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Sample records for 239pu 241am 243am

  1. (239)Pu, (240)Pu, and (241)Am determination in hot particles by low level gamma-spectrometry.

    PubMed

    Jiménez-Ramos, M C; Hurtado, S; Chamizo, E; García-Tenorio, R; León-Vintró, L; Mitchell, P I

    2010-06-01

    A nondestructive method based on low-energy, high-resolution photon spectrometry is presented which allows accurate determination of (239)Pu, (240)Pu, and (241)Am (as a daughter of (241)Pu) activities in radioactive particles containing relatively high levels of plutonium isotopes. The proposed method requires only one measurement for the establishment of an absolute efficiency curve. Since the density and composition of the radioactive particles of interest may vary, a self-absorption correction is required for the accurate determination of isotopic activities and ratios. This correction is carried out for each individual particle using the convenient gamma-ray emissions of (241)Am.

  2. Alpha and conversion electron spectroscopy of 238,239Pu and 241Am and alpha-conversion electron coincidence measurements

    SciTech Connect

    Dion, Michael P.; Miller, Brian W.; Warren, Glen A.

    2016-09-01

    A technique to determine the isotopics of a mixed actinide sample has been proposed by measuring the coincidence of the alpha particle during radioactive decay with the conversion electron (or Auger) emitted during the relaxation of the daughter isotope. This presents a unique signature to allow the deconvolution of isotopes that possess overlapping alpha particle energy. The work presented here are results of conversion electron spectroscopy of 241Am, 238Pu and 239Pu using a dual-stage peltier-cooled 25 mm2 silicon drift detector. A passivated ion implanted planar silicon detector provided measurements of alpha spectroscopy. The conversion electron spectra were evaluated from 20–55 keV based on fits to the dominant conversion electron emissions, which allowed the relative conversion electron emission intensities to be determined. These measurements provide crucial singles spectral information to aid in the coincident measurement approach.

  3. Radiological implications of inhaled 239Pu and 241Am in dusts at the former nuclear test site in Maralinga.

    PubMed

    Stradling, G N; Stather, J W; Gray, S A; Moody, J C; Ellender, M; Pearce, M J; Collier, C G

    1992-12-01

    The biokinetics of 239Pu and 241Am present in three dust samples obtained from Maralinga were investigated after their deposition in the rat lung. Results were used as an experimental basis for assessing the radiological implications for human exposure. The transfer rates of these actinides to blood in the various dusts differed by 50-fold. The most transportable forms were compatible with a material that had 25% class W and 75% class Y characteristics. The doses per unit intake for adults, children, and infants exposed to an aerosol of 5 microns AMAD were calculated to be, respectively, 0.059, 0.076, and 0.140 mSv Bq-1. The corresponding doses for the least transportable forms were the same as those calculated for a class Y compound, namely 0.036, 0.049, and 0.096 mSv Bq-1. The behavior of the actinides in humans was predicted by combining the transfer rates to blood with mechanical clearance data obtained after volunteers had inhaled 85Sr or 88Y labeled fused aluminosilicate particles. The results suggested that monitoring of 241Am in the chest could be used to advantage for assessing intakes incurred by workers involved with any further decontamination procedures but would be of little practical value for assessing inadvertent public exposure. The paper includes comments on the relevance of the 1990 ICRP recommendations and the proposed new dosimetric model for the respiratory tract.

  4. Alpha and conversion electron spectroscopy of 238,239Pu and 241Am and alpha-conversion electron coincidence measurements

    NASA Astrophysics Data System (ADS)

    Dion, Michael P.; Miller, Brian W.; Warren, Glen A.

    2016-09-01

    A technique to determine the isotopic constituents of a mixed actinide sample has been proposed by a coincident alpha-conversion electron measurement. This presents a unique signature to allow the unfolding of isotopes that possess overlapping alpha particle energy and reduce backgrounds of an unseparated sample. The work presented here are results of conversion electron spectroscopy of 241Am, 238Pu and 239Pu using a dual-stage peltier-cooled 25 mm2 silicon drift detector and alpha spectroscopy with a passivated ion implanted planar silicon detector. The conversion electron spectra were evaluated from 20-55 keV based on fits to the dominant conversion electron emissions, which allowed the relative conversion electron emission intensities to be determined. These measurements provide crucial singles spectral information and calibration to aid in the coincident measurement approach. Furthermore, an alpha-conversion electron spectrometer was assembled using the silicon based detectors described and results of a coincident spectrum analysis is reported for 241Am.

  5. Transmutation of 129I, 237Np, 238Pu, 239Pu, and 241Am using neutrons produced in target-blanket system 'Energy plus Transmutation' by relativistic protons

    NASA Astrophysics Data System (ADS)

    Adam, J.; Katovsky, K.; Balabekyan, A.; Kalinnikov, V. G.; Krivopustov, M. I.; Kumawat, H.; Solnyshkin, A. A.; Stegailov, V. I.; Stetsenko, S. G.; Tsoupko-Sitnikov, V. M.; Westmeier, W.

    2007-02-01

    Target-blanket facility `Energy + Transmutation' was irradiated by proton beam extracted from the Nuclotron Accelerator in Laboratory of High Energies of Joint Institute for Nuclear Research in Dubna, Russia. Neutrons generated by the spallation reactions of 0.7, 1.0, 1.5 and 2 GeV protons and lead target interact with subcritical uranium blanket. In the neutron field outside the blanket, radioactive iodine, neptunium, plutonium and americium samples were irradiated and transmutation reaction yields (residual nuclei production yields) have been determined using g-spectroscopy. Neutron field's energy distribution has also been studied using a set of threshold detectors. Results of transmutation studies of 129I, 237Np, 238Pu, 239Pu and 241Am are presented.

  6. Comparative toxicity of /sup 226/Ra, /sup 239/Pu, /sup 241/Am, /sup 249/Cf, and /sup 252/Cf in C57BL/Do black and albino mice

    SciTech Connect

    Taylor, G.N.; Mays, C.W.; Lloyd, R.D.; Gardner, P.A.; Talbot, L.R.; McFarland, S.S.; Pollard, I.A.; Atherton, D.R.; VanMoorhem, D.; Brammer, D.

    1983-09-01

    Groups of C57BL/Do (black and albino) mice were injected with graded activities of /sup 226/Ra, /sup 239/Pu, /sup 241/Am, /sup 249/Cf, or /sup 252/Cf and were followed throughout life. Bone sarcoma was the principal radiation-induced end point, and the risks associated with average skeletal doses of the four transuranium radionuclides, relative to radium, were determined. The relative biological effectiveness (RBE) was calculated for each emitter by dividing its risk coefficient (bone sarcomas per 10(/sup 6/) mouse-rad) by the risk coefficient for /sup 226/Ra. Combined data for males and females in both black and albino mice gave the following values +/- SD for the RBE relative to /sup 226/Ra . 1.0: /sup 239/Pu . 15.3 +/- 3.9, /sup 241/Am . 4.9 +/- 1.4, /sup 249/Cf . 5.0 +/- 1.4, and /sup 252/Cf . 2.6 +/- 0.8. About 70% of the tumors occurred in the axial skeleton, and the risk coefficient for females averaged about four times higher than for males when all five nuclides were included. The RBE of fission fragment irradiation from /sup 252/Cf for cancer induction, relative to alpha irradiation, for the combined data in all of the animals given /sup 252/Cf and /sup 249/Cf, was 0.02 +/- 0.28, in agreement with the calculated theoretical value of 0.03, based on the ratio of summed track lengths in tissue.

  7. Comparative toxicity of /sup 226/Ra, /sup 239/Pu, /sup 241/Am, /sup 249/Cf, and /sup 252/Cf in C57BL/Do black and albino mice

    SciTech Connect

    Taylor, G.N.; Mays, C.W.; Lloyd, R.D.; Gardner, P.A.; TAlbot, L.R.; McFarland, S.S.; Pollard, T.A.; Atherton, D.R.; vanMoorhem, D.; Brammer, D.

    1983-09-01

    Groups of C57BL/Do (black and albino) mice were injected with graded activities of /sup 226/Ra, /sup 239/Pu, /sup 241/Am, /sup 249/Cf, or /sup 252/Cf and were followed throughout life. Bone sarcoma was the principal radiation-induced end point, and the risks associated with average skeletal doses of the four transuranium radionuclides, relative to radium, were determined. The relative biological effectiveness (RBE) was calculated for each emitter by dividing its risk coefficient (bone sarcomas per 10/sup 6/ mouse-rad) by the risk coefficient for /sup 226/Ra. Combined data for males and females in both black and albino mice gave the following values +- SD for the RBE relative to /sup 226/Ra = 1.0: /sup 239/Pu = 15.3 +- 3.9, /sup 241/Am = 4.9 +- 1.4, /sup 249/Cf = 5.0 +- 1.4, and /sup 252/Cf = 2.6 +- 0.8. About 70% of the tumors occurred in the axial skeleton, and the risk coefficient for females averaged about four times higher than for males when all five nuclides were included. The RBE of fission fragment irradiation from /sup 252/Cf for cancer induction, relative to ..cap alpha.. irradiation, for the combined data in all of the animals given /sup 252/Cf and /sup 249/Cf, was 0.02 +- 0.28, in agreement with the calculated theoretical value of 0.03, based on the ratio of summed track lengths in tissue.

  8. Determination of (235)U, (239)Pu, (240)Pu, and (241)Am in a nuclear bomb particle using a position-sensitive α-γ coincidence technique.

    PubMed

    Peräjärvi, Kari A; Ihantola, Sakari; Pöllänen, Roy C; Toivonen, Harri I; Turunen, Jani A

    2011-02-15

    A nuclear bomb particle containing 1.6 ng of Pu was investigated nondestructively with a position-sensitive α detector and a broad-energy HPGe γ-ray detector. An event-mode data acquisition system was used to record the data. α-γ coincidence counting was shown to be well suited to nondestructive isotope ratio determination. Because of the very small background, the 51.6 keV γ rays of (239)Pu and the 45.2 keV γ rays of (240)Pu were identified, which enabled isotopic ratio calculations. In the present work, the (239)Pu/((239)Pu+(240)Pu) atom ratio was determined to be 0.950 ± 0.010. The uncertainties were much smaller than in the previous more conventional nondestructive studies on this particle. Obtained results are also in good agreement with the data from the destructive mass spectrometric studies obtained previously by other investigators.

  9. Neutron-induced fission cross section measurement of 233U, 241Am and 243Am in the energy range 0.5 MeV ⩽ En ⩽ 20 MeV at n_TOF at CERN

    NASA Astrophysics Data System (ADS)

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

    2012-10-01

    Neutron-induced fission cross section measurements of 233U, 243Am and 241Am relative to 235U have been carried out at the neutron time-of-flight facility n_TOF at CERN. A fast ionization chamber has been employed. All samples were located in the same detector; therefore the studied elements and the reference 235U target are subject to the same neutron beam.

  10. Analysis of plutonium isotope ratios including (238)Pu/(239)Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS.

    PubMed

    Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

    2017-04-01

    Isotope ratio analysis of individual uranium-plutonium (U-Pu) mixed oxide particles contained within environmental samples taken from nuclear facilities is proving to be increasingly important in the field of nuclear safeguards. However, isobaric interferences, such as (238)U with (238)Pu and (241)Am with (241)Pu, make it difficult to determine plutonium isotope ratios in mass spectrometric measurements. In the present study, the isotope ratios of (238)Pu/(239)Pu, (240)Pu/(239)Pu, (241)Pu/(239)Pu, and (242)Pu/(239)Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the (240)Pu/(239)Pu, (241)Pu/(239)Pu, and (242)Pu/(239)Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of plutonium with UTEVA resins. Furthermore, (238)Pu/(239)Pu isotope ratios were able to be calculated by using both the (238)Pu/((239)Pu+(240)Pu) activity ratios that had been measured through alpha spectrometry and the (240)Pu/(239)Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including (238)Pu/(239)Pu, in individual U-Pu mixed oxide particles.

  11. Neutron Capture Cross Section of 239Pu

    NASA Astrophysics Data System (ADS)

    Mosby, S.; Arnold, C.; Bredeweg, T. A.; Couture, A.; Jandel, M.; O'Donnell, J. M.; Rusev, G.; Ullmann, J. L.; Chyzh, A.; Henderson, R.; Kwan, E.; Wu, C. Y.

    2014-09-01

    The 239Pu(n,γ) cross section has been measured over the energy range 10 eV - 10 keV using the Detector for Advanced Neutron Capture Experiments (DANCE) as part of a campaign to produce precision (n,γ) measurements on 239Pu in the keV region. Fission coincidences were measured with a PPAC and used to characterize the prompt fission γ-ray spectrum in this region. The resulting spectra will be used to better characterize the fission component of another experiment with a thicker target to extend the (n,γ) cross section measurement well into the keV region.

  12. A feasibility study for transportable 241Am-in-lung and 241Am-in-nose-blow monitoring systems for use following a weapons accident.

    PubMed

    Youngman, M J; Etherington, G; Smith, J R H

    2003-01-01

    In a nuclear weapon accident involving fire or conventional explosion, most of the radiation dose received by people in the immediate vicinity would result from inhalation of 239Pu. This is accompanied by the nuclide 241Am, which is much easier to determine by external counting because of the 60 keV gamma ray emission. In the event of an accident, a priority would be to identify any people who have had intakes of 239Pu which were so large that decorporation therapy should be considered. Direct measurement of lung content provides the most rapid and convenient method for assessing intakes by inhalation. A transportable system has been considered as this could be deployed close to the site of the accident and would allow rapid measurements to be made. The feasibility of a transportable 241Am-in-nose-blow and nasal swab measurement system has also been considered. This would be used to help select people for 241Am-in-lung measurements.

  13. Neutron Capture Cross Section of 239Pu

    NASA Astrophysics Data System (ADS)

    Mosby, S.; Arnold, C.; Bredeweg, T. A.; Chyzh, A.; Couture, A.; Henderson, R.; Jandel, M.; Kwan, E.; O'Donnell, J. M.; Rusev, G.; Ullmann, J. L.; Wu, C. Y.

    2014-05-01

    The Detector for Advanced Neutron Capture Experiments (DANCE) has been used to measure the 239Pu(n,γ) cross section from 10 eV to the keV region. Three experimental run conditions were used to characterize the prompt fission γ-ray spectrum across the entire energy regime, measure the cross section in the resolved resonance region, and obtain necessary count rate well into the keV region. The preliminary cross sections are in good agreement with current evaluations from 10 eV to 80 keV.

  14. Bone tumor location in dogs given skeletal irradiation by {sup 239}Pu or {sup 226}Ra

    SciTech Connect

    Lloyd, R.D.; Taylor, G.N.; Miller, S.C.

    1997-10-01

    Statistical analyses have indicated that there was a significant difference between dogs injected with bone volume-seeking {sup 226} Ra as compared to those given bone surface-seeking {sup 239}Pu with respect to location within the skeleton of 334 radiation-induced primary bone malignancies. Corresponding differences also were event when dogs given bone volume-seeking {sup 90}Sr or bone surface-seeking {sup 241}Am, {sup 228}Th {sup 248,252}Cf, or {sup 224}Ra (which decays mostly on bone surfaces because of its short, 3.6 d half time) were included along with the {sup 226}Ra or {sup 239}Pu, respectively (562 total tumors). Further analysis suggested that higher values of percent red marrow (M) and bone turnover rate (R) are correlated with increased probability. of tumor appearance at a particular location within the skeleton for the surface seekers. Proportionately higher values of M and R are associated with skeletal sites containing mostly trabecular bone as compared to those with mostly compact (cortical) bone. Coefficients of determination (r{sup 2}) for the relationship between percent of total tumors vs the combination of percent red marrow and turnover rate (= MR) was about 0.7 for the surface seekers but only about 0.1 for the volume seekers. This indicates that the neoplastic effects of surface seekers, but not volume seekers, are associated with the presence of trabecular bone at the various sites of radio nuclide deposition within the skeleton. 10 refs., 3 tabs.

  15. 239Pu Resonance Evaluation for Thermal Benchmark System Calculations

    SciTech Connect

    Leal, Luiz C; Noguere, G; De Saint Jean, C; Kahler, A.

    2013-01-01

    Analyses of thermal plutonium solution critical benchmark systems have indicated a deciency in the 239Pu resonance evaluation. To investigate possible solutions to this issue, the Organisation for Economic Co-operation and Development (OECD) Nuclear Energy Agency (NEA) Working Party for Evaluation Cooperation (WPEC) established Subgroup 34 to focus on the reevaluation of the 239Pu resolved resonance parameters. In addition, the impacts of the prompt neutron multiplication (nubar) and the prompt neutron ssion spectrum (PFNS) have been investigated. The objective of this paper is to present the results of the 239Pu resolved resonance evaluation eort.

  16. 239Pu Resonance Evaluation for Thermal Benchmark System Calculations

    NASA Astrophysics Data System (ADS)

    Leal, L. C.; Noguere, G.; de Saint Jean, C.; Kahler, A. C.

    2014-04-01

    Analyses of thermal plutonium solution critical benchmark systems have indicated a deficiency in the 239Pu resonance evaluation. To investigate possible solutions to this issue, the Organisation for Economic Co-operation and Development (OECD) Nuclear Energy Agency (NEA) Working Party for Evaluation Cooperation (WPEC) established Subgroup 34 to focus on the reevaluation of the 239Pu resolved resonance parameters. In addition, the impacts of the prompt neutron multiplicity (νbar) and the prompt neutron fission spectrum (PFNS) have been investigated. The objective of this paper is to present the results of the 239Pu resolved resonance evaluation effort.

  17. Concordant 241Pu-241Am Dating of Environmental Samples: Results from Forest Fire Ash

    NASA Astrophysics Data System (ADS)

    Goldstein, S. J.; Oldham, W. J.; Murrell, M. T.; Katzman, D.

    2010-12-01

    We have measured the Pu, 237Np, 241Am, and 151Sm isotopic systematics for a set of forest fire ash samples from various locations in the western U.S. including Montana, Wyoming, Idaho, and New Mexico. The goal of this study is to develop a concordant 241Pu (t1/2 = 14.4 y)-241Am dating method for environmental collections. Environmental samples often contain mixtures of components including global fallout. There are a number of approaches for subtracting the global fallout component for such samples. One approach is to use 242Pu/239Pu as a normalizing isotope ratio in a three-isotope plot, where this ratio for the non-global fallout component can be estimated or assumed to be small. This study investigates a new, complementary method of normalization using the long-lived fission product, 151Sm (t1/2 = 90 y). We find that forest fire ash concentrates actinides and fission products with ~1E10 atoms 239Pu/g and ~1E8 atoms 151Sm/g, allowing us to measure these nuclides by mass spectrometric (MIC-TIMS) and radiometric (liquid scintillation counting) methods. The forest fire ash samples are characterized by a western U.S. regional isotopic signature representing varying mixtures of global fallout with a local component from atmospheric testing of nuclear weapons at the Nevada Test Site (NTS). Our results also show that 151Sm is well correlated with the Pu nuclides in the forest fire ash, suggesting that these nuclides have similar geochemical behavior in the environment. Results of this correlation indicate that the 151Sm/239Pu atom ratio for global fallout is ~0.164, in agreement with an independent estimate of 0.165 based on 137Cs fission yields for atmospheric weapons tests at the NTS. 241Pu-241Am dating of the non-global fallout component in the forest fire ash samples yield ages in the late 1950’s-early 1960’s, consistent with a peak in NTS weapons testing at that time. The age results for this component are in agreement using both 242Pu and 151Sm normalizations

  18. Soft tissue tumors induced by monomeric {sup 239}Pu

    SciTech Connect

    Lloyd, R.D.; Angus, W.; Taylor, G.N.; Miller, S.C.

    1995-10-01

    Individual records of soft tissue tumor occurrence (lifetime incidence) among 236 beagles injected with {sup 239}Pu citrate as young adults and 131 comparable control beagles given no radioactivity enabled us to analyze the possible effects on soft tissue tumor induction resulting from internal exposure to {sup 239}Pu. A significant trend was identified in the proportion of animals having malignant liver tumors with increasing radiation dose from {sup 239}. There was also a significant difference in the relative numbers of both malignant liver tumors (18.1 expected, 66 observed). Malignant tumors of the mouth, pancreas, and skin were more frequent among controls than among the dogs given {sup 239}Pu as well as tumors (malignant plus benign) of the mouth, pancreas, testis, and vagina. For all other tumor sites or types, there was no significant difference for both malignant and all (malignant plus benign) tumors. Mammary tumor occurrence appeared not to be associated with {sup 239}Pu incorporation. We conclude that the only soft-tissue neoplasia induced by the intake of {sup 239}Pu directly into blood is probably a liver tumor. 20 refs., 6 tabs.

  19. AN INTERLABORATORY COMPARISON ON THE DETERMINATION OF 241Am, 244Cm AND 252Cf IN URINE.

    PubMed

    Gerstmann, Udo C; Taubner, Kerstin; Hartmann, Martina

    2016-09-01

    An intercomparison exercise on the determination of (241)Am, (244)Cm and (252)Cf in urine was performed. Since it was designed with regard to emergency preparedness, the detection limit for each nuclide was set to 0.1 Bq per 24-h urine sample. Most of the participating laboratories were established bioassay laboratories. However, some laboratories that routinely determine (241)Am only in environmental samples were also invited in order to explore their potential for emergency bioassay analysis. Another aspect of the intercomparison was to investigate the performance of all laboratories concerning the chemical yields of the (243)Am tracer in comparison with (244)Cm and (252)Cf. In summary, both types of laboratories showed good results. There was a negative bias for the results of (244)Cm and (252)Cf, which can be explained by slightly different radiochemical behaviours of americium, curium and californium and which is in agreement with results reported in the literature.

  20. Beneficial uses of /sup 241/Am

    SciTech Connect

    Mangeng, C.A.; Thayer, G.R.

    1984-05-01

    This report assesses the uses of /sup 241/Am and the associated costs and supply. The study shows that /sup 241/Am-fueled radioisotope thermoelectric generators in the range of 1 to 5 W electrical provide the most promising use of kilogram amounts of this isotope. For medical uses, where purity is essential, irradiation of /sup 241/Am can produce 97% pure /sup 238/Pu at $21,000/g. Using a pyro-metallurgical process, /sup 241/Am could be recovered from molten salt extraction (MSE) residues at an estimated incremental cost of $83/g adjusted to reflect the disposal costs of waste products. This cost of recovery is less than the $300/g cost for disposal of the /sup 241/Am contained in the MSE residues.

  1. Transport of (137)Cs, (241)Am and Pu isotopes in the Curonian Lagoon and the Baltic Sea.

    PubMed

    Lujanienė, G; Remeikaitė-Nikienė, N; Garnaga, G; Jokšas, K; Šilobritienė, B; Stankevičius, A; Šemčuk, S; Kulakauskaitė, I

    2014-01-01

    Activities of (137)Cs, (241)Am and (239,240)Pu were analyzed with special emphasis on better understanding of radionuclide transport from land via the Neman River estuaries to the Baltic Sea and behavior in the marine environment. Although activity concentrations of (137)Cs in water samples collected the Baltic Sea were almost 100 times higher as compared to the Curonian Lagoon, its activities in the bottom sediments were found to be comparable. Activity (238)Pu/(239,240)Pu and atom (240)Pu/(239)Pu ratios indicated a different contribution of the Chernobyl-originated Pu to the suspended particulate matter (SPM) and bottom sediments. The largest amount of the Chernobyl-derived Pu was found in the smallest suspended matter particles of 0.2-1 μm in size collected in the Klaipeda Strait in 2011-2012. The decrease of characteristic activity (238)Pu/(239,240)Pu and atom (240)Pu/(239)Pu ratios towards the global fallout ones in surface soil and the corresponding increase of plutonium (Pu) ratios in the suspended particulate matter and bottom sediments have indicated that the Chernobyl-derived Pu, primarily deposited on the soil surface, was washed out and transported to the Baltic Sea. Behavior of (241)Am was found to be similar to that of Pu isotopes.

  2. Radionuclide concentrations in soils and vegetation at Low-Level Radioactive Waste Disposal Area G during the 1998 growing season (with a cumulative summary of {sup 3}H and {sup 239}Pu over time)

    SciTech Connect

    P. R. Fresquez; M. H. Ebinger; R. J. Wechsler; L. Naranjo, Jr.

    1999-11-01

    Soils and unwashed overstory and understory vegetation were collected at eight locations within and around Area G, a disposal facility for low-level, radioactive solid waste at Los Alamos National Laboratory. The samples were analyzed for {sup 3}H, {sup 238}Pu, {sup 239}Pu, {sup 90}Sr, {sup 241}Am, {sup 137}Cs, {sup tot}U. Most of the radionuclide concentrations in soils and vegetation were within the upper 95% level of background concentrations except for {sup 3}H and {sup 239}Pu. Tritium concentrations in vegetation from most sites were greater than background concentrations of about 2 pCi mL{sup {minus}1}. The concentrations of {sup 239}Pu in soils and understory vegetation were largest in samples collected several meters north of the transuranic waste pad area and were consistent with previous results. Based on {sup 3}H and {sup 239}Pu data through 1998, it was shown that concentrations were (1) significantly greater than background concentrations (p < 0.05) in soils and vegetation collected from most locations at Area G, and (2) there was no systematic increase or decrease in concentrations with time apparent in the data.

  3. Neutron Resonance Parameters and Covariance Matrix of 239Pu

    SciTech Connect

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

    2008-08-01

    In order to obtain the resonance parameters in a single energy range and the corresponding covariance matrix, a reevaluation of 239Pu was performed with the code SAMMY. The most recent experimental data were analyzed or reanalyzed in the energy range thermal to 2.5 keV. The normalization of the fission cross section data was reconsidered by taking into account the most recent measurements of Weston et al. and Wagemans et al. A full resonance parameter covariance matrix was generated. The method used to obtain realistic uncertainties on the average cross section calculated by SAMMY or other processing codes was examined.

  4. AMS of natural 236U and 239Pu produced in uranium ores

    NASA Astrophysics Data System (ADS)

    Wilcken, K. M.; Barrows, T. T.; Fifield, L. K.; Tims, S. G.; Steier, P.

    2007-06-01

    The rare isotopes 236U and 239Pu are produced naturally by neutron capture in uranium ores. Here we measure 236U and 239Pu by accelerator mass spectrometry (AMS) in the same ore samples for the first time. To ensure efficient extraction of both elements and isotopic equilibrium between the 239Pu in the ore and a 242Pu spike, we developed a new sample preparation protocol. AMS has clear advantages over previous methods because it achieves better discrimination against molecular interferences with higher sensitivity and shorter counting times. Measurements of 236U and 239Pu hold considerable promise as proxy indicators of neutron flux and uranium concentration.

  5. Vertical distributions of radionuclides ((239+240)Pu, (240)Pu/(239)Pu, and (137)Cs) in sediment cores of Lake Bosten in Northwestern China.

    PubMed

    Liao, Haiqing; Bu, Wenting; Zheng, Jian; Wu, Fengchang; Yamada, Masatoshi

    2014-04-01

    Artificial radionuclides ((137)Cs, (239+240)Pu, (241)Pu, (241)Am) deposited in lacustrine sediments have been used for dating as well as radionuclide source identification. In the present work, we investigated the vertical distributions of (239+240)Pu and (137)Cs activities, (240)Pu/(239)Pu atom ratios, and (239+240)Pu/(137)Cs activity ratios in sediment cores collected from Lake Bosten, which is the lake closest to the Lop Nor Chinese Nuclear Weapon Test site in northwestern China. Uniformly high concentrations of (239+240)Pu and (137)Cs were found in the upper layers deposited since 1964 in the sediment cores, and these were controlled by the resuspension of soil containing radionuclides from the nearby land surface. As the Chinese nuclear tests varied remarkably in yield, the mixing of the tropospheric deposition from these tests and the stratospheric deposition of global fallout has led to a (240)Pu/(239)Pu atom ratio that is similar to that of global fallout and to a (239+240)Pu/(137)Cs activity ratio that is slightly higher than that of global fallout. However, a low (240)Pu/(239)Pu atom ratio of 0.080 and high (239+240)Pu/(137)Cs activity ratio of 0.087, significantly different from the global fallout values, were observed in one sediment core (07BS10-2), indicating the inhomogenous tropospheric deposition from the Chinese nuclear tests in Lake Bosten during 1967-1973. These results are important to understand the influence of the CNTs on the radionuclide contamination in Lake Bosten.

  6. Gamma-ray Output Spectra from 239 Pu Fission

    DOE PAGES

    Ullmann, John

    2015-05-25

    Gamma-ray multiplicities, individual gamma-ray energy spectra, and total gamma energy spectra following neutron-induced fission of 239Pu were measured using the DANCE detector at Los Alamos. Corrections for detector response were made using a forward-modeling technique based on propagating sets of gamma rays generated from a paramaterized model through a GEANT model of the DANCE array and adjusting the parameters for best fit to the measured spectra. The results for the gamma-ray spectrum and multiplicity are in general agreement with previous results, but the measured total gamma-ray energy is about 10% higher. A dependence of the gamma-ray spectrum on the gamma-raymore » multplicity was also observed. Global model calculations of the multiplicity and gamma energy distributions are in good agreement with the data, but predict a slightly softer total-energy distribution.« less

  7. Chronic cigarette smoke exposure increases the pulmonary retention and radiation dose of {sup 239}Pu inhaled as {sup 239}PuO{sub 2} by F344 rats

    SciTech Connect

    Finch, G.L.; Lundgren, D.L.; Barr, E.B.; Chen, B.T.; Griffith, W.C.; Hobbs, C.H.; Hoover, M.D.; Nikula, K.J.; Mauderly, J.L.

    1998-12-01

    As a portion of a study to examine how chronic cigarette smoke exposure might alter the risk of lung tumors from inhaled {sup 239}PuO{sub 2} in rats, the effects of smoke exposure on alpha-particle lung dosimetry over the life-span of exposed rats were determined. Male and female rats were exposed to inhaled {sup 239}PuO{sub 2} alone or in combination with cigarette smoke. Animals exposed to filtered air along served as controls for the smoke exposure. Whole-body exposure to mainstream smoke diluted to concentrations of either 100 or 250 mg total particulate matter m{sup {minus}3} began at 6 wk of age and continued for 6 h d{sup {minus}1}, 5 d wk{sup {minus}1}, for 30 mo. A single, pernasal, acute exposure to {sup 239}PuO{sub 2} was given to all rats at 12 wk of age. Exposure to cigarette smoke caused decreased body weight gains in a concentration dependent manner. Lung-to-body weight ratios were increased in smoke-exposed rats. Rats exposed to cigarette smoke before the {sup 239}PuO{sub 2} exposure deposited less {sup 239}Pu in the lung than did controls. Except for male rats exposed to LCS, exposure to smoke retarded the clearance of {sup 239}Pu from the lung compared to control rats through study termination at 870 d after {sup 239}PuO{sub 2} exposure. Radiation doses to lungs were calculated by sex and by exposure group for rats on study for at least 360 d using modeled body weight changes, lung-to-body weight ratios, and standard dosimetric calculations. For both sexes, estimated lifetime radiation doses from the time of {sup 239}PuO{sub 2} exposure to death were 3.8 Gy, 4.4 Gy, or 6.7 Gy for the control, LCS, or HCS exposure groups, respectively. Assuming an approximately linear dose-response relationship between radiation dose and lung neoplasm incidence, approximate increases of 20% or 80% in tumor incidence over controls would be expected in rats exposed to {sup 239}PuO{sub 2} and LCS or {sup 239}PuO{sub 2} and HCS, respectively.

  8. A Method for Continuous (239)Pu Determinations in Arctic and Antarctic Ice Cores.

    PubMed

    Arienzo, M M; McConnell, J R; Chellman, N; Criscitiello, A S; Curran, M; Fritzsche, D; Kipfstuhl, S; Mulvaney, R; Nolan, M; Opel, T; Sigl, M; Steffensen, J P

    2016-07-05

    Atmospheric nuclear weapons testing (NWT) resulted in the injection of plutonium (Pu) into the atmosphere and subsequent global deposition. We present a new method for continuous semiquantitative measurement of (239)Pu in ice cores, which was used to develop annual records of fallout from NWT in ten ice cores from Greenland and Antarctica. The (239)Pu was measured directly using an inductively coupled plasma-sector field mass spectrometer, thereby reducing analysis time and increasing depth-resolution with respect to previous methods. To validate this method, we compared our one year averaged results to published (239)Pu records and other records of NWT. The (239)Pu profiles from the Arctic ice cores reflected global trends in NWT and were in agreement with discrete Pu profiles from lower latitude ice cores. The (239)Pu measurements in the Antarctic ice cores tracked low latitude NWT, consistent with previously published discrete records from Antarctica. Advantages of the continuous (239)Pu measurement method are (1) reduced sample preparation and analysis time; (2) no requirement for additional ice samples for NWT fallout determinations; (3) measurements are exactly coregistered with all other chemical, elemental, isotopic, and gas measurements from the continuous analytical system; and (4) the long half-life means the (239)Pu record is stable through time.

  9. Plutonium isotopes and 241Am in the atmosphere of Lithuania: A comparison of different source terms

    NASA Astrophysics Data System (ADS)

    Lujanienė, G.; Valiulis, D.; Byčenkienė, S.; Šakalys, J.; Povinec, P. P.

    2012-12-01

    137Cs, 241Am and Pu isotopes collected in aerosol samples during 1994-2011 were analyzed with special emphasis on better understanding of Pu and Am behavior in the atmosphere. The results from long-term measurements of 240Pu/239Pu atom ratios showed a bimodal frequency distribution with median values of 0.195 and 0.253, indicating two main sources contributing to the Pu activities at the Vilnius sampling station. The low Pu atom ratio of 0.141 could be attributed to the weapon-grade plutonium derived from the nuclear weapon test sites. The frequency of air masses arriving from the North-West and North-East correlated with the Pu atom ratio indicating the input from the sources located in these regions (the Novaya Zemlya test site, Siberian nuclear plants), while no correlation with the Chernobyl region was observed. Measurements carried out during the Fukushima accident showed a negligible impact of this source with Pu activities by four orders of magnitude lower as compared to the Chernobyl accident. The activity concentration of actinides measured in the integrated sample collected in March-April, 2011 showed a small contribution of Pu with unusual activity and atom ratios indicating the presence of the spent fuel of different origin than that of the Chernobyl accident.

  10. Neutron transmission and capture of 241Am

    NASA Astrophysics Data System (ADS)

    Lampoudis, C.; Kopecky, S.; Plompen, A.; Schillebeeckx, P.; Wynants, R.; Gunsing, F.; Sage, C.; Bouland, O.; Noguere, G.

    2013-03-01

    A set of neutron transmission and capture experiments based on the Time Of Flight (TOF) technique, were performed in order to determine the 241Am capture cross section in the energy range from 0.01 eV to 1 keV. The GELINA facility of the Institute for Reference Materials and Measurements (IRMM) served as the neutron source. A pair of C6D6 liquid scintillators was used to register the prompt gamma rays emerging from the americium sample, while a Li-glass detector was used in the transmission setup. Results from the capture and transmission data acquired are consistent with each other, but appear to be inconsistent with the evaluated data files. Resonance parameters have been derived for the data up to the energy of 100 eV.

  11. Plant uptake and transport of /sup 241/Am

    SciTech Connect

    Wallace, A.; Romney, E.M.; Mueller, R.T. Sr.; soufi, S.M.

    1981-07-01

    We conducted several experiments with /sup 241/Am to obtain a more complete understanding of how this transuranium element is absorbed and transported in plants. In a plant species (Tamarix pentandra Pall.) that has salt glands in the leaves excreting NaCl and other ions, /sup 241/Am was not pumped through these glands. Cyanide, which forms complexes with any metals, when applied to a calcareous soil, greatly increased the transport of /sup 241/Am into stems and leaves of bush bean plants. Radioactive cyanide (/sup 14/C) was also transported to leaves and stems. When radish was grown in both calcareous and noncalcareous soils, /sup 241/Am appeared to be fixed on the peel so firmly that it was resistant to removal by HNO/sub 3/ washing. The chelating agent DTPA induced increased transport of /sup 241/Am to leaves and into the fleshy roots of the radish.

  12. Distribution of sup 137 Cs, sup 90 Sr, sup 238 Pu, sup 239 Pu, sup 241 Am and sup 244 Cm in Pond B, Savannah River Site

    SciTech Connect

    Whicker, F.W. ); Pinder, J.E. III; Bowling, J.W. ); Alberts, J.J. . Marine Inst.); Brisbin, I.L. Jr. )

    1989-05-01

    The gradual senescence of present-day operating nuclear facilities, and resultant contamination of aquatic and terrestrial ecosystems, emphasize the importance of understanding the behavior of radionuclides in the environment. Observations and deductions concerning mechanisms of radionuclide transport can contribute significantly to knowledge of fundamental ecological processes. This study emphasized the ecosystem-level distribution of several long-lived radionuclides in an abandoned reactor cooling impoundment after a twenty year period of chemical and biological equilibration. 90 refs., 14 figs., 5 tabs.

  13. Transmutation of 129I, 237Np, 238Pu, 239Pu and 241Am Using Neutrons Produced in Target-Blanket System ``Energy & Transmutation'' Bombarded by Relativistic Protons

    NASA Astrophysics Data System (ADS)

    Adam, J.; Katovsky, K.; Balabekyan, A.; Solnyshkin, A. A.; Kalinnikov, V. G.; Stegailov, V. I.; Tsoupko-Sitnikov, V. M.; Stetsenko, S. G.; Krivopustov, M. I.; Pronskikh, V. S.; Vladimirova, N. M.; Kumawat, H.

    2005-05-01

    Target-blanket facility "Energy & Transmutation" was irradiated by a 2 GeV proton beam extracted from the Nuclotron Accelerator at the Joint Institute for Nuclear Research in Dubna, Russia. Radioactive samples made from iodine, neptunium, plutonium and americium were irradiated by spallation neutrons produced in the "E&T" facility. Transmutation reaction yields (residual nuclei production yields) have been determined using methods of γ-spectroscopy. The energy spectrum of the neutron field has been studied by using a set of threshold detectors.

  14. 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.

  15. Determination of (239)Pu, (240)Pu, (241)Pu and (242)Pu at femtogram and attogram levels - evidence for the migration of fallout plutonium in an ombrotrophic peat bog profile.

    PubMed

    Quinto, Francesca; Hrnecek, Erich; Krachler, Michael; Shotyk, William; Steier, Peter; Winkler, Stephan R

    2013-04-01

    The isotopic composition of plutonium ((239)Pu, (240)Pu, (241)Pu and (242)Pu) was investigated in a ∼0.5 m long peat core from an ombrotrophic bog (Black Forest, Germany) using clean room procedures and accelerator mass spectrometry (AMS). This sophisticated analytical approach was ultimately needed to detect reliably the Pu concentrations present in the peat samples at femtogram (fg) and attogram (ag) levels. The mean (240)Pu/(239)Pu isotopic ratio of 0.19 ± 0.02 (N = 32) in the peat layers, representing approximately the last 80 years, was in good agreement with the accepted value of 0.18 for the global fallout in the Northern Hemisphere. This finding is largely supported by the corresponding and rather constant (241)Pu/(239)Pu (0.0012 ± 0.0005) and (242)Pu/(239)Pu (0.004 ± 0.001) ratios. Since the Pu isotopic composition characteristic of the global fallout was also identified in peat samples pre-dating the period of atmospheric atom bomb testing (AD 1956-AD 1980), migration of Pu within the peat profile is clearly indicated. These results highlight, for the first time, the mobility of Pu in a peat bog with implications for the migration of Pu in other acidic, organic rich environments such as forest soils and other wetland types. These findings constitute a direct observation of the behaviour of Pu at fg and ag levels in the environment. The AMS measurements of Pu concentrations (referring to a corresponding activity of (240+239)Pu from 0.07 mBq g(-1) to 5 mBq g(-1)) essentially confirm our a priori estimates based on existing (241)Am and (137)Cs data in the investigated peat core and agree well with the global fallout levels from the literature. Exclusively employing the Pu isotope ratios established for the peat samples, the date of the Pu irradiation (AD 1956, correctable to AD 1964) was calculated and subsequently compared to the (210)Pb age of the peat layers; this comparison provided an additional hint that global fallout derived Pu is not fixed in

  16. Sensitivities of five alpha continuous air monitors for detection of airborne {sup 239}Pu

    SciTech Connect

    McIsaac, C.V.; Amaro, C.R.

    1992-07-01

    Results of measurements of the sensitivities of five alpha continuous air monitors (CAMs) for detection of airborne {sup 239}Pu are presented. Four commercially available alpha CAMs (Kurz model 8311, Merlin Gerin Edgar, RADeCO model 452, and Victoreen model 758) and a prototype alpha CAM currently in use at Argonne National Laboratory- West (ANL-W) were tested sampling natural ambient air and laboratory-generated atmospheres laden with either blank dust or dust containing nCi/g concentrations of {sup 239}Pu. Cumulative alpha spectra were stored at 30 or 60 minute intervals during each sampling and were subsequently analyzed using three different commonly used alpha spectrum analysis algorithms. The effect of airborne dust concentration and sample filter porosity on detector resolution and sensitivity for airborne {sup 239}Pu are described.

  17. Sensitivities of five alpha continuous air monitors for detection of airborne sup 239 Pu

    SciTech Connect

    McIsaac, C.V.; Amaro, C.R.

    1992-07-01

    Results of measurements of the sensitivities of five alpha continuous air monitors (CAMs) for detection of airborne {sup 239}Pu are presented. Four commercially available alpha CAMs (Kurz model 8311, Merlin Gerin Edgar, RADeCO model 452, and Victoreen model 758) and a prototype alpha CAM currently in use at Argonne National Laboratory- West (ANL-W) were tested sampling natural ambient air and laboratory-generated atmospheres laden with either blank dust or dust containing nCi/g concentrations of {sup 239}Pu. Cumulative alpha spectra were stored at 30 or 60 minute intervals during each sampling and were subsequently analyzed using three different commonly used alpha spectrum analysis algorithms. The effect of airborne dust concentration and sample filter porosity on detector resolution and sensitivity for airborne {sup 239}Pu are described.

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

    NASA Astrophysics Data System (ADS)

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

    2008-10-01

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

  19. Fission Cross-section Measurements of (233)U, (245)Cm and (241,243)Am at CERN n_TOF Facility

    SciTech Connect

    Calviani, M.; Koehler, Paul Edward; N_TOF collaboration,

    2011-01-01

    Neutron-induced fission cross-sections of minor actinides have been measured using the n-TOF white neutron source at CERN, Geneva, as part of a large experimental program aiming at collecting new data relevant for nuclear astrophysics and for the design of advanced reactor systems. The measurements at n-TOF take advantage of the innovative features of the n-TOF facility, namely the wide energy range, high instantaneous neutron flux and good energy resolution. Final results on the fission cross-section of {sup 233}U, {sup 245}Cm and {sup 243}Am from thermal to 20 MeV are here reported, together with preliminary results for {sup 241}Am. The measurement have been performed with a dedicated Fast Ionization Chamber (FIC), a fission fragment detector with a very high efficiency, relative to the very well known cross-section of {sup 235}U, measured simultaneously with the same detector.

  20. Potential of Vetiveria zizanoides L. Nash for phytoremediation of plutonium ((239)Pu): Chelate assisted uptake and translocation.

    PubMed

    Singh, Shraddha; Fulzele, D P; Kaushik, C P

    2016-10-01

    Plants have demonstrated a great potential to remove toxic elements from soils and solutions and been successfully used for phytoremediation of important radionuclides. Uptake potential of vetiver plants (V. zizanoides) for the remediation of (239)Pu in hydroponic and soil conditions was studied in the present work. High efficiency of V. zizanoides for the removal of (239)Pu was recorded with 66.2% being removed from the hydroponic solution after 30 days. However, remediation of (239)Pu from soil was limited. Remediation of (239)Pu from soil was increased with the addition of chelating agents citric acid (CA) and diethylenetriaminepentaacetic acid (DTPA). Accumulation of (239)Pu was recorded higher in roots than shoots, however its translocation from roots to shoots increased in the presence of chelators in hydroponic as well as soil conditions. DTPA was found more effective than CA showing higher translocation index (TI). Increase in TI was observed 8 and 6 times in the solution and soil respectively when plants were exposed to (239)Pu-DTPA in comparison to only (239)Pu. The present study demonstrates that V. zizanoides plant is a potential plant for phytoremediation of (239)Pu.

  1. Nucleogenic 36Cl, 236U and 239Pu in uranium ores

    NASA Astrophysics Data System (ADS)

    Wilcken, K. M.; Fifield, L. K.; Barrows, T. T.; Tims, S. G.; Gladkis, L. G.

    2008-08-01

    The nucleogenic isotopes 36Cl, 236U and 239Pu are produced naturally in subsurface environments via neutron capture of thermal and epithermal neutrons. Concentrations are, however, very low and accelerator mass spectrometry (AMS) is required for quantitative measurements. A particular challenge is presented by the measurement of 236U/ 238U ratios down to the level of 10 -13 that is expected from rocks with low uranium concentration. Here, we present the AMS methodology that has been developed at the ANU for measuring 236U/ 238U ratios at this level. The more established methodologies for 36Cl and 239Pu measurements are also summarised. These capabilities are then used to characterize the 36Cl, 236U and 239Pu concentrations in a range of uranium ores. A simple model of the neutron production and capture processes in subsurface environments has been developed and is presented. It is shown that nucleogenic 36Cl, 236U and 239Pu can be used to determine both thermal and epithermal neutron fluxes in subsurface environments. Potential applications include uranium exploration and monitoring of the environmental impact of uranium mining.

  2. Dosimetry studies on prototype 241Am sources for brachytherapy.

    PubMed

    Nath, R; Gray, L

    1987-06-01

    Sealed sources of 241Am emit primarily 60 keV photons which, because of multiple Compton scattering, produce dose distributions in water that are comparable to those from 226Ra or 137Cs. However, americium gamma rays can be shielded by thin layers of high atomic number materials since the half value layer thickness is only 1/8th of a mm of lead for americium gamma rays as compared to a value of 12 mm for 226Ra gamma rays. This may allow effective in vivo shielding of critical organs, for example; the bladder can be partially shielded by hypaque solution, and the rectum and sigmoid colon by barium sulfate. In addition, the exposure to medical personnel involved in intracavitary application and patient care may be reduced substantially by the use of relatively thin lead aprons and light weight, portable shields. To investigate the feasibility of 241Am sources for intracavitary irradiation, dosimetry studies on prototype 241Am sources have been performed and a computer model for the determination of dose distributions around encapsulated cylindrical sources of 241Am has been developed and tested. Results of dosimetry measurements using ionization chambers, lithium fluoride thermoluminescent dosimeters, a scanning scintillation probe, and film dosimetry, confirm theoretical predictions that these sources can deliver dose rates adequate for intracavitary irradiation. Further dosimetry measurements in simulated clinical situations using lead foils and test tubes filled with hypaque or barium sulfate, confirm the predicted effectiveness of in vivo shielding which can be readily achieved with 241Am sources.

  3. 241Am (n,gamma) isomer ratio measurement

    SciTech Connect

    Bond, Evelyn M; Vieira, David J; Moody, Walter A; Slemmons, Alice K

    2011-01-05

    The objective of this project is to improve the accuracy of the {sup 242}Cm/{sup 241}Am radiochemistry ratio. We have performed an activation experiment to measure the {sup 241}Am(n,{gamma}) cross section leading to either the ground state of {sup 242g}Am (t{sub 1/2} = 16 hr) which decays to {sup 242}Cm (t{sub 1/2} = 163 d) or the long-lived isomer {sup 242m}Am (t{sub 1/2} = 141 yr). This experiment will develop a new set of americium cross section evaluations that can be used with a measured {sup 242}Cm/{sup 241}Am radiochemical measurement for nuclear forensic purposes. This measurement is necessary to interpret the {sup 242}Cm/{sup 241}Am ratio because a good measurement of this neutron capture isomer ratio for {sup 241}Am does not exist. The targets were prepared in 2007 from {sup 241}Am purified from LANL stocks. Gold was added to the purified {sup 241}Am as an internal neutron fluence monitor. These targets were placed into a holder, packaged, and shipped to Forschungszentrum Karlsruhe, where they were irradiated at their Van de Graff facility in February 2008. One target was irradiated with {approx}25 keV quasimonoenergetic neutrons produced by the {sup 7}Li(p,n) reaction for 3 days and a second target was also irradiated for 3 days with {approx}500 keV neutrons. Because it will be necessary to separate the {sup 242}Cm from the {sup 241}Am in order to measure the amount of {sup 242}Cm by alpha spectrometry, research into methods for americium/curium separations were conducted concurrently. We found that anion exchange chromatography in methanol/nitric acid solutions produced good separations that could be completed in one day resulting in a sample with no residue. The samples were returned from Germany in July 2009 and were counted by gamma spectrometry. Chemical separations have commenced on the blank sample. Each sample will be spiked with {sup 244}Cm, dissolved and digested in nitric acid solutions. One third of each sample will be processed at a time

  4. Microscopic Calculation of Fission Fragment Energies for the 239Pu(nth,f) Reaction

    SciTech Connect

    Younes, W; Gogny, D

    2011-10-03

    We calculate the total kinetic and excitation energies of fragments produced in the thermal-induced fission of {sup 239}Pu. This result is a proof-of-principle demonstration for a microscopic approach to the calculation of fission-fragment observables for applied data needs. In addition, the calculations highlight the application of a fully quantum mechanical description of scission, and the importance of exploring scission configurations as a function of the moments of the fragments, rather than through global constraints on the moments of the fissioning nucleus. Using a static microscopic calculation of configurations at and near scission, we have identified fission fragments for the {sup 239}Pu (n{sub th}, f) reaction and extracted their total kinetic and excitation energies. Comparison with data shows very good overall agreement between theory and experiment. Beyond their success as a proof of principle, these calculations also highlight the importance of local constraints on the fragments themselves in microscopic calculations.

  5. Dependence of dose coefficients for inhaled 239Pu on absorption parameters.

    PubMed

    Suzuki, K; Sekimoto, H; Ishigure, N

    2001-01-01

    With regard to dissolution of particles in the respiratory tract after inhalation, the International Commission on Radiological Protection (ICRP) has classified all radionuclides into only three types according to the chemical form of compounds, and default values of absorption parameters are proposed for each type. However, it is just a simplification to estimate doses for practical use, and there is a possibility of unfitness in such an assortment. A code has been developed to reproduce the ICRP's dose coefficients for 239Pu, which is one of the most important elements for occupational exposure. By using this code, the respective absorption parameters were modified, and the effect owing to these changes evaluated. It was shown consequently that changes of absorption parameters do not greatly influence the effective doses of 239Pu for workers.

  6. Prompt γ-ray production in neutron-induced fission of 239Pu

    NASA Astrophysics Data System (ADS)

    Ullmann, J. L.; Bond, E. M.; Bredeweg, T. A.; Couture, A.; Haight, R. C.; Jandel, M.; Kawano, T.; Lee, H. Y.; O'Donnell, J. M.; Hayes, A. C.; Stetcu, I.; Taddeucci, T. N.; Talou, P.; Vieira, D. J.; Wilhelmy, J. B.; Becker, J. A.; Chyzh, A.; Gostic, J.; Henderson, R.; Kwan, E.; Wu, C. Y.

    2013-04-01

    Background: The prompt gamma-ray spectrum from fission is important for understanding the physics of nuclear fission, and also in applications involving fission. Relatively few measurements of the prompt gamma spectrum from 239Pu(n,f) have been published.Purpose: This experiment measured the multiplicity, individual gamma energy spectrum, and total gamma energy spectrum of prompt fission gamma rays from 239Pu(n,f) in the neutron energy range from thermal to 30 keV, to test models of fission and to provide information for applications.Method: Gamma rays from neutron-induced fission of 239Pu were measured using the DANCE gamma-ray calorimeter. Fission events were tagged by detecting fission products in a parallel-plate avalanche counter in the center of DANCE. The measurements were corrected for detector response using a geant4 model of DANCE. A detailed analysis for the gamma rays from the 1+ resonance complex at 10.93 eV is presented.Results: A six-parameter analytical parametrization of the fission gamma-ray spectrum was obtained. A Monte Carlo Hauser-Feshbach calculation provided good general agreement with the data, but some differences remain to be resolved.Conclusions: An analytic parametrization can be made of the gamma-ray multiplicity, energy distribution, and total-energy distribution for the prompt gamma rays following neutron-induced fission of 239Pu. This parametrization may be useful for applications. Modern Monte Carlo Hauser-Feshbach calculations can do a good job of calculating the fission gamma-ray emission spectrum, although some details remain to be understood.

  7. Distribution of skeletal malignancies in beagles injected with {sup 239}Pu citrate

    SciTech Connect

    Lloyd, R.D.; Taylor, G.N.; Angus, W.

    1994-04-01

    The distribution of skeletal malignancies among our beagles injected with {sup 239}Pu as young adults roughly seems to follow the distribution of skeletal mass and skeletal {sup 239}Pu. These findings are similar to those we reported previously for a group of dogs given {sup 226}Ra. Although there were differences in tumor distribution between the animals given {sup 239}Ra and those given {sup 239}Pu, most of them were not statistically significant; however, the radium dogs seemed to show a greater sensitivity to bone tumor origin in the tibia, while there may have been a tendency among the plutonium dogs toward increased relative sensitivity in the scapula, lumbar vertebrae, sacrum, and ribs. In contrast, the most common site for the formation of naturally-occurring bone malignancy in the dog is the distal radius. Perhaps there were too few tumors and too few dogs to establish statistical significance. A correlation between tumor location and at least two anatomical-physiological factors in the skeleton indicated that these two factors (site-specific bone turnover rate and percent of red marrow at the site, which is correlated with vascularity) may influence the appearance of malignancies both individually and in combination. Except for the femur, there appeared to be no difference between the relative distribution of skeletal malignancies of low-level (30 Bq-2 Bq kg{sup -1} injected) and high-level (3-122 kBq kg{sup -1}) dogs. Distribution of bone tumors between the axial and appendicular skeleton was 50% vs. 50% for {sup 239}Pu (42 and 42), but it was 39% axial vs. 61% appendicular (22 and 35, respectively) for dogs given {sup 226}Ra. This difference was not significant (p > 0.2). 15 refs., 4 tabs.

  8. Nevada test site fallout atom ratios: /sup 240/Pu//sup 239/Pu and /sup 241/Pu//sup 239/Pu

    SciTech Connect

    Hicks, H.G.; Barr, D.W.

    1984-02-01

    The exposure of the population in Utah to external gamma radiation from the fallout from nuclear weapons tests carried out between 1951 and 1958 at the Nevada Test Site (NTS) has been reconstructed from recent measurements of /sup 137/Cs and plutonium in soil. The fraction of /sup 137/Cs in the fallout from NTS events was calculated from the total plutonium and the /sup 240/Pu//sup 239/Pu ratios measured in the soil, using the values of 0.180 +- 0.006 and 0.032 +- 0.003 for that ratio in global fallout and NTS fallout, respectively. The total population exposure from NTS events was then calculated on the basis of exposure rates resulting from short-lived radionuclides associated with the /sup 137/Cs at the time of deposition. While the /sup 240/Pu//sup 239/Pu ratio is constant in global fallout, this ratio varies greatly in the fallout from individual events. While the composition of fallout on Utah from NTS events is rather uniform, the Off-Site Radiation Exposure Review Project is currently reconstructing radiation exposures for locations close to NTS where the fallout may be predominantly from one event. Therefore, the authors compiled the pertinent ratios in order to provide information concerning the exposure resulting from any individual event. The plutonium ratios measured at 30 days postshot were compiled from unpublished values in the archives of the Nuclear Chemistry Division of LLNL and INC-11 of LANL. These ratios are pertinent to fallout data. Dates for each event were taken from a publication by the Nevada Operations Office of the Department of Energy. 3 references.

  9. Chromosomal aberrations in lymphocytes of peripheral blood among Mayak facility workers who inhaled insoluble forms of 239PU.

    PubMed

    Okladnikova, N D; Scott, B R; Tokarskaya, Z B; Zhuntova, G V; Khokhryakov, V F; Syrchikov, V A; Grigoryeva, E S

    2005-01-01

    A cytogenetic study was performed on 79 plutonium (Pu) workers chronically exposed to alpha radiation from inhaled, low-transportable (insoluble) compounds of airborne 239Pu and to external gamma rays. Body burden estimates for 239Pu ranged from 0 to 15.5 kBq. Chromosomal aberrations (CAs) (stable and unstable) among peripheral blood lymphocytes and cumulative alpha radiation doses were evaluated approximately 25 y after first contact with 239Pu. For the cytogenetic analyses, a standard two-day peripheral blood lymphocyte culture technique was applied. While alpha radiation doses continually increase up to the time of cytogenetic measurements, significant gamma ray exposures essentially ceased long before the time of measurement, so that alpha and gamma doses were not correlated. For the exposed workers, the mean 239Pu body burden (estimate), evaluated at the time of the cytogenetic measurement, was 1.23 +/- 0.26 kBq and the corresponding mean absorbed external gamma ray dose (estimate) to the total body was 0.076 +/- 0.009 Gy. Single and multivariate regression analyses were performed on the CA data. Stable, unstable and total aberrations increased as the 239Pu body burden increased over the range 0-4.5 kBq. However, above this range little additional increase was observed. CAs were weakly correlated with time since the first intake of 239Pu. No relationship between chromatid aberrations and 239Pu incorporation was found. Unstable (but not stable) aberrations were correlated with gamma radiation dose. No significant relationship of CA and smoking was found.

  10. 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.

  11. Commentary on Inhaled 239PuO2 in Dogs — A Prophylaxis against Lung Cancer?

    DOE PAGES

    Cuttler, Jerry M.; Feinendegen, Ludwig E.

    2015-01-01

    Several studies on the effect of inhaled plutonium-dioxide particulates and the incidence of lung tumors in dogs reveal beneficial effects when the cumulative alpha-radiation dose is low. There is a threshold at an exposure level of about 100 cGy for excess tumor incidence and reduced lifespan. The observations conform to the expectations of the radiation hormesis dose-response model and contradict the predictions of the LNT hypothesis. These studies suggest investigating the possibility of employing low-dose alpha-radiation, such as from 239PuO2 inhalation, as a prophylaxis against lung cancer.

  12. Preliminary Evaluation and Uncertainty Quantification of the Prompt Fission Neutron Spectrum of {sup 239}Pu

    SciTech Connect

    Neudecker, D.; Talou, P.; Taddeucci, T.N.; Haight, R.C.; Kawano, T.; Lee, H.Y.; Smith, D.L.; Capote, R.; Rising, M.E.; White, M.C.

    2015-01-15

    Low evaluated uncertainties were obtained in a previous evaluation of the {sup 239}Pu prompt fission neutron spectrum and associated covariances for incident neutrons of 0.5 MeV, which were enlarged a-posteriori before being incorporated into ENDF/B-VII.1. These low evaluated uncertainties triggered an in-depth study and improved estimate of experimental as well as model uncertainties. Here, we will summarize these efforts and show that the improved estimate of experimental and model uncertainties leads to corresponding evaluated uncertainties in good agreement with uncertainties obtained in a statistical analysis based primarily on experimental information.

  13. Preliminary Evaluation and Uncertainty Quantification of the Prompt Fission Neutron Spectrum of 239Pu

    NASA Astrophysics Data System (ADS)

    Neudecker, D.; Talou, P.; Taddeucci, T. N.; Haight, R. C.; Kawano, T.; Lee, H. Y.; Smith, D. L.; Capote, R.; Rising, M. E.; White, M. C.

    2015-01-01

    Low evaluated uncertainties were obtained in a previous evaluation of the 239Pu prompt fission neutron spectrum and associated covariances for incident neutrons of 0.5 MeV, which were enlarged a-posteriori before being incorporated into ENDF/B-VII.1. These low evaluated uncertainties triggered an in-depth study and improved estimate of experimental as well as model uncertainties. Here, we will summarize these efforts and show that the improved estimate of experimental and model uncertainties leads to corresponding evaluated uncertainties in good agreement with uncertainties obtained in a statistical analysis based primarily on experimental information.

  14. Improving the Assay of 239Pu in Spent and Melted Fuel Using the Nuclear Resonance Fluorescence Integral Resonance Transmission Method

    NASA Astrophysics Data System (ADS)

    Angell, C. T.; Hayakawa, T.; Shizuma, T.; Hajima, R.; Quiter, B. J.; Ludewigt, B. A.; Karwowski, H.; Rich, G.

    2015-10-01

    Non-destructive assay (NDA) of 239Pu in spent nuclear fuel is possible using the isotope-specific nuclear resonance fluorescence (NRF) integral resonance transmission (IRT) method. The IRT method measures the absorption of photons from a quasi-monoenergetic γ-ray beam due to all resonances in the energy width of the beam. According to calculations the IRT method could greatly improve assay times for 239Pu in nuclear fuel. To demonstrate and verify the IRT method, the IRT signature was first measured in 181Ta, whose nuclear resonant properties are similar to those of 239Pu, and then measured in 239Pu. These measurements were done using the quasi-monoenergetic beam at the High Intensity γ-ray Source (HIγS) in Durham, NC, USA. The IRT signature was observed as a decrease in scattering strength when the same isotope material was placed upstream of the scattering target. The results confirm the validity of the IRT method in both 181Ta and 239Pu.

  15. The geochemistry of fallout plutonium in the North Atlantic: II. 240Pu /239Pu ratios and their significance

    NASA Astrophysics Data System (ADS)

    Buesseler, Ken O.; Sholkovitz, Edward R.

    1987-10-01

    A systematic decrease in the 240Pu /239Pu ratio in marine sediments is found with increasing water depth along a transect of cores between Woods Hole and Bermuda. The 240Pu /239Pu atom ratios range from ≅O.18 on the shelf to ≅O.10 at 5000 m but do not change with depth in individual cores. A model is presented which can account for the range of 240Pu /239Pu ratios found in this and other similar studies ( NOSHKIN and GATROUSIS, 1974; SCOTTet al., 1983). We propose that there have been at least two distinct sources of fallout Pu to this region. The major source of Pu is global stratospheric fallout, characterized by a 240Pu /239Pu ratio of 0.18 and a relatively long residence time in seawater. The second source is characterized by a much lower 240Pu /239Pu ratio, and relative to global fallout it must have been much more efficiently removed from the water column to deep-sea sediments. We suggest that surface-based low yield testing at the Nevada Test Site is the only source of low ratio fallout Pu which could account for the timing, inventories, and refractory characteristics of this second component of fallout Pu inputs to the North Atlantic.

  16. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  18. Partial (gamma)-Ray Cross Sections for the Reaction 239Pu(n,2n(gamma)i) and the 239Pu(n,2n) Cross Section

    SciTech Connect

    Beacker, J.A.; Bernstein, L.A.; Younes, W.; McNabb, D.P.; Garrett, P.E.; Archer, D.; McGrath, C.A.; Stoyer, M.A.; Chen, H.; Ormand, W.E.; Nelson, R.O.; Chadwick, M.B.; Johns, G.D.; Drake, D.; Young, P.G.; Devlin, M.; Fotiades, N.; Wilburn, W.S.

    2001-09-14

    Absolute partial {gamma}-ray cross sections for production of discrete {gamma} rays in the {sup 239}Pu(n,2n{gamma}i){sup 238}Pu reaction have been measured. The experiments were performed at LANSCE/WNR on the 60R flight line. Reaction {gamma}-rays were measured using the large-scale Compton-suppressed array of Ge detectors, GEANIE. The motivation for this experiment, an overview of the partial {gamma}-ray cross-section measurement, and an introduction to the main experimental issues will be presented. The energy resolution of the Ge detectors allowed identification of reaction {gamma} rays above the background of sample radioactivity and fission {gamma} rays. The use of planar Ge detectors with their reduced sensitivity to neutron interactions and improved line shape was also important to the success of this experiment. Absolute partial {gamma}-ray cross sections are presented for the 6{sub 1}{sup +} {yields} 4{sub 1}{sup +} member of the ground state rotational band in {sup 238}Pu, together with miscellaneous other {gamma}-ray partial cross sections. The n,2n reaction cross section shape and magnitude as a function of neutron energy was extracted from these partial cross sections using nuclear modeling (enhanced Hauser-Feshbach) to relate partial {gamma}-ray cross sections to the n,2n cross section. The critical nuclear modeling issue is the ratio of a partial cross section to the reaction channel cross section, and not the prediction of the absolute magnitude.

  19. 239Pu(n,2n) 238Pu cross section inferred from IDA calculations and GEANIE measurements

    SciTech Connect

    Chen, H; Ormand, W E; Dietrich, F S

    2000-09-01

    This report presents the latest {sup 239}Pu(n,2n){sup 238}Pu cross sections inferred from calculations performed with the nuclear reaction-modeling code system, IDA, coupled with experimental measurements of partial {gamma}-ray cross sections for incident neutron energies ranging from 5.68 to 17.18 MeV. It is found that the inferred {sup 239}Pu(n,2n){sup 238}Pu cross section peaks at E{sub inc} {approx} 11.4 MeV with a peak value of approximately 326 mb. At E{sub inc} {approx} 14 MeV, the inferred {sup 239}Pu(n,2n){sup 238}Pu cross section is found to be in good agreement with previous radio-chemical measurements by Lockheed. However, the shape of the inferred {sup 239}Pu(n,2n){sup 238}Pu cross section differs significantly from previous evaluations of ENDL, ENDF/B-V and ENDF/B-VI. In our calculations, direct, preequilibrium, and compound reactions are included. Also considered in the modeling are fission and {gamma}-cascade processes in addition to particle emission. The main components of physics adopted and the parameters used in our calculations are discussed. Good agreement of the inferred {sup 239}Pu(n,2n){sup 238}Pu cross sections derived separately from IDA and GNASH calculations is shown. The two inferences provide an estimate of variations in the deduced {sup 239}Pu(n,2n){sup 238}Pu cross section originating from modeling.

  20. Exposure of F344 rats to aerosols of {sup 239}PuO{sub 2} and chronically inhaled cigarette smoke

    SciTech Connect

    Finch, G.L.; Nikula, K.J.; Barr, E.B.; Bechtold, W.E.; Chen, B.T.; Griffith, W.C.; Hobbs, C.H.; Hoover, M.D.; Mauderly, J.L.

    1994-11-01

    Nuclear workers may be accidently exposed to radioactive materials such as {sup 239}PuO{sub 2} by inhalation, and thus have increased risk for lung cancer compared to the general population. Of additional concern is the possibility that interactions between radionuclides and other carcinogens may increase the risk of cancer induction. An important and common lung carcinogen is cigarette smoke. This study is being conducted to better determine the combined effects of inhaled {sup 239}PuO{sub 2} and cigarette smoke on the induction of lung cancer in rats.

  1. Neutron capture and (n,2n) measurements on 241Am

    SciTech Connect

    Vieira, D; Jandel, M; Bredeweg, T; Bond, E; Clement, R; Couture, A; Haight, R; O'Donnell, J; Reifarth, R; Ullmann, J; Wilhelmy, J; Wouters, J; Tonchev, A; Hutcheson, A; Angell, C; Crowell, A; Fallin, B; Hammond, S; Howell, C; Karowowski, H; Kelley, J; Pedroni, R; Tornow, W; Macri, R; Agvaanluvsan, U; Becker, J; Dashdorj, D; Stoyer, M; Wu, C

    2007-07-18

    We report on a set of neutron-induced reaction measurements on {sup 241}Am which are important for nuclear forensics and advanced nuclear reactor design. Neutron capture measurements have been performed on the DANCE detector array at the Los Alamos Neutron Scattering CEnter (LANSCE). In general, good agreement is found with the most recent data evaluations up to an incident neutron energy of {approx} 300 keV where background limits the measurement. Using mono-energetic neutrons produced in the {sup 2}H(d,n){sup 3}He reaction at Triangle University Nuclear Laboratory (TUNL), we have measured the {sup 241}Am(n,2n) excitation function from threshold (6.7 MeV) to 14.5 MeV using the activation method. Good agreement is found with previous measurements, with the exception of the three data points reported by Perdikakis et al. around 11 MeV, where we obtain a much lower cross section that is more consistent with theoretical estimates.

  2. Performance of Cladding on MOX Fuel with Low 240Pu/239Pu Ratio

    SciTech Connect

    McCoy, Kevin; Blanpain, Patrick; Morris, Robert Noel

    2014-01-01

    The U.S. Department of Energy has decided to dispose of a portion of its surplus plutonium by reconstituting it into mixed oxide (MOX) fuel and irradiating it in commercial power reactors. As part of fuel qualification, four lead assemblies were manufactured and irradiated to a maximum fuel rod average burnup of 47.3 MWd/kg heavy metal. This was the world s first commercial irradiation of MOX fuel with a 240Pu/239Pu ratio less than 0.10. Five fuel rods with varying burnups and plutonium contents were selected from one of the assemblies and shipped to Oak Ridge National Laboratory for hot cell examination. This paper discusses the results of those examinations with emphasis on cladding performance. Exams relevant to the cladding included visual and eddy current exams, profilometry, microscopy, hydrogen analysis, gallium analysis, and mechanical testing. There was no discernible effect of the type of MOX fuel on the performance of the cladding.

  3. Calculation of 239Pu fission observables in an event-by-event simulation

    SciTech Connect

    Vogt, R; Randrup, J; Pruet, J; Younes, W

    2010-03-31

    The increased interest in more exclusive fission observables has demanded more detailed models. We describe a new computational model, FREYA, that aims to meet this need by producing large samples of complete fission events from which any observable of interest can then be extracted consistently, including any interesting correlations. The various model assumptions are described and the potential utility of the model is illustrated. As a concrete example, we use formal statistical methods, experimental data on neutron production in neutron-induced fission of {sup 239}Pu, along with FREYA, to develop quantitative insights into the relation between reaction observables and detailed microscopic aspects of fission. Current measurements of the mean number of prompt neutrons emitted in fission taken together with less accurate current measurements for the prompt post-fission neutron energy spectrum, up to the threshold for multi-chance fission, place remarkably fine constraints on microscopic theories.

