at LANL-LANSCE. WNR provides a white spectrum of neutrons peaking at 2 MeV and reaching up to 800 MeV, with neutron energies being deduced from measurements of the neutron time of flight (TOF). A thin-backed 232 ThF4 target of 2 cm diameter with a thorium areal density of 178.9 μg/cm2 was placed between two arrays of Hammamatsu PIN diodes (active area 4 cm2 each). The beam was collimated to 1 cm diameter. The target was placed 45 degrees off of the beam axis, with the detectors at 60 degrees and 120 degrees from the beam axis. Over 25,000 fission fragment coincidence events were recorded, allowing for sixteen energy bins between 2.59 and 87.31 MeV. We believe that this will be the most comprehensive published measurement of the TKE for 232 Th(n,f) with En = 2.59 - 87.31 MeV. This work was supported in part by the Director, Office of Energy Research, Division of Nuclear Physics of the Office of High Energy and Nuclear Physics of the USDoE under Grant DE-FG06-97ER41026. This work has benefited from the use of the Los Alamos Neutron Science Center at the Los Alamos National Laboratory. This facility is funded by the USDoE under DOE Contract No. DE-AC52-06NA25396.

  4. Quantification of transfer of (238)U, (226)Ra, (232)Th, (40)K and (137)Cs in mosses of a semi-natural ecosystem.

    PubMed

    Dragović, S; Mihailović, N; Gajić, B

    2010-02-01

    There is a lack of appropriate data on transfer of some radionuclides on many terrestrial biota groups. To expand the available data concentration ratios of (238)U, (226)Ra, (232)Th, (40)K and (137)Cs in mosses are presented in this paper. The relationship between concentration ratios of radionuclides and physicochemical characteristics of the underlying soil was also investigated. The data on concentration ratios obtained here will provide a useful addition to the currently used database of transfer parameters, particularly for natural radionuclides.

  5. A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy

    NASA Astrophysics Data System (ADS)

    Knowles, Justin; Skutnik, Steven; Glasgow, David; Kapsimalis, Roger

    2016-10-01

    Rapid nondestructive assay methods for trace fissile material analysis are needed in both nuclear forensics and safeguards communities. To address these needs, research at the Oak Ridge National Laboratory High Flux Isotope Reactor Neutron Activation Analysis facility has developed a generalized nondestructive assay method to characterize materials containing fissile isotopes. This method relies on gamma-ray emissions from short-lived fission products and makes use of differences in fission product yields to identify fissile compositions of trace material samples. Although prior work has explored the use of short-lived fission product gamma-ray measurements, the proposed method is the first to provide a complete characterization of isotopic identification, mass ratios, and absolute mass determination. Successful single fissile isotope mass recoveries of less than 6% recovery bias have been conducted on standards of 235U and 239Pu as low as 12 ng in less than 10 minutes. Additionally, mixtures of fissile isotope standards containing 235U and 239Pu have been characterized as low as 198 ng of fissile mass with less than 7% recovery bias. The generalizability of this method is illustrated by evaluating different fissile isotopes, mixtures of fissile isotopes, and two different irradiation positions in the reactor. It is anticipated that this method will be expanded to characterize additional fissile nuclides, utilize various irradiation facilities, and account for increasingly complex sample matrices.

  6. Comparative measurement of prompt fission γ -ray emission from fast-neutron-induced fission of 235U and 238U

    NASA Astrophysics Data System (ADS)

    Lebois, M.; Wilson, J. N.; Halipré, P.; Oberstedt, A.; Oberstedt, S.; Marini, P.; Schmitt, C.; Rose, S. J.; Siem, S.; Fallot, M.; Porta, A.; Zakari, A.-A.

    2015-09-01

    Prompt fission γ -ray (PFG) spectra have been measured in a recent experiment with the novel directional fast-neutron source LICORNE at the ALTO facility of the IPN Orsay. These first results from the facility involve the comparative measurement of prompt γ emission in fast-neutron-induced fission of 235U and 238U . Characteristics such as γ multiplicity and total and average radiation energy are determined in terms of ratios between the two systems. Additionally, the average photon energies were determined and compared with recent data on thermal-neutron-induced fission of 235U . PFG spectra are shown to be similar within the precision of the present measurement, suggesting that the extra incident energy does not significantly impact the energy released by prompt γ rays. The origins of some small differences, depending on either the incident energy or the target mass, are discussed. This study demonstrates the potential of the present approach, combining an innovative neutron source and new-generation detectors, for fundamental and applied research on fission in the near future.

  7. A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy

    DOE PAGES

    Knowles, Justin R.; Skutnik, Steven E.; Glasgow, David C.; ...

    2016-06-23

    Rapid non-destructive assay methods for trace fissile material analysis are needed in both nuclear forensics and safeguards communities. To address these needs, research at the High Flux Isotope Reactor Neutron Activation Analysis laboratory has developed a generalized non-destructive assay method to characterize materials containing fissile isotopes. This method relies on gamma-ray emissions from short-lived fission products and capitalizes off of differences in fission product yields to identify fissile compositions of trace material samples. Although prior work has explored the use of short-lived fission product gamma-ray measurements, the proposed method is the first to provide a holistic characterization of isotopic identification,more » mass ratios, and absolute mass determination. Successful single fissile isotope mass recoveries of less than 6% error have been conducted on standards of 235U and 239Pu as low as 12 nanograms in less than 10 minutes. Additionally, mixtures of fissile isotope standards containing 235U and 239Pu have been characterized as low as 229 nanograms of fissile mass with less than 12% error. The generalizability of this method is illustrated by evaluating different fissile isotopes, mixtures of fissile isotopes, and two different irradiation positions in the reactor. Furthermore, it is anticipated that this method will be expanded to characterize additional fissile nuclides, utilize various irradiation sources, and account for increasingly complex sample matrices.« less

  8. Fission Fragment Angular Distribution measurements of 235U and 238U at CERN n_TOF facility

    NASA Astrophysics Data System (ADS)

    Leal-Cidoncha, E.; Durán, I.; Paradela, C.; Tarrío, D.; Leong, L. S.; Tassan-Got, L.; Audouin, L.; Altstadt, S.; Andrzejewski, J.; Barbagallo, M.; Bécares, V.; Bečvář, F.; Belloni, F.; Berthoumieux, E.; Billowes, J.; Boccone, V.; Bosnar, D.; Brugger, M.; Calviani, M.; Calviño, F.; Cano-Ott, D.; Carrapiço, C.; Cerutti, F.; Chiaveri, E.; Chin, M.; Colonna, N.; Cortés, G.; Cortés-Giraldo, M. A.; Diakaki, M.; Domingo-Pardo, C.; Dressler, R.; Dzysiuk, N.; Eleftheriadis, C.; Ferrari, A.; Fraval, K.; Ganesan, S.; García, A. R.; Giubrone, G.; Gómez-Hornillos, M. B.; Gonçalves, I. F.; González-Romero, E.; Griesmayer, E.; Guerrero, C.; Gunsing, F.; Gurusamy, P.; Hernández-Prieto, A.; Jenkins, D. G.; Jericha, E.; Kadi, Y.; Käppeler, F.; Karadimos, D.; Kivel, N.; Koehler, P.; Kokkoris, M.; Krtička, M.; Kroll, J.; Lampoudis, C.; Langer, C.; Lederer, C.; Leeb, H.; Lo Meo, S.; Losito, R.; Mallick, A.; Manousos, A.; Marganiec, J.; Martínez, T.; Massimi, C.; Mastinu, P. F.; Mastromarco, M.; Meaze, M.; Mendoza, E.; Mengoni, A.; Milazzo, P. M.; Mingrone, F.; Mirea, M.; Mondelaers, W.; Pavlik, A.; Perkowski, J.; Plompen, A.; Praena, J.; Quesada, J. M.; Rauscher, T.; Reifarth, R.; Riego, A.; Robles, M. S.; Roman, F.; Rubbia, C.; Sabaté-Gilarte, M.; Sarmento, R.; Saxena, A.; Schillebeeckx, P.; Schmidt, S.; Schumann, D.; Tagliente, G.; Tain, J. L.; Tsinganis, A.; Valenta, S.; Vannini, G.; Variale, V.; Vaz, P.; Ventura, A.; Versaci, R.; Vermeulen, M. J.; Vlachoudis, V.; Vlastou, R.; Wallner, A.; Ware, T.; Weigand, M.; Weiß, C.; Wright, T.; Žugec, P.

    2016-03-01

    Neutron-induced fission cross sections of 238U and 235U are used as standards in the fast neutron region up to 200 MeV. A high accuracy of the standards is relevant to experimentally determine other neutron reaction cross sections. Therefore, the detection effciency should be corrected by using the angular distribution of the fission fragments (FFAD), which are barely known above 20 MeV. In addition, the angular distribution of the fragments produced in the fission of highly excited and deformed nuclei is an important observable to investigate the nuclear fission process. In order to measure the FFAD of neutron-induced reactions, a fission detection setup based on parallel-plate avalanche counters (PPACs) has been developed and successfully used at the CERN-n_TOF facility. In this work, we present the preliminary results on the analysis of new 235U(n,f) and 238U(n,f) data in the extended energy range up to 200 MeV compared to the existing experimental data.

  9. Mass Yields and Average Total Kinetic Energy Release in Fission for 235U, 238U, and 239Pu

    NASA Astrophysics Data System (ADS)

    Duke, Dana

    2015-10-01

    Mass yield distributions and average total kinetic energy (TKE) in neutron induced fission of 235U, 238U, and 239Pu targets were measured with a gridded ionization chamber. Despite decades of fission research, our understanding of how fragment mass yields and TKE depend on incident neutron energy is limited, especially at higher energies (above 5-10 MeV). Improved accuracy in these quantities is important for nuclear technology as it enhances our simulation capabilities and increases the confidence in diagnostic tools. The data can also guide and validate theoretical fission models where the correlation between the fragment mass and TKE is of particular value for constraining models. The Los Alamos Neutron Science Center - Weapons Neutron Research (LANSCE - WNR) provides a neutron beam with energies from thermal to hundreds of MeV, well-suited for filling in the gaps in existing data and exploring fission behavior in the fast neutron region. The results of the studies on target nuclei 235U, 238U, and 239Pu will be presented with a focus on exploring data trends as a function of neutron energy from thermal through 30 MeV. Results indicate clear evidence of structure due to multi-chance fission in the TKE . LA-UR-15-24761.

  10. Determination of (238)U, (232)Th and (40)K activity concentrations in riverbank soil along the Chao Phraya river basin in Thailand.

    PubMed

    Santawamaitre, T; Malain, D; Al-Sulaiti, H A; Bradley, D A; Matthews, M C; Regan, P H

    2014-12-01

    The activity concentrations of (238)U, (232)Th and (40)K in riverbank soil along the Chao Phraya river basin was determined through gamma-ray spectrometry measurements made using a hyper-pure germanium detector in a low background configuration. The ranges of activity concentrations of (238)U, (232)Th and (40)K were found to be 13.9 ↔ 76.8, 12.9 ↔ 142.9 and 178.4 ↔ 810.7 Bq kg(-1), respectively. The anthropogenic radionuclide, (137)Cs, was not observed in statistically significant amounts above the background level in the current study. The absorbed gamma dose rate in air at 1 m above the ground surface, the outdoor annual effective dose equivalent, the values of the radium equivalent activity and the external hazard index associated with all the soil samples in the present work were evaluated. The results indicate that the radiation hazard from primordial radionuclides in all soil samples from the area studied in this current work is not significant.

  11. Assessment of (226)Ra, (238)U, (232)Th, (137)Cs and (40)K activities from the northern coastline of Oman Sea (water and sediments).

    PubMed

    Darabi-Golestan, F; Hezarkhani, A; Zare, M R

    2017-02-27

    Water and sediment samples were collected from northern coast of Oman Sea covering from Goatr to Hormoz canyon seaport. Water and sediment quality assessment for naturally or anthropogenic radionuclides at Oman Sea as a main strategic golf for trade and transit, is an important issue. Correspondence analysis (CA) by R-mode analysis represents that sigma(T)-temperature-conductivity-O2 parameters are well-correlated with (226)Ra, (232)Th and (40)K. Accordingly Q-mode analysis revealed an indicator samples of ST13W for different radionuclides, ST03W for O2, and simultaneously ST34W-ST21W-ST08W-ST04W for sigma(T) parameters. The CA results overlapped with factor and cluster analysis results that explained 85.8% of total variance of water samples. Descriptive analysis of sediments indicates more significant variation than water samples. The (232)Th and (226)Ra generally showing that ST13D to ST25D sediments that restricted to Pi Bashk coastline are concentrated from (137)Cs and (40)K. By comparison with reference-values from Iran and other parts of the world, they are acceptable with respect to environmental and radioisotope hazards.

  12. Assessment of environmental (226)Ra, (232)Th and (40)K concentrations in the region of elevated radiation background in Segamat District, Johor, Malaysia.

    PubMed

    Saleh, Muneer Aziz; Ramli, Ahmad Termizi; Alajerami, Yasser; Aliyu, Abubakar Sadiq

    2013-10-01

    Extensive environmental survey and measurements of gamma radioactivity in the soil samples collected from Segamat District were conducted. Two gamma detectors were used for the measurements of background radiation in the area and the results were used in the computation of the mean external radiation dose rate and mean weighted dose rate, which are 276 nGy h(-1) and 1.169 mSv y(-1), respectively. A high purity germanium (HPGe) detector was used in the assessment of activity concentrations of (232)Th, (226)Ra and (40)K. The results of the gamma spectrometry range from 11 ± 1 to 1210 ± 41 Bq kg(-1) for (232)Th, 12 ± 1 to 968 ± 27 Bq kg(-1) for (226)Ra, and 12 ± 2 to 2450 ± 86 Bq kg(-1) for (40)K. Gross alpha and gross beta activity concentrations range from 170 ± 50 to 4360 ± 170 Bq kg(-1) and 70 ± 20 to 4690 ± 90 Bq kg(-1), respectively. These results were used in the plotting of digital maps (using ARCGIS 9.3) for isodose. The results are compared with values giving in UNSCEAR 2000.

  13. Reactive transport of uranium in a groundwater bioreduction study: Insights from high-temporal resolution 238U/235U data

    NASA Astrophysics Data System (ADS)

    Shiel, A. E.; Johnson, T. M.; Lundstrom, C. C.; Laubach, P. G.; Long, P. E.; Williams, K. H.

    2016-08-01

    We conducted a detailed investigation of U isotopes in conjunction with a broad geochemical investigation during field-scale biostimulation and desorption experiments. This investigation was carried out in the uranium-contaminated alluvial aquifer of the Rifle field research site. In this well-characterized setting, a more comprehensive understanding of U isotope geochemistry is possible. Our results indicate that U isotope fractionation is consistently observed across multiple experiments at the Rifle site. Microbially-mediated reduction is suggested to account for most or all of the observed fractionation as abiotic reduction has been demonstrated to impart much smaller, often near-zero, isotopic fractionation or isotopic fractionation in the opposite direction. Data from some time intervals are consistent with a simple model for transport and U(VI) reduction, where the fractionation factor (ε = +0.65‰ to +0.85‰) is consistent with experimental studies. However, during other time intervals the observed patterns in our data indicate the importance of other processes in governing U concentrations and 238U/235U ratios. For instance, we demonstrate that departures from Rayleigh behavior in groundwater systems arise from the presence of adsorbed species. We also show that isotope data are sensitive to the onset of oxidation after biostimulation ends, even in the case where reduction continues to remove contaminant uranium downstream. Our study and the described conceptual model support the use of 238U/235U ratios as a tool for evaluating the efficacy of biostimulation and potentially other remedial strategies employed at Rifle and other uranium-contaminated sites.

  14. Multilevel fitting of {sup 235}U resonance data sensitive to Bohr-and Brosa-fission channels

    SciTech Connect

    Moore, M.S.

    1995-05-01

    The recent determination of the K, J dependence of the neutron induced fission cross section of {sup 235}U by the Dubna group has led to a renewed interest in the mechanism of fission from saddle to scission. The K quantum numbers designate the so-called Bohr fission channels, which describe the fission properties at the saddle point. Certain other fission properties, e.g., the fragment mass and kinetic-energy distribution, are related to the properties of the scission point. The neutron energy dependence of the fragment kinetic energies has been measured by Hambsch et al., who analyzed their data according to a channel description of Brosa et al. How these two channel descriptions, the saddle-point Bohr channels and the scission-point Brosa channels, relate to one another is an open question, and is the subject matter of the present paper. We use the correlation coefficient between various data sets, in which variations are reported from resonance to resonance, as a measure of both-the statistical reliability of the data and of the degree to which different scission variables relate to different Bohr channels. We have carried out an adjustment of the ENDF/B-VI multilevel evaluation of the fission cross section of {sup 235}U, one that provides a reasonably good fit to the energy dependence of the fission, capture, and total cross sections below 100 eV, and to the Bohr-channel structure deduced from an earlier measurement by Pattenden and Postma. We have also further explored the possibility of describing the data of Hambsch et al. in the Brosa-channel framework with the same set of fission-width vectors, only in a different reference system. While this approach shows promise, it is clear that better data are also needed for the neutron energy variation of the scission-point variables.

  15. Measurement of activity concentrations of 40K, 226Ra and 232Th for assessment of radiation hazards from soils of the southwestern region of Nigeria.

    PubMed

    Ajayi, Oladele Samuel

    2009-08-01

    Activity concentrations of the selected radionuclides (40)K, (226)Ra and (232)Th were measured in surface soil samples collected from 38 cities in the southwest region of Nigeria by means of gamma spectroscopy with a high-purity germanium detector. Measured activity concentration values of (40)K varied from 34.9 +/- 4.4 to 1,358.6 +/- 28.5 Bq kg(-1) (given on a dry mass (DM) basis) with a mean value of 286.5 +/- 308.5 Bq kg(-1); that of (226)Ra varied from 9.3 +/- 3.7 to 198.1 +/- 13.8 Bq kg(-1) with a mean value of 54.5 Bq kg(-1) and a standard deviation of 38.7 Bq kg(-1), while that of (232)Th varied from 5.4 +/- 1.1 to 502.0 +/- 16.5 Bq kg(-1) with a mean value of 91.1 Bq kg(-1) and standard deviation of 100.9 Bq kg(-1). The mean activity concentration values obtained for (226)Ra and (232)Th are greater than the world average values reported by the United Nations Scientific Committee on Effects of Atomic Radiation for areas of normal background radiation. Radiological indices were estimated for the radiation/health hazards of the natural radioactivity of all soil samples. Estimated absorbed dose rates in air varied from 12.42 +/- 2.25 to 451.33 +/- 19.06 nGy h(-1), annual outdoor effective dose rates from 0.015 +/- 0.003 to 0.554 +/- 0.023 mSv year(-1), internal hazard index from 0.10 +/- 0.03 to 3.02 +/- 0.16, external hazard index from 0.07 +/- 0.01 to 2.60 +/- 0.11, representative level index from 0.19 +/- 0.03 to 6.84 +/- 0.29, activity index from 0.09 +/- 0.02 to 3.42 +/- 0.15, and radium equivalent activity from 26.95 +/- 5.04 to 963.15 +/- 41.87 Bq kg(-1). Only the mean value of the representative level index exceeds the limit for areas of normal background radiation. All other indices show mean values that are lower than the recommended limits.

  16. Process for producing enriched uranium having a {sup 235}U content of at least 4 wt. % via combination of a gaseous diffusion process and an atomic vapor laser isotope separation process to eliminate uranium hexafluoride tails storage

    DOEpatents

    Horton, J.A.; Hayden, H.W. Jr.

    1995-05-30

    An uranium enrichment process capable of producing an enriched uranium, having a {sup 235}U content greater than about 4 wt. %, is disclosed which will consume less energy and produce metallic uranium tails having a lower {sup 235}U content than the tails normally produced in a gaseous diffusion separation process and, therefore, eliminate UF{sub 6} tails storage and sharply reduce fluorine use. The uranium enrichment process comprises feeding metallic uranium into an atomic vapor laser isotope separation process to produce an enriched metallic uranium isotopic mixture having a {sup 235} U content of at least about 2 wt. % and a metallic uranium residue containing from about 0.1 wt. % to about 0.2 wt. % {sup 235} U; fluorinating this enriched metallic uranium isotopic mixture to form UF{sub 6}; processing the resultant isotopic mixture of UF{sub 6} in a gaseous diffusion process to produce a final enriched uranium product having a {sup 235}U content of at least 4 wt. %, and up to 93.5 wt. % or higher, of the total uranium content of the product, and a low {sup 235}U content UF{sub 6} having a {sup 235}U content of about 0.71 wt. % of the total uranium content of the low {sup 235}U content UF{sub 6}; and converting this low {sup 235}U content UF{sub 6} to metallic uranium for recycle to the atomic vapor laser isotope separation process. 4 figs.

  17. Process for producing enriched uranium having a .sup.235 U content of at least 4 wt. % via combination of a gaseous diffusion process and an atomic vapor laser isotope separation process to eliminate uranium hexafluoride tails storage

    DOEpatents

    Horton, James A.; Hayden, Jr., Howard W.

    1995-01-01

    An uranium enrichment process capable of producing an enriched uranium, having a .sup.235 U content greater than about 4 wt. %, is disclosed which will consume less energy and produce metallic uranium tails having a lower .sup.235 U content than the tails normally produced in a gaseous diffusion separation process and, therefore, eliminate UF.sub.6 tails storage and sharply reduce fluorine use. The uranium enrichment process comprises feeding metallic uranium into an atomic vapor laser isotope separation process to produce an enriched metallic uranium isotopic mixture having a .sup.235 U content of at least about 2 wt. % and a metallic uranium residue containing from about 0.1 wt. % to about 0.2 wt. % .sup.235 U; fluorinating this enriched metallic uranium isotopic mixture to form UF.sub.6 ; processing the resultant isotopic mixture of UF.sub.6 in a gaseous diffusion process to produce a final enriched uranium product having a .sup.235 U content of at least 4 wt. %, and up to 93.5 wt. % or higher, of the total uranium content of the product, and a low .sup.235 U content UF.sub.6 having a .sup.235 U content of about 0.71 wt. % of the total uranium content of the low .sup.235 U content UF.sub.6 ; and converting this low .sup.235 U content UF.sub.6 to metallic uranium for recycle to the atomic vapor laser isotope separation process.

  18. Measurement of 232Th(n,5n γ) cross sections from 29 MeV to 42 MeV

    NASA Astrophysics Data System (ADS)

    Kerveno, M.; Nolte, R.; Baumann, P.; Dessagne, Ph.; Jericha, E.; Jokic, S.; Koning, A. J.; Lukic, S.; Meulders, J. P.; Nachab, A.; Pavlik, A.; Reginatto, M.; Rudolf, G.

    2014-10-01

    The excitation function of the reaction 232 Th( n, 5 nγ)228 Th from 29 to 42 MeV has been measured for the first time at the quasi-monoenergetic neutron beam of the UCL cyclotron CYCLONE employing the 7Li(p,n) source reaction. Taking advantage of the good energy resolution of the planar High-Purity Germanium (HPGe) detectors, prompt γ-ray spectroscopy was used to detect the γ-rays resulting from the decay of excited states of nuclei created by the (n, xn) reactions. The neutron beam was characterized by a combination of time of flight measurements carried out using a liquid scintillation detector and a 238U fission ionization chamber. Fluence measurements were performed using a proton recoil telescope. The results are compared with TALYS-1.4 code calculations.

  19. Towards A Modern Calibration Of The 238U/235U Paleoredox Proxy: Apparent Uranium Isotope Fractionation Factor During U(VI)-U(IV) Reduction In The Black Sea

    NASA Astrophysics Data System (ADS)

    Rolison, J. M.; Stirling, C. H.; Middag, R.; Rijkenberg, M. J. A.; De Baar, H. J. W.

    2015-12-01

    The isotopic compositions of redox-sensitive metals, including uranium (U), in marine sediments have recently emerged as powerful diagnostic tracers of the redox state of the ancient ocean-atmosphere system. Interpretation of sedimentary isotopic information requires a thorough understating of the environmental controls on isotopic fractionation in modern anoxic environments before being applied to the paleo-record. In this study, the relationship between ocean anoxia and the isotopic fractionation of U was investigated in the water column and sediments of the Black Sea. The Black Sea is the world's largest anoxic basin and significant removal of U from the water column and high U accumulation rates in modern underlying sediments have been documented. Removal of U from the water column occurs during the redox transition of soluble U(VI) to relatively insoluble U(IV). The primary results of this study are two-fold. First, significant 238U/235U fractionation was observed in the water column of the Black Sea, suggesting the reduction of U induces 238U/235U fractionation with the preferential removal of 238U from the aqueous phase. Second, the 238U/235U of underlying sediments is related to the water column through the isotope fractionation factor of the reduction reaction but is influenced by mass transport processes. These results provide important constraints on the use of 238U/235U as a proxy of the redox state of ancient oceans.

  20. Uranium 238U/235U isotope ratios as indicators of reduction: results from an in situ biostimulation experiment at Rifle, Colorado, U.S.A.

    PubMed

    Bopp, Charles John; Lundstrom, Craig C; Johnson, Thomas M; Sanford, Robert A; Long, Philip E; Williams, Kenneth H

    2010-08-01

    The attenuation of groundwater contamination via chemical reaction is traditionally evaluated by monitoring contaminant concentration through time. However, this method can be confounded by common transport processes (e.g., dilution, sorption). Isotopic techniques bypass the limits of concentration methods, and so may provide improved accuracy in determining the extent of reaction. We apply measurements of 238U/235U to a U bioremediation field experiment at the Rifle Integrated Field Research Challenge Site in Rifle, Colorado. An array of monitoring and injection wells was installed on a 100 m2 plot where U(VI) contamination was present in the groundwater. Acetate-amended groundwater was injected along an up-gradient gallery to encourage the growth of dissimilatory metal reducing bacteria (e.g., Geobacter species). During amendment, U concentration dropped by an order of magnitude in the experiment plot. We measured 238U/235U in samples from one monitoring well by MC-ICP-MS using a double isotope tracer method. A significant approximately 1.00 per thousand decrease in 238U/235U occurred in the groundwater as U(VI) concentration decreased. The relationship between 238U/235U and concentration corresponds approximately to a Rayleigh distillation curve with an effective fractionation factor (alpha) of 1.00046. We attribute the observed U isotope fractionation to a nuclear field shift effect during enzymatic reduction of U(VI)(aq) to U(IV)(s).

  1. SAS2H input for computing core activities of 4.5, 5.0, and 5.5 weight % {sup 235}U fuel for Sequoyah Nuclear Plant

    SciTech Connect

    Hermann, O.W.

    1994-08-01

    Sequoyah Nuclear Plant core activities at initial fuel enrichments of 4.5, 5.0, and 5.5 wt% {sup 235}U, required in nuclear safety evaluations, were computed by the SAS2H analysis sequence and the ORIGEN-S code within the SCALE-4.2 code system.

  2. SUPPLEMENTARY COMPARISON: Activity measurements of a suite of radionuclides (90Sr, 137Cs, 210Pb, 210Po, 228Ra, 234U, 235U, 238U, 238Pu, 239,240Pu) in soil reference material (Rocky Flats II): CCRI(II)-S2

    NASA Astrophysics Data System (ADS)

    Nour, S.; Inn, K. G. W.; Karam, L. R.

    2009-01-01

    In 2005, the CCRI decided that a comparison undertaken from 2002 to 2007 by the NIST (SIM) in the development of a new soil (Rocky Flats II) standard reference material (SRM) was sufficiently well constructed that it could be converted into a supplementary comparison under CCRI(II), with comparison identifier CCRI(II)-S2, so as to support calibration and measurement capability (CMC) claims for radionuclide measurements in reference material (specifically, low calcium-content soils). Previous comparisons of radionuclides have been of single or multiple nuclides in non-complex matrices and results of such could not be extended to support capabilities to measure the same nuclides in reference materials. The results of this comparison have been reported to the participants, and have been used to determine the certified reference value of the SRM. The key comparison working group (KCWG) of the CCRI(II) has approved this approach as a mechanism to link all the results to certified 'reference values' in lieu of the key comparison reference value (KCRV) of these specified radionuclides in this type of matrix (soil) so as to support CMCs of similar materials. Main text. To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/. The final report has been peer-reviewed and approved for publication by the CCRI Section II, according to the provisions of the CIPM Mutual Recognition Arrangement (MRA).

  3. Investigating Uranium Mobility Using Stable Isotope Partitioning of 238U/235U and a Reactive Transport Model

    NASA Astrophysics Data System (ADS)

    Bizjack, M.; Johnson, T. M.; Druhan, J. L.; Shiel, A. E.

    2015-12-01

    We report a numerical reactive transport model which explicitly incorporates the effectively stable isotopes of uranium (U) and the factors that influence their partitioning in bioactive systems. The model reproduces trends observed in U isotope ratios and concentration measurements from a field experiment, thereby improving interpretations of U isotope ratios as a tracer for U reactive transport. A major factor contributing to U storage and transport is its redox state, which is commonly influenced by the availability of organic carbon to support metal-reducing microbial communities. Both laboratory and field experiments have demonstrated that biogenic reduction of U(VI) fractionates the stable isotope ratio 238U/235U, producing an isotopically heavy solid U(IV) product. It has also been shown that other common reactive transport processes involving U do not fractionate isotopes to a consistently measurable level, which suggests the capacity to quantify the extent of bioreduction occurring in groundwater containing U using 238U/235U ratios. A recent study of a U bioremediation experiment at the Rifle IFRC site (Colorado, USA) applied Rayleigh distillation models to quantify U stable isotope fractionation observed during acetate amendment. The application of these simplified models were fit to the observations only by invoking a "memory-effect," or a constant source of low-concentration, unfractionated U(VI). In order to more accurately interpret the measured U isotope ratios, we present a multi-component reactive transport model using the CrunchTope software. This approach is capable of quantifying the cycling and partitioning of individual U isotopes through a realistic network of transport and reaction pathways including reduction, oxidation, and microbial growth. The model incorporates physical heterogeneity of the aquifer sediments through zones of decreased permeability, which replicate the observed bromide tracer, major ion chemistry, U concentration, and U

  4. Biological availability of (238)U, (234)U and (226)Ra for wild berries and meadow grasses in natural ecosystems of Belarus.

    PubMed

    Sokolik, G A; Ovsiannikova, S V; Voinikava, K V; Ivanova, T G; Papenia, M V

    2014-01-01

    This work is devoted to investigation of behavior of (234)U, (238)U and (226)Ra by determining the soil to plant transfer under different natural conditions such as forest or swamped areas and meadow lands with different soil types. The paper summarizes the data on investigation of uranium and radium uptake by wild berries and natural meadow grasses in the typical conditions of Belarus. Parameters characterizing the biological availability of (234)U, (238)U and (226)Ra for bilberry (Vaccinium myrtillus), lingonberry (Vaccinium viti-idaea), blueberry (Vaccinium iliginosum) and cranberry (Vaccinium oxycoccus palustris) as well as for widely occurring mixed meadow vegetation, which belongs to the sedge-grass or grass-sedge associations and forbs, have been established. In the sites under investigation, the deposition levels of (238+239+240)Pu were less than 0.37 kBq m(-2) and (137)Cs deposition ranged between less than 0.37 and 37 kBq m(-2). It was found that activity concentrations of radionuclides in berries varied in the ranges of 0.037-0.11 for (234)U, 0.036-0.10 for (238)U and 0.11-0.43 Bq kg(-1) for (226)Ra, but in the mixed meadow grasses they were 0.32-4.4, 0.24-3.9 and 0.14-6.9 Bq kg(-1) accordingly. The (234)U/(238)U activity ratios were 1.02 ± 0.01 for wild berries, 1.20 ± 0.09 for underground meadow grasses and 1.02 ± 0.02 for proper soils. The concentration ratios (CRs, dry weight basis) of (234)U and (238)U for mixed meadow grasses were 0.036-0.42 and 0.041-0.46 respectively. The correspondent geometric means (GM) were 0.13 and 0.15 with geometric standard deviations (GSD) of 2.4. The CRs of (226)Ra for meadow grasses were 0.031-1.0 with GM 0.20 and GSD 2.6. The CRs of (234)U, (238)U and (226)Ra for wild berries ranged within 0.0018-0.008 (GM is 0.0034, GSD is 1.8), 0.0018-0.008 (GM is 0.0035, GSD is 1.8) and 0.005-0.033 (GM is 0.016, GSD is 2.1) accordingly. The highest CR values of uranium for mixed meadow grasses were found in the

  5. Transfer Rates of 238U and 232Th for E. globulus, A. mearnsii, H. filipendula and Hazardous Effects of the Usage of Medicinal Plants From Around Gold Mine Dump Environs

    PubMed Central

    Tshivhase, Victor M.; Njinga, Raymond L.; Mathuthu, Manny; Dlamini, Thulani C.

    2015-01-01

    Medicinal plant consumption can be a source of human exposure to radioactive elements such as 238U and 232Th, which can lead to internal radiation doses. The uptake of 238U and 232Th from soils to the leaf samples of three different medicinal plant species (Eucalyptus globulus, Acacia mearnsii and Hyparrhenia filipendula) from the purlieu of the Princess gold mine dump, an abandoned contaminated tailings storage site (TSS), located at longitude 27°55′00″E and latitude 26°09′30″S in Davidsonville (Roodepoort, west of Johannesburg, South Africa) was measured. This was done using ICP-MS spectrometry and substantial differences were observed in the soil-plant transfer factor (TF) values between these radionuclides. The plant species E. globulus exhibited the highest uptake of 238U, with an average TF of 3.97, while that of H. filipendula was 0.01 and the lowest TF of 0.15 × 10−2 was measured for A. mearnsii. However, in the case of 232Th, the highest average TF was observed for A. mearnsii (0.29), followed by E. globulus (0.10) and lowest was measured for H. filipendula (0.27 × 10−2). The ratio of TF average value i.e., 238U to 232Th in the soil-plant leaves was 38.05 for E. globulus, 0.01 for A. mearnsii and 4.38 for H. filipendula. PMID:26690462

  6. Calculation of the absolute detection efficiency of a moderated /sup 235/U neutron detector on the Tokamak Fusion Test Reactor

    SciTech Connect

    Ku, L.P.; Hendel, H.W.; Liew, S.L.

    1989-02-01

    Neutron transport simulations have been carried out to calculate the absolute detection efficiency of a moderated /sup 235/U neutron detector which is used on the TFTR as a part of the primary fission detector diagnostic system for measuring fusion power yields. Transport simulations provide a means by which the effects of variations in various shielding and geometrical parameters can be explored. These effects are difficult to study in calibration experiments. The calculational model, benchmarked against measurements, can be used to complement future detector calibrations, when the high level of radioactivity resulting from machine operation may severely restrict access to the tokamak. We present a coupled forward-adjoint algorithm, employing both the deterministic and Monte Carlo sampling methods, to model the neutron transport in the complex tokamak and detector geometries. Sensitivities of the detector response to the major and minor radii, and angular anisotropy of the neutron emission are discussed. A semi-empirical model based on matching the calculational results with a small set of experiments produces good agreement (+-15%) for a wide range of source energies and geometries. 20 refs., 6 figs., 4 tabs.

  7. Determination of Nuclear Charge Distributions of Fission Fragments from ^{235}U (n_th, f) with Calorimetric Low Temperature Detectors

    NASA Astrophysics Data System (ADS)

    Grabitz, P.; Andrianov, V.; Bishop, S.; Blanc, A.; Dubey, S.; Echler, A.; Egelhof, P.; Faust, H.; Gönnenwein, F.; Gomez-Guzman, J. M.; Köster, U.; Kraft-Bermuth, S.; Mutterer, M.; Scholz, P.; Stolte, S.

    2016-08-01

    Calorimetric low temperature detectors (CLTD's) for heavy-ion detection have been combined with the LOHENGRIN recoil separator at the ILL Grenoble for the determination of nuclear charge distributions of fission fragments produced by thermal neutron-induced fission of ^{235}U. The LOHENGRIN spectrometer separates fission fragments according to their mass-to-ionic-charge ratio and their kinetic energy, but has no selectivity with respect to nuclear charges Z. For the separation of the nuclear charges, one can exploit the nuclear charge-dependent energy loss of the fragments passing through an energy degrader foil (absorber method). This separation requires detector systems with high energy resolution and negligible pulse height defect, as well as degrader foils which are optimized with respect to thickness, homogeneity, and energy loss straggling. In the present, contribution results of test measurements at the Maier Leibnitz tandem accelerator facility in Munich with ^{109}Ag and ^{127}I beams with the aim to determine the most suitable degrader material, as well as measurements at the Institut Laue-Langevin will be presented. These include a systematic study of the quality of Z-separation of fission fragments in the mass range 82le A le 132 and a systematic measurement of ^{92}Rb fission yields, as well as investigations of fission yields toward the symmetry region.

  8. (n,γ) by the Internal Surrogate Ratio Method: A Benchmark using ^235U(d,p)

    NASA Astrophysics Data System (ADS)

    Allmond, J. M.

    2008-10-01

    The Surrogate Reaction Technique, first proposed in 1970 [1], has recently been under investigation by a Richmond / LLNL / LBNL / Yale collaboration. These studies are currently performed at LBNL using the STARS and LiBerACE detector arrays. Both absolute [1] and ratio [2] methods have been employed to circumvent technical challenges presented by the fabrication of unstable targets and by the production of high-flux neutron beams. The ^235U(d,p) surrogate reaction at 21 MeV benchmarks the (n,γ) cross section by use of the internal ratio method (same compound nucleus but different exit channel). The present study marks the first benchmark of the internal ratio method. Previous tests of the Surrogate Ratio Method have focused on determining (n,f) cross sections using the external ratio method (different compound nucleus but same exit channel). Results of this study are presented.This work was performed under the auspices of the U.S. Department of Energy under contract numbers DE-FG52-06NA26206 (UR), DE-AC52-07NA27344 (LLNL), and DE-AC02-05CH11231 (LBNL).[1]J.D. Cramer and H.C. Britt, Nucl. Sci. Eng. 41, 177 (1970). [2]C. Plettner, et al., Phys. Rev. C 71 051602 (2005).

  9. Yields of short-lived fission products produced following {sup 235}U(n{sub th},f)

    SciTech Connect

    Tipnis, S.V.; Campbell, J.M.; Couchell, G.P.; Li, S.; Nguyen, H.V.; Pullen, D.J.; Schier, W.A.; Seabury, E.H.; England, T.R.

    1998-08-01

    Measurements of gamma-ray spectra, following the thermal neutron fission of {sup 235}U have been made using a high purity germanium detector at the University of Massachusetts Lowell (UML) Van de Graaff facility. The gamma spectra were measured at delay times ranging from 0.2 s to nearly 10thinsp000 s following the rapid transfer of the fission fragments with a helium-jet system. On the basis of the known gamma transitions, forty isotopes have been identified and studied. By measuring the relative intensities of these transitions, the relative yields of the various precursor nuclides have been calculated. The results are compared with the recommended values listed in the ENDF/B-VI fission product data base (for the lifetimes and the relative yields) and those published in the Nuclear Data Sheets (for the beta branching ratios). This information is particularly useful for the cases of short-lived fission products with lifetimes of the order of fractions of a second or a few seconds. Independent yields of many of these isotopes have rather large uncertainties, some of which have been reduced by the present study. {copyright} {ital 1998} {ital The American Physical Society}

  10. Detection of 235U in hydrogenous cargo with Differential Die-Away Analysis and optimized neutron detectors

    NASA Astrophysics Data System (ADS)

    Jordan, Kelly A.; Gozani, Tsahi

    2007-08-01

    Differential Die-Away Analysis (DDAA) is a sensitive technique for detecting the presence of fissile materials such as 235U and 239Pu. In DDAA, a neutron generator produces repetitive pulses of neutrons that are directed into a cargo being inspected. As each pulse passes through the cargo, the neutrons are thermalized and absorbed. The thermalization process is very rapid and the population of the source and epithermal neutrons decays away within microseconds. The population of thermal neutrons, however, decays much slower with the diffusion decay time of the inspected medium (thermal neutron "die away" time), on the order of hundreds of microseconds. If Special Nuclear Material (SNM) is present, the thermalized neutrons from the source will cause fissions that produce a new source of neutrons. These fast fission neutrons decay with a time very similar to that of the thermal neutron die-away of the surrounding cargo. The sensitivity of DDAA for a given source of neutrons critically depends on optimizing the fast/epithermal neutron detection system. Optimization involves both time response and detection efficiency. Optimized detectors were able to detect fissile material throughout pallets of cargo.

  11. Photo-fission Product Yield Measurements at Eγ=13 MeV on 235U, 238U, and 239Pu

    NASA Astrophysics Data System (ADS)

    Tornow, W.; Bhike, M.; Finch, S. W.; Krishichayan, Fnu; Tonchev, A. P.

    2016-09-01

    We have measured Fission Product Yields (FPYs) in photo-fission of 235U, 238U, and 239Pu at TUNL's High-Intensity Gamma-ray Source (HI γS) using mono-energetic photons of Eγ = 13 MeV. Details of the experimental setup and analysis procedures will be discussed. Yields for approximately 20 fission products were determined. They are compared to neutron-induced FPYs of the same actinides at the equivalent excitation energies of the compound nuclear systems. In the future photo-fission data will be taken at Eγ = 8 . 0 and 10.5 MeV to find out whether photo-fission exhibits the same so far unexplained dependence of certain FPYs on the energy of the incident probe, as recently observed in neutron-induced fission, for example, for the important fission product 147Nd. Work supported by the U. S. Dept. of Energy, under Grant No. DE-FG02-97ER41033, and by the NNSA, Stewardship Science Academic Alliances Program, Grant No. DE-NA0001838 and the Lawrence Livermore, National Security, LLC under Contract No. DE-AC52-07NA27344.

  12. Study on the radioactivity and soil-to-plant transfer factor of (226)Ra, (234)U and (238)U radionuclides in irrigated farms from the northwestern Saudi Arabia.

    PubMed

    Al-Hamarneh, Ibrahim F; Alkhomashi, N; Almasoud, Fahad I

    2016-08-01

    The present study addresses the soil-to-plant transfer factors (TFs) of (226)Ra, (234)U and (238)U for 13 types of vegetables and agricultural crops planted under semi-arid environment in the northwestern part of Saudi Arabia. Crop plants along with plant-growing soils were collected from selected farms, which are irrigated from the non-renewable Saq aquifer, and investigated for their radioactivity content by means of alpha spectrometry after applying a radiochemical separation procedure. Hence, TF data for plant roots, green parts (stem and leaves) and fruits were calculated and contrasted to those reported in the literature. Substantial differences were observed in the TFs of Ra and U radioisotopes among plant species. In crop fruits, eggplant exhibited the highest uptake of (226)Ra (TF value of 0.11), while beans (0.16) have the highest TF for (234)U and (238)U. The geometric mean TF values indicated that the crop roots tend to accumulate Ra and U about four to six-folds higher than fruits. The relation between TF values and soil concentrations showed a weak correlation. Activity ratios between radionuclides in crop plants indicated the preferential translocation of U in fruits than Ra even though Ra is more available for root uptake. The fruit/root (F/R) ratios obtained for the investigated plants shown that pepper had the smallest F/R ratios (0.07 ± 0.01, 0.12 ± 0.02 and 0.11 ± 0.02 for (226)Ra, (234)U and (238)U, respectively), while the highest F/R ratios were observed in potatoes (0.71 ± 0.15, 0.44 ± 0.10 and 0.40 ± 0.08 for (226)Ra, (234)U and (238)U, respectively). The TF and F/R ratios data of natural radionuclides in the study region can hopefully improve the scientific knowledge for future studies.

  13. A study on possible use of Urtica dioica (common nettle) plants as uranium ((234)U, (238)U) contamination bioindicator near phosphogypsum stockpile.

    PubMed

    Olszewski, Grzegorz; Boryło, Alicja; Skwarzec, Bogdan

    The aim of this study was to determine uranium concentrations in common nettle (Urtica dioica) plants and corresponding soils samples which were collected from the area of phosphogypsum stockpile in Wiślinka (northern Poland). The uranium concentrations in roots depended on its concentrations in soils. Calculated BCF and TF values showed that soils characteristics and air deposition affect uranium absorption and that different uranium species have different affinities to U. dioica plants. The values of (234)U/(238)U activity ratio indicate natural origin of these radioisotopes in analyzed plants. Uranium concentration in plants roots is negatively weakly correlated with distance from phosphogypsum stockpile.

  14. Determination of specific activity of (226)Ra, (232)Th and (40)K for assessment of radiation hazards from Turkish pumice samples.

    PubMed

    Turhan, Seref; Gündüz, Lüfullah

    2008-02-01

    The specific activity of (226)Ra, (232)Th and (40)K in 52 Turkish pumice samples collected from 11 geographical areas located in Central Anatolia, Eastern Anatolia, Mediterranean and Aegean regions was determined by gamma-ray spectrometry with a high-purity germanium (HPGe) detector. The specific activity of (226)Ra, (232)Th and (40)K ranged from 12.7+/-0.5 to 256.2+/-9.1Bqkg(-1) with a mean of 89.1+/-65.2Bqkg(-1), 12.3+/-1.0 to 237.9+/-12.2Bqkg(-1) with a mean of 87.0+/-61.4Bqkg(-1) and 300.1+/-5.5 to 1899.0+/-30.8Bqkg(-1) with a mean of 1211.9+/-419.8Bqkg(-1), respectively. Elemental concentrations were determined for U (from 1.0 to 20.7ppm with a mean of 7.2+/-5.3ppm), Th (from 3.0 to 58.6ppm with a mean of 21.4+/-15.1ppm) and K (from 1.0 to 6.1% with a mean of 3.9+/-1.3%). The radium equivalent activity (Ra(eq)), the activity index, the emanation coefficient, the (222)Rn mass exhalation rate, the indoor absorbed dose rate and the effective dose rate were estimated for the radiation hazard of the natural radioactivity in all samples. The calculated mean Ra(eq) value was 306.6+/-177.7Bqkg(-1) (54.6+/-5.5 to 737.6+/-49.0Bqkg(-1)) for all pumice samples. This value is lower than the recommended limit value of 370Bqkg(-1) for building raws and products. The emanation coefficient and the (222)Rn mass exhalation rate of all samples ranged from 29.4 to 42.9% with a mean of 36.2% and from 11.0 to 196.4microBqkg(-1)s(-1) with a mean of 73.5microBqkg(-1)s(-1), respectively. The mean indoor absorbed dose rate and the corresponding mean effective dose rate were 274.6+/-153.6nGyh(-1) (50.4-644.6nGyh(-1)) and 1.35+/-0.75mSvy(-1) (0.24-3.16mSvy(-1)), respectively. For all pumice samples the mean indoor absorbed dose rate is about three times higher than the population-weighted average of 84nGyh(-1), while the mean effective dose rate values except for PUM 05, PUM 06, PUM 10 and PUM 15 exceed the dose criterion of 1mSvy(-1).

  15. Delayed Fission Gamma-ray Characteristics of Th-232 U-233 U-235 U-238 and Pu-239

    SciTech Connect

    Lane, Taylor; Parma, Edward J.

    2015-08-01

    Delayed fission gamma-rays play an important role in determining the time dependent ioniz- ing dose for experiments in the central irradiation cavity of the Annular Core Research Reactor (ACRR). Delayed gamma-rays are produced from both fission product decay and from acti- vation of materials in the core, such as cladding and support structures. Knowing both the delayed gamma-ray emission rate and the time-dependent gamma-ray energy spectrum is nec- essary in order to properly determine the dose contributions from delayed fission gamma-rays. This information is especially important when attempting to deconvolute the time-dependent neutron, prompt gamma-ray, and delayed gamma-ray contribution to the response of a diamond photo-conducting diode (PCD) or fission chamber in time frames of milliseconds to seconds following a reactor pulse. This work focused on investigating delayed gamma-ray character- istics produced from fission products from thermal, fast, and high energy fission of Th-232, U-233, U-235, U-238, and Pu-239. This work uses a modified version of CINDER2008, a transmutation code developed at Los Alamos National Laboratory, to model time and energy dependent photon characteristics due to fission. This modified code adds the capability to track photon-induced transmutations, photo-fission, and the subsequent radiation caused by fission products due to photo-fission. The data is compared against previous work done with SNL- modified CINDER2008 [ 1 ] and experimental data [ 2 , 3 ] and other published literature, includ- ing ENDF/B-VII.1 [ 4 ]. The ability to produce a high-fidelity (7,428 group) energy-dependent photon fluence at various times post-fission can improve the delayed photon characterization for radiation effects tests at research reactors, as well as other applications.

  16. R-MATRIX ANALYSIS of 232Th NEUTRON TRANSMISSIONS and CAPTURE CROSS SECTIONS in the ENERGY RANGE THERMAL to 4 keV

    SciTech Connect

    Derrien, Herve; Leal, Luiz C; Larson, Nancy M

    2008-01-01

    Neutron resonance parameters of 232Th were obtained from the Reich-Moore SAMMY analysis of high-resolution neutron transmission measurements performed at the Oak Ridge Electron Linear Accelerator (ORELA) by Olsen in 1981, along with the high-resolution neutron capture measurements performed in 2005 at the Geel Linear Accelerator (GELINA, Belgium) by Schillebeeckx and at the n-TOF facility (CERN, Switzerland) by Aerts. The ORELA data were analyzed previously by Olsen with the Breit-Wigner multilevel code SIOB, and the results were used in the ENDF/B-VI evaluation. In the new analysis of the Olsen neutron transmissions by the modern computer code SAMMY, better accuracy is obtained for the resonance parameters by including in the experimental data base the recent experimental neutron capture data. The experimental data base and the method of analysis are described in the report. The neutron transmissions and the capture cross sections calculated with the resonance parameters are compared to the experimental values. A description is given of the statistical properties of the resonance parameters. The new evaluation results in a decrease in the capture resonance integral and improves the prediction of integral thermal benchmarks.

  17. Activity concentrations of 226Ra, 232Th, 40K and 137Cs radionuclides in Turkish medicinal herbs, their ingestion doses and cancer risks

    NASA Astrophysics Data System (ADS)

    Parmaksız, Aydın; Ağuş, Yusuf

    2014-11-01

    Twenty-two medicinal herb samples, each representing a distinct species, were collected from Turkish markets and measured by the gamma spectrometric method. The activity concentration of 226Ra in medicinal herbs was found in the range of minimum detectable activity (MDA) and 15.1 ± 2.2 Bqkg-1. The activity concentration of 232Th ranged from MDA values to 3.5 ± 0.8 Bqkg-1. The activity concentration of 40K varied between 50.0 ± 16.8 and 1311.5 ± 57.3 Bqkg-1. All 137Cs activity concentrations of medicinal herbs were found to have lower than MDA values. The bone surface dose, lower large intestine and colon doses were found to be 182.9, 18.8 and 18.7 µSvy-1, respectively. The highest committed effective dose originated from the annual ingestion of 1 kg medicinal herb was calculated notably low as 9.0 µSv. The cancer risk of ingestion of medicinal herbs was found to be small enough to be neglected. The selected Turkish medicinal herbs are considered safe for human consumption.

  18. Large scale accelerator production of (225)Ac: Effective cross sections for 78-192MeV protons incident on (232)Th targets.

    PubMed

    Griswold, J R; Medvedev, D G; Engle, J W; Copping, R; Fitzsimmons, J M; Radchenko, V; Cooley, J C; Fassbender, M E; Denton, D L; Murphy, K E; Owens, A C; Birnbaum, E R; John, K D; Nortier, F M; Stracener, D W; Heilbronn, L H; Mausner, L F; Mirzadeh, S

    2016-12-01

    Actinium-225 and (213)Bi have been used successfully in targeted alpha therapy (TAT) in preclinical and clinical research. This paper is a continuation of research activities aiming to expand the availability of (225)Ac. The high-energy proton spallation reaction on natural thorium metal targets has been utilized to produce millicurie quantities of (225)Ac. The results of sixteen irradiation experiments of thorium metal at beam energies between 78 and 192MeV are summarized in this work. Irradiations have been conducted at Brookhaven National Laboratory (BNL) and Los Alamos National Laboratory (LANL), while target dissolution and processing was carried out at Oak Ridge National Laboratory (ORNL). Excitation functions for actinium and thorium isotopes, as well as for some of the fission products, are presented. The cross sections for production of (225)Ac range from 3.6 to 16.7mb in the incident proton energy range of 78-192MeV. Based on these data, production of curie quantities of (225)Ac is possible by irradiating a 5.0gcm(-2 232)Th target for 10 days in either BNL or LANL proton irradiation facilities.

  19. Vertical and horizontal distribution of radionuclides (232Th, 238U and 40K) in sediment from Manjung coastal water area Perak, Malaysia

    NASA Astrophysics Data System (ADS)

    Abdullah, Anisa; Hamzah, Zaini; Saat, Ahmad; Wood, Ab. Khalik

    2016-01-01

    Distribution of radionuclides from anthropogenic activities has been widely studied in marine coastal area. Due to rapid population growth and socio-economic development in Manjung area such as coal fired power plant, iron foundries, port development, waste discharged from factories and agriculture runoff may contribute to increase in pollution rate. The radioactive materials from anthropogenic activities could deteriorate the quality of the marine ecosystem and thus lead to possible radiological health risk to the population. Radionuclides (232Th, 238U and 40K) content in surface and profile sediment from Manjung coastal area was determined in this study. Radionuclides in sediment from seven locations were collected using sediment core sampling and measurements were carried out using Energy Dispersive X-ray Fluorescence (EDXRF) spectroscopy. The results show that the concentration of radionuclides in surface sediment and distribution trend of depth vertical profile sediment generally varies depending on locations. Enrichment factors (EF), geo-accumulation index (Igeo) and pollution index (PI) were applied to determine level of pollution of this study area. The radiological risks related to human exposure were evaluated based on external hazard index (Hex).

  20. Vertical and horizontal distribution of radionuclides ({sup 232}Th, {sup 238}U and {sup 40}K) in sediment from Manjung coastal water area Perak, Malaysia

    SciTech Connect

    Abdullah, Anisa Hamzah, Zaini; Wood, Ab. Khalik; Saat, Ahmad

    2016-01-22

    Distribution of radionuclides from anthropogenic activities has been widely studied in marine coastal area. Due to rapid population growth and socio-economic development in Manjung area such as coal fired power plant, iron foundries, port development, waste discharged from factories and agriculture runoff may contribute to increase in pollution rate. The radioactive materials from anthropogenic activities could deteriorate the quality of the marine ecosystem and thus lead to possible radiological health risk to the population. Radionuclides ({sup 232}Th, {sup 238}U and {sup 40}K) content in surface and profile sediment from Manjung coastal area was determined in this study. Radionuclides in sediment from seven locations were collected using sediment core sampling and measurements were carried out using Energy Dispersive X-ray Fluorescence (EDXRF) spectroscopy. The results show that the concentration of radionuclides in surface sediment and distribution trend of depth vertical profile sediment generally varies depending on locations. Enrichment factors (EF), geo-accumulation index (I{sub geo}) and pollution index (PI) were applied to determine level of pollution of this study area. The radiological risks related to human exposure were evaluated based on external hazard index (H{sub ex})

  1. Fragment Angular Distributions in Neutron-Induced Fission of {sup 235}U and {sup 239}Pu using a Time Projection Chamber

    SciTech Connect

    Kleinrath, Verena

    2015-07-01

    Fission fragment angular distributions can lend insights into fission barrier shapes and level densities at the scission point, both important for fission theory development. Fragment emission anisotropies are also valuable for precision cross section ratio measurements, if the distributions are different for the two isotopes used in the ratio. Available angular data is sparse for {sup 235}U and even more so for {sup 239}Pu, especially at neutron energies above 5 MeV. The Neutron Induced Fission Fragment Tracking Experiment (NIFFTE) time projection chamber, which enables precise tracking of charged particles, can be used to study angular distributions and emission anisotropies of fission fragments in neutron-induced fission. In-beam data collected at the Los Alamos Neutron Science Center with a {sup 235}U/{sup 239}Pu target during the 2014 run-cycle will provide angular distributions as a function of incident neutron energy for these isotopes. (LA-UR-1426972). (authors)

  2. Uranium concentrations and /sup 234/U//sup 238/U activity ratios in fault-associated groundwater as possible earthquake precursors

    SciTech Connect

    Finkel, R.C.

    1981-05-01

    In order to assess the utility of uranium isotopes as fluid phase earthquake precursors, uranium concentrations and /sup 234/U//sup 238/U activity ratios have been monitored on a monthly or bimonthly basis in water from 24 wells and springs associated with Southern California fault zones. Uranium concentrations vary from 0.002 ppb at Indian Canyon Springs on the San Jacinto fault to 8.3 ppb at Lake Hughes well on the San Andreas fault in the Palmdale area. /sup 234/U//sup 238/U activity ratios vary from 0.88 at Agua Caliente Springs on the Elsinore fault to 5.4 at Niland Slab well on the San Andreas fault in the Imperial Valley. There was one large earthquake in the study area during 1979, the 15 October 1979 M = 6.6 Imperial Valley earthquake. Correlated with this event, uranium concentrations varied by a factor of more than 60 and activity ratios by a factor of 3 at the Niland Slab site, about 70 km from the epicenter. At the other sites monitored, uranium concentrations varied in time, but with no apparent pattern, while uranium activity ratios remained essentially constant throughout the monitoring period.

  3. Uranium 238U/235U isotope ratios as indicators of reduction: Results from an in situ biostimulation experiment at Rifle, Colorado, USA

    SciTech Connect

    Bopp IV, C.J.; Lundstrom, C.C.; Johnson, T.M.; Sanford, R.A.; Long, P.E.; Williams, K.H.

    2010-02-01

    The attenuation of groundwater contamination via chemical reaction is traditionally evaluated by monitoring contaminant concentration through time. However, this method can be confounded by common transport processes (e.g. dilution, sorption). Isotopic techniques bypass the limits of concentration methods, and so may provide improved accuracy in determining the extent of reaction. We apply measurements of {sup 238}U/{sup 235}U to a U bioremediation field experiment at the Rifle Integrated Field Research Challenge Site in Rifle, Colorado (USA). An array of monitoring and injection wells was installed on a 100 m{sup 2} plot where U(VI) contamination was present in the groundwater. Acetate-amended groundwater was injected along an up-gradient gallery to encourage the growth of dissimilatory metal reducing bacteria (e.g. Geobacter species). During amendment, U concentration dropped by an order of magnitude in the experiment plot. We measured {sup 238}U/{sup 235}U in samples from one monitoring well by MC-ICP-MS using a double isotope tracer method. A significant {approx}1.00{per_thousand} decrease in {sup 238}U/{sup 235}U occurred in the groundwater as U(VI) concentration decreased. The relationship between {sup 238}U/{sup 235}U and concentration corresponds approximately to a Rayleigh distillation curve with an effective fractionation factor ({alpha}) of 1.00046. We attribute the observed U isotope fractionation to a nuclear field shift effect during enzymatic reduction of U(VI){sub (aq)} to U(IV){sub (s)}.

