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At least 991 records · Page 55

Fuel cycle for a fusion neutron source

The concept of a tokamak-based stationary fusion neutron source (FNS) for scientific research (neutron diffraction, etc.), tests of structural materials for future fusion reactors, nuclear waste transmutation, fission reactor fuel production, and control of subcritical nuclear systems (fusion–fission hybrid reactor) is being developed in Russia. The fuel cycle system is one of the most important systems of FNS that provides circulation and reprocessing of the deuterium–tritium fuel mixture in all fusion reactor systems: the vacuum chamber, neutral injection system, cryogenic pumps, tritium purification system, separation system, storage system, and tritium-breeding blanket. The existing technologies need to be significantly upgraded since the engineering solutions adopted in the ITER project can be only partially used in the FNS (considering the capacity factor higher than 0.3, tritium flow up to 200 m{sup 3}Pa/s, and temperature of reactor elements up to 650°C). The deuterium–tritium fuel cycle of the stationary FNS is considered. The TC-FNS computer code developed for estimating the tritium distribution in the systems of FNS is described. The code calculates tritium flows and inventory in tokamak systems (vacuum chamber, cryogenic pumps, neutral injection system, fuel mixture purification system, isotope separation system, tritium storage system) and takes into account tritium loss in the fuel cycle due to thermonuclear burnup and β decay. For the two facility versions considered, FNS-ST and DEMO-FNS, the amount of fuel mixture needed for uninterrupted operation of all fuel cycle systems is 0.9 and 1.4 kg, consequently, and the tritium consumption is 0.3 and 1.8 kg per year, including 35 and 55 g/yr, respectively, due to tritium decay.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

AXAF Detector Backgrounds Produced By Cosmic Ray Protons

One of the science instruments on the Advanced X-ray Astrophysics Facility (AXAF), planned for launch in 1998 into a highly elliptical (10,000 km x 140,000 km) orbit, is a microchannel plate High Resolution Camera (HRC). This detector is designed to provide imaging and spectroscopic observations of x-rays emitted by stellar sources in the 0.1 to 10 keV energy range. Described here are analyses made to determine the expected time-dependent detector background from prompt and delayed (activation) radiation initiated by galactic cosmic-ray (GCR) proton interactions in the spacecraft and payload. Numerical simulations were made using the coupled set of Monte Carlo radiation transport codes, analysis software, and data bases shown. The major codes are HETC for nucleon-meson transport, EGS for simulating electromagnetic cascades, and MORSE for low-energy (less than 15 MeV) neutron transport. The simulation follows the transport history of photons in the energy range from - 100 GeV down to approx. 0.1 keV due to gamma-ray sources from neutral pion decay, high-energy (spallation) collisions, and low-energy neutron inelastic scattering and capture reactions. Also included is radioisotope production and the tracking of gamma-rays, electrons, and positrons from induced radioactivity.

Armstrong, T. W.↗

Radiation Induced Redox Chemistry of Californium-249

A complete understanding of californium chemistry necessitates knowledge of its radiation induced redox behavior, owing to its inherent nuclear instability propagating self-radiolysis. Only a handful of studies have investigated californium radiation chemistry, due to lack of availability and difficulty associated with handling highly radioactive material. To date, reaction rate coefficients have only been experimentally determined for the reduction of Cf(III) by the hydrated electron (e¯aq, k > 3 × 109 M–1 s–1), and subsequent decay of the corresponding transient Cf(II) (k = (7 ± 1) × 105 s–1)[1]. However, there are a number of other important transient radiolysis products radiolytically generated in solutions pertinent to Cf manipulations, e.g. the hydrogen atom (H•, Eo = 2.31 V), hydroxyl radical (•OH, Eo = –2.73 V), and nitrate radical (NO3•, Eo = –2.3 – –2.6 V). These species are more than capable of influencing the redox behavior of Cf, and have been shown to do so with a number of actinides, e.g. neptunium and americium. Here we present a time-resolved picosecond pulsed electron irradiation study for californium-249.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Influence of surface potential on the adhesive force of radioactive gold surfaces

