Science.gov

Sample records for 240pu 241pu 242pu

  1. Prompt fission γ -ray spectrum characteristics from 240Pu(sf ) and 242Pu(sf )

    NASA Astrophysics Data System (ADS)

    Oberstedt, S.; Oberstedt, A.; Gatera, A.; Göök, A.; Hambsch, F.-J.; Moens, A.; Sibbens, G.; Vanleeuw, D.; Vidali, M.

    2016-05-01

    In this paper we present first results for prompt fission γ -ray spectra (PFGS) characteristics from the spontaneous fission (sf) of 240Pu and 242Pu. For 242Pu(sf ) we obtained, after proper unfolding of the detector response, an average energy per photon ɛ¯γ=(0.843 ±0.012 ) MeV, an average multiplicity M¯γ=(6.72 ±0.07 ) , and an average total γ -ray energy release per fission E¯γ ,tot = (5.66 ± 0.06) MeV. The 240Pu(sf ) emission spectrum was obtained by applying a so-called detector-response transformation function determined from the 242Pu spectrum measured in exactly the same geometry. The results are an average energy per photon ɛ¯γ=(0.80 ±0.07 ) MeV, the average multiplicity M¯γ = (8.2 ± 0.4), and an average total γ -ray energy release per fission E¯γ ,tot = (6.6 ± 0.5) MeV. The PFGS characteristics for 242Pu(sf ) are in very good agreement with those from thermal-neutron-induced fission on 241Pu and scales well with the corresponding prompt neutron multiplicity. Our results in the case of 240Pu(sf ), although drawn from a limited number of events, show a significantly enhanced average multiplicity and average total energy, but may be understood from a different fragment yield distribution in 240Pu(sf ) compared to that of 242Pu(sf ).

  2. Fragment mass and kinetic energy distributions for /sup 242/Pu(sf), /sup 241/Pu(n/sub th/,f), and /sup 242/Pu(. gamma. ,f)

    SciTech Connect

    Thierens, H.; Jacobs, E.; D'hondt, P.; De Clercq, A.; Piessens, M.; De Frenne, D.

    1984-02-01

    Energy correlation measurements were performed for the spontaneous fission of /sup 242/Pu, the thermal-neutron-induced fission of /sup 241/Pu, and the photofission of /sup 242/Pu with 12-, 15-, 20-, and 30-MeV bremsstrahlung. The photofission cross section for /sup 242/Pu was determined up to 30 MeV. For /sup 242/Pu(sf) the overall kinetic energy distribution is strongly asymmetric and the overall mass distribution has a very high peak yield (9%). Important deviations of the average total kinetic energy release and the average light and heavy fragment masses and from the systematics of Unik et al. are also observed for this fissioning system. These effects can be explained in the framework of the static scission point model by the strong preferential formation of a shell-stabilized scission configuration with the neutron number of the heavy and light fragments in the vicinity of the spherical N = 82 neutron shell and the deformed N = 66 neutron shell, respectively. A decrease of with the average excitation energy , d/d = -0.30 +- 0.04, is observed in the photofission of /sup 242/Pu.

  3. 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. PMID:24401459

  4. Calculated gamma-ray spectra for keV neutron capture in /sup 240/Pu, /sup 242/Pu, and /sup 238/U

    SciTech Connect

    Reffo, G.; Fabbri, F.; Kappeler, F.; Wisshak, K.

    1983-03-01

    Capture gamma-ray spectra of /sup 240/Pu, /sup 242/Pu, and /sup 238/U were calculated in the framework of the spherical optical model and the statistical model. A consistent set of input parameters was determined from available experimental information or from model-guided systematics. The complete gamma-ray cascades were calculated considering all possible transitions up to multiplicity seven. All experimental information on level schemes and gamma-ray transition probabilities of the compound nuclei was explicitly included as input. The capture gamma-ray spectra were used to correct experimental data for the capture cross sections of /sup 240/Pu and /sup 242/Pu from a relative measurement using a Moxon-Rae detector with a graphite converter and with /sup 197/Au and /sup 238/U as standards. This correction is required to take into account that the detector efficiency is not exactly proportional to the gamma-ray energy. The resulting correction factors proved to be negligible for measurements relative to /sup 238/U; whereas, they are about 3% if gold is used as a standard.

  5. 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.

  6. 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. PMID:24328266

  7. Vertical distribution of (241)Pu in the southern Baltic Sea sediments.

    PubMed

    Strumińska-Parulska, Dagmara I

    2014-12-15

    The vertical distribution of plutonium (241)Pu in marine sediments can assist in determining the deposition history and sedimentation process of analyzed regions. In addition, (241)Pu/(239+240)Pu activity ratio could be used as a sensitive fingerprint for radioactive source identification. The present preliminary studies on vertical distribution of (241)Pu in sediments from four regions of the southern Baltic Sea are presented. The distribution of (241)Pu was not uniform and depended on sediment geomorphology and depth as well as location. The highest concentrations of plutonium were found in the surface layers of all analyzed sediments and originated from the Chernobyl accident. PMID:25455816

  8. Highly accurate measurements of the spontaneous fission half-life of 240,242Pu

    NASA Astrophysics Data System (ADS)

    Salvador-Castiñeira, P.; Bryś, T.; Eykens, R.; Hambsch, F.-J.; Moens, A.; Oberstedt, S.; Sibbens, G.; Vanleeuw, D.; Vidali, M.; Pretel, C.

    2013-12-01

    Fast spectrum neutron-induced fission cross-section data for transuranic isotopes are of special demand from the nuclear data community. In particular highly accurate data are needed for the new generation IV nuclear applications. The aim is to obtain precise neutron-induced fission cross sections for 240Pu and 242Pu. To do so, accurate data on spontaneous fission half-lives must be available. Also, minimizing uncertainties in the detector efficiency is a key point. We studied both isotopes by means of a twin Frisch-grid ionization chamber with the goal of improving the present data on the neutron-induced fission cross section. For the two plutonium isotopes the high α-particle decay rates pose a particular problem to experiments due to piling-up events in the counting gas. Argon methane and methane were employed as counting gases, the latter showed considerable improvement in signal generation due to its higher drift velocity. The detection efficiency for both samples was determined, and improved spontaneous fission half-lives were obtained with very low statistical uncertainty (0.13% for 240Pu and 0.04% for 242Pu): for 240Pu, T1/2,SF=1.165×1011 yr (1.1%), and for 242Pu, T1/2,SF=6.74×1010 yr (1.3%). Systematic uncertainties are due to sample mass (0.4% for 240Pu and 0.9% for 242Pu) and efficiency (1%).

  9. 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

  10. Measurement of the 242Pu neutron capture cross section

    NASA Astrophysics Data System (ADS)

    Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; Bucher, B.; Bredeweg, T. A.; Baramsai, B.; Couture, A.; Jandel, M.; Mosby, S.; O'Donnell, J. M.; Ullmann, J. L.; Chyzh, A.; Dance Collaboration

    2015-10-01

    Precision (n,f) and (n, γ) cross sections are important for the network calculations of the radiochemical diagnostic chain for the U.S. DOE's Stockpile Stewardship Program. 242Pu(n, γ) cross section is relevant to the network calculations of Pu and Am. Additionally, new reactor concepts have catalyzed considerable interest in the measurement of improved cross sections for neutron-induced reactions on key actinides. To date, little or no experimental data has been reported on 242Pu(n, γ) for incident neutron energy below 50 keV. A new measurement of the 242Pu(n, γ) reaction was performed with the DANCE together with an improved PPAC for fission-fragment detection at LANSCE during FY14. The relative scale of the 242Pu(n, γ) cross section spans four orders of magnitude for incident neutron energies from thermal to ~ 30 keV. The absolute scale of the 242Pu(n, γ) cross section is set according to the measured 239Pu(n,f) resonance at 7.8 eV; the target was spiked with 239Pu for this measurement. The absolute 242Pu(n, γ) neutron capture cross section is ~ 30% higher than the cross section reported in ENDF for the 2.7 eV resonance. Latest results to be reported. Funded by U.S. DOE Contract No. DE-AC52-07NA27344 (LLNL) and DE-AC52-06NA25396 (LANL). U.S. DOE/NNSA Office of Defense Nuclear Nonproliferation Research and Development. Isotopes (ORNL).

  11. Microscopic Calculations of 240Pu Fission

    SciTech Connect

    Younes, W; Gogny, D

    2007-09-11

    Hartree-Fock-Bogoliubov calculations have been performed with the Gogny finite-range effective interaction for {sup 240}Pu out to scission, using a new code developed at LLNL. A first set of calculations was performed with constrained quadrupole moment along the path of most probable fission, assuming axial symmetry but allowing for the spontaneous breaking of reflection symmetry of the nucleus. At a quadrupole moment of 345 b, the nucleus was found to spontaneously scission into two fragments. A second set of calculations, with all nuclear moments up to hexadecapole constrained, was performed to approach the scission configuration in a controlled manner. Calculated energies, moments, and representative plots of the total nuclear density are shown. The present calculations serve as a proof-of-principle, a blueprint, and starting-point solutions for a planned series of more comprehensive calculations to map out a large set of scission configurations, and the associated fission-fragment properties.

  12. Tissue, cellular, and subcellular distribution of /sup 241/Pu in the rat testes

    SciTech Connect

    Miller, S.C.; Bowman, B.M.

    1983-05-01

    The distribution and localization of /sup 241/Pu in rat testes were determined by quantitative autoradiography. Rats were given intravenous injection of /sup 241/Pu citrate and tissues were collected 1 week later. The tissue distribution of /sup 241/Pu was determined by light microscope autoradiography. Significant concentrations of /sup 241/Pu were observed in the interstitial tissue but not in seminiferous tubules. The cellular distribution and subcellular localization of /sup 241/Pu were determined by electron microscope autoradiography. Within the interstitial tissue, /sup 241/Pu was concentrated in microphages. There was no preferential localization of /sup 241/Pu in any other interstitial tissue components. Within interstitial tissue macrophages, /sup 241/Pu was concentrated in the lysosomal system of the cell. Other organellar compartments of the cell did not preferentially incorporate /sup 241/Pu. The association of /sup 241/Pu with the macrophage lysosomal system may explain the long retention times of Pu in testes as observed in experimental studies.

  13. Consistent Data Assimilation of Isotopes: 242Pu and 105Pd

    SciTech Connect

    G. Palmiotti; H. Hiruta; M. Salvatores

    2012-09-01

    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 are analyzed using the EMPIRE evaluated files for 242Pu and 105Pd. In particular irradiation experiments (PROFIL-1 and -2, TRAPU-1, -2 and -3) provide information about capture cross sections, and a critical configuration, COSMO, where fission spectral indexes were measured, provides information about fission cross section. The observed discrepancies between calculated and experimental results are used in conjunction with the computed sensitivity coefficients and covariance matrix for nuclear parameters in a consistent data assimilation. The results obtained by the consistent data assimilation indicate that not so large modifications on some key identified nuclear parameters allow to obtain reasonable C/E. However, for some parameters such variations are outside the range of 1 s of their initial standard deviation. This can indicate a possible conflict between differential measurements (used to calculate the initial standard deviations) and the integral measurements used in the statistical data adjustment. Moreover, an inconsistency between the C/E of two sets of irradiation experiments (PROFIL and TRAPU) is observed for 242Pu. This is the end of this project funded by the Nuclear Physics Program of the DOE Office of Science. We can indicate that a proof of principle has been demonstrated for a few isotopes for this innovative methodology. However, we are still far from having explored all the possibilities and made this methodology to be considered proved and robust. In particular many issues are worth further investigation: • Non-linear effects • Flexibility of nuclear parameters in describing cross sections • Multi-isotope consistent assimilation • Consistency between differential and integral

  14. Neutron-induced fission cross sections of 242Pu from 0.3 MeV to 3 MeV

    NASA Astrophysics Data System (ADS)

    Salvador-Castiñeira, P.; Bryś, T.; Eykens, R.; Hambsch, F.-J.; Göök, A.; Moens, A.; Oberstedt, S.; Sibbens, G.; Vanleeuw, D.; Vidali, M.; Pretel, C.

    2015-10-01

    The majority of the next generation of nuclear power plants (GEN-IV) will work in the fast-neutron-energy region, as opposed to present day thermal reactors. This leads to new and more accurate nuclear-data needs for some minor actinides and structural materials. Following those upcoming demands, the Organisation for Economic Cooperation and Development Nuclear Energy Agency performed a sensitivity study. Based on the latter, an improvement in accuracy from the present 20% to 5% is required for the 242Pu(n ,f ) cross section. Within the same project both the 240Pu(n ,f ) cross section and the 242Pu(n ,f ) cross section were measured at the Van de Graaff accelerator of the Joint Research Centre at the Institute for Reference Materials and Measurements, where quasimonoenergetic neutrons were produced in an energy range from 0.3 MeV up to 3 MeV. A twin Frisch-grid ionization chamber has been used in a back-to-back configuration as fission-fragment detector. The 242Pu(n ,f ) cross section has been normalized to three different isotopes: 237Np(n ,f ) , 235U(n ,f ) , and 238U(n ,f ) . A comprehensive study of the corrections applied to the data and the uncertainties associated is given. The results obtained are in agreement with previous experimental data at the threshold region up to 0.8 MeV. The resonance-like structure at 0.8 to 1.1 MeV, visible in the evaluations and in most previous experimental values, was not reproduced with the same intensity in this experiment. For neutron energies higher than 1.1 MeV, the results of this experiment are slightly lower than the Evaluated Nuclear Data File/B-VII.1 evaluation but in agreement with the experiment of Tovesson et al. (2009) as well as Staples and Morley (1998). Finally, for energies above 1.5 MeV, the results show consistency with the present evaluations.

  15. Perturbation in the 240Pu/239Pu global fallout ratio in local sediments following the nuclear accidents at Thule (Greenland) and Palomares (Spain).

    PubMed

    Mitchell, P I; León Vintró, L; Dahlgaard, H; Gascó, C; Sánchez-Cabeza, J A

    1997-08-25

    It is well established that the main source of the plutonium found in marine sediments throughout the Northern Hemisphere is global stratospheric fallout, characterized by a typical 240Pu/239Pu atom ratio of approximately 0.18. Measurement of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing (e.g. Bikini Atoll, Nevada test site, Mururoa Atoll), has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the 240Pu/239Pu ratio has been examined in samples of sediment (and soil) collected at Thule (Greenland) and Palomares (Spain), where accidents involving the release and dispersion of plutonium from fractured nuclear weapons occurred in 1968 and 1966, respectively. The 240Pu/239Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution, and confirmed in the case of the most active samples by high-resolution X-ray spectrometry. Only samples which displayed plutonium heterogeneities, i.e. hot particles or concentrations well in excess (at least two orders of magnitude) of those expected from global fallout, were selected for analysis. The analytical results showed that at Thule the mean 240Pu/239Pu atom ratio was 0.033 +/- 0.004 (n = 4), while at Palomares the equivalent ratio appeared to be significantly higher at 0.056 +/- 0.003 (n = 4). Both ratios are indicative of low burn-up plutonium and are consistent with those reported for weapons-grade plutonium. It is noteworthy that the mean 238Pu/239Pu activity ratio in the Thule samples, at 0.0150 +/- 0.0017 (n = 4), was also lower than that measured in the Palomares samples, namely, 0.0275 +/- 0.0012 (n = 4). The 241Pu/239Pu ratios were similarly different. Finally, the data show, in contrast to Palomares, that not all of the samples from the Thule accident site were contaminated with plutonium of identical isotopic composition. PMID:9241884

  16. Absolute measurement of the 242Pu neutron-capture cross section

    NASA Astrophysics Data System (ADS)

    Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; Bucher, B.; Chyzh, A.; Bredeweg, T. A.; Baramsai, B.; Couture, A.; Jandel, M.; Mosby, S.; O'Donnell, J. M.; Ullmann, J. L.; Dance Collaboration

    2016-04-01

    The absolute neutron-capture cross section of 242Pu was measured at the Los Alamos Neutron Science Center using the Detector for Advanced Neutron-Capture Experiments array along with a compact parallel-plate avalanche counter for fission-fragment detection. The first direct measurement of the 242Pu(n ,γ ) cross section was made over the incident neutron energy range from thermal to ≈6 keV, and the absolute scale of the (n ,γ ) cross section was set according to the known 239Pu(n ,f ) resonance at En ,R=7.83 eV. This was accomplished by adding a small quantity of 239Pu to the 242Pu sample. The relative scale of the cross section, with a range of four orders of magnitude, was determined for incident neutron energies from thermal to ≈40 keV. Our data, in general, are in agreement with previous measurements and those reported in ENDF/B-VII.1; the 242Pu(n ,γ ) cross section at the En ,R=2.68 eV resonance is within 2.4 % of the evaluated value. However, discrepancies exist at higher energies; our data are ≈30 % lower than the evaluated data at En≈1 keV and are approximately 2 σ away from the previous measurement at En≈20 keV.

  17. Absolute measurement of the 242Pu neutron-capture cross section

    DOE PAGESBeta

    Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; Bucher, B.; Chyzh, A.; Bredeweg, T. A.; Baramsai, B.; Couture, A.; Jandel, M.; Mosby, S.; et al

    2016-04-21

    Here, the absolute neutron-capture cross section of 242Pu was measured at the Los Alamos Neutron Science Center using the Detector for Advanced Neutron-Capture Experiments array along with a compact parallel-plate avalanche counter for fission-fragment detection. The first direct measurement of the 242Pu(n,γ) cross section was made over the incident neutron energy range from thermal to ≈ 6 keV, and the absolute scale of the (n,γ) cross section was set according to the known 239Pu(n,f) resonance at En,R = 7.83 eV. This was accomplished by adding a small quantity of 239Pu to the 242Pu sample. The relative scale of the crossmore » section, with a range of four orders of magnitude, was determined for incident neutron energies from thermal to ≈ 40 keV. Our data, in general, are in agreement with previous measurements and those reported in ENDF/B-VII.1; the 242Pu(n,γ) cross section at the En,R = 2.68 eV resonance is within 2.4% of the evaluated value. However, discrepancies exist at higher energies; our data are ≈30% lower than the evaluated data at En ≈ 1 keV and are approximately 2σ away from the previous measurement at En ≈ 20 keV.« less

  18. Cluster approach to the structure of 240Pu

    NASA Astrophysics Data System (ADS)

    Shneidman, T. M.; Adamian, G. G.; Antonenko, N. V.; Jolos, R. V.; Zhou, Shan-Gui

    2015-09-01

    The cluster approach, which allows us to take into account both shape deformation parameters and cluster degrees of freedom, is developed to describe alternating-parity rotational bands. The important ingredient of the model is the dinuclear system concept in which the wave function of the nucleus is treated as a superposition of a mononucleus and two-cluster configurations. The model is applied to describe the multiple positive and negative parity rotational bands in 240Pu . The observed excitation spectrum and the angular momentum dependences of the parity splitting and of the electric E 1 and E 2 transition moments are explained. Special emphasis is made on the investigation of the recently measured positive parity 02+ rotational band of reflection-asymmetric nature. The results suggest that this band might be understood as being built on the lowest excited state in the mass asymmetry degree of freedom. The B (E 1 )/B (E 2 ) branching ratios between the reduced transition probabilities of decay from the states of the 02+ band to the first negative parity band and to the groundstate band, respectively, are calculated and compared with experimental data.

  19. Determination of /sup 239,240/Pu in bottom sediments of the Baltic Sea

    SciTech Connect

    Kuznetsov, Yu.V.; Legin, V.K.; Pospelov, Yu.N.; Simonyak, Z.N.

    1988-11-01

    We present a technique for determining the /sup 239,240/Pu content, using /sup 236/Pu as the monitor of chemical yield, in samples of soils and bottom sediments - objects of the external environment. Plutonium is extracted from the matrix material by leaching with a mixture of concentrated acids HCl-HNO/sub 3/, after which it is separated by ion-exchange methods. After electrodeposition onto stainless steel discs the activity of the nuclides of plutonium is measured by the method of alpha-spectrometry. The average chemical yields during the analysis of the samples was 40-60%, the relative standard deviation was 10%, and the lower limit of detectability was 0.3 Bq. We present results of the determination of the /sup 239,240/Pu content in surface samples of bottom sediments from the Gulf of Finland and that past of the Baltic Sea which adjoins the territory of the USSR. It is found that the unit activity of /sup 239,240/Pu in the bottom sediments varies within the limits of 0.4-1.2 Bq/kg and lies at the global level. Global genesis of /sup 239,240/Pu in the bottom sediments of the Gulf of Finland and the open parts of the Baltic Sea is also confirmed by the values which are found for the ratios /sup 238/Pu//sup 239,240/Pu and /sup 239,240/Pu//sup 137/Cs.

  20. Measurement of the 240,242Pu Neutron-induced Fission Cross Sections

    NASA Astrophysics Data System (ADS)

    Salvador-Castiñeira, P.; Bevilacqua, R.; Bryś, T.; Hambsch, F.-J.; Oberstedt, S.; Pretel, C.; Vidali, M.

    The neutron-induced fission cross section of 240,242Pu has been measured at the Van de Graaff facility of the Institute for Reference Materials and Measurements (JRC-IRMM). A Twin-Frisch Grid Ionization Chamber (TFGIC) has been used in a back-to-back geometry with the secondary standards 237Np and 238U to normalize the cross section. The energy range measured is from 0.2 keV up to 3 MeV. Preliminary results show some discrepancies around 1 MeV for the 242Pu with the ENDF/B-VII.1 evaluation. The spontaneous fission half-life has been measured for both isotopes, too. Preliminary results show reasonable agreement with the recommended values.

  1. New Superheavy Element Isotopes: 242Pu(48Ca,5n)285114

    SciTech Connect

    Ellison, Paul A; Gregorich, Kenneth E.; Berryman, Jill S.; Bleuel, Darren L.; Clark, Roderick M.; Dragojevic, Irena; Dvorak, Jan; Fallon, Paul; Fineman-Sotomayor, Carolina; Gates, Jacklyn M.; Gothe, Oliver R.; Lee, I-Yang; Loveland, Walter D.; McLaughlin, Joseph P.; Paschalis, Stefanos; Petri, Marina-Kalliopi; Qian, Jing; Stavsetra, Liv; Wiedeking, Mathis; Nitsche, Heino

    2010-10-22

    The new, neutron-deficient, superheavy element isotope {sup 285}114 was produced in {sup 48}Ca irradiations of {sup 242}Pu targets at a center-of-target beam energy of 256 MeV (E* = 50 MeV). The {alpha} decay of {sup 285}114 was followed by the sequential {alpha} decay of four daughter nuclides, {sup 281}Cn, {sup 277}Ds, {sup 273}Hs, and {sup 269}Sg. {sup 265}Rf was observed to decay by spontaneous fission. The measured {alpha}-decay Q values were compared with those from a macroscopic-microscopic nuclear mass model to give insight into superheavy element shell effects. The {sup 242}Pu({sup 48}Ca,5n){sup 285}114 cross section was 0.6{sub -0.5}{sup +0.9} pb.

  2. Statistical properties of 243Pu, and 242Pu(n ,γ ) cross section calculation

    NASA Astrophysics Data System (ADS)

    Laplace, T. A.; Zeiser, F.; Guttormsen, M.; Larsen, A. C.; Bleuel, D. L.; Bernstein, L. A.; Goldblum, B. L.; Siem, S.; Garotte, F. L. Bello; Brown, J. A.; Campo, L. Crespo; Eriksen, T. K.; Giacoppo, F.; Görgen, A.; Hadyńska-KlÈ©k, K.; Henderson, R. A.; Klintefjord, M.; Lebois, M.; Renstrøm, T.; Rose, S. J.; Sahin, E.; Tornyi, T. G.; Tveten, G. M.; Voinov, A.; Wiedeking, M.; Wilson, J. N.; Younes, W.

    2016-01-01

    The level density and γ -ray strength function (γ SF ) of 243Pu have been measured in the quasicontinuum using the Oslo method. Excited states in 243Pu were populated using the 242Pu(d ,p ) reaction. The level density closely follows the constant-temperature level density formula for excitation energies above the pairing gap. The γ SF displays a double-humped resonance at low energy as also seen in previous investigations of actinide isotopes. The structure is interpreted as the scissors resonance and has a centroid of ωSR=2.42 (5 ) MeV and a total strength of BSR=10.1 (15 ) μN2 , which is in excellent agreement with sum-rule estimates. The measured level density and γ SF were used to calculate the 242Pu(n ,γ ) cross section in a neutron energy range for which there were previously no measured data.

  3. Neutron-induced Fission Cross Section of 240,242Pu

    NASA Astrophysics Data System (ADS)

    Salvador-Castiñeira, P.; Bryś, T.; Eykens, R.; Hambsch, F.-J.; Göök, A.; Oberstedt, S.; Pretel, C.; Sibbens, G.; Vanleeuw, D.; Vidali, M.

    A sensitivity analysis for the new generation of fast reactors [Salvatores (2008)] has shown the importance of improved cross section data for several actinides. Among them, the 240,242Pu(n,f) cross sections require an accuracy improvement to 1-3% and 3-5%, respectively, from the current level of 6% and 20%. At the Van de Graaff facility of the Institute for Reference Materials and Measurements (JRC-IRMM) the fission cross section of the two isotopes was measured relative to two secondary standard reactions, 237Np(n,f) and 238U(n,f), using a twin Frisch-grid ionization chamber. The secondary standard reactions were benchmarked through measurements against the primary standard reaction 235U(n,f) in the same geometry. Sample masses were determined by means of low-geometry alpha counting or/and a 2π Frisch-grid ionization chamber, with an uncertainty lower than 2%. The neutron flux and the impact of scattering from material between source and target was examined, the largest effect having been found in cross section ratio measurements between a fissile and a fertile isotope. Our 240,242Pu(n,f) cross sections are in agreement with previous experimental results and slightly lower than present evaluations. In case of the 242Pu(n,f) reaction no evidence for a resonance at En=1.1 MeV was found.

  4. Determination of 241Pu in nuclear waste slurries: a comparative study using LSC and ICP-MS.

    PubMed

    Jäggi, M; Röllin, S; Alvarado, J A Corcho; Eikenberg, J

    2012-02-01

    (241)Pu was determined in slurry samples from a nuclear reactor decommissioning project at the Paul Scherrer Institute (Switzerland). To validate the results, the (241)Pu activities of five samples were determined by LSC (TriCarb and Quantulus) and ICP-MS, with each instrument at a different laboratory. In lack of certified reference materials for (241)Pu, the methods were further validated using the (241)Pu information values of two reference sediments (IAEA-300 and IAEA-384). Excellent agreement with the results was found between LSC and ICP-MS in the nuclear waste slurries and the reference sediments. PMID:22079960

  5. Modeling and production of 240Am by deuteron-induced activation of a 240Pu target

    NASA Astrophysics Data System (ADS)

    Finn, Erin C.; McNamara, Bruce; Greenwood, Larry; Wittman, Richard; Soderquist, Charles; Woods, Vincent; VanDevender, Brent; Metz, Lori; Friese, Judah

    2015-04-01

    A novel reaction pathway for production of 240Am is reported. Models of reaction cross-sections in EMPIRE II suggest that deuteron-induced activation of a 240Pu target produces maximum yields of 240Am from 11.5 MeV incident deuterons. This activation had not been previously reported in the literature. A 240Pu target was activated under the modeled optimum conditions to produce 240Am. The modeled cross-section for the 240Pu(d, 2n)240Am reaction is on the order of 20-30 mbarn, but the experimentally estimated value is 5.6 ± 0.2 mbarn. We discuss reasons for the discrepancy as well as production of other Am isotopes that contaminate the final product.

  6. Modeling and production of 240Am by deuteron-induced activation of a 240Pu target

    SciTech Connect

    Finn, Erin C.; McNamara, Bruce K.; Greenwood, Lawrence R.; Wittman, Richard S.; Soderquist, Chuck Z.; Woods, Vincent T.; VanDevender, Brent A.; Metz, Lori A.; Friese, Judah I.

    2015-02-01

    A novel reaction pathway for production of 240Am is reported. Models of reaction cross-sections in EMPIRE II suggests that deuteron-induced activation of a 240Pu target produces maximum yields of 240Am from 11.5 MeV incident deuterons. This activation had not been previously reported in the literature. A 240Pu target was activated under the modeled optimum conditions to produce 240Am. The modeled cross-section for the 240Pu(d, 2n)240Am reaction is on the order of 20-30 mbarn, but the experimentally estimated value is 5.3 ± 0.2 mbarn. We discuss reasons for the discrepancy as well as production of other Am isotopes that contaminate the final product.

  7. Comprehensive appraisal of {sup 239+240}Pu in soils around Rocky Flats, Colorado

    SciTech Connect

    Litaor, M.I.; Allen, L.; Ellerbroek, D.

    1995-12-01

    Plutonium contamination of soils around Rocky Flats Environmental & Technology Site, near Golden, Colorado, resulted from past outdoor storage practices and subsequent remobilization due to inadequate cleanup practices. Until now human-health risk assessment has not been performed because of a lack of sufficient information regarding the spatial extent of {sup 239+240}Pu in soils. The purpose of this work was to elucidate the extent of plutonium contamination in surface soils, and to assess the uncertainty associated with the spatial distribution of {sup 239+240}Pu around Rocky Flats Environmental & Technology Site.

  8. 137Cs and (239+240)Pu levels in the Asia-Pacific regional seas.

    PubMed

    Duran, E B; Povinec, P P; Fowler, S W; Airey, P L; Hong, G H

    2004-01-01

    137Cs and (239+240)Pu data in seawater, sediment and biota from the regional seas of Asia-Pacific extending from 50 degrees N to 60 degrees S latitude and 60 degrees E to 180 degrees E longitude based on the Asia-Pacific Marine Radioactivity Database (ASPAMARD) are presented and discussed. 137Cs levels in surface seawater have been declining to its present median value of about 3 Bq/m3 due mainly to radioactive decay, transport processes, and the absence of new significant inputs. (239+240)Pu levels in surface seawater are much lower, with a median of about 6 mBq/m3. (239+240)Pu appears to be partly scavenged by particles and is therefore more readily transported down the water column. As with seawater, (239+240)Pu concentrations are lower than 137Cs in surface sediment. The median 137Cs concentration in surface sediment is 1.4 Bq/kg dry, while that of (239+240)Pu is only 0.2 Bq/kg dry. The vertical profiles of both 137Cs and (239+240)Pu in the sediment column of coastal areas are different from deep seas which can be attributed to the higher sedimentation rates and additional contribution of run-offs from terrestrial catchment areas in the coastal zone. Comparable data for biota are far less extensive than those for seawater and sediment. The median 137Cs concentration in fish (0.2 Bq/kg wet) is higher than in crustaceans (0.1 Bq/kg wet) or mollusks (0.1 Bq/kg wet). Benchmark values (as of 2001) for 137Cs and (239+240)Pu concentrations in seawater, sediment and biota are established to serve as reference values against which the impact of future anthropogenic inputs can be assessed. ASPAMARD represents one of the most comprehensive compilations of available data on 137Cs and (239+240)Pu in particular, and other anthropogenic as well as natural radionuclides in seawater, sediment and biota from the Asia-Pacific regional seas. PMID:15245845

  9. Reliable determination of 237Np in environmental solid samples using 242Pu as a potential tracer.

    PubMed

    Qiao, Jixin; Hou, Xiaolin; Roos, Per; Miró, Manuel

    2011-04-15

    This paper reports an analytical method for rapid determination of neptunium ((237)Np) in environmental solid samples exploiting automated sequential injection (SI)-based anion exchange separation. Pivotal issues on analytical method performance were investigated including sorption behavior of (237)Np onto various AG 1-type anion exchangers; suitability of (242)Pu as a tracer for (237)Np determination in environmental solid samples; and long-term chemical stability of tetravalent Np. Experimental results revealed that the degree of resin cross-linking has a significant influence on the separation efficiency in terms of chemical yields of (237)Np and removal of interfering nuclides. Although ca. 30% of sorbed Np onto AG 1- × 4 was stripped out during HCl rinsing step for the removal of Th, chemical yield ratios of (237)Np to (242)Pu were proven steady with an average value of 0.67 ± 0.04 (n=15) under selected experimental conditions. Disulfite-8M HNO(3) was selected as a redox pair for valence adjustment to Np(IV) and the tetravalent Np in the sample solution was demonstrated to be stabilized for up to 5 days under 3°C. The analytical results for reference materials showed a good agreement with the expected values, thereby demonstrating the usefulness of (242)Pu as a non-isotopic tracer for (237)Np chemical yield monitoring. The on-column separation procedure fosters rapid analysis as required in emergency situations since each individual sample can be handled within 2.5h, and leads to a significant decrease in labor intensity compared to conventional batch-wise protocols. PMID:21376978

  10. Room-temperature electron spectroscopy of 239Pu and 240Pu

    NASA Astrophysics Data System (ADS)

    Ahmad, I.; Kondev, F. G.; Greene, J. P.; Zhu, S.

    2015-06-01

    Passivated, implanted, planar silicon (PIPS) detectors have been used for the measurement of electron spectra. The commercially available PIPS detectors, available in thicknesses of 100 μm, 300 μm, and 500 μm, have an energy resolution (FWHM) of ~ 2.2 keV, which is essentially the same as that of PIN diodes. Alpha and electron spectra of mass-separated 239Pu and 240Pu sources have been measured with a 300-μm thick PIPS detector and the electron to alpha ratios for the conversion lines of the 51.62- and 45.24-keV transitions have been determined. A procedure has been developed to determine the amount of 239Pu and 240Pu in a mixed source. The α-particle emission rate of the mixed source is measured, which is the sum of individual rates. From the electron spectrum of the mixed source, measured with the same setup as the alpha spectrum, the rates of 239Pu electron lines are determined. Using the electron rate of the 239Pu line and the electron to alpha ratio measured for the pure source, the α-particle emission rate of 239Pu is determined. The difference from the total α-particle emission rate gives the α-particle emission rate of 240Pu. In addition, electron intensities and conversion coefficients of the 239Pu and 240Pu transitions have been measured.

  11. Presence of plutonium isotopes, 239Pu and 240Pu, in soils from Chile

    NASA Astrophysics Data System (ADS)

    Chamizo, E.; García-León, M.; Peruchena, J. I.; Cereceda, F.; Vidal, V.; Pinilla, E.; Miró, C.

    2011-12-01

    Plutonium is present in every environmental compartment, due to a variety of nuclear activities. The Southern Hemisphere has received about 20% of the global 239Pu and 240Pu environmental inventory, with an important contribution of the so-called tropospheric fallout from both the atmospheric nuclear tests performed in the French Polynesia and in Australia by France and United Kingdom, respectively. In this work we provide new data on the impact of these tests to South America through the study of 239Pu and 240Pu in soils from different areas of Northern, Central and Southern Chile. The obtained results point out to the presence of debris from the French tests in the 20-40° Southern latitude range, with 240Pu/ 239Pu atomic ratios quite heterogeneous and ranging from 0.02 to 0.23. They are significantly different from the expected one for the global fallout in the Southern Hemisphere for the 30-53°S latitude range (0.185 ± 0.047), but they follow the same trend as the reported values by the Department of Energy of United States for other points with similar latitudes. The 239 + 240Pu activity inventories show as well a wider variability range in that latitude range, in agreement with the expected heterogeneity of the contamination.

  12. A multi-radionuclide approach to evaluate the suitability of (239+240)Pu as soil erosion tracer.

    PubMed

    Meusburger, Katrin; Mabit, Lionel; Ketterer, Michael; Park, Ji-Hyung; Sandor, Tarjan; Porto, Paolo; Alewell, Christine

    2016-10-01

    Fallout radionuclides have been used successfully worldwide as tracers for soil erosion, but relatively few studies exploit the full potential of plutonium (Pu) isotopes. Hence, this study aims to explore the suitability of the plutonium isotopes (239)Pu and (240)Pu as a method to assess soil erosion magnitude by comparison to more established fallout radionuclides such as (137)Cs and (210)Pbex. As test area an erosion affected headwater catchment of the Lake Soyang (South Korea) was selected. All three fallout radionuclides confirmed high erosion rates for agricultural sites (>25tha(-1)yr(-1)). Pu isotopes further allowed determining the origin of the fallout. Both (240)Pu/(239)Pu atomic ratios and (239+240)Pu/(137)Cs activity ratios were close to the global fallout ratio. However, the depth profile of the (239+240)Pu/(137)Cs activity ratios in undisturbed sites showed lower ratios in the top soil increments, which might be due to higher migration rates of (239+240)Pu. The activity ratios further indicated preferential transport of (137)Cs from eroded sites (higher ratio compared to the global fallout) to the depositional sites (smaller ratio). As such the (239+240)Pu/(137)Cs activity ratio offered a new approach to parameterize a particle size correction factor that can be applied when both (137)Cs and (239+240)Pu have the same fallout source. Implementing this particle size correction factor in the conversion of (137)Cs inventories resulted in comparable estimates of soil loss for (137)Cs and (239+240)Pu. The comparison among the different fallout radionuclides highlights the suitability of (239+240)Pu through less preferential transport compared to (137)Cs and the possibility to gain information regarding the origin of the fallout. In conclusion, (239+240)Pu is a promising soil erosion tracer, however, since the behaviour i.e. vertical migration in the soil and lateral transport during water erosion was shown to differ from that of (137)Cs, there is a clear

  13. New measurement of the 242Pu(n,γ) cross section at n_TOF

    NASA Astrophysics Data System (ADS)

    Lerendegui-Marco, J.; Guerrero, C.; Cortés-Giraldo, M. A.; Quesada, J. M.; Mendoza, E.; Cano-Ott, D.; Eberhardt, K.; Junghans, A.

    2016-03-01

    The use of MOX fuel (mixed-oxide fuel made of UO2 and PuO2) in nuclear reactors allows substituting a large fraction of the enriched Uranium by Plutonium reprocessed from spent fuel. With the use of such new fuel composition rich in Pu, a better knowledge of the capture and fission cross sections of the Pu isotopes becomes very important. In particular, a new series of cross section evaluations have been recently carried out jointly by the European (JEFF) and United States (ENDF) nuclear data agencies. For the case of 242Pu, the two only neutron capture time-of-flight measurements available, from 1973 and 1976, are not consistent with each other, which calls for a new time-of flight capture cross section measurement. In order to contribute to a new evaluation, we have perfomed a neutron capture cross section measurement at the n_TOF-EAR1 facility at CERN using four C6D6 detectors, using a high purity target of 95 mg. The preliminary results assessing the quality and limitations (background, statistics and γ-flash effects) of this new experimental data are presented and discussed, taking into account that the aimed accuracy of the measurement ranges between 7% and 12% depending on the neutron energy region.

  14. Microscopic modeling of mass and charge distributions in the spontaneous fission of 240Pu

    NASA Astrophysics Data System (ADS)

    Sadhukhan, Jhilam; Nazarewicz, Witold; Schunck, Nicolas

    2016-01-01

    We propose a methodology to calculate microscopically the mass and charge distributions of spontaneous fission yields. We combine the multidimensional minimization of collective action for fission with stochastic Langevin dynamics to track the relevant fission paths from the ground-state configuration up to scission. The nuclear potential energy and collective inertia governing the tunneling motion are obtained with nuclear density functional theory in the collective space of shape deformations and pairing. We obtain a quantitative agreement with experimental data and find that both the charge and mass distributions in the spontaneous fission of 240Pu are sensitive both to the dissipation in collective motion and to adiabatic fission characteristics.

  15. Comprehensive appraisal of 239 + 240Pu in soils around Rocky Flats, Colorado.

    PubMed

    Litaor, M I; Ellerbroek, D; Allen, L; Dovala, E

    1995-12-01

    Plutonium contamination of soils around Rocky Flats Environmental & Technology Site, near Golden, Colorado, resulted from past outdoor storage practices and subsequent remobilization due to inadequate cleanup practices. Until now human-health risk assessment has not been performed because of a lack of sufficient information regarding the spatial extent of 239 + 240Pu in soils. The purpose of this work was to elucidate the extent of plutonium contamination in surface soils, and to assess the uncertainty associated with the spatial distribution of 239 + 240Pu around Rocky Flats Environmental & Technology Site. Four data sets were collected or compiled for this investigation: (1) samples collected from 240 plots of 1.01- or 4.05-hectare by compositing 25 evenly-spaced samples from the upper 0.64 cm in each plot; (2) samples collected from the upper 5 cm of soil in 167 of the same 240 plots by compositing 10 samples from the center of each plot; (3) historical data compiled from samples collected between 1969 and 1973, considered to be the most indicative of the original release; and (4) the exhaustive data set that contains the samples from 1, 2, and 3 and other published data sets collected between 1974 and 1994. These latter samples varied in depth and method of sampling. Plutonium activity reported in the exhaustive data set ranged from 0.03 Bq kg-1 to 407,000 Bq kg-1 with a mean of 1,443 Bq kg-1, median of 6.6 Bq kg-1, standard deviation of 18,463 Bq kg-1, and a coefficient of variation of 12.6. The technique of nonparametric indicator kriging was used to model four conditional cumulative distribution functions of 239 + 240Pu in soils around Rocky Flats Environmental & Technology Site. Each of the conditional cumulative distribution functions was used to generate an E-type (mean of the conditional cumulative distribution functions) surface. The resulted surfaces were consistent with the hypothesis that the westerly winds were the dominant mechanism of plutonium

  16. Suitability of 239+240Pu and 137Cs as tracers for soil erosion assessment in Swiss mountain grasslands

    NASA Astrophysics Data System (ADS)

    Alewell, Christine; Meusburger, Katrin; Juretzko, Gregor; Mabit, Lionel; Ketterer, Michael E.

    2014-05-01

    We compare the suitability of the anthropogenic FRNs, 137Cs and 239+240Pu as soil erosion tracers in two alpine valleys of Switzerland (Ursern Valley, Canton Uri, Central Swiss Alps and Val Piora, Ticino, Southern Alps). We sampled reference and potentially erosive sites in transects along both valleys. 137Cs measurements of soil samples were done with a Li-drifted Germanium detector and 239+240Pu with ICP-MS. Our data indicates a heterogeneous deposition of the 137Cs, since most of the fallout origins from the Chernobyl April/May 1986 accident, when large parts of the European Alps were still snow-covered. In contrast, 239+240Pu fallout originated mainly from 1950's-1960's atmospheric nuclear weapons tests, resulting in a more homogenous distribution and thus seems to be a more suitable tracer in mountainous grasslands. Soil erosion assessment using 239+240Pu as a tracer pointed to a huge dynamic and high heterogeneity of erosive processes (between sedimentation of 0.9 to 6.4 t ha1yr1 and erosion of 2.3 to 14.1 t ha1yr1 in the Ursern Valley and sedimentation of 0.7 to 77 t ha1yr1 and erosion of 1 to 5.3 t ha1yr1at Val Piora). Our study represents a novel, successful application of 239+240Pu as a tracer of soil erosion in a mountain environment.

  17. 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.

  18. Activity ratios of 137Cs, 90Sr and 239+240Pu in environmental samples.

    PubMed

    Bossew, P; Lettner, H; Hubmer, A; Erlinger, C; Gastberger, M

    2007-01-01

    Both global and Chernobyl fallout have resulted in environmental contamination with radionuclides such as 137Cs, 90Sr and 239+240Pu. In environmental samples, 137Cs and 239+240Pu can be divided into the contributions of either source, if also the isotopes 134Cs and 238Pu are measurable, based on the known isotopic ratios in global and Chernobyl fallout. No analogous method is available for 90Sr. The activity ratios of Sr to Cs and Pu, respectively, are known for the actual fallout mainly from air filter measurements; but due to the high mobility of Sr in the environment, compared to Cs and Pu, these ratios generally do not hold for the inventory many years after deposition. In this paper we suggest a method to identify the mean contributions of global and Chernobyl fallout to total Sr in soil, sediment and cryoconite samples from Alpine and pre-Alpine regions of Austria, based on a statistical evaluation of Sr/Cs/Pu radionuclide activity ratios. Results are given for Sr:Cs, Sr:Pu and Cs:Pu ratios. Comparison with fallout data shows a strong depletion of Sr against Cs and Pu. PMID:17407799

  19. Alpha-particle emission probabilities in the decay of 240Pu.

    PubMed

    Sibbens, G; Pommé, S; Altzitzoglou, T; García-Toraño, E; Janssen, H; Dersch, R; Ott, O; Sánchez, A Martín; Montero, M P Rubio; Loidl, M; Coron, N; de Marcillac, P; Semkow, T M

    2010-01-01

    Sources of enriched (240)Pu were prepared by vacuum evaporation on quartz substrates. High-resolution alpha-particle spectrometry of (240)Pu was performed with high statistical accuracy using silicon detectors and with low statistical accuracy using a bolometer. The alpha-particle emission probabilities of six transitions were derived from the spectra and compared with literature values. Additionally, some alpha-particle emission probabilities were derived from gamma-ray intensity measurements with a high-purity germanium detector. The alpha-particle emission probabilities of the three main transitions at 5168.1, 5123.6 and 5021.2 keV were derived from seven aggregate spectra analysed with five different fit functions and the results were compatible with evaluated data. Two additional weak peaks at 4863.5 and 4492.0 keV were fitted separately, using the exponential of a polynomial function to represent the underlying tailing of the larger peaks. The peak at 4655 keV could not be detected by alpha-particle spectrometry, while gamma-ray spectrometry confirms that its intensity is much lower than expected from literature. PMID:20106670

  20. Precision of gamma-ray measurements of the effective specific power and effective {sup 240}Pu fraction of plutonium

    SciTech Connect

    Sampson, T.E.

    1992-05-01

    This paper uses gamma-ray spectrometry data from replicate measurements on 40 plutonium-bearing samples to examine the repeatability of the effective {sup 240}Pu fraction ({sup 240}Pu{sub eff}) and the effective specific power (P{sub eff}) calculated from the isotopic distribution analyzed with gamma-ray spectrometry codes. The measurements were used to identify the error component arising from repeatability in the determination of the isotopic composition of plutonium in the sample and the contribution of the error component to the uncertainty in total plutonium mass measurements from neutron coincidence counting ({sup 240}Pu{sub eff}) and calorimetry (P{sub eff}). The 40 samples had {sup 240}Pu{sub eff} percentages ranging from 2 to 39% and P{sub eff} values ranging from 2 to 16 mW/g Pu. Four different gamma-ray spectrometry codes (FRAM, MGA, Blue Box, and PUJRC) were used to analyze the data (not all samples were analyzed with each code). All analyses showed that the % relative standard deviation of P{sub eff} was smaller than that of {sup 240}Pu{sub eff}. This result coupled with a cursory examination of uncertainties in coincidence counting of well-characterized samples and water-bath calorimetry errors for the same types of samples lead to the conclusion that smaller uncertainties will be present in the total plutonium mass determined by the combination of calorimetry/gamma-ray spectrometry than in the mass determined by coincidence counting/gamma-ray spectrometry. An additional examination of the biases arising from the {sup 240}Pu correlation used in the gamma-ray spectrometry codes also supported this conclusion. 17 refs.

  1. Plutonium-239, /sup 240/Pu and /sup 210/Po contents of tobacco and cigarette smoke

    SciTech Connect

    Mussalo-Rauhamaa, H.; Jaakkola, T.

    1985-08-01

    The /sup 239/Pu and /sup 240/Pu found in the environment has mainly been produced by atmospheric nuclear tests. The accumulation of fallout Pu in man from inhalation and ingestion and its distribution in the body has previously been studied. Information about the accumulation is needed because of the expanding production of this highly radiotoxic substance. In the present work the Pu content of tobacco and cigarette smoke was determined to evaluate the contribution of smoking to total Pu intake by man. For comparison the /sup 210/Po content of tobacco and smoke were analyzed. The release of /sup 210/Po in tobacco smoke and the radiation dose for man have been widely studied because of the high incidence of lung cancer among smokers.

  2. Induced Fission of ^{240}Pu within a Real-Time Microscopic Framework.

    PubMed

    Bulgac, Aurel; Magierski, Piotr; Roche, Kenneth J; Stetcu, Ionel

    2016-03-25

    We describe the fissioning dynamics of ^{240}Pu from a configuration in the proximity of the outer fission barrier to full scission and the formation of the fragments within an implementation of density functional theory extended to superfluid systems and real-time dynamics. The fission fragments emerge with properties similar to those determined experimentally, while the fission dynamics appears to be quite complex, with many excited shape and pairing modes. The evolution is found to be much slower than previously expected, and the ultimate role of the collective inertia is found to be negligible in this fully nonadiabatic treatment of nuclear dynamics, where all collective degrees of freedom (CDOF) are included (unlike adiabatic treatments with a small number of CDOF). PMID:27058076

  3. Microscopic modeling of mass and charge distributions in the spontaneous fission of 240Pu

    DOE PAGESBeta

    Sandhukhan, Jhilam; Nazarewicz, Witold; Schunck, Nicolas

    2016-01-20

    We propose a methodology to calculate microscopically the mass and charge distributions of spontaneous fission yields. We combine the multidimensional minimization of collective action for fission with stochastic Langevin dynamics to track the relevant fission paths from the ground-state configuration up to scission. The nuclear potential energy and collective inertia governing the tunneling motion are obtained with nuclear density functional theory in the collective space of shape deformations and pairing. As a result, we obtain a quantitative agreement with experimental data and find that both the charge and mass distributions in the spontaneous fission of 240Pu are sensitive both tomore » the dissipation in collective motion and to adiabatic fission characteristics.« less

  4. Induced Fission of 240Pu within a Real-Time Microscopic Framework

    NASA Astrophysics Data System (ADS)

    Bulgac, Aurel; Magierski, Piotr; Roche, Kenneth J.; Stetcu, Ionel

    2016-03-01

    We describe the fissioning dynamics of 240Pu from a configuration in the proximity of the outer fission barrier to full scission and the formation of the fragments within an implementation of density functional theory extended to superfluid systems and real-time dynamics. The fission fragments emerge with properties similar to those determined experimentally, while the fission dynamics appears to be quite complex, with many excited shape and pairing modes. The evolution is found to be much slower than previously expected, and the ultimate role of the collective inertia is found to be negligible in this fully nonadiabatic treatment of nuclear dynamics, where all collective degrees of freedom (CDOF) are included (unlike adiabatic treatments with a small number of CDOF).

  5. 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.

  6. Microscopic Calculation of 240Pu Scission with a Finite-Range Effective Force

    SciTech Connect

    Younes, W; Gogny, D

    2009-05-04

    Hartree-Fock-Bogoliubov calculations of hot fission in {sup 240}Pu have been performed with a newly-implemented code that uses the D1S finite-range effective interaction. The hot-scission line is identified in the quadrupole-octupole-moment coordinate space. Fission-fragment shapes are extracted from the calculations. A benchmark calculation for {sup 226}Th is obtained and compared to results in the literature. In addition, technical aspects of the use of HFB calculations for fission studies are examined in detail. In particular, the identification of scission configurations, the sensitivity of near-scission calculations to the choice of collective coordinates in the HFB iterations, and the formalism for the adjustment of collective-variable constraints are discussed. The power of the constraint-adjustment algorithm is illustrated with calculations near the critical scission configurations with up to seven simultaneous constraints.

  7. ZPR-6 assembly 7 high {sup 240}Pu core experiments : a fast reactor core with mixed (Pu,U)-oxide fuel and a centeral high{sup 240}Pu zone.

    SciTech Connect

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

    2009-02-23

    ZPR-6 Assembly 7 (ZPR-6/7) encompasses a series of experiments performed at the ZPR-6 facility at Argonne National Laboratory in 1970 and 1971 as part of the Demonstration Reactor Benchmark Program (Reference 1). Assembly 7 simulated a large sodium-cooled LMFBR with mixed oxide fuel, depleted uranium radial and axial blankets, and a core H/D near unity. ZPR-6/7 was designed to test fast reactor physics data and methods, so configurations in the Assembly 7 program were as simple as possible in terms of geometry and composition. ZPR-6/7 had a very uniform core assembled from small plates of depleted uranium, sodium, iron oxide, U{sub 3}O{sub 8} and Pu-U-Mo alloy loaded into stainless steel drawers. The steel drawers were placed in square stainless steel tubes in the two halves of a split table machine. ZPR-6/7 had a simple, symmetric core unit cell whose neutronic characteristics were dominated by plutonium and {sup 238}U. The core was surrounded by thick radial and axial regions of depleted uranium to simulate radial and axial blankets and to isolate the core from the surrounding room. The ZPR-6/7 program encompassed 139 separate core loadings which include the initial approach to critical and all subsequent core loading changes required to perform specific experiments and measurements. In this context a loading refers to a particular configuration of fueled drawers, radial blanket drawers and experimental equipment (if present) in the matrix of steel tubes. Two principal core configurations were established. The uniform core (Loadings 1-84) had a relatively uniform core composition. The high {sup 240}Pu core (Loadings 85-139) was a variant on the uniform core. The plutonium in the Pu-U-Mo fuel plates in the uniform core contains 11% {sup 240}Pu. In the high {sup 240}Pu core, all Pu-U-Mo plates in the inner core region (central 61 matrix locations per half of the split table machine) were replaced by Pu-U-Mo plates containing 27% {sup 240}Pu in the plutonium

  8. Analysis of 137Cs and 239,240Pu concentrations in surface waters of the Pacific Ocean

    NASA Astrophysics Data System (ADS)

    Hirose, Katsumi; Aoyama, Michio

    2003-09-01

    Geographical and temporal variations of anthropogenic radionuclides, 137Cs and 239,240Pu, in surface waters of the North Pacific Ocean were studied using the HAM database, which is a comprehensive data set on 137Cs, 239,240Pu, and other anthropogenic radionuclides. The geographical distributions suggest that 137Cs and 239,240Pu concentrations in surface waters of the Pacific Ocean in the 1960s were controlled by global fallout from the 1961-1962 US and former USSR atmospheric nuclear weapons tests. The changes in surface 137Cs concentrations in the Pacific that occurred after 1970 were caused by physical processes. In the 1990s, surface 137Cs showed a homogeneous distribution throughout the Pacific. Biogeochemical and physical processes are important factors controlling surface 239,240Pu concentrations. The time-series data on anthropogenic radionuclides suggest that wind-driven circulation, subduction, and upwelling of Pacific surface and subsurface waters control the geographic distributions of anthropogenic radionuclides and their fates.

  9. Comparative distribution of 241 Am and 239,240 Pu in soils around the Rocky Flats Environmental Technology Site.

    PubMed

    Ibrahim, S A; Schierman, M J; Whicker, F W

    1996-04-01

    The distribution and behavior of 241 Am and 239,240 Pu in soils from the buffer zone of the Rocky Flats Environmental Technology Site have been investigated. Concentrations of both radionuclides decreased at similar rates with soil depth. More than 80% of the total inventory of both contaminants was found in the upper 9 cm of the soils with over 50% of the inventory residing in the top 3 cm. Comparison with earlier studies indicate that the plutonium depth profile has not changed significantly over the last 25 y. The inventories of 241 Am and 239,240 Pu decreased with distance from the 903 Pad (a former waste storage site) according to a power function, and the plume extended mainly toward the east. The lateral movement of the two contaminants away from the 903 Pad was not significantly different. The median activity ratio of 241 Am: 239,240 Pu ranged from 17 to 19% and was independent of sampling location and soil depth. This observation provided further evidence that the movement of both contaminants is indistinguishable in the study area. Because of the strong correlation between the two radionuclides, 241 Am concentrations can then be used to infer 239,240 Pu by counting the 241 Am via gamma spectroscopy. PMID:8617592

  10. Measurement of fallout radionuclides, (239)(,240)Pu and (137)Cs, in soil and creek sediment: Sydney Basin, Australia.

    PubMed

    Smith, B S; Child, D P; Fierro, D; Harrison, J J; Heijnis, H; Hotchkis, M A C; Johansen, M P; Marx, S; Payne, T E; Zawadzki, A

    2016-01-01

    Soil and sediment samples from the Sydney basin were measured to ascertain fallout radionuclide activity concentrations and atom ratios. Caesium-137 ((137)Cs) was measured using gamma spectroscopy, and plutonium isotopes ((239)Pu and (240)Pu) were quantified using accelerator mass spectrometry (AMS). Fallout radionuclide activity concentrations were variable ranging from 0.6 to 26.1 Bq/kg for (137)Cs and 0.02-0.52 Bq/kg for (239+240)Pu. Radionuclides in creek sediment samples were an order of magnitude lower than in soils. (137)Cs and (239+240)Pu activity concentration in soils were well correlated (r(2) = 0.80) although some deviation was observed in samples collected at higher elevations. Soil ratios of (137)Cs/(239+240)Pu (decay corrected to 1/1/2014) ranged from 11.5 to 52.1 (average = 37.0 ± 12.4) and showed more variability than previous studies. (240)Pu/(239)Pu atom ratios ranged from 0.117 to 0.165 with an average of 0.146 (±0.013) and an error weighted mean of 0.138 (±0.001). These ratios are lower than a previously reported ratio for Sydney, and lower than the global average. However, these ratios are similar to those reported for other sites within Australia that are located away from former weapons testing sites and indicate that atom ratio measurements from other parts of the world are unlikely to be applicable to the Australian context. PMID:26344369

  11. Suitability of 239+240Pu and 137Cs as tracers for soil erosion assessment in mountain grasslands.

    PubMed

    Alewell, Christine; Meusburger, Katrin; Juretzko, Gregor; Mabit, Lionel; Ketterer, Michael E

    2014-05-01

    Anthropogenic radionuclides have been distributed globally due to nuclear weapons testing, nuclear accidents, nuclear weapons fabrication, and nuclear fuel reprocessing. While the negative consequences of this radioactive contamination are self-evident, the ubiquitous fallout radionuclides (FRNs) distribution form the basis for the use as tracers in ecological studies, namely for soil erosion assessment. Soil erosion is a major threat to mountain ecosystems worldwide. We compare the suitability of the anthropogenic FRNs, 137Cs and 239+240Pu as soil erosion tracers in two alpine valleys of Switzerland (Urseren Valley, Canton Uri, Central Swiss Alps and Val Piora, Ticino, Southern Alps). We sampled reference and potentially erosive sites in transects along both valleys. 137Cs measurements of soil samples were performed with a Li-drifted Germanium detector and 239+240Pu with ICP-MS. Our data indicates a heterogeneous deposition of the 137Cs, since most of the fallout origins from the Chernobyl April/May 1986 accident, when large parts of the European Alps were still snow-covered. In contrast, 239+240Pu fallout originated mainly from 1950s to 1960s atmospheric nuclear weapons tests, resulting in a more homogenous distribution and thus seems to be a more suitable tracer in mountainous grasslands. Soil erosion assessment using 239+240Pu as a tracer pointed to a huge dynamic and high heterogeneity of erosive processes (between sedimentation of 1.9 and 7 t ha(-1) yr(-1) and erosion of 0.2-16.4 t ha(-1) yr(-1) in the Urseren Valley and sedimentation of 0.4-20.3 t ha(-1) yr(-1) and erosion of 0.1-16.4 t ha(-1) yr(-1) at Val Piora). Our study represents a novel and successful application of 239+240Pu as a tracer of soil erosion in a mountain environment. PMID:24374184

  12. 239,240Pu and inorganic substances in aerosols from the vicinity of a waste isolation pilot plant: the importance of resuspension.

    PubMed

    Arimoto, R; Kirchner, T; Webb, J; Conley, M; Stewart, B; Schoep, D; Walthall, M

    2002-10-01

    Aerosol samples were collected and analyzed to characterize the spatial and temporal variations in the concentrations of plutonium and selected inorganic substances in the atmosphere around the Waste Isolation Pilot Plant (WIPP). High-volume aerosol sampling was conducted at three sites: (1) On Site, (2) Near Field, and (3) Cactus Flats. 239,240Pu was determined by alpha spectrometry following chemical separations; mass loadings were determined gravimetrically. A separate set of low-volume aerosol samples was analyzed for major ions using ion chromatography and for trace elements by inductively-coupled plasma emission spectrometry and mass spectrometry. The average 239,240Pu activity concentrations in total suspended particle (TSP) samples (12 to 16 nBq m(-3)) were consistent with those previously reported, but they varied strongly with season, with the highest values generally in spring. Further, the 239,240Pu activity concentrations were comparable among the three sites, and therefore there was no evidence for elevated 239,240Pu activities due to WIPP operations. The fraction of the 239,240Pu activity concentrations in the PM10, samples (particles less than 10 microm diameter) relative to TSP was lower than the corresponding PM10/TSP ratios of either high-volume mass or several inorganics (sulfate, aluminum or lead), indicating that 239,240Pu tends to be on large particles. Aerosol mass loadings (microg m(-3)) and 239,240Pu activity concentrations were correlated for all sets of samples, but at On Site, the TSP samples showed higher mass to 239,240Pu ratios than the other sites. Thus activities or processes occurring at or near the WIPP site evidently produced aerosols that contributed to the mass loadings but contained less 239,244Pu than ambient aerosols. About 63% of the variability in 239,240Pu activity concentrations was explained by wind travel, sampling location, length of the sampling interval, and aerosol mass. 239,240Pu activity concentrations also were

  13. Experimental values for 241Am and 239+240Pu Kd's in French agricultural soils.

    PubMed

    Roussel-Debet, Sylvie

    2005-01-01

    Experiments resulted in determination of K(d) values for (241)Am and (239+240)Pu in 6 soils whose characteristics are representative of agricultural soils found around French nuclear power plant sites. These experiments were conducted in stirred batch reactors and the sorption isotherms were plotted. For americium, the experimental K(d) values varied from 60 to 4000 Lkg(-1) (d.w.) and correlated well with soil pH, K(d) increased with increasing pH. As regards plutonium, the experimental K(d) values varied between 300 and 9600 Lkg(-1) and decreased with increasing total sand content. The estimation of the total residence time determined by using a particular and experimentally refined value for K(d)-with a model similar to those currently used for impact assessments-illustrates the importance of establishing values that are better suited to specific soils than generic values. Lastly, depending on the type of evaluation envisioned, it might be important to look for a specific value of K(d)-and even modelling-more suited to the specificity of the scenario studied, by performing more complex, or even in situ, experiments. PMID:15603906

  14. Radioecologycal study of {sup 239/240}Pu in Bangka Island and Muria Peninsula: Determination of {sup 239/240}Pu in marine sediment and seawater as part of baseline data collecting for sitting of candidates of first Indonesia NPP

    SciTech Connect

    Suseno, Heny; Wisnubroto, Djarot S.

    2014-03-24

    Radioisotope Pu-239/240 are alpha emitting nuclides important indicators of radioactive contamination of the marine environment. Global fallout is the main source of plutonium in the marine environment. There are very limited study on {sup 239/240}Pu in Indonesia coastal environments. The data of this radioisotopes is needed for baseline data of nuclear power plant (NPP) site candidates both in Bangka Island and Muria Peninsula. Bottom sediments play an important role in radioecological studies of the marine environment because a large proportion of radioactive substances entering the sea is adsorbed over time onto suspended particulate matter and deposited in sediments. Plutonium is particle reactive and deposited in marine sediment. Radioisotope {sup 239/240}Pu was determinated by alpha spectrometry after radiochemical procedure that was performed in both water and marine sediment from Bangka Island and Muria Peninsula. The sediment baseline of concentration {sup 239/240}Pu in Bangka Island and Muria Peninsula were range from 0.013 to 0.021 Bq.kg{sup −1} and 0.018 to 0.024 Bq.kg{sup −1} respectively. The water baseline concentration this isotope were range from 2.73 to 4.05 mBq.m{sup −3} and 2.98 to 4.50 mBq.m{sup −3}.

  15. Towards high accurate neutron-induced fission cross sections of 240,242Pu: Spontaneous fission half-lives

    NASA Astrophysics Data System (ADS)

    Salvador-Castiñeira, P.; Bryś, T.; Eykens, R.; Hambsch, F.-J.; Moens, A.; Oberstedt, S.; Pretel, C.; Sibbens, G.; Vanleeuw, D.; Vidali, M.

    2013-12-01

    Fast spectrum neutron-induced fission cross sections of transuranic isotopes are being of special demand in order to provide accurate data for the new GEN-IV nuclear power plants. To minimize the uncertainties on these measurements accurate data on spontaneous fission half-lives and detector efficiencies are a key point. High α-active actinides need special attention since the misinterpretation of detector signals can lead to low efficiency values or underestimation in fission fragment detection. In that context, 240,242Pu isotopes have been studied by means of a Twin Frisch-Grid Ionization Chamber (TFGIC) for measurements of their neutron-induced fission cross section. Gases with different drift velocities have been used, namely P10 and CH4. The detector efficiencies for both samples have been determined and improved spontaneous fission half-life values were obtained.

  16. The depth distribution of sup 90 Sr, sup 137 Cs, and sup 239,240 Pu in soil profile samples

    SciTech Connect

    Price, K.R.

    1989-04-01

    A special study was conducted at the Hanford Site and vicinity to investigate the depth distribution of {sup 90}Sr, {sup 137}Cs, and {sup 239,240}Pu in soil at two locations. Duplicate sets of samples were collected at each location from the soil surface to a depth of 30 cm in increments of 2.5 cm. Results from an onsite location near a retired nuclear fuel reprocessing facility were compared to results from a background location upwind and distant from the Site. The study showed that, regardless of location, the top 5 cm of soil contained 51 to 74% of the {sup 90}Sr, 99% of the {sup 137}Cs, and 96% of the {sup 239,240}Pu. Soil at the background location received radionuclides only from deposition of worldwide fallout, and averaged 1.6 pCi/cm{sup 2} of {sup 90}Sr, 3.0 pCi/cm{sup 2} of {sup 137}Cs, and 0.071 pCi/cm{sup 2} of {sup 239,240}Pu. Soil at the onsite location received radionuclides from deposition of both worldwide fallout and past operations of the retired fuel reprocessing facility and contained 4 times as much {sup 90}Sr, 5 times as much {sup 137}Cs, and 44 times as much {sup 239,240}Pu as the background location. (Pacific Northwest Laboratory is operated for the US Department of Energy by Battelle Memorial Institute under Contract AC06-76RLO1830.) 8 refs., 2 figs.

  17. Numerical simulation of 137Cs and (239,240)Pu concentrations by an ocean general circulation model.

    PubMed

    Tsumune, Daisuke; Aoyama, Michio; Hirose, Katsumi

    2003-01-01

    We simulated the spatial distributions and the temporal variations of 137Cs and (239,240)Pu concentrations in the ocean by using the ocean general circulation model which was developed by National Center of Atmospheric Research. These nuclides are introduced into seawaters from global fallout due to atmospheric nuclear weapons tests. The distribution of radioactive deposition on the world ocean is estimated from global precipitation data and observed values of annual deposition of radionuclides at the Meteorological Research Institute in Japan and several observed points in New Zealand. Radionuclides from global fallout have been transported by advection, diffusion and scavenging, and this concentration reduces by radioactive decay in the ocean. We verified the results of the model calculations by comparing simulated values of 137Cs and (239,240)Pu in seawater with the observed values included in the Historical Artificial Radionuclides in the HAM database, which has been constructed by the Meteorological Research Institute. The vertical distributions of the calculated 137Cs concentrations were in good agreement and are in good agreement with the observed profiles in the 1960s up to 250 m, in the 1970s up to 500 m, in the 1980s up to 750 m and in the 1990s up to 750 m. However, the calculated 137Cs concentrations were underestimated compared with the observed 137Cs at the deeper layer. This may suggest other transport processes of 137Cs to deep waters. The horizontal distributions of 137Cs concentrations in surface water could be simulated. A numerical tracer release experiment was performed to explain the horizontal distribution pattern. A maximum (239,240)Pu concentration layer occurs at an intermediate depth for both observed and calculated values, which is formed by particle scavenging. The horizontal distributions of the calculated (239,240)Pu concentrations in surface water could be simulated by considering the scavenging effect. PMID:12860090

  18. Pu-239 and Pu-240 inventories and Pu-240/ Pu-239 atom ratios in the water column off Sanriku, Japan.

    NASA Astrophysics Data System (ADS)

    Yamada, Masatoshi; Zheng, Jian; Aono, Tatsuo

    2013-04-01

    A magnitude 9.0 earthquake and subsequent tsunami occurred in the Pacific Ocean off northern Honshu, Japan, on 11 March 2011 which caused severe damage to the Fukushima Dai-ichi Nuclear Power Plant. This accident has resulted in a substantial release of radioactive materials to the atmosphere and ocean, and has caused extensive contamination of the environment. However, no information is available on the amounts of radionuclides such as Pu isotopes released into the ocean at this time. Investigating the background baseline concentration and atom ratio of Pu isotopes in seawater is important for assessment of the possible contamination in the marine environment. Pu-239 (half-life: 24,100 years), Pu-240 (half-life: 6,560 years) and Pu-241 (half-life: 14.325 years) mainly have been released into the environment as the result of atmospheric nuclear weapons testing. The atom ratio of Pu-240/Pu-239 is a powerful fingerprint to identify the sources of Pu in the ocean. The Pu-239 and Pu-240 inventories and Pu-240/Pu-239 atom ratios in seawater samples collected in the western North Pacific off Sanriku before the accident at Fukushima Dai-ichi Nuclear Power Plant will provide useful background baseline data for understanding the process controlling Pu transport and for distinguishing additional Pu sources. Seawater samples were collected with acoustically triggered quadruple PVC sampling bottles during the KH-98-3 cruise of the R/V Hakuho-Maru. The Pu-240/Pu-239 atom ratios were measured with a double-focusing SF-ICP-MS, which was equipped with a guard electrode to eliminate secondary discharge in the plasma and to enhance overall sensitivity. The Pu-239 and Pu-240 concentrations were 2.07 and 1.67 mBq/m3 in the surface water, respectively, and increased with depth; a subsurface maximum was identified at 750 m depth, and the concentrations decreased with depth, then increased at the bottom layer. The total Pu-239+240 inventory in the entire water column (depth interval 0

  19. Characterization of ^{239,240}Pu Radionuclide Adsorption to Soil Particles and Mineral Dust Aerosols

    NASA Astrophysics Data System (ADS)

    Tatro, D. P.; Arimoto, R.; McMillan, N. J.; Barnes, M.