  4. Evaluation of. nu. -bar/sub rho/ for /sup 239/Pu

    SciTech Connect

    Fort, E. ); Frehaut, J. ); Tellier, H. ); Long, P. )

    1988-08-01

    The average number of prompt neutrons ..nu..-bar/sub rho/ emitted per fission event has been evaluated for /sup 239/Pu with a special emphasis on the fluctuations experimentally observed in the low-energy range. These fluctuations have a significant impact on applications, especially the reactivity coefficient of advanced water reactors. Consequently, the ..nu..-bar/sub rho/ curve has to be defined in the same fine energy mesh as the fission cross section for accurate neutron source calculations. In this range, formalisms are proposed to calculate ..nu..-bar/sub rho/ from the resonance parameters, resolved or averaged. Using the JEF-1 library as a data base, an analysis of several thermal, low-moderated, or fast systems shows a good convergence of the selected microscopic and integral information.

  5. Carcinogenic responses of transgenic heterozygous p53 knockout mice to inhaled 239PuO2 or metallic beryllium.

    PubMed

    Finch, G L; March, T H; Hahn, F F; Barr, E B; Belinsky, S A; Hoover, M D; Lechner, J F; Nikula, K J; Hobbs, C H

    1998-01-01

    The transgenic heterozygous p53+/- knockout mouse has been a model for assessing the tumorigenicity of selected carcinogens administered by noninhalation routes of exposure. The sensitivity of the model for predicting cancer by inhaled chemicals has not been examined. This study addresses this issue by acutely exposing p53+/- mice of both sexes by nose-only inhalation to either air (controls), or to 1 of 2 levels of 239PuO2 (500 or 100 Bq 239Pu) or beryllium (Be) metal (60 or 15 micrograms). Additional wild-type p53+/+ mice were exposed by inhalation to either 500 Bq of 239PuO2 or 60 micrograms of Be metal. These carcinogens were selected because they operate by differing mechanisms and because of their use in other pulmonary carcinogenesis studies in our laboratory. Four or 5 of the 15 mice per sex from each group were sacrificed 6 mo after exposure, and only 2 pulmonary neoplasms were observed. The remainder of the mice were held for life-span observation and euthanasia as they became moribund. Survival of the p53+/- knockout mice was reduced compared to the p53+/+ wild-type mice. No lung neoplasms were observed in p53+/- mice exposed to air alone. Eleven of the p53+/- mice inhaling 239PuO2 developed pulmonary neoplasms. Seven p53+/+ mice exposed to 239PuO2 also developed pulmonary neoplasms, but the latency period for pulmonary neoplasia was significantly shorter in the p53+/ mice. Four pulmonary neoplasms were observed in p53+/- mice exposed to the higher dose of Be, whereas none were observed in the wild-type mice or in the heterozygous mice exposed to the lower dose of Be. Thus, both p53+/- and p53+/+ mice were susceptible to 239Pu-induced carcinogenesis, whereas the p53+/- but not the p53+/+ mice were susceptible to Be-induced carcinogenesis. However, only 2 pulmonary neoplasms (1 in each of the 239PuO2 exposure groups) were observed in the 59 p53+/ mice that were sacrificed or euthanatized within 9 mo after exposure, indicating that the p53+/- knockout

  6. 239Pu Prompt Fission Neutron Spectra Impact on a Set of Criticality and Experimental Reactor Benchmarks

    NASA Astrophysics Data System (ADS)

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

    2014-04-01

    A large set of nuclear data are investigated to improve the calculation predictions of the new neutron transport simulation codes. With the next generation of nuclear power plants (GEN IV projects), one expects to reduce the calculated uncertainties which are mainly coming from nuclear data and are still very important, before taking into account integral information in the adjustment process. In France, future nuclear power plant concepts will probably use MOX fuel, either in Sodium Fast Reactors or in Gas Cooled Fast Reactors. Consequently, the knowledge of 239Pu cross sections and other nuclear data is crucial issue in order to reduce these sources of uncertainty. The Prompt Fission Neutron Spectra (PFNS) for 239Pu are part of these relevant data (an IAEA working group is even dedicated to PFNS) and the work presented here deals with this particular topic. The main international data files (i.e. JEFF-3.1.1, ENDF/B-VII.0, JENDL-4.0, BRC-2009) have been considered and compared with two different spectra, coming from the works of Maslov and Kornilov respectively. The spectra are first compared by calculating their mathematical moments in order to characterize them. Then, a reference calculation using the whole JEFF-3.1.1 evaluation file is performed and compared with another calculation performed with a new evaluation file, in which the data block containing the fission spectra (MF=5, MT=18) is replaced by the investigated spectra (one for each evaluation). A set of benchmarks is used to analyze the effects of PFNS, covering criticality cases and mock-up cases in various neutron flux spectra (thermal, intermediate, and fast flux spectra). Data coming from many ICSBEP experiments are used (PU-SOL-THERM, PU-MET-FAST, PU-MET-INTER and PU-MET-MIXED) and French mock-up experiments are also investigated (EOLE for thermal neutron flux spectrum and MASURCA for fast neutron flux spectrum). This study shows that many experiments and neutron parameters are very sensitive to

  7. Isotopic yield measurement in the heavy mass region for {sup 239}Pu thermal neutron induced fission

    SciTech Connect

    Bail, A.; Serot, O.; Mathieu, L.; Litaize, O.; Materna, T.; Koester, U.; Faust, H.; Letourneau, A.; Panebianco, S.

    2011-09-15

    Despite the huge number of fission yield data available in the different evaluated nuclear data libraries, such as JEFF-3.1.1, ENDF/B-VII.0, and JENDL-4.0, more accurate data are still needed both for nuclear energy applications and for our understanding of the fission process itself. It is within the framework of this that measurements on the recoil mass spectrometer Lohengrin (at the Institut Laue-Langevin, Grenoble, France) was undertaken, to determine isotopic yields for the heavy fission products from the {sup 239}Pu(n{sub th},f) reaction. In order to do this, a new experimental method based on {gamma}-ray spectrometry was developed and validated by comparing our results with those performed in the light mass region with completely different setups. Hence, about 65 fission product yields were measured with an uncertainty that has been reduced on average by a factor of 2 compared to that previously available in the nuclear data libraries. In addition, for some fission products, a strongly deformed ionic charge distribution compared to a normal Gaussian shape was found, which was interpreted as being caused by the presence of a nanosecond isomeric state. Finally, a nuclear charge polarization has been observed in agreement, with the one described on other close fissioning systems.

  8. Photofission product yields of 238U and 239Pu with 22-MeV bremsstrahlung

    NASA Astrophysics Data System (ADS)

    Wen, Xianfei; Yang, Haori

    2016-06-01

    In homeland security and nuclear safeguards applications, non-destructive techniques to identify and quantify special nuclear materials are in great demand. Although nuclear materials naturally emit characteristic radiation (e.g. neutrons, γ-rays), their intensity and energy are normally low. Furthermore, such radiation could be intentionally shielded with ease or buried in high-level background. Active interrogation techniques based on photofission have been identified as effective assay approaches to address this issue. In designing such assay systems, nuclear data, like photofission product yields, plays a crucial role. Although fission yields for neutron-induced reactions have been well studied and readily available in various nuclear databases, data on photofission product yields is rather scarce. This poses a great challenge to the application of photofission techniques. In this work, short-lived high-energy delayed γ-rays from photofission of 238U were measured in between linac pulses. In addition, a list-mode system was developed to measure relatively long-lived delayed γ-rays from photofission of 238U and 239Pu after the irradiation. Time and energy information of each γ-ray event were simultaneously recorded by this system. Cumulative photofission product yields were then determined using the measured delayed γ-ray spectra.

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

    NASA Astrophysics Data System (ADS)

    Reed, B. Cameron

    2017-01-01

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

  10. Probing energy dissipation, γ-ray and neutron multiplicity in the thermal neutron-induced fission of 239Pu

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    The incorporation of the four-dimensional Langevin equations led to an integrative description of fission cross-section, fragment mass distribution and the multiplicity and energy distribution of prompt neutrons and γ-rays in the thermal neutron-induced fission of 239Pu. The dynamical approach presented in this paper thoroughly reproduces several experimental observables of the fission process at low excitation energy.

  11. Study of neutron-deficient isotopes of Fl in the 239Pu, 240Pu + 48Ca reactions

    NASA Astrophysics Data System (ADS)

    Voinov, A. A.; Utyonkov, V. K.; Brewer, N. T.; Oganessian, Yu Ts; Rykaczewski, K. P.; Abdullin, F. Sh; Dmitriev, S. N.; Grzywacz, R. K.; Itkis, M. G.; Miernik, K.; Polyakov, A. N.; Roberto, J. B.; Sagaidak, R. N.; Shirokovsky, I. V.; Shumeiko, M. V.; Tsyganov, Yu S.; Subbotin, V. G.; Sukhov, A. M.; Sabelnikov, A. V.; Vostokin, G. K.; Hamilton, J. H.; Stoyer, M. A.; Strauss, S. Y.

    2016-07-01

    The results of the experiments aimed at the synthesis of Fl isotopes in the 239Pu + 48Ca and 240Pu + 48Ca reactions are presented. The experiment was performed using the Dubna gas-filled recoil separator at the U400 cyclotron. In the 239Pu+48Ca experiment one decay of spontaneously fissioning 284Fl was detected at 245-MeV beam energy. In the 240Pu+48Ca experiment three decay chains of 285Fl were detected at 245 MeV and four decays were assigned to 284Fl at the higher 48Ca beam energy of 250 MeV. The α-decay energy of 285Fl was measured for the first time and decay properties of its descendants 281Cn, 277Ds, 273Hs, 269Sg, and 265Rf were determined more precisely. The cross section of the 239Pu(48Ca,3n)284Fl reaction was observed to be about 20 times lower than those predicted by theoretical models and 50 times less than the value measured in the 244Pu+48Ca reaction. The cross sections of the 240Pu(48Ca,4-3n)284,285Fl at both 48Ca energies are similar and exceed that observed in the reaction with lighter isotope 239Pu by a factor of 10. The decay properties of the synthesized nuclei and their production cross sections indicate rapid decrease of stability of superheavy nuclei with departing from the neutron number N=184 predicted to be the next magic number.

  12. Neutron capture cross section of {sup 241}Am

    SciTech Connect

    Jandel, M.; Bredeweg, T. A.; Bond, E. M.; Chadwick, M. B.; Clement, R. R.; Couture, A.; O'Donnell, J. M.; Haight, R. C.; Kawano, T.; Reifarth, R.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wouters, J. M.; Agvaanluvsan, U.; Parker, W. E.; Wu, C. Y.; Becker, J. A.

    2008-09-15

    The neutron capture cross section of {sup 241}Am for incident neutrons from 0.02 eV to 320 keV has been measured with the detector for advanced neutron capture experiments (DANCE) at the Los Alamos Neutron Science Center. The thermal neutron capture cross section was determined to be 665{+-}33 b. Our result is in good agreement with other recent measurements. Resonance parameters for E{sub n}<12 eV were obtained using an R-matrix fit to the measured cross section. The results are compared with values from the ENDF/B-VII.0, Mughabghab, JENDL-3.3, and JEFF-3.1 evaluations. {gamma}{sub n} neutron widths for the first three resonances are systematically larger by 5-15% than the ENDF/B-VII.0 values. The resonance integral above 0.5 eV was determined to be 1553{+-}7 b. Cross sections in the resolved and unresolved energy regions above 12 eV were calculated using the Hauser-Feshbach theory incorporating the width-fluctuation correction of Moldauer. The calculated results agree well with the measured data, and the extracted averaged resonance parameters in the unresolved resonance region are consistent with those for the resolved resonances.

  13. Use of fission track analysis technique for the determination of MicroBequerel level of 239Pu in urine samples from radiation workers handling MOX fuel.

    PubMed

    Yadav, J R; Rao, D D; Kumar, Ranjeet; Aggarwal, S K

    2011-07-01

    Fission track analysis (FTA) technique for the determination of (239)Pu excreted through urine has been standardized using blank samples, tracer and (239)Pu spikes. Double stage anion exchange separation protocol has been applied and an average radiochemical recovery of (239)Pu of 18% was obtained. An average track registration efficiency of 11 tracks per μBq of (239)Pu, irradiated to 0.35×10(17) neutron fluence was established. Reagent blank urine samples from 11 controlled subjects were analyzed by FTA and an average of 149±14 tracks was obtained. Minimum detectable activity of 34μBqL(-1) of urine sample was obtained and will be useful for monitoring chronic exposure cases handling MOX fuel.

  14. Brazilian gamma-neutron dosemeter: response to 241AmBe and 252Cf neutron sources.

    PubMed

    Souto, E B; Campos, L L

    2011-03-01

    With the aim of improving the monitoring of workers potentially exposed to neutron radiation in Brazil, the IPEN/CNEN-SP in association with PRO-RAD designed and developed a passive individual gamma-neutron mixed-field dosemeter calibrated to be used to (241)AmBe sources. To verify the dosimetry system response to different neutron spectra, prototypes were irradiated with a (252)Cf source and evaluated using the dose-calculation algorithm developed for (241)AmBe sources.

  15. Placental transfer and distribution of /sup 241/Am in the rat

    SciTech Connect

    Hisamatsu, S.; Takizawa, Y.

    1983-04-01

    The placental transfer and distribution of /sup 241/Am in the feto-placental system were studied in pregnant rats. Rats were injected intravenously with /sup 241/Am citrate at 15 or 18 days of gestation. Groups injected at 15 days of gestation were sacrificed 2, 24, 48, or 120 hr after injection, and the group injected at 18 days was sacrificed 24 hr after. The radioactivities of /sup 241/Am in fetus, fetal membrane, and placenta were determined, and its distribution in the feto-placental system was investigated by high-speed autoradiography using a silver-activated zinc sulfide-coated membrane as an intensifying screen. The deposition of /sup 241/Am in feto-placenta units increased with the number of days of gestation. Results of autoradiography revealed that major deposition sites of /sup 241/Am in the fetus are the skeleton and liver. Heavy deposition of /sup 241/Am in the yolksac splanchnopleure and its existence in the exocoelom strongly suggest that the yolk sac placenta plays an important role in the placental transfer of this nuclide.

  16. Determination of Plutonium Activity Concentrations and 240Pu/239Pu Atom Ratios in Brown Algae (Fucus distichus) Collected from Amchitka Island, Alaska.

    SciTech Connect

    Hamilton, T F; Brown, T A; Marchetti, A A; Martinelli, R E; Kehl, S R

    2005-05-02

    Plutonium-239 ({sup 239}Pu) and plutonium-240 ({sup 240}Pu) activity concentrations and {sup 240}Pu/{sup 239}Pu atom ratios are reported for Brown Algae (Fucus distichus) collected from the littoral zone of Amchitka Island (Alaska) and at a control site on the Alaskan peninsula. Plutonium isotope measurements were performed in replicate using Accelerator Mass Spectrometry (AMS). The average {sup 240}Pu/{sup 239}Pu atom ratio observed in dried Fucus d. collected from Amchitka Island was 0.227 {+-} 0.007 (n=5) and compares with the expected {sup 240}Pu/{sup 239}Pu atom ratio in integrated worldwide fallout deposition in the Northern Hemisphere of 0.1805 {+-} 0.0057 (Cooper et al., 2000). In general, the characteristically high {sup 240}Pu/{sup 239}Pu content of Fucus d. analyzed in this study appear to indicate the presence of a discernible basin-wide secondary source of plutonium entering the marine environment. Of interest to the study of plutonium source terms within the Pacific basin are reports of elevated {sup 240}Pu/{sup 239}Pu atom ratios in fallout debris from high-yield atmospheric nuclear tests conducted in the Marshall Islands during the 1950s (Diamond et al., 1960), the wide range of {sup 240}Pu/{sup 239}Pu atom ratio values (0.19 to 0.34) observed in sea water, sediments, coral and other environmental media from the North Pacific Ocean (Hirose et al., 1992; Buesseler, 1997) and updated estimates of the relative contributions of close-in and intermediate fallout deposition on oceanic inventories of radionuclidies, especially in the Northern Pacific Ocean (Hamilton, 2004).

  17. Reactor Decay Heat in {sup 239}Pu: Solving the {gamma} Discrepancy in the 4-3000-s Cooling Period

    SciTech Connect

    Algora, A.; Jordan, D.; Tain, J. L.; Rubio, B.; Agramunt, J.; Perez-Cerdan, A. B.; Molina, F.; Caballero, L.; Nacher, E.; Krasznahorkay, A.; Hunyadi, M. D.; Gulyas, J.; Vitez, A.; Csatlos, M.; Csige, L.; Aeysto, J.; Penttilae, H.; Moore, I. D.; Eronen, T.; Jokinen, A.

    2010-11-12

    The {beta} feeding probability of {sup 102,104,105,106,107}Tc, {sup 105}Mo, and {sup 101}Nb nuclei, which are important contributors to the decay heat in nuclear reactors, has been measured using the total absorption technique. We have coupled for the first time a total absorption spectrometer to a Penning trap in order to obtain sources of very high isobaric purity. Our results solve a significant part of a long-standing discrepancy in the {gamma} component of the decay heat for {sup 239}Pu in the 4-3000 s range.

  18. 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.

  19. Time-dependent local and average structural evolution of δ-phase 239Pu-Ga alloys

    DOE PAGES

    Smith, Alice I.; Page, Katharine L.; Siewenie, Joan E.; ...

    2016-08-05

    Here, plutonium metal is a very unusual element, exhibiting six allotropes at ambient pressure, between room temperature and its melting point, a complicated phase diagram, and a complex electronic structure. Many phases of plutonium metal are unstable with changes in temperature, pressure, chemical additions, or time. This strongly affects structure and properties, and becomes of high importance, particularly when considering effects on structural integrity over long periods of time [1]. This paper presents a time-dependent neutron total scattering study of the local and average structure of naturally aging δ-phase239Pu-Ga alloys, together with preliminary results on neutron tomography characterization.

  20. Reactor decay heat in 239Pu: solving the γ discrepancy in the 4-3000-s cooling period.

    PubMed

    Algora, A; Jordan, D; Taín, J L; Rubio, B; Agramunt, J; Perez-Cerdan, A B; Molina, F; Caballero, L; Nácher, E; Krasznahorkay, A; Hunyadi, M D; Gulyás, J; Vitéz, A; Csatlós, M; Csige, L; Aysto, J; Penttilä, H; Moore, I D; Eronen, T; Jokinen, A; Nieminen, A; Hakala, J; Karvonen, P; Kankainen, A; Saastamoinen, A; Rissanen, J; Kessler, T; Weber, C; Ronkainen, J; Rahaman, S; Elomaa, V; Rinta-Antila, S; Hager, U; Sonoda, T; Burkard, K; Hüller, W; Batist, L; Gelletly, W; Nichols, A L; Yoshida, T; Sonzogni, A A; Peräjärvi, K

    2010-11-12

    The β feeding probability of (102,104,105,106,107)Tc, 105Mo, and 101Nb nuclei, which are important contributors to the decay heat in nuclear reactors, has been measured using the total absorption technique. We have coupled for the first time a total absorption spectrometer to a Penning trap in order to obtain sources of very high isobaric purity. Our results solve a significant part of a long-standing discrepancy in the γ component of the decay heat for 239Pu in the 4-3000 s range.

  1. Reactor Decay Heat in 239Pu: Solving the Gamma Discrepancy in the 4–3000-s Cooling Period

    SciTech Connect

    Algora, A.; Sonzogni, A.; Algora,A.; Jordan,D.; Tain,J.L.; Rubio,B.; Agramunt,J.; Perez-Cerdan,A.B.; Molina,F; Caballero,L.; Nacher,E.; Krasznahorkay,A.; Hunyadi,M.D.; Gulyas,J; Vitez,A.; Csatlos,M.; Csige,L.; Aysto,J.; Penttila,H.; Moore,I.D.; Eronen,T.; Jokinen,A.; Nieminen,A.; Hakala,J.; Karvonen,P.; Kankainen,A.; Saastamoinen,A.; Rissanen,J.; Kessler,T.; Weber,C.; Ronkainen,J.; Rahaman,S.; Elomaa,V.; Rinta-Antila,S.; Hager,U.; Sonoda,T.; Burkard,K.; Huller,W.; Batist,L.; Gelletly,W.; Nichols,A.L.; Yoshida,T.; Sonzogni,A.A.; Perajarvi,K.

    2010-11-08

    The {beta} feeding probability of {sup 102,104,105,106,107}Tc, {sup 105}Mo, and {sup 101}Nb nuclei, which are important contributors to the decay heat in nuclear reactors, has been measured using the total absorption technique. We have coupled for the first time a total absorption spectrometer to a Penning trap in order to obtain sources of very high isobaric purity. Our results solve a significant part of a long-standing discrepancy in the {gamma} component of the decay heat for {sup 239}Pu in the 4-3000 s range.

  2. High-precision study of time- and temperature-dependence of the elastic properties of 239Pu

    NASA Astrophysics Data System (ADS)

    Maiorov, B.; Ramshaw, B. J.; Shekhter, A.; Betts, J. B.; Freibert, F.; Migliori, A.

    2015-03-01

    It is important to determine the origin of changes in elastic properties in 239Pu as a function of time. The measurement of mechanical resonance frequencies can be made with extreme precision and used to compute the elastic moduli without corrections giving important insight in this problem. The precision of these measurements enabled observation of changes in elastic properties of 1 part in 107 for measurements lasting hours up to several days. The most-likely source of these changes include a) ingrowth of radioactive decay products such as He and U, b) the introduction of radiation damage, c) phase instabilities associated with transformations to the delta phase or to Pu3Ga. Using Resonant Ultrasound Spectroscopy, measurements were made of the mechanical resonance frequencies of 300mg cylinders of fine-grained polycrystalline alpha-phase 239Pu with about 600PPM Ga. We present the surprising result that at temperatures below 60K, there is a strong dependence on temperature of the rate of change of elastic moduli with time. Older results showed that the sign of this rate of change reverses at higher temperature. Such studies of nascent state are key to exploring damage evolution and its impact on specific volume and elastic moduli. Future studies will continue these measurements to above ambient temperatures.

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

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  4. Comparison of early mortality in baboons and dogs after inhalation of /sup 239/PuO/sub 2/

    SciTech Connect

    Bair, W.J.; Metivier, H.; Park, J.F.; Masse, R.; Stevens, D.L.; Lafuma, J.; Watson, C.R.; Nolibe, D.

    1980-06-01

    Results from experiments with baboons were compared with those from experiments with dogs to determine the relative sensitivity of the two species to early mortality from inhaled /sup 239/PuO/sub 2/. To ensure a valid comparison of data developed at two laboratories, methodology differences were minimized by establishing a common pool of raw data, using the same computer programs to analyze the data, and standardizing assumptions regarding the calculation of plutonium concentration in lungs. Several comparison methods were used involving variations in estimating different parameters used in these calculations. Although nearly all comparisons suggested baboons were slightly more sensitive, none of the methods for comparing the relationship between dose and survival time showed consistently significant differences between baboons and dogs. Although the baboons were physiologically and morphologically immature when exposed to plutonium, whereas the dogs were mature, we concluded that adult baboons and dogs are similarly sensitive to the early effects of inhaled /sup 239/PuO/sub 2/. Since only early mortality was considered in this comparison, the results do not apply to possible late effects caused by much lower levels of plutonium than were used in these experiments.

  5. Measurement of 239Pu in urine samples at ultra-trace levels using a 1 MV compact AMS system

    NASA Astrophysics Data System (ADS)

    Hernández-Mendoza, H.; Chamizo, E.; Yllera, A.; García-León, M.; Delgado, A.

    2010-04-01

    Routine bioassay monitoring of Pu intake in exposed workers of research and nuclear industry is usually performed by alpha spectrometry. This technique involves large sample volumes of urine and time-consuming preparative and counting protocols. Compact accelerator mass spectrometry (AMS) facilities make feasible the determination of ultra low-level Pu activity concentrations and Pu isotopic ratios in biological samples (blood, urine and feces), being a rapid and cost-effective measurement technique. The plutonium results in urine samples presented here have been obtained on the 1 MV compact AMS system sited at the Centro Nacional de Aceleradores (CNA), in Seville, Spain. In this work, a different methodological approach has been developed alternative to the "classical" preparation of urine samples for alpha spectrometry. The procedure avoids the Pu precipitation step, and involves acid sample evaporation and acid digestion in a microwave oven. Finally, purification of plutonium was achieved by using chromatography columns filled up with BioRad AG1X2 anion exchange resin (Bio-Rad Laboratories Inc.). The total time needed for analysis is about 10 h, unlike the "classical" methods based on alpha spectrometry which need about 1 week. At present, it has been demonstrated that this method allows quantifying 239Pu activity concentrations in urine of, at least, 30 μBq (13 fg 239Pu). We can conclude that the procedure would be suitable to perform in vitro routine bioassay measurements. Moreover, the innovative application of AMS opens new and interesting analytical alternatives in this field.

  6. Pulmonary retention and tissue distribution of {sup 239}Pu nitrate in F344 rats and syrian hamsters inhaling carbon tetrachloride

    SciTech Connect

    Benson, J.M.; Barr, E.B.; Lundgren, D.L.; Nikula, K.J.

    1994-11-01

    Carbon tetrachloride (CCl{sub 4}) has been used extensively in the nuclear weapons industry, so it is possible that nuclear plant workers have been exposed to CCl{sub 4} and plutonium compounds. Potential for future exposure exists during {open_quotes}cleanup{close_quotes} operations at weapon production sites such as the Hanford, Washington, and Rocky Flats, Colorado, facilities. The current Threshold Limit Value for CCl{sub 4} is 5 ppm; however, concentrations of CCl{sub 4} occurring in the nuclear weapons facilities over the past 40-50 y are unknown and may have exceeded this value. The pilot study described in this report is designed to determine whether subchronic inhalation of CCl{sub 4} by CDF{sup register}(F-344)/CrlBR rats and Syrian golden hamsters, at concentrations expected to produce some histologic changes in liver, alters the hepatic retention and toxic effects of inhaled {sup 239}Pu nitrate {sup 239}Pu(NO{sub 3}){sub 4}.

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

    DOE PAGES

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

    2016-06-23

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

  8. 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.

  9. Case Study: Three Acute 241Am Inhalation Exposures with DTPA Therapy

    SciTech Connect

    Carbaugh, Eugene H.; Lynch, Timothy P.; Cannon, Curt; Lewis, Loren L.

    2010-10-01

    Three workers incurred inhalation exposures to 241Am oxide as a result of waste sorting and compaction activities. The magnitudes of the exposures were not fully recognized until the following day when an in vivo chest count identified a significant lung deposition of 241Am in a male worker, and DTPA chelation therapy was initiated. Two additional workers (one female and one male) were then identified as sufficiently exposed to also warrant therapy. In vivo bioassay measurements were performed over the ensuing 6 months to quantify the 241Am activity in the lungs, liver, and skeleton. Urine and fecal samples were collected and showed readily detectable 241Am. Clinical lab tests and medical evaluations all showed normal results. There were no significant adverse clinical health effects from the therapy. The estimated 241Am inhalation intakes for the three workers were 1800 Bq, 630 Bq, and 150 Bq. Lung retention showed somewhat longer pulmonary clearance half-times than standard inhalation class W or absorption Type M assumptions. The three underwent slightly different therapy regimes, with therapy effectiveness factors (defined as the ratio of the reference doses without therapy relative to the final assessed doses) of 4.65, 1.93, and 1.67, respectively.

  10. Progress on 241Am Production for Use in Radioisotope Power Systems

    NASA Astrophysics Data System (ADS)

    Baker, S. R.; Bell, K. J.; Brown, J.; Carrigan, C.; Carrott, M. J.; Gregson, C.; Clough, M.; Maher, C. J.; Mason, C.; Rhodes, C. J.; Rice, T. G.; Sarsfield, M. J.; Stephenson, K.; Taylor, R. J.; Tinsley, T. P.; Woodhead, D. A.; Wiss, T.

    2014-08-01

    Electrical power sources used in outer planet missions are a key enabling technology for data acquisition and communications. Power sources generate electricity from the thermal energy from alpha decay of the radioisotope 238Pu via thermo-electric conversion. Production of 238Pu requires specialist facilities including a nuclear reactor and reprocessing plants that are expensive to build and operate, so naturally, a more economical alternative is attractive to the industry. Within Europe 241Am is a feasible alternative to 238Pu that can provide a heat source for radioisotope thermoelectric generators (RTGs) and radioisotope heating units (RHUs). As a daughter product of 241Pu decay, 241Am is present at 1000s kg levels within the UK civil plutonium stockpile.A chemical separation process is required to extract the 241Am in a pure form and this paper describes such a process, successfully developed to the proof of concept stage.

  11. Accumulation of (241)Am by suspended matter, diatoms and aquatic weeds of the Yenisei River.

    PubMed

    Zotina, T A; Bolsunovsky, A Ya; Bondareva, L G

    2010-02-01

    In this work we experimentally estimated the capacities of the key components of the Yenisei River (Russia): particulate suspended matter (seston), diatom microalgae, and submerged macrophytes for accumulating (241)Am from water. In our experiments large particles of seston (>8mum), comparable in size with diatoms, took up most of americium from water. The accumulation of americium by isolated diatom algae (Asterionella formosa and Diatoma vulgare) was lower than by total seston. The concentration factors (CFs) of (241)Am for seston of the Yenisei River in our experiments were (2.8-6.9).10(5); for diatoms - (1.5-4.2).10(4). The CFs for aquatic plant Elodea canadensis were within the same order of magnitude as those for diatoms. Activity concentration and CFs of (241)Am were nearly the same in experiments under dark and light conditions. This is indicative of an energy independent mechanism of americium uptake from the water by diatoms and submerged macrophytes.

  12. Study on migration behaviour of 237Np and 241Am in near-surface environments.

    PubMed

    Tanaka, Tadao; Ya-Anant, Nanthavan

    2011-07-01

    Laboratory-scale experiments were performed to investigate migration behaviour of (237)Np and (241)Am, which were deposited onto the ground surface from spent fuel reprocessing facilities. Migration experiments by column method were conducted for a sandy soil and a reddish soil by varying the volume of eluting solution. There seemed to be two chemical species of (237)Np in the sandy soil column: one is cationic and the other is particulate form. The particulates moved without significant interaction with the sandy soil. The sorption of cationic (237)Np was controlled by both a reversible ion-exchange reaction and irreversible reactions. Most of (241)Am was formed into rather large particulates and trapped in the sandy soil column. The (237)Np and (241)Am loaded into the reddish soil column moved deeper with increasing eluting volume. The sorption was mainly controlled by ion-exchange reaction. The migration behaviour might be evaluated by the distribution coefficient.

  13. Biological effects of α-radiation exposure by (241)Am in Arabidopsis thaliana seedlings are determined both by dose rate and (241)Am distribution.

    PubMed

    Biermans, Geert; Horemans, Nele; Vanhoudt, Nathalie; Vandenhove, Hildegarde; Saenen, Eline; Van Hees, May; Wannijn, Jean; Vangronsveld, Jaco; Cuypers, Ann

    2015-11-01

    Human activity has led to an increasing amount of radionuclides in the environment and subsequently to an increased risk of exposure of the biosphere to ionising radiation. Due to their high linear energy transfer, α-emitters form a threat to biota when absorbed or integrated in living tissue. Among these, (241)Am is of major concern due to high affinity for organic matter and high specific activity. This study examines the dose-dependent biological effects of α-radiation delivered by (241)Am at the morphological, physiological and molecular level in 14-day old seedlings of Arabidopsis thaliana after hydroponic exposure for 4 or 7 days. Our results show that (241)Am has high transfer to the roots but low translocation to the shoots. In the roots, we observed a transcriptional response of reactive oxygen species scavenging and DNA repair pathways. At the physiological and morphological level this resulted in a response which evolved from redox balance control and stable biomass at low dose rates to growth reduction, reduced transfer and redox balance decline at higher dose rates. This situation was also reflected in the shoots where, despite the absence of a transcriptional response, the control of photosynthesis performance and redox balance declined with increasing dose rate. The data further suggest that the effects in both organs were initiated in the roots, where the highest dose rates occurred, ultimately affecting photosynthesis performance and carbon assimilation. Though further detailed study of nutrient balance and (241)Am localisation is necessary, it is clear that radionuclide uptake and distribution is a major parameter in the global exposure effects on plant performance and health.

  14. First measurements of (236)U concentrations and (236)U/(239)Pu isotopic ratios in a Southern Hemisphere soil far from nuclear test or reactor sites.

    PubMed

    Srncik, M; Tims, S G; De Cesare, M; Fifield, L K

    2014-06-01

    The variation of the (236)U and (239)Pu concentrations as a function of depth has been studied in a soil profile at a site in the Southern Hemisphere well removed from nuclear weapon test sites. Total inventories of (236)U and (239)Pu as well as the (236)U/(239)Pu isotopic ratio were derived. For this investigation a soil core from an undisturbed forest area in the Herbert River catchment (17°30' - 19°S) which is located in north-eastern Queensland (Australia) was chosen. The chemical separation of U and Pu was carried out with a double column which has the advantage of the extraction of both elements from a relatively large soil sample (∼20 g) within a day. The samples were measured by Accelerator Mass Spectrometry using the 14UD pelletron accelerator at the Australian National University. The highest atom concentrations of both (236)U and (239)Pu were found at a depth of 2-3 cm. The (236)U/(239)Pu isotopic ratio in fallout at this site, as deduced from the ratio of the (236)U and (239)Pu inventories, is 0.085 ± 0.003 which is clearly lower than the Northern Hemisphere value of ∼0.2. The (236)U inventory of (8.4 ± 0.3) × 10(11) at/m(2) was more than an order of magnitude lower than values reported for the Northern Hemisphere. The (239)Pu activity concentrations are in excellent agreement with a previous study and the (239+240)Pu inventory was (13.85 ± 0.29) Bq/m(2). The weighted mean (240)Pu/(239)Pu isotopic ratio of 0.142 ± 0.005 is slightly lower than the value for global fallout, but our results are consistent with the average ratio of 0.173 ± 0.027 for the southern equatorial region (0-30°S).

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

    SciTech Connect

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

    1982-06-10

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

  16. Accelerator Mass Spectrometric (AMS) Measurements of Plutonium Activity Concentrations and 240Pu/239Pu Atom Ratios In Soil Extracts Supplied by the Carlsbad Environmental Monitoring & Research Center

    SciTech Connect

    Hamilton, T F; Brown, T A; Marchetti, A A; Martinelli, R E; Kehl, S R

    2005-02-28

    Plutonium-239 ({sup 239}Pu) and plutonium-239+240 ({sup 239+240}Pu) activities concentrations and {sup 240}Pu/{sup 239}Pu atom ratios are reported for a series of chemically purified soil extracts received from the Carlsbad Environmental Monitoring & Research Center (CEMRC) in New Mexico. Samples were analyzed without further purification at the Lawrence Livermore National Laboratory (LLNL) using accelerator mass spectrometry (AMS). This report also includes a brief description of the AMS system and internal laboratory procedures used to ensure the quality and reliability of the measurement data.

  17. Total kinetic energy release in 239Pu(n ,f ) post-neutron emission from 0.5 to 50 MeV incident neutron energy

    NASA Astrophysics Data System (ADS)

    Meierbachtol, K.; Tovesson, F.; Duke, D. L.; Geppert-Kleinrath, V.; Manning, B.; Meharchand, R.; Mosby, S.; Shields, D.

    2016-09-01

    The average total kinetic energy (T K E ¯) in 239Pu(n ,f ) has been measured for incident neutron energies between 0.5 and 50 MeV. The experiment was performed at the Los Alamos Neutron Science Center (LANSCE) using the neutron time-of-flight technique, and the kinetic energy of fission fragments post-neutron emission was measured in a double Frisch-gridded ionization chamber. This represents the first experimental study of the energy dependence of T K E ¯ in 239Pu above neutron energies of 6 MeV.

  18. Distribution of nuclear bomb Pu in Nishiyama area, Nagasaki, estimated by accurate and precise determination of 240Pu/239Pu ratio in soils.

    PubMed

    Yoshida, S; Muramatsu, Y; Yamazaki, S; Ban-Nai, T

    2007-01-01

    Plutonium isotopes in forest soils collected in Nishiyama area, Nagasaki, were successfully determined by high resolution inductively coupled plasma mass spectrometry after the treatment with a microwave decomposition system. The (240)Pu/(239)Pu atom ratios observed in the samples in the Nishiyama area were obviously lower than the range of the global fallout. The low ratios (minimum 0.032) observed in Nishiyama area indicated the influence of detonation of the Pu nuclear weapon in 1945. Since the area is contaminated also by global fallout, the (240)Pu/(239)Pu atom ratio can be more sensitive indicator of bomb-derived Pu than Pu activity concentration.

  19. Determination of 240Pu/239Pu atom ratio in coastal surface seawaters from the western North Pacific Ocean and Japan Sea.

    PubMed

    Yamada, Masatoshi; Zheng, Jian

    2008-01-01

    Surface seawater samples were collected from a site in the vicinity of the nuclear fuel reprocessing facility at Rokkasho, Japan and sites along the Japan Sea coast. (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were determined by alpha-spectrometry and isotope-dilution sector-field ICP-MS. The (240)Pu/(239)Pu atom ratio with the mean value of 0.227 +/- 0.006 was significantly higher than the mean global fallout ratio of 0.18. The contribution of the Pacific Proving Grounds close-in fallout was estimated to be 33% of the (239+240)Pu.

  20. In vivo measurement of 241Am in the lungs confounded by activity deposited in other organs.

    PubMed

    Lobaugh, Megan L; Spitz, Henry B; Glover, Samuel E

    2015-01-01

    Radioactive material deposited in multiple organs of the body is likely to confound a result of an in vivo measurement performed over the lungs, the most frequently monitored organ for occupational exposure. The significance of this interference was evaluated by measuring anthropometric torso phantoms containing lungs, liver, skeleton, and axillary lymph nodes, each with a precisely known quantity of 241Am uniformly distributed in the organs. Arrays of multiple high-resolution germanium detectors were positioned over organs within the torso phantom containing 241Am or over proximal organs without activity to determine the degree of measurement confounding due to photons emitted from other source organs. A set of four mathematical response functions describes the measured count rate with detectors positioned over each of the relevant organs and 241Am contained in the measured organ or one of the other organs selected as a confounder. Simultaneous solution of these equations by matrix algebra, where the diagonal terms of the matrix are calibration factors for a direct measurement of activity in an organ and the off-diagonal terms reflect the contribution (i.e., interference or cross-talk) produced by 241Am in a confounding organ, yields the activity deposited in each of the relevant organs. The matrix solution described in this paper represents a method for adjusting a result of 241Am measured directly in one organ for interferences that may arise from 241Am deposited elsewhere and represents a technically valid procedure to aid in evaluating internal dose based upon in vivo measurements for those radioactive materials known to deposit in multiple organs.

  1. Soft tissue tumors in beagles injected with {sup 241}Am citrate

    SciTech Connect

    Lloyd, R.D.; Taylor, G.N.; Angus, W.

    1995-02-01

    The occurrence of soft tissue tumors has been studied in 117 beagles assigned to 8 dosage groups of between 2 and 26 animals each and injected with 0.07 to 104 kBq {sup 241}Am kg{sup -1} as the citrate. In addition, 133 control beagles given no radioactivity were used as a comparison group. All 250 dogs were maintained under identical conditions and were observed for their entire lifespans. An important competing risk for the appearance of soft tissue tumors appeared to be the occurrence of skeletal malignancy, and at the highest injected activity (104) kBq kg{sup -1}, kidney and liver failure brought about the death of both of the two dogs in this group. Thyroid and liver were the only soft tissues that exhibited greater concentrations of {sup 241}Am than the skeleton. Liver tumors were associated {sup 241}Am exposure (p < 0.001), but the thyroid tumor rate was not increased significantly in the irradiated animals (p > 0.10) as compared with the occurrence in controls. There was a greater relative occurrence of all vaginal tumors in control animals than in dogs given {sup 241}Am, a situation also found for all tumors of the pancreas, skin, testis, and mammary glands and for malignant ovarian tumors. All of these differences were statistically significant. The survival of animals given 0.07 to 0.59 kBq {sup 241}Am Kg{sup -1} could not be established (p > 0.10) as significantly different from controls, but the survival of all groups given 1.8 to 104 kBq kg{sup -1} was decreased (p < 0.05). There was no indication in our studies of a positive association between relative exposure to {sup 241}Am and the occurrence of mammary tumors, mast cell sarcomas originating outside the liver, lymphosarcoma or tumors of marrow, including leukemia. 20 refs., 1 fig., 8 tabs.

  2. Species-dependent effective concentration of DTPA in plasma for chelation of 241Am

    PubMed Central

    Sueda, Katsuhiko; Sadgrove, Matthew P.; Jay, Michael; Di Pasqua, Anthony J.

    2013-01-01

    Diethylenetriaminepentaacetic acid (DTPA) is a chelating agent that is used to facilitate the elimination of radionuclides, such as americium, from contaminated individuals. Its primary site of action is in the blood, where it competes with various biological ligands, including transferrin and albumin, for the binding of radioactive metals. To evaluate the chelation potential of DTPA under these conditions, the competitive binding of 241Am between DTPA and plasma proteins was studied in rat, beagle and human plasma in vitro. Following incubation of DTPA and 241Am in plasma, the 241Am-bound ligands were fractionated by ultrafiltration and ion-exchange chromatography, and each fraction was assayed for 241Am content by gamma scintillation counting. Dose-response curves of DTPA for 241Am binding were established, and these models were used to calculate the 90% maximal effective concentration, or EC90, of DTPA in each plasma system. The EC90 were determined to be 31.4, 15.9 and 10.0 μM in rat, beagle and human plasma, respectively. These values correspond to plasma concentrations of DTPA that maximize 241Am chelation while minimizing excess DTPA. Based on the pharmacokinetic profile of DTPA in humans, after a standard 30 μmol kg−1 intravenous bolus injection, the plasma concentration of DTPA remains above EC90 for approximately 5.6 h. Likewise, the effective duration of DTPA in rat and beagle were determined to be 0.67 and 1.7 h, respectively. These results suggest that species differences must be considered when translating DTPA efficacy data from animals to humans and offer further insights into improving the current DTPA treatment regimen. PMID:23799506

  3. Evaluating the 239Pu prompt fission neutron spectrum induced by thermal to 30 MeV neutrons

    DOE PAGES

    Neudecker, Denise; Talou, Patrick; Kawano, Toshihiko; ...

    2016-03-15

    We present a new evaluation of the 239Pu prompt fission neutron spectrum (PFNS) induced by thermal to 30 MeV neutrons. Compared to the ENDF/B-VII.1 evaluation, this one includes recently published experimental data as well as an improved and extended model description to predict PFNS. For instance, the pre-equilibrium neutron emission component to the PFNS is considered and the incident energy dependence of model parameters is parametrized more realistically. Experimental and model parameter uncertainties and covariances are estimated in detail. Also, evaluated covariances are provided between all PFNS at different incident neutron energies. In conclusion, selected evaluation results and first benchmarkmore » calculations using this evaluation are briefly discussed.« less

  4. Development of an 241Am applicator for intracavitary irradiation of gynecologic cancers.

    PubMed

    Nath, R; Peschel, R E; Park, C H; Fischer, J J

    1988-05-01

    Sealed sources of 241Am that emit primarily 60 keV photons produce relative dose distributions in water comparable to those from 137Cs or 226Ra sources and can produce dose rates of up to 100 cGy/hr at 1 cm in water. Also, 241Am gamma rays can be effectively shielded by thin layers of high atomic number materials (HVL is 1/8th mm of lead) placed on the applicator or inside some body cavities (for example, hypaque in bladder, barium sulphate in rectum). These properties of 241Am sources open a new approach to optimizing intracavitary irradiation of various cancers by allowing a reduction in dose and volume of irradiated critical organs or by increasing tumor doses. The relative ease with which highly effective shielding is achievable with 241Am sources would allow the design and fabrication of partially shielded applicators which can produce asymmetric dose distributions to allow unidirectional irradiation of localized lesions. Design and dosimetry characteristics of a gynecological applicator containing 241Am sources are presented. The applicator consists of a 2, 3, or 4 segment vaginal plaque (loaded with 2 and 5 Ci 241Am sources) and a tandem made up of a single 8 Ci 241Am source. Dose rates at 2 cm from the plaques are 42.0, 47.4, 58.3 and 56.7 cGy/hr for 5-5, 5-4-5, 5-5-5, and 5-4-4-5 Ci plaques, respectively. The 5-4-5 Ci plaque in combination with the 8 Ci tandem produces dose rates of 60.0 and 22.8 cGy/hr to points A and B, respectively. Surface dose rates on the plaque applicators are 143, 124, 142 and 132 cGy/hr for 5-5, 5-4-5, 5-5-5 and 5-4-4-5 Ci applicators, respectively. The shielding effect of a 0.5 mm thick lead foil on one side of the 5-4-5 Ci applicator is found to be a factor of 16.8; for example, the dose rate at 2 cm from the unshielded side is 42.0 cGy/hr compared to a dose rate of 2.5 cGy/hr at 2 cm from the shielded side. Initial clinical experience with this applicator in the treatment of recurrent gynecological lesions is also presented.

  5. Determination of Pu isotopes and 241Am in a reference fallout material using SF-ICP-MS.

    PubMed

    Zheng, Jian; Zhang, Yongsan; Yamada, Masatoshi; Wu, Fengchang; Igarashi, Yasuhito; Hirose, Katsumi

    2011-07-01

    This paper reports on the characterisation of activities of Pu and (241)Am, and Pu isotopic composition in a reference fallout material prepared by the Meteorological Research Institute (MRI), Japan, from samples collected at 14 stations throughout Japan in 1963-1979. The acid leaching and total digestion were used to compare whether there is difference in Pu and (241)Am activities and Pu isotopic composition between these two methods. The results of activities of (239+240)Pu and (241)Pu, and Pu isotopic composition have been reported in the previous work (Sci. Total Environ. 2010, 408, 1139-1144). In this study, the (241)Am activity and (241)Am/(239+240)Pu activity ratio in the reference fallout material are reported, and the usefulness of Pu atom ratios and (241)Am/(239+240)Pu activity ratio for source identification is discussed.

  6. Standardization of 241Am by digital coincidence counting, liquid scintillation counting and defined solid angle counting.

    PubMed

    Balpardo, C; Capoulat, M E; Rodrigues, D; Arenillas, P

    2010-01-01

    The nuclide (241)Am decays by alpha emission to (237)Np. Most of the decays (84.6%) populate the excited level of (237)Np with energy of 59.54 keV. Digital coincidence counting was applied to standardize a solution of (241)Am by alpha-gamma coincidence counting with efficiency extrapolation. Electronic discrimination was implemented with a pressurized proportional counter and the results were compared with two other independent techniques: Liquid scintillation counting using the logical sum of double coincidences in a TDCR array and defined solid angle counting taking into account activity inhomogeneity in the active deposit. The results show consistency between the three methods within a limit of a 0.3%. An ampoule of this solution will be sent to the International Reference System (SIR) during 2009. Uncertainties were analysed and compared in detail for the three applied methods.

  7. Investigation of the 241Am(n ,2 n )240Am cross section

    NASA Astrophysics Data System (ADS)

    Kalamara, A.; Vlastou, R.; Kokkoris, M.; Diakaki, M.; Tsinganis, A.; Patronis, N.; Axiotis, M.; Lagoyannis, A.

    2016-01-01

    The 241Am(n ,2 n )240Am reaction cross section has been measured at four energies, 10.0, 10.4, 10.8, and 17.1 MeV, by means of the activation technique, relative to the 27Al(n ,α )24Na reaction reference cross section. Quasi-monoenergetic neutron beams were produced via the 2H(d ,n )3He and the 3H(d ,n )4He reactions at the 5.5 MV Tandem T11/25 accelerator laboratory of NCSR "Demokritos". The high purity 241Am targets were provided by JRC-IRMM, Geel, Belgium. The induced γ -ray activity of 240Am was measured with high-resolution high-purity germanium (HPGe) detectors. Auxiliary Monte Carlo simulations were performed with the mcnp code. The present results are in agreement with data obtained earlier and predictions obtained with the empire code.

  8. Postmortem tissue contents of {sup 241}Am in a person with a massive acute exposure

    SciTech Connect

    McInroy, J.F.; Kathren, R.L.; Toohey, R.E. |

    1995-09-01

    {sup 241}Am was determined radiochemically in the tissues of USTUR Case 246, a 76-y-old man who died of cardiovascular disease 11 y after massive percutaneous exposure following a chemical explosion in a glove box. This worker was treated extensively with a chelation drug, DTPA, for over 4 y after exposure. The estimate {sup 241}Am deposition at the time of death was 540 kBq, of which 90% was in the skeleton, 5.1% in the liver, and 3.5% in muscle and fat. Among the soft tissues, the highest concentrations were observed in liver (22 Bq g{sup -1}), certain cartilaginous structures such as the larynx (15 Bq g{sup -1}) and the red marrow (9.7 Bq g{sup -1}), as compared with the mean soft tissue concentration of approximately 1 Bq g{sup -1}. Concentration in muscle was approximately that of the soft tissue average, while concentrations in the pancreas, a hilar lymph node and fat were less than the average. Concentrations in bone ash were inversely related to the ratio of ash weight to wet weight a surrogate for bone volume-to-surface ratio. the distribution of activity in this case is reasonable consistent with that observed in another human case, when allowance is made for chelation therapy, and also tends to support more recent models of {sup 241}Am metabolism. 26 refs., 2 figs., 4 tabs.

  9. Neutron-induced transmutation reactions in 237Np, 238Pu, and 239Pu at the massive natural uranium spallation target

    NASA Astrophysics Data System (ADS)

    Zavorka, L.; Adam, J.; Baldin, A. A.; Caloun, P.; Chilap, V. V.; Furman, W. I.; Kadykov, M. G.; Khushvaktov, J.; Pronskikh, V. S.; Solnyshkin, A. A.; Sotnikov, V.; Stegailov, V. I.; Suchopar, M.; Tsoupko-Sitnikov, V. M.; Tyutyunnikov, S. I.; Voronko, V.; Vrzalova, J.

    2015-04-01

    Transmutation reactions in the 237Np, 238Pu, and 239Pu samples were investigated in the neutron field generated inside a massive (m = 512 kg) natural uranium spallation target. The uranium target assembly QUINTA was irradiated with the deuteron beams of kinetic energy 2, 4, and 8 GeV provided by the Nuclotron accelerator at the Joint Institute for Nuclear Research (JINR) in Dubna. The neutron-induced transmutation of the actinide samples was measured off-line by implementing methods of gamma-ray spectrometry with HPGe detectors. Results of measurement are expressed in the form of both the individual reaction rates and average fission transmutation rates. For the purpose of validation of radiation transport programs, the experimental results were compared with simulations of neutron production and distribution performed by the MCNPX 2.7 and MARS15 codes employing the INCL4-ABLA physics models and LAQGSM event generator, respectively. In general, a good agreement between the experimental and calculated reaction rates was found in the whole interval of provided beam energies.

  10. Fission Mode Influence on Prompt Neutrons and γ-rays Emitted in the Reaction 239Pu(nth,f)

    NASA Astrophysics Data System (ADS)

    Serot, O.; Litaize, O.; Regnier, D.

    Recently, a Monte-Carlo code, which simulates the fission fragment de-excitation process, has been developed at CEA- Cadarache. Our aim is to get a tool capable to predict spectra and multiplicities of prompt particles (neutron and gamma) and to investigate possible correlations between fission observables. One of the main challenges is to define properly the share of the available excitation energy at scission between the two nascent fission fragments. Initially, after the full acceleration of the fission fragments, these excitation energies were treated within a Fermi-gas approximation in aT2 (where a and T stand for the level density parameter and the nuclear temperature) and a mass dependent law of the temperature ratio (RT=TL/TH, with TL and TH the temperature of the light and heavy fragment) has been proposed. With this RT-law, the main fission observables of the 252Cf(sf) could be reproduced. Here, in order to take into account the fission modes by which the fissioning nucleus undergoes to fission, we have adopted a specific RT-law for each fission mode. For actinides, the main fission modes are called Standard I, Standard II and Super Long (following Brosa's terminology). This new procedure has been applied in the case of the thermal neutron induced fission of 239Pu, reaction for which fission modes are rather well known.

  11. The CIELO Collaboration: Neutron Reactions on 1H, 16O, 56Fe, 235,238U, and 239Pu

    NASA Astrophysics Data System (ADS)

    Chadwick, M. B.; Dupont, E.; Bauge, E.; Blokhin, A.; Bouland, O.; Brown, D. A.; Capote, R.; Carlson, A.; Danon, Y.; De Saint Jean, C.; Dunn, M.; Fischer, U.; Forrest, R. A.; Frankle, S. C.; Fukahori, T.; Ge, Z.; Grimes, S. M.; Hale, G. M.; Herman, M.; Ignatyuk, A.; Ishikawa, M.; Iwamoto, N.; Iwamoto, O.; Jandel, M.; Jacqmin, R.; Kawano, T.; Kunieda, S.; Kahler, A.; Kiedrowski, B.; Kodeli, I.; Koning, A. J.; Leal, L.; Lee, Y. O.; Lestone, J. P.; Lubitz, C.; MacInnes, M.; McNabb, D.; McKnight, R.; Moxon, M.; Mughabghab, S.; Noguere, G.; Palmiotti, G.; Plompen, A.; Pritychenko, B.; Pronyaev, V.; Rochman, D.; Romain, P.; Roubtsov, D.; Schillebeeckx, P.; Salvatores, M.; Simakov, S.; Soukhovitskiı˜, E. Sh.; Sublet, J. C.; Talou, P.; Thompson, I.; Trkov, A.; Vogt, R.; van der Marck, S.

    2014-04-01

    CIELO (Collaborative International Evaluated Library Organization) provides a new working paradigm to facilitate evaluated nuclear reaction data advances. It brings together experts from across the international nuclear reaction data community to identify and document discrepancies among existing evaluated data libraries, measured data, and model calculation interpretations, and aims to make progress in reconciling these discrepancies to create more accurate ENDF-formatted files. The focus will initially be on a small number of the highest-priority isotopes, namely 1H, 16O, 56Fe, 235,238U, and 239Pu. This paper identifies discrepancies between various evaluations of the highest priority isotopes, and was commissioned by the OECD's Nuclear Energy Agency WPEC (Working Party on International Nuclear Data Evaluation Co-operation) during a meeting held in May 2012. The evaluated data for these materials in the existing nuclear data libraries - ENDF/B-VII.1, JEFF-3.1, JENDL-4.0, CENDL-3.1, ROSFOND, IRDFF 1.0 - are reviewed, discrepancies are identified, and some integral properties are given. The paper summarizes a program of nuclear science and computational work needed to create the new CIELO nuclear data evaluations.

  12. Neutron emission effects on fragment mass and kinetic energy distribution from fission of 239Pu induced by thermal neutrons

    NASA Astrophysics Data System (ADS)

    Montoya, M.; Rojas, J.; Lobato, I.

    2010-08-01

    The average of fragment kinetic energy (E*) and the multiplicity of prompt neutrons (ν) as a function of fragment mass (m*), as well as the fragment mass yield (Y(m*)) from thermal neutron-induced fission of 239Pu have been measured by Tsuchiya et al.. In that work the mass and kinetic energy are calculated from the measured kinetic energy of one fragment and the difference of time of flight of the two complementary fragments. However they do not present their results about the standard deviation σE*(m*). In this work we have made a numerical simulation of that experiment which reproduces its results, assuming an initial distribution of the primary fragment kinetic energy (E(A)) with a constant value of the standard deviation as function of fragment mass (σE(A)). As a result of the simulation we obtain the dependence σE*(m*) which presents an enhancement between m* = 92 and m* = 110, and a peak at m* = 121.

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

    NASA Astrophysics Data System (ADS)

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

    2016-09-01

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

  14. Different Interaction Mechanisms of Eu(III) and (243)Am(III) with Carbon Nanotubes Studied by Batch, Spectroscopy Technique and Theoretical Calculation.

    PubMed

    Wang, Xiangxue; Yang, Shubin; Shi, Weiqun; Li, Jiaxing; Hayat, Tasawar; Wang, Xiangke

    2015-10-06

    Herein the sorption of Eu(III) and (243)Am(III) on multiwalled carbon nanotubes (CNTs) are studied, and the results show that Eu(III) and (243)Am(III) could form strong inner-sphere surface complexes on CNT surfaces. However, the sorption of Eu(III) on CNTs is stronger than that of (243)Am(III) on CNTs, suggesting the difference in the interaction mechanisms or properties of Eu(III) and (243)Am(III) with CNTs, which is quite different from the results of Eu(III) and (243)Am(III) interaction on natural clay minerals and oxides. On the basis of the results of density functional theory calculations, the binding energies of Eu(III) on CNTs are much higher than those of (243)Am(III) on CNTs, indicating that Eu(III) could form stronger complexes with the oxygen-containing functional groups of CNTs than (243)Am(III), which is in good agreement with the experimental results of higher sorption capacity of CNTs for Eu(III). The oxygen-containing functional groups contribute significantly to the uptake of Eu(III) and (243)Am(III), and the binding affinity increases in the order of ≡S-OH < ≡S-COOH < ≡S-COO(-). This paper highlights the interaction mechanism of Eu(III) and (243)Am(III) with different oxygen-containing functional groups of CNTs, which plays an important role for the potential application of CNTs in the preconcentration, removal, and separation of trivalent lanthanides and actinides in environmental pollution cleanup.

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

    SciTech Connect

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

    2008-12-15

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

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

    SciTech Connect

    Kleinrath, Verena

    2015-07-01

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

  17. Effects of combined exposure of F344 rats to inhaled {sup 239}PuO{sub 2} and a chemical carcinogen (NNK)

    SciTech Connect

    Lundgren, D.L.; Belinsky, S.A.; Nikula, K.J.; Griffith, W.C.; Hoover, M.D.

    1994-11-01

    Workers in nuclear weapons facilitates have a significant potential for exposure to chemical carcinogens and to radiation from external sources or from internally deposited radionuclides such as {sup 239}Pu. Although the carcinogenic effects of inhaled {sup 239}Pu and many chemicals have been studied individually, very little information is available on their combined effects. One chemical carcinogen that workers could be exposed to, via tobacco smoke, is the tobacco-specific nitrosamine 4-(N-Methyl-N-nitrosamino)-1-(3-pyridyl)-1-butanone (NNK), a product of the curing of tobacco and pyrolysis of nicotine in tobacco. NNK causes lung tumors in rats, regardless of the route of administration and to a lesser extent tumors in the liver, nasal passages, and pancreas. The purpose of this study is to characterize the effects of combined exposure of rats to NNK and internally deposited plutonium, as well as to these agents alone.

  18. Second interlaboratory comparison study for the analysis of 239Pu in synthetic urine at the microBq (-100 aCi) level by mass spectrometry

    SciTech Connect

    McCurdy, D; Lin, Z; Inn, K W; Bell III, R; Wagner, S; Efurd, D W; Steiner, R; Duffy, C; Hamilton, T F; Brown, T A; Marchetti, A A

    2005-01-28

    As a follow up to the initial 1998 intercomparison study, a second study was initiated in 2001 as part of the ongoing evaluation of the capabilities of various ultra-sensitive methods to analyze {sup 239}Pu in urine samples. The initial study was sponsored by the Department of Energy, Office of International Health Programs to evaluate and validate new technologies that may supersede the existing fission tract analysis (FTA) method for the analysis of {sup 239}Pu in urine at the {micro}Bq/l level. The ultra-sensitive techniques evaluated in the second study included accelerator mass spectrometry (AMS) by LLNL, thermal ionization mass spectrometry (TIMS) by LANL and FTA by the University of Utah. Only the results for the mass spectrometric methods will be presented. For the second study, the testing levels were approximately 4, 9, 29 and 56 {micro}Bq of {sup 239}Pu per liter of synthetic urine. Each test sample also contained {sup 240}Pu at a {sup 240}Pu/{sup 239}Pu atom ratio of {approx}0.15 and natural uranium at a concentration of 50 {micro}Bq/ml. From the results of the two studies, it can be inferred that the best performance at the {micro}Bq level is more laboratory specific than method specific. The second study demonstrated that LANL-TIMS and LLNL-AMS had essentially the same quantification level for both isotopes. Study results for bias and precision and acceptable performance compared to ANSI N13.30 and ANSI N42.22 have been compiled.

  19. 240Pu/239Pu isotopic ratios and 239 + 240Pu total measurements in surface and deep waters around Mururoa and Fangataufa atolls compared with Rangiroa atoll (French Polynesia).

    PubMed

    Chiappini, R; Pointurier, F; Millies-Lacroix, J C; Lepetit, G; Hemet, P

    1999-09-30

    The average values of 240Pu/239Pu mass isotopic ratios of plutonium deposited in Mururoa and Fangataufa atoll sediments by French atmospheric nuclear tests range from 3.5 to 5%. In order to assess the near field and far field influence of those deposits in the open ocean, two water profiles were measured for 239 + 240Pu and 240Pu/239Pu using, for the first time, an Inductively Coupled Plasma Mass Spectrometer which was developed to achieve femtogram detection limits. One site was located at the limit of the French territorial waters, which is 22 km distant from Mururoa. The second site was located close to Rangiroa atoll, at a distance of approximately 1200-km from French nuclear test sites. The sample volumes were approximately 500 litres and plutonium was purified prior to mass spectrometry and alpha spectrometry measurements. In Rangiroa, the 239 + 240Pu profile is comparable with those already determined in world open oceans but the maximum detected activity, 9 mBq/m3 at 500-600 m is a lot lower than those measured in the northern hemisphere. 240Pu/239Pu ratios were measured between 500 and 1000 m and were not statistically different from the typical 0.18 +/- 0.01 ratio which characterises the global fallout. Consequently, any influence of plutonium from the tests in Mururoa and Fangataufa is not apparent at Rangiroa. The vertical distribution of 239 + 240Pu near Mururoa shows similar changes with depth but with a slight increase in concentration. 240Pu/239Pu mass ratios vary with depth, from 7 to 10% in the upper 500 m and in the deep waters (below 1000 m) to 15-16% between 600 and 1000 m. A contribution from plutonium deposited in the sediments at Mururoa and Fangataufa is observed at the limit of territorial waters, especially in surface and deep waters.

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

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  1. Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements.

    PubMed

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin; Pan, Shaoming; Roos, Per

    2014-02-01

    This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5 × 10(5) for 20 g soil compared to the level reported in the literature, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation.

  2. Reassessment of 239Pu on planchets from human urine samples at ultra-trace levels using Aridus-ICPSFMS and AMS.

    PubMed

    Hernández-Mendoza, Héctor; Chamizo, Elena; Delgado, Antonio; García-León, Manuel; Yllera, Abel

    2012-12-01

    New analytical methods developed at the facilities here, based on two ultra-sensitive mass spectrometry (MS) techniques, inductively coupled plasma sector field mass spectrometer with a desolvator system (Aridus-ICP-SFMS) and accelerator MS (AMS), have been applied in this work for the reassessment of (239)Pu in alpha spectrometry (AS) planchets corresponding to spiked human urine samples. The obtained (239)Pu minimum detectable activities (MDAs) values by Aridus-ICP-SFMS and AMS were 3 fg (∼6.92 µBq) and 0.4 fg (∼0.92 µBq), respectively, per sample, which are much better than those attainable by AS [50 fg (∼115.3 µBq) of (239)Pu per sample, approximately]. Therefore, it is demonstrated that the MS techniques employed in this work are very powerful tools for internal dosimetry studies in human urine samples, giving excellent results when the reassessment of AS planchets is needed (samples with a Pu concentration below or at the MDA levels measurable by AS). This work is the continuation of an article published in J. Anal. At. Spectrom. 25 (1410-1415) 2010.

  3. 243Am + 48Ca: A Second Look at the Rf/Db Data Set

    SciTech Connect

    Henderson, R A; Moody, K J

    2008-01-29

    In December of 2005 a series of experiments were performed at the U400 Cyclotron at the Flerov Laboratory of Nuclear Reactions in Dubna, Russia, using the reaction {sup 243}Am ({sup 48}Ca,3n) {sup 288}115 which, after a sequence of five alpha decays, produces a long-lived ({approx}1d) fission activity that had been detected previously in experiments using the Dubna Gas Filled Recoil Separator (DGFRS). These experiments were attempts to establish the elemental identity of the fissioning species as dubnium (element 105), which in turn confirms the identity of the original parent nucleus as element 115 through genetic correlation of the subsequent alpha decays. A series of approximately 24-hour bombardments were followed by chemical separations designed to isolate the Group Four and Five chemical fractions, and then separate the Nb and Ta fractions, which are Group Five homologues of dubnium and should therefore behave chemically similar. The samples were prepared for alpha and fission measurement and counted for an extended period of time. Fission events were detected in the Ta-like fractions only, which correspond to the fission coming from either the {sup 268}Db isotope directly or long-lived electron-capture decay in {sup 268}Db followed by a short half-life fission of {sup 268}Rf. In May of 2007 the Rf and Db fractions were recounted for very long times on alpha spectrometers to look at what species remained after approximately 1.5 years of time. One of the issues to be resolved was the potential for actinide contamination of the counting samples, which might have adverse affects on the observed data from the original experiment. In the original experiment the samples had significant quantities of {beta}-{gamma} activity which made the absolute identification of the alpha activity in each sample difficult. By allowing the {beta}-{gamma} activity to decay away, it gives us the opportunity to make definitive identifications of any alpha emitting isotopes on the

  4. Evaluation of the 239Pu prompt fission neutron spectrum induced by neutrons of 500 keV and associated covariances

    NASA Astrophysics Data System (ADS)

    Neudecker, D.; Talou, P.; Kawano, T.; Smith, D. L.; Capote, R.; Rising, M. E.; Kahler, A. C.

    2015-08-01

    We present evaluations of the prompt fission neutron spectrum (PFNS) of 239Pu induced by 500 keV neutrons, and associated covariances. In a previous evaluation by Talou et al. (2010), surprisingly low evaluated uncertainties were obtained, partly due to simplifying assumptions in the quantification of uncertainties from experiment and model. Therefore, special emphasis is placed here on a thorough uncertainty quantification of experimental data and of the Los Alamos model predicted values entering the evaluation. In addition, the Los Alamos model was extended and an evaluation technique was employed that takes into account the qualitative differences between normalized model predicted values and experimental shape data. These improvements lead to changes in the evaluated PFNS and overall larger evaluated uncertainties than in the previous work. However, these evaluated uncertainties are still smaller than those obtained in a statistical analysis using experimental information only, due to strong model correlations. Hence, suggestions to estimate model defect uncertainties are presented, which lead to more reasonable evaluated uncertainties. The calculated keff of selected criticality benchmarks obtained with these new evaluations agree with each other within their uncertainties despite the different approaches to estimate model defect uncertainties. The keff one standard deviations overlap with some of those obtained using ENDF/B-VII.1, albeit their mean values are further away from unity. Spectral indexes for the Jezebel critical assembly calculated with the newly evaluated PFNS agree with the experimental data for selected (n,γ) and (n,f) reactions, and show improvements for high-energy threshold (n,2n) reactions compared to ENDF/B-VII.1.

  5. Electronic structure of polycrystalline Cd metal using {sup 241}Am radioisotope

    SciTech Connect

    Dhaka, M. S.; Sharma, G.; Mishra, M. C.; Sharma, B. K.

    2014-04-24

    Electronic structure study of the polycrystalline cadmium metal is reported. The experimental measurement is undertaken on a polycrystalline sheet sample using 59.54 keV radioisotope of {sup 241}Am. These results are compared with the ab initio calculations. The theoretical calculations are performed using linear combination of atomic orbitals (LCAO) method employing the density functional theories (DFT) and Hartree-Fock (HF) and augmented plane wave (APW) methods. The spherically averaged APW and LCAO based theoretical Compton profiles are in good agreement with the experimental measurement however the APW based theoretical calculations show best agreement.

  6. Orally administered DTPA penta-ethyl ester for the decorporation of inhaled 241Am

    PubMed Central

    Sueda, Katsuhiko; Sadgrove, Matthew P.; Huckle, James E.; Leed, Marina G. D.; Weber, Waylon M.; Doyle-Eisele, Melanie; Guilmette, Raymond A.; Jay, Michael

    2014-01-01

    Diethylenetriaminepentaacetic acid (DTPA) is an effective decorporation agent to facilitate the elimination of radionuclides from the body, but its permeability-limited oral bioavailability limits its utility in mass-casualty emergencies. To overcome this limitation, a prodrug strategy using the penta-ethyl ester form of DTPA is under investigation. Pharmacokinetic and biodistribution studies were conducted in rats by orally administering [14C]DTPA penta-ethyl ester, and this prodrug and its hydrolysis products were analyzed as a single entity. Compared to a previous reporting of intravenously administered DTPA, the oral administration of this prodrug resulted in a sustained plasma concentration profile with higher plasma exposure and lower clearance. An assessment of the urine composition revealed that the bioactivation was extensive but incomplete, with no detectable levels of the penta- or tetra-ester forms. Tissue distribution at 12 h was limited, with approximately 73% of the administered dose being associated with the gastrointestinal tract. In the efficacy study, rats were exposed to aerosols of 241Am nitrate before receiving a single oral treatment of the prodrug. The urinary excretion of 241Am was found to be 19% higher than with the control. Consistent with prior reports of DTPA, the prodrug was most effective when the treatment delays were minimized. PMID:24619514

  7. Determination of (n,γ) Cross Sections of 241Am by Cold Neutron Activation

    NASA Astrophysics Data System (ADS)

    Genreith, C.; Rossbach, M.; Révay, Zs.; Kudejova, P.

    2014-05-01

    Accurate cross section data of actinides are crucial for criticality calculations of GEN IV reactors and transmutation but also for analytical purposes such as nuclear waste characterization, decommissioning of nuclear installations and safeguard applications. Tabulated data are inconsistent and sometimes associated with large uncertainties. Neutron activation with external cold neutron beams from high flux reactors offers a chance for determination of accurate capture cross sections scalable to the whole 1/√{E}-region even for isotopes with low-lying resonances like 241Am. Preparation of 241Am samples for irradiation at the PGAA station of the FRM II in Garching has been optimized together with PTB in Braunschweig. Two samples were irradiated together with gold flux monitors to extract the thermal neutron capture cross section after appropriate corrections for attenuation of neutrons and photons in the sample. For one sample, the thermal ground state neutron capture cross section was measured as 663.0 ± 28.8 b. The thermal neutron capture cross section was calculated to 725.4 ± 34.4 b. For the other sample, a ground state neutron capture cross section of 649.9 ± 28.2 b was measured and a thermal neutron capture cross section of 711.1 ± 33.9 b was derived.