Radioactive particles may acquire surface potential through self-charging, and thus can behave differently from natural aerosols in atmospheric systems with respect to aggregation, deposition, resuspension, and transport to areas surrounding a radioactive source. Here, this work focuses on the adhesive force between radioactive particles and metallic surfaces, which relates to the deposition and resuspension of particles on surrounding surfaces. Scanning surface potential microscopy was employed to measure the surface potential of radioactive gold foil. Atomic force microscopy was used to investigate the adhesive force for gold that acquired surface charge either by irradiation or by application of an equivalent electrical bias. Overall, the adhesive force increases with increasing surface potential or relative humidity. However, a behavior that does not follow the general trend was observed for the irradiated gold at a high decay rate. A comparison between experimental measurements and calculated values revealed that the surface potential promotes adhesion. The contribution of the electrostatic force at high levels of relative humidity was lower than the one found using theoretical calculations due to the effects caused by enhanced adsorption rate of water molecules under a high surface charge density. Lastly, the results of this study can be used to provide a better understanding of the behavior of radioactive particles in atmospheric systems.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DECOVALEX-2015: an international collaboration for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems

Here, an important part of the performance and safety assessment of disposal systems for radioactive waste and spent nuclear fuel in deep geological formations is to evaluate the impact of the coupled effects of mechanical deformation, fluid and gas flow through the repository, and thermal loading from the decaying waste. It was recognized early on in safety and performance assessments conducted for geologic disposal sites that to be able to conduct such an evaluation, there was a need to rigorously enhance the theoretical background and to develop models capable of simulating coupled thermo-hydro-mechanical (THM) processes. More recently, chemical processes have also been added to enable the study of fully coupled THMC processes in geosystems.

58 GEOSCIENCES↗

Reconstructing the direction of reactor antineutrinos via electron scattering in Gd-doped water Cherenkov detectors

The potential of elastic antineutrino-electron scattering (ν¯ e + e – → ν¯ e + e – ) in a Gd-doped water Cherenkov detector to determine the direction of a nuclear reactor antineutrino flux was investigated using the recently proposed WATCHMAN antineutrino experiment as a baseline model. The expected scattering rate was determined assuming a 13 km standoff from a 3.758 GWt light water nuclear reactor. Background was estimated via independent simulations and by appropriately scaling published measurements from similar detectors. Many potential backgrounds were considered, including solar neutrinos, misidentified reactor-based inverse beta decay interactions, cosmogenic radionuclide and water-borne radon decays, and gamma rays from the photomultiplier tubes, detector walls, and surrounding rock. The detector response was modeled using a GEANT4-based simulation package. The results indicate that with the use of low radioactivity PMTs and sufficient fiducialization, water-borne radon and cosmogenic radionuclides pose the largest threats to sensitivity. The directional sensitivity was then analyzed as a function of radon contamination, detector depth, and detector size. Lastly, the results provide a list of theoretical conditions that, if satisfied in practice, would enable nuclear reactor antineutrino directionality in a Gd-doped water Cherenkov detector approximately 10 km from a large power reactor.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Fusion reaction 48 Ca+ 249 Bk leading to formation of the element Ts (Z = 117)

The heaviest currently known nuclei, which have up to 118 protons, have been produced in 48 Ca induced reactions with actinide targets. Among them, the element tennessine (Ts), which has 117 protons, has been synthesized by fusing 48 Ca with the radioactive target 249 Bk, which has a half-life of 327 d. The experiment was performed at the gas-filled recoil separator TASCA. In this work, two long and two short α decay chains were observed. The long chains were attributed to the decay of 294 Ts. The possible origin of the short-decay chains is discussed in comparison with the known experimental data. They are found to fit with the decay chain patterns attributed to 293 Ts. The present experimental results confirm the previous findings at the Dubna Gas-Filled Recoil Separator on the decay chains originating from the nuclei assigned to Ts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Silicon-Equivalent Neutron Dose Estimations

Radiation transport calculations are often used to estimate dose or exposure to components and personnel surrounding a radiation source. The sources for these calculations are decaying radionuclides within the various nuclear materials. Under long-term radiation exposure, some components may show signs of material damage such as hardening, cracking, discoloration, etc. resulting from the dose received from nearby radioactive sources. Radiation dose quantities are a useful means to correlate material damage or degradation to radiation interactions. The degradation is often dependent on how incident radiation interacts and deposits energy into the material. This dependence implies that radiation dose should be properly defined for the material effect of interest. Generic dose quantities, such as total energy deposited, may not necessarily correlate well for degradation of any given material.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Distribution Development for Residual Inventory at the New York West Valley Site - 20400

