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Sample records for 234u 235u 236u

  1. Determination of 234U/238U, 235U/238U and 236U/238U isotope ratios in urine using sector field inductively coupled plasma mass spectrometry.

    PubMed

    Xiao, Ge; Jones, Robert L; Saunders, David; Caldwell, Kathleen L

    2014-12-01

    Quantification of the isotopic composition of uranium in urine at low levels of concentration is important for assessing both military and civilian populations' exposures to uranium. However, until now there has been no convenient, precise method established for rapid determination of multiple uranium isotope ratios. Here, the authors report a new method to measure (234)U/(238)U, (235)U/(238)U and (236)U/(238)U. It uses solid-phase chelation extraction (via TRU columns) of actinides from the urine matrix, followed by measurement using a magnetic sector field inductively coupled plasma mass spectrometer (SF-ICP-MS-Thermo Element XR) equipped with a high-efficiency nebulizer (Apex PFA microflow) and coupled with a membrane desolvating nebulizer system (Aridus II™). This method provides rapid and reliable results and has been used successfully to analyse Certified Reference Materials. PMID:24563523

  2. Determination of 234U/238U, 235U/238U and 236U/238U Isotope Ratios in Urine Using Sector Field Inductively Coupled Plasma Mass Spectrometry (SF-ICP-MS)

    PubMed Central

    Xiao, Ge; Jones, Robert L.; Saunders, David; Caldwell, Kathleen L.

    2016-01-01

    Quantification of the isotopic composition of uranium in urine at low levels of concentration is important for assessing both military and civilian populations’ exposures to uranium. However, until now there has been no convenient, precise method established for rapid determination of multiple uranium isotope ratios. Here we report a new method to measure 234U/238U, 235U/238U and 236U/238U. It uses solid phase chelation extraction (via TRU columns) of actinides from the urine matrix, followed by measurement using a magnetic sector field inductively coupled plasma mass spectrometer (SF-ICP-MS - Thermo Element XR) equipped with a high efficiency nebulizer (Apex PFA microflow) and coupled with a membrane desolvating introduction system (Aridus II™). This method provides rapid and reliable results, and has been used successfully to analyze Certified Reference Materials (CRM). PMID:24563523

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

    NASA Astrophysics Data System (ADS)

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

    2006-03-01

    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-π 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.

  4. 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.

  5. 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.

  6. 206Pb- 230Th- 234U- 238U and 207Pb- 235U geochronology of Quaternary opal, Yucca Mountain, Nevada

    NASA Astrophysics Data System (ADS)

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

    2000-09-01

    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/ 238U activity, and 230Th/ 238U activity. 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-lived isotopes are

  7. 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

  8. Redundant 230Th/ 234U/ 238U, 231Pa/ 235U and 14C dating of fossil corals for accurate radiocarbon age calibration

    NASA Astrophysics Data System (ADS)

    Chiu, Tzu-Chien; Fairbanks, Richard G.; Mortlock, Richard A.; Cao, Li; Fairbanks, Todd W.; Bloom, Arthur L.

    2006-09-01

    230Th/ 234U/ 238U dating of fossil corals by mass spectrometry is remarkably precise, but some samples exposed to freshwater over thousands of years may gain and/or lose uranium and/or thorium and consequently yield inaccurate ages. Although a δ 234U initial value equivalent to modern seawater and modern corals has been an effective quality control criterion, for samples exposed to freshwater but having δ 234U initial values indistinguishable from modern seawater and modern corals, there remains a need for additional age validation in the most demanding applications such as the 14C calibration (Fairbanks et al., 2005. Radiocarbon calibration curve spanning 0 to 50,000 years BP based on paired 230Th/ 234U/ 238U and 14C dates on pristine corals. Quaternary Science Reviews 24(16-17), 1781-1796). In this paper we enhance screening criteria for fossil corals older than 30,000 years BP in the Fairbanks0805 radiocarbon calibration data set (Fairbanks et al., 2005) by measuring redundant 230Th/ 234U/ 238U and 231Pa/ 235U dates via multi-collector magnetic sector inductively coupled plasma mass spectrometry (MC-MS-ICPMS) using techniques described in Mortlock et al. (2005. 230Th/ 234U/ 238U and 231Pa/ 235U ages from a single fossil coral fragment by multi-collector magnetic-sector inductively coupled plasma mass spectrometry. Geochimica et Cosmochimica Acta 69(3), 649-657.). In our present study, we regard paired 231Pa/ 235U and 230Th/ 234U/ 238U ages concordant when the 231Pa/ 235U age (±2 σ) overlaps with the associated 230Th/ 234U/ 238U age (±2 σ). Out of a representative set of 11 Fairbanks0805 (Fairbanks et al., 2005) radiocarbon calibration coral samples re-measured in this study, nine passed this rigorous check on the accuracy of their 230Th/ 234U/ 238U ages. The concordancy observed between 230Th/ 234U/ 238U and 231Pa/ 235U dates provides convincing evidence to support closed system behavior of these fossil corals and validation of their 230Th/ 234U/ 238U

  9. Analysis of prompt fission neutrons in 235U(nth,f) and fission fragment distributions for the thermal neutron induced fission of 234U

    NASA Astrophysics Data System (ADS)

    Al-Adili, A.; Tarrío, D.; Hambsch, F.-J.; Göök, A.; Jansson, K.; Solders, A.; Rakopoulos, V.; Gustafsson, C.; Lantz, M.; Mattera, A.; Oberstedt, S.; Prokofiev, A. V.; Vidali, M.; Österlund, M.; Pomp, S.

    2016-06-01

    This paper presents the ongoing analysis of two fission experiments. Both projects are part of the collaboration between the nuclear reactions group at Uppsala and the JRC-IRMM. The first experiment deals with the prompt fission neutron multiplicity in the thermal neutron induced fission of 235U(n,f). The second, on the fission fragment properties in the thermal fission of 234U(n,f). The prompt fission neutron multiplicity has been measured at the JRC-IRMM using two liquid scintillators in coincidence with an ionization chamber. The first experimental campaign focused on 235U(nth,f) whereas a second experimental campaign is foreseen later for the same reaction at 5.5 MeV. The goal is to investigate how the so-called sawtooth shape changes as a function of fragment mass and excitation energy. Some harsh experimental conditions were experienced due to the large radiation background. The solution to this will be discussed along with preliminary results. In addition, the analysis of thermal neutron induced fission of 234U(n,f) will be discussed. Currently analysis of data is ongoing, originally taken at the ILL reactor. The experiment is of particular interest since no measurement exist of the mass and energy distributions for this system at thermal energies. One main problem encountered during analysis was the huge background of 235U(nth,f). Despite the negligible isotopic traces in the sample, the cross section difference is enormous. Solution to this parasitic background will be highlighted.

  10. Giant resonance for the actinide nuclei: Photoneutron and photofission cross sections for /sup 235/U, /sup 236/U, /sup 238/U, and /sup 232/Th

    SciTech Connect

    Caldwell, J.T.; Dowdy, E.J.; Berman, B.L.; Alvarez, R.A.; Meyer, P.

    1980-04-01

    The photoneutron cross sections sigma (..gamma..,n) and sigma (..gamma..,2n), and total photofission cross sections sigma (..gamma..,F) have been measured for /sup 235/U, /sup 236/U, /sup 238/U, and /sup 232/Th from threshold to 18.3 MeV using monoenergetic photons from the annihilation in flight of fast positrons and neutron-multiplicity detection in an efficient 4..pi.. neutron detector. Use of the ring-ratio technique allowed both the average photofission neutron energy for each nucleus to be obtained as a function of photon energy and, for /sup 236/U and /sup 238/U, the determination of the partial cross sections for first-chance sigma (..gamma.., f ) and second-chance sigma (..gamma..,n f ) photofission as well. Information extracted from the data includes integrated cross sections and their moments, giant-resonance parameters, deformation and radius parameters, and relative and absolute neutron and fission probabilities.

  11. 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. PMID:25913057

  12. 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

  13. 230Th/ 234U/ 238U and 231Pa/ 235U ages from a single fossil coral fragment by multi-collector magnetic-sector inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Mortlock, Richard A.; Fairbanks, Richard G.; Chiu, Tzu-chien; Rubenstone, James

    2005-02-01

    The 230Th/ 234U/ 238U age dating of corals via alpha counting or mass spectrometry has significantly contributed to our understanding of sea level, radiocarbon calibration, rates of ocean and climate change, and timing of El Nino, among many applications. Age dating of corals by mass spectrometry is remarkably precise, but many samples exposed to freshwater yield inaccurate ages. The first indication of open-system 230Th/ 234U/ 238U ages is elevated 234U/ 238U initial values, very common in samples older than 100,000 yr. For samples younger than 100,000 yr that have 234U/ 238U initial values close to seawater, there is a need for age validation. Redundant 230Th/ 234U/ 238U and 231Pa/ 235U ages in a single fossil coral fragment are possible by Multi-Collector Magnetic Sector Inductively Coupled Plasma Mass Spectrometry (MC-MS-ICPMS) and standard anion exchange column chemistry, modified to permit the separation of uranium, thorium, and protactinium isotopes from a single solution. A high-efficiency nebulizer employed for sample introduction permits the determination of both 230Th/ 234U/ 238U and 231Pa/ 235U ages in fragments as small as 500 mg. We have obtained excellent agreement between 230Th/ 234U/ 238U and 231Pa/ 235U ages in Barbados corals (30 ka) and suggest that the methods described in this paper can be used to test the 230Th/ 234U/ 238U age accuracy. Separate fractions of U, Th, and Pa are measured by employing a multi-dynamic procedure, whereby 238U is measured on a Faraday cup simultaneously with all minor isotopes measured with a Daly ion counting detector. The multi-dynamic procedure also permits correcting for both the Daly to Faraday gain and for mass discrimination during sample analyses. The analytical precision of 230Th/ 234U/ 238U and 231Pa/ 235U dates is generally better than ±0.3% and ±1.5%, respectively (2 Relative Standard deviation [RSD]). Additional errors resulting from uncertainties in the decay constant for 231Pa and from undetermined

  14. Rotation of the compound nucleus 236U ∗ in the fission reaction 235U( n,f) induced by cold polarised neutrons

    NASA Astrophysics Data System (ADS)

    Goennenwein, F.; Mutterer, M.; Gagarski, A.; Guseva, I.; Petrov, G.; Sokolov, V.; Zavarukhina, T.; Gusev, Yu.; von Kalben, J.; Nesvizhevski, V.; Soldner, T.

    2007-08-01

    Surprisingly, for one of the best investigated nuclear reactions a new phenomenon was discovered. In an experiment performed at the High Flux Reactor of the Institut Laue Langevin in Grenoble, France, the reaction 235U(n , f) was studied. Fission was induced by cold polarised neutrons. Besides the two main fragments also ternary light charged particles were measured. The centres or the detector assemblies for fragments and light particles were positioned at right angles relative to each other in a plane perpendicular to the neutron beam. It is well known that the majority of ternary particles are emitted closely perpendicular to the fission axis. With the neutron spin pointing parallel or anti-parallel to the neutron beam it was observed that, upon flipping periodically the neutron spin, the distributions of angles between fragments and light particles are wobbling back and forth. The phenomenon is traced to the rotation of the scissioning nucleus while the light particles are ejected. This interpretation is corroborated by trajectory calculations for ternary α-particles being accelerated in a rotating Coulomb field provided by the two main fragments. The angle through which the fission axis and the trajectories of α-particles rotate is very small and barely exceeds 0.2°. This so far unreported feature of nuclear fission has been called the “ROT-effect”.

  15. Fission cross sections of some thorium, uranium, neptunium and plutonium isotopes relative to /sup 235/U

    SciTech Connect

    Meadows, J W

    1983-10-01

    Earlier results from the measurements, at this Laboratory, of the fission cross sections of /sup 230/Th, /sup 232/Th, /sup 233/U, /sup 234/U, /sup 236/U, /sup 238/U, /sup 237/Np, /sup 239/Pu, /sup 240/Pu, and /sup 242/Pu relative to /sup 235/U are reviewed with revisions to include changes in data processing procedures, alpha half lives and thermal fission cross sections. Some new data have also been included. The current experimental methods and procedures and the sample assay methods are described in detail and the sources of error are presented in a systematic manner. 38 references.

  16. Neutron induced fission of 234U

    NASA Astrophysics Data System (ADS)

    Hambsch, F.-J.; Al-Adili, A.; Oberstedt, S.; Pomp, S.

    2012-02-01

    The fission fragment properties of 234U(n,f) were investigated as a function of incident neutron energy from 0.2 MeV up to 5 MeV. The fission fragment mass, angular distribution and kinetic energy were measured with a double Frisch-grid ionization chamber using both analogue and digital data acquisition techniques. The reaction 234U(n,f) is relevant, since it involves the same compound nucleus as formed after neutron evaporation from highly excited 236U*, the so-called second-chance fission of 235U. Experimental data on fission fragment properties like fission fragment mass and total kinetic energy (TKE) as a function of incident neutron energy are rather scarce for this reaction. For the theoretical modelling of the reaction cross sections for Uranium isotopes this information is a crucial input parameter. In addition, 234U is also an important isotope in the Thorium-based fuel cycle. The strong anisotropy of the angular distribution around the vibrational resonance at En = 0.77 MeV could be confirmed using the full angular range. Fluctuations in the fragment TKE have been observed in the threshold region around the strong vibrational resonance at En = 0.77 MeV. The present results are in contradiction with corresponding literature values. Changes in the mass yield around the vibrational resonance and at En = 5 MeV relative to En = 2 MeV show a different signature. The drop in mean TKE around 2.5 to 3 MeV points to pair breaking as also observed in 235,238U(n,f). The measured two-dimensional mass yield and TKE distribution have been described in terms of fission modes. The yield of the standard 1 (S1) mode shows fluctuations in the threshold of the fission cross section due to the influence of the resonance and levels off at about 20% yield for higher incident neutron energies. The S2 mode shows the respective opposite behaviour. The mean TKE of both modes decreases with En. The decrease in mean TKE overrules the increase in S1 yield, so the mean TKE is dropping

  17. Concentrations of 238U, 234U, 235U, 232Th, 230Th, 228Th, 226Ra, 228Ra, 224Ra, 210Po, 210Pb and 212Pb in drinking water in Italy: reconciling safety standards based on measurements of gross alpha and beta.

    PubMed

    Jia, Guogang; Torri, Giancarlo; Magro, Leandro

    2009-11-01

    Some important naturally occurring alpha- and beta-radionuclides in drinking water samples collected in Italy were determined and the radiological quality evaluated. The mean activity concentrations (mBqL(-1)) of the radionuclides in the water samples were almost in the order: 26+/-36 ((234)U)>21+/-30 ((238)U)>8.9+/-15 ((226)Ra)>4.8+/-6.3 ((228)Ra)>4.0+/-4.1 ((210)Pb)>3.2+/-3.7 ((210)Po)>2.7+/-1.2 ((212)Pb)>1.4+/-1.8 ((224)Ra)> 1.1+/-1.3 ((235)U)>0.26+/-0.39 ((228)Th)>0.0023+/-0.0009 ((230)Th)>0.0013+/-0.0006 ((232)Th). The mean estimated dose (microSvyr(-1)) to an adult from the water intake was in this order: 2.8+/-3.3 ((210)Po)>2.4+/-3.2 ((228)Ra)>2.1+/-2.1 ((210)Pb)>1.8+/-3.1 ((226)Ra)>0.94+/-1.30 ((234)U)>0.70+/-0.98 ((238)U)>0.069+/-0.087 ((224)Ra)>0.036+/-0.044 ((235)U)>0.014+/-0.021 ((228)Th)>0.012+/-0.005 ((212)Pb)>0.00035+/-0.00029 ((230)Th)>0.00022+/-0.00009 ((232)Th). It is obvious that (210)Po, (228)Ra, (210)Pb and (226)Ra are the most important dose contributors in the drinking water intake. As far as the seventeen brands of analysed drinking water were concerned, the committed effective doses were in the range of 2.81-38.5 microSvyr(-1), all well below the reference level of the committed effective dose (100 microSvyr(-1)) recommended by the WHO. These data throw some light on the scale of the radiological impact on the public from some naturally occurring radionuclides in drinking water, and can also serve as a comparison for the dose contribution from artificial radionuclides released to the environment as a result of human practices. Based on the radionuclide composition in the analysed waters, comment was made on the new screening level for gross alpha activity in guidelines for drinking-water quality recommended by the WHO, 2004. PMID:19635638

  18. Isotopic composition ( 238U/ 235U) of some commonly used uranium reference materials

    NASA Astrophysics Data System (ADS)

    Condon, Daniel J.; McLean, Noah; Noble, Stephen R.; Bowring, Samuel A.

    2010-12-01

    We have determined 238U/ 235U ratios for a suite of commonly used natural (CRM 112a, SRM 950a, and HU-1) and synthetic (IRMM 184 and CRM U500) uranium reference materials by thermal ionisation mass-spectrometry (TIMS) using the IRMM 3636 233U- 236U double spike to accurately correct for mass fractionation. Total uncertainty on the 238U/ 235U determinations is estimated to be <0.02% (2σ). These natural 238U/ 235U values are different from the widely used 'consensus' value (137.88), with each standard having lower 238U/ 235U values by up to 0.08%. The 238U/ 235U ratio determined for CRM U500 and IRMM 184 are within error of their certified values; however, the total uncertainty for CRM U500 is substantially reduced (from 0.1% to 0.02%). These reference materials are commonly used to assess mass-spectrometer performance and accuracy, calibrate isotope tracers employed in U, U-Th and U-Pb isotopic studies, and as a reference for terrestrial and meteoritic 238U/ 235U variations. These new 238U/ 235U values will thus provide greater accuracy and reduced uncertainty for a wide variety of isotopic determinations.

  19. 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.

  20. Fissile Nuclei Rotation Effect in {sup 235}U(n,{gamma}f) Process

    SciTech Connect

    Danilyan, Gevorg; Krakhotin, Vyacheslav; Kuznetsov, Valery; Novitsky, Vadim; Pavlov, Valery; Shatalov, Pavel; Granz, Peter; Mezei, Ferenz; Russina, Margarita; Wilpert, Thomas; Klenke, Jens

    2009-01-28

    A small shift of an angular distribution of prompt {gamma}-rays relative to the fission axis of {sup 236}U* {sup 235}U(n,{gamma}f) process is presented. This effect has been observed in the experiment at BER-II reactor of BENSC/HMI (Berlin). The sign of the shift depends on the direction of the incident neutron beam polarization. This phenomena can be explained by the rotation of fissile nucleus {sup 236}U*, like the effect that has been observed recently at ILL in ternary fission of {sup 235}U by cold polarized neutrons. The main surprise of this result is the detection of scission gamma-rays radiated by a fissile nucleus during the time interval of the order of 10{sup -21} s before or after the moment of the neck rupture. Detailed measurements of trigger {gamma}-rays energy dependence are in progress at the neutron beam 'MEPHISTO' of FRM-II reactor (Garching)

  1. Background reduction in 236U/238U measurements

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  2. 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. PMID:26823129

  3. 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.

  4. Radioisotope dilution analyses of geological samples using 236U and 229Th

    USGS Publications Warehouse

    Rosholt, J.N.

    1984-01-01

    The use of 236U and 229Th in alpha spectrometric measurements has some advantages over the use of other tracers and measurement techniques in isotope dilution analyses of most geological samples. The advantages are: (1) these isotopes do not occur in terrestrial rocks, (2) they have negligible decay losses because of their long half lives, (3) they cause minimal recoil contamination to surface-barrier detectors, (4) they allow for simultaneous determination of the concentration and isotopic composition of uranium and thorium in a variety of sample types, and (5) they allow for simple and constant corrections for spectral inferences, 0.5% of the 238U activity is subtracted for the contribution of 235U in the 236U peak and 1% of the 229Th activity is subtracted from the 230Th activity. Disadvantages in using 236U and 229Th are: (1) individual separates of uranium and thorium must be prepared as very thin sources for alpha spectrometry, (2) good resolution in the spectrometer system is required for thorium isotopic measurements where measurement times may extend to 300 h, and (3) separate calibrations of the 236U and 229Th spike solution with both uranium and thorium standards are required. The use of these tracers in applications of uranium-series disequilibrium studies has simplified the measurements required for the determination of the isotopic composition of uranium and thorium because of the minimal corrections needed for alpha spectral interferences. ?? 1984.

  5. Band structure of 235U

    NASA Astrophysics Data System (ADS)

    Ward, D.; Macchiavelli, A. O.; Clark, R. M.; Cline, D.; Cromaz, M.; Deleplanque, M. A.; Diamond, R. M.; Fallon, P.; Görgen, A.; Hayes, A. B.; Lane, G. J.; Lee, I.-Y.; Nakatsukasa, T.; Schmidt, G.; Stephens, F. S.; Svensson, C. E.; Teng, R.; Vetter, K.; Wu, C. Y.

    2012-12-01

    Over a period of several years we have performed three separate experiments at Lawrence Berkeley National Laboratory's 88-Inch Cyclotron in which 235U (thick target) was Coulomb-excited. The program involved stand-alone experiments with Gammmasphere and with the 8pi Spectrometer using 136Xe beams at 720 MeV, and a CHICO-Gammasphere experiment with a 40Ca beam at 184 MeV. In addition to extending the known negative-parity bands to high spin, we have assigned levels in some seven positive-parity bands which are in some cases (e.g., [631]1/2, [624]7/2, and [622]5/2) strongly populated by E3 excitation. The CHICO data have been analyzed to extract E2 and E3 matrix elements from the observed yields. Additionally, many M1 matrix elements could be extracted from the γ-ray branching ratios. A number of new features have emerged, including the unexpected attenuation of magnetic transitions between states of the same Nilsson multiplet, the breakdown of Coriolis staggering at high spin, and the effect of E3 collectivity on Coriolis interactions.

  6. Rotation of Nuclei as Observed in Ternary Fission of the Reaction 235U(nth,f) Induced by Polarized Neutron

    NASA Astrophysics Data System (ADS)

    Gönnenwein, F.; Gagarski, A.; Guseva, I.; Petrov, G.; Sokolov, V.; Zavarukhkina, T.; Mutterer, M.; Nesvizhevski, V.; Bunakov, V.; Kadmensky, S.

    2007-05-01

    Ternary fission of the standard reaction 235U(nth,f) induced by cold polarized neutrons has been investigated. Fission fragments and light charged particles were recorded in coincidence. Following cold neutron capture the compound nucleus 236U* has spin 3- or 4-. At the saddle point of the fissioning 236U* nucleus these states are collective. They are expected to retain a sizable collectivity down to the scission point. In fact, a collective rotation has been sensed by the shift in the angular distribution of the light charged particles which depends on the orientation of neutron polarization. Direct observation of the rotation of 236U* excited in a cold neutron reaction is reported here for the first time. It is proposed to call the new phenomenon the "ROT-effect".

  7. Identification of a shape isomer in 235U.

    PubMed

    Oberstedt, A; Oberstedt, S; Gawrys, M; Kornilov, N

    2007-07-27

    The shape isomer in 235U has been searched for in a neutron-induced fission experiment on 234U, which was performed at the isomer spectrometer NEPTUNE of the EC-JRC IRMM. A neutron source, with a tunable pulse frequency in the Hz to kHz range and its individually adjustable neutron pulse width in connection with an appropriate detector system turned out to be the ideal instrument to perform an isomer search, when decay half-lives above 100 micros are expected. From the delayed fission events observed for two different NEPTUNE settings and at mean incident neutron energies En=0.95 and 1.27 MeV the isomeric fission half-life could be determined to be T1/2=(3.6+/-1.8) ms. The corresponding cross section was determined to sigmaif=(10+/-8) microb. With these results an experimental confirmation for the existence of a superdeformed shape isomer in odd-uranium isotopes is given for the first time. PMID:17678355

  8. Anthropogenic 236U at Rocky Flats, Ashtabula river harbor, and Mersey estuary: three case studies by sector inductively coupled plasma mass spectrometry.

    PubMed

    Ketterer, M E; Hafer, K M; Link, C L; Royden, C S; Hartsock, W J

    2003-01-01

    236U (t(1/2)=2.3 x 10(7) y) is formed as a result of thermal neutron capture by (235)U. In naturally occurring U ores, where a high neutron flux is present from spontaneous fission of (238)U, (236)U/(238)U atom ratios are approximately 10(-4) ppm. In the natural Earth's crust, unaffected by nuclear fallout, these ratios are expected to be on the order of 10(-8) ppm. Reactor-irradiated U, however, exhibits high (236)U/(238)U atom ratios approaching 10(4) ppm. As a result, the presence of very small quantities of reactor-irradiated U will significantly enhance the "background" (236)U/(238)U atom ratio. When sufficiently elevated (236)U/(238)U ratios are present, the determination of (236)U/(238)U by rapid inductively coupled plasma mass spectrometric (ICPMS) methods is attractive. We have used sector ICPMS at medium resolving power (R=3440) to measure (236)U/(238)U atom ratios with a determination limit of 0.2 ppm. The limiting factors in the measurement are the (235)U(1)H(+) isobar and background signal at m/z 236 arising from the (238)U(+) peak tail. Based upon the analysis of replicates and considerations of possible systematic errors, uncertainties of +/-5% are found for (236)U/(238)U atom ratios of 1-100 ppm. This procedure has been demonstrated in studies of anthropogenic (236)U in the environment at three locations: (a) offsite soils from the vicinity of the Rocky Flats Environmental Technology site (Golden, Colorado, USA); (b) sediments from the Ashtabula River (Ohio, USA); and (c) sediments from the Mersey estuary (Liverpool, UK). In each of these three locations, definite plumes of elevated (236)U/(238)U are identified and characterized. Maximum (236)U/(238)U atom ratios observed in RFETS-vicinity soils, the Ashtabula River, and the Mersey Estuary are 2.8, 140, and 4.4 ppm, respectively. PMID:12691718

  9. Evaluating 238U/235U in U-bearing accessory minerals

    NASA Astrophysics Data System (ADS)

    Hiess, J.; Condon, D. J.; Noble, S. R.; McLean, N.; Bowring, S. A.; Mattinson, J. M.

    2010-12-01

    U-daughter (U-Pb, Pb-Pb, and U-series) geochronology and cosmochronology utilize the absolute value of the present day 238U/235U ratio to calculate and compare dates. For decades, this value has been assumed to be invariant and equal to 137.88, but recent experiments indicate that there is potential for ‘per mil level’ variation in 238U/235U in natural materials, hypothesized to be the result of redox reactions. These studies have largely focused on materials formed in low-temperature environments (e.g. speleothems, corals) and U ore deposits. At present there are no published high-precision high-accuracy 238U/235U data for U-bearing accessory minerals commonly used for U-Pb geochronology. We present accurate and precise 238U/235U determinations for a suite of common U-bearing accessory minerals (zircon, monazite etc.), from a variety of geological environments and ages. Measurements have been made by thermal ionization mass spectrometry, accurately correcting for mass fractionation using the IRMM 3636 233U-236U double spike. Accessory mineral 238U/235U ratios are generally lower than the ‘consensus’ value of 137.88. Systematic discordance has been observed in 238U/206Pb and 235U/207Pb dates obtained for closed-system minerals, and has been used to reassess the relative decay constants of 238U and 235U (Mattinson, 2000, 2010; Schoene et al., 2006). However, these attempts assumed values (i.e., 137.88 or 137.80) for all present-day 238U/235U ratios. Our new determination of coupled 238U/206Pb, 235U/207Pb and 238U/235U measurements on the same closed system zircons, all traceable to SI units, permit further refinement of λ238U/λ235U estimates. Mattinson J.M. 2000. Revising the "gold standard" - the Uranium decay constants of Jaffey et al., 1971. EOS, AGU Fall meeting Supplement Abstract V61A-02. Mattinson J.M. 2010. Analysis of the relative decay constants of 235U and 238U by multi-step CA-TIMS measurements of closed-system natural zircon samples. Chemical

  10. Enrichment Monitor for 235U Fuel Tubes

    SciTech Connect

    Winn, W.G.

    2001-08-22

    This report describes the performance of this prototype y-monitor of 235 Uranium enrichment. In this proposed method y-rates associated with 235U and 232U are correlated with enrichment. Instrumentation for appraising fuel tubes with this method has been assembled and tested.

  11. First 236U data from the Arctic Ocean and use of 236U/238U and 129I/236U as a new dual tracer

    NASA Astrophysics Data System (ADS)

    Casacuberta, N.; Masqué, P.; Henderson, G.; Rutgers van-der-Loeff, M.; Bauch, D.; Vockenhuber, C.; Daraoui, A.; Walther, C.; Synal, H.-A.; Christl, M.

    2016-04-01

    The first dataset of 236U/238U in the water column of the Arctic Ocean (AO) is presented and shows the widest range of ratios reported so far in the open ocean, from (5 ± 5) to (3840 ± 260) ×10-12. Surface samples and depth profiles were collected during two GEOTRACES expeditions in 2011-2012 and analyzed for the concentrations of 236U and 129I, with the aim of investigating whether the combination of 236U/238U and 129I/236U can be used as a new oceanographic tool in the AO. Results show that the distributions of the 236U/238U and 129I/236U atomic ratios are consistent with the different water masses in the AO. High 236U/238U and 129I/236U ratios in the upper water column (> 2000 ×10-12 and >200, respectively) illustrate the penetration of Atlantic waters (AW) into the AO. Lower values were found in Pacific waters (PW) and deep waters of the AO. Rivers seem to represent a temporally and spatially-constrained third anthropogenic source of 236U but more data are needed to confirm this. In a simple mixing model, the combination of 236U/238U and 129I/236U reveals a high contribution (>99%) of natural background waters (pre-nuclear era) in the deep and bottom waters of the Amerasian basin, indicating an apparent water mass renewal time of >1000 years. Despite the relatively high apparent age of the Amerasian Basin deep waters, this work shows the potential of using the dual-tracer approach as a new oceanographic tool in the Arctic Ocean.

  12. 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. PMID:16545893

  13. 238U/235U determinations of some commonly used reference materials and U-bearing accessory minerals (Invited)

    NASA Astrophysics Data System (ADS)

    Condon, D.; Noble, S.; McLean, N.; Bowring, S. A.

    2009-12-01

    We have determined 238U/235U ratios for a suite of commonly used natural (CRM 112a, SRM 950a, HU-1) and synthetic (IRMM 184 and CRM U500) uranium reference materials in addition to several U-bearing accessory phases (zircon and monazite) by thermal ionisation mass-spectrometry (TIMS) using the IRMM 3636 233U-236U double spike to accurately correct for mass fractionation. The 238U/235U values for the natural uranium reference materials differ, by up to 0.1%, from the widely used ‘consensus’ value (137.88) with all having 238U/235U values less than 137.88. Similarly, initial 238U/235U data from zircon and monazite yield 238U/235U values that are lower than the ‘consensus’ value. The data obtained from U-bearing minerals is used to assess how the uncertainty in the 238U/235U ratio contributes to the systematic discordance observed in 238U/206Pb and 235U/207Pb dates (Mattinson, 2000; Schoene et al., 2006) which has traditionally been wholly attributed to error in the U decay constants. The 238U/235U determinations made on the synthetic reference materials yield results that are considerably more precise and accurate than the certified values (0.02% vs. 0.1% for CRM U500). The calibration of isotopic tracers used for U-daughter geochronology that are partially based upon these reference materials, and the resultant age determinations, will benefit from increased accuracy and precision. Mattinson, J.M., 2000. Revising the “gold standard”—the uranium decay constants of Jaffey et al., 1971. Eos Trans. AGU, Spring Meet. Suppl., Abstract V61A-02. Schoene B., Crowley J.L., Condon D.C., Schmitz M.D., Bowring S.A., 2006, Reassessing the uranium decay constants for geochronology using ID-TIMS U-Pb data. Geochimica et Cosmochimica Acta 70: 426-445

  14. Assessment of uranium exposure from total activity and 234U:238U activity ratios in urine.

    PubMed

    Nicholas, T; Bingham, D

    2011-03-01

    Radiation workers at Atomic Weapons Establishment (AWE) are monitored for uranium exposure by routine bioassay sampling (primarily urine sampling). However, the interpretation of uranium in urine and faecal results in terms of occupational intakes is difficult because of the presence of uranium due to intakes from environmental (dietary) sources. For uranium in urine data obtained using current analytical techniques at AWE, the mean, median and standard deviation of excreted uranium concentrations were 0.006, 0.002 and 0.012 μg per g creatinine, respectively. These values are consistent with what might be expected from local dietary intakes and the knowledge that occupational exposures at AWE are likely to be very low. However, some samples do exceed derived investigation levels (DILs), which have been set up taking account of the likely contribution from environmental sources. We investigate how the activity and isotopic composition of uranium in the diet affects the sensitivity of uranium in urine monitoring for occupational exposures. We conclude that DILs based on both total uranium in urine activity and also (234)U:(238)U ratios are useful given the likely variation in dietary contribution for AWE workers. Assuming a background excretion rate and that the enrichment of the likely exposure is known, it is possible to assess exposures using (234)U:(238)U ratios and/or total uranium activity. The health implications of internalised uranium, enriched to <5-8 % by mass (235)U, centre on its nephrotoxicity; the DILs for bioassay samples at AWE are an order of magnitude below the conservative recommendations made by the literature. PMID:21036806

  15. Excess of (236)U in the northwest Mediterranean Sea.

    PubMed

    Chamizo, E; López-Lora, M; Bressac, M; Levy, I; Pham, M K

    2016-09-15

    In this work, we present first (236)U results in the northwestern Mediterranean. (236)U is studied in a seawater column sampled at DYFAMED (Dynamics of Atmospheric Fluxes in the Mediterranean Sea) station (Ligurian Sea, 43°25'N, 07°52'E). The obtained (236)U/(238)U atom ratios in the dissolved phase, ranging from about 2×10(-9) at 100m depth to about 1.5×10(-9) at 2350m depth, indicate that anthropogenic (236)U dominates the whole seawater column. The corresponding deep-water column inventory (12.6ng/m(2) or 32.1×10(12) atoms/m(2)) exceeds by a factor of 2.5 the expected one for global fallout at similar latitudes (5ng/m(2) or 13×10(12) atoms/m(2)), evidencing the influence of local or regional (236)U sources in the western Mediterranean basin. On the other hand, the input of (236)U associated to Saharan dust outbreaks is evaluated. An additional (236)U annual deposition of about 0.2pg/m(2) based on the study of atmospheric particles collected in Monaco during different Saharan dust intrusions is estimated. The obtained results in the corresponding suspended solids collected at DYFAMED station indicate that about 64% of that (236)U stays in solution in seawater. Overall, this source accounts for about 0.1% of the (236)U inventory excess observed at DYFAMED station. The influence of the so-called Chernobyl fallout and the radioactive effluents produced by the different nuclear installations allocated to the Mediterranean basin, might explain the inventory gap, however, further studies are necessary to come to a conclusion about its origin. PMID:27262827

  16. 31 CFR 540.315 - Uranium-235 (U235).

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 31 Money and Finance:Treasury 3 2012-07-01 2012-07-01 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...

  17. 31 CFR 540.315 - Uranium-235 (U235).

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 31 Money and Finance:Treasury 3 2013-07-01 2013-07-01 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...

  18. 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...

  19. 31 CFR 540.315 - Uranium-235 (U235).

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 31 Money and Finance:Treasury 3 2014-07-01 2014-07-01 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...

  20. 31 CFR 540.315 - Uranium-235 (U235).

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 31 Money and Finance:Treasury 3 2011-07-01 2011-07-01 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...

  1. Neutron capture therapy with sup 235 U seeds

    SciTech Connect

    Liu, H.B.; Brugger, R.M.; Shih, J.A. )

    1992-05-01

    A combination of brachytherapy and neutron capture therapy has been evaluated using {sup 235}U metal seeds and external neutron beam irradiation. When thermal neutrons are absorbed by {sup 235}U, high-energy neutrons and gamma rays are produced and some of these deposit energy in surrounding tissue. A Monte Carlo program, using the code MCNP, has been used to evaluate two sizes of {sup 235}U seeds in a water phantom. The results of flux suppression around the seeds and dose distributions are illustrated and discussed. The results show that high doses can be delivered in a relatively short time by using {sup 235}U seeds with neutron capture therapy. This therapy with multiple needles or seeds can be envisioned as a substitute for traditional brachytherapy to give an effective killing dose.

  2. Dynamics of neutron-induced fission of 235U using four-dimensional Langevin equations

    NASA Astrophysics Data System (ADS)

    Pahlavani, M. R.; Mirfathi, S. M.

    2015-08-01

    Background: Langevin equations have been suggested as a key approach to the dynamical analysis of energy dissipation in excited nuclei, formed during heavy-ion fusion-fission reactions. Recently, a few researchers theoretically reported investigations of fission for light nuclei in a low excitation energy using the Langevin approach, without considering the contribution of pre- and post-scission particles and γ -ray emission. Purpose: We study the dynamical evolution of mass distribution of fission fragments, and neutron and γ -ray multiplicity for 236U as compound nuclei that are constructed after fusion of a neutron and 235U. Method: Energy dissipation of the compound nucleus through fission is calculated using the Langevin dynamical approach combined with a Monte Carlo method. Also the shape of the fissioning nucleus is restricted to "funny hills" parametrization. Results: Fission fragment mass distribution, neutron and γ -ray multiplicity, and the average kinetic energy of emitted neutrons and γ rays at a low excitation energy are calculated using a dynamical model, based on the four-dimensional Langevin equations. Conclusions: The theoretical results show reasonable agreement with experimental data and the proposed dynamical model can well explain the energy dissipation in low energy induced fission.

  3. Reaction paths and host phases of uranium isotopes (235U; 238U), Saanich Inlet

    NASA Astrophysics Data System (ADS)

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

    2009-12-01

    In recent times, Uranium has become increasingly the focus of stable isotope fractionation studies. Variations in 238U/235U have been reported as a result of redox reactions [1,2] from the nuclear field shift effect [3], and a mass-dependent, microbially-mediated, kinetic isotope effect [4]. The 238U/235U variability caused by changes in environmental redox conditions leads to an increase in the 238U/235U ratios of the reduced U species sequestered into marine sediments. This points to U isotope variability as a new tool to study ancient ocean redox changes. However, the process by which reduced sediments become enriched in the heavy isotopes of U is not yet known, and hence the utility of 238U/235U as a redox tracer remains to be demonstrated. In order to further constrain sedimentary U enrichment and related isotope effect, we are investigating U isotopic compositions of water samples and fresh surface sediment grab samples over a range of redox conditions in the seasonally anoxic Saanich Inlet, on the east coast of Vancouver Island. U was sequentially extracted from sediments in order to characterize specific fractions for their isotopic composition. The measurements were carried out by MC-ICPMS using 233U/236U-double spike technique. The data are reported as δ238U relative to NBL 112a with a 238U/235U ratio of 137.88 (2sd). External precision is better than 0.10‰ (2sd). Fifteeen analyses of seawater yielded δ238U of -0.42±0.08‰ (2sd). The results for the water samples indicate a homogenous δ238U value throughout the Saanich Inlet water column that matches the global seawater signature. All of the water samples from above and below average -0.42±0.05‰ (2sd). In contrast, a plankton net sample yielded a distinctly different, (about 0.5‰ lighter) isotope value. Bacterial reduction experiments [4] have also shown isotope enrichment factors of about -0.3‰. In addition, metal isotope fractionation occurs during adsorption with the light isotope being

  4. Novel method to study neutron capture of 235U and 238U simultaneously at keV energies.

    PubMed

    Wallner, A; Belgya, T; Bichler, M; Buczak, K; Dillmann, I; Käppeler, F; Lederer, C; Mengoni, A; Quinto, F; Steier, P; Szentmiklosi, L

    2014-05-16

    The neutron capture cross sections of the main uranium isotopes, (235)U and (238)U, were measured simultaneously for keV energies, for the first time by combining activation technique and atom counting of the reaction products using accelerator mass spectrometry. New data, with a precision of 3%-5%, were obtained from mg-sized natural uranium samples for neutron energies with an equivalent Maxwell-Boltzmann distribution of kT ∼ 25 keV and for a broad energy distribution peaking at 426 keV. The cross-section ratio of (235)U(n,γ)/(238)U(n,γ) can be deduced in accelerator mass spectrometry directly from the atom ratio of the reaction products (236)U/(239)U, independent of any fluence normalization. Our results confirm the values at the lower band of existing data. They serve as important anchor points to resolve present discrepancies in nuclear data libraries as well as for the normalization of cross-section data used in the nuclear astrophysics community for s-process studies. PMID:24877933

  5. Observations of 231Pa/ 235U disequilibrium in volcanic rocks

    NASA Astrophysics Data System (ADS)

    Pickett, David A.; Murrell, Michael T.

    1997-04-01

    We present here the first survey of ( 231Pa/ 235U) ratios in volcanic rocks; such measurements are made possible by new mass spectrometric techniques. The data place new constraints on the timing and extent of magma source and evolutionary processes, particularly due to the sensitivity of the 231Pa- 235U pair and its intermediate time scale ( 231Pat 1/2 = 33 ky). ( 231Pa/ 235U) is found to vary widely, from 0.2 in carbonatites to 1.1-2.9 in basalts and 0.9-2.2 in arcs. Substantial Pa enrichment is nearly ubiquitous, suggestive of the relative incompatibility of Pa, qualitatively consistent with available partitioning data. The level of 231Pa- 235U disequilibrium typically far exceeds that of 230Th- 238U and is comparable to 226Ra- 230Th. The high ( 231Pa/ 235U) ratios in MORB and other basalts reflect a large degree of discrimination between two incompatible elements, posing challenges for modelling of melt generation and migration. Fundamental differences in ( 231Pa/ 235U) among different basaltic environments are likely related to contrasts in melting zone conditions (e.g., melting rate). Strong ( 231Pa/ 235U) disequilibria in continental basalts, for which ( 230Th/ 238U) disequilibria are small or absent, demonstrate that Pa-U fractionation is possible in both garnet and spinel mantle stability fields. In arcs, correlation of ( 231Pa/ 235U) and ( 230Th/ 238U) is consistent with U enrichment via slab-derived fluids, a process which is additional to the still dominant Pa enrichment. An important new constraint is provided by the observation that the near-equilibrium ( 230Th/ 238U) common to arcs and continental basalts is not typically accompanied by near-equilibrium ( 231Pa/ 235U), arguing against the influence of long magma history, crustal material, or equilibrium mantle sources in affecting decay-series ratios. Small sample sets from two silicic centers illustrate: (1) recent, rapid U enrichment in the magma chamber (El Chichón); and (2) the failure of

  6. Mass and abundance 236U sensitivities at CIRCE

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

    The actinides (e.g. 236U and xPu isotopes) are present in environmental samples at the ultra trace level since atmospheric tests of NWs (Nuclear Weapons) performed in the past, deliberate dumping of nuclear waste, nuclear fuel reprocessing, on a large scale and operation of NPPs (Nuclear Power Plants) on a small scale have led to the release of a wide range of radioactive nuclides in the environment. Their detection requires the most sensitive AMS (Accelerator Mass Spectrometry) techniques and at the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy, an upgraded actinide AMS system, based on a 3-MV pelletron tandem accelerator, has been operated. In this paper the progress made in order to push the 236U mass sensitivity and 236U/238U isotopic ratio down to the natural levels is reported. A uranium contamination mass of about 0.05 μg and a 236U/238U isotopic ratio sensitivities at the level of 3.2 × 10-13 are presently achievable.

  7. 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.

  8. Cleanup levels for Am-241, Pu-239, U-234, U-235 & U-238 in soils at the Rocky Flats Environmental Technology Site

    SciTech Connect

    Roberts, R.; Colby, B.; Brooks, L.; Slaten, S.

    1997-07-03

    This presentation briefly outlines a cleanup program at a Rocky Flats site through viewgraphs and an executive summary. Exposure pathway analyses to be performed are identified, and decontamination levels are listed for open space and office worker exposure areas. The executive summary very briefly describes the technical approach, RESRAD computer code to be used for analyses, recommendations for exposure levels, and application of action levels to multiple radionuclide contamination. Determination of action levels for surface and subsurface soils, based on radiation doses, is discussed. 1 tab.

  9. Neutron-induced fission cross section of {sup 234}U and {sup 237}Np measured at the CERN Neutron Time-of-Flight (n{sub T}OF) facility

    SciTech Connect

    Paradela, C.; Duran, I.; Tarrio, D.; Alvarez, H.; Tassan-Got, L.; Berthier, B.; Ferrant, L.; Isaev, S.; Le Naour, C.; Stephan, C.; Trubert, D.; David, S.; Abbondanno, U.; Fujii, K.; Milazzo, P. M.; Moreau, C.; Aerts, G.

    2010-09-15

    A high-resolution measurement of the neutron-induced fission cross section of {sup 234}U and {sup 237}Np has been performed at the CERN Neutron Time-of-Flight facility. The cross sections have been determined in a wide energy range from 1 eV to 1 GeV using the evaluated {sup 235}U cross section as reference. In these measurements the energy determination for the {sup 234}U resonances could be improved, whereas previous discrepancies for the {sup 237}Np resonances were confirmed. New cross-section data are provided for high neutron energies that go beyond the limits of prior evaluations, obtaining important differences in the case of {sup 237}Np.

  10. Nuclear excitation by electronic transition of 235U

    NASA Astrophysics Data System (ADS)

    Chodash, P. A.; Burke, J. T.; Norman, E. B.; Wilks, S. C.; Casperson, R. J.; Fisher, S. E.; Holliday, K. S.; Jeffries, J. R.; Wakeling, M. A.

    2016-03-01

    Background: 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. Purpose: An experiment was performed to determine whether NEET of 235U occurs and to determine its excitation rate. Method: A pulsed Nd:YAG laser operating at 1064 nm with a pulse energy of 790 mJ and a pulse width of 9 ns was used to generate a uranium plasma. The plasma was collected on a catcher plate and electrons from the catcher plate were accelerated and focused onto a microchannel plate detector. An observation of a decay with a 26-min half-life would suggest the creation of Um235 and the possibility that NEET of 235U occurred. Results: A 26-min decay consistent with the decay of Um235 was not observed and there was no evidence that NEET occurred. An upper limit for the NEET rate of 235U was determined to be λNEET<1.8 ×10-4 s-1, with a confidence level of 68.3%. Conclusions: The upper limit determined from this experiment is consistent with most of the past measurements. Discrepancies between this experiment and past measurements can be explained by assuming that past experiments misinterpreted the data.

  11. Nuclear excitation by electronic transition of 235U

    DOE PAGESBeta

    Chodash, P. A.; Norman, E. B.; Burke, J. T.; Casperson, R. J.; Fisher, S. E.; Holliday, K. S.; Jeffries, J. R.; Wakeling, M. A.; Wilks, S. C.

    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.

  12. Extreme fractionation of 234U 238U and 230Th 234U in spring waters, sediments, and fossils at the Pomme de Terre Valley, southwestern Missouri

    USGS Publications Warehouse

    Szabo, B. J.

    1982-01-01

    Isotopic fractionation as great as 1600% exists between 234U and 238U in spring waters, sediments, and fossils in the Pomme de Terre Valley, southwestern Missouri. The activity ratios of 234U 238U in five springs range from 7.2 to 16 in water which has been discharged for at least the past 30,000 years. The anomalies in 234U 238U ratio in deep water have potential usefulness in hydrologic investigations in southern Missouri. Clayey units overlying the spring bog sediments of Trolinger Spring are enriched in 230Th relative to their parent 234U by as much as 720%. The results indicate that both preferential displacement via alpha recoil ejection and the preferential emplacement via recoiling and physical entrapment are significant processes that are occurring in the geologic environment. ?? 1982.

  13. 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.

  14. 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.

  15. Precise determination of the open ocean 234U/238U composition

    NASA Astrophysics Data System (ADS)

    Andersen, M. B.; Stirling, C. H.; Zimmermann, B.; Halliday, A. N.

    2010-12-01

    Uranium has a long residence time in the open oceans, and therefore, its salinity-normalized U concentration and 234U/238U activity ratio (expressed herein as δ234U, the ‰ deviation from secular equilibrium) are assumed to be uniform. The marine 234U/238U activity ratio is currently in radioactive disequilibrium and shows a ˜15% excess of 234U with respect to the secular equilibrium value due to continuous input from riverine sources. Knowledge of the marine δ234U, and how it has evolved through the Quaternary, is important for validating age accuracy in the U series dating of marine carbonates, which is increasingly relied upon for providing a chronological basis in paleoclimate research. However, accurate and precise measurements of δ234U are technically difficult. Thus, existing compilations of the open ocean δ234U value vary by up to ˜10‰, and the assumed uniformity in the oceanic δ234U remains to be confirmed. Using MC-ICPMS techniques and a suite of multiple Faraday cups instead of the typical configurations based on a combined Faraday cup-multiplier array, a long-term reproducibility of better than ±0.3‰ (2σ) is achieved for δ234U measurements. Applying these very high precision techniques to open ocean seawater samples, an average δ234U of 146.8 ± 0.1‰ (2σm, n = 19) is obtained. These high-precision seawater measurements yield an external reproducibility of better than ±0.4‰ (2σ) and show that the open oceans have a uniform δ234U on the sub-‰ level. These new data constrain the vertical mixing time of the open oceans to less than 1000 years.

