Highly concentrated, aqueous mullite slurries were characterized and stabilized at solids concentrations as high as 60 vol% using less than 2 vol% of an organic polyelectrolyte dispersant. The maximum slurry concentration (60 vol%) is within 3 vol% of the maximum consolidated density of the slurry. The slurries were subsequently cast into parts by a solid freeform fabrication technique termed robocasting and characterized. Sedimentation analysis and viscometry provided the means of slurry characterization, while knowledge of polyelectrolyte and interparticle forces was used to interpret the sedimentation and viscometry data. Through proper control of slurry conditions, pseudoplastic mullite slurries were fabricated for use in the robocasting process. The slurries were robocast at 52 vol% solids and subsequently yielded a green density of 55 vol%. Fired densities of the robocasted slurries were high, with mullite >96% dense at 1,650 C.
The authors use low energy electron microscopy to identify a correlation between the growth shape of three-dimensional Pb islands on Cu(100)and the domain structure of the underlying Pb overlayer. Deposition of 0.6 monolayer Pb on Cu(100) produces a compressed c(2x2) overlayer, designated c(5{radical}2x{radical}2)R45{degree}, with periodic rows of anti-phase boundaries. They found that heating the surface to temperatures above 100 C coarsens the orientational domains of this structure to sizes that are easily resolved in the low energy electron microscope. Three-dimensional Pb islands, grown on the coarsened domains, are found to be asymmetric with orientations that correlate with the domain structure. Once nucleated with a preferred growth orientation, islands continue to grow with the same preferred orientation, even across domain boundaries.
Atomistic computer simulation methods have been employed to model the structure of the (10{bar 1}4) surfaces of calcite, dolomite and magnesite. The authors calculations show that under vacuum conditions, calcite undergoes the greatest degree of surface relaxation with rotation and distortion of the carbonate group accompanied by movement of the calcium ion. The magnesite surface is the least distorted of the three carbonates, with dolomite being intermediate to the two end members. When water molecules are placed on the surface to produce complete monolayer coverage, the calcite surface is stabilized and the amount of relaxation is substantially reduced. In contrast, the dolomite and magnesite surfaces are destabilized by hydration as indicated by a significant increase in the surface energies relative to the dry surface.
The goal of this work is to develop techniques for measuring gradients in particle concentration within filled polymers, such as encapsulant. A high concentration of filler particles is added to such materials to tailor physical properties such as thermal expansion coefficient. Sedimentation and flow-induced migration of particles can produce concentration gradients that are most severe near material boundaries. Therefore, techniques for measuring local particle concentration should be accurate near boundaries. Particle gradients in an alumina-filled epoxy resin are measured with a spatial resolution of 0.2 mm using an x-ray beam attenuation technique, but an artifact related to the finite diameter of the beam reduces accuracy near the specimen's edge. Local particle concentration near an edge can be measured more reliably using microscopy coupled with image analysis. This is illustrated by measuring concentration profiles of glass particles having 40 {micro}m median diameter using images acquired by a confocal laser fluorescence microscope. The mean of the measured profiles of volume fraction agrees to better than 3% with the expected value, and the shape of the profiles agrees qualitatively with simple theory for sedimentation of monodisperse particles. Extending this microscopy technique to smaller, micron-scale filler particles used in encapsulant for microelectronic devices is illustrated by measuring the local concentration of an epoxy resin containing 0.41 volume fraction of silica.
Laser induced fluorescence was used to measure the spatially resolved CF, CF{sub 2} and SiF radical density in inductively driven discharges containing fluorocarbon gases. Measurements of the spatially resolved CF density were performed in C{sub 2}F{sub 6} and CHF{sub 3} containing discharges as functions of inductive power, pressure and bias condition on a silicon substrate. In addition, CF rotational temperatures were calculated, assuming saturated spectra. Measurements of the spatially resolved CF{sub 2} and SiF density were performed in C{sub 4}F{sub 8}, C{sub 2}F{sub 6} and CHF{sub 3} containing discharges as functions of inductive power, pressure and bias condition. SiF rotational temperatures were also estimated. As the induction coil power was increased, the SiF density in the center (r = 0 cm) increased while the CF{sub 2} density decreased and the CF density slightly decreased. In all cases, the radical density in the center of the glow increased with pressure changes from 5 to 30 mTorr while changes in the bias power had little influence on any of the measured radical densities. The spatial distribution of the CF and SiF density peaked in the center of the discharge. The CF{sub 2} density had a local maximum in the center of the plasma with a decreasing density at the edge of the glow. However, the CF{sub 2} density outside the glow region was a factor of 2--6 higher than the density inside the glow region, depending on the gas. CF and SiF rotational temperatures were between 450 and 750 K.
Algorithms developed to enable the use of atomistic molecular simulation methods with parallel computers are reviewed. Methods appropriate for bonded as well as non-bonded (and charged) interactions are included. While strategies for obtaining parallel molecular simulations have been developed for the full variety of atomistic simulation methods, molecular dynamics and Monte Carlo have received the most attention. Three main types of parallel molecular dynamics simulations have been developed, the replicated data decomposition, the spatial decomposition, and the force decomposition. For Monte Carlo simulations, parallel algorithms have been developed which can be divided into two categories, those which require a modified Markov chain and those which do not. Parallel algorithms developed for other simulation methods such as Gibbs ensemble Monte Carlo, grand canonical molecular dynamics, and Monte Carlo methods for protein structure determination are also reviewed and issues such as how to measure parallel efficiency, especially in the case of parallel Monte Carlo algorithms with modified Markov chains are discussed.