The New York State Energy Research and Development Authority (NYSERDA) is the owner of the Western New York Nuclear Service Center (WNYNSC), a 1,351 ha site located approximately 48 km south of Buffalo, New York. In 1962, Nuclear Fuel Services, Inc. (NFS) entered into Agreements with the Atomic Energy Commission and New York State to construct the first commercial reprocessing plant of nuclear fuel in the United States. NFS, a private company, built and operated the spent fuel reprocessing plant and waste disposal facilities, processing 640 Mg of spent nuclear fuel from 1966 to 1972 under an Atomic Energy Commission license. Nuclear fuel reprocessing operations ended in 1972 and never reopened, leaving behind radioactive and chemical wastes. Operations led to contamination in a number of facilities and locations. Some of that contamination has migrated from waste disposal zones to other layers, formations, and features on and off the WNYNSC. Phase I decommissioning activities are ongoing and involve the removal of a number of areas and structures that have been associated with contamination. The purpose of this work is to outline the approach for characterizing contamination not associated with disposed wastes, contaminated structures, or specific releases. In this work, the term, residual radiological activity, is used to describe environmental contamination that exists subsequent to the completion of Phase I decommissioning activities, that is not associated with disposed wastes, contaminated structures, or specific releases. Contamination from the Site was quantified relative to data that characterize the concentrations of radionuclides that exist in background. Background concentrations are those present in the area but having no influence from Site related activities. The existence of residual radiological activity that is elevated relative to background has the potential to contribute to future risks to human health and the environment. As a consequence, the residual inventory information is used to inform the West Valley Probabilistic Performance Assessment (PPA) model to characterize potential future risks to human health and the environment. The centralized West Valley Data Management System (DMS) was the source of information for the data assembled in this analysis. The DMS is a fairly large compilation consisting of thousands of records from investigation studies, with sample dates ranging from 1990 to present. Samples from monitoring wells, boreholes, geoprobe studies, surface water, surface soils, storm water outfalls, ventilation stack filters, plant and animal tissues, and more are included in the DMS. Results are typically reported in units of activity per unit volume. For the purpose of the analyses presented here, all results were converted into consistent units of pCi per unit volume. Since 1990, data have been collected from various locations across the WNYNSC at different times with varying frequency over the course of several decades. As a consequence, a number of potential issues can arise with respect to the assembly of a dataset that is deemed adequate for the characterization of residual radiological activity. These issues were assessed and resolved to the extent possible through careful consideration of the properties of the distributions. The intent was to use data which characterize the current state of the Site. Radionuclides can be designated to one of several groups depending on their origin. In this work the groups considered were 1) Naturally Occurring Radioactive Material (NORM), 2) fallout, and 3) Other (including power plant, medical research, etc). This grouping is a useful construct with respect to the interpretation of fixed laboratory results. For example, NORM radionuclides that exist within a decay chain should have approximately equivalent distributions of concentrations if they are representative of background conditions. Insights such as these can be used as a check to identify sample results that need to be further investigated or omitted due to issues associated with reported results from fixed laboratory analyses. This type of analysis provided a foundation for the assessment of the adequacy of sample results for use in subsequent components of an assessment. The general process for the assessment of residual radiological contamination at the Site consists of a sequence of several steps. First, for each analyte, several statistical tests were performed to assess the weight of evidence against the null hypothesis that the mean of the distribution of concentrations was equal to zero. If the mean of the distribution of concentrations for a given radionuclide was not found to be greater than zero, then it was removed from consideration as a component of the residual radiological contamination. If there was significant evidence to reject the hypothesis of the mean being equal to zero, the second step was to compare the distribution of the data from the Site to that of the corresponding background. A suite of tests was used to compare the distributions of the site and background data. The results of these tests were collectively used to determine if site data are elevated relative to background. The third step was to develop distributions using a Bayesian framework to characterize the distribution of mean of the increment present above background for each of the radionuclides. The Bayesian model implemented allowed for the comparison of site-specific records to background concentrations to better approximate contamination attributed to the Site. A final screening step was employed for radionuclides that exceed background. This screening step compared 95% upper confidence limits (UCLs) from the increment distribution developed in the previous step to the risk screening levels. This approach yields a list of analytes that were determined to be elevated relative to background.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Joint IAEA/NNSA International Workshop Nuclear Forensics Methodologies for Practitioners 2013 Scenario Based Exercise – Version 4.0 Instructor’s Manual

