Measuring soil moisture near soil surface...minor differences due to neutron source type

Treesearch

Robert R. Ziemer; Irving Goldberg; Norman A. MacGillivray

1967-01-01

Moisture measurements were made in three media?paraffin, water, saturated sand?with four neutron miusture meters, each containing 226-radium-beryllium, 227-actinium-beryllium, 238-plutonium-beryllium, or 241-americium-beryllium neutron sources. Variability in surface detection by the different sources may be due to differences in neutron sources, in length of source,...

Measuring soil moisture near soil surface ... minor differences due to neutron source type

Treesearch

Robert R. Ziemer; Irving Goldberg; Norman A. MacGillivray

1967-01-01

Abstract - Moisture measurements were made in three media--paraffin, water, saturated sand--with four neutron moisture meters, each containing 226-radium-beryllium, 227-actinium-beryllium, 239-plutonium-beryllium, or 241-americium-beryllium neutron sources. Variability in surface detection by the different sources may be due to differences in neutron sources, in...

Large Scale Accelerator Production of 225Ac: Effective Cross sections for 78-192 MeV Protons Incident on 232Th Targets

DOE PAGES

Griswold, Justin R; Medvedev, Dmitri G.; Engle, Jonathan W.; ...

2016-09-28

Actinium-225 and 213Bi have been used successfully in targeted alpha therapy (TAT) in preclinical and clinical research. This paper is a continuation of research activities aiming to expand the availability of 225Ac. The high energy proton spallation reaction on natural thorium metal target has been utilized to produce millicurie quantities of 225Ac. The results of sixteen irradiation experiments of Th metal at beam energies between 78 and 200 MeV are summarized in this work. Irradiations have been conducted at Brookhaven National Laboratory (BNL) and Los Alamos National Laboratory (LANL), while target dissolution and processing was carried out at Oak Ridgemore » National Laboratory (ORNL). Excitation functions for actinium and thorium isotopes as well as for some of the fission products are presented. The cross sections for production of 225Ac range from 3.6 to 16.7 mb in the incident proton energy range of 78 to 192 MeV. Based on these data, production of Curie quantities of 225Ac is possible by irradiating a 5.0 g cm -2232Th target for 10 days in either BNL or LANL proton irradiation facilities.« less

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

PubMed

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

2016-12-01

Actinium-225 and 213 Bi have been used successfully in targeted alpha therapy (TAT) in preclinical and clinical research. This paper is a continuation of research activities aiming to expand the availability of 225 Ac. The high-energy proton spallation reaction on natural thorium metal targets has been utilized to produce millicurie quantities of 225 Ac. The results of sixteen irradiation experiments of thorium metal at beam energies between 78 and 192MeV are summarized in this work. Irradiations have been conducted at Brookhaven National Laboratory (BNL) and Los Alamos National Laboratory (LANL), while target dissolution and processing was carried out at Oak Ridge National Laboratory (ORNL). Excitation functions for actinium and thorium isotopes, as well as for some of the fission products, are presented. The cross sections for production of 225 Ac range from 3.6 to 16.7mb in the incident proton energy range of 78-192MeV. Based on these data, production of curie quantities of 225 Ac is possible by irradiating a 5.0gcm -2 232 Th target for 10 days in either BNL or LANL proton irradiation facilities. Copyright © 2016 Elsevier Ltd. All rights reserved.

Shape of intrinsic alpha pulse height spectra in lanthanide halide scintillators

NASA Astrophysics Data System (ADS)

Wolszczak, W.; Dorenbos, P.

2017-06-01

Internal contamination with actinium-227 and its daughters is a serious drawback in low-background applications of lanthanide-based scintillators. In this work we showed the important role of nuclear γ de-excitations on the shape of the internal alpha spectrum measured in scintillators. We calculated with Bateman equations the activities of contamination isotopes and the time evolution of actinium-227 and its progenies. Next, we measured the intrinsic background spectra of LaBr3(Ce), LaBr3(Ce,Sr) and CeBr3 with a digital spectroscopy technique, and we analyzed them with a pulse shape discrimination method (PSD) and a time-amplitude analysis. Finally, we simulated the α background spectrum with Geant4 tool-kit, consequently taking into account complex α-γ-electron events, the α / β ratio dependence on the α energy, and the electron/γ nonproportionality. We found that α-γ mixed events have higher light yield than expected for alpha particles alone, which leads to overestimation of the α / β ratio when it is measured with internal 227Th and 223Ra isotopes. The time-amplitude analysis showed that the α peaks of 219Rn and 215Po in LaBr3(Ce) and LaBr3(Ce,Sr) are not symmetric. We compared the simulation results with the measured data and provided further evidence of the important role of mixed α-γ-electron events for understanding the shape of the internal α spectrum in scintillators.

METHOD OF MAKING ALLOYS OF BERYLLIUM WITH PLUTONIUM AND THE LIKE

DOEpatents

Runnals, O.J.C.

1959-02-24

The production of alloys of beryllium with one or more of the metals uranium, plutonium, actinium, americium, curium, thorium, and cerium are described. A halide salt of the metal to be alloyed with the beryllium is heated at 1300 deg C in the presence of beryllium to reduce the halide to metal and cause the latter to alloy directly with the beryllium. Although the heavy metal halides are more stable, thermodynamically, than the beryllium halides, the reducing reaction proceeds to completion if the beryllium halide product is continuously removed by vacuum distillation.

Systematization of actinides using cluster analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kopyrin, A.A.; Terent`eva, T.N.; Khramov, N.N.

1994-11-01

A representation of the actinides in multidimensional property space is proposed for systematization of these elements using cluster analysis. Literature data for their atomic properties are used. Owing to the wide variation of published ionization potentials, medians are used to estimate them. Vertical dendograms are used for classification on the basis of distances between the actinides in atomic-property space. The properties of actinium and lawrencium are furthest removed from the main group. Thorium and mendelevium exhibit individualized properties. A cluster based on the einsteinium-fermium pair is joined by californium.

An overview of targeted alpha therapy with 225Actinium and 213Bismuth.

PubMed

Morgenstern, Alfred; Apostolidis, Christos; Kratochwil, Clemens; Sathekge, Mike; Krolicki, Leszek; Bruchertseifer, Frank

2018-05-01

Recent reports of the remarkable therapeutic efficacy of 225Ac-labeled PSMA-617 for therapy of metastatic castration-resistant prostate cancer have underlined the clinical potential of targeted alpha therapy. This review describes methods for the production of 225Ac and its daughter nuclide 213Bi and summarizes the current clinical experience with both alpha emitters with particular focus on recent studies of targeted alpha therapy of bladder cancer, brain tumors, neuroendocrine tumors and prostate cancer. Copyright© Bentham Science Publishers; For any queries, please email at epub@benthamscience.org.

Method of making alloys of beryllium with plutonium and the like

DOEpatents

Runnals, O J.C.

1959-02-24

The production or alloys of beryllium with one or more of the metals uranium, plutonium, actinium, americium, curium, thorium, and cerium is described. A halide salt or the metal to be alloyed with the beryllium is heated at l3O0 deg C in the presence of beryllium to reduce the halide to metal and cause the latter to alloy directly with the beryllium. Although the heavy metal halides are more stable, thermodynamically, than the beryllium halides, the reducing reaction proceeds to completion if the beryllium halide product is continuously removed by vacuum distillation.

A Radium-223 Microgenerator from Cyclotron-Produced Trace Actinium-227

PubMed Central

Abou, Diane S.; Pickett, Juile; Mattson, John E.; Thorek, Daniel L. J.

2016-01-01

The alpha particle emitter Radium-223 dichloride (223RaCl2) has recently been approved for treatment of late-stage bone metastatic prostate cancer. There is considerable interest in studying this new agent outside of the clinical setting, however the supply of 223Ra is limited and expensive. We have engineered a 223Ra microgenerator using traces of 227Ac previously generated from cyclotron-produced 225Ac. Radiochemically pure 223RaCl2 was made, characterized, evaluated in vivo, and the source was recovered in high yield for regeneration of the microgenerator. PMID:27835737

Fission of actinide nuclei using multi-nucleon transfer reactions

NASA Astrophysics Data System (ADS)

Léguillon, Romain; Nishio, Katsuhisa; Hirose, Kentaro; Orlandi, Riccardo; Makii, Hiroyuki; Nishinaka, Ichiro; Ishii, Tetsuro; Tsukada, Kazuaki; Asai, Masato; Chiba, Satoshi; Ohtsuki, Tsutomu; Araki, Shohei; Watanabe, Yukinobu; Tatsuzawa, Ryotaro; Takaki, Naoyuki

2014-09-01

We are promoting a campaign to measure fission-fragment mass distributions for neutron-rich actinide nuclei populated by transfer reactions from their ground state up to an excitation energy of several tens MeV. We thus obtain the excitation energy dependence of the mass distribution. The experiment was carried out at the 20 MV JAEA tandem facility at Tokai. We report on the data obtained in the direct reaction 18 O + 232 Th . Transfer-channels and excitation energies of the fissioning nuclei were identified using silicon dE-E detectors located at forward angle. Two fission fragments were detected in coincidence using multi-wire proportional counters. Fission fragment masses were determined by kinematic consideration. We obtained the fission fragment mass distributions for 13 nuclei from actinium to uranium and some fission barrier heights. We are promoting a campaign to measure fission-fragment mass distributions for neutron-rich actinide nuclei populated by transfer reactions from their ground state up to an excitation energy of several tens MeV. We thus obtain the excitation energy dependence of the mass distribution. The experiment was carried out at the 20 MV JAEA tandem facility at Tokai. We report on the data obtained in the direct reaction 18 O + 232 Th . Transfer-channels and excitation energies of the fissioning nuclei were identified using silicon dE-E detectors located at forward angle. Two fission fragments were detected in coincidence using multi-wire proportional counters. Fission fragment masses were determined by kinematic consideration. We obtained the fission fragment mass distributions for 13 nuclei from actinium to uranium and some fission barrier heights. Present study is supported by the Ministry of Education, Culture, Sports, Science and Technology of Japan.

CATIONIC EXCHANGE PROCESS FOR THE SEPARATION OF RARE EARTHS

DOEpatents

Choppin, G.R.; Thompson, S.G.; Harvey, B.G.