    2006-12-01

    The release of ^{239,240}Pu into the environment by nuclear weapons testing 50 years ago initiated the cyclic mobilization of Pu-contaminated soil particles via the resuspension of dust resulting in a widespread distribution of Pu and other radionuclides. It is unclear what enables the aeolian transport of Pu in the environment; plausible hypotheses of Pu binding to dust and soil particles include Pu adsorption to iron oxides/hydroxides, organic acids, or silicate minerals such as clays. To investigate the connections between surface soils, dust and radionuclides, samples of soil and/or dust were collected from the Project Gnome Site in Eddy County, NM, the Jemez Mountains near Los Alamos, NM, and two 50-year old attics and wind-blown dust in Big Spring, TX. This study tests the hypothesis that Pu is adsorbed onto Fe oxides and hydroxides that coat dust/soil particles. The samples are generally low in organic carbon (0.2 - 4.8%, except for the unburned Los Alamos sample at 9.4%), as measured by LOI (Loss On Ignition) at 360 °C. The citrate-bicarbonate-dithionite method (CDB) of Fe oxide removal, first proposed by Mehra and Jackson in 1960, was used to selectively extract Fe oxides from the samples while leaving silicate Fe intact. Chemical digestion of each sample creates two fractions, the extracted supernatant and a solid pellet residue. If the Pu were associated with Fe oxides, then Fe and Pu should both be selectively removed from the bulk sample during the CBD process, leaving the pellet depleted in Fe and Pu and the supernatant enriched. For Fe, this was confirmed by scanning electron microscope and petrographic analyses. Preliminary radiochemical analyses of Pu activity also verify this hypothesis. Pu activity is significantly lower in pellets than bulk samples (Pu activitypellet/Pu activitybulk average = 0.07, range 0.02-0.12); Pu activity in supernatants is significantly higher than in bulk samples (Pu activitysupernatant/Pu activitybulk average = 4

  20. 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

  1. 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.

  2. Comparison of 241Am, (239,240)Pu and 137Cs concentrations in soil around rocky flats.

    PubMed

    Hulse, S E; Ibrahim, S A; Whicker, F W; Chapman, P L

    1999-03-01

    Gamma spectroscopy measurements were used to estimate concentrations of 241Am and 137Cs in soil profiles to depths of 21 cm at on-site and off-site locations around the Rocky Flats Environmental Technology Site and at regional background locations east of the Front Range between Colorado's borders with New Mexico and Wyoming. Concentrations of these radionuclides were compared with concentrations of (239,240)Pu in the same samples. Concentrations of 241Am in soil from depths of 0 to 3 cm decreased in an easterly direction from more than 5.3 kBq kg(-1) near the 903 pad to background levels of 1.3 Bq kg(-1) 5 to 7 km away at a rate that was nearly proportional to the inverse square of distance. Deposits of 137Cs were ubiquitous, averaging 0.12 kBq kg(-1) in soil from depths of 0 to 3 cm, but were unevenly distributed around Rocky Flats and the regional background locations. Deviations from the uniform exponential rate at which soil concentrations of 137Cs typically decreased with depth, -0.25 cm(-1) at undisturbed sites, enabled us to determine that about 10% of our sampling sites had been disturbed by erosion, tillage, or other factors. The mean rate at which (239,240)Pu decreased with depth was about the same, -0.23 cm(-1), throughout the study area. Soil concentrations of 241Am decreased with depth at a similar mean rate of -0.22 cm(-1) at locations close to the 903 pad where measurements were robust. Ratios between 241Am or (239,240)Pu and 137Cs proved more useful for delineating the extent and pattern of contamination from Rocky Flats than did activity concentrations in soil. PMID:10025653

  3. Comparison of {sup 241}Am, {sup 239,240}Pu, and {sup 137}Cs concentrations in soil around Rocky Flats

    SciTech Connect

    Hulse, S.E.; Ibrahim, S.A.; Whicker, F.W.; Chapman, P.L.

    1999-03-01

    Gamma spectroscopy measurements were used to estimate concentrations of {sup 241}Am and {sup 137}Cs in soil profiles to depths of 21 cm at on-site and off-site locations around the Rocky Flats Environmental Technology Site and at regional background locations east of the Front Range between Colorado`s borders with New Mexico and Wyoming. Concentrations of these radionuclides were compared with concentrations of {sup 239,240}Pu in the same samples. Concentrations of {sup 241}Am in soil from depths of 0 to 3 cm decreased in an easterly direction from more than 5.3 kBq kg{sup {minus}1} 5 to 7 km away at a rate that was nearly proportional to the inverse square of distance. Deposits of {sup 137}Cs were ubiquitous, averaging 0.12 kBq kg{sup {minus}1} in soil from depths of 0 to 3 cm, but were unevenly distributed around Rocky Flats and the regional background locations. Deviations from the uniform exponential rate at which soil concentrations of {sup 137}Cs typically decreased with depth, {minus}0.25 cm{sup {minus}1} at undisturbed sites, enabled the authors to determine that about 10% of their sampling sites had been disturbed by erosion, tillage, or other factors. The mean rate at which {sup 239,240}Pu decreased with depth was about the same, {minus}0.23 cm{sup {minus}1}, throughout the study area. Soil concentrations of {sup 241}Am decreased with depth at a similar mean rate of {minus}0.22 cm{sup {minus}1} at locations close to the 903 pad where measurements were robust. Ratios between {sup 241}Am or {sup 239,240}Pu and {sup 137}Cs proved more useful for delineating the extent and pattern of contamination from Rocky Flats than did activity concentrations in soil.

  4. Transport of 137Cs and 239,240Pu with ice-rafted debris in the Arctic Ocean

    USGS Publications Warehouse

    Landa, E.R.; Reimnitz, E.; Beals, D.M.; Pochkowski, J.M.; Winn, W.G.; Rigor, I.

    1998-01-01

    Ice rafting is the dominant mechanism responsible for the transport of fine-grained sediments from coastal zones to the deep Arctic Basin. Therefore, the drift of ice-rafted debris (IRD) could be a significant transport mechanism from the shelf to the deep basin for radionuclides originating from nuclear fuel cycle activities and released to coastal Arctic regions of the former Soviet Union. In this study, 28 samples of IRD collected from the Arctic ice pack during expeditions in 1989-95 were analyzed for 137Cs by gamma spectrometry and for 239Pu and 240Pu by thermal ionization mass spectrometry. 137Cs concentrations in the IRD ranged from less than 0.2 to 78 Bq??kg-1 (dry weight basis). The two samples with the highest 137Cs concentrations were collected in the vicinity of Franz Josef Land, and their backward trajectories suggest origins in the Kara Sea. Among the lowest 137Cs values are seven measured on sediments entrained on the North American shelf in 1989 and 1995, and sampled on the shelf less than six months later. Concentrations of 239Pu + 240Pu ranged from about 0.02 to 1.8 Bq??kg-1. The two highest values came from samples collected in the central Canada Basin and near Spitsbergen; calculated backward trajectories suggest at least 14 years of circulation in the Canada Basin in the former case, and an origin near Severnaya Zemlya (at the Kara Sea/Laptev Sea boundary) in the latter case. While most of the IRD samples showed 240Pu/239Pu ratios near the mean global fallout value of 0.185, five of the samples had lower ratios, in the 0.119 to 0.166 range, indicative of mixtures of Pu from fallout and from the reprocessing of weapons-grade Pu. The backward trajectories of these five samples suggest origins in the Kara Sea or near Severnaya Zemlya.

  5. 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).

  6. Migration of (137)Cs, (90)Sr, and (239+240)Pu in Mediterranean forests: influence of bioavailability and association with organic acids in soil.

    PubMed

    Guillén, J; Baeza, A; Corbacho, J A; Muñoz-Muñoz, J G

    2015-06-01

    The understanding of downward migration of anthropogenic radionuclides in soil is a key factor in the assessment of their environmental behavior. There are several factors that can affect this process, such as the radionuclide source, their chemical form, soil and environmental characteristics, etc. Two Mediterranean pinewood ecosystems in Spain, which were affected mainly by global fallout, were selected to assess the migration of (137)Cs, (90)Sr, and (239+240)Pu. Using auxiliary modeling (diffusion-convection equation and compartmental model), it followed from field observations that the migration velocities of (90)Sr and (239+240)Pu were similar and higher than that of (137)Cs. The downward migration of radionuclides can be considered a consequence of their association with soil particles. A sequential speciation procedure also confirmed that (90)Sr was the most bioavailable radionuclide followed by (239+240)Pu and (137)Cs. Although this can explain the different velocity of (90)Sr and (137)Cs, bioavailability could not explain by itself the similar velocities of (239+240)Pu and (90)Sr. The presence of organic acids in the soil can also influence the migration of radionuclides attached to them, which decreased in the order: (239+240)Pu > (90)Sr > (137)Cs. Thus, the joint consideration of bioavailable and humic + fulvic acid fractions can explain the observed differences in the downward velocities. PMID:25827576

  7. Distribution and source of (129)I, (239)(,240)Pu, (137)Cs in the environment of Lithuania.

    PubMed

    Ežerinskis, Ž; Hou, X L; Druteikienė, R; Puzas, A; Šapolaitė, J; Gvozdaitė, R; Gudelis, A; Buivydas, Š; Remeikis, V

    2016-01-01

    Fifty five soil samples collected in the Lithuania teritory in 2011 and 2012 were analyzed for (129)I, (137)Cs and Pu isotopes in order to investigate the level and distribution of artificial radioactivity in Lithuania. The activity and atomic ratio of (238)Pu/((239,24)0)Pu, (129)I/(127)I and (131)I/(137)Cs were used to identify the origin of these radionuclides. The (238)Pu/(239+240)Pu and (240)Pu/(239)Pu ratios in the soil samples analyzed varied in the range of 0.02-0.18 and 0.18-0.24, respectively, suggesting the global fallout as the major source of Pu in Lithuania. The values of 10(-9) to 10(-6) for (129)I/(127)I atomic ratio revealed that the source of (129)I in Lithuania is global fallout in most cases though several sampling sites shows a possible impact of reprocessing releases. Estimated (129)I/(131)I ratio in soil samples from the southern part of Lithuania shows negligible input of the Chernobyl fallout. No correlation of the (137)Cs and Pu isotopes with (129)I was observed, indicating their different sources terms. Results demonstrate uneven distribution of these radionuclides in the Lithuanian territory and several sources of contamination i.e. Chernobyl accident, reprocessing releases and global fallout. PMID:26476410

  8. 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.

  9. References to Studies of 137Cs, 90Sr and 239+240Pu in the Pacific Ocean a Bibliography

    SciTech Connect

    Noshkin, V.E.

    2001-02-01

    This report contains a listing of publications known to this author on reported concentrations, reviews and discussions of {sup 137}Cs, {sup 90}Sr and {sup 239+240}Pu in seawater, sediment and the biota from parts of the North and South Pacific Ocean. Each reference has been assigned an accession number consisting of the first three letters of the first author's last name followed by the first letter of the first name, the year of the publication and an assigned number. Studies in both the coastal areas and the open ocean are included as well as those providing data within lagoons of coral atolls. Some references to the radionuclides in the Indian Ocean are also provided.

  10. Measurement of 240Pu/239Pu isotopic ratios in soils from the Marshall Islands using ICP-MS.

    PubMed

    Muramatsu, Y; Hamilton, T; Uchida, S; Tagami, K; Yoshida, S; Robison, W

    2001-10-20

    Nuclear weapons tests conducted by the United States in the Marshall Islands produced significant quantities of regional or tropospheric fallout contamination. Here we report on some preliminary inductively coupled plasma-mass spectrometry (ICP-MS) measurements of plutonium isolated from seven composite soil samples collected from Bikini, Enewetak and Rongelap Atolls in the northern Marshall Islands. These data show that 240Pu/239Pu isotopic signatures in surface soils from the Marshall Island vary significantly and could potentially be used to help quantify the range and extent of fallout deposition (and associated impacts) from specific weapons tests. 137Cs and 60Co were also determined on the same set of soil samples for comparative purposes. PMID:11669263

  11. A comparative study of (239,240)Pu in soil near the former Rocky Flats Nuclear Weapons Facility, Golden, CO.

    PubMed

    Margulies, Todd D; Schonbeck, Niels D; Morin-Voillequé, Normie C; James, Katherine A; LaVelle, James M

    2004-01-01

    The Rocky Flats Nuclear Weapons Plant near Golden, CO released plutonium into the environment during almost 40 years of operation. Continuing concern over possible health impacts of these releases has been heightened by lack of public disclosure of the US Department of Energy (DOE) activities. A dose reconstruction study for the Rocky Flats facilities, begun in 1990, provided a unique opportunity for concerned citizens to design and implement field studies without participation of the DOE, its contractors, or other government agencies. The Citizens Environmental Sampling Committee was formed in late 1992 and conducted a field sampling program in 1994. Over 60 soil samples, including both surface and core samples, were collected from 28 locations where past human activities would have minimal influence on contaminant distributions in soil. Cesium-137 activity was used as a means to assess whether samples were collected in undisturbed locations. The distribution of plutonium (as (239,240)Pu) in soil was consistent with past sampling conducted by DOE, the Colorado Department of Public Health and Environment, and others. Elevated levels of (239,240)Pu were found immediately east of the Rocky Flats Plant, with concentrations falling rapidly with distance from the plant to levels consistent with background from fallout. Samples collected in areas south, west, and north of the plant were generally consistent with background from fallout. No biases in past sampling due to choice of sampling locations or sampling methodology were evident. The study shows that local citizens, when provided sufficient resources, can design and implement technical studies that directly address community concerns where trust in the regulated community and/or regulators is low. PMID:15172724

  12. Bioturbation depths, rates and processes in Massachusetts Bay sediments inferred from modeling of 210Pb and 239 + 240Pu profiles

    USGS Publications Warehouse

    Crusius, John; Bothner, Michael H.; Sommerfield, Christopher K.

    2004-01-01

    Profiles of 210Pb and 239 + Pu from sediment cores collected throughout Massachusetts Bay (water depths of 36-192 m) are interpreted with the aid of a numerical sediment-mixing model to infer bioturbation depths, rates and processes. The nuclide data suggest extensive bioturbation to depths of 25-35 cm. Roughly half the cores have 210Pb and 239 + 240Pu profiles that decrease monotonically from the surface and are consistent with biodiffusive mixing. Bioturbation rates are reasonably well constrained by these profiles and vary from ~0.7 to ~40 cm2 yr-1. As a result of this extensive reworking, however, sediment ages cannot be accurately determined from these radionuclides and only upper limits on sedimentation rates (of ~0.3 cm yr-1) can be inferred. The other half of the radionuclide profiles are characterized by subsurface maxima in each nuclide, which cannot be reproduced by biodiffusive mixing models. A numerical model is used to demonstrate that mixing caused by organisms that feed at the sediment surface and defecate below the surface can cause the subsurface maxima, as suggested by previous work. The deep penetration depths of excess 210Pb and 239 + 240Pu suggest either that the organisms release material over a range of >15 cm depth or that biodiffusive mixing mediated by other organisms is occurring at depth. Additional constraints from surficial sediment 234Th data suggest that in this half of the cores, the vast majority of the present-day flux of recent, nuclide-bearing material to these core sites is transported over a timescale of a month or more to a depth of a few centimeters below the sediment surface. As a consequence of the complex mixing processes, surface sediments include material spanning a range of ages and will not accurately record recent changes in contaminant deposition.

  13. Determination of (241)Pu by the method of disturbed radioactive equilibrium using 2πα-counting and precision gamma-spectrometry.

    PubMed

    Alekseev, I; Kuzmina, T

    2016-04-01

    A simple technique is proposed for the determination of the content of (241)Pu, which is based on disturbance of radioactive equilibrium in the genetically related (237)U←(241)Pu→(241)Am decay chain of radionuclides, with the subsequent use of 2πα-counting and precision gamma-spectroscopy for monitoring the process of restoration of that equilibrium. It has been shown that the data on dynamics of accumulation of the daughter (241)Am, which were obtained from the results of measurements of α- and γ-spectra of the samples, correspond to the estimates calculated for the chain of two genetically related radionuclides, the differences in the estimates of (241)Pu radioactivity not exceeding 2%. Combining the different methods of registration (2πα-counting, semiconductor alpha- and gamma-spectrometry) enables the proposed method to be efficiently applied both for calibration of (241)Pu-sources (from several hundreds of kBq and higher) and for radioisotopic analysis of plutonium mixtures. In doing so, there is a deep purification of (241)Pu from its daughter decay products required due to unavailability of commercial detectors that could make it possible, based only on analysis of alpha-spectra, to conduct quantitative analysis of the content of (238)Pu and (241)Am. PMID:26868275

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

    SciTech Connect

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

    2011-01-01

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

  15. Use of anthropogenic radioisotopes to estimate rates of soil redistribution by wind II: The potential for future use of 239+240Pu

    NASA Astrophysics Data System (ADS)

    Van Pelt, R. Scott; Ketterer, Michael E.

    2013-06-01

    In the previous paper, the use of soilborne 137Cs from atmospheric fallout to estimate rates of soil redistribution, particularly by wind, was reviewed. This method relies on the assumption that the source of 137Cs in the soil profile is from atmospheric fallout following the period of atmospheric weapons testing so that the temporal and, to a certain extent, the spatial patterns of 137Cs deposition are known. One of the major limitations occurs when local or regional sources of 137Cs contamination mask the pulse from global fallout, making temporal estimates of redistribution difficult or impossible. Like 137Cs, Pu exhibits strong affinity for binding to soil particle surfaces, and therefore, re-distribution of Pu inventory indicates inferred soil re-distribution. Compared to 137Cs, 239Pu and 240Pu offer several important advantages: (a) the two major Pu isotopes have much longer half-lives than 137Cs and (b) the ratio 240Pu/239Pu is used to examine whether the Pu is from stratospheric fallout. In this paper, we review the literature concerning Pu in soil and of current attempts to use this tracer to estimate rates of soil redistribution. We also present preliminary, unpublished data from a pilot study designed to test whether or not 239+240Pu can be used to estimate rates of soil redistribution by wind. Based on similarities of profile distribution and relative inventories between 137Cs measurements and 239+240Pu measurements of split samples from a series of fields with documented wind erosion histories, we conclude that 239+240Pu may well be the anthropogenic radioisotope of choice for future soil redistribution investigations.

  16. Transfer of aged 239+240Pu, 238Pu, 241Am, and 137Cs to cattle grazing a contaminated arid environment.

    PubMed

    Gilbert, R O; Engel, D W; Anspaugh, L R

    1989-09-01

    In this paper, estimates are obtained of the fraction of ingested 239+240Pu, 238Pu, 241Am and 137Cs transferred to blood, muscle, liver, kidney, femur, vertebra, and gonads of a reproducing herd of 17 beef cattle, individuals of which grazed within fenced enclosures for up to 1064 days under natural conditions with no supplemental feeding at an arid site contaminated 16 years previously with transuranic radionuclides. The estimated geometric mean (GM) GI-to-blood fractional transfer of 238Pu (0.0001) was about 20 times larger than the estimated transfer of 239+240Pu (0.000005), while the estimated transfer of 241Am (0.00001) was about 2 times larger than that of 239+240Pu. These GM GI-to-blood transfers were smaller than the GI-to-blood transfer value of 0.001 recommended by the International Commission on Radiological Protection (ICRP) for humans exposed via food chains or occupationally from unknown mixtures or compounds of plutonium and americium. Statistical tests indicated significantly (p less than 0.05) larger GI-to-tissue transfers of (1) 238Pu as compared to 239+240Pu for all tissues examined, (2) of 238Pu as compared to 241Am for muscle, liver, femur, and vertebra, and (3) of 241Am as compared to 239+240Pu for blood serum, femur, and kidney. The estimated GM fractional transfers of 137Cs from GI to muscle and liver were 0.03 (n = 8) and 0.001 (n = 3), respectively, assuming a 50-day biological half-time of 137Cs in cattle tissue. PMID:2814465

  17. 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. PMID:23565016

  18. AMS of the Minor Plutonium Isotopes

    PubMed Central

    Steier, P.; Hrnecek, E.; Priller, A.; Quinto, F.; Srncik, M.; Wallner, A.; Wallner, G.; Winkler, S.

    2013-01-01

    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu = (5.7 ± 1.0) × 10−5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method. PMID:23565016

  19. Minimum Critical Values Study

    SciTech Connect

    Fox, P.B.

    2005-07-11

    This report provides minimum critical values for various 30-cm water-reflected uranium and plutonium oxide and nitrate aqueous mixtures as calculated by the SCALE CSAS1X sequence using the 238-group ENDF/B-V neutron cross-section library. The minimum values were determined through parametric searches in one-dimensional geometry. The calculations have been performed to obtain the minimum values: critical volume and mass for spheres, critical radius for cylinders, critical thickness for slabs, and minimum critical concentration (infinite geometry) for the following homogeneous mixtures: (1) UO{sub 2}-H{sub 2}O for 3, 4, 5, 20, and 100 wt % {sup 235}U; (2) UNH for 3, 4, 5, 20, and 100 wt % {sup 235}U; (3) PuO{sub 2}-H{sub 2}O for 100/0/0, 95/5/0, 90/5/5, 80/10/10, and 71/17/11/1 wt % of {sup 239}Pu/{sup 240}Pu/{sup 241}Pu(/{sup 242}Pu); and (4) PuNH for 100/0/0, 95/5/0, 90/5/5, 80/10/10, and 71/17/11/1 wt % of {sup 239}Pu/{sup 240}Pu/{sup 241}Pu(/{sup 242}Pu). All bounding surfaces were fully reflected by 30 cm of H{sub 2}O.

  20. Distribution of 90Sr, 137Cs and 239,240Pu in Caspian Sea water and biota

    NASA Astrophysics Data System (ADS)

    Povinec, Pavel P.; Froehlich, Klaus; Gastaud, Janine; Oregioni, Beniamino; Pagava, Samson V.; Pham, Mai K.; Rusetski, Vladimir

    2003-09-01

    Two sampling expeditions were carried out in the Caspian Sea in 1995 and 1996. The aim was to investigate oceanographic conditions, water dynamics of the Sea and to measure radionuclide concentrations using 90Sr, 137Cs and 239,240Pu as tracers in the water column. Of the three basins comprising the Caspian Sea, the two deep basins (the central and southern basins) appear to be rapidly ventilated on a time scale of about 30 years, as shown by the penetration of radionuclides to bottom waters. The main source of radionuclides in the Sea has been global fallout and subsequent river run-off from catchment areas. At the stations visited, there were no signs of radioactive waste dumping, although the 90Sr levels found were higher than expected from global fallout, which may be due to remobilization of 90Sr from soil and its transport by rivers to the Sea. Radionuclide concentrations in fish and caviar are within the expected ranges and are not of radiological importance for consumption of fish and caviar from the Caspian Sea.

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

    PubMed

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

    2016-01-01

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

  2. [Accumulation of 238, 239 + 240Pu and 241Am in Boar Organs and Tissues on the Territory of the Belarusian Part of the ChNPP Exclusion Zone].

    PubMed

    Bondar, Yu I; Zabrotski, V N; Sadchikov, V I; Kalinin, V N

    2015-01-01

    The paper is devoted to determination of α-emitting radionuclides of 238, 239 + 240Pu and 241Am in liver, lungs, muscular and bone tissues of the boars on the territory of the Belarusian part of the ChNPP exclusion zone. It is shown that the content of Pu and Am isotopes in boar organs and tissues decreases in the following order: liver > bone tissues > lungs ≥ muscular tissues. The results received allow evaluation of penetration of 238, 239 + 240Pu and 241Am through the biological chain "soil-ration-organs and tissues". It is calculated that 1.7% of a boar's ration falls on the soil getting into the stomach with food. Translocation and accumulation coefficients characterizing the transfer of radionuclides through the chain "soil-vegetation-organs and tissues" were calculated. The conclusion about accumulation of Pu in the boar's body is made. PMID:26964350

  3. Neutron-induced fission cross section of 240Pu from 0.5 MeV to 3 MeV

    NASA Astrophysics Data System (ADS)

    Salvador-Castiñeira, P.; Bryś, T.; Eykens, R.; Hambsch, F.-J.; Göök, A.; Moens, A.; Oberstedt, S.; Sibbens, G.; Vanleeuw, D.; Vidali, M.; Pretel, C.

    2015-07-01

    240Pu has recently been pointed out by a sensitivity study of the Organization for Economic Cooperation and Development (OECD) Nuclear Energy Agency (NEA) to be one of the isotopes whose fission cross section lacks accuracy to meet the upcoming needs for the future generation of nuclear power plants (GEN-IV). In the High Priority Request List (HPRL) of the OECD, it is suggested that the knowledge of the 240Pu(n ,f ) cross section should be improved to an accuracy within 1-3 %, compared to the present 5%. A measurement of the 240Pu cross section has been performed at the Van de Graaff accelerator of the Joint Research Center (JRC) Institute for Reference Materials and Measurements (IRMM) using quasi-monoenergetic neutrons in the energy range from 0.5 MeV to 3 MeV. A twin Frisch-grid ionization chamber (TFGIC) has been used in a back-to-back configuration as fission fragment detector. The 240Pu(n ,f ) cross section has been normalized to three different isotopes: 237Np(n ,f ) , 235U (n ,f ) , and 238U (n ,f ) . Additionally, the secondary standard reactions were benchmarked through measurements against the primary standard reaction 235U (n ,f ) in the same geometry. A comprehensive study of the corrections applied to the data and the associated uncertainties is given. The results obtained are in agreement with previous experimental data at the threshold region. For neutron energies higher than 1 MeV, the results of this experiment are slightly lower than the ENDF/B-VII.1 evaluation, but in agreement with the experiments of Laptev et al. (2004) as well as Staples and Morley (1998).

  4. Examining (239+240)Pu, (210)Pb and historical events to determine carbon, nitrogen and phosphorus burial in mangrove sediments of Moreton Bay, Australia.

    PubMed

    Sanders, Christian J; Santos, Isaac R; Maher, Damien T; Breithaupt, Joshua L; Smoak, Joseph M; Ketterer, Michael; Call, Mitchell; Sanders, Luciana; Eyre, Bradley D

    2016-01-01

    Two sediment cores were collected in a mangrove forest to construct geochronologies for the previous century using natural and anthropogenic radionuclide tracers. Both sediment cores were dated using (239+240)Pu global fallout signatures as well as (210)Pb, applying both the Constant Initial Concentration (CIC) and the Constant Rate of Supply (CRS) models. The (239+240)Pu and CIC model are interpreted as having comparable sediment accretion rates (SAR) below an apparent mixed region in the upper ∼5 to 10 cm. In contrast, the CRS dating method shows high sediment accretion rates in the uppermost intervals, which is substantially reduced over the lower intervals of the 100-year record. A local anthropogenic nutrient signal is reflected in the high total phosphorus (TP) concentration in younger sediments. The carbon/nitrogen molar ratios and δ(15)N values further support a local anthropogenic nutrient enrichment signal. The origin of these signals is likely the treated sewage discharge to Moreton Bay which began in the early 1970s. While the (239+240)Pu and CIC models can only produce rates averaged over the intervals of interest within the profile, the (210)Pb CRS model identifies elevated rates of sediment accretion, organic carbon (OC), nitrogen (N), and TP burial from 2000 to 2013. From 1920 to 2000, the three dating methods provide similar OC, N and TP burial rates, ∼150, 10 and 2 g m(-2) year(-1), respectively, which are comparable to global averages. PMID:26004816

  5. Can 239 + 240Pu replace 137Cs as an erosion tracer in agricultural landscapes contaminated with Chernobyl fallout?

    PubMed

    Schimmack, W; Auerswald, K; Bunzl, K

    2001-01-01

    Erosion studies often use 137Cs from the global fallout (main period: 1953-1964) as a tracer in the soil. In many European countries, where 137Cs was deposited in considerable amounts also by the Chernobyl fallout in 1986, the global fallout fraction (GF-Cs) has to be separated from the Chernobyl fraction by means of the isotope 134Cs. In a few years, this will no longer be possible due to the short half-life of 134Cs (2 yr). Because GF-Cs in the soil can then no longer be determined, the potential of using 239 + 240Pu as a tracer is evaluated. This radionuclide originates in most European countries essentially only from the global fallout. The activities and spatial distributions of Pu and GF-Cs were compared in the soil of a steep field (inclination about 20%, area ca. 3 ha, main soil type Dystric Eutrochrept), sampled at 48 nodes of a 25 x 25 m2 grid. The reference values were determined at 12 points adjacent to the field. Their validity was assured by an inventory study of radiocaesium in a 70 ha area surrounding the field sampling 275 nodes of a 50 x 50 m2 grid. In the field studied, the activity concentrations of GF-Cs and Pu in the Ap horizon were not correlated (Spearman correlation coefficient R = 0.20, p > 0.05), and the activity balance of Pu differed from that of GF-Cs. Whereas no net loss of GF-Cs from the field was observed as compared to the reference site, Pu was more mobile with an average loss of ca. 11% per unit area. In addition, the spatial pattern of GF-Cs and Pu in the field differed significantly. The reason may be that due to their different associations with soil constituents, Pu and Cs represent different fractions of the soil, exhibiting different properties with respect to erosion/deposition processes. This indicates that both radionuclides or one of them may not be appropriate to quantity past erosion. When tracer losses are used to calibrate or verify erosion prediction models, systematic deviations may not only stem from model

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

    SciTech Connect

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

    1995-12-31

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

  7. 210Pb, 137Cs and 239,240Pu in East China Sea Sediments: Sources, Pathways and Budgets of Sediments and Radionuclides

    NASA Astrophysics Data System (ADS)

    Su, C.; Huh, C.

    2001-05-01

    Profiles of 210Pb, 137Cs and 239,240Pu measured in eighty-three sediment cores collected from various sedimentary regimes in the East China Sea were analyzed to elucidate the sources, routes and budgets of sediments as well as these radionuclides. Distributions of sedimentation rates and nuclide inventories reveal alongshore transport of sediments, 137Cs and 239,240Pu from the mouth of the Yangtze River toward the south, and it is largely confined to the inner-shelf area (water depth <70 m). Mass balance calculations of the budgets of nuclides suggest that the East China Sea is a sink for the particle-reactive 210Pb and 239,240Pu, with up to 20% of their sedimentary budgets supplied via boundary scavenging. In contrast, due to lower affinity of 137Cs for particles and rapid turnover of the shelf water, the East China Sea serves as a source for 137Cs. About two-thirds of the cumulative inputs of 137Cs have been transported out of the East China Sea, leaving the remaining one-third in sediments and the overlying water column. As for the sediment budget, mass balance can not be established due to a shortfall in sediment supply of more than 30% based on a comparison between input terms documented thus far and the sedimentation flux derived from this study. It could be that our sedimentation rates are overestimated, and/or that long-distance transport from the Yellow River's dispersal system to the ECS is underestimated previously. Alternatively, there is no reason to expect the attainment of equilibrium between sediment input and output in the East China Sea on decadal time scales.

  8. Parity splitting and E1/E2 branching in the alternating parity band of {sup 240}Pu from two-center octupole wave functions using supersymmetric quantum mechanics

    SciTech Connect

    Jolos, R. V.; Brentano, P. von

    2011-08-15

    An interpretation is suggested of the recently published experimental data on the alternating parity bands in {sup 240}Pu. The interpretation is based on the assumption that the main role in the description of the properties of the alternating parity bands plays the octupole mode which preserves the axial symmetry. The mathematical technique of the supersymmetric quantum mechanics is used for the realization of the model with the two-center octupole wave functions. A good description of the parity splitting and of the ratio of the dipole and quadrupole transitional moments is obtained for the first two bands.

  9. 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. PMID:18695410

  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. Method for determination of neptunium in large-sized urine samples using manganese dioxide coprecipitation and 242Pu as yield tracer.

    PubMed

    Qiao, Jixin; Hou, Xiaolin; Roos, Per

    2013-02-01

    A novel method for bioassay of large volumes of human urine samples using manganese dioxide coprecipitation for preconcentration was developed for rapid determination of (237)Np. (242)Pu was utilized as a nonisotopic tracer to monitor the chemical yield of (237)Np. A sequential injection extraction chromatographic (SI-EC) system coupled with inductively coupled plasma mass spectrometry (ICPMS) was exploited to facilitate the rapid column separation and quantification. The analytical results demonstrated satisfactory performance of the MnO(2) coprecipitation as indicated by the high chemical yields close to 100% and high separation capacity of processing up to 5 L of human urine samples. The MnO(2) coprecipitation process is simple and straightforward in which a batch (8-12) of samples can be pretreated within 4 h (i.e., <0.5 h/sample). In connection with the automated column separation and ICPMS quantification, which takes less than 1.5 h in total, the overall analytical time was on average less than 2 h for each sample. The high effectiveness and sample throughput make the developed method well suited for urine bioassay of (237)Np in routine monitoring of occupationally internal radiation exposure and rapid analysis of neptunium contamination level for emergency preparedness. PMID:23252688

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

    DOE PAGESBeta

    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.; et al

    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

  13. 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

    2015-04-01

    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. PMID:25723106

  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. Role of natural organic matter on iodine and (239)(,240)Pu distribution and mobility in environmental samples from the northwestern Fukushima Prefecture, Japan.

    PubMed

    Xu, Chen; Zhang, Saijin; Sugiyama, Yuko; Ohte, Nobuhito; Ho, Yi-Fang; Fujitake, Nobuhide; Kaplan, Daniel I; Yeager, Chris M; Schwehr, Kathleen; Santschi, Peter H

    2016-03-01

    In order to assess how environmental factors are affecting the distribution and migration of radioiodine and plutonium that were emitted from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, we quantified iodine and (239,240)Pu concentration changes in soil samples with different land uses (urban, paddy, deciduous forest and coniferous forest), as well as iodine speciation in surface water and rainwater. Sampling locations were 53-63 km northwest of the FDNPP within a 75-km radius, in close proximity of each other. A ranking of the land uses by their surface soil (<4 cm) stable (127)I concentrations was coniferous forest > deciduous forest > urban > paddy, and (239,240)Pu concentrations ranked as deciduous forest > coniferous forest > paddy ≥ urban. Both were quite distinct from that of (134)Cs and (137)Cs: urban > coniferous forest > deciduous forest > paddy, indicating differences in their sources, deposition phases, and biogeochemical behavior in these soil systems. Although stable (127)I might not have fully equilibrated with Fukushima-derived (129)I, it likely still works as a proxy for the long-term fate of (129)I. Surficial soil (127)I content was well correlated to soil organic matter (SOM) content, regardless of land use type, suggesting that SOM might be an important factor affecting iodine biogeochemistry. Other soil chemical properties, such as Eh and pH, had strong correlations to soil (127)I content, but only within a given land use (e.g., within urban soils). Organic carbon (OC) concentrations and Eh were positively, and pH was negatively correlated to (127)I concentrations in surface water and rain samples. It is also noticeable that (127)I in the wet deposition was concentrated in both the deciduous and coniferous forest throughfall and stemfall water, respectively, comparing to the bulk rainwater. Further, both forest throughfall and stemflow water consisted exclusively of organo-iodine, suggesting all inorganic iodine in the

  17. 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.

  18. 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. PMID:26736181

  19. 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

  20. Resolving Chernobyl vs. global fallout contributions in soils from Poland using Plutonium atom ratios measured by inductively coupled plasma mass spectrometry.

    PubMed

    Ketterer, Michael E; Hafer, Kevin M; Mietelski, Jerzy W

    2004-01-01

    Plutonium in Polish forest soils and the Bór za Lasem peat bog is resolved between Chernobyl and global fallout contributions via inductively coupled plasma mass spectrometric measurements of 240Pu/230Pu and 241Pu/239Pu atom ratios in previously prepared NdF3 alpha spectrometric sources. Compared to global fallout, Chernobyl Pu exhibits higher abundances of 240Pu and 241Pu. The ratios 240Pu/230Pu and 241Pu/239Pu co-vary and range from 0.186 to 0.348 and 0.0029 to 0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407 x [240Pu/239Pu] - 0.0413; r2 = 0.9924). Two-component mixing models are developed to apportion 239+240Pu and 241Pu activities; various estimates of the percentage of Chernobyl-derived 239+240Pu activity in forest soils range from < 10% to > 90% for the sample set. The 240Pu/230Pu - 241Pu/239Pu atom ratio mixing line extrapolates to estimate 241Pu/239Pu and the 241Pu/239+240Pu activity ratio for the Chernobyl source term (0.123 +/- 0.0007; 83 +/- 5; 1 May 1986). Sample 241Pu activities, calculated using existing alpha spectrometric 239+240Pu activities, and the 240Pu/230Pu and 241Pu/239Pu atom ratios, agree relatively well with previous liquid scintillation spectrometry measurements. Chernobyl Pu is most evident in locations from northeastern Poland. The 241Pu activities and/or the 241Pu/239Pu atom ratios are more sensitive than 240Pu/239Pu or 238Pu/239+240Pu activity ratios at detecting small Chernobyl 239+240Pu inputs, found in southern Poland. The mass spectrometric data show that the 241Pu activity is 40-62% Chernobyl-derived in southern Poland, and 58-96% Chernobyl in northeastern Poland. The Bór za Lasem peat bog (49.42 degrees N, 19.75 degrees E), located in the Orawsko-Nowotarska valley of southern Poland, consists of global fallout Pu. PMID:15023447

  1. Tracing the dispersion of contaminated sediment with plutonium isotope measurements in coastal catchments of Fukushima Prefecture

    NASA Astrophysics Data System (ADS)

    Evrard, Olivier; Pointurier, Fabien; Onda, Yuichi; Chartin, Caroline; Hubert, Amélie; Lepage, Hugo; Pottin, Anne-Claire; Lefèvre, Irène; Bonté, Philippe; Laceby, J. Patrick; Ayrault, Sophie

    2015-04-01

    The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurement of Pu isotopic atom and activity ratios is required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we measured Pu isotopic ratios in recently deposited sediments along rivers draining the most contaminated part of the inland radioactive plume. To this end, we carried out a thorough chemical purification and concentration of Pu from sediment samples (5 g dry material) and precise isotopic measurements using a double-focusing sector field ICP-MS. Results showed that the entire range of measured Pu isotopes (i.e., 239Pu, 240Pu, 241Pu, and 242Pu) were detected in all samples, although in extremely low concentrations. The 241Pu/239Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113±0.00008 on average in the Northern Hemisphere between 31°-71°N). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout, representing up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (45 km) from FDNPP and deposited in rivers representing a potential source of Pu to the ocean.

  2. 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.

  3. Age determination of single plutonium particles after chemical separation

    NASA Astrophysics Data System (ADS)

    Shinonaga, T.; Donohue, D.; Ciurapinski, A.; Klose, D.

    2009-01-01

    Age determination of single plutonium particles was demonstrated using five particles of the standard reference material, NBS 947 (Plutonium Isotopic Standard. National Bureau of Standards, Washington, D.C. 20234, August 19, 1982, currently distributed as NBL CRM-137) and the radioactive decay of 241Pu into 241Am. The elemental ratio of Am/Pu in Pu particles found on a carbon planchet was measured by wavelength dispersive X-ray spectrometry (WDX) coupled to a scanning electron microscope (SEM). After the WDX measurement, each plutonium particle, with an average size of a few μm, was picked up and relocated to a silicon wafer inside the SEM chamber using a micromanipulator. The silicon wafer was then transferred to a quartz tube for dissolution in an acid solution prior to chemical separation. After the Pu was chemically separated from Am and U, the isotopic ratios of Pu ( 240Pu/ 239Pu, 241Pu/ 239Pu and 242Pu/ 239Pu) were measured with a thermal ionization mass spectrometer (TIMS) for the calculation of Pu age. The age of particles determined in this study was in good agreement with the expected age (35.9 a) of NBS 947 within the measurement uncertainty.

  4. Determination of plutonium isotopic composition by gamma-ray spectroscopy

    SciTech Connect

    Sampson, T.E.; Hsue, S.T.; Parker, J.L.; Johnson, S.S.; Bowersox, D.F.

    1981-01-01

    We discuss the general approach, computerized data analysis methods, and results of measurements used to determine the isotopic composition of plutonium by gamma-ray spectroscopy. The simple techniques are designed to be applicable to samples of arbitrary size, geometry, age, chemical, and isotopic composition. The combination of the gamma spectroscopic measurement of isotopic composition coupled with calorimetric measurement of total sample power is shown to give a totally nondestructive determination of sample plutonium mass with a precision of 0.6% for 1000-g samples of PuO/sub 2/ with 12% /sup 240/Pu content. The precision of isotopic measurements depends upon many factors, including sample size, sample geometry, and isotopic content. Typical ranges are found to be /sup 238/Pu, 1 to 10%; /sup 239/Pu, 0.1 to 0.5%; /sup 240/Pu, 2 to 5%; /sup 241/Pu, 0.3 to 0.7%; /sup 242/Pu (determined by isotopic correlation); and /sup 241/Am, 0.2 to 10%.

  5. 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.

  6. 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

  7. Novel insights into Fukushima nuclear accident from isotopic evidence of plutonium spread along coastal rivers.

    PubMed

    Evrard, Olivier; Pointurier, Fabien; Onda, Yuichi; Chartin, Caroline; Hubert, Amélie; Lepage, Hugo; Pottin, Anne-Claire; Lefèvre, Irène; Bonté, Philippe; Laceby, J Patrick; Ayrault, Sophie

    2014-08-19

    The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurements of Pu isotopic atom and activity ratios are required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP-MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., (239)Pu, (240)Pu, (241)Pu, and (242)Pu) were detected in all samples, although in extremely low concentrations. The (241)Pu/(239)Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113 ± 0.00008 on average for the Northern Hemisphere between 31°-71° N: Kelley, J. M.; Bond, L. A.; Beasley, T. M. Global distribution of Pu isotopes and (237)Np. Sci. Total. Env. 1999, 237/238, 483-500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high (241)Pu/(239)Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean. PMID:25014620

  8. Measurements of cross sections and decay properties of the isotopes of elements 112, 114, and 116 produced in the fusion reactions 233,238 U , 242Pu , and 248Cm + 48Ca

    NASA Astrophysics Data System (ADS)

    Oganessian, Yu. Ts.; Utyonkov, V. K.; Lobanov, Yu. V.; Abdullin, F. Sh.; Polyakov, A. N.; Shirokovsky, I. V.; Tsyganov, Yu. S.; Gulbekian, G. G.; Bogomolov, S. L.; Gikal, B. N.; Mezentsev, A. N.; Iliev, S.; Subbotin, V. G.; Sukhov, A. M.; Voinov, A. A.; Buklanov, G. V.; Subotic, K.; Zagrebaev, V. I.; Itkis, M. G.; Patin, J. B.; Moody, K. J.; Wild, J. F.; Stoyer, M. A.; Stoyer, N. J.; Shaughnessy, D. A.; Kenneally, J. M.; Wilk, P. A.; Lougheed, R. W.; Il'Kaev, R. I.; Vesnovskii, S. P.

    2004-12-01

    We have studied the dependence of the production cross sections of the isotopes 282,283 112 and 286,287 114 on the excitation energy of the compound nuclei 286112 and 290114 . The maximum cross section values of the xn -evaporation channels for the reaction 238U ( 48Ca ,xn) 286-x 112 were measured to be σ3n = 2.5 +1.8 -1.1 pb and σ4n = 0.6 +1.6 -0.5 pb ; for the reaction 242Pu ( 48Ca ,xn) 290-x 114 : σ2n ˜0.5 pb , σ3n = 3.6 +3.4 -1.7 pb , and σ4n = 4.5 +3.6 -1.9 pb . In the reaction 233U ( 48Ca ,2 4n) 277 279 112 at E*=34.9±2.2 MeV we measured an upper cross section limit of σxn ⩽0.6 pb . The observed shift of the excitation energy associated with the maximum sum evaporation residue cross section σER (E*) to values significantly higher than that associated with the calculated Coulomb barrier can be caused by the orientation of the deformed target nucleus in the entrance channel of the reaction. An increase of σER in the reactions of actinide targets with 48Ca is consistent with the expected increase of the survivability of the excited compound nucleus upon closer approach to the closed neutron shell N=184 . In the present work we detected 33 decay chains arising in the decay of the known nuclei 282112 , 283112 , 286114 , 287114 , and 288114 . In the decay of 287114 (α) → 283112 (α) → 279110 (SF) , in two cases out of 22, we observed decay chains of four and five sequential α transitions that end in spontaneous fission of 271Sg ( Tα/SF = 2.4 +4.3 -1.0 min) and 267Rf ( TSF ˜2.3 h) , longer decay chains than reported previously. We observed the new nuclide 292116 ( Tα = 18 +16 -6 ms, Eα =10.66±0.07 MeV) in the irradiation of the 248Cm target at a higher energy than in previous experiments. The observed nuclear decay properties of the nuclides with Z=104 118 are compared with theoretical nuclear mass calculations and the systematic trends of spontaneous fission properties. As a whole, they give a consistent pattern of decay of the 18 even- Z

  9. Measurement of Absolute Fission Yields in the Fast Neutron-Induced Fission of Actinides: {sup 238}U, {sup 237}Np, {sup 238}Pu, {sup 240}Pu, {sup 243}Am, and {sup 244}Cm by Track-Etch-cum-Gamma Spectrometry

    SciTech Connect

    Iyer, R.H.; Naik, H.; Pandey, A.K.; Kalsi, P.C.; Singh, R.J.; Ramaswami, A.; Nair, A.G.C.

    2000-07-15

    The absolute fission yields of 46 fission products in {sup 238}U (99.9997 at.%), 46 fission products in {sup 237}Np, 27 fission products in {sup 238}Pu (99.21 at.%), 30 fission products in {sup 240}Pu (99.48 at.%), 30 fission products in {sup 243}Am (99.998 at.%), and 32 fission products in {sup 244}Cm (99.43 at.%) induced by fast neutrons were determined using a fission track-etch-cum-gamma spectrometric technique. In the case of highly alpha-active and sparingly available actinides - e.g., {sup 238}Pu, {sup 240}Pu, {sup 243}Am, and {sup 244}Cm - a novel recoil catcher technique to collect the fission products on a Lexan polycarbonate foil followed by gamma-ray spectrometry was developed during the course of this work. This completely removed interferences from (a) gamma rays of daughter products in secular equilibrium with the target nuclide (e.g., {sup 243}Am-{sup 239}Np), (b) activation products of the catcher foil [e.g., {sup 24}Na from Al(n,{alpha})], and (c) activation products of the target [e.g., {sup 238}Np from {sup 237}Np(n,{gamma}) and {sup 239}Np from {sup 238}U(n,{gamma})] reactions, making the gamma spectrometric analysis very simple and accurate. The high-yield asymmetric fission products were analyzed by direct gamma spectrometry, whereas the low-yield symmetric products (e.g., Ag, Cd, and Sb) as well as some of the asymmetric fission products (e.g., Br) and rare earths (in the case of {sup 238}U and {sup 237}Np) were radiochemically separated and then analyzed by gamma-ray spectrometry. The neutron spectra in the irradiation positions of the reactors were measured and delineated in the thermal to 10-MeV region using threshold activation detectors. The present data were compared with the ENDF/VI and UKFY2 evaluated data files. From the measured cumulative yields, the mass-chain yields have been deduced using charge distribution systematics. The mass yields, along with similar data for other fast neutron-induced fissioning systems, show several

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  11. Association of Chernobyl-derived 239+240Pu, 241Am, 90Sr and 137Cs with different molecular size fractions of organic matter in the soil solution of two grassland soils.

    PubMed

    Bunzl, K; Kracke, W; Agapkina, G I; Tikhomirov, A; Shcheglov, A I

    1998-10-01

    Radiocesium is normally bound only rather weakly and unspecifically by humic substances, in contrast to the actinides Pu and Am. Recently, however, it was observed that fallout 137Cs in the soil solution from an Of-horizon of a podzol forest soil (slightly decomposed plant material) was associated essentially only with one single size fraction of the humic substances. In deeper soil layers with well humified material (AOh-horizon), radiocesium was associated with all size fractions of the dissolved organic matter (DOM). To examine whether this unexpected behaviour is also observable for DOM isolated from other soils, we determined the association of fallout 137Cs, 90Sr, 238Pu, 239+240Pu and 241Am with various size fractions of DOM from in situ soil solutions isolated from two layers (0-2 cm and 2-5 cm) of two grassland soils (a soddy podzolic soil and a peat soil) within the 10 km zone of the nuclear reactor at Chernobyl (Ukraine). The four size fractions of DOM as obtained by gel filtration of the soil solution were (mean nominal molecular weight in daltons): fraction I: > or = 2000, fraction II: 1300; fraction III: 560, fraction IV: inorganic compounds. The results for the well humified DOM (humus accumulation horizon of podzol, deeper layer of peat soil) showed that Pu and Am are essentially associated with the high molecular weight fractions, while Sr is present only in the 'inorganic' fraction. Radiocesium is found in all the size fractions separated. A quite similar pattern was also found for Pu, Am, and Sr in the soil solution from only slightly decomposed plant material (0-2 cm of peat soil), but not for radiocesium. This radionuclide was again essentially only observable in one single low molecular weight fraction of DOM. The above results thus support our recent observations in the different horizons of a forest podzol mentioned above, even though no reason for the different binding of radiocesium by well humified soil organic matter and by only slightly

  12. Plutonium isotopic determination from gamma-ray spectra

    SciTech Connect

    Skourikhine, A.N.; Strittmatter, R.B.; Zardecki, A.

    1998-12-31

    The use of low- and medium-resolution room-temperature detectors for the nondestructive assay of nuclear materials has widespread applications to the safeguarding of nuclear materials. The challenge to using these detectors is the inherent difficulty of the spectral analysis to determine the amount of specific nuclear materials in the measured samples. This is especially true for extracting plutonium isotopic content from low- and medium-resolution spectral lines that are not well resolved. In this paper, neural networks trained by stochastic and singular value decomposition algorithms are applied to retrieve the plutonium isotopic content from a simulated NaI spectra. The simulated sample consists of isotopes {sup 238}Pu, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, and {sup 241}Am. It is demonstrated that the neutral network optimized by singular value decomposition (SVD) and stochastic training algorithms is capable of estimating plutonium content consistently resulting in an average error much smaller than the error previously reported.

  13. Application of ICP-QMS for the determination of plutonium in environmental samples for safeguards purposes.

    PubMed

    Godoy, Maria Luiza D P; Godoy, José Marcus; Roldão, Luiz Alfredo

    2007-01-01

    Aiming to determine the plutonium amount as well as its isotopic composition, in particular, in swipe samples for safeguards purposes, an analytical method was developed with a plutonium separation step based on extraction chromatography using 2 cm TEVA columns and detection with quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with membrane desolvation system. The method was successfully applied to New Brunswick plutonium certified reference materials as well as to Lawrence Livermore National Laboratory round robin samples, based on the round robin samples provided by the Institute for Reference Materials and Measurements (Belgium), as part of the Regular European Interlaboratory Measurement Evaluation Programme (REIMEP), campaign 16 (isotopic abundances of plutonium in plutonium nitrate samples), with a total plutonium amount between 1 and 0.25 ng per sample. After the introduction of an additional separation step, it was also possible to carry out precise and accurate total plutonium, (240)Pu/(239)Pu, (241)Pu/(239)Pu and (242)Pu/(239)Pu atom ratios determination in sediment sample showing its applicability to environmental samples in general, reaching a detection limit equivalent to 5 mBq(239)Pu kg(-1). PMID:17543430

  14. In-plant measurements of gamma-ray transmissions for precise K-edge and passive assay of plutonium concentration and isotopic fractions in product solutions. Final report on TASTEX Task G

    SciTech Connect

    Russo, P.A.; Hsue, S.T.; Sprinkle, J.K. Jr.; Johnson, S.S.; Asakura, Y.; Kondo, I.; Masui, J.; Shoji, K.

    1982-08-01

    An instrument based upon high-resolution gamma-ray measurements has been tested for more than 1 year at the Tokai Reprocessing Facility for determination of plutonium concentration by K-edge absorption densitometry and for determination of plutonium isotopic fractions by transmission-corrected passive gamma-ray spectrometry. The nondestructive assay instrument was designed and built at Los Alamos National Laboratory for the Tokai Advanced Safeguards Technology Exercise (TASTEX). It was used at Tokai for the timely assay of more than 100 product solution samples during the TASTEX evaluations. The results were compared to reference values obtained by conventional destructive analysis of these samples. The precision and accuracy of plutonium concentrations measured by the K-edge technique are shown to be within 0.6% (1delta) in these applications. The precisions and accuracies of the isotopic fractions determined by these passive gamma-ray methods are shown to be within 0.4% for /sup 239/Pu, 1% for /sup 240/Pu and /sup 241/Pu, and 10% for /sup 242/Pu.

  15. Radioactinide Additions to the Electronic Gamma-ray Spectrum Catalogue

    SciTech Connect

    R.J. Gehrke; J.R. Davidson; P.J. Taylor; R.G. Helmer; J.W. Mandler

    2001-05-01

    With the completion of a CD ROM version of the original R. L. HEATH''s Gamma-ray Spectrum Catalogue, it became obvious that a number of radionuclides are missing which are important to various fields of nuclear science and technology. With a large amount of transuranic waste awaiting permanent disposal across the Department of Energy (DOE) complex and the need for its assay in order to dispose of it, it was decided that the addition of the radioactinides encountered in transuranic waste should be the first priority. In response to this need, the spectra of 233U, 235U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am and 243Am have been acquired with modern Ge detectors, and prepared for graphics presentation along with the parent and progeny decay chains and decay schemes. The associated tables of -ray energies and emission probabilities have been downloaded from the Evaluated Nuclear Structure Data file (ENSDF) database. This information is being incorporated into the Gamma-Ray Spectrometry Center Web Site at http://id.inel.gov/gamma

  16. A priori precision estimation for neutron triples counting

    SciTech Connect

    Croft, S.; Swinhoe, M. T.; Henzl, V.

    2011-07-01

    The nondestructive assay of Plutonium bearing items for criticality, safety, security, safeguards, inventory balance, process control, waste management and compliance is often undertaken using correlated neutron counting. In particular Multiplicity Shift Register analysis allows one to extract autocorrelation parameters from the pulse train which can, within the framework of a simple interpretational model, be related to the effective {sup 240}Pu spontaneous fission mass present. The effective {sup 240}Pu mass is a weighted sum of the {sup 238}Pu, {sup 240}Pu and {sup 242}Pu masses so if the relative isotopic composition of the Pu can be established from the measured {sup 240}Pu effective mass one can estimate the total Pu mass and also the masses of the individual isotopes, example the fissile species {sup 239}Pu and {sup 241}Pu. In multiplicity counting three counting rates are obtained. These are the Singles, Doubles and Triples rates. The Singles rate is just the gross, totals or trigger rate. The Doubles and Triples rates are calculated from factorial moments of the observed signal triggered neutron multiplicity distributions following spontaneous fission in the item and can be thought of as the rate of observed coincident pairs and coincident triplets on the pulse train. Coincident events come about because the spontaneous fission and induced fission chains taking place in the item result in bursts of neutrons. These remain time correlated during the detection process and so retain information, through the burst size distribution, about the Pu content. In designing and assessing the performance of a detector system to meet a given goal it is necessary to make a priori estimates of the counting precision for all three kinds of rates. This is non-trivial because the counting does not obey the familiar rules of a Poissonian counting experiment because the pulse train has time correlated events on it and the train is sampled by event triggered gates that may

  17. 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.

  18. Neutron-induced Fission Cross Section of 240242Pu up to En = 3 MeV

    NASA Astrophysics Data System (ADS)

    Salvador-Castiñeira, P.; Bryś, T.; Hambsch, F.-J.; Oberstedt, S.; Pretel, C.; Vidali, M.

    2014-05-01

    The neutron-induced fission cross sections of 240,242Pu have been measured at JRC-IRMM with incident neutron energy from 0.2 MeV up to 3 MeV. A Twin-Frisch Grid Ionization Chamber (TFGIC) has been used in a back-to-back geometry. The measurements have been performed using the secondary standards 237Np and 238U as a reference. The purity of the plutonium samples was 99.89% for 240Pu and 99.97% for 242Pu. The results obtained follow the ENDF/B-VII.1 evaluation for 240Pu, but some discrepancies are visible around E/n = 1 MeV for 242Pu. In addition, the spontaneous fission half-life has been measured for both isotopes.

  19. TRU Waste Assay Methodology with the Combined Thermal Epithermal Neutron (CTEN) System

    SciTech Connect

    Veilleux, J. M.; Enter, J. A.

    2003-02-27

    The CTEN assay system is designed to measure plutonium bearing 208-L waste drums and make the transuranic versus low-level waste determination. The system was certified for Waste Isolation Pilot Plant operations and the Environmental Protection Agency approved the CTEN in 2002. It is the only system capable of making the transuranic/low-level waste (TRU/LLW) determination since it can routinely assay below 100 nCi/g. The system conducts a measurement by using either (or both) an active 14 MeV neutron pulse to induce fission in 239Pu and 241Pu or measures the spontaneous fission properties of 238Pu, 240Pu and 242Pu. When the coincidence neutron signal is combined with mass fraction data from a gamma system, the result is the total plutonium mass. The system's lower limit of detection is as low as 2 mg of weapons grade plutonium, making it an ideal platform to make the TRU/LLW determination. Analysis of an assay is made with visual basic application driven subroutines and Micros oft Excel spreadsheets. Input values and calculations include: the raw neutron scaler and coincidence counts; mass fraction information; plutonium mass; alpha, total and TRU activity; thermal power, 239Pu Equivalent Curies; fissile gram equivalent mass; decay heat; and uncertainties associated with each parameter. A general diagnostic analysis is performed for each assay to facilitate a technical review of the results. The results of analysis from 372 waste drums are summarized. The results indicate that modifying current operating procedures involving the use of acceptable knowledge isotope data and use of the lower detection limit could increase the number of certifiable assays from 38% to 66%.

  20. 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

  1. 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.

  2. 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

    2015-01-01

    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+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. PMID:25881009

  3. 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. PMID:16124281

  4. FFTF (Fast Flux Test Facility) Reactor Characterization Program: Absolute Fission-rate Measurements

    SciTech Connect

    Fuller, J.L.; Gilliam, D.M.; Grundl, J.A.; Rawlins, J.A.; Daughtry, J.W.

    1981-05-01

    Absolute fission rate measurements using modified National Bureau of Standards fission chambers were performed in the Fast Flux Test Facility at two core locations for isotopic deposits of {sup 232}Th, {sup 233}U, {sup 235}U, {sup 238}U, {sup 237}Np, {sup 239}Pu, {sup 240}Pu, and {sup 241}Pu. Monitor chamber results at a third location were analyzed to support other experiments involving passive dosimeter fission rate determinations.

  5. FFTF (FAST FLUX TEST FACILITY) REACTOR CHARACTERIZATION PROGRAM ABSOLUTE FISSION RATE MEASUREMENTS

    SciTech Connect

    FULLER JL; GILLIAM DM; GRUNDL JA; RAWLINS JA; DAUGHTRY JW

    1981-05-01

    Absolute fission rate measurements using modified National Bureau of Standards fission chambers were performed in the Fast Flux Test Facility at two core locations for isotopic deposits of {sup 232}Th, {sup 233}U, {sup 235}U, {sup 238}U, {sup 237}Np, {sup 239}Pu, {sup 240}Pu, and {sup 241}Pu. Monitor chamber results at a third location were analyzed to support other experiments involving passive dosimeter fission rate determinations.

  6. Measurement of Neutron Induced and Spontaneous Fission in Pu-242 at DANCE

    NASA Astrophysics Data System (ADS)

    Chyzh, Andrii; Wu, C. Y.; Henderson, R.; Couture, A.; Lee, H. Y.; Ullmann, J.; O'Donnell, J. M.; Jandel, M.; Haight, R. C.; Bredeweg, T. A.; Dance Collaboration

    2013-10-01

    Neutron capture and fission reactions are important in nuclear engineering and physics. DANCE (Detector for Advanced Neutron Capture Measurement, LANL) combined with PPAC (avalanche technique based fission tagging detector, LLNL) were used to study neutron induced and spontaneous fission in 242Pu. 2 measurements were performed in 2013. The first experiment was done without the incident neutron beam with the fission tagging ability to study γ-rays emitted in the spontaneous fission of 242Pu. The second one - with the neutron beam to measure both the neutron capture and fission reactions. This is the first direct measurement of prompt fission γ-rays in 242Pu. The γ-ray multiplicity, γ-ray energy, and total energy of γ-rays per fission in 242Pu will be presented. These distributions of the 242Pu spontaneous fission will be compared to those in the 241Pu neutron induced fission. This work was performed under the auspices of the US Department of Energy by Los Alamos National Laboratory under Contract DE-AC52-06NA25396 and Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

  7. 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. PMID:25050458

  8. ZPR-6 assembly 7 high {sup 240} PU core : a cylindrical assemby with mixed (PU, U)-oxide fuel and a central high {sup 240} PU zone.

    SciTech Connect

    Lell, R. M.; Schaefer, R. W.; McKnight, R. D.; Tsiboulia, A.; Rozhikhin, Y.; Nuclear Engineering Division; Inst. of Physics and Power Engineering

    2007-10-01

    Over a period of 30 years more than a hundred Zero Power Reactor (ZPR) critical assemblies were constructed at Argonne National Laboratory. The ZPR facilities, ZPR-3, ZPR-6, ZPR-9 and ZPPR, were all fast critical assembly facilities. The ZPR critical assemblies were constructed to support fast reactor development, but data from some of these assemblies are also well suited to form the basis for criticality safety benchmarks. Of the three classes of ZPR assemblies, engineering mockups, engineering benchmarks and physics benchmarks, the last group tends to be most useful for criticality safety. Because physics benchmarks were designed to test fast reactor physics data and methods, they were as simple as possible in geometry and composition. The principal fissile species was {sup 235}U or {sup 239}Pu. Fuel enrichments ranged from 9% to 95%. Often there were only one or two main core diluent materials, such as aluminum, graphite, iron, sodium or stainless steel. The cores were reflected (and insulated from room return effects) by one or two layers of materials such as depleted uranium, lead or stainless steel. Despite their more complex nature, a small number of assemblies from the other two classes would make useful criticality safety benchmarks because they have features related to criticality safety issues, such as reflection by soil-like material. The term 'benchmark' in a ZPR program connotes a particularly simple loading aimed at gaining basic reactor physics insight, as opposed to studying a reactor design. In fact, the ZPR-6/7 Benchmark Assembly (Reference 1) had a very simple core unit cell assembled from plates of depleted uranium, sodium, iron oxide, U3O8, and plutonium. The ZPR-6/7 core cell-average composition is typical of the interior region of liquid-metal fast breeder reactors (LMFBRs) of the era. It was one part of the Demonstration Reactor Benchmark Program,a which provided integral experiments characterizing the important features of demonstration-size LMFBRs. As a benchmark, ZPR-6/7 was devoid of many 'real' reactor features, such as simulated control rods and multiple enrichment zones, in its reference form. Those kinds of features were investigated experimentally in variants of the reference ZPR-6/7 or in other critical assemblies in the Demonstration Reactor Benchmark Program.

  9. Development of Superconducting High-Resolution Gamma-Ray Spectrometers for Nuclear Safeguards

    NASA Astrophysics Data System (ADS)

    Dreyer, Jonathan Glen

    Superconducting high-resolution gamma-ray spectrometers based on molybdenum/ copper transition edge sensors (TES) with tin absorbers have been developed for nuclear safeguard applications. This dissertation focuses on plutonium analysis, specifically the direct measurement of the 242Pu gamma-ray signature at 44.915 keV. As existing nondestructive analysis methods cannot directly measure this or any other 242Pu signature, the feasibility of making such a measurement using a TES based system is presented. Analysis from of Monte Carlo simulations and analytical noise models shows that the direct detection of this gamma-ray line of is possible and can be quantified in the presence of a 240Pu gamma-ray line with a line separation of 324 eV, even if the emission from the 240Pu is several orders of magnitude stronger. Spectroscopic measurements conducted in a liquid cryogen system offered an energy resolution of 180 eV, adequate for the measurement of 242Pu; however, TES operation in a liquid-cryogen-free pulse tube refrigerator degraded sensor performance such that this measurement was no longer possible. The numerical noise model indicates that the energy resolution of this device is adequate to demonstrate a direct measurement of 242Pu if the noise pickup from the mechanical cooler can be suppressed. This work shows that the precise measurement of low-intensity gamma-ray signatures, such as the 44.915 keV gamma ray from 242Pu, will require arrays of low-noise TES sensors and that such a system would offer invaluable information in the analysis of plutonium bearing materials.

  10. Bioreduction amenability testing of actinide contaminated soils. The systems: Am{sup 241}-Pu{sup 238}, Am{sup 241}-Pu{sup 239/40}, U

    SciTech Connect

    Korich, D.G.; Sharp, J.E.

    1995-01-01

    Bioreductive processing of actinide contaminated soils can achieve extraction levels in excess of 97% for both plutonium and uranium contaminants. Reasonable reaction rates of 4 to 6 day resident times for Pu-Am have been demonstrated on 4 gram sample charges. Longer reaction times of 17 days required for uranium extraction can be improved by soil sample preconditioning and/or an increase in process reagent concentrations. The environmentally benign treatment process operates at pH 6--7, preserves the original soil matrix, and utilizes standard processing equipment. The process reagent component (inoculum SD-1 and biological growth medium PX100{trademark}) are available for utilization in an integrated system. Process techniques developed by MBX, involving graduated volume bioreactors have been proven to alleviate biological toxicity problems in treatment leachates. Bioreduction processing of actinide contaminated soils, preconditioning of soil charges, and recycling or vegetation of unacceptable tailings can be combined to provide an effective and environmentally attractive method of remediation. The soil test program was designed to determine the applicability of the MBX bioreductive technology to solubilize Pu and Am from RFP, Mound and LANL soils and uranium from Hanford and Fernald soils.

  11. /sup 239/ /sup 240/Pu and /sup 238/Pu in sediments of the Hudson River estuary

    SciTech Connect

    Linsalata, P.; Wrenn, M.E.; Cohen, N.; Singh, N.P.