  16. 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. PMID:26555366

  17. Measurement of the (236)U(n,f) cross section from 170 MeV to 2 MeV at the CERN n_TOF Facility

    SciTech Connect

    Sarmento, R.; Goncalves, I. F.; Vaz, P.; Carrapico, C.; Carrillo de Albornoz, A.; Marques, L.; Salgado, J.; Tavora, L.; Calviani, M.; Andriamonje, S.; Chiaveri, E.; Guerrero, C.; Vlachoudis, V.; Colonna, N.; Barbagallo, M.; Marrone, S.; Tagliente, G.; Terlizzi, R.; Belloni, F.; Fuji, K.; Milazzo, P. M.; Moreau, C.; Alvarez-Velarde, F.; Cano-Ott, D.; Gonzalez-Romero, E.; Guerrero, C.; Martinez, T.; Mendoza, E.; Villamarin, D.; Vicente, M. C.; Andrzejewski, Jozef; Karamanis, D.; Marganiec, J.; Assimakopoulos, P. A.; Karadimos, D.; Papachristodoulou, C.; Patronis, N.; Audouin, L.; David, S.; Ferrant, L.; Isaev, S.; Jericha, E.; Leeb, H.; Oberhummer, H.; Pigni, M. T.; Baumann, P.; Kerveno, M.; Lukic, S.; Rudolf, G.; Becvar, F.; Krticka, M.; Calvino, F.; Capote, R.; Frais-Koelbl, H.; Griesmayer, E.; Mengoni, A.; Praena, J.; Capote, R.; Lozano, M.; Quesada, J.; Cennini , P.; Chapel, V.; Ferreira-Marques, R.; Lindote, A.; Lopes, I.; Neves, F.; et al.

    2011-01-01

    The neutron-induced fission cross section of {sup 236}U was measured at the neutron Time-of-Flight (n-TOF) facility at CERN relative to the standard {sup 235}U(n,f) cross section for neutron energies ranging from above thermal to several MeV. The measurement, covering the full range simultaneously, was performed with a fast ionization chamber, taking advantage of the high resolution of the n-TOF spectrometer. The n-TOF results confirm that the first resonance at 5.45 eV is largely overestimated in some nuclear data libraries. The resonance triplet around 1.2 keV was measured with high resolution and resonance parameters were determined with good accuracy. Resonances at high energy have also been observed and characterized and different values for the cross section are provided for the region between 10 keV and the fission threshold. The present work indicates various shortcomings of the current nuclear data libraries in the subthreshold region and provides the basis for an accurate re-evaluation of the {sup 236}U(n,f) cross section, which is of great relevance for the development of emerging or innovative nuclear reactor technologies.

  18. Dipole strength in the {sup 235}U(gamma,gamma{sup '}) reaction up to 2.8 MeV

    SciTech Connect

    Yevetska, O.; Enders, J.; Fritzsche, M.; Neumann-Cosel, P. von; Romig, C.; Savran, D.; Sonnabend, K.; Oberstedt, S.; Richter, A.

    2010-04-15

    Spectra of the {sup 235}U(gamma,gamma{sup '}) reaction were measured at the S-DALINAC at bremsstrahlung end-point energies E{sub 0}=3.5 and 4.4 MeV and scattering angles of 90 deg. and 135 deg. with respect to the beam axis. Discrete transitions are observed at excitation energies below 2.3 MeV only. The deduced cross sections are in rough agreement with the findings of Bertozzi et al. [Phys. Rev. C 78, 041601(R) (2008)] except for the most prominent transition, where the present result is lower by a factor of about 2. Evidence for unresolved dipole strength is found in the spectra by means of a fluctuation analysis, which was carried out up to an excitation energy of 2.8 MeV. If this unresolved strength exhibits the same ratio of E1/M1 cross sections as observed in the even-mass neighbor {sup 236}U, then the energy centroid E{sub x}=2.5(3) MeV and total strength SIGMAB(M1)arrow up=3.6(1.3)mu{sub N}{sup 2} of the M1 part are in good agreement with the systematics of the scissors mode in even-even actinide nuclei.

  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. PMID:23142336

  20. Status of 236U analyses at ETH Zurich and the distribution of 236U and 129I in the North Sea in 2009

    NASA Astrophysics Data System (ADS)

    Christl, Marcus; Casacuberta, Nuria; Lachner, Johannes; Maxeiner, Sascha; Vockenhuber, Christof; Synal, Hans-Arno; Goroncy, Ingo; Herrmann, Jürgen; Daraoui, Abdelouahed; Walther, Clemens; Michel, Rolf

    2015-10-01

    Compact, low energy accelerator mass spectrometry (AMS) has evolved over the past years as one of the most sensitive, selective, and robust techniques for the analysis of heavy and long lived radionuclides. In this study, we will first focus on the analytical capabilities of the compact AMS system TANDY, mainly for 236U analyses, and then present a new dual tracer approach, that combines 129I and 236U. The measured 129I/236U ratios of samples collected in the North Sea in 2009 are in reasonable agreement with the expectations from documented or estimated releases from the two major nuclear reprocessing plants located at Sellafield (GB) and La Hague (F), suggesting that the 129I/236U ratio can be used as a water mass tag in the North Atlantic region. However, our results indicate that, in contrast to 129I, additional contributions of bomb produced 236U cannot be neglected in the North Sea region. This complicates the simple and straight forward use of the 129I/236U ratio as a quantitative tool for the calculation of transport times of North Sea water in the Arctic Ocean.

  1. Measurement of 235U(n,n'γ) and 235U(n,2nγ) reaction cross sections

    NASA Astrophysics Data System (ADS)

    Kerveno, M.; Thiry, J. C.; Bacquias, A.; Borcea, C.; Dessagne, P.; Drohé, J. C.; Goriely, S.; Hilaire, S.; Jericha, E.; Karam, H.; Negret, A.; Pavlik, A.; Plompen, A. J. M.; Romain, P.; Rouki, C.; Rudolf, G.; Stanoiu, M.

    2013-02-01

    The design of generation IV nuclear reactors and the studies of new fuel cycles require knowledge of the cross sections of various nuclear reactions. Our research is focused on (n,xnγ) reactions occurring in these new reactors. The aim is to measure unknown cross sections and to reduce the uncertainty on present data for reactions and isotopes of interest for transmutation or advanced reactors. The present work studies the 235U(n,n'γ) and 235U(n,2nγ) reactions in the fast neutron energy domain (up to 20 MeV). The experiments were performed with the Geel electron linear accelerator GELINA, which delivers a pulsed white neutron beam. The time characteristics enable measuring neutron energies with the time-of-flight (TOF) technique. The neutron induced reactions [in this case inelastic scattering and (n,2n) reactions] are identified by on-line prompt γ spectroscopy with an experimental setup including four high-purity germanium (HPGe) detectors. A fission ionization chamber is used to monitor the incident neutron flux. The experimental setup and analysis methods are presented and the model calculations performed with the TALYS-1.2 code are discussed.

  2. Aspects Of The Coriolis Interaction In 235U

    SciTech Connect

    Ward, D.; Clark, R.M.; Cromaz, M.; Deleplanque, M.A.; Diamond, R.M.; Fallon, P.; Lee, I.Y.; Macchiavelli, A.O.; Stephens, F.S.; Lane, G.J.; Goergen, A.; Svensson, C.E.; Vetter, K.; Cline, D.; Hayes, A.B.; Teng, R.; Wu, C.-Y.; Nakatsukasa, T.

    2005-04-05

    We have performed three separate experiments at LBNL's 88-Inch Cyclotron over a period of several years in which 235U (thick target) was Coulomb-excited. It involved stand-alone experiments with Gammasphere and with the 8PI Spectrometer using 136Xe beams at 720 MeV, and a CHICO-Gammasphere experiment with an 40Ar beam at 180 MeV. In addition to extending the known negative-parity bands to high spin, we have assigned levels in some seven positive-parity bands which are in some cases ( e.g. [631]1/2, [624]7/2 and [622]5/2) strongly populated by E3 excitation. The CHICO data has been analyzed to extract E2 and E3 matrix elements from the observed yields. Additionally, many E1 and M1 matrix elements could be extracted from the {gamma}-ray branching ratios.

  3. 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. PMID:9314233

  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. PMID:23182403

  5. 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.

  6. 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.

  7. 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). PMID:26359847

  8. Toward epsilon levels of measurement precision on 234U/238U by using MC-ICPMS

    NASA Astrophysics Data System (ADS)

    Andersen, M. B.; Stirling, C. H.; Potter, E.-K.; Halliday, A. N.

    2004-10-01

    Variations in 234U/238U have wide-ranging applications as tracers for ground- and river-water fluxes and is an essential component in U-series dating. Analytical developments for measuring 234U/238U have progressed from direct alpha-counting, with precisions at the percent level, to thermal ionization and multiple-collector inductively coupled plasma mass spectrometry (TIMS and MC-ICPMS, respectively) isotopic measurement techniques. However, 234U/238U is difficult to measure with better than permil precision because of the small atomic ratios for most geological samples (~10-4 range). Using a Nu Instruments Nu Plasma MC-ICPMS, we have developed two analytical techniques for the precise measurement of 234U/238U: (1) a conventional standard-bracketing protocol using multiple Faraday cups and electron multipliers with ion counting capabilities (FM) and (2) a standard-bracketing Faraday cup protocol (FF). Both are capable of measuring 234U/238U with precisions at the epsilon level (1 epsilon = 1 part in 104): (1) The conventional standard-bracketing FM measurements are conducted as static measurements with the minor 234U isotope measured in a conventional discrete dynode electron multiplier (SEM) equipped with ion counter and a retardation filter. The Faraday-multiplier gain is measured using bracketing measurements of the U metal standard CRM-145. The external reproducibility of 234U/238U (reformulated into [delta]-notation as [delta]234U), interspersed with frequent measurements of the gain, is at the +/-0.6[per mille sign] level (2[sigma]) for both uraninite and carbonate standards, takes ~75 min and consumes ~120 ng of U per measurement. (2) The static standard-bracketing FF protocol measures all three natural U isotopes in Faraday collectors. This is not usually possible using a standard multiple-Faraday array due to the large differences in the abundances of naturally occurring U isotopes. In our study, this is achieved by replacing the standard 1011 [Omega

  9. Recent measurements of 234U/238U isotope ratio in spring waters from the Hadzici area.

    PubMed

    Vidic, Alfred; Ilić, Zorana; Benedik, Ljudmila

    2013-06-01

    The Hadzici area has become interesting for investigation since depleted uranium ammunition had been employed in 1995 during the NATO air strike campaign in Bosnia and Herzegovina. The purpose of this study is to determine uranium concentration and (234)U/(238)U activity ratio in the spring waters of this area and to investigate their relationship, as well as spatial variations. The spring water samples were taken at 18 sites in total. For the determination of uranium radioisotopes, radiochemical separation procedure followed by alpha-particle spectrometry was applied. Uranium concentration in analyzed waters range from 0.15 to 1.12 μg/L. Spring waters from carbonate based sediments have a lower uranium concentration of between 0.15 and 0.43 μg/L, in comparison to waters sampled within sandstone-based sediments ranging from 0.53 to 1.12 μg/L. Dissolved uranium shows significant spatial variability and correlation with bedrock type confirmed by Principal Component Analysis and Hierarchical Cluster Analysis. The majority of the analyzed waters have a (234)U/(238)U activity ratio ranging from 1.02 to 1.90, of which half of the results range between 1.02 and 1.16. No apparent depleted uranium (DU) contamination was observed, as (234)U/(238)U activity ratio is dependent on geochemical conditions in the environment. Even though the tested spring waters demonstrate significant variability in uranium concentration, (234)U/(238)U activity ratio and (234)U excess, waters with similar uranium isotopic signatures are observable within the region. The guidelines on the spatial redistribution of dissolved uranium (corresponding to (238)U mass concentration), along with (234)U/(238)U activity ratios were provided by the Inverse Distance Weighting (IDW) method. Waters having similar isotopic signature have been delineated. PMID:23410592

  10. Depth profile of 236U/238U in soil samples in La Palma, Canary Islands

    PubMed Central

    Srncik, M.; Steier, P.; Wallner, G.

    2011-01-01

    The vertical distribution of the 236U/238U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the 240Pu/239Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios 236U/238U, 240Pu/239Pu and 236U/239Pu, respectively. The 236U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio 240Pu/239Pu indicated a global fallout signature we assume the same origin as the probable source for 236U. Our measured 236U/239Pu value of around 0.2 is within the expected range for this contamination source. PMID:21481502

  11. A comparison of fallout (236)U and (239)Pu uptake by Australian vegetation.

    PubMed

    Froehlich, M B; Dietze, M M A; Tims, S G; Fifield, L K

    2016-01-01

    The isotopes (236)U and (239)Pu, both produced during nuclear weapons tests carried out in the 1950s and 1960s, are present in the environment and may be used as tracers for soil erosion studies. Although these radionuclides occur only at ultra-trace levels in nature, they can be readily measured by accelerator mass spectrometry with the 14UD heavy ion accelerator at the Australian National University. We have analysed a series of vegetation samples for their (236)U and (239)Pu concentration and compared the results with those found in the surrounding soil. (236)U could be measured in all collected samples whereas (239)Pu could not be detected in several vegetation samples due to its very low concentration, although it was readily detectable in the soil. We find that, relative to plutonium, (236)U is preferentially taken up by plants with enrichment factors ((236)U/(239)Pu)veg/((236)U/(239)Pu)soil that range between 7 and 52 in the present study. PMID:26141188

  12. 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

  13. Occurrence of naturally enriched {sup 235}U: Implications for plutonium behavior in natural environments

    SciTech Connect

    Bros, R.; Gauthier-Lafaye, F.; Stille, P.; Turpin, L.; Holliger, Ph.

    1993-03-01

    It is generally accepted that uranium and most of the fission products, with the exception of the alkalis, alkaline earths and rare gases, remained in the irradiated uranium oxides during the nuclear reactions that took place 2.0 Ga ago in the Oklo uranium deposit (Gabon). New isotope investigations show that clay minerals from argillaceous rocks neighboring the natural fission reactor 10 at Oklo have depleted {sup 235}U with {sup 235}U/{sup 238}U ratios ranging between 0.00560 and the common natural value of 0.00725. One sample, however, is enriched in {sup 235}U with a {sup 235}U/{sup 238}U ratio of 0.007682. Leach experiments of this sample with dilute 1N HCl revealed that the {sup 235}U enrichment is actually restricted to the insoluble residue ({sup 235}U/{sup 238}U = 0.010511), whereas the leachate remains depleted in {sup 235}U. This unique discovery of very enriched uranium, together with samarium, neodymium, rubidium, and strontium isotopic analyses, indicate that a small amount of plutonium could have been more mobile than uranium in the reactor 10, and it is suggested that plutonium was incorporated in the crystallographic structure of clay minerals such as the chlorites. 28 refs., 3 figs., 1 tab.

  14. 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

  15. Chronology of Pu isotopes and 236U in an Arctic ice core.

    PubMed

    Wendel, C C; Oughton, D H; Lind, O C; Skipperud, L; Fifield, L K; Isaksson, E; Tims, S G; Salbu, B

    2013-09-01

    In the present work, state of the art isotopic fingerprinting techniques are applied to an Arctic ice core in order to quantify deposition of U and Pu, and to identify possible tropospheric transport of debris from former Soviet Union test sites Semipalatinsk (Central Asia) and Novaya Zemlya (Arctic Ocean). An ice core chronology of (236)U, (239)Pu, and (240)Pu concentrations, and atom ratios, measured by accelerator mass spectrometry in a 28.6m deep ice core from the Austfonna glacier at Nordaustlandet, Svalbard is presented. The ice core chronology corresponds to the period 1949 to 1999. The main sources of Pu and (236)U contamination in the Arctic were the atmospheric nuclear detonations in the period 1945 to 1980, as global fallout, and tropospheric fallout from the former Soviet Union test sites Novaya Zemlya and Semipalatinsk. Activity concentrations of (239+240)Pu ranged from 0.008 to 0.254 mBq cm(-2) and (236)U from 0.0039 to 0.053 μBq cm(-2). Concentrations varied in concordance with (137)Cs concentrations in the same ice core. In contrast to previous published results, the concentrations of Pu and (236)U were found to be higher at depths corresponding to the pre-moratorium period (1949 to 1959) than to the post-moratorium period (1961 and 1962). The (240)Pu/(239)Pu ratio ranged from 0.15 to 0.19, and (236)U/(239)Pu ranged from 0.18 to 1.4. The Pu atom ratios ranged within the limits of global fallout in the most intensive period of nuclear atmospheric testing (1952 to 1962). To the best knowledge of the authors the present work is the first publication on biogeochemical cycles with respect to (236)U concentrations and (236)U/(239)Pu atom ratios in the Arctic and in ice cores. PMID:23770554

  16. 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).

  17. Feasibility of using 236U to reconstruct close-in fallout deposition from the Hiroshima atomic bomb.

    PubMed

    Sakaguchi, A; Kawai, K; Steier, P; Imanaka, T; Hoshi, M; Endo, S; Zhumadilov, K; Yamamoto, M

    2010-10-15

    The first results on the feasibility of using (236)U to reconstruct the level and spatial distribution of close-in fallout deposition from the Hiroshima A-bomb are reported, coupled with the use of global fallout (137)Cs and (239+240)Pu. The results for global fallout (236)U in soil samples (0-30cm) from Ishikawa prefecture showed that the deposition density of (236)U from the global fallout can be accurately evaluated using AMS. All deposited (236)U, (137)Cs and (239+240)Pu appeared to have been recovered using 30-cm cores. It was also noted from the depth profiles for (236)U/(239+240)Pu and (236)U/(137)Cs ratios that the downward behavior of (236)U in the soil was apparently similar to that of (239+240)Pu, while the (137)Cs was liable to be retained in upper layers compared with (236)U and (239+240)Pu. The accumulated levels were 1.78×10(13)atomsm(-2) for (236)U, 4340Bqm(-2) for (137)Cs and 141Bqm(-2) for (239+240)Pu. The ratios of (236)U/(137)Cs and (236)U/(239+240)Pu were (4.10±0.12)×10(9) and (1.26±0.04)×10(11)atomsBq(-1), respectively. Results of (236)U, (137)Cs and (239+240)Pu measurements for the seven soil cores (0-30cm) from Hiroshima were discussed on the basis of ratios of (236)U/(137)Cs and (236)U/(239+240)Pu by comparing with those from the background area in Ishikawa, indicating that the global fallout dominates the current level of (236)U accumulation in soil in the Black-rain area around Hiroshima after the Hiroshima bomb, and the contribution of the close-in fallout (236)U produced by the Hiroshima A-bomb seems difficult to observe. PMID:20797770

  18. 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

  19. 234U/238U as a ground-water tracer, SW Nevada-SE California

    USGS Publications Warehouse

    Ludwig, K. R.; Peterman, Z.E.; Simmons, K.R.; Gutentag, E.D.

    1993-01-01

    The 234U/238U ratio of uranium in oxidizing ground waters is potentially an excellent ground-water tracer because of its high solubility and insensitivity to chemical reactions. Moreover, recent advances in analytical capability have made possible very precise uranium-isotopic analyses on modest (approx.100 ml) amounts of normal ground water. Preliminary results on waters from SW Nevada/Se California indicate two main mixing trends, but in detail indicate significant complexity requiring three or more main components.

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

    DOE PAGESBeta

    Gaffney, Amy M.; Hubert, Amélie; Kinman, William S.; Magara, Masaaki; Okubo, Ayako; Pointurier, Fabien; Schorzman, Kerri C.; Steiner, Robert E.; Williams, Ross W.

    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.

  1. Investigating Uranium Isotopic Distributions in Environmental Samples Using AMS and MC-ICPMS

    SciTech Connect

    Buchholz, B A; Brown, T A; Hamilton, T F; Hutcheon, I D; Marchetti, A A; Martinelli, R E; Ramon, E C; Tumey, S J; Williams, R W

    2005-12-09

    Major, minor, and trace uranium isotopes were measured at Lawrence Livermore National Laboratory in environmentally acquired samples using different instruments to span large variations in concentrations. Multi-collector inductively-coupled plasma mass spectrometry (MC-ICPMS) can be used to measure major and minor isotopes: {sup 238}U, {sup 235}U, {sup 234}U and {sup 236}U. Accelerator mass spectrometry (AMS) can be used to measure minor and trace isotopes: {sup 234}U, {sup 236}U, and {sup 233}U. The main limit of quantification for minor or trace uranium isotopes is the abundance sensitivity of the measurement technique; i.e., the ability to measure a minor or trace isotope of mass M in the presence of a major isotope at M{+-}1 mass units. The abundance sensitivity for {sup 236}U/{sup 235}U isotope ratio measurements using MC-ICPMS is around {approx}2x10{sup -6}. This compares with a {sup 236}U/{sup 235}U abundance sensitivity of {approx}1x10{sup -7} for the current AMS system, with the expectation of 2-3 orders of magnitude improvement in sensitivity with the addition of another high energy filter. Comparing {sup 236}U/{sup 234}U from MC-ICPMS and AMS produced agreement within {approx}10% for samples at {sup 236}U levels high enough to be measurable by both techniques.

  2. Investigating uranium isotopic distributions in environmental samples using AMS and MC-ICPMS

    NASA Astrophysics Data System (ADS)

    Buchholz, B. A.; Brown, T. A.; Hamilton, T. F.; Hutcheon, I. D.; Marchetti, A. A.; Martinelli, R. E.; Ramon, E. C.; Tumey, S. J.; Williams, R. W.

    2007-06-01

    Major, minor and trace uranium isotopes were measured at Lawrence Livermore National Laboratory in environmentally acquired samples using different instruments to span large variations in concentrations. Multi-collector inductively-coupled plasma mass spectrometry (MC-ICPMS) can be used to measure major and minor isotopes: 238U, 235U, 234U and 236U. Accelerator mass spectrometry (AMS) can be used to measure minor and trace isotopes: 234U, 236U and 233U. The main limit of quantification for minor or trace uranium isotopes is the abundance sensitivity of the measurement technique; i.e. the ability to measure a minor or trace isotope of mass M in the presence of a major isotope at M ± 1 mass units. The abundance sensitivity for 236U/235U isotope ratio measurements using MC-ICPMS is around ∼2 × 10-6. This compares with a 236U/235U abundance sensitivity of ∼1 × 10-7 for the current AMS system, with the expectation of 2-3 orders of magnitude improvement in sensitivity with the addition of another high energy filter. Comparing 236U/234U from MC-ICPMS and AMS produced agreement within ∼10% for samples at 236U levels high enough to be measurable by both techniques.

  3. Fractionation of 238U/235U by reduction during low temperature uranium mineralisation processes

    NASA Astrophysics Data System (ADS)

    Murphy, Melissa J.; Stirling, Claudine H.; Kaltenbach, Angela; Turner, Simon P.; Schaefer, Bruce F.

    2014-02-01

    Investigations of ‘stable’ uranium isotope fractionation during low temperature, redox transformations may provide new insights into the usefulness of the 238U/235U isotope system as a tracer of palaeoredox processes. Sandstone-hosted uranium deposits accumulate at an oxidation/reduction interface within an aquifer from the low temperature reduction of soluble U(VI) complexes in groundwaters, forming insoluble U(IV) minerals. This setting provides an ideal environment in which to investigate the effects of redox transformations on 238U/235U fractionation. Here we present the first coupled measurements of 238U/235U isotopic compositions and U concentrations for groundwaters and mineralised sediment samples from the same redox system in the vicinity of the high-grade Pepegoona sandstone-hosted uranium deposit, Australia. The mineralised sediment samples display extremely variable 238U/235U ratios (herein expressed as δUCRM145238, the per-mil deviation from the international NBL standard CRM145). The majority of mineralised sediment samples have δUCRM145238 values between -1.30±0.05 and 0.55±0.12‰, spanning a ca. 2‰ range. However, one sample has an unusually light isotopic composition of -4.13±0.05‰, which suggests a total range of U isotopic variability of up to ca. 5‰, the largest variation found thus far in a single natural redox system. The 238U/235U isotopic signature of the mineralised sediments becomes progressively heavier (enriched in 238U) along the groundwater flow path. The groundwaters show a greater than 2‰ variation in their 238U/235U ratios, ranging from δUCRM145238 values of -2.39±0.07 to -0.71±0.05‰. The majority of the groundwater data exhibit a clear systematic relationship between 238U/235U isotopic composition and U concentration; samples with the lowest U concentrations have the lowest 238U/235U ratios. The preferential incorporation of 238U during reduction of U(VI) to U(IV) and precipitation of uranium minerals leaves

  4. U-Pb chronology of the Solar System's oldest solids with variable 238U/ 235U

    NASA Astrophysics Data System (ADS)

    Amelin, Yuri; Kaltenbach, Angela; Iizuka, Tsuyoshi; Stirling, Claudine H.; Ireland, Trevor R.; Petaev, Michail; Jacobsen, Stein B.

    2010-12-01

    Accurate determination of the absolute ages of the oldest Solar System objects — chondrules and Ca-Al-rich inclusions (CAIs), requires knowledge of their 238U/ 235U ratios. This ratio was assumed to be invariant in all U-Pb dating of meteorites so far, but the recent discovery of U isotope variations in CAIs (Brennecka et al., 2010a) shows that this assumption is invalid. We present the first combined high-precision U and Pb isotopic data for a CAI, and U isotopic data for chondrules and whole rock fractions of the Allende meteorite. The Pb-Pb isochron age of the CAI SJ101 is 4567.18 ± 0.50 Ma, calculated using the measured 238U/ 235U = 137.876 ± 0.043 (2σ), reported relative to 238U/ 235U = 137.837 of the CRM 145 standard. Our best current estimate of the average terrestrial value is: 238U/ 235U = 137.821 ± 0.014.The error in the age includes uncertainties in the Pb-Pb isochron intercept and in the 238U/ 235U ratio. Allende bulk rock and chondrules have 238U/ 235U = 137.747 ± 0.017 (2σ), distinctly lower than the CAI. The difference in the 238U/ 235U ratio of 0.129 ± 0.046 (2σ) between the CAI and chondrules and bulk meteorite increases the 207Pb- 206Pb age difference by ~ 1.4 Ma, and eliminates apparent disagreement between the CAI-chondrule formation time interval determinations with the U-Pb and extinct nuclide ( 26Al- 26Mg and 182Hf- 182W) data. We discuss standardisation of 238U/ 235U measurements for U-Pb geochronology and cosmochronology, elemental and isotopic fractionation induced by intensive acid leaching, ages of CAIs in the context of 238U/ 235U variability, and possible causes of U isotopic variations in CAIs and meteorites.

  5. Temporal and vertical distributions of anthropogenic 236U in the Japan Sea using a coral core and seawater samples

    NASA Astrophysics Data System (ADS)

    Sakaguchi, Aya; Nomura, Tomoya; Steier, Peter; Gloser, Robin; Sasaki, Keiichi; Watanabe, Tsuyoshi; Nakakuki, Tomoeki; Takahashi, Yoshio; Yamano, Hiroya

    2016-01-01

    The input history of 236U to the surface water of the Japan Sea was reconstructed through measurement of the 236U/238U atom ratio in annual bands of a coral skeleton which was collected at Iki Island in the Tsushima Strait, the main entrance to the Japan Sea. The 236U/238U atom ratios and concentrations of U isotopes were measured for the period 1935-2010 using AMS and ICP-MS. The 236U/238U atom ratios revealed three prominent peaks: 4.51 × 10-9 in 1955, 6.15 × 10-9 in 1959 and 4.14 × 10-9 in 1963; thereafter the isotope ratios gradually decreased over the next several decades, attaining a value of ca.1.3 × 10-9 for the present day. A simplified depth profile model for 236U in the Japan Sea, using the reconstructed 236U value for the surface water together with observed depth profiles for 236U in the water column in 2010, yielded diffusion coefficients of 3.4-5.6 cm2/s for 6 sampling points. The diffusion coefficient values obtained for the northern stations were relatively large, and fitting uncertainty was also larger for stations in the northern region. It may be presumed that the distribution of 236U in the water columns have been influenced not only by diffusion but also by subduction of the surface water in the Japan Sea.

  6. Advances in Multicollector ICPMS for precise and accurate isotope ratio measurements of Uranium isotopes

    NASA Astrophysics Data System (ADS)

    Bouman, C.; Lloyd, N. S.; Schwieters, J.

    2011-12-01

    The accurate and precise determination of uranium isotopes is challenging, because of the large dynamic range posed by the U isotope abundances and the limited available sample material. Various mass spectrometric techniques are used for the measurement of U isotopes, where TIMS is the most accepted and accurate one. Multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) can offer higher productivity compared to TIMS, but is traditionally limited by low efficiency of sample utilisation. This contribution will discuss progress in MC-ICPMS for detecting 234U, 235U, 236U and 238U in various uranium reference materials from IRMM and NBL. The Thermo Scientific NEPTUNE Plus with Jet Interface offers a modified dry plasma ICP interface using a large interface pump combined with a special set of sample and skimmer cones giving ultimate sensitivity for all elements across the mass range. For uranium, an ion yield of > 3 % was reported previously [1]. The NEPTUNE Plus also offers Multi Ion Counting using discrete dynode electron multipliers as well as two high abundance-sensitivity filters to discriminate against peak tailing effects on 234U and 236U originating from the major uranium beams. These improvements in sensitivity and dynamic range allow accurate measurements of 234U, 235U and 236U abundances on very small samples and at low concentration. In our approach, minor U isotopes 234U and 236U were detected on ion counters with high abundance sensitivity filters, whereas 235U and 238U were detected on Faraday Cups using a high gain current amplifier (10e12 Ohm) for 235U. Precisions and accuracies for 234U and 236U were down to ~1%. For 235U, subpermil levels were reached.

  7. European roe deer antlers as an environmental archive for fallout (236)U and (239)Pu.

    PubMed

    Froehlich, M B; Steier, P; Wallner, G; Fifield, L K

    2016-01-01

    Anthropogenic (236)U and (239)Pu were measured in European roe deer antlers hunted between 1955 and 1977 which covers and extends beyond the period of intensive nuclear weapons testing (1954-1962). The antlers were hunting trophies, and hence the hunting area, the year of shooting and the approximate age of each animal is given. Uranium and plutonium are known to deposit in skeletal tissue. Since antler histology is similar to bone, both elements were expected in antlers. Furthermore, roe deer shed their antlers annually, and hence antlers may provide a time-resolved environmental archive for fallout radionuclides. The radiochemical procedure is based on a Pu separation step by anion exchange (Dowex 1 × 8) and a subsequent U purification by extraction chromatography using UTEVA(®). The samples were measured by Accelerator Mass Spectrometry at the VERA facility (University of Vienna). In addition to the (236)U and (239)Pu concentrations, the (240)Pu/(239)Pu isotopic ratios were determined with a mean value of 0.172 ± 0.023 which is in agreement with the ratio of global fallout (∼0.18). Rather high (236)U/(238)U ratios of the order of 10(-6) were observed. These measured ratios, where the (236)U arises only from global fallout, have implications for the use of the (236)U/(238)U ratio as a fingerprint for nuclear accidents or releases from nuclear facilities. Our investigations have shown the potential to use antlers as a temporally resolved archive for the uptake of actinides from the environment. PMID:26119579

  8. Investigation of 234U(n,f) as a Function of Incident Neutron Energy

    NASA Astrophysics Data System (ADS)

    Al-Adili, A.; Hambsch, F.-J.; Oberstedt, S.; Pomp, S.

    2011-10-01

    Measurements of the reaction 234U(n,f) have been performed at incident neutron energies from 0.2 MeV to 5 MeV at the 7 MV Van De Graaf accelerator at IRMM. A twin Frisch-grid ionization chamber was used for fission-fragment detection. Parallel digital and analogue data acquisitions were applied in order to compare the two techniques. First results on the angular anisotropy and preliminary mass distributions are presented along with a first comparison between the two techniques.

  9. Fission decay of the giant quadrupole resonance for /sup 234/U

    SciTech Connect

    Arruda-Neto, J.D.T.; Berman, B.L.; Herdade, S.B.; Nascimento, I.C.

    1981-06-01

    The electrofission cross section for /sup 234/U from 5.5 to 25.4 MeV has been measured. From a combined analysis of it and the previously measured photofission cross section, using virtual-photon spectra calculated in the distorted-wave Born approximation, the E2 photofission cross section has been determined. Parameters of the fission-decay branch of the giant quadrupole resonance for this nucleus have been obtained. A comparison of the E2 and E1 integrated photofission cross sections for the even uranium isotopes shows that the E1 fission channel increases in strength more rapidly with fissility than does the E2 channel.

  10. Experimental Evidence for Hyperdeformed States in U Isotopes

    NASA Astrophysics Data System (ADS)

    Krasznahorkay, A.; Hunyadi, M.; Harakeh, M. N.; Csatlós, M.; Faestermann, T.; Gollwitzer, A.; Graw, G.; Gulyás, J.; Habs, D.; Hertenberger, R.; Maier, H. J.; Máté, Z.; Rudolph, D.; Thirolf, P.; Timár, J.; Valnion, B. D.

    1998-03-01

    Sharp transmission resonances have been observed in the 235U\\(d,pf\\) 236U reaction. The shapes of the resonances as well as the angular distributions of the associated fission fragments are analyzed together with the data obtained previously for 234U. The resonances are interpreted as being hyperdeformed rotational bands with ħ2/2θ = 1.8+0.5-0.7 and 1.6+1.0-0.4 keV and K values of 1, 2, and 4 for 234U and 236U, respectively.

  11. Resource Note on Photofission of Nuclei for {sup 235}U and {sup 239}Pu Detection

    SciTech Connect

    Nieto, Michael Martin

    2004-11-15

    Open-source data exist, in widely scattered places, on photofission of the important nuclear isotopes {sup 235}U and {sup 239}Pu. These data are useful for studies aimed at detecting these materials at ports of entry. An introductory survey is given to access that data.

  12. E2(T = 0) photofission of /sup 236/U and statistical calculations

    SciTech Connect

    Arruda-Neto, J.D.T.

    1988-03-01

    The E2(T = 0) photofission cross section of /sup 236/U was determined at energies near the barrier, by means of both the long-wavelength approximation and recent statistical calculations. The calculated E2(T = 0) cross section was compared with available experimental data from the literature;this indicated that a large E2(T = 0) fission probability is compatible with statistical concepts

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

    USGS Publications Warehouse

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

    1991-01-01

    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 234U/238U 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 234U/238U 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 (??10 ka or better on samples younger than ~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 50-1000 ka coral. -Authors

  14. 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.

  15. Potential sources affecting the activity concentrations of 238U, 235U, 232Th and some decay products in lettuce and wheat samples.

    PubMed

    Jeambrun, M; Pourcelot, L; Mercat, C; Boulet, B; Pelt, E; Chabaux, F; Cagnat, X; Gauthier-Lafaye, F

    2012-11-01

    The activity concentrations of radionuclides within the uranium and thorium series were determined in wheat and lettuce at five sites in France, and in their respective potential sources: crop soils of wheat and crop soils and irrigation waters of lettuce. These data were used to calculate concentration ratios and to enrich the database supported by the technical report series N°472 of the IAEA (2010). For wheat and lettuce, the activity concentrations were in the same range for all radionuclides studied, except for (210)Pb, which had higher activity concentrations in wheat, ranging between 1.3 and 11 Bq kg(−1) (fresh weight) as compared to 0.4 and 0.7 Bq kg(−1) (fresh weight) for lettuce. For wheat, the range of activity concentrations (mBq kg(−1); fresh weight) decreased as (210)Pb > (226)Ra (56–1511) ≈ (228)Ra (86–769) > (228)Th (19–176) ≈ (238)U (11–169) ≈ (234)U (12–150) ≈ (230)Th (9.08–197.18) ≈ (232)Th (8.61–121.45) > (235)U (0.53–7.9). For lettuce, it decreased as (228)Ra (<320–1221) > (210)Pb (409–746) > (226)Ra (30–599) ≈ (228)Th (<29–347) > (238)U (8–120) ≈ (234)U (8–121) ≈ (230)Th (5.21–134.63) ≈ (232)Th (5.25–156.99) > (235)U (0.35–5.63). The species differences may reflect different plant physiologies. Through the study of activity ratios of wheat and lettuce in relation with those of the various radionuclide sources it has been possible to highlight the contribution of the main sources of natural radionuclides. Indeed, irrigation water when the uranium concentration is enhanced (>30 mBq L(−1)) contributed significantly to the activity concentration of uranium in lettuces. Concerning the high activity concentrations of (210)Pb, it could be explained by atmospheric particle deposition. The effect of soil particles resuspension and their adhesion to the plant surface seemed to be important in some cases. The soil-to-plant transfer factors were calculated for lettuce and wheat. The values were

  16. 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

  17. 234U/238U activity ratio disequilibrium technique for studying uranium mobility in the Opalinus Clay at Mont Terri, Switzerland.

    PubMed

    Pekala, M; Kramers, J D; Waber, H N

    2010-06-01

    Mobility of naturally occurring 238U and 234U radionuclides was studied in a low permeability, reducing claystone formation (Opalinus Clay) near its contact with an overlying oxidising aquifer (Dogger Limestones) at Mont Terri, Switzerland. Our data point to a limited redistribution of U in some of the studied samples. Observed centimetre-scale U mobility is explained by slow diffusive transport of 234U in the pore waters of the Opalinus Clay driven by spatially variable in situ supply (by alpha-recoil) of 234U from the rock matrix. Metre-scale mobility is interpreted as a result of infiltration of meteoric water into the overlying aquifer which developed gradients of U concentration across the two rock formations. This triggered a slow in-diffusion of U with (234U/238U)>1 into the Opalinus Clay as attested by a clear-cut pattern of decreasing bulk rock (234U/238U) inwards the Opalinus Clay, away from the Dogger Limestones. PMID:20189405

  18. Bomb fall-out 236U as a global oceanic tracer using an annually resolved coral core

    NASA Astrophysics Data System (ADS)

    Winkler, Stephan R.; Steier, Peter; Carilli, Jessica

    2012-12-01

    Anthropogenic 236U (t½=23.4 My) is an emerging isotopic ocean tracer with interesting oceanographic properties, but only with recent advances in accelerator mass spectrometry techniques is it now possible to detect the levels from global fall-out of nuclear weapons testing across the water column. To make full use of this tracer, an assessment of its input into the ocean over the past decades is required. We captured the bomb-pulse of 236U in an annually resolved coral core record from the Caribbean Sea. We thereby establish a concept which gives 236U great advantage - the presence of reliable, well-resolved chronological archives. This allows studies of not only the present distribution pattern, but gives access to the temporal evolution of 236U in ocean waters over the past decades.

  19. Bomb fall-out (236)U as a global oceanic tracer using an annually resolved coral core.

    PubMed

    Winkler, Stephan R; Steier, Peter; Carilli, Jessica

    2012-12-15

    Anthropogenic (236)U (t ½=23.4 My) is an emerging isotopic ocean tracer with interesting oceanographic properties, but only with recent advances in accelerator mass spectrometry techniques is it now possible to detect the levels from global fall-out of nuclear weapons testing across the water column. To make full use of this tracer, an assessment of its input into the ocean over the past decades is required. We captured the bomb-pulse of (236)U in an annually resolved coral core record from the Caribbean Sea. We thereby establish a concept which gives (236)U great advantage - the presence of reliable, well-resolved chronological archives. This allows studies of not only the present distribution pattern, but gives access to the temporal evolution of (236)U in ocean waters over the past decades. PMID:23564966

  20. Bomb fall-out 236U as a global oceanic tracer using an annually resolved coral core

    PubMed Central

    Winkler, Stephan R.; Steier, Peter; Carilli, Jessica

    2012-01-01

    Anthropogenic 236U (t½=23.4 My) is an emerging isotopic ocean tracer with interesting oceanographic properties, but only with recent advances in accelerator mass spectrometry techniques is it now possible to detect the levels from global fall-out of nuclear weapons testing across the water column. To make full use of this tracer, an assessment of its input into the ocean over the past decades is required. We captured the bomb-pulse of 236U in an annually resolved coral core record from the Caribbean Sea. We thereby establish a concept which gives 236U great advantage – the presence of reliable, well-resolved chronological archives. This allows studies of not only the present distribution pattern, but gives access to the temporal evolution of 236U in ocean waters over the past decades. PMID:23564966

  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. Studies of Neutron-Induced Fission of 235U, 238U, and 239Pu

    NASA Astrophysics Data System (ADS)

    Duke, Dana; TKE Team

    2014-09-01

    A Frisch-gridded ionization chamber and the double energy (2E) analysis method were used to study mass yield distributions and average total kinetic energy (TKE) release from neutron-induced fission of 235U, 238U, and 239Pu. Despite decades of fission research, little or no TKE data exist for high incident neutron energies. Additional average TKE information at incident neutron energies relevant to defense- and energy-related applications will provide a valuable observable for benchmarking simulations. The data can also be used as inputs in theoretical fission models. The Los Alamos Neutron Science Center-Weapons Neutron Research (LANSCE - WNR) provides a neutron beam 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 238U, 235U, and 239Pu will be presented. LA-UR-14-24921.

  4. A new experimental proposal for {sup 235}U PFNS to answer a fifty years old question

    SciTech Connect

    Kornilov, N.; Massey, T.; Grimes, S.; Voinov, A.

    2011-07-01

    The Prompt Fission Neutron Spectrum (PFNS) from {sup 235}U(n,f) is very important for various nuclear applications. It has been investigated in different experiments. In spite of {approx}50 years of experimental efforts, a continuing conflict exists at thermal neutron energy. Microscopic experimental PFNS cannot describe macroscopic data. In this report we discuss the current status of this problem and suggest a new experiment, which could possibly resolve this problem. (authors)

  5. Greenland meltwater impacts on the 234U/238U composition of seawater, the role of subglacial residence time.

    NASA Astrophysics Data System (ADS)

    Arendt, C. A.; Aciego, S.; Sims, K. W. W.; Stevenson, E. I.

    2014-12-01

    The chemical composition of seawater depends on the sources and sinks of the constituent elements, including those derived from continental weathering and transported by rivers. Glacial melt rivers compose a significant percentage of contributing water in the high latitudes, and potentially impact the overall composition of seawater. The magnitude of the chemical changes glacial melt can have on adjacent seawater depends on the composition of glacial melt, which is directly influenced by the subglacial residence time of meltwater. Long residence times correlate to subglacial water with both high cation concentrations and 234U/238U isotopic compositions. Thus, the residence time of subglacial water and corresponding subglacial geochemistry impacts the 234U/238U composition of proximal seawater and potentially global seawater. To test the influence of subglacial water residence times on seawater chemistry we examined the U-series composition of four outlet glaciers directly connected to the Southern Greenland Ice Sheet located near Narsarsuaq, Ilulissat, Nuuk and Kulusuk, and adjacent seawater at each site. All outlet glaciers in this study are located within three of the five primary drainage basins beneath the Greenland Ice Sheet, each in varying stages of subglacial hydrologic evolution, resulting in unique chemical compositions of meltwater draining from each location. At these four locations we found subglacial water residence time values of 10-1000 years. In regions where the U concentration, 234U/238U isotopic composition and residence times were high (1.01 ppb, 1.263 and ~1,000 years in Narsarsuaq) the adjacent seawater 234U/238U composition was elevated (1.152) compared to regions where the U concentration, 234U/238U isotopic composition and residence times were low (0.05 ppb, 1.008 and ~10 years in Illulisat) the adjacent seawater 234U/238U composition remained around the assumed seawater average (1.145). Through this study we observed a direct impact of

  6. Effect of /sup 235/U concentration on fast neutron space and time eigenvalues and eigenfunctions in uranium

    SciTech Connect

    Mohan, R.; Ahmed, F.; Kothari, L.S.

    1985-05-01

    The results of a detailed study of a fast neutron diffusion length and pulsed problem in depleted and enriched subcritical uranium assemblies (0.2 to 4% /sup 235/U) are reported. The multigroup space- and time-dependent equations are solved using the eigenfunction expansion method. The effect of /sup 235/U concentration on space (diffusion length problem) and time (pulsed problem) eigenvalues and eigenfunctions, particularly on the ''discrete'' eigenvalue and eigenfunction, is discussed. The approach to equilibrium (both in space and in time) of fast neutrons changes with changing /sup 235/U concentration.

  7. 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

  8. Use of integral experiments for the assessment of the 235U capture cross section within the CIELO Project

    NASA Astrophysics Data System (ADS)

    Ichou, Raphaelle; Leclaire, Nicolas; Leal, Luiz; Ivanov, Evgeny

    2016-03-01

    A new 235U capture cross-section evaluation, evaluated by ORNL and the CEA Bruyères-le-Châtel (BRC) has been proposed within the CIELO project. IRSN, who participates in the CIELO project, contributes with data testing and has carried out benchmark calculations using few benchmarks, extracted from the ICSBEP database, for testing the new 235U evaluation. The benchmarks have been selected by privileging the experiments showing small experimental uncertainties and a significant sensitivity to 235U capture cross-section. The keff calculations were performed with both the MCNP 6 code and the 5.C.1 release of the MORET 5 code, using the ENDF/B-VII.1 library for all isotopes except 235U, for which both the ENDF/B-VII.1 and the new 235U evaluation was used. The benchmark selection allowed highlighting a significant effect on keff of the new 235U capture cross-section. The results of this data testing, provided as input for the evaluators, are presented here.

  9. Fragment mass and kinetic energy distributions for the photofission of sup 234 U with 12-, 15-, and 20-MeV bremsstrahlung

    SciTech Connect

    Verboven, M.; Jacobs, E.; Piessens, M.; Pomme, S.; De Frenne, D.; De Clercq, A. )

    1990-07-01

    Energy correlation measurements were performed for the photofission of {sup 234}U with bremsstrahlung with endpoint energy 12, 15, and 20 MeV. Overall fragment provisional and postneutron masses, and postneutron and preneutron kinetic energies, are deduced. The behavior of the fragment mass and total kinetic energy with changing {sup 234}U compound nucleus excitation energy is studied.

  10. 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'.

  11. Transition from Asymmetric to Symmetric Fission in the 235U(n,f) Reaction

    SciTech Connect

    Younes, W; Becker, J A; Bernstein, L A; Garrett, P E; McGrath, C A; McNabb, D P; Nelson, R O; Johns, G D; Wilburn, W S; Drake, D M

    2001-07-19

    Prompt {gamma} rays from the neutron-induced fission of {sup 235}U have been studied using the GEANIE spectrometer situated at the LANSCE/WNR ''white'' neutron facility. Gamma-ray production cross sections for 29 ground-state-band transitions in 18 even-even fission fragments were obtained as a function of incident neutron energy, using the time-of-flight technique. Independent yields were deduced from these cross sections and fitted with standard formulations of the fragment charge and mass distributions to study the transition from asymmetric to symmetric fission. The results are interpreted in the context of the disappearance of shell structure at high excitation energies.

  12. Are 0. 1%-accurate gamma-ray assays possible for /sup 235/U solutions

    SciTech Connect

    Parker, J.L.

    1983-01-01

    The factors influencing the accuracy of passive gamma-ray assay of uniform, homogeneous solution samples have been studied in some detail, particularly for the assay of /sup 235/U in uranium solutions. Factors considered are the overall long-term electronic stability, the information losses caused by the rate-related electronic processes of pulse pileup and dead-time, and the self-attenuation of gamma rays within the samples. Both experimental and computational studies indicate that gamma-ray assay procedures for solution samples of moderate size (from approx. 10 to perhaps a few hundred milliliters) are now capable of accuracies approaching 0.1% in many practical cases.

  13. U-234/U-238 ratio: Qualitative estimate of groundwater flow in Rocky Flats monitoring wells

    SciTech Connect

    Laul, J.C.

    1994-02-01

    Groundwater movement through various pathways is the primary mechanism for the transport of radionuclides and trace elements in a water/rock interaction. About three dozen wells, installed in the Rocky Flats Plant (RFP) Solar Evaporation Ponds (SEP) area, are monitored quarterly to evaluate the extent of any lateral and downgradient migration of contaminants from the Solar Evaporation Ponds: 207-A; 207-B North, 207-B Center, and 207-B South; and 207-C. The Solar Ponds are the main source for the various contaminants: radionuclides (U-238, U-234, Pu-239, 240 and Am-241); anions; and trace metals to groundwaters. The U-238 concentrations in Rocky Flats groundwaters vary from <0.2 to 69 pCi/I (IpCi = 3 ug). However, the activity U-234/U-238 ratios are low and range mostly 1.2 to 2.7. The low activity ratios can be interpreted to suggest that the groundwaters are moving slow (

  14. Prompt Fission Neutron Experiments on 235U(n,f) and 252Cf(SF)

    NASA Astrophysics Data System (ADS)

    Göök, A.; Hambsch, F.-J.; Oberstedt, S.; Vidali, M.

