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At least 19 records

Shell effects in quasi-fission for calcium induced reactions forming thorium isotopes

Quantum shell effects induce an asymmetric fission mode in actinides, which disappears in neutron deficient isotopes. Quasi-fission, characterized by a significant mass transfer in heavy ion collisions at low-energies, is expected to be affected by similar shell effects. This is studied in 40−56 Ca+176 reactions with the time-dependent Hartree-Fock approach. All reactions exhibit a mass equilibration process that stops when a heavy fragment with 𝑍 ≃ 54 protons is formed. Unlike the fission of thorium compound nuclei, quasi-fission does not exhibit a transition to symmetric modes in neutron deficient systems. This observation is interpreted in terms of potential energy surfaces that show a persistence of an asymmetric valley with an increasing barrier preventing its population in fission of the most neutron deficient thorium isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Exploring the use of thorium isotope compositions and concentrations as nuclear forensic signatures for uranium ore concentrates

This interlaboratory study measured thorium concentrations and isotope compositions in uranium ore concentrates from different geographical locations to examine whether thorium impurities may be useful forensic signatures for uranium ore concentrates found out of regulatory control. Measured 230 Th/ 232 Th in fifteen uranium ore concentrates record over three orders of magnitude of compositional variation. Results demonstrate that 230 Th/ 232 Th used in combination with U/Th ratios resulted in a unique signature for individual uranium ore concentrates from different processing locations. Data presented here suggest potential for 230 Th/ 232 Th and U/Th to be used as comparative signatures to investigate the provenance of seized uranium ore concentrates.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Natural thorium isotopes in marine sediment core off Labuan port

Sediment core was collected from Labuan port and analyzed to determine the radioactivity of thorium (Th) isotopes. The objectives of this study are to determine the possible sources of Th isotopes at Labuan port and estimates the sedimentation rate based on {sup 228}Th/{sup 232}Th model. The results suggest the {sup 230}Th and {sup 232}Th might be originated from terrestrial sedimentary rock while {sup 228}Th originated by authigenic origin. High ratio value of {sup 230}Th/{sup 232}Th detected at the top surface sediment indicates the increasing of {sup 230}Th at the recent years which might be contributed from the anthropogenic sources. The sedimentation rate of core sediment from Labuan Port was successfully estimated by using {sup 228}Th/{sup 232}Th model. The result show high sedimentation rate with 4.67 cm/year indicates rapid deposition occurred at this study area due to the high physical activity at the Labuan port. By assume the constant sedimentation rate at this area; we estimated the age of 142 cm core sediment obtained from Labuan port is 32 years started from 1981 to 2012. This chronology will be used in forthcoming research to investigate the historical profile of anthropogenic activities affecting the Labuan port.

07 ISOTOPE AND RADIATION SOURCES↗

Determination of the Galaxy age by the method of uranium–thorium–plutonium isotopic ratios

The dependence of the Galaxy age (Т{sub G}), as determined by the method of uranium–thorium isotopic ratios, on the parameters of the nucleosynthesis model is studied within the theory of galactic nucleosynthesis. It is shown that ТG depends strongly both on the scenario of the production of nuclei in the r-process and those features of neutron-rich nuclei that are used in the respective analysis and on galactic-nucleosynthesis parameters. The effect of a sudden nucleosynthesis spike before the formation of a solar system on the Galaxy age is evaluated. The region of admissible values of the parameters of galacticnucleosynthesis theory is discussed. The method of uranium–thorium isotopic ratios is supplemented with the {sup 244}Pu/{sup 238}U ratio for yet another cosmochronometer pair, and the Galaxy age is estimated on the basis of the model modified in this way.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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

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 target has been utilized to produce millicurie quantities of 225 Ac. 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 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 16.7 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 -2232 Th target for 10 days in either BNL or LANL proton irradiation facilities.

139Ce↗

A new thorium-229 reference material

A new reference material was characterized for 229 Th molality and thorium isotope amount ratios. This reference material is intended for use in nuclear forensic analyses as an isotope dilution mass spectrometry spike. The reference material value and expanded uncertainty (k = 2) for the 229 Th molality is (1.1498 ± 0.0016)×10 -10 mol g -1 solution. The value and expanded uncertainty (k = 2) for the n( 230 Th)/n( 229 Th) ratio is (5.18 ± 0.26)×10 -5 and the n( 232 Th)/n( 229 Th) ratio is (3.815 ± 0.092)×10 -4 .

07 ISOTOPE AND RADIATION SOURCES↗

Project Overview: LA13-FY13-123-PD08

This project was a two year, LANL-led effort focused on extending the application of ion emitter sources in thermal ionization mass spectrometry based analysis of trace actinide systems. Particular emphasis was geared towards thorium isotope quantitation, both as a TIMS “worst case” scenario in terms of ionization efficiency and a desirable target for future chronometric measurements. Additional points of focus included source performance characteristics and identification of next-generation emitter strategies addressing remaining development challenges.