  8. 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.

  9. Fission fragment charge and mass distributions in 239Pu(n ,f ) in the adiabatic nuclear energy density functional theory

    NASA Astrophysics Data System (ADS)

    Regnier, D.; Dubray, N.; Schunck, N.; Verrière, M.

    2016-05-01

    Background: Accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data are available, together with the variety of potential applications, is an incentive to develop a fully microscopic approach to fission dynamics. Purpose: In this work, we calculate the pre-neutron emission charge and mass distributions of the fission fragments formed in the neutron-induced fission of 239Pu using a microscopic method based on nuclear density functional theory (DFT). Methods: Our theoretical framework is the nuclear energy density functional (EDF) method, where large-amplitude collective motion is treated adiabatically by using the time-dependent generator coordinate method (TDGCM) under the Gaussian overlap approximation (GOA). In practice, the TDGCM is implemented in two steps. First, a series of constrained EDF calculations map the configuration and potential-energy landscape of the fissioning system for a small set of collective variables (in this work, the axial quadrupole and octupole moments of the nucleus). Then, nuclear dynamics is modeled by propagating a collective wave packet on the potential-energy surface. Fission fragment distributions are extracted from the flux of the collective wave packet through the scission line. Results: We find that the main characteristics of the fission charge and mass distributions can be well reproduced by existing energy functionals even in two-dimensional collective spaces. Theory and experiment agree typically within two mass units for the position of the asymmetric peak. As expected, calculations are sensitive to the structure of the initial state and the prescription for the collective inertia. We emphasize that results are also sensitive to the continuity of the collective landscape near scission. Conclusions: Our analysis confirms

  10. Event-by-event evaluation of the prompt fission neutron spectrum from 239Pu(n,f)

    SciTech Connect

    Vogt, R; Randrup, J; Brown, D A; Descalle, M A; Ormand, W E

    2011-11-28

    We have developed an improved evaluation method for the spectrum of neutrons emitted in fission of {sup 239}Pu induced by incident neutrons with energies up to 20 MeV. The covariance data, including incident energy correlations introduced by the evaluation method, were used to fix the input parameters in our event-by-event model of fission, FREYA, by applying formal statistical methods. Formal estimates of uncertainties in the evaluation were developed by randomly sampling model inputs and calculating likelihood functions based on agreement with the evaluated . Our approach is able to employ a greater variety of fission measurements than the relatively coarse spectral data alone. It also allows the study of numerous fission observables for more accurate model validation. The combination of an event-by-event Monte Carlo fission model with a statistical-likelihood analysis is thus a powerful tool for evaluation of fission-neutron data. Our empirical model FREYA follows the complete fission event from birth of the excited fragments through their decay via neutron emission until the fragment excitation energy is below the neutron separation energy when neutron emission can no longer occur. The most recent version of FREYA incorporates pre-equilibrium neutron emission, the emission of the first neutron before equilibrium is reached in the compound nucleus, and multi-chance fission, neutron evaporation prior to fission when the incident neutron energy is above the neutron separation energy. Energy, momentum, charge and mass number are conserved throughout the fission process. The best available values of fragment masses and total kinetic energies are used as inputs to FREYA. We fit three parameters that are not well under control from previous measurements: the shift in the total fragment kinetic energy; the energy scale of the asymptotic level density parameter, controlling the fragment 'temperature' for neutron evaporation; and the relative excitation of the

  11. Plutonium concentration and (240)Pu/(239)Pu atom ratio in biota collected from Amchitka Island, Alaska: recent measurements using ICP-SFMS.

    PubMed

    Bu, Kaixuan; Cizdziel, James V; Dasher, Douglas

    2013-10-01

    Three underground nuclear tests, including the Unites States' largest, were conducted on Amchitka Island, Alaska. Monitoring of the radiological environment around the island is challenging because of its remote location. In 2008, the Department of Energy (DOE) Office of Legacy Management (LM) became responsible for the long term maintenance and surveillance of the Amchitka site. The first DOE LM environmental survey occurred in 2011 and is part of a cycle of activities that will occur every 5 years. The University of Alaska Fairbanks, a participant in the 2011 study, provided the lichen (Cladonia spp.), freshwater moss (Fontinalis neomexicanus), kelp (Eualaria fistulosa) and horse mussel (Modiolus modiolus) samples from Amchitka Island and Adak Island (a control site). These samples were analyzed for (239)Pu and (240)Pu concentration and (240)Pu/(239)Pu atom ratio using inductively coupled plasma sector field mass spectrometry (ICP-SFMS). Plutonium concentrations and (240)Pu/(239)Pu atom ratios were generally consistent with previous terrestrial and marine studies in the region. The ((239)+)(240)Pu levels (mBq kg(-1), dry weight) ranged from 3.79 to 57.1 for lichen, 167-700 for kelp, 27.9-148 for horse mussel, and 560-573 for moss. Lichen from Adak Island had higher Pu concentrations than Amchitka Island, the difference was likely the result of the higher precipitation at Adak compared to Amchitka. The (240)Pu/(239)Pu atom ratios were significantly higher in marine samples compared to terrestrial and freshwater samples (t-test, p < 0.001); lichen and moss averaged 0.184 ± 0.007, similar to the integrated global fallout ratio, whereas kelp and mussel (soft tissue) averaged 0.226 ± 0.003. These observations provide supporting evidence that a large input of isotopically heavier Pu occurred into the North Pacific Ocean, likely from the Marshall Island high yield nuclear tests, but other potential sources, such as the Kamchatka Peninsula Rybachiy Naval Base and

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

    NASA Astrophysics Data System (ADS)

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

    2013-01-01

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

  13. (239)Pu neutron resonance parameters revisited and covariance matrix in the neutron energy range from thermal to 2.5 keV

    SciTech Connect

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

    2008-01-01

    To obtain the resonance parameters in a single energy range up to 2.5 keV neutron energy and the corresponding covariance matrix, a reevaluation of 239Pu was performed with the analysis code SAMMY. The most recent experimental data were analyzed in the energy range thermal to 2.5 keV. The experimental data were renormalized, aligned on a common energy scale, and corrected for residual background. Average neutron transmission and cross sections calculated with the new resonance parameters were compared to the corresponding experimental data and to ENDF/B-VI.

  14. Determination of 241Am in Urine Using Sector Field Inductively Coupled Plasma Mass Spectrometry (SF-ICP-MS)

    PubMed Central

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

    2016-01-01

    Quantification of 241Am in urine at low levels is important for assessment of individuals’ or populations’ accidental, environmental, or terrorism-related internal contamination, but no convenient, precise method has been established to rapidly determine these low levels. Here we report a new analytical method to measure 241Am as developed and validated at the Centers for Disease Control and Prevention (CDC) by means of the selective retention of Am from urine directly on DGA resin, followed by SF-ICP-MS detection. The method provides rapid results with a Limit of Detection (LOD) of 0.22 pg/L (0.028 Bq/L), which is lower than 1/3 of the C/P CDG for 241Am at 5 days post-exposure. The results obtained by this method closely agree with CDC values as measured by Liquid Scintillation Counting, and with National Institute of Standards Technology (NIST) Certified Reference Materials (CRM) target values. PMID:27375308

  15. Report on the effectiveness of flocculation for removal of {sup 239}Pu at concentrations of 1 pCi/L and 0.1 pCi/L. RFP Pond Water Characterization and Treatment (LATO-EG&G-91-022): Task C deliverables: 5.1.2 and 5.2.2

    SciTech Connect

    Triay, I.R.; Bayhurst, G.K.; Mitchell, A.J.; Cisneros, M.R.; Efurd, D.W.; Roensch, F.R.; Rokop, D.J.; Aguilar, R.D.; Attrep, M.; Nuttall, H.E.

    1993-08-01

    The objective of this work is to assess the effectiveness of flocculation for the removal of Pu from Rocky Flats Plant (RFP) pond waters spiked with {sup 239}Pu at the 1.0 and 0.1 pCi/L level. The flocculation treatment procedure is described in detail. Results are presented for treatment studies for the removal of Pu from C-2 pond water spiked with {sup 239}Pu and from distilled water spiked with {sup 239}Pu.

  16. Measurement/Evaluation Techniques and Nuclear Data Associated with Fission of 239Pu by Fission Spectrum Neutrons

    SciTech Connect

    Baisden, P; Bauge, E; Ferguson, J; Gilliam, D; Granier, T; Jeanloz, R; McMillan, C; Robertson, D; Thompson, P; Verdon, C; Wilkerson, C; Young, P

    2010-03-16

    This Panel was chartered to review and assess new evaluations of work on fission product data, as well as the evaluation process used by the two U.S. nuclear weapons physics laboratories. The work focuses on fission product yields resulting from fission spectrum neutrons incident on plutonium, and includes data from measurements that had not been previously published as well as new or revised fission product cumulative yield data, and related quantities such as Q values and R values. This report documents the Panel's assessment of the work presented by Los Alamos National Laboratory (LANL) and Lawrence Livermore National Laboratory (LLNL). Based on the work presented we have seven key observations: (1) Experiments conducted in the 1970s at LANL, some of which were performed in association with a larger, NIST-led, program, have recently been documented. A preliminary assessment of this work, which will be referred to in this document as ILRR-LANL, shows it to be technically sound. (2) LLNL has done a thorough, unbiased review and evaluation of the available literature and is in the process of incorporating the previously unavailable LANL data into its evaluation of key fission product yields. The results of the LLNL effort, which includes a preliminary evaluation of the ILRR-LANL data, have been documented. (3) LANL has also conducted an evaluation of fission product yields for fission spectrum neutrons on plutonium including a meta-analysis of benchmark data as part of a planned upgrade to the ENDF/B compilation. We found that the approach of using meta-analysis provides valuable additional insight for evaluating the sparse data sets involved in this assessment. (4) Both laboratories have provided convincing evidence for energy dependence in the fission product yield of {sup 147}Nd produced from the bombardment of {sup 239}Pu with fission spectrum neutrons over an incident neutron energy range of 0.2 to 1.9 MeV. (5) Consistent, complete, and explicit treatment of

  17. Exploratory study of fission product yield determination from photofission of 239Pu at 11 MeV with monoenergetic photons

    NASA Astrophysics Data System (ADS)

    Bhike, Megha; Tornow, W.; Krishichayan, Tonchev, A. P.

    2017-02-01

    Measurements of fission product yields play an important role for the understanding of fundamental aspects of the fission process. Recently, neutron-induced fission product-yield data of 239Pu at energies below 4 MeV revealed an unexpected energy dependence of certain fission fragments. In order to investigate whether this observation is prerogative to neutron-induced fission, a program has been initiated to measure fission product yields in photoinduced fission. Here we report on the first ever photofission product yield measurement with monoenergetic photons produced by Compton back-scattering of FEL photons. The experiment was performed at the High-Intensity Gamma-ray Source at Triangle Universities Nuclear Laboratory on 239Pu at Eγ=11 MeV. In this exploratory study the yield of eight fission products ranging from 91Sr to 143Ce has been obtained.

  18. Measurement of the 240Pu/239Pu mass ratio using a transition-edge-sensor microcalorimeter for total decay energy spectroscopy

    DOE PAGES

    Hoover, Andrew S.; Bond, Evelyn M.; Croce, Mark P.; ...

    2015-02-27

    In this study, we have developed a new category of sensor for measurement of the 240Pu/239Pu mass ratio from aqueous solution samples with advantages over existing methods. Aqueous solution plutonium samples were evaporated and encapsulated inside of a gold foil absorber, and a superconducting transition-edge-sensor microcalorimeter detector was used to measure the total reaction energy (Q-value) of nuclear decays via heat generated when the energy is thermalized. Since all of the decay energy is contained in the absorber, we measure a single spectral peak for each isotope, resulting in a simple spectral analysis problem with minimal peak overlap. We foundmore » that mechanical kneading of the absorber dramatically improves spectral quality by reducing the size of radioactive inclusions within the absorber to scales below 50 nm such that decay products primarily interact with atoms of the host material. Due to the low noise performance of the microcalorimeter detector, energy resolution values of 1 keV fwhm (full width at half-maximum) at 5.5 MeV have been achieved, an order of magnitude improvement over α-spectroscopy with conventional silicon detectors. We measured the 240Pu/239Pu mass ratio of two samples and confirmed the results by comparison to mass spectrometry values. These results have implications for future measurements of trace samples of nuclear material.« less

  19. The need for precise and well-documented experimental data on prompt fission neutron spectra from neutron-induced fission of 239Pu

    DOE PAGES

    Neudecker, Denise; Taddeucci, Terry Nicholas; Haight, Robert Cameron; ...

    2016-01-06

    The spectrum of neutrons emitted promptly after 239Pu(n,f)—a so-called prompt fission neutron spectrum (PFNS)—is a quantity of high interest, for instance, for reactor physics and global security. However, there are only few experimental data sets available that are suitable for evaluations. In addition, some of those data sets differ by more than their 1-σ uncertainty boundaries. We present the results of MCNP studies indicating that these differences are partly caused by underestimated multiple scattering contributions, over-corrected background, and inconsistent deconvolution methods. A detailed uncertainty quantification for suitable experimental data was undertaken including these effects, and test-evaluations were performed with themore » improved uncertainty information. The test-evaluations illustrate that the inadequately estimated effects and detailed uncertainty quantification have an impact on the evaluated PFNS and associated uncertainties as well as the neutron multiplicity of selected critical assemblies. A summary of data and documentation needs to improve the quality of the experimental database is provided based on the results of simulations and test-evaluations. Furthermore, given the possibly substantial distortion of the PFNS by multiple scattering and background effects, special care should be taken to reduce these effects in future measurements, e.g., by measuring the 239Pu PFNS as a ratio to either the 235U or 252Cf PFNS.« less

  20. A study of 239Pu production rate in a water cooled natural uranium blanket mock-up of a fusion-fission hybrid reactor

    NASA Astrophysics Data System (ADS)

    Feng, Song; Liu, Rong; Lu, Xinxin; Yang, Yiwei; Xu, Kun; Wang, Mei; Zhu, Tonghua; Jiang, Li; Qin, Jianguo; Jiang, Jieqiong; Han, Zijie; Lai, Caifeng; Wen, Zhongwei

    2016-03-01

    The 239Pu production rate is important data in neutronics design for a natural uranium blanket of a fusion-fission hybrid reactor, and the accuracy and reliability should be validated by integral experiments. The distribution of 239Pu production rates in a subcritical natural uranium blanket mock-up was obtained for the first time with a D-T neutron generator by using an activation technique. Natural uranium foils were placed in different spatial locations of the mock-up, the counts of 277.6 keV γ-rays emitted from 239Np generated by 238U capture reaction were measured by an HPGe γ spectrometer, and the self-absorption of natural uranium foils was corrected. The experiment was analyzed using the Super Monte Carlo neutron transport code SuperMC2.0 with recent nuclear data of 238U from the ENDF/B-VII.0, ENDF/B-VII.1, JENDL-4.0u2, JEFF-3.2 and CENDL-3.1 libraries. Calculation results with the JEFF-3.2 library agree with the experimental ones best, and they agree within the experimental uncertainty in general with the average ratios of calculation results to experimental results (C/E) in the range of 0.93 to 1.01.

  1. Measurement of the 240Pu/239Pu mass ratio using a transition-edge-sensor microcalorimeter for total decay energy spectroscopy.

    PubMed

    Hoover, Andrew S; Bond, Evelyn M; Croce, Mark P; Holesinger, Terry G; Kunde, Gerd J; Rabin, Michael W; Wolfsberg, Laura E; Bennett, Douglas A; Hays-Wehle, James P; Schmidt, Dan R; Swetz, Daniel; Ullom, Joel N

    2015-04-07

    We have developed a new category of sensor for measurement of the (240)Pu/(239)Pu mass ratio from aqueous solution samples with advantages over existing methods. Aqueous solution plutonium samples were evaporated and encapsulated inside of a gold foil absorber, and a superconducting transition-edge-sensor microcalorimeter detector was used to measure the total reaction energy (Q-value) of nuclear decays via heat generated when the energy is thermalized. Since all of the decay energy is contained in the absorber, we measure a single spectral peak for each isotope, resulting in a simple spectral analysis problem with minimal peak overlap. We found that mechanical kneading of the absorber dramatically improves spectral quality by reducing the size of radioactive inclusions within the absorber to scales below 50 nm such that decay products primarily interact with atoms of the host material. Due to the low noise performance of the microcalorimeter detector, energy resolution values of 1 keV fwhm (full width at half-maximum) at 5.5 MeV have been achieved, an order of magnitude improvement over α-spectroscopy with conventional silicon detectors. We measured the (240)Pu/(239)Pu mass ratio of two samples and confirmed the results by comparison to mass spectrometry values. These results have implications for future measurements of trace samples of nuclear material.

  2. Relative radiosensitivity of bone tumor induction among beagles as a function of age at injection of {sup 239}Pu or {sup 226}Ra

    SciTech Connect

    Lloyd, R.D.; Taylor, G.N.; Jee, W.S.S.; Miller, S.C.

    1999-01-01

    A comparison was made of the response to induction of skeletal malignancy from exposure of beagles to monomeric {sup 239}Pu or to {sup 226}Ra as juveniles (3 mo of age), young adults (1.5 y of age), or mature adults (5 y of age). This indicated that of these age groups, animals injected as young adults are most sensitive per Gy of average skeletal dose evaluated at 1 y before death. Dogs exposed either as juveniles or as mature adults appeared to be less sensitive. Relative radiosensitivities (RRS) of juvenile and mature beagles ranged between about 0.3 and 0.7 that of dogs injected as young adults. Mean values of RRS for both radionuclides were about 0.5, but RRS values derived from dogs given monomeric {sup 239}Pu appeared to be most reliable and were 0.27 {+-} 0.09 for dogs injected as juveniles and 0.41 {+-} 0.13 for animals exposed as mature adults.

  3. The Need for Precise and Well-documented Experimental Data on Prompt Fission Neutron Spectra from Neutron-induced Fission of {sup 239}Pu

    SciTech Connect

    Neudecker, D. Taddeucci, T.N.; Haight, R.C.; Lee, H.Y.; White, M.C.; Rising, M.E.

    2016-01-15

    The spectrum of neutrons emitted promptly after {sup 239}Pu(n,f)—a so-called prompt fission neutron spectrum (PFNS)—is a quantity of high interest, for instance, for reactor physics and global security. However, there are only few experimental data sets available that are suitable for evaluations. In addition, some of those data sets differ by more than their 1-σ uncertainty boundaries. We present the results of MCNP studies indicating that these differences are partly caused by underestimated multiple scattering contributions, over-corrected background, and inconsistent deconvolution methods. A detailed uncertainty quantification for suitable experimental data was undertaken including these effects, and test-evaluations were performed with the improved uncertainty information. The test-evaluations illustrate that the inadequately estimated effects and detailed uncertainty quantification have an impact on the evaluated PFNS and associated uncertainties as well as the neutron multiplicity of selected critical assemblies. A summary of data and documentation needs to improve the quality of the experimental database is provided based on the results of simulations and test-evaluations. Given the possibly substantial distortion of the PFNS by multiple scattering and background effects, special care should be taken to reduce these effects in future measurements, e.g., by measuring the {sup 239}Pu PFNS as a ratio to either the {sup 235}U or {sup 252}Cf PFNS.

  4. Chest wall thickness measurements: The alternative approach extended for {sup 241}Am

    SciTech Connect

    Kramer, G.H.; Burns, L.C.

    1997-02-01

    The Human Monitoring Laboratory has extended the technique of determining the chest wall thickness of an individual using information from the spectrum produced by internally deposited radionuclides. The technique has been investigated both theoretically and practically using germanium detectors and the Lawrence Livermore Torso Phantom. The phantom was used with a lung set containing homogeneously distributed {sup 241}Am. Chest wall thicknesses were varied by using a series of muscle equivalent overlay plates that gave a range of 1.6 cm to 3.9 cm thickness. It was found that a 3-cm chest wall thickness can be estimated to within 18%. Using a spectral addition technique 1 kBq was estimated to be the {open_quotes}practical{close_quotes} lower limit of activity for this method. 7 refs., 2 figs., 3 tabs.

  5. Deterministic effects of {sup 241}Am exposure in the Hanford americium accident case

    SciTech Connect

    Filipy, R.E.; Toohey, R.E.; Kathren, R.L.; Dietert, S.E.

    1995-09-01

    Lifetime follow-up of USTUR Case 246 demonstrated the lack of severe biological effects resulting from his exposure to {sup 241}Am. Deterministic effects observed were limited to hematological changes, including lymphopenia and thrombocytopenia. These hematological changes were consistent with those observed in experimental animals following actinide exposure. Cataracts were removed from the left and right eyes at 547, and 1,030 d after the accident, respectively, but were considered to be trauma-induced rather than radiation-induced. No abnormal findings were reported from gross of histological examinations of tissue samples removed at autopsy, other than those resulting from the subject`s pre-existing cardiovascular disease. 30 refs., 7 figs., 1 tab.

  6. Determination of 239Pu and 240Pu isotope ratio for a nuclear bomb particle using X-ray spectrometry in conjunction with γ-ray spectrometry and non-destructive α-particle spectrometry

    NASA Astrophysics Data System (ADS)

    Pöllänen, R.; Ruotsalainen, K.; Toivonen, H.

    2009-11-01

    A nuclear bomb particle from Thule containing Pu and U was analyzed using X-ray spectrometry in combination with γ-ray spectrometry and non-destructive α-spectrometry. The main objective was to investigate the possibility to determine the 239Pu and 240Pu isotope ratios. Previously, X-ray spectrometry together with the above-mentioned methods has been successfully applied for radiochemically processed samples, but not for individual particles. In the present paper we demonstrate the power of non-destructive analysis. The 239Pu/( 239Pu+ 240Pu) atom ratio for the Thule particle was determined, using two different approaches, to be 0.93±0.07 and 0.91±0.05. These results are consistent with weapons-grade material and the results obtained by other investigators.

  7. Determination of 240Pu/239Pu isotopic ratios in human tissues collected from areas around the Semipalatinsk Nuclear Test Site by sector-field high resolution ICP-MS.

    PubMed

    Yamamoto, M; Oikawa, S; Sakaguchi, A; Tomita, J; Hoshi, M; Apsalikov, K N

    2008-09-01

    Information on the 240Pu/239Pu isotope ratios in human tissues for people living around the Semipalatinsk Nuclear Test Site (SNTS) was deduced from 9 sets of soft tissues and bones, and 23 other bone samples obtained by autopsy. Plutonium was radiochemically separated and purified, and plutonium isotopes (239Pu and 240Pu) were determined by sector-field high resolution inductively coupled plasma-mass spectrometry. For most of the tissue samples from the former nine subjects, low 240Pu/239Pu isotope ratios were determined: bone, 0.125 +/- 0.018 (0.113-0.145, n = 4); lungs, 0.063 +/- 0.010 (0.051-0.078, n = 5); and liver, 0.148 +/- 0.026 (0.104-0.189, n = 9). Only 239Pu was detected in the kidney samples; the amount of 240Pu was too small to be measured, probably due to the small size of samples analyzed. The mean 240Pu/239Pu isotope ratio for bone samples from the latter 23 subjects was 0.152 +/- 0.034, ranging from 0.088 to 0.207. A significant difference (a two-tailed Student's t test; 95% significant level, alpha = 0.05) between mean 240Pu/239Pu isotope ratios for the tissue samples and for the global fallout value (0.178 +/- 0.014) indicated that weapons-grade plutonium from the atomic bombs has been incorporated into the human tissues, especially lungs, in the residents living around the SNTS. The present 239,240Pu concentrations in bone, lung, and liver samples were, however, not much different from ranges found for human tissues from other countries that were due solely to global fallout during the 1970's-1980's.

  8. Upper concentration limits for {sup 239}Pu traces in some {open_quotes}KTB{close_quotes}-samples and in one Hawaiian lava

    SciTech Connect

    Barth, H.; Ganz, M.; Brandt, R.

    1994-11-01

    Trace quantities of plutonium are observed in the environment all over the world, and include both man-made {sup 238-242}Pu and natural {sup 239}Pu in uranium ores. Typical concentrations range from 10{sup {minus}14} g Pu/g sample up to 10{sup {minus}12} g Pu/g in pitchblende. We have determined some upper concentration limits for the plutonium in samples from KTB (Kontinentales Tiefbohrprogramm, Germany) which are in the range of 10{sup {minus}15} down to 3{center_dot}10{sup {minus}17} g Pu/g sample. In addition, we have investigated one sample of Hawaiian lava, with a limit of 5{center_dot}10{sup {minus}15}. We could not confirm previous reports on the observation of plutonium in some Pacific Lavas, nor do our results show any evidence for cold fusion neutrons producing plutonium in fluids of great depth in the crust.

  9. Estimating Reaction Cross Sections from Measured (Gamma)-Ray Yields: The 238U(n,2n) and 239Pu(n,2n) Cross Sections

    SciTech Connect

    Younes, W

    2002-11-18

    A procedure is presented to deduce the reaction-channel cross section from measured partial {gamma}-ray cross sections. In its simplest form, the procedure consists in adding complementary measured and calculated contributions to produce the channel cross section. A matrix formalism is introduced to provide a rigorous framework for this approach. The formalism is illustrated using a fictitious product nucleus with a simple level scheme, and a general algorithm is presented to process any level scheme. In order to circumvent the cumbersome algebra that can arise in the matrix formalism, a more intuitive graphical procedure is introduced to obtain the same reaction cross-section estimate. The features and limitations of the method are discussed, and the technique is applied to extract the {sup 235}U (n,2n) and {sup 239}Pu(n,2n) cross sections from experimental partial {gamma}-ray cross sections, coupled with (enhanced) Hauser-Feshbach calculations.

  10. Integration of measurements with atmospheric dispersion models: Source term estimation for dispersal of (239)Pu due to non-nuclear detonation of high explosive

    NASA Astrophysics Data System (ADS)

    Edwards, L. L.; Harvey, T. F.; Freis, R. P.; Pitovranov, S. E.; Chernokozhin, E. V.

    1992-10-01

    The accuracy associated with assessing the environmental consequences of an accidental release of radioactivity is highly dependent on our knowledge of the source term characteristics and, in the case when the radioactivity is condensed on particles, the particle size distribution, all of which are generally poorly known. This paper reports on the development of a numerical technique that integrates the radiological measurements with atmospheric dispersion modeling. This results in a more accurate particle-size distribution and particle injection height estimation when compared with measurements of high explosive dispersal of (239)Pu. The estimation model is based on a non-linear least squares regression scheme coupled with the ARAC three-dimensional atmospheric dispersion models. The viability of the approach is evaluated by estimation of ADPIC model input parameters such as the ADPIC particle size mean aerodynamic diameter, the geometric standard deviation, and largest size. Additionally we estimate an optimal 'coupling coefficient' between the particles and an explosive cloud rise model. The experimental data are taken from the Clean Slate 1 field experiment conducted during 1963 at the Tonopah Test Range in Nevada. The regression technique optimizes the agreement between the measured and model predicted concentrations of (239)Pu by varying the model input parameters within their respective ranges of uncertainties. The technique generally estimated the measured concentrations within a factor of 1.5, with the worst estimate being within a factor of 5, very good in view of the complexity of the concentration measurements, the uncertainties associated with the meteorological data, and the limitations of the models. The best fit also suggest a smaller mean diameter and a smaller geometric standard deviation on the particle size as well as a slightly weaker particle to cloud coupling than previously reported.

  11. Alveolar macrophage kinetics after inhalation of 239PuO2 by CBA/Ca mice: changes in synthesis of DNA.

    PubMed Central

    Kellington, J P; Gibson, K; Buckle, T M; Talbot, R J; Hornby, S B

    1992-01-01

    For workers in the nuclear industry, the primary route for the entry of radioactive materials into the body is by inhalation, and the rate of clearance of particles from the pulmonary region of the lung is an important factor in determining radiation dose. It is the function of alveolar macrophages (AM) to maintain the sterility of the lung and to remove insoluble particles from the respiratory surfaces and airways. The AM population is not static, and under normal conditions the loss of macrophages from the alveoli via the conducting airways is balanced by renewal. Studies of the effects of external irradiation on the kinetics of AM are numerous, but to date little is known about the effects of inhaled radioactive particles. In this investigation the effects of inhaled 239PuO2 (plutonium dioxide) particles on the synthesis of DNA by AM were studied at times up to 77 days after exposure. We also measured the number of cells recovered by bronchoalveolar lavage and the incidence of AM with nuclear aberrations. The latter provides a sensitive indicator of the effects of radiation. One of the earliest effects observed after exposure to 239PuO2 is a reduction in the number of AM recovered by lavage. This reduction is associated with a 3-fold reduction in the proportion of AM undergoing DNA synthesis at early times after exposure. The overall mean pulse labeling index of AM recovered from sham-exposed mice is 1.68%, and no trend is observed with time.(ABSTRACT TRUNCATED AT 250 WORDS) PMID:1396470

  12. 241Am migration in a sandy aquifer studied by long-term column experiments.

    PubMed

    Artinger, Robert; Schuessler, Wolfram; Scherbaum, Franz; Schild, Dieter; Kim, Jae-Il

    2002-11-15

    The migration behavior of 241Am(III) in a sandy aquifer was studied under near-natural conditions by long-term column experiments of more than 1 year duration. Columns with 50 cm length and 5 cm in diameter were packed with aeolian quartz sand and equilibrated with two different groundwaters having an original dissolved organic carbon concentration (DOC) of 1.1 and 7.2 mg x dm(-3), respectively,from the Gorleben site (Lower Saxony, Germany). In each experiment, 1 cm3 of Am-spiked groundwater ([Am] = 0.2 to 2 micromol x dm(-3)) was injected into the column. The flow rate of the groundwater was adjusted to 0.28 m x d(-1). A small colloid-borne Am fraction was found to elute together with tritiated water. After 414 and 559 days, respectively, the experiments were terminated. Whereas the nonsorbing tracer of tritiated water would have covered a distance of about 350 m in that time period, the maximum of the Am activity was detected between 32 and 40 mm column length. Applying selective dissolution analysis to the sand surface, Am was found to be preferentially bound to iron hydroxide/oxide sites. From this Am distribution, a retardation factor R of about 10(4) was determined and compared to static batch experiments. The Am breakthrough was calculated forthe conditions of the column experiment

  13. [Experimental study of 241Am transfer from herbal food to organs and tissues of crucian carp].

    PubMed

    Zotina, T A; Trofimova, E A; Dement'ev, D V; Bolsunovskiĭ, A Ia

    2011-01-01

    Freshwater fishes (Carassius auratus gibelio, crucian carp) were fed through catheter with homogenized biomass of submerged macrophytes labeled with transuranium element 241Am. The intensity of excretion of americium and its accumulation in organs and tissues of fishes were investigated. The highest release of americium (up to 70%) was recorded on the second day after feeding. 94-98% of americium were excreted during 3-4 days; however, americium was also recorded in the excrements after 11 days. Americium was registered in organs and tissues of fishes, including those tissues that had no direct contact with americium (bones and muscles). This implies assimilation of americium via digestive tract. The activity concentration of americium in bones (11 Bq/kg, fresh mass) was twice as high as that in muscles, heads and external tissues and organs (skin, scales and fins). The highest activity concentration of americium was registered in viscera (33 Bq/kg, 48% of the total activity in the body). Accumulation of americium in muscles enhances the probability of the further transfer of americium along a food chain.

  14. Measurement of the {sup 241}Am(n,2n) reaction cross section using the activation method

    SciTech Connect

    Perdikakis, G.; Papadopoulos, C.T.; Vlastou, R.; Kokkoris, M.; Galanopoulos, S.; Patronis, N.; Lagoyannis, A.; Spyrou, A.; Zarkadas, Ch.; Kalyva, G.; Kossionides, S.; Karamanis, D.

    2006-06-15

    In the context of the n{sub T}OF Collaboration, the measurement of the cross section of the reaction {sup 241}Am(n,2n){sup 240}Am, has been performed, for the first time at neutron energies from 8.8 to 11.4 MeV, by the activation method, relative to the {sup 27}Al(n,a){sup 24}Na reaction reference cross section. The monoenergetic neutron beam was produced at the 5.5 MV TANDEM accelerator of NCSR ''Demokritos,'' by means of the {sup 2}H(d,n){sup 3}He reaction, using a deuterium filled gas cell. The radioactive target consisted of a 37 GBq {sup 241}Am source enclosed in a Pb container. After the end of the irradiation, the activity induced by the neutron beam at the target and reference, was measured off-line by a 56% relative efficiency, HPGe detector.

  15. Investigation of the radiation risk due to environmental contamination by 241Am from lightning rods disposed at uncontrolled garbage dumps.

    PubMed

    Marumo, Júlio T; Isiki, Vera L K; Miyamoto, Hissae; Ferreira, Rafael V P; Bellini, Maria H; de Lima, Luis F C P

    2008-02-01

    Radioactive lightning rods were manufactured in Brazil until 1989, when the licenses for using radioactive sources in these products were lifted by the national nuclear authority. Since then, these rods have been replaced by the Franklin type and collected as radioactive waste. However, only 20% of the estimated total number of installed rods has been delivered to the Brazilian Nuclear Commission. This situation causes concern, since there is the possibility of the rods to be disposed as domestic waste. In Brazil, 64% of the municipal solid waste is disposed at garbage dumps without sufficient control. In addition, (241)Am, the radionuclide most commonly employed, is classified as a high-toxicity element, when incorporated. In the present study, (241)Am migration experiments were performed by means of a lysimeter system, in order to evaluate the risk of contamination caused by radioactive lightning rods disposed as common solid waste. (241)Am sources removed from lightning rods were placed inside lysimeters filled with organic waste that was collected at the restaurant of the Instituto de Pesquisas Energéticas e Nucleares. The generated leachate was periodically analyzed, and characteristics such as pH, redox potential, solid content and the concentration of the radioactive material were determined. The equivalent dose for members of the public was calculated considering ingestion of contaminated drinking water as the major path of exposure. Estimated doses were about 20-times below the effective dose limit of 1 mSv year(-1) for members of the public as recommended by the International Commission on Radiological Protection. This suggests the radiation risk caused by lightning rods disposed at uncontrolled garbage dumps to be low. It should be noted, however, that the number of investigated lightning rods was quite small. The results of this study might therefore not be entirely representative and should be interpreted with care. They provide, however, a very first

  16. Recoil-α-fission and recoil-α-α-fission events observed in the reaction 48Ca + 243Am

    NASA Astrophysics Data System (ADS)

    Forsberg, U.; Rudolph, D.; Andersson, L.-L.; Di Nitto, A.; Düllmann, Ch. E.; Fahlander, C.; Gates, J. M.; Golubev, P.; Gregorich, K. E.; Gross, C. J.; Herzberg, R.-D.; Heßberger, F. P.; Khuyagbaatar, J.; Kratz, J. V.; Rykaczewski, K.; Sarmiento, L. G.; Schädel, M.; Yakushev, A.; Åberg, S.; Ackermann, D.; Block, M.; Brand, H.; Carlsson, B. G.; Cox, D.; Derkx, X.; Dobaczewski, J.; Eberhardt, K.; Even, J.; Gerl, J.; Jäger, E.; Kindler, B.; Krier, J.; Kojouharov, I.; Kurz, N.; Lommel, B.; Mistry, A.; Mokry, C.; Nazarewicz, W.; Nitsche, H.; Omtvedt, J. P.; Papadakis, P.; Ragnarsson, I.; Runke, J.; Schaffner, H.; Schausten, B.; Shi, Yue; Thörle-Pospiech, P.; Torres, T.; Traut, T.; Trautmann, N.; Türler, A.; Ward, A.; Ward, D. E.; Wiehl, N.

    2016-09-01

    Products of the fusion-evaporation reaction 48Ca + 243Am were studied with the TASISpec set-up at the gas-filled separator TASCA at the GSI Helmholtzzentrum für Schwerionenforschung, Darmstadt, Germany. Amongst the detected thirty correlated α-decay chains associated with the production of element Z = 115, two recoil-α-fission and five recoil- α- α-fission events were observed. The latter five chains are similar to four such events reported from experiments performed at the Dubna gas-filled separator, and three such events reported from an experiment at the Berkeley gas-filled separator. The four chains observed at the Dubna gas-filled separator were assigned to start from the 2n-evaporation channel 289115 due to the fact that these recoil- α- α-fission events were observed only at low excitation energies. Contrary to this interpretation, we suggest that some of these recoil- α- α-fission decay chains, as well as some of the recoil- α- α-fission and recoil-α-fission decay chains reported from Berkeley and in this article, start from the 3n-evaporation channel 288115.

  17. Results of the Excreta Bioassay Quality Control Program for April 1, 2009 through March 31, 2010

    SciTech Connect

    Antonio, Cheryl L.

    2012-07-19

    A total of 58 urine samples and 10 fecal samples were submitted during the report period (April 1, 2009 through March 31, 2010) to General Engineering Laboratories, South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for Sr, 238Pu, 239Pu, 241Am, 243Am 235U, 238U, elemental uranium and fecal analyses for 241Am, 238Pu and 239Pu were tested this year as well as four tissue samples for 238Pu, 239Pu, 241Am and 241Pu. The number of QC urine samples submitted during the report period represented 1.3% of the total samples submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 33% of the analyses processed by GEL during the third year of this contract were quality control samples. GEL tested the performance of 21 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty (Table 4).

  18. Influence of self-absorption corrections in the quantification of 210Pb and 241Am for sediment dating

    NASA Astrophysics Data System (ADS)

    González, J. Carrazana; Vargas, M. Jurado; Castillo, R. Gil

    2016-10-01

    The nuclides 210Pb and 241Am are used in geochronological studies. In this work, we examine the influence of the sediment chemical composition on the self-attenuation corrections needed for the accurate determination of specific activities for 210Pb and 241Am used for sediment dating. A theoretical exercise was carried out evaluating the relative bias obtained by four different analytical laboratories in the quantification of the 210Pb and 241Am activity concentration by gamma-ray spectrometry. The laboratories considered the same density for the sediment sample, but each one used a different chemical composition in the Monte Carlo calculations, and six different HPGe detectors (including n and p-types). An estimate of the impact that would have the relative biases found in the estimation of the 210Pb sediment ages, applying the Constant Rate of Supply (CRS) dating model, is also given. In addition, the performance scores that the laboratories would have obtained in a hypothetical IAEA proficiency test are also presented.

  19. Development of the MICROMEGAS detector for measuring the energy spectrum of alpha particles by using a 241Am source

    NASA Astrophysics Data System (ADS)

    Kim, Do Yoon; Ham, Cheolmin; Shin, Jae Won; Park, Tae-Sun; Hong, Seung-Woo; Andriamonje, Samuel; Kadi, Yacine; Tenreiro, Claudio

    2016-05-01

    We have developed MICROMEGAS (MICRO MEsh GASeous) detectors for detecting a particles emitted from an 241Am standard source. The voltage applied to the ionization region of the detector is optimized for stable operation at room temperature and atmospheric pressure. The energy of a particles from the 241Am source can be varied by changing the flight path of the a particle from the 241Am source. The channel numbers of the experimentally-measured pulse peak positions for different energies of the a particles are associated with the energies deposited by the alpha particles in the ionization region of the detector as calculated by using GEANT4 simulations; thus, the energy calibration of the MICROMEGAS detector for a particles is done. For the energy calibration, the thickness of the ionization region is adjusted so that a particles may completely stop in the ionization region and their kinetic energies are fully deposited in the region. The efficiency of our MICROMEGAS detector for a particles under the present conditions is found to be ~97.3%.

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

    SciTech Connect

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

    1982-01-01

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

  1. Microdistribution and long-term retention of 239Pu (NO3)4 in the respiratory tracts of an acutely exposed plutonium worker and experimental beagle dogs.

    PubMed

    Nielsen, Christopher E; Wilson, Dulaney A; Brooks, Antone L; McCord, Stacey L; Dagle, Gerald E; James, Anthony C; Tolmachev, Sergei Y; Thrall, Brian D; Morgan, William F

    2012-11-01

    The long-term retention of inhaled soluble forms of plutonium raises concerns as to the potential health effects in persons working in nuclear energy or the nuclear weapons program. The distributions of long-term retained inhaled plutonium-nitrate [(239)Pu (NO(3))(4)] deposited in the lungs of an accidentally exposed nuclear worker (Human Case 0269) and in the lungs of experimentally exposed beagle dogs with varying initial lung depositions were determined via autoradiographs of selected histologic lung, lymph node, trachea, and nasal turbinate tissue sections. These studies showed that both the human and dogs had a nonuniform distribution of plutonium throughout the lung tissue. Fibrotic scar tissue effectively encapsulated a portion of the plutonium and prevented its clearance from the body or translocation to other tissues and diminished dose to organ parenchyma. Alpha radiation activity from deposited plutonium in Human Case 0269 was observed primarily along the subpleural regions while no alpha activity was seen in the tracheobronchial lymph nodes of this individual. However, relatively high activity levels in the tracheobronchial lymph nodes of the beagles indicated the lymphatic system was effective in clearing deposited plutonium from the lung tissues. In both the human case and beagle dogs, the appearance of retained plutonium within the respiratory tract was inconsistent with current biokinetic models of clearance for soluble forms of plutonium. Bound plutonium can have a marked effect on the dose to the lungs and subsequent radiation exposure has the potential to increase cancer risk.

  2. Determination of the 240Pu/ 239Pu atomic ratio in soils from Palomares (Spain) by low-energy accelerator mass spectrometry

    NASA Astrophysics Data System (ADS)

    Chamizo, E.; García-León, M.; Synal, H.-A.; Suter, M.; Wacker, L.

    2006-08-01

    In 1966, the nuclear fuel of two thermonuclear bombs was released over the Spanish region of Palomares, due to a B52 bomber accident during a refuelling operation. Since then, much effort has been made to assess its impact to the different environmental compartments of this area in South-East Spain, mostly by measuring the 239+240Pu activity concentration and the 238Pu/239+240Pu activity ratio. Nevertheless, these measurements do not give enough information on the problem. In order to recognize unambiguously small traces of the weapon-grade plutonium released in the accident, the ratio of the two major isotopes of plutonium, 240Pu/239Pu, has to be determined. In this work, this ratio has been measured in low- and high-activity samples from Palomares by means of low-energy accelerator mass spectrometry (AMS). That way, we will show the potential of the new generation of compact AMS facilities in terms of plutonium characterization at ultra-trace levels.

  3. Inhaled /sup 239/PuO/sub 2/ and/or total-body gamma radiation: Early mortality and morbidity in rats and dogs

    SciTech Connect

    Filipy, R.E.; Decker, J.R.; Lai, Y.L.; Lauhala, K.E.; Buschbom, R.L.; Hiastala, M.P.; McGee, D.R.; Park, J.F.; Kuffel, E.G.; Ragan, H.A.; Cannon, W.C.; Yaniv, S.S.; Scott, B.R.

    1988-08-01

    Rats and beagle dogs were given doses of /sup 60/Co gamma radiation and/or body burdens of /sup 239/PuO/sub 2/ within lethal ranges in an experiment to determine and compare morbidity and mortality responses of both species within 1 year after exposure. Radiation-induced morbidity was assessed by measuring changes in body weights, hematologic parameters, and pulmonary-function parameters. Gamma radiation caused transient morbidity, reflected by immediately depressed blood cell concentrations and by long-term loss of body weight and diminished pulmonary function in animals of both species that survived the acute gamma radiation syndrome. Inhaled plutonium caused a loss of body weight and diminished pulmonary function in both species, but its only effect on blood cell concentrations was lymphocytopenia in dogs. Combined gamma irradiation and plutonium lung burdens were synergistic, in that animals receiving both radiation insults had higher morbidity and mortality rates than would be predicted based on the effect of either kind of radiation alone. Plutonium lung burdens enhanced the effect of gamma radiation in rats within the first 30 days of exposure, and gamma radiation enhanced the long-term effect of plutonium lung burdens in both species. Rats were less sensitive to both kinds of radiation, whether administered alone or in combination. 71 refs., 105 figs., 48 tabs.

  4. Comparative effects of protracted exposures to 60Co gamma-radiation and 239Pu alpha-radiation on breeding performance in female mice..

    PubMed

    Searle, A G; Beechey, C V; Green, D; Howells, G R

    1980-02-01

    Breeding performances are compared of hybrid female mice given 239Pu (5 or 10 mu Cikg-1 body mass in 1% trisodium citrate via the tail-vein), or kept in a 10 rad/day or 20 rad/day 60Co gamma-irradiation field (but mated in the control area), or unirradiated. Ovarian dose-rates from the injected plutonium were initially 0.8 and 1.7 rad/day, changing little thereafter; actual gamma-ray dose-rates to breeding females averaged around 8 and 16 rad/day respectively. Both gamma-ray treatments affected reproductive performance more than the plutonium injections, with respet to duration of fertility and to offspring per litter in successive 4-weekly periods, though overall mean litter-sizes were not significantly less than controls. The r.b.e. for these effects on reproduction, attributed to germ-cell killing, is about 2.5 for the alpha-particles vs. gamma-rays, lower than for testis mass reduction in males. This low r.b.e. may be connected with inhomogeneity of alpha-particle dose within the ovary, but it is known that fission neutron versus gamma r.b.e.'s for impairment of female fertility are also lower than those for impairment of male fertility.

  5. Microdistribution and Long-Term Retention of 239Pu (NO3)4 in the Respiratory Tracts of an Acutely Exposed Plutonium Worker and Experimental Beagle Dogs

    SciTech Connect

    Nielsen, Christopher E.; Wilson, Dulaney A.; Brooks, Antone L.; McCord, Stacey; Dagle, Gerald E.; James, Anthony C.; Tolmachev, Sergei Y.; Thrall, Brian D.; Morgan, William F.

    2012-11-01

    The long-term retention of inhaled soluble forms of plutonium raises concerns as to the potential health effects in persons working in nuclear energy or the nuclear weapons program. The distributions of long-term retained inhaled plutonium-nitrate [239Pu (NO3)4] deposited in the lungs of an accidentally exposed nuclear worker (Human Case 0269) and in the lungs of experimentally exposed beagle dogs with varying initial lung depositions were determined via autoradiographs of selected histological lung, lymph node, trachea, and nasal turbinate tissue sections. These studies showed that both the human and dogs had a non-uniform distribution of plutonium throughout the lung tissue. Fibrotic scar tissue effectively encapsulated a portion of the plutonium and prevented its clearance from the body or translocation to other tissues and diminished dose to organ parenchyma. Alpha radiation activity from deposited plutonium in Human Case 0269 was observed primarily along the sub-pleural regions while no alpha activity was seen in the tracheobronchial lymph nodes of this individual. However, relatively high activity levels in the tracheobronchial lymph nodes of the beagles indicated the lymphatic system was effective in clearing deposited plutonium from the lung tissues. In both the human case and beagle dogs, the appearance of retained plutonium within the respiratory tract was inconsistent with current biokinetic models of clearance for soluble forms of plutonium. Bound plutonium can have a marked effect on the dose to the lungs and subsequent radiation exposure has the potential increase in cancer risk.

  6. The Association of Inbreeding With Lung Fibrosis Incidence in Beagle Dogs That Inhaled 238PuO2 or 239PuO2.

    SciTech Connect

    Wilson, Dulaney A.; Brigantic, Andrea M.; Morgan, William F.

    2011-09-12

    Studies of health effects in animals after exposure to internally deposited radionuclides were intended to supplement observational studies in humans. Both nuclear workers and Beagle dogs have exhibited plutonium associated lung fibrosis; however, the dogs smaller gene pool may limit the applicability of findings to humans. Data on Beagles that inhaled either plutonium-238 dioxide (238PuO2) or plutonium-239 dioxide (239PuO2) were analyzed. Wright's Coefficient of Inbreeding was used to measure genetic or familial susceptibility and was assessed as an explanatory variable when modeling the association between lung fibrosis incidence and plutonium exposure. Lung fibrosis was diagnosed in approximately 80% of the exposed dogs compared with 23.7% of the control dogs. The maximum degree of inbreeding was 9.4%. Regardless of isotope, the addition of inbreeding significantly improved the model in female dogs but not in males. In female dogs an increased inbreeding coefficient predicted decreased hazard of a lung fibrosis diagnosis. Lung fibrosis was common in these dogs with inbreeding affecting models of lung fibrosis incidence in females but not in males. The apparent protective effect in females predicted by these models of lung fibrosis incidence is likely to be minimal given the small degree of inbreeding in these groups.

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

    NASA Astrophysics Data System (ADS)

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

    2014-09-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2008-01-01

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

  9. Au Lα x-rays induced by photons from 241Am: Comparison of experimental results and the predictions of PENELOPE.

    PubMed

    Gonzales, D; Requena, S; Williams, S

    2012-01-01

    The results of experiments performed, measuring the Lα x-rays emitted by Au due to excitation by photons of various energies from an (241)Am sample at forward-scattered angles in the range 0° to 65°, are compared to the predictions of the Monte Carlo code, PENELOPE. The experimental data are in good agreement with the predictions of the program. A comparison of the angular distributions of the probability densities (as predicted by the program) related to the Au Lα and Lβ x-rays suggests that PENELOPE does not simulate the phenomena described by Flügge et al. (1972).

  10. An attempt to decrease anisotropic emissions of neutrons from a cylindrical 241Am-Be-encapsulation source.

    PubMed

    Kowatari, M; Tanimura, Y; Yoshizawa, M

    2014-10-01

    An attempt to decrease the anisotropic emissions of neutrons from a cylindrical (241)Am-Be-encapsulated X3 source was conducted with Monte Carlo calculations and experiments. The influence of metal materials and shapes of the external casing to the anisotropy factor were focussed on. Results obtained by calculations using MCNP4C implied that a light and spherical-shaped external casing decreases the anisotropic emission of neutrons. Experimental results using the spherical-shaped aluminium protection case also revealed that the anisotropy factor was close to 1.0 with wide zenith angle ranges.

  11. Ultra-trace determination of (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu by triple quadruple collision/reaction cell-ICP-MS/MS: Establishing a baseline for global fallout in Qatar soil and sediments.

    PubMed

    Amr, Mohamed A; Helal, Abdul-Fattah I; Al-Kinani, Athab T; Balakrishnan, Perumal

    2016-03-01

    The development of practical, fast, and reliable methods for the ultra-trace determination of anthropogenic radionuclides (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu by triple quadruple collision/reaction cell inductively coupled plasma mass spectrometry (CRC-ICP-MS/MS) were investigated in term of its accuracy and precision for producing reliable results. The radionuclides were extracted from 1 kg of the environmental soil samples by concentrated nitric and hydrochloric acids. The leachate solutions were measured directly by triple quadrupole CRC-ICP-MS/MS. For quality assurance, a chemical separation of the concerned radionuclides was conducted and then measured by single quadrupole-ICP-MS. The developed methods were next applied to measure the anthropogenic radionuclides (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu in soil samples collected throughout the State of Qatar. The average concentrations of (90)Sr, (137)Cs, (238)Pu, (239)Pu, and (240)Pu were 0.606 fg/g (3.364 Bq/kg), 0.619 fg/g (2.038 Bq/kg), 0.034 fg/g (0.0195 Bq/kg), 65.59 fg/g (0.150 Bq/kg), and 12.06 fg/g (0.103 Bq/kg), respectively.

  12. Orally Administered DTPA Di-ethyl Ester for Decorporation of 241Am in dogs: Assessment of Safety and Efficacy in an Inhalation-Contamination Model

    PubMed Central

    Huckle, James E.; Sadgrove, Matthew P.; Pacyniak, Erik; Leed, Marina G. D.; Weber, Waylon M.; Doyle-Eisele, Melanie; Guilmette, Raymond A.; Agha, Bushra J.; Susick, Robert L.; Mumper, Russell J.; Jay, Michael

    2016-01-01

    Purpose Currently two injectable products of diethylenetriaminepentaacetic acid (DTPA) are U.S. Food and Drug Administration (FDA) approved for decorporation of 241Am, however, an oral product is considered more amenable in a mass casualty situation. The diethyl ester of DTPA, named C2E2, is being developed as an oral drug for treatment of internal radionuclide contamination. Materials and methods Single dose decorporation efficacy of C2E2 administered 24-hours post contamination was determined in beagle dogs using a 241Am nitrate inhalation contamination model. Single and multiple dose toxicity studies in beagle dogs were performed as part of an initial safety assessment program. In addition, the genotoxic potential of C2E2 was evaluated by the in vitro bacterial reverse mutation Ames test, mammalian cell chromosome aberration cytogenetic assay and an in vivo micronucleus test. Results Oral administration of C2E2 significantly increased 241Am elimination over untreated controls and significantly reduced the retention of 241Am in tissues, especially liver, kidney, lung and bone. Daily dosing of 200 mg/kg/day for 10 days was well tolerated in dogs. C2E2 was found to be neither mutagenic or clastogenic. Conclusions The di-ethyl ester of DTPA (C2E2) was shown to effectively enhance the elimination of 241Am after oral administration in a dog inhalation-contamination model and was well tolerated in toxicity studies. PMID:25912343

  13. The U.S. Transuranium Registry report of the 241Am content of a whole body. Part IV: Preparation and analysis of the tissues and bones.

    PubMed

    McInroy, J F; Boyd, H A; Eutsler, B C; Romero, D

    1985-10-01

    Los Alamos National Laboratory has analyzed autopsy tissue for the USTR, as a part of its study of the uptake, distribution and retention of Pu and other transuranic elements in occupationally exposed workers since 1978. In April 1979, Los Alamos received the internal organs and bone samples from the first whole-body donation to the USTR. The donor was known to have an internal deposition of 241Am. All soft tissue, the bones from the right half of the skeleton, and the odd-numbered vertebrae were received at Los Alamos in February 1980. The bones were subdivided along anatomical areas of interest. All soft tissues and bone specimens were analyzed for their 241Am content. A total deposition of 147.4 nCi 241Am was measured. Approximately 18% of the 241Am remaining in the body (disregarding that in the left hand), was found in the soft tissues, and 82% was in the bones and teeth. The soft tissues and organs containing the largest amounts of 241Am were the combined soft tissue (striated muscle, connective tissue and skin) 8.8%; liver, 6.4% and respiratory tract, 1.5%. The remaining organs accounted for 0.9% of the systemic burden.

  14. A MCNP-based calibration method and a voxel phantom for in vivo monitoring of 241Am in skull

    NASA Astrophysics Data System (ADS)

    Moraleda, M.; Gómez-Ros, J. M.; López, M. A.; Navarro, T.; Navarro, J. F.

    2004-07-01

    Whole body counter (WBC) facilities are currently used for assessment of internal radionuclide body burdens by directly measuring the radiation emitted from the body. Previous calibration of the detection devices requires the use of specific anthropomorphic phantoms. This paper describes the MCNP-based Monte Carlo technique developed for calibration of the germanium detectors (Canberra LE Ge) used in the CIEMAT WBC for in vivo measurements of 241Am in skull. The proposed method can also be applied for in vivo counting of different radionuclides distributed in other anatomical regions as well as for other detectors. A computer software was developed to automatically generate the input files for the MCNP code starting from any segmented human anatomy data. A specific model of a human head for the assessment of 241Am was built based on the tomographic phantom VOXELMAN of Yale University. The germanium detectors were carefully modelled from data provided by the manufacturer. This numerical technique has been applied to investigate the best counting geometry and the uncertainty due to improper positioning of the detectors.

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

    SciTech Connect

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

    1991-01-01

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

  16. Current Inconsistencies in {sup 238}Pu, {sup 241,243}Am and {sup 242}Cm Evaluations and their Impact on Uncertainties

    SciTech Connect

    Maslov, V.M.

    2008-12-15

    Improvements in the nuclear reaction modeling and nuclear parameter systematics, consistent with the description of neutron data on major actinides {sup 232}Th, {sup 233}U, {sup 235}U, {sup 238}U and {sup 239}Pu will be shown to provide a sound basis for critical assessment of the fission, capture, inelastic scattering, and (n,xn) reaction cross sections on minor actinides. This will largely help to avoid substituting possible model deficiencies by enlarging parameter uncertainties in the conventional nuclear models. In a number of minor actinides, the uncertainty estimation of cross sections and prompt fission neutron spectra would require complete re-evaluation of basic data. Otherwise, extremely large cross section uncertainty estimates will have to be adopted, especially in the case of poorly investigated Np, Pu, Am, Cm targets.

  17. Long-term {alpha}- and spontaneous fission measurement of a Rf/Db sample chemically prepared in a {sup 48}Ca on {sup 243}Am experiment

    SciTech Connect

    Dressler, Rugard; Eichler, Robert; Schumann, Dorothea; Shishkin, Sergey

    2009-05-15

    Results from long-term measurements of a chemically separated Db/Rf sample prepared from the products of a {sup 48}Ca on {sup 243}Am irradiation are presented. The sample with the highest spontaneous fission activity out of eight samples produced in the course of chemical experiments performed in 2004 was selected for these measurements. We conclude that there is no evidence for SF-decay originating from heavy actinide isotopes in this sample. Hence, it is appropriate to assign the SF-events observed in this experiment to decay products of {sup 288}115.

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  19. ESTIMATION OF NEUTRON SCATTER CORRECTION FOR CALIBRATION OF PERSONNEL DOSIMETER AND DOSERATEMETER AGAINST 241Am-Be SOURCE-MONTE CARLO SIMULATION AND MEASUREMENTS.

    PubMed

    Dawn, Sandipan; Bakshi, A K; Sathian, Deepa; Selvam, T Palani

    2016-10-07

    Neutron scatter contributions as a function of distance along the transverse axis of (241)Am-Be source were estimated by three different methods such as shadow cone, semi-empirical and Monte Carlo. The Monte Carlo-based FLUKA code was used to simulate the existing room used for the calibration of CR-39 detector as well as LB6411 doseratemeter for selected distances from (241)Am-Be source. The modified (241)Am-Be spectra at different irradiation geometries such as at different source detector distances, behind the shadow cone, at the surface of the water phantom were also evaluated using Monte Carlo calculations. Neutron scatter contributions, estimated using three different methods compare reasonably well. It is proposed to use the scattering correction factors estimated through Monte Carlo simulation and other methods for the calibration of CR-39 detector and doseratemeter at 0.75 and 1 m distance from the source.

  20. Monte Carlo modeling of spallation targets containing uranium and americium

    NASA Astrophysics Data System (ADS)

    Malyshkin, Yury; Pshenichnov, Igor; Mishustin, Igor; Greiner, Walter

    2014-09-01

    Neutron production and transport in spallation targets made of uranium and americium are studied with a Geant4-based code MCADS (Monte Carlo model for Accelerator Driven Systems). A good agreement of MCADS results with experimental data on neutron- and proton-induced reactions on 241Am and 243Am nuclei allows to use this model for simulations with extended Am targets. It was demonstrated that MCADS model can be used for calculating the values of critical mass for 233,235U, 237Np, 239Pu and 241Am. Several geometry options and material compositions (U, U + Am, Am, Am2O3) are considered for spallation targets to be used in Accelerator Driven Systems. All considered options operate as deep subcritical targets having neutron multiplication factor of k∼0.5. It is found that more than 4 kg of Am can be burned in one spallation target during the first year of operation.

  1. New Results for Elements 115, 117, and 118 Produced in the Reactions 243Am+48Ca and 249BK/249Cf+48Ca

    NASA Astrophysics Data System (ADS)

    Utyonkov, V. K.; Oganessian, Yu. Ts.; Abdullin, F. Sh.; Alexander, C.; Binder, J.; Boll, R. A.; Dmitriev, S. N.; Ezold, J.; Felker, K.; Gostic, J. M.; Grzywacz, R. K.; Hamilton, J. H.; Henderson, R. A.; Itkis, M. G.; Miernik, K.; Miller, D.; Moody, K. J.; Polyakov, A. N.; Ramayya, A. V.; Roberto, J. B.; Ryabinin, M. A.; Rykaczewski, K. P.; Sagaidak, R. N.; Shaughnessy, D. A.; Shirokovsky, I. V.; Shumeiko, M. V.; Stoyer, M. A.; Stoyer, N. J.; Subbotin, V. G.; Sukhov, A. M.; Tsyganov, Yu. S.; Voinov, A. A.; Vostokin, G. K.

    2014-09-01

    The reactions of 243Am and 249Bk with 48Ca have been reinvestigated to provide new evidence for the discovery of elements 113, 115, and 117. Three isotopes 287-289115 were synthesized in the 243Am+48Ca reactions at five projectile energies, providing excitation functions and α-decay spectra of the produced isotopes. Decay properties of 287,288115 and of all the daughter products agree with the data of the experiment in which these nuclei were synthesized for the first time. The new 289115 events demonstrate the same decay properties as those observed for 289115 populated by a decay of 293117 produced in the 249Bk+48Ca reaction to provide cross-bombardment evidence. Results of recent experiments at the Dubna gas-filled recoil separator aimed at studying production crosssections, excitation functions, and nuclear decay properties for isotopes 293,294117 synthesized in the 249Bk+48Ca reaction at five projectile energies are presented. In addition, a single decay of 294118 was observed from the reaction with 249Cf - a result of the in-growth of 249Cf in the 249Bk target.

  2. Experience in the management of disused lightning rods containing 241Am in a research institute in Brazil.

    PubMed

    Vicente, Roberto; Potiens, Ademar; Sakata, Solange; Dellamano, José

    2013-11-01

    Radioactive lightning rods (RLR) were manufactured and installed in Brazil for almost two decades, before they were prohibited in 1989. Structures protected by this type of lightning preventers included residential buildings, schools, commercial and industrial facilities, among others. It is estimated that about 3.4 TBq of 241Am were used by manufacturers, and a total of 75,000 pieces with a mean activity of about 46 MBq were in the market. While only a fraction of the total has been recovered, the almost twenty thousand pieces already collected at the Nuclear and Energy Research Institute (IPEN) had their sources successfully separated from the remaining recyclable metal scrap and are now encapsulated in lead containers for final disposal.

  3. Response function measurements of an NE102A organic scintillator using an 241Am-Be source

    NASA Astrophysics Data System (ADS)

    Naqvi, A. A.; Aksoy, A.; Khiari, F. Z.; Coban, A.; Nagadi, M. M.; Al-Ohali, M. A.; Al-Jalal, M. A.

    1994-07-01

    The response function of a 125 mm diameter NE102A organic scintillation detector has been measured over the 2.7-14.8 MeV neutron energy range. The detector response function was derived from the light output for monoenergetic neutrons and gamma rays. The light output of the detector for monoenergetic neutrons was measured by selecting narrowgates in the time-of-flight (TOF) spectrum for a 241Am-Be neutron source. In order to provide check points on the data, the detector light output was also measured for monoenergetic neutrons from the D(d, n) and T(d, n) reactions. The response function of the NE102A detector is in good agreement (within 1-5%) with the published data of Cecil et al. [Nucl. Instr. and Meth. 161 (1979) 439].

  4. Measurements of M and L X-ray energies and relative intensities emanating from (241)Am source.

    PubMed

    Verma, H R

    2017-04-01

    Energies and relative Intensities of 13 X-ray transitions in the M X-ray spectrum (per 100 disintegrations of (241)Am) viz. M4N1, Mξ1,2, M3N1, Mα, Mβ, Mγ, M2N1, M3O4,5+M3P1, M3Q1, M1N3, M2N4+M1N3, M2O1 and M1O2,3 lines along with L1-L3 have been measured in addition to the 21L X-ray lines viz. Lℓ, Lt, Ls, Lα2, Lα1, Lη, Lβ6, Lβ2,15, Lβ4, Lβ5,7, Lβ1, Lβ3, Lβ9,10, Lγ5, Lγ1, Lγ2,8, Lγ3,6, Lγ4,4, Lγ13 including two new lines at 19.63 and 23.17keV, have been measured. Since the M and L X-ray lines of 93Np in the decay of (241)Am source are frequently used for energy and efficiency calibration of the Si(Li)/HpGe detectors, the present measurements have been undertaken with an objective to update the data since there are either no concrete data available (even in the Table of Radioactive Isotopes and Table of Radionuclides) or there exist inconsistencies/disparities in the data available in the earlier publications. We confirm the existence of L1-L3 X-ray transition (falling in the region of M X-ray energy range) and Lt, Ls and Lβ9,10 (forbidden transitions as per selection rules). However, the origin of the two new L X-ray lines at 19.63 and 23.17keV, both with intensities of 0.05±0.01%, could not be ascertained.

  5. 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.

  6. Bioavailability of trace contaminants ({sup 241}Am, {sup 57}Co, {sup 137}Cs) to a benthic bivalve from pore waters and sediments

    SciTech Connect

    Gagnon, C.; Stupakoff, I.; Fisher, N.S.

    1995-12-31

    Sediments are major repositories of contaminants in marine ecosystems and can serve as a source of some contaminants for benthic organisms. The authors used the clam Macoma balthica, a species employed in monitoring coastal contamination, to compare experimentally three uptake sources: overlying water, ingested surface sediment and anoxic pore water. They studied the bioavailability of selected radionuclides ({sup 241}Am, {sup 57}Co, {sup 137}Cs) representing a large range of particle reactivity. For comparison, the authors also used CH{sub 3} {sup 203}Hg, which is highly assimilated by marine organisms. Clams were exposed separately to contaminated overlying water, surface oxic sediment and anoxic sediment. Radioactivity in animals was determined at the end of the exposure period. {sup 137}CS, which is not particle reactive in seawater, was not bioaccumulated from any source. {sup 241}Am and {sup 57}Co concentration factors in clams obtained from overlying water were approximately an order of magnitude lower than that of CH{sub 3} {sup 203}Hg. Ingested oxidized sediment particles do not appear to be a significant source for these radionuclides. {sup 241}Am, {sup 57}Co and CH{sub 3} {sup 203}Hg were bioconcentrated from anoxic pore waters, but the highly particle-reactive {sup 241}Am was mostly adsorbed onto the clam`s shell. The bioconcentration of CH{sub 3} {sup 203}Hg from pore waters was, however, only one tenth of that from overlying water.

  7. Simultaneous determination of radiocesium ((135)Cs, (137)Cs) and plutonium ((239)Pu, (240)Pu) isotopes in river suspended particles by ICP-MS/MS and SF-ICP-MS.

    PubMed

    Cao, Liguo; Zheng, Jian; Tsukada, Hirofumi; Pan, Shaoming; Wang, Zhongtang; Tagami, Keiko; Uchida, Shigeo

    2016-10-01

    Due to radioisotope releases in the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, long-term monitoring of radiocesium ((135)Cs and (137)Cs) and Pu isotopes ((239)Pu and (240)Pu) in river suspended particles is necessary to study the transport and fate of these long-lived radioisotopes in the land-ocean system. However, it is expensive and technically difficult to collect samples of suspended particles from river and ocean. Thus, simultaneous determination of multi-radionuclides remains as a challenging topic. In this study, for the first time, we report an analytical method for simultaneous determination of radiocesium and Pu isotopes in suspended particles with small sample size (1-2g). Radiocesium and Pu were sequentially pre-concentrated using ammonium molybdophosphate and ferric hydroxide co-precipitation, respectively. After the two-stage ion-exchange chromatography separation from the matrix elements, radiocesium and Pu isotopes were finally determined by ICP-MS/MS and SF-ICP-MS, respectively. The interfering elements of U ((238)U(1)H(+) and (238)U(2)H(+) for (239)Pu and (240)Pu, respectively) and Ba ((135)Ba(+) and (137)Ba(+) for (135)Cs and (137)Cs, respectively) were sufficiently removed with the decontamination factors of 1-8×10(6) and 1×10(4), respectively, with the developed method. Soil reference materials were utilized for method validation, and the obtained (135)Cs/(137)Cs and (240)Pu/(239)Pu atom ratios, and (239+240)Pu activities showed a good agreement with the certified/information values. In addition, the developed method was applied to analyze radiocesium and Pu in the suspended particles of land water samples collected from Fukushima Prefecture after the FDNPP accident. The (135)Cs/(137)Cs atom ratios (0.329-0.391) and (137)Cs activities (23.4-152Bq/g) suggested radiocesium contamination of the suspended particles mainly originated from the accident-released radioactive contaminates, while similar Pu contamination of suspended

  8. Standardization of (166m)Ho and 243Am/239Np by live-timed anti-coincidence counting with extending dead time.

    PubMed

    da Silva, C J; Loureiro, J S; Delgado, J U; Poledna, R; Moreira, D S; Iwahara, A; Tauhata, L; da Silva, R L; Lopes, R T

    2012-09-01

    The National Laboratory for Metrology of Ionizing Radiation (LNMRI)/Brazil acquired (166m)Ho and (243)Am/(239)Np solutions from commercial suppliers in order to realize primary standardization and therefore reducing the associated uncertainties. The method used in the standardization was the live-timed 4πβ(LS)-γ(ΝaI(Tl)) anticoincidence counting. The live-timed anticoincidence system is operated since 2006 in LNMRI and is composed of two MTR2 modules donated by Laboratoire National Henri Becquerel (LNE-LNHB)/France. The data acquisition system uses a homemade LabView program and an Excel file for calculus. These systems have been used for primary standardization at LNMRI for many radionuclides and recently took part in the (124)Sb and (177)Lu International Key Comparisons with good performance.

  9. Interpretation of cytogenetic damage induced in the germ line of male mice exposed for over 1 year to /sup 239/Pu alpha particles, fission neutrons, or /sup 60/Co gamma rays

    SciTech Connect

    Grahn, D.; Lee, C.H.; Farrington, B.F.

