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Sample records for 239pu 240pu isotope

  1. Presence of plutonium isotopes, {sup 239}Pu and {sup 240}Pu, in soils from Chile

    Chamizo, E., E-mail: echamizo@us.es [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Garcia-Leon, M., E-mail: manugar@us.es [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad de Sevilla, Avda. Reina Mercedes sn, 41012 Seville (Spain); Peruchena, J.I., E-mail: jiperuchena@gmail.com [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Cereceda, F., E-mail: francisco.cereceda@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Vidal, V., E-mail: victor.vidal@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Pinilla, E., E-mail: epinilla@unex.es [Departamento de Quimica Analitica, Facultad de Ciencias, Universidad de Extremadura, Avda. de Elvas sn, 06071 Badajoz (Spain); Miro, C., E-mail: cmiro@unex.es [Departamento de Fisica Aplicada, Universidad de Extremadura, Avda. de la Universidad sn, 10071 Caceres (Spain)

    2011-12-15

    Plutonium is present in every environmental compartment, due to a variety of nuclear activities. The Southern Hemisphere has received about 20% of the global {sup 239}Pu and {sup 240}Pu 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 {sup 239}Pu and {sup 240}Pu 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 Degree-Sign Southern latitude range, with {sup 240}Pu/{sup 239}Pu 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 Degree-Sign 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 {sup 239+240}Pu activity inventories show as well a wider variability range in that latitude range, in agreement with the expected heterogeneity of the contamination.

  2. Plutonium isotopes 238Pu, 239+240Pu, 241Pu and 240Pu/239Pu atomic ratios in the southern Baltic Sea ecosystem

    Dagmara I. Strumińska-Parulska

    2010-09-01

    Full Text Available The paper summarizes the results of plutonium findings in atmospheric fallout samples and marine samples from the southern Baltic Sea during our research in 1986-2007. The activities of 238Pu and 239+240Pu isotopes were measured with an alpha spectrometer. The activities of 241Pu were calculated indirectly by 241Am activity measurements 16-18 years after the Chernobyl accident. The 240Pu/239Pu atomic ratios were measured using accelerator mass spectrometry (AMS. The 241Pu activities indicate that the main impact of the Chernobyl accident was on the plutonium concentration in the components of the Baltic Sea ecosystem examined in this work. The highest 241Pu/239+240Pu activity ratio was found in sea water (140 ± 33. The AMS measurements of atmospheric fallout samples collected during 1986 showed a significant increase in the 240Pu/239Pu atomic ratio from 0.29 ± 0.04 in March 1986 to 0.47 ± 0.02 in April 1986.

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

    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.

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

    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.

  5. 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.

    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

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

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

    2014-04-01

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

  7. (137)Cs, (239+240)Pu concentrations and the (240)Pu/(239)Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary.

    Pan, S M; Tims, S G; Liu, X Y; Fifield, L K

    2011-10-01

    A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of (137)Cs and plutonium (Pu) isotopes. The (137)Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the (137)Cs and (239+240)Pu. The shape of the vertical (137)Cs distribution in the sediment core was similar to that of the Pu. The maximum (137)Cs and (239+240)Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average (240)Pu/(239)Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the (240)Pu/(239)Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The (137)Cs and (239+240)Pu inventories were estimated to be 7100 ± 1200 Bq/m(2) and 407 ± 27 Bq/m(2), respectively. Approximately 40% of the (239+240)Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure (240)Pu/(239)Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.

  8. Estimation of uncertainties in resonance parameters of {sup 56}Fe, {sup 239}Pu, {sup 240}Pu and {sup 238}U

    Nakagawa, Tsuneo; Shibata, Keiichi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1997-05-01

    Uncertainties have been estimated for the resonance parameters of {sup 56}Fe, {sup 239}Pu, {sup 240}Pu and {sup 238}U contained in JENDL-3.2. Errors of the parameters were determined from the measurements which the evaluation was based on. The estimated errors have been compiled in the MF32 of the ENDF format. The numerical results are given in tables. (author)

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

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

    2015-04-07

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

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

    Yamada, Masatoshi; Zheng, Jian; Wang, Zhong-Liang [Nakaminato Laboratory for Marine Radioecology, National Institute of Radiological Sciences, Isozaki 3609, Hitachinaka, Ibaraki 311-1202 (Japan)

    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 {sup 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 {sup 137}Cs activities showed a wide variation with values ranging from 1.1 Bq m{sup -3} in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m{sup -3} in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of {sup 137}Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of {sup 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 {sup 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{sup -1} in the Sulu and Indonesian Seas, 0.033 yr{sup -1} in the Bay of Bengal and Andaman Sea, and 0.029 yr{sup -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. {sup 239+240}Pu activities and {sup 240}Pu/{sup 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 {sup 240}Pu/{sup 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

  11. Perturbation in the {sup 240}Pu/{sup 239}Pu global fallout ratio in local sediment following the nuclear accidents at Thule (Greenland) and Palomares (Spain)

    Mitchell, P.I.; Vintro, L.L. [University Coll., Dublin (Ireland). Dept. of Physics; Dahlgaard, H. [Risoe National Lab., Roskilde (Denmark); Gasco, C.; Sanchez-Cabeza, J.A. [Barcelona Univ. (Spain). Dept. de Fisica Teorica

    1995-12-31

    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 {sup 240}Pu/{sup 239}Pu atom ratio of {approx}0.18. Measurements of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing, has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the {sup 240}Pu/{sup 239}Pu ratio has been examined in samples of sediment 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 {sup 240}Pu/{sup 239}Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution. The analytical results showed that at Thule the mean {sup 240}Pu/{sup 239}Pu atom ratio was 0.033{+-}0.004, while at Palomares the equivalent ratio appeared to be significantly higher at 0.056{+-}0.003. Both ratios are consistent with those reported for soils samples at the Nevada site and Nagasaki, and are clearly indicative of weapons-grade plutonium. 27 refs., 1 fig., 2 tabs.

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

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

    2013-10-01

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

  13. Simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu by high resolution inductively coupled plasma mass spectrometer (HR ICP-MS) in marine sediments; Mesure des isotopes du plutonium des sediments marins par spectrometrie de masse a plasma couple inductivement haute resolution (HR ICP-MS)

    Bruneau, F

    1999-07-01

    Transuranics elements are of particular interest in radioecological studies because of their radiotoxicity and their potential use to decipher source fingerprints and transport processes. The simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu in environmental samples requires a specific chemical procedure. This work deals with an analytical procedure which yields a very high grade of purification of Pu suitable for ultra low level detection by HR ICP-MS, from marine sediments. After the elimination of major elements (Fe, Al, Mg...) by a first chromatographic separation, a new device of purification by solvent extraction and concentration by a second chromatographic separation is used to obtain a concentrated and high purified solution of plutonium. The chemical procedure have been validated on IAEA certified sediment samples and on sediment samples collected in the roads of Cherbourg which had been previously analysed by other techniques (a spectrometry and thermo-ionisation mass spectrometer). (author)

  14. Evaluation of fission cross sections and covariances for {sup 233}U, {sup 235}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, and {sup 241}Pu

    Kawano, Toshihiko [Kyushu Univ., Fukuoka (Japan); Matsunobu, Hiroyuki [Data Engineering, Inc. (Japan); Murata, Toru [AITEL Corporation, Tokyo (JP)] [and others

    2000-02-01

    A simultaneous evaluation code SOK (Simultaneous evaluation on KALMAN) has been developed, which is a least-squares fitting program to absolute and relative measurements. The SOK code was employed to evaluate the fission cross sections of {sup 233}U, {sup 235}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, and {sup 241}Pu for the evaluated nuclear data library JENDL-3.3. Procedures of the simultaneous evaluation and the experimental database of the fission cross sections are described. The fission cross sections obtained were compared with evaluated values given in JENDL-3.2 and ENDF/B-VI. (author)

  15. Determination of the {sup 240}Pu/{sup 239}Pu atom ratio in low activity environmental samples by alpha spectrometry and spectral deconvolution

    Leon Vintro, L. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Mitchell, P.I. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Condren, O.M. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Moran, M. [Lawrence Livermore National Lab., Livermore, CA (United States); Vives i Batlle, J. [University Coll., Dublin (Ireland). Dept. of Experimental Phys.; Sanchez-Cabeza, J.A. [Dept. de Fisica, Universidad Autonoma de Barcelona, Bellaterra (Spain)

    1996-02-01

    In this paper, a simple technique, based on commercially-available software developed for gamma spectra analysis (MicroSAMPO {sup trademark}), is described by which this complex multiplet can be resolved at the much lower activities typical of many environmental samples. In our approach, it is not necessary to make any alterations to the normal alpha spectrometric set-up (including energy dispersion), other than to improve collimation. The instrumental function is defined for each spectrum by fitting a modified gaussian with exponential tails to the comparatively well-resolved {sup 242}Pu ``doublet`` (used as tracer) and, if present, the {sup 238}Pu ``doublet``. The fitted peaks are used to create an energy calibration file with which, using published energy data, the positions (in channels) of the component peaks of the multiplet are predicted. These positions are not altered subsequently when MicroSAMPO`s interactive multiplet analysis facility is used to quantify the relative spectral intensities of the components. Before calculating the {sup 240}Pu/{sup 239}Pu ratio, it is advisable to correct for coincidence summing of alpha particles and conversion electrons. The technique has been applied to the determination of the {sup 240}Pu/{sup 239}Pu ratio in a set of environmental samples, most of which were supplied by IAEA-MEL under their laboratory intercomparison programme. Subsequently, replicate samples were analysed independently using thermal ionisation mass spectrometry. The agreement between the two sets of data was most satisfactory. Further validation of this deconvolution technique was provided by the good agreement between the measured alpha-emission probabilities for the component peaks in the {sup 239,240}Pu multiplet and published values. (orig.).

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

    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.

  17. Migration of plutonium from freshwater ecosystem at Hanford. [/sup 238/Pu, /sup 239/Pu, /sup 240/Pu

    Emery, R. M.; Klopfer, D. C.; McShane, M. C.

    1977-09-01

    A reprocessing waste pond at Hanford has been inventoried to determine quantities of plutonium (Pu) that have been accumulated since its formation in 1944. Expressions of export were developed from these inventory data and from informed assumptions about the vectors which act to mobilize material containing Pu. This 14-acre pond provides a realistic illustration of the mobility of Pu in a lentic ecosystem. The ecological behavior of Pu in this pond is similar to that in other contaminated aquatic systems having widely differing limnological characteristics. Since its creation, this pond has received about one Ci of /sup 239/,/sup 240/Pu and /sup 238/Pu, most of which has been retained by its sediments. Submerged plants, mainly diatoms and Potamogeton, accumulate >95% of the Pu contained in biota. Emergent insects are the only direct biological route of export, mobilizing about 5 x 10/sup 3/ nCi of Pu annually, which is also the estimated maximum quantity of the Pu exported by waterfowl, birds and mammals collectively. There is no apparent significant export by wind, and it is not likely that Pu has migrated to the ground water below U-Pond via percolation. Although this pond has a rapid flushing rate, a eutrophic nutrient supply with a diverse biotic profile, and interacts with an active terrestrial environment, it appears to effectively bind Pu and prevent it from entering pathways to man and other life.

  18. Time-resolved record of (236)U and (239,240)Pu isotopes from a coral growing during the nuclear testing program at Enewetak Atoll (Marshall Islands).

    Froehlich, M B; Chan, W Y; Tims, S G; Fallon, S J; Fifield, L K

    2016-12-01

    A comprehensive series of nuclear tests were carried out by the United States at Enewetak Atoll in the Marshall Islands, especially between 1952 and 1958. A Porites Lutea coral that was growing in the Enewetak lagoon within a few km of all of the high-yield tests contains a continuous record of isotopes, which are of interest (e.g. (14)C, (236)U, (239,240)Pu) through the testing period. Prior to the present work, (14)C measurements at ∼2-month resolution had shown pronounced peaks in the Δ(14)C data that coincided with the times at which tests were conducted. Here we report measurements of (236)U and (239,240)Pu on the same coral using accelerator mass spectrometry, and again find prominent peaks in the concentrations of these isotopes that closely follow those in (14)C. Consistent with the (14)C data, the magnitudes of these peaks do not, however, correlate well with the explosive yields of the corresponding tests, indicating that smaller tests probably contributed disproportionately to the debris that fell in the lagoon. Additional information about the different tests can also be obtained from the (236)U/(239)Pu and (240)Pu/(239)Pu ratios, which are found to vary dramatically over the testing period. In particular, the first thermonuclear test, Ivy-Mike, has characteristic (236)U/(239)Pu and (240)Pu/(239)Pu signatures which are diagnostic of the first arrival of nuclear test material in various archives.

  19. 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.

    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.

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

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

    2014-06-01

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

  1. 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.

    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.

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

    G. Palmiottti; H. Hiruta; M. Salvatores

    2011-09-01

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

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

    Chamizo, Elena; López-Lora, Mercedes [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Villa, María [Departamento de Física Aplicada II, Universidad de Sevilla, Av. Reina Mercedes 4A, 41012 Seville (Spain); Servicio de Radioisótopos, Centro de Investigación, Tecnología e Innovación, Universidad de Sevilla, Av. Reina Mercedes 4B, 41012 Seville (Spain); Casacuberta, Núria [Laboratory of Ion Beam Physics, ETH Zürich, Otto-Stern-Weg 5, CH-8093 Zürich (Switzerland); López-Gutiérrez, José María [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Departamento de Física Aplicada I, Escuela Universitaria Politécnica, Universidad de Sevilla, Virgen de África 7, 41011 Seville (Spain); Pham, Mai Khanh [IAEA-Environment Laboratories, Monte Carlo 98000 (Monaco)

    2015-10-15

    The performance of the 1 MV AMS system at the CNA (Centro Nacional de Aceleradores, Seville, Spain) for {sup 236}U and {sup 239,240}Pu measurements has been extensively investigated. A very promising {sup 236}U/{sup 238}U abundance sensitivity of about 3 × 10{sup −11} has been recently achieved, and background figures for {sup 239}Pu of about 10{sup 6} atoms were reported in the past. These promising results lead to the use of conventional low energy AMS systems for the analysis of {sup 236}U and {sup 239}Pu and its further application in environmental studies. First {sup 236}U 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 {sup 236}U/{sup 239}Pu 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 {sup 236}U/{sup 238}U determinations at, at least, 7 × 10{sup −10} level. Finally, these results are discussed in their environmental context.

  4. Determination of plutonium isotopes in seawater reference materials using isotope-dilution ICP-MS.

    Zheng, Jian; Yamada, Masatoshi

    2012-09-01

    We analyzed the activities of (239)Pu, (240)Pu, (239+240)Pu, (241)Pu, the ratio of number of atoms (atom ratio) for (240)Pu/(239)Pu, and the activity ratio of (241)Pu/(239+240)Pu in seawater reference materials, IAEA-443 and IAEA-381, using a highly sensitive isotope dilution sector field inductively coupled plasma mass spectrometry method. With a mean chemical yield of 65% determined with (242)Pu as a tracer, we found that the experimentally established values in IAEA-443 for (239)Pu, (240)Pu, (241)Pu and (239+240)Pu activities are almost the same as those in IAEA-381. Regarding the (239+240)Pu activity, we provided the most precise and accurate result among the twelve laboratories, which participated in the interlaboratory comparison. In addition, for the (240)Pu/(239)Pu atom ratio, our results for IAEA-381 (0.2315±0.0008) and IAEA-443 (0.2325±0.0008) are in good agreement with the IAEA information value (0.229±0.006), but have much smaller uncertainty. Since the new seawater reference material, IAEA-443, is commercially available, it can be used not only for method validation for seawater plutonium isotope ratio and activity analysis, but also for more general use as a plutonium isotope standard for mass discrimination correction for other environmental samples.

  5. Characterization of a {sup 239}PuBe isotopic neutron source

    Vega C, H. R.; Hernandez D, V. M. [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Cipres No. 10, Fracc. La Penuela, 98068 Zacatecas (Mexico); Rivera M, T. [IPN, Centro de Investigacion en Ciencia Aplicada y Tecnologia Avanzada, Calz. Legaria No. 694, Col. Irrigacion, 11500 Mexico D. F. (Mexico); Sanchez, A., E-mail: fermineutron@yahoo.com [IPN, Escuela Superior de Fisica y Matematicas, 07738 Mexico D. F. (Mexico)

    2012-10-15

    A Bonner sphere spectrometer was used to determine the features of a {sup 239}PuBe neutron source used to operate the ESFM-Ipn Subcritical Reactor. The spectrometer is a {sup 6}Lil(Eu) scintillator and 2, 3, 5, 8, 10 and 12 inches-diameter polyethylene spheres, that was located 100 cm from the neutron source. The 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, using the MCNP5 code, was carried out to estimate the spectrum and integral features being less that values obtained experimentally due to the presence of {sup 241}Pu in the Pu used to fabricate the source. Using the experimental information the actual neutron yield and the mass fraction of {sup 241}Pu was estimated. (Author)

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

    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

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

    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.

  8. Resolving Nevada Test Site and global fallout plutonium in attic dust and soils using [sup 137]Cs/[sup 239+240]Pu activity ratios

    Cizdziel, J. (Univ. of Nevada, Reno, NV (United States)); Hodge, V. (Univ. of Nevada, Las Vegas, NV (United States). Dept. of Chemistry); Faller, S. (Environmental Protection Agency, Las Vegas, NV (United States). Radiation and Indoor Environments National Lab.)

    1999-07-01

    A simple equation using only [sup 137]Cs/[sup 239+240]Pu activity ratios was developed and evaluated as a means of resolving the plutonium in attic dust and soil from Nevada and Utah that came from Nevada Test Site fallout from that which came from global fallout. Applied to a historical data set of [sup 137]Cs and [sup 239+240]Pu activity concentrations in soils from Nevada and Utah, the activity ratio method gives results similar to the traditional [sup 240]Pu/[sup 239]Pu isotope mass ratio method. Considering the difficulty and expense of determining the [sup 240]Pu/[sup 239]Pu atom ratios, this activity ratio method is simpler, faster, and less costly, and may be useful for detecting and/or monitoring plutonium contamination in soils. Applied to samples of attic dust and soil collected from throughout southern Nevada and Utah during 1996 and 1997, it was found that all sites surveyed showed the presence of Nevada Test Site plutonium. Over 90% of the plutonium found in the samples from Beatty, Tonopah, and Queen City Summit, Nevada can be attributed to the Nevada Test Site.

  9. A multi-radionuclide approach to evaluate the suitability of {sup 239+240}Pu as soil erosion tracer

    Meusburger, Katrin, E-mail: Katrin.Meusburger@unibas.ch [Environmental Geosciences, University of Basel, Bernoullistrasse 30, CH-4056 Basel (Switzerland); Mabit, Lionel, E-mail: L.Mabit@iaea.org [Soil and Water Management and Crop Nutrition Laboratory, FAO/IAEA Agriculture & Biotechnology Laboratory, IAEA Laboratories, Seibersdorf (Austria); Ketterer, Michael, E-mail: mkettere@msudenver.edu [Chemistry Department, Metropolitan State University of Denver, CO (United States); Park, Ji-Hyung, E-mail: jhp@ewha.ac.kr [Department of Environmental Science & Engineering, Ewha Womans University, Seoul 120-750 (Korea, Republic of); Sandor, Tarjan [Radioanalytical Reference Laboratory, Central Agricultural Office Food and Feed Safety Directorate (Hungary); Porto, Paolo, E-mail: paolo.porto@unirc.it [Dipartimento di AGRARIA, Università degli Studi “Mediterranea” di Reggio Calabria (Italy); Alewell, Christine, E-mail: Christine.Alewell@unibas.ch [Environmental Geosciences, University of Basel, Bernoullistrasse 30, CH-4056 Basel (Switzerland)

    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 {sup 239}Pu and {sup 240}Pu as a method to assess soil erosion magnitude by comparison to more established fallout radionuclides such as {sup 137}Cs and {sup 210}Pb{sub ex}. 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 (> 25 t ha{sup −1} yr{sup −1}). Pu isotopes further allowed determining the origin of the fallout. Both {sup 240}Pu/{sup 239}Pu atomic ratios and {sup 239+240}Pu/{sup 137}Cs activity ratios were close to the global fallout ratio. However, the depth profile of the {sup 239+240}Pu/{sup 137}Cs activity ratios in undisturbed sites showed lower ratios in the top soil increments, which might be due to higher migration rates of {sup 239+240}Pu. The activity ratios further indicated preferential transport of {sup 137}Cs from eroded sites (higher ratio compared to the global fallout) to the depositional sites (smaller ratio). As such the {sup 239+240}Pu/{sup 137}Cs activity ratio offered a new approach to parameterize a particle size correction factor that can be applied when both {sup 137}Cs and {sup 239+240}Pu have the same fallout source. Implementing this particle size correction factor in the conversion of {sup 137}Cs inventories resulted in comparable estimates of soil loss for {sup 137}Cs and {sup 239+240}Pu. The comparison among the different fallout radionuclides highlights the suitability of {sup 239+240}Pu through less preferential transport compared to {sup 137}Cs and the possibility to gain information regarding the origin of the fallout. In conclusion, {sup 239+240}Pu is a promising soil erosion tracer, however, since the behaviour i.e. vertical migration in the

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

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

    2016-01-01

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

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

    Ezerinskis, Z.; Hou, Xiaolin; Druteikiene, R.;

    2016-01-01

    Fifty five soil samples collected in the Lithuania teritory in 2011 and 2012 were analyzed for 129I, 137Cs and Pu isotopes in order to investigate the level and distribution of artificial radioactivity in Lithuania. The activity and atomic ratio of 238Pu/239,240Pu, 129I/127I and 131I/137Cs were...... used to identify the origin of these radionuclides. The 238Pu/239þ240Pu and 240Pu/239Pu ratios in the soil samples analyzed varied in the range of 0.02e0.18 and 0.18e0.24, respectively, suggesting the global fallout as the major source of Pu in Lithuania. The values of 109 to 106 for 129I/127I atomic...... ratio revealed that the source of 129I in Lithuania is global fallout in most cases though several sampling sites shows a possible impact of reprocessing releases. Estimated 129I/131I ratio in soil samples from the southern part of Lithuania shows negligible input of the Chernobyl fallout...

  12. Isotope dilution gamma spectrometry for Pu using low energy photons

    Paul, S.; Sarkar, A.; Alamelu, D.; Shah, R.V.; Aggarwal, S.K. [Bhabha Atomic Reseach Centre, Mumbai (India). Fuel Chemistry Div.

    2012-07-01

    Isotope dilution gamma spectrometry (IDGS) for determination of the Pu concentration, using high resolution gamma-ray spectrometry (HRGS) in the 40-150 keV energy range, is developed and described. The methodology involves purification of Pu by an anion exchange procedure, followed by the determination of Pu isotopic composition using HRGS. For isotope dilution, a pre-calibrated power reactor grade Pu ({proportional_to} 70 at. % {sup 239}Pu) solution from an Indian PHWR was used as a spike for research reactor grade Pu ({proportional_to} 95 at. % {sup 239}Pu) samples and vice versa. Changes in {sup 240}Pu/{sup 239}Pu (45.24 keV/51.62 keV) and {sup 241}Pu/{sup 239}Pu (148.57 keV/129.29 keV) activity ratios in the spiked samples were determined by gamma spectrometry. Using the atom ratios calculated from the measured activity ratios, the concentration of Pu in the sample was calculated using two different efficiency calibration methods. The isotopic composition and concentration of Pu samples both from power reactor and research reactor grade agreed well with the values obtained by isotope dilution-thermal ionization mass spectrometry. The present method also shows the superiority of using the {sup 240}Pu/{sup 239}Pu atom ratio against the {sup 241}Pu/{sup 239}Pu atom ratio in IDGS with respect to the accuracy and precision. (orig.)

  13. Analysis Method of 241Pu Radioactivity by Isotope Dilution-Extraction Liquid Scintillation Spectrometer

    2008-01-01

    <正>241Pu is the only pure β emitter with the maximum energy of 20.81 keV in plutonium isotopes of 238Pu, 239Pu, 240Pu and 242Pu, in which 241Pu is mostly specific radioactivity because its half-life is 14.29 a.

  14. Distribution characteristics of ¹³⁷Cs, Pu isotopes and ²⁴¹Am in soil in Korea.

    Lee, S H; Oh, J S; Lee, J M; Lee, K B; Park, T S; Lujaniene, G; Valiulis, D; Sakalys, J

    2013-11-01

    Cesium-137, Plutonium isotopes and (241)Am were studied in soil samples collected from Korea between 2006 and 2008 to provide information on the distribution and origin of Pu isotopes and (241)Am. The vertical profiles of radionuclides showed higher activity concentrations at the surface layer and then gradually decreased with depth. A good correlation between (137)Cs and (239,240)Pu was observed, whereas a poor relationship between (137)Cs and (241)Am was found. The (238)Pu/(239,240)Pu, (241)Am/(239,240)Pu and (239,240)Pu/(137)Cs activity ratios were concordant to those of the global fallout ratios. Furthermore, the atomic ratios of (240)Pu/(239)Pu in the samples provided the information of Pu depositional history and the origin of Pu isotopes in Korea.

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

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

    2007-06-01

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

  16. Rapid and simultaneous determination of neptunium and plutonium isotopes in environmental samples by extraction chromatography using sequential injection analysis and ICP-MS

    Qiao, Jixin; Hou, Xiaolin; Roos, Per

    2010-01-01

    This paper reports an automated analytical method for rapid and simultaneous determination of plutonium isotopes (239Pu and 240Pu) and neptunium (237Np) in environmental samples. An extraction chromatographic column packed with TrisKem TEVA® resin was incorporated in a sequential injection (SI...

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

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin

    2014-01-01

    This paper reports an analytical method for the determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation...

  18. Plutonium Isotopes ((239-241)Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed.

    Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Golser, Robin; Gómez-Guzmán, José Manuel; Korschinek, Gunther; Kortmann, Florian; Lierse von Gostomski, Christoph; Ludwig, Peter; Steier, Peter; Tazoe, Hirofumi; Yamada, Masatoshi

    2017-02-21

    The concentration of plutonium (Pu) and the isotopic ratios of (240)Pu to (239)Pu and (241)Pu to (239)Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular, (241)Pu is a well-suited indicator for a recent entry of Pu because (241)Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated (240)Pu/(239)Pu ratio of up to 0.22 ± 0.02 compared to global fallout ((240)Pu/(239)Pu = 0.180 ± 0.007), whereas all measured (241)Pu-to-(239)Pu ratios were consistent with nuclear weapon fallout ((241)Pu/(239)Pu < 2.4 × 10(-3)), which means that no impact from the Fukushima accident was detected. From the average (241)Pu-to-(239)Pu ratio of 8-2(+3) ×10(-4) at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the (239)Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.

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

    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.

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

    Chamizo, E., E-mail: elechacal@alum.us.e [Centro Nacional de Aceleradores (CNA), Isla de la Cartuja, 41092 Seville (Spain); Jimenez-Ramos, M.C.; Enamorado, S.M. [Centro Nacional de Aceleradores (CNA), Isla de la Cartuja, 41092 Seville (Spain); Garcia-Leon, M. [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad de Sevilla, 41012 Sevilla (Spain); Garcia-Tenorio, R. [Departamento de Fisica Aplicada II, E.T.S.A, Universidad de Sevilla, 41012 Sevilla (Spain); Mas, J.L. [Departamento de Fisica Aplicada I, Universidad de Sevilla, 41012 Sevilla (Spain); Masque, P. [Institut de Ciencia i Tecnologia Ambientals, Department de Fisica, Universitat Autonoma de Barcelona, 08193 Bellaterra (Spain); Merino, J. [Amphos 21, Pg. de Rubi 29-31, E-08197 Valldoreix (Spain); Sanchez-Cabeza, J.A. [Institut de Ciencia i Tecnologia Ambientals, Department de Fisica, Universitat Autonoma de Barcelona, 08193 Bellaterra (Spain); International Atomic Energy Agency, Marine Environment Laboratories, MC-98000 (Monaco)

    2010-04-15

    The measurement of plutonium isotopes, {sup 239}Pu and {sup 240}Pu, 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 {sup 240}Pu/{sup 239}Pu 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 {sup 240}Pu/{sup 239}Pu 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 {sup 238}Pu/{sup (239+240)}Pu activity ratios, samples were also studied by alpha-spectrometry (AS). The obtained AS {sup 239+240}Pu activity concentration results fit in with the AMS ones in a wide dynamic range, thus validating the AMS technique.

  1. 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.

    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.

  2. Transport process of Pu isotope in marginal seas of the western North Pacific Ocean

    Yamada, Masatoshi [Department of Radiation Chemistry, Institute of Radiation Emergency Medicine, Hirosaki University, Hirosaki, 036-8564, Aomori (Japan); Zheng, Jian [Research Center for Radiation Protection, National Institute of Radiological Sciences, 4-9-1 Anagawa, Inage, 263-8555, Chiba (Japan)

    2014-07-01

    Significant quantities of Pu isotopes have been released into the marine environment as the result of atmospheric nuclear weapons testing. Most radionuclides globally dispersed in atmospheric nuclear weapons testing were released into the environment during the 1950's and 1960's. In the western North Pacific Ocean, the principal source can be further distinguished as two distinct sources of Pu: close-in tropospheric fallout from nuclear weapons testing at the Pacific Proving Grounds (PPG) in the Marshall Islands and global stratospheric fallout. Since the {sup 240}Pu/{sup 239}Pu atom ratio is characteristic for the Pu emission source, information on Pu isotopic signature is very useful to better understand the transport process in the oceans and to identify the sources of Pu. The mean atom ratio of {sup 240}Pu/{sup 239}Pu from the global stratospheric fallout is 0.180 ±0.014 based on soil sample data, whereas that from close-in tropospheric fallout from the PPG is 0.33 - 0.36. The {sup 240}Pu/{sup 239}Pu atom ratios in seawater samples collected in marginal seas of the western North Pacific Ocean will provide important and useful data for understanding the process controlling Pu transport and for distinguishing future Pu sources. The objectives of this study were to measure the {sup 239+240}Pu concentrations and {sup 240}Pu/{sup 239}Pu atom ratios in seawater from the Sea of Okhotsk, Japan Sea, South China Sea and Sulu Sea and to discuss the transport process of Pu. Large-volume seawater samples (250 L each) were collected from the surface to the bottom in marginal seas of the western North Pacific Ocean with acoustically triggered quadruple PVC sampling bottles during the R/V Hakuho-Maru cruise. The {sup 239}Pu and {sup 240}Pu concentrations and {sup 240}Pu/{sup 239}Pu 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. In

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

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

    2016-07-05

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

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

    Wilcken, K.M. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia)]. E-mail: k.wilcken@suerc.gla.ac.uk; Barrows, T.T. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia); Fifield, L.K. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia); Tims, S.G. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia); Steier, P. [VERA Laboratory, Institute for Isotopic Research and Nuclear Physics, University of Vienna, Waehringer Strasse 17, A-1090 Vienna (Austria)

    2007-06-15

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

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

    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.

  6. Analysis on the Isotopic Ratio of Picogram Pu by TIMS%皮克量级钚同位素丰度比的TIMS分析

    杨天丽; 龙开明; 刘雪梅; 刘钊; 汤磊

    2005-01-01

    The isotopic abundance ratios for Pu at 6.7 pg level were measured by thermal surface ionization mass spectrometry (TIMS). During the preparation of Pu samples carbon power was used as an emitting and stabilizing reagent, which increase the collection efficiency, the ion current intense and the ion emission stability for Pu. The measurment results indicate that the relative standard deviation of 2.7% for the isotopic abundance ratios of 240Pu to 239Pu is achieved when the 240Pu ion current is 8-20 cps.

  7. Plutonium concentration and isotopic ratio in soil samples from central-eastern Japan collected around the 1970s

    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.

  8. Ultratrace and isotope ratios analyses of some radionuclides by ICP-MS

    Helal, A.I.; Zahran, N.F.; Abd El-Lateef, A.M.; Mohsen, H.T. [Central Lab. for Elemental and Isotopic Analysis, N.R.C. Atomic Energy Authority, Cairo (Egypt); Amr, M.A. [Central Lab. for Elemental and Isotopic Analysis, N.R.C. Atomic Energy Authority, Cairo (Egypt); Nuclear Physics Dept., N.R.C., Atomic Energy Authority, Cairo (Egypt); Bashter, I.I. [Physics Dept., Faculty of Science, Zagazig Univ. (Egypt); Abbas, Y. [Physics Dept., Faculty of Science, Suez Canal Univ., Ismailia (Egypt)

    2004-07-01

    Extensive work is under way using high resolution-ICP-MS for {sup 90}Sr, {sup 234}U, {sup 235}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, and {sup 241}Am detection. Sample preparation procedures based on liquid-liquid extraction and ion exchange chromatography were developed. Sr, U, Pu, and Am were separated from their matrix and concentrated to improve the power of detection in the mass spectrometer. A microconcentric nebulizer with a desolvation introduction system (Ardius) is used. Instrumental limits of detection using Sr and U standard solutions are 0.01 ppt and 0.006 ppt for Sr and U, respectively. A study is presented on the mass interferences for the specified radionuclides. In the environmental samples investigated the {sup 90}Sr/{sup 86}Sr isotope ratio is 6.02 x 10{sup -9} and for {sup 240}Pu/{sup 239}Pu the isotope ratio is 0.17. (orig.)

  9. Release of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant accident to the marine environment was negligible.

    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.

  10. Neutron Capture Cross Section of 239Pu

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

    2014-09-01

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

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

    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.

  12. AMS of the Minor Plutonium Isotopes.

    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.

  13. Nucleogenic {sup 36}Cl, {sup 236}U and {sup 239}Pu in uranium ores

    Wilcken, K.M. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia); Scottish Universities Environmental Research Centre, Scottish Enterprise Technology Park, Rankine Avenue, East Kilbride G75 0QF (United Kingdom)], E-mail: K.Wilcken@suerc.gla.ac.uk; Fifield, L.K.; Barrows, T.T.; Tims, S.G.; Gladkis, L.G. [Department of Nuclear Physics, RSPhysSE, Australian National University, Canberra, ACT 0200 (Australia)

    2008-08-15

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

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

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

    2008-08-01

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

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

    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.

  16. Plutonium isotope ratio variations in North America

    Steiner, Robert E [Los Alamos National Laboratory; La Mont, Stephen P [Los Alamos National Laboratory; Eisele, William F [Los Alamos National Laboratory; Fresquez, Philip R [Los Alamos National Laboratory; Mc Naughton, Michael [Los Alamos National Laboratory; Whicker, Jeffrey J [Los Alamos National Laboratory

    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.

  17. [ECG indices in dogs after inhalation of 239Pu].

    Karpova, V N

    1985-11-01

    Dogs of both sexes aged 2 to 4 were subjected to inhalation inoculation with polymer 239Pu or submicron 239PuO2 aerosols in amounts close to acute, subacute and chronically effective ones. ECG was recorded in standard, amplified and single leads (V3). All calculations were done by lead II. Signs of the right heart overburdening were noted in the presence of the P-pulmonale complex, deep S1 wave or cardiac electrical axis of SI-SII-SIII type. Signs of the right heart overburdening were revealed after inhalation of polimer 239Pu (70%). The absence of similar changes in damage caused by 239Pu could be attributed to its fast resorption from the lungs resulting in more moderate lesion of the respiratory organs.

  18. Extension of 239+240Pu sediment geochronology to coarse-grained marine sediments

    Kuehl, Steven A.; Ketterer, Michael E.; Miselis, Jennifer L.

    2012-01-01

    Sediment geochronology of coastal sedimentary environments dominated by sand has been extremely limited because concentrations of natural and bomb-fallout radionuclides are often below the limit of measurement using standard techniques. ICP-MS analyses of 239+240Pu from two sites representative of traditionally challenging (i.e., low concentration) environments provide a "proof of concept" and demonstrate a new application for bomb-fallout radiotracers in the study of sandy shelf-seabed dynamics. A kasten core from the New Zealand shelf in the Southern Hemisphere (low fallout), and a vibracore from the sandy nearshore of North Carolina (low particle surface area) both reveal measurable 239+240Pu activities at depth. In the case of the New Zealand site, independently verified steady-state sedimentation results in a 239+240Pu profile that mimics the expected atmospheric fallout. The depth profile of 239+240Pu in the North Carolina core is more uniform, indicating significant sediment resuspension, which would be expected in this energetic nearshore environment. This study, for the first time, demonstrates the utility of 239+240Pu in the study of sandy environments, significantly extending the application of bomb-fallout isotopes to coarse-grained sediments, which compose the majority of nearshore regions.

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

    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.

  20. Microscopic Calculations of 240Pu Fission

    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.

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

    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.

  2. Determination of plutonium content in high burnup pressurized water reactor fuel samples and its use for isotope correlations for isotopic composition of plutonium.

    Joe, Kihsoo; Jeon, Young-Shin; Han, Sun-Ho; Lee, Chang-Heon; Ha, Yeong-Keong; Song, Kyuseok

    2012-06-01

    The content of plutonium isotopes in high burnup pressurized water reactor fuel samples was examined using both alpha spectrometry and mass spectrometry after anion exchange separation. The measured values were compared with results calculated by the ORIGEN-2 code. On average, the ratios (m/c) of the measured values (m) over the calculated values (c) were 1.22±0.16 for (238)Pu, 1.02±0.14 for (239)Pu, 1.08±0.06 for (240)Pu, 1.06±0.16 for (241)Pu, and 1.13±0.08 for (242)Pu. Using the Pu data obtained in this work, correlations were derived between the alpha activity ratios of (238)Pu/((239)Pu+(240)Pu), the alpha specific activities of Pu, and the atom % abundances of the Pu isotopes. Using these correlations, the atom % abundances of the plutonium isotopes in the target samples were calculated. These calculated results agreed within a range from 2 to 8% of the experimentally derived values according to the isotopes of plutonium.

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

    Reed, B. Cameron

    2017-01-01

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

  4. Preliminary Study on the Determination of ~(235)U and ~(239)Pu Using Delayed Neutron Counting Method

    2011-01-01

    The preliminary study on the fast measurements of 235U and 239Pu in samples containing 235U, 239Pu and 235U-239Pu mixture using delayed neutron counting method is introduced. All samples were irradiated for 30 s using the 30 kW Miniature Neutron

  5. Conversion electron spectrometry of Pu isotopes with a silicon drift detector.

    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.

  6. Distribution of Pu isotopes and {sup 137}Cs in and around the former soviet union`s Semipalatinsk nuclear test site

    Yamamoto, Masayoshi [Kanazawa Univ., Tatsunokuchi, Ishikawa (Japan). Low Level Radioactivity Laboratory; Hoshi, Masaharu; Takada, Jun; Tsukatani, Tsuneo; Sekerbaev, A.Kh.; Busev, B.I.

    1999-03-01

    This paper is a report on our survey of residual radioactivity, Pu isotopes and {sup 137}Cs, within and without the territory of the Semipalatinsk nuclear test site. Soil samples within the test site were collected at approximately 30 sites along the roads connecting Kurchatov City, ground zero for the first USSR nuclear test, Balapan, Degelen Mountain and Salzhal settlement. Furthermore, outside the test site, the soil was sampled at about 20 sites, including some settlements (Mostik, Dolon, Tchagan, etc.), forest and pasture areas, along the roads from Semipalatinsk City to Kurchatov City and north Korosteli settlement. The contamination levels of long-lived radionuclides, {sup 137}Cs, {sup 238}Pu and {sup 239,240}Pu as well as {sup 240}Pu/{sup 239}Pu atomic ratio in the soil were determined by non-destructive {gamma}-spectrometric method and radiochemical separation followed by {alpha}-spectrometric and/or ICP-MS methods, respectively. The results showed that although {sup 137}Cs was within typical environmental levels except for an areas near ground zero and Balapan, {sup 239,240}Pu was elevated levels contaminated with weapons-grade plutonium in all area we visited. From the stepwise leaching of Pu from the soil, 50-80% of total {sup 239,240}Pu in most samples was found to be tightly incorporated into the soil components which might have been melted at time of detonation. (author)

  7. Plutonium isotopes in the ocean off Japan after Fukushima

    Buesseler, K.; Black, E.; Pike, S. [Woods Hole Oceanographic Institution (United States); Kenna, T. [Lamont-Doherty Earth Observatory (United States); Masque, P. [Universitat Autonoma de Barcelona (Spain)

    2014-07-01

    The Fukushima Dai-ichi nuclear power plants (NPPs) are known to be an unprecedented accidental source of {sup 137}Cs, {sup 134}Cs and other volatile radionuclides to the ocean. Much less is known however about the extent of input of refractory radionuclides such as plutonium to the environment. Limited available data from land soils and vegetation, suggest at least some atmospheric delivery of particulate Pu but at very low levels relative to pre-existing fallout sources. To resolve Fukushima derived Pu from weapons testing derived Pu, information regarding the Pu isotopic composition is needed. The {sup 240}Pu/{sup 239}Pu atom ratio determined by mass spectrometric techniques, and the {sup 238}Pu/{sup 239,240}Pu activity ratio as measured by alpha counting are diagnostic with respect to Pu source. We review and present new data on the Pu isotopic ratios and concentrations in the oceans, combining several data sets on dissolved (from bottle sampling), suspended particulates (from filtration), sinking particles (from sediment traps) and seafloor sediments (from cores) to look for the Fukushima Pu signal. In most samples, the {sup 240}Pu/{sup 239}Pu ratios are in the range of 0.20-0.23, characteristic of Pu ocean signal which is a combination of global fallout with a characteristic ratio of 0.18 and local fallout from the Pacific Proving Grounds with ratios higher than 0.24, and known from prior studies to influence the ocean off Japan. In 2011, in surface ocean waters, we found ratios {sup 240}Pu/{sup 239}Pu >0.3, which implies a component of Fukushima Pu had been delivered to the ocean, given NPP derived end-member ratios of 0.35-0.45. Fukushima derived Pu was not found deeper in the water column or even at all stations, consistent with its rapid removal from the ocean and the high background of pre-existing Pu in the waters and sediments, masking the new Fukushima sources. With this data a mass balance will be made between Pu from global fallout, local fallout and

  8. Vertical distributions of plutonium isotopes in marine sediment cores off the Fukushima coast after the Fukushima Dai-ichi Nuclear Power Plant accident

    W. T. Bu

    2013-04-01

    Full Text Available The Fukushima Dai-ichi Nuclear Power Plant (FDNPP accident led to the release of large amounts of radionuclides into the atmosphere as well as direct discharges into the sea. In contrast to the intensive studies on the distribution of the released high volatility fission products, such as 131I, 134Cs and 137Cs, similar studies of the actinides, especially the Pu isotopes, are limited. To obtain the vertical distribution of Pu isotopes in marine sediments and to better assess the possible contamination of Pu from the FDNPP accident in the marine environment, we determined the activities of 239+240Pu and 241Pu as well as the atom ratios of 240Pu/239Pu and 241Pu/239Pu in sediment core samples collected in the western North Pacific off Fukushima from July 2011 to July 2012. We also measured surface sediment samples collected from seven Japanese estuaries before the FNDPP accident to establish the comprehensive background baseline data. The observed results of both the Pu activities and the Pu atom ratios for the sediments in the western North Pacific were comparable to the baseline data, suggesting that the FDNPP accident did not cause detectable Pu contamination to the studied regions prior to the sampling time. The Pu isotopes in the western North Pacific 30 km off the Fukushima coast originated from global fallout and Pacific Proving Ground close-in fallout.

  9. Modeling and production of {sup 240}Am by deuteron-induced activation of a {sup 240}Pu target

    Finn, Erin C., E-mail: Erin.Finn@pnnl.gov; McNamara, Bruce, E-mail: Bruce.McNamara@pnnl.gov; Greenwood, Larry, E-mail: Larry.Greenwood@pnnl.gov; Wittman, Richard, E-mail: Richard.Wittman@pnnl.gov; Soderquist, Charles, E-mail: Chuck.Soderquist@pnnl.gov; Woods, Vincent, E-mail: Vincent.Woods@pnnl.gov; VanDevender, Brent, E-mail: Brent.Vandevender@pnnl.gov; Metz, Lori, E-mail: Lori.Metz@pnnl.gov; Friese, Judah, E-mail: Judah.Friese@pnnl.gov

    2015-04-15

    A novel reaction pathway for production of {sup 240}Am is reported. Models of reaction cross-sections in EMPIRE II suggest that deuteron-induced activation of a {sup 240}Pu target produces maximum yields of {sup 240}Am from 11.5 MeV incident deuterons. This activation had not been previously reported in the literature. A {sup 240}Pu target was activated under the modeled optimum conditions to produce {sup 240}Am. The modeled cross-section for the {sup 240}Pu(d, 2n){sup 240}Am 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.

  10. Neutron Resonance Parameters and Covariance Matrix of 239Pu

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

    2008-08-01

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

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

    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.

  12. Chronology of Pu isotopes and {sup 236}U in an Arctic ice core

    Wendel, C.C., E-mail: cato.wendel@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Oughton, D.H., E-mail: deborah.oughton@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Lind, O.C., E-mail: ole-christian.lind@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Skipperud, L., E-mail: lindis.skipperud@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway); Fifield, L.K., E-mail: keith.fifield@anu.edu.au [Department of Nuclear Physics, Australian National University, Canberra ACT 0200 (Australia); Isaksson, E., E-mail: elisabeth.isaksson@npolar.no [Norwegian Polar Institute, Fram Centre, Hjalmar Johansens Gate 14, N9296 Tromsø (Norway); Tims, S.G., E-mail: steve.tims@anu.edu.au [Department of Nuclear Physics, Australian National University, Canberra ACT 0200 (Australia); Salbu, B., E-mail: brit.salbu@umb.no [Isotope Laboratory, Department of Plant and Environmental Sciences, Agricultural University of Norway, P.O. Box 5003, N-1432 Aas (Norway)

    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 {sup 236}U, {sup 239}Pu, and {sup 240}Pu concentrations, and atom ratios, measured by accelerator mass spectrometry in a 28.6 m 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 {sup 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 {sup 239+240}Pu ranged from 0.008 to 0.254 mBq cm{sup −2} and {sup 236}U from 0.0039 to 0.053 μBq cm{sup −2}. Concentrations varied in concordance with {sup 137}Cs concentrations in the same ice core. In contrast to previous published results, the concentrations of Pu and {sup 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 {sup 240}Pu/{sup 239}Pu ratio ranged from 0.15 to 0.19, and {sup 236}U/{sup 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 {sup 236}U concentrations and {sup 236}U/{sup 239}Pu atom ratios in the Arctic and in ice cores. - Highlights: • Concentrations and atom ratios of Pu and {sup 236}U determined in an Arctic ice core. • Concentrations of U and Pu found to be higher pre- than post-moratorium. • U and Pu concentrations

  13. Medida de isótopos de Plutonio, 239Pu y 240Pu, mediante espectrometría de masas con aceleradores de baja energía

    Chamizo Calvo, Elena

    2009-01-01

    El primer bloque, sobre la descripción de la técnica y de los dos sistemas empleados, comprende los Capítulos 2, 3 y 4. En el Capítulo 2 presentaremos los fundamento s del AMS de baja energía y las características de diseño de sus instalaciones. De esta forma, veremos que un sistema compacto de AMS no es simplemente una versión a escala de uno convencional, y justificaremos las razones por las que la comunidad científica se ha visto obligada durante 20 años a usar grandes aceleradores. En el ...

  14. Gamma-ray Output Spectra from 239Pu Fission

    Ullmann John

    2015-01-01

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

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

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

    2016-10-01

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

  16. Multi-collector Isotope Ratio Mass Spectrometer -- Operational Performance Report

    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.

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

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

    2016-09-01

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

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

    Suseno, Heny; Wisnubroto, Djarot S.

    2014-03-01

    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 239/240Pu 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 239/240Pu 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 239/240Pu in Bangka Island and Muria Peninsula were range from 0.013 to 0.021 Bq.kg-1 and 0.018 to 0.024 Bq.kg-1 respectively. The water baseline concentration this isotope were range from 2.73 to 4.05 mBq.m-3 and 2.98 to 4.50 mBq.m-3.

  19. 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

    Suseno, Heny, E-mail: henis@batan.go.id [Radioactive Waste Technology Center - The Indonesian National Nuclear Energy Agency (Indonesia); Wisnubroto, Djarot S. [The Indonesian National Nuclear Energy Agency (Indonesia)

    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}.

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

    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

  1. The plutonium isotopic composition of marine biota on Enewetak Atoll: a preliminary assessment.

    Hamilton, Terry F; Martinelli, Roger E; Kehl, Steven R; McAninch, Jeffrey E

    2008-10-01

    We have determined the level and distribution of gamma-emitting radionuclides, plutonium activity concentrations, and 240Pu/239Pu atom ratios in tissue samples of giant clam (Tridacna gigas and Hippopus hippopus), a top snail (Trochus nilaticas) and sea cucumber (Holothuria atra) collected from different locations around Enewetak Atoll. The plutonium isotopic measurements were performed using ultra-high sensitivity accelerator mass spectrometry (AMS). Elevated levels of plutonium were observed in the stomachs (includes the stomach lining) of Tridacna clam (0.62 to 2.98 Bq kg(-1), wet wt.), in the soft parts (edible portion) of top snails (0.25 to 1.7 Bq kg(-1)), wet wt.) and, to a lesser extent, in sea cucumber (0.015 to 0.22 Bq kg(-1), wet wt.) relative to muscle tissue concentrations in clam (0.006 to 0.021 Bq kg(-1), wet wt.) and in comparison with previous measurements of plutonium in fish. These data and information provide a basis for re-evaluating the relative significance of dietary intakes of plutonium from marine foods on Enewetak Atoll and, perhaps most importantly, demonstrate that discrete 240Pu239Pu isotope signatures might well provide a useful investigative tool to monitor source-term attribution and consequences on Enewetak Atoll. One potential application of immediate interest is to monitor and assess the health and ecological impacts of leakage of plutonium (as well as other radionuclides) from a low-level radioactive waste repository on Runit Island relative to background levels of fallout contamination in Enewetak Atoll lagoon.

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

    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.

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

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

    2016-10-01

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

  4. Rapid Separation of 239Pu and 241Am in Environment Soil Samples

    YANG; Jin-ling; ZHANG; Ji-qiao; HUANG; Kun; DING; You-qian; ZHAO; Ya-ping

    2015-01-01

    In the nuclear sites and the surroundings which are the main environmental monitored area,the allowances of 239Pu and 241 Am are less than0.1Bq/g as the extremely toxic species.So it is very important and practical to establish rapid and convenient analysis methods for them.With

  5. Yield-Energy Evaluation of 85Kr of 239Pu+n Fission

    2008-01-01

    <正>The yields of 85Kr, the important production of the 239Pu fission, were re-evaluated over the incident neutron energy 1-15 MeV, based upon all the experimental data. The yields as function of energ

  6. Solid Phase Extraction Disk Procedure to Determine 239Pu in Soils

    ZHANG Ji-qiao;ZHAO Ya-ping;DING You-qian;ZHANG Sheng-dong;YANG Jin-ling

    2016-11-01

    Full Text Available 239Pu in many soil samples should be analyzed to survey radioactive pollution level in nuclear facilities and its affinity environment efficiently. In order to input the opt conditions for column experiment, the experiments of the static adsorption coefficient of 239Pu to solid phase extraction disk with different contact time, concentration of HNO3 and different temperature were carried out. The chemical procedure for the rapid separation and determination of 239Pu in soils had been formulated, which using solid phase extraction disk (EmporeTM Anion Exchange-SR as extraction material and liquid scintillation spectrometry counting as measurement. In the procedure, soil sample usage was 10 g, and were leached by 8 mol/L HNO3, the chemical recovery of the procedure was about 78.9%, and the minimum detectable concentration was 3.7 Bq/kg. It took less than 3 hours once and the presence of 137Cs, 90Sr-90Y and natural uranium, 241Am, 99Tc did not interfere with the procedure, owning high DF of them. The procedure can be used extensively in determination of 239Pu in soils.