  4. Feasibility study of 235U and 239Pu characterization in radioactive waste drums using neutron-induced fission delayed gamma rays

    NASA Astrophysics Data System (ADS)

    Nicol, T.; Pérot, B.; Carasco, C.; Brackx, E.; Mariani, A.; Passard, C.; Mauerhofer, E.; Collot, J.

    2016-10-01

    This paper reports a feasibility study of 235U and 239Pu characterization in 225 L bituminized waste drums or 200 L concrete waste drums, by detecting delayed fission gamma rays between the pulses of a deuterium-tritium neutron generator. The delayed gamma yields were first measured with bare samples of 235U and 239Pu in REGAIN, a facility dedicated to the assay of 118 L waste drums by Prompt Gamma Neutron Activation Analysis (PGNAA) at CEA Cadarache, France. Detectability in the waste drums is then assessed using the MCNPX model of MEDINA (Multi Element Detection based on Instrumental Neutron Activation), another PGNAA cell dedicated to 200 L drums at FZJ, Germany. For the bituminized waste drum, performances are severely hampered by the high gamma background due to 137Cs, which requires the use of collimator and shield to avoid electronics saturation, these elements being very penalizing for the detection of the weak delayed gamma signal. However, for lower activity concrete drums, detection limits range from 10 to 290 g of 235U or 239Pu, depending on the delayed gamma rays of interest. These detection limits have been determined by using MCNPX to calculate the delayed gamma useful signal, and by measuring the experimental gamma background in MEDINA with a 200 L concrete drum mock-up. The performances could be significantly improved by using a higher interrogating neutron emission and an optimized experimental setup, which would allow characterizing nuclear materials in a wide range of low and medium activity waste packages.

  5. Measurement of {sup 235}U content and flow of UF{sub 6} using delayed neutrons or gamma rays following induced fission

    SciTech Connect

    Stromswold, D.C.; Peurrung, A.J.; Reeder, P.L.; Perkins, R.W.

    1996-06-01

    Feasibility experiments conducted at Pacific Northwest National Laboratory demonstrate that either delayed neutrons or energetic gamma rays from short-lived fission products can be used to monitor the blending of UF{sub 6} gas streams. A {sup 252}Cf neutron source was used to induce {sup 235}U fission in a sample, and delayed neutrons and gamma rays were measured after the sample moved {open_quotes}down-stream.{close_quotes} The experiments used a UO{sub 2} powder that was transported down the pipe to simulate the flowing UF{sub 6} gas. Computer modeling and analytic calculation extended the test results to a flowing UF{sub 6} gas system. Neutron or gamma-ray measurements made at two downstream positions can be used to indicate both the {sup 235}U content and UF{sub 6} flow rate. Both the neutron and gamma-ray techniques have the benefits of simplicity and long-term reliability, combined with adequate sensitivity for low-intrusion monitoring of the blending process. Alternatively, measuring the neutron emission rate from (a, n) reactions in the UF{sub 6} provides an approximate measure of the {sup 235}U content without using a neutron source to induce fission.

  6. 234U/238U Disequilibrium along stylolitic discontinuities in deep Mesozoic limestone formations of the Eastern Paris basin: evidence for discrete uranium mobility over the last 1-2 million years

    NASA Astrophysics Data System (ADS)

    Deschamps, P.; Hillaire-Marcel, C. E.; Michelot, J.-L.; Doucelance, R.; Ghaleb, B.; Buschaert, S.

    The (234U/238) equilibrium state of borehole core samples from the deep, low-permeability limestone formations surrounding the target argilite layer of the Meuse/Haute-Marne experimental site of the French agency for nuclear waste management -ANDRA- (Agence nationale pour la gestion des déchets radioactifs) was examined to improve understanding of naturally occurring radionuclide behaviour in such geological settings. Highly precise, accurate MC-ICP-MS measurements of the (234U/238U) activity ratio show that limestone samples characterised by pressure dissolution structures (stylolites or dissolution seams) display systematic (234U/238U) disequilibria, while the pristine carbonate samples remain in the secular equilibrium state. The systematic feature is observed throughout the zones marked by pressure dissolution structures: (i) the material within the seams shows a deficit of 234U over 238U ((234U/238U) down to 0.80) and (ii) the surrounding carbonate matrix is characterised by an activity ratio greater than unity (up to 1.05). These results highlight a centimetric-scale uranium remobilisation in the limestone formations along these sub-horizontal seams. Although their nature and modalities are not fully understood, the driving processes responsible for these disequilibria were active during the last 1-2 Ma.

  7. Fission Product Data Measured at Los Alamos for Fission Spectrum and Thermal Neutrons on 239Pu, 235U, 238U

    NASA Astrophysics Data System (ADS)

    Selby, H. D.; Mac Innes, M. R.; Barr, D. W.; Keksis, A. L.; Meade, R. A.; Burns, C. J.; Chadwick, M. B.; Wallstrom, T. C.

    2010-12-01

    where the present results are about 4%-relative higher for neutrons incident on 239Pu and 235U. Additionally, our results illustrate the importance of representing the incident energy dependence of fission product yields over the fast neutron energy range for high-accuracy work, for example the 147Nd from neutron reactions on plutonium. An upgrade to the ENDF library, for ENDF/B-VII.1, based on these and other data, is described in a companion paper to this work.

  8. Measurement of 238U and 232Th in Petrol, Gas-oil and Lubricant Samples by Using Nuclear Track Detectors and Resulting Radiation Doses to the Skin of Mechanic Workers.

    PubMed

    Misdaq, M A; Chaouqi, A; Ouguidi, J; Touti, R; Mortassim, A

    2015-10-01

    Workers in repair shops of vehicles (cars, buses, truck, etc.) clean carburetors, check fuel distribution, and perform oil changes and greasing. To explore the exposure pathway of (238)U and (232)Th and its decay products to the skin of mechanic workers, these radionuclides were measured inside petrol, gas-oil, and lubricant material samples by means of CR-39 and LR-115 type II solid state nuclear track detectors (SSNTDs), and corresponding annual committed equivalent doses to skin were determined. The maximum total equivalent effective dose to skin due to the (238)U and (232)Th series from the application of different petrol, gas-oil, and lubricant samples by mechanic workers was found equal to 1.2 mSv y(-1) cm(-2).

  9. Study of secondary neutron interactions with 232Th, 129I, and 127I nuclei with the uranium assembly “QUINTA” at 2, 4, and 8GeV deuteron beams of the JINR Nuclotron accelerator

    DOE PAGES

    Adam, J.; Chilap, V. V.; Furman, V. I.; ...

    2015-11-04

    The natural uranium assembly, “QUINTA”, was irradiated with 2, 4, and 8 GeV deuterons. The 232Th, 127I, and 129I samples have been exposed to secondary neutrons produced in the assembly at a 20-cm radial distance from the deuteron beam axis. The spectra of gamma rays emitted by the activated 232Th, 127I, and 129I samples have been analyzed and several tens of product nuclei have been identified. For each of those products, neutron-induced reaction rates have been determined. The transmutation power for the 129I samples is estimated. Furthermore, experimental results were compared to those calculated with well-known stochastic and deterministic codes.

  10. Allanite from the El Muerto Pegmatite, Oaxaca, Mexico: A Potential New Standard for 232Th-208Pb Dating by LA-ICP-MS

    NASA Astrophysics Data System (ADS)

    Price, J.; Crowley, J. L.; Solari, L.; Prol-Ledesma, R.

    2012-12-01

    Allanite dating may be important to studies addressing tectonomagmatic evolution, provenance of monocyclic sediment, and mineral weathering. Obtaining accurate allanite ages by SIMS has been challenging and time-consuming due to the mineral's extreme chemical variability which often prevents finding adequately matrix-matched standards. Isotopic measurements by LA-ICP-MS minimize the need for standards of nearly identical composition to the unknown allanite being analyzed, and it is done relatively rapidly. Dating by LA-ICP-MS requires high quality standards for isotopic fractionation corrections. However, readily accessible and well characterized allanite standards are scarce. We investigated gemstone allanite from the El Muerto pegmatite, Oaxaca, Mexico, as a potential new geochronology standard for 232Th-208Pb allanite dating by LA-ICP-MS. Compositional homogeneity was thoroughly investigated by scanning and backscatter electron microscopy, cathodoluminescence, quantitative and qualitative energy dispersive x-ray spectroscopy, electron microprobe, and LA-ICP-MS. The possibility of metamictization was investigated by extensive X-ray diffraction analyses. The El Muerto allanite was U-Pb dated by ID-TIMS, with common Pb ratios determined from cogenetic K-feldspar by ID-TIMS and LA-MC-ICP-MS. Future work includes Th-Pb dating by ID-TIMS. The samples investigated are homogeneous with respect to major and trace elements. Major element compositional results are generally in agreement with published values, and no metamictization was identified despite the allanite being nearly 1 Ga. The only limitation of the El Muerto allanite is that it contains small, generally <100 μm, scarce inclusions of quartz, calciothorite, albite, calcite, and biotite. However, these grains are easily recognized and avoided during LA-ICP-MS analyses. Based on these results, the El Muerto allanite has the potential to serve as a standard for LA-ICP-MS dating.

  11. A precise 232Th-208Pb chronology of fine-grained monazite: Age of the Bayan Obo REE-Fe-Nb ore deposit, China

    USGS Publications Warehouse

    Wang, Jingyuan; Tatsumoto, M.; Li, X.; Premo, W.R.; Chao, E.C.T.

    1994-01-01

    We have obtained precise Th-Pb internal isochron ages on monazite and bastnaesite for the world's largest known rare earth elements (REE)-Fe-Nb ore deposit, the Bayan Obo of Inner Mongolia, China. The monazite samples, collected from the carbonate-hosted ore zone, contain extremely small amounts of uranium (less than 10 ppm) but up to 0.7% ThO2. Previous estimates of the age of mineralization ranged from 1.8 to 0.255 Ga. Magnetic fractions of monazite and bastnaesite samples (<60-??m size) showed large ranges in 232Th 204Pb values (900-400,000) and provided precise Th-Pb internal isochron ages for paragenetic monazite mineralization ranging from 555 to 398 Ma within a few percent error (0.8% for two samples). These results are the first indication that REE mineralization within the giant Bayan Obo ore deposit occurred over a long period of time. The initial lead isotopic compositions (low 206Pb 204Pb and high 208Pb 204Pb) and large negative ??{lunate}Nd values for Bayan Obo ore minerals indicate that the main source(s) for the ores was the lower crust which was depleted in uranium, but enriched in thorium and light rare earth elements for a long period of time. Zircon from a quartz monzonite, located 50 km south of the ore complex and thought to be related to Caledonian subduction, gave an age of 451 Ma, within the range of monazite ages. Textural relations together with the mineral ages favor an epigenetic rather than a syngenetic origin for the orebodies. REE mineralization started around 555 Ma (disseminated monazite in the West, the Main, and south of the East Orebody), but the main mineralization (banded ores) was related to the Caledonian subduction event ca. 474-400 Ma. ?? 1994.

  12. Monte Carlo Hauser-Feshbach predictions of prompt fission γ rays: Application to nth+235U, nth+239Pu, and 252Cf (sf)

    NASA Astrophysics Data System (ADS)

    Becker, B.; Talou, P.; Kawano, T.; Danon, Y.; Stetcu, I.

    2013-01-01

    The prompt neutron and γ emission from primary fission fragments are calculated for thermal neutron induced fission of 235U and 239Pu and for spontaneous fission of 252Cf using a Monte Carlo Hauser-Feshbach approach for the evaporation of the excited fission fragments. Remaining free model parameters, such as excitation energy sharing and initial spin distribution, are determined by comparison of the neutron emission characteristics with experimental data. Using the obtained parameters the γ-ray characteristics, e.g., γ spectrum, multiplicity distribution, average multiplicity and energy, and multiplicity distribution, are calculated and compared with available experimental data.

  13. Investigation of the angular dependence of the escape of /sup 233/U and /sup 235/U fission fragments as a result of capture of a polarized thermal neutron

    SciTech Connect

    Vesna, V.A.; Knyaz'kov, V.A.; Kolomenskii, E.A.; Lobashev, V.M.; Pirozhkov, A.N.; Popeko, L.A.; Smotritskii, L.M.; Solov'ev, S.M.; Titov, N.A.

    1980-06-05

    The P-parity nonconserving asymmetry of the fission of /sup 233/U and /sup 235/U was measured by using the integral method. The escape asymmetry coefficients of a light fragment are equal to (3.60 +- /sup -/0.34) x 10/sup -4/ and (0.75 +- 0.12) x 10/sup -4/, respectively. The violation of spatial parity is accompanied by a P-parity-conserving, left-right asymmetry with the coefficients (-3.24 +- 0.33) x 10/sup -4/ and (1.65 +- 0.11) x 10/sup -4/, respectively.

  14. Monte Carlo cross-section testing for fast [sup 235]U/[sup 238]U criticals: ENDF/B-V versus ENDF/B-VI

    SciTech Connect

    Weinman, J.P. )

    1993-01-01

    The purpose of this study is to compare the results of using either the reference cross-section data set ENDF/B-V or ENDF/B-VI RACER vectorized Monte Carlo calculations on several fast critical experiments. Seven benchmark cores were chosen that span a range of [sup 235]U enrichments and neutron leakage fractions. These include Godiva, Flat-Top-25, Zero-Power Reactor (ZPR)-Ill 6F, Vera-1 B, ZPR-III 12, ZPR- III 12, and Zebra-2.

  15. Reaction rate calibration techniques at ZPPR for /sup 239/Pu fission, /sup 235/U fission, /sup 238/U fission, and /sup 238/U capture

    SciTech Connect

    Brumbach, S.B.; Maddison, D.W.

    1982-06-10

    Reaction-rate calibration techniques used at ZPPR are described for /sup 239/Pu fission, /sup 235/U fission, /sup 238/U fission and /sup 238/U capture. In addition to these absolute reaction rates, calibration techniques are described for fission-rate ratios and the ratio of /sup 238/U capture to /sup 239/U capture to /sup 239/Pu fission. Uncertainty estimates are presented for all calibrations. Intercomparison measurements are reported which support the validity of the calibration techniques and their estimated uncertainties.

  16. Measurement of the neutron-induced fission cross-section of 243Am relative to 235U from 0.5 to 20 MeV

    NASA Astrophysics Data System (ADS)

    Belloni, F.; Calviani, M.; Colonna, N.; Mastinu, P.; Milazzo, P. M.; Abbondanno, U.; Aerts, G.; Álvarez, H.; Alvarez-Velarde, F.; Andriamonje, S.; Andrzejewski, J.; Audouin, L.; Badurek, G.; Barbagallo, M.; Baumann, P.; Bečvář, F.; Berthoumieux, E.; Calviño, F.; Cano-Ott, D.; Capote, R.; Carrapiço, C.; Cennini, P.; Chepel, V.; Chiaveri, E.; Cortes, G.; Couture, A.; Cox, J.; Dahlfors, M.; David, S.; Dillmann, I.; Domingo-Pardo, C.; Dridi, W.; Duran, I.; Eleftheriadis, C.; Embid-Segura, M.; Ferrari, A.; Ferreira-Marques, R.; Fujii, K.; Furman, W.; Goncalves, I.; Gonzalez-Romero, E.; Goverdovski, A.; Gramegna, F.; Guerrero, C.; Gunsing, F.; Haas, B.; Haight, R.; Heil, M.; Herrera-Martinez, A.; Igashira, M.; Jericha, E.; Käppeler, F.; Kadi, Y.; Karadimos, D.; Karamanis, D.; Kerveno, M.; Koehler, P.; Kossionides, E.; Krtička, M.; Lamboudis, C.; Leeb, H.; Lindote, A.; Lopes, I.; Lozano, M.; Lukic, S.; Marganiec, J.; Marrone, S.; Martínez, T.; Massimi, C.; Meaze, M. H.; Mengoni, A.; Moreau, C.; Mosconi, M.; Neves, F.; Oberhummer, H.; O'Brien, S.; Pancin, J.; Papachristodoulou, C.; Papadopoulos, C.; Paradela, C.; Patronis, N.; Pavlik, A.; Pavlopoulos, P.; Perrot, L.; Pigni, M. T.; Plag, R.; Plompen, A.; Plukis, A.; Poch, A.; Praena, J.; Pretel, C.; Quesada, J.; Rauscher, T.; Reifarth, R.; Rosetti, M.; Rubbia, C.; Rudolf, G.; Rullhusen, P.; Salgado, J.; Santos, C.; Sarchiapone, L.; Savvidis, I.; Stephan, C.; Tagliente, G.; Tain, J. L.; Tarrio, D.; Tassan-Got, L.; Tavora, L.; Terlizzi, R.; Vannini, G.; Vaz, P.; Ventura, A.; Villamarin, D.; Vincente, M. C.; Vlachoudis, V.; Vlastou, R.; Voss, F.; Walter, S.; Wiescher, M.; Wisshak, K.

    2011-12-01

    The ratio of the neutron-induced fission cross-sections of 243Am and 235U was measured in the energy range from 0.5 to 20 MeV with uncertainties of ≈ 4%. The experiment was performed at the CERN n_TOF facility using a fast ionization chamber. With the good counting statistics that could be achieved thanks to the high instantaneous flux and the low backgrounds, the present results are useful for resolving discrepancies in previous data sets and are important for future reactors with improved fuel burn-up.

  17. Certified reference materials for radionuclides in Bikini Atoll sediment (IAEA-410) and Pacific Ocean sediment (IAEA-412).

    PubMed

    Pham, M K; van Beek, P; Carvalho, F P; Chamizo, E; Degering, D; Engeler, C; Gascó, C; Gurriaran, R; Hanley, O; Harms, A V; Herrmann, J; Hult, M; Ikeuchi, Y; Ilchmann, C; Kanisch, G; Kis-Benedek, G; Kloster, M; Laubenstein, M; Llaurado, M; Mas, J L; Nakano, M; Nielsen, S P; Osvath, I; Povinec, P P; Rieth, U; Schikowski, J; Smedley, P A; Suplinska, M; Sýkora, I; Tarjan, S; Varga, B; Vasileva, E; Zalewska, T; Zhou, W

    2016-03-01

    The preparation and characterization of certified reference materials (CRMs) for radionuclide content in sediments collected offshore of Bikini Atoll (IAEA-410) and in the open northwest Pacific Ocean (IAEA-412) are described and the results of the certification process are presented. The certified radionuclides include: (40)K, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (234)U, (238)U, (239)Pu, (239+240)Pu and (241)Am for IAEA-410 and (40)K, (137)Cs, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (235)U, (238)U, (239)Pu, (240)Pu and (239+240)Pu for IAEA-412. The CRMs can be used for quality assurance and quality control purposes in the analysis of radionuclides in sediments, for development and validation of analytical methods and for staff training.

  18. R-matrix analysis of {sup 235}U neutron transmission and cross sections in the energy range 0 to 2.25 keV

    SciTech Connect

    Leal, L.C.; Derrien, H.; Larson, N.M.; Wright, R.Q.

    1997-11-01

    This document describes a new R-matrix analysis of {sup 235}U cross section data in the energy range from 0 to 2,250 eV. The analysis was performed with the computer code SAMMY, that has recently been updated to permit, for the first time, inclusion of both differential and integral data within the analysis process. Fourteen differential data sets and six integral quantities were used in this evaluation: two measurements of fission plus capture, one of fission plus absorption, six of fission alone, two of transmission, and one of eta, plus standard values of thermal cross sections for fission, capture, and scattering, and of K1 and the Westcott g-factors for both fission and absorption. An excellent representation was obtained for the high-resolution transmission, fission, and capture cross-section data as well as for the integral quantities. The result is a single set of resonance parameters spanning the entire range up to 2,250 eV, a decided improvement over the present ENDF/VI evaluation, in which eleven discrete resonance parameter sets are required to cover that same energy range. This new evaluation is expected to greatly improve predictability of the criticality safety margins for nuclear systems in which {sup 235}U is present.

  19. True ternary fission, the collinear decay into fragments of similar size in the 252Cf(sf) and 235U(nth, f) reactions

    NASA Astrophysics Data System (ADS)

    von Oertzen, W.; Nasirov, A. K.

    2014-06-01

    The collinear cluster decay in 252Cf(sf, fff), with three cluster fragments of different masses (e.g. 132Sn, 52-48Ca, 68-72Ni), which has been observed by the FOBOS group in JINR, has established a new decay mode of heavy nuclei, the collinear cluster tripartition (CCT). The same type of ternary fission decay has been observed in the reaction 235U(nth, fff). This kind of “true ternary fission” of heavy nuclei has been predicted many times in theoretical works during the last decades. In the present note we discuss true ternary fission (TFFF) into three nuclei of almost equal size (e.g. Z=98→Zi=32, 34, 32) in the same systems. The possible fission channels are predicted from potential-energy (PES) calculations. These PES's show pronounced minima for several ternary fragmentation decays, e.g. for 252Cf(sf) and for 235U(nth, f). They suggest the existence of a variety of collinear ternary fission modes. The TFFF-decays chosen in this letter have very similar dynamical features as the previously observed collinear CCT-decays. The data obtained in the above mentioned experiments allow us to extract the yield for these TFFF-decays in both systems by using specific gates on the measured parameters. These yields are a few 1.0ṡ10-6/(binary fission).

  20. Trajectoires de moindre action et temps de vie pour trois modes de désintégration du noyau ^{234}U

    NASA Astrophysics Data System (ADS)

    Benfoughal, T.; Mirea, M.

    1996-10-01

    A numerical method is used to obtain the optimum cold fission paths for three decay modes of ^{234}U. The WKB-integral is minimized with respect the necking and the elongation. A term which takes into account the effect of the diffuse surface is added to the deformation energy in the framework of the macroscopic model of binary system with different charge densities. The effective masses are computed with more correct coordinates of deformation in order to include the variations of the asymmetry during the processes. Calculations are performed to obtain the fission trajectories in a large range of mass-asymmetry including cold fission, cluster emission and alpha-decay. Estimations of T_{1/2} are reported. Les trajectoires optimales de fission pour trois modes de désintégration du noyau ^{234}U sont obtenus à l'aide d'une méthode numérique. L'intégrale WKB est minimisée en fonction des coordonnées généralisées qui caractérisent le col et l'élongation. Un terme d'énergie qui prend en considération les effets dus à une surface diffuse du noyau est ajouté à l'énergie de déformation calculée dans le cadre du modèle macroscopique des systèmes binaires avec différentes densités de charge. Les masses effectives sont calculées avec des coordonnées généralisées choisis pour inclure les variations de l'asymétrie durant le processus nucléaire. Des calculs ont été effectués por obtenir les trajectoires de fission dans un grand domaine d'asymétrie de masse rendant compte de la fission froide, de l'émission spontanée de noyaux lourds et de la désintégration alpha. Des estimations de temps de vie sont reproduites.

  1. Age of the moon: An isotopic study of uranium-thorium-lead systematics of lunar samples

    USGS Publications Warehouse

    Tatsumoto, M.; Rosholt, J.N.

    1970-01-01

    Concentrations of U, Th, and Pb in Apollo 11 samples studied are low (U. 0.16 to 0.87; Th, 0.53 to 3.4; Pb, 0.29 to 1.7, in ppm) but the extremely radiogenic lead in samples allows radiometric dating. The fine dust and the breccia have a concordant age of 4.66 billion years on the basis of 207Pb/206Pb, 206Pb/238U, 207Pb/235U, and 208Pb/232Th ratios. This age is comparable with the age of meteorites and with the age generally accepted for the earth. Six crystalline and vesicular samples are distinctly younger than the dust and breccia. The 238U/235U ratio is the same as that in earth rocks, and 234U is in radioactive equilibrium with parent 238U.

  2. Age of the moon: an isotopic study of uranium-thorium-lead systematics of lunar samples.

    PubMed

    Tatsumoto, M; Rosholt, J N

    1970-01-30

    Concentrations of U, Th, and Pb in Apollo 11 samples studied are low (U. 0.16 to 0.87; Th, 0.53 to 3.4; Pb, 0.29 to 1.7, in ppm) but the extremely radiogenic lead in samples allows radiometric dating. The fine dust and the breccia have a concordant age of 4.66 billion years on the basis of (207)Pb/(206)Pb, (206)Pb/(238)U, (207)Pb/(235U), and(208)Pb/(232)Th ratios. This age is comparable with the age of meteorites and with the age generally accepted for the earth. Six crystalline and vesicular samples are distinctly younger than the dust and breccia. The (238)U/(235)U ratio is the same as that in earth rocks, and (234)U is in radioactive equilibrium with parent (238)U.

  3. Effects of Neutron Emission on Fragment Mass and Kinetic Energy Distribution from Thermal Neutron-Induced Fission of {sup 235}U

    SciTech Connect

    Montoya, M.; Rojas, J.; Saetone, E.

    2007-10-26

    The mass and kinetic energy distribution of nuclear fragments from thermal neutron-induced fission of {sup 235}U(n{sub th},f) have been studied using a Monte-Carlo simulation. Besides reproducing the pronounced broadening in the standard deviation of the kinetic energy at the final fragment mass number around m = 109, our simulation also produces a second broadening around m = 125. These results are in good agreement with the experimental data obtained by Belhafaf et al. and other results on yield of mass. We conclude that the obtained results are a consequence of the characteristics of the neutron emission, the sharp variation in the primary fragment kinetic energy and mass yield curves. We show that because neutron emission is hazardous to make any conclusion on primary quantities distribution of fragments from experimental results on final quantities distributions.

  4. High-accuracy determination of the 238U/235U fission cross section ratio up to ≈1 GeV at n_TOF at CERN

    NASA Astrophysics Data System (ADS)

    Paradela, C.; Calviani, M.; Tarrío, D.; Leal-Cidoncha, E.; Leong, L. S.; Tassan-Got, L.; Le Naour, C.; Duran, I.; Colonna, N.; Audouin, L.; Mastromarco, M.; Lo Meo, S.; Ventura, A.; Aerts, G.; Altstadt, S.; Álvarez, H.; Álvarez-Velarde, F.; Andriamonje, S.; Andrzejewski, J.; Badurek, G.; Barbagallo, M.; Baumann, P.; Bécares, V.; Bečvář, F.; Belloni, F.; Berthier, B.; Berthoumieux, E.; Billowes, J.; Boccone, V.; Bosnar, D.; Brugger, M.; Calviño, F.; Cano-Ott, D.; Capote, R.; Carrapiço, C.; Cennini, P.; Cerutti, F.; Chiaveri, E.; Chin, M.; Cortés, G.; Cortés-Giraldo, M. A.; Cosentino, L.; Couture, A.; Cox, J.; David, S.; Diakaki, M.; Dillmann, I.; Domingo-Pardo, C.; Dressler, R.; Dridi, W.; Eleftheriadis, C.; Embid-Segura, M.; Ferrant, L.; Ferrari, A.; Finocchiaro, P.; Fraval, K.; Fujii, K.; Furman, W.; Ganesan, S.; García, A. R.; Giubrone, G.; Gómez-Hornillos, M. B.; Gonçalves, I. F.; González-Romero, E.; Goverdovski, A.; Gramegna, F.; Griesmayer, E.; Guerrero, C.; Gunsing, F.; Gurusamy, P.; Haight, R.; Heil, M.; Heinitz, S.; Igashira, M.; Isaev, S.; Jenkins, D. G.; Jericha, E.; Kadi, Y.; Käppeler, F.; Karadimos, D.; Karamanis, D.; Kerveno, M.; Ketlerov, V.; Kivel, N.; Kokkoris, M.; Konovalov, V.; Krtička, M.; Kroll, J.; Lampoudis, C.; Langer, C.; Lederer, C.; Leeb, H.; Losito, R.; Lozano, M.; Manousos, A.; Marganiec, J.; Martínez, T.; Marrone, S.; Massimi, C.; Mastinu, P.; Mendoza, E.; Mengoni, A.; Milazzo, P. M.; Mingrone, F.; Mirea, M.; Mondelaers, W.; Moreau, C.; Mosconi, M.; Musumarra, A.; O'Brien, S.; Pancin, J.; Patronis, N.; Pavlik, A.; Pavlopoulos, P.; Perkowski, J.; Perrot, L.; Pigni, M. T.; Plag, R.; Plompen, A.; Plukis, L.; Poch, A.; Pretel, C.; Praena, J.; Quesada, J.; Rauscher, T.; Reifarth, R.; Riego, A.; Roman, F.; Rudolf, G.; Rubbia, C.; Rullhusen, P.; Salgado, J.; Santos, C.; Sarchiapone, L.; Sarmento, R.; Saxena, A.; Schillebeeckx, P.; Schmidt, S.; Schumann, D.; Stephan, C.; Tagliente, G.; Tain, J. L.; Tavora, L.; Terlizzi, R.; Tsinganis, A.; Valenta, S.; Vannini, G.; Variale, V.; Vaz, P.; Versaci, R.; Vermeulen, M. J.; Villamarin, D.; Vincente, M. C.; Vlachoudis, V.; Vlastou, R.; Voss, F.; Wallner, A.; Walter, S.; Ware, T.; Weigand, M.; Weiß, C.; Wiesher, M.; Wisshak, K.; Wright, T.; Žugec, P.; n TOF Collaboration

    2015-02-01

    The 238U to 235U fission cross section ratio has been determined at n_TOF up to ≈1 GeV, with two different detection systems, in different geometrical configurations. A total of four datasets has been collected and compared. They are all consistent to each other within the relative systematic uncertainty of 3-4%. The data collected at n_TOF have been suitably combined to yield a unique fission cross section ratio as a function of neutron energy. The result confirms current evaluations up to 200 MeV. Good agreement is also observed with theoretical calculations based on the INCL ++/ Gemini++ combination up to the highest measured energy. The n_TOF results may help solve a long-standing discrepancy between the two most important experimental datasets available so far above 20 MeV, while extending the neutron energy range for the first time up to ≈1 GeV.

  5. 234U/238U and δ87Sr in peat as tracers of paleosalinity in the Sacramento-San Joaquin Delta of California, USA

    USGS Publications Warehouse

    Drexler, Judith Z.; Paces, James B.; Alpers, Charles N.; Windham-Myers, Lisamarie; Neymark, Leonid; Bullen, Thomas D.; Taylor, Howard E.

    2013-01-01

    The purpose of this study was to determine the history of paleosalinity over the past 6000+ years in the Sacramento-San Joaquin Delta (the Delta), which is the innermost part of the San Francisco Estuary. We used a combination of Sr and U concentrations, d87Sr values, and 234U/238U activity ratios (AR) in peat as proxies for tracking paleosalinity. Peat cores were collected in marshes on Browns Island, Franks Wetland, and Bacon Channel Island in the Delta. Cores were dated using 137Cs, the onset of Pb and Hg contamination from hydraulic gold mining, and 14C. A proof of concept study showed that the dominant emergent macrophyte and major component of peat in the Delta, Schoenoplectus spp., incorporates Sr and U and that the isotopic composition of these elements tracks the ambient water salinity across the Estuary. Concentrations and isotopic compositions of Sr and U in the three main water sources contributing to the Delta (seawater, Sacramento River water, and San Joaquin River water) were used to construct a three-end-member mixing model. Delta paleosalinity was determined by examining variations in the distribution of peat samples through time within the area delineated by the mixing model. The Delta has long been considered a tidal freshwater marsh region, but only peat samples from Franks Wetland and Bacon Channel Island have shown a consistently fresh signal (<0.5 ppt) through time. Therefore, the eastern Delta, which occurs upstream from Bacon Channel Island along the San Joaquin River and its tributaries, has also been fresh for this time period. Over the past 6000+ years, the salinity regime at the western boundary of the Delta (Browns Island) has alternated between fresh and oligohaline (0.5-5 ppt).

  6. Trace metal cycling and 238U/235U in New Zealand's fjords: Implications for reconstructing global paleoredox conditions in organic-rich sediments

    NASA Astrophysics Data System (ADS)

    Hinojosa, Jessica L.; Stirling, Claudine H.; Reid, Malcolm R.; Moy, Christopher M.; Wilson, Gary S.

    2016-04-01

    Reconstructing the history of ocean oxygenation provides insight into links between ocean anoxia, biogeochemical cycles, and climate. Certain redox-sensitive elements respond to changes in marine oxygen content through phase shifts and concomitant isotopic fractionation, providing new diagnostic proxies of past ocean hypoxia. Here we explore the behavior and inter-dependence of a suite of commonly utilized redox-sensitive trace metals (U, Mo, Fe, and Mn) and the emerging "stable" isotope system of U (238U/235U, or δ238U) in New Zealand fjords. These semi-restricted basins have chemical conditions spanning the complete redox spectrum from fully oxygenated to suboxic to intermittently anoxic/euxinic. In the anoxic water column, U and Mo concentrations decrease, while Fe and Mn concentrations increase. Similarly, signals of past euxinic conditions can be found by U, Mo, Fe, and Mn enrichment in the underlying sediments. The expected U isotopic shift toward a lower δ238U in the anoxic water column due to U(VI)-U(IV) reduction is not observed; instead, water column δ238U profiles are consistent in fjords of all oxygen content, falling within previously reported ranges for open ocean seawater (δ238U = -0.42 ± 0.07‰). Additionally, surface sediment δ238U results show evidence for competing U isotope fractionation processes. One site indicates increased export of 238U from seawater to the underlying sediments (fractionation between aqueous seawater U and particulate sediment U, or ΔU(aq)-U(solid) = -0.25‰), consistent with redox-driven fractionation. Another site suggests potential U(VI) adsorption-driven fractionation, reflecting increased export of 235U from seawater to sediments (ΔU(aq)-U(solid) = 0.25‰). We discuss several potential factors that could alter δ238U in waters and sediments beyond redox-driven shifts, including adsorption to organic matter in waters of high primary productivity, reaction rates for competing processes of U adsorption and

  7. The 238U/235U isotope ratio of the Earth and the solar system: Constrains from a gravimetrically calibrated U double spike and implications for absolute Pb-Pb ages

    NASA Astrophysics Data System (ADS)

    Weyer, Stefan; Noordmann, Janine; Brennecka, Greg; Richter, Stephan

    2010-05-01

    The ratio of 238U and 235U, the two primordial U isotopes, has been assumed to be constant on Earth and in the solar system. The commonly accepted value for the 238U/235U ratio, which has been used in Pb-Pb dating for the last ~ 30 years, was 137.88. Within the last few years, it has been shown that 1) there are considerable U isotope variations (~1.3‰) within terrestrial material produced by isotope fractionation during chemical reactions [1-3] and 2) there are even larger isotope variations (at least 3.5‰) in calcium-aluminum-rich inclusions (CAIs) in meoteorites that define the currently accepted age of the solar system [4]. These findings are dramatic for geochronology, as a known 238U/235U is a requirement for Pb-Pb dating, the most precise dating technique for absolute ages. As 238U/235U variations can greatly affect the reported absolute Pb-Pb age, understanding and accurately measuring variation of the 238U/235U ratio in various materials is critical, With these new findings, the questions also arises of "How well do we know the average U isotope composition of the Earth and the solar system?" and "How accurate can absolute Pb-Pb ages be?" Our results using a gravimetrically calibrated 233U/236U double spike IRMM 3636 [5] indicate that the U standard NBL 950a, which was commonly used to define the excepted "natural" 238U/235U isotope ratio, has a slightly lower 238U/235U of 137.836 ± 0.024. This value is indistinguishable from the U isotope compositions for NBL 960 and NBL112A, which have been determined by several laboratories, also using the newly calibrated U double spike IRMM 3636 [6]. These findings provide new implications about the average U isotope composition of the Earth and the solar system. Basalts display a very tight range of U isotope variations (~0.25-0.32‰ relative to SRM 950a). Their U isotope composition is also very similar to that of chondrites [4], which however appear to show a slightly larger spread. Accepting terrestrial

  8. ESR dating of tooth enamel: comparison with {230Th }/{234U } speleothem dates at La Chaise-de-Vouthon (Charente), France

    NASA Astrophysics Data System (ADS)

    Blackwell, Bonnie; Porat, N.; Schwarcz, H. P.; Debénath, A.

    One way to assess a new dating method's reliability is by comparing its results with those from well established, independent techniques. A controlled test of the electron spin resonance (ESR) dating method as it is currently being applied to teeth was attempted for the time range 100-250 ka, beyond that of 14C, at the archaeological site of La Chaise-de-Vouthon (Charente, France). Although absent in modern enamel, a single ESR signal with g = 2.0018 in fossil tooth enamel hydroxyapatite increases in amplitude with increasing irradiation doses. ESR ages are derived from the ratio of the AD, the radiation dose needed to produce the observed ESR signal, relative to the natural, environmental dose rate (ED) experienced by the tooth after deposition. Since the age depends on the uranium (U) uptake history assumed, three ages are calculated assuming: (1) early U uptake (EU); (2) continuous (linear) uptake (LU); (3) recent uptake (RU). Generally, the LU age agrees best with known ages determined by other methods, although the RU model is better for some teeth. ESR dating assumes that the fossil has not suffered recrystallization or significant diagenetic alteration. In the preliminary test, three teeth were dated. In Bourgeois-Delaunay, a bovid molar associated with Palaeolithic artefacts was collected from layers dated at 101 ± 12 to 114 ± 7 ka by {230Th }/{234U } dating of the over- and underlying stalagmitic floors. From Suard, two Equus teeth were collected from beneath a stalagmitic floor dating 112 ± 12 ka. ESR dating teeth significantly underestimated the true age for the teeth: the mean ESR ages range from 37 to 94 ka with standard errors of 2-6 ka, and good replicability. Although more teeth at La Chaise need to be tested to ascertain that the underestimation does not result from random variation commonly seen among teeth within one unit, the consistent underestimation suggests a fault in one of the assumptions underlying the dating method. The most obvious

  9. Coulomb and even-odd effects in cold and super-asymmetric fragmentation for thermal neutron induced fission of 235U

    NASA Astrophysics Data System (ADS)

    Montoya, M.

    2016-07-01

    Even-odd effects of the maximal total kinetic energy (Kmax) as a function of charge (Z) and mass (A) of fragments from thermal neutron induced fission of actinides are questioned by other authors. In this work, visiting old results on thermal neutron induced fission of 235U, those even-odd effects are reconfirmed. The cases seeming to contradict even-odd effects are interpreted with the Coulomb effect hypothesis. According to Coulomb effect hypothesis, Kmax is equal to the Coulomb interaction energy of the most compact scission configuration. As a consequence, between two isobaric charge splits with similar Q-values, the more asymmetrical one will get the more compact scission configuration and then it will reach the higher Kmax-value. In some cases, the more asymmetrical charge split corresponds, by coincidence, to an odd charge split; consequently its higher Kmax-value may be misinterpreted as anti-even-odd effect. Another experimental result reported in the literature is the increasing of even-odd effects on charge distribution on the more asymmetrical fragmentations region. In this region, the difference between Kmax and Q-values increases with asymmetry, which means that the corresponding scission configuration needs higher total deformation energy to occur. Higher deformation energy of the fragments implies lower free energy to break nucleon pairs. Consequently, in the asymmetric fragmentation region, the even-odd effects of the distribution of proton number and neutron number must increase with asymmetry.

  10. Effects of Fission Yield Data in the Calculation of Antineutrino Spectra for ^{235}U(n,fission) at Thermal and Fast Neutron Energies.

    PubMed

    Sonzogni, A A; McCutchan, E A; Johnson, T D; Dimitriou, P

    2016-04-01

    Fission yields form an integral part of the prediction of antineutrino spectra generated by nuclear reactors, but little attention has been paid to the quality and reliability of the data used in current calculations. Following a critical review of the thermal and fast ENDF/B-VII.1 ^{235}U fission yields, deficiencies are identified and improved yields are obtained, based on corrections of erroneous yields, consistency between decay and fission yield data, and updated isomeric ratios. These corrected yields are used to calculate antineutrino spectra using the summation method. An anomalous value for the thermal fission yield of ^{86}Ge generates an excess of antineutrinos at 5-7 MeV, a feature which is no longer present when the corrected yields are used. Thermal spectra calculated with two distinct fission yield libraries (corrected ENDF/B and JEFF) differ by up to 6% in the 0-7 MeV energy window, allowing for a basic estimate of the uncertainty involved in the fission yield component of summation calculations. Finally, the fast neutron antineutrino spectrum is calculated, which at the moment can only be obtained with the summation method and may be relevant for short baseline reactor experiments using highly enriched uranium fuel.

  11. Attenuation of a non-parallel beam of gamma radiation by thick shielding—application to the determination of the 235U enrichment with NaI detectors

    NASA Astrophysics Data System (ADS)

    Mortreau, Patricia; Berndt, Reinhard

    2005-09-01

    The traditional method used to determine the Uranium enrichment by nondestructive analysis is based on the "enrichment meter principle" [1]. It involves measuring the intensity of the 186 keV net peak area of 235U in "quasi-infinite" samples. A prominent factor, which affects the peak intensity, is the presence of gamma absorbing material (e.g., container wall, detector cover) between the sample and the detector. Its effect is taken into consideration in a commonly called "wall thickness" correction factor. Often calculated on the basis of approximations, its performance is adequate for small attenuation factors applicable to the case of narrow beams. However these approximations do not lead to precise results when wide non-parallel beams are attenuated through thick container walls. This paper is dedicated to the calculation by numerical integration of the geometrical correction factor ( Kwtc) which describes the effective mean path length of the radiation through the absorbing layer. This factor was calculated as a function of various measurement parameters (types and dimensions of the detector, of the collimator and of the shielding) for the most commonly used collimator shapes and detectors. Both coherent scattering (Rayleigh) and incoherent scattering (Compton) are taken into account for the calculation of the radiation interaction within the detector.

  12. Energy Dependence of Neutron-Induced Fission Product Yields of 235U, 238U and 239Pu Between 0.5 and 14.8 MeV

    NASA Astrophysics Data System (ADS)

    Gooden, Matthew; Tornow, Werner; Tonchev, Anton; Vieira, Dave; Wilhelmy, Jerry; Arnold, Charles; Fowler, Malcolm; Stoyer, Mark

    2014-09-01

    Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements have been performed. The energy dependence of a number of cumulative fission products between 0.5 and 14.8 MeV have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of activation utilizing specially designed dual-fission chambers and γ-ray counting. The dual-fission chambers are back-to-back ionization chambers encasing a target with thin deposits of the same target isotope in each chamber. This method allows for the direct measurement of the fission rate in the activation target with no reference to the fission cross-section, reducing uncertainties. γ-ray counting was performed on well-shield HPGe detectors over a period of 2 months per activation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 4.6 and 14.8 MeV.

  13. Theoretical analyses of (n,xn) reactions on sup 235 U, sup 238 U, sup 237 Np, and sup 239 Pu for ENDF/B-VI

    SciTech Connect

    Young, P.G.; Arthur, E.D.

    1991-01-01

    Theoretical analyses were performed of neutron-induced reactions on {sup 235}U, {sup 238}U, {sup 237}Np, and {sup 239}Pu between 0.01 and 20 MeV in order to calculate neutron emission cross sections and spectra for ENDF/B-VI evaluations. Coupled-channel optical model potentials were obtained for each target nucleus by fitting total, elastic, and inelastic scattering cross section data, as well as low-energy average resonance data. The resulting deformed optical model potentials were used to calculate direct (n,n{prime}) cross sections and transmission coefficients for use in Hauser-Feshbach statistical theory analyses. A fission model with multiple barrier representation, width fluctuation corrections, and preequilibrium corrections were included in the analyses. Direct cross sections for higher-lying vibrational states were calculated using DWBA theory, normalized using B(E{ell}) values determined from (d,d{prime}) and Coulomb excitation data, where available, and from systematics otherwise. Initial fission barrier parameters and transition state density enhancements appropriate to the compound systems involved were obtained from previous analyses, especially fits to charged-particle fission probability data. The parameters for the fission model were adjusted for each target system to obtain optimum agreement with direct (n,f) cross section measurements, taking account of the various multichance fission channels, that is, the different compound systems involved. The results from these analyses were used to calculate most of the neutron (n,n), (n,n{prime}), and (n,xn) cross section data in the ENDF/B/VI evaluations for the above nuclei, and all of the energy-angle correlated spectra. The deformed optical model and fission model parameterizations are described. Comparisons are given between the results of these analyses and the previous ENDF/B-V evaluations as well as with the available experimental data. 14 refs., 3 figs., 1 tab.

  14. Thallium, uranium, and {sup 235}U/{sup 238}U ratios in the digestive gland of American lobster (Homarus americanus) from an industrialized harbor

    SciTech Connect

    Chou, C.L.; Uthe, J.F.

    1995-01-01

    Only a few studies have concentrated on elements such as thallium (TI). Uranium (U) has been studied as a radionuclide of concern in food and the environment. Foodstuffs contain 10-100 ng U{center_dot}{sup -1} with vegetables and cereals contributing most heavily to the daily intake of ca 1.5 ug U. Between 10-30% of ingested U is absorbed, with most being stored in bone. Rainbow trout (onchorynchus mykiss) and longnose sucker (Catostomus catostomus) from a lake with naturally high radioactivity contained < 5 ng U{center_dot}g{sup -1} in the flesh. Trout bone contained 40 ng U{center_dot}g{sup -1}. Higher tissue U concentrations occurred in fish from areas receiving U mining wastes. Bioconcentration factors for bone and flesh were estimated to be low, 118 and 14.7, respectively. This paper describes the Inductively coupled plasma-mass spectrometry (ICP-MS) determination of Tl and U in digestive gland tissue from lobsters captured in the vicinity of Belledune Harbor, New Brunswick, Canada. The harbor is the site of a lead smelter, a fertilizer plant, and a coal-fired power station (the latter due to enter production in late 1993) and thus has the potential of adding significant amounts of Tl to the local marine environment. The accumulation of Tl from water by marine shellfish is low, at least for bivalves, and the accumulated Tl is eliminated in a number of days when the animals are transferred to clean water. Bioconcentration factors for U in finfish ranged from 0.4-17 for larger species. However, because of the high concentrations of various trace elements in lobster digestive gland, its desirability as a foodstuff, and its relatively large size (approximately 20% of the edible tissue yield), we have investigated Tl and U concentrations and {sup 235U}/{sup 238U} ratios in it. 15 refs., 1 fig., 3 tabs.

  15. Beta and gamma decay heat measurements between 0.1s--50,000s for neutron fission of {sup 235}U, {sup 238}U and {sup 239}Pu. Final report, June 1, 1992--December 31, 1996

    SciTech Connect

    Schier, W. A.; Couchell, G. P.

    1996-01-01

    This is a final reporting on the composition of separate beta and gamma decay heat measurements following neutron fission of {sup 235}U and {sup 238}U and {sup 239}Pu and on cumulative and independent yield measurements of fission products of {sup 235}U and {sup 238}U. What made these studies unique was the very short time of 0.1 s after fission that could be achieved by incorporating the helium jet and tape transport system as the technique for transporting fission fragments from the neutron environment of the fission chamber to the low-background environment of the counting area. This capability allowed for the first time decay heat measurements to extend nearly two decades lower on the logarithmic delay time scale, a region where no comprehensive aggregate decay heat measurements had extended to. This short delay time capability also allowed the measurement of individual fission products with half lives as short as 0.2s. The purpose of such studies was to provide tests both at the aggregate level and at the individual nuclide level of the nation`s evaluated nuclear data file associated with fission, ENDF/B-VI. The results of these tests are in general quite encouraging indicating this data base generally predicts correctly the aggregate beta and aggregate gamma decay heat as a function of delay time for {sup 235}U, {sup 238}U and {sup 239}Pu. Agreement with the measured individual nuclide cumulative and independent yields for fission products of {sup 235}U and {sup 238}U was also quite good although the present measurements suggest needed improvements in several individual cases.

  16. Ingestion dose from 238U, 232Th, 226Ra, 40K and 137Cs in cereals, pulses and drinking water to adult population in a high background radiation area, Odisha, India.

    PubMed

    Lenka, Pradyumna; Sahoo, S K; Mohapatra, S; Patra, A C; Dubey, J S; Vidyasagar, D; Tripathi, R M; Puranik, V D

    2013-03-01

    A natural high background radiation area is located in Chhatrapur, Odisha in the eastern part of India. The inhabitants of this area are exposed to external radiation levels higher than the global average background values, due to the presence of uranium, thorium and its decay products in the monazite sands bearing placer deposits in its beaches. The concentrations of (232)Th, (238)U, (226)Ra, (40)K and (137)Cs were determined in cereals (rice and wheat), pulses and drinking water consumed by the population residing around this region and the corresponding annual ingestion dose was calculated. The annual ingestion doses from cereals, pulses and drinking water varied in the range of 109.4-936.8, 10.2-307.5 and 0.5-2.8 µSv y(-1), respectively. The estimated total annual average effective dose due to the ingestion of these radionuclides in cereals, pulses and drinking water was 530 µSv y(-1). The ingestion dose from cereals was the highest mainly due to a high consumption rate. The highest contribution of dose was found to be from (226)Ra for cereals and drinking water and (40)K was the major dose contributor from the intake of pulses. The contribution of man-made radionuclide (137)Cs to the total dose was found to be minimum. (226)Ra was found to be the largest contributor to ingestion dose from all sources.

  17. Neutron scattering cross sections for /sup 232/Th and /sup 238/U inferred from proton scattering and charge exchange measurements. [7 MeV, 26 and 27 MeV

    SciTech Connect

    Hansen, L.F.; Grimes, S.M.; Pohl, B.A.; Poppe, C.H.; Wong, C.

    1980-01-01

    Differential cross sections for the (p,n) reactions to the isobaric analog states (IAS) of /sup 232/Th and /sup 238/U targets were measured at 26 and 27 MeV. The analysis of the data was done in conjunction with the proton elastic and inelastic (2/sup +/, 4/sup +/, 6/sup +/) differential cross sections measured at 26 MeV. Because collective effects are important in this mass region, deformed coupled-channels calculations were carried out for the simultaneous analysis of the proton and neutron outgoing channels. The sensitivity of the calculations was studied with respect to the optical model parameters used in the calculations, the shape of the nuclear charge distribution, the type of coupling scheme assumed among the levels, the magnitude of the deformation parameters, and the magnitude of the isovector potentials, V/sub 1/ and W/sub 1/. A Lane model-consistent analysis of the data was used to infer optical potential parameters for 6- to 7-MeV neutrons. The neutron elastic differential cross sections obtained from these calculations are compared with measurements available in the literature, and with results obtained using neutron parameters from global sets reported at these energies. 7 figures, 3 tables.

  18. Fission Product Data Measured at Los Alamos for Fission Spectrum and Thermal Neutrons on {sup 239}Pu, {sup 235}U, {sup 238}U

    SciTech Connect

    Selby, H.D.; Mac Innes, M.R.; Barr, D.W.; Keksis, A.L.; Meade, R.A.; Burns, C.J.; Chadwick, M.B.; Wallstrom, T.C.

    2010-12-15

    over to the ENDF/B-VII.0 library, except for {sup 99}Mo where the present results are about 4%-relative higher for neutrons incident on {sup 239}Pu and {sup 235}U. Additionally, our results illustrate the importance of representing the incident energy dependence of fission product yields over the fast neutron energy range for high-accuracy work, for example the {sup 147}Nd from neutron reactions on plutonium. An upgrade to the ENDF library, for ENDF/B-VII.1, based on these and other data, is described in a companion paper to this work.

  19. ZPR-3 Assembly 12 : A cylindrical assembly of highly enriched uranium, depleted uranium and graphite with an average {sup 235}U enrichment of 21 atom %.

    SciTech Connect

    Lell, R. M.; McKnight, R. D.; Perel, R. L.; Wagschal, J. J.; Nuclear Engineering Division; Racah Inst. of Physics

    2010-09-30

    Over a period of 30 years, more than a hundred Zero Power Reactor (ZPR) critical assemblies were constructed at Argonne National Laboratory. The ZPR facilities, ZPR-3, ZPR-6, ZPR-9 and ZPPR, were all fast critical assembly facilities. The ZPR critical assemblies were constructed to support fast reactor development, but data from some of these assemblies are also well suited for nuclear data validation and to form the basis for criticality safety benchmarks. A number of the Argonne ZPR/ZPPR critical assemblies have been evaluated as ICSBEP and IRPhEP benchmarks. Of the three classes of ZPR assemblies, engineering mockups, engineering benchmarks and physics benchmarks, the last group tends to be most useful for criticality safety. Because physics benchmarks were designed to test fast reactor physics data and methods, they were as simple as possible in geometry and composition. The principal fissile species was {sup 235}U or {sup 239}Pu. Fuel enrichments ranged from 9% to 95%. Often there were only one or two main core diluent materials, such as aluminum, graphite, iron, sodium or stainless steel. The cores were reflected (and insulated from room return effects) by one or two layers of materials such as depleted uranium, lead or stainless steel. Despite their more complex nature, a small number of assemblies from the other two classes would make useful criticality safety benchmarks because they have features related to criticality safety issues, such as reflection by soil-like material. ZPR-3 Assembly 12 (ZPR-3/12) was designed as a fast reactor physics benchmark experiment with an average core {sup 235}U enrichment of approximately 21 at.%. Approximately 68.9% of the total fissions in this assembly occur above 100 keV, approximately 31.1% occur below 100 keV, and essentially none below 0.625 eV - thus the classification as a 'fast' assembly. This assembly is Fast Reactor Benchmark No. 9 in the Cross Section Evaluation Working Group (CSEWG) Benchmark Specifications

  20. ZPR-3 Assembly 6F : A spherical assembly of highly enriched uranium, depleted uranium, aluminum and steel with an average {sup 235}U enrichment of 47 atom %.

    SciTech Connect

    Lell, R. M.; McKnight, R. D; Schaefer, R. W.; Nuclear Engineering Division

    2010-09-30

    Over a period of 30 years, more than a hundred Zero Power Reactor (ZPR) critical assemblies were constructed at Argonne National Laboratory. The ZPR facilities, ZPR-3, ZPR-6, ZPR-9 and ZPPR, were all fast critical assembly facilities. The ZPR critical assemblies were constructed to support fast reactor development, but data from some of these assemblies are also well suited for nuclear data validation and to form the basis for criticality safety benchmarks. A number of the Argonne ZPR/ZPPR critical assemblies have been evaluated as ICSBEP and IRPhEP benchmarks. Of the three classes of ZPR assemblies, engineering mockups, engineering benchmarks and physics benchmarks, the last group tends to be most useful for criticality safety. Because physics benchmarks were designed to test fast reactor physics data and methods, they were as simple as possible in geometry and composition. The principal fissile species was {sup 235}U or {sup 239}Pu. Fuel enrichments ranged from 9% to 95%. Often there were only one or two main core diluent materials, such as aluminum, graphite, iron, sodium or stainless steel. The cores were reflected (and insulated from room return effects) by one or two layers of materials such as depleted uranium, lead or stainless steel. Despite their more complex nature, a small number of assemblies from the other two classes would make useful criticality safety benchmarks because they have features related to criticality safety issues, such as reflection by soil-like material. ZPR-3 Assembly 6 consisted of six phases, A through F. In each phase a critical configuration was constructed to simulate a very simple shape such as a slab, cylinder or sphere that could be analyzed with the limited analytical tools available in the 1950s. In each case the configuration consisted of a core region of metal plates surrounded by a thick depleted uranium metal reflector. The average compositions of the core configurations were essentially identical in phases A - F. ZPR-3

  1. (238)U/(235)U isotope ratios of crustal material, rivers and products of hydrothermal alteration: new insights on the oceanic U isotope mass balance.

    PubMed

    Noordmann, Janine; Weyer, Stefan; Georg, R Bastian; Jöns, Svenja; Sharma, Mukul

    2016-01-01

    In this study, the U isotope composition, n((238)U)/n((235)U), of major components of the upper continental crust, including granitic rocks of different age and post-Archaean shales, as well as that of rivers (the major U source to the oceans) was investigated. Furthermore, U isotope fractionation during the removal of U at mid-ocean ridges, an important sink for U from the oceans, was investigated by the analyses of hydrothermal water samples (including low- and high-temperature fluids), low-temperature altered basalts and calcium carbonate veins. All analysed rock samples from the continental crust fall into a limited range of δ(238)U between -0.45 and -0.21 ‰ (relative to NBL CRM 112-A), with an average of -0.30 ± 0.15 ‰ (2 SD, N = 11). Despite differences in catchment lithologies, all major rivers define a relatively narrow range between -0.31 and -0.13 ‰, with a weighted mean isotope composition of -0.27 ‰, which is indistinguishable from the estimate for the upper continental crust (-0.30 ‰). Only some tributary rivers from the Swiss Alps display a slightly larger range in δ(238)U (-0.29 to +0.01 ‰) and lower U concentrations (0.87-3.08 nmol/kg) compared to the investigated major rivers (5.19-11.69 nmol/kg). These findings indicate that only minor net U isotope fractionation occurs during weathering and transport of material from the continental crust to the oceans. Altered basalts display moderately enriched U concentrations (by a factor of 3-18) compared to those typically observed for normal mid-ocean ridge basalts. These, and carbonate veins within altered basalts, show large U isotope fractionation towards both heavy and light U isotope compositions (ranging from -0.63 to +0.27 ‰). Hydrothermal water samples display low U concentrations (0.3-1 nmol/kg) and only limited variations in their U isotope composition (-0.43 ± 0.25 ‰) around the seawater value. Nevertheless, two of the investigated fluids display

  2. Certified Reference Material IAEA-446 for radionuclides in Baltic Sea seaweed.

    PubMed

    Pham, M K; Benmansour, M; Carvalho, F P; Chamizo, E; Degering, D; Engeler, C; Gascó, C; Gwynn, J P; Harms, A V; Hrnecek, E; Ibanez, F L; Ilchmann, C; Ikaheimonen, T; Kanisch, G; Kloster, M; Llaurado, M; Mauring, A; Møller, B; Morimoto, T; Nielsen, S P; Nies, H; Norrlid, L D R; Pettersson, H B L; Povinec, P P; Rieth, U; Samuelsson, C; Schikowski, J; Silobritiene, B V; Smedley, P A; Suplinska, M; Vartti, V-P; Vasileva, E; Wong, J; Zalewska, T; Zhou, W

    2014-05-01

    A Certified Reference Material (CRM) for radionuclides in seaweed (Fucus vesiculosus) from the Baltic Sea (IAEA-446) is described and the results of the certification process are presented. The (40)K, (137)Cs, (234)U and (239+240)Pu radionuclides were certified for this material, and information values for 12 other radionuclides ((90)Sr, (99)Tc, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (230)Th, (232)Th, (235)U, (238)U, (239)Pu and (240)Pu) are presented. The CRM can be used for Quality Assurance/Quality Control of analysis of radionuclides in seaweed and other biota samples, as well as for development and validation of analytical methods, and for training purposes.

  3. Uranium isotopes (U-234/U-238) in rivers of the Yukon Basin (Alaska and Canada) as an aid in identifying water sources, with implications for monitoring hydrologic change in arctic regions

    USGS Publications Warehouse

    Kraemer, Thomas F.; Brabets, Timothy P.