1960-02-16

A process for separating mixtures of elements in the lanthanum and actinium series of the periodic table is described. The mixture of elements is dissolved in 0.05 M HCI, wherein the elements exist as tripositive ions. The resulting solution is then transferred to a column of cationic exchange resin and the column eluted with 0.1 to 0.6 M aqueous ammonium alpha hydroxy isobutyrate solution of pH 3.8 to 5.0. The use of ammonium alpha hydroxy isobutyrate as an eluting agent results in sharper and more rapid separations than previously obtainable with eluants such as citric, tartaric, glycolic, and lactic acids.

Reflection asymmetry in odd-A and odd-odd actinium nuclei

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ahmad, I.

1993-09-01

Theoretical calculations and measurements indicate that octupole correlations are at a maximum in the ground states of the odd-proton nuclei Ac and Pa. It has been expected that odd-odd nuclei should have even larger amount of octupole-octupole correlations. We have recently made measurements on the structure of {sup 224}Ac. Although spin and parity assignments could not be made, two bands starting at 354.1 and 360.0 keV have properties characteristic of reflection asymmetric shape. These two bands have very similar rotational constants and also similar alpha decay rates, which suggest similarity between the wavefunctions of these bands. These signatures provide evidencemore » for octupole correlations in these nuclides.« less

Simultaneous Separation of Actinium and Radium Isotopes from a Proton Irradiated Thorium Matrix

DOE PAGES

Mastren, Tara; Radchenko, Valery; Owens, Allison; ...

2017-08-15

A new method has been developed for the isolation of 223,224,225Ra, in high yield and purity, from a proton irradiated 232Th matrix. We report an all-aqueous process using multiple solid-supported adsorption steps including a citrate chelation method developed to remove >99.9% of the barium contaminants by activity from the final radium product. Moreover, we developed a procedure involving the use of three columns in succession, and the separation of 223,224,225Ra from the thorium matrix was obtained with an overall recovery yield of 91 ± 3%, average radiochemical purity of 99.9%, and production yields that correspond to physical yields based onmore » previously measured excitation functions.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mesick, Katherine Elizabeth; Coupland, Daniel David S.; Stonehill, Laura Catherine

Cs 2LiLaBr 6:Ce 3+ (CLLB) is an elpasolite scintillator that offers excellent linearity and gamma-ray energy resolution and sensitivity to thermal neutrons with the ability to perform pulse-shape discrimination (PSD) to distinguish gammas and neutrons. Our investigation of CLLB has indicated the presence of intrinsic radioactive alpha background that we have determined to be from actinium contamination of the lanthanum component. We measured the pulse shapes for gamma, thermal neutron, and alpha events and determined that PSD can be performed to separate the alpha background with a moderate figure of merit of 0.98. Here, we also measured the electron-equivalent-energy ofmore » the alpha particles in CLLB and simulated the intrinsic alpha background from 227Ac to determine the quenching factor of the alphas.« less

The discovery of radioactivity

NASA Astrophysics Data System (ADS)

Radvanyi, Pierre; Villain, Jacques

2017-11-01

The radioactivity of uranium was discovered in 1896 by Henri Becquerel who, starting from a wrong idea, progressively realized what he was observing, regularly informing the French Academy of Sciences of the progress he was doing. In the next years, it was found that thorium was radioactive too, and two new radioactive elements, polonium and radium, were discovered by Pierre and Marie Curie, while a third one, actinium, was identified by André Debierne. The study of the penetrating power and of the effect of electric and magnetic fields allowed scientists to demonstrate the complexity of nuclear radiation with its three components α, β, γ. The Comptes rendus de l'Académie des sciences allow the reader to see how difficult it was to understand the nature of radioactivity, which was essentially elucidated by Ernest Rutherford and Frederick Soddy.

Towards high-resolution laser ionization spectroscopy of the heaviest elements in supersonic gas jet expansion

PubMed Central

Ferrer, R.; Barzakh, A.; Bastin, B.; Beerwerth, R.; Block, M.; Creemers, P.; Grawe, H.; de Groote, R.; Delahaye, P.; Fléchard, X.; Franchoo, S.; Fritzsche, S.; Gaffney, L. P.; Ghys, L.; Gins, W.; Granados, C.; Heinke, R.; Hijazi, L.; Huyse, M.; Kron, T.; Kudryavtsev, Yu.; Laatiaoui, M.; Lecesne, N.; Loiselet, M.; Lutton, F.; Moore, I. D.; Martínez, Y.; Mogilevskiy, E.; Naubereit, P.; Piot, J.; Raeder, S.; Rothe, S.; Savajols, H.; Sels, S.; Sonnenschein, V.; Thomas, J-C; Traykov, E.; Van Beveren, C.; Van den Bergh, P.; Van Duppen, P.; Wendt, K.; Zadvornaya, A.

2017-01-01

Resonant laser ionization and spectroscopy are widely used techniques at radioactive ion beam facilities to produce pure beams of exotic nuclei and measure the shape, size, spin and electromagnetic multipole moments of these nuclei. However, in such measurements it is difficult to combine a high efficiency with a high spectral resolution. Here we demonstrate the on-line application of atomic laser ionization spectroscopy in a supersonic gas jet, a technique suited for high-precision studies of the ground- and isomeric-state properties of nuclei located at the extremes of stability. The technique is characterized in a measurement on actinium isotopes around the N=126 neutron shell closure. A significant improvement in the spectral resolution by more than one order of magnitude is achieved in these experiments without loss in efficiency. PMID:28224987

METHOD FOR THE RECOVERY AND PURIFICATION OF BERKELIUM

DOEpatents

Hulet, E.K.

1959-10-20

A solvent extraction process is described for the separation of berkelium from a mixture of elements in the lanthanum and actinium series of the periodic table. In particular, the mixture of elements is dissolved in 1.0N nitric acid, and the resulting solution is extracted with n-tributyl phosphate containlng a stoichiometric excess of solid sodium bismuthate. The berkelium present in the nitric acid solution is oxidized to the IV oxidation state and is preferentially- extracted into the n-tributyl phosphate. The organic phase, containing berkelium in an oxidized state, is extracted with 0.1N hydrochloric acid solution containing a small quantity- of a reducing agent such as yvdrazine hydrochloride. The berkelium is reduced to the III oxidation state and is extracted into the aqueous phase. The berkelium is then recovered from the aqueous phase.

Process for radioisotope recovery and system for implementing same

DOEpatents

Meikrantz, David H [Idaho Falls, ID; Todd, Terry A [Aberdeen, ID; Tranter, Troy J [Idaho Falls, ID; Horwitz, E Philip [Naperville, IL

2009-10-06

A method of recovering daughter isotopes from a radioisotope mixture. The method comprises providing a radioisotope mixture solution comprising at least one parent isotope. The at least one parent isotope is extracted into an organic phase, which comprises an extractant and a solvent. The organic phase is substantially continuously contacted with an aqueous phase to extract at least one daughter isotope into the aqueous phase. The aqueous phase is separated from the organic phase, such as by using an annular centrifugal contactor. The at least one daughter isotope is purified from the aqueous phase, such as by ion exchange chromatography or extraction chromatography. The at least one daughter isotope may include actinium-225, radium-225, bismuth-213, or mixtures thereof. A liquid-liquid extraction system for recovering at least one daughter isotope from a source material is also disclosed.

Process for radioisotope recovery and system for implementing same

DOEpatents

Meikrantz, David H.; Todd, Terry A.; Tranter, Troy J.; Horwitz, E. Philip

2007-01-02

A method of recovering daughter isotopes from a radioisotope mixture. The method comprises providing a radioisotope mixture solution comprising at least one parent isotope. The at least one parent isotope is extracted into an organic phase, which comprises an extractant and a solvent. The organic phase is substantially continuously contacted with an aqueous phase to extract at least one daughter isotope into the aqueous phase. The aqueous phase is separated from the organic phase, such as by using an annular centrifugal contactor. The at least one daughter isotope is purified from the aqueous phase, such as by ion exchange chromatography or extraction chromatography. The at least one daughter isotope may include actinium-225, radium-225, bismuth-213, or mixtures thereof. A liquid-liquid extraction system for recovering at least one daughter isotope from a source material is also disclosed.

New mass anchor points for neutron-deficient heavy nuclei from direct mass measurements of radium and actinium isotopes

NASA Astrophysics Data System (ADS)

Rosenbusch, M.; Ito, Y.; Schury, P.; Wada, M.; Kaji, D.; Morimoto, K.; Haba, H.; Kimura, S.; Koura, H.; MacCormick, M.; Miyatake, H.; Moon, J. Y.; Morita, K.; Murray, I.; Niwase, T.; Ozawa, A.; Reponen, M.; Takamine, A.; Tanaka, T.; Wollnik, H.

2018-06-01

The masses of the exotic isotopes Ac-214210 and Ra-214210 have been measured with a multireflection time-of-flight mass spectrograph. These isotopes were obtained in flight as fusion-evaporation products behind the gas-filled recoil ion separator GARIS-II at RIKEN. The new direct mass measurements serve as an independent and direct benchmark for existing α -γ spectroscopy data in this mass region. Further, new mass anchor points are set for U and Np nuclei close to the N =126 shell closure for a future benchmark of the Z =92 subshell for neutron-deficient heavy isotopes. Our mass results are in general in good agreement with the previously indirectly determined mass values. Together with the measurement data, reasons for possible mass ambiguities from decay-data links between ground states are discussed.

Pulse-shape discrimination and energy quenching of alpha particles in Cs 2LiLaBr 6:Ce 3+

DOE PAGES

Mesick, Katherine Elizabeth; Coupland, Daniel David S.; Stonehill, Laura Catherine

2016-10-19

Cs 2LiLaBr 6:Ce 3+ (CLLB) is an elpasolite scintillator that offers excellent linearity and gamma-ray energy resolution and sensitivity to thermal neutrons with the ability to perform pulse-shape discrimination (PSD) to distinguish gammas and neutrons. Our investigation of CLLB has indicated the presence of intrinsic radioactive alpha background that we have determined to be from actinium contamination of the lanthanum component. We measured the pulse shapes for gamma, thermal neutron, and alpha events and determined that PSD can be performed to separate the alpha background with a moderate figure of merit of 0.98. Here, we also measured the electron-equivalent-energy ofmore » the alpha particles in CLLB and simulated the intrinsic alpha background from 227Ac to determine the quenching factor of the alphas.« less

Development of ion beam sputtering techniques for actinide target preparation

NASA Astrophysics Data System (ADS)

Aaron, W. S.; Zevenbergen, L. A.; Adair, H. L.