  7. Angular distributions of low-spin states in {sup 240}Pu by means of the {sup 242}Pu(p,t){sup 240}Pu reaction

    Spieker, Mark; Endres, Janis; Pascu, Sorin; Zilges, Andreas [Koeln Univ. (Germany). Inst. fuer Kernphysik; Bucurescu, Dorel; Zamfir, Nicolae-Victor [Horia Hulubei National Institute of Physics and Nuclear Engineering, Bucharest (Romania); Faestermann, Thomas [Physik Department, Technische Universitaet Muenchen (Germany); Hertenberger, Ralf; Wirth, Hans-Friedrich [Fakultaet fuer Physik, Ludwig-Maximilians-Universitaet Muenchen (Germany)

    2013-07-01

    Since recent experimental and theoretical studies revealed the importance of octupole correlations in the actinide region and especially in {sup 240}Pu, a {sup 242}Pu(p,t){sup 240}Pu experiment has been conducted at the Q3D magnetic spectrograph of the Maier-Leibnitz laboratory in Munich. Excited states in {sup 240}Pu were investigated up to an excitation energy of 3 MeV. Angular distributions have been measured at 9 laboratory angles between 5 {sup circle} and 40 {sup circle}. The comparison of the experimental angular distributions with DWBA calculations allowed the assignment of several low-spin states. Most of them were seen for the first time. The experimental data, especially the data on the 21 J{sup π}= 0{sup +} states, are presented and discussed in the framework of the spdf-version of the Interacting Boson Model.

  8. Characterization of a neutron source of {sup 239}PuBe; Caracterizacion de una fuente de neutrones de {sup 239}PuBe

    Hernandez V, R.; Chacon R, A.; Hernandez D, V. M.; Mercado, G. A.; Vega C, H. R. [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Calle Cipres No. 10, Fracc. La Penuela, 98068 Zacatecas (Mexico); Ramirez G, J. [Instituto Nacional de Estadistica Geografia e Informatica, Direccion General de Innovacion y Tecnologia de Informacion, Av. Heroes de Nacozari Sur 2301, Fracc. Jardines del Parque, 20276 Aguascalientes (Mexico)], e-mail: ruben_zac@yahoo.com

    2009-10-15

    The spectrum equivalent dose and environmental equivalent dose f a {sup 239}PuBe source have been determined. The appropriate handling of a neutron source depends on the knowledge of its characteristics, such as its energy distribution, total rate of flowing and dosimetric magnitudes. In many facilities have not spectrometer that allows to determine the spectrum and then area monitors are used that give a dosimetric magnitude starting from measuring the flowing rate and the use of conversion factors, however this procedure has many limitations and it is preferable to measure the spectra and starting from this information the interest dosimetric magnitudes are calculated. In this work a Bonner sphere spectrometer has been used with a {sup 6}LiI(Eu) scintillator obtaining the count rates that produce, to a distance of 100 cm, a {sup 239}PuBe source of 1.85E(11) Bq. The spectrum was reconstructed starting from the count rates using BUNKIUT code and response matrix UTA4. With the spectrum information was calculated the source intensity, total flow, energy average, equivalent dose rate, environmental equivalent dose rate, equivalent dose coefficient and environmental equivalent dose coefficient. By means of two area monitors for neutrons, Eberline ASP-1 and LB 6411 of Berthold the equivalent dose and environmental equivalent dose were measured. The determinate values were compared with those reported in literature and it found that are coincident inside 17%. (Author)

  9. High-/sup 240/Pu sector experiments in ZPPR assembly 4

    McFarlane, H F; Beck, C L

    1976-12-01

    The complete high-/sup 240/Pu fuel experiment in ZPPR assembly 4 is reviewed. Results of criticality, enrichment, small-sample perturbation, sodium void, /sup 238/U Doppler, control rod substitution and reaction rate measurements are presented. Comparison of these measured values with calculated results are included where possible. The relationship between the ZPPR high-/sup 240/Pu fuel experiments and the results obtained in previous critical experience is considered.

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

    Suzuki, K; Sekimoto, H; Ishigure, N

    2001-01-01

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

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

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

    2013-04-01

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

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

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

    2016-09-01

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

  13. Measurement of the fission cross-section of $^{240}$Pu and $^{242}$Pu at CERN's n_TOF Facility

    Pavlik, A F; Gonzalez romero, E M

    The n_TOF Collaboration proposes to continue the fission program, already started in 2002-2004, taking advantage of the newly constructed Work Sector Type A, with the measurement of the two isotopes : $^{240}$ Pu and $^{242}$ Pu. They are both of major importance for reactor physics applications and are included in the Nuclear Energy Agency (NEA) High Priority List [1], in the NEA WPEC Subgroup 26 Report on the accuracy of nuclear data for advanced reactor designe [2] and in the EU 6$^{th}$ Framework Programme IP-EUROTRANS/NUDATRA reports [3]. Based on those requests, the measurement of the fission cross-section of the two Pu isotopes is one of the objectives of the project ANDES of the FP7 EURATOM program [4].

  14. Transuranic advanced disposal systems: preliminary /sup 239/Pu waste-disposal criteria for Hanford

    Kennedy, W.E. Jr.; Aaberg, R.L.; Napier, B.A.; Soldat, J.K.

    1982-09-01

    This report contains the draft results of a study sponsored by the US Department of Energy (DOE) to determine preliminary /sup 239/Pu waste disposal criteria for the Hanford Site. The purpose of this study is to provide a preliminary evaluation of the feasibility of various defense TRU advanced disposal options at the Hanford Site. Advanced waste disposal options include those developed to provide greater confinement than provided by shallow-land burial. They will be used to complement the waste geologic disposal in achieving permanent disposal of selected TRU wastes. An example systems analysis is discussed with assumed performance objectives and Hanford-specific disposal conditions, waste forms, site characteristics, and engineered barriers. Preliminary waste disposal criteria for /sup 239/Pu are determined by applying the Allowable Residual Contamination Level (ARCL) method. This method is based on compliance with a radiation dose rate limit through a site-specific analysis of the potential for radiation exposure to individuals. A 10,000-year environmental performance period is assumed, and the dose rate limit for human intrusion is assumed to be 500 mrem/yr to any exposed individual. Preliminary waste disposal criteria derived by this method for /sup 239/Pu in soils at the Hanford Site are: 0.5 nCi/g in soils between the surface and a depth of 1 m, 2200 nCi/g of soil at a depth of 5 m, and 10,000 nCi/g of soil at depths 10 m and below. These waste disposal criteria are based on exposure scenarios that reflect the dependence of exposure versus burial depth. 5 figures, 7 tables.

  15. Validation of new {sup 240}Pu cross section and covariance data via criticality calculation

    Kim, Do Heon; Gil, Choong-Sup; Kim, Hyeong Il; Lee, Young-Ouk, E-mail: kimdh@kaeri.re.kr, E-mail: csgil@kaeri.re.kr, E-mail: hikim@kaeri.re.kr, E-mail: yolee@kaeri.re.kr [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of); Leal, Luiz C.; Dunn, Michael E., E-mail: leallc@ornl.gov, E-mail: dunnme@ornl.gov [Oak Ridge National Laboratory, TN (United States)

    2011-07-01

    Recent collaboration between KAERI and ORNL has completed an evaluation for {sup 240}Pu neutron cross section with covariance data. The new {sup 240}Pu cross section data has been validated through 28 criticality safety benchmark problems taken from the ICSBEP and/or CSEWG specifications with MCNP calculations. The calculation results based on the new evaluation have been compared with those based on recent evaluations such as ENDF/B-VII.0, JEFF-3.1.1, and JENDL-4.0. In addition, the new {sup 240}Pu covariance data has been tested for some criticality benchmarks via the DANTSYS/SUSD3D-based nuclear data sensitivity and uncertainty analysis of k{sub eff}. The k{sub eff} uncertainty estimates by the new covariance data has been compared with those by JENDL-4.0, JENDL-3.3, and Low-Fidelity covariance data. (author)

  16. 137Cs and (239+240)Pu levels in the Asia-Pacific regional seas.

    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.

  17. Transuranic advanced disposal systems: preliminary /sup 239/Pu waste-disposal criteria for Hanford

    Kennedy, W.E. Jr.; Napier, B.A.; Soldat, J.K.

    1982-08-01

    An evaluation of the feasibility and potential application of advanced disposal systems is being conducted for defense transuranic (TRU) wastes at the Hanford Site. The advanced waste disposal options include those developed to provide greater confinement than provided by shallow-land burial. An example systems analysis is discussed with assumed performance objectives and various Hanford-specific disposal conditions, waste forms, site characteristics, and engineered barriers. Preliminary waste disposal criteria for /sup 239/Pu are determined by applying the Allowable Residual Contamination Level (ARCL) method. This method is based on compliance with a radiation dose rate limit through a site-specific analysis of the potential for radiation exposure to individuals. A 10,000 year environmental performance period is assumed, and the dose rate limit for human intrusion is assumed to be 500 mrem/y to any exposed individual. Preliminary waste disposal criteria derived by this method for /sup 239/Pu in soils at the Hanford Site are: 0.5 nCi/g in soils between the surface and a depth of 1 m, 2200 nCi/g of soil at a depth of 5 m, and 10,000 nCi/g of soil at depths 10 m and below. These waste disposal criteria are based on exposure scenarios that reflect the dependence of exposure versus burial depth. 2 figures, 5 tables.

  18. 239Pu(n,2n) 238Pu cross section inferred from IDA calculations and GEANIE measurements

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

    2000-09-01

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

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

    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 (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+240Pu activities, and hence contain most or all of the cumulative deposition

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

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

    2010-03-31

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

  1. Investigation of zircon/zirconia ceramics doped with {sup 239}Pu and {sup 238}Pu

    Burakov, B.E.; Anderson, E.B.; Zamoryanskaya, M.V.; Nikolaeva, E.V.; Strykanova, E.E.; Yagovkina, M.A. [V.G. Khlopin Radium Institute, Saint Petersburg (Russian Federation)

    2001-07-01

    Several samples of crystalline double-phase ceramics based on zircon, (Zr,Pu)SiO{sub 4} and zirconia, (Zr,Pu)O{sub 2}, were synthesized by sintering in air, precursors containing approximately 5-6 and 10 wt% {sup 239}Pu, respectively. One sample doped with 5-6 wt% {sup 238-39-40}Pu was also obtained under the same conditions. All ceramic samples were studied by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), electron probe microanalysis (EPMA) and MCC-1 leach test in deionized water at 90 C. Results indicate that even radiation damaged zircon/zirconia ceramics retain high chemical resistance and mechanical durability. (author)

  2. Dependence of dose coefficients for {sup 239}Pu on transfer rates and absorption parameters

    Suzuki, K.; Sekimoto, H. [Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology, Tokyo (Japan); Ishigure, N. [Division of Radiotoxicology and Protection, National Institute of Radiological Sciences, Chiba (Japan)

    2000-05-01

    As it is reported of the biokinetic models and parameter values of the International Commission on Radiological Protection (ICRP) for dose estimation have uncertainties owing to insufficiency of human data. For most radionuclides, the data underlying such models and parameters of ICRP usually depend on animal experiments. Moreover, these values or model parameter are also greatly different between mammalian species. Recently, various radiation protection organizations are considering the biokinetic uncertainties from standpoints of data's sources, quality and completeness. In practice, a sensitivity analysis of doses to parameters is significant for the purpose of risk assessment. In general, movement or material in the body is depicted as a system of first-order processes, and parameter values are expressed as transfer rates between compartments. In this study, we made a code to reproduce the ICRP's dose coefficients for {sup 239}Pu, which is one of the most important elements for occupational exposure and its effective dose is much concerned with its own distribution in the body for dominance of alpha-decay. By using this code, we modified each transfer rate in a factor of 2, 3 and 4 in order to evaluate the effects, and calculated the sensitivities of effective doses due to these changes. Additionally, we examined the effects of modification of absorption parameters f{sub r}, S{sub r} and S{sub s}, which represent the absorption of particles from respiratory tract into blood. Consequently, the transfer rates that give a large sensitivity were specified, and it was shown that changes of transfer rates and absorption parameters are not so influential on effective doses for {sup 239}Pu in many cases. (author)

  3. Spatial statistical analysis of contamination level of 241Am and 239Pu, Thule, North-West Greenland

    Strodl Andersen, J. (JSA EnviroStat (Denmark))

    2011-10-15

    A spatial analysis of data on radioactive pollution on land at Thule, North-West Greenland is presented. The data comprises levels of 241Am and 239,240Pu on land. Maximum observed level of 241Am is 2.8x105 Bq m-2. Highest levels were observed near Narsaarsuk. This area was also sampled most intensively. In Groennedal the maximum observed level of 241Am is 1.9-104 Bq m-2. Prediction of the overall amount of 241Am and 239,240Pu is based on grid points within the range from the nearest measurement location. The overall amount is therefore highly dependent on the model. Under the optimal spatial model for Narsaarsuk, within the area of prediction, the predicted total amount of 241Am is 45 GBq and the predicted total amount of 239,240Pu is 270 GBq. (Author)

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

    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 ).

  5. Measurement of the ${240}$Pu(n,f) reaction cross-section

    Following proposal CERN-INTC-2010-042 / INTC-P-280 (“Measurement of the fission cross-section of $^{240}$Pu and $^{242}$Pu at CERN’s n_TOF Facility”), the parallel measurement of the $^{240}$Pu(n,f) and $^{242}$Pu(n,f) reaction cross-sections was carried out at n_TOF EAR-1. While the $^{242}$Pu measurement was successful, unexpected sample-induced damage to the detectors caused by the high α-activity of the 240Pu samples resulted in a deterioration of the detector performance over the data taking period of several months, which compromised the measurement. This obstacle can be eliminated by performing the measurement in EAR-2, where the higher neutron flux will allow collecting data in a much shorter time, thus preventing the degradation of the detectors. In addition to this obvious advantage, the measurement would also benefit from the stronger suppression of the sample-induced α-background, due to the shorter times-of-flight involved.

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

    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.

  7. 239Pu Prompt Fission Neutron Spectra Impact on a Set of Criticality and Experimental Reactor Benchmarks

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

    2014-04-01

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

  8. {sup 238}Pu, {sup 239+240}Pu and {sup 241}Am levels in the terrestrial and aquatic environment of the Loire and Garonne rivers basins (France)

    Rousseau, G.; Mokili, M.B.; Le Roy, C.; Pagano, V. [SUBATECH/IN2P3 (France); Gontier, G.; Boyer, C. [EDF-DPI-DIN-CIDEN (France); Chardon, P. [CNRS/IN2P3 (France); Hemidy, P.Y. [EDF-DPN-UNIE-GPRE-IEV (France)

    2014-07-01

    Plutonium and americium long-lived alpha emitter isotopes can be found in the environment because of atmospheric global fallout due to thermonuclear tests performed between 1945 and 1980, to the American SNAP 9A satellite explosion in 1964, to the Chernobyl nuclear power plant accident,... In France, the nuclear safety authority does not allow the release of artificial alpha emitters from nuclear power plants. Thus, monitoring is performed to verify the absence of these alpha emitters in liquid discharges to respect the limits set by the regulations. These thresholds ensure a very low dosimetric impact to the population compared to other radionuclides. With the objective of environmental monitoring around nuclear facilities, activity measurements of long-lived alpha emitters are carried out to detect the traces of these radionuclides. Analysis of low activity by alpha spectrometry after chemical steps were performed and used to determine the {sup 238}Pu, {sup 239+240}Pu and {sup 241}Am activities on a large set of environmental solid samples likely to be encountered in environmental monitoring as soils, sediments, terrestrial and aquatic bio-indicators. The samples collected in the terrestrial and aquatic environment of the Loire and Garonne rivers basins (France) was investigated for the 2009-2014 period. It was found that the mean activity concentration of the most frequently detected was for the radionuclide {sup 238}Pu: from <0.00031 to 0.0061 Bq/kg dry in terrestrial samples and from <0.00086 to 0.011 Bq/kg dry in aquatic samples; for the radionuclide {sup 239+240}Pu: from 0.00041 to 0.150 Bq/kg dry in terrestrial samples and from 0.0023 to 0.240 Bq/kg dry in aquatic samples and for the radionuclide {sup 241}Am: from <0.00086 to 0.087 Bq/kg dry in terrestrial samples and from 0.0022 to 0.120 Bq/kg dry in aquatic samples. {sup 238}Pu/{sup 239+240}Pu and {sup 241}Am/{sup 239+240}Pu ratios determined are in accordance with an environmental contamination due to

  9. Using 239Pu as a tracer for fine sediment sources in the Daly River, Northern Australia

    Lal, R.; Fifield, L. K.; Tims, S. G.; Wasson, R. J.; Howe, D.

    2015-04-01

    The Daly River drains a large (52500 km2) and mainly undisturbed catchment in the Australian wet-dry tropics. Clearing and cropping since 2002 have raised concerns about possible increased sediment input into the river and motivated this study of its fine sediment sources. Using 239Pu as a tracer it is shown that the fine sediments originate mainly from erosion by gullying and channel change. Although the results also indicate that the surface soil contribution to the river channel sediments from sheet erosion has increased to 5-22% for the Daly River and 7-28% for the Douglas River (a tributary of the Daly River) in 2009 vs. 3-6% for the Daly River and 4-9% for the Douglas River in 2005. This excess top soil likely originates from thecleared land adjacent to the Daly River since 2005. However, channel widening largely as a result of hydrologic change is still the dominant sediment source in this catchment.

  10. Using 239Pu as a tracer for fine sediment sources in the Daly River, Northern Australia

    Lal R.

    2015-01-01

    Full Text Available The Daly River drains a large (52500 km2 and mainly undisturbed catchment in the Australian wet–dry tropics. Clearing and cropping since 2002 have raised concerns about possible increased sediment input into the river and motivated this study of its fine sediment sources. Using 239Pu as a tracer it is shown that the fine sediments originate mainly from erosion by gullying and channel change. Although the results also indicate that the surface soil contribution to the river channel sediments from sheet erosion has increased to 5-22% for the Daly River and 7-28% for the Douglas River (a tributary of the Daly River in 2009 vs. 3-6% for the Daly River and 4-9% for the Douglas River in 2005. This excess top soil likely originates from thecleared land adjacent to the Daly River since 2005. However, channel widening largely as a result of hydrologic change is still the dominant sediment source in this catchment.

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

    Wen, Xianfei; Yang, Haori

    2016-06-01

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

  12. Detection of long-lived plutonium isotopes in environmental samples by Accelerator Mass Spectrometry (AMS)

    Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Gomez Guzman, Jose Manuel; Korschinek, Gunther; Ludwig, Peter [Technische Universitaet Muenchen (Germany); Shinonaga, Taeko [Helmholtz Zentrum Muenchen (Germany)

    2013-07-01

    The Plutonium isotopes {sup 239}Pu (T{sub 1/2}=2.4.10{sup 4}a), {sup 240}Pu (T{sub 1/2}=6.5.10{sup 3}a) and {sup 242}Pu (T{sub 1/2}=3.7.10{sup 5}a) are anthropogenic radionuclides emitted into the environment by nuclear activities. Pu is accumulated in the human body and hence, poses a considerable hazard to human health. Due to the long half-lives, these isotopes are present in the biosphere on large time scales and a build-up can be expected. Therefore it is important to study the contamination pathway of Pu into the drinking water. At the Maier-Leibnitz-Laboratory in Munich a method to detect long-lived Pu isotopes by Accelerator Mass Spectrometry (AMS) is being developed. AMS requires only few milligrams of sample material, which is a substantial advantage over decay counting techniques. Consequently, more samples from different locations can be taken which is essential when searching for locally increased Pu concentrations as in the Pacific Ocean after the Fukushima accident in March 2011. Samples from different locations in the Pacific Ocean and from the snow-hydrosphere are planned to be investigated by AMS. The principle detection method using AMS and an overview of the status of the project is presented.

  13. Probing energy dissipation, γ-ray and neutron multiplicity in the thermal neutron-induced fission of {sup 239}Pu

    Pahlavani, M.R.; Mirfathi, S.M. [University of Mazandaran, Department of Nuclear Physics, Faculty of Basic Science, Babolsar (Iran, Islamic Republic of)

    2016-04-15

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

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

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

    2013-01-01

    Surface and soil core samples from northeast China were analyzed for Pu isotopes. The measured 240Pu/239Pu atomic ratios and 239 1 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 an...

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

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

    2011-07-01

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

  16. {sup 239+240}Pu in the Barents Sea Regions. Sources and radioecological assessment

    Iosjpe, Mikhail [Norwegian Radiation Protection Authority, P.O. Box 55, N-1332 Oesteraas (Norway)

    2014-07-01

    The radioecological assessment for {sup 239+240}Pu in the Barents sea regions was made using the compartment modelling approach. The following sources of radioactive contamination were under consideration: global fallout from atmospheric testing of nuclear weapons, transport of {sup 239+240}Pu from the Sellafield and La Hauge nuclear plants and underwater testing of nuclear weapons in Chernaya Bay, Novaya Zemlya. The box model developed at NRPA uses a modified approach for compartmental modeling, which takes into account the dispersion of radionuclides over time. The box structures for surface, mid-depth and deep water layers have been developed based on the description of polar, Atlantic and deep waters in the Arctic Ocean and the Northern Seas, as well as site-specific information for the boxes. The volume of the three water layers in each box has been calculated using detailed bathymetry together with Geographical Information Systems. The box model includes the processes of advection of radioactivity between compartments, sedimentation, diffusion of radioactivity through pore water in sediments, resuspension, mixing due to bioturbation, particle mixing and a burial process for radionuclides in deep sediment layers. Radioactive decay is calculated for all compartments. The contamination of biota is further calculated from the known radionuclide concentrations in filtered seawater in the different water regions. Doses to man are calculated on the basis of seafood consumptions, in accordance with available data for seafood catches and assumptions about human diet in the respective areas. Dose to biota are determined on the basis of calculated radionuclide concentrations in marine organisms, water and sediment, using dose conversion factors. Results of the calculations show that atmospheric deposition is the dominant source for the Barents Sea, except for the Chernaya Bay region. It is also demonstrated that the impact of the Sellafield nuclear facilities has

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

    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.

  18. Fission Barrier for 240Pu in the Quadrupole Constrained Relativistic Mean Field Approach

    L(U) Hong-Feng; GENG Li-Sheng; MENG Jie

    2006-01-01

    @@ The fission barrier for 240Pu is investigated beyond the second saddle point in the potential energy surface by the constrained relativistic mean field method with the newly proposed parameter set PK1. The microscopic correction for the centre-of-mass motion is essential to provide the correct potential energy surface. The shell effects that stabilize the nuclei against the fission is also investigated by the Strutinsky method. The shapes for the ground state, fission isomer and saddle-points, etc, are studied in detail.

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

    Sadhukhan, Jhilam; Schunck, Nicolas

    2016-01-01

    In this letter, we outline a methodology to calculate microscopically mass and charge distributions of spontaneous fission yields. We combine the multi-dimensional 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 characteristics.

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

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

    2010-01-15

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

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

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

    2009-07-23

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

  2. Alpha-particle emission probabilities in the decay of {sup 240}Pu

    Sibbens, G., E-mail: goedele.sibbens@ec.europa.e [European Commission, Joint Research Centre, Institute for Reference Materials and Measurements, Retieseweg 111, B-2440 Geel (Belgium); Pomme, S.; Altzitzoglou, T. [European Commission, Joint Research Centre, Institute for Reference Materials and Measurements, Retieseweg 111, B-2440 Geel (Belgium); Garcia-Torano, E. [Laboratorio de Metrologia de Radiaciones Ionizantes, CIEMAT, Avda. Complutense 22, 28040 Madrid (Spain); Janssen, H.; Dersch, R.; Ott, O. [Physikalisch-Technische Bundesanstalt (PTB), Bundesallee 100, 38116 Braunschweig (Germany); Martin Sanchez, A. [Departamento de Fisica, Universidad de Extremadura, Badajoz, E-06071 (Spain); Rubio Montero, M.P. [Departamento de Fisica Aplicada, Universidad de Extremadura, Merida, Badajoz, E-06800 (Spain); Loidl, M. [Laboratoire National Henri Becquerel, LNE/CEA-LIST, 91191 Gif-sur-Yvette (France); Coron, N.; Marcillac, P. de [Institut d' Astrophysique Spatiale, CNRS, 91405 Orsay Campus (France); Semkow, T.M. [Wadsworth Center, New York State Department of Health, Albany, NY 12201 (United States)

    2010-07-15

    Sources of enriched {sup 240}Pu were prepared by vacuum evaporation on quartz substrates. High-resolution alpha-particle spectrometry of {sup 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.

  3. Determination of Fission Product Yields of 235U, 238U and 239Pu for Neutron Energies from 0.5 to 14.8 MeV

    Gooden, Matthew; Arnold, Charles; Becker, John; Bhatia, Chitra; Bhike, Megha; Fowler, Malcolm; Howell, Calvin; Kelley, John; Stoyer, Mark; Tonchev, Anton; Tornow, Werner; Vieira, Dave; Wilhelmy, Jerry

    2014-03-01

    A joint TUNL-LANL-LLNL collaboration has been formed to study the issue of possible energy dependences for certain fission product isotopes. Work has been carried out at the TUNL 10 MV Tandem accelerator which produces nearly mono-energetic neutrons via either 2H(d,n)3He,3H(d,n)4He,or3H(p,n)3He reactions. Three dual fission ionization chambers dedicated to 235U, 238U and 239Pu thick target foils and thin monitor foils respectively, were exposed to the neutron beams. After irradiation, thick target foils were gamma counted over a period of 1-2 months and characteristic gamma rays from fission products were recorded using HPGe detectors at TUNL's low background counting area. Using the dual fission chambers, relative fission product yield were determined at a high precision of 2-3 % as well as absolute fission product yields at a lower precision of 5-6 %. Preliminary results will be presented for a number of fission product isotopes over the incident neutron energy range of 0.5 to 14.8 MeV.

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

    Dion, Michael P., E-mail: michael.dion@pnnl.gov; Miller, Brian W.; Warren, Glen A.

    2016-09-11

    A technique to determine the isotopic constituents of a mixed actinide sample has been proposed by a coincident alpha-conversion electron measurement. This presents a unique signature to allow the unfolding of isotopes that possess overlapping alpha particle energy and reduce backgrounds of an unseparated sample. The work presented here are results of conversion electron spectroscopy of {sup 241}Am, {sup 238}Pu and {sup 239}Pu using a dual-stage peltier-cooled 25 mm{sup 2} silicon drift detector and alpha spectroscopy with a passivated ion implanted planar silicon detector. The conversion electron spectra were evaluated from 20–55 keV based on fits to the dominant conversion electron emissions, which allowed the relative conversion electron emission intensities to be determined. These measurements provide crucial singles spectral information and calibration to aid in the coincident measurement approach. Furthermore, an alpha-conversion electron spectrometer was assembled using the silicon based detectors described and results of a coincident spectrum analysis is reported for {sup 241}Am.

  5. Spatial statistical analysis of contamination level of 241Am and 239Pu, Thule, North-West Greenland

    Strodl Andersen, Jens

    A spatial analysis of data on radioactive pollution on land at Thule, North-West Greenland is presented. The data comprises levels of 241Am and 239,240Pu on land. Maximum observed level of 241Am is 2.8×105 Bq m-2. Highest levels were observed near Narsaarsuk. This area was also sampled most...... intensively. In Grønnedal the maximum observed level of 241Am is 1.9×104 Bq m-2. Prediction of the overall amount of 241Am and 239,240Pu is based on grid points within the range from the nearest measurement location. The overall amount is therefore highly dependent on the model. Under the optimal spatial...

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

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

    2010-11-08

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

  7. Commentary on inhaled {sup 239}PuO{sub 2} in dogs - a prophylaxis against lung cancer?

    Cuttler, J.M. [Cuttler and Assoc., Vaughan, Ontario (Canada); Feinendegen, L. [Brookhaven National Laboratories, Upton, New York (United States)

    2015-06-15

    Several studies on the effect of inhaled plutonium-dioxide particulates and the incidence of lung tumors in dogs reveal beneficial effects when the cumulative alpha-radiation dose is low. There is a threshold at an exposure level of about 100 cGy for excess tumor incidence and reduced lifespan. The observations conform to the expectations of the radiation hormesis dose-response model and contradict the predictions of the Linear No-Threshold (LNT) hypothesis. These studies suggest investigating the possibility of employing low-dose alpha-radiation, such as from {sup 239}PuO {sub 2} inhalation, as a prophylaxis against lung cancer. (author)

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

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

    2014-09-01

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

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

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

    2011-09-12

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

  10. Transmutation of $^{239}$Pu and Other Nuclides Using Spallation Neutrons Produced by Relativistic Protons Reacting with Massive U- and Pb-Targets

    Adam, J; Bamblevski, V P; Barabanov, M Yu; Bradnova, V; Chaloun, P; Hella, K M; Kalinnikov, V G; Krivopustov, M I; Kulakov, B A; Perelygin, V P; Pronskikh, V S; Pavliouk, A V; Solnyshkin, A A; Sosnin, A N; Stegailov, V I; Tsoupko-Sitnikov, V M; Zaverioukha, O S; Adloff, J C; Debeauvais, M; Brandt, R; Langrock, E J; Vater, P; Van, J S; Westmeier, W; Dwivedi, K K; Guo Shi Lun; Li Li Qiang; Hashemi-Nezhad, S R; Kievets, M K; Lomonosova, E M; Zhuk, I V; Modolo, G; Odoj, R; Zamani-Valassiadou, M

    2001-01-01

    Experimental studies on the transmutation of some long-lived radioactive waste nuclei, such as ^{129}I, ^{237}Np, and ^{239}Pu, as well as on natural uranium and lanthanum (all of them used as sensors) were carried out at the Synchrophasotron of the Laboratory for High Energies (JINR, Dubna). Spallation neutrons were produced by relativistic protons with energies in the range of 0.5 GeV\\le E(p)\\le 1.5 GeV interacting with 20 cm long uranium or lead target stacks. The targets were surrounded by 6 cm paraffin moderators. The radioactive sensors mentioned above were positioned on the outside surface of the moderator and contained typically approximately 0.5 up to 1 gram of long-lived isotopes. The highly radioactive targets were produced perfectly well-sealed in aluminum containers by the Institute of Physics and Power Engineering, Obninsk, Russia. From the experimentally observed transmutation rates one can easily extrapolate, that in a subcritical nuclear power assembly (or "energy amplifier") using a 10 mA pr...

  11. Spatial distribution of (241)Am, (137)Cs, (238)Pu, (239,240)Pu and (241)Pu over 17 year periods in the Ravenglass saltmarsh, Cumbria, UK.

    Oh, J-S; Warwick, P E; Croudace, I W

    2009-01-01

    Ninety five surface scrape samples were collected at the Ravenglass saltmarsh and analysed for radionuclides by alpha spectrometry ((238)Pu and (239,240)Pu), gamma spectrometry ((241)Am and (137)Cs) and liquid scintillation counting ((241)Pu). Both (241)Am and (137)Cs activities are compared with those reported by Horrill [1983. Concentrations and spatial distribution of radioactivity in an ungrazed saltmarsh. In: Coughtrey, P.J. (Ed.), Ecological Aspects of Radionuclide Release. British Ecological Society Special Publication No. 3. Blackwell, Oxford, pp. 119-215.] Significant decreases in activities for both radionuclides were observed which is caused by the declining levels of discharges from the Sellafield nuclear reprocessing plant since the 1980s. It has been concluded that the spatial distribution of these radionuclides are controlled by the tidal currents and the clay contents in the sediments. There is evidence of surface erosion of the saltmarsh and redistribution of radionuclides in the saltmarsh using isotopic ratios of measured Pu.

  12. 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.

    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

  13. 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.

    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

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

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

    2012-12-01

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

  15. Pu isotopes in soils collected downwind from Lop Nor: regional fallout vs. global fallout.

    Bu, Wenting; Ni, Youyi; Guo, Qiuju; Zheng, Jian; Uchida, Shigeo

    2015-07-17

    For the first time, soil core samples from the Jiuquan region have been analyzed for Pu isotopes for radioactive source identification and radiological assessment. The Jiuquan region is in downwind from the Lop Nor Chinese nuclear test (CNT) site. The high Pu inventories (13 to 546 Bq/m(2)) in most of the sampling locations revealed that this region was heterogeneously contaminated by the regional fallout Pu from the CNTs. The contributions of the CNTs to the total Pu in soils were estimated to be more than 40% in most cases. The (240)Pu/(239)Pu atom ratios in the soils ranged from 0.059 to 0.186 with an inventory-weighted average of 0.158, slightly lower than that of global fallout. This atom ratio could be considered as a mixed fingerprint of Pu from the CNTs. In addition, Pu in soils of Jiuquan region had a faster downward migration rate compared with other investigated places in China.

  16. Plutonium, (137)Cs and uranium isotopes in Mongolian surface soils.

    Hirose, K; Kikawada, Y; Igarashi, Y; Fujiwara, H; Jugder, D; Matsumoto, Y; Oi, T; Nomura, M

    2017-01-01

    Plutonium ((238)Pu and (239,240)Pu), (137)Cs and plutonium activity ratios ((238)Pu/(239,240)Pu) as did uranium isotope ratio ((235)U/(238)U) were measured in surface soil samples collected in southeast Mongolia. The (239,240)Pu and (137)Cs concentrations in Mongolian surface soils (surface soils (0.013-0.06) coincided with that of global fallout. The (235)U/(238)U atom ratios in the surface soil show the natural one. There was a good correlation between the (239,240)Pu and (137)Cs concentrations in the surface soils. We introduce the migration depth to have better understanding of migration behaviors of anthropogenic radionuclides in surface soil. We found a difference of the migration behavior between (239,240)Pu and (137)Cs from (137)Cs/(239,240)Pu - (137)Cs plots for the Mongolian and Tsukuba surface soils; plutonium in surface soil is migrated easier than (137)Cs.

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

    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.

  18. Fission Product Yields of 233U, 235U, 238U and 239Pu in Fields of Thermal Neutrons, Fission Neutrons and 14.7-MeV Neutrons

    Laurec, J.; Adam, A.; de Bruyne, T.; Bauge, E.; Granier, T.; Aupiais, J.; Bersillon, O.; Le Petit, G.; Authier, N.; Casoli, P.

    2010-12-01

    The yields of more than fifteen fission products have been carefully measured using radiochemical techniques, for 235U(n,f), 239Pu(n,f) in a thermal spectrum, for 233U(n,f), 235U(n,f), and 239Pu(n,f) reactions in a fission neutron spectrum, and for 233U(n,f), 235U(n,f), 238U(n,f), and 239Pu(n,f) for 14.7 MeV monoenergetic neutrons. Irradiations were performed at the EL3 reactor, at the Caliban and Prospero critical assemblies, and at the Lancelot electrostatic accelerator in CEA-Valduc. Fissions were counted in thin deposits using fission ionization chambers. The number of fission products of each species were measured by gamma spectrometry of co-located thick deposits.

  19. Applicability of 239Pu as a tracer for soil erosion in the wet-dry tropics of northern Australia

    Lal, R.; Tims, S. G.; Fifield, L. K.; Wasson, R. J.; Howe, D.

    2013-01-01

    The technique of accelerator mass spectroscopy (AMS) has been employed to determine modern soil loss rates through the analysis of 239Pu profiles in soil cores from the Daly basin in Northern Territory, Australia. In areas in which soil conservation banks were not present or were only added recently (soil loss rates over the past ∼50 years were 7.5-19.5 t ha-1 a-1. The measured rates are up to 5 times higher compared to agricultural and uncultivated areas within soil conservation banks in other parts of the catchment. High intensity seasonal rainfall combined with reduction in land cover due to grazing and episodic bush fires are primary factors influencing erosion although other impacts on the landscape such as tillage generated runoff and land clearing seem to be responsible for accelerated sediment production.

  20. Applicability of {sup 239}Pu as a tracer for soil erosion in the wet-dry tropics of northern Australia

    Lal, R., E-mail: rajeev.lal@anu.edu.au [Department of Nuclear Physics, Research School of Physics and Engineering, Australian National University, Canberra, ACT 0200 (Australia); Tims, S.G.; Fifield, L.K. [Department of Nuclear Physics, Research School of Physics and Engineering, Australian National University, Canberra, ACT 0200 (Australia); Wasson, R.J.; Howe, D. [Charles Darwin University, Darwin, NT 0810 (Australia)

    2013-01-15

    The technique of accelerator mass spectroscopy (AMS) has been employed to determine modern soil loss rates through the analysis of {sup 239}Pu profiles in soil cores from the Daly basin in Northern Territory, Australia. In areas in which soil conservation banks were not present or were only added recently (<25a) and which had a history of grazing and cultivation the measured soil loss rates over the past {approx}50 years were 7.5-19.5 t ha{sup -1} a{sup -1}. The measured rates are up to 5 times higher compared to agricultural and uncultivated areas within soil conservation banks in other parts of the catchment. High intensity seasonal rainfall combined with reduction in land cover due to grazing and episodic bush fires are primary factors influencing erosion although other impacts on the landscape such as tillage generated runoff and land clearing seem to be responsible for accelerated sediment production.

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

    Regnier, D; Schunck, N; Verriere, M

    2016-01-01

    Accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r-process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data is available is an incentive to develop a fully microscopic approach to fission dynamics. In this work, we calculate the pre-neutron emission charge and mass distributions of the fission fragments formed in the neutron-induced fission of 239Pu using a microscopic method based on nuclear energy density functional (EDF) method, where large amplitude collective motion is treated adiabatically using the time dependent generator coordinate method (TDGCM) under the Gaussian overlap approximation (GOA). Fission fragment distributions are extracted from the flux of the collective wave packet through the scission line. We find that the main characteristics of the fission charge and mass distributions can be well reproduced by existing energy functionals even in tw...

  2. Evaluating the 239Pu Prompt Fission Neutron Spectrum Induced by Thermal to 30 MeV Neutrons

    Neudecker, D.; Talou, P.; Kawano, T.; Kahler, A. C.; Rising, M. E.; White, M. C.

    2016-03-01

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

  3. Evaluating the 239Pu Prompt Fission Neutron Spectrum Induced by Thermal to 30 MeV Neutrons

    Neudecker D.

    2016-01-01

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

  4. Fission Product Yield Study of 235U, 238U and 239Pu Using Dual-Fission Ionization Chambers

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

    2014-05-01

    To resolve long-standing differences between LANL and LLNL regarding the correct fission basis for analysis of nuclear test data [M.B. Chadwick et al., Nucl. Data Sheets 111, 2891 (2010); H. Selby et al., Nucl. Data Sheets 111, 2891 (2010)], a collaboration between TUNL/LANL/LLNL has been established to perform high-precision measurements of neutron induced fission product yields. The main goal is to make a definitive statement about the energy dependence of the fission yields to an accuracy better than 2-3% between 1 and 15 MeV, where experimental data are very scarce. At TUNL, we have completed the design, fabrication and testing of three dual-fission chambers dedicated to 235U, 238U, and 239Pu. The dual-fission chambers were used to make measurements of the fission product activity relative to the total fission rate, as well as for high-precision absolute fission yield measurements. The activation method was employed, utilizing the mono-energetic neutron beams available at TUNL. Neutrons of 4.6, 9.0, and 14.5 MeV were produced via the 2H(d,n)3He reaction, and for neutrons at 14.8 MeV, the 3H(d,n)4He reaction was used. After activation, the induced γ-ray activity of the fission products was measured for two months using high-resolution HPGe detectors in a low-background environment. Results for the yield of seven fission fragments of 235U, 238U, and 239Pu and a comparison to available data at other energies are reported. For the first time results are available for neutron energies between 2 and 14 MeV.

  5. {sup 137}Cs, {sup 239+24}Pu and {sup 24}Pu/{sup 239}Pu atom ratios in the surface waters of the western North Pacific Ocean, eastern Indian Ocean and their adjacent seas

    Yamada, Masatoshi [Nakaminato Laboratory for Marine Radioecology, National Institute of Radiological Sciences, Isozaki 3609, Hitachinaka, Ibaraki 311-1202 (Japan)]. E-mail: m_yamada@nirs.go.jp; Zheng Jian [Nakaminato Laboratory for Marine Radioecology, National Institute of Radiological Sciences, Isozaki 3609, Hitachinaka, Ibaraki 311-1202 (Japan); Wang Zhongliang [Nakaminato Laboratory for Marine Radioecology, National Institute of Radiological Sciences, Isozaki 3609, Hitachinaka, Ibaraki 311-1202 (Japan); State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guanshui Road 46, Guiyang 550002 (China)

    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 {sup 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 {sup 137}Cs activities showed a wide variation with values ranging from 1.1 Bq m{sup -3} in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m{sup -3} in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of {sup 137}Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of {sup 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 {sup 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{sup -1} in the Sulu and Indonesian Seas, 0.033 yr{sup -1} in the Bay of Bengal and Andaman Sea, and 0.029 yr{sup -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. {sup 239+24}Pu activities and {sup 24}Pu/{sup 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 {sup 24}Pu / {sup 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

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

    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).

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

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

    1992-02-01

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

  8. Short-Lived Fission Products Yield Measurement for 239pu(nth ,f)%239Pu(nth,f)短寿命裂变产物产额测量

    刘世龙; 杨毅; 冯晶

    2012-01-01

    采用γ能谱相对测量方法,以97Zr为内标参考核素,完成了239Pu( nth,f)短寿命裂变产物88Rb、95Y、101Mo、101Tc、…Csg、142 La等核素的累积产额测量.实验测得88Rb、”Y、101Mo、101Tc、38Csg、142La的累积产额数据分别为(1.32±0.05)%、(4.69±0.22)%、(6.13±0.32)%、(6.10土0.22)%、(6.24±0.24)%、(4.74±o.17)%.对高纯锗探测器中高能端效率刻度、样品封装与辐照、γ谱测量几何条件设计、γ谱测量与数据分析进行了研究.实验测量裂变产物核素分别位于非对称裂变质量分布双驼峰曲线轻峰的左侧、中部和右侧,重峰的中部与右侧.%The cumulative fission yields of short-lived nuclides 88Rb, 95Y, 101Mo, 101Tc, 119 Cs81 and 14!La in thermal neutron induced fission of 230Pu have been determined by gamma-ray spectrometry relative method. "Zr is selected as the reference nuclide. The determined cumulative fission yields are given as following: the Y(88Rb) = (1. 32 + 0. 05) %, Y(95Y) = (4.69 + 0.22)%, Y(101Mo) = (6. 13 + 0. 32 )%, Y(10'Tc)= (6.10 + 0.22)%, Y(I38Cse) = (6. 24 + 0. 24)%, Y(14ELa) = (4. 74 + 0. 17)%. The major work include HPGe detector efficiency calibration, sample sealing and irradiation, gamma-ray measurement and data analysis. The determined nuclides are located in left, middle, right of light group, and in middle, right of heavy group for asymmetric fission model. The accurate yields data supply a gap for domestic nuclear database, and reflect the fission products mass distribution character in thermal neutron induced fission of 239Pu.

  9. Isotopic composition and distribution of plutonium in northern South China Sea sediments revealed continuous release and transport of Pu from the Marshall Islands.

    Wu, Junwen; Zheng, Jian; Dai, Minhan; Huh, Chih-An; Chen, Weifang; Tagami, Keiko; Uchida, Shigeo

    2014-03-18

    The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios in sediments of the northern South China Sea and its adjacent Pearl River Estuary were determined to examine the spatial and temporal variations of Pu inputs. We clarified that Pu in the study area is sourced from a combination of global fallout and close-in fallout from the Pacific Proving Grounds in the Marshall Islands where above-ground nuclear weapons testing was carried out during the period of 1952-1958. The latter source dominated the Pu input in the 1950s, as evidenced by elevated (240)Pu/(239)Pu atom ratios (>0.30) in a dated sediment core. Even after the 1950s, the Pacific Proving Grounds was still a dominant Pu source due to continuous transport of remobilized Pu from the Marshall Islands, about 4500 km away, along the North Equatorial Current followed by the transport of the Kuroshio current and its extension into the South China Sea through the Luzon Strait. Using a simple two end-member mixing model, we have quantified the contributions of Pu from the Pacific Proving Grounds to the northern South China Sea shelf and the Pearl River Estuary are 68% ± 1% and 30% ± 5%, respectively. This study also confirmed that there were no clear signals of Pu from the Fukushima Daiichi Nuclear Power Plant accident impacting the South China Sea.

  10. Photofission product yields of {sup 238}U and {sup 239}Pu with 22-MeV bremsstrahlung

    Wen, Xianfei; Yang, Haori, E-mail: haori.yang@oregonstate.edu

    2016-06-11

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

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

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

    2015-04-01

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

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

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

    2010-08-01

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

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

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

    2016-09-01

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

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

    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.

  15. Assinatura da deposição atmosférica de testes nucleares em sedimentos da costa brasileira (240+239Pu e 137Cs

    Christian J. Sanders

    2012-01-01

    Full Text Available The aim of this review is to take a look at Cold War era nuclear tests signatures found in Brazilian coastal sediments. Both137Cs and 240+239Pu signatures have been documented in mangrove, coastal mudflats and continental shelf sediments, associated with above ground nuclear tests beginning in the 1950's. The dates associated to the anthropogenic radionuclide signatures 137Cs and 240+239Pu along sediment columns are confirmed by 210Pb geochronology in many of the studies highlighted in this review. The results outlined in this review characterize the extent to which nuclear fallout products reach the Brazilian coast in quantities sufficient for detection, allowing the use of these radioisotopes as geochronometers.

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

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

    2012-12-01

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

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

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

    2016-10-01

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

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

    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.

  19. A modelling study on {sup 137}Cs and {sup 239,240}Pu behaviour in the Alboran Sea, western Mediterranean

    Perianez, R. [Departamento Fisica Aplicada I, E.U. Ingenieria Tecnica Agricola, Universidad de Sevilla, Ctra., Utrera km 1, 41013 Sevilla (Spain)], E-mail: rperianez@us.es

    2008-04-15

    A model for simulating the dispersion processes of {sup 137}Cs and {sup 239,240}Pu in the Alboran Sea is described. The model consists of two hydrodynamic models: a 2D depth-averaged model and a two-layer model which provide tidal and geostrophic currents, respectively; a sediment transport model which provides suspended particle concentrations and sedimentation rates over the domain; and the radionuclide dispersion model including interactions of dissolved radionuclides with suspended particles and bed sediments. These processes are formulated using kinetic transfer coefficients. The hydrodynamic and sediment models are run and validated in advance, and their results are then used to simulate the dispersion of {sup 137}Cs and {sup 239,240}Pu, which are introduced from atmospheric fallout. Radionuclide concentrations in the water column and distributions in bed sediments have been compared with measurements in the sea. Both set of data are, in general, in agreement. The model has also been applied to calculate radionuclide fluxes through the Strait of Gibraltar. These computed fluxes have been compared with previous estimations as well.

  20. Coupled study of radionuclides and stable lead isotopes in Western Mediterranean; Etude couplee des radionucleides et des isotopes stables du plomb en Mediterranee occidentale

    Miralles, J

    2004-05-15

    The aim of this work is to identified an environmental deposit able to have stored the atmospheric signal over large time-scale leaning our investigations on lead stable isotopes ({sup 206}Pb, {sup 207}Pb, {sup 208}Pb) and radionuclide ({sup 210}Pb, {sup 137}Cs, {sup 239}Pu, {sup 240}Pu) analysis. Owing to prior studies on anthropogenic lead sources, emission intensity and sedimentary accumulation, we choose to investigate the marine sediments of the Western Mediterranean. In the Gulf of Lions, the sedimentary accumulation is 110 {+-} 7 {mu}g.cm{sup -2} high in good agreement with the atmospheric inventory estimate we made from salt marshes of Camargue (99 {mu}g.cm{sup -2}). The reconstructed lead accumulation through a modelling step coupling {sup 210}Pb and stable isotopes corroborates the regional anthropogenic emissions (Ferrand, 1996). Briefly, in this context of the marine sediments are a relevant proxy to study past lead atmospheric concentration over the last hundred years. In the Alboran Sea, the study area is less constrained and more complex in terms of climatic, meteorological and hydrological conditions. The sedimentary inventory is of 153 {+-} 47 {mu}g.cm{sup -2}, 1,5 higher than in the margin sediments of the Gulf of Lions. The analysis of aerosols, sediments and settling particles evidences a continuity between the atmospheric signal and the sedimentary record. In spite of this encouraging results, the knowledge of the Alboran system is still too restricted in order to unambiguously conclude on accuracy of deep marine sediments of this area to study past atmospheric fallouts. (author)

  1. Estimation of multi-group cross section covariances for {sup 235,238}U, {sup 239}Pu, {sup 241}Am, {sup 56}Fe, {sup 23}Na and {sup 27}Al

    De Saint Jean, C.; Archier, P.; Noguere, G.; Litaize, O.; Vaglio-Gaudard, C.; Bernard, D.; Leray, O. [CEA, DEN, DER, Cadarache, F-13108 Saint-Paul-lez-Durance (France)

    2012-07-01

    This paper presents the methodology used to estimate multi-group covariances for some major isotopes used in reactor physics. The starting point of this evaluation is the modelling of the neutron induced reactions based on nuclear reaction models with parameters. These latest are the vectors of uncertainties as they are absorbing uncertainties and correlation arising from the confrontation of nuclear reaction model to microscopic experiment. These uncertainties are then propagated towards multi-group cross sections. As major breakthroughs were then asked by nuclear reactor physicists to assess proper uncertainties to be used in applications, a solution is proposed by the use of integral experiment information at two different stages in the covariance estimation. In this paper, we will explain briefly the treatment of all type of uncertainties, including experimental ones (statistical and systematic) as well as those coming from validation of nuclear data on dedicated integral experiment (nuclear data oriented). We will illustrate the use of this methodology with various isotopes such as {sup 235,238}U, {sup 239}Pu, {sup 241}Am, {sup 56}Fe, {sup 23}Na and {sup 27}Al. (authors)

  2. Studies on the Precise Measurement of Isotope of Trace Plutonium in Uranium by MC-ICP-MS%多接收电感耦合等离子体质谱法精确测量铀中痕量钚同位素方法研究

    李力力; 李金英; 赵永刚; 常志远; 张继龙; 王同兴

    2009-01-01

    The infinitesimal plutonium impurity was contained in the uranium product obtained by reprocessing. The precise measurement of the isotope ratio of plutonium was beneficial to the identification of the corresponding source of uranium product. Basing on the separation of trace plutonium from uranium matrix, the operating parameters of MC-ICP-MS were studied and optimized for determining the isotope ratio of trace plutonium, such as the adjustment of resolution, selection of mode of ion extraction, elimination of background and interference, etc. The correction method of the mass discrimination was explored for MCICP-MS measuring isotope ratio. The isotope ratio of ~(239)pu/~(240)Pu in two selected uranium products obtained by reprocessing, which was measured and corrected by measuring plutonium reference material. The ratio of uranium and plutonium is more than 10~(10), and the sum of relative uncertainty for plutonium measurement is better than 5%. The measuring method of isotope ratiois establishes for ng · L~(-1) level of plutonium.%经过核燃料后处理得到的铀产品中含有极微量钚杂质,对其同位素组成进行分析有利于对应铀材料的溯源.本工作在铀钚化学分离的基础上,对影响MC-ICP-MS法精确测量痕量钚同位素丰度比值的仪器条件进行了优化,研究了仪器分辨率、离子提取模式的选择、"背景和干扰"等参数的影响,探索研究了MC-ICP-MS上质量偏倚的校正方法.对选择的两个后处理铀产品中痕量钚同位素比进行了测量,当铀钚比例达10~(10)时,测得的~(239)Pu/~(240)Pu相对不确定度优于5%.并且建立了在MC-ICP-MS上测量ng·L~(-1)量级钚同位素丰度比值的方法.

