The King County Wastewater Treatment Division (WTD) have concern about the aftermath of a radiological dispersion event (RDE) leading to the introduction of significant quantities of radioactive material into its combined sanitary and storm sewer system. Radioactive material could come from the use of a radiological dispersion device (RDD). RDDs include "dirty bombs" that are not nuclear detonations but are explosives designed to spread radioactive material. Radioactive material also could come from deliberate introduction or dispersion of radioactive material into the environment, including waterways and water supply systems. Volume 2 of PNNL-15163 assesses the radiological instrumentation needs for detection of radiological or nuclear terrorism, in support of decisions to treat contaminated wastewater or to bypass the West Point Treatment Plant (WPTP), and in support of radiation protection of the workforce, the public, and the infrastructure of the WPTP. Fixed radiation detection instrumentation should be deployed in a defense-in-depth system that provides 1) early warning of significant radioactive material on the way to the WPTP, including identification of the radionuclide(s) and estimates of the soluble concentrations, with a floating detector located in the wet well at the Interbay Pump Station and telemetered via the internet to all authorized locations; 2) monitoring …

The U.S. Department of Energy Advanced Fuel Cycle Initiative (AFCI) is sponsoring a project at Oak Ridge National Laboratory with the objective of conducting the research and development necessary to evaluate the use of sphere-pac transmutation fuel. Sphere-pac fuels were studied extensively in the 1960s and 1970s. More recently, this fuel form is being studied internationally as a potential plutonium-burning fuel. For transmutation fuel, sphere-pac fuels have potential advantages over traditional pellet-type fuels. This report provides a review of development efforts related to the preparation of sphere-pac fuels and their irradiation tests. Based on the results of these tests, comparisons with pellet-type fuels are summarized, the advantages and disadvantages of using sphere-pac fuels are highlighted, and sphere-pac options for the AFCI are recommended. The Oak Ridge National Laboratory development activities are also outlined.

The movement of high-specific-activity radioactive particles (i.e., alpha recoil) has been observed and studied since the early 1900s. These studies have been motivated by concerns about containment of radioactivity and the protection of human health. Additionally, studies have investigated the potential advantage of alpha recoil to effect separations of various isotopes. This report provides a review of the observations and results of a number of the studies.

Although computer simulation has played a central role in the study of nucleation and growth since the earliest molecular dynamics simulations almost 50 years ago, confusion surrounding the effect of finite size on such simulations have limited their applicability. Modeling solidification in molten tantalum on the BlueGene/L computer, we report here on the first atomistic simulation of solidification that verifies independence from finite size effects during the entire nucleation and growth process, up to the onset of coarsening. We show that finite size scaling theory explains the observed maximal grain sizes for systems up to about 8,000,000 atoms. For larger simulations, a cross-over from finite size scaling to more physical size-independent behavior is observed.

The sterically demanding 1,2,4-tri-t-butylcyclopentadienylligand (1,2,4-(Me3C)3C5H2, hereafter Cp') has been used to preparemonomeric cerium metallocenes, Cp 2CeX (X = Cl, I, OSO2CF3), which areused to synthesize the benzyl, Cp'2CeCH2C6H5. The benzyl is a usefulstarting material for preparing other complexes in the Cp'2CeZ system (Z= BF4, F, NH2, C6H5, H). X-ray crystal structures of Cp'2CeOSO2CF3,Cp'2CeF, Cp'2CeCH2C6H5, and Cp'2CeH are presented. The benzyl slowlydecomposes in solution to toluene and a metallacycle,[Cp'][(Me3C)2C5H2(CMe2CH2)]Ce. The ring CMe3 groups of both themetallacycle and the hydride, Cp'2CeH, can be fully deuterated byprolonged exposure to C6D6, providing a useful labeling tool inmechanistic studies.The hydride activates C-F and/or C-H bonds influorobenzenes, C6HxF6-x , x = 0-5. The reactions are selective, with theselectivity depending on the presence of two fluorines ortho to thereaction site more than on the type of bond activated. Complexes of thetype Cp'2CeC6HxF5-x , x = 0-4, are formed as intermediates, which slowlydecompose in solution to Cp'2CeF and fluorobenzynes, C6HxF4-x, x = 0-4,which are trapped. The rate at which Cp'2CeC6HxF5-x complexes decomposeincreases as the number of fluorines decreases. Complexes with oneortho-fluorine decompose much faster than those with two ortho-fluorines.The metallacycle activates only C-H bonds in fluorobenzenes, permittingthe synthesis of specific Cp'2CeC6HxF5-x complexes. The crystal structureof Cp'2CeC6F5 is presented. …

An investigation was undertaken of the effect of gamma radiation on metastable pitting of mild carbon steels immersed in a solution similar to those existing at high level waste (HLW) deposits in the US. The object was to observe the extent to which a dosage rate of 1 Mrad/hour (10 Kgrey/hour) affected measurable electrochemical parameters such as pitting potential, open circuit potential, rate of metastable pitting and repassivation potential. Methods for reliably measuring electrochemical potentials in a high radiation field were developed. Exploratory analyses were made of the ion product release and electrolyte composition change in a confined volume simulating the conditions of a corrosion initiated pit during gamma irradiation. As expected the results indicated that the metastable pitting rate (as well as the general rate of corrosion) was significantly enhanced by a radiation field.