1985-06-01

Ion beam sputtering is a routine method for the preparation of thin films used as targets because it allows the use of a minimum quantity of starting material, and losses are much lower than most other vacuum deposition techniques. Work is underway in the Isotope Research Materials Laboratory (IRML) at ORNL to develop the techniques that will make the preparation of actinide targets up to 100 μg/cm 2 by ion beam sputtering a routinely available service from IRML. The preparation of the actinide material in a form suitable for sputtering is a key to this technique, as is designing a sputtering system that allows the flexibility required for custom-ordered target production. At present, development work is being conducted on low-activity actinides in a bench-top system. The system will then be installed in a hood or glove box approved for radioactive materials handling where processing of radium, actinium, and plutonium isotopes among others will be performed.

Background radiation and individual dosimetry in the costal area of Tamil Nadu, India.

PubMed

Matsuda, Naoki; Brahmanandhan, G M; Yoshida, Masahiro; Takamura, Noboru; Suyama, Akihiko; Koguchi, Yasuhiro; Juto, Norimichi; Raj, Y Lenin; Winsley, Godwin; Selvasekarapandian, S

2011-07-01

South coast of India is known as the high-level background radiation area (HBRA) mainly due to beach sands that contain natural radionuclides as components of the mineral monazite. The rich deposit of monazite is unevenly distributed along the coastal belt of Tamil Nadu and Kerala. An HBRA site that laid in 2×7 m along the sea was found in the beach of Chinnavillai, Tamil Nadu, where the maximum ambient dose equivalent reached as high as 162.7 mSv y(-1). From the sands collected at the HBRA spot, the high-purity germanium semi-conductor detector identified six nuclides of thorium series, four nuclides of uranium series and two nuclides belonging to actinium series. The highest radioactivity observed was 43.7 Bq g(-1) of Th-228. The individual dose of five inhabitants in Chinnavillai, as measured by the radiophotoluminescence glass dosimetry system, demonstrated the average dose of 7.17 mSv y(-1) ranging from 2.79 to 14.17 mSv y(-1).

Tumor Immunotargeting Using Innovative Radionuclides

PubMed Central

Kraeber-Bodéré, Françoise; Rousseau, Caroline; Bodet-Milin, Caroline; Mathieu, Cédric; Guérard, François; Frampas, Eric; Carlier, Thomas; Chouin, Nicolas; Haddad, Ferid; Chatal, Jean-François; Faivre-Chauvet, Alain; Chérel, Michel; Barbet, Jacques

2015-01-01

This paper reviews some aspects and recent developments in the use of antibodies to target radionuclides for tumor imaging and therapy. While radiolabeled antibodies have been considered for many years in this context, only a few have reached the level of routine clinical use. However, alternative radionuclides, with more appropriate physical properties, such as lutetium-177 or copper-67, as well as alpha-emitting radionuclides, including astatine-211, bismuth-213, actinium-225, and others are currently reviving hopes in cancer treatments, both in hematological diseases and solid tumors. At the same time, PET imaging, with short-lived radionuclides, such as gallium-68, fluorine-18 or copper-64, or long half-life ones, particularly iodine-124 and zirconium-89 now offers new perspectives in immuno-specific phenotype tumor imaging. New antibody analogues and pretargeting strategies have also considerably improved the performances of tumor immunotargeting and completely renewed the interest in these approaches for imaging and therapy by providing theranostics, companion diagnostics and news tools to make personalized medicine a reality. PMID:25679452

Nuclear Data Evaluation for Mass Chain A=217:Odd-Proton Nuclei

PubMed Central

Nafee, Sherif S.; Shaheen, Salem A.; Al-Ramady, Amir M.

2016-01-01

Thallium (Tl81217), Bismuth (Bi83217), Astatine (At85217), Francium (Fr87217), Actinium (Ac89217) and Protactinium (Pa91217) are of odd-proton numbers among the mass chain A = 217. In the present work, the half-lives and gamma transitions for the six nuclei have been studied and adopted based on the recently published interactions or unevaluated nuclear data sets XUNDL. The Q (α) has been updated based on the recent published work of the Atomic Mass Evaluation AME2012 as well. Moreover, the total conversion electrons as well as the K-Shell to L-Shell, L-Shell to M-Shell and L-Shell to N-Shell Conversion Electron Ratios have been calculated using BrIcc code v2.3. An updated skeleton decay scheme for each of the above nuclei has been presented here. The decay hindrance factors (HF) calculated using the ALPHAD program, which is available from Brookhaven National Laboratory’s website, have been calculated for the α- decay data sets for 221Fr-, 221Ac- and 221Pa- α-decays. PMID:26761207

DOE Office of Scientific and Technical Information (OSTI.GOV)

Douglas, Matthew; Bernacki, Bruce E.; Erchinger, Jennifer L.

Liquid scintillation counting (LSC) is a versatile and commonplace method for radiometric measurement of charged particle emitting radionuclides. The LSC method provides utility in a range of environmental science applications including hydrological studies of water transport, anthropogenic releases of radionuclides into the environment, and vertical mixing rates within oceans. Instrumental measurement background is one limiting factor of radiometric measurement sensitivity. As part of the development of a custom low background LSC system located in a shallow underground laboratory at Pacific Northwest National Laboratory, a number of measurement applications of LSC have been considered and are summarized here. The focus ismore » on determining which aspects of such measurements would gain the greatest benefit from the reduction of LSC backgrounds by a factor of 10-100 relative to values reported in the literature. Examples of benefits include lowering the minimum detectable activity, reducing the sample size required, and shortening the elapsed timeline of the processing and analysis sequence. In particular tritium, strontium, and actinium isotopes are examined as these isotopes cover a range of requirements related to the LSC measurement method (e.g., 3H: low energy; Sr: spectral deconvolution; Ac: alpha/beta discrimination).« less

Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins.

PubMed

Mastren, Tara; Stein, Benjamin W; Parker, T Gannon; Radchenko, Valery; Copping, Roy; Owens, Allison; Wyant, Lance E; Brugh, Mark; Kozimor, Stosh A; Nortier, F Meiring; Birnbaum, Eva R; John, Kevin D; Fassbender, Michael E

2018-06-05

Protactinium-230 ( t 1/2 = 17.4 d) is the parent isotope of 230 U ( t 1/2 = 20.8 d), a radionuclide of interest for targeted alpha therapy (TAT). Column chromatographic methods have been developed to separate no-carrier-added 230 Pa from proton irradiated thorium targets and accompanying fission products. Results reported within demonstrate the use of novel sulfur bearing chromatographic extraction resins for the selective separation of protactinium. The recovery yield of 230 Pa was 93 ± 4% employing a R 3 P═S type commercially available resin and 88 ± 4% employing a DGTA (diglycothioamide) containing custom synthesized extraction chromatographic resin. The radiochemical purity of the recovered 230 Pa was measured via high purity germanium γ-ray spectroscopy to be >99.5% with the remaining radioactive contaminant being 95 Nb due to its similar chemistry to protactinium. Measured equilibrium distribution coefficients for protactinium, thorium, uranium, niobium, radium, and actinium on both the R 3 P═S type and the DGTA resin in hydrochloric acid media are reported, to the best of our knowledge, for the first time.

Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins

DOE PAGES

Mastren, Tara; Stein, Benjamin W.; Parker, T. Gannon; ...

2018-05-14

Protactinium-230 (t 1/2 = 17.4 d) is the parent isotope of 230U (t 1/2 = 20.8 d), a radionuclide of interest for targeted alpha therapy (TAT). Column chromatographic methods have been developed to separate no-carrier-added 230Pa from proton irradiated thorium targets and accompanying fission products. Results reported within this paper demonstrate the use of novel sulfur bearing chromatographic extraction resins for the selective separation of protactinium. The recovery yield of 230Pa was 93 ± 4% employing a R 3P=S type commercially available resin and 88 ± 4% employing a DGTA (diglycothioamide) containing custom synthesized extraction chromatographic resin. The radiochemical puritymore » of the recovered 230Pa was measured via high purity germanium γ-ray spectroscopy to be >99.5% with the remaining radioactive contaminant being 95Nb due to its similar chemistry to protactinium. Finally, measured equilibrium distribution coefficients for protactinium, thorium, uranium, niobium, radium, and actinium on both the R 3P=S type and the DGTA resin in hydrochloric acid media are reported, to the best of our knowledge, for the first time.« less

Pulse-shape discrimination and energy quenching of alpha particles in Cs2LiLaBr6:Ce3+

NASA Astrophysics Data System (ADS)

Mesick, K. E.; Coupland, D. D. S.; Stonehill, L. C.

2017-01-01

Cs2LiLaBr6:Ce3+(CLLB) is an elpasolite scintillator that offers excellent linearity and gamma-ray energy resolution and sensitivity to thermal neutrons with the ability to perform pulse-shape discrimination (PSD) to distinguish gammas and neutrons. Our investigation of CLLB has indicated the presence of intrinsic radioactive alpha background that we have determined to be from actinium contamination of the lanthanum component. We measured the pulse shapes for gamma, thermal neutron, and alpha events and determined that PSD can be performed to separate the alpha background with a moderate figure of merit of 0.98. We also measured the electron-equivalent-energy of the alpha particles in CLLB and simulated the intrinsic alpha background from 227Ac to determine the quenching factor of the alphas. A linear quenching relationship Lα =Eα × q +L0 was found at alpha particle energies above 5 MeV, with a quenching factor q = 0.71 MeVee / MeV and an offset L0 = - 1.19 MeVee .

Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mastren, Tara; Stein, Benjamin W.; Parker, T. Gannon

Protactinium-230 (t 1/2 = 17.4 d) is the parent isotope of 230U (t 1/2 = 20.8 d), a radionuclide of interest for targeted alpha therapy (TAT). Column chromatographic methods have been developed to separate no-carrier-added 230Pa from proton irradiated thorium targets and accompanying fission products. Results reported within this paper demonstrate the use of novel sulfur bearing chromatographic extraction resins for the selective separation of protactinium. The recovery yield of 230Pa was 93 ± 4% employing a R 3P=S type commercially available resin and 88 ± 4% employing a DGTA (diglycothioamide) containing custom synthesized extraction chromatographic resin. The radiochemical puritymore » of the recovered 230Pa was measured via high purity germanium γ-ray spectroscopy to be >99.5% with the remaining radioactive contaminant being 95Nb due to its similar chemistry to protactinium. Finally, measured equilibrium distribution coefficients for protactinium, thorium, uranium, niobium, radium, and actinium on both the R 3P=S type and the DGTA resin in hydrochloric acid media are reported, to the best of our knowledge, for the first time.« less

Purification of lanthanides for double beta decay experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Polischuk, O. G.; Barabash, A. S.; Belli, P.

2013-08-08

There are several potentially double beta active isotopes among the lanthanide elements. However, even high purity grade lanthanide compounds contain {sup 238}U, {sup 226}Ra and {sup 232,228}Th typically on the level of ∼ (0.1 - 1) Bq/kg. The liquid-liquid extraction technique was used to remove traces of U, Ra and Th from CeO{sub 2}, Nd{sub 2}O{sub 3} and Gd{sub 2}O{sub 3}. The radioactive contamination of the samples before and after the purification was tested by using ultra-low-background HPGe γ spectrometry at the underground Gran Sasso National Laboratories of the INFN (Italy). After the purification the radioactive contamination of gadolinium oxidemore » by Ra and Th was decreased at least one order of magnitude. The efficiency of the approach to purify cerium oxide from Ra was on same level, while the radioactive contamination of neodymium sample before and after the purification is below the sensitivity of analytical methods. The purification method is much less efficient for chemically very similar radioactive elements like lanthanum, lutetium and actinium. R and D of the methods to remove the pollutions with improved efficiency is in progress.« less

Development of an Ultra-Low Background Liquid Scintillation Counter for Trace Level Analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Erchinger, Jennifer L.; Orrell, John L.; Aalseth, Craig E.

2015-09-01

Low-level liquid scintillation counting (LSC) has been established as one of the radiation detection techniques useful in elucidating environmental processes and environmental monitoring around nuclear facilities. The Ultra-Low Background Liquid Scintillation Counter (ULB-LSC) under construction in the Shallow Underground Laboratory at Pacific Northwest National Laboratory aims to further reduce the MDAs and/or required sample processing. Through layers of passive shielding in conjunction with an active veto and 30 meters water equivalent overburden, the background reduction is expected to be 10 to 100 times below typical analytic low-background liquid scintillation systems. Simulations have shown an expected background of around 14 countsmore » per day. A novel approach to the light collection will use a coated hollow light guide cut into the inner copper shielding. Demonstration LSC measurements will show low-energy detection, spectral deconvolution, and alpha/beta discrimination capabilities, from trials with standards of tritium, strontium-90, and actinium-227, respectively. An overview of the system design and expected demonstration measurements will emphasize the potential applications of the ULB-LSC in environmental monitoring for treaty verification, reach-back sample analysis, and facility inspections.« less

Review of Gallium-68 PSMA PET/CT Imaging in the Management of Prostate Cancer

PubMed Central

Lenzo, Nat P.; Meyrick, Danielle; Turner, J. Harvey

2018-01-01

Over 90% of prostate cancers over-express prostate specific membrane antigen (PSMA) and these tumor cells may be accurately targeted for diagnosis by 68Ga-PSMA-positron emission tomography/computed tomography (68Ga-PSMA-PET/CT) imaging. This novel molecular imaging modality appears clinically to have superseded CT, and appears superior to MR imaging, for the detection of metastatic disease. 68Ga-PSMA PET/CT has the ability to reliably stage prostate cancer at presentation and can help inform an optimal treatment approach. Novel diagnostic applications of 68Ga-PSMA PET/CT include guiding biopsy to improve sampling accuracy, and guiding surgery and radiotherapy. In addition to facilitating the management of metastatic castrate resistant prostate cancer (mCRPC), 68Ga-PSMA can select patients who may benefit from targeted systemic radionuclide therapy. 68Ga-PSMA is the diagnostic positron-emitting theranostic pair with the beta emitter Lutetium-177 PSMA (177Lu-PSMA) and alpha-emitter Actinium-225 PSMA (225Ac-PSMA) which can both be used to treat PSMA-avid metastases of prostate cancer in the molecular tumor-targeted approach of theranostic nuclear oncology. PMID:29439481

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jaggi, Jaspreet Singh; Seshan, Surya V.; McDevitt, Michael R.

Purpose: Internal irradiation of kidneys as a consequence of radioimmunotherapy, radiation accidents, or nuclear terrorism can result in radiation nephropathy. We attempted to modify pharmacologically, the functional and morphologic changes in mouse kidneys after injection with the actinium ({sup 225}Ac) nanogenerator, an in vivo generator of {alpha}- and {beta}-particle emitting elements. Methods and Materials: The animals were injected with 0.35 {mu}Ci of the {sup 225}Ac nanogenerator, which delivers a dose of 27.6 Gy to the kidneys. Then, they were randomized to receive captopril (angiotensin-converting enzyme inhibitor), L-158,809 (angiotensin II receptor-1 blocker), spironolactone (aldosterone receptor antagonist), or a placebo. Results: Fortymore » weeks after the {sup 225}Ac injection, the placebo-control mice showed a significant increase in blood urea nitrogen (BUN) (87.6 {+-} 6.9 mg/dL), dilated Bowman spaces, and tubulolysis with basement membrane thickening. Captopril treatment accentuated the functional (BUN 119.0 {+-} 4.0 mg/dL; p <0.01 vs. placebo controls) and histopathologic damage. In contrast, L-158,809 offered moderate protection (BUN 66.6 {+-} 3.9 mg/dL; p = 0.02 vs. placebo controls). Spironolactone treatment, however, significantly prevented the development of histopathologic and functional changes (BUN 31.2 {+-} 2.5 mg/dL; p <0.001 vs. placebo controls). Conclusions: Low-dose spironolactone and, to a lesser extent, angiotensin receptor-1 blockade can offer renal protection in a mouse model of internal {alpha}-particle irradiation.« less

Alpha-emitting nuclides in the marine environment

NASA Astrophysics Data System (ADS)

Pentreath, R. J.

1984-06-01

The occurrence of alpha-emitting nuclides and their daughter products in the marine environment continues to be a subject of study for many reasons. Those nuclides which occur naturally, in the uranium, thorium and actinium series, are of interest because of their value in determining the rates of geological and geochemical processes in the oceans. Studies of them address such problems as the determination of rates of transfer of particulate matter, deposition rates, bioturbation rates, and so on. Two of the natural alpha-series nuclides in which a different interest has been expressed are 210Po and 226Ra, because their concentrations in marine organisms are such that they contribute to a significant fraction of the background dose rates sustained both by the organisms themselves and by consumers of marine fish and shellfish. To this pool of naturally-occurring nuclides, human activities have added the transuranium nuclides, both from the atmospheric testing of nuclear devices and from the authorized discharges of radioactive wastes into coastal waters and the deep sea. Studies have therefore been made to understand the chemistry of these radionuclides in sea water, their association with sedimentary materials, and their accumulation by marine organisms, the last of these being of particular interest because the transuranics are essentially "novel" elements to the marine fauna and flora. The need to predict the long-term behaviour of these nuclides has, in turn, stimulated research on those naturally-occurring nuclides which may behave in a similar manner.

Coupling of Uranium and Thorium Series Isotope Systematics for Age Determination of Late Pleistocene Zircons using LA-ICP-MS

NASA Astrophysics Data System (ADS)

Sakata, S.; Hirakawa, S.; Iwano, H.; Danhara, T.; Hirata, T.

2014-12-01

Zircon U-Th-Pb dating method is one of the most important tools for estimating the duration of magmatism by means of coupling of uranium, actinium and thorium decay series. Using U-Pb dating method, its reliability is principally guaranteed by the concordance between 238U-206Pb and 235U-207Pb ages. In case of dating Quaternary zircons, however, the initial disequilibrium effect on 230Th and 231Pa should be considered. On the other hands, 232Th-208Pb dating method can be a simple but powerful approach for investigating the age of crystallization because of negligible influence from initial disequilibrium effect. We have developed a new correction model for accurate U-Pb dating of the young zircon samples by taking into consideration of initial disequilibrium and a U-Pb vs Th-Pb concordia diagram for reliable age calibration was successfully established. Hence, the U-Th-Pb dating method can be applied to various zircons ranging from Hadean (4,600 Ma) to Quaternary (~50 ka) ages, and this suggests that further detailed information concerning the thermal history of the geological sequences can be made by the coupling of U-Th-Pb, fission track and Ar-Ar ages. In this presentation, we will show an example of U-Th-Pb dating for zircon samples from Sambe Volcano (3 to 100 ka), southwest Japan and the present dating technique using LA-ICP-MS.

Alpha-particle radiotherapy: For large solid tumors diffusion trumps targeting.

PubMed

Zhu, Charles; Sempkowski, Michelle; Holleran, Timothy; Linz, Thomas; Bertalan, Thomas; Josefsson, Anders; Bruchertseifer, Frank; Morgenstern, Alfred; Sofou, Stavroula

2017-06-01

Diffusion limitations on the penetration of nanocarriers in solid tumors hamper their therapeutic use when labeled with α-particle emitters. This is mostly due to the α-particles' relatively short range (≤100 μm) resulting in partial tumor irradiation and limited killing. To utilize the high therapeutic potential of α-particles against solid tumors, we designed non-targeted, non-internalizing nanometer-sized tunable carriers (pH-tunable liposomes) that are triggered to release, within the slightly acidic tumor interstitium, highly-diffusive forms of the encapsulated α-particle generator Actinium-225 ( 225 Ac) resulting in more homogeneous distributions of the α-particle emitters, improving uniformity in tumor irradiation and increasing killing efficacies. On large multicellular spheroids (400 μm-in-diameter), used as surrogates of the avascular areas of solid tumors, interstitially-releasing liposomes resulted in best growth control independent of HER2 expression followed in performance by (a) the HER2-targeting radiolabeled antibody or (b) the non-responsive liposomes. In an orthotopic human HER2-negative mouse model, interstitially-releasing 225 Ac-loaded liposomes resulted in the longest overall and median survival. This study demonstrates the therapeutic potential of a general strategy to bypass the diffusion-limited transport of radionuclide carriers in solid tumors enabling interstitial release from non-internalizing nanocarriers of highly-diffusing and deeper tumor-penetrating molecular forms of α-particle emitters, independent of cell-targeting. Copyright © 2017 Elsevier Ltd. All rights reserved.