    For nuclear modeling and improved evaluation of nuclear data knowledge about fluctuations of the prompt neutron multiplicity as a function of incident neutron energy is requested for the major actinides 235U and 239Pu. Experimental investigations of the prompt fission neutron emission in resonance neutron induced fission on 235U are taking place at the GELINA facility of the IRMM. The experiment employs an array of neutron scintillation-detectors (SCINTIA) in conjunction with a newly designed 3D position sensitive twin Frisch-grid ionization chamber. A preparatory experiment on prompt fission neutron emission in 252Cf(SF) was undertaken to verify analysis procedures relevant for the implementation of the SCINTIA neutron detector array. The available literature data on the TKE dependence of the multiplicity show strong deviations. Therefore, effort was focused on investigating experimental factors in low efficiency neutron counting experiments that may lead to faulty determination of this dependence. Taking these factors into account a result that agree well with data from high efficiency neutron counting experiments is obtained.

  15. 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.

  16. E2 giant resonances and an M1 component in the photofission of /sup 236/U

    SciTech Connect

    Arruda-Neto, J.D.T.; Herdade, S.B.; Berman, B.L.; Nascimento, I.C.

    1980-11-01

    Electrofission and photofission yields and electrofission-fragment angular distributions for /sup 236/U have been measured with fission-track detectors for incident electron energies from 5.5 to 33.0 MeV. Analysis of these data with the use of virtual-photon spectra calculated in distorted-wave Born approximation, combined with the known photofission cross section, results in the simultaneous determination for this nucleus of (a) a giant isoscalar E2 resonance located at 10.8 +- 0.4 MeV, having a width of 6 +- 1 MeV, and exhausting approx.70% of the isoscalar energy-weighted sum rule, and (b) a small M1 component located at 5.8 +- 0.2 MeV whose strength is <2% of that of the giant isoscalar E2 resonance. No evidence is seen for a giant isovector E2 resonance between 22 and 30 MeV.

  17. Fragment Characteristics from Photofission of 234U and 238U Induced by 6.0 - 9.0 Mev Bremsstrahlung

    NASA Astrophysics Data System (ADS)

    Göök, A.; Barday, R.; Chernykh, M.; Eckardt, C.; Enders, J.; Neumann-Cosel, P. Von; Poltoratska, Y.; Wagner, M.; Richter, A.; Oberstedt, S.; Hambsch, F.-J.; Oberstedt, A.

    2011-10-01

    As a preparatory experiment for a search for parity violation in photofission, fission of 238U and 234U induced by 6 - 9 MeV bremsstrahlung has been investigated at the superconducting Darmstadt electron linear accelerator S-DALINAC. Using a twin Frisch grid ionization chamber fission fragment energy and mass distributions have been determined by means of the double kinetic energy technique. The experiment was performed in order to test the ionization chamber's performance in a bremsstrahlung environment. Results on the fission fragment characteristics from the 238U(γ,f) reaction are found to be in good agreement with literature values. In addition results on fission fragment mass and energy distributions from the 234U(γ,f) reaction are presented for the first time in this energy region.

  18. Behavior of isotope (18O/16O, 234U/238U) systems during the formation of uranium deposits of the "sandstone" type

    NASA Astrophysics Data System (ADS)

    Golubev, V. N.; Dubinina, E. O.; Chernyshev, I. V.; Ikonnikova, T. A.

    2016-01-01

    The uneven character of the distribution of 18O/16O and 234U/238U values was established in the vertical cross section of the productive sequence of the Dybryn uranium deposit (Vitim uranium-ore region, Buryatia). Both a deficiency and an excess of 234U in relation to the equilibrium 234U/238U ratio in the vertical sequence may provide evidence for the extremely low rate of the infiltration water flow. The behavior of oxygen isotope characteristics for different size fractions of terrigenous rocks provides evidence for active uranium redistribution and openness of the isotope system of this element during interaction of terrigenous-sedimentary rocks with infiltration waters.

  19. 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

  20. On the Search for Nuclear Resonance Fluorescence Signatures of 235U and 238U above 3 MeV

    SciTech Connect

    Warren, Glen A.; Caggiano, Joseph A.; Bertozzi, William; Korbly, Steve; Ledoux, Robert; Park, William H.

    2010-02-01

    Nuclear resonance fluorescence is a physical process that provides an isotope-specific signature that could be used for the identification and characterization of materials. The technique involves the detection of prompt discrete-energy photons emitted from a sample that is exposed to MeV-energy photons. Potential applications of the technique range from detection of high explosives to characterization of special nuclear materials such as 235U. Pacific Northwest National Laboratory and Passport Systems have collaborated to conduct a pair of measurements to search for a nuclear resonance fluorescence response of 235U above 3 MeV and of 238U above 5 MeV using an 8 g sample of highly enriched uranium and a 90 g sample of depleted uranium. No new signatures were observed. The minimum detectable integrated cross section for 235U is presented.

  1. Investigating Prompt Fission Neutron Emission from 235U(n,f) in the Resolved Resonance Region

    NASA Astrophysics Data System (ADS)

    Göök, Alf; Hambsch, Franz-Josef; Oberstedt, Stephan

    2016-03-01

    Investigations of prompt emission in fission is of importance in understanding the fission process in general and the sharing of excitation energy among the fission fragments in particular. Experimental activities at IRMM on prompt neutron emission from fission in response to OECD/NEA nuclear data requests is presented in this contribution. Main focus lies on currently on-going investigations of prompt neutron emission from the reaction 235U(n,f) in the region of the resolved resonances. For this reaction strong fluctuations of fission fragment mass distributions and mean total kinetic energy have been observed [Nucl. Phys. A 491, 56 (1989)] as a function of incident neutron energy in the resonance region. In addition fluctuations of prompt neutron multiplicities were also observed [Phys. Rev. C 13, 195 (1976)]. The goal of the present study is to verify the current knowledge of prompt neutron multiplicity fluctuations and to study correlations with fission fragment properties.

  2. 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.

  3. High-Resolution Correlated Fission Product Measurements of 235U (nth , f) with SPIDER

    NASA Astrophysics Data System (ADS)

    Shields, Dan; Spider Team

    2015-10-01

    The SPIDER detector (SPectrometer for Ion DEtermination in fission Research) has obtained high-resolution, moderate-efficiency, correlated fission product data needed for many applications including the modeling of next generation nuclear reactors, stockpile stewardship, and the fundamental understanding of the fission process. SPIDER simultaneously measures velocity and energy of both fission products to calculate fission product yields (FPYs), neutron multiplicity (ν), and total kinetic energy (TKE). These data will be some of the first of their kind available to nuclear data evaluations. An overview of the SPIDER detector, analytical method, and preliminary results for 235U (nth , f) will be presented. LA-UR-15-20130 This work benefited from the use of the LANSCE accelerator facility and was performed under the auspices of the US Department of Energy by Los Alamos Security, LLC under Contract DE-AC52-06NA25396.

  4. Measurements of γ-ray Energy and Multiplicity from 235U(nthermal) using STEFF

    NASA Astrophysics Data System (ADS)

    Pollitt, A. J.; Smith, A. G.; Tsekhanovich, I.; Dare, J. A.; Murray, L.

    2015-05-01

    The amount of energy carried by γ-rays during the fission process is an important consideration when developing new reactor designs. Many studies of γ-ray energy and multiplicity, from a multitude of fissioning systems, were measured during the 1970s. However the data from such experiments largely underestimates the heating effect caused by γ-rays in the structure of a reactor. It is therefore essential to obtain more accurate measurements of the energy carried during γ-ray emission. As such, the OECD Nuclear Energy Agency has put out a high priority request [1] for measurements of the mean γ-ray energy and multiplicity to an accuracy better than 7.5 percent from several fissioning systems; including 235U(nthermal). Measurements of the rays from these fissioning nuclei were performed with the SpecTrometer for Exotic Fission Fagments (STEFF).

  5. High Precision Measurements of 235U/238U Isotopic Fractionations Resulting From Uranium Reduction Induced by Zero Valent Iron

    NASA Astrophysics Data System (ADS)

    Rademacher, L.; Lundstrom, C.; Johnson, T.

    2003-12-01

    Uranium is a widespread natural and anthropogenic contaminant in surface and subsurface waters. Like several other inorganic contaminants, uranium is mobile under oxidizing conditions but may be immobilized by chemical reduction. U(VI) moves with groundwater as (UO2)2+ and as soluble complexes with carbonate, phosphate, and fluoride. In many groundwater systems, uranium undergoes chemical reduction to U(IV), which is insoluble and immobile. Therefore, understanding the extent of reduction is essential for predicting the mobility of uranium in groundwater. Mass dependent isotopic fractionations of redox sensitive contaminants frequently found in groundwater (including chromate, selenate, and nitrate) have proven exceptionally useful for estimating the rate and extent of reduction and immobilization. Until recently, however, analytical limitations have prevented these techniques from being applied to heavier redox sensitive elements, such as uranium. The advent of highly sensitive multi-collector inductively coupled plasma mass spectrometers (MC-ICP-MS) enables high precision measurements of previously undetected variations in many elements. Laboratory reduction experiments with zero valent iron (ZVI) were performed in a controlled environment to test the hypothesis that uranium isotopes, specifically 235U/238U, behave similarly to other redox sensitive contaminants and produce a mass dependent fractionation during the transformation between valence states. Because of the large abundance differences between 235U and 238U, initial experiments used U500, an enriched uranium standard with approximately equal parts 235U and 238U. Results suggest that the highly sensitive MC-ICP-MS distinguishes 235U/238Uvariations to approximately + 0.02per mil. Measured isotopic fractionations between the 235U/238U of the initial and final experimental solutions (~70% reduced) are approximately 1.1 per mil, and increase with decreasing concentration. Measured variations in 235U/238U

  6. 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.

  7. 238U/235U variations in meteorites: extant 247Cm and implications for Pb-Pb dating.

    PubMed

    Brennecka, G A; Weyer, S; Wadhwa, M; Janney, P E; Zipfel, J; Anbar, A D

    2010-01-22

    The 238U/235U isotope ratio has long been considered invariant in meteoritic materials (equal to 137.88). This assumption is a cornerstone of the high-precision lead-lead dates that define the absolute age of the solar system. Calcium-aluminum-rich inclusions (CAIs) of the Allende meteorite display variable 238U/235U ratios, ranging between 137.409 +/- 0.039 and 137.885 +/- 0.009. This range implies substantial uncertainties in the ages that were previously determined by lead-lead dating of CAIs, which may be overestimated by several million years. The correlation of uranium isotope ratios with proxies for curium/uranium (that is, thorium/uranium and neodymium/uranium) provides strong evidence that the observed variations of 238U/235U in CAIs were produced by the decay of extant curium-247 to uranium-235 in the early solar system, with an initial 247Cm/235U ratio of approximately 1.1 x 10(-4) to 2.4 x 10(-4). PMID:20044543

  8. 238U/235U Variations in Meteorites: Extant 247Cm and Implications for Pb-Pb Dating

    NASA Astrophysics Data System (ADS)

    Brennecka, G. A.; Weyer, S.; Wadhwa, M.; Janney, P. E.; Zipfel, J.; Anbar, A. D.

    2010-01-01

    The 238U/235U isotope ratio has long been considered invariant in meteoritic materials (equal to 137.88). This assumption is a cornerstone of the high-precision lead-lead dates that define the absolute age of the solar system. Calcium-aluminum-rich inclusions (CAIs) of the Allende meteorite display variable 238U/235U ratios, ranging between 137.409 ± 0.039 and 137.885 ± 0.009. This range implies substantial uncertainties in the ages that were previously determined by lead-lead dating of CAIs, which may be overestimated by several million years. The correlation of uranium isotope ratios with proxies for curium/uranium (that is, thorium/uranium and neodymium/uranium) provides strong evidence that the observed variations of 238U/235U in CAIs were produced by the decay of extant curium-247 to uranium-235 in the early solar system, with an initial 247Cm/235U ratio of approximately 1.1 × 10-4 to 2.4 × 10-4.

  9. Angular correlations in emission of prescission neutrons from {sup 235}U fission induced by slow polarized neutrons

    SciTech Connect

    Danilyan, G. V.; Wilpert, T.; Granz, P.; Krakhotin, V. A.; Mezei, F.; Novitsky, V. V.; Pavlov, V. S.; Russina, M. V.; Shatalov, P. B.

    2008-12-15

    A new approach to searching for and studying scission neutrons, which is based on the analysis of specific angular correlations in nuclear fission induced by polarized neutrons, is described and used to evaluate the fraction of scission neutrons in the total number of prompt neutrons of {sup 235}U fission emitted perpendicularly to the fission axis.

  10. He stripping for AMS of 236U and other actinides using a 3 MV tandem accelerator

    NASA Astrophysics Data System (ADS)

    Winkler, Stephan R.; Steier, Peter; Buchriegler, Josef; Lachner, Johannes; Pitters, Johanna; Priller, Alfred; Golser, Robin

    2015-10-01

    Interest in the long-lived radioisotope 236U (t1/2 = 23.4 million years) has significantly increased recently, due to the emergence of environmental and earth science applications. Presently, only a few (AMS) accelerator mass spectrometry instruments are suited for this measurement. One major limitation is the relatively low total detection efficiency (on the order of 10-4), which is partly caused by a low stripping yield of the positive ion charge state selected after the tandem accelerator. It has been shown that high yield can be achieved using helium as stripper gas for uranium ion energies below 0.35 MeV. Here we investigate the potential of He stripping of U at the 3-MV tandem accelerator VERA. Phenomenological charge state distributions for U and Th are presented for terminal voltages from 1.0 to 1.7 MV. These terminal voltages provide better background rejection than possible below 1 MeV, and are suited to the widely used 1-3 MV workhorses of many accelerator mass spectrometry laboratories. The methods can be applied to other actinides also.

  11. 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.

  12. 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

  13. Sequential injection method for rapid and simultaneous determination of 236U, 237Np, and Pu isotopes in seawater.

    PubMed

    Qiao, Jixin; Hou, Xiaolin; Steier, Peter; Golser, Robin

    2013-11-19

    An automated analytical method implemented in a novel dual-column tandem sequential injection (SI) system was developed for simultaneous determination of (236)U, (237)Np, (239)Pu, and (240)Pu in seawater samples. A combination of TEVA and UTEVA extraction chromatography was exploited to separate and purify target analytes, whereupon plutonium and neptunium were simultaneously isolated and purified on TEVA, while uranium was collected on UTEVA. The separation behavior of U, Np, and Pu on TEVA-UTEVA columns was investigated in detail in order to achieve high chemical yields and complete purification for the radionuclides of interest. (242)Pu was used as a chemical yield tracer for both plutonium and neptunium. (238)U was quantified in the sample before the separation for deducing the (236)U concentration from the measured (236)U/(238)U atomic ratio in the separated uranium target using accelerator mass spectrometry. Plutonium isotopes and (237)Np were measured using inductively coupled plasma mass spectrometry after separation. The analytical results indicate that the developed method is robust and efficient, providing satisfactory chemical yields (70-100%) of target analytes and relatively short analytical time (8 h/sample). PMID:24134480

  14. (236)U and (239,)(240)Pu ratios from soils around an Australian nuclear weapons test site.

    PubMed

    Tims, S G; Froehlich, M B; Fifield, L K; Wallner, A; De Cesare, M

    2016-01-01

    The isotopes (236)U, (239)Pu and (240)Pu are present in surface soils as a result of global fallout from nuclear weapons tests carried out in the 1950's and 1960's. These isotopes potentially constitute artificial tracers of recent soil erosion and sediment movement. Only Accelerator Mass Spectrometry has the requisite sensitivity to measure all three isotopes at these environmental levels. Coupled with its relatively high throughput capabilities, this makes it feasible to conduct studies of erosion across the geographical extent of the Australian continent. In the Australian context, however, global fallout is not the only source of these isotopes. As part of its weapons development program the United Kingdom carried out a series of atmospheric and surface nuclear weapons tests at Maralinga, South Australia in 1956 and 1957. The tests have made a significant contribution to the Pu isotopic abundances present in the region around Maralinga and out to distances ∼1000 km, and impact on the assessment techniques used in the soil and sediment tracer studies. Quantification of the relative fallout contribution derived from detonations at Maralinga is complicated owing to significant contamination around the test site from numerous nuclear weapons safety trials that were also carried out around the site. We show that (236)U can provide new information on the component of the fallout that is derived from the local nuclear weapons tests, and highlight the potential of (236)U as a new fallout tracer. PMID:26141189

  15. 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)

  16. 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.

  17. Mass spectrometric sup 230 Th- sup 234 U- sup 238 U dating of the Devils Hole calcite vein

    SciTech Connect

    Ludwig, K.R.; Simmons, K.R.; Szabo, B.J.; Riggs, A.C. ); Winograd, I.J.; Landwehr, J.M. ); Hoffman, R.J. )

    1992-10-09

    The Devils Hole calcite vein contains a long-term climatic record, but requires accurate chronologic control for its interpretation. Mass-spectrometric U-series ages for samples from core DH-11 yielding {sup 230}Th ages with precisions ranging from less than 1,000 years (2{sigma}) for samples younger than {approximately}140 ka (thousands of years ago) to less than 50,000 years for the oldest samples ({approximately}566 ka). The {sup 234}U/{sup 238}U ages could be determined to a precision of {approximately}20,000 years for all ages. Calcite accumulated continuously from 566 ka until {approximately}60 ka at an average rate of 0.7 millimeter per 10{sup 3} years. The precise agreement between replicate analyses and the concordance of the {sup 230}Th/{sup 238}U and {sup 234}U/{sup 238}U ages for the oldest samples indicate that the DH-11 samples were closed systems and validate the dating technique in general.

  18. 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.

  19. 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.

  20. 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

  1. Certification of a new series of gravimetrically prepared synthetic reference materials for n( 236U)/ n( 238U) isotope ratio measurements

    NASA Astrophysics Data System (ADS)

    Richter, Stephan; Alonso, Adolfo; Aregbe, Yetunde; Eykens, Roger; Jacobsson, Ulf; Kehoe, Frances; Kuehn, Heinz; Verbruggen, Andre; Wellum, Roger

    2010-04-01

    A new series of gravimetrically prepared synthetic isotope reference materials, the so-called IRMM-075 series, with n( 236U)/ n( 238U) isotope ratios varying from 10 -4 to 10 -9 has been prepared and certified. This series is suited for calibration of n( 236U)/ n( 238U) measurements made by various mass spectrometric techniques such as TIMS (Thermal Ionization Mass Spectrometry), ICPMS (Inductively Coupled Plasma Mass Spectrometry), AMS (Accelerator Mass Spectrometry) and RIMS (Resonance Ionization Mass Spectrometry). Natural uranium with low 236U isotope abundance and highly enriched 236U were both purified using well proven chemical methodology. The oxides were calcined into U 3O 8 in an oven installed in a glove-box with controlled humidity. Primary solutions of the same concentration were prepared by dissolving the oxides of 236U and natural U. From the 236U solution a series of four dilutions was made by weighing. Weighed amounts of the dilutions of 236U and weighed amounts of natural U were mixed to form a set of n( 236U)/ n( 238U) mixtures at a concentration of 1 mg U g -1. Verification of the mixtures IRMM-075/1-6 was performed by TIMS measurements using Faraday collectors and a secondary electron multiplier in combination with an energy filter for improved abundance sensitivity. The results agreed well with the certified values obtained from the gravimetrical mixing calculations. The uncertainties of the calculated isotopic ratios are significantly lower compared to typical uncertainties from mass spectrometric techniques such as TIMS and ICPMS and in particular to AMS and RIMS. The methods for the preparation and mixing of the IRMM-075/1-6 series are described and the certification and verification procedures are reported.

  2. Review of PGDP assessment of criticality safety problems in increasing product assay to 5 wt % /sup 235/U

    SciTech Connect

    Petrie, L.M.; Turner, J.C.; Stewart, G.B.

    1985-02-01

    Paducah Gaseous Diffusion Plant (PGDP) performed an evaluation of the PGDP facilities to determine the feasibility of increasing product assay from 2.0 wt % to 5.0 wt % /sup 235/U and to determine the impact of this increase on plant criticality safety; their conclusions are reported in KY-710. This report critiques the methods used and conclusions reached in KY-710. 4 figures, 5 tables.

  3. Investigation of the effects of nuclear level density parameters on the cross sections for the 234U(γ,f) reaction

    NASA Astrophysics Data System (ADS)

    Pekdogan, Hakan; Aydin, Abdullah; Hakki Sarpun, Ismail

    2015-07-01

    In this study, we have investigated the effects of nuclear level density parameters on the cross sections for the 234U(γ,f) reaction up to 20 MeV. The cross sections on 234U(γ,f) reaction were calculated for different level density models using the TALYS 1.6 code. First, it was determined the level density model that was the closest to the experimental data. Secondly, cross sections obtained for different level density parameters of this model were compared with experimental data from the EXFOR database. Thus it was determined the best level density parameter fit to experimental data.

  4. 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.

  5. R-matrix analysis of the 236U(n,γ) reaction in the resolved resonance energy region

    NASA Astrophysics Data System (ADS)

    Mezentseva, Zh.; Berthoumieux, E.; Borella, A.; Cennini, P.; Furman, W.; Goverdovski, A.; Gunsing, F.; Mengoni, A.; Schillebeeckx, P.; Wynants, R.

    2009-01-01

    The neutron capture cross section of 236U was measured in the neutron energy range from 1 eV to 10 keV by the neutron time-of-flight method at the GELINA white pulsed neutron source of the Institute for Reference Materials and Measurements (IRMM) in Geel (Belgium). The gamma rays originating from neutron capture events were detected by two C6D6-based liquid scintillators using the pulse height weighting technique. The weighting function has been derived from Monte-Carlo simulations of the detector response to monoenergetic gamma rays. The sample under investigation with a total amount of 338 mg of 236U was located in the neutron beam at a distance of 28.6 m from the source. The shape of the neutron flux was determined by a 10B neutron counter, placed approximately 60 cm upstream in the neutron beam line. The neutron capture yield in the resolved resonance region up to 1 keV has been derived from time-of-flight spectra.

  6. R-matrix analysis of the {sup 236}U(n,{gamma}) reaction in the resolved resonance energy region

    SciTech Connect

    Mezentseva, Zh.; Berthoumieux, E.; Gunsing, F.; Cennini, P.; Furman, W.; Goverdovski, A.; Mengoni, A.

    2009-01-28

    The neutron capture cross section of {sup 236}U was measured in the neutron energy range from 1 eV to 10 keV by the neutron time-of-flight method at the GELINA white pulsed neutron source of the Institute for Reference Materials and Measurements (IRMM) in Geel (Belgium). The gamma rays originating from neutron capture events were detected by two C{sub 6}D{sub 6}-based liquid scintillators using the pulse height weighting technique. The weighting function has been derived from Monte-Carlo simulations of the detector response to monoenergetic gamma rays.The sample under investigation with a total amount of 338 mg of {sup 236}U was located in the neutron beam at a distance of 28.6 m from the source. The shape of the neutron flux was determined by a {sup 10}B neutron counter, placed approximately 60 cm upstream in the neutron beam line.The neutron capture yield in the resolved resonance region up to 1 keV has been derived from time-of-flight spectra.

  7. Explaining discrepant depth profiles of {sup 234}U/{sup 238}U and {sup 230}Th{sub exc} in Mn-crusts

    SciTech Connect

    Neff, U.; Bollhoefer, A.; Frank, N.; Mangini, A.

    1999-08-01

    Manganese encrustations are an important archive for the reconstruction of deep ocean circulation in the past. However, because of discordant growth rates derived from the decrease of the activity ratios of {sup 234}U/{sup 238}U and of {sup 230}Th{sub exc} with depth, their dating via the measurement of depth profiles of {sup 230}Th and {sup 231}Pa has been recently put into question (Chabaux et al., 1997). In this study the authors present high precision depth profiles of uranium and thorium isotopes (TIMS) of a hydrogenous Mn-crust from the South China Sea. Indeed, the depth profiles of {sup 234}U/{sup 238}U and {sup 238}Th{sub exc} deliver very different growth rates of 8.80 {+-} 1.20 and 2.64 {+-} 0.12 mm/Ma, respectively. The authors solve this discrepancy with a simple model which assumes exchange of uranium adsorbed in the Mn-crust with uranium dissolved in the pore water. The best agreement to the data is obtained applying an exchange coefficient of 5 {times} 10{sup {minus}6} [a{sup {minus}1}]. Application of this model to the data set of Chabaux et al. (1997), reproduces very well their profiles of the {delta}{sup 234}U. The authors conclude that {sup 234}U/{sup 238}U dating of Mn-encrustations is not reliable because of open-system conditions for uranium.

  8. 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.

  9. 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.

  10. 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.

  11. 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.

  12. Yield and cross section of {sup 232}Th and {sup 236}U fission induced by {gamma} quanta with energies up to 11 MeV

    SciTech Connect

    Soldatov, A.S.; Smirenkin, G.N.

    1995-02-01

    The results of relative measurements of photofission yields are presented for {sup 232}Th and {sup 236}U nuclei in the region 7-11 MeV of end-point bremsstrahlung energies. The cross section and yield of {sup 238}U photofission is taken as the standard. The photofission cross sections for the {sup 232}Th and {sup 236}U nuclei are reconstructed from these data. The experimental data processing is refined, and the information obtained is revised. This paper is a continuation of the earlier publication. 21 refs., 5 figs.

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

    DOE PAGESBeta

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

    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

  14. 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.

  15. 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.

  16. Measurements of the /sup 235/U(n,f) standard cross section at the National Bureau of Standards

    SciTech Connect

    Johnson, R.G.; Carlson, A.D.; Wasson, O.A.; Duvall, K.C.; Behrens, J.W.; Meier, M.M.; Patrick, B.D.; Dias, M.S.

    1988-01-01

    The primary mission of the Neutron Interactions and Dosimetry Group at the National Bureau of Standards (NBS) is the measurement of the standard neutron cross sections. The group has had a long-term program for the measurement of one of the most important of these cross sections---the neutron-induced fission cross section of /sup 235/U. Since the ENDF/B-VI evaluation has been recently released, it is appropriate to review the measurements of the /sup 235/U(n,f) cross section which have been made at the NBS using accelerator-based neutron sources. In the 0.1--20 MeV region where this cross section is a standard, six separate measurements of the differential cross section, using a variety of techniques have been made. Both the NBS 150-MeV Electron Linac and the 3-MV Positive Ion Accelerator have been used as neutron sources. Two of the measurements are relative to the H(n,p) cross section while the remainder are absolute. These measurements will be reviewed and compared to ENDF/B-VI. The current status of this program and possible future improvements will be discussed. 11 refs., 3 figs., 1 tab.

  17. Fission Product Yields for 14 MeV Neutrons on 235U, 238U and 239Pu

    NASA Astrophysics Data System (ADS)

    Mac Innes, M.; Chadwick, M. B.; Kawano, T.

    2011-12-01

    We report cumulative fission product yields (FPY) measured at Los Alamos for 14 MeV neutrons on 235U, 238U and 239Pu. The results are from historical measurements made in the 1950s-1970s, not previously available in the peer reviewed literature, although an early version of the data was reported in the Ford and Norris review. The results are compared with other measurements and with the ENDF/B-VI England and Rider evaluation. Compared to the Laurec (CEA) data and to ENDF/B-VI evaluation, good agreement is seen for 235U and 238U, but our FPYs are generally higher for 239Pu. The reason for the higher plutonium FPYs compared to earlier Los Alamos assessments reported by Ford and Norris is that we update the measured values to use modern nuclear data, and in particular the 14 MeV 239Pu fission cross section is now known to be 15-20% lower than the value assumed in the 1950s, and therefore our assessed number of fissions in the plutonium sample is correspondingly lower. Our results are in excellent agreement with absolute FPY measurements by Nethaway (1971), although Nethaway later renormalized his data down by 9% having hypothesized that he had a normalization error. The new ENDF/B-VII.1 14 MeV FPY evaluation is in good agreement with our data.

  18. 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.

  19. A GENERALIZED METHOD FOR CHARACTERIZATION OF 235U AND 239PU CONTENT USING SHORT-LIVED FISSION PRODUCT GAMMA SPECTROSCOPY

    SciTech Connect

    Knowles, Justin R; Skutnik, Steven E; Glasgow, David C; Kapsimalis, Roger J

    2016-01-01

    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, 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. 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.

  20. Uranium half-lives: a critical review

    SciTech Connect

    Holden, N.E.

    1981-01-01

    The experimental data are evaluated and values for the spontaneous fission half-life of /sup 238/U and the total half-lives for /sup 232/U, /sup 233/U, /sup 234/U, /sup 235/U, /sup 236/U, and /sup 238/U are recommended. Also the variation of the isotopic abundance of /sup 234/U in nature and the error involved in the assumption of secular equilibrium between /sup 234/U and /sup 238/U in the determination of the specific activity of natural uranium samples are discussed. The recommended half-life values and 95% confidence limits are: /sup 238/U spontaneous fission: 8.09 +- 0.26 x 10/sup 15/ years; /sup 232/U total: 69.8 +- 1.0 years; /sup 233/U total: 1.592 +- 0.002 x 10/sup 5/ years; /sup 234/U total: 2.454 +- 0.006 x 10/sup 5/ years; /sup 235/U total: 7.037 +- 0.011 x 10/sup 8/ years; /sup 236/U total: 2.342 +- 0.003 x 10/sup 7/ years /sup 238/U total: 4.468 +- 0.005 x 10/sup 9/ years.

  1. 234U/238U Disequilibria along sedimentary discontinuities in a deep formation: late diagenetic U-relocation processes vs. large scale fluid circulation evidence ?

    NASA Astrophysics Data System (ADS)

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

    2003-04-01

    This work is part of geological investigations undertaken by the French Agency for Nuclear Waste Management (ANDRA) in order to study the safety of radioactive waste repository in deep geological clay layers. The target formation, from Mesozoic sedimentary rocks of the eastern Paris basin (France), is a thick (130--145 m), 400--500 m deep, Callovo-Oxfordian argilite unit, that is over- and underlain by Oxfordian and Bathonian limestones, respectively. Borehole core samples have been analysed for their uranium content and 234U/238U isotopic composition in order to examine the state of radioactive equilibrium existing between these two radionuclides naturally occurring in the rock. Any observations of disequilibrium should allow i) to document the mobility of these actinides in such deposits, and ii) to constrain the time scale of the geological phenomena responsible for it. Highly precise and accurate (234U/238U) analyses were obtained using Multiple Collector Inductively Coupled Plasma Mass Spectrometry. The overall reproducibility, including both chemical separation and spectrometric measurement, is about 0.15% (2σ). Most samples of the target formation and its bounding rocks display secular equilibrium. However, in the Bathonian formation near the interface with the argilite layer, significant (234U/238U) disequilibria are observed along sub-horizontal sedimentary discontinuities, identified as styloliths, indicating that the process involved has been active during the last Ma. Isotopic and elemental compositions of uranium have been determined along a transect, perpendicular to a major discontinuity. The transect exhibits a symmetric pattern relative to this discontinuity with: (1) an increase of the U-concentration towards the stylolitic joint and (2) a sharp transition between significant (234U/238U) < 1 disequilibria in the stylolith to an excess of 234U ((234U/238U) = 1.05) in the vicinity of the joint, followed by a smooth decrease of the activity ratio

  2. Determination of cross sections for the 238U(n,3n)236U reaction induced by 14-MeV neutrons with accelerator mass spectrometry

    NASA Astrophysics Data System (ADS)

    Wang, Xianggao; Jiang, Shan; He, Ming; Dong, Kejun; Xiao, Caijing; Hu, Yueming; You, Qubo; Chen, Hongtao; Hou, Long; Yu, WeiXiang; Ruan, Xichao

    2013-01-01

    The cross sections of the 238U(n,3n)236U reaction induced by neutrons with energies around 14 MeV were determined using a combination of the activation technique and accelerator mass spectrometry (AMS) at the China Institute of Atomic Energy (CIAE). U3O8 samples were irradiated for 198 h by neutrons produced by the 3H(d,n)4He reaction on a 600-kV neutron generator at CIAE. Neutron flux was continuously determined by the activation of flux monitors, Co foils, closely attached to the sample. To accurately determine the long half-life product 236U, an AMS procedure was established with a sensitivity of about 10-11 for 236U/238U. As a result, the cross sections of 238U(n,3n)236U for the incident neutron energies of (14.18±0.30) and (14.65±0.40) MeV were obtained to be (489.3±48.0) and (556.7±27.8) mb, respectively.

  3. Fragment characteristics from fission of 238U and 234U induced by 6.5-9.0 MeV bremsstrahlung

    NASA Astrophysics Data System (ADS)

    Göök, A.; Chernykh, M.; Eckardt, C.; Enders, J.; von Neumann-Cosel, P.; Oberstedt, A.; Oberstedt, S.; Richter, A.

    2011-02-01

    Fission of 238U and 234U induced by bremsstrahlung of 6.5-9.0 MeV endpoint energy has been investigated at the superconducting Darmstadt electron linear accelerator S-DALINAC. Using a twin Frisch grid ionization chamber, fission-fragment energy and mass distributions have been determined by means of the double kinetic-energy technique. Results on the fission-fragment characteristics from U238(γ,f) are in agreement with results from the literature. In addition fission-fragment mass and energy distributions from U234(γ,f) are presented for the first time in this energy region. An analysis of fission modes within the Brosa model has been performed. The relative yield of the S1 mode was found to be (13±3)% in 234U and (35±2)% in 238U.

  4. Early diagenesis of travertine deposits from the Tibetan Plateau - implications for 230Th/234U dating and palaeoenvironmental reconstruction

    NASA Astrophysics Data System (ADS)

    Wang, Zhijun; Meyer, Michael; Hoffmann, Dirk; Spötl, Christoph; Aldenderfer, Mark; Sanders, Diethard

    2014-05-01

    Travertine is calcium carbonate precipitated from hydrothermal springs. These terrestrial carbonate deposits can be used as high-resolution archives for reconstructing palaeoclimatic and palaeoenvironmental change and are also suitable for uranium-series disequilibrium (230Th/234U) dating. In many instances such spring deposits are associated with archaeological remains (e.g. stone artifacts and other traces of prehistoric human activity) and are therefore of interest for palaeoclimatologists and archaeologists alike. However, travertines are often affected by early diagenesis that can impact on the closed-system U-series behavior and on their geochemical signature. Hence, careful evaluation of the travertine microfabrics is required before these types of hot spring deposits can be accurately dated and used for paleoenviromental reconstruction. The Tibetan plateau hosts numerous hydrothermal spring deposits that occur along neotectonic faults. In this study, samples were collected from two archaeological travertine sites, i.e. Chusang and Tirthapuri, located in southern and western Tibet, respectively. Microscopic analysis of thin sections reveals a wide variety of crystal fabrics, including micrite, microspar and sparite, the latter can be composed of columnar or mosaic crystals, respectively. Areas where dendritic crystals are preserved are identified in our micrographs as well. Many of the Chusang and Tirthapuri travertine samples are porous. Drusy sparite is rimming most of the pore walls and a complex succession of secondary calcite phases precipitated in these pore spaces as well. The different generations of pore cement comprise micrite and sparite that can be laminated or fibrous in character and show sometimes evidence of an aragonite precursor. Detrital material like quartz, feldspar and other grains as well as humic and fulvic acids have been washed into the travertine pores too. Based on our microscopic analysis a complex growth history can be

  5. Use of 234U and 238U isotopes to identify fertilizer-derived uranium in the Florida Everglades

    USGS Publications Warehouse

    Zielinski, R.A.; Simmons, K.R.; Orem, W.H.

    2000-01-01

    Surface water and peat in the northern Everglades have very low natural concentrations of U and are therefore sensitive to the addition of small amounts of U from anthropogenic sources such as fertilizer. Peat samples collected along a nutrient gradient in the northern Everglades have unusually high concentrations of U (> 1 ??g/g, dry basis) and also have a distinctive 234U/238U activity ratio (AR). AR values for U-enriched peat fall in the narrow range of AR values for commercial phosphate fertilizer (1.00 ??0.05) In contrast, AR values for low-U peat from background sites exceed 1.05. The spatial distribution of anomalous U concentration, and of fertilizer-like AR values in peat, parallel a previously documented pattern of P enrichment These results strongly suggest that some of the U in nutrient-impacted peatlands is fertilizer-derived. Agricultural drainage water sampled in the northern Everglades has high concentrations of dissolved U (0.3-2.4 ??g/1) compared to surface water from background sites ( 1.05). Synoptic sampling of surface water along drainage canals indicate that Lake Okeechobee, and some drainage from agricultural fields, are sources of dissolved U, whereas wetlands farther downstream act as sinks for U. Historically cultivated agricultural soft has only a marginally elevated (+0.2 ??g/g) average concentration of U compared to nearby uncultivated soil and incorporates only 20% of the U from an aqueous solution that was slurried with the soil. In contrast, a similar experiment with fresh Everglades peat indicated uptake of 90% of the added U. These experiments support the proposed removal of U from agricultural fields and concentration of U in downstream peatlands. The methodology of this study can be used to describe the behavior of fertilizer-derived U in other low-U environments.

  6. 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.

  7. Photofission and photoneutron cross sections and photofission neutron multiplicities for /sup 233/U, /sup 234/U, /sup 237/Np, and /sup 239/Pu

    SciTech Connect

    Berman, B.L.; Caldwell, J.T.; Dowdy, E.J.; Dietrich, S.S.; Meyer, P.; Alvarez, R.A.

    1986-12-01

    The photonuclear cross sections for /sup 233/U, /sup 234/U, /sup 237/Np, and /sup 239/Pu have been measured from threshold up to 18 MeV. The source of radiation was the monoenergetic photon beam from the annihilation in flight of fast positrons. The branching among the neutron-producing reaction channels was determined by measuring the photofission prompt neutron multiplicities nu-bar/sub p/. One interesting result is the complete absence of any (..gamma..,2n) cross section for /sup 233/U and /sup 234/U. The values of nu-bar/sub p/(E) for /sup 234/U agree with those measured with neutrons incident on /sup 233/U. The parameters of the giant dipole resonance deduced from the total photonuclear cross sections show that these nuclei have large static deformations, as expected. The integrated photofission cross sections are large (as are the absolute fission probabilities), and account for 60% to 80% of the total photonuclear absorption strength.

  8. Study of Photon Strength Function of Actinides: the Case of (235)U, (238)Np and (241)Pu

    SciTech Connect

    Guerrero, C.; Koehler, Paul Edward; N_TOF collaboration,

    2011-01-01

    The decay from excited levels in medium and heavy nuclei can be described in a statistical approach by means of Photon Strength Functions and Level Density distributions. The study of electromagnetic cascades following neutron capture based on the use of high efficiency detectors has been shown to be well suited for probing the properties of the Photon Strength Function of heavy (high level density) and/or radioactive (high background) nuclei. In this work we have investigated for the first time the validity of the recommended PSF of actinides, in particular {sup 235}U, {sup 238}Np and {sup 241}Pu. Our study includes the search for resonance structures in the PSF below Sn and draws conclusions regarding their existence and their characteristics in terms of energy, width and electromagnetic nature.

  9. Prompt fission γ-rays from the reactions 252Cf(SF) and 235U(nth, f) - new data

    NASA Astrophysics Data System (ADS)

    Oberstedt, S.; Belgya, T.; Billnert, R.; Bryś, T.; Geerts, W.; Hambsch, F.-J.; Kis, Z.; Martinez, T.; Oberstedt, A.; Szentmiklosi, L.; Vidali, M.

    2013-12-01

    We present new spectral data of prompt γ-ray emission from the spontaneous fission of 252Cf. This work was performed in direct response to an OECD/NEA high priority data request. We discuss the impact of our new data on evaluated nuclear data tables not only for this nuclide, but also for 238U and 241Pu, which are always produced in a reactor. Furthermore, we will show results from our investigation of prompt γ-ray emission from the reaction 235 U(nth, f), measured in at the Centre for Energy Research of the Hungarian Academy of Sciences in Budapest, Hungary. Spectral data obtained with three different detectors are consistent and led to an uncertainty on total energy and multiplicity considerably smaller than requested by the OECD/NEA.

  10. 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.

  11. 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.

  12. 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.

  13. Determination of irradiated reactor uranium in soil samples in Belarus using 236U as irradiated uranium tracer.

    PubMed

    Mironov, Vladislav P; Matusevich, Janna L; Kudrjashov, Vladimir P; Boulyga, Sergei F; Becker, J Sabine

    2002-12-01

    This work presents experimental results on the distribution of irradiated reactor uranium from fallout after the accident at Chernobyl Nuclear Power Plant (NPP) in comparison to natural uranium distribution in different soil types. Oxidation processes and vertical migration of irradiated uranium in soils typical of the 30 km relocation area around Chernobyl NPP were studied using 236U as the tracer for irradiated reactor uranium and inductively coupled plasma mass spectrometry as the analytical method for uranium isotope ratio measurements. Measurements of natural uranium yielded significant variations of its concentration in upper soil layers from 2 x 10(-7) g g(-1) to 3.4 x 10(-6) g g(-1). Concentrations of irradiated uranium in the upper 0-10 cm soil layers at the investigated sampling sites varied from 5 x 10(-12) g g(-1) to 2 x 10(-6) g g(-1) depending on the distance from Chernobyl NPP. In the majority of investigated soil profiles 78% to 97% of irradiated "Chernobyl" uranium is still contained in the upper 0-10 cm soil layers. The physical and chemical characteristics of the soil do not have any significant influence on processes of fuel particle destruction. Results obtained using carbonate leaching of 236U confirmed that more than 60% of irradiated "Chernobyl" uranium is still in a tetravalent form, ie. it is included in the fuel matrix (non-oxidized fuel UO2). The average value of the destruction rate of fuel particles determined for the Western radioactive trace (k = 0.030 +/- 0.005 yr(-1)) and for the Northern radioactive trace (k = 0.035 + 0.009 yr(-1)) coincide within experimental errors. Use of leaching of fission products in comparison to leaching of uranium for study of the destruction rate of fuel particles yielded poor coincidence due to the fact that use of fission products does not take into account differences in the chemical properties of fission products and fuel matrix (uranium). PMID:12509057

  14. 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.

  15. Measurement of electrofission cross sections and photofission yields of sup 235 U and sup 238 U in the energy region 1. 33--4. 32 GeV

    SciTech Connect

    Arakelyan, E.A.; Bayatyan, G.L.; Grigoryan, N.K.; Knyazyan, S.G.; Margaryan, A.T.; Marikyan, G.G. )

    1989-05-01

    Measurements of the electrofission cross sections and photofission yields in the nuclei {sup 235}U and {sup 238}U are reported for electron and bremsstrahlung spectrum energies in the region 1--5 GeV. The data were obtained in experiments with a multiwire low-pressure chamber for detection of fission fragments.

  16. 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.

  17. 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

  18. 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

  19. 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. PMID:27108351

  20. On monitoring anthropogenic airborne uranium concentrations and (235)U/(238)U isotopic ratio by Lichen - bio-indicator technique.

    PubMed

    Golubev, A V; Golubeva, V N; Krylov, N G; Kuznetsova, V F; Mavrin, S V; Aleinikov, A Yu; Hoppes, W G; Surano, K A

    2005-01-01

    Lichens are widely used to assess the atmospheric pollution by heavy metals and radionuclides. However, few studies are available in publications on using lichens to qualitatively assess the atmospheric pollution levels. The paper presents research results applying epiphytic lichens as bio-monitors of quantitative atmospheric contamination with uranium. The observations were conducted during 2.5 years in the natural environment. Two experimental sites were used: one in the vicinity of a uranium contamination source, the other one - at a sufficient distance away to represent the background conditions. Air and lichens were sampled at both sites monthly. Epiphytic lichens Hypogimnia physodes were used as bio-indicators. Lichen samples were taken from various trees at about 1.5m from the ground. Air was sampled with filters at sampling stations. The uranium content in lichen and air samples as well as isotopic mass ratios (235)U/(238)U were measured by mass-spectrometer technique after uranium pre-extraction. Measured content of uranium were 1.45 mgkg(-1) in lichen at 2.09 E-04 microgm(-3) in air and 0.106 mgkg(-1) in lichen at 1.13 E-05 microgm(-3) in air. The relationship of the uranium content in atmosphere and that in lichens was determined, C(AIR)=exp(1.1 x C(LICHEN)-12). The possibility of separate identification of natural and man-made uranium in lichens was demonstrated in principle. PMID:16083999

  1. Angular-anisotropy coefficients for fragment originating from the resonance-neutron-induced fission of {sup 235}U oriented nuclei

    SciTech Connect

    Tambovtsev, D. I.

    2008-04-15

    Statistical distributions of the coefficients measured for the angular distribution of fragments originating from the fission of {sup 235}U oriented nuclei that was induced by resonance neutrons obtained by using booster targets at the electron accelerator in Harwell and at a pulsed reactor in Dubna were approximated by a curve that was calculated under the assumption of a normal distribution of partial-wave fission amplitudes. A cutoff from below at a level of one-half of the average partial-wave width was introduced in this distribution. The calculation was performed with allowance for the K = 0, 1 and 2 channels for J = 3 and the K = 1 and 2 channels for J =4. The contributions of the K channels to the total probability were in the ratio 0.15 : 0.53 : 0.32 for J = 3 and in the ratio 0.625 : 0.375 for J = 4. A strong suppression of the K = 0 channel in the J = 3 spin subsystem in contrast to the situation observed in photofission can be interpreted as an indication of the possible partial conservation of K in resonance states formed from the entrance channel, which features only maximum values of K equal to J and J - 1.

  2. 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.

  3. 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.

  4. 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.

    2016-03-01

    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 82≤ A ≤ 132 and a systematic measurement of ^{92} Rb fission yields, as well as investigations of fission yields toward the symmetry region.

  5. Design of a high-flux epithermal neutron beam using 235U fission plates at the Brookhaven Medical Research Reactor.

    PubMed

    Liu, H B; Brugger, R M; Rorer, D C; Tichler, P R; Hu, J P

    1994-10-01

    Beams of epithermal neutrons are being used in the development of boron neutron capture therapy for cancer. This report describes a design study in which 235U fission plates and moderators are used to produce an epithermal neutron beam with higher intensity and better quality than the beam currently in use at the Brookhaven Medical Research Reactor (BMRR). Monte Carlo calculations are used to predict the neutron and gamma fluxes and absorbed doses produced by the proposed design. Neutron flux measurements at the present epithermal treatment facility (ETF) were made to verify and compare with the computed results where feasible. The calculations indicate that an epithermal neutron beam produced by a fission-plate converter could have an epithermal neutron intensity of 1.2 x 10(10) n/cm2.s and a fast neutron dose per epithermal neutron of 2.8 x 10(-11) cGy.cm2/nepi plus being forward directed. This beam would be built into the beam shutter of the ETF at the BMRR. The feasibility of remodeling the facility is discussed. PMID:7869995

  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. Abundance of low-energy gamma rays in the decay of 238U, 234U, 230Th, 227Ac, 226Ra and 214Pb

    NASA Astrophysics Data System (ADS)

    Komura, K.; Yamamoto, M.; Ueno, K.

    1990-11-01

    Abundance of low-energy gamma rays emitted from 238U (49.5 keV), 227Ac (50.0 keV), 234U (53.2 keV), 214Pb (53.2 keV), 230Th (67.7 and 143.9 keV) and 226Ra (186 keV) was determined using a high-purity Ge low energy photon spectrometer. The results are: 49.5 keV (238U): 0.059±0.002%, 50.0 keV (227Ac): 8.18±0.17%, 53.2 keV (234U): 0.156±0.006%, 53.2 keV (214Pb): 0.927±0.025%, 67.7 keV (230Th): 0.463±0.012%, 143.9 keV (230Th): 0.078±0.007%, 186.0 keV (226Ra): 3.688±0.099%.

  8. 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.

  9. 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.

  10. Searches for T-odd correlations in the emission of prompt neutrons in the polarized-neutron-induced fission of 235U nuclei

    NASA Astrophysics Data System (ADS)

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

    2010-07-01

    The results of an experiment aimed at searches for formally T-odd correlations in the angular distribution of prompt neutrons from the fission of 235U nuclei are presented. The experiment was performed in the MEPHISTO polarized cold-neutron beam from the Munich FRMII reactor. The correlation coefficient proved to be (-3.5 ± 3.4) × 10-5 for a three-vector correlation (TRI effect) and (-5.0 ± 3.4) × 10-5 for a five-vector correlation (ROT effect). This means that no significant effects were discovered within the measurement errors. A comparison with the analogous effects in the ternary fission of 235U nuclei was performed. The values of the corresponding correlations in the angular distribution of prompt fission gamma rays were refined.

  11. The Investigation of the Doppler-Effect of the α-Value of 235U and 239Pu for Different Temperatures

    NASA Astrophysics Data System (ADS)

    Grigoriev, Yu. V.; Kitaev, V. Ya.; Sinitsa, V. V.; Mezentseva, Zh. V.; Faikov-Stanczyk, H.; Janeva, N. B.

    2005-05-01

    The time-of-flight spectra for γ -ray multiplicities from 1 to 15 were measured on the 122-m flight path of the IBR-30 pulsed neutron booster using the 16-section liquid scintillation detector for thin metallic radiator-samples of 235U (0.25 mm) and 239Pu (0.3 mm) at the presence of 235U and 239Pu filter-samples with a thickness of 0.5 mm at two temperatures (100 K and 293 K). Multiplicity spectra, Doppler-coefficients of the capture, fission cross-sections, and alpha values (their ratio) were determined from the time-of-flight spectra for above-mentioned temperatures.