    1980-12-01

    Plutonium-239,240 and plutonium-238 were determined in 59 Hudson River sediment dredge samples collected during 1973-77 in the vicinity of the Indian Point Nuclear Power Station. Acid leaching followed by solvent extraction, electrodeposition, and alpha-spectrometry were used to extract, purify, and quantitate plutonium isotopes present in these samples. Annual median plutonium-238/plutonium-239,240 isotopic activity ratios in surficial sediments were 0.032 (1973-74), 0.035 (1975), 0.042 (1976), and 0.040 (1977). The source of these nuclides in the estuary was identified by analysis of the sample isotopic activity ratios. On the basis of the sampling regimen and the methods used, it is concluded that no input, other than that of fallout, has contributed significantly to the plutonium burden in Hudson sediments. (1 map, 9 references, 9 tables)

  12. Spatially resolved analysis of plutonium isotopic signatures in environmental particle samples by laser ablation-MC-ICP-MS.

    PubMed

    Konegger-Kappel, Stefanie; Prohaska, Thomas

    2016-01-01

    Laser ablation-multi-collector-inductively coupled plasma mass spectrometry (LA-MC-ICP-MS) was optimized and investigated with respect to its performance for determining spatially resolved Pu isotopic signatures within radioactive fuel particle clusters. Fuel particles had been emitted from the Chernobyl nuclear power plant (ChNPP) where the 1986 accident occurred and were deposited in the surrounding soil, where weathering processes caused their transformation into radioactive clusters, so-called micro-samples. The size of the investigated micro-samples, which showed surface alpha activities below 40 mBq, ranged from about 200 to 1000 μm. Direct single static point ablations allowed to identify variations of Pu isotopic signatures not only between distinct fuel particle clusters but also within individual clusters. The resolution was limited to 100 to 120 μm as a result of the applied laser ablation spot sizes and the resolving power of the nuclear track radiography methodology that was applied for particle pre-selection. The determined (242)Pu/(239)Pu and (240)Pu/(239)Pu isotope ratios showed a variation from low to high Pu isotope ratios, ranging from 0.007(2) to 0.047(8) for (242)Pu/(239)Pu and from 0.183(13) to 0.577(40) for (240)Pu/(239)Pu. In contrast to other studies, the applied methodology allowed for the first time to display the Pu isotopic distribution in the Chernobyl fallout, which reflects the differences in the spent fuel composition over the reactor core. The measured Pu isotopic signatures are in good agreement with the expected Pu isotopic composition distribution that is typical for a RBMK-1000 reactor, indicating that the analyzed samples are originating from the ill-fated Chernobyl reactor. The average Pu isotope ratios [(240)Pu/(239)Pu = 0.388(86), (242)Pu/(239)Pu = 0.028(11)] that were calculated from all investigated samples (n = 48) correspond well to previously published results of Pu analyses in contaminated samples from

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

    SciTech Connect

    Meadows, J W

    1983-10-01

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

  14. Isotopic evidence of plutonium release into the environment from the Fukushima DNPP accident

    PubMed Central

    Zheng, Jian; Tagami, Keiko; Watanabe, Yoshito; Uchida, Shigeo; Aono, Tatsuo; Ishii, Nobuyoshi; Yoshida, Satoshi; Kubota, Yoshihisa; Fuma, Shoichi; Ihara, Sadao

    2012-01-01

    The Fukushima Daiichi nuclear power plant (DNPP) accident caused massive releases of radioactivity into the environment. The released highly volatile fission products, such as 129mTe, 131I, 134Cs, 136Cs and 137Cs were found to be widely distributed in Fukushima and its adjacent prefectures in eastern Japan. However, the release of non-volatile actinides, in particular, Pu isotopes remains uncertain almost one year after the accident. Here we report the isotopic evidence for the release of Pu into the atmosphere and deposition on the ground in northwest and south of the Fukushima DNPP in the 20–30 km zones. The high activity ratio of 241Pu/239+240Pu (> 100) from the Fukushima DNPP accident highlights the need for long-term 241Pu dose assessment, and the ingrowth of 241Am. The results are important for the estimation of reactor damage and have significant implication in the strategy of decontamination. PMID:22403743

  15. Isotopic evidence of plutonium release into the environment from the Fukushima DNPP accident.

    PubMed

    Zheng, Jian; Tagami, Keiko; Watanabe, Yoshito; Uchida, Shigeo; Aono, Tatsuo; Ishii, Nobuyoshi; Yoshida, Satoshi; Kubota, Yoshihisa; Fuma, Shoichi; Ihara, Sadao

    2012-01-01

    The Fukushima Daiichi nuclear power plant (DNPP) accident caused massive releases of radioactivity into the environment. The released highly volatile fission products, such as (129m)Te, (131)I, (134)Cs, (136)Cs and (137)Cs were found to be widely distributed in Fukushima and its adjacent prefectures in eastern Japan. However, the release of non-volatile actinides, in particular, Pu isotopes remains uncertain almost one year after the accident. Here we report the isotopic evidence for the release of Pu into the atmosphere and deposition on the ground in northwest and south of the Fukushima DNPP in the 20-30 km zones. The high activity ratio of (241)Pu/(239+240)Pu (> 100) from the Fukushima DNPP accident highlights the need for long-term (241)Pu dose assessment, and the ingrowth of (241)Am. The results are important for the estimation of reactor damage and have significant implication in the strategy of decontamination. PMID:22403743

  16. 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. PMID:18677996

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

    PubMed

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

    2008-11-01

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

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

    PubMed

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

    2006-01-01

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

  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. Preparation of a multi-isotope plutonium AMS standard and preliminary results of a first inter-lab comparison

    NASA Astrophysics Data System (ADS)

    Dittmann, B.-A.; Dunai, T. J.; Dewald, A.; Heinze, S.; Feuerstein, C.; Strub, E.; Fifield, L. K.; Froehlich, M. B.; Tims, S. G.; Wallner, A.; Christl, M.

    2015-10-01

    The motivation of this work is to establish a new multi-isotope plutonium standard for isotopic ratio measurements with accelerator mass spectrometry (AMS), since stocks of existing solutions are declining. To this end, certified reference materials (CRMs) of each of the individual isotopes 239Pu, 240Pu, 242Pu and 244Pu were obtained from JRC IRMM (Joint Research Center Institute for Reference Materials and Measurements). These certified reference materials (IRMM-081a, IRMM-083, IRMM-043 and IRMM-042a) were diluted with nitric acid and mixed to obtain a stock standard solution with an isotopic ratio of approximately 1.0:1.0:1.0:0.1 (239Pu:240Pu:242Pu:244Pu). From this stock solution, samples were prepared for measurement of the plutonium isotopic composition by AMS. These samples have been measured in a round-robin exercise between the AMS facilities at CologneAMS, at the ANU Canberra and ETH Zurich to verify the isotopic ratio and to demonstrate the reproducibility of the measurements. The results show good agreement both between the different AMS measurements and with the gravimetrically determined nominal ratios.

  1. Unsafe coulomb excitation of {sup 240-244}Pu.

    SciTech Connect

    Wiedenhoever, I.

    1998-12-01

    The high spin states of {sup 240}Pu and {sup 244}Pu have been investigated with GAMMASPHERE at ATLAS, using Coulomb excitation with a {sup 208}Pb beam at energies above the Coulomb barrier. Data on a transfer channel leading to {sup 242}Pu were obtained as well. In the case of {sup 244}Pu, the yrast band was extended to 34{h_bar}, revealing the completed {pi}i{sub 13/2} alignment, a ''first'' for actinide nuclei. The yrast sequence of {sup 242}Pu was also extended to higher spin and a similar backbend was delineated. In contrast, while the ground state band of {sup 240}Pu was measured up to the highest rotational frequencies ever reported in the actinide region ({approximately} 300 keV), no sign of particle alignment was observed. In this case, several observables such as the large B(E1)/B(E2) branching ratios in the negative parity band, and the vanishing energy staggering between the negative and positive parity bands suggest that the strength of octupole correlations increases with rotational frequency. These stronger correlations may well be responsible for delaying or suppressing the {pi}i{sub 13/2} particle alignment.

  2. A fast semi-quantitative method for Plutonium determination in an alpine firn/ice core

    NASA Astrophysics Data System (ADS)

    Gabrieli, J.; Cozzi, G.; Vallelonga, P.; Schwikowski, M.; Sigl, M.; Boutron, C.; Barbante, C.

    2009-04-01

    Plutonium is present in the environment as a consequence of atmospheric nuclear tests carried out in the 1960s, nuclear weapons production and releases by the nuclear industry over the past 50 years. Plutonium, unlike uranium, is essentially anthropogenic and it was first produced and isolated in 1940 by deuteron bombardment of uranium in the cyclotron of Berkeley University. It exists in five main isotopes, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, derived from civilian and military sources (weapons production and detonation, nuclear reactors, nuclear accidents). In the environment, 239Pu is the most abundant isotope. Approximately 6 tons of 239Pu have been released into the environment as a result of 541 atmospheric weapon tests Nuclear Pu fallout has been studied in various environmental archives, such as sediments, soil and herbarium grass. Mid-latitude ice cores have been studied as well, on Mont Blanc, the Western Alps and on Belukha Glacier, Siberian Altai. We present a Pu record obtained by analyzing 52 discrete samples of an alpine firn/ice core from Colle Gnifetti (M. Rosa, 4450 m a.s.l.), dating from 1945 to 1991. The239Pu signal was recorded directly, without preliminary cleaning or preconcentration steps, using an ICP-SFMS (Thermo Element2) equipped with a desolvation system (APEX). 238UH+ interferences were negligible for U concentrations lower than 50 ppt as verified both in spiked fresh snow and pre-1940 ice samples. The shape of 239Pu profile reflects the three main periods of atmospheric nuclear weapons testing: the earliest peak starts in 1954/55 to 1958 and includes the first testing period which reached a maximum in 1958. Despite a temporary halt in testing in 1959/60, the Pu concentration decreased only by half with respect to the 1958 peak. In 1961/62 Pu concentrations rapidly increased reaching a maximum in 1963, which was about 40% more intense than the 1958 peak. After the sign of the "Limited Test Ban Treaty" between USA and URSS in 1964, Pu

  3. Polonium, uranium and plutonium radionuclides in aquatic and land ecosystem of Poland.

    PubMed

    Skwarzec, Bogdan; Strumińska-Parulska, Dagmara I; Boryło, Alicja; Kabat, Krzysztof

    2012-01-01

    This article presents the results of study about distribution, inflow and accumulation of polonium, uranium and plutonium in aquatic and land environment of Poland and the southern Baltic Sea. Radionuclides of (210)Po, (234)U and (238)U as well as (239+240)Pu and (241)Pu are strongly accumulated in Baltic organisms and plants and transferred through the trophic chain. The values of bioconcentration factor (BCF) in Baltic plants and animals are higher for polonium and plutonium in comparison with uranium. The principal source of radionuclides in the southern Baltic Sea is their inflow with rivers. Total annual runoff of polonium, uranium and plutonium from the Vistula and the Odra as well as the Pomeranian rivers were calculated at 95 GBq of (210)Po, 750 GBq of (234+238)U and 160 MBq of (238+239+240)Pu. Seasonal and spatial variability of (210)Po, (238)U and (239+240)Pu levels in the Vistula and the Odra drainage basins were assessed by application of neural-network based classification, especially cluster analysis (CA), principal component analysis (PCA) and self-organizing maps (SOM). The result for the Vistula river indicated correlation between polonium and plutonium as well as polonium and uranium. In the Odra drainage basin, the biggest differences were observed in the case of (238)U. To assess if there are statistically significant differences in mean concentration values of (210)Po, (238)U and (239+240)Pu for the Vistula and the Odra rivers drainage basins were obtained by used of the non-parametric tests. Comparing to the Vistula catchment area, statistically differences concentration of (210)Po and (239+240)Pu in all year was observed for river samples collected on the Odra drainage basin. PMID:22320701

  4. CALORIMETER-BASED ADJUSTMENT OF MULTIPLICITY DETERMINED 240PU EFF KNOWN-A ANALYSIS FOR THE ASSAY OF PLUTONIUM

    SciTech Connect

    Dubose, F.

    2012-02-21

    In nuclear material processing facilities, it is often necessary to balance the competing demands of accuracy and throughput. While passive neutron multiplicity counting is the preferred method for relatively fast assays of plutonium, the presence of low-Z impurities (fluorine, beryllium, etc.) rapidly erodes the assay precision of passive neutron counting techniques, frequently resulting in unacceptably large total measurement uncertainties. Conversely, while calorimeters are immune to these impurity effects, the long count times required for high accuracy can be a hindrance to efficiency. The higher uncertainties in passive neutron measurements of impure material are driven by the resulting large (>>2) {alpha}-values, defined as the ({alpha},n):spontaneous fission neutron emission ratio. To counter impurity impacts for high-{alpha} materials, a known-{alpha} approach may be adopted. In this method, {alpha} is determined for a single item using a combination of gamma-ray and calorimetric measurements. Because calorimetry is based on heat output, rather than a statistical distribution of emitted neutrons, an {alpha}-value determined in this way is far more accurate than one determined from passive neutron counts. This fixed {alpha} value can be used in conventional multiplicity analysis for any plutonium-bearing item having the same chemical composition and isotopic distribution as the original. With the results of single calorimeter/passive neutron/gamma-ray measurement, these subsequent items can then be assayed with high precision and accuracy in a relatively short time, despite the presence of impurities. A calorimeter-based known-{alpha} multiplicity analysis technique is especially useful when requiring rapid, high accuracy, high precision measurements of multiple plutonium bearing items having a common source. The technique has therefore found numerous applications at the Savannah River Site. In each case, a plutonium (or mixed U/Pu) bearing item is divided into multiple containers. A single item from that batch is then selected for both neutron and calorimetric measurements; all remaining items undergo a neutron measurement only. Using the technique mentioned above, the 'true' {alpha} value determined from the first (calorimeter and passive neutron measured) item is used in multiplicity analysis for all other items in the batch. The justification for using this {alpha} value in subsequent calculations is the assumption that the chemical composition and isotopic distribution of all batch items are the same, giving a constant ({alpha},n):spontaneous fission ratio. This analysis method has been successfully applied to the KIS Facility, significantly improving measurement uncertainties and reducing processing times for numerous items. Comprehensive plans were later developed to extend the use of this method to other applications, including the K-Area Shuffler and the H-Area Pu-Blending Project. While only the feasibility study for the Shuffler has been completed, implementation of the method in the H-Area Pu-Blending Project is currently in progress and has been successfully applied to multiple items. This report serves to document the details of this method in order to serve as a reference for future applications. Also contained herein are specific examples of the application of known-{alpha} multiplicity analysis.

  5. 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.

  6. Determination of plutonium in environmental samples by AMS and alpha spectrometry.

    PubMed

    Hrnecek, E; Steier, P; Wallner, A

    2005-01-01

    Environmental samples from nuclear weapons test sites at the atolls of Mururoa and Fangataufa (French Polynesia, south Pacific) have been analyzed for their content of plutonium isotopes by applying the independent techniques of decay counting (Alpha Spectrometry) and accelerator mass spectrometry (AMS). Here, we propose the combination of both techniques which results in a maximum of information on the isotopic signature of Pu in environmental samples. Plutonium was chemically separated from the bulk material by anion exchange. (242)Pu was used as an internal standard for both AMS and alpha spectrometry. The samples for alpha spectrometry were prepared by micro-precipitation with NdF(3). After alpha spectrometry, the samples were reprocessed for AMS. Pu was co-precipitated with Fe(OH)(3) and finally, solid samples were prepared. At the VERA (Vienna Environmental Research Accelerator) facility, the various Pu isotopes were separated by their isotopic masses and quantified by the AMS technique. A good agreement of the results obtained from the AMS measurements was found with those obtained from Alpha Spectrometry. Overall, the data agree on average within 10% of each other. Isotope ratios for (238)Pu, (239)Pu and (240)Pu can be extracted from our investigations. Alpha spectrometry delivers data for the (238)Pu and the combination of ((239+240))Pu concentrations in those samples. In addition, the AMS technique provides information on the individual concentrations of (240)Pu and (239)Pu. PMID:15982894

  7. Subthreshold Photofission of Even-Even Nuclei

    SciTech Connect

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

    2005-09-01

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

  8. Automated monitoring of in-process plutonium concentration

    SciTech Connect

    Rebagay, T.V.; Huff, G.A.; Hofstetter, K.J.

    1982-01-01

    An automated low-level plutonium monitor capable of measuring total and isotopic plutonium abundances in solutions is described. To demonstrate near real-time assay of in-process plutonium, we installed a monitor on a flowing stream of a laboratory experimental facility. The stream was composed of uranium and plutonium in nitric acid at concentrations typical of a plant using a Purex flowsheet modified to permit coprocessing of spent nuclear fuel. The plutonium isotopic abundances were typical of those found in light water reactor grade fuel. The plutonium isotopic concentrations in the stream with the exception of /sup 242/Pu were determined by direct lambda-ray spectrometry. The /sup 242/Pu abundance was calculated by isotope correlation techniques. Additional data were obtained on coprocessed uranium-plutonium solutions denatured with fission products (/sup 103/Ru, /sup 144/Ce//sup 144/Pr, and /sup 95/Zr//sup 95/Nb). /sup 239/Pu and /sup 240/Pu concentrations can be determined to within 2% and 5%, respectively, of the concentrations determined by mass spectrometry.

  9. 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. PMID:15167781

  10. Concurrent determination of 237Np and Pu isotopes using ICP-MS: analysis of NIST environmental matrix standard reference materials 4357, 1646a, and 2702.

    PubMed

    Matteson, Brent S; Hanson, Susan K; Miller, Jeffrey L; Oldham, Warren J

    2015-04-01

    An optimized method was developed to analyze environmental soil and sediment samples for (237)Np, (239)Pu, and (240)Pu by ICP-MS using a (242)Pu isotope dilution standard. The high yield, short time frame required for analysis, and the commercial availability of the (242)Pu tracer are significant advantages of the method. Control experiments designed to assess method uncertainty, including variation in inter-element fractionation that occurs during the purification protocol, suggest that the overall precision for measurements of (237)Np is typically on the order of ± 5%. Measurements of the (237)Np concentration in a Peruvian Soil blank (NIST SRM 4355) spiked with a known concentration of (237)Np tracer confirmed the accuracy of the method, agreeing well with the expected value. The method has been used to determine neptunium and plutonium concentrations in several environmental matrix standard reference materials available from NIST: SRM 4357 (Radioactivity Standard), SRM 1646a (Estuarine Sediment) and SRM 2702 (Inorganics in Marine Sediment). PMID:25644752

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

    PubMed

    Higgy, R H; Pimpl, M

    1998-12-01

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

  12. Monte Carlo simulation of transfer reactions using extended R-matrix theory picturing surrogate-type WFCF features

    NASA Astrophysics Data System (ADS)

    Bouland, Olivier H.

    2016-03-01

    This article supplies an overview of issues related to the interpretation of surrogate measurement results for neutron-incident cross section predictions; difficulties that are somehow masked by the historical conversion route based on Weisskopf-Ewing approximation. Our proposal is to handle the various difficulties by using a more rigorous approach relying on Monte Carlo simulation of transfer reactions with extended R-matrix theory. The multiple deficiencies of the historical surrogate treatment are recalled but only one is examined in some details here; meaning the calculation of in-out-going channel Width Fluctuation Correction Factors (WFCF) which behavior witness partly the failure of Niels Bohr's compound nucleus theoretical landmark. Relevant WFCF calculations according to neutron-induced surrogate- and cross section-types as a function of neutron-induced fluctuating energy range [0 - 2.1 MeV] are presented and commented in the case of the 240Pu* and 241Pu* compound nucleus isotopes.

  13. 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

  14. 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.

  15. Plutonium isotopes in the terrestrial environment at the Savannah River Site, USA: a long-term study.

    PubMed

    Armstrong, Christopher R; Nuessle, Patterson R; Brant, Heather A; Hall, Gregory; Halverson, Justin E; Cadieux, James R

    2015-02-01

    This work presents the findings of a long-term plutonium (Pu) study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at the Savannah River National Laboratory (SRNL) in the A-Area. Plutonium content and isotopic abundances were measured over this time period by α particle and thermal ionization mass spectrometry (3STIMS). We detail the complete process of the sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the (238)Pu/(239+240)Pu activity ratios attributed to SRS are substantially different than fallout due to past (238)Pu production on the site. The (240)Pu/(239)Pu atom ratios are reasonably consistent from year to year and are lower than fallout indicating an admixture of weapons-grade material, while the (242)Pu/(239)Pu atom ratios are higher than fallout values, again due to actinide production activities. Overall, the plutonium signatures obtained in this study reflect a distinctive mixture of weapons-grade, heat source, and higher burn-up plutonium with fallout material. This study provides a unique opportunity for developing and demonstrating a blue print for long-term low-level monitoring of trace plutonium in the environment. PMID:25535652

  16. Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study

    DOE PAGESBeta

    Armstrong, Christopher R.; Nuessle, Patterson R.; Brant, Heather A.; Hall, Gregory; Halverson, Justin E.; Cadieux, James R.

    2015-01-16

    This work presents the findings of a long term plutonium study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at Savannah River National Laboratory (SRNL) in A-area. Plutonium content and isotopic abundances were measured over this time period by alpha spectrometry and three stage thermal ionization mass spectrometry (3STIMS). Here we detail the complete sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the 238Pu/239+240Pu activity ratios attributed to SRS are abovemore » atmospheric global fallout ranges. The 240Pu/239Pu atom ratios are reasonably consistent from year to year and are lower than fallout, while the 242Pu/239Pu atom ratios are higher than fallout values. Overall, the plutonium signatures obtained in this study reflect a mixture of weapons-grade, higher burn-up, and fallout material. This study provides a blue print for long term low level monitoring of plutonium in the environment.« less

  17. Plutonium Detection with Straw Neutron Detectors

    SciTech Connect

    Mukhopadhyay, Sanjoy; Maurer, Richard; Guss, Paul

    2014-03-27

    A kilogram of weapons grade plutonium gives off about 56,000 neutrons per second of which 55,000 neutrons come from spontaneous fission of 240Pu (~6% by weight of the total plutonium). Actually, all even numbered isotopes (238Pu, 240Pu, and 242Pu) produce copious spontaneous fission neutrons. These neutrons induce fission in the surrounding fissile 239Pu with an approximate multiplication of a factor of ~1.9. This multiplication depends on the shape of the fissile materials and the surrounding material. These neutrons (typically of energy 2 MeV and air scattering mean free path >100 meters) can be detected 100 meters away from the source by vehicle-portable neutron detectors. [1] In our current studies on neutron detection techniques, without using 3He gas proportional counters, we designed and developed a portable high-efficiency neutron multiplicity counter using 10B-coated thin tubes called straws. The detector was designed to perform like commercially available fission meters (manufactured by Ortec Corp.) except instead of using 3He gas as a neutron conversion material, we used a thin coating of 10B.

  18. 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.

  19. 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. PMID:26651177

  20. Plutonium measurements by accelerator mass spectrometry at LLNL

    SciTech Connect

    McAninch, J E; Hamilton, T F; Broan, T A; Jokela, T A; Knezovich, T J; Ognibene, T J; Proctor, I D; Roberts, M L; Southon, J R; Vogel, J S; Sideras-Haddad, E

    1999-10-26

    Mass spectrometric methods provide sensitive, routine, and cost-effective analyses of long-lived radionuclides. Here the authors report on the status of work at Lawrence Livermore National Laboratory (LLNL) to develop a capability for actinide measurements by accelerator mass spectrometry (AMS) to take advantage of the high potential of AMS for rejection of interferences. This work demonstrates that the LLNL AMS spectrometer is well-suited for providing high sensitivity, robust, high throughput measurements of plutonium concentrations and isotope ratios. Present backgrounds are {approximately}2 x 10{sup 7}atoms per sample for environmental samples prepared using standard alpha spectrometry protocols. Recent measurements of {sup 239+240}Pu and {sup 241}Pu activities and {sup 240}Pu/{sup 239}Pu isotope ratios in IAEA reference materials agree well with IAEA reference values and with alpha spectrometry and recently published ICP-MS results. Ongoing upgrades of the AMS spectrometer are expected to reduce backgrounds below 1 x 10{sup 6} atoms per sample while allowing simplifications of the sample preparation chemistry. These simplifications will lead to lower per-sample costs, higher throughput, faster turn around and, ultimately, to larger and more robust data sets.

  1. Transuranic isotopes and 90Sr in attic dust in the vicinity of two nuclear establishments in northern Germany.

    PubMed

    Schmitz-Feuerhake, I; Mietelski, J W; Gaca, P

    2003-05-01

    Attic dust was chosen as the test medium in order to search for traces of man-made bone seeking alpha and beta emitters. The samples were taken from 5 houses in the community of Elbmarsch situated at the river Elbe, adjacent to the Krümmel nuclear power plant and the nuclear research center of Geesthacht. Five houses in other regions of northern Germany were taken as a control. 238Pu, (239,240)Pu, 241Am, and 244Cm were measured by alpha spectrometry after chemical separation. Additionally, 241Pu was measured by liquid scintillation spectrometry, and the fission product 90Sr was measured in a separate investigation. All nuclides except 244Cm showed activities above the detection limit in the Elbmarsch samples and an elevated mean concentration compared to the control. It can be concluded from the activity ratio 241Am/(239,240)Pu that the Elbmarsch contamination cannot be accounted for by the background levels of transuranic nuclides resulting from weapons fallout. The derived release of alpha emitters is assumed to have contributed to the induction of a leukemia cluster in children, which was observed in Elbmarsch between 1990 and 1996. PMID:12747479

  2. 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. PMID:26107287

  3. PLANTS AS BIO-MONITORS FOR 137CS, 238PU, 239, 240PU AND 40K AT THE SAVANNAH RIVER SITE

    SciTech Connect

    Caldwell, E.; Duff, M.; Ferguson, C.

    2010-12-16

    The nuclear fuel cycle generates a considerable amount of radioactive waste, which often includes nuclear fission products, such as strontium-90 ({sup 90}Sr) and cesium-137 ({sup 137}Cs), and actinides such as uranium (U) and plutonium (Pu). When released into the environment, large quantities of these radionuclides can present considerable problems to man and biota due to their radioactive nature and, in some cases as with the actinides, their chemical toxicity. Radionuclides are expected to decay at a known rate. Yet, research has shown the rate of elimination from an ecosystem to differ from the decay rate due to physical, chemical and biological processes that remove the contaminant or reduce its biological availability. Knowledge regarding the rate by which a contaminant is eliminated from an ecosystem (ecological half-life) is important for evaluating the duration and potential severity of risk. To better understand a contaminants impact on an environment, consideration should be given to plants. As primary producers, they represent an important mode of contamination transfer from sediments and soils into the food chain. Contaminants that are chemically and/or physically sequestered in a media are less likely to be bio-available to plants and therefore an ecosystem.

  4. Evidence for Hydroxamate Siderophores and Other N-Containing Organic Compounds Controlling (239,240)Pu Immobilization and Remobilization in a Wetland Sediment.

    PubMed

    Xu, Chen; Zhang, Saijin; Kaplan, Daniel I; Ho, Yi-Fang; Schwehr, Kathleen A; Roberts, Kimberly A; Chen, Hongmei; DiDonato, Nicole; Athon, Matthew; Hatcher, Patrick G; Santschi, Peter H

    2015-10-01

    Pu concentrations in wetland surface sediments collected downstream of a former nuclear processing facility in F-Area of the Savannah River Site (SRS), USA, were ∼2.5 times greater than those measured in the associated upland aquifer sediments; similarly, the Pu concentration solid/water ratios were orders of magnitude greater in the wetland than in the low-organic matter content aquifer soils. Sediment Pu concentrations were correlated to total organic carbon and total nitrogen contents and even more strongly to hydroxamate siderophore (HS) concentrations. The HS were detected in the particulate or colloidal phases of the sediments but not in the low molecular weight fractions (<1000 Da). Macromolecules which scavenged the majority of the potentially mobile Pu were further separated from the bulk mobile organic matter fraction ("water extract") via an isoelectric focusing experiment (IEF). An electrospray ionization Fourier-transform ion cyclotron resonance ultrahigh resolution mass spectrometry (ESI FTICR-MS) spectral comparison of the IEF extract and a siderophore standard (desferrioxamine; DFO) suggested the presence of HS functionalities in the IEF extract. This study suggests that while HS are a very minor component in the sediment particulate/colloidal fractions, their concentrations greatly exceed those of ambient Pu, and HS may play an especially important role in Pu immobilization/remobilization in wetland sediments. PMID:26313339

  5. R-matrix analysis of the {sup 240}Pu neutron cross sections in the thermal to 5700 eV energy range

    SciTech Connect

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

    1997-08-01

    Resonance analysis of high resolution neutron transmission data and of fission cross sections were performed in the neutron energy range from the thermal regions to 5,700 eV by using the Reich-Moore Bayesian code SAMMY. The experimental data base is described and the method of analysis is given. The experimental data were carefully examined in order to identify more resonances than those found in the current evaluated data files. The statistical properties of the resonance parameters are given. A new set of the average values of the parameters is proposed, which could be used for calculation of the average cross sections in the unresolved resonance region. The resonance parameters are available IN ENDF-6 format at the national or international data centers.

  6. The history and source of particulate 137Cs and 239,240Pu deposition in sediments of the Ob River Delta, Siberia.

    PubMed

    Sayles, F L; Livingston, H D; Panteleyev, G P

    1997-08-25

    This paper presents the first results of a project designed to examine the transfer of particle-associated artificial radionuclides down the Ob River in Siberia to its delta over the past 5 decades. The main sources include fallout from atmospheric nuclear weapons tests and weapons complexes and test sites of the Former Soviet Union in or near the Ob watershed. The approach is to measure the accumulation of the radionuclides in undisturbed delta sediments-obtaining a record of their deposition over time. These records were found in sediments of shallow lakes apart from, and connected to, the main channel. Sediment cores were collected in the summer of 1994 using a shallow draft catamaran to reach these lakes from a support ship in the main channel. Measurements are presented on the depth distributions of 137Cs and Pu isotopes and their inventories in a series of dated sediment cores-including one from a location in the Taz Estuary (which does not receive Ob River sediments). Sediment dating was carried out using the excess 210Pb technique. The results obtained are compared with known information on the temporal history of releases from the various sources and characteristics of the isotopic composition of the sources. The results show that good records of radionuclide deposition indicate that the major fraction of 137Cs and Pu isotopes deposited in these delta sediments comes from atmospheric nuclear weapons test fallout-both delivered directly from the atmosphere and from downstream transport of watershed sediments. No more than 25% of the observed inventories could be derived from other sources. PMID:9241876

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

    SciTech Connect

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

    1997-07-03

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

  8. Determination of Pu in urine at ultratrace level by sector field inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Zoriy, M. V.; Pickhardt, C.; Ostapczuk, P.; Hille, R.; Becker, J. S.

    2004-04-01

    A new analytical procedure has been developed for the determination of Pu in urine at the low ag ml-1 concentration level by double-focusing sector field inductively coupled plasma mass spectrometry (ICP-SFMS). One liter of urine doped with 4 pg 242Pu was analyzed after co-precipitation with Ca3(PO4)2 followed by extraction chromatography on TEVA resin in order to enrich the Pu and remove uranium and matrix elements. Figures of merit of ICP-SFMS for the determination of Pu were studied using two nebulizers, PFA-100 and direct injection high-efficiency nebulizer (DIHEN), for solution introduction with uptake rates of 0.58 and 0.06 ml min-1, respectively. The sensitivity for Pu in ICP-SFMS was determined to be 2000 and 1380 MHz ppm-1 for the PFA-100 and DIHEN nebulizers, respectively. Due to the low solution uptake rate of DIHEN the absolute sensitivity was about seven times better and yielded 1380 counts fg-1 in comparison to 207 counts fg-1 measured with the PFA-100 nebulizer. Recovery using 242Pu tracer was about 70%. The limits of detection for 239Pu in 1 l of urine, based on an enrichment factor of 100 for PFA-100 nebulizer and 1000 for DIHEN, were 9×10-18 and 1.02×10-18 g ml-1, respectively. Measurements of 240Pu/239Pu isotopic ratio in synthetically prepared urine standard solution yielded a precision of 1.8 and 1.9% and accuracy of 1.5 and 1.8% for the PFA-100 and DIHEN nebulizers, respectively.

  9. 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

  10. 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

    weapons testing at that time. The age results for this component are in agreement using both {sup 242}Pu and {sup 151}Sm normalizations, although the errors for the {sup 151}Sm correction are currently larger due to the greater uncertainty of their measurements. Additional efforts to develop a concordant {sup 241}Pu-{sup 241}Am dating method for environmental collections are underway with emphasis on soil cores.

  11. The use of non-destructive passive neutron measurement methods in dismantling and radioactive waste characterization

    SciTech Connect

    Jallu, F.; Allinei, P. G.; Bernard, P.; Loridon, J.; Soyer, P.; Pouyat, D.; Torreblanca, L.; Reneleau, A.

    2011-07-01

    The cleaning up and dismantling of nuclear facilities lead to a great volume of technological radioactive wastes which need to be characterized in order to be sent to the adequate final disposal or interim storage. The control and characterization can be performed with non-destructive nuclear measurements such as gamma-ray spectrometry. Passive neutron counting is an alternative when the alpha-gamma emitters cannot be detected due to the presence of a high gamma emission resulting from fission or activation products, or when the waste matrix is too absorbing for the gamma rays of interest (too dense and/or made of high atomic number elements). It can also be a complement to gamma-ray spectrometry when two measurement results must be confronted to improve the confidence in the activity assessment. Passive neutron assays involve the detection of spontaneous fission neutrons emitted by even nuclides ({sup 238}Pu, {sup 240}Pu, {sup 242}Pu, {sup 242}Cm, {sup 244}Cm...) and neutrons resulting from ({alpha}, n) reactions with light nuclides (O, F, Be...). The latter is conditioned by the presence of high {alpha}-activity radionuclides ({sup 234}U, {sup 238}Pu, {sup 240}Pu, {sup 241}Am...) and low-Z elements, which depends on the chemical form (metallic, oxide or fluorine) of the plutonium or uranium contaminant. This paper presents the recent application of passive neutron methods to the cleaning up of a nuclear facility located at CEA Cadarache (France), which concerns the Pu mass assessment of 2714 historic, 100 litre radioactive waste drums produced between 1980 and 1997. Another application is the dismantling and decommissioning of an uranium enrichment facility for military purposes, which involves the {sup 235}U and total uranium quantifications in about a thousand, large compressors employed in the gaseous diffusion enrichment process. (authors)

  12. Long-term development of the radionuclide exposure of murine rodent populations in Belarus after the Chernobyl accident.

    PubMed

    Ryabokon, N I; Smolich, I I; Kudryashov, V P; Goncharova, R I

    2005-12-01

    As a determinant of the associated health risks, the behavior of radionuclides in natural ecosystems needs to be better understood. Therefore, the activity concentration of various long-lived radionuclides released due to the Chernobyl accident, and the corresponding contributions to the whole-body dose rate, was studied as a function of time in mammalian indicator species inhabiting the natural forest ecosystems of Belarus, the bank vole (Clethrionomys glareolus) and the yellow-necked mouse (Apodemus flavicollus). The activity concentrations of 137Cs, 134Cs, 90Sr, 238Pu, 239,240Pu, 241Pu and 241Am in soil and in animals were measured at five monitoring sites with different ground deposition of radionuclides at different distances from the destroyed reactor. The observed temporal pattern of the radionuclide activity concentration in the studied animal populations reflects the changes in biological availability of these isotopes for biota, mostly due to fuel particle destruction and appearance of dissolved and exchangeable forms of radionuclides. The time course of 134+137Cs activity concentrations in animal populations appeared as a sequence of increase, peak and decrease. Maximal levels of radiocesium occurred 1-2 years after deposition, followed by an exponential decrease. Concentrations of incorporated 90Sr increased up to the tenth year after deposition. The activity concentrations of transuranic elements (238Pu, 239,240Pu, 241Pu and 241Am) were much lower than those of the other radionuclides, in the studied animals. A considerable activity of 241Am in animals from areas with high levels of contamination was firstly detected 5 years after deposition, it increased up to the tenth year and is expected to increase further in the future. Maximal values of the whole-body absorbed dose rates occurred during the year of deposition, followed by a decrease in the subsequent period. Generally, this decrease was monotonic, mainly determined by the decrease of the

  13. UPWARD MOVEMENT OF PLUTONIUM TO SURFACE SEDIMENTS DURING AN 11-YEAR FIELD STUDY

    SciTech Connect

    Kaplan, D.; Beals, D.; Cadieux, J.; Halverson, J.

    2010-01-25

    An 11-y lysimeter study was established to monitor the movement of Pu through vadose zone sediments. Sediment Pu concentrations as a function of depth indicated that some Pu moved upward from the buried source material. Subsequent numerical modeling suggested that the upward movement was largely the result of invading grasses taking up the Pu and translocating it upward. The objective of this study was to determine if the Pu of surface sediments originated from atmosphere fallout or from the buried lysimeter source material (weapons-grade Pu), providing additional evidence that plants were involved in the upward migration of Pu. The {sup 240}Pu/{sup 239}Pu and {sup 242}Pu/{sup 239}Pu atomic fraction ratios of the lysimeter surface sediments, as determined by Thermal Ionization Mass Spectroscopy (TIMS), were 0.063 and 0.00045, respectively; consistent with the signatures of the weapons-grade Pu. Our numerical simulations indicate that because plants create a large water flux, small concentrations over multiple years may result in a measurable accumulation of Pu on the ground surface. These results may have implications on the conceptual model for calculating risk associated with long-term stewardship and monitored natural attenuation management of Pu contaminated subsurface and surface sediments.

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

    PubMed

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

    2016-06-21

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

  15. Actinide Targets for Neutron Cross Section Measurements (C)

    SciTech Connect

    J. D. Baker; C. A. McGrath

    2006-04-01

    The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross-sections for certain "minor" actinides, those other than the most common (235U, 238U, and 239Pu). For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from “minor” actinides that currently have poorly known (n,g) and (n,f) cross sections. A program of measurements under AFCI has begun to correct this. One of the initial hurdles has been to produce well-characterized, highly isotopically enriched, and chemically pure actinide targets on thin backings. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched 240Pu, and 242Pu. Thus far, we have electrodeposited these actinide targets. In the future, we plan to study reductive distillation to achieve homogeneous, adherent targets on thin metal foils and polymer backings. As we move forward, separated isotopes become scarcer, and safety concerns become greater. The chemical purification and electodeposition techniques will be described.

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

    PubMed

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

    2013-11-19

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

  17. Separation Of Uranium And Plutonium Isotopes For Measurement By Multi Collector Inductively Coupled Plasma Mass Spectroscopy

    SciTech Connect

    Martinelli, R E; Hamilton, T F; Williams, R W; Kehl, S R

    2009-03-29

    Uranium (U) and plutonium (Pu) isotopes in coral soils, contaminated by nuclear weapons testing in the northern Marshall Islands, were isolated by ion-exchange chromatography and analyzed by mass spectrometry. The soil samples were spiked with {sup 233}U and {sup 242}Pu tracers, dissolved in minerals acids, and U and Pu isotopes isolated and purified on commercially available ion-exchange columns. The ion-exchange technique employed a TEVA{reg_sign} column coupled to a UTEVA{reg_sign} column. U and Pu isotope fractions were then further isolated using separate elution schemes, and the purified fractions containing U and Pu isotopes analyzed sequentially using multi-collector inductively coupled plasma mass spectrometer (MCICP-MS). High precision measurements of {sup 234}U/{sup 235}U, {sup 238}U/{sup 235}U, {sup 236}U/{sup 235}U, and {sup 240}Pu/{sup 239}Pu in soil samples were attained using the described methodology and instrumentation, and provide a basis for conducting more detailed assessments of the behavior and transfer of uranium and plutonium in the environment.

  18. Actinide Targets for Neutron Cross Section Measurements

    SciTech Connect

    John D. Baker; Christopher A. McGrath

    2006-10-01

    The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross-sections for certain "minor" actinides, those other than the most common (235U, 238U, and 239Pu). For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from "minor" actinides that currently have poorly known or in some cases not measured (n,?) and (n,f) cross sections. A program of measurements under AFCI has begun to correct this. One of the initial hurdles has been to produce well-characterized, highly isotopically enriched, and chemically pure actinide targets on thin backings. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched 239Pu, 240Pu, and 242Pu. Thus far, we have electrodeposited these actinide targets. In the future, we plan to study reductive distillation to achieve homogeneous, adherent targets on thin metal foils and polymer backings. As we move forward, separated isotopes become scarcer, and safety concerns become greater. The chemical purification and electodeposition techniques will be described.

  19. 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.

  20. Upward movement of plutonium to surface sediments during an 11-year field study.

    PubMed

    Kaplan, D I; Demirkanli, D I; Molz, F J; Beals, D M; Cadieux, J R; Halverson, J E

    2010-05-01

    An 11-year lysimeter study was established to monitor the movement of Pu through vadose zone sediments. Sediment Pu concentrations as a function of depth indicated that some Pu moved upward from the buried source material. Subsequent numerical modeling suggested that the upward movement was largely the result of invading grasses taking up the Pu and translocating it upward. The objective of this study was to determine if the Pu of surface sediments originated from atmosphere fallout or from the buried lysimeter source material (weapons-grade Pu), providing additional evidence that plants were involved in the upward migration of Pu. The (240)Pu/(239)Pu and (242)Pu/(239)Pu atomic fraction ratios of the lysimeter surface sediments, as determined by Thermal Ionization Mass Spectroscopy (TIMS), were 0.063 and 0.00045, respectively; consistent with the signatures of the weapons-grade Pu. Our numerical simulations indicate that because plants create a large water flux, small concentrations over multiple years may result in a measurable accumulation of Pu on the ground surface. These results may have implications on the conceptual model for calculating risk associated with long-term stewardship and monitored natural attenuation management of Pu contaminated subsurface and surface sediments. PMID:20227801

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

    SciTech Connect

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

    2009-01-01

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

  2. Verification of a Depletion Method in SCALE for the Advanced High Temperature Reactor

    SciTech Connect

    KELLY, RYAN; Ilas, Dan

    2012-01-01

    This study describes a new method utilizing the Dancoff factor to model a non-standard TRISO fuel form characteristic of the AHTR reactor design concept for depletion analysis using the TRITON sequence of SCALE and the validation of this method by code-to-code comparisons. The fuel used in AHTR has the TRISO particles concentrated along the edges of a slab fuel element. This particular geometry prevented the use of a standard DOUBLEHET treatment, previously developed in SCALE to handle NGNP-designed fuel. The new method permits fuel depletion on complicated geometries that traditionally can be handled only by continuous energy based depletion code systems. The method was initially tested on a fuel design typical of the NGNP, where the DOUBLEHET treatment is available. A more comprehensive study was performed using the VESTA code that uses the continuous energy MCNP5 code as a transport solver and ORIGEN2.2 code for depletion calculations. Comparisons of the results indicate good agreement of whole core characteristics, such as the multiplication factor, and the isotopics, including their spatial distribution. Key isotopes analyzed included 235U, 239Pu, 240Pu and 241Pu. The results from this study indicate that the Dancoff factor method can generate estimates of core characteristics with reasonable precision for scoping studies of configurations where the DOUBLEHET treatment is unavailable.

  3. Verification of a Depletion Method in SCALE for the Advanced High Temperature Reactor

    SciTech Connect

    KELLY, RYAN; Ilas, Dan

    2013-01-01

    This study describes a new approach employing the Dancoff correction method to model the TRISO-based fuel form used by the Advanced High-Temperature Reactor (AHTR) reactor design concept. The Dancoff correction method is used to perform isotope depletion analysis using the TRITON sequence of SCALE and is verified by code-to-code comparisons. The current AHTR fuel design has TRISO particles concentrated along the edges of a slab fuel element. This geometry prevented the use of the DOUBLEHET treatment, previously developed in SCALE to model spherical and cylindrical fuel. The new method permits fuel depletion on complicated geometries that traditionally can be handled only by continuous energy based depletion code systems. The method was initially tested on a fuel configuration typical of the Next Generation Nuclear Plant (NGNP), where DOUBLEHET treatment is possible. A confirmatory study was performed on the AHTR reference core geometry using the VESTA code, which uses the continuous energy MCNP5 code as a transport solver and ORIGEN2.2 code for depletion calculations. Comparisons of the results indicate good agreement of whole core characteristics, such as the multiplication factor and the isotopics, including their spatial distribution. Key isotopes analyzed included 235U, 239Pu, 240Pu, and 241Pu. The results from this study indicate that the Dancoff factor method can generate estimates of core characteristics with reasonable precision for scoping studies of configurations where DOUBLEHET treatment cannot be performed.

  4. Neutronic Benchmarks for the Utilization of Mixed-Oxide Fuel: Joint U.S./Russian Progress Report for Fiscal Year 1997 - Volume 4, Part 2--Saxton Plutonium Program Critical Experiments

    SciTech Connect

    Abdurrahman, NM

    2000-10-12

    Critical experiments with water-moderated, single-region PuO{sub 2}-UO{sub 2} or UO{sub 2}, and multiple-region PuO{sub 2}-UO{sub 2}- and UO{sub 2}-fueled cores were performed at the CRX reactor critical facility at the Westinghouse Reactor Evaluation Center (WREC) at Waltz Mill, Pennsylvania in 1965 [1]. These critical experiments were part of the Saxton Plutonium Program. The mixed oxide (MOX) fuel used in these critical experiments and then loaded in the Saxton reactor contained 6.6 wt% PuO{sub 2} in a mixture of PuO{sub 2} and natural UO{sub 2}. The Pu metal had the following isotopic mass percentages: 90.50% {sup 239}Pu; 8.57% {sup 239}Pu; 0.89% {sup 240}Pu; and 0.04% {sup 241}Pu. The purpose of these critical experiments was to verify the nuclear design of Saxton partial plutonium cores while obtaining parameters of fundamental significance such as buckling, control rod worth, soluble poison worth, flux, power peaking, relative pin power, and power sharing factors of MOX and UO{sub 2} lattices. For comparison purposes, the core was also loaded with uranium dioxide fuel rods only. This series is covered by experiments beginning with the designation SX.

  5. Compilation of fission product yields Vallecitos Nuclear Center

    SciTech Connect

    Rider, B.F.

    1980-01-01

    This document is the ninth in a series of compilations of fission yield data made at Vallecitos Nuclear Center in which fission yield measurements reported in the open literature and calculated charge distributions have been utilized to produce a recommended set of yields for the known fission products. The original data with reference sources, as well as the recommended yields are presented in tabular form for the fissionable nuclides U-235, Pu-239, Pu-241, and U-233 at thermal neutron energies; for U-235, U-238, Pu-239, and Th-232 at fission spectrum energies; and U-235 and U-238 at 14 MeV. In addition, U-233, U-236, Pu-240, Pu-241, Pu-242, Np-237 at fission spectrum energies; U-233, Pu-239, Th-232 at 14 MeV and Cf-252 spontaneous fission are similarly treated. For 1979 U234F, U237F, Pu249H, U234He, U236He, Pu238F, Am241F, Am243F, Np238F, and Cm242F yields were evaluated. In 1980, Th227T, Th229T, Pa231F, Am241T, Am241H, Am242Mt, Cm245T, Cf249T, Cf251T, and Es254T are also evaluated.

  6. Concentration and speciation of plutonium, americium, uranium, thorium, potassium and 137Cs in a venice canal sediment sample

    NASA Astrophysics Data System (ADS)

    Testa, C.; Desideri, D.; Guerra, F.; Meli, M. A.; Roselli, C.; Degetto, S.

    1999-01-01

    A sequential extraction method consisting of six operationally-defined fractions has been developed for determining the geochemical partitioning of natural (U, Th, 40K) and antropogenic (Pu, Am, 137Cs) radionuclides in a 40 50 cm deep sediment sample collected in a Venice canal. Extraction chromatography with Microthene-TOPO (U, Th), Microthene-TNOA (Pu) and Microthene-HDEHP (Am) column was used for the chemical separation of a single radionuclide; the final recoveries were calculated by adding 236U, 229Th, 242Pu and 243Am as the yield tracers. After electrodeposition the alpha spectrometry was carried out. 137Cs and 40K were measured by gamma spectrometry. The total concentrations in the wet sample (Bq/kgd), obtained by a complete disgregation of the matrix by wet and dry treatment, were the following: 239+240Pu=1.03±0.07, 238Pu=0.022±0.005, 241Am=0.337±0.027, 137Cs=9.78±0.78, 238U=28.84±1.62, 232Th=21.42±1.93, 40K=376.05±12.78. The mean ratio 238Pu/239+240Pu (0.02) shows a contamination due essentially to fall-out and U and Th alpha spectra indicate the natural origin of two elements. The absence of 134Cs in the sample proves that at 40 50 cm depth the sediment was not affected by the Chernobyl fall-out. As far as the speciation is concerned the following fractions were considered: water soluble, carbonates, Fe-Mn oxides, organic matter, acid soluble, residue. Pu (˜67%) an Am (˜95%) were present principally in the carbonate fraction; U was more distributed and about 30% and 45% appeared in the carbonate fraction and in the residue respectively; the majority of Th was present in the residue (˜60%); 40K was totally present in the residue; finally 137Cs was found mostly in the acid soluble fraction (˜53%) and in the residue (˜47%). Some stable elements (Fe, Mn, Al, Ti, Ca, Pb, Ba) were also determined in the different fractions to get more information about the chemical association of the single radionuclides.

  7. Concentration and speciation of plutonium, americium, uranium, thorium, potassium and 137Cs in a venice canal sediment sample

    NASA Astrophysics Data System (ADS)

    Testa, C.; Desideri, D.; Guerra, F.; Meli, M. A.; Roselli, C.; Degetto, S.

    1999-01-01

    A sequential extraction method consisting of six operationally-defined fractions has been developed for determining the geochemical partitioning of natural (U, Th, 40K) and antropogenic (Pu, Am, 137Cs) radionuclides in a 40-50 cm deep sediment sample collected in a Venice canal. Extraction chromatography with Microthene-TOPO (U, Th), Microthene-TNOA (Pu) and Microthene-HDEHP (Am) column was used for the chemical separation of a single radionuclide; the final recoveries were calculated by adding 236U, 229Th, 242Pu and 243Am as the yield tracers. After electrodeposition the alpha spectrometry was carried out. 137Cs and 40K were measured by gamma spectrometry. The total concentrations in the wet sample (Bq/kgd), obtained by a complete disgregation of the matrix by wet and dry treatment, were the following: 239+240Pu=1.03±0.07, 238Pu=0.022±0.005, 241Am=0.337±0.027, 137Cs=9.78±0.78, 238U=28.84±1.62, 232Th=21.42±1.93, 40K=376.05±12.78. The mean ratio 238Pu/239+240Pu (0.02) shows a contamination due essentially to fall-out and U and Th alpha spectra indicate the natural origin of two elements. The absence of 134Cs in the sample proves that at 40-50 cm depth the sediment was not affected by the Chernobyl fall-out. As far as the speciation is concerned the following fractions were considered: water soluble, carbonates, Fe-Mn oxides, organic matter, acid soluble, residue. Pu (˜67%) an Am (˜95%) were present principally in the carbonate fraction; U was more distributed and about 30% and 45% appeared in the carbonate fraction and in the residue respectively; the majority of Th was present in the residue (˜60%); 40K was totally present in the residue; finally 137Cs was found mostly in the acid soluble fraction (˜53%) and in the residue (˜47%). Some stable elements (Fe, Mn, Al, Ti, Ca, Pb, Ba) were also determined in the different fractions to get more information about the chemical association of the single radionuclides.

  8. Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY11 Status Report

    SciTech Connect

    Kulisek, Jonathan A.; Anderson, Kevin K.; Bowyer, Sonya M.; Casella, Andrew M.; Gesh, Christopher J.; Warren, Glen A.

    2011-09-30

    Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration, of which PNNL is a part, to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of today's confirmatory assay methods. This document is a progress report for FY2011 PNNL analysis and algorithm development. Progress made by PNNL in FY2011 continues to indicate the promise of LSDS analysis and algorithms applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model, which accounts for self-shielding effects using empirical basis vectors calculated from the singular value decomposition (SVD) of a matrix containing the true self-shielding functions of the used fuel assembly models. The potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space was demonstrated. Also, in FY2011, PNNL continued to develop an analytical model. Such efforts included the addition of six more non-fissile absorbers in the analytical shielding function and the non-uniformity of the neutron flux across the LSDS assay chamber. A hybrid analytical-empirical approach was developed to determine the mass of total Pu (sum of the masses of 239Pu, 240Pu, and 241Pu), which is an important quantity in safeguards. Results using this hybrid method were of approximately the same accuracy as the pure

  9. LOS ALAMOS NEUTRON SCIENCE CENTER CONTRIBUTIONS TO THE DEVELOPMENT OF FUTURE POWER REACTORS

    SciTech Connect

    GAVRON, VICTOR I.; HILL, TONY S.; PITCHER, ERIC J.; TOVESSON, FREDERIK K.

    2007-01-09

    The Los Alamos Neutron Science Center (LANSCE) is a large spallation neutron complex centered around an 800 MeV high-currently proton accelerator. Existing facilities include a highly-moderated neutron facility (Lujan Center) where neutrons between thermal and keV energies are produced, and the Weapons Neutron Research Center (WNR), where a bare spallation target produces neutrons between 0.1 and several hundred MeV.The LANSCE facility offers a unique capability to provide high precision nuclear data over a large energy region, including that for fast reactor systems. In an ongoing experimental program the fission and capture cross sections are being measured for a number of minor actinides relevant for Generation-IV reactors and transmutation technology. Fission experiments makes use of both the highly moderated spallation neutron spectrum at the Lujan Center, and the unmoderated high energy spectrum at WNR. By combininb measurements at these two facilities the differential fission cross section is measured relative to the {sup 235}U(n,f) standard from subthermal energies up to about 200 MeV. An elaborate data acquisition system is designed to deal with all the different types of background present when spanning 10 energy decades. The first isotope to be measured was {sup 237}Np, and the results were used to improve the current ENDF/B-VII evaluation. Partial results have also been obtained for {sup 240}Pu and {sup 242}Pu, and the final results are expected shortly. Capture cross sections are measured at LANSCE using the Detector for Advanced Neutron Capture Experiments (DANCE). This unique instrument is highly efficient in detecting radiative capture events, and can thus handle radioactive samples of half-lives as low as 100 years. A number of capture cross sections important to fast reaction applications have been measured with DANCE. The first measurement was on {sup 237}Np(n,{gamma}), and the results have been submitted for publication. Other capture

  10. Application of wavelet scaling function expansion continuous-energy resonance calculation method to MOX fuel problem

    SciTech Connect

    Yang, W.; Wu, H.; Cao, L.

    2012-07-01

    More and more MOX fuels are used in all over the world in the past several decades. Compared with UO{sub 2} fuel, it contains some new features. For example, the neutron spectrum is harder and more resonance interference effects within the resonance energy range are introduced because of more resonant nuclides contained in the MOX fuel. In this paper, the wavelets scaling function expansion method is applied to study the resonance behavior of plutonium isotopes within MOX fuel. Wavelets scaling function expansion continuous-energy self-shielding method is developed recently. It has been validated and verified by comparison to Monte Carlo calculations. In this method, the continuous-energy cross-sections are utilized within resonance energy, which means that it's capable to solve problems with serious resonance interference effects without iteration calculations. Therefore, this method adapts to treat the MOX fuel resonance calculation problem natively. Furthermore, plutonium isotopes have fierce oscillations of total cross-section within thermal energy range, especially for {sup 240}Pu and {sup 242}Pu. To take thermal resonance effect of plutonium isotopes into consideration the wavelet scaling function expansion continuous-energy resonance calculation code WAVERESON is enhanced by applying the free gas scattering kernel to obtain the continuous-energy scattering source within thermal energy range (2.1 eV to 4.0 eV) contrasting against the resonance energy range in which the elastic scattering kernel is utilized. Finally, all of the calculation results of WAVERESON are compared with MCNP calculation. (authors)

  11. A comprehensive appraisal of 241Am in soils around Rocky Flats, Colorado.

    PubMed

    Litaor, M I; Allen, L

    1996-09-01

    Soils east of Rocky Flats Plant (RFETS) near Golden, Colorado, were contaminated with actinides because of accidental release of oils laden with plutonium isotopes. Consequently, these soils were contaminated by 241Am due to radioactive decay of 241Pu (t1/2 = 14.4 y). A spatial analysis of 241Am activity in soils east of RFETS was conducted to elucidate the magnitude and the mode of 241Am dispersion in the soil environment. 241Am activity of 178 soil samples ranged from 0.037 Bq kg-1 to 10,004 Bq kg-1 with a mean of 214 Bq kg-1, median of 7.28 Bq kg-1, standard deviation of 942 Bq kg-1, and a coefficient of variation of 4.3. Spatial analysis of 241Am in soils around RFETS was conducted using indicator kriging, which is a nonparametric technique especially suitable to model a conditional cumulative distribution function (ccdf) of highly skewed environmental data such as 241Am. The ccdf was used to generate an E-type (mean of the conditional cdf) surface. The resulted surfaces were consistent with the hypothesis that the westerly winds were the dominant mechanism of americium dispersal. The spatial distribution and dispersal mechanisms of 241Am were similar to those of 239+240Pu. The ccdf was also used to construct probability of exceedence maps of 241Am in soils. For the purpose of this report two threshold values for the probability maps were selected: (1) the mean measured background activity of 241Am (0.4 Bq kg-1), and (2) the programmatic preliminary remediation goal for residential occupancy scenario (87.7 Bq kg-1). The probability-of-exceedance maps provide estimates of spatial uncertainty associated with each threshold. The E-type maps in conjunction with the probability-of-exceedance maps provide a robust framework for future cleanup options and land use decisions. PMID:8698577

  12. Performance assessment requirements for the identification and tracking of transuranic waste intended for disposal at the Waste Isolation Pilot Plant

    SciTech Connect

    Snider, C.A.; Weston, W.W.

    1997-11-01

    To demonstrate compliance with environmental radiation protection standards for management and disposal of transuranic (TRU) radioactive wastes, a performance assessment (PA) of the Waste Isolation Pilot Plant (WIPP) was made of waste-waste and waste-repository interactions and impacts on disposal system performance. An estimate of waste components and accumulated quantities was derived from a roll-up of the generator/storage sites` TRU waste inventories. Waste components of significance, and some of negligible effect, were fixed input parameters in the model. The results identified several waste components that require identification and tracking of quantities to ensure that repository limits are not exceeded. The rationale used to establish waste component limits based on input estimates is discussed. The distinction between repository limits and waste container limits is explained. Controls used to ensure that no limits are exceeded are identified. For waste components with no explicit repository based limits, other applicable limits are contained in the WIPP Waste Acceptance Criteria (WAC). The 10 radionuclides targeted for identification and tracking on either a waste container or a waste stream basis include Am-241, Pu-238, Pu-239, Pu-240, Pu-242, U-233, U-234, U-238, Sr-90, and Cs-137. The accumulative activities of these radionuclides are to be inventoried at the time of emplacement in the WIPP. Changes in inventory curie content as a function of radionuclide decay and ingrowth over time will be calculated and tracked. Due to the large margin of compliance demonstrated by PA with the 10,000 year release limits specified, the quality assurance objective for radioassay of the 10 radionuclides need to be no more restrictive than those already identified for addressing the requirements imposed by transportation and WIPP disposal operations in Section 9 of the TRU Waste Characterization Quality Assurance Program Plan. 6 refs.

  13. Airborne Plutonium and non-natural Uranium from the Fukushima DNPP found at 120 km distance a few days after reactor hydrogen explosions.

    PubMed

    Shinonaga, Taeko; Steier, Peter; Lagos, Markus; Ohkura, Takehisa

    2014-04-01

    Plutonium (Pu) and non-natural uranium (U) originating from the Fukushima Daiichi Nuclear Power Plant (FDNPP) were identified in the atmosphere at 120 km distance from the FDNPP analyzing the ratio of number of atoms, following written as n(isotope)/n(isotope), of Pu and U. The n((240)Pu)/n((239)Pu), n((241)Pu)/n((239)Pu), n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U) in aerosol samples collected before and after the FDNPP incident were analyzed by accelerator mass spectrometry (AMS) and inductively coupled plasma mass spectrometry (ICPMS). The activity concentrations of (137)Cs and (134)Cs in the same samples were also analyzed by gamma spectrometry before the destructive analysis. Comparing the time series of analytical data on Pu and U obtained in this study with previously reported data on Pu, U, and radioactive Cs, we concluded that Pu and non-natural U from the FDNPP were transported in the atmosphere directly over a 120 km distance by aerosol and wind within a few days after the reactor hydrogen explosions. Effective dose of Pu were calculated using the data of Pu: (130 ± 21) nBq/m(3), obtained in this study. We found that the airborne Pu contributes only negligibly to the total dose at the time of the incident. However the analytical results show that the amount of Pu and non-natural U certainly increased in the environment after the incident. PMID:24621142

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

    SciTech Connect

    Younes, W; Britt, H C

    2003-03-31

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

  15. LLD Determination for PFP Residues Using the ANTECH Calorimeters

    SciTech Connect

    WESTSIK, G.A.

    2003-07-07

    The Plutonium Finishing Plant (PFP) facility performs waste characterization measurements for disposal of transuranic waste (TRU) at the Waste Isolation Pilot Plant (WIPP). The WIPP's performance assessment requires monitoring and tracking of the following ten radionuclides in the waste that is accepted and disposed of at the WIPP facility. Activities and mass values must be reported for: {sup 241}Am, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu, {sup 242}Pu, {sup 233}U, {sup 234}U, {sup 238}U, {sup 90}Sr and {sup 137}Cs on a payload container basis. In addition the system must be able to report other nuclides, which contribute to the FGE, decay heat or contribute to more than 95% of the total radiological hazard. PFP reports the activity and mass of these radionuclides when positively identified in any waste container. In situations where one of the 10 WIPP tracked radionuclides is not positively identified on a PFP assay, PFP either reports a ''zero'', indicating the nuclide was not positively identified in the waste assay and is not identified by the acceptable knowledge (AK), or ''

  16. Multipurpose Radiation Resistant Semiconductor Detectors for Alpha, Neutron & Low Energy Gamma Ray Measurements at High Temperatures in High-Intensity Gamma Ray

    SciTech Connect

    Ruddy, Frank H.

    2005-06-01

    Work scheduled under year two of DOE Grant DE-FG02-04ER63734 is on schedule and all year-two milestones have or will be met. Results to date demonstrate that unprecedented silicon carbide (SiC) energy resolution has been obtained, and that SiC detectors may achieve energy resolution that exceeds that obtainable with the best silicon alpha spectrometers. Fast-neutron energy spectrometry measurements indicate that recoil-ion energy spectrometry should be possible with SiC detectors. Furthermore, SiC detectors have been demonstrated to perform well even after gamma-ray exposures of 1.E09 Rad. This result and the previously demonstrated capability of SiC detectors to operate in elevated-temperature environments are very promising for potential DOE EMSP applications. A new class of multipurpose, radiation-resistant semiconductor detectors that can be used in elevated-temperature and high-radiation environments is being developed under this grant. These detectors, based on silicon carbide (SiC) semiconductor are designed to have larger active volumes than previously available SiC detectors, and are being tested for their response to alpha particles, X-rays and low energy gamma rays, and fast neutrons. Specifically, SiC radiation detectors with larger areas and 100-micrometer thick active regions have been designed and manufactured according to detector-design specifications. Detectors based on a Schottky diode design were specified in order to minimize the effects of the detector entrance window on alpha particle measurements. During manufacture of the Schottky diodes, the manufacturer also provided a set of large-volume SiC p-i-n diodes for testing Extensive alpha particle measurements have been carried out to test and quantify the response of the SiC Schottky diodes. Exposures to 148-Gd, 213-Po, 217-At, 221-Fr, 225-Ac, 237-Np, 238-Pu, 240-Pu, and 242-Pu sources were used to obtain detailed alpha response data in the alpha energy range from 3182.787 keV to 8375.9 ke

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

    SciTech Connect

    None, None

    1997-04-01

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

  18. Very High Temperature Reactor (VHTR) Deep Burn Core and Fuel Analysis -- Complete Design Selection for the Pebble Bed Reactor

    SciTech Connect

    B. Boer; A. M. Ougouag

    2010-09-01

    The Deep-Burn (DB) concept focuses on the destruction of transuranic nuclides from used light water reactor fuel. These transuranic nuclides are incorporated into TRISO coated fuel particles and used in gas-cooled reactors with the aim of a fractional fuel burnup of 60 to 70% in fissions per initial metal atom (FIMA). This high performance is expected through the use of multiple recirculation passes of the fuel in pebble form without any physical or chemical changes between passes. In particular, the concept does not call for reprocessing of the fuel between passes. In principle, the DB pebble bed concept employs the same reactor designs as the presently envisioned low-enriched uranium core designs, such as the 400 MWth Pebble Bed Modular Reactor (PBMR-400). Although it has been shown in the previous Fiscal Year (2009) that a PuO2 fueled pebble bed reactor concept is viable, achieving a high fuel burnup, while remaining within safety-imposed prescribed operational limits for fuel temperature, power peaking and temperature reactivity feedback coefficients for the entire temperature range, is challenging. The presence of the isotopes 239-Pu, 240-Pu and 241-Pu that have resonances in the thermal energy range significantly modifies the neutron thermal energy spectrum as compared to a ”standard,” UO2-fueled core. Therefore, the DB pebble bed core exhibits a relatively hard neutron energy spectrum. However, regions within the pebble bed that are near the graphite reflectors experience a locally softer spectrum. This can lead to power and temperature peaking in these regions. Furthermore, a shift of the thermal energy spectrum with increasing temperature can lead to increased absorption in the resonances of the fissile Pu isotopes. This can lead to a positive temperature reactivity coefficient for the graphite moderator under certain operating conditions. The effort of this task in FY 2010 has focused on the optimization of the core to maximize the pebble discharge

  19. Combined use of medium mass resolution and desolvation introduction system for accurate plutonium determination in the femtogram range by inductively coupled plasma-sector-field mass spectrometry

    NASA Astrophysics Data System (ADS)

    Pointurier, Fabien; Pottin, Anne-Claire; Hémet, Philippe; Hubert, Amélie

    2011-03-01

    Formation of a polyatomic species made of an atom of a heavy element like lead, mercury or iridium, and atoms abundant in plasma (argon, nitrogen, oxygen, and hydrogen) when using an inductively coupled plasma-sector-field mass spectrometer (ICP-SFMS) may lead to false detection of femtograms (fg) of plutonium or bias in the measured concentrations. Mathematical corrections, based on the measurement of heavy element concentrations in the sample solutions and determination of the extents of formation of the polyatomic interferences, are efficient but time-consuming and degrade detection limits. We describe and discuss a new method based on the combination of, on the one hand, medium mass resolution (MR) of the ICP-SFMS to separate plutonium isotopes physically from interfering polyatomic species, and, on the other, use of a desolvation introduction system (DIS) to enhance sensitivity, thus partly compensating for the loss of transmission due to use of a higher resolution. Plutonium peaks are perfectly separated from the major interfering species (PbO 2, HgAr, and IrO 3) with a mass resolution of ~ 4000. The resulting nine-fold transmission loss is partly compensated by a five-fold increase in sensitivity obtained with the DIS and a lower background. The instrumental detection limits for plutonium isotopes, calculated for measurements of pure synthetic solutions, of the new method (known as MR-DIS method) and of the one currently used in the laboratory (LR method), based on a low mass resolution equal to 360, a microconcentric nebulizer and two in-line cooled spray chambers, are roughly equivalent, at around 0.2 fg ml - 1 . Regarding the measurement of real-life samples, the results obtained with both methods agree and the corresponding analytical detection limits for plutonium isotopes 239Pu, 240Pu and 241Pu are of a few fg·ml - 1 of sample solution, slightly lower with the MR-DIS method than with the current LR method. Although less sensitive than other plutonium

  20. Corrections for Exchange and Screening Effects in Low-energy Beta Decays

    SciTech Connect

    Mougeot, X. Bé, M.-M.; Bisch, C.; Loidl, M.