Understanding the Radioactive Ingrowth and Decay of Naturally Occurring Radioactive Materials in the Environment: An Analysis of Produced Fluids from the Marcellus Shale.

PubMed

Nelson, Andrew W; Eitrheim, Eric S; Knight, Andrew W; May, Dustin; Mehrhoff, Marinea A; Shannon, Robert; Litman, Robert; Burnett, William C; Forbes, Tori Z; Schultz, Michael K

2015-07-01

The economic value of unconventional natural gas resources has stimulated rapid globalization of horizontal drilling and hydraulic fracturing. However, natural radioactivity found in the large volumes of "produced fluids" generated by these technologies is emerging as an international environmental health concern. Current assessments of the radioactivity concentration in liquid wastes focus on a single element-radium. However, the use of radium alone to predict radioactivity concentrations can greatly underestimate total levels. We investigated the contribution to radioactivity concentrations from naturally occurring radioactive materials (NORM), including uranium, thorium, actinium, radium, lead, bismuth, and polonium isotopes, to the total radioactivity of hydraulic fracturing wastes. For this study we used established methods and developed new methods designed to quantitate NORM of public health concern that may be enriched in complex brines from hydraulic fracturing wastes. Specifically, we examined the use of high-purity germanium gamma spectrometry and isotope dilution alpha spectrometry to quantitate NORM. We observed that radium decay products were initially absent from produced fluids due to differences in solubility. However, in systems closed to the release of gaseous radon, our model predicted that decay products will begin to ingrow immediately and (under these closed-system conditions) can contribute to an increase in the total radioactivity for more than 100 years. Accurate predictions of radioactivity concentrations are critical for estimating doses to potentially exposed individuals and the surrounding environment. These predictions must include an understanding of the geochemistry, decay properties, and ingrowth kinetics of radium and its decay product radionuclides.

RADIOLOGICAL PHYSICS DIVISION SEMIANNUAL REPORT FOR JULY THROUGH DECEMBER 1958

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

1959-05-01

ABS>Progress is reported in the following studies: the decay time of irradiated scintillation solutions; the performance of twin scintillation detectors for measuring neutrons in the presence of gamma radiation; the measurement of cosmic ray neutron background with a twin scintillation fast neutron spectrometer; the diffusion and absorption of gases in plastic-walled ionization chambers; calculations of the drift velocity and the energy distribution of electrons of helium, neon, argon, and nitrogen under the action of a uniform electric field; the development of equipment for tracer studies of atmospheric diffusion; the deposition and retention of isotopes of actinium, radon, radium, and thoriummore » in bone; the effects of age on calcium metabolism in bone,; the development of a mathematical theory of the retention of radioactive elements by bone; the development of a reproducible method for directly determining individual alpha activities in mixtures; the design of a flow-gas Geiger counter; a survey of the natural radioactivity of a number of municipal water supplies; measurements of activity in individuals by means of the human spectrometer; measurements of the cesium-l37 content of human subjects; measurements of the atmospheric content of cesium-137 as a function of time; a comparison of background radioactivity at the Laboratory and a site approximately 250 feet below grade level; development of a spectrometric method for measurements of radioactivity in soil; the effects of meteorological variables on the distribution of radon in the atmosphere; and studies of atmospheric diffusion. A list of publications during the period is included. (For preceding period see ANL-5919.) (C.H.)« less

Radiometals as payloads for radioimmunotherapy for lymphoma.

PubMed

DeNardo, Gerald L; Kennel, Stephen J; Siegel, Jeffry A; Denardo, Sally J

2004-10-01

Because of their remarkable effectiveness in radioimmunotherapy (RIT), 2 anti-CD20 monoclonal antibody (MAb) drugs, one labeled with indium 111 for imaging or yttrium 90 for therapy, and another labeled with iodine I 131 for imaging and therapy, have been approved for use in patients with non-Hodgkin's lymphoma (NHL). Successful RIT for lymphomas is due in large part to the rapid and efficient binding of the targeted MAb to lymphoma cells. Carcinomas are more difficult to access, necessitating novel strategies matched with radionuclides with specific physical properties. Because there are many radionuclides from which to choose, a systematic approach is required to select those preferred for a specific application. Thus far, radionuclides with g emissions for imaging and particulate emissions for therapy have been investigated. Radionuclides of iodine were the first to be used for RIT. Many conventionally radioiodinated MAbs are degraded after endocytosis by target cells, releasing radioiodinated peptides and amino acids. In contrast, radiometals have been shown to have residualizing properties, advantageous when the MAb is localized in malignant tissue. b-emitting lanthanides like those of 90Y, lutetium 177, etc. have attractive combinations of biologic, physical, radiochemical, production, economic, and radiation safety characteristics. Other radiometals, such as copper-67 and copper-64, are also of interest. a-emitters, including actinium-225 and bismuth-213, have been used for therapy in selected applications. Evidence for the impact of the radionuclide is provided by data from the randomized pivotal phase III trial of 90Y ibritumomab tiuxetan (Zevalin) in patients with NHL; responses were about 2 times greater in the 90Y ibritumomab tiuxetan arm than in the rituximab arm. It is clear that RIT has emerged as a safe and efficient method for treatment of NHL, especially in specific settings.

Alpha-emitting isotopes and chromium in a coastal California aquifer

USGS Publications Warehouse

Densmore, Jill N.; Izbicki, John A.; Murtaugh, Joseph M.; Swarzenski, Peter W.; Bullen, Thomas D.

2014-01-01

The unadjusted 72-h gross alpha activities in water from two wells completed in marine and alluvial deposits in a coastal southern California aquifer 40 km north of San Diego were 15 and 25 picoCuries per liter (pCi/L). Although activities were below the Maximum Contaminant Level (MCL) of 15 pCi/L, when adjusted for uranium activity; there is concern that new wells in the area may exceed MCLs, or that future regulations may limit water use from the wells. Coupled well-bore flow and depth-dependent water-quality data collected from the wells in 2011 (with analyses for isotopes within the uranium, actinium, and thorium decay-chains) show gross alpha activity in marine deposits is associated with decay of naturally-occurring 238U and its daughter 234U. Radon activities in marine deposits were as high as 2230 pCi/L. In contrast, gross alpha activities in overlying alluvium within the Piedra de Lumbre watershed, eroded from the nearby San Onofre Hills, were associated with decay of 232Th, including its daughter 224Ra. Radon activities in alluvium from Piedra de Lumbre of 450 pCi/L were lower than in marine deposits. Chromium VI concentrations in marine deposits were less than the California MCL of 10 μg/L (effective July 1, 2014) but δ53Cr compositions were near zero and within reported ranges for anthropogenic chromium. Alluvial deposits from the nearby Las Flores watershed, which drains a larger area having diverse geology, has low alpha activities and chromium as a result of geologic and geochemical conditions and may be more promising for future water-supply development.

An aerial radiological survey of the Nevada Test Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hendricks, T J; Riedhauser, S R

1999-12-01

A team from the Remote Sensing Laboratory conducted an aerial radiological survey of the US Department of Energy's Nevada Test Site including three neighboring areas during August and September 1994. The survey team measured the terrestrial gamma radiation at the Nevada Test Site to determine the levels of natural and man-made radiation. This survey included the areas covered by previous surveys conducted from 1962 through 1993. The results of the aerial survey showed a terrestrial background exposure rate that varied from less than 6 microroentgens per hour (mR/h) to 50 mR/h plus a cosmic-ray contribution that varied from 4.5 mR/hmore » at an elevation of 900 meters (3,000 feet) to 8.5 mR/h at 2,400 meters (8,000 feet). In addition to the principal gamma-emitting, naturally occurring isotopes (potassium-40, thallium-208, bismuth-214, and actinium-228), the man-made radioactive isotopes found in this survey were cobalt-60, cesium-137, europium-152, protactinium-234m an indicator of depleted uranium, and americium-241, which are due to human actions in the survey area. Individual, site-wide plots of gross terrestrial exposure rate, man-made exposure rate, and americium-241 activity (approximating the distribution of all transuranic material) are presented. In addition, expanded plots of individual areas exhibiting these man-made contaminations are given. A comparison is made between the data from this survey and previous aerial radiological surveys of the Nevada Test Site. Some previous ground-based measurements are discussed and related to the aerial data. In regions away from man-made activity, the exposure rates inferred from the gamma-ray measurements collected during this survey agreed very well with the exposure rates inferred from previous aerial surveys.« less

Understanding the Radioactive Ingrowth and Decay of Naturally Occurring Radioactive Materials in the Environment: An Analysis of Produced Fluids from the Marcellus Shale

PubMed Central

Nelson, Andrew W.; Eitrheim, Eric S.; Knight, Andrew W.; May, Dustin; Mehrhoff, Marinea A.; Shannon, Robert; Litman, Robert; Burnett, William C.; Forbes, Tori Z.

2015-01-01

Background The economic value of unconventional natural gas resources has stimulated rapid globalization of horizontal drilling and hydraulic fracturing. However, natural radioactivity found in the large volumes of “produced fluids” generated by these technologies is emerging as an international environmental health concern. Current assessments of the radioactivity concentration in liquid wastes focus on a single element—radium. However, the use of radium alone to predict radioactivity concentrations can greatly underestimate total levels. Objective We investigated the contribution to radioactivity concentrations from naturally occurring radioactive materials (NORM), including uranium, thorium, actinium, radium, lead, bismuth, and polonium isotopes, to the total radioactivity of hydraulic fracturing wastes. Methods For this study we used established methods and developed new methods designed to quantitate NORM of public health concern that may be enriched in complex brines from hydraulic fracturing wastes. Specifically, we examined the use of high-purity germanium gamma spectrometry and isotope dilution alpha spectrometry to quantitate NORM. Results We observed that radium decay products were initially absent from produced fluids due to differences in solubility. However, in systems closed to the release of gaseous radon, our model predicted that decay products will begin to ingrow immediately and (under these closed-system conditions) can contribute to an increase in the total radioactivity for more than 100 years. Conclusions Accurate predictions of radioactivity concentrations are critical for estimating doses to potentially exposed individuals and the surrounding environment. These predictions must include an understanding of the geochemistry, decay properties, and ingrowth kinetics of radium and its decay product radionuclides. Citation Nelson AW, Eitrheim ES, Knight AW, May D, Mehrhoff MA, Shannon R, Litman R, Burnett WC, Forbes TZ, Schultz MK. 2015. Understanding the radioactive ingrowth and decay of naturally occurring radioactive materials in the environment: an analysis of produced fluids from the Marcellus Shale. Environ Health Perspect 123:689–696; http://dx.doi.org/10.1289/ehp.1408855 PMID:25831257

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Watson, David J.; Strom, Daniel J.