  12. Basic characterization of highly enriched uranium by gamma spectrometry

    NASA Astrophysics Data System (ADS)

    Nguyen, Cong Tam; Zsigrai, József

    2006-05-01

    Gamma-spectrometric methods suitable for the characterization of highly enriched uranium samples encountered in illicit trafficking of nuclear materials are presented. In particular, procedures for determining the 234U, 235U, 238U, 232U and 236U contents and the age of highly enriched uranium are described. Consequently, the total uranium content and isotopic composition can be calculated. For determining the 238U and 232U contents a low-background chamber was used. In addition, age dating of uranium was also performed using low-background spectrometry.

  13. 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)}.

  14. Validating the ENDF-B/VII{sup 235}U(n{sub th},f) prompt fission neutron spectrum using updated dosimetry cross sections (IRDFF)

    SciTech Connect

    Capote, R.; Zolotarev, K. I.; Pronyaev, V. G.; Trkov, A.

    2012-07-01

    The International Reactor Dosimetry File IRDF-2002 released in 2004 by the IAEA contains cross-section data and corresponding uncertainties for 66 dosimetry reactions. New cross-section evaluations have become available recently that re-define some of these dosimetry reactions for reactor applications including: 1) high fidelity evaluation work undertaken by one of the authors (KIZ); 2) evaluations from the ENDF/B-VII libraries that cover reactions within the International Evaluation of Neutron Cross-Section Standards; and 3) evaluations from JENDL-3.1 and JENDL-4 libraries. Overall, 37 new evaluations of dosimetry reactions have been assessed to determine whether they should be adopted to update and improve IRDF-2002. A new dosimetry library (International Reactor Dosimetry File for Fission and Fusion - IRDFF) was assembled based on new evaluations combined with selected IRDF-2002 evaluations. A grand-total of 74 dosimetry reactions are included into the IRDFF dosimetry library available at www-nds.iaea.org/IRDFFI. The assembled library was used to validate the {sup 235}U(n{sub th},f) ENDF-B/VII.0 prompt fission neutron spectrum. An excellent average C/E value of 1.002 +/- 0.02 is achieved for reactions with mean neutron energy of the integrated response (E50%) lower than 11 MeV. C/E data for reactions with E50%-response higher than 11 MeV decreases up to 0.8. We conclude that the ENDF-B/VII.0 {sup 235}U(n{sub th},f) prompt fission neutron spectrum from 1-11 MeV is validated within quoted uncertainties by available integral measurements in {sup 235}U(n{sub th},f) neutron field. Further investigations for high-threshold reactions are needed and new measurements of spectrum average cross sections for those reactions in the {sup 235}U(n{sub th},f) neutron field are recommended. (authors)

  15. Quantification of 235U and 238U activity concentrations for undeclared nuclear materials by a digital gamma-gamma coincidence spectroscopy.

    PubMed

    Zhang, Weihua; Yi, Jing; Mekarski, Pawel; Ungar, Kurt; Hauck, Barry; Kramer, Gary H

    2011-06-01

    The purpose of this study is to investigate the possibility of verifying depleted uranium (DU), natural uranium (NU), low enriched uranium (LEU) and high enriched uranium (HEU) by a developed digital gamma-gamma coincidence spectroscopy. The spectroscopy consists of two NaI(Tl) scintillators and XIA LLC Digital Gamma Finder (DGF)/Pixie-4 software and card package. The results demonstrate that the spectroscopy provides an effective method of (235)U and (238)U quantification based on the count rate of their gamma-gamma coincidence counting signatures. The main advantages of this approach over the conventional gamma spectrometry include the facts of low background continuum near coincident signatures of (235)U and (238)U, less interference from other radionuclides by the gamma-gamma coincidence counting, and region-of-interest (ROI) imagine analysis for uranium enrichment determination. Compared to conventional gamma spectrometry, the method offers additional advantage of requiring minimal calibrations for (235)U and (238)U quantification at different sample geometries. PMID:21411329

  16. Isotopic compositions of (236)U and Pu isotopes in "black substances" collected from roadsides in Fukushima prefecture: fallout from the Fukushima Dai-ichi nuclear power plant accident.

    PubMed

    Sakaguchi, Aya; Steier, Peter; Takahashi, Yoshio; Yamamoto, Masayoshi

    2014-04-01

    Black-colored road dusts were collected in high-radiation areas in Fukushima Prefecture. Measurement of (236)U and Pu isotopes and (134,137)Cs in samples was performed to confirm whether refractory elements, such as U and Pu, from the fuel core were discharged and to ascertain the extent of fractionation between volatile and refractory elements. The concentrations of (134,137)Cs in all samples were exceptionally high, ranging from 0.43 to 17.7 MBq/kg, respectively. (239+240)Pu was detected at low levels, ranging from 0.15 to 1.14 Bq/kg, and with high (238)Pu/(239+240)Pu activity ratios of 1.64-2.64. (236)U was successfully determined in the range of (0.28 to 6.74) × 10(-4) Bq/kg. The observed activity ratios for (236)U/(239+240)Pu were in reasonable agreement with those calculated for the fuel core inventories, indicating that trace amounts of U from the fuel cores were released together with Pu isotopes but without large fractionation. The quantities of U and (239+240)Pu emitted to the atmosphere were estimated as 3.9 × 10(6) Bq (150 g) and 2.3 × 10(9) Bq (580 mg), respectively. With regard to U, this is the first report to give a quantitative estimation of the amount discharged. Appreciable fractionation between volatile and refractory radionuclides associated with the dispersal/deposition processes with distance from the Fukushima Dai-ichi Nuclear Power Plant was found. PMID:24601520

  17. 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.

  18. Incomplete-fusion reactions for {gamma}-ray spectroscopy: Application to the study of high-spin states in {sup 234}U

    SciTech Connect

    Lane, G. J.; Dracoulis, G. D.; Byrne, A. P.; McGoram, T. R.; Poletti, A. R.

    1999-09-02

    Incomplete-fusion reactions occur when breakup of the projectile results in only part of the beam particle fusing with the target, the remnant being emitted with an energy equivalent to the beam velocity. Such reactions have been demonstrated to populate slightly neutron-rich nuclei compared to conventional fusion-evaporation reactions, opening possibilities for the study of nuclei along the neutron-rich side of the line of stability. Results from a study of {sup 211}Po are presented to illustrate the use of incomplete-fusion reactions for {gamma}-ray spectroscopy. New results from a test-run which populated high-spin states in {sup 234}U via the {sup 232}Th({sup 9}Be,{alpha}3n) reaction are also presented. An interesting feature of the latter reaction is that the high fission probabilities for the compound nuclei which follow complete fusion, results in the residues from incomplete fusion forming the dominant residue channels.

  19. Determination of {sup 230}Th, {sup 234}U, {sup 239}Pu, and {sup 240}Pu in soils by ICP-MS using flow-injection preconcentration

    SciTech Connect

    Hollenbach, M.; Grohs, J.; Mamich, S.; Kroft, M.

    1995-12-31

    The US Department of Energy needs improved analytical methods for alpha-emitting radionuclides to support environmental restoration and waste management projects. Inductively coupled plasma-mass spectrometry (ICP-MS) has been used successfully to measure radionuclides with relatively long half-lives; however, ICP-MS used with conventional sample introduction techniques lacks the sensitivity or selectivity to measure shorter-lived radionuclides at levels important for environmental monitoring. New methods were developed for measuring {sup 230}Th, {sup 234}U, {sup 239}Pu, and {sup 240}Pu in soils. Samples are dried, ground, and dissolved by fusion. A flow injection (FI) analysis system is used to separate and concentrate the analytes by solid-phase extraction. The FI eluent is pumped directly into the nebulizer of the ICP-MS. The use of FI resulted in greater sensitivity and freedom from interferences when compared with direct aspiration. Detection limits are improved by approximately a factor of 20. The detection limits are approximately 3 Bq/kg (4 ng/kg) for {sup 230}Th, 0.6 Bq/kg (3 ng/kg) for {sup 234}U, 0.4 Bq/kg (0.2 ng/kg) for {sup 239}Pu, and 2 Bq/kg (0.3 ng/kg) for {sup 240}Pu. The FI-ICP-MS methods are faster, less labor intensive, and generate less laboratory waste than traditional radiochemical methods. The FI-ICP-MS gives individual results for {sup 239}Pu and {sup 240}Pu which cannot be resolved by the usual radiochemical method. The accuracy of the methods was verified by analyzing reference soils.

  20. 234U/238U isotope ratios in groundwater from Southern Nevada: a comparison of alpha counting and magnetic sector ICP-MS.

    PubMed

    Cizdziel, James; Farmer, Dennis; Hodge, Vernon; Lindley, Kazumasa; Stetzenbach, Klaus

    2005-11-01

    The 234U/238U activity ratio (AR) is extensively used as a geochemical tool to investigate movement and flow relationships in major hydrological units, information that is particularly important when considering nuclear waste disposal. It is usually determined by radiochemical separation and concentration of U, followed by energy-specific alpha particle counting. Alternatively, sector field inductively coupled plasma mass spectrometry (SF-ICP-MS) can be used to measure U isotopic signatures directly in groundwater samples. Here, we compare the two methods for samples of spring and groundwater from southern Nevada. Results for samples stripped from stainless steel disks, previously used for alpha counting, and for splits of groundwater samples show good agreement between the methods. However, SF-ICP-MS is faster, requires much less sample, and produces essentially no waste. We demonstrate applicability of the SF-ICP-MS method for groundwater collected from over 25 wells on and near the Nevada Test Site during 2003. Uranium concentrations ranged from 0.17 to 9.87 ppb with a mean of 2.9 ppb, while 234U/238U AR values ranged from 1.9 to 11.5 with a mean of 4.3. Groundwater collected from deep wells in the northern part of the study area tended to have moderate to high U concentrations and AR values, possibly representative of older volcanic-type waters, whereas groundwater from wells in the Fortymile Wash area had relatively low AR and U concentrations, suggesting younger waters with a possible local recharge component. PMID:16227084

  1. Trace element distribution and 235U/238U ratios in Euphrates waters and in soils and tree barks of Dhi Qar province (southern Iraq).

    PubMed

    Riccobono, Francesco; Perra, Guido; Pisani, Anastasia; Protano, Giuseppe

    2011-09-01

    To assess the quality of the environment in southern Iraq after the Gulf War II, a geochemical survey was carried out. The survey provided data on the chemistry of Euphrates waters, as well as the trace element contents, U and Pb isotopic composition, and PAH levels in soil and tree bark samples. The trace element concentrations and the (235)U/(238)U ratio values in the Euphrates waters were within the usual natural range, except for the high contents of Sr due to a widespread presence of gypsum in soils of this area. The trace element contents in soils agreed with the common geochemistry of soils from floodplain sediments. Some exceptions were the high contents of Co, Cr and Ni, which had a natural origin related to ophiolitic outcrops in the upper sector of the Euphrates basin. The high concentrations of S and Sr were linked to the abundance of gypsum in soils. A marked geochemical homogeneity of soil samples was suggested by the similar distribution pattern of rare earth elements, while the (235)U/(238)U ratio was also fairly homogeneous and within the natural range. The chemistry of the tree bark samples closely reflected that of the soils, with some notable exceptions. Unlike the soils, some tree bark samples had anomalous values of the (235)U/(238)U ratio due to mixing of depleted uranium (DU) with the natural uranium pool. Moreover, the distribution of some trace elements (such as REEs, Th and Zr) and the isotopic composition of Pb in barks clearly differed from those of the nearby soils. The overall results suggested that significant external inputs occurred implying that once formed the DU-enriched particles could travel over long distances. The polycyclic aromatic hydrocarbon concentrations in tree bark samples showed that phenanthrene, fluoranthene and pyrene were the most abundant components, indicating an important role of automotive traffic. PMID:21774965

  2. 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.

  3. Product yields of sup 235 U, sup 238 U, sup 237 Np, and sup 239 Pu by photofission reactions with 20-, 30-, and 60-MeV Bremsstrahlung

    SciTech Connect

    Kase, T.; Yamadera, A.; Nakamura, T. ); Shibata, S. ); Fujiwara, I. )

    1992-08-01

    This paper reports that as a basic study of photonuclear transmutation of actinides in high-level radioactive wastes using electron-produced bremsstrahlung, the absolute yields of cumulative mass distributions and the transmutation rate of {sup 235}U, {sup 238}U, {sup 237}Np, and {sup 239}Pu by photofission reactions induced by 20-, 30-, and 60-MeV bremsstrahlung were measured. The results of mass yield distributions and transmutation yields agree well with other experimental results and those calculated using photofission cross sections, respectively. The transmutation efficiency per electron increases about one order of magnitude with electron energy from 20 to 60 MeV.

  4. Monte Carlo cross section testing for thermal and intermediate {sup 235}U/{sup 238}U critical assemblies, ENDF/B-V vs ENDF/B-VI

    SciTech Connect

    Weinman, J.P.

    1997-06-01

    The purpose of this study is to investigate the eigenvalue sensitivity to changes in ENDF/B-V and ENDF/B-VI cross section data sets by comparing RACER vectorized Monte Carlo calculations for several thermal and intermediate spectrum critical experiments. Nineteen Oak Ridge and Rocky Flats thermal solution benchmark critical assemblies that span a range of hydrogen-to-{sup 235}U (H/U) concentrations (2052 to 27.1) and above-thermal neutron leakage fractions (0.555 to 0.011) were analyzed. In addition, three intermediate spectrum critical assemblies (UH3-UR, UH3-NI, and HISS-HUG) were studied.

  5. Analysis of 236U and plutonium isotopes, 239,240Pu, on the 1 MV AMS system at the Centro Nacional de Aceleradores, as a potential tool in oceanography

    NASA Astrophysics Data System (ADS)

    Chamizo, Elena; López-Lora, Mercedes; Villa, María; Casacuberta, Núria; López-Gutiérrez, José María; Pham, Mai Khanh

    2015-10-01

    The performance of the 1 MV AMS system at the CNA (Centro Nacional de Aceleradores, Seville, Spain) for 236U and 239,240Pu measurements has been extensively investigated. A very promising 236U/238U abundance sensitivity of about 3 × 10-11 has been recently achieved, and background figures for 239Pu of about 106 atoms were reported in the past. These promising results lead to the use of conventional low energy AMS systems for the analysis of 236U and 239Pu and its further application in environmental studies. First 236U results obtained on our AMS system for marine samples (sediments and water) are presented here. Results of two new IAEA reference materials (IAEA-410 and IAEA-412, marine sediments from Pacific Ocean) are reported. The obtained 236U/239Pu atom ratios, of 0.12 and 0.022, respectively, show a dependency with the contamination source (i.e. local fallout from the US tests performed at the Bikini Atoll and general fallout). The results obtained for a third IAEA reference material (IAEA-381, seawater from the Irish Sea), are also presented. In the following, the uranium and plutonium isotopic compositions obtained on a set of 5 intercomparison seawater samples from the Arctic Ocean provided by the ETH Zürich are discussed. By comparing them with the obtained results on the 600 kV AMS facility Tandy at the ETH Zürich, we demonstrate the solidity of the CNA technique for 236U/238U determinations at, at least, 7 × 10-10 level. Finally, these results are discussed in their environmental context.

  6. Determination of transfer time for sediments in alluvial plains using 238U-234U-230Th disequilibria: The case of the Ganges river system

    NASA Astrophysics Data System (ADS)

    Chabaux, François; Blaes, Estelle; Granet, Mathieu; Roupert, Raphaël di Chiara; Stille, Peter

    2012-11-01

    An approach to deriving the transfer time of sediments within alluvial plains by using the variation of the U-series nuclides in sediments collected along rivers is presented in this article and discussed in the light of new data from samples from different locations within the Ganges watershed and its outlet. These data indicate that the upstream-downstream variation of 238U-234U-230Th disequilibria in the sediments, with different variation trends for suspended and coarse-grained sediments, is probably a general feature of all Himalayan rivers flowing across the Indo-Gangetic plain. The data therefore confirm the occurrence of very different transfer times within the plain, depending on the sediments granulometry, with much shorter transfer time for the fine-grained (a few ky or less) than for the coarse-grained sediments (100 ky or more). A new solving approach, using a parallel stochastic Quantum-behaved Particle Swarm Optimization (p-QPSO), has been developed for identifying the unknown parameters of the model necessary for the determination of the transfer time. The data of sediments collected at the Ganges outlet show significant variations of the 234U/230Th activity ratios for the fine-grained sediment end-member collected in 2004 and 2008. Such variations indicate that the fine-grained sediments transit quickly (a year or less) within the plain. The highly variable activity ratios might be the result of quickly changing weathering intensities. Conversely, the U-Th variations observed for the 2004 and 2008 bedload from the Ganges basin cannot result from a short sedimentary transfer time. They probably result from the dredge sampling procedure, which might be influenced by local placer effects controlling the abundance of U and Th carrying minerals. Dredging may not allow the sampling of a representative bedload, hence it may cause an artificial mineralogical and, therefore, an U-Th variability for bedload sediments collected at different periods. At this

  7. Use of delayed gamma rays for active non-destructive assay of 235U irradiated by pulsed neutron source (plasma focus)

    NASA Astrophysics Data System (ADS)

    Andola, Sanjay; Niranjan, Ram; Kaushik, T. C.; Rout, R. K.; Kumar, Ashwani; Paranjape, D. B.; Kumar, Pradeep; Tomar, B. S.; Ramakumar, K. L.; Gupta, S. C.

    2014-07-01

    A pulsed neutron source based on plasma focus device has been used for active interrogation and assay of 235U by monitoring its delayed high energy γ-rays. The method involves irradiation of fissile material by thermal neutrons obtained after moderation of a burst of neutrons emitted upon fusion of deuterium in plasma focus (PF) device. The delayed gamma rays emitted from the fissile material as a consequence of induced fission were detected by a large volume sodium iodide (NaI(Tl)) detector. The detector is coupled to a data acquisition system of 2k input size with 2k ADC conversion gain. Counting was carried out in pulse height analysis mode for time integrated counts up to 100 s while the temporal profile of delayed gamma has been obtained by counting in multichannel scaling mode with dwell time of 50 ms. To avoid the effect of passive (natural) and active (from surrounding materials) backgrounds, counts have been acquired for gamma energy between 3 and 10 MeV. The lower limit of detection of 235U in the oxide samples with this set-up is estimated to be 14 mg.

  8. Characterisation of airborne uranium and thorium contamination in northern England through measurement of U, Th and 235U/238U in tree bark.

    PubMed

    Bellis, D J; Ma, R; McLeod, C W

    2001-02-01

    Samples of tree bark were collected from four locations in Northern England (a typical rural site, a coal-fired power station, a uranium (isotopic) enrichment plant and a nuclear fuel fabrication facility), to assess the nature and extent of airborne uranium and thorium contamination. The U and Th concentrations of bark were determined by inductively coupled plasma mass spectrometry after conventional nebulisation of bark digests, whilst measurement of 235U/238U isotopic ratio utilised high efficiency nebulisation. Uranium concentrations varied between and within the sites (range, 0.01-12 micrograms g-1), with maximum values recorded within 1 km of the nuclear fuel fabrication plant (Springfields). In comparison, the concentration of Th in bark was low (mean, 0.018 microgram g-1) at all sites with the exception of the area affected by coal combustion (0.2-0.8 microgram g-1). The U/Th ratio varied from 0.5 to 3900 compared with the average crustal ratio of 0.3. Low values (< 2) were recorded at the 'coal' and 'rural' sites whilst Capenhurst and Springfields showed high values indicating the relative magnitude of uranium elevation. Significant enrichment of the natural 235U/238U ratio (0.00725) was observed near the nuclear installations, in particular, the enrichment plant (Capenhurst). PMID:11354728

  9. [Determination of 235U/238U isotope ratios in camphor tree bark samples by MC-ICP-MS after separation of uranium from matrix elements].

    PubMed

    Wang, Xiao-Ping; Zhang, Ji-Long

    2007-07-01

    Twelve camphor (cinnamomum camphora) tree bark samples were collected from Hiroshima and Kyoto, and the matrix element composition and morphology of the outer surface of these camphor tree bark samples were studied by EDXS and SEM respectively. After a dry decomposition, DOWEX 1-X8 anion exchange resin was used to separate uranium from matrix elements in these camphor tree bark samples. Finally, 235U/238 U isotope ratios in purified uranium solutions were determined by MC-ICP-MS. It was demonstrated that the outer surface of these camphor tree bark samples is porous and rough, with Al, Ca, Fe, K, Mg, Si, C, O and S as its matrix element composition. Uranium in these camphor tree bark samples can be efficiently separated and quantitatively recovered from the matrix element composition. Compared with those collected from Kyoto, the camphor tree bark samples collected from Hiroshima have significantly higher uranium contents, which may be due to the increased aerosol mass concentration during the city reconstruction. Moreover, the 235 U/23.U isotope ratios in a few camphor tree bark samples collected from Hiroshima are slightly higher than 0.007 25. PMID:17944430

  10. Actinides AMS at CIRCE and 236U and Pu measurements of structural and environmental samples from in and around a mothballed nuclear power plant

    NASA Astrophysics Data System (ADS)

    De Cesare, M.; Fifield, L. K.; Sabbarese, C.; Tims, S. G.; De Cesare, N.; D'Onofrio, A.; D'Arco, A.; Esposito, A. M.; Petraglia, A.; Roca, V.; Terrasi, F.

    2013-01-01

    Accelerator mass spectrometry (AMS) is presently the most sensitive technique for the measurement of long-lived actinides, e.g. 236U and 239Pu. A new actinide line is in operation at the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy. Using the actinide line a uranium mass sensitivity of around 4 μg has been reached measuring with a 16-strip silicon detector, and a 239Pu background level of below 0.1 fg has been obtained. In this work we also discuss preliminary results for environmental and structural samples from in and around the Garigliano nuclear power plant (GNPP), presently in the decommissioning phase. Measurements on environmental samples from the vicinity of the plant allow the assessment of contamination, if any, over the years. Measurements of structural samples from the plant are relevant to the optimization of the decommissioning program for the GNPP.

  11. Determination of total and isotopic uranium and total thorium in soils by inductively coupled plasma-mass spectrometry

    SciTech Connect

    Bolin, R.N.

    1995-12-31

    Inductively coupled plasma-mass spectrometry (ICP-MS), using standard sample introduction by peristaltic pumping, is presented as a method to determine total and isotopic uranium ({sup 234}U, {sup 235}U, {sup 236}U, and {sup 238}U) and thorium ({sup 232}Th) in soil samples. Initial sample preparation consists of oven drying to determine moisture content, and grinding and mixing the soil to make it homogeneous. This is followed by a nitric/hydrofluoric acid digestion to bring the uranium into solution. Bismuth ({sup 209}Bi) is added prior to digestion to monitor for losses due to sample preparation and analysis. An addition digestion, using nitric/perchloric acid is performed if the total thorium concentration is required on the sample. The uranium and thorium content of this solution and the {sup 235}U/{sup 238}U ratio are measured on an initial pass through the ICP-MS. The total uranium measurement is based on the {sup 238}U isotope measurement with correction for the presence of the U isotopes. To determine the concentration of the less abundant {sup 234}U and {sup 236}U isotopes, the digestate is further concentrated by using a solid phase extraction column (TRU.Spec by EiChrom Industries, Inc.) before a second pass through the ICP-MS.

  12. Surrogate measurement of the {sup 238}Pu(n,f) cross section

    SciTech Connect

    Ressler, J. J.; Burke, J. T.; Escher, J. E.; Bernstein, L. A.; Bleuel, D. L.; Casperson, R. J.; Gostic, J.; Henderson, R.; Scielzo, N. D.; Thompson, I. J.; Wiedeking, M.; Angell, C. T.; Goldblum, B. L.; Munson, J.; Basunia, M. S.; Phair, L. W.; Beausang, C. W.; Hughes, R. O.; Hatarik, R.; Ross, T. J.

    2011-05-15

    The neutron-induced fission cross section of {sup 238}Pu was determined using the surrogate ratio method. The (n,f) cross section over an equivalent neutron energy range 5-20 MeV was deduced from inelastic {alpha}-induced fission reactions on {sup 239}Pu, with {sup 235}U({alpha},{alpha}{sup '}f) and {sup 236}U({alpha},{alpha}{sup '}f) used as references. These reference reactions reflect {sup 234}U(n,f) and {sup 235}U(n,f) yields, respectively. The deduced {sup 238}Pu(n,f) cross section agrees well with standard data libraries up to {approx}10 MeV, although larger values are seen at higher energies. The difference at higher energies is less than 20%.

  13. Isotopic Compositions of Uranium Reference Materials

    NASA Astrophysics Data System (ADS)

    Jacobsen, B.; Borg, L. E.; Williams, R. W.; Brennecka, G.; Hutcheon, I. D.

    2009-12-01

    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 238U/235U, as well as the minor isotopes of U. Differences of ~1.3‰ are now being observed in 238U/235U 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 238U/235U ratios were measured with a TRITON TIMS using a mixed 233U-236U isotopic tracer to correct for instrument fractionation. This tracer was extremely pure and resulted in only very minor corrections on the measured 238U/235U ratios of ~0.03. The values obtained for 238U/235U 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. Our 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 238U/235U ratio. Thus, the isotopic compositions determined using both instruments are compatible. The values obtained for 234U/235U are: SRM950a = (7.437 ± 0.043)x10-3 (n=18), and CRM112a = (7.281 ± 0.050)x10-3 (n=16), both of which are in good agreement with published values. The value for 236U/235U in SRM950a was determined to be (8.48 ± 2.63)x10-6, whereas 236U was not detected in CRM112a. We are currently obtaining the U isotopic composition of

  14. 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.

  15. Calculation of 1.25% 235U enriched UO2 solution safe slab, safe cylinder diameter, minimum safe mass, and ion exchange module for the CVDF

    SciTech Connect

    Roblyer, S.P.

    1997-06-26

    Support calculations were performed to establish safe parameters such as fissionable material slab thickness, diameter and safe mass. These calculations were performed by MCNP for the balance of plant equipment that contains homogeneous UO{sub 2} solutions with a maximum enrichment of 1.25 Wt% {sup 235}U . The calculations were performed with the most limiting concentration of moderator and reflection so that only the safety parameters identified in the problem description need to be controlled. These calculations represent the most limiting cases for all uranium enrichments and transuranic levels due to fuel exposure for balance of plant equipment used for handling of waste water containing fissionable materials from the MCO draining and drying activities.

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

    DOE PAGESBeta

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

    2015-07-28

    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

  17. 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. PMID:26225462

  18. 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).

  19. 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

  20. 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. PMID:27081973

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

    NASA Astrophysics Data System (ADS)

    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 235U 235 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 86Ge 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.

  2. Improvements in 230Th dating, 230Th and 234U half-life values, and U-Th isotopic measurements by multi-collector inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Cheng, Hai; Lawrence Edwards, R.; Shen, Chuan-Chou; Polyak, Victor J.; Asmerom, Yemane; Woodhead, Jon; Hellstrom, John; Wang, Yongjin; Kong, Xinggong; Spötl, Christoph; Wang, Xianfeng; Calvin Alexander, E.

    2013-06-01

    We have developed techniques for measuring 234U and 230Th on Faraday cups with precisions of 1-3 epsilon units (1 ɛ-unit=1 part in 104) using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Using a Thermo-Scientific Neptune with desolvation nebulization, we obtained ionization/transmission efficiencies of 1-2% for both U and Th. We set up protocols to correct for tailing, prepared U and Th gravimetric standards, tested a Th mass fractionation correction procedure based on U isotopes, and identified natural calcite samples likely to be in U-Th isotopic secular equilibrium. The measured atomic ratios, 234U/238U=54.970 (±0.019)×10-6 and 230Th/238U=16.916 (±0.018)×10-6, for these calcite samples were identical within errors (quoted 2σ uncertainties calculated combining all sources of error). Half-life values calculated from these ratios are consistent with previous values, but have much smaller errors: 245,620±260 a for 234U and 75,584±110 a for 230Th (quoted 2σ uncertainties calculated using all sources of error). In calculating a 230Th age, some of the systematic errors included in estimating the full error in the half-lives effectively cancel. Removing these uncertainties (uncertainty in the 238U half-life value, uncertainty in our gravimetric uranium and thorium standards, and uncertainty in the absolute isotopic composition of the uranium standard), yields effective uncertainties for the purposes of 230Th dating of ±70 a for the 234U half-life value and ±30 a for the 230Th half-life value. Under ideal circumstances, with our methods, the 2σ uncertainty in age, including uncertainty in half-life values is ±10 a at 10 ka, ±100 a at 130 ka, ±300 a at 200 ka, ±1 ka at 300 ka, ±2 ka at 400 ka, ±6 ka at 500 ka, and ±12 ka at 600 ka. The isotopic composition of a sample with an age <800 ka can clearly be resolved from the isotopic composition of a sample in secular equilibrium, assuming closed system behavior. Using these

  3. 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.

  4. 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.

  5. Experimental Determination of the Ratio of {sup 238}U Capture to {sup 235}U Fission in LEU-HTR Pebble-Bed Configurations

    SciTech Connect

    Koeberl, O.; Chawla, R.

    2004-01-15

    The shift toward low-enrichment uranium (LEU) fuel for gas-cooled high-temperature reactors (HTRs) has revealed a lack of experimental data for validating neutronics codes that are used for the design and licensing of such systems. In the framework of the LEU-HTR experimental program at the PROTEUS critical facility, the safety-related effects of accidental moderation increase (ingress of water or other hydrogeneous compounds) in pebble-bed HTR core configurations employing low-enriched (16.7%) fuel were investigated. An important neutron balance component in this context is the integral reaction rate ratio of {sup 238}U capture (C{sub 8}) relative to {sup 235}U fission (F{sub 5}).It was necessary to develop new experimental techniques for the accurate measurement of C{sub 8}/F{sub 5} in the doubly heterogeneous fuel pebbles. These have involved the utilization of specially prepared particle foils on the one hand and the counting of whole fuel pebbles on the other. Core-center measurements employing both experimental methods have been carried out in two different HTR-PROTEUS configurations (with and without accidental moderation increase simulation, respectively). In each case, satisfactory agreement was obtained between the experimental results based on the two techniques. By carrying out a comparison of particle-foil C{sub 8}/F{sub 5} measurements in the PROTEUS reactor's thermal column with the results of standard foil-activation measurement techniques, the systematic uncertainty (1{sigma}) of the core-center measurements could be reduced by {approx}0.6%, yielding a net experimental error of {+-}1% with either of the new methods. A comparison of the experimental results with calculations based on the MICROX-2/TWODANT codes in conjunction with JEF-1 cross sections has indicated that this calculational route overpredicts the core-center C{sub 8}/F{sub 5} value by {approx}2.5% in both the investigated configurations.

  6. Investigations of the Space Parity Violation and Interference Effects in the Fragment Angular Distributions of 235U, 233U, and 239Pu Fission by Resonance Neutrons

    NASA Astrophysics Data System (ADS)

    Sokolov, V. E.; Gagarski, A. M.; Guseva, I. S.; Golosovskaya, S. P.; Krasnoshchokova, I. S.; Petrov, G. A.; Petrova, V. I.; Petukhov, A. K.; Pleva, Yu. S.; Alfimenkov, V. P.; Chernikov, A. N.; Lason, L.; Mareev, Yu. D.; Novitski, V. V.; Pikelner, L. B.; Pikelner, T. L.; Tsulaya, M. I.

    2005-05-01

    Investigations of the space parity nonconserving (PNC) asymmetry of 233U, 235U, and 239Pu fission fragment emission and parity conserving (PC) interference effects of left-right and forward-backward asymmetries were carried out on the neutron beams of the reactor IBR-30 (JINR, Dubna) over the range of neutron energies from 0.02 eV to about 100 eV. All experimental results obtained have been found to be in a good mutual accordance within the frames of modern theoretical conceptions about the mechanisms of PNC and PC effects forming in fission process induced by slow neutrons. In case of the P-even interference effects of asymmetry the evident mutual well-marked irregularities in their neutron energy dependencies up to about 100 eV were observed. It is connected with the interference of s, p-resonances at fission compound stage according to modern theory. As a remarkable result of the PNC effect measurements the resonance behavior of the PNC asymmetry coefficients in the low neutron energy region (En < 2 eV) was observed. Unfortunately, the statistical accuracy of the PNC effect measurements is not enough for observation of these resonance effects in other cases of more high energies. Results of simultaneous analysis of all three asymmetry effects for all three nuclei are presented. The satisfactory combined description of the experimental points is received. As a result of theoretical evaluation of these data main parameters and the estimates of nuclear matrix elements of the weak interaction for some p-resonances in the low energy range were extracted.

  7. NUSIMEP-7: uranium isotope amount ratios in uranium particles.

    PubMed

    Truyens, J; Stefaniak, E A; Aregbe, Y

    2013-11-01

    The Institute for Reference Materials and Measurements (IRMM) has extensive experience in the development of isotopic reference materials and the organization of interlaboratory comparisons (ILC) for nuclear measurements in compliance with the respective international guidelines (ISO Guide 34:2009 and ISO/IEC 17043:2010). The IRMM Nuclear Signatures Interlaboratory Measurement Evaluation Program (NUSIMEP) is an external quality control program with the objective of providing materials for measurements of trace amounts of nuclear materials in environmental matrices. Measurements of the isotopic ratios of the elements uranium and plutonium in small amounts, typical of those found in environmental samples, are required for nuclear safeguards and security, for the control of environmental contamination and for the detection of nuclear proliferation. The measurement results of participants in NUSIMEP are evaluated according to international guidelines in comparison to independent external certified reference values with demonstrated metrological traceability and uncertainty. NUSIMEP-7 focused on measurements of uranium isotope amount ratios in uranium particles aiming to support European Safeguards Directorate General for Energy (DG ENER), the International Atomic Energy Agency's (IAEA) network of analytical laboratories for environmental sampling (NWAL) and laboratories in the field of particle analysis. Each participant was provided two certified test samples: one with single and one with double isotopic enrichment. These NUSIMEP test samples were prepared by controlled hydrolysis of certified uranium hexafluoride in a specially designed aerosol deposition chamber at IRMM. Laboratories participating in NUSIMEP-7 received the test samples of uranium particles on two graphite disks with undisclosed isotopic ratio values n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U). The uranium isotope ratios had to be measured using their routine analytical

  8. Study on Prompt Fission Neutron Spectra and Associated Covariances for 235U(nth,f) and 239Pu(nth,f)

    NASA Astrophysics Data System (ADS)

    Berge, L.; Litaize, O.; Serot, O.; Jean, C. De Saint; Archier, P.; Peneliau, Y.

    normalization of experimental spectra, and the uncertainty on the energy-dependent neutron detection efficiency. We show the resulting PFNS and associated covariance matrix in the case of thermal neutron-induced fission of 235U and 239Pu.

  9. 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.

  10. 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

  11. 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

  12. Fragment-mass, kinetic energy, and angular distributions for 234U(n ,f ) at incident neutron energies from En=0.2 MeV to 5.0 MeV

    NASA Astrophysics Data System (ADS)

    Al-Adili, A.; Hambsch, F.-J.; Pomp, S.; Oberstedt, S.; Vidali, M.

    2016-03-01

    This work investigates the neutron-induced fission of 234U and the fission-fragment properties for neutron energies between En=0.2 and 5.0 MeV with a special highlight on the prominent vibrational resonance at En=0.77 MeV. Angular, energy, and mass distributions were determined based on the double-energy technique by means of a twin Frisch-grid ionization chamber. The experimental data are parametrized in terms of fission modes based on the multimodal random neck-rupture model. The main results are a verified strong angular anisotropy and fluctuations in the energy release as a function of incident-neutron energy.

  13. (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

  14. 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.

  15. 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.

  16. Indirect Determination of the 230Th(n,f) and 231Th(n,f) Cross Sections for Thorium-Based Nuclear Energy Systems

    SciTech Connect

    Stroberg, S.R.; Allmond, J.M.; Angell, C.; Bernstein, L.A.; Bleuel, D.L.; Burke, J.T.; Gibelin, J.; Phair, L.; Scielzo, N.D.; Swanberg, E.; Wiedeking, M.; Norman, E.B.; Goldblum, Bethany

    2009-09-11

    The Surrogate Ratio Method (SRM) was employed in the first experimental determination of the 231Th(n,f) cross section, relative to the 235U(n,f) cross section, over an equivalent neutron energy range of 360 keV to 10 MeV. The 230Th(n,f) cross section was also deduced using the SRM, relative to the 234U(n,f) cross section, over an equivalent neutron energy range of 220 keV to 25 MeV. The desired compound nuclei were populated using (3He,3He) and (3He) reactions on targets of 232Th and 236U and relative fission decay probabilities were measured. The surrogate 230,231Th(n,f) cross sections were compared to cross section evaluations and directly-measured experimental data, where available.

  17. 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.

  18. Indirect determination of the {sup 230}Th(n,f) and {sup 231}Th(n,f) cross sections for thorium-based nuclear energy systems

    SciTech Connect

    Goldblum, B. L.; Stroberg, S. R.; Angell, C.; Swanberg, E.; Allmond, J. M.; Bernstein, L. A.; Bleuel, D. L.; Burke, J. T.; Scielzo, N. D.; Wiedeking, M.; Gibelin, J.; Phair, L.; Norman, E. B.

    2009-10-15

    The surrogate ratio method (SRM) was employed in the first experimental determination of the {sup 231}Th(n,f) cross section, relative to the {sup 235}U(n,f) cross section, over an equivalent neutron energy range of 360 keV to 10 MeV. The {sup 230}Th(n,f) cross section was also deduced using the SRM, relative to the {sup 234}U(n,f) cross section, over an equivalent neutron energy range of 220 keV to 25 MeV. The desired compound nuclei were populated using ({sup 3}He,{sup 3}He') and ({sup 3}He,{alpha}) reactions on targets of {sup 232}Th and {sup 236}U and relative fission decay probabilities were measured. The surrogate {sup 230,231}Th(n,f) cross sections were compared to cross section evaluations and directly-measured experimental data, where available.

  19. 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)

  20. 235U, 238U, 232Th, 40K and 137Cs activity concentrations in marine sediments along the northern coast of Oman Sea using high-resolution gamma-ray spectrometry.

    PubMed

    Zare, Mohammad Reza; Mostajaboddavati, Mojtaba; Kamali, Mahdi; Abdi, Mohammad Reza; Mortazavi, Mohammad Seddigh

    2012-09-01

    The natural radioactivity levels in sediment samples of the northern coast of Oman Sea, covering the coastal strip from Hormoz canyon to Goatr seaport, as the first time has been determined. The results of measurements will serve as background reference level for Oman Sea coastlines. Sediments from 36 coastal and near shore locations were collected for analysis. Analysis on the collected samples were carried out to determine (235)U, (238)U, (232)Th, (40)K and (137)Cs using two high purity germanium detectors with 38.5% and 55% relative efficiencies. The concentration of (235)U, (238)U, (232)Th, (40)K and (137)Cs in sediment samples ranged between 1.01 and 2.87 Bq/kg, 11.83 and 22.68 Bq/kg, 10.7 and 25.02 Bq/kg, 222.89 and 535.07 Bq/kg and 0.14 and 2.8 Bq/kg, respectively. 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. PMID:22717321

  1. Validation of MCNP with X6.XS cross-section set on the SUN Sparc Station 1+ computer for nominally 5 weight percent {sup 235}U enriched uranium systems

    SciTech Connect

    Lewis, K.D. |

    1994-09-01

    The national Atomic Vapor Laser Isotope Separation (AVLIS) project has conducted extensive nuclear criticality safety analyses both in the design of Uranium Demonstration System (UDS) equipment and in AVLIS plant design/plant deployment activities. Currently, the design limit of an AVLIS plant calls for uranium product enriched in {sup 235}U to 5 wt %. Since an objective of an AVLIS plant is to deliver its product in a form readily usable by customers, uranium enriched in {sup 235}U will appear in a variety of forms, including metallic; as oxides, e.g., UO{sub 2}, UO{sub 3}; as fluorides, e.g., UF{sub 6}, UF{sub 4}, UO{sub 2}F{sub 2}; as nitrates or nitrides, e.g., UO{sub 2} (NO{sub 3}){sub 2}; and perhaps as uranium salts mixed with hydrocarbons such as oil. A wide range of neutron moderation levels, ranging from zero to optimal, and beyond can also be anticipated in an AVLIS plant, because of decontamination and cleaning activities and other wet chemistry processes that may be required.

  2. 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. PMID:26490904

  3. 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.

  4. 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.

  5. Use of {sup 59}Ni, {sup 99}Tc, and {sup 236}U to monitor the release of radionuclides from objects containing spent nuclear fuel dumped in the Kara Sea

    SciTech Connect

    Mount, M.E.; Layton, D.W.; Lynn, N.M.; Hamilton, T.F.

    1998-04-01

    Between 1965 and 1981, five objects - six naval reactor pressure vessels (RPVs) from four former Soviet Union submarines and a special containers from the icebreaker Lenin, each of which contained damaged spent nuclear fuel (SNF) - were dumped in a variety of containments, using a number of sealing methods, at four sites in the Kara Sea. All objects were dumped at sites that varied in depth from 12 to 300 m. This paper examines the use of the long-lived radionuclides {sup 59}Ni, {sup 99}Tc, and {sup 236}U encased within these objects to monitor the breakdown of the containments due to corrosion. Included are discussions of the radionuclide inventory and their release rate model, the estimated radionuclide mass in a typical seawater sample, and the potential for radionuclide measurement via Accelerator Mass Spectrometry (AMS).

  6. Concentration and characteristics of depleted uranium in biological and water samples collected in Bosnia and Herzegovina.

    PubMed

    Jia, Guogang; Belli, Maria; Sansone, Umberto; Rosamilia, Silvia; Gaudino, Stefania

    2006-01-01

    During Balkan conflicts in 1994-1995, depleted uranium (DU) ordnance was employed and was left in the battlefield. Health concern is related to the risk arising from contamination of the environment with DU penetrators and dust. In order to evaluate the impact of DU on the environment and population in Bosnia and Herzegovina, radiological survey of DU in biological and water samples were carried out over the period 12-24 October 2002. The uranium isotopic concentrations in biological samples collected in Bosnia and Herzegovina, mainly lichens, mosses and barks, were found to be in the range of 0.27-35.7 Bq kg(-1) for (238)U, 0.24-16.8 Bq kg(-1) for (234)U, and 0.02-1.11 Bq kg(-1) for (235)U, showing uranium levels to be higher than in the samples collected at the control site. Moreover, the (236)U in some of the samples was detectable. The isotopic ratios of (234)U/(238)U showed DU to be detectable in many biological samples at most sites examined, but in very low levels. The presence of DU in the biological samples was as a result of DU contamination in air. The uranium concentrations in water samples collected in Bosnia and Herzegovina were found to be in the range of 0.27-16.2 m Bq l(-1) for (238)U, 0.41-15.6 m Bq l(-1) for (234)U and 0.012-0.695 m Bq l(-1) for (235)U, and two water samples were observed to be DU positive; these values are much lower than those in mineral water found in central Italy and below the WHO guideline for public drinking water. From radiotoxicological point of view, at this moment there is no significant radiological risk related to these investigated sites in terms of possible DU contamination of water and/or plants. PMID:16806612

  7. 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.

  8. 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

  9. Dynamics of melt generation beneath mid-ocean ridge axes: Theoretical analysis based on [sup 238]U-[sup 230]Th-[sup 226]Ra and [sup 235]U-[sup 231]Pa disequilibria

    SciTech Connect

    Zhenwei Qin )

    1993-04-01

    Although slow melting favors the generation of basaltic melt from a mantle matrix with large radioactive disequilibrium between two actinide nuclides (McKenzie, 1985a), it results in long residence time in a magma chamber, during which the disequilibrium may be removed. An equilibrium melting model modified after McKenzie (1985a) is presented here which suggests that, for a given actinide parent-daughter pair, there exists a specific melting rate at which disequilibrium between these two nuclides reaches its maximum. This melting rate depends on the decay constant of the daughter nuclide concerned and the magma chamber volume scaled to that of its source. For a given scaled chamber size, large radioactive disequilibrium between two actinide nuclides in basalts will be observed if the melting rate is such that the residence time of the magma in the chamber is comparable to the mean life of the daughter nuclide. With a chamber size 1% in volume of the melting source, the melting rates at which maximum disequilibrium in basalts is obtained are 10[sup [minus]7], 2 [times] 10[sup [minus]7], and 3 [times] 10[sup [minus]6] y[sup [minus]1], respectively for [sup 238]U-[sup 230]Th, [sup 235]U-[sup 231]Pa, and [sup 230]Th-[sup 226]Ra. This implies that, while large disequilibrium between [sup 238]U-[sup 230]Th and between [sup 235]U-[sup 231]Pa may occur together, large [sup 230]Th-[sup 226]Ra disequilibrium will not coexist with large [sup 238]U-[sup 230]Th disequilibrium, consistent with some observations. The active mantle melting zone which supplies melt to a ridge axis is inferred to be only about 10 km thick and 50 km wide. The fraction of melt present in such a mantle source at any time is about 0.01 and 0.04, respectively, if melting rate is 10[sup [minus]7] and 10[sup [minus]6] y[sup [minus]1]. The corresponding residence time of the residual melt in the matrix is 10[sup 5] and 4 [times] 10[sup 4] y. 27 refs., 3 figs.

  10. Absolute photofission cross section of sup 197 Au, @Pb, sup 209 Bi, sup 232 Th, sup 238 U, and sup 235 U nuclei by 69-MeV monochromatic and polarized photons

    SciTech Connect

    Martins, J.B.; Moreira, E.L.; Tavares, O.A.P.; Vieira, J.L. Centro Brasileiro de Pesquisas Fisicas-CBPF, Rua Dr. Xavier Sigaud 150, 22290 Rio de Janeiro-RJ, ); Casano, L.; D'Angelo, A.; Schaerf, C. Istituto Nazionale di Fisica Nucleare-INFN, Sezione di Roma 2, Roma, ); Terranova, M.L. Istituto Nazionale di Fisica Nucleare-INFN, Sezione di Roma 2, Roma, Italy); Babusci, D. ); Girolami, B. Istituto Nazionale di Fisica Nuclea

    1991-07-01

    Absolute cross-section measurements for the photofission reactions of {sup 197}Au, {sup nat}Pb, {sup 209}Bi, {sup 232}Th, {sup 238}U, and {sup 235}U nuclei have been performed at an incident photon energy of 69 MeV using monochromatic and polarized photon beams and dielectric fission-track detectors. Nuclear fissility values have been obtained and results are in agreement with those from other laboratories, although in some cases discrepancies are observed between one other. For nuclei in the region of the actinides the fissility result is {approx gt}0.4, while for Au, Pb, and Bi nuclei it only is {similar to}10{sup {minus}3}--10{sup {minus}2}. Results have been interpreted in terms of the primary Levinger's quasideuteron nuclear photoabsorption followed by a mechanism of evaporation-fission competition for the excited nuclei. Shell effects have been taken into account, and they are clearly manifested when fissility is evaluated. The influence of photon polarization on photofission of {sup 238}U also has been investigated, and results have shown isotropy in the fragment azimuthal distribution.

  11. 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.

  12. Ultratrace uranium fingerprinting with isotope selective laser ionization spectrometry.

    PubMed

    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 for ultratrace measurement of the minor isotopes (234)U, (235)U, and (236)U with respect to (238)U. The inherent isotopic selectivity of three-step excitation with single-mode continuous wave lasers results in measurement of the minor isotopes at relative abundances below 1 ppm and is not limited by isobaric interferences such as (235)UH(+) during measurement of (236)U. This relative abundance limit is attained 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 microg 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. PMID:18613650

  13. 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.

  14. 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.

  15. 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.

  16. Uranium isotope measurements by quadrupole ICP-MS for process monitoring of enrichment

    SciTech Connect

    Policke, T.A.; Bolin, R.N.; Harris, T.L.

    1998-12-31

    Historically, uranium isotopic ratio measurements in the nuclear industry have been performed using Thermal Ionization Mass Spectrometry (TIMS); primarily due to the high level of precision that can be achieved. TIMS analysis, however, requires sample purification and intricate sample loading. Quadrupole (low resolution, single detector) inductively coupled plasma--mass spectrometry, Q-ICP-MS, overcomes these disadvantages and is a cost-effective alternative, i.e., in terms of initial capital, maintenance, and operating costs. This paper presents a simple, single standard approach for measuring uranium isotope content in various solid and liquid nuclear materials along with some comparison data of Q-ICP-MS and TIMS. Intensity ratios of {sup 234}U, {sup 235}U, {sup 236}U, and {sup 238}U to total U intensity are produced, providing the enrichment level or percent {sup 235}U. A detailed description of the instrument and data collection parameters are also provided. Optimal precision and accuracy are achieved through the use of a single standard which is closely matched to the enrichment and concentration of the samples. Depending upon the standard chosen, enrichments between depleted and 97% can be quantified. Standard deviations for the major uranium isotopes are typically within 0.02 absolute and at least an order of magnitude lower for the minor U isotope abundances.