    2012-01-01

    The ability to detect hydrologic variation in large arctic river systems is of major importance in understanding and predicting effects of climate change in high-latitude environments. Monitoring uranium isotopes (234U and 238U) in river water of the Yukon River Basin of Alaska and northwestern Canada (2001–2005) has enhanced the ability to identify water sources to rivers, as well as detect flow changes that have occurred over the 5-year study. Uranium isotopic data for the Yukon River and major tributaries (the Porcupine and Tanana rivers) identify several sources that contribute to river flow, including: deep groundwater, seasonally frozen river-valley alluvium groundwater, and high-elevation glacial melt water. The main-stem Yukon River exhibits patterns of uranium isotopic variation at several locations that reflect input from ice melt and shallow groundwater in the spring, as well as a multi-year pattern of increased variability in timing and relative amount of water supplied from higher elevations within the basin. Results of this study demonstrate both the utility of uranium isotopes in revealing sources of water in large river systems and of incorporating uranium isotope analysis in long-term monitoring of arctic river systems that attempt to assess the effects of climate change.

  4. Effects of rotation of fissioning nuclei in the angular distributions of prompt neutrons and gamma rays originating from the polarized-neutron-induced fission of 233U and 235U nuclei

    NASA Astrophysics Data System (ADS)

    Danilyan, G. V.; Klenke, J.; Kopach, Yu. N.; Krakhotin, V. A.; Novitsky, V. V.; Pavlov, V. S.; Shatalov, P. B.

    2014-06-01

    The results of an experiment devoted to searches for effects of rotation of fissioning nuclei in the angular distributions of prompt neutrons and gamma rays originating from the polarized-neutron-induced fission of 233U nuclei are presented. The effects discovered in these angular distributions are opposite in sign to their counterparts in the polarized-neutron-induced fission of 235U nuclei. This is at odds with data on the relative signs of respective effects in the angular distribution of alpha particles from the ternary fission of the same nuclei and may be indicative of problems in the model currently used to describe the effect in question. The report on which this article is based was presented at the seminar held at the Institute of Theoretical and Experimental Physics and dedicated to the 90th anniversary of the birth of Yu.G. Abov, corresponding member of Russian Academy of Sciences, Editor in Chief of the journal Physics of Atomic Nuclei.

  5. In situ Th and U isotope determinations of low-U geological samples using laser ablation single-collector sector-field ICPMS

    NASA Astrophysics Data System (ADS)

    Mertz-Kraus, R.; Jochum, K. P.; Sharp, W. D.; Stoll, B.; Weis, U.; Andreae, M. O.

    2009-12-01

    In situ spatially resolved U-series dating of geological and biological silicates, phosphates and carbonates (e.g., bone, speleothem, coral, and pedogenic silica and carbonate), facilitates measurement of the rates of natural processes (e.g., precipitation, crystallization) during the past 500,000 years. We present a LA-ICPMS technique for precise and accurate determination of Th and U isotopic ratios applicable to samples with U concentrations as low as 0.4 µg/g. Previously, in situ U-series determinations have been done using multi-collector ICPMS. We use a single-collector sector-field ICPMS connected to a 213 Nd:YAG laser ablation system. Precision and accuracy were determined for different matrices, such as synthetic NIST SRM 612, diverse silicate MPI-DING and USGS reference glasses, 91500 zircon, and a travertine previously analyzed by TIMS.230Th and 234U (~0.00001 to 0.0001 µg/g), required laser tracks up to 1800 µm long, rastering over a 400 x 400 µm square and measurement times of 5 to 25 minutes. We applied corrections for background (< 0.2 cps), the tails of 232Th, 235U and 238U peaks on 230Th and 234U (0.1 to 6 cps corresponding to a proportion of 0.3 to 30 % of the measured peak for 232Th and 238U concentrations of 0.003 to 10 µg/g), instrumental mass fractionation (~1 % per atomic mass unit), and differences in element sensitivity of Th and U using the certified values of the reference glasses.230Th/238U and 234U/238U determinations varies between 1.6 and 5 % depending on the extent of peak tailing corrections. We obtained 230Th/238U = 1.65 x 10-5 and 234U/238U = 5.29 x 10-5 for BCR-2G (1.7 µg/g U, 5.9 µg/g Th) which agree within 2 % and 4 %, respectively, with TIMS values (Matthews et al., 2008). For the travertine (2.5 µg/g U, 0.003 µg/g Th) the mean values for four scans (~0.14 mg sample each) are 230Th/238U = 2.47 x 10-5 and 234U/238U = 7.49 x 10-5, within 2 % of TIMS values. Matthews K. et al. (2008), Evaluation of Solid Geologic

  6. Criticality Expermints with Subcritical Clusters of 2.35 Wt% and 4.31 Wt% 2.35U Enriched UO2 Rods in Water at a Water-to-Fuel Volume Ratio of 1.6

    SciTech Connect

    SR Bierman; ED Clayton

    1980-07-01

    The fourth in a series of Nuclear Regulatory Commission funded criticality experiments have provided data for 2.35 wt% and 4.31 wt% {sup 235}U enriched U0{sub 2} rods at a water-to-fuel volume ratio of 1.6. The results from some 147 critical experiments are presented. They include for each enrichment: {sm_bullet}The critical size of single lattices or clusters of fuel {sm_bullet}The critical separation between sub-critical clusters of fuel {sm_bullet}The critical separation between sub-critical clusters of fuel having fixed neutron absorbers between the fuel clusters {sm_bullet}The isolation distance between fuel clusters {sm_bullet}The critical size of fuel clusters containing water holes and voids {sm_bullet}The critical size of fuel clusters separated by flux traps The fixed neutron absorbers for which data were obtained include 304-L steel, borated 304-L steel, copper, copper containing 1 wt% cadmium, cadmium, aluminium, zirconium and two trade name materials containing boron (Boral and Borofl ex).

  7. Porosity of the melting zone and variations in the solid mantle upwelling rate beneath Hawaii: Inferences from {sup 238}U-{sup 230}Th-{sup 226}Ra and {sup 235}U-{sup 231}Pa disequilibria

    SciTech Connect

    Sims, K.W.W.; DePaolo, D.J.; Murrell, M.T.; Baldridge, W.S.; Goldstein, S.; Clague, D.; Jull, M.

    1999-12-01

    Measurements of {sup 238}U-{sup 230}Th-{sup 226}Ra and {sup 235}U-{sup 231}Pa disequilibria in a suite of tholeiitic-to-basanitic lavas provide estimates of porosity, solid mantle upwelling rate and melt transport times beneath Hawaii. The observation that ({sup 230}Th/{sup 238}U) {gt} 1 indicates that garnet is required as a residual phase in the magma sources for all of the lavas. Both chromatographic porous flow and dynamic melting of a garnet peridotite source can adequately explain the combined U-Th-Ra and U-Pa data for these Hawaiian basalts. For chromatographic porous flow, the calculated maximum porosity in the melting zone ranges from 0.3--3% for tholeiites and 0.1--1% for alkali basalts and basanites, and solid mantle upwelling rates range from 40 to 100 cm/yr for tholeiites and from 1 to 3 cm/yr for basanites. For dynamic melting, the escape or threshold porosity is 0.5--2% for tholeiites and 0.1--0.8% for alkali basalts and basanites, and solid mantle upwelling rates range from 10 to 30 cm/yr for tholeiites and from 0.1 to 1 cm/yr for basanites. Assuming a constant melt productivity, calculated total melt fractions range from 15% for the tholeiitic basalts to 3% for alkali basalts and basanites.

  8. Energy Dependence of Fission Product Yields from 235U, 238U and 239Pu for Incident Neutron Energies Between 0.5 and 14.8 MeV

    NASA Astrophysics Data System (ADS)

    Gooden, M.; Arnold, C.; Bredeweg, T.; Vieira, D.; Wilhelmy, J.; Tonchev, A.; Stoyer, M.; Bhike, M.; Krishichayan, F.; Tornow, W.; Fowler, M.

    2015-10-01

    Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements has been performed. The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of fission counting using specially designed dual-fission chambers and ?-ray counting. Each dual-fission chamber is a back-to-back ionization chamber encasing an activation target in the center with thin deposits of the same target isotope in each chamber. This method allows for the direct measurement of the total number of fissions in the activation target with no reference to the fission cross-section, thus reducing uncertainties. ?-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of 2 months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6, 5.5, 7.5, 8.9 and 14.8 MeV. These results are compared to previous measurements and theoretical estimates. This work was performed under the auspices of the USDoE by Los Alamos National Security, LLC under Contract DE-AC52-06NA25396.

  9. Beta and gamma decay heat measurements between 0.1s - 50,000s for neturon fission of {sup 235}U, {sup 238}U and {sup 239}Pu. Progress report, June 1, 1992--December 31, 1994

    SciTech Connect

    Schier, W.A.; Couchell, G.P.

    1997-05-01

    In the investigations reported here, a helium-jet/tape-transport system was used for the rapid transfer of fission products to a low-background environment where their aggregate beta and gamma-ray spectra were measured as a function of delay time after neutron induced fission of {sup 235}U, {sup 238}U and {sup 239}Pu. Beta and gamma-ray energy distributions have been deduced for delay times as short as 0.2 s and extending out to 100,000s. Instrumentation development during the initial phase of the project included: (1) assembly and characterization of a NaI(Tl) spectrometer for determining aggregate gamma-ray energy distributions, (2) development and characterization of a beta spectrometer (having excellent gamma-ray rejection) for measuring aggregate beta-particle energy distributions, (3) assembly and characterization of a Compton-suppressed HPGe spectrometer for determining gamma-ray intensities of individual fission products to deduce fission-product yields. Spectral decomposition and analysis codes were developed for deducing energy distributions from measured aggregate beta and gamma spectra. The aggregate measurements in the time interval 0.2 - 20s after fission are of special importance since in this region data from many short-lived nuclei are missing and summation calculations in this region rely on model calculations for a large fraction of their predicted beta and gamma decay heat energy spectra. Comparison with ENDF/B-VI fission product data was performed in parallel with the measurements through a close collaboration with Dr. T. England at LANL, assisted by one of our graduate students. Such aggregate measurements provide tests of the Gross Theory of beta decay used to calculated missing contributions to this data base. Fission-product yields deduced from the HPGe studies will check the accuracy of the semi-empirical Gaussian dispersion model used presently by evaluators in the absence of measured yields.

  10. NEUTRON TOTAL CROSS SECTIONS OF 235U FROM TRANSMISSION MEASUREMENTS IN THE ENERGY RANGE 2 keV to 300 keV AND STATISTICAL MODEL ANALYSIS OF THE DATA

    SciTech Connect

    Derrien, H.

    2000-05-22

    The average {sup 235}U neutron total cross sections were obtained in the energy range 2 keV to 330 keV from high-resolution transmission measurements of a 0.033 atom/b sample. The experimental data were corrected for the contribution of isotope impurities and for resonance self-shielding effects in the sample. The results are in very good agreement with the experimental data of Poenitz et al. in the energy range 40 keV to 330 keV and are the only available accurate experimental data in the energy range 2 keV to 40 keV. ENDF/B-VI evaluated data are 1.7% larger. The SAMMY/FITACS code was used for a statistical model analysis of the total cross section, selected fission cross sections and {alpha} data in the energy range 2 keV to 200 keV. SAMMY/FITACS is an extended version of SAMMY which allows consistent analysis of the experimental data in the resolved and unresolved resonance region. The Reich-Moore resonance parameters were obtained from a SAMMY Bayesian fits of high resolution experimental neutron transmission and partial cross section data below 2.25 keV, and the corresponding average parameters and covariance data were used in the present work as input for the statistical model analysis of the high energy range of the experimental data. The result of the analysis shows that the average resonance parameters obtained from the analysis of the unresolved resonance region are consistent with those obtained in the resolved energy region. Another important result is that ENDF/B-VI capture cross section could be too small by more than 10% in the energy range 10 keV to 200 keV.

  11. Neutron Total Cross Sections of {sup 235}U From Transmission Measurements in the Energy Range 2 keV to 300 keV and Statistical Model Analysis of the Data

    SciTech Connect

    Derrien, H.; Harvey, J.A.; Larson, N.M.; Leal, L.C.; Wright, R.Q.

    2000-05-01

    The average {sup 235}U neutron total cross sections were obtained in the energy range 2 keV to 330 keV from high-resolution transmission measurements of a 0.033 atom/b sample.1 The experimental data were corrected for the contribution of isotope impurities and for resonance self-shielding effects in the sample. The results are in very good agreement with the experimental data of Poenitz et al.4 in the energy range 40 keV to 330 keV and are the only available accurate experimental data in the energy range 2 keV to 40 keV. ENDF/B-VI evaluated data are 1.7% larger. The SAMMY/FITACS code 2 was used for a statistical model analysis of the total cross section, selected fission cross sections and data in the energy range 2 keV to 200 keV. SAMMY/FITACS is an extended version of SAMMY which allows consistent analysis of the experimental data in the resolved and unresolved resonance region. The Reich-Moore resonance parameters were obtained 3 from a SAMMY Bayesian fits of high resolution experimental neutron transmission and partial cross section data below 2.25 keV, and the corresponding average parameters and covariance data were used in the present work as input for the statistical model analysis of the high energy range of the experimental data. The result of the analysis shows that the average resonance parameters obtained from the analysis of the unresolved resonance region are consistent with those obtained in the resolved energy region. Another important result is that ENDF/B-VI capture cross section could be too small by more than 10% in the energy range 10 keV to 200 keV.

  12. Radiation Doses to Members of the U.S. Population from Ubiquitous Radionuclides in the Body: Part 1, Autopsy and In Vivo Data

    SciTech Connect

    Watson, David J.; Strom, Daniel J.

    2011-02-25

    This paper is part one of a three-part series investigating annual effective doses to residents of the United States from intakes of ubiquitous radionuclides, including radionuclides occurring naturally, radionuclides whose concentrations are technologically enhanced, and anthropogenic radionuclides. This series of papers explicitly excludes intakes from inhaling 222Rn, 220Rn, and their short-lived decay products; it also excludes intakes of radionuclides in occupational and medical settings. The goal of part one of this work was to review, summarize, and characterize all published and some unpublished data for U.S. residents on ubiquitous radionuclide concentrations in tissues and organs. Forty-five papers and reports were obtained and their data reviewed, and three data sets were obtained via private communication. The 45 radionuclides of interest are the 238U series (14 nuclides), the actinium series (headed by 235U; 11 nuclides), and the 232Th series (11 nuclides); primordial radionuclides 87Rb and 40 K; cosmogenic and fallout radionuclides 14C and 3H; and purely anthropogenic radionuclides 137Cs-137mBa, 129I, and 90Sr-90Y. Measurements judged to be relevant were available for only 15 of these radionuclides: 238U, 235U, 234U, 232Th, 230Th, 228Th, 228Ra, 226Ra, 210Pb, 210Po, 137Cs, 87Rb, 40K, 14C, and 3H. Recent and relevant measurements were not available for 129I and 90Sr-90Y. A total of 11,714 radionuclide concentration measurements were found in one or more tissues or organs from 14 States. Data on age, sex, geographic locations, height, and weight of subjects were available only sporadically. Too often authors did not provide meaningful values of uncertainty of measurements so that variability in data sets is confounded with measurement uncertainty. The following papers detail how these shortcomings are overcome to achieve the goals of the three-part series.

  13. Energy Dependence of Fission Product Yields from {sup 235}U, {sup 238}U and {sup 239}Pu for Incident Neutron Energies Between 0.5 and 14.8 MeV

    SciTech Connect

    Gooden, M.E.; Arnold, C.W.; Becker, J.A.; Bhatia, C.; Bhike, M.; Bond, E.M.; Bredeweg, T.A.; Fallin, B.; Fowler, M.M.; Howell, C.R.; Kelley, J.H.; Krishichayan; Macri, R.; Rusev, G.; Ryan, C.; Sheets, S.A.; Stoyer, M.A.; Tonchev, A.P.; Tornow, W.; and others

    2016-01-15

    Fission Product Yields (FPY) have historically been one of the most observable features of the fission process. They are known to have strong variations that are dependent on the fissioning species, the excitation energy, and the angular momentum of the compound system. However, consistent and systematic studies of the variation of these FPY with energy have proved challenging. This is caused primarily by the nature of the experiments that have traditionally relied on radiochemical procedures to isolate specific fission products. Although radiochemical procedures exist that can isolate all products, each element presents specific challenges and introduces varying degrees of systematic errors that can make inter-comparison of FPY uncertain. Although of high importance in fields such as nuclear forensics and Stockpile Stewardship, accurate information about the energy dependence of neutron induced FPY are sparse, due primarily to the lack of suitable monoenergetic neutron sources. There is a clear need for improved data, and to address this issue, a collaboration was formed between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL) and the Triangle Universities Nuclear Laboratory (TUNL) to measure the energy dependence of FPY for {sup 235}U, {sup 238}U and {sup 239}Pu. The measurements have been performed at TUNL, using a 10 MV Tandem Van de Graaff accelerator to produce monoenergetic neutrons at energies between 0.6 MeV to 14.8 MeV through a variety of reactions. The measurements have utilized a dual-fission chamber, with thin (10-100 μg/cm2) reference foils of similar material to a thick (100-400 mg) activation target held in the center between the chambers. This method allows for the accurate determination of the number of fissions that occurred in the thick target without requiring knowledge of the fission cross section or neutron fluence on target. Following activation, the thick target was removed from the dual-fission chamber

  14. Energy Dependence of Fission Product Yields from 235U, 238U and 239Pu for Incident Neutron Energies Between 0.5 and 14.8 MeV

    NASA Astrophysics Data System (ADS)

    Gooden, M. E.; Arnold, C. W.; Becker, J. A.; Bhatia, C.; Bhike, M.; Bond, E. M.; Bredeweg, T. A.; Fallin, B.; Fowler, M. M.; Howell, C. R.; Kelley, J. H.; Krishichayan; Macri, R.; Rusev, G.; Ryan, C.; Sheets, S. A.; Stoyer, M. A.; Tonchev, A. P.; Tornow, W.; Vieira, D. J.; Wilhelmy, J. B.

    2016-01-01

    Fission Product Yields (FPY) have historically been one of the most observable features of the fission process. They are known to have strong variations that are dependent on the fissioning species, the excitation energy, and the angular momentum of the compound system. However, consistent and systematic studies of the variation of these FPY with energy have proved challenging. This is caused primarily by the nature of the experiments that have traditionally relied on radiochemical procedures to isolate specific fission products. Although radiochemical procedures exist that can isolate all products, each element presents specific challenges and introduces varying degrees of systematic errors that can make inter-comparison of FPY uncertain. Although of high importance in fields such as nuclear forensics and Stockpile Stewardship, accurate information about the energy dependence of neutron induced FPY are sparse, due primarily to the lack of suitable monoenergetic neutron sources. There is a clear need for improved data, and to address this issue, a collaboration was formed between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL) and the Triangle Universities Nuclear Laboratory (TUNL) to measure the energy dependence of FPY for 235U, 238U and 239Pu. The measurements have been performed at TUNL, using a 10 MV Tandem Van de Graaff accelerator to produce monoenergetic neutrons at energies between 0.6 MeV to 14.8 MeV through a variety of reactions. The measurements have utilized a dual-fission chamber, with thin (10-100 μg/cm2) reference foils of similar material to a thick (100-400 mg) activation target held in the center between the chambers. This method allows for the accurate determination of the number of fissions that occurred in the thick target without requiring knowledge of the fission cross section or neutron fluence on target. Following activation, the thick target was removed from the dual-fission chamber and gamma

  15. Energy dependence of fission product yields from 235U, 238U and 239Pu for incident neutron energies between 0.5 and 14.8 MeV

    DOE PAGES

    Gooden, M. E.; Arnold, C. W.; Becker, J. A.; ...

    2016-01-06

    In this study, Fission Product Yields (FPY) have historically been one of the most observable features of the fission process. They are known to have strong variations that are dependent on the fissioning species, the excitation energy, and the angular momentum of the compound system. However, consistent and systematic studies of the variation of these FPY with energy have proved challenging. This is caused primarily by the nature of the experiments that have traditionally relied on radiochemical procedures to isolate specific fission products. Although radiochemical procedures exist that can isolate all products, each element presents specific challenges and introduces varyingmore » degrees of systematic errors that can make inter-comparison of FPY uncertain. Although of high importance in fields such as nuclear forensics and Stockpile Stewardship, accurate information about the energy dependence of neutron induced FPY are sparse, due primarily to the lack of suitable monoenergetic neutron sources. There is a clear need for improved data, and to address this issue, a collaboration was formed between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL) and the Triangle Universities Nuclear Laboratory (TUNL) to measure the energy dependence of FPY for 235U, 238U and 239Pu. The measurements have been performed at TUNL, using a 10 MV Tandem Van de Graaff accelerator to produce monoenergetic neutrons at energies between 0.6 MeV to 14.8 MeV through a variety of reactions. The measurements have utilized a dual-fission chamber, with thin (10-100 μg/cm2) reference foils of similar material to a thick (100-400 mg) activation target held in the center between the chambers. This method allows for the accurate determination of the number of fissions that occurred in the thick target without requiring knowledge of the fission cross section or neutron fluence on target. Following activation, the thick target was removed from the dual

  16. ZPR-3 Assembly 11 : A cylindrical sssembly of highly enriched uranium and depleted uranium with an average {sup 235}U enrichment of 12 atom % and a depleted uranium reflector.

    SciTech Connect

    Lell, R. M.; McKnight, R. D.; Tsiboulia, A.; Rozhikhin, Y.; National Security; Inst. of Physics and Power Engineering

    2010-09-30

    Over a period of 30 years, more than a hundred Zero Power Reactor (ZPR) critical assemblies were constructed at Argonne National Laboratory. The ZPR facilities, ZPR-3, ZPR-6, ZPR-9 and ZPPR, were all fast critical assembly facilities. The ZPR critical assemblies were constructed to support fast reactor development, but data from some of these assemblies are also well suited for nuclear data validation and to form the basis for criticality safety benchmarks. A number of the Argonne ZPR/ZPPR critical assemblies have been evaluated as ICSBEP and IRPhEP benchmarks. Of the three classes of ZPR assemblies, engineering mockups, engineering benchmarks and physics benchmarks, the last group tends to be most useful for criticality safety. Because physics benchmarks were designed to test fast reactor physics data and methods, they were as simple as possible in geometry and composition. The principal fissile species was {sup 235}U or {sup 239}Pu. Fuel enrichments ranged from 9% to 95%. Often there were only one or two main core diluent materials, such as aluminum, graphite, iron, sodium or stainless steel. The cores were reflected (and insulated from room return effects) by one or two layers of materials such as depleted uranium, lead or stainless steel. Despite their more complex nature, a small number of assemblies from the other two classes would make useful criticality safety benchmarks because they have features related to criticality safety issues, such as reflection by soil-like material. ZPR-3 Assembly 11 (ZPR-3/11) was designed as a fast reactor physics benchmark experiment with an average core {sup 235}U enrichment of approximately 12 at.% and a depleted uranium reflector. Approximately 79.7% of the total fissions in this assembly occur above 100 keV, approximately 20.3% occur below 100 keV, and essentially none below 0.625 eV - thus the classification as a 'fast' assembly. This assembly is Fast Reactor Benchmark No. 8 in the Cross Section Evaluation Working Group

  17. Vegetation-derived insights on the mobilization and potential transport of radionuclides from the Nopal I natural analog site, Mexico

    SciTech Connect

    Leslie, B.W.; Pickett, D.A.; Pearcy, E.C.

    1999-07-01

    The Nopal I uranium (U) deposit, Pena Blanca, Mexico is a source term and contaminant transport natural analog to the proposed high-level nuclear waste repository at Yucca Mountain, Nevada. In an attempt to characterize the mobilization and potential transport of radionuclides in the unsaturated zone at the Nopal I deposit, vegetation growing on ore piles was analyzed for {sup 238}U, {sup 235}U, and {sup 232}Th decay-series isotopes. Specimens of Phacelia robusta growing on high-grade piles of U ore were collected and analyzed by alpha autoradiography, and by alpha and gamma spectrometry. Activities for U, thorium (Th), and radium (Ra) isotopes (Bq/kg dried plant) were 300, 1,000, and 7,000 for {sup 238}U, {sup 230}Th, and {sup 226}Ra, respectively. The {sup 226}Ra activities in these specimens are among the highest ever measured for plants; furthermore, the plant-to-soil {sup 226}Ra concentration ratio is higher than expected. These results demonstrate the large mobility and bio-availability of Ra in the Nopal I environment, and support previous indications of recent loss of {sup 226}Ra from the ore body. Comparison between the activities of {sup 238}U and {sup 232}Th decay-chain Th isotopes in the plants and in the ore substrate indicate that relative mobilization into pore solutions of {sup 228}Th > {sup 230}Th > {sup 232}Th, in a ratio of about 50--25:4:1, respectively. The similarity of the plant's {sup 234}U/{sup 238}U activity ratio ({approximately}1.2) to that of a caliche deposit that formed adjacent to the Nopal ore body around 54 ka suggests the {sup 234}U/{sup 238}U activity ratio of U released from the ore is approximately 1.2. The U and {sup 226}Ra isotope activities of the plants and ore substrate, and solubility considerations, are used to assess a source term model of the potential Yucca Mountain repository. These results suggest the use of a natural analog source term model in performance assessments may be non-conservative.

  18. High-precision measurements of uranium and thorium isotopic ratios by multi-collector inductively coupled plasma mass spectrometry (MC-ICPMS)

    NASA Astrophysics Data System (ADS)

    Wang, Lisheng; Ma, Zhibang; Duan, Wuhui

    2015-04-01

    Isotopic compositions of U-Th and 230Th dating have been widely used in earth sciences, such as chronology, geochemistry, oceanography and hydrology. In this study, five ages of different carbonate samples were measured using 230Th dating technique with U-Th high-precision isotopic measurements by multi-collector inductively coupled plasma mass spectrometry, in Uranium-series Chronology Laboratory, Institute of Geology and Geophysics, Chinese Academy of Sciences.In this study, the precision and accuracy of uranium isotopic composition were estimated by measuring the uranium ratios of NBS-CRM 112A, NBS-CRM U500 and HU-1. The mean measured ratios, 234U/238U = 52.86 (±0.04) × 10-6 and δ234U = -38.36 (±0.77) × 10-3 for NBS-CRM 112A, 234U/238U = 10.4184 (±0.0001) × 10-3, 236U/238U = 15.43 (±0.01) × 10-4 and 238U/235U = 1.00021 (±0.00002) for NBS-CRM U500, 234U/238U = 54.911 (±0.007) and δ234U = -1.04 (±0.13) × 10-3 for HU-1 (95% confidence levels). The U isotope data for standard reference materials are in excellent agreement with previous studies, further highlighting the reliability and analytical capabilities of our technique. We measured the thorium isotopic ratios of three different thorium standards by MC-ICPMS. The three standards (Th-1, Th-2 and Th-3) were mixed by HU-1 and NBS 232Th standard, with the 230Th/232Th ratios from 10-4 to 10-6. The mean measured atomic ratios, 230Th/232Th = 2.1227 (±0.0024) × 10-6, 2.7246 (±0.0026) × 10-5, and 2.8358 (±0.0007) × 10-4 for Th-1, Th-2 and Th-3 (95% confidence levels), respectively. Using this technique, the following standard samples were dated by MC-ICPMS. Sample RKM-4, collected from Babardos Kendal Hill terrace, was used during the first stage of the Uranium-Series Intercomparison Project (USIP-I). Samples 76001, RKM-5 and RKM-6 were studied during the second stage of the USIP program (USIP-II). Sample 76001 is a laminated flowstone, collected from Sumidero Terejapa, Chiapas, Mexico, and samples

  19. Environmental characterization and radio-ecological impacts of non-nuclear industries on the Red Sea coast.

    PubMed

    El Mamoney, M H; Khater, Ashraf E M

    2004-01-01

    The Red Sea is a deep semi-enclosed and narrow basin connected to the Indian Ocean by a narrow sill in the south and to the Suez Canal in the north. Oil industries in the Gulf of Suez, phosphate ore mining activities in Safaga-Quseir region and intensified navigation activities are non-nuclear pollution sources that could have serious radiological impacts on the marine environment and the coastal ecosystems of the Red Sea. It is essential to establish the radiological base-line data, which does not exist yet, and to investigate the present radio-ecological impact of the non-nuclear industries to preserve and protect the coastal environment of the Red Sea. Some natural and man-made radionuclides have been measured in shore sediment samples collected from the Egyptian coast of the Red Sea. The specific activities of 226Ra and 210Pb (238U) series, 232Th series, 40K and 137Cs (Bq/kg dry weight) were measured using gamma ray spectrometers based on hyper-pure germanium detectors. The specific activities of 210Po (210Pb) and uranium isotopes (238U, 235U and 234U) (Bq/kg dry weight) were measured using alpha spectrometers based on surface barrier (PIPS) detectors after radiochemical separation. The absorbed radiation dose rates in air (nGy/h) due to natural radionuclides in shore sediment and radium equivalent activity index (Bq/kg) were calculated. The specific activity ratios of 228Ra/226Ra, 210Pb/226Ra, 226Ra/238U and 234U/238U were calculated for evaluation of the geo-chemical behaviour of these radionuclides. The average specific activity of 226Ra (238U) series, 232Th series, 40K and 210Pb were 24.7, 31.4, 427.5 and 25.6 Bq/kg, respectively. The concentration of 137Cs in the sediment samples was less than the lower limit of detection. The Red Sea coast is an arid region with very low rainfall and the sediment is mainly composed of sand. The specific activity of 238U, 235U and 234U were 25.3, 2.9 and 25.0 Bq/kg. The average specific activity ratios of 226Ra/228Ra, 210

  20. Health Effects Due to Radionuclides Content of Solid Minerals within Port of Richards Bay, South Africa

    PubMed Central

    Masok, Felix B.; Masiteng, Paulus L.; Mavunda, Risimati D.; Maleka, Peane P.

    2016-01-01

    This study assessed the radiological health hazards to various body organs of workers working within Transnet Precinct in Richards Bay in Kwazulu-Natal, South Africa due to radionuclide content of mineral ores often stored within the facility. Thirty samples were collected from five mineral ores (rock phosphate, rutile, zircon, coal and hematite) and analyzed for 238U, 234U, 226Ra, 210Pb, 235U, 232Th, 228Ra, 228Th and 40K using delayed neutron activation analysis and low energy gamma spectroscopy. Rutile was found to be the most radioactive mineral ore within the facility with 210Pb concentration of 759.00 ± 106.00 Bq·kg−1. Effective annual dose rate in (mSv·y−1) delivered to different organs of the body: testes, bone marrow, whole body, lungs and ovaries from mineral ores were such that dose from mineral ores decreased in the order coal > rutile > rock phosphate > hematite > zircon. The organs with the highest received dose rate were the testes and this received dose was from coal. However, all of the calculated absorbed dose rates to organs of the body were below the maximum permissible safety limits. PMID:27898013

  1. Evaluation of the diffuse contamination of soils caused by residues coming from the large scale production of phosphate fertilisers

    NASA Astrophysics Data System (ADS)

    Martinez, M. J.; Perez-Sirvent, C.; Martinez-Lopez, S.; Bolivar, J. P.; Mosqueda, F.; Vaca, F.; Garcia-Tenorio, R.

    2012-04-01

    The obtaining of phosphate fertilizers results in large amounts of residues that are frequently accumulated in deposits or pools occupying a wide area. These residues are acidic, and contain variable amounts of trace elements and radionuclides. The potentially polluting agents can be leached by rainwater, and so transferred to the surface waters and then to the groundwater after soil infiltration. Since the distribution and thickness of the residue deposits are variable, the contaminants cannot be easily traced back to a single, well defined source, and so a diffuse contamination (nonpoint source pollution) of the surrounding soils and waters occurs. This communication reports the results obtained in the study of soils close to the phosphogypsum deposits placed near Rio Tinto (Huelva, Spain). The zone is affected not only by the mentioned residues but also by the tides due to the vicinity of the sea. The samples studied had a low organic content and a low acidity with average values of 30 mS/cm for the EC. The mineralogical study allowed illite, goethite, quartz, gypsum and kaolinite to be identified as the main mineralogical components. Although the arsenic level was relatively high (about 600 mg/Kg) the data proved that this element is not mobilized into water. Analytical data for 238U , 234U, 235U, 228Th, 230Th, 232Th, 226Ra, 228Ra, 210Po, 40K , 137Cs were also obtained.

  2. Uranium, plutonium, and thorium isotopes in the atmosphere and the lithosphere

    SciTech Connect

    Essien, I.O.

    1983-01-01

    Concentration of /sup 238/U in rain and snow collected at Fayetteville (36/sup 0/N, 94/sup 0/W), Arkansas, showed a marked increase during the summer months of 1980, while Mount St. Helens remained active. This observed increase of /sup 238/U can be explained as due to the fallout of natural uranium from the eruption of Mount St. Helens. Large increases in the concentration of thorium isotopes detected in rain and snow samples during the last months of 1982 and early months of 1983 probably originated from the eruption of El Chichon volcano, which occurred on 28 March 1982. About 450 Ci of /sup 232/Th is estimated to have been injected into the atmosphere by this eruption. Isotopic anomalies were observed in atmospheric samples such as rain and snow. These anomalies can be attributed to various natural as well as man-made sources: nuclear weapon tests, nuclear accidents involving the burn-up of nuclear powered satellites, and volcanic eruptions. The variation of /sup 234/U//sup 238/U ratios in radioactive minerals when leached with nitric acid were also noticed and this variation, while /sup 235/U//sup 238/U remained fairly constant, can be explained in terms of the ..cap alpha..-recoil effect and changes in oxidation state of uranium. Difference found in /sup 239/Pu//sup 238/U ratios in terrestrial samples and uranium minerals can be explained as due to fallout contamination.

  3. Preparation of actinide specimens for the US/UK joint experiment in the Dounreay Prototype Fast Reactor

    SciTech Connect

    Quinby, T C; Adair, H L; Kobisk, E H

    1982-05-01

    A joint research program involving the United States and the United Kingdom was initiated about four years ago for the purpose of studying the fuel behavior of higher actinides using in-core irradiation in the fast reactor at Dounreay, Scotland. Simultaneously, determination of integral cross sections of a wide variety of higher actinide isotopes (physics specimens) was proposed. Coincidental neutron flux and energy spectral measurements were to be made using vanadium encapsulated dosimetry materials in the immediate region of the fuel pellets and physics samples. The higher actinide samples chosen for the fuel study were /sup 241/Am and /sup 244/Cm in the forms of Am/sub 2/O/sub 3/, Cm/sub 2/O/sub 3/, and Am/sub 6/Cm(RE)/sub 7/O/sub 21/, where (RE) represents a mixture of lanthanides. Milligram quantities of actinide oxides of /sup 248/Cm, /sup 246/Cm, /sup 244/Cm, /sup 243/Cm, /sup 243/Am, /sup 241/Am, /sup 244/Pu, /sup 242/Pu, /sup 241/Pu, /sup 240/Pu, /sup 239/Pu, /sup 238/Pu, /sup 237/Np, /sup 238/U, /sup 236/U, /sup 235/U, /sup 234/U, /sup 233/U, /sup 232/Th, /sup 230/Th, and /sup 231/Pa were encapsulated to obtain nuclear cross section and reaction rate data for these materials.

  4. Natural radionuclide mobility and its influence on U-Th-Pb dating of secondary minerals from the unsaturated zone at Yucca Mountain, Nevada

    USGS Publications Warehouse

    Neymark, L.A.; Amelin, Y.V.

    2008-01-01

    Extreme U and Pb isotope variations produced by disequilibrium in decay chains of 238U and 232Th are found in calcite, opal/chalcedony, and Mn-oxides occurring as secondary mineral coatings in the unsaturated zone at Yucca Mountain, Nevada. These very slowly growing minerals (mm my-1) contain excess 206Pb and 208Pb formed from excesses of intermediate daughter isotopes and cannot be used as reliable 206Pb/238U geochronometers. The presence of excess intermediate daughter isotopes does not appreciably affect 207Pb/235U ages of U-enriched opal/chalcedony, which are interpreted as mineral formation ages. Opal and calcite from outer (younger) portions of coatings have 230Th/U ages from 94.6 ?? 3.7 to 361.3 ?? 9.8 ka and initial 234U/238U activity ratios (AR) from 4.351 ?? 0.070 to 7.02 ?? 0.12, which indicate 234U enrichment from percolating water. Present-day 234U/238U AR is ???1 in opal/chalcedony from older portions of the coatings. The 207Pb/235U ages of opal/chalcedony samples range from 0.1329 ?? 0.0080 to 9.10 ?? 0.21 Ma, increase with microstratigraphic depth, and define slow long-term average growth rates of about 1.2-2.0 mm my-1, in good agreement with previous results. Measured 234U/238U AR in Mn-oxides, which pre-date the oldest calcite and opal/chalcedony, range from 0.939 ?? 0.006 to 2.091 ?? 0.006 and are >1 in most samples. The range of 87Sr/86Sr ratios (0.71156-0.71280) in Mn-oxides overlaps that in the late calcite. These data indicate that Mn-oxides exchange U and Sr with percolating water and cannot be used as a reliable dating tool. In the U-poor calcite samples, measured 206Pb/207Pb ratios have a wide range, do not correlate with Ba concentration as would be expected if excess Ra was present, and reach a value of about 1400, the highest ever reported for natural Pb. Calcite intergrown with opal contains excesses of both 206Pb and 207Pb derived from Rn diffusion and from direct ??-recoil from U-rich opal. Calcite from coatings devoid of opal

  5. Breeding of 233U in the thorium-uranium fuel cycle in VVER reactors using heavy water

    NASA Astrophysics Data System (ADS)

    Marshalkin, V. E.; Povyshev, V. M.

    2015-12-01

    A method is proposed for achieving optimal neutron kinetics and efficient isotope transmutation in the 233U-232Th oxide fuel of water-moderated reactors with variable water composition (D2O, H2O) that ensures breeding of the 233U and 235U isotopes. The method is comparatively simple to implement.

  6. Breeding of {sup 233}U in the thorium–uranium fuel cycle in VVER reactors using heavy water

    SciTech Connect

    Marshalkin, V. E. Povyshev, V. M.

    2015-12-15

    A method is proposed for achieving optimal neutron kinetics and efficient isotope transmutation in the {sup 233}U–{sup 232}Th oxide fuel of water-moderated reactors with variable water composition (D{sub 2}O, H{sub 2}O) that ensures breeding of the {sup 233}U and {sup 235}U isotopes. The method is comparatively simple to implement.

  7. Characterization of contaminant transport using naturally-occurring U-series disequilibria. 1998 annual progress report

    SciTech Connect

    Murrell, M.; Ku, T.L.

    1998-06-01

    'The goal of the research is to study the migratory behavior of contaminants in subsurface fractured systems using naturally occurring uranium- and thorium-series radionuclides as tracers under in-situ physico-chemical and hydrogeologic conditions. Naturally occurring U- and Th-series disequilibria can provide information on the rates of adsorption-desorption and transport of contaminants as well as on fluid transport and rock dissolution in a natural setting. The authors are developing a realistic model of contaminant migration in the Snake River Plain Aquifer beneath the INEEL by evaluating the retardation processes involved in the rock/water interaction. The major tasks are to: (1) determine the natural distribution of U, Th, Pa and Ra isotopes in the groundwater as well as in rock minerals and sorbed phases, and (2) study rock/water interaction processes using U/Th series disequilibria and a statistical analysis-based model code for the calculation of in-situ retardation factors of radionuclides and rock/water interaction time scales. This study will also provide an improved understanding of the hydrogeologic features of the site and their impact on the migration of contaminants. This report summarizes results after 20 months of a 36-month project. Studies performed at LANL include analysis of the long-lived nuclides {sup 238}U, {sup 235}U, {sup 234}U, {sup 230}Th, {sup 226}Ra, {sup 232}Th, and {sup 231}Pa by thermal ionization mass spectrometry (TIMS). Studies performed at the Univ. of Southern California include the measurement of short-lived naturally occurring radionuclides by decay-counting techniques and the development of models to predict the migration behavior of these radionuclides. Initial efforts began with analysis of 31, 0.5L water samples obtained through routine sampling by USGS and INEEL personnel. One significant observation from these data is that {sup 234}U/{sup 238}U activity ratios are highest in waters that emanate from local recharge

  8. Natural radionuclides in lichens, mosses and ferns in a thermal power plant and in an adjacent coal mine area in southern Brazil.

    PubMed

    Galhardi, Juliana Aparecida; García-Tenorio, Rafael; Díaz Francés, Inmaculada; Bonotto, Daniel Marcos; Marcelli, Marcelo Pinto

    2017-02-01

    The radio-elements (234)U, (235)U, (238)U, (230)Th, (232)Th and (210)Po were characterized in lichens, mosses and ferns species sampled in an adjacent coal mine area at Figueira City, Paraná State, Brazil, due to their importance for the assessment of human exposure related to the natural radioactivity. The coal is geologically associated with a uranium deposit and has been used as a fossil fuel in a thermal power plant in the city. Samples were initially prepared at LABIDRO (Isotopes and Hydrochemistry Laboratory), UNESP, Rio Claro (SP), Brazil. Then, alpha-spectrometry after several radiochemical steps was used at the Applied Nuclear Physics Laboratories, University of Seville, Seville, Spain, for measuring the activity concentration of the radionuclides. It was (210)Po the radionuclide that most bio-accumulates in the organisms, reaching the highest levels in mosses. The ferns species were less sensitive as bio-monitor than the mosses and lichens, considering polonium in relation to other radionuclides. Fruticose lichens exhibited lower polonium content than the foliose lichens sampled in the same site. Besides biological features, environmental characteristics also modify the radio-elements absorption by lichens and mosses like the type of vegetation covering these organisms, their substrate, the prevailing wind direction, elevation and climatic conditions. Only (210)Po and (238)U correlated in ferns and in soil and rock materials, being particulate emissions from the coal-fired power plant the most probable U-source in the region. Thus, the biomonitors used were able to detect atmospheric contamination by the radionuclides monitored.

  9. Measurement and calculation of high-actinide burnup in the prototype fast reactor

    SciTech Connect

    Broadhead, B.L.; Raman, S.; Dickens, J.K. )

    1991-01-01

    An agreement was signed in May 1979 as a part of a long-term cooperative program between the United Kingdom and the US under the liquid-metal fast breeder reactor agreement of 1976. This agreement included an experiment to carry out irradiations of physics specimens of fissile and fertile actinides to improve our knowledge of basic nuclear physics phenomena. Three fuel pins were prepared by the US to contain the actinide physics samples; two of these pins were irradiated at the Dounreay prototype fast reactor (PFR) for a total irradiation of 63 full-power days. The third pin has only recently been removed from the PFT, following an irradiation of > 500 full-power days. Each pin houses 35 capsules containing milligram quantities of actinide oxides of {sup 231}Pa, {sup 230}Th, {sup 232}Th, {sup 233}U, {sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U, {sup 237}Np, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, {sup 244}Pu, {sup 241}Am, {sup 243}Am, {sup 243}Cm, {sup 244}Cm, {sup 246}Cm, and {sup 248}Cm. Following the return of the first fuel pin (FP-1) to the United States in May 1984, the actinide samples were prepared for studies of fission product yields, isotopics, and material concentrations. The measurements were repeated for the second fuel pin (FP-2) to remedy several problems encountered in the processing of the FP-1 pin. A brief description of the measured and calculated {sup 137}Cs yields for both FP-1 and FP-2 are included in this paper.

  10. Simultaneous determination of gross alpha, gross beta and ²²⁶Ra in natural water by liquid scintillation counting.

    PubMed

    Fons, J; Zapata-García, D; Tent, J; Llauradó, M

    2013-11-01

    The determination of gross alpha, gross beta and (226)Ra activity in natural waters is useful in a wide range of environmental studies. Furthermore, gross alpha and gross beta parameters are included in international legislation on the quality of drinking water [Council Directive 98/83/EC]. In this work, a low-background liquid scintillation counter (Wallac, Quantulus 1220) was used to simultaneously determine gross alpha, gross beta and (226)Ra activity in natural water samples. Sample preparation involved evaporation to remove (222)Rn and its short-lived decay daughters. The evaporation process concentrated the sample ten-fold. Afterwards, a sample aliquot of 8 mL was mixed with 12 mL of Ultima Gold AB scintillation cocktail in low-diffusion vials. In this study, a theoretical mathematical model based on secular equilibrium conditions between (226)Ra and its short-lived decay daughters is presented. The proposed model makes it possible to determine (226)Ra activity from two measurements. These measurements also allow determining gross alpha and gross beta simultaneously. To validate the proposed model, spiked samples with different activity levels for each parameter were analysed. Additionally, to evaluate the model's applicability in natural water, eight natural water samples from different parts of Spain were analysed. The eight natural water samples were also characterised by alpha spectrometry for the naturally occurring isotopes of uranium ((234)U, (235)U and (238)U), radium ((224)Ra and (226)Ra), (210)Po and (232)Th. The results for gross alpha and (226)Ra activity were compared with alpha spectrometry characterization, and an acceptable concordance was obtained.

  11. OSMOSE program : statistical review of oscillation measurements in the MINERVE reactor R1-UO2 configuration.

    SciTech Connect

    Stoven, G.; Klann, R.; Zhong, Z.; Nuclear Engineering Division

    2007-08-28

    The OSMOSE program is a collaboration on reactor physics experiments between the United States Department of Energy and the France Commissariat Energie Atomique. At the working level, it is a collaborative effort between the Argonne National Laboratory and the CEA Cadarache Research Center. The objective of this program is to measure very accurate integral reaction rates in representative spectra for the actinides important to future nuclear system designs, and to provide the experimental data for improving the basic nuclear data files. The main outcome of the OSMOSE measurement program will be an experimental database of reactivity-worth measurements in different neutron spectra for the heavy nuclides. This database can then be used as a benchmark to verify and validate reactor analysis codes. The OSMOSE program (Oscillation in Minerve of isotopes in Eupraxic Spectra) aims at improving neutronic predictions of advanced nuclear fuels through oscillation measurements in the MINERVE facility on samples containing the following separated actinides: {sup 232}Th, {sup 233}U, {sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U, {sup 237}Np, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, {sup 241}Am, {sup 243}Am, {sup 244}Cm, and {sup 245}Cm. The first part of this report provides an overview of the experimental protocol and the typical processing of a series of experimental results which is currently performed at CEA-Cadarache. In the second part of the report, improvements to this technique are presented, as well as the program that was created to process oscillation measurement results from the MINERVE facility in the future.

  12. High-Precision Isotope Analysis of Uranium and Thorium by TIMS

    NASA Astrophysics Data System (ADS)

    Neymark, L. A.; Paces, J. B.

    2006-12-01

    =134).The mean fractionation factor in these analyses is 0.09±0.06 percent per mass unit. The ^{236}U/238U value of about 1.1×10-9 measured in this standard defines an upper limit for the ^{236}U background in the analyses. The mean atomic 234U/238U and activity 230Th/238U for 29 runs of an internal secular equilibrium uranium ore standard is (54.82±0.02) ×10-6 and 1.002±0.002, respectively. The Th isotopic composition in the IRMM-036 standard was obtained after addition of high-purity ^{229}Th tracer and measuring 232Th/^{229}Th and 230Th/^{229}Th ratios in separate lower- and higher-temperature runs, respectively. The resulting 230Th/232Th for 30 runs is 31.09±0.04 ×10-7, in excellent agreement with the certified value of 31.13±0.78 ×10-7. The USGS laboratory measured four samples of depleted to low-enriched uranium in the recent Regular European Inter-laboratory Measurement Evaluation Program (REIMEP-18). The results of these analyses are close to the certified values.

  13. The Ins and Outs of U and Th Isotopic Measurements Using a Nu Plasma 1700 MC-ICP- MS

    NASA Astrophysics Data System (ADS)

    Pietruszka, A. J.; Rooney, T. O.

    2007-12-01

    The Nu Plasma 1700 is a relatively new type of large-geometry MC-ICP-MS that offers the potential to improve the accuracy and precision of U and Th isotopic measurements compared to previous instruments (e.g., the Plasma 54-30, or P54-30). The higher resolution of the Nu Plasma 1700 translates to more than a factor of 6 improvement in the abundance sensitivity at high mass (compared to the P54-30), and virtually eliminates the necessity of a tail correction on 230Th during the measurement of 232Th/230Th ratios (the major source of uncertainty using the P54-30). However, the Nu Plasma 1700 uses a discrete dynode secondary electron multiplier for ion-counting, which has a smaller dynamic range than the Daly detector used by the P54- 30. This prevents the placement of a relatively large 235U signal on the ion-counter, and thus, requires alternative methods to correct for the effects of instrumental mass bias. Initial efforts in our laboratory have focused on the development of standard-sample bracketing (SSB) techniques to correct for mass bias, with a careful evaluation of possible instrumental artifacts such as matrix effects, drift in the bias between the Faraday collectors and the ion-counting detector (Faraday/IC bias), and non-linearity of both the ion-counting detector and the retardation lens. Experiments with solution standards suggest that the major source of uncertainty on U and Th isotopic measurements using the Nu Plasma 1700 in SSB mode is drift in the Faraday/IC bias. Nevertheless, SSB analyses for U and Th solution standards are reproducible to 0.3% for 238U/234U and 0.4% for 232Th/230Th (±2σ), which is similar to the results obtained on the Plasma 54-30 (Luo et al., 1997; Pietruszka et al., 2002). So far, accuracy has been evaluated by repeatedly analyzing the UCSC Th isotopic standard against a previously characterized in-house Th isotopic standard in SSB mode. The result agrees within error of previous determinations for UCSC Th using the Plasma

  14. U-series disequilibrium of basaltic rocks from Kick'em-Jenny submarine volcano, Lesser Antilles island arc

    NASA Astrophysics Data System (ADS)

    Huang, F.; Lundstrom, C. C.

    2005-12-01

    Kick'em Jenny (KEJ) submarine volcano located 9 km to the north of Grenada in the Lesser Antilles volcanic arc produces lavas ranging in composition from high MgO basalts to moderately evolved andesites. We have determined U-series disequilibria in 12 porphyritic lavas erupted from KEJ volcano by TIMS and MC-ICP-MS methods to constrain the timing and identify the processes creating the magma diversity observed. The SiO2 contents of samples studied here vary from 47 to 55 wt.% SiO2 while REE patterns evolve from slightly LREE enriched, MREE/HREE = 1 patterns to strongly LREE enriched, MREE depleted concave-up patterns. Separate dissolutions of sample KEJ100 indicate an external reproducibility (1s) of 0.7% for (230Th/238U) (n=4), 0.8% for (230Th/232Th) (n=4) and 0.6% for (226Ra/230Th) (n=3), respectively. For all sample, (234U/238U) lies within 0.7% of unity, suggesting that secondary alteration by seawater has not disturbed the U-series data significantly. Sample ages for these submarine erupted samples are unknown, resulting in uncertain values for initial (226Ra/230Th); however, 10 out of 12 of the measured (226Ra/230Th) range between 3.16 and 1.13 and are thus unequivocally young with respect to decay of 230Th and 231Pa since eruption. The U (0.535 - 4.876 ppm) and Th (1.25 - 10.78 ppm) concentrations increase with SiO2 contents. (230Th/232Th) has a restricted range, varying from 0.994 to 1.093 with the exception of one sample. (230Th/238U) ranges from 0.684 to 0.875 while (231Pa/235U) ranges from 1.76 up to 2.84, among the highest 231Pa excess in island arcs yet reported. These data confirm previous observations of the unusual behavior of KEJ lavas relative to global observations in having both large 238U and 231Pa excesses. Combined with (226Ra/230Th), these disequilibria observations require that 238U excesses reflect more than solely fluid addition to the mantle wedge from the subducted oceanic slab.

  15. Precise determination of U isotopic compositions in low concentration carbonate samples by MC-ICP-MS.

    PubMed

    Wang, Ruo-Mei; You, Chen-Feng

    2013-03-30

    We developed a fast and simple analytical procedure for precise determination of U isotopic compositions in low concentration natural samples. The main advantage of the new method is that it requires only 12ng U and can obtain all U isotopic ratios without using spike. Five carbonate reference materials (JCp-1, RKM-4, RKM-5, GBW04412 and GBW04413) and 3 international standards with different matrices (IAPSO, IRMM-3184 and CRM-U010) were analyzed for ((234)U/(238)U) and (238)U/(235)U ratios by MC-ICPMS. Using our method, the results for these standards are in close agreement with the certified values, 1.144 ± 0.004, 0.966 ± 0.004 and 0.990 ± 0.003 for ((234)U/(238)U) and 137.72 ± 0.13, 137.64 ± 0.15 and 98.63 ± 0.04 for (238)U/(235)U, in IAPSO, IRMM-3184 and CRM-U010, respectively. The long-term reproducibility of ((234)U/(238)U) and (238)U/(235)U is 0.970 ± 0.002 and 137.56 ± 0.09; 1.144 ± 0.004 and 137.72 ± 0.13, respectively, for in-house U solution and IAPSO. The new ((234)U/(238)U) results for carbonates show much better precision than previous studies and also reflect their age variability. The obtained (238)U/(235)U ratios, representing the first measurements in these carbonate specimens, are rather constant. The method described here requires only 12 ng of U for analysis and can be completed in 5.2 min. The approach provides a fast method to measure ((234)U/(238)U) and (238)U/(235)U ratios in sample matrices commonly encountered in studies of chemical weathering, oceanography and paleoclimatology.

  16. Prompt Fission Neutron Spectra of Actinides

    SciTech Connect

    Capote, R; Chen, Y J; Hambsch, F J; Kornilov, N V; Lestone, J P; Litaize, O; Morillon, B; Neudecker, D; Oberstedt, S; Ohsawa, T; Smith, D. L.

    2016-01-01

    The energy spectrum of prompt neutrons emitted in fission (PFNS) plays a very important role in nuclear science and technology. A Coordinated Research Project (CRP) “Evaluation of Prompt Fission Neutron Spectra of Actinides”was established by the IAEA Nuclear Data Section in 2009, with the major goal to produce new PFNS evaluations with uncertainties for actinide nuclei. The following technical areas were addressed: (i) experiments and uncertainty quantification (UQ): New data for neutron-induced fission of 233U, 235U, 238U, and 239Pu have been measured, and older data have been compiled and reassessed. There is evidence from the experimental work of this CRP that a very small percentage of neutrons emitted in fission are actually scission neutrons; (ii) modeling: The Los Alamos model (LAM) continues to be the workhorse for PFNS evaluations. Monte Carlo models have been developed that describe the fission phenomena microscopically, but further development is needed to produce PFNS evaluations meeting the uncertainty targets; (iii) evaluation methodologies: PFNS evaluations rely on the use of the least-squares techniques for merging experimental and model data. Considerable insight was achieved on how to deal with the problem of too small uncertainties in PFNS evaluations. The importance of considering that all experimental PFNS data are “shape” data was stressed; (iv) PFNS evaluations: New evaluations, including covariance data, were generated for major actinides including 1) non-model GMA evaluations of the 235U(nth,f), 239Pu(nth,f), and 233U(nth,f) PFNS based exclusively on experimental data (0.02 ≤ E ≤ 10 MeV), which resulted in PFNS average energies E of 2.00±0.01, 2.073±0.010, and 2.030±0.013 MeV, respectively; 2) LAM evaluations of neutron-induced fission spectra on uranium and plutonium targets with improved UQ for incident energies from thermal up to 30 MeV; and 3) Point-by-Point calculations for 232Th, 234U and 237Np targets; and (v) data

  17. Method for radioactivity monitoring

    DOEpatents

    Umbarger, C. John; Cowder, Leo R.

    1976-10-26

    The disclosure relates to a method for analyzing uranium and/or thorium contents of liquid effluents preferably utilizing a sample containing counting chamber. Basically, 185.7-keV gamma rays following .sup.235 U alpha decay to .sup.231 Th which indicate .sup.235 U content and a 63-keV gamma ray doublet found in the nucleus of .sup.234 Pa, a granddaughter of .sup.238 U, are monitored and the ratio thereof taken to derive uranium content and isotopic enrichment .sup.235 U/.sup.235 U + .sup.238 U) in the liquid effluent. Thorium content is determined by monitoring the intensity of 238-keV gamma rays from the nucleus of .sup.212 Bi in the decay chain of .sup.232 Th.

  18. Thorium-230 dating of natural waters at the Nevada Test Site

    SciTech Connect

    Bakhtiar, S.N.

    1990-01-01

    Radiocarbon determinations have been used in the past to estimate the ages of groundwater from the Paleozoic aquifer underlying the Nevada Test Site and adjacent areas. We measured the concentrations of {sup 230}Th, {sup 232}Th, {sup 234}U and {sup 238}U in several water samples taken from the wells and spring at the Nevada Test Site and calculated the {sup 230}Th ages. 2 refs.

  19. Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers

    DOE PAGES

    Kayzar, Theresa M.; Williams, Ross W.

    2015-09-26

    The model age or ‘date of purification’ of a nuclear material is an important nuclear forensic signature. In this study, chemical separation and MC-ICP-MS measurement techniques were developed for 226 Ra and 227Ac: grand-daughter nuclides in the 238U and 235U decay chains respectively. The 230Th-234U, 226Ra-238U, 231Pa-235U, and 227Ac-235U radiochronometers were used to calculate model ages for CRM-U100 standard reference material and two highly-enriched pieces of uranium metal from the International Technical Working Group Round Robin 3 Exercise. In conclusion, the results demonstrate the accuracy of the 226Ra-238U and 227Ac-235U chronometers and provide information about nuclide migration during uranium processing.

  20. ORALLOY (93.15 235U) METAL ANNULI WITH BERYLLIUM CORE

    SciTech Connect

    John D. Bess; Leland M. Montierth; Raymond L. Reed; John T. Mihalczo

    2010-09-01

    A variety of critical experiments were constructed of enriched uranium metal during the 1960s and 1970s at the Oak Ridge Critical Experiments Facility (ORCEF) in support of criticality safety operations at the Y-12 Plant. The purposes of these experiments included the evaluation of storage, casting, and handling limits for the Y-12 Plant and providing data for verification of calculation methods and cross-sections for nuclear criticality safety applications. These included solid cylinders of various diameters, annuli of various inner and outer diameters, two and three interacting cylinders of various diameters, and graphite and polyethylene reflected cylinders and annuli. Of the hundreds of delayed critical experiments, two were performed that consisted of uranium metal annuli with a solid beryllium metal core. The outer diameter of the annuli was approximately 13 or 15 inches with an inner diameter of 7 inches. The diameter of the core was approximately 7 inches. The critical height of the configurations was approximately 5 and 4 inches, respectively. The uranium annuli consisted of multiple stacked rings with diametral thicknesses of approximately 2 inches apiece and varying heights. The 15-inch experiment was performed on June 4, 1963, and the 13-inch experiment on July 12, 1963 by J. T. Mihalczo and R. G. Taylor (Ref. 1) with accompanying logbook. Both detailed and simplified model specifications are provided in this evaluation. Both of these fast-spectra experiments were determined to represent acceptable benchmarks. The calculated eigenvalues for both the detailed and simple models are within approximately 0.6% of the benchmark values, but significantly greater than 3s from the benchmark value because the uncertainty in the benchmark is very small: <±0.0004 (1s). There is significant variability between results using different neutron cross section libraries, the greatest being a ?keff of ~0.67%. Unreflected and unmoderated experiments with the same highly enriched uranium metal parts were performed at the Oak Ridge Critical Experiments Facility in the 1960s and are evaluated in HEU MET FAST 051. Thin graphite reflected (2 inches or less) experiments also using the same highly enriched uranium metal parts are evaluated in HEU MET FAST 071. Polyethylene-reflected configurations are evaluated in HEU-MET-FAST-076. A stack of highly enriched metal discs with a thick beryllium reflector is evaluated in HEU-MET-FAST-069.