    2014-06-15

    The beta spectra of {sup 241}Pu and {sup 63}Ni have been recently measured using metallic magnetic calorimeters. This powerful experimental technique allows theoretical beta spectra calculations to be tested at low energy with an accuracy never before achievable. Their comparison with classical beta calculations exhibits a significant deviation below 4 keV for {sup 241}Pu and 8 keV for {sup 63}Ni. The atomic exchange effect explains the main part of this deviation in the {sup 63}Ni beta spectrum. This effect has a significant contribution, equivalent to the magnitude of the screening, in the {sup 241}Pu beta spectrum.

  1. Improved methods of measurement and analysis of conversion electron and beta-particle spectra

    PubMed

    Dragoun; Spalek; Rysavy; Kovalik; Yakushev; Brabec; Frana; Venos

    2000-03-01

    A general statistical test of the stability of measurement conditions was demonstrated on the beta-spectra of 241Pu cumulated during four years. The alpha- and gamma-ray spectroscopy indicated stability of the 241Pu source. Monte Carlo modelling of individual collision events clarified the role of electron scattering and energy losses within a radioactive source down to energies of several hundreds of eV. The impact ionization by beta-particles of carbon and oxygen atoms in a surface contamination layer on the 241Pu and 63Ni sources was observed. PMID:10724379

  2. Contributions of Rocky Flats releases to the total plutonium in regional soils.

    PubMed

    Ibrahim, S A; Webb, S B; Whicker, F W

    1997-01-01

    Total 239,240Pu and the 240Pu:239Pu atom ratio were measured in soil samples from around the Rocky Flats Environmental Technology Site (RFETS) during 1992-1994. Mass isotopic data provided a sensitive technique to resolve low levels of RFETS 239,240Pu superimposed on plutonium from global fallout. Concentrations of 239,240Pu within this sample set ranged from 1.1 Bq kg(-1) offsite to 57 Bq kg(-1) onsite, and the 240Pu:239Pu atom ratio increased from 0.055 onsite to 0.123 at approximately 19 km east of the RFETS boundary. The relationship between 24OPu:239Pu atom ratios and distance indicated that a measurable RFETS contribution may have extended to > or = 19 km offsite in the easterly direction. Although the RFETS contribution to total plutonium at the offsite locations ranged from 24-90%, the overall inventory was relatively small. Total inventory estimates, for one transect, based on 239,240Pu and from 240Pu:239Pu atom ratio measurements were not significantly different. PMID:8972825

  3. Sources of plutonium to the tropical Northwest Pacific Ocean (1943-1999) identified using a natural coral archive

    NASA Astrophysics Data System (ADS)

    Lindahl, Patric; Asami, Ryuji; Iryu, Yasufumi; Worsfold, Paul; Keith-Roach, Miranda; Choi, Min-Seok

    2011-03-01

    The Pu isotopes, 239Pu and 240Pu, were determined in annually-banded skeletons of an accurately dated (1943-1999) modern coral ( Porites lobata) from Guam Island to identify historical Pu sources to the tropical Northwest Pacific Ocean. Activity concentrations of 239+240Pu and 240Pu/ 239Pu atom ratios were determined in the dated coral bands using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands and global fallout were identified as the two main sources. The Guam site was dominated by PPG close-in fallout in the 1950s, with an average 240Pu/ 239Pu atom ratio of 0.315 ± 0.005. In addition, a higher 240Pu/ 239Pu atom ratio (0.456 ± 0.020) was observed that could be attributed to fallout from the "Ivy Mike" thermonuclear detonation in 1952. The atom ratio decreased in the 1960s and 1970s due to increase in the global fallout with a low 240Pu/ 239Pu atom ratio (˜0.18). Recent coral bands (1981-1999) are dominated by the transport of remobilised Pu, with high 240Pu/ 239Pu atom ratios, from the Marshall Islands to Guam Island along the North Equatorial Current (NEC). This remobilised Pu was estimated to comprise 69% of the total Pu in the recent coral bands, although its contribution was variable over time.

  4. Plutonium and americium behavior in coral atoll environments

    SciTech Connect

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

    1984-02-01

    Inventories of /sup 239 +240/Pu and /sup 241/Am greatly in excess of global fallout levels persist in the benthic environments of Bikini and Enewetak Atolls. Quantities of /sup 239 +240/Pu and lesser amounts of /sup 241/Am are continuously mobilizing from these sedimentary reservoirs. The amount of /sup 239 +240/Pu mobilized to solution at any time represents 0.08 to 0.09% of the sediment inventories to a depth of 16 cm. The mobilized /sup 239 +240/Pu has solute-like characteristics and different valence states coexist in solution - the largest fraction of the soluble plutonium is in an oxidized form (+V,VI). The adsorption of plutonium to sediments is not completely reversible because of changes that occur in the relative amounts of the mixed oxidation states in solution with time. Further, any characteristics of /sup 239 +240/Pu described at one location may not necessarily be relevant in describing its behavior elsewhere following mobilization and migration. The relative amounts of /sup 241/Am to /sup 239 +240/Pu in the sedimentary deposits at Enewetak and Bikini may be altered in future years because of mobilization and radiological decay. Mobilization of /sup 239 +240/Pu is not a process unique to these atolls, and quantities in solution derived from sedimentary deposits can be found at other global sites. These studies in the equatorial Pacific have significance in assessing the long-term behavior of the transuranics in any marine environment. 22 references, 1 figure, 13 tables.

  5. Characterization of Pu concentration and its isotopic composition in soils of Gansu in northwestern China.

    PubMed

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

    2009-01-01

    The total 239+240Pu activities and 240Pu/239Pu atom ratios in surface soil samples (0-5cm) in the Kumtag Desert in western Gansu Province, and in a soil core sample in Lanzhou were investigated using a sector-field ICP-MS. In the surface soil samples, 239+240Pu activities in fine particles (<150microm) were 1.3-2.1 times of those in coarse particles (150microm-1mm) which ranged from 0.005 to 0.157mBq/g. Atom ratios of 240Pu/239Pu in the surface soils ranged from 0.168 to 0.192 with a mean of 0.182+/-0.008. The mean ratio was similar to the typical global fallout value although the Kumtag Desert was believed to have received close-in fallout derived from Chinese nuclear weapons tests mainly conducted in the 1970s. Furthermore, the mean 240Pu/239Pu atom ratio observed in the soil core sample in Lanzhou was similar to the typical global fallout value. In the soil core sample, 239+240Pu activities in the various layers ranged from 0.012 to 0.23mBq/g, and the inventory of 239+240Pu (32.4Bq/m2, 0-23cm) was slightly lower than that expected from global fallout (42Bq/m2) at the same latitude. Rapid downward migration of Pu isotopes was observed in Lanzhou soil core sample layers. The contribution of the 10-cm deep top layers of surface soils to total inventory was only 17%, while the contribution of deeper layers (10-23cm) was as high as 83%. The 239+240Pu activity levels and 240Pu/239Pu atom ratios in soils in Gansu Province, China are similar to those in atmospheric deposition samples collected in the spring in recent years in Japan. PMID:19058885

  6. A preliminary study for the development of reference material using oyster for determination of (137)Cs, (90)Sr and plutonium isotopes.

    PubMed

    Lee, Sang-Han; Oh, Jung-Suk; Lee, Jong-Man; Lee, Kyung-Bum; Park, Tae-Soon; Lee, Min-Kie; Kim, Seung-Hwan; Choi, Jong-Ki

    2016-03-01

    A new reference material for the determination of (137)Cs, (90)Sr and Pu isotopes ((238)Pu and (239,240)Pu) is being developed using dried oyster matrix by Korea Research Institute of Standards and Science (KRISS). The oyster was collected from Tongyoung harbour, southern part of Korea and the artificial radionuclides ((137)Cs, (90)Sr, (238)Pu and (239,240)Pu) were spiked into the material. After pretreatment and processing, the material was tested for homogeneity and massic activities were determined by measuring (137)Cs, (90)Sr, (238)Pu and (239,240)Pu. The reference value and extended uncertainty for those isotopes will be reported later. PMID:26688367

  7. Final Report on Utilization of TRU TRISO Fuel as Applied to HTR Systems Part I: Pebble Bed Reactors

    SciTech Connect

    Brian Boer; Abderrafi M. Ougouag

    2011-03-01

    The Deep-Burn (DB) concept [ ] focuses on the destruction of transuranic nuclides from used light water reactor (LWR) fuel. These transuranic nuclides are incorporated into tri-isotopic (TRISO) coated fuel particles and used in gas-cooled reactors with the aim of a fractional fuel burnup of 60 to 70% in fissions per initial metal atom (FIMA). This high performance is expected through the use of multiple recirculation passes of the fuel in pebble form without any physical or chemical changes between passes. In particular, the concept does not call for reprocessing of the fuel between passes. In principle, the DB pebble bed concept employs the same reactor designs as the presently envisioned low-enriched uranium core designs, such as the 400 MWth Pebble Bed Modular Reactor (PBMR-400) [ ]. Although it has been shown in the previous Fiscal Year (FY) (2009) that a PuO2 fueled pebble bed reactor concept is viable, achieving a high fuel burnup while remaining within safety-imposed prescribed operational limits for fuel temperature, power peaking, and temperature reactivity feedback coefficients for the entire temperature range, is challenging. The presence of the isotopes 239Pu, 240Pu, and 241Pu that have resonances in the thermal energy range significantly modifies the neutron thermal energy spectrum as compared to a standard, UO2-fueled core. Therefore, the DB pebble bed core exhibits a relatively hard neutron energy spectrum. However, regions within the pebble bed that are near the graphite reflectors experience a locally softer spectrum. This can lead to power and temperature peaking in these regions. Furthermore, a shift of the thermal energy spectrum with increasing temperature can lead to increased absorption in the resonances of the fissile Pu isotopes. This can lead to a positive temperature reactivity coefficient for the graphite moderator under certain operating conditions. Regarding the coated particle performance, the FY 2009 investigations showed that no

  8. SALTSTONE VAULT CLASSIFICATION SAMPLES MODULAR CAUSTIC SIDE SOLVENT EXTRACTION UNIT/ACTINIDE REMOVAL PROCESS WASTE STREAM APRIL 2011

    SciTech Connect

    Eibling, R.

    2011-09-28

    Savannah River National Laboratory (SRNL) was asked to prepare saltstone from samples of Tank 50H obtained by SRNL on April 5, 2011 (Tank 50H sampling occurred on April 4, 2011) during 2QCY11 to determine the non-hazardous nature of the grout and for additional vault classification analyses. The samples were cured and shipped to Babcock & Wilcox Technical Services Group-Radioisotope and Analytical Chemistry Laboratory (B&W TSG-RACL) to perform the Toxic Characteristic Leaching Procedure (TCLP) and subsequent extract analysis on saltstone samples for the analytes required for the quarterly analysis saltstone sample. In addition to the eight toxic metals - arsenic, barium, cadmium, chromium, mercury, lead, selenium and silver - analytes included the underlying hazardous constituents (UHC) antimony, beryllium, nickel, and thallium which could not be eliminated from analysis by process knowledge. Additional inorganic species determined by B&W TSG-RACL include aluminum, boron, chloride, cobalt, copper, fluoride, iron, lithium, manganese, molybdenum, nitrate/nitrite as Nitrogen, strontium, sulfate, uranium, and zinc and the following radionuclides: gross alpha, gross beta/gamma, 3H, 60Co, 90Sr, 99Tc, 106Ru, 106Rh, 125Sb, 137Cs, 137mBa, 154Eu, 238Pu, 239/240Pu, 241Pu, 241Am, 242Cm, and 243/244Cm. B&W TSG-RACL provided subsamples to GEL Laboratories, LLC for analysis for the VOCs benzene, toluene, and 1-butanol. GEL also determines phenol (total) and the following radionuclides: 147Pm, 226Ra and 228Ra. Preparation of the 2QCY11 saltstone samples for the quarterly analysis and for vault classification purposes and the subsequent TCLP analyses of these samples showed that: (1) The saltstone waste form disposed of in the Saltstone Disposal Facility in 2QCY11 was not characteristically hazardous for toxicity. (2) The concentrations of the eight RCRA metals and UHCs identified as possible in the saltstone waste form were present at levels below the UTS. (3) Most of the

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

    SciTech Connect

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

    2008-05-30

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

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

    SciTech Connect

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

    2010-02-04

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

  11. 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.

  12. A method to determine the time since last purification of weapons grade plutonium.

    PubMed

    Keegan, R P; Gehrke, R J

    2003-01-01

    A non-destructive technique to determine the time since last purification of weapons grade plutonium based on the 241Pu decay series has been developed and demonstrated to provide results that are consistent with our historical and process knowledge. This method is based on the use of the Bateman equations and the decay chain 241Pu-->237U & 241Am-->237Np-->233Pa. Secular equilibrium is assumed between the (2.1 x 10(6) year) 237Np and the (27 day) 233Pa. The proposed method is dependent upon the efficiency of the plutonium separation process but makes no assumption about the relative abundance of 241Pu in 239Pu. Even though the technique was developed for weapons grade plutonium, it is expected to apply to almost any material that contains plutonium. PMID:12941503

  13. 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. PMID:21911246

  14. 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. PMID:25659922

  15. Sediment core record of global fallout and Bikini close-in fallout Pu in Sagami Bay, Western Northwest Pacific margin.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2004-07-01

    The total 239-240Pu activity and 240Pu/239Pu atom ratio in the sediments in Sagami Bay of the western Northwest Pacific margin were investigated using ICP-MS with a shield torch system. 239+240Pu inventories in the examined sediment cores were found to be much higher than those predicted from atmospheric global fallout (42 MBq/km2) at the same latitude. In addition, elevated 240Pu/239Pu atom ratios ranging from 0.22 to 0.28 were observed in the sediment samples. On the basis of the vertical profiles of 239+240Pu and characterized 240Pu/239Pu atom ratios in a sediment core collected in the center of Sagami Bay, we identified two distinct sources of fallout Pu in the bay: the global stratospheric fallout with characteristic 240Pu/239Pu ratio of 0.18 and the transported close-in fallout derived from Bikini and Enewetak surface nuclear weapon test series in the 1950s. We propose that the Pu transportation was mainly due to oceanic processes (for example, through the North Equatorial Current and the Kuroshio Current). Using a two fallout end-member model, we find that the contribution of Bikini close-in fallout Pu ranged from 44 to 59% in Sagami Bay sediments. To the best of our knowledge, this is the first report that Pu contamination, which originated from Bikini and Enewetak nuclear weapon test series in the 1950s, has extended westwards as far as the Japanese coast. PMID:15296298

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

    PubMed

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

    2010-10-15

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

  17. I. Nuclear Production Reaction and Chemical Isolation Procedure for Americium-240 II. New Superheavy Element Isotopes: Plutonium-242(Calcium-48,5n)(285)114

    NASA Astrophysics Data System (ADS)

    Ellison, Paul Andrew

    2011-12-01

    Part I discusses the study of a new nuclear reaction and chemical separation procedure for the production of 240Am. Thin 242Pu, natTi, and natNi targets were coincidently activated with protons from the 88-Inch Cyclotron, producing 240Am, 48V, and 57Ni, respectively. The radioactive decay of these isotopes was monitored using high-purity Ge gamma ray detectors in the weeks following irradiation. The excitation function for the 242 Pu(p, 3n)240Am nuclear reaction was measured to be lower than theoretical predictions, but high enough to be the most viable nuclear reaction for the large-scale production of 240 Am. Details of the development of a chemical separation procedure for isolating 240Am from proton-irradiated 242Pu are discussed. The separation procedure, which includes two anion exchange columns and two extraction chromatography columns, was experimentally investi- gated using tracer-level 241Am, 239Pu, and model proton-induced fission products 95Zr, 95Nb, 125Sb, and 152Eu. The separation procedure was shown to have an Am/Pu separation factor of >2x10 7 and an Am yield of ˜70%. The separation procedure was found to purify the Am sample from >99.9% of Eu, Zr, Nb, and Sb. The procedure is well suited for the processing of ˜1 gram of proton-irradiated 242Pu to produce a neutron-induced fission target consisting of tens of nanograms of 240Am. Part II describes the use of the Berkeley Gas-filled Separator at the Lawrence Berkeley National Laboratory 88-Inch Cyclotron for the study of the 242Pu(48Ca,5n)285114 nuclear re- action. The new, neutron-deficient, superheavy element isotope 285114 was produced in 48Ca irradiations of 242Pu targets at a center-of-target beam energy of 256 MeV ( E* = 50 MeV). The alpha decay of 285114 was followed by the sequential alpha decay of four daughter nuclides, 281Cn, 277Ds, 273Hs, and 269 Sg. 265Rf was observed to decay by spontaneous fission. The measured alpha-decay Q-values were compared with those from a macroscopic

  18. Discovery of new superheavy element isotopes

    NASA Astrophysics Data System (ADS)

    Gates, Jacklyn

    2011-04-01

    The first confirmation of element 114 production and decay was performed in 2009 with the Berkeley Gas-filled Separator at the Lawrence Berkeley National Laboratory 88-Inch Cyclotron. The 48 Ca + 242Pu reaction was used. Compound nucleus evaporation residues were separated from beam and other reaction products with the Berkeley Gas-filled separator and implanted in the focal plane detector system. Production and decay of one atom each of 287 114 (via the 242Pu(48 Ca, 3n)287 114 reaction) and 286 114(via the 242Pu(48 Ca,4n)286 114 reaction) were observed. Production cross sections, decay modes, decay energies, and half-lives and for these element 114 isotopes and their daughters were consistent with those reported by the Dubna Gas Filled Recoil Separator Group (Yuri Oganessian , J. Phys. G: Nucl. Part. Phys. 34 (2007) R165--R242). In 2010, the 48 Ca + 242Pu reaction was used again, at an increased beam energy to optimize the production of new isotope, 285 114, by the 242Pu(48 Ca,5n)285 114 reaction. The production and decay of one atom of 286 114 (via the 242Pu(48 Ca,4n)286 114 reaction) was observed, re-confirming the properties of this isotope. In addition, a single event corresponding to the production and decay of 285 114 (via the 242Pu(48 Ca,5n)285 114 reaction) was observed. The implantation of 285 114 in the detector was followed by five α-decays and a spontaneous fission event, indicating the α-decays of new isotopes, 285 114, 281Cp, 277Ds, 273Hs, 269Sg, and the spontaneous fission of new isotope, 265Rf. The decay properties of all these new isotopes match expectations based on microscopic-macroscopic mass models supplemented with extrapolations of previously reported superheavy element isotope decay properties. However, some systematic differences between observed and predicted α-decay Q-values may be used to refine models of nuclear shell effects in heavy element isotopes. Financial support was provided by the Office of High Energy and Nuclear Physics

  19. 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.

  20. 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. PMID:24144889

  1. Comparative behavior of plutonium and americium in the equatorial Pacific

    SciTech Connect

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

    1983-01-01

    Inventories of /sup 239 +240/Pu and /sup 241/Am greatly in excess of global fallout levels persist in the benthic environments of Bikini and Enewetak Atolls. The amount of /sup 239 +240/Pu mobilized to solution at the atolls can be predicted from a distribution coefficient K/sub d/ of 2.3 x 10/sup 5/ and the mean sediment concentrations. The mobilized /sup 239 +240/Pu has solute-like characteristics and different valence states coexist in solution - the largest fraction of the soluble plutonium is in an oxidized form (+V,VI). The adsorption of plutonium to sediments is not completely reversible because of changes that occur in the relative amounts of the mixed oxidation states in solution with time. Characteristics of /sup 239 +240/Pu described at one location may not necessarily describe its behavior elsewhere. The relative amounts of /sup 241/Am to /sup 239 +240/Pu may be altered in future years because of mobilization and radiological decay.

  2. Artificial radionuclides in the atmosphere over Lithuania.

    PubMed

    Lujaniene, G; Aninkevicius, V; Lujanas, V

    2009-02-01

    Measurements of airborne radioactive aerosol concentration were carried out on the basis of 1-3 days samples after the Chernobyl disaster and during the period of 1992-2003. Transport of "hot" particles of different composition resulted in the high activity concentrations of (137)Cs, (238)Pu, (239,240)Pu and (241)Am in the atmosphere in Vilnius at the end of April 1986. The (240)Pu/(239)Pu atom ratio showed clear evidence of non-global plutonium originating from the Chernobyl accident in the atmosphere over Lithuania. The (240)Pu/(239)Pu atom ratio ranged from 0.14 to 0.40 in monthly samples in Vilnius in 1995-2003. An increase in activity concentration of (137)Cs by a factor of 100 (up to 300 microBq/m(3)) was found following forest fires in the Ukraine and Belarus. However, no transport of the Chernobyl plutonium was observed and the (240)Pu/(239)Pu atom ratio in samples collected during the forest fires was found to be 0.229 and 0.185, respectively. The exponential decrease in the (240)Pu/(239)Pu atom ratio from 0.30 to 0.19 (mean values) was observed in 1995-2003. PMID:17884261

  3. Characterisation of the plutonium isotopic composition of a sediment core from Palomares, Spain, by low-energy AMS and alpha-spectrometry

    NASA Astrophysics Data System (ADS)

    Chamizo, E.; Jiménez-Ramos, M. C.; Enamorado, S. M.; García-León, M.; García-Tenorio, R.; Mas, J. L.; Masqué, P.; Merino, J.; Sanchez-Cabeza, J. A.

    2010-04-01

    The measurement of plutonium isotopes, 239Pu and 240Pu, at 670 kV on the compact accelerator mass spectrometry (AMS) system at the Centro Nacional de Aceleradores (CNA) in Seville, Spain, is now a reality. In this work, we present first Pu AMS results for environmental samples: a sediment core collected in a submarine canyon in the Mediterranean coast of the Spanish region of Palomares, affected by a nuclear accident in 1966. From the study of the 240Pu/ 239Pu atomic ratio profile, showing on average levels lower than 11%, we confirm that the weapon-grade plutonium released on land during the accident, with a characteristic 240Pu/ 239Pu atomic ratio of 5.8%, has found its way into the marine environment. A two-plutonium sources mixture model (Palomares and fallout) is used to elucidate the percentage of the plutonium coming from the accident. As a validation exercise of the Pu AMS measuring technique and in order to obtain the 238Pu/ (239+240)Pu activity ratios, samples were also studied by alpha-spectrometry (AS). The obtained AS 239+240Pu activity concentration results fit in with the AMS ones in a wide dynamic range, thus validating the AMS technique.

  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. PMID:26631455

  5. Plutonium, cesium and uranium series radionuclides in the Hudson River estuary and other environments. Annual technical progress report, 1 December 1980-30 November 1981

    SciTech Connect

    Simpson, H.J.; Trier, R.M.

    1981-01-01

    Radionuclide activities were measured in sediment cores and suspended particle samples throughout the salinity range of the Hudson River estuary. Activities of /sup 137/Cs, /sup 134/Cs, /sup 60/Co, /sup 239/ /sup 240/Pu, and /sup 238/Pu indicate reasonably rapid accumulation rates in the sediments of marginal cove areas, and very rapid deposition in the harbor region adjacent to New York City, resulting in /sup 239/ /sup 240/Pu accumulations there more than an order of magnitude greater than the fallout delivery rate. Fallout /sup 239/ /sup 240/Pu reaching the Hudson is almost completely retained within the systems by particle deposition, while 80 to 90% of the /sup 137/Cs derived from both reactor releases and fallout is exported to the coastal waters in solution. Depth profiles of radionuclides in Hudson sediments are not significantly altered by physical mixing processes in the sediments in areas accumulating particles at greater than 1 cm/yr.

  6. Modelling the distribution of plutonium in the Pacific Ocean.

    PubMed

    Nakano, Masanao; Povinec, Pavel P

    2003-01-01

    An Oceanic General Circulation Model (OGCM) including a plutonium scavenging model as well as an advection-diffusion model has been developed for modelling the distribution of plutonium in the Pacific Ocean. Calculated 239, 240Pu water profile concentrations and 239, 240Pu inventories in water and sediment of the Pacific Ocean have showed a reasonable agreement with the experimental results. The presence of local fallout plutonium in central North Pacific waters has been confirmed. The observed 240Pu/239Pu mass ratios confirm that plutonium originating from local fallout from nuclear weapons tests carried out at Bikini and Enewetak Atolls is more rapidly removed from surface waters to deeper waters than plutonium originating from global fallout. The developed OGCM can be used for modelling the dispersion of other non-conservative tracers in the ocean as well. PMID:12860091

  7. Plutonium, cesium and uranium series radionuclides in the Hudson River estuary and other environments. Annual technical progress report, December 1, 1979-November 30, 1980

    SciTech Connect

    Simpson, H. J.; Trier, R. M.; Olsen, C. R.

    1980-01-01

    Radionuclide activities were measured in a large number of sediment cores and suspended particle samples throughout the salinity range of the Hudson River estuary. Activities of /sup 137/Cs, /sup 134/Cs and /sup 60/Co determined by gamma spectrometry and /sup 239/ /sup 240/Pu and /sup 238/Pu determined by alpha spectrometry indicate reasonably rapid accumulation rates in the sediments of marginal cove areas, and very rapid deposition in the harbor region adjacent to New York City, resulting in /sup 239/ /sup 240/Pu accumulations there more than an order of magnitude greater than the fallout delivery rate. Measurable amounts of reactor-derived /sup 134/Cs and /sup 60/Co are found in nearly al sediment samples containing appreciable /sup 137/Cs between 15 km upstream of Indian Point and the downstream extent of our sampling about 70 km south of the reactor. Fallout /sup 239/ /sup 240/Pu reaching the Hudson appears to be almost completely retained within the systems by particle deposition, while 70 to 90% of the /sup 137/Cs derived from both reactor releases and fallout has been exported to the coastal waters in solution. Activity levels of /sup 239/ /sup 240/Pu in New York harbor sediments indicate a significant source in addition to suspended particles carried down the Hudson. The most likely cause appears to be transport into the estuary of particles from offshore waters having higher specific activities of /sup 239/ /sup 240/Pu. Measurements of fallout /sup 239/ /sup 240/Pu in a saline lake with a high carbonate ion concentration yielded water column activities about two orders of magnitude greater than has been found for fallout plutonium in other continental waters, indicating extensive mobility in some natural water environments. Experiments using lake water suggest that carbonate ion may indeed be a critical factor in regulating plutonium solubility and that low molecular weight complexes are primarily responsible for enhanced plutonium solubility.

  8. 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. PMID:24636561

  9. 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. PMID:22549140

  10. Plutonium and radiocesium in the water column of the Hudson River estuary

    NASA Astrophysics Data System (ADS)

    Linsalata, P.; Simpson, H. J.; Olsen, C. R.; Cohen, N.; Trier, R. M.

    1985-12-01

    Isotopes of plutonium (Pu), cesium (Cs), and cobalt (Co) introduced into the Hudson River Estuary from fallout deposition, the erosion of fallout-contaminated surface soils, and nuclear reactor effluent (isotopes of Cs and Co only) have been measured in water column samples collected from 1975 to 1980 Isotopic measurements conducted independently by two research groups utilizing different sampling and analytical techniques have been summarized. The major conclusions drawn from the work are that for water samples collected by the two laboratories over similar time periods, the mean concentrations of nonfilterable239,240Pu (<0.45 μm) were identical at 0.13 fCi/l, mean concentrations of both137Cs and239,240Pu in suspended particulates were more divergent at 2,270±920 pCi/kg (±1 SD) and 1,430±430 pCi/kg for137Cs, and 19±8 pCi/kg and 12±4 pCi/kg for239,240Pu The behavior of239,240Pu and137Cs within the water column is shown to diverge within brackish waters Specifically, the magnitude of the137Cs distribution coefficient ( K d ) can be expressed as an inverse power function of the chloride ion concentrations for chlorinities between 0.1 and 4 g Cl-/l No difference in the239,240Pu K d has been observed between fresh and brackish waters Based on the expected inventories of239,240Pu and137Cs within watershed soils, the current downstream transport of these radionuclides represents fractional mobilization rates on the order of 1 4 (×10-4) per year

  11. Multipurpose Radiation Resistant Semiconductor Detectors for Alpha, Neutron & Low Energy Gamma Ray Measurements at High Temperatures in High-Intensity Gamma Ray

    SciTech Connect

    Ruddy, Frank H.

    2005-06-01

    Work scheduled under year two of DOE Grant DE-FG02-04ER63734 is on schedule and all year-two milestones have or will be met. Results to date demonstrate that unprecedented silicon carbide (SiC) energy resolution has been obtained, and that SiC detectors may achieve energy resolution that exceeds that obtainable with the best silicon alpha spectrometers. Fast-neutron energy spectrometry measurements indicate that recoil-ion energy spectrometry should be possible with SiC detectors. Furthermore, SiC detectors have been demonstrated to perform well even after gamma-ray exposures of 1.E09 Rad. This result and the previously demonstrated capability of SiC detectors to operate in elevated-temperature environments are very promising for potential DOE EMSP applications. A new class of multipurpose, radiation-resistant semiconductor detectors that can be used in elevated-temperature and high-radiation environments is being developed under this grant. These detectors, based on silicon carbide (SiC) semiconductor are designed to have larger active volumes than previously available SiC detectors, and are being tested for their response to alpha particles, X-rays and low energy gamma rays, and fast neutrons. Specifically, SiC radiation detectors with larger areas and 100-micrometer thick active regions have been designed and manufactured according to detector-design specifications. Detectors based on a Schottky diode design were specified in order to minimize the effects of the detector entrance window on alpha particle measurements. During manufacture of the Schottky diodes, the manufacturer also provided a set of large-volume SiC p-i-n diodes for testing Extensive alpha particle measurements have been carried out to test and quantify the response of the SiC Schottky diodes. Exposures to 148-Gd, 213-Po, 217-At, 221-Fr, 225-Ac, 237-Np, 238-Pu, 240-Pu, and 242-Pu sources were used to obtain detailed alpha response data in the alpha energy range from 3182.787 keV to 8375.9 ke

  12. 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.

  13. Distribution of neptunium and plutonium in New Mexico lichen samples (Usnea arizonica) contaminated by atmospheric fallout

    DOE PAGESBeta

    Oldham, Jr., Warren J.; Hanson, Susan K.; Lavelle, Kevin B.; Miller, Jeffrey L.

    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.

  14. Plutonium isotopes in settling particles: transport and scavenging of Pu in the western Northwest Pacific.

    PubMed

    Zheng, Jian; Yamada, Masatoshi

    2006-07-01

    We examined the vertical distributions of 239+240Pu activity and 240Pu/239Pu atom ratio in settling particles and quantified the particulate 239+240Pu fluxes in the water column in the western Northwest Pacific. Settling particle samples were collected using sediment traps. Plutonium isotopes were analyzed using a sector field high-resolution ICP-MS. To the best of our knowledge, this is the first time that both Pu activity and Pu isotope ratio data have been obtained for settling particles in the Pacific Ocean. The high (>0.18) 240Pu/239Pu atom ratios in settling particles indicate that plutonium from the Pacific Proving Grounds (PPG) source in the central Pacific is transported toward the western Northwest Pacific. Evidence indicates that Pu scavenging onto the settling particles is strongly dependent upon the bulk mass flux. The results suggest that advective lateral transport of dissolved Pu from the open ocean to the ocean margin and removal of Pu into the margin sediments by particle scavenging is a common phenomenon in the Pacific Ocean. Plutonium can be considered as a useful tracer to study the transport and fate of other contaminants that readily adsorb to particles in marine environments. PMID:16856723

  15. Plutonium, cesium, uranium, and thorium series radionuclides in the Hudson River estuary and other environments. Annual technical progress report, December 1, 1982-November 30, 1983

    SciTech Connect

    Simpson, H.J.; Trier, R.M.; Anderson, R.F.

    1983-01-01

    We have measured radionuclide activities in a large number of sediment cores and suspended particle samples throughout the salinity range of the Hudson River estuary. Activities of /sup 137/Cs, /sup 134/Cs and /sup 60/Co determined by gamma spectrometry and /sup 239/ /sup 240/Pu and /sup 238/Pu determined by alpha spectrometry indicate reasonably rapid accumulation rates in the sediments of marginal cove areas, and very rapid deposition in the harbor region adjacent to New York City, resulting in /sup 239/ /sup 240/Pu accumulations there more than an order of magnitude greater than the fallout delivery rate. Fallout /sup 239/ /sup 240/Pu moving downstream in the Hudson appears to be almost completely retained within the system by particle deposition, while more than 50% of the /sup 137/Cs derived from both reactor releases and fallout has been exported from the tidal Hudson to coastal waters. Measurements of fallout /sup 239/ /sup 240/ Pu in a saline lake with a high carbonate ion concentration yielded water column activities about two orders of magnitude greater than has been found for fallout plutonium in other continental waters, indicating extensive mobility in some natural water environments. Experiments using lake water suggest that carbonate ion is likely to be a critical factor in regulating plutonium solubility in some environments and that low molecular weight complexes are primarily responsible for enhanced plutonium solubility. 5 references.

  16. US Mussel Watch 1976-1978: an overview of the trace-metal, DDE, PCB, hydrocarbon, and artificial radionuclide data. [Mytilus edulis, M. californianus, Crassostrea sp

    SciTech Connect

    Farrington, J.W.; Goldberg, E.D.; Risebrough, R.W.; Martin, J.H.; Bowen, V.T.

    1983-08-01

    Data are presented for trace metals, polychlorinated biphenyls (PCBs), aromatic hydrocarbons and /sup 239/ /sup 240/Pu in Mytilus edulis, M. californianus, and Crassostrea sp. collected in the US Mussel Watch program in 1976-1978 from 62 locations on the US east and west coasts. General similarities in geographical distributions of concentrations were present in all 3 years with at least an order of magnitude elevation of concentrations of Pb, PCBs, and fossil fuel hydrocarbons in bivalves sampled near the larger urban areas. Elevated Cd and /sup 239/ /sup 240/Pu concentrations in bivalves from the central California coast are apparently related to enrichments of Cd and nuclear weapons testing fallout /sup 239/ /sup 240/Pu in intermediate depth water of the North Pacific and upwelling of this water associated with the California Current system. Data have revealed no evidence of local or regional systematic elevations of environmental concentrations of /sup 239/ /sup 240/Pu as a result of effluent releases from nuclear power reactors.

  17. Plutonium in Soils from Northeast China and Its Potential Application for Evaluation of Soil Erosion

    PubMed Central

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

    2013-01-01

    Surface and soil core samples from northeast China were analyzed for Pu isotopes. The measured 240Pu/239Pu atomic ratios and 239 + 240Pu/137Cs activity ratios revealed that the global fallout is the dominant source of Pu and 137Cs at these sites. Migration behavior of Pu varying with land type and human activities resulted in different distribution of Pu in surface soils. A sub-surface maximum followed by exponential decline of 239 + 240Pu concentrations was observed in an undisturbed soil core, with a total 239 + 240Pu inventory of 86.9 Bq/m2 and more than 85% accumulated in 0 ~ 20 cm layers. While only half inventory of Pu was obtained in another soil core and no sub-surface maximum value occurred. Erosion of topsoil in the site should be the most possible reason for the significantly lower Pu inventory, which is also supported by the reported 137Cs profiles. These results demonstrated that Pu could be applied as an ideal substitute of 137Cs for soil erosion study in the future. PMID:24336360

  18. Depositional behaviors of plutonium and thorium isotopes at Tsukuba and Mt. Haruna in Japan indicate the sources of atmospheric dust.

    PubMed

    Hirose, K; Igarashi, Y; Aoyama, M; Inomata, Y

    2010-02-01

    Monthly plutonium and thorium depositions at Tsukuba (28m asl) and Mt. Haruna (1370m asl) were measured during 2006 and 2007 (Jan 2006-Dec 2007 at Tsukuba, Nov 2006-Dec 2007 at Mt. Haruna). The monthly (239,240)Pu depositions ranged from 0.044 to 2.67mBq m(-2) at Tsukuba and from 0.05 to 0.9mBq m(-2) at Mt. Haruna during the measurement periods. Monthly (239,240)Pu deposition did not differ markedly between the two sites except in April 2007. Seasonal pattern of monthly (239,240)Pu depositions at both sites showed high in spring and low in summer, and typical of seasonal variations in northeastern Asia. Thorium deposition at Tsukuba was higher than that at Mt. Haruna except in May and June 2007. (230)Th/(232)Th activity ratios were used to partition deposition samples into locally and remotely derived fractions. The results revealed that a major proportion of total (239,240)Pu and Th deposits are derived from remote sources, especially in spring. PMID:19804923

  19. Cesium, americium and plutonium isotopes in ground level air of vilnius

    NASA Astrophysics Data System (ADS)

    Lujaniene, G.; Šapolaite, J.; Remeikis, V.; Lujanas, V.; Jermolajev, A.; Aninkevičius, V.

    2006-01-01

    Systematic observations of radionuclide composition and concentration in the atmosphere have been carried out at the Institute of Physics in Vilnius since 1963. Increases in activity concentration of radionuclides in the atmosphere were observed after nuclear weapon tests and the Chernobyl NPP accident. At present the radiation situation in Lithuania is determined by two main sources of radionuclides, forest fire and resuspension products transferred from highly polluted region of the Ukraine and Belarus. The activity concentrations of 137Cs were measured in two to three days samples while plutonium and americium in monthly samples. The extremely high activity concentrations of 238Pu, 239,240Pu, 241Am determined in the atmosphere during the Chernobyl accident can be explained by transport of “hot particles” of different composition. Activity concentration in 1995 2003 of 241Am and 239,240Pu isotopes ranged from 0.3 to 500 and from 1 to 500 nBq/m3, respectively. 238Pu/239,240Pu activity ratio in measured samples differs from 0.03 to 0.45. A decrease in 240Pu/239Pu atomic ratio from 0.30 to 0.19 was observed in 1995 2003.

  20. Radionuclide transport from soil to air, native vegetation, kangaroo rats and grazing cattle on the Nevada test site.

    PubMed

    Gilbert, R O; Shinn, J H; Essington, E H; Tamura, T; Romney, E M; Moor, K S; O'Farrell, T P

    1988-12-01

    Between 1970 and 1986 the Nevada Applied Ecology Group (NAEG), U.S. Department of Energy, conducted environmental radionuclide studies at weapons-testing sites on or adjacent to the Nevada Test Site. In this paper, NAEG studies conducted at two nuclear (fission) sites (NS201, NS219) and two nonnuclear (nonfission) sites (Area 13 [Project 57] and Clean Slate 2) are reviewed, synthesized and compared regarding (1) soil particle-size distribution and physical-chemical characteristics of 239 + 240Pu-bearing radioactive particles, (2) 239 + 240Pu resuspension rates and (3) transuranic and fission-product radionuclide transfers from soil to native vegetation, kangaroo rats and grazing cattle. The data indicate that transuranic radionuclides were transferred more readily on the average from soil to air, the external surfaces of native vegetation and to tissues of kangaroo rats at Area 13 than at NS201 or NS219. The 239 + 240Pu resuspension factor for undisturbed soil at Area 13 was three to four orders-of-magnitude larger than at NS201 and NS219, the geometric mean (GM) vegetation-over-soil 239 + 240Pu concentration ratio was from ten to 100 times larger than at NS201, and the GM GI-over-soil, carcass-over-soil and pelt-over-soil 239 + 240Pu ratios for kangaroo rats were about ten times larger than at NS201. These results are consistent with the finding that Area 13, compared with NS201 or NS219, has a higher percentage of radioactivity associated with smaller soil particles and a larger percentage of resuspendable and respirable soil. However, the resuspension factor increased by a factor of 27 at NS201 when the surface soil was disturbed, and by a factor of 12 at NS219 following a wildfire. The average (GM) concentration of 239 + 240Pu for the GI (and contents) of Area 13 kangaroo rats and for the rumen contents of beef cattle that grazed Area 13 were very similar (400 vs. 440 Bq kg-1 dry wt, respectively) although the variability between individuals was very large. The

  1. Sequential injection approach for simultaneous determination of ultratrace plutonium and neptunium in urine with accelerator mass spectrometry.

    PubMed

    Qiao, Jixin; Hou, Xiaolin; Roos, Per; Lachner, Johannes; Christl, Marcus; Xu, Yihong

    2013-09-17

    An analytical method was developed for simultaneous determination of ultratrace level plutonium (Pu) and neptunium (Np) using iron hydroxide coprecipitation in combination with automated sequential injection extraction chromatography separation and accelerator mass spectrometry (AMS) measurement. Several experimental parameters affecting the analytical performance were investigated and compared including sample preboiling operation, aging time, amount of coprecipitating reagent, reagent for pH adjustment, sedimentation time, and organic matter decomposition approach. The overall analytical results show that preboiling and aging are important for obtaining high chemical yields for both Pu and Np, which is possibly related to the aggregation and adsorption behavior of organic substances contained in urine. Although the optimal condition for Np and Pu simultaneous determination requires 5-day aging time, an immediate coprecipitation without preboiling and aging could also provide fairly satisfactory chemical yields for both Np and Pu (50-60%) with high sample throughput (4 h/sample). Within the developed method, (242)Pu was exploited as chemical yield tracer for both Pu and Np isotopes. (242)Pu was also used as a spike in the AMS measurement for quantification of (239)Pu and (237)Np concentrations. The results show that, under the optimal experimental condition, the chemical yields of (237)Np and (242)Pu are nearly identical, indicating the high feasibility of (242)Pu as a nonisotopic tracer for (237)Np determination in real urine samples. The analytical method was validated by analysis of a number of urine samples spiked with different levels of (237)Np and (239)Pu. The measured values of (237)Np and (239)Pu by AMS exhibit good agreement (R(2) ≥ 0.955) with the spiked ones confirming the reliability of the proposed method. PMID:23952680

  2. Radionuclide uptake by trees at a radwaste pond in Washington State.

    PubMed

    Landeen, D S; Mitchell, R M

    1986-06-01

    This paper presents work conducted in the summer of 1980 by Rockwell Hanford Operations, Hanford, WA, in support of a proposed effort to decommission and decontaminate a Hanford radwaste pond (216-U-10 Pond). The radionuclide values presented here are in addition to the U-Pond work that was recently published (La83) and are below any levels of environmental concern and within state and federal guidelines. U-Pond was constructed in 1944 for the surface disposal of industrial waste waters from nuclear separation processes and is one of the longest used aquatic, low-level, radioactive waste-disposal sites in the world. Tree leaf/twig, root, core and soil samples were collected and analyzed for 137Cs, 90Sr and 239Pu/240Pu. Strontium-90 was more readily taken up by trees than 137Cs or 239Pu/240Pu. Soil concentration values for 137Cs and 239Pu/240Pu were significantly greater (p less than or equal to 0.05) than all tree component parts. Radionuclide concentration ratios were higher for 90Sr (0.01-1355.0) than for 137Cs and 239Pu/240Pu for all tree components examined. Concentration ratios for 239Pu/240Pu ranged from 10(-6) to 10(-2) and are comparable to other studies conducted at the U.S. Department of Energy's Oak Ridge and Savannah River laboratories. These data represent the first quantitative information with respect to radionuclide uptake by trees on the Hanford Site. PMID:3710785

  3. Anomalous plutonium isotopic ratios in sediments of Lake Qinghai from the Qinghai-Tibetan Plateau, China.

    PubMed

    Wu, Fengchang; Zheng, Jian; Liao, Haiqing; Yamada, Masatoshi; Wan, Guojiang

    2011-11-01

    The vertical profiles of (239+240)Pu and (137)Cs activities and (240)Pu/(239)Pu isotopic ratios are determined for three sediment cores of Lake Qinghai from the Qinghai-Tibetan Plateau, China, and compared with those in sediments of another three lakes (Lakes Bosten, Sugan, and Shuangta), the only existing ones closest to Lop Nor area, China's nuclear weapons test site in the northwestern part of the country. The mean inventory of 47.7 ± 18.7 MBq km(-2) for (239+240)Pu activity in Lake Qinghai is comparable to the average value of global fallout expected at the same latitude, yet the mean inventory of 1112.0 ± 78.0 MBq km(-2) for (137)Cs is slightly lower than that of global fallout. Anomalously low (240)Pu/(239)Pu isotopic ratios (0.038-0.125) were found in the 3-6.5 cm deep sediment layers, indicating the trace Pu input from early nuclear weapons research activities at Atomic City in the lake's watershed during the 1950-60s. Model calculation indicated that the Pu input accounted for approximately 5-16% of the total Pu inventory. The observation of low (240)Pu/(239)Pu ratio in the deep sediment layer provided a new time marker for recent sediment dating in the lake and around the area. The results are of great significance to the further understanding of sources, records, and environmental impacts of global and regional nuclear activities in the environment and provide important chronological information for further studies on the water eutrophication process and climatic change, and reconstruction of pollution history of organic contaminants and heavy metals in the watershed of Lake Qinghai. PMID:21950768

  4. Plutonium and 137Cs in surface water of the South Pacific Ocean.

    PubMed

    Hirose, K; Aoyama, M; Fukasawa, M; Kim, C S; Komura, K; Povinec, P P; Sanchez-Cabeza, J A

    2007-08-01

    The present plutonium and 137Cs concentrations in South Pacific Ocean surface waters were determined. The water samples were collected in the South Pacific mid-latitude region (32.5 degrees S) during the BEAGLE expedition conducted in 2003-04 by JAMSTEC. 239,240Pu concentrations in surface seawater of the South Pacific were in the range of 0.5 to 4.1 mBq m(-3), whereas 137Cs concentrations ranged from 0.07 to 1.7 Bq m(-3). The observed 239,240Pu and 137Cs concentrations in the South Pacific were almost of the same level as those in the North Pacific subtropical gyre. The surface 239,240Pu in the South Pacific subtropical gyre showed larger spatial variations than 137Cs, as it may be affected by physical and biogeochemical processes. The 239,240Pu/137Cs activity ratios, which reflect biogeochemical processes in seawater, were generally smaller than that observed in global fallout, except for the most eastern station. The 239,240Pu/137Cs ratios in the South Pacific tend to be higher than that in the North Pacific. The relationships between anthropogenic radionuclides and oceanographic parameters such as salinity and nutrients were examined. The 137Cs concentrations in the western South Pacific (the Tasman Sea) and the eastern South Pacific were negatively correlated with the phosphate concentration, whereas there is no correlation between the 137Cs and nutrients concentrations in the South Pacific subtropical gyre. The mutual relationships between anthropogenic radionuclides and oceanographic parameters are important for better understanding of transport processes of anthropogenic radionuclides and their fate in the South Pacific. PMID:17459459

  5. Fallout of uranium and plutonium from recent volcanic eruptions

    SciTech Connect

    Sandoval, D.N.

    1984-01-01

    The concentrations of /sup 234/U, /sup 235/U, /sup 238/U in rain water were measured in a total of 102 individual samples which were collected at Fayetteville, Arkansas, from July 1980 through April 1983. A spectacular increase in the heavy isotope of uranium (/sup 238/U) was observed in the months of July, August (1980); January through April, November and December 1981. This large increase in /sup 238/U in rain appeared to have had its origin in the May 1980 eruption of Mount St. Helens. An increase in the concentration of /sup 238/U in rain, smaller than 1981, was observed, which seems to have originated from the El Chichon volcano eruption in March 1982, and the spring peak or so-called cycling effect. A striking increase in the average bimonthly concentration of /sup 239,240/Pu occurred during the months of September-October 1980 (15.6 fCi/l) and March-April 1981 (29.4 fCi/l). The excess deposition of /sup 239,240/Pu brought down by the rain at Fayetteville, Arkansas, from March 1980 through December 1982 was found to be 1.01 fCi/cm/sup 2/. The total amount of /sub 239,240/Pu deposited at Fayetteville, Arkansas, from March through December 1982, was found to be about 30 times higher than the total amount calculated from reported literature values. The excess /sup 239,240/Pu has been attributed to stratospheric /sub 239,240/Pu from nuclear weapons testing prior to the 25th Chinese nuclear test.

  6. Sources and pathways of artificial radionuclides to soils at a High Arctic site.

    PubMed

    Lokas, E; Bartmiński, P; Wachniew, P; Mietelski, J W; Kawiak, T; Srodoń, J

    2014-11-01

    Activity concentrations, inventories and activity ratios of (137)Cs, (238)Pu, (239 + 240)Pu and (241)Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900 ± 940, 47 ± 6, 886 ± 80 and 296 ± 19 Bq/m(2) for (137)Cs, (238)Pu, (239 + 240)Pu and (241)Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The (238)Pu/(239 + 240)Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The (238)Pu/(239 + 240)Pu and (239 + 240)Pu/(137)Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources. PMID:24946703

  7. Radionuclide transport from soil to air, native vegetation, kangaroo rats and grazing cattle on the Nevada test site

    SciTech Connect

    Gilbert, R.O.; Shinn, J.H.; Essington, E.H.; Tamura, T.; Romney, E.M.; Moor, K.S.; O'Farrell, T.P.

    1988-12-01

    Between 1970 and 1986 the Nevada Applied Ecology Group (NAEG), U.S. Department of Energy, conducted environmental radionuclide studies at weapons-testing sites on or adjacent to the Nevada Test Site. In this paper, NAEG studies conducted at two nuclear (fission) sites (NS201, NS219) and two nonnuclear (nonfission) sites (Area 13 (Project 57) and Clean Slate 2) are reviewed, synthesized and compared regarding (1) soil particle-size distribution and physical-chemical characteristics of 239 + 240Pu-bearing radioactive particles, (2) 239 + 240Pu resuspension rates and (3) transuranic and fission-product radionuclide transfers from soil to native vegetation, kangaroo rats and grazing cattle. The data indicate that transuranic radionuclides were transferred more readily on the average from soil to air, the external surfaces of native vegetation and to tissues of kangaroo rats at Area 13 than at NS201 or NS219. The 239 + 240Pu resuspension factor for undisturbed soil at Area 13 was three to four orders-of-magnitude larger than at NS201 and NS219, the geometric mean (GM) vegetation-over-soil 239 + 240Pu concentration ratio was from ten to 100 times larger than at NS201, and the GM GI-over-soil, carcass-over-soil and pelt-over-soil 239 + 240Pu ratios for kangaroo rats were about ten times larger than at NS201. These results are consistent with the finding that Area 13, compared with NS201 or NS219, has a higher percentage of radioactivity associated with smaller soil particles and a larger percentage of resuspendable and respirable soil. However, the resuspension factor increased by a factor of 27 at NS201 when the surface soil was disturbed, and by a factor of 12 at NS219 following a wildfire.

  8. Nuclear and dosimetric features of an isotopic neutron source

    NASA Astrophysics Data System (ADS)

    Vega-Carrillo, H. R.; Hernández-Dávila, V. M.; Rivera, T.; Sánchez, A.

    2014-02-01

    A multisphere neutron spectrometer was used to determine the features of a 239PuBe neutron source that is used to operate the ESFM-IPN Subcritical Reactor. To determine the source main features it was located a 100 cm from the spectrometer which was a 6LiI(Eu) scintillator and 2, 3, 5, 8, 10 and 12 in.-diameter polyethylene spheres. Count rates obtained with the spectrometer were unfolded using the NSDUAZ code and neutron spectrum, total fluence, and ambient dose equivalent were determined. A Monte Carlo calculation was carried out to estimate the spectrum and integral features being less than values obtained experimentally due to the presence of 241Pu in the Pu used to fabricate the source. Actual neutron yield and the mass fraction of 241Pu was estimated.

  9. Plutonium in Colorado residents: results of autopsy bone samples collected during 1975-1979.

    PubMed

    Ibrahim, S A; Warren, G M; Whicker, F W; Efurd, D W

    2002-08-01

    Concentrations of (239,240)Pu and the 240Pu/239Pu atom ratios were measured in rib samples from 55 non-occupationally exposed Colorado residents. Samples were collected at autopsy during 1975-1979 under an earlier study intended to compare plutonium levels in liver and lung of people who lived at various proximities to the Rocky Flats Environmental Technology Site (RFETS) near Denver. Overall, median (239,240)Pu concentrations from rib samples were 100, 80, and 57 microBq g(-1) ash weight for area locations A, B, and C, respectively. Area A encompassed subjects who lived within 25 km of RFETS, area B was between 25 and 50 km from RFETS, and area C included all of Colorado outside 50 km from the site and east of the continental divide. The corresponding median plutonium skeletal burdens estimated for these area locations were 146, 93, and 71 mBq, respectively. A statistically significant difference was noted only between plutonium concentrations in male rib samples and their skeletal burdens from area A compared to area C. However, based on a regression analysis of all study subjects, distance from RFETS was not statistically correlated to plutonium rib concentrations or skeletal burdens in this sample. Overall, median 240Pu/239Pu atom ratios were 0.20, 0.18, and 0.17 for areas A, B, and C, respectively. Although higher (239,240)Pu concentrations and skeletal burdens were indicated in area A males than area C males, we cannot conclude that RFETS releases may have caused this difference. The decreasing trends in the 240Pu/239Pu ratios with distance from RFETS are contrary with such a conclusion and strongly indicate that the material was primarily global fallout rather than weapons-grade plutonium that was processed at RFETS. Furthermore, there are other plausible explanations for the differences observed between area A and C residents. These include a decreasing trend in global fallout from the Rocky Mountain foothills eastward, smoking history differences, sample

  10. Interpretation of actinide-distribution data obtained from non-destructive and destructive post-test analyses of an intact-core column of Culebra dolomite.

    PubMed

    Perkins, W G; Lucero, D A

    2001-02-01

    The US Department of Energy (DOE), with technical assistance from Sandia National Laboratories, has successfully received EPA certification and opened the Waste Isolation Pilot Plant (WIPP), a nuclear waste disposal facility located approximately 42 km east of Carlsbad, NM. Performance assessment (PA) analyses indicate that human intrusions by inadvertent, intermittent drilling for resources provide the only credible mechanisms for significant releases of radionuclides from the disposal system. For long-term brine releases, migration pathways through the permeable layers of rock above the Salado formation are important. Major emphasis is placed on the Culebra Member of the Rustler Formation because this is the most transmissive geologic layer overlying the WIPP site. In order to help quantify parameters for the calculated releases, radionuclide transport experiments have been carried out using intact-core columns obtained from the Culebra dolomite member of the Rustler Formation within the WIPP site. This paper deals primarily with results of analyses for 241Pu and 241Am distributions developed during transport experiments in one of these cores. Transport experiments were done using a synthetic brine that simulates Culebra brine at the core recovery location (the WIPP air-intake shaft (AIS)). Hydraulic characteristics (i.e., apparent porosity and apparent dispersion coefficient) for intact-core columns were obtained via experiments using the conservative tracer 22Na. Elution experiments carried out over periods of a few days with tracers 232U and 239Np indicated that these tracers were weakly retarded as indicated by delayed elution of the species. Elution experiments with tracers 241Pu and 241Am were attempted but no elution of either species has been observed to date, including experiments of many months' duration. In order to quantify retardation of the non-eluted species 241Pu and 241Am after a period of brine flow, non-destructive and destructive analyses of

  11. Interpretation of Actinide-Distribution Data Obtained from Non-Destructive and Destructive Post-Test Analyses of an Intact-Core Column of Culebra Dolomite

    SciTech Connect

    LUCERO, DANIEL A; PERKINS, W GEORGE

    1999-08-26

    The US DOE, with technical assistance from Sandia National Laboratories, has successfully received EPA certification and opened the Waste Isolation Pilot Plant (WIPP), a nuclear waste disposal facility located approximately 42 km east of Carlsbad, New Mexico. Performance assessment analyses indicate that human intrusions by inadvertent, intermittent drilling for resources provide the only credible mechanisms for releases of radionuclides from the disposal system. In modeling long-term brine releases, subsequent to a drilling event, potential migration pathways through the permeable layers of rock above the Salado formation were analyzed. Major emphasis is placed on the Culebra Member of the Rustler Formation because this is the most transmissive geologic layer overlying the WIPP site. In order to help quantify parameters for the calculated releases, radionuclide transport experiments have been earned out using intact-core columns obtained from the Culebra dolomite member of the Rustler Formation within the WIPP site. This paper deals primarily with results of analyses for {sup 241}Pu and {sup 241}Am distributions developed during transport experiments in one of these cores. Transport experiments were done using a synthetic brine that simulates Culebra brine at the core recovery location (the WIPP air-intake shaft--AIS). Hydraulic characteristics (i.e., apparent porosity and apparent dispersion coefficient) for intact-core columns were obtained via experiments using the conservative tracer {sup 22}Na. Elution experiments carried out over periods of a few days with tracers {sup 232}U and {sup 239}Np indicated that these tracers were weakly retarded as indicated by delayed elution of the species. Elution experiments with tracers {sup 241}Pu and {sup 241}Am were attempted, but no elution of either species has been observed to date, including experiments of many months' duration. In order to quantify retardation of the non-eluted species {sup 241}Pu and {sup 241}Am

  12. 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.

  13. US Mussel Watch Program: Transuranic element data from Woods Hole Oceanographic Institution 1976-1983. Technical report

    SciTech Connect

    Palmieri, J.; Livingston, H.; Farrington, J.W.

    1984-05-01

    Bivalves (Mytilus edulis, Mytilus californianus, Crassostrea virginica and Ostrea equestris) were collected once per year during 1976, 1977, and 1978 along the United States coast and analyzed for (239,240)Pu, (241)Am and (137)Cs as part of the U.S. Mussel Watch program. Monthly samples were collected during 1976-1980 from Narragansett Bay, Rhode Island and Bodega Head, California and analyzed for (239,240)Pu, (241)Am, and (137)Cs. There is no evidence in the data for systematic regional or local elevated concentrations of radionuclides as a result of releases from the nuclear fuel cycle. Monthly fluctuations in radionuclide concentrations in the Narragansett Bay mussels appear to be primarily influenced by spawning.

  14. Sources and Spatial Distribution of Metal Pollutants in Soils near the El Paso Smelter: A Forensic Study with Pb and Pu Isotopes.

    NASA Astrophysics Data System (ADS)

    Ketterer, Michael; Moan, Matthew; Gremillion, Paul

    2010-05-01

    Lead and copper smelting has been conducted at El Paso since the late 1800's, and as a result, environmental media near the smelter have become contaminated. A study has been conducted to investigate the sources and spatial distribution of metal pollutants (Pb, Cd, Zn, Hg, As, Cu) and concomitant tracers (Ag, In, Sb, Bi) in soils from the smelter vicinity. Sampled locations were residential and non-residential locations in El Paso (Texas, USA), Anapra (New Mexico, USA) and Ciudad Juarez (Chihuahua, Mexico). Lead isotope studies indicate that the soil Pb is derived from smelting, and is consistent with two-component mixing between lead ores from Chihuahua (northern Mexico) having 206Pb/204Pb of 18.6 - 18.8 and ores from the Hanover, New Mexico (USA) mining district with 206Pb/204Pb of ~ 17.6. The Pb isotope results also exclude other common anthropogenic Pb sources such as paint and gasoline emissions as being major contributors. Concentrations of Hg and Pb of up to 10 and 11,000 ppm were found in surface soils within 1 km of the smelter. The metal concentration results clearly indicate that soils near the smelter (< 5 km) exhibit much higher concentrations of smelter-related elements than do soils from control locations (> 10 km distant). A general trend of decreasing concentrations vs. distance from the smelter was also observed. However, the results indicate that metal concentrations vary widely even at a fixed distance from the smelter point source. This phenomenon results from a combination of natural and anthropogenic processes that disturb and re-distribute soils in the surface environment. The site conditions consist of a very arid environment with little vegetation cover that is frequently disturbed by high winds and severe episodic rainfall. To study these effects, we have investigated stratospheric fallout plutonium (239+240Pu) as a proxy measure of disturbed vs. undisturbed soil conditions. The premise is that 'undisturbed' locations will have high 239+240

  15. Global fallout Pu recorded in lacustrine sediments in Lake Hongfeng, SW China.

    PubMed

    Zheng, Jian; Wu, Fengchang; Yamada, Masatoshi; Liao, Haiqing; Liu, Congqiang; Wan, Guojiang

    2008-03-01

    Studies on the distribution and isotope compositions of fallout Pu are important for source characterization of possible future non-fallout Pu contamination in aquatic environments, and useful for dating of recent sediments to understand the pollution history of environmental contaminants. We present the historical record of atmospheric Pu fallout reconstructed from a sediment core from Lake Hongfeng, China. The Pu activity profile was in agreement with the 137Cs profile. Inventories were 50.7 Bq m(-2) for 239+240Pu and 1586 Bq m(-2) for 137Cs. The average 240Pu/239Pu atom ratio was 0.185+/-0.009, indicating that Pu originated from global stratospheric fallout rather than from direct tropospheric or close-in fallout from the Chinese nuclear testing conducted in the 1970s. Our data suggested that Lake Hongfeng would be an ideal setting for monitoring atmospheric fallout and environmental changes in this region. PMID:17651874

  16. Determination of plutonium content in TRR spent fuel by nondestructive neutron counting

    NASA Astrophysics Data System (ADS)

    Chen, Yen-Fu; Sheu, Rong-Jiun; Chiao, Ling-Huan; Yuan, Ming-Chen; Jiang, Shiang-Huei

    2010-07-01

    For the nuclear safeguard purpose, this work aims to nondestructively determine the plutonium content in the Taiwan Research Reactor (TRR) spent fuel rods in the storage pool before the stabilization process, which transforms the metal spent fuel rods into oxide powder. A SPent-fuel-Neutron-Counter (SPNC) system was designed and constructed to carry out underwater scan measurements of neutrons emitting from the spent fuel rod, from which the 240Pu mass in the fuel rod will be determined. The SAS2 H control module of the SCALE 5.1 code package was applied to calculate the 240Pu-to-Pu mass ratio in the TRR spent fuel rod according to the given power history. This paper presents the methodology and design of our detector system as well as the measurements of four TRR spent fuel rods in the storage pool and the comparison of the measured results with the facility declared values.

  17. The High Altitude Sampling Program: Radioactivity in the stratosphere: Final report

    SciTech Connect

    Leifer, R; Juzdan, Z R

    1986-12-01

    Radioactivity data are presented from Project Airstream (aircraft) for the year 1983 and for Project Ashcan (balloon) for the years 1982 and 1984. Due to budgetary constraints both Projects Airstream and Ashcan have been terminated. This will be the final report containing radioactivity data collected during projects airstream and ashcan. Included are gross gamma, gamma spectral and radiochemical analyses of filter samples. Quality control samples submitted along with the air filter samples were analyzed and the results are presented. Low activity on many of the filters precludes the estimation of the stratospheric inventories of /sup 239,240/Pu and /sup 90/Sr. Based on data with count errors <20%, the mean Northern Hemisphere stratospheric /sup 90/Sr and /sup 239,240/Pu concentration for November 1983 was 0.2 +- 0.1 and 0.009 +- 0.006 Bq/1000 scm, respectively.

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

    PubMed

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

    2014-05-01

    A Certified Reference Material (CRM) for radionuclides in seaweed (Fucus vesiculosus) from the Baltic Sea (IAEA-446) is described and the results of the certification process are presented. The (40)K, (137)Cs, (234)U and (239+240)Pu radionuclides were certified for this material, and information values for 12 other radionuclides ((90)Sr, (99)Tc, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (230)Th, (232)Th, (235)U, (238)U, (239)Pu and (240)Pu) are presented. The CRM can be used for Quality Assurance/Quality Control of analysis of radionuclides in seaweed and other biota samples, as well as for development and validation of analytical methods, and for training purposes. PMID:24291528

  19. Analysis of core soil and water samples from the Cactus Crater Disposal Site at Enewetak atoll

    SciTech Connect

    Robison, W.L.; Noshkin, V.E.

    1981-02-18

    Core soil samples and water samples were collected from the Cactus Crater Disposal Site at Enewetak for analysis of /sup 137/Cs, /sup 90/Sr, /sup 239 +240/Pu and /sup 241/Am by both gamma spectroscopy and, through a contractor laboratory, by wet chemistry procedures. The samples processing methods, the analytical methods and the analytical quality control are all procedures developed for the continuing Marshall Island radioecology and dose assessment work.

  20. Radionuclide Concentrations in Honey Bees from Area G at TA-54 during 1998

    SciTech Connect

    Haarmann, T.K.; Fresquez, P.R.

    1999-06-01

    Honey bees were collected from two colonies located at Los Alamos National Laboratory's Area G, Technical Area 54, and from one control (background) colony located near Jemez Springs, NM. Samples were analyzed for various radionuclides. Area G sample results from both colonies were higher than the upper (95%) level background concentration for {sup 239,240}Pu, {sup 3}H, and total uranium. Sample results from one colony were higher than the upper (95%) level background concentration for {sup 238}Pu.

  1. Accumulation of atmospheric radionuclides and heavy metals in cryoconite holes on an Arctic glacier.

    PubMed

    Łokas, Edyta; Zaborska, Agata; Kolicka, Małgorzata; Różycki, Michał; Zawierucha, Krzysztof

    2016-10-01

    Surface of glaciers is covered by mineral and organic dust, together with microorganisms forming cryoconite granules. Despite fact that glaciers and ice sheets constitute significance part of land surface, reservoir of freshwater, and sites of high biological production, the knowledge on the cryoconite granules still remain unsatisfactory. This study presents information on radionuclide and heavy metal contents in cryoconites. Cryoconites collected from the Hans Glacier in SW Spitsbergen reveal high activity concentrations of anthropogenic ((238,239,240)Pu, (137)Cs, (90)Sr) and natural ((210)Pb) radionuclides. The (238)Pu/(239+240)Pu activity ratios in these cryoconites significantly exceed the mean global fallout ratio (0.025). The (238)Pu/(239+240)Pu ranged from 0.064 to 0.118. The (239+240)Pu/(137)Cs varied from 0.011 ± 0.003 to 0.030 ± 0.007. Such activity ratios as observed in these cryoconites were significantly higher than the values characterizing global fallout, pointing to possible contributions of these radionuclides from other sources. Heavy metals (Pb, Cd, Cu, Zn, Fe, and Mn) in cryoconites exceed both UCC concentrations and local rocks' concentrations, particularly for cadmium. The concentration ratios of stable lead isotopes ((206)Pb/(207)Pb, (208)Pb/(206)Pb) were determined to discriminate between the natural and anthropogenic sources of Pb in cryoconites and to confirm the strong anthropogenic contribution to heavy metal deposition in the Arctic. In investigated cryoconite holes, two groups of invertebrates, both extremophiles, Tardigrada and Rotifera were detected. Our study indicate that cryoconites are aggregates of mineral and organic substances on surfaces of glaciers are able to accumulate large amounts of airborne pollutants bound to extracellular polymeric substances secreted by microorganisms. PMID:27372266

  2. Sources and migration of plutonium in groundwater at the Savannah River site.

    PubMed

    Dai, Minhan; Kelley, James M; Buesseler, Ken O

    2002-09-01

    The isotopic composition, size distribution, and redox speciation of plutonium (Pu) in the groundwater in the vicinity of the F-area seepage basins at the U.S. Department of Energy Savannah River Site (SRS) were examined. A low 240Pu/239Pu ratio in the upstream control well signifies a Pu source otherthan global fallout and indicates reactor-produced Pu. Elevated 240Pu/239Pu atom ratios downstream from the seepage basins are due to the decay of transplutonium isotopes, mainly 244Cm to 240Pu, which were generated at the SRS. Evidence suggests that the migration of basin-released Pu isotopes is minor. Rather, it is the transplutonium isotopes that migrate preferentially downstream and in the process decay to yield progeny Pu isotopes. Size fractionation studies with cross-flow ultrafiltration show that <4% of the 239Pu or 240Pu is found in the colloidal fraction, a finding that is consistent with the higher Pu oxidation states observed in the SRS groundwater. The observation of a low abundance of colloid-associated Pu in SRS groundwater cannot be extrapolated to all sites, but is in contrast to the conclusions of prior groundwater Pu studies at the SRS and elsewhere. This work is unique in its application of a novel combination of sampling and processing protocols as well as its use of thermal ionization mass spectrometry for the detection of Pu isotopes. This allows quantification of the Pu source terms and better determination of the ambient Pu size and redox speciation representative of in situ conditions. PMID:12322739

  3. Solubility of hot fuel particles from Chernobyl--influencing parameters for individual radiation dose calculations.

    PubMed

    Garger, Evgenii K; Meisenberg, Oliver; Odintsov, Oleksiy; Shynkarenko, Viktor; Tschiersch, Jochen

    2013-10-15

    Nuclear fuel particles of Chernobyl origin are carriers of increased radioactivity (hot particles) and are still present in the atmosphere of the Chernobyl exclusion zone. Workers in the zone may inhale these particles, which makes assessment necessary. The residence time in the lungs and the transfer in the blood of the inhaled radionuclides are crucial for inhalation dose assessment. Therefore, the dissolution of several kinds of nuclear fuel particles from air filters sampled in the Chernobyl exclusion zone was studied. For this purpose filter fragments with hot particles were submersed in simulated lung fluids (SLFs). The activities of the radionuclides (137)Cs, (90)Sr, (239+240)Pu and (241)Am were measured in the SLF and in the residuum of the fragments by radiometric methods after chemical treatment. Soluble fractions as well as dissolution rates of the nuclides were determined. The influence of the genesis of the hot particles, represented by the (137)Cs/(239+240)Pu ratio, on the availability of (137)Cs was demonstrated, whereas the dissolution of (90)Sr, (239+240)Pu and (241)Am proved to be independent of genesis. No difference in the dissolution of (137)Cs and (239+240)Pu was observed for the two applied types of SLF. Increased solubility was found for smaller hot particles. A two-component exponential model was used to describe the dissolution of the nuclides as a function of time. The results were applied for determining individual inhalation dose coefficients for the workers at the Chernobyl construction site. Greater dose coefficients for the respiratory tract and smaller coefficients for the other organs were calculated (compared to ICRP default values). The effective doses were in general lower for the considered radionuclides, for (241)Am even by one order of magnitude. PMID:24054559

  4. Radionuclides in fishes and mussels from the Farallon Islands Nuclear Waste Dump Site, California

    SciTech Connect

    Suchanek, T.H.; Lagunas-Solar, M.C.; Carvacho, O.