    1983-09-01

    The relative biological effectiveness (RBE) of /sup 239/Pu ..cap alpha.. particles, fission neutrons (0.85 MeV), and /sup 60/Co ..gamma.. rays has been evaluated for the induction of reciprocal chromosome translocations in spermatogonia and of chromosome/chromatid fragments and chromatid rearrangements in the primary spermatocyte of adult male B6CF/sub 1/ mice. Age concurrency was maintained for both internal and external radiations which were delivered at about 1 rad/week for /sup 239/Pu (single intravenous dose of 10 ..mu..Ci/kg), 0.67, 1.67, and 2.67 rad/week for neutrons, and 6.95, 17.4, and 32 rad/week for ..gamma.. rays for at least 60 weeks. In terms of frequency of translocations, the response to the alpha emitter was nonlinear (concave downward) with little dose-response predictability; to cumulative neutron exposures the response was linear, without evidence of a dose-rate effect; and to ..gamma.. radiation the responses were linear, and a significant dose-rate effect was seen. RBE estimates are variable. The overall response to the ..cap alpha.. emitter is interpreted to be a complex function of (a) microdosimetric heterogeneity, (b) a nearly invariant deposition pattern in the gonad, (c) the high sensitivity of differentiating spermatogonia to cell killing, and (d) the capacity of stem cells in relatively radiation-free areas to progressively assume the major spermatogenic role.

  10. EFFICIENCY STUDY OF A LEGe DETECTOR SYSTEM FOR THE ASSESSMENT OF 241Am IN SKULL AT CIEMAT WHOLE BODY COUNTER.

    PubMed

    Pérez López, B; Navarro, J F; López Ponte, M A; Nogueira, P

    2016-09-01

    (241)Am incorporation due to an incident or chronic exposure causes an internal dose, which can be evaluated from the total activity of this isotope in the skeleton several months after the intake. For this purpose, it is necessary to perform in vivo measurements of this bone-seeker radionuclide in appropriate counting bone geometries with very low attenuation of surrounded tissue and to extrapolate to total activity in the skeleton (ICRP 89, Basic anatomical and physiological data for use in radiological protection: reference values. 2001. 265). The work here presented refers to direct measurements of americium in the Cohen skull phantom at the CIEMAT Whole Body Counter (WBC) using low-energy germanium (LEGe) detectors inside a shielding room. The main goal was to determinate the most adequate head counting geometry for the in vivo detection of americium in the bone. The calibration of the in vivo LEGe system was performed with four detectors with 2 cm of distance to Cohen phantom. Two geometries were measured, on junction of frontal to parietal bones and frontal bone. The efficiencies are very similar in both geometries, the preferred counting geometry is the most comfortable for the person, with the LEGe detectors in the highest part of the frontal bone, near the junction with the parietal bone, CIEMAT WBC participated in a skull intercomparison exercise organised by WG7 of EURADOS (European Radiation Dosimetry Group e.V.). Efficiencies using three different skull phantoms were obtained. Measurements were performed for different head counting positions, four of them in the plane of symmetry and others over the temporal bone. The detector was placed in parallel with the calibration phantom at a distance of 1 cm. The main gamma emission of (241)Am, 59.5 keV (36 %), was used for comparing efficiency values. The lower efficiency was obtained over the frontal and occipital bones. Measurement with one LEGe detector over the parietal bone is the most efficient. The

  11. Evidence for age-related performance degradation of (241)Am foil sources commonly used in UK schools.

    PubMed

    Whitcher, R; Page, R D; Cole, P R

    2014-06-01

    The characteristics of alpha radiation have for decades been demonstrated in UK schools using small sealed (241)Am sources. There is a small but steady number of schools who report a considerable reduction in the alpha count rate detected by an end-window GM detector compared with when the source was new. This cannot be explained by incorrect apparatus or set-up, foil surface contamination, or degradation of the GM detector. The University of Liverpool and CLEAPSS collaborated to research the cause of this performance degradation. The aim was to find what was causing the performance degradation and the ramifications for both the useful and safe service life of the sources. The research shows that these foil sources have greater energy straggling with a corresponding reduction in spectral peak energy. A likely cause for this increase in straggling is a significant diffusion of the metals over time. There was no evidence to suggest the foils have become unsafe, but precautionary checks should be made on old sources.

  12. Detection and dosimetry studies on the response of silicon diodes to an 241Am-Be source

    NASA Astrophysics Data System (ADS)

    Lotfi, Y.; Zaki Dizaji, H.; Abbasi Davani, F.

    2014-06-01

    Silicon diode detectors show potential for the development of an active personal dosimeter for neutron and photon radiation. Photons interact with the constituents of the diode detector and produce electrons. Fast neutrons interact with the constituents of the diode detector and converter, producing recoil nuclei and causing (n,α) and (n,p) reactions. These photon- and neutron-induced charged particles contribute to the response of diode detectors. In this work, a silicon pin diode was used as a detector to produce pulses created by photon and neutron. A polyethylene fast neutron converter was used as a recoil proton source in front of the detector. The total registered photon and neutron efficiency and the partial contributions of the efficiency, due to interactions with the diode and converter, were calculated. The results show that the efficiency of the converter-diode is a function of the incident photon and neutron energy. The optimized thicknesses of the converter for neutron detection and neutron dosimetry were found to be 1 mm and 0.1 mm respectively. The neutron records caused by the (n,α) and (n,p) reactions were negligible. The photon records were strongly dependent upon the energy and the depletion layer of the diode. The photons and neutrons efficiency of the diode-based dosimeter was calculated by the MCNPX code, and the results were in good agreement with experimental results for photons and neutrons from an 241Am-Be source.

  13. Characterisation of a setup for mixed beam exposures of cells to 241Am alpha particles and X-rays.

    PubMed

    Staaf, Elina; Brehwens, Karl; Haghdoost, Siamak; Pachnerová-Brabcová, Katerina; Czub, Joanna; Braziewicz, Janusz; Nievaart, Sander; Wojcik, Andrzej

    2012-09-01

    Exposure of humans to mixed fields of high- and low-linear energy transfer (LET) radiation occurs in many situations-for example, in urban areas with high levels of indoor radon as well as background gamma radiation, during airplane flights or certain forms of radiation therapy. From the perspective of health risk associated with exposure to mixed fields, it is important to understand the interactions between different radiation types. In most cellular investigations on mixed beams, two types of irradiations have been applied sequentially. Simultaneous irradiation is the desirable scenario but requires a dedicated irradiation facility. The authors have constructed a facility where cells can be simultaneously exposed to (241)Am alpha particles and 190-kV X-rays at 37°C. This study presents the technical details and the dosimetry of the setup, as well as validates the performance of the setup for clonogenic survival in AA8 Chinese hamster ovary cells. No significant synergistic effect was observed. The relative biological effectiveness of the alpha particles was 2.56 for 37 % and 1.90 for 10 % clonogenic survival.

  14. 137Cs, 239+240Pu and 240Pu/239Pu atom ratios in the surface waters of the western North Pacific Ocean, eastern Indian Ocean and their adjacent seas.

    PubMed

    Yamada, Masatoshi; Zheng, Jian; Wang, Zhong-Liang

    2006-07-31

    Surface seawater samples were collected along the track of the R/V Hakuho-Maru cruise (KH-96-5) from Tokyo to the Southern Ocean. The (137)Cs activities were determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas, the eastern Indian Ocean, the Bay of Bengal, the Andaman Sea, and the South China Sea. The (137)Cs activities showed a wide variation with values ranging from 1.1 Bq m(-3) in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m(-3) in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of (137)Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of (137)Cs from the surface waters were roughly estimated from the two data sets of Miyake et al. [Miyake Y, Saruhashi K, Sugimura Y, Kanazawa T, Hirose K. Contents of (137)Cs, plutonium and americium isotopes in the Southern Ocean waters. Pap Meteorol Geophys 1988;39:95-113] and this study to be 0.016 yr(-1) in the Sulu and Indonesian Seas, 0.033 yr(-1) in the Bay of Bengal and Andaman Sea, and 0.029 yr(-1) in the South China Sea. These values were much lower than that in the coastal surface water of the western Northwest Pacific Ocean. This was likely due to less horizontal and vertical mixing of water masses and less scavenging. (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were also determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas and the South China Sea. The (240)Pu/(239)Pu atom ratios ranged from 0.199+/-0.026 to 0.248+/-0.027 on average, and were significantly higher than the global stratospheric fallout ratio of 0.18. The contributions of the North Pacific Proving Grounds close-in fallout Pu were estimated to be 20% for the western North Pacific Ocean, 39% for the Sulu and Indonesian Seas and 42% for the South China Sea by using the two end-member mixing model. The higher (240)Pu/(239)Pu

  15. Standardisation of water-moderated 241Am-Be neutron source using De Pangher neutron long counter: experimental and Monte Carlo modelling.

    PubMed

    Ghodke, Shobha; Kumari, Sujatha; Singh, Yashoda; Sathian, V; Mahant, A K; Sharma, D N

    2012-02-01

    A convenient neutron source is made for calibration of neutron survey instruments and personal dosimeters that are used in various nuclear installations such as fuel reprocessing, waste management, fuel fabrication and oil and well logging facilities, etc. This source consists of a bare (241)Am-Be neutron source placed at the centre of a 15-cm radius stainless steel spherical shell filled with distilled water. This paper describes the standardisation of the source at Bhabha Atomic Research Centre, using De Pangher neutron long counter both experimentally and using the Monte Carlo simulation. The ratio of neutron yield of water moderated to the bare (241)Am-Be neutron source was found to be 0.573. From the simulation, the neutron-fluence-weighted average energy of water-moderated (241)Am-Be source (fluence-weighted average energy of 2.25 MeV, dose-weighted average energy of 3.55 MeV) was found to be nearly the same as that of a (252)Cf source (fluence-weighted average energy of 2.1 MeV, dose-weighted average energy of 2.3 MeV). This source can be used for calibration in addition to (252)Cf, to study the variation in response of neutron monitoring instruments.

  16. Complex aberrations in lymphocytes exposed to mixed beams of (241)Am alpha particles and X-rays.

    PubMed

    Staaf, Elina; Deperas-Kaminska, Marta; Brehwens, Karl; Haghdoost, Siamak; Czub, Joanna; Wojcik, Andrzej

    2013-08-30

    Modern radiotherapy treatment modalities are associated with undesired out-of-field exposure to complex mixed beams of high and low energy transfer (LET) radiation that can give rise to secondary cancers. The biological effectiveness of mixed beams is not known. The aim of the investigation was the analysis of chromosomal damage in human peripheral blood lymphocytes (PBL) exposed to a mixed beam of X-rays and alpha particles. Using a dedicated exposure facility PBL were exposed to increasing doses of alpha particles (from (241)Am), X-rays and a mixture of both. Chromosomal aberrations were analysed in chromosomes 2, 8 and 14 using fluorescence in situ hybridisation. The found and expected frequencies of simple and complex aberrations were compared. Simple aberrations showed linear dose-response relationships with doses. A higher than expected frequency of simple aberrations was only observed after the highest mixed beam dose. A linear-quadratic dose response curve for complex aberrations was observed after mixed-beam exposure. Higher than expected frequencies of complex aberrations were observed for the two highest doses. Both the linear-quadratic dose-response relationship and the calculation of expected frequencies show that exposure of PBL to mixed beams of high and low LET radiation leads to a higher than expected frequency of complex-type aberrations. Because chromosomal changes are associated with cancer induction this result may imply that the cancer risk of exposure to mixed beams in radiation oncology may be higher than expected based on the additive action of the individual dose components.

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

    SciTech Connect

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

    1996-01-01

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

  18. Interpretation of cytogenetic damage induced in the germ line of male mice exposed for over 1 year to /sup 239/Pu alpha particles, fission neutrons, or /sup 60/Co gamma rays

    SciTech Connect

    Grahn, D.; Lee, C.H.; Farrington, B.F.

    1983-09-01

    The relative biological effectiveness (RBE) of /sup 239/Pu alpha particles, fission neutrons (0.85 MeV), and /sup 60/Co gamma rays has been evaluated for the induction of reciprocal chromosome translocations in spermatogonia and of chromosome/chromatid fragments and chromatid rearrangements in the primary spermatocyte of adult male B6CF1 mice. Age concurrency was maintained for both internal and external radiations which were delivered at about 1 rad/week for /sup 239/Pu (single intravenous dose of 10 microCi/kg), 0.67, 1.67, and 2.67 rad/week for neutrons, and 6.95, 17.4, and 32 rad/week for gamma rays for at least 60 weeks. In terms of frequency of translocations, the response to the alpha emitter was nonlinear (concave downward) with little dose-response predictability; to cumulative neutron exposures the response was linear, without evidence of a dose-rate effect; and to gamma radiation the responses were linear, and a significant dose-rate effect was seen. RBE estimates are variable. For translocations, the n/gamma ratio is between 10 and 24, depending upon weekly dose level, and the ratio is 1 or less for the alpha particle relative to the neutron. For fragments, the n/gamma ratio is 18 to 22, depending upon age factors, and alpha/n is 1.5. For chromatid rearrangements, n/gamma is 7 and alpha/n is essentially indeterminate, but much below one. The overall response to the alpha emitter is interpreted to be a complex function of (a) microdosimetric heterogeneity, (b) a nearly invariant deposition pattern in the gonad, (c) the high sensitivity of differentiating spermatogonia to cell killing, and (d) the capacity of stem cells in relatively radiation-free areas to progressively assume the major spermatogenic role.

  19. New Insights into the 243Am 48Ca Reaction Products Previously Observed in the Experiments on Elements 113, 115, and 117

    SciTech Connect

    Oganessian, Yuri Ts.; Abdullin, F. Sh.; Dmitriev, S.; Gostic, J. M.; Hamilton, Joseph; Henderson, R.; Itkis, M. G.; Moody, K.; Polyakov, A. N.; Ramayya, A. V.; Roberto, James B; Rykaczewski, Krzysztof Piotr; Sagaidak, R. N.; Shaughnessy, D.; Shirokovsky, I. V.; Stoyer, M.; Subbotin, V. G.; Sukhov, A. M.; Tsyganov, Yu. S.; Utyonkov, V.; Voinov, A. A.; Vostokin, G. K.

    2012-01-01

    Results of a new series of experiments on the study of production cross sections and decay properties of the isotopes of element 115 in the reaction {sup 243}Am + {sup 48}Ca are presented. Twenty-one new decay chains originating from {sup 288}115 were established as the product of the 3n-evaporation channel by measuring the excitation function at three excitation energies of the compound nucleus {sup 291}115. The decay properties of all newly observed nuclei are in full agreement with those we measured in 2003. At the lowest excitation energy E* = 33 MeV, for the first time we registered the product of the 2n-evaporation channel, {sup 289}115, which was also observed previously in the reaction {sup 249}Bk + {sup 48}Ca as the daughter nucleus of the decay of {sup 293}117. The maximum cross section for the production of {sup 288}115 is found to be 8.5 pb at E* {approx} 36 MeV.

  20. New insights into the 243Am + 48Ca reaction products previously observed in the experiments on elements 113, 115, and 117.

    PubMed

    Oganessian, Yu Ts; Abdullin, F Sh; Dmitriev, S N; Gostic, J M; Hamilton, J H; Henderson, R A; Itkis, M G; Moody, K J; Polyakov, A N; Ramayya, A V; Roberto, J B; Rykaczewski, K P; Sagaidak, R N; Shaughnessy, D A; Shirokovsky, I V; Stoyer, M A; Subbotin, V G; Sukhov, A M; Tsyganov, Yu S; Utyonkov, V K; Voinov, A A; Vostokin, G K

    2012-01-13

    Results of a new series of experiments on the study of production cross sections and decay properties of the isotopes of element 115 in the reaction (243)Am+(48)Ca are presented. Twenty-one new decay chains originating from (288)115 were established as the product of the 3n-evaporation channel by measuring the excitation function at three excitation energies of the compound nucleus (291)115. The decay properties of all newly observed nuclei are in full agreement with those we measured in 2003. At the lowest excitation energy E*=33 MeV, for the first time we registered the product of the 2n-evaporation channel, (289)115, which was also observed previously in the reaction (249)Bk+(48)Ca as the daughter nucleus of the decay of (293)117. The maximum cross section for the production of (288)115 is found to be 8.5 pb at E*≈36 MeV.

  1. Effects of deformations and orientations in the fission of the actinide nuclear system 254Fm* formed in the 11B + 243Am reaction

    NASA Astrophysics Data System (ADS)

    Kaur, Manpreet; Sharma, Manoj K.; Gupta, Raj K.

    2012-12-01

    We have studied the decay of actinide nuclear system 254Fm* formed in 11B + 243Am reaction using the dynamical cluster decay model (DCM), with choices of spherical, quadrupole deformation β2 alone and higher multipole deformations β2-β4. For β2 deformations, the optimum orientations θiopt are used whereas for higher multipole deformations the compact orientations θic of decaying fragments are taken in to account. Besides static-β2 deformations, the effects of dynamical-β2 deformations are also explored. The calculated cross sections find excellent agreement with the available experimental data with spherical as well as deformed choices of fragmentations, enabling us to account for the role of important nuclear deformation effects in the 11B-induced nuclear reaction. Spontaneous decay of 254Fm with cold elongated configuration and optimum orientation is also worked out. The mass distributions of excited fermium isotopes in the neighborhood of 254Fm* are also explored. In addition, the roles of temperature, angular momentum, and fission fragment anisotropies are investigated in the context of the chosen reaction.

  2. Characterization of neutron flux spectra in the irradiation sites of a 37 GBq 241Am-Be isotopic source

    NASA Astrophysics Data System (ADS)

    Yücel, Haluk; Budak, Mustafa Guray; Karadag, Mustafa; Yüksel, Alptuğ Özer

    2014-11-01

    For the applicability of instrumental neutron activation analysis (NAA) technique, an irradiation unit with a 37 GBq 241Am-Be neutron source was installed at Institute of Nuclear Sciences of Ankara University. Design and configuration properties of the irradiation unit are described. It has two different sample irradiation positions, one is called site #1 having a pneumatic sample transfer system and the other is site #2 having a location for manual use. In order to characterize neutron flux spectra in the irradiation sites, the measurement results were obtained for thermal (Фth) and epithermal neutron fluxes (Фepi), thermal to epithermal flux ratio (f) and epithermal spectrum shaping factors (α) by employing cadmium ratios of gold (Au) and molybdenum (Mo) monitors. The activities produced in these foils were measured by using a p-type, 44.8% relative efficiency HPGe well detector. For the measured γ-rays, self-absorption and true coincidence summing effects were taken into account. Additionally, thermal neutron self-shielding and resonance neutron self-shielding effects were taken into account in the measured results. For characterization of site #1, the required parameters were found to be Фth = (2.11 ± 0.05) × 103 n cm-2 s-1, Фepi = (3.32 ± 0.17) × 101 n cm-2 s-1, f = 63.6 ± 1.5, α = 0.045 ± 0.009, respectively. Similarly, those parameters were measured in site #2 as Фth = (1.49 ± 0.04) × 103 n cm-2 s-1, Фepi = (2.93 ± 0.15) × 101 n cm-2 s-1, f = 50.9 ± 1.3 and α = 0.038 ± 0.008. The results for f-values indicate that good thermalization of fast neutrons on the order of 98% was achieved in both sample irradiation sites. This is because an optimum combination of water and paraffin moderator is used in the present configuration. In addition, the shielding requirements are met by using natural boron oxide powder (5.5 cm) and boron loaded paraffin layers against neutrons, and a 15 cm thick lead bricks against gamma-rays from source and its

  3. Results of The Excreta Bioassay Quality Control Program For April 1, 2010 Through March 31, 2011

    SciTech Connect

    Antonio, Cheryl L.

    2012-07-19

    A total of 76 urine samples and 10 spiked fecal samples were submitted during the report period (April 1, 2010 through March 31, 2011) to GEL Laboratories, LLC in South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for 14C, Sr, for 238Pu, 239Pu, 241Am, 243Am, 235U, 238U, 238U-mass and fecal analyses for 241Am, 238Pu and 239Pu were tested this year. The number of QC urine samples submitted during the report period represented 1.1% of the total samples submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 31% of the analyses processed by GEL during the first year of contract 112512 were quality control samples. GEL tested the performance of 23 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty except the slightly elevated relative bias for 243,244Cm (Table 4).

  4. Results Of The Excreta Bioassay Quality Control Program For April 1, 2007 Through March 31, 2008

    SciTech Connect

    Antonio, Cheryl L.

    2008-12-31

    A total of 79 urine samples, 3 blank fecal and 5 spiked artificial fecal samples were submitted during the report period (April 1, 2007 through March 31, 2008) to General Engineering Laboratories, South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for tritium, Sr, 238Pu, 239Pu, 241Am, 243Am 235U, 238U, elemental uranium and fecal analyses for 241Am, 238Pu and 239Pu were tested this year. The number of QC urine samples submitted during the report period represented 1.8% of the total samples submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 35% of the analyses processed by GEL during the third year of this contract were quality control samples. GEL tested the performance of 24 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty (Table 4). IDP concluded that GEL was performing well for all analyses tested, and concerns identified earlier were satisfactorily resolved.

  5. Results of The Excreta Bioassay Quality Control Program For April 1, 2008 through March 31, 2009

    SciTech Connect

    Antonio, Cheryl L.

    2010-06-01

    A total of 62 urine samples and 6 spiked fecal samples were submitted during the report period (April 1, 2008 through March 31, 2009) to General Engineering Laboratories, South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for Sr, 238Pu, 239Pu, 241Am, 243Am 235U, 238U, elemental uranium and fecal analyses for 241Am, 238Pu and 239Pu were tested this year. The number of QC urine samples submitted during the report period represented 1.3% of the total samples submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 34% of the analyses processed by GEL during the third year of this contract were quality control samples. GEL tested the performance of 21 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty. IDP concluded that GEL was performing well for all analyses tested, and concerns identified earlier were satisfactorily resolved (see section on Follow-up on Concerns During the Fourth Contract Year).

  6. Results of the Excreta Bioassay Quality Control Program For April 1, 2006 Through March 31, 2007

    SciTech Connect

    Antonio, Cheryl L.

    2008-02-19

    A total of 66 urine samples, 6 blank fecal and 6 spiked artificial fecal samples were submitted during the report period (April 1, 2006 through March 31, 2007) to General Engineering Laboratories, South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for tritium, Sr, 238Pu, 239Pu, 241Am, 243Am 235U, 238U, elemental uranium and fecal analyses for 241Am, 238Pu and 239Pu were tested this year. The number of QC urine samples submitted during the report period represented 1.7% of the total samples submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 36% of the analyses processed by GEL during the second year of this contract were quality control samples. GEL tested the performance of 16 radioisotopes, all of which met or exceeded the specifications in the Statement of Work. IDP concluded that GEL was performing well for all analyses tested, and concerns identified earlier were satisfactorily resolved.

  7. ANSI/ANS-8.15-1981(R87): Nuclear criticality control of special actinide elements

    SciTech Connect

    Brewer, R.W.; Pruvost, N.L.; Rombough, C.T.

    1996-12-31

    The American National Standard, {open_quotes}Nuclear Criticality Safety in Operations with Fissionable Materials Outside Reactotors{close_quotes} American National Standards Institute/American Nuclear Society (ANSI/ANS)-8.1-1983(R88) provides guidance for the nuclides {sup 233}U, {sup 235}U, and {sup 239}Pu. These three nuclides are of primary interest in out-of-reactor criticality safety since they are the most commonly encountered in the vast majority of operations. However, some operations can involve nuclides other than {sup 233}U, {sup 235}U, and {sup 239}Pu in sufficient quantities that their effect on criticality safety could be of concern. ANSI/ANS-8.15-1981(R87) {open_quotes}Nuclear Criticality Control of Special Actinide Elements,{close_quotes} provides guidance for 15 such nuclides. The standard was approved for use on November 9, 1981. When it received its first 5-yr review, no changes were made, and it was reaffirmed effective October 30, 1987. The standard was again reviewed and reaffirmed without changes in December 1995. The next 5-yr review of the standard is due in December 2000. The affected nuclides are {sup 237}Np, {sup 238}Pu, {sup 240}Pu, {sup 242}Pu, {sup 241}Am, {sup 243}Am, {sup 244}Cm, {sup 239}Pu, {sup 241}Pu, {sup 242m}Am, {sup 243}Cm, {sup 245}Cm, {sup 247}Cm, {sup 249}Cf, and {sup 251}Cf.

  8. Study on retardation mechanism of {sup 3}H, {sup 99}Tc, {sup 137}Np and {sup 241}Am in compacted sodium bentonite

    SciTech Connect

    Sato, H.; Ashida, T.; Kohara, Y.; Yui, M.

    1993-12-31

    The apparent diffusion coefficients were measured at room temperature (about 23{degrees}C) under atmospheric condition by the one-dimensional non-steady state diffusion method for {sup 3}H, {sup 99}Tc, {sup 137}Cs, {sup 237}Np and {sup 241}Am in compacted sodium-bentonite saturated with water. Sodium-bentonite which, is commercially available as KunigelVi{reg_sign}, was used in this study. Experiments were carried out in the density range of 0.4-2.0({times} 10{sup 3}kg/m{sup 3}). Bentonite in the cell was prepared to be saturated with distilled water. The measured apparent diffusion coefficient decreases with increasing dry density of bentonite. That the apparent diffusion coefficient of {sup 3}H decreased as a function of dry density of bentonite appears to be the effect of the change of porous structure with dry density of bentonite. {sup 99}Tc is pertechnetate ion under atmospheric condition. Retardation for {sup 137}Cs may be caused by ion-exchange on bentonite. The sorption, anion-exclusion and molecular filtration are considered as a retardation mechanism for {sup 237}Np and {sup 241}Am because those dominant species are negatively charged and of large ionic size.

  9. 241 Am ( n ,γ) cross section in the neutron energy region between 0.02 eV and 300 keV

    NASA Astrophysics Data System (ADS)

    Jandel, M.; Bredeweg, T. A.; Bond, E. M.; Chadwick, M. B.; Clement, R. R.; Couture, A.; O'Donnell, J. M.; Haight, R. C.; Reifarth, R.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wouters, J. M.; Macri, R. A.; Wu, C. Y.; Becker, J. A.

    2008-04-01

    The Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos National Laboratory (LANL) was used for a neutron capture cross section measurement on 241 Am . The high granularity of the DANCE array (160 BaF2 detectors in a 4π geometry) enables an efficient detection of prompt gamma rays following neutron capture. The preliminary results on the 241 Am ( n ,γ) cross section are presented from 0.02 eV to 300 keV. The cross section at thermal energy E n = 0.0253 eV was determined to be 665±33 barns. Resonance parameters were obtained using the SAMMY7 fit to the measured cross section in the resonance region. Significant discrepancies were found between our results and data evaluations for the first three lowest lying resonances. The cross section for neutrons with E n >l keV agrees well with the ENDF/B-VII.0 and JENDL-3.3 evaluations.

  10. Effects of arctic temperatures on distribution and retention of the nuclear waste radionuclides 241Am, 57Co, and 137Cs in the bioindicator bivalve Macoma balthica

    USGS Publications Warehouse

    Hutchins, D.A.; Stupakoff, I.; Hook, S.; Luoma, S.N.; Fisher, N.S.

    1998-01-01

    The disposal of radioactive wastes in Arctic seas has made it important to understand the processes affecting the accumulation of radionuclides in food webs in coldwater ecosystems. We examined the effects of temperature on radionuclide assimilation and retention by the bioindicator bivalve Macoma balthica using three representative nuclear waste components, 241Am, 57Co, and 137Cs. Experiments were designed to determine the kinetics of processes that control uptake from food and water, as well as kinetic constants of loss. 137Cs was not accumulated in soft tissue from water during short exposures, and was rapidly lost from shell with no thermal dependence. No effects of temperature on 57Co assimilation or retention from food were observed. The only substantial effect of polar temperatures was that on the assimilation efficiency of 241Am from food, where 10% was assimilated at 2??C and 26% at 12??C. For all three radionuclides, body distributions were correlated with source, with most radioactivity obtained from water found in the shell and food in the soft tissues. These results suggest that in general Arctic conditions had relatively small effects on the biological processes which influence the bioaccumulation of radioactive wastes, and bivalve concentration factors may not be appreciably different between polar and temperate waters.

  11. {sup 241}Am(n,{gamma}) cross section in the neutron energy region between 0.02 eV and 300 keV

    SciTech Connect

    Jandel, M.; Bredeweg, T. A.; Bond, E. M.; Chadwick, M. B.; Clement, R. R.; Couture, A.; O' Donnell, J. M.; Haight, R. C.; Reifarth, R.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wouters, J. M.; Macri, R. A.; Wu, C. Y.; Becker, J. A.

    2008-04-17

    The Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos National Laboratory (LANL) was used for a neutron capture cross section measurement on {sup 241}Am. The high granularity of the DANCE array (160 BaF2 detectors in a 4{pi} geometry) enables an efficient detection of prompt gamma rays following neutron capture. The preliminary results on the {sup 241}Am(n,{gamma}) cross section are presented from 0.02 eV to 300 keV. The cross section at thermal energy E{sub n} = 0.0253 eV was determined to be 665{+-}33 barns. Resonance parameters were obtained using the SAMMY7 fit to the measured cross section in the resonance region. Significant discrepancies were found between our results and data evaluations for the first three lowest lying resonances. The cross section for neutrons with E{sub n}>l keV agrees well with the ENDF/B-VII.0 and JENDL-3.3 evaluations.

  12. A method of measurement of (239)Pu, (240)Pu, (241)Pu in high U content marine sediments by sector field ICP-MS and its application to Fukushima sediment samples.

    PubMed

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Aono, Tatsuo; Tazoe, Hirofumi; Tagami, Keiko; Uchida, Shigeo; Yamada, Masatoshi

    2014-01-01

    An accurate and precise analytical method is highly needed for the determination of Pu isotopes in marine sediments for the long-term marine environment monitoring that is being done since the Fukushima Dai-ichi Nuclear Power Plant accident. The elimination of uranium from the sediment samples needs to be carefully checked. We established an analytical method based on anion-exchange chromatography and SF-ICP-MS in this work. A uranium decontamination factor of 2 × 10(6) was achieved, and the U concentrations in the final sample solutions were typically below 4 pg mL(-1), thus no extra correction of (238)U interferences from the Pu spectra was needed. The method was suitable for the analysis of (241)Pu in marine sediments using large sample amounts (>10 g). We validated the method by measuring marine sediment reference materials and our results agreed well with the certified and the literature values. Surface sediments and one sediment core sample collected after the nuclear accident were analyzed. The characterization of (241)Pu/(239)Pu atom ratios in the surface sediments and the vertical distribution of Pu isotopes showed that there was no detectable Pu contamination from the nuclear accident in the marine sediments collected 30 km off the plant site.

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  14. 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.

  15. 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.

  16. Measurement of the neutron-induced fission cross-section of 241Am at the time-of-flight facility n_TOF

    NASA Astrophysics Data System (ADS)

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

    2013-01-01

    The neutron-induced fission cross-section of 241Am has been measured relative to the standard fission cross-section of 235U between 0.5 and 20MeV. The experiment was performed at the CERN n_TOF facility. Fission fragments were detected by a fast ionization chamber by discriminating against the α-particles from the high radioactivity of the samples. The high instantaneous neutron flux and the low background of the n_TOF facility enabled us to obtain uncertainties of ≈ 5%. With the present results it was possible to resolve discrepancies between previous data sets and to confirm current evaluations, thus providing important information for design studies of future reactors with improved fuel burn-up.

  17. 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.

  18. Production cross sections of {sub 105}{sup 261}Ha from the {sup 250}Cf({sup 15}N,4n) and {sup 243}Am({sup 22}Ne,4n) reactions

    SciTech Connect

    Lane, M.R.; Gregorich, K.E.; Lee, D.M.; Wierczinski, B.; McGrath, C.A.; Hendricks, M.B.; Shaughnessy, D.A.; Strellis, D.A.; Sylwester, E.R.; Wilk, P.A.; Hoffman, D.C. |

    1998-12-01

    We have measured the production cross section of 1.8-s {sup 261}Ha from two different reactions. It was produced in the {sup 250}Cf({sup 15}N,4n) reaction at 84 MeV and in the {sup 243}Am({sup 22}Ne,4n) reaction at 116 MeV. Our rotating wheel system with a special parent-daughter stepping mode was used to detect {alpha}-{alpha} correlations between {sup 261}Ha and {sup 257}Lr. We measured 13 and 9 correlations in the two reactions, respectively. Assuming a 100{percent} {alpha} branch, we have determined the production cross section of {sup 261}Ha to be 0.51{plus_minus}0.20thinspnb in the {sup 250}Cf({sup 15}N,4n) reaction at 84 MeV, and 0.25{plus_minus}0.11thinspnb in the {sup 243}Am({sup 22}Ne,4n) reaction at 116 MeV. Based on the number of fission events observed in the latter reaction, we have been able to set an upper limit of 18{percent} for the spontaneous fission branch of {sup 261}Ha. {copyright} {ital 1998} {ital The American Physical Society}

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

    SciTech Connect

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

    2016-01-15

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

  20. 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

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

    DOE PAGES

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

    2016-01-06

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

  2. Effective atomic number of some sugars and amino acids for scattering of (241)Am and (137)Cs gamma rays at low momentum transfer.

    PubMed

    Vinaykumar, L; Umesh, T K

    2015-09-01

    In this paper, we report the effective atomic number of some H, C, N and O based sugars and amino acids. These have been determined by using a handy expression which is based on the theoretical angle integrated small angle (coherent+incoherent) scattering cross sections of seven elements of Z≤13 in four angular ranges of (0-4°), (0-6°), (0-8°) and (0-10°)for (241)Am (59.54 keV) and (137)Cs (661.6 keV) gamma rays. The theoretical scattering cross sections were computed by a suitable numerical integration of the atomic form factor and incoherent scattering function compilations of Hubbell et al. (1975) which make use of the non-relativistic Hartree-Fock (NRHF) model for the atomic charge distribution of the elements in the angular ranges of interest. The angle integrated small angle scattering cross sections of the H, C, N and O based sugars and amino acids measured by a new method reported recently by the authors were used in the handy expression to derive their effective atomic number. The results are compared with the other available data and discussed. Possible conclusions are drawn based on the present study.

  3. Effects of humic substances on the 241Am migration in a sandy aquifer: column experiments with Gorleben groundwater/sediment systems

    NASA Astrophysics Data System (ADS)

    Artinger, R.; Kienzler, B.; Schüßler, W.; Kim, J. I.

    1998-12-01

    Migration experiments were performed to study the influence of aquatic humic substances on the transport behavior of 241Am(III). Four groundwaters with different humic substance concentrations (DOC: 1 to 80 mg/l) were sampled together with Pleistocene aeolian quartz sand from the Gorleben site. Sand, groundwaters and humic substances were characterized by different analytical methods (e.g., ICP-MS, X-ray diffraction, X-ray fluorescence analysis, ultrafiltration). The sand was equilibrated with each groundwater under inert gas atmosphere with 1% CO 2 for a period of at least 3 months. As confirmed by ultrafiltration, the size distribution of humic colloids remained unchanged during equilibration. The hydraulic properties of sand columns were characterized with tritiated water as an inert tracer. Column and batch experiments were carried out with each groundwater as a function of the reaction period and flow velocity. In addition, the influence of the equilibration period of Am with groundwater was investigated prior to the injection into a column. The results revealed that increasing humic substance concentration reduced the Am sorption onto sand and enhanced the transport as colloid-borne Am species. The migration of colloid-borne Am was slightly faster than the groundwater flow velocity. Furthermore, the migration behavior of Am was found to depend on kinetically controlled interaction of humic colloid-bound Am with the sand surface. The application of the laboratory data to natural conditions was examined. The results were found applicable for the assessment of humic colloid facilitated radionuclide migration in natural aquifers.

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

    PubMed

    Yücel, Haluk

    2007-11-01

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

  5. Characteristics of Symmetric and Asymmetric Fission Modes as a Function of the Compound Nucleus Excitation in the Proton-Induced Fission of 233Pa, 239Np and 243Am

    SciTech Connect

    Beresova, M.; Kliman, J.; Krupa, L.; Bogatchev, A. A.; Itkis, I. M.; Itkis, M. G.; Kniajeva, G. N.; Kondratiev, N. A.; Kozulin, E. M.; Pokrovsky, I. V.; Dorvaux, O.; Khlebnikov, S.; Lyapin, V.; Rubchenia, W.; Stuttge, L.; Trzaska, W.; Vakhtin, D.

    2007-05-22

    Average preequilibrium average statistical prescission and postscission neutron multiplicities as well as average {gamma}-ray multiplicity , average energy emitted by {gamma}-rays and average energy per one gamma quantum <{epsilon}{gamma}> as a function of mass and total kinetic energy (TKE) of fission fragments were measured in the proton-induced reactions p+232Th{yields}233Pa, p+238U{yields}239Np and p+242Pu{yields}243Am (at proton energy Ep=13, 20, 40 and 55 MeV). The fragment mass and energy distributions (MEDs) have been analyzed in terms of the multimodal fission. The decomposition of the experimental MEDs onto the MEDs of the distinct modes has been fulfilled in the framework of a method that is free from any parameterization of the distinct fission mode mass distribution shapes. The main characteristics for symmetric and asymmetric modes have been studied in their dependence on the compound nucleus composition and proton energy. The manifestation of multimodal fission in average {gamma}-ray multiplicities of fission fragments was also studied in this work.

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

    SciTech Connect

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

    1982-05-01

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

  7. Bayesian integration of radioisotope dating (210Pb, 137Cs, 241Am, 14C) and an 18-20th century mining history of Brotherswater, English Lake District

    NASA Astrophysics Data System (ADS)

    Schillereff, Daniel; Chiverrell, Richard; Macdonald, Neil; Hooke, Janet; Welsh, Katharine; Piliposyan, Gayane; Appleby, Peter

    2014-05-01

    Lake sediment records are often a useful tool for investigating landscape evolution as geomorphic changes in the catchment are reflected by altered sediment properties in the material transported through the watershed and deposited at the lake bed. Recent research at Brotherswater, an upland waterbody in the Lake District, northwest England, has focused on reconstructing historical floods from their sedimentary signatures and calculating long-term sediment and carbon budgets from fourteen sediment cores extracted from across the basin. Developing accurate chronological control is essential for these tasks. One sediment core (BW11-2; 3.5 m length) from the central basin has been dated using artificial radionuclide measurements (210Pb, 137Cs, 241Am) for the uppermost sediments and radiocarbon (14C) for lower sediments. The core appears to span the past 1500 years, however a number of problems have arisen. We present our explanations for these errors, the independent chronological techniques used to generate an accurate age-depth model for this core and methods for its transferral to the other 13 cores extracted from the basin. Two distinct 137Cs markers, corresponding to the 1986 Chernobyl disaster and 1960s weapons testing, confirm the 210Pb profile for sediment deposition since ~1950, but calculations prior to this appear erroneous, possibly due to a hiatus in the sediment record. We used high-resolution geochemical profiles (measured by XRF) to cross-correlate with a second 210Pb-dated chronology from a more distal location, which returned more sensible results. Unfortunately, the longer 14C sequence exhibits two age-reversals (radiocarbon dates that are too old). We believe the uppermost two dates are erroneous, due to a shift in inflow location as a flood prevention method ~1900 A.D., dated using information from historical maps. The lower age-reversal coincides with greater supply of terrigenous material to the lake (increased Zr, K, Ti concentrations

  8. Evaluation of Measurements of 238Pu, 239Pu and 240Pu in Urine at the Microbecquerel Level Using Thermal Ionization Mass Spectrometry and Alpha Spectrometry at Los Alamos National Laboratory: Results of a Two Year Comparison Test (LA-UR-06-8055)

    SciTech Connect

    Bores, Norman; Schultz, Michael K

    2008-01-01

    The Intercomparison Studies Program (ISP) at the Oak Ridge National Laboratory (ORNL, Oak Ridge, TN, USA) provides natural-matrix urine quality-assurance/quality-control (QA/QC) samples to radiobioassay analysis laboratories. In 2003, a single laboratory (Los Alamos National Laboratory LANL, Los Alamos NM USA) requested a change in the test-samples provided previously by the ISP. The change was requested to evaluate measurement performance for analyses conducted using thermal-ionization mass spectrometry (TIMS). Radionuclides included {sup 239}Pu at two activity levels (75-150 {micro}Bq {sm_bullet} sample{sup -1} and 1200-1600 {micro}Bq {sm_bullet} sample{sup -1}) and {sup 238}Pu (3700-7400 {micro}Bq {sm_bullet} sample{sup -1}). In addition, {sup 240}Pu was added to the samples so that the {sup 239+240}Pu specific activity was 3700-7400 {micro}Bq {sm_bullet} sample{sup -1}. In this paper, the results of testing during the period May, 2003 through September, 2005 are presented and discussed.

  9. Efficacy of orally administered amphipathic polyaminocarboxylic acid chelators for the removal of plutonium and americium: comparison with injected Zn-DTPA in the rat.

    PubMed

    Miller, Scott C; Liu, Gang; Bruenger, Fred W; Lloyd, Ray D

    2006-01-01

    Chelators are used to promote excretion of actinides and some other metals, but few are orally effective. The relative efficacies of orally administered triethylenetetraminepentaacetic acids (TT) with varying lipophilic properties on the removal of 241Am and 239Pu and comparison with parenteral Zn-DTPA was determined. The actinides were administered to adult rats 2 weeks prior to initiation of 30 d of chelation treatment. The TT compounds were given orally while Zn-DTPA was given twice weekly by injection. Total body content of 241Am was measured before and during the treatment period and organ contents of 241Am and 239Pu were measured at the end of the study. Significant reductions in 241Am occurred within the first week, with Zn-DTPA being the most effective. By 3 weeks, the most lipophilic chelator, C22TT was as effective as Zn-DTPA. After 30 d, reductions in organ content of 239Pu and 241Am directly correlated with increasing lipophilicity of the TT chelators. Oral C22TT was as effective as injected Zn-DTPA in liver and bone, the major organs of actinide deposition. The removal of 239Pu from the liver and reduction of redeposition of 239Pu in newly formed bone by C22TT was confirmed by neutron-induced autoradiographs. The amphipathic TT chelators may be useful as orally administered alternatives to current parenteral DTPA for the removal of actinide elements from the body, particularly for longer-term therapeutic applications.

  10. [239Pu and chromosomal aberrations in human peripheral blood lymphocytes].

    PubMed

    Okladnikova, N D; Osovets, S V; Kudriavtseva, T I

    2009-01-01

    The genome status in somatic cells was assessed using the chromosomal aberration (CA) test in peripheral blood lymphocytes from 194 plutonium workers exposed to occupational radiation mainly from low-transportable compounds of airborne 230Pu. Pu body burden at the time of cytogenetic study varied from values close to the method sensitivity to values multiply exceeding the permissible level. Standard (routine) methods of peripheral blood lymphocytes cultivation were applied. Chromatid- and chromosomal-type structural changes were estimated. Aberrations were estimated per 100 examined metaphase cells. The quantitative relationship between the CA frequency and Pu body burden and the absorbed dose to the lung was found. Mathematical processing of results was carried out based on the phenomenological model. The results were shown as theoretical and experimental curves. The threshold of the CA yield was 0.43 +/- 0.03 kBq (Pu body burden) and 6.12 +/- 1.20 cGy (absorbed dose to the lung).

  11. Fission Rate Ratios of FCA-IX Assemblies as Integral Experiment for Assessment of TRU's Fission Cross Sections

    NASA Astrophysics Data System (ADS)

    Fukushima, Masahiro; Tsujimoto, Kazufumi; Okajima, Shigeaki

    2016-03-01

    At the fast critical assembly (FCA) of JAEA, central fission rate ratios for TRU such as 237Np, 238Pu, 239Pu, 242Pu, 241Am, 243Am, and 244Cm were measured in the seven uraniumfueled assemblies (FCA-IX assemblies) with systematically changed neutron spectra. The FCA-IX assemblies were constructed with simplicity both in geometry and composition. By virtue of these FCA-IX assemblies where the simple combinations of uranium fuel and diluent (graphite and stainless steel) in their core regions were systematically varied, the neutron spectra of them cover from the intermediate to fast one. Taking their advantages, benchmark models with respect to the central fission rate ratios had been recently developed for the evaluation of the TRU's fission cross sections. As an application of these benchmark models, the Japanese Evaluated Nuclear Data Library JENDL-4.0 was utilized by a Monte Carlo calculation code. Several results show large discrepancies between the calculation and experimental values. The benchmark models would be well suited for the evaluation and modification of the nuclear data for the TRU's fission cross sections.

  12. EMP Attachment 1 DOE-SC PNNL Site Sampling and Analysis Plan

    SciTech Connect

    Meier, Kirsten M.

    2011-11-10

    This Sampling and Analysis Plan (SAP) is written for the radiological environmental air surveillance program for the DOE-SC PNNL Site, Richland Washington. It provides the requirements for planning sampling events, and the requirements imposed on the analytical laboratory analyzing the air samples. The actual air sampling process is in procedure EPRP-AIR-029. The rationale for analyte selection, media, and sampling site location has been vetted through the data quality objectives (DQO) process (Barnett et al. 2010). The results from the DQO process have been reviewed and approved by the Washington State Department of Health. The DQO process (Barnett et al. 2010) identified seven specific radionuclides for analysis along with the need for gross alpha and gross beta radiological analyses. The analytes are {sup 241}Am, {sup 243}Am, {sup 244}Cm, {sup 60}Co, {sup 238}Pu, {sup 239}Pu, and {sup 233}U. The report also determined that air samples for particulates are the only sample matrix required for the monitoring program. These samples are collected on 47-mm glass-fiber filters.

  13. Highly enriched isotopes of uranium and transuranium elements for scientific investigation

    NASA Astrophysics Data System (ADS)

    Vesnovskii, Stanislav P.; Polynov, Vladimir N.

    1992-08-01

    The paper describes the production of highly enriched isotopes of uranium, plutonium, americium and curium by means of electromagnetic separation for scientific and applied research in physics, chemistry, geology and other fields. The equipment and radiochemical methods used allows to provide the isotopic pure samples in quantities sufficient to set up nuclear physics experiments, to produce reference materials and standard sources for calibration of radiometrical and mass spectrometrical equipment and for use in radionuclear metrology. For a series of nuclei unique characteristics of isotopic enrichment and radiochemical and chemical purity were achieved: 233U: 99.97%; 235U: 99.97%; 236U: 98.0%; 238U: 99.997%; 238Pu: 99.6%; 239Pu: 99.9977%; 240Pu: 99.9-100%; 241Pu: 96.998%; 242Pu: 97.8-99.96%; 244Pu: 96.7%; 241Am: 99.6%; 242mAm: 85.6%; 243Am: 99.2-99.94%; 243Cm: 99.99%; 245Cm: 99.998%; 246Cm: 99.8%; 247Cm: 90%; 248Cm: 97%. Methods of radiochemical and chemical separation, product certification, fabrication of special sources or targets and layers of highly enriched isotopes on various substrates are presented.

  14. Measured solubilities and speciations of neptunium, plutonium, and americium in a typical groundwater (J-13) from the Yucca Mountain region; Milestone report 3010-WBS 1.2.3.4.1.3.1

    SciTech Connect

    Nitsche, H.; Gatti, R.C.; Standifer, E.M.

    1993-07-01

    Solubility and speciation data are important in understanding aqueous radionuclide transport through the geosphere. They define the source term for transport retardation processes such as sorption and colloid formation. Solubility and speciation data are useful in verifying the validity of geochemical codes that are part of predictive transport models. Results are presented from solubility and speciation experiments of {sup 237}NpO{sub 2}{sup +}, {sup 239}Pu{sup 4+}, {sup 241}Am{sup 3+}/Nd{sup 3+}, and {sup 243}Am{sup 3+} in J-13 groundwater (from the Yucca Mountain region, Nevada, which is being investigated as a potential high-level nuclear waste disposal site) at three different temperatures (25{degree}, 60{degree}, and 90{degree}C) and pH values (5.9, 7.0, and 8.5). The solubility-controlling steady-state solids were identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The neptunium solubility decreased with increasing temperature and pH. Plutonium concentrations decreased with increasing temperature and showed no trend with pH. The americium solutions showed no clear solubility trend with increasing temperature and increasing pH.

  15. Twenty-four Years of Follow-Up for a Hanford Plutonium Wound Case

    SciTech Connect

    Carbaugh, Eugene H.; Lynch, Timothy P.; Antonio, Cheryl L.; Medina-Del Valle, Fernando

    2010-10-01

    A 1985 plutonium puncture wound resulted in the initial deposition of 48 kBq of transuranic alpha activity, primarily 239Pu and 241Am, in a worker’s right index finger. Surgical excisions in the week following reduced the long-term residual wound activity to 5.4 kBq, and 164 DTPA chelation therapy administrations over a 17-month period resulted in urinary excretion of about 7 kBq. The case was published in 1988, but now 20 additional years of follow-up data are available. Annual bioassay measurements have included wound counts, skeleton counts, liver counts, lung counts, axillary lymph node counts, and urinalyses for plutonium and 241Am. These measurements have shown relatively stable levels of 241Am at the wound site, with gradually increasing amounts of 241Am detected in the skeleton. Liver counts has shown erratic detection of 241Am, and lung counts indicate 241Am as shine from the axillary lymph nodes and skeleton. Urine excretion of 239Pu since termination of chelation therapy has typically ranged from 10 to 20 mBq d-1, with 241Am excretion being about 10% of that for 239Pu. In addition, the worker has undergone annual routine medical exams, which have not identified any adverse health effects associated with the intake.

  16. Rapid determination of actinides in urine by inductively coupled plasma mass spectrometry and alpha spectrometry: a hybrid approach.

    PubMed

    Maxwell, Sherrod L; Jones, Vernon D

    2009-11-15

    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 3h. 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 6h 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. (239)Pu, (242)Pu, (237)Np, (243)Am, (234)U, (235)U and (238)U were measured by ICP-MS, while (236)Pu, (238)Pu, (239)Pu, (241)Am, (243)Am and (244)Cm 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

  17. 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

  18. Highly enriched isotope samples of uranium and transuranium elements for scientific investigation

    NASA Astrophysics Data System (ADS)

    Vesnovskii, Stanislav P.; Polynov, Vladimir N.; Danilin, Lev. D.

    1992-02-01

    The paper describes the production of highly enriched isotopes of uranium, plutonium, americium and curium by electromagnetic separation for scientific and applied researches in physics, chemistry, geology, medicine, biology and other fields. Using the equipment described, the isotopes are produced in quantities sufficient to set up nuclear physical experiments, to produce nuclear reference materials and standard sources for calibration of radiometrical and mass spectrometrical equipment, in radionuclide metrology, etc. For the following isotopes the indicated degrees of isotopic enrichment were achieved: 233U - 99.97%; 235U - 99.97%; 236U - 98.0%; 238U - 99.997%; 238Pu - 99.6%; 239Pu - 99.9977%; 240Pu - 99.9-100%; 241Pu - 96.998%; 242Pu - 97.8-99.96%; 244Pu - 96.7%; 241Am - 99.6%; 242Am - 73.6%; 243Am - 99.2-99.94%; 243Cm - 99.99%; 245Cm - 99.998%; 246Cm - 99.8%; 247Cm - 90%; 248Cm - 97%. Methods for preparing layers of highly enriched isotopes on various substances are presented: - electrochemical deposition of transuranic elements from aqueous-organic and organic media and vacuum spraying: - the method of foil and coating formation via compounds in the vapour phase; - the method of fabrication of layers of transuranic elements on superthin (1-2 μm) metal substrates with additional isolating polymer-metal coatings (0.2-0.4 μm), that substantially decrease material transfer from the active layer and increase safety of product handling.

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

    SciTech Connect

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

    1991-01-01

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

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

    SciTech Connect

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

    2007-08-28

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

  1. Stations VZD and VZE: composition of ending inventory reports

    SciTech Connect

    Not Available

    1984-02-10

    The inventory of the following materials at stations VZD and VZE is given: depleted uranium; enriched uranium; /sup 242/Pu; /sup 241/Am; /sup 243/Am; curium; berkelium; californium; plutonium; lithium; /sup 233/U, normal uranium; neptunium; /sup 238/Pu; deuterium; tritium; and thorium.

  2. Investigations of the binding of 239Pu to liver cell membranes.

    PubMed

    Planas-Bohne, F; Kampmann, G; Olinger, H

    1989-07-15

    The binding of Pu to liver cell membranes was studied and compared with that of iron with which plutonium shares some physiological properties. The binding of both metals is sensitive to pH changes and they can be dissociated from their binding sites by chelating agents and transferrin. The metal-binding proteins can be extracted with detergents. Both metals have at least two binding sites, the molecular weights of which lie between 150 and 400 kDa; the isoelectric points for iron are 5.5 and 6.5, and for plutonium 6.0 and 6.5. The significance of these results for plutonium uptake into liver cells is discussed.

  3. Event-by-Event Study of Prompt Neutrons from 239Pu

    SciTech Connect

    Vogt, R; Randrup, J; Pruet, J; Younes, W

    2010-01-15

    Employing a recently developed Monte Carlo model, we study the fission of {sup 240}Pu induced by neutrons with energies from thermal to just below the threshold for second chance fission. Current measurements of the mean number of prompt neutrons emitted in fission, together with less accurate measurements of the neutron energy spectra, place remarkably fine constraints on predictions of microscopic calculations. In particular, the total excitation energy of the nascent fragments must be specified to within 1 MeV to avoid disagreement with measurements of the mean neutron multiplicity. The combination of the Monte Carlo fission model with a statistical likelihood analysis also presents a powerful tool for the evaluation of fission neutron data. Of particular importance is the fission spectrum, which plays a key role in determining reactor criticality. We show that our approach can be used to develop an estimate of the fission spectrum with uncertainties several times smaller than current experimental uncertainties for outgoing neutron energies of less than 2 MeV.

  4. Event-by-event study of prompt neutrons from 239Pu(n,f)

    SciTech Connect

    Vogt, R; Randrup, J; Pruet, J; Younes, W

    2009-07-23

    Employing a recently developed Monte-Carlo model, we study the fission of {sup 240}Pu induced by neutrons with energies from thermal to just below the threshold for second chance fission. Current measurements of the mean number of prompt neutrons emitted in fission, together with less accurate measurements of the neutron energy spectra, place remarkably fine constraints on predictions of microscopic calculations. In particular, the total excitation energy of the nascent fragments must be specified to within 1MeV to avoid disagreement with measurements of the mean neutron multiplicity. The combination of the Monte-Carlo fission model with a statistical likelihood analysis also presents a powerful tool for the evaluation of fission neutron data. Of particular importance is the fission spectrum, which plays a key role in determining reactor criticality. We show that our approach can be used to develop an estimate of the fission spectrum with uncertainties several times smaller than current experimental uncertainties for outgoing neutron energies of less than 2 MeV.

  5. Fission Product Yields from Fission Spectrum n+ 239Pu for ENDF/B-VII.1

    NASA Astrophysics Data System (ADS)

    Chadwick, M. B.; Kawano, T.; Barr, D. W.; Mac Innes, M. R.; Kahler, A. C.; Graves, T.; Selby, H.; Burns, C. J.; Inkret, W. C.; Keksis, A. L.; Lestone, J. P.; Sierk, A. J.; Talou, P.

    2010-12-01

    We describe a new cumulated fission product yield (FPY) evaluation for fission spectrum neutrons on plutonium that updates the ENDF/B-VI evaluation by England and Rider, for the forthcoming ENDF/B-VII.1 database release. We focus on FPs that are needed for high accuracy burnup assessments; that is, for inferring the number of fissions in a neutron environment. Los Alamos conducted an experiment in the 1970s in the Bigten fast critical assembly to determine fission product yields as part of the Interlaboratory Reaction Rate (ILRR) collaboration, and this has defined the Laboratory's fission standard to this day. Our evaluation includes use of the LANL-ILRR measurements (not previously available to evaluators) as well as other Laboratory FPY measurements published in the literature, especially the high-accuracy mass spectrometry data from Maeck and others. Because the measurement database for some of the FPs is small — especially for 99Mo — we use a meta-analysis that incorporates insights from other accurately-measured benchmark FP data, using R-value ratio measurements. The meta-analysis supports the FP measurements from the LANL-ILRR experiment. Differences between our new evaluations and ENDF/B-VI are small for some FPs (less than 1-2%-relative for 95Zr, 140Ba, 144Ce), but are larger for 99Mo (4%-relative) and 147Nd (5%-relative, at 1.5 MeV) respectively. We present evidence for an incident neutron energy dependence to the 147Nd fission product yield that accounts for observed differences in the FPY at a few-hundred keV average energy in fast reactors versus measurements made at higher average neutron energies in Los Alamos' fast critical assemblies. Accounting for such FPY neutron energy dependencies is important if one wants to reach a goal of determining the number of fissions to accuracies of 1-2%. An evaluation of the energy-dependence of fission product yields is given for all A values based on systematical trends in the measured data, with a focus on the energy dependence over the fast neutron energy range from 0.2-2 MeV. Based on these trends, we present an evaluation of the FPY data at 0.5 and 2.0 MeV average incident neutron energies. This new set of ENDF/B-VII data will enable users to linearly interpolate between the pooled FPY data at ˜0.5 MeV and our new data at 2 MeV to obtain FPYs at other energies. We intend to release the ENDF/B-VII.1 database in December 2011, and all released data are subject to CSEWG approval. It is possible that the released evaluated data will differ from those presented in this paper; the evaluated date presented here can be referred to as ENDF/B-VII.1 beta 0.

  6. Matrix effects corrections in DDT assay of {sup 239}Pu with the CTEN instrument

    SciTech Connect

    Hollas, C.L.; Arnone, G.; Brunson, G.; Coop, K.

    1997-11-01

    The accuracy of transuranic (TRU) waste assay using the differential die-away technique depends upon significant corrections to compensate for the effects of the matrix material in which the TRU waste is located. We have used a new instrument, the combined thermal/epithermal neutron (CTEN) instrument for the assay of TRU waste, to develop methods to improve the accuracy of these corrections. Neutrons from a pulsed 14-MeV neutron generator are moderated in the walls of the CTEN cavity and induce fission in the TRU material. The prompt neutrons from these fission events are detected in cadmium-wrapped {sup 3}He neutron detectors. We have developed methods of data acquisition and analysis to extract correlation in the neutron signals resulting from fission during active interrogation. This correlation information, in conjunction with the total number of neutrons detected, is used to determine the fraction of fission neutrons transmitted through the matrix material into the {sup 3}He detectors. This determination allows us to cleanly separate the matrix effects into two processes: matrix modification upon the neutron interrogating flux and matrix modification upon the fraction of fission neutrons transmitted to the neutron detectors. Recent results indicate that for some matrix systems, corrections for position dependent effects within the matrix are possible. 7 refs., 7 figs., 1 tab.

  7. Uncertainty analysis of doses from ingestion of plutonium and americium.

    PubMed

    Puncher, M; Harrison, J D

    2012-02-01

    Uncertainty analyses have been performed on the biokinetic model for americium currently used by the International Commission on Radiological Protection (ICRP), and the model for plutonium recently derived by Leggett, considering acute intakes by ingestion by adult members of the public. The analyses calculated distributions of doses per unit intake. Those parameters having the greatest impact on prospective doses were identified by sensitivity analysis; the most important were the fraction absorbed from the alimentary tract, f(1), and rates of uptake from blood to bone surfaces. Probability distributions were selected based on the observed distribution of plutonium and americium in human subjects where possible; the distributions for f(1) reflected uncertainty on the average value of this parameter for non-specified plutonium and americium compounds ingested by adult members of the public. The calculated distributions of effective doses for ingested (239)Pu and (241)Am were well described by log-normal distributions, with doses varying by around a factor of 3 above and below the central values; the distributions contain the current ICRP Publication 67 dose coefficients for ingestion of (239)Pu and (241)Am by adult members of the public. Uncertainty on f(1) values had the greatest impact on doses, particularly effective dose. It is concluded that: (1) more precise data on f(1) values would have a greater effect in reducing uncertainties on doses from ingested (239)Pu and (241)Am, than reducing uncertainty on other model parameter values and (2) the results support the dose coefficients (Sv Bq(-1) intake) derived by ICRP for ingestion of (239)Pu and (241)Am by adult members of the public.

  8. Proton-induced fission of actinides at energies 26.5 and 62.9 MeV—Theoretical interpretation

    NASA Astrophysics Data System (ADS)

    Demetriou, P.; Keutgen, Th.; Prieels, R.; El Masri, Y.

    2011-10-01

    Fission properties of proton-induced fission on 232Th, 237Np, 238U, 239Pu and 241Am targets, measured at the Louvain-la-Neuve cyclotron facility at proton energies of 26.5 and 62.9 MeV, are compared with the predictions of the state-of-the-art nuclear reaction code TALYS. The sensitivity of the calculations to the input parameters of the code and possible improvements are discussed.

  9. Calibration of a large hyperpure germanium array for in-vivo detection of the actinides with a tissue-equivalent torso phantom

    SciTech Connect

    Berger, C.D.; Lane, B.H.

    1983-01-01

    For calibration of the array for internally deposited /sup 238/Pu, /sup 239/Pu, and /sup 241/Am, a tissue-equivalent anthropomorphic phantom, was used for efficiency determinations at the ORNL facility. This phantom consists of a tissue-equivalent torso into which is imbedded an adult male skeleton, interchangeable organs containing a homogeneous distribution of various radionuclides, and two sets of chest overlay plates for simulation of progressively thicker tissue over the chest, as well as differing thoracic fat contents. (PSB)

  10. Analysis of actinides in an ombrotrophic peat core - evidence of post-depositional migration of fallout radionuclides

    NASA Astrophysics Data System (ADS)

    Quinto, Francesca; Hrnecek, Erich; Krachler, Michael; Shotyk, William; Steier, Peter; Winkler, Stephan R.

    2013-04-01

    Plutonium (239Pu, 240Pu, 241Pu, 242Pu) and uranium (236U, 238U) isotopes were analyzed in an ombrotrophic peat core from the Black Forest, Germany, representing the last 80 years of atmospheric deposition. The reliable determination of these isotopes at ultra-trace levels was possible using ultra-clean laboratory procedures and accelerator mass spectrometry. The 240Pu/239Pu isotopic ratios are constant along the core with a mean value of 0.19 ±0.02 (N = 32). This result is consistent with the acknowledged average 240Pu/239Pu isotopic ratio from global fallout in the Northern Hemisphere. The global fallout origin of Pu is confirmed by the corresponding 241Pu/239Pu (0.0012 ±0.0005) and 242Pu/239Pu (0.004 ± 0.001) isotopic ratios. The identification of the Pu isotopic composition characteristic for global fallout in peat layers pre-dating the period of atmospheric atom bomb testing (AD 1956 - AD 1980) is a clear evidence of the migration of Pu downwards the peat profile. The maximum of global fallout derived 236U is detected in correspondence to the age/depth layer of maximum stratospheric fallout (AD 1963). This finding demonstrates that the 236U bomb peak can be successfully used as an independent chronological marker complementing the 210Pb dating of peat cores. The profiles of the global fallout derived 236U and 239Pu are compared with those of 137Cs and 241Am. As typical of ombrothrophic peat, the temporal fallout pattern of 137Cs is poorly retained. Similarly like for Pu, post-depositional migration of 241Am in peat layers preceding the era of atmospheric nuclear tests is observed.

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

    SciTech Connect

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

    2005-02-25

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

  12. The OSMOSE program for the qualification of integral cross sections of actinides: Preliminary results in a PWR-UOx spectrum

    SciTech Connect

    Hudelot, J. P.; Antony, M.; Bernard, D.; Fougeras, P.

    2006-07-01

    The need for improved nuclear data for minor actinides has been stressed by various organizations throughout the world - especially for studies relating to plutonium management, waste incineration, transmutation of waste, and Pu burning in future nuclear concepts. Several international programs have indicated a strong desire to obtain accurate integral reaction rate data for improving the major and minor actinides cross sections. Data on major actinides (i.e. {sup 235}U, {sup 236}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu and {sup 241}Am) are reasonably well-known and available in the Evaluated Nuclear Data Files (JEFF, JENDL, ENDF-BX However information on the minor actinides (i.e. {sup 232}Th, {sup 233}U, {sup 237}Np, {sup 238}Pu, {sup 242}Am, {sup 243}Am, {sup 243}Cm, {sup 235}Cm, {sup 244}Cm, {sup 245}Cm, {sup 246}Cm and {sup 247}Cm) is less well-known and considered to be relatively poor in some cases, having to rely on model and extrapolation of few data points. In this framework, the ambitious OSMOSE program between the Commissariat a l'Energie Atomique (CEA), Electricite de France (EDF) and the U.S. Dept. of Energy (DOE) has been undertaken with the aim of measuring the integral absorption rate parameters of actinides in the MINERVE experimental facility located at the CEA Cadarache Research Center. The OSMOSE Program (Oscillation in Minerve of isotopes in 'Eupraxic' Spectra) includes a complete analytical program associated with the experimental measurement program and aims at understanding and resolving potential discrepancies between calculated and measured values. In the OSMOSE program, the reactivity worth of samples containing separated actinides are measured in different neutron spectra using an oscillation technique with an overall expected accuracy better than 3%. Reactivity effects of less than 10 pcm (0.0001 or approximately 1.5 cents) are measured and compared with calibrations to determine the differential reactivity

  13. Electrochemical oxidation of 243Am(III) in nitric acid by a terpyridyl-derivatized electrode

    SciTech Connect

    Dares, C. J.; Lapides, A. M.; Mincher, B. J.; Meyer, T. J.

    2015-11-05

    A high surface area, tin-doped indium oxide electrode surface-derivatized with a terpyridine ligand has been applied to the oxidation of trivalent americium to Am(V) and Am(VI) in nitric acid. Potentials as low as 1.8 V vs. the saturated calomel electrode are used, 0.7 V lower than the 2.6 V potential for one-electron oxidation of Am(III) to Am(IV) in 1 M acid. This simple electrochemical procedure provides, for the first time, a method for accessing the higher oxidation states of Am in non-complexing media for developing the coordination chemistries of Am(V) and Am(VI) and, more importantly, for separation of americium from nuclear waste streams.

  14. Rapid monitoring for transuranic contaminants during buried waste retrieval

    SciTech Connect

    McIsaac, C.V.; Sill, C.W.; Gehrke, R.J.; Shaw, P.G.; Randolph, P.D.; Amaro, C.R.; Pawelko, R.J.; Thompson, D.N.; Loomis, G.G.

    1991-03-01

    This document reports results of research performed in support of possible future transuranic waste retrieval operations at the Idaho National Engineering Laboratory Radioactive Waste Management Complex. The focus of this research was to evaluate various methods of performing rapid and, as much as possible, on-line'' quantitative measurements of {sup 239}Pu or {sup 241}Am, either as airborne or loose contamination. Four different alpha continuous air monitors were evaluated for lower levels of detection of airborne {sup 239}Pu. All of the continuous air monitors were evaluated by sampling ambient air. In addition, three of the continuous air monitors were evaluated by sampling air synthetically laden with clean dust and dust spiked with {sup 239}Pu. Six methods for making quantitative measurements of loose contamination were investigated. They were: (1) microwave digestion followed by counting in a photon electron rejecting alpha liquid scintillation spectrometer, (2) rapid radiochemical separation followed by alpha spectrometry, (3) measurement of the {sup 241}Am 59 keV gamma ray using a thin window germanium detector, (4) measurement of uranium L-shell x-rays, (5) gross alpha counting using a large-area Ag activated ZnS scintillator, and (6) direct counting of alpha particles using a large-area ionization chamber. 40 refs., 42 figs., 24 tabs.

  15. Laser-optical studies of the spontaneous-fission isomer /sup 240m/Am

    SciTech Connect

    Beene, J.R.; Bemis, C.E. Jr.; Kramer, S.D.; Young, J.P.

    1982-01-01

    Improved optical pumping experiments on the /sup 240m/Am fission isomer have been performed using the Laser Induced Nuclear Polarization (LINUP) technique. Results of these experiments are discussed in terms of the constraints they place on the spectroscopic properties of /sup 240m/Am. In addition, a quantitative analysis of the isomer shift in terms of nuclear shape is undertaken making use of recent muonic x-ray data on /sup 241/Am and /sup 243/Am.

  16. Study of the fission isomer 240mAm (S. F. ) using laser-induced nuclear polarization. [Cross section of 238U(7Li,5n) at 48 MeV

    SciTech Connect

    Beene, J. R.; Bemis, Jr., C. E.; Young, J. P.; Kramer, S. D.

    1980-01-01

    The optical isomer shift was measured for the spontaneously fissioning isomer /sup 240m/Am. This shift is approximately 27 times greater than the /sup 241/Am-/sup 243/Am isotope shift, and confirms the conventional identification of fission isomers with large deformation. The measured isomer shift is consistent with a nuclear quadrupole moment of 30.4 b, in agreement with theoretical expectations. 2 figures. (RWR)

  17. American National Standard: for nuclear criticality control of special actinide elements

    SciTech Connect

    Not Available

    1981-01-01

    This standard is applicable to operations with the following: /sup 237/Np, /sup 238/Pu, /sup 240/Pu, /sup 241/Pu, /sup 242/Pu, /sup 241/Am, /sup 242m/Am, /sup 243/Am, /sup 243/Cm, /sup 244/Cm, /sup 245/Cm, /sup 247/Cm, /sup 249/Cf and /sup 251/Cf. Subcritical mass limits are presented for isolated fissionable units. The limits are not applicable to interacting units.

  18. Total and spontaneous fission half-lives of the americium and curium nuclides

    SciTech Connect

    Holden, N.E.

    1984-01-01

    The total half-life and the half-life for spontaneous fission are evaluated for the various long-lived nuclides of interest. Recommended values are presented for /sup 241/Am, /sup 242m/Am, /sup 243/Am, /sup 242/Cm, /sup 243/Cm, /sup 244/Cm, /sup 245/Cm, /sup 246/Cm, /sup 247/Cm, /sup 248/Cm, and /sup 250/Cm. The uncertainties are provided at the 95% confidence limit for each of the recommended values.

  19. Transuranic concentrations in reef and pelagic fish from the Marshall Islands. [/sup 239/Pu, /sup 240/Pu

    SciTech Connect

    Noshkin, V.E.; Eagle, R.J.; Wong, K.M.; Jokela, T.A.