[Participants will serve as border guards for Reimerland. They will be given brief instruction on the operation of hand-held RadioIsotope DetectorS (RIDS) and be provided an intelligence briefing that tells them to be on the lookout for suspicious activity at their post. Their instruction will include directing suspicious vehicles to a location for secondary screening. If, after secondary screening, suspicions of a criminal act involving nuclear and or radioactive materials remain, participants have been instructed to request assistance from the NLEA, who will then setup and manage a radiological crime scene. Participants will watch a demonstration of two vehicles containing radioactive materials driving through and setting off a portal monitor. The first vehicle, a semi-tractor trailer, sets off only a gamma alarm. After the driver provides a shipping manifest of fertilizer, participants, posing as border guards, are expected to waive this vehicle through inspection. The second vehicle, an SUV, set off both gamma and 2 neutron alarms. The alarming of the neutron monitor should prompt participants to set up a secondary inspection of the vehicle immediately. The driver of the vehicle indicates he is in legal possession of an industrial instrument containing an old 133Ba source that has decayed to a level no longer requiring official paperwork according to the IAEA and internationally accepted transportation regulations. Authorities have verified that the industrial source does fit the description of one that is sold commercially. However, upon setting up a secondary screening, participants will use hand-held detectors to locate several other radioactive sources emanating from a black duffle bag in the rear of the vehicle (Figure 1). Hand held detectors detect the presence of 133Ba, and Pu. Upon questioning, the driver only commits to having the 133Ba industrial source and cannot account for the detection of neutrons within his vehicle. Since neutron alarms also sounded, participants should indicate that a neutron alarm would be inconsistent with a 133Ba source alone and should therefore conclude further investigation is warranted. This will prompt participants to call in a response team from the NLEA to set up a radiological crime scene around the vehicle in question. The response team is able to shoot a 3-D X-ray radiograph of the duffle bag without moving it to ensure it is rendered safe and moveable without disturbing the contents in the field (Figure 2). At this point, the duffle bag is entered into inventory as evidence and a chain of custody form is initiated. Swipes are taken from the outer bag to confirm there is no dispersible contamination. The bag and its contents are considered valuable for the investigation by the lead investigator. He determines the duffle bag is safe to transport to RRL for evidence inventory and analysis. The duffle bag and its contents are packaged and sent off to the RRL.]

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

In-gas-jet laser spectroscopy with S 3 -LEB

The Super Separator Spectrometer-Low Energy Branch (S 3 -LEB) is a low-energy radioactive ion beam experiment under commissioning as part of the GANIL-SPIRAL2 facility. It will be used for the production and study of exotic nuclei by in-gas laser ionization and spectroscopy (IGLIS), decay spectroscopy, and mass spectrometry. Here, we report recent results from the off-line commissioning of S 3 -LEB, including first laser spectroscopy measurements in both the gas cell and the supersonic gas jet, the determination of the transport efficiency of laser ions from the gas cell through the RFQ chain, and time-of-flight measurements with the multi-reflection time-of-flight mass spectrometer PILGRIM. The measurements were performed using erbium, introduced by evaporation from a heated filament in the gas environment. The reported laser spectroscopy results include a characterization of the pressure broadening in the gas cell, proof-of-principle isotope shift measurements, and hyperfine-structure measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radioactive 7Be materials flown on LDEF

Following the discovery of the atmospheric cosmogenic radionuclide Be-7 on the Long Duration Exposure Facility (LDEF), we began a search for other known nuclides produced by similar mechanisms. None of the others have the narrow gamma-ray line emission of Be-7 decay which enable its rapid detection and quantification. A search for Be-10 atoms on LDEF clamp plates using accelerator mass spectrometry is described. An unexpected result was obtained.

Gregory, John C.↗

Topmetal CMOS direct charge sensing plane for neutrinoless double-beta decay search in high-pressure gaseous TPC

We propose a novel charge sensing concept for high-pressure Time Projection Chamber (TPC) to search for Neutrinoless Double-Beta Decay (NLDBD) with ton-scale isotope mass and beyond. A meter-sized plane, tiled with an array of CMOS integrated sensors called Topmetal that directly collect charge without gas avalanche gain, is to be deployed into a high-pressure gaseous TPC with working gases containing suitable NLDBD candidate isotopes such as Xe-136 and Se-82. The Topmetal sensor has an electronic noise <30 e- per pixel, which allows the detector to reach <1% FWHM energy resolution at the NLDBD Q-value for both Xe-136 and 82SeF6 gases by measuring ionization charges alone. The elimination of charge avalanche gain allows the direct sensing of slow-drifting ions, which enables the use of highly electronegative gas SeF6 in which free electrons do not exist. It supports the swapping of working gases without hardware modification, which is a unique way to validate signals against radioactive backgrounds. Since the sensor manufacturing and plane assembling could leverage unaltered industrial mass-production processes, stability, uniformity, scalability, and cost-effectiveness that are required for ton-scale experiments could all be reached. The strengths of TPC such as 3D ionization tracking and decay daughter tagging are retained. This development could lead to a competitive NLDBD experiment at and above ton-scale. The conceptual considerations, simulations, and initial prototyping are discussed.