47 OTHER INSTRUMENTATION↗

On the equilibrium isotopic composition of the thorium–uranium–plutonium fuel cycle

The equilibrium isotopic compositions and the times to equilibrium in the process of thorium–uranium–plutonium oxide fuel recycling in VVER-type reactors using heavy water mixed with light water are estimated. It is demonstrated thEhfat such reactors have a capacity to operate with self-reproduction of active isotopes in the equilibrium mode.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Rapid fusion method for the determination of refractory thorium and uranium isotopes in soil samples

Recently, approximately 80% of participating laboratories failed to accurately determine uranium isotopes in soil samples in the U.S Department of Energy Mixed Analyte Performance Evaluation Program (MAPEP) Session 30, due to incomplete dissolution of refractory particles in the samples. Failing laboratories employed acid dissolution methods, including hydrofluoric acid, to recover uranium from the soil matrix. The failures illustrate the importance of rugged soil dissolution methods for the accurate measurement of analytes in the sample matrix. A new rapid fusion method has been developed by the Savannah River National Laboratory (SRNL) to prepare 1-2 g soil sample aliquots very quickly, with total dissolution of refractory particles. Soil samples are fused with sodium hydroxide at 600 ºC in zirconium crucibles to enable complete dissolution of the sample. Uranium and thorium are separated on stacked TEVA and TRU extraction chromatographic resin cartridges, prior to isotopic measurements by alpha spectrometry on cerium fluoride microprecipitation sources. Plutonium can also be separated and measured using this method. Batches of 12 samples can be prepared for measurement in <5 hours.

54 ENVIRONMENTAL SCIENCES↗

Defining Processing Times for Accelerator Produced 225Ac and Other Isotopes from Proton Irradiated Thorium

During the purification of radioisotopes, decay periods or time dependent purification steps may be required to achieve a certain level of radiopurity in the final product. Actinum-225 (Ac-225), Silver-111 (Ag-111), Astatine-211 (At-211), Ruthenium-105 (Ru-105), and Rhodium-105 (Rh-105) are produced in a high energy proton irradiated thorium target. Experimentally measured cross sections, along with MCNP6-generated cross sections, were used to determine the quantities of Ac-225, Ag-111, At-211, Ru-105, Rh-105, and other co-produced radioactive impurities produced in a proton irradiated thorium target at Brookhaven Linac Isotope Producer (BLIP). Ac-225 and Ag-111 can be produced with high radiopurity by the proton irradiation of a thorium target at BLIP.

07 ISOTOPE AND RADIATION SOURCES↗

Berkeley Low Background Facility

The Berkeley Low Background Facility (BLBF) at Lawrence Berkeley National Laboratory (LBNL) in Berkeley, California provides low background gamma spectroscopy services to a wide array of experiments and projects. The analysis of samples takes place within two unique facilities; locally within a carefully-constructed, low background laboratory on the surface at LBNL and at the Sanford Underground Research Facility (SURF) in Lead, SD. These facilities provide a variety of gamma spectroscopy services to low background experiments primarily in the form of passive material screening for primordial radioisotopes (U, Th, K) or common cosmogenic/anthropogenic products; active screening via neutron activation analysis for U,Th, and K as well as a variety of stable isotopes; and neutron flux/beam characterization measurements through the use of monitors. A general overview of the facilities, services, and sensitivities will be presented. Recent activities and upgrades will also be described including an overview of the recently installed counting system at SURF (recently relocated from Oroville, CA in 2014), the installation of a second underground counting station at SURF in 2015, and future plans. The BLBF is open to any users for counting services or collaboration on a wide variety of experiments and projects.

07 ISOTOPE AND RADIATION SOURCES↗

Description of alpha decay and cluster radioactivity in the dinuclear system model

A unified description of cluster radioactivity and α-decay of cold nuclei in the dinuclear system model is proposed. Quantum dynamical fluctuations along the charge (mass) asymmetry coordinate determine the spectroscopic factor, and tunneling along the relative distance coordinate determines the penetrability of the barrier of the nucleus–nucleus interaction potential. A new method for calculating the spectroscopic factor is proposed. The hindrance factors for the orbital angular momentum transfer are studied. A potential reason for the half-life to deviate from the Geiger–Nuttall law in α-decays of neutron-deficient nuclei {sup 194,} {sup 196}Rn is found. The fine structure of α-decays of U and Th isotopes is predicted and characterized. The model is used to describe α-decays from the rotational band of even–even nuclei. The known half-lives in the regions of “lead” and “tin” radioactivities are reproduced well, and the most probable cluster yields are predicted. The cluster decay of excited nuclei is discussed. The relation of cluster radioactivity to spontaneous fission and highly deformed nuclear states is analyzed.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