    1996-08-01

    The Farallon Islands Nuclear Waste Dump Site (FINWDS), approximately 30 miles west of San Francisco, California, received at least 500 TBq encapsulated in more than 47,500 containers from approximately 1945 to 1970. During several seasons in 1986/87 deep-sea bottom feeding fishes (Dover sole = Microstomus pacificus; sablefish = Anoplopoma fimbria; thornyheads = Sebastolobus spp.) and intertidal mussels (Mytilus californianus) were collected from the vicinity of the FINWDS and from comparable depths at a reference site near Point Arena, CA. Tissues were analyzed for several radionuclides ({sup 137}Cs, {sup 238}Pu, {sup 239+240}Pu, and {sup 241}Am). Radionuclide concentrations for fish mussel tissue ranged from non-detectable to 4,340 mBq kg{sup {minus}1} wet weight, with the following means for Farallon fishes: {sup 137}Cs = 1,110 mBq kg{sup {minus}1}; {sup 238}Pu = 390 mBq kg{sup {minus}1}; {sup 239+240}Pu = 130 mBq kg{sup {minus}1}; and {sup 241}Am = 1,350 mBq kg{sup {minus}1}. There were no statistically significant differences in the radionuclide concentrations observed in samples from the Farallon Islands compared to reference samples from Point Arena, CA. Concentrations of both {sup 238}Pu and {sup 241}Am in fish tissues (from both sites) were notably higher than those reported in literature from any other sites worldwide, including potentially contaminated sites. Concentrations of {sup 239+240}Pu from both sites were typical of low values found at some contaminated sites worldwide. These results show {approximately} 10 times higher concentrations of {sup 239+240}Pu and {approximately}40-50 times higher concentrations of {sup 238}Pu than those values reported for identical fish species from 1977 collections at the FINWDS. Radionuclide concentrations were converted to a hypothetical per capita annual radionuclide intake for adults. 51 refs., 5 figs., 3 tabs.

  5. New evaluation of the alpha and gamma emission intensities in the decay of (244)Cm.

    PubMed

    Badikov, Sergey A; Chechev, Valery P

    2016-03-01

    A method for self-consistent evaluation of the absolute emission probabilities for particles and photons accompanying radionuclide decays was applied to the evaluation of the (244)Cm alpha decay data. The absolute emission probabilities evaluated by the method meet the accurate balance relationships. The self-consistency of the results was reached through an iterative scheme of calculations, using the DDEP recommended probabilities for alpha transitions to the five (240)Pu highly excited levels as an initial approximation. PMID:26712410

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

    PubMed

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

    2014-04-01

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

  7. 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 .

  8. Organic nature of colloidal actinides transported in surface water environments.

    PubMed

    Santschi, Peter H; Roberts, Kimberly A; Guo, Laodong

    2002-09-01

    Elevated levels of (239,240)Pu and 241Am have been present in surficial soils of the Rocky Flats Environmental Technology Site (RFETS), CO, since the 1960s, when soils were locally contaminated in the 1960s by leaking drums stored on the 903 Pad. Further dispersion of contaminated soil particles was by wind and water. From 1998 until 2001, we examined actinide ((239,240)Pu and 241Am) concentrations and phase speciation in the surface environment at RFETS through field studies and laboratory experiments. Measurements of total (239,240)Pu and 241Am concentrations in storm runoff and pond discharge samples, collected during spring and summer times in 1998-2000, demonstrate that most of the (239,240)Pu and 241Am transported from contaminated soils to streams occurred in the particulate (> or = 0.45 microm; 40-90%) and colloidal (approximately 2 nm or 3 kDa to 0.45 microm; 10-60%) phases. Controlled laboratory investigations of soil resuspension, which simulated storm and erosion events, confirmed that most of the Pu in the 0.45 microm filter-passing phase was in the colloidal phase (> or = 80%) and that remobilization of colloid-bound Pu during soil erosion events can be greatly enhanced by humic and fulvic acids present in these soils. Most importantly, isoelectric focusing experiments of radiolabeled colloidal matter extracted from RFETS soils revealed that colloidal Pu is in the four-valent state and is mostly associated with a negatively charged organic macromolecule with a pH(IEP) of 3.1 and a molecular weight of 10-15 kDa, rather than with the more abundant inorganic (iron oxide and clay) colloids. This finding has important ramifications for possible remediation, erosion controls, and land-management strategies. PMID:12322742

  9. Plutonium, cesium, uranium and thorium series radionuclides in the Hudson River estuary and other environments. Annual technical progress report, December 1, 1983-November 30, 1984

    SciTech Connect

    Simpson, H.J.; Trier, R.M.; Anderson, R.F.

    1984-01-01

    Radionuclide activities were measured in sediment cores and suspended particle samples from the Hudson River estuary. Activities of /sup 137/Cs, /sup 134/Cs, and /sup 60/Co, /sup 239/ /sup 240/Pu and /sup 238/Pu indicate rapid accumulation in marginal cove areas, and very rapid deposition in the harbor adjacent to New York City, resulting in /sup 239/ /sup 240/Pu accumulations of more than an order of magnitude greater than the fallout delivery rate. Fallout /sup 239/ /sup 240/Pu moving downstream appears to be retained within the system by particle deposition, while more than 50% of the /sup 137/Cs derived from both reactor releases and fallout has been exported. Significant movement of dissolved plutonium into the estuary from adjacent coastal waters may be occurring. Depth profiles of radionuclides are not significantly altered by physical mixing processes in areas accumulating particles at greater than 1 cm/yr. Transport of fallout radionuclides appears to have decreased faster than would be calculated from continuous removal from a well-mixed soil reservoir, indicating that sequestering of a substantial portion of the soil fallout burden has occurred in the watershed soils over the past two decades. Measurements of fallout /sup 239/ /sup 240/Pu in a saline lake with a high carbonate ion concentration yielded water column activities two orders of magnitude greater than that found for fallout plutonium in other continental waters, indicating extensive mobility in some natural water environments. Experiments using lake water suggest that carbonate ions are likely to be important in regulating plutonium solubility in some environments and that low molecular weight complexes are primarily responsible for enhanced plutonium solubility. 45 references, 17 figures, 14 tables.

  10. Plutonium, cesium, uranium, and thorium series radionuclides in the Hudson River estuary and other environments. Annual technical progress report, December 1, 1981-November 30, 1982

    SciTech Connect

    Simpson, H.J.; Trier, R.M.; Anderson, R.F.

    1982-01-01

    Radionuclide activities were measured in a large number of sediment cores and suspended particle samples throughout the salinity range of the Hudson River estuary. Activities of /sup 137/Cs, /sup 134/Cs and /sup 60/Co determined by gamma spectrometry and /sup 239/ /sup 240/Pu and /sup 238/Pu determined by alpha spectrometry indicate reasonably rapid accumulation rates in the sediments of marginal cove areas, and very rapid deposition in the harbor region adjacent to New York City, resulting in /sup 239/ /sup 240/Pu accumulations there more than an order of magnitude greater than the fallout delivery rate. Fallout /sup 239/ /sup 240/Pu moving downstream in the Hudson appears to be almost completely retained within the system by particle deposition, while 80 to 90% of the /sup 137/Cs derived from both reactor releases and fallout has been exported to the coastal waters in solution. Measurements of fallout /sup 239/ /sup 240/Pu in a saline lake with a high carbonate ion concentration yielded water column activities about two orders of magnitude greater than has been found for fallout plutonium in other continental waters, indicating extensive mobility in some natural water environments. Experiments using lake water suggest that carbonate ion is likely to be a critical factor in regulating plutonium solubility in some environments and that low molecular weight complexes are primarily responsible for enhanced plutonium solubility. Activities of several other nuclides of interest in radioactive waste management (/sup 238/U, /sup 234/U, /sup 232/Th, /sup 230/Th, /sup 228/Th, /sup 231/Pa) were also found to be orders of magnitude greater in high carbonate waters than in other natural waters.

  11. Impact of environmental curium on plutonium migration and isotopic signatures.

    PubMed

    Kurosaki, Hiromu; Kaplan, Daniel I; Clark, Sue B

    2014-12-01

    Plutonium (Pu), americium (Am), and curium (Cm) activities were measured in sediments from a former radioactive waste disposal basin located on the Savannah River Site, South Carolina, and in subsurface aquifer sediments collected downgradient from the basin. In situ Kd values (Pu concentration ratio of sediment/groundwater) derived from this field data and previously reported groundwater concentration data compared well to laboratory Kd values reported in the literature. Pu isotopic signatures confirmed multiple sources of Pu contamination. The ratio of (240)Pu/(239)Pu was appreciably lower for sediment samples compared to the associated groundwater. This isotopic ratio difference may be explained by the following: (1) (240)Pu produced by decay of (244)Cm may exist predominantly in high oxidation states (Pu(V)O2(+) and Pu(VI)O2(2+)) compared to Pu derived from the disposed waste effluents, and (2) oxidized forms of Pu sorb less to sediments than reduced forms of Pu. Isotope-specific Kd values calculated from measured Pu activities in the sediments and groundwater indicated that (240)Pu, which is derived primarily from the decay of (244)Cm, had a value of 10 ± 2 mL g(-1), whereas (239)Pu originating from the waste effluents discharged at the site had a value of 101 ± 8 mL g(-1). One possible explanation for the isotope-specific sorption behavior is that (240)Pu likely existed in the weaker sorbing oxidation states, +5 or +6, than (239)Pu, which likely existed in the +3 or +4 oxidation states. Consequently, remediation strategies for radioactively contaminated systems must consider not only the discharged contaminants but also their decay products. In this case, mitigation of Cm as well as Pu will be required to completely address Pu migration from the source term. PMID:25350948

  12. Biogeochemical studies of long-lived radionuclides in marine environments

    SciTech Connect

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

    1985-01-01

    Research results from several studies relevant to seabed dispoal of radioactive wastes are briefly discussed. The studies include: (1) mobilization of plutonium from Enewetak and Bikini lagoon sediments to seawater; (2) concentrations of /sup 90/Sr, /sup 137/Cs, /sup 239+240/Pu, /sup 241/Am, /sup 207/Bi and /sup 210/Pb-/sup 210/Bi-/sup 210/Po in fish from the Marshall Islands; and (3) plutonium in northeast Atlantic sediments. (ACR)

  13. LA-ICP-MS for Pu source identification at Mayak PA, the Urals, Russia.

    PubMed

    Cagno, S; Hellemans, K; Lind, O C; Skipperud, L; Janssens, K; Salbu, B

    2014-02-01

    Information on Pu in environmental samples is traditionally based on the determination of the (240+239)Pu activity via Alpha Spectrometry (AS). A large number of alpha spectrometry sources (planchettes) containing radiochemically separated Pu are therefore stored worldwide and are available for further analyses. These archive samples represent a resource from which valuable information on isotopic composition of alpha emitters including Pu can be obtained. The relative abundances of Pu isotopes can be used to trace specific Pu sources and characterize the relative contributions of different Pu sources in a sample. Thus, in addition to the total (239+240)Pu activity, determination of the (240)Pu/(239)Pu ratio can provide valuable information on the nature of the Pu emitting sources. The Pu isotopic ratios can be determined by mass spectrometry techniques such as Sector Field Inductively Coupled Plasma Mass Spectrometry (SF-ICPMS) or Accelerator Mass Spectrometry (AMS) that require dissolution and complete destruction of the material deposited on the planchettes. In this study Laser Ablation (LA)-quadrupole-ICP-MS has been employed for the analysis of (239)Pu/(240)Pu ratios from alpha-planchettes prepared from samples originating from the Mayak PA nuclear facility, Russia. The results are compared with data from AMS and show that the (240)Pu/(239)Pu ratios obtained by LA-ICP-MS can be utilized to distinguish weapons-grade Pu from civil reprocessing sources. Moreover, isotope ratio mapping can also be performed across the planchettes, allowing e.g. the visualization of possible inhomogeneities in the Pu-isotope distribution on their surface. Thus, this solid sample technique can be applied to extract additional information from existing archives of samples. PMID:24424783

  14. Plutonium as a tracer for soil erosion assessment in northeast China.

    PubMed

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

    2015-04-01

    Soil erosion is one of the most serious environmental and agricultural problems faced by human society. Assessing intensity is an important issue for controlling soil erosion and improving eco-environmental quality. The suitability of the application of plutonium (Pu) as a tracer for soil erosion assessment in northeast China was investigated by comparing with that of 137Cs. Here we build on preliminary work, in which we investigated the potential of Pu as a soil erosion tracer by sampling additional reference sites and potential erosive sites, along the Liaodong Bay region in northeast China, for Pu isotopes and 137Cs. 240Pu/239Pu atomic ratios in all samples were approximately 0.18, which indicated that the dominant source of Pu was the global fallout. Pu showed very similar distribution patterns to those of 137Cs at both uncultivated and cultivated sites. 239+240Pu concentrations in all uncultivated soil cores followed an exponential decline with soil depth, whereas at cultivated sites, Pu was homogenously distributed in plow horizons. Factors such as planted crop types, as well as methods and frequencies of irrigation and tillage were suggested to influence the distribution of radionuclides in cultivated land. The baseline inventories of 239+240Pu and 137Cs were 88.4 and 1688 Bq m(-2) respectively. Soil erosion rates estimated by 239+240Pu tracing method were consistent with those obtained by the 137Cs method, confirming that Pu is an effective tracer with a similar tracing behavior to that of 137Cs for soil erosion assessment. PMID:25544336

  15. Optimization of Heterogeneous Utilization of Thorium in PRWs to Enhance Proliferation Resistance & Reduce Waste

    SciTech Connect

    Mujid Kazimi

    2003-12-18

    Typical pressurized water reactors, although loaded with uranium fuel, produce 225 to 275 kg of plutonium per gigawatt year of operation. Although the spent fuel is highly radioactive, it nevertheless offers a potential proliferation pathway because the plutonium is relatively easy to separate, amounts to many critical masses, and aside from the alpha (n reaction on the 240 Pu isotope) does not present any significant intrinsic barrier to weapon assembly

  16. Distribution and behaviour of transuranic elements in the physical and biological compartments of the channel french shore

    NASA Astrophysics Data System (ADS)

    Germain, P.; Miramand, P.

    1984-06-01

    Biological samples (algae, suspension feeders molluscs living in contact with sediments, annelids), sediments and sea water were taken at 5 stations along the Channel shore from 1978 to 1981 in order to determine 239+240Pu, 238Pu, 241Am and 244Cm levels. In Northern Cotentin, radioactivity levels for 239+240Pu, 238Pu and 241Am were respectively about 1-10, 0.5-7 and 1-19 pCi kg -1 fresh weight in biological samples, 24-90, 11-28 and 24-31 pCi kg -1 dry weight in sediments, 1-7, 5-40 and 2-15 fCi 1 -1 in sea water. For stations far from the La Hague outlet (Seine river and Mont Saint Michel bays) levels for 239+240Pu, 238Pu and 241Am were respectively about 0.3-5, 0.1-2 and 0.2-3 pCi kg -1 fresh weight in biological samples, 30-80, 5-26 and 14-40 pCi kg -1 dry weight in sediments, and 1-, 3-4 and 3-8 fCi 1 -1 in sea water. Labelling of industrial wastes was demonstrated by the values of the 238Pu/ 239+240Pu ratios. The evolution of plutonium isotopes in sea water and in the other environmental compartments and the bio-availability of americium are discussed. Sediment-animal transfers are quantified and their processes specified. An assessment of plutonium and americium hazards from ingestion of molluscs shows that the ingested activity represents 1.1×10 -4 only of the ALI (ingestion) recommended by ICRP for members of the public.

  17. 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

  18. Pu and 137Cs in the Yangtze River estuary sediments: distribution and source identification.

    PubMed

    Liu, Zhiyong; Zheng, Jian; Pan, Shaoming; Dong, Wei; Yamada, Masatoshi; Aono, Tatsuo; Guo, Qiuju

    2011-03-01

    Pu isotopes and (137)Cs were analyzed using sector field ICP-MS and γ spectrometry, respectively, in surface sediment and core sediment samples from the Yangtze River estuary. (239+240)Pu activity and (240)Pu/(239)Pu atom ratios (>0.18) shows a generally increasing trend from land to sea and from north to south in the estuary. This spatial distribution pattern indicates that the Pacific Proving Grounds (PPG) source Pu transported by ocean currents was intensively scavenged into the suspended sediment under favorable conditions, and mixed with riverine sediment as the water circulated in the estuary. This process is the main control for the distribution of Pu in the estuary. Moreover, Pu is also an important indicator for monitoring the changes of environmental radioactivity in the estuary as the river basin is currently the site of extensive human activities and the sea level is rising because of global climate changes. For core sediment samples the maximum peak of (239+240)Pu activity was observed at a depth of 172 cm. The sedimentation rate was estimated on the basis of the Pu maximum deposition peak in 1963-1964 to be 4.1 cm/a. The contributions of the PPG close-in fallout Pu (44%) and the riverine Pu (45%) in Yangtze River estuary sediments are equally important for the total Pu deposition in the estuary, which challenges the current hypothesis that the riverine Pu input was the major source of Pu budget in this area. PMID:21306104

  19. Neutronics Benchmarks for the Utilization of Mixed-Oxide Fuel: Joint U.S./Russian Progress Report for Fiscal Year 1997

    SciTech Connect

    Akkurt, H

    2001-01-11

    In 1967, a series of critical experiments were conducted at the Westinghouse Reactor Evaluation Center (WREC) using mixed-oxide (MOX) PuO{sub 2}-UO{sub 2} and/or UO{sub 2} fuels in various lattices and configurations . These experiments were performed under the joint sponsorship of the Empire State Atomic Development Associates (ESADA) plutonium program and Westinghouse . The purpose of these experiments was to develop experimental data to validate analytical methods used in the design of a plutonium-bearing replacement fuel for water reactors. Three different fuels were used during the experimental program: two MOX fuels and a low-enriched UO{sub 2} fuel. The MOX fuels were distinguished by their {sup 240}Pu content: 8 wt% {sup 240}Pu and 24 wt% {sup 240}Pu. Both MOX fuels contained 2.0 wt % PuO{sub 2} in natural UO{sub 2} . The UO{sub 2} fuel with 2.72 wt % enrichment was used for comparison with the plutonium data and for use in multiregion experiments.

  20. ESADA Plutonium Program Critical Experiments: Power Distribution Measurements

    SciTech Connect

    Akkurt, H.

    2001-06-12

    In 1967, a series of critical experiments were conducted at the Westinghouse Reactor Evaluation Center (WREC) using mixed-oxide (MOX) PuO{sub 2}-UO{sub 2} and/or UO{sub 2} fuels in various lattices and configurations. These experiments were performed under the joint sponsorship of Empire State Atomic Development Associates (ESADA) plutonium program and Westinghouse. The purpose of these experiments was to develop experimental data useful in validating analytical methods used in the design of plutonium-bearing replacement fuel for water reactors. Three different fuel types were used during the experimental program: two MOX fuels and a low-enriched UO{sub 2} fuel. The MOX fuels were distinguished by their {sup 240}Pu content: 8 wt % {sup 240}Pu and 24 wt % {sup 240}Pu. Both MOX fuels contained 2.0 wt % PuO{sub 2} in natural UO{sub 2}. The UO{sub 2} fuel with 2.72 wt % enrichment was used for comparison with the plutonium data and for use in multiregion experiments.

  1. Risk-Quantified Decision-Making at Rocky Flats

    SciTech Connect

    Myers, Jeffrey C.

    2008-01-15

    Surface soils in the 903 Pad Lip Area of the Rocky Flats Environmental Technology Site (RFETS) were contaminated with {sup 239/240}Pu by site operations. To meet remediation goals, accurate definition of areas where {sup 239/240}Pu activity exceeded the threshold level of 50 pCi/g and those below 50- pCi/g needed definition. In addition, the confidence for remedial decisions needed to be quantified and displayed visually. Remedial objectives needed to achieve a 90 percent certainty that unremediated soils had less than a 10 percent chance of {sup 239/240}Pu activity exceeding 50-pCi/g. Removing areas where the chance of exceedance is greater than 10 percent creates a 90 percent confidence in the remedial effort results. To achieve the stipulated goals, the geostatistical approach of probability kriging (Myers 1997) was implemented. Lessons learnt: Geostatistical techniques provided a risk-quantified approach to remedial decision-making and provided visualizations of the excavation area. Error analysis demonstrated compliance and confirmed that more than sufficient soils were removed. Error analysis also illustrated that any soils above the threshold that were not removed would be of nominal activity. These quantitative approaches were useful from a regulatory, engineering, and stakeholder satisfaction perspective.

  2. Dynamics of radionuclide exchange in the calcareous algae Halimeda at Enewetak Atoll

    SciTech Connect

    Spies, R.B.; Marsh, K.V.; Kercher, J.R.

    1981-01-01

    Measurements of /sup 239+240/Pu in the detrital inclusions and in acid-soluble and acid-insoluble fractions of Halimeda macrophysa showed a 10-fold higher concentration in the acid-insoluble coenocytic filaments than in the acid-soluble fraction. In a depuration experiment with Halimeda incrassata at Enewetak Atoll the loss rate of six radionuclides was measured. Data for /sup 60/Co, /sup 137/Cs, and /sup 102m/Rh were fit to loss curves by using one term for exponential loss; data for /sup 155/Eu, /sup 239+240/Pu, and /sup 241/Am required two terms. For each radionuclide, compartment size and transfer functions were determined for the appropriate one- and two-compartment models. Of 26 possible two-compartment models, only seven gave solutions with our data. Nearly identical loss rates were obtained for /sup 155/Eu, /sup 239+240/Pu, and /sup 241/Am in the fast-exchanging compartments for all seven models. The uptake rates for these nuclides were also similar when uptake rates were normalized to local sediment concentrations. The fast-exchanging compartment probably corresponds to the mucilage surface layer of the coenocytic filaments. The identity of the slow-exchanging compartment is less certain but it may correspond to the skeletal surface.

  3. Dynamics of radionuclide exchange in the calcareous algae Halimeda at Enewetak Atoll

    SciTech Connect

    Spies, R.B.; Marsh, K.V.; Kercher, J.R.

    1981-01-01

    Measurements of /sup 239 +240/Pu in the detrital inclusions and in acid-soluble and acid-insoluble fractions of Halimeda macrophysa showed a 10-fold higher concentration in the acid-insoluble coenocytic filaments than in the acid-soluble fraction. In a depuration experiment with Halimeda incrassata at Enewetak Atoll the loss rate of six radionuclides was measured. Data for /sup 60/Co, /sup 137/Cs, and /sup 102//sup m/Rh were fit to loss curves by using one term for exponential loss; data for /sup 155/Eu, /sup 239 +240/Pu, and /sup 241/Am required two terms. For each radionuclide, compartment size and transfer functions were determined for the apropriate one- and two-compartment models. Of 26 possible two-compartment models, only seven gave solutions with our data. Nearly identical loss rates were obtained for /sup 155/Eu, /sup 239 +240/Pu, and /sup 241/Am in the fast-exchanging compartments for all seven models. The uptake rates for these nuclides were also similar when uptake rates were normalized to local sediment concentrations. The fast-exchanging compartment probably corresponds to the mucilage surface layer of the coenocytic filaments. The identity of the slow-exchanging compartment is less certain but it may correspond to the skeletal surface.

  4. Determination of 90Sr and Pu isotopes in contaminated groundwater samples by inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Zoriy, Miroslav V.; Ostapczuk, Peter; Halicz, Ludwik; Hille, Ralf; Becker, J. Sabine

    2005-04-01

    A sensitive analytical method for determining the artificial radionuclides 90Sr, 239Pu and 240Pu at the ultratrace level in groundwater samples from the Semipalatinsk Test Site area in Kazakhstan by double-focusing sector field inductively coupled plasma mass spectrometry (ICP-SFMS) was developed. In order to avoid possible isobaric interferences at m/z 90 for 90Sr determination (e.g. 90Zr+, 40Ar50Cr+, 36Ar54Fe+, 58Ni16O2+, 180Hf2+, etc.), the measurements were performed at medium mass resolution under cold plasma conditions. Pu was separated from uranium by means of extraction chromatography using Eichrom TEVA resin with a recovery of 83%. The limits of detection for 90Sr, 239Pu and 240Pu in water samples were determined as 11, 0.12 and 0.1 fg ml-1, respectively. Concentrations of 90Sr and 239Pu in contaminated groundwater samples ranged from 18 to 32 and from 28 to 856 fg ml-1, respectively. The 240Pu/239Pu isotopic ratio in groundwater samples was measured as 0.17. This isotope ratio indicates that the most probable source of contamination of the investigated groundwater samples was the nuclear weapons tests at the Semipalatinsk Test Site conducted by the USSR in the 1960s.

  5. Uranium comparison by means of AMS and ICP-MS and Pu and 137Cs results around an Italian Nuclear Power Plant

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

    Italy built and commissioned 4 nuclear power plants between 1958-1978, which delivered a total of 1500 MW. All four were closed down after the Chernobyl accident following a referendum in 1987. One of the plants was Garigliano, commissioned in 1959. This plant used a 160 MW BWR1 (SEU of 2.3 %) and was operational from 1964 to 1979, when it was switched off for maintenance. It was definitively stopped in 1982, and is presently being decommissioned. We report here details on the chemistry procedure and on the measurements for soil samples, collected up to 4.5 km from the Nuclear Plant. A comparison between uranium (238U) concentration as determined by means of AMS (Accelerator Mass Spectrometry) and by ICP-MS (Inductively Coupled Plasma-Mass Spectrometry) techniques respectively at the ANU (Australian National University) and at the Ecowise company in Canberra, Australia, is reported, as well as 236U and 239;240Pu concentration results detected by AMS. 236U/238U and 240Pu/239Pu isotopic ratios by means of AMS are also provided. A contamination from Chernobyl is visible in the 137Cs/239+240Pu activity ratio measurements.

  6. Sediment studies at Bikini Atoll part 2. inventories of transuranium elements in surface sediments

    SciTech Connect

    Noshkin, V.E.; Eagle, R.J.; Wong, K.M.; Robison, W.L.

    1997-10-01

    This is the second of three reports on Bikini sediment studies, which discusses the concentrations and inventories of {sup 241}Am and {sup 239+240}Pu in sediments from the lagoon. Surface sediment samples were collected from 87 locations over the entire lagoon at Bikini Atoll during 1979. The collections were made to map the distribution of long-lived radionuclides associated with the bottom material and to show what modifications occurred in the composition of the sediment as a result of the testing program. Present inventories for {sup 241}Am and {sup 239+240}Pu in the surface 2 cm of sediment are estimated to be 14 and 17 TBq, respectively. These values are estimated to represent only 14% of the total inventory in the sediment column. Sediment inventories of {sup 239+240}Pu and {sup 241}Am are changing only slowly with time through chemical- physical processes that continuously mobilize small amounts of the transuranics to the water column. The lowest concentrations and inventories are associated with deposits logoonward of the eastern reef.

  7. Determination of alpha-emitting Pu isotopes in environmental samples.

    PubMed

    Vioque, I; Manjón, G; García-Tenorio, R; El-Daoushy, F

    2002-04-01

    This paper presents an improved radiochemical procedure for the determination of alpha-emitting Pu isotopes in environmental samples (soils, sediments, vegetation) by alpha-particle spectrometry. Quantitative Pu recovery yields were obtained (average 60%), 0.1 mBq being the average minimum detectable activity by the complete technique. Special efforts were made to ensure the removal of traces of different natural alpha-emitting radionuclides, which can interfere with the correct determination of 239+240Pu and 238Pu concentrations. The radiochemical procedure was validated by application to reference material and by participation in intercomparison exercises. This radiochemical procedure was applied to the different layers of a high-resolution sediment core taken from a lake in Sweden. The 239+240Pu and 238Pu/239+240Pu profiles obtained in the high-resolution sediment core correctly reproduced the expected evolution of these quantities as observed historically in the atmosphere, validating the procedure for this purpose and showing the power of these radionuclides for dating purposes. PMID:12022654

  8. 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. PMID:21890207

  9. Development of Metallic Magnetic Calorimeters for Nuclear Safeguards Applications

    SciTech Connect

    Bates, Cameron Russell

    2015-03-11

    Many nuclear safeguards applications could benefit from high-resolution gamma-ray spectroscopy achievable with metallic magnetic calorimeters. This dissertation covers the development of a system for these applications based on gamma-ray detectors developed at the University of Heidelberg. It demonstrates new calorimeters of this type, which achieved an energy resolution of 45.5 eV full-width at half-maximum at 59.54 keV, roughly ten times better than current state of the art high purity germanium detectors. This is the best energy resolution achieved with a gamma-ray metallic magnetic calorimeter at this energy to date. In addition to demonstrating a new benchmark in energy resolution, an experimental system for measuring samples with metallic magnetic calorimeters was constructed at Lawrence Livermore National Laboratory. This system achieved an energy resolution of 91.3 eV full-width at half-maximum at 59.54 keV under optimal conditions. Using this system it was possible to characterize the linearity of the response, the count-rate limitations, and the energy resolution as a function of temperature of the new calorimeter. With this characterization it was determined that it would be feasible to measure 242Pu in a mixed isotope plutonium sample. A measurement of a mixed isotope plutonium sample was performed over the course of 12 days with a single two-pixel metallic magnetic calorimeter. The relative concentration of 242Pu in comparison to other plutonium isotopes was determined by direct measurement to less than half a percent accuracy. This is comparable with the accuracy of the best-case scenario using traditional indirect methods. The ability to directly measure the relative concentration of 242Pu in a sample could enable more accurate accounting and detection of indications of undeclared activities in nuclear safeguards, a better constraint on source material in forensic samples containing plutonium, and improvements in verification in a future plutonium

  10. Development of Metallic Magnetic Calorimeters for Nuclear Safeguards Applications

    NASA Astrophysics Data System (ADS)

    Bates, Cameron Russell

    Many nuclear safeguards applications could benefit from high-resolution gamma-ray spectroscopy achievable with metallic magnetic calorimeters. This dissertation covers the development of a system for these applications based on gamma-ray detectors developed at the University of Heidelberg. It demonstrates new calorimeters of this type, which achieved an energy resolution of 45.5 eV full-width at half-maximum at 59.54 keV, roughly ten times better than current state of the art high purity germanium detectors. This is the best energy resolution achieved with a gamma-ray metallic magnetic calorimeter at this energy to date. In addition to demonstrating a new benchmark in energy resolution, an experimental system for measuring samples with metallic magnetic calorimeters was constructed at Lawrence Livermore National Laboratory. This system achieved an energy resolution of 91.3 eV full-width at half-maximum at 59.54 keV under optimal conditions. Using this system it was possible to characterize the linearity of the response, the count-rate limitations, and the energy resolution as a function of temperature of the new calorimeter. With this characterization it was determined that it would be feasible to measure 242Pu in a mixed isotope plutonium sample. A measurement of a mixed isotope plutonium sample was performed over the course of 12 days with a single two-pixel metallic magnetic calorimeter. The relative concentration of 242Pu in comparison to other plutonium isotopes was determined by direct measurement to less than half a percent accuracy. This is comparable with the accuracy of the best-case scenario using traditional indirect methods. The ability to directly measure the relative concentration of 242Pu in a sample could enable more accurate accounting and detection of indications of undeclared activities in nuclear safeguards, a better constraint on source material in forensic samples containing plutonium, and improvements in verification in a future plutonium

  11. Radiological Aspects of Deep-Burn Fusion-Fission Hybrid Waste in a Repository

    SciTech Connect

    Shaw, H F; Blink, J A; Farmer, J C; Karmer, K J; Latkowski, J F; Zhao, P

    2008-11-25

    The quantity, radioactivity, and isotopic characteristics of the spent fission fuel from a hybrid fusion-fission system capable of extremely high burnups are described. The waste generally has higher activity per unit mass of heavy metal, but much lower activity per unit energy generated. The very long-term radioactivity is dominated by fission products. Simple scaling calculations suggest that the dose from a repository containing such waste would be dominated by {sup 129}I, {sup 135}Cs, and {sup 242}Pu. Use of such a system for generating energy would greatly reduce the need for repository capacity.

  12. Fission cross section calculations of actinides with EMPIRE code

    SciTech Connect

    Sin, M.; Oblozinsky, P.; Herman,M.; Capote,R.

    2010-04-30

    The cross sections of the neutron induced reactions on {sup 233,234,236}U, {sup 237}Np, {sup 238,242}Pu, {sup 241,243}Am, {sup 242,246}Cm carried out in the energy range 1 keV-20 MeV with EMPIRE code are presented, emphasizing the fission channel. Beside a consistent, accurate set of evaluations, the paper contains arguments supporting the choice of the reaction models and input parameters. A special attention is paid to the fission parameters and their uncertainties.

  13. Reproducibility and calibration of MMC-based high-resolution gamma detectors

    DOE PAGESBeta

    Bates, C. R.; Pies, C.; Kempf, S.; Hengstler, D.; Fleischmann, A.; Gastaldo, L.; Enss, C.; Friedrich, S.

    2016-07-15

    Here, we describe a prototype γ-ray detector based on a metallic magnetic calorimeter with an energy resolution of 46 eV at 60 keV and a reproducible response function that follows a simple second-order polynomial. The simple detector calibration allows adding high-resolution spectra from different pixels and different cool-downs without loss in energy resolution to determine γ-ray centroids with high accuracy. As an example of an application in nuclear safeguards enabled by such a γ-ray detector, we discuss the non-destructive assay of 242Pu in a mixed-isotope Pu sample.

  14. Reproducibility and calibration of MMC-based high-resolution gamma detectors

    NASA Astrophysics Data System (ADS)

    Bates, C. R.; Pies, C.; Kempf, S.; Hengstler, D.; Fleischmann, A.; Gastaldo, L.; Enss, C.; Friedrich, S.

    2016-07-01

    We describe a prototype γ-ray detector based on a metallic magnetic calorimeter with an energy resolution of 46 eV at 60 keV and a reproducible response function that follows a simple second-order polynomial. The simple detector calibration allows adding high-resolution spectra from different pixels and different cool-downs without loss in energy resolution to determine γ-ray centroids with high accuracy. As an example of an application in nuclear safeguards enabled by such a γ-ray detector, we discuss the non-destructive assay of 242Pu in a mixed-isotope Pu sample.

  15. Actinide neutron-induced fission cross section measurements at LANSCE

    SciTech Connect

    Tovesson, Fredrik K; Laptev, Alexander B; Hill, Tony S

    2010-01-01

    Fission cross sections of a range of actinides have been measured at the Los Alamos Neutron Science Center (LANSCE) in support of nuclear energy applications in a wide energy range from sub-thermal energies up to 200 MeV. A parallel-plate ionization chamber are used to measure fission cross sections ratios relative to the {sup 235}U standard while incident neutron energies are determined using the time-of-flight method. Recent measurements include the {sup 233,238}U, {sup 239-242}Pu and {sup 243}Am neutron-induced fission cross sections. Obtained data are presented in comparison with ex isting evaluations and previous data.

  16. Report of hot-lab activities at the University of Munich

    NASA Astrophysics Data System (ADS)

    Grossmann, R.; Maier, H. J.; Friebel, H. U.

    2006-05-01

    In the hot-lab facility of the University of Munich a technological equipment of newest standard enables the production of radioactive targets of highest quality. In the last 2 years targets have been prepared of the following nuclides: 14C, 235U, 238U, 232Th, 242Pu and 99Tc. Thereby, not only have standard target frames with carbon or tantalum backings been used, but also special plunger target assemblies with stretched flat nickel or titanium backing foils. A special task was the preparation of sputter targets in the form of Fe 314C pellets.

  17. Experiments on the Synthesis of Superheavy Elements with 48CA Beams at the Separator Vassilissa

    NASA Astrophysics Data System (ADS)

    Oganessian, Yu. Ts.; Yeremin, A. V.; Belozerov, A. V.; Chelnokov, M. L.; Chepigin, V. I.; Gorshkov, V. A.; Kabachenko, A. P.; Korotkov, S. P.; Malyshev, O. N.; Popeko, A. G.; Roháč, J.; Sagaidak, R. N.; Hofmann, S.; Münzenberg, G.; Veselsky, M.; Saro, S.; Iwasa, N.; Morita, K.; Giardina, G.

    2001-04-01

    The study of the decay properties and formation cross sections of the isotopes of elements 110, 112 and 114 were performed at the FLNR JINR with the use of the high intensity 48Ca beams and an electrostatic separator VASSILISSA. 232Th, 238U and 242Pu targets were used in the experiments. At the beam energies corresponding to the calculated cross section maxima of the 3n evaporation channels the isotopes 277110, 283112 and 287114 were produced and identified. The cross section limits were obtained at excitation energies of the compound nucleus corresponding to the maxima of the 4n evaporation channels for the reactions with 232Th and 238U targets.

  18. Sources, distribution, and mobility of plutonium and radiocesium in soils, sediments and water of the Hudson River Estuary and watershed

    SciTech Connect

    Linsalata, P.

    1984-01-01

    Results of /sup 239/ /sup 240/Pu, /sup 238/Pu and /sup 137/Cs measurements are reported for soil cores sampled within the watershed, for many sediment cores and surface dredge samples taken along the length of the Hudson River Estuary and for water samples collected on a continuous basis in both fresh and estuarine reaches. Accumulations of /sup 239/ /sup 240/Pu and /sup 137/Cs measured within sediment cores taken from discrete regions of the river-estuary were summed to arrive at total sediment inventories of 1.6 +/- 0.7 Ci and 53 +/- 20 Ci, respectively. The variability observed in the sediment accumulation of radionuclides is discussed in terms of the physical and chemical characteristics of the river-estuary. Plutonium-239,240 and /sup 137/Cs were similary distributed in sediments and water sampled from fresh water reaches of the Hudson with activity ratios (i.e., /sup 239/ /sup 240/Pu//sup 1/2number/sup 7/Cs) ranging from 0.01 to 0.03. Distribution coefficients, which were determined both in vitro and in situ were similar for both nuclides (i.e., from 1 x 10/sup 5/ to 3 x 10/sup 5/ L.kg/sup -1/) in fresh water, but diverged significantly (as a result of increased /sup 137/Cs solubility) in brackish waters that exhibited chlorinities in excess of 1-2 g Cl/sup -/.L/sup -1/. The concentrations of /sup 239/ /sup 240/Pu and /sup 137/Cs observed in fresh water samples were primarily functions of the suspended load. Approximately 60-70% of the annual downstream transport of /sup 239/ /sup 240/Pu and /sup 137/Cs calculated during 1980 and 1981 (i.e., 4 +/- 0.5 mCi and 515 +/- 84 mCi, respectively) was associated with suspended particulates greater than or equal to 0.45 ..mu..m. An empirical model was developed to determine the rates of vertical migration of these nuclides in soils of the watershed.

  19. Organic matter controls on iodine and plutonium in atmospheric depositions, streams, and soils in the Fukushima Prefecture

    NASA Astrophysics Data System (ADS)

    Xu, C.; Zhang, S.; Sugiyama, Y.; Ohte, N.; Ho, Y. F.; Fujitake, N.; Kaplan, D. I.; Yeager, C. M.; Schwehr, K. A.; Santschi, P. H.

    2015-12-01

    In order to assess how environmental factors are controlling the distribution and migration of radioiodine and plutonium that were emitted from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, we quantified iodine and 239,240Pu concentration changes in soil samples with different land uses (urban, paddy, deciduous forest and coniferous forest), as well as iodine speciation in surface water and rainwater. A ranking of the land uses by their stable 127I and by their 239,240Pu concentrations were quite distinct from that of 134,137Cs, indicating 137Cs might not be a good geochemical proxy for radioactive 129I or Pu in the long-term, post-FDNPP accident. Being a proxy for the long-term fate of 129I, soil 127I content was well correlated to soil organic matter (SOM) content, regardless of land use type, suggesting that SOM might be an important factor controlling iodine biogeochemistry. Other soil chemical properties, such as Eh and pH, had strong correlations to soil 127I content, but only within a given land use (e.g., within urban soils). Organic carbon (OC) and Eh were positively, and pH was negatively correlated to 127I concentrations in surface water and rain samples. It is also noticeable that 127I in the bulk deposition was concentrated along the rainwater passage likely due to plant evapotranspiration activity, with all inorganic iodine being completely converted to organo-iodine by plant organic matter. 239,240Pu activities of all soil samples were well within the global fallout range, but the Fukushima-derived 239,240Pu was detectable at a distance ~61 km away, NW of FDNPP. However, it is confined to the litter layer, even three years after the FDNPP accident-derived emissions. 239,240Pu activities were significantly correlated with soil OC and nitrogen contents, indicating Pu may be associated with nitrogen-containing SOM, similar to what has been observed at other locations in the United States, e.g., Savannah River Site (SRS) and Rocky Flats

  20. Isomeric ratio measurements with the ILL LOHENGRIN spectrometer

    NASA Astrophysics Data System (ADS)

    Chebboubi, A.; Kessedjian, G.; Litaize, O.; Serot, O.; Faust, H.; Bernard, D.; Blanc, A.; Köster, U.; Méplan, O.; Mutti, P.; Sage, C.

    2016-03-01

    The modelling of γ heating and neutron damage inside a nuclear reactor is essential to design the next generation of nuclear reactors. The determination of the fission fragment momentum is a key element to perform accurate calculations of the γ heating. One way to assess this information is to look at the isomeric ratio of different nuclei. According to the lifetime of the isomeric state, different experimental techniques were developed at the LOHENGRIN spectrometer. A focus on the measurement of isomeric ratios of 136I in neutron induced fission of 241Pu is presented. A discussion with the current assumptions used in the evaluation process for isomeric ratio is also shown.

  1. Present Status of Nuclear Data for Nuclear Nonproliferation

    NASA Astrophysics Data System (ADS)

    Igashira, M.

    2015-10-01

    The present status of nuclear data was reviewed from the viewpoint of the research and development of non-destructive inspection methods for international controlled materials such as 235U, 239Pu, 241Pu, D2O, 6LiD, and 9Be. The nuclear characteristics of these materials were discussed, and neutron- and photon-reaction cross section data were reviewed. It was found that the accuracy of neutron data was enough for the research and development but that of photon data was not enough.

  2. Production and Decay of Element 114 Isotopes with the BGS (LBNL) and TASCA (GSI)

    NASA Astrophysics Data System (ADS)

    Gates, Jacklyn

    2010-11-01

    During the last 10 years, the Dubna Gas Filled Recoil Separator (DGFRS) group has published numerous reports of the production and decay of superheavy elements (SHE) with Z=112-118 in ^48Ca irradiations of actinide targets. Recently the production of element 114 in the ^242Pu(^48Ca,3-4n) reaction was verified at the Lawrence Berkeley National Laboratory using the Berkeley Gas-filled Separator (BGS). Later experiments at the BGS successfully extended the region of known SHE nuclides along the neutron-deficient side using the ^242Pu(^48Ca,5n)^285114 reaction. Almost concurrently with the BGS, the TransActinide Separator and Chemistry Apparatus at the GSI Helmholtzzentrum fúr Schwerionenforschung investigated the ^244Pu(^48Ca,3-4n) reaction and observed cross sections on the order of 10 pb for the production of element 114 when the more neutron-rich ^244Pu target was used. An alpha-decay branch in ^281Ds was also discovered, leading to the new nucleus ^277Hs. Cross sections, decay modes and decay properties all agree with those published by the DGFRS group. Implications of these results on the field of heavy elements will be discussed.

  3. Oxidation state and local structure of plutonium reacted with magnetite, mackinawite, and chukanovite.

    PubMed

    Kirsch, Regina; Fellhauer, David; Altmaier, Marcus; Neck, Volker; Rossberg, Andre; Fanghänel, Thomas; Charlet, Laurent; Scheinost, Andreas C

    2011-09-01

    Due to their redox reactivity, surface sorption characteristics, and ubiquity as corrosion products or as minerals in natural sediments, iron(II)-bearing minerals control to a large extent the environmental fate of actinides. Pu-L(III)-edge XANES and EXAFS spectra were used to investigate reaction products of aqueous (242)Pu(III) and (242)Pu(V) reacted with magnetite, mackinawite, and chukanovite under anoxic conditions. As Pu concentrations in the liquid phase were rapidly below detection limit, oxidation state and local structure of Pu were determined for Pu associated with the solid mineral phase. Pu(V) was reduced in the presence of all three minerals. A newly identified, highly specific Pu(III)-sorption complex formed with magnetite. Solid PuO(2) phases formed in the presence of mackinawite and chukanovite; in the case of chukanovite, up to one-third of plutonium was also present as Pu(III). This highlights the necessity to consider, under reducing anoxic conditions, Pu(III) species in addition to tetravalent PuO(2) for environmental risk assessment. Our results also demonstrate the necessity to support thermodynamic calculations with spectroscopic data. PMID:21755920

  4. New antineutrino energy spectra predictions from the summation of beta decay branches of the fission products.

    PubMed

    Fallot, M; Cormon, S; Estienne, M; Algora, A; Bui, V M; Cucoanes, A; Elnimr, M; Giot, L; Jordan, D; Martino, J; Onillon, A; Porta, A; Pronost, G; Remoto, A; Taín, J L; Yermia, F; Zakari-Issoufou, A-A

    2012-11-16

    In this Letter, we study the impact of the inclusion of the recently measured beta decay properties of the (102;104;105;106;107)Tc, (105)Mo, and (101)Nb nuclei in an updated calculation of the antineutrino energy spectra of the four fissible isotopes (235,238)U and (239,241)Pu. These actinides are the main contributors to the fission processes in pressurized water reactors. The beta feeding probabilities of the above-mentioned Tc, Mo, and Nb isotopes have been found to play a major role in the γ component of the decay heat of (239)Pu, solving a large part of the γ discrepancy in the 4-3000 s range. They have been measured by using the total absorption technique, insensitive to the pandemonium effect. The calculations are performed by using the information available nowadays in the nuclear databases, summing all the contributions of the beta decay branches of the fission products. Our results provide a new prediction of the antineutrino energy spectra of (235)U, (239,241)Pu, and, in particular, (238)U for which no measurement has been published yet. We conclude that new total absorption technique measurements are mandatory to improve the reliability of the predicted spectra. PMID:23215477

  5. WDC - Advanced system for characterization of {alpha}-bearing waste in 200 l and 400 l drums: performances and lessons learned from the first industrial measurement campaigns

    SciTech Connect

    Libens, A.; Vandorpe, M.; Cuchet, J.M.

    2007-07-01

    The Waste Drum Characterization installation was originally developed for the assay of alpha-bearing waste in standard 200 1 (55 gallons) drums during the dismantling operations of the Siemens mixed-oxide (MOX) facility in Hanau (Germany). That installation was validated and qualified by the German authorities, its main performances being: - Counting efficiency for coincident neutrons: approx. 1%; Lowest Limit of Detection (LLD): 75 mg {sup 240}Pu{sub eq}; Pu content per drum: up to 100 g tot. (35 g {sup 240}Pu{sub eq}) - Measurement duration: approx. 20 minutes. The success of this system, a passive neutron coincidence counter combined with a high resolution gamma spectrometer, led to the radiological characterization and qualification of about 1,700 drums during the period 2001 - 2004. In 2005, after completion of the dismantling operations of the Siemens MOX facility, Tecnubel took over the WDC installation which could be used in the frame of the future dismantling of the Belgonucleaire's MOX plant in Dessel (Belgium), which can be comparable to the Siemen's one. This second (and new) life for the WDC means that it must be rigorously retested and validated against the Belgian authorities requirements. Furthermore, and additionally to the future use in the Belgonucleaire's facility, Tecnubel was faced with new challenges, namely: Assay of 400 l drums together with the 200 l packages; Determination of the real LLD taking into account the background in different Belgian nuclear facilities, the determination of a value of {approx}5 mg {sup 240}Pu{sub eq} being an objective; - Assay of mixed alpha/beta-gamma wastes; Transportability of the WDC from one plant to another; Assistance to different nuclear operators for the licensing of the WDC for their own waste types. This paper describes the installation itself and its performances, presents the difficulties encountered during the new challenge and the results of the performed revalidation tests; it gives the

  6. The effect of carbonate soil on transport and dose estimates for long-lived radionuclides at a U.S. Pacific test site

    SciTech Connect

    Conrado, C L; Hamilton, T F; Robison, W L; Stoker, A C

    1999-01-01

    The US conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are Cesium-137 ({sup 137}Cs), Strontium-90 ({sup 90}Sr), Plutonium-239+240 ({sup 239+240}Pu) and Americium-241 ({sup 241}Am). {sup 137}Cs in the coral soils is more available for uptake by plants than {sup 137}Cs associated with continental soils of North America or Europe. Soil-to-plant {sup 137}Cs median concentration ratios (CR) (kBq kg{sup {minus}1} dry weight plant/kBq kg{sup {minus}1} dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, {sup 90}Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of {sup 137}Cs and {sup 90}Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for {sup 239+240}Pu and {sup 241}Am are very similar to those observed in continental soils. Values range from 10{sup {minus}6} to 10{sup {minus}4} for both {sup 239+240}Pu and {sup 241}Am. No significant difference is observed between the two in coral soil.

  7. 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.

  8. Plutonium gamma-ray measurements for mutual reciprocal inspections of dismantled nuclear weapons

    SciTech Connect

    Koenig, Z.M.; Carlson, J.B.; Clark, D.; Gosnell, T.B.

    1995-07-01

    The O`Leary-Mikhailov agreement of March 1994 stated that the U.S. and the Russian Federation would engage in mutual reciprocal inspections (MRI) of fissile materials removed from dismantled nuclear weapons. It was decided to begin with the plutonium (Pu) removed from dismantled weapons and held in storage containers. Later discussions between U.S. and Russian technical experts led to the conclusion that, to achieve the O`Leary-Mikhailov objectives, Pu MRI would need to determine that the material in the containers has properties consistent with a nuclear-weapon component. Such a property is a {sup 240}Pu/{sup 239}Pu ratio consistent with weapons-grade material. One of the candidate inspection techniques under consideration for Pu MRI is to use a narrow region (630-670 keV) of the plutonium gamma-ray spectrum, taken with a high-purity germanium detector, to determine that it is weapons-grade plutonium as well as to estimate the minimum mass necessary to produce the observed gamma-ray intensity. We developed software (the Pu600 code) for instrument control and analysis especially for this purpose. In November 1994, U.S. and Russian scientists met at the Lawrence Livermore National Laboratory for joint experiments to evaluate candidate Pu MRI inspection techniques. In one of these experiments, gamma-ray intensities were measured from three unclassified weapons-grade plutonium source standards and one reactor-grade standard (21% {sup 240}pu). Using our software, we determined the {sup 240}Pu/{sup 239}Pu ratio of these standards to accuracies within {+-}10%, which is adequate for Pu MRI. The minimum mass estimates varied, as expected, directly with the exposed surface area of the standards.

  9. Plutonium and other alpha emitters in mushrooms from Poland, Spain and Ukraine.

    PubMed

    Mietelsk, J W; Baeza, A S; Guillen, J; Buzinny, M; Tsigankov, N; Gaca, P; Jasińska, M; Tomankiewicz, E

    2002-05-01

    The paper presents results on Pu, U and Th isotope activity concentration measurements in some mushroom samples collected in Poland, Spain and Ukraine. The sampling sites differ a lot with regard to observed levels of Pu, its origin and isotope ratios as well as the environmental properties. Some of the Polish samples were collected in the northeastern part of the country with up to 30 Bq/m2 of Chernobyl Pu deposition. Other Polish and the Spanish samples are from areas with almost exclusively global fallout Pu present. Ukrainian samples were collected in a highly contaminated area with a deposition of about 3.7 kBq/m2 of Chernobyl (239-240)Pu. The maximum (239+240)Pu activity concentration was found equal to (54+/-4) Bq/kg (dw--dry weight) for a Ukrainian Cantharellus cibarius sample. Ukrainian samples have an extremely high radiocesium level, with maximum of (51+/-4) MBq/kg (dw). The maximum (239+240)Pu activity concentration for Polish samples was (81+/-5) mBq/kg (dw) for Xerocomus badius. From the isotopic ratio in this sample it can be concluded that Chernobyl fallout is the origin of Pu. More than twice as large was the Spanish maximum for Hebeloma cylindrosporum but with only global fallout Pu. Some aspects of the transfer of nuclides to fruit bodies is discussed and in some cases the transfer factors or aggregation coefficients were calculated. Especially high transfer factors were found for Hebeloma cylindrosporum from Spain. PMID:11993947

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

    PubMed

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

    2013-09-01

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

  11. Historical trace element distribution in sediments from the Mississippi River delta

    USGS Publications Warehouse

    Swarzenski, P.W.; Baskaran, M.; Rosenbauer, R.J.; Orem, W.H.

    2006-01-01

    Five sediment cores were collected on the shelf of the inner Mississippi Bight in June 2003 for a suite of radionuclides to establish geochronologies and trace elements to examine patterns of contaminant deposition and accumulation. Core sites were chosen to reflect a matrix of variable water depths, proximity to the Mississippi River mouth as the primary source for terrigenous particles, and extent and duration of summertime water column hypoxia. The vertical distribution of 239,240Pu and 210Pbxs (= 210Pbtotal - 226Ra) provided reliable geochronological age constraints to develop models for mass accumulation rates and historic trace element inputs and variations. Mass accumulation rates ranged from 0.27 to 0.87 g cm-2 yr-1 and were internally consistent using either 210Pbxs or 239,240Pu. Measured inventories of 137Cs, 239,240Pu, and 210Pbxs were compared to atmospheric deposition rates to quantify potential sediment focusing or winnowing. Observed variability in calculated mass accumulation rates may be attributed foremost to site-specific proximity to the river mouth (i.e., sediment source), variability in water depth, and enhanced sediment focusing at the Mississippi River canyon site. Trace element concentrations were first normalized to Al, and then Al-normalized enrichment factors (ANEF) were calculated based on preanthropogenic and crustal trace element abundances. These ANEFs were typically > 1 for V and Ba, while for most other elements studied, either no enrichment or depletion was observed. The enrichment of Ba may be related, in part, to the seasonal occurrence of oxygen-depleted subsurface waters off the Mississippi River delta, as well as being an ubiquitous by-product of the petroleum industry. ?? 2006 Estuarine Research Federation.

  12. Short term soil erosion dynamics in alpine grasslands - Results from a Fallout Radionuclide repeated-sampling approach

    NASA Astrophysics Data System (ADS)

    Arata, Laura; Meusburger, Katrin; Zehringer, Markus; Ketterer, Michael E.; Mabit, Lionel; Alewell, Christine

    2016-04-01

    Improper land management and climate change has resulted in accelerated soil erosion rates in Alpine grasslands. To efficiently mitigate and control soil erosion and reduce its environmental impact in Alpine grasslands, reliable and validated methods for comprehensive data generation on its magnitude and spatial extent are mandatory. The use of conventional techniques (e.g. sediment traps, erosion pins or rainfall simulations) may be hindered by the extreme topographic and climatic conditions of the Alps. However, the application of the Fallout Radionuclides (FRNs) as soil tracers has already showed promising results in these specific agro-ecosystems. Once deposited on the ground, FRNs strongly bind to fine particles at the surface soil and move across the landscape primarily through physical processes. As such, they provide an effective track of soil and sediment redistribution. So far, applications of FRN in the Alps include 137Cs (half-life: 30.2 years) and 239+240Pu (239Pu [half-life = 24110 years] and 240Pu [half-life = 6561 years]). To investigate short term (4-5 years) erosion dynamics in the Swiss Alps, the authors applied a FRNs repeated sampling approach. Two study areas in the central Swiss Alps have been investigated: the Urseren Valley (Canton Uri), where significant land use changes occurred in the last centuries, and the Piora Valley (Canton Ticino), where land use change plays a minor role. Soil samples have been collected at potentially erosive sites along the valleys over a period of 4-5 years and measured for 137Cs and 239+240Pu activity. The inventory change between the sampling years indicates high erosion and deposition dynamics at both valleys. High spatial variability of 137Cs activities at all sites has been observed, reflecting the heterogeneous distribution of 137Cs fallout after the Chernobyl power plant accident in 1986. Finally, a new modelling technique to convert the inventory changes to quantitative estimates of soil erosion has

  13. Anharmonicity of the excited octupole band in actinides using supersymmetric quantum mechanics

    NASA Astrophysics Data System (ADS)

    Jolos, R. V.; von Brentano, P.; Casten, R. F.

    2013-09-01

    Background: Low-lying octupole collective excitations play an important role in the description of the structure of nuclei in the actinide region. Ground state alternating parity rotational bands combining both positive and negative parity states are known in several nuclei. However, only recently it has been discovered in 240Pu an excited positive parity rotational band having an octupole nature and demonstrating strong anharmonicity of the octupole motion in the band head energies.Purpose: To suggest a model describing both ground state and excited alternating parity bands, which includes a description of the anharmonic effects in the bandhead excitation energies and can be used to predict the energies of the excited rotational bands of octupole nature and the E1 transition probabilities.Methods: The mathematical technique of the supersymmetric quantum mechanics with a collective Hamiltonian depending only on the octupole collective variable which keeps axial symmetry is used to describe the ground state and excited alternating parity rotational bands.Results: The excitation energies of the states belonging to the lowest negative parity and the excited positive parity bands are calculated for 232Th, 238U, and 240Pu. The E1 transition matrix elements are also calculated for 240Pu.Conclusions: It is shown that the suggested model describes the excitation energies of the states of the lowest negative parity band with the accuracy around 10 keV. The anharmonicity in the bandhead energy of the excited positive parity band is described also. The bandhead energy of the excited positive parity band is described with the accuracy around 100 keV.

  14. Evaluating global atmospheric transport of plutonium with dust aerosols

    NASA Astrophysics Data System (ADS)

    Velarde, R.; Arimoto, R.; Gill, T. E.; Kang, C.; Goodell, P.

    2009-12-01

    The resuspension of soils contaminated with radionuclides from nuclear weapons tests is a mechanism by which plutonium can be re-distributed throughout the environment. To better understand the global atmospheric transport of plutonium, we measured the activity of Pu in aerosol samples from four widely separated sites that receive dust from distant sources in both Asia and Africa. High-volume aerosol samples were collected from Barbados (2005 - 2006); Gosan, South Korea (2005 - 2006); Izaña, Canary Islands (1989 - 1996); and Mauna Loa Observatory, Hawaii (2005 - 2006) to evaluate the relationship between Pu activity and mineral dust concentrations (using crustal elements such as aluminum as a dust proxy). The activity of 239,240Pu (239Pu + 240Pu) in the aerosol samples was determined by alpha spectrometry following a series of chemical separations. Concentrations of other elements were determined by a variety of techniques. Pu activity was below the detection limit in many samples. In those samples where it was detected, the Gosan site had the highest dust concentrations and highest total plutonium activity, while Mauna Loa Observatory had the lowest dust concentrations and lowest 239,240Pu activity. The Izaña samples had the second highest concentrations of dust and plutonium activity, while Barbados had the third highest levels of both crustal aerosols and plutonium activity. The dust concentrations are consistent with previous observations at these remote sites, and we propose that the plutonium (primarily from past atmospheric nuclear weapons testing, much of which took place in arid lands) was deposited on erodible soil surfaces and subsequently transported as part of the overall mineral dust load. The results of this study have implications for the global transport and fate of Pu through its association with dust, the biogeochemical and environmental impacts of other substances associated with dust, and the workings of the dust cycle itself.

  15. Radionuclide concentrations in honey bees from Area G at TA-54 during 1997. Progress report

    SciTech Connect

    Haarmann, T.K.; Fresquez, P.R.

    1998-07-01

    Honey bees were collected from two colonies located at Los Alamos National Laboratory`s Area G, Technical Area 54, and from one control (background) colony located near Jamez Springs, NM. Samples were analyzed for the following: cesium ({sup 137}Cs), americium ({sup 241}Am), plutonium ({sup 238}Pu and {sup 239,240}Pu), tritium ({sup 3}H), total uranium, and gross gamma activity. Area G sample results from both colonies were higher than the upper (95%) level background concentration for {sup 238}Pu and {sup 3}H.

  16. Transfer of aged Pu to cattle grazing on a contaminated environment.

    PubMed

    Gilbert, R O; Engel, D W; Smith, D D; Shinn, J H; Anspaugh, L R; Eisele, G R

    1988-03-01

    Estimates are obtained of the fraction of ingested or inhaled 239+240Pu transferred to blood and tissues of a reproducing herd of beef cattle, individuals of which grazed within fenced enclosures for up to 1064 d under natural conditions with no supplemental feeding at an arid site contaminated 16 y previously with Pu oxide. The estimated (geometric mean [GM]) fraction of Pu transferred from the gastrointestinal tract to blood serum was about 5 x 10(-6) (geometric standard error [GSE] = 1.4) with an approximate upper bound of about 2 x 10(-5). These results are in reasonable agreement with the value of 1 x 10(-5) recommended for human radiation protection purposes by the International Commission on Radiological Protection (ICRP) for insoluble Pu oxides that are free of very small particles. Also, results from a laboratory study by Stanley (St75), in which large doses of 238Pu were orally administered daily to dairy cattle for 19 consecutive days, suggest that aged 239+240Pu at this arid grazing site may not be more biologically available to blood serum than fresh 239+240Pu oxide. The estimated fractions of 239+240Pu transferred from blood serum to tissues of adult grazing cattle were: femur (3.2 X 10(-2), 1.8; GM, GSE), vertebra (1.4 X 10(-1), 1.6), liver (2.3 X 10(-1), 2.0), muscle (1.3 X 10(-1), 1.9), female gonads (7.9 X 10(-5), 1.5), and kidney (1.4 X 10(-3), 1.7). The blood-to-tissue fractional transfers for cattle initially exposed in utero were greater than those exposed only as adults by a factor of about 4 for femur (statistically significant) and of about 2 for other tissues (not significant). The estimated (GM) fraction of inhaled Pu initially deposited in the pulmonary lung was 0.34 (GSE = 1.3) for adults and 0.15 (GSE = 1.3) for cattle initially exposed in utero (a statistically significant difference), which may be compared with the expected fraction of 0.11 at the study site using the ICRP lung model for humans. PMID:3346164

  17. Plants as bio-monitors for Cs-137, Pu-238, Pu-239,240 and K-40 at the Savannah River Site.

    PubMed

    Caldwell, Eric Frank; Duff, Martine C; Ferguson, Caitlin E; Coughlin, Daniel P

    2011-05-01

    The Savannah River Site was constructed in South Carolina to produce plutonium (Pu) in the 1950s. Discharges associated with these now-ceased operations have contaminated large areas within the site, particularly streams associated with reactor cooling basins. Evaluating the exposure risk of contamination to an ecosystem requires methodologies that can assess the bioavailability of contaminants. Plants, as primary producers, represent an important mode of transfer of contaminants from soils and sediments into the food chain. The objective of this study was to identify local area plants for their ability to act as bio-monitors of radionuclides. The concentrations of cesium-137 ((137)Cs), potassium-40 ((40)K), (238)Pu and (239,240)Pu in plants and their associated soils were determined using γ and α spectrometry. The ratio of contamination concentration found in the plant relative to the soil was calculated to assess a concentration ratio (CR). The highest CR for (137)Cs was found in Pinus palustris needles (CR of 2.18). The correlation of soil and plant (137)Cs concentration was strong (0.76) and the R(2) (0.58) from the regression was significant (p = 0.006). This suggests the ability to predict the degree of (137)Cs contamination of a soil through analysis of the pine needles. The (238)Pu and (239,240)Pu concentrations were most elevated within the plant roots. Extremely high CR values were found in Sparganium americanum (bur-reed) roots with a value of 5.86 for (238)Pu and 5.66 for (239,240)Pu. The concentration of (40)K was measured as a known congener of (137)C. Comparing (40)K and (137)C concentrations in each plant revealed an inverse relationship for these radioisotopes. Correlating (40)K and (137)Cs was most effective in identifying plants that have a high affinity for (137)Cs uptake. The P. palustris and S. americanum proved to be particularly strong accumulators of all K congeners from the soil. Some species that were measured, warrant further

  18. Effect of carbonate soil on transport and dose estimates from long-lived radionuclides at U. S. Pacific Test Site

    SciTech Connect

    Conrado, C.L.; Hamilton, T.F.; Robison, W.L.; Stoker, A.C.

    1998-09-01

    The United States conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are Cesium-137 ({sup 137} Cs), Strontium-90 ({sup 90} Sr), Plutonium-239+ 240 ({sup 239+240}Pu) and Americium-241 ({sup 241}Am). {sup 137}Cs in the coral soils is more available for uptake by plants than {sup 137}Cs associated with continental soils of North America or Europe. Soil-to-plant {sup 137}Cs median concentration ratios (CR) (kBq kg{sup {minus}1} dry weight plant/kBq kg {sup {minus}1} dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, {sup 90}Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of {sup 137}Cs and {sup 90}Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for {sup 239+240}Pu and {sup 241}Am are very similar to those observed in continental soils. Values range from 10{sup {minus}6} to 10{sup {minus}4} for both {sup 239+240}Pu and {sup 241}Am. No significant difference is observed between the two in coral soil. The uptake of {sup 137}Cs by plants is enhanced because of the absence of mineral binding sites and the low concentration of potassium in the coral soil. {sup 137}Cs is bound to the organic fraction of the soil, whereas {sup 90}Sr, {sup 239+240}Pu and {sup 241}Am are primarily bound to soil particles. Assessment of plant uptake for {sup 137}Cs and {sup 90}Sr into locally grown food crops was a major contributing factor in (1) reliably predicting the radiological dose for returning residents, and (2) developing a strategy to limit the

  19. Alternating-parity collective states of yrast and nonyrast bands in lanthanide and actinide nuclei

    SciTech Connect

    Nadirbekov, M. S. Yuldasheva, G. A.; Denisov, V. Yu.

    2015-03-15

    Excited collective states of even-even nuclei featuring quadrupole and octupole deformations are studied within a nonadiabatic collective model with a Gaussian potential energy. Rotational states of the yrast band and vibrational-rotational states of nonyrast bands are considered in detail. The energies of alternating-parity excited states of the yrast band in the {sup 164}Er, {sup 220}Ra, and {sup 224}Th nuclei; the yrast and first nonyrast bands in the {sup 154}Sm and {sup 160}Gd nuclei; and the yrast, first nonyrast, and second nonyrast bands in the {sup 224}Ra and {sup 240}Pu nuclei are described well on the basis of the proposed model.