  3. Decay Heat Analyses after Thermal-Neutron Fission of {sup 235}U and {sup 239}Pu by SCALE-6.1.3 with Recently Available Fission Product Yield Data

    Kim, Do Heon; Gil, Choong-Sup; Lee, Young-Ouk [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

    2014-10-15

    The heat reaches about 1.5% after one hour and falls to 0.4% after a day. After a week it will be about 0.2%. The reactor, however, still requires further cooling for several years to keep the fuel rods safe. In general, the decay heat in the reactors can be calculated using a summation calculation method, which is simply the sum of the activities of the fission products produced during the fission process and after the reactor shutdown weighted by the mean decay energies. Consequently, the method is strongly dependent on the available nuclear structure data. Nowadays, the method has been implemented in various burnup and depletion programs such as ORIGEN and CINDER. In this study, the decay heat measurements after thermal-neutron fission of {sup 235}U and {sup 239}Pu have been evaluated by the ORIGEN-S with the decay data and fission product yield libraries included in the SCALE-6.1.3 software package. The new libraries were applied to the decay heat calculations, and the results were compared with those by the ORIGEN reference calculation. The decay heat measurements for very short cooling times after thermal-neutron fission of {sup 235}U and {sup 239}Pu have been evaluated by the ORIGEN-S summation calculation. The reference calculation results by the latest ORIGEN data libraries of the SCALE-6.1.3 have been validated with the measurements by ORNL and Studsvik. In addition, the generation of the new ORIGEN yield libraries has been completed based on the ENDF/B-VII.1, JEFF-3.1.1, JENDL/FPY-2011, and JENDL-4.0. The new libraries have been successfully applied to the decay heat calculations and comparative analyses have been devoted to verifying the importance of the fission product yield data when estimating the decay heat values for each isotope in a very short time. The decay data library occupies an important position in the ORIGEN summation calculation along with the fission product yield library.

  4. Methodological Study on AMS Measurement of Ultra-trace Pu Isotope Ratios at CIAE

    DONG; Ke-jun; ZHAO; Qing-zhang; WANG; Chen; HE; Ming; JIANG; Shan; ZHANG; Hui; PANG; Yi-jun; SHEN; Hong-tao; WANG; Xiao-ming; XU; Yong-ning; WU; Shao-yong; YANG; Xu-ran; WANG; Xiang-gao

    2015-01-01

    The determination of ultra-trace plutonium is very important in different fields.A new measurement method of plutonium isotopic ratios with accelerator mass spectrometry(AMS)was developed at China Institute of Atomic Energy(CIAE).Two laboratory reference standards of 239Pu/240 Pu(ST1)and 239Pu/242 Pu(ST2)are17.241and 10.059,a flow blank,a commercial blank and three real samples were respectively

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

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

    2016-05-01

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

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

    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.

  7. Polonium 210Po, uranium (234U, 238U and plutonium (238Pu, 239+240Pu bioaccumulation in marine birds

    Strumińska-Parulska D. I.

    2013-04-01

    Full Text Available The aim of this work was the determination of 210Po, 234U, 238U, 238Pu and 239+240Pu concentration in marine birds which permanently or temporally live in the southern Baltic Sea coast. We chose 11 species of seabirds: three species permanently residing at southern Baltic Sea, four species of wintering birds and three species of migrating birds. The results show that analyzed radionuclides are non-uniformly distributed in the marine birds. The highest activities of 210Po were observed in feathers, muscles and liver. The highest uranium content was found in liver, rest of viscera and feathers, while plutonium in the digestion organs and feathers. Omnivore seabirds accumulated more polonium, plutonium than species that feed on fish, while herbivore seabirds accumulated more uranium than carnivore.

  8. Exploratory study of fission product yields of neutron-induced fission of 235U , 238U , and 239Pu at 8.9 MeV

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

    2015-06-01

    Using dual-fission chambers each loaded with a thick (200 -400 -mg /c m2) actinide target of 235 ,238U or 239Pu and two thin (˜10 -100 -μ g /c m2) reference foils of the same actinide, the cumulative yields of fission products ranging from 92Sr to 147Nd have been measured at En= 8.9 MeV . The 2H(d ,n ) 3He reaction provided the quasimonoenergetic neutron beam. The experimental setup and methods used to determine the fission product yield (FPY) are described, and results for typically eight high-yield fission products are presented. Our FPYs for 235U(n ,f ) , 238U(n ,f ) , and 239Pu(n ,f ) at 8.9 MeV are compared with the existing data below 8 MeV from Glendenin et al. [Phys. Rev. C 24, 2600 (1981), 10.1103/PhysRevC.24.2600], Nagy et al. [Phys. Rev. C 17, 163 (1978), 10.1103/PhysRevC.17.163], Gindler et al. [Phys. Rev. C 27, 2058 (1983), 10.1103/PhysRevC.27.2058], and those of Mac Innes et al. [Nucl. Data Sheets 112, 3135 (2011), 10.1016/j.nds.2011.11.009] and Laurec et al. [Nucl. Data Sheets 111, 2965 (2010), 10.1016/j.nds.2010.11.004] at 14.5 and 14.7 MeV, respectively. This comparison indicates a negative slope for the energy dependence of most fission product yields obtained from 235U and 239Pu , whereas for 238U the slope issue remains unsettled.

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

    Nicol, T. [CEA, DEN, Cadarache, Nuclear Measurement Laboratory, F-13108 Saint-Paul-lez-Durance (France); FZJ, Institute of Energy and Climate Research – Nuclear Waste Management and Reactor Safety, Wilhelm-Johnen-Straße, d-52425 Jülich (Germany); Pérot, B., E-mail: bertrand.perot@cea.fr [CEA, DEN, Cadarache, Nuclear Measurement Laboratory, F-13108 Saint-Paul-lez-Durance (France); Carasco, C. [CEA, DEN, Cadarache, Nuclear Measurement Laboratory, F-13108 Saint-Paul-lez-Durance (France); Brackx, E. [CEA, DEN, Marcoule, Metallography and Chemical Analysis Laboratory, F-30207 Bagnols-sur-Cèze (France); Mariani, A.; Passard, C. [CEA, DEN, Cadarache, Nuclear Measurement Laboratory, F-13108 Saint-Paul-lez-Durance (France); Mauerhofer, E. [FZJ, Institute of Energy and Climate Research – Nuclear Waste Management and Reactor Safety, Wilhelm-Johnen-Straße, d-52425 Jülich (Germany); Collot, J. [Laboratoire de Physique Subatomique et de Cosmologie, Université Grenoble Alpes, CNRS/IN2P3 Grenoble (France)

    2016-10-01

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

  10. Cross-section measurements for {sup 239}Pu(n,f) and {sup 6}Li(n,{alpha}) with a lead slowing-down spectrometer

    Rochman, D. [National Nuclear Data Center, Brookhaven National Laboratory, Upton, NY 11973-5000 (United States)]. E-mail: drochman@bnl.gov; Haight, R.C. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: haight@lanl.gov; O' Donnell, J.M. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: odonnell@lanl.gov; Wender, S.A. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: wender@lanl.gov; Vieira, D.J. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: vieira@lanl.gov; Bond, E.M. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: bond@lanl.gov; Bredeweg, T.A. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: toddb@lanl.gov; Wilhelmy, J.B. [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)]. E-mail: j_wilhelmy@lanl.gov; Granier, T. [Commissariat a l' Energie Atomique, 91680 Bruyeres-le-Chatel (France)]. E-mail: granier@cea.fr; Ethvignot, T. [Commissariat a l' Energie Atomique, 91680 Bruyeres-le-Chatel (France)]. E-mail: ethvignot@cea.fr; Petit, M. [Commissariat a l' Energie Atomique, 91680 Bruyeres-le-Chatel (France)]. E-mail: petit@cea.fr; Danon, Y. [Rensselaer Polytechnic Institute, Troy, NY 12180 (United States)]. E-mail: danony@rpi.edu; Romano, C. [Rensselaer Polytechnic Institute, Troy, NY 12180 (United States)]. E-mail: romanc2@rpi.edu

    2006-08-01

    We present fission cross-section measurements with {approx}10ng of {sup 239}Pu performed using the LANSCE Lead Slowing-Down Spectrometer. Results of Li6(n,{alpha}) measurements with a sample size of 760ng of {sup 6}Li are also reported. This technical achievement demonstrates the feasibility of measuring neutron-induced fission cross-section on samples with 10ng of fissile actinides that are available on ultra-small quantities. Furthermore, results on neutron-induced alpha emission show that measurements for astrophysics purposes are feasible with the LSDS.

  11. Cross-section measurements for 239Pu(n,f) and 6Li(n, α) with a lead slowing-down spectrometer

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

    2006-08-01

    We present fission cross-section measurements with ˜10 ng of 239Pu performed using the LANSCE Lead Slowing-Down Spectrometer. Results of Li6(n,α) measurements with a sample size of 760 ng of 6Li are also reported. This technical achievement demonstrates the feasibility of measuring neutron-induced fission cross-section on samples with 10 ng of fissile actinides that are available on ultra-small quantities. Furthermore, results on neutron-induced alpha emission show that measurements for astrophysics purposes are feasible with the LSDS.

  12. 福岛核事故向环境释放的 Pu研究进展%Plutonium Isotopes Released f rom Fukushima Daiichi Nuclear Power Plant Accident into Environment

    倪有意; 卜文庭; 郭秋菊; 胡丹; 许宏

    2015-01-01

    福岛核事故向环境释放的放射性核素中包含了锕系元素Pu ,其中以极毒组的239 Pu、240 Pu和高毒组的241 Pu为主。本文总结并分析了针对福岛核事故向环境释放的 Pu的相关研究。据估计,福岛核事故向环境中排放的239+240 Pu总量约为109 Bq ,是切尔诺贝利核事故排放量的万分之一。此次事故排放的Pu同位素原子比(240 Pu/239 Pu和241 Pu/239 Pu)及活度比(A (238 Pu)/A (239+240 Pu))明显异于全球沉降值,可作为事故中Pu溯源的判定依据。事故所排放的Pu全部来源于核电站1~3号反应堆堆芯而非乏燃料池。现有研究报道的数据表明,在福岛核电站周围30 km范围内的陆地环境中存在来自核事故排放的Pu污染,污染相对严重的“热点”区域和该地区与核电站的相对位置没有明显关联,主要是受地形和降水的影响。而对于人们关心的海洋环境,来自福岛核事故的Pu污染非常小。核事故向海洋中排放的Pu相对于核事故前海洋环境中的Pu污染水平可忽略不计。%On March 11 , 2011 , a catastrophic tsunami induced by a magnitude 9.0 earthquake caused the terrible Fukushima Daiichi Nuclear Power Plant (FDNPP) acci‐dent ,leading to the release of a large amount of radionuclides into the environment .T he published studies on plutonium isotopes in the environment after the FDNPP accident were reviewed in this paper .The total atmospheric released amounts of Pu from the FDNPP accident were estimated to be 109 Bq ,that is only 1/10 000 of that released from the Chernobyl accident .The Pu isotopes were released from the damaged reactors ,not from the spent fuel pools in the FDNPP .The Pu isotopic ratios (240 Pu/239 Pu ,241 Pu/239 Pu) and activity ratios of A(238 Pu)/A(239+ 240 Pu) were significantly different from that of global fallout ,serving as powerful fingerprints for Pu source identification .To date , the plutonium

  13. 242Pu as tracer for simultaneous determination of 237Np and 239,240Pu in environmental samples

    Chen, Q.J.; Dahlgaard, H.; Nielsen, S.P.;

    2002-01-01

    A procedure has been developed using Pu-242 as tracer for simultaneous determination of Np-237 and Pu-239,Pu-240 in environmental samples. The validity of the method has been demonstrated by ICPMS and alpha-spectroscopy for up to 10 gram soil and sediment, seawater up to 200 litres. The paper...... describes a suitable chemical procedure for Np and Pu including a quantitative pre-concentration of neptunium and plutonium, preparation of Np4+ and Pu4+, NP(NO3)(6)(2-) and Pu(NO3)(6)(2-), The ratio of Np-237/Pu-242 (or Np-237/Pu-239) before and after the procedure has been determined using 10 g soil (free...... from Np and Pu) R-before/R-after = 1.004 +/- 3.3% (S.D n = 20) and 1 litre seawater R-before/R-after = 1.019+/-1.9% (S.D., n = 12). Results from the intercomparison samples LAEA-135, LAEA-381 and from environmental samples are presented....

  14. Historical changes in 239Pu and 240Pu sources in sedimentary records in the East China Sea: Implications for provenance and transportation

    Wang, Jinlong; Baskaran, Mark; Hou, Xiaolin

    2017-01-01

    Concentrations and isotopic compositions of plutonium (Pu) are widely used for its source identification and to determine transport processes of Pu-associated particulate matter and water. We investigated the concentrations of 239Pu and 240Pu and their ratios in a number of sediment samples from...

  15. Ultra-trace plutonium determination in small volume seawater by sector field inductively coupled plasma mass spectrometry with application to Fukushima seawater samples.

    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.

  16. 熔岩玻璃体239Pu在地下水中的迁移模拟研究%Migration Simulation of 239 Pu in Groundwater From Melt Glass

    包敏; 王群书

    2014-01-01

    According to the circumstances of an underground nuclear test CHESHIRE at the Nevada Test Site ,a model was developed to simulate the dissolution and migration of 239 Pu from melt glass in groundwater .The release rate of 239 Pu was calculated and the released 239 Pu was divided into dissolved fraction and colloid fraction . The pollution plumes for dissolved 239 Pu and colloid 239 Pu were simulated in 100 000 years by software FEFLOW .The results show that the dissolved 239 Pu can’t migration far away from the melt glass and sorption coefficient is the key parameter .If sorption coefficient is more than 10 mL/g ,the long distance migration of dissolved 239 Pu can be ignored .The colloid 239 Pu plume will be long-standing in the downstream of the melt glass .The 239 Pu con-centration at 1.3 km away from the melt glass would be 10-2 Bq/L for a long time .The parameters effecting colloid 239 Pu migration are the melt glass release rate ,the colloid fraction ratio and aquifer conductivity .It can be concluded that only colloid 239 Pu can migrate far away from the melt glass .%针对内华达核试验场CHESHIRE地下核试验状况和近场水文地质参数,建立了熔岩玻璃体239 Pu的溶解释放和迁移模型。估算了熔岩玻璃体释放产生239 Pu的速率,将释放出的239 Pu分为溶解态和胶体态,以软件FEFLOW作为建模工具,数值模拟了10万年内溶解态239 Pu和胶体态239 Pu在地下水中的污染羽分布。模拟结果表明,溶解态239 Pu不能发生远距离迁移,影响迁移的关键参数是分配系数,当分配系数大于10 mL/g后,可忽略溶解态239 Pu的远距离迁移;胶体态239 Pu在爆心下游形成较固定的污染晕,距爆心1.3 km处的胶体态239 Pu的模拟活度浓度长期处于10-2 Bq/L ;影响胶体态239 Pu迁移的主要因素包括熔岩玻璃体的溶解速度、熔岩玻璃体释放239 Pu形成胶体态239 Pu的比例、岩层渗透系数。由

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

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

    2007-02-01

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

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

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

    1992-10-01

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

  19. A study on artificial radionuclides ({sup 134}Cs, {sup 137}Cs and {sup 239+240}Pu) distribution in the sediment form lake euiam

    Kim, Seung Hwan; Lee, Sang Han; Oh, Jung Suk; Choi, Jong Ki [Korea Research Institute of Standards and Science, Daejeon (Korea, Republic of); Kang, Tae Gu [National Institute of Environmental Research, Sejong (Korea, Republic of)

    2015-12-15

    The objective of this study is to identify the radionuclide distribution in public water by carrying out the analysis of artificial radionuclides(({sup 134}Cs, {sup 137}Cs, {sup 239+240}Pu), natural radionuclide({sup 210}Pb) and TOC in the lake Euiam sediment in Chuncheon, South Korea. The {sup 134}Cs concentration in all lake sediments showed below MDA values, and the {sup 137}Cs concentration in lake sediment were ranged from MDA to 8.79 Bq · kg{sup -1}-dry. The {sup 137}Cs concentrations in surface sediment were reported to be 2.4 to 4.2 Bq · kg{sup -1}-dry. The lowest concentration of {sup 137}Cs was reported at St. 4 and the highest concentration was reported at St. 3, respectively. The {sup 239+240}Pu concentration in lake sediment were ranged from 0.049 to 0.47 Bq · kg{sup -1}-dry. The lowest concentration of was reported at St. 2 and the highest concentration was reported at St. 3. The correlation(r) between the {sup 239+240}Pu concentration and {sup 137}Cs concentration in lake sediment presented higher values (0.54 to 0.97) and this suggests the behavior and origin of {sup 137}Cs is identical to the {sup 239+240}Pu in the sediment. The {sup 134}Cs concentration below MDA value and the {sup 239+240}Pu/{sup 134}Cs ratio(mean value of 0.041) indicated that the artificial radionuclides in the sediment were originated from global fallout by the atmospheric testing of nuclear weapons conducted by former USSR and U.S.A, but not from the Fukushima Daiichi NPP accident. The sedimentation rate derived from {sup 2}'1{sup 0}Pb age-dating method at St. 2 is calculated to be 0.31±0.06 cm · y{sup -1}. This value is similar to the value (0.41±0.05 cm · y{sup -1}) estimated from the {sup 137}Cs maximum peak produced from early 1960's. The content of TOC in lake Euiam sediments varied from 0.20 to 13.01%. While the highest correlation between TOC and {sup 137}Cs concentration in the sediment were found at St. 1, the others presented the low correlation.

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

    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.

  1. Variation of the activity concentrations and fluxes of natural (210Po, 210Pb) and anthropogenic (239,240Pu, 137Cs) radionuclides in the Strait of Gibraltar (Spain).

    Gascó, C; Antón, M P; Delfanti, R; González, A M; Meral, J; Papucci, C

    2002-01-01

    The activity concentrations and fluxes of natural (210Pb, 210Po) and anthropogenic (239,240Pu, 137Cs) radionuclides have been determined in the different water masses crossing the Strait of Gibraltar. New data have been gathered during four multidisciplinary and multinational sampling campaigns, performed between 1997 and 1999 within the framework of the CANIGO-FLUGIST Project. Mean activity concentrations of 210Po (1.53+/-0.34 Bq m(-3), n = 30) and 210Pb (1.16+/-0.50 Bq m(-3), n = 31) in the Atlantic water entering the Mediterranean basin are about double those measured in the Mediterranean outflow, namely 0.84+/-0.34 Bq m(-3) (n = 22) for 210Po and 0.66+/-0.34 Bq m(-3) (n = 22) for 210Pb. The opposite trend is observed for 231,240Pu, with average concentrations of 9.9+/-3.0 mBq m(-3) (n = 29) in the incoming Atlantic flow and 22.0+/-3.0 mBq m(-3) (n = 22) in the outpouring Mediterranean water. In the case of 137Cs, the same concentrations were quantified in the waters moving inwards (2.52+/-0.28 Bq m(-3), n = 27) and outwards (2.14+/-0.52 Bq m(-3), n = 21) from the Mediterranean Sea. On this basis, the Mediterranean basin experiences a net annual input flux of 14 TBq of 210Pb and 19 TBq of 210Po, and a net annual loss of 0.34 TBq of 239,240Pu, while--at present--137Cs input and output fluxes appear to be balanced.

  2. Spatial distribution of {sup 241}Am, {sup 137}Cs, {sup 238}Pu, {sup 239,240}Pu and {sup 241}Pu over 17 year periods in the Ravenglass saltmarsh, Cumbria, UK

    Oh, J.-S. [GAU-Radioanalytical, School of Ocean and Earth Science, National Oceanography Centre, Southampton SO14 3ZH (United Kingdom)], E-mail: jsoh@noc.soton.ac.uk; Warwick, P.E. [GAU-Radioanalytical, School of Ocean and Earth Science, National Oceanography Centre, Southampton SO14 3ZH (United Kingdom)], E-mail: pew@noc.soton.ac.uk; Croudace, I.W. [GAU-Radioanalytical, School of Ocean and Earth Science, National Oceanography Centre, Southampton SO14 3ZH (United Kingdom)], E-mail: iwc@noc.soton.ac.uk

    2009-07-15

    Ninety five surface scrape samples were collected at the Ravenglass saltmarsh and analysed for radionuclides by alpha spectrometry ({sup 238}Pu and {sup 239,240}Pu), gamma spectrometry ({sup 241}Am and {sup 137}Cs) and liquid scintillation counting ({sup 241}Pu). Both {sup 241}Am and {sup 137}Cs activities are compared with those reported by Horrill [1983. Concentrations and spatial distribution of radioactivity in an ungrazed saltmarsh. In: Coughtrey, P.J. (Ed.), Ecological Aspects of Radionuclide Release. British Ecological Society Special Publication No. 3. Blackwell, Oxford, pp. 119-215.] Significant decreases in activities for both radionuclides were observed which is caused by the declining levels of discharges from the Sellafield nuclear reprocessing plant since the 1980s. It has been concluded that the spatial distribution of these radionuclides are controlled by the tidal currents and the clay contents in the sediments. There is evidence of surface erosion of the saltmarsh and redistribution of radionuclides in the saltmarsh using isotopic ratios of measured Pu.

  3. Capture and Fission rate of 232-Th, 238-U, 237-Np and 239-Pu from spallation neutrons in a huge block of lead.

    Vlachoudis, Vasilis

    2000-01-01

    The study is centered on the research of the incineration possibility of nuclear waste, by the association of a particle accelerator with a multiplying medium of neutrons, in the project "Energy Amplifier" of C. Rubbia. It consists of the experimental determination of the rates of capture and fission of certain elements (232-Th, 238-U, 237-Np and 239-Pu) subjected to a fluence of fast spallation neutrons. These neutrons are produced by the interaction of high kinetic energy protons (several GeV) provided by the CERN-PS accelerator, on a large lead solid volume. The measurement techniques used in this work, are based on the activation of elements in the lead volume and the subsequent gamma spectroscopy of the activated elements, and also by the detection of fission fragment traces. The development, of a Monte Carlo code makes it possible, on one hand, to better understand the relevant processes, and on the other hand, to validate the code, by comparison with measurements, for the design and the construction of...

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

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

    2012-11-01

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

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

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

    1988-08-01

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

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

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

    2012-11-01

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

  7. Possible differences in biological availability of isotopes of plutonium: Report of a workshop

    Kercher, J.R.; Gallegos, G.M. [eds.

    1993-09-01

    This paper presents the results of a workshop conducted on the apparent different bioavailability of isotopes {sup 238}Pu and {sup 239}Pu. There is a substantial body of evidence that {sup 238}Pu as commonly found in the environment is more biologically available than {sup 239}Pu. Studies of the Trinity Site, Nevada Test Site from nonnuclear and nuclear events, Rocky Flats, Enewetak and Bikini, and the arctic tundra support this conclusion and indicate that the bioavailability of {sup 238}Pu is more than an order of magnitude greater than that of {sup 239}Pu. Plant and soil studies from controlled environments and from Savannah River indicate no isotopic difference in availability of Pu to plants; whereas studies at the Trinity Site do suggest a difference. While it is possible that these observations can be explained by problems in the experimental procedure and analytical techniques, this possibility is remote given the ubiquitous nature of the observations. Studies of solubility of Pu in the stomach contents of cattle grazing at the Nevada Test Site and from fish from Bikini Atoll both found that {sup 238}Pu was more soluble than {sup 239}Pu. Studies of the Los Alamos effluent stream indicate that as particle size decreases, the content of {sup 238}Pu relative to {sup 239}Pu increases.

  8. Even–odd effects in prompt emission of spontaneously fissioning even–even Pu isotopes

    Tudora, A., E-mail: anabellatudora@hotmail.com [University of Bucharest, Faculty of Physics, Bucharest Magurele, POB MG-11, R-76900 (Romania); Hambsch, F.-J. [EC-JRC Institute for Reference Materials and Measurements (IRMM), Retieseweg 111, B-2440, Geel (Belgium); Giubega, G.; Visan, I. [University of Bucharest, Faculty of Physics, Bucharest Magurele, POB MG-11, R-76900 (Romania)

    2015-01-15

    The available experimental Y(A,TKE) data for {sup 236,238,240,242,244}Pu(SF) together with the Zp model prescription with appropriate parameters allows the investigation of even–odd effects in fragment distributions. The size of the global even–odd effect in Y(Z) is decreasing from {sup 244}Pu(SF) to {sup 236}Pu(SF) confirming the general observation of a decrease of the even–odd effect with the fissility parameter. Charge polarizations (ΔZ) and root-mean squares (rms) as a function of A of {sup 236–244}Pu(SF) were obtained for the first time. In the asymmetric fission region both ΔZ(A) and rms(A) exhibit oscillations with a periodicity of about 5 mass units due to the even–odd effects. The total average charge deviations 〈ΔZ〉 (obtained by averaging ΔZ(A) over the experimental Y(A) distribution) are of about |0.5| for all studied Pu(SF) systems. The comparison of the calculated ΔZ(A) and rms(A) of {sup 240}Pu(SF) with those of {sup 239}Pu(n{sub th},f) reported by Wahl shows an in-phase oscillation with a higher amplitude in the case of {sup 240}Pu(SF), confirming the higher even–odd effect in the case of SF. As in the previously studied cases ({sup 233,235}U(n{sub th},f), {sup 239}Pu(n{sub th},f), {sup 252}Cf(SF)) the even–odd effects in the prompt emission of {sup 236–244}Pu(SF) are mainly due to the Z even–odd effects in fragment distributions and charge polarizations and the N even–odd effects in the average neutron separation energies from fragments 〈Sn〉. The size of the global N even–odd effect in 〈Sn〉 is decreasing with the fissility parameter, being higher for the Pu(SF) systems compared to the previously studied systems. The prompt neutron multiplicities as a function of Z, ν(Z), exhibit sawtooth shapes with a visible staggering for asymmetric fragmentations. The size of the global Z even–odd effect in ν(Z) exhibits a decreasing trend with increasing fissility. The average prompt neutron multiplicities as a

  9. Uncertainty analyses in the resolved resonance region of {sup 235}U, {sup 238}U, and {sup 239}Pu with the Reich-Moore R-matrix theory for JENDL-3.2

    Kawano, Toshihiko [Kyushu University, Interdisciplinary Graduate School of Engineering Sciences, Kasuga, Fukuoka (Japan); Shibata, Keiichi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    2002-08-01

    A simple method to estimate covariances for resolved resonance parameters was developed. Although a large number of resolved resonances are observed for major actinides, uncertainties in averaged cross sections are more important than those in resonance parameters in reactor calculations. The method developed here derives a covariance matrix for the resolved resonance parameters which gives an appropriate uncertainty of the averaged cross sections. The method was adopted to evaluate the covariance data for {sup 235}U, {sup 238}U, and {sup 239}Pu resonance parameters in JENDL-3.2, with the Reich-Moore R-matrix formula. (author)

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

    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.

  11. Almost twenty years' search of transuranium isotopes in effluents discharged to air from nuclear power plants with VVER reactors.

    Hölgye, Z; Filgas, R

    2006-04-01

    Airborne effluents of 5 stacks (stacks 1-5) of three nuclear power plants, with 9 pressurized water reactors VVER of 4,520 MWe total power, were searched for transuranium isotopes in different time periods. The search started in 1985. The subject of this work is a presentation of discharge data for the period of 1998-2003 and a final evaluation. It was found that 238Pu, 239,240Pu, 241Am, 242Cm, and 244Cm can be present in airborne effluents. Transuranium isotope contents in most of the quarterly effluent samples from stacks 2, 4 and 5 were not measurable. Transuranium isotopes were present in the effluents from stack l during all 9 years of the study and from stack 3 since the 3rd quarter of 1996 as a result of a defect in the fuel cladding. A relatively high increase of transuranium isotopes in effluents from stack 3 occurred in the 3rd quarter of 1999, and a smaller increase occurred in the 3rd quarter of 2003. In each instance 242Cm prevailed in the transuranium isotope mixtures. 238Pu/239,240Pu, 241Am/239,240Pu, 242Cm/239,240Pu, and 244Cm/239,240Pu ratios in fuel for different burn-up were calculated, and comparison of these ratios in fuel and effluents was performed.

  12. Sequential Injection Method for Rapid and Simultaneous Determination of 236U, 237Np, and Pu Isotopes in Seawater

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

    2013-01-01

    An automated analytical method implemented in a novel dual-column tandem sequential injection (SI) system was developed for simultaneous determination of 236U, 237Np, 239Pu, and 240Pu 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. 242Pu was used as a chemical yield tracer for both plutonium and neptunium. 238U was quantified in the sample before the separation for deducing the 236U concentration from the measured 236U/238U atomic ratio in the separated uranium target using accelerator mass spectrometry...

  13. Accelerator mass spectrometry (AMS) in plutonium analysis.

    Strumińska-Parulska, Dagmara I

    The paper summarizes the results of the (240)Pu/(239)Pu atomic ratio studies in atmospheric fallout samples collected in 1986 over Gdynia (Poland) as well as three Baltic fish species collected in 1997 using the accelerator mass spectrometry. A new generation of AMS has been developed during last years and this method is an efficient and good technique to measure long-lived radioisotopes in the environment and provides the most accurate determination of the atomic ratios between (240)Pu and (239)Pu. The nuclide compositions of plutonium in filter samples correspond to their means of production. AMS measurements of atmospheric fallout collected in April showed sufficient increase of the (240)Pu/(239)Pu atomic ratio from 0.28 from March to 0.47. Also such high increase of (240)Pu/(239)Pu atomic ratio, close to reactor core (240)Pu/(239)Pu atomic ratio, was observed in September and equaled 0.47.

  14. Off-Site Radiation Exposure Review Project: Phase 2 soils program

    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.

  15. Influences of parameter uncertainties within the ICRP-66 respiratory tract model: regional tissue doses for 239PuO2 and 238UO2/238U3O8.

    Farfán, Eduardo B; Huston, Thomas E; Bolch, W Emmett; Vernetson, William G; Bolch, Wesley E

    2003-04-01

    This paper extends an examination of the influence of parameter uncertainties on regional doses to respiratory tract tissues for short-ranged alpha particles using the ICRP-66 respiratory tract model. Previous papers examined uncertainties in the deposition and clearance aspects of the model. The critical parameters examined in this study included target tissue depths, thicknesses, and masses, particularly within the thoracic or lung regions of the respiratory tract. Probability density functions were assigned for the parameters based on published data. The probabilistic computer code LUDUC (Lung Dose Uncertainty Code) was used to assess regional and total lung doses from inhaled aerosols of 239PuO2 and 238UO2/238U3O8. Dose uncertainty was noted to depend on the particle aerodynamic diameter. Additionally, dose distributions were found to follow a lognormal distribution pattern. For 239PuO2 and 238UO2/238U3O8, this study showed that the uncertainty in lung dose increases by factors of approximately 50 and approximately 70 for plutonium and uranium oxides, respectively, over the particle size range from 0.1 to 20 microm. For typical exposure scenarios involving both radionuclides, the ratio of the 95% dose fractile to the 5% dose fractile ranged from approximately 8-10 (corresponding to a geometric standard deviation, or GSD, of about 1.7-2) for particle diameters of 0.1 to 1 microm. This ratio increased to about 370 for plutonium oxide (GSD approximately 4.5) and to about 600 for uranium oxide (GSD approximately 5) as the particle diameter approached 20 microm. However, thoracic tissue doses were quite low at larger particle sizes because most of the deposition occurred in the extrathoracic airways. For 239PuO2, median doses from LUDUC were found be in general agreement with those for Reference Man (via deterministic LUDEP 2.0 calculations) in the particle range of 0.1 to 5 microm. However, median doses to the basal cell nuclei of the bronchial airways (BB

  16. New measurements of (n,γ) and (n,fission) cross sections and capture-to-fission ratios for ^233,235U and ^239Pu using the DANCE 4π BaF2 array

    Bredeweg, T. A.; Jandel, M.; Fowler, M. M.; Bond, E. M.; Haight, R. C.; Keksis, A. L.; O'Donnell, J. M.; Reifarth, R.; Rundberg, R. S.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wouters, J. M.; Becker, J. A.; Parker, W. E.; Wu, C. Y.; Baker, J. D.; McGrath, C. A.

    2009-10-01

    Accurate neutron nuclear data are important to many issues in stockpile stewardship, nuclear reactor design and re-certification, nuclear non-proliferation and nuclear forensics. Of particular interest are the production and destruction reactions for all of the major and most of the minor actinides. The competition between capture and fission in many of the actinides presents both an obstacle and an opportunity for large γ detector arrays such as DANCE. Additional instrumentation is required to deconvolve the two contributions to the total observed γ-ray spectrum. However, conducting a simultaneous measurement can simplify background treatment and other sources of systematic uncertainty. An outline of the current experimental program will be presented along with results from neutron capture measurements on ^233,235U and ^239Pu.

  17. Synchronous Changes of the Shape of Histograms Constructed from the Results of Measurements of 90-Sr Beta-Decay and 239-Pu Alpha-Decay Observed in More than 3000 km Distant Laboratories

    Filin E. Y.

    2015-07-01

    Full Text Available It was discovered many years ago that histograms constructed from the results of mea- surements of various natural processes are not random. The histogram shape was demonstrated to be determined by the diurnal rotation and circumsolar movement of the Earth and to be independent of the nature of the process considered [1-17]. The results of those works change our basic views about stochasticity of natural processes. When the time series of physical measurements, which are traditionally considered stochastic, are transformed into the series of histograms constructed for an optimally small num- ber of the results (i.e., optimally short segment of the time series, one can see regular changes in the histogram shape. The paper illustrates the main manifestations of this phenomenon by comparing the results of 90 Sr -radioactivity and 239 Pu -decay mea- surements, with the distance between the laboratories in which the data were collected being about 3000 km.

  18. Analysis of Sub-picogram Plutonium by Isotope Mass Spectrometry%亚皮克量级钚的质谱分析技术

    龙开明; 汤磊; 贾宝亭; 刘雪梅; 杨天丽; 刘钊

    2005-01-01

    By using active carbon powder as ionization enhance matter, the detect sensitivity of 239Pu ,which was 0.5 pg (1±0.15, 95% confidence level), was about 20 times that of the tradition method. The sub-picogram plutonium sample was determined quantitatively by isotope dilution mass spectrometry (IDMS).

  19. Measurements of the neutron-induced fission cross sections of /sup 240/Pu and /sup 242/Pu relative to /sup 235/U. [0. 02 to 30 MeV, tables

    Behrens, J. W.; Browne, J. C.; Carlson, G. W.

    1976-03-01

    A continuation is given of the fission-cross-section ratio measurements in progress at the Lawrence Livermore Laboratory. Preliminary results are provided for the /sup 240/Pu//sup 235/U and /sup 242/Pu//sup 235/U ratios from 0.02 to 30 MeV and 0.1 to 30 MeV, respectively. Using the threshold-cross-section method, the ratios were normalized to the values 1.368 +- 0.030 and 1.116 +- 0.025, respectively, from 1.75 to 4.00 MeV.

  20. Radiotoxicological analyses of {sup 239+240}Pu and {sup 241}Am in biological samples by anion-exchange and extraction chromatography: a preliminary study for internal contamination evaluations

    Ridone, S.; Arginelli, D.; Bortoluzzi, S.; Canuto, G.; Montalto, M.; Nocente, M.; Vegro, M. [Italian National Agency for New Technologies, Energy and the Environment (ENEA), Research Centre of Saluggia, Radiation Protection Institute, Saluggia, VC (Italy)

    2006-07-01

    Many biological samples (urines and faeces) have been analysed by means of chromatographic extraction columns, utilising two different resins (AG 1-X2 resin chloride and T.R.U.), in order to detect the possible internal contamination of {sup 239{sup +}}{sup 240}Pu and {sup 241}Am, for some workers of a reprocessing nuclear plant in the decommissioning phase. The results obtained show on one hand the great suitability of the first resin for the determination of plutonium, and on the other the great selectivity of the second one for the determination of americium.

  1. Estimation of covariances of {sup 16}O, {sup 23}Na, Fe, {sup 235}U, {sup 238}U and {sup 239}Pu neutron nuclear data in JENDL-3.2

    Shibata, Keiichi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment; Nakajima, Yutaka; Kawano, Toshihiko; Oh, Soo-Youl; Matsunobu, Hiroyuki; Murata, Toru

    1997-10-01

    Covariances of nuclear data have been estimated for 6 nuclides contained in JENDL-3.2. The nuclides considered are {sup 16}O, {sup 23}Na, Fe, {sup 235}U, {sup 238}U, and {sup 239}Pu, which are regarded as important for the nuclear design study of fast reactors. The physical quantities for which covariances are deduced are cross sections, resolved and unresolved resonance parameters, and the first order Legendre-polynomial coefficient for the angular distribution of elastically scattered neutrons. As for {sup 235}U, covariances were obtained also for the average number of neutrons emitted in fission. The covariances were estimated by using the same methodology that had been used in the JENDL-3.2 evaluation in order to keep a consistency between mean values and their covariances. The least-squares fitting code GMA was used in estimating covariances for reactions of which JENDL-3.2 cross sections had been evaluated by taking account of measurements. In nuclear model calculations, the covariances were calculated by the KALMAN system. The covariance data obtained were compiled in the ENDF-6 format, and will be put into the JENDL-3.2 Covariance File which is one of JENDL special purpose files. (author). 193 refs.

  2. 232Th、233U、238Pu、240Pu、242Pu、241Am、242Cm、243Cm和244Cm的裂变释放热能研究%Thermal Energy Released in Fission of 232 Th,233 U,238 Pu, 240 Pu,242 Pu,241 Am,242 Cm,243 Cm and 244 Cm

    赵艳飞; 马续波; 陈义学

    2013-01-01

    In the nuclear reactor design ,the precise calculation of thermal fission energy is of great significance .In the pressurized water reactor ,high energy neutron-induced fission rarely occurs ,the isotopes including 233 U ,241 Am and 243 Cm are mostly induced by thermal neutrons ,while the other isotopes such as 232Th ,238Pu ,240Pu ,242Pu ,242Cm and 244 Cm are by fast neutron . In order to carry out this work , the nuclear data extracted from the latest evaluated nuclear data file (ENDF/B-Ⅶ ) were adopted ,and the energy-conservation law for the calculation of total fission energy were used , meanw hile ,with the consideration of capture energy and the correction of βand γ ,the thermal fission energy of nine isotopes was obtained .Compared with the data excerpted from IAEA issued WIMS-D database ,the results are reasonable .The thermal fission energy and its uncertainties of the nine isotopes are :(193.939 ± 0.176) MeV for 232 Th , (200.063 ± 0.084) MeV for 233 U ,(208.786 ± 1.133 ) MeV for 238 Pu ,(211.266 ± 0.220 ) MeV for 240 Pu ,(213.862 ± 0.299 ) MeV for 242 Pu ,(215.077 ± 0.210 ) MeV for 241 Am ,(218.821 ± 0.159) MeV for 242Cm ,(218.525 ± 0.388) MeV for 243Cm ,and (220.067 ± 0.131) MeV for 244 Cm ,respectively .%在核反应堆设计中,对每次裂变释放热能进行精确计算具有重要意义。在压水堆内,高能中子诱发核裂变份额很小,233 U、241 Am、243 Cm主要由热中子诱发裂变,232 T h、238 Pu、240 Pu、242 Pu、242 Cm、244 Cm主要由快中子诱发裂变。本文采用最新的核评价数据库 ENDF/B-Ⅶ,利用质量守恒法计算裂变释放总能,同时研究了中微子带走的能量,中子俘获能及β、γ修正项,最终给出了9种核素裂变释放热能。与IAEA颁布的WIMS-D格式数据库中的裂变释放热能数据的对比表明,本文所用方法计算结果合理。9种核素每次裂变释放热能分别为:232 Th ,(193.939±0.176) MeV ;233 U ,(200.063

  3. Determination of {sup 238}Pu, {sup 239+240}Pu, {sup 241}Pu and {sup 241}Am in radioactive waste from IPEN reactor

    Geraldo, Bianca; Taddei, Maria Helena T.; Cheberle, Sandra M.; Ferreira, Marcelo T., E-mail: bgeraldo@cnen.gov.b, E-mail: mhtaddei@cnen.gov.b, E-mail: scsantos@cnen.gov.b, E-mail: ferreira@cnen.gov.b [Brazilian Nuclear Energy Commission (LAPOC/CNEN-MG), Pocos de Caldas, MG (Brazil). Lab. of Pocos de Caldas; Marumo, Julio T., E-mail: jtmarumo@ipen.b [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil)

    2011-07-01

    Ion exchange resin is a common type of radioactive waste arising from treatment of coolant water of the main circuit of research and nuclear power reactors. This waste contains high concentrations of fission and activation products. The management of this waste includes its characterization in order to determine and quantify specific radionuclides including those known as difficult-to-measure radionuclides (RDM). The analysis of RDMs generally involves expensive and time-consuming complex radiochemical analysis for purification and separation of the radionuclides. The objective of this work is to show an easy methodology for quantifying plutonium and americium isotopes in spent ion exchange resin, used for purification of the cooling water of the IEA-R1 reactor located at the Nuclear and Energy Research Institute, IPEN-CNEN/SP. The resins were destroyed by acid digestion, followed by purification and separation of the Pu and Am isotopes with anionic and chromatographic resins. {sup 238}Pu, {sup 239}+{sup 24}'0Pu, and {sup 24}'1Am isotopes were analyzed in an alpha spectrometer equipped with surface barrier detectors. {sup 241}Pu isotope was analyzed by liquid scintillation counting. Chemical recovery yield ranged from 73 to 98% for Pu and 77 to 98% for Am, demonstrating that the methodology is suitable for identification and quantification of the isotopes studied in spent resins. (author)

  4. Long-range tropospheric transport of uranium and plutonium weapons fallout from Semipalatinsk nuclear test site to Norway.

    Wendel, Cato Christian; Fifield, L Keith; Oughton, Deborah H; Lind, Ole Christian; Skipperud, Lindis; Bartnicki, Jerzy; Tims, Stephen G; Høibråten, Steinar; Salbu, Brit

    2013-09-01

    A combination of state-of-the-art isotopic fingerprinting techniques and atmospheric transport modelling using real-time historical meteorological data has been used to demonstrate direct tropospheric transport of radioactive debris from specific nuclear detonations at the Semipalatinsk test site in Kazakhstan to Norway via large areas of Europe. A selection of archived air filters collected at ground level at 9 stations in Norway during the most intensive atmospheric nuclear weapon testing periods (1957-1958 and 1961-1962) has been screened for radioactive particles and analysed with respect to the concentrations and atom ratios of plutonium (Pu) and uranium (U) using accelerator mass spectrometry (AMS). Digital autoradiography screening demonstrated the presence of radioactive particles in the filters. Concentrations of (236)U (0.17-23nBqm(-3)) and (239+240)Pu (1.3-782μBqm(-3)) as well as the atom ratios (240)Pu/(239)Pu (0.0517-0.237) and (236)U/(239)Pu (0.0188-0.7) varied widely indicating several different sources. Filter samples from autumn and winter tended to have lower atom ratios than those sampled in spring and summer, and this likely reflects a tropospheric influence in months with little stratospheric fallout. Very high (236)U, (239+240)Pu and gross beta activity concentrations as well as low (240)Pu/(239)Pu (0.0517-0.077), (241)Pu/(239)Pu (0.00025-0.00062) and (236)U/(239)Pu (0.0188-0.046) atom ratios, characteristic of close-in and tropospheric fallout, were observed in filters collected at all stations in Nov 1962, 7-12days after three low-yield detonations at Semipalatinsk (Kazakhstan). Atmospheric transport modelling (NOAA HYSPLIT_4) using real-time meteorological data confirmed that long range transport of radionuclides, and possibly radioactive particles, from Semipalatinsk to Norway during this period was plausible. The present work shows that direct tropospheric transport of fallout from atmospheric nuclear detonations periodically may have

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

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

    2016-01-01

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

  6. Pu and Am determination in the environment—method development

    Afonin, M.; Simonoff, M.; Donard, O.; Michel, H.; Ardisson, G.

    2003-01-01

    A high resolution inductively coupled plasma mass spectrometric (HR-ICP-MS) method for the determination of plutonium isotopes, Am and the 240Pu/239Pu isotope ratio utilising modification of Pu-02-RC Plutonium in Soil Samples, Pu-03-RC Plutonium in Soil Residue—Total Dissolution Method, Pu-11-RC Plutonium Purification—Ion Exchange Technique, Pu-12-RC Plutonium and/or Americium in Soil or Sediments, HASL-300 was developed. Total plutonium concentrations (239+240Pu) measured in environmental samples by this HR-ICP-MS method were in good agreement with recommended data obtained from a-spectrometry. It was achieved the decreasing of the time to analyze the samples over than 33%.

  7. RAPID DETERMINATION OF 237 NP AND PU ISOTOPES IN WATER BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY

    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.

  8. Accumulation of polonium 210Po, uranium (234U and 238U and plutonium (238Pu and 239+240Pu in tissues and organs of deer Carvidae from northern Poland

    Strumińska-Parulska D. I.

    2013-04-01

    Full Text Available Livers, kidneys and muscles of large herbivorous animals: roe deer (Capreolus capreolus, red deer (Cervus elaphus and fallow deer (Dama dama, collected in northern Poland, were the subject of the investigation. Polonium, uranium and plutonium activities were measured using alpha spectrometry along with relevant radiochemical procedures. The average concentrations of 210Po ranged between 0.02±0.01 Bq kg−1 ww in muscles and 7.15±0.12 Bq kg−1 ww in kidneys. The concentration of 238U ranged widely between 2.49±0.18 and 69.37±5.45 mBq kg−1 ww. The average concentrations of 239+240Pu ranged between 0.18±0.04 mBq kg−1 ww in muscle and 2.77±0.60 mBq kg−1 ww in kidneys. Statistical analysis showed that the sampling location, sex, age and species did not influence on the radioisotope activities in the analyzed samples.

  9. Measurements of low-level anthropogenic radionuclides from soils around Maralinga

    Tims, Stephen G.; Tsifakis, Dimitrios; Srncik, Michaela; Fifield, L. Keith; Hancock, Gary J.; De Cesare, Mario

    2013-12-01

    The isotopes 239Pu and 240Pu 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 constitute artificial tracers of recent soil erosion and sediment movement. In practice the high throughput capabilities and high sensitivity of the AMS technique makes the study of Australia's geographically large areas viable using Pu 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 contribution from the Maralinga tests to the Pu isotopic abundances present in the region around Maralinga is largely unknown. In global fallout, for example, the 240Pu/239Pu ratio is typically in the range 0.17 - 0.19, but the influence of the regional tests could lead to values outside this range. This would impact on the assessment techniques used in the soil and sediment tracer studies. We report recent measurements on soil samples collected from across the Maralinga Test site.

  10. Measurements of low-level anthropogenic radionuclides from soils around Maralinga

    Tims Stephen G.

    2013-12-01

    Full Text Available The isotopes 239Pu and 240Pu 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 constitute artificial tracers of recent soil erosion and sediment movement. In practice the high throughput capabilities and high sensitivity of the AMS technique makes the study of Australia’s geographically large areas viable using Pu 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 contribution from the Maralinga tests to the Pu isotopic abundances present in the region around Maralinga is largely unknown. In global fallout, for example, the 240Pu/239Pu ratio is typically in the range 0.17 - 0.19, but the influence of the regional tests could lead to values outside this range. This would impact on the assessment techniques used in the soil and sediment tracer studies. We report recent measurements on soil samples collected from across the Maralinga Test site.

  11. 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.

    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.

  12. Status of the compact 1 MV AMS facility at the Centro Nacional de Aceleradores (Spain)

    Chamizo, E. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Lopez-Gutierrez, J.M. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Dpto. de Fisica Aplicada I, Escuela Universitaria Politecnica, c/. Virgen de Africa 7, 41011 Seville (Spain)], E-mail: lguti@us.es; Ruiz-Gomez, A.; Santos, F.J. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Garcia-Leon, M. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Dpto. Fisica Atomica, Molecular y Nuclear, Avda. Reina Mercedes, s/n, 41012 Seville (Spain); Maden, C. [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Alfimov, V. [Institute of Particle Physics, HPK, ETH Hoenggerberg, CH-8093 Zurich (Switzerland)

    2008-05-15

    Since February 2006, the new 1 MV multielement compact AMS facility SARA (Spanish Accelerator for Radionuclides Analyses) at the Centro Nacional de Aceleradores (CNA) in Sevilla (Spain) is fully operative. During the first one and a half year of operation, the viability of the system for the measurement of {sup 10}Be, {sup 14}C, {sup 129}I and plutonium isotopes, {sup 239}Pu and {sup 240}Pu, has been evaluated. First results have demonstrated that, in terms of precision and detection limits, the performance of the device compares to other compact AMS facilities, although some progress can still be done in order to optimize its capacities. At this moment, background levels are in the order of 10{sup -14} for {sup 10}Be/{sup 9}Be, 10{sup -13} for {sup 129}I/{sup 127}I, 10{sup -15} for {sup 14}C/{sup 12}C (processed and unprocessed blank) and about 10{sup 6} atoms for plutonium isotopes: {sup 239}Pu, {sup 240}Pu and {sup 242}Pu. In this work, the current status of the AMS measurements at CNA for the above mentioned radionuclides is described.

  13. Radioecological studies at the National Center of Accelerators based on the use of the accelerator mass spectrometry; Estudios radioecologicos en el Centro Nacional de Aceleradores basados en el uso de la Espectrometria de Masas con Acelerador (AMS)

    Chamizo, E.; Lopez-Gutierrez, J. M.; Gomez-Guzman, J. M.; Santos, F. J.; Garcia-Leon, M.; Garcia-Tenorio, R.

    2013-03-01

    Since mid-2006 a compact Accelerator Mass Spectrometry (AMS) of 1 MV, Tandetron type, named SARA (Spanish Accelerator for Radionuclide Analysis) is installed at the National Accelerator Centre in Seville. After an initial period, to set-up the equipment and to study its capability to detect the long-lived radionuclides {sup 1}4C, {sup 1}0B, {sup 2}6Al, {sup 1}29I and plutonium isotopes ({sup 2}39Pu and {sup 2}40Pu) compared to other techniques of mass spectrometry (MS), numerous research lines in fields as diverse as archaeology, geology, palaeontology, oceanography, internal dosimetry, astrophysics and characterization of radioactive waste, among others, have been opened. In particular, since 2008 numerous contributions in the field of Radioecology have been done, based in the measurements of {sup 1}29I and Pu isotopes ({sup 2}39Pu and {sup 2}40Pu). In this article, some of these radioecological researches are summarized and presented, with special emphasis on showing that its accomplishment requires the application of the AMS technique, to be able to achieve sensitivities and detection limits which are impossible to reach when radiometric and mass spectrometry conventional techniques are applied. (Author) 13 refs.