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

The discovery of plutonium reorganized the periodic table and aided the discovery of new elements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clark, David L

2009-01-01

The modern Periodic Table derives principally from the work of the great Russian scientist Dimitri Mendeleev, who in 1869 enunciated a 'periodic law' that the properties of the elements are a periodic function of their atomic weights, and arranged the 65 known elements in a 'periodic table'. Fundamentally, every column in the main body of the Periodic Table is a grouping of elements that display similar chemical and physical behavior. Similar properties are therefore exhibited by elements with widely different mass. Chemical periodicity is central to the study of chemistry, and no other generalization comes close to its ability tomore » systematize and rationalize known chemical facts. With the development of atomic theory, and an understanding of the electronic structure of atoms, chemical periodicity and the periodic table now find their natural explanation in the electronic structure of atoms. Moving from left to right along any row, the elements are arranged sequentially according to nuclear charge (the atomic number). Electrons counter balance that nuclear charge, hence each successive element has one more electron in its configuration. The electron configuration, or distribution of electrons among atomic orbitals, may be determined by application of the Pauli principle (paired spin in the same orbital) and the aufbau principle (which outlines the order of filling of electrons into shells of orbitals - s, p, d, f, etc.) such that in a given atom, no two electrons may have all four quantum numbers identical. In 1939, only three elements were known to be heavier than actinium: thorium, protactinium, and uranium. All three exhibited variable oxidation states and a complex chemistry. Thorium, protactinium and uranium were assumed to be d-transition metals and were placed in the Periodic Table under hafnium, tantalum, and tungsten, respectively. By 1940, McMillan and Abelson bombarded uranium atoms with slow neutrons and successfully identified atoms of element 93, which they named neptunium after the planet Neptune. This rapidly set the stage for the discovery of the next succeeding element, plutonium (Seaborg, McMillan, Kennedy, and Wahl, 1940), named after the next planet away from the Sun, Pluto. The newly discovered elements were presumed to fit comfortably in the Periodic Table under rhenium and osmium, respectively. However, subsequent tracer chemical experiments showed that neptunium and plutonium were closer in their chemical properties to uranium than their presumed homologues, rhenium and osmium. Spectroscopic evidence also indicated that the new elements were not typical transition elements, but had f-electrons in their valence shell. Thus, several researchers, including McMillan and Wahl, and Zachariasen at Los Alamos, suggested that these elements might be part of a second inner-transition series in which the 5f-electron subshell was being filled. It was not clear, however, where the new series would begin. McMillian had proposed a 'uraninide series' that started with neptunium, but attempts to isolate elements with atomic numbers 95 and 96 based on assumed similarities to uranium were unsuccessful. Both Wahl and Zacharias en had proposed a thoride series that started with protactinium. In 1944, Seaborg proposed that the series started with thorium, and that all of the elements heavier than actinium constituted an 'actinide' series similar to the lanthanides. Because the 5f-shell began filling in the same relative position as the 4f-shell, the electronic configuration of elements in the two series would be similar. Guided by the hypothesis that elements 95 and 96 were homologues of europium and gadolinium, new experiments were designed and the elements were uniquely synthesized and separated from all others. The new elements were subsequently named americium and curium. Seaborg's 'Actinide Concept' thus played a major role in the discovery of the transplutonium elements. It provided the framework that supported synthesis, isolation, and identification of the succeeding actinide elements berkelium through lawrencium and beyond to the element with Atomic Number 118. But as research has progressed in the study of the actinide elements, it has become clear that the 5f series has a unique chemistry that is distinct from the lanthanides. One of the focal points of study in actinide research has been to better define the scope and limitations of the actinide concept. Seaborg's actinide concept of heavy element electronic structure, prediction that the actinides form a transition series analogous to the rare earth series of lanthanide elements, is now well accepted in the scientific community and included in all standard configurations of the Periodic Table.« less

Theoretical investigation of M@Pb122- and M@Sn122- Zintl clusters (M = Lrn+, Lun+, La3+, Ac3+ and n = 0, 1, 2, 3).

PubMed

Joshi, Meenakshi; Chandrasekar, Aditi; Ghanty, Tapan K

2018-06-06

The positions of lawrencium (Lr), lutetium (Lu), actinium (Ac) and lanthanum (La) in the periodic table have been a controversial topic for quite some time. According to studies carried out by different groups with their justifications, these elements may potentially be placed in the d-block, p-block or all four in a 15 element f-block. The present work looks into this issue from a new perspective, which involves encapsulation of these four elements into Zintl ion clusters, Pb122- and Sn122-, followed by the determination of the structural, thermodynamic and electronic properties of these endohedral M@Pb122- and M@Sn122- clusters (M = Lrn+, Lun+ with n = 0, 1, 2, 3) using first principles based density functional theory (DFT). These parameters are compared with similar clusters encapsulated La3+ and Ac3+ ions in order to seek out similarities and differences to draw conclusions about their placement in the periodic table. For the first time the structural, energetic, and electronic properties of these metal atom/ion encapsulated Pb122- and Sn122- clusters have been investigated thoroughly. Structural parameters such as bond distances, geometry and symmetry, electronic properties viz. the density of states, the molecular orbital ordering, the electron localization function, bond critical point properties and charge distributions have been analyzed. Additionally, the thermodynamic property of the binding energy during the encapsulation process has also been calculated. All M@Pb12+ and M@Sn12+ (M = Lr and Lu) clusters form stable 18 bonding electron magic number systems with shell closing. They show negative values of binding energy and relatively large HOMO-LUMO energy gaps indicating the stability of such clusters. All the calculated parameters for Lr encapsulated clusters closely match with the corresponding calculated parameters of Lu encapsulated clusters, confirming the similarity between Lr and Lu metal atoms in various oxidation states, though their atomic ground state valence electronic configurations are different. The effect of spin orbit coupling has also been investigated using the ZORA approach. It is interesting to discover that La and Ac showed striking similarities to Lr and Lu with respect to all the properties investigated and have formed a stable 18-electron system.

Modeling Cell and Tumor-Metastasis Dosimetry with the Particle and Heavy Ion Transport Code System (PHITS) Software for Targeted Alpha-Particle Radionuclide Therapy.

PubMed

Lee, Dongyoul; Li, Mengshi; Bednarz, Bryan; Schultz, Michael K

2018-06-26

The use of targeted radionuclide therapy for cancer is on the rise. While beta-particle-emitting radionuclides have been extensively explored for targeted radionuclide therapy, alpha-particle-emitting radionuclides are emerging as effective alternatives. In this context, fundamental understanding of the interactions and dosimetry of these emitted particles with cells in the tumor microenvironment is critical to ascertaining the potential of alpha-particle-emitting radionuclides. One important parameter that can be used to assess these metrics is the S-value. In this study, we characterized several alpha-particle-emitting radionuclides (and their associated radionuclide progeny) regarding S-values in the cellular and tumor-metastasis environments. The Particle and Heavy Ion Transport code System (PHITS) was used to obtain S-values via Monte Carlo simulation for cell and tumor metastasis resulting from interactions with the alpha-particle-emitting radionuclides, lead-212 ( 212 Pb), actinium-225 ( 225 Ac) and bismuth-213 ( 213 Bi); these values were compared to the beta-particle-emitting radionuclides yttrium-90 ( 90 Y) and lutetium-177 ( 177 Lu) and an Auger-electron-emitting radionuclide indium-111 ( 111 In). The effect of cellular internalization on S-value was explored at increasing degree of internalization for each radionuclide. This aspect of S-value determination was further explored in a cell line-specific fashion for six different cancer cell lines based on the cell dimensions obtained by confocal microscopy. S-values from PHITS were in good agreement with MIRDcell S-values (cellular S-values) and the values found by Hindié et al. (tumor S-values). In the cellular model, 212 Pb and 213 Bi decay series produced S-values that were 50- to 120-fold higher than 177 Lu, while 225 Ac decay series analysis suggested S-values that were 240- to 520-fold higher than 177 Lu. S-values arising with 100% cellular internalization were two- to sixfold higher for the nucleus when compared to 0% internalization. The tumor dosimetry model defines the relative merit of radionuclides and suggests alpha particles may be effective for large tumors as well as small tumor metastases. These results from PHITS modeling substantiate emerging evidence that alpha-particle-emitting radionuclides may be an effective alternative to beta-particle-emitting radionuclides for targeted radionuclide therapy due to preferred dose-deposition profiles in the cellular and tumor metastasis context. These results further suggest that internalization of alpha-particle-emitting radionuclides via radiolabeled ligands may increase the relative biological effectiveness of radiotherapeutics.

Radiation Doses to Members of the U.S. Population from Ubiquitous Radionuclides in the Body: Part 3, Results, Variability, and Uncertainty

DOE Office of Scientific and Technical Information (OSTI.GOV)

Watson, David J.; Strom, Daniel J.