  17. 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.

  18. 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.

  19. 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.

  20. Determination of (226)Ra, (232)Th, (40)K, (235)U and (238)U activity concentration and public dose assessment in soil samples from bauxite core deposits in Western Cameroon.

    PubMed

    Mekongtso Nguelem, Eric Jilbert; Moyo Ndontchueng, Maurice; Motapon, Ousmanou

    2016-01-01

    Determination of activity concentrations in twenty five (25) soil samples collected from various points in bauxite ore deposit in Menoua Division in Western of Cameroon was done using gamma spectrometry based Broad Energy Germanium (BEGe6530) detector. The average terrestrial radionuclides of (40)K, (226)Ra, (232)Th, (235)U and (238)U were measured as 671 ± 272, 125 ± 58, 157 ± 67, 6 ± 3 and 99 ± 69 Bq kg(-1), respectively. The observed activity concentrations of radionuclides were compared with other published values in the world. The outdoor absorbed dose rate in air varied from 96.1 to 321.2 nGy h(-1) with an average of 188.2 ± 59.4 nGy h(-1). The external annual effective dose rate and external hazard index were estimated as 0.23 ± 0.07 mSv year(-1) for outdoor, 0.92 ± 0.29 mSv year(-1) for indoor and 1.13 for the external hazard index, respectively. These radiological safe parameters were relatively higher than the recommended safe limits of UNSCEAR. Consequently, using of soil as building material might lead to an increase the external exposure to natural radioactivity and future applications research need to be conducted to have a global view of radioactivity level in the area before any undergoing bauxite ore exploitation. PMID:27536536

  1. Evaluating the status of uranium isotope ratio measurements using an inter-laboratory comparison campaign

    NASA Astrophysics Data System (ADS)

    Richter, S.; Alonso, A.; Truyens, J.; Kühn, H.; Verbruggen, A.; Wellum, R.

    2007-07-01

    The REIMEP 18 (Regular European Inter-laboratory Measurement Evaluation Programme) campaign for the measurement isotopic ratios of uranium in nitric acid solution was completed in December 2006. The task for all participating laboratories was to measure the uranium isotopic composition of four uranium samples ranging from depleted to slightly enriched uranium. With 71 participating laboratories REIMEP 18 has become the largest nuclear isotopic measurement campaign organized by IRMM so far. Participation in this kind of measurement campaign is an integral part of the external quality control required for nuclear safeguards laboratories worldwide. For the first time also a significant number of academic laboratories, mainly from the geochemistry area was included. Certification measurements were carried out at IRMM using state-of-the-art mass spectrometric methodology. A MAT511 UF6-gas source mass spectrometer (GSMS) was used to determine the n(235U)/n(238U) ratios and a TRITON thermal-ionization mass-spectrometer (TIMS) for the minor isotope ratios n(234U)/n(238U) and n(236U)/n(238U). Verification measurements on ampouled samples were performed successfully prior to sample shipping and showed good agreement with the certified ratios. The results of the REIMEP 18 campaign confirm in general the excellent capability of nuclear safeguards and scientific laboratories in measuring isotopic abundances of uranium, although some problems were discovered for the measurements of the minor isotope ratios n(234U)/n(238U) and n(236U)/n(238U) and the calculation of measurement uncertainties for isotope ratios in general. This paper describes the outcome of the REIMEP 18 campaign. It includes a graphical evaluation and discussion of the results, an evaluation of the applied measurement and calibration techniques and a discussion of conclusions and actions to be taken.

  2. 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

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

    DOE PAGESBeta

    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.; et al

    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

  4. 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

  5. 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

  6. Optimized Chemical Separation and Measurement by TE TIMS Using Carburized Filaments for Uranium Isotope Ratio Measurements Applied to Plutonium Chronometry.

    PubMed

    Sturm, Monika; Richter, Stephan; Aregbe, Yetunde; Wellum, Roger; Prohaska, Thomas

    2016-06-21

    An optimized method is described for U/Pu separation and subsequent measurement of the amount contents of uranium isotopes by total evaporation (TE) TIMS with a double filament setup combined with filament carburization for age determination of plutonium samples. The use of carburized filaments improved the signal behavior for total evaporation TIMS measurements of uranium. Elevated uranium ion formation by passive heating during rhenium signal optimization at the start of the total evaporation measurement procedure was found to be a result from byproducts of the separation procedure deposited on the filament. This was avoided using carburized filaments. Hence, loss of sample before the actual TE data acquisition was prevented, and automated measurement sequences could be accomplished. Furthermore, separation of residual plutonium in the separated uranium fraction was achieved directly on the filament by use of the carburized filaments. Although the analytical approach was originally tailored to achieve reliable results only for the (238)Pu/(234)U, (239)Pu/(235)U, and (240)Pu/(236)U chronometers, the optimization of the procedure additionally allowed the use of the (242)Pu/(238)U isotope amount ratio as a highly sensitive indicator for residual uranium present in the sample, which is not of radiogenic origin. The sample preparation method described in this article has been successfully applied for the age determination of CRM NBS 947 and other sulfate and oxide plutonium samples. PMID:27240571

  7. 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

  8. Radiogenic isotopic approaches for quantifying radionuclide transport (Invited)

    NASA Astrophysics Data System (ADS)

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

    2009-12-01

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

  9. Report on 238Pu(n,x) surrogate cross section measurement

    SciTech Connect

    Burke, J T; Ressler, J J; Henderson, R A; Scielzo, N D; Escher, J E; Thompson, I J; Gostic, J; Bleuel, D; Weideking, M; Bernstein, L A

    2010-03-31

    The goal of this year's effort is to measure the {sup 238}Pu(n,f) and {sup 238}Pu(n,2n) cross section from 100 keV to 20 MeV. We designed a surrogate experiment that used the reaction {sup 239}Pu(a,a{prime}x) as a surrogate for {sup 238}Pu(n,x). The experiment was conducted using the STARS/LIBERACE experimental facility located at the 88 Inch Cyclotron at Lawrence Berkeley National Laboratory in January 2010. A description of the experiment and status of the data analysis is given. In order to obtain a reliable {sup 238}Pu(n,x) cross section we designed the experiment using the surrogate ratio technique. This technique allows one to measure a desired, unknown, cross section relative to a known cross section. In the present example, the {sup 238}Pu(n,x) cross section of interest is determined relative to the known {sup 235}U(n,x) cross section. To increase confidence in the results, and to reduce overall uncertainties, we are also determining the {sup 238}Pu(n,x) cross section relative to the known {sup 234}U(n,x) cross section. The compound nuclei of interest for this experiment were produced using inelastic alpha scattering. For example, {sup 236}U(a,a{prime}x) served as a surrogate for {sup 235}U(n,x); analogous reactions were considered for the other cross sections. Surrogate experiments determine the probabilities for the decay of the compound nuclei into the various channels of interest (fission, gamma decay) by measuring particle-fission (p-f) or particle?gamma (p?g) reaction spectra. By comparing the decay probabilities associated with the unknown cross section to that of a known cross section it is possible to obtain the ratio of these cross sections and thus determine the unknown, desired cross section.

  10. 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.

  11. The Effect of Redox Mechanisms on the Fractionation of Uranium `Stable' Isotopes

    NASA Astrophysics Data System (ADS)

    Kaltenbach, A.; Stirling, C. H.; Porcelli, D.; Hilton, D. R.; Kulongoski, J. T.

    2010-12-01

    Uranium is the heaviest naturally occurring element. It consists of three natural isotopes, 238U, 235U and 234U and has four oxidation states, U(III)-U(VI), of which only U(IV) and U(VI) are common. In the oxidized, hexavalent condition, U(VI) exists as uranyl ion (UO22+), which forms soluble, non-reactive complexes with carbonates. In the reduced condition, tetravalent U(IV) forms immobile minerals with hydroxides, fluorides and phosphates that are removed from the water column. In the recent years, isotopic fractionation between 235U and 238U has been detected in a range of terrestrial environments. Changes to U concentrations in natural waters occur due to biological uptake, adsorption/desorption to/from particulates and surfaces, diffusion into sediments, and chemically and biologically induced redox mechanisms (Swarzenski et al., 1999, Mar. Chem. 67, 181). The largest isotopic shifts evidently occur during the reduction of U(VI) to U(IV) in waters, during which precipitation changes the dissolved U concentration. However, the exact mechanisms controlling 235U/238U fractionation remain unclear. Some results implicate mass-dependent zero-point energy effects (preferential removal of 235U over 238U) (Rademacher et al., 2006, Environ. Sci. Technol. 40, 6943) as the main cause for the isotopic variations measured, while others suggest volume-dependent nuclear field shift effects (preferential removal of 238U over 235U) (Weyer et al., 2008, GCA 72, 345, Bopp et al., 2010, Environ. Sci. Technol. 44, 5927), which are predicted to be of the opposite sign and up to three times larger than mass-dependent effects. In this study, profiles of two different water masses were examined for their uranium concentration and their 235U/238U isotopic composition to determine the magnitude of the natural isotopic shifts as well as their origins. One set of samples was collected from a 160 m depth profile in the Framvaren Fjord, an anoxic basin. In this basin, the biogeochemical

  12. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2006-12-01

    The U.S. Geological Survey (USGS) Yucca Mountain Project Branch laboratory in Denver, Colorado, conducts routine high-precision isotope analyses of uranium (U) and thorium (Th) using thermal ionization mass- spectrometry (TIMS). The measurements are conducted by a ThermoFinnigan Triton\\texttrademark equipped with a Faraday multi-collector system and an energy filter in front of an active-film-type secondary electron multiplier (SEM). The abundance sensitivity of the instrument (signal at mass 237 over 238U in natural U) with the energy filter is about 15 ppb and peak tails are reduced by a factor of about 100 relative to the Faraday cup measurements. Since instrument installation in April 2004, more than 500 rock and water samples have been analyzed in support of isotope-geochemical studies for the U.S. Department of Energy`s Yucca Mountain Project. Isotope ratios of sub-nanogram to microgram U and Th samples are measured on graphite-coated single- filament and double-filament assemblies using zone-refined rhenium filaments. Ion beams less than 5 mV are measured with the SEM, which is corrected for non-linearity on the basis of measurements of NIST U-500 and 4321B standards with ion beams ranging from 0.01 to 8 mV. Inter-calibration between the SEM and the Faraday multi-collector is performed for every mass cycle using a 5 mV beam switched between Faraday cup and SEM (bridging technique), because SEM-Faraday inter-calibrations prior to the measurement failed to produce acceptable results. Either natural (^{235}U) or artificial (^{236}U, ^{229}Th) isotopes were used for the bridging. Separate runs are conducted for minor isotopes using SEM only. These techniques result in high within-run precisions of less than 0.1 to 0.2 percent for 234U/238U and 0.2 to 0.5 percent for 230Th/238U. The performance of the instrument is monitored using several U and Th isotope standards. The mean measured 234U/238U in NIST SRM 4321B is (52.879±0.004)×10-6 (95 percent confidence, n

  14. 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

  15. 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.

  16. 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. PMID:24621142

  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. Uranium-series dating of lacustrine limestones from pan deposits with final Acheulian assemblage at Rooidam, Kimberley district, South Africa

    USGS Publications Warehouse

    Szabo, B. J.; Butzer, K.W.

    1979-01-01

    Lacustrine limestone samples from sedimentary pan deposits at Rooidam, near Kimberley, South Africa, that contain late Acheulian (Fauresmith) artifacts have been dated by 230Th 234U and 231Pa 235U methods. Results indicate a minimum age of about 200,000 yr B.P. for the terminal Acheulian in the interior of South Africa. ?? 1979.

  19. Rapid U separation and its precise isotopic measurements using ICP-QMS

    NASA Astrophysics Data System (ADS)

    Douville, E.; Salle, E.; Gourgiotis, A.; Ayrault, S.; Frank, N.

    2007-12-01

    Here we present a largely simplified analytical separation technique for U from marin carbonates and sediments and U isotopic measurements obtained by inductively coupled plasma-source quadrupole mass spectrometer (ICP-QMS) Xseries II - Thermo Scientific. The separation of U is done from dissolved carbonates and sediments using a single ion exchange column packed with ~500 μg of UTEVA resin from EICHROM industries. The column is pre-cleaned and loaded by several rinses of MilliQ water and 3N HNO3. Then earth alkali, transition metals and lanthanides are eluted quantitatively using 3N HNO3. Pure Th and U solutions are then successively extracted from the column using 3N HCl and 1N HCl at ~100% yield. U solutions at ~25-50 ppb were injected into the ICP-QMS at conventional sample flow rates of approximately 1ml/minute, without particular injection systems such as a desolvator or μ - nebuliser. 30 scans with 180 sweeps and a dwell time of 50 ms per isotope were used to collect 233U, 234U, 235U and 236U on an electron multiplier. Baseline sensitivity was followed on mass 228 with <1cps at ~ 1000cps on mass 234. Then, mass discrimination was corrected using the 233U/236U spike of known isotopic ratio and HU1 reference solutions were used to test the reproducibility and to correct drifts using standard - sample bracketing. Overall ICPMS analyses yield a stunning reproducibility of <0.4 % at 2 σ, which is close to the one obtained by conventional TIMS instruments ~0.2-0.4 %. We have applied this technique to organic rich sediments and marine carbonate samples previously measured by TIMS and found a perfect agreement for both U concentration and its isotopic composition. This rapid and effective chemical purification and isotopic measurement of U allows to process more than 20 samples a day allowing to investigate large numbers of natural samples for weathering, tracer and geochronological studies.

  20. 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

  1. Search for the gamma-branch of the shape isomers of separated U isotopes using muon for nuclide excitation

    SciTech Connect

    Mireshghi, A.

    1982-12-01

    We have searched for back-decay gamma rays from the shape isomeric states in /sup 235/U, /sup 236/U, and /sup 238/U possibly excited in muon radiationless transition. The energies and intensities of gamma rays following muon atomic capture were measured as a function of time after muon stopping. Background was suppressed by requiring that the candidate gamma ray be followed by another gamma ray (..mu..-capture gamma ray). The prompt gamma-ray spectra included the U-muonic x rays. The measured /sup 235/U and /sup 238/U x-ray energies were in good agreement with previously reported results. The x-ray spectrum from /sup 236/U has not been previously reported. The /sup 236/U spectrum is very similar to that of /sup 238/U, except that the K x-rays exhibit an isotope shift of approximately 20 keV, the /sup 236/U energies being higher. In the analysis of the delayed spectra of /sup 236/U and /sup 238/U using the GAMANL peak searching program, and with an effective lower-limit detection efficiency of .15% per stopping muon, no candidate gamma rays for the back decay transitions from the shape isomeric state were observed.

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

    DOE PAGESBeta

    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.

  3. Difficulties in using 234u/238u ratios to detect enriched or depleted uranium.

    PubMed

    Fleischer, Robert L

    2008-03-01

    Uranium that is highly enriched in U (HEU) is also often also enriched in U because it too is a lower-mass isotope than U and thus its concentration would be preferentially increased in any mass-sensitive enrichment process. Thus the ratio U/U might be regarded as a surrogate for U/U-the usual measure of enrichment. For this reason it has been suggested that U/U measurements be used to detect contamination by HEU. The purpose of this Note is to point out that, because of alpha-recoil effects, U/U varies widely in natural systems, and for this reason it would not be a dependable indicator of the presence of HEU. The same variations would cause U/U ratios to be doubtful indicators of depleted uranium. PMID:18301103

  4. A more accurate and penetrating method to measure the enrichment and mass of UF6 storage containers using passive neutron self-interrogation

    SciTech Connect

    Menlove, Howard O; Swinhoe, Martyn T; Miller, Karen A

    2010-01-01

    This paper describes an unattended mode neutron measurement that can provide the enrichment of the uranium in UF{sub 6} cylinders. The new passive neutron measurement provides better penetration into the uranium mass than prior gamma-ray enrichment measurement methods. The Passive Neutron Enrichment Monitor (PNEM) provides a new measurement technique that uses passive neutron totals and coincidence counting together with neutron self-interrogation to measure the enrichment in the cylinders. The measurement uses the neutron rates from two detector pods. One of the pods has a bare polyethylene surface next to the cylinder and the other polyethylene surface is covered with Cd to prevent thermal neutrons from returning to the cylinder. The primary neutron source from the enriched UF{sub 6} is the alpha-particle decay from the {sub 234}U that interacts with the fluorine to produce random neutrons. The singles neutron counting rate is dominated by the {sub 234}U neutrons with a minor contribution from the induced fissions in the {sub 235}U. However, the doubles counting rate comes primarily from the induced fissions (i.e., multiplication) in the {sub 235}U in enriched uranium. The PNEM concept makes use of the passive neutrons that are initially produced from the {sub 234}U reactions that track the {sub 235}U enrichment during the enrichment process. The induced fission reactions from the thermal-neutron albedo are all from the {sub 235}U and provide a measurement of the {sub 235}U. The Cd ratio has the desirable feature that all of the thermal-neutron-induced fissions in {sub 235}U are independent of the original neutron source. Thus, the ratio is independent of the uranium age, purity, and prior reactor history.

  5. Stand Up of Uranium Capability for Swipe Analysis

    SciTech Connect

    Matthew Watrous; Anthony Appelhans; Robert Hague; Tracy Houghton; John Olson

    2013-11-01

    swipe material at nanogram (~2 x 10-9 g) levels for a typical sample, a level easily detected with ICPMS. The abundance of the isotopes ranges over 4 orders of magnitude for the naturally occurring 234U, 235U and 238U and a goal was set to be able to detect the presence of 236U at 6 orders of magnitude lower than the 238U. The 236U measurement is particularly important because the presence of 236U is a strong indicator that the uranium as been in a nuclear reactor. To demonstrate these capabilities the following sample types were used: blank swipe material, blank process reagents, swipe material spiked with a natural abundance U isotope standard, swipe material spiked with an environmental standard (Columbia River sediment), and swipes taken at various locations within the processing laboratories and the INL environment. This report summarizes the method used to extract the U from the swipe material, the ICPMS analyses that demonstrate the limit of detection (LOD) and the limit of quantification (LOQ) for the U isotopes of interest, the precision of the measured isotope ratios and the dependence of precision on the quantity of U present, and the method proposed to determine if an off-normal ratio is statistically relevant.

  6. Use of uranium isotopes as a temporal and spatial tracer of nuclear contamination in the environment.

    PubMed

    Tortorello, R; Widom, E; Renwick, W H

    2013-10-01

    The Fernald Feed Materials Production Center (FFMPC) was established in 1951 to process natural uranium (U) ore, enriched uranium (EU) and depleted uranium (DU). This study tests the utility of U isotopic ratios in sediment cores and lichens as indicators of the aerial extent, degree and timing of anthropogenic U contamination, using the FFMPC as a test case. An 80-cm-long sediment core was extracted from an impoundment located approximately 6.7 km southwest of the FFMPC. Elemental concentrations of thorium (2.7-6.2 μg g(-1)) and U (0.33-1.33 μg g(-1)) as well as major and minor U isotopes were analyzed in the core. The lack of measurable (137)Cs in the deepest sample as well as a natural (235)U/(238)U signature and no measurable (236)U, are consistent with pre-FFMPC activity. Anomalously elevated U with respect to Th concentrations occur in seven consecutive samples immediately above the base of the core (62-76 cm depth). Samples with elevated U concentrations also show variable (235)U/(238)U (0.00645-0.00748), and all contain measurable (236)U ((236)U/(238)U = 2.1 × 10(-6)-3.6 × 10(-5)). Correspondence between the known releases of U dust from the FFMPC through time and variations in sediment core U concentrations, (235)U/(238)U and (236)U/(238)U ratios provide evidence for distinct releases of both DU and EU. Furthermore, these relationships demonstrate that the sediment core serves as a robust archive of past environmental U contamination events. Samples in the upper 40 cm display natural (235)U/(238)U, but measurable (236)U/(238)U ((236)U/(238)U = 5.68 × 10(-6)-1.43 × 10(-5)), further indicating the continued presence of anthropogenic U in present-day sediment. Three local lichen samples were also analyzed, and all display either EU or DU signatures coupled with elevated (236)U/(238)U, recording airborne U contamination from the FFMPC. PMID:23871969

  7. Fission mode fluctuations in the resonances of 235U(n,f)

    NASA Astrophysics Data System (ADS)

    Hambsch, F. J.; Knitter, H. H.; Budtz-Jørgensen, C.; Theobald, J. P.

    1989-01-01

    Fission fragment mass- and total kinetic energy distributions were measured for single, isolated resonances and neutron energy bins covering the incident neutron energy range from 0.006 eV to 130 eV. The measurements were performed at the Geel Electron Linear Accelerator (GELINA) of the European Communities using a Frisch-gridded ionization chamber. Fluctuations of the fission fragment mass distributions as function of resonance energy were observed, which are correlated with fluctuations of the reaction Q-value and with the measured total kinetic energy averaged over all fragments. In the resonance region the fluctuations in from resonance to resonance are observed with amplitudes up to about 450 keV. The correlations between the mass-distribution fluctuations and other parameters like spin J, spin orientation quantum number K, angular distribution fluctuations and the fluctuations of the average number of neutrons emitted in fission, overlinev, are evaluated and discussed. An interpretation of the overlinev- fluctuations observed in other experiments is given in terms of the mass distribution fluctuations. The fluctuations of the mass-distribution parameters and of the total kinetic energy distributions as function of mass are viewed in the frame of the fission channel model of Bohr and Wheeler and of the recent multi-fission mode random neck-rupture model of Brosa, Grossmann and Müller.

  8. 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.

  9. 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.

  10. Inorganic, radioisotopic and organic analysis of 241-AP-101 tank waste

    SciTech Connect

    SK Fiskum; PR Bredt; JA Campbell; LR Greenwood; OT Farmer; GJ Lumetta; GM Mong; RT Ratner; CZ Soderquist; RG Swoboda; MW Urie; JJ Wagner

    2000-06-28

    Battelle received five samples from Hanford waste tank 241-AP-101, taken at five different depths within the tank. No visible solids or organic layer were observed in the individual samples. Individual sample densities were measured, then the five samples were mixed together to provide a single composite. The composite was homogenized and representative sub-samples taken for inorganic, radioisotopic, and organic analysis. All analyses were performed on triplicate sub-samples of the composite material. The sample composite did not contain visible solids or an organic layer. A subsample held at 10 C for seven days formed no visible solids. The characterization of the 241-AP-101 composite samples included: (1) Inductively-coupled plasma spectrometry for Ag, Al, Ba, Bi, Ca, Cd, Cr, Cu, Fe, K, La, Mg, Mn, Na, Nd, Ni, P, Pb, Pd, Ru, Rh, Si, Sr, Ti, U, Zn, and Zr (Note: Although not specified in the test plan, As, B, Be, Co, Li, Mo, Sb, Se, Sn, Tl, V, W, and Y were also measured and reported for information only) (2) Radioisotopic analyses for total alpha and total beta activities, {sup 3}H, {sup 14}C, {sup 60}Co, {sup 79}Se, {sup 90}Sr, {sup 99}Tc as pertechnetate, {sup 106}Ru/Rh, {sup 125}Sb, {sup 134}Cs, {sup 137}Cs, {sup 152}Eu, {sup 154}Eu, {sup 155}Eu, {sup 238}Pu, {sup 239+240}Pu, {sup 241}Am, {sup 242}Cm, and {sup 243+244}Cm; (3) Inductively-coupled plasma mass spectrometry for {sup 237}Np, {sup 239}Pu, {sup 240}Pu, {sup 99}Tc, {sup 126}Sn, {sup 129}I, {sup 231}Pa, {sup 233}U, {sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U, {sup 241}AMU, {sup 242}AMU, {sup 243}AMU, As, B, Be, Ce, Co, Cs, Eu, I, Li, Mo, Pr, Rb, Sb, Se, Ta, Te, Th, Tl, V, and W; (4) total U by kinetic phosphorescence analysis; (5) Ion chromatography for Cl, F, NO{sub 2}, NO{sub 3}, PO{sub 4}, SO{sub 4}, acetate, formate, oxalate, and citrate; (6) Density, inorganic carbon and organic carbon by two different methods, mercury, free hydroxide, ammonia, and cyanide. The 241-AP-101 composite met all

  11. 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.

  12. Topical report on actinide-only burnup credit for PWR spent nuclear fuel packages. Revision 1

    SciTech Connect

    None, None

    1997-04-01

    A methodology for performing and applying nuclear criticality safety calculations, for PWR spent nuclear fuel (SNF) packages with actinide-only burnup credit, is described. The changes in the U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, and Am-241 concentration with burnup are used in burnup credit criticality analyses. No credit for fission product neutron absorbers is taken. The methodology consists of five major steps. (1) Validate a computer code system to calculate isotopic concentrations of SNF created during burnup in the reactor core and subsequent decay. A set of chemical assay benchmarks is presented for this purpose as well as a method for assessing the calculational bias and uncertainty, and conservative correction factors for each isotope. (2) Validate a computer code system to predict the subcritical multiplication factor, k{sub eff}, of a spent nuclear fuel package. Fifty-seven UO{sub 2}, UO{sub 2}/Gd{sub 2}O{sub 3}, and UO{sub 2}/PuO{sub 2} critical experiments have been selected to cover anticipated conditions of SNF. The method uses an upper safety limit on k{sub eff} (which can be a function of the trending parameters) such that the biased k{sub eff}, when increased for the uncertainty is less than 0.95. (3) Establish bounding conditions for the isotopic concentration and criticality calculations. Three bounding axial profiles have been established to assure the ''end effect'' is accounted for conservatively. (4) Use the validated codes and bounding conditions to generate package loading criteria (burnup credit loading curves). Burnup credit loading curves show the minimum burnup required for a given initial enrichment. The utility burnup record is compared to this requirement after the utility accounts for the uncertainty in its record. Separate curves may be generated for each assembly design, various minimum cooling times and burnable absorber histories. (5) Verify that SNF assemblies meet the package loading criteria

  13. Undiagnosed illnesses and radioactive warfare.

    PubMed

    Duraković, Asaf

    2003-10-01

    The internal contamination with depleted uranium (DU) isotopes was detected in British, Canadian, and United States Gulf War veterans as late as nine years after inhalational exposure to radioactive dust in the Persian Gulf War I. DU isotopes were also identified in a Canadian veteran's autopsy samples of lung, liver, kidney, and bone. In soil samples from Kosovo, hundreds of particles, mostly less than 5 microm in size, were found in milligram quantities. Gulf War I in 1991 resulted in 350 metric tons of DU deposited in the environment and 3-6 million grams of DU aerosol released into the atmosphere. Its legacy, Gulf War disease, is a complex, progressive, incapacitating multiorgan system disorder. The symptoms include incapacitating fatigue, musculoskeletel and joint pains, headaches, neuropsychiatric disorders, affect changes, confusion, visual problems, changes of gait, loss of memory, lymphadenopathies, respiratory impairment, impotence, and urinary tract morphological and functional alterations. Current understanding of its etiology seems far from being adequate. After the Afghanistan Operation Anaconda (2002), our team studied the population of Jalalabad, Spin Gar, Tora Bora, and Kabul areas, and identified civilians with the symptoms similar to those of Gulf War syndrome. Twenty-four-hour urine samples from 8 symptomatic subjects were collected by the following criteria: 1) the onset of symptoms relative to the bombing raids; 2) physical presence in the area of the bombing; and 3) clinical manifestations. Control subjects were selected among the sympotom-free residents in non-targeted areas. All samples were analyzed for the concentration and ratio of four uranium isotopes, (234)U, (235)U, (236)U and (238)U, by using a multicollector, inductively coupled plasma ionization mass spectrometry. The first results from the Jalalabad province revealed urinary excretion of total uranium in all subjects significantly exceeding the values in the nonexposed population

  14. U-Pb systems and U isotopic composition of the sandstone-hosted paleovalley Dybryn uranium deposit, Vitim uranium district, Russia

    NASA Astrophysics Data System (ADS)

    Golubev, V. N.; Chernyshev, I. V.; Chugaev, A. V.; Eremina, A. V.; Baranova, A. N.; Krupskaya, V. V.

    2013-11-01

    The isotopic (U-Pb, 238U-235U, 234U-238U) and chemical study of whole-rock samples and finegrained fractions of rocks in a vertical section of the terrigenous sequence at the Dybryn uranium deposit in the Khiagda ore field shows that a wide U-Pb isotopic age range (26.9-6.5 Ma) is caused by oxidation and disturbance of the U-Pb isotopic system in combination with protracted uranium ore deposition. The oxidation of rocks resulted in the loss of uranium relative to lead and eventually to an overestimated 206Pb/238U age at sites with a low U content. The 238U/235U ratios in the studied samples are within the range of 137.74-137.88. Samples with a high uranium content are characterized by a decreasing 238U/235U ratio with a decrease in 207Pb/235U and 206Pb/238U ages. A nonequilibrium 234U/238U ratio in most studied samples furnishes evidence for young (<1.5 Ma) transformation of the Miocene uranium ore, which is responsible for uranium migration and its redeposition.

  15. 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

  16. Precise and accurate measurement of U and Th isotopes via ICP-MS using a single solution

    NASA Astrophysics Data System (ADS)

    Mertz-Kraus, R.; Sharp, W. D.; Ludwig, K. R.

    2012-04-01

    , allowing the sample's 238U/235U ratio to be measured. In step 3, we monitor peak-tails at half-mass positions (229.5, 231.5, 234.5) and on mass 237 while aspirating sample solution. Tail measurement requires a distinct cup configuration to maintain 238U in the cups; however, no sample is consumed during automated cup reconfiguration. We monitor the accuracy of 234U/238U ratios using CRM 145, which gives a weighted mean atom ratio of (5.2846 ± 0.0029) - 10-5 (all errors 2σ), consistent with published and reference values. The reproducibility of 230Th/238U ratios is monitored using the Schwartzwalder Mine secular-equilibrium standard (SM). We detect no bias in 230Th/238U or 234U/238U ratios measured for SM at beam intensities ranging over a factor of four, consistent with accurate correction for IC yields. Aladdin's cave coral (AC-1) was analyzed to check our ICP-MS method (and the preceding purification by ion exchange) on a carbonate and yields a mean age of 125.43 ± 0.38 ka, in agreement with published values. We are currently applying the method to corals, speleothems, pedogenic coatings, and tufas.

  17. Evaluating the potential of the MegaSIMS for nuclear forensics

    NASA Astrophysics Data System (ADS)

    Boehnke, P.; McKeegan, K. D.; Coath, C. D.; Hutcheon, I. D.; Steele, R. C.; Harrison, M.

    2013-12-01

    Nuclear forensics investigates the illicit movement of nuclear materials. Measurements of uranium isotopic compositions are an important key as they permit provenance tracing and determination of intended use. Traditional secondary ion mass spectrometers (SIMS) are incapable of resolving 235UH from 236U due to the high mass resolving power (MRP ~38,000) needed, significantly limiting their ability to accurately measure 236U/235U, particularly for highly enriched uranium. This limitation can significantly inhibit the ability to establish details about enrichment processes. The MegaSIMS is a unique combination of SIMS and accelerator mass spectrometry (AMS) and allows for molecular interference free measurements, while retaining the spatial resolution and ease of sample preparation common in SIMS analyses. The instrument was primarily designed to measure the oxygen isotope composition of the solar wind [1] and its capability for measuring high mass elements has not been evaluated previously. We evaluated the potential of the MegaSIMS by measuring 236U/235U without hydride interference. While preliminary results show abundance sensitivity of ~E-9 and an MRP of ~1,200 at the high mass side of 238 amu, precision is limited by the detector geometry and slow magnet switching. Future work will include developing electrostatic peak switching as well as refining the measurement precision and abundance sensitivity of the MegaSIMS for nuclear forensics. [1] McKeegan, Kallio, Heber, Jarzebinski, Mao, Coath, Kunihiro, Wiens, Nordholt, Moses Jr., Reisenfeld, Jurewicz, and Burnett, 2011. Science. 332, 1528-1532.

  18. Improving the Sensitivity of Uranium Isotope Ratio Measurements

    NASA Astrophysics Data System (ADS)

    Friedrich, J.; Snow, J.

    2003-12-01

    Accurate and precise measurements of natural and anthropogenic 235/238 U isotope ratios are important for a range of investigations where the amount of sample is extremely restricted and/or the analyte is only present in ultra-trace quantities. Examples include biological, cosmochemical, environmental, geological, and radiological studies. We have developed and validated a novel method using our Nu Instruments Nu Plasma Multi Collector Inductively Coupled Plasma Mass Spectrometer (MC-ICPMS) and a 233U, 236U mixed double spike for the measurement of 235U/238U ratios. Our multi-dynamic technique employs the installed quadrupole zoom optics and fixed positioning of the ion counting detectors such that rather than the commonly used mass dispersion of 1 or 2, we utilize a mass dispersion of 1.5. Using this configuration, we can simultaneously monitor the 235U and 238U ion beams in the first cycle followed by a second cycle that simultaneously monitors the 233U and 236U beams. This innovative approach allows us to correct for the considerable, but consistent, instrumental mass fractionation and ion-counter amplification bias within each sequence. Since we were hesitant to use a U500 (235U, 238U equal atom) solution for spike calibration because of possible enriched U laboratory and instrumentation contamination, we used a U960 (terrestrial 235U/238U) solution for isotopic calibration of the spike. This standardization corrected for the small amounts of 235U and 238U in the spike solution by using a U960 standard solution. With a mean intraday 2-sigma precision of 1.5 permil and an overall 2-sigma precision of 2.25 permil using individual sample sizes of 350 pg (8.8 x10 E11 atoms), we are confident our technique will be useful for identifying U isotopic anomalies present in many sample types.

  19. 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

  20. Subthreshold Photofission of Even-Even Nuclei

    SciTech Connect

    Kadmensky, S.G.; Rodionova, L.V.

    2005-09-01

    Within quantum-mechanical fission theory, the angular distributions of fragments originating from the subthreshold photofission of the even-even nuclei {sup 232}Th, {sup 234}U, {sup 236}U, {sup 238}U, {sup 238}Pu, {sup 240}Pu, and {sup 242}Pu are analyzed for photon energies below 7 MeV. Special features of various fission channels are assessed under the assumption that the fission barrier has a two-humped shape. It is shown that the maximum value of the relative orbital angular momentum L{sub m} of fission fragments can be found upon taking into account deviations from the predictions of A. Bohr's formula for the angular distributions of fission fragments. The result is L{sub m} {approx_equal} 30. The existence of an 'isomeric shelf' for the angular distributions of fragments from {sup 236}U and {sup 238}U photofission in the low-energy region is confirmed.

  1. Isotopic evidence of natural uranium and spent fuel uranium releases into the environment.

    PubMed

    Pourcelot, L; Boulet, B; Le Corre, C; Loyen, J; Fayolle, C; Tournieux, D; Van Hecke, W; Martinez, B; Petit, J

    2011-02-01

    Uranium and plutonium isotopes were measured in soils, sediments and waters in an area subject to the past and present discharges from the uranium conversion plant of Malvési (France). The isotopes (236)U and (239)Pu are well known activation products of uranium and they prove to be powerful tracers of spent fuel releases in soils and sediments. On the other hand (234)U and (238)U activities measured in waters can be used to distinguish between releases and background uranium sources. Such findings contribute to improve the monitoring of the actinides releases by nuclear fuel facilities (mining sites, conversion, enrichment and fuel plants, reprocessing plants). PMID:21132170

  2. Polyatomic interferences on high precision uranium isotope ratio measurements by MC-ICP-MS: Applications to environmental sampling for nuclear safeguards

    DOE PAGESBeta

    Pollington, Anthony D.; Kinman, William S.; Hanson, Susan K.; Steiner, Robert E.

    2015-09-04

    Modern mass spectrometry and separation techniques have made measurement of major uranium isotope ratios a routine task; however accurate and precise measurement of the minor uranium isotopes remains a challenge as sample size decreases. One particular challenge is the presence of isobaric interferences and their impact on the accuracy of minor isotope 234U and 236U measurements. Furthermore, we present techniques used for routine U isotopic analysis of environmental nuclear safeguards samples and evaluate polyatomic interferences that negatively impact accuracy as well as methods to mitigate their impacts.

  3. Improving Precision and Accuracy of Isotope Ratios from Short Transient Laser Ablation-Multicollector-Inductively Coupled Plasma Mass Spectrometry Signals: Application to Micrometer-Size Uranium Particles.

    PubMed

    Claverie, Fanny; Hubert, Amélie; Berail, Sylvain; Donard, Ariane; Pointurier, Fabien; Pécheyran, Christophe

    2016-04-19

    The isotope drift encountered on short transient signals measured by multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) is related to differences in detector time responses. Faraday to Faraday and Faraday to ion counter time lags were determined and corrected using VBA data processing based on the synchronization of the isotope signals. The coefficient of determination of the linear fit between the two isotopes was selected as the best criterion to obtain accurate detector time lag. The procedure was applied to the analysis by laser ablation-MC-ICPMS of micrometer sized uranium particles (1-3.5 μm). Linear regression slope (LRS) (one isotope plotted over the other), point-by-point, and integration methods were tested to calculate the (235)U/(238)U and (234)U/(238)U ratios. Relative internal precisions of 0.86 to 1.7% and 1.2 to 2.4% were obtained for (235)U/(238)U and (234)U/(238)U, respectively, using LRS calculation, time lag, and mass bias corrections. A relative external precision of 2.1% was obtained for (235)U/(238)U ratios with good accuracy (relative difference with respect to the reference value below 1%). PMID:27031645

  4. Initial Report for the Aquifer Background Study: Summary of Uranium and Plutonium Data from INEEL Groundwater Samples

    SciTech Connect

    Robert C. Roback; Don L. Koeppen

    2003-06-01

    As part of the “Aquifer Background Study,” Los Alamos National Laboratory (LANL) under contract with the Idaho National Engineering and Environmental Laboratory (INEEL) has undertaken a study to determine uranium and plutonium abundances and isotopic composition in groundwater samples collected at the INEEL. To date, four samples have been analyzed for uranium and plutonium and an additional nine samples have been analyzed for uranium. It is expected that several more samples will be analyzed for this study. This report summarizes the results from this initial set of samples. Of the 13 samples analyzed for uranium, four samples have 238U/235U ratios that differ from the natural value of 137.88. These four samples and two additional samples also contain 236U at 3-sigma level above detection limits. The presence of 236U and the non-natural 238U/235U ratios unequivocally indicate the presence of anthropic uranium in four of the samples. A small component of anthropic uranium is also present in two additional samples with positive 236U detection but natural 238U/235U isotope ratios. Two of the samples with anthropic uranium, as well as two samples with no detectable anthropic uranium were analyzed for plutonium. No plutonium was detected in these four samples at detection limits of approximately 5E7 239Pu atoms for three of the samples and approximately 1E8 239Pu atoms for the forth sample. These detection limits correspond to (239+240)Pu activity ratios (assuming a 240Pu/239Pu atom ratio of 0.18) of 0.002 and 0.004 pCi/L respectively.

  5. 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.

  6. Evolution of isotopic composition of reprocessed uranium during the multiple recycling in light water reactors with natural uranium feed

    SciTech Connect

    Smirnov, A. Yu. Sulaberidze, G. A.; Alekseev, P. N.; Dudnikov, A. A.; Nevinitsa, V. A. Proselkov, V. N.; Chibinyaev, A. V.

    2012-12-15

    A complex approach based on the consistent modeling of neutron-physics processes and processes of cascade separation of isotopes is applied for analyzing physical problems of the multiple usage of reprocessed uranium in the fuel cycle of light water reactors. A number of scenarios of multiple recycling of reprocessed uranium in light water reactors are considered. In the process, an excess absorption of neutrons by the {sup 236}U isotope is compensated by re-enrichment in the {sup 235}U isotope. Specific consumptions of natural uranium for re-enrichment of the reprocessed uranium depending on the content of the {sup 232}U isotope are obtained.

  7. Determination of Background Uranium Concentration in the Snake River Plain Aquifer under the Idaho National Engineering and Environmental Laboratory's Radioactive Waste Management Complex

    SciTech Connect

    Molly K. Leecaster; L. Don Koeppen; Gail L. Olson

    2003-06-01

    Uranium occurs naturally in the environment and is also a contaminant that is disposed of at the Radioactive Waste Management Complex (RWMC) at the Idaho National Engineering and Environmental Laboratory. To determine whether uranium concentrations in the Snake River Plain Aquifer, which underlies the laboratory, are elevated as a result of migration of anthropogenic uranium from the Subsurface Disposal Area in the RWMC, uranium background concentrations are necessary. Guideline values are calculated for total uranium, 234U, 235U, and 238U from analytical results from up to five datasets. Three of the datasets include results of samples analyzed using isotope dilution thermal ionization mass spectrometry (ID-TIMS) and two of the datasets include results obtained using alpha spectrometry. All samples included in the statistical testing were collected from aquifer monitoring wells located within 10 miles of the RWMC. Results from ID-TIMS and alpha spectrometry are combined when the data are not statistically different. Guideline values for total uranium were calculated using four of the datasets, while guideline values for 234U were calculated using only the alpha spectrometry results (2 datasets). Data from all five datasets were used to calculate 238U guideline values. No limit is calculated for 235U because the ID-TIMS results are not useful for comparison with routine monitoring data, and the alpha spectrometry results are too close to the detection limit to be deemed accurate or reliable for calculating a 235U guideline value. All guideline values presented represent the upper 95% coverage 95% confidence tolerance limits for background concentration. If a future monitoring result is above this guideline, then the exceedance will be noted in the quarterly monitoring report and assessed with respect to other aquifer information. The guidelines (tolerance limits) for total U, 234U, and 238U are 2.75 pCi/L, 1.92 pCi/L, and 0.90 pCi/L, respectively.

  8. Neutron-Induced Fission Measurements at the Dance and Lsds Facilities at Lanl

    NASA Astrophysics Data System (ADS)

    Jandel, M.; Bredeweg, T. A.; Bond, E. M.; Chadwick, M. B.; Couture, A.; O'Donnell, J. M.; Fowler, M. M.; Haight, R. C.; Hayes-Sterbenz, A. C.; Rundberg, R. S.; Rusev, G. Y.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wu, C. Y.; Becker, J. A.; Alexander, C. W.; Belier, G.

    2014-09-01

    New results from neutron-induced fission measurements performed at the Detector for Advanced Neutron Capture Experiments (DANCE) and Lead Slowing Down Spectrometer (LSDS) are presented. New correlated data on promptfission γ-ray (PFG) distributions were measured using the DANCE array for resonant neutron-induced fission of 233U, 235U and 239Pu. The deduced properties of PFG emission are presented using a simple parametrization. An accurate knowledge of fission γ-ray spectra enables us to analyze the isomeric states of 236U created after neutron capture on 235U. We briefly discuss these new results. Finally, we review details and preliminary results of the challenging 237U(n,f) cross section measurement at the LSDS facility.

  9. 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…

  10. Commissioning the NIFFTE Time Projection Chamber: Towards the 238U / 235U (n, f) Cross-section Ratio

    NASA Astrophysics Data System (ADS)

    Meharchand, R.; Asner, D. M.; Baker, R. G.; Bundgaard, J.; Burgett, E.; Cunningham, M.; Deaven, J.; Duke, D. L.; Greife, U.; Grimes, S.; Heffner, M.; Hill, T.; Isenhower, D.; Klay, J. L.; Kleinrath, V.; Kornilov, N.; Laptev, A. B.; Loveland, W.; Massey, T. N.; Qu, H.; Ruz, J.; Sangiorgio, S.; Seilhan, B.; Snyder, L.; Stave, S.; Tatishvili, G.; Thornton, R. T.; Tovesson, F.; Towell, D.; Towell, R. S.; Watson, S.; Wendt, B.; Wood, L.

    2014-05-01

    The Neutron Induced Fission Fragment Tracking Experiment (NIFFTE) collaboration is developing a Time Projection Chamber (TPC) to measure neutron-induced fission cross sections with unprecedented accuracy. Modifying TPC technology for nuclear physics applications is a challenging endeavor, and frequent testing and evaluation is required to ensure that all components are behaving as expected. In-beam tests of the NIFFTE TPC at the Los Alamos Neutron Science Center (LAN-SCE) commenced in 2010. An overview of the NIFFTE TPC experiments performed at LANSCE will be presented, along with preliminary performance results.

  11. 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.

  12. Simultaneous {sup 233}U and{sup 235}U characterization through the assay of delayed neutron temporal behavior

    SciTech Connect

    Sellers, M. T.; Corcoran, E. C.; Kelly, D. G.

    2012-07-01

    Aqueous solutions containing dissolved uranium-233 and uranium-235 were irradiated for 60's in the SLOWPOKE-2 reactor at the Royal Military College of Canada. The temporal behavior of the delayed neutrons produced was recorded by the Facility's Delayed Neutron Counting (DNC) system. The percentage of uranium-233 as a function of total fissile mass present in each sample ranged from 0 to 100% and was predicted by the DNC system with average absolute errors of {+-} 4%. Future work will upgrade the system electronics and software to reduce both uncertainties in timings and electrical noise. Mixture analysis will also be expanded to include plutonium-239 and fissile materials contained in non-aqueous matrices. (authors)

  13. 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

  14. HEU age determination

    SciTech Connect

    Moorthy, A.R.; Kato, W.Y.

    1994-12-31

    A criteria that a sample of highly enriched uranium (HEU) had come from a weapons stockpile and not newly produced in an enrichment plant is to show that the HEU had been produced a significant time in the past. The time since the HEU has produced in an enrichment plant is defined as the age of the HEU in this paper. The HEU age is determined by measuring quantitatively the daughter products {sup 230}Th and {sup 231}Pa of {sup 234}U and {sup 235}U, respectively, by first chemical separation of the thorium and protactinium and then conducting alpha spectrometry of the daughter products.

  15. Desert varnish: potential for age dating via uranium-series isotopes

    SciTech Connect

    Knauss, K.G.; Ku, T.L.

    1980-01-01

    Trace metals and natural radioisotopes are measured in an unusually thick and presumed ancient desert varnish from the Colorado Plateau in Utah. Uranium and thorium concentrations in the sequence: varnish-altered rind-heartrock (Shinarump formation sandstone) indicate that uranium with little accompanying thorium is derived from external sources. The varnish forms a closed system for /sup 230/Th and /sup 231/Pa with equilibrium values for both /sup 230/Th//sup 234/U and /sup 231/Pa//sup 235/U. Selective leaching of the ferromanganese oxides followed by analysis of both the leachate and silicate residue is proposed to allow age determinations.

  16. Desert varnish: potential for age dating via uranium-series isotopes

    SciTech Connect

    Knauss, K.G.; Ku, T.L.

    1980-01-01

    Trace metals and natural radioisotopes are measured in an unusually thick and presumed ancient desert varnish from the Colorado Plateau in Utah. Uranium and thorium concentrations in the sequence: varnish--altered rind--heartrock (Shinarump formation sandstone) indicate that uranium with little accompanying thorium is derived from external sources. The varnish forms a closed system for /sup 230/Th and /sup 231/Pa with equilibrium values for both /sup 230/Th//sup 234/U and /sup 231/Pa//sup 235/U. Selective leaching of the ferromanganese oxides followed by analysis of both the leachate and silicate residue is proposed to allow age determinations.

  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. Neutron-Induced Fission Cross Sections Measurements at n_TOF

    SciTech Connect

    Audouin, L.; Tassan-Got, L.; Isaev, S.; Koehler, Paul Edward; Collaboration, n_TOF

    2008-01-01

    The neutron-induced fission cross sections of {sup 233}U, {sup 234}U, {sup 235}U, {sup 238}U, {sup 232}Th, {sup 237}Np, {sup 209}Bi, {sup nat}Pb have been measured at the n{_}TOF facility at CERN over 9 orders of magnitude in neutron energy using {sup 235}U as a reference. Parallel Plate Avalanche Counters were used to detect both fission fragments in coincidence, thus efficiently discriminating fissions from other reactions. Data benefit from the remarkable energy resolution of the n{_}TOF facility. They are found in overall good agreement with databases and previous measurements, but some clear discrepancies can be put in evidence. These data are the first full coverage of the high-energy region (up to 1 GeV).

  19. 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.

  20. Determining the isotopic compositions of uranium and fission products in radioactive environmental microsamples using laser ablation ICP-MS with multiple ion counters.