  1. ORALLOY (93.2 235U) METAL CYLINDER WITH BERYLLIUM TOP REFLECTOR

    SciTech Connect

    John D. Bess; Leland M. Montierth; Raymond Reed; John T. Mihalczo

    2010-09-01

    A variety of critical experiments were constructed of enriched uranium metal during the 1960s and 1970s at the Oak Ridge Critical Experiments Facility (ORCEF) in support of criticality safety operations at the Y-12 Plant. The purposes of these experiments included the evaluation of storage, casting, and handling limits for the Y-12 Plant and providing data for verification of calculation methods and cross-sections for nuclear criticality safety applications. These included solid cylinders of various diameters, annuli of various inner and outer diameters, two and three interacting cylinders of various diameters, and graphite and polyethylene reflected cylinders and annuli. Of the hundreds of delayed critical experiments, one experiment was comprised of a stack of approximately 7-inch-diameter metal discs. The bottom of the stack consisted of uranium with an approximate height of 4-1/8 inches. The top of the stack consisted of beryllium with an approximate height of 5-9/16 inches. This experiment was performed on August 20, 1963 by J. T. Mihalczo and R. G. Taylor (Ref. 1) with accompanying logbook. Both detailed and simplified model specifications are provided in this evaluation. This fast-spectra experiment was determined to represent an acceptable benchmark. The calculated eigenvalues for both the detailed and simple models are within approximately 0.5% of the benchmark values, but significantly greater than 3s from the benchmark value because the uncertainty in the benchmark is very small: ±0.0002 (1s). There is significant variability between results using different neutron cross section libraries, the greatest being a ?keff of ~0.65% . Unreflected and unmoderated experiments with the same highly enriched uranium metal parts were performed at the Oak Ridge Critical Experiments Facility in the 1960s and are evaluated in HEU MET FAST 051. Thin graphite reflected (2 inches or less) experiments also using the same highly enriched uranium metal parts are evaluated in HEU MET FAST 071. Polyethylene-reflected configurations are evaluated in HEU-MET-FAST-076. Highly enriched metal annuli with beryllium cores are evaluated in HEU-MET-FAST-059.

  2. Direct measurement of 235U in spent fuel rods with Gamma-ray mirrors

    NASA Astrophysics Data System (ADS)

    Ruz, J.; Brejnholt, N. F.; Alameda, J. B.; Decker, T. A.; Descalle, M. A.; Fernandez-Perea, M.; Hill, R. M.; Kisner, R. A.; Melin, A. M.; Patton, B. W.; Soufli, R.; Ziock, K.; Pivovaroff, M. J.

    2015-03-01

    Direct measurement of plutonium and uranium X-rays and gamma-rays is a highly desirable non-destructive analysis method for the use in reprocessing fuel environments. The high background and intense radiation from spent fuel make direct measurements difficult to implement since the relatively low activity of uranium and plutonium is masked by the high activity from fission products. To overcome this problem, we make use of a grazing incidence optic to selectively reflect Kα and Kβ fluorescence of Special Nuclear Materials (SNM) into a high-purity position-sensitive germanium detector and obtain their relative ratios.

  3. Utilization of /sup 252/Cf-/sup 235/U fueled subcritical multiplier for neutron activation analysis

    SciTech Connect

    Wogman, N.A.; Lepel, E.A.

    1983-10-05

    Neutron activation analysis is normally performed at thermal fluxes of 10/sup 13/ n/cm/sup 2//s irradiating samples of a few milligrams. When a ten thousand-fold larger sample is available, neutron activation can be performed at proportionately lower fluxes. Thus, a 10 g sample irradiated at 10/sup 9/ n/cm/sup 2//s contains as much activity as a 1 mg sample irradiated at 10/sup 13/ n/cm/sup 2//s. This paper describes the utilization of a subcritical multiplier operating at about 10/sup 9/ n/cm/sup 2//s for the activation of a broad range of sample types and elemental concentrations.

  4. Improving reactor models with a precision beta spectroscopy experiment of the 235U fission spectrum

    NASA Astrophysics Data System (ADS)

    Boswell, Melissa; Gehring, Amanda; Ullmann, John; Haines, Todd; Devlin, Matthew; Elliott, Steven; Rielage, Keith; Goett, John; White, Brandon

    2016-09-01

    The reactor neutrino anomaly could be an indication of non-standard neutrino physics models (e.g. sterile neutrinos), or the discrepancy could be the result of uncertainties in the modeled reactor neutrino spectrum. Understanding the aggregate β spectrum is extremely important for improving the confidence in the underlying predicted reactor neutrino spectrum. The original β spectrum measurement was preformed at the Institut Laue-Langevin (ILL) reactor in the early 1980's and suffered from a number of limitations. A recent attempt at reproducing the ILL experiment concluded that their uncertainties were driven by a low signal to noise ratio, and that the best way to decrease the uncertainties was to conduct the experiment at a neutron beam line similar to the one at Los Alamos. In this talk I will discuss the advantages of reproducing this experiment at the Lujan center at LANL, our proposed experimental setup, and finally steps we are taking to evaluate the systematics associated with these measurements at an accelerator-based neutron beam. Furthermore we will also discuss additional measurement with 238U and 239Pu that are also important to the non-proliferation communities.

  5. Tables of Neutron-Induced Fission Cross Section for Various Pu, U, and Th Isotopes, Deduced from Measured Fission Probabilites

    SciTech Connect

    Younes, W; Britt, H C

    2003-03-31

    Cross sections for neutron-induced fission of {sup 231,233}Th, {sup 234,235,236,237,239}U, and {sup 240,241,243}Pu are presented in tabular form for incident neutron energies of 0.1 {le} E{sub n}(MeV) {le} 2.5. The cross sections were obtained by converting measured fission probabilities from (t,pf) reactions on mass-A targets to (n,f) cross sections on mass-A + 1 neutron targets, by using modeling to compensate for the differences in the reaction mechanisms. Data from Britt et al. were used for the {sup 234}U(t,pf) reaction, from Cramer et al. for the {sup 230,232}Th(t,pf), {sup 236,238}U(t,pf), and {sup 240,242}Pu(t,pf) reactions, and from Britt et al. for the {sup 233,235}U(t,pf) and {sup 239}Pu(t,pf) reactions. The fission probabilities P{sub (t,pf)}(E{sub x}), measured as a function of excitation energy E{sub x} of the compound system formed by the (t,p) reaction, are listed in the tables with the corresponding deduced cross sections as a function of incident neutron energy E{sub n}, {sigma}{sub (n,f)}(E{sub n}). The excitation energy and incident neutron energy are related by E{sub x} = E{sub n} + B{sub n}, where B{sub n}, where B{sub n} is the neutron binding energy. Comparison with ENDF/B-VI evaluations of the well-measured {sup 234,235,236}U(n,f) and {sup 240,241}Pu(n,f) cross sections confirms the accuracy of the present results within a 10% standard deviation above E{sub n} = 1 MeV. Below E{sub n} = 1 MeV, localized deviations of at most {+-} 20% are observed.

  6. Modeling report of the CEA cadarache MINERVE reactor for the OSMOSE project.

    SciTech Connect

    Klann, R.; Perret, G.; Hudelot, J. P.; Antony, M.

    2005-02-25

    The OSMOSE program (Oscillation in Minerve of isotopes in ''Eupraxic'' spectra) is a collaboration between the U.S. Department of Energy (DOE) and the Commissariat a l' Energie Atomique (CEA). It aims at measuring integral absorption rates of minor actinides by the oscillation technique in the MINERVE experimental facility located at the CEA Cadarache Research Center. The OSMOSE program also includes a complete analytical program to understand and resolve potential discrepancies between calculated and measured values. The OSMOSE program began in 2001 and will continue until 2013. The Argonne National Laboratory has developed Monte Carlo and deterministic calculation models of the MINERVE facility to determine core and safety parameters such as axial and radial fission rate distributions, control rod worth, spectral indices, and the reactivity worth of oscillated samples. Oscillation samples include calibration samples with different uranium enrichments and boron concentrations and the OSMOSE samples--separated actinides including {sup 232}Th, {sup 233}U, {sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U, {sup 237}Np, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, {sup 241}Am, {sup 243}Am, {sup 244}Cm and {sup 245}Cm. Seven different neutron spectra will be created in the MINERVE facility: an overmoderated UO{sub 2} matrix (representative of a fuel processing plant or flooded storage cask), a UO{sub 2} matrix in water (representative of LWRs), a mixed oxide fuel matrix (representative of cores containing MOX fuels), two epithermal spectra (representative of under-moderated reactors), a moderated fast spectrum (representative of fast reactors which have some slowing down due to moderators such as lead-bismuth or sodium), and a very hard spectrum (representative of fast reactors with little moderation from reactor coolant). The different spectra are achieved by changing the experimental lattice within the MINERVE reactor. The currently investigated core

  7. Concentration of natural radionuclides in raw water and packaged drinking water and the effect of water treatment.

    PubMed

    Manu, Anitha; Santhanakrishnan, V; Rajaram, S; Ravi, P M

    2014-12-01

    The raw water (RW) samples collected from natural sources are subjected to water treatment process, including reverse osmosis (RO), and are packed in bottles as packaged drinking water (PDW). Raw water (21 samples) taken from deep wells of Chennai and Secunderabad which are used in the production of PDW, were analysed for (234)U, (235)U, (238)U, (226)Ra, (228)Ra and (210)Pb activity concentrations. Activity Concentrations of (234)U, (235)U, (238)U, (226)Ra, (228)Ra, (210)Pb and (210)Po in PDW were also analysed. The mean activity concentrations of (234)U, (235)U, (238)U, (226)Ra, (228)Ra and (210)Pb in RW at Chennai were 12.1, ≤1.3, 7.1, 2.6, 27.5, and 16.3 mBq/L respectively. The mean activity concentrations of (234)U, (235)U, (238)U, (226)Ra, (228)Ra and (210)Pb in RW at Secunderabad were found to be 40.9, 1.7, 41.5 84.5, 100.1, and 17.0 mBq/L respectively. The mean concentrations of (234)U, (235)U, (238)U, (226)Ra, (228)Ra, (210)Pb and (210)Po in PDW at Chennai were found to be ≤1.3, ≤1.3, ≤1.3, ≤0.2, ≤1.7, 28.0 and 1.2 mBq/L at Secunderabad were found to be ≤1.3, ≤1.3, 1.7, 4.3, 5.0 and 28.1 mBq/L. The study indicated a considerable reduction in the concentration of natural radionuclides due to water treatment. The reduction ratios of RW to PDW for (234)U, (238)U, (226)Ra, (228)Ra were 97, 96, 94 and 95%. In case of (210)Pb, the PDW showed higher concentration of (210)Pb than RW. This was due to its in growth from (222)Rn which was not removed in the RO process.

  8. Thorium distributions in high- and low-dust regions and the significance for iron supply

    NASA Astrophysics Data System (ADS)

    Hayes, Christopher T.; Rosen, Jeffrey; McGee, David; Boyle, Edward A.

    2017-02-01

    Thorium and uranium isotopes (232Th, 230Th, 238U, and 234U) were investigated to refine their use for estimating mineral dust deposition and Fe delivery to the ocean. U concentrations and isotope ratios were consistent with conservative behavior and can safely be described using published U-salinity relationships and global average seawater isotopic composition. Near Barbados, waters affected by the Amazon outflow contained elevated 232Th. This signals one region where the thorium-dust method is inaccurate because of a confounding continental input. Dissolved 232Th fluxes in this region suggest that Amazonian Fe supply to the adjacent open ocean is much larger than local atmospheric deposition. The colloidal content of dissolved Th south of Bermuda was found to be quite small (2-6%), similar to that found north of Hawaii, despite the order of magnitude higher dust deposition in the Atlantic. This finding supports the assumption that dissolved 232Th and 230Th are scavenged at the same rate despite their different sources and also sheds light on the increase of dissolved 232Th fluxes with integrated depth. Outside the region influenced by Amazon River waters, dissolved 232Th fluxes are compared with Bermudan aerosol Fe deposition to estimate that fractional Th solubility is around 20% in this region. Finally, new dissolved and soluble Fe, Mn, and Cr data from the subtropical North Pacific support the idea that Fe concentrations in the remote ocean are highly buffered, whereas 232Th has a larger dynamic range between high- and low-dust regions.

  9. Thorium-uranium disequilibrium in a geothermal discharge zone at Yellowstone

    SciTech Connect

    Sturchio, N.C.; Binz, C.M.; Lewis C.H. III

    1987-07-01

    Whole rock samples of hydrothermally-altered Biscuit Basin rhyolite from Yellowstone drill cores Y-7 and Y-8 were analyzed for /sup 230/Th, /sup 234/U, /sup 238/U, and /sup 232/Th. Extreme disequilibrium was found, with (/sup 230/Th//sup 234/U) ranging from 0.30 to 1.27. Values of (/sup 230/Th//sup 232/Th) and (/sup 234/U//sup 232/Th) define a linear correlation with a slope of 0.16 +/- 0.01, which corresponds to a (/sup 230/Th//sup 234/) age of approximately 19 ka. The (/sup 230/Th//sup 234/U) disequilibrium was apparently caused by U redistribution which occurred mostly at about 19 ka, and is not related simply to the relative degree of hydrothermal alteration and self-sealing of the rhyolite. Mass balance of U requires a large flux of U-bearing ground water through the rhyolite at the time of U redistribution; rough estimates of minimum water/rock ratio range from 10/sup 2/ to 10/sup 4/, for a range of possible ground water U concentrations. Conservative hydraulic calculations indicate that the required ground water flux could have occurred within a period of hundreds of years prior to self-sealing. The disequilibrium data are consistent with a model involving U redistribution during the initial stages of development of a geothermal discharge zone that formed in response to the hydrogeologic effects of glacial melting and unloading during the decline of the Pinedale Glaciation.

  10. Surrogate Reactions in the Actinide Region

    SciTech Connect

    Burke, J T; Bernstein, L A; Scielzo, N D; Bleuel, D L; Lesher, S R; Escher, J; Ahle, L; Dietrich, F S; Hoffman, R D; Norman, E B; Sheets, S A; Phair, L; Fallon, P; Clark, R M; Gibelin, J; Jewett, C; Lee, I Y; Macchiavelli, A O; McMahan, M A; Moretto, L G; Rodriguez-Vieitez, E; Wiedeking, M; Lyles, B F; Beausang, C W; Allmond, J M; Ai, H; Cizewski, J A; Hatarik, R; O'Malley, P D; Swan, T

    2008-01-30

    Over the past three years we have studied various surrogate reactions (d,p), ({sup 3}He,t), ({alpha},{alpha}{prime}) on several uranium isotopes {sup 234}U, {sup 235}U, {sup 236}U, and {sup 238}U. An overview of the STARS/LIBERACE surrogate research program as it pertains to the actinides is discussed. A summary of results to date will be presented along with a discussion of experimental difficulties encountered in surrogate experiments and future research directions.

  11. 238U, 232Th profiling and U-series isotope analysis of fossil teeth by laser ablation-ICPMS

    NASA Astrophysics Data System (ADS)

    Eggins, Stephen; Grün, Rainer; Pike, Alistair W. G.; Shelley, Michael; Taylor, Lois

    2003-05-01

    U and Th concentration profiles in fossil hominid and faunal teeth have been measured by laser ablation ICPMS. These profiles record diverse modes of U and Th uptake, particularly within enamel, that can be broadly related to the state of sample preservation. Observed U profiles are in general inconsistent with existing diffusion-adsorption models developed for U-uptake in bone and teeth. Where the models appear applicable, calculated diffusion rates are several orders of magnitude smaller than previous estimates. Laser ablation ICPMS offers a means of rapidly characterizing U and Th distributions in the enamel and dentine components of teeth as a precursor to ESR and U-series dating. In particular, it should allow the identification of teeth (and also bone) samples that have simple U-uptake histories and are amenable to precise dating by time-consuming and expensive Th-U and Pa-U TIMS techniques. We also demonstrated the use of laser ablation ICPMS to measure U-series isotopes in dentine and enamel samples with relatively high U concentrations (>20 ppm). These results, obtained using a quadrupole ICPMS, illustrate significant promise for in situ U-series isotope analysis, particularly when combined with the greater sensitivity and multi-collection capabilities of new sector ICPMS instrumentation. The latter may permit precise isotope ratio measurements on samples containing only a few ppm of U.

  12. Radioactivity in rocks and soil and interaction with groundwater in an arid region

    NASA Astrophysics Data System (ADS)

    Alshamsi, Dalal; Murad, Ahmed; Aldahan, Ala; Hou, Xiaolin; El Saiy, Ayman

    2014-05-01

    Interaction of groundwater with soil and rocks changes the chemical composition of the water both spatially and temporally. In arid regions, surficial recharge of groundwater is generally limited to sporadic rainfall events which may cause rapid interaction between the recharge water and the aquifers materials. Among the elements that commonly increase in concentration as groundwater interact with the aquifer materials are the radioactive elements such as uranium and thorium and their decay chain products. Here, we present data on 235U, 238U, 232Th as well as 137Cs in some sediments and rock aquifers located in the United Arab Emirates (UAE) in southeastern Arabian Peninsula. The Quaternary sediments are composed of silt, sand and gravel with varying proportions of quartz, carbonates, feldspars, evaporites, while the carbonates are mainly limestones, dolomitic limestones, dolomite and calcareous mudstones. These carbonate rocks cover ages extending from 10-230 Myr. After complete digestion using fluoric and nitric acids and chemical separation, the isotopes were measured using ICP-MS. The 235U, 238U and 232Th concentrations ranges are 2.66-32.5 ng/g, 354.7-4453 ng/g and 13.2-1367 ng/g respectively in the carbonate rocks. In the sediments the concentrations are 4.6-17.5 ng/g for 235U, 631.7-2406 ng/g for 238U and 25.6-799.6 ng/g for 232Th. Although it is difficult to quantify the amounts of uranium isotopes that enter the hydrological system from the aquifers, it seems that in the presence of carboxyl ions, uranium forms highly soluble complexes which can be transported to large distances in groundwater. The variations in 232Th concentrations are probably controlled by the availability of sulfate salt rocks (like gypsum) interacting with thorium and forming soluble thorium compounds which can also explain the highly variable concentrations in groundwater.

  13. Evaluation of metal and radionuclide data from neutron activation and acid-digestion-based spectrometry analyses of background soils: Significance in environmental restoration

    SciTech Connect

    Lee, S.Y.; Watkins, D.R.; Jackson, B.L.; Schmoyer, R.L.; Lietzke, D.A.; Burgoa, B.B.; Branson, J.T.; Ammons, J.T.

    1995-12-31

    A faster, more cost-effective, and higher-quality data acquisition procedure for natural background-level metals and radionuclides in soils is needed for remedial investigations of contaminated sites. In this project, a total of 120 soil samples were collected from uncontaminated areas on and near the Oak Ridge Reservation. The samples were taken at three different depths and from three different geologic groups to establish background concentrations of metals and radionuclides. The objective of this presentation is to discuss the advantages and disadvantages of neutron activation analysis (NAA) compared with those of acid-digestion-based spectrometry (ADS) methods; the advantages and disadvantages were evaluated from Al, Sb, As, Cr, Co, Fe, Mg, Mn, Hg, K, Ag, {sup 232}Th, {sup 235}U, {sup 238}U, V, and Zn data. The ADS methods used for this project were inductively coupled plasma (ICP), ICP-mass spectrometry (ICP-MS), and alpha spectrometry. The scatter plots showed that the NAA results for As, Co, Fe, Mn, {sup 232}Th, and {sup 238}U are reasonably correlated with the results from the other analytical methods. Compared to NAA, however, the ADS methods underestimated Al, Cr, Mg, K, V, and Zn. The skew distributions were caused by incomplete dissolution of the analytes during acid digestion of the soil samples. Because of the high detection limits of the spectrometric methods, the NAA results and the ADS results for some elements, including Sb, Hg, and Ag, did not show a definite relationship. The NAA results were highly correlated with the alpha spectrometry results for {sup 232}Th and {sup 238}U but poorly correlated for {sup 235}U, probably because of a larger counting error associated with the lower activity of the isotope. The NAA methods, including the delayed neutron counting method, were far superior techniques for quantifying background levels of radionuclides ({sup 232}Th, {sup 235}U, and {sup 238}U) and metals (Al, Cr, Mg, K, V, and Zn) in soils.

  14. U-Th-Ra variations in Himalayan river sediments (Gandak river, India): Weathering fractionation and/or grain-size sorting?

    NASA Astrophysics Data System (ADS)

    Bosia, Clio; Chabaux, François; Pelt, Eric; France-Lanord, Christian; Morin, Guillaume; Lavé, Jérôme; Stille, Peter

    2016-11-01

    Understanding the origin of U-Th-Ra variations in the Ganga river sediments is a prerequisite for correctly using U-series nuclides to constrain the sediment transport times in Himalayan rivers. For this purpose, U, Th, and Ra concentrations, along with 238U-234U-230Th-226Ra radioactive disequilibria, were analyzed in bank, bedload and suspended sediments from the Gandak river, one of the main tributaries of the Ganga river. The data confirm that U and Th budgets of the Himalayan sediments are significantly influenced by minor resistant minerals, such as zircon, garnet and Ti-bearing minerals, the dissolution of which required the use of a high-pressure acid digestion process. Most importantly, the results indicate that the variations in (238U/232Th) and (230Th/232Th) activity ratios and 238U-234U-230Th-226Ra disequilibria in sediments along the river alluvial plain mainly reflect modifications in the mineralogical and grain-size compositions rather than the degree of weathering during transport. The (238U/232Th) and (230Th/232Th) activity ratios in the bank and bed sediments are related to variations in the minor primary minerals strongly enriched in U and Th (i.e., zircon, REE-bearing minerals and Ti-bearing minerals), whereas the activity ratios in the suspended load are related to variations in the proportions of clay, Fe-oxyhydroxides and the silt-sand fraction, which contains U- and Th-bearing minor minerals. The data also indicate that 238U-234U-230Th-226Ra disequilibria are strongly influenced by secondary mineral phases: the 230Th budget is likely mainly controlled by Fe-oxyhydroxides, and the 226Ra budget is likely mainly controlled by clay minerals. Therefore, the variations in the 238U-234U-230Th-232Th system in the sediments of the Gandak river cannot simply be interpreted as the result of fractionation due to chemical transformation of the bulk sediment during its transport within the alluvial plain and/or the result of radioactive decay. Consequently

  15. Distribution of uranium and thorium in groundwater of arid climate region

    NASA Astrophysics Data System (ADS)

    Murad, Ahmed; Alshamsi, Dalal; Aldahan, Ala; Hou, Xiaolin

    2014-05-01

    Uranium, thorium and their decay products are the most common radionuclides in groundwater in addition to potassium-40. Once groundwater is used for drinking, domestic and irrigation purposes, the radionuclides will then pose environmental and health related hazard originating from radioactivity and toxicity. In the investigation presented here, assessment of 238U, 235U and 232Th concentrations in groundwater across of the United Arab Emirates (UAE) is evaluated in terms of quality and sources. The region is dominated by arid climate conditions and radioactivity assessment of groundwater is essential for safe use of groundwater. Furthermore, the results were linked to data from other arid regions and worldwide. Groundwater samples (total dissolved solids,TDS, 142.5 mg L-1 to 12770 mg L-1) from 67 different wells were collected across geomorphologically different areas and most of the wells are actively used for agriculture. The aquifers are recent sand dunes, Quaternary (3 million years to present) sediments, and older carbonate rocks (230-10 million years). The 235U, 238U and 232Th measurements were carried out using ICP-MS system equipped with an Xt-skimmer cone and a concentric nebulizer under hot plasma conditions. Concentrations of 235U, 238U and 232Th range at (0.125-508.4) ng L-1, (25.81-69237) ng L-1 and (0.236-2529) ng L-1, respectively. Apparently, most 235U, 238U, 232Th concentrations in the sampled groundwater are below the WHO proposed permissible level of 60000 ng/L for total uranium (1 Bq L-1 for 235U and 10 Bq L-1 for 238U) and 5000 ng L-1 (1Bq L-1) for 232Th. A few samples show high concentrations of uranium that are associated with high TDS values and occur within interbedded limestones and shales aquifer. Comparison with worldwide groundwater data suggests that 238U concentration is highest in the arid regions groundwater where the recharge to aquifers is relatively low. The situation for 232Th concentrations seems less affected by climatic

  16. Modern Measurements of Uranium Decay Rates

    NASA Astrophysics Data System (ADS)

    Parsons-Moss, T.; Faye, S. A.; Williams, R. W.; Wang, T. F.; Renne, P. R.; Mundil, R.; Harrison, M.; Bandong, B. B.; Moody, K.; Knight, K. B.

    2015-12-01

    It has been widely recognized that accurate and precise decay constants (λ) are critical to geochronology as highlighted by the EARTHTIME initiative, particularly the calibration benchmarks λ235U and λ238U. [1] Alpha counting experiments in 1971[2] measured λ235U and λ238U with ~0.1% precision, but have never been independently validated. We are embarking on new direct measurements of λ235U, λ238U, λ234Th, and λ234U using independent approaches for each nuclide. For the measurement of λ235U, highly enriched 235U samples will be chemically purified and analyzed for U concentration and isotopic composition by multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Thin films will be electrodeposited from these solutions and the α activity will be measured in an α-γ coincidence counting apparatus, which allows reduced uncertainty in counting efficiency while achieving adequate counting statistics. For λ238U measurement we will measure ingrowth of 234Th in chemically purified, isotopically enriched 238U solutions, by quantitatively separating the Th and allowing complete decay to 234U. All of the measurements will be done using MC-ICP-MS aiming at 0.05% precision. This approach is expected to result in values of λ238U with less than 0.1% uncertainty, if combined with improved λ234Th measements. These will be achieved using direct decay measurements with an E-∆E charged particle telescope in coincidence with a gamma detector. This system allows measurement of 234Th β-decay and simultaneous detection and identification of α particles emitted by the 234U daughter, thus observing λ234U at the same time. The high-precision λ234U obtained by the direct activity measurements can independently verify the commonly used values obtained by indirect methods.[3] An overarching goal of the project is to ensure the quality of results including metrological traceability in order to facilitate implementation across diverse disciplines. [1] T

  17. Chemical weathering rates in deep-sea sediments: Comparison of multicomponent reactive transport models and estimates based on 234U

    NASA Astrophysics Data System (ADS)

    Maher, K.; Steefel, C. I.; Depaolo, D. J.

    2004-12-01

    Chemical weathering rates in natural systems are typically much slower than expected based on experiments and theory. There are several possible explanations. However, because it has been difficult to determine what effects in particular reduce the rates in specific settings, natural rates remain difficult to predict. Silicate-rich deep-sea sediments provide an ideal in-situ laboratory for investigating weathering rates because certain potentially important factors, such as advective transport through heterogeneous media, limitations on the availability of reactive surface area due to low porosity and/or cementation, unsaturated flow conditions, and seasonal variations in fluid flux and temperature, do not occur in this setting. Geochemical profiles from Site 984 in the North Atlantic are modeled using a multi-component reactive transport model (CRUNCH) to determine in-situ rates of plagioclase dissolution and other diagenetic processes, including sulfate reduction and anaerobic methane oxidation. Various possible processes which might contribute to slower rates in the field are considered, including the effect of mineral saturation state, secondary precipitation of clays, inhibition by dissolved aluminum, and the availability of reactive surface area. The reactive transport model includes an isotopic solid-solution formulation that tracks the isotopic composition of precipitating (calcite) and dissolving (plagioclase and calcite) phases, thus allowing the determination of plagioclase dissolution rates. The rate constants for plagioclase determined by geochemical transport modeling of major element profiles are within the same range determined from U-series calculations and suggest that natural weathering rates for this system are on the order of 10-17.5 to 10-17.7 mol/m2/sec assuming estimates of reactive surface area are correct, several orders of magnitude slower than laboratory-derived rates. The slow plagioclase rates are most likely due to the fact that dissolution takes place close to equilibrium, but the close to equilibrium conditions require either slow clay precipitation or precipitation of soluble clays. Unavailability of reactive surface area could also explain the slow rates, but this is considered less likely because of the very high porosity (about 80%) and the low cementation.

  18. The role of the particle size spectrum in estimating POC fluxes from Th234/U238 disequilibrium

    NASA Astrophysics Data System (ADS)

    Burd, Adrian B.; Jackson, George A.; Moran, S. B.

    2007-06-01

    Thorium-234 is increasingly being used as a tracer for particulate organic carbon (POC) export in the oceans. In particular, POC fluxes are being estimated using disequilibrium between Th234 and its parent radionuclide, U238, and estimates of the POC/Th234 ratio of particles settling out of the water column. We have investigated the effect of variations in the particle size distribution on these estimates by using model particle size spectra and size distributions of organic carbon and Th234. Simulations indicate that the POC/Th234 ratio is sensitive to differences in the distributions of organic carbon and Th234 with particle size. If these size distributions differ, then the POC/Th234 ratio is a function of particle size and estimates of the POC/Th234 ratio using size-fractioned samples are inaccurate. Consequently, size fractioning techniques, such as filtration, yield biased estimates if the quantity being measured varies with particle size. We used a model with phytoplankton, fecal pellets and aggregates to examine the assumption that the particles responsible for the Th234 flux are also responsible for the POC flux. We found that variations in the size distributions of these three populations affected POC and Th234 fluxes differently, suggesting that changes in biological interactions can lead to a preferential increase in POC or Th234 flux. We suggest that further examination of the distributions of organic carbon and Th234 with particle size and type is required to refine our understanding of the factors affecting the POC/Th234 ratio.

  19. Radiological investigation of lignite ash. The case of the West Macedonia Lignite Center (Greece)

    SciTech Connect

    Tsikritzis, L.I.; Fotakis, M.; Tzimkas, N.; Tsikritzi, R.; Trikoilidou, E.; Kolovos, N.

    2009-07-01

    This article investigates the natural radioactivity of 26 ash samples, laboratory produced from lignite samples collected in the West Macedonia Lignite Center in Northern Greece. The activity concentrations of {sup 40}K, {sup 235}U, {sup 238}U, {sup 226}Ra, {sup 228}Ra, and 232Th were measured by spectroscopy and found four to five times higher than those in the original lignite samples. The radionuclides transfer factors depend on the characteristics of the combustion process and were found higher for {sup 232}Th, {sup 228}Ra, and 40K, because of their closer affinity with the inorganic fraction of the lignite. Compared with other results found in the published literature, the studied ash has relatively high content in radioactivity, but the resulting radiation dose from the radionuclide emissions in the West Macedonia Lignite Center do not contribute significantly to the total effective dose.

  20. The geochemistry of uranium and thorium isotopes in the Western Desert of Egypt

    SciTech Connect

    Dabous, A.A.

    1994-11-01

    The concentrations of {sup 238}U, {sup 234}U, {sup 232}Th, and {sup 228}Th have been measured in the groundwaters of the Bahariya and Farafra oases of the Western Desert of Egypt. These waters are characterized by normal amounts of U, but unusually high concentrations of Th. The pattern of variation of the parent isotopes, {sup 238}U and {sup 232}Th, as well as the daughter isotopes, {sup 234}U, {sup 230}Th, and {sup 228}Th, is systematic within and between the two oases. From the unusually consistent distribution of the {sup 234}U/{sup 238}U activity ratios one can conclude that the samples from both oases are representative of a two-component mixing system. One component, characterized by low U content and a high {sup 234}U/{sup 238}U activity ratio, is typical of deep artesian systems and probably represents flowthrough water derived from the Nubian highlands to the south. The second component is characterized by a greater U concentration and a low activity ratio. This signature is hypothesized as being derived by leaching of downward infiltrating water during pluvial times. The source of the U may be the uraniferous phosphate strata that overly the sandstone aquifer in both oasis areas. Higher Th values are associated with the artesian flow component of the mixing system and suggests that Th-bearing minerals may be abundant in the Nubian sandstone aquifer. The distribution of {sup 230}Th and {sup 228}Th in the water samples supports this interpretation.

  1. Spatially-Resolved Analyses of Aerodynamic Fallout from a Uranium-Fueled Nuclear Test

    DOE PAGES

    Lewis, L. A.; Knight, K. B.; Matzel, J. E.; ...

    2015-07-28

    The fiive silicate fallout glass spherules produced in a uranium-fueled, near-surface nuclear test were characterized by secondary ion mass spectrometry, electron probe microanalysis, autoradiography, scanning electron microscopy, and energy-dispersive x-ray spectroscopy. Several samples display compositional heterogeneity suggestive of incomplete mixing between major elements and natural U (238U/235U = 0.00725) and enriched U. Samples exhibit extreme spatial heterogeneity in U isotopic composition with 0.02 < 235U/238U < 11.84 among all five spherules and 0.02 < 235U/238U < 7.41 within a single spherule. Moreover, in two spherules, the 235U/238U ratio is correlated with changes in major element composition, suggesting the agglomeration ofmore » chemically and isotopically distinct molten precursors. Two samples are nearly homogenous with respect to major element and uranium isotopic composition, suggesting extensive mixing possibly due to experiencing higher temperatures or residing longer in the fireball. Linear correlations between 234U/238U, 235U/238U, and 236U/238U ratios are consistent with a two-component mixing model, which is used to illustrate the extent of mixing between natural and enriched U end members.« less

  2. Spatially-resolved analyses of aerodynamic fallout from a uranium-fueled nuclear test.

    PubMed

    Lewis, L A; Knight, K B; Matzel, J E; Prussin, S G; Zimmer, M M; Kinman, W S; Ryerson, F J; Hutcheon, I D

    2015-10-01

    Five silicate fallout glass spherules produced in a uranium-fueled, near-surface nuclear test were characterized by secondary ion mass spectrometry, electron probe microanalysis, autoradiography, scanning electron microscopy, and energy-dispersive x-ray spectroscopy. Several samples display compositional heterogeneity suggestive of incomplete mixing between major elements and natural U ((238)U/(235)U = 0.00725) and enriched U. Samples exhibit extreme spatial heterogeneity in U isotopic composition with 0.02 < (235)U/(238)U < 11.84 among all five spherules and 0.02 < (235)U/(238)U < 7.41 within a single spherule. In two spherules, the (235)U/(238)U ratio is correlated with changes in major element composition, suggesting the agglomeration of chemically and isotopically distinct molten precursors. Two samples are nearly homogenous with respect to major element and uranium isotopic composition, suggesting extensive mixing possibly due to experiencing higher temperatures or residing longer in the fireball. Linear correlations between (234)U/(238)U, (235)U/(238)U, and (236)U/(238)U ratios are consistent with a two-component mixing model, which is used to illustrate the extent of mixing between natural and enriched U end members.

  3. Variations in the uranium isotopic compositions of uranium ores from different types of uranium deposits

    NASA Astrophysics Data System (ADS)

    Uvarova, Yulia A.; Kyser, T. Kurt; Geagea, Majdi Lahd; Chipley, Don

    2014-12-01

    Variations in 238U/235U and 234U/238U ratios were measured in uranium minerals from a spectrum of uranium deposit types, as well as diagenetic phosphates in uranium-rich basins and peraluminous rhyolites and associated autunite mineralisation from Macusani Meseta, Peru. Mean δ238U values of uranium minerals relative to NBL CRM 112-A are 0.02‰ for metasomatic deposits, 0.16‰ for intrusive, 0.18‰ for calcrete, 0.18‰ for volcanic, 0.29‰ for quartz-pebble conglomerate, 0.29‰ for sandstone-hosted, 0.44‰ for unconformity-type, and 0.56‰ for vein, with a total range in δ238U values from -0.30‰ to 1.52‰. Uranium mineralisation associated with igneous systems, including low-temperature calcretes that are sourced from U-rich minerals in igneous systems, have low δ238U values of ca. 0.1‰, near those of their igneous sources, whereas uranium minerals in basin-hosted deposits have higher and more variable values. High-grade unconformity-related deposits have δ238U values around 0.2‰, whereas lower grade unconformity-type deposits in the Athabasca, Kombolgie and Otish basins have higher δ238U values. The δ234U values for most samples are around 0‰, in secular equilibrium, but some samples have δ234U values much lower or higher than 0‰ associated with addition or removal of 234U during the past 2.5 Ma. These δ238U and δ234U values suggest that there are at least two different mechanisms responsible for 238U/235U and 234U/238U variations. The 234U/238U disequilibria ratios indicate recent fluid interaction with the uranium minerals and preferential migration of 234U. Fractionation between 235U and 238U is a result of nuclear-field effects with enrichment of 238U in the reduced insoluble species (mostly UO2) and 235U in oxidised mobile species as uranyl ion, UO22+, and its complexes. Therefore, isotopic fractionation effects should be reflected in 238U/235U ratios in uranium ore minerals formed either by reduction of uranium to UO2 or chemical

  4. Determination of U isotope ratios in sediments using ICP-QMS after sample cleanup with anion-exchange and extraction chromatography.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2006-01-15

    The determination of uranium is important for environmental radioactivity monitoring, which investigates the releases of uranium from nuclear facilities and of naturally occurring radioactive materials by the coal, oil, natural gas, mineral, ore refining and phosphate fertilizer industries, and it is also important for studies on the biogeochemical behavior of uranium in the environment. In this paper, we describe a quadrupole ICP-MS (ICP-QMS)-based analytical procedure for the accurate determination of U isotope ratios ((235)U/(238)U atom ratio and (234)U/(238)U activity ratio) in sediment samples. A two-stage sample cleanup using anion-exchange and TEVA extraction chromatography was employed in order to obtain accurate and precise (234)U/(238)U activity ratios. The factors that affect the accuracy and precision of U isotope ratio analysis, such as detector dead time, abundance sensitivity, dwell time and mass bias were carefully evaluated and corrected. With natural U, a precision lower than 0.5% R.S.D. for (235)U/(238)U atom ratio and lower than 2.0% R.S.D. for (234)U/(238)U activity ratio was obtained with less than 90 ng uranium. The developed analytical method was validated using an ocean sediment reference material and applied to an investigation into the uranium isotopic compositions in a sediment core in a brackish lake in the vicinity of U-related nuclear facilities in Japan.

  5. MCNP6 simulated performance of Micro-Pocket Fission Detectors (MPFDs) in the Transient REActor Test (TREAT) Facility

    DOE PAGES

    Reichenberger, Michael A.; Patel, Vishal K.; Roberts, Jeremy A.; ...

    2017-03-03

    Here, Micro-Pocket Fission Detectors (MPFDs) are under development for in-core neutron flux measurements at the Transient REActor Test facility (TREAT) and in other experiments at Idaho National Laboratory (INL). The sensitivity of MPFDs to the energy dependent neutron flux at TREAT has been determined for 0.0300-μm thick active material coatings of 242Pu, 232Th, natural uranium, and 93% enriched 235U. Self-shielding effects in the active material of the MPFD was also confirmed to be negligible. Finally, fission fragment energy deposition was found to be in conformance with previously reported results.

  6. Sharp change-over from compound nuclear fission to quasifission

    SciTech Connect

    Ghosh, T. K.; Banerjee, K.; Bhattacharya, C.; Bhattacharya, S.; Kundu, S.; Mali, P.; Meena, J. K.; Mukherjee, G.; Mukhopadhyay, S.; Rana, T. K.; Bhattacharya, P.; Golda, K. S.

    2009-05-15

    Fission fragment mass distributions have been measured from the decay of the compound nucleus {sup 246}Bk that has been populated via two entrance channels. These entrance channels have a slight difference in their mass asymmetries that puts them on either side of the Businaro Gallone mass asymmetry parameter. Both target nuclei were deformed. Near the Coulomb barrier, at similar excitation energies, the width of the fission fragment mass distribution was found to be drastically different for the {sup 14}N+{sup 232}Th reaction compared to the {sup 11}B+{sup 235}U reaction. The entrance channel mass asymmetry was found to affect the fusion process sharply.

  7. NUCLEAR DATA REVIEW

    SciTech Connect

    HOLDEN,N.E.

    2004-12-01

    Non-neutron nuclear data are periodically reviewed and evaluated. The recommended values are published in the Table of the Isotopes of the Chemical Rubber Company's Handbook of Chemistry and Physics. A 2004 review has begun to re-examine some data of interest to the International Union of Geological Sciences (IUGS) sub-commission on Geochronology dealing with radioactive decay constants and isotopic abundance ratios. Among the decay constants that are being evaluated are those of the following nuclides: {sup 40}K, {sup 87}Rb, {sup 138}La, {sup 147}Sm, {sup 176}Lu, {sup 174}Hf, {sup 187}Re, {sup 190}Pt, {sup 232}Th, {sup 235}U, {sup 238}U.

  8. Evaluation of {sup 235}U, {sup 238}U, {sup 6}Li, and {sup 27}Al Cross Sections

    SciTech Connect

    Chandler, J.R.

    2001-05-17

    Good nuclear data are essential for accurate prediction of reactor parameters. Several cross section libraries are currently available for use with GLASS physics calculations. In recent Mark 15 and Mark 22 studies, cross section data were developed to provide more accurate buckling calculations for Mark 15 and Mark 22 charges. This report documents evaluation of these new data for universal application.

  9. Utilization of a /sup 252/Cf-/sup 235/U fueled subcritical multiplier for neutron activation analysis. Rev

    SciTech Connect

    Wogman, N.A.; Lepel, E.A.

    1984-02-01

    A /sup 252/Cf neutron activation analysis facility developed in 1975 has been used for the routine multielement analysis of a wide variety of solid and liquid samples. The present neutron flux is on the order of 10/sup 9/ thermal neutrons per cm/sup 2/ per second. Following activation, the radioisotopes are analyzed through their photon emissions with lithium drifted germanium detectors, anticoincidence shielded germanium detectors and NaI(T1) coincidence spectrometers. Although over 65 elements have been measured in environmental materials with this system, typical analyses include the elements Na, Al, Cl, K, Ca, Ti, V, Mn, Br, Sr, Rb, Ba, and Dy. Detection limits range from the sub parts per million upward. Over 8000 samples have been analyzed at an amortized neutron cost per sample of $31.

  10. Determination of the 235U Mass and Enrichment within Small UF6 Cylinders via a Neutron Coincidence Well Counting System

    SciTech Connect

    McElroy, Robert Dennis; Croft, Dr. Stephen; Young, Brian M; Venkataraman, Ram

    2011-01-01

    The construction of three new uranium enrichment facilities in the United States has sparked renewed interest in the development and enhancement of methods to determine the enrichment and fissile mass content of UF6 cylinders. We describe the design and examine the expected performance of a UF6 bottle counter developed for the assay of Type 5A cylinders. The counter, as designed and subsequently constructed, is a tall passive neutron well counter with a clam-shell configuration and graphite end plugs operated in fast neutron mode. Factory performance against expectation is described. The relatively high detection efficiency and effectively 4 detection geometry provide a near-ideal measurement configuration, making the UF6 bottle counter a valuable tool for the evaluation of the neutron coincidence approach to UF6 cylinder assay. The impacts of non-uniform filling, voids, enrichment, and mixed enrichments are examined

  11. The Current State of Genetics Training in Psychiatric Residency: Views of 235 U.S. Educators and Trainees

    ERIC Educational Resources Information Center

    Hoop, Jinger G.; Savla, Gauri; Roberts, Laura Weiss; Zisook, Sidney; Dunn, Laura B.

    2010-01-01

    Objective: As researchers make progress in understanding genetic aspects of mental illness and its treatment, psychiatrists will increasingly need to understand and interpret genetic information specific to psychiatric disorders. Little is known about the extent to which residency programs are preparing psychiatrists for this new role. This study…

  12. U-Th-Ra disequilibria in sediments of the Dora Baltea river (Italia)

    NASA Astrophysics Data System (ADS)

    Chabaux, F.; Deloche, A.; Pelt, E.; Granet, M.; Perrone, Th.; Boutin, R.; Viville, D.; Rihs, S.; Stille, P.

    2012-04-01

    In order to constrain the transfer time of sediments in Alpine rivers, we propose to use the U-series nuclides approach recently developed for Himalayan rivers (e.g., Chabaux et al., 2008; Granet et al., 2010). Therefore, a series of bank sediments has beeen collected along the Dora Baltea river (Italia), one of the Po's tributaries draining the southern slope of the Mont Blanc Massif. In addition to U series nuclides, major and trace element concentrations and Sr and Nd isotope ratios have been analyzed for each sample. The study indicates that the (234U/238U)-, (230Th/234U)- and the (226Ra/230Th)- activity ratios are very similar for all the samples, whereas the 230Th/232Th ratios can differ from one sample to another. Such a variation, consistent with the Sr and Nd isotope data, is certainly the consequence of mineralogical heterogeneities in the samples. This suggests that the use of 238U-230Th-232Th systematics alone is probably insufficient for constraining the transfer time of sediments in the Po rivers alluvial plain, whereas the combination of 238U-230Th disequilibrium with the 230Th-226Ra disequilibrium can help to constrain such time information.

  13. HEU age determination

    SciTech Connect

    Moorthy, A.R.; Kato, W.Y.

    1995-08-01

    A technique has been developed to determine the Highly Enriched Uranium (HEU) Age which is defined as the time since the HEU was produced in an enrichment process. The HEU age is determined from the ratios of relevant uranium parents and their daughters viz {sup 230}Th/{sup 234}U and {sup 231}Pa/{sup 235}U. Uranium isotopes are quantitatively measured by their characteristic gammas and their daughters by alpha spectroscopy. In some of the samples where HEU is enriched more than 99%, the only mode of HEU age determination is by the measurement of {sup 231}Pa since there is negligible quantity of {sup 230}Th due to very low atom concentrations of {sup 234}U in the sample. In this paper we have presented data and methodology of finding the age of two HEU samples.

  14. Uranium-thorium isotope geochemistry of saline ground waters from central Missouri

    SciTech Connect

    Banner, J.L.; Chen, J.H.; Wasserburg, G.J.

    1989-03-01

    The isotopic and elemental distributions of uranium and thorium were examined in a suite of saline ground waters from central Missouri using mass spectrometric techniques. The waters were sampled from natural springs and artesian wells in Mississippian and Ordovician aquifers and have a wide range in salinity (5 to 26 /per thousand/), deltaD (/minus/108 to /minus/45 /per thousand/), and delta/sup 18/O (/minus/14.7 to /minus/6.5 /per thousand/) values. The suite of samples has a large range in /sup 238/U (50 to 200 x 10/sup /minus/12/g/g) and /sup 232/Th (0.3 to 9.1 x 10/sup /minus/12/g/g) concentrations and extremely high /sup 234/U//sup 238/U activity ratios ranging from 2.15 to 16.0. These isotopic compositions represent pronounced uranium-series disequilibrium compared with the value of modern seawater (1.15) or the equilibrium value (1.00). For such /sup 234/U-enriched waters, /sup 234/U//sup 238/U isotope ratios can be determined with a precision of /+-/ 10 /per thousand/ (2sigma) on 10 mL of sample and less than /+-/5 /per thousand/ on 100 mL. In contrast to the large /sup 234/U enrichments, /sup 230/Th//sup 238/U activity ratios in the ground waters are significantly lower than the equilibrium value. The more saline samples have markedly higher /sup 234/U//sup 238/U activity ratios and lower deltaD and delta/sup 18/O values. Unfiltered and filtered (< 0.1 ..mu..m) aliquots of a saline sample have the same isotopic composition and concentration of uranium, indicating uranium essentially occurs entirely as a dissolved species. The filtered/unfiltered concentration ratio for thorium in this sample is 0.29, demonstrating the predominant association of thorium with particulates.

  15. Total and spontaneous fission half-lives of the uranium and plutonium nuclides

    SciTech Connect

    Holden, N.E.

    1984-01-01

    The total half-life and the half-life for spontaneous fission are evaluated for the various long-lived nuclides of interest. Recommended values are presented for /sup 232/U, /sup 233/U, /sup 234/U, /sup 235/U, /sup 236/U, /sup 238/U, /sup 236/Pu, /sup 238/Pu, /sup 239/Pu, /sup 240/Pu, /sup 241/Pu, /sup 242/Pu, and /sup 244/Pu. The uncertainties are provided at the 95% confidence limit for each of the recommended values.

  16. UDATE1: A computer program for the calculation of uranium-series isotopic ages

    USGS Publications Warehouse

    Rosenbauer, R.J.

    1991-01-01

    UDATE1 is a FORTRAN-77 program with an interface for an Apple Macintosh computer that calculates isotope activities from measured count rates to date geologic materials by uranium-series disequilibria. Dates on pure samples can be determined directly by the accumulation of 230Th from 234U and of 231Pa from 235U. Dates for samples contaminated by clays containing abundant natural thorium can be corrected by the program using various mixing models. Input to the program and file management are made simple and user friendly by a series of Macintosh modal dialog boxes. ?? 1991.

  17. Electron spin resonance (ESR) dating of hominid-bearing deposits in the Caverna delle Fate, Ligure, Italy

    NASA Astrophysics Data System (ADS)

    Falgueres, Christophe; Yokoyama, Yuji; Bibron, Roland

    1990-07-01

    Stalagmitic floors interstratified with Mousterian deposits from the Caverna delle Fate (Italy) have been dated by the electron spin resonance (ESR) method. Three samples dated fall between 60,000 and 74,000 yr and indicate the age of the Mousterian deposits. They are in good agreement with ages determined by nondestructive γ-ray spectrometry of the human remains from 231Pa/ 235U and 230Th /234U ratios, which are, respectively, 75,000 -14,000+21,000 and 82,000 -25,000+36,000 yr. These dates are consistent with the morphological characteristics of the bones as Neanderthal remains.

  18. Radioactivity of cigarettes and the importance of (210)Po and thorium isotopes for radiation dose assessment due to smoking.

    PubMed

    Kubalek, Davor; Serša, Gregor; Štrok, Marko; Benedik, Ljudmila; Jeran, Zvonka

    2016-05-01

    Tobacco and tobacco smoke are very complex mixtures. In addition to various chemical and organic compounds they also contain natural radioactive elements (radionuclides). In this work, the natural radionuclide activity concentrations ((234)U, (238)U, (228)Th, (230)Th, (232)Th, (226)Ra, (210)Pb and (210)Po) of nine different cigarette samples available on the Slovenian market are reported. In addition to (210)Po, the transfer of thorium isotopes from a cigarette to a smoker's body and lungs have been determined for the first time. Cigarette smoke and exhaled air from smokers' lungs were collected from volunteer smokers (C-4 brand) to determinate what quantity of (210)Po and thorium isotopes is transferred from the tobacco to the smoker's lungs. Cigarette ash and smoked filters were also collected and analysed. Among the determined isotopes, (210)Pb and (210)Po showed the highest activity concentrations. During the smoking of one cigarette approximately 22% of (210)Po (and presumably its predecessor (210)Pb), 0.6% of (228)Th, 24% of (230)Th, and 31% of (232)Th are transferred from the cigarette and retained in the smoker's body. The estimated annual effective dose for smokers is 61 μSv/year from (210)Po; 9 μSv/year from (210)Pb; 6 μSv/year from (228)Th; 47 μSv/year from (230)Th, and 37 μSv/year from (232)Th. These results show the importance of thorium isotopes in contributing to the annual effective dose for smoking.

  19. The measurement of gamma-emitting radionuclides in beach sand cores of coastal regions of Ramsar, Iran using HPGe detectors.

    PubMed

    Tari, Marziyeh; Moussavi Zarandi, Sayyed Ali; Mohammadi, Kheirollah; Zare, Mohammad Reza

    2013-09-15

    Radionuclides which present in different beach sands are sources of external exposure that contribute to the total radiation exposure of human. (226)Ra, (235)U, (232)Th, (40)K and (137)Cs analysis has been carried out in sand samples collected at six depth levels, from eight locations of the northern coast of Iran, Ramsar, using high-resolution gamma-ray spectroscopy. The average Specific activities of natural radionuclides viz., (226)Ra, (235)U, (232)Th, (40)K and (137)Cs, in the 0-36 cm depth sand were found as: 19.2±0.04, 2.67±0.17, 17.9±0.06, 337.5±0.61 and 3.35±0.12 Bq kg(-1), respectively. The effects of organic matter content and pH value of sand samples on the natural radionuclide levels were also investigated. Finally, the measured radionuclide concentrations in the Ramsar beach were compared with the world average values, as reported by UNSCEAR (2000). None of the studied beaches were considered as a radiological risk.

  20. Distribution of naturally occurring radioactivity and ¹³⁷Cs in the marine sediment of Farasan Island, southern Red Sea, Saudi Arabia.

    PubMed

    Al-Zahrany, A A; Farouk, M A; Al-Yousef, A A

    2012-11-01

    The present work is a part of a project dedicated to measure the marine radioactivity near the Saudi Arabian coasts of the Red Sea and Arabian Gulf for establishing a marine radioactivity database, which includes necessary information on the background levels of both naturally occurring and man-made radionuclides in the marine environment. Farasan Islands is a group of 84 islands (archipelago), under the administration of the Kingdom of Saudi Arabia, in the Red Sea with its main island of Farasan, which is 50 km off the coast of Jazan City. The levels of natural radioactivity of (238)U, (235)U, (226)Ra, (232)Th and (40)K and man-made radionuclides such as (137)Cs in the grab sediment and water samples around Farasan Island have been measured using gamma-ray spectroscopy. The average activity concentrations of (238)U, (235)U, (226)Ra, (232)Th, (40)K and (137)Cs in the sediment samples were found to be 35.46, 1.75, 3.31, 0.92, 34.34 and 0.14 Bq kg(-1), respectively.

  1. Simulated (n,f) cross section of isomeric 235m-U

    SciTech Connect

    Becker, J; Britt, H; Younes, W

    2003-12-18

    The neutron-induced fission cross section on the {sup 235}U, T{sub 1/2} {approx} 26 min isomer has been deduced for incident neutron energies in the range E{sub n}=0.1-2.5 MeV, using the surrogate-reaction technique. In this technique, {sup 236}U fission probabilities measured in the {sup 234}U(t, pf) reaction have been converted into {sup 235}U(n,f) and {sup 235m}U(n,f) cross sections, using reaction theory to compensate for the differences in angular-momentum and parity distributions in the fissioning systems, transferred by the (t,p) and neutron-induced reactions. Based on the comparison between the {sup 235}U(n,f) cross section extracted in this work and independent experimental data, the deduced {sup 235m}U(n,f) cross section is believed to be reliable to 20% below E{sub n} {approx} 0.5 MeV and 10% at higher energies. The surrogate-reaction technique, its validation in the case of the {sup 235}U(n,f) cross section, and the deduced {sup 235m}U(n,f) cross section are discussed. Validation of this method allows (n,f) cross sections for many short-lived nuclei, as well as isomeric nuclei, to be extracted from measured fission probabilities.

  2. Uranium-series dating of pedogenic silica and carbonate, Crater Flat, Nevada

    USGS Publications Warehouse

    Ludwig, K. R.; Paces, J.B.

    2002-01-01

    A 230Th-234U-238U dating study on pedogenic silica-carbonate clast rinds and matrix laminae from alluvium in Crater Flat, Nevada was conducted using small-sample thermal-ionization mass spectrometry (TIMS) analyses on a large suite of samples. Though the 232Th content of these soils is not particularly low (mostly 0.1-9 ppm), the high U content of the silica component (mostly 4-26 ppm) makes them particularly suitable for 230Th/U dating on single, 10 to 200 mg totally-digested samples using TIMS. We observed that (1) both micro- (within-rind) and macro-stratigraphic (mappabe deposit) order of the 230Th/U ages were preserved in all cases; (2) back-calculated initial 234U/238U fall in a restricted range (typically 1.67??0.19), so that 234U/238U ages with errors of about 100 kyr (2??) could be reliably determined for the oldest, 400 to 1000 ka rinds: and (3) though 13 of the samples were >350 ka, only three showed evidence for an open-system history, even though the sensitivity of such old samples to isotopic disruption is very high. An attempt to use leach-residue techniques to separate pedogenic from detrital U and Th failed, yielding corrupt 230Th/U ages. We conclude that 230Th/U ages determined from totally dissolved, multiple sub-mm size subsamples provide more reliable estimates of soil chronology than methods employing larger samples, chemical enhancement of 238U/232Th, or isochrons. Copyright ?? 2002 Elsevier Science Ltd.

  3. Large Scale Accelerator Production of 225Ac: Effective Cross sections for 78-192 MeV Protons Incident on 232Th Targets

    DOE PAGES

    Griswold, Justin R; Medvedev, Dmitri G.; Engle, Jonathan W.; ...

    2016-09-28

    Actinium-225 and 213Bi have been used successfully in targeted alpha therapy (TAT) in preclinical and clinical research. This paper is a continuation of research activities aiming to expand the availability of 225Ac. The high energy proton spallation reaction on natural thorium metal target has been utilized to produce millicurie quantities of 225Ac. The results of sixteen irradiation experiments of Th metal at beam energies between 78 and 200 MeV are summarized in this work. Irradiations have been conducted at Brookhaven National Laboratory (BNL) and Los Alamos National Laboratory (LANL), while target dissolution and processing was carried out at Oak Ridgemore » National Laboratory (ORNL). Excitation functions for actinium and thorium isotopes as well as for some of the fission products are presented. The cross sections for production of 225Ac range from 3.6 to 16.7 mb in the incident proton energy range of 78 to 192 MeV. Based on these data, production of Curie quantities of 225Ac is possible by irradiating a 5.0 g cm-2232Th target for 10 days in either BNL or LANL proton irradiation facilities.« less

  4. Preliminary Results on Direct Observation of True Ternary fission in the reaction {sup 232}Th+d (10 MeV)

    SciTech Connect

    Pyatkov, Yu.; Kamanin, D.; Alexandrov, A.; Alexandrova, I.; Kondratyev, N.; Kuznetsova, E.; Tyukavkin, A.; Zhuchko, V.; Krasznohorkay, A.; Csatlos, M.; Csige, L.; Gulyas, J.; Naqvi, F.; Tornyi, T.