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

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

    2016-08-01

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

  15. Development of an ultra-sensitive detection method for transuranium elements with respect to ocean water samples from Fukushima

    Hain, Karin Margarete

    2016-03-30

    The development of a detection method for the identification of a possible emission of actinides into the Pacific Ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, was the major aim of this PhD thesis. It is shown in this work that in addition to the isotopic plutonium ratio {sup 240}Pu/{sup 239}Pu, which is an important signature for different contamination sources, the {sup 241}Pu/{sup 239}Pu ratio has to be determined, to distinguish between a Fukushima entry of actinides and nuclear weapon fallout in the Pacific Ocean. Furthermore, this study was aiming for the improvement of the data on the neptunium ({sup 237}Np) distribution in the ocean. For the detection of the trace concentrations of actinides in the order of mBq/m{sup 3} in a small sample volume of 20 L ocean water, the ultra-sensitive method accelerator mass spectrometry (AMS) was chosen. A chemical separation procedure for Pu and Np based on extraction chromatography was developed using mass spectrometry and radiometric analysis to determine the chemical recovery. {sup 241}Am, which causes isobaric background to {sup 241}Pu in mass spectrometric measurements, was separated with a suppression of at least 10{sup -4} from Pu by this method. The detection method adjusted to Pu and Np was successfully verified by analyzing the concentration of Pu in certified reference material with AMS at the Maier-Leibnitz-Laboratory (MLL) in Munich. Due to a temporary closure of the MLL, 12 sea water samples, collected in autumn 2012, were prepared at the Radiochemie Muenchen and measured at the Vienna Environmental Research Laboratory (VERA). The sampling station closest to the FDNPP was located at a distance of 39.6 km. Three of the samples showed a slightly elevated {sup 240}Pu/{sup 239}Pu ratio of up to 0.23{sup +0.04}{sub -0.03} compared to global fallout ({sup 240}Pu/{sup 239}Pu = 0.180±0.007), whereas all measured {sup 241}Pu/{sup 239}Pu ratios were clearly consistent with nuclear weapon

  16. Comparison of Pu and (137)Cs as tracers of soil and sediment transport in a terrestrial environment.

    Everett, S E; Tims, S G; Hancock, G J; Bartley, R; Fifield, L K

    2008-02-01

    Following atmospheric nuclear weapons testing in the 1950s and 1960s significant quantities of (137)Cs and (239+240)Pu were deposited worldwide. In recent decades, (137)Cs has been commonly used as a tracer of soil erosion and sedimentation, particularly in the Northern Hemisphere where atomic deposition was three times as great as in the Southern Hemisphere. The relatively short 30-year half-life of this isotope means that its sensitivity as a tracer is rapidly decreasing. In contrast, with half-lives of 24,110 and 6561 years, the sensitivity of the two plutonium isotopes remains essentially the same as when it was deposited. Here we use the technique of Accelerator Mass Spectrometry to demonstrate the potential of anthropogenic Pu as an alternative to (137)Cs as a tracer of soil transport in Australia. We measure an average (137)Cs/(239+240)Pu activity ratio of 27.3+/-1.5 and an average (240)Pu/(239)Pu atom ratio of 0.149+/-0.003, both slightly lower than the global average.

  17. Isotopic evidence for trapped fissiogenic REE and nucleogenic Pu in apatite and Pb evolution at the Oklo natural reactor

    Horie, Kenji; Hidaka, Hiroshi; Gauthier-Lafaye, François

    2004-01-01

    A part of the boundary layer of reactor zone 10 at the Oklo natural reactor shows a unique petrologic texture, which contains high-grade uraninite and massive apatite concretions. In order to study distribution behavior of fission products around the boundary between the reactor zone and the wall rock and to clarify the relation of migration mechanisms of fission products with geochemical factors, in-situ isotopic analyses of Nd, Sm, Gd, Pb and U in uraninite and apatite from the sample were performed by Sensitive High Resolution Ion Microprobe (SHRIMP). Sm and Gd isotopic ratios of uraninite and apatite show evidence of neutron irradiation with fluence between 4.4-6.8×10 19 n/cm 2. Judging from the isotopic anomalies of Nd and U, the apatite coexisting with the uraninite plays an important role in trapping fissiogenic LREE and nucleogenic 239Pu into the structure. Systematic Pb isotopic data from apatite, uraninite, galena and minium suggest the following chronological interpretations. The apatite formed 1.92±0.01 Ga ago and trapped fissiogenic light REE and nucleogenic 239Pu that migrated from the reactor during the criticality. The uraninite around the boundary between reactor and sandstone dissolved once 1.1˜1.2 Ga ago. Galena grains were formed by U-Pb mobilization in association with the intrusion of dolerite dyke 0.45˜0.83 Ga ago. Minium was derived from recent dissolution of galena under locally oxidizing conditions.

  18. Dating of a sediment core from Lake Biel (Switzerland) and source characterization of fallout Pu; {sup 210}Pb- und {sup 137}Cs-Datierung eines Sedimentbohrkerns aus dem Bieler See (CH) und Ursprungsbestimmung von Pu-Fallout

    Pregler, Anja

    2016-08-01

    A sediment core from Lake Biel was dated by means of the naturally occurring radioactive isotope {sup 210}Pb as well as by the anthropogenic isotope {sup 137}Cs. The latter one can be detected as radioactive fallout of certain events in the sediment layers and accordingly be correlated with a distinct date. A verification of the correlated events is accomplished by particular isotope ratios of the anthropogenic isotopes {sup 238}Pu, {sup 239}Pu and {sup 240}Pu as well as {sup 241}Am as a decay product of the short-lived {sup 241}Pu. Furthermore, the percentage of the total {sup 137}Cs fallout was calculated corresponding to the specific events.

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

    De Cesare M.

    2015-01-01

    Full Text Available 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.

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

    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.

  1. Seasonal variations in activity concentrations of {sup 137}Cs, {sup 40}K, {sup 7}Be, {sup 228}Ac, {sup 99}Tc, {sup 90}Sr, and {sup 239/240}Pu in Fucus vesiculosus and Ascophyllum nodosum from the South-Eastern coast of Norway

    Raaum, A.; Christensen, G.C. [Institute for Energy Technology, Health and Safety Dept., Kjeller (Norway)

    2004-07-01

    Brown algae have been proven to be useful indicator organisms for heavy metals and radionuclides in the marine environments due to their ability to concentrate elements from the ambient water. There is quite a lot of data available on {sup 137}Cs in brown algae, especially for Fucus Vesiculosus. Fucus Vesiculosus is also commonly used to monitor the impact of the releases of {sup 99}Tc from the reprocessing plant in Sellafield. There is however a lack of data for other long-lived anthropogenic nuclides as {sup 90}Sr and Pu, and for natural occurring radionuclides. There is also a need for more knowledge about the mechanisms for uptake and accumulation of the different elements, and about different factors influencing the uptake. In this study activity concentrations of {sup 137}Cs, {sup 40}K, {sup 7}Be, {sup 228}Ac, {sup 99}Tc, {sup 90}Sr and {sup 239/240}Pu are measured in whole plants of Fucus vesiculosus and Ascophyllum nodosum collected over a period of one year from the south-eastern coast of Norway. Significant differences between the two species have been found. For {sup 137}Cs, {sup 40}K, {sup 7}Be, {sup 228}Ra and {sup 239/240}Pu, the activity concentrations were significantly higher in Fucus vesiculosus than in Ascophyllum nodosum, whereas for {sup 99}Tc the activity concentrations were higher in Ascophyllum nodosum than in Fucus vesiculosus. There were great seasonal variations in the concentrations of the measured radionuclides. For {sup 99}Tc there was also a difference in the temporal pattern for the two species. Possible uptake mechanisms will be discussed based on the results and on the known physiological differences between the two species. (author)

  2. DETERMINATION OF 237NP AND PU ISOTOPES IN LARGE SOIL SAMPLES BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY

    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.

  3. Manmade radionuclide vector in Austrian soil and vegetation near Temelin nuclear power plant

    Sinojmeri, M.; Ringer, V. [Oesterreichische Agentur fuer Gesundheit und Ernaehrungssicherheit - AGES (Austria)

    2014-07-01

    Since Chernobyl NPP accident an environmental monitoring program concerning the Upper Austrian region near Czech Republic Nuclear Power Plant, NPP Temelin, is in progress between AGES and BMLFUV, the Austrian Federal Ministry of Agriculture, Forestry, Environment, Water and Food, in Austria. This paper presents the results obtained during the sampling campaign over biennial period of 2010-2011. Soil samples, grass and different cereal species were collected. Beside Cs-134, Cs-137 and Sr-89, Sr-90 isotopes, at this phase the number of isotopes determined was extended with plutonium isotopes Pu-238, Pu-239, Pu-240, Pu-241 and Am-241. A comparison of these results with the existing data so far is presented. New knowledge was obtained related the bio-kinetic parameters of these elements in the environment. Document available in abstract form only. (authors)

  4. Comparative analysis between measured and calculated concentrations of major actinides using destructive assay data from Ohi-2 PWR

    Oettingen Mikołaj

    2015-09-01

    Full Text Available In the paper, we assess the accuracy of the Monte Carlo continuous energy burnup code (MCB in predicting final concentrations of major actinides in the spent nuclear fuel from commercial PWR. The Ohi-2 PWR irradiation experiment was chosen for the numerical reconstruction due to the availability of the final concentrations for eleven major actinides including five uranium isotopes (U-232, U-234, U-235, U-236, U-238 and six plutonium isotopes (Pu-236, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242. The main results were presented as a calculated-to-experimental ratio (C/E for measured and calculated final actinide concentrations. The good agreement in the range of ±5% was obtained for 78% C/E factors (43 out of 55. The MCB modeling shows significant improvement compared with the results of previous studies conducted on the Ohi-2 experiment, which proves the reliability and accuracy of the developed methodology.

  5. Neutron powder diffraction study of 239PuD x

    Bartscher, W.; Boeuf, A.; Caciuffo, R.; Fournier, J. M.; Haschke, J. M.; Manes, L.; Rebizant, J.; Rustichelli, F.; Ward, J. W.

    1985-05-01

    A neutron powder diffraction study has been carried out on several deuterids of Plutonium (PuD 2.25,PuD 2.33, PuD 2.65) to determine the positions of deuterium atoms in the host metal f.c.c. lattice. It has been found that vacancies occur in the tetrahedral sites. Moreover, with increasing deuterium concentration, octahedral interstitial deuterium atoms are displaced from their ideal positions. These results can be explained by the formation of clusters. Finally, at low temperature, these compounds become ferromagnetically ordered. An ordered magnetic moment μ 0≈0.8 μ B has been measured on all compounds.

  6. [239Pu and chromosomal aberrations in human peripheral blood lymphocytes].

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

    2009-01-01

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

  7. Toxicological versus Radiological Hazards of {sup 239}Pu

    Tansky, R.R.

    2001-07-26

    Plutonium is frequently referred to as ''the most toxic substance known to man''. While there are other chemicals that cause more immediately serious health consequences, plutonium does have the lowest permissible levels for any of the radioactive elements. Concentration limits for plutonium and its compounds are based on its radiotoxicity, specifically carcinogenicity, not on its chemical toxicity.

  8. Some comments on the toxicity of /sup 239/Pu

    Rowland, R.E.

    1978-01-01

    There is no simple method of expressing a concept such as toxicity. The toxicity of a material depends upon its form (solid, liquid, or gas), the method of entry into the body (ingestion, inhalation, or abrasion), and the individual it enters (young, old, sick, well, heavy cigarette smoker, or consumer of alcohol). Thus, statements such as ''plutonium is the most toxic material known to man'' are not only incorrect; they are meaningless. By taking the one aspect of plutonium which can be quantitated in a meaningful manner, the induction of malignant bone sarcomas in humans, the incremental risk presented to those who have been exposed to this radioelement has been shown to be quite small. By means of a hypothetical exposure of radium dial workers to plutonium instead of radium, an industry-wide exposure to plutonium would have been less harmful than the actual exposure to radium, in spite of the fact that plutonium appears to be far more toxic than radium. Further, the observation that, after radium was recognized as a toxic material, it no longer was a hazard in the dial industry, clearly demonstrates that hazardous radioactive materials can be handled safely. This has been demonstrated again with plutonium, for even though much larger quantities have been handled by many more individuals, there are no demonstrable cases of malignancies induced by this hazardous material. The absence of clearly demonstrable excesses of lung cancer in the large group of long-term thorium workers is reassuring, for it may imply that low doses to the lung have a very low probability of inducing lung cancers. It is concluded that plutonium, a highly toxic material, can be handled safely, as are many other hazardous materials that play important roles in our daily lives.

  9. Pu isotopes and {sup 241}Am activities determination in the evaluation of radiochemical sequential analyzes methodology for evaporator concentrate samples using alpha spectrometry

    Reis Junior, Aluisio S.; Temba, Eliane S.C.; Kastner, Geraldo F.; Monteiro, Roberto P.G., E-mail: reisas@cdtn.br [Centro de Desenvolvimento da Tecnologia Nuclear (SERTA/CDTN/CNEN-MG), Belo Horizonte, MG (Brazil). Servico do Reator e Tecnicas Analiticas

    2015-07-01

    Alpha spectrometry analyzes were used for activity determinations of Pu and Am isotopes in evaporator concentrate samples from nuclear power plants. In this work it was used tracers for isotopes determination and quantification. The radiometric yields ranged from 60% to 100% and the Lower Limit of Detection was estimated as being 2.05 mBqKg{sup -1}. The relative standard deviations for replicate analysis were calculated for {sup 241}Am, 15.13% (sample J) and 9.38% (sample N), and for {sup 239+240}Pu, 8.16% (sample J) and 7.95% (sample N). (author)

  10. {sup 239,} {sup 240,} {sup 241}Pu fingerprinting of plutonium in western US soils using ICPMS: solution and laser ablation measurements

    Cizdziel, James V. [University of Nevada - Las Vegas, Harry Reid Center for Environmental Studies, Las Vegas, NV (United States); Ketterer, Michael E. [Northern Arizona University, Department of Chemistry and Biochemistry, Box 5698, Flagstaff, AZ (United States); Farmer, Dennis [University of Nevada - Las Vegas, Department of Health Physics, Las Vegas, NV (United States); Faller, Scott H. [US Environmental Protection Agency, Radiation and Indoor Environments National Laboratory, Box 98517, Las Vegas, NV (United States); Hodge, Vernon F. [University of Nevada - Las Vegas, Department of Chemistry, Las Vegas, NV (United States)

    2008-01-15

    .013 [{sup 240}Pu/{sup 239}Pu] - 0.0001; r {sup 2} = 0.971) with NTS and global fallout end-members. A rapid total dissolution procedure, followed by extraction chromatography and SF-ICPMS solution Pu analysis, generates excellent agreement with certified {sup 239+240}Pu activities for standard reference materials NIST 4350b, NIST 4353, NIST 4357, and IAEA 385. {sup 239+240}Pu activities and atom ratios determined by total dissolution reveal isotopic information in agreement with the LA-ICPMS dataset regarding the ubiquitous mixing of NTS and stratospheric fallout Pu sources in the regional environment. For several specific samples, the total dissolution method reveals that Pu is incompletely recovered by simpler HNO{sub 3}-HCl leaching procedures, since some of the Pu originating from the NTS is contained in refractory siliceous particles. (orig.)

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

    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.

  12. {\\alpha}-accompanied cold ternary fission of $^{238-244}$Pu isotopes in equatorial and collinear configuration

    Santhosh, K P; Priyanka, B

    2015-01-01

    The cold ternary fission of $^{238}$Pu, $^{240}$Pu, $^{242}$Pu and $^{244}$Pu isotopes, with $^{4}$He as light charged particle, in equatorial and collinear configuration has been studied within the Unified ternary fission model (UTFM). The fragment combination $^{100}$Zr+$^{4}$He+$^{134}$Te possessing the near doubly magic nuclei $^{134}$Te (N=82, Z=52) gives the highest yield in the alpha accompanied ternary fission of $^{238}$Pu. For the alpha accompanied ternary fission of $^{240}$Pu, $^{242}$Pu and $^{244}$Pu isotopes, the highest yield was found for the fragment combination with doubly magic nuclei $^{132}$Sn (N=82, Z=50) as the heavier fragment. The deformation and orientation of fragments have also been taken into account for the alpha accompanied ternary fission of $^{238-244}$Pu isotopes, and it has been found that in addition to closed shell effect, ground state deformation also plays an important role in determining the isotopic yield in the ternary fission process. The emission probability and ki...

  13. Determination of origin and intended use of plutonium metal using nuclear forensic techniques.

    Rim, Jung H; Kuhn, Kevin J; Tandon, Lav; Xu, Ning; Porterfield, Donivan R; Worley, Christopher G; Thomas, Mariam R; Spencer, Khalil J; Stanley, Floyd E; Lujan, Elmer J; Garduno, Katherine; Trellue, Holly R

    2017-01-19

    Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials' properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% (240)Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modeling feedback and trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. Based on this investigation, the most likely intended use for these plutonium foils was (239)Pu fission foil targets for physics experiments, such as cross-section measurements, etc.

  14. DEVELOPMENT OF AN IMPROVED SODIUM TITANATE FOR THE PRETREATMENT OF HIGH LEVEL NUCLEAR WASTE AT THE SAVANNAH RIVER SITE

    Hobbs D. T.; Poirier, M. R.; Barnes, M. J.; Stallings, M. E.; Nyman, M. D.

    2005-11-22

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 137}Cs, {sup 90}Sr and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes planned at SRS include caustic side solvent extraction, for {sup 137}Cs removal, and sorption of {sup 90}Sr and alpha-emitting radionuclides onto monosodium titanate (MST). The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu and {sup 240}Pu. This paper describes recent results to produce an improved sodium titanate material that exhibits increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the baseline MST material.

  15. The design and implementation of the AVNG measurement system

    Macarthur, Duncan W [Los Alamos National Laboratory; Thron, Jonathan [Los Alamos National Laboratory; Razinkov, Sergey [RFNC-VNIIEF; Livke, Alexander [RFNC-VNIIEF; Kondratov, Sergey [RFNC-VNIIEF

    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.

  16. Advanced alpha spectrum analysis based on the fitting and covariance analysis of dependent variables

    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. Ultra-sensitive detection of plutonium by accelerator mass spectrometry

    Fifield, L.K.; Cresswell, R.G.; Ophel, T.R.; Ditada, M. [Australian National Univ., Canberra, ACT (Australia). Dept. of Nuclear Physics; Day, J.P.; Clacher, A. [Manchester Univ. (United Kingdom). Dept. of Chemistry; Priest, N.D. [AEA Technology, Harwell (United Kingdom)

    1996-12-31

    On the bases of the measurements performed to date, a sensitivity of 10{sup 6} atoms is achievable with accelerator mass spectroscopy (AMS) for each of the plutonium isotopes. Not only does this open the way to the sort of study outlined, but it also makes possible other novel applications, of which two examples are given: (i)the ration of {sup 240}Pu to {sup 239}Pu as a sensitive indicator of the source of the plutonium; (ii) the biochemistry of plutonium in humans. The ultra-sensitive atom counting capability of AMS will make it possible to use the very long-lived {sup 244}Pu (8x10{sup 7}a) in human volunteer studies without any significant increase in radiation body burden. This paper will describe the AMS technique as applied to plutonium using the ANU`s 14UD accelerator, will present the results obtained to date, and will discuss the prospects for the future.

  18. Sequential determination of natural ({sup 232}Th, {sup 238}U) and anthropogenic ({sup 137}Cs, {sup 90}Sr, {sup 241}Am, {sup 239+240}Pu) radionuclides in environmental matrix

    Michel, H.; Levent, D.; Barci, V.; Barci-Funel, G.; Hurel, C. [Laboratoire de Radiochimie, Sciences Analytiques et Environnement (LRSAE), Universite de Nice Sophia-Antipolis 06108 Nice Cedex (France)

    2008-07-01

    A new sequential method for the determination of both natural (U, Th) and anthropogenic (Sr, Cs, Pu, Am) radionuclides has been developed for application to soil and sediment samples. The procedure was optimised using a reference sediment (IAEA-368) and reference soils (IAEA-375 and IAEA-326). Reference materials were first digested using acids (leaching), 'total' acids on hot plate, and acids in microwave in order to compare the different digestion technique. Then, the separation and purification were made by anion exchange resin and selective extraction chromatography: Transuranic (TRU) and Strontium (SR) resins. Natural and anthropogenic alpha radionuclides were separated by Uranium and Tetravalent Actinide (UTEVA) resin, considering different acid elution medium. Finally, alpha and gamma semiconductor spectrometer and liquid scintillation spectrometer were used to measure radionuclide activities. The results obtained for strontium-90, cesium-137, thorium-232, uranium- 238, plutonium-239+240 and americium-241 isotopes by the proposed method for the reference materials provided excellent agreement with the recommended values and good chemical recoveries. (authors)

  19. The feasibility of using Pu discharges from Sellafield to investigate the sediment dynamics of the Severn Estuary and the Welsh coast

    Dunne, J.A.; Richards, D.A. [School of Geographical Sciences and Bristol Isotope Group, University of Bristol (United Kingdom)

    2014-07-01

    Decades of nuclear weapons testing and very low level radioactive waste discharges from civil nuclear sites have resulted in a global distribution of Pu isotopes. Given that the sources of these isotopes are spatially and temporally well-known, their distribution throughout the environment can provide insight into the processes that have governed their dispersal. Plutonium-239 and {sup 240}Pu have long half-lives and their atomic abundance ratio is indicative of the source, be it atmospheric fallout or releases from the nuclear industry. Plutonium is also strongly adsorbed on sediments. These characteristics make Pu an excellent tool for monitoring ocean currents, tracking sediment transport and examining the fate of the products of nuclear activities. We intend to exploit the discharges of Pu from Sellafield nuclear reprocessing plant to investigate transit times and sediment regime in inter-tidal sediments from proximal (Ravenglass Estuary, Cumbria) and distal (Portishead, North Somerset) sites. Continuing developments in analytical techniques (extraction chromatography and ion exchange) and inductively coupled plasma mass spectrometry (ICP-MS) permit isotopic analysis at low abundances (on the order of femto-grams), with reasonable efficiency and cost in comparison to traditional radiometric techniques. A major advantage of this technique is the ability to distinguish between {sup 239}Pu and {sup 240}Pu, which is not possible with alpha-spectrometry due to similar alpha energies. We present initial results using MC-ICP-MS, following methods in Lindahl et al. (2011). Document available in abstract form only. (authors)

  20. Analytical method for the determination of Np and Pu in sea water by AMS with respect to the Fukushima accident

    Hain, K., E-mail: karin.hain@mytum.de [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Faestermann, T.; Famulok, N.; Fimiani, L.; Gómez-Guzmán, J.M.; Korschinek, G. [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Kortmann, F.; Lierse von Gostomski, Ch. [Radiochemie München, Technische Universität München, Walther-Meißner-Str.3, 85748 Garching (Germany); Ludwig, P. [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Shinonaga, T. [Helmholtz Zentrum München, German Research Center for Environmental Health, Institute of Radiation Protection, Ingolstädter Landstrasse 1, 855764 Neuherberg (Germany)

    2015-10-15

    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. {sup 241}Am, which causes isobaric background to {sup 241}Pu in mass spectrometric measurements, was successfully separated from the Pu fraction by this method. Water samples which were spiked with {sup 242}Pu and {sup 237}Np or {sup 239}Np, 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 {sup 240}Pu, {sup 241}Pu and {sup 237}Np obtained in this study are in agreement with the certified and literature values within the uncertainties. Due to strong isotopic interference of {sup 239}Pu with {sup 238}U, it was not possible to analyze the concentration of {sup 239}Pu. 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.

  1. Compilation of multigroup cross-section covariance matrices for several important reactor materials

    Drischler, J.D.; Weisbin, C.R.

    1977-10-01

    Multigroup cross-section covariance matrices are presented for fission in /sup 235/U, /sup 238/U, /sup 239/Pu, and /sup 241/Pu; capture in /sup 235/U, /sup 238/U, /sup 239/Pu, /sup 240/Pu, and /sup 241/Pu; fission neutron yield (anti nu) for /sup 235/U, /sup 238/U, /sup 239/Pu, and /sup 240/Pu; elastic scattering for Na and Fe; non-elastic reactions for Na and Fe; first-level inelastic scattering for /sup 238/U; and all reactions provided in the ENDF/B-IV covariance description of N, O, and C. Other data files generated are included for reference but have not yet been tested. The report presents the nultigroup data in six, ten, and fifteen energy group forms corresponding to weighting of the covariance data with fission (GODIVA), LMFBR (ZPR-6/7) and 1/E spectra, respectively.

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

    Pham, M. K.; van Beek, P.; Carvalho, F. P.

    2016-01-01

    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: 40K, 210Pb (210Po), 226Ra, 228Ra, 228Th, 232Th, 234U, 238U, 239Pu, 239+240Pu and 241Am for IAEA-410 and 40K, 137Cs, 210Pb (210Po), 226Ra, 228Ra, 228Th, 232Th, 235U, 238U, 239Pu, 240Pu and 239+240Pu for IAEA-412. The CRMs can be used for quality assurance and quality control purposes...

  3. Plutonium measurements by accelerator mass spectrometry at LLNL

    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.

  4. Natural decrease of the intensity level of artificial radioactive isotopes in the Barents Sea

    Matishov, G. G.; Matishov, D. G.; Solatie, D.; Kasatkina, N. E.; Leppanen, A.

    2009-08-01

    The results of radioecological investigations carried out within the framework of the Russian-Finnish high-latitude expedition in 2007 are presented. The characteristics of the present-day accumulation level of the significant radioecological isotopes 137Cs, 90Sr and 239,240Pu in the Barents Sea are described. The comparative analysis is performed for the radiation pollution of the environment in the 1980s and 1990s and in the first decade of the 21st century. Natural purification processes in the marine environment are the main factors of the decrease in the intensity level of artificial radioactive isotopes. These processes include repeated dilution, nuclear decay, occlusion by sediments and suspended solid material, and accumulation by aquatic inhabitants. A stable decreasing trend is observed for the intensity level of artificial radioactive isotopes in the Barents Sea.

  5. Long-lived radionuclides in residues from operation and decommissioning of nuclear power plants

    Lopez-Gutierrez, J.M., E-mail: lguti@us.es [Centro Nacional de Aceleradores (CNA), c/Thomas Alva Edison n Degree-Sign 7, 41092 Sevilla (Spain); University of Sevilla, Departamento de Fisica Aplicada I, c/Virgen de Africa, n Degree-Sign 7, 41011 Sevilla (Spain); Gomez-Guzman, J.M.; Chamizo, E.; Peruchena, J.I. [Centro Nacional de Aceleradores (CNA), c/Thomas Alva Edison n Degree-Sign 7, 41092 Sevilla (Spain); Garcia-Leon, M. [University of Sevilla, Departamento de Fisica Atomica, Molecular y Nuclear, Apdo. 1065, 41080 Sevilla (Spain)

    2013-01-15

    Radioactive residues, in order to be classified as Low-Level Waste (LLW), need to fulfil certain conditions; the limitation of the maximum activity from long-lived radionuclides is one of these requirements. In order to verify compliance to this limitation, the abundance of these radionuclides in the residue must be determined. However, performing this determination through radiometric methods constitutes a laborious task. In this work, {sup 129}I concentrations, {sup 239+240}Pu activities, and {sup 240}Pu/{sup 239}Pu ratios are determined in low-level radioactive residues, including resins and dry sludge, from nuclear power plants in Spain. The use of Accelerator Mass Spectrometry (AMS) enables high sensitivities to be achieved, and hence these magnitudes can be re determined with good precision. Results present a high dispersion between the {sup 129}I and {sup 239+240}Pu activities found in various aliquots of the same sample, which suggests the existence of a mixture of resins with a variety of histories in the same container. As a conclusion, it is shown that activities and isotopic ratios can provide information on the processes that occur in power plants throughout the history of the residues. Furthermore, wipes from the monitoring of surface contamination of the Jose Cabrera decommissioning process have been analyzed for {sup 129}I determination. The wide range of measured activities indicates an effective dispersal of {sup 129}I throughout the various locations within a nuclear power plant. Not only could these measurements be employed in the contamination monitoring of the decommissioning process, but also in the modelling of the presence of other iodine isotopes.

  6. Vertical distribution and migration of global fallout Pu in forest soils in southwestern China.

    Bu, Wenting; Zheng, Jian; Guo, Qiuju; Uchida, Shigeo

    2014-10-01

    Soil samples collected in southwestern China were analyzed for Pu isotopes. The (240)Pu/(239)Pu atom ratios were around 0.18, which indicated the dominant source of global fallout. Consistent sub-surface maximums followed by exponential decline of (239+240)Pu activities in the soil cores were observed. Most of the Pu has still remained in the 0-10 cm layers since its deposition. Convection velocities and dispersion coefficients for Pu migration in the soils were estimated by the convection-dispersion equation (CDE) model. The effective convection velocities and effective dispersion coefficients ranged from 0.05 to 0.11 cm/y and from 0.06 to 0.29 cm(2)/y, respectively. Other factors that control the vertical migration of Pu in soil besides precipitation, soil particle size distribution and organic matter were suggested. Long-term migration behaviors of Pu in the soils were simulated. The results provide the Pu background baseline for further environmental monitoring and source identification of non-global fallout Pu inputs in the future.

  7. Direct isotope ratio analysis of individual uranium-plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry.

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

    2015-02-01

    Uranium and plutonium isotope ratios in individual uranium-plutonium (U-Pu) mixed particles with various U/Pu atomic ratios were analyzed without prior chemical separation by thermal ionization mass spectrometry (TIMS). Prior to measurement, micron-sized particles with U/Pu ratios of 1, 5, 10, 18, and 70 were produced from uranium and plutonium certified reference materials. In the TIMS analysis, the peaks of americium, plutonium, and uranium ion signals were successfully separated by continuously increasing the evaporation filament current. Consequently, the uranium and plutonium isotope ratios, except the (238)Pu/(239)Pu ratio, were successfully determined for the particles at all U/Pu ratios. This indicates that TIMS direct analysis allows for the measurement of individual U-Pu mixed particles without prior chemical separation.

  8. Corrigendum to "Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO2 nuclear fuel"

    Piro, M. H. A.; Banfield, J.; Clarno, K.; Simunovic, S.; Besmann, T. M.; Lewis, B. J.; Thompson, W. T.

    2016-09-01

    Figs. 7-9 in "Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO2 nuclear fuel" [1] have a consistent error corresponding to the relative proportions of iodine. Reported concentrations of iodine in the original manuscript are approximately ten times higher than expected, and are comparable in atomic proportions to cesium. One would expect that the amount of cesium would be about one order of magnitude greater than iodine based on the difference in fission yields of 235U and 239Pu. A practical consequence of this error would affect the predicted quantity and chemical composition of iodine on the fuel surface, which is related to iodine-induced stress corrosion cracking [2].

  9. Using radiosilver and plutonium isotopes to trace the dispersion of contaminated sediment in Fukushima coastal catchments

    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.

  10. Isotope ratio analysis of individual sub-micrometer plutonium particles with inductively coupled plasma mass spectrometry.

    Esaka, Fumitaka; Magara, Masaaki; Suzuki, Daisuke; Miyamoto, Yutaka; Lee, Chi-Gyu; Kimura, Takaumi

    2010-12-15

    Information on plutonium isotope ratios in individual particles is of great importance for nuclear safeguards, nuclear forensics and so on. Although secondary ion mass spectrometry (SIMS) is successfully utilized for the analysis of individual uranium particles, the isobaric interference of americium-241 to plutonium-241 makes difficult to obtain accurate isotope ratios in individual plutonium particles. In the present work, an analytical technique by a combination of chemical separation and inductively coupled plasma mass spectrometry (ICP-MS) is developed and applied to isotope ratio analysis of individual sub-micrometer plutonium particles. The ICP-MS results for individual plutonium particles prepared from a standard reference material (NBL SRM-947) indicate that the use of a desolvation system for sample introduction improves the precision of isotope ratios. In addition, the accuracy of the (241)Pu/(239)Pu isotope ratio is much improved, owing to the chemical separation of plutonium and americium. In conclusion, the performance of the proposed ICP-MS technique is sufficient for the analysis of individual plutonium particles.

  11. Plutonium isotopes in the atmosphere of Central Europe: Isotopic composition and time evolution vs. circulation factors.

    Kierepko, Renata; Mietelski, Jerzy W; Ustrnul, Zbigniew; Anczkiewicz, Robert; Wershofen, Herbert; Holgye, Zoltan; Kapała, Jacek; Isajenko, Krzysztof

    2016-11-01

    This paper reports evidence of Pu isotopes in the lower part of the troposphere of Central Europe. The data were obtained based on atmospheric aerosol fraction samples collected from four places in three countries (participating in the informal European network known as the Ring of Five (Ro5)) forming a cell with a surface area of about 200,000km(2). We compared our original data sets from Krakow (Poland, 1990-2007) and Bialystok (Poland, 1991-2007) with the results from two other locations, Prague (Czech Republic; 1997-2004) and Braunschweig (Germany; 1990-2003) to find time evolution of the Pu isotopes. The levels of the activity concentration for (238)Pu and for ((239+240))Pu were estimated to be a few and some tens of nBqm(-3), respectively. However, we also noted some results were much higher (even about 70 times higher) than the average concentration of (238)Pu in the atmosphere. The achieved complex data sets were used to test a new approach to the problem of solving mixing isotopic traces from various sources (here up to three) in one sample. Results of our model, supported by mesoscale atmospheric circulation parameters, suggest that Pu from nuclear weapon accidents or tests and nuclear burnt-up fuel are present in the air.

  12. Cumulative fission yields of short-lived isotopes under natural-abundance-boron-carbide-moderated neutron spectrum

    Finn, Erin C.; Metz, Lori A.; Greenwood, Lawrence R.; Pierson, Bruce; Wittman, Richard S.; Friese, Judah I.; Kephart, Rosara F.

    2015-04-09

    The availability of gamma spectroscopy data on samples containing mixed fission products at short times after irradiation is limited. Due to this limitation, data interpretation methods for gamma spectra of mixed fission product samples, where the individual fission products have not been chemically isolated from interferences, are not well-developed. The limitation is particularly pronounced for fast pooled neutron spectra because of the lack of available fast reactors in the United States. Samples containing the actinide isotopes 233, 235, 238U, 237Np, and 239Pu individually were subjected to a 2$ pulse in the Washington State University 1 MW TRIGA reactor. To achieve a fission-energy neutron spectrum, the spectrum was tailored using a natural abundance boron carbide capsule to absorb neutrons in the thermal and epithermal region of the spectrum. Our tailored neutron spectrum is unique to the WSU reactor facility, consisting of a soft fission spectrum that contains some measurable flux in the resonance region. This results in a neutron spectrum at greater than 0.1 keV with an average energy of 70 keV, similar to fast reactor spectra and approaching that of 235U fission. Unique fission product gamma spectra were collected from 4 minutes to 1 week after fission using single-crystal high purity germanium detectors. Cumulative fission product yields measured in the current work generally agree with published fast pooled fission product yield values from ENDF/B-VII, though a bias was noted for 239Pu. The present work contributes to the compilation of energy-resolved fission product yield nuclear data for nuclear forensic purposes.

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

    Pham, M.K.; Benmansour, M.; Carvalho, F.P.

    2014-01-01

    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 40K, 137Cs, 234U and 239þ240Pu radionuclides were certified for this material, and information values...... for 12 other radionuclides (90Sr, 99Tc, 210Pb (210Po), 226Ra, 228Ra, 228Th, 230Th, 232Th, 235U, 238U, 239Pu and 240Pu) 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...

  14. Neutron spectra and dosimetric features of isotopic neutron sources: a review

    Vega C, H. R. [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Cipres No. 10, Fracc. La Penuela, 98060 Zacatecas, Zac. (Mexico); Martinez O, S. A., E-mail: fermineutron@yahoo.com [Universidad Pedagogica y Tecnologica de Colombia, Grupo de Fisica Nuclear Aplicada y Simulacion, Av. Central del Norte 39-115, 150003 Tunja, Boyaca (Colombia)

    2015-10-15

    A convenient way to produce neutrons is the isotopic neutron source, where the production is through (α, n), (γ, n), and spontaneous fission reactions. Isotopic neutron sources are small, easy to handle, and have a relative low cost. On the other hand the neutron yield is small and mostly of them produces neutrons with a wide energy distribution. In this work, a review is carried out about the the main features of {sup 24}NaBe, {sup 24}NaD{sub 2}O, {sup 116}InBe, {sup 140}LaBe, {sup 238}PuLi, {sup 239}PuBe, {sup 241}AmB, {sup 241}AmBe, {sup 241}AmF, {sup 241}AmLi, {sup 242}CmBe, {sup 210}PoBe, {sup 226}RaBe, {sup 252}Cf and {sup 252}Cf/D{sub 2}O isotopic neutron source. Also, using Monte Carlo methods, the neutron spectra in 31 energy groups, the neutron mean energy; the Ambient dose equivalent, the Personal dose equivalent and the Effective dose were calculated for these isotopic neutron sources. (Author)

  15. Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope

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

    2016-01-01

    Owing to the rich history of heavy element production in the unique high flux reactors that operated at the Savannah River Site, USA (SRS) decades ago, trace quantities of plutonium with highly unique isotopic characteristics still persist today in the SRS terrestrial environment. Development of an effective sampling, processing, and analysis strategy enables detailed monitoring of the SRS environment, revealing plutonium isotopic compositions, e.g., 244Pu, that reflect the unique legacy of plutonium production at SRS. This work describes the first long-term investigation of anthropogenic 244Pu occurrence in the environment. Environmental samples, consisting of collected foot borne debris, were taken at SRS over an eleven year period, from 2003 to 2014. Separation and purification of trace plutonium was carried out followed by three stage thermal ionization mass spectrometry (3STIMS) measurements for plutonium isotopic content and isotopic ratios. Significant 244Pu was measured in all of the years sampled with the highest amount observed in 2003. The 244Pu content, in femtograms (fg = 10−15 g) per gram, ranged from 0.31 fg/g to 44 fg/g in years 2006 and 2003 respectively. In all years, the 244Pu/239Pu atom ratios were significantly higher than global fallout, ranging from 0.003 to 0.698 in years 2014 and 2003 respectively. PMID:26898531

  16. Low-Level Plutonium Bioassay Measurements at the Lawrence Livermore National Laboratory

    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

  17. Neutron resonance parameters of dysprosium isotopes using neutron capture yields

    Shin, S. G.; Kye, Y. U.; Cho, M. H. [POSTECH, Pohang (Korea, Republic of); Namkung, W. [Pohang Accelerator Laboratory, Pohang (Korea, Republic of); Kim, G. N. [Kyungpook National University, Daegu (Korea, Republic of); Lee, M. W.; Kang, Y. R. [Dongnam Inst. Of Radiological and Medical Science, Busan (Korea, Republic of)

    2015-10-15

    Dysprosium is used in the field of nuclear reactor system because it has a very large thermal neutron absorption cross-section. The dysprosium alloyed with special stainless steels is attractive for control in nuclear reactor because of the ability to absorb neutrons readily without swelling or contracting over time and its high melting point. Dysprosium is also one of fission products from the thermal fission of {sup 234}U, {sup 233}U, and {sup 239}Pu. The fission products are accumulated in the reactor core by the burn-up of the nuclear fuel and the poison effect is increased. Therefore, it is required to understand how Dysprosium as both a poison and an absorbing material in the control rod has an effect on the neutron population in a nuclear reactor system over all energy regions. Neutron Capture experiments on Dy isotopes were performed at the electron linear accelerator (LINAC) facility of the Rensselear Polytechnic Institute (RPI) in the neutron energy region from 10 eV to 1 keV. Resonance parameters were extracted by fitting the neutron capture data using the SAMMY multilevel R-matrix Bayesian code.

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

    Xu, Yihong [School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023 (China); Qiao, Jixin [Center for Nuclear Technologies, Technical University of Denmark, Risø Campus, DK-4000 Roskilde (Denmark); Pan, Shaoming, E-mail: span@nju.edu.cn [School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023 (China); Hou, Xiaolin, E-mail: xiho@dtu.dk [Center for Nuclear Technologies, Technical University of Denmark, Risø Campus, DK-4000 Roskilde (Denmark); Xi' an AMS Center, SKLLQG, Institute of Earth Environment, CAS, Xi' an 710075 (China); Roos, Per [Center for Nuclear Technologies, Technical University of Denmark, Risø Campus, DK-4000 Roskilde (Denmark); Cao, Liguo [School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023 (China)

    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 {sup 137}Cs. 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 {sup 137}Cs. {sup 240}Pu/{sup 239}Pu 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 {sup 137}Cs at both uncultivated and cultivated sites. {sup 239+240}Pu 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 {sup 239+240}Pu and {sup 137}Cs were 88.4 and 1688 Bq m{sup −2} respectively. Soil erosion rates estimated by {sup 239+240}Pu tracing method were consistent with those obtained by the {sup 137}Cs method, confirming that Pu is an effective tracer with a similar tracing behavior to that of {sup 137}Cs for soil erosion assessment. - Highlights: • The potential for the use of Pu as a soil erosion tracer was investigated. • Pu would be a good tracer given its long half-life. • Depth profiles of Pu in soils were systematically studied and compared to {sup 137}Cs. • Pu is an effective soil erosion tracer with behavior similar to that of {sup 137}Cs. • Thus, Pu provides a means of

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

    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.

  20. Benchmark of SCALE (SAS2H) isotopic predictions of depletion analyses for San Onofre PWR MOX fuel

    Hermann, O.W.

    2000-02-01

    The isotopic composition of mixed-oxide (MOX) fuel, fabricated with both uranium and plutonium, after discharge from reactors is of significant interest to the Fissile Materials Disposition Program. The validation of the SCALE (SAS2H) depletion code for use in the prediction of isotopic compositions of MOX fuel, similar to previous validation studies on uranium-only fueled reactors, has corresponding significance. The EEI-Westinghouse Plutonium Recycle Demonstration Program examined the use of MOX fuel in the San Onofre PWR, Unit 1, during cycles 2 and 3. Isotopic analyses of the MOX spent fuel were conducted on 13 actinides and {sup 148}Nd by either mass or alpha spectrometry. Six fuel pellet samples were taken from four different fuel pins of an irradiated MOX assembly. The measured actinide inventories from those samples has been used to benchmark SAS2H for MOX fuel applications. The average percentage differences in the code results compared with the measurement were {minus}0.9% for {sup 235}U and 5.2% for {sup 239}Pu. The differences for most of the isotopes were significantly larger than in the cases for uranium-only fueled reactors. In general, comparisons of code results with alpha spectrometer data had extreme differences, although the differences in the calculations compared with mass spectrometer analyses were not extremely larger than that of uranium-only fueled reactors. This benchmark study should be useful in estimating uncertainties of inventory, criticality and dose calculations of MOX spent fuel.

  1. Plutonium contamination in soils in open space and residential areas near Rocky Flats, Colorado.

    Litaor, M I

    1999-02-01

    Spatial analysis of the 240Pu:239Pu isotopic ratio of 42 soil samples collected around Rocky Flats Plant near Golden, Colorado, was conducted to assess the effect of Rocky Flats Plant activity on the soil environment. Two probability maps that quantified the uncertainty of the spatial distribution of plutonium isotopic ratios were constructed using the sequential Gaussian simulation technique (sGs). Assuming a plutonium isotopic ratio range of 0.152+/-0.003 to 0.169+/-0.009 is characteristic to global fallout in Colorado, and a mean value of 0.155 is representative for the Rocky Flats Plant area, the main findings of the current work were (1) the areas northwest and southwest of Rocky Flats Plant exhibited a plutonium ratio > or = 0.155, thus were minimally impacted by the plant activity; (2) the study area east of Rocky Flats Plant (approximately 120 km2) exhibited a plutonium isotopic ratio open space and residential areas amounted to 111.2 GBq, with a standard error of estimate of 50.8 GBq.

  2. Arctic Ocean sea ice drift origin derived from artificial radionuclides.

    Cámara-Mor, P; Masqué, P; Garcia-Orellana, J; Cochran, J K; Mas, J L; Chamizo, E; Hanfland, C

    2010-07-15

    Since the 1950s, nuclear weapon testing and releases from the nuclear industry have introduced anthropogenic radionuclides into the sea, and in many instances their ultimate fate are the bottom sediments. The Arctic Ocean is one of the most polluted in this respect, because, in addition to global fallout, it is impacted by regional fallout from nuclear weapon testing, and indirectly by releases from nuclear reprocessing facilities and nuclear accidents. Sea-ice formed in the shallow continental shelves incorporate sediments with variable concentrations of anthropogenic radionuclides that are transported through the Arctic Ocean and are finally released in the melting areas. In this work, we present the results of anthropogenic radionuclide analyses of sea-ice sediments (SIS) collected on five cruises from different Arctic regions and combine them with a database including prior measurements of these radionuclides in SIS. The distribution of (137)Cs and (239,240)Pu activities and the (240)Pu/(239)Pu atom ratio in SIS showed geographical differences, in agreement with the two main sea ice drift patterns derived from the mean field of sea-ice motion, the Transpolar Drift and Beaufort Gyre, with the Fram Strait as the main ablation area. A direct comparison of data measured in SIS samples against those reported for the potential source regions permits identification of the regions from which sea ice incorporates sediments. The (240)Pu/(239)Pu atom ratio in SIS may be used to discern the origin of sea ice from the Kara-Laptev Sea and the Alaskan shelf. However, if the (240)Pu/(239)Pu atom ratio is similar to global fallout, it does not provide a unique diagnostic indicator of the source area, and in such cases, the source of SIS can be constrained with a combination of the (137)Cs and (239,240)Pu activities. Therefore, these anthropogenic radionuclides can be used in many instances to determine the geographical source area of sea-ice.

  3. Plutonium and Uranium Atom Ratios and Activity Levels in Cochiti Lake Bottom Sediments Provided by Pueblo de Cochiti

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

    1999-05-01

    Historical operations at the Los Alamos National Laboratory have contaminated stream sediments with plutonium and other radionuclides. A small portion of these contaminated sediments has been carried by floods into the Rio Grande drainage system, eventually to be trapped by Cochiti Lake located on Pueblo de Cochiti lands approximately 8 km downstream of the Laboratory. In this study, lake bottom sediment samples provided by the Pueblo de Cochiti were analyzed by thermal ionization mass spectrometry to determine plutonium and uranium activity levels and isotopic atom ratios. This specialized analytical method allows us to take isotopic fingerprints of radionuclides found in the sediment and to determine how much plutonium and uranium came from the Laboratory and how much was deposited by worldwide fallout or is natural. Two distinct types of samples were processed: segments of a continuous vertical core of the entire accumulated sediment sequence and other samples from across the lake bottom at the water/sediment interface. Based on measurement of the {sup 240}Pu/{sup 239}Pu atom ratio, Laboratory-derived plutonium is present in eight of nine samples at the core site. On a depth-weighted basis, approximately one-half of the {sup 239}Pu and {sup 240}Pu came from early operations at the Laboratory; the remaining plutonium came from fallout dispersed by above-ground nuclear tests. In contrast to the core site, the samples from the other locations showed little or no evidence of Laboratory-derived plutonium, with more than 90 percent of the plutonium attributable to fallout. The overall amount of plutonium in all the samples is of the same magnitude as other reservoirs in the region. The net increase in plutonium over upstream reservoirs unaffected by Laboratory activities is a maximum of 0.014 pCi/g or 3.5 times. All of the samples reflect natural uranium compositions. Laboratory-derived uranium is not identifiable, presumably because the sediment contains abundant

  4. High-resolution laser spectroscopy of long-lived plutonium isotopes

    Voss, A.; Sonnenschein, V.; Campbell, P.; Cheal, B.; Kron, T.; Moore, I. D.; Pohjalainen, I.; Raeder, S.; Trautmann, N.; Wendt, K.

    2017-03-01

    Long-lived isotopes of plutonium were studied using two complementary techniques, high-resolution resonance ionization spectroscopy (HR-RIS) and collinear laser spectroscopy (CLS). Isotope shifts have been measured on the 5 f67 s27F0→5 f56 d27 s (J =1 ) and 5 f67 s27F1→5 f67 s 7 p (J =2 ) atomic transitions using the HR-RIS method and the hyperfine factors have been extracted for the odd mass nuclei Pu,241239. CLS was performed on the 5 f67 s 8F1 /2→J =1 /2 (27 523.61 cm-1) ionic transition with the hyperfine A factors measured for 239Pu. Changes in mean-squared charge radii have been extracted and show a good agreement with previous nonoptical methods, with an uncertainty improvement by approximately one order of magnitude. Plutonium represents the heaviest element studied to date using collinear laser spectroscopy.

  5. Plutonium and uranium contamination in soils from former nuclear weapon test sites in Australia

    Child, D. P.; Hotchkis, M. A. C.

    2013-01-01

    The British government performed a number of nuclear weapon tests on Australian territory from 1952 through to 1963 with the cooperation of the Australian government. Nine fission bombs were detonated in South Australia at Emu Junction and Maralinga, and a further three fission weapons were detonated in the Monte Bello Islands off the coast of Western Australia. A number of soil samples were collected by the Australian Radiation Laboratories in 1972 and 1978 during field surveys at these nuclear weapon test sites. They were analysed by gamma spectrometry and, for a select few samples, by alpha spectrometry to measure the remaining activities of fission products, activation products and weapon materials. We have remeasured a number of these Montebello Islands and Emu Junction soil samples using the ANTARES AMS facility, ANSTO. These samples were analysed for plutonium and uranium isotopic ratios and isotopic concentrations. Very low 240Pu/239Pu ratios were measured at both sites (∼0.05 for Alpha Island and ∼0.02 for Emu Field), substantially below global fallout averages. Well correlated but widely varying 236U and plutonium concentrations were measured across both sites, but 233U did not correlate with these other isotopes and instead showed correlation with distance from ground zero, indicating in situ production in the soils.

  6. Uranium isotope separation from 1941 to the present

    Maier-Komor, Peter, E-mail: Peter@Maier-Komor.d [Retired from Physik-Department E12, Technische Universitaet Muenchen, D-85747 Garching (Germany)

    2010-02-11

    Uranium isotope separation was the key development for the preparation of highly enriched isotopes in general and thus became the seed for target development and preparation for nuclear and applied physics. In 1941 (year of birth of the author) large-scale development for uranium isotope separation was started after the US authorities were warned that NAZI Germany had started its program for enrichment of uranium and might have confiscated all uranium and uranium mines in their sphere of influence. Within the framework of the Manhattan Projects the first electromagnetic mass separators (Calutrons) were installed and further developed for high throughput. The military aim of the Navy Department was to develop nuclear propulsion for submarines with practically unlimited range. Parallel to this the army worked on the development of the atomic bomb. Also in 1941 plutonium was discovered and the production of {sup 239}Pu was included into the atomic bomb program. {sup 235}U enrichment starting with natural uranium was performed in two steps with different techniques of mass separation in Oak Ridge. The first step was gas diffusion which was limited to low enrichment. The second step for high enrichment was performed with electromagnetic mass spectrometers (Calutrons). The theory for the much more effective enrichment with centrifugal separation was developed also during the Second World War, but technical problems e.g. development of high speed ball and needle bearings could not be solved before the end of the war. Spying accelerated the development of uranium separation in the Soviet Union, but also later in China, India, Pakistan, Iran and Iraq. In this paper, the physical and chemical procedures are outlined which lead to the success of the project. Some security aspects and Non-Proliferation measures are discussed.

  7. Uranium isotope separation from 1941 to the present

    Maier-Komor, Peter

    2010-02-01

    Uranium isotope separation was the key development for the preparation of highly enriched isotopes in general and thus became the seed for target development and preparation for nuclear and applied physics. In 1941 (year of birth of the author) large-scale development for uranium isotope separation was started after the US authorities were warned that NAZI Germany had started its program for enrichment of uranium and might have confiscated all uranium and uranium mines in their sphere of influence. Within the framework of the Manhattan Projects the first electromagnetic mass separators (Calutrons) were installed and further developed for high throughput. The military aim of the Navy Department was to develop nuclear propulsion for submarines with practically unlimited range. Parallel to this the army worked on the development of the atomic bomb. Also in 1941 plutonium was discovered and the production of 239Pu was included into the atomic bomb program. 235U enrichment starting with natural uranium was performed in two steps with different techniques of mass separation in Oak Ridge. The first step was gas diffusion which was limited to low enrichment. The second step for high enrichment was performed with electromagnetic mass spectrometers (Calutrons). The theory for the much more effective enrichment with centrifugal separation was developed also during the Second World War, but technical problems e.g. development of high speed ball and needle bearings could not be solved before the end of the war. Spying accelerated the development of uranium separation in the Soviet Union, but also later in China, India, Pakistan, Iran and Iraq. In this paper, the physical and chemical procedures are outlined which lead to the success of the project. Some security aspects and Non-Proliferation measures are discussed.

