The harmonic generation process in a harmonic cascade (HC) FEL is subject to noise degradation which is proportional to the square of the total harmonic order. In this paper, we study the shot noise evolution in the first-stage modulator and radiator of a HC FEL that produces the dominant noise contributions. We derive the effective input noise for a modulator operating in the low-gain regime, and analyze the radiator noise for a density-modulated beam. The significance of these noise sources in different harmonic cascade designs is also discussed.

The principal goal of this project was to assess the molecular nature and stability of radionuclide immobilization during weathering reactions in bulk Hanford sediments and their high surface area clay mineral constitutents.

The principal goal of this project was to assess the molecular nature and stability of radionuclide immoblization during weathering reactions in bulk Hanford sediments and their high surface area clay mineral constituents. We focused on the unique aqueous geochemical conditions that are representative of waste-impacted locations in the Hanford site vadose zone; high ionic strength, high pH and high Al concentrations. The specific objectives of the work were to measure the coupling of clay mineral weathering and contaminant uptake kinetics of Cs, Sr and I; determine the molecular structure of contaminant binding sites and their change with weathering time during and after exposure to synthetic tank waste leachate; establish the stability of neoformed weathering products and their sequestered contaminbants upon exposure of the solids to more natural soil solutaions afer remofal of the caustic waste source; and integrate macroscopic, microscopic and spectroscopic data to distinguish labile from non-labile contaminant binding environments, including their dependence on system composition and weathering time.

X-ray absorption spectroscopy and electron energy loss spectroscopy are complementary analytical techniques on energy and spatial resolution. These techniques are based on the same fundamental physical process of core excitation with either an incident photon or incident electron. In the proper experimental configuration the electron and photon inelastic scattering amplitudes are comparable and thus the x-ray and electron absorption edges look identical. We have applied these two complementary analytical techniques to investigate the electronic structure of C ion implanted U. Implantation of C{sup +} ions into U{sup 238} has been shown to produce a physically and chemically modified surface layer that passivates the surface preventing further air oxidation and corrosion. Comparison of the resultant spectra reveal that transitions between the initial state and a series of final states yield numerous strong features at the absorption edge that can provide structural information and information on the local chemical environment, including the character of the U 5f state.

This report summarizes the research performed on the LDRD project 02-ERD-071 to develop a quantum-limited microwave amplifier based on a dc Superconducting Quantum Interference Device (dc-SQUID). This project began in June 2002 and concluded in May 2005. This project produced the lowest noise temperature amplifiers ever produced, both in absolute terms and in relation to the Standard Quantum Limit. Being an order of magnitude lower in noise than the best HFET devices available, they are of great interest to a number of groups. Potential applications are numerous, from dark-matter searches to national security applications in Quantum Information Processing. Collaborations started during this project are continuing with the goal of single-spin detection using the rf-SET. Publications are forthcoming covering both the experimental results and the theoretical modeling. The most important publication with the noise temperature results will appear after the low frequency follow-up experiment. The other publications in production cover the input impedance measurements and the resulting transmission line models.

The principal goal of this project was to assess the molecular nature and stability of radionuclide (137-Cs, 90-Sr, and 129-I) immobilization during weathering reactions in bulk Hanford sediments and their high surface area clay mineral constituents. We focused on the unique aqueous geochemical conditions that are representative of waste-impacted locations in the Hanford site vadose zone: high ionic strength, high pH and high Al concentrations. The specific objectives of the work were to (i) measure the coupling of clay mineral weathering and contaminant uptake kinetics of Cs+, Sr2+ and I-; (ii) determine the molecular structure of contaminant binding sites and their change with weathering time during and after exposure to synthetic tank waste leachate (STWL); (iii) establish the stability of neoformed weathering products and their sequestered contaminants upon exposure of the solids to more “natural” soil solutions (i.e., after removal of the caustic waste source); and (iv) integrate macroscopic, microscopic and spectroscopic data to distinguish labile from non-labile contaminant binding environments, including their dependence on system composition and weathering time. During this funding period, we completed a large set of bench-scale collaborative experiments and product characterization aimed at elucidating the coupling between mineral transformation reactions and contaminant sequestration/stabilization. Our experiments …