    PubMed

    Boulyga, Sergei F; Prohaska, Thomas

    2008-01-01

    This paper presents the application of a multicollector inductively coupled plasma mass spectrometer (MC-ICP-MS)--a Nu Plasma HR--equipped with three ion-counting multipliers and coupled to a laser ablation system (LA) for the rapid and sensitive determination of the 235U/238U, 236U/238U, 145Nd/143Nd, 146Nd/143Nd, 101Ru/(99Ru+99Tc) and 102Ru/(99Ru+99Tc) isotope ratios in microsamples collected in the vicinity of Chernobyl. Microsamples with dimensions ranging from a hundred mum to about 1 mm and with surface alpha activities of 3-38 mBq were first identified using nuclear track radiography. U, Nd and Ru isotope systems were then measured sequentially for the same microsample by LA-MC-ICP-MS. The application of a zoom ion optic for aligning the ion beams into the ion counters allows fast switching between different isotope systems, which enables all of the abovementioned isotope ratios to be measured for the same microsample within a total analysis time of 15-20 min (excluding MC-ICP-MS optimization and calibration). The 101Ru/(99Ru+99Tc) and 102Ru/(99Ru+99Tc) isotope ratios were measured for four microsamples and were found to be significantly lower than the natural ratios, indicating that the microsamples were contaminated with the corresponding fission products (Ru and Tc). A slight depletion in 146Nd of about 3-5% was observed in the contaminated samples, but the Nd isotopic ratios measured in the contaminated samples coincided with natural isotopic composition within the measurement uncertainty, as most of the Nd in the analyzed samples originates from the natural soil load of this element. The 235U/238U and 236U/238U isotope ratios were the most sensitive indicators of irradiated uranium. The present work yielded a significant variation in uranium isotope ratios in microsamples, in contrast with previously published results from the bulk analysis of contaminated samples originating from the vicinity of Chernobyl. Thus, the 235U/238U ratios measured in ten

  1. Depth distributions of uranium-236 and cesium-137 in the Japan/East Sea; toward the potential use as a new oceanic circulation tracer

    NASA Astrophysics Data System (ADS)

    Sakaguchi, A.; Kadokura, A.; Steier, P.; Takahashi, Y.; Shizuma, K.; Yamamoto, M.

    2012-04-01

    137Cs (T1/2=30.2 y) has been spread all over the world as a fission product of atmospheric nuclear weapons tests in the 1960s. This nuclide has been used as a powerful tool for oceanography due to the well-defined origin and conservative behaviour in water . However, the number of atoms has decayed already to one thirds compared with its initial levels, and it will become more difficult to measure. In this situation, we focus on 236U (T1/2=2.342-107 y) as a candidate for a new isotopic tracer for oceanography. The detection of 236U in the environment has become possible only recently, by the development of measuring techniques with high sensitivity based on AMS. Our group showed that global fallout from bomb tests contains 236U, which might be produced as nuclear reactions of 235U(n,γ) and/or 238U(n,3n). So 236U has been therefore globally distributed in the surface environment. Thus, 236U has a similar potential as a tracer for environmental dynamics as 137Cs, especially for oceanography. In this study, a comprehensive attempt was made to measure the concentration of 236U in marine samples such as water, suspended solid and bottom sediments to clarify the environmental behaviour of this isotope. Furthermore, the discussion of the circulation of deep and bottom water in "Miniature Ocean", the Japan Sea, has been attempted. Bottom sediments (4 sites) and seawater samples (7 sites) were collected from the Japan Sea. The sediment core was cut into 1 cm segments from the surface to 5 cm in depth within a few hours after the sampling. About 20 L of seawater samples were collected from some depths in each site, and immediately after the sampling, the water was filtered with 0.45 μm pore-size membrane-filters. After the appropriate pre-treatment for each sample, uranium isotope and 137Cs were measured with AMS and Ge-detector, respectively. 236U was successfully detected for all seawater samples, and 236U/238U atom ratios in seawater were in the range of (0

  2. Determination of Reportable Radionuclides for DWPF Sludge Batch 3 (Macrobatch 4)

    SciTech Connect

    Bannochie, C

    2005-05-01

    The Waste Acceptance Product Specifications (WAPS) 1.2 require that ''The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115''. As part of the strategy to meet WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production through the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, IAEA Safeguards Reporting for HLW, requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The Defense Waste Processing Facility (DWPF) is receiving radioactive sludge slurry from High Level Waste Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the previous contents of Tank 40 (Sludge Batch 2) and the sludge that was transferred to Tank 40 from Tank 51. The blend of sludge from Tank 51 and Tank 40 defines Macrobatch 4 (also referred to as Sludge Batch 3). This report develops the list of reportable radionuclides and associated activities and determines the radionuclide activities as a function of time. The DWPF will use this list and the activities as one of the inputs for the

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

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

    MTE method is in the analytical performance achieved for the "minor" ratios 234U/238U and 236U/238U. The MTE method is now routinely used at all collaborating laboratories and possibly more in the future. Additional applications for the MTE method, e.g. to take advantage of the good external precision in combination with the possibilities of internal background and detector calibrations or mass jumps between different cup configurations, are presented as well. One interesting application concerns new absolute isotope ratio measurements for Ca with an unprecedented level of accuracy. This is important because up to now most reported Ca isotope data are only calculated as relative deviations from a standard like NIST-SRM 915. Using the MTE method measurements on new gravimetrically prepared Ca isotope mixtures were performed. A significantly improved level of accuracy at the level of about 0.02% for both the 42Ca/40Ca and 44Ca/40Ca ratios was obtained.

  4. Isotopic Systematics (U, nitrate and Sr) of the F-Area Acidic Contamination Plume at the Savannah River Site: Clues to Contaminant History and Mobility

    NASA Astrophysics Data System (ADS)

    Christensen, J. N.; Conrad, M. E.; Bill, M.; Denham, M.; Wan, J.; Rakshit, S.; Stringfellow, W. T.; Spycher, N.

    2010-12-01

    Seepage basins in the F-Area of the Savannah River Site were used from 1955 to 1989 for the disposal of low-level radioactive acidic (ave. pH ˜2.9) waste solutions from site operations involving irradiated uranium billets and other materials used in the production of radionuclides. These disposal activities resulted in a persistent acidic groundwater plume (pH as low as 3.2) beneath the F-Area including contaminants such as tritium, nitrate, 90Sr, 129I and uranium and that has impinged on surface water (Four Mile Branch) about 600 m from the basins. After cessation of disposal in 1989, the basins were capped in 1991. Since that time, remediation has consisted of a pump-and-treat system that has recently been replaced with in situ treatment using a funnel-and-gate system with injection of alkaline solutions in the gates to neutralize pH. In order to delineate the history of contamination and the current mobility and fate of contaminants in F-Area groundwater, we have undertaken a study of variations in the isotopic compositions of U (234U/238U, 235U/238U, 236U/238U), Sr (87Sr/86Sr) and nitrate (δ15N, δ18O) within the contaminant plume. This data can be used to trace U transport within the plume, evaluate chemical changes of nitrate, and potentially track plume/sediment chemical interaction and trace the migration of 90Sr. We have analyzed a suite of groundwater samples from monitoring wells, as well as pore-water samples extracted from aquifer sediment cores to map out the isotopic variation within the plume. The isotopic compositions of U from well samples and porewater samples are all consistent with the variable burn-up of depleted U. The variation in U isotopic composition requires at least three different endmembers, without any significant influence of background natural U. The δ15N and δ18O of nitrate from F-Area plume groundwater are distinct both from natural and unaltered synthetic nitrate, and likely represents fractionation due to waste volume

  5. Performance testing of the upgraded uranium isotopics multi-group analysis code MGAU

    NASA Astrophysics Data System (ADS)

    Berlizov, A. N.; Gunnink, R.; Zsigrai, J.; Nguyen, C. T.; Tryshyn, V. V.

    2007-06-01

    The paper describes recent developments of the MGAU (Multi-Group Analysis for Uranium) method, which resulted in the creation of an upgraded version 4.0 of the MGAU code. The major improvements concerned the procedure of the intrinsic efficiency calibration, particularly in the 120-205 keV region. The results of the tests carried out with the use of certified reference uranium isotopic materials SRM 969 and CRM 146 showed a significantly improved performance of the upgraded MGAU code for the accurate characterization of 235U and 234U abundances. The relative systematic biases of the abundances measured were evaluated not to exceed 1% and 3% over the concentration intervals 0.32-93.2 and 0.002-0.98 mass% for 235U and 234U, respectively. The influence of an up to 4-5 mm steel equivalent absorber and sample thickness on the measurement results was found to be much smaller than in previous versions of the code.

  6. 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. PMID:25944955

  7. Use of U-Series Isotopic Disequilibrium to Investigate the Nature and Distribution of Actively Flowing Fractures

    NASA Astrophysics Data System (ADS)

    Nichols, P. J.; Paces, J. B.; Neymark, L. A.; Rajaram, H.

    2011-12-01

    Groundwater transport of radioisotopes from underground nuclear tests at the Nevada National Security Site (NNSS) is of concern to the U.S. Department of Energy. Extensive testing was conducted near or below the regional water table (saturated zone; SZ) at Pahute Mesa and within the unsaturated (or partially saturated) zone at Rainier Mesa. Groundwater flow in these rocks is believed to occur mainly through a connected network of fractures. To better understand flow in these fractured rocks, we analyzed U-series isotopes (238U-234U-230Th) from drill core samples. In rock isolated from flow over the last million years, isotopes in the 238U decay chain reach a state of radioactive secular equilibrium, where 234U/238U and 230Th/238U activity ratios (AR) = 1.0. More recent water-rock interaction results in mobilization of 234U relative to 238U, and U relative to Th in migrating waters. Rock surfaces that incorporate this U or are leached of 234U and U will show U-series disequilibrium. Isotope data can thus provide time-sensitive information on hydrologic conditions in host rocks without directly observing or measuring flowing water. To investigate NNSS fracture networks, core was selected from confining units (bedded and zeolitized felsic tuffs) and aquifers (felsic welded tuffs and lavas) in five boreholes on Pahute Mesa and two boreholes on Rainier Mesa. Samples include interiors of intact core as well as natural fracture surfaces and brecciated core. Intact core and brecciated samples were crushed and powdered. Fracture surfaces were sampled using dental burs to remove the outer 0.1 to 0.5 mm of fracture surfaces, which may have thin mineral coatings of zeolites, clays, and Mn oxides. Samples were totally digested, spiked with a 236U-229Th tracer, and analyzed by a solid-source TRITON° mass spectrometer equipped with an energy filter and single ion counter. Results show that 8 of 9 intact core samples have 234U/238U AR within ±5% of 1.0, suggesting little or no

  8. Estimation of (n,f) Cross-Sections by Measuring Reaction Probability Ratios

    SciTech Connect

    Plettner, C; Ai, H; Beausang, C W; Bernstein, L A; Ahle, L; Amro, H; Babilon, M; Burke, J T; Caggiano, J A; Casten, R F; Church, J A; Cooper, J R; Crider, B; Gurdal, G; Heinz, A; McCutchan, E A; Moody, K; Punyon, J A; Qian, J; Ressler, J J; Schiller, A; Williams, E; Younes, W

    2005-04-21

    Neutron-induced reaction cross-sections on unstable nuclei are inherently difficult to measure due to target activity and the low intensity of neutron beams. In an alternative approach, named the 'surrogate' technique, one measures the decay probability of the same compound nucleus produced using a stable beam on a stable target to estimate the neutron-induced reaction cross-section. As an extension of the surrogate method, in this paper they introduce a new technique of measuring the fission probabilities of two different compound nuclei as a ratio, which has the advantage of removing most of the systematic uncertainties. This method was benchmarked in this report by measuring the probability of deuteron-induced fission events in coincidence with protons, and forming the ratio P({sup 236}U(d,pf))/P({sup 238}U(d,pf)), which serves as a surrogate for the known cross-section ratio of {sup 236}U(n,f)/{sup 238}U(n,f). IN addition, the P({sup 238}U(d,d{prime}f))/P({sup 236}U(d,d{prime}f)) ratio as a surrogate for the {sup 237}U(n,f)/{sup 235}U(n,f) cross-section ratio was measured for the first time in an unprecedented range of excitation energies.

  9. Uranium beam characterization at CIRCE for background and contamination determinations.

    PubMed

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

    2015-09-01

    The Accelerator Mass Spectrometry (AMS) is the most sensitive technique, compared either to the Inductively Coupled Plasma (ICP-MS) or Thermal Ionization (TI-MS) mass spectrometer, for the actinide (e.g. (236)U, (x)Pu isotopes) measurements. They are present in environmental samples at the ultra trace level since atmospheric tests of Nuclear Weapons (NWs) performed in the past, deliberate dumping of nuclear waste, nuclear fuel reprocessing, on a large scale, and operation of Nuclear Power Plants (NPPs), on a small scale, have led to the release of a wide range of radioactive nuclides in the environment. At the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy, an upgraded actinide AMS system, based on a 3-MV pelletron tandem accelerator, has been developed and routinely operated. At CIRCE a charge state distribution as a function of terminal voltage, the beam emittance, measured in the 20° actinides dedicated beam line, as well as the energy and position validation of the U ions were performed in order to determine the best measurement conditions. A (236)U/(238)U isotopic ratio background level of about 5×10(-12) or 3×10(-13), depending on the Time of Flight-Energy (TOF-E) configurations, as well as the spatial distribution of the (235)U, (238)U interferences ions and a (236)U contamination mass of about 0.5 fg have been determined. PMID:26103623

  10. Distribution of uranium isotopes in surface water of the Llobregat river basin (Northeast Spain).

    PubMed

    Camacho, A; Devesa, R; Vallés, I; Serrano, I; Soler, J; Blázquez, S; Ortega, X; Matia, L

    2010-12-01

    A study is presented on the distribution of (234)U, (238)U, (235)U isotopes in surface water of the Llobregat river basin (Northeast Spain), from 2001 to 2006. Sixty-six superficial water samples were collected at 16 points distributed throughout the Llobregat river basin. Uranium isotopes were measured by alpha spectrometry (PIPS detectors). The test procedure was validated according to the quality requirements of the ISO17025 standard. The activity concentration for the total dissolved uranium ranges from 20 to 261mBqL(-1). The highest concentrations of uranium were detected in an area with formations of sedimentary rock, limestone and lignite. A high degree of radioactive disequilibrium was noted among the uranium isotopes. The (234)U/(238)U activity ratio varied between 1.1 and 1.9 and the waters with the lowest uranium activity registered the highest level of (234)U/(238)U activity ratio. Correlations between uranium activity in the tested water and chemical and physical characteristics of the aquifer were found. PMID:20870317

  11. Certification of the Uranium Isotopic Ratios in Nbl Crm 112-A, Uranium Assay Standard (Invited)

    NASA Astrophysics Data System (ADS)

    Mathew, K. J.; Mason, P.; Narayanan, U.

    2010-12-01

    Isotopic reference materials are needed to validate measurement procedures and to calibrate multi-collector ion counting detector systems. New Brunswick Laboratory (NBL) provides a suite of certified isotopic and assay standards for the US and international nuclear safeguards community. NBL Certified Reference Material (CRM) 112-A Uranium Metal Assay Standard with a consensus value of 137.88 for the 238U/235U ratio [National Bureau of Standards -- NBS, currently named National Institute for Standards and Technology, Standard Reference Material (SRM) 960 had been renamed CRM 112-A] is commonly used as a natural uranium isotopic reference material within the earth science community. We have completed the analytical work for characterizing the isotopic composition of NBL CRM 112-A Uranium Assay Standard and NBL CRM 145 (uranyl nitrate solution prepared from CRM 112-A). The 235U/238U isotopic ratios were characterized using the total evaporation (TE) and the modified total evaporation (MTE) methods. The 234U/238U isotope ratios were characterized using a conventional analysis technique and verified using the ratios measured in the MTE analytical technique. The analysis plan for the characterization work was developed such that isotopic ratios that are traceable to NBL CRM U030-A are obtained. NBL is preparing a certificate of Analysis and will issue a certificate for Uranium Assay and Isotopics. The results of the CRM 112-A certification measurements will be discussed. These results will be compared with the average values from Richter et al (2010). A comparison of the precision and accuracy of the measurement methods (TE, MTE and Conventional) employed in the certification will be presented. The uncertainties in the 235U/238U and 234U/238U ratios, calculated according to the Guide to the Expression of Uncertainty in Measurements (GUM) and the dominant contributors to the combined standard uncertainty will be discussed.

  12. Characterization of Nuclear Fuel using Multivariate Statistical Analysis

    SciTech Connect

    Robel, M; Robel, M; Robel, M; Kristo, M J; Kristo, M J

    2007-11-27

    Various combinations of reactor type and fuel composition have been characterized using principle components analysis (PCA) of the concentrations of 9 U and Pu isotopes in the 10 fuel as a function of burnup. The use of PCA allows the reduction of the 9-dimensional data (isotopic concentrations) into a 3-dimensional approximation, giving a visual representation of the changes in nuclear fuel composition with burnup. Real-world variation in the concentrations of {sup 234}U and {sup 236}U in the fresh (unirradiated) fuel was accounted for. The effects of reprocessing were also simulated. The results suggest that, 15 even after reprocessing, Pu isotopes can be used to determine both the type of reactor and the initial fuel composition with good discrimination. Finally, partial least squares discriminant analysis (PSLDA) was investigated as a substitute for PCA. Our results suggest that PLSDA is a better tool for this application where separation between known classes is most important.

  13. Uranium from German Nuclear Power Projects of the 1940s--A Nuclear Forensic Investigation.

    PubMed

    Mayer, Klaus; Wallenius, Maria; Lützenkirchen, Klaus; Horta, Joan; Nicholl, Adrian; Rasmussen, Gert; van Belle, Pieter; Varga, Zsolt; Buda, Razvan; Erdmann, Nicole; Kratz, Jens-Volker; Trautmann, Norbert; Fifield, L Keith; Tims, Stephen G; Fröhlich, Michaela B; Steier, Peter

    2015-11-01

    Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel. Through measurement of the (230)Th/(234)U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the (87)Sr/(86)Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of (236)U and (239)Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence. PMID:26501922

  14. Uranium from German Nuclear Power Projects of the 1940s— A Nuclear Forensic Investigation

    PubMed Central

    Mayer, Klaus; Wallenius, Maria; Lützenkirchen, Klaus; Horta, Joan; Nicholl, Adrian; Rasmussen, Gert; van Belle, Pieter; Varga, Zsolt; Buda, Razvan; Erdmann, Nicole; Kratz, Jens-Volker; Trautmann, Norbert; Fifield, L Keith; Tims, Stephen G; Fröhlich, Michaela B; Steier, Peter

    2015-01-01

    Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel.3b,d, 4 Through measurement of the 230Th/234U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the 87Sr/86Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of 236U and 239Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence. PMID:26501922

  15. Determination of 238Pu(n ,f ) and 236Np(n ,f ) cross sections using surrogate reactions

    NASA Astrophysics Data System (ADS)

    Pal, A.; Santra, S.; Nayak, B. K.; Mahata, K.; Desai, V. V.; Chattopadhyay, D.; Tripathi, R.

    2015-05-01

    The cross sections for 238Pu(n ,f ) reaction for equivalent neutron energy of 13.0-22.0 MeV have been determined by the "surrogate ratio" method by measuring 235U(6Li,d f ) and 232Th(6Li,d f ) transfer induced fission reactions proceeding through the excited fissioning nuclei 239Pu and 236U, respectively, and using 235U(n ,f ) cross-section data as the reference. Similarly, the cross sections for the 236Np(n ,f ) reaction in the equivalent neutron energy range 9.9-22.0 MeV have been determined by the "hybrid surrogate ratio" method via the measurements of 235U(6Li,α f ) and 235U(6Li,d f ) transfer induced fission reactions, using 238Pu(n ,f ) cross-section data as the reference. The empire-3.1 calculations for 238Pu(n ,f ) and 236Np(n ,f ) cross sections agree well with the present data, however, they are slightly underestimated by the endf/b-vii.1 evaluations.

  16. Alpha particle induced gamma yields in uranium hexafluoride

    NASA Astrophysics Data System (ADS)

    Croft, Stephen; Swinhoe, Martyn T.; Miller, Karen A.

    2013-01-01

    Fluorine has a relatively large (α,n) production cross-section in the MeV range, the energy range of interest for special nuclear materials. In the uranium fuel cycle enriched UF6 in particular is a reasonably prolific source of (α,n) neutrons because along with 235U, 234U becomes enriched and it has a relatively short half-life. This enables the mass content of storage cylinders containing UF6 to be verified by neutron counting methods. In association with such measurements high resolution gamma-ray spectrometry (HRGS) measurements using a high-purity Ge detector are often undertaken to determine the 235U enrichment based off the intensity of the direct 186 keV line. The specific (α,n) neutron production, neutrons per second per gram of U, is sensitive to the relative isotopic composition, particularly the 234U concentration, and the traditional gross neutron counting approach is needed to quantitatively interpret the data. In addition to F(α,n) neutrons, α-induced reaction γ-rays are generated, notably at 110, 197, 582, 891, 1236 and 1275 keV. If one could observe 19F(α,xγ) gamma-lines in the HRGS spectra the thought was that perhaps the α-activity could be estimated directly, and in turn the 234U abundance obtained. For example, by utilizing the ratio of the detected 197-186 keV full energy peaks. However, until now there has been no readily available estimate of the expected strength of the reaction gamma-rays nor any serious consideration as to whether they might be diagnostic or not. In this work we compute the thick target yields of the chief reaction gamma-rays in UF6 using published thin target data. Comparisons are made to the neutron production rates to obtain γ/n estimates, and also to the 235U decay line at 186 keV which we take as a fiducial line. It is shown that the reaction gamma-rays are produced but are far too weak for practical safeguards purposes. Now that the underlying numerical data is readily available however, it can be used to

  17. 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.

  18. 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.

  19. Multiple ion counting ICPMS double spike method for precise U isotopic analysis at ultra-trace levels

    NASA Astrophysics Data System (ADS)

    Snow, Jonathan E.; Friedrich, Jon M.

    2005-04-01

    Of the various methods for the measurement of the isotopic composition of U in solids and solutions, few offer both sensitivity and precision. In recent years, the use of ICPMS technology for this determination has become increasingly prevalent. Here we describe a method for the determination of the 235U/238U ratio in very small quantities (<=350 pg) with an accuracy of better than 3[per mille sign]. We measured several terrestrial standard materials and repeated analyses of the U960 isotopic composition standard. We used a 233U/236U double spike, with multiple ion counting on an unmodified Nu Instruments multicollector ICPMS and a non-standard detector configuration that allows an approximately 20-fold sensitivity gain over the best conventional techniques. This technique shows promise for the detection of isotopic tracers in the environment (for example anthropogenic 238U) at very extreme dilutions, or in cases where the total amount of analyte is necessarily limited.

  20. Simultaneous determination of the quantity and isotopic ratios of uranium in individual micro-particles by isotope dilution thermal ionization mass spectrometry (ID-TIMS).

    PubMed

    Park, Jong-Ho; Choi, Eun-Ju

    2016-11-01

    A method to determine the quantity and isotopic ratios of uranium in individual micro-particles simultaneously by isotope dilution thermal ionization mass spectrometry (ID-TIMS) has been developed. This method consists of sequential sample and spike loading, ID-TIMS for isotopic measurement, and application of a series of mathematical procedures to remove the contribution of uranium in the spike. The homogeneity of evaporation and ionization of uranium content was confirmed by the consistent ratio of n((233)U)/n((238)U) determined by TIMS measurements. Verification of the method was performed using U030 solution droplets and U030 particles. Good agreements of resulting uranium quantity, n((235)U)/n((238)U), and n((236)U)/n((238)U) with the estimated or certified values showed the validity of this newly developed method for particle analysis when simultaneous determination of the quantity and isotopic ratios of uranium is required. PMID:27591656

  1. 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.

  2. Natural and man-made radioactivity in soils and plants around the research reactor of Inshass.

    PubMed

    Higgy, R H; Pimpl, M

    1998-12-01

    The specific radioactivities of the U-series, 232Th, 137Cs and 40K were measured in soil samples around the Inshass reactor in Cairo, using a gamma-ray spectrometer with a HpGe detector. The alpha activity of 238U, 234U and 235U was measured in the same soil samples by surface barrier detectors after radiochemical separation and the obtained results were compared with the specific activities determined by gamma-measurements. The alpha-activity of 238Pu, 239+240Pu, 241Am, 242Cm and 244Cm was measured after radiochemical separation by surface barrier detectors for both soil and plant samples. Then beta-activity of 241Pu was measured using liquid scintillation spectrometry. PMID:9776618

  3. A new Certified Reference Material for radionuclides in Irish sea sediment (IAEA-385).

    PubMed

    Pham, M K; Sanchez-Cabeza, J A; Povinec, P P; Andor, K; Arnold, D; Benmansour, M; Bikit, I; Carvalho, F P; Dimitrova, K; Edrev, Z H; Engeler, C; Fouche, F J; Garcia-Orellana, J; Gascó, C; Gastaud, J; Gudelis, A; Hancock, G; Holm, E; Legarda, F; Ikäheimonen, T K; Ilchmann, C; Jenkinson, A V; Kanisch, G; Kis-Benedek, G; Kleinschmidt, R; Koukouliou, V; Kuhar, B; Larosa, J; Lee, S-H; Lepetit, G; Levy-Palomo, I; Liong Wee Kwong, L; Llauradó, M; Maringer, F J; Meyer, M; Michalik, B; Michel, H; Nies, H; Nour, S; Oh, J-S; Oregioni, B; Palomares, J; Pantelic, G; Pfitzner, J; Pilvio, R; Puskeiler, L; Satake, H; Schikowski, J; Vitorovic, G; Woodhead, D; Wyse, E

    2008-11-01

    A new Certified Reference Material (CRM) for radionuclides in sediment (IAEA-385) is described and the results of the certification process are presented. Eleven radionuclides ((40)K, (137)Cs, (226)Ra, (228)Ra, (230)Th, (232)Th, (234)U, (238)U, (238)Pu, (239+240)Pu and (241)Am) have been certified and information mass activities with 95% confidence intervals are given for seven other radionuclides ((90)Sr, (210)Pb((210)Po), (235)U, (239)Pu, (240)Pu and (241)Pu). Results for less frequently reported radionuclides ((60)Co, (99)Tc, (134)Cs, (155)Eu, (224)Ra and (239)Np) and information on some activity and mass ratios are also reported. The CRM can be used for quality assurance/quality control of the analysis of radionuclides in sediment samples, for the development and validation of analytical methods and for training purposes. PMID:18513984

  4. Certified reference material for radionuclides in fish flesh sample IAEA-414 (mixed fish from the Irish Sea and North Sea).

    PubMed

    Pham, M K; Sanchez-Cabeza, J A; Povinec, P P; Arnold, D; Benmansour, M; Bojanowski, R; Carvalho, F P; Kim, C K; Esposito, M; Gastaud, J; Gascó, C L; Ham, G J; Hegde, A G; Holm, E; Jaskierowicz, D; Kanisch, G; Llaurado, M; La Rosa, J; Lee, S-H; Liong Wee Kwong, L; Le Petit, G; Maruo, Y; Nielsen, S P; Oh, J-S; Oregioni, B; Palomares, J; Pettersson, H B L; Rulik, P; Ryan, T P; Sato, K; Schikowski, J; Skwarzec, B; Smedley, P A; Tarján, S; Vajda, N; Wyse, E

    2006-01-01

    A certified reference material (CRM) for radionuclides in fish sample IAEA-414 (mixed fish from the Irish Sea and North Seas) is described and the results of the certification process are presented. Nine radionuclides (40K, 137Cs, 232Th, 234U, 235U, 238U, 238Pu, 239+240Pu and 241Am) were certified for this material. Information on massic activities with 95% confidence intervals is given for six other radionuclides (90Sr, 210Pb(210Po), 226Ra, 239Pu, 240Pu 241Pu). Less frequently reported radionuclides (99Tc, 129I, 228Th, 230Th and 237Np) and information on some activity and mass ratios are also included. The CRM can be used for quality assurance/quality control of the analysis of radionuclides in fish sample, for the development and validation of analytical methods and for training purposes. The material is available from IAEA, Vienna, in 100 g units. PMID:16549351

  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. 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. PMID:26631455

  7. 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.

  8. 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.

  9. 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.

  10. 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. PMID:24291528

  11. Isotopic evidence for reductive immobilization of uranium across a roll-front mineral deposit

    DOE PAGESBeta

    Brown, Shaun T.; Basu, Anirban; Christensen, John N.; Reimus, Paul; Heikoop, Jeffrey; Simmons, Ardyth; Woldegabriel, Giday; Maher, Kate; Weaver, Karrie; Clay, James; et al

    2016-06-21

    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

  12. NBL CRM 112-A: A new certified isotopic composition

    NASA Astrophysics Data System (ADS)

    Thomas, R. B.; Essex, R. M.; Mason, P.

    2007-12-01

    NBL CRM 112-A Uranium Metal Assay Standard is commonly used as a natural uranium isotopic reference material within the earth science mass spectrometry community. The metal is from the same parent material as NBS SRM 960, the uranyl nitrate solution, CRM 145, and the high-purity uranyl nitrate solution CRM 145-B. Because CRM 112-A has not yet been certified for isotopic composition, it has been assumed that this material has a natural 235U/238U (0.0072527), and the δ234U has been determined by measurement (e.g. -37.1‰; Cheng et al., 2000). These values have been widely used to calibrate the concentration of spikes and standards, and to correct measurements for instrument or mass bias. New, preliminary, isotopic measurements on CRM 145 and CRM 112-A performed at New Brunswick Laboratory suggest that these reference materials have a slightly lower 235U/238U and δ234U than have been commonly used. If this is the case, then data using the accepted values may be slightly biased. The significance of this bias will depend on the uncertainty of the measurement, how the CRM 112-A data is used to correct measurement data, the cited values that were used to correct the data, and the final certified values of the CRM. This fall, New Brunswick Laboratory is certifying the isotopic composition of the CRM 112-A metal using high precision thermal ionization mass spectrometry techniques. Upon completion of certification, the new CRM 112- A standard with certified isotopic ratios will provide the earth science community with a well characterized and traceable reference for calibrating and correcting their mass spectrometry measurement systems.

  13. 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.

  14. Isotopic Evidence for Reductive Immobilization of Uranium Across a Roll-Front Mineral Deposit.

    PubMed

    Brown, Shaun T; Basu, Anirban; Christensen, John N; Reimus, Paul; Heikoop, Jeffrey; Simmons, Ardyth; Woldegabriel, Giday; Maher, Kate; Weaver, Karrie; Clay, James; DePaolo, Donald J

    2016-06-21

    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 (238)U/(235)U of groundwater varies by approximately 3‰ and is correlated with U concentrations. Fluid samples down-gradient of the ore zone are the most depleted in (238)U and have the lowest U concentrations. Activity ratios of (234)U/(238)U 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 (234)U/(238)U and (238)U/(235)U 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. 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. PMID:27203292

  15. 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

  16. U and Th-series isotopes: a probe into time-dependent erosion processes in soils

    NASA Astrophysics Data System (ADS)

    Hillaire-Marcel, Claude; Ghaleb, Bassam; Barbecot, Florent

    2010-05-01

    Disequilibria between 238U-234Th-234U-230Th-226Ra-210Pb-210Po, 235U-231Pa and 232Th-228Ra-228Th, offer probes into time dependent processes over time scales ranging 106 a to a few days, thus the means to document soil erosion rates over a large array of time scales and hydroclimatic forcings. Because lithology constitutes a boundary condition, we intend to illustrate the behavior of such isotopes in carbonate-rich soils, with examples from cool-temperate (St Lawrence Lowlands, Canada) or arid settings (Palmyre area, Syria) but special attention to Mediterranean environments (SE France). In this later case, a >12 m thick unsaturated zone has been sampled, near Beziers, in the recharge zone of the "Astian carbonate sand Aquifer", firstly along a naturally exposed section, then in a cored sequence. Geochemical and mineralogical analyses, including stable isotopes were complemented by 228U, 234U, 230Th, 226Ra, 210Pb and 228Th, 232Th measurements from soil surface, down to about 12 m below surface. Whereas the upper 7 m depict geochemical and isotopic features linked to dissolution/re-precipitation processes with highly variable radioactive disequilibria, the lower part of the sequence shows distinctive properties. In this deep horizon, strong excesses in 234U and 230Th over parent isotopes (i.e. 238U and 234U, respectively) are observed simultaneously whereas 226Ra and 230Th are in secular equilibrium. We interpret these features as an indication for a slow-process enrichment in 234Th(234U) and 230Th, linked to dissolved U-decay during groundwater recharge events. 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 222Rn-diffusion. It is concluded from this example that beside the strong impact on U- and Th-series disequilibria of fast chemical process occurring in the upper soil horizons, slower processes still leave an imprint with longer

  17. 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

  18. Deducing the 237U(n,f) cross-section using the Surrogate Ratio Method

    SciTech Connect

    Burke, J T; Bernstein, L A; Escher, J; Ahle, L; Church, J A; Dietrich, F S; Moody, K J; Norman, E B; Phair, L; Fallon, P; Clark, R M; Deleplanque, M A; Descovich, M; Cromaz, M; Lee, I Y; Macchiavelli, A O; McMahan, M A; Moretto, L G; Rodriguez-Vieitez, E; Stephens, F S; Ai, H; Beausang, C; Cridder, B

    2005-12-29

    The authors have deduced the cross section for {sup 237}U(n,f) over an equivalent neutron energy range from 0 to 20 MeV using the Surrogate Ratio method. A 55 MeV {sup 4}He beam from the 88 Inch Cyclotron at Lawrence Berkeley National Laboratory was used to induce fission in the following reactions: {sup 238}U({alpha},{alpha}{prime}f) and {sup 236}U({alpha},{alpha}{prime}f). The {sup 238}U reaction was a surrogate for {sup 237}U(n,f) and the {sup 236}U reaction was used as a surrogate for {sup 235}U(n,f). Scattered alpha particles were detected in a fully depleted segmented silicon telescope array (STARS) over an angle range of 35{sup o} to 60{sup o} with respect to the beam axis. The fission fragments were detected in a third independent silicon detector located at backward angles between 106{sup o} and 131{sup o}.

  19. Dynamical approach to isotopic-distribution of fission fragments from actinide nuclei

    NASA Astrophysics Data System (ADS)

    Ishizuka, Chikako; Chiba, Satoshi; Karpov, Alexander V.; Aritomo, Yoshihiro

    2016-06-01

    Measurements of the isotope distribution of fission fragments, often denoted as the primary fission yield (pre-neutron yield) or independent fission yield (post-neutron yield) are still challenging at low excitation energies, so that it is important to investigate it within a theory. Such quantities are vital for applications as well. In this study, fragment distributions from the fission of U isotopes at low excitation energies are studied using a dynamical model. The potential energy surface is derived from the two center shell model including the shell and pairing corrections. In order to calculate the charge distribution of fission fragments, we introduce a new parameter ηZ as the charge asymmetry, in addition to three parameters describing a nuclear shape, z as the distance between two centers of mass, δ as fragment deformation, and ηA as the mass asymmetry. Using this model, we calculated the isotopic distribution of 236U for the n-induced process 235U + n → 236U at low excitation energies. As a result, we found that the current model can well reproduce isotopic fission-fragment distribution which can be compared favorably with major libraries.

  20. The production of Neptunium-236g.

    PubMed

    Jerome, S M; Ivanov, P; Larijani, C; Parker, D J; Regan, P H

    2014-12-01

    Radiochemical analysis of (237)Np is important in a number of fields, such as nuclear forensics, environmental analysis and measurements throughout the nuclear fuel cycle. However analysis is complicated by the lack of a stable isotope of neptunium. Although various tracers have been used, including (235)Np, (239)Np and even (236)Pu, none are entirely satisfactory. However, (236g)Np would be a better candidate for a neptunium yield tracer, as its long half-life means that it is useable as both a radiometric and mass spectrometric measurements. This radionuclide is notoriously difficult to prepare, and limited in scope. In this paper, we examine the options for the production of (236g)Np, based on work carried out at NPL since 2011. However, this work was primarily aimed at the production of (236)Pu, and not (236g)Np and therefore the rate of production are based on the levels of (236)Pu generated in the irradiation of (i) (238)U with protons, (ii) (235)U with deuterons, (iii) (236)U with protons and (iv) (236)U with deuterons. The derivation of a well-defined cross section is complicated by the relevant paucity of information on the variation of the (236m)Np:(236g)Np production ratio with incident particle energy. Furthermore, information on the purity of (236g)Np so produced is similarly sparse. Accordingly, the existing data is assessed and a plan for future work is presented. PMID:24731718

  1. Deducing the 237U(n,f) cross-section using the Surrogate Ratio Method

    SciTech Connect

    Burke, J T; Bernstein, L A; Escher, J; Ahle, L; Church, J A; Dietrich, F; Moody, K J; Norman, E B; Phair, L W; Fallon, P; Clark, R; Delaplanque, M; Descovich, M; Cromaz, M; Lee, I Y; Macchiavelli, A O; McMahan, M A; Moretto, L G; Rodriguez-Vieitez, E; Stephens, F S

    2005-08-16

    The authors have deduced the {sup 237}U(n,f) cross-section over an equivalent neutron energy range of 0 to 20 MeV using the Surrogate Ratio method. A 55 MeV {sup 4}He{sup 2+} beam from the 88 Inch Cyclotron at Lawrence Berkeley National Laboratory was used to induce fission in the following reactions {sup 238}U({alpha},{alpha}'f) and {sup 236}U({alpha},{alpha}'f). The {sup 238}U reaction was a surrogate for {sup 237}U(n,f) and the {sup 236}U reaction was used as a surrogate for {sup 235}U(n,f). The energies of the scattered alpha particles were detected in a fully depleted segmented silicon telescope array (STARS) over an angle range of 35{sup o} to 60{sup o} with respect to the beam axis. The fission fragments were detected in a third independent silicon detector located at backward angles between 106{sup o} to 131{sup o}.

  2. 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.

  3. 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.

  4. Isotopic and Geochemical Tracers for U(VI) Reduction and U Mobility at an in Situ Recovery U Mine.

    PubMed

    Basu, Anirban; Brown, Shaun T; Christensen, John N; DePaolo, Donald J; Reimus, Paul W; Heikoop, Jeffrey M; Woldegabriel, Giday; Simmons, Ardyth M; House, Brian M; Hartmann, Matt; Maher, Kate

    2015-05-19

    In situ recovery (ISR) uranium (U) mining mobilizes U in its oxidized hexavalent form (U(VI)) by oxidative dissolution of U from the roll-front U deposits. Postmining natural attenuation of residual U(VI) at ISR mines is a potential remediation strategy. Detection and monitoring of naturally occurring reducing subsurface environments are important for successful implementation of this remediation scheme. We used the isotopic tracers (238)U/(235)U (δ(238)U), (234)U/(238)U activity ratio, and (34)S/(32)S (δ(34)S), and geochemical measurements of U ore and groundwater collected from 32 wells located within, upgradient, and downgradient of a roll-front U deposit to detect U(VI) reduction and U mobility at an ISR mining site at Rosita, TX, USA. The δ(238)U in Rosita groundwater varies from +0.61‰ to -2.49‰, with a trend toward lower δ(238)U in downgradient wells. The concurrent decrease in U(VI) concentration and δ(238)U with an ε of 0.48‰ ± 0.08‰ is indicative of naturally occurring reducing environments conducive to U(VI) reduction. Additionally, characteristic (234)U/(238)U activity ratio and δ(34)S values may also be used to trace the mobility of the ore zone groundwater after mining has ended. These results support the use of U isotope-based detection of natural attenuation of U(VI) at Rosita and other similar ISR mining sites. PMID:25909757

  5. Determination of long-lived actinides in soil leachates by inductively coupled plasma: Mass spectrometry

    SciTech Connect

    Crain, J.S.; Smith, L.L.; Yaeger, J.S.; Alvarado, J.A.

    1994-06-01

    Inductively coupled plasma -- mass spectrometry (ICP-MS) was used to concurrently determine multiple long-lived (t{sub 1/2} > 10{sup 4} y) actinide isotopes in soil samples. Ultrasonic nebulization was found to maximize instrument sensitivity. Instrument detection limits for actinides in solution ranged from 50 mBq L{sup {minus}1} ({sup 239}Pu) to 2 {mu}Bq L{sup {minus}1} ({sup 235}U) Hydride adducts of {sup 232}Th and {sup 238}U interfered with the determinations of {sup 233}U and {sup 239} Pu; thus, extraction chromatography was, used to eliminate the sample matrix, concentrate the analytes, and separate uranium from the other actinides. Alpha spectrometric determinations of {sup 230}Th, {sup 239}Pu, and the {sup 234}U/{sup 238}U activity ratio in soil leachates compared well with ICP-MS determinations; however, there were some small systematic differences (ca. 10%) between ICP-MS and a-spectrometric determinations of {sup 234}U and {sup 238}U activities.

  6. Uranium Isotopes in Calcium Carbonate: A Possible Proxy for Paleo-pH and Carbonate Ion Concentration?

    NASA Astrophysics Data System (ADS)

    Chen, X.; Romaniello, S. J.; Herrmann, A. D.; Wasylenki, L. E.; Anbar, A. D.

    2015-12-01

    Natural variations of 238U/235U in marine carbonates are being explored as a paleoredox proxy. However, in order for this proxy to be robust, it is important to understand how pH and alkalinity affect the fractionation of 238U/235U during coprecipitation with calcite and aragonite. Recent work suggests that the U/Ca ratio of foraminiferal calcite may vary with seawater [CO32-] concentration due to changes in U speciation[1]. Here we explore analogous isotopic consequences in inorganic laboratory co-precipitation experiments. Uranium coprecipitation experiments with calcite and aragonite were performed at pH 8.5 ± 0.1 and 7.5 ± 0.1 using a constant addition method [2]. Dissolved U in the remaining solution was periodically collected throughout the experiments. Samples were purified with UTEVA resin and 238U/235U was determined using a 233U-236U double-spike and MC-ICP-MS, attaining a precision of ± 0.10 ‰ [3]. Small but resolvable U isotope fractionation was observed in aragonite experiments at pH ~8.5, preferentially enriching heavier U isotopes in the solid phase. 238U/235U of the dissolved U in these experiments can be fit by Rayleigh fractionation curves with fractionation factors of 1.00002 - 1.00009. In contrast, no resolvable U isotope fractionation was detected in an aragonite experiment at pH ~7.5 or in calcite experiments at either pH. Equilibrium isotope fractionation among dissolved U species is the most likely mechanism driving these isotope effects. Our quantitative model of this process assumes that charged U species are preferentially incorporated into CaCO3 relative to the neutral U species Ca2UO2(CO3)3(aq), which we hypothesize to have a lighter equilibrium U isotope composition than the charged U species. According to this model, the magnitude of U isotope fractionation should scale with the fraction of the neutral U species in the solution, in agreement with our experimental results. These findings suggest that U isotope variations in

  7. Uranium Isotope Fractionation During Coprecipitation with Aragonite and Calcite

    NASA Astrophysics Data System (ADS)

    Chen, X.; Romaniello, S. J.; Herrmann, A. D.; Wasylenki, L. E.; Anbar, A. D.

    2014-12-01

    Natural variations in the 238U/235U ratio of marine carbonates may provide a useful way of constraining past variations in ocean redox conditions. However, before applying this novel redox proxy, it is essential to explore possible isotopic fractionation during U coprecipitation with aragonite and calcite. We investigated these effects in laboratory experiments. Aragonite and calcite coprecipitation experiments were conducted at pH 8.5±0.1 using a constant addition method [1]. More than 90% of the U was incorporated into the solid phase at the end of each experiment. Samples were purified using UTEVA chemistry and δ238/235U was measured using 233U-236U double-spike MC-ICP-MS with a precision of ±0.10‰ [2]. The aragonite experiment demonstrated a 238U/235U Rayleigh fractionation factor of α=1.00008±0.00002 with the 238U preferentially incorporated. In contrast, the calcite experiment demonstrated no resolvable U isotope fractionation (α=1.00001±0.00003). To determine if U isotopes are affected during the early diagenetic conversion of aragonite to calcite, natural carbonate samples were collected along an aragonite-calcite transition across a single coral head in the Key Largo limestone, and characterized for U concentration and δ238/235U [3]. We found that the mean δ238/235U in aragonite (-0.33±0.07‰ 2se) was slightly heavier than that in calcite (-0.37±0.02‰ 2se). Further work is needed to address the mechanisms leading to differential isotopic fractionation of U(VI) during incorporation into aragonite and calcite. Possible drivers include differences in coordination in the crystal structure or equilibrium isotopic fractionation between various aqueous U(VI) species prior to incorporation. [1] Reeder et al. (2001) GCA 65, 3491-3503. [2] Weyer et al., (2008) GCA 72, 345-359. [3] Gill et al., (2008) GCA 72, 4699-4722.

  8. Determination of total and isotopic uranium by inductively coupled plasma-mass spectrometry at the Fernald Environmental Management Project

    SciTech Connect

    Miller, F.L.; Bolin, R.N.; Feller, M.T.; Danahy, R.J.

    1995-04-01

    At the Fernald Environmental Management Project (FEMP) in southwestern Ohio, ICP-mass spectrometry (ICP-MS), with sample introduction by peristaltic pumping, is used to determine total and isotopic uranium (U-234, U-235, U-236 and U-238) in soil samples. These analyses are conducted in support of the environmental cleanup of the FEMP site. Various aspects of the sample preparation and instrumental analysis will be discussed. Initial sample preparation consists of oven drying to determine moisture content, and grinding and rolling to homogenize the sample. This is followed by a nitric/hydrofluoric acid digestion to bring the uranium in the sample into solution. Bismuth is added to the sample prior to digestion to monitor for losses. The total uranium (U-238) content of this solution and the U{sup 235}/U{sup 238} ratio are measured on the first pass through the ICP-MS. To determine the concentration of the less abundant U{sup 234} and U{sup 236} isotopes, the digestate is further concentrated by using Eichrom TRU-Spec extraction columns before the second pass through the ICP-MS. Quality controls for both the sample preparation and instrumental protocols will also be discussed. Finally, an explanation of the calculations used to report the data in either weight percent or activity units will be given.

  9. IXth millenium B.C. ceramics from Niger: detection of a U-series disequilibrium and TL dating

    NASA Astrophysics Data System (ADS)

    Guibert, P.; Schvoerer, M.; Etcheverry, M. P.; Szepertyski, B.; Ney, C.

    A set of pottery sherds collected from two ancient neolithic sites in Niger (Tagalagal and Adrar Bous 10) has been dated by thermoluminescence. The natural radioactivity of these ceramics and of their surrounding sediments was measured using low background gamma spectrometry and atomic emission plasma spectrometry. With gamma spectrometry, the comparison between the activity of 238U (deduced from the 235U and 234Th gamma emissions) and that of 226Ra (deduced from 214Pb and 214Bi γ emissions in equilibrium with 222Rn) shows a significant disequilibrium of the U-series. The activity ratio {38U}/{226Ra}, which is greater than unity in this case, is interpreted as a result of either uranium enrichment ( 234U, 235U, 238U) or radium impoverishment that has been occurring since the burying of the archaeological artefacts. The effects of the changes in radiochemical composition on the annual dose are discussed and various determinations of the annual dose are analysed according to different hypotheses of disequilibrium (either permanent state or recent occurrence). The TL results: Tagalagal — 9820±780-10, 180±780 years/1993, Adrar Bous 10 — 9530±750-10,500±730 years/1993, are consistent with the radiocarbon dates obtained from charcoals collected at the same locations (the uncalibrated 14C dates belong to the 9100-9370 BP range). These results are of fundamental interest for the chronology of early neolithic cultures.

  10. 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.

  11. 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.

  12. Equilibrium uranium isotope fractionation by nuclear volume and mass-dependent processes

    NASA Astrophysics Data System (ADS)

    Schauble, E. A.

    2006-12-01

    Uranium serves as a geochemical tracer of oxidation near the Earth's surface, and is also the basis for several isotopic geochronometers. It is thus important to understand possible non-radiogenic and non-radioactive isotopic fractionation of uranium in natural systems. This study presents theoretical estimates of equilibrium uranium isotope fractionations in U-bearing molecules and complexes, calculated using first-principles computational chemistry. Ion-exchange experiments (1,2) have indicated that mass-dependent mechanisms, alone, cannot explain 238U/234U and 238U/^{235}U fractionations, so nuclear volume (i.e., field shift) fractionation effects are also considered in theoretical calculations. The results indicate that equilibrium isotopic fractionation is likely when U4+ and U6+ species equilibrate. Nuclear volume fractionation leads to higher 238U/^{235}U in U4+-bearing species, overwhelming a smaller mass- dependent fractionation in the opposite direction. The calculated net fractionation between U(H2O)_94+ and UO2Cl3(H2O)_2^- is approximately 1 per mil at 20-150°C, in agreement with earlier experiments. These results also reproduce the apparent non mass-dependent signature observed in 238U/234U relative to 238U/^{235}U. In addition to redox reactions, significant fractionation is expected between different U6+-bearing uranyl complexes (e.g., UO2(H2O)_52+, UO2(NO3)_3^-, UO2(CO3)(H2O)3). These results suggest that U-isotope composition could be used as a proxy for the oxidation state and speciation of natural waters, and that U-isotope ratios are not constant in materials formed or equilibrated at low temperatures. More generally, nuclear volume fractionations are expected to partially cancel or reverse mass-dependent fractionations caused by redox transitions among the high oxidation states (≥+2) of lanthanides, actinides, and heavy transition elements. References: 1. Nomura, Higuchi and Fujii, 1996, J. Am. Chem. Soc., v. 118, p. 9127-9130. 2. Bigeleisen

  13. DETERMINATION OF REPORTABLE RADIONUCLIDES FOR DWPF SLUDGE BATCH 7B (MACROBATCH 9)

    SciTech Connect

    Crawford, C. L.; Diprete, D. P.