  8. Characterization and Source Term Assessments of Radioactive Particles from Marshall Islands Using Non-Destructive Analytical Techniques

    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. Rapid isolation of plutonium in environmental solid samples using sequential injection anion exchange chromatography followed by detection with inductively coupled plasma mass spectrometry

    Qiao Jixin, E-mail: jixin.qiao@risoe.d [Radiation Research Division, Riso National Laboratory for Sustainable Energy, Technical University of Denmark, DK-4000 Roskilde (Denmark); Hou Xiaolin; Roos, Per [Radiation Research Division, Riso National Laboratory for Sustainable Energy, Technical University of Denmark, DK-4000 Roskilde (Denmark); Miro, Manuel [Department of Chemistry, Faculty of Sciences, University of the Balearic Islands, Carretera de Valldemossa km. 7.5, E-07122 Palma de Mallorca, Illes Balears (Spain)

    2011-01-31

    This paper reports an automated analytical method for rapid determination of plutonium isotopes ({sup 239}Pu and {sup 240}Pu) in environmental solid extracts. Anion exchange chromatographic columns were incorporated in a sequential injection (SI) system to undertake the automated separation of plutonium from matrix and interfering elements. The analytical results most distinctly demonstrated that the crosslinkage of the anion exchanger is a key parameter controlling the separation efficiency. AG 1-x4 type resin was selected as the most suitable sorbent material for analyte separation. Investigation of column size effect upon the separation efficiency revealed that small-sized (2 mL) columns sufficed to handle up to 50 g of environmental soil samples. Under the optimum conditions, chemical yields of plutonium exceeded 90% and the decontamination factors for uranium, thorium and lead ranged from 10{sup 3} to 10{sup 4}. The determination of plutonium isotopes in three standard/certified reference materials (IAEA-375 soil, IAEA-135 sediment and NIST-4359 seaweed) and two reference samples (Irish Sea sediment and Danish soil) revealed a good agreement with reference/certified values. The SI column-separation method is straightforward and less labor intensive as compared with batch-wise anion exchange chromatographic procedures. Besides, the automated method features low consumption of ion-exchanger and reagents for column washing and elution, with the consequent decrease in the generation of acidic waste, thus bearing green chemical credentials.

  10. Rapid isolation of plutonium in environmental solid samples using sequential injection anion exchange chromatography followed by detection with inductively coupled plasma mass spectrometry.

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

    2011-01-31

    This paper reports an automated analytical method for rapid determination of plutonium isotopes ((239)Pu and (240)Pu) in environmental solid extracts. Anion exchange chromatographic columns were incorporated in a sequential injection (SI) system to undertake the automated separation of plutonium from matrix and interfering elements. The analytical results most distinctly demonstrated that the crosslinkage of the anion exchanger is a key parameter controlling the separation efficiency. AG 1-×4 type resin was selected as the most suitable sorbent material for analyte separation. Investigation of column size effect upon the separation efficiency revealed that small-sized (2 mL) columns sufficed to handle up to 50 g of environmental soil samples. Under the optimum conditions, chemical yields of plutonium exceeded 90% and the decontamination factors for uranium, thorium and lead ranged from 10(3) to 10(4). The determination of plutonium isotopes in three standard/certified reference materials (IAEA-375 soil, IAEA-135 sediment and NIST-4359 seaweed) and two reference samples (Irish Sea sediment and Danish soil) revealed a good agreement with reference/certified values. The SI column-separation method is straightforward and less labor intensive as compared with batch-wise anion exchange chromatographic procedures. Besides, the automated method features low consumption of ion-exchanger and reagents for column washing and elution, with the consequent decrease in the generation of acidic waste, thus bearing green chemical credentials.

  11. DEVELOPMENT OF AN IMPROVED TITANATE-BASED SORBENT FOR STRONTIUM AND ACTINIDE SEPARATIONS UNDER STRONGLY ALKALINE CONDITIONS

    Hobbs, D.; Peters, T.; Taylor-Pashow, K.; Fink, S.

    2010-02-18

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 134,137}Cs, {sup 90}Sr, and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes at SRS include the sorption of {sup 90}Sr and alpha-emitting radionuclides onto monosodium titanate (MST) and caustic side solvent extraction of {sup 137}Cs. The MST and separated {sup 137}Cs is encapsulated along with the sludge fraction of high-level waste (HLW) into a borosilicate glass waste form for eventual entombment at a federal repository. The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu, and {sup 240}Pu; {sup 237}Np; and uranium isotopes, {sup 235}U and {sup 238}U. This paper describes recent results evaluating the performance of an improved sodium titanate material that exhibits increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the current baseline material, MST.

  12. Plutonium measurements on the 1 MV AMS system at the Centro Nacional de Aceleradores (CNA)

    Chamizo, Elena [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain)], E-mail: elechacal@alum.us.es; Enamorado, Santiago Miguel [Centro Nacional de Aceleradores (CNA), Avda. Thomas Alva Edison 7, Isla de la Cartuja, 41092 Seville (Spain); Garcia-Leon, Manuel [Departamento de Fisica Atomica, Molecular y Nuclear, Avda. Reina Mercedes, s/n, 41012 Seville (Spain); Suter, Martin; Wacker, Lukas [Institute of Particle Physics, ETH-Zurich, CH-8093 Zurich (Switzerland)

    2008-11-15

    Plutonium isotopes have been recently added to the list of radionuclides that can be measured with the new generation of compact AMS facilities. In this paper we present first experimental results concerning the development of the plutonium AMS technique at 680 kV on the 1 MV AMS system at the Centro Nacional de Aceleradores (CNA) in Sevilla, Spain. This is the first compact AMS machine designed and manufactured by High Voltage Engineering Europa. As we demonstrate, the obtained backgrounds for {sup 239,240}Pu, of about 10{sup 6} atoms, and the {sup 239}Pu/{sup 238}U mass suppression factor, in the range of 10{sup -9}, compare to the ones achieved on other AMS facilities. With the measurement of reference materials provided by the International Atomic Energy Agency (IAEA-375, IAEA-Soil-6, IAEA-381) and samples already studied on the 600 kV compact ETH/PSI AMS system at Zuerich, we show that the CNA system can be perfectly used for the routine measurement of plutonium isotopes at environmental levels.

  13. Reference material manufacture and certification for the AVNG

    Hauck, Danielle K [Los Alamos National Laboratory; Mac Arthur, Duncan [Los Alamos National Laboratory; Thron, Jonathan L [Los Alamos National Laboratory; Livke, Alexander [VNIIEF; Kondratov, Sergey [VNIIEF; Razinkov, Sergey [VNIIEF

    2010-01-01

    Testing and demonstration of any radiation measurement system requires the use of appropriate radioactive sources. The AVNG implementation that we describe is an attribute measurement system 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.' The AVNG was tested using a number of reference material (RM) sources with masses and isotopic ratios above and below these thresholds. The AVNG was demonstrated in June 2009 using several of these sources in addition to detector calibration sources. Since the AVNG was designed to measure multi-kg plutonium sources, the RM was manufactured specifically for use with this system. In addition, the RM was used to test the thresholds in the AVNG, so the size and composition of each RM was certified prior to use. In this presentation, we will describe the various steps in the manufacture and certification of these RM sources.

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

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

    2010-12-01

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

  15. The 239 Pu(n,2n)238Pu cross section: preliminary calculations

    Chen, H; Reffo, G; Ross, M A; White, R M

    1999-03-12

    The primary motivation for the present work is to provide theoretical values for the ratio of the partial 239Pu(n,2nx{gamma})238Pu to total 239 Pu(n,2n)238Pu cross section for several discrete gamma transitions. Results and conclusions of preliminary calculations from threshold to 20 MeV are presented. Calculations are based on theoretical models with parameters obtained from the literature or from our ad hoc systematics. Optical model cross sections and transmission coefficients were determined using the coupled-channels method. The calculations included a preequilibrium component followed by multiple particle and gamma-ray emissions. Fission competition was included at all stages of de-excitation. Suggestions for further verifications and possible improvements are provided.

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

    Hollas, C.L.; Arnone, G.; Brunson, G.; Coop, K. [Los Alamos National Lab., NM (United States)

    1997-11-01

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

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

    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

  18. Determination of Isotopic Composition of Uranium and Plutonium in Simulated 1AF Feed Solution by TIMS%TIMS测定模拟1AF料液中铀钚同位素组分

    蒋军清; 高月华; 汪南杰; 姜国杜

    2012-01-01

    The precise determination of the uranium and plutonium isotopic composition in the simulated 1AF feed solution by solvent extraction/ion exchange separation-thermal ioni-zation mass spectroscopy(TIMS) was studied in this paper. The precise determination of uranium and plutonium isotopic composition was realized by optimization of chemical separations, and minimization of possible interferences, and proper selection of instrument parameters. Under the selected conditions, the uranium and plutonium isotopic composition in the 1AF feed solution were accurately determined. The relative standard deviations of the main isotopes 235U and 239Pu are less than 0. 05%.%采用溶剂萃取/离子交换分离-热表面电离质谱法,对模拟1AF料液中铀钚同位素组分测定技术进行了研究.通过对化学分离条件、仪器测量参数、信号强度、各种干扰等测定条件的研究和选择,实现了铀、钚同位素组分的精密测定.在选定的条件下,测定了模拟1AF料液中的铀钚同位素,主要同位素235 U和239pu测定精密度(sr)均优于0.05%.

  19. Elemental bio-imaging of thorium, uranium, and plutonium in tissues from occupationally exposed former nuclear workers.

    Hare, Dominic; Tolmachev, Sergei; James, Anthony; Bishop, David; Austin, Christine; Fryer, Fred; Doble, Philip

    2010-04-15

    Internal exposure from naturally occurring radionuclides (including the inhaled long-lived actinides (232)Th and (238)U) is a component of the ubiquitous background radiation dose (National Council on Radiation Protection and Measurements. Ionizing radiation exposure of the population of the United States; NCRP Report No. 160; NCRP: Bethesda, MD, 2009). It is of interest to compare the concentration distribution of these natural alpha-emitters in the lungs and respiratory lymph nodes with those resulting from occupational exposure, including exposure to anthropogenic plutonium and depleted and enriched uranium. This study examines the application of laser ablation-inductively coupled plasma-mass spectrometry (LA-ICPMS) to quantifying and visualizing the mass distribution of uranium and thorium isotopes from both occupational and natural background exposure in human respiratory tissues and, for the first time, extends this application to the direct imaging of plutonium isotopes. Sections of lymphatic and lung tissues taken from deceased former nuclear workers with a known history of occupational exposure to specific actinide elements (uranium, plutonium, or americium) were analyzed by LA-ICPMS. Using a previously developed LA-ICPMS protocol for elemental bio-imaging of trace elements in human tissue and a new software tool, we generated images of thorium ((232)Th), uranium ((235)U and (238)U), and plutonium ((239)Pu and (240)Pu) mass distributions in sections of tissue. We used a laboratory-produced matrix-matched standard to quantify the (232)Th, (235)U, and (238)U concentrations. The plutonium isotopes (239)Pu and (240)Pu were detected by LA-ICPMS in 65 mum diameter localized regions of both a paratracheal lymph node and a sample of lung tissue from a person who was occupationally exposed to refractory plutonium (plutonium dioxide). The average (overall) (239)Pu concentration in the lymph node was 39.2 ng/g, measured by high purity germanium (HPGe) gamma

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

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

    1997-09-22

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

  1. Measurement of Uranium Isotopes in Particles of U3O8 by Secondary Ion Mass Spectrometry-Single-Stage Accelerator Mass Spectrometry (SIMS-SSAMS).

    Fahey, Albert J; Groopman, Evan E; Grabowski, Kenneth S; Fazel, Kamron C

    2016-07-19

    A commercial secondary ion mass spectrometer (SIMS) was coupled to a ± 300 kV single-stage accelerator mass spectrometer (SSAMS). Positive secondary ions generated with the SIMS were injected into the SSAMS for analysis. This combined instrument was used to measure the uranium isotopic ratios in particles of three certified reference materials (CRM) of uranium, CRM U030a, CRM U500, and CRM U850. The ability to inject positive ions into the SSAMS is unique for AMS systems and allows for simple analysis of nearly the entire periodic table because most elements will readily produce positive ions. Isotopic ratios were measured on samples of a few picograms to nanograms of total U. Destruction of UH(+) ions in the stripper tube of the SSAMS reduced hydride levels by a factor of ∼3 × 10(4) giving the UH(+)/U(+) ratio at the SSAMS detector of ∼1.4 × 10(-8). These hydride ion levels would allow the measurement of (239)Pu at the 10 ppb level in the presence of U and the equivalent of ∼10(-10 236)U concentration in natural uranium. SIMS-SSAMS analysis of solid nuclear materials, such as these, with signals nearly free of molecular interferences, could have a significant future impact on the way some measurements are made for nuclear nonproliferation.

  2. An assessment of the reported leakage of anthropogenic radionuclides from the underground nuclear test sites at Amchitka Island, Alaska, USA to the surface environment

    Dasher, Douglas E-mail: ddasher@envircon.state.ak.us; Hanson, Wayne; Read, Stan; Faller, Scott; Farmer, Dennis; Efurd, Wes; Kelley, John; Patrick, Robert

    2002-07-01

    Three underground nuclear tests representing approximately 15-16% of the total effective energy released during the United States underground nuclear testing program from 1951 to 1992 were conducted at Amchitka Island, Alaska. In 1996, Greenpeace reported that leakage of radionuclides, {sup 241}Am and {sup 239+240}Pu, from these underground tests to the terrestrial and freshwater environments had been detected. In response to this report, a federal, state, tribal and non-governmental team conducted a terrestrial and freshwater radiological sampling program in 1997. Additional radiological sampling was conducted in 1998. An assessment of the reported leakage to the freshwater environment was evaluated by assessing {sup 3} H values in surface waters and {sup 240}Pu/{sup 239}Pu ratios in various sample media. Tritium values ranged from 0.41 Bq/l{+-}0.11 two sigma to 0.74 Bq/l{+-}0.126 two sigma at the surface water sites sampled, including the reported leakage sites. Only at the Long Shot test site, where leakage of radioactive gases to the near-surface occurred in 1965, were higher {sup 3}H levels of 5.8 Bq/l{+-}0.19 two sigma still observed in 1997, in mud pit no. 3. The mean {sup 240}Pu/{sup 239}Pu for all of the Amchitka samples was 0.1991{+-}0.0149 one standard deviation, with values ranging from 0.1824{+-}1.43% one sigma to 0.2431{+-}6.56% one sigma. The measured {sup 3}H levels and {sup 240}Pu/{sup 239}Pu ratios in freshwater moss and sediments at Amchitka provide no evidence of leakage occurring at the sites reported by Buske and Miller (1998 Nuclear-Weapons-Free America and Alaska Community Action on Toxics, Anchorage, Ak, p. 38) and Miller and Buske (1996 Nuclear Flashback: The Return to Anchitka, p. 35). It was noted that the marine sample; {sup 240}Pu/{sup 239}Pu ratios are statistically different than the global fallout ratios presented by Krey et al. (1976) and Kelley, Bond, and Beasley (1999). The additional non-fallout component {sup 240}Pu/{sup 239}Pu

  3. Estimation of Radiation Doses in the Marshall Islands Based on Whole Body Counting of Cesium-137 (137Cs) and Plutonium Urinalysis

    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

  4. Estimation of Radiation Doses in the Marshall Islands Based on Whole Body Counting of Cesium-137 (137Cs) and Plutonium Urinalysis

    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

  5. Radio-ecological researches in the Sea of Japan and northwestern part of the Pacific Ocean after accident on the Japanese nuclear power plant 'Fukushima-1': the content of plutonium isotopes and strontium-90 in sea water

    Fedorova, A. [Research and Production Association - RPA Typhoon (Russian Federation)

    2014-07-01

    In April-May 2011 and in August-September 2012 'Roshydromet' has conducted radio ecological researches in the Sea of Japan and on the water area of northwestern part of the Pacific Ocean (Kuril-Kamchatka area and the area of the Kuroshio current), which had purpose to make assessment of contamination hazard that can be caused to the coast of Russian Far East because of emergency releases of radioactive materials on the nuclear power plant 'Fukushima-1'. During the research works was done the sampling and processing of sea water samples not only for detection of Cs{sup 134}, Cs{sup 137}, but also for such radio-ecological significant long-living radionuclides, as {sup 90}Sr, plutonium isotopes ({sup 239,240}Pu) and tritium. Information about radionuclides was required for correct assessment of nuclear power plant 'Fukushima-1' aftermath on the Far Eastern sea water areas, but was not available in the beginning of research. In the present report the radiochemical measuring results on content of plutonium isotopes and {sup 90}Sr in the sea water from researched areas are presented. Sampling was done from the various horizons. Surface and deep water samples were filtered via the compound filter which made it possible to filter particles bigger than 1 micron. Radiochemical testing of the {sup 90}Sr and plutonium isotopes content was done separately on a suspension and in a filtrate of sea water samples. The content of {sup 90}Sr in the filtrate of the sea water that had been selected in 2011, ranges 0,7-2,4 Bq/m{sup 3}, in suspensions the interval makes 0,0013-0,021 Bq/m3. The results received in researches in 2012 are in range of 0,5-2,6 Bq/m{sup 3} of the sea water filtrate. According to results of IAEA in 2000, the average content of {sup 90}Sr in surface water of the Sea of Japan made 1,6 Bq/m{sup 3}. Hereby, the data obtained in researches in 2011-2012 agrees with results which had been presented by IAEA before the accident. The

  6. Semi-empirical Calculation for Yield of 240Pu Spontaneous Fission

    SHU; Neng-chuan; LIU; Li-le; CHEN; Xiao-song; LIU; Ting-jin; SUN; Zheng-jun; CHEN; Yong-jing; QIAN; Jing

    2012-01-01

    <正>The spontaneous fission yield has important implication in the nuclear engineering. This work used semi-empirical model to calculate its chain yield, the result shows good agreement with the measured data. There are only 3 sets of measured data, and only too gave the chain yields and cumulative yields, covering 17 chains. It is not enough to satisfy the requirement of users. So it is needed to use theoretical model to calculate the chain yield without measured data.

  7. Artificial (Pu {sup 90}Sr, {sup 241}Am) and natural (U) isotopes in human bones from Poland

    Mietelski, J.W.; Tomankiewicz, E. [Institute of Nuclear Phyics (Poland); Golec, E.; Golec, J.; Nowak, S.; Szczygiel, E. [The 5th Military Clinical Hospital and Polyclinic (Poland); Kuzma, K. [General Hospital (Poland)

    2014-07-01

    In two papers we have presented results if analyses of artificial isotopes ({sup 238,239,240}Pu, {sup 241}Am and {sup 90}Sr) content in human bones, using samples collected during hip joint replacement surgery. Since the patients were members of general population (not exposed in any particular form to artificial radionuclides) results can be treated as current background level for Poland and perhaps also whole central Europe. During this project the open question appeared - what is the level in human bones of natural alpha emitters like {sup 238}U-, {sup 234}U, for instance. Therefore about 30 human hip joint bone samples are being now analysed for the presence of uranium along with mentioned above artificial radionuclides. Samples are ashen and sequential radiochemical analyse is applied for separation of Pu, Sr and Am isotopes followed by separation of uranium using anion exchange resin. Measurements of plutonium, americium and uranium are performed using alpha spectrometry. That for {sup 90}Sr is done by LSC. Results will be presented during conference. Document available in abstract form only. (authors)

  8. Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean

    Lindahl, Patric [Department of Radiation Physics, Lund University Hospital, SE-221 85 Lund (Sweden) and Korea Ocean Research and Development Institute, Ansan P.O. Box 29, Seoul 425-600 (Korea, Republic of)]. E-mail: patriclindahl@yahoo.com; Roos, Per [Risoe National Laboratory, P.O. Box 49, DK-4000 Roskilde (Denmark); Holm, Elis [Department of Radiation Physics, Lund University Hospital, SE-221 85 Lund (Sweden); Risoe National Laboratory, P.O. Box 49, DK-4000 Roskilde (Denmark); Dahlgaard, Henning [Risoe National Laboratory, P.O. Box 49, DK-4000 Roskilde (Denmark)

    2005-07-01

    The long-lived anthropogenic radionuclides {sup 237}Np, {sup 239}Pu and {sup 240}Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The {sup 237}Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16 {+-} 0.02 to 1.02 {+-} 0.09 mBq kg{sup -1} (dry weight) and 0.65 {+-} 0.02 to 1.69 {+-} 0.02 mBq m{sup -3}, respectively, depending on the location and sampling year. Most of the {sup 237}Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The {sup 240}Pu/{sup 239}Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17 {+-} 0.03. The {sup 237}Np and {sup 239}Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16 {+-} 0.01 to 0.62 {+-} 0.08 mBq m{sup -3} and from 0.64 {+-} 0.05 to 4.27 {+-} 0.08 mBq m{sup -3}, respectively, and the {sup 237}Np/{sup 239}Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.

  9. Radioelement studies in the oceans. Progress report, January 1, 1977--December 31, 1977. [Transport of fallout radionuclides in Atlantic and Pacific Oceans and Mediterranean Sea during 1977

    Bowen, V.T.

    1978-04-01

    Data are reported on the content of various fallout radionuclides in samples of seawater and sediments collected during 1977 in the Atlantic Ocean, Mediterranean Sea, and Pacific Ocean. Methods used for the preparation of samples for radiometric analysis are described briefly. Radionuclides found included /sup 137/Cs, /sup 134/Cs, /sup 242/Cm, /sup 244/Cm, /sup 90/Sr, /sup 238/Pu, /sup 239/Pu, /sup 240/Pu, and /sup 241/Am. A list is included of publications during the time period covered by this report.

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

    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

  11. Arctic Ocean sea ice drift origin derived from artificial radionuclides

    Camara-Mor, P., E-mail: patricia.camara@uab.es [Institut de Ciencia i Tecnologia Ambientals, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); Masque, P. [Institut de Ciencia i Tecnologia Ambientals, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); Dpt. de Fisica, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); Garcia-Orellana, J. [Institut de Ciencia i Tecnologia Ambientals, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); Dpt. de Fisica, Universitat Autonoma de Barcelona, E-08193. Bellaterra (Spain); School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY 11794-5000 (United States); Cochran, J.K. [School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY 11794-5000 (United States); Mas, J.L. [Dpto. de Fisica Aplicada, Universidad de Sevilla, 41012, Seville. Spain (Spain); Chamizo, E. [Centro Nacional de Aceleradores (CNA), Avd. Thomas Alva Edison 7, Isla de la Cartuja, E-41092, Seville (Spain); Hanfland, C. [Alfred Wegener Institute for Polar and Marine Research, Am Handelshafen 12, D-27570 Bremerhaven (Germany)

    2010-07-15

    Since the 1950s, nuclear weapon testing and releases from the nuclear industry have introduced anthropogenic radionuclides into the sea, and in many instances their ultimate fate are the bottom sediments. The Arctic Ocean is one of the most polluted in this respect, because, in addition to global fallout, it is impacted by regional fallout from nuclear weapon testing, and indirectly by releases from nuclear reprocessing facilities and nuclear accidents. Sea-ice formed in the shallow continental shelves incorporate sediments with variable concentrations of anthropogenic radionuclides that are transported through the Arctic Ocean and are finally released in the melting areas. In this work, we present the results of anthropogenic radionuclide analyses of sea-ice sediments (SIS) collected on five cruises from different Arctic regions and combine them with a database including prior measurements of these radionuclides in SIS. The distribution of {sup 137}Cs and {sup 239,240}Pu activities and the {sup 240}Pu/{sup 239}Pu atom ratio in SIS showed geographical differences, in agreement with the two main sea ice drift patterns derived from the mean field of sea-ice motion, the Transpolar Drift and Beaufort Gyre, with the Fram Strait as the main ablation area. A direct comparison of data measured in SIS samples against those reported for the potential source regions permits identification of the regions from which sea ice incorporates sediments. The {sup 240}Pu/{sup 239}Pu atom ratio in SIS may be used to discern the origin of sea ice from the Kara-Laptev Sea and the Alaskan shelf. However, if the {sup 240}Pu/{sup 239}Pu atom ratio is similar to global fallout, it does not provide a unique diagnostic indicator of the source area, and in such cases, the source of SIS can be constrained with a combination of the {sup 137}Cs and {sup 239,240}Pu activities. Therefore, these anthropogenic radionuclides can be used in many instances to determine the geographical source area of sea-ice.

  12. Effect of anaerobic contributions to the uranium content in marine sediments; Efecto de aportes anaerobios en el contenido de uranio en sedimentos marinos

    Ordonez R, E. [ININ, Departamento de Quimica, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico); Ruiz F, A. C. [UNAM, Instituto de Ciencias del Mar y Limnologia, Unidad Academica Mazatlan, Cap. Joel Montes Camarena, Cerro del Vigia, 82040 Mazatlan, Sinaloa (Mexico); Jimenez D, E.; Guerrero J, M., E-mail: eduardo.ordonez@inin.gob.mx [Universidad Autonoma del Estado de Mexico, Facultad de Planeacion Urbana y Regional, Paseo Tollocan esq. Mariano Matamoros, 50130 Toluca, Estado de Mexico (Mexico)

    2014-10-15

    In this work a sediment group obtained in the seabed near the mouth of the Santiago River, physical analyzes show that there is little activity of microscopic marine life, revealed by exoskeletons of foraminifera. Although the amount of organic matter occurs normally, around 20%, is assumed that this contribution is due to the large amount of organic waste scattered by the effluent of the river, causing an abnormally high anaerobic activity, clearly shown by the large amount of pyrite specific framboids found along the nucleus profile of 23 cm of sediment. In the analyzed fractions the uranium concentration and its isotope ratio was studied: which vary from 3.19 Bq/kg for the more superficial fractions down gradually to less than 1 Bq/kg for deeper fractions. An outstanding fact is that the surface fractions have an isotope ratio {sup 234}U/{sup 238}U unusually low for fractions 1-4 cm of deep, close to 0.4, indicating a strong reaction of few years ago on the radiogenic descendants of {sup 238}U, leaching essentially the {sup 234}Th and causing this abnormal radioactive imbalance. The plutonium has become an element found commonly in the surface layers of the sea and coastlines, finding in the top layer an activity of 2.78 Bq/kg ({sup 239}Pu + {sup 240}Pu). The high contamination of the mouth of Santiago River has changed the conditions of the micro fauna as well as of the chemical equilibrium of the natural elements. (Author)

  13. Heterogeneous reduction of {sup 239}PuO{sub 2} by aqueous Fe(II) in the presence of hematite

    Felmy, A.R.; Moore, D.A.; Qafoku, O.; Buck, E.; Ilton, E.S. [Pacific Northwest National Laboratory, Richland, WA (United States); Conradson, S.D. [Los Alamos National Laboratory, NM (United States)

    2013-07-01

    The reduction of PuO{sub 2}(am) by Fe(II) in the presence and absence of hematite was studied over a range of pH values and oxidation/reduction potentials. In contrast to thermodynamic predictions, the presence of hematite did not have a major effect on the overall reduction of PuO{sub 2}(am) to aqueous Pu(III). Instead the aqueous Pu(III) concentrations at longer time frames were accurately predicted using the measured Fe(II) concentration and existing thermodynamic data for the reaction: H{sub 2}O + H{sup +} + Fe{sup 2+} + PuO{sub 2}(am) {r_reversible} Pu{sup 3+} + Fe(OH){sub 3}(am) with log K = -0.6. The accuracy of this approach in all solutions containing aqueous Fe(II), coupled with the apparent lack of oxidation of Fe(II) by O{sub 2}(g), suggests that the Fe(OH){sub 3}(am) is formed by the oxidation of Fe(II) to Fe(III) by radiolysis. The continued generation of reactive amorphous iron hydroxide by radiolysis prevents thermodynamic equilibrium from being reached with more stable ferric oxide compounds, except possibly under acidic conditions where amorphous ferric hydroxide is soluble. The use of measured pe values, instead of aqueous Fe(II) measurements, also yields reasonable predictions of the final Pu(III) concentrations although the predictions are more uncertain. (orig.)

  14. Evaluation of fission product yields from fission spectrum n+239Pu using a meta analysis of benchmark data

    Chadwick, Mark B.

    2009-10-01

    Los Alamos conducted a dual fission-chamber experiment in the 1970s in the Bigten critical assembly to determine fission product data in a fast (fission neutron spectrum) environment, and this defined the Laboratory's fission basis today. We describe how the data from this experiment are consistent with other benchmark fission product yield measurements for 95,97Zr, 140Ba, 143,144Ce, 137Cs from the NIST-led ILRR fission chamber experiments, and from Maeck's mass-spectrometry data. We perform a new evaluation of the fission product yields that is planned for ENDF/B-VII.1. Because the measurement database for some of the FPs is small—especially for 147Nd and 99Mo—we use a meta-analysis that incorporates insights from other accurately-measured benchmark FP data. The %-relative changes compared to ENDF/B-VI are small for some FPs (less than 1% for 95Zr, 140Ba, 144Ce), but are larger for 99Mo (3%) and 147Nd (5%). We suggest an incident neutron energy dependence to the 147Nd fission product yield that accounts for observed differences in the FPY at a few-hundred keV average energy in fast reactors versus measurements made at higher average energies.

  15. Combined application of alpha-track and fission-track techniques for detection of plutonium particles in environmental samples prior to isotopic measurement using thermo-ionization mass spectrometry.

    Lee, Chi-Gyu; Suzuki, Daisuke; Esaka, Fumitaka; Magara, Masaaki; Kimura, Takaumi

    2011-07-15

    The fission track technique is a sensitive detection method for particles which contain radio-nuclides like (235)U or (239)Pu. However, when the sample is a mixture of plutonium and uranium, discrimination between uranium particles and plutonium particles is difficult using this technique. In this study, we developed a method for detecting plutonium particles in a sample mixture of plutonium and uranium particles using alpha track and fission track techniques. The specific radioactivity (Bq/g) for alpha decay of plutonium is several orders of magnitude higher than that of uranium, indicating that the formation of the alpha track due to alpha decay of uranium can be disregarded under suitable conditions. While alpha tracks in addition to fission tracks were detected in a plutonium particle, only fission tracks were detected in a uranium particle, thereby making the alpha tracks an indicator for detecting particles containing plutonium. In addition, it was confirmed that there is a linear relationship between the numbers of alpha tracks produced by plutonium particles made of plutonium certified standard material and the ion intensities of the various plutonium isotopes measured by thermo-ionization mass spectrometry. Using this correlation, the accuracy in isotope ratios, signal intensity and measurement errors is presumable from the number of alpha tracks prior to the isotope ratio measurements by thermal ionization mass spectrometry. It is expected that this method will become an effective tool for plutonium particle analysis. The particles used in this study had sizes between 0.3 and 2.0 μm.

  16. The new extended HVE 1 MV multi-element AMS system for low background installed at the Aarhus AMS Dating Centre

    Heinemeier, Jan; Olsen, Jesper [AMS " 1" 4C Dating Centre, Department of Physics and Astronomy, Aarhus University, Aarhus (Denmark); Klein, Matthias; Mous, Dirk [High Voltage Engineering Europa B.V., Amersfoort (Netherlands)

    2015-10-15

    Aarhus University, Department of Physics and Astronomy has installed a new multi-element AMS system at its AMS {sup 14}C Dating Centre. It is manufactured by High Voltage Engineering Europa B.V. and based on a 1 MV Tandetron accelerator with a dual gas system (Ar and He) for the terminal stripper. The injector is equipped with two independently operating ion sources and a 120 degree bouncer magnet with high resolution and a bending power of 340 amu at 35 keV, supporting the measurements of actinides. The high-energy (HE) spectrometer features a degrader foil for isobar suppression and a second HE magnet for suppression of ions scattered in the HE ESA, which ensures very low detection limits. The control system supports different methods for isotope switching: “traditional” fast bouncing, adjusting the Hall-probe controlled magnet fields (for, e.g., {sup 3}H), or changing the complete set of operation parameters (e.g., for actinides). During the on-site acceptance tests, the following background levels were measured: <10{sup −16} for tritium, <10{sup −15} for {sup 14}C, <10{sup −15} for {sup 10}Be (down to <10{sup −16} in a later 3 h run), 2 × 10{sup −15} for {sup 26}Al, 2 × 10{sup −13} for {sup 129}I and 9 × 10{sup −12} for {sup 41}Ca and for {sup 239}Pu ({sup 240}Pu) a 1.5 (0.5) pg per mg iron, which demonstrates the multi-element capability of the system.

  17. Evaluation of the anthropogenic radionuclide concentrations in sediments and fauna collected in the Beaufort Sea and northern Alaska

    Efurd, D.W.; Miller, G.G.; Rokop, D.J. [and others

    1997-07-01

    This study was performed to establish a quality controlled data set about the levels of radio nuclide activity in the environment and in selected biota in the U.S. Arctic. Sediment and biota samples were collected by the National Oceanic and Atmospheric Administration (NOAA), the National Biological Service, and the North Slope Borough`s Department of Wildlife Management to determine the impact of anthropogenic radionuclides in the Arctic. The results summarized in this report are derived from samples collected in northwest Alaska with emphasis on species harvested for subsistence in Barrow, Alaska. Samples were analyzed for the anthropogenic radionuclides {sup 90}Sr, {sup 137}Cs, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu and {sup 241}Am. The naturally occurring radionuclides {sup 40}K, {sup 212}Pb and {sup 214}Pb were also measured. One goal of this study was to determine the amounts of anthropogenic radionuclides present in the Beaufort Sea. Sediment samples were isotopically fingerprinted to determine the sources of radio nuclide activities. Biota samples of subsistence and ecological value were analyzed to search for evidence of bio-accumulation of radionuclides and to determine the radiation exposures associated with subsistence living in northern Alaska. The anthropogenic radio nuclide content of sediments collected in the Beaufort Sea was predominantly the result of the deposition of global fallout. No other sources of anthropogenic radionuclides could be conclusively identified in the sediments. The anthropogenic radio nuclide concentrations in fish, birds and mammals were very low. Assuming that ingestion of food is an important pathway leading to human contact with radioactive contaminants and given the dietary patterns in coastal Arctic communities, it can be surmised that marine food chains are presently not significantly affected.

  18. Seaborg's Plutonium? A Case Study in Nuclear Forensics

    Norman, Eric B.; Thomas, Keenan J.; Telhami, Kristina E.

    2015-10-01

    Passive X-ray and gamma-ray analysis was performed on UC Berkeley's EH&S Sample S338. The object was found to contain 239Pu. No other radioactive isotopes were observed. The mass of 239Pu contained in this object was determined to be 2.0 +- 0.3 μg. These observations are consistent with the identification of this object as containing the 2.77- μg PuO2 (2.44 μg 239Pu) sample produced in 1942 and described by Glenn Seaborg and his collaborators as the first sample of 239Pu that was large enough to be weighed. This work was supported in part by the U.S. Dept. of Energy National Nuclear Security Administration under Award No. DE-NA0000979.

  19. Procedures for determination of 239,240Pu, 241Am, 237Np, 234,238U, 2

    Chen, Q.J.; Aarkrog, Asker; Nielsen, Sven Poul;

    2001-01-01

    Since 1987, the Department of Nuclear Safety Research, Risø National Laboratory has developed procedures for analysis of low-level amounts of radioactivity in large samples of 200 liters seawater, 10 gram sediment, soil and other environmental materials.These analytical procedures provide high ch...

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

    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.

  1. Certified reference materials and reference methods for nuclear safeguards and security.

    Jakopič, R; Sturm, M; Kraiem, M; Richter, S; Aregbe, Y

    2013-11-01

    Confidence in comparability and reliability of measurement results in nuclear material and environmental sample analysis are established via certified reference materials (CRMs), reference measurements, and inter-laboratory comparisons (ILCs). Increased needs for quality control tools in proliferation resistance, environmental sample analysis, development of measurement capabilities over the years and progress in modern analytical techniques are the main reasons for the development of new reference materials and reference methods for nuclear safeguards and security. The Institute for Reference Materials and Measurements (IRMM) prepares and certifices large quantities of the so-called "large-sized dried" (LSD) spikes for accurate measurement of the uranium and plutonium content in dissolved nuclear fuel solutions by isotope dilution mass spectrometry (IDMS) and also develops particle reference materials applied for the detection of nuclear signatures in environmental samples. IRMM is currently replacing some of its exhausted stocks of CRMs with new ones whose specifications are up-to-date and tailored for the demands of modern analytical techniques. Some of the existing materials will be re-measured to improve the uncertainties associated with their certified values, and to enable laboratories to reduce their combined measurement uncertainty. Safeguards involve the quantitative verification by independent measurements so that no nuclear material is diverted from its intended peaceful use. Safeguards authorities pay particular attention to plutonium and the uranium isotope (235)U, indicating the so-called 'enrichment', in nuclear material and in environmental samples. In addition to the verification of the major ratios, n((235)U)/n((238)U) and n((240)Pu)/n((239)Pu), the minor ratios of the less abundant uranium and plutonium isotopes contain valuable information about the origin and the 'history' of material used for commercial or possibly clandestine purposes, and

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

    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

  3. Leatherback Isotopes

    National Oceanic and Atmospheric Administration, Department of Commerce — SWFSC is currently working on a project identifying global marine isotopes using leatherback turtles (Dermochelys coriacea) as the indicator species. We currently...

  4. Isotopic Paleoclimatology

    Bowen, R.

    Paleotemperature scales were calculated by H. C. Urey and others in the 1950s to assess past temperatures, and later work using the stable isotopes of oxygen, hydrogen, and carbon employed standards such as Peedee belemnite (PDB) and Standard Mean Ocean Water (SMOW). Subsequently, subjects as diverse as ice volume and paleotemperatures, oceanic ice and sediment cores, Pleistocene/Holocene climatic changes, and isotope chronostratigraphy extending back to the Precambrian were investigated.

  5. Isotopic chirality

    Floss, H.G. [Univ. of Washington, Seattle, WA (United States)

    1994-12-01

    This paper deals with compounds that are chiral-at least in part, due to isotope substitution-and their use in tracing the steric course of enzyme reaction in vitro and in vivo. There are other applications of isotopically chiral compounds (for example, in analyzing the steric course of nonenzymatic reactions and in probing the conformation of biomolecules) that are important but they will not be discussed in this context.

  6. Safety and Environmental Protection Division. Progress report, January 1, 1974--December 31, 1975. [Radionuclides in Bikini foods during 1974 and 1975 and environmental monitoring data for BNL during 1975

    None

    1977-01-01

    Progress is reported in the analysis of food chain samples collected during 1974 and 1975 at the Bikini Atoll in the Marshall Islands for /sup 90/Sr, /sup 137/Cs, /sup 239/Pu, /sup 240/Pu, and /sup 241/Am remaining in the environment from the 1946-1958 nuclear tests. Data on levels of radioactivity in environmental samples and SO/sub 2/ and NO/sub x/ in air samples collected in the vicinity of Brookhaven National Laboratory during 1975 are reported. Samples of surface air, surface waters, ground water, sediments and biota from streams, soils, grass, and milk were analyzed. Abstracts of papers published during 1974 and 1975 are included. (CH)

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

    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.

  8. Actinides detection in the Pacific Coast of Mexico; Deteccion de actinidos en el Litoral Pacifico de Mexico

    Ordonez R, E.; Almazan T, M. G.; Cruz C, G. J.; Ramirez S, R., E-mail: eduardo.ordonez@inin.gob.mx [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

    2013-10-15

    In this work is evaluated the activity of the alpha emitters, uranium and plutonium, in sand samples and seawater coming from diverse points of the Mexican Pacific Coast (Baja California, Jalisco, Colima and Guerrero). The used techniques were: radiochemistry separation and alpha spectrometry, with these techniques could be observed that the sand contains natural uranium and trace quantities of {sup 239}Pu and {sup 240}Pu combinations. The biggest activity in Pu was found in Finisterra, Baja California Sur (0.13 Bq/kg) and the minor (0 Bq/kg) in Miramar, Colima. The relationship between the geographical localization and the Pu activity suggests that while there is more interaction of the site with the oceanic currents, more is the content of Pu in the sands of the coast. (Author)

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

    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

  10. Multigroup covariance matrices for fast-reactor studies

    Smith, J.D. III; Broadhead, B.L.

    1981-04-01

    This report presents the multigroup covariance matrices based on the ENDF/B-V nuclear data evaluations. The materials and reactions have been chosen according to the specifications of ORNL-5517. Several cross section covariances, other than those specified by that report, are included due to the derived nature of the uncertainty files in ENDF/B-V. The materials represented are Ni, Cr, /sup 16/O, /sup 12/C, Fe, Na, /sup 235/U, /sup 238/U, /sup 239/Pu, /sup 240/Pu, /sup 241/Pu, and /sup 10/B (present due to its correlation to /sup 238/U). The data have been originally processed into a 52-group energy structure by PUFF-II and subsequently collapsed to smaller subgroup strutures. The results are illustrated in 52-group correlation matrix plots and tabulated into thirteen groups for convenience.

  11. Applications of Event-by-Event Fission Modeling with FREYA

    Vogt R.

    2012-02-01

    Full Text Available 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 239Pu(nth,f, 240Pu(sf and 252Cf(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.

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

    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

  13. Changes in the Shape of Histograms Constructed from the Results of 239-Pu Alpha-Activity Measurements Correlate with the Deviations of the Moon from the Keplerian Orbit

    Shapovalov S. N.

    2009-10-01

    Full Text Available We have found that the shape of the histograms, constructed on the basis of the results of radioactivity measurements, changes in correlation with the distortions of the lunar Keplerian orbit (due to the gravitational influence of the Sun. Taking into account that the phenomenon of "macroscopic fluctuations" (regular changes in the fine structure of histograms constructed from the results of measurements of natural processes does not depend on the nature of the process under study, one can consider the correlation of the histogram shape with the Moon's deviations from the Keplerian orbit to be independent from the nature of the process the histograms were obtained on.

  14. Changes in the Shape of Histograms Constructed from the Results of 239-Pu Alpha-Activity Measurements Correlate with the Deviations of the Moon from the Keplerian Orbit

    Shapovalov S. N.

    2009-10-01

    Full Text Available We have found that the shape of the histograms, constructed on the basis of the results of radioactivity measurements, changes in correlation with the distortions of the lunar Keplerian orbit (due to the gravitational influence of the Sun. Taking into account that the phenomenon of “macroscopic fluctuations” (regular changes in the fine structure of histograms constructed from the results of measurements of natural processes does not depend on the nature of the process under study, one can consider the correlation of the histogram shape with the Moon’s deviations from the Keplerian orbit to be independent from the nature of the process the histograms were obtained on.

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

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

    2010-03-01

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

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

    Whicker, F.W. (Colorado State Univ., Fort Collins, CO (USA)); Pinder, J.E. III; Bowling, J.W. (Savannah River Ecology Lab., Aiken, SC (USA)); Alberts, J.J. (Georgia Univ., Sapelo Island, GA (USA). Marine Inst.); Brisbin, I.L. Jr. (Savannah River Ecology Lab., Aiken, SC (USA))

    1989-05-01

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

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

    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.

  18. Variability in PuO{sub 2} Intake by Inhalation: Implications for Worker Protection at the US Department of Energy

    Scott, B.R.; Fencl, A.F

    1999-07-01

    This paper describes the stochastic exposure (SE) paradigm where, at most, small numbers of airborne toxic particles are presented for inhalation. The focus is on alpha-emitting plutonium dioxide (PuO{sub 2}) particles that may be inhaled by Department of Energy (DOE) workers. Consideration of the SE paradigm is important because intake of only a few highly radioactive PuO{sub 2} particles such as {sup 238}PuO{sub 2}, could greatly exceed the annual limit on intake (ALI) used to control worker exposure. For the SE paradigm, credible intake distributions evaluated over the population at risk are needed, rather than unreliable point estimates of intake. Credible distributions of radiation doses and health risks are also needed. Because there are limited data on humans who inhaled PuO{sub 2}, these distributions must be calculated. Calculated distributions are presented that relate to the intake of radioactivity via inhaling polydisperse PuO{sub 2} particles. The results indicate that a large variability in radioactivity intake is expected when relatively small numbers of PuO{sub 2} particles are inhaled. For the SE paradigm, one cannot know how many PuO{sub 2} particles were inhaled by an individual involved in a given inhalation exposure scenario. Thus, rather than addressing questions such as 'Did the calculated worker's intake of {sup 238}PuO{sub 2} exceed the ALI?', it is better to address questions such as 'What is the probability that {sup 238}PuO{sub 2} intake by a given worker occurred and exceeded the ALI?' Mathematical tools for addressing the latter question are presented, and examples of their applications are provided, with emphasis on possible DOE worker exposures at the Rocky Flats facility near Denver, Colorado. The alpha-emitting isotopes {sup 238}Pu, {sup 239}Pu, {sup 240}Pu and {sup 242}Pu are found at Rocky Flats. Although {sup 238}Pu is thought to be present in relatively small amounts there, intake via inhalation of only

  19. Modernizing the Fission Basis

    Tonchev, Anton; Henderson, Roger; Schunck, Nicolas; Sroyer, Mark; Vogt, Ramona

    2016-09-01

    In 1939, Niels Bohr and John Wheeler formulated a theory of neutron-induced nuclear fission based on the hypothesis of the compound nucleus. Their theory, the so-called ``Bohr hypothesis,'' is still at the heart of every theoretical fission model today and states that the decay of a compound nucleus for a given excitation energy, spin, and parity is independent of its formation. We propose the first experiment to validate to 1-2% absolute uncertainties the practical consequences of the Bohr hypothesis during induced nuclear fission. We will compare the fission product yields (FPYs) of the same 240Pu compound nucleus produced via two different reactions (i) n+239Pu and (ii) γ+240 Pu. These high-precision FPYs measurements will be extremely beneficial for our fundamental understanding of the nuclear fission process and nuclear reactions from first principles. This work was performed under the auspices of US DOE by LLNL under Contract DE-AC52-07NA27344. Funding was provided via the LDRD-ERD-069 project.

  20. 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.

    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.

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

    Pham, M.K. [Marine Environment Laboratories, International Atomic Energy Agency, MC 98000 Principality of Monaco (Monaco)], E-mail: m.pham@iaea.org; Sanchez-Cabeza, J.A.; Povinec, P.P. [Marine Environment Laboratories, International Atomic Energy Agency, MC 98000 Principality of Monaco (Monaco); Andor, K. [Frederic Joliot-Curie National Research Inst. for Radiobiology and Radiohygiene, Anna u. 5, 1221 Budapest (Hungary); Arnold, D. [Physikalisch-Technische Bundesanstalt, Bundesallee 100, 38116 Braunschweig (Germany); Benmansour, M. [Centre National de l' Energies des Sciences et des Techniques Nucleaires, 1382 Agdal, Rabat 10001 (Morocco); Bikit, I. [Dept. of Physics, Faculty of Science and Mathematics, University of Novi Sad, Trg Dositeja Obradovica 4, 21000 Novi Sad, Serbia (Serbia ); Carvalho, F.P. [Instituto Tecnologico e Nuclear, E.N. 10, P-2686-953 Sacavem (Portugal); Dimitrova, K. [Executive Environment Agency of Bulgaria, Regional Laboratory Varna, 4 Jan Palah Str., Varna 9000 (Bulgaria); Edrev, Z.H. [Regional Inspectorate of Environment and Waters, 2 Stara Planina str., 6000 Stara Zagora (Bulgaria); Engeler, C. [Radiochemistry Dept., Institute for Inland Water Management and Waste Water Treatment, P.O. Box 17, 8200 AA Lelystad (Netherlands); Fouche, F.J. [South African Nuclear Energy Corporation NECSA Ltd., P.O. Box 582, Pretoria 0001 (South Africa); Garcia-Orellana, J. [Dept. de Fisica, Universitat Automona de Barcelona, 08193-Cerdanyola del Valles (Spain); Gasco, C. [Instituto de Medio Ambiente, Radioecologia del Medio Acuatico, Av. de la Complutense 22, 28040 Madrid (Spain); Gastaud, J. [Marine Environment Labs., International Atomic Energy Agency, MC 98000 Principality of Monaco (Monaco); Gudelis, A. [Institute of Physics, Nuclear and Environmental Radioactivity Research Lab., Savanoriu Ave 231, 2053 Vilnius (Lithuania); Hancock, G. [CSIRO Land and Water, Clunies Ross St., GPO Box 1666, Canberra, ACT 2601 (Australia)] (and others)

    2008-11-15

    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 ({sup 40}K, {sup 137}Cs, {sup 226}Ra, {sup 228}Ra, {sup 230}Th, {sup 232}Th, {sup 234}U, {sup 238}U, {sup 238}Pu, {sup 239+240}Pu and {sup 241}Am) have been certified and information mass activities with 95% confidence intervals are given for seven other radionuclides ({sup 90}Sr, {sup 210}Pb({sup 210}Po), {sup 235}U, {sup 239}Pu, {sup 240}Pu and {sup 241}Pu). Results for less frequently reported radionuclides ({sup 60}Co, {sup 99}Tc, {sup 134}Cs, {sup 155}Eu, {sup 224}Ra and {sup 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.

  2. Northern Marshall Islands radiological survey: sampling and analysis summary

    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.

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

    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

  4. Stable isotope studies

    Ishida, T.

    1992-01-01

    The research has been in four general areas: (1) correlation of isotope effects with molecular forces and molecular structures, (2) correlation of zero-point energy and its isotope effects with molecular structure and molecular forces, (3) vapor pressure isotope effects, and (4) fractionation of stable isotopes. 73 refs, 38 figs, 29 tabs.

  5. Effect of precipitation, sorption and stable of isotope on maximum release rates of radionuclides from engineered barrier system (EBS) in deep repository.

    Malekifarsani, A; Skachek, M A

    2009-10-01

    shown that the concentrations of the following radionuclides are limited by solubility and precipitate around the waste and buffer: U, Np, Ra, Sm, Zr, Se, Tc, and Pd. The Sensitivity of maximum release rates in case precipitation shows that some nuclides such as Cs-135, Nb-94, Nb-93 m, Zr-93, Sn-126, Th-230, Pu-240, Pu-242, Pu-239, Cm-245, Am-243, Cm-245, U-233, Ac-227, Pb-210, Pa-231 and Th-229 are very little changed in case the maximum release rate from EBS corresponding to eliminate precipitation in buffer material. Some nuclides such as Se-79, Tc-99, Pd-107, Th-232, U-236, U-233, Ra-226, Np-237 U-235, U-234, and U-238 are virtually changed in the maximum release rate compared to case that taking account precipitation. In Sensitivity of maximum release rates in case to taking account stable isotopes (according to the table of inventory) there are only some nuclides with their stable isotopes in the vitrified waste. And calculation shows that Pd-107 and Se-79 are very increase in case eliminate stable isotope. The Sensitivity of maximum release rates in case retardation with sorption shows that some nuclides such as Pu-240, Pu-241, Pu-239, Cm-245, Am-241, Cm-246, and Am-243 are increased in some time in case maximum release rate from EBS corresponding to eliminate retardation in buffer material. Some nuclides such as U-235, U-233 and U-236 have a little decrease in case maximum release because their parents have short live and before decay to their daughter will released from the EBS. If the characteristic time taken for a nuclide to diffuse across the buffer exceeds its half-life, then the release rate of that nuclide from the EBS will be attenuated by radioactive decay. Thus, the retardation of the diffusion process due to sorption tends to reduce the release rates of short-lived nuclides more effectively than for the long-lived ones. For example, release rates of Pu-240, Cm-246 and Am-241, which are relatively short-lived and strongly sorbing, are very small

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

    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.

  7. The effect of permafrost on soil erosion using meteoric 10Be, 137Cs and 239+240Pu in the Eastern Swiss Alps

    Pichler, Barbara; Brandovà, Dagmar; Alewell, Christine; Ivy-Ochs, Susan; Kubik, Peter W.; Kneisel, Christof; Meusburger, Katrin; Ketterer, Michael; Egli, Markus

    2013-04-01

    Permafrost ecosystems are highly sensitive to climate warming. The expected changes in the thermal and hydrological soil regime might have crucial consequences on soil erosion processes. Therefore, the determination of erosional activities on the long- (since the beginning of soil formation) and mid-term (last 50-60 yr) using cosmogenic and anthropogenic radionuclides can provide important information on past and ongoing processes. Permafrost soils in the Alps and their behaviour with climate change are only rarely studied. The expected new insights will lead to a better understanding of the processes of high mountain soils and are a further step towards improving climate-related modelling of fast warming scenarios and increasing system disequilibria. Our aim is to quantify soil erosion processes in permafrost soils and nearby unfrozen soils in the Alpine (sites at 2700 m asl) and the sub-Alpine (sites 1800 m asl) range of the Swiss Alps (Upper Engadine). We hypothesise that permafrost soils differ distinctly in their long- and mid-term soil erosion rates due to different water retention capacities. Long-term soil erosion was assessed using meteoric 10Be. Meteoric 10Be in a soil profile was estimated assuming that it is has been deposited as a function of precipitation and adsorbed in the fine earth fraction (

  8. Statistical clumped isotope signatures

    Röckmann, T.; Popa, M. E.; Krol, M. C.; Hofmann, M. E. G.