Mei, Yuan↗

Bubble Formation and Lattice Parameter Changes Resulting from He Irradiation of Defect-Fluorite Gd2Zr2O7

Pyrochlores have long been considered as potential candidates for advanced ceramic waste-forms for the immobilization of radioactive waste nuclides. This work provides evidence that Gd2Zr2O7, often considered the most radiation tolerant pyrochlore, could be susceptible to radiation damage in the form of bubble nucleation at the highest He doses expected over geological time. Ion irradiations were utilized to experimentally simulate the radiation damage and He accumulation produced by ..alpha..-decay. Samples were pre-damaged using 7 MeV Au3+ to induce the pyrochlore to defect-fluorite phase transformation, which would occur due to ..alpha..-recoil damage within several hundred years of storage in a Gd2Zr2O7 waste-form. These samples were then implanted to various He concentrations in order to study the long-term effects of He accumulation. Helium bubbles 1-3 nm in diameter were observed in TEM at a concentration of 4.6 at.% He. Some bubbles remained isolated, while others formed chains 10-30 nm in length parallel to the surface. GIXRD measurements showed lattice swelling after irradiating pristine Gd2Zr2O7 with 7 MeV Au3+ to a fluence of 2.2 x 1015 Au/cm2. An increase in lattice swelling was also measured after 2.2 x 1015 Au/cm2 + 2 x 1015 He/cm2 and 2.2 x 1015 Au/cm2 + 2 x 1016 He/cm2. A decrease in lattice swelling was measured after irradiation with 2.2 x 1015 Au/cm2 + 2 x 1017 He/cm2, the fluence where bubbles and bubble chains were observed in TEM. Bubble chains are thought to form in order to reduce lattice strain normal to the surface, which is produced by the Au and He irradiation damage.

36 MATERIALS SCIENCE↗

Detection and quantification of trace technetium in the presence of molybdenum using laser-induced breakdown spectroscopy

Technetium (Tc) is a very important element that is encountered in many aspects, from its presence in radioactive waste and its potential environmental impact to its use as a medical radioisotope. Its detection and quantification in liquid samples is traditionally cumbersome, involving detailed sample preparation and analysis by mass spectrometry or scintillation. This article demonstrates the first comprehensive emission spectral analysis of Tc from a liquid sample by immobilization in a polymer and analysis by laser-induced breakdown spectroscopy (LIBS). A survey of LIBS spectra was completed to identify the strongest analytical lines for quantification of trace Tc in the presence of Mo. The quantification of Tc in a Mo-containing matrix was selected because Tc radioisotopes are the daughter products of Mo isotope decay. The first reported calibration curves by LIBS are provided with limits of detection and quantification down to 0.710 µg mL −1 and 1.39 µg mL −1 , respectively. Ultimately, this study demonstrated the feasibility of trace Tc quantification using LIBS and will serve as a reference for future research related to monitoring this radioactive species.

Andrews, Hunter B. [Oak Ridge National Laboratory ↗

Radon induced surface contaminations in low background experiments

In neutrinoless double-beta decay and dark matter searches, one of the main issues is to increase the experimental sensitivity through careful material selection and production, minimizing the background contributions. In order to achieve the required, extremely low, counting rates, very stringent requirements must be fulfilled in terms of bulk material radiopurity. As the experimental sensitivity increases, the bulk impurities in the detector components decrease, and surface contaminations start to play an increasingly significant role In fully active detectors, like cryogenic particle detectors, surface contaminations are a critical issue (as shown by the CUORICINO experiment). {sup 222}Rn is by far the most intense source of airborne radioactivity, and if a radio-pure material is exposed to environment where the Radon concentration is not minimized, {sup 210}Pb and {sup 210}Po contaminations can occur. The mechanisms and the dynamics of Radon-induced surface contaminations are reviewed, and specific solutions to prevent and to reject the induced background are presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Purification of lanthanides for double beta decay experiments

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 oxide 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.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