A magnetically coupled microbalance system has been used to measure adsorption and desorption isotherms and rates of desorption for carbon tetrachloride on dry prepared porous silica particles with narrow pore size distributions in the mesoporous range. Pore size distributions estimated from the carbon tetrachloride isotherms were found to be in close agreement with those determined using standard low temperature nitrogen adsorption. Three different types of particles were studied, with average pore diameters of 2.7 nm, 4.6 nm, and 5.9 nm. Prior to desorption rate studies, evacuated particulate samples were charged with volatile organic vapor at pressures sufficient to fill all mesopores with condensed fluid. Desorption rates into dry flowing helium were determined at 25 °C and atmospheric pressure, using the microbalance system combined with chromatographic analysis of the exit helium stream. Initial rates were found to decrease significantly, as mass adsorbed decreased. This residual mass was desorbing at such a low rate, that it can be considered a migration resistant fraction of the original mass adsorbed. Attempts to remove this residual mass at higher temperatures were partially successful; however, differences between the microbalance and gas chromatograph responses leave open uncertainty about whether the residual mass was pure carbon tetrachloride. To …

Fractional crystallization is being considered as a pretreatment method to support supplemental treatment of retrieved single-shell tank (SST) saltcake waste at the Hanford Site. The goal of the fractional crystallization process is to optimize the separation of the radioactivity (radionuclides) from the saltcake waste and send it to the Waste Treatment and Immobilization Plant and send the bulk of the saltcake to the supplemental treatment plant (bulk vitrification). The primary factors that influence the separation efficiency are (1) solid/liquid separation efficiency, (2) contaminant inclusions, and (3) co-precipitation. This is a report of testing for factors (2) and (3) with actual tank waste samples. For the purposes of this report, contaminant inclusions are defined as the inclusion of supernatant, containing contaminating radionuclides, in a pocket within the precipitating saltcake crystals. Co-precipitation is defined as the simultaneous precipitation of a saltcake crystal with a contaminating radionuclide. These two factors were tested for various potential fractional crystallization product salts by spiking the composite tank waste samples (SST Early or SST Late, external letter CH2M-0600248, ''Preparation of Composite Tank Waste Samples for ME-21 Project'') with the desired target salt and then evaporating to precipitate that salt. SST Early represents the typical composition of dissolved …

This document provides requirements, design, data-file specifications, test plan, and Quality Assurance/Quality Control protocol for the linkage between the statistical package R and the Framework for Risk Analysis in Multimedia Environmental Systems (FRAMES) Versions 1.x and 2.0. The requirements identify the attributes of the system. The design describes how the system will be structured to meet those requirements. The specification presents the specific modifications to FRAMES to meet the requirements and design. The test plan confirms that the basic functionality listed in the requirements (black box testing) actually functions as designed, and QA/QC confirms that the software meets the client’s needs.

Although significant progress has been achieved in understanding the genetic and biochemical bases of the spore germination process, the structural basis for breaking the dormant spore state remains poorly understood. We have used atomic force microscopy (AFM) to probe the high-resolution structural dynamics of single Bacillus atrophaeus spores germinating under native conditions. Here we show that AFM can reveal previously unrecognized germination-induced alterations in spore coat architecture and topology as well as the disassembly of outer spore coat rodlet structures. These results and previous studies in other microorganisms suggest that the spore coat rodlets are structurally similar to amyloid fibrils. AFM analysis of the nascent surface of the emerging germ cell revealed a porous network of peptidoglycan fibers. The results are consistent with a honeycomb model structure for synthetic peptidoglycan oligomers determined by nuclear magnetic resonance. AFM is a promising experimental tool for investigating the morphogenesis of spore germination and cell wall peptidoglycan structure.

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The microstructures and properties of powder metallurgy TiAl alloys fabricated by hot extrusion of gas-atomized powder at different elevated temperatures were investigated. Microstructure of the alloy fabricated at 1150 C consisted of a mixture of fine ({gamma} + {alpha}{sub 2}) equiaxed grains and coarse ordered B2 grains. Particles of ordered hexagonal {omega} phase were also observed in some B2 grains. The alloy containing B2 grains displayed a low-temperature superplastic behavior: a tensile elongation of 310% was measured when the alloy was tested at 800 C under a strain rate of 2 x 10{sup -5} s{sup -1}. Microstructure of the alloy fabricated at 1250 C consisted of a mixture of fine ({gamma} + {alpha}{sub 2}) equiaxed grains, coarse {alpha}{sub 2} grains, and lamellar ({gamma} + {alpha}{sub 2}) colonies. An observation of stacking faults associated with fine {gamma} lamellae in {alpha}{sub 2} grains reveals that the stacking fault of {alpha}{sub 2} phase plays an important role in the formation of lamellar ({gamma} + {alpha}{sub 2}) colonies. Unlike the alloy fabricated at 1150{sup o}, the alloy fabricated at 1250{sup o} displayed no low-temperature superplasticity, but a tensile elongation of 260% at 1000 C was measured. Microstructure of the alloy fabricated at 1400 C …