With support from this award we studied a novel silicon microtexturing process and its application in silicon-based infrared photodetectors. By irradiating the surface of a silicon wafer with intense femtosecond laser pulses in the presence of certain gases or liquids, the originally shiny, flat surface is transformed into a dark array of microstructures. The resulting microtextured surface has near-unity absorption from near-ultraviolet to infrared wavelengths well below the band gap. The high, broad absorption of microtextured silicon could enable the production of silicon-based photodiodes for use as inexpensive, room-temperature multi-spectral photodetectors. Such detectors would find use in numerous applications including environmental sensors, solar energy, and infrared imaging. The goals of this study were to learn about microtextured surfaces and then develop and test prototype silicon detectors for the visible and infrared. We were extremely successful in achieving our goals. During the first two years of this award, we learned a great deal about how microtextured surfaces form and what leads to their remarkable optical properties. We used this knowledge to build prototype detectors with high sensitivity in both the visible and in the near-infrared. We obtained room-temperature responsivities as high as 100 A/W at 1064 nm, two orders of magnitude …

Natural convection plays an important role in determining the thermal load from molten core accumulated in the reactor vessel lower head during a severe accident. Several numerical and experimental programs were conducted to study the heat transfer in the molten pool. Previous investigations were mostly related to the rectangular and semicircular pools. Except for COPO, UCLA, ACOPO, and BALI, previous investigations suffer from inadequate representation of high modified Rayleigh number (Ra') in the hemispherical pool that may be formed in the reactor core and lower plenum. Thus, experimental work is conducted utilizing SIGMA SP (Simulant Internal Gravitated Material Apparatus Spherical Pool) producing high Ra' turbulent natural convection in a hemispherical pool up to 5.3 x ~1011. The heating method has already been tested in SIGMA CP (Circular Pool). Six thin cable-type heaters, each with a diameter of 6 mm, are employed to simulate internal heating in the pool. They are uniformly distributed in the hemispherical pool to supply a maximum of 7.8 kW power to the pool. SIGMA SP has the inner and outer diameters of 500 mm and 520 mm, respectively. The upper flat plate and the curved wall of pool, with a 10 mm thick stainless steel plate, …

Nature's inherent ability to cleanse itself is at the heart of Monitored Natural Attenuation (MNA). The complexity comes when one attempts to measure and calculate this inherent ability, called the Natural Attenuation Capacity (NAC), and determine if it is sufficient to cleanse the system to agreed upon criteria. An approach that is simple in concept for determining whether the NAC is sufficient for MNA to work is the concept of a mass balance. Mass balance is a robust framework upon which all decisions can be made. The inflows to and outflows from the system are balanced against the NAC of the subsurface system. For MNA to be acceptable, the NAC is balanced against the contaminant loading to the subsurface system with the resulting outflow from the system being in a range that is acceptable to the regulating and decision-making parties. When the system is such that the resulting outflow is not within an acceptable range, the idea of taking actions that are sustainable and that will bring the system within the acceptable range of outflows is evaluated. These sustainable enhancements are being developed under the Enhanced Attenuation (EA) concept.

PLEIADES (Picosecond Laser Electron Interaction for the Dynamic Evaluation of Structures) produces tunable 30-140 keV x-rays with 0.3-5 ps pulse lengths and up to 10{sup 7} photons/pulse by colliding a high brightness electron beam with a high power laser. The electron beam is created by an rf photo-injector system, accelerated by a 120 MeV linac, and focused to 20 {micro}m with novel permanent magnet quadrupoles. To produce Compton back scattered x-rays, the electron bunch is overlapped with a Ti:Sapphire laser that delivers 500 mJ, 100 fs, pulses to the interaction point. K-edge radiography at 115 keV on Uranium has verified the angle correlated energy spectrum inherent in Compton scattering and high-energy tunability of the Livermore source. Current upgrades to the facility will allow laser pumping of targets synchronized to the x-ray source enabling dynamic diffraction and time-resolved studies of high Z materials. Near future plans include extending the radiation energies to >400 keV, allowing for nuclear fluorescence studies of materials.