  20. [Plutonium at the ecosystems of impact zone the Beloyarsk NPP].

    PubMed

    Mikhaĭlovskaia, L N; Molchanova, I V; Karavaeva, E N

    2007-01-01

    The distribution of the plutonium at the ecosystems of impact zone the Beloyarsk NPP was studied. Higher quantity of Pu (to 500 Bq/m2) was revealed in the bottom sediments of the Olkhovsk bog where low-level radioactive water of the Beloyarsk NPP have been discharged. The total amount of the radionuclide in a soil cover did not exceed 140 Bq/m2. The contribution of the Beloyarsk NPP to contamination of the investigated ecosystems was accounted with using ratio 238Pu/239.240Pu. It was 64.1-99.3% both in the bottom sediments and soils. PMID:17953434

  1. Transfer of aged Pu to cattle grazing on a contaminated environment

    SciTech Connect

    Gilbert, R.O.; Engel, D.W.; Smith, D.D.; Shinn, J.H.; Anspaugh, L.R.; Eisele, G.R.

    1988-03-01

    Estimates are obtained of the fraction of ingested or inhaled 239+240Pu transferred to blood and tissues of a reproducing herd of beef cattle, individuals of which grazed within fenced enclosures for up to 1064 d under natural conditions with no supplemental feeding at an arid site contaminated 16 y previously with Pu oxide. The estimated (geometric mean (GM)) fraction of Pu transferred from the gastrointestinal tract to blood serum was about 5 x 10(-6) (geometric standard error (GSE) = 1.4) with an approximate upper bound of about 2 x 10(-5). These results are in reasonable agreement with the value of 1 x 10(-5) recommended for human radiation protection purposes by the International Commission on Radiological Protection (ICRP) for insoluble Pu oxides that are free of very small particles. Also, results from a laboratory study by Stanley (St75), in which large doses of /sup 238/Pu were orally administered daily to dairy cattle for 19 consecutive days, suggest that aged 239+240Pu at this arid grazing site may not be more biologically available to blood serum than fresh 239+240Pu oxide. The estimated fractions of 239+240Pu transferred from blood serum to tissues of adult grazing cattle were: femur (3.2 X 10(-2), 1.8; GM, GSE), vertebra (1.4 X 10(-1), 1.6), liver (2.3 X 10(-1), 2.0), muscle (1.3 X 10(-1), 1.9), female gonads (7.9 X 10(-5), 1.5), and kidney (1.4 X 10(-3), 1.7). The blood-to-tissue fractional transfers for cattle initially exposed in utero were greater than those exposed only as adults by a factor of about 4 for femur (statistically significant) and of about 2 for other tissues (not significant). The estimated (GM) fraction of inhaled Pu initially deposited in the pulmonary lung was 0.34 (GSE = 1.3) for adults and 0.15 (GSE = 1.3) for cattle initially exposed in utero (a statistically significant difference).

  2. [The distribution of the radionuclides in the main components of lake ecosystems within the Chernobyl NPP exclusion zone].

    PubMed

    2005-01-01

    The results of the studies devoted to the distribution of radionuclides 90Sr, 137Cs, 238Pu, 239 + 240Pu and 241Am in 1998-2003 in main components of Glubokoe Lake and Dalekoe-1 Lake located within Krasnensky flood lands of the Pripyat River (inner exclusion zone of the Chernobyl NPP) were analysed. The data about the radionuclide content in bottom sediments, in water, in seston, in macrozoobenthos (including bivalvia molluscs), in gasteropods molluscs, in higher aquatic plants and in fish are presented. PMID:16080615

  3. Accumulation of artificial radionuclides in agricultural plants in the area used for surface nuclear tests.

    PubMed

    Kozhakhanov, T E; Lukashenko, S N; Larionova, N V

    2014-11-01

    The paper reports on the study of artificial radionuclide accumulation in agricultural crops grown at the territory with high concentration of radionuclides, and first of all - with high concentration of transuranium elements. As a result of this work, peculiarities of accumulation and distribution of artificial radionuclides in the vegetative and generative organs of the studied plants have been revealed. Basic accumulation factors have been found for (137)Cs, (90)Sr, (239+240)Pu, and (241)Am in agricultural products. Accumulation factor dependence on type of planting was found for the investigated types of plants. It has been found that the vegetative organs accumulate radionuclides most of all. PMID:25128979

  4. Event-by-Event Fission Modeling of Prompt Neutrons and Photons from Neutron-Induced and Spontaneous Fission with FREYA

    NASA Astrophysics Data System (ADS)

    Vogt, Ramona; Randrup, Jorgen

    2013-04-01

    The event-by-event fission Monte Carlo code FREYA (Fission Reaction Event Yield Algorithm) generates large samples of complete fission events. Using FREYA, it is possible to obtain the fission products as well as the prompt neutrons and photons emitted during the fission process, all with complete kinematic information. We can therefore extract any desired correlation observables. Concentrating on ^239Pu(n,f), ^240Pu(sf) and ^252Cf(sf), we compare our FREYA results with available data on prompt neutron and photon emission and present predictions for novel fission observables that could be measured with modern detectors.

  5. Manifestation of cluster effects in the structure of actinides

    NASA Astrophysics Data System (ADS)

    Shneidman, T. M.; Adamian, G. G.; Antonenko, N. V.; Jolos, R. V.; Zhou, Shan-Gui

    2016-01-01

    We developed a cluster model which allows to take into account both shape deformation parameters and cluster degrees of freedom. The model is based on the assumption that the wave function of nucleus can be treated as a superposition of a mononucleus and two-cluster configurations. The model is applied to describe the multiple negative-parity bands in deformed actinides. Special emphasis is made on the investigation of the recently measured positive parity 0+2 rotational band of reflection-asymmetric nature in 240Pu. The results suggest that this band might be understood as the one built on the lowest excited state in mass asymmetry degree of freedom.

  6. Pu isotopes in the western North Pacific Ocean before the accident at Fukushima Dai-ichi Nuclear Power Station

    NASA Astrophysics Data System (ADS)

    Yamada, M.; Zheng, J.; Aono, T.

    2011-12-01

    Anthropogenic radionuclides such as Pu-239 (half-life: 24100 yr), Pu-240 (half-life: 6560 yr) and Pu-241 (half-life: 14.325 yr) mainly have been released into the environment as the result of atmospheric nuclear weapons testing. In the North Pacific Ocean, two distinct sources of Pu isotopes can be identified; i.e., the global stratospheric fallout and close-in tropospheric fallout from nuclear weapons testing at the Pacific Proving Grounds in the Marshall Islands. The atom ratio of Pu-240/Pu-239 is a powerful fingerprint to identify the sources of Pu in the ocean. The Pu-240/Pu-239 atom ratios in seawater and marine sediment samples collected in the western North Pacific before the accident at Fukushima Dai-ichi Nuclear Power Station will provide useful background data for understanding the process controlling Pu transport and for distinguishing future Pu sources. The atom ratios of Pu-240/Pu-239 in water columns from the Yamato and Tsushima Basins in the Japan Sea were significantly higher than the mean global fallout ratio of 0.18; however, there were no temporal variation of atom ratios during the period from 1984 to 1993 in the Japan Sea. The total Pu-239+240 inventories in the whole water columns were approximately doubled during the period from 1984 to 1993 in the two basins. The atom ratio of Pu-240/Pu-239 in surface water from Sagami Bay, western North Pacific Ocean, was 0.224 and showed no notable variation from the surface to the bottom with the mean atom ratio being 0.234. The atom ratios for the Pacific coast, near the Rokkasho nuclear fuel reprocessing plant, were approximately the same as the 0.224 ratio obtained from Sagami Bay, western North Pacific margin. The atom ratios in the surficial sediments from Sagami Bay ranged from 0.229 to 0.247. The mean atom ratio in the sediment columns in the East China Sea ranged from 0.248 for the Changjiang estuary to 0.268 for the shelf edge. The observed atom ratios were significantly higher than the mean

  7. [Migration in soil and accumulation in plants of peaceful nuclear explosion products in Perm region].

    PubMed

    Raskosha, N G; Shuktova, I I

    2015-01-01

    The data on the migration capacity in soil and accumulation of 238Pu, 239, 240Pu, 137Cs and 90Sr by plants in the area of a peaceful nuclear explosion located in the taiga zone are presented. The influence of the soil parameters on the distribution and transformation forms of the radionuclides in the podzolic soil profile was studied. The major amounts of man-made radionuclides were found in the matter of the ground lip. The accumulation parameters of pollutants by plants were the highest for the leaves, young branches and conifer of trees. PMID:25962279

  8. Superconducting calorimetric alpha particle sensors for nuclear nonproliferation applications

    SciTech Connect

    Horansky, Robert D.; Ullom, Joel N.; Beall, James A.; Hilton, Gene C.; Irwin, Kent D.; Dry, Donald E.; Hastings, Elizabeth P.; Lamont, Stephen P.; Rudy, Clifford R.; Rabin, Michael W.

    2008-09-22

    Identification of trace nuclear materials is usually accomplished by alpha spectrometry. Current detectors cannot distinguish critical elements and isotopes. We have developed a detector called a microcalorimeter, which achieves a resolution of 1.06 keV for 5.3 MeV alphas, the highest resolving power of any energy dispersive measurement. With this exquisite resolution, we can unambiguously identify the {sup 240}Pu/{sup 239}Pu ratio in Pu, a critical measurement for ascertaining the intended use of nuclear material. Furthermore, we have made a direct measurement of the {sup 209}Po ground state decay.

  9. Nuclear scission and quantum localization.

    PubMed

    Younes, W; Gogny, D

    2011-09-23

    We examine nuclear scission within a fully quantum-mechanical microscopic framework, focusing on the nonlocal aspects of the theory. Using (240)Pu hot fission as an example, we discuss the identification of the fragments and the calculation of their kinetic, excitation, and interaction energies, through the localization of the orbital wave functions. We show that the disentanglement of the fragment wave functions is essential to the quantum-mechanical definition of scission and the calculation of physical observables. Finally, we discuss the fragments' prescission excitation mechanisms and give a nonadiabatic description of their evolution beyond scission. PMID:22026846

  10. Spatial patterns and ratios of ¹³⁷Cs, ⁹⁰Sr, and Pu isotopes in the top layer of undisturbed meadow soils as indicators for contamination origin.

    PubMed

    Lukšienė, Benedikta; Puzas, Andrius; Remeikis, Vidmantas; Druteikienė, Rūta; Gudelis, Arūnas; Gvozdaitė, Rasa; Buivydas, Šarūnas; Davidonis, Rimantas; Kandrotas, Gintautas

    2015-05-01

    Spatial distribution of activity concentrations of (137)Cs, (90)Sr, and (239,240)Pu in the top layer of undisturbed meadow soils was compared between two regional transects across Lithuania: one in the SW region, more affected by the Chernobyl radioactive fallout, and the other in the NE region. Radiochemical, γ-, α-, β-, and mass spectrometric methods were used to determine the radionuclide activity. Our results validate that higher activity concentrations in the top soil layer were present in the SW region, despite the fact that sampling was performed after 22 years of the Chernobyl Nuclear Power Plant (NPP) accident. Using the activity concentration ratio (137)Cs/(239,240)Puglobal, the contribution of the Chernobyl NPP accident to the total radiocesium activity concentrations in these meadow soils was evaluated and found to be in the range of 6.5-59.1%. Meanwhile, the activity concentration ratio (238)Pu/(239,240)Pu showed that Chernobyl-derived Pu occurred at almost half of the sampling sites. The locations with maximal values of 47% of Chernobyl-derived Pu material were close to northeastern Poland, where deposition of most of non-volatile radioisotopes from the Chernobyl plume was determined. PMID:25893760

  11. Characterization and source term assessments of radioactive particles from Marshall Islands using non-destructive analytical techniques

    NASA Astrophysics Data System (ADS)

    Jernström, J.; Eriksson, M.; Simon, R.; Tamborini, G.; Bildstein, O.; Marquez, R. Carlos; Kehl, S. R.; Hamilton, T. F.; Ranebo, Y.; Betti, M.

    2006-08-01

    Six plutonium-containing particles stemming from Runit Island soil (Marshall Islands) were characterized by non-destructive analytical and microanalytical methods. Composition and elemental distribution in the particles were studied with synchrotron radiation based micro X-ray fluorescence spectrometry. Scanning electron microscope equipped with energy dispersive X-ray detector and with wavelength dispersive system as well as a secondary ion mass spectrometer were used to examine particle surfaces. Based on the elemental composition the particles were divided into two groups: particles with pure Pu matrix, and particles where the plutonium is included in Si/O-rich matrix being more heterogenously distributed. All of the particles were identified as nuclear fuel fragments of exploded weapon components. As containing plutonium with low 240Pu/ 239Pu atomic ratio, less than 0.065, which corresponds to weapons-grade plutonium or a detonation with low fission yield, the particles were identified to originate from the safety test and low-yield tests conducted in the history of Runit Island. The Si/O-rich particles contained traces of 137Cs ( 239 + 240 Pu/ 137Cs activity ratio higher than 2500), which indicated that a minor fission process occurred during the explosion. The average 241Am/ 239Pu atomic ratio in the six particles was 3.7 × 10 - 3 ± 0.2 × 10 - 3 (February 2006), which indicated that plutonium in the different particles had similar age.

  12. Plutonium concentrations in lichens of Rocky Flats environs

    SciTech Connect

    Thomas, R.S.; Ibrahim, S.A.

    1995-03-01

    Xanthoparmelia spp. lichens were used to study the spatial distribution of plutonium concentrations in nonvascular plants surrounding the Rocky Flats nuclear weapons facility with respect to distance, direction, age, and washing. Plutonium concentrations in lichens were inversely related to distance from the initial contamination site with a directional component which corroborated wind-borne transport as the primary means of dispersion. Ultrasonic washing and the relative age of the lichen proved to be significant only at p = 0.21 and p = 0.96, respectively. Isotopic ratios of {sup 239,240}Pu to {sup 238}Pu were highly variable at low activities but remained consistent at 62.6 for samples with high total plutonium activity. Correlation of Xanthoparmelia spp. lichen {sup 239,240}Pu concentrations to surface soil concentrations showed a direct relationship (r = 0.767; p < 0.001). The correlation was supported by soil retention studies which revealed a lichen soil content ranging from 11 to 18% on a dry mass basis with a possible particle size selectivity in the different concentration ratios adjacent to and away from the initial contamination site. Results suggest that further study into the in situ biomonitoring of surface soil by Xanthoparmelia spp. lichens is promising. 38 refs., 4 figs., 3 tabs.

  13. ANALYSIS AND EXAMINATION OF MOX FUEL FROM NONPROLIFERATION PROGRAMS

    SciTech Connect

    McCoy, Kevin; Machut, Dr McLean; Morris, Robert Noel; Blanpain, Patrick; Hemrick, James Gordon

    2013-01-01

    The U.S. Department of Energy has decided to dispose of a portion of the nation s surplus plutonium by reconstituting it into mixed oxide (MOX) fuel and irradiating it in commercial power reactors. Four lead assemblies were manufactured and irradiated to a maximum fuel rod burnup of 47.3 MWd/kg heavy metal. This was the first commercial irradiation of MOX fuel with a 240Pu/239Pu ratio of 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. The performance of the rods was analyzed with AREVA s next-generation GALILEO code. The results of the analysis confirmed that the fuel rods had performed safely and predictably, and that GALILEO is applicable to MOX fuel with a low 240Pu/239Pu ratio as well as to standard MOX. The results are presented and compared to the GALILEO database. In addition, the fuel cladding was tested to confirm that traces of gallium in the fuel pellets had not affected the mechanical properties of the cladding. The irradiated cladding was found to remain ductile at both room temperature and 350 C for both the axial and circumferential directions.

  14. Neutron coincidence imaging for active and passive neutron assays

    SciTech Connect

    Estep, R. J.; Brunson, G. S.; Melton, S. G.

    2001-01-01

    Neutron multiplicity assay algorithms for {sup 240}Pu assume a point source of fission neutrons that are detected in a single detector channel. The {sup 240}Pu in real waste, however, is more likely to be distributed throughout the container in some random way. For different reasons, this leads to significant errors when using either multiplicity or simpler coincidence analyses. Reduction of these errors can be achieved using tomographic imaging. In this talk we report on our results from using neutron singles and coincidence data between tagged detector pairs to provide enhanced tomographic imaging capabilities to a crate nondestructive assay system. Only simulated passive coincidence data is examined here, although the higher signal rates from active coincidence counting hold more promise for waste management. The active coincidence approach has significantly better sensitivity than the passive and is not significantly perturbed by (alpha,n) contributions. Our study was based primarily on simulated neutron pulse trains derived from the Los Alamos SIM3D software, which were subjected to analysis using the Los Alamos CTEN-FIT and TGS-FIT software. We found significantly improved imaging capability using the coincidence and singles rate data than could be obtained using the singles rate alone.

  15. Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations

    PubMed Central

    Schneider, Stephanie; Walther, Clemens; Bister, Stefan; Schauer, Viktoria; Christl, Marcus; Synal, Hans-Arno; Shozugawa, Katsumi; Steinhauser, Georg

    2013-01-01

    The contamination of Japan after the Fukushima accident has been investigated mainly for volatile fission products, but only sparsely for actinides such as plutonium. Only small releases of actinides were estimated in Fukushima. Plutonium is still omnipresent in the environment from previous atmospheric nuclear weapons tests. We investigated soil and plants sampled at different hot spots in Japan, searching for reactor-borne plutonium using its isotopic ratio 240Pu/239Pu. By using accelerator mass spectrometry, we clearly demonstrated the release of Pu from the Fukushima Daiichi power plant: While most samples contained only the radionuclide signature of fallout plutonium, there is at least one vegetation sample whose isotope ratio (0.381 ± 0.046) evidences that the Pu originates from a nuclear reactor (239+240Pu activity concentration 0.49 Bq/kg). Plutonium content and isotope ratios differ considerably even for very close sampling locations, e.g. the soil and the plants growing on it. This strong localization indicates a particulate Pu release, which is of high radiological risk if incorporated. PMID:24136192

  16. 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.

  17. Area 11 case study of radionuclide movement by storm channel erosion: A baseline method and initial evaluation

    SciTech Connect

    Shinn, J.H.; Gouveia, F.J.; Patton, S.E.; Fry, C.O.

    1993-04-01

    At the Nevada Test Site (NTS), where radionuclide contamination is found in surface soils, there is potential for water erosion to move radionuclides beyond the boundaries of controlled areas and into channels cut by infrequent storms. This loss of control and the increased risk of further movement are issues which require the development of a method for the quantitative monitoring of contamination and calculation of the radionuclide-movement rate. In this report the authors develop a method which is used to measure the amount and rate of movement of americium-241 ({sup 241}Am) in a storm channel, and which offers special features for establishment of baseline concentrations. This method was applied to the standing problem of the erosion of the plutonium contaminated {open_quotes}ground zero{close_quotes} area of site {open_quotes}11D{close_quotes} in Area 11 of NTS. By establishing {sup 241}Am concentrations in the storm channel, the concentrations of {sup 239+240}Pu can also be calculated using a previously determined {sup 239+240}Pu/{sup 241}Am ratio from soil samples collected in Area 11. The method utilizes systematic field surveys with a field instrument for detection of low-energy radiation (FIDLER), and provides a computational method which, when validated, could become a standard procedure for monitoring radionuclide movement in the washes and storm channels throughout the NTS.

  18. Plutonium concentrations in lichens of Rocky Flats environs.

    PubMed

    Thomas, R S; Ibrahim, S A

    1995-03-01

    Xanthoparmelia spp. lichens were used to study the spatial distribution of plutonium concentrations in nonvascular plants surrounding the Rocky Flats nuclear weapons facility with respect to distance, direction, age, and washing. Plutonium concentrations in lichens were inversely related to distance from the initial contamination site with a directional component which corroborated wind-borne transport as the primary means of dispersion. Ultrasonic washing and the relative age of the lichen proved to be significant only at p = 0.21 and p = 0.96, respectively. Isotopic ratios of 239,240Pu to 238Pu were highly variable at low activities but remained consistent at 62.6 for samples with high total plutonium activity. Correlation of Xanthoparmelia spp. lichen 239,240Pu concentrations to surface soil concentrations showed a direct relationship (r = 0.767; p < 0.001). The correlation was supported by soil retention studies which revealed a lichen soil content ranging from 11 to 18% on a dry mass basis with a possible particle size selectivity in the different concentration ratios adjacent to and away from the initial contamination site. Results suggest that further study into the in situ biomonitoring of surface soil by Xanthoparmelia spp. lichens is promising. PMID:7860301

  19. Main results of the 2012 joint Norwegian-Russian expedition to the dumping sites of the nuclear submarine K-27 and solid radioactive waste in Stepovogo Fjord, Novaya Zemlya.

    PubMed

    Gwynn, Justin P; Nikitin, Aleksander; Shershakov, Viacheslav; Heldal, Hilde Elise; Lind, Bjørn; Teien, Hans-Christian; Lind, Ole Christian; Sidhu, Rajdeep Singh; Bakke, Gunnar; Kazennov, Alexey; Grishin, Denis; Fedorova, Anastasia; Blinova, Oxana; Sværen, Ingrid; Lee Liebig, Penny; Salbu, Brit; Wendell, Cato Christian; Strålberg, Elisabeth; Valetova, Nailja; Petrenko, Galina; Katrich, Ivan; Logoyda, Igor; Osvath, Iolanda; Levy, Isabelle; Bartocci, Jean; Pham, Mai Khanh; Sam, Adam; Nies, Hartmut; Rudjord, Anne Liv

    2016-01-01

    This paper reports the main results of the 2012 joint Norwegian-Russian expedition to investigate the radioecological situation of the Stepovogo Fjord on the eastern coast of Novaya Zemlya, where the nuclear submarine K-27 and solid radioactive waste was dumped. Based on in situ gamma measurements and the analysis of seawater and sediment samples taken around the submarine, there was no indication of any leakage from the reactor units of K-27. With regard to the radioecological status of Stepovogo Fjord, activity concentrations of all radionuclides in seawater, sediment and biota in 2012 were in general lower than reported from the previous investigations in the 1990s. However in 2012, the activity concentrations of (137)Cs and, to a lesser extent, those of (90)Sr remained elevated in bottom water from the inner part of Stepovogo Fjord compared with surface water and the outer part of Stepovogo Fjord. Deviations from expected (238)Pu/(239,240)Pu activity ratios and (240)Pu/(239)Pu atom ratios in some sediment samples from the inner part of Stepovogo Fjord observed in this study and earlier studies may indicate the possibility of leakages from dumped waste from different nuclear sources. Although the current environmental levels of radionuclides in Stepovogo Fjord are not of immediate cause for concern, further monitoring of the situation is warranted. PMID:25716076

  20. Radionuclide bioconcentration factors and sediment partition coefficients in Arctic Seas subject to contamination from dumped nuclear wastes

    SciTech Connect

    Fisher, N.S. . Marine Sciences Research Center); Fowler, S.W.; Boisson, F.; Carroll, J. . Marine Environment Lab.); Rissanen, K. ); Salbu, B. . Lab. for Analytical Chemistry); Sazykina, T.G. ); Sjoeblom, K.L. )

    1999-06-15

    The disposal of large quantities of radioactive wastes in Arctic Seas by the former Soviet Union has prompted interest in the behavior of long-lived radionuclides in polar waters. Previous studies on the interactions of radionuclides prominent in radioactive wastes have focused on temperate waters; the extent to which the bioconcentration factors and sediment partitioning from these earlier studies could be applied to risk assessment analyses involving high latitude systems is unknown. Here the authors present concentrations in seawater and calculated in situ bioconcentration factors for [sup 90]Sr, [sup 137]Cs, and [sup 239+240]Pu (the three most important radionuclides in Arctic risk assessment models) in macroalgae, crustaceans, bivalve molluscs, sea birds, and marine mammals as well as sediment K[sub d] values for 13 radionuclides and other elements in samples taken from the Kara and Barents Seas. The data analysis shows that, typically, values for polar and temperate waters are comparable, but exceptions include 10-fold higher concentration factors for [sup 239+240]Pu in Arctic brown macroalgae, 10-fold lower K[sub d] values for [sup 90]Sr in Kara Sea sediment than in typical temperate coastal sediment, and 100-fold greater Ru K[sub d] values in Kara Sea sediment. For most elements application of temperate water bioconcentration factors and K[sub d] values to Arctic marine systems appears to be valid.

  1. MATERIAL PROPERTIES OF PLUTONIUM-BEARING OXIDES STORED IN STAINLESS STEEL CONTAINERS

    SciTech Connect

    Kessinger, G.; Almond, P.; Bridges, N.; Bronikowski, M.; Crowder, M.; Duffey, J.; Livingston, R.; Mcelwee, M.; Missimer, D.; Scogin, J.; Summer, M.; Jurgensen, A.

    2010-02-01

    The destructive examination (DE) of 3013 containers after storage is part of the Surveillance and Monitoring Program based on the Department of Energy's standard for long-term storage of Pu (DOE-STD-3013). The stored, Pu-bearing materials may contain alkali halide contamination that varies from trace amounts of salt to about 50 weight percent, with smaller fractions of other compounds and oxides. These materials were characterized prior to packaging, and surveillance characterizations are conducted to determine the behavior of the materials during long term storage. The surveillance characterization results are generally in agreement with the pre-surveillance data. The predominant phases identified by X-ray diffraction are in agreement with the expected phase assemblages of the as-received materials. The measured densities are in reasonable agreement with the expected densities of materials containing the fraction of salts and actinide oxide specified by the pre-surveillance data. The radiochemical results are generally in good agreement with the pre-surveillance data for mixtures containing 'weapons grade' Pu (nominally 94% {sup 239}Pu and 6% {sup 240}Pu); however, the ICP-MS results from the present investigation generally produce lower concentrations of Pu than the pre-surveillance analyses. For mixtures containing 'fuel grade' Pu (nominally 81-93% {sup 239}Pu and 7-19% {sup 240}Pu), the ICP-MS results from the present investigation appear to be in better agreement with the pre-surveillance data than the radiochemistry results.

  2. Trench ‘Bathtubbing’ and Surface Plutonium Contamination at a Legacy Radioactive Waste Site

    PubMed Central

    2013-01-01

    Radioactive waste containing a few grams of plutonium (Pu) was disposed between 1960 and 1968 in trenches at the Little Forest Burial Ground (LFBG), near Sydney, Australia. A water sampling point installed in a former trench has enabled the radionuclide content of trench water and the response of the water level to rainfall to be studied. The trench water contains readily measurable Pu activity (∼12 Bq/L of 239+240Pu in 0.45 μm-filtered water), and there is an associated contamination of Pu in surface soils. The highest 239+240Pu soil activity was 829 Bq/kg in a shallow sample (0–1 cm depth) near the trench sampling point. Away from the trenches, the elevated concentrations of Pu in surface soils extend for tens of meters down-slope. The broader contamination may be partly attributable to dispersion events in the first decade after disposal, after which a layer of soil was added above the trenched area. Since this time, further Pu contamination has occurred near the trench-sampler within this added layer. The water level in the trench-sampler responds quickly to rainfall and intermittently reaches the surface, hence the Pu dispersion is attributed to saturation and overflow of the trenches during extreme rainfall events, referred to as the ‘bathtub’ effect. PMID:24256473

  3. Actinide measurements by AMS using fluoride matrices

    NASA Astrophysics Data System (ADS)

    Cornett, R. J.; Kazi, Z. H.; Zhao, X.-L.; Chartrand, M. G.; Charles, R. J.; Kieser, W. E.

    2015-10-01

    Actinides can be measured by alpha spectroscopy (AS), mass spectroscopy or accelerator mass spectrometry (AMS). We tested a simple method to separate Pu and Am isotopes from the sample matrix using a single extraction chromatography column. The actinides in the column eluent were then measured by AS or AMS using a fluoride target matrix. Pu and Am were coprecipitated with NdF3. The strongest AMS beams of Pu and Am were produced when there was a large excess of fluoride donor atoms in the target and the NdF3 precipitates were diluted about 6-8 fold with PbF2. The measured concentrations of 239,240Pu and 241Am agreed with the concentrations in standards of known activity and with two IAEA certified reference materials. Measurements of 239,240Pu and 241Am made at A.E. Lalonde AMS Laboratory agree, within their statistical uncertainty, with independent measurements made using the IsoTrace AMS system. This work demonstrated that fluoride targets can produce reliable beams of actinide anions and that the measurement of actinides using fluorides agree with published values in certified reference materials.

  4. Radiological situation in the vicinity of Semipalatinsk nuclear test site: Dolon, Mostik, Cheremushka and Budene settlements.

    PubMed

    Sakaguchi, Aya; Yamamoto, Masayoshi; Hoshi, Masaharu; Imanaka, Tetsuji; Apsalikov, Kazbek N; Gusev, Boris I

    2006-02-01

    The present situation of radioactive contamination at the village of Dolon and nearby villages such as Mostik, Cheremushka and Budene was investigated to serve as an aid to resolve dose discrepancy between model calculations and TL measurements made for external gamma-ray dose in air in Dolon. The paper was focused on the reevaluation of the accumulated levels and distribution of long-lived radionuclides 137Cs and Pu isotopes in soil using long core samples up to a depth of 30 and 100 cm. The inventories of 137Cs and 239,240Pu found were in the wide range of 140-10,310 and 140-14,320 Bq/m2, respectively. Most of the Pu in soil was tightly incorporated into various sizes of fused particles. Both 137Cs and 239,240Pu in soil were accumulated in the smaller soil size fraction of <125 microm, and the presence of hot particles, probably due to Pu, was clearly observed by star-like patterns from alpha-tracks. The obtained data will be helpful for evaluating the current and future radiation risks to the people living around there. PMID:16571924

  5. Plutonium, 241Am and 137Cs ratios, inventories and vertical profiles in Washington and Oregon continental shelf sediments

    NASA Astrophysics Data System (ADS)

    Beasley, T. M.; Carpenter, R.; Jennings, C. D.

    1982-10-01

    Continental shelf sediments from nine locations off Washington and Oregon have 239,240Pu inventories which average 8.0 ± 2.6 mCi/km 2. The Columbia River and seawaters advecting over the shelf supply Pu which is removed to underlying sediments, principally through scavenging by inorganic paniculate matter. Mass balance calculations argue that less than 20 percent of the advected Pu need be scavenged from the water column to balance river input and total shelf sediment inventories. The percentage of the Pu removed through scavenging is consistent with observed participate concentrations in shelf waters and published sediment/water distribution coefficients. No marked separation of Pu from 137Cs is observed with depth in Pacific shelf sediments as has been reported in Atlantic coastal sediments. This interocean distinctness can be explained by differences in particle mixing and downward diffusion of Cs in sediments of varying porosities. The transuranic inventories and Pu/Cs ratios in the Pacific sediments do not support the hypothesis of Livingston and Bowen that Pu is remobilized within the sediment column by 'complexone' formation with (principally) organic substances. Excess 210Pb/ 239,240Pu inventory ratios in eight representative cores from the Washington shelf average 100 ± 19, even though absolute values of both inventories vary by much larger factors. This reasonably constant ratio, for a given water depth, permits estimation of total Pu inventories and prediction of sites of unusual Pu accumulation from data on the more easily measured natural radionuclide.

  6. Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations

    NASA Astrophysics Data System (ADS)

    Schneider, Stephanie; Walther, Clemens; Bister, Stefan; Schauer, Viktoria; Christl, Marcus; Synal, Hans-Arno; Shozugawa, Katsumi; Steinhauser, Georg

    2013-10-01

    The contamination of Japan after the Fukushima accident has been investigated mainly for volatile fission products, but only sparsely for actinides such as plutonium. Only small releases of actinides were estimated in Fukushima. Plutonium is still omnipresent in the environment from previous atmospheric nuclear weapons tests. We investigated soil and plants sampled at different hot spots in Japan, searching for reactor-borne plutonium using its isotopic ratio 240Pu/239Pu. By using accelerator mass spectrometry, we clearly demonstrated the release of Pu from the Fukushima Daiichi power plant: While most samples contained only the radionuclide signature of fallout plutonium, there is at least one vegetation sample whose isotope ratio (0.381 +/- 0.046) evidences that the Pu originates from a nuclear reactor (239+240Pu activity concentration 0.49 Bq/kg). Plutonium content and isotope ratios differ considerably even for very close sampling locations, e.g. the soil and the plants growing on it. This strong localization indicates a particulate Pu release, which is of high radiological risk if incorporated.

  7. Radionuclide Concentration in Soils and Vegetation at Low-Level Radioactive Waste Disposal Area G during 2005

    SciTech Connect

    P.R. Fresquez; M.W. McNaughton; M.J. Winch

    2005-10-01

    Soil samples were collected at 15 locations and unwashed overstory and understory vegetation samples were collected from up to nine locations within and around the perimeter of Area G, the primary disposal facility for low-level radioactive solid waste at Los Alamos National Laboratory (LANL). Soil and plant samples were also collected from the proposed expansion area west of Area G for the purpose of gaining preoperational baseline data. Soil and plant samples were analyzed for radionuclides that have shown a history of detection in past years; these included {sup 3}H, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 234}U, {sup 235}U, and {sup 238}U for soils and {sup 3}H, {sup 238}Pu, and {sup 239,240}Pu for plants. As in previous years, the highest levels of {sup 3}H in soils and vegetation were detected at the south portion of Area G near the {sup 3}H shafts; whereas, the highest concentrations of the Pu isotopes were detected in the northern and northeastern portions near the pads for transuranic waste. All concentrations of radionuclides in soils and vegetation, however, were still very low (pCi range) and far below LANL screening levels and regulatory standards.

  8. Burnup estimation of fuel sourcing radioactive material based on monitored Cs and Pu isotopic activity ratios in Fukushima N. P. S. accident

    SciTech Connect

    Yamamoto, T.; Suzuki, M.; Ando, Y.

    2012-07-01

    After the severe core damage of Fukushima Dai-Ichi Nuclear Power Station, radioactive material leaked from the reactor buildings. As part of monitoring of radioactivity in the site, measurements of radioactivity in soils at three fixed points have been performed for {sup 134}Cs and {sup 137}Cs with gamma-ray spectrometry and for Pu, Pu, and {sup 240}Pu with {alpha}-ray spectrometry. Correlations of radioactivity ratios of {sup 134}Cs to {sup 137}Cs, and {sup 238}Pu to the sum of {sup 239}Pu and {sup 240}Pu with fuel burnup were studied by using theoretical burnup calculations and measurements on isotopic inventories, and compared with the Cs and Pu radioactivity rations in the soils. The comparison indicated that the burnup of the fuel sourcing the radioactivity was from 18 to 38 GWd/t, which corresponded to that of the fuel in the highest power and, therefore, the highest decay heat in operating high-burnup fueled BWR cores. (authors)

  9. Radioactivity In Marine Organisms From Northeast Atlantic Ocean

    SciTech Connect

    Carvalho, Fernando P.; Oliveira, Joao M.

    2008-08-07

    Naturally-occurring radionuclides such as {sup 238}U, {sup 234}U, {sup 230}Th, {sup 226}Ra, {sup 210}Po, {sup 210}Pb and {sup 232}Th, and artificial radionuclides such as {sup 137}Cs, {sup 239+240}Pu and {sup 241}Am, were measured in a large number of marine species. In common fish species, typical concentrations of {sup 210}Po ranged from 10{sup 2} to 10{sup 4} mBq kg{sup -1} (wet weight), {sup 226}Ra concentrations ranged from 1x10{sup 2} to 5xl0{sup 2} mBq kg{sup -1}, {sup 238}U was at about 10 mBq kg{sup -1} and {sup 232}Th at about 0.5 mBq kg{sup -1}. Radiation doses to marine organisms originated by naturally-occurring and artificial radionuclides accumulated in tissues and by external radiation sources were computed and compared. Internal sources generally give higher contribution to the absorbed radiation dose than external sources. Amongst radionuclides accumulated in fish muscle and acting as internal radiation sources, natural {sup 210}Po and {sup 40}K give the largest contribution to the absorbed radiation dose, while artificial radionuclides such as {sup 137}Cs and {sup 239+240}Pu contribute with less than 0.5% to the absorbed radiation dose from all internal sources.

  10. Energy Dependent Bias in the Weighted Point Model.

    SciTech Connect

    Santi, P. A.; Geist, W. H.

    2005-01-01

    While the weighted point multiplicity model has successfully reduced the bias that is associated with variable multiplication of neutrons within a sample (which was assumed constant in the standard point multiplicity model), other potential sources of bias still exists within the weighted point model. One significant source of bias arises from the assumption that the energies of the neutrons from ({alpha},n) reactions on impurities in the sample have the same average energy as neutrons emitted from the spontaneous fission of {sup 240}Pu. An investigation into the effects that neutron energy has on the assay results (effective {sup 240}Pu mass, alpha, and multiplication) of the weighted point multiplicity model has been performed using MCNPX, Version 2.5f for impure plutonium metal samples in a number of different detector systems. The effects of energy dependence of the detection efficiency and gate fractions on the assay results, as well as the measured singles, doubles, and triples rates were also studied. Methods for mitigating the effects of neutron energy on the weighted-point multiplicity model results will be presented and discussed.

  11. A practical strategy for reducing the future security risk of United States spent nuclear fuel

    SciTech Connect

    Chodak, P. III; Buksa, J.J.

    1997-06-01

    Depletion calculations show that advanced oxide (AOX) fuels can be used in existing light water reactors (LWRs) to achieve and maintain virtually any desired level of US (US) reactor-grade plutonium (R-Pu) inventory. AOX fuels are composed of a neutronically inert matrix loaded with R-Pu and erbium. A 1/2 core load of 100% nonfertile, 7w% R-Pu AOX and 3.9 w% UO{sub 2} has a net total plutonium ({sup TOT}Pu) destruction rate of 310 kg/yr. The 20% residual {sup TOT}Pu in discharged AOX contains > 55% {sup 242}Pu making it unattractive for nuclear explosive use. A three-phase fuel-cycle development program sequentially loading 60 LWRs with 100% mixed oxide, 50% AOX with a nonfertile component displacing only some of the {sup 238}U, and 50% AOX, which is 100% nonfertile, could reduce the US plutonium inventory to near zero by 2050.

  12. Actinide targets for the synthesis of super-heavy elements

    NASA Astrophysics Data System (ADS)

    Roberto, J. B.; Alexander, C. W.; Boll, R. A.; Burns, J. D.; Ezold, J. G.; Felker, L. K.; Hogle, S. L.; Rykaczewski, K. P.

    2015-12-01

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing the production of rare actinides including 249Bk, 251Cf, and 254Es are described.

  13. The production and certification of a plutonium equal-atom reference material: NBL CRM 128

    SciTech Connect

    Crawford, D.W. . Office of Safeguards and Security); Gradle, C.G.; Soriano, M.D. )

    1990-07-01

    This report describes the design, production, and certification of the New Brunswick Laboratory plutonium equal-atom certified reference material (CRM), NBL CRM 128. The primary use of this CRM is for the determination of bias corrections encountered in the operation of a mass spectrometer. This reference material is available to the US Department of Energy contractor-operated and government-operated laboratories, as well as to the international nuclear safeguards community. The absolute, or unbiased, certified value for the CRM's Pu-242/Pu-239 ratio is 1.00063 {plus minus} 0.00026 (95% confidence interval) as of October 1, 1984. This value was obtained through the quantitative blending of high-purity, chemically and isotopically characterized separated isotopes, as well as through intercomparisons of CRM samples with calibration mixtures using thermal ionization mass spectrometry. 32 tabs.

  14. Fission cross section measurements of actinides at LANSCE

    SciTech Connect

    Tovesson, Fredrik; Laptev, Alexander B; Hill, Tony S

    2010-01-01

    Fission cross sections of a range of actinides have been measured at the Los Alamos Neutron Science Center (LANSCE) in support of nuclear energy applications. By combining measurement at two LANSCE facilities, Lujan Center and the Weapons Neutron Research center (WNR), differential cross sections can be measured from sub-thermal energies up to 200 MeV. Incident neutron energies are determined using the time-of-flight method, and parallel-plate ionization chambers are used to measure fission cross sections relative to the {sup 235}U standard. Recent measurements include the {sup 233,238}U, {sup 239,242}Pu and {sup 243}Am neutron-induced fission cross sections. In this paper preliminary results for cross section data of {sup 243}Am and {sup 233}U will be presented.

  15. In-beam separation and mass determination of superheavy nuclei. Part II

    NASA Astrophysics Data System (ADS)

    Malyshev, O. N.; Yeremin, A. V.; Popeko, A. G.; Belozerov, A. V.; Chelnokov, M. L.; Chepigin, V. I.; Gorshkov, V. A.; Hofmann, S.; Itkis, M. G.; Kabachenko, A. P.; Oganessian, Yu. Ts.; Sagaidak, R. N.; Šáro, Š.; Shutov, A. V.; Svirikhin, A. I.

    2004-01-01

    Within the past 15 years, the recoil separator VASSILISSA has been used for the investigations of evaporation residues produced in complete fusion reactions induced by heavy ions. The study of decay properties and formation of cross-sections of the isotopes of elements 110, 112 and 114 was performed using high-intensity 48Ca beams and 232Th, 238U, 242Pu targets. For further experiments aimed at the synthesis of the superheavy element isotopes ( Z⩾110) with the use of intense 48Ca extracted beams, improvements in the ion optical system of the separator and the focal plane detector system have been made. The results from the test reactions and new results for the isotope 283112 are presented.

  16. The Reaction Mechanism in Heavy-Ion Collisions Leading to the Superheavy Compound Systems

    NASA Astrophysics Data System (ADS)

    Itkis, M. G.; Beghini, S.; Behera, B. R.; Bogatchev, A. A.; Corradi, L.; Dorvaux, O.; Fioretto, E.; Gadea, A.; Hanappe, F.; Itkis, I. M.; Kliman, J.; Knyazheva, G. N.; Kondratiev, N. A.; Kozulin, E. M.; Krupa, L.; Latina, A.; Montagnoli, G.; Oganessian, Yu. Ts.; Pokrovsky, I. V.; Prokhorova, E. V.; Rowley, N.; Rubchenya, V. A.; Rusanov, A. Ya.; Sagaidak, R. N.; Scarlassara, F.; Stefanini, A. M.; Stuttge, L.; Szilner, S.; Trotta, M.; Trzaska, W. H.

    2008-08-01

    Results of the experiments aimed at the study of fission and quasi-fission processes in the reactions 36S+238U, 48Ca+144,154Sm, 168Er, 208Pb, 238U, 244Pu, 248Cm; 50Ti+208Pb, 244Pu;58Fe+208Pb, 244Pu, 248Cm, and 64Ni+186W, 242Pu leading to the formation of heavy and super-heavy systems with Z=82-122 are presented. Cross sections, mass-energy and angular distributions for fission and quasifission fragments have been studied at energies close and below the Coulomb barrier. The influence of the reaction entrance channel properties as mass asymmetry, deformations and neutron excess, shell effects in the interacting nuclei and producing compound nucleus the mechanism of the fusion-fission and the competitive process of quasi-fission are discussed.

  17. The Processes of Fusion-Fission and Quasi-Fission of Superheavy Nuclei

    NASA Astrophysics Data System (ADS)

    Itkis, M. G.; Bogachev, A. A.; Itkis, I. M.; Kliman, J.; Knyazheva, G. N.; Kondratiev, N. A.; Kozulin, E. M.; Krupa, L.; Oganessian, Yu. Ts.; Pokrovsky, I. V.; Prokhorova, E. V.; Rusanov, A. Ya.; Sagaidak, R. N.; Behera, B. R.; Corradi, L.; Fioretto, E.; Gadea, A.; Latina, A.; Stefanini, A. M.; Szilner, S.; Beghini, S.; Montagnoli, G.; Scarlassara, F.; Trotta, M.; Bouchat, V.; Hanappe, F.; Materna, T.; Dorvaux, O.; Rowley, N.; Schmitt, C.; Stuttge, L.

    2008-11-01

    Results of the experiments aimed at the study of fission and quasi-fission processes in the reactions 48Ca + 144,154Sm, 168Er, 208Pb, 238U, 244Pu, 248Cm; 50Ti + 208Pb, 244Pu; 58Fe + 208Pb, 244Pu, 248Cm, and 64Ni + 186W, 242Pu leading to the formation of heavy and super-heavy systems with Z = 82-122 are presented. Cross sections, mass-energy and angular distributions for fission and quasi-fission fragments have been studied at energies close and below the Coulomb barrier. The influence of the reaction entrance channel properties such as mass asymmetry, deformations, neutron excess, shell effects in the interacting nuclei and producing compound nucleus, the mechanism of the fusion-fission and the competitive process of quasi-fission are discussed.

  18. Connecting the Super-Heavy Island to the Nuclear Mainland

    NASA Astrophysics Data System (ADS)

    Rykaczewski, K.; Miernik, K.; Grzywacz, R.; Miller, D.

    2011-10-01

    The reactions between radioactive actinide targets and doubly-magic 48Ca beam led the identification of 6 new super-heavy elements (SHE) and 48 nuclei. Since the observed decay chains are ended by a fission process, these super-heavy nuclei are forming an isolated island in the nuclear chart. The HRIBF development of new detector system and digital data acquisition sensitive to very short-lived α-emitters made possible to attempt the studies extending the SHE island. The experiments aiming in new nuclei produced in the reactions with 248Cm and 239,242Pu targets and 40 , 44 , 48Ca projectiles and connecting the SHE island to the known nuclear mainland will be discussed. Research sponsored by the Office of Nuclear Physics, U.S. Department of Energy.

  19. Actinide targets for the synthesis of super-heavy elements

    DOE PAGESBeta

    Roberto, J.; Alexander, Charles W.; Boll, Rose Ann; Ezold, Julie G.; Felker, Leslie Kevin; Rykaczewski, Krzysztof Piotr; Hogle, Susan L.

    2015-06-18

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing themore » production of rare actinides including 249Bk, 251Cf, and 254Es are described.« less

  20. Fission cross-sections, prompt fission neutron and γ-ray emission in request for nuclear applications

    NASA Astrophysics Data System (ADS)

    Hambsch, F.-J.; Salvador-Castiñeira, P.; Oberstedt, S.; Göök, A.; Billnert, R.

    2016-06-01

    In recent years JRC-IRMM has been investigating fission cross-sections of 240,242Pu in the fast-neutron energy range relevant for innovative reactor systems and requested in the High Priority Request List (HPRL) of the OECD/Nuclear Energy Agency (NEA). In addition to that, prompt neutron multiplicities are being investigated for the major isotopes 235U, 239Pu in the neutron-resonance region using a newly developed scintillation detector array (SCINTIA) and an innovative modification of the Frisch-grid ionisation chamber for fission-fragment detection. These data are highly relevant for improved neutron data evaluation and requested by the OECD/Working Party on Evaluation Cooperation (WPEC). Thirdly, also prompt fission γ-ray emission is investigated using highly efficient lanthanide-halide detectors with superior timing resolution. Again, those data are requested in the HPRL for major actinides to solve open questions on an under-prediction of decay heat in nuclear reactors. The information on prompt fission neutron and γ-ray emission is crucial for benchmarking nuclear models to study the de-excitation process of neutron-rich fission fragments. Information on γ-ray emission probabilities is also useful in decommissioning exercises on damaged nuclear power plants like Fukushima Daiichi to which JRC-IRMM is contributing. The results on the 240,242Pu fission cross section, 235U prompt neutron multiplicity in the resonance region and correlations with fission fragments and prompt γ-ray emission for several isotopes will be presented and put into perspective.

  1. A compact gas-filled avalanche counter for DANCE

    DOE PAGESBeta

    Wu, C. Y.; Chyzh, A.; Kwan, E.; Henderson, R. A.; Gostic, J. M.; Carter, D.; Bredeweg, T. A.; Couture, A.; Jandel, M.; Ullmann, J. L.

    2012-08-04

    A compact gas-filled avalanche counter for the detection of fission fragments was developed for a highly segmented 4π γ-ray calorimeter, namely the Detector for Advanced Neutron Capture Experiments located at the Lujan Center of the Los Alamos Neutron Science Center. It has been used successfully for experiments with 235U, 238Pu,239Pu, and 241Pu isotopes to provide a unique signature to differentiate the fission from the competing neutron-capture reaction channel. We also used it to study the spontaneous fission in 252Cf. The design and performance of this avalanche counter for targets with extreme α-decay rate up to ~2.4×108/s are described.

  2. Nuclear Data Sheets for A=241

    DOE PAGESBeta

    Nesaraja, Caroline D.

    2015-11-27

    This paper presents available information pertaining to the nuclear structure of ground and excited states for all known nuclei with mass numbers A=24, which have been compiled and evaluated. The adopted level and decay schemes, as well as the detailed nuclear properties and configuration assignments based on experimental data are presented for these nuclides. When there are insufficient data, expected values from systematics of nuclear properties or/and theoretical calculations are quoted. Unexpected or discrepant experimental results are also noted. A summary and compilation of the discovery of various isotopes in this mass region is given in 2013Fr02 (241Np,241Pu, 241Am, 241Cm,more » 241Bk, and 241Cf), 2011Me01 (241Es), and 2013Th02 (241Fm).« less

  3. Precision spectroscopy with reactor antineutrinos

    NASA Astrophysics Data System (ADS)

    Huber, Patrick; Schwetz, Thomas

    2004-09-01

    In this work we present an accurate parameterization of the antineutrino flux produced by the isotopes 235U, 239Pu, and 241Pu in nuclear reactors. We determine the coefficients of this parameterization, as well as their covariance matrix, by performing a fit to spectra inferred from experimentally measured beta spectra. Subsequently we show that flux shape uncertainties play only a minor role in the KamLAND experiment, however, we find that future reactor-neutrino experiments to measure the mixing angle θ13 are sensitive to the fine details of the reactor-neutrino spectra. Finally, we investigate the possibility to determine the isotopic composition in nuclear reactors through an antineutrino measurement. We find that with a three month exposure of a 1ton detector the isotope fractions and the thermal reactor power can be determined at a few percent accuracy, which may open the possibility of an application for safeguard or nonproliferation objectives.

  4. Effect of the electron decay of metallic fission products on the chemical and phase compositions of an uranium-plutonium fuel irradiated by fast neutrons

    NASA Astrophysics Data System (ADS)

    Bondarenko, G. G.; Bulatov, G. S.; Gedgovd, K. N.; Lyubimov, D. Yu.; Yakushkin, M. M.

    2011-11-01

    After fast-neutron irradiation, uranium-plutonium nitride U0.8Pu0.2N is shown to acquire a complex structure consisting of a solid solution that is based on the nitrides of uranium, plutonium, americium, neptunium, zirconium, yttrium, and lanthanides and contains condensed phases U2N3, CeRu2, BaTe, Ba3N2, CsI, Sr3N2, LaSe, metallic molybdenum, technetium, and U(Ru, Rh, Pd)3 intermetallics. The contents and compositions of these phases are calculated at a temperature of 900 K and a burn-up fraction up to 14% (U + Pu). The change in the composition of the irradiated uranium-plutonium nitride is studied during the electron decay of metallic radionuclides. The kinetics of transformation of U103Ru3, 137CsI, 140Ba3N2, and 241PuN is calculated.

  5. National Low-Level Waste Management Program Radionuclide Report Series

    SciTech Connect

    J.P. Adams; M.L. Carboneau; W.E. Allred

    1999-02-01

    The National Low Level Waste Management Program at the Idaho National Engineering and Environmental Laboratory has published a report containing key information about selected radionuclides that are most likely to contribute significantly to the radiation exposures estimated from a performance assessment of a low-level radioactive waste (LLW) disposal facility. The information includes physical and chemical characteristics, production means, waste forms, behavior of the radionuclide in soils, plants, groundwater, and air, and biological effects in animals and humans. The radionuclides included in this study comprise all of the nuclides specifically listed in 10CFR61.55, Tables 1 and 2, 3 H, 14 C, 59 Ni, 60 Co, 63 Ni, 90 Sr, 94 Nb, 99 Tc, 129 I, 137 Cs, 241 Pu, and 242 Cm. Other key radionuclides addressed in the report include 237 Np, 238 U, 239 Pu, and 241 Am. This paper summarizes key information contained within this report.

  6. National Low-Level Waste Management Program Radionuclide Report Series

    SciTech Connect

    Adams, James Paul; Carboneau, Michael Leonard; Allred, William Edgar

    1999-03-01

    The National Low Level Waste Management Program at the Idaho National Engineering and Environmental Laboratory has published a report containing key information about selected radionuclides that are most likely to contribute significantly to the radiation exposures estimated from a performance assessment of a low-level radioactive waste (LLW) disposal facility. The information includes physical and chemical characteristics, production means, waste forms, behavior of the radionuclide in soils, plants, groundwater, and air, and biological effects in animals and humans. The radionuclides included in this study comprise all of the nuclides specifically listed in 10CFR61.55, Tables 1 and 2, 3 H, 14 C, 59 Ni, 60 Co, 63 Ni, 90 Sr, 94 Nb, 99 Tc, 129 I, 137 Cs, 241 Pu, and 242 Cm. Other key radionuclides addressed in the report include 237 Np, 238 U, 239 Pu, and 241 Am. This paper summarizes key information contained within this report.

  7. Americium

    NASA Astrophysics Data System (ADS)

    Runde, Wolfgang H.; Schulz, Wallace W.

    Americium, element 95, was discovered in 1944-45 by Seaborg et al. (1950) at the Metallurgical Laboratory of the University of Chicago as a product of the irradiation of plutonium with neutrons: 239{Pu}( n,γ )^{240} Put( n,γ )^{241} Pu → - β ^-}^{241}{Am} This reaction is still the best method for the production of pure 241Am. In post-World War II work at the University of Chicago, Cunningham isolated Am(OH)3 and measured the first absorption spectrum of the Am3+ aquo ion (Cunningham, 1948). By the 1950s, the major center for americium chemistry research in the world was at Los Alamos. Since the 1970s, the majority of publications on americium have come from researchers in the former USSR and West Germany. Extensive reviews of americium chemistry can be found in Freeman and Keller (1985), Gmelin (1979), Penneman and Asprey (1955), and Schulz (1976).

  8. Monte Carlo simulations of differential die-away instrument for determination of fissile content in spent fuel assemblies

    NASA Astrophysics Data System (ADS)

    Lee, Tae-Hoon; Menlove, Howard O.; Swinhoe, Martyn T.; Tobin, Stephen J.

    2011-10-01

    The differential die-away (DDA) technique has been simulated by using the MCNPX code to quantify its capability of measuring the fissile content in spent fuel assemblies. For 64 different spent fuel cases of various initial enrichment, burnup and cooling time, the count rate and signal to background ratios of the DDA system were obtained, where neutron backgrounds are mainly coming from the 244Cm of the spent fuel. To quantify the total fissile mass of spent fuel, a concept of the effective 239Pu mass was introduced by weighing the relative contribution to the signal of 235U and 241Pu compared to 239Pu and the calibration curves of DDA count rate vs. 239Pu eff were obtained by using the MCNPX code. With a deuterium-tritium (DT) neutron generator of 10 9 n/s strength, signal to background ratios of sufficient magnitude are acquired for a DDA system with the spent fuel assembly in water.

  9. Application of Neutron-Absorbing Structural-Amorphous Metal (SAM) Coatings for Spent Nuclear Fuel (SNF) Container to Enhance Criticality Safety Controls

    SciTech Connect

    Choi, Jor-Shan; Lee, Chuck; Farmer, Joseph; Day, Dan; Wall, Mark; Saw, Cheng; Boussoufi, Moe; Liu, Ben; Egbert, Harold; Branagan, Dan; D'Amato, Andy

    2007-07-01

    Spent nuclear fuel contains fissionable materials ({sup 235}U, {sup 239}Pu, {sup 241}Pu, etc.). To prevent nuclear criticality in spent fuel storage, transportation, and during disposal, neutron-absorbing materials (or neutron poisons, such as borated stainless steel, Boral{sup TM}, Metamic{sup TM}, Ni-Gd, and others) would have to be applied. The success in demonstrating that the High-Performance Corrosion- Resistant Material (HPCRM){sup [1]} can be thermally applied as coating onto base metal to provide for corrosion resistance for many naval applications raises the interest in applying the HPCRM to USDOE/OCRWM spent fuel management program. The fact that the HPCRM relies on the high content of boron to make the material amorphous - an essential property for corrosion resistance - and that the boron has to be homogeneously distributed in the HPCRM qualify the material to be a neutron poison. (authors)

  10. Analysis of spent fuel assay with a lead slowing down spectrometer

    SciTech Connect

    Gavron, Victor I; Smith, L Eric; Ressler, Jennifer J

    2008-01-01

    Assay of fissile materials in spent fuel that are produced or depleted during the operation of a reactor, is of paramount importance to nuclear materials accounting, verification of the reactor operation history, as well as for criticality considerations for storage. In order to prevent future proliferation following the spread of nuclear energy, we must develop accurate methods to assay large quantities of nuclear fuels. We analyze the potential of using a Lead Slowing Down Spectrometer for assaying spent fuel. We conclude that it is possible to design a system that will provide around 1% statistical precision in the determination of the {sup 239}Pu, {sup 241}Pu and {sup 235}U concentrations in a PWR spent-fuel assembly, for intermediate-to-high burnup levels, using commercial neutron sources, and a system of {sup 238}U threshold fission detectors. Pending further analysis of systematic errors, it is possible that missing pins can be detected, as can asymmetry in the fuel bundle.

  11. Analysis of spent fuel assay with a lead slowing down spectrometer

    SciTech Connect

    Gavron, Victor I; Smith, L. Eric; Ressler, Jennifer J

    2010-10-29

    Assay of fissile materials in spent fuel that are produced or depleted during the operation of a reactor, is of paramount importance to nuclear materials accounting, verification of the reactor operation history, as well as for criticality considerations for storage. In order to prevent future proliferation following the spread of nuclear energy, we must develop accurate methods to assay large quantities of nuclear fuels. We analyze the potential of using a Lead Slowing Down Spectrometer for assaying spent fuel. We conclude that it is possible to design a system that will provide around 1% statistical precision in the determination of the {sup 239}Pu, {sup 241}Pu and {sup 235}U concentrations in a PWR spent-fuel assembly, for intermediate-to-high burnup levels, using commercial neutron sources, and a system of {sup 238}U threshold fission detectors. Pending further analysis of systematic errors, it is possible that missing pins can be detected, as can asymmetry in the fuel bundle.

  12. Spectrum tailoring of the neutron energy spectrum in the context of delayed neutron detection

    SciTech Connect

    Koehler, William E; Tobin, Steve J; Sandoval, Nathan P; Fensin, Mike L

    2010-01-01

    For the purpose of measuring plutonium mass in spent fuel, a delayed neutron instrument is of particular interest since, if properly designed, the delayed neutron signal from {sup 235}U is significantly stronger than the signature from {sup 239}Pu or {sup 241}Pu. A key factor in properly designing a delayed neutron instrument is to minimize the fission of {sup 238}U. This minimization is achieved by keeping the interrogating neutron spectrum below {approx} 1 MeV. In the context of spent fuel measurements it is desirable to use a 14 MeV (deuterium and tritium) neutron generator for economic reasons. Spectrum tailoring is the term used to describe the inclusion of material between the 14 MeV neutrons and the interrogated object that lower the neutron energy through nuclear reactions and moderation. This report quantifies the utility of different material combination for spectrum tailoring.

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  14. New Prompt Fission γ-ray Data in Response to the OECD/NEA High Priority Request

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

    In this paper we report about new prompt fission γ-ray measurements, which we have performed with highly efficient γ-ray detectors based on lanthanide-halide crystals, aiming at very fast timing in conjunction with a good energy resolution. About four decades after the experiments were performed, whose results are still used for current evaluations, we present new spectral prompt fission γ-ray data from the reactions 252Cf(SF) and 235U(nth, f). Based on our new findings we recommend to replace the current ENDF/B-VII.1 evaluation for 252Cf(SF) and 235U(nth,f) as well as to perform new measurements for 238U(n, f) and 241Pu(n, f).

  15. Prompt Fission γ-ray Spectra Characteristics - A First Summary

    NASA Astrophysics Data System (ADS)

    Oberstedt, S.; Billnert, R.; Gatera, A.; Geerts, W.; Halipré, P.; Hambsch, F.-J.; Lebois, M.; Oberstedt, A.; Marini, P.; Vidali, M.; Wilson, J. N.

    In this work we give an overview of our investigations of prompt γ-ray emission in nuclear fission. This work was conducted during the last five years in response to a high priority nuclear data request formulated by the OECD/NEA. The aim was to reveal data deficiencies responsible for a severe under-prediction of the prompt γ heating in nuclear reactor cores. We obtained new prompt fission γ-ray spectral (PFGS) data for 252Cf(SF) as well as for thermal-neutron induced fission on 235U(nth,f) and 241Pu(nth,f). In addition, first PFGS measurements with a fast-neutron beam were accomplished, too. The impact of the new data and future data needs are discussed.

  16. A Time-Measurement System Based on Isotopic Ratios.

    SciTech Connect

    Vo, Duc T.; Karpius, P. J.; MacArthur, D. W.; Thron, J. L.

    2007-01-01

    A time-measurement system can be built based on the ratio of gamma-ray peak intensities from two radioactive isotopes. The ideal system would use a parent isotope with a short half-life decaying to a long half-life daughter. The activities of the parent-daughter isotopes would be measured using a gamma-ray detector system. The time can then be determined from the ratio of the activities. The best-known candidate for such a system is the {sup 241}Pu-{sup 241}Am parent-daughter pair. However, this {sup 241}Pu-{sup 241}Am system would require a high-purity germanium detector system and sophisticated software to separate and distinguish between the many gamma-ray peaks produced by the decays of the two isotopes. An alternate system would use two different isotopes, again one with a short half-life and one with a half-life that is long relative to the other. The pair of isotopes {sup 210}Pb and {sup 241}Am (with half-lives of 22 and 432 years, respectively) appears suitable for such a system. This time-measurement system operates by measuring the change in the ratio of the 47-keV peak of {sup 210}Pb to the 60-keV peak of {sup 241}Am. For the system to work reasonably well, the resolution of the detector would need to be such that the two gamma-ray peaks are well separated so that their peak areas can be accurately determined using a simple region-of-interest (ROI) method. A variety of detectors were tested to find a suitable system for this application. The results of these tests are presented here.

  17. Method for Ultratrace Level (241)Am Determination in Large Soil Samples by Sector Field-Inductively Coupled Plasma Mass Spectrometry: With Emphasis on the Removal of Spectral Interferences and Matrix Effect.

    PubMed

    Wang, Zhongtang; Zheng, Jian; Cao, Liguo; Tagami, Keiko; Uchida, Shigeo

    2016-07-19

    A new method using sector field-inductively coupled plasma mass spectrometry (SF-ICPMS) was developed for the determination of (241)Am in large soil samples to provide realistic soil-plant transfer parameter data for dose assessment of nuclear waste disposal plans. We investigated four subjects: extraction behaviors of interfering elements (Bi, Tl, Hg, Pb, Hf, and Pt) on DGA resin (normal type, abbreviated as DGA-N); soil matrix element removal (Mg, Fe, Al, K, Na) using Fe(OH)3, CaF2, and CaC2O4 coprecipitations; Am and rare earth elements (REEs) separation on DGA-N and TEVA resins; and optimization of SF-ICPMS (equipped with a high efficiency nebulizer (HEN)) for Am determination. Our method utilized concentrated HNO3 to leach Am from 2 to 20 g soil samples. The CaC2O4 coprecipitation was used to remove major metals in soil and followed by Am/interfering elements separation using the proposed UTEVA + DGA-N procedure. After a further separation of REEs on TEVA resin, (241)Am was determined by HEN-SF-ICPMS. This method eliminated the matrix effect in ICPMS (241)Am measurement for large soil samples. The high decontamination factors (DFs) of interfering elements enable their thorough removal, and in particular, the DF of Pu (7 × 10(5)) was the highest ever reported in (241)Am studies; thus, this method is capable of analyzing (241)Pu-contaminated Fukushima Daiichi Nuclear Power Plant (FDNPP) sourced soil samples. A low detection limit of 0.012 mBq g(-1) for (241)Am was achieved. The chemical recovery of Am (76-82%) was stable for soil samples. This method can be employed for the low level (241)Am determination in large size soil samples that are contaminated with (241)Pu. PMID:27322003

  18. A field strategy to monitor radioactivity associated with investigation derived wastes returned from deep drilling sites

    SciTech Connect

    Rego, J.H.; Smith, D.K.; Friensehner, A.V.

    1995-05-26

    The U.S. Department of Energy, Nevada Operations Office, Underground Test Area Operable Unit (UGTA) is drilling deep (>1500m) monitoring wells that penetrate both unsaturated (vadose) and saturated zones potentially contaminated by sub-surface nuclear weapons testing at the Nevada Test Site, Nye County, Nevada. Drill site radiological monitoring returns data on drilling effluents to make informed management decisions concerning fluid management. Because of rapid turn-around required for on-site monitoring, a representative sample will be analyzed simultaneously for {alpha}, {beta} and {gamma} emitters by instrumentation deployed on-site. For the purposes of field survey, accurate and precise data is returned, in many cases, with minimal sample treatment. A 30% efficient high purity germanium detector and a discriminating liquid scintillation detector are being evaluated for {gamma} and {alpha}/{beta} monitoring respectively. Implementation of these detector systems complements a successful on-site tritium monitoring program. Residual radioactivity associated with underground nuclear tests include tritium, activation products, fission products and actinides. Pulse shape discrimination (PSD) is used in {alpha}/{beta} liquid scintillation counting and is a function of the time distribution of photon emission. In particular, we hope to measure {sup 241}Am produced from {sup 241}Pu by {beta} decay. Because {sup 241}Pu is depleted in fissile bomb fuels, maximum PSD resolution will be required. The high purity germanium detector employs a multichannel analyzer to count gamma emitting radionuclides; we will designate specific window configurations to selectively monitor diagnostic fission product radionuclides (i.e., {sup 137}Cs).

  19. Using radiosilver and plutonium isotopes to trace the dispersion of contaminated sediment in Fukushima coastal catchments

    NASA Astrophysics Data System (ADS)

    Evrard, O.; Ayrault, S.; Pointurier, F.; Onda, Y.; Laceby, J. P.; Lepage, H.; Chartin, C.; Cirella, M.; Pottin, A. C.; Hubert, A.; Lefèvre, I.

    2015-12-01

    The Fukushima Dai-ichi nuclear power plant (FDNPP) accident in March 2011 resulted in a 3000-km² radioactive pollution plume consisting predominantly of radiocesium (137Cs and 134Cs). This plume is drained by several rivers to the Pacific Ocean after flowing through less contaminated, but densely inhabited coastal plains. As the redistribution of radionuclide contaminated sediment could expose the local population to higher radiation rates, novel fingerprinting methods were developed to trace the downstream dispersion of contaminated sediment. First, the heterogeneous deposition of metastable silver-110 (110mAg) across these coastal catchments was used to investigate sediment migration. In particular, the 110mAg/137Cs activity ratio was measured in soils and river sediment demonstrating the occurrence of a seasonal cycle of soil erosion during typhoons and spring snowmelt in 2011 and 2012. However, due to the rapid decay of 110mAg (half-life of 250 days), alternative methods were required to continue tracking sediment from 2013 onwards. One promising method includes the analyses of plutonium isotopes to further understand sediment migration in the Fukushima region. For example, 241Pu/239Pu atom ratios measured in sediment collected in Fukushima coastal rivers shortly after the accident were shown to be significantly higher (0.0017 - 0.0884) than corresponding values attributed to the global fallout (0.00113 ± 0.00008). Additional analyses were conducted on sediment sampled in 2013 and 2014 after the start of decontamination works. These analyses show that the 241Pu/239Pu atom ratios decreased towards the global fallout values in rivers draining decontaminated paddy fields, demonstrating the effectiveness of remediation works.