    2010-04-30

    Results of the first direct observation of the true ternary fission of {sup 234}Pa* nucleus are presented. The yield of the effect depending of the experimental geometry is about 10{sup -5}/binary fission. Mass of the lightest fragment in the triplet lies mainly in the range of (20 divide 40) a.m.u. Connection between the effect and known heavy ion or lead radioactivity is discussed.

  5. Radioactivity in honey of the central Italy.

    PubMed

    Meli, Maria Assunta; Desideri, Donatella; Roselli, Carla; Feduzi, Laura; Benedetti, Claudio

    2016-07-01

    Natural radionuclides and (137)Cs in twenty seven honeys produced in a region of the Central Italy were determined by alpha ((235)U, (238)U, (210)Po, (232)Th and (228)Th) and gamma spectrometry ((137)Cs, (40)K, (226)Ra and (228)Ra). The study was carried out in order to estimate the background levels of natural ((40)K, (238)U and (232)Th and their progeny) and artificial radionuclides ((137)Cs) in various honey samples, as well as to compile a data base for radioactivity levels in that region. (40)K showed a mean activity of 28.1±23.0Bqkg(-1) with a range of 7.28-101Bqkg(-1). The mean of (210)Po activity resulted 0.40±0.46Bqkg(-1) with a range of 0.03-1.98Bqkg(-1). The mean of (238)U activity resulted 0.020±0.010Bqkg(-1). (226)Ra and (228)Ra resulted always <0.34 and <0.57Bqkg(-1) respectively, (235)U, (228)Th and (232)Th were always <0.007Bqkg(-1). (137)Cs resulted <0.10Bqkg(-1) in all samples. The committed effective doses due to (210)Po from ingestion of honey for infants, children and adults account for 0.002-5.13% of the natural radiation exposure in Italy. The honeys produced in Central Italy were of good quality in relation to the studied parameters, confirming the general image of a genuine and healthy food associated to this traditional products.

  6. Direct uranium isotope ratio analysis of single micrometer-sized glass particles

    PubMed Central

    Kappel, Stefanie; Boulyga, Sergei F.; Prohaska, Thomas

    2012-01-01

    We present the application of nanosecond laser ablation (LA) coupled to a ‘Nu Plasma HR’ multi collector inductively coupled plasma mass spectrometer (MC-ICP-MS) for the direct analysis of U isotope ratios in single, 10–20 μm-sized, U-doped glass particles. Method development included studies with respect to (1) external correction of the measured U isotope ratios in glass particles, (2) the applied laser ablation carrier gas (i.e. Ar versus He) and (3) the accurate determination of lower abundant 236U/238U isotope ratios (i.e. 10−5). In addition, a data processing procedure was developed for evaluation of transient signals, which is of potential use for routine application of the developed method. We demonstrate that the developed method is reliable and well suited for determining U isotope ratios of individual particles. Analyses of twenty-eight S1 glass particles, measured under optimized conditions, yielded average biases of less than 0.6% from the certified values for 234U/238U and 235U/238U ratios. Experimental results obtained for 236U/238U isotope ratios deviated by less than −2.5% from the certified values. Expanded relative total combined standard uncertainties Uc (k = 2) of 2.6%, 1.4% and 5.8% were calculated for 234U/238U, 235U/238U and 236U/238U, respectively. PMID:22595724

  7. The radiological impact of phosphogypsum stockpile in Wiślinka (northern Poland) on the Martwa Wisła river water.

    PubMed

    Olszewski, Grzegorz; Boryło, Alicja; Skwarzec, Bogdan

    The aim of this work was to determine the concentrations of uranium ((234)U, (235)U, (238)U), polonium ((210)Po) and lead ((210)Pb) radioisotopes in water samples and to explore the impact of the phosphogypsum stack on the Martwa Wisła waters. The (238)U, (210)Po and (210)Pb concentrations in analyzed water samples reached maximum values of 11.7 ± 0.3, 2.0 ± 0.1 and 3.2 ± 0.1 mBq L(-1) and activity ratios were maximally 1.18 ± 0.01 for (234)U/(238)U, 0.041 ± 0.018 for (235)U/(238)U and 0.69 ± 0.10 for (210)Po/(210)Pb. The obtained results suggest that this impact is rather insignificant and does not affect significantly the Martwa Wisła river.

  8. Measurement of Uranium Isotope Ratios in Keratinous Materials: A Noninvasive Bioassay for Special Nuclear Material.

    PubMed

    Brockman, John D; Brown, John W N; Morrell, Jonathan S; Robertson, J David

    2016-09-06

    Hair, toenail, and fingernail are noninvasive, integrative biological monitors routinely used to assess mineral intake.1-4 In this study, we demonstrate the feasibility of distinguishing between exposure to natural, depleted, and enriched U by measuring the (235)U/(238)U, (234)U/(238)U, and (236)U/(238)U ratios in the hair, fingernails, and toenails of occupationally exposed workers and control volunteers. The exposure history of cases and controls to non-natural U was assessed through voluntary self-reporting using a simple questionnaire. The measured U isotope ratios and U concentration in the hair, toenail, and fingernail of cases were compared to a nonexposed control group. No difference was observed in the uranium concentration between the two groups. Significant differences between the cases and the control group were observed in the (235)U/(238)U and (236)U/(238)U isotope ratios but not the (234)U/(238)U. This is the first time that hair, fingernail, and toenail have been demonstrated to be sensitive to occupational exposure to enriched and depleted U, a result with significant implications for proliferation compliance monitoring.

  9. Spectral interference corrections for the measurement of (238)U in materials rich in thorium by a high resolution gamma-ray spectrometry.

    PubMed

    Yücel, H; Solmaz, A N; Köse, E; Bor, D

    2009-11-01

    In this study, the spectral interferences are investigated for the analytical peaks at 63.3 keV of (234)Th and 1001.0 keV of (234m)Pa, which are often used in the measurement of (238)U activity by the gamma-ray spectrometry. The correction methods are suggested to estimate the net peak areas of the gamma-rays overlapping the analytical peaks, due to the contribution of (232)Th that may not be negligible in materials rich in natural thorium. The activity results for the certified reference materials (CRMs) containing U and Th were measured with a well type Ge detector. The self-absorption and true coincidence-summing (TCS) effects were also taken into account in the measurements. It is found that ignoring the contributions of the interference gamma-rays of (232)Th and (235)U to the mixed peak at 63.3 keV of (234)Th ((238)U) leads to the remarkably large systematic influence of 0.8-122% in the measured (238)U activity, but in case of ignoring the contribution of (232)Th via the interference gamma-ray at 1000.7 keV of (228)Ac to the mixed peak at 1001 keV of (234m)Pa ((238)U) results in relatively smaller systematic influence of 0.05-3%, depending on thorium contents in the samples. The present results showed that the necessary correction for the spectral interferences besides self-absorption and TCS effects is also very important to obtain more accurate (238)U activity results. Additionally, if one ignores the contribution of (232)Th to both (238)U and (40)K activities in materials, the maximum systematic influence on the effective radiation dose is estimated to be ~6% and ~1% via the analytical peaks at 63.3 and 1001 keV for measurement of the (238)U activity, respectively.

  10. Non-destructive Assay Measurements Using the RPI Lead Slowing Down Spectrometer

    SciTech Connect

    Becker, Bjorn; Weltz, Adam; Kulisek, Jonathan A.; Thompson, J. T.; Thompson, N.; Danon, Yaron

    2013-10-01

    The use of a Lead Slowing-Down Spectrometer (LSDS) is consid- ered as a possible option for non-destructive assay of fissile material of used nuclear fuel. The primary objective is to quantify the 239Pu and 235U fissile content via a direct measurement, distinguishing them through their characteristic fission spectra in the LSDS. In this pa- per, we present several assay measurements performed at the Rensse- laer Polytechnic Institute (RPI) to demonstrate the feasibility of such a method and to provide benchmark experiments for Monte Carlo cal- culations of the assay system. A fresh UOX fuel rod from the RPI Criticality Research Facility, a 239PuBe source and several highly en- riched 235U discs were assayed in the LSDS. The characteristic fission spectra were measured with 238U and 232Th threshold fission cham- bers, which are only sensitive to fission neutron with energy above the threshold. Despite the constant neutron and gamma background from the PuBe source and the intense interrogation neutron flux, the LSDS system was able to measure the characteristic 235U and 239Pu responses. All measurements were compared to Monte Carlo simula- tions. It was shown that the available simulation tools and models are well suited to simulate the assay, and that it is possible to calculate the absolute count rate in all investigated cases.

  11. Comparison of measured and calculated uranium isotopic concentrations in cascade streams at the Paducah Gaseous Diffusion Plant

    SciTech Connect

    Blumkin, S.

    1982-06-16

    A test has been performed at the Paducah Gaseous Diffusion Plant (PGDP) in connection with studies for the US Arms Control and Disarmament Agency on the possibility of utilizing measurements of the concentrations of the minor uranium isotopes in /sup 235/U enrichment cascade external streams as a safeguards technique (MIST). This is the fourth plant test that has been performed in connection with the MIST studies, the first three having been done at the Oak Ridge Gaseous Diffusion Plant (ORGDP). The main objectives of the test were to measure the isotopic composition and flow rates of the plant external streams over a period of time; to design an appropriate plant model in the manner an IAEA safeguards team might do it and calculate the isotopic compositions of the plant streams; and to compare the calculated isotopic values with the measured ones. The calculated /sup 235/U to /sup 234/U concentration ratios in the product and tails streams did not match the average measured values in the high-power period as well as they did for the low-power period, when the same isotopic composition for natural U was assumed at both power levels - the actual composition of the natural U fed to the plant during the test not having been measured. Recalculation of the /sup 235/U to /sup 234/U concentrations with another assumed value for the /sup 234/U concentration in natural U, that is still within the range of reported observed values for it, resulted in better agreement with the measured plant stream values: + 0.7% for the product stream and + 0.2% in the tails stream for the single-cascade model and + 0.8% and - 0.7% respectively for a two-cascade plant model. The record on sources of the natural U that was fed during the test supports the assumption that the average /sup 234/U concentration in the natural U fed was probably different during the two operating periods.

  12. Separation Of Uranium And Plutonium Isotopes For Measurement By Multi Collector Inductively Coupled Plasma Mass Spectroscopy

    SciTech Connect

    Martinelli, R E; Hamilton, T F; Williams, R W; Kehl, S R

    2009-03-29

    Uranium (U) and plutonium (Pu) isotopes in coral soils, contaminated by nuclear weapons testing in the northern Marshall Islands, were isolated by ion-exchange chromatography and analyzed by mass spectrometry. The soil samples were spiked with {sup 233}U and {sup 242}Pu tracers, dissolved in minerals acids, and U and Pu isotopes isolated and purified on commercially available ion-exchange columns. The ion-exchange technique employed a TEVA{reg_sign} column coupled to a UTEVA{reg_sign} column. U and Pu isotope fractions were then further isolated using separate elution schemes, and the purified fractions containing U and Pu isotopes analyzed sequentially using multi-collector inductively coupled plasma mass spectrometer (MCICP-MS). High precision measurements of {sup 234}U/{sup 235}U, {sup 238}U/{sup 235}U, {sup 236}U/{sup 235}U, and {sup 240}Pu/{sup 239}Pu in soil samples were attained using the described methodology and instrumentation, and provide a basis for conducting more detailed assessments of the behavior and transfer of uranium and plutonium in the environment.

  13. Isotopic Analysis of Uranium in NIST SRM Glass by Femtosecond Laser Ablation

    SciTech Connect

    Duffin, Andrew M.; Hart, Garret L.; Hanlen, Richard C.; Eiden, Gregory C.

    2013-05-19

    We employed femtosecond Laser Ablation Multicollector Inductively Coupled Mass Spectrometry for the 11 determination of uranium isotope ratios in a series of standard reference material glasses (NIST 610, 612, 614, and 12 616). This uranium concentration in this series of SRM glasses is a combination of isotopically natural uranium in 13 the materials used to make the glass matrix and isotopically depleted uranium added to increase the uranium 14 elemental concentration across the series. Results for NIST 610 are in excellent agreement with literature values. 15 However, other than atom percent 235U, little information is available for the remaining glasses. We present atom 16 percent and isotope ratios for 234U, 235U, 236U, and 238U for all four glasses. Our results show deviations from the 17 certificate values for the atom percent 235U, indicating the need for further examination of the uranium isotopes in 18 NIST 610-616. Our results are fully consistent with a two isotopic component mixing between the depleted 19 uranium spike and natural uranium in the bulk glass.

  14. Protactinium and isotopes of thorium in metalliferous sediments from the Bauer depression

    SciTech Connect

    Arslanov, K.A.; Kuznetsov, V.Yu.; Lokshin, N.V.; Pospelov, Yu.N.

    1989-01-01

    Results are presented of a study of the vertical distribution of /sup 238/U, /sup 234/U, /sup 232/Th, /sup 230/Th, and /sup 231/Pa isotopes in a column of metalliferous sediments from the Bauer depression (southeastern part of the Pacific Ocean). On the basis of the obtained data a hypothesis is formulated concerning the authigenic production of /sup 230/Th and /sup 231/Pa in these deposits, i.e, the similarity of the physicochemical behavior of /sup 230/Th and /sup 231/Pa found in pelagic sediments is found in these specific sediments also. We present arguments in favor of the identical behavior of these radionuclides in the marine environment. With the help of the ionium method of dating marine sediments, the average rate of sedimentation of the investigated column of metalliferous sediments from the Bauer depression was calculated.

  15. A database of radionuclide activity and metal concentrations for the Alligator Rivers Region uranium province.

    PubMed

    Doering, Che; Bollhöfer, Andreas

    2016-10-01

    This paper presents a database of radionuclide activity and metal concentrations for the Alligator Rivers Region (ARR) uranium province in the Australian wet-dry tropics. The database contains 5060 sample records and 57,473 concentration values. The data are for animal, plant, soil, sediment and water samples collected by the Environmental Research Institute of the Supervising Scientist (ERISS) as part of its statutory role to undertake research and monitoring into the impacts of uranium mining on the environment of the ARR. Concentration values are provided in the database for 11 radionuclides ((227)Ac, (40)K, (210)Pb, (210)Po, (226)Ra, (228)Ra, (228)Th, (230)Th, (232)Th, (234)U, (238)U) and 26 metals (Al, As, Ba, Ca, Cd, Co, Cr, Cu, Fe, Hg, K, Mg, Mn, Na, Ni, P, Pb, Rb, S, Sb, Se, Sr, Th, U, V, Zn). Potential uses of the database are discussed.

  16. Uranium series isotopes concentration in sediments at San Marcos and Luis L. Leon reservoirs, Chihuahua, Mexico

    NASA Astrophysics Data System (ADS)

    Méndez-García, C.; Renteria-Villalobos, M.; García-Tenorio, R.; Montero-Cabrera, M. E.

    2014-07-01

    Spatial and temporal distribution of the radioisotopes concentrations were determined in sediments near the surface and core samples extracted from two reservoirs located in an arid region close to Chihuahua City, Mexico. At San Marcos reservoir one core was studied, while from Luis L. Leon reservoir one core from the entrance and another one close to the wall were investigated. 232Th-series, 238U-series, 40K and 137Cs activity concentrations (AC, Bq kg-1) were determined by gamma spectrometry with a high purity Ge detector. 238U and 234U ACs were obtained by liquid scintillation and alpha spectrometry with a surface barrier detector. Dating of core sediments was performed applying CRS method to 210Pb activities. Results were verified by 137Cs AC. Resulting activity concentrations were compared among corresponding surface and core sediments. High 238U-series AC values were found in sediments from San Marcos reservoir, because this site is located close to the Victorino uranium deposit. Low AC values found in Luis L. Leon reservoir suggest that the uranium present in the source of the Sacramento - Chuviscar Rivers is not transported up to the Conchos River. Activity ratios (AR) 234U/overflow="scroll">238U and 238U/overflow="scroll">226Ra in sediments have values between 0.9-1.2, showing a behavior close to radioactive equilibrium in the entire basin. 232Th/overflow="scroll">238U, 228Ra/overflow="scroll">226Ra ARs are witnesses of the different geological origin of sediments from San Marcos and Luis L. Leon reservoirs.

  17. Determination of 238u/235u, 236u/238u and uranium concentration in urine using sf-icp-ms and mc-icp-ms: an interlaboratory comparison.

    PubMed

    Parrish, Randall R; Thirlwall, Matthew F; Pickford, Chris; Horstwood, Matthew; Gerdes, Axel; Anderson, James; Coggon, David

    2006-02-01

    Accidental exposure to depleted or enriched uranium may occur in a variety of circumstances. There is a need to quantify such exposure, with the possibility that the testing may post-date exposure by months or years. Therefore, it is important to develop a very sensitive test to measure precisely the isotopic composition of uranium in urine at low levels of concentration. The results of an interlaboratory comparison using sector field (SF)-inductively coupled plasma-mass spectrometry (ICP-MS) and multiple collector (MC)-ICP-MS for the measurement of uranium concentration and U/U and U/U isotopic ratios of human urine samples are presented. Three urine samples were verified to contain uranium at 1-5 ng L and shown to have natural uranium isotopic composition. Portions of these urine batches were doped with depleted uranium (DU) containing small quantities of U, and the solutions were split into 100 mL and 400 mL aliquots that were subsequently measured blind by three laboratories. All methods investigated were able to measure accurately U/U with precisions of approximately 0.5% to approximately 4%, but only selected MC-ICP-MS methods were capable of consistently analyzing U/U to reasonable precision at the approximately 20 fg L level of U abundance. Isotope dilution using a U tracer demonstrates the ability to measure concentrations to better than +/-4% with the MC-ICP-MS method, though sample heterogeneity in urine samples was shown to be problematic in some cases. MC-ICP-MS outperformed SF-ICP-MS methods, as was expected. The MC-ICP-MS methodology described is capable of measuring to approximately 1% precision the U/U of any sample of human urine over the entire range of uranium abundance down to <1 ng L, and detecting very small amounts of DU contained therein.

  18. Multi Proxy Reconstruction (δ98/95Mo, δ238/235U) of Global Ocean Oxygenation during the Early Eocene

    NASA Astrophysics Data System (ADS)

    Bagard, M. L.; Davies, M. K.; Dickson, A.; Cohen, A. S.

    2014-12-01

    Early Eocene climate is characterised by extreme and persistent warmth punctuated by abrupt global warming events ('hyperthermals'), such as the Paleocene-Eocene Thermal Maximum (PETM, ~56 Ma ago), when global temperatures became even warmer. These hyperthermals were associated with perturbations to the global carbon cycle that would have had a profound effect on the distribution of O2in the oceans. However, the timing and extent of any fluctuations in global ocean oxygenation during these events are still poorly constrained. In this study, we investigate how seawater oxygen levels responded to environmental changes in the early Eocene by determining the Mo and U stable isotope compositions of anoxic sediments from the Arctic Ocean obtained by the Integrated Ocean Drilling Program Expedition 302. It has previously been shown that these two isotope systems each respond to changes in seawater oxygen levels and that they may be used to reconstruct the extent of global marine anoxia in Earth's past. Furthermore, since Mo and U have different residence times in the oceans and their isotope fractionations display different sensitivities to dissolved oxygen concentrations, the use of both proxies enables us to estimate past changes in seawater oxygenation with greater confidence. By combining the information provided by these two isotope systems, we are able to better constrain the onset and the severity of the episodes of seawater anoxia during the Eocene, thereby allowing us to better understand the Earth processes that control ocean oxygenation levels.

  19. Calculation of K{sub {infinity}} for homogeneous {sup 235}U metal mixtures: Will the real K{sub {infinity}} please stand up?

    SciTech Connect

    Jordan, W.C.; Petrie, L.M.; Wright, R.Q.; Parks, C.V.

    1997-06-01

    This paper very briefly analyzes a journal article about calculating k{sub {infinity}} for metals mixed with uranium 235, and compares the article results with other calculation methods. The article suggested that continuous energy cross sections gave more accurate results than groupwise cross sections. The mixtures described in the article were dry, fast systems with several unusual characteristics; however, the majority of multigroup libraries used for analysis were developed for well moderated thermal systems. The results of calculations performed using several different codes and cross sections for three uranium/metal mixtures are presented in this paper. 1 tab.

  20. Determination of (235)U, (239)Pu, (240)Pu, and (241)Am in a nuclear bomb particle using a position-sensitive α-γ coincidence technique.

    PubMed

    Peräjärvi, Kari A; Ihantola, Sakari; Pöllänen, Roy C; Toivonen, Harri I; Turunen, Jani A

    2011-02-15

    A nuclear bomb particle containing 1.6 ng of Pu was investigated nondestructively with a position-sensitive α detector and a broad-energy HPGe γ-ray detector. An event-mode data acquisition system was used to record the data. α-γ coincidence counting was shown to be well suited to nondestructive isotope ratio determination. Because of the very small background, the 51.6 keV γ rays of (239)Pu and the 45.2 keV γ rays of (240)Pu were identified, which enabled isotopic ratio calculations. In the present work, the (239)Pu/((239)Pu+(240)Pu) atom ratio was determined to be 0.950 ± 0.010. The uncertainties were much smaller than in the previous more conventional nondestructive studies on this particle. Obtained results are also in good agreement with the data from the destructive mass spectrometric studies obtained previously by other investigators.

  1. Reactivity measurements on an experimental assembly of 4. 31 wt % sup 235 U enriched UO sub 2 fuel rods arranged in a shipping cask geometry

    SciTech Connect

    Bierman, S.R.

    1989-10-01

    A research program was initiated for the US Department of Energy (DOE) Sandia National Laboratory Transportation Systems Development Department in 1982 to provide benchmark type experimental criticality data in support of the design and safe operations of nuclear fuel transportation systems. The overall objective of the program is to identify and provide the experimental data needed to form a consistent, firm, and complete data base for verifying calculational models used in the criticality analyses of nuclear transport and related systems. A report, PNL-6205, issued in June 1988 (Bierman 1988) covered measurement results obtained from a series of experimental assemblies (TIC-1, 2, 3 and 4) involving neutron flux traps. The results obtained on a fifth experimental assembly (TIC-5), modeled after a calculational problem of the Organization for Economic Cooperation and Development (OECD) Nuclear Energy Agency (NEA) Committee on the Safety of Nuclear Installations (CSNI) Working Group, are covered in this report. 10 refs., 10 figs., 7 tabs.

  2. Geochronology and petrogenesis of MORB from the Juan de Fuca and Gorda ridges by 238U230Th disequilibrium

    USGS Publications Warehouse

    Goldstein, S.J.; Murrell, M.T.; Janecky, D.R.; Delaney, J.R.; Clague, D.A.

    1991-01-01

    A highly precise mass spectrometric method of analysis was used to determine 238U234U230Th232Th in axial and off-axis basalt glasses from Juan de Fuca (JDF) and Gorda ridges. Initial 230Th activity excesses in the axial samples range from 3 to 38%, but generally lie within a narrow range of 12 to 15%. Secondary alteration effects were evaluated using ??234U and appear to be negligible; hence the 230Th excesses are magmatic in origin. Direct dating of MORB was accomplished by measuring the decrease in excess 230Th in off-axis samples. 238U230Th ages progressively increase with distance from axis. Uncertainties in age range from 10 to 25 ka for UTh ages of 50 to 200 ka. The full spreading rate based on UTh ages for Endeavour segment of JDF is 5.9 ?? 1/2 cm/yr, with asymmetry in spreading between the Pacific (4.0 ?? 0.6 cm/yr) and JDF (1.9 ?? 0.6 cm/yr) plates. For northern Gorda ridge, the half spreading rate for the JDF plate is found to be 3.0 ?? 0.4 cm/yr. These rates are in agreement with paleomagnetic spreading rates and topographic constraints. This suggests that assumptions used to determine ages, including constancy of initial 230Th 232Th ratio over time, are generally valid for the areas studied. Samples located near the axis of spreading are typically younger than predicted by these spreading rates, which most likely reflects recent volcanism within a 1-3 km wide zone of crustal accretion. Initial 230Th/232Th ratios and 230Th activity were also used to examine the recent Th/U evolution and extent of melting of mantle sources beneath these ridges. A negative anomaly in 230Th 232Th for Axial seamount lavas provides the first geochemical evidence of a mantle plume source for Axial seamount and the Cobb-Eickelberg seamount chain and indicates recent depletion of other JDF segment sources. Large 230Th activity excesses for lavas from northern Gorda ridge and Endeavour segment indicate formation from a lower degree of partial melting than other segments. An

  3. Elemental bio-imaging of thorium, uranium, and plutonium in tissues from occupationally exposed former nuclear workers.

    PubMed

    Hare, Dominic; Tolmachev, Sergei; James, Anthony; Bishop, David; Austin, Christine; Fryer, Fred; Doble, Philip

    2010-04-15

    Internal exposure from naturally occurring radionuclides (including the inhaled long-lived actinides (232)Th and (238)U) is a component of the ubiquitous background radiation dose (National Council on Radiation Protection and Measurements. Ionizing radiation exposure of the population of the United States; NCRP Report No. 160; NCRP: Bethesda, MD, 2009). It is of interest to compare the concentration distribution of these natural alpha-emitters in the lungs and respiratory lymph nodes with those resulting from occupational exposure, including exposure to anthropogenic plutonium and depleted and enriched uranium. This study examines the application of laser ablation-inductively coupled plasma-mass spectrometry (LA-ICPMS) to quantifying and visualizing the mass distribution of uranium and thorium isotopes from both occupational and natural background exposure in human respiratory tissues and, for the first time, extends this application to the direct imaging of plutonium isotopes. Sections of lymphatic and lung tissues taken from deceased former nuclear workers with a known history of occupational exposure to specific actinide elements (uranium, plutonium, or americium) were analyzed by LA-ICPMS. Using a previously developed LA-ICPMS protocol for elemental bio-imaging of trace elements in human tissue and a new software tool, we generated images of thorium ((232)Th), uranium ((235)U and (238)U), and plutonium ((239)Pu and (240)Pu) mass distributions in sections of tissue. We used a laboratory-produced matrix-matched standard to quantify the (232)Th, (235)U, and (238)U concentrations. The plutonium isotopes (239)Pu and (240)Pu were detected by LA-ICPMS in 65 mum diameter localized regions of both a paratracheal lymph node and a sample of lung tissue from a person who was occupationally exposed to refractory plutonium (plutonium dioxide). The average (overall) (239)Pu concentration in the lymph node was 39.2 ng/g, measured by high purity germanium (HPGe) gamma

  4. Radioactivity In Marine Organisms From Northeast Atlantic Ocean

    SciTech Connect

    Carvalho, Fernando P.; Oliveira, Joao M.

    2008-08-07

    Naturally-occurring radionuclides such as {sup 238}U, {sup 234}U, {sup 230}Th, {sup 226}Ra, {sup 210}Po, {sup 210}Pb and {sup 232}Th, and artificial radionuclides such as {sup 137}Cs, {sup 239+240}Pu and {sup 241}Am, were measured in a large number of marine species. In common fish species, typical concentrations of {sup 210}Po ranged from 10{sup 2} to 10{sup 4} mBq kg{sup -1} (wet weight), {sup 226}Ra concentrations ranged from 1x10{sup 2} to 5xl0{sup 2} mBq kg{sup -1}, {sup 238}U was at about 10 mBq kg{sup -1} and {sup 232}Th at about 0.5 mBq kg{sup -1}. Radiation doses to marine organisms originated by naturally-occurring and artificial radionuclides accumulated in tissues and by external radiation sources were computed and compared. Internal sources generally give higher contribution to the absorbed radiation dose than external sources. Amongst radionuclides accumulated in fish muscle and acting as internal radiation sources, natural {sup 210}Po and {sup 40}K give the largest contribution to the absorbed radiation dose, while artificial radionuclides such as {sup 137}Cs and {sup 239+240}Pu contribute with less than 0.5% to the absorbed radiation dose from all internal sources.

  5. U-series Disequilibria in Continental Arcs: NE Japan Case

    NASA Astrophysics Data System (ADS)

    Tepley, F. J.; Gill, J. B.; Williams, R. W.

    2005-12-01

    Basalts and andesites from continental arcs typically are close to equilibrium between (238U) and (230Th), and have subdued excesses of 226Ra compared to oceanic arcs (Turner et al., 2003). There is ambiguity whether these and other geochemical features derive from subducted sediment, subcontinental lithosphere, or the crust. We report new 238U-234U-230Th-226Ra data for 20 historical to Holocene samples from Asama in the south of NE Japan to Tarumai in the north. Most straddle the equiline with <5% excess U or Th, yet have 10-60% excess 226Ra. The only significant excess U occurs at Usu and Iwaki in the north where it correlates with higher (230Th)/(232Th) as in other arcs (e.g., Mariana). Otherwise (230Th)/(232Th) ratios are 0.75-1.05 which is less than in the surrounding Izu and Kurile oceanic arcs. Most ratios <0.95 are associated with trace element evidence of crustal contamination that drags samples down the equiline. The exception is Iwate where Th/U ratios are ~4.0 even in depleted basalts. Excess 226Ra is greater in basalts than andesites. The excess 226Ra, plus elevated 10Be and Th, is attributed to ubiquitous slab inputs that are overprinted by even higher Th contents from a crustal source with Th/U >4.

  6. Corrigendum to "A redox-stratified ocean 3.2 billion years ago" [Earth Planet. Sci. Lett. 430 (2015) 43-53

    NASA Astrophysics Data System (ADS)

    Satkoski, Aaron M.; Beukes, Nicolas J.; Li, Weiqiang; Beard, Brian L.; Johnson, Clark M.

    2017-02-01

    The authors have discovered a calculation error in the concentration data for U, Th and Pb. This error does not affect any measured isotopic compositions: 206Pb/204Pb, 207Pb/204Pb, 238U/204Pb, 232Th/204Pb, and 235U/204Pb; these all remain the same. None of the Fe isotope data are affected. Hence, none of the conclusions for open or closed-system U-Th-Pb behavior are affected, nor the conclusions of a redox gradient between shallow- and deep-water U contents. The magnitude of the shallow- and deep-water U content contrast remains the same, where U contents in shallow seawater are estimated to have been about three times that of deep-water samples.

  7. OSL dating of sediments from Negro and Solimões rivers - Amazon, Brazil

    NASA Astrophysics Data System (ADS)

    Fiore, M.; Soares, E. A. A.; Mittani, J. C. R.; Yee, M.; Tatumi, S. H.

    2014-02-01

    In this work, the OSL dating results of Quaternary fluvial deposits from the confluence of Negro and Solimões rivers were studied. The equivalent doses (De) of sediments were obtained using a Single Aliquot Regeneration (SAR) protocol. Statistic studies were made using frequency histogram, weighted histogram and Radial plot in order to analyze the De fluctuations. Ages from 74.5 to 205 thousand of years (Pleistocene) were recorded. The gamma-ray spectroscopy was used to evaluate the natural radioisotopes concentrations of the samples and low concentrations were found with values between 0.64 and 3.71 ppm for 235U and 238U; 2.01-9.77 ppm for 232Th; already, for 40K, the concentration was negligible. The OSL dating of sediments has contributed to a better understanding of the evolution of Negro and Solimões rivers, in Amazon, Brazil.

  8. Measuring and modelling the radiological impact of a phosphogypsum deposition site on the surrounding environment.

    PubMed

    Bituh, Tomislav; Petrinec, Branko; Skoko, Božena; Vučić, Zlatko; Marović, Gordana

    2015-03-01

    Phosphogypsum (PG) is a waste product (residue) from the production of phosphoric acid characterized by technologically enhanced natural radioactivity. Croatia's largest PG deposition site is situated at the edge of Lonjsko Polje Nature Park, a sensitive ecosystem possibly endangered by PG particles. This field study investigates two aspects relevant for the general radiological impact of PG: risk assessment for the environment and risk assessment for occupationally exposed workers and local inhabitants. Activity concentrations of natural radionuclides ((238)U, (235)U, (232)Th, (226)Ra, (210)Pb, and (40)K) were measured in the PG (at the deposition site), soil, and grass samples (in the vicinity of the site). The ERICA Assessment Tool was used to estimate the radiological impact of PG particles on non-human biota of the Lonjsko Polje Nature Park. The average annual effective dose for occupationally exposed workers was 0.4 mSv which was within the worldwide range.

  9. Current Inconsistencies in {sup 238}Pu, {sup 241,243}Am and {sup 242}Cm Evaluations and their Impact on Uncertainties

    SciTech Connect

    Maslov, V.M.

    2008-12-15

    Improvements in the nuclear reaction modeling and nuclear parameter systematics, consistent with the description of neutron data on major actinides {sup 232}Th, {sup 233}U, {sup 235}U, {sup 238}U and {sup 239}Pu will be shown to provide a sound basis for critical assessment of the fission, capture, inelastic scattering, and (n,xn) reaction cross sections on minor actinides. This will largely help to avoid substituting possible model deficiencies by enlarging parameter uncertainties in the conventional nuclear models. In a number of minor actinides, the uncertainty estimation of cross sections and prompt fission neutron spectra would require complete re-evaluation of basic data. Otherwise, extremely large cross section uncertainty estimates will have to be adopted, especially in the case of poorly investigated Np, Pu, Am, Cm targets.

  10. AN INTEGRAL REACTOR PHYSICS EXPERIMENT TO INFER ACTINIDE CAPTURE CROSS-SECTIONS FROM THORIUM TO CALIFORNIUM WITH ACCELERATOR MASS SPECTROMETRY

    SciTech Connect

    G. Youinou; M. Salvatores; M. Paul; R. Pardo; G. Palmiotti; F. Kondev; G. Imel

    2010-04-01

    The principle of the proposed experiment is to irradiate very pure actinide samples in the Advanced Test Reactor (ATR) at INL and, after a given time, determine the amount of the different transmutation products. The determination of the nuclide densities before and after neutron irradiation will allow inference of effective neutron capture cross-sections. This approach has been used in the past and the novelty of this experiment is that the atom densities of the different transmutation products will be determined using the Accelerator Mass Spectroscopy (AMS) technique at the ATLAS facility located at ANL. It is currently planned to irradiate the following isotopes: 232Th, 235U, 236U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 243Am and 248Cm.

  11. MANTRA: An Integral Reactor Physics Experiment to Infer Actinide Capture Cross-sections from Thorium to Californium with Accelerator Mass Spectrometry

    SciTech Connect

    G. Youinou; C. McGrath; G. Imel; M. Paul; R. Pardo; F. Kondev; M. Salvatores; G. Palmiotti

    2011-08-01

    The principle of the proposed experiment is to irradiate very pure actinide samples in the Advanced Test Reactor at INL and, after a given time, determine the amount of the different transmutation products. The determination of the nuclide densities before and after neutron irradiation will allow inference of effective neutron capture cross-sections. This approach has been used in the past and the novelty of this experiment is that the atom densities of the different transmutation products will be determined using the Accelerator Mass Spectrometry technique at the ATLAS facility located at ANL. It is currently planned to irradiate the following isotopes: 232Th, 235U, 236U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 243Am, 244Cm and 248Cm.

  12. Czech results at criticality dosimetry intercomparison 2002.

    PubMed

    Frantisek, Spurný; Jaroslav, Trousil

    2004-01-01

    Two criticality dosimetry systems were tested by Czech participants during the intercomparison held in Valduc, France, June 2002. The first consisted of the thermoluminescent detectors (TLDs) (Al-P glasses) and Si-diodes as passive neutron dosemeters. Second, it was studied to what extent the individual dosemeters used in the Czech routine personal dosimetry service can give a reliable estimation of criticality accident exposure. It was found that the first system furnishes quite reliable estimation of accidental doses. For routine individual dosimetry system, no important problems were encountered in the case of photon dosemeters (TLDs, film badge). For etched track detectors in contact with the 232Th or 235U-Al alloy, the track density saturation for the spark counting method limits the upper dose at approximately 1 Gy for neutrons with the energy >1 MeV.

  13. Rates of carbonate soil evolution from carbon, U- and Th-series isotope studies: Example of the Astian sands (SE France)

    NASA Astrophysics Data System (ADS)

    Barbecot, Florent; Ghaleb, Bassam; Hillaire-Marcel, Claude

    2015-04-01

    In carbonate rich soils, C-isotopes (14C, 13C) and carbonate mass budget may inform on centennial to millennial time scale dissolution/precipitation processes and weathering rates, whereas disequilibria between in the U- and Th-decay series provide tools to document high- (228Ra-228Th-210Pb) to low- (234U, 230Th, 231Pa, 226Ra) geochemical processes rate, covering annual to ~ 1Ma time scales, governing both carbonate and silicate soil fractions. Because lithology constitutes a boundary condition, we intend to illustrate the behavior of such isotopes in soils developed over Astian sands formation (up to ~ 30% carbonate) from the Béziers area (SE France). A >20 m thick unsaturated zone was sampled firstly along a naturally exposed section, then in a cored sequence. Geochemical and mineralogical analyses, including stable isotopes and 14C-measurements, were complemented with 228U, 234U, 230Th, 226Ra, 210Pb and 228Th, 232Th measurements. Whereas the upper 7 m depict geochemical and isotopic features forced by dissolution/precipitation processes leading to variable radioactive disequilibria, but overall deficits in more soluble elements of the decay series, the lower part of the sequence shows strong excesses in 234U and 230Th over parent isotopes (i.e., 238U and 234U, respectively). These features might have been interpreted as the result of successive phases of U-loss and gains. However, 226Ra and 230Th are in near-equilibrium, thus leading to conclude at a more likely slow enrichment process in both 234Th(234U) and 230Th, which we link to dissolved U-decay during groundwater recharge events. In addition, 210Pb deficits (vs parent 226Ra) are observed down to 12 m along the natural outcropping section and below the top-soil 210Pb-excess in the cored sequence, due to gaseous 222Rn-diffusion over the cliff outcrop. Based on C-isotope and chemical analysis, reaction rates at 14C-time scale are distinct from those estimates at the short- or long-lived U-series isotopes

  14. Uranium-series disequilibrium, sedimentation, diatom frustules, and paleoclimate change in Lake Baikal

    USGS Publications Warehouse

    Edgington, D.N.; Robbins, J.A.; Colman, Steven M.; Orlandini, K.A.; Gustin, M.-P.

    1996-01-01

    The large volume of water, approximately one-fifth of the total surface fresh water on the planet, contained in Lake Baikal in southeastern Siberia is distinguished by having a relatively high concentration of uranium (ca. 2 nM), and, together with the surface sediments, an unusually high 234U/238U alpha activity ratio of 1.95. About 80% of the input of uranium to the lake, with a 234U/238U ratio of 2.0, comes from the Selenga River. Profiles of uranium, as well as the extent of isotopic disequilibrium in a 9 m sediment core collected on Academic Ridge, generally show high values during interglacial periods corresponding to high diatom frustule numbers (DiFr) and biogenic silica (BSi) data that have been reported elsewhere. During glacial periods (low DiFr and BSi), uranium progeny (234U and 230Th) were in secular equilibrium with low concentrations of their parent 238U. Radionuclide distributions were interpreted in terms of a quantitative model allowing for adsorption of riverine inputs of uranium onto two classes of sedimenting particles with differing 238U/232Th ratios and uranium progeny in secular equilibrium. If the 234U/238U activity ratio of adsorbed uranium has remained constant, mean sedimentation rates can be independently estimated as 3.6 ?? 0.6 and 3.7 ?? 0.9 cm ?? kyr-1 for the decay of 234U and in-growth of 230Th, respectively. These rates are consistent with a mean rate of 3.76 cm ?? kyr-1, calculated by optimization of the correspondence between adsorbed 238U and ??18O in dated oceanic sediments. The adsorbed uranium apparently tracks variable river flow during interglacials and is drastically reduced during periods of glaciation. Evidently, uranium has not been significantly redistributed within Baikal sediments over at least the past 250 kyr and is a unique, biologically non-essential, tracer for climate-sensitive processes, which provide their own internal geochronometers, potentially useful for ages up to 1 Myr BP.

  15. Radioactive investigation of NORM samples from Southern Kuwait soil using high-resolution gamma-ray spectroscopy

    NASA Astrophysics Data System (ADS)

    Bajoga, A. D.; Alazemi, N.; Regan, P. H.; Bradley, D. A.

    2015-11-01

    Activity concentrations of soil and sand samples from southern part of Kuwait have been deduced for members of the 238U(226Ra) and 232Th(228Ac) decay chains, together with initial evaluations also provided of the concentrations for members of the 235U, 4n+1 chain. Additional activity concentration measurements have also been established for the single primordial radionuclide 40K and the anthropogenic radionuclides 137Cs from the same samples. The calculated activity concentration values and associated radiation hazard indices calculated were evaluated. The current results indicate activity concentrations ranging from 0.15±0.04 to 9.97±0.20 Bq/kg for Cs. For 226Ra, 232Th and 40K this ranges from 9.02±0.13 to 17.48±0.18, 7.90±0.10 to 14.29±0.22, and 259.6±4.7 137Cs to 347.3±6.0 Bq/kg, respectively. The mean values for dose rates, radium equivalent, hazard indices, and annual effective dose equivalent are 24.65±0.26 nG/h, 50.72±0.50 Bq/kg, 0.17, 0.14, and 30.0±0.3 μSv/yr, respectively. These are compared with analogous measurements from other locations both in the Middle Eastern Region and far-afield.

  16. Naturally Occurring Radionuclides of Ash Produced by Coal Combustion. The Case of the Kardia Mine in Northern Greece

    SciTech Connect

    Fotakis, M.; Tsikritzis, L.; Tzimkas, N.; Kolovos, N.; Tsikritzi, R.

    2008-08-07

    West Macedonia Lignite Center (WMLC), located in Northwest Greece, releases into the atmosphere about 21,400 tons/year of fly ash through the stacks of four coal fired plants. The lignite ash contains naturally occurring radionuclides, which are deposited on the WMLC basin. This work investigates the natural radioactivity of twenty six ash samples, laboratory produced from combustion of lignite, which was sampled perpendicularly to the benches of the Kardia mine. The concentrations of radionuclides {sup 40}K, {sup 235}U, {sup 238}U, {sup 226}Ra, {sup 228}Ra and {sup 232}Th, were measured spectroscopically and found round one order of magnitude as high as those of lignite. Subsequently the Radionuclide Partitioning Coefficients of radionuclides were calculated and it was found that they are higher for {sup 232}Th, {sup 228}Ra and {sup 40}K, because the latter have closer affinity with the inorganic matrix of lignite. During combustion up to one third of the naturally occurring radioisotopes escape from the solid phase into the flue gases. With comparison to relative global data, the investigated ash has been found to have relatively high radioactivity, but the emissions of the WMLC radionuclides contribute only 0.03% to the mean annual absorbed dose.

  17. Comparative analysis of dose rates in bricks determined by neutron activation analysis, alpha counting and X-ray fluorescence analysis for the thermoluminescence fine grain dating method

    NASA Astrophysics Data System (ADS)

    Bártová, H.; Kučera, J.; Musílek, L.; Trojek, T.

    2014-11-01

    In order to evaluate the age from the equivalent dose and to obtain an optimized and efficient procedure for thermoluminescence (TL) dating, it is necessary to obtain the values of both the internal and the external dose rates from dated samples and from their environment. The measurements described and compared in this paper refer to bricks from historic buildings and a fine-grain dating method. The external doses are therefore negligible, if the samples are taken from a sufficient depth in the wall. However, both the alpha dose rate and the beta and gamma dose rates must be taken into account in the internal dose. The internal dose rate to fine-grain samples is caused by the concentrations of natural radionuclides 238U, 235U, 232Th and members of their decay chains, and by 40K concentrations. Various methods can be used for determining trace concentrations of these natural radionuclides and their contributions to the dose rate. The dose rate fraction from 238U and 232Th can be calculated, e.g., from the alpha count rate, or from the concentrations of 238U and 232Th, measured by neutron activation analysis (NAA). The dose rate fraction from 40K can be calculated from the concentration of potassium measured, e.g., by X-ray fluorescence analysis (XRF) or by NAA. Alpha counting and XRF are relatively simple and are accessible for an ordinary laboratory. NAA can be considered as a more accurate method, but it is more demanding regarding time and costs, since it needs a nuclear reactor as a neutron source. A comparison of these methods allows us to decide whether the time- and cost-saving simpler techniques introduce uncertainty that is still acceptable.

  18. U-series ages of solitary corals from the California coast by mass spectrometry

    USGS Publications Warehouse

    Stein, Martin; Wasserburg, G.J.; Lajoie, K.R.; Chen, J.-H.

    1991-01-01

    The purpose of this study is to evaluate the feasibility of dating fossil solitary corals from Pleistocene marine strandlines outside tropical latitudes using the recently developed high sensitivity, high-precision U-series technique based on thermal-ionization mass-spectrometry (TIMS). The TIMS technique is much more efficient than conventional a spectrometry and, as a result, multiple samples of an individual coral skeleton, or different specimens from the same bed can be analyzed. Detached and well-rounded fossil specimens of the solitary coral Balanophyllia elegans were collected from relict littoral deposits on emergent marine terraces along the California coast at Cayucos terrace (elevation 8 m, previously dated at 124 and 117 Ky by ?? counting), Shell Beach terrace (elevation about 25 m, previously undated), Nestor terrace, San Diego (elevation 23 m, previously dated at 131 to 109 Ky ), Bird Rock terrace, San Diego ( elevation 8 m, previously dated at 81 Ky ). Attached living specimens were collected from the intertidal zone on the modern terrace at Moss Beach. Concentrations of 232Th in both living and fossil specimens are much higher than in reef-building corals (12 to 624 pmol/g vs. 0.1 to 1.6 pmol/g, respectively). However, because 230Th/232Th in Balanophyllia elegans are very low (2.22 ?? 10-3 to 4.33 ?? 10-4), the high 232Th concentrations have negligible effect on the 230Th-234U dates. The high 232Th concentration in the living specimen (33.1 pmol/g) indicates that a significant amount of 232Th is incorporated in the aragonitic skeleton during growth, or attached to clay-sized silicates trapped in the skeletal material. The calculated initial 234U activities in the fossil specimens of Balanophyllia elegans are higher than the 234U activity in modern seawater or in the modern specimen. The higher initial activities could possibly reflect the influx of 234U-enriched continental water into Pleistocene coastal waters, or it could reflect minor diagenetic

  19. U-series Chronology of volcanoes in the Central Kenya Peralkaline Province, East African Rift

    NASA Astrophysics Data System (ADS)

    Negron, L. M.; Ma, L.; Deino, A.; Anthony, E. Y.

    2012-12-01

    We are studying the East African Rift System (EARS) in the Central Kenya Peralkaline Province (CKPP), and specifically the young volcanoes Mt. Suswa, Longonot, and Menengai. Ar dates by Al Deino on K-feldspar phenocrysts show a strong correlation between older Ar ages and decreasing 230Th/232Th, which we interpret to reflect the age of eruption. This system has been the subject of recent research done by several UTEP alumni including Antony Wamalwa using potential field and magnetotelluric (MT) data to identify and characterize fractures and hydrothermal fluids. Also research on geochemical modeling done by John White, Vanessa Espejel and Peter Omenda led to the hypothesis of possible disequilibrium in these young, mainly obsidian samples in their post eruptive history. A pilot study of 8 samples, (also including W-2a USGS standard and a blank) establish the correlation that was seen between the ages found by Deino along with the 230/232Th ratios. All 8 samples from Mt. Suswa showed a 234U/238U ratio of (1) which indicates secular equilibrium or unity and that these are very fresh samples with no post-eruptive decay or leaching of U isotopes. The pilot set was comprised of four samples from the ring-trench group (RTG) with ages ranging from 7ka-present, two samples from the post-caldera stage ranging from 31-10ka, one sample from the syn-caldera stage dated at 41ka, and one sample from the pre-caldera stage dated at 112ka. The young RTG had a 230/232Th fractionation ratio of 0.8 ranging to the older pre-caldera stage with a 230/232Th ratio of 0.6. From this current data and research of 14C ages by Nick Rogers, the data from Longonot volcano was also similar to the 230/232Th ratio we found. Rogers' data places Longonot volcano ages to be no more than 20ka with the youngest samples also roughly around 0.8 disequilibrium. These strong correlations between the pilot study done for Mt. Suswa, 40Ar ages by Deino, along with 14C ages from Rogers have led to the

  20. Open system U-series ages of corals from a subsiding reef in New Caledonia: Implications for sea level changes, and subsidence rate

    NASA Astrophysics Data System (ADS)

    Frank, N.; Turpin, L.; Cabioch, G.; Blamart, D.; Tressens-Fedou, M.; Colin, C.; Jean-Baptiste, P.

    2006-09-01

    On the Amédée islet, 4 drill cores were recovered from the barrier reef of Western New Caledonia. The coral reef is slowly subsiding and is thus percolated by sea water during sea level highstands. The cores sample a ˜ 10 m thick Holocene reef overlying a 24 m thick reef of marine isotope stage (MIS) 5.5, which in turn overlies older reef material from MIS 7.5 and beyond. ( 234U/ 238U) and ( 230Th/ 238U) ratios and 232Th were determined by thermal ionization mass spectrometry on aragonitic coral samples that were carefully investigated using X-ray diffraction and scanning electron microscopy. The petrographic study shows an increasing coral weathering with growing coral age that causes different degree of U-series open system behavior and 232Th accumulation. Holocene corals exhibit a small degree of early diagenesis and yield 230Th/ 238U ages according to the Holocene sea level rise from ˜ 8200 years to 5000 years BP. Corals from the last Interglacial section have experienced more frequent replacement of aragonite fibers and minor dissolution, and U-series open system behavior is evident. To estimate the impact of recoil processes and alteration on the U-series system two models by Villemant and Feuillet [B. Villemant, N. Feuillet, Dating open systems by the 238U- 234U- 230Th method: application to Quaternary reef terraces, Earth and Planetary Science Letters 210(2003) 105-118.] and Thompson et al. [W. G. Thompson, M. W. Spiegelman, S. L. Goldstein, R. C. Speed, An open-system model for U-series age determinations of fossil corals, Earth and Planetary Science Letters 210(2003) 365-381.] have been tested. These models yield identical ages within uncertainty, which are in agreement to the sea level history of the past 250,000 years, as long as physico-chemical alteration and re-crystallization is small. Consequently, we were able to estimate the subsidence rate from the subsidence observed between the end of MIS 5.5 and the early Holocene, which is ˜ 0.16 ± 0

  1. The Characterization of Biotic and Abiotic Media Upgradient and Downgradient of the Los Alamos Canyon Weir

    SciTech Connect

    P.R. Fresquez

    2006-01-15

    As per the Mitigation Action Plan for the Special Environmental Analysis of the actions taken in response to the Cerro Grande Fire, sediments, vegetation, and small mammals were collected directly up- and downgradient of the Los Alamos Canyon weir, a low-head sediment control structure located on the northeastern boundary of Los Alamos National Laboratory, to determine contaminant impacts, if any. All radionuclides ({sup 3}H, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu, {sup 90}Sr, {sup 241}Am, {sup 234}U, {sup 235}U and {sup 238}U) and trace elements (Ag, As, Ba, Be, Cd, Cr, Cu, Hg, Ni, Pb, Sb, Se, and Tl) in these media were low and most were below regional upper level background concentrations (mean plus three sigma). The very few constituents that were above regional background concentrations were far below screening levels (set from State and Federal standards) for the protection of the human food chain and the terrestrial environment.

  2. Concentrations of Radionuclides and Trace Elements in Soils and Vegetation Around the DARHT Facility during 2004

    SciTech Connect

    P.R. Fresquez

    2004-10-01

    Samples of soil, sediment, and unwashed overstory and understory vegetation were collected at four locations around the Dual-Axis Radiographic Hydrodynamic Test (DARHT) facility at Los Alamos National Laboratory (LANL). All samples were analyzed for concentrations of {sup 3}H, {sup 137}Cs, {sup 90}Sr, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 234}U, {sup 235}U, {sup 238}U, Ag, As, Ba, Be, Cd, Cr, Cu, Hg, Ni, Pb, Sb, Se, and Tl. These results, which represent five years since the start of operations, were compared with baseline statistical reference level (BSRL) data established over a four-year-long preoperational period prior to DARHT operations, and to LANL and U.S. Environmental Protection Agency Screening Action Levels (SALs). Most radionuclides and trace elements in soil, sediment, and vegetation were below BSRL values and those soils/sediments that were above BSRLs were far below SALs.

  3. Benchmarking the External Surrogate Ratio Method using the (alpha,alpha' f) reaction at STARS

    SciTech Connect

    Lesher, S R; Bernstein, L A; Ai, H; Beausang, C W; Bleuel, D; Burke, J T; Clark, R M; Fallon, P; Gibelin, J; Lee, I Y; Lyles, B F; Macchiavelli, A O; McMahan, M A; Moody, K J; Norman, E B; Phair, L; Rodriguez-Vieitez, E; Wiedeking, M

    2008-01-09

    We measured the ratio of the fission probabilities of {sup 234}U* relative to {sup 236}U* formed via an ({alpha},{alpha}{prime}) direct reactions using the STARS array at the 88-inch cyclotron at the Lawrence Berkeley National Laboratory. This ratio has a shape similar to the ratio of neutron capture probabilities from {sup 233}U(n; f) and {sup 235}U(n; f), indicating the alpha reactions likely formed a compound nucleus. This result indicates that the ratios of fission exit channel probabilities for two actinide nuclei populated via ({alpha}, {alpha}{prime}) can be used to determine an unknown fission cross section relative to a known one. The validity of the External Surrogate Ratio Method (ESRM) is tested and the results support the conclusions of Burke et al. [1].

  4. Determination of alpha-emitting uranium isotopes in soft tissues by solvent extraction and alpha-spectrometry.

    PubMed

    Singh, N P; Wrenn, M E

    1983-04-01

    A radiochemical procedure has been developed for the determination of alpha-emitting isotopes of uranium ((238)U, (235)U and (234)U) in soft tissues. Known amounts of sample are spiked with (232)U internal tracer and wet-ashed. Uranium is co-precipitated with iron hydroxide as carrier, and extracted into 20% trilaurylamine solution in xylene after dissolution of the precipitate in 10M hydrochloric acid. The uranium, after stripping into an aqueous phase, is electro-deposited onto a platinum disc and counted by alpha-spectrometry. The radiochemical recovery ranges from 60 to 85% for bovine liver samples. The average radiochemical recoveries for human tissues vary from 53 to 78%.

  5. Protactinium-231 measurement and application to a uranium series transport model

    NASA Astrophysics Data System (ADS)

    Golian, C.; Nightingale, T.; Airey, P. L.

    1984-06-01

    Precise measurements of small deviations of 230Th/ 234U and 231Pa/ 235U contribute to the modelling of the geochemical transport of uranium series nuclides. The use of alpha-spectrometry to measure the second-order daughter product 227Th was the analytical technique chosen. It was thereby assumed that the intermediate 227Ac is immobile. Complete methematical expressions for the count rate in various regions of the spectrum have been developed. They allow calculation of the initial yield from the cumulative counts of 227Th and the interfering 223Ra. 224Ra and 212Bi for extended time periods. The resulting increase in precision is particularly useful at low levels. The approach to modelling the transport of uranium series nuclides down-gradient of deposits within the Alligator Rivers Uranium Province of the Northern Territory of Australia is outlined. Some preliminary data are presented which call into question the assumption of the immobility of the 227Ac.

  6. Recommended Method To Account For Daughter Ingrowth For The Portsmouth On-Site Waste Disposal Facility Performance Assessment Modeling

    SciTech Connect

    Phifer, Mark A.; Smith, Frank G. III

    2013-06-21

    A 3-D STOMP model has been developed for the Portsmouth On-Site Waste Disposal Facility (OSWDF) at Site D as outlined in Appendix K of FBP 2013. This model projects the flow and transport of the following radionuclides to various points of assessments: Tc-99, U-234, U-235, U-236, U-238, Am-241, Np-237, Pu-238, Pu-239, Pu-240, Th-228, and Th-230. The model includes the radioactive decay of these parents, but does not include the associated daughter ingrowth because the STOMP model does not have the capability to model daughter ingrowth. The Savannah River National Laboratory (SRNL) provides herein a recommended method to account for daughter ingrowth in association with the Portsmouth OSWDF Performance Assessment (PA) modeling.

  7. Radiological Control of Water in Reactor Pond of MR Reactor in NRC 'Kurchatov Institute', During Dismantling Work - 13462

    SciTech Connect

    Stepanov, Alexey; Simirsky, Yury; Semin, Ilya; Volkovich, Anatoly; Ivanov, Oleg

    2013-07-01

    The analysis of the activity and radionuclide composition of water from the MR reactor pond for α,β,γ-ray radionuclides was made. To solve this problem we use a wide range of laboratory equipment: gamma spectrometric complex, beta spectrometric complex, vacuum alpha spectrometer, and spectrometric complex with liquid scintillator. The water from MR reactor pond contains: Cs-137 (2,6*10{sup 2} Bq/g), Co-60(1,8 Bq/g), Sr-90 (1,0*10{sup 2} Bq/g), H-3 (7,0*10{sup 3} Bq/g), and components of nuclear fuel (U-232,U-234,U-235,U-236,U-238). Therefore the cleaning water from radioactivity waste occurs to be quite a complicated radiochemical task. (authors)

  8. Uranium-series dating of some pleistocene marine deposits in Southern California

    USGS Publications Warehouse

    Szabo, B. J.; Vedder, J.G.

    1971-01-01

    Analyses of uranium isotopes and their long-lived daughter products showed evidence of uranium migration in most of the 22 fossil mollusk shell samples from marine terrace deposits in southern California. Two samples, however, remained an ideal closed system as indicated by concordant 230Th/234U and 231Pa/235U dates. The closed-system age of the lowest exposed marine terrace deposit along part of the mainland coast of southern California is 69 000 ?? 10 000 yr, and correlation of this discontinuous deposit is afforded between the Newport Beach-Laguna Beach area and the Palos Verdes Hills. Some mollusk shell samples were dated by the open-system model; the remaining samples were found to be unsuitable for uranium-series dating. ?? 1971.

  9. Isotopic evidence for reductive immobilization of uranium across a roll-front mineral deposit

    DOE PAGES

    Brown, Shaun T.; Basu, Anirban; Christensen, John N.; ...