A salt solution (doped with Tc-99), that simulates the salt waste stream to be processed at the Saltstone Production Facility, was immobilized in grout waste forms with and without (1) ground granulated blast furnace slag and (2) pretreatment with iron salts. The degree of immobilization of Tc-99 was measured through monolithic and crushed grout leaching tests. Although Fe (+2) was shown to be effective in reducing Tc-99 to the +4 state, the strong reducing nature of the blast furnace slag present in the grout formulation dominated the reduction of Tc-99 in the cured grouts. An effective diffusion coefficient of 4.75 x 10{sup -12} (Leach Index of 11.4) was measured using the ANSI/ANS-16.1 protocol. The leaching results show that, even in the presence of a concentrated salt solution, blast furnace slag can effectively reduce pertechnetate to the immobile +4 oxidation state. The measured diffusivity was introduced into a flow and transport model (PORFLOW) to calculate the release of Tc-99 from a Saltstone Vault as a function of hydraulic conductivity of the matrix.

This report presents requirements for advanced simulation of nuclear reactor and chemical processing plants that are of interest to the Global Nuclear Energy Partnership (GNEP) initiative. Justification for advanced simulation and some examples of grand challenges that will benefit from it are provided. An integrated software tool that has its main components, whenever possible based on first principles, is proposed as possible future approach for dealing with the complex problems linked to the simulation of nuclear reactor and chemical processing plants. The main benefits that are associated with a better integrated simulation have been identified as: a reduction of design margins, a decrease of the number of experiments in support of the design process, a shortening of the developmental design cycle, and a better understanding of the physical phenomena and the related underlying fundamental processes. For each component of the proposed integrated software tool, background information, functional requirements, current tools and approach, and proposed future approaches have been provided. Whenever possible, current uncertainties have been quoted and existing limitations have been presented. Desired target accuracies with associated benefits to the different aspects of the nuclear reactor and chemical processing plants were also given. In many cases the possible gains associated …

Early projections of the Sludge Batch 4 (SB4) composition predicted relatively high concentrations of alumina (Al{sub 2}O{sub 3}, 23.5 wt%) and sulfate (SO{sub 4}{sup 2-}, 1.2 wt%) in the sludge. A high concentration of Al{sub 2}O{sub 3} in the sludge, combined with Na{sub 2}O additions in the frit, raises the potential for nepheline crystallization in the glass. However, strategic frit development efforts at the Savannah River National Laboratory (SRNL) have shown that frits containing a relatively high concentration of B{sub 2}O{sub 3} can both suppress nepheline crystallization and improve melt rates. A high sulfate concentration is a concern to the DWPF as it can lead to the formation of sulfate inclusions in the glass and/or the formation of a molten, sulfate-rich phase atop the melt pool. To avoid these issues, a sulfate concentration limit of 0.4 wt% SO{sub 4}{sup 2-} in glass was originally set in the Product Composition Control System (PCCS) used at DWPF. It was later shown that this limit could be increased to 0.6 wt% SO{sub 4}{sup 2-} in glass for the Frit 418, Sludge Batch 3 (SB3) system.

Our goal (see Project Objectives) is to deliver a dosimetry system which will enable both a Pu body burden of 0.3 kBq, and a 30 cGy {gamma} ray dose, to be separately estimated with a confidence limit of {+-}30%. In terms of the numbers analyzed and the data we have accrued, we have direct quantitative evidence that we are on track to providing such a comprehensive independent dosimetry system for Mayak workers. We had previously demonstrated that intra-chromosomal aberrations measured in peripheral blood lymphocytes can be used as a sensitive long-lived low-background quantitative biomarker of densely-ionizing radiation dose in individuals exposed many years ago. We propose to calibrate the system such that it can be used to estimate both the densely-ionizing internal plutonium exposure and the sparsely-ionizing external exposure in Mayak workers exposed to different combinations of these over a prolonged period, mostly many years ago. Our objective is to deliver a dosimetry system (set of calibration parameters) which will enable both a comparatively low Pu body burden of 0.3 kBq, and a comparatively low 30 cGy {gamma} ray dose (one of these or both of these) to be estimated with a confidence limit of {+-}30% (higher doses will of …