  20. Exchange effects in. beta. decays of many-electron atoms

    SciTech Connect

    Harston, M.R. University Chemical Laboratory, Lensfield Road, Cambridge CB21EW ); Pyper, N.C. )

    1992-05-01

    The effect on the {beta} spectrum of exchange between bound and continuum electrons is discussed for decay of a many-electron atom. Results of calculations of the exchange distortion of the {beta} spectrum are presented using both a screened hydrogenic and a Hartree-Fock approximation for the electron wave functions. The results of the two approaches agree well and show that the inclusion of exchange leads to an enhancement of the {beta} spectrum, particularly at low electron energy. This corrects an error in a previous calculation that found that exchange decreased the {beta} intensity. For the low-energy {beta}{sup {minus}} emitters {sup 106}Ru and {sup 241}Pu, the present calculation indicates that the enhancement due to exchange is of the order of several percent over much of the spectrum, becoming larger at very low electron energy. Exchange with 1{ital s} electrons dominates in the high-energy part of the spectrum, but exchange with {ital ns} ({ital n}{ge}2) electrons becomes significant in the low-energy region. The inclusion of exchange leads to an increase in the phase-space integral by 6.4% for {sup 106}Ru and 7.5% for {sup 241}Pu. Results are presented for exchange effects in other {beta} spectra, including those of {sup 14}C and {sup 35}S, in which experimentally measured distortions have been interpreted as evidence for a heavy antineutrino of mass 17 keV. The distortions due to exchange are found to be significantly smaller than the measured distortions.

  1. Improved predictions of reactor antineutrino spectra

    SciTech Connect

    Mueller, Th. A.; Lhuillier, D.; Letourneau, A.

    2011-05-15

    Precise predictions of the antineutrino spectra emitted by nuclear reactors is a key ingredient in measurements of reactor neutrino oscillations as well as in recent applications to the surveillance of power plants in the context of nonproliferation of nuclear weapons. We report new calculations including the latest information from nuclear databases and a detailed error budget. The first part of this work is the so-called ab initio approach where the total antineutrino spectrum is built from the sum of all {beta} branches of all fission products predicted by an evolution code. Systematic effects and missing information in nuclear databases lead to final relative uncertainties in the 10-20% range. A prediction of the antineutrino spectrum associated with the fission of {sup 238}U is given based on this ab initio method. For the dominant isotopes we developed a more accurate approach combining information from nuclear databases and reference electron spectra associated with the fission of {sup 235}U, {sup 239}Pu, and {sup 241}Pu, measured at Institut Laue-Langevin (ILL) in the 1980s. We show how the anchor point of the measured total {beta} spectra can be used to suppress the uncertainty in nuclear databases while taking advantage of all the information they contain. We provide new reference antineutrino spectra for {sup 235}U, {sup 239}Pu, and {sup 241}Pu isotopes in the 2-8 MeV range. While the shapes of the spectra and their uncertainties are comparable to those of the previous analysis of the ILL data, the normalization is shifted by about +3% on average. In the perspective of the reanalysis of past experiments and direct use of these results by upcoming oscillation experiments, we discuss the various sources of errors and their correlations as well as the corrections induced by off-equilibrium effects.

  2. Estimation of Radiation Doses in the Marshall Islands Based on Whole Body Counting of Cesium-137 (137Cs) and Plutonium Urinalysis

    SciTech Connect

    Daniels, J; Hickman, D; Kehl, S; Hamilton, T

    2007-06-11

    Under the auspices of the U.S. Department of Energy (USDOE), researchers from the Lawrence Livermore National Laboratory (LLNL) have recently implemented a series of initiatives to address long-term radiological surveillance needs at former nuclear test sites in the Republic of the Marshall Islands (RMI). The aim of this radiological surveillance monitoring program (RSMP) is to provide timely radiation protection for individuals in the Marshall Islands with respect to two of the most important internally deposited fallout radionuclides-cesium-137 ({sup 137}Cs) and long-lived isotopes 239 and 240 of plutonium ({sup 239+240}Pu) (Robison et al., 1997 and references therein). Therefore, whole-body counting for {sup 137}Cs and a sensitive bioassay for the presence of {sup 239+240}Pu excreted in urine were adopted as the two most applicable in vivo analytical methods to assess radiation doses for individuals in the RMI from internally deposited fallout radionuclides (see Hamilton et al., 2006a-c; Bell et al., 2002). Through 2005, the USDOE has established three permanent whole-body counting facilities in the Marshall Islands: the Enewetak Radiological Laboratory on Enewetak Atoll, the Utrok Whole-Body Counting Facility on Majuro Atoll, and the Rongelap Whole-Body Counting Facility on Rongelap Atoll. These whole-body counting facilities are operated and maintained by trained Marshallese technicians. Scientists from LLNL provide the technical support and training necessary for maintaining quality assurance for data acquisition and dose reporting. This technical basis document summarizes the methodologies used to calculate the annual total effective dose equivalent (TEDE; or dose for the calendar year of measurement) based on whole-body counting of internally deposited {sup 137}Cs and the measurement of {sup 239+240}Pu excreted in urine. Whole-body counting provides a direct measure of the total amount (or burden) of {sup 137}Cs present in the human body at the time of

  3. Americium, plutonium and uranium contamination and speciation in well waters, streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site, Kazakhstan.

    PubMed

    León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Jiménez Nápoles, H; Priest, N D

    2009-04-01

    New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with

  4. Radiation release at the nation's only operating deep geological repository--an independent monitoring perspective.

    PubMed

    Thakur, P; Ballard, S; Hardy, R

    2014-11-01

    Recent incidents at the nation's only operating deep geologic nuclear waste repository, the Waste Isolation Pilot Plant (WIPP), resulted in the release of americium and plutonium from one or more defense-related transuranic (TRU) waste containers into the environment. WIPP is a U.S. Department of Energy mined geologic repository that has been in operation since March, 1999. Over 85,000 m3 of waste in various vented payload containers have been emplaced in the repository. The primary radionuclides within the disposed waste are 239+240Pu and 241Am, which account for more than 99% of the total TRU radioactivity disposed and scheduled for disposal in the repository. For the first time in its 15 years of operation, there was an airborne radiation release from the WIPP at approximately 11:30 PM Mountain Standard Time (MST) on Friday, February 14, 2014. The radiation release was likely caused by a chemical reaction inside a TRU waste drum that contained nitrate salts and organic sorbent materials. In a recent news release, DOE announced that photos taken of the waste underground showed evidence of heat and gas pressure resulting in a deformed lid, in material expelled through that deformation, and in melted plastic and rubber and polyethylene in the vicinity of that drum. Recent entries into underground Panel 7 have confirmed that at least one waste drum containing a nitrate salt bearing waste stream from Los Alamos National Laboratory was breached underground and was the most likely source of the release. Further investigation is underway to determine if other containers contributed to the release. Air monitoring across the WIPP site intensified following the first reports of radiation detection underground to ascertain whether or not there were releases to the ground surface. Independent analytical results of air filters from sampling stations on and near the WIPP facility have been released by us at the Carlsbad Environmental Monitoring & Research Center and confirmed

  5. Reconstruction of local fallout composition and gamma-ray exposure in a village contaminated by the first USSR nuclear test in the Semipalatinsk nuclear test site in Kazakhstan.

    PubMed

    Imanaka, Tetsuji; Yamamoto, Masayoshi; Kawai, Kenta; Sakaguchi, Aya; Hoshi, Masaharu; Chaizhunusova, Nailya; Apsalikov, Kazbek

    2010-11-01

    After the disintegration of the USSR in end of 1991, it became possible for foreign scientists to visit Kazakhstan, in order to investigate the radiological consequences of nuclear explosions that had been conducted at the Semipalatinsk nuclear test site (SNTS). Since the first visit in 1994, our group has been continuing expeditions for soil sampling at various areas around SNTS. The current level of local fallout at SNTS was studied through γ-spectrometry for (137)Cs as well as α-spectrometry for (239,240)Pu. Average values of soil inventory from wide areas around SNTS were 3,500 and 3,700 Bq m(-2) for (137)Cs and (239,240)Pu, respectively, as of January 1, 2000. The average level of (137)Cs is comparable to that in Japan due to global fallout, while the level of (239,240)Pu is several tens of times larger than that in Japan. Areas of strong contamination were found along the trajectories of radioactive fallout, information on which was declassified after the collapse of the USSR. Our recent efforts of soil sampling were concentrated on the area around the Dolon village heavily affected by the radioactive plume from the first USSR atomic bomb test in 1949 and located 110 km east from ground zero of the explosion. Using soil inventory data, retrospective dosimetry was attempted by reconstructing γ-ray exposure from fission product nuclides deposited on the ground. Adopting representative parameters for the initial (137)Cs deposition (13 kBq m(-2)), the refractory/volatile deposition ratio (3.8) and the plume arrival time after explosion (2.5 h), an absorbed dose in air of 600 mGy was obtained for the 1-year cumulative dose in Dolon village, due to the first bomb test in 1949. Considering possible ranges of the parameters, 350 and 910 mGy were estimated for high and low cases of γ-ray dose in air, respectively. It was encouraging that the deduced value was consistent with other estimations using thermal luminescence and archived monitoring data. The present

  6. Nuclear Data Sheets for A = 240

    SciTech Connect

    Singh, Balraj; Browne, E.

    2008-10-15

    Evaluated experimental data for radioactive decays and reactions for known nuclides (U, Np, Pu, Am, Cm, Bk, Cf) of A = 240 are presented together with adopted values for level energies, {gamma}-ray energies, relative branching ratios and other nuclear properties. This revision was primarily motivated by the need for re-evaluation of absolute gamma-ray intensities from the {epsilon} decay of {sup 240}Am to {sup 240}Pu. These quantities are essential for determining precise and accurate cross-sections for the {sup 241}Am(n,2n){sup 240}Am reaction using fast neutrons (see e.g. Americium Workshop, Santa Fe, New Mexico, September 2007, 2008To06, 2007Ta01, 2006Pe14) and {sup 241}Am({gamma},n) reaction (see e.g. 2006Ri08). For {sup 240}U, the {gamma}-ray data have now become available. The data sets for {sup 244}Pu {alpha} decay to {sup 240}U; {sup 244}Cm {alpha} decay to {sup 240}Pu and {sup 244}Cf {alpha} decay to {sup 240}Cm have been adapted from evaluations by 1998Ak04 and 2003Ak04. For {sup 244}Cm decay, evaluation by 2006BeZL under the Decay Data Evaluation Project (DDEP) is also used. The {gamma}-ray data (energies and intensities) for {sup 240}Cm decay are not considered (by the evaluators) as well established. Most detailed data are available only for {sup 240}Pu. Extensive data in the second potential well are available for this nuclide together with fission isomers and several superdeformed (SD) structures. For other nuclides spectroscopic data are rather sparse in the literature; especially for the following radioactive decays: The {epsilon} decays of {sup 240}Cf, {sup 240}Bk and {sup 240}Cm; multipolarities of {gamma}-ray transitions in {sup 240}Np from {sup 240}U {beta}{sup -} decay; {gamma}-ray transitions from {sup 244}Cf {alpha} decay and %{epsilon} branch of {sup 244}Cf decay; spins and parities of excited states in {sup 240}U and multipolarities of associated {gamma}-ray transitions in {sup 240}U. This work supersedes earlier full evaluations of A

  7. Flux of transuranium nuclides and chlorinated hydrocarbons in the northwestern Mediterranean

    NASA Astrophysics Data System (ADS)

    Fowler, S. W.; Ballestra, S.; Villeneuve, J.-P.

    1990-09-01

    The transuranium nuclides, plutonium and americium, and selected chlorinated hydrocarbon compounds have been measured in sediment trap samples, bottom sediments and waters. These measurements have been used to quantify vertical fluxes and elucidate particulate biogeochemical cycles, of these man-made contaminants in the northwestern Mediterranean. Sediment trap experiments in the Gulf of Lions (Lacaze-Duthiers Canyon) have shown that transuranic fluxes are considerably higher in the Gulf of Lions, than those which have been reported for the northeast Pacific; principally this is due to the relatively high mass fluxes in this region of the Mediterranean. Water, surface sediment and sediment trap data indicate that 241Am is being transported downward (via particle settling) more rapidly than 239+240Pu. From direct flux measurement, residence times for 239+240Pu and 241Am in the upper 300 m were computed to be 2.5 and 0.14 years, respectively. Comparison of 239+240Pu concentrations in the water column, in 1986, with similar measurements made 5-11 years earlier suggests that fallout input to the Mediterranean has decreased by nearly a factor of 2 during the period 1975-1986. Fluxes of PCB, HCB, γ-HCH and DDT residues varied by as much as an order of magnitude, or more, both temporally and with depth. The average fluxes of most of the compounds in the Lacaze-Duthiers Canyon, during 1985-1986, were quite similar to those measured off the coast of Monaco several years earlier. Generally, the increased chlorinated hydrocarbon fluxes observed with depth were a direct result of the much higher mass fluxes which occurred at depth. Demonstrated differences in PCB concentrations in the settling particles, deposited surface sediments and overlying sediment floc indicate that simple bottom sediment resuspension is not a major contributor to the enhanced PCB flux noted at depth. The PCB concentration in sedimenting particulate material collected from deeper waters, is similar to

  8. USTUR WHOLE BODY CASE 0269: DEMONSTRATING EFFECTIVENESS OF I.V. CA-DTPA FOR PU

    SciTech Connect

    James, Anthony C.; Sasser , Lyle B.; Stuit, Dorothy B.; Glover, Samuel E.; Carbaugh, Eugene H.

    2008-01-28

    This whole body donation case (USTUR Registrant) involved a single acute inhalation of an acidic Pu(NO3)4 solution in the form of an aerosol ‘mist.’ Chelation treatment with i.v. Ca-EDTA was initiated on the day of the intake, and continued intermittently over 6 months. After 2½ years with no further treatment, a course of i.v. Ca-DTPA was administered. A total of 400 measurements of 239+240Pu excreted in urine were recorded; starting on the first day (both before and during the initial Ca-EDTA chelation), and continuing for 37 years. This sampling included all intervals of chelation. In addition, 91 measurements of 239+240Pu-in-feces were recorded over this whole period. The Registrant died about 38 years after the intake, at age 79 y, with extensive carcinomatosis secondary to adenocarcinoma of the prostate gland. At autopsy, all major soft tissue organs were harvested for radiochemical analyses of their 238Pu, 239+240Pu and 241Am content. Also, all types of bone (comprising about half the skeleton) were harvested for radiochemical analyses, as well as samples of skin, subcutaneous fat and muscle. This comprehensive dataset has been applied to derive ‘chelation-enhanced’ transfer rates in the ICRP Publication 67 plutonium biokinetic model, representing the behaviour of blood-borne and tissue-incorporated plutonium during intervals of therapy. The resulting model of the separate effects of i.v. Ca-EDTA and Ca-DTPA chelation shows that the therapy administered in this case succeeded in reducing substantially the long-term burden of plutonium in all body organs, except for the lungs. The calculated reductions in organ content at the time of death are approximately 40% for the liver, 60% for other soft tissues (muscle, skin, glands, etc.), 50% for the kidneys, and 50% for the skeleton. Essentially all of the substantial reduction in skeletal burden occurred in trabecular bone. This modeling exercise demonstrated that 3-y-delayed Ca-DTPA therapy was as

  9. Radionuclide concentrations in vegetation at the Los Alamos National Laboratory in 1998

    SciTech Connect

    G. J. Gonzales; P. R. Fresquez; M. A. Mullen; L. Naranjo, Jr.

    2000-03-01

    This report summarizes and evaluates the concentrations of {sup 3}H, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 90}Sr, and total U in understory and overstory vegetation collected from Los Alamos National Laboratory (LANL), its perimeter, and regional background areas in 1998. Comparisons to conservative toxicity reference value safe limits were also made. The arithmetic mean LANL radionuclide concentrations in understory were 501 pCi L{sup {minus}1} for {sup 3}H, 0.581 pCi ash g{sup {minus}1} for {sup 137}Cs, 0.001 pCi ash g{sup {minus}1} for {sup 238}Pu, 0.008 pCi ash g{sup {minus}1} for {sup 239,240}Pu, 0.007 pCi ash g{sup {minus}1} for {sup 241}Am, 1.46 pCi ash g{sup {minus}1} for {sup 90}Sr, and 0.233 {micro}g ash g{sup {minus}1} for total uranium. The mean LANL radionuclide concentrations in overstory were 463 pCi L{sup {minus}1} for {sup 3}H, 1.51 pCi ash g{sup {minus}1} for {sup 137}Cs, 0.0004 pCi ash g{sup {minus}1} {sup 238}Pu, 0.008 pCi ash g{sup {minus}1} for {sup 239,240}Pu, 0.014 pCi ash g{sup {minus}1} for {sup 241}Am, 1.97 pCi ash g{sup {minus}1} for {sup 90}Sr, and 0.388 {micro}g ash g{sup {minus}1} for total uranium. Concentrations of radionuclides and total U in both understory and overstory vegetation at LANL generally were not statistically higher than in perimeter and regional background vegetation ({alpha} = 0.05). The exceptions were LANL {sup 3}H > perimeter {sup 3}H (understory) and LANL {sup 3}H background {sup 3}H (overstory). All maximum radionuclide concentrations were lower than toxicity reference values. With the exception of total U, the relationship between contaminant concentration in soil vs. vegetation was insignificant ({alpha} = 0.05). Generally, as the concentration of total U in soil decreased, the concentration in vegetation increased. This held true for both understory and overstory and regardless of whether data were separated by general location (LANL, perimeter, and background) or not. There was no

  10. The concentration of radionuclides and metals in vegetation adjacent to and in the SRL Seepage Basins

    SciTech Connect

    Murphy, C. E. Jr.

    1992-12-14

    In 1991 the trees on the dikes surrounding the SRL Seepage Basins were sampled and analyzed to inventory the contaminants transported from the basins into the vegetation. Tree leaves and wood were collected and analyzed for [sup 90]Sr, [sup 60]Co, [sup 137]Cs, [sup 238]Pu, [sup 239,240]Pu, [sup 242,244]Cm, [sup 241]Am, Ba, Cr, Hg, Mg, Mn, Ni, and Pb. The concentrations of contaminants were influenced by sample type (leaves versus wood), species type (pines versus hardwoods), and location relative to distance from the basin. The total inventory of each contaminant in the trees was estimated. The relationships between leaf and wood, pines and hardwood, location, and mass of the material in each of these classes were used to weight the total inventory estimate. The radionuclide with the largest inventory was 0.7 mCi for [sup 90]Sr. The metallic contaminant with the largest inventory was Mn at 200 gm.

  11. Prototype fast neutron counter for the assay of impure plutonium

    SciTech Connect

    Wachter, J.R.; Adams, E.L.; Ensslin, N.

    1987-01-01

    A fast coincident neutron counter using liquid scintillators and gamma-ray/neutron pulse-shape discrimination has been constructed for the analysis of plutonium samples with unknown self-multiplication and (..cap alpha..,n) production. The counter was used to measure plutonium-bearing materials that cover a range of masses and (..cap alpha..,n) reaction rates of importance to the safeguards community. Measured values of the /sup 240/Pu effective mass differed, on average, from their declared values by 0.4% for plutonium oxides and by -2.2% for metal and MgO-loaded samples. Poorer results were obtained for materials with large (..cap alpha..,n) reaction rates and low self-multiplication such as plutonium ash and plutonium fluoride.

  12. Background concentrations of radionuclides in soils and river sediments in northern New Mexico, 1974-1986

    SciTech Connect

    Purtymun, W.D.; Peters, R.J.; Buhl, T.E.; Maes, M.N.; Brown, F.H.

    1987-11-01

    This report documents the range and the upper limit for background concentrations of radionuclides and radioactivity in soils and river sediments that occur as natural rock-forming minerals and worldwide fallout from atmospheric nuclear weapons tests. Documentation is based on the collection of soil and sediment in northern New Mexico and analyzed for /sup 137/Cs, /sup 238/Pu, /sup 239,240/Pu, /sup 90/Sr, total uranium, gross gamma, and tritium. The data used to establish the statistical range and upper limit of background concentration cover a 9- or 13-year period ending in 1986. The knowledge of background levels is necessary to interpret soil and sediment data collected for the annual environmental surveillance report and other reports relating to radionuclides or radioactivity in soils and sediments. 11 refs., 1 fig., 5 tabs.

  13. Minor Actinides, Major Challenges, the Needs for and Benefits of International Collaboration

    NASA Astrophysics Data System (ADS)

    Plompen, A. J. M.

    2014-04-01

    The role of experiments for the determination of minor actinide nuclear data is presented as essential to meet the tight uncertainties requirements derived by sensitivity analyses for innovative systems designed to significantly reduce the amount of high level nuclear waste. Recent, ongoing and planned experiments are highlighted emphasizing international collaboration and the European context. Specifically, the role of the MANREAD CRP, the European projects ANDES, ERINDA and EURFRAT, and the NEA databank and WPEC subgroups will be addressed. For 241Am capture and 240Pu fission are used to illustrate the generic situation with minor actinide experimental data and the discrepancy between achieved and target uncertainties. The importance of new high quality experiments, high quality reporting, diversity, new techniques, methods and facilities is stressed.

  14. The underwater coincidence counter for plutonium measurements in mixed-oxide fuel assemblies manual

    SciTech Connect

    G. W. Eccleston; H. O. Menlove; M. Abhold; M. Baker; J. Pecos

    1999-05-01

    This manual describes the Underwater Coincidence Counter (UWCC) that has been designed for the measurement of plutonium in mixed-oxide (MOX) fuel assemblies prior to irradiation. The UWCC uses high-efficiency {sup 3}He neutron detectors to measure the spontaneous-fission and induced-fission rates in the fuel assembly. Measurements can be made on MOX fuel assemblies in air or underwater. The neutron counting rate is analyzed for singles, doubles, and triples time correlations to determine the {sup 240}Pu effective mass per unit length of the fuel assembly. The system can verify the plutonium loading per unit length to a precision of less than 1% in a measurement time of 2 to 3 minutes. System design, components, performance tests, and operational characteristics are described in this manual.

  15. Multi-collector Isotope Ratio Mass Spectrometer -- Operational Performance Report

    SciTech Connect

    Appelhans, Anthony D; Olson, John E; Watrous, Matthew G; Ward, Michael B.; Dahl, David A.

    2010-12-01

    This report describes the operational testing of a new magnetic sector mass spectrometer that utilizes seven full-sized discrete dynode electron multipliers operating simultaneously. The instrument includes a newly developed ion dispersion lens that enables the mass dispersed individual isotope beams to be separated sufficiently to allow a full-sized discrete dynode pulse counting multiplier to be used to measure each isotope beam. The performance of the instrument was measured using SRM 996 (244Pu spike) at loadings of 2.4 and 12 fg on resin beads and with SRM 4350B Columbia River Sediment samples. The measured limit of detection (3s) for 240Pu was 3.4 attograms for SRM 996. The limit of quantitation (LOQ), defined as 10 s, was 11.2 attograms. The measured concentration of 239Pu in the CRS standard was 152 ± 6 fg/g.

  16. Advanced alpha spectrum analysis based on the fitting and covariance analysis of dependent variables

    NASA Astrophysics Data System (ADS)

    Ihantola, S.; Pelikan, A.; Pöllänen, R.; Toivonen, H.

    2011-11-01

    The correct handling of statistical uncertainties is crucial especially when unfolding alpha spectra that contain a low number of counts or overlapping peaks from different nuclides. For this purpose, we have developed a new spectrum analysis software package called ADAM, which performs a full covariance calculus for alpha-particle emitting radionuclides. By analyzing a large number of simulated and measured spectra, the program was proved to give unbiased peak areas and statistically correct uncertainty limits. This applies regardless of the peak areas and the number of unknown parameters during the fitting. In addition, ADAM performs reliable deconvolution for multiplets, which opens the way for the determination of isotope ratios, such as 239Pu/240Pu.

  17. Induced fission of Pu240 within a real-time microscopic framework

    DOE PAGESBeta

    Bulgac, Aurel; Magierski, Piotr; Roche, Kenneth J.; Stetcu, Ionel

    2016-03-25

    Here, we describe the fissioning dynamics of 240Pu from a configuration in the proximity of the outer fission barrier to full scission and the formation of the fragments within an implementation of density functional theory extended to superfluid systems and real-time dynamics. The fission fragments emerge with properties similar to those determined experimentally, while the fission dynamics appears to be quite complex, with many excited shape and pairing modes. The evolution is found to be much slower than previously expected, and the ultimate role of the collective inertia is found to be negligible in this fully nonadiabatic treatment of nuclearmore » dynamics, where all collective degrees of freedom (CDOF) are included (unlike adiabatic treatments with a small number of CDOF).« less

  18. Geotrupine beetles (Coleoptera: Scarabaeoidea) as bio-monitors of man-made radioactivity.

    PubMed

    Mietelski, Jerzy W; Szwałko, Przemysław; Tomankiewicz, Ewa; Gaca, Paweł; Grabowska, Sylwia

    2003-04-01

    Adults of the geotrupine beetle Anoplotrupes stercorosus (Coleoptera, Geotrupidae), a common European forest insect species, were used in the role of bio-monitors for mainly man-made radionuclides in a forest environment. Activities of 137Cs, 40K, 238Pu, (239+240)Pu, 90Sr and 241Am were studied. Samples originated from four areas in Poland, two from the north-east and two from the south of the country. The north-eastern areas were previously recognized as the places where hot particle fallout from Chernobyl took place. Results confirmed the differences in the activities between north-eastern and southern locations. Significant correlations were found between activities of 40K and 137Cs, and between activities of plutonium and americium isotopes. An additional study of the concentration of radionuclides within the bodies of beetles showed a general pattern of distribution of radioisotopes in the insect body. PMID:12729271

  19. Initial performance of the advanced inventory verification sample system (AVIS)

    SciTech Connect

    Marlow, Johnna B; Swinhoe, Martyn T; Menlove, Howard O; Rael, Carlos D

    2009-01-01

    This paper describes the requirements, design and initial performance of the Advanced Inventory Verification Sample System (AVIS) a non-destructive assay (NDA) system to measure small samples of bulk mixed uranium-plutonium oxide (MOX) materials (powders and pellets). The AVIS design has evolved from previously developed conceptual physics and engineering designs for the Inventory Sample Verification System (INVS), a safeguards system for nondestructive assay of small samples. The AVIS is an integrated gamma-neutron system. Jointly designed by the Nuclear Material Control Center (NMCC) and the Los Alamos National Laboratory (LANL), AVIS is intended to meet a performance specification of a total measurement uncertainty of less than 0.5% in the neutron ({sup 240}Pu{sub effective}) measurement. This will allow the AVIS to replace destructive chemical analysis for many samples, with concomitant cost, exposure and waste generation savings for the facility. Data taken to date confirming the performance of the AVIS is presented.

  20. A survey of radioactive fallout data in Alaska

    SciTech Connect

    DePhillips, M.P.

    1995-10-23

    Considerable attention has been directed by the scientific community to assessing the levels and fate of radionuclides in Arctic ecosystems. The following text and tables present available data and discussion of radionuclide fallout in Alaska. A literature search of 23 on-line databases (Table 1) using Alaska, Strontium (Sr), Cesium (Cs), Plutonium (Pu) and Radionuclide as constraint terms responded with 177 possible citations. After eliminating duplicate citations, 31 articles were available: 17 were relevant to the subject matter; the remainder addressed geologic issues. All of the cited literature addressed {sup 137}Cs, {sup 90}Sr and {sup 239,240}Pu as a result of radionuclide fallout from nuclear testing or accidental release.

  1. [Man-made radionuclides and their accumulation by plants of different taxonomic groups from the soils of the eastern ural radioactive trace].

    PubMed

    Molchanova, I V; Mikhaĭlovskaia, L N; Pozolotina, V N; Antonova, E V

    2014-01-01

    Investigations of the spatial and vertical distribution of 90Sr, 137Cs and 239, 240Pu in the soils of the Eastern Ural Radioactive Trace (EURT) and accumulation of these radionuclides by plants were carried out in 2003-2011. Investigations showed that the spatial distribution of the radionuclides with increasing distances from the epicenter of the accident is satisfactorily approximated by the exponential function. During the post-accidental period the essential amount of radionuclides is located in the 15-20 cm root layer of the soil. Uptake by plants of 90Sr is determined, first of all, by the level of the soil contamination. For 137Cs, reliable differences in its accumulation ability between representatives of the higher plants and lower ones are remained in the whole gradient of contamination. PMID:25764849

  2. Current assessment of integrated content of long-lived radionuclides in soils of the head part of the East Ural Radioactive Trace.

    PubMed

    Molchanova, I; Mikhailovskaya, L; Antonov, K; Pozolotina, V; Antonova, E

    2014-12-01

    Based on the datasets obtained during investigations from 2003 to 2012, the spatial distributions of (90)Sr, (137)Cs, and (239,240)Pu content in the soils of the head part of the East Ural Radioactive Trace (EURT) were mapped using the geographic information system ArcGIS. Taking into account the presence of spatial autocorrelation and anisotropy in the source data, an ordinary kriging method was applied to interpolate values of radionuclide contamination density at unsampled places. Further geostatistical data analysis was performed to determine the basic parameters of spatial dependencies and to integrally assess the contamination by long-lived radionuclides in soils of the central, east peripheral, and west peripheral parts of the trace. This analysis was based on simplified geometric models (sector- and rectangle-shaped areas). The Monte Carlo method was used to quantitatively assess the uncertainty of the values for the integrated quantities resulting from the statistical errors of the source data approximation. PMID:25262151

  3. [Dynamic study of the cytogenetic effects in blood lymphocytes from humans living in the Chernobyl Atomic Energy Station exclusion zone without permission].

    PubMed

    Bezdrobnaia, L K; Tsyganok, T V; Romanova, E P; Tarasenko, L V; Fedorchenko, V I

    2002-01-01

    The cytogenetic examination of a group of people, self-residing in ChNPP Exclusion Zone with soil contamination density 137Cs 74-477 kBq/m2, 90Sr 33-289 kBq/m2, 238, 239 + 240Pu 1.5-10.0 kBq/m2, was conducted in 1998-1999 and also 2001. It is shown, that after 12-15 years of the accident the level of chromosome damages in Zone self-residents' lymphocytes detected by a routine analysis is higher then at the residents of control Yagotin district, Kiev region and comes to a plateau. Lymphocytes with multiple chromosome damages are detected. The probability of its transuranium elements induction which are present in the Zone is discussed at present. PMID:12530160

  4. Sources of plutonium in the atmosphere and stratosphere-troposphere mixing

    NASA Astrophysics Data System (ADS)

    Hirose, Katsumi; Povinec, Pavel P.

    2015-10-01

    Plutonium isotopes have primarily been injected to the stratosphere by the atmospheric nuclear weapon tests and the burn-up of the SNAP-9A satellite. Here we show by using published data that the stratospheric plutonium exponentially decreased with apparent residence time of 1.5 ± 0.5 years, and that the temporal variations of plutonium in surface air followed the stratospheric trends until the early 1980s. In the 2000s, plutonium and its isotope ratios in the atmosphere varied dynamically, and sporadic high concentrations of 239,240Pu reported for the lower stratospheric and upper tropospheric aerosols may be due to environmental events such as the global dust outbreaks and biomass burning.

  5. AFCI-2.0 Library of Neutron Cross Section Covariances

    SciTech Connect

    Herman, M.; Herman,M.; Oblozinsky,P.; Mattoon,C.; Pigni,M.; Hoblit,S.; Mughabghab,S.F.; Sonzogni,A.; Talou,P.; Chadwick,M.B.; Hale.G.M.; Kahler,A.C.; Kawano,T.; Little,R.C.; Young,P.G.

    2011-06-26

    Neutron cross section covariance library has been under development by BNL-LANL collaborative effort over the last three years. The primary purpose of the library is to provide covariances for the Advanced Fuel Cycle Initiative (AFCI) data adjustment project, which is focusing on the needs of fast advanced burner reactors. The covariances refer to central values given in the 2006 release of the U.S. neutron evaluated library ENDF/B-VII. The preliminary version (AFCI-2.0beta) has been completed in October 2010 and made available to the users for comments. In the final 2.0 release, covariances for a few materials were updated, in particular new LANL evaluations for {sup 238,240}Pu and {sup 241}Am were adopted. BNL was responsible for covariances for structural materials and fission products, management of the library and coordination of the work, while LANL was in charge of covariances for light nuclei and for actinides.

  6. Concepts for Alpha Coincidence Detection

    SciTech Connect

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

    2015-03-01

    The effectiveness of conventional measurement techniques for environmental monitoring is limited by background and other interferences. We are exploring a new measurement approach involving the detection of α particles in coincidence with conversion electrons as a means to simultaneously assay environmental samples for actinides without chemical separation. The initial target isotopes studied in this work are 238Pu, 239Pu, 240Pu and 241Am. We explore various aspects of the design, such as impact of the mounting of the source material, resolution requirements and impact of a background on isotopic uncertainties. We conclude that a dual gas proportional counter and a dual-sided, large-area silicon detector could provide similar performance for the measurement scenario examined.

  7. Dose Estimates from Ingestion of Marine and Terrestrial Animals Harvested in the Beaufort Sea and Northwestern Alaska

    SciTech Connect

    W. C. T. Inkret; M. E. Schillaci; D. W. Efurd; M. E. Ennis; M. J. Hameedi; J. M. Inkret; T. H. T. Little; G. Miller

    2000-11-01

    Between 1993 and 1995, marine and terrestrial animal samples were collected from the Beaufort Sea and northwest Alaska. These samples were analyzed at Los Alamos National Laboratory for the presence of the anthropogenic radionuclides, {sup 90}Sr, {sup 137}Cs, {sup 238}Pu, {sup 239+240}Pu, and {sup 241}Am. The measurement data were combined with food consumption rates based on survey results for populations residing in three northwest Alaskan communities and published age-dependent ingestion dose coefficients to estimate potential radiological impacts from the consumption of traditional animal foods harvested in this region. The results of this study indicate that committed equivalent doses to adults from {sup 90}Sr and {sup 137}Cs, due to consumption of traditional food sources are consistent with currently accepted estimates of average doses to adults in North America due to atmospheric nuclear weapons testing fallout.

  8. Concentrations of Radionuclides and Trace Elements in Soils and Vegetation Around the DARHT Facility during 2004

    SciTech Connect

    P.R. Fresquez

    2004-10-01

    Samples of soil, sediment, and unwashed overstory and understory vegetation were collected at four locations around the Dual-Axis Radiographic Hydrodynamic Test (DARHT) facility at Los Alamos National Laboratory (LANL). All samples were analyzed for concentrations of {sup 3}H, {sup 137}Cs, {sup 90}Sr, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 234}U, {sup 235}U, {sup 238}U, Ag, As, Ba, Be, Cd, Cr, Cu, Hg, Ni, Pb, Sb, Se, and Tl. These results, which represent five years since the start of operations, were compared with baseline statistical reference level (BSRL) data established over a four-year-long preoperational period prior to DARHT operations, and to LANL and U.S. Environmental Protection Agency Screening Action Levels (SALs). Most radionuclides and trace elements in soil, sediment, and vegetation were below BSRL values and those soils/sediments that were above BSRLs were far below SALs.

  9. The Characterization of Biotic and Abiotic Media Upgradient and Downgradient of the Los Alamos Canyon Weir

    SciTech Connect

    P.R. Fresquez

    2006-01-15

    As per the Mitigation Action Plan for the Special Environmental Analysis of the actions taken in response to the Cerro Grande Fire, sediments, vegetation, and small mammals were collected directly up- and downgradient of the Los Alamos Canyon weir, a low-head sediment control structure located on the northeastern boundary of Los Alamos National Laboratory, to determine contaminant impacts, if any. All radionuclides ({sup 3}H, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu, {sup 90}Sr, {sup 241}Am, {sup 234}U, {sup 235}U and {sup 238}U) and trace elements (Ag, As, Ba, Be, Cd, Cr, Cu, Hg, Ni, Pb, Sb, Se, and Tl) in these media were low and most were below regional upper level background concentrations (mean plus three sigma). The very few constituents that were above regional background concentrations were far below screening levels (set from State and Federal standards) for the protection of the human food chain and the terrestrial environment.

  10. Radiological dose assessments of atolls in the Northern Marshall Islands

    SciTech Connect

    Robison, W.L.

    1983-11-01

    Methods and models used to estimate the radiation doses to a returning population of the atolls in the Marshall Islands are presented. In this environment natural processes have acted on source-term radionuclides for nearly 30 years. The data bases developed for the models, and the results of the radiological dose analyses at the various atolls are described. The major radionuclides in order of their contribution to the total estimated doses were /sup 137/Cs, /sup 90/Sr, /sup 239/ /sup 240/Pu, /sup 241/Am, and /sup 60/Co. Exposure pathways in order of their contribution to the estimated doses were: terrestrial food chain, external ..gamma.., marine food chain, inhalation, and cistern water and ground water. 56 references, 13 figures, 16 tables.

  11. Concentrations of radionuclides in reef and lagoon pelagic fish from the Marshall Islands

    SciTech Connect

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

    1981-07-01

    A radiological survey was conducted from September through November of 1978 to assess the concentrations of persistent man-made radionuclides in the terrestrial and marine environments of 11 atolls and 2 islands of the Northern Marshall Islands. The atolls and islands include Rongelap, Utirik, Taka, Bikar, Rongerik, Ailinginae, Likiep, Jemo, Ailuk, Mejet, Wotho, Ujelang and Bikini. Over 4000 terrestrial and marine samples were collected for radionuclide analysis from 76 different islands. Soils, vegetation, indigenous animals, and cistern and groundwater were collected from the islands. Reef fish, pelagic species, clams, lagoon water, and sediments were obtained from the lagoons. A report is given of all available concentration data for /sup 137/Cs, /sup 90/Sr, /sup 239+240/Pu, /sup 238/Pu, /sup 241/Am as well as naturally occurring /sup 40/K and other gamma emitting radionuclides in tissues and organs of different species of fish collected from the atolls.

  12. SUBSURFACE MOBILE PLUTONIUM SPECIATION: SAMPLING ARTIFACTS FOR GROUNDWATER COLLOIDS

    SciTech Connect

    Kaplan, D.; Buesseler, K.

    2010-06-29

    A recent review found several conflicting conclusions regarding colloid-facilitated transport of radionuclides in groundwater and noted that colloids can both facilitate and retard transport. Given these contrasting conclusions and the profound implications even trace concentrations of plutonium (Pu) have on the calculated risk posed to human health, it is important that the methodology used to sample groundwater colloids be free of artifacts. The objective of this study was: (1) to conduct a field study and measure Pu speciation, ({sup 239}Pu and {sup 240}Pu for reduced-Pu{sub aq}, oxidized-Pu{sub aq}, reduced-Pu{sub colloid}, and oxidized-Pu{sub colloid}), in a Savannah River Site (SRS) aquifer along a pH gradient in F-Area, (2) to determine the impact of pumping rate on Pu concentration, Pu speciation, and Pu isotopic ratios, (3) determine the impact of delayed sample processing (as opposed to processing directly from the well).

  13. The concentration of radionuclides and metals in vegetation adjacent to and in the SRL Seepage Basins

    SciTech Connect

    Murphy, C. E. Jr.

    1992-12-14

    In 1991 the trees on the dikes surrounding the SRL Seepage Basins were sampled and analyzed to inventory the contaminants transported from the basins into the vegetation. Tree leaves and wood were collected and analyzed for {sup 90}Sr, {sup 60}Co, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu, {sup 242,244}Cm, {sup 241}Am, Ba, Cr, Hg, Mg, Mn, Ni, and Pb. The concentrations of contaminants were influenced by sample type (leaves versus wood), species type (pines versus hardwoods), and location relative to distance from the basin. The total inventory of each contaminant in the trees was estimated. The relationships between leaf and wood, pines and hardwood, location, and mass of the material in each of these classes were used to weight the total inventory estimate. The radionuclide with the largest inventory was 0.7 mCi for {sup 90}Sr. The metallic contaminant with the largest inventory was Mn at 200 gm.

  14. Applications of Event-by-Event Fission Modeling with FREYA

    SciTech Connect

    Vogt, R; Randrup, J

    2011-09-16

    The recently developed code FREYA (Fission Reaction Event Yield Algorithm) generates large samples of complete fission events, consisting of two receding product nuclei as well as a number of neutrons and photons, all with complete kinematic information. Thus it is possible to calculate arbitrary correlation observables whose behavior may provide unique insight into the fission process. We first discuss the present status of FREYA, which has now been extended to include spontaneous fission. Concentrating on {sup 239}Pu(n{sub th},f), {sup 240}Pu(sf) and {sup 252}Cf(sf), we discuss the neutron multiplicity correlations, the dependence of the neutron energy spectrum on the neutron multiplicity, and the relationship between the fragment kinetic energy and the number of neutrons and their energies. We also suggest novel fission observables that could be measured with modern detectors.

  15. Radionuclides in Arctic sea ice: Tracers of sources, fates and ice transit time scales

    NASA Astrophysics Data System (ADS)

    Masqué, P.; Cochran, J. K.; Hirschberg, D. J.; Dethleff, D.; Hebbeln, D.; Winkler, A.; Pfirman, S.

    2007-08-01

    Arctic sea ice can incorporate sediment and associated chemical species during its formation in shallow shelf environments and can also intercept atmospherically transported material during transit. Release of this material in ice ablation areas (e.g. the Fram Strait) enhances fluxes of both sediments and associated species in such areas. We have used a suite of natural ( 7Be, 210Pb) and anthropogenic ( 137Cs, 239Pu, 240Pu) radionuclides in sea ice, sea-ice sediments (SIS), sediment trap material and bottom sediments from the Fram Strait to estimate transit times of sea ice from source to ablation areas, calculate radionuclide fluxes to the Fram Strait and investigate the role of sea-ice entrained sediments in sedimentation processes. Sea ice intercepts and transports the atmospherically supplied radionuclides 7Be and 210Pb, which are carried in the ice and are scavenged by any entrained SIS. All of the 7Be and most of the excess 210Pb measured in SIS collected in the Fram Strait are added to the ice during transit through the Arctic Ocean, and we use these radionuclides as chronometers to calculate ice transit times for individual ice floes. Transit times estimated from the 210Pb inventories in two ice cores are 1-3 years. Values estimated from the 7Be/ 210Pb excess activity ratio of SIS are about 3-5 years. Finally, equilibrium values of the activity ratio of 210Pb to its granddaughter 210Po in the ice cores indicate transit times of at least 2 years. These transit times are consistent with back-trajectory analyses of the ice floes. The latter, as well as the clay-mineral assemblage of the SIS (low smectite and high illite content), suggest that the sampled sea-ice floes originated from the eastern Siberian Arctic shelf seas such as the eastern Laptev Sea and the East Siberian Sea. This result is in agreement with the relatively low activities of 239,240Pu and 137Cs and the 240Pu/ 239Pu atom ratios (˜0.18, equivalent to that in global fallout) in SIS, indicating

  16. Sources of plutonium in the atmosphere and stratosphere-troposphere mixing.

    PubMed

    Hirose, Katsumi; Povinec, Pavel P

    2015-01-01

    Plutonium isotopes have primarily been injected to the stratosphere by the atmospheric nuclear weapon tests and the burn-up of the SNAP-9A satellite. Here we show by using published data that the stratospheric plutonium exponentially decreased with apparent residence time of 1.5 ± 0.5 years, and that the temporal variations of plutonium in surface air followed the stratospheric trends until the early 1980s. In the 2000s, plutonium and its isotope ratios in the atmosphere varied dynamically, and sporadic high concentrations of (239,240)Pu reported for the lower stratospheric and upper tropospheric aerosols may be due to environmental events such as the global dust outbreaks and biomass burning. PMID:26508010

  17. Characterization of the scission point from fission-fragment velocities

    NASA Astrophysics Data System (ADS)

    Caamaño, M.; Farget, F.; Delaune, O.; Schmidt, K.-H.; Schmitt, C.; Audouin, L.; Bacri, C.-O.; Benlliure, J.; Casarejos, E.; Derkx, X.; Fernández-Domínguez, B.; Gaudefroy, L.; Golabek, C.; Jurado, B.; Lemasson, A.; Ramos, D.; Rodríguez-Tajes, C.; Roger, T.; Shrivastava, A.

    2015-09-01

    The isotopic yield distributions and kinematic properties of fragments produced in the transfer-induced fission of 240Pu and fusion-induced fission of 250Cf, with 9 MeV and 45 MeV excitation energy, respectively, were measured in inverse kinematics with the spectrometer VAMOS. The kinematics of identified fission fragments allow to derive properties of the scission configuration such as the distance between fragments, the total kinetic energy, the neutron multiplicity, the total excitation energy, and, for the first time, the proton- and neutron-number sharing during the emergence of the fragments. These properties of the scission point are studied as functions of the fragment atomic number. The correlation between these observables, gathered in one single experiment and for two different fissioning systems at different excitation energies, give valuable information for the understanding and modeling of the fission process.

  18. Fiber optic calorimetry

    SciTech Connect

    Rudy, C.; Bayliss, S.; Bracken, D.; Bush, J.; Davis, P.

    1998-01-01

    A twin-bridge calorimeter using optical fiber as the sensor element was constructed and tested. This system demonstrates the principle and capability of using fiber for heat-flow measurements of special nuclear material. This calorimeter uses piezoelectric-generated phase-carrier modulation with subsequent electronic signal processing to allow phase shifts as small as 1 microradian ({mu}rad) to be measured. The sensing element consists of 21-m lengths of single-mode optical fiber wrapped around sample and reference chambers. The sensitivity of the calorimeter was determined to be 74 radians (rad) of phase shift per milliwatt of thermal power. One milliwatt of thermal power is equivalent to 400 mg of plutonium (6% {sup 240}Pu). The system noise base was about 0.2 rad, equivalent to about 1 mg of plutonium.

  19. Fiber Optic Calorimetry

    SciTech Connect

    Rudy, C.; Bayliss, S.; Bracken, D.; Bush, J.; Davis, P.

    1997-12-12

    A twin-bridge calorimeter using optical fiber as the sensor element was constructed and tested. This system demonstrates the principle and capability of using optical fibers for heat-flow measurements of special nuclear material. This calorimeter uses piezoelectric-generated phase-carrier modulation with subsequent electronic signal processes to allow phase shifts as small as 1 microradian ({micro}rad) to be measured. The sensing element consists of 21-m lengths of single-mode optical fiber wrapped around sample and reference chambers. The sensitivity of the calorimeter was determined to be 74 radians (rad) of phase shift per milliwatt of thermal power. One milliwatt of thermal power is equivalent to 400 mg of plutonium (6% {sup 240}Pu). The system noise base was about 0.2 rad, equivalent to about 1 mg of plutonium.

  20. 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

  1. Distribution of artificial radionuclides in lacustrine sediments in China.

    PubMed

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

    2011-07-01

    Establishing accurate historical records of the distribution, inventory and source of artificial radionuclides in the environment is important for environmental monitoring and radiological health protection due to their potential toxicity, and is also useful for identification and risk assessment of possible future environmental inputs of radionuclides from nuclear weapons tests and accidental release from the nuclear fuel reprocessing facilities or nuclear power reactors. A sector-field inductively coupled plasma mass spectrometer was used to study the recent sedimentation of Pu isotopes in 11 lakes in China. The distribution of (137)Cs was investigated using the conventional radiometric analytical methods. Based on the isotopic compositions of Pu and the activity ratio of (137)Cs/(239+240)Pu, the sources of artificial radionuclides were identified. The potential applications of Pu isotopes for sediment dating and for regional and global environmental change studies were discussed. PMID:21498412

  2. The design and implementation of the AVNG measurement system

    SciTech Connect

    Macarthur, Duncan W; Thron, Jonathan; Razinkov, Sergey; Livke, Alexander; Kondratov, Sergey

    2010-01-01

    An attribute measurement system (AMS) measures a number of unclassified attributes of potentially classified material. By displaying these unclassified results only as red or green lights, the AMS protects potentially classified information while still generating confidence in the measurement result. The AVNG that we describe is an AMS built by RFNC-VNIIEF in Sarov, Russia. The AVNG detects neutron and gamma radiation signatures and displays the three unclassified attributes of 'plutonium presence,' 'plutonium mass >2 kg,' and 'plutonium isotopic ratio ({sup 240}Pu to {sup 239}Pu) < 0.1.' In this presentation, we will describe the design of the AVNG neutron and gamma detector subsystems, as well as the design of the entire AMS incorporating these detectors. We will also describe the construction of the AVNG and the final design that was demonstrated in June 2009.

  3. Sources of plutonium in the atmosphere and stratosphere-troposphere mixing

    PubMed Central

    Hirose, Katsumi; Povinec, Pavel P.

    2015-01-01

    Plutonium isotopes have primarily been injected to the stratosphere by the atmospheric nuclear weapon tests and the burn-up of the SNAP-9A satellite. Here we show by using published data that the stratospheric plutonium exponentially decreased with apparent residence time of 1.5 ± 0.5 years, and that the temporal variations of plutonium in surface air followed the stratospheric trends until the early 1980s. In the 2000s, plutonium and its isotope ratios in the atmosphere varied dynamically, and sporadic high concentrations of 239,240Pu reported for the lower stratospheric and upper tropospheric aerosols may be due to environmental events such as the global dust outbreaks and biomass burning. PMID:26508010

  4. Interspecies comparison of the metabolism and dosimetry of inhaled mixed oxides of plutonium and uranium

    SciTech Connect

    Boecker, B.B.; Mewhinney, J.A.; Eidson, A.F.

    1997-12-01

    Three studies were conducted to provide information on the biological fate, distribution of radiation doses among tissues, and implications for potential health consequences of an inhalation exposure to mixed-oxide nuclear fuel materials. In each study, Fischer-344 rats, beagle dogs, and cynomolgus monkeys inhaled one of three aerosols: 750{degrees}C calcined mixed oxides of UO{sub 2} and PuO{sub 2}, 1750{degrees}C sintered (U,Pu)O{sub 2}, or 850{degrees}C calcined {open_quotes}pure{close_quotes} PuO{sub 2}. These materials were collected from glove-box enclosures immediately after industrial processing of mixed-oxide fuel materials. Lung retention, tissue distribution, and mode of excretion of {sup 238-240}Pu, {sup 241}Am, and uranium (when present) were quantified by radiochemical analysis of tissue and excreta samples from animals sacrificed at selected times to 6.5 yr after inhalation exposure.

  5. Recent advances in modeling fission cross sections over intermediate structures

    SciTech Connect

    Bouland, Olivier; Lynn, J. Eric; Talou, Patrick

    2009-01-01

    More accurate fission cross section calculations in presence of underlying intermediate structure are strongly desired. This paper recalls the common approximations used below the fission threshold and quantifies their impact. In particular, an exact expanded R-matrix Monte Carlo calculation of the intermediate structure, deeply mixed with the fluctuations of the class-I and II decay amplitudes, is shown. This paper also insists on the microscopic structure of the level densities as a function of the nucleus deformation and show preliminary neutron induced fission cross section calculations for {sup 239}Pu and {sup 240}Pu using newly calculated combinatorial level densities. Comparisons with recent evaluated and measured fission cross sections are made.

  6. 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.

  7. Improved precision and accuracy in quantifying plutonium isotope ratios by RIMS

    DOE PAGESBeta

    Isselhardt, B. H.; Savina, M. R.; Kucher, A.; Gates, S. D.; Knight, K. B.; Hutcheon, I. D.

    2015-09-01

    Resonance ionization mass spectrometry (RIMS) holds the promise of rapid, isobar-free quantification of actinide isotope ratios in as-received materials (i.e. not chemically purified). Recent progress in achieving this potential using two Pu test materials is presented. RIMS measurements were conducted multiple times over a period of two months on two different Pu solutions deposited on metal surfaces. Measurements were bracketed with a Pu isotopic standard, and yielded absolute accuracies of the measured 240Pu/239Pu ratios of 0.7% and 0.58%, with precisions (95% confidence intervals) of 1.49% and 0.91%. In conclusion, the minor isotope 238Pu was also quantified despite the presence ofmore » a significant quantity of 238U in the samples.« less

  8. Assessing radiation impact at a protected coastal sand dune site: an intercomparison of models for estimating the radiological exposure of non-human biota.

    PubMed

    Wood, Michael D; Beresford, Nicholas A; Barnett, Catherine L; Copplestone, David; Leah, Richard T

    2009-12-01

    This paper presents the application of three publicly available biota dose assessment models (the ERICA Tool, R&D128/SP1a and RESRAD-BIOTA) to an assessment of the Drigg coastal sand dunes. Using measured (90)Sr, (99)Tc, (137)Cs, (238)Pu, (239+240)Pu and (241)Am activity concentrations in sand dune soil, activity concentration and dose rate predictions are made for a range of organisms including amphibians, birds, invertebrates, mammals, reptiles, plants and fungi. Predicted biota activity concentrations are compared to measured data where available. The main source of variability in the model predictions is the transfer parameters used and it is concluded that developing the available transfer databases should be a focus of future research effort. The value of taking an informed user approach to investigate the way in which models may be expected to be applied in practice is highlighted and a strategy for the future development of intercomparison exercises is presented. PMID:19447531

  9. Radionuclide concentrations in fish and invertebrates from Bikini Atoll

    SciTech Connect

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

    1988-01-01

    As in other global studies, /sub 137/Cs was found in the highest concentrations in edible flesh of all species of fish and in the lowest concentrations in the bone or liver. The mean concentration of /sup 137/Cs in muscle of reef fish from the southern part of the atoll is comparable to the global-fallout concentration measured in market samples of fish collected from Chicago, IL, USA, in 1982. Strontium-90 is associated generally with non-edible parts of fish, such as bone or viscera. Twenty-five to fifty percent of the total body burden of /sub 60/Co is accumulated in the muscle tissue; the remainder is distributed among the liver, skin, and viscera. The mean concentration of /sub 60/Co in fish has been decreasing at a rate faster than radiological decay alone. Most striking is the range of /sup 207/Bi concentrations among different species of fish collected at the same time and place. Highest concentrations of /sup 207/Bi were consistently detected in the muscle and other tissues of goatfish and some of the pelagic lagoon fish. In other reef fish, such as mullet, surgeonfish, and parrotfish, /sub 207/Bi was usually below detection limits by gamma spectrometry. Over 70% of the whole-body activity of /sup 207/Bi in goatfish is associated with the muscle tissue, whereas less than 5% is found in the muscle of mullet and surgeonfish. Neither /sup 239 +240/Pu nor /sup 241/Am is accumulated significantly in the muscle tissue of any species of fish. Apparently, /sup 238/Pu is in a more readily available form for accumulation by fishes than /sup 239 +240/Pu. Based on a daily ingestion rate of 200 g of fish flesh, dose rates to individuals through the fish-food ingestion pathway are well below current Federal guidelines. 24 refs., 1 fig., 27 tabs

  10. 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.

  11. Tracing the origin of suspended sediment in a large Mediterranean river by combining continuous river monitoring and measurement of artificial and natural radionuclides.

    PubMed

    Zebracki, Mathilde; Eyrolle-Boyer, Frédérique; Evrard, Olivier; Claval, David; Mourier, Brice; Gairoard, Stéphanie; Cagnat, Xavier; Antonelli, Christelle

    2015-01-01

    Delivery of suspended sediment from large rivers to marine environments has important environmental impacts on coastal zones. In France, the Rhone River (catchment area of 98,000 km(2)) is by far the main supplier of sediment to the Mediterranean Sea and its annual solid discharge is largely controlled by flood events. This study investigates the relevance of alternative and original fingerprinting techniques based on the relative abundances of a series of radionuclides measured routinely at the Rhone River outlet to quantify the relative contribution of sediment supplied by the main tributaries during floods. Floods were classified according to the relative contribution of the main subcatchments (i.e., Oceanic, Cevenol, extensive Mediterranean and generalised). Between 2000 and 2012, 221 samples of suspended sediment were collected at the outlet and were shown to be representative of all flood types that occurred during the last decade. Three geogenic radionuclides (i.e., (238)U, (232)Th and (40)K) were used as fingerprints in a multivariate mixing model in order to estimate the relative contribution of the main subcatchment sources-characterised by different lithologies-in sediment samples collected at the outlet. Results showed that total sediment supply originating from Pre-Alpine, Upstream, and Cevenol sources amounted to 10, 7 and 2.10(6)tons, respectively. These results highlight the role of Pre-Alpine tributaries as the main sediment supplier (53%) to the Rhone River during floods. Other fingerprinting approaches based on artificial radionuclide activity ratios (i.e., (137)Cs/(239+240)Pu and (238)Pu/(239+240)Pu) were tested and provided a way to quantify sediment remobilisation or the relative contributions of the southern tributaries. In the future, fingerprinting methods based on natural radionuclides should be further applied to catchments with heterogeneous lithologies. Methods based on artificial radionuclides should be further applied to catchments

  12. Isotopic Pu, Am and Cm signatures in environmental samples contaminated by the Fukushima Dai-ichi Nuclear Power Plant accident.

    PubMed

    Yamamoto, M; Sakaguchi, A; Ochiai, S; Takada, T; Hamataka, K; Murakami, T; Nagao, S

    2014-06-01

    Dust samples from the sides of roads (black substances) have been collected together with litter and soil samples at more than 100 sites contaminated heavily in the 20-km exclusion zones around Fukushima Dai-ichi Nuclear Power Plant (FDNPP) (Minamisoma City, and Namie, Futaba and Okuma Towns), in Iitate Village located from 25 to 45 km northwest of the plant and in southern areas from the plant. Isotopes of Pu, Am and Cm have been measured in the samples to evaluate their total releases into the environment from the FDNPP and to get the isotopic compositions among these nuclides. For black substances and litter samples, in addition to Pu isotopes, (241)Am, (242)Cm and (243,244)Cm were determined for most of samples examined, while for soil samples, only Pu isotopes were determined. The results provided a coherent data set on (239,240)Pu inventories and isotopic composition among these transuranic nuclides. When these activity ratios were compared with those for fuel core inventories in the FDNPP accident estimated by a group at JAEA, except (239,240)Pu/(137)Cs activity ratios, fairly good agreements were found, indicating that transuranic nuclides, probably in the forms of fine particles, were released into the environment without their large fractionations. The obtained data may lead to more accurate information about the on-site situation (e.g., burn-up, conditions of fuel during the release phase, etc.), which would be difficult to get otherwise, and more detailed information on the dispersion and deposition processes of transuranic nuclides and the behavior of these nuclides in the environment. PMID:24531259

  13. Tracer-level radioactive pilot-scale test of in situ vitrification for the stabilization of contaminated soil sites at ORNL

    SciTech Connect

    Spalding, B.P.; Jacobs, G.K.; Naney, M.T.; Dunbar, N.W.; Tixier, J.S.; Powell, T.D.

    1992-11-01

    A field demonstration of in situ vitrification (ISV) was completed in May 1991, and produced approximately 12 Mg of melted earthen materials containing 12.7 mCi of radioactivity within 500 g of sludge in amodel of an old seepage trench waste disposal unit. Past waste disposal operations at Oak Ridge National Laboratory have left several contaminated seepage sites. In planning for remediation of such sites, ISV technology has been identified as a leading candidate because of the high risks associated with any retrieval option and because of the usual high quality of vitreous waste form. Major isotopes placed in the test trench were {sup 137}Cs and {sup 90}Sr, with lesser amounts of {sup 6O}Co, {sup 241}Am, and {sup 239,240}Pu. A total of 29 MWh of electrical power was delivered to the ground over a 5-day period producing a melt depth of 8.5 ft. During melting, 2.4% of the {sup 137}Cs volatilized from the melt into an off-gas containment hood and was captured quantitatively on a high efficiency particulate air filter. No volatilization of {sup 90}Sr, {sup 241}Am, or {sup 239,240}Pu was detected and > 99.993% retention of these isotopes in the melt was estimated. The use of added rare earth tracers (Ce, La, and Nd), as surrogates for transuranic isotopes, led to estimated melt retentions of >99.9995% during the test. The molten material, composed of the native soil and dolomitic limestone used for filling the test trench, reached a processing temperature of 1500{degrees}C. Standardized leaching procedures using Product Consistency Testing indicated that the ISV product has excellent characteristics relative to other vitreous nuclear waste forms.

  14. Systematic effects in neutron coincidence and multiplicity counting

    SciTech Connect

    Evans, Louise G; Favorite, Jeffrey A; Swinhoe, Martyn T

    2010-01-01

    Correlated neutron counting, including neutron coincidence and multiplicity counting, is an important tool in nuclear material accountancy verification. The accuracy of such measurements is of interest to the safeguards community because as the accuracy of NDA improves, the number of samples that are required to undergo destructive analysis (DA) decreases. The accuracy of a neutron mUltiplicity measurement can be affected by a number of variables. Monte Carlo neutron transport simulations with MCNPX have been performed to understand how the properties of the sample affect the count rate. These resultant count rates have been analyzed with the 'point model' in order to determine the effect on the deduced plutonium mass. The sample properties that have been investigated are density, sample position within the detector cavity, moisture content, isotopic composition, plutonium to total actinide ratio and heavy metal fraction. These parameters affect the Singles, Doubles and Triples count rates in different ways. In addition, different analysis methods use these measured quantities in different combinations, so that the final sensitivity of the {sup 240}Pu mass to each parameter also depends on the analysis method used. For example, the passive calibration curve method only used the Doubles rate to produce the {sup 240}Pu mass and so is not sensitive to changes in the Singles rate (to first order). The analysis methods considered here were passive calibration curve (non-multiplication corrected), known alpha (multiplication corrected) and multiplicity with known efficiency. The effects were studied on both a small mass MOX sample (1 g Pu) and a large MOX sample (6000 g Pu) both measured in high efficiency neutron multiplicity counters. In order to determine the final effect of each parameter it is necessary to know not only the sensitivity of the plutonium mass to that parameter, but also the range over which the parameter can realistically vary. Some estimates are

  15. Territory contamination with the radionuclides representing the fuel component of Chernobyl fallout.

    PubMed

    Kashparov, V A; Lundin, S M; Zvarych, S I; Yoshchenko, V I; Levchuk, S E; Khomutinin, Y V; Maloshtan, I M; Protsak, V P

    2003-12-30

    The data obtained through a series of experiments were used to specify the correlation of activities of the fuel component radionuclides of Chernobyl fallout and to create the maps of the 30-km Chernobyl zone terrestrial density of contamination with 154Eu, 238Pu, 239+240Pu and 241Am (on 01.01.2000). In the year 2000, total inventories of the fuel component radionuclides in the upper 30-cm soil layer of the 30-km Chernobyl zone in Ukraine (outside the ChNPP industrial site, excluding the activity located in the radioactive waste storages and in the cooling pond) were estimated as: 90Sr--7.7 x 10(14) Bq; 137Cs--2.8 x 10(15) Bq; 154Eu--1.4 x 10(13) Bq; 238Pu--7.2 x 10(12) Bq; 239+240Pu--1.5 x 10(13) Bq; 241Am--1.8 x 10(13) Bq. These values correspond to 0.4-0.5% of their amounts in the ChNPP unit 4 at the moment of the accident. The current estimate is 3 times lower than the previous widely-cited estimates. Inventories of the fuel component radionuclides were also estimated in other objects within the 30-km zone and outside it. This allowed more accurate data to be obtained on the magnitude of a relative release of radionuclides in the fuel particles (FP) matrix during the Chernobyl accident outside the ChNPP industrial site. It amounts to 1.5+/-0.5% of these radionuclides in the reactor, which is 2 times lower than the previous estimates. Two-thirds of the radionuclides release in the FP was deposited on the territory of Ukraine. PMID:14630415

  16. Radioactive aerosols released from the Chernobyl Shelter into the immediate environment.

    PubMed

    Garger, E K; Kashpur, V A; Li, W B; Tschiersch, J

    2006-07-01

    The release of radioactive particles through large gaps in the containment of the destroyed Chernobyl reactor was assessed during two measurement periods. In 1996-1999, a total radionuclide flow rate of 274 Bq s(-1) or 8.64 x 10(9) Bq year(-1) was determined. These releases were predominantly due to (137)Cs (78.5%), (90)Sr (21.1%), and (239+240)Pu (0.4%). The mean activity concentration in the aerosol measured directly at the gaps was about 240 mBq m(-3) with an activity median aerodynamic diameter (AMAD) of 2.4 microm for (137)Cs, 120 mBq m(-3) with an AMAD in the range 3.1-13 microm for (90)Sr, 1.8 mBq m(-3) with an AMAD in the range 3.5-11 microm for (239+240)Pu, and 2.0 mBq m(-3) with an AMAD of 1.5 microm for (241)Am. The resulting total inhalation dose rate calculated close to the gaps was about 100 nSv h(-1). In the near environment, the mean (137)Cs activity in the aerosol was 2.2 mBq m(-3) with an AMAD of 2.2 microm, which gave rise to an inhalation dose rate of about two orders of magnitude lower than the corresponding dose rate at the gaps. Occasionally, however, dose levels were measured in the near environment that were similar to those at the gaps. In 2000-2003, lower activity concentrations were observed. The decrease was more pronounced at the gaps than in the near environment. The results indicate that effective dose due to inhalation must be considered for the dose assessment of construction workers who will be deployed at the Chernobyl site to reconstruct the old or to build the new Shelter, in the future. PMID:16733725

  17. Radioactive substances in tap water.

    PubMed

    Atsuumi, Ryo; Endo, Yoshihiko; Suzuki, Akihiko; Kannotou, Yasumitu; Nakada, Masahiro; Yabuuchi, Reiko

    2014-01-01

    A 9.0 magnitude (M) earthquake with an epicenter off the Sanriku coast occurred at 14: 46 on March 11, 2011. TEPCO Fukushima Daiichi Nuclear Power Plant (F-1 NPP) was struck by the earthquake and its resulting tsunami. Consequently a critical nuclear disaster developed, as a large quantity of radioactive materials was released due to a hydrogen blast. On March 16(th), 2011, radioiodine and radioactive cesium were detected at levels of 177 Bq/kg and 58 Bq/kg, respectively, in tap water in Fukushima city (about 62km northwest of TEPCO F-1 NPP). On March 20th, radioiodine was detected in tap water at a level of 965 Bq/kg, which is over the value-index of restrictions on food and drink intake (radioiodine 300 Bq/kg (infant intake 100 Bq/kg)) designated by the Nuclear Safety Commission. Therefore, intake restriction measures were taken regarding drinking water. After that, although the all intake restrictions were lifted, in order to confirm the safety of tap water, an inspection system was established to monitor all tap water in the prefecture. This system has confirmed that there has been no detection of radioiodine or radioactive cesium in tap water in the prefecture since May 5(th), 2011. Furthermore, radioactive strontium ((89) Sr, (90)Sr) and plutonium ((238)Pu, (239)Pu+(240)Pu) in tap water and the raw water supply were measured. As a result, (89) Sr, (238)Pu, (239)Pu+(240)Pu were undetectable and although (90)Sr was detected, its committed effective dose of 0.00017 mSv was much lower than the yearly 0.1 mSv of the World Health Organization guidelines for drinking water quality. In addition, the results did not show any deviations from past inspection results. PMID:25030724

  18. Particle count monitoring of reverse osmosis water treatment for removal of low-level radionuclides

    SciTech Connect

    Moritz, E.J.; Hoffman, C.R.; Hergert, T.R.