    2016-01-01

    High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of a m

  9. Plutonium and americium in arctic waters, the North Sea and Scottish and Irish coastal zones

    Hallstadius, L.; Aarkrog, Asker; Dahlgaard, Henning;

    1986-01-01

    collected from the Irish coast in 1983. Fallout is found to dominate as a source of 239+240Pu north of latitude 65°N, while for 238Pu a substantial fraction originates from European nuclear fuel reprocessing facilities. The 238Pu/239+240Pu isotope ratio provides clear evidence of the transport of effluent...... of the Irish Sea) to Spitsbergen. 241Am found in Arctic waters probably originates from the decay of fallout 241Pu and, like Pu, tentatively has a residence time of the order of several years. Americium from Sellafield has an estimated mean residence time of 4–6 months in Scottish waters....

  10. Isotopes in heterogeneous catalysis

    Hargreaves, Justin SJ

    2006-01-01

    The purpose of this book is to review the current, state-of-the-art application of isotopic methods to the field of heterogeneous catalysis. Isotopic studies are arguably the ultimate technique in in situ methods for heterogeneous catalysis. In this review volume, chapters have been contributed by experts in the field and the coverage includes both the application of specific isotopes - Deuterium, Tritium, Carbon-14, Sulfur-35 and Oxygen-18 - as well as isotopic techniques - determination of surface mobility, steady state transient isotope kinetic analysis, and positron emission profiling.

  11. Generation of Radixenon Isotopes

    McIntyre, Justin I.; Bowyer, Ted W.; Hayes, James C.; Heimbigner, Tom R.; Morris, Scott J.; Panisko, Mark E.; Pitts, W. K.; Pratt, Sharon L.; Reeder, Paul L.; Thomas, Charles W.

    2003-06-30

    Pacific Northwest National Laboratory has developed an automated system for separating Xe from air and can detect the following radioxenon isotopes, 131mXe, 133mXe, 133Xe, and 135Xe. This report details the techniques used to generate the various radioxenon isotopes that are used for the calibration of the detector as well as other isotopes that have the potential to interfere with the fission produced radioxenon isotopes. Fission production is covered first using highly enriched uranium followed by a description and results from an experiment to produce radioxenon isotopes from neutron activation of ambient xenon.

  12. Contribution to the micro-calorimetric study of the characteristics of radio-elements and to their qualitative and quantitative analysis; Contribution a l'etude microcalorimetrique des caracteristiques des radio-elements et a leurs analyses qualitative et quantitative

    Ozias, Y. [Centre de Production de Plutonium de Marcoule, 30 (France)

    1964-10-01

    The principle of this study consists in using the E. CALVET microcalorimeter for recording the energy flux emitted by radio-elements as a function of time, and in determining from this curve either their characteristics (half-life and radiation energy), or the composition of a mixture of radio-elements. In the first part the theoretical relationships describing radioactivity have been adapted to the microcalorimetric study. In the second part an experimental determination has been made using the E. CALVET microcalorimeter of the characteristics of various radio-elements, yttrium 90, phosphorus 32, sulphur 35, iodine 131, etc and of their mixtures. In particular a study has been made of the isotopic analysis of a {sup 239}Pu - {sup 240}Pu mixture, sometimes in the presence of {sup 241}Pu. The microcalorimetric method is not as sensitive as conventional counting methods, its limit appears to be at the present about 1 micro-watt for the apparatus used, it is however the most direct method in the case of emitters of weakly absorbed radiation ({alpha} and {beta}). For the {gamma} emitters only a part of the energy is absorbed by the walls of the container. The determination of their characteristics and of their masses in the mixtures depends neither on the shape, on the dilution or even less on the auto-absorption of the source. For high activity samples this auto-absorption is the cause of great difficulties in conventional methods which complicate the operations: divisions, dissolutions, dilutions, all of which are liable to introduce errors. The calorimetric method makes it possible to work on the untreated sample. All these measurements have been carried out using the conventional E CALVET calorimeter; to carry out an exact measurement of the energy due to {gamma} radiation, however, it is necessary to build special apparatus with a lead block the size of which is given by the author's calculations. The calorimetric method makes it possible to attain an

  13. Analytical Results of Radionuclide Immission Measurements for Radioactive Waste Storage Facility ZWILAG 1997-2001: Final Report; Spezialnuklid-Analysen fuer die Beweissicherung ZWILAG 1997-2001: Abschlussbericht der Immissionsmessungen

    Eikenberg, J.; Bajo, S.; Hitz, J.; Beer, H.; Gann, C.; Ruethi, M.; Wyer, L.; Ziegler, J

    2002-07-01

    This report summarizes the analytical results of radionuclide immission measurements performed in the frame of the project 'Beweissicherung' ZWlLAG AG, period 1997- 2001. Focus of the project 'Beweissicherung' was a detailed monitoring program for determining the activity concentrations of natural terrestrial ({sup 40}K, {sup 238}U, {sup 232}Th including progenies), cosmogenic ({sup 7}Be, {sup 14}C) and, particularly, anthropogenic radio-isotopes ({sup 63}Ni, {sup 90}Sr + {sup 90}Y, {sup 137}Cs, {sup 239}Pu, {sup 241}Am, {sup 244}Cm) in soil samples prior to storage of nuclear components into the ZWlLAG facility. As discussed in detail, most of the anthropogenic radioisotopes analysed here were deposited via aerosol-fallout caused by the Chernobyl reactor accident in the year 1986 as weIl as by subsurface atomic weapon tests that were carried out predominantly in the early 60ies of the last century. The relative contributions of both anthropogenic sources could be roughly estimated by use of isotope ratios between all anthropogenic isotopes. While the major fraction of {sup 137}Cs ( ca. 85%) can be attributed to the Chernobyl event, more than 95% of the anthropogenic {alpha}-emitting actinides were derived from the atmospheric nuclear weapon experiments. The measured activity concentrations and isotope ratios found here are consistent with results obtained from other soil samples collected from reference locations in Northern Switzerland and surrounding areas. The following typical values (in Bq/kg) were obtained for the top-soil layer (0-5 cm): {sup 90}Sr: 2-5, {sup 137}Cs: 50 - 100, {sup 239+240}Pu: 0.3 - 0.6, {sup 238}Pu: 0.01 - 0.02, {sup 241}Am: 0.1 - 0.3 and {sup 244}Cm < 0.01 (at reference date, i.e. October, 6, 1997, date of initial sampling). In addition, also the contents of the natural, primordially generated radio-isotopes (U-, Th-series, {sup 40}K) are typical for soils from North Alpine regions. The measurements yielded activities

  14. Downward migration of Chernobyl-derived radionuclides in soils in Poland and Sweden

    Matisoff, Gerald, E-mail: gerald.matisoff@case.edu [Case Western Reserve University, Cleveland, OH 44106-7216 (United States); Ketterer, Michael E. [Northern Arizona University, Flagstaff, AZ 86011-5698 (United States); Rosen, Klas [Swedish University of Agricultural Sciences, Uppsala (Sweden); Mietelski, Jerzy W. [Henryk Niewodniczanski Institute of Nuclear Physics, Krakow (Poland); Vitko, Lauren F. [Case Western Reserve University, Cleveland, OH 44106-7216 (United States); Persson, Henning [Swedish University of Agricultural Sciences, Uppsala (Sweden); Lokas, Edyta [Henryk Niewodniczanski Institute of Nuclear Physics, Krakow (Poland)

    2011-01-15

    Research highlights: {yields} {sup 137}Cs and {sup 239,240}Pu move down into the soil profile. {yields} {sup 137}Cs is from Chernobyl fallout; {sup 239,240}Pu is from stratospheric fallout from the 1960s. {yields} Solute transport and bioturbation models describe some but not all of the radionuclide profiles. - Abstract: Vertical profiles of {sup 137}Cs and {sup 239,240}Pu were measured in soils collected from two sites in southern Sweden and three sites in southern Poland and were modeled using both a solute transport model and a bioturbation model to better understand their downward migration. A time series of measured {sup 137}Cs profiles indicates that {sup 137}Cs from Chernobyl was found at the soil surface in 1986 but it has migrated progressively downward into the soil 4.5-25.5 cm since. However, because of dispersion during the migration and mixing following Chernobyl deposition and the much higher activities of {sup 137}Cs from Chernobyl, stratospheric fallout of {sup 137}Cs from the 1960s cannot be identified as a second {sup 137}Cs activity maximum lower in the soil column at any of the sites. Conversely, the {sup 240}Pu/{sup 239}Pu ratio indicates that no Chernobyl-derived Pu is present in any of the cores with the exception of one sample in Sweden. This difference may be attributed to the nature of the release from Chernobyl. Cesium volatilized at the reactor temperature during the accident, and was released as a vapor whereas Pu was not volatile and was only released in the form of minute fuel particles that traveled regionally. Both the solute diffusion and the bioturbation models accurately simulate the downward migration of the radionuclides at some sites but poorly describe the distributions at other sites. The distribution coefficients required by the solute transport model are about 100 times lower than reported values from the literature indicating that even though the solute transport model can simulate the profile shapes, transport as a

  15. Discovery of the Cobalt Isotopes

    Szymanski, T.; Thoennessen, M.

    2009-01-01

    Twenty-six cobalt isotopes have so far been observed; the discovery of these isotopes is discussed. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  16. Discovery of the Arsenic Isotopes

    Shore, A; Heim, M; Schuh, A; Thoennessen, M

    2009-01-01

    Twenty-nine arsenic isotopes have so far been observed; the discovery of these isotopes is discussed. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  17. Intracellular Cadmium Isotope Fractionation

    Horner, T. J.; Lee, R. B.; Henderson, G. M.; Rickaby, R. E.

    2011-12-01

    Recent stable isotope studies into the biological utilization of transition metals (e.g. Cu, Fe, Zn, Cd) suggest several stepwise cellular processes can fractionate isotopes in both culture and nature. However, the determination of fractionation factors is often unsatisfactory, as significant variability can exist - even between different organisms with the same cellular functions. Thus, it has not been possible to adequately understand the source and mechanisms of metal isotopic fractionation. In order to address this problem, we investigated the biological fractionation of Cd isotopes within genetically-modified bacteria (E. coli). There is currently only one known biological use or requirement of Cd, a Cd/Zn carbonic anhydrase (CdCA, from the marine diatom T. weissfloggii), which we introduce into the E. coli genome. We have also developed a cleaning procedure that allows for the treating of bacteria so as to study the isotopic composition of different cellular components. We find that whole cells always exhibit a preference for uptake of the lighter isotopes of Cd. Notably, whole cells appear to have a similar Cd isotopic composition regardless of the expression of CdCA within the E. coli. However, isotopic fractionation can occur within the genetically modified E. coli during Cd use, such that Cd bound in CdCA can display a distinct isotopic composition compared to the cell as a whole. Thus, the externally observed fractionation is independent of the internal uses of Cd, with the largest Cd isotope fractionation occurring during cross-membrane transport. A general implication of these experiments is that trace metal isotopic fractionation most likely reflects metal transport into biological cells (either actively or passively), rather than relating to expression of specific physiological function and genetic expression of different metalloenzymes.

  18. Chromium isotope variations

    D'Arcy, Joan Mary

    is incorporated into carbonates. Hence, ancient carbonates can potentially record the Cr isotopic composition (δ53Cr ‰) of seawater in the geological past. Reliable application and interpretation of this proxy requires a detailed knowledge about processes that fractionate Cr on the Earth’s surface...... deposited during the Early Ordovician — a time of known redox instability in ancient oceans – exhibit a significant positive Cr isotope excursion of +0.5‰. This excursion is interpreted as the reductive drawn down of dissolved Cr in seawater in response to the development of a proximal anoxic sink......, and the quantification the Cr isotope composition of major Cr fluxes into and out of ocean. This thesis adds to the current knowledge of the Cr isotope system and is divided into two studies. The focus of the first study was to determine what processes control the Cr isotopic compositionof river water and to quantify...

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

    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

  20. Perchlorate isotope forensics

    Böhlke, J.K.; Sturchio, N.C.; Gu, B.; Horita, J.; Brown, G.M.; Jackson, W.A.; Batista, J.; Hatzinger, P.B.

    2005-01-01

    Perchlorate has been detected recently in a variety of soils, waters, plants, and food products at levels that may be detrimental to human health. These discoveries have generated considerable interest in perchlorate source identification. In this study, comprehensive stable isotope analyses ( 37Cl/35Cl and 18O/17O/ 16O) of perchlorate from known synthetic and natural sources reveal systematic differences in isotopic characteristics that are related to the formation mechanisms. In addition, isotopic analyses of perchlorate extracted from groundwater and surface water demonstrate the feasibility of identifying perchlorate sources in contaminated environments on the basis of this technique. Both natural and synthetic sources of perchlorate have been identified in water samples from some perchlorate occurrences in the United States by the isotopic method. ?? 2005 American Chemical Society.

  1. Isotope Production Facility (IPF)

    Federal Laboratory Consortium — The Los Alamos National Laboratory has produced radioactive isotopes for medicine and research since the mid 1970s, when targets were first irradiated using the 800...

  2. Calcium stable isotope geochemistry

    Gausonne, Nikolaus [Muenster Univ. (Germany). Inst. fuer Mineralogie; Schmitt, Anne-Desiree [Strasbourg Univ. (France). LHyGeS/EOST; Heuser, Alexander [Bonn Univ. (Germany). Steinmann-Inst. fuer Geologie, Mineralogie und Palaeontologie; Wombacher, Frank [Koeln Univ. (Germany). Inst. fuer Geologie und Mineralogie; Dietzel, Martin [Technische Univ. Graz (Austria). Inst. fuer Angewandte Geowissenschaften; Tipper, Edward [Cambridge Univ. (United Kingdom). Dept. of Earth Sciences; Schiller, Martin [Copenhagen Univ. (Denmark). Natural History Museum of Denmark

    2016-08-01

    This book provides an overview of the fundamentals and reference values for Ca stable isotope research, as well as current analytical methodologies including detailed instructions for sample preparation and isotope analysis. As such, it introduces readers to the different fields of application, including low-temperature mineral precipitation and biomineralisation, Earth surface processes and global cycling, high-temperature processes and cosmochemistry, and lastly human studies and biomedical applications. The current state of the art in these major areas is discussed, and open questions and possible future directions are identified. In terms of its depth and coverage, the current work extends and complements the previous reviews of Ca stable isotope geochemistry, addressing the needs of graduate students and advanced researchers who want to familiarize themselves with Ca stable isotope research.

  3. Isotopes in Greenland Precipitation

    Faber, Anne-Katrine

    the Arctic Ocean. A comprehensive database is created based on ice core and weather station data from Greenland within the period 1890-2014. Present day annual and seasonal mean values are computed for 326 locations in Greenland. Parameterization of the spatial distribution of temperature and δ18O are used...... of model and data can be used to improve the understanding of climate changes. This is done through analysis of isotope modelling, observations and ice core measurements. This dissertation comprises three projects: (1) Modelling the isotopic response to changes in Arctic sea surface conditions, (2......) Constructing a new Greenland database of observations and present-day ice core measurements, and (3) Performance test of isotope-enabled CAM5 for Greenland. The recent decades of rapid Arctic sea ice decline are used as a basis for an observational-based model experiment using the isotope-enabled CAM model 3...

  4. Isotopically controlled semiconductors

    Haller, E.E.

    2004-11-15

    A review of recent research involving isotopically controlled semiconductors is presented. Studies with isotopically enriched semiconductor structures experienced a dramatic expansion at the end of the Cold War when significant quantities of enriched isotopes of elements forming semiconductors became available for worldwide collaborations. Isotopes of an element differ in nuclear mass, may have different nuclear spins and undergo different nuclear reactions. Among the latter, the capture of thermal neutrons which can lead to neutron transmutation doping, can be considered the most important one for semiconductors. Experimental and theoretical research exploiting the differences in all the properties has been conducted and will be illustrated with selected examples. Manuel Cardona, the longtime editor-in-chief of Solid State Communications has been and continues to be one of the major contributors to this field of solid state physics and it is a great pleasure to dedicate this review to him.

  5. Isotopes through the looking glass

    Mårtensson Pendrill, Ann Marie

    2000-08-01

    Nuclear distributions affect many aspects of atomic spectra. As an example, recent experimental results for the hyperfine anomaly in Fr isotopes are considered. These depend on nuclear charge and magnetization distributions. The variations in charge radii for these isotopes were studied earlier by measuring optical isotope shifts. The hyperfine anomalies for the odd-odd isotopes involve the neutron distributions, of interest for studies of parity nonconserving effects along a chain of isotopes.

  6. Methods of isotopic geochronology

    Gorokhov, I. M.; Levchenkov, O. A.

    Papers are presented on such topics as the age of the chemical elements; the age of meteorites, the moon, and the earth; isotopic ages of the most ancient terrestrial formations; and the Archean evolution of Enderby Land in the Antarctic as evidenced by isotopic dating. Consideration is also given to a uranium-lead geochronology technique for investigating Precambrian ore deposits, a Pb-Pb technique of zircon dating, and the potentials and limitations of Sm-Nd geochronology.

  7. Oxygen Isotopes in Meteorites

    Clayton, R. N.

    2003-12-01

    Oxygen isotope abundance variations in meteorites are very useful in elucidating chemical and physical processes that occurred during the formation of the solar system (Clayton, 1993). On Earth, the mean abundances of the three stable isotopes are 16O: 99.76%, 17O: 0.039%, and 18O: 0.202%. It is conventional to express variations in abundances of the isotopes in terms of isotopic ratios, relative to an arbitrary standard, called SMOW (for standard mean ocean water), as follows:The isotopic composition of any sample can then be represented by one point on a "three-isotope plot," a graph of δ17O versus δ18O. It will be seen that such plots are invaluable in interpreting meteoritic data. Figure 1 shows schematically the effect of various processes on an initial composition at the center of the diagram. Almost all terrestrial materials lie along a "fractionation" trend; most meteoritic materials lie near a line of "16O addition" (or subtraction). (4K)Figure 1. Schematic representation of various isotopic processes shown on an oxygen three-isotope plot. Almost all terrestrial materials plot along a line of "fractionation"; most primitive meteoritic materials plot near a line of "16O addition." The three isotopes of oxygen are produced by nucleosynthesis in stars, but by different nuclear processes in different stellar environments. The principal isotope, 16O, is a primary isotope (capable of being produced from hydrogen and helium alone), formed in massive stars (>10 solar masses), and ejected by supernova explosions. The two rare isotopes are secondary nuclei (produced in stars from nuclei formed in an earlier generation of stars), with 17O coming primarily from low- and intermediate-mass stars (shielding in the UV photodissociation of CO (van Dishoeck and Black, 1988). This process results from the large differences in abundance between C16O, on the one hand, and C17O and C18O on the other. Photolysis of CO occurs by absorption of stellar UV radiation in the

  8. Risk assessment of soil-based exposures to plutonium at experimental sites located on the Nevada Test Site and adjoining areas

    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.

  9. Calculation Analysis of San Onofre Depletion MOX Fuel Experiment

    Pavlovichev, AM

    2001-08-31

    The report provides calculation results of isotopic composition of spent MOX fuel irradiated in Sun Onofre PWR reactor. The calculation was performed by means of the MCU/BURNUP Monte Carlo code. The code is developed in Kurchatov Institute, Russia. The predicted isotope contents are compared with the measured ones. A purpose of this work is a verification both the code and the model of experiment description. Predicted plutonium content exceeds the measured one approximately by 3%. It is arise mainly from error of {sup 239}Pu isotope. Isotopic contents of the main plutonium and uranium isotopes are predicted with satisfactory precision.

  10. Beta and gamma decay heat measurements between 0.1s-50,000s for neutron fission of {sup 235}U, {sup 238}U and {sup 239}Pu. Progress report, March 1, 1993--January 31, 1994

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

    1994-06-01

    Decay heat measurements following the fast fission of {sup 238}U are well underway. The He-jet system and spectrometers were moved to the 1 MW research reactor to gain sufficient fast neutron flux for these measurements. On the Van de Graaff accelerator, the He-jet capillary has been shortened so that beta and gamma measurements following the thermal neutron fission of {sup 235}U could be made down to delay times near 0.1 s. Gamma-ray response functions are now well characterized for gamma energies up to 1.5 MeV for our large Nal spectrometer. Such response functions out to high energies are needed to extract energy distributions of our measured gamma spectra. The response function unfolding program, FERD-PC, has been operated successfully with trial spectra. Comparisons of individual fission products for {sup 235}U(n{sub th}f) with ENDF/B-VI at short delay times suggest several improvements to the data base particularly in production probabilities. The new data acquisition and data analysis systems have arrived and will soon be brought on line extending considerably the capabilities of our research group.

  11. Isotope geochemistry. Biological signatures in clumped isotopes of O₂.

    Yeung, Laurence Y; Ash, Jeanine L; Young, Edward D

    2015-04-24

    The abundances of molecules containing more than one rare isotope have been applied broadly to determine formation temperatures of natural materials. These applications of "clumped" isotopes rely on the assumption that isotope-exchange equilibrium is reached, or at least approached, during the formation of those materials. In a closed-system terrarium experiment, we demonstrate that biological oxygen (O2) cycling drives the clumped-isotope composition of O2 away from isotopic equilibrium. Our model of the system suggests that unique biological signatures are present in clumped isotopes of O2—and not formation temperatures. Photosynthetic O2 is depleted in (18)O(18)O and (17)O(18)O relative to a stochastic distribution of isotopes, unlike at equilibrium, where heavy-isotope pairs are enriched. Similar signatures may be widespread in nature, offering new tracers of biological and geochemical cycling.

  12. Stable isotopes. Applications and production; Les isotopes stables. Applications - production

    Goldstein, S.; Louvet, P.; Soulie, E. [eds.

    1994-12-31

    This conference presents 46 communications concerning stable isotope production, utilization and application, grouped in 6 sessions and posters. The various themes are: biological applications (pharmacology, medical diagnosis, metabolism and protein studies, toxicity and response studies, labelled compounds), analysis procedures (NMR analysis for macromolecules, tracer studies), nuclear applications (utilization of stable isotopes in nuclear reactors), biological, physical and chemical applications (mass transfer, mobility, crystallography, isotopic exchange), stable isotope production (ion chromatography, ion cyclotron resonance, cryogenic distillation).

  13. Deformation of C isotopes

    Kanada-Enyo, Y

    2004-01-01

    Systematic analysis of the deformations of proton and neutron densities in even-even C isotopes was done based on the method of antisymmetrized molecular dynamics. The $E2$ transition strength was discussed in relation to the deformation. We analyze the $B(E2;2^+_1\\to 0^+_1)$ in $^{16}$C, which has been recently measured to be abnormally small. The results suggest the difference of the deformations between proton and neutron densities in the neutron-rich C isotopes. It was found that stable proton structure in C isotopes plays an important role in the enhancement the neutron skin structure as well as in the systematics of $B(E2)$ in the neutron-rich C.

  14. Isotopes in Condensed Matter

    G Plekhanov, Vladimir

    2013-01-01

    This book provides a concise introduction to the newly created sub-discipline of solid state physics isotopetronics. The role of isotopes in materials and their properties are describe  in this book. The problem of the enigma of the atomic mass in microphysics is briefly discussed.  The range of the applications of isotopes is wide: from biochemical process in living organisms to modern technical applications in quantum information. Isotopetronics promises to improve nanoelectronic and optoelectronic devices. With numerous illustrations this book is useful to researchers, engineers and graduate students.

  15. Artificial radionuclides in a high resolution water column profile from the Catalan Sea (the Northwestern Mediterranean)

    Merino, J.; Sanchez-Cabeza, J.A.; Bruach, J.M.; Masque, P.; Pujol, Ll. [Universitat Autonoma de Barcelona, Bellatera (Spain). Grup de Fisica de les Radiacions

    1997-12-31

    {sup 137}Cs, {sup 239,240}Pu and {sup 90}Sr concentration profiles (0-1200 m) were determined in filtered large volume water samples collected from the Catalan Sea (the Northwestern Mediterranean) in August 1993. Plutonium isotopes were also measured in the suspended matter. {sup 137}Cs concentrations showed a maximum surface activity of 4.45 {+-} 0.38 Bq m{sup -3} and decreased along the water column to a minimum value. The total {sup 137}Cs inventory in the water column was 3.30 {+-} 0.13 kBq m{sup -2}. {sup 90}Sr concentration profile showed a similar behaviour, but levels rose slightly near the bottom. On the other hand, soluble {sup 239,240}Pu concentrations showed a broad subsurface maximum centered at about 400 m depth, where its maximum value was found. This observation is in agreement with that found by others in open ocean waters of the Atlantic and Pacific Oceans, as well as in the Mediterranean Sea. The soluble {sup 239,240}Pu inventory was 17.4 {+-} 0.5 Bq m{sup -2}. In comparison with the inventories reported earlier, the vertical flux of plutonium was determined to be 1.97 {+-} 0.14 Bq m{sup -2} y{sup -1}, roughly 10% of the annual standing inventory. This indicated that {sup 239,240}Pu may be used to trace particulate vertical transport processes in open sea waters. (author) 21 refs.

  16. Discoveries of isotopes by fission

    M Thoennessen

    2015-09-01

    Of the about 3000 isotopes presently known, about 20% have been discovered in fission. The history of fission as it relates to the discovery of isotopes as well as the various reaction mechanisms leading to isotope discoveries involving fission are presented.

  17. A sensitivity study on DUPIC fuel composition

    Choi, Hang Bok; Roh, Gyu Hong

    1997-01-01

    In DUPIC fuel cycle, the spent pressurized water reactor (PWR) fuel is refabricated as a DUPIC fuel by a dry process. Because the spent PWR fuel composition depends on the initial enrichment and burnup condition of PWR fuel, the composition of a DUPIC fuel is not uniquely defined. Therefore, for the purpose of reducing the effects of such a composition heterogeneity on core performance, a composition adjustment of DUPIC fuel was studies. The composition adjustment was made in two steps: mixing two spent PWR fuel assemblies of higher and lower {sup 239}Pu contents and blending in fresh uranium with the mixed spent PWR fuels. Because the fuel and core performances depend on both the absolute amount of fissile isotopes and the ratio of major fissile isotope contents, a parametric study was performed to determine the reference compositions of {sup 235}U and {sup 239}Pu. The reference enrichments of {sup 235}U and {sup 239}Pu were determined such that the DUPIC core performance is comparable to that of a natural uranium core with high spent PWR fuel utilization and low fuel cycle cost. Under this condition, it is possible to utilize 90% of spent PWR fuels as the DUPIC fuel formula. On average, the amounts of slightly enriched and depleted uranium used for blending correspond to 8.6% and 10.6%, respectively, of the mass of candidate spent PWR fuels. (author). 16 refs., 30 tabs., 9 figs.

  18. 238Pu: accumulation, tissue distribution, and excretion in Mayak workers after exposure to plutonium aerosols.

    Suslova, Klara G; Sokolova, Alexandra B; Khokhryakov, Viktor V; Miller, Scott C

    2012-03-01

    The alpha spectrometry measurements of specific activity of 238Pu and 239Pu in urine from bioassay examinations of 1,013 workers employed at the radiochemical and plutonium production facilities of the Mayak Production Association and in autopsy specimens of lung, liver, and skeleton from 85 former nuclear workers who died between 1974-2009, are summarized.The accumulation fraction of 238Pu in the body and excreta has not changed with time in workers involved in production of weapons-grade plutonium production (e.g., the plutonium production facility and the former radiochemical facility). The accumulation fraction of 238Pu in individuals exposed to plutonium isotopes at the newer Spent Nuclear Fuel Reprocessing Plant ranged from 0.13% up to 27.5% based on the autopsy data. No statistically significant differences between 238Pu and 239Pu in distribution by the main organs of plutonium deposition were found in the Mayak workers. Based on the bioassay data,the fraction of 238Pu activity in urine is on average 38-69% of the total activity of 238Pu and 239Pu, which correlates with the isotopic composition in workplace air sampled at the Spent Nuclear Fuel Reprocessing Plant. In view of the higher specific activity of 238Pu, the contribution of 238Pu to the total internal dose, particularly in the skeleton and liver, might be expected to continue to increase, and continued surveillance is recommended.

  19. Isotopic Implicit Surface Meshing

    Boissonnat, Jean-Daniel; Cohen-Steiner, David; Vegter, Gert

    2004-01-01

    This paper addresses the problem of piecewise linear approximation of implicit surfaces. We first give a criterion ensuring that the zero-set of a smooth function and the one of a piecewise linear approximation of it are isotopic. Then, we deduce from this criterion an implicit surface meshing algor

  20. Forensic Stable Isotope Biogeochemistry

    Cerling, Thure E.; Barnette, Janet E.; Bowen, Gabriel J.; Chesson, Lesley A.; Ehleringer, James R.; Remien, Christopher H.; Shea, Patrick; Tipple, Brett J.; West, Jason B.

    2016-06-01

    Stable isotopes are being used for forensic science studies, with applications to both natural and manufactured products. In this review we discuss how scientific evidence can be used in the legal context and where the scientific progress of hypothesis revisions can be in tension with the legal expectations of widely used methods for measurements. Although this review is written in the context of US law, many of the considerations of scientific reproducibility and acceptance of relevant scientific data span other legal systems that might apply different legal principles and therefore reach different conclusions. Stable isotopes are used in legal situations for comparing samples for authenticity or evidentiary considerations, in understanding trade patterns of illegal materials, and in understanding the origins of unknown decedents. Isotope evidence is particularly useful when considered in the broad framework of physiochemical processes and in recognizing regional to global patterns found in many materials, including foods and food products, drugs, and humans. Stable isotopes considered in the larger spatial context add an important dimension to forensic science.

  1. Isotope hydrograph separation

    Fritz, P. [UFZ-Umweltforschungszentrum, Centre of Environmental Research Leipzig-Halle, Leipzig (Germany)

    2000-07-01

    Storm-runoff thus reflects the complex hydraulic behaviour of drainage basins and water-links of such systems. Water of different origin may participate in the events and in this lecture, the application of isotope techniques to separate storm hydrographs into different components will be presented.

  2. GEOCHRONOMETRY & ISOTOPE GEOLOGY

    2007-01-01

    <正>20072750 Huang Sijing(State Key Laboratory of Oil/Gas Reservoir Geology and Exploitation,Chengdu University of Technology,Chengdu 610059,China);Pei Changrong Age Calibration for the Boundary between Lower and Middle Triassic by Strontium Isotope Stratigraphy in Eastern Sichuan Province

  3. GEOCHRONOMETRY ISOTOPE GEOLOGY

    2004-01-01

    <正>20040631 Chen Jiangfeng (School of Earth and Space Sciences, University of Science and Technology of China, Hefei, Anhui) ; Xie Zhi Relationships Between Rb-Sr, Ar - Ar Geochronometers and Oxygen Isotopic Equilibrium of Intrusions from Eastern Anhui Province, China (Geological Journal of China Universities, ISSN 1006 - 7493, CN 32 -

  4. GEOCHRONOMETRY & ISOTOPE GEOLOGY

    2009-01-01

    <正>20090432 Zhou Shuqing (School of Energy Resources, China University of Geosciences Beijing 100083, China); Huang Haiping Stable Isotopic Records vs. Important Events in Life Evolution and the Concurrent Environment (Geological Review, ISSN0371-5736, CN11-1952, 54(2), 2008, p.225-231, 3 illus., 1 table, 77 refs.)

  5. GEOCHRONOMETRY & ISOTOPE GEOLOGY

    2014-01-01

    <正>20141014Wang Hairan(State Key Laboratory of Continental Dynamics,Department of Geology,Northwest University,Xi’an710069,China);Zhao Hongge Theory and Application of Zircon U-Pb Isotope Dating Technique(Geology and Resources,ISSN1671-1947,CN21-1458/P,22(3),2013,p.229

  6. GEOCHRONOMETRY & ISOTOPE GEOLOGY

    2007-01-01

    <正>20070454 Bao Zengkuan (Institute of High Energy Physics, CAS, Beijing 100049, China); Yuan Wanming Apatite (U-Th)/He Dating and Its Application (Acta Petrologica et Mineralogica, ISSN1000-6524, CN11-1966/P, 24(2), 2005, p.126-132, 2 illus., 25 refs.) Key words: isotopic geochronology

  7. Using anisotropies in prompt fission neutron coincidences to assess the neutron multiplication of highly multiplying subcritical plutonium assemblies

    Mueller, J.M., E-mail: jonathan_mueller@ncsu.edu; Mattingly, J.

    2016-07-21

    There is a significant and well-known anisotropy between the prompt neutrons emitted from a single fission event; these neutrons are most likely to be observed at angles near 0° or 180° relative to each other. However, the propagation of this anisotropy through different generations of a fission chain reaction has not been previously studied. We have measured this anisotropy in neutron–neutron coincidences from a subcritical highly-multiplying assembly of plutonium metal. The assembly was a 4.5 kg α-phase plutonium metal sphere composed of 94% {sup 239}Pu and 6% {sup 240}Pu by mass. Data were collected using two EJ-309 liquid scintillators and two EJ-299 plastic scintillators. The angular distribution of neutron–neutron coincidences was measured at 90° and 180° and found to be largely isotropic. Simulations were performed using MCNPX-PoliMi of similar plutonium metal spheres of varying sizes and a correlation between the neutron multiplication of the assembly and the anisotropy of neutron–neutron coincidences was observed. In principle, this correlation could be used to assess the neutron multiplication of an unknown assembly.

  8. Progress on Nuclear Data Covariances: AFCI-1.2 Covariance Library

    Oblozinsky,P.; Oblozinsky,P.; Mattoon,C.M.; Herman,M.; Mughabghab,S.F.; Pigni,M.T.; Talou,P.; Hale,G.M.; Kahler,A.C.; Kawano,T.; Little,R.C.; Young,P.G

    2009-09-28

    Improved neutron cross section covariances were produced for 110 materials including 12 light nuclei (coolants and moderators), 78 structural materials and fission products, and 20 actinides. Improved covariances were organized into AFCI-1.2 covariance library in 33-energy groups, from 10{sup -5} eV to 19.6 MeV. BNL contributed improved covariance data for the following materials: {sup 23}Na and {sup 55}Mn where more detailed evaluation was done; improvements in major structural materials {sup 52}Cr, {sup 56}Fe and {sup 58}Ni; improved estimates for remaining structural materials and fission products; improved covariances for 14 minor actinides, and estimates of mubar covariances for {sup 23}Na and {sup 56}Fe. LANL contributed improved covariance data for {sup 235}U and {sup 239}Pu including prompt neutron fission spectra and completely new evaluation for {sup 240}Pu. New R-matrix evaluation for {sup 16}O including mubar covariances is under completion. BNL assembled the library and performed basic testing using improved procedures including inspection of uncertainty and correlation plots for each material. The AFCI-1.2 library was released to ANL and INL in August 2009.

  9. Mercuric iodide room-temperature array detectors for gamma-ray imaging

    Patt, B. [Xsirius, Inc, Camarillo, CA (United States)

    1994-11-15

    Significant progress has been made recently in the development of mercuric iodide detector arrays for gamma-ray imaging, making real the possibility of constructing high-performance small, light-weight, portable gamma-ray imaging systems. New techniques have been applied in detector fabrication and then low noise electronics which have produced pixel arrays with high-energy resolution, high spatial resolution, high gamma stopping efficiency. Measurements of the energy resolution capability have been made on a 19-element protypical array. Pixel energy resolutions of 2.98% fwhm and 3.88% fwhm were obtained at 59 keV (241-Am) and 140-keV (99m-Tc), respectively. The pixel spectra for a 14-element section of the data is shown together with the composition of the overlapped individual pixel spectra. These techniques are now being applied to fabricate much larger arrays with thousands of pixels. Extension of these principles to imaging scenarios involving gamma-ray energies up to several hundred keV is also possible. This would enable imaging of the 208 keV and 375-414 keV 239-Pu and 240-Pu structures, as well as the 186 keV line of 235-U.

  10. Resuspension and atmospheric transport of radionuclides due to wildfires near the Chernobyl Nuclear Power Plant in 2015: An impact assessment

    Evangeliou, N.; Zibtsev, S.; Myroniuk, V.; Zhurba, M.; Hamburger, T.; Stohl, A.; Balkanski, Y.; Paugam, R.; Mousseau, T. A.; Møller, A. P.; Kireev, S. I.

    2016-05-01

    In April and August 2015, two major fires in the Chernobyl Exclusion Zone (CEZ) caused concerns about the secondary radioactive contamination that might have spread over Europe. The present paper assessed, for the first time, the impact of these fires over Europe. About 10.9 TBq of 137Cs, 1.5 TBq of 90Sr, 7.8 GBq of 238Pu, 6.3 GBq of 239Pu, 9.4 GBq of 240Pu and 29.7 GBq of 241Am were released from both fire events corresponding to a serious event. The more labile elements escaped easier from the CEZ, whereas the larger refractory particles were removed more efficiently from the atmosphere mainly affecting the CEZ and its vicinity. During the spring 2015 fires, about 93% of the labile and 97% of the refractory particles ended in Eastern European countries. Similarly, during the summer 2015 fires, about 75% of the labile and 59% of the refractory radionuclides were exported from the CEZ with the majority depositing in Belarus and Russia. Effective doses were above 1 mSv y-1 in the CEZ, but much lower in the rest of Europe contributing an additional dose to the Eastern European population, which is far below a dose from a medical X-ray.

  11. Using anisotropies in prompt fission neutron coincidences to assess the neutron multiplication of highly multiplying subcritical plutonium assemblies

    Mueller, J. M.; Mattingly, J.

    2016-07-01

    There is a significant and well-known anisotropy between the prompt neutrons emitted from a single fission event; these neutrons are most likely to be observed at angles near 0° or 180° relative to each other. However, the propagation of this anisotropy through different generations of a fission chain reaction has not been previously studied. We have measured this anisotropy in neutron-neutron coincidences from a subcritical highly-multiplying assembly of plutonium metal. The assembly was a 4.5 kg α-phase plutonium metal sphere composed of 94% 239Pu and 6% 240Pu by mass. Data were collected using two EJ-309 liquid scintillators and two EJ-299 plastic scintillators. The angular distribution of neutron-neutron coincidences was measured at 90° and 180° and found to be largely isotropic. Simulations were performed using MCNPX-PoliMi of similar plutonium metal spheres of varying sizes and a correlation between the neutron multiplication of the assembly and the anisotropy of neutron-neutron coincidences was observed. In principle, this correlation could be used to assess the neutron multiplication of an unknown assembly.

  12. GEOCHRONOMETRY &ISOTOPE GEOLOGY

    2013-01-01

    <正>20131727 Huang Xiaowen(State Key Laboratory of Ore Deposit Geochemistry,Institute of Geochemistry,Chinese Academy of Sciences,Guiyang 550002,China);Qi Liang Preliminary Study on Sample-Preparation for Re-Os Isotopic Dating of Pyrite(Geochimica,ISSN0379-1726,CN44-1398/P,41(4),2012,p.380-386,3illus.,2tables,25refs)Key words:pyrite,Re-Os dating

  13. GEOCHRONOMETRY & ISOTOPE GEOLOGY

    2005-01-01

    <正>20050934 Chen Zhihong (Chinese Academy of Geological Sciences, Beijing 100037, China); Lu Songnian Age of the Fushui Intermediate-Mafic Intrusive Complex in the Qinling Orogen, New Zircon U - Pb and Whole -Rock Sm and Nd Isotope Chronological Evidence (Geological Bulletin of China, ISSN 1671-2552, CN11-4648/P, 23(4), 2004, p. 322-328, 3 illus. , 3 tables, 10 refs. )

  14. GEOCHRONOMETRY & ISOTOPE GEOLOGY

    2013-01-01

    <正>20132601 Cui Yurong(Tianjin Institute of Geology and Mineral Resources,China Geological Survey,Tianjin 300170,China);Zhou Hongying In Situ LA-MC-ICP-MS U-Pb Isotopic Dating of Monazite(Acta Geoscientica Sinica,ISSN0375-5444,CN11-1856/P,33(6),2012,p.865-876,6illus.,4tables,41refs.)Key words:monazite,U-Pb dating

  15. ISOTOPE METHODS IN HOMOGENEOUS CATALYSIS.

    BULLOCK,R.M.; BENDER,B.R.

    2000-12-01

    The use of isotope labels has had a fundamentally important role in the determination of mechanisms of homogeneously catalyzed reactions. Mechanistic data is valuable since it can assist in the design and rational improvement of homogeneous catalysts. There are several ways to use isotopes in mechanistic chemistry. Isotopes can be introduced into controlled experiments and followed where they go or don't go; in this way, Libby, Calvin, Taube and others used isotopes to elucidate mechanistic pathways for very different, yet important chemistries. Another important isotope method is the study of kinetic isotope effects (KIEs) and equilibrium isotope effect (EIEs). Here the mere observation of where a label winds up is no longer enough - what matters is how much slower (or faster) a labeled molecule reacts than the unlabeled material. The most careti studies essentially involve the measurement of isotope fractionation between a reference ground state and the transition state. Thus kinetic isotope effects provide unique data unavailable from other methods, since information about the transition state of a reaction is obtained. Because getting an experimental glimpse of transition states is really tantamount to understanding catalysis, kinetic isotope effects are very powerful.

  16. Nuclear physics and stable isotopes; Physique nucleaire et isotopes stables

    Goutte, D. [CEA Centre d`Etudes de Saclay, 91 - Gif-sur-Yvette (France). Dept. d`Astrophysique, de la Physique des Particules, de la Physique Nucleaire et de l`Instrumentation Associee

    1994-12-31

    The aim of this paper is to show that fundamental research in nuclear physics requires utilization of stable isotopes; stable isotopes are essential as target material since a large quantity of nucleus have to be studied in order to appreciate all the complexity of the nuclear structure, but also as a tool, such as beams, for the same purpose. Examples are given with samarium, tin and germanium isotopes. 7 figs.

  17. Nickel isotopes and methanogens

    Neubeck, A.; Ivarsson, M.

    2013-12-01

    Methanogens require Ni for their growth and as a consequence the microbial fractionation of Ni isotopes can be used as a biomarker for activity of methanogenic communities1. Anaerobic laboratory experiments was performed using methanogens to investigate methanogenic growth in a modified nutrient media2 with olivine Fo91 (5g/l) added as an additional mineral nutrient source and as the only H2 provider. One of the investigated methanogens showed an increased growth in the experiments with added olivine. There were also a close relationship between the mobilized Ni and the growth of the methanogen. Ni is an element that previously has been neglected in the study of fossilized microorganisms and their interaction with mineral substrates and, thus, there are no records or published data of Ni in association with microfossils. However, we have detected enrichments of Ni in fossilized microorganisms and ichno-fossils, respectively, from three separate locations. Ni is not present in the host rock in any of the samples. Thus, Ni is present in association with fossilized microorganisms from environments and more extensive analysis is required to understand the magnitude, uptake, preservation and fractionation of Ni in microfossils. In order to analyze Ni isotope fractionation from microbe-mineral interaction, we plan to use a high-resolution Laser-Ablation Time-of-Flight Mass Spectrometer (LMS)3. In situ profile ablation will provide detailed and localized data on fractionation patterns between microfossils and their host rock. Also, this technique will allow us to identify the change in Ni isotopic fractionation in rock samples caused by abiotic and biogenic processes in a faster and easier way and with less risk for contamination compared to the wet chemistry analyses of Ni isotopes. 1. Cameron, V., Vance, D., Archer, C. & House, C. H. A biomarker based on the stable isotopes of nickel. Proceedings of the National Academy of Sciences 106, 10944-10948 (2009). 2. Schn

  18. Therapeutic use of radioactive isotopes

    Caroline Duc

    2013-01-01

    In December, researchers from ISOLDE-CERN, the Paul Scherrer Institute (PSI) and the Institut Laue-Langevin (ILL) published the results of an in vivo study which successfully proved the effectiveness of four terbium isotopes for diagnosing and treating cancerous tumours.   Four terbium isotopes suitable for clinical purposes. “ISOLDE is the only installation capable of supplying terbium isotopes of such purity and intensity in the case of three out of the four types used in this study,” explains Karl Johnson, a physicist at ISOLDE.  “Producing over a thousand different isotopes, our equipment offers the widest choice of isotopes in the world!” Initially intended for fundamental physics research, ISOLDE has diversified its activities over time to invest in various projects in the materials science, biochemistry and nuclear medicine fields. The proof-of-concept study has confirmed that the four terbium isotopes 149Tb, 152Tb, 155Tb produ...

  19. Lithium isotope separation by laser

    Arisawa, T.; Maruyama, Y.; Suzuki, Y.; Shiba, K.

    1982-01-01

    A lithium isotope separation was performed using a laser isotope separation method. It was found that the lithium atoms with a natural isotopic abundance enhanced its /sup 6/Li concentration up to over 90% by tuning the laser wavelength to the /sup 2/Psub(1/2) of /sup 6/Li. Too high power, however, leads to a loss of enrichment due to the power broadening effect which was analysed by the equation of motion of density matrices.

  20. Fission waves can oscillate

    Osborne, Andrew G

    2016-01-01

    Under the right conditions, self sustaining fission waves can form in fertile nuclear materials. These waves result from the transport and absorption of neutrons and the resulting production of fissile isotopes. When these fission, additional neutrons are produced and the chain reaction propagates until it is poisoned by the buildup of fission products. It is typically assumed that fission waves are soliton-like and self stabilizing. However, we show that in uranium, coupling of the neutron field to the 239U->239Np->239Pu decay chain can lead to a Hopf bifurcation. The fission reaction then ramps up and down, along with the wave velocity. The critical driver for the instability is a delay, caused by the half-life of 239U, between the time evolution of the neutron field and the production of 239Pu. This allows the 239Pu to accumulate and burn out in a self limiting oscillation that is characteristic of a Hopf bifurcation. Time dependent results are obtained using a numerical implementation of a reduced order r...

  1. Calibration of 242 Pu Tracer by Mass Spectrometry%质谱法标定242 Pu指示剂

    李冬梅; 徐江; 杜丽丽

    2014-01-01

    将高纯242 Pu浓度标准溶液与239 Pu混合,质谱法测量R239/242(A)先标定四水硫酸钚中239 Pu的浓度;再将四水硫酸钚与待标定的242 Pu指示剂混合,测量R239/242(A),标定242 Pu 指示剂的浓度。质谱测量还可标定得到242 Pu指示剂中的钚同位素丰度。采用两次同位素稀释质谱法标定242 Pu 指示剂快捷简便,可在2日内完成。测量精度高,242 Pu浓度的相对合成标准不确定度为0.75%,该指示剂可满足高精度分析工作的需求。%242 Pu is commonly employed as tracer for determination of 239 Pu in environmental samples.The 239 Pu concentration in Pu(SO4 )2 ·4H2 O solution was determined by isotope dilution-mass spectrometry (ID-MS)using a high pure 242 Pu spike.Then the 242 Pu tracer in our laboratary was calibrated by ID-MS using the calibrated 239 Pu solution as spike.By meas-uring the atom ratio of 239 Pu to 242 Pu twice by ID-MS,the concentration and abundance of the 242 Pu tracer in laboratary were finally calibrated.This method was proved to be efficient with high precision.The process could be finished within two days with an uncertainty of 0.75%. The calibrated 242 Pu tracer in laboratory could meet the demand of high-precision analysis.

  2. Cold regions isotope applications

    Perrigo, L.D.; Divine, T.E.

    1976-04-01

    Pacific Northwest Laboratories (PNL) started the Cold Regions Isotope Applications Program in FY-1975 to identify special conditions in the Arctic and similar geographic areas (Cold Regions) where radioisotope power, heater, or sterilization systems would be desirable and economically viable. Significant progress was made in the first year of this program and all objectives for this initial 12-month period were achieved. The major conclusions and recommendations resulting for this effort are described below. The areas of interest covered include: radiosterilization of sewage; heating of septic tanks; and radioisotope thermoelectric generators as power sources for meteorological instruments and navigational aids. (TFD)

  3. Si Isotopes of Brownleeite

    Nakamura-Messenger, K.; Messenger, Scott R.; Ito, M.; Keller, L. P.; Clemett, S. J.; Jones, J. H.; Tatsuoka, H.; Zolensky, M. E.; Tatsuoka, H.

    2010-01-01

    Brownleeite is a manganese silicide, ideally stoichiometric MnSi, not previously observed in nature until its discovery within an interplanetary dust particle (IDP) that likely originated from a comet [1]. Three discrete brownleeite grains in the IDP L2055 I3 (4 microns in size, hereafter IDP I3) were identified with maximum dimensions of 100, 250 and 600 nm and fully analyzed using scanning-transmission electron microscopy (STEM) [1]. One of the grains (100 nm in size) was poikilitically enclosed by low-Fe, Mn-enriched (LIME) olivine. LIME olivine is epitaxial to the brownleeite with the brownleeite (200) parallel to the olivine c* [1]. LIME olivine is an enigmatic phase first reported from chondritic porous IDPs and some unequilibrated ordinary chondrites [ 2], that is commonly observed in chondritic-porous IDPs. Recently, LIME olivine has been also found in comet Wild-2 (Stardust) samples [3], indicating that LIME olivine is a common mineral component of comets. LIME olivine has been proposed to form as a high temperature condensate in the protosolar nebula [2]. Brownleeite grains also likely formed as high-temperature condensates either in the early Solar System or in the outflow of an evolved star or supernova explosion [1]. The isotopic composition of the brownleeite grains may strongly constrain their ultimate source. To test this hypothesis, we performed isotopic analyses of the brownleeite and the associated LIME olivine, using the NASA/JSC NanoSIMS 50L ion microprobe.

  4. Calcium isotopes in wine

    Holmden, C. E.

    2011-12-01

    The δ 44/40Ca values of bottled wine vary between -0.76% to -1.55% on the seawater scale and correlate weakly with inverse Ca concentration and Mg/Ca ratio, such that the lowest δ 44/40Ca values have the highest Ca concentrations and lowest Mg/Ca ratios. The correlation is notable in the sense that the measured wines include both whites and reds sampled from different wine growing regions of the world, and cover a wide range of quality. Trends among the data yield clues regarding the cause of the observed isotopic fractionation. White wines, and wines generally perceived to be of lower quality, have lower δ 44/40Ca values compared to red wines and wines of generally perceived higher quality. Quality was assessed qualitatively through sensory evaluation, price, and scores assigned by critics. The relationship between δ 44/40Ca and wine quality was most apparent when comparing wines of one varietal from one producer from the same growing region. In the vineyard, wine quality is related to factors such as the tonnage of the crop and the ripeness of the grapes at the time of harvesting, the thickness of the skins for reds, the age of the vines, as well as the place where the grapes were grown (terroir). Quality is also influenced by winemaking practices such as fermentation temperature, duration of skin contact, and barrel ageing. Accordingly, the relationship between δ 44/40Ca and wine quality may originate during grape ripening in the vineyard or during winemaking in the cellar. We tested the grape ripening hypothesis using Merlot grapes sampled from a vineyard in the Okanagan, British Columbia, using sugar content (degrees Brix) as an indicator of ripeness. The grapes were separated into pulp, skin, and pip fractions and were analyzed separately. Thus far, there is no clear evidence for a systematic change in δ 44/40Ca values associated with progressive ripening of grapes in the vineyard. On the day of harvesting, the δ 44/40Ca value of juice squeezed from

  5. {sup 90}Sr, {sup 238}U, {sup 234}U, {sup 137}Cs, {sup 40}K and {sup 239/240}Pu in Emmental type cheese produced in different regions of Western Europe

    Froidevaux, P. E-mail: pascal.froidevaux@inst.hospvd.ch; Geering, J.-J.; Pillonel, L.; Bosset, J.-O.; Valley, J.-F

    2004-07-01

    A method is presented for the determination of {sup 90}Sr and uranium in Emmental type cheese collected in dairy plants from different European countries. Results display a significant correlation (r=0.708, Student t-test=6.02) between the {sup 90}Sr content of the cheese and the altitude of grazing. The highest {sup 90}Sr activity is 1.13 Bq kg{sup -1} of cheese and the lowest is 0.29 Bq kg{sup -1}. Uranium activity is very low with a highest {sup 238}U value of 27 mBq kg{sup -1}. In addition, {sup 234}U/{sup 238}U ratio shows a large enrichment in {sup 234}U for every location. Without any significant indication of the geographic origin of the cheese, this enrichment is believed to be due to the geological features of the pasture, soil and underground water. These results tend to prove that the contamination of milk by uranium originates principally from the water that the cows drink instead of the forage. This finding may have a great importance in models dealing with dairy food contamination by radionuclides following a nuclear accident. Also, the {sup 90}Sr content and to a lesser extent the {sup 234}U/{sup 238}U ratio could be used to trace the authenticity of the origin of the cheese. {sup 137}Cs activity is lower than the detection limit of 0.1 Bq kg{sup -1} in all the samples collected (n=20). Based on natural {sup 40}K activity in cheese (15-21 Bq kg{sup -1}), the decontamination factor for the alkaline cations from milk to cheese is about 20. Plutonium activity stays below the detection limit of 0.3 mBq kg{sup -1}.