    2016-05-20

    We use uranium (U) isotope ratios to detect and quantify the extent of natural U reduction in groundwater across a roll front redox gradient. Our study was conducted at the Smith Ranch-Highland in situ recovery (ISR) U mine in eastern Wyoming, USA, where economic U deposits occur in the Paleocene Fort Union formation. To evaluate the fate of aqueous U in and adjacent to the ore body, we investigated the chemical composition and isotope ratios of groundwater samples from the roll-front type ore body and surrounding monitoring wells of a previously mined area. The 238U/235U of groundwater varies by approximatelymore » 3‰ and is correlated with U concentrations. Fluid samples down-gradient of the ore zone are the most depleted in 238U and have the lowest U concentrations. Activity ratios of 234U/238U are ~5.5 up-gradient of the ore zone, ~1.0 in the ore zone, and between 2.3 and 3.7 in the down-gradient monitoring wells. High-precision measurements of 234U/238U and 238U/235U allow for development of a conceptual model that evaluates both the migration of U from the ore body and the extent of natural attenuation due to reduction. We find that the premining migration of U down-gradient of the delineated ore body is minimal along eight transects due to reduction in or adjacent to the ore body, whereas two other transects show little or no sign of reduction in the down-gradient region. Lastly, these results suggest that characterization of U isotopic ratios at the mine planning stage, in conjunction with routine geochemical analyses, can be used to identify where more or less postmining remediation will be necessary.« less

  10. Radionuclide Transport in Fracture-Granite Interface Zones

    SciTech Connect

    Hu, Q; Mori, A

    2007-09-12

    In situ radionuclide migration experiments, followed by excavation and sample characterization, were conducted in a water-conducting shear zone at the Grimsel Test Site (GTS) in Switzerland to study diffusion paths of radionuclides in fractured granite. In this work, we employed a micro-scale mapping technique that interfaces laser ablation sampling with inductively coupled plasma-mass spectrometry (LA/ICP-MS) to measure the fine-scale (micron-range) distribution of actinides ({sup 234}U, {sup 235}U, and {sup 237}Np) in the fracture-granite interface zones. Long-lived {sup 234}U, {sup 235}U, and {sup 237}Np were detected in flow channels, as well as in the adjacent rock matrix, using the sensitive, feature-based mapping of the LA/ICP-MS technique. The injected sorbing actinides are mainly located within the advective flowing fractures and the immediately adjacent regions. The water-conducting fracture studied in this work is bounded on one side by mylonite and the other by granitic matrix regions. These actinides did not penetrate into the mylonite side as much as the relatively higher-porosity granite matrix, most likely due to the low porosity, hydraulic conductivity, and diffusivity of the fracture wall (a thickness of about 0.4 mm separates the mylonite region from the fracture) and the mylonite region itself. Overall, the maximum penetration depth detected with this technique for the more diffusive {sup 237}Np over the field experimental time scale of about 60 days was about 10 mm in the granitic matrix, illustrating the importance of matrix diffusion in retarding radionuclide transport from the advective fractures. Laboratory tests and numerical modeling of radionuclide diffusion into granitic matrix was conducted to complement and help interpret the field results. Measured apparent diffusivity of multiple tracers in granite provided consistent predictions for radionuclide transport in the fractured granitic rock.

  11. Hybrid Enrichment Assay Methods for a UF6 Cylinder Verification Station: FY10 Progress Report

    SciTech Connect

    Smith, Leon E.; Jordan, David V.; Orton, Christopher R.; Misner, Alex C.; Mace, Emily K.

    2010-08-01

    Pacific Northwest National Laboratory (PNNL) is developing the concept of an automated UF6 cylinder verification station that would be located at key measurement points to positively identify each cylinder, measure its mass and enrichment, store the collected data in a secure database, and maintain continuity of knowledge on measured cylinders until the arrival of International Atomic Energy Agency (IAEA) inspectors. At the center of this unattended system is a hybrid enrichment assay technique that combines the traditional enrichment-meter method (based on the 186 keV peak from 235U) with non-traditional neutron-induced high-energy gamma-ray signatures (spawned primarily by 234U alpha emissions and 19F(alpha, neutron) reactions). Previous work by PNNL provided proof-of-principle for the non-traditional signatures to support accurate, full-volume interrogation of the cylinder enrichment, thereby reducing the systematic uncertainties in enrichment assay due to UF6 heterogeneity and providing greater sensitivity to material substitution scenarios. The work described here builds on that preliminary evaluation of the non-traditional signatures, but focuses on a prototype field system utilizing NaI(Tl) and LaBr3(Ce) spectrometers, and enrichment analysis algorithms that integrate the traditional and non-traditional signatures. Results for the assay of Type-30B cylinders ranging from 0.2 to 4.95 wt% 235U, at an AREVA fuel fabrication plant in Richland, WA, are described for the following enrichment analysis methods: 1) traditional enrichment meter signature (186 keV peak) as calculated using a square-wave convolute (SWC) algorithm; 2) non-traditional high-energy gamma-ray signature that provides neutron detection without neutron detectors and 3) hybrid algorithm that merges the traditional and non-traditional signatures. Uncertainties for each method, relative to the declared enrichment for each cylinder, are calculated and compared to the uncertainties from an attended

  12. Mixing and cycling of uranium, thorium and 210Pb in Puget Sound sediments

    NASA Astrophysics Data System (ADS)

    Carpenter, R.; Peterson, M. L.; Bennett, J. T.; Somayajulu, B. L. K.

    1984-10-01

    Activity profiles of excess 234Th, excess 210Pb, 232Th, 230Th, 234U and 238U, and 228/232Th ratios determined in eight box cores of sediment from six sites in central Puget Sound provide new insights into the dynamic nature of solid phase mixing in surface sediments, the exchange of 228Ra and other soluble species across the sediment-water interface, and the cycling of U, Th and 210Pb in this coastal zone. Comparison of excess 234Th inventories in sediments with its production rate in the overlying water column indicates a mean residence time of at most 14 days for particles in the central Puget Sound water column. Surface sediment horizons with excess 234Th have no excess 228Th which might be used to ascertain sediment accumulation rates over the past decade. Instead, deficiencies of 228Th due to loss of soluble 228Ra from pore water to the overlying water persist to 20-30 cm, revealing that exchange of soluble chemicals between pore and overlying waters reaches these depths in the extensively bioturbated sediments of Puget Sound. Solid phase U isotope concentrations tend to increase by up to a factor of two with depth in sediments, as a result of dissolved U being biologically pumped down into sediments where it is partially removed when conditions become mildly reducing. 232Th and 230Th activities and 230/232Th ratios are constant with depth in sediments, indicating constant detrital phase compositions and essentially no authigenic 230Th. Steady state 210Pb depositional activities in and fluxes to Puget Sound sediments average only about onehalf those for sediments of the open Washington coast north of the Columbia River mouth, primarily because of a much lower supply of dissolved 210Pb in sea waters adverting into Puget Sound. Excess 234Th profiles in sediments reveal much more detail about the depth dependency, dynamic nature and recent history of solid phase mixing processes than excess 210Pb profiles. At least six of eight 234Th profiles show that mixing

  13. Computational simulation of (nat)UO2, (232)ThO2 and U3O8-Al pills to estimate (p,fission) (99)Mo yield in the modeled targets irradiated by CYCLONE30 accelerator.

    PubMed

    Jozvaziri, Atieh; Gholamzadeh, Zohreh; Yousefi, Kamran; Mirvakili, Seyed Mohammad; Alizadeh, Masoomeh; Aboudzadeh, Mohammadreza

    2017-03-01

    (99)Mo is important for both therapy and imaging purposes. Accelerator and reactor-based procedures are applied to produce it. Newly proton-fission method has been taken in attention by some research centers. In the present work, computationally investigation of the (99)Mo yield in different fissionable targets irradiated by proton was aimed. The results showed UO2 pill target could be efficiently used to produce 11.12Ci/g-U saturation yield of (99)Mo using 25MeV proton irradiation of the optimized-dimension target with 70µA current.

  14. ISOTOPIC COMPOSITIONS OF URANIUM REFERENCE MATERIALS

    SciTech Connect

    Jacobsen, B; Borg, L; Williams, R; Brennecka, G; Hutcheon, I

    2009-09-03

    Uranium isotopic compositions of a variety of U standard materials were measured at Lawrence Livermore National Laboratory and are reported here. Both thermal ionization mass spectrometry (TIMS) and multi-collector inductively couple plasma mass spectrometry (MC-ICPMS) were used to determine ratios of the naturally occurring isotopes of U. Establishing an internally coherent set of isotopic values for a range of U standards is essential for inter-laboratory comparison of small differences in {sup 238}U/{sup 235}U, as well as the minor isotopes of U. Differences of {approx} 1.3{per_thousand} are now being observed in {sup 238}U/{sup 235}U in natural samples, and may play an important role in understanding U geochemistry where tracing the origin of U is aided by U isotopic compositions. The {sup 238}U/{sup 235}U ratios were measured with a TRITON TIMS using a mixed {sup 233}U-{sup 236}U isotopic tracer to correct for instrument fractionation. this tracer was extremely pure and resulted in only very minor corrections on the measured {sup 238}U/{sup 235}U ratios of {approx} 0.03. The values obtained for {sup 238}U/{sup 235}U are: IRMM184 = 137.698 {+-} 0.020 (n = 15), SRM950a = 137.870 {+-} 0.018 (n = 8), and CRM112a = 137.866 {+-} 0.030 (n = 16). Uncertainties represent 2 s.d. of the population. The measured value for IRMM184 is in near-perfect agreement with the certified value of 137.697 {+-} 0.042. However, the U isotopic compositions of SRM950a and CRM112a are not certified. Minor isotopes of U were determined with a Nu Plasma HR MC-ICPMS and mass bias was corrected by sample/standard bracketing to IRMM184, using its certified {sup 238}U/{sup 235}U ratio. Thus, the isotopic compositions determined using both instruments are compatible. The values obtained for {sup 234}U/{sup 235}U are: SRM950a = (7.437 {+-} 0.043) x 10{sup -3} (n = 18), and CRM112a = (7.281 {+-} 0.050) x 10{sup -3} (n = 16), both of which are in good agreement with published values. The value for

  15. U-isotopes and (226)Ra as tracers of hydrogeochemical processes in carbonated karst aquifers from arid areas.

    PubMed

    Guerrero, José Luis; Vallejos, Ángela; Cerón, Juan Carlos; Sánchez-Martos, Francisco; Pulido-Bosch, Antonio; Bolívar, Juan Pedro

    2016-07-01

    Sierra de Gádor is a karst macrosystem with a highly complex geometry, located in southeastern Spain. In this arid environment, the main economic activities, agriculture and tourism, are supported by water resources from the Sierra de Gádor aquifer system. The aim of this work was to study the levels and behaviour of some of the most significant natural radionuclides in order to improve the knowledge of the hydrogeochemical processes involved in this groundwater system. For this study, 28 groundwater and 7 surface water samples were collected, and the activity concentrations of the natural U-isotopes ((238)U, (235)U and (234)U) and (226)Ra by alpha spectrometry were determined. The activity concentration of (238)U presented a large variation from around 1.1 to 65 mBq L(-1). Elevated groundwater U concentrations were the result of oxidising conditions that likely promoted U dissolution. The PHREEQC modelling code showed that dissolved U mainly existed as uranyl carbonate complexes. The (234)U/(238)U activity ratios were higher than unity for all samples (1.1-3.8). Additionally, these ratios were in greater disequilibrium in groundwater than surface water samples, the likely result of greater water-rock contact time. (226)Ra presented a wide range of activity concentrations, (0.8 up to about 4 × 10(2) mBq L(-1)); greatest concentrations were detected in the thermal area of Alhama. Most of the samples showed (226)Ra/(234)U activity ratios lower than unity (median = 0.3), likely the result of the greater mobility of U than Ra in the aquifer system. The natural U-isotopes concentrations were strongly correlated with dissolution of sulphate evaporites (mainly gypsum). (226)Ra had a more complex behaviour, showing a strong correlation with water salinity, which was particularly evident in locations where thermal anomalies were detected. The most saline samples showed the lowest (234)U/(238)U activity ratios, probably due to fast uniform bulk mineral dissolution

  16. HEU age determination

    SciTech Connect

    Moorthy, A.R.; Kato, W.Y.

    1997-07-01

    A new technique has been developed to determine the age of highly enriched uranium (HEU) in solids. Uranium age is defined as the time since the uranium-containing material was last subjected to a process capable of separating uranium from its radioactive-decay daughters. [Most chemical processing, uranium enrichment, volatilization processes, and phase transformations (especially relevant for uranium hexafluoride) can result in separation of the uranium parent material from the decay-product daughters.] Determination of the uranium age, as defined here, may be relevant in verifying arms-control agreements involving uranium-containing nuclear weapons. The HEU age is determined from the ratios of relevant uranium daughter isotopes and their parents, viz {sup 230}Th/{sup 234}U and {sup 231}Pa/{sup 235}U. Uranium isotopes are quantitatively measured by their characteristic gamma rays and their daughters by alpha spectroscopy. In some of the samples, where HEU is enriched more than 99%, the only mode of HEU age determination is by the measurement of {sup 231}Pa since there is negligible quantity of {sup 230}Th due to very low atom concentrations of {sup 234}U in the samples. In this report the methodology and the data for determining the age of two HEU samples are presented.

  17. Uranium-series dating of actinide decay series mobility at Pena Blanca

    SciTech Connect

    Dixon, P.R.; Goldstein, S.J.; Murrell, M.T.

    1997-12-31

    Studies of U-series disequilibria near uranium ore deposits can provide valuable information on the mobility of actinides and their daughters over the range of timescales needed to assess the stability of proposed waste repositories. We have applied highly sensitive TIMS methods to obtain 238U-234U-230Th dates for three whole rock samples within a {approximately}30 in long fracture emanating into surrounding tuff from the deposit at Pena Blanca, Mexico. The 238U-234U-230Th data lie on a whole-rock isochron that requires closed-system behavior for the last 380 ka. Preliminary 231Pa-235U data for the U-rich vein also indicates closed system behavior for at least the last 100 ka. In contrast, 226Ra/230Th activity ratios range from 0.76-0.99 which indicates more recent Ra mobility within the fracture most likely due to surface water infiltration. Our results require uranium, thorium and protactinium stability despite recent radium mobility and provide important constraints on repository stability over {approximately}100 ka timescales.

  18. Application of Inductively Coupled Plasma Mass Spectrometry to the determination of uranium isotope ratios in individual particles for nuclear safeguards

    NASA Astrophysics Data System (ADS)

    Zhang, Xiao Zhi; Esaka, Fumitaka; Esaka, Konomi T.; Magara, Masaaki; Sakurai, Satoshi; Usuda, Shigekazu; Watanabe, Kazuo

    2007-10-01

    The capability of inductively coupled plasma mass spectrometry (ICP-MS) for the determination of uranium isotope ratios in individual particles was determined. For this purpose, we developed an experimental procedure including single particle transfer with a manipulator, chemical dissolution and isotope ratio analysis, and applied to the analysis of individual uranium particles in certified reference materials (NBL CRM U050 and U350). As the result, the 235U/ 238U isotope ratio for the particle with the diameter between 0.5 and 3.9 μm was successfully determined with the deviation from the certified ratio within 1.8%. The relative standard deviation (R.S.D.) of the 235U/ 238U isotope ratio was within 4.2%. Although the analysis of 234U/ 238U and 236U/ 238U isotope ratios gave the results with inferior precision, the R.S.D. within 20% was possible for the measurement of the particle with the diameter more than 2.1 μm. The developed procedure was successfully applied to the analysis of a simulated environmental sample prepared from a mixture of indoor dust (NIST SRM 2583) and uranium particles (NBL CRM U050, U350 and U950a). From the results, the proposed procedure was found to be an alternative analytical tool for nuclear safeguards.

  19. General Constraints on Cross Sections Deduced from Surrogate Reactions

    SciTech Connect

    Younes, W

    2003-08-14

    Cross sections that cannot be measured in the laboratory, e.g. because the target lifetime is too short, can be inferred indirectly from a different reaction forming the same compound system, but with a more accessible beam/target combination (the ''surrogate-reaction'' technique). The reactions share the same compound system and a common decay mechanism, but they involve different formation processes. Therefore, an implicit constraint is imposed on the inferred cross section deduced from the measured surrogate-reaction data, through the common decay mechanism. In this paper, the mathematical consequences of this implicit constraint are investigated. General formulas are derived from upper and lower bounds on the inferred cross section, estimated from surrogate data in a procedure which does not require any modeling of the common decay process. As an example, the formulas developed here are applied to the case of the {sup 235}U(n,f) cross section, deduced from {sup 234}U(t,pf) surrogate data. The calculated bounds are not very tight in this particular case. However, by introducing a few qualitative assumptions about the physics of the fission process, meaningful bounds on the deduced cross section are obtained. Upper and lower limits for the cross-section ratio of the (n,f) reaction on the {sup 235}U isomer at E{sub x} = 77 eV relative to the (n,f) reaction on the ground state are also calculated. The generalization of this technique to other surrogate reactions is discussed.

  20. Test and evaluation results of the /sup 252/Cf shuffler at the Savannah River Plant

    SciTech Connect

    Crane, T.W.

    1981-03-01

    The /sup 252/Cf Shuffler, a nondestructive assay instrument employing californium neutron source irradiation and delayed-neutron counting, was developed for measuring /sup 235/U content of scrap and waste items generated at the Savannah River Plant (SRP) reactor fuel fabrication facility. The scrap and waste items include high-purity uranium-aluminum alloy ingots as well as pieces of castings, saw and lathe chips from machining operations, low-purity items such as oxides of uranium or uranium intermixed with flux materials found in recovery operations, and materials not recoverable at SRP such as floor sweepings or residues from the uranium scrap recovery operation. The uranium contains about 60% /sup 235/U with the remaining isotopes being /sup 236/U, /sup 238/U, and /sup 234/U in descending order. The test and evaluation at SRP concluded that the accuracy, safety, reliability, and ease of use made the /sup 252/Cf Shuffler a suitable instrument for routine use in an industrial, production-oriented plant.

  1. Consequences of slow growth for 230Th/U dating of Quaternary opals, Yucca Mountain, NV, USA

    USGS Publications Warehouse

    Neymark, L.A.; Paces, J.B.

    2000-01-01

    Thermal ionization mass-spectrometry 234U/238U and 230Th/238U data are reported for uranium-rich opals coating fractures and cavities within the silicic tuffs forming Yucca Mountain, NV, the potential site of a high-level radioactive waste repository. High uranium concentrations (up to 207 ppm) and extremely high 230Th/232Th activity ratios (up to about 106) make microsamples of these opals suitable for precise 230Th/U dating. Conventional 230Th/U ages range from 40 to greater than 600 ka, and initial 234U/238U activity ratios between 1.03 and 8.2. Isotopic evidence indicates that the opals have not experienced uranium mobility; however, wide variations in apparent ages and initial 234U/238U ratios for separate subsamples of the same outermost mineral surfaces, positive correlation between ages and sample weights, and negative correlation between 230Th/U ages and calculated initial 234U/238U are inconsistent with the assumption that all minerals in a given subsample was deposited instantaneously. The data are more consistent with a conceptual model of continuous deposition where secondary mineral growth has occurred at a constant, slow rate up to the present. This model assumes that individual subsamples represent mixtures of older and younger material, and that calculations using the resulting isotope ratios reflect an average age. Ages calculated using the continuous-deposition model for opals imply average mineral growth rates of less than 5 mm/m.y. The model of continuous deposition also predicts discordance between ages obtained using different radiometric methods for the same subsample. Differences in half-lives will result in younger apparent ages for the shorter-lived isotope due to the greater influence of younger materials continuously added to mineral surfaces. Discordant 14C, 230Th/U and U-Pb ages obtained from outermost mineral surfaces at Yucca Mountain support this model. (C) 2000 Elsevier Science B.V. All rights reserved.

  2. U-series Dating of Stalagmites from Borneo

    NASA Astrophysics Data System (ADS)

    Adkins, J. F.; Partin, J.; Cobb, K.; Clark, B.

    2006-12-01

    In a series of field campaigns dating back to the fall of 2003 we have collected over 60 stalagmites from the Gunung Buda cave system in Sarawak, Malaysia (4°N, 115°E). At least twenty of these samples have excellent calcite preservation and span an age range from modern to over 500,000 years old. The bulk of the collection is of early glacial to Holocene age and can provide multiple overlapping records of climate variability from the Western Pacific Warm Pool. However, generating absolute U-series ages from this collection is challenging. The host rock is a Miocene aged limestone that is covered by rainforest with virtually no topsoil development. This setting leaves the typical stalagmite sample with a low uranium concentration (100s of ppb), a low initial δ234U (-650‰ to -100‰), and a relatively high detrital Th concentration (10s to 100s of pmol/g). We have generated age models in these difficult circumstances by making over 150 MC-ICP-MS measurements of the 238U-234U-230Th-232Th disequilibrium system. Ages are limited by our correction for initial 230Th. This is a common problem in U-series dating of stalagmites that we have addressed by generating a "histogram" of initial 230/232 values. With 14 isochrons from four separate stalagmites spanning the glacial maximum through the Holocene we can conservatively constrain the initial 230/232 atom ratio to be 60±10x10-6. There are small differences in the weighted mean of this value between stalagmites, but no systematic differences with time within a stalagmite. The very low δ234U values are intriguing and must represent the effects of recent weathering of the host limestone. These low and variable δ234U ratios also make it imperative to calculate the initial 230/232 ratios with full three-dimensional isochrons, extrapolating to zero U-238 on a "Rosholt Diagram" does not produce a consistent answer between the samples. Overall we can produce 2 sigma age errors that are better than 1% for the combined

  3. U-Pb ages of uraniferous opals and implications for the history of beryllium, fluorine, and uranium mineralization at Spor Mountain, Utah

    USGS Publications Warehouse

    Ludwig, K. R.; Lindsey, D.A.; Zielinski, R.A.; Simmons, K.R.

    1980-01-01

    The U-Pb isotope systematics of uraniferous opals from Spor Mountain, Utah, were investigated to determine the suitability of such material for geochronologic purposes, and to estimate the timing of uranium and associated beryllium and fluorine mineralization. The results indicate that uraniferous opals can approximate a closed system for uranium and uranium daughters, so that dating samples as young as ???1 m.y. should be possible. In addition, the expected lack of initial 230Th and 231Pa in opals permits valuable information on the initial 234U/238U to be obtained on suitable samples of ???10 m.y. age. The oldest 207Pb/235U apparent age observed, 20.8 ?? 1 m.y., was that of the opal-fluorite core of a nodule from a beryllium deposit in the Spor Mountain Formation. This age is indistinguishable from that of fission-track and K-Ar ages from the host rhyolite, and links the mineralization to the first episode of alkali rhyolite magmatism and related hydrothermal activity at Spor Mountain. Successively younger ages of 13 m.y. and 8-9 m.y. on concentric outer zones of the same nodule indicate that opal formed either episodically or continuously for over 10 m.y. Several samples of both fracture-filling and massive-nodule opal associated with beryllium deposits gave 207Pb/235U apparent ages of 13-16 m.y., which may reflect a restricted period of mineralization or perhaps an averaging of 21- and <13-m.y. periods of opal growth. Several samples of fracture-filling opal in volcanic rocks as young as 6 m.y. gave 207Pb/235U ages of 3.4-4.8 m.y. These ages may reflect hot-spring activity after the last major eruption of alkali rhyolite. ?? 1980.

  4. Image segmentation for uranium isotopic analysis by SIMS: Combined adaptive thresholding and marker controlled watershed approach

    SciTech Connect

    Willingham, David G.; Naes, Benjamin E.; Heasler, Patrick G.; Zimmer, Mindy M.; Barrett, Christopher A.; Addleman, Raymond S.

    2016-05-31

    A novel approach to particle identification and particle isotope ratio determination has been developed for nuclear safeguard applications. This particle search approach combines an adaptive thresholding algorithm and marker-controlled watershed segmentation (MCWS) transform, which improves the secondary ion mass spectrometry (SIMS) isotopic analysis of uranium containing particle populations for nuclear safeguards applications. The Niblack assisted MCWS approach (a.k.a. SEEKER) developed for this work has improved the identification of isotopically unique uranium particles under conditions that have historically presented significant challenges for SIMS image data processing techniques. Particles obtained from five NIST uranium certified reference materials (CRM U129A, U015, U150, U500 and U850) were successfully identified in regions of SIMS image data 1) where a high variability in image intensity existed, 2) where particles were touching or were in close proximity to one another and/or 3) where the magnitude of ion signal for a given region was count limited. Analysis of the isotopic distributions of uranium containing particles identified by SEEKER showed four distinct, accurately identified 235U enrichment distributions, corresponding to the NIST certified 235U/238U isotope ratios for CRM U129A/U015 (not statistically differentiated), U150, U500 and U850. Additionally, comparison of the minor uranium isotope (234U, 235U and 236U) atom percent values verified that, even in the absence of high precision isotope ratio measurements, SEEKER could be used to segment isotopically unique uranium particles from SIMS image data. Although demonstrated specifically for SIMS analysis of uranium containing particles for nuclear safeguards, SEEKER has application in addressing a broad set of image processing challenges.

  5. Measurements of (234)U and (238)U in hair, urine, and drinking water among drilled bedrock well water users for the evaluation of hair as a biomonitor of uranium intake.

    PubMed

    Israelsson, Axel; Pettersson, Håkan

    2014-08-01

    Hair is evaluated and compared with urine as a biomonitor for human intake of uranium. Concentrations of U and U and the activity ratio between them are measured in the hair, urine, and drinking water of 24 drilled bedrock well water users in Östergötland, Sweden. The samples are measured with α-spectrometry after radiochemical preparation using liquid-liquid separation with tributylphosphate. The results show that there is a stronger correlation between the uranium concentrations in the drinking water of each subject and the hair of the subject (r = 0.50) than with the urine (r = 0.21). There is also a stronger correlation between the activity ratios of water and hair (r = 0.91) than between water and urine (r = 0.56). These results imply that hair may serve as a robust indicator of chronic uranium intake. One obvious advantage over sampling urine is that hair samples reflect a much longer excretion period: weeks compared to days. The absorbed fraction of uranium, the f value, is calculated as the ratio between the excreted amount of uranium in urine and hair per day and the daily drinking water intake of uranium. The f values stretch from 0.002 to 0.10 with a median of 0.023.

  6. Rapid time scales of basalt to andesite differentiation at Anatahan volcano, Mariana Islands

    NASA Astrophysics Data System (ADS)

    Reagan, Mark; Tepley, Frank J.; Gill, James B.; Wortel, Matthew; Hartman, Brian

    2005-08-01

    We present comprehensive U-series data ( 238U- 234U- 230Th- 226Ra- 210Pb- 210Po and ( 230Th)/( 232Th)) for an andesite from an oceanic arc. The juvenile Anatahan andesite has U-Th systematics colinear with other historical Mariana volcanic rocks, and is most similar to those of the other volcano in the Mariana arc with a significant proportion of silicic andesite: Uracas. Like Uracas, the parental basalt for the Anatahan andesite was generated by relatively low degrees of flux melting from a source previously enriched in a sediment component from the subducting slab. However, the Anatahan andesite is much more strongly enriched in 226Ra over 230Th than Uracas lavas, and has one of the highest ( 226Ra)/( 232Th) ratios of siliceous andesites globally. The long-lived disequilibria between 238U- 230Th- 226Ra in the Anatahan andesite are inherited from basalt genesis, not created during differentiation or eruption. Thus, the time between genesis of the parental basalt and eruption of andesite at Anatahan is shorter than for Uracas. Moreover, the near-equilibrium ( 210Pb)/( 226Ra) value indicates that the magma body did not persistently lose or gain 222Rn for more than 2 years before eruption. This permits differentiation of the parental basalt to form andesite within this 2-year time period, although a differentiation time period between 100 and a few thousand years also is possible. The relative activities between 210Po and 210Pb suggest erupted scoria degassed Po less than most lavas despite eruption plume heights of ˜10 km, which further suggests an unusually rapid ascent before eruption. These data also show that juvenile material was ejected from the first day of the eruption. Phreatomagmatic ejecta overlying the main Anatahan scoria is strongly enriched in 210Po over 210Pb, indicating that a significant proportion of the Po degassed from rising magmas sublimes in its shallow fumarolic conduit system.

  7. Fluxes of metals to a manganese nodule: Radiochemical, chemical, structural, and mineralogical studies

    USGS Publications Warehouse

    Moore, W.S.; Ku, T.-L.; Macdougall, J.D.; Burns, V.M.; Burns, R.; Dymond, J.; Lyle, M.W.; Piper, D.Z.

    1981-01-01

    Fluxes of metals to the top and bottom surfaces of a manganese nodule were determined by combining radiochemical (230Th, 231Pa, 232Th, 238U, 234U) and detailed chemical data. The top of the nodule had been growing in its collected orientation at 4.7 mm Myr-1 for at least 0.5 Myr and accreting Mn at 200 ??g cm-2 kyr-1. The bottom of the nodule had been growing in its collected orientation at about 12 mm Myr-1 for at least 0.3 Myr and accreting Mn at about 700 ??g cm-2 yr-1. Although the top of the nodule was enriched in iron relative to the bottom, the nodule had been accreting Fe 50% faster on the bottom. 232Th was also accumulating more rapidly in the bottom despite a 20-fold enrichment of 230Th on the top. The distribution of alpha-emitting nuclides calculated from detailed radiochemical measurements matched closely the pattern revealed by 109-day exposures of alpha-sensitive film to the nodule. However, the shape and slope of the total alpha profile with depth into the nodule was affected strongly by 226Ra and 222Rn migrations making the alpha-track technique alone an inadequate method of measuring nodule growth rates. Diffusion of radium in the nodule may have been affected by diagenetic reactions which produce barite, phillipsite and todorokite within 1 mm of the nodule surface; however, our sampling interval was too broad to document the effect. We have not been able to resolve the importance of nodule diagenesis on the gross chemistry of the nodule. ?? 1981.

  8. Radionuclide concentrations in raw and purified phosphoric acids from Brazil and their processing wastes: implications for radiation exposures.

    PubMed

    da Conceição, Fabiano Tomazini; Antunes, Maria Lúcia Pereira; Durrant, Steven F

    2012-02-01

    Radionuclides from the U and Th natural series are present in alkaline rocks, which are used as feedstock in Brazil for the production of raw phosphoric acid, which can be considered as a NORM (naturally occurring radioactive material). As a result of the purification of raw phosphoric acid to food-grade phosphoric acid, two by-products are generated, i.e., solid and liquid wastes. Taking this into account, the main aim of this study was to evaluate the fluxes of natural radionuclide in the production of food-grade phosphoric acids in Brazil, to determine the radiological impact caused by ingestion of food-grade phosphoric acid, and to evaluate the solid waste environmental hazards caused by its application in crop soils. Radiological characterization of raw phosphoric acid, food-grade phosphoric acid, solid waste, and liquid waste was performed by alpha and gamma spectrometry. The (238)U, (234)U, (226)Ra, and (232)Th activity concentrations varied depending on the source of raw phosphoric acid. Decreasing radionuclides activity concentrations in raw phosphoric acids used by the producer of the purified phosphoric acid were observed as follows: Tapira (raw phosphoric acid D) > Catalão (raw phosphoric acids B and C) > Cajati (raw phosphoric acid A). The industrial purification process produces a reduction in radionuclide activity concentrations in food-grade phosphoric acid in relation to raw phosphoric acid produced in plant D and single raw phosphoric acid used in recent years. The most common use of food-grade phosphoric acid is in cola soft drinks, with an average consumption in Brazil of 72 l per person per year. Each liter of cola soft drink contains 0.5 ml of food-grade phosphoric acid, which gives an annual average intake of 36 ml of food-grade phosphoric acid per person. Under these conditions, radionuclide intake through consumption of food-grade phosphoric acid per year per person via cola soft drinks is not hazardous to human health in Brazil

  9. Using U-series Isotopes To Determine Sources Of Pedogenic Carbonates: Comparison Of Natural And Agricultural Soils In The Semi-arid Southern New Mexico And Western Texas

    NASA Astrophysics Data System (ADS)

    Nyachoti, S. K.; Ma, L.; Borrok, D. M.; Jin, L.; Tweedie, C. E.

    2012-12-01

    Pedogenic carbonates commonly precipitate from infiltrating soil water in arid and semi-arid lands and are observed in soils of southern New Mexico and western Texas. These carbonates could form an impermeable layer in the soil horizons impairing water infiltration, thus affecting crop growth and yield. It is important to determine the source of C and Ca in these carbonates and to understand conditions favoring their formation, kinetics and precipitation rates. In this study, major elements and U-series isotopes in bulk calcic soils, and weak acid leachates and residues were measured from one irrigated alfalfa site in the Hueco basin near El Paso, TX and one natural shrubland site on the USDA Jornada experimental range in southern NM. The combined geochemical and isotopic results allow us to determine the formation ages of the carbonates; investigate the mobility of U, Th, and major elements in these soils; and infer for the effects of irrigation on carbonate formation in agricultural soils. Our results show distinctive U and Th isotope systems in the two soil profiles analyzed. For example, (234U/238U) ratios in the Jornada bulk soils decrease from ~1.01 to 0.96 towards the surface, consistent with a preferential loss of 234U over 238U during chemical weathering. At the Jornada site, (238U/232Th) ratios decrease while (230Th/238U) increase towards the surface, consistent with a general depletion of U and the immobility of Th in the natural soils. By contrast at the Alfalfa site, (234U/238U) ratios of bulk soils increase from ~ 0.97 to 1.02 towards the surface, suggesting an additional source of external uranium, most likely the irrigation water from Rio Grande which has a (234U/238U) ratio of ~ 1.5 near El Paso. The (238U/232Th) and (230Th/238U) ratios also imply leaching of U from shallower soils but precipitation in greater depths at Alfalfa site; suggests that partial dissolution and re-precipitation of younger carbonates occur. Calculated carbonate ages from U

  10. Anthropogenic and geogenic radionuclides content in an undisturbed Slovenian forest soil

    NASA Astrophysics Data System (ADS)

    P, Jankong; L, Mabit; A, Toloza; v, Zupanc

    2010-05-01

    The measurements of natural background radiation and anthropogenic radionuclides in terrestrial environment, especially in soil, have been carried out in many countries for several decades to establish base line data of radiation level. So far, the knowledge of radionuclides concentration levels in Slovenia is limited to a few investigations and the use of anthropogenic 137Cs radionuclide has not yet been used as soil landscape tracer in Slovenia. Therefore, the purposes of this study were: (i) to collect the inventory information of naturally occurring isotope (40K, 226Ra, 232Th, 235U and 238U) and man-made radionuclides (137Cs) as well as their depth/vertical distribution in soil; (ii) to complete radio-ecological survey information in Slovenia and provide information regarding the external dose-rate based on the depth distributions of the gamma emitters in the soil of the study area; and (iii) to establish a reference inventory value of 137Cs fallout in order to prepare for a future investigation to test 137Cs as soil tracer under Slovenian agro-environment. To estimate the natural level of radioactivity and the initial fallout of 137Cs, twenty soil profiles (0-40cm) divided into four increments of 10 cm were collected in an undisturbed forest located in East Slovenia in Šalamenci close to the Hungarian and Austrian borders at the beginning of the Pannonian plains. Depending on the depth increment, the average activity concentration of 137Cs, 40K, 226Ra, 232Th, 235U and 238U were found to be respectively from 0.47 ± 0.27 to 70 ± 33 Bq kg-1, from 535 ± 16 to 703 ± 20 Bq kg-1, from 51 ± 3 to 49 ± 2 Bq kg-1, from 54 ± 6 to 62 ± 4 Bq kg-1, from 7.8 ± 0.8 to 8.1 ± 0.3 Bq kg-1and from 58 ± 22 to 68 ± 27 Bq kg-1. On average the top soil mass activity of 40K is 7 to 8 times higher than that of 137Cs and the depth distribution of this isotope, instead of showing a constant amount along the soil profile, presents an increase with depth. The external gamma

  11. Letter Report: Looking Ahead at Nuclear Fuel Resources

    SciTech Connect

    J. Stephen Herring

    2013-09-01

    The future of nuclear energy and its ability to fulfill part of the world’s energy needs for centuries to come depend on a reliable input of nuclear fuel, either thorium or uranium. Obviously, the present nuclear fuel cycle is completely dependent on uranium. Future thorium cycles will also depend on 235U or fissile isotopes separated from used fuel to breed 232Th into fissile 233U. This letter report discusses several emerging areas of scientific understanding and technology development that will clarify and enable assured supplies of uranium and thorium well into the future. At the most fundamental level, the nuclear energy community needs to appreciate the origins of uranium and thorium and the processes of planetary accretion by which those materials have coalesced to form the earth and other planets. Secondly, the studies of geophysics and geochemistry are increasing understanding of the processes by which uranium and thorium are concentrated in various locations in the earth’s crust. Thirdly, the study of neutrinos and particularly geoneutrinos (neutrinos emitted by radioactive materials within the earth) has given an indication of the overall global inventories of uranium and thorium, though little indication for those materials’ locations. Crustal temperature measurements have also given hints of the vertical distribution of radioactive heat sources, primarily 238U and 232Th, within the continental crust. Finally, the evolving technologies for laser isotope separation are indicating methods for reducing the energy input to uranium enrichment but also for tailoring the isotopic vectors of fuels, burnable poisons and structural materials, thereby adding another tool for dealing with long-term waste management.

  12. Study of calculated and measured time dependent delayed neutron yields. [TX, for calculating delayed neutron yields; MATINV, for matrix inversion; in FORTRAN for LSI-II minicomputer

    SciTech Connect

    Waldo, R.W.

    1980-05-01

    Time-dependent delayed neutron emission is of interest in reactor design, reactor dynamics, and nuclear physics studies. The delayed neutrons from neutron-induced fission of /sup 232/U, /sup 237/Np, /sup 238/Pu, /sup 241/Am, /sup 242m/Am, /sup 245/Cm, and /sup 249/Cf were studied for the first time. The delayed neutron emission from /sup 232/Th, /sup 233/U, /sup 235/U, /sup 238/U, /sup 239/Pu, /sup 241/Pu, and /sup 242/Pu were measured as well. The data were used to develop an empirical expression for the total delayed neutron yield. The expression gives accurate results for a large variety of nuclides from /sup 232/Th to /sup 252/Cf. The data measuring the decay of delayed neutrons with time were used to derive another empirical expression predicting the delayed neutron emission with time. It was found that nuclides with similar mass-to-charge ratios have similar decay patterns. Thus the relative decay pattern of one nuclide can be established by any measured nuclide with a similar mass-to-charge ratio. A simple fission product yield model was developed and applied to delayed neutron precursors. It accurately predicts observed yield and decay characteristics. In conclusion, it is possible to not only estimate the total delayed neutron yield for a given nuclide but the time-dependent nature of the delayed neutrons as well. Reactors utilizing recycled fuel or burning actinides are likely to have inventories of fissioning nuclides that have not been studied until now. The delayed neutrons from these nuclides can now be incorporated so that their influence on the stability and control of reactors can be delineated. 8 figures, 39 tables.

  13. Uranium and radium diffusion in organic-rich sediments (sapropels)

    NASA Astrophysics Data System (ADS)

    Gourgiotis, A.; Reyss, J.-L.; Frank, N.; Guihou, A.; Anagnostou, C.

    2011-09-01

    Among the late Quaternary Mediterranean sapropels, the S5 (125 ka) is one of the best preserved due to its high organic carbon content that has limited postdepositional oxidation. The high uranium content in this sapropel, >40 dpm g-1, makes this layer interesting for studying uranium series disequilibrium in organic-rich sediments. For this reason, the present work provides isotopic measurements of the U decay series in a S5 sapropel by applying more precise mass spectrometric methods, TIMS/MC-ICPMS, and gamma spectrometry. Assuming that U in the sapropel mostly originated from seawater the (234U/238U), (230Th/238U), (226Ra/230Th) and (231Pa/235U) activity ratios show systematic deviations from the theoretical values for a closed-system evolution of the U series over the 125 ka since sapropel formation. The radiogenic 234Urad and 226Ra show clear evidence of migration in the sapropel with modeled diffusion coefficients of (7.1 ± 1.1) × 10-12 cm2 s-1 and (1.6 ± 0.2) × 10-10 cm2 s-1, respectively. The diffusion of 234Urad cannot explain the high (230Th/238U) and (231Pa/235U) activity ratios observed in the sapropel. Two possible mechanisms or a combination of both are proposed for explaining the irregular (230Th/238U) and (231Pa/235U) activity profiles in sapropel S5. The first one is an enhanced export flux of 230Thxs and 231Paxs excesses exceeding the production rate in seawater, during the time of sapropel formation, and the second one is diffusion of authigenic Uauth in the sapropel. However, the ambiguous determination of 230Thxs and 231Paxs in the sapropel and the poorly understood processes that might lead to Uauth migration in anoxic sediments still limit a final explanation for the deviation of (230Th/238U) and (231Pa/235U) activity ratios from their expected theoretical values.

  14. Theoretical studies of {sup 238}U-{sup 230}Th-{sup 226}Ra and {sup 235}U-{sup 231}Pa disequilibria in young lavas produced by mantle melting

    SciTech Connect

    Zou, H.; Zindler, A.

    2000-05-01

    This paper provides ready-to-use equations to describe variations in uranium-series (U-series) disequilibrium as a function of elemental distribution coefficients, melting porosity, melting rate, and melting time. The effects of these melting parameters on U-series disequilibria are quantitatively evaluated in both an absolute and relative sense. The importance of net elemental fractionation and ingrowth of daughter nuclides are also described and compared in terms of their relative contributions to total U-series disequilibrium. In addition, the authors compare the production of U-series disequilibrium during mantle melting to trace element fractionations produced by melting in a similar context. Trace element fractionations depend externally on the degree to which a source is melted, whereas U-series disequilibrium depends upon both the degree and rate of melting. In contrast to previous models, their approach to modeling U-series disequilibrium during dynamic melting collapses simply to a description of trace element behavior during dynamic melting when the appropriate decay terms are omitted. Their formulation shows that extremely small degrees of melting, sometimes called upon to explain observed extents of U-series disequilibrium, are not always required.

  15. Applications of New Synthetic Uranium Reference Materials for Research in Geochemistry

    NASA Astrophysics Data System (ADS)

    Richter, Stephan; Alonso, Adolfo; Aregbe, Yetunde; Eykens, Roger; Jacobsson, Ulf; Kuehn, Heinz; Verbruggen, Andre; Weyer, Stefan

    2010-05-01

    For many applications in geochemistry research isotope ratio measurements play a significant role. In geochronology isotope abundances of uranium and its daughter products thorium and lead are being used to determine the age and history of various samples of geological interest. For measuring the isotopic compositions of these elements by mass spectrometry, suitable isotope reference materials are needed to validate measurement procedures and to calibrate multi-collector and ion counting detector systems. IRMM is a recognized provider for nuclear isotope reference materials to the nuclear industry and nuclear safeguards authorities, which are also being applied widely for geochemical applications. Firstly, the double spike IRMM-3636 with a 233U/236U ratio of 1:1 was prepared which allows internal mass fractionation correction for high precision 235U/238U ratio measurements. The 234U abundance of this double spike material is low enough to allow an accurate and precise correction of 234U/238U ratios, even for measurements of close to equilibrium uranium samples. The double spike IRMM-3636 is offered in 3 concentrations: 1mg/g, 0.1mg/g and 0.005mg/g. Secondly, the 236U single spike IRMM-3660 was prepared and is offered in 3 concentrations: 1mg/g, 0.1mg/g and 0.01mg/g. Thirdly, a "Quad"-isotope reference material, IRMM-3101, has been prepared which is characterized by 233U/235U/236U/238U=1/1/1/1. This material is useful for checking Faraday cup efficiencies and inter-calibration of MIC (multiple ion counting) detectors. The quad-IRM is offered in 3 concentrations: 1mg/g, 0.1mg/g and 0.01mg/g. As one example for the significant influence of synthetic reference materials for geochemical research, the IRMM-074 series of gravimetrically prepared uranium mixtures for linearity testing of secondary electron multipliers (SEMs) has been applied for the redetermination of the secular equilibrium 234U/238U value and the 234U half-life by Cheng et al (2009). Due to the use of

  16. Lead Slowing Down Spectrometer FY2013 Annual Report

    SciTech Connect

    Warren, Glen A.; Kulisek, Jonathan A.; Gavron, Victor A.; Danon, Yaron; Weltz, Adam; Harris, Jason; Stewart, T.

    2013-10-29

    Executive Summary The Lead Slowing Down Spectrometry (LSDS) project, funded by the Materials Protection And Control Technology campaign, has been evaluating the feasibility of using LSDS techniques to assay fissile isotopes in used nuclear fuel assemblies. The approach has the potential to provide considerable improvement in the assay of fissile isotopic masses in fuel assemblies compared to other non-destructive techniques in a direct and independent manner. This report is a high level summary of the progress completed in FY2013. This progress included: • Fabrication of a 4He scintillator detector to detect fast neutrons in the LSDS operating environment. Testing of the detector will be conducted in FY2014. • Design of a large area 232Th fission chamber. • Analysis using the Los Alamos National Laboratory perturbation model estimated the required number of neutrons for an LSDS measurement to be 10 to the 16th source neutrons. • Application of the algorithms developed at Pacific Northwest National Laboratory to LSDS measurement data of various fissile samples conducted in 2012. The results concluded that the 235U could be measured to 2.7% and the 239Pu could be measured to 6.3%. Significant effort is yet needed to demonstrate the applicability of these algorithms for used-fuel assemblies, but the results reported here are encouraging in demonstrating that we are making progress toward that goal. • Development and cost-analysis of a research plan for the next critical demonstration measurements. The plan suggests measurements on fresh fuel sub assemblies as a means to experimentally test self-attenuation and the use of fresh mixed-oxide fuel as a means to test simultaneous measurement of 235U and 239Pu.

  17. The Use of Thorium within the Nuclear Power Industry - 13472

    SciTech Connect

    Miller, Keith

    2013-07-01

    Thorium is 3 to 4 times more abundant than uranium and is widely distributed in nature as an easily exploitable resource in many countries. Unlike natural uranium, which contains ∼0.7% fissile {sup 235}U isotope, natural thorium does not contain any fissile material and is made up of the fertile {sup 232}Th isotope only. Therefore thorium and thorium-based fuel as metal, oxide or carbide, has been utilized in combination with fissile {sup 235}U or {sup 239}Pu in nuclear research and power reactors for conversion to fissile {sup 233}U, thereby enlarging fissile material resources. During the pioneering years of nuclear energy, from the mid 1950's to mid 1970's, there was considerable interest worldwide to develop thorium fuels and fuel cycles in order to supplement uranium reserves. Thorium fuels and fuel cycles are particularly relevant to countries having large thorium deposits but very limited uranium reserves for their long term nuclear power programme. The feasibility of thorium utilization in high temperature gas cooled reactors (HTGR), light water reactors (LWR), pressurized heavy water reactors (PHWRs), liquid metal cooled fast breeder reactors (LMFBR) and molten salt breeder reactors (MSBR) were demonstrated. The initial enthusiasm for thorium fuels and fuel cycles was not sustained among the developing countries later, due to new discovery of uranium deposits and their improved availability. However, in recent times, the need for proliferation-resistance, longer fuel cycles, higher burnup, and improved waste form characteristics, reduction of plutonium inventories and in situ use of bred-in fissile material has led to renewed interest in thorium-based fuels and fuel cycles. (authors)

  18. Modern U-Pb chronometry of meteorites: advancing to higher time resolution reveals new problems

    USGS Publications Warehouse

    Amelin, Y.; Connelly, J.; Zartman, R.E.; Chen, J.-H.; Gopel, C.; Neymark, L.A.

    2009-01-01

    In this paper, we evaluate the factors that influence the accuracy of lead (Pb)-isotopic ages of meteorites, and may possibly be responsible for inconsistencies between Pb-isotopic and extinct nuclide timescales of the early Solar System: instrumental mass fractionation and other possible analytical sources of error, presence of more than one component of non-radiogenic Pb, migration of ancient radiogenic Pb by diffusion and other mechanisms, possible heterogeneity of the isotopic composition of uranium (U), uncertainties in the decay constants of uranium isotopes, possible presence of "freshly synthesized" actinides with short half-life (e.g. 234U) in the early Solar System, possible initial disequilibrium in the uranium decay chains, and potential fractionation of radiogenic Pb isotopes and U isotopes caused by alpha-recoil and subsequent laboratory treatment. We review the use of 232Th/238U values to assist in making accurate interpretations of the U-Pb ages of meteorite components. We discuss recently published U-Pb dates of calcium-aluminum-rich inclusions (CAIs), and their apparent disagreement with the extinct nuclide dates, in the context of capability and common pitfalls in modern meteorite chronology. Finally, we discuss the requirements of meteorites that are intended to be used as the reference points in building a consistent time scale of the early Solar System, based on the combined use of the U-Pb system and extinct nuclide chronometers.

  19. An accurate method to measure alpha-emitting natural radionuclides in atmospheric filters: Application in two NORM industries

    NASA Astrophysics Data System (ADS)

    Lozano, R. L.; Bolívar, J. P.; San Miguel, E. G.; García-Tenorio, R.; Gázquez, M. J.

    2011-12-01

    In this work, an accurate method for the measurement of natural alpha-emitting radionuclides from aerosols collected in air filters is presented and discussed in detail. The knowledge of the levels of several natural alpha-emitting radionuclides (238U, 234U, 232Th, 230Th, 228Th, 226Ra and 210Po) in atmospheric aerosols is essential not only for a better understanding of the several atmospheric processes and changes, but also for a proper evaluation of the potential doses, which can inadvertently be received by the population via inhalation. The proposed method takes into account the presence of intrinsic amounts of these radionuclides in the matrices of the quartz filters used, as well as the possible variation in the humidity of the filters throughout the collection process. In both cases, the corrections necessary in order to redress these levels have been evaluated and parameterized. Furthermore, a detailed study has been performed into the optimisation of the volume of air to be sampled in order to increase the accuracy in the determination of the radionuclides. The method as a whole has been applied for the determination of the activity concentrations of U- and Th-isotopes in aerosols collected at two NORM (Naturally Occurring Radioactive Material) industries located in the southwest of Spain. Based on the levels found, a conservative estimation has been performed to yield the additional committed effective doses to which the workers are potentially susceptible due to inhalation of anthropogenic material present in the environment of these two NORM industries.

  20. Bioaccumulation of natural radionuclides in molluscs from the Ebro Delta area.

    PubMed

    Fonollosa, E; Peñalver, A; Aguilar, C; Borrull, F

    2017-01-01

    (210)Po, (210)Pb, (234)U, (238)U, (232)Th and (230)Th were analysed in the edible part of four different species of bivalves typically produced and consumed in the Ebro Delta area. The results show that the main contributor to the radioactive content in these species was (210)Po, with values ranging between 263.1 ± 26.6 and 813.0 ± 72.9 Bq/kg (d.w.), which are higher than the usual reported activity levels in other geographical areas. This can probably be attributed to the activities of a phosphate industrial plant located upstream on the Ebro River, which may lead to enhanced levels of naturally occurring radioactive isotopes in the aquatic ecosystem. To determine the possible impact on health, the committed effective doses through the consumption of the different species were evaluated and the cumulative total annual effective dose for their consumption was estimated to 187.6 μSv/year, which is in the range of 200-1000 μSv/year given by UNSCEAR.

  1. Determination of trace element concentrations and stable lead, uranium and thorium isotope ratios by quadrupole-ICP-MS in NORM and NORM-polluted sample leachates.

    PubMed

    Mas, J L; Villa, M; Hurtado, S; García-Tenorio, R

    2012-02-29

    This work focuses on the monitoring of the potential pollution in scenarios that involve NORM-related industrial activities (environmental or in-door scenarios). The objective was to develop a method to determine extent and origin of the contamination, suitable for monitoring (i.e. simple, fast and economical) and avoiding the use of too many different instruments. It is presented a radiochemical method that allows the determination of trace element concentrations and 206Pb/207Pb/208Pb, 238U/234U and 232Th/230Th isotope ratios using a single sample aliquot and a single instrument (ICP-QMS). Eichrom UTEVA® extraction chromatography minicolumns were used to separate uranium and thorium in sample leachates. Independent ICP-MS determinations of uranium and thorium isotope ratios were carried out afterwards. Previously a small aliquot of the leachate was used for the determination of trace element concentrations and lead isotope ratios. Several radiochemical arrangements were tested to get maximum performances and simplicity of the method. The performances of the method were studied in terms of chemical yields of uranium and thorium and removal of the potentially interfering elements. The established method was applied to samples from a chemical industry and sediments collected in a NORM-polluted scenario. The results obtained from our method allowed us to infer not only the extent, but also the sources of the contamination in the area.

  2. Heavy-Ion Transfer Reactions with Deformed Nuclei

    NASA Astrophysics Data System (ADS)

    Helmer, Karl Gerard

    1992-01-01

    One-neutron transfer reactions involving actinide nuclei are used to investigate the effects of rotational motion on transfer populations. Deexcitation gamma rays were measured using a particle -particle-gamma triple coincidence method. Rotational states up to 28^{+ }(30^{+}) were seen in ^{234}U originating from the reaction ^{235}U( ^{206}Pb, ^ {207}Pb)^{234} U at a laboratory bombarding energy of 1394 MeV. Angular distributions for both inelastic excitation and transfer are presented and the one-neutron transfer reaction cross section as well as the grazing angle have been extracted. This study demonstrates the feasibility of using heavy-ion induced transfer reactions for spectroscopic studies. The second section of this thesis explores the question of diabolical pair transfer in nuclear physics using the reactions ^{206}Pb( ^{156}Gd, ^ {154}Gd)^{208} Pb (diabolical case) and ^{206 }Pb(^{156}Gd, ^{158}Gd)^ {204}Pb (nondiabolic case) at a laboratory bombarding energy of 888 MeV. Early calculations by Nikam, Ring and Canto predicted oscillatory behavior of pair transfer matrix elements as the cranking frequency was varied, within the cranking Hartree-Fock-Bogoliubov (CHFB) model, and explained this behavior as a manifestation of Berry's phase. Significant suppression of the high spin population in the diabolical nucleus was predicted. The diabolical point is supplied by the crossing of the ground-state band with the two-quasiparticle band. The strength of this band interaction is predicted to be oscillatory with chemical potential in the CHFB model. The study of pair transfer populations can therefore shed light not only on the possible existence of Berry's phase in nuclear systems, but also on whether the band interaction goes strictly to zero as predicted by the CHFB model. The results of this experiment agree with the latest calculations that the expected effects are more subtle than the earliest calculations predicted.

  3. Applications of New Synthetic Uranium Reference Materials for Geochemistry Research (Invited)

    NASA Astrophysics Data System (ADS)

    Richter, S.; Weyer, S.; Alonso, A.; Aregbe, Y.; Kuehn, H.; Eykens, R.; Verbruggen, A.; Wellum, R.

    2009-12-01

    For many applications in geochemistry research isotope ratio measurements play a significant role. In geochronology isotope abundances of uranium and its daughter products thorium and lead are being used to determine the age and history of various samples of geological interest. For measuring the isotopic compositions of these elements by mass spectrometry, suitable isotope reference materials are needed to validate measurement procedures and to calibrate multi-collector and ion counting detector systems. IRMM is a recognized provider for nuclear isotope reference materials to the nuclear industry and nuclear safeguards authorities, which are also being applied widely for geochemical applications. The preparation of several new synthetic uranium reference materials at IRMM during the recent five years has provided significant impacts on geochemical research. As an example, the IRMM-074 series of gravimetrically prepared uranium mixtures for linearity testing of secondary electron multipliers (SEMs) has been applied for the redetermination of the secular equilibrium 234U/238U value and the 234U half-life by Cheng et al (2009). Due to the use of IRMM-074, results with smaller uncertainties were obtained, which are shifted by about 0.04% compared to the commonly used values published earlier by Cheng et al. in 2000. This has a significant impact for U isotope measurements in geochemistry.. As a further example, the new double spike IRMM-3636 with a 233U/236U ratio of 1:1 and an expanded uncertainty as low as 0.016% (coverage factor k=2, 95% confidence level) was prepared gravimetrically. This double spike allows internal mass fractionation correction for high precision 235U/238U ratio measurements of close to natural samples. Using the new double spike IRMM-3636, the 235U/238U ratios for several commonly used natural U standard materials from NIST/NBL and IRMM, such as e.g. NBS960 (=NBL CRM-112a), NBS950a,b and IRMM-184, have been re-measured with improved precision

  4. Nuclear data verification based on Monte Carlo simulations of the LLNL pulsed-sphere benchmark experiments (1979 & 1986) using the Mercury code

    SciTech Connect

    Descalle, M; Pruet, J

    2008-06-09

    Livermore's nuclear data group developed a new verification and validation test suite to ensure the quality of data used in application codes. This is based on models of LLNL's pulsed sphere fusion shielding benchmark experiments. Simulations were done with Mercury, a 3D particle transport Monte Carlo code using continuous-energy cross-section libraries. Results were compared to measurements of neutron leakage spectra generated by 14MeV neutrons in 17 target assemblies (for a blank target assembly, H{sub 2}O, Teflon, C, N{sub 2}, Al, Si, Ti, Fe, Cu, Ta, W, Au, Pb, {sup 232}Th, {sup 235}U, {sup 238}U, and {sup 239}Pu). We also tested the fidelity of simulations for photon production associated with neutron interactions in the different materials. Gamma-ray leakage energy per neutron was obtained from a simple 1D spherical geometry assembly and compared to three codes (TART, COG, MCNP5) and several versions of the Evaluated Nuclear Data File (ENDF) and Evaluated Nuclear Data Libraries (ENDL) cross-section libraries. These tests uncovered a number of errors in photon production cross-sections, and were instrumental to the V&V of different cross-section libraries. Development of the pulsed sphere tests also uncovered the need for new Mercury capabilities. To enable simulations of neutron time-of-flight experiments the nuclear data group implemented an improved treatment of biased angular scattering in MCAPM.

  5. Radioactivity concentrations in soil and vegetables from the northern Jordan Rift Valley and the corresponding dose estimates.

    PubMed

    Ababneh, Anas M; Masa'deh, Maisoun S; Ababneh, Zaid Q; Awawdeh, Mufeed A; Alyassin, Abdalmajeid M

    2009-02-01

    The Jordan Rift Valley (JRV) is considered the food bowl of Jordan, especially during the winter season. In this study, soil and vegetable samples collected from greenhouses in the northern JRV were analysed for their radioactive content. The activity concentrations of (238)U, (235)U, (232)Th, (226)Ra, (137)Cs and (40)K in soil were found to be (+/-SD) 33 +/- 12, 2.2 +/- 0.7, 11.2 +/- 3.3, 40.5 +/- 15.5, 3.5 +/- 1.3 and 156.0 +/- 46.6 (Bq kg(-1)), respectively. In vegetables, the activity concentration of (40)K was found in the range of 698-1439 Bq kg(-1), while those of (226)Ra and (228)Ra were found to be in the range of <0.61-2.56 and <0.69-3.35 Bq kg(-1), respectively. Transfer factors for (40)K were found to be high and ranged from 5 to 8, while those for (226)Ra and (228)Ra were found to be from <0.01 to 0.07 and from <0.09 to 0.42, respectively. The calculated external annual effective dose is found to be within the worldwide range.