    2014-05-01

    The Waste Acceptance Product Specifications (WAPS) 1.2 require that “The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115”. As part of the strategy to comply with WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production through the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu- 242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the heel from Sludge Batch 7a (SB7a) and Sludge Batch 7b (SB7b) that was transferred to Tank 40 from Tank 51. The blend of sludge in Tank 40 is also referred to as Macrobatch 9 (MB9). This report develops the list of reportable radionuclides and associated activities as a function of time. The DWPF will use this list and the activities as one of the inputs for the development of the Production Records that relate to

  14. Determination Of Reportable Radionuclides For DWPF Sludge Batch 7B (Macrobatch 9)

    SciTech Connect

    Crawford, C. L.; DiPrete, D. P.

    2013-08-22

    The Waste Acceptance Product Specifications (WAPS) 1.2 require that “The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115”. As part of the strategy to comply with WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production through the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the heel from Sludge Batch 7a (SB7a) and Sludge Batch 7b (SB7b) that was transferred to Tank 40 from Tank 51. The blend of sludge in Tank 40 is also referred to as Macrobatch 9 (MB9). This report develops the list of reportable radionuclides and associated activities as a function of time. The DWPF will use this list and the activities as one of the inputs for the development of the Production Records that relate to

  15. DETERMINATION OF REPORTABLE RADIONUCLIDES FOR DWPF SLUDGE BATCH 4 MACROBATCH 5

    SciTech Connect

    Bannochie, C; Ned Bibler, N; David Diprete, D

    2008-05-30

    The Waste Acceptance Product Specifications (WAPS)1 1.2 require that 'The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115'. As part of the strategy to meet WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production through the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP)2 and Waste Form Qualification Report (WQR)3. However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the previous contents of Tank 40 (Sludge Batch 3) and the sludge that was transferred to Tank 40 from Tank 51. The blend of sludge from Tank 51 and Tank 40 defines Sludge Batch 4 (also referred to as Macrobatch 5 (MB5)). This report develops the list of reportable radionuclides and associated activities and determines the radionuclide activities as a function of time. The DWPF will use this list and the activities as one of

  16. Results of Characterization and Retrieval Testing on Tank 241-C-110 Heel Solids

    SciTech Connect

    Callaway, William S.

    2013-09-30

    dissolution tests. Most of the {sup 99}Tc and {sup 137}Cs present in the initial heel solids composites was removed in the water dissolution tests. The estimated activities/weights of {sup 129}I, {sup 234}U, {sup 235}U, {sup 236}U, and {sup 238}U in the dry residual solids were <25% of the weights/activities in the initial composite solids. Gibbsite and nordstrandite [both Al(OH){sub 3}] were the major solid phases identified in the solids remaining after completion of the dissolution tests. Chemical analysis indicated that the residual solids may have contained up to 62 wt% Al(OH){sub 3}. Significant quantities of unidentified phosphate-, iron-, bismuth-, silicon-, and strontium- bearing species were also present in the residual solids. The reference density of gibbsite (and nordstrandite) is 2.42 g/mL. The measured density of the residual solids, 2.65 g/mL, would be a reasonable value for solids containing gibbsite as the major component with minor quantities of other, higher density solids. Sieve analysis indicated that 22.2 wt% of the residual solids were discrete particles >710 μm in size, and 77.8 wt% were particulates <710 μm in size. Light-scattering measurements suggested that nearly all of the <710-μm particulates with diameters >12 μm were weakly bound aggregates of particles with diameters <2 μm. The <710-μm residual solids settled very slowly when dispersed in reagent water. The physical appearance of a suspension containing ≈0.4 vol% of the solids in pure water changed very little over a period of 46.5 hours. It should be noted that the distribution of particle sizes in the residual solids and the observed settling behavior were both strongly influenced by the procedures followed in the dissolution tests.

  17. DETERMINATION OF REPORTABLE RADIONUCLIDES FOR DWPF SLUDGE BATCH 5 (MACROBATCH 6)

    SciTech Connect

    Bannochie, C.; Bibler, N.; Diprete, D.

    2010-02-04

    The Waste Acceptance Product Specifications (WAPS) 1.2 require that ''The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115''. As part of the strategy to comply with WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production through the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the heel from Tank 40 (Sludge Batch 4 (SB4)), Sludge Batch 5 (SB5) that was transferred to Tank 40 from Tank 51, and H-Canyon Np transfers completed after the start of processing. The blend of sludge in Tank 40 is also referred to as Macrobatch 6 (MB6). This report develops the list of reportable radionuclides and associated activities and determines the radionuclide activities as a function of time. The DWPF will use

  18. DETERMINATION OF REPORTABLE RADIONUCLIDES FOR DWPF SLUDGE BATCH 6 (MACROBATCH 7)

    SciTech Connect

    Bannochie, C.; Diprete, D.

    2011-06-01

    The Waste Acceptance Product Specifications (WAPS) 1.2 require that 'The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115'. As part of the strategy to comply with WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production through the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the heel from Sludge Batch 5 (SB5) with H-Canyon Np transfers completed after the start of processing SB5, and Sludge Batch 6 (SB6) that was transferred to Tank 40 from Tank 51. The blend of sludge in Tank 40 is also referred to as Macrobatch 7 (MB7). This report develops the list of reportable radionuclides and associated activities as a function of time. The DWPF will use this list and the activities as one of the

  19. Uranium-series dating of corals in situ using laser-ablation MC-ICPMS

    NASA Astrophysics Data System (ADS)

    Potter, Emma-Kate; Stirling, Claudine H.; Wiechert, Uwe H.; Halliday, Alex N.; Spötl, Christoph

    2005-01-01

    The in situ U-series dating of corals has been achieved using laser-ablation multiple-collector inductively coupled plasma mass spectrometry (LA MC-ICPMS). Utilising a 193 nm excimer laser coupled to a Nu Instruments Nu Plasma equipped with multiple ion counters, percent-level analytical precision for 234U/238U and 230Th/238U is obtained. Approximately 70 [mu]g of carbonate is consumed during each analysis, containing approximately 0.2 ng of 238U, ~10 pg of 234U and less than 3 fg of 230Th. A two-cycle, fast magnet jumping procedure is adopted. In the first cycle 238U is measured in a Faraday collector while the low-abundance isotopes 234U, 232Th, and 230Th are measured simultaneously in ion counters. In the second cycle 235U is measured in an ion counter. All samples are bracketed with an isotopically characterised sample to correct for electron multiplier gain and variable elemental fractionation. U-series ages are then calculated from the measured 234U/238U and 230Th/238U. Here, we demonstrate the applicability of this technique by analysing a series of coral samples that have been previously characterised by conventional thermal ionisation mass spectrometry (TIMS) and solution-nebulisation multiple-collector ICP mass spectrometry. Excellent agreement is obtained with independent age estimates. The samples have varying degrees of preservation and ages ranging between <10 and 600 thousand years (ka). The age uncertainties achieved are +/-1 ka at 3 ka and +/-7 ka at 125 ka. Therefore the technique can be used to distinguish between major climatic sub-stages throughout the last 140,000 years spanning the last glacial-interglacial cycle, as recorded in coral reef terraces. The laser-ablation U-series results are independent of coral species. U-series age uncertainties are comparable to those attained using [alpha]-spectrometry but require ~104 times less sample and no chemical preparation.

  20. 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.

  1. Increasing the Accuracy in the Measurement of the Minor Isotopes of Uranium: Care in Selection of Reference Materials, Baselines and Detector Calibration

    NASA Astrophysics Data System (ADS)

    Poths, J.; Koepf, A.; Boulyga, S. F.

    2008-12-01

    The minor isotopes of uranium (U-233, U-234, U-236) are increasingly useful for tracing a variety of processes: movement of anthropogenic nuclides in the environment (ref 1), sources of uranium ores (ref 2), and nuclear material attribution (ref 3). We report on improved accuracy for U-234/238 and U-236/238 by supplementing total evaporation protocol TIMS measurement on Faraday detectors (ref 4)with multiplier measurement for the minor isotopes. Measurement of small signals on Faraday detectors alone is limited by noise floors of the amplifiers and accurate measurement of the baseline offsets. The combined detector approach improves the reproducibility to better than ±1% (relative) for the U-234/238 at natural abundance, and yields a detection limit for U-236/U-238 of <0.2 ppm. We have quantified contribution of different factors to the uncertainties associated with these peak jumping measurement on a single detector, with an aim of further improvement. The uncertainties in the certified values for U-234 and U-236 in the uranium standard NBS U005, if used for mass bias correction, dominates the uncertainty in their isotopic ratio measurements. Software limitations in baseline measurement drives the detection limit for the U-236/U-238 ratio. This is a topic for discussion with the instrument manufacturers. Finally, deviation from linearity of the response of the electron multiplier with count rate limits the accuracy and reproducibility of these minor isotope measurements. References: (1) P. Steier et al(2008) Nuc Inst Meth(B), 266, 2246-2250. (2) E. Keegan et al (2008) Appl Geochem 23, 765-777. (3) K. Mayer et al (1998) IAEA-CN-98/11, in Advances in Destructive and Non-destructive Analysis for Environmental Monitoring and Nuclear Forensics. (4) S. Richter and S. Goldberg(2003) Int J Mass Spectrom, 229, 181-197.

  2. 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.

  3. SPECT Imaging of Mice with 99mTc-Radiopharmaceuticals Obtained from 99Mo Produced by 100Mo(n,2n)99Mo and Fission of 235U

    NASA Astrophysics Data System (ADS)

    Hashimoto, Kazuyuki; Nagai, Yasuki; Kawabata, Masako; Sato, Nozomi; Hatsukawa, Yuichi; Saeki, Hideya; Motoishi, Shoji; Ohta, Masayuki; Konno, Chikara; Ochiai, Kentaro; Kawauchi, Yukimasa; Ohta, Akio; Shiina, Takayuki; Takeuchi, Nobuhiro; Ashino, Hiroki; Nakahara, Yuto

    2015-04-01

    The distribution of 99mTc-radiopharmaceutical in mouse was determined by single photon emission computed tomography (SPECT) for the first time using 99mTc, which was separated by thermochromatography from 99Mo produced via the 100Mo(n,2n)99Mo reaction with accelerator neutrons. The SPECT image was comparable to that obtained using the fission product 99Mo. Radionuclidic and radiochemical purities of the separated 99mTc and its aluminum concentration met the United States Pharmacopeia regulatory requirements for 99mTc from the fission product 99Mo. These results provide important evidence that the 99mTc-radiopharmaceutical formulated using the (n,2n) 99Mo can be a promising substitute for the fission product 99Mo. The current and forthcoming problem of ensuring a reliable and constant supply of 99Mo in Japan can be partially mitigated.

  4. Dose distributions in a human head phantom for neutron capture therapy using moderated neutrons from the 2.5 MeV proton-7Li reaction or from fission of 235U

    NASA Astrophysics Data System (ADS)

    Tanaka, Kenichi; Kobayashi, Tooru; Sakurai, Yoshinori; Nakagawa, Yoshinobu; Endo, Satoru; Hoshi, Masaharu

    2001-10-01

    The feasibility of neutron capture therapy (NCT) using an accelerator-based neutron source of the 7Li(p,n) reaction produced by 2.5 MeV protons was investigated by comparing the neutron beam tailored by both the Hiroshima University radiological research accelerator (HIRRAC) and the heavy water neutron irradiation facility in the Kyoto University reactor (KUR-HWNIF) from the viewpoint of the contamination dose ratios of the fast neutrons and the gamma rays. These contamination ratios to the boron dose were estimated in a water phantom of 20 cm diameter and 20 cm length to simulate a human head, with experiments by the same techniques for NCT in KUR-HWNIF and/or the simulation calculations by the Monte Carlo N-particle transport code system version 4B (MCNP-4B). It was found that the 7Li(p,n) neutrons produced by 2.5 MeV protons combined with 20, 25 or 30 cm thick D2O moderators of 20 cm diameter could make irradiation fields for NCT with depth-dose characteristics similar to those from the epithermal neutron beam at the KUR-HWNIF.

  5. 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

  6. 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.

  7. Actinides in deer tissues at the rocky flats environmental technology site.

    PubMed

    Todd, Andrew S; Sattelberg, R Mark

    2005-11-01

    Limited hunting of deer at the future Rocky Flats National Wildlife Refuge has been proposed in U.S. Fish and Wildlife planning documents as a compatible wildlife-dependent public use. Historically, Rocky Flats site activities resulted in the contamination of surface environmental media with actinides, including isotopes of americium, plutonium, and uranium. In this study, measurements of actinides [Americium-241 (241Am); Plutonium-238 (238Pu); Plutonium-239,240 (239,240Pu); uranium-233,244 (233,234U); uranium-235,236 (235,236U); and uranium-238 (238U)] were completed on select liver, muscle, lung, bone, and kidney tissue samples harvested from resident Rocky Flats deer (N = 26) and control deer (N = 1). In total, only 17 of the more than 450 individual isotopic analyses conducted on Rocky Flats deer tissue samples measured actinide concentrations above method detection limits. Of these 17 detects, only 2 analyses, with analytical uncertainty values added, exceeded threshold values calculated around a 1 x 10(-6) risk level (isotopic americium, 0.01 pCi/g; isotopic plutonium, 0.02 pCi/g; isotopic uranium, 0.2 pCi/g). Subsequent, conservative risk calculations suggest minimal human risk associated with ingestion of these edible deer tissues. The maximum calculated risk level in this study (4.73 x 10(-6)) is at the low end of the U.S. Environmental Protection Agency's acceptable risk range. PMID:16639905

  8. 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

  9. Analysis of Savannah Survey Sediment Collections of 30 Sep 04

    SciTech Connect

    Wimer, N; Hutcheon, I; Esser, B; Ramon, E

    2004-12-03

    This report summarizes laboratory radiochemical analyses of sediment samples collected by the Defense Threat Reduction Agency during the DoD Savannah Survey operations of Sep 04. The analytic goal was to determine if Wassaw Sound sediment collections of 30 Sep 04 display evidence for local anthropogenic uranium, as distinct from the recognized regional background stemming from the Savannah River Site (SRS). Radiochemical methods were selected to maximize detection sensitivity for such anthropogenic uranium. Within the suite of twelve collections, there would be evidence for a localized source if individual collections were to differ from the population as a whole. If in fact non-natural uranium were observed, definitive determination of whether the source was SRS effluent or a localized release would likely involve additional field sampling. These collections were logged by the LLNL Forensics Science Center, photographed, and laboratory chain-of-custody was begun. The inventory received at LLNL is reported in Table 1. The separate collections were not assigned any relative priority among them. LLNL has separately reviewed detailed records of the item in question, and determined what materials are involved and what radiochemical assays are of value. Attempting quantitative estimates of source-item material release, transport, and collection levels would be quite uncertain. Rather, present assays examine for departure from natural background isotopic compositions. To summarize the findings, analyses for all collections displayed natural uranium isotopic composition--considering the {sup 238}U/{sup 235}U and {sup 236}U/{sup 235}U ratios--within measurement uncertainties, which were quite low. No one collection or set of collections stood apart from the others in its uranium isotopes. These {sup 238}U/{sup 235}U data uncertainty levels also determined with 99.5% confidence (a three-standard-deviation determination) that no more than 0.46% of the total uranium present

  10. Applications of high resolution ICP-AES in the nuclear industry

    SciTech Connect

    Johnson, S.G.; Giglio, J.J.; Goodall, P.S.; Cummings, D.G.

    1998-07-01

    Application of high resolution ICP-AES to selected problems of importance in the nuclear industry is a growing field. The advantages in sample preparation time, waste minimization and equipment cost are considerable. Two examples of these advantages are presented in this paper, burnup analysis of spent fuel and analysis of major uranium isotopes. The determination of burnup, an indicator of fuel cycle efficiency, has been accomplished by the determination of {sup 139}La by high resolution inductively coupled plasma atomic emission spectroscopy (HR-ICP-AES). Solutions of digested samples of reactor fuel rods were introduced into a shielded glovebox housing an inductively coupled plasma (ICP) and the resulting atomic emission transmitted to a high resolution spectrometer by a 31 meter fiber optic bundle. Total and isotopic U determination by thermal ionization mass spectrometry (TIMS) is presented to allow for the calculation of burnup for the samples. This method of burnup determination reduces the time, material, sample handling and waste generated associated with typical burnup determinations which require separation of lanthanum from the other fission products with high specific activities. Work concerning an alternative burnup indicator, {sup 236}U, is also presented for comparison. The determination of {sup 235}U:{sup 238}U isotope ratios in U-Zr fuel alloys is also presented to demonstrate the versatility of HR-ICP-AES.

  11. Laser spectrometry and laser ablation - an ideal solution for the analysis of nuclear materials

    SciTech Connect

    Goodall, P.; Johnson, S.G.

    1996-09-01

    Nuclear materials, consisting primarily of actinides and lanthanides, produce a plethora of emission lines from the ICP. This provides an entertaining problem for the analyst applying ICP-AES. Laser ablation ICP-AES (LA-ICP-AES) offers unique advantages for the analysis of nuclear materials as it allows remote analysis of these materials in heavily shielded environments. The use of high resolution spectrometry, when coupled with LA-ICP-AES, simplifies the spectral chaos normally encountered with these materials. This obviates the requirement for analyte separation which standard ICP-AES instrumentation demands. Examples of the analysis of nuclear fuels and materials used in the reprocessing of that fuel will be presented (e.g., the determination of U, La, Y, Ce and Nd in molten salts.). In addition to bulk (or local) chemical composition, it is also possible to extract isotopic information using high resolution LA-ICP-AES (e.g., the determination of {sup 236}U for the estimation of {open_quotes}burn-up{close_quotes} of {sup 235}U in a nuclear reactor). Laser excited atomic fluorescence (LEAFS) has the advantage of high specificity at the expense of instrumental sophistication but provides one solution to the spectral complexity encountered with nuclear materials. The potential of laser ablation coupled to ICP-LEAFS will be discussed and the determination of lanthanides by LA-ICP-LEAFS described.

  12. Spent fuel temperature and age determination from the analysis of uranium and plutonium isotopics

    SciTech Connect

    Scott, Mark R; Eccleston, George W; Bedell, Jeffrey J; Lockard, Chanelle M

    2009-01-01

    The capability to determine the age (time since irradiation) of spent fuel can be useful for verification and safeguards. While the age of spent fuel can be determined based on measurements of short-lived fission products, these measurements are not routinely done nor generally reported. As an alternative, age can also be determined if the uranium (U) and plutonium (Pu) isotopic values are available. Uranium isotopics are not strongly affected by fuel temperature, and bumup is determined from the {sup 235}U and {sup 236}U isotopic values. Age is calculated after estimating the {sup 241}Pu at the end of irradiation while accounting for the fuel temperature, which is determined from {sup 239}Pu or {sup 240}Pu. Burnup and age determinations are calibrated to reactor models that provide uranium and plutonium isotopics over the range of fuel irradiation. The reactor model must contain sufficient fidelity on details of the reactor type, fuel burnup, irradiation history, initial fuel enrichment and fuel temperature to obtain accurate isotopic calculations. If the latter four are unknown, they can be derived from the uranium and plutonium isotopics. Fuel temperature has a significant affect on the production of plutonium isotopics; therefore, one group cross section reactor models, such as ORIGEN, cannot be used for these calculations. Multi-group cross section set codes, such as Oak Ridge National Laboratory's TRITON code, must be used.

  13. Survey of plutonium and uranium atom ratios and activity levels in Mortandad Canyon

    SciTech Connect

    Gallaher, B.M.; Efurd, D.W.; Rokop, D.J.; Benjamin, T.M.; Stoker, A.K.

    1997-10-01

    For more than three decades, Mortandad Canyon has been the primary release area of treated liquid radioactive waste from the Los Alamos National Laboratory (Laboratory). In this survey, six water samples and seven stream sediment samples collected in Mortandad Canyon were analyzed by thermal ionization mass spectrometry to determine the plutonium and uranium activity levels and atom ratios. By measuring the {sup 240}Pu/{sup 239}Pu atom ratios, the Laboratory plutonium component was evaluated relative to that from global fallout. Measurements of the relative abundance of {sup 235}U and {sup 236}U were also used to identify non-natural components. The survey results indicate that the Laboratory plutonium and uranium concentrations in waters and sediments decrease relatively rapidly with distance downstream from the major industrial sources. Plutonium concentrations in shallow alluvial groundwater decrease by approximately 1,000-fold along a 3,000-ft distance. At the Laboratory downstream boundary, total plutonium and uranium concentrations were generally within regional background ranges previously reported. Laboratory-derived plutonium is readily distinguished from global fallout in on-site waters and sediments. The isotopic ratio data indicate off-site migration of trace levels of Laboratory plutonium in stream sediments to distances approximately two miles downstream of the Laboratory boundary.

  14. Survey of plutonium and uranium atom ratios and activity levels in Mortandad Canyon

    SciTech Connect

    Gallaher, B.M.; Benjamin, T.M.; Rokop, D.J.; Stoker, A.K.

    1997-09-22

    For more than three decades Mortandad Canyon has been the primary release area of treated liquid radioactive waste from the Los Alamos National Laboratory (Laboratory). In this survey, six water samples and seven stream sediment samples collected in Mortandad Canyon were analyzed by thermal ionization mass spectrometry (TIMS) to determine the plutonium and uranium activity levels and atom ratios. Be measuring the {sup 240}Pu/{sup 239}Pu atom ratios, the Laboratory plutonium component was evaluated relative to that from global fallout. Measurements of the relative abundance of {sup 235}U and {sup 236}U were also used to identify non-natural components. The survey results indicate the Laboratory plutonium and uranium concentrations in waters and sediments decrease relatively rapidly with distance downstream from the major industrial sources. Plutonium concentrations in shallow alluvial groundwater decrease by approximately 1000 fold along a 3000 ft distance. At the Laboratory downstream boundary, total plutonium and uranium concentrations were generally within regional background ranges previously reported. Laboratory derived plutonium is readily distinguished from global fallout in on-site waters and sediments. The isotopic ratio data indicates off-site migration of trace levels of Laboratory plutonium in stream sediments to distances approximately two miles downstream of the Laboratory boundary.

  15. Capture and fission with DANCE and NEUANCE

    DOE PAGESBeta

    Jandel, M.; Baramsai, B.; Bond, E.; Rusev, G.; Walker, C.; Bredeweg, T. A.; Chadwick, M. B.; Couture, A.; Fowler, M. M.; Hayes, A.; et al

    2015-12-23

    A summary of the current and future experimental program at DANCE is presented. Measurements of neutron capture cross sections are planned for many actinide isotopes with the goal to reduce the present uncertainties in nuclear data libraries. Detailed studies of capture gamma rays in the neutron resonance region will be performed in order to derive correlated data on the de-excitation of the compound nucleus. New approaches on how to remove the DANCE detector response from experimental data and retain the correlations between the cascade gamma rays are presented. Studies on 235U are focused on quantifying the population of short-lived isomericmore » states in 236U after neutron capture. For this purpose, a new neutron detector array NEUANCE is under construction. It will be installed in the central cavity of the DANCE array and enable the highly efficient tagging of fission and capture events. In addition, developments of fission fragment detectors are also underway to expand DANCE capabilities to measurements of fully correlated data on fission observables.« less

  16. SOFIA, a Next-Generation Facility for Fission Yields Measurements and Fission Study. First Results and Perspectives

    NASA Astrophysics Data System (ADS)

    Audouin, L.; Pellereau, E.; Taieb, J.; Boutoux, G.; Béliera, G.; Chatillon, A.; Ebran, A.; Gorbinet, T.; Laurent, B.; Martin, J.-F.; Tassan-Got, L.; Jurado, B.; Alvarez-Pol, H.; Ayyad, Y.; Benlliure, J.; Caamano, M.; Cortina-Gil, D.; Fernandez-Dominguez, B.; Paradela, C.; Rodriguez-Sanchez, J.-L.; Vargas, J.; Casarejos, E.; Heinz, A.; Kelic-Heil, A.; Kurz, N.; Nociforo, C.; Pietri, S.; Prochazka, A.; Rossi, D.; Schmidt, K.-H.; Simon, H.; Voss, B.; Weick, H.; Winfield, J. S.

    2015-10-01

    Fission fragments play an important role in nuclear reactors evolution and safety. However, fragments yields are poorly known : data are essentially limited to mass yields from thermal neutron-induced fissions on a very few nuclei. SOFIA (Study On FIssion with Aladin) is an innovative experimental program on nuclear fission carried out at the GSI facility, which aims at providing isotopic yields on a broad range of fissioning systems. Relativistic secondary beams of actinides and pre-actinides are selected by the Fragment Separator (FRS) and their fission is triggered by electromagnetic interaction. The resulting excitation energy is comparable to the result of an interaction with a low-energy neutron, thus leading to useful data for reactor simulations. For the first time ever, both fission fragments are completely identified in charge and mass in a new recoil spectrometer, allowing for precise yields measurements. The yield of prompt neutrons can then be deduced, and the fission mechanism can be ascribed, providing new constraints for fission models. During the first experiment, all the technical challenges were matched : we have thus set new experimental standards in the measurements of relativistic heavy ions (time of flight, position, energy loss).This communication presents a first series of results obtained on the fission of 238U; many other fissioning systems have also been measured and are being analyzed presently. A second SOFIA experiment is planned in September 2014, and will be focused on the measurement of the fission of 236U, the analog of 235U+n.

  17. Capture and fission with DANCE and NEUANCE

    NASA Astrophysics Data System (ADS)

    Jandel, M.; Baramsai, B.; Bond, E.; Rusev, G.; Walker, C.; Bredeweg, T. A.; Chadwick, M. B.; Couture, A.; Fowler, M. M.; Hayes, A.; Kawano, T.; Mosby, S.; Stetcu, I.; Taddeucci, T. N.; Talou, P.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.

    2015-12-01

    A summary of the current and future experimental program at DANCE is presented. Measurements of neutron capture cross sections are planned for many actinide isotopes with the goal to reduce the present uncertainties in nuclear data libraries. Detailed studies of capture gamma rays in the neutron resonance region will be performed in order to derive correlated data on the de-excitation of the compound nucleus. New approaches on how to remove the DANCE detector response from experimental data and retain the correlations between the cascade gamma rays are presented. Studies on 235U are focused on quantifying the population of short-lived isomeric states in 236U after neutron capture. For this purpose, a new neutron detector array NEUANCE is under construction. It will be installed in the central cavity of the DANCE array and enable the highly efficient tagging of fission and capture events. In addition, developments of fission fragment detectors are also underway to expand DANCE capabilities to measurements of fully correlated data on fission observables.

  18. 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.

  19. 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.

  20. 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. PMID:19362761

  1. Rapid determination of uranium isotopes in urine by inductively coupled plasma-mass spectrometry.

    PubMed

    Shi, Y; Dai, X; Collins, R; Kramer-Tremblay, S

    2011-08-01

    Following a radiological or nuclear emergency involving uranium exposure, rapid analytical methods are needed to analyze the concentration of uranium isotopes in human urine samples for early dose assessment. The inductively coupled plasma mass spectrometry (ICP-MS) technique, with its high sample throughput and high sensitivity, has advantages over alpha spectrometry for uranium urinalysis after minimum sample preparation. In this work, a rapid sample preparation method using an anion exchange chromatographic column was developed to separate uranium from the urine matrix. A high-resolution sector field ICP-MS instrument, coupled with a high sensitivity desolvation sample introduction inlet, was used to determine uranium isotopes in the samples. The method can analyze up to 24 urine samples in two hours with the limits of detection of 0.0014, 0.10, and 2.0 pg mL(-1) for (234)U, (235)U, and (238)U, respectively, which meet the requirement for isotopic analysis of uranium in a radiation emergency. PMID:21709502

  2. 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.

  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. The ability of Helianthus annuus L. and Brassica juncea to uptake and translocate natural uranium and 226Ra under different milieu conditions.

    PubMed

    Vera Tomé, F; Blanco Rodríguez, P; Lozano, J C

    2009-01-01

    Seedlings of Helianthus annuus L. (HA) and Brassica juncea (BJ) were used to test the effect of the pH, the presence of phosphates, and the addition of ethylene-diamine-tetraacetic acid (EDTA) or citrate on the uptake and the translocation of uranium isotopes ((238)U, (235)U, and (234)U) and (226)Ra. The results indicated that the presence of phosphates generally reduces the uptake and transfer of uranium from the roots to the shoots of HA. In the case of BJ, while phosphate enhanced the retention of uranium by roots, the translocation was poorer. Likewise, for (226)Ra, the best translocation was in the absence of phosphates for both species. The addition of citrate increased the translocation of uranium for both species, but had no clear effect on the transfer of (226)Ra. The effect of EDTA was much more moderate both for uranium and for (226)Ra, and for both plant species. Only noticeable was a slightly better uptake of (226)Ra by BJ at neutral pH, although the translocation was lower. PMID:18848715

  5. Distribution of naturally occurring radionuclides (U, Th) in Timahdit black shale (Morocco).

    PubMed

    Galindo, C; Mougin, L; Fakhi, S; Nourreddine, A; Lamghari, A; Hannache, H

    2007-01-01

    Attention has been focused recently on the use of Moroccan black oil shale as the raw material for production of a new type of adsorbent and its application to U and Th removal from contaminated wastewaters. The purpose of the present work is to provide a better understanding of the composition and structure of this shale and to determine its natural content in uranium and thorium. A black shale collected from Timahdit (Morocco) was analyzed by powder X-ray diffraction and SEM techniques. It was found that calcite, dolomite, quartz and clays constitute the main composition of the inorganic matrix. Pyrite crystals are also present. A selective leaching procedure, followed by radiochemical purification and alpha-counting, was performed to assess the distribution of naturally occurring radionuclides. Leaching results indicate that 238U, 235U, 234U, 232Th, 230Th and 228Th have multiple modes of occurrence in the shale. U is interpreted to have been concentrated under anaerobic conditions. An integrated isotopic approach showed the preferential mobilization of uranium carried by humic acids to carbonate and apatite phases. Th is partitioned between silicate minerals and pyrite. PMID:17098337

  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. 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.

  8. 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.

  9. 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.

  10. 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.

  11. 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. PMID:24274286

  12. Natural radioactivity, dose assessment and uranium uptake by agricultural crops at Khan Al-Zabeeb, Jordan.

    PubMed

    Al-Kharouf, Samer J; Al-Hamarneh, Ibrahim F; Dababneh, Munir

    2008-07-01

    Khan Al-Zabeeb, an irrigated cultivated area lies above a superficial uranium deposits, is regularly used to produce vegetables and fruits consumed by the public. Both soil and plant samples collected from the study area were investigated for their natural radioactivity to determine the uranium uptake by crops and hence to estimate the effective dose equivalent to human consumption. Concentrations of (238)U, (235)U, (232)Th, (226)Ra, (222)Rn, (137)Cs and (40)K in nine soil profiles were measured by gamma-ray spectrometry whereas watermelon and zucchini crops were analyzed for their uranium content by means of alpha spectrometry after radiochemical separation. Correlations between measured radionuclides were made and their activity ratios were determined to evaluate their geochemical behavior in the soil profiles. Calculated soil-plant transfer factors indicate that the green parts (leaves, stems and roots) of the studied crops tend to accumulate uranium about two orders of magnitude higher than the fruits. The maximum dose from ingestion of 1 kg of watermelon pulp was estimated to be 3.1 and 4.7 nSv y(-1) for (238)U and (234)U, respectively. Estimations of the annual effective dose equivalent due to external exposure showed extremely low values. Radium equivalent activity and external hazard index were seen to exceed the permissible limits of 370 Bq kg(-1) and 1, respectively. PMID:18359539

  13. Evaluation of in vivo and in vitro dose detection limits for different radionuclides and measurement techniques.

    PubMed

    Bitar, A; Maghrabi, M; Doubal, A W

    2016-07-01

    Personal monitoring programs for workers handling radioactive materials are influenced by numerous factors as the measurements of radioactivity in tissues or/and in excreta can be carried out using different techniques. This paper summaries the basic procedures needed for accurate and fast measurement of different radionuclides like (235)U, (234)U, (238)U, (226)Ra, (210)Po, (131)I, (99m)Tc, (134)Cs, (137)Cs, (57)Co, (58)Co, and (60)Co. Overviews of in vitro and in vivo monitoring methods are provided as well as methods used to calculate detection limits and internal radiation dose. For the radionuclides of interest, in vivo and in vitro detection limits were converted into committed effective doses to evaluate the applicability and limitations of the systems used at the laboratory. The results proved that the systems' sensitivity is suitable for use in routine monitoring of workers subject to risk of internal exposure from such radionuclides. Consequently, monitoring programs suggested by the Syrian internal dosimetry laboratory are suitable to detect committed effective doses even below 1mSv in most cases. PMID:27108068

  14. Innovations in Mass Spectrometry for Precise and Accurate Isotope Ratio Determination from Very Small Analyte Quantities (Invited)

    NASA Astrophysics Data System (ADS)

    Lloyd, N. S.; Bouman, C.; Horstwood, M. S.; Parrish, R. R.; Schwieters, J. B.

    2010-12-01

    This presentation describes progress in mass spectrometry for analysing very small analyte quantities, illustrated by example applications from nuclear forensics. In this challenging application, precise and accurate (‰) uranium isotope ratios are required from 1 - 2 µm diameter uranium oxide particles, which comprise less than 40 pg of uranium. Traditionally these are analysed using thermal ionisation mass spectrometry (TIMS), and more recently using secondary ionisation mass spectrometry (SIMS). Multicollector inductively-coupled plasma mass spectrometry (MC-ICP-MS) can offer higher productivity compared to these techniques, but is traditionally limited by low efficiency of analyte utilisation (sample through to ion detection). Samples can either be introduced as a solution, or sampled directly from solid using laser ablation. Large multi-isotope ratio datasets can help identify provenance and intended use of anthropogenic uranium and other nuclear materials [1]. The Thermo Scientific NEPTUNE Plus (Bremen, Germany) with ‘Jet Interface’ option offers unparalleled MC-ICP-MS sensitivity. An analyte utilisation of c. 4% has previously been reported for uranium [2]. This high-sensitivity configuration utilises a dry high-capacity (100 m3/h) interface pump, special skimmer and sampler cones and a desolvating nebuliser system. Coupled with new acquisition methodologies, this sensitivity enhancement makes possible the analysis of micro-particles and small sample volumes at higher precision levels than previously achieved. New, high-performance, full-size and compact discrete dynode secondary electron multipliers (SEM) exhibit excellent stability and linearity over a large dynamic range and can be configured to simultaneously measure all of the uranium isotopes. Options for high abundance-sensitivity filters on two ion beams are also available, e.g. for 236U and 234U. Additionally, amplifiers with high ohm (1012 - 1013) feedback resistors have been developed to

  15. 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

  16. Benchmark Evaluation of the NRAD Reactor LEU Core Startup Measurements

    SciTech Connect

    J. D. Bess; T. L. Maddock; M. A. Marshall

    2011-09-01

    The Neutron Radiography (NRAD) reactor is a 250-kW TRIGA-(Training, Research, Isotope Production, General Atomics)-conversion-type reactor at the Idaho National Laboratory; it is primarily used for neutron radiography analysis of irradiated and unirradiated fuels and materials. The NRAD reactor was converted from HEU to LEU fuel with 60 fuel elements and brought critical on March 31, 2010. This configuration of the NRAD reactor has been evaluated as an acceptable benchmark experiment and is available in the 2011 editions of the International Handbook of Evaluated Criticality Safety Benchmark Experiments (ICSBEP Handbook) and the International Handbook of Evaluated Reactor Physics Benchmark Experiments (IRPhEP Handbook). Significant effort went into precisely characterizing all aspects of the reactor core dimensions and material properties; detailed analyses of reactor parameters minimized experimental uncertainties. The largest contributors to the total benchmark uncertainty were the 234U, 236U, Er, and Hf content in the fuel; the manganese content in the stainless steel cladding; and the unknown level of water saturation in the graphite reflector blocks. A simplified benchmark model of the NRAD reactor was prepared with a keff of 1.0012 {+-} 0.0029 (1s). Monte Carlo calculations with MCNP5 and KENO-VI and various neutron cross section libraries were performed and compared with the benchmark eigenvalue for the 60-fuel-element core configuration; all calculated eigenvalues are between 0.3 and 0.8% greater than the benchmark value. Benchmark evaluations of the NRAD reactor are beneficial in understanding biases and uncertainties affecting criticality safety analyses of storage, handling, or transportation applications with LEU-Er-Zr-H fuel.

  17. 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.

  18. 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

  19. Effect of Radium mobility on the U-Pb systematic and age determination of uraninite.

    NASA Astrophysics Data System (ADS)

    Deloule, Etienne; Brouand, Marc

    2014-05-01

    The U-Pb radio chronometer is commonly used to date the formation of uraninite, a major component of uranium deposit. Uraninite was first used in 1905, when Rutherford determines ages up to 500 Ma in using their He/U ratio, and in 1907 when Boltwood determine the first U-Pb ages (413-535 Ma). During the last decade, in situ U-Pb datation on Uraninite has been developed, either in using 'chemical ages' with the determination by EMP of U and Pb contents, either in using 'isotopic ages' with the determination of Pb and U isotopic ratios and contents by SIMS, providing a large amount of age from archean up to Cenozoic ages. It is noticeable that the determination of chemical age relies on the assumption that the U-Pb system stay closed over time. This assumption can be supported by many isotopic measurements providing concordant or close to concordance 238U-206Pb and 235U-207Pb ages. However, during the last year, SIMS U-Pb age determination on Uraninite from the Imouraren (Niger) uranium deposit provides contrasted results. On one hand, samples provide concordant U-Pb ages with an average value of 99 ±2 Ma. On the other hand, samples provide largely discordant ages, with 207Pb/206Pb ages up to 340 Ma. Duplicated measurements and careful data examination allowed us to discard any common lead contamination as a source of discordance. Therefore we set the in situ measurement of the U series nuclides 238U - 234U - 230Th - 226Ra. The high transmission at high mass resolution of the CRPG -Cameca IMS 1270 ion microprobe allowed us to get significant secondary beam intensities for the smaller isotopes and to determine the activity ratios with a few % precision. These measurements points out that 234U and 230Th are at equilibrium with 238U, when 226Ra may be largely depleted, up to 50%. This points out that in the geological context of the deposit, hydrothermal fluids may leach Ra. To explain the observed discordant ages, Ra should have been lost during a large amount of time

  20. 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.

  1. Radiation doses to members of the U.S. population from ubiquitous radionuclides in the body: Part 1, autopsy and in vivo data.

    PubMed

    Watson, David J; Strom, Daniel J

    2011-04-01

    This paper is Part 1 of a three-part series investigating steady-state effective dose rates 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 (222)Rn, (220)Rn, and their short-lived decay products; it also excludes intakes of radionuclides in occupational and medical settings. In this work, it is assumed that instantaneous dose rates in target organs are proportional to steady-state radionuclide concentrations in source regions. The goal of Part 1 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 (238)U series (14 nuclides), the actinium series (headed by (235)U; 11 nuclides), and the (232)Th series (11 nuclides); primordial radionuclides (87)Rb and (40)K; cosmogenic and fallout radionuclides (14)C and (3)H; and purely anthropogenic radionuclides (137)Cs-(137m)Ba, (129)I, and (90)Sr-(90)Y. Measurements judged to be relevant were available for only 15 of these radionuclides: (238)U, (235)U, (234)U, (232)Th, (230)Th, (228)Th, (228)Ra, (226)Ra, (210)Pb, (210)Po, (137)Cs, (87)Rb, (40)K, (14)C, and (3)H. Recent and relevant measurements were not available for (129)I and (90)Sr-(90)Y. A total of 11,741 radionuclide concentration measurements were found in one or more tissues or organs from 14 states. Data on age, gender, 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

  2. Analysis of HEU samples from the ULBA Metallurgical Plant

    SciTech Connect

    Gift, E.H.

    1995-05-01

    In early March 1994, eight highly enriched uranium (HEU) samples were collected from materials stored at the Ulba Metallurgical Plant in Oskamen (Ust Kamenogorsk), Kazakhstan. While at the plant site, portions of four samples were dissolved and analyzed by mass spectrograph at the Ulba analytical laboratory by Ulba analysts. Three of these mass spectrograph solutions and the eight HEU samples were subsequently delivered to the Y-12 Plant for complete chemical and isotopic analyses. Chemical forms of the eight samples were uranium metal chips, U0{sub 2} powder, uranium/beryllium oxide powder, and uranium/beryllium alloy rods. All were declared by the Ulba plant to have a uranium assay of {approximately}90 wt % {sup 235}U. The uranium/beryllium powder and alloy samples were also declared to range from about 8 to 28 wt % uranium. The chemical and uranium isotopic analyses done at the Y-12 Plant confirm the Ulba plant declarations. All samples appear to have been enriched using some reprocessed uranium, probably from recovery of uranium from plutonium production reactors. As a result, all samples contain some {sup 236}U and {sup 232}U and have small but measurable quantities of plutonium. This plutonium could be the result of either contamination carried over from the enrichment process or cross-contamination from weapons material. It is not the result of direct reactor exposure. Neither the {sup 232}U nor the plutonium concentrations are sufficiently high to provide a significant industrial health hazard. Both are well within established or proposed acceptance criteria for storage at Y-12. The trace metal analyses showed that, with the exception of beryllium, there are no trace metals in any of these HEU samples that pose a significant health hazard.

  3. Analysis of the Reuse of Uranium Recovered from the Reprocessing of Commercial LWR Spent Fuel

    SciTech Connect

    DelCul, Guillermo Daniel; Trowbridge, Lee D; Renier, John-Paul; Ellis, Ronald James; Williams, Kent Alan; Spencer, Barry B; Collins, Emory D

    2009-02-01

    This report provides an analysis of the factors involved in the reuse of uranium recovered from commercial light-water-reactor (LWR) spent fuels (1) by reenrichment and recycling as fuel to LWRs and/or (2) by recycling directly as fuel to heavy-water-reactors (HWRs), such as the CANDU (registered trade name for the Canadian Deuterium Uranium Reactor). Reuse is an attractive alternative to the current Advanced Fuel Cycle Initiative (AFCI) Global Nuclear Energy Partnership (GNEP) baseline plan, which stores the reprocessed uranium (RU) for an uncertain future or attempts to dispose of it as 'greater-than-Class C' waste. Considering that the open fuel cycle currently deployed in the United States already creates a huge excess quantity of depleted uranium, the closed fuel cycle should enable the recycle of the major components of spent fuel, such as the uranium and the hazardous, long-lived transuranic (TRU) actinides, as well as the managed disposal of fission product wastes. Compared with the GNEP baseline scenario, the reuse of RU in the uranium fuel cycle has a number of potential advantages: (1) avoidance of purchase costs of 11-20% of the natural uranium feed; (2) avoidance of disposal costs for a large majority of the volume of spent fuel that is reprocessed; (3) avoidance of disposal costs for a portion of the depleted uranium from the enrichment step; (4) depending on the {sup 235}U assay of the RU, possible avoidance of separative work costs; and (5) a significant increase in the production of {sup 238}Pu due to the presence of {sup 236}U, which benefits somewhat the transmutation value of the plutonium and also provides some proliferation resistance.

  4. Oxidation states of uranium in depleted uranium particles from Kuwait.

    PubMed

    Salbu, B; Janssens, K; Lind, O C; Proost, K; Gijsels, L; Danesi, P R

    2005-01-01

    The oxidation states of uranium in depleted uranium (DU) particles were determined by synchrotron radiation based mu-XANES, applied to individual particles isolated from selected samples collected at different sites in Kuwait. Based on scanning electron microscopy with X-ray microanalysis prior to mu-XANES, DU particles ranging from submicrons to several hundred micrometers were observed. The median particle size depended on sources and sampling sites; small-sized particles (median 13 microm) were identified in swipes taken from the inside of DU penetrators holes in tanks and in sandy soil collected below DU penetrators, while larger particles (median 44 microm) were associated with fire in a DU ammunition storage facility. Furthermore, the (236)U/(235)U ratios obtained from accelerator mass spectrometry demonstrated that uranium in the DU particles originated from reprocessed fuel (about 10(-2) in DU from the ammunition facility, about 10(-3) for DU in swipes). Compared to well-defined standards, all investigated DU particles were oxidized. Uranium particles collected from swipes were characterized as UO(2), U(3)O(8) or a mixture of these oxidized forms, similar to that observed in DU affected areas in Kosovo. Uranium particles formed during fire in the DU ammunition facility were, however, present as oxidation state +5 and +6, with XANES spectra similar to solid uranyl standards. Environmental or health impact assessments for areas affected by DU munitions should therefore take into account the presence of respiratory UO(2), U(3)O(8) and even UO(3) particles, their corresponding weathering rates and the subsequent mobilisation of U from oxidized DU particles. PMID:15511555

  5. 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.

  6. 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

  7. 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. PMID:23514714

  8. A comparative experimental study of gross alpha methods in natural waters.

    PubMed

    Montaña, M; Fons, J; Corbacho, J A; Camacho, A; Zapata-García, D; Guillén, J; Serrano, I; Tent, J; Baeza, A; Llauradó, M; Vallés, I

    2013-04-01

    The aim of the present work was to compare the results obtained with gross alpha methods such as evaporation, co-precipitation and total evaporation by liquid scintillation counting and to check whether these results are representative of the real total alpha activity concentration on the sample. The study was carried out on eight natural waters with very different radioactive characteristics. For all the samples uranium ((238)U, (235)U, and (234)U), radium ((226)Ra and (224)Ra), (210)Po, and (232)Th isotopes were also assayed by using radiochemical separation and alpha spectrometry in order to determine the sum of the activities of these alpha emitters. Precision (expressed as relative standard deviation) was below 28% for evaporation and below 18% for co-precipitation. In the case of total by liquid scintillation counting it was below 10% for samples with Total Alpha activity above 0.1 Bq/L (this value is about three times the MDA). Furthermore, for most of the studied waters, the Total Alpha activity and the gross alpha activity determined by the three methods were comparable. The obtained bias by the evaporation, co-precipitation, and total evaporation by liquid scintillation counting methods was lower than 40%, 25% and 20%, respectively. The ANOVA test was applied to find out if there was significant variability among the methods. For the samples with the most common radiochemical characteristics there were no significant differences among the three studied methods. However differences were detected for samples with a high saline content or with a very low activity level. PMID:23220539

  9. 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)

  10. Actinide-series disequilibrium as a tool to establish the chronology of deep-sea hydrothermal activity

    SciTech Connect

    Lalou, C.; Reyss, J.L.; Brichet, E. )

    1993-03-01

    This paper describes the different radiochronological methods used to date geologically recent (i.e., <400,000 years) deep-sea hydrothermal deposits as well as the basic conditions necessary to obtain reliable dates. The limitations of the different techniques also are described. Using measurements of [sup 210]Pb/Pb, [sup 228]Th/[sup 228]Ra, [sup 230]Th/[sup 234]U, [sup 231]Pa/[sup 235]U, and [sup 228]Ra/[sup 226]Ra, the authors have undertaken an exhaustive chronological study of the hydrothermal deposits along the East Pacific Rise, the Mid-Atlantic Ridge, and in some back-arc basins. The objectives of this study were to obtain regional chronologies and to establish a general synthesis on the evolution of the hydrothermal processes at the scale of the mid-oceanic ridge system. Some results obtained by other authors are included in this synthesis. The dependence of the general trends of temporal development of the hydrothermal chimneys, edifices, and fields on their tectonic settings is discussed. This study demonstrates that hydrothermal activity does not represent a regular input of matter to the ocean, and that its pulsed character must be taken into account in all modeling attempts (chemical, biological, and tectonic) affected by hydrothermal processes. In areas of rapid spreading, like the East Pacific Rise, recent and fossil deposits are spatially separated. By contrast, at the slow spreading Mid-Atlantic Ridge, fossil and present activity are found in the same location. 54 refs., 5 figs., 4 tabs.

  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. PMID:9929173

  12. Radionuclide transport in fractured granite interface zones

    NASA Astrophysics Data System (ADS)

    Hu, Q. H.; Möri, A.

    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 migration paths of radionuclides in fractured granite. In this work, a micro-scale mapping technique was applied by interfacing laser ablation sampling with inductively coupled plasma-mass spectrometry (LA-ICP-MS) to detect the small scale (micron-range) distribution of actinides in the interface zones between fractures and the granitic rock matrix. Long-lived 234U, 235U, and 237Np were detected in flow channels, as well as in the diffusion accessible rock matrix, using the sensitive, feature-based mapping of the LA-ICP-MS technique. The retarded actinides are mainly located at the fracture walls and in the fine grained fracture filling material as well as within the immediately adjacent wallrock. The water-conducting fracture studied in this work is bounded on one side by mylonite and the other by granitic matrix regions. Actinides studied in this work did not penetrate into the mylonite side as much as into the granite matrix, most likely due to the lower porosity, the enhanced sorption capacity and the disturbed diffusion paths of the mylonite region itself. Overall, the maximum penetration depth detected with this technique for 237Np and uranium isotopes 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 modelling of radionuclide diffusion into granitic matrix was conducted to complement and help interpret the field results.