    1980-09-01

    Concentrations of /sup 239 + 240/Pu are reported in tissues of several species of reef and pelagic fish caught at 14 different atolls in the northern Marshall Islands. Several regularities that are species dependent are evident in the distribution of /sup 239 + 240/Pu among different body tissues. Concentrations in liver always exceeded those in bone and concentrations were lowest in the muscle of all fish analyzed. A progressive discrimination against /sup 239 + 240/Pu was observed at successive trophic levels at all atolls except Bikini and Enewetak, where it was difficult to conclude if any real difference exists between the average concentration factor for /sup 239 + 240/Pu among all fish, which include bottom feeding and grazing herbivores, bottom feeding carnivores, and pelagic carnivores from different atoll locations. The average concentration of /sup 239 + 240/Pu in the muscle of surgeonfish from Bikini and Enewetak was not significantly different from the average concentrations determined in these fish at the other, lesser contaminated atolls. Concentrations among all 3rd, 4th, and 5th trophic level species are highest at Bikini where higher environmental concentrations are found. The reasons for the anomalously low concentrations in herbivores from Bikini and Enewetak are not known.

  20. Modelling the dispersion of 137Cs and 239Pu released from dumped waste in the Kara Sea

    NASA Astrophysics Data System (ADS)

    Harms, Ingo H.

    1997-10-01

    Three-dimensional, baroclinic, circulation models are applied to study the dispersal of radioactivity in the Barents Sea and Kara Sea. The release is supposed to occur at underwater dump sites for radioactive waste in the Kara Sea, used by the former Soviet Union. Two different spatial scales of dispersion are considered: the regional scale (the far field), which covers the shelves of the Barents and Kara Seas and the local scale (the near field) which is focused mainly on Abrasimov Bay where the dumping partly took place. The regional-scale model results suggest that, even for a worst case scenario, the radioactive contamination of Siberian coastal waters would be relatively small compared to observations in other marine systems (e.g the Baltic Sea and the Irish Sea). Realistic gradual release scenarios show very low concentrations in the central and eastern Kara Sea. A significant contamination of surrounding seas like the Laptev Sea, the Arctic Ocean or the Barents Sea by radioactive waste dispersion from the Kara Sea seems to be unlikely.

  1. Use of plutonium isotope activity ratios in dating recent sediments. [/sup 238/Pu//sup 239/Pu + /sup 240/Pu

    SciTech Connect

    Beasley, T. M.

    1982-01-01

    The majority of plutonium presently in the biosphere has come from the testing of nuclear devices. In the early 1950s, the Pu-238/239+240 activity ratio of fallout debris was > 0.04; in the more extensive test series of 1961 to 1962, the Pu-238/239+240 activity ratios were quite consistent at 0.02 to 0.03 and maximum fallout delivery occurred in mid-1963. A significant perturbation in Pu isotope activity ratios occurred in mid-1966 with the deposition of Pu-238 from the SNAP-9A reentry and burn-up. Recently deposited sediments have recorded these events and where accumulation rates are rapid (> 1 cm/y), changes in Pu isotope activity ratios can be used as a geochronological tool.

  2. Fission Product Yields from Fission Spectrum n+{sup 239}Pu for ENDF/B-VII.1

    SciTech Connect

    Chadwick, M.B.; Kawano, T.; Barr, D.W.; Mac Innes, M.R.; Kahler, A.C.; Graves, T.; Selby, H.; Burns, C.J.; Inkret, W.C.; Keksis, A.L.; Lestone, J.P.; Sierk, A.J.; Talou, P.

    2010-12-15

    We describe a new cumulated fission product yield (FPY) evaluation for fission spectrum neutrons on plutonium that updates the ENDF/B-VI evaluation by England and Rider, for the forthcoming ENDF/B-VII.1 database release. We focus on FPs that are needed for high accuracy burnup assessments; that is, for inferring the number of fissions in a neutron environment. Los Alamos conducted an experiment in the 1970s in the Bigten fast critical assembly to determine fission product yields as part of the Interlaboratory Reaction Rate (ILRR) collaboration, and this has defined the Laboratory's fission standard to this day. Our evaluation includes use of the LANL-ILRR measurements (not previously available to evaluators) as well as other Laboratory FPY measurements published in the literature, especially the high-accuracy mass spectrometry data from Maeck and others. Because the measurement database for some of the FPs is small - especially for {sup 99}Mo - we use a meta-analysis that incorporates insights from other accurately-measured benchmark FP data, using R-value ratio measurements. The meta-analysis supports the FP measurements from the LANL-ILRR experiment. Differences between our new evaluations and ENDF/B-VI are small for some FPs (less than 1-2%-relative for {sup 95}Zr, {sup 140}Ba, {sup 144}Ce), but are larger for {sup 99}Mo (4%-relative) and {sup 147}Nd (5%-relative, at 1.5 MeV) respectively. We present evidence for an incident neutron energy dependence to the {sup 147}Nd fission product yield that accounts for observed differences in the FPY at a few-hundred keV average energy in fast reactors versus measurements made at higher average neutron energies in Los Alamos' fast critical assemblies. Accounting for such FPY neutron energy dependencies is important if one wants to reach a goal of determining the number of fissions to accuracies of 1-2%. An evaluation of the energy-dependence of fission product yields is given for all A values based on systematical trends in the measured data, with a focus on the energy dependence over the fast neutron energy range from 0.2-2 MeV. Based on these trends, we present an evaluation of the FPY data at 0.5 and 2.0 MeV average incident neutron energies. This new set of ENDF/B-VII data will enable users to linearly interpolate between the pooled FPY data at {approx}0.5 MeV and our new data at 2 MeV to obtain FPYs at other energies.

  3. Fission fragment charge and mass distributions in 239Pu(n, f ) in the adiabatic nuclear energy density functional theory

    DOE PAGES

    Regnier, D.; Dubray, N.; Schunck, N.; ...

    2016-05-13

    Here, accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data are available, together with the variety of potential applications, is an incentive to develop a fully microscopic approach to fission dynamics.

  4. 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.

  5. Isotopic ratio correlation for the isotopic composition analysis of plutonium in Am-Pu mixed samples having high americium content.

    PubMed

    Patra, Sabyasachi; Agarwal, Chhavi; Chaudhury, Sanhita; Newton Nathaniel, T; Gathibandhe, M; Goswami, A

    2013-08-01

    Interference of high amount of americium in the plutonium isotopic composition analysis has been studied by simulating gamma-ray spectra for Am-Pu samples over a wide composition range (5-97% (241)Am) for both power and research reactor grade plutonium. An alternate way for isotopic composition analysis has been proposed by correlating the isotopic ratios available in our old database with the experimentally obtained (241)Pu/(239)Pu isotopic ratio. The proposed method has been validated using simulated spectra of known isotopic compositions.

  6. Determination of the counting efficiency of phoswich detectors for the assessment of internal contamination in lungs and lymph nodes by using a mathematical model

    NASA Astrophysics Data System (ADS)

    Righetti, M. A.; Hernandez, D.; Spano, F.

    1989-08-01

    This article presents the comparison between the results obtained by applying a mathematical and a physical model to the determination of the calibration factors for the direct measurements of the 239Pu and 241Am burden in lungs and lymph nodes. The mathematical model simulates the photon transport through a modified MIRD-V male phantom using the Monte Carlo technique. The physical model is a Livermore phantom supplied by the IAEA under the frame of the contract no. 3698/RI/CF. The results obtained show a good agreement between both models, since the differences are smaller than 13%.

  7. In situ subterranean determination of actinides by high-resolution gamma-ray spectrometry

    SciTech Connect

    Brodzinski, R. L.

    1981-04-01

    A system utilizing high resolution germanium diode gamma-ray spectroscopy for the simple, safe, and economical in situ determination of actinides is described. Six isotopes, /sup 235/U, /sup 238/U, /sup 237/Np, /sup 239/Pu, /sup 241/Pu, and /sup 241/Am, can be simultaneously measured at the 10 nCi g/sup -1/ level in less than 7 minutes. Collimators provide for measurement of horizontal strata as thin as 1 cm or solid angles as small as 0.1 steradians. Information obtainable with the system is discussed and compared to that obtainable with neutron activation/detection systems.

  8. Separation of actinides using capillary extraction chromatography-inductively coupled plasma mass spectrometry.

    PubMed

    Peterson, Dominic S; Montoya, Velma M

    2009-08-01

    Trace levels of actinides have been separated on capillary extraction chromatography columns. Detection of the actinides was achieved using an inductively coupled plasma mass spectrometer, which was coupled with the extraction chromatography system. In this study, we compare 30-cm long, 4.6 mm i.d. columns to capillary columns (750 microm i.d.) with lengths from 30 cm up to 150 cm. The columns that were tested were packed with TRU resin. We were able to separate a mixture of five actinides ((232)Th, (238)U, (237)Np, (239)Pu, and (241)Am). This work has application to rapid bioassay as well as automated separations of actinide materials.

  9. Comparative skeletal distribution of Am and Pu in man, monkey, and baboon

    SciTech Connect

    Lynch, T.P.; Kathren, R.L.; Dagle, G.E.; McInroy, J.F. )

    1989-01-01

    The skeletal distribution of Am and Pu in four human cases was compared with the skeletal distributions of these radioelements in baboons and monkeys. Excellent agreement was noted among the four human cases; data were available for Am in all four and Pu in three. A statistically significant correlation was found between the {sup 241}Am and {sup 239}Pu + {sup 240}Pu skeletal distributions in the humans and those in nonhuman primates. Trabecular bone had the highest concentrations of {sup 241}Am and {sup 239+240}Pu in humans, baboons, and monkeys. Scaling factors are proposed to convert the percentages of skeletal activity in animal bones to the corresponding percentages in the bones of the human skeleton.

  10. High resolution alpha particle detectors based on 4H-SiC epitaxial layer

    NASA Astrophysics Data System (ADS)

    Zat'ko, B.; Dubecký, F.; Šagátová, A.; Sedlačová, K.; Ryć, L.

    2015-04-01

    We fabricated and characterized 4H-SiC Schottky diodes as a spectrometric detector of alpha particles. A thin blocking contact of Ni/Au (15 nm) was used to minimize the influence on alpha particles energy. Current-voltage characteristics of the detector were measured and a low current density below 0.3 nAcm-2 was observed at room temperature. 239Pu241Am244Cm was used as a source of alpha particles within the energy range between 5.1 MeV and 5.8 MeV for detector testing. The charge collection efficiency close to 100 % at reverse bias exceeding 50 V was determined. The best spectrometric performance shows a pulse height spectrum at a reverse bias of 200 V giving an energy resolution of 0.25 % in the full width and half maximum for 5.486 MeV of 241Am.

  11. Few groups neutron spectra, and dosimetric features, of isotopic neutron sources.

    PubMed

    Vega-Carrillo, Hector Rene; Martinez-Ovalle, Segundo Agustín

    2016-11-01

    Using Monte Carlo methods, the neutron spectra in 31 energy groups of several isotopic neutron sources were estimated. For each source the neutron mean energy; the Ambient dose equivalent, the Personal dose equivalent and the Effective dose per unit fluence rate were calculated. A convenient way to produce neutrons is the isotopic neutron source, where the production is through (α, n), (γ, n), and spontaneous fission reactions. Isotopic neutron sources are small, easy to handle, and have a relative low cost. On the other hand the neutron yield is small and mostly of them produces neutrons with a wide energy distribution. In this work, the main features of (24)NaBe, (24)NaD2O, (116)InBe, (140)LaBe, (238)PuLi, (239)PuBe, (241)AmB, (241)AmBe, (241)AmF, (241)AmLi, (242)CmBe, (210)PoBe, (226)RaBe, (252)Cf and (252)Cf/D2O isotopic neutron source are also compiled.

  12. Histopathology and {sup 241}Am microdistribution in skeletal USTUR case 246

    SciTech Connect

    Priest, N.D.; Humphreys, J.A.H.; Freemont, A.; Kathren, R.L.

    1995-09-01

    Histopathology and qualitative autoradiography studies were undertaken on bone removed at autopsy from USTUR Case 246. The histopathology examination revealed extensive bone marrow peritrabecular fibrosis and decreased cellularity in most samples. In addition, histological indicators suggest that bone cell turnover was suppressed at most sites, although turnover was found to be essentially normal in a vertebral body sample. The autoradiographic studies showed that bone turnover that had occurred resulted in the redistribution of americium within bone. However, surface deposits of americium remained conspicuous at many sites, particularly those with low bone growth activity. A few percent of the americium was present in the bone marrow. the dosimetric and toxicology findings indicate that current assumptions about the metabolic behavior of bone-seeking radionuclides are likely to be unrealistically simplistic. 15 refs., 9 figs.

  13. Two new rodent models for actinide toxicity studies. [/sup 237/Pu, /sup 241/Am

    SciTech Connect

    Taylor, G.N.; Jones, C.W.; Gardner, P.A.; Lloyd, R.D.; Mays, C.W.; Charrier, K.E.

    1981-04-01

    Two small rodent species, the grasshopper mouse (Onychomys leucogaster) and the deer mouse (Peromyscus maniculatus), have tenacious and high retention in the liver and skeleton of plutonium and americium following intraperitoneal injection of Pu and Am in citrate solution. Liver retention of Pu and Am in the grasshopper mouse is higher than liver retention in the deer mouse. Both of these rodents are relatively long-lived, breed well in captivity, and adapt suitably to laboratory conditions. It is suggested that these two species of mice, in which plutonium retention is high and prolonged in both the skeleton and liver, as it is in man, may be useful animal models for actinide toxicity studies.

  14. Species-dependent chelation of (241)Am by DTPA Di-ethyl ester.

    PubMed

    Huckle, James E; Sadgrove, Matthew P; Mumper, Russell J; Jay, Michael

    2015-04-01

    Diethylenetriaminepentaacetic acid (DTPA) is an FDA-approved chelating agent for enhancing the elimination of transuranic elements such as americium from the body. Early access to therapy minimizes deposition of these radionuclides in tissues such as the bone. Due to its poor oral bioavailability, DTPA is administered as an IV injection, delaying access. Therefore, a diethyl-ester analog of DTPA, named C2E2, was synthesized as a means to increase oral absorption. As a hexadentate ligand, it was hypothesized that C2E2 was capable of binding americium directly. Therefore, the protonation constants and americium stability constant for C2E2 were determined by potentiometric titration and a solvent extraction method, respectively. C2E2 was shown to bind americium with a log K of 19.6. The concentrations of C2E2, its metabolite C2E1, and DTPA required to achieve effective binding in rat, beagle, and human plasma were studied in vitro. Dose response curves for each ligand were established, and the 50% maximal effective concentrations were determined for each species. As expected, higher concentrations of C2E2 were required to achieve the same degree of binding as DTPA. The results indicated that chelation in beagle plasma is more representative of the human response than rats. Finally, the pharmacokinetics of C2E2 were investigated in beagles, and the data was fit to a two-compartment model with elimination from the central compartment, along with first-order absorption. Based on the in vitro data, a 100 mg kg dose of C2E2 can be expected to have an effective duration of action of 3.8 h in beagles.

  15. Species-Dependent Chelation of 241Am by DTPA Di-ethyl Ester

    PubMed Central

    Huckle, James E.; Sadgrove, Matthew P.; Mumper, Russell J.; Jay, Michael

    2014-01-01

    Diethylenetriaminepentaacetic acid (DTPA) is an FDA approved chelating agent for enhancing the elimination of transuranic elements such as americium from the body. Early access to therapy minimizes deposition of these radionuclides in tissues such as the bone. Due to its poor oral bioavailability, DTPA is administered as an IV injection, delaying access. Therefore a diethyl-ester analog of DTPA, named C2E2, was synthesized as a means to increase oral absorption. As a hexadentate ligand, it was hypothesized that C2E2 was capable of binding americium directly. Therefore, the protonation constants and americium stability constant for C2E2 were determined by potentiometric titration and a solvent extraction method, respectively. C2E2 was shown to bind americium with a log K of 19.6. The concentrations of C2E2, its metabolite C2E1, and DTPA required to achieve effective binding in rat, beagle, and human plasma were studied in vitro. Dose response curves for each ligand were established and the 50% maximal effective concentrations were determined for each species. As expected, higher concentrations of C2E2 were required to achieve the same degree of binding as DTPA. The results indicated that chelation in beagle plasma is more representative of the human response than rats. Finally, the pharmacokinetics of C2E2 were investigated in beagles and the data was fit to a two-compartment model with elimination from the central compartment, along with first-order absorption. Based on the in vitro data, a 100 mg kg−1 dose of C2E2 can be expected to have an effective duration of action of 3.8 hours in beagles. PMID:25706138

  16. Kilogram-scale purification of americium by ion exchange

    SciTech Connect

    Wheelwright, E.J.

    1980-05-01

    Sequential anion and cation exchange processes have been used for the final purification of /sup 241/Am recovered during the reprocessing of aged plutonium metallurgical scrap. Plutonium was removed by absorption on Dowex 1, X-3.5 (30 to 50 mesh) anion exchange resin from 6.5 to 7.5 M HNO/sub 3/ feed solution. Following a water dilution to 0.75 to 1.0 M HNO/sub 3/, americium was absorbed on Dowex 50W, X-8 (50 to 100 mesh) cation exchange resin. Final purification was accomplished by elution of the absorbed band down 3 to 4 successive beds of the same resin, preloaded with Zn/sup 2+/, with an NH/sub 4/OH buffered chelating agent. The recovery of mixed /sup 241/Am-/sup 243/Am from power reactor reprocessing waste has been demonstrated. Solvent extraction was used to recover a HNO/sub 3/ solution of mixed lanthanides and actinides from waste generated by the reprocessing of 13.5 tons of Shippingport Power Reactor blanket fuel. Sequential cation exchange band-displacement processes were then used to separate americium and curium from the lanthanides and then to separate approx. 60 g of /sup 244/Cm from 1000 g of mixed /sup 241/Am-/sup 243/Am.

  17. Radionuclide concentrations in vegetation at radioactive-waste disposal Area G during the 1994 growing season

    SciTech Connect

    Fresquez, P.R.; Biggs, J.B.; Bennett, K.D.

    1995-07-01

    Overstory (pinon pine) and understory (grass and forb) vegetation samples were collected within and around selected points at Area G-a low-level radioactive solid-waste disposal facility at Los Alamos National Laboratory-for the analysis of tritium ({sup 3}H), strontium ({sup 90}Sr), plutonium ({sup 238} Pu and {sup 239}Pu), cesium ({sup 137}Cs), americium ({sup 241}Am), and total uranium. In general, most vegetation samples collected within and around Area G contained radionuclide levels in higher concentrations than vegetation collected from background areas. Tritium, in particular, was detected as high as 5,800 pCi/mL in overstory vegetation collected outside the fence just west of the tritium shafts; this suggests that tritium is migrating from this waste repository through subsurface pathways. Also, understory vegetation collected north of the transuranic (TRU) pads (outside the fence of Area G) contained the highest values of {sup 90}Sr, {sup 238}Pu, {sup 239}Pu, {sup 137}Cs, and {sup 241}Am, and may be a result of surface holding, storage, or disposal activities.

  18. Radionuclide Leaching from Residual Solids Remaining after Acid Dissolution of K East Area Sludge Composite

    SciTech Connect

    Delegard, C.H.; Rinehart, D.E.; Carlson, C.D.; Soderquist, C.Z.; Fadeff, S.K.

    1999-04-02

    Laboratory tests were performed to examine the efficacy of various leach treatments for decontaminating dissolver residual solids (KEACRESID1) produced during a 24-hour dissolution of K East Basin floor and Weasel Pit sludge composite in boiling 6 M HNO{sub 3}. The scope of this testing has been described in Section 4.5 of ''Testing Strategy to Support the Development of K Basin Sludge Treatment Process'' (Flament 1998). Radionuclides sorbed or associated with the residual solids generated in the K Basin sludge treatment process can restrict disposal of this solid to the Environmental Restoration Disposal Facility (ERDF). The starting dissolver residual solid for this testing, KEACRESID1, is a visibly heterogeneous material. This material contains radionuclides at concentrations above the ERDF Waste Acceptance Criteria for transuranics (TRU) by about a factor of 3, for {sup 239}Pu by a factor of 10, and for {sup 241}Am by a factor of 1.6. It meets the ERDF criterion for {sup 137}Cs by a factor of 4 and for uranium by a factor of 10. Therefore, the radionuclides of greatest interest in this leaching study are first {sup 239}Pu, and then {sup 241}Am, {sup 137}Cs, and uranium.

  19. Radionuclide Leaching from Residual Solids Remaining after Acid Dissolution of Composite K East Canister Sludge

    SciTech Connect

    Delegard, C.H.; Rinehart, D.E.; Soderquist, C.Z.; Fadeff, S.K.

    1999-04-02

    Laboratory tests were performed to examine mixed nitric/hydrofluoric acid leach treatments for decontaminating dissolver residual solids (KECDVSR24H-2) produced during a 20- to 24-hr dissolution of a composite K East (KE) Basin canister sludge in 95 C 6 M nitric acid (HNO{sub 3}). The scope of this testing has been described in Section 4.5 of ''Testing Strategy to Support the Development of K Basin Sludge Treatment Process'' (Flament 1998). Radionuclides sorbed or associated with the residual solids generated in the K Basin sludge treatment process can restrict disposal of this solid to the Environmental Restoration Disposal Facility (ERDF). The starting dissolver residual solid for this testing, KECDVSR24H-2, contains radionuclides at concentrations which exceed the ERDF Waste Acceptance Criteria for TRU by about a factor of 70, for {sup 239}Pu by a factor of 200, and for {sup 241}Am by a factor of 50. The solids also exceed the ERDF criterion for {sup 137}Cs by a factor of 2 and uranium by a factor of 5. Therefore, the radionuclides of greatest interest in this leaching study are first {sup 239}Pu and {sup 241}Am (both components of TRU) and then uranium and {sup 137}Cs.

  20. Quantitative Analysis of Plutonium Content in Particles Collected from a Certified Reference Material by Total Nuclear Reaction Energy (Q Value) Spectroscopy

    NASA Astrophysics Data System (ADS)

    Croce, M. P.; Hoover, A. S.; Rabin, M. W.; Bond, E. M.; Wolfsberg, L. E.; Schmidt, D. R.; Ullom, J. N.

    2016-08-01

    Microcalorimeters with embedded radioisotopes are an emerging category of sensor with advantages over existing methods for isotopic analysis of trace-level nuclear materials. For each nuclear decay, the energy of all decay products captured by the absorber (alpha particles, gamma rays, X-rays, electrons, daughter nuclei, etc.) is measured in one pulse. For alpha-decaying isotopes, this gives a measurement of the total nuclear reaction energy (Q value) and the spectra consist of well-separated, narrow peaks. We have demonstrated a simple mechanical alloying process to create an absorber structure consisting of a gold matrix with small inclusions of a radioactive sample. This absorber structure provides an optimized energy thermalization environment, resulting in high-resolution spectra with minimal tailing. We have applied this process to the analysis of particles collected from the surface of a plutonium metal certified reference material (CRM-126A from New Brunswick Laboratory) and demonstrated isotopic analysis by microcalorimeter Q value spectroscopy. Energy resolution from the Gaussian component of a Bortels function fit was 1.3 keV FWHM at 5244 keV. The collected particles were integrated directly into the detector absorber without any chemical processing. The ^{238}Pu/^{239}Pu and ^{240}Pu/^{239}Pu mass ratios were measured and the results confirmed against the certificate of analysis for the reference material. We also demonstrated inter-element analysis capability by measuring the ^{241}Am/^{239}Pu mass ratio.

  1. Radionuclide contaminant analysis of small mammals at Area G, TA-54, 1994

    SciTech Connect

    Biggs, J.; Bennett, K.; Fresquez, P.

    1995-09-01

    Small mammals were sampled at two waste burial sites (1 and 2) at Area G, TA-54 and a control site outside Area G (Site 3) to identify radionuclides that are present within surface and subsurface soils at waste burial sites, to compare the amount of radionuclide uptake by small mammals at waste burial sites to a control site, and to identify the primary mode of contamination to small mammals, either through surface contact or ingestion/inhalation. Three composite samples of at least five animals per sample were collected at each site. Pelts and carcasses of each animal were separated and analyzed independently. Samples were analyzed for {sup 241}Am, {sup 90}Sr, {sup 238}Pu, {sup 239}Pu, total U, and gamma spectroscopy (including {sup 137}Cs). Significantly higher (parametric t-test at p = 0.05) levels of total U, {sup 241}Am, {sup 238}Pu, {sup 239}Pu, and {sup 40}K were detected in pelts as compared to the carcasses of small mammals at TA-54. Concentrations of other measured radionuclides in carcasses were nearly equal to or exceeded the mean concentrations in the pelts. The authors results show higher concentrations in pelts compared to carcasses which is similar to what has been found at waste burial/contaminated sites outside of Los Alamos National Laboratory. Site 1 had significantly higher (alpha = 0.05, F = 0.0095) total U concentrations in carcasses than Sites 2 and 3. Site 2 had significantly higher (alpha = 0.05, F = 0.0195) {sup 239}Pu concentrations in carcasses than either Site 1 or Site 3. A significant difference in {sup 90}Sr concentration existed between Sites 1 and 2 (alpha = 0.05, F = 0.0681) and concentrations of {sup 40}K at Site 1 were significantly different from Site 3.

  2. Comparative food-chain behavior and distribution of actinide elements in and around a contaminated fresh-water pond

    SciTech Connect

    Garten, C.T. Jr.; Trabalka, J.R.; Bogle, M.A.

    1981-01-01

    The bioaccumulation of /sup 233/ /sup 234/U, /sup 238/U, /sup 238/Pu, /sup 239/ /sup 240/Pu, /sup 241/Am, and /sup 244/Cm in both native and introduced biota was studied at Pond 3513, a former low-level radioactive waste settling basin at Oak Ridge National Laboratory. This system, which was decommissioned in 1976 after more than 30 years use, contains approximately 5 Ci of /sup 239/ /sup 240/Pu; inventories of other actinide isotopes are considerably less. Significantly higher concentrations of actinides in fish that were allowed access to sediments indicated that sedimentary particulates may be the primary source of transuranics to biota in shallow fresh-water ecosystems. Our study determined habitat, in particular the degree of association of an organism with the sediment-water interface, to be the primary factor in controlling transuranic concentrations in aquatic biota. In most of the biological samples analyzed, excluding samples suspected of being contaminated by sediment, /sup 241/Am//sup 239/Pu, /sup 244/Cm//sup 239/Pu, and /sup 238/U//sup 239/Pu ratios were greater than the respective ratio in sediment while /sup 233/ /sup 234/U//sup 238/U, and /sup 239/ /sup 240/Pu//sup 238/Pu ratios were not different from the respective ratios in sediment. The relative uptake of actinides from contaminated sediment by aquatic and terrestrial biota at this site was U > Cm greater than or equal to Am > Pu. The relative extractability of actinides from shoreline sediment was U > Cm approx. = Am > Pu; we also observed the same relative ranking for sediment-water exchange in situ. Concentrations of transuranics in water, terrestrial vegetation, and vertebrate carcasses were less than 10% of the recommended public exposure maximum permissible concentration (MPC) of the ICRP.

  3. Concordant plutonium-241-americium-241 dating of environmental samples: results from forest fire ash

    SciTech Connect

    Goldstein, Steven J; Oldham, Warren J; Murrell, Michael T; Katzman, Danny

    2010-12-07

    We have measured the Pu, {sup 237}Np, {sup 241}Am, and {sup 151}Sm isotopic systematics for a set of forest fire ash samples from various locations in the western U.S. including Montana, Wyoming, Idaho, and New Mexico. The goal of this study is to develop a concordant {sup 241}Pu (t{sub 1/2} = 14.4 y)-{sup 241}Am dating method for environmental collections. Environmental samples often contain mixtures of components including global fallout. There are a number of approaches for subtracting the global fallout component for such samples. One approach is to use {sup 242}/{sup 239}Pu as a normalizing isotope ratio in a three-isotope plot, where this ratio for the nonglobal fallout component can be estimated or assumed to be small. This study investigates a new, complementary method of normalization using the long-lived fission product, {sup 151}Sm (t{sub 1/2} = 90 y). We find that forest fire ash concentrates actinides and fission products with {approx}1E10 atoms {sup 239}Pu/g and {approx}1E8 atoms {sup 151}Sm/g, allowing us to measure these nuclides by mass spectrometric (MIC-TIMS) and radiometric (liquid scintillation counting) methods. The forest fire ash samples are characterized by a western U.S. regional isotopic signature representing varying mixtures of global fallout with a local component from atmospheric testing of nuclear weapons at the Nevada Test Site (NTS). Our results also show that {sup 151}Sm is well correlated with the Pu nuclides in the forest fire ash, suggesting that these nuclides have similar geochemical behavior in the environment. Results of this correlation indicate that the {sup 151}Sm/{sup 239}Pu atom ratio for global fallout is {approx}0.164, in agreement with an independent estimate of 0.165 based on {sup 137}Cs fission yields for atmospheric weapons tests at the NTS. {sup 241}Pu-{sup 241}Am dating of the non-global fallout component in the forest fire ash samples yield ages in the late 1950's-early 1960's, consistent with a peak in NTS

  4. Temporal record of Pu isotopes in inter-tidal sediments from the northeastern Irish Sea.

    PubMed

    Lindahl, Patric; Worsfold, Paul; Keith-Roach, Miranda; Andersen, Morten B; Kershaw, Peter; Leonard, Kins; Choi, Min-Seok; Boust, Dominique; Lesueur, Patrick

    2011-11-01

    A depth profile of (239)Pu and (240)Pu specific activities and isotope ratios was determined in an inter-tidal sediment core from the Esk Estuary in the northeastern Irish Sea. The study site has been impacted with plutonium through routine radionuclide discharges from the Sellafield nuclear reprocessing plant in Cumbria, NW England. A pronounced sub-surface maximum of ~10 k Bq kg(-1) was observed for (239+240)Pu, corresponding to the peak in Pu discharge from Sellafield in 1973, with a decreasing trend with depth down to ~0.04 k Bq kg(-1) in the deeper layers. The depth profile of (239+240)Pu specific activities together with results from gamma-ray spectrometry for (137)Cs and (241)Am was compared with reported releases from the Sellafield plant in order to estimate a reliable sediment chronology. The upper layers (1992 onwards) showed higher (239+240)Pu specific activities than would be expected from the direct input of annual Sellafield discharges, indicating that the main input of Pu is from the time-integrated contaminated mud patch of the northeastern Irish Sea. The (240)Pu/(239)Pu atom ratios ranged from ~0.03 in the deepest layers to >0.20 in the sub-surface layers with an activity-weighted average of 0.181. The decreasing (240)Pu/(239)Pu atom ratio with depth reflects the changing nature of operations at the Sellafield plant from weapons-grade Pu production to reprocessing spent nuclear fuel with higher burn-up times in the late 1950s. In addition, recent annual (240)Pu/(239)Pu atom ratios in winkles collected during 2003-2008 from three stations along the Cumbrian coastline showed no significant spatial or temporal differences with an overall average of 0.204, which supports the hypothesis of diluted Pu input from the contaminated mud patch.

  5. Activities of Pu and Am isotopes and isotopic ratios in a soil contaminated by weapons-grade plutonium.

    PubMed

    Lee, M H; Clark, S B

    2005-08-01

    An accident and fire at the former McGuire Air Force Base and Boeing Michigan Aeronautical Research Center (BOMARC) site in New Jersey resulted in dispersion of weapons-grade plutonium in particulate form to the local environment. Soil samples collected at the BOMARC site were measured for their activities and isotopic ratios of Pu and Am isotopes by radioanalytical techniques. The activities of the Pu and Am isotopes in the BOMARC soil were markedly higher than fallout levels, and they decreased nearly exponentially with increasing particle size of the soil. The measured (241)Am activity was compared to calculated values based on decay of (241)Pu. The activity ratios of (238)Pu/(239,240)Pu, (241)Pu/(239,240)Pu, and (241)Am/(239,240)Pu observed in the BOMARC soil were much lower than those attributed to nuclear reprocessing plants and Chernobyl fallout. From the activity ratios of (241)Pu/(239,240)Pu and (241)Am/(239,240)Pu, the origin of the Pu isotopes was identified as weapons-grade and the time since production of the material was estimated. Furthermore, the atomic ratio of (240)Pu/(239)Pu in the BOMARC soil was remarkably lower than the fallout value influenced by nuclear weapons testing and the Chernobyl accident. The atomic ratio of (240)Pu/(239)Pu was very close to the value of the weapons-grade Pu detected from the Thule accident in Greenland. This work demonstrates the utility of radioanalytical measurements and decay calculations for defining characteristics of the source term and discriminating multiple processes that contribute to a source. Such an approach would also be needed to respond to a terrorist event involving an improvised nuclear device or radiological dispersal device.

  6. Report on 241,242Am(n,x) surrogate cross section measurement

    SciTech Connect

    Burke, J T; Ressler, J J; Gostic, J; Henderson, R A; Bernstein, L A; Escher, J E; Bleuel, D; Kritcher, A; Matoon, C; Scielzo, N D; Stoyer, M A

    2011-02-16

    The main goal of this measurement is to determine the {sup 242}Am(n,f) and {sup 241}Am(n,f) cross sections via the surrogate {sup 243}Am. Gamma-ray data was also collected for the purpose of measuring the (n,2n) cross-sections. The experiment was conducted using the STARS/LIBERACE experimental facility located at the 88 Inch Cyclotron at Lawrence Berkeley National Laboratory the first week of February 2011. A description of the experiment and status of the data analysis follow.

  7. Study of Neutron-Induced Fission Cross Sections of U, Am, and Cm at n_TOF

    NASA Astrophysics Data System (ADS)

    Milazzo, P. M.; Abbondanno, U.; Aerts, G.; Alvarez, H.; Alvarez-Velarde, F.; Andriamonje, S.; Andrzejewski, J.; Assimakopoulos, P.; Audouin, L.; Badurek, G.; Baumann, P.; Becčvář, F.; Belloni, 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.; Dillman, I.; Domingo-Pardo, C.; Dridi, W.; Duran, I.; Eleftheriadis, C.; Embid-Segura, M.; Ferrant, L.; Ferrari, A.; Ferreira-Marques, R.; Fujii, K.; Furman, W.; Goncalves, I.; Gonzalez-Romero, E.; Gramegna, F.; Guerrero, C.; Gunsing, F.; Heil, M.; Herrera-Martinez, A.; Jericha, E.; Käppeler, F.; Kadi, Y.; Karadimos, D.; Karamanis, D.; Kerveno, M.; Koehler, P.; Kossionides, E.; Krtička, M.; Lamboudis, C.; Leeb, H.; Lindote, A.; Lopes, I.; Lozano, M.; Lukic, S.; Marganiec, J.; Marrone, S.; Martinez, T.; Massimi, C.; Mastinu, P.; Mengoni, A.; Mosconi, M.; Neves, F.; Oberhummer, H.; O'Brien, S.; Pancin, J.; Papachristodoulou, C.; Paradela, C.; Patronis, N.; Pavlik, A.; Pavlopoulos, P.; Perrot, L.; Plag, R.; Plukis, A.; Poch, A.; Praena, J.; Pretel, C.; Quesada, J.; Reifarth, R.; Rubbia, C.; Rudolf, G.; Salgado, J.; Santos, C.; Sarchiapone, L.; Savvidis, I.; Stephan, C.; Tagliente, G.; Tain, J. L.; Tassan-Got, L.; Tavora, L.; Terlizzi, R.; Vannini, G.; Vaz, P.; Ventura, A.; Villamarin, D.; Vincente, M. C.; Vlachoudis, V.; Vlastou, R.; Voss, F.; Walter, S.; Wiescher, M.; Wisshak, K.

    2010-08-01

    Neutron induced fission cross sections of several isotopes have been measured at the CERN n_TOF spallation neutron facility. Between them some measurements involve isotopes (233U, 241Am, 243Am, 245Cm) relevant for applications to nuclear technologies. The n_TOF facility delivers neutrons with high instantaneous flux and in a wide energy range, from thermal up to 250 MeV. The experimental apparatus consists of an ionization chamber that discriminates fission fragments and α particles coming from natural radioactivity of the samples. All the measurements were performed referring to the standard cross section of 235U.

  8. Deconvolution of mixed gamma emitters using peak parameters

    SciTech Connect

    Gadd, Milan S; Garcia, Francisco; Magadalena, Vigil M

    2011-01-14

    When evaluating samples containing mixtures of nuclides using gamma spectroscopy the situation sometimes arises where the nuclides present have photon emissions that cannot be resolved by the detector. An example of this is mixtures of {sup 241}Am and plutonium that have L x-ray emissions with slightly different energies which cannot be resolved using a high-purity germanium detector. It is possible to deconvolute the americium L x-rays from those plutonium based on the {sup 241}Am 59.54 keV photon. However, this requires accurate knowledge of the relative emission yields. Also, it often results in high uncertainties in the plutonium activity estimate due to the americium yields being approximately an order of magnitude greater than those for plutonium. In this work, an alternative method of determining the relative fraction of plutonium in mixtures of {sup 241}Am and {sup 239}Pu based on L x-ray peak location and shape parameters is investigated. The sensitivity and accuracy of the peak parameter method is compared to that for conventional peak decovolution.

  9. Comparative analysis of (239)Pu, (137)Cs, (210)Pb and (40)K spatial distributions in the top soil layer at the Baltic coast.

    PubMed

    Luksiene, B; Druteikiene, R; Gvozdaite, R; Gudelis, A

    2006-01-01

    This paper presents the results of an investigation into the spatial distribution of radionuclides of artificial ((239,240)Pu, (137)Cs) and natural ((210)Pb, (40)K) origins in the upper (0-5 cm) soil layers on the Baltic coastline of Lithuania ( approximately 5 km(2) area). The samples were analysed by gamma ray spectrometry and combined radiochemical procedures. The highest (210)Pb, (239,240)Pu and (137)Cs activity concentrations were determined in the forest samples, whereas (40)K activity was rather homogeneous across the study area. Relatively high (239,240)Pu and (40)K activity concentrations were determined along the surf zone. The (210)Pb and (137)Cs activity concentrations showed a gradual increase from the surf zone to the forest. The average activity concentrations of (239,240)Pu, (137)Cs, (210)Pb and (40)K in the beach and forest samples, respectively, were as follows: 0.32+/-0.08 and 0.74+/-0.14; 50+/-4 and 1190+/-50; 4.7+/-2.0 and 48+/-6; 186+/-15 and 216+/-17 Bq/kg.

  10. Leaching of UO2 pellets doped with alpha-emitters (238/239Pu) in synthetic deep Callovian-Oxfordian groundwater

    NASA Astrophysics Data System (ADS)

    Tribet, M.; Jégou, C.; Broudic, V.; Marques, C.; Rigaux, P.; Gavazzi, A.

    2010-03-01

    The reactivity of a polycrystalline UO2 surface under alpha irradiation in contact with groundwater is investigated, in the hypothesis of direct disposal of spent fuel in a deep geological repository. Two series of plutonium-doped UO2 samples (specific alpha activity of 18 and 385 MBq·g-1UO2) were leached in a synthetic Callovian-Oxfordian deep groundwater under anoxic conditions (Ar/CO2 3000 ppm, 3.5 bar relative pressure) to assess both the impact of alpha radiolysis of water and the complexing capacity of the groundwater ions on the dissolution of UO2. This study follows a prior one performed in pure and carbonated waters. Firstly, technical developments were necessary for the analyses in the groundwater solution because of its high salt concentrations: quantification limits were determined for the measurement of uranium and radiolytic H2O2 traces in this medium. Secondly, given the very high reactivity of these samples in the presence of air and in order to minimize any prior surface oxidation, a strict experimental protocol was followed, based on high-temperature annealing in Ar + 4% H2 with preleaching cycles. Each type of UO2 pellet was then leached under static conditions for 30 days (anoxic conditions, deep groundwater solutions). Results on the evolution of uranium releases are presented. For the lowest alpha activity (18 MBq·g-1UO2), uranium releases in groundwater were below the quantification limit of 2 × 10-8 mol·L-1 with a kinetic phosphorescence analyzer, even after 30 days. However, for higher alpha activity (385 MBq·g-1UO2) the uranium releases begin to exceed the quantification limit after 14 days of leaching and then increase exponentially. This increase is comparable to results previously obtained in carbonated solutions.

  11. On the similarity of 239Pu α-activity histograms when the angular velocities of the Earth diurnal rotation, orbital movement and rotation of collimators are equalized

    NASA Astrophysics Data System (ADS)

    Shnoll, S. E.; Rubinstein, I. A.; Shapovalov, S. N.; Tolokonnikova, A. A.; Shlektaryov, V. A.; Kolombet, V. A.; Kondrashova, M. N.

    2016-01-01

    It was shown earlier that the persistent "scatter" of results of measurements of any nature is determined by the diurnal and orbital movement of the Earth. The movement is accompanied by "macroscopic fluctuations" (MF)—regular, periodic changes in the shape of histograms, spectra of fluctuation amplitudes of the measured parameters. There are two near-daily periods ("sidereal", 1436 min; and "solar", 1440 min) and three yearly ones ("calendar", 365 average solar days; "tropical", 365 days 5 h and 48 min; and "sidereal", 365 days 6 h and 9 min). This periodicity was explained by the objects whose parameters are measured passing through the same spatial-temporal heterogeneities as the Earth rotates and shifts along its orbit.

  12. U, Pu, and Am nuclear signatures of the Thule hydrogen bomb debris.

    PubMed

    Eriksson, Mats; Lindahl, Patric; Roos, Per; Dahlgaard, Henning; Holm, Elis

    2008-07-01

    This study concerns an arctic marine environment that was contaminated by actinide elements after a nuclear accident in 1968, the so-called Thule accident In this study we have analyzed five isolated hot particles as well as sediment samples containing particles from the weapon material for the determination of the nuclear fingerprint of the accident. We report that the fissile material in the hydrogen weapons involved in the Thule accident was a mixture of highly enriched uranium and weapon-grade plutonium and that the main fissile material was 235U (about 4 times more than the mass of 239Pu). In the five hot particles examined, the measured uranium atomic ratio was 235U/238U = 1.02 +/- 0.16 and the Pu-isotopic ratios were as follows: 24Pu/239Pu = 0.0551 +/- 0.0008 (atom ratio), 238Pu/239+240Pu = 0.0161 +/- 0.0005 (activity ratio), 241Pu/239+240Pu = 0.87 +/- 0.12 (activity ratio), and 241Am/ 239+240Pu = 0.169 +/- 0.005 (activity ratio) (reference date 2001-10-01). From the activity ratios of 241Pu/241Am, we estimated the time of production of this weapon material to be from the late 1950s to the early 1960s. The results from reanalyzed bulk sediment samples showed the presence of more than one Pu source involved in the accident, confirming earlier studies. The 238Pu/239+240PU activity ratio and the 240Pu/ 239Pu atomic ratio were divided into at least two Pu-isotopic ratio groups. For both Pu-isotopic ratios, one ratio group had identical ratios as the five hot particles described above and for the other groups the Pu isotopic ratios were lower (238Pu/ 239+240PU activity ratio approximately 0.01 and the 240Pu/P239Pu atomic ratio 0.03). On the studied particles we observed that the U/Pu ratio decreased as a function of the time these particles were present in the sediment. We hypothesis that the decrease in the ratio is due to a preferential leaching of U relative to Pu from the particle matrix.

  13. Radionuclide Contaminant Analysis of Small Mammals at Area G, Technical Area 54, 1997 (with cumulative summary 1994-1997)

    SciTech Connect

    James R. Biggs; Kathryn D. Bennett; P. R. Fresquez

    1998-12-01

    In 1997, small mammals were sampled at four locations at Area G, Technical Area 54, a control site within the proposed Area G expansion area, and a background site on Frijoles Mesa. The purpose of the sampling was to (1) identify radionuclides that are present within rodent tissues at waste burial sites, (2) compare the amount of radionuclide uptake by small mammals at waste burial sites to a control site, and (3) identifi the primary mode of contamination to small mammals, either through surface contact or ingestion/inhalation. Three composite samples of approximately five animals per sample were collected at each site. Pelts and carcasses of each animal were separated and analyzed independently. Samples were analyzed for 241Am, 90Sr, 238Pu, 239Pu, total U, 137Cs, and 3H. Higher levels of total U and 137CS were detected in pelts as compared to the carcasses of small mammals, and 90Sr was found to be higher in carcasses. Concentrations of other measured radionuclides in carcasses were not found to be statistically different (p< 0.05) from that measured in pelts. However, pelts generally had higher concentrations than carcasses, indicating surface contamination may be the primary contamination mode. Low sample sizes in total number of animals captured during 1997 prevented statistical analysis to compare site to site to all but four sites. Mean concentrations of 241Am, 238Pu, 239Pu, and 3H in small mammal carcasses were found to be statistically greater at the transuranic (TRU) waste pad #2. In addition, mean concentrations of total U, ~lAm, and 3H in pelts of small mammals were also statistically greater. The Control Site and Background Site consistently had the lowest mean concentrations of radionuclides. Year to year comparison of mean radionuclide concentrations was conducted where suftlcient sample size existed. We found 241Am, 238Pu, 239Pu, and 3H mean concentrations in carcasses to be statistically greater in 1997 than previous years at TRU waste pad #2

  14. Interaction of Fast Nucleons with Actinide Nuclei Studied with GEANT4

    NASA Astrophysics Data System (ADS)

    Malyshkin, Yu.; Pshenichnov, I.; Mishustin, I.; Greiner, W.

    2014-04-01

    We model interactions of protons and neutrons with energies from 1 to 1000 MeV with 241Am and 243Am nuclei. The calculations are performed with the Monte Carlo model for Accelerator Driven Systems (MCADS) which we developed based on the GEANT4 toolkit of version 9.4. This toolkit is widely used to simulate the propagation of particles in various materials which contain nuclei up to uranium. After several extensions we apply this toolkit also to proton- and neutron-induced reactions on Am. The fission and radiative neutron capture cross sections, neutron multiplicities and distributions of fission fragments were calculated for 241Am and 243Am and compared with experimental data. As demonstrated, the fission of americium by energetic protons with energies above 20 MeV can be well described by the Intra-Nuclear Cascade Liège (INCL) model combined with the fission-evaporation model ABLA. The calculated average numbers of fission neutrons and mass distributions of fission products agree well with the corresponding data. However, the proton-induced fission below 20 MeV is described less accurately. This is attributed to the limitations of the Intra-Nuclear Cascade model at low projectile energies.

  15. Use of in vivo counting measurements to estimate internal doses from (241)Am in workers from the Mayak production association.

    PubMed

    Sokolova, Alexandra B; Suslova, Klara G; Efimov, Alexander V; Miller, Scott C

    2014-08-01

    Comparisons between results of in vivo counting measurements of americium burden and results from radiochemical analyses of organ samples taken at autopsy of 11 cases of former Mayak workers were made. The in vivo counting measurements were performed 3-8 y before death. The best agreement between in vivo counting measurements for americium and autopsy data was observed for the skull. For lungs and liver, the ratios of burden measured by in vivo counting to those obtained from radiochemical analyses data ranged from 0.7-3.8, while those for the skull were from 1.0-1.1. There was a good correlation between the estimates of americium burden in the entire skeleton obtained from in vivo counting with those obtained from autopsy data. Specifically, the skeletal burden ratio, in vivo counting/autopsy, averaged 0.9 ± 0.1. The prior human americium model, D-Am2010, used in vivo counting measurements for americium in the skeleton to estimate the contents of americium and plutonium at death. The results using this model indicate that in vivo counting measurements of the skull can be used to estimate internal doses from americium in the Mayak workers. Additionally, these measurements may also be used to provide a qualitative assessment of internal doses from plutonium.

  16. LITERATURE REVIEW ON MAXIMUM LOADING OF RADIONUCLIDES ON CRYSTALLINE SILICOTITANATE

    SciTech Connect

    Adu-Wusu, K.; Pennebaker, F.

    2010-10-13

    Plans are underway to use small column ion exchange (SCIX) units installed in high-level waste tanks to remove Cs-137 from highly alkaline salt solutions at Savannah River Site. The ion exchange material slated for the SCIX project is engineered or granular crystalline silicotitanate (CST). Information on the maximum loading of radionuclides on CST is needed by Savannah River Remediation for safety evaluations. A literature review has been conducted that culminated in the estimation of the maximum loading of all but one of the radionuclides of interest (Cs-137, Sr-90, Ba-137m, Pu-238, Pu-239, Pu-240, Pu-241, Am-241, and Cm-244). No data was found for Cm-244.

  17. Atmospheric transport of radionuclides emitted due to wildfires near the Chernobyl Nuclear Power Plant in 2015

    NASA Astrophysics Data System (ADS)

    Evangeliou, Nikolaos; Zibtsev, Sergey; Myroniuk, Viktor; Zhurba, Marina; Hamburger, Thomas; Stohl, Andreas; Balkanski, Yves; Paugam, Ronan; Mousseau, Timothy A.; Møller, Anders P.; Kireev, Sergey I.

    2016-04-01

    In 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) have caused concerns about the secondary radioactive contamination that might have spread over Europe. The total active burned area was estimated to be about 15,000 hectares, of which 9000 hectares burned in April and 6000 hectares in August. The present paper aims to assess, for the first time, the transport and impact of these fires over Europe. For this reason, direct observations of the prevailing deposition levels of 137Cs and 90Sr, 238Pu, 239Pu, 240Pu and 241Am in the CEZ were processed together with burned area estimates. Based on literature reports, we made the conservative assumption that 20% of the deposited labile radionuclides 137Cs and 90Sr, and 10% of the more refractory 238Pu, 239Pu, 240Pu and 241Am, were resuspended by the fires. We estimate that about 10.9 TBq of 137Cs, 1.5 TBq of 90Sr, 7.8 GBq of 238Pu, 6.3 GBq of 239Pu, 9.4 GBq of 240Pu and 29.7 GBq of 241Am were released from both fire events. These releases could be classified as of "Level 3" on the relative INES (International Nuclear Events Scale) scale, which corresponds to a serious incident, in which non-lethal deterministic effects are expected from radiation. To simulate the dispersion of the resuspended radionuclides in the atmosphere and their deposition onto the terrestrial environment, we used a Lagrangian dispersion model. Spring fires redistributed radionuclides over the northern and eastern parts of Europe, while the summer fires also affected Central and Southern Europe. The more labile elements escaped more easily from the CEZ and then reached and deposited in areas far from the source, whereas the larger refractory particles were removed more efficiently from the atmosphere and thus did mainly affect the CEZ and its vicinity. For the spring 2015 fires, we estimate that about 80% of 137Cs and 90Sr and about 69% of 238Pu, 239Pu, 240Pu and 241Am were deposited over areas outside the CEZ. 93% of the labile and 97% of

  18. Baseline concentrations of radionuclides and heavy metals in soils and vegetation around the DARHT facility: Construction phase (1996)

    SciTech Connect

    Fresquez, P.R.; Haagenstad, H.T.; Naranjo, L. Jr.

    1997-04-01

    As part of the Department of Energy`s Mitigation Action Plan for the Dual Axis Radiographic Hydrodynamic Test (DARHT) Facility at Los Alamos National Laboratory (LANL), baseline concentrations of radionuclides ({sup 3}H, {sup 137}Cs, {sup 90}Sr, {sup 238}Pu, {sup 239}Pu, {sup 241}Am, total U), and heavy metals (Ag, As, Ba, Be, Cd, Cr, Cu, Hg, Ni, Pb, Sb, Se and Tl) in soil, sediment, and vegetation (overstory and understory) around the DARHT facility during the construction phase in 1996 were determined. Also, U and Be concentrations in soil samples collected in 1993 from within the proposed DARHT facility area are reported. Most radionuclides in soils, sediments, and vegetation were within current background and/or long-term regional statistical reference levels.

  19. Urine Radiobioassay Intercomparison Results From The Intercomparison Studies Program At Oak Ridge National Laboratory

    SciTech Connect

    Bores, Norman; Schultz, Michael K

    2008-01-01

    The Intercomparison Studies Program (ISP) at the Oak Ridge National Laboratory (ORNL, Oak Ridge, TN USA) provides natural-matrix human urine quality-assurance/quality-control (QA/QC) samples to radiobioassay analysis laboratories. Samples are provided to these laboratories as 'single-blind' or 'double-blind' unknowns, spiked with radioactive-solution standards at 'low' levels (e.g., 0-250 mBq {center_dot} kg{sup -1} for alpha-emitters). Participants use the results as a tool for self-evaluation and a measure of performance. In this paper, sample preparation and the results of testing during the years 2000-2004 for the radionuclides natural uranium (U-nat), {sup 238}Pu, {sup 239}Pu, and {sup 241}Am are presented and discussed.

  20. The Am-243 Neutron Capture Measurement at the n_TOF Facility

    NASA Astrophysics Data System (ADS)

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

    2013-03-01

    The 243Am neutron capture cross section has been measured at the n_TOF facility1 in the 0.7 eV-2 keV energy range. The n_TOF Total Absorption Calorimeter2 (TAC) composed by 40 BaF2 crystals has been used in the measurement for detecting the electromagnetic cascades produced in the 243Am(n, γ) reactions. All current evaluations in the resolved resonance region are based essentially in fission measurements and in only one transmission measurement.3 The analysis of the measurement has been finished recently, and it is ready for its distribution to the EXFOR nuclear database. In addition, the data obtained with the TAC provide valuable information on the level density in the compound nucleus 244Am and on its electromagnetic de-excitation scheme. In particular, the 243Am data will be combined with data from previous measurements of 241Am, 240Pu, 237Np and 233,234,236U and with future measurements of 235,238U for a systematic investigation of the photon strength functions in actinides.

  1. Systematic evaluation of options to avoid generation of noncertifiable transuranic (TRU) waste at Los Alamos National Laboratory

    SciTech Connect

    Boak, J.M.; Kosiewicz, S.T.; Triay, I.; Gruetzmacher, K.; Montoya, A.

    1998-03-01

    At present, >35% of the volume of newly generated transuranic (TRU) waste at Los Alamos National Laboratory is not certifiable for transport to the Waste Isolation Pilot Plant (WIPP). Noncertifiable waste would constitute 900--1,000 m{sup 3} of the 2,600 m{sup 3} of waste projected during the period of the Environmental Management (EM) Accelerated Cleanup: Focus on 2006 plan (DOE, 1997). Volume expansion of this waste to meet thermal limits would increase the shipped volume to {approximately}5,400 m{sup 3}. This paper presents the results of efforts to define which TRU waste streams are noncertifiable at Los Alamos, and to prioritize site-specific options to reduce the volume of certifiable waste over the period of the EM Accelerated Cleanup Plan. A team of Los Alamos TRU waste generators and waste managers reviewed historic generation rates and thermal loads and current practices to estimate the projected volume and thermal load of TRU waste streams for Fiscal Years 1999--2006. These data defined four major problem TRU waste streams. Estimates were also made of the volume expansion that would be required to meet the permissible wattages for all waste. The four waste streams defined were: (1) {sup 238}Pu-contaminated combustible waste from production of Radioactive Thermoelectric Generators (RTGs) with {sup 238}Pu activity which exceeds allowable shipping limits by 10--100X. (2) {sup 241}Am-contaminated cement waste from plutonium recovery processes (nitric and hydrochloric acid recovery) are estimated to exceed thermal limits by {approximately}3X. (3) {sup 239}Pu-contaminated combustible waste, mainly organic waste materials contaminated with {sup 239}Pu and {sup 241}Am, is estimated to exceed thermal load requirements by a factor of {approximately}2X. (4) Oversized metal waste objects, (especially gloveboxes), cannot be shipped as is to WIPP because they will not fit in a standard waste box or drum.

  2. Distributions of Pu isotopes in seawater and bottom sediments in the coast of the Japanese archipelago before and soon after the Fukushima Dai-ichi Nuclear Power Station accident.

    PubMed

    Oikawa, Shinji; Watabe, Teruhisa; Takata, Hyoe

    2015-04-01

    A radioactivity measurement survey was carried out from 24 April 2008 to 3 June 2011 to determine the levels of plutonium isotopes and (240)Pu/(239)Pu atom ratios in the marine environments off the sites of commercial nuclear power stations around the Japanese islands; the sampling period extended to two months after the Fukushima Dai-ichi Nuclear Power Station accident. In our previous study (Oikawa et al., 2015), data on Pu isotopes and (241)Am in sediments have already been reported. In this study, we report those on Pu isotopes in seawater as well as sediments, and the characteristics of sediments in addition (e.g., ignition loss and biogenic opals). Concentrations of (239+240)Pu in seawater and bottom sediments remained nearly constant at all sampling locations during the survey period. In addition, no regional differences were observed in the (239+240)Pu concentrations in surface waters. Higher (239+240)Pu concentrations were found in bottom waters at deeper sampling locations, but the (240)Pu/(239)Pu atom ratios were nearly constant regardless of the water depth. Higher (239+240)Pu concentrations were also found in bottom sediments at deeper sampling locations, but vice versa for (240)Pu/(239)Pu atom ratios as reported in the previous report. The sediments samples from deeper locations showed the higher percentage of ignition loss as well as the higher content of biogenic opal. There was likely to be some driving force participating in the transfer of Pu isotopes associated with biogenic substances to the deeper seabed. The present survey showed that the accident at the Fukushima Dai-ichi Nuclear Power Station did not contribute much to the inventory of Pu isotopes in the adjacent sea area.

  3. Analytical method for the determination of Np and Pu in sea water by AMS with respect to the Fukushima accident

    NASA Astrophysics Data System (ADS)

    Hain, K.; Faestermann, T.; Famulok, N.; Fimiani, L.; Gómez-Guzmán, J. M.; Korschinek, G.; Kortmann, F.; Lierse v. Gostomski, Ch.; Ludwig, P.; Shinonaga, T.

    2015-10-01

    A chemical separation procedure for plutonium (Pu) and neptunium (Np) was developed using extraction chromatography, mass spectrometry and radiometric analysis to determine their concentrations and isotopic ratios in sea water. 241Am, which causes isobaric background to 241Pu in mass spectrometric measurements, was successfully separated from the Pu fraction by this method. Water samples which were spiked with 242Pu and 237Np or 239Np, respectively, were used for chemical yield determination. The chemical yields of Pu and Np, which were determined by alpha and gamma spectrometry at the Radiochemie München (RCM), of more than 85% were obtained. The developed method was applied to analyze the concentration of Pu and Np in the certified reference material, IAEA-443, by Accelerator Mass Spectrometry (AMS) at the Maier-Leibnitz-Laboratory (MLL) to check the applicability of the method to sea water samples. The concentrations of 240Pu, 241Pu and 237Np obtained in this study are in agreement with the certified and literature values within the uncertainties. Due to strong isotopic interference of 239Pu with 238U, it was not possible to analyze the concentration of 239Pu. Some modifications of the chemical separation method to suppress the uranium (U) fraction are under consideration. This method can be used for the analysis of Pu and Np in Pacific Ocean water samples collected after the Fukushima accident.

  4. Ageing of a phosphate ceramic used to immobilize chloride contaminated actinide waste

    SciTech Connect

    Metcalfe, Brian L.; Donald, Ian W.; Fong, Shirley K.; Gerrard, Lee A.; Strachan, Denis M.; Scheele, Randall D.

    2009-03-31

    AWE has developed a process for the immobilization of ILW waste containing a significant quantity of chloride using Ca3(PO4)2 as the host material. Waste ions are incorporated into two phosphate based phases, chlorapatite, Ca5(PO4)3Cl, and spodiosite, Ca2(PO4)Cl. Non-active trials performed at AWE using samarium as the actinide surrogate demonstrated the durability of these phases in aqueous solution. Trials of the process using actinide-doped material were performed at PNNL which confirmed the immobilized wasteform resistant to aqueous leaching. Initial leach trials conducted on 239Pu /241Am loaded ceramic at 40°C/28 days gave normalized mass losses of 1.2 x 10-5 g.m-2 and 2.7 x 10-3 g.m-2 for Pu and Cl respectively. In order to assess the response of the phases to radiation-induced damage, accelerated ageing trials were performed on samples in which the 239Pu was replaced by 238Pu. No changes to the crystalline structure of the waste were detected using XRD after the samples had experienced a radiation dose of 4 x 1018 α.g-1. Leach trials showed that there had been an increase in the P and Ca release rates but no change in the Pu release rate.

  5. Radionuclide transfer to marine biota species: review of Russian language studies.

    PubMed

    Fesenko, S; Fesenko, E; Titov, I; Karpenko, E; Sanzharova, N; Fonseca, A Gondin; Brown, J

    2010-11-01

    An extensive programme of experiments on transfer of radionuclides to aquatic species was conducted in the former USSR starting from the early 1950s. Only a few of these studies were made available in the English language literature or taken into account in international reviews of radionuclide behaviour in marine ecosystems. Therefore, an overview of original information on radionuclide transfer to marine biota species available from Russian language literature sources is presented here. The concentration ratio (CR) values for many radionuclides and for marine species such as: (239)Pu, (106)Ru and (95)Zr (crustacean), (54)Mn, (90)Sr, (95)Nb, (106)Ru, (137)Cs (239)Pu, (241)Am and natural U (molluscs), and (54)Mn, (90)Sr, (137)Cs and (144)Ce (fish) are in good agreement with those previously published, whilst for some of them, in particular, for (32)P and (110)Ag (crustaceans), (35)S (molluscs), (32)P, (35)S, (95)Nb, and (106)Ru (macroalgae) and (60)Co and (239,240)Pu (fish) the data presented here suggest that changes in the default CR reference values presented in recent marine reviews may be required. The data presented here are intended to supplement substantially the CR values being collated within the handbook on Wildlife Transfer Coefficients, coordinated under the IAEA EMRAS II programme.

  6. Conversion electron spectrometry of Pu isotopes with a silicon drift detector.

    PubMed

    Pommé, S; Paepen, J; Peräjärvi, K; Turunen, J; Pöllänen, R

    2016-03-01

    An electron spectrometry set-up was built at IRMM consisting of a vacuum chamber with a moveable source holder and windowless Peltier-cooled silicon drift detector (SDD). The SDD is well suited for measuring low-energy x rays and electrons emitted from thin radioactive sources with low self-absorption. The attainable energy resolution is better than 0.5keV for electrons of 30keV. It has been used to measure the conversion electron spectra of three plutonium isotopes, i.e. (238)Pu, (239)Pu, (240)Pu, as well as (241)Am (being a decay product of (241)Pu). The obtained mixed x-ray and electron spectra are compared with spectra obtained with a close-geometry set-up using another SDD in STUK and spectra measured with a Si(Li) detector at IRMM. The potential of conversion electron spectrometry for isotopic analysis of mixed plutonium samples is investigated. With respect to the (240)Pu/(239)Pu isotopic ratio, the conversion electron peaks of both isotopes are more clearly separated than their largely overlapping peaks in alpha spectra.

  7. Vertical migration of radionuclides in the vicinity of the chernobyl confinement shelter.

    PubMed

    Bondarkov, Mikhail D; Zheltonozhsky, Viktor A; Zheltonozhskaya, Maryna V; Kulich, Nadezhda V; Maksimenko, Andrey M; Farfán, Eduardo B; Jannik, G Timothy; Marra, James C

    2011-10-01

    Studies of vertical migration of Chernobyl-origin radionuclides in the 5-km zone of the Chernobyl Nuclear Power Plant (ChNPP) in the area of the Red Forest experimental site were completed. Measurements were made by gamma spectrometric methods using high purity germanium (HPGe) detectors with beryllium windows. Alpha-emitting isotopes of plutonium were determined by the measurement of the x-rays from their uranium progeny. The presence of 60Co, 134,137Cs, 154,155Eu, and 241Am in all soil layers down to a depth of 30 cm was observed. The presence of 137Cs and 241Am was noted in the area containing automorphous soils to a depth of 60 cm. In addition, the upper soil layers at the test site were found to contain 243Am and 243Ñm. Over the past 10 years, the 241Am/137Cs ratio in soil at the experimental site has increased by a factor of 3.4, nearly twice as much as would be predicted based solely on radioactive decay. This may be due to "fresh" fallout emanating from the ChNPP Confinement Shelter.

  8. VERTICAL MIGRATION OF RADIONUCLIDES IN THE VICINITY OF THE CHERNOBYL CONFINEMENT SHELTER

    SciTech Connect

    Farfan, E.; Jannik, T.; Marra, J.

    2011-10-01

    Studies on vertical migration of Chernobyl-origin radionuclides in the 5-km zone of the Chernobyl Nuclear Power Plant (ChNPP) in the area of the Red Forest experimental site were completed. Measurements were made by gamma spectrometric methods using high purity germanium (HPGe) detectors with beryllium windows. Alpha-emitting isotopes of plutonium were determined by the measurement of the x-rays from their uranium progeny. The presence of {sup 60}Co, {sup 134,137}Cs, {sup 154,155}Eu, and {sup 241}Am in all soil layers down to a depth of 30 cm was observed. The presence of {sup 137}Cs and {sup 241}Am were noted in the area containing automorphous soils to a depth of 60 cm. In addition, the upper soil layers at the test site were found to contain {sup 243}Am and {sup 243}Cm. Over the past ten years, the {sup 241}Am/{sup 137}Cs ratio in soil at the experimental site has increased by a factor of 3.4, nearly twice as much as would be predicted based solely on radioactive decay. This may be due to 'fresh' fallout emanating from the ChNPP Confinement Shelter.

  9. Air Monitoring Leads to Discovery of New Contamination at Radioactive Waste Disposal Site (Area G) at LANL

    SciTech Connect

    Kraig, D.H.; Conrad, R.C.

    1999-06-08

    Air monitoring at Area G, the low-level radioactive waste disposal area at Los Alamos National Laboratory, revealed increased air concentrations of {sup 239}Pu and {sup 241}Am at one location along the north boundary. This air monitoring location is a couple of meters north of a dirt road used to access the easternmost part of Area G. Air concentrations of {sup 238}Pu were essentially unaffected, which was puzzling because the {sup 238}Pu and {sup 239}Pu are present in the local, slightly contaminated soils. Air concentrations of these radionuclides increased about a factor of ten in early 1995 and remained at those levels until the first quarter of 1996. During the spring of 1996 air concentrations again increased by a factor of about ten. No other radionuclides were elevated and no other Area G stations showed elevations of these radionuclides. After several formal meetings didn't provide an adequate cause for the elevations, a gamma survey was performed and showed a small area of significant contamination just south of the monitor location. We found in February, 1995, a trench for a water line had been dug within a meter of so of the air stations. Then, during early 1996, the dirt road was rerouted such that its new path was directly over the unknown contamination. It appears that the trenching brought contaminated material to the surface and caused the first rise in air concentrations and then the rerouting of the road over the contamination caused the second rise, during 1996. We also found that during 1976 and 1977 contaminated soils from the clean-up of an old processing facility had been spread over the filled pits in the vicinity of the air monitors. These soils were very low in 238Pu which explains why we saw very little {sup 238}Pu in the increased air concentrations. A layer of gravel and sand was spread over the contaminated area. Although air concentrations of {sup 239}Pu and {sup 241}Am dropped considerably, the y have not returned to pre-1995 levels.

  10. Comparative skeletal distribution of americium and plutonium in man, monkey and baboon

    SciTech Connect

    Lynch, T.P.; Dagle, G.E.; Kathren, R.L.; McInroy, J.F.

    1988-10-01

    The skeletal distributions of americium and plutonium in four humans were compared with the skeletal distributions of these radioelements in baboons and monkeys. With respect to the skeletal distribution of these elements, excellent agreement was noted among the four human cases; americium data was available for all four cases and plutonium for three. The human case database was thus adequate for comparison with those of other primates. A statistically significant correlation was found between the /sup 241/Am and /sup 239/Pu + /sup 240/Pu skeletal distributions in the humans and those in non-human primates. Trabecular bone had the highest concentrations of /sup 241/Am and /sup 239 +240/Pu in man, baboon, and monkey. Scaling factors are proposed to convert the percentages of skeletal activity in animal bones to the corresponding percentages in the bones of the human skeleton. However, considerable variation was found between the humans and animals in the percentages of the skeletal activity found in the same bone. 12 refs., 7 tabs.

  11. Mechanical environmental transport of actinides and ¹³⁷Cs from an arid radioactive waste disposal site.

    PubMed

    Snow, Mathew S; Clark, Sue B; Morrison, Samuel S; Watrous, Matthew G; Olson, John E; Snyder, Darin C

    2015-10-01

    Aeolian and pluvial processes represent important mechanisms for the movement of actinides and fission products at the Earth's surface. Soil samples taken in the early 1970's near a Department of Energy radioactive waste disposal site (the Subsurface Disposal Area, SDA, located in southeastern Idaho) provide a case study for studying the mechanisms and characteristics of environmental actinide and (137)Cs transport in an arid environment. Multi-component mixing models suggest actinide contamination within 2.5 km of the SDA can be described by mixing between 2 distinct SDA end members and regional nuclear weapons fallout. The absence of chemical fractionation between (241)Am and (239+240)Pu with depth for samples beyond the northeastern corner and lack of (241)Am in-growth over time (due to (241)Pu decay) suggest mechanical transport and mixing of discrete contaminated particles under arid conditions. Occasional samples northeast of the SDA (the direction of the prevailing winds) contain anomalously high concentrations of Pu with (240)Pu/(239)Pu isotopic ratios statistically identical to those in the northeastern corner. Taken together, these data suggest flooding resulted in mechanical transport of contaminated particles into the area between the SDA and a flood containment dike in the northeastern corner, following which subsequent contamination spreading in the northeastern direction resulted from wind transport of discrete particles.

  12. Sedimentation and mixing rates of radionuclides in Barents Sea sediments off Novaya Zemlya

    NASA Astrophysics Data System (ADS)

    Smith, J. N.; Ellis, K. M.; Naes, K.; Dahle, S.; Matishov, D.