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

    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

  7. Competition from Isotopic Modelling

    Virginie Fabre

    2011-01-01

    Full Text Available During later MOIS3, in Europe two populations were present, autochthonous Neanderthals and modern humans. Ecological competition between these two populations has often been evoked but never demonstrated. Our aim is to establish whether resource competition occurred. In this paper, in order to examine the possibility of ecological competition between these two populations, 599 isotopic data were subjected to rigorous statistical treatment and analysis through mixing models. The aim of this paper was to compare dietary strategies of Neanderthals and modern humans over time. Our conclusions suggest that Neanderthals and modern humans shared dietary habits in the particular environmental context of MOIS3 characterised in Europe by climatic deterioration. In this environmental context, the resource competition between Neanderthals and modern humans may have accelerated the disappearance of the Neanderthal population.

  8. Isotope Effects in ESR Spectroscopy

    Werner Herrmann

    2013-06-01

    Full Text Available In order to present the relationship between ESR spectroscopy and isotope effects three levels are considered: (i ESR spectroscopy is described on a general level up to the models for interpretation of the experimental spectra, which go beyond the usually used time and mass independent spin-Hamilton operator, (ii the main characteristics of the generalized isotope effects are worked out, and finally (iii the basic, mainly quantum mechanical effects are used to describe the coupling of electron spins with the degrees of freedom, which are accessible under the selected conditions, of the respective paramagnetic object under investigation. The ESR parameters and the respective models are formalized so far, that they include the time and mass depending influences and reflect the specific isotope effects. Relations will be established between the effects in ESR spectra to spin relaxation, to spin exchange, to the magnetic isotope effect, to the Jahn-Teller effects, as well as to the influence of zero-point vibrations. Examples will be presented which demonstrate the influence of isotopes as well as the kind of accessible information. It will be differentiated with respect to isotope effects in paramagnetic centres itself and in the respective matrices up to the technique of ESR imaging. It is shown that the use of isotope effects is indispensable in ESR spectroscopy.

  9. Compelling Research Opportunities using Isotopes

    None

    2009-04-23

    Isotopes are vital to the science and technology base of the US economy. Isotopes, both stable and radioactive, are essential tools in the growing science, technology, engineering, and health enterprises of the 21st century. The scientific discoveries and associated advances made as a result of the availability of isotopes today span widely from medicine to biology, physics, chemistry, and a broad range of applications in environmental and material sciences. Isotope issues have become crucial aspects of homeland security. Isotopes are utilized in new resource development, in energy from bio-fuels, petrochemical and nuclear fuels, in drug discovery, health care therapies and diagnostics, in nutrition, in agriculture, and in many other areas. The development and production of isotope products unavailable or difficult to get commercially have been most recently the responsibility of the Department of Energy's Nuclear Energy program. The President's FY09 Budget request proposed the transfer of the Isotope Production program to the Department of Energy's Office of Science in Nuclear Physics and to rename it the National Isotope Production and Application program (NIPA). The transfer has now taken place with the signing of the 2009 appropriations bill. In preparation for this, the Nuclear Science Advisory Committee (NSAC) was requested to establish a standing subcommittee, the NSAC Isotope Subcommittee (NSACI), to advise the DOE Office of Nuclear Physics. The request came in the form of two charges: one, on setting research priorities in the short term for the most compelling opportunities from the vast array of disciplines that develop and use isotopes and two, on making a long term strategic plan for the NIPA program. This is the final report to address charge 1. NSACI membership is comprised of experts from the diverse research communities, industry, production, and homeland security. NSACI discussed research opportunities divided into three areas: (1

  10. Carbon isotope geochemistry and geobiology

    Desmarais, D.

    1985-01-01

    Carbon isotope fractionation values were used to understand the history of the biosphere. For example, plankton analyses confirmed that marine extinctions at the end of the Cretaceous period were indeed severe (see Hsu's article in Sundquist and Broeker, 1984). Variations in the isotopic compositions of carbonates and evaporitic sulfates during the Paleozoic reflect the relative abundances of euxinic (anoxic) marine environments and organic deposits from terrestrial flora. The carbon isotopic composition of Precambrian sediments suggest that the enzyme ribulose bisphosphate carboxylase has existed for perhaps 3.5 billion years.

  11. Isotope-edited infrared spectroscopy.

    Buchner, Ginka S; Kubelka, Jan

    2012-01-01

    Isotope-edited infrared (IR) spectroscopy is a powerful tool for studying structural and dynamical properties of peptides and proteins with site-specific resolution. Labeling of selected amide carbonyls with (13)C results in detectable sidebands of amide I' vibrations, which provide information about local conformation and/or solvent exposure without structural perturbation to the protein. Incorporation of isotopically labeled amino acids at specific positions is achieved by the chemical synthesis of the studied proteins. We describe the basic procedures for synthesis of (13)C isotopically edited protein samples, experimental IR spectroscopic measurements, and analysis of the site-specific structural changes from the thermal unfolding IR data.

  12. Apparatus and process for separating hydrogen isotopes

    Heung, Leung K; Sessions, Henry T; Xiao, Xin

    2013-06-25

    The apparatus and process for separating hydrogen isotopes is provided using dual columns, each column having an opposite hydrogen isotopic effect such that when a hydrogen isotope mixture feedstock is cycled between the two respective columns, two different hydrogen isotopes are separated from the feedstock.

  13. Design optimization of radiation shielding structure for lead slowing-down spectrometer system

    Jeong Dong Kim; Sangjoon Ahn; Yong Deok Lee; Chang Je Park

    2015-01-01

    A lead slowing-down spectrometer (LSDS) system is a promising nondestructive assay technique that enables a quantitative measurement of the isotopic contents of major fissile isotopes in spent nuclear fuel and its pyroprocessing counterparts, such as 235U, 239Pu, 241Pu, and, potentially, minor actinides. The LSDS system currently under development at the Korea Atomic Energy Research Institute (Daejeon, Korea) is planned to utilize a high-flux (>1012 n/cm2·s) neutron source comprised of a high...

  14. Alignments in the nobelium isotopes

    ZHENG Shi-Zie; XU Fu-Rong; YUAN Cen-Xi; QI Chong

    2009-01-01

    Total-Routhian-Surface calculations have been performed to investigate the deformation and align-ment properties of the No isotopes. It is found that normal deformed and superdeformed states in these nuclei can coexist at low excitation energies. In neutron-deficient No isotopes, the superdeformed shapes can even become the ground states. Moreover, we plotted the kinematic moments of inertia of the No isotopes, which follow very nicely available experimental data. It is noted that, as the rotational frequency increases, align-ments develop at hω=0.2-0.3 MeV. Our calculations show that the occupation of the vj orbital plays an important role in the alignments of the No isotopes.

  15. Isotopic Changes During Digestion: Protein

    Tuross, N.

    2013-12-01

    Nutrient and hydrological inputs traverse a complicated route of pH, enzymatic and cellular processes in digestion in higher animals. The end products of digestion are the starting products for biosynthesis that are often used to interpret past life-ways. Using an artificial gut system, the isotopic changes (dD, d18O, d13C and d15N) of protein are documented. Three separate protein sources are subjected to the conditions, chemical and enzymatic, found in the stomach and upper small intestine with only a small shift in the oxygen isotopic composition of the proteins observed. Middle to lower small intestine parameters produced both greater isotopic effects and significantly lower molecular weight products. The role of the gastric enterocyte and the likely involvement of the internal milieu of this cell in the isotopic composition of amino acids that are transported to the liver are reported.

  16. Isotope-based quantum information

    G Plekhanov, Vladimir

    2012-01-01

    The present book provides to the main ideas and techniques of the rapid progressing field of quantum information and quantum computation using isotope - mixed materials. It starts with an introduction to the isotope physics and then describes of the isotope - based quantum information and quantum computation. The ability to manipulate and control electron and/or nucleus spin in semiconductor devices provides a new route to expand the capabilities of inorganic semiconductor-based electronics and to design innovative devices with potential application in quantum computing. One of the major challenges towards these objectives is to develop semiconductor-based systems and architectures in which the spatial distribution of spins and their properties can be controlled. For instance, to eliminate electron spin decoherence resulting from hyperfine interaction due to nuclear spin background, isotopically controlled devices are needed (i.e., nuclear spin-depleted). In other emerging concepts, the control of the spatial...

  17. Paleoproxies: Heavy Stable Isotope Perspectives

    Nagler, T. F.; Hippler, D.; Siebert, C.; Kramers, J. D.

    2002-12-01

    Recent advances in isotope ratio mass spectrometry, namely multiple collector ICP-MS and refined TIMS techniques, will significantly enhance the ability to measure heavy stable isotope fractionation, which will lead to the development of a wide array of process-identifying (bio)-geochemical tools. Thus far research in this area is not easily assessable to scientists outside the isotope field. This is due to the fact that analyzing heavy stable isotopes does not provide routine numbers which are per se true (the preciser the truer) but is still a highly experimental field. On the other hand resolving earth science problems requires specialists familiar with the environment being studied. So what is in there for paleoceanographers? In a first order approach, relating isotope variations to physical processes is straightforward. A prominent example are oxygen isotope variations with temperature. The total geological signal is of course far more complicated. At low temperatures, heavy stable isotopes variations have been reported for e.g. Ca, Cr, Fe, Cu, Zn, Mo and Tl. Fractionation mechanisms and physical parameters responsible for the observed variations are not yet resolved for most elements. Significant equilibrium isotope fractionation is expected from redox reactions of transition metals. However a difference in coordination number between two coexisting speciations of an element in the same oxidation state can also cause fractionation. Protonation of dissolved Mo is one case currently discussed. For paleoceanography studies, a principal distinction between transition metals essential for life (V to Zn plus Mo) or not will be helpful. In case of the former group, distinction between biogenic and abiogenic isotope fractionation will remain an important issue. For example, abiotic Fe redox reactions result in isotope fractionations indistinguishable in direction and magnitude from microbial effects. Only a combination of different stable isotope systems bears the

  18. A Dependence of the Electronuclear System Parameters on the Component Concentration in Fuel MOX

    Barashenkov, V S

    2001-01-01

    A dependence of the parameters of a electronuclear system with U-Pu fuel MOX on the relative share of plutonium and its isotope ^{240}Pu in fuel is investigated by means of mathematical modelling. As an example, we consider an experimental system with a heat power 10-20 kW designed in Dubna on the basis of the 660 MeV proton phasotron. The 2 % admixture of ^{240}Pu decreases the value of the neutron multiplication coefficient from 0.95 down to 0.90, neutron yield and heat power are diminished almost twice. Such a decrease can be compensated by the increase of Plutonium share in MOX from 25 up to 27 %.

  19. Isotopes a very short introduction

    Ellam, Rob

    2016-01-01

    An isotope is a variant form of a chemical element, containing a different number of neutrons in its nucleus. Most elements exist as several isotopes. Many are stable while others are radioactive, and some may only exist fleetingly before decaying into other elements. In this Very Short Introduction, Rob Ellam explains how isotopes have proved enormously important across all the sciences and in archaeology. Radioactive isotopes may be familiar from their use in nuclear weapons, nuclear power, and in medicine, as well as in carbon dating. They have been central to establishing the age of the Earth and the origins of the solar system. Combining previous and new research, Ellam provides an overview of the nature of stable and radioactive isotopes, and considers their wide range of modern applications. ABOUT THE SERIES: The Very Short Introductions series from Oxford University Press contains hundreds of titles in almost every subject area. These pocket-sized books are the perfect way to get ahead in a new subjec...

  20. Exotic Structure of Carbon Isotopes

    Suzuki, T; Hagino, K; Suzuki, Toshio; Sagawa, Hiroyuki; Hagino, Kouichi

    2002-01-01

    We studied firstly the ground state properties of C-isotopes using a deformed Hartree-Fock (HF)+ BCS model with Skyrme interactions. Shallow deformation minima are found in several neutron$-$rich C-isotopes. It is shown also that the deformation minima appear in both the oblate and the prolate sides in $^{17}$C and $^{19}$C having almost the same binding energies. Secondly, we carried out shell model calculations to study electromagnetic moments and electric dipole transitions of the C-isotopes. We point out the clear configuration dependence of the quadrupole and magnetic moments in the odd C-isotopes, which will be useful to find out the deformations and the spin-parities of the ground states of these nuclei. We studied electric dipole states of C-isotopes focusing on the interplay between low energy Pigmy strength and giant dipole resonances. Reasonable agreement is obtained with available experimental data for the photoreaction cross sections both in the low energy region below $\\hbar \\omega $=14 MeV and ...

  1. Handbook of environmental isotope geochemistry

    Baskaran, Mark (ed.) [Wayne State Univ., Detroit, MI (United States). Dept. Geology

    2011-07-01

    Applications of radioactive and stable isotopes have revolutionized our understanding of the Earth and near-earth surface processes. The utility of the isotopes are ever-increasing and our sole focus is to bring out the applications of these isotopes as tracers and chronometers to a wider audience so that they can be used as powerful tools to solve environmental problems. New developments in this field remain mostly in peer-reviewed journal articles and hence our goal is to synthesize these findings for easy reference for students, faculty, regulators in governmental and non-governmental agencies, and environmental companies. While this volume maintains its rigor in terms of its depth of knowledge and quantitative information, it contains the breadth needed for wide variety problems and applications in the environmental sciences. This volume presents all of the newer and older applications of isotopes pertaining to the environmental problems in one place that is readily accessible to readers. This book not only has the depth and rigor that is needed for academia, but it has the breadth and case studies to illustrate the utility of the isotopes in a wide variety of environments (atmosphere, oceans, lakes, rivers and streams, terrestrial environments, and sub-surface environments) and serves a large audience, from students and researchers, regulators in federal, state and local governments, and environmental companies. (orig.)

  2. Radiation exposure from anthropogenic actinides in the northern Ukraine; Strahlenexposition durch anthropogene Actinoide in der noerdlichen Ukraine

    Hippler, Sven

    2006-10-31

    As a consequence of the Chernobyl accident, a large area of the northern Ukraine has been contaminated with many different radioactive substances to such an extent that the population hat to be evacuated. Officially, this exclusion still persists today. Meanwhile, people started returning to their dwellings without permission, and they continue living today within the contaminated area. This raises the question of how severe the radiation exposure to the illegal resettlers really is and of whether the restrictions are still justified. Currently, the radiation exposure is mainly being caused by {sup 137}Cs and {sup 90}Sr. But in the long-term, the influence of the long-living man-made actinoids will become important. In this study, their portion of the contamination of the evacuated area and the resulting contribution to the radiation exposure were examined in detail by considering the situation of the village Khristinovka as an example. For these purposes, many different environmental samples from Khristinovka (e.g. soil, food) have been analysed. The determination of the activity concentration of the actinoids was carried out by α-spectrometric measurements after radiochemical separations. Among the different man-made actinoids, only the nuclides {sup 238}Pu, {sup 239}Pu, {sup 240}Pu and {sup 241}Am are of immediate relevance. The most important actinoid is plutonium because of its slow migration in soil. Therefore, the long-living plutonium nuclides will contribute to the radiation exposure even when {sup 90}Sr and {sup 137}Cs will have decayed nearly completely. The observed deposition densities of (126 ± 7) Bq m{sup -2} {sup 239,} {sup 240}Pu and (38.7 ± 3.4) Bq m{sup -2} {sup 238}Pu are comparable to the official statements for this area. Thereby it is possible to distinguish between the contributions which originate from Chernobyl and the nuclear weapons fallout by means of the activity ratios between various radionuclides present. The additional annual

  3. Photonuclear reactions on titanium isotopes

    Belyshev, S. S. [Moscow State University (Russian Federation); Dzhilavyan, L. Z. [Russian Academy of Sciences, Institute for Nuclear Research (Russian Federation); Ishkhanov, B. S.; Kapitonov, I. M. [Moscow State University (Russian Federation); Kuznetsov, A. A., E-mail: kuznets@depni.sinp.msu.ru; Orlin, V. N.; Stopani, K. A. [Moscow State University, Skobeltsyn Institute of Nuclear Physics (Russian Federation)

    2015-03-15

    The photodisintegration of titanium isotopes in the giant-dipole-resonance energy region is studied by the photon-activation method. Bremsstrahlung photons whose spectrum has the endpoint energy of 55 MeV is used. The yields and integrated cross sections are determined for photoproton reactions on the titanium isotopes {sup 47,48,49,50}Ti. The respective experimental results are compared with their counterparts calculated on the basis of the TALYS code and a combined photonucleon-reaction model. The TALYS code disregards the isospin structure of the giant dipole resonance and is therefore unable to describe the yield of photoproton reactions on the heavy titanium isotopes {sup 49,50}Ti.

  4. The terrestrial uranium isotope cycle.

    Andersen, Morten B; Elliott, Tim; Freymuth, Heye; Sims, Kenneth W W; Niu, Yaoling; Kelley, Katherine A

    2015-01-15

    Changing conditions on the Earth's surface can have a remarkable influence on the composition of its overwhelmingly more massive interior. The global distribution of uranium is a notable example. In early Earth history, the continental crust was enriched in uranium. Yet after the initial rise in atmospheric oxygen, about 2.4 billion years ago, the aqueous mobility of oxidized uranium resulted in its significant transport to the oceans and, ultimately, by means of subduction, back to the mantle. Here we explore the isotopic characteristics of this global uranium cycle. We show that the subducted flux of uranium is isotopically distinct, with high (238)U/(235)U ratios, as a result of alteration processes at the bottom of an oxic ocean. We also find that mid-ocean-ridge basalts (MORBs) have (238)U/(235)U ratios higher than does the bulk Earth, confirming the widespread pollution of the upper mantle with this recycled uranium. Although many ocean island basalts (OIBs) are argued to contain a recycled component, their uranium isotopic compositions do not differ from those of the bulk Earth. Because subducted uranium was probably isotopically unfractionated before full oceanic oxidation, about 600 million years ago, this observation reflects the greater antiquity of OIB sources. Elemental and isotope systematics of uranium in OIBs are strikingly consistent with previous OIB lead model ages, indicating that these mantle reservoirs formed between 2.4 and 1.8 billion years ago. In contrast, the uranium isotopic composition of MORB requires the convective stirring of recycled uranium throughout the upper mantle within the past 600 million years.

  5. Non-linear Isotope Effects

    Schmidt, Johan Albrecht

    The isotopic fractionation associated with photodissociation of N2O, OCS and CO2, at different altitudes in Earth’s atmosphere, is investigated theoretically using constructed quantum mechanical models of the dissociation processes (i.e. potential energy surfaces and relevant coupling elements...... or moderate, and overall sulfur fractionation in the stratosphere is very weak which does not exclude OCS from being an acceptable background the Stratospheric Sulfate Aerosol layer. (iii) CO2 photolysis in the upper stratosphere and lower mesosphere is highly fractionating in both isotopes, enriching...

  6. The separation of stable isotopes of carbon

    Oziashvili, E. D.; Egiazarov, A. S.

    1989-04-01

    The present state of work on the separation of carbon isotopes by diffusion, fractional distillation, chemical isotopic exchange, and the selective excitation and dissociation of molecules in electrical discharges or in the field of laser radiation has been examined. The characteristics of new laboratory and industrial assemblies for separating carbon isotopes have been described. Promising directions of study aimed at developing effective technological processes for separating carbon isotopes have been noted. The bibliography contains 148 references.

  7. Brief review on the development of isotope hydrology in China

    汪集旸; 孙占学

    2001-01-01

    The development of isotope hydrology in China is briefly reviewed. It includes oxygen and hydrogen isotopes of precipitation, application of isotope hydrological methodologies in solving water resources problems, isotope hydrological studies on brines and salt lake waters, as well as isotope hydrological investigations of thermal waters. The review focuses on isotope hydrology in China during the last two decades.

  8. Substitution of stable isotopes in Chlorella

    Flaumenhaft, E.; Katz, J. J.; Uphaus, R. A.

    1969-01-01

    Replacement of biologically important isotopes in the alga Chlorella by corresponding heavier stable isotopes produces increasingly greater deviations from the normal cell size and changes the quality and distribution of certain cellular components. The usefulness of isotopically altered organisms increases interest in the study of such permuted organisms.

  9. Dry phase reactor for generating medical isotopes

    Mackie, Thomas Rockwell; Heltemes, Thad Alexander

    2016-05-03

    An apparatus for generating medical isotopes provides for the irradiation of dry-phase, granular uranium compounds which are then dissolved in a solvent for separation of the medical isotope from the irradiated compound. Once the medical isotope is removed, the dissolved compound may be reconstituted in dry granular form for repeated irradiation.

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

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

    2014-05-01

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

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

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

    2013-08-22

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

  12. Bayesian stable isotope mixing models

    In this paper we review recent advances in Stable Isotope Mixing Models (SIMMs) and place them into an over-arching Bayesian statistical framework which allows for several useful extensions. SIMMs are used to quantify the proportional contributions of various sources to a mixtur...

  13. Research Progress of Isotope Technology

    Department; of; Isotope

    2015-01-01

    Radioactive isotope is one of the origins of nonnuclear power technology.In the 12th Five Year Plan period,CIAE made breakthrough progresses on several important fields such as research and development of preparation of radioactive nuclides,preparation of radioactive source and study of radiopharmaceuticals relied on different financial support,successfully

  14. Operation of Electromagnetic Isotope Separator

    MI; Ya-jing

    2015-01-01

    In 2015,we mainly completed the installation of the electromagnetic isotope separator comprehensive technical transformation projects,including the work of installation,debugging,commissioning and acceptance.In June 30,2015,according to the schedule requirements,the project

  15. Isotope Harvesting Opportunities at FRIB

    Morrissey, David

    2017-01-01

    The fragmentation of fast heavy ion beams now at the National Superconducting Cyclotron Laboratory (NSCL) and in the future at the Facility for Rare Isotope Beams (FRIB) under construction produce an unprecedentedly broad spectrum of radionuclides but only a small fraction are used in the on-line rare-isotope program. Projectile fragmentation facilities provide an electromagnetically purified beam of a single projectile fragment for nuclear physics experiments ranging from low energy astrophysics, through nuclear structure studies, to probing fundamental symmetries. By augmenting the NSCL and FRIB production facilities with complimentary collection and purification of discarded ions, called isotope harvesting with chemical purification, many other nuclides will become available for off-line experiments in parallel with the primary experiment. A growing user community has established a list of key target isotopes and is working with the FRIB design team to allow inclusion of necessary equipment in the future. An overview of the possibilities and the techniques will be presented in this talk. Supported by Office of Science, US DOE and Michigan State University.

  16. Calcium isotope analysis by mass spectrometry.

    Boulyga, Sergei F

    2010-01-01

    The variations in the isotopic composition of calcium caused by fractionation in heterogeneous systems and by nuclear reactions can provide insight into numerous biological, geological, and cosmic processes, and therefore isotopic analysis finds a wide spectrum of applications in cosmo- and geochemistry, paleoclimatic, nutritional, and biomedical studies. The measurement of calcium isotopic abundances in natural samples has challenged the analysts for more than three decades. Practically all Ca isotopes suffer from significant isobaric interferences, whereas low-abundant isotopes can be particularly affected by neighboring major isotopes. The extent of natural variations of stable isotopes appears to be relatively limited, and highly precise techniques are required to resolve isotopic effects. Isotope fractionation during sample preparation and measurements and instrumental mass bias can significantly exceed small isotope abundance variations in samples, which have to be investigated. Not surprisingly, a TIMS procedure developed by Russell et al. (Russell et al., 1978. Geochim Cosmochim Acta 42: 1075-1090) for Ca isotope measurements was considered as revolutionary for isotopic measurements in general, and that approach is used nowadays (with small modifications) for practically all isotopic systems and with different mass spectrometric techniques. Nevertheless, despite several decades of calcium research and corresponding development of mass spectrometers, the available precision and accuracy is still not always sufficient to achieve the challenging goals. The present article discusses figures of merits of presently used analytical methods and instrumentation, and attempts to critically assess their limitations. In Sections 2 and 3, mass spectrometric methods applied to precise stable isotope analysis and to the determination of (41)Ca are described. Section 4 contains a short summary of selected applications, and includes tracer experiments and the potential use

  17. A global Ge isotope budget

    Baronas, J. Jotautas; Hammond, Douglas E.; McManus, James; Wheat, C. Geoffrey; Siebert, Christopher

    2017-04-01

    We present measurements of Ge isotope composition and ancillary data for samples of river water, low- and high-temperature hydrothermal fluids, and seawater. The dissolved δ74Ge composition of analyzed rivers ranges from 2.0 to 5.6‰, which is significantly heavier than previously determined values for silicate rocks (δ74Ge = 0.4-0.7‰, Escoube et al., Geostand. Geoanal. Res., 36(2), 2012) from which dissolved Ge is primarily derived. An observed negative correlation between riverine Ge/Si and δ74Ge signatures suggests that the primary δ74Ge fractionation mechanism during rock weathering is the preferential incorporation of light isotopes into secondary weathering products. High temperature (>150 °C) hydrothermal fluids analyzed in this study have δ74Ge of 0.7-1.6‰, most likely fractionated during fluid equilibration with quartz in the reaction zone. Low temperature (25-63 °C) hydrothermal fluids are heavier (δ74Ge between 2.9‰ and 4.1‰) and most likely fractionated during Ge precipitation with hydrothermal clays. Seawater from the open ocean has a δ74Gesw value of 3.2 ± 0.4‰, and is indistinguishable among the different ocean basins at the current level of precision. This value should be regulated over time by the isotopic balance of Ge sources and sinks, and a new compilation of these fluxes is presented, along with their estimated isotopic compositions. Assuming steady-state, non-opal Ge sequestration during sediment authigenesis likely involves isotopic fractionation Δ74Gesolid-solution that is -0.6 ± 1.8‰.

  18. Modelling stable water isotopes: Status and perspectives

    Werner M.

    2010-12-01

    Full Text Available Modelling of stable water isotopes H2 18O and HDO within various parts of the Earth’s hydrological cycle has clearly improved our understanding of the interplay between climatic variations and related isotope fractionation processes. In this article key principles and major research results of stable water isotope modelling studies are described. Emphasis is put on research work using explicit isotope diagnostics within general circulation models as this highly complex model setup bears many resemblances with studies using simpler isotope modelling approaches.

  19. TANGRA-Setup for the Investigation of Nuclear Fission induced by 14.1 MeV neutrons

    RUSKOV I.; Kopatch, Y; BYSTRITSKY V.; Skoy, V.; SHVETSOV V.; Hambsch, Franz-Josef; Oberstedt, Stephan; CAPOTE NOY R.; Sedyshev, P.; GROZDANOV D.; IVANOV I. Zh.; ALEKSAKHIN V. Yu.; BOGOLUBOV E. P.; BARMAKOV Y.; Khabarov, S. V.

    2015-01-01

    The new experimental setup TANGRA (Tagged Neutrons & Gamma Rays), for the investigation of neutron induced nuclear reactions, e.g. (n,xn’), (n,xn’γ), (n,γ), (n,f), on a number of important isotopes for nuclear science and engineering (235,238U, 237Np, 239Pu, 244,245,248Cm) is under construction and being tested at the Frank Laboratory of Neutron Physics (FLNP) of the Joint Institute for Nuclear Research (JINR) in Dubna. The TANGRA setup consists of: a portable neutron generator ING-27, wit...

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

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

    2014-05-01

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

  1. Heavy atom isotope effects on enzymatic reactions

    Paneth, Piotr

    1994-05-01

    The theory of isotope effects, which has proved to be extremely useful in providing geometrical details of transition states in a variety of chemical reactions, has recently found an application in studies of enzyme-catalyzed reactions. These reactions are multistep in nature with few steps being partially rate-limiting, thus interpretation of these isotope effects is more complex. The theoretical framework of heavy-atom isotope effects on enzymatic reactions is critically analyzed on the basis of recent results of: carbon kinetic isotope effects on carbonic anhydrase and catalytic antibodies; multiple carbon, deuterium isotope effects on reactions catalyzed by formate decarboxylase; oxygen isotope effects on binding processes in reactions catalyzed by pyruvate kinase; and equilibrium oxygen isotope effect on binding an inhibitor to lactate dehydrogenase. The advantages and disadvantages of reaction complexity in learning details of formal and molecular mechanisms are discussed in the examples of reactions catalyzed by phosphoenolpyruvate carboxylase, orotidine decarboxylase and glutamine synthetase.

  2. Zinc isotopic compositions of breast cancer tissue.

    Larner, Fiona; Woodley, Laura N; Shousha, Sami; Moyes, Ashley; Humphreys-Williams, Emma; Strekopytov, Stanislav; Halliday, Alex N; Rehkämper, Mark; Coombes, R Charles

    2015-01-01

    An early diagnostic biomarker for breast cancer is essential to improve outcome. High precision isotopic analysis, originating in Earth sciences, can detect very small shifts in metal pathways. For the first time, the natural intrinsic Zn isotopic compositions of various tissues in breast cancer patients and controls were determined. Breast cancer tumours were found to have a significantly lighter Zn isotopic composition than the blood, serum and healthy breast tissue in both groups. The Zn isotopic lightness in tumours suggests that sulphur rich metallothionein dominates the isotopic selectivity of a breast tissue cell, rather than Zn-specific proteins. This reveals a possible mechanism of Zn delivery to Zn-sequestering vesicles by metallothionein, and is supported by a similar signature observed in the copper isotopic compositions of one breast cancer patient. This change in intrinsic isotopic compositions due to cancer has the potential to provide a novel early biomarker for breast cancer.

  3. Measuring SNM Isotopic Distributions using FRAM

    Geist, William H. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2015-12-02

    The first group of slides provides background information on the isotopic composition of plutonium. It is shown that 240Pu is the critical isotope in neutron coincidence/multiplicity counting. Next, response function analysis to determine isotopic composition is discussed. The isotopic composition can be determined by measuring the net peak counts from each isotope and then taking the ratio of the counts for each isotope relative to the total counts for the element. Then FRAM (Fixed energy Response function Analysis with Multiple efficiencies) is explained. FRAM can control data acquisition, automatically analyze newly acquired data, analyze previously acquired data, provide information on the quality of the analysis, and facilitate analysis in unusual situations (non-standard energy calibrations, gamma rays from non-SNM isotopes, poor spectra (within limits)).

  4. Isotope hydrology of catchment basins: lithogenic and cosmogenic isotopic systems

    Nimz, G. J., LLNL

    1998-06-01

    A variety of physical processes affect solute concentrations within catchment waters. The isotopic compositions of the solutes can indicate which processes have determined the observed concentrations. These processes together constitute the physical history of the water. Many solutes in natural waters are derived from the interaction between the water and the rock and/or soil within the system - these are termed `lithogenic` solutes. The isotopic compositions of these solutes provide information regarding rock-water interactions. Many other solutes have their isotopic compositions determined both within and outside of the catchment - i.e., in addition to being derived from catchment rock and soil, they are solutes that are also transported into the catchment. Important members of this group include solutes that have isotopic compositions produced by atomic particle interactions with other nuclides. The source of the atomic particles can be cosmic radiation (producing `cosmogenic` nuclides in the atmosphere and land surface), anthropogenic nuclear reactions (producing `thermonuclear` nuclides), or radioactive and fission decay of naturally-occurring elements, principally {sup 238}U (producing `in-situ` lithogenic nuclides in the deep subsurface). Current language usage often combines all of the atomic particle-produced nuclides under the heading `cosmogenic nuclides`, and for simplicity we will often follow that usage here, although always indicating which variety is being discussed. This paper addresses the processes that affect the lithogenic and cosmogenic solute concentrations in catchment waters, and how the isotopic compositions of the solutes can be used in integrative ways to identify these processes, thereby revealing the physical history of the water within a catchment system. The concept of a `system` is important in catchment hydrology. A catchment is the smallest landscape unit that can both participate in all of the aspects of the hydrologic cycle and

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

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

    2000-06-28

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

  6. Assessment and reduction of proliferation risk of reactor-grade plutonium regarding construction of ‘fizzle bombs’ by terrorists

    Serfontein, Dawid E., E-mail: Dawid.Serfontein@nwu.ac.za [School for Mechanical and Nuclear Engineering, North West University (PUK-Campus), PRIVATE BAG X6001 (Internal Post Box 360), Potchefstroom 2520 (South Africa); Mulder, Eben J. [School for Mechanical and Nuclear Engineering, North West University (South Africa); Reitsma, Frederik [Calvera Consultants (South Africa)

    2014-05-01

    The approximately 23.7 wt% {sup 240}Pu in reactor-grade plutonium denatures the {sup 239}Pu to the extent that it cannot fuel high yield nuclear weapons. {sup 240}Pu has a high spontaneous fission rate, which increases the spontaneous neutron flux within the fuel. When such a nuclear weapon is triggered, these neutrons cause the nuclear fission chain reaction to pre-detonate which blows the imploding fuel shell apart before the designed level of compression and reactivity could be attained, thereby greatly reducing the average energy yield of such “fizzle” bombs. Therefore reactor-grade plutonium is normally viewed as highly proliferation resistant. In this article the literature on the proliferation resistance of reactor-grade plutonium and on the mechanism and effect of fizzle bombs is reviewed in order to test this view. It is shown that even very low yield fizzle bombs, exploded in urban areas, would still cause serious blast damage as well as radioactive contamination. Combined with the high levels of induced terror, fizzle bombs might thus be attractive psychological weapons for terrorists. Therefore reactor-grade plutonium may not be sufficiently proliferation resistant against nuclear terrorism. However, denaturisation with more than 9% {sup 238}Pu produces high levels of decay heat which will melt or explode the high explosives around uncooled implosion type weapons, rendering them useless. Unfortunately, reactor-grade Pu contains only 2.7% {sup 238}Pu and is thus not sufficiently proliferation resistant in this respect. It is also shown that the associated neptunium poses a substantial proliferation risk. In the present study strong improvement of the proliferation resistance was demonstrated by simulation of incineration of reactor-grade plutonium in the 400 MW{sub th} Pebble Bed Modular Reactor Demonstration Power Plant. Results for modified fuel cycles, aimed at transmutating {sup 237}Np to {sup 238}Pu are also reported. However, these

  7. Deposition of artificial radionuclides from atmospheric Nuclear Weapon Tests estimated by soil inventories in French areas low-impacted by Chernobyl

    Le Roux, Gael, E-mail: gael.leroux@ensat.f [Institut de Radioprotection et Surete Nucleaire, DEI/SESURE, Laboratoires d' Etudes Radioecologiques en milieu Continental et Marin, CEN Cadarache Bat. 153 BP 3, 13115 St Paul lez Durance (France); Duffa, Celine; Vray, Francoise; Renaud, Philippe [Institut de Radioprotection et Surete Nucleaire, DEI/SESURE, Laboratoires d' Etudes Radioecologiques en milieu Continental et Marin, CEN Cadarache Bat. 153 BP 3, 13115 St Paul lez Durance (France)

    2010-03-15

    Soil inventories of anthropogenic radionuclides were investigated in altitudinal transects in 2 French regions, Savoie and Montagne Noire. Rain was negligible in these 2 areas the days after the Chernobyl accident. Thus anthropogenic radionuclides are coming hypothetically only from Global Fallout following Atmospheric Nuclear Weapon Tests. This is confirmed by the isotopic signatures ({sup 238}Pu/{sup 239+240}Pu; {sup 137}Cs/{sup 239+240}Pu; and {sup 241}Am/{sup 239+240}Pu) close to Global Fallout value. In Savoie, a peat core age-dated by {sup 210}Pb{sub ex} confirmed that the main part of deposition of anthropogenic radionuclides occurred during the late sixties and the early seventies. In agreement with previous studies, the anthropogenic radionuclide inventories are well correlated with the annual precipitations. However, this is the first time that a study investigates such a large panel of annual precipitation and therefore of anthropogenic radionuclide deposition. It seems that at high-altitude sites, deposition of artificial radionuclides was higher possibly due to orographic precipitations.

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

    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.

  9. Lasers utilizing CO2 isotopes

    Pechenin, Iu. V.; Domanov, M. S.

    1980-08-01

    The emission spectra and power characteristics of CW (C-12)(O-16)2, (C-13)(O-16)2, (C-12)(O-16)(O-18)2 and (C-12)(O-18) lasers are investigated. Laser output power is found to depend equally on the proportion of carbon and oxygen isotopes in the active medium for all isotopes except the asymmetrical (C-12)(O-16)(O-18), in which maximum output power is four to five times less due to the doubling of emission lines and limited enrichment caused by recombination into (C-12)(O-16)2 and (C-12)(O-18)2 molecules during discharge. The unsaturated gain is observed to increase linearly with enrichment, with that of nonsymmetrical molecules half that of the symmetrical molecules, while the maximum power output is independent of enrichment.

  10. Interstellar Isotopes: Prospects with ALMA

    Charnley Steven B.

    2010-01-01

    Cold molecular clouds are natural environments for the enrichment of interstellar molecules in the heavy isotopes of H, C, N and O. Anomalously fractionated isotopic material is found in many primitive Solar System objects, such as meteorites and comets, that may trace interstellar matter that was incorporated into the Solar Nebula without undergoing significant processing. Models of the fractionation chemistry of H, C, N and O in dense molecular clouds, particularly in cores where substantial freeze-out of molecules on to dust has occurred, make several predictions that can be tested in the near future by molecular line observations. The range of fractionation ratios expected in different interstellar molecules will be discussed and the capabilities of ALMA for testing these models (e.g. in observing doubly-substituted isotopologues) will be outlined.

  11. Natural fractionation of uranium isotopes

    Noordmann, Janine

    2015-01-24

    The topic of this thesis was the investigation of U (n({sup 238}U) / n({sup 235}U)) isotope variations in nature with a focus on samples (1) that represent the continental crust and its weathering products (i.e. granites, shales and river water) (2) that represent products of hydrothermal alteration on mid-ocean ridges (i.e. altered basalts, carbonate veins and hydrothermal water) and (3) from restricted euxinic basins (i.e. from the water column and respective sediments). The overall goal was to explore the environmental conditions and unravel the mechanisms that fractionate the two most abundant U isotopes, n({sup 238}U) and n({sup 235}U), on Earth.

  12. A novel methodology to investigate isotopic biosignatures

    Horner, T. J.; Lee, R. B. Y.; Henderson, G. M.; Rickaby, R. E. M.

    2012-04-01

    An enduring goal of trace metal isotopic studies of Earth History is to find isotopic 'fingerprints' of life or of life's individual physiochemical processes. Generally, such signatures are sought by relating an isotopic effect observed in controlled laboratory conditions or a well-characterized environment to a more complex system or the geological record. However, such an approach is ultimately limited because life exerts numerous isotopic fractionations on any one element so it is hard to dissect the resultant net fractionation into its individual components. Further, different organisms, often with the same apparent cellular function, can express different isotopic fractionation factors. We have used a novel method to investigate the isotopic fractionation associated with a single physiological process-enzyme specific isotopic fractionation. We selected Cd isotopes since only one biological use of Cd is known, CdCA (a Cd/Zn carbonic anhydrase from the coastal diatom T. Weissflogii). Thus, our investigation can also inform the long standing mystery as to why this generally toxic element appears to have a nutrient-like dissolved isotopic and concentration profile in the oceans. We used the pET-15b plasmid to insert the CdCA gene into the E. coli genome. There is no known biochemical function for Cd in E. coli, making it an ideal vector for studying distinct physiological processes within a single organism. The uptake of Cd and associated isotopic fractionation was determined for both normal cells and those expressing CdCA. It was found that whole cells always exhibited a preference for the light isotopes of Cd, regardless of the expression of CdCA; adsorption of Cd to cell surfaces was not seen to cause isotopic fractionation. However, the cleaning procedure employed exerted a strong control on the observed isotopic composition of cells. Using existing protein purification techniques, we measured the Cd isotopic composition of different subcellular fractions of E

  13. Pb isotopes during mingling and melting

    Waight, Tod Earle; Lesher, Charles E.

    2010-01-01

    Pb isotopic data are presented for hybrid rocks formed by mingling between mantle-derived tholeiitic magma of the Eocene Miki Fjord macrodike (East Greenland) and melt derived from the adjacent Precambrian basement. Bulk mixing and AFC processes between end-members readily identified in the field...... fail to model the Pb isotope systematics. Selective contamination during diffusional exchange, which can explain the complex Sr and Nd isotope compositions of the hybrid rocks (Blichert-Toft et al., 1992), cannot fully account for the variability of the Pb isotopic data using the identified crustal end......-members. The crustal anatectic end-member, although similar in Sr and Nd isotope composition, has a markedly different Pb isotopic composition than its source gneiss. The differences are consistent with preferential incorporation of radiogenic Pb from accessory phases such as metamict zircon or loosely-bound Pb from...

  14. Normalization of oxygen and hydrogen isotope data

    Coplen, T.B.

    1988-01-01

    To resolve confusion due to expression of isotopic data from different laboratories on non-corresponding scales, oxygen isotope analyses of all substances can be expressed relative to VSMOW or VPDB (Vienna Peedee belemnite) on scales normalized such that the ??18O of SLAP is -55.5% relative to VSMOW. H3+ contribution in hydrogen isotope ratio analysis can be easily determined using two gaseous reference samples that differ greatly in deuterium content. ?? 1988.

  15. Silicon isotopes: from cosmos to benthos

    Chakrabarti, Ramananda

    2015-01-01

    Silicon is the second most abundant element on the Earth and one of the more abundant elements in our Solar System. Variations in the relative abundance of the stable isotopes of Si (Si isotope fractionation) in different natural reservoirs, both terrestrial (surface and deep Earth) as well as extra-terrestrial (e.g. meteorites, lunar samples), are a powerful tracer of present and past processes involving abiotic as well as biotic systems. The versatility of the Si isotope tracer is reflected...

  16. Production of radioactive isotopes from stable isotopes, for nuclear medicine; A partir d`isotopes stables, production d`isotopes radioactifs pour la medecine nucleaire

    Bourdoiseau, M. [CEA Centre d`Etudes de Saclay, 91 - Gif-sur-Yvette (France). Office des Rayonnements Ionisants

    1994-12-31

    Around 15 radioactive isotopes only are used for nuclear medicine diagnosis (kinetics or preferential fixation in the body); characteristics of these {gamma} and {beta}-minus emitters are presented: period, energy, production mode (isotopic filiation, fission product separation, cyclotron, reactor); details are given on applications, production mode, properties and consumption of various isotopes: Technetium 99m, Thallium 201, Iodine 123, Indium 111, Gallium 67, Rhenium 186, Erbium 169, Yttrium 90, Iron 59, Chromium 51, Krypton 81m. 1 tab.

  17. Quantitative microbial ecology through stable isotope probing.

    Hungate, Bruce A; Mau, Rebecca L; Schwartz, Egbert; Caporaso, J Gregory; Dijkstra, Paul; van Gestel, Natasja; Koch, Benjamin J; Liu, Cindy M; McHugh, Theresa A; Marks, Jane C; Morrissey, Ember M; Price, Lance B

    2015-11-01

    Bacteria grow and transform elements at different rates, and as yet, quantifying this variation in the environment is difficult. Determining isotope enrichment with fine taxonomic resolution after exposure to isotope tracers could help, but there are few suitable techniques. We propose a modification to stable isotope probing (SIP) that enables the isotopic composition of DNA from individual bacterial taxa after exposure to isotope tracers to be determined. In our modification, after isopycnic centrifugation, DNA is collected in multiple density fractions, and each fraction is sequenced separately. Taxon-specific density curves are produced for labeled and nonlabeled treatments, from which the shift in density for each individual taxon in response to isotope labeling is calculated. Expressing each taxon's density shift relative to that taxon's density measured without isotope enrichment accounts for the influence of nucleic acid composition on density and isolates the influence of isotope tracer assimilation. The shift in density translates quantitatively to isotopic enrichment. Because this revision to SIP allows quantitative measurements of isotope enrichment, we propose to call it quantitative stable isotope probing (qSIP). We demonstrated qSIP using soil incubations, in which soil bacteria exhibited strong taxonomic variations in (18)O and (13)C composition after exposure to [(18)O]water or [(13)C]glucose. The addition of glucose increased the assimilation of (18)O into DNA from [(18)O]water. However, the increase in (18)O assimilation was greater than expected based on utilization of glucose-derived carbon alone, because the addition of glucose indirectly stimulated bacteria to utilize other substrates for growth. This example illustrates the benefit of a quantitative approach to stable isotope probing.

  18. The trend of stable isotope separation

    Yonekawa, Shigeru [Power Reactor and Nuclear Fuel Development Corp., Kamisaibara, Okayama (Japan). Ningyo Toge Works; Aoki, Eiji; Yato, Yumio

    1994-12-01

    Recently, stable isotopes are used in the field of medical science, nuclear physics, environmental science and agriculture. This report reviews the present status of stable isotope enrichment in ORNL, Urenco, Russia and PNC. Further the utilization method of the stable isotopes in the field of medical science, nuclear power and material science are described, and the application possibility of Laser separation method and Gas Centrifuge method are estimated. There are many overseas actual results of stable isotope separation with Gas Centrifuge method, therefore this method is possible enough in principle. (author).

  19. Scattering lengths of calcium and barium isotopes

    Dammalapati, U.; Willmann, L.; Knoop, S. [Kernfysisch Versneller Instituut (KVI), University of Groningen, Zernikelaan 25, 9747 AA Groningen (Netherlands); LaserLaB Vrije Universiteit, De Boelelaan 1081, 1081 HV Amsterdam (Netherlands)

    2011-11-15

    We have calculated the s-wave scattering length of all the even isotopes of calcium (Ca) and barium (Ba) in order to investigate the prospect of Bose-Einstein condensation (BEC). For Ca we have used an accurate molecular potential based on detailed spectroscopic data. Our calculations show that Ca does not provide other isotopes alternative to the recently Bose condensed {sup 40}Ca that suffers strong losses because of a very large scattering length. For Ba we show by using a model potential that the even isotopes cover a broad range of scattering lengths, opening the possibility of BEC for at least one of the isotopes.

  20. Copper isotope fractionation by desert shrubs

    Navarrete, Jesica U., E-mail: jnavarrete2@miners.utep.edu [University of Texas at El Paso, Department of Geological Sciences, 500 W. University Ave, El Paso, TX 79968 (United States); Viveros, Marian; Ellzey, Joanne T. [University of Texas at El Paso, Department of Biological Sciences, El Paso, TX 79968 (United States); Borrok, David M. [University of Texas at El Paso, Department of Geological Sciences, 500 W. University Ave, El Paso, TX 79968 (United States)

    2011-06-15

    Copper has two naturally occurring stable isotopes of masses 63 and 65 which can undergo mass dependent fractionation during various biotic and abiotic chemical reactions. These interactions and their resulting Cu isotope fractionations can be used to determine the mechanisms involved in the cycling of Cu in natural systems. In this study, Cu isotope changes were investigated at the organismal level in the metal-accumulating desert plant, Prosopis pubescens. Initial results suggest that the lighter Cu isotope was preferentially incorporated into the leaves of the plant, which may suggest that Cu was actively transported via intracellular proteins. The roots and stems show a smaller degree of Cu isotope fractionation and the direction and magnitude of the fractionations was dependent upon the levels of Cu exposure. Based on this and previous work with bacteria and yeast, a trend is emerging that suggests the lighter Cu isotope is preferentially incorporated into biological components, while the heavier Cu isotope tends to become enriched in aqueous solutions. In bacteria, plants and animals, intracellular Cu concentrations are strictly regulated via dozens of enzymes that can bind, transport, and store Cu. Many of these enzymes reduce Cu(II) to Cu(I). These initial results seem to fit into a broader picture of Cu isotope cycling in natural systems where oxidation/reduction reactions are fundamental in controlling the distributions of Cu isotopes.

  1. Simultaneous photon and neutron interrogation using an electron accelerator in order to quantify actinides in encapsulated radioactive wastes; Double interrogation simultanee neutrons et photons utilisant un accelerateur d'electrons pour la caracterisation separee des actinides dans les dechets radioactifs enrobes

    Jallu, F

    1999-09-24

    Measuring out alpha emitters, such as ({sup 234,235,236,238}U {sup 238,239,240,242,}2{sup 44P}u, {sup 237}Np {sup 241,243}Am...), in solid radioactive waste, allows us to quantify the alpha activity in a drum and then to classify it. The SIMPHONIE (SIMultaneous PHOton and Neutron Interrogation Experiment) method, developed in this Ph.D. work, combines both the Active Neutron Interrogation and the Induced Photofission Interrogation techniques simultaneously. Its purpose is to quantify in only one measurement, fissile ({sup 235}U, {sup 239,241}Pu...) and fertile ({sup 236,238}U, {sup 238,240}Pu...) elements separately. In the first chapter of this Ph.D. report, we present the principle of the Radioactive Waste Management in France. The second chapter deals with the physical properties of neutron fission and of photofission. These two nuclear reactions are the basis of the SIMPHONIE method. Moreover, one of our purposes was to develop the ELEPHANT (ELEctron PHoton And Neutron Transport) code in view to simulate the electron, photon and neutron transport, including the ({gamma}, n), ({gamma}, 2n) and ({gamma}, f) photonuclear reactions that are not taken into account in the MCNP4 (Monte Carlo N-Particle) code. The simulation codes developed and used in this work are detailed in the third chapter. Finally, the fourth chapter gives the experimental results of SIMPHONIE obtained by using the DGA/ETCA electron linear accelerators located at Arcueil, France. Fissile ({sup 235}U, {sup 239}Pu) and fertile ({sup 238}U) samples were studied. Furthermore, comparisons between experimental results and calculated data of photoneutron production in tungsten, copper, praseodymium and beryllium by using an electron LINear Accelerator (LINAC) are given. This allows us to evaluate the validity degree of the ELEPHANT code, and finally the feasibility of the SIMPHONIE method. (author)

  2. Low and intermediate level waste in SFR-1. Reference Waste Inventory 2007

    Almkvist, Lisa (Vattenfall Power Consultant AB, Stockholm (SE)); Gordon, Anna (Swedish Nuclear Fuel and Waste Management Co., Stockholm (SE))

    2007-11-15

    The objective with this report is to describe all the waste and the waste package that is expected to be deposited in SFR 1 at the time of closure. The report will form the basis for the release calculation in the safety analysis for SFR 1. Three different scenarios are explored in this report; the waste inventory is based on an estimated operational lifetime of the Swedish nuclear power plants of 50 and 60 years and that closure of the SFR 1 repository will take place in 2040 or 2050 respectively. The third scenario is where the repository is full (one part where the activity adds up to 1016 Bq and one part where the repository is considered full regarding volume). In the report, data about geometries, weights, materials, chemicals and radionuclide are given. No chemotoxic material has been identified in the waste. The inventory is estimated using the Prosit-interface which extracts information from the Triumf database. The inventory is based on so called 'waste types' and the waste types' 'reference waste package'. The reference waste package combined with a prognosis of the number of waste packages to be delivered to SFR 1 gives the final waste inventory for SFR 1. All reference waste packages are thoroughly described in the appendices of this report. The reference waste packages are as far as possible based on actual experiences and measurements. The radionuclide inventory is also based on actual measurements. The inventory is based on measurements of 60Co and 137Cs in waste packages and on measurements of 239Pu and 240Pu in reactor water. Other nuclides in the inventory are calculated with correlation factors

  3. Low and intermediate level waste in SFR-1. Reference waste inventory

    Riggare, P.; Johansson, Claes

    2001-06-01

    The objective with this report is to describe all the waste and the waste package that is expected to be deposited in SFR-1 at the time of closure. This report is a part of the SAFE project (Safety Assessment of Final Repository for Radioactive Operational Waste), i.e. the renewed safety assessment of SFR-1. The accounted waste inventory has been used as input to the release calculation that has been performed in the SAFE project. The waste inventory is based on an estimated operational lifetime of the Swedish nuclear power plants of 40 years and that closure of the SFR repository will happen in 2030. In the report, data about geometries, weights, materials, chemicals and radionuclide are given. No chemo toxic material has been identified in the waste. The inventory is based on so called waste types and the waste types reference waste package. The reference waste package combined with a prognosis of the number of waste packages to the year 2030 gives the final waste inventory for SFR-1. All reference waste packages are thoroughly described in the appendices of this report. The reference waste packages are as far as possible based on actual experiences and measurements. The radionuclide inventory is also based on actual measurements. The inventory is based on measurements of {sup 60}Co and {sup 137} Cs in waste packages and on measurements {sup 239}Pu and {sup 240}Pu in reactor water. Other nuclides in the inventory are calculated with correlation factors. In the SAFE project's prerequisites it was said that one realistic and one conservative (pessimistic) inventory should be produced. The conservative one should then be used for the release calculations. In this report one realistic and one conservative radionuclide inventory is presented. The conservative one adds up to 10{sup 16} Bq. Regarding materials there is only one inventory given since it is not certain what is a conservative assumption.