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

A new method has been developed for the isolation of 223,224,225 Ra, in high yield and purity, from a proton irradiated 232 Th 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 223,224,225 Ra 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 on previously measured excitation functions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the {sup 233}U isotope in the VVER reactors using thorium and heavy water

A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium–uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D{sub 2}O, H{sub 2}O) is proposed. The method is characterized by efficient breeding of the {sup 233}U isotope and safe reactor operation and is comparatively simple to implement.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Simultaneous Separation of Protactinium-230 and Uranium-230 Isotopes from a Proton-Irradiated Thorium Matrix

The use of radioisotopes in cancer therapy is becoming increasingly important. As a potential candidate for targeted alpha therapy, 230 U (t 1/2 = 20.8 d), the decay daughter of 230 Pa (t 1/2 = 17.4 d) is currently being investigated for cancer treatment. For radioisotopes to be used in biomedicine, they must be radiochemically pure and free from carrier interference. This can be challenging given their short half-life. Thus, in this study, radiological separation methods for harvesting isotopes for use in biomedicine must be simple, fast, and capable of obtaining the required purity levels. Herein, we demonstrate a new rapid method for the separation of 230 U and 230 Pa from a proton-irradiated 232 Th metal target and from coproduced fission products with high recovery and purity. A dual-column approach was used, in which the first column was an anion exchange (AX) column and the second column was a DGA column. The MP-1 AX resin was used for the primary separation of the three major components (U, Pa, and Th, as well as fission products), and the DGA column was used for further purification of the separated 230 U. The method is simple and allows for straightforward separation of U, Pa, Th, and fission products; also, the entire process from target dissolution to shipment of 230 U could be completed in 3 days with an overall 230 U recovery yield of 96 ± 3%. Additionally, separated 230 Pa fractions can be used to harvest ingrown 230 U after initial separation.

DGA resin↗

U.S. Department of Energy Isotope Program

The National Isotope Development Center (NIDC) interfaces with the User Community and manages the coordination of isotope production across the facilities and business operations involved in the production, sale, and distribution of isotopes. A virtual center, the NIDC is funded by the Isotope Development and Production for Research and Applications (IDPRA) subprogram of the Office of Nuclear Physics in the U.S. Department of Energy Office of Science. PNNL’s Isotope Program operates in a multi-program category-2 nuclear facility, the Radiochemical Processing Laboratory (RPL), that contains 16 hot cells and 20 gloveboxes. As part of the DOE Isotope Program, the Pacific Northwest National Laboratory dispenses strontium-90, neptunium-237, radium-223, and thorium-227. PNNL’s Isotope Program uses a dedicated hot-cell for strontium-90 dispensing and a dedicated glovebox for radium-223 and thorium-227 dispensing. PNNL’s Isotope Program has access to state of the art analytical equipment in the RPL to support their research and production activities. DOE Isotope Program funded research at PNNL has advanced the application of automated radiochemistry for isotope such as zirconium-89 and astatine-211 in partnership with the University of Washington.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Natural Transmutation of Actinides via the Fission Reaction in the Closed Thorium–Uranium–Plutonium Fuel Cycle

It is shown for a closed thorium–uranium–plutonium fuel cycle that, upon processing of one metric ton of irradiated fuel after each four-year campaign, the radioactive wastes contain ~54 kg of fission products, ~0.8 kg of thorium, ~0.10 kg of uranium isotopes, ~0.005 kg of plutonium isotopes, ~0.002 kg of neptunium, and “trace” amounts of americium and curium isotopes. This qualitatively simplifies the handling of high-level wastes in nuclear power engineering.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Th and U fuel photofission study by NTD for AD-MSR subcritical assembly

During the last decade a considerable effort has been devoted for developing energy generating systems based on advanced nuclear technology within the design concepts of GEN-IV. Thorium base fuel systems such as accelerator driven nuclear reactors are one of the often mentioned attractive and affordable options. Several radiotherapy linear accelerators are on the market and due to their reliability, they could be employed as drivers for subcritical liquid fuel assemblies. Bremsstrahlung photons with energies above 5.5MeV, induce (γ,n) and (e,e’n) reactions in the W-target. Resulting gamma radiation and photo or fission neutrons may be absorbed in target materials such as thorium and uranium isotopes to induce sustained fission or nuclear transmutation in waste radioactive materials. Relevant photo driven and photo-fission reaction cross sections are important for actinides {sup 232}Th, {sup 238}U and {sup 237}Np in the radiotherapy machines energy range of 10-20 MV. In this study we employ passive nuclear track detectors (NTD) to determine fission rates and neutron production rates with the aim to establish the feasibility for gamma and photo-neutron driven subcritical assemblies. To cope with these objectives a 20 MV radiotherapy machine has been employed with a mixed fuel target. Results will support further development for a subcritical assembly employing a thorium containing liquid fuel. It is expected that acquired technological knowledge will contribute to the Venezuelan nuclear energy program.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