    Radionuclide measurements have been conducted on sediment cores collected in 1992 in the south-eastern region of the Barents Sea, known as the Pechora Sea. Cesium-137 and 239,24OPu activities in surface sediments are generally less than 30 Bq/kg, with the highest levels being measured in sediments off the southwestern coastline of the island of Novaya Zemlya. High correlations between both 137Cs and 239,24OPu and the concentration of fine (< 63 μm) particles in surface sediments indicate that much of the variance in radionuclide concentrations throughout the Pechora Sea can be explained by particle size fractionation. However, elevated activities of 137Cs (138 Bq/kg), 60Co (92 Bq/kg), 241Am (433 Bq/kg), and especially 239,24OPu (8.47 × 103 Bq/kg) were measured in one surface sediment sample from the fjord of Chernaya Bay on the southern coast of Novaya Zemlya. The source of radioactive contamination is two underwater nuclear tests conducted in Chernaya Bay in 1955 and 1957. The 238Pu /239,240Vu activity ratio of 0.0245 in Chernaya Bay is equivalent to values measured in global fallout. The 240Pu /239Pu atom ratio (0.0304), measured by mass spectrometry, is much lower than values (0.18) typical of global fallout, but is consistent with ratios measured for fallout from the early (1951-1955) series of weapons tests at the Nevada Test Site. The timing of the Chernaya Bay source term, estimated from the 241Am /241Pu ratio, is consistent with the timing of the 1955 and 1957 underwater nuclear tests. Relatively low initial yields of 241Pu ( 241Pu /239Pu atom ratio = 0.00 123) in these tests have resulted in relatively low 241Am /239,240Pu activity ratios (0.05) in recent sediments in Chernaya Bay. Radionuclide tracer profiles in cores from the Pechora Sea can be simulated using a two-layer biodiffusion model with rapid, near-homogeneous mixing in the surface mixed layer and reduced mixing in the deep layer. Lead-210 profiles are consistent with a wide range of

  13. The influence of radioactive decay on actinide magnetic susceptibility measurements obtained using the Evans method.

    PubMed

    Autillo, Matthieu; Kaden, Peter; Geist, Andreas; Guerin, Laetitia; Moisy, Philippe; Berthon, Claude

    2014-05-14

    In order to explain the higher magnetic susceptibility of some aquo actinide ions than predicted by Hund's rules, the molar magnetic susceptibilities of two americium isotopes ((241)Am and (243)Am) were measured using the Evans method. The results obtained show a growing change in the magnetic susceptibility with α and also a β(-) activity increase in solution. β(-) particle effects appear to be stronger than radicals formed by α particles on the experimental values. The temperature dependence of Am(iii) magnetic susceptibility has been observed but from experiments carried out here, it appears to be difficult to prove whether this effect arises from radicals or β(-). Finally, magnetic susceptibilities of americium recorded in different media (HClO4, HCl, and HNO3) have been compared to alpha and beta emissions' impact.

  14. ANDES Measurements for Advanced Reactor Systems

    NASA Astrophysics Data System (ADS)

    Plompen, A. J. M.; Hambsch, F.-J.; Kopecky, S.; Nyman, M.; Rouki, C.; Salvador Castiñeira, P.; Schillebeeckx, P.; Belloni, F.; Berthoumieux, E.; Gunsing, F.; Lampoudis, C.; Calviani, M.; Guerrero, C.; Cano-Ott, D.; Gonzalez Romero, E.; Aïche, M.; Jurado, B.; Mathieu, L.; Derckx, X.; Farget, F.; Rodrigues Tajes, C.; Bacquias, A.; Dessagne, Ph.; Kerveno, M.; Borcea, C.; Negret, A.; Colonna, N.; Goncalves, I.; Penttilä, H.; Rinta-Antila, S.; Kolhinen, V. S.; Jokinen, A.

    2014-05-01

    A significant number of new measurements was undertaken by the ANDES “Measurements for advanced reactor systems” initiative. These new measurements include neutron inelastic scattering from 23Na, Mo, Zr, and 238U, neutron capture cross sections of 238U, 241Am, neutron induced fission cross sections of 240Pu, 242Pu, 241Am, 243Am and 245Cm, and measurements that explore the limits of the surrogate technique. The latter study the feasibility of inferring neutron capture cross sections for Cm isotopes, the neutron-induced fission cross section of 238Pu and fission yields and fission probabilities through full Z and A identification in inverse kinematics for isotopes of Pu, Am, Cm and Cf. Finally, four isotopes are studied which are important to improve predictions for delayed neutron precursors and decay heat by total absorption gamma-ray spectrometry (88Br, 94Rb, 95Rb, 137I). The measurements which are performed at state-of-the-art European facilities have the ambition to achieve the lowest possible uncertainty, and to come as close as is reasonably achievable to the target uncertainties established by sensitivity studies. An overview is presented of the activities and achievements, leaving detailed expositions to the various parties contributing to the conference.

  15. Sequential isotopic determination of plutonium, thorium, americium, strontium and uranium in environmental and bioassay samples.

    PubMed

    Wang, Jeng-Jong; Chen, Ing-Jane; Chiu, Jih-Hung

    2004-01-01

    A procedure has been developed to provide sequential analysis of 238Pu, 230Th, 241Am, 238U, and 90Sr in environmental and bioassay samples. Tracers and/or carriers (242Pu, 243Am, 232U, and stable strontium) are added into the sample as chemical yield monitors, and then, plutonium, thorium, strontium, americium, and uranium are sequentially separated and purified by Dowex ion-exchange resin, EiChroM Sr-resin, EiChroM TRU-resin, and Chelate-100 resin, respectively. The radioactivities of 90Sr and the actinides are measured using the liquid scintillation counter and alpha-particle spectrometer, respectively. Acidified water, glass-fiber air filter, soil, synthetic urine and synthetic feces samples of US National Institute of Standard and Technology Radiochemical Intercomparison Program(NRIP) were analyzed to verify this method. All the analytical results of 238Pu, 230Th, 90Sr, 241Am and 238U meet the traceability limit per ANSI N42.22, and when appropriate, evaluation of radiobioassay measurement bias and precision per ANSI N13.30.

  16. Evaluation of (241)Am deposited in different parts of the leg bones and skeleton to justify in vivo measurements of the knee for estimating total skeletal activity.

    PubMed

    Khalaf, Majid; Brey, Richard R; Derryberry, DeWayne

    2013-01-01

    The percentage of Am deposited in different parts of leg bones relative to the total leg activity was calculated from radiochemical analysis results from six whole body donors participating in the U.S. Transuranium and Uranium Registries (USTUR). In five of these six USTUR cases, the percentage of Am deposited in the knee region as well as in the entire leg was separately calculated relative to total skeletal activity. The purpose of this study is to find a region in the leg that is both suitable for in vivo measurement of Am deposited in the bones and has a good correlation with the total skeletal Am burden. In all analyzed cases, the femur was the bone with the highest percentage of Am deposited in the leg (48.8%). In the five cases that have complete whole skeletal analysis, the percentage of Am activity in the knee relative to entire skeletal activity was 4.8%, and the average value of its coefficient of variation was 10.6%. The percentage of Am in the leg relative to total skeletal activity was 20% with an average coefficient of variation of 13.63%. The Am activity in the knee as well as in the leg was strongly correlated (R = 99.5% and R = 99.1%, respectively) with the amount of Am activity in the entire skeleton using a simple linear relationship. The highest correlation was found between the amount of Am deposited in the knee and the amount of Am deposited in the entire skeleton. This correlation is important because it might enable an accurate assessment of the total skeletal Am burden to be performed from in vivo monitoring of the knee region. In all analyzed cases, an excellent correlation (R = 99.9%) was found between the amount of Am activity in the knee and the amount of Am activity in the entire leg. The results of this study suggest three simple models: two models to predict the total skeletal activity based on either leg or knee activity, and the third model to predict the total leg activity based on knee activity. The results also suggest that the knee region is a suitable position for in vivo measurements of Am deposited in the bones and also for an accurate and efficient detection system. Detector efficiency should be apparently calibrated based on only the Am burden in the knee region bones instead of Am activity deposited in the entire leg.

  17. US Transuranium Registry report of the 241Am content of a whole body. Part IV: Preparation and analysis of the tissues and bones

    SciTech Connect

    McInroy, J.F.; Boyd, H.A.; Eutsler, B.C.; Romero, D.

    1985-10-01

    Los Alamos National Laboratory has analyzed autopsy tissue for the USTR, as a part of its study of the uptake, distribution and retention of Pu and other transuranic elements in occupationally exposed workers since 1978. In April 1979, Los Alamos received the internal organs and bone samples from the first whole-body donation to the USTR. The donor was known to have an internal deposition of SU Am. All soft tissue, the bones from the right half of the skeleton, and the odd-numbered vertebrae were received at Los Alamos in February 1980. The bones were subdivided along anatomical areas of interest. All soft tissues and bone specimens were analyzed for their SU Am content. A total deposition of 147.4 nCi SU Am was measured. Approximately 18% of the SU Am remaining in the body (disregarding that in the left hand), was found in the soft tissues, and 82% was in the bones and teeth. The soft tissues and organs containing the largest amounts of SU Am were the combined soft tissue (striated muscle, connective tissue and skin) 8.8%; liver, 6.4% and respiratory tract, 1.5%. The remaining organs accounted for 0.9% of the systemic burden.

  18. Collective doses to man from dumping of radioactive waste in the Arctic Seas.

    PubMed

    Nielsen, S P; Iosjpe, M; Strand, P

    1997-08-25

    A box model for the dispersion of radionuclides in the marine environment covering the Arctic Ocean and the North Atlantic Ocean has been constructed. Collective doses from ingestion pathways have been calculated from unit releases of the radionuclides 3H, 60Co, 63Ni, 90Sr, 129I, 137Cs, 239Pu and 241Am into a fjord on the east coast of NovayaZemlya. The results show that doses for the shorter-lived radionuclides (e.g. 137Cs) are derived mainly from seafood production in the Barents Sea. Doses from the longer-lived radionuclides (e.g. 239Pu) are delivered through marine produce further away from the Arctic Ocean. Collective doses were calculated for two release scenarios, both of which are based on information of the dumping of radioactive waste in the Barents and Kara Seas by the former Soviet Union and on preliminary information from the International Arctic Sea Assessment Programme. A worst-case scenario was assumed according to which all radionuclides in liquid and solid radioactive waste were available for dispersion in the marine environment at the time of dumping. Release of radionuclides from spent nuclear fuel was assumed to take place by direct corrosion of the fuel ignoring the barriers that prevent direct contact between the fuel and the seawater. The second scenario selected assumed that releases of radionuclides from spent nuclear fuel do not occur until after failure of the protective barriers. All other liquid and solid radioactive waste was assumed to be available for dispersion at the time of discharge in both scenarios. The estimated collective dose for the worst-case scenario was about 9 manSv and that for the second scenario was about 3 manSv. In both cases, 137Cs is the radionuclide predicted to dominate the collective doses as well as the peak collective dose rates.

  19. Plutonium in the WIPP environment: its detection, distribution and behavior.

    PubMed

    Thakur, P; Ballard, S; Nelson, R

    2012-05-01

    The Waste Isolation Pilot Plant (WIPP) is the only operating deep underground geologic nuclear repository in the United States. It is located in southeastern New Mexico, approximately 655 m (2150 ft) below the surface of the Earth in a bedded Permian evaporite salt formation. This mined geologic repository is designed for the safe disposal of transuranic (TRU) wastes generated from the US defense program. Aerosol and soil samples have been collected near the WIPP site to investigate the sources of plutonium in the WIPP environment since the late 1990s, well before WIPP received its first shipment. Activities of (238)Pu, (239+240)Pu and (241)Am were determined by alpha spectrometry following a series of chemical separations. The concentrations of Al and U were determined in a separate set of samples by inductively coupled plasma mass spectrometry. The annual airborne concentrations of (239+240)Pu during the period from 1998 to 2010 show no systematic interannual variations. However, monthly (239+240)Pu particulate concentrations show a typical seasonal variation with a maximum in spring, the time when strong and gusty winds frequently give rise to blowing dust. Resuspension of soil particles containing weapons fallout is considered to be the predominant source of plutonium in the WIPP area. Further, this work characterizes the source, temporal variation and its distribution with depth in a soil profile to evaluate the importance of transport mechanisms affecting the fate of these radionuclides in the WIPP environment. The mean (137)Cs/(239+240)Pu, (241)Am/(239+240)Pu activity ratio and (240)Pu/(239)Pu atom ratio observed in the WIPP samples are consistent with the source being largely global fallout. There is no evidence of any release from the WIPP contributing to radionuclide concentrations in the environment.

  20. Review and Assessment of Neutron Cross Section and Nubar Covariances for Advanced Reactor Systems

    SciTech Connect

    Maslov,V.M.; Oblozinsky, P.; Herman, M.

    2008-12-01

    In January 2007, the National Nuclear Data Center (NNDC) produced a set of preliminary neutron covariance data for the international project 'Nuclear Data Needs for Advanced Reactor Systems'. The project was sponsored by the OECD Nuclear Energy Agency (NEA), Paris, under the Subgroup 26 of the International Working Party on Evaluation Cooperation (WPEC). These preliminary covariances are described in two recent BNL reports. The NNDC used a simplified version of the method developed by BNL and LANL that combines the recent Atlas of Neutron Resonances, the nuclear reaction model code EMPIRE and the Bayesian code KALMAN with the experimental data used as guidance. There are numerous issues involved in these estimates of covariances and it was decided to perform an independent review and assessment of these results so that better covariances can be produced for the revised version in future. Reviewed and assessed are uncertainties for fission, capture, elastic scattering, inelastic scattering and (n,2n) cross sections as well as prompt nubars for 15 minor actinides ({sup 233,234,236}U, {sup 237}Np, {sup 238,240,241,242}Pu, {sup 241,242m,243}Am and {sup 242,243,244,245}Cm) and 4 major actinides ({sup 232}Th, {sup 235,238}U and {sup 239}Pu). We examined available evaluations, performed comparison with experimental data, taken into account uncertainties in model parameterization and made use state-of-the-art nuclear reaction theory to produce the uncertainty assessment.

  1. Separation of americium, curium, and plutonium from irradiated targets

    SciTech Connect

    Felker, L.K.; Benker, D.E.; Chattin, F.R.

    1995-04-01

    The Radiochemical Engineering Development Center (REDC) at Oak Ridge National Laboratory (ORNL) processes highly irradiated targets for the Mark 42 program to separate Am, Cm, and Pu. The target feed material for each assembly was 3.3 kg of plutonium (78% {sup 239}Pu) that was irradiated at the Savannah River Site to yield approximately 100 g each of {sup 243}Am and {sup 244}Cm, and 100-g quantities of {sup 242}Pu for special DOE projects. The REDC has plans to process ten of these target assemblies over the next few years. The first assembly has been dissolved, and approximately 1/4 of this material has been used to test the processing flowsheet. Various aqueous processes developed at the REDC over the past years were utilized to dissolve the target segments, separate the bulk of the impurities from the transuranics, separate the plutonium from the transplutonium actinides, and separate the rare earth fission products from the Am-Cm. The separation of the Am-Cm products to the desired purity levels presented new processing challenges for REDC operations. Through a combination of precipitation and cation-exchange operations, an Am product containing part-per-million levels of Cm was obtained. Standard REDC processing techniques were used to prepare the products as oxides for shipment. Future processing will focus on the reduction of waste solutions, improvement of yields, and application of new technologies for improved processing.

  2. Chemical resolution of Pu+ from U+ and Am+ using a band-pass reaction cell inductively coupled plasma mass spectrometer.

    PubMed

    Tanner, Scott D; Li, Chunsheng; Vais, Vladimir; Baranov, Vladimir I; Bandura, Dmitry R

    2004-06-01

    Determination of the concentration and distribution of the Pu and Am isotopes is hindered by the isobaric overlaps between the elements themselves and U, generally requiring time-consuming chemical separation of the elements. A method is described in which chemical resolution of the elemental ions is obtained through ion-molecule reactions in a reaction cell of an ICPMS instrument. The reactions of "natural" U(+), (242)Pu(+), and (243)Am(+) with ethylene, carbon dioxide, and nitric oxide are reported. Since the net sensitivities to the isotopes of an element are similar, chemical resolution is inferred when one isobaric element reacts rapidly with a given gas and the isobar (or in this instance surrogate isotope) is unreactive or slowly reactive. Chemical resolution of the m/z 238 isotopes of U and Pu can be obtained using ethylene as a reaction gas, but little improvement in the resolution of the m/z 239 isobars is obtained. However, high efficiency of reaction of U(+) and UH(+) with CO(2), and nonreaction of Pu(+), allows the sub-ppt determination of (239)Pu, (240)Pu, and (242)Pu (single ppt for (238)Pu) in the presence of 7 orders of magnitude excess U matrix without prior chemical separation. Similarly, oxidation of Pu(+) by NO, and nonreaction of Am(+), permit chemical resolution of the isobars of Pu and Am over 2-3 orders of magnitude relative concentration. The method provides the potential for analysis of the actinides with reduced sample matrix separation.

  3. Preparation of alpha sources using magnetohydrodynamic electrodeposition for radionuclide metrology.

    PubMed

    Panta, Yogendra M; Farmer, Dennis E; Johnson, Paula; Cheney, Marcos A; Qian, Shizhi

    2010-02-01

    Expanded use of nuclear fuel as an energy resource and terrorist threats to public safety clearly require the development of new state-of-the-art technologies and improvement of safety measures to minimize the exposure of people to radiation and the accidental release of radiation into the environment. The precision in radionuclide metrology is currently limited by the source quality rather than the detector performance. Electrodeposition is a commonly used technique to prepare massless radioactive sources. Unfortunately, the radioactive sources prepared by the conventional electrodeposition method produce poor resolution in alpha spectrometric measurements. Preparing radioactive sources with better resolution and higher yield in the alpha spectrometric range by integrating magnetohydrodynamic convection with the conventional electrodeposition technique was proposed and tested by preparing mixed alpha sources containing uranium isotopes ((238)U, (234)U), plutonium ((239)Pu), and americium ((241)Am) for alpha spectrometric determination. The effects of various parameters such as magnetic flux density, deposition current and time, and pH of the sample solution on the formed massless radioactive sources were also experimentally investigated.

  4. High-Resistivity Semi-insulating AlSb on GaAs Substrates Grown by Molecular Beam Epitaxy

    NASA Astrophysics Data System (ADS)

    Vaughan, E. I.; Addamane, S.; Shima, D. M.; Balakrishnan, G.; Hecht, A. A.

    2016-04-01

    Thin-film structures containing AlSb were grown using solid-source molecular beam epitaxy and characterized for material quality, carrier transport optimization, and room-temperature radiation detection response. Few surface defects were observed, including screw dislocations resulting from shear strain between lattice-mismatched layers. Strain was also indicated by broadening of the AlSb peak in x-ray diffraction measurements. Threading dislocations and interfacial misfit dislocations were seen with transmission electron microscopy imaging. Doping of the AlSb layer was introduced during growth using GaTe and Be to determine the effect on Hall transport properties. Hall mobility and resistivity were largest for undoped AlSb samples, at 3000 cm2/V s and 106 Ω cm, respectively, and increased doping levels progressively degraded these values. To test for radiation response, p-type/intrinsic/ n-type (PIN) diode structures were grown using undoped AlSb on n-GaAs substrates, with p-GaSb cap layers to protect the AlSb from oxidation. Alpha-particle radiation detection was achieved and spectra were produced for 241Am, 252Cf, and 239Pu sources. Reducing the detector surface area increased the pulse height observed, as expected based on voltage-capacitance relationships for diodes.

  5. 243,244Cm studies in C57BL/Do mice.

    PubMed

    Jones, C W; Mays, C W; Lloyd, R D; Packer, S M; Taylor, G N; Smith, J M; McFarland, S S

    1985-06-01

    Three groups of C57BL/Do mice were injected with different activities of 243,244Cm so that the long-term biological effects could be evaluated. The biological retention, R, of injected curium in the skeleton at t days after injection could be represented by the equations R = 0.245e-0.000379t and R = 0.208e-0.000494t for male and female mice, respectively. Effective skeletal retention equations were used to calculate the cumulative mean skeletal dose in rad at 140 days before death in each group of mice. The primary objective of this study was to determine the relative biological effectiveness (RBE) of 243,244Cm compared to 226Ra, using bone sarcoma induction as the end point. Combined data (bone sarcomas per 10(6) mouse-rad) for male and female mice permitted the RBE value +/- SD for 243,244Cm to be calculated as 4.4 +/- 1.8 compared to 1.0 for 226Ra. A comparison of RBE values form a previous study in this mouse strain and the value for 243,244Cm from this study suggests that the trivalent actinides 241Am, 243,244Cm, and 249Cf are about three times less effective for bone sarcoma induction than 239Pu.

  6. Northern Marshall Islands radiological survey: sampling and analysis summary

    SciTech Connect

    Robison, W.L.; Conrado, C.L.; Eagle, R.J.; Stuart, M.L.

    1981-07-23

    A radiological survey was conducted in the Northern Marshall Islands to document reamining external gamma exposures from nuclear tests conducted at Enewetak and Bikini Atolls. An additional program was later included to obtain terrestrial and marine samples for radiological dose assessment for current or potential atoll inhabitants. This report is the first of a series summarizing the results from the terrestrial and marine surveys. The sample collection and processing procedures and the general survey methodology are discussed; a summary of the collected samples and radionuclide analyses is presented. Over 5400 samples were collected from the 12 atolls and 2 islands and prepared for analysis including 3093 soil, 961 vegetation, 153 animal, 965 fish composite samples (average of 30 fish per sample), 101 clam, 50 lagoon water, 15 cistern water, 17 groundwater, and 85 lagoon sediment samples. A complete breakdown by sample type, atoll, and island is given here. The total number of analyses by radionuclide are 8840 for /sup 241/Am, 6569 for /sup 137/Cs, 4535 for /sup 239 +240/Pu, 4431 for /sup 90/Sr, 1146 for /sup 238/Pu, 269 for /sup 241/Pu, and 114 each for /sup 239/Pu and /sup 240/Pu. A complete breakdown by sample category, atoll or island, and radionuclide is also included.

  7. Resuspension and atmospheric transport of radionuclides due to wildfires near the Chernobyl Nuclear Power Plant in 2015: An impact assessment

    PubMed Central

    Evangeliou, N.; Zibtsev, S.; Myroniuk, V.; Zhurba, M.; Hamburger, T.; Stohl, A.; Balkanski, Y.; Paugam, R.; Mousseau, T. A.; Møller, A. P.; Kireev, S. I.

    2016-01-01

    In April and August 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) caused concerns about the secondary radioactive contamination that might have spread over Europe. The present paper assessed, for the first time, the impact of these fires over Europe. About 10.9 TBq of 137Cs, 1.5 TBq of 90Sr, 7.8 GBq of 238Pu, 6.3 GBq of 239Pu, 9.4 GBq of 240Pu and 29.7 GBq of 241Am were released from both fire events corresponding to a serious event. The more labile elements escaped easier from the CEZ, whereas the larger refractory particles were removed more efficiently from the atmosphere mainly affecting the CEZ and its vicinity. During the spring 2015 fires, about 93% of the labile and 97% of the refractory particles ended in Eastern European countries. Similarly, during the summer 2015 fires, about 75% of the labile and 59% of the refractory radionuclides were exported from the CEZ with the majority depositing in Belarus and Russia. Effective doses were above 1 mSv y−1 in the CEZ, but much lower in the rest of Europe contributing an additional dose to the Eastern European population, which is far below a dose from a medical X-ray. PMID:27184191

  8. Rapid determination of alpha emitters using Actinide resin.

    PubMed

    Navarro, N; Rodriguez, L; Alvarez, A; Sancho, C

    2004-01-01

    The European Commission has recently published the recommended radiological protection criteria for the clearance of building and building rubble from the dismantling of nuclear installations. Radionuclide specific clearance levels for actinides are very low (between 0.1 and 1 Bq g(-1)). The prevalence of natural radionuclides in rubble materials makes the verification of these levels by direct alpha counting impossible. The capability of Actinide resin (Eichrom Industries, Inc.) for extracting plutonium and americium from rubble samples has been tested in this work. Besides a strong affinity for actinides in the tri, tetra and hexavalent oxidation states, this extraction chromatographic resin presents an easy recovery of absorbed radionuclides. The retention capability was evaluated on rubble samples spiked with certified radionuclide standards (239Pu and 241Am). Samples were leached with nitric acid, passed through a chromatographic column containing the resin and the elution fraction was measured by LSC. Actinide retention varies from 60% to 80%. Based on these results, a rapid method for the verification of clearance levels for actinides in rubble samples is proposed.

  9. Processing Irradiated Beryllium For Disposal

    SciTech Connect

    T. J. Tranter; R. D. Tillotson; N. R. Mann; G. R. Longhurst

    2005-11-01

    The purpose of this research was to develop a process for decontaminating irradiated beryllium that will allow it to be disposed of through normal radwaste channels. Thus, the primary objectives of this ongoing study are to remove the transuranic (TRU) isotopes to less than 100 nCi/g and remove {sup 60}Co, and {sup 137}Cs, to levels that will allow the beryllium to be contact handled. One possible approach that appears to have the most promise is aqueous dissolution and separation of the isotopes by selected solvent extraction followed by precipitation, resulting in a granular form for the beryllium that may be fixed to prevent it from becoming respirable and therefore hazardous. Beryllium metal was dissolved in nitric and fluorboric acids. Isotopes of {sup 241}Am, {sup 239}Pu, {sup 85}Sr, and {sup 137}Cs were then added to make a surrogate beryllium waste solution. A series of batch contacts was performed with the spiked simulant using chlorinated cobalt dicarbollide (CCD) and polyethylene glycol diluted with sulfone to extract the isotopes of Cs and Sr. Another series of batch contacts was performed using a combination of octyl (phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) in tributyl phosphate (TBP) diluted with dodecane for extracting the isotopes of Pu and Am. The results indicate that greater than 99.9% removal can be achieved for each isotope with only three contact stages.

  10. Resuspension and atmospheric transport of radionuclides due to wildfires near the Chernobyl Nuclear Power Plant in 2015: An impact assessment.

    PubMed

    Evangeliou, N; Zibtsev, S; Myroniuk, V; Zhurba, M; Hamburger, T; Stohl, A; Balkanski, Y; Paugam, R; Mousseau, T A; Møller, A P; Kireev, S I

    2016-05-17

    In April and August 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) caused concerns about the secondary radioactive contamination that might have spread over Europe. The present paper assessed, for the first time, the impact of these fires over Europe. About 10.9 TBq of (137)Cs, 1.5 TBq of (90)Sr, 7.8 GBq of (238)Pu, 6.3 GBq of (239)Pu, 9.4 GBq of (240)Pu and 29.7 GBq of (241)Am were released from both fire events corresponding to a serious event. The more labile elements escaped easier from the CEZ, whereas the larger refractory particles were removed more efficiently from the atmosphere mainly affecting the CEZ and its vicinity. During the spring 2015 fires, about 93% of the labile and 97% of the refractory particles ended in Eastern European countries. Similarly, during the summer 2015 fires, about 75% of the labile and 59% of the refractory radionuclides were exported from the CEZ with the majority depositing in Belarus and Russia. Effective doses were above 1 mSv y(-1) in the CEZ, but much lower in the rest of Europe contributing an additional dose to the Eastern European population, which is far below a dose from a medical X-ray.

  11. Resuspension and atmospheric transport of radionuclides due to wildfires near the Chernobyl Nuclear Power Plant in 2015: An impact assessment

    NASA Astrophysics Data System (ADS)

    Evangeliou, N.; Zibtsev, S.; Myroniuk, V.; Zhurba, M.; Hamburger, T.; Stohl, A.; Balkanski, Y.; Paugam, R.; Mousseau, T. A.; Møller, A. P.; Kireev, S. I.

    2016-05-01

    In April and August 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) caused concerns about the secondary radioactive contamination that might have spread over Europe. The present paper assessed, for the first time, the impact of these fires over Europe. About 10.9 TBq of 137Cs, 1.5 TBq of 90Sr, 7.8 GBq of 238Pu, 6.3 GBq of 239Pu, 9.4 GBq of 240Pu and 29.7 GBq of 241Am were released from both fire events corresponding to a serious event. The more labile elements escaped easier from the CEZ, whereas the larger refractory particles were removed more efficiently from the atmosphere mainly affecting the CEZ and its vicinity. During the spring 2015 fires, about 93% of the labile and 97% of the refractory particles ended in Eastern European countries. Similarly, during the summer 2015 fires, about 75% of the labile and 59% of the refractory radionuclides were exported from the CEZ with the majority depositing in Belarus and Russia. Effective doses were above 1 mSv y‑1 in the CEZ, but much lower in the rest of Europe contributing an additional dose to the Eastern European population, which is far below a dose from a medical X-ray.

  12. Tissue-equivalent torso phantom for calibration of transuranic-nuclide counting facilities

    SciTech Connect

    Griffith, R.V.; Anderson, A.L.; Dean, P.N.; Fisher, J.C.; Sundbeck, C.W.

    1986-01-16

    Several tissue-equivalent human-torso phantoms have been constructed for the calibration of counting systems used for in-vivo measurement of transuranic radionuclides. The phantoms contain a simulated human rib cage (in some cases, real bone) and removable model organs, and they include tissue-equivalent chest plates that can be placed over the torso to simulate people with a wide range of statures. The organs included are the lungs, liver, and tracheobronchial lymph nodes. Polyurethane with varying concentrations of added calcium was used to simulate the linear photon-attenuation properties of various human tissues, including lean muscle, adipose-muscle mixtures, cartilage, and bone. Foamed polyurethane was used to simulate lung tissue. Organs have been loaded with highly pure /sup 238/Pu, /sup 239/Pu, /sup 241/Am, and other radionuclides of interest. The validity of the phantom as a calibration standard has been checked in separate intercomparison studies using human subjects whose lungs contained a plutonium simulant. The resulting phantom calibration factors generally compared to within +-20% of the average calibration factors obtained for the human subjects.

  13. Measurement of alpha particle energy using windowless electret ion chambers.

    PubMed

    Dua, S K; Kotrappa, P; Srivastava, R; Ebadian, M A; Stieff, L R

    2002-10-01

    Electret ion chambers are inexpensive, lightweight, robust, commercially available, passive, charge-integrating devices for accurate measurement of different ionizing radiations. In an earlier work a chamber of dimensions larger than the range of alpha particles having aluminized Mylar windows of different thickness was used for measurement of alpha radiation. Correlation between electret mid-point voltage, alpha particle energy, and response was developed and it was shown that this chamber could be used for estimating the effective energy of an unknown alpha source. In the present study, the electret ion chamber is used in the windowless mode so that the alpha particles dissipate their entire energy inside the volume, and the alpha particle energy is determined from the first principles. This requires that alpha disintegration rate be accurately known or measured by an alternate method. The measured energies were within 1 to 4% of the true values for different sources (230Th, 237Np, 239Pu, 241Am, and 224Cm). This method finds application in quantitative determination of alpha energy absorbed in thin membrane and, hence, the absorbed dose.

  14. Separation of Transmutation - and Fission-Produced Radioisotopes from Irradiated Beryllium

    SciTech Connect

    Troy J. Tranter; RIchard D. Tillotson; Nick R. Mann; Glen R. Longhurst

    2011-11-01

    The primary objective of this study was to test the effectiveness of a two-step solvent extraction-precipitation process for separating transmutation and fission products from irradiated beryllium. Beryllium metal was dissolved in nitric and fluoroboric acids. Isotopes of 241Am, 239Pu, 85Sr, 60Co, and 137Cs were then added to make a surrogate beryllium waste solution. A series of batch contacts was performed with the spiked simulant using chlorinated cobalt dicarbollide and polyethylene glycol diluted with sulfone to extract the isotopes of Cs and Sr. Another series of batch contacts was performed using a combination of octyl (phenyl)-N,Ndiisobutylcarbamoylmethylphosphine oxide in tributyl phosphate diluted with dodecane for extracting the isotopes of Pu and Am. The 60Co was separated by first forming a cobalt complex and then selectively precipitating the beryllium as a hydroxide. The results indicate that greater than 99.9% removal can be achieved for each radionuclide. Transuranic isotope contamination levels are reduced to less than 100 nCi/g, and sources of high beta-gamma radiation (60Co, 137Cs, and 90Sr) are reduced to levels that will allow the beryllium to be contact handled. The separation process may be applicable to a recycle or waste disposition scenario.

  15. Apparatus and method for quantitative assay of generic transuranic wastes from nuclear reactors

    DOEpatents

    Caldwell, John T.; Kunz, Walter E.; Atencio, James D.

    1984-01-01

    A combination of passive and active neutron measurements which yields quantitative information about the isotopic composition of transuranic wastes from nuclear power or weapons material manufacture reactors is described. From the measurement of prompt and delayed neutron emission and the incidence of two coincidentally emitted neutrons from induced fission of fissile material in the sample, one can quantify .sup.233 U, .sup.235 U and .sup.239 Pu isotopes in waste samples. Passive coincidence counting, including neutron multiplicity measurement and determination of the overall passive neutron flux additionally enables the separate quantitative evaluation of spontaneous fission isotopes such as .sup.240 Pu, .sup.244 Cm and .sup.252 Cf, and the spontaneous alpha particle emitter .sup.241 Am. These seven isotopes are the most important constituents of wastes from nuclear power reactors and once the mass of each isotope present is determined by the apparatus and method of the instant invention, the overall alpha particle activity can be determined to better than 1 nCi/g from known radioactivity data. Therefore, in addition to the quantitative analysis of the waste sample useful for later reclamation purposes, the alpha particle activity can be determined to decide whether "permanent" low-level burial is appropriate for the waste sample.

  16. Apparatus and method for quantitative assay of generic transuranic wastes from nuclear reactors

    DOEpatents

    Caldwell, J.T.; Kunz, W.E.; Atencio, J.D.

    1982-03-31

    A combination of passive and active neutron measurements which yields quantitative information about the isotopic composition of transuranic wastes from nuclear power or weapons material manufacture reactors is described. From the measurement of prompt and delayed neutron emission and the incidence of two coincidentally emitted neutrons from induced fission of fissile material in the sample, one can quantify /sup 233/U, /sup 235/U and /sup 239/Pu isotopes in waste samples. Passive coincidence counting, including neutron multiplicity measurement and determination of the overall passive neutron flux additionally enables the separate quantitative evaluation of spontaneous fission isotopes such as /sup 240/Pu, /sup 244/Cm and /sup 252/Cf, and the spontaneous alpha particle emitter /sup 241/Am. These seven isotopes are the most important constituents of wastes from nuclear power reactors and once the mass of each isotope present is determined by the apparatus and method of the instant invention, the overall alpha particle activity can be determined to better than 1 nCi/g from known radioactivity data. Therefore, in addition to the quantitative analysis of the waste sample useful for later reclamation purposes, the alpha particle activity can be determined to decide whether permanent low-level burial is appropriate for the waste sample.

  17. Dose coefficients and derived guidance and clinical decision levels for contaminated wounds

    SciTech Connect

    Bertelli, Luiz; Toohey, Richard E

    2009-01-01

    The NCRP Wound Model describing the retention of selected radionuclides at the site of a contaminated wound and their uptake into the transfer compartment has been combined with the ICRP element-specific systemic models for those radionuclides to derive dose coefficients for intakes via contaminated wounds. Those coefficients have been used to generate derived guidance levels (i.e., the activity in a wound that would result in an effective dose of 20 or 50 mSv, or in some cases, a committed organ equivalent dose of 500 mSv), and clinical decision levels (i.e., activity levels that would indicate the need for consideration of medical intervention to remove activity from the wound site or administration of decorporation therapy or both), typically set at 5 times the derived guidance levels. Data are provided for the radionuclides commonly encountered at nuclear power plants and nuclear weapons, fuel fabrication or recycling, waste disposal, medical and research facilities. These include: {sup 60}Co, {sup 90}Sr, {sup 99m}Tc, {sup 131}I, {sup 137}Cs, {sup 192}Ir, {sup 210}Po, {sup 226,228}Ra, {sup 228,232}Th, {sup 235,238}U, {sup 237}Np, {sup 238,239}Pu, {sup 241}Am, {sup 242,244}Cm, and {sup 252}Cf.

  18. Comparative behavior of three long-lived radionuclides in forest ecosystems

    SciTech Connect

    Auerbach, S.I.

    1986-01-01

    This paper deals with studies in three forest ecosystems in eastern Tennessee, an area of rich temperate deciduous forests, sometimes referred to as mixed mesophytic forests. Two of these forest ecosystems were contaminated as a result of waste disposal operations. The third was experimentally tagged with millicurie quantities of /sup 137/Cs. One of these ecosystems is a floodplain forest that is typical of this region. This forest has been growing on alluvial soils since 1944. Prior to that time the area was a temporary holding pond within White Oak Creek which received radioactive effluents from ORNL. Radiocesium was deposited in the pond sediments as were /sup 90/Sr, /sup 239/Pu, /sup 241/Am, and other radionuclides. The dam which created the pond failed in late 1944, and the area was allowed to revert to natural conditions. The result was the development of a floodplain forest consisting of three different forest communities. The soils are fertile alluvials representative of bottomlands. The overstory tree species are principally ash, sycamore, boxelder, willow, and sweetgum (Fraxinus americana L., Plantanus occidentalis L., Acer negundo L., Salix nigra Marsh, and Liquidambar styraciflua L., respectively).

  19. Neutron imaging of radioactive sources

    NASA Astrophysics Data System (ADS)

    Hameed, F.; Karimzadeh, S.; Zawisky, M.

    2008-08-01

    Isotopic neutron sources have been available for more than six decades. At the Atomic Institute in Vienna, operating a 250 kW TRIGA reactor, different neutron sources are in use for instrument calibration and fast neutron applications but we have only little information about their construction and densities. The knowledge of source design is essential for a complete MCNP5 modeling of the experiments. Neutron radiography (NR) and neutron tomography (NT) are the best choices for the non-destructive inspection of the source geometry and homogeneity. From the transmission analysis we gain information about the shielding components and the densities of the radio-isotopes in the cores. Three neutron sources, based on (alpha, n) reaction, have been investigated, two 239PuBe sources and one 241AmBe source. In the NR images the internal structure was clearly revealed using high-resolving scintillation and imaging plate detectors. In one source tablet a crack was detected which causes asymmetric neutron emission. The tomography inspection of strong absorbing materials is more challenging due to the low beam intensity of 1.3x105 n/cm2s at our NT instrument, and due to the beam hardening effect which requires an extension of reconstruction software. The tomographic inspection of a PuBe neutron source and appropriate measures for background and beam hardening correction are presented.

  20. Analytical microscopy and environment. Current developments using bioindicators of pollution by stable and radioactive elements.

    PubMed

    Chassard-Bouchaud, C

    1996-05-01

    Ecotoxicological investigations were performed on three sets of bioindicators. The first one concerns marine pollution of invertebrates (molluscs: the mussel Mytilus edulis and related species, crustaceans: the crab Liocarcinus puber and related species), contaminated by stable or radioactive elements originating from wastes discharged into sea water. The second one concerns freshwater pollution of vertebrates (fish: the brown trout Salmo trutta fario), contaminated by aluminium dissolved in rivers, as a consequence of an atmospheric pollution by acid rain. The third one concerns the atmospheric pollution of trees by plutonium (Casuarina equisetifolia). Mechanisms involved in the uptake, storage and elimination processes of these toxicants were studied, with a special emphasis on cellular and subcellular aspects of concentration sites. Two microanalytical methods were employed: Secondary Ion Mass Spectrometry (SIMS), using the ion microscope and the ion microprobe, and X-ray spectrometry using the electron microprobe (EMP). In marine organisms, the target organs and tissues of bioaccumulation of stable and radioactive elements (238U, 239Pu and 241Am), were shown to be mainly digestive gland, gill and exoskeleton. The target organelles were shown to be spherocrystals and lysosomes. Amoebocytes, enzymatically equipped with lysosomal phosphatase, were involved in the phagocytic clearance of metal pollutants. In trout, insolubilisation of Al phosphate within lysosomes and a high metal concentration within bones were observed. The tree Casuarina equisetifolia exhibits a particular ability to concentrate atmospheric plutonium within its leaves.

  1. Further studies on the influence of chemical form and dose on absorptions of Np, Pu, Am and Cm from the gastrointestinal tracts of adult and neonatal rodents.

    PubMed

    Sullivan, M F; Miller, B M; Ruemmler, P S; Ryan, J L

    1985-01-01

    Absorption of isotopes of the actinide elements Np, Pu, Am and Cm from various organic media and/or in combination with plant or animal ligands or tissue is compared with their absorption from an inorganic nitrate medium. Gastrointestinal (GI) transport of 238Pu, 239Pu, 241Am and 244Cm at high concentrations from citrate medium by adult rats and/or mice was higher than from nitric acid medium. Neptunium-237 absorption, however, was not increased by citrate; probably because its oxidation state was reduced from 237Np(V) to 237Np(IV) by the medium and by the GI content. Increasing the mass of the 237Np dose resulted in increased absorption. Neither incorporation of 238Pu in rat liver nor retention of 238Pu oxide in rat lungs enhanced absorption when those Pu-containing tissues were administered intragastrically to either adult or neonatal rats. Ranking of GI absorption of the various forms of Pu gavaged in these studies suggests that transport is in the order: Pu citrate greater than Pu phytate greater than biologically incorporated Pu greater than Pu nitrate.

  2. Thin extractive membrane for monitoring actinides in aqueous streams.

    PubMed

    Chavan, Vivek; Paul, Sumana; Pandey, Ashok K; Kalsi, P C; Goswami, A

    2013-09-15

    Alpha spectrometry and solid state nuclear track detectors (SSNTDs) are used for monitoring ultra-trace amount of alpha emitting actinides in different aqueous streams. However, these techniques have limitations i.e. alpha spectrometry requires a preconcentration step and SSNTDs are not chemically selective. Therefore, a thin polymer inclusion membrane (PIM) supported on silanized glass was developed for preconcentraion and determination of ultra-trace concentration of actinides by α-spectrometry and SSNTDs. PIMs were formed by spin coating on hydrophobic glass slide or solvent casting to form thin and self-supported membranes, respectively. Sorption experiments indicated that uptakes of actinides in the PIM were highly dependent on acidity of solution i.e. Am(III) sorbed up to 0.1 molL(-1) HNO₃, U(VI) up to 0.5 molL(-1) HNO₃ and Pu(IV) from HNO₃ concentration as high as 4 molL(-1). A scheme was developed for selective sorption of target actinide in the PIM by adjusting acidity and oxidation state of actinide. The actinides sorbed in PIMs were quantified by alpha spectrometry and SSNTDs. For SSNTDs, neutron induced fission-fragment tracks and α-particle tracks were registered in Garware polyester and CR-39 for quantifications of natural uranium and α-emitting actinides ((241)Am/(239)Pu/(233)U), respectively. Finally, the membranes were tested to quantify Pu in 4 molL(-1) HNO3 solutions and synthetic urine samples.

  3. Mercuric iodide room-temperature array detectors for gamma-ray imaging

    SciTech Connect

    Patt, B.

    1994-11-15

    Significant progress has been made recently in the development of mercuric iodide detector arrays for gamma-ray imaging, making real the possibility of constructing high-performance small, light-weight, portable gamma-ray imaging systems. New techniques have been applied in detector fabrication and then low noise electronics which have produced pixel arrays with high-energy resolution, high spatial resolution, high gamma stopping efficiency. Measurements of the energy resolution capability have been made on a 19-element protypical array. Pixel energy resolutions of 2.98% fwhm and 3.88% fwhm were obtained at 59 keV (241-Am) and 140-keV (99m-Tc), respectively. The pixel spectra for a 14-element section of the data is shown together with the composition of the overlapped individual pixel spectra. These techniques are now being applied to fabricate much larger arrays with thousands of pixels. Extension of these principles to imaging scenarios involving gamma-ray energies up to several hundred keV is also possible. This would enable imaging of the 208 keV and 375-414 keV 239-Pu and 240-Pu structures, as well as the 186 keV line of 235-U.

  4. Dating of sediments from four Swiss prealpine lakes with (210)Pb determined by gamma-spectrometry: progress and problems.

    PubMed

    Putyrskaya, V; Klemt, E; Röllin, S; Astner, M; Sahli, H

    2015-07-01

    In this paper the most important problems in dating lake sediments with unsupported (210)Pb are summarized and the progress in gamma-spectrometry of the unsupported (210)Pb is discussed. The main topics of these studies concern sediment samples preparation for gamma-spectrometry, measurement techniques and data analysis, as well as understanding of accumulation and sedimentation processes in lakes. The vertical distributions of artificial ((137)Cs, (241)Am, (239)Pu) and natural radionuclides ((40)K, (210,214)Pb, (214)Bi) as well as stable trace elements (Fe, Mn, Pb) in sediment cores from four Swiss lakes were used as examples for the interpretation, inter-comparison and validation of depth-age relations established by three (210)Pb-based models (CF-CSR, CRS and SIT). The identification of turbidite layers and the influence of the turbidity flows on the accuracy of sediment dating is demonstrated. Time-dependent mass sedimentation rates in lakes Brienz, Thun, Biel and Lucerne are discussed and compared with published data.

  5. Radionuclide contaminant analysis of small mammels, plants and sediments within Mortandad Canyon, 1994

    SciTech Connect

    Bennett, K.; Biggs, J.; Fresquez, P.

    1996-01-01

    Small mammals, plants and sediments were sampled at one upstream location (Site 1) and two downstream locations (Site 2 and Site 3) from the National Pollution Discharge Elimination System outfall {number_sign}051-051 in Mortandad Canyon, Los Alamos County, New Mexico. The purpose of the sampling was to identify radionuclides potentially present, to quantitatively estimate and compare the amount of radionuclide uptake at specific locations (Site 2 and Site 3) within Mortandad Canyon to an upstream site (Site 1), and to identify the primary mode (inhalation ingestion, or surface contact) of contamination to small mammals. Three composite samples of at least five animals per sample were collected at each site. Pelts and carcasses of each animal were separated and analyzed independently. In addition, three composite samples were also collected for plants and sediments at each site. Samples were analyzed for {sup 241}Am, {sup 90}Sr, {sup 238}Pu, {sup 239}Pu, and total U. With the exception of total U, all mean radionuclide concentrations in small mammal carcasses and sediments were significantly higher at Site 2 than Site 1 or Site 3. No differences were detected in the mean radionuclide concentration of plant samples between sites. However, some radionuclide concentrations found at all three sites were higher than regional background. No differences were found between mean carcass radionuclide concentrations and mean pelt radionuclide concentrations, indicating that the two primary modes of contamination may be equally occurring.

  6. EURADOS intercomparison on emergency radiobioassay.

    PubMed

    Li, Chunsheng; Battisti, Paolo; Berard, Philippe; Cazoulat, Alain; Cuellar, Antonio; Cruz-Suarez, Rodolfo; Dai, Xiongxin; Giardina, Isabella; Hammond, Derek; Hernandez, Carolina; Kiser, Stephen; Ko, Raymond; Kramer-Tremblay, Sheila; Lecompte, Yannick; Navarro, Eva; Navas, Cristina; Sadi, Baki; Sierra, Inmaculada; Verrezen, Freddy; Lopez, Maria A

    2015-12-01

    Nine laboratories participated in an intercomparison exercise organised by the European Radiation Dosimetry Group (EURADOS) for emergency radiobioassay involving four high-risk radionuclides ((239)Pu, (241)Am, (90)Sr and (226)Ra). Diverse methods of analysis were used by the participating laboratories for the in vitro determination of each of the four radionuclides in urine samples. Almost all the methods used are sensitive enough to meet the requirements for emergency radiobioassay derived for this project in reference to the Clinical Decision Guide introduced by the NCRP. Results from most of the methods meet the requirements of ISO 28218 on accuracy in terms of relative bias and relative precision. However, some technical gaps have been identified. For example, some laboratories do not have the ability to assay samples containing (226)Ra, and sample turnaround time would be expected to be much shorter than that reported by many laboratories, as timely results for internal contamination and early decisions on medical intervention are highly desired. Participating laboratories are expected to learn from each other on the methods used to improve the interoperability among these laboratories.

  7. NSDann2BS, a neutron spectrum unfolding code based on neural networks technology and two bonner spheres

    SciTech Connect

    Ortiz-Rodriguez, J. M.; Reyes Alfaro, A.; Reyes Haro, A.; Solis Sanches, L. O.; Miranda, R. Castaneda; Cervantes Viramontes, J. M.; Vega-Carrillo, H. R.

    2013-07-03

    In this work a neutron spectrum unfolding code, based on artificial intelligence technology is presented. The code called ''Neutron Spectrometry and Dosimetry with Artificial Neural Networks and two Bonner spheres'', (NSDann2BS), was designed in a graphical user interface under the LabVIEW programming environment. The main features of this code are to use an embedded artificial neural network architecture optimized with the ''Robust design of artificial neural networks methodology'' and to use two Bonner spheres as the only piece of information. In order to build the code here presented, once the net topology was optimized and properly trained, knowledge stored at synaptic weights was extracted and using a graphical framework build on the LabVIEW programming environment, the NSDann2BS code was designed. This code is friendly, intuitive and easy to use for the end user. The code is freely available upon request to authors. To demonstrate the use of the neural net embedded in the NSDann2BS code, the rate counts of {sup 252}Cf, {sup 241}AmBe and {sup 239}PuBe neutron sources measured with a Bonner spheres system.

  8. 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.

  9. Estimated (n,f) cross sections for 236,236m237,238-Np, 237,237m-Pu, and 240,241,242,242m,243,244,244m-Am isotopes

    SciTech Connect

    Younes, W; Becker, J; Britt, H

    2004-01-16

    Neutron-induced fission cross sections on targets of {sup 236,236m,237,238}Np, {sup 237,237m}Pu, and {sup 240,241,242,242m,243,244,244m}Am have been estimated for incident neutron energies of up to 6 MeV, using the ''surrogate'' technique and the ({sup 3}He,df) and ({sup 3}He,tf) reactions on stable targets to measure fission probabilities. In isotopes where low-lying isomeric states are known to exist, the (n,f) cross section on the corresponding isomeric targets has been estimated, using the surrogate technique. For targets of {sup 237}Np, {sup 241}Am, {sup 242m}Am, {sup 243}Am, measurements of the (n,f) cross section exist, and comparison with the surrogate-method results suggests that the (n,f) cross sections estimated by the surrogate technique are reliable to within 10% for incident neutron energies E{sub n}{approx}>2 MeV. Tabulated values of the estimated (n,f) cross sections are given in an appendix.

  10. Utilization of natural hematite as reactive barrier for immobilization of radionuclides from radioactive liquid waste.

    PubMed

    El Afifi, E M; Attallah, M F; Borai, E H

    2016-01-01

    Potential utilization of hematite as a natural material for immobilization of long-lived radionuclides from radioactive liquid waste was investigated. Hematite ore has been characterized by different analytical tools such as Fourier transformer infrared (FTIR), X-ray fluorescence (XRF), powder X-ray diffraction (XRD), thermogravimetry (TG) and differential thermal (DT) analysis, scanning electron microscopy (SEM) and BET-surface area. In this study, europium was used as REEs(III) and as a homolog of Am(III)-isotopes (such as (241)Am of 432.6 y, (242m)Am of 141 y and (243)Am of 7370 y). Micro particles of the hematite ore were used for treatment of radioactive waste containing (152+154)Eu(III). The results indicated that 96% (4.1 × 10(4) Bq) of (152+154)Eu(III) was efficiently retained onto hematite ore. Kinetic experiments indicated that the processes could be simulated by a pseudo-second-order model and suggested that the process may be chemisorption in nature. The applicability of Langmuir, Freundlich and Temkin models was investigated. It was found that Langmuir isotherm exhibited the best fit with the experimental results. It can be concluded that hematite is an economic and efficient reactive barrier for immobilization of long-lived radio isotopes of actinides and REEs(III).

  11. Neutron capture and neutron-induced fission experiments on americium isotopes with DANCE

    SciTech Connect

    Jandel, Marian

    2008-01-01

    Neutron capture cross section data on Am isotopes were measured using the Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos National Laboratory. The neutron capture cross section was determined for {sup 241}Am for neutron energies between thermal and 320 keV. Preliminary results were also obtained for {sup 243}Am for neutron energies between 35 eV and 200 keV. The results on concurrent neutron-induced fission and neutron-capture measurements on {sup 242m}Am will be presented, where the fission events were actively triggered during the experiments. In these experiments, the Parallel-Plate Avalanche Counter (PPAC) detector that surrounds the target located in the center of the DANCE array was used as a fission-tagging detector to separate (n,{gamma}) from (n,f) events. The first evidence of neutron capture on {sup 242m}Am in the resonance region in between 2 and 9 eV of the neutron energy was obtained.

  12. Neutron capture and neutron-induced fission experiments on americium isotopes with DANCE

    SciTech Connect

    Jandel, M.; Bredeweg, T. A.; Fowler, M. M.; Bond, E. M.; Couture, A.; Haight, R. C.; Keksis, A. L.; O'Donnell, J. M.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wouters, J. M.; Stoyer, M. A.; Wu, C. Y.; Becker, J. A.; Haslett, R. J.; Henderson, R. A.

    2009-01-28

    Neutron capture cross section data on Am isotopes were measured using the Detector for Advanced Neutron Capture Experiments (DANCE) at Los Alamos National Laboratory. The neutron capture cross section was determined for {sup 241}Am for neutron energies between thermal and 320 keV. Preliminary results were also obtained for {sup 243}Am for neutron energies between 10 eV and 250 keV. The results on concurrent neutron-induced fission and neutron-capture measurements on {sup 242m}Am will be presented where the fission events were actively triggered during the experiments. In these experiments, a Parallel-Plate Avalanche Counter (PPAC) detector that surrounds the target located in the center of the DANCE array was used as a fission-tagging detector to separate (n,{gamma}) events from (n,f) events. The first direct observation of neutron capture on {sup 242m}Am in the resonance region in between 2 and 9 eV of the neutron energy was obtained.

  13. 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.

  14. Elemental bio-imaging of thorium, uranium, and plutonium in tissues from occupationally exposed former nuclear workers.

    PubMed

    Hare, Dominic; Tolmachev, Sergei; James, Anthony; Bishop, David; Austin, Christine; Fryer, Fred; Doble, Philip

    2010-04-15

    Internal exposure from naturally occurring radionuclides (including the inhaled long-lived actinides (232)Th and (238)U) is a component of the ubiquitous background radiation dose (National Council on Radiation Protection and Measurements. Ionizing radiation exposure of the population of the United States; NCRP Report No. 160; NCRP: Bethesda, MD, 2009). It is of interest to compare the concentration distribution of these natural alpha-emitters in the lungs and respiratory lymph nodes with those resulting from occupational exposure, including exposure to anthropogenic plutonium and depleted and enriched uranium. This study examines the application of laser ablation-inductively coupled plasma-mass spectrometry (LA-ICPMS) to quantifying and visualizing the mass distribution of uranium and thorium isotopes from both occupational and natural background exposure in human respiratory tissues and, for the first time, extends this application to the direct imaging of plutonium isotopes. Sections of lymphatic and lung tissues taken from deceased former nuclear workers with a known history of occupational exposure to specific actinide elements (uranium, plutonium, or americium) were analyzed by LA-ICPMS. Using a previously developed LA-ICPMS protocol for elemental bio-imaging of trace elements in human tissue and a new software tool, we generated images of thorium ((232)Th), uranium ((235)U and (238)U), and plutonium ((239)Pu and (240)Pu) mass distributions in sections of tissue. We used a laboratory-produced matrix-matched standard to quantify the (232)Th, (235)U, and (238)U concentrations. The plutonium isotopes (239)Pu and (240)Pu were detected by LA-ICPMS in 65 mum diameter localized regions of both a paratracheal lymph node and a sample of lung tissue from a person who was occupationally exposed to refractory plutonium (plutonium dioxide). The average (overall) (239)Pu concentration in the lymph node was 39.2 ng/g, measured by high purity germanium (HPGe) gamma

  15. Recent Results from Lohengrin on Fission Yields and Related Decay Properties

    NASA Astrophysics Data System (ADS)

    Serot, O.; Amouroux, C.; Bidaud, A.; Capellan, N.; Chabod, S.; Ebran, A.; Faust, H.; Kessedjian, G.; Köester, U.; Letourneau, A.; Litaize, O.; Martin, F.; Materna, T.; Mathieu, L.; Panebianco, S.; Regis, J.-M.; Rudigier, M.; Sage, C.; Urban, W.

    2014-05-01

    The Lohengrin mass spectrometer is one of the 40 instruments built around the reactor of the Institute Laue-Langevin (France) which delivers a very intense thermal neutron flux. Usually, Lohengrin was combined with a high-resolution ionization chamber in order to obtain good nuclear charge discrimination within a mass line, yielding an accurate isotopic yield determination. Unfortunately, this experimental procedure can only be applied for fission products with a nuclear charge less than about 42, i.e. in the light fission fragment region. Since 2008, a large collaboration has started with the aim of studying various fission aspects, mainly in the heavy fragment region. For that, a new experimental setup which allows isotopic identification by γ-ray spectrometry has been developed and validated. This technique was applied on the 239Pu(nth,f) reaction where about 65 fission product yields were measured with an uncertainty that has been reduced on average by a factor of 2 compared with what was that previously available in nuclear data libraries. The same γ-ray spectrometric technique is currently being applied to the study of the 233U(nth,f) reaction. Our aim is to deduce charge and mass distributions of the fission products and to complete the experimental data that exist mainly for light fission fragments. The measurement of 41 mass yields from the 241Am(2nth,f) reaction has been also performed. In addition to these activities on fission yield measurements, various new nanosecond isomers were discovered. Their presence can be revealed from a strong deformed ionic charge distribution compared to a 'normal' Gaussian shape. Finally, a new neutron long-counter detector designed to have a detection efficiency independent of the detected neutron energy has been built. Combining this neutron device with a Germanium detector and a beta-ray detector array allowed us to measure the beta-delayed neutron emission probability Pn of some important fission products for reactor

  16. Status of the WAND (Waste Assay for Nonradioactive Disposal) project as of July 1997

    SciTech Connect

    Arnone, G.J.; Foster, L.A.; Foxx, C.L.; Hagan, R.C.; Martin, E.R.; Myers, S.C.; Parker, J.L.

    1998-03-01

    The WAND (Waste Assay for Nonradioactive Disposal) system can scan thought-to-be-clean, low-density waste (mostly paper and plastics) to determine whether the levels of any contaminant radioactivity are low enough to justify their disposal in normal public landfills or similar facilities. Such a screening would allow probably at least half of the large volume of low-density waste now buried at high cost in LANL`s Rad Waste Landfill (Area G at Technical Area 54) to be disposed of elsewhere at a much lower cost. The WAND System consists of a well-shielded bank of six 5-in.-diam. phoswich scintillation detectors; a mechanical conveyor system that carries a 12-in.-wide layer of either shredded material or packets of paper sheets beneath the bank of detectors; the electronics needed to process the outputs of the detectors; and a small computer to control the whole system and to perform the data analysis. WAND system minimum detectable activities (MDAs) for point sources range from {approximately}20 dps for {sup 241}Am to approximately 10 times that value for {sup 239}Pu, with most other nuclides of interest being between those values, depending upon the emission probabilities of the radiations emitted (usually gamma rays and/or x-rays). The system can also detect beta particles that have energies {ge}100 keV, but it is not easy to define an MDA based on beta radiation detection because of the greater absorption of beta particles relative to photons in low Z-materials. The only radioactive nuclides not detectable by the WAND system are pure alpha emitters and very-low-energy beta emitters. At this time, operating procedures and quality assurance procedures are in place and training materials are available to operators. The system is ready to perform useful work; however, it would be both possible and desirable to upgrade the electronic components and the analysis algorithms.

  17. Functional Sorbents for Selective Capture of Plutonium, Americium, Uranium, and Thorium in Blood

    SciTech Connect

    Yantasee, Wassana; Sangvanich, Thanapon; Creim, Jeffrey A.; Pattamakomsan, Kanda; Wiacek, Robert J.; Fryxell, Glen E.; Addleman, Raymond S.; Timchalk, Charles

    2010-09-01

    Nano-engineered solid sorbents for chelation of actinides (239Pu, 241Am, uranium, thorium) from human blood were developed and evaluated in vitro. These sorbents, known as the self-assembled monolayer on mesoporous supports (SAMMSTM), are hybrid materials created from attachment of organic moieties onto extremely high surface area mesoporous silica. The organic moieties known to be effective at capturing actinides including three isomers of hydroxypyridinone, diphosphonic acid, acetamide phosphonic acid, glycinyl urea, and diethylenetriamine pentaacetate analog were evaluated. SAMMS are being reported elsewhere as potential candidates for orally administered drug for radionuclide decorporation. Herein, actinide decorporation of SAMMS in blood were evaluated to assess their viability for sorbent hemoperfusion in renal insufficient patients, whose kidney clear radionuclides at very slow rate. Sorption affinity (Kd), sorption rate, selectivity, and stability of SAMMS were measured in batch contact experiments. An isomer of hydroxypyridinone (3,4-HOPO) on SAMMS demonstrated the highest affinity for decorporation of all four actinides and outperformed the DTPA analog on SAMMS and on commercial resins by a factor of 103-fold in term of affinity. A fifty percent reduction of actinides in blood was achieved within minutes with no evidence of protein fouling and material leaching in blood after 24 hr of contact time. Less than 0.4 wt.% of Si was dissolved from 3,4-HOPO-SAMMS across the pH of 0 to 8. The engineered form of SAMMS (bead format) was further evaluated in a 100-fold scaled-down hemoperfusion device and showed no blood clotting after 2 hr. A 0.2 g of SAMMS could reduce 50 wt.% of 100 ppb uranium in 50 mL of plasma in just 18 min and that of 500 dpm mL-1 in just 24 min. 3,4-HOPO-SAMMS has a long shelf-life in air and at room temperature for at least 8 years, indicating their feasibility for stockpiling in preparedness for emergency.

  18. Sensitivity analysis of Monju using ERANOS with JENDL-4.0

    SciTech Connect

    Tamagno, P.; Van Rooijen, W. F. G.; Takeda, T.; Konomura, M.

    2012-07-01

    This paper deals with sensitivity analysis using JENDL-4.0 nuclear data applied to the Monju reactor. In 2010 the Japan Atomic Energy Agency - JAEA - released a new set of nuclear data: JENDL-4.0. This new evaluation is expected to contain improved data on actinides and covariance matrices. Covariance matrices are a key point in quantification of uncertainties due to basic nuclear data. For sensitivity analysis, the well-established ERANOS [1] code was chosen because of its integrated modules that allow users to perform a sensitivity analysis of complex reactor geometries. A JENDL-4.0 cross-section library is not available for ERANOS. Therefore a cross-section library had to be made from the original nuclear data set, available as ENDF formatted files. This is achieved by using the following codes: NJOY, CALENDF, MERGE and GECCO in order to create a library for the ECCO cell code (part of ERANOS). In order to make sure of the accuracy of the new ECCO library, two benchmark experiments have been analyzed: the MZA and MZB cores of the MOZART program measured at the ZEBRA facility in the UK. These were chosen due to their similarity to the Monju core. Using the JENDL-4.0 ECCO library we have analyzed the criticality of Monju during the restart in 2010. We have obtained good agreement with the measured criticality. Perturbation calculations have been performed between JENDL-3.3 and JENDL-4.0 based models. The isotopes {sup 239}Pu, {sup 238}U, {sup 241}Am and {sup 241}Pu account for a major part of observed differences. (authors)

  19. Evaluation of the anthropogenic radionuclide concentrations in sediments and fauna collected in the Beaufort Sea and northern Alaska

    SciTech Connect

    Efurd, D.W.; Miller, G.G.; Rokop, D.J.

    1997-07-01

    This study was performed to establish a quality controlled data set about the levels of radio nuclide activity in the environment and in selected biota in the U.S. Arctic. Sediment and biota samples were collected by the National Oceanic and Atmospheric Administration (NOAA), the National Biological Service, and the North Slope Borough`s Department of Wildlife Management to determine the impact of anthropogenic radionuclides in the Arctic. The results summarized in this report are derived from samples collected in northwest Alaska with emphasis on species harvested for subsistence in Barrow, Alaska. Samples were analyzed for the anthropogenic radionuclides {sup 90}Sr, {sup 137}Cs, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu and {sup 241}Am. The naturally occurring radionuclides {sup 40}K, {sup 212}Pb and {sup 214}Pb were also measured. One goal of this study was to determine the amounts of anthropogenic radionuclides present in the Beaufort Sea. Sediment samples were isotopically fingerprinted to determine the sources of radio nuclide activities. Biota samples of subsistence and ecological value were analyzed to search for evidence of bio-accumulation of radionuclides and to determine the radiation exposures associated with subsistence living in northern Alaska. The anthropogenic radio nuclide content of sediments collected in the Beaufort Sea was predominantly the result of the deposition of global fallout. No other sources of anthropogenic radionuclides could be conclusively identified in the sediments. The anthropogenic radio nuclide concentrations in fish, birds and mammals were very low. Assuming that ingestion of food is an important pathway leading to human contact with radioactive contaminants and given the dietary patterns in coastal Arctic communities, it can be surmised that marine food chains are presently not significantly affected.

  20. Development of site-specific soil cleanup criteria: New Brunswick Laboratory, New Jersey site

    SciTech Connect

    Veluri, V.R.; Moe, H.J.; Robinet, M.J.; Wynveen, R.A.

    1983-03-01

    The potential human exposure which results from the residual soil radioactivity at a decommissioned site is a prime concern during D and D projects. To estimate this exposure, a pathway analysis approach is often used to arrive at the residual soil radioactivity criteria. The development of such a criteria for the decommissioning of the New Brunswick Laboratory, New Jersey site is discussed. Contamination on this site was spotty and located in small soil pockets spread throughout the site area. Less than 1% of the relevant site area was contaminated. The major contaminants encountered at the site were /sup 239/Pu, /sup 241/Am, normal and natural uranium, and natural thorium. During the development of the pathway analysis to determine the site cleanup criteria, corrections for the inhomogeneity of the contamination were made. These correction factors and their effect upon the relevant pathway parameters are presented. Major pathways by which radioactive material may reach an individual are identified and patterns of use are specified (scenario). Each pathway is modeled to estimate the transfer parameters along the given pathway, such as soil to air to man, etc. The transfer parameters are then combined with dose rate conversion factors (ICRP 30 methodology) to obtain soil concentration to dose rate conversion factors (pCi/g/mrem/yr). For an appropriate choice of annual dose equivalent rate, one can then arrive at a value for the residual soil concentration. Pathway modeling, transfer parameters, and dose rate factors for the three major pathways; inhalation, ingestion and external exposure, which are important for the NBL site, are discussed.

  1. Characterization and Source Term Assessments of Radioactive Particles from Marshall Islands Using Non-Destructive Analytical Techniques

    SciTech Connect

    Jernstrom, J; Eriksson, M; Simon, R; Tamborini, G; Bildstein, O; Carlos-Marquez, R; Kehl, S R; Betti, M; Hamilton, T

    2005-06-11

    A considerable fraction of radioactivity entering the environment from different nuclear events is associated with particles. The impact of these events can only be fully assessed where there is some knowledge about the mobility of particle bound radionuclides entering the environment. The behavior of particulate radionuclides is dependent on several factors, including the physical, chemical and redox state of the environment, the characteristics of the particles (e.g., the chemical composition, crystallinity and particle size) and on the oxidative state of radionuclides contained in the particles. Six plutonium-containing particles stemming from Runit Island soil (Marshall Islands) were characterized using non-destructive analytical and microanalytical methods. By determining the activity of {sup 239,240}Pu and {sup 241}Am isotopes from their gamma peaks structural information related to Pu matrix was obtained, and the source term was revealed. Composition and elemental distribution in the particles were studied with synchrotron radiation based micro X-ray fluorescence (SR-{mu}-XRF) spectrometry. Scanning electron microscope equipped with energy dispersive X-ray detector (SEMEDX) and secondary ion mass spectrometer (SIMS) were used to examine particle surfaces. Based on the elemental composition the particles were divided into two groups; particles with plain Pu matrix, and particles where the plutonium is included in Si/O-rich matrix being more heterogeneously distributed. All of the particles were identified as fragments of initial weapons material. As containing plutonium with low {sup 240}Pu/{sup 239}Pu atomic ratio, {approx}2-6%, which corresponds to weapons grade plutonium, the source term was identified to be among the safety tests conducted in the history of Runit Island.

  2. Monte Carlo simulation of skull and knee voxel phantoms for the assessment of skeletal burden of low-energy photon emitters.

    PubMed

    Nadar, M Y; Akar, D K; Patni, H K; Singh, I S; Mishra, L; Rao, D D; Pradeepkumar, K S

    2014-12-01

    In case of internal contamination due to long-lived actinides by inhalation or injection pathway, a major portion of activity will be deposited in the skeleton and liver over a period of time. In this study, calibration factors (CFs) of Phoswich and an array of HPGe detectors are estimated using skull and knee voxel phantoms. These phantoms are generated from International Commission of Radiation Protection reference male voxel phantom. The phantoms as well as 20 cm diameter phoswich, having 1.2 cm thick NaI (Tl) primary and 5cm thick CsI (Tl) secondary detector and an array of three HPGe detectors (each of diameter of 7 cm and thickness of 2.5 cm) are incorporated in Monte Carlo code 'FLUKA'. Biokinetic models of Pu, Am, U and Th are solved using default parameters to identify different parts of the skeleton where activity will accumulate after an inhalation intake of 1 Bq. Accordingly, CFs are evaluated for the uniform source distribution in trabecular bone and bone marrow (TBBM), cortical bone (CB) as well as in both TBBM and CB regions for photon energies of 18, 60, 63, 74, 93, 185 and 238 keV describing sources of (239)Pu, (241)Am, (238)U, (235)U and (232)Th. The CFs are also evaluated for non-uniform distribution of activity in TBBM and CB regions. The variation in the CFs for source distributed in different regions of the bones is studied. The assessment of skeletal activity of actinides from skull and knee activity measurements is discussed along with the errors.

  3. Fabrication and characterization of MCC approved testing material - ATM-12 glass

    SciTech Connect

    Wald, J.W.