This paper is part three of a three-part series investigating annual effective doses to residents of the United States from intakes of ubiquitous radionuclides, including radionuclides occurring naturally, radionuclides whose concentrations are technologically enhanced, and anthropogenic radionuclides. The radionuclides of interest are the 238U series (14 nuclides), the actinium series (headed by 235U; 11 nuclides), and the 232Th series (11 nuclides); primordial radionuclides 87Rb and 40K; cosmogenic and fallout radionuclides 14C and 3H; and purely anthropogenic radionuclides 137Cs-137mBa, 129I and 90Sr-90Y. This series of papers explicitly excludes intakes from inhaling 222Rn, 220Rn, and their short-lived decay products; it also excludesmore » intakes of radionuclides in occupational and medical settings. Part one reviewed, summarized, characterized, and grouped all published and some unpublished data for U.S. residents on ubiquitous radionuclide concentrations in tissues and organs. Part two described the methods used to organize the data collected in part one and segregate it into the ages and genders defined by the study, imputed missing values from the existing data, apportioned activity in bone, and imputed activity in hollow organ contents and the remainder of the body. This paper estimates equivalent doses to target tissues from source regions and maps target tissues to lists of tissues with International Commission on Radiation Protection (ICRP) tissue-weighting factors or to surrogate tissue regions when there is no direct match. Effective doses, using ICRP tissue-weighting factors recommended in 1977, 1990, and 2007, are then calculated, and an upper bound of variability of the effective dose is estimated by calculating the average coefficients of variation (CV), assuming all variance is due to variability. Most of the data were for adult males, whose average annual effective dose is estimated to be 337 μSv (CV = 0.65, geometric mean = 283 μSv, geometric standard deviation sG = 1.81) using 2007 ICRP tissue-weighting factors. This result is between the National Council on Radiation Protection & Measurements’ 1987 estimate of 390 μSv (using 1977 wTs) and its 2009 estimate of 285 μSv (using 2007 wTs) and is higher than the United Nations Scientific Committee on the Effects of Atomic Radiation’s 2000 estimate of 310 μSv (using 1990 wTs). The methods and software developed for this project are sufficiently detailed and sufficiently general to be usable with autopsy data from any or all countries.« less

Optimizing labelling conditions of 213Bi-DOTATATE for preclinical applications of peptide receptor targeted alpha therapy.

PubMed

Chan, Ho Sze; de Blois, Erik; Konijnenberg, Mark W; Morgenstern, Alfred; Bruchertseifer, Frank; Norenberg, Jeffrey P; Verzijlbergen, Fred J; de Jong, Marion; Breeman, Wouter A P

2017-01-01

213 Bismuth ( 213 Bi, T 1/2 = 45.6 min) is one of the most frequently used α-emitters in cancer research. High specific activity radioligands are required for peptide receptor radionuclide therapy. The use of generators containing less than 222 MBq 225 Ac (actinium), due to limited availability and the high cost to produce large-scale 225 Ac/ 213 Bi generators, might complicate in vitro and in vivo applications though.Here we present optimized labelling conditions of a DOTA-peptide with an 225 Ac/ 213 Bi generator (< 222 MBq) for preclinical applications using DOTA-Tyr 3 -octreotate (DOTATATE), a somatostatin analogue. The following labelling conditions of DOTATATE with 213 Bi were investigated; peptide mass was varied from 1.7 to 7.0 nmol, concentration of TRIS buffer from 0.15 mol.L -1 to 0.34 mol.L -1 , and ascorbic acid from 0 to 71 mmol.L -1 in 800 μL. All reactions were performed at 95 °C for 5 min. After incubation, DTPA (50 nmol) was added to stop the labelling reaction. Besides optimizing the labelling conditions, incorporation yield was determined by ITLC-SG and radiochemical purity (RCP) was monitored by RP-HPLC up to 120 min after labelling. Dosimetry studies in the reaction vial were performed using Monte Carlo and in vitro clonogenic assay was performed with a rat pancreatic tumour cell line, CA20948. At least 3.5 nmol DOTATATE was required to obtain incorporation ≥ 99 % with 100 MBq 213 Bi (at optimized pH conditions, pH 8.3 with 0.15 mol.L -1 TRIS) in a reaction volume of 800 μL. The cumulative absorbed dose in the reaction vial was 230 Gy/100 MBq in 30 min. A minimal final concentration of 0.9 mmol.L -1 ascorbic acid was required for ~100 MBq (t = 0) to minimize radiation damage of DOTATATE. The osmolarity was decreased to 0.45 Osmol/L.Under optimized labelling conditions, 213 Bi-DOTATATE remained stable up to 2 h after labelling, RCP was ≥ 85 %. In vitro showed a negative correlation between ascorbic acid concentration and cell survival. 213 Bismuth-DOTA-peptide labelling conditions including peptide amount, quencher and pH were optimized to meet the requirements needed for preclinical applications in peptide receptor radionuclide therapy.

The release of dissolved actinium to the ocean: A global comparison of different end-members

USGS Publications Warehouse

Geibert, W.; Charette, M.; Kim, G.; Moore, W.S.; Street, J.; Young, M.; Paytan, A.

2008-01-01

The measurement of short-lived 223Ra often involves a second measurement for supported activities, which represents 227Ac in the sample. Here we exploit this fact, presenting a set of 284 values on the oceanic distribution of 227Ac, which was collected when analyzing water samples for short-lived radium isotopes by the radium delayed coincidence counting system. The present work compiles 227Ac data from coastal regions all over the northern hemisphere, including values from ground water, from estuaries and lagoons, and from marine end-members. Deep-sea samples from a continental slope off Puerto Rico and from an active vent site near Hawaii complete the overview of 227Ac near its potential sources. The average 227Ac activities of nearshore marine end-members range from 0.4??dpm m- 3 at the Gulf of Mexico to 3.0??dpm m- 3 in the coastal waters of the Korean Strait. In analogy to 228Ra, we find the extension of adjacent shelf regions to play a substantial role for 227Ac activities, although less pronounced than for radium, due to its weaker shelf source. Based on previously published values, we calculate an open ocean 227Ac inventory of 1.35 * 1018??dpm 227Acex in the ocean, which corresponds to 37??moles, or 8.4??kg. This implies a flux of 127??dpm m-2 y- 1 from the deep-sea floor. For the shelf regions, we obtain a global inventory of 227Ac of 4.5 * 1015??dpm, which cannot be converted directly into a flux value, as the regional loss term of 227Ac to the open ocean would have to be included. Ac has so far been considered to behave similarly to Ra in the marine environment, with the exception of a strong Ac source in the deep-sea due to 231Paex. Here, we present evidence of geochemical differences between Ac, which is retained in a warm vent system, and Ra, which is readily released [Moore, W.S., Ussler, W. and Paull, C.K., 2008-this issue. Short-lived radium isotopes in the Hawaiian margin: Evidence for large fluid fluxes through the Puna Ridge. Marine Chemistry]. Another potential mechanism of producing deviations in 227Ac/228Ra and daughter isotope ratios from the expected production value of lithogenic material is observed at reducing environments, where enrichment in uranium may occur. The presented data here may serve as a reference for including 227Ac in circulation models, and the overview provides values for some end-members that contribute to the global Ac distribution. ?? 2007 Elsevier B.V. All rights reserved.

Applications of High Intensity Proton Accelerators

NASA Astrophysics Data System (ADS)

Raja, Rajendran; Mishra, Shekhar

2010-06-01

Superconducting radiofrequency linac development at Fermilab / S. D. Holmes -- Rare muon decay experiments / Y. Kuno -- Rare kaon decays / D. Bryman -- Muon collider / R. B. Palmer -- Neutrino factories / S. Geer -- ADS and its potential / J.-P. Revol -- ADS history in the USA / R. L. Sheffield and E. J. Pitcher -- Accelerator driven transmutation of waste: high power accelerator for the European ADS demonstrator / J. L. Biarrotte and T. Junquera -- Myrrha, technology development for the realisation of ADS in EU: current status & prospects for realisation / R. Fernandez ... [et al.] -- High intensity proton beam production with cyclotrons / J. Grillenberger and M. Seidel -- FFAG for high intensity proton accelerator / Y. Mori -- Kaon yields for 2 to 8 GeV proton beams / K. K. Gudima, N. V. Mokhov and S. I. Striganov -- Pion yield studies for proton driver beams of 2-8 GeV kinetic energy for stopped muon and low-energy muon decay experiments / S. I. Striganov -- J-Parc accelerator status and future plans / H. Kobayashi -- Simulation and verification of DPA in materials / N. V. Mokhov, I. L. Rakhno and S. I. Striganov -- Performance and operational experience of the CNGS facility / E. Gschwendtner -- Particle physics enabled with super-conducting RF technology - summary of working group 1 / D. Jaffe and R. Tschirhart -- Proton beam requirements for a neutrino factory and muon collider / M. S. Zisman -- Proton bunching options / R. B. Palmer -- CW SRF H linac as a proton driver for muon colliders and neutrino factories / M. Popovic, C. M. Ankenbrandt and R. P. Johnson -- Rapid cycling synchrotron option for Project X / W. Chou -- Linac-based proton driver for a neutrino factory / R. Garoby ... [et al.] -- Pion production for neutrino factories and muon colliders / N. V. Mokhov ... [et al.] -- Proton bunch compression strategies / V. Lebedev -- Accelerator test facility for muon collider and neutrino factory R&D / V. Shiltsev -- The superconducting RF linac for muon collider and neutrino factory - summary of working group 2 / J. Galambos, R. Garoby and S. Geer -- Prospects for a very high power CW SRF linac / R. A. Rimmer -- Indian accelerator program for ADS applications / V. C. Sahni and P. Singh -- Ion accelerator activities at VECC (particularly, operating at low temperature) / R. K. Bhandari -- Chinese efforts in high intensity proton accelerators / S. Fu, J. Wang and S. Fang -- ADSR activity in the UK / R. J. Barlow -- ADS development in Japan / K. Kikuchi -- Project-X, SRF, and very large power stations / C. M. Ankenbrandt, R. P. Johnson and M. Popovic -- Power production and ADS / R. Raja -- Experimental neutron source facility based on accelerator driven system / Y. Gohar -- Transmutation mission / W. S. Yang -- Safety performance and issues / J. E. Cahalan -- Spallation target design for accelerator-driven systems / Y. Gohar -- Design considerations for accelerator transmutation of waste system / W. S. Yang -- Japan ADS program / T. Sasa -- Overview of members states' and IAEA activities in the field of Accelerator Driven Systems (ADS) / A. Stanculescu -- Linac for ADS applications - accelerator technologies / R. W. Garnett and R. L. Sheffield -- SRF linacs and accelerator driven sub-critical systems - summary working groups 3 & 4 / J. Delayen -- Production of Actinium-225 via high energy proton induced spallation of Thorium-232 / J. Harvey ... [et al.] -- Search for the electric dipole moment of Radium-225 / R. J. Holt, Z.-T. Lu and R. Mueller -- SRF linac and material science and medicine - summary of working group 5 / J. Nolen, E. Pitcher and H. Kirk.