    1995-03-01

    Laser diode particle counting technology and analytical measurements were used to evaluate a pilot-scale reverse osmosis (RO) water treatment system for removal of particulate matter and sub-picocurie low-level radionuclides. Stormwater mixed with Waste Water Treatment Plant (WWTP) effluent from the Rocky Flats Environmental Technology Site (RFETS), formerly a Department of Energy (DOE) nuclear weapons production facility, were treated. No chemical pretreatment of the water was utilized during this study. The treatment system was staged as follows: multimedia filtration, granular activated carbon adsorption, hollow tube ultrafiltration, and reverse osmosis membrane filtration. Various recovery rates and two RO membrane models were tested. Analytical measurements included total suspended solids (TSS), total dissolved solids (TDS), gross alpha ({alpha}) and gross beta ({beta}) activity, uranium isotopes {sup 233/234}U and {sup 238}U, plutonium {sup 239/240}Pu, and americium {sup 241}Am. Particle measurement between 1--150 microns ({mu}) included differential particle counts (DPC), and total particle counts (TPC) before and after treatment at various sampling points throughout the test. Performance testing showed this treatment system produced a high quality effluent in clarity and purity. Compared to raw water levels, TSS was reduced to below detection of 5 milligrams per liter (mg/L) and TDS reduced by 98%. Gross {alpha} was essentially removed 100%, and gross {beta} was reduced an average of 94%. Uranium activity was reduced by 99%. TPC between 1-150{mu} were reduced by an average 99.8% to less than 1,000 counts per milliliter (mL), similar in purity to a good drinking water treatment plant. Raw water levels of {sup 239/240}Pu and {sup 241}Am were below reliable quantitation limits and thus no removal efficiencies could be determined for these species.

  19. Isotopic fingerprinting of the world's first nuclear device using post-detonation materials.

    PubMed

    Bellucci, Jeremy J; Simonetti, Antonio; Wallace, Christine; Koeman, Elizabeth C; Burns, Peter C

    2013-04-16

    In the event of a rogue nuclear attack or interception of illicit nuclear materials, timely forensic investigations are critical for accurate source attribution. Uranium (U) and plutonium (Pu) isotopic ratios of intercepted materials or postdetonation samples are, perhaps, the most valuable evidence in modern nuclear forensics. These ratios simultaneously provide information regarding the material's ''age'' (i.e., time elapsed since last purification), actinide concentrations, and relevant isotopic ratios/enrichment values. Consequently, these isotope signatures are invaluable in determining the origin, processing history, and intended purpose of any nuclear material. Here we show, for the first time, that it is feasible to determine the U and Pu isotopic compositions of historic nuclear devices from their postdetonation materials utilizing in situ U isotopic measurements. The U isotopic compositions of trinitite glass, produced subsequent to the world's first atomic explosion, indicate two sources: the device's tamper, composed of natural U that underwent fission during detonation, and natural U from the geological background. Enrichments in (234,235,236)U reflect the in situ decay of (238,239,240)Pu, the fuel used in the device. Time-integrated U isotopic modeling yields "supergrade" compositions, where (240)Pu/(239)Pu ≈ 0.01-0.03 and (238)Pu/(239)Pu ≈ 0.00011-0.00017, which are consistent with the Pu originating from the Hanford reactor. Spatially resolved U isotopic data of postdetonation debris reveal important details of the device in a relatively short time frame (hours). This capacity serves as an important deterrent to future nuclear threats and/or terrorist activities and is critical for source attribution and international security. PMID:23517046

  20. Risk assessment of soil-based exposures to plutonium at experimental sites located on the Nevada Test Site and adjoining areas

    SciTech Connect

    Layton, D.W.; Anspaugh, L.R.; Bogen, K.T.; Straume, T.

    1993-06-01

    In the late 1950s and early 1960s, a series of tests was conducted at or near the Nevada Test Site to study issues involving plutonium-bearing devices. These tests resulted in the dispersal of about 5 TBq of {sup 239,240}Pu on the surficial soils at the test locations. Access to the sites is strictly controlled; therefore, it does not constitute a threat to human health at the present time. However, because the residual {sup 239} Pu decays slowly (half-life of 24,110 y), the sites could indeed represent a long-term hazard if they are not remediated and if institutional controls are lost. To investigate the magnitude of the potential health risks for this no-remediation case, we defined three basic exposure scenarios that could bring individuals in contact with {sup 239,240}Pu at the sites: (1) a resident living in a subdivision located at a test site, (2) a resident farmer, and (3) a worker at a commercial facility. Our screening analyses indicated that doses to organs are dominated by the intemal deposition of Pu via the inhalation pathway, and thus our risk assessment focused on those factors that affect inhalation exposures and associated doses, including inhalation rates, activity patterns, tenure at a residence or occupation, indoor/outdoor air relationships, and resuspension outdoors. Cancer risks were calculated as a function of lifetime cumulative doses to the key target organs (i.e., bone surface, liver, and lungs) and risk factors for those organs. Uncertainties in the predicted cancer risks were analyzed using Monte-Carlo simulations of the probability distributions used to represent assessment parameters. The principal sources of uncertainty in the estimated risks were population mobility, the relationship between indoor and outdoor contaminant levels, and the dose and risk factors for bone, liver, and lung.

  1. Variability in background levels of surface soil radionuclides in the vicinity of the US DOE waste isolation pilot plant.

    PubMed

    Kirchner, T B; Webb, J L; Webb, S B; Arimoto, R; Schoep, D A; Stewart, B D

    2002-01-01

    Concentrations of radionuclides were measured in soils from a grid of locations surrounding the US Department of Energy Waste Isolation Pilot Plant (WIPP) in southeastern New Mexico and from a grid on a reference site approximately 20 km southeast of the WIPP site. Each of the two grids has 16 sampling locations (grid nodes) systematically distributed within an area of 16.580 ha. Sampling was conducted prior to the arrival of the first waste shipment at WIPP. Thus, the 137Cs and 23,240Pu in the soil are expected to have been deposited as global fallout, although the Gnome Site, 8.8 km southwest of the WIPP, is also a potential source of 239,240Pu and fission products. The reference grid has significantly higher concentrations of fallout and natural radionuclides than the WIPP grid. Up to 80% of the total variability in radionuclide concentrations across the two grids is attributable to differences between grid nodes. Differences between replicates within a location account for 44-50% of the variability in concentrations of the uranium isotopes, but only 11-17% of the variability in the concentrations of the other radionuclides. Samples having similar abundance of radionuclides were spatially aggregated across the terrain. The activity concentrations of the radionuclides were strongly correlated with the concentrations of Al and Pb, and with the percentages of sand, silt and clay in the soil. Normalizing radionuclide concentrations to the concentration of Al or percent fine particles can help adjust for differences in soil textures among samples and facilitate the detection of gradients or temporal changes in soil concentrations. PMID:12054041

  2. LONG-TERM DYNAMICS OF RADIONUCLIDE VERTICAL MIGRATION IN SOILS OF THE CHERNOBYL NUCLEAR POWER PLANT EXCLUSION ZONE

    SciTech Connect

    Farfan, E

    2009-11-19

    The radioactive fallout from the Chernobyl Nuclear Power Plant (ChNPP) accident consisted of fuel and condensation components. An important radioecological task associated with the late phase of the accident is to evaluate the dynamics of radionuclide mobility in soils. Identification of the variability (or invariability) in the radionuclide transfer parameters makes it possible to (1) accurately predict migration patterns and biological availability of radionuclides and (2) evaluate long-term exposure trends for the population who may reoccupy the remediated abandoned areas. In 1986-1987, a number of experimental plots were established within various tracts of the fallout plume to assist with the determination of the long-term dynamics of radionuclide vertical migration in the soils. The transfer parameters for {sup 137}Cs, {sup 90}Sr, and {sup 239,240}Pu in the soil profile, as well as their ecological half-time of the radionuclide residence (T{sub 1/2}{sup ecol}) values in the upper 5-cm thick soil layers of different grasslands were estimated at various times since the accident. Migration characteristics in the grassland soils tend to decrease as follows: {sup 90}Sr > {sup 137}Cs {ge} {sup 239,240}Pu. It was found that the {sup 137}Cs absolute T{sub 1/2}{sup ecol} values are 3-7 times higher than its radioactive decay half-life value. Therefore, changes in the exposure dose resulting from the soil deposited {sup 137}Cs now depend only on its radioactive decay. The {sup 90}Sr T{sub 1/2}{sup ecol} values for the 21st year after the fallout tend to decrease, indicating an intensification of its migration capabilities. This trend appears consistent with a pool of mobile {sup 90}Sr forms that grows over time due to destruction of the fuel particles.

  3. Nevada test site radionuclide inventory and distribution program: Report number 4, Areas 18 and 20

    SciTech Connect

    McArthur, R D; Mead, S W

    1988-04-01

    As part of the Radionuclide Inventory and Distribution Program on the Nevada Test Site, in situ measurements of gamma-emitting radionuclides were made at more than 600 locations in six regions near ground zeros in Areas 18 and 20. In addition, several soil samples were collected from each region and analyzed to determine inverse relaxation lengths and radionuclide ratios. Analysis of the data from Area 20 led to estimated inventories of 23 Ci of /sup 241/Am, 30 Ci of /sup 238/Pu, 41 Ci of /sup 239,240/Pu, 18 Ci of /sup 60/Co, 6.4 Ci of /sup 137/Cs, 6.0 Ci of /sup 90/Sr, 17 Ci of /sup 152/Eu, 19 Ci of /sup 154/Eu, and 6.6 Ci of /sup 155/Eu. For Area 18, the estimated inventories were 27 Ci of /sup 241/Am, 4.9 Ci of /sup 238/Pu, 150 Ci of /sup 239,240/Pu, 1.3 Ci of /sup 60/Co, 4.9 Ci of /sup 137/Cs, 13 Ci of /sup 90/Sr, 2.1 Ci of /sup 152/Eu, 1.3 Ci of /sup 154/Eu, and 1.4 Ci of /sup 155/Eu. The locations of the measurements in Area 18 were chosen by importance sampling, which permits the calculation of an estimate of the sampling error. Maps of radionuclide distributions were also generated for all regions except the area near the Palanquin and Cabriolet ground zeros. 3 refs., 65 figs., 7 tabs.

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

    SciTech Connect

    Robert C. Roback; Don L. Koeppen

    2003-06-01

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

  5. Late Holocene Climate Change Inferred From Varved Proglacial Lake Sediments on Northeastern Baffin Island, Arctic Canada

    NASA Astrophysics Data System (ADS)

    Thomas, E. K.; Briner, J. P.; Axford, Y.

    2007-12-01

    The Arctic has a disproportionately large response to changes in radiative forcing of climate, and glaciers and arctic lacustrine ecosystems respond sensitively to these changes. Lacustrine ecosystems throughout the Arctic are undergoing rapid regime shifts, including dramatically increased primary productivity and changing aquatic floral and faunal assemblages. Our work on organic lake sediments from northeast Baffin Island shows a large increase in primary productivity, changes in insect (Chironomidae) assemblages including the disappearance of cold stenotherms, and a rise in chironomid-inferred summer water temperatures of at least 1.5°C over the past 50 years, reaching temperatures that were unprecedented in the past 5000 years. Here, we pursue the use of varve thickness, an abiotic temperature proxy, to expand our understanding of late Holocene temperature changes on northeast Baffin Island. We obtained a 14C- and 239+240Pu-dated surface core/percussion core pair from a proglacial lake. Together these cores span > 8000 years and the sediments are varved, as verified by the 239+240Pu analysis, for at least the past 700 years. Magnetic susceptibility was high during the early Holocene, decreased to near-zero values during the mid-Holocene and increased during the past 2500 years to reach the highest values seen in the record around 1000 years ago. Loss-on- ignition had an opposite trend, with the highest values in the mid-Holocene. Sedimentation rate was constant during most of the Holocene (0.03 cm yr -1) and increased during the past 1000 years to 0.05 cm yr -1. These parameters indicate that following the absence of an active glacier during the middle Holocene, glacier activity initiated ~2500 years ago and reached peak activity over the last 1000 years. Our ongoing work to obtain a varve-thickness record for at least the last 700 years, and its calibration to a nearby weather station, will be presented.

  6. Radionuclide Concentrations in soils an Vegetation at Low-Level Radioactive Waste Disposal Area G During 2004

    SciTech Connect

    P.R. Fresquez; E.A. Lopez

    2004-11-01

    Soil samples were collected at 15 locations and unwashed overstory and understory vegetation samples were collected at nine locations within and around the perimeter of Area G, the primary disposal facility for low-level radioactive solid waste at Los Alamos National Laboratory (LANL). These samples were analyzed for {sup 3}H, {sup 238}Pu, {sup 239,240}Pu, {sup 90}Sr, {sup 241}Am, {sup 137}Cs, {sup 234}U, {sup 235}U, and {sup 238}U. Soil samples collected at Area G contained detectable concentrations of 3H (27%), {sup 239,240}Pu (60%), {sup 238}Pu (40%), and {sup 241}Am (47%) above regional statistical reference levels (RSRLs). In contrast, the levels of {sup 137}Cs, {sup 90}Sr, and U in all of the soil samples at Area G were either nondetectable or within RSRLs. The highest levels of {sup 3}H in soils were detected in the southwestern portion of Area G near the {sup 3}H shafts, whereas the highest concentrations of the Pu isotopes were detected in the northern and northeastern portions. All concentrations of {sup 3}H and Pu in soils, however, were far below LANL screening action levels. As for vegetation, most radionuclides in/on plants were either nondetectable or within RSRLs. The exceptions were {sup 3}H in overstory and some understory vegetation, particularly in the southwestern portion of Area G, which correlated very well with the soils data in that area. Also, there was some foliar contamination from {sup 241}Am and Pu isotopes in/on a few plant samples--the highest concentrations occurring in the northern section of Area G.

  7. The Northern Marshall Islands radiological survey: Data and dose assessments

    SciTech Connect

    Robison, W.L.; Noshkin, V.E.; Conrado, C.L.

    1997-07-01

    Fallout from atmospheric nuclear tests, especially from those conducted at the Pacific Proving Grounds between 1946 and 1958, contaminated areas of the Northern Marshall Islands. A radiological survey at some Northern Marshall Islands was conducted from September through November 1978 to evaluate the extent of residual radioactive contamination. The atolls included in the Northern Marshall Islands Radiological Survey (NMIRS) were Likiep, Ailuk, Utirik, Wotho, Ujelang, Taka, Rongelap, Rongerik, Bikar, Ailinginae, and Mejit and Jemo Islands. The original test sites, Bikini and Enewetak Atolls, were also visited on the survey. An aerial survey was conducted to determine the external gamma exposure rate. Terrestrial (soil, food crops, animals, and native vegetation), cistern and well water samples, and marine (sediment, seawater, fish and clams) samples were collected to evaluate radionuclide concentrations in the atoll environment. Samples were processed and analyzed for {sup 137}Cs, {sup 90}Sr, {sup 239+240}Pu and {sup 241}Am. The dose from the ingestion pathway was calculated using the radionuclide concentration data and a diet model for local food, marine, and water consumption. The ingestion pathway contributes 70% to 90% of the estimated dose. Approximately 95% of the dose is from {sup 137}Cs accounts for about 10% to 30% of the dose. {sup 239+240}Pu and {sup 241}Am are the major contributors to dose via the inhalation pathway; however, inhalation accounts for only about 1% of the total estimated dose, based on surface soil levels and resuspension studies. All doses are computed for concentrations decay corrected to 1996. The maximum annual effective dose from manmade radionuclides at these atolls ranges from .02 mSv y{sup -1}. The background dose in the Marshall Islands is estimated to be 2.4 mSv y{sup -1} to 4.5 mSv y{sup -1}. The 50-y integral dose ranges from 0.5 to 65 mSv. 35 refs., 2 figs., 9 tabs.

  8. 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.

  9. Plutonium and tritium produced in the Hanford Site production reactors

    SciTech Connect

    Roblyer, S.P.

    1994-09-28

    In a news release on December 7, 1993, the Secretary of Energy announced declassification action that included totals for plutonium and tritium production in the Hanford Site production reactors. This information was reported as being preliminary because it was not fully supported by documentation. Subsequently, production data were made available from the US Department of Energy-Headquarters (DOE-HQ) records that indicated an increase of about one and one-half metric tons in total plutonium production. The Westinghouse Hanford Company was tasked by the US Department of Energy-Richland Operations Office to substantiate production figures and DOE-HQ data and to provide a defensible report of weapons- (6 wt% {sup 240}Pu) and nonweapons- (fuels-)grade (nominally 9 wt% or higher {sup 240}Pu) plutonium and tritium production in the Hanford Site production reactors. The task was divided into three parts. The first part was to determine plutonium and tritium production based on available reported accountability records. The second part was to determine plutonium production independently by calculational checks based on reactor thermal power generation and plutonium conversion factors representing the various reactor fuels. The third part was to resolve differences, if they occurred, in the reported and calculational results. In summary, the DOE-HQ-reported accountability records of plutonium and tritium production were determined to be the most defensible record of Hanford Site reactor production. The DOE-HQ records were consistently supported by the independent calculational checks and the records of operational data. Total production quantities are 67.4 MT total plutonium, which includes 12.9 MT of nonweapons-grade plutonium. The total tritium production was 10.6 kg.

  10. The Concentration of (236)Pu Daughters in Plutonium for Application to MOX Production from Plutonium from Dismantled US Nuclear Weapons

    SciTech Connect

    Sampson, T.E.; Cremers, T.L.

    2001-05-01

    The isotope {sup 236}Pu in the weapons-grade plutonium to be used in the US MOX (mixed-oxide) plant is of concern because the daughter products of {sup 236}Pu are sources of high-energy gamma rays. The {sup 208}Tl daughter of {sup 236}Pu emits intense, high-energy gamma rays that are important for radiation exposure calculations for plant design. It is generally thought that the concentrations of {sup 236}Pu and its daughters are well below 10{sup {minus}10}, but these concentrations are generally below the detection limits of most analytical techniques. One technique that can be used to determine the concentration {sup 208}Tl is the direct measurement of the intensity of the {sup 208}Tl gamma rays in the gamma-ray spectrum from plutonium. Thallium-208 will be in equilibrium with {sup 228}Th, and may very well be in equilibrium with {sup 232}U for most aged plutonium samples. We have used the FRAM isotopic analysis software to analyze dozens of archived high-resolution gamma ray spectra from various samples of US and foreign plutonium. We are able to quantify the ratio of minor isotopes with measurable gamma-ray emissions to the major isotope of plutonium and hence, through the measurement of the plutonium isotopic distribution of the sample, to elemental plutonium itself. Excluding items packaged in fluoropolymer vials, all samples analyzed with {sup 240}Pu < 9% gave {sup 228}Th/Pu ratios < 3.4 e-012 and all samples of US-produced plutonium, including {sup 240}Pu values up to 16.4%, gave {sup 228}Th/Pu ratios < 9.4 e-012. None of these values is significant from a radiation dose standpoint.

  11. Pairing-induced speedup of nuclear spontaneous fission

    DOE PAGESBeta

    Sadhukhan, Jhilam; Dobaczewski, J.; Nazarewicz, W.; Sheikh, J. A.; Baran, A.

    2014-12-22

    Collective inertia is strongly influenced at the level crossing at which the quantum system changes its microscopic configuration diabatically. Pairing correlations tend to make the large-amplitude nuclear collective motion more adiabatic by reducing the effect of these configuration changes. Competition between pairing and level crossing is thus expected to have a profound impact on spontaneous fission lifetimes. To elucidate the role of nucleonic pairing on spontaneous fission, we study the dynamic fission trajectories of 264Fm and 240Pu using the state-of-the-art self-consistent framework. We employ the superfluid nuclear density functional theory with the Skyrme energy density functional SkM* and a density-dependentmore » pairing interaction. Along with shape variables, proton and neutron pairing correlations are taken as collective coordinates. The collective inertia tensor is calculated within the nonperturbative cranking approximation. The fission paths are obtained by using the least action principle in a four-dimensional collective space of shape and pairing coordinates. Pairing correlations are enhanced along the minimum-action fission path. For the symmetric fission of 264Fm, where the effect of triaxiality on the fission barrier is large, the geometry of the fission pathway in the space of the shape degrees of freedom is weakly impacted by pairing. This is not the case for 240Pu, where pairing fluctuations restore the axial symmetry of the dynamic fission trajectory. The minimum-action fission path is strongly impacted by nucleonic pairing. In some cases, the dynamical coupling between shape and pairing degrees of freedom can lead to a dramatic departure from the static picture. As a result, in the dynamical description of nuclear fission, particle-particle correlations should be considered on the same footing as those associated with shape degrees of freedom.« less

  12. Study of radioactive isotopes of beryllium, polonium, uranium, and plutonium in the atmosphere

    SciTech Connect

    Lee, S.C.

    1986-01-01

    Radiochemical measurements were carried out for /sup 239.240/Pu in a total of 94 rain and snow samples collected at Fayetteville (36/sup 0/ N, 94/sup 0/W), Arkansas, during the period between May 1983 and November 1985. The concentrations of /sup 7/Be in most of these samples were also measured and these results were compared with previous samples. Average concentrations of cosmic-ray-produced radionuclide /sup 7/Be in rain remained fairly constant year after year. The annual rate of /sup 7/Be deposition at Fayetteville, Arkansas, was calculated from these data to be 5.2 dpm/cm/sup 2//year, which corresponds to a value of 2.8 x 10/sup -2/ atoms/cm/sup 2//second for the /sup 7/Be production rate in the atmosphere. The concentrations of bomb-produced radionuclides such as /sup 89/Sr, /sup 90/Sr and /sup 239.240/Pu in rain have drastically decreased since the last nuclear test explosion was conducted by the government of People's Republic of China in 1980. The concentrations of uranium isotopes and radon daughters in rain, on the other hand, were found to be affected by atmospheric injections of volcanic ashes from the 1980 eruption of Mount St. Helens and the 1982 eruption of El Chichon volcano in Mexico. Moreover, the burnups of the nuclear-powered Soviet satellites have caused marked increases in the levels of /sup 235/U and /sup 234/U in some of the rain samples. A sharp increase in the /sup 210/Po//sup 7/Be ratio in rain samples collected toward the end of 1980 and the beginning of 1981 was attributed to an atmospheric injection of /sup 210/Po from a series of major eruptions of Mount St. Helens.

  13. Radionuclide concentrations in terrestrial vegetation and soil on and around the Hanford Site, 1983 through 1993

    SciTech Connect

    Poston, T.M.; Antonio, E.J.; Cooper, A.T.

    1995-08-01

    This report reviews concentrations of {sup 60}Co, {sup 90}Sr, {sup 137}Cs, U isotopes, {sup 238}Pu, {sup 239,240}Pu, and {sup 241}Am in soil and vegetation samples collected from 1983 through 1993 during routine surveillance of the Hanford Site. Sampling locations were grouped in study areas associated with operational areas on the Site. While radionuclide concentrations were very low and representative of background concentrations from historic fallout, some study areas on the Site contained slightly elevated concentrations compared to other study areas onsite and offsite. The 100 Areas had concentrations of {sup 60}Co comparable to the minimum detectable concentration of 0.02 pCi/g in soil. Concentrations of {sup 90}Sr, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu, and {sup 241}Am in 200 Area soils were slightly elevated. The 300 Area had a slight elevation of U in soil. These observations were expected because many of the sampling locations were selected to monitor specific facilities or operations at the operational areas. Generally, concentrations of the radionuclides studied were greater and more readily measured in soil samples compared to vegetation samples. The general pattern of concentrations of radionuclide concentrations in vegetation by area mirrored that observed in soil. Declines in {sup 90}Sr in soil appear to be attributed to radioactive decay and possibly downward migration out of the sampling horizon. The other radionuclides addressed in this report strongly sorb to soil and are readily retained in surface soil. Because of their long half-lives compared to the length of the study period, there was no significant indication that concentrations of U isotopes and Pu isotopes were decreasing over time.

  14. A Discordancy Between Short-Term Sedimentation Rate Using Pb-210, Cs-137 and Pu and Long-Term Sedimentation Rate Using C-14

    NASA Astrophysics Data System (ADS)

    Baskaran, M.; Filley, T. R.; Bianchi, T. S.; Freeman, K. H.; Hatcher, P. G.

    2005-12-01

    Short-lived radionuclides (210Pb, 137Cs, etc) have been successfully utilized to obtain sedimentation rates in freshwater and coastal marine environments over the past 3 decades. Combined use of 210Pb and Pu enable to delineate sedimentation from sediment mixing. However independent validation of short-term accumulation rates using other long-lived isotopes, such as 14C are very limited. We collected a sediment core from a sinkhole lake, Mud Lake, Florida, USA and analyzed it for 210Pb, 137Cs, 239,240Pu and 14C. The sediment inventories of 137Cs, and 239,240Pu are comparable to the regional global fallout values while 210Pb inventory is comparable to the value reported for this region. A plot of depth against 14C age yields an intercept value of 1070 yrs, indicating a reservoir correction age of 1070 yrs. Most of the data points fall either on the straight line or close to the line possibly suggesting that the relative proportion of fossil carbon had remained constant throughout the core. Due to sediment compaction, a comparison of linear sedimentation rate obtained using short-lived radionuclides with those 14C could yield considerable difference and hence we compared the mass accumulation rates obtained from these isotopes. The 210Pbxs-based sediment mass accumulation rate of 17 mg cm-2 y-1, is almost a factor of 3 higher than that obtained using 14C -derived mass accumulation rate of 6 mg cm-2 y-1. The peak fallout of Pu is well preserved in the lake core suggesting relatively minimum sediment mixing. The factors that could cause this discordancy between the long-term and short-term mass accumulation rates will be discussed.

  15. Pairing-induced speedup of nuclear spontaneous fission

    NASA Astrophysics Data System (ADS)

    Sadhukhan, Jhilam; Dobaczewski, J.; Nazarewicz, W.; Sheikh, J. A.; Baran, A.

    2014-12-01

    Background: Collective inertia is strongly influenced at the level crossing at which the quantum system changes its microscopic configuration diabatically. Pairing correlations tend to make the large-amplitude nuclear collective motion more adiabatic by reducing the effect of these configuration changes. Competition between pairing and level crossing is thus expected to have a profound impact on spontaneous fission lifetimes. Purpose: To elucidate the role of nucleonic pairing on spontaneous fission, we study the dynamic fission trajectories of 264Fm and 240Pu using the state-of-the-art self-consistent framework. Methods: We employ the superfluid nuclear density functional theory with the Skyrme energy density functional SkM* and a density-dependent pairing interaction. Along with shape variables, proton and neutron pairing correlations are taken as collective coordinates. The collective inertia tensor is calculated within the nonperturbative cranking approximation. The fission paths are obtained by using the least action principle in a four-dimensional collective space of shape and pairing coordinates. Results: Pairing correlations are enhanced along the minimum-action fission path. For the symmetric fission of 264Fm, where the effect of triaxiality on the fission barrier is large, the geometry of the fission pathway in the space of the shape degrees of freedom is weakly impacted by pairing. This is not the case for 240Pu, where pairing fluctuations restore the axial symmetry of the dynamic fission trajectory. Conclusions: The minimum-action fission path is strongly impacted by nucleonic pairing. In some cases, the dynamical coupling between shape and pairing degrees of freedom can lead to a dramatic departure from the static picture. Consequently, in the dynamical description of nuclear fission, particle-particle correlations should be considered on the same footing as those associated with shape degrees of freedom.

  16. Transuranic resuspension

    SciTech Connect

    Sehmel, G.A.

    1984-04-01

    Characteristics of aged resuspension sources are more uncertain than those of new resuspension sources, which can be investigated using inert-particle controlled-tracer sources. Even though airborne concentrations are low, one aged uniform-area source which can be used for resuspension studies is the accumulated radionuclide fallout in the soil from stratospheric and tropospheric fallout debris. Airborne radionuclide concentrations from this source were investigated at convenient locations on the Hanford site. The objective is to summarize plutonium and americium resuspension research conducted by the Pacific Northwest Laboratory from 1977 to 1983. Airborne plutonium was determined at five sites in the Hanford area, and both plutonium and americium were determined at two Hanford sites. Airborne plutonium and americium were examined as a function of aerodynamic particle diameter, sampling height, wind speed increments, and wind direction increments. The following results are discussed: airborne radionuclide concentrations, ..mu..Ci/cm/sup 3/ of sampled air; radionuclide activity densities, ..mu..Ci/g of airborne solids; airborne plutonium fluxes, ..mu..Ci/(m/sup 2/ day); /sup 241/Am//sup 239 +240/Pu) activity ratios, (..mu..Ci /sup 241/Am)/(..mu..Ci/sup 239 +240/Pu); and airborne solid concentrations, ..mu..g/m/sup 3/ of sampled air. In addition, a relationship based on field data for aged plutonium sources at Bikini Atoll, the Hanford site, and Rocky Flats was developed to estimate the maximum expected plutonium activity density on airborne solids compared to activity densities for bulk surface-soil samples. As a result, it is possible to more accurately predict resuspension factor ranges as a function of the resuspension source activity densities. 31 references, 18 figures, 5 tables.

  17. Concentrations of radionuclides in fish collected from Bikini Atoll between 1977 and 1984

    SciTech Connect

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

    1986-07-01

    This report summarizes all available data on the concentrations of radionuclides in fish from Bikini Atoll between 1977 and 1984. As found in other global studies, /sup 137/Cs is most highly accumulated in edible flesh of all species of fish, the lowest fractions are found in the bone or liver. The mean concentration of /sup 137/Cs in muscle of reef fish from the southern part of the atoll is comparable to the global fallout concentration measured in market samples of fish collected from Chicago, Illinois, in 1982. /sup 90/Sr is generally associated with non-edible parts of fish, such as bone or viscera. Twenty-five to fifty percent of the total body burden of /sup 60/Co is accumulated in the muscle tissue; the remainder is distributed among the liver, skin, and viscera. The mean concentration of /sup 60/Co in fish has been decreasing at a rate faster than radiological decay alone. Most striking is the range of /sup 207/Bi concentrations among different species of fish collected at the same time and place. Highest concentrations of /sup 207/Bi were consistently detected in the muscle (and other tissues) of goatfish and some of the pelagic lagoon fish. In other reef fish, such as mullet, surgeonfish, and parrotfish, /sup 207/Bi was usually below detection limits by gamma spectrometry. Over 70% of the whole-body activity of /sup 207/Bi in goatfish is associated with the muscle tissue, whereas less than 5% is found in the muscle of mullet and surgeonfish. Neither /sup 239 +240/Pu nor /sup 241/Am is significantly accumulated in the muscle tissue of any species of fish. Apparently, /sup 238/Pu is in a more readily available form for accumulation by fishes than /sup 239 +240/Pu. Based on a daily ingestion rate of 200 q of fish flesh, dose rates to individuals through the fish-food ingestion pathway are well below current Federal guidelines.

  18. Tracer-level radioactive pilot-scale test of in situ vitrification for the stabilization of contaminated soil sites at ORNL

    SciTech Connect

    Spalding, B.P.; Jacobs, G.K.; Naney, M.T. ); Dunbar, N.W. ); Tixier, J.S.; Powell, T.D. )

    1992-11-01

    A field demonstration of in situ vitrification (ISV) was completed in May 1991, and produced approximately 12 Mg of melted earthen materials containing 12.7 mCi of radioactivity within 500 g of sludge in amodel of an old seepage trench waste disposal unit. Past waste disposal operations at Oak Ridge National Laboratory have left several contaminated seepage sites. In planning for remediation of such sites, ISV technology has been identified as a leading candidate because of the high risks associated with any retrieval option and because of the usual high quality of vitreous waste form. Major isotopes placed in the test trench were [sup 137]Cs and [sup 90]Sr, with lesser amounts of [sup 6O]Co, [sup 241]Am, and [sup 239,240]Pu. A total of 29 MWh of electrical power was delivered to the ground over a 5-day period producing a melt depth of 8.5 ft. During melting, 2.4% of the [sup 137]Cs volatilized from the melt into an off-gas containment hood and was captured quantitatively on a high efficiency particulate air filter. No volatilization of [sup 90]Sr, [sup 241]Am, or [sup 239,240]Pu was detected and > 99.993% retention of these isotopes in the melt was estimated. The use of added rare earth tracers (Ce, La, and Nd), as surrogates for transuranic isotopes, led to estimated melt retentions of >99.9995% during the test. The molten material, composed of the native soil and dolomitic limestone used for filling the test trench, reached a processing temperature of 1500[degrees]C. Standardized leaching procedures using Product Consistency Testing indicated that the ISV product has excellent characteristics relative to other vitreous nuclear waste forms.

  19. Radionuclide desorption kinetics on synthetic Zn/Ni-labeled montmorillonite nanoparticles

    NASA Astrophysics Data System (ADS)

    Huber, F. M.; Heck, S.; Truche, L.; Bouby, M.; Brendlé, J.; Hoess, P.; Schäfer, T.

    2015-01-01

    Sorption/desorption kinetics for selected radionuclides (99Tc(VII), 232Th(IV), 233U(VI), 237Np(V), 242Pu and 243Am(III)) under Grimsel (Switzerland) ground water conditions (pH 9.7 and ionic strength of ∼1 mM) in the presence of synthetic Zn or Ni containing montmorillonite nanoparticles and granodiorite fracture filling material (FFM) from Grimsel were examined in batch studies. The structurally bound Zn or Ni in the octahedral sheet of the synthetic colloids rendered them suitable as colloid markers. Only a weak interaction of the montmorillonite colloids with the fracture filling material occurs over the experimental duration of 10,000 h (∼13 months). The tri- and tetravalent radionuclides are initially strongly associated with nanoparticles in contrast to 99Tc(VII), 233U(VI) and 237Np(V) which showed no sorption to the montmorillonite colloids. Radionuclide desorption of the nanoparticles followed by sorption to the fracture filling material is observed for 232Th(IV), 242Pu and 243Am(III). Based on the conceptual model that the driving force for the kinetically controlled radionuclide desorption from nanoparticles and subsequent association to the FFM is the excess in surface area offered by the FFM, the observed desorption kinetics are related to the colloid/FFM surface area ratio. The observed decrease in concentration of the redox sensitive elements 99Tc(VII), 233U(VI) and 237Np(V) may be explained by reduction to lower oxidation states in line with Eh-pH conditions prevailing in the experiments and thermodynamic considerations leading to (i) precipitation of a sparingly soluble phase, (ii) sorption to the fracture filling material, (iii) possible formation of eigencolloids and/or (iv) sorption to the montmorillonite colloids. Subsequent to the sorption/desorption kinetics study, an additional experiment was conducted investigating the potential remobilization of radionuclides/colloids attached to the FFM used in the sorption/desorption kinetic

  20. Preserving Plutonium-244 as a National Asset

    SciTech Connect

    Patton, Bradley D; Alexander, Charles W; Benker, Dennis; Collins, Emory D; Romano, Catherine E; Wham, Robert M

    2011-01-01

    Plutonium-244 (244 Pu) is an extremely rare and long-lived isotope of plutonium with a half-life of 80 million years. Measureable amounts of 244 Pu are found in neither reactor-grade nor weapons-grade plutonium. Production of this isotope requires a very high thermal flux to permit the two successive neutron captures that convert 242 Pu to 243 Pu to 244 Pu, particularly given the short (about 5 hour) half-life of 243 Pu. Such conditions simply do not exist in plutonium production processes. Therefore, 244 Pu is ideal for precise radiochemical analyses measuring plutonium material properties and isotopic concentrations in items containing plutonium. Isotope dilution mass spectrometry is about ten times more sensitive when using 244 Pu rather than 242 Pu for determining plutonium isotopic content. The isotope can also be irradiated in small quantities to produce superheavy elements. The majority of the existing global inventory of 244 Pu is contained in the outer housing of Mark-18A targets at the Savannah River Site (SRS). The total inventory is about 20 grams of 244 Pu in about 400 grams of plutonium distributed among the 65 targets. Currently, there are no specific plans to preserve these targets. Although the cost of separating and preserving this material would be considerable, it is trivial in comparison to new production costs. For all practical purposes, the material is irreplaceable, because new production would cost billions of dollars and require a series of irradiation and chemical separation cycles spanning up to 50 years. This paper will discuss a set of options for overcoming the significant challenges to preserve the 244 Pu as a National Asset: (1) the need to relocate the material from SRS in a timely manner, (2) the need to reduce the volume of material to the extent possible for storage, and (3) the need to establish an operational capability to enrich the 244 Pu in significant quantities. This paper suggests that if all the Mark-18A plutonium is

  1. Delayed neutron detection with an integrated differential die-away and delayed neutron instrument

    SciTech Connect

    Blanc, Pauline; Tobin, Stephen J; Lee, Taehoon; Hu, Jianwei S; Hendricks, John; Croft, Stephen

    2010-01-01

    The Next Generation Safeguards Initiative (NGSI) of the U.S. Department of Energy (DOE) has funded a multilab/university collaboration to quantify the plutonium (Pu) mass and detect the diversion of pins from spent nuclear fuel. The first two years of this NGSI effort was focused on quantifying the capability of a range of nondestructive assay (NDA) techniques with Monte Carlo (MCNPX) modeling and the second current phase involves measuring Spent Fuel. One of the techniques of interest in this paper involves measuring delayed neutrons. A delayed neutron instrument using 36 fission chambers and a 14 MeV neutron generator so called DT generator (Deuterium + Tritium) surrounding the fuel was previously studied as part of the NGSI effort. This paper will quantify the capability of a standalone delayed neutron instrument using 4 {sup 3}He gas filled tubes and a DT generator with significant spectrum tailoring, located far from the fuel. So that future research can assess how well a delayed neutron instrument will function as part of an integrated NDA system. A new design is going to be used to respond to the need of the techniques. This design has been modeled for a water media and is currently being optimized for borated water and air media as part of ongoing research. This new design was selected in order to minimize the fission of {sup 238}U, to use a more realistic neutron generator design in the model, to reduce cost and facilitate the integration of a delayed neutron (DN) with a differential die-away (DDA) instrument. Since this paper will focus on delayed neutron detection, the goal is to quantify the signal from {sup 235}U, {sup 239}Pu and {sup 241}Pu, which are the isotopes present in Spent Fuel that respond significantly to a neutron interrogation. This report will quantify the capability of this new delayed neutron design to measure the combined mass of {sup 235}U, {sup 239}Pu and {sup 241}Pu for 16 of the 64 assemblies of the NGSI Spent Fuel library in one

  2. Fluorescence studies of neptunium and plutonium hexafluoride vapors

    SciTech Connect

    Beitz, J.V.; Williams, C.W.; Carnall, W.T.

    1982-03-01

    The first observation of fluorescence from gas phase, electronically excited, transuranic hexafluorides is reported. Fluorescence peaking at 1360 nm was observed from /sup 237/NpF/sub 6/ gas excited at 1064 nm. The measured fluroescence lifetime was 3.53 +- 0.01 ms, independent of NpF/sub 6/ pressure. Fluourescence peaking at 2300 nm has been observed from /sup 242/PuF/sub 6/ gas excited at 1064 nm. The measured fluorescence lifetime was 204 +- 12 ..mu..s, independent of PuF/sub 6/ pressure. In both cases the emitting state is assigned as a vibronic component of the first excited electronic state of the hexafluoride based on previously reported absorption spectra and energy level calculations. Fluorescence in the 1900 and 4800 nm region was observed from PuF/sub 6/ gas excited at 532 nm. The lifetime of this fluorescence was 86 +- 4. The emitting state giving rise to this shorter-lived fluorescence was not identified. Estimated fluorescence quantum yields are reported.

  3. In-gas-cell laser ionization studies of plutonium isotopes at IGISOL

    NASA Astrophysics Data System (ADS)

    Pohjalainen, I.; Moore, I. D.; Kron, T.; Raeder, S.; Sonnenschein, V.; Tomita, H.; Trautmann, N.; Voss, A.; Wendt, K.

    2016-06-01

    In-gas-cell resonance laser ionization has been performed on long-lived isotopes of Pu at the IGISOL facility, Jyväskylä. This initiates a new programme of research towards high-resolution optical spectroscopy of heavy actinide elements which can be produced in sufficient quantities at research reactors and transported to facilities elsewhere. In this work a new gas cell has been constructed for fast extraction of laser-ionized elements. Samples of 238-240,242Pu and 244Pu have been evaporated from Ta filaments, laser ionized, mass separated and delivered to the collinear laser spectroscopy station. Here we report on the performance of the gas cell through studies of the mass spectra obtained in helium and argon, before and after the radiofrequency quadrupole cooler-buncher. This provides valuable insight into the gas phase chemistry exhibited by Pu, which has been additionally supported by measurements of ion time profiles. The resulting monoatomic yields are sufficient for collinear laser spectroscopy. A gamma-ray spectroscopic analysis of the Pu samples shows a good agreement with the assay provided by the Mainz Nuclear Chemistry department.

  4. Examination of the effect of alpha radiolysis on plutonium(V) sorption to quartz using multiple plutonium isotopes.

    PubMed

    Hixon, Amy E; Arai, Yuji; Powell, Brian A

    2013-08-01

    The objective of this research was to determine if radiolysis at the mineral surface was a plausible mechanism for surface-mediated reduction of plutonium. Batch sorption experiments were used to monitor the amount of plutonium sorbed to high-purity quartz as a function of time, pH, and total alpha radioactivity. Three systems were prepared using both (238)Pu and (242)Pu in order to increase the total alpha radioactivity of the mineral suspensions while maintaining a constant plutonium concentration. The fraction of sorbed plutonium increased with increasing time and pH regardless of the total alpha radioactivity of the system. Increasing the total alpha radioactivity of the solution had a negligible effect on the sorption rate. This indicated that surface-mediated reduction of Pu(V) in these systems was not due to radiolysis. Additionally, literature values for the Pu(V) disproportionation rate constant did not describe the experimental results. Therefore, Pu(V) disproportionation was also not a main driver for surface-mediated reduction of plutonium. Batch desorption experiments and X-ray absorption near edge structure spectroscopy were used to show that Pu(IV) was the dominant oxidation state of sorbed plutonium. Thus, it appears that the observed surface-mediated reduction of Pu(V) in the presence of high-purity quartz was based on the thermodynamic favorability of a Pu(IV) surface complex. PMID:23683959

  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. Determination of 237Np and Pu isotopes in large soil samples by inductively coupled plasma mass spectrometry.

    PubMed

    Maxwell, Sherrod L; Culligan, Brian K; Jones, Vernon D; Nichols, Sheldon T; Bernard, Maureen A; Noyes, Gary W

    2010-12-01

    A new method for the determination of (237)Np and Pu isotopes in large soil samples has been developed that provides enhanced uranium removal to facilitate assay by inductively coupled plasma mass spectrometry (ICP-MS). This method allows rapid preconcentration and separation of plutonium and neptunium in large soil samples for the measurement of (237)Np and Pu isotopes by ICP-MS. (238)U can interfere with (239)Pu measurement by ICP-MS as (238)UH(+) mass overlap and (237)Np via (238)U peak tailing. The method provides enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then transferring Pu to DGA resin for additional purification. The decontamination factor for removal of uranium from plutonium for this method is greater than 1×10(6). Alpha spectrometry can also be applied so that the shorter-lived (238)Pu isotope can be measured successfully. (239) Pu, (242)Pu and (237)Np were measured by ICP-MS, while (236)Pu and (238)Pu were measured by alpha spectrometry. PMID:21056724

  7. 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.

  8. Preferential Radionuclide Transport in a Tuff with Altered Zones: Micro-scale Mapping

    NASA Astrophysics Data System (ADS)

    Hu, Q.; Liu, X.; Zuo, R.

    2009-12-01

    Understanding radionuclide transport in fractured rock is important for performance assessment of proposed radioactive waste disposal sites. We performed laboratory tests to study water imbibition and radionuclide transport into initially dry tuff by contacting one end of a sample with water containing a mixture of tracers (Re, 99Tc, Sr, Cs, 235U, 237Np, and 242Pu). The tuff sample, collected from Yucca Mountain, Nevada, is a cube 1-cm on each side and has a 1-mm thick altered gray zone embedded within the tuff matrix. Such gray zones are observed to be adjacent to lithophysae and fractures, are primarily quartz and tridymite, and have different hydraulic and chemical properties from the rock matrix. Capillary-driven imbibition transports tracer chemicals away from the imbibing face, causing separation of non-sorbing and sorbing tracers in tuff. Using a micro-scale profiling technique of laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS), we directly mapped the distribution of radionuclides along the altered zone (as well as transverse to the unaltered matrix). We found that the altered zone shows higher permeability, and less retardation of sorbing radionuclides, than the unaltered matrix, leading to preferential transport along the altered zone. Transverse profiling of the unaltered matrix indicated only limited penetration of strongly sorbing radionuclides, such as Pu.

  9. Fluorescence studies of neptunium and plutonium hexafluoride vapors

    NASA Astrophysics Data System (ADS)

    Beitz, James V.; Williams, Clayton W.; Carnall, W. T.

    1982-03-01

    The first observation of fluorescence from gas phase, electronically excited, transuranic hexafluorides is reported. Fluorescence peaking at 1360 nm was observed from 237NpF6 gas excited at 1064 nm. The measured fluroescence lifetime was 3.53±0.01 ms, independent of NpF6 pressure. Fluourescence peaking at 2300 nm has been observed from 242PuF6 gas excited at 1064 nm. The measured fluorescence lifetime was 204±12 μs, independent of PuF6 pressure. In both cases the emitting state is assigned as a vibronic component of the first excited electronic state of the hexafluoride based on previously reported absorption spectra and energy level calculations. Fluorescence in the 1900 and 4800 nm region was observed from PuF6 gas excited at 532 nm. The lifetime of this fluorescence was 86±4. The emitting state giving rise to this shorter-lived fluorescence was not identified. Estimated fluorescence quantum yields are reported.

  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. Determination of trace amounts of plutonium in environmental samples by RIMS using a high repetition rate solid state laser system

    NASA Astrophysics Data System (ADS)

    Grüning, C.; Huber, G.; Kratz, J. V.; Passler, G.; Trautmann, N.; Waldek, A.; Wendt, K.

    2001-08-01

    A reliable and easy to handle high repetition rate solid state laser system has been set up for routine applications of Resonance Ionization Mass Spectrometry (RIMS). It consists of three Titanium-Sapphire (Ti:Sa) lasers pumped by one Nd:YAG laser, providing up to 3 W of tunable laser light each in a wavelength range from 725 nm to 895 nm. The isotope shifts for 238Pu to 244Pu have been measured in an efficient ionization scheme with λ1=420.76 nm, λ2=847.28 nm and λ3=767.53 nm. An overall detection efficiency of the RIMS apparatus of ɛ=1×10-5 is routinely reached, resulting in a detection limit of 2×106atoms (0.8 fg) of plutonium. The isotopic compositions of synthetic samples and the NIST standard reference material SRM996 were measured. The content of 238Pu to 242Pu has been determined in dust samples from the surroundings of a nuclear power plant and 244Pu was determined in urine samples for the National Radiation Protection Board (NRPB), U.K. Routine operation of plutonium ultratrace detection could thus be established.

  12. Sub-micron Hard X-ray Fluorescence Imaging of Synthetic Elements

    PubMed Central

    Jensen, Mark P.; Aryal, Baikuntha P.; Gorman-Lewis, Drew; Paunesku, Tatjana; Lai, Barry; Vogt, Stefan; Woloschak, Gayle E.

    2013-01-01

    Synchrotron-based X-ray fluorescence microscopy (SXFM) using hard X-rays focused into sub-micron spots is a powerful technique for elemental quantification and mapping, as well as microspectroscopic measurement such as μ-XANES (X-ray absorption near edge structure). We have used SXFM to image and simultaneously quantify the transuranic element plutonium at the L3 or L2 edge as well as lighter biologically essential elements in individual rat pheochromocytoma (PC12) cells after exposure to the long-lived plutonium isotope 242Pu. Elemental maps reveal that plutonium localizes principally in the cytoplasm of the cells and avoids the cell nucleus, which is marked by the highest concentrations of phosphorus and zinc, under the conditions of our experiments. The minimum detection limit under typical acquisition conditions for an average 202 μm2 cell is 1.4 fg Pu/cell or 2.9 × 10−20 moles Pu/μm2, which is similar to the detection limit of K-edge SXFM of transition metals at 10 keV. Copper electron microscopy grids were used to avoid interference from gold X-ray emissions, but traces of strontium present in naturally occurring calcium can still interfere with plutonium detection using its Lα X-ray emission. PMID:22444530

  13. DETERMINATION OF 237NP AND PU ISOTOPES IN LARGE SOIL SAMPLES BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY

    SciTech Connect

    Maxwell, S.

    2010-07-26

    A new method for the determination of {sup 237}Np and Pu isotopes in large soil samples has been developed that provides enhanced uranium removal to facilitate assay by inductively coupled plasma mass spectrometry (ICP-MS). This method allows rapid preconcentration and separation of plutonium and neptunium in large soil samples for the measurement of {sup 237}Np and Pu isotopes by ICP-MS. {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 {sup 238}U peak tailing. The method provides enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then transferring Pu to DGA resin for additional purification. The decontamination factor for removal of uranium from plutonium for this method is greater than 1 x 10{sup 6}. Alpha spectrometry can also be applied so that the shorter-lived {sup 238}Pu isotope can be measured successfully. {sup 239}Pu, {sup 242}Pu and {sup 237}Np were measured by ICP-MS, while {sup 236}Pu and {sup 238}Pu were measured by alpha spectrometry.

  14. 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.

  15. Transfer reactions in inverse kinematics: An experimental approach for fission investigations

    NASA Astrophysics Data System (ADS)

    Rodríguez-Tajes, C.; Farget, F.; Derkx, X.; Caamaño, M.; Delaune, O.; Schmidt, K.-H.; Clément, E.; Dijon, A.; Heinz, A.; Roger, T.; Audouin, L.; Benlliure, J.; Casarejos, E.; Cortina, D.; Doré, D.; Fernández-Domínguez, B.; Jacquot, B.; Jurado, B.; Navin, A.; Paradela, C.; Ramos, D.; Romain, P.; Salsac, M. D.; Schmitt, C.

    2014-02-01

    Inelastic and multinucleon transfer reactions between a 238U beam, accelerated at 6.14 MeV/u, and a 12C target were used for the production of neutron-rich, fissioning systems from U to Cm. A Si telescope, devoted to the detection of the targetlike nuclei, provided a characterization of the fissioning systems in atomic and mass numbers, as well as in excitation energy. Cross sections and angular and excitation-energy distributions were measured for the inelastic and transfer channels. Possible excitations of the targetlike nuclei were experimentally investigated for the first time, by means of γ-ray measurements. The decays from the first excited states of 12C, 11B, and 10Be were observed with probabilities of 0.12-0.14, while no evidence for the population of higher-lying states was found. Moreover, the fission probabilities of 238U, 239Np and 240,241,242Pu and 244Cm were determined as a function of the excitation energy.

  16. Fast neutron measurements at the nELBE time-of-flight facility

    NASA Astrophysics Data System (ADS)

    Junghansa, A. R.; Beyer, R.; Grosse, E.; Hannaske, R.; Kögler, T.; Massarczyk, R.; Schwengner, R.; Wagner, A.

    2015-05-01

    The compact neutron-time-of-flight facility nELBE at the superconducting electron accelerator ELBE of Helmholtz-Zentrum Dresden-Rossendorf has been rebuilt. A new enlarged experimental hall with a flight path of up to 10 m is available for neutron time-of-flight experiments in the fast energy range from about 50 keV to 10 MeV. nELBE is intended to deliver nuclear data of fast neutron nuclear interactions e.g. for the transmutation of nuclear waste and improvement of neutron physical simulations of innovative nuclear systems. The experimental programme consists of transmission measurements of neutron total cross sections, elastic and inelastic scattering cross section measurements, and neutron induced fission cross sections. The inelastic scattering to the first few excited states in 56Fe was investigated by measuring the gamma production cross section with an HPGe detector. The neutron induced fission of 242Pu was studied using fast ionisation chambers with large homogeneous actinide deposits.

  17. Separation of Am-Cm from Al(NO/sub 3/)/sub 3/ waste solutions by in-canyon-tank precipitation as oxalates

    SciTech Connect

    Gray, L.W.; Burney, G.A.; Wilson, T.W.; McKibben, J.M.; Bibler, N.E.; Holtzscheiter, E.W.; Campbell, T.G.

    1982-04-01

    A process for recovery of Am-Cm residues from high-activity waste concentrates has been developed specifically for application in Savannah River Plant (SRP) canyon tanks. The Am-Cm residues were collected from a campaign to produce plutonium containing high isotopic concentrations of /sup 242/Pu. The separation of Am-Cm from the high-activity waste stream, containing about 2M Al(NO/sub 3/)/sub 3/, is necessary to produce an acceptable feed solution for a later pressurized cation exchange chromatography separation and purification step. The new process includes formic acid denitration, adjustment of contaminating cations by evaporation and water dilution, and oxalate precipitation of the actinides and lanthanides. After washing, the precipitate was dissolved in 8M nitric acid and the oxalate was destroyed by nitric acid oxidation that was catalyzed by manganous ions. This new process generates about one-fourth the waste of the californium solvent extraction process, which it replaced. The new process also produces a cleaner feed solution for the pressurized cation exchange chromatography separation and purification step.

  18. Synthesis of nuclei of the superheavy element 114 in reactions induced by 48Ca

    NASA Astrophysics Data System (ADS)

    Oganessian, Yu. Ts.; Yeremin, A. V.; Popeko, A. G.; Bogomolov, S. L.; Buklanov, G. V.; Chelnokov, M. L.; Chepigin, V. I.; Gikal, B. N.; Gorshkov, V. A.; Gulbekian, G. G.; Itkis, M. G.; Kabachenko, A. P.; Lavrentev, A. Yu.; Malyshev, O. N.; Rohac, J.; Sagaidak, R. N.; Hofmann, S.; Saro, S.; Giardina, G.; Morita, K.

    1999-07-01

    The stability of heavy nuclides, which tend to decay by α-emission and spontaneous fission, is determined by the structural properties of nuclear matter. Nuclear binding energies and lifetimes increase markedly in the vicinity of closed shells of neutrons or protons (nucleons), corresponding to `magic' numbers of nucleons; these give rise to the most stable (spherical) nuclear shapes in the ground state. For example, with a proton number of Z = 82 and a neutron number of N = 126, the nucleus 208Pb is `doubly-magic' and also exceptionally stable. The next closed neutron shell is expected at N = 184, leading to the prediction of an `island of stability' of superheavy nuclei, for a broad range of isotopes with Z = 104 to 120 (refs 1, 2). The heaviest known nuclei have lifetimes of less than a millisecond, but nuclei near the top of the island of stability are predicted to exist for many years. (In contrast, nuclear matter consisting of about 300 nucleons with no shell structure would undergo fission within about 10-20 seconds.) Calculations indicate that nuclei with N > 168 should already benefit from the stabilizing influence of the closed shell at N = 184. Here we report the synthesis of an isotope containing 114 protons and 173 neutrons, through fusion of intense beams of 48Ca ions with 242Pu targets. The isotope decays by α-emission with a half-life of about five seconds, providing experimental confirmation of the island of stability.

  19. Capture and Fusion-Fission Processes in Heavy Ion Induced Reactions

    NASA Astrophysics Data System (ADS)

    Itkis, M. G.; Beghini, S.; Behera, B. R.; Bogatchev, A. A.; Bouchat, V.; Corradi, L.; Dorvaux, O.; Fioretto, E.; Gadea, A.; Hanappe, F.; Itkis, I. M.; Jandel, M.; Kliman, J.; Knyazheva, G. N.; Kondratiev, N. A.; Kozulin, E. M.; Krupa, L.; Latina, A.; Lyapin, V. G.; Materna, T.; Montagnoli, G.; Oganessian, Yu. Ts.; Pokrovsky, I. V.; Prokhorova, E. V.; Rowley, N.; Rubchenya, V. A.; Rusanov, A. Ya.; Sagaidak, R. N.; Scarlassara, F.; Schmitt, C.; Stefanini, A. M.; Stuttge, L.; Szilner, S.; Trotta, M.; Trzaska, W. H.; Voskresenski, V. M.

    2005-11-01

    Results of the experiments aimed at the study of fission and quasi-fission processes in the reactions 12C+204Pb, 48Ca+144,154Sm, 168Er, 208Pb, 238U, 244Pu, 248Cm; 58Fe+208Pb, 244Pu, 248Cm, and 64Ni+186W, 242Pu are presented. The choice of the above-mentioned reactions was inspired by the experiments on the production of the isotopes 283112, 289114 and 283116 at Dubna using the same reactions. The 58Fe and 64Ni projectiles were chosen since the corresponding projectile-target combinations lead to the synthesis of even heavier elements. The experiments were carried out at the U-400 accelerator of the Flerov Laboratory of Nuclear Reactions (JINR, Russia), the XTU Tandem accelerator of the National Laboratory of Legnaro (LNL, Italy) and the Accelerator of the Laboratory of University of Jyvaskyla (JYFL, Finland) using the time-of-flight spectrometer of fission fragments CORSET and the neutron multi-detector DEMON. The role of shell effects and the influence of the entrance channel asymmetry and the deformations of colliding nucleus on the mechanism of the fusion-fission and the competitive process of quasi-fission are discussed.

  20. Shell effects in fission and quasi-fission of heavy and superheavy nuclei

    NASA Astrophysics Data System (ADS)

    Itkis, M. G.; A¨ysto¨, J.; Beghini, S.; Bogachev, A. A.; Corradi, L.; Dorvaux, O.; Gadea, A.; Giardina, G.; Hanappe, F.; Itkis, I. M.; Jandel, M.; Kliman, J.; Khlebnikov, S. V.; Kniajeva, G. N.; Kondratiev, N. A.; Kozulin, E. M.; Krupa, L.; Latina, A.; Materna, T.; Montagnoli, G.; Oganessian, Yu. Ts.; Pokrovsky, I. V.; Prokhorova, E. V.; Rowley, N.; Rubchenya, V. A.; Rusanov, A. Ya.; Sagaidak, R. N.; Scarlassara, F.; Stefanini, A. M.; Stuttge, L.; Szilner, S.; Trotta, M.; Trzaska, W. H.; Vakhtin, D. N.; Vinodkumar, A. M.; Voskressenski, V. M.; Zagrebaev, V. I.

    2004-04-01

    Results of the experiments aimed at the study of fission and quasi-fission processes in the reactions 12C+ 204Pb, 48Ca+ 144,154Sm, 168Er, 208Pb, 244Pu, 248Cm; 58Fe+ 208Pb, 244Pu, 248Cm, and 64Ni+ 186W, 242Pu are presented in the work. The choice of the above-mentioned reactions was inspired by recent experiments on the production of the isotopes 283112, 289114 and 283116 at Dubna [1],[2] using the same reactions. The 58Fe and 64Ni projectiles were chosen since the corresponding projectile-target combinations lead to the synthesis of even heavier elements. The experiments were carried out at the U-400 accelerator of the Flerov Laboratory of Nuclear Reactions (JINR, Russia), the XTU Tandem accelerator of the National Laboratory of Legnaro (LNL, Italy) and the Accelerator of the Laboratory of University of Jyvaskyla (JYFL, Finland) using the time-of-flight spectrometer of fission fragments CORSET[3] and the neutron multi-detector DEMON[4],[5]. The role of shell effects and the influence of the entrance channel on the mechanism of the compound nucleus fusion-fission and the competitive process of quasi-fission are discussed.

  1. Confirmation of the Decay of 283112 and First Indication for Hg-like Behavior of Element 112

    NASA Astrophysics Data System (ADS)

    Eichler, R.; Aksenov, N. V.; Belozerov, A. V.; Bozhikov, G. A.; Chepigin, V. I.; Dressler, R.; Dmitriev, S. N.; Gäggeler, H. W.; Gorshkov, V. A.; Haenssler, F.; Itkis, M. G.; Lebedev, V. Ya.; Laube, A.; Malyshev, O. N.; Oganessian, Yu. Ts.; Petruschkin, O. V.; Piguet, D.; Rasmussen, P.; Shishkin, S. V.; Shutov, A. V.; Svirikhin, A. I.; Tereshatov, E. E.; Vostokin, G. K.; Wegrzecki, M.; Yeremin, A. V.

    2007-05-01

    Two gas phase adsorption chemistry experiments aimed at the chemical characterization of element 112 using its isotope 283112 have been performed at the Flerov Laboratory for Nuclear Reactions (FLNR) Dubna, Russia. The applied Insitu-Volatilization and On-line Detection (IVO) technique is a thermochromatographic system combining the determination of the deposition temperature of volatile elements on a surface along a temperature gradient with an efficient detection of the deposited species by event-by-event alpha and SF-fragment spectroscopy. Two possibilities to produce the isotope 283112 were used: 1.) the direct production reaction 238U( 48Ca,3n) 283112; 2.) the reaction 242Pu( 48Ca,3n), where the primary product 287114, decays via alpha emission to 283112 with a half-life of 0.5 s. The chemistry experiments were aimed at a chemical identification of 283112 and an independent confirmation of its decay properties. In the direct reaction no decays related to 283112 were observed. However, two decay chains unambiguously attributed to the decay of 283112 were observed using the second production path. Previously reported observation of 283112 and 279Ds and their decay properties were confirmed. From its thermochromatorgaphic deposition first thermochemical data were deduced for element 112, unveiling it as a typical group 12 element.

  2. Superheavy Elements --- A Probe for Nuclear Matter at the Extremes

    NASA Astrophysics Data System (ADS)

    Ackermann, D.

    The spherical shell stabilised superheavy elements (SHE) predictedat the extreme of high Z and A are a nuclear structure phenomenon. They owe their existence to shell effects, an energy contribution of quantum mechanical origin to the nuclear potential, without which they would not be bound. Experimental activities in this field, apart from attempts to directly synthesise new elements, have to investigate reaction mechanism studies and, in particular, they have to pursue nuclear structure investigations to study the development of single particle levels towards the expected gaps for the proton (at Z = 114, 120 or 126) and neutron (at N = 184) shell closures in the region of spherical SHE. A number of exciting results in terms of the synthesis of new elements have reached the border of that region. In particular, the results obtained at the Flerov Laboratory of Nuclear Reactions (FLNR) for a rich number of decay patterns for ^{48}Ca induced reactions on actinide targets have by now been confirmed for reactions on ^{238}U, ^{244}Pu and ^{248}Cm at GSI, and on ^{242}Pu at LBNL. In recent years the development of efficient experimental set-ups, including separators and advanced particle and photon detection arrangements, allowed for more detailed nuclear structure studies for nuclei at and beyond Z = 100. Among the most interesting features is the observation of K-isomeric states. The heaviest example for such a structure feature was found in ^{270}Ds. In a recent experiment the knowledge on this nucleus and its decay products could be largely extended.

  3. New elements from Dubna

    NASA Astrophysics Data System (ADS)

    Oganessian, Yu. Ts.; Utyonkov, V. K.; Lobanov, Yu. V.; Abdullin, F. Sh.; Polyakov, A. N.; Shirokovsky, I. V.; Tsyganov, Yu. S.; Gulbekian, G. G.; Bogomolov, S. L.; Gikal, B. N.; Mezentsev, A. N.; Iliev, S.; Subbotin, V. G.; Sukhov, A. M.; Voinov, A. A.; Buklanov, G. V.; Subotic, K.; Zagrebaev, V. I.; Itkis, M. G.; Patin, J. B.; Moody, K. J.; Wild, J. F.; Stoyer, M. A.; Stoyer, N. J.; Shaughnessy, D. A.; Kenneally, J. M.; Wilk, P. A.; Lougheed, R. W.

    2005-09-01

    We have studied the dependence of the production cross-sections of the isotopes 282, 283112 and 286-288114 on the excitation energy of the compound nuclei 286112 and 290114. The maximum cross-sections of the xn-evaporation channels for the reaction 238U(48Ca, xn)286-x112 were measured to be: σ3n = 2.5+1.8-1.1pb and σ4n = 0.6+1.6-0.5pb; for the reaction 242Pu(48Ca, xn)290-x114: σ2n ˜ 0.5pb, σ3n = 3.6+3.4-1.7pb and σ4n = 4.5+3.6-1.9pb. In the reaction 233U(48Ca, 2-4n)277-279112 we measured an upper cross-section limit of σxn≤0.6pb. An increase of σER in the reactions of actinide targets with 48Ca can be due to the expected increase of the survivability of the excited compound nucleus upon closer approach to the closed neutron shell N = 184. The observed nuclear decay properties of the nuclides with Z = 104-118 are compared with theoretical nuclear mass calculations and the systematic trends of α-decay properties. As a whole, they give a consistent pattern of decay of the 18 even-Z neutron-rich nuclides with Z = 104-118 and N = 163-177.

  4. Low-Level Plutonium Bioassay Measurements at the Lawrence Livermore National Laboratory

    SciTech Connect

    Hamilton, T; Brown, T; Hickman, D; Marchetti, A; Williams, R; Kehl, S

    2007-06-18

    Plutonium-239 ({sup 239}Pu) and plutonium-240 ({sup 240}Pu) are important alpha emitting radionuclides contained in radioactive debris from nuclear weapons testing. {sup 239}Pu and {sup 240}Pu are long-lived radionuclides with half-lives of 24,400 years and 6580 years, respectively. Concerns over human exposure to plutonium stem from knowledge about the persistence of plutonium isotopes in the environment and the high relative effectiveness of alpha-radiation to cause potential harm to cells once incorporated into the human body. In vitro bioassay tests have been developed to assess uptakes of plutonium based on measured urinary excretion patterns and modeled metabolic behaviors of the absorbed radionuclides. Systemic plutonium absorbed by the deep lung or from the gastrointestinal tract after ingestion is either excreted or distributed to other organs, primarily to the liver and skeleton, where it is retained for biological half-times of around 20 and 50 years, respectively. Dose assessment and atoll rehabilitation programs in the Marshall Islands have historically given special consideration to residual concentrations of plutonium in the environment even though the predicted dose from inhalation and/or ingestion of plutonium accounts for less than 5% of the annual effective dose from exposure to fallout contamination. Scientists from the Lawrence Livermore National Laboratory (LLNL) have developed a state-of-the-art bioassay test to assess urinary excretion rates of plutonium from Marshallese populations. This new heavy-isotope measurement system is based on Accelerator Mass Spectrometry (AMS). The AMS system at LLNL far exceeds the standard measurement requirements established under the latest United States Department of Energy (DOE) regulation, 10CFR 835, for occupational monitoring of plutonium, and offers several advantages over classical as well as competing new technologies for low-level detection and measurement of plutonium isotopes. The United States

  5. Radionuclides, Heavy Metals, and Polychlorinated Biphenyls in Soils Collected Around the Perimeter of Low-Level Radioactive Waste Disposal Area G during 2006

    SciTech Connect

    P. R. Fresquez

    2007-02-28

    Twenty-one soil surface samples were collected in March around the perimeter of Area G, the primary disposal facility for low-level radioactive solid waste at Los Alamos National Laboratory (LANL). Three more samples were collected in October around the northwest corner after elevated tritium levels were detected on an AIRNET station located north of pit 38 in May. Also, four soil samples were collected along a transect at various distances (48, 154, 244, and 282 m) from Area G, starting from the northeast corner and extending to the Pueblo de San Ildefonso fence line in a northeasterly direction (this is the main wind direction). Most samples were analyzed for radionuclides ({sup 3}H, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 234}U, {sup 235}U, and {sup 238}U), inorganic elements (Al, Ba, Be, Ca, Cr, Co, Cu, Fe, Mg, Mn, Ni, K, Na, V, Hg, Zn, Sb, As, Cd, Pb, Se, Ag, and Tl) and polychlorinated biphenyl (PCB) concentrations. As in previous years, the highest levels of {sup 3}H in soils (690 pCi/mL) were detected along the south portion of Area G near the {sup 3}H shafts; whereas, the highest concentrations of {sup 241}Am (1.2 pCi/g dry) and the Pu isotopes (1.9 pCi/g dry for {sup 238}Pu and 5 pCi/g dry for {sup 239,240}Pu) were detected along the northeastern portions near the transuranic waste pads. Concentrations of {sup 3}H in three soil samples and {sup 241}Am and Pu isotopes in one soil sample collected around the northwest corner in October increased over concentrations found in soils collected at the same locations earlier in the year. Almost all of the heavy metals, with the exception of Zn and Sb in one sample each, in soils around the perimeter of Area G were below regional statistical reference levels (mean plus three standard deviations) (RSRLs). Similarly, only one soil sample collected on the west side contained PCB concentrations--67 {micro}g/kg dry of aroclor-1254 and 94 {micro}g/kg dry of aroclor-1260. Radionuclide and inorganic element

  6. 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).

  7. Americium and plutonium in water, biota, and sediment from the central Oregon coast

    SciTech Connect

    Nielsen, R. D.

    1982-06-01

    Plutonium-239, 240 and americium-241 were measured in t