  4. Critical experiments on single-unit spherical plutonium geometries reflected and moderated by oil

    Rothe, R.E.

    1997-05-01

    Experimental critical configurations are reported for several dozen spherical and hemispherical single-unit assemblies of plutonium metal. Most were solid but many were hollow-centered, thick, shell-like geometries. All were constructed of nested plutonium (mostly {sup 2139}Pu) metal hemispherical shells. Three kinds of critical configurations are reported. Two required interpolation and/or extrapolation of data to obtain the critical mass because reflector conditions were essentially infinite. The first finds the plutonium essentially fully reflected by a hydrogen-rich oil; the second is essentially unreflected. The third kind reports the critical oil reflector height above a large plutonium metal assembly of accurately known mass (no interpolation required) when that mass was too great to permit full oil reflection. Some configurations had thicknesses of mild steel just outside the plutonium metal, separating it from the oil. These experiments were performed at the Rocky Flats Critical Mass Laboratory in the late 1960s. They have not been published in a form suitable for benchmark-quality comparisons against state-of-the-art computational techniques until this paper. The age of the data and other factors lead to some difficulty in reconstructing aspects of the program and may, in turn, decrease confidence in certain details. Whenever this is true, the point is acknowledged. The plutonium metal was alpha-phase {sup 239}Pu containing 5.9 wt-% {sup 240}Pu. All assemblies were formed by nesting 1.667-mm-thick (nominal) bare plutonium metal hemispherical shells, also called hemishells, until the desired configuration was achieved. Very small tolerance gaps machined into radial dimensions reduced the effective density a small amount in all cases. Steel components were also nested hemispherical shells; but these were nominally 3.333-mm thick. Oil was used as the reflector because of its chemical compatibility with plutonium metal.

  5. SCALED ELECTRON MODEL OF A DOGBONE MUON RLA WITH MULTI-PASS ARCS

    Kevin Beard, Rolland Johnson, Vasiliy Morozov, Yves Roblin, Andrew Hutton, Geoffrey Krafft, Slawomir Bogacz

    2012-07-01

    The design of a dogbone RLA with linear-field multi-pass arcs was earlier developed for accelerating muons in a Neutrino Factory and a Muon Collider. It allows for efficient use of expensive RF while the multi-pass arc design based on linear combined-function magnets exhibits a number of advantages over separate-arc or pulsed-arc designs. Such an RLA may have applications going beyond muon acceleration. This paper describes a possible straightforward test of this concept by scaling a GeV scale muon design for electrons. Scaling muon momenta by the muon-to-electron mass ratio leads to a scheme, in which a 4.5 MeV electron beam is injected at the middle of a 3 MeV/pass linac with two double-pass return arcs and is accelerated to 18 MeV in 4.5 passes. All spatial dimensions including the orbit distortion are scaled by a factor of 7.5, which arises from scaling the 200 MHz muon RF to a readily available at CEBAF 1.5 GHz. The footprint of a complete RLA fits in an area of 25 by 7 m. The scheme utilizes only fixed magnetic fields including injection and extraction. The hardware requirements are not very demanding, making it straightforward to implement. In this report, we have shown first of all that measuring the energy spectrum of the fast neutrons in the liquid scintillators allows one to distinguish the two chemical forms of plutonium. In addition, combining this information with the Feynman 2-neutron and 3-neutron correlations allows one to extract the {alpha}-ratio without explicitly knowing the multiplication. Given the {alpha}-ratio one can then extract the multiplication as well as the {sup 239}Pu and {sup 240}Pu masses directly from the moment equations.

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

    Snider, C.A. [Department of Energy, Carlsbad, NM (United States); Weston, W.W. [Westinghouse Electric Corp., Carlsbad, NM (United States)

    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.

  7. Uranium isotopes fingerprint biotic reduction

    Stylo, Malgorzata; Neubert, Nadja; Wang, Yuheng; Monga, Nikhil; Romaniello, Stephen J.; Weyer, Stefan; Bernier-Latmani, Rizlan

    2015-01-01

    Knowledge of paleo-redox conditions in the Earth’s history provides a window into events that shaped the evolution of life on our planet. The role of microbial activity in paleo-redox processes remains unexplored due to the inability to discriminate biotic from abiotic redox transformations in the rock record. The ability to deconvolute these two processes would provide a means to identify environmental niches in which microbial activity was prevalent at a specific time in paleo-history and to correlate specific biogeochemical events with the corresponding microbial metabolism. Here, we demonstrate that the isotopic signature associated with microbial reduction of hexavalent uranium (U), i.e., the accumulation of the heavy isotope in the U(IV) phase, is readily distinguishable from that generated by abiotic uranium reduction in laboratory experiments. Thus, isotope signatures preserved in the geologic record through the reductive precipitation of uranium may provide the sought-after tool to probe for biotic processes. Because uranium is a common element in the Earth’s crust and a wide variety of metabolic groups of microorganisms catalyze the biological reduction of U(VI), this tool is applicable to a multiplicity of geological epochs and terrestrial environments. The findings of this study indicate that biological activity contributed to the formation of many authigenic U deposits, including sandstone U deposits of various ages, as well as modern, Cretaceous, and Archean black shales. Additionally, engineered bioremediation activities also exhibit a biotic signature, suggesting that, although multiple pathways may be involved in the reduction, direct enzymatic reduction contributes substantially to the immobilization of uranium. PMID:25902522

  8. CO Isotopes in Planetary Nebulae

    Balser, Dana S.; McMullin, Joseph P.; Wilson, T. L.

    2002-01-01

    Standard stellar evolution theory is inconsistent with the observed isotopic carbon ratio, 12C/13C, in evolved stars. This theory is also inconsistent with the 3He/H abundance ratios observed in Galactic HII regions, when combined with chemical evolution theory. These discrepancies have been attributed to an extra, non-standard mixing which further processes material during the RGB and should lower both the 12C/13C and 3He/H abundance ratios for stars with masses < 2 solar masses. Measurement...

  9. Silicon isotope fractionation during magmatic differentiation

    Savage, Paul S.; Georg, R. Bastian; Williams, Helen M.; Burton, Kevin W.; Halliday, Alex N.

    2011-10-01

    The Si isotopic composition of Earth's mantle is thought to be homogeneous (δ 30Si = -0.29 ± 0.08‰, 2 s.d.) and not greatly affected by partial melting and recycling. Previous analyses of evolved igneous material indicate that such rocks are isotopically heavy relative to the mantle. To understand this variation, it is necessary to investigate the degree of Si isotopic fractionation that takes place during magmatic differentiation. Here we report Si isotopic compositions of lavas from Hekla volcano, Iceland, which has formed in a region devoid of old, geochemically diverse crust. We show that Si isotopic composition varies linearly as a function of silica content, with more differentiated rocks possessing heavier isotopic compositions. Data for samples from the Afar Rift Zone, as well as various igneous USGS standards are collinear with the Hekla trend, providing evidence of a fundamental relationship between magmatic differentiation and Si isotopes. The effect of fractionation has been tested by studying cumulates from the Skaergaard Complex, which show that olivine and pyroxene are isotopically light, and plagioclase heavy, relative to the Si isotopic composition of the Earth's mantle. Therefore, Si isotopes can be utilised to model the competing effects of mafic and felsic mineral fractionation in evolving silicate liquids and cumulates. At an average SiO 2 content of ˜60 wt.%, the predicted δ 30Si value of the continental crust that should result from magmatic fractionation alone is -0.23 ± 0.05‰ (2 s.e.), barely heavier than the mantle. This is, at most, a maximum estimate, as this does not take into account weathered material whose formation drives the products toward lighter δ 30Si values. Mass balance calculations suggest that removal of continental crust of this composition from the upper mantle will not affect the Si isotopic composition of the mantle.

  10. Exploring the isotopic niche: isotopic variance, physiological incorporation, and the temporal dynamics of foraging

    Justin Douglas Yeakel

    2016-01-01

    Full Text Available Consumer foraging behaviors are dynamic, changing in response to prey availability, seasonality, competition, and even the consumer's physiological state. The isotopic composition of a consumer is a product of these factors as well as the isotopic `landscape' of its prey, i.e. the isotopic mixing space. Stable isotope mixing models are used to back-calculate the most likely proportional contribution of a set of prey to a consumer's diet based on their respective isotopic distributions, however they are disconnected from ecological process. Here we build a mechanistic framework that links the ecological and physiological processes of an individual consumer to the isotopic distribution that describes its diet, and ultimately to the isotopic composition of its own tissues, defined as its `isotopic niche’. By coupling these processes, we systematically investigate under what conditions the isotopic niche of a consumer changes as a function of both the geometric properties of its mixing space and foraging strategies that may be static or dynamic over time. Results of our derivations reveal general insight into the conditions impacting isotopic niche width as a function of consumer specialization on prey, as well as the consumer's ability to transition between diets over time. We show analytically that moderate specialization on isotopically unique prey can serve to maximize a consumer's isotopic niche width, while temporally dynamic diets will tend to result in peak isotopic variance during dietary transitions. We demonstrate the relevance of our theoretical findings by examining a marine system composed of nine invertebrate species commonly consumed by sea otters. In general, our analytical framework highlights the complex interplay of mixing space geometry and consumer dietary behavior in driving expansion and contraction of the isotopic niche. Because this approach is established on ecological mechanism, it is well-suited for enhancing the

  11. Stable isotope utilization methodology; Methodologie de l`emploi des isotopes stables

    Roth, E. [Conservatoire National des Arts et Metiers (CNAM), 75 - Paris (France)

    1994-12-31

    The various applications of stable isotope utilization are reviewed, as a function of their specific properties: poly-isotopic abundance modification is used for tracer applications; the accurate measurement of the stable isotope abundance may be applied to isotopic dilution for ultra-trace measurement, physical constant determination, fluid volume and concentration measurement; isotopic effects, such as reaction equilibrium differences are used for separation and identification of molecule active centers (pharmacology, paleoclimatology, hydrogeological studies) while reaction rate differences (competitive and non competitive methods) are used for the study of reaction mechanisms, such as enzymatic reactions. Analysis techniques (mass spectrometry, nuclear magnetic resonance, optical methods) are reviewed. 2 figs., 18 refs.

  12. ISOTOPES

    1996-01-01

    1 A New Therapeutic Agent for Radiation Synovectomy: Preparation of 166Ho-EDTMP-HA Bai Hongsheng Jin Xiaohai Du Jin Wang Fan Chen Daming Fan Hongqiang Cheng Zhen In order to treat the patient with inflammatory synovial disease, HA particle is labeled with 166Ho by EDTMP under the condition of pH6.0-8.0 and vibration time 15 min, its labeling efficiency is more than 98%, the size of particle is mainly in the range of 2-5 μm. The absorbed capacity is 5 mg Ho per 1g HA. Study on stability of 166Ho-EDTMP-HA in vitro shows that loss of 166Ho is less than 2% for166Ho-EDTMP-HA incubated 72 h in the 0.9% saline and 1% BSA solution at 37 ℃ .Biodistribution in vivo and extra articular leakage are investigated following injection of 166Ho-EDTMP-HA into knee of normal rabbits. The experimental results show that the extra leakage of 166Ho-EDTMP-HA is 0.32% at 48 h post-injection, most of 166Ho radioactivity leaked from the knee joint is excreted in the urine. 99% of 166Ho radioactivity is retained in the knee joint of rabbits. Thereby 166Ho-EDTMP-HA, as a new therapeutical agent of radiation synovectomy, had a value of further clinical study.

  13. Isotope Program Report June FY2016

    Lewis, Jr, Benjamin E. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Egle, Brian [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2016-09-01

    Isotope Program Monthly Highlights are briefly described. These include data on isotopes shipped, updates on equipment fabrication and testing, a potential new approach for nondestructive measurement of the amount of Cf-252 deposited on a surface, and efforts to recover and purify uranium-234 obtained from old PuBe sources.

  14. Advanced Mass Spectrometers for Hydrogen Isotope Analyses

    Chastagner, P.

    2001-08-01

    This report is a summary of the results of a joint Savannah River Laboratory (SRL) - Savannah River Plant (SRP) ''Hydrogen Isotope Mass Spectrometer Evaluation Program''. The program was undertaken to evaluate two prototype hydrogen isotope mass spectrometers and obtain sufficient data to permit SRP personnel to specify the mass spectrometers to replace obsolete instruments.

  15. Applications of stable isotopes in clinical pharmacology

    Schellekens, Reinout C A; Stellaard, Frans; Woerdenbag, Herman J; Frijlink, Henderik W; Kosterink, Jos G W

    2011-01-01

    This review aims to present an overview of the application of stable isotope technology in clinical pharmacology. Three main categories of stable isotope technology can be distinguished in clinical pharmacology. Firstly, it is applied in the assessment of drug pharmacology to determine the pharmacok

  16. Magnesium isotope geochemistry in arc volcanism

    Teng, Fang-Zhen; Hu, Yan; Chauvel, Catherine

    2016-06-01

    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ26Mg of the Martinique Island lavas varies from -0.25 to -0.10, in contrast to the narrow range that characterizes the mantle (-0.25 ± 0.04, 2 SD). These high δ26Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid-mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration.

  17. Magnesium isotope geochemistry in arc volcanism.

    Teng, Fang-Zhen; Hu, Yan; Chauvel, Catherine

    2016-06-28

    Incorporation of subducted slab in arc volcanism plays an important role in producing the geochemical and isotopic variations in arc lavas. The mechanism and process by which the slab materials are incorporated, however, are still uncertain. Here, we report, to our knowledge, the first set of Mg isotopic data for a suite of arc lava samples from Martinique Island in the Lesser Antilles arc, which displays one of the most extreme geochemical and isotopic ranges, although the origin of this variability is still highly debated. We find the δ(26)Mg of the Martinique Island lavas varies from -0.25 to -0.10, in contrast to the narrow range that characterizes the mantle (-0.25 ± 0.04, 2 SD). These high δ(26)Mg values suggest the incorporation of isotopically heavy Mg from the subducted slab. The large contrast in MgO content between peridotite, basalt, and sediment makes direct mixing between sediment and peridotite, or assimilation by arc crust sediment, unlikely to be the main mechanism to modify Mg isotopes. Instead, the heavy Mg isotopic signature of the Martinique arc lavas requires that the overall composition of the mantle wedge is buffered and modified by the preferential addition of heavy Mg isotopes from fluids released from the altered subducted slab during fluid-mantle interaction. This, in turn, suggests transfer of a large amount of fluid-mobile elements from the subducting slab to the mantle wedge and makes Mg isotopes an excellent tracer of deep fluid migration.

  18. The isotopic dipole moment of HDO

    Assafrao, Denise; Mohallem, Jose R [Laboratorio de Atomos e Moleculas Especiais, Departamento de Fisica, ICEx, Universidade Federal de Minas Gerais, CP 702, 30123-970, Belo Horizonte, MG (Brazil)

    2007-03-14

    An adiabatic variational approximation is used to study the monodeuterated water molecule, HDO, accounting for the isotopic effect. The isotopic dipole moment, pointing from D to H, is then calculated for the first time, yielding (1.5 {+-} 0.1) x 10{sup -3} Debye, being helpful in the interpretation of experiments. (fast track communication)

  19. Atomic lithium vapor laser isotope separation

    Olivares, I E

    2002-01-01

    An atomic vapor laser isotope separation in lithium was performed using tunable diode lasers. The method permits also the separation of the isotopes between the sup 6 LiD sub 2 and the sup 7 LiD sub 1 lines using a self-made mass separator which includes a magnetic sector and an ion beam designed for lithium. (Author)

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

    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.

  1. Activation of Alveolar Macrophages after Plutonium Oxide Inhalation in Rats: Involvement in the Early Inflammatory Response

    Van der Meeren, A.; Tourdes, F.; Gremy, O.; Grillon, G.; Abram, M.C.; Poncy, J.L.; Griffiths, N. [CEA, DSV, DRR, SRCA, Centre DAM Ile de France, F-91297 Bruyeres Le Chatel, Arpajon (France)

    2008-07-01

    Alveolar macrophages play an important role in the distribution, clearance and inflammatory reactions after particle inhalation, which may influence long-term events such as fibrosis and tumorigenesis. The objectives of the present study were to investigate the early inflammatory events after plutonium oxide inhalation in rats and involvement of alveolar macrophages. Lung changes were studied from 3 days to 3 months after inhalation of PuO{sub 2} or different isotopic compositions (70% or 97% {sup 239}Pu) and initial lung deposits (range 2.1 to 43.4 kBq/rat). Analyses of bronchoalveolar lavages showed early increases in the numbers of granulocytes, lymphocytes and multi-nucleated macrophages. The activation of macrophages was evaluated ex vivo by measurement of inflammatory mediator levels in culture supernatants. TNF-alpha and chemokine MCP-1, MIP-2 and CINC-1 production was elevated from 7 days after inhalation and remained so up to 3 months. In contrast, IL-1 beta, IL-6 and IL-10 production was unchanged. At 6 weeks, pulmonary macrophage numbers and activation state were increased as observed from an immunohistochemistry study of lung sections with anti-ED1. Similarly, histological analyses of lung sections also showed evidence of inflammatory responses. In conclusion, our results indicate early inflammatory changes in the lungs of PuO{sub 2}-contaminated animals and the involvement of macrophages in this process. A dose-effect relationship was observed between the amount of radionuclide inhaled or retained at the time of analysis and inflammatory mediator production by alveolar macrophages 14 days after exposure. For similar initial lung deposits, the inflammatory manifestation appears higher for 97% {sup 239}Pu than for 70% {sup 239}Pu. (authors)

  2. Second international conference on isotopes. Conference proceedings

    Hardy, C.J. [ed.

    1997-10-01

    The Second International Conference on Isotopes (2ICI) was hosted by the Australian Nuclear Association in Sydney, NSW, Australia. The Theme of the Second Conference: Isotopes for Industry, Health and a Better Environment recognizes that isotopes have been used in these fields successfully for many years and offer prospects for increasing use in the future. The worldwide interest in the use of research reactors and accelerators and in applications of stable and radioactive isotopes, isotopic techniques and radiation in industry, agriculture, medicine, environmental studies and research in general, was considered. Other radiation issues including radiation protection and safety were also addressed. International and national overviews and subject reviews invited from leading experts were included to introduce the program of technical sessions. The invited papers were supported by contributions accepted from participants for oral and poster presentation. A Technical Exhibition was held in association with the Conference. This volume contains the full text or extended abstracts of papers number 61- to number 114

  3. Manus Water Isotope Investigation Field Campaign Report

    Conroy, Jessica L [University of Illinois, Urbana-Champaign; Cobb, Kim M [Georgia Institute of Technology; Noone, David [University of Colorado, Boulder

    2016-03-01

    The objective of this field campaign was to investigate climatic controls on the stable isotopic composition of water vapor, precipitation, and seawater in the western tropical Pacific. Simultaneous measurements of the stable isotopic composition of vapor and precipitation from April 28 to May 8, 2013, at the Manus Tropical Western Pacific Atmospheric Radiation Measurement site, provided several key insights into the nature of the climate signal archived in precipitation and vapor isotope ratios. We observed a large shift from lower to higher isotopic values in vapor and precipitation because of the passage of a mesoscale convective system west of the site and a transition from a regional stormy period into a more quiescent period. During the quiescent period, the stable isotopic composition of vapor and precipitation indicated the predominance of oceanic evaporation in determining the isotopic composition of boundary-layer vapor and local precipitation. There was not a consistent relationship between intra-event precipitation amount at the site and the stable isotopic composition of precipitation, thus challenging simplified assumptions about the isotopic “amount effect” in the tropics on the time scale of individual storms. However, some storms did show an amount effect, and deuterium excess values in precipitation had a significant relationship with several meteorological variables, including precipitation, temperature, relative humidity, and cloud base height across all measured storms. The direction of these relationships points to condensation controls on precipitation deuterium excess values on intra-event time scales. The relationship between simultaneous measurements of vapor and precipitation isotope ratios during precipitation events indicates the ratio of precipitation-to-vapor isotope ratios can diagnose precipitation originating from a vapor source unique from boundary-layer vapor and rain re-evaporation.

  4. Lead Isotopes in Highway Runoff

    Ferreira, M.; Lau, S.; Green, P. G.; Stenstrom, M. K.

    2011-12-01

    Lead (Pb) isotopes have been used extensively to study the provenance of lead pollution on air, water, and sediments. In this study, we measured Pb isotopes and Pb aqueous concentration in highway runoff in three west Los Angeles sites. Those three sites, part of a long-term study sponsored by the California Department of Transportation, represent small catchment areas, and host heavy traffic. In addition, there were no inputs of sand or salt to the highway because the sites are almost completely impervious and also due to the lack of snow to be controlled. Highway runoff from the three sites was collected for 7 storms during the 2004-2005 Winter. Grab samples were collected every 15 minutes during the first hour, and hourly afterwards. A total of 202 samples were collected and filtered into five size fractions (100μm). Aqueous concentration of Pb range from 0.08μg/L to 46.95μg/L (7.98±10.89μg/L) and it is not correlated with any of the lead isotope ratios. The 208Pb/206Pb ratio ranges from 1.983 to 2.075 (2.024±0.026) and there is no statistical difference for the mean value of the 208Pb/206Pb ratio for the four particulate size fractions (0.45-8μm, 8-20μm, 20-100μm, >100μm). However, the 208Pb/206Pb ratio of nearby soils yield 2.060±0.021 and it is statistically different from the ratios obtained for the highway runoff. This hints that the lead present in highway runoff does not come from local soils. The 207Pb/206Pb ratio ranges from 0.804 to 0.847 (0.827±0.011) and there is no statistical difference for the mean value of the 207Pb/206Pb ratio for the four particulate size fractions (0.45-8μm, 8-20μm, 20-100μm, >100μm). Surprisingly, there is also no statistical difference with the 207Pb/206Pb ratio of nearby soils (0.833±0.009).

  5. Chromium isotope uptake in carbonates

    Rodler, Alexandra

    composition of contemporaneous seawater. Marine carbonates are ubiquitous throughout Earth’s rock record rendering them a particularly interesting archive for constraining past changes in ocean chemistry. This thesis includes an investigation of the fractionation behavior of Cr isotopesduring coprecipitation......Chromium (Cr) is a redox sensitive element potentially capable of tracing fine-scale fluctuations of the oxygenation of Earth’s early surface environments and seawater. The Cr isotope composition of carbonates could perhaps be used as paleo-redox proxy to elucidate changes in the geological past...... related to the rise of oxygen and the evolution of the biosphere. However, before the Cr isotopesystem can be applied to faithfully delineate paleo-environmental changes, careful assessment of the signal robustness and a thorough understanding of the Cr cycle in Earth system processes is necessary...

  6. Measurement of isotope abundance variations in nature by gravimetric spiking isotope dilution analysis (GS-IDA).

    Chew, Gina; Walczyk, Thomas

    2013-04-02

    Subtle variations in the isotopic composition of elements carry unique information about physical and chemical processes in nature and are now exploited widely in diverse areas of research. Reliable measurement of natural isotope abundance variations is among the biggest challenges in inorganic mass spectrometry as they are highly sensitive to methodological bias. For decades, double spiking of the sample with a mix of two stable isotopes has been considered the reference technique for measuring such variations both by multicollector-inductively coupled plasma mass spectrometry (MC-ICPMS) and multicollector-thermal ionization mass spectrometry (MC-TIMS). However, this technique can only be applied to elements having at least four stable isotopes. Here we present a novel approach that requires measurement of three isotope signals only and which is more robust than the conventional double spiking technique. This became possible by gravimetric mixing of the sample with an isotopic spike in different proportions and by applying principles of isotope dilution for data analysis (GS-IDA). The potential and principle use of the technique is demonstrated for Mg in human urine using MC-TIMS for isotopic analysis. Mg is an element inaccessible to double spiking methods as it consists of three stable isotopes only and shows great potential for metabolically induced isotope effects waiting to be explored.

  7. ORNL Resolved Resonance Covariance Generation for ENDF/B-VII.1

    Leal, L.; Guber, K.; Wiarda, D.; Arbanas, G.; Derrien, H.; Sayer, R.; Larson, N.; Dunn, M.

    2012-12-01

    Resonance-parameter covariance matrix (RPCM) evaluations in the resolved resonance regionwere done at the Oak Ridge National Laboratory (ORNL) for the chromium isotopes, titanium isotopes, 19F, 58Ni, 60Ni, 35Cl, 37Cl, 39K, 41K, 55Mn, 233U, 235U, 238U, and 239Pu using the computer code SAMMY. The retroactive approach of the code SAMMY was used to generate the RPCMs for 233U. For 235U, the approach used for covariance generation was similar to the retroactive approach with the distinction that real experimental data were used as opposed to data generated from the resonance parameters. RPCMs for 238U and 239Pu were generated together with the resonance parameter evaluations. The RPCMs were then converted in the ENDF format using the FILE32 representation. Alternatively, for computer storage reasons, the FILE32 was converted in the FILE33 cross section covariance matrix (CSCM). Both representations were processed using the computer code PUFF-IV. This paper describes the procedures used to generate the RPCM and CSCM in the resonance region for ENDF/B-VII.1. The impact of data uncertainty in nuclear reactor benchmark calculations is also presented.

  8. Uranium-series constraints on radionuclide transport and groundwater flow at the Nopal I uranium deposit, Sierra Pena Blanca, Mexico.

    Goldstein, Steven J; Abdel-Fattah, Amr I; Murrell, Michael T; Dobson, Patrick F; Norman, Deborah E; Amato, Ronald S; Nunn, Andrew J

    2010-03-01

    Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ( approximately 10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that (230)Th/(238)U activity ratios range from 0.005 to 0.48 and (226)Ra/(238)U activity ratios range from 0.006 to 113. (239)Pu/(238)U mass ratios for the saturated zone are 1000 times lower than the U mobility. Saturated zone mobility decreases in the order (238)U approximately (226)Ra > (230)Th approximately (239)Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.

  9. Uranium-series constraints on radionuclide transport and groundwater flow at the Nopal I uranium deposit, Sierra Pena Blanca, Mexico

    Goldstein, S.J.; Abdel-Fattah, A.I.; Murrell, M.T.; Dobson, P.F.; Norman, D.E.; Amato, R.S.; Nunn, A. J.

    2009-10-01

    Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ({approx}10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that {sup 230}Th/{sup 238}U activity ratios range from 0.005-0.48 and {sup 226}Ra/{sup 238}U activity ratios range from 0.006-113. {sup 239}Pu/{sup 238}U mass ratios for the saturated zone are <2 x 10{sup -14}, and Pu mobility in the saturated zone is >1000 times lower than the U mobility. Saturated zone mobility decreases in the order {sup 238}U{approx}{sup 226}Ra > {sup 230}Th{approx}{sup 239}Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.

  10. The isotope effect: Prediction, discussion, and discovery

    Kragh, Helge

    2011-01-01

    The precise position of a spectral line emitted by an atomic system depends on the mass of the atomic nucleus and is therefore different for isotopes belonging to the same element. The possible presence of an isotope effect followed from Bohr's atomic theory of 1913, but it took several years before it was confirmed experimentally. Its early history involves the childhood not only of the quantum atom, but also of the concept of isotopy. Bohr's prediction of the isotope effect was apparently at odds with early attempts to distinguish between isotopes by means of their optical spectra. However, in 1920 the effect was discovered in HCl molecules, which gave rise to a fruitful development in molecular spectroscopy. The first detection of an atomic isotope effect was no less important, as it was by this means that the heavy hydrogen isotope deuterium was discovered in 1932. The early development of isotope spectroscopy illustrates the complex relationship between theory and experiment, and is also instructive with...

  11. Compound specific isotope analysis of organophosphorus pesticides.

    Wu, Langping; Yao, Jun; Trebse, Polonca; Zhang, Ning; Richnow, Hans H

    2014-09-01

    Compound-specific isotope analysis (CSIA) has been established as a tool to study the environmental fate of a wide range of contaminants. In this study, CSIA was developed to analyse the stable carbon isotope signatures of the widely used organophosphorus pesticides: dichlorvos, omethoate and dimethoate. The linearity of the GC-C-IRMS system was tested for target pesticides and led to an acceptable isotope composition within the uncertainty of the instrument. In order to assess the accuracy of the developed method, the effect of the evaporation procedure on measured carbon isotope composition (δ(13)C) values was studied and showed that concentration by evaporation of solvents had no significant isotope effect. The CSIA was then applied to investigate isotope fractionation of the hydrolysis and photolysis of selected pesticides. The carbon isotope fractionation of tested pesticides was quantified by the Rayleigh model, which revealed a bulk enrichment factor (ε) of -0.2±0.1‰ for hydrolysis of dichlorvos, -1.0±0.1‰ and -3.7±1.1‰ for hydrolysis and photolysis of dimethoate respectively. This study is a first step towards the application of CSIA to trace the transport and degradation of organophosphorus pesticides in the environment.

  12. Si isotope homogeneity of the solar nebula

    Pringle, Emily A.; Savage, Paul S.; Moynier, Frédéric [Department of Earth and Planetary Sciences and McDonnell Center for the Space Sciences, Washington University in St. Louis, One Brookings Drive, St. Louis, MO 63130 (United States); Jackson, Matthew G. [Department of Earth Science, University of California, Santa Barbara, CA 93109 (United States); Barrat, Jean-Alix, E-mail: eapringle@wustl.edu, E-mail: savage@levee.wustl.edu, E-mail: pringle@ipgp.fr, E-mail: moynier@ipgp.fr, E-mail: jackson@geol.ucsb.edu, E-mail: Jean-Alix.Barrat@univ-brest.fr [Université Européenne de Bretagne, Université de Brest, CNRS UMR 6538 (Domaines Océaniques), I.U.E.M., Place Nicolas Copernic, F-29280 Plouzané Cedex (France)

    2013-12-20

    The presence or absence of variations in the mass-independent abundances of Si isotopes in bulk meteorites provides important clues concerning the evolution of the early solar system. No Si isotopic anomalies have been found within the level of analytical precision of 15 ppm in {sup 29}Si/{sup 28}Si across a wide range of inner solar system materials, including terrestrial basalts, chondrites, and achondrites. A possible exception is the angrites, which may exhibit small excesses of {sup 29}Si. However, the general absence of anomalies suggests that primitive meteorites and differentiated planetesimals formed in a reservoir that was isotopically homogenous with respect to Si. Furthermore, the lack of resolvable anomalies in the calcium-aluminum-rich inclusion measured here suggests that any nucleosynthetic anomalies in Si isotopes were erased through mixing in the solar nebula prior to the formation of refractory solids. The homogeneity exhibited by Si isotopes may have implications for the distribution of Mg isotopes in the solar nebula. Based on supernova nucleosynthetic yield calculations, the expected magnitude of heavy-isotope overabundance is larger for Si than for Mg, suggesting that any potential Mg heterogeneity, if present, exists below the 15 ppm level.

  13. Stable isotopic characterisation of francolite formation

    McArthur, J. M.; Benmore, R. A.; Coleman, M. L.; Soldi, C.; Yeh, H.-W.; O'Brien, G. W.

    1986-02-01

    Stable isotopic data are presented for 112 samples of francolite from 18 separate phosphate deposits. Values of δ 13C and δ 34S in most offshore deposits suggest formation within oxic or suboxic environments either by carbonate replacement or direct precipitation of francolite from water of normal marine compositions. The exceptions are concretionary francolite from Namibia, which has an isotopic composition in keeping with its formation within organic-rich sediments, and that from offshore Morocco, which has an isotopic signature of the anoxic/suboxic interface. Onshore deposits from Jordan, Mexico, South Africa and, possibly, the Permian Phosphoria Formation in the western U.S.A., are substantially depleted in 18O: they appear to be too altered for deductions to be made about their environments of formation. In other onshore deposits which are unaltered, or minimally altered, the isotopic composition suggests that some formed within sulphate-reducing sediments (Sedhura, Morocco) whilst francolite from the Georgina Basin of Australia formed at the oxic/anoxic boundary, where oxidation of biogenic H 2S decreases the δ 34S of pore water. In general, pelletal samples show non-oxic isotopic signatures, whilst non-pelletal samples show oxic isotopic signatures, but samples from Namibia, Peru (Ica Plateau) and the Californian and Moroccan margins are exceptions to this rule. Morphology may therefore be a misleading indicator of francolite genesis as no definitive relation exists between phosphorite type and isotopic signature.

  14. Beneficial uses and production of isotopes

    2001-01-01

    Isotopes, radioactive and stable, are used worldwide in various applications related to medical diagnosis or care, industry and scientific research. More than fifty countries have isotope production or separation facilities operated for domestic supply, and sometimes for international markets. This publication provides up-to-date information on the current status of, and trends in, isotope uses and production. It also presents key issues, conclusions and recommendations, which will be of interest to policy makers in governmental bodies, scientists and industrial actors in the field.

  15. The Facility for Rare Isotope Beams

    Wrede C.

    2015-01-01

    Full Text Available The Facility for Rare Isotope Beams (FRIB is a United States Department of Energy user facility currently under construction on the campus of Michigan State University. Based on a 400 kW, 200 MeV/u heavy-ion driver linac, FRIB will deliver high-quality fast, thermalized, and re-accelerated beams of rare isotopes with unprecedented intensities to a variety of experimental areas and equipment. New science opportunities at the frontiers of nuclear structure, nuclear astrophysics, fundamental symmetries, and societal applications will be enabled by this future world-leading rare-isotope beam facility.

  16. The Facility for Rare Isotope Beams

    Wrede, C.

    2015-05-01

    The Facility for Rare Isotope Beams (FRIB) is a United States Department of Energy user facility currently under construction on the campus of Michigan State University. Based on a 400 kW, 200 MeV/u heavy-ion driver linac, FRIB will deliver high-quality fast, thermalized, and re-accelerated beams of rare isotopes with unprecedented intensities to a variety of experimental areas and equipment. New science opportunities at the frontiers of nuclear structure, nuclear astrophysics, fundamental symmetries, and societal applications will be enabled by this future world-leading rare-isotope beam facility.

  17. Isotopic Fractionation of Selenium Oxyanions in Wetlands

    Clark, S. K.; Johnson, T. M.

    2004-05-01

    As oxic surface waters pass through aquatic macrophytes and over anoxic sediments in wetlands and lakes, the dissolved Se load often decreases; and, Se isotope ratio measurements can provide information about the mechanisms involved. Previous work on microbially induced isotopic fractionation of Se oxyanions under nearly natural conditions using wetland sediments shows consistent Se isotopic shifts during reduction of Se(VI) and Se(IV) to insoluble Se(0). However, previous isotopic studies of total dissolved selenium in wetlands found little to no isotopic shift as dissolved selenium concentrations decreased. This suggests that plant/algal uptake, followed by deposition and degradation, is the primary route of Se transfer into sediments. However, it is possible that the effective isotopic fractionation between Se in the surface water and Se deposited into sediments is somehow much less than the fractionation induced by the reduction reaction, or that cycling of organically bound Se is involved. In this study, we report Se isotope data for Se(VI), Se(IV) and total dissolved Se, Se(T), in surface waters from three wetland/lake sites: Sweitzer Lake, CO; 33-Mile Reservoir, WY; and, a small pond adjacent to Benton Lake, MT. We isolated Se(IV) via hydride generation, and Se(VI) via ion exchange. Se(T), including any organic components, was also analyzed. Isotope analysis was performed on an Isoprobe MC-ICPMS, using a method modified from that of Rouxel et al. (2002). We used the 82Se + 74Se double spike approach, and spiked samples before species separation. Our results for all three locations indicate similar trends in concentration changes and isotopic shifts between the inflow and outflow waters. Se(T) concentrations decrease by 45-70%, and Se(VI) concentrations decrease by 60-90%, whereas Se(IV) concentrations increase by 60-150%. Concomitant 80Se/76Se shifts are +0.5-0.8‰ for Se(T); -0.1-0.5‰ for Se(VI); and +0.4-6.5‰ for Se(IV). These data provide greater

  18. Isotope effects of hafnium in solvent extraction using crown ethers

    Fujii, Toshiyuki; Moriyama, Hirotake [Research Reactor Institute, Kyoto University, Osaka (Japan); Hirata, Takafumi [Laboratory for Planetary Sciences, Tokyo Institute of Technology, Tokyo (Japan); Nishizawa, Kazushige [Department of Nuclear Engineering, Graduate School of Engineering, Osaka University, Osaka (Japan)

    2001-06-01

    Hafnium isotopes were fractionated in a liquid-liquid extraction system by using seven types of crown ethers, tributyl phosphate, or {omicron}-diethoxybenzene. The largest isotope effect was observed in the isotope pair of {sup 177}Hf-{sup 179}Hf with dibenzo-24-crown-8; the isotope enrichment factor was observed to be 0.0129{+-}0.0032. (author)

  19. Environmental geochemistry of calcium isotopes: Applications of a new stable isotope approach

    LIU Zhanmin; LIU Congqiang; HAN Guilin; WANG Zhongliang; XUE Zichen; SONG Zhaoliang; YANG Cheng

    2006-01-01

    This paper summarizes isotope fractionation mechanism, analytical method and applications in environmental geochemistry of calcium isotopes. Calcium isotopic composition can be used to constrain material sources and study geological and environmental processes as the isotopic composition of calcium (δ 44Ca) and fractionation processes depend on geochemical circumstances in nature. Recently, thanks to current advances in analytical technology of calcium isotopes, calcium isotopes are broadly used in biological and geochemical studies, such as the mechanism of plants imbibing nutrients through their roots, calcium transport in the environmental ecosystem, calcium cycle in oceans and paleo-oceans and paleo-climate. The elementary data show that δ44Ca values vary from -2.88‰ to 0.92‰ in natural samples.

  20. Newtonian kinetic isotope effects. Observation, prediction, and origin of heavy-atom dynamic isotope effects.

    Kelly, Kelmara K; Hirschi, Jennifer S; Singleton, Daniel A

    2009-06-24

    Intramolecular (13)C kinetic isotope effects were determined for the dimerization of cyclopentadiene. Substantial isotope effects were observed in three positions, despite the C(2) symmetry of the cycloaddition transition state and the absence of dynamical bottlenecks after this transition state. The observed isotope effects were predicted well from trajectory studies by extrapolating the outcomes of trajectories incorporating superheavy isotopes of carbon, ranging from (20)C to (140)C. Trajectory studies suggest that the isotope effects are unrelated to zero-point energy or the geometrical and momentum properties of the transition state. However, steepest-descent paths in mass-weighted coordinates correctly predict the direction of the isotope effects, supporting a novel origin in Newton's second law of motion.

  1. Isotope effects on desorption kinetics of hydrogen isotopes implanted into stainless steel by glow discharge

    Matsuyama, M.; Kondo, M.; Noda, N. [Hydrogen Isotope Research Center, University of Toyama, Gofuku, Toyama (Japan); Tanaka, M.; Nishimura, K. [National Institute for Fusion Science, Toki-shi, Gifu (Japan)

    2015-03-15

    In a fusion device the control of fuel particles implies to know the desorption rate of hydrogen isotopes by the plasma-facing materials. In this paper desorption kinetics of hydrogen isotopes implanted into type 316L stainless steel by glow discharge have been studied by experiment and numerical calculation. The temperature of a maximum desorption rate depends on glow discharge time and heating rate. Desorption spectra observed under various experimental conditions have been successfully reproduced by numerical simulations that are based on a diffusion-limited process. It is suggested, therefore, that desorption rate of a hydrogen isotope implanted into the stainless steel is limited by a diffusion process of hydrogen isotope atoms in bulk. Furthermore, small isotope effects were observed for the diffusion process of hydrogen isotope atoms. (authors)

  2. Short course on St-02 applications of isotope dilutions and isotopic measurements

    Miller, P.

    1998-01-05

    This short course includes information on these topics and subtopics: (I) Nuclear Properties: (A) Historic roots; (B) Nomenclature; (C) Nuclear Stability and abundance; (D) Uses of isotopic techniques; (II) Instrumentation: (A) Sources; (B) Mass resolving elements; (C) Detectors; (III) Making Isotopic Measurements by ICP-MS: (A) Deadtime Correction; (B) Mass Discrimination; (C) Signal /Noise considerations; (IV) Applications and examples: (A) Isotope dilution; (B) Double Spike; (C) Biological Application; (D) Environmental Application; (E) Geological.

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

    Irrgeher, Johanna; Zitek, Andreas; Prohaska, Thomas

    2014-05-01

    During the last decade stable isotope tracers have emerged as versatile tool in ecological research. Besides 'intrinsic' isotope tracers caused by the natural variation of isotopes, the intentional introduction of 'extrinsic' enriched stable isotope tracers into biological systems has gained significant interest. Hereby the induced change in the natural isotopic composition of an element allows amongst others for studying the fate and fluxes of metals, trace elements and species in organisms or provides an intrinsic marker or tag of particular biological samples. Due to the shoreless potential of this methodology, the number of publications dealing with applications of isotope (double) spikes as tracers to address research questions in 'real world systems' is constantly increasing. However, some isotope systems like the natural Sr isotopic system, although potentially very powerful for this type of application, are still rarely used, mainly because their adequate measurement/determination poses major analytical challenges; as e.g. Sr is available in significant amounts in natural samples. In addition, biological systems underlie complex processes such as metabolism, adsorption/desorption or oxidation/reduction. As a consequence, classic evaluation approaches such as the isotope dilution mass spectrometry equation are often not applicable because of the unknown amount of tracer finally present in the sample. Isotope pattern deconvolution (IPD), based on multiple linear regression, serves as simplified alternative data processing strategy to double spike isotope dilution calculations. The outstanding advantage of this mathematical tool lies in the possibility of deconvolving the isotope pattern in a spiked sample without knowing the quantities of enriched isotope tracer being incorporated into the natural sample matrix as well as the degree of impurities and species-interconversion (e.g. from sample preparation). Here, the potential of IPD for environmental tracer

  4. Stable isotope production with laser techniques; Production d`isotopes stables a l`aide des techniques laser

    Petit, A. [CEA Centre d`Etudes de Saclay, 91 - Gif-sur-Yvette (France). Dept. des Procedes d`Enrichissement

    1994-12-31

    Laser properties may be used for stable isotope production either by selective photoionization of an atom particular isotope, either by selective photodissociation of a molecule. Principles of both processes are reviewed and examples of calcium 43 isotope separation through photoionization and of carbon and oxygen isotope separation by photodissociation are presented. 4 figs., 1 tab., 11 refs.

  5. Beam delivery for stable isotope separation

    Forbes, Andrew; Strydom, Hendrick J.; Botha, Lourens R.; Ronander, Einar

    2002-10-01

    In the multi-photon dissociation process of Carbon isotope enrichment, IR photons are used to selectively excite a molecule with the given isotopic base element. This enrichment process is very sensitive to the beam's intensity and wavelength. Because the intensity is determined by the propagation of the field, the enrichment factors are also very dependent on the field propagation. In this paper, the influence of the wavelength and intensity of the beam, on the isotope selective dissociation of a CFC compound is investigated both experimentally and theoretically. Consideration is also given to some of the factors that influence the delivery of various beams to the reactor chamber, and their subsequent propagation through the reactor. The results show that suitable beam forming can lead to an improved isotope separation process.

  6. On the progress in stable isotope separation

    Prusakov, V.N. [Kurchatov Institute, Moscow (Russian Federation)

    1994-12-31

    The principles and process of centrifuge isotope separation are reviewed; the fundamental advantage of the centrifuge over gaseous diffusion arises from the fact that the primary isotope separation effect occurs at thermodynamic equilibrium; thus, gas centrifuge enrichment uses only about 1/20 to 1/30 of the electricity per SWU (separation work unit) consumed by gaseous diffusion. The various substances that can be used in centrifuge isotope separation are listed (fluorides, oxyfluorides, {pi}-complexes, boron hydrides, metal-organic compounds, halides...). The centrifuge method productivity is much greater than with the electromagnetic separation technique; examples of centrifuge stable and radioactive isotope separation are given; the method of the residue reduction is also presented with the example of separating radioactive krypton-85 out of a nuclear reactor krypton blend. 4 figs.

  7. Stable Oxygen-18 and Deuterium Isotopes

    Müller, Sascha

    development within a given lowland headwater catchment (stream water isotopes). Based on our investigations on the precipitation isotopic composition a local meteoric water line (LMWL) was constructed and expressed as: δ2H=7.4 δ18O + 5.36‰. Moreover, we showed that under maritime temperature climate influence......, humidity is the main driver for the temporal and spatial isotopic development and temperature plays only a secondary role. Based on our investigations at a coastal lagoon aquifer we could improve quantifications of seasonal saltwater-wedge dynamics, based on isotopic tracers combined with salinity. We can...... link the observed seasonal regression/transgression pattern to the inland recharge cycle, which is expressed in hydraulic head configuration and submarine groundwater discharge rates at the fieldsite. Nonetheless, those observed dynamics could not be simulated due to numerical limitations. By the use...

  8. Development of proliferation resistant isotope separation technology

    Jeong, Doyoung; Ko, Kwanghoon; Kim, Taeksoo; Park, Hyunmin; Lim, Gwon; Cha, Yongho; Han, Jaemin; Baik, Sunghoon; Cha, Hyungki

    2012-02-15

    This project was accomplished with an aim of establishing the industrial facilities for isotope separation in Korea. The experiment for the measurement of neutrino mass that has been an issue in physics, needs very much of enriched calcium-48 isotope. However, calcium-48 isotope can be produced only by the electro-magnetic method and, thus, its price is very expensive. Therefore, we expect that ALSIS can replace the electro-magnetic method for calcium-48 isotope production. In this research stage, the research was advanced systematically with core technologies, such as atomic vapor production, the measurement of vapor characteristics and stable and powerful laser development. These researches will be the basis of the next research stages. In addition, the international research trends and cooperation results are reported in this report.

  9. Isotope effects of hydrogen and atom tunnelling

    Buchachenko, A. L.; Pliss, E. M.

    2016-06-01

    The abnormally high mass-dependent isotope effects in liquid-phase hydrogen (deuterium) atom transfer reactions, which are customarily regarded as quantum effects, are actually the products of two classical effects, namely, kinetic and thermodynamic ones. The former is determined by the rate constants for atom transfer and the latter is caused by nonbonded (or noncovalent) isotope effects in the solvation of protiated and deuterated reacting molecules. This product can mimic the large isotope effects that are usually attributed to tunnelling. In enzymatic reactions, tunnelling is of particular interest; its existence characterizes an enzyme as a rigid molecular machine in which the residence time of reactants on the reaction coordinate exceeds the waiting time for the tunnelling event. The magnitude of isotope effect becomes a characteristic parameter of the internal dynamics of the enzyme catalytic site. The bibliography includes 61 references.

  10. Quantification of isotopic turnover in agricultural systems

    Braun, A.; Auerswald, K.; Schnyder, H.

    2012-04-01

    The isotopic turnover, which is a proxy for the metabolic rate, is gaining scientific importance. It is quantified for an increasing range of organisms, from microorganisms over plants to animals including agricultural livestock. Additionally, the isotopic turnover is analyzed on different scales, from organs to organisms to ecosystems and even to the biosphere. In particular, the quantification of the isotopic turnover of specific tissues within the same organism, e.g. organs like liver and muscle and products like milk and faeces, has brought new insights to improve understanding of nutrient cycles and fluxes, respectively. Thus, the knowledge of isotopic turnover is important in many areas, including physiology, e.g. milk synthesis, ecology, e.g. soil retention time of water, and medical science, e.g. cancer diagnosis. So far, the isotopic turnover is quantified by applying time, cost and expertise intensive tracer experiments. Usually, this comprises two isotopic equilibration periods. A first equilibration period with a constant isotopic input signal is followed by a second equilibration period with a distinct constant isotopic input signal. This yields a smooth signal change from the first to the second signal in the object under consideration. This approach reveals at least three major problems. (i) The input signals must be controlled isotopically, which is almost impossible in many realistic cases like free ranging animals. (ii) Both equilibration periods may be very long, especially when the turnover rate of the object under consideration is very slow, which aggravates the first problem. (iii) The detection of small or slow pools is improved by large isotopic signal changes, but large isotopic changes also involve a considerable change in the input material; e.g. animal studies are usually carried out as diet-switch experiments, where the diet is switched between C3 and C4 plants, since C3 and C4 plants differ strongly in their isotopic signal. The

  11. The production of stable isotopes in Spain

    Urgel, M.; Iglesias, J.; Casas, J.; Saviron, J. M.; Quintanilla, M.

    1965-07-01

    The activities developed in the field of the production of stable isotopes by means of ion-exchange chromatography and thermal diffusion techniques are reported. The first method was used to study the separation of the nitrogen and boron isotopes, whereby the separation factor was determined by the break through method. Values ranging from 1,028 to 1,022 were obtained for the separation factor of nitrogen by using ammonium hydroxide solutions while the corresponding values as obtained for boron amounted to 1,035-1,027 using boric acid solutions. Using ammonium chloride or acetate and sodium borate, respectively, resulted in the obtention of values for the separation factor approaching unity. The isotopic separation has been carried out according to the method of development by displacement. The separation of the isotopes of the noble gases, oxygen, nitrogen and carbon has been accomplished resorting to the method of thermal diffusion. (Author) 16 refs.

  12. Use of fluorescent screens for isotope radiography

    Hubbard, S. K.

    1979-01-01

    Radiographic examination can be performed on items beyond the limitation of conventional isotope radiography without a great loss of resolution. With proper film and screen selection and scatter radiation control, fluorescent screens can be a valuable additional tool for radiography.

  13. Carbon isotopic fractionation in heterotrophic microbial metabolism

    Blair, N.; Leu, A.; Munoz, E.; Olsen, J.; Kwong, E.; Des Marais, D.

    1985-01-01

    Differences in the natural-abundance carbon stable isotopic compositions between products from aerobic cultures of Escherichia coli K-12 were measured. Respired CO2 was 3.4 percent depleted in C-13 relative to the glucose used as the carbon source, whereas the acetate was 12.3 percent enriched in C-13. The acetate C-13 enrichment was