Biological pathways of exposure and ecotoxicity values for uranium and associated radionuclides: Chapter D in Hydrological, geological, and biological site characterization of breccia pipe uranium deposits in Northern Arizona

USGS Publications Warehouse

Hinck, Jo E.; Linder, Greg L.; Finger, Susan E.; Little, Edward E.; Tillitt, Donald E.; Kuhne, Wendy

2010-01-01

This chapter compiles available chemical and radiation toxicity information for plants and animals from the scientific literature on naturally occurring uranium and associated radionuclides. Specifically, chemical and radiation hazards associated with radionuclides in the uranium decay series including uranium, thallium, thorium, bismuth, radium, radon, protactinium, polonium, actinium, and francium were the focus of the literature compilation. In addition, exposure pathways and a food web specific to the segregation areas were developed. Major biological exposure pathways considered were ingestion, inhalation, absorption, and bioaccumulation, and biota categories included microbes, invertebrates, plants, fishes, amphibians, reptiles, birds, and mammals. These data were developed for incorporation into a risk assessment to be conducted as part of an environmental impact statement for the Bureau of Land Management, which would identify representative plants and animals and their relative sensitivities to exposure of uranium and associated radionuclides. This chapter provides pertinent information to aid in the development of such an ecological risk assessment but does not estimate or derive guidance thresholds for radionuclides associated with uranium. Previous studies have not attempted to quantify the risks to biota caused directly by the chemical or radiation releases at uranium mining sites, although some information is available for uranium mill tailings and uranium mine closure activities. Research into the biological impacts of uranium exposure is strongly biased towards human health and exposure related to enriched or depleted uranium associated with the nuclear energy industry rather than naturally occurring uranium associated with uranium mining. Nevertheless, studies have reported that uranium and other radionuclides can affect the survival, growth, and reproduction of plants and animals. Exposure to chemical and radiation hazards is influenced by a plant’s or an animal’s life history and surrounding environment. Various species of plants, invertebrates, fishes, amphibians, reptiles, birds, and mammals found in the segregation areas that are considered species of concern by State and Federal agencies were included in the development of the site-specific food web. The utilization of subterranean habitats (burrows in uranium-rich areas, burrows in waste rock piles or reclaimed mining areas, mine tunnels) in the seasonally variable but consistently hot, arid environment is of particular concern in the segregation areas. Certain species of reptiles, amphibians, birds, and mammals in the segregation areas spend significant amounts of time in burrows where they can inhale or ingest uranium and other radionuclides through digging, eating, preening, and hibernating. Herbivores may also be exposed though the ingestion of radionuclides that have been aerially deposited on vegetation. Measured tissues concentrations of uranium and other radionuclides are not available for any species of concern in the segregation areas. The sensitivity of these animals to uranium exposure is unknown based on the existing scientific literature, and species-specific uranium presumptive effects levels were only available for two endangered fish species known to inhabit the segregation areas. Overall, the chemical toxicity data available for biological receptors of concern were limited, although chemical and radiation toxicity guidance values are available from several sources. However, caution should be used when directly applying these values to northern Arizona given the unique habitat and life history strategies of biological receptors in the segregation areas and the fact that some guidance values are based on models rather than empirical (laboratory or field) data. No chemical toxicity information based on empirical data is available for reptiles, birds, or wild mammals; therefore, the risks associated with uranium and other radionuclides are unknown for these biota.

Mortality of employees of the Atomic Weapons Establishment, 1951-82.

PubMed Central

Beral, V.; Fraser, P.; Carpenter, L.; Booth, M.; Brown, A.; Rose, G.

1988-01-01

A total of 22,552 workers employed by the Atomic Weapons Establishment between 1951 and 1982 were followed up for an average of 18.6 years. Of the 3115 who died, 865 (28%) died of cancer. Mortality was 23% lower than the national average for all causes of death and 18% lower for cancer. These low rates were consistent with the findings in other workforces in the nuclear industry and reflect, at least in part, the selection of healthy people to work in the industry and the disproportionate recruitment of people from the higher social classes. At some time during their employment 9389 (42%) of the workers were monitored for exposure to radiation, the average cumulative whole body exposure to external radiation being 7.8 mSv. Their mortality was generally similar to that of other employees, even when exposures were lagged by 10 years. The rate ratio after a 10 year lag in workers with a radiation record compared with other workers was 1.01 (95% confidence interval 0.92 to 1.10) for all causes of death and 1.06 (0.89 to 1.27) for all malignant neoplasms. The only significant differences were for prostatic cancer (rate ratio 2.23; 95% confidence interval 1.13 to 4.40) and for cancers of ill defined and secondary sites (rate ratio 2.37; 1.23 to 4.56). Cancers of lymphatic and haemopoietic tissues were notable for their low occurrence in the study population, with only four deaths from leukaemia and two from multiple myeloma in workers with a radiation record, 9.16 and 3.55 deaths respectively being expected on the basis of national rates. Among workers who had a radiation record 3742 (40%) were also monitored for possible internal exposure to plutonium, 3044 (32%) to uranium, 1562 (17%) to tritium, 638 (7%) to polonium, and 281 (3%) to actinium. In these workers mortality from malignant neoplasms as a whole was not increased, but after a 10 year lag death rates from prostatic and renal cancers were generally more than twice the national average, these excesses arising in a small group of workers monitored for exposure to multiple radionuclides. Though mortality from lung cancer in workers monitored for exposure to plutonium was below the national average, it was some two thirds higher than in other radiation workers, the excess being of borderline statistical significance. Mortality from malignant neoplasms as a whole showed a weak and non-significant increasing trend with increasing level of cumulative whole body exposure to external radiation. When the exposures were lagged by 10 years the trend became stronger and significant, the estimated increase in relative risk per 10 mSv being 7.6% (95% confidence interval 0.4% to 15.3%). This trend was confined almost entirely to workers who were also monitored for exposure to radionuclides (p<0.001), the main contributions coming from lung cancer and prostatic cancer. Exposures of the lung and prostate from internal sources of radiation were not quantified, except for the contribution from tritium. It was therefore not possible to assess the extent to which the associations were due to internally deposited radionuclides rather than external exposure. The finding for prostatic cancer taken in conjunction with the results of other studies suggest a specific occupational hazard in a small group of workers in the nuclear industry who had comparatively high exposures to external radiation and who were also monitored for internal exposure to multiple radionuclides. Research is needed to discover whether any of the radionuclides and other substances concerned are concentrated in the prostate. The occurrence of lung cancer in this workforce requires further investigation taking into account smoking habits and tissue doses from inhaled radionuclides. PMID:3142540

Grain Boundary Character Distributions In Isostructural Materials

NASA Astrophysics Data System (ADS)

Ratanaphan, Sutatch

Anisotropic grain boundary character distributions (GBCDs), which influence macroscopic materials properties, are thought to be controlled by the grain boundary energy anisotropy. Structurally, grain boundary could be viewed as two free surfaces joined together. Grain boundary energy could be simply defined by the total excess energy for creating two free surfaces minus the energy gained when new bonds are formed between these surfaces. This implies that different crystal structure should have different GBEDs and GBCDs. It was recently discovered that grain boundary energy distributions (GBED) in isostructural materials, a class of materials that share the same crystal structure, are directly related to one another. This suggests that GBCDs in isostructural materials might also be related in a similar way. To test this hypothesis, electron backscatter diffraction (EBSD) was used to map grain orientations in Ag, Au, Cu, Fe, and Mo. The GBCDs were determined from the stereological interpretation of EBSD maps containing on the order of 100,000 grains. It was found that the GBCDs of face-centered cubic (FCC) metals are statistically correlated, while the GBCDs of body-centered cubic (BCC) Fe and Mo are not correlated to the GBCD of FCC metals. The degree of the correlations among the FCC metals is weaker if there are significant differences in grain shape or texture. For example, Ag has the weakest correlation to the other FCC materials and also has quantitatively different grain shapes and texture. The relationship between the populations and energies of grain boundaries was also studied. By comparing the GBCDs of Al, Au, Cu, and Ni to the energies of 388 grain boundaries previously calculated by the Embedded Atom Method (EAM), we observed a moderately inverse correlation between the relative areas of grain boundaries and their energies. Interestingly, there are strong inverse correlations between the energies and populations of the most common grain boundaries (Sigma3, Sigma9, and Sigma27). Because the enhancement of twin related boundaries due to the prevalence Sigma3 boundaries results in a decrease in the grain boundary populations for the other boundary types, this inverse correlation is influenced by the crystallographic constraints at triple junctions. In other words, having an anisotropic misorientation distribution with strong maxima for certain boundaries biases the inverse correlation between grain boundary population and energy for other boundaries and causes different slopes at each misorientation. Interestingly, the inverse correlation at each misorientation is consistent with the Boltzmann distribution. Based on our results, it is possible to predict the GBCDs and GBEDs in isostructural polycrystalline materials by using a single GBCD and GBED. This principle is demonstrated by predicting the GBCD and GBED of Actinium (Ac). To investigate the GBED in the isostructural BCC metals, the energies of 408 grain boundaries in Fe and Mo were computed using atomistic simulations based on the embedded-atom method (EAM) potential. We found that the calculated boundary energies in Fe and Mo were strongly correlated and scaled with the ratio of the cohesive energy divided by the square of the lattice constant (Ecoh/a02). We would expect that the GBCD of Fe and Mo might be correlated in a similar manner to that of FCC metals. To test this hypothesis, we compared the GBCDs of Fe and Mo. We found that the GBCDs of Fe and Mo are moderately and strongly correlated when all boundary types and only Sigma3 boundaries were considered, respectively. In this thesis, the results demonstrated that the GBCDs of isostructural materials are correlated with one another and the magnitudes of correlation coefficients varied. Reduced correlations were observed when there were differences in the microstructure and crystallographic texture. The inverse relationship between grain boundary population and energy is more strongly correlated at each misorientation than over the entire five macroscopic parameters of grain boundary, especially when there is significant misorientation texture. This relationship leads to GBCDs of isostructural materials that are also more strongly correlated at each misorientation than over the entire grain boundary space.