    1985-10-01

    The Materials Characterization Center (MCC) Approved Testing Material ATM-12 is a borosilicate glass that incorporates elements typical of high-level waste (HLW) resulting from the reprocessing of commercial nuclear reactor fuels. The composition has been adjusted to match that predicted for HLW type 76-68 glass at an age of 300 y. Radioactive constituents contained in this glass include depleted uranium, {sup 99}Tc, {sup 237}Np, {sup 239}Pu, and {sup 241}Am. The glass was produced by the MCC at the Pacific Northwest Laboratory (PNL). ATM-12 glass ws produced from July to November of 1984 at the request of the Nevada Nuclear Waste Site Investigations (NNWSI) Program and is the third in a series of glasses produced for NNWSI. Most of the glass produced was in the form of cast bars; special castings and crushed material were also produced. Three kilograms of ATM-12 glass were produced from a feedstock melted in a nitrogen-atmosphere glove box at 1150{sup 0}C in a platinum crucible, and formed into stress-annealed rectangular bars and the special casting shapes requested by NNWSI. Bars of ATM-12 were nominally 1.9 x 1.9 x 10 cm, with an average mass of 111 g each. Nineteen bars and 37 special castings were made. ATM-12 glass has been provided to the NNWSI Program, in the form of bars, crushed powder and special castings. As of August 1985 approximately 590 g of ATM-12 is available for distribution. Requests for materials or services related to this glass should be directed to the Materials Characterization Center Program Office, PNL.

  4. Americium in the beagle dog: biokinetic and dosimetric model.

    PubMed

    Luciani, A; Polig, E; Lloyd, R D; Miller, S C

    2006-05-01

    A biokinetic model of the systemic distribution of americium in the beagle dog is presented. The model is based on a previous biokinetic model of plutonium. The data sets used for the development of the model were the measurements of excreted activity (urine and feces) and organ burdens (skeleton, liver, and other soft tissues) for different levels of initial injected activity. In developing the model, the compartmental structure of the skeleton of the plutonium model was adopted, and only the numerical values of parameters were adapted. The model well describes the fractions of americium in the skeleton, liver, and soft tissues and the total fraction excreted in urine and feces. The tuning of the liver clearance parameter provides a realistic description of the change in the partitioning between liver and skeleton for different injection levels. The most significant features of the biokinetics and dosimetry of americium and plutonium in beagles are compared. The total fractions of the clearance to the skeleton and the liver are roughly equal to the value for plutonium, but the partitioning of americium between these organs is reversed with respect to the partitioning of plutonium. 241Am doses to liver and skeleton are similar to 239Pu doses, owing to some counteracting factors. For the highest injection level, the liver mass is dependent on the time post injection. For the skeletal tissues, the dose to the cortical endosteum by far exceeds the dose to the trabecular endosteum and the red marrow. The model provides the basis for statistical survival analyses and risk estimates.

  5. Study of calculated and measured time dependent delayed neutron yields. [TX, for calculating delayed neutron yields; MATINV, for matrix inversion; in FORTRAN for LSI-II minicomputer

    SciTech Connect

    Waldo, R.W.

    1980-05-01

    Time-dependent delayed neutron emission is of interest in reactor design, reactor dynamics, and nuclear physics studies. The delayed neutrons from neutron-induced fission of /sup 232/U, /sup 237/Np, /sup 238/Pu, /sup 241/Am, /sup 242m/Am, /sup 245/Cm, and /sup 249/Cf were studied for the first time. The delayed neutron emission from /sup 232/Th, /sup 233/U, /sup 235/U, /sup 238/U, /sup 239/Pu, /sup 241/Pu, and /sup 242/Pu were measured as well. The data were used to develop an empirical expression for the total delayed neutron yield. The expression gives accurate results for a large variety of nuclides from /sup 232/Th to /sup 252/Cf. The data measuring the decay of delayed neutrons with time were used to derive another empirical expression predicting the delayed neutron emission with time. It was found that nuclides with similar mass-to-charge ratios have similar decay patterns. Thus the relative decay pattern of one nuclide can be established by any measured nuclide with a similar mass-to-charge ratio. A simple fission product yield model was developed and applied to delayed neutron precursors. It accurately predicts observed yield and decay characteristics. In conclusion, it is possible to not only estimate the total delayed neutron yield for a given nuclide but the time-dependent nature of the delayed neutrons as well. Reactors utilizing recycled fuel or burning actinides are likely to have inventories of fissioning nuclides that have not been studied until now. The delayed neutrons from these nuclides can now be incorporated so that their influence on the stability and control of reactors can be delineated. 8 figures, 39 tables.

  6. Low energy AMS of americium and curium

    NASA Astrophysics Data System (ADS)

    Christl, Marcus; Dai, Xiongxin; Lachner, Johannes; Kramer-Tremblay, Sheila; Synal, Hans-Arno

    2014-07-01

    Accelerator mass spectrometry (AMS) has evolved over the past years as one of the most sensitive, selective, and robust techniques for actinide analyses. While analyses of U and Pu isotopes have already become routine at the ETH Zurich 0.5 MV AMS system "Tandy", there is an increasing demand for highly sensitive analyses of the higher actinides such as Am and Cm for bioassay applications and beyond. In order to extend the actinide capabilities of the compact ETH Zurich AMS system and to develop new, more sensitive bioassay routines, a pilot study was carried out. The aim was to investigate and document the performance and the potential background of Am and Cm analyses with low energy AMS. Our results show that 241Am and Cm isotopes can be determined relative to a 243Am tracer if samples and AMS standards are prepared identically with regard to the matrix elements, in which the sample is dispersed. In this first test, detection limits for Cm and Am isotopes are all in the sub-femtogram range and even below 100 ag for Cm isotopes. In a systematic background study in the mass range of the Cm isotopes, two formerly unknown metastable triply charged Th molecules were found on amu(244) and amu(248). The presence of such a background is not a principal problem for AMS if the stripper pressure is increased accordingly. Based on our first results, we conclude that ultra-trace analyses of Am and Cm isotopes for bioassay are very well possible with low energy AMS.

  7. Neutron scattering studies in the actinide region. Progress report, August 1, 1992--July 31, 1993

    SciTech Connect

    Kegel, G.H.R.; Egan, J.J.

    1993-09-01

    This report discusses the following topics: Prompt fission neutron energy spectra for {sup 235}U and {sup 239}Pu; Two-parameter measurement of nuclear lifetimes; ``Black`` neutron detector; Data reduction techniques for neutron scattering experiments; Inelastic neutron scattering studies in {sup 197}Au; Elastic and inelastic scattering studies in {sup 239}Pu; and neutron induced defects in silicon dioxide MOS structures.

  8. The role of plutonium as a resource now and in the future

    SciTech Connect

    Ray, D.L.

    1988-01-01

    This paper is the author's predictions of the role of plutonium as a resource. /sup 238/Pu is considered as a fuel for radiothermal generators in satellites and space probes. /sup 239/Pu is acknowledged to be vital in weapons applications. /sup 239/Pu and /sup 240/Pu are discussed from the viewpoint of commercial electrical generation.

  9. Determining Pu-239 content by resonance transmission analysis using a filtered reactor beam.

    SciTech Connect

    Klann, R. T.

    1998-11-25

    A novel technique has been developed at Argonne National Laboratory to determine the {sup 239}Pu content in EBR-II blanket elements using resonance transmission analysis (RTA) with a filtered reactor beam. The technique uses cadmium and gadolinium filters along with a {sup 239}Pu fission chamber to isolate the 0.3 eV resonance in {sup 239}Pu. In the energy range from 0.1 to 0.5 eV, the total microscopic cross-section of {sup 239}Pu is significantly larger than the cross-sections of {sup 238}U and {sup 235}U. This large difference in cross-section allows small amounts of {sup 239}Pu to be detected in uranium samples. Tests using a direct beam from a 250 kW TRIGA reactor have been performed with stacks of depleted uranium and {sup 239}Pu foils. Preliminary measurement results are in good agreement with the predicted results up to about two weight percent of {sup 239}Pu in the sample. In addition, measured {sup 239}Pu masses were in agreement with actual sample masses with uncertainties less than 3.8 percent.

  10. Accelerator mass spectrometry (AMS) in plutonium analysis.

    PubMed

    Strumińska-Parulska, Dagmara I

    The paper summarizes the results of the (240)Pu/(239)Pu atomic ratio studies in atmospheric fallout samples collected in 1986 over Gdynia (Poland) as well as three Baltic fish species collected in 1997 using the accelerator mass spectrometry. A new generation of AMS has been developed during last years and this method is an efficient and good technique to measure long-lived radioisotopes in the environment and provides the most accurate determination of the atomic ratios between (240)Pu and (239)Pu. The nuclide compositions of plutonium in filter samples correspond to their means of production. AMS measurements of atmospheric fallout collected in April showed sufficient increase of the (240)Pu/(239)Pu atomic ratio from 0.28 from March to 0.47. Also such high increase of (240)Pu/(239)Pu atomic ratio, close to reactor core (240)Pu/(239)Pu atomic ratio, was observed in September and equaled 0.47.

  11. National low-level waste management program radionuclide report series, Volume 14: Americium-241

    SciTech Connect

    Winberg, M.R.; Garcia, R.S.

    1995-09-01

    This report, Volume 14 of the National Low-Level Waste Management Program Radionuclide Report Series, discusses the radiological and chemical characteristics of americium-241 ({sup 241}Am). This report also includes discussions about waste types and forms in which {sup 241}Am can be found and {sup 241}Am behavior in the environment and in the human body.

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

    SciTech Connect

    Kahler, A.; 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, Micheal W; Arcilla, r; Mughabghab, S F; Sublet, J C; Trkov, A.; Trumbull, T H; Dunn, Michael E

    2011-01-01

    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 [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 unrnoderated and uranium reflected (235)U and (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 selected actinide reaction rates such as (236)U; (238,242)Pu and (241,243)Am capture in fast systems. Other deficiencies, such as the overprediction of Pu solution system critical eigenvalues

  14. 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

  15. Phytoremediation: role of terrestrial plants and aquatic macrophytes in the remediation of radionuclides and heavy metal contaminated soil and water.

    PubMed

    Sharma, Sunita; Singh, Bikram; Manchanda, V K

    2015-01-01

    Nuclear power reactors are operating in 31 countries around the world. Along with reactor operations, activities like mining, fuel fabrication, fuel reprocessing and military operations are the major contributors to the nuclear waste. The presence of a large number of fission products along with multiple oxidation state long-lived radionuclides such as neptunium ((237)Np), plutonium ((239)Pu), americium ((241/243)Am) and curium ((245)Cm) make the waste streams a potential radiological threat to the environment. Commonly high concentrations of cesium ((137)Cs) and strontium ((90)Sr) are found in a nuclear waste. These radionuclides are capable enough to produce potential health threat due to their long half-lives and effortless translocation into the human body. Besides the radionuclides, heavy metal contamination is also a serious issue. Heavy metals occur naturally in the earth crust and in low concentration, are also essential for the metabolism of living beings. Bioaccumulation of these heavy metals causes hazardous effects. These pollutants enter the human body directly via contaminated drinking water or through the food chain. This issue has drawn the attention of scientists throughout the world to device eco-friendly treatments to remediate the soil and water resources. Various physical and chemical treatments are being applied to clean the waste, but these techniques are quite expensive, complicated and comprise various side effects. One of the promising techniques, which has been pursued vigorously to overcome these demerits, is phytoremediation. The process is very effective, eco-friendly, easy and affordable. This technique utilizes the plants and its associated microbes to decontaminate the low and moderately contaminated sites efficiently. Many plant species are successfully used for remediation of contaminated soil and water systems. Remediation of these systems turns into a serious problem due to various anthropogenic activities that have

  16. Report on INL Activities for Uncertainty Reduction Analysis of FY11

    SciTech Connect

    G. Plamiotti; H. Hiruta; M. Salvatores

    2011-09-01

    This report presents the status of activities performed at INL under the ARC Work Package on 'Uncertainty Reduction Analyses' that has a main goal the reduction of uncertainties associated with nuclear data on neutronic integral parameters of interest for the design of advanced fast reactors under consideration by the ARC program. First, an analysis of experiments was carried out. For both JOYO (the first Japanese fast reactor) and ZPPR-9 (a large size zero power plutonium fueled experiment performed at ANL-W in Idaho) the performance of ENDF/B-VII.0 is quite satisfying except for the sodium void configurations of ZPPR-9, but for which one has to take into account the approximation of the modeling. In fact, when one uses a more detailed model (calculations performed at ANL in a companion WP) more reasonable results are obtained. A large effort was devoted to the analysis of the irradiation experiments, PROFIL-1 and -2 and TRAPU, performed at the French fast reactor PHENIX. For these experiments a pre-release of the ENDF/B-VII.1 cross section files was also used, in order to provide validation feedback to the CSWEG nuclear data evaluation community. In the PROFIL experiments improvements can be observed for the ENDF/B-VII.1 capture data in 238Pu, 241Am, 244Cm, 97Mo, 151Sm, 153Eu, and for 240Pu(n,2n). On the other hand, 240,242Pu, 95Mo, 133Cs and 145Nd capture C/E results are worse. For the major actinides 235U and especially 239Pu capture C/E's are underestimated. For fission products, 105,106Pd, 143,144Nd and 147,149Sm are significantly underestimated, while 101Ru and 151Sm are overestimated. Other C/E deviations from unity are within the combined experimental and calculated statistical uncertainty. From the TRAPU analysis, the major improvement is in the predicted 243Cm build-up, presumably due to an improved 242Cm capture evaluation. The COSMO experiment was also analyzed in order to provide useful feedback on fission cross sections. It was found out that ENDF

  17. Stopping powers of LiF thin films deposited onto self-supporting Al foils for swift protons

    NASA Astrophysics Data System (ADS)

    Damache, Smail; Moussa, Djamel; Ouichaoui, Saâd

    2013-08-01

    The energy losses of ˜(0.273-3.334) MeV protons in LiF thin films deposited by vacuum evaporation onto self-supporting Al foils have been measured using the transmission method. The thicknesses of selected and used LiF/Al target samples were accurately determined via systematic energy loss measurements for alpha particles from a very thin mixed 241Am/239Pu/233U radioactive source. The samples were investigated in detail for their stoichiometry and their impurity contents by backscattering Rutherford spectrometry and nuclear reaction analysis. Then, LiF stopping powers have been determined with overall relative uncertainty of less than 2.7% arising mainly from errors in the determination of target sample thicknesses. These S(E) data are reported and discussed in comparison to previous experimental data sets from the literature and to values calculated by the Sigmund-Schinner binary collision stopping theory both for molecular LiF, and for the LiF compound assuming Bragg-Kleeman's additivity rule. Our S(E) data show to be in excellent agreement with the latter theory for molecular LiF over the whole proton energy range explored, which supports the use of modified electronic hydrogen wave functions for evaluating atomic shell corrections in the case of low-Z2 target materials. In contrast, they exhibit a slightly increasing deviation from theoretical values derived for the LiF compound with assuming stopping force additivity as the proton energy decreases from E ≈ 400 keV towards lower proton velocities. This deviation in excess relative to experimental data, amounting only up to (at most) ˜2.5%, can be ascribed to strong effects of 2s-state valence electrons of Li atoms within the LiF compound. Besides, the comparison to values calculated by the SRIM-2008 computer code indicates that this program satisfactorily accounts for our S(E) data above E ≈ 1.30 MeV but underestimates them with substantially increasing deviations (up to ˜11%) towards lower proton

  18. Radionuclides in the Great Lakes basin.

    PubMed Central

    Ahier, B A; Tracy, B L

    1995-01-01

    The Great Lakes basin is of radiologic interest due to the large population within its boundaries that may be exposed to various sources of ionizing radiation. Specific radionuclides of interest in the basin arising from natural and artificial sources include 3H, 14C, 90Sr, 129I, 131I, 137Cs, 222Rn, 226Ra, 235U, 238U, 239Pu, and 241Am. The greatest contribution to total radiation exposure is the natural background radiation that provides an average dose of about 2.6 mSv/year to all basin residents. Global fallout from atmospheric nuclear weapons tests conducted before 1963 has resulted in the largest input of anthropogenic radioactivity into the lakes. Of increasing importance is the radionuclide input from the various components of the nuclear fuel cycle. Although the dose from these activities is currently very low, it is expected to increase if there is continued growth of the nuclear industry. In spite of strict regulations on design and operation of nuclear power facilities, the potential exists for a serious accident as a result of the large inventories of radionuclides contained in the reactor cores; however, these risks are several orders of magnitude less than the risks from other natural and man-made hazards. An area of major priority over the next few decades will be the management of the substantial amounts of radioactive waste generated by nuclear fuel cycle activities. Based on derived risk coefficients, the theoretical incidence of fatal and weighted nonfatal cancers and hereditary defects in the basin's population, attributable to 50 years of exposure to natural background radiation, is conservatively estimated to be of the order of 3.4 x 10(5) cases. The total number of attributable health effects to the year 2050 from fallout radionuclides in the Great Lakes basin is of the order of 5.0 x 10(3). In contrast, estimates of attributable health effects from 50 years of exposure to current nuclear fuel cycle effluent in the basin are of the order of 2

  19. Durability of Actinide Ceramic Waste Forms Under Conditions of Granitoid Rocks

    SciTech Connect

    Burakov, B. E.; Anderson, E. B.

    2002-02-26

    Three samples of {sup 239}Pu-{sup 241}Am-doped ceramics obtained from previous research were used for alteration experiments simulating corrosion of waste forms in ion-saturated solutions. These were ceramics based on: pyrochlore, (Ca,Hf,Pu,U,Gd){sub 2}Ti{sub 2}O{sub 7}, containing 10 wt.% Pu and 0.1 wt.% Am; zircon, (Zr,Pu)SiO{sub 4}, containing 5-6 wt.% Pu and 0.05 wt.% Am; cubic zirconia, (Zr,Gd,Pu)O{sub 2}, containing 10 wt.% Pu and 0.1 wt.% Am. All these samples were milled in an agate mortar to obtain powder with particle sizes less than 30 micron. Sample of granite taken from the depth 500-503 m was studied and then used for preparing ion-saturated water solutions. A rock sample was ground, washed and classified. A fraction with particle size 0.10-0.25 mm was selected for alteration experiments. Powdered ceramic samples were separately placed into deionized water together with ground granite (approximately 1gram granite per 12-ml water) in special Teflon{trademark} vessels and set at 90 C in the oven for 3 months. After alteration experiments, the ceramic powders were studied by precise XRD analysis. Aqueous solutions and granite grains were analyzed for Am and Pu contents. The results show that alteration did not cause significant phase transformation in all ceramic samples. For all altered samples, the Am contents in aqueous solutions after experiments were similar (approximately n x 10{sup 2} Bq/ml) as well as Am amounts absorbed on granite grains (approximately n x 10{sup 5} Bq/g). Results on Pu contents were varied: for the solutions--from 60 Bq/ml for pyrochlore ceramic to 2.1 x 10{sup 3} Bq/ml for zircon ceramic; and for the absorption on granite--from 2.6 x 10{sup 4} Bq/g for zirconia ceramic to 1.4-6.8 x 10{sup 5} Bq/g for pyrochlore and zircon ceramics.

  20. Elk and Deer Study, Material Disposal Area G, Technical Area 54: Source document

    SciTech Connect

    J. K. Ferenbaugh; P. R. Fresquez; M. H. Ebinger; G. J. Gonzales; P. A. Jordan

    1999-09-01

    As nuclear research has become more prevalent, environmental contamination from the disposal of radioactive waste has become a prominent issue. At Los Alamos National Laboratory (LANL) in northern New Mexico, radioactive contamination from disposal operations has raised some very specific concerns. Material Disposal Area G (Area G) is the primary low-level radioactive waste disposal site at LANL and occupies an area adjacent to land belonging to the Native American community of the Pueblo of San Ildefonso. Analyses of soil and vegetation collected from the perimeter of Area G have shown concentrations of radionuclides greater than background concentrations established for northern New Mexico. As a result, Pueblo residents had become concerned that contaminants from Area G could enter tribal lands through various ecological pathways. The residents specifically questioned the safety of consuming meat from elk and deer that forage near Area G and then migrate onto tribal lands. Consequently, this study addresses the uptake of {sup 3}H, {sup 90}Sr, {sup tot}U, {sup 238}Pu, {sup 239}Pu, {sup 241}Am, and {sup 137}Cs by elk (Cervus elaphus) and deer (Odocoileus hemionus) that forage around the perimeter of Area G and the associated doses to the animals and to humans who consume these animals. Radionuclide uptake by and internal dose to animals was estimated using equations modified from National Council on Radiological Protection Report 76. The Residual Radiation computer code was used to estimate the external dose to animals and the dose to humans consuming meat. Soil and water concentrations from the perimeter of Area G and from background regions in northern New Mexico were averaged over 4 years (1993--1996) and used as input data for the models. Concentration estimates generated by the model correspond to the concentration range measured in actual tissue samples from elk and deer collected at LANL. The highest dose estimates for both animals (0.028 mrad/d) and humans

  1. 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

  2. Functional sorbents for selective capture of plutonium, americium, uranium, and thorium in blood.

    PubMed

    Yantasee, Wassana; Sangvanich, Thanapon; Creim, Jeffery A; Pattamakomsan, Kanda; Wiacek, Robert J; Fryxell, Glen E; Addleman, R Shane; Timchalk, Charles

    2010-09-01

    Self-assembled monolayer on mesoporous supports (SAMMS) are hybrid materials created from attachment of organic moieties onto very high surface area mesoporous silica. SAMMS with surface chemistries including three isomers of hydroxypyridinone, diphosphonic acid, acetamide phosphonic acid, glycinyl urea, and diethylenetriamine pentaacetate (DTPA) analog were evaluated for chelation of actinides ((239)Pu, (241)Am, uranium, thorium) from blood. Direct blood decorporation using sorbents does not have the toxicity or renal challenges associated with traditional chelation therapy and may have potential applications for critical exposure cases, reduction of nonspecific dose during actinide radiotherapy, and for sorbent hemoperfusion in renal insufficient patients, whose kidneys clear radionuclides at a very slow rate. Sorption affinity (K(d)), sorption rate, selectivity, and stability of SAMMS were measured in batch contact experiments. An isomer of hydroxypyridinone (3,4-HOPO) on SAMMS demonstrated the highest affinity for all four actinides from blood and plasma and greatly outperformed the DTPA analog on SAMMS and commercial resins. In batch contact, a fifty percent reduction of actinides in blood was achieved within minutes, and there was no evidence of protein fouling or material leaching in blood after 24 h. The engineered form of SAMMS (bead format) was further evaluated in a 100-fold scaled-down hemoperfusion device and showed no blood clotting after 2 h. A 0.2 g quantity of SAMMS could reduce 50 wt.% of 100 ppb uranium in 50 mL of plasma in 18 min and that of 500 dpm mL(-1) in 24 min. 3,4-HOPO-SAMMS has a long shelf-life in air and at room temperature for at least 8 y, indicating its feasibility for stockpiling in preparedness for an emergency. The excellent efficacy and stability of SAMMS materials in complex biological matrices suggest that SAMMS can also be used as orally administered drugs and for wound decontamination. By changing the organic groups of

  3. Growth and luminescent properties of scintillators based on the single crystalline films of Lu{sub 3−x}Gd{sub x}Al{sub 5}O{sub 12}:Ce garnet

    SciTech Connect

    Zorenko, Yu; Gorbenko, V.; Vasylkiv, Ja; Zelenyj, A.; Fedorov, A.; Kucerkova, R.; Mares, J.A.; Nikl, M.; Bilski, P.; Twardak, A.

    2015-04-15

    Highlights: • Single crystalline films of Lu{sub 3−x}Gd{sub x}Al{sub 5}O{sub 12} garnets at x = 0 ÷ 3.0 were grown by LPE method onto YAG substrates. • Lattice constant of Lu{sub 3−}Gd{sub x}Al{sub 5}O{sub 12}:Ce film and the misfit m between films and YAG substrate changed linearly with increasing of Gd content. • Effective Gd{sup 3+}–Ce{sup 3+} energy transfer occurs in the Lu{sub 3−x}Gd{sub x}Al{sub 5}O{sub 12}:Ce films. • Best scintillation light yield is observed in the Lu{sub 3}Al{sub 5}O{sub 12}:Ce and Lu{sub 2.4}Gd{sub 0.6}Al{sub 5}O{sub 12}:Ce films. • Increase of the Gd content in x = 1.5–2.5 range results in decreasing the scintillation LY of Lu{sub 3−x}Gd{sub x}Al{sub 5}O{sub 12}:Ce films. - Abstract: The work is related to the growth of scintillators based on the single crystalline films (SCF) of Ce{sup 3+} doped Lu{sub 3−}Gd{sub x}Al{sub 5}O{sub 12} mixed rare-earth garnets by Liquid Phase Epitaxy (LPE) method. We have shown, that full set of Lu{sub 3−}Gd{sub x}Al{sub 5}O{sub 12} SCFs with x values ranging from 0 to 3.0 can be successfully crystallized by the LPE method onto Y{sub 3}Al{sub 5}O{sub 12} (YAG) substrates from the melt-solutions based on PbO-B{sub 2}O{sub 3} flux. The absorption, X-ray excited luminescence, photoluminescence, thermoluminescence and light yield measurements, the latter under excitation by α-particles of {sup 239}Pu and {sup 241}Am radioisotopes, were applied for their characterization.

  4. 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

  5. Plutonium in human urine: Normal levels in the US public. 1991 Annual report, Volume 2

    SciTech Connect

    Wrenn, M.E.; Singh, N.P.; Xue, Ying-Hua

    1997-03-01

    A neutron induced fission track method was successfully developed for assaying {sup 239}Pu in human urine with a detection limit below 20 aCi/sample. The technique involves the co-precipitation of {sup 239}Pu with rhodizonic acid, separation of {sup 239}Pu from potentially interfering natural uranium and other inorganic materials by ion-exchange techniques, collection of the sample onto lexan detectors, irradiation of sample in MIT reactor at a fluence of 1.1 x 10{sup 17} n/cm{sup 2}, etching of the lexan slide and counting the track either manually or by some automated counting system.

  6. Distribution of neptunium and plutonium in New Mexico lichen samples (Usnea arizonica) contaminated by atmospheric fallout

    DOE PAGES

    Oldham, Jr., Warren J.; Hanson, Susan K.; Lavelle, Kevin B.; ...

    2015-08-30

    In this study, the concentrations of 237Np, 239Pu and 240Pu were determined in lichen samples (Usnea arizonica) that were collected from ten locations in New Mexico between 2011 and 2013 using isotope dilution inductively-coupled plasma mass spectrometry (ID-ICP-MS). The observed isotopic ratios for 237Np/239Pu and 240Pu/239Pu indicate trace contamination from global and regional fallout (e.g. Trinity test and atmospheric testing at the Nevada Test Site). The fact that actinide contamination is detected in recent lichen collections suggests continuous re-suspension of fallout radionuclides even 50 years after ratification of the Limited Test Ban Treaty.

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

    NASA Astrophysics Data System (ADS)

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

    2012-01-01

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

  8. Seaborg's Plutonium? A Case Study in Nuclear Forensics

    NASA Astrophysics Data System (ADS)

    Norman, Eric B.; Thomas, Keenan J.; Telhami, Kristina E.

    2015-10-01

    Passive X-ray and gamma-ray analysis was performed on UC Berkeley's EH&S Sample S338. The object was found to contain 239Pu. No other radioactive isotopes were observed. The mass of 239Pu contained in this object was determined to be 2.0 +- 0.3 μg. These observations are consistent with the identification of this object as containing the 2.77- μg PuO2 (2.44 μg 239Pu) sample produced in 1942 and described by Glenn Seaborg and his collaborators as the first sample of 239Pu that was large enough to be weighed. This work was supported in part by the U.S. Dept. of Energy National Nuclear Security Administration under Award No. DE-NA0000979.

  9. Seaborg's plutonium? A case study in nuclear forensics

    NASA Astrophysics Data System (ADS)

    Norman, Eric B.; Thomas, Keenan J.; Telhami, Kristina E.

    2015-10-01

    Passive X-ray and gamma-ray analysis was performed on a curious sample from UC Berkeley's Hazardous Material Facility inventory, and the object was found to contain 239Pu. No other radioactive isotopes were observed. The mass of 239Pu contained in this object was determined to be 2.0 ± 0.3 μg. These observations are consistent with the identification of this object as containing the 2.77-μg PuO2 (2.44 μg 239Pu) sample produced in 1942 and described by Seaborg and his collaborators as the first sample of 239Pu that was large enough to be weighed.

  10. Fusion-breeder program

    SciTech Connect

    Moir, R.W.

    1982-11-19

    The various approaches to a combined fusion-fission reactor for the purpose of breeding /sup 239/Pu and /sup 233/U are described. Design aspects and cost estimates for fuel production and electricity generation are discussed. (MOW)

  11. a Microscopic Theory of Low Energy Fission:. Fragment Properties

    NASA Astrophysics Data System (ADS)

    Younes, W.; Gogny, D.; Schunck, N.

    2014-09-01

    We present fully microscopic time-dependent calculations of fission-fragment properties (mass distributions, pre-scission energies, total kinetic and excitation energies) for the 235U(n, f) and 239Pu (n, f) reactions. The mass distributions for both reactions have been obtained as a function of incident neutron energy from thermal to 5 MeV. The various energies have been calculated for the thermal 239Pu (n, f) reaction. We compare our calculations to experimental results, wherever possible.

  12. Evaluating criticality safety of TRU waste with NDA measurements and risk analyses

    SciTech Connect

    Hochel, R.C.; Hofstetter, K.J.; Sigg, R.A.; Winn, W.G.; Chay, S.C.

    1994-09-01

    The criticality safety of {sup 239}Pu in 55-gal. drums stored in TRU waste containers (concrete culverts) was evaluated using NDA neutron and gamma measurements and risk analyses. The neutron measurements yielded a {sup 239}Pu mass and k{sub eff} for a culvert, which contains up to 14 drums. The gamma measurements helped reveal and correct for any interfering neutron sources in the waste. Conservation probabilistic risk analyses were developed for both drums and culverts.

  13. Plutonium Isotopes ((239-241)Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed.

    PubMed

    Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Golser, Robin; Gómez-Guzmán, José Manuel; Korschinek, Gunther; Kortmann, Florian; Lierse von Gostomski, Christoph; Ludwig, Peter; Steier, Peter; Tazoe, Hirofumi; Yamada, Masatoshi

    2017-02-21

    The concentration of plutonium (Pu) and the isotopic ratios of (240)Pu to (239)Pu and (241)Pu to (239)Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular, (241)Pu is a well-suited indicator for a recent entry of Pu because (241)Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated (240)Pu/(239)Pu ratio of up to 0.22 ± 0.02 compared to global fallout ((240)Pu/(239)Pu = 0.180 ± 0.007), whereas all measured (241)Pu-to-(239)Pu ratios were consistent with nuclear weapon fallout ((241)Pu/(239)Pu < 2.4 × 10(-3)), which means that no impact from the Fukushima accident was detected. From the average (241)Pu-to-(239)Pu ratio of 8-2(+3) ×10(-4) at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the (239)Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.

  14. Plutonium isotope ratio variations in North America

    SciTech Connect

    Steiner, Robert E; La Mont, Stephen P; Eisele, William F; Fresquez, Philip R; Mc Naughton, Michael; Whicker, Jeffrey J

    2010-12-14

    Historically, approximately 12,000 TBq of plutonium was distributed throughout the global biosphere by thermo nuclear weapons testing. The resultant global plutonium fallout is a complex mixture whose {sup 240}Pu/{sup 239}Pu atom ratio is a function of the design and yield of the devices tested. The average {sup 240}Pu/{sup 239}Pu atom ratio in global fallout is 0.176 + 014. However, the {sup 240}Pu/{sup 239}Pu atom ratio at any location may differ significantly from 0.176. Plutonium has also been released by discharges and accidents associated with the commercial and weapons related nuclear industries. At many locations contributions from this plutonium significantly alters the {sup 240}Pu/{sup 239}Pu atom ratios from those observed in global fallout. We have measured the {sup 240}Pu/{sup 239}Pu atom ratios in environmental samples collected from many locations in North America. This presentation will summarize the analytical results from these measurements. Special emphasis will be placed on interpretation of the significance of the {sup 240}Pu/{sup 239}Pu atom ratios measured in environmental samples collected in the Arctic and in the western portions of the United States.

  15. Methods for the assessment of long-lived radionuclides in humans resulting from nuclear activities or accidents: Fission track analysis of trace amounts plutonium-239 and a copper hexacyanoferrate kit for monitoring radiocaesium

    NASA Astrophysics Data System (ADS)

    Johansson, Lena Camilla

    Fission track analysis (FTA) was developed to be applied to ultra-low levels of 239Pu in bioassay samples. An analytical protocol was established for the FTA processing. The detection limit was determined to 1.5 μBq and the calibration constant was 24 fission fragments per μBq 239Pu. Naturally occurring nuclides of thorium and uranium, present in biological and environmental samples, did not interfere in the determination of 239Pu. Self-absorption of fission fragments was shown to be insignificant. The study included the determination of 239Pu in urine samples from twenty Chernobyl clean-up workers. All urine samples contained activities below the detection limit for radioanalytical analysis using alpha spectrometry (0.5 mBq). Seven of the samples were further investigated using a thermal ionization mass spectrometer with a sensitivity of 106 atoms 239Pu. The content of 239Pu in the samples showed to be below 1μBq (106 atoms), with only one exception. It was not possible to draw any major conclusions from the 239Pu results, regarding the clean-up workers' exposure from radionuclides released by the Chernobyl accident. A kit was designed for selective adsorption of radiocaesium in urine samples to be used in situ by contaminated subjects. The kit consisted of copper hexacyanoferrate impregnated cotton filters held by filter holders for sample flow-through. After use, the adsorbed fraction of caesium was >=90% in urine samples. The kit facilitates the screening of a population exposed to radiocaesium. Parameters influencing the adsorption efficiency, such as potassium, sodium and calcium concentration of the sample and the sample pH, were investigated and shown to be insignificant for urine samples.

  16. Multimedia contaminant environmental exposure assessment methodology as applied to Los Alamos, New Mexico

    SciTech Connect

    Whelan, G.; Thompson, F.L.; Yabusaki, S.B.

    1983-02-01

    The MCEA (Multimedia Contaminant Environmental Exposure Assessment) methodology assesses exposures to air, water, soil, and plants from contaminants released into the environment by simulating dominant mechanisms of contaminant migration and fate. The methodology encompasses five different pathways (i.e., atmospheric, terrestrial, overland, subsurface, and surface water) and combines them into a highly flexible tool. The flexibility of the MCEA methodology is demonstrated by encompassing two of the pathways (i.e., overland and surface water) into an effective tool for simulating the migration and fate of radionuclides released into the Los Alamos, New Mexico region. The study revealed that: (a) the /sup 239/Pu inventory in lower Los Alamos Canyon increased by approximately 1.1 times for the 50-y flood event; (b) the average contaminant /sup 239/Pu concentrations (i.e., weighted according to the depth of the respective bed layer) in lower Los Alamos Canyon for the 50-y flood event decreased by 5.4%; (c) approx. 27% of the total /sup 239/Pu contamination resuspended from the entire bed (based on the assumed cross sections) for the 50-y flood event originated from lower Pueblo Canyon; (d) an increase in the /sup 239/Pu contamination of the bed followed the general deposition patterns experienced by the sediment in Pueblo-lower Los Alamos Canyon; likewise, a decrease in the /sup 239/Pu contamination of the bed followed general sediment resuspension patterns in the canyon; (e) 55% of the /sup 239/Pu reaching the San Ildefonso Pueblo in lower Los Alamos Canyon originated from lower Los Alamos Canyon; and (f) 56% of the /sup 239/Pu contamination reaching the San Ildefonso Pueblo in lower Los Alamos Canyon was carried through towards the Rio Grande. 47 references, 41 figures, 29 tables.

  17. [Influence of Professional Contact with Plutonium-239 on Indicators of the Immune Status of the Personnel at Siberian Chemical Plant].

    PubMed

    Oradovskaya, I V; Radzivil, T T

    2015-01-01

    The results of the examination and monitoring of the personnel at the Siberian Chemical Plant (SChP) and adult population of Seversk are presented. The results of primary examination of the personnel who professionally contact the ionizing radiation (IR) from external sources and incorporated 239Pu showed that clinical symptoms of dysfunction of the immune system manifested themselves with a frequency of 75.30%. Infectious-inflammatory diseases (46.95%) and the combined pathology of infectious and allergic character (20.12%) were the most widespread. The allergic diseases (AD) without manifestations of an infectious component were observed not often (7.62%). The monitoring which was carried out for 10 years revealed a decrease in a percentage of persons with clinical signs of disorders of the immune system up to 60.68% among the personnel at the Chemical-Steel Plant and even more among the whole group of the studied personnel at SChP--49.68% (389 : 783). Among the population their frequency made up 51.78%. Features of clinical manifestations of dysfunction ofthe immune system depending on accumulation of 239Pu in the organism are established. Similar dynamics of infectious and infectious and allergic syndromes is revealed when the activity of 239Pu is 40 nCi. AD frequency reliably increased .when the activity of 239Pu is 20 nCi, but if accumulation is higher than 20-40 nCi it decreases and again increases when the activity is over 40 nCi. Pathologies of infectious and allergic genesis are most often observed when the content of 239Pu in an organism is over 40 nCi. Indicators of the immune status (IS) of the personnel at SChP with incorporated 239Pu are analyzed. 59 people--carriers of 239Pu and 408 people without 239Pu accumulated in an organism are examined. In comparison with the control, IS indicators characteristic for all dose loading groups are revealed: increase of lymphocytes, existence of dissociation in indicators of relative and absolute values of the T

  18. Biosorption of americium-241 by immobilized Rhizopus arrihizus.

    PubMed

    Liao, Jiali; Yang, Yuanyou; Luo, Shunzhong; Liu, Ning; Jin, Jiannan; Zhang, Taiming; Zhao, Pengji

    2004-01-01

    Rhizopus arrihizus (R. arrihizus), a fungus, which in previous experiments had shown encouraging ability to remove 241Am from solutions, was immobilized by calcium alginate and other reagents. The various factors affecting 241Am biosorption by the immobilized R. arrihizus were investigated. The results showed that not only can immobilized R. arrihizus adsorb 241Am as efficiently as free R. arrihizus, but that also can be used repeatedly or continuously. The biosorption equilibrium was achieved within 2 h, and more than 94% of 241Am was removed from 241Am solutions of 1.08 MBq/l by immobilized R. arrihizu in the pH range 1-7. Temperature did not affect the adsorption on immobilized R. arrihizus in the range 15-45 degrees C. After repeated adsorption for 8 times, the immobilized R. arrihizus still adsorbed more than 97% of 241Am. At this time, the total adsorption of 241Am was more than 88.6 KBq/g, and had not yet reached saturation. Ninety-five percent of the adsorbed 241Am was desorbed by saturated EDTA solution and 98% by 2 mol/l HNO(3).

  19. Extraction of actinide (III, IV, V, VI) ions and TcO4- byN,N,N',N'- tetraisobutyl-3-oxa-glutaramide

    SciTech Connect

    Tian, Guoxin; Zhang, Ping; Wang, Jianchen; Rao, Linfeng

    2005-05-01

    The extraction behavior of U(VI), Np(V), Pu(IV), Am(III), and TcO{sub 4}{sup -} with N, N, N', N'-tetraisobutyl-3-oxa-glutaramide (TiBOGA) were investigated. An organic phase of 0.2 mol/L TiBOGA in 40/60% (V/V) 1-octanol/kerosene showed good extractability for actinides (III, IV, V VI) and TcO{sub 4}{sup -}from aqueous solutions of HNO{sub 3} (0.1 to 4 mol/L). At 25 C, the distribution ratio of the actinide ions (D{sub An}) generally increased as the concentration of HNO{sub 3} in the aqueous phase was increased from 0.1 to 4 mol/L, while the D{sub Tc} at first increased, then decreased, with a maximum of 3.0 at 2 mol/L HNO{sub 3}. Based on the slope analysis of the dependence of D{sub M} (M = An or Tc) on the concentrations of reagents, the formula of extracted complexes were assumed to be UO{sub 2}L{sub 2}(NO{sub 3}){sub 2}, NpO{sub 2}L{sub 2}(NO{sub 3}), PuL(NO{sub 3}){sub 4}, AmL{sub 3}(NO{sub 3}){sub 3}, and HL{sub 2}(TcO{sub 4}) where L = TiBOGA. The enthalpy and entropy of the corresponding extraction reactions, {Delta}{sub r}H and {Delta}{sub r}S, were calculated from the dependence of D on temperature in the range of 15-55 C. For U(VI), Np(V), Am(III) and TcO{sub 4}{sup -}, the extraction reactions are enthalpy driven and disfavored by entropy ({Delta}{sub r}H < 0 and {Delta}{sub r}S < 0). In contrast, the extraction reaction of Pu(IV) is entropy driven and disfavored by enthalpy ({Delta}{sub r}H > 0 and {Delta}{sub r}S > 0). A test run with 0.2 mol/L TiBOGA in 40/60% 1-octanol/kerosene was performed to separate actinides and TcO{sub 4}{sup -} from a simulated acidic high-level liquid waste (HLLW), using tracer amounts of {sup 238}U(VI), {sup 237}Np(V), {sup 239}Pu(VI), {sup 241}Am(III) and {sup 99}TcO{sub 4}{sup -}. The distribution ratios of U(VI), Np(V), Pu(VI), Am(III) and TcO{sub 4}{sup -} were 12.4, 3.9, 87, > 1000 and 1.5, respectively, confirming that TiBOGA is a promising extractant for the separation of all actinides and TcO{sub 4}{sup -} from

  20. OSMOSE experiment representativity studies.

    SciTech Connect

    Aliberti, G.; Klann, R.; Nuclear Engineering Division

    2007-10-10

    The OSMOSE program aims at improving the neutronic predictions of advanced nuclear fuels through measurements in the MINERVE facility at the CEA-Cadarache (France) on samples containing the following separated actinides: Th-232, U-233, U-234, U-235, U-236, U-238, Np-237, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, Am-241, Am-243, Cm-244 and Cm-245. The goal of the experimental measurements is to produce a database of reactivity-worth measurements in different neutron spectra for the separated heavy nuclides. This database can then be used as a benchmark for integral reactivity-worth measurements to verify and validate reactor analysis codes and integral cross-section values for the isotopes tested. In particular, the OSMOSE experimental program will produce very accurate sample reactivity-worth measurements for a series of actinides in various spectra, from very thermalized to very fast. The objective of the analytical program is to make use of the experimental data to establish deficiencies in the basic nuclear data libraries, identify their origins, and provide guidelines for nuclear data improvements in coordination with international programs. To achieve the proposed goals, seven different neutron spectra can be created in the MINERVE facility: UO2 dissolved in water (representative of over-moderated LWR systems), UO2 matrix in water (representative of LWRs), a mixed oxide fuel matrix, two thermal spectra containing large epithermal components (representative of under-moderated reactors), a moderated fast spectrum (representative of fast reactors which have some slowing down in moderators such as lead-bismuth or sodium), and a very hard spectrum (representative of fast reactors with little moderation from reactor coolant). The different spectra are achieved by changing the experimental lattice within the MINERVE reactor. The experimental lattice is the replaceable central part of MINERVE, which establishes the spectrum at the sample location. This configuration

  1. Berkelium

    NASA Astrophysics Data System (ADS)

    Hobart, David E.; Peterson, Joseph R.

    As was the case for the previously discovered transuranium elements, element 97 was first produced via a nuclear bombardment reaction. In December 1949 ion-exchange separation of the products formed by the bombardment of 241Am with accelerated alpha particles provided a new electron-capture activity eluting just ahead of curium (Thompson et al., 1950a,b). This activity was assigned to an isotope (mass number 243) of element 97. The new element was named berkelium after Berkeley, California, USA, the city of its discovery, in a manner parallel to the naming of its lanthanide analog, terbium, after Ytterby, Sweden. The initial investigations of the chemical properties of berkelium were limited to tracer experiments (ion exchange and coprecipitation), and these were sufficient to establish the stability of Bk(III) and the accessibility of Bk(IV) in aqueous solution and to estimate the electrochemical potential of the Bk(IV)/Bk(III) couple (Thompson et al., 1950b,c). Because a complete study of the chemistry of an element is not possible by tracer methods alone, a program for long-term neutron irradiation of about 8 g of 239Pu was initiated in 1952 in the Materials Testing Reactor (Arco, Idaho, USA) to provide macroquantities of berkelium (Cunningham, 1959). In 1958 about 0.6 mg of 249Bk was separated, purified, and used in experiments to determine the absorption spectrum of Bk(III) in aqueous solution and to measure the magnetic susceptibility of Bk(III) (Cunningham, 1959). No Bk(III) absorption was observed over the wavelength range 450-750 nm, but an upper limit of about 20 was set for the molar absorptivity of any Bk(III) absorption in this wavelength region. The magnetic susceptibility, measured from 77 to 298 K with the Bk(III) ions sorbed in a single bead of cation-exchange resin, was found to conform to the Curie-Weiss law with an effective moment of 8.7 mB, suggesting a 5f8 electronic configuration for the Bk(III) ion. The first structure determination of a

  2. Release of the 2008 Evaluated Nuclear Data Library (ENDL2008)

    SciTech Connect

    Brown, D A; Descalle, M; Hoffman, R; Kelley, K; Navratil, P; Pruet, J; Summers, N; Thompson, I; Vogt, R

    2009-05-08

    Livermore's N-Division is now releasing the first version of a major new nuclear data library. This includes some 500 evaluations (roughly four times the number in the previous standard) and many physics improvements important for calculating weapon performance, output effects, attribution signatures, key radiochemical diagnostics and performance of conventional and hybrid fission/fusion reactors. As this library is more extensive and on a much firmer nuclear physics footing than the previous ENDL99 it should become, after a period of trial use by the applied community, the new standard for programmatic applications at Livermore. This work was supported by ASC-PEM and Campaign 4. Our basic philosophy in this release was to adopt the best work of the world's different nuclear data efforts. We have drawn heavily from the U.S. ENDF project (led by Brookhaven), the Japanese JENDL project (JAEA), and the European JEFF project (NEA). Because those efforts tend to focus on reactor applications they do not include an account of the charged particles emitted following a reaction. To enable broader applications we have used theory-based calculations to add a complete description of charged particles in all evaluations in the new library. This release also includes results from the last ten years of theory and experimental work here at Livermore. Some of the most important results include the surrogate campaign for unstable uranium isotopes, the LLNL/LANL 239Pu(n,2n) evaluation, the 241Am(n,2n) evaluation validated by the recent Livermore-led experiments, and measurements of 48Ti(n,2n). As well, we have adopted more than a hundred theory-based evaluations for radiochemical diagnostics completed by R. Hoffman and M. Mustafa and that use improved optical models, level densities, and decay scheme evaluations from the theory effort. These were extended to be transport complete (they now include a description of all of the particles emitted in reactions) to enable their use in

  3. Thin film AlSb carrier transport properties and room temperature radiation response

    NASA Astrophysics Data System (ADS)

    Vaughan, Erin Ivey

    from 241Am, 252Cf, and 239Pu sealed sources, with good peak resolution and signal to noise response. Both GaSb PN diodes and AlSb PIN diodes exhibited larger pulses for smaller surface area samples, in good agreement with voltage-capacitance relationships for junctions. Microwave photoconductive decay (MW-PCD) measurements were performed on the Hall samples to determine the effect of doping on the minority carrier lifetime. Contrary to expectations, more heavily doped samples presented with longer decay times, some as large as hundreds of microseconds. There also appeared to be multiple exponential decay curves, potentially associated with different decay mechanisms. Collectively, the studies presented here reinforce the predicted nature of AlSb with respect to radiation detection.

  4. Possible differences in biological availability of isotopes of plutonium: Report of a workshop

    SciTech Connect

    Kercher, J.R.; Gallegos, G.M.

    1993-09-01

    This paper presents the results of a workshop conducted on the apparent different bioavailability of isotopes {sup 238}Pu and {sup 239}Pu. There is a substantial body of evidence that {sup 238}Pu as commonly found in the environment is more biologically available than {sup 239}Pu. Studies of the Trinity Site, Nevada Test Site from nonnuclear and nuclear events, Rocky Flats, Enewetak and Bikini, and the arctic tundra support this conclusion and indicate that the bioavailability of {sup 238}Pu is more than an order of magnitude greater than that of {sup 239}Pu. Plant and soil studies from controlled environments and from Savannah River indicate no isotopic difference in availability of Pu to plants; whereas studies at the Trinity Site do suggest a difference. While it is possible that these observations can be explained by problems in the experimental procedure and analytical techniques, this possibility is remote given the ubiquitous nature of the observations. Studies of solubility of Pu in the stomach contents of cattle grazing at the Nevada Test Site and from fish from Bikini Atoll both found that {sup 238}Pu was more soluble than {sup 239}Pu. Studies of the Los Alamos effluent stream indicate that as particle size decreases, the content of {sup 238}Pu relative to {sup 239}Pu increases.

  5. 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

  6. Assessment of Degree of Applicability of Benchmarks for Gadolinium Using KENO V.a and the 238-Group SCALE Cross-Section Library

    SciTech Connect

    Goluoglu, S.

    2003-12-01

    A review of the degree of applicability of benchmarks containing gadolinium using the computer code KENO V.a and the gadolinium cross sections from the 238-group SCALE cross-section library has been performed for a system that contains {sup 239}Pu, H{sub 2}O, and Gd{sub 2}O{sub 3}. The system (practical problem) is a water-reflected spherical mixture that represents a dry-out condition on the bottom of a sludge receipt and adjustment tank around steam coils. Due to variability of the mixture volume and the H/{sup 239}Pu ratio, approximations to the practical problem, referred to as applications, have been made to envelop possible ranges of mixture volumes and H/{sup 239}Pu ratios. A newly developed methodology has been applied to determine the degree of applicability of benchmarks as well as the penalty that should be added to the safety margin due to insufficient benchmarks.

  7. Identifying Sources of Non-fallout Nuclear Contamination in Hudson River Sediments by Plutonium and Neptunium isotope ratios.

    NASA Astrophysics Data System (ADS)

    Kenna, T. C.; Chillrud, S. N.

    2002-12-01

    In an effort to identify and characterize nuclear contaminants released from sources contained within the Hudson River drainage basin, Pu isotopes and 237Np have been measured in a series of sediment cores collected from various locations within the region. During the last several decades, the Hudson River has received input of radioactive contamination from several sources. The first and most significant, has been global fallout, which was a result of atmospheric testing of nuclear weapons primarily by governments of the United States and Former Soviet Union in the 1950s and 1960s. The second, is contamination resulting from reactor releases at the Indian Point Nuclear Power Plant (IPNPP) located on the Hudson River about 35 miles north of New York City. This facility began operation in 1962. A third source of radioactive contamination to the region is contamination resulting from activities at the Knolls Atomic Power Laboratory (KAPL) located on the Mohawk River, which began operation in 1946. Our research entails identifying different sources of nuclear contamination by measurement of plutonium and neptunium isotopic ratios by inductively coupled plasma mass spectrometry (ICP-MS). The isotopic composition of a nuclear contaminant is a sensitive indicator of its origin. By comparing the isotopic composition measured in fluvial sediments to mean values reported for global fallout (i.e. 240Pu/239Pu = 0.18 ñ 0.014, 237Np/239Pu = 0.48 ñ 0.07, and 241Pu/239Pu = .00194 ñ 00028) it is possible to identify contaminants as non-fallout in origin. To date, we have analyzed selected samples from 3 sediment cores collected from the following locations: 1) the Mohawk River downstream of KAPL, 2) the Hudson River above its confluence with the Mohawk River, and 3) the lower Hudson River at a location in close proximity to IPNPP. Isotopic analysis of sediments from the Mohawk River indicates contamination that is clearly non-fallout in origin (240Pu/239Pu ranges between 0

  8. Feasibility study of plutonium isotopic analysis of resin beads by nondestructive gamma-ray spectroscopy

    SciTech Connect

    Li, T.K.

    1985-01-01

    We have initiated a feasibility study on the use of nondestructive low-energy gamma-ray spectroscopy for plutonium isotopic analysis on resin beads. Seven resin bead samples were measured, with each sample containing an average of 9 ..mu..g of plutonium; the isotopic compositions of the samples varied over a wide range. The gamma-ray spectroscopy results, obtained from 4-h counting-time measurements, were compared with mass spectrometry results. The average ratios of gamma-ray spectroscopy to mass spectrometry were 1.014 +- 0.025 for /sup 238/Pu//sup 239/Pu, 0.996 +- 0.018 for /sup 240/Pu//sup 239/Pu, and 0.980 +- 0.038 for /sup 241/Pu//sup 239/Pu. The rapid, automated, and accurate nondestructive isotopic analysis of resin beads may be very useful to process technicians and International Atomic Energy Agency inspectors. 3 refs., 1 fig., 3 tabs.

  9. The effect of isotope on the dosimetry of inhaled plutonium oxide

    SciTech Connect

    Guilmette, R.A., Griffith, W.C.; Hickman, A.W.

    1991-12-31

    Results of experimental studies in which animals inhaled {sup 238}PuO{sub 2} or {sup 239}PuO{sub 2} aerosols have shown that the biokinetics and associated radiation dose patterns for these two isotopes differ significantly due to differences in in-vivo solubility caused by the 260-fold difference in specific activity between {sup 238}PuO{sub 2} and {sup 239}PuO{sub 2}. We have adapted a biokinetics and dosimetry model derived from results of the ITRI dog studies to humans and have calculated dose commitments and annual limits on intake (ALI) for both Pu isotopes. Our results show that the ALI calculated in this study is one-third that for class Y {sup 238}Pu from ICRP 30, and one-half or equal to that for class Y {sup 239}Pu, depending on how activity in the thoracic lymph nodes is treated dosimetrically.

  10. Effects of combined exposure of F344 rats to radiation and chronically inhaled cigarette smoke

    SciTech Connect

    Finch, G.L.; Nikula, K.J.; Barr, E.B.

    1995-12-01

    Nuclear workers may be exposed to radiation in various forms, such as low-LET {gamma}-irradiation or {alpha}-irradiation from inhaled {sup 239}PuO{sub 2} particles. These workers may then have increased risk for lung cancer compared to the general population. Of additional concern is the possibility that interactions between radiation and other carcinogens may increase the risk of cancer induction, compared to the risks from either type of agent alone. An important and common lung carcinogen is cigarette smoke. The purpose of this project is to better determine the combined effects of chronically inhaled cigarette smoke and either inhaled {sup 239}PuO{sub 2} or external, thoracic X-irradiation on the induction of lung cancer in rats. Histologic and dosimetric evaluations of rats in the CS + {sup 239}PuO{sub 2} study continue, and the study of CS + X rays is beginning.

  11. Resolving global versus local/regional Pu sources in the environment using sector ICP-MS

    USGS Publications Warehouse

    Ketterer, M.E.; Hafer, K.M.; Link, C.L.; Kolwaite, D.; Wilson, Jim; Mietelski, J.W.

    2004-01-01

    Sector inductively coupled plasma mass spectrometry is a versatile method for the determination of plutonium activities and isotopic compositions in samples containing this element at fallout levels. Typical detection limits for 239+240Pu are 0.1, 0.02 and 0.002 Bq kg -1Pu for samples sizes of 0.5 g, 3 g, and 50 g of soil, respectively. The application of sector ICP-MS-based Pu determinations is demonstrated in studies in sediment chronology, soil Pu inventory and depth distribution, and the provenance of global fallout versus local or regional Pu sources. A sediment core collected from Sloans Lake (Denver, Colorado, USA) exhibits very similar 137Cs and 239+240Pu activity profiles; 240Pu/239Pu atom ratios indicate possible small influences from the Nevada Test Site and/or the Rocky Flats Environmental Technology Site. An undisturbed soil profile from Lockett Meadow (Flagstaff, Arizona, USA) exhibits an exponential decrease in 239+240Pu activity versus depth; 240Pu/239Pu in the top 3 cm is slightly lower than the global fallout range of 0.180 ?? 0.014 due to possible regional influence of Nevada Test Site fallout. The 239??240Pu inventory at Lockett Meadow is 56 ?? 4 Bq m-2, consistent with Northern Hemisphere mid-latitude fallout. Archived NdF3 sources, prepared from Polish soils, demonstrate that substantial 239+240Pu from the 1986 Chernobyl disaster has been deposited in north eastern regions of Poland; compared to global fallout, Chernobyl Pu exhibits higher abundances of 240Pu and 241Pu. The ratios 240Pu/239pu and 241Pu/239Pu co-vary and range from 0.186-0.348 and 0.0029-0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407??[240Pu/239Pu] - 0.0413; r2 = 0.9924). ?? The Royal Society of Chemistry 2004.

  12. Characterization of Pu concentration and its isotopic composition in a reference fallout material.

    PubMed

    Zhang, Yongsan; Zheng, Jian; Yamada, Masatoshi; Wu, Fengchang; Igarashi, Yasuhito; Hirose, Katsumi

    2010-02-01

    Because there is no reference material for fallout plutonium isotope monitoring, preparation of such a material is necessary for quality control of fallout radionuclides analysis for atmospheric environmental studies. In this work, we report the characterization of Pu activity and its isotopic composition in a reference fallout material prepared by the Meteorological Research Institute (MRI), Japan. This material was prepared from samples collected at 14 stations throughout Japan in 1963-1979, with reference values of (137)Cs, (90)Sr and (239)(+)(240)Pu activities. We analyzed the activities of (239)(+)(240)Pu and (241)Pu, and the atom ratios of (240)Pu/(239)Pu and (241)Pu/(239)Pu using an isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The (239)(+)(240)Pu activities in this fallout material using acid leaching and total digestion were 6.56+/-0.20 mBq/g and 6.79+/-0.16 mBq/g, respectively. Atom ratios of (240)Pu/(239)Pu were 0.1915+/-0.0030 and 0.1922+/-0.0044, respectively. Both (240)Pu/(239)Pu and (241)Pu/(239)Pu atom ratios were slightly higher than those of global fallout, which could be attributed to the deposition of fallout radionuclides resulting from the Chinese nuclear weapons tests conducted in the 1970s. The dominant host phases of (239)(+)(240)Pu were found to be organic matter-sulfides (70%) with a relative high (240)Pu/(239)Pu atom ratio, and Fe-Mn oxides (19%) using a sequential extraction method.

  13. Self-regulating neutron coincidence counter

    DOEpatents

    Baron, N.

    1980-06-16

    A device for accurately measuring the mass of /sup 240/Pu and /sup 239/Pu in a sample having arbitrary moderation and mixed with various contaminants. The device utilizes a thermal neutron well counter which has two concentric rings of neutron detectors separated by a moderating material surrounding the well. Neutron spectroscopic information derived by the two rings of detectors is used to measure the quantity of /sup 239/Pu and /sup 240/Pu in device which corrects for background radiation, deadtime losses of the detector and electronics and various other constants of the system.

  14. Active and passive CT for waste assay using LaBr3(Ce) detector

    NASA Astrophysics Data System (ADS)

    Roy, Tushar; More, M. R.; Ratheesh, Jilju; Sinha, Amar

    2017-01-01

    An active and passive computed tomography system has been developed that localizes and quantifies 239Pu in a waste drum. The active (transmission) measurement uses an external gamma source and LaBr3(Ce) detector to determine the attenuation map of waste drum contents at different selected energies. The passive (emission) measurement uses multiple LaBr3(Ce) detectors to record the spectra of gamma-rays emitted from within the drum. The active and passive data sets are then coupled to quantitatively assay drum contents for 239Pu.

  15. Nuclear waste forms for actinides.

    PubMed

    Ewing, R C

    1999-03-30

    The disposition of actinides, most recently 239Pu from dismantled nuclear weapons, requires effective containment of waste generated by the nuclear fuel cycle. Because actinides (e.g., 239Pu and 237Np) are long-lived, they have a major impact on risk assessments of geologic repositories. Thus, demonstrable, long-term chemical and mechanical durability are essential properties of waste forms for the immobilization of actinides. Mineralogic and geologic studies provide excellent candidate phases for immobilization and a unique database that cannot be duplicated by a purely materials science approach. The "mineralogic approach" is illustrated by a discussion of zircon as a phase for the immobilization of excess weapons plutonium.

  16. Applications of Photonuclear Physics for International Safeguards and Security

    SciTech Connect

    Johnson, M S; Hall, J M; McNabb, D P; McFarland, J; Norman, E; Bertozzi, W; Korbly, S; Ledoux, R; Park, W

    2010-04-16

    Studies of nuclear resonance fluorescence based applications are presented. Important for these applications are data for isotopes such as {sup 239}Pu. Nuclear resonance fluorescence measurements of {sup 239}Pu were performed at the free electron laser facility at UC Santa Barbara using photons from a bremsstrahlung beam with an endpoint energies between 4.0 MeV and 5.5 MeV. Though no discrete states with significant confidence level were measured, we have excluded the region above 27(3) eV-barns, or 4-sigma, where we would expect only a small chance of false positives. Details of the measurements and the results are presented here.

  17. Subchronic inhalation of carbon tetrachloride alters the tissue retention of acutely inhaled plutonium-239 nitrate in F344 rats and syrian golden hamsters

    SciTech Connect

    Benson, J.M.; Barr, E.B.; Lundgren, D.L.

    1995-12-01

    Carbon tetrachloride (CCl{sub 4}) has been used extensively in the nuclear weapons industry, so it is likely that nuclear plant workers have been exposed to both CCl{sub 4} and plutonium compounds. Future exposures may occur during {open_quotes}cleanup{close_quotes} operations at weapons productions sites such as the Hanford, Washington, and Rocky Flats, Colorado, facilities. Inhalation of 20 and 100 ppm CCl{sub 4} by hamsters reduces uptake of {sup 239}Pu solubilized from lung, shunting the {sup 239}Pu to the skeleton.

  18. Plutonium isotopes derived from Nagasaki atomic bomb in the sediment of Nishiyama reservoir at Nagasaki, Japan.

    PubMed

    Saito-Kokubu, Y; Esaka, F; Yasuda, K; Magara, M; Miyamoto, Y; Sakurai, S; Usuda, S; Yamazaki, H; Yoshikawa, S; Nagaoka, S

    2007-04-01

    The source of plutonium in sediments deposited at Nishiyama reservoir at Nagasaki was characterized by their (240)Pu/(239)Pu atom ratio. The average ratio was approximately 0.03, except in two layers. The main source of the plutonium was the Nagasaki atomic bomb. The plutonium continues to flow into the reservoir even now. The (240)Pu/(239)Pu atom ratios in two layers were higher than the average, which showed that plutonium in these layers were made of those of nuclear tests added to those of the atomic bomb.

  19. Americium-241 and plutonium-237 turnover in mussels ( Mytilus galloprovincialis) living in field enclosures

    NASA Astrophysics Data System (ADS)

    Guary, J. C.; Fowler, S. W.

    1981-02-01

    Loss of 241Am and 237Pu from contaminated mussels ( Mytilus galloprovincialis) living in situ in the Mediterranean Sea is described as the sum of three exponential functions. In the case of 241Am, two short-lived compartments representing a total of 80% of the incorporated radionuclide turned over rapidly with biological half-lives of 2 and 3 weeks. The remaining fraction of 241Am, associated with a long-lived compartment, was lost at an extremely slow rate ( Tb1/2=1·3 years). Plutonium-237 turnover in the two short-lived compartments (containing 70% of the Pu) was more rapid ( Tb1/2=1-2 days and 2 weeks) than that of 241Am; however, there was some indication that subsequent loss rates of the two radionuclides in long-lived compartments may be similar if determined over comparable periods of time. Loss rates of 241Am differed for the various tissues, with the most rapid rates occurring in gill, viscera and shell. Abrupt changes in loss observed in muscle and mantle suggested a translocation of 241Am to muscle and mantle during depuration. Whole shell contained by far the largest fraction (˜90%) of both 241Am and 237Pu taken up; in addition, these radionuclides are not irreversibly bound to mussel shell but readily leach into the water. These observations suggest that mollusc shell may influence the biogeochemistry of transuranic elements in littoral zones.

  20. Americium behaviour in plastic vessels.

    PubMed

    Legarda, F; Herranz, M; Idoeta, R; Abelairas, A

    2010-01-01

    The adsorption of (241)Am dissolved in water in different plastic storage vessels was determined. Three different plastics were investigated with natural and distilled waters and the retention of (241)Am by these plastics was studied. The same was done by varying vessel agitation time, vessel agitation speed, surface/volume ratio of water in the vessels and water pH. Adsorptions were measured to be between 0% and 70%. The adsorption of (241)Am is minimized with no water agitation, with PET or PVC plastics, and by water acidification.

  1. Determination of plutonium isotopes in seawater reference materials using isotope-dilution ICP-MS.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2012-09-01

    We analyzed the activities of (239)Pu, (240)Pu, (239+240)Pu, (241)Pu, the ratio of number of atoms (atom ratio) for (240)Pu/(239)Pu, and the activity ratio of (241)Pu/(239+240)Pu in seawater reference materials, IAEA-443 and IAEA-381, using a highly sensitive isotope dilution sector field inductively coupled plasma mass spectrometry method. With a mean chemical yield of 65% determined with (242)Pu as a tracer, we found that the experimentally established values in IAEA-443 for (239)Pu, (240)Pu, (241)Pu and (239+240)Pu activities are almost the same as those in IAEA-381. Regarding the (239+240)Pu activity, we provided the most precise and accurate result among the twelve laboratories, which participated in the interlaboratory comparison. In addition, for the (240)Pu/(239)Pu atom ratio, our results for IAEA-381 (0.2315±0.0008) and IAEA-443 (0.2325±0.0008) are in good agreement with the IAEA information value (0.229±0.006), but have much smaller uncertainty. Since the new seawater reference material, IAEA-443, is commercially available, it can be used not only for method validation for seawater plutonium isotope ratio and activity analysis, but also for more general use as a plutonium isotope standard for mass discrimination correction for other environmental samples.

  2. Spatial and temporal distribution of Pu in the Northwest Pacific Ocean using modern coral archives.

    PubMed

    Lindahl, Patric; Andersen, Morten B; Keith-Roach, Miranda; Worsfold, Paul; Hyeong, Kiseong; Choi, Min-Seok; Lee, Sang-Hoon

    2012-04-01

    Historical (239)Pu activity concentrations and (240)Pu/(239)Pu atom ratios were determined in skeletons of dated modern corals collected from three locations (Chuuk Lagoon, Ishigaki Island and Iki Island) to identify spatial and temporal variations in Pu inputs to the Northwest Pacific Ocean. The main Pu source in the Northwest Pacific is fallout from atmospheric nuclear weapons testing which consists of global fallout and close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands. PPG close-in fallout dominated the Pu input in the 1950s, as was observed with higher (240)Pu/(239)Pu atom ratios (>0.30) at the Ishigaki site. Specific fallout Pu contamination from the Nagasaki atomic bomb and the Ivy Mike thermonuclear detonation at the PPG were identified at Ishigaki Island from the (240)Pu/(239)Pu atom ratios of 0.07 and 0.46, respectively. During the 1960s and 1970s, global fallout was the major Pu source to the Northwest Pacific with over 60% contribution to the total Pu. After the cessation of the atmospheric nuclear tests, the PPG again dominated the Pu input due to the continuous transport of remobilised Pu from the Marshall Islands along the North Equatorial Current and the subsequent Kuroshio Current. The Pu contributions from the PPG in recent coral bands (1984 onwards) varied over time with average estimated PPG contributions between 54% and 72% depending on location.

  3. Application of Reactor Antineutrinos: Neutrinos for Peace

    NASA Astrophysics Data System (ADS)

    Suekane, F.

    2013-02-01

    In nuclear reactors, 239Pu are produced along with burn-up of nuclear fuel. 239Pu is subject of safeguard controls since it is an explosive component of nuclear weapon. International Atomic Energy Agency (IAEA) is watching undeclared operation of reactors to prevent illegal production and removal of 239Pu. In operating reactors, a huge numbers of anti electron neutrinos (ν) are produced. Neutrino flux is approximately proportional to the operating power of reactor in short term and long term decrease of the neutrino flux per thermal power is proportional to the amount of 239Pu produced. Thus rector ν's carry direct and real time information useful for the safeguard purposes. Since ν can not be hidden, it could be an ideal medium to monitor the reactor operation. IAEA seeks for novel technologies which enhance their ability and reactor neutrino monitoring is listed as one of such candidates. Currently neutrino physicists are performing R&D of small reactor neutrino detectors to use specifically for the safeguard use in response to the IAEA interest. In this proceedings of the neutrino2012 conference, possibilities of such reactor neutrinos application and current world-wide R&D status are described.

  4. Time-resolved record of (236)U and (239,240)Pu isotopes from a coral growing during the nuclear testing program at Enewetak Atoll (Marshall Islands).

    PubMed

    Froehlich, M B; Chan, W Y; Tims, S G; Fallon, S J; Fifield, L K

    2016-12-01

    A comprehensive series of nuclear tests were carried out by the United States at Enewetak Atoll in the Marshall Islands, especially between 1952 and 1958. A Porites Lutea coral that was growing in the Enewetak lagoon within a few km of all of the high-yield tests contains a continuous record of isotopes, which are of interest (e.g. (14)C, (236)U, (239,240)Pu) through the testing period. Prior to the present work, (14)C measurements at ∼2-month resolution had shown pronounced peaks in the Δ(14)C data that coincided with the times at which tests were conducted. Here we report measurements of (236)U and (239,240)Pu on the same coral using accelerator mass spectrometry, and again find prominent peaks in the concentrations of these isotopes that closely follow those in (14)C. Consistent with the (14)C data, the magnitudes of these peaks do not, however, correlate well with the explosive yields of the corresponding tests, indicating that smaller tests probably contributed disproportionately to the debris that fell in the lagoon. Additional information about the different tests can also be obtained from the (236)U/(239)Pu and (240)Pu/(239)Pu ratios, which are found to vary dramatically over the testing period. In particular, the first thermonuclear test, Ivy-Mike, has characteristic (236)U/(239)Pu and (240)Pu/(239)Pu signatures which are diagnostic of the first arrival of nuclear test material in various archives.