  6. Survey of natural and anthropogenic radioactivity in environmental samples from Yugoslavia.

    PubMed

    Esposito, M; Polić, P; Bartolomei, P; Benzi, V; Martellini V; Cvetković, O; Damjanov, V; Simić, M; Zunić, Z; Zivancević, B; Simić, S; Jovanović, V

    2002-01-01

    The radioactivity of 238U, 226Ra, 232Th, 40K and 137Cs in sediments, soil, turf and honey from Serbia and Kosovo (Yugoslavia) was measured using gamma and alpha spectrometry in order to estimate the radiation hazard from natural and man-made sources, as well as to compile a database for radioactivity levels in those regions. One sample, collected in the vicinity of a "depleted uranium" (DU) shell of the recent Balkan war, revealed a high 238U activity and a non-natural 235U/238U activity ratio, confirming therefore its anthropogenic origin. However, some other soil samples coming from characteristic DU craters did not show any characteristic level of radioactivity. The other sediment and turf samples taken all around the country show low radioactivity levels for all the isotopes here considered. With the aim of obtaining some indication about radioactivity migration in the food chain, several honey samples have been examined too. All samples show very low radioactivity content, often indistinguishable from natural background.

  7. The evaluation of half-lives and other decay data used in nuclear astrophysics and cosmochronology

    SciTech Connect

    Chechev, V. P.

    2011-12-15

    The current status of some decay data used in nuclear astrophysics and cosmochronology is presented. The half-life of {sup 79}Se has been evaluated as 3.6(3) Multiplication-Sign 10{sup 5} yr. The total energy of non-neutrino radiation released in act of {sup 37}Ar decay has been obtained being 2.709 (16) keV per disintegration. The recommended half-life values of the long-lived radionuclides (T{sub 1/2} Greater-Than-Or-Equivalent-To 10{sup 6} yr) of {sup 26}Al, {sup 40}K, {sup 53}Mn, {sup 60}Fe, {sup 87}Rb, {sup 93}Zr, {sup 98}Tc, {sup 107}Pd, {sup 129}I, {sup 135}Cs, {sup 146}Sm, {sup 176}Lu, {sup 182}Hf, {sup 187}Re, {sup 205}Pb, {sup 232}Th, {sup 235}U, {sup 238}U, {sup 244}Pu, and {sup 247}Cm are given based on the evaluations published until 2010.

  8. Radioactivity as a significant energy source in prebiotic synthesis.

    PubMed

    Garzón, L; Garzón, M L

    2001-01-01

    Radioactivity in the continental crust (due mainly to the isotopes 238U, 235U, 232Th and 40K), as a energy source for chemical evolution in the early Archean (between 3.5 and approximately 4 Ga bp), is reviewed. The most important radioactive source in the continental crust is due to the production and accumulation of radioactive gases within the crust voids (porosity). The study of such mechanism has allowed us to reach a deeper understanding about the nature of the radioactive source and to describe its behavior, particularly with regard to prebiotic chemical evolution. An effective total energy of 3 x 10(18) Ja-1 has been obtained for a depth of 1 km, 4 Ga ago. If a depth of 30 km is taken, the obtained value is almost equal to the UV solar energy radiation (lambda < 150 nm). Within the voids the radioactive source of the continental crust played a relevant role in prebiotic synthesis. In uranium deposits of the same age, the role of radioactivity must have been even more relevant in favoring chemical evolution.

  9. The impact of accretion material composition and properties on interior structure dynamics of Kuiper belt objects

    NASA Astrophysics Data System (ADS)

    Shchuko, Oleg; Shchuko, Svetlana D.; Kartashov, Daniil; Orosei, Roberto

    The building material of the forming Kuiper belt objects is supposed in the model to consist of solid dust material of protosolar cloud fringe regions and H2 O amorphous ice. A spheri-cally symmetric celestial body was being created as a result of accretion. The body's internal structure was determined by the composition and the properties of the accretion material and the evolution of the structure -by internal thermal processes. The accretion material compo-sition and structure have been studied, which provide now the existence of large icy Kuiper belt objects. Radionuclides 26 Al, 40 K, 232 Th, 235 U and 238 U embedded in solid dust matter particles have been main sources of radiogenic heat for the Kuiper belt object life time. The impact of the heat-and-power potentials of radiogenic heat sources on H2 O phase transition dynamics in the celestial body matter has been investigated. The parameter variation domains of these potentials have been found at which there can be formed areas partly or fully filled with H2 O of different phase states. In addition, the dynamic boundaries of areas have been determined where the ice component is presented by amorphous ice or cubic and hexagonal crystal ice. The parameter domains of celestial body accretion and radiogenic heat processes have been determined where the body evolution may have a catastrophic scenario up to its complete destruction.

  10. Radiolytic Hydrogen Production in the South Pacific Subseafloor Basaltic Aquifer

    NASA Astrophysics Data System (ADS)

    Dzaugis, M. E.; Spivack, A. J.; Dunlea, A. G.; Murray, R. W.; D'Hondt, S.

    2015-12-01

    Hydrogen (H2) is produced in geological settings by dissociation of water due to radiation from natural radioactive decay of uranium (238U, 235U), thorium (232Th) and potassium (40K). To quantify the potential significance of radiolytic H2 as an electron donor for microbes within the South Pacific subseafloor basaltic aquifer, we calculate radiolytic H2 production rates in basement fractures utilizing measured radionuclide concentrations in 42 basalt samples from IODP Expedition 329. The samples are from three sites with very different basement ages and a wide range of alteration types. Major and trace element concentrations vary by up to an order of magnitude from sample to sample. Comparison of our samples to each other and to previous studies of fresh East Pacific Rise basalt suggests that between-sample variation in radionuclide concentrations is primarily due to differences in initial (pre-alteration) concentrations (which can vary between eruptive events), rather than to alteration type or extent. Local maxima in radionuclide (U, Th, and K) concentrations produce 'hotspots' of radiolytic H2 production; calculated radiolytic rates differ by up to a factor of 80 from sample to sample. Fracture width also greatly influences H2 production. Due to the low penetration distance of alpha radiation, microfractures are 'hotpots' for radiolytic H2 production. For example, radiolytic H2 production rates normalized to water volume are 170 times higher in 1μm-wide fractures than in 10cm-wide fractures.

  11. Radiological impact of natural radioactivity in Egyptian phosphate rocks, phosphogypsum and phosphate fertilizers.

    PubMed

    El-Bahi, S M; Sroor, A; Mohamed, Gehan Y; El-Gendy, N S

    2017-05-01

    In this study, the activity concentrations of the natural radionuclides in phosphate rocks and its products were measured using a high- purity germanium detector (HPGe). The obtained activity results show remarkable wide variation in the radioactive contents for the different phosphate samples. The average activity concentration of (235)U, (238)U, (226)Ra, (232)Th and (40)K was found as (45, 1031, 786, 85 and 765Bq/kg) for phosphate rocks, (28, 1234, 457, 123 and 819Bq/kg) for phosphate fertilizers, (47, 663, 550, 79 and 870Bq/kg) for phosphogypsum and (25, 543, 409, 54 and 897Bq/kg) for single super phosphate respectively. Based on the measured activities, the radiological parameters (activity concentration index, absorbed gamma dose rate in outdoor and indoor and the corresponding annual effective dose rates and total excess lifetime cancer risk) were estimated to assess the radiological hazards. The total excess lifetime cancer risk (ELCR) has been calculated and found to be high in all samples, which related to high radioactivity, representing radiological risk for the health of the population.

  12. Implementation of neural networks for classification of moss and lichen samples on the basis of gamma-ray spectrometric analysis.

    PubMed

    Dragović, Snezana; Onjia, Antonije; Dragović, Ranko; Bacić, Goran

    2007-07-01

    Mosses and lichens have an important role in biomonitoring. The objective of this study is to develop a neural network model to classify these plants according to geographical origin. A three-layer feed-forward neural network was used. The activities of radionuclides ((226)Ra, (238)U, (235)U, (40)K, (232)Th, (134)Cs, (137)Cs and (7)Be) detected in plant samples by gamma-ray spectrometry were used as inputs for neural network. Five different training algorithms with different number of samples in training sets were tested and compared, in order to find the one with the minimum root mean square error. The best predictive power for the classification of plants from 12 regions was achieved using a network with 5 hidden layer nodes and 3,000 training epochs, using the online back-propagation randomized training algorithm. Implementation of this model to experimental data resulted in satisfactory classification of moss and lichen samples in terms of their geographical origin. The average classification rate obtained in this study was (90.7 +/- 4.8)%.

  13. Numerical Study on Effects of Fuel Mixture Fraction and Li-6 Enrichment on Neutronic Parameters of a Fusion-Fission Hybrid Reactor

    NASA Astrophysics Data System (ADS)

    Yapııcıı, Hüseyin; Genç, Gamze; Demir, Nesrin

    2004-09-01

    This study presents the effects of mixture fractions of nuclear fuels (mixture of fissile-fertile fuels and mixture of two different fertile fuels) and 6Li enrichment on the neutronic parameters (the tritium breeding ratio, TBR, the fission rate, FR, the energy multiplication ratio, M, the fissile breeding rate, FBR, the neutron leakage out of blanket, L, and the peak-to-average fission power density ratio, Γ) of a deuterium-tritium (D-T) fusion neutron-driven hybrid blanket. Three different fertile fuels (232Th, 238U and 244Cm), and one fissile fuel (235U) were selected as the nuclear fuel. Two different coolants (pressurized helium and natural lithium) were used for the nuclear heat transfer out of the fuel zone (FZ). The Boltzmann transport equation was solved numerically for obtaining the neutronic parameters with the help of the neutron transport code XSDRNPM/SCALE4.4a. In addition, these calculations were performed by also using the MCNP4B code. The sub-limits of the mixture fractions and 6Li enrichment were determined for the tritium self-sufficiency. The considered hybrid reactor can be operated in a self-sufficiency mode in the cases with the fuel mixtures mixed with a fraction of equal to or greater than these sub-limits. Furthermore, the numerical results show that the fissile fuel breeding and fission potentials of the blankets with the helium coolant are higher than with the lithium coolant.

  14. Environmental radioactivity measurements and applications - Difficulties, current status and future trends

    NASA Astrophysics Data System (ADS)

    Anagnostakis, Marios J.

    2015-11-01

    For several decades natural and artificial radioactivity in the environment have been extensively studied all around the world. Nuclear accidents - mainly that of Chernobyl - have led to the development of the field of radioecology, while detector systems and techniques - with predominant that of γ-spectrometry - have been continuously developed through the years to meet researchers' needs. The study of natural radionuclides that was originally limited to 226Ra, 232Th and 40K was then extended to include radionuclides such as 234Th, 210Pb, 235U and 7Be, which allowed the study of radioactive equilibrium. Besides their importance from the radiation protection point of view, many radionuclides are also used as tracers of environmental processes, such as aerosol and transportation of air masses studies (7Be, 10Be, 22Na), soil erosion, sedimentation and geochronology (210Pb, 137Cs), marine ecosystems studies and studies related to climate change. All these studies require specialized samplings strategies and sampling preparation techniques as well as high quality measurements, while the improvement of detection limits is often of vital importance. This work is a review of environmental radioactivity measurements and applications, mainly focused in the field of γ-spectrometry, for which difficulties and limitations will be presented, together with future trends, new challenges and applications.

  15. The fission track detector revisited: application to individual neutron dosimetry.

    PubMed

    Prêtre, S; Aroua, A; Boschung, M; Grecescu, M; Valley, J F; Wernli, C

    1996-08-01

    A system based on fission fragment tracks had previously been developed for individual neutron dosimetry. The dosimeter detects both fast neutrons by means of the 232Th(n,f) reaction, and thermal and albedo neutrons by means of the 235U(n,f) reaction. The fission tracks produced in a plastic foil are chemically etched and counted by spark discharges. The response of the dosimeter has recently been re-investigated in 36 different neutron fields: monoenergetic beams, reference fields near isotopic sources, and radiation fields encountered in a variety of situations inside nuclear power plants. The results obtained have been compared to those computed by convolution of the neutron spectra with the energy response functions of the dosimeters. In practical situations, it is essential to know the shape of the neutron spectrum, approximately at least, in order to perform an acceptably accurate dose evaluation. For that purpose, the neutron fields encountered inside nuclear power plants have been grouped into four categories, for which algorithms for dose evaluation have been developed. Concerning the neutron equivalent dose, the error associated with this approach does not exceed a factor of 2, a performance which is comparable to other detection systems used in the field of individual neutron dosimetry.

  16. Neutron Scattering Cross Section Measurements for 169Tm via the (n,n') Technique

    SciTech Connect

    Alimeti, Afrim; Kegel, Gunter H.R.; Egan, James J.; DeSimone, David J.; McKittrick, Thomas M.; Ji, Chuncheng; Tremblay, Steven E.; Roldan, Carlos; Chen Xudong; Kim, Don S.

    2005-05-24

    The neutron physics group at the University of Massachusetts Lowell (UML) has been involved in a program of scattering cross-section measurements for highly deformed nuclei such as 159Tb, 169Tm, 232Th, 235U, 238U, and 239Pu. Ko et al. have reported neutron inelastic scattering data from 169Tm for states above 100 keV via the (n,n'{gamma}) reaction at incident energies in the 0.2 MeV to 1.0 MeV range. In the present research, in which the time-of-flight method was employed, direct (n,n') measurements of neutrons scattered from 169Tm in the 0.2 to 1.0 MeV range were taken. It requires that our 5.5-MeV Van de Graaff accelerator be operated in the pulsed and bunched beam mode producing subnanosecond pulses at a 5-MHz repetition frequency. Neutrons are produced by the 7Li(p,n)7Be reaction using a thin metallic elemental lithium target.

  17. Coupling of Uranium and Thorium Series Isotope Systematics for Age Determination of Late Pleistocene Zircons using LA-ICP-MS

    NASA Astrophysics Data System (ADS)

    Sakata, S.; Hirakawa, S.; Iwano, H.; Danhara, T.; Hirata, T.

    2014-12-01

    Zircon U-Th-Pb dating method is one of the most important tools for estimating the duration of magmatism by means of coupling of uranium, actinium and thorium decay series. Using U-Pb dating method, its reliability is principally guaranteed by the concordance between 238U-206Pb and 235U-207Pb ages. In case of dating Quaternary zircons, however, the initial disequilibrium effect on 230Th and 231Pa should be considered. On the other hands, 232Th-208Pb dating method can be a simple but powerful approach for investigating the age of crystallization because of negligible influence from initial disequilibrium effect. We have developed a new correction model for accurate U-Pb dating of the young zircon samples by taking into consideration of initial disequilibrium and a U-Pb vs Th-Pb concordia diagram for reliable age calibration was successfully established. Hence, the U-Th-Pb dating method can be applied to various zircons ranging from Hadean (4,600 Ma) to Quaternary (~50 ka) ages, and this suggests that further detailed information concerning the thermal history of the geological sequences can be made by the coupling of U-Th-Pb, fission track and Ar-Ar ages. In this presentation, we will show an example of U-Th-Pb dating for zircon samples from Sambe Volcano (3 to 100 ka), southwest Japan and the present dating technique using LA-ICP-MS.

  18. Kinetics of radioisotope exchange between brine and rock in a geothermal system

    SciTech Connect

    Hammond, D.E.; Zukin, J.G.; Teh-Lung Ku

    1988-11-10

    A wide range of isotopes in the /sup 238/U, /sup 235/U, and /sup 232/Th decay chains was measured in geothermal brines collected from two production zones at 1898 and 3220 m in the Salton Sea Scientific Drilling Project well. High concentrations of radium, radon, and lead isotopes are generated and maintained by the input of these isotopes from solid phases into brine by both recoil and leaching processes, by the high chloride content of the brine which complexes radium and lead, and by the apparent absence of suitable unoccupied adsorption sites. In contrast, uranium, thorium, actinium, bismuth, and polonium isotopes all have low concentrations due to their efficient sorption from brine to rock. Measurements of short-lived isotopes in these decay series yield insights regarding the mechanisms controlling radioisotope exchange, and they permit estimation of rates of brine-rock interaction. For example, the /sup 228/Ac//sup 228/Ra activity ratio of 0.2 in brines indicates that the mean residence time of actinium in solution before sorption onto solid surfaces is less than 2.5 hours.

  19. Detrital Zircon U-Pb Geochronology Applied to Tectonics

    NASA Astrophysics Data System (ADS)

    Gehrels, George

    2014-05-01

    Detrital zircon geochronology is rapidly developing into an essential tool in Earth science research because of the widespread occurrence of zircon in sedimentary systems; the wide range of information that can be extracted from zircon crystals; the ability to determine ages with reasonable precision, accuracy, and efficiency; and the wide range of new ideas about how to use detrital zircon geochronologic information. The U-Pb system is particularly powerful because three chronometers are available (238U+206Pb, 235U+207Pb, and 232Th+208Pb), but challenges arise because of complexities from inheritance and Pb loss. Ages can be used to constrain the age of deposition of the host sediment, reconstruct provenance, characterize a sedimentary unit, and characterize many different aspects of source regions. Detrital zircon geochronology has an exciting future given the growth history recorded in individual crystals; the variety of detrital minerals that can provide complementary information; and the large number of geochemical, isotopic, and chronologic systems that can be applied to these minerals.

  20. Direct ion microprobe U-Pb dating of fossil tooth of a Permian shark

    NASA Astrophysics Data System (ADS)

    Sano, Yuji; Terada, Kentaro

    1999-12-01

    We report here direct ion microprobe dating of fossil tooth (dentine) of a Permian fresh-water shark, Orthacanthus senckenbergianus using the SHRIMP instrument recently installed at Hiroshima University. Fifteen spots on the small sample (approximately 2 mm×1 mm) indicate a 238U/ 206Pb isochron age of 266±18 Ma and a Tera-Wasserburg concordia intercept age of 266±24 Ma in a three-dimensional 238U/ 206Pb- 207Pb/ 206Pb- 204Pb/ 206Pb diagram. These Permian ages are consistent with a 235U/ 207Pb age of 453±170 Ma and a 232Th- 208Pb age of 235±310 Ma, suggesting indistinguishable depositional and early diagenetic ages of the fossil in its sedimentary sequences. The success of the method depends on the chemical fractionation of uranium from lead in a specimen a few hundred microns in size and the consequent variations in lead isotopic compositions due to radioactive decay.

  1. Natural radionuclides in waste water discharged from coal-fired power plants in Serbia.

    PubMed

    Janković, Marija M; Todorović, Dragana J; Sarap, Nataša B; Krneta Nikolić, Jelena D; Rajačić, Milica M; Pantelić, Gordana K

    2016-12-01

    Investigation of the natural radioactivity levels in water around power plants, as well as in plants, coal, ash, slag and soil, and to assess the associated radiation hazard is becoming an emerging and interesting topic. This paper is focused on the results of the radioactivity analysis in waste water samples from five coal-fired power plants in Serbia (Nikola Tesla A, Nikola Tesla B, Kolubara, Morava and Kostolac), which were analyzed in the period 2003-2015. River water samples taken upstream and downstream from the power plants, drain water and overflow water were analyzed. In the water samples gamma spectrometry analysis was performed as well as determination of gross alpha and beta activity. Natural radionuclide (40)K was detected by gamma spectrometry, while the concentrations of other radionuclides, (226)Ra, (235)U and (238)U, usually were below the minimum detection activity (MDA). (232)Th and artificial radionuclide (137)Cs were not detected in these samples. Gross alpha and beta activities were determined by the α/β low level proportional counter Thermo Eberline FHT 770 T. In the analyzed samples, gross alpha activity ranged from MDA to 0.47 Bq L(-)(1), while the gross beta activity ranged from MDA to 1.55 Bq L(-)(1).

  2. Microscopic description of low-lying M1 excitations in odd-mass actinide nuclei

    NASA Astrophysics Data System (ADS)

    Tabar, Emre; Yakut, Hakan; Kuliev, Ali Akbar

    2017-01-01

    A restoration method of a broken symmetry which allows self-consistent determination of the separable effective restoration forces is now adapted to odd-mass nuclei in order to restore violated rotational invariance (RI-) of the Quasiparticle Phonon Nuclear Model (QPNM) Hamiltonian. Because of the self-consistency of the method, these effective forces contain no arbitrary parameters. Within RI-QPNM, the properties of the low-lying magnetic dipole excitations in odd-mass deformed 229-233Th and 233-239U nuclei have been investigated for the first time. It has been shown that computed fragmentation of the M1 strengths below 4 MeV in these nuclei is much stronger than that in neighboring doubly even 228-232Th and 232-238U nuclei. For 235U the summed M1 strength in the energy range 1.5-2.8 MeV is in agreement with the relevant experimental data where the missing strength was extracted by means of a fluctuation analysis.

  3. Radionuclides in Small Mammals Collected at the Dual-Axis Radiographic Hydrodynamic Test (DARHT) Facility during 2001-- 2003

    SciTech Connect

    P.R. Fresquez

    2005-01-20

    Rodents are effective indicators of environmental contamination and the Dual-Axis Radiographic Hydrodynamic Test (DARHT) Facility Mitigation Action Plan specifies the (radionuclide) comparison of small mammals to baseline levels to determine if there are any impacts as a result of operations. Consequently, samples of (whole body) field mice (Peromyscus spp.) were collected from within the grounds of the DARHT facility at Los Alamos National Laboratory, Technical Area 15, from 2001 through 2003. Samples were analyzed for {sup 3}H, {sup 137}Cs, {sup 90}Sr, {sup 241}Am, {sup 238}Pu, {sup 239,240}Pu, {sup 234}U, {sup 235}U, and {sup 238}U. Results, which represent three years since the start of operations in 2000, were compared with baseline statistical reference level (BSRL) data established over a four-year-long preoperational period. Most radionuclides in mice were either at nondetectable levels or within BSRLs. The few radionuclides that were above BSRLs included U isotopes; and the ratios of some samples indicated depleted U sources. Although the amounts of U in some samples were just above BSRLs, and since depleted U is less soluble and less toxic (chemical and radioactive) than naturally occurring U, the very small levels in the mice collected around the DARHT facility grounds are unlikely to pose a threat to predators that feed upon them.

  4. An alternative procedure for uranium analysis in drinking water using AQUALIX columns: application to varied French bottled waters.

    PubMed

    Bouvier-Capely, C; Bonthonneau, J P; Dadache, E; Rebière, F

    2014-01-01

    The general population is chronically exposed to uranium ((234)U, (235)U, and (238)U) and polonium ((210)Po) mainly through day-to-day food and beverage intake. The measurement of these naturally-occurring radionuclides in drinking water is important to assess their health impact. In this work the applicability of calix[6]arene-derivatives columns for uranium analysis in drinking water was investigated. A simple and effective method was proposed on a specific column called AQUALIX, for the separation and preconcentration of U from drinking water. This procedure is suitable for routine analysis and the analysis time is considerably shortened (around 4h) by combining the separation on AQUALIX with fast ICP-MS measurement. This new method was tested on different French bottled waters (still mineral water, sparkling mineral water, and spring water). Then, the case of simultaneous presence of uranium and polonium in water was considered due to interferences in alpha spectrometry measurement. A protocol was proposed using a first usual step of spontaneous deposition of polonium on silver disc in order to separate Po, followed by the uranium extraction on AQUALIX column before alpha spectrometry counting.

  5. In-beam studies of high-spin states of actinide nuclei

    SciTech Connect

    Stoyer, M.A. . Nuclear Science Div. California Univ., Berkeley, CA . Dept. of Chemistry)

    1990-11-15

    High-spin states in the actinides have been studied using Coulomb- excitation, inelastic excitation reactions, and one-neutron transfer reactions. Experimental data are presented for states in {sup 232}U, {sup 233}U, {sup 234}U, {sup 235}U, {sup 238}Pu and {sup 239}Pu from a variety of reactions. Energy levels, moments-of-inertia, aligned angular momentum, Routhians, gamma-ray intensities, and cross-sections are presented for most cases. Additional spectroscopic information (magnetic moments, M{sub 1}/E{sub 2} mixing ratios, and g-factors) is presented for {sup 233}U. One- and two-neutron transfer reaction mechanisms and the possibility of band crossings (backbending) are discussed. A discussion of odd-A band fitting and Cranking calculations is presented to aid in the interpretation of rotational energy levels and alignment. In addition, several theoretical calculations of rotational populations for inelastic excitation and neutron transfer are compared to the data. Intratheory comparisons between the Sudden Approximation, Semi-Classical, and Alder-Winther-DeBoer methods are made. In connection with the theory development, the possible signature for the nuclear SQUID effect is discussed. 98 refs., 61 figs., 21 tabs.

  6. Radionuclide Concentration in Soils and Vegetation at Low-Level Radioactive Waste Disposal Area G during 2005

    SciTech Connect

    P.R. Fresquez; M.W. McNaughton; M.J. Winch

    2005-10-01

    Soil samples were collected at 15 locations and unwashed overstory and understory vegetation samples were collected from up to nine locations within and around the perimeter of Area G, the primary disposal facility for low-level radioactive solid waste at Los Alamos National Laboratory (LANL). Soil and plant samples were also collected from the proposed expansion area west of Area G for the purpose of gaining preoperational baseline data. Soil and plant samples were analyzed for radionuclides that have shown a history of detection in past years; these included {sup 3}H, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 234}U, {sup 235}U, and {sup 238}U for soils and {sup 3}H, {sup 238}Pu, and {sup 239,240}Pu for plants. As in previous years, the highest levels of {sup 3}H in soils and vegetation were detected at the south portion of Area G near the {sup 3}H shafts; whereas, the highest concentrations of the Pu isotopes were detected in the northern and northeastern portions near the pads for transuranic waste. All concentrations of radionuclides in soils and vegetation, however, were still very low (pCi range) and far below LANL screening levels and regulatory standards.

  7. Neutron-Induced Fission Cross Section Measurements for Uranium Isotopes and Other Actinides at LANSCE

    SciTech Connect

    Laptev, Alexander B.; Tovesson, Fredrik K.; Hill, Tony S.

    2012-08-16

    A well established program of neutron-induced fission cross section measurement at Los Alamos Neutron Science Center (LANSCE) is supporting the Fuel Cycle Research program (FC R&D). The incident neutron energy range spans from sub-thermal up to 200 MeV by combining two LANSCE facilities, the Lujan Center and the Weapons Neutron Research center (WNR). The time-of-flight method is implemented to measure the incident neutron energy. A parallel-plate fission ionization chamber was used as a fission fragment detector. The event rate ratio between the investigated foil and a standard {sup 235}U foil is translated into a fission cross section ratio. Thin actinide targets with deposits of <200 {micro}g/cm{sup 2} on stainless steel backing were loaded into a fission chamber. In addition to previously measured data for {sup 237}Np, {sup 239-242}Pu, {sup 243}Am, new measurements include the recently completed {sup 233,238}U isotopes, {sup 236}U data which is being analyzed, and {sup 234}U data acquired in the 2011-2012 LANSCE run cycle. The new data complete the full suite of Uranium isotopes which were investigated with this experimental approach. When analysis of the new measured data is completed, data will be delivered to evaluators. Having data for multiple Uranium isotopes will support theoretical modeling capabilities and strengthens nuclear data evaluation.

  8. Levels of depleted uranium in Kosovo soils.

    PubMed

    Sansone, U; Stellato, L; Jia, G; Rosamilia, S; Gaudino, S; Barbizzi, S; Belli, M

    2001-01-01

    The United Nations Environment Programme (UNEP) has performed a field survey at 11 sites located in Kosovo, where depleted uranium (DU) ammunitions were used by the North Atlantic Treaty Organization (NATO) during the last Balkans conflict (1999). Soil sampling was performed to assess the spread of DU ground contamination around and within the NATO target sites and the migration of DU along the soil profile. The 234U/238U and 235U/238U activity concentration ratios have been used as an indicator of natural against anthropogenic sources of uranium. The results show that levels of 238U activity concentrations in soils above 100 Bq x kg(-1) can be considered a 'tracer' of the presence of DU in soils. The results also indicate that detectable ground surface contamination by DU is limited to areas within a few metres from localised points of concentrated contamination caused by penetrator impacts. Vertical distribution of DU along the soil profile is measurable up to a depth of 10-20 cm. This latter aspect is of particular relevance for the potential risk of future contamination of groundwater.

  9. High levels of natural radioactivity in biota from deep-sea hydrothermal vents: a preliminary communication.

    PubMed

    Charmasson, Sabine; Sarradin, Pierre-Marie; Le Faouder, Antoine; Agarande, Michèle; Loyen, Jeanne; Desbruyères, Daniel

    2009-06-01

    Hydrothermal deep-sea vent fauna is naturally exposed to a peculiar environment enriched in potentially toxic species such as sulphides, heavy metals and natural radionuclides. It is now well established that some of the organisms present in such an environment accumulate metals during their lifespan. Though only few radionuclide measurements are available, it seems likely that hydrothermal vent communities are exposed to high natural radiation doses. Various archived biological samples collected on the East Pacific Rise and the Mid-Atlantic Ridge in 1996, 2001 and 2002 were analysed by ICP-MS in order to determine their uranium contents ((238)U, (235)U and (234)U). In addition (210)Po-Pb were determined in 2 samples collected in 2002. Vent organisms are characterized by high U, and Po-Pb levels compared to what is generally encountered in organisms from outside hydrothermal vent ecosystems. Though the number of data is low, the results reveal various trends in relation to the site, the location within the mixing zone and/or the organisms' trophic regime.

  10. Isotopes of uranium and plutonium in the atmosphere. [Cosmos-954 fall in Canada

    SciTech Connect

    Sakuragi, Y.

    1982-01-01

    The activities of /sup 234/U, /sup 235/U and /sup 238/U were measured in 24 individual rain samples and two composite rains collected at Fayetteville, Arkansas, during the months of March 1979 and March 1980 through May 1981. Uranium-234 and -235 were found to be highly enriched in several rain samples collected during the months of April and May 1980. Uranium-238 concentrations, on the other hand, were unusually high during the months of July, August and early September 1980. The concentrations of /sup 238/Pu and /sup 238/ /sup 240/Pu were measured in 76 individual rain samples and two composite rains which were collected at Fayetteville, Arkansas, during the period from February 1979 through December 1980. Plutonium-238 and plutonium-239,240 concentrations were found to be extremely high during the months of July, August and early September 1980. The anomalous uranium highly enriched in the light isotopes of uranium appears to have originated from the Soviet satellite Cosmos-954 which fell over Canada on 24 January 1978. The uranium fallout occurred just about the time Mount St. Helens erupted on 18 May 1980 and began to inject a large amount of natural uranium into the atmosphere. The pattern of variations of the concentrations of /sup 238/U in rain after the eruption of Mount St. Helens was found to be similar to that of plutonium isotopes.

  11. Radionuclide Concentrations in Soils and Vegetation at Low-Level Radioactive Waste Disposal Area G during the 1997 Growing Season

    SciTech Connect

    L. Naranjo, Jr.; P. R. Fresquez; R. J. Wechsler

    1998-08-01

    Soil and overstory and understory vegetation (washed and unwashed) collected at eight locations within and around Area G-a low-level radioactive solid-waste disposal facility at Los Alamos National Laboratory-were analyzed for 3H, 238Pu, 239Pu, 137CS, 234U, 235U, 228AC, Be, 214Bi, 60Co, 40& 54Mn, 22Na, 214Pb and 208Tl. In general, most radionuclide concentrations, with the exception of 3Ef and ~9Pu, in soils and overstory and understory vegetation collected from within and around Area G were within upper (95'%) level background concentrations. Although 3H concentrations in vegetation from most sites were significantly higher than background (>2 pCi mL-l), concentrations decreased markedly in comparison to last year's results. The highest `H concentration in vegetation was detected from a juniper tree that was growing over tritium shaft /+150; it contained 530,000 pCi 3H mL-l. Also, as in the pas~ the transuranic waste pad area contained the highest levels of 239Pu in soils and in understory vegetation as compared to other areas at Area G.

  12. Radionuclide concentrations in soils and vegetation at radioactive-waste disposal Area G during the 1996 growing season. Progress report

    SciTech Connect

    Fresquez, P.R.; Vold, E.L.; Naranjo, L. Jr.

    1997-07-01

    Soil and overstory and understory vegetation (washed and unwashed) collected at eight locations within and around Area G--a low-level radioactive solid-waste disposal facility at Los Alamos National laboratory--were analyzed for {sup 3}H, {sup 90}Sr, {sup 238}Pu, {sup 239}Pu, {sup 137}Cs, {sup 234}U, {sup 235}U, {sup 238}U, {sup tot}U, {sup 228}Ac, {sup 214}Bi, {sup 60}Co, {sup 40}K, {sup 54}Mn, {sup 22}Na, {sup 214}Pb, and {sup 208}Tl. Also, heavy metals (Ag, As, Ba, Be, Cd, Cr, Hg, Ni, Pb, Sb, Se, and Tl) in soil and vegetation were determined. In general, most radionuclide concentrations, with the exception of {sup 3}H and {sup 239}Pu, in soils and washed and unwashed overstory and understory vegetation collected from within and around Area G were within upper limit background concentrations. Tritium was detected as high as 14,744 pCi mL{sup {minus}1} in understory vegetation collected from transuranic (TRU) waste pad {number_sign}4, and the TRU waste pad area contained the highest levels of {sup 239}Pu in soils and in understory vegetation as compared to other areas at Area G.

  13. Spectroscopy of Actinide Nuclei - Perspectives with Position Sensitive HPGe Detectors

    NASA Astrophysics Data System (ADS)

    Reiter, P.; Birkenbach, B.; Kotthaus, T.

    Recent advances in in-beam gamma-ray spectroscopy of actinide nuclei are based on highly efficient arrays of escape-suppressed spectrometers. The sensitivity of these detector arrays is greatly enhanced by the combination with powerful mass separators or particle detector systems. This technique is demonstrated by an experiment to investigate excited states in 234U after the one-neutron-transfer reaction 235U(d,t). In coincidence with the outgoing tritons, γ-rays were detected with the highly efficient MINIBALL spectrometer. In the near future an even enhanced sensitivity will be achieved by utilizing position sensitive HPGe detectors which will exploit the novel detection method of gamma-ray energy tracking in electrically segmented germanium detectors. An example for this novel approach is the investigation neutron-rich actinide Th and U nuclei after multi nucleon transfer reactions employing the AGATA demonstrator and PRISMA setup at LNL, Italy. A primary 136Xe beam hitting a 238U target was used to produce the nuclei of interest. Beam-like reaction products after neutron transfer were selected by the PRISMA spectrometer. Coincident γ-rays from excited states in beam and target like particles were measured with the position sensitive AGATA HPGe detectors. Improved Doppler correction and quality of the γ-spectra is based on the novel γ-ray tracking technique, which was successfully exploited in this region.

  14. Ultratrace Uranium Fingerprinting with Isotope Selective Laser Ionization Spectrometry

    SciTech Connect

    Ziegler, Summer L.; Bushaw, Bruce A.

    2008-08-01

    Uranium isotope ratios can provide source information for tracking uranium contamination in a variety of fields, ranging from occupational bioassay to monitoring aftereffects of nuclear accidents. We describe the development of Isotope Selective Laser Ionization Spectrometry (ISLIS) for ultratrace measurement of the minor isotopes 234U, 235U, and 236U with respect to 238U. Optical isotopic selectivity in three-step excitation with single-mode continuous wave lasers is capable of measuring the minor isotopes at relative abundances below 1 ppm, and is not limited by isobaric interferences such as 235UH+ during measurement of 236U. This relative abundance limit approaches the threshold for measurement of uranium minor isotopes with conventional mass spectrometry, typically 10-7, but without mass spectrometric analysis of the laser-created ions. Uranyl nitrate standards from an international blind comparison were used to test analytical performance for different isotopic compositions and with quantities ranging from 11 ng to 10 µg total uranium. Isotopic ratio determination was demonstrated over a linear dynamic range of 7 orders of magnitude with a few percent relative precision and detection limits below 500 fg for the minor isotopes.

  15. The use of secondary ion mass spectrometry in forensic analyses of ultra-small samples

    NASA Astrophysics Data System (ADS)

    Cliff, John

    2010-05-01

    less than 300 picograms of bacteria. Perhaps the most successful application of SIMS for forensic purposes to date is in the field of nuclear forensics. An example that has been used by laboratories associated with the International Atomic Energy Agency is the examination of environmental samples for enriched uranium particles indicative of clandestine weapons production activities.. The analytical challenge in these types of measurements is to search complex environmental matrices for U-bearing particles which must then be analyzed for 234U, 235U, and 236U content with high precision and accuracy. Older-generation SIMS instruments were hampered by small geometries that made resolution of significant interferences problematic. In addition, automated particle search software was proprietary and difficult to obtain. With the development of new search software, the IMS 1280 is capable of searching a sample in a matter of hours, flagging U-bearing particles for later analyses, and providing a rough 235U content. Particles of interest can be revisited for high precision analyses, and all U-isotopes can be measured simultaneously in multicollector mode, dramatically improving analysis time and internal precision. Further, the large geometry of the instrument allows complete resolution of isobaric interferences that have traditionally limited SIMS analyses of difficult samples. Examples of analyses of micron-sized standard particles indicate that estimates of 235U enrichment can be obtained with an external relative precision of 0.1% and 234U and 236U contents can be obtained with a relative precision of less than 1%. Analyses of 'real' samples show a dramatic improvement in the data quality obtained compared with small-geometry SIMS instruments making SIMS the method of choice for these high-profile samples when accurate, precise, and rapid results are required.

  16. Early diagenesis impact on precise U-series dating of deep-sea corals: Example of a 100 200-year old Lophelia pertusa sample from the northeast Atlantic

    NASA Astrophysics Data System (ADS)

    Pons-Branchu, Edwige; Hillaire-Marcel, Claude; Deschamps, Pierre; Ghaleb, Bassam; Sinclair, Daniel J.

    2005-10-01

    Deep-sea coral has proved useful for paleoceanographic reconstructions and for documenting 14C-ages of water masses using 230Th-ages. However, for precise and accurate U-series dating, further information on coral-age structure, growth rate and diagenetic evolution is still needed. To document such processes, we used U-Th- 226Ra systematics in a 40 cm diameter, Lophelia pertusa specimen collected in 1912 from the Eastern Atlantic (Sea of the Hebrides). External parts of the specimen are thought to have been alive when collected whereas more internal parts were likely dead. The "live-collected" and "dead" parts of the skeleton were sampled and analyzed for their 230Th, 232Th, 234U, 238U, 226Ra and Ba contents by thermal ionization and multicollector inductively coupled plasma mass spectrometry. 230Th/ 234U ratios in the most recent parts yielded ages of 86 ± 6 a and 92 ± 9 a, in agreement with the date of recovery. The older parts yielded 230Th ages ranging from 169 ± 15 to 211 ± 10 a (n = 5), but had a 31% higher U content than more recent parts of the skeleton. This raises concerns about the possibility of secondary diagenetic U uptake, although an environmentally controlled U/Ca shift between coral growth stages cannot be ruled out. 226Ra/Ba measurements were made, and model- 226Ra/Ba ages averaging 250 ± 12 yr were calculated for the older part, assuming a constant initial 226Ra/Ba ratio in bottom waters. These ages are slightly older than 230Th-ages, suggesting either that 226Ra/Ba ratios of ambient-seawater changed over time or that a diagenetic phenomenon have affected the U-series system, or both. Scanning electron microscope observations revealed bioerosion and secondary biomineralization in the older part of the coral skeleton, supporting the hypothesis that diagenetic processes may have influenced the ages obtained by the U-series toolbox. Modeled U-series ages for such an open system are discussed. However, a comparison between 14C- and 230Th

  17. Can calcretes be used to date pedogenic processes in soil profiles under semi arid climate ? An example from U-Th isochrons in calcretes from South India.

    NASA Astrophysics Data System (ADS)

    Durand, Nicolas; Hamelin, Bruno; Deschamps, Deschamps; Gunnel, Yanni; Curmi, Pierre

    2015-04-01

    Pedogenic carbonates, such as calcretes, have often been questioned as possible markers of the pedogenetic evolution of soil profiles under semi-arid climate. However, providing precise chronological constraints on their formation is a perequisite to determine the climatic and paleo-environmental conditions prevailing during and after their formation, and to improve our understanding of the physical and chemical conditions that promoted their development and preservation. On the other hand, these authigenic calcium carbonate precipitates provide us with an interesting test of the U-Th radioactive disequilibrium dating method, the reliability of which has been demonstrated extensively in aragonitic marine formations, and calcitic continental speleothems, but remain much more questionable in highly porous and chemically complex media such as soil profiles. In this study, we combined U-Th systematics with detailed micromorphologic observations of calcretes from South India, investigated at different spatial scales, from the landscape to the soil profile, down to the micro-fabrics of the samples. The U-Th analyses were performed by Thermo-Ionization Mass Spectrometry. Since calcretes are impure carbonates, mixed with various amounts of parent rock and weathered minerals, all ages had to be computed using the isochron technique to correct for the detrital component. This method involves the extraction of several coeval subsamples from a single soil horizon and their U-Th analyses after total dissolution (TDS method). The isochron age is derived from the slope of the mixing line between the pure authigenic carbonate and the detrital phase, and the precision established statistically using the probability of fit and weighted mean deviations (MSWD). Our results show that each set of samples taken from decimetric blocks is characterized by a well defined isochron line, clearly distinct from each other in the 3D Osmond diagram (232Th/238U; 230Th/238U ; 234U/238U). The

  18. Uranium biogeochemistry across the redox transition zone of a permanently stratified fjord: Framvaren, Norway

    USGS Publications Warehouse

    Swarzenski, P.W.; McKee, B.A.; Skei, J.M.; Todd, J.F.

    1999-01-01

    During August 1995, the vertical concentration profile of dissolved and particulate uranium exhibited strong non-conservative characteristics in the upper 30 m of Framvaren Fjord. There was a pronounced peak in both particulate (> 0.2 ??m; 1.09 nM) and dissolved (< 0.2 ??m; 17.06 nM) uranium in the finely stratified waters at the O2/H2S interface which is positioned well within the euphotic zone at about 20-21 m. Such concentration maxima at the redox boundary are also observed for dissolved organic carbon (DEC), Sr and Ba. Dissolved U levels seen in the water column from 18 m down to 30 m exceeded the high salinity (salinity = 35) U concentrations (13.63 ?? 0.84 nM; Chen, J.H., Edwards, R.L., Wasserburg, G.L., 1986. 238U, 234U and 232Th in seawater. Earth Planet Sci. Lett. 80, 241-251.) observed uniformly in the open ocean. A prolific population of S microbes (e.g., Chromatium, Chlorobium sp.) flourishes at the O2/H2S interface. The source of elevated U at the redox boundary must be due to microbial uptake and subsequent release processes rather than dilution from oceanic uranium. Uranium oxidation state determinations in waters from 1, 22 and 30 m depth reveal that reduced U(IV) is not present in significant abundance, and that the chemical and/or biological reduction of hexavalent uranium is largely inhibited. Our results suggest that U and other trace constituents such as DOC, Sr, Ba, Fe(II), Mn(II) are greatly modified by direct and indirect microbial transformation reactions which are most concentrated across the redox transition zone in Framvaren Fjord.

  19. Impact of vegetation change on the mobility of uranium- and thorium-series nuclides in soils

    NASA Astrophysics Data System (ADS)

    Gontier, A.; Rihs, S.; Turpault, M.-P.; Chabaux, F.

    2012-04-01

    The effect of land cover change on chemical mobility and soil response was investigated using short- and long-lived nuclides from the U- and Th series. Indeed, the matching of these nuclides half-live to the pedogenic processes rates make these nuclides especially suitable to investigate either time or mechanism of transfers within a soil-water-plant system. This study was carried out from the experimental Breuil-Chenue site (Morvan mountains, France). The native forest (150 year-old) was partially clear-felled and replaced in 1976 by mono-specific plantations distributed in different stands. Following this cover-change, some mineralogical changes in the acid brown soil were recognized (Mareschal, 2008). Three soil sections were sampled under the native forest and the replanted oak and Douglas spruce stands respectively. The (238U), (234U), (230Th), (226Ra), (232Th) and (228Ra) activities were analysed by thermal ionization mass spectrometry (TIMS), inductively coupled plasma mass spectrometry (MC-ICPMS) and gamma spectrometry. Significant differences in U, Th, and Ra activities were observed between the soils located under the native forest or the replanted-trees stands, mostly dominated by a large uranium mobilization from the replanted soils. Moreover, all the investigated U and Th-series activity ratios show a contrasted trend between the shallowest horizons (0-50cm) and the deepest one (below 50cm), demonstrating the chemical effect of the vegetation change on the shallow soil layers. Using a continuous open-system leaching model, the coupled radioactive disequilibria measured in the different soil layers permit to quantify the rate of the radionuclides mobilities. Reference: Mareschal, L., 2008. Effet des substitutions d'essences forestières sur l'évolution des sols et de leur minéralogie : bilan après 28 ans dans le site expérimental de Breuil (Morvan) Université Henri Poincaré, Nancy-I.

  20. Distribution of natural radionuclides in the production and use of phosphate fertilizers in Brazil.

    PubMed

    Saueia, C H R; Mazzilli, B P

    2006-01-01

    The Brazilian phosphate fertilizer is obtained by wet reaction of igneous phosphate rock with concentrated sulphuric acid, giving as final product, phosphoric acid and dehydrated calcium sulphate (phosphogypsum) as by-products. Phosphoric acid is the starting material for triple superphosphate (TSP), single superphosphate (SSP), monoammonium phosphate (MAP) and diammonium phosphate (DAP). The phosphate rock used as raw material presents in its composition radionuclides of the U and Th natural series. Taking this into account, the main aim of this paper is to evaluate the fluxes of natural radionuclides and radioactive disequilibria involved in the Brazilian industrial process of phosphoric acid production; to determine the content of radioactivity in several commercial fertilizers produced by this industry; to estimate their radiological impact in crop soils and the long term exposure due to their application. Radiological characterization of phosphate rock, phosphogypsum and phosphate fertilizers was performed by alpha and gamma spectrometry. The fertilizer samples, which are derived directly from phosphoric acid, MAP and DAP, presented in their composition low activity concentrations for 226Ra, 228Ra and 210Pb. As for U and Th, the concentrations found in MAP and DAP are more significant, up to 822 and 850Bqkg(-1), respectively. SSP and TSP, which are obtained by mixing phosphoric acid with different amounts of phosphate rock, presented higher concentrations of radionuclides, up to 1158Bqkg(-1) for (238)U, 1167Bqkg(-1) for (234)U, 1169Bqkg(-1) for 230Th, 879Bqkg(-1) for 226Ra, 1255Bqkg(-1) for 210Pb, 521Bqkg(-1) for 232Th, 246Bqkg(-1) for 228Ra and 302Bqkg(-1) for 228Th. Long term exposure due to successive fertilizer applications was evaluated. Internal doses due to the application of phosphate fertilizer for 10, 50 and 100 years were below 1mSvy(-1), showing that the radiological impact of such practice is negligible.

  1. Accumulation rates of Th-230, Pa-231, and some transition metals on the Bermuda Rise

    USGS Publications Warehouse

    Bacon, M.P.; Rosholt, J.N.

    1982-01-01

    Measurements of 238U, 234U, 230Th, 232Th, 231Pa, Mn, Fe, Co, Ni, Cu, and Zn were made on 23 samples from core GPC-5, a 29-m giant piston core from a water depth of 4583 m on the northeastern Bermuda Rise (33??41.2???N, 57??36.9???W). This area is characterized by rapid deposition of sediment transported by abyssal currents. Unsupported 230Th and 231Pa are present throughout the core but, because of large variations in the sedimentation rate, show marked departures from exponential decay with depth. The trend with depth of the 231Paex 230Thex ratio is consistent with the average accumulation rate of 36 cm/1000 y reported earlier on the basis of radiocarbon dating and CaCO3 stratigraphy. When expressed on a carbonate-free basis, concentrations of Mn, Co, Ni, Cu, Zn, 230Thex, and 231Paex all show cyclic variations positively correlated with those of CaCO3. The correlations can be explained by a model in which all of these constituents, including CaCO3, are supplied to the sediments from the water column at a constant rate. Concentration variations are controlled mainly by varying inputs of terrigenous detritus, with low inputs occurring during interglacials and high inputs during glacials. Relationships between the metal and 230Thex concentrations permit estimates of the rates at which the metals are removed to the sediment by scavenging from the water column. The results, in ??g/cm2-1000 y, are: 4300 ?? 1100 for Mn, 46 ?? 16 for Ni and 76 ?? 26 for Cu. These rates are somewhat larger than ocean-wide averages estimated by other methods, and the absolute rate of 230Th accumulation in GPC-5 averages about nine times higher than production in the overlying water column. This part of the Bermuda Rise and similar bottom-current deposits may act as important accumulators of elements scavenged from seawater. ?? 1982.

  2. Radionuclides transfer into halophytes growing in tidal salt marshes from the Southwest of Spain.

    PubMed

    Luque, Carlos J; Vaca, Federico; García-Trapote, Ana; Hierro, Almudena; Bolívar, Juan P; Castellanos, Eloy M

    2015-12-01

    Estuaries are sinks of materials and substances which are released directly into them or transported from rivers that drain the basin. It is usual to find high organic matter loads and fine particles in the sediments. We analyzed radionuclide concentrations ((210)Po, (230)Th, (232)Th, (234)U, (238)U, (226)Ra, (228)Th, (228)Ra, (40)K) in sediments and three different organs (roots, stems and leaves) of three species of halophytes plants (Spartina maritima, Spartina densiflora and Sarcocornia perennis). The study was carried out in two tidal salt marshes, one polluted by U-series radionuclides and another nearby that was unpolluted and was used as a control (or reference) area. The Tinto River salt marsh shows high levels of U-series radionuclides coming from mining and industrial discharges. On the contrary, the unperturbed Piedras River salt marsh is located about 25 km from the Tinto marsh, and shows little presence of contaminants and radionuclides. The results of this work have shown that natural radionuclide concentrations (specially the U-isotopes) in the Tinto salt marsh sediments are one order of magnitude higher than those in the Piedras marsh. These radionuclide enhancements are reflected in the different organs of the plants, which have similar concentration increases as the sediments where they have grown. Finally, the transfer factor (TF) of the most polluted radionuclides (U-isotopes and (210)Po) in the Tinto area are one order of magnitude higher than in the Piedras area, indicating that the fraction of each radionuclide in the sediment originating from the pollution is more available for the plants than the indigenous fraction. This means that the plants of the salt marshes are unhelpful as bioindicators or for the phytoremediation of radionuclides.

  3. Alpha-emitting isotopes and chromium in a coastal California aquifer

    USGS Publications Warehouse

    Densmore, Jill N.; Izbicki, John A.; Murtaugh, Joseph M.; Swarzenski, Peter W.; Bullen, Thomas D.

    2014-01-01

    The unadjusted 72-h gross alpha activities in water from two wells completed in marine and alluvial deposits in a coastal southern California aquifer 40 km north of San Diego were 15 and 25 picoCuries per liter (pCi/L). Although activities were below the Maximum Contaminant Level (MCL) of 15 pCi/L, when adjusted for uranium activity; there is concern that new wells in the area may exceed MCLs, or that future regulations may limit water use from the wells. Coupled well-bore flow and depth-dependent water-quality data collected from the wells in 2011 (with analyses for isotopes within the uranium, actinium, and thorium decay-chains) show gross alpha activity in marine deposits is associated with decay of naturally-occurring 238U and its daughter 234U. Radon activities in marine deposits were as high as 2230 pCi/L. In contrast, gross alpha activities in overlying alluvium within the Piedra de Lumbre watershed, eroded from the nearby San Onofre Hills, were associated with decay of 232Th, including its daughter 224Ra. Radon activities in alluvium from Piedra de Lumbre of 450 pCi/L were lower than in marine deposits. Chromium VI concentrations in marine deposits were less than the California MCL of 10 μg/L (effective July 1, 2014) but δ53Cr compositions were near zero and within reported ranges for anthropogenic chromium. Alluvial deposits from the nearby Las Flores watershed, which drains a larger area having diverse geology, has low alpha activities and chromium as a result of geologic and geochemical conditions and may be more promising for future water-supply development.

  4. Cold water corals of the Northeast Atlantic margin: Archives of intermediate water circulation during the Holocene

    NASA Astrophysics Data System (ADS)

    Frank, N.; Paterne, M.; Ayliffe, L.; Lutringer, A.; Blamart, D.; van Weering, T.

    2003-04-01

    We present combined 230Th/U and 14C dating and stable isotope analyses on benthic corals from the northeastern North Atlantic in order to investigate past changes of the thermohaline circulation. The reef forming cold water corals Lophelia pertusa and Madrepora oculata were raised from intermediate depth (˜750m bsl) from carbonate mounds along Rockall and Porcupine Bank and Porcupine Seabight.The 230Th/U ages range from today to 247,400yr. The δ234U, 230Th/232Th, and X-ray images indicate negligible alteration of the investigated corals, i.e. open system behavior. Very young deep-sea corals were accurately dated by means of 230Th/U dating. One in-situ living Lophelia coral yielded a mean age of 1995AD, matching the date of collection in 1999AD. From this coral, the measured and calculated seawater Δ14C values are indistinguishable, and the reservoir age Rinterm of the upper intermediate waters is 710±80 years. Several modern corals, being dated between 1950AD and 1986AD, recorded the atmospheric 14C/12C increase due to the nuclear tests in the early 60s. The modern pre-bomb Δ14C value of the North Atlantic intermediate waters was determined at an average of -65±7o/oo, and the mean reservoir age at 500±50 years. Finally, several investigated benthic coral grew during the second step of the deglaciation and during the Holocene climate optimum (from 10,900 to about 8,000 CAL yr BP). The reservoir age of average 530±65 years is equivalent to that of today indicating that, during the studied coral growth episodes, a modern type oceanic circulation, as well as the air-sea and surface to deeper adjacent water 14CO2 exchanges prevailed in the Northeast Atlantic Ocean.

  5. Geochemical and isotopic properties of Heinrich layers H2 to H0 off Hudson Strait

    NASA Astrophysics Data System (ADS)

    Nuttin, L.; Ghaleb, B.; Hillaire-Marcel, C.

    2011-12-01

    Information about the precise timing and transport/depositional mechanism of fine detrital-carbonate sedimentary pulses, which occurred off Hudson Strait during Heinrich-events and linked to ice-margin instability in this area, is still much fragmentary (see Hesse et al., Geology 32: 449-452, 2004). Here, we intend to document the properties and duration of the most recent of these sedimentary pulses (H2, H1, H0) based on mineralogical, geochemical and isotopic data in a 895-cm long core (HU08-029-004; 2674 m water-depth; 61°27'N, 58°2'W) raised from the lower slope, about 100 nm off Hudson Strait shelf edge. Measurements of 238U, 234U, 230Th and 232Th, supplemented by semi-quantitative mineralogical analysis and light isotope data (C, Corg, Cinorg, C/N, 14C, δ13C and δ18O) are used to document sedimentary features in this core. First investigations provide an estimated average sedimentation rate of ~33 cm/ka on the whole studied sequence. 230Th-excesses over supported fraction are estimated following Veiga-Pires & Hillaire-Marcel (Paleoceanography 14: 187-199, 1999). H-layer thicknesses are about 60 cm, 100 cm and 28 cm respectively (H2, H1, H0). They depict up to 60% of fine detrital carbonates (mostly calcite) and are also highlighted by relatively low 230Th-excesses (nearly 0 dpm/g) compared with excesses of about 3 dpm/g in the overlying Holocene sediments. The low 230Th-excesses in H-layers do indicate a very fast depositional process but prevent any meaningful estimation of sedimentation rates due to uncertainties in their estimates.

  6. Uranium-thorium series radionuclides in brines and reservoir rocks from two deep geothermal boreholes in the Salton Sea Geothermal Field, southeastern California

    NASA Astrophysics Data System (ADS)

    Zukin, Jeffrey G.; Hammond, Douglas E.; Teh-Lung, Ku; Elders, Wilfred A.

    1987-10-01

    Naturally occurring U and Th series radionuclides have been analyzed in high temperature brines (~300°C, 25 wt% dissolved solids) and associated rocks from two deep geothermal wells located on the northeastern margin of the Salton Sea Geothermal Field (SSGF). These data are part of a study of the SSGF as a natural analog of possible radionuclide behavior near a nuclear waste repository constructed in salt beds, and permit evaluation of some characteristics of water-rock interaction in the SSGF. Rock/Brine concentration ratios ( Rc = (dpm/ g) rock/(dpm/ g) brine) were found to vary from near unity for isotopes of Ra, Pb and Rn to about 5 × 10 5 for 232Th. The high sorptivity of 232Th is closely followed by that of 238U and 234U ( Rc ~ 5 × 10 4), suggesting that U is retained in the +4 oxidation state by the reducing conditions in the brines. The relatively high solubility of 210Pb and 212Pb is attributed to formation of chloride complexes, while the high Ra solubility is attributed to chloride complexing, a lack of suitable adsorption sites due to the high brine salinity and temperature, and the reducing conditions that prevent MnO 2 and RaSO 4 from forming. The 228Ra /226Ra ratios in the brines are approximately equal to those of their parents ( 232Th /230Th ) in associated rocks, indicating that Ra equilibration in the brine-rock system is achieved within the mean life of 228Ra (8.3 years). The 224Ra /228Ra ratios in these brines are about 0.7, indicating that either (1) brine composition is not homogeneous and 224Ra decays in fracture zones deficient in Ra and Th as the brine travels to the wellhead or (2) Ra equilibration in the brine-host rock system is not complete within the mean life of 224Ra (5.2 days) because the desorption of 224Ra from the solid phase is impeded. The 228Ac /228Ra activity ratio in the SSGF brines studied is <0.1, and from this ratio the residence time of 228Ac in the brine before sorption onto solid surfaces is estimated to be <70

  7. Comment on "Radiocarbon Calibration Curve Spanning 0 to 50,000 Years B.P. Based on Paired 230Th/234U/238U and 14C Dates on Pristine Corals" by R.G. Fairbanks, R. A. Mortlock, T.-C. Chiu, L. Cao, A. Kaplan, T. P. Guilderson, T. W. Fairbanks, A. L. Bloom, P

    SciTech Connect

    Reimer, P J; Baillie, M L; Bard, E; Beck, J W; Blackwell, P G; Buck, C E; Burr, G S; Edwards, R L; Friedrich, M; Guilderson, T P; Hogg, A G; Hughen, K A; Kromer, B; McCormac, G; Manning, S; Reimer, R W; Southon, J R; Stuiver, M; der Plicht, J v; Weyhenmeyer, C E

    2005-10-02

    Radiocarbon calibration curves are essential for converting radiocarbon dated chronologies to the calendar timescale. Prior to the 1980's numerous differently derived calibration curves based on radiocarbon ages of known age material were in use, resulting in ''apples and oranges'' comparisons between various records (Klein et al., 1982), further complicated by until then unappreciated inter-laboratory variations (International Study Group, 1982). The solution was to produce an internationally-agreed calibration curve based on carefully screened data with updates at 4-6 year intervals (Klein et al., 1982; Stuiver and Reimer, 1986; Stuiver and Reimer, 1993; Stuiver et al., 1998). The IntCal working group has continued this tradition with the active participation of researchers who produced the records that were considered for incorporation into the current, internationally-ratified calibration curves, IntCal04, SHCal04, and Marine04, for Northern Hemisphere terrestrial, Southern Hemisphere terrestrial, and marine samples, respectively (Reimer et al., 2004; Hughen et al., 2004; McCormac et al., 2004). Fairbanks et al. (2005), accompanied by a more technical paper, Chiu et al. (2005), and an introductory comment, Adkins (2005), recently published a ''calibration curve spanning 0-50,000 years''. Fairbanks et al. (2005) and Chiu et al. (2005) have made a significant contribution to the database on which the IntCal04 and Marine04 calibration curves are based. These authors have now taken the further step to derive their own radiocarbon calibration extending to 50,000 cal BP, which they claim is superior to that generated by the IntCal working group. In their papers, these authors are strongly critical of the IntCal calibration efforts for what they claim to be inadequate screening and sample pretreatment methods. While these criticisms may ultimately be helpful in identifying a better set of protocols, we feel that there are also several erroneous and misleading statements made by these authors which require a response by the IntCal working group. Furthermore, we would like to comment on the sample selection criteria, pretreatment methods, and statistical methods utilized by Fairbanks et al. in derivation of their own radiocarbon calibration.