  13. 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. PMID:16049580

  14. Inhalation and intravenous studies of UF6/UO2F2 in dogs.

    PubMed

    Morrow, P; Gelein, R; Beiter, H; Scott, J; Picano, J; Yuile, C

    1982-12-01

    Nineteen UF6/UO2F2 inhalation studies were undertaken in purebred, female beagle dogs (N = 16) to examine inter alia, (a) the possible relations of exposure, whole body, lung and renal uranium levels to excretion rates; (b) the threshold U6+ dose and renal concentration for renal injury; (c) the distribution and retention functions for U6+ in major tissues; (d) biochemical indicators of renal injury; and (e) aspects of U-induced tolerance. Each of these issues was investigated in the context of the chemical toxicity of U6+ following brief exposures to 235UO2F2 in the presence or absence of HF (the decomposition products of 235UF6). Both gamma-(235U) and alpha-(234U) counting methods were applied. In nine studies on 5 dogs, UO2F2 was administered intravenously. The major findings from both types of studies include: (1) UO2F2 retention time in the lungs is shorter than for UO3 or uranyl nitrate, viz. greater than 80% translocated with T 1/2 of less than 20 min; (2) the urinary elimination of U6+ follows closely to the ICRP excretion equation; (c) an absorbed dose of approximately 10 micrograms U6+ kg-1 body weight appears to be effective in producing renal injury; (d) a renal concentration of 0.3 micrograms g-1 kidney is close to a threshold concentration for renal injury; and (e) urinary and blood biochemical changes and histopathologic data were acquired and evaluated in both novice and tolerant animals. This report, considers all of these objectives and findings: Those involving biochemical indices and uranium-induced tolerance will be more fully reported elsewhere. In general, the dog studies attest to the usefulness of the intravenous human studies for certain U6+ dose-response data and interface well with new retention data on intravenous uranyl citrate in dogs by Stevens et al. PMID:7152950

  15. 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..

  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. INDEPENDENT VERIFICATION SURVEY REPORT FOR EXPOSURE UNITS Z2-24, Z2-31, Z2-32, AND Z2-36 IN ZONE 2 OF THE EAST TENNESSEE TECHNOLOGY PARK OAK RIDGE, TENNESSEE

    SciTech Connect

    2013-10-10

    The U.S. Department of Energy (DOE) Oak Ridge Office of Environmental Management selected Oak Ridge Associated Universities (ORAU), through the Oak Ridge Institute for Science and Education (ORISE) contract, to perform independent verification (IV) at Zone 2 of the East Tennessee Technology Park (ETTP) in Oak Ridge, Tennessee. ORAU has concluded IV surveys, per the project-specific plan (PSP) (ORAU 2013a) covering exposure units (EUs) Z2-24, -31, -32, and -36. The objective of this effort was to verify the following. • Target EUs comply with requirements in the Zone 2 Record of Decision (ROD) (DOE 2005), as implemented by using the dynamic verification strategy presented in the dynamic work plan (DWP) (BJC 2007) • Commitments in the DWP were adequately implemented, as verified via IV surveys and soil sampling The Zone 2 ROD establishes maximum remediation level (RLmax) values and average RL (RLavg) values for the primary contaminants of concern (COCs) U-234, U-235, U-238, Cs-137, Np-237, Ra-226, Th-232, arsenic, mercury, and polychlorinated biphenyls (PCBs). Table 1.1 lists Zone 2 COCs with associated RLs. Additional radiological and chemical contaminants were also identified during past characterization and monitoring actions, though the ROD does not present RLs for these potential contaminants. IV activities focused on the identification and quantification of ROD-specific COCs in surface soils, but also generated data for other analytes to support future decisions. ORAU personnel also reviewed EU-specific phased construction completion reports (PCCRs) to focus IV activities and identify potential judgmental sample locations, if any.

  18. 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.

  19. 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.

  20. 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.

  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 natural uranium in small, 1 g samples is usually accomplished by radiochemical analysis in order to measure alpha particles emitted by 238U, 235U, and 234U. However, uranium in larger bulk samples can also be measured non-destructively using gamma spectrometry to detect the low

  2. Uranium series disequilibria in ground waters from a fractured bedrock aquifer (Morungaba Granitoids--Southern Brazil): implications to the hydrochemical behavior of dissolved U and Ra.

    PubMed

    Reyes, Erika; Marques, Leila S

    2008-10-01

    Activity concentrations of dissolved (234)U, (238)U, (226)Ra and (228)Ra were determined in ground waters from two deep wells drilled in Morungaba Granitoids (Southern Brazil). Sampling was done monthly for little longer than 1 year. Significant disequilibrium between (238)U, (234)U and (226)Ra were observed in all samples. The variation of (238)U and (234)U activity concentrations and (234)U/(238)U activity ratios is related to seasonal changes. Although the distance between the two wells is short (about 900 m), systematic differences of activity concentrations of U isotopes, as well as of (234)U/(238)U, (226)Ra/(234)U and (228)Ra/(226)Ra activity ratios were noticed, indicating distinct host rock-water interactions. Slightly acidic ground water percolation through heterogeneous host rock, associated with different recharge processes, may explain uranium and radium isotope behavior. PMID:18514535

  3. Determination the total neutron yields of several semiconductor compounds using various alpha emitters

    NASA Astrophysics Data System (ADS)

    Abdullah, Ramadhan Hayder; Sabr, Barzan Nehmat

    2016-03-01

    In the present work, the cross-sections of (α,n) reactions available in the literature as a function of α-particle energies for light and medium elements have been rearranged for α-particle energies from near threshold up to 10 MeV in steps of (0.050MeV) using the (Excel and Matlab) computer programs. The obtained data were used to calculate the neutron yields (n/106α) using the quick basic-computer program (Simpson Rules). The stopping powers of alpha particle energies from near threshold to 10 MeV for light and medium elements such as (nat.Be,10B,11B,13C,14N,nat.O,nat.F,nat.Mg,nat.Al,29Si,30Si, nat.P and 46.48Ti) have been calculated using the Zeigler formula. The kinetic energies (Tα) and the branching ratios of each α-emitters such as (211Bi, 210Po, 211Po, 215Po, 217At, 218Rn, 219Rn, 222Rn, 224Ra, 226Ra, 215Th, 228Th, 232U, 234U, 236U, 238U, 238Pu, 239Pu, 241Am, 245Es, 252Fm, 254Fm, 256Fm, 257Fm and 257Md) are taken into consideration to calculate the mean kinetic energy . The polynomial expressions were used to fitting the calculated weighted average of neutron yields (n/106α) for natural light and medium elements such as (Be, B, C, N, O, F, Mg, Al, Si, P and Ti) to determine the adopted neutron yields from the best fitting equation with minimum (CHISQ) at mean kinetic energies of various α-emitters. The total neutron yields (n/s/gx/ppmi) of the mentioned natural light and medium elements have been calculated using the adopted neutron yields (n/106α) from the fitting equations at mean kinetic energies of various α-emitters. The total neutron yields (n/s/gα-emitters/gcompounds) of semiconductor compounds such as (AlN, AlP, BN, BP, SiC, TiO2, BeSiN2, MgCN2, MgSiN2 and MgSiP2) have been calculated by mixing (1gram) of compounds with (1gram) of pure α-emitters using the quick basic computer program. The aim of the present work is to constructed and fabricate the neutron sources theoretically

  4. Procedures for accurate U and Th isotope measurements by high precision MC-ICPMS

    NASA Astrophysics Data System (ADS)

    Hoffmann, Dirk L.; Prytulak, Julie; Richards, David A.; Elliott, Tim; Coath, Christopher D.; Smart, Peter L.; Scholz, Denis

    2007-07-01

    We present multi-collector (MC) inductively coupled plasma mass spectrometry (ICPMS) protocols developed to obtain high precision, accurate determinations of U and Th isotope ratios that are applicable to a wide range of geological materials. MC-ICPMS provides a means to make high precision measurements but a recent laboratory inter-comparison, Regular European Inter-laboratory Measurement Evaluation Programme (REIMEP)-18, indicates that accurate results for U isotope ratios are not currently achieved by all facilities using MC-ICPMS. We detail a suite of protocols that can be used for a wide variety of U and Th isotope ratios and total loads. Particular attention is devoted to instrument optimisation, instrumental backgrounds, stability and memory effects, multiplier nonlinearity and yield determinations. Our results indicate that the extent of mass fractionation of U and Th analyses run under similar instrumental conditions is 0.48% per amu and 0.45% per amu, respectively, but cannot be distinguished at per mil precision levels. However, we note that multiplier-Faraday cup gain can be significantly different for U and Th by 1% and thus a U standard should not be used to correct Th measurements. For this reason, a combination of thermal ionisation mass spectrometry (TIMS) and MC-ICPMS methods have been used to determine the isotopic ratio of an in-house Th standard (TEDDi). As part of our methods, TEDDi and the U standard NBL-112a are used as bracketing standards for Th and U samples, respectively. While the in-house Th standard has 229Th-230Th-232Th composition specific for bracketing low 232Th analyses, the methods have been also successful for silicates with 230Th/232Th <10-5. Using NBL-112a, TEDDi and a gravimetrically calibrated mixed 229Th-236U spike, we demonstrate secular equilibrium in natural materials such as Table Mountain Latite and a Long Valley Glass Mountain sample with a reproducibility of ±3.8 per mil for 230Th/238U and ±2.8 per mil for 234U

  5. Advances in ID-TIMS and LA-MC-ICP-MS U-Pb mass spectrometry with applications to geochronology and environmental U analysis

    NASA Astrophysics Data System (ADS)

    Parrish, R. R.; Noble, S. R.; Condon, D. J.; Horstwood, M. S.; Bowring, S.; Schoene, B.; Crowley, Q.

    2006-12-01

    Recent advances highlighted are the analysis of tiny quantities of U and Pb isotopes, ID-TIMS U-Pb dating using EARTHTIME double spike tracers and improved detectors, and the performance of integrated LA-MC- ICP-MS systems for U-Pb dating. Detector improvements: The use of 1012 ohm resistors with faraday detectors has shown that their noise levels conform closely to prediction and overlap ion intensities previously in the realm of ion counting detectors, enabling multiple faraday ion detection for <20 pg of radiogenic Pb. A trade-off in slower response time, however, hinders rapid peak-switching data acquisition and favours use in static multicollection mode. Sub-ng high precision U analysis of complex matrices: The accurate measurement of U isotopes, including ^{236}U at the <1e^{-5} level, in sub-ng quantities of uranium, represents a very significant challenge to the detection of human internal uranium contamination many years after exposure. We have used MC-ICP-MS instruments with mixed SEM-faraday detectors along with improvements in chemical separation and purification to measure uranium isotopes in urine with detection limits of a few fg. In a large study >95% of samples intentionally blind-doped with very small amounts (~3 fg to 40 pg) of either depleted uranium or pure ^{236}U were accurately quantified from a sample cohort of more than 300 urine samples. ID-TIMS: Recent developments spearheaded by the EARTHTIME project (www.earth-time.org) has driven a community effort to improve inter-laboratory U-Pb comparability (and accuracy) via the development of mixed U-Pb tracer solutions for community use. In addition a ^{202}Pb-^{205}Pb-^{233}U-^{235}U double spike has been mixed as part of this project aimed at achieving increased precision via real time Pb mass bias determination. LA-MC-ICP-MS: The Pb/U and 207Pb/206Pb precision by LA-(MC)-ICP-MS can be comparable to SIMS U-Pb dating of zircon. A weakness of LA-ICP-MS U-Pb analysis has been the large

  6. URANIUM-SERIES DISEQUILIBRIUM IN TUFF AND GRANITE:HYDROGEOLOGICAL IMPLICATIONS

    SciTech Connect

    M. Gasscoyne; N.H. Miller

    2000-10-27

    Uranium occurs naturally at trace levels in the major rock-forming minerals (quartz, feldspars, micas) in volcanic and plutonic rocks and is concentrated in accessory minerals (zircon, sphene, apatite). It may attain concentrations as high as 1000 ppm in the accessory minerals. Radiometric age determinations on zircon and sphene have shown that uranium migration from these minerals is generally negligible over prolonged periods of geologic time. Zircon grains separated from highly weathered igneous rocks have been found to retain most of their uranium. In contrast, the uranium fixed onto mineral grain boundaries or present in less-resistant minerals such as biotite or hornblende can be readily leached by groundwater. The ubiquitous presence of uranium in a rock makes it an ideal ''natural analogue'' for understanding the mobility of uranium at a potential site for nuclear fuel waste disposal and one that is easily overlooked in the search for suitable analogues for a disposal site. Several of the intermediate radionuclides in the decay series of the two long-lived isotopes of uranium ({sup 238}U and {sup 235}U) have half-lives greater than one year and are, therefore, of geological interest. In a sealed rock mass with no water-rock interactions, all intermediate radionuclides attain radioactive equilibrium with one another within a maximum 1-2 million years. Because rocks of the Yucca Mountain area and the Canadian Shield (both potential sites for nuclear waste disposal in the United States and Canadian programs, respectively) are considerably older, this condition (known as secular equilibrium) should exist in these rocks, and all daughter/parent radionuclide activity ratios should equal unity (1.000). If the ratios are found not to equal unity, then the rock has been disturbed, probably by groundwater transport of more soluble radionuclides into or away from the rock. How recently this migration has occurred can be determined from the half-life of the

  7. Predicting 232U Content in Uranium

    SciTech Connect

    AJ Peurrung

    1999-01-07

    The minor isotope 232U may ultimately be used for detection or confirmation of uranium in a variety of applications. The primary advantage of 232 U as an indicator of the presence of enriched uranium is the plentiful and penetrating nature of the radiation emitted by its daughter radionuclide 208Tl. A possible drawback to measuring uranium via 232U is the relatively high uncertainty in 232U abundance both within and between material populations. An important step in assessing this problem is to ascertain what determines the 232U concentration within any particular sample of uranium. To this end, we here analyze the production and eventual enrichment of 232 U during fuel-cycle operations. The goal of this analysis is to allow approximate prediction of 232 U quantities, or at least some interpretation of the results of 232U measurements. We have found that 232U is produced via a number of pathways during reactor irradiation of uranium and is subsequently concentrated during the later enrichment of the uranium' s 235U Content. While exact calculations are nearly impossible for both the reactor-production and cascade-enrichment parts of the prediction problem, estimates and physical bounds can be provided as listed below and detailed within the body of the report. Even if precise calculations for the irradiation and enrichment were possible, the ultimate 212U concentration would still depend upon the detailed fuel-cycle history. Assuming that a thennal-diffusion cascade is used to produce highly enriched uranium (HEU), dilution of reactor-processed fuel at the cascade input and the long-term holdup of 232U within the cascade both affect the 232U concentration in the product. Similar issues could be expected to apply for the other isotope-separation technologies that are used in other countries. Results of this analysis are listed below: 0 The 232U concentration depends strongly on the uranium enrichment, with depleted uranium (DU) containing between 1600 and 8000 times

  8. Measurements with the high flux lead slowing-down spectrometer at LANL

    NASA Astrophysics Data System (ADS)

    Danon, Y.; Romano, C.; Thompson, J.; Watson, T.; Haight, R. C.; Wender, S. A.; Vieira, D. J.; Bond, E.; Wilhelmy, J. B.; O'Donnell, J. M.; Michaudon, A.; Bredeweg, T. A.; Schurman, T.; Rochman, D.; Granier, T.; Ethvignot, T.; Taieb, J.; Becker, J. A.

    2007-08-01

    A Lead Slowing-Down Spectrometer (LSDS) was recently installed at LANL [D. Rochman, R.C. Haight, J.M. O'Donnell, A. Michaudon, S.A. Wender, D.J. Vieira, E.M. Bond, T.A. Bredeweg, A. Kronenberg, J.B. Wilhelmy, T. Ethvignot, T. Granier, M. Petit, Y. Danon, Characteristics of a lead slowing-down spectrometer coupled to the LANSCE accelerator, Nucl. Instr. and Meth. A 550 (2005) 397]. The LSDS is comprised of a cube of pure lead 1.2 m on the side, with a spallation pulsed neutron source in its center. The LSDS is driven by 800 MeV protons with a time-averaged current of up to 1 μA, pulse widths of 0.05-0.25 μs and a repetition rate of 20-40 Hz. Spallation neutrons are created by directing the proton beam into an air-cooled tungsten target in the center of the lead cube. The neutrons slow down by scattering interactions with the lead and thus enable measurements of neutron-induced reaction rates as a function of the slowing-down time, which correlates to neutron energy. The advantage of an LSDS as a neutron spectrometer is that the neutron flux is 3-4 orders of magnitude higher than a standard time-of-flight experiment at the equivalent flight path, 5.6 m. The effective energy range is 0.1 eV to 100 keV with a typical energy resolution of 30% from 1 eV to 10 keV. The average neutron flux between 1 and 10 keV is about 1.7 × 109 n/cm2/s/μA. This high flux makes the LSDS an important tool for neutron-induced cross section measurements of ultra-small samples (nanograms) or of samples with very low cross sections. The LSDS at LANL was initially built in order to measure the fission cross section of the short-lived metastable isotope of U-235, however it can also be used to measure (n, α) and (n, p) reactions. Fission cross section measurements were made with samples of 235U, 236U, 238U and 239Pu. The smallest sample measured was 10 ng of 239Pu. Measurement of (n, α) cross section with 760 ng of Li-6 was also demonstrated. Possible future cross section measurements

  9. Measurements of daily urinary uranium excretion in German peacekeeping personnel and residents of the Kosovo region to assess potential intakes of depleted uranium (DU).

    PubMed

    Oeh, U; Priest, N D; Roth, P; Ragnarsdottir, K V; Li, W B; Höllriegl, V; Thirlwall, M F; Michalke, B; Giussani, A; Schramel, P; Paretzke, H G

    2007-08-01

    Following the end of the Kosovo conflict, in June 1999, a study was instigated to evaluate whether there was a cause for concern of health risk from depleted uranium (DU) to German peacekeeping personnel serving in the Balkans. In addition, the investigations were extended to residents of Kosovo and southern Serbia, who lived in areas where DU ammunitions were deployed. In order to assess a possible DU intake, both the urinary uranium excretion of volunteer residents and water samples were collected and analysed using inductively coupled plasma-mass spectrometry (ICP-MS). More than 1300 urine samples from peacekeeping personnel and unexposed controls of different genders and age were analysed to determine uranium excretion parameters. The urine measurements for 113 unexposed subjects revealed a daily uranium excretion rate with a geometric mean of 13.9 ng/d (geometric standard deviation (GSD)=2.17). The analysis of 1228 urine samples from the peacekeeping personnel resulted in a geometric mean of 12.8 ng/d (GSD=2.60). It follows that both unexposed controls and peacekeeping personnel excreted similar amounts of uranium. Inter-subject variation in uranium excretion was high and no significant age-specific differences were found. The second part of the study monitored 24 h urine samples provided by selected residents of Kosovo and adjacent regions of Serbia compared to controls from Munich, Germany. Total uranium and isotope ratios were measured in order to determine DU content. (235)U/(238)U ratios were within +/-0.3% of the natural value, and (236)U/(238)U was less than 2 x 10(-7), indicating no significant DU in any of the urine samples provided, despite total uranium excretion being relatively high in some cases. Measurements of ground and tap water samples from regions where DU munitions were deployed did not show any contamination with DU, except in one sample. It is concluded that both peacekeeping personnel and residents serving or living in the Balkans

  10. ENDF/B-VII.1 Neutron Cross Section Data Testing with Critical Assembly Benchmarks and Reactor Experiments

    SciTech Connect

    G. Palmiotti

    2011-12-01

    The ENDF/B-VII.1 library is the latest revision to the United States' Evaluated Nuclear Data File (ENDF). The ENDF library is currently in its seventh generation, with ENDF/B-VII.0 being released in 2006. This revision expands upon that library, including the addition of new evaluated files (was 393 neutron files previously, now 418 including replacement of elemental vanadium and zinc evaluations with isotopic evaluations) and extension or updating of many existing neutron data files. Complete details are provided in the companion paper [1]. This paper focuses on how accurately application libraries may be expected to perform in criticality calculations with these data. Continuous energy cross section libraries, suitable for use with the MCNP Monte Carlo transport code, have been generated and applied to a suite of nearly one thousand critical benchmark assemblies defined in the International Criticality Safety Benchmark Evaluation Project's International Handbook of Evaluated Criticality Safety Benchmark Experiments. This suite covers uranium and plutonium fuel systems in a variety of forms such as metallic, oxide or solution, and under a variety of spectral conditions, including unmoderated (i.e., bare), metal reflected and water or other light element reflected. Assembly eigenvalues that were accurately predicted with ENDF/B-VII.0 cross sections such as unmoderated and uranium reflected 235U and 239Pu assemblies, HEU solution systems and LEU oxide lattice systems that mimic commercial PWR configurations continue to be accurately calculated with ENDF/B-VII.1 cross sections, and deficiencies in predicted eigenvalues for assemblies containing selected materials, including titanium, manganese, cadmium and tungsten are greatly reduced. Improvements are also confirmed for selected actinide reaction rates such as 236U capture. Other deficiencies, such as the overprediction of Pu solution system critical eigenvalues and a decreasing trend in calculated eigenvalue for

  11. ENDF/B-VII.1 Neutron Cross Section Data Testing with Critical Assembly Benchmarks and Reactor Experiments

    NASA Astrophysics Data System (ADS)

    Kahler, A. C.; MacFarlane, R. E.; Mosteller, R. D.; Kiedrowski, B. C.; Frankle, S. C.; Chadwick, M. B.; McKnight, R. D.; Lell, R. M.; Palmiotti, G.; Hiruta, H.; Herman, M.; Arcilla, R.; Mughabghab, S. F.; Sublet, J. C.; Trkov, A.; Trumbull, T. H.; Dunn, M.

    2011-12-01

    The ENDF/B-VII.1 library is the latest revision to the United States' Evaluated Nuclear Data File (ENDF). The ENDF library is currently in its seventh generation, with ENDF/B-VII.0 being released in 2006. This revision expands upon that library, including the addition of new evaluated files (was 393 neutron files previously, now 423 including replacement of elemental vanadium and zinc evaluations with isotopic evaluations) and extension or updating of many existing neutron data files. Complete details are provided in the companion paper [M. B. Chadwick et al., "ENDF/B-VII.1 Nuclear Data for Science and Technology: Cross Sections, Covariances, Fission Product Yields and Decay Data," Nuclear Data Sheets, 112, 2887 (2011)]. This paper focuses on how accurately application libraries may be expected to perform in criticality calculations with these data. Continuous energy cross section libraries, suitable for use with the MCNP Monte Carlo transport code, have been generated and applied to a suite of nearly one thousand critical benchmark assemblies defined in the International Criticality Safety Benchmark Evaluation Project's International Handbook of Evaluated Criticality Safety Benchmark Experiments. This suite covers uranium and plutonium fuel systems in a variety of forms such as metallic, oxide or solution, and under a variety of spectral conditions, including unmoderated (i.e., bare), metal reflected and water or other light element reflected. Assembly eigenvalues that were accurately predicted with ENDF/B-VII.0 cross sections such as unmoderated and uranium reflected 235U and 239Pu assemblies, HEU solution systems and LEU oxide lattice systems that mimic commercial PWR configurations continue to be accurately calculated with ENDF/B-VII.1 cross sections, and deficiencies in predicted eigenvalues for assemblies containing selected materials, including titanium, manganese, cadmium and tungsten are greatly reduced. Improvements are also confirmed for selected

  12. ENDF/B-VII.1 Neutron Cross Section Data Testing with Critical Assembly Benchmarks and Reactor Experiments

    SciTech Connect

    Kahler, A.C.; Herman, M.; Kahler,A.C.; MacFarlane,R.E.; Mosteller,R.D.; Kiedrowski,B.C.; Frankle,S.C.; Chadwick,M.B.; McKnight,R.D.; Lell,R.M.; Palmiotti,G.; Hiruta,H.; Herman,M.; Arcilla,R.; Mughabghab,S.F.; Sublet,J.C.; Trkov,A.; Trumbull,T.H.; Dunn,M.

    2011-12-01

    The ENDF/B-VII.1 library is the latest revision to the United States Evaluated Nuclear Data File (ENDF). The ENDF library is currently in its seventh generation, with ENDF/B-VII.0 being released in 2006. This revision expands upon that library, including the addition of new evaluated files (was 393 neutron files previously, now 423 including replacement of elemental vanadium and zinc evaluations with isotopic evaluations) and extension or updating of many existing neutron data files. Complete details are provided in the companion paper [M. B. Chadwick et al., 'ENDF/B-VII.1 Nuclear Data for Science and Technology: Cross Sections, Covariances, Fission Product Yields and Decay Data,' Nuclear Data Sheets, 112, 2887 (2011)]. This paper focuses on how accurately application libraries may be expected to perform in criticality calculations with these data. Continuous energy cross section libraries, suitable for use with the MCNP Monte Carlo transport code, have been generated and applied to a suite of nearly one thousand critical benchmark assemblies defined in the International Criticality Safety Benchmark Evaluation Project's International Handbook of Evaluated Criticality Safety Benchmark Experiments. This suite covers uranium and plutonium fuel systems in a variety of forms such as metallic, oxide or solution, and under a variety of spectral conditions, including unmoderated (i.e., bare), metal reflected and water or other light element reflected. Assembly eigenvalues that were accurately predicted with ENDF/B-VII.0 cross sections such as unmoderated and uranium reflected {sup 235}U and {sup 239}Pu assemblies, HEU solution systems and LEU oxide lattice systems that mimic commercial PWR configurations continue to be accurately calculated with ENDF/B-VII.1 cross sections, and deficiencies in predicted eigenvalues for assemblies containing selected materials, including titanium, manganese, cadmium and tungsten are greatly reduced. Improvements are also confirmed for

  13. Uranium Isotope Systematic in Saanich Inlet

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

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

  14. Precision and accuracy of decay constants and age standards

    NASA Astrophysics Data System (ADS)

    Villa, I. M.

    2011-12-01

    40 years of round-robin experiments with age standards teach us that systematic errors must be present in at least N-1 labs if participants provide N mutually incompatible data. In EarthTime, the U-Pb community has produced and distributed synthetic solutions with full metrological traceability. Collector linearity is routinely calibrated under variable conditions (e.g. [1]). Instrumental mass fractionation is measured in-run with double spikes (e.g. 233U-236U). Parent-daughter ratios are metrologically traceable, so the full uncertainty budget of a U-Pb age should coincide with interlaboratory uncertainty. TIMS round-robin experiments indeed show a decrease of N towards the ideal value of 1. Comparing 235U-207Pb with 238U-206Pb ages (e.g. [2]) has resulted in a credible re-evaluation of the 235U decay constant, with lower uncertainty than gamma counting. U-Pb microbeam techniques reveal the link petrology-microtextures-microchemistry-isotope record but do not achieve the low uncertainty of TIMS. In the K-Ar community, N is large; interlaboratory bias is > 10 times self-assessed uncertainty. Systematic errors may have analytical and petrological reasons. Metrological traceability is not yet implemented (substantial advance may come from work in progress, e.g. [7]). One of the worst problems is collector stability and linearity. Using electron multipliers (EM) instead of Faraday buckets (FB) reduces both dynamic range and collector linearity. Mass spectrometer backgrounds are never zero; the extent as well as the predictability of their variability must be propagated into the uncertainty evaluation. The high isotope ratio of the atmospheric Ar requires a large dynamic range over which linearity must be demonstrated under all analytical conditions to correctly estimate mass fractionation. The only assessment of EM linearity in Ar analyses [3] points out many fundamental problems; the onus of proof is on every laboratory claiming low uncertainties. Finally, sample

  15. Uranium-series age determination of calcite veins, VC-1 drill core, Valles Caldera, New Mexico

    NASA Astrophysics Data System (ADS)

    Sturchio, Neil C.; Binz, Carl M.

    1988-06-01

    Uranium-series analysis (238U-234U-230Th) of 13 calcite veins from the hydrothermally altered Madera Limestone in the VC-1 drill core was performed to determine the ages of the veins and their relation to the Valles hydrothermal system. Thermal water from VC-1 and two hot springs in San Diego Canyon was analyzed for U and (234U/238U) to help evaluate the constancy of initial (234U/238U). The (230Th/234U) age of one of the veins is ˜95 kyr, and those of two other veins are ˜230 and ˜250 kyr. Five of the veins have near equilibrium (230Th/234U) and are probably older than ˜0.3 m.y. Uranium concentrations in the remaining veins are too low for analysis by the α-spectrometry techniques employed in this study. Of the five veins near (230Th/234U) equilibrium, four are also near (234U/238U) equilibrium, suggesting ages greater than ˜1.0 m.y., but one has (234U/238U) = 1.15, suggesting an age between ˜0.3 and ˜1.0 m.y. Calculated initial (234U/238U) of the veins yielding relatively young ages are neither equal to each other nor to (234U/238U) in thermal water from VC-1, indicating inconstancy of initial (234U/238U) that may be related to variations in groundwater mixing proportions. Three of the four veins that yield relatively young ages consist of coarse, sparry, vuggy calcite, suggesting that this may be the type of calcite vein which forms under conditions resembling those encountered presently in VC-1. The analytical data are consistent with closed-system behavior of U and Th in the VC-1 calcite veins.

  16. Impact of prompt-neutron corrections on final fission-fragment distributions

    NASA Astrophysics Data System (ADS)

    Al-Adili, A.; Hambsch, F.-J.; Pomp, S.; Oberstedt, S.

    2012-11-01

    Background: One important quantity in nuclear fission is the average number of prompt neutrons emitted from the fission fragments, the prompt neutron multiplicity, ν¯. The total number of prompt fission neutrons, ν¯tot, increases with increasing incident neutron energy. The prompt-neutron multiplicity is also a function of the fragment mass and the total kinetic energy of the fragmentation. Those data are only known in sufficient detail for a few thermal-neutron-induced fission reactions on, for example, 233,235U and 239Pu. The enthralling question has always been asked how the additional excitation energy is shared between the fission fragments. The answer to this question is important in the analysis of fission-fragment data taken with the double-energy technique. Although in the traditional approach the excess neutrons are distributed equally across the mass distribution, a few experiments showed that those neutrons are predominantly emitted by the heavy fragments.Purpose: We investigated the consequences of the ν(A,TKE,En) distribution on the fission fragment observables.Methods: Experimental data obtained for the 234U(n,f) reaction with a Twin Frisch Grid Ionization Chamber, were analyzed assuming two different methods for the neutron evaporation correction. The effect of the two different methods on the resulting fragment mass and energy distributions is studied.Results: We found that the preneutron mass distributions obtained via the double-energy technique become slightly more symmetric, and that the impact is larger for postneutron fission-fragment distributions. In the most severe cases, a relative yield change up to 20-30% was observed.Conclusions: We conclude that the choice of the prompt-neutron correction method has strong implications on the understanding and modeling of the fission process and encourages new experiments to measure fission fragments in coincidence with prompt fission neutrons. Even more, the correct determination of postneutron

  17. Concentrations of Radionuclides and Trace Elements in Environmantal Media arond te Dual-Axis Radiographic Hydrodynamic Test Facilit at Los Alamos National Laboratory during 2005

    SciTech Connect

    G.J.Gonzales; P.R. Fresquez; C.D.Hathcock; D.C. Keller

    2006-05-15

    The Mitigation Action Plan (MAP) for the Dual-Axis Radiographic Hydrodynamic Test (DARHT) facility at Los Alamos National Laboratory requires that samples of biotic and abiotic media be collected after operations began to determine if there are any human health or environmental impacts. The DARHT facility is the Laboratory's principal explosive test facility. To this end, samples of soil and sediment, vegetation, bees, and birds were collected around the facility in 2005 and 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. Bird populations have also been monitored. Contaminant results, which represent up to six sample years since the start of operations, were compared with (1) baseline statistical reference levels (BSRLs) established over a four-year preoperational period before DARHT facility operations, (2) screening levels (SLs), and (3) regulatory standards. Most radionuclides and trace elements were below BSRLs and those few samples that contained radionuclides and trace elements above BSRLs were below SLs. Concentrations of radionuclides and nonradionuclides in biotic and abiotic media around the DARHT facility do not pose a significant human health hazard. The total number of birds captured and number of species represented were similar in 2003 and 2004, but both of these parameters increased substantially in 2005. Periodic interruption of the scope and schedule identified in the MAP generally should have no impact on meeting the intent of the MAP. The risk of not sampling one of the five media in any given year is that if a significant impact to contaminant levels were to occur there would exist a less complete understanding of the extent of the change to the baseline for these media and to the ecosystem as a whole. Since the MAP is a requirement that was established under the regulatory framework of the

  18. Variations in Cenozoic seawater uranium reconstructed from well preserved aragonitic fossil corals

    NASA Astrophysics Data System (ADS)

    Gothmann, A. O.; Higgins, J. A.; Bender, M. L.; Stolarski, J.; Adkins, J. F.; McKeon, R. E.; Farley, K. A.; Wang, X.; Planavsky, N.

    2015-12-01

    U/Ca ratios were measured in a subset (n ≈ 30) of well preserved scleractinian fossil corals previously described by Gothmann et al. (2015) in order to investigate Cenozoic changes in seawater [U]. He/U dating studies and measurements of 234U/238U and δ238/235U provide constraints on fossil coral U preservation. He/U ages also demonstrate the ability of well preserved coral aragonite to retain most of its radiogenic He over million year timescales. We find that fossil coral U/Ca has increased by a factor of ~4 between the Early Cenozoic and today. This number is calculated from the change in seawater [Ca2+] implied by brine inclusions and other proxies, and the assumption that the U/Ca in shallow water corals equals the seawater ratio. The change cannot be attributed to a dependence of coral U uptake on seawater pH or [CO32-] (e.g., Inoue et al., 2011), which would lead to a decrease in U/Ca going forward in time. Instead, we suggest that seawater [U] has increased since the Early Cenozoic. Possible explanations for the inferred change include: (1) a small decrease in uranium uptake in suboxic and anoxic sediments over the Cenozoic, (2) a decrease in the rate of low-temperature hydrothermal alteration, and associated U uptake, over the Cenozoic, and (3) a decrease in U removal from seawater resulting from an increase in UO2-CO3 complexation, as originally suggested by Broecker (1971). References: Broecker, W. S. (1971) A Kinetic Model for the Chemical Composition of Sea Water. Quaternary Research, 1, 188-207. Gothmann, A.M., Stolarski, J., Adkins, J.F., Dennis, K.J., Schrag, D.P., Schoene, B., Bender, M.L. (2015) Fossil corals as an archive of secular variations in seawater chemistry. Geochimica et Cosmochimica Acta, 160, 188-208. Inoue, M., Suwa, R., Suzuki, A., Sakai, K., and Kawahata, H., (2011) Effects of seawater pH on growth and skeletal U/Ca ratios of Acropora digitifera coral polyps. Geophysical Research Letters 38, 12801-12804.

  19. Analysis of the Younger Dryas Impact Layer

    SciTech Connect

    Firestone, Richard B.; West, Allen; Revay, Zsolt; Hagstrum, Jonathon T,; Belgya, Thomas; Hee, Shane S. Que; Smith, Alan R.

    2010-02-27

    We have uncovered a thin layer of magnetic grains and microspherules, carbon spherules, and glass-like carbon at nine sites across North America, a site in Belgium, and throughout the rims of 16 Carolina Bays. It is consistent with the ejecta layer from an impact event and has been dated to 12.9 ka BP coinciding with the onset of Younger Dryas (YD) cooling and widespread megafaunal extinctions in North America. At many locations the impact layer is directly below a black mat marking the sudden disappearance of the megafauna and Clovis people. The distribution pattern of the Younger Dryas boundary (YDB) ejecta layer is consistent with an impact near the Great Lakes that deposited terrestrial-like ejecta near the impact site and unusual, titanium-rich projectile-like ejecta further away. High water content associated with the ejecta, up to 28 at. percent hydrogen (H), suggests the impact occurred over the Laurentide Ice Sheet. YDB microspherules and magnetic grains are highly enriched in TiO{sub 2}. Magnetic grains from several sites are enriched in iridium (Ir), up to 117 ppb. The TiO{sub 2}/FeO, K/Th, TiO{sub 2}/Zr, Al{sub 2}O{sub 3}/FeO+MgO, CaO/Al{sub 2}O{sub 3}, REE/ chondrite, FeO/MnO ratios and SiO{sub 2}, Na{sub 2}O, K{sub 2}O, Cr{sub 2}O{sub 3}, Ni, Co, U, Th and other trace element abundances are inconsistent with all terrestrial and extraterrestrial (ET) sources except for KREEP, a lunar igneous rock rich in potassium (K), rare-earth elements (REE), phosphorus (P), and other incompatible elements including U and Th. Normal Fe, Ti, and {sup 238}U/{sup 235}U isotopic abundances were found in the magnetic grains, but {sup 234}U was enriched over equilibrium values by 50 percent in Murray Springs and by 130 percent in Belgium. 40K abundance is enriched by up to 100 percent in YDB sediments and Clovis chert artifacts. Highly vesicular carbon spherules containing nanodiamonds, glass-like carbon, charcoal and soot found in large quantities in the YDB layer are

  20. Comparative analysis of isotopic composition of spent fuel from Takahama-3 PWR PIE database using TRIPOLI-PEPIN code

    SciTech Connect

    Lee, Y. K.

    2006-07-01

    Evaluation of isotopic composition of spent nuclear fuel is essential for reactor physics and fuel cycle back-end applications. A TRIPOLI-PEPIN coupled depletion code, TR4PEP, has been developed to meet these requirements. It combines the continuous-energy Monte Carlo transport code, TRIPOLI4.3 [1] and the point depletion code, PEPIN-2 [2], to perform the burnup dependent material data calculation. The depletion calculation flow of TR4PEP code has been presented on a previous study. Its application on PWR UO{sub 2} and MOX spent fuel has been validated against several international numerical benchmarks. Compared to industry standard deterministic cell codes and other Monte Carlo based depletion codes, TR4PEP deep-burn depletion calculations have shown satisfactory results. [3] In addition to the numerical benchmarks, the analysis of available post irradiation examination (PIE) results by TR4PEP is also important The PIE results at fuel assembly level are accessible only from spent fuel reprocessing plant and these data are not easy to use for code validation due to the dissolution of several assemblies in the same time. The PIE results at fuel pellet level depend not only on the method for the isotopic measurements but also on the irradiation environment and history. A free access PIE database on isotopic composition of spent nuclear fuel is obtainable from OECD/NEA. [4] Both PWR and BWR PIE data at fuel pellet level are taken into account in this database but the only 17 x 17 type PWR fuel available in this database is from Takahama-3 PIE results. To validate TR4PEP with Takahama-3 PIE results, two irradiated UO{sub 2} samples, SF95-4 from fuel assembly NT3G23 and SF97-5 from NT3G24, are considered in this study. Both samples have an initial {sup 235}U enrichment of 4.11 wt% and their burnup are respectively 36.69 and 47.03 GWd/t. Comparative analysis of isotopic composition from SF95-4 and SF97-5 including 19 actinides from {sup 234}U to {sup 247}Cm and 18

  1. RAPID DETERMINATION OF ACTINIDES IN URINE BY INDUCTIVELY-COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY: A HYBRID APPROACH

    SciTech Connect

    Maxwell, S.; Jones, V.

    2009-05-27

    A new rapid separation method that allows separation and preconcentration of actinides in urine samples was developed for the measurement of longer lived actinides by inductively coupled plasma mass spectrometry (ICP-MS) and short-lived actinides by alpha spectrometry; a hybrid approach. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration, if required, is performed using a streamlined calcium phosphate precipitation. Similar technology has been applied to separate actinides prior to measurement by alpha spectrometry, but this new method has been developed with elution reagents now compatible with ICP-MS as well. Purified solutions are split between ICP-MS and alpha spectrometry so that long- and short-lived actinide isotopes can be measured successfully. The method allows for simultaneous extraction of 24 samples (including QC samples) in less than 3 h. Simultaneous sample preparation can offer significant time savings over sequential sample preparation. For example, sequential sample preparation of 24 samples taking just 15 min each requires 6 h to complete. The simplicity and speed of this new method makes it attractive for radiological emergency response. If preconcentration is applied, the method is applicable to larger sample aliquots for occupational exposures as well. The chemical recoveries are typically greater than 90%, in contrast to other reported methods using flow injection separation techniques for urine samples where plutonium yields were 70-80%. This method allows measurement of both long-lived and short-lived actinide isotopes. 239Pu, 242Pu, 237Np, 243Am, 234U, 235U and 238U were measured by ICP-MS, while 236Pu, 238Pu, 239Pu, 241Am, 243Am and 244Cm were measured by alpha spectrometry. The method can also be adapted so that the separation of uranium isotopes for assay is not required, if uranium assay by direct dilution of the urine sample is preferred instead

  2. Recent fission cross section standards measurements

    SciTech Connect

    Wasson, O.A.

    1985-01-01

    The /sup 235/U(n,f) reaction is the standard by which most neutron induced fission cross sections are determined. Most of these cross sections are derived from relatively easy ratio measurements to /sup 235/U. However, the more difficult /sup 235/U(n,f) cross section measurements require the use of advanced neutron detectors for the determination of the incident neutron fluence. Examples of recent standard cross section measurements are discussed, various neutron detectors are described, and the status of the /sup 235/U(n,f) cross section standard is assessed. 23 refs., 8 figs., 4 tabs.

  3. Uranium-236 as a new oceanic tracer: A first depth profile in the Japan Sea and comparison with caesium-137

    PubMed Central

    Sakaguchi, Aya; Kadokura, Akinobu; Steier, Peter; Takahashi, Yoshio; Shizuma, Kiyoshi; Hoshi, Masaharu; Nakakuki, Tomoeki; Yamamoto, Masayoshi

    2012-01-01

    We present a feasibility study for using 236U as an oceanic circulation tracer based on depth profiles of 236U and 137Cs in the Japan/East Sea. The concentration of the predominantly anthropogenic 236U, measured with Accelerator Mass Spectrometry (AMS), decreased from (13±3)×106 atom/kg in surface water to (1.6±0.3)×106 atom/kg close to the sea floor (2800 m). The profile has a smooth trend with depth and concentration values are generally proportional to that of 137Cs for the same water samples, but with a slightly lower ratio of 137Cs/236U below 2000 m. The cumulative inventory of dissolved 236U in the water column was estimated to be (13.7±0.9)×1012 atom/m2, which is similar to the global-fallout level (17.8×1012 atom/m2) in Japan. Additional analyses of suspended solids (SS) and bottom sediments yielded negligible amounts of 236U. Our results suggest that 236U behaves as a conservative nuclide in seawater, with potential advantages over other tracers of oceanic circulation. PMID:23564965

  4. Constrains on the Uranium Isotopic Composition of Seawater and Implications for Coral U/Th Geochronology

    NASA Astrophysics Data System (ADS)

    Chutcharavan, P. M.; Dutton, A.; Ellwood, M. J.

    2015-12-01

    Coral U-series geochronology is an important tool for calibrating records of sea level change during the late Quaternary and coral 14C dates for the radiocarbon timescale. However, coralline aragonite is highly susceptible to diagenesis, and samples must be carefully screened to ensure a specimen is unaltered. One method used to accept or reject U-series ages is the initial coral 234U/238U activity ratio, which reflects the 234U/238U activity of seawater at the time of coral skeleton formation. Due to the long residence time of uranium in the ocean (~400,000 years), researchers often assume that seawater 234U/238U has remained constant throughout the late Pleistocene. Coral specimens whose U-series ages yield an initial 234U/238U value that is significantly different than modern seawater are considered altered. Several studies have demonstrated that coral initial 234U/238U and, hence, seawater 234U/238U may have varied significantly on glacial-interglacial timescales, but the cause of this variability is subject to debate. To evaluate the pattern and mechanisms of 234U/238U variability in seawater over the last glacial cycle, we draw upon a compilation of U-series measurements of shallow and deep water corals to better define the observed variability. Observed trends from the coral record will be assessed using a simple two-box model of the ocean to determine how changes to the ocean's uranium isotope budget during glacial cycles can explain shifts in seawater 234U/238U. An improved understanding the evolution of seawater 234U/238U composition will enable more robust interpretations of both closed-system and open-system ages for corals. Such interpretations of U-series ages are essential to the development of robust chronologies for climate and sea level change and for improving the calibration of the radiocarbon timescale.

  5. U-series constraints on the Holocene human presence in the Cuatro Cienegas basin, Mexico

    NASA Astrophysics Data System (ADS)

    Noble, S. R.; Felstead, N.; Gonzalez, S.; Leng, M. J.; Metcalfe, S. E.; Patchett, P. J.

    2010-12-01

    U-series tufa ages dating a human trackway have been obtained, part of a larger Late Pleistocene - Recent palaeoclimate and human occupation study of the Cuatro Cienegas basin, NE Mexico. Our analytical approach, including tracer calibration, couples aspects of what we consider best practice in the U-series community with our U-Pb experiences which includes the EarthTime U-Pb tracer calibration exercise. The recently discovered trackway is near a small hydrothermal pool within the basin [1], an ecologically highly significant oasis in the Chihuahuan desert. The oasis comprises >200 freshwater hydrothermal pools and a river system, and the related ecosystem hosts >70 endemic species[2]. Pools are fed by waters that circulate a deep karstic system and that originate in the surrounding upper Jurassic-lower Cretaceous Sierra Madre Oriental mountains (>3000m) [3]. The area hosted nomadic hunter-gatherers during the Holocene, and possibly as early as Late Pleistocene (~12 ka BP). Despite the basin's ecological significance, only three palaeoenvironmental studies have been published to date, and limited geochronological constraints are available. A pollen study of drill core through peats and tufas proximal to the pools suggested a long period of climatic stability and biogeographic isolation[4], a notion supported by the large number of endemic species, but other palynological and plant macrofossil data suggest that large climatic changes occurred post Late Pleistocene [5]. The 10 m long in situ trackway is preserved in tufa and five samples from the uppermost surfaces were analysed to date the footprints. The tufas comprise clean carbonate with no petrographic evidence of replacement and little contaminant detrital material (on some exposed upper surfaces). Powdered tufa was processed following [6-8], and analysed by TIMS (Triton, U) and MC-ICP-MS (Th, Nu HR), although our future analyses will primarily be obtained on a Neptune. Samples were spiked with a 229Th/236U

  6. Disequilibrium of uranium isotopes in some Syrian groundwater.

    PubMed

    Abdul-Hadi, A; Alhassanieh, O; Ghafar, M

    2001-07-01

    Uranium concentration in groundwater samples from three areas of Syria was determined using alpha-spectrometry and INAA. It was in the range of 0-6.13 microg/l in the phosphate areas, and lower than 1 ppb in the volcanic areas. The activity ratio of 234U/238U was investigated, and disequilibrium of uranium isotopes was found to occur (234U/238U = 0.52-2.02). The excess of 234U was calculated. This excess can be interpreted by higher mobility of 234U, which more readily forms the soluble (UO2)2+ ion in comparison with 238U, most of which remains in the insoluble 4+ state. This excess increases with increase in uranium concentration. Thorium concentration was measured using INAA, it was found to be in the rang 0-1.15 microg/l. PMID:11339524

  7. Uranium and thorium isotopes and their state of equilibria in lungs from uranium miners.

    PubMed

    Wrenn, M E; Singh, N P; Saccomanno, G

    1983-01-01

    Radiochemical analysis of seven lungs obtained at autopsy show that concentrations ranged between 6 and 63 pCi/kg for 238U and 6-66 pCi/kg, for 234U. Similarly, 230Th ranged from 17 to 54 pCi/kg, two orders of magnitude higher than 230Th observed in the lungs of the general population from the Western mining region. For individual lungs, 238U and 234U were close to equilibrium with an average ratio of 238U/234U of 0.94 and a range of 0.80-1.02. Surprisingly, 230Th was close to equilibrium with 234U with a 230Th/234U ratio of 1.1 and a range from 0.54 to 2.6. Equilibrium between U and Th isotopes is in contrast to the disequilibrium reported in beagles which chronically inhaled carnotite, where the 230Th/234U ratio was observed to range from 5.4 to 7.4 with an average of 6.3. The average radiation dose rate to lung from each of the three radionuclides was calculated as follows: D = 18.7 CE where D = dose rate in mrad/year, C = activity concentration in tissue in pCi/g and E = energy absorbed per disintegration in MeV. The combined radiation dose rate (at death) due to three long-lived radionuclides 238U, 234U and 230Th varied from 2.5 to 14.2 mrad/yr with a mean of 9.6 mrad/yr. The concentration of 226Ra and daughters in the lung was not determined. An upper limit to the dose rate from the whole chain, calculated assuming 226Ra through 210Po are in equilibrium with 238U, 234U and 230Th, would be 30 mrad/yr. PMID:6862915

  8. Coupled uranium isotope and sea-level variations in the oceans

    NASA Astrophysics Data System (ADS)

    Esat, Tezer M.; Yokoyama, Yusuke

    2010-12-01

    Globally, rivers supply uranium to the oceans with excess 234U relative to secular equilibrium and 234U taken-up by corals can be used for dating. In addition, the 234U abundance in sea water, at the time the coral was growing, can be measured independently. The veracity of U-series ages used in determining past sea-level variations is depe