  5. National Low-Level Waste Management Program Radionuclide Report Series, Volume 17: Plutonium-239

    SciTech Connect

    J. P. Adams; M. L. Carboneau

    1999-03-01

    This report, Volume 17 of the National Low-Level Waste Management Program Radionuclide Report Series, discusses the radiological and chemical characteristics of plutonium-239 (Pu-239). This report also discusses waste types and forms in which Pu-239 can be found, waste and disposal information on Pu-239, and Pu-239 behavior in the environment and in the human body.

  6. What Are the Legal and Policy Implications of Conducting Preemption and Interdiction Against a Weapons of Mass Destruction?

    DTIC Science & Technology

    2002-01-01

    kg 17 kg 20 kg Uranium 233 Neptunium 237 Americium 241 15 kg 60 kg 100 kg Source: O’Neil 1997, 4. 38 With regard to the question of preassembly or...1996, 2). That is not specifically enriched weapons grade HEU or Pu 239, but does include Pu 239, Pu 240, Pu 241, Pu 242, Uranium 233, Neptunium - 237

  7. Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean.

    PubMed

    Lindahl, Patric; Roos, Per; Holm, Elis; Dahlgaard, Henning

    2005-01-01

    The long-lived anthropogenic radionuclides (237)Np, (239)Pu and (240)Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The (237)Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16+/-0.02 to 1.02+/-0.09 mBq kg(-1) (dry weight) and 0.65+/-0.02 to 1.69+/-0.02 mBq m(-3), respectively, depending on the location and sampling year. Most of the (237)Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The (240)Pu/(239)Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17+/-0.03. The (237)Np and (239)Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16+/-0.01 to 0.62+/-0.08 mBq m(-3) and from 0.64+/-0.05 to 4.27+/-0.08 mBq m(-3), respectively, and the (237)Np/(239)Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.

  8. Applying a low energy HPGe detector gamma ray spectrometric technique for the evaluation of Pu/Am ratio in biological samples.

    PubMed

    Singh, I S; Mishra, Lokpati; Yadav, J R; Nadar, M Y; Rao, D D; Pradeepkumar, K S

    2015-10-01

    The estimation of Pu/(241)Am ratio in the biological samples is an important input for the assessment of internal dose received by the workers. The radiochemical separation of Pu isotopes and (241)Am in a sample followed by alpha spectrometry is a widely used technique for the determination of Pu/(241)Am ratio. However, this method is time consuming and many times quick estimation is required. In this work, Pu/(241)Am ratio in the biological sample was estimated with HPGe detector based measurements using gamma/X-rays emitted by these radionuclides. These results were compared with those obtained from alpha spectroscopy of sample after radiochemical analysis and found to be in good agreement.

  9. Ultra-trace plutonium determination in small volume seawater by sector field inductively coupled plasma mass spectrometry with application to Fukushima seawater samples.

    PubMed

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Aono, Tatsuo; Tagami, Keiko; Uchida, Shigeo; Tazoe, Hirofumi; Yamada, Masatoshi

    2014-04-11

    Long-term monitoring of Pu isotopes in seawater is required for assessing Pu contamination in the marine environment from the Fukushima Dai-ichi Nuclear Power Plant accident. In this study, we established an accurate and precise analytical method based on anion-exchange chromatography and SF-ICP-MS. This method was able to determine Pu isotopes in seawater samples with small volumes (20-60L). The U decontamination factor was 3×10(7)-1×10(8), which provided sufficient removal of interfering U from the seawater samples. The estimated limits of detection for (239)Pu and (240)Pu were 0.11fgmL(-1) and 0.08fgmL(-1), respectively, which corresponded to 0.01mBqm(-3) for (239)Pu and 0.03mBqm(-3) for (240)Pu when a 20L volume of seawater was measured. We achieved good precision (2.9%) and accuracy (0.8%) for measurement of the (240)Pu/(239)Pu atom ratio in the standard Pu solution with a (239)Pu concentration of 11fgmL(-1) and (240)Pu concentration of 2.7fgmL(-1). Seawater reference materials were used for the method validation and both the (239+240)Pu activities and (240)Pu/(239)Pu atom ratios agreed well with the expected values. Surface and bottom seawater samples collected off Fukushima in the western North Pacific since March 2011 were analyzed. Our results suggested that there was no significant variation of the Pu distribution in seawater in the investigated areas compared to the distribution before the accident.

  10. Twenty-four years of follow-up for a Hanford plutonium wound case.

    PubMed

    Carbaugh, Eugene H; Lynch, Timothy P; Antonio, Cheryl L; Medina-Del Valle, Fernando

    2010-10-01

    A 1985 plutonium puncture wound resulted in the initial deposition of 48 kBq of transuranic alpha activity, primarily 239+240Pu and 241Am, in a worker's right index finger. Surgical excisions in the week following reduced the long-term residual wound activity to 5.4 kBq, and 164 DTPA chelation therapy administrations over 17 mo resulted in urinary excretion of about 7 kBq. The case was published in 1988, but now 24 y of follow-up data are available. Annual bioassays have included in-vivo measurements of 241Am in the wound, skeleton, liver, lung, and axillary lymph nodes, and urinalyses for plutonium and 241Am. These measurements have shown relatively stable levels of 241Am at the wound site, with gradually increasing amounts of 241Am detected in the skeleton. Liver measurements have shown erratic detection of 241Am, and the lung measurements indicate Am but as interference from activity in the axillary lymph nodes and skeleton rather than activity in the lung. Urine excretion of Pu since termination of chelation therapy has typically ranged from 10 to 20 mBq d, with Am excretion about 10% of that for 239+240Pu. Annual routine medical exams have not identified any adverse health effects associated with the intake.

  11. Effect of americium-241 on luminous bacteria. Role of peroxides.

    PubMed

    Alexandrova, M; Rozhko, T; Vydryakova, G; Kudryasheva, N

    2011-04-01

    The effect of americium-241 ((241)Am), an alpha-emitting radionuclide of high specific activity, on luminous bacteria Photobacterium phosphoreum was studied. Traces of (241)Am in nutrient media (0.16-6.67 kBq/L) suppressed the growth of bacteria, but enhanced luminescence intensity and quantum yield at room temperature. Lower temperature (4 °C) increased the time of bacterial luminescence and revealed a stage of bioluminescence inhibition after 150 h of bioluminescence registration start. The role of conditions of exposure the bacterial cells to the (241)Am is discussed. The effect of (241)Am on luminous bacteria was attributed to peroxide compounds generated in water solutions as secondary products of radioactive decay. Increase of peroxide concentration in (241)Am solutions was demonstrated; and the similarity of (241)Am and hydrogen peroxide effects on bacterial luminescence was revealed. The study provides a scientific basis for elaboration of bioluminescence-based assay to monitor radiotoxicity of alpha-emitting radionuclides in aquatic solutions.

  12. Determination of plutonium and other transuranic elements by inductively coupled plasma mass spectrometry: A historical perspective and new frontiers in the environmental sciences

    NASA Astrophysics Data System (ADS)

    Ketterer, Michael E.; Szechenyi, Scott C.

    2008-07-01

    Inductively coupled plasma mass spectrometry (ICPMS), particularly with sector field mass analyzers (SF-ICPMS), has emerged in the past several years as an excellent analytical technique for rapid, highly sensitive determination of transuranic elements (TRU) in environmental samples. SF-ICPMS has advantages of simplicity of sample preparation, high sample throughput, widespread availability in laboratories worldwide, and relatively straightforward operation when compared to other competing mass spectrometric techniques. Arguably, SF-ICPMS is the preferred technique for routine, high-throughput determination of 237Np and the Pu isotopes, excepting 238Pu, at fg-pg levels in environmental samples. Many research groups have now demonstrated the SF-ICPMS determination of 239 + 240 Pu activities, 240Pu/ 239Pu and other Pu atom ratios in several different application areas. Many studies have examined the relative contribution of global fallout vs. local/regional Pu sources in the environment through measurement of 240Pu/ 239Pu and, in some cases, 241Pu/ 239Pu and 242Pu/ 239Pu. "Stratospheric fallout", which was deposited from thermonuclear tests, conducted largely during the 1952-1964 time period, is characterized by a well-defined 240Pu/ 239Pu of ~ 0.18, while most other sources have different ratios. Examples of local/regional Pu sources are the Nevada Test Site, the Chernobyl plume, and accidents at Palomares, Spain and Thule, Greenland. The determination of Pu activities and atom ratios has stimulated much interest in the use of Pu as a marine tracer; several studies have shown that Pu is transported over long distances by ocean currents. 240Pu/ 239Pu ratios > 0.20 in sediments and seawater of the North Pacific are ascribed to ocean current transport of fallout from the Pacific Proving Ground. In nuclear forensics, much effort is focused on detection and fingerprinting of small amounts of TRU in environmental samples consisting of bulk material or individual isolated

  13. Effects of americium-241 and humic substances on Photobacterium phosphoreum: Bioluminescence and diffuse reflectance FTIR spectroscopic studies

    NASA Astrophysics Data System (ADS)

    Kamnev, Alexander A.; Tugarova, Anna V.; Selivanova, Maria A.; Tarantilis, Petros A.; Polissiou, Moschos G.; Kudryasheva, Nadezhda S.

    The integral bioluminescence (BL) intensity of live Photobacterium phosphoreum cells (strain 1883 IBSO), sampled at the stationary growth stage (20 h), was monitored for further 300 h in the absence (control) and presence of 241Am (an α-emitting radionuclide of a high specific activity) in the growth medium. The activity concentration of 241Am was 2 kBq l-1; [241Am] = 6.5 × 10-11 M. Parallel experiments were also performed with water-soluble humic substances (HS, 2.5 mg l-1; containing over 70% potassium humate) added to the culture medium as a possible detoxifying agent. The BL spectra of all the bacterial samples were very similar (λmax = 481 ± 3 nm; FWHM = 83 ± 3 nm) showing that 241Am (also with HS) influenced the bacterial BL system at stages prior to the formation of electronically excited states. The HS added per se virtually did not influence the integral BL intensity. In the presence of 241Am, BL was initially activated but inhibited after 180 h, while the system 241Am + HS showed an effective activation of BL up to 300 h which slowly decreased with time. Diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy, applied to dry cell biomass sampled at the stationary growth phase, was used to control possible metabolic responses of the bacteria to the α-radioactivity stress (observed earlier for other bacteria under other stresses). The DRIFT spectra were all very similar showing a low content of intracellular poly-3-hydroxybutyrate (at the level of a few percent of dry biomass) and no or negligible spectroscopic changes in the presence of 241Am and/or HS. This assumes the α-radioactivity effect to be transmitted by live cells mainly to the bacterial BL enzyme system, with negligible structural or compositional changes in cellular macrocomponents at the stationary growth phase.

  14. Effects of Americium-241 and humic substances on Photobacterium phosphoreum: bioluminescence and diffuse reflectance FTIR spectroscopic studies.

    PubMed

    Kamnev, Alexander A; Tugarova, Anna V; Selivanova, Maria A; Tarantilis, Petros A; Polissiou, Moschos G; Kudryasheva, Nadezhda S

    2013-01-01

    The integral bioluminescence (BL) intensity of live Photobacterium phosphoreum cells (strain 1883 IBSO), sampled at the stationary growth stage (20 h), was monitored for further 300 h in the absence (control) and presence of (241)Am (an α-emitting radionuclide of a high specific activity) in the growth medium. The activity concentration of (241)Am was 2 kBq l(-1); [(241)Am]=6.5×10(-11) M. Parallel experiments were also performed with water-soluble humic substances (HS, 2.5 mg l(-1); containing over 70% potassium humate) added to the culture medium as a possible detoxifying agent. The BL spectra of all the bacterial samples were very similar (λ(max)=481±3 nm; FWHM=83±3 nm) showing that (241)Am (also with HS) influenced the bacterial BL system at stages prior to the formation of electronically excited states. The HS added per se virtually did not influence the integral BL intensity. In the presence of (241)Am, BL was initially activated but inhibited after 180 h, while the system (241)Am+HS showed an effective activation of BL up to 300 h which slowly decreased with time. Diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy, applied to dry cell biomass sampled at the stationary growth phase, was used to control possible metabolic responses of the bacteria to the α-radioactivity stress (observed earlier for other bacteria under other stresses). The DRIFT spectra were all very similar showing a low content of intracellular poly-3-hydroxybutyrate (at the level of a few percent of dry biomass) and no or negligible spectroscopic changes in the presence of (241)Am and/or HS. This assumes the α-radioactivity effect to be transmitted by live cells mainly to the bacterial BL enzyme system, with negligible structural or compositional changes in cellular macrocomponents at the stationary growth phase.

  15. Effect of low-level alpha-radiation on bioluminescent assay systems of various complexity.

    PubMed

    Rozhko, Tatiana V; Kudryasheva, Nadezhda S; Kuznetsov, Alexander M; Vydryakova, Galina A; Bondareva, Lydia G; Bolsunovsky, Alexander Ya

    2007-01-01

    This study addresses the effects of low-level alpha-radiation on bioluminescent assay systems of different levels of organization: in vivo and in vitro. Three bioluminescent assay systems are used: intact bacteria, lyophilized bacteria, and bioluminescent system of coupled enzyme reactions. Solutions of 241Am(NO3)3 are used as a source of alpha-radiation. It has been shown that activation processes predominate in all the three bioluminescent assay systems subjected to short-term exposure (20-55 h) and inhibition processes in the systems subjected to longer-term exposure to radiation. It has been found that these effects are caused by the radiation component of 241Am3+ impact. The intensity of the 241Am3+ effect on the bioluminescent assay systems has been shown to depend on the 241Am3+ concentration, level of organization and integrity of the bioluminescent assay system. The bioluminescent assay systems in vivo have been found to be highly sensitive to 241Am3+ (up to 10(-17) M).

  16. Nuclear waste forms for actinides

    PubMed Central

    Ewing, Rodney C.

    1999-01-01

    The disposition of actinides, most recently 239Pu from dismantled nuclear weapons, requires effective containment of waste generated by the nuclear fuel cycle. Because actinides (e.g., 239Pu and 237Np) are long-lived, they have a major impact on risk assessments of geologic repositories. Thus, demonstrable, long-term chemical and mechanical durability are essential properties of waste forms for the immobilization of actinides. Mineralogic and geologic studies provide excellent candidate phases for immobilization and a unique database that cannot be duplicated by a purely materials science approach. The “mineralogic approach” is illustrated by a discussion of zircon as a phase for the immobilization of excess weapons plutonium. PMID:10097054

  17. Neutron-induced fission: properties of prompt neutron and γ rays as a function of incident energy

    NASA Astrophysics Data System (ADS)

    Stetcu, I.; Talou, P.; Kawano, T.

    2016-06-01

    We have applied the Hauser-Feshbach statistical theory, in a Monte-Carlo implementation, to the de-excitation of fission fragments, obtaining a reasonable description of the characteristics of neutrons and gamma rays emitted before beta decays toward stability. Originally implemented for the spontaneous fission of 252Cf and the neutroninduced fission of 235U and 239Pu at thermal neutron energy, in this contribution we discuss the extension of the formalism to incident neutron energies up to 20 MeV. For the emission of pre-fission neutrons, at incident energies beyond second-chance fission, we take into account both the pre-equilibrium and statistical pre-fission components. Phenomenological parameterizations of mass, charge and TKE yields are used to obtain the initial conditions for the fission fragments that subsequently decay via neutron and emissions. We illustrate this approach for 239Pu(n,f).

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

    SciTech Connect

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

    2008-01-01

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

  19. Off-Site Radiation Exposure Review Project: Phase 2 soils program

    SciTech Connect

    McArthur, R.D.; Miller, F.L. Jr.

    1989-12-01

    To help estimate population doses of radiation from fallout originating at the Nevada Test Site, soil samples were collected throughout the western United States. Each sample was prepared by drying and ball-milling, then analyzed by gamma-spectrometry to determine the amount of {sup 137}Cs it contained. Most samples were also analyzed by chemical separation and alpha-spectrometry to determine {sup 239 + 240}Pu and by isotope mass spectroscopy to determine the ratios of {sup 240}Pu to {sup 239}Pu and {sup 241}Pu to {sup 239}Pu. The total inventories of cesium and plutonium at 171 sites were computed from the results. This report describes the sample collection, processing, and analysis, presents the analytical results, and assesses the quality of the data. 10 refs., 9 figs., 12 tabs.

  20. Comparison of attenuation correction methods for TGS and SGS: Do we really need selenium-75?

    SciTech Connect

    Estep, R.J.; Prettyman, T.H.; Sheppard, G.A.

    1996-09-01

    We compared attenuation-coefficient mapping techniques for use in tomographic gamma scanner (TGS) image reconstructions to determine whether there is a significant improvement when using fully coupled methods. For the constrained least-squares image reconstruction method tested here, we found no significant improvement. We also compared the effectiveness of different transmission source combinations for 129- and 414-keV {sup 239}Pu TGS assays. We concluded that the best source combination for TGS assays of {sup 239}Pu and other isotopes is a mixture of {sup 133}Ba, {sup 54}Mn, and {sup 60}Co. Three other source combinations were found to be at least as effective as {sup 75}Se.

  1. The Geochemical Behaviour of Tc, Np, and Pu in Spent Nuclear Fuel in an Oxidizing Environment

    SciTech Connect

    Buck, Edgar C.; Hanson, Brady D.; McNamara, Bruce K.; R. Giere and P. Stille

    2004-10-01

    Studies at the Nopal and Shinkolowbwe uranium deposits show that the primary uraninite (UO2) altered to a suite of secondary uranyl minerals similar to those observed in corrosion tests with uranium oxide . Although the Nopal I deposit tells us something about the possible fate of uranium, it tells us little about the likely fate of the important long-lived radionuclides; iodine (129I), cesium (135Cs), technetium (99Tc), neptunium (237Np), and plutonium (239Pu). Most performance assessment (PA) models, assume conservatively, that as the UO2 matrix corrodes, the key radionuclides (129I, 99Tc, 237Np, and 239Pu) will be released congruently. In so doing, these PA models force increased reliance on human engineered barriers.

  2. In-cell reaction rate distributions and cell-average reaction rates in fast critical assemblies

    SciTech Connect

    Brumbach, S.B.; Gasidlo, J.M.

    1985-08-01

    Measurements are described for determining average values of fission rates in /sup 235/U, /sup 238/U and /sup 239/Pu and capture rates in /sup 238/U for heterogeneous cells used to construct fast critical assemblies. The measurements are based on irradiations of foils of /sup 238/U, /sup 235/U and /sup 239/Pu with counting of fission and capture products using gamma-ray spectroscopy. Both plate and pin cells are considered. Procedures are described for inferring cell-average reaction rate values from a single foil location based on a cell using a quantity called a cell factor. Cell factors are determined from special measurements in which several foils are irradiated within a cell. Comparisons are presented between cell factors determined by measurements and by Monte Carlo calculations which lend credibility to the measurement procedures.

  3. Advanced modeling of prompt fission neutrons

    SciTech Connect

    Talou, Patrick

    2009-01-01

    Theoretical and numerical studies of prompt fission neutrons are presented. The main results of the Los Alamos model often used in nuclear data evaluation work are reviewed briefly, and a preliminary assessment of uncertainties associated with the evaluated prompt fission neutron spectrum for n (0.5 MeV)+{sup 239}Pu is discussed. Advanced modeling of prompt fission neutrons is done by Monte Carlo simulations of the evaporation process of the excited primary fission fragments. The successive emissions of neutrons are followed in the statistical formalism framework, and detailed information, beyond average quantities, can be inferred. This approach is applied to the following reactions: {sup 252}Cf (sf), n{sub th} + {sup 239}Pu, n (0.5 MeV)+{sup 235}U, and {sup 236}Pu (sf). A discussion on the merits and present limitations of this approach concludes this presentation.

  4. Lead Slowing Down Spectrometry Analysis of Data from Measurements on Nuclear Fuel

    SciTech Connect

    Warren, Glen A.; Anderson, Kevin K.; Kulisek, Jonathan A.; Danon, Yaron; Weltz, Adam; Gavron, Victor A.; Harris, Jason; Stewart, Trevor N.

    2015-01-12

    Improved non-destructive assay of isotopic masses in used nuclear fuel would be valuable for nuclear safeguards operations associated with the transport, storage and reprocessing of used nuclear fuel. Our collaboration is examining the feasibility of using lead slowing down spectrometry techniques to assay the isotopic fissile masses in used nuclear fuel assemblies. We present the application of our analysis algorithms on measurements conducted with a lead spectrometer. The measurements involved a single fresh fuel pin and discrete 239Pu and 235U samples. We are able to describe the isotopic fissile masses with root mean square errors over seven different configurations to 6.35% for 239Pu and 2.7% for 235U over seven different configurations. Funding Source(s):

  5. 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.

  6. Consideration of Nuclear Criticality When Directly Disposing Highly Enriched Spent Nuclear Fuel in Unsaturated Tuff - II: Geochemical Constraints

    SciTech Connect

    Rechard, Rob P.; Sanchez, Lawrence C.; Trellue, Holly R.

    2003-11-15

    This article presents several reasonable cases in which four mechanisms - dissolution, physical mixing, adsorption, and precipitation (either chemical change or evaporation) - might concentrate fissile material in and around a disposal container for radioactive waste at the proposed repository at Yucca Mountain, Nevada. The possible masses, concentrations, and volume are then compared to criticality limits. The cases examined evaluate the geologic barrier role in preventing criticality since engineered options for preventing criticality (e.g., boron or gadolinium neutron absorber in the disposal container) are not considered. The solid concentrations able to form in the natural environment are insufficient for criticality to occur because (a) solutions of {sup 235}U and {sup 239}Pu are clearly not critical; (b) physical mixing of fissile material with the entire potential iron oxide (as goethite - FeOOH) in a waste package is not critical; (c) the adsorption of {sup 239}Pu on consolidated iron oxide in a waste package is not critical; (d) the adsorption of {sup 235}U on consolidated iron oxide in a waste package is not critical when accounting for reduced adsorption because of carbonates at high pH; (e) the filtration of iron oxide colloids, containing fissile material, by the thin invert material is not critical; (f) insufficient retention through precipitation of {sup 235}U or {sup 239}Pu occurs in the invert; (g) adsorption of {sup 235}U and {sup 239}Pu on devitrified or clinoptolite-rich tuff below the repository is not critical; (h) the average precipitation/adsorption of {sup 235}U as uranyl silicates in the tuff is not critical by analogy with calcite deposition in lithophysae at Yucca Mountain; and (i) precipitation/adsorption (caused by cyclic drying) as uranyl silicates on fracture surfaces of the tuff is not critical by analogy with the oxidation of UO{sub 2}, migration of U{sup VI}, and precipitation in fractures at the Nopal I ore deposit in Mexico.

  7. Detection of thermal-induced prompt fission neutrons of highly-enriched uranium: A position sensitive technique

    NASA Astrophysics Data System (ADS)

    Tartaglione, A.; Di Lorenzo, F.; Mayer, R. E.

    2009-07-01

    Cargo interrogation in search for special nuclear materials like highly-enriched uranium or 239Pu is a first priority issue of international borders security. In this work we present a thermal-pulsed neutron-based approach to a technique which combines the time-of-flight method and demonstrates a capability to detect small quantities of highly-enriched uranium shielded with high or low Z materials providing, in addition, a manner to know the approximate position of the searched material.

  8. Fission Product Gamma-Ray Line Pairs Sensitive to Fissile Material and Neutron Energy

    SciTech Connect

    Marrs, R E; Norman, E B; Burke, J T; Macri, R A; Shugart, H A; Browne, E; Smith, A R

    2007-11-15

    The beta-delayed gamma-ray spectra from the fission of {sup 235}U, {sup 238}U, and {sup 239}Pu by thermal and near-14-MeV neutrons have been measured for delay times ranging from 1 minute to 14 hours. Spectra at all delay times contain sets of prominent gamma-ray lines with intensity ratios that identify the fissile material and distinguish between fission induced by low-energy or high-energy neutrons.

  9. Anthropogenic plutonium in the North Jiangsu tidal flats of the Yellow Sea in China.

    PubMed

    Liu, Zhiyong; Zheng, Jian; Pan, Shaoming; Gao, Jianhua

    2013-08-01

    The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were analyzed using a double-focusing SF-ICP-MS for sediment core samples obtained in 2007-2008 from the North Jiangsu tidal flats in the Yellow Sea in China. Particular attention was focused on the (240)Pu/(239)Pu atom ratios in the sediment to identify the origins of Pu isotopes. The profiles of (239+240)Pu activities in the sediment cores are similar to those of the (137)Cs activities. The (240)Pu/(239)Pu atom ratios in the tidal flats showed typical global fallout values, indicating that this area did not receive the possible early direct close-in fallout or oceanic current transported Pu from the Pacific Proving Grounds (PPG). If any, the contribution of the PPG source Pu to the total Pu inventory is negligible. This is different from the sediments in the Yangtze River estuary in the East China Sea, where the PPG source Pu contributed ca. 45 % to the total inventory. In addition, the observation of the global fallout origin Pu in the North Jiangsu tidal flats indicated that the nuclear power plant in the region was not causing any alteration/contamination to the (240)Pu/(239)Pu atom ratios. The (239+240)Pu and (137)Cs activities/inventories in the sediment cores showed correlation to the mean clay sediment compositions (fine particles) in the tidal flats. Therefore, mud deposits are served as sinks for the anthropogenic radionuclides in the tidal flats and the Yellow Sea. Integrated with the previously reported spatial distributions of (239+240)Pu and (137)Cs activities in the surface sediments of the Yellow Sea, the mechanism of Pu transport with the ocean currents and the scavenging characteristics in the Yellow Sea were discussed.

  10. The Microscopic Theory of Fission

    SciTech Connect

    Younes, W; Gogny, D

    2009-06-09

    Fission-fragment properties have been calculated for thermal neutron-induced fission on a {sup 239}Pu target, using constrained Hartree-Fock-Bogoliubov calculations with a finite-range effective interaction. A quantitative criterion based on the interaction energy between the nascent fragments is introduced to define the scission configurations. The validity of this criterion is benchmarked against experimental measurements of the kinetic energies and of multiplicities of neutrons emitted by the fragments.

  11. Implementation of Energy-Dependent Q Values for Fission

    SciTech Connect

    Beck, B; Brown, D A; Daffin, F; Hedstrom, J; Vogt, R

    2007-08-08

    We discuss how the fission Q values for {sup 235}U, {sup 238}U and {sup 239}Pu depend on the energy of the incident neutron. We then describe how these values have been implemented in mcfgen etc. This paper describes the calculation of energy-dependent fission Q values by Madland [1] and explains how it has been implemented in the ENDL database for use in the LLNL codes.

  12. Experiments on the synthesis of superheavy nuclei 284Fl and 285Fl in the Pu,240239+48Ca reactions

    NASA Astrophysics Data System (ADS)

    Utyonkov, V. K.; Brewer, N. T.; Oganessian, Yu. Ts.; Rykaczewski, K. P.; Abdullin, F. Sh.; Dmitriev, S. N.; Grzywacz, R. K.; Itkis, M. G.; Miernik, K.; Polyakov, A. N.; Roberto, J. B.; Sagaidak, R. N.; Shirokovsky, I. V.; Shumeiko, M. V.; Tsyganov, Yu. S.; Voinov, A. A.; Subbotin, V. G.; Sukhov, A. M.; Sabel'nikov, A. V.; Vostokin, G. K.; Hamilton, J. H.; Stoyer, M. A.; Strauss, S. Y.

    2015-09-01

    Irradiations of 239Pu and 240Pu targets with 48Ca beams aimed at the synthesis of Z =114 flerovium isotopes were performed at the Dubna Gas Filled Recoil Separator. A new spontaneously fissioning (SF) isotope 284Fl was produced for the first time in the 240Pu+48Ca (250 MeV) and 239Pu+48Ca (245 MeV) reactions. The cross section of the 239Pu(48Ca,3 n )284Fl reaction channel was about 20 times lower than predicted by theoretical models and about 50 times lower than the maximum fusion-evaporation cross section for the 3 n and 4 n channels measured in the 244Pu+48Ca reaction. In the 240Pu+48Ca experiment, performed at 245 MeV in order to maximize the 3 n -evaporation channel, three decay chains of 285Fl were detected. The α -decay energy of 285Fl was measured for the first time and decay properties of its descendants 281Cn, 277Ds, 273Hs, 269Sg, and 265Rf were determined with higher accuracy. The assignment of SF events observed during the irradiation of the 240Pu target with a 250 MeV 48Ca beam to 284Fl decay is presented and discussed. The cross sections at both 48Ca energies are similar and exceed that observed in the reaction with the lighter isotope 239Pu by a factor of 10. The decay properties of the synthesized nuclei and their production cross sections indicate a rapid decrease of stability of superheavy nuclei as the neutron number decreases from the predicted magic neutron number N =184 .

  13. Alpha spectrometry — A tool for nuclear data measurements

    NASA Astrophysics Data System (ADS)

    Wiltshire, R. A. P.

    1984-06-01

    Alpha spectrometry is a precise technique which can be applied to the measurement of data such as half-lives and the production cross-sections of higher actinides. The application of this technique to the measurement of 239Pu and 242Cm half-lives, to the production cross-sections for curium isotopes in fast reactor spectra and to the analysis of irradiated fuel for alpha emitting higher actinide nuclides are discussed.

  14. OPERATIONS TOGGLE, ARBOR and BEDROCK Events: DIAMOND SCULLS, DIDO QUEEN, HUSKY ACE, MING BLADE, HYBLA FAIR and DINING CAR, 20 July 1972 - 5 April 1975

    DTIC Science & Technology

    1987-11-30

    58m co 58 Co 60 iOpp8r ( 29 ) . . . . . . . . . . . . . Cu 64 Curium (96, . . . . . . . . . . . . . Cm 242 Cm 243 Cm 244 Cm 245 Cm 246...was conducted in the LOS pipe. 242 On 12 April (D+7), miners continued to prepare the tunnel for experiment recovery. Work also continued in...Pt 191 Pt 193m Pt 197m Pt 197 Plutonium (94) . . . . . . . . . . Pu 236 Pu 239 Pu 240 Pu 241 Pu 242 Polonium (84

  15. Extended optical model for fission

    DOE PAGES

    Sin, M.; Capote, R.; Herman, M. W.; ...

    2016-03-07

    A comprehensive formalism to calculate fission cross sections based on the extension of the optical model for fission is presented. It can be used for description of nuclear reactions on actinides featuring multi-humped fission barriers with partial absorption in the wells and direct transmission through discrete and continuum fission channels. The formalism describes the gross fluctuations observed in the fission probability due to vibrational resonances, and can be easily implemented in existing statistical reaction model codes. The extended optical model for fission is applied for neutron induced fission cross-section calculations on 234,235,238U and 239Pu targets. A triple-humped fission barrier ismore » used for 234,235U(n,f), while a double-humped fission barrier is used for 238U(n,f) and 239Pu(n,f) reactions as predicted by theoretical barrier calculations. The impact of partial damping of class-II/III states, and of direct transmission through discrete and continuum fission channels, is shown to be critical for a proper description of the measured fission cross sections for 234,235,238U(n,f) reactions. The 239Pu(n,f) reaction can be calculated in the complete damping approximation. Calculated cross sections for 235,238U(n,f) and 239Pu(n,f) reactions agree within 3% with the corresponding cross sections derived within the Neutron Standards least-squares fit of available experimental data. Lastly, the extended optical model for fission can be used for both theoretical fission studies and nuclear data evaluation.« less

  16. Improving neutronics simulations and uncertainties via a selection of nuclear data

    NASA Astrophysics Data System (ADS)

    Rochman, D.; Koning, A. J.; van der Marck, S. C.

    2015-12-01

    This work presents a novel approach to improve neutronics simulations, as in the case of criticality calculations, by simply combining the results of a limited set of random evaluations. Another outcome of this work is to lower uncertainties due to nuclear data by integrating the information from criticality benchmarks into the neutronics simulations scheme. Examples are presented for the 239Pu nuclear data and calculations of criticality benchmarks and a MOX fuel pincell.

  17. Managing the Nuclear Fuel Cycle: Policy Implications of Expanding Global Access to Nuclear Power

    DTIC Science & Technology

    2008-01-20

    reprocessing is currently conducted in France, Britain, and Russia. The 239Pu they produce is blended with uranium to make mixed- oxide ( MOX ) fuel, in which...Association, Mixed Oxide Fuel ( MOX ), November 2006, at [http://www.world-nuclear.org/info/inf29.html]. 53 World Nuclear Association, Uranium Markets, March...older plants to reprocess gas-cooled reactor fuel, and India has a 275-ton plant.51 About 200 metric tons of MOX fuel is used annually, about 2% of

  18. Development of a multimedia radionuclide exposure model for low-level waste management

    SciTech Connect

    Onishi, Y.; Whelan, G.; Skaggs, R.L.

    1982-03-01

    A method is being developed for assessing exposures of the air, water, and plants to low-level waste (LLW) as a part of an overall development effort of a LLW site evaluation methodology. The assessment methodology will predict LLW exposure levels in the environment by simulating dominant mechanisms of LLW migration and fate. The methodology consists of a series of physics-based models with proven histories of success; the models interact with each other to simulate LLW transport in the ecosystem. A scaled-down version of the methodology was developed first by combining the terrestrial ecological model, BIOTRAN; the overland transport model, ARM; the instream hydrodynamic model, DKWAV; and the instream sediment-contaminant transport model, TODAM (a one-dimensional version of SERATRA). The methodology was used to simulate the migration of /sup 239/Pu from a shallow-land disposal site (known as Area C) located near the head of South Mortandad Canyon on the LANL site in New Mexico. The scenario assumed that /sup 239/Pu would be deposited on the land surface through the natural processes of plant growth, LLW uptake, dryfall, and litter decomposition. Runoff events would then transport /sup 239/Pu to and in the canyon. The model provided sets of simulated LLW levels in soil, water and terrestrial plants in the region surrounding the site under a specified land-use and a waste management option. Over a 100-yr simulation period, only an extremely small quantity (6 x 10/sup -9/ times the original concentration) of buried /sup 239/Pu was taken up by plants and deposited on the land surface. Only a small fraction (approximately 1%) of that contamination was further removed by soil erosion from the site and carried to the canyon, where it remained. Hence, the study reveals that the environment around Area C has integrity high enough to curtail LLW migration under recreational land use.

  19. Extended optical model for fission

    NASA Astrophysics Data System (ADS)

    Sin, M.; Capote, R.; Herman, M. W.; Trkov, A.

    2016-03-01

    A comprehensive formalism to calculate fission cross sections based on the extension of the optical model for fission is presented. It can be used for description of nuclear reactions on actinides featuring multi-humped fission barriers with partial absorption in the wells and direct transmission through discrete and continuum fission channels. The formalism describes the gross fluctuations observed in the fission probability due to vibrational resonances, and can be easily implemented in existing statistical reaction model codes. The extended optical model for fission is applied for neutron induced fission cross-section calculations on 234,235,238U and 239Pu targets. A triple-humped fission barrier is used for U,235234(n ,f ) , while a double-humped fission barrier is used for 238U(n ,f ) and 239Pu(n ,f ) reactions as predicted by theoretical barrier calculations. The impact of partial damping of class-II/III states, and of direct transmission through discrete and continuum fission channels, is shown to be critical for a proper description of the measured fission cross sections for 234,235,238U(n ,f ) reactions. The 239Pu(n ,f ) reaction can be calculated in the complete damping approximation. Calculated cross sections for U,238235(n ,f ) and 239Pu(n ,f ) reactions agree within 3% with the corresponding cross sections derived within the Neutron Standards least-squares fit of available experimental data. The extended optical model for fission can be used for both theoretical fission studies and nuclear data evaluation.

  20. 238Pu: accumulation, tissue distribution, and excretion in Mayak workers after exposure to plutonium aerosols.

    PubMed

    Suslova, Klara G; Sokolova, Alexandra B; Khokhryakov, Viktor V; Miller, Scott C

    2012-03-01

    The alpha spectrometry measurements of specific activity of 238Pu and 239Pu in urine from bioassay examinations of 1,013 workers employed at the radiochemical and plutonium production facilities of the Mayak Production Association and in autopsy specimens of lung, liver, and skeleton from 85 former nuclear workers who died between 1974-2009, are summarized.The accumulation fraction of 238Pu in the body and excreta has not changed with time in workers involved in production of weapons-grade plutonium production (e.g., the plutonium production facility and the former radiochemical facility). The accumulation fraction of 238Pu in individuals exposed to plutonium isotopes at the newer Spent Nuclear Fuel Reprocessing Plant ranged from 0.13% up to 27.5% based on the autopsy data. No statistically significant differences between 238Pu and 239Pu in distribution by the main organs of plutonium deposition were found in the Mayak workers. Based on the bioassay data,the fraction of 238Pu activity in urine is on average 38-69% of the total activity of 238Pu and 239Pu, which correlates with the isotopic composition in workplace air sampled at the Spent Nuclear Fuel Reprocessing Plant. In view of the higher specific activity of 238Pu, the contribution of 238Pu to the total internal dose, particularly in the skeleton and liver, might be expected to continue to increase, and continued surveillance is recommended.

  1. Release of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant accident to the marine environment was negligible.

    PubMed

    Bu, Wenting; Fukuda, Miho; Zheng, Jian; Aono, Tatsuo; Ishimaru, Takashi; Kanda, Jota; Yang, Guosheng; Tagami, Keiko; Uchida, Shigeo; Guo, Qiuju; Yamada, Masatoshi

    2014-08-19

    Atmospheric deposition of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has been observed in the terrestrial environment around the FDNPP site; however, their deposition in the marine environment has not been studied. The possible contamination of Pu in the marine environment has attracted great scientific and public concern. To fully understand this possible contamination of Pu isotopes from the FDNPP accident to the marine environment, we collected marine sediment core samples within the 30 km zone around the FDNPP site in the western North Pacific about two years after the accident. Pu isotopes ((239)Pu, (240)Pu, and (241)Pu) and radiocesium isotopes ((134)Cs and (137)Cs) in the samples were determined. The high activities of radiocesium and the (134)Cs/(137)Cs activity ratios with values around 1 (decay corrected to 15 March 2011) suggested that these samples were contaminated by the FDNPP accident-released radionuclides. However, the activities of (239+240)Pu and (241)Pu were low compared with the background level before the FDNPP accident. The Pu atom ratios ((240)Pu/(239)Pu and (241)Pu/(239)Pu) suggested that global fallout and the pacific proving ground (PPG) close-in fallout are the main sources for Pu contamination in the marine sediments. As Pu isotopes are particle-reactive and they can be easily incorporated with the marine sediments, we concluded that the release of Pu isotopes from the FDNPP accident to the marine environment was negligible.

  2. Optical detection of special nuclear materials: an alternative approach for standoff and remote sensing

    NASA Astrophysics Data System (ADS)

    Johnson, J. Bruce; Reeve, S. W.; Burns, W. A.; Allen, Susan D.

    2010-04-01

    Termed Special Nuclear Material (SNM) by the Atomic Energy Act of 1954, fissile materials, such as 235U and 239Pu, are the primary components used to construct modern nuclear weapons. Detecting the clandestine presence of SNM represents an important capability for Homeland Security. An ideal SNM sensor must be able to detect fissile materials present at ppb levels, be able to distinguish between the source of the detected fissile material, i.e., 235U, 239Pu, 233U or other fission source, and be able to perform the discrimination in near real time. A sensor with such capabilities would provide not only rapid identification of a threat but, ultimately, information on the potential source of the threat. For example, current detection schemes for monitoring clandestine nuclear testing and nuclear fuel reprocessing to provide weapons grade fissile material rely largely on passive air sampling combined with a subsequent instrumental analysis or some type of wet chemical analysis of the collected material. It would be highly useful to have a noncontact method of measuring isotopes capable of providing forensic information rapidly at ppb levels of detection. Here we compare the use of Kr, Xe and I as "canary" species for distinguishing between 235U and 239Pu fission sources by spectroscopic methods.

  3. Non-destructive Assay Measurements Using the RPI Lead Slowing Down Spectrometer

    SciTech Connect

    Becker, Bjorn; Weltz, Adam; Kulisek, Jonathan A.; Thompson, J. T.; Thompson, N.; Danon, Yaron

    2013-10-01

    The use of a Lead Slowing-Down Spectrometer (LSDS) is consid- ered as a possible option for non-destructive assay of fissile material of used nuclear fuel. The primary objective is to quantify the 239Pu and 235U fissile content via a direct measurement, distinguishing them through their characteristic fission spectra in the LSDS. In this pa- per, we present several assay measurements performed at the Rensse- laer Polytechnic Institute (RPI) to demonstrate the feasibility of such a method and to provide benchmark experiments for Monte Carlo cal- culations of the assay system. A fresh UOX fuel rod from the RPI Criticality Research Facility, a 239PuBe source and several highly en- riched 235U discs were assayed in the LSDS. The characteristic fission spectra were measured with 238U and 232Th threshold fission cham- bers, which are only sensitive to fission neutron with energy above the threshold. Despite the constant neutron and gamma background from the PuBe source and the intense interrogation neutron flux, the LSDS system was able to measure the characteristic 235U and 239Pu responses. All measurements were compared to Monte Carlo simula- tions. It was shown that the available simulation tools and models are well suited to simulate the assay, and that it is possible to calculate the absolute count rate in all investigated cases.

  4. Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s.

    PubMed

    Yang, Guosheng; Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

    2015-04-16

    Obtaining Pu background data in the environment is essential for contamination source identification and assessment of environmental impact of Pu released from the Fukushima Daiichi nuclear power plant (FDNPP) accident. However, no baseline information on Pu isotopes in Fukushima Prefecture has been reported. Here we analyzed 80 surface soil samples collected from the central-eastern Japan during 1969-1977 for (239+240)Pu activity concentration and (240)Pu/(239)Pu atom ratio to establish the baseline before the FDNPP accident. We found that (239+240)Pu activity concentrations ranged from 0.004 -1.46 mBq g(-1), and (240)Pu/(239)Pu atom ratios varied narrowly from 0.148 to 0.229 with a mean of 0.186 ± 0.015. We also reconstructed the surface deposition density of (241)Pu using the (241)Pu/(239)Pu atom ratio in the Japanese fallout reference material. The obtained results indicated that, for the FDNPP-accident released (241)Pu, a similar radiation impact can be estimated as was seen for the global fallout deposited (241)Pu in the last decades.

  5. Differential die-away technique for determination of the fissile contents in spent fuel assembly

    SciTech Connect

    Lee, Tachoon; Menlove, Howard O; Swinhoe, Nartyn T; Tobin, Stephen J

    2010-01-01

    Monte Carlo simulations were performed for the differential die-away (DDA) technique to quantify its capability to measure the fissile contents in spent fuel assemblies of 64 different cases in terms of initial enrichment, burnup, and cooling time. The DDA count rate varies according to the contents of fissile isotopes such as {sup 235}U, {sup 239}Pu, and {sup 241}Pu contained in the spent fuel assembly. The effective {sup 239}Pu concept was introduced to quantify the total fissile mass of spent fuel by weighting the relative signal contributions of {sup 235}U and {sup 241}Pu compared to that of {sup 239}Pu. The Monte Carlo simulation results show that the count rate of the DDA instrument for a spent fuel assembly of 4% initial enrichment, 45 GWD/MTU burnup, and 5 year cooling time is {approx} 9.8 x 10{sup 4} counts per second (c/s) with the 100-Hz repeated interrogation pattern of 0 to 10 {micro}s interrogation, 0.2 ms to 1 ms counting time, and 1 x 10{sup 9} n/s neutron source. The {sup 244}Cm neutron background count rate for this counting time scheme is {approx} 1 x 10{sup 4} c/s, and thus the signal to background ratio is {approx}10.

  6. Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s

    PubMed Central

    Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

    2015-01-01

    Obtaining Pu background data in the environment is essential for contamination source identification and assessment of environmental impact of Pu released from the Fukushima Daiichi nuclear power plant (FDNPP) accident. However, no baseline information on Pu isotopes in Fukushima Prefecture has been reported. Here we analyzed 80 surface soil samples collected from the central-eastern Japan during 1969–1977 for 239+240Pu activity concentration and 240Pu/239Pu atom ratio to establish the baseline before the FDNPP accident. We found that 239+240Pu activity concentrations ranged from 0.004 –1.46 mBq g−1, and 240Pu/239Pu atom ratios varied narrowly from 0.148 to 0.229 with a mean of 0.186 ± 0.015. We also reconstructed the surface deposition density of 241Pu using the 241Pu/239Pu atom ratio in the Japanese fallout reference material. The obtained results indicated that, for the FDNPP-accident released 241Pu, a similar radiation impact can be estimated as was seen for the global fallout deposited 241Pu in the last decades. PMID:25881009

  7. Plutonium in surface soil near the southwestern boundary of the Hanford project

    SciTech Connect

    Price, K.R.; Dirkes, R.L.

    1981-05-01

    Samples of airborne particles collected near the Prosser Barricade in another study showed low /sup 240/Pu//sup 239/Pu ratios that are indicative of Hanford-produced plutonium. In an effort to locate evidence of a trail or the remains of a large short-term release of plutonium that may have occurred during past Hanford operations, surface soil samples were collected along the southweastern boundary of the Hanford Site in December 1979. Results indicated the possibility of slightly elevated levels of /sup 239/ /sup 240/Pu (0.016 pCi/g) occurring in the general vicinity of the Arid Land Ecology Field lab extending to the junction of Highway 240 and Horn Rapids Road as compared to lower levels (0.006 pCi/g) in a northwesterly direction along the base of Rattlesnake Mountain and the eastern slope of Yakima Ridge. Assuming the worldwide average /sup 240/Pu//sup 239/Pu ratio of 0.18 for soil of the Pacific Northwest, the plutonium in these soil samples may be slightly less enriched with /sup 240/Pu (/sup 240/Pu//sup 239/Pu = 0.16). No evidence was discovered of an acute release remaining intact and crossing the southwestern boundary during the operating history of plutonium facilities in the 200 Areas.

  8. Technical Basis Document: A Statistical Basis for Interpreting Urinary Excretion of Plutonium Based on Accelerator Mass Spectrometry (AMS) for Selected Atoll Populations in the Marshall Islands

    SciTech Connect

    Bogen, K; Hamilton, T F; Brown, T A; Martinelli, R E; Marchetti, A A; Kehl, S R; Langston, R G

    2007-05-01

    We have developed refined statistical and modeling techniques to assess low-level uptake and urinary excretion of plutonium from different population group in the northern Marshall Islands. Urinary excretion rates of plutonium from the resident population on Enewetak Atoll and from resettlement workers living on Rongelap Atoll range from <1 to 8 {micro}Bq per day and are well below action levels established under the latest Department regulation 10 CFR 835 in the United States for in vitro bioassay monitoring of {sup 239}Pu. However, our statistical analyses show that urinary excretion of plutonium-239 ({sup 239}Pu) from both cohort groups is significantly positively associated with volunteer age, especially for the resident population living on Enewetak Atoll. Urinary excretion of {sup 239}Pu from the Enewetak cohort was also found to be positively associated with estimates of cumulative exposure to worldwide fallout. Consequently, the age-related trends in urinary excretion of plutonium from Marshallese populations can be described by either a long-term component from residual systemic burdens acquired from previous exposures to worldwide fallout or a prompt (and eventual long-term) component acquired from low-level systemic intakes of plutonium associated with resettlement of the northern Marshall Islands, or some combination of both.

  9. Deducing the 236Pu(n,f) and 237Pu(n,f) cross sections via the surrogate ratio method

    NASA Astrophysics Data System (ADS)

    Hughes, R. O.; Beausang, C. W.; Ross, T. J.; Burke, J. T.; Casperson, R. J.; McCleskey, M.; Cooper, N.; Escher, J. E.; Gell, K. B.; Good, E.; Humby, P.; Saastimoinen, A.; Tarlow, T. D.

    2013-10-01

    The short half-lives associated with certain minor actinide nuclei that are relevant to stockpile stewardship pursuits and the development of next-generation nuclear reactors make direct neutron measurements very challenging. In certain cases, a stable beam and target ``surrogate reaction'' can be used in lieu of the neutron-induced reaction, and the (n,f) cross section can then be deduced indirectly. Agreement between surrogate and direct measurements for (n,f) cross sections in actinide nuclei is usually within 10%. The present work reports on the measurement of the 236Pu(n,f) and 237Pu(n,f) cross sections via 239Pu(p,tf) and 239Pu(p,df) surrogate reactions, respectively. The experiment was performed at the Texas A&M University Cyclotron Facility using a 28.5 MeV proton beam to bombard 239Pu and 235U targets. Outgoing light ions were detected in coincidence with fission fragments using the STAR-LiTe detector array. Results of the analysis will be presented. This work was supported by DoE Grant Numbers: DE-FG52-09NA29454 and DE-FG02-05ER41379 (Richmond), DE-AC52-07NA27344 (LLNL) and DE-FG52-09NA29467 (TAMU).

  10. RAPID DETERMINATION OF 237 NP AND PU ISOTOPES IN WATER BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY

    SciTech Connect

    Maxwell, S.; Jones, V.; Culligan, B.; Nichols, S.; Noyes, G.

    2010-06-23

    A new method that allows rapid preconcentration and separation of plutonium and neptunium in water samples was developed for the measurement of {sup 237}Np and Pu isotopes by inductively-coupled plasma mass spectrometry (ICP-MS) and alpha spectrometry; a hybrid approach. {sup 238}U can interfere with {sup 239}Pu measurement by ICP-MS as {sup 238}UH{sup +} mass overlap and {sup 237}Np via peak tailing. The method provide enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then moving Pu to DGA resin for additional removal of uranium. The decontamination factor for uranium from Pu is almost 100,000 and the decontamination factor for U from Np is greater than 10,000. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration is performed using a streamlined calcium phosphate precipitation method. Purified solutions are split between ICP-MS and alpha spectrometry so that long and short-lived Pu isotopes can be measured successfully. The method allows for simultaneous extraction of 20 samples (including QC samples) in 4 to 6 hours, and can also be used for emergency response. {sup 239}Pu, {sup 242}Pu and {sup 237}Np were measured by ICP-MS, while {sup 236}Pu, {sup 238}Pu, and {sup 239}Pu were measured by alpha spectrometry.

  11. Global distribution of Pu isotopes and 237Np.

    PubMed

    Kelley, J M; Bond, L A; Beasley, T M

    1999-09-30

    Inventories and compositions of Pu isotopes and 237Np in archived soil samples collected in the 1970s from 54 locations around the world were determined to provide regional baselines for recognizing possible future environmental inputs of non-fallout Pu and Np. As sample sizes used in this work were small (typically 1 g), inhomogeneities in Pu and Np concentrations were easily recognizable and, as a result, we were able to determine that atypical debris in South America, from French testing in the South Pacific, is more widely and uniformly distributed than previously supposed. From our results we conclude that fallout 237Np/239Pu atom ratios are generally lower in the Southern Hemisphere (approximately 0.35) than in the Northern Hemisphere (approximately 0.47.) Moreover, 237Np/239Pu atom ratios are more device-dependent, hence more variable, than counterpart 240Pu/239Pu atom ratios. Given predictable trends caused by sample inhomogeneities, with only two exceptions, the Pu results of this work are entirely consistent with (and in several instances improve on) results previously reported for these same samples. However, unlike earlier interpretations used to explain these results, we recommend that fallout isotopic signatures be represented by mixing lines, rather than averages, to better reflect regional variations of stratospheric fallout inventories relative to tropospheric fallout inventories, and provide the theoretical basis for doing so. Finally, the Np results of this work constitute one of the largest single compilations of such data reported to date.

  12. Relationship of natural incidence and radiosensitivity for bone cancer in dogs

    SciTech Connect

    Taylor, G.N.; Lloyd, R.D.; Miller, S.C.; Jee, W.S.S.

    1997-10-01

    A comparison of the risk coefficients for {sup 239}Pu- or {sup 226}Ra-induced bone cancer in two canine breeds, one with a relatively low (beagle) and the other with a very high (St. Bernard) natural incidence, indicated only slightly higher risk in the giant breed. The differences in risk for skeletal malignancy in {sup 239}Pu and {sup 226}Ra dogs were nonsignificant (p > 0.05). Likewise, the values of the {sup 239}Pu:{sup 226}Ra {open_quotes}toxicity ratios{close_quotes} for these respective breeds, using bone cancer as the endpoint, were not significantly different at the 0.05 level. The anatomical distribution of the radiation-induced bone tumors tended to be a function of both the bone mass and the skeletal distribution of the radio nuclide, not the site of predilection for naturally occurring bone neoplasia. Although the etiology of the higher natural incidence of bone cancer in the St. Bernard was not determined, several possible factors, including a higher osteoblastic activity level in the St. Bernards, are presented. These data suggest that making extrapolations of radiation-induced bone cancer risk from animals to humans is valid. 26 refs., 5 tabs.

  13. Effects of combined exposure of F344 rats to inhaled Plutonium-239 dioxide and a chemical carcinogen (NNK)

    SciTech Connect

    Lundgren, D.L.; Carlton, W.W.; Griffith, W.C.

    1995-12-01

    Workers in nuclear weapons facilities have a significant potential for exposure to chemical carcinogens and to radiation from external sources or from internally deposited radionuclides such as {sup 239}Pu. Although the carcinogenic effects of inhaled {sup 239}Pu and many chemicals have been studied individually, very little information is available on their combined effects. One chemical carcinogen that workers could be exposed to via tobacco smoke is the tobacco-specific nitrosamine 4-(N-methyl-n-nitrosamino)-1-(3-pyridyl)-1(3-pyridyl)-1-butanone (NNK), a product of tobacco curing and the pyrolysis of nicotine in tobacco. NNK causes lung tumors in rats, regardless of the route of administration and to a lesser extent liver, nasal, and pancreatic tumors. From the results presented, it can be concluded that exposure to a chemical carcinogen (NNK) in combination with {alpha}-particle radiation from inhaled {sup 239}PuO{sub 2} acts in, at best, an additive manner in inducing lung cancer in rats.

  14. Analysis of thorium-salted fuels to improve uranium utilization in the once-through fuel cycle

    SciTech Connect

    Eschbach, E.A.; Merrill, E.T.; Prichard, A.W.

    1981-09-01

    Calculations and analyses indicate that no improvement can be achieved in uranium utilization for the once-through LWR fuel cycle over use of slightly enriched uranium by employing thorium distributed with uranium. The study included thorium additions: (1) slight amounts, (2) larger amounts, in either intimately mixed or in duplex pellets, (3) in spectrally shifted or not spectrally shifted reactors, and (4) in three- or five-year reactivity limited exposures. While thorium-uranium combinations improves the initial conversion ratio, the reactivity lifetime was not extended enough to override the additional uranium required. The effective fission cross-section of the bred /sup 233/U relative to /sup 239/Pu's in typical LWR neutron spectra is not large enough for /sup 233/U to make as great a contribution to end-of-life reactivity as /sup 239/Pu in a slightly enriched uranium fuel element. /sup 233/U's reactivity contribution relative to /sup 239/Pu's is lower in fuel configurations such as slightly enriched uranium LWR fuel loads. On the other hand, /sup 233/U's reactivity contribution appears more positive for reactors that involve lower average concentrations of thermal neutron absorbers. If /sup 238/U-thorium fuels reprocessed, the recovered /sup 233/U would increase uranium utilization, but may not reduce fuel cycle costs. The thorium-salted fuels exhibit substantially flatter reactivity characteristics with exposure time. Spectral shift helped the utilization of uranium and thorium.

  15. AMS of the Minor Plutonium Isotopes.

    PubMed

    Steier, P; Hrnecek, E; Priller, A; Quinto, F; Srncik, M; Wallner, A; Wallner, G; Winkler, S

    2013-01-01

    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure (239)Pu, (240)Pu, (241)Pu, (242)Pu and (244)Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of (244)Pu/(239)Pu = (5.7 ± 1.0) × 10(-5) based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the (242)Pu/(240)Pu ratio as an estimate of the initial (241)Pu/(239)Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

  16. Radionuclide concentrations in/on vegetation at radioactive-waste disposal Area G during the 1995 growing season. Progress report

    SciTech Connect

    Fresquez, P.R.; Vold, E.L.; Naranjo, L. Jr.

    1996-03-01

    Overstory (pinon pine) and understory (grass and forb) vegetation were collected within and around selected points at Area G--a low- level radioactive solid-waste disposal facility at Los Alamos National Laboratory--for the analysis of tritium ({sup 3}H), strontium ({sup 90}Sr), plutonium ({sup 238}Pu and {sup 239}Pu), cesium ({sup 137}Cs), and total uranium. Also, heavy metals (Ag, As, Ba, Be, Cd, Cr, Hg, Ni, Pb, Sb, Se, and Tl) in/on vegetation were determined. In general, most (unwashed) vegetation collected within and around Area G contained {sup 3}H, uranium, {sup 238}Pu, and {sup 239}Pu in higher concentrations than vegetation collected from background areas. Tritium, in particular, was detected as high as 7300 pCi mL{sup -1} in understory vegetation collected from the west side of the transuranic (TRU) pads. The south and west ends of the tritium shaft field also contained elevated levels of {sup 3}H in overstory, and especially in understory vegetation, as compared to background; this suggests that {sup 3}H may be migrating from this waste repository through surface and subsurface pathways. Also, understory vegetation collected north of the TRU pads (adjacent to the fence line of Area G) contained the highest values of {sup 238}Pu and {sup 239}Pu as compared to background, and may be a result of surface holding, storage, and/or disposal activities.

  17. 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.

  18. Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s

    NASA Astrophysics Data System (ADS)

    Yang, Guosheng; Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

    2015-04-01

    Obtaining Pu background data in the environment is essential for contamination source identification and assessment of environmental impact of Pu released from the Fukushima Daiichi nuclear power plant (FDNPP) accident. However, no baseline information on Pu isotopes in Fukushima Prefecture has been reported. Here we analyzed 80 surface soil samples collected from the central-eastern Japan during 1969-1977 for 239+240Pu activity concentration and 240Pu/239Pu atom ratio to establish the baseline before the FDNPP accident. We found that 239+240Pu activity concentrations ranged from 0.004 -1.46 mBq g-1, and 240Pu/239Pu atom ratios varied narrowly from 0.148 to 0.229 with a mean of 0.186 +/- 0.015. We also reconstructed the surface deposition density of 241Pu using the 241Pu/239Pu atom ratio in the Japanese fallout reference material. The obtained results indicated that, for the FDNPP-accident released 241Pu, a similar radiation impact can be estimated as was seen for the global fallout deposited 241Pu in the last decades.

  19. [Study of the influence of peroral zincacin on the removing of ingested Americium].

    PubMed

    Zhorova, E S; Il'in, L A; Ivannikov, A T; Popov, B A; Parfenova, I M

    2002-01-01

    Effect of different cincacine doses was studied in rats ingesting americium citrate during 2 weeks. As a result new data showing the possibility and efficacy of per oral cincacine administration at americium intake into digestive tract have been obtained. Dose dependence of cincacine efficacy has been stated for per oral 241Am intake. Preparation administration at a dose of 25 mumol/kg reduces amount of 241Am in skeleton, liver and kidney by 93, 90 and 33%, respectively and is optimum for radionuclide removal from the body and for the prevention of its deposition in organs. Digestive system organs and kidney structure at cincacine administration at a dose of 150 and 300 mumol/kg) to the rats ingesting 241Am have been studied.

  20. Integration of Americium Heat Source into the Advanced Stirling Radioisotope Generator

    NASA Astrophysics Data System (ADS)

    Schulze, Erich; Quinn, Richard

    2014-08-01

    The Lockheed Martin developed Advanced Stirling Radioisotope Generator (ASRG) design uses similar technology as proposed for the European Space Agency (ESA) Radioisotope Power System (RPS) development program but different isotopes. The RPS uses americium, 241Am isotope, while the ASRG uses plutonium, 238Pu isotope. The 238Pu isotope provides four times greater thermal output per kilogram than the 241Am isotope. Lockheed Martin performed an internally funded feasibility assessment that determined integration of a 241Am fueled heat source into the ASRG is achievable with no changes to ASRG technology and only structural and volumetric design considerations required. Lockheed Martin is interested in developing collaborative partnerships with the United Kingdom (UK) for the ESA RPS development program.

  1. Transportability Class of Americium in K Basin Sludge under Ambient and Hydrothermal Processing Conditions

    SciTech Connect

    Delegard, Calvin H.; Schmitt, Bruce E.; Schmidt, Andrew J.

    2006-08-01

    This report establishes the technical bases for using a ''slow uptake'' instead of a ''moderate uptake'' transportability class for americium-241 (241Am) for the K Basin Sludge Treatment Project (STP) dose consequence analysis. Slow uptake classes are used for most uranium and plutonium oxides. A moderate uptake class has been used in prior STP analyses for 241Am based on the properties of separated 241Am and its associated oxide. However, when 241Am exists as an ingrown progeny (and as a small mass fraction) within plutonium mixtures, it is appropriate to assign transportability factors of the predominant plutonium mixtures (typically slow) to the Am241. It is argued that the transportability factor for 241Am in sludge likewise should be slow because it exists as a small mass fraction as the ingrown progeny within the uranium oxide in sludge. In this report, the transportability class assignment for 241Am is underpinned with radiochemical characterization data on K Basin sludge and with studies conducted with other irradiated fuel exposed to elevated temperatures and conditions similar to the STP. Key findings and conclusions from evaluation of the characterization data and published literature are summarized here. Plutonium and 241Am make up very small fractions of the uranium within the K Basin sludge matrix. Plutonium is present at about 1 atom per 500 atoms of uranium and 241Am at about 1 atom per 19000 of uranium. Plutonium and americium are found to remain with uranium in the solid phase in all of the {approx}60 samples taken and analyzed from various sources of K Basin sludge. The uranium-specific concentrations of plutonium and americium also remain approximately constant over a uranium concentration range (in the dry sludge solids) from 0.2 to 94 wt%, a factor of {approx}460. This invariability demonstrates that 241Am does not partition from the uranium or plutonium fraction for any characterized sludge matrix. Most of the K Basin sludge characterization

  2. Unfolding the fast neutron spectra of a BC501A liquid scintillation detector using GRAVEL method

    NASA Astrophysics Data System (ADS)

    Chen, YongHao; Chen, XiMeng; Lei, JiaRong; An, Li; Zhang, XiaoDong; Shao, JianXiong; Zheng, Pu; Wang, XinHua

    2014-10-01

    Accurate knowledge of the neutron energy spectra is useful in basic research and applications. The overall procedure of measuring and unfolding the fast neutron energy spectra with BC501A liquid scintillation detector is described. The recoil proton spectrum of 241Am-Be neutrons was obtained experimentally. With the NRESP7 code, the response matrix of detector was simulated. Combining the recoil proton spectrum and response matrix, the unfolding of neutron spectra was performed by GRAVEL iterative algorithm. A MatLab program based on the GRAVEL method was developed. The continuous neutron spectrum of 241Am-Be source and monoenergetic neutron spectrum of D-T source have been unfolded successfully and are in good agreement with their standard reference spectra. The unfolded 241Am-Be spectrum are more accurate than the spectra unfolded by artificial neural networks in recent years.

  3. Alpha Coincidence Spectroscopy studied with GEANT4

    SciTech Connect

    Dion, Michael P.; Miller, Brian W.; Tatishvili, Gocha; Warren, Glen A.

    2013-11-02

    Abstract The high-energy side of peaks in alpha spectra, e.g. 241Am, as measured with a silicon detector has structure caused mainly by alpha-conversion electron and to some extent alphagamma coincidences. We compare GEANT4 simulation results to 241Am alpha spectroscopy measurements with a passivated implanted planar silicon detector. A large discrepancy between the measurements and simulations suggest that the GEANT4 photon evaporation database for 237Np (daughter of 241Am decay) does not accurately describe the conversion electron spectrum and therefore was found to have large discrepancies with experimental measurements. We describe how to improve the agreement between GEANT4 and alpha spectroscopy for actinides of interest by including experimental measurements of conversion electron spectroscopy into the photon evaporation database.

  4. A modeling study of contaminant transport resulting from flooding of Pit 9 at the Radioactive Waste Management Complex, Idaho National Engineering Laboratory

    SciTech Connect

    Magnuson, S.O.; Sondrup, A.J.

    1992-09-01

    A simulation study was conducted to determine if dissolved-phase transport due to flooding is a viable mechanism for explaining the presence of radionuclides in sedimentary interbeds below the Radioactive Waste Management Complex. In particular, the study focused on {sup 241}Am migration due to flooding of Pit 9 in 1969. A kinetically-controlled source term model was used to estimate the mass of {sup 241}Am that leached as a function of a variable surface infiltration rate. This mass release rate was then used in a numerical simulation of unsaturated flow and transport to estimate the advance due to flooding of the {sup 241}Am front down towards the 110 ft interbed. The simulation included the effect of fractures by superimposing them onto elements that represented the basalt matrix. For the base case, hydraulic and transport parameters were assigned using the best available data. The advance of the {sup 241}Am front due to flooding for this case was minimal, on the order of a few meters. This was due to the strong tendency for {sup 241}Am to sorb onto both basalts and sediments. In addition to the base case simulation, a parametric sensitivity study was conducted which tested the effect of sorption in the fractures, in the kinetic source term, and in the basalt matrix. Of these, the only case which resulted in significant transport was when there was no sorption in the basalt matrix. The indication being that other processes such as transport by radiocolloids or organic complexation may have contributed. However, caution is advised in interpreting these results due to approximations in the numerical method that was used incorporate fractures into the simulation. The approximations are a result of fracture apertures being significantly smaller than the elements over which they are superimposed. The sensitivity of the {sup 241}Am advance to the assumed hydraulic conductivity for the fractures was also tested.

  5. An in situ survey of Clean Slate 1, 2, and 3, Tonopah Test Range, Central Nevada. Date of survey: September--November 1993

    SciTech Connect

    1995-08-01

    A ground-based in situ radiological survey was conducted downwind of the Clean Slate 1, 2, and 3 nuclear safety test sites at the Tonopah Test Range in central Nevada from September through November 1993. The purpose of the study was to corroborate the americium-241 ({sup 241}Am) soil concentrations that were derived from the aerial radiological survey of the Clean Slate areas, which was conducted from August through October 1993. The presence of {sup 241}Am was detected at 140 of the 190 locations, with unrecoverable or lost data accounting for fifteen (15) of the sampling points. Good agreement was obtained between the aerial and in situ results.

  6. Long-range tropospheric transport of uranium and plutonium weapons fallout from Semipalatinsk nuclear test site to Norway.

    PubMed

    Wendel, Cato Christian; Fifield, L Keith; Oughton, Deborah H; Lind, Ole Christian; Skipperud, Lindis; Bartnicki, Jerzy; Tims, Stephen G; Høibråten, Steinar; Salbu, Brit

    2013-09-01

    A combination of state-of-the-art isotopic fingerprinting techniques and atmospheric transport modelling using real-time historical meteorological data has been used to demonstrate direct tropospheric transport of radioactive debris from specific nuclear detonations at the Semipalatinsk test site in Kazakhstan to Norway via large areas of Europe. A selection of archived air filters collected at ground level at 9 stations in Norway during the most intensive atmospheric nuclear weapon testing periods (1957-1958 and 1961-1962) has been screened for radioactive particles and analysed with respect to the concentrations and atom ratios of plutonium (Pu) and uranium (U) using accelerator mass spectrometry (AMS). Digital autoradiography screening demonstrated the presence of radioactive particles in the filters. Concentrations of (236)U (0.17-23nBqm(-3)) and (239+240)Pu (1.3-782μBqm(-3)) as well as the atom ratios (240)Pu/(239)Pu (0.0517-0.237) and (236)U/(239)Pu (0.0188-0.7) varied widely indicating several different sources. Filter samples from autumn and winter tended to have lower atom ratios than those sampled in spring and summer, and this likely reflects a tropospheric influence in months with little stratospheric fallout. Very high (236)U, (239+240)Pu and gross beta activity concentrations as well as low (240)Pu/(239)Pu (0.0517-0.077), (241)Pu/(239)Pu (0.00025-0.00062) and (236)U/(239)Pu (0.0188-0.046) atom ratios, characteristic of close-in and tropospheric fallout, were observed in filters collected at all stations in Nov 1962, 7-12days after three low-yield detonations at Semipalatinsk (Kazakhstan). Atmospheric transport modelling (NOAA HYSPLIT_4) using real-time meteorological data confirmed that long range transport of radionuclides, and possibly radioactive particles, from Semipalatinsk to Norway during this period was plausible. The present work shows that direct tropospheric transport of fallout from atmospheric nuclear detonations periodically may have

  7. Expected total counts for the Self-Interrogation Neutron Resonance Densitometry measurements of spent nuclear fuel

    SciTech Connect

    Rossa, Riccardo; Borella, Alessandro; Van der Meer, Klaas; Labeau, Pierre-Etienne; Pauly, Nicolas

    2015-07-01

    The Self-Interrogation Neutron Resonance Densitometry (SINRD) is a passive neutron technique that aims at a direct quantification of {sup 239}Pu in spent fuel assemblies by measuring the attenuation of the neutron flux in the energy region close to the 0.3 eV resonance of {sup 239}Pu. The {sup 239}Pu mass is estimated by calculating the SINRD signature, that is the ratio between the neutron counts in the fast energy region and around the 0.3 eV resonance region. The SINRD measurement approach in this study consisted in introducing a small neutron detector in the central guide tube of a PWR 17x17 fuel assembly. In order to measure the neutron flux in the energy regions defined in the SINRD signature, different detector types were used. The response of a bare {sup 238}U fission chamber is considered for the determination of the fast neutron flux, while other thermal-epithermal detectors wrapped in neutron absorbers are envisaged to measure the neutron flux around the resonance region. This paper provides an estimation of the total neutron counts that can be achieved with the detector types proposed for the SINRD measurement. In the first section a set of detectors are evaluated in terms of total neutron counts and sensitivity to the {sup 239}Pu content, in order to identify the optimal measurement configuration for each detector type. Then a study is performed to increase the total neutron counts by increasing the detector size. The study shows that the highest total neutron counts are achieved by using either {sup 3}He or {sup 10}B proportional counters because of the high neutron efficiency of these detectors. However, the calculations indicate that the biggest contribution to the measurement uncertainty is due to the measurement of the fast neutron flux. Finally, similar sensitivity to the {sup 239}Pu content is obtained by using the different detector types for the measurement of the neutron flux close to th