  8. Heating and melting of small icy satellites by the decay of 26Al

    NASA Technical Reports Server (NTRS)

    Prialnik, D.; Bar-Nun, A.; Owen, T. (Principal Investigator)

    1990-01-01

    We study the effect of radiogenic heating due to 26Al on the thermal evolution of small icy satellites. Our object is to find the extent of internal melting as a function of the satellite radius and of the initial 26Al abundance. The implicit assumption, based on observations of young stars, is that planet and satellite accretion occurred on a time scale of approximately 10(6) yr (comparable with the lifetime of 26Al). The icy satellites are modeled as spheres of initially amorphous ice, with chondritic abundances of 40K, 232Th, 235U, 238U, corresponding to an ice/dust mass ratio of 1. Evolutionary calculations are carried out, spanning 4.5 x 10(9) yr, for different combinations of the two free parameters. Heat transfer by subsolidus convection is neglected for these small satellites. Our main conclusion is that the initial 26Al abundance capable of melting icy bodies of satellite size to a significant extent is more than 10 times lower than that prevailing in the interstellar medium (or that inferred from the Ca-Al rich inclusions of the Allende meteorite, approximately 7 x 10(-7) by mass). We find, for example, that an initial 26Al mass fraction of approximately 4 x 10(-8) is sufficient for melting almost completely icy spheres with radii of 800 km, typical of the larger icy planetary satellites. We also find that for any given 26Al abundance, there is a narrow range of radii below which only marginal melting occurs and above which most of the ice melts (and refreezes later). Since extensive melting may have important consequences, such as differentiation, gas release, and volcanic activity, the effect of 26Al should be included in future studies of satellite interiors.

  9. Outdoor radioactivity and health risks in Balikesir, northwestern Turkey.

    PubMed

    Kapdan, E; Varinlioglu, A; Karahan, G

    2012-02-01

    External irradiation from radionuclides naturally present in the environment or released from man-made practices or events is usually an important component of the exposure of human populations. These exposures derive primarily from gamma radiation arising from the decay of these radionuclides at locations outside the human body. The main objective of this study is to evaluate the radioactivity levels and health risks due to terrestrial radionuclides in the soil of Balikesir, one of the largest cities of the country, northwestern Turkey. For this purpose, activity concentrations of radionuclides in soil and outdoor gamma dose rates (terrestrial and cosmic) have been investigated in the city of Balikesir. In addition, maps for the radionuclide activity concentrations of soil and the outdoor gamma dose rate distributions have been plotted for the region. The average activities of radionuclides, (238)U, (232)Th, (40)K, (235)U and (137)Cs in the soil were determined to be 37.6 ± 10.8, 54.7 ± 15.1, 674.5 ± 203.2, 3.6 ± 1.6, 3.4 ± 2.2 Bq kg(-1), respectively, in the region. The average outdoor gamma dose rates due to terrestrial and cosmic radiations were found to be 78.5 ± 12.4 and 48.9 ± 5.8 nGy h(-1) with the total of 127.4 ± 18.9 nGy h(-1) in the region. Annual effective dose due to environmental outdoor gamma radiation exposures was determined to be 156.3 nSv. The mean estimated cancer risk values were found to be 0.063 × 10(-2) for the region using risk factors of ICRP 103. The results of the study were discussed with the studies done in other cities of Turkey and the worldwide averages.

  10. Radiolytic Hydrogen Production in the Subseafloor Basaltic Aquifer.

    PubMed

    Dzaugis, Mary E; Spivack, Arthur J; Dunlea, Ann G; Murray, Richard W; D'Hondt, Steven

    2016-01-01

    Hydrogen (H2) is produced in geological settings by dissociation of water due to radiation from radioactive decay of naturally occurring uranium ((238)U, (235)U), thorium ((232)Th) and potassium ((40)K). To quantify the potential significance of radiolytic H2 as an electron donor for microbes within the South Pacific subseafloor basaltic aquifer, we use radionuclide concentrations of 43 basalt samples from IODP Expedition 329 to calculate radiolytic H2 production rates in basement fractures. The samples are from three sites with very different basement ages and a wide range of alteration types. U, Th, and K concentrations vary by up to an order of magnitude from sample to sample at each site. Comparison of our samples to each other and to the results of previous studies of unaltered East Pacific Rise basalt suggests that significant variations in radionuclide concentrations are due to differences in initial (unaltered basalt) concentrations (which can vary between eruptive events) and post-emplacement alteration. However, there is no clear relationship between alteration type and calculated radiolytic yields. Local maxima in U, Th, and K produce hotspots of H2 production, causing calculated radiolytic rates to differ by up to a factor of 80 from sample to sample. Fracture width also greatly influences H2 production, where microfractures are hotspots for radiolytic H2 production. For example, H2 production rates normalized to water volume are 190 times higher in 1 μm wide fractures than in fractures that are 10 cm wide. To assess the importance of water radiolysis for microbial communities in subseafloor basaltic aquifers, we compare electron transfer rates from radiolysis to rates from iron oxidation in subseafloor basalt. Radiolysis appears likely to be a more important electron donor source than iron oxidation in old (>10 Ma) basement basalt. Radiolytic H2 production in the volume of water adjacent to a square cm of the most radioactive SPG basalt may support as

  11. Presentation to JAEA Visitors, July 24, 2012

    SciTech Connect

    Gavron, Victor

    2012-07-19

    There are 7 Reasons for characterizing spent fuel nuclide concentrations: (1) Provide IAEA with the capability to independently verify the mass of plutonium at any site that has spent fuel; (2) Shipper/receiver difference; (3) Determination of the input accountability mass of an electrochemical (pyro-chemical) processing facility; (4) Continuity of knowledge at spent fuel storage site; (5) Optimal reloads through knowledge of true actinide content; (6) Burnup credit for fuel transport and storage; and (7) Provide confidence to the public that the shipment of spent fuel around the world is being undertaken in a rigorous manner, assuring that material is not diverted during shipment. Types of fuel of interest are: Fast Reactor Fuel, Normal burnup low enriched uranium (LEU), Mixed oxide (MOX), Low burnup LEU, and Research reactor. MCNPX calculates the slowing down and the energy spread for a given time. The principles are: (1) Neutrons slow down in LSDS; (2) Slow neutrons capture preferentially on a fission resonance; (3) Fission emits high-energy neutrons; (4) High-energy neutrons detected in threshold detector (that is not sensitive to slow neutrons) (e.g., {sup 238}U, {sup 232}Th); and (5) The detection time is characteristic of the slow neutron energy. Following each PSR pulse, the entire signal is digitized in 2 nanosecond intervals, and subsequently analyzed Analysis involves applying a digital filter to extract fission pulses in a background of initial oscillations and noise throughout. Some of the noise is not random. Depending on the threshold setting and filter parameters, both the normalization and the trend change. Original PNNL LSDS design required a 1-meter radius cylindrical LSDS. Much higher efficiency would allow us to use a (1.2m) LSDS (this is the LANL LSDS size), or a less intense source, or a combination of both. We still estimate 10{sup 16} total neutrons from the source to obtain 2-3% precision in {sup 239}Pu and {sup 235}U assay.

  12. Chemical and isotopic studies of granitic Archean rocks, Owl Creek Mountains, Wyoming: Uranium-thorium-lead systematics of an Archean granite from the Owl Creek Mountains, Wyoming

    SciTech Connect

    Stuckless, J.S.; Nkomo, I.T.; Butt, K.A.

    1986-01-01

    Isotopic analyses of apparently unaltered whole-rock samples of a granite from the Owl Creek Mountains, Wyo., yield a lead-lead isochron age of 2730 {plus minus} 35 Ma, which is somewhat older than the age obtained by the rubidium-strontium whole-rock method. Thorium-lead data for the same samples deviate markedly from an isochronal relation; however, calculated initial {sup 208}Pb/{sup 204}Pb ratios correlate with whole-rock {delta}{sup 18}O values and lead to the conclusion that the {sup 232}Th-{sup 208}Pb data are not colinear because of an originally heterogeneous granitic magma. Relationships in the {sup 207}Pb/{sup 235}U-{sup 206}Pb/{sup 238}U system show that uranium was mobilized during early Laramide time or shortly before, such that most surface and shallow drill-core samples lost 60-80 percent of their uranium, and some fractured, deeper drill-core samples gained from 50 to 10,000 percent uranium. Fission-track maps show that much uranium is located along edges and cleavages of biotite and magnetic where it is readily accessible to oxidizing ground water. Furthermore, qualitative comparisons of uranium distribution in samples with excess radiogenic lead and in samples with approximately equilibrium amounts of uranium and lead suggest that the latter contain more uranium in these readily accessible sites. Unlike other granites that have uranium distributions and isotopic systematics similar to those observed in this study, the granite of the Owl Creek Mountains is not associated with economic uranium deposits.

  13. MARE: Mars Radioactivity Experiment

    NASA Astrophysics Data System (ADS)

    di Lellis, A. M.; Capria, M. T.; Espinasse, S.; Magni, G.; Orosei, R.; Piccioni, G.; Federico, C.; Minelli, G.; Pauselli, C.; Scarpa, G.

    1999-09-01

    MARE is an experiment for the measurement of the beta and gamma radioactivity in space and in the Martian soil, both at the surface and in the subsurface. This will be accomplished by means of a dosimeter and a spectrometer. The radiation dose rate to which crews will be exposed is one of the hazards that has to be quantified before the human exploration of Mars may begin. Data for evaluating radioactivity levels at Martian surface are of great interest for environmental studies related to life in general. The dosimeter will be able to measure the beta and gamma radiation dose received, with a responsivity which is very close to that of a living organism. The dosimeter is based on thermo-luminescence pills which emit an optical signal proportional to the absorbed dose when heated. Radioactive elements ((40) K, (235) U, (238) U and (232) Th) can be used as a mean of tracing the evolution of a terrestrial planet. These radioactive elements are the source of the internal heat, which drives convection in the mantle. They have been redistributed in this process and they are now concentrated in the crust where they are accessible for study. Their different behavior during the fractionation process can be used as a mean to investigate the geochemical characteristic of Mars. The spectrometer, a scintillation radiation absorber system for single event counting, is capable of detecting gamma photons with energies between 200 KeV and 10 MeV. The detected events will be processed in such a way to allow the recognition of the spectral signature of different decay processes, and thus the identification and the measurement of the concentrations of different radionuclides in the Martian soil.

  14. Radiolytic Hydrogen Production in the Subseafloor Basaltic Aquifer

    PubMed Central

    Dzaugis, Mary E.; Spivack, Arthur J.; Dunlea, Ann G.; Murray, Richard W.; D’Hondt, Steven

    2016-01-01

    Hydrogen (H2) is produced in geological settings by dissociation of water due to radiation from radioactive decay of naturally occurring uranium (238U, 235U), thorium (232Th) and potassium (40K). To quantify the potential significance of radiolytic H2 as an electron donor for microbes within the South Pacific subseafloor basaltic aquifer, we use radionuclide concentrations of 43 basalt samples from IODP Expedition 329 to calculate radiolytic H2 production rates in basement fractures. The samples are from three sites with very different basement ages and a wide range of alteration types. U, Th, and K concentrations vary by up to an order of magnitude from sample to sample at each site. Comparison of our samples to each other and to the results of previous studies of unaltered East Pacific Rise basalt suggests that significant variations in radionuclide concentrations are due to differences in initial (unaltered basalt) concentrations (which can vary between eruptive events) and post-emplacement alteration. However, there is no clear relationship between alteration type and calculated radiolytic yields. Local maxima in U, Th, and K produce hotspots of H2 production, causing calculated radiolytic rates to differ by up to a factor of 80 from sample to sample. Fracture width also greatly influences H2 production, where microfractures are hotspots for radiolytic H2 production. For example, H2 production rates normalized to water volume are 190 times higher in 1 μm wide fractures than in fractures that are 10 cm wide. To assess the importance of water radiolysis for microbial communities in subseafloor basaltic aquifers, we compare electron transfer rates from radiolysis to rates from iron oxidation in subseafloor basalt. Radiolysis appears likely to be a more important electron donor source than iron oxidation in old (>10 Ma) basement basalt. Radiolytic H2 production in the volume of water adjacent to a square cm of the most radioactive SPG basalt may support as many as

  15. Heating and melting of small icy satellites by the decay of 26Al.

    PubMed

    Prialnik, D; Bar-Nun, A

    1990-05-20

    We study the effect of radiogenic heating due to 26Al on the thermal evolution of small icy satellites. Our object is to find the extent of internal melting as a function of the satellite radius and of the initial 26Al abundance. The implicit assumption, based on observations of young stars, is that planet and satellite accretion occurred on a time scale of approximately 10(6) yr (comparable with the lifetime of 26Al). The icy satellites are modeled as spheres of initially amorphous ice, with chondritic abundances of 40K, 232Th, 235U, 238U, corresponding to an ice/dust mass ratio of 1. Evolutionary calculations are carried out, spanning 4.5 x 10(9) yr, for different combinations of the two free parameters. Heat transfer by subsolidus convection is neglected for these small satellites. Our main conclusion is that the initial 26Al abundance capable of melting icy bodies of satellite size to a significant extent is more than 10 times lower than that prevailing in the interstellar medium (or that inferred from the Ca-Al rich inclusions of the Allende meteorite, approximately 7 x 10(-7) by mass). We find, for example, that an initial 26Al mass fraction of approximately 4 x 10(-8) is sufficient for melting almost completely icy spheres with radii of 800 km, typical of the larger icy planetary satellites. We also find that for any given 26Al abundance, there is a narrow range of radii below which only marginal melting occurs and above which most of the ice melts (and refreezes later). Since extensive melting may have important consequences, such as differentiation, gas release, and volcanic activity, the effect of 26Al should be included in future studies of satellite interiors.

  16. Monte Carlo simulation of skull and knee voxel phantoms for the assessment of skeletal burden of low-energy photon emitters.

    PubMed

    Nadar, M Y; Akar, D K; Patni, H K; Singh, I S; Mishra, L; Rao, D D; Pradeepkumar, K S

    2014-12-01

    In case of internal contamination due to long-lived actinides by inhalation or injection pathway, a major portion of activity will be deposited in the skeleton and liver over a period of time. In this study, calibration factors (CFs) of Phoswich and an array of HPGe detectors are estimated using skull and knee voxel phantoms. These phantoms are generated from International Commission of Radiation Protection reference male voxel phantom. The phantoms as well as 20 cm diameter phoswich, having 1.2 cm thick NaI (Tl) primary and 5cm thick CsI (Tl) secondary detector and an array of three HPGe detectors (each of diameter of 7 cm and thickness of 2.5 cm) are incorporated in Monte Carlo code 'FLUKA'. Biokinetic models of Pu, Am, U and Th are solved using default parameters to identify different parts of the skeleton where activity will accumulate after an inhalation intake of 1 Bq. Accordingly, CFs are evaluated for the uniform source distribution in trabecular bone and bone marrow (TBBM), cortical bone (CB) as well as in both TBBM and CB regions for photon energies of 18, 60, 63, 74, 93, 185 and 238 keV describing sources of (239)Pu, (241)Am, (238)U, (235)U and (232)Th. The CFs are also evaluated for non-uniform distribution of activity in TBBM and CB regions. The variation in the CFs for source distributed in different regions of the bones is studied. The assessment of skeletal activity of actinides from skull and knee activity measurements is discussed along with the errors.

  17. PRELIMINARY CROSS SECTION AND NU-BAR COVARIANCES FOR WPEC SUBGROUP 26

    SciTech Connect

    ROCHMAN,D.

    2007-01-31

    We report preliminary cross section covariances developed for the WPEC Subgroup 26 for 45 out of 52 requested materials. The covariances were produced in 15- and 187-group representations as follows: (1) 36 isotopes ({sup 16}O, {sup 19}F, {sup 23}Na, {sup 27}Al, {sup 28}Si, {sup 52}Cr, {sup 56,56}Fe, {sup 58}Ni, {sup 90,91,92,94}Zr, {sup 166,167,168,170}Er, {sup 206,207,208}Pb, {sup 209}Bi, {sup 233,234,236}U, {sup 237}Np, {sup 238,240,241,242}Pu, {sup 241,242m,243}Am, {sup 242,243,244,245}Cm) were evaluated using the BNL-LANL methodology. For the thermal region and the resolved and unresolved resonance regions, the methodology has been based on the Atlas-Kalman approach, in the fast neutron region the Empire-Kalman method has been used; (2) 6 isotopes ({sup 155,156,157,158,160}Gd and {sup 232}Th) were taken from ENDF/B-VII.0; and (3) 3 isotopes ({sup 1}H, {sup 238}U and {sup 239}Pu) were taken from JENDL-3.3. For 6 light nuclei ({sup 4}He, {sup 6,7}Li, {sup 9}Be, {sup 10}B, {sup 12}C), only partial cross section covariance results were obtained, additional work is needed and they do not report the results here. Likewise, the cross section covariances for {sup 235}U, which they recommend to take from JENDL-3.3, will be included once the multigroup processing is successfully completed. Covariances for the average number of neutrons per fission, total {nu}-bar, are provided for 10 actinides identified as priority by SG26. Further work is needed to resolve some of the issues and to produce covariances for the full set of 52 materials.

  18. The early thermal evolution of Mars

    NASA Astrophysics Data System (ADS)

    Bhatia, G. K.; Sahijpal, S.

    2016-01-01

    Hf-W isotopic systematics of Martian meteorites have provided evidence for the early accretion and rapid core formation of Mars. We present the results of numerical simulations performed to study the early thermal evolution and planetary scale differentiation of Mars. The simulations are confined to the initial 50 Myr (Ma) of the formation of solar system. The accretion energy produced during the growth of Mars and the decay energy due to the short-lived radio-nuclides 26Al, 60Fe, and the long-lived nuclides, 40K, 235U, 238U, and 232Th are incorporated as the heat sources for the thermal evolution of Mars. During the core-mantle differentiation of Mars, the molten metallic blobs were numerically moved using Stoke's law toward the center with descent velocity that depends on the local acceleration due to gravity. Apart from the accretion and the radioactive heat energies, the gravitational energy produced during the differentiation of Mars and the associated heat transfer is also parametrically incorporated in the present work to make an assessment of its contribution to the early thermal evolution of Mars. We conclude that the accretion energy alone cannot produce widespread melting and differentiation of Mars even with an efficient consumption of the accretion energy. This makes 26Al the prime source for the heating and planetary scale differentiation of Mars. We demonstrate a rapid accretion and core-mantle differentiation of Mars within the initial ~1.5 Myr. This is consistent with the chronological records of Martian meteorites.

  19. Uranium and Strontium Isotopic Study of the Hydrology of the Alluvial Aquifer at the Rifle Former U Mine Tailings Site, Colorado

    NASA Astrophysics Data System (ADS)

    Christensen, J. N.; Shiel, A. E.; Conrad, M. E.; Williams, K. H.; Dong, W.; Tokunaga, T. K.; Wan, J.; Long, P. E.; Hubbard, S. S.

    2014-12-01

    The Rifle Site consists of a floodplain along the Colorado River that was remediated through the removal of surface material underlying former uranium-vanadium mill tailings. The semi-arid (precip. = ~30 cm/year) catchment for the site has an area of ~1km2. The Rifle Site provides an excellent field laboratory for the study of the fluxes of water and carbon from the vadose zone to groundwater (LBNL SFA2.0, http://esd.lbl.gov/research/projects/sssfa2/). A network of monitoring wells, particularly a set instrumented in the vadose zone, provide the opportunity to closely sample groundwater and vadose zone porewater both in space and time. In order to better understand the spatial and temporal variation of vadose zone interaction with groundwater within the Rifle floodplain and provide constraints for a Rifle hydrological model, we have analyzed the Sr isotopic compositions, 234U/238U activity ratios, and d238U of groundwater, vadose zone porewater (sampled through depth-distributed lysimeters) and surface water including the Colorado River. Significant contrasts in 87Sr/86Sr and 234U/238U allow the identification of different sources contributing to Rifle groundwater, while d238U provides an additional tracer and insights into redox processes. Vadose zone porewater is characterized by high 87Sr/86Sr and Sr concentrations and falls at one end of a mixing line with Rifle groundwater, while upgradient groundwater with lower 87Sr/86Sr and Sr concentrations falls at the other end. A mixing model using vadose zone porewater and upgradient groundwater as endmembers suggests that the contribution of vertical recharge through the floodplain increases to ~20% systematically across the floodplain towards the Colorado River. An exception to this pattern is a well located 150m from the river with recent high U concentrations (>300 ppb) and U and Sr isotopic compositions consistent with a 38% vadose zone contribution. U and Sr isotopes show that an irrigation-return ditch that cuts

  20. A Record of Uranium-Series Transport in Fractured, Unsaturated Tuff at Nopal I, Sierra Peña Blanca, Chihuahua, Mexico

    NASA Astrophysics Data System (ADS)

    Denton, J.; Goldstein, S. J.; Paviet, P.; Nunn, A. J.; Amato, R. S.; Hinrichs, K. A.

    2015-12-01

    In this study we utilize U-series disequilibria measurements to investigate mineral fluid interactions and the role fractures play in the geochemical evolution of an analogue for a high level nuclear waste repository, the Nopal I uranium ore deposit. Samples of fracture-fill materials have been collected from a vertical drill core and surface fractures. High uranium concentrations in these materials (12-7700 ppm) indicate U mobility and transport from the deposit in the past. U concentrations generally decrease with horizontal distance away from the ore deposit but show no trend with depth. Isotopic activity ratios indicate a complicated geochemical evolution in terms of the timing and extent of actinide mobility, possibly due to changing environmental (redox) conditions over the history of the deposit. 234U/238U activity ratios are generally distinct from secular equilibrium and indicate some degree of open system U behavior during the past 1.2 Ma. However, calculated closed system 238U-234U-230Th model ages are generally >313 ka and >183 ka for the surface fracture and drill core samples respectively, suggesting closed system behavior for U and Th over this most recent time period. Whole rock isochrons drawn for the drill core samples show that at two of three depths fractures have remained closed with respect to U and Th mobility for >200 ka. However, open system behavior for U in the last 350 ka is suggested at 67 m depth. 231Pa/235U activity ratios within error of unity suggest closed system behavior for U and Pa for at least the past 185 ka. 226Ra/230Th activity ratios are typically <1 (0.7-1.2), suggesting recent (<8 ka) radium loss and mobility due to ongoing fluid flow in the fractures. Overall, the mainly closed system behavior of U-Th-Pa over the past ~200 ka provides one indicator of the geochemical immobility of these actinides over long time-scales for potential nuclear waste repositories sited in fractured, unsaturated tuff.

  1. Plutonium age dating reloaded

    NASA Astrophysics Data System (ADS)

    Sturm, Monika; Richter, Stephan; Aregbe, Yetunde; Wellum, Roger; Mayer, Klaus; Prohaska, Thomas

    2014-05-01

    Although the age determination of plutonium is and has been a pillar of nuclear forensic investigations for many years, additional research in the field of plutonium age dating is still needed and leads to new insights as the present work shows: Plutonium is commonly dated with the help of the 241Pu/241Am chronometer using gamma spectrometry; in fewer cases the 240Pu/236U chronometer has been used. The age dating results of the 239Pu/235U chronometer and the 238Pu/234U chronometer are scarcely applied in addition to the 240Pu/236U chronometer, although their results can be obtained simultaneously from the same mass spectrometric experiments as the age dating result of latter. The reliability of the result can be tested when the results of different chronometers are compared. The 242Pu/238U chronometer is normally not evaluated at all due to its sensitivity to contamination with natural uranium. This apparent 'weakness' that renders the age dating results of the 242Pu/238U chronometer almost useless for nuclear forensic investigations, however turns out to be an advantage looked at from another perspective: the 242Pu/238U chronometer can be utilized as an indicator for uranium contamination of plutonium samples and even help to identify the nature of this contamination. To illustrate this the age dating results of all four Pu/U clocks mentioned above are discussed for one plutonium sample (NBS 946) that shows no signs of uranium contamination and for three additional plutonium samples. In case the 242Pu/238U chronometer results in an older 'age' than the other Pu/U chronometers, contamination with either a small amount of enriched or with natural or depleted uranium is for example possible. If the age dating result of the 239Pu/235U chronometer is also influenced the nature of the contamination can be identified; enriched uranium is in this latter case a likely cause for the missmatch of the age dating results of the Pu/U chronometers.

  2. Enhanced techniques for the measurement of ultra-low level (pg and fg) actinide analysis by ICP-MS for forensic and geologic applications

    NASA Astrophysics Data System (ADS)

    Pollington, A. D.; Kinman, W.; Hanson, S. K.

    2014-12-01

    Recent advances in mass spectrometry have led to an improved ability to measure high precision isotope ratios at increasingly low analyte concentrations. Combining techniques for enhanced ionization with better counting of small ion beams, we routinely measure isotope ratios on 100's of pg uranium samples and ≤10 pg plutonium samples with relative standard deviations of 1‰ on major isotope ratios and 10‰ on minor ratios achievable. With slightly larger samples (≤1 ng total U), these precisions can be as low as 0.01‰ (10 ppm) and 1‰ respectively. These techniques can be applied to both nuclear forensics questions where only a small amount of sample is available, as well as geologic questions such as U-Pb or U-Th disequilibrium geochronology from either single small crystals, or microsampled domains from within a heterogeneous sample. The analytical setup is a Cetac Aridus II desolvating nebulizer interfaced with a ThermoScientific Neptune Plus equipped with a jet-type sample cone and x-type skimmer cone. The combination of the desolvating nebulizer with the enhanced cone setup leads to an increase in sensitivity on the order of 10x that of a standard glass spray chamber (~1000V/ppm U). The Neptune Plus is equipped with 9 Faraday cups and 5 electron multipliers (two behind RPQ energy filters for improved abundance sensitivtiy). This allows for the simultaneous collection of all isotopes of either U or Pu with a combination of Faraday cups (e.g., 235U and 238U) and electron multipliers (e.g., 234U and 236U) with other configurations also available (e.g., 235U and 238U can instead be measured on electron multipliers in small samples). As sample sizes get small, the contributions from environmental blanks, as well as interfering species, become increasing concerns. In this study, we will present data on efforts to minimize the contribution of environmental U using scaled down chemical procedures as well as the effect of polyatomic species on the precision

  3. Biogeochemical aspects of uranium mineralization, mining, milling, and remediation

    USGS Publications Warehouse

    Campbell, Kate M.; Gallegos, Tanya J.; Landa, Edward R.

    2015-01-01

    Natural uranium (U) occurs as a mixture of three radioactive isotopes: 238U, 235U, and 234U. Only 235U is fissionable and makes up about 0.7% of natural U, while 238U is overwhelmingly the most abundant at greater than 99% of the total mass of U. Prior to the 1940s, U was predominantly used as a coloring agent, and U-bearing ores were mined mainly for their radium (Ra) and/or vanadium (V) content; the bulk of the U was discarded with the tailings (Finch et al., 1972). Once nuclear fission was discovered, the economic importance of U increased greatly. The mining and milling of U-bearing ores is the first step in the nuclear fuel cycle, and the contact of residual waste with natural water is a potential source of contamination of U and associated elements to the environment. Uranium is mined by three basic methods: surface (open pit), underground, and solution mining (in situ leaching or in situ recovery), depending on the deposit grade, size, location, geology and economic considerations (Abdelouas, 2006). Solid wastes at U mill tailings (UMT) sites can include both standard tailings (i.e., leached ore rock residues) and solids generated on site by waste treatment processes. The latter can include sludge or “mud” from neutralization of acidic mine/mill effluents, containing Fe and a range of coprecipitated constituents, or barium sulfate precipitates that selectively remove Ra (e.g., Carvalho et al., 2007). In this chapter, we review the hydrometallurgical processes by which U is extracted from ore, the biogeochemical processes that can affect the fate and transport of U and associated elements in the environment, and possible remediation strategies for site closure and aquifer restoration.This paper represents the fourth in a series of review papers from the U.S. Geological Survey (USGS) on geochemical aspects of UMT management that span more than three decades. The first paper (Landa, 1980) in this series is a primer on the nature of tailings and radionuclide

  4. Temporal variation and provenance of thorium deposition observed at Tsukuba, Japan.

    PubMed

    Hirose, Katsumi; Kikawada, Yoshikazu; Igarashi, Yasuhito

    2012-06-01

    Temporal variations of monthly thorium (Th) deposition observed at Tsukuba, Japan during the period 1990-2007, comparing with plutonium deposition, was studied. The monthly (232)Th deposition as did (239,240)Pu, varied according to season and inter-annually. In particular, (232)Th deposition increased significantly in spring coinciding with Asian dust (Kosa) events. The (230)Th/(232)Th activity ratios vary according to sources and can therefore be used to differentiate between locally derived and remotely derived (232)Th. The (230)Th/(232)Th activity ratios in deposition samples showed large variability with high ratios occurring in early spring. These high (230)Th/(232)Th ratios in deposition can be attributed to local dust storms, especially in early spring, that cause resuspension of soils from cultivated fields which are characterized by high (230)Th/(232)Th activity ratios. The results reveal that both locally and remotely derived (232)Th deposition showed seasonal variations with maxima in spring, although the remotely derived fraction is dominant rather than the locally derived one. The (232)Th deposition maxima later in spring is attributable to the remotely derived fraction, corresponding to the Kosa events. Annual (232)Th deposition exhibited an increasing trend, suggesting the presence of sources other than soil dust such as fly ash from increasing coal burning.

  5. U-Pb Ages of Secondary Silica at Yucca Mountain, Nevada: Implications for the Paleohydrology of the Unsaturated Zone

    SciTech Connect

    L.A. Neymark; Y. Amelin; J.B. Paces; Z.E. Peterman

    2001-08-20

    U, Th, and Pb isotopes were analyzed in layers of opal and chalcedony from individual millimeter- to centimeter-thick calcite and silica coatings at Yucca Mountain, Nevada, USA, a site that is being evaluated for a potential high-level nuclear waste repository. These calcite and silica coatings on fractures and in lithophysal cavities in Miocene-age tuffs in the unsaturated zone (UZ) precipitated from descending water and record a long history of percolation through the UZ. Opal and chalcedony have high concentrations of U (10 to 780 ppm) and low concentrations of common Pb as indicated by large values of {sup 206}Pb/{sup 204}Pb (up to 53,806), thus making them suitable for U-Pb age determinations. Interpretations of U-Pb isotopes in opal samples at Yucca Mountain are complicated by the incorporation of excess {sup 234}U at the time of mineral formation, resulting in reverse discordance of U-Pb ages. However, the {sup 207}Pb/{sup 235}U ages are much less affected by deviation from initial secular equilibrium and provide reliable ages of most silica deposits between 0.6 and 9.8 Ma. For chalcedony subsamples showing normal age discordance, these ages may represent minimum times of deposition. Typically, {sup 207}Pb/{sup 235}U ages are consistent with the microstratigraphy in the mineral coating samples, such that the youngest ages are for subsamples from outer layers, intermediate ages are from inner layers, and oldest ages are from innermost layers. {sup 234}U and {sup 230}Th in most silica layers deeper in the coatings are in secular equilibrium with {sup 238}U, which is consistent with their old age and closed system behavior during the past 0.5 m.y. U-Pb ages for subsamples of silica layers from different microstratigraphic positions in individual calcite and silica coating samples collected from lithophysal cavities in the welded part of the Topopah Spring Tuff yield slow long-term average depositional rates of 1 to 5 mm/m.y. These data imply that the deeper

  6. U-Pb ages of secondary silica at Yucca Mountain, Nevada: Implications for the paleohydrology of the unsaturated zone

    USGS Publications Warehouse

    Neymark, L.A.; Amelin, Y.; Paces, J.B.; Peterman, Z.E.

    2002-01-01

    Uranium, Th and Pb isotopes were analyzed in layers of opal and chalcedony from individual mm- to cm-thick calcite and silica coatings at Yucca Mountain, Nevada, USA, a site that is being evaluated for a potential high-level nuclear waste repository. These calcite and silica coatings on fractures and in lithophysal cavities in Miocene-age tuffs in the unsaturated zone (UZ) precipitated from descending water and record a long history of percolation through the UZ. Opal and chalcedony have high concentrations of U (10 to 780 ppm) and low concentrations of common Pb as indicated by large values of 206Pb/204Pb (up to 53,806), thus making them suitable for U-Pb age determinations. Interpretations of U-Pb isotope systems in opal samples at Yucca Mountain are complicated by the incorporation of excess 234U at the time of mineral formation, resulting in reverse discordance of U-Pb ages. However, the 207PB/235U ages are much less affected by deviation from initial secular equilibrium and provide reliable ages of most silica deposits between 0.6 and 9.8 Ma. For chalcedony subsamples showing normal age discordance, these ages may represent minimum times of deposition. Typically, 207Pb/235U ages are consistent with the microstratigraphy in the mineral coating samples, such that the youngest ages are for subsamples from outer layers, intermediate ages are from inner layers, and oldest ages are from innermost layers. 234U and 230Th in most silica layers deeper in the coatings are in secular equilibrium with 238U, which is consistent with their old age and closed system behavior during the past -0.5 Ma. The ages for subsamples of silica layers from different microstratigraphic positions in individual calcite and silica coating samples collected from lithophysal cavities in the welded part of the Topopah Spring Tuff yield slow long-term average growth rates of 1 to 5 mm/Ma. These data imply that the deeper parts of the UZ at Yucca Mountain maintained long-term hydrologic stability

  7. Lead Slowing-Down Spectrometry for Spent Fuel Assay: FY12 Status Report

    SciTech Connect

    Warren, Glen A.; Anderson, Kevin K.; Casella, Andrew M.; Danon, Yaron; Devlin, M.; Gavron, A.; Haight, R. C.; Harris, Jason; Imel, G. R.; Kulisek, Jonathan A.; O'Donnell, J. M.; Stewart, T.; Weltz, Adam

    2012-10-01

    Executive Summary The Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign is supporting a multi-institutional collaboration to study the feasibility of using Lead Slowing Down Spectroscopy (LSDS) to conduct direct, independent and accurate assay of fissile isotopes in used fuel assemblies. The collaboration consists of Pacific Northwest National Laboratory (PNNL), Los Alamos National Laboratory (LANL), Rensselaer Polytechnic Institute (RPI), Idaho State University (ISU). There are three main challenges to implementing LSDS to assay used fuel assemblies. These challenges are the development of an algorithm for interpreting the data with an acceptable accuracy for the fissile masses, the development of suitable detectors for the technique, and the experimental benchmarking of the approach. This report is a summary of the progress in these areas made by the collaboration during FY2012. Significant progress was made on the project in FY2012. Extensive characterization of a “semi-empirical” algorithm was conducted. For example, we studied the impact on the accuracy of this algorithm by the minimization of the calibration set, uncertainties in the calibration masses, and by the choice of time window. Issues such a lead size, number of required neutrons, placement of the neutron source and the impact of cadmium around the detectors were also studied. In addition, new algorithms were developed that do not require the use of plutonium fission chambers. These algorithms were applied to measurement data taken by RPI and shown to determine the 235U mass within 4%. For detectors, a new concept for a fast neutron detector involving 4He recoil from neutron scattering was investigated. The detector has the potential to provide a couple of orders of magnitude more sensitivity than 238U fission chambers. Progress was also made on the more conventional approach of using 232Th fission chambers as fast neutron detectors. For

  8. Determination of ²²⁶Ra, ²²⁸Ra and ²¹⁰Pb in NORM products from oil and gas exploration: problems in activity underestimation due to the presence of metals and self-absorption of photons.

    PubMed

    Landsberger, S; Brabec, C; Canion, B; Hashem, J; Lu, C; Millsap, D; George, G

    2013-11-01

    Typical calibration of solid environmental samples for the determination of (226)Ra, (228)Ra and (210)Pb entails the use of standard reference materials which have a very similar matrix. However, TENORM samples from the oil and gas exploration contain unusually high amounts of calcium, strontium and barium which can severely attenuate the photons of (210)Pb and (226)Ra with their characteristic 46.1 keV and 186.2 keV gamma-rays, respectively and to some extent (228)Ra with the characteristic gamma-rays of 911.2 keV and 969.0 keV. We used neutron activation analysis to evaluate the content of TENORM for calcium, barium and strontium and then used a software program SELABS to determine the self-absorption. Our results confirm that even in Petrie containers with small dimensions the (210)Pb can be underestimated by almost by a factor of four while (226)Ra can be underestimated by 5%. The (228)Ra activities are virtually unaffected due to the higher energy gamma-rays. However, the implications for TENORM studies that employ large Marinelli containers having sample sizes between 0.25 and 1.0 L may be severely compromised by the presence of high Z elements in elevated concentrations. The usual spectral interferences on (226)Ra, (228)Ra and (210)Pb coming from other radionuclides in the (234)U, (235)U and (238)U decay chains are virtually nonexistent due the very high activity levels of (226)Ra, (228)Ra and (210)Pb in the tens of thousands of Bq/kg.

  9. Determination of elemental impurities and U and O isotopic compositions with a view to identify the geographical and industrial origins of uranium ore concentrates

    NASA Astrophysics Data System (ADS)

    Salaun, A.; Hubert, A.; Pointurier, F.; Aupiais, J.; Pili, E.; Richon, P.; Fauré, A.; Diallo, S.

    2012-12-01

    First events of illicit trafficking of nuclear and radiological materials occurred 50 years ago. Nuclear forensics expertise are aiming at determining the use of seized material, its industrial history and provenance (geographical area, place of production or processing), at assisting in the identification and dismantling of illicit trafficking networks. This information is also valuable in the context of inspections of declared facilities to verify the consistency of operator's declaration. Several characteristics can be used to determine the origin of uranium ore concentrates such as trace elemental impurity patterns (Keegan et al., 2008 ; Varga et al., 2010a, 2010b) or uranium, oxygen and lead isotopic compositions (Tamborini et al., 2002a, 2002b ; Wallenius et al., 2006; Varga et al., 2009). We developed analytical procedures for measuring the isotopic compositions of uranium (234U/238U and 235U/238U) and oxygen (18O/16O) and levels of elemental impurities (e.g. REE, Th) from very small amounts of uranium ore concentrates (or yellow cakes). Micrometer particles and few milligrams of material are used for oxygen isotope measurements and REE determination, respectively. Reference materials were analyzed by mass spectrometry (TIMS, SF-ICP-MS and SIMS) to validate testing protocols. Finally, materials of unknown origin were analyzed to highlight significant differences and determine whether these differences allow identifying the origin of these ore concentrates. References: Keegan, E., et al. (2008). Applied Geochemistry 23, 765-777. Tamborini, G., et al. (2002a). Analytical Chemistry 74, 6098-6101. Tamborini, G., et al. (2002b). Microchimica Acta 139, 185-188. Varga, Z., et al. (2009). Analytical Chemistry 81, 8327-8334. Varga, Z., et al. (2010a). Talanta 80, 1744-1749. Varga, Z., et al. (2010b). Radiochimica Acta 98, 771-778 Wallenius, M., et al. (2006). Forensic Science International 156, 55-62.

  10. Airborne Plutonium and non-natural Uranium from the Fukushima DNPP found at 120 km distance a few days after reactor hydrogen explosions.

    PubMed

    Shinonaga, Taeko; Steier, Peter; Lagos, Markus; Ohkura, Takehisa

    2014-04-01

    Plutonium (Pu) and non-natural uranium (U) originating from the Fukushima Daiichi Nuclear Power Plant (FDNPP) were identified in the atmosphere at 120 km distance from the FDNPP analyzing the ratio of number of atoms, following written as n(isotope)/n(isotope), of Pu and U. The n((240)Pu)/n((239)Pu), n((241)Pu)/n((239)Pu), n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U) in aerosol samples collected before and after the FDNPP incident were analyzed by accelerator mass spectrometry (AMS) and inductively coupled plasma mass spectrometry (ICPMS). The activity concentrations of (137)Cs and (134)Cs in the same samples were also analyzed by gamma spectrometry before the destructive analysis. Comparing the time series of analytical data on Pu and U obtained in this study with previously reported data on Pu, U, and radioactive Cs, we concluded that Pu and non-natural U from the FDNPP were transported in the atmosphere directly over a 120 km distance by aerosol and wind within a few days after the reactor hydrogen explosions. Effective dose of Pu were calculated using the data of Pu: (130 ± 21) nBq/m(3), obtained in this study. We found that the airborne Pu contributes only negligibly to the total dose at the time of the incident. However the analytical results show that the amount of Pu and non-natural U certainly increased in the environment after the incident.

  11. Neanderthal skeleton from Tabun: U-series data by gamma-ray spectrometry.

    PubMed

    Schwarcz, H P; Simpson, J J; Stringer, C B

    1998-12-01

    The Neanderthal hominid Tabun C1, found in Israel by Garrod & Bate, was attributed to either layer B or C of their stratigraphic sequence. We have used gamma-ray spectrometry to determine the 230Th/234U and 231Pa/235U ratios of two bones from this skeleton, the mandible and a femur. The ages calculated from these ratios depend on the uranium uptake history of the bones. Assuming a model of early U (EU) uptake the age of the Tabun C1 mandible is 34+/-5 ka. The EU age of the femur is 19+/-2 ka. The femur may have experienced continuous (linear) U uptake which would give an age of 33+/-4 ka, in agreement with the mandible's EU age, but implies marked inhomogeneity in U uptake history at the site. These new age estimates for the skeleton suggest that it was younger than deposits of layer C. This apparent age is less than those of other Neanderthals found in Israel, and distinctly younger than the ages of the Skhul and Qafzeh burials. This suggests that Neanderthals did not necessarily coexist with the earliest modern humans in the region. All of the more complete Neanderthal fossils from Israel are now dated to the cool period of the last glacial cycle, suggesting that Neanderthals may have arrived in this region as a result of the southward expansion of their habitable range. The young age determined for the Tabun skeleton would suggest that Neanderthals survived as late in the Levant as they did in Europe.

  12. Extended Late Pleistocene Sea Level Record

    NASA Astrophysics Data System (ADS)

    Fairbanks, R. G.; Cao, L.; Mortlock, R. A.

    2006-12-01

    Several hundred new closed system 230Th/234U and radiocarbon dates and the addition of more cores and coral samples from the islands of Barbados, Kiritimati and Araki contribute to an enhanced sea level record for the late Pleistocene ranging from the present to 240,000 yrs BP. Application of more rigorous sample screening criteria, including redundant 231Pa/235U dates have resulted in more closed system ages and better sea level resolution. In addition, a multibeam survey has mapped an extensive glacial lowstand reef on a ridge south of Barbados that is capped by a set of pinnacle reefs that grew during the early deglaciation. Among our new observations, the more detailed Barbados sea level record now resolves a Younger Dryas still- stand and a sea level drop between 16,140 and 14,690, overlapping the timing of H1 by some age estimates. The coral ages bracketing melt water pulse 1A have been further refined to 14,082 +/- 28 yrs BP and 13,632 +/- 32 yrs BP (2-sigma). The Isotope Stage 3 interstadial ended with sea level near 87.5 meters below present at 29,500 years ago before dropping to full glacial levels. The last glacial sea level lowstand began as early as 26,000 yrs BP. Extensive dating of Marine Isotope Stage 3 interstadial reefs on the islands of Araki and Barbados have added considerable resolution to this time interval and reliably bracket lowstand intervals separating the interstadials. A new diagenesis model has improved our prospecting success for closed system ages from older reefs and added some critical dates to the sparse closed-system data set for MIS-5 and MIS-7 high stand reefs..

  13. The use of non-destructive passive neutron measurement methods in dismantling and radioactive waste characterization

    SciTech Connect

    Jallu, F.; Allinei, P. G.; Bernard, P.; Loridon, J.; Soyer, P.; Pouyat, D.; Torreblanca, L.; Reneleau, A.

    2011-07-01

    The cleaning up and dismantling of nuclear facilities lead to a great volume of technological radioactive wastes which need to be characterized in order to be sent to the adequate final disposal or interim storage. The control and characterization can be performed with non-destructive nuclear measurements such as gamma-ray spectrometry. Passive neutron counting is an alternative when the alpha-gamma emitters cannot be detected due to the presence of a high gamma emission resulting from fission or activation products, or when the waste matrix is too absorbing for the gamma rays of interest (too dense and/or made of high atomic number elements). It can also be a complement to gamma-ray spectrometry when two measurement results must be confronted to improve the confidence in the activity assessment. Passive neutron assays involve the detection of spontaneous fission neutrons emitted by even nuclides ({sup 238}Pu, {sup 240}Pu, {sup 242}Pu, {sup 242}Cm, {sup 244}Cm...) and neutrons resulting from ({alpha}, n) reactions with light nuclides (O, F, Be...). The latter is conditioned by the presence of high {alpha}-activity radionuclides ({sup 234}U, {sup 238}Pu, {sup 240}Pu, {sup 241}Am...) and low-Z elements, which depends on the chemical form (metallic, oxide or fluorine) of the plutonium or uranium contaminant. This paper presents the recent application of passive neutron methods to the cleaning up of a nuclear facility located at CEA Cadarache (France), which concerns the Pu mass assessment of 2714 historic, 100 litre radioactive waste drums produced between 1980 and 1997. Another application is the dismantling and decommissioning of an uranium enrichment facility for military purposes, which involves the {sup 235}U and total uranium quantifications in about a thousand, large compressors employed in the gaseous diffusion enrichment process. (authors)

  14. Study of radioactive isotopes of beryllium, polonium, uranium, and plutonium in the atmosphere

    SciTech Connect

    Lee, S.C.

    1986-01-01

    Radiochemical measurements were carried out for /sup 239.240/Pu in a total of 94 rain and snow samples collected at Fayetteville (36/sup 0/ N, 94/sup 0/W), Arkansas, during the period between May 1983 and November 1985. The concentrations of /sup 7/Be in most of these samples were also measured and these results were compared with previous samples. Average concentrations of cosmic-ray-produced radionuclide /sup 7/Be in rain remained fairly constant year after year. The annual rate of /sup 7/Be deposition at Fayetteville, Arkansas, was calculated from these data to be 5.2 dpm/cm/sup 2//year, which corresponds to a value of 2.8 x 10/sup -2/ atoms/cm/sup 2//second for the /sup 7/Be production rate in the atmosphere. The concentrations of bomb-produced radionuclides such as /sup 89/Sr, /sup 90/Sr and /sup 239.240/Pu in rain have drastically decreased since the last nuclear test explosion was conducted by the government of People's Republic of China in 1980. The concentrations of uranium isotopes and radon daughters in rain, on the other hand, were found to be affected by atmospheric injections of volcanic ashes from the 1980 eruption of Mount St. Helens and the 1982 eruption of El Chichon volcano in Mexico. Moreover, the burnups of the nuclear-powered Soviet satellites have caused marked increases in the levels of /sup 235/U and /sup 234/U in some of the rain samples. A sharp increase in the /sup 210/Po//sup 7/Be ratio in rain samples collected toward the end of 1980 and the beginning of 1981 was attributed to an atmospheric injection of /sup 210/Po from a series of major eruptions of Mount St. Helens.

  15. Fallout of uranium and plutonium from recent volcanic eruptions

    SciTech Connect

    Sandoval, D.N.

    1984-01-01

    The concentrations of /sup 234/U, /sup 235/U, /sup 238/U in rain water were measured in a total of 102 individual samples which were collected at Fayetteville, Arkansas, from July 1980 through April 1983. A spectacular increase in the heavy isotope of uranium (/sup 238/U) was observed in the months of July, August (1980); January through April, November and December 1981. This large increase in /sup 238/U in rain appeared to have had its origin in the May 1980 eruption of Mount St. Helens. An increase in the concentration of /sup 238/U in rain, smaller than 1981, was observed, which seems to have originated from the El Chichon volcano eruption in March 1982, and the spring peak or so-called cycling effect. A striking increase in the average bimonthly concentration of /sup 239,240/Pu occurred during the months of September-October 1980 (15.6 fCi/l) and March-April 1981 (29.4 fCi/l). The excess deposition of /sup 239,240/Pu brought down by the rain at Fayetteville, Arkansas, from March 1980 through December 1982 was found to be 1.01 fCi/cm/sup 2/. The total amount of /sub 239,240/Pu deposited at Fayetteville, Arkansas, from March through December 1982, was found to be about 30 times higher than the total amount calculated from reported literature values. The excess /sup 239,240/Pu has been attributed to stratospheric /sub 239,240/Pu from nuclear weapons testing prior to the 25th Chinese nuclear test.

  16. Radionuclide Concentrations in soils an Vegetation at Low-Level Radioactive Waste Disposal Area G During 2004

    SciTech Connect

    P.R. Fresquez; E.A. Lopez

    2004-11-01

    Soil samples were collected at 15 locations and unwashed overstory and understory vegetation samples were collected at nine locations within and around the perimeter of Area G, the primary disposal facility for low-level radioactive solid waste at Los Alamos National Laboratory (LANL). These samples were analyzed for {sup 3}H, {sup 238}Pu, {sup 239,240}Pu, {sup 90}Sr, {sup 241}Am, {sup 137}Cs, {sup 234}U, {sup 235}U, and {sup 238}U. Soil samples collected at Area G contained detectable concentrations of 3H (27%), {sup 239,240}Pu (60%), {sup 238}Pu (40%), and {sup 241}Am (47%) above regional statistical reference levels (RSRLs). In contrast, the levels of {sup 137}Cs, {sup 90}Sr, and U in all of the soil samples at Area G were either nondetectable or within RSRLs. The highest levels of {sup 3}H in soils were detected in the southwestern portion of Area G near the {sup 3}H shafts, whereas the highest concentrations of the Pu isotopes were detected in the northern and northeastern portions. All concentrations of {sup 3}H and Pu in soils, however, were far below LANL screening action levels. As for vegetation, most radionuclides in/on plants were either nondetectable or within RSRLs. The exceptions were {sup 3}H in overstory and some understory vegetation, particularly in the southwestern portion of Area G, which correlated very well with the soils data in that area. Also, there was some foliar contamination from {sup 241}Am and Pu isotopes in/on a few plant samples--the highest concentrations occurring in the northern section of Area G.

  17. Uranium isotopic composition and uranium concentration in special reference material SRM A (uranium in KCl/LiCl salt matrix)

    SciTech Connect

    Graczyk, D.G.; Essling, A.M.; Sabau, C.S.; Smith, F.P.; Bowers, D.L.; Ackerman, J.P.

    1997-07-01

    To help assure that analysis data of known quality will be produced in support of demonstration programs at the Fuel Conditioning Facility at Argonne National Laboratory-West (Idaho Falls, ID), a special reference material has been prepared and characterized. Designated SRM A, the material consists of individual units of LiCl/KCl eutectic salt containing a nominal concentration of 2.5 wt. % enriched uranium. Analyses were performed at Argonne National Laboratory-East (Argonne, IL) to determine the uniformity of the material and to establish reference values for the uranium concentration and uranium isotopic composition. Ten units from a batch of approximately 190 units were analyzed by the mass spectrometric isotope dilution technique to determine their uranium concentration. These measurements provided a mean value of 2.5058 {+-} 0.0052 wt. % U, where the uncertainty includes estimated limits to both random and systematic errors that might have affected the measurements. Evidence was found of a small, apparently random, non-uniformity in uranium content of the individual SRM A units, which exhibits a standard deviation of 0.078% of the mean uranium concentration. Isotopic analysis of the uranium from three units, by means of thermal ionization mass spectrometry with a special, internal-standard procedure, indicated that the uranium isotopy is uniform among the pellets with a composition corresponding to 0.1115 {+-} 0.0006 wt. % {sup 234}U, 19.8336 {+-} 0.0059 wt. % {sup 235}U, 0.1337 {+-} 0.0006 wt. % {sup 236}U, and 79.9171 {+-} 0.0057 wt. % {sup 238}U.

  18. High resolution isotopic analysis of U-bearing particles via fusion of SIMS and EDS images

    SciTech Connect

    Tarolli, Jay G.; Naes, Benjamin E.; Garcia, Benjamin J.; Fischer, Ashley E.; Willingham, David

    2016-01-01

    Image fusion of secondary ion mass spectrometry (SIMS) images and X-ray elemental maps from energy-dispersive spectroscopy (EDS) was performed to facilitate the isolation and re-analysis of isotopically unique U-bearing particles where the highest precision SIMS measurements are required. Image registration, image fusion and particle micromanipulation were performed on a subset of SIMS images obtained from a large area pre-screen of a particle distribution from a sample containing several certified reference materials (CRM) U129A, U015, U150, U500 and U850, as well as a standard reference material (SRM) 8704 (Buffalo River Sediment) to simulate particles collected on swipes during routine inspections of declared uranium enrichment facilities by the International Atomic Energy Agency (IAEA). In total, fourteen particles, ranging in size from 5 – 15 µm, were isolated and re-analyzed by SIMS in multi-collector mode identifying nine particles of CRM U129A, one of U150, one of U500 and three of U850. These identifications were made within a few percent errors from the National Institute of Standards and Technology (NIST) certified atom percent values for 234U, 235U and 238U for the corresponding CRMs. This work represents the first use of image fusion to enhance the accuracy and precision of isotope ratio measurements for isotopically unique U-bearing particles for nuclear safeguards applications. Implementation of image fusion is essential for the identification of particles of interests that fall below the spatial resolution of the SIMS images.

  19. Investigating Pu and U isotopic compositions in sediments: a case study in Lake Obuchi, Rokkasho Village, Japan using sector-field ICP-MS and ICP-QMS.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2005-08-01

    The objectives of the present work were to study isotope ratios and the inventory of plutonium and uranium isotope compositions in sediments from Lake Obuchi, which is in the vicinity of several nuclear fuel facilities in Rokkasho, Japan. Pu and its isotopes were determined using sector-field ICP-MS and U and its isotopes were determined with ICP-QMS after separation and purification with a combination of ion-exchange and extraction chromatography. The observed (240)Pu/(239)Pu atom ratio (0.186 +/- 0.016) was similar to that of global fallout, indicating that the possible early tropospheric fallout Pu did not deliver Pu from the Pacific Proving Ground to areas above 40 degrees N. The previously reported higher Pu inventory in the deep water area of Lake Obuchi could be attributed to the lateral transportation of Pu deposited in the shallow area which resulted from the migration of deposited global fallout Pu from the land into the lake by river runoff and from the Pacific Ocean by tide movement and sea water scavenging, as well as from direct soil input by winds. The (235)U/(238)U atom ratios ranged from 0.00723 to 0.00732, indicating the natural origin of U in the sediments. The average (234)U/(238)U activity ratio of 1.11 in a sediment core indicated a significant sea water U contribution. No evidence was found for the release of U containing wastes from the nearby nuclear facilities. These results will serve as a reference baseline on the levels of Pu and U in the studied site so that any further contamination from the spent nuclear fuel reprocessing plants, the radioactive waste disposal and storage facilities, and the uranium enrichment plant can be identified, and the impact of future release can be rapidly assessed.

  20. Identifying the sources of subsurface contamination at the Hanford site in Washington using high-precision uranium isotopic measurements

    SciTech Connect

    Christensen, John N.; Dresel, P. Evan; Conrad, Mark E.; Maher, Kate; DePaolo, Donald J.

    2004-03-30

    In the mid-1990s, a groundwater plume of uranium (U) was detected in monitoring wells in the B-BX-BY Waste Management Area (WMA) at the Hanford Site in Washington. This area has been used since the late 1940s to store high-level radioactive waste and other products of U fuel-rod processing. Using multiple collector ICP source magnetic sector mass spectrometry (MC ICPMS) high precision uranium isotopic analyses were conducted of samples of vadose zone contamination and of groundwater. The ratios {sup 236}U/{sup 238}U, {sup 234}U/{sup 238}U and {sup 238}U/{sup 235}U are used to distinguish contaminant sources. Based on the isotopic data, the source of the groundwater contamination appears to be related to a 1951 overflow event at tank BX-102 that spilled high level U waste into the vadose zone. The U isotopic variation of the groundwater plume is a result of mixing between contaminant U from this spill and natural background U. Vadose zone U contamination at tank B-110 likely predates the recorded tank leak and can be ruled out as a source of groundwater contamination, based on the U isotopic composition. The locus of vadose zone contamination is displaced from the initial locus of groundwater contamination, indicating that lateral migration in the vadose zone was at least 8 times greater than vertical migration. The time evolution of the groundwater plume suggests an average U migration rate of {approx}0.7-0.8 m/day showing slight retardation relative to a ground water flow of {approx}1 m/day.

  1. Comparison of Grab, Air, and Surface Results for Radiation Site Characterization

    NASA Astrophysics Data System (ADS)

    Glassford, Eric Keith

    2011-12-01

    The use of proper sampling methods and sample types for evaluating sites believed to be contaminated with radioactive materials is necessary to avoid misrepresenting conditions at the site. This study was designed to investigate if the site characterization, based upon uranium contamination measured in different types of samples, is dependent upon the mass of the sample collected. A bulk sample of potentially contaminated interior dirt was collected from an abandoned metal processing mill that rolled uranium between 1948 and 1956. The original mill dates from 1910 and has a dirt floor. The bulk sample was a mixture of dirt, black and yellow particles of metal dust, and small fragments of natural debris. Small mass (approximately 0.75 grams (g)) and large mass (approximately 70g) grab samples were prepared from the bulk sample material to simulate collection of a "grab" type sample. Air sampling was performed by re-suspending a portion of the bulk sample material using a vibration table to simulate airborne contamination that might be present during site remediation. Additionally, samples of removable contaminated surface dust were collected on 47 mm diameter filter paper by wiping the surfaces of the exposure chamber used to resuspend the bulk material. Certified reference materials, one containing a precisely known quantity of U 3O8 and one containing a known quantity of natural uranium, were utilized to calibrate the gamma spectrometry measurement system. Non-destructive gamma spectrometry measurements were used to determine the content of uranium-235 (235U) at 185 keV and 143 keV, thorium-234 (234Th) at 63 keV, and protactinium-234m (234mPa) at 1001 keV in each sample. Measurement of natura