Development of a novel metal matrix composite based on the Al-B alloy system has been undertaken. Preparation of this discontinuously reinforced material is based on the precipitation of high aspect ratio AlB{sub 2} from an Al-B alloy. This paper describes a number of efforts forced on preparing high volume fractions (> 30 v%) of AlB{sub 2} in aluminum. New insights into the behavior of the Al-B alloys system allowed this effort to be successful.
Wire array Z-pinches on the Z accelerator provide the most intense laboratory source of soft x-rays in the world. The unique combination of a highly-Planckian radiation source with high x-ray production efficiency (15% wall plug), large x-ray powers and energies ( >150 TW, {ge}1 MJ in 7 ns), large characteristic hohlraum volumes (0.5 to >10 cm{sup 3}), and long pulse-lengths (5 to 20 ns) may make Z-pinches a good match to the requirements for driving high-yield scale ICF capsules with adequate radiation symmetry and margin. The Z-pinch driven hohlraum approach of Hammer and Porter [Phys.Plasmas, 6, 2129(1999)] may provide a conservative and robust solution to the requirements for high yield, and is currently being studied on the Z accelerator. This paper describes a multiple region, 0-d hohlraum energetic model for Z-pinch driven hohlraums in four configurations. The authors observe consistency between the models and the measured x-ray powers and hohlraum wall temperatures to within {+-}20% in flux, for the four configurations.
To address lithium-ion cell safety issues in demanding power applications, electrical and thermal abuse tests were performed on 18650 sized cells. Video and electrically monitored abuse tests in air included short circuit, forced overcharge, forced reversal, and controlled overheating (thermal) modes. Controlled overheating tests to 200 C were performed in a sealed chamber under a helium atmosphere and the gases released from the cell during thermal runaway were analyzed at regular intervals using gas chromatography and mass spectrometry. In addition to alkane and alkene solvent breakdown fragments, significant H{sub 2} was detected and evidence that HF was evolved was also found.
As part of a project for the Defense Advanced Research Projects Agency, Sandia National Laboratories Intelligent Systems and Robotics Center is developing and testing the feasibility of using a cooperative team of robotic sentry vehicles to guard a perimeter, perform a surround task, and travel extended distances. This paper describes the authors most recent activities. In particular, this paper highlights the development of a Differential Global Positioning System (DGPS) leapfrog capability that allows two or more vehicles to alternate sending DGPS corrections. Using this leapfrog technique, this paper shows that a group of autonomous vehicles can travel 22.68 kilometers with a root mean square positioning error of only 5 meters.
A molecular dynamics (MD) study of the lithium ultraphosphate glass series, xLi{sub 2}O{center_dot}(1{minus}x)P{sub 2}O{sub 5} (0 {le} x < 0.5) was used to investigate the changes in the Li environment with increasing modifier concentration. The results from the MD simulations indicate that no major structural variations in the Li coordination environment are observed. Changes in the type of oxygen coordinated to the modifier are observed and correlate with the T{sub g} minimum. Additionally, changes in the number of shared phosphorus vertices are observed with increasing modifier concentration, in support of recent models involving the role of the modifier in the extended range structure of phosphate glasses. Empirical calculations of the {sup 6}Li NMR chemical shifts directly from the MD simulation structures is also reported and compared to recent experimental solid-state NMR results.
A theoretical analysis of laser-driven collisional ejection of inner-shell electrons is presented to explain the previously observed anomalous kilovolt L-shell x-ray emission spectra from atomic Xe cluster targets excited by intense sub-picosecond 248nrn ultraviolet radiation. For incident ponderomotively-driven electrons photoionized by strong above threshold ionization, the collisional ejection mechanism is shown to be highly l-state and significantly n-state (i.e. radially) selective for time periods shorter than the collisional dephasing time of the photoionized electronic wavefunction. The resulting preference for the collisional ejection of 2p electrons by an ionized 4p state produces the measured anomalous Xe(L) emission which contains direct evidence for (i) the generation of Xe{sup 27+}(2p{sup 5}3d{sup 10}) and Xe{sup 28+}(2p{sup 5}3d{sup 9}) ions exhibiting inner-shell population inversion and (ii) a coherent correlated electron state collision responsible for the production of double 2p vacancies. For longer time periods, the selectivity of this coherent impact ionization mechanism is rapidly reduced by the combined effects of intrinsic quantum mechanical spreading and dephasing--in agreement with the experimentally observed and extremely strong {minus}{lambda}{sup {minus}6} pump-laser wavelength dependence of the efficiency of inner-shell (2p) vacancy production in Xe clusters excited in underdense plasmas.
A highly selective, coherent impact ionization mechanism is proposed for the efficient generation of inner-shell population inversion in laser-driven plasmas. The theoretical analysis is consistent with observed L-shell (2p{l_arrow}3d) emission spectra from laser-excited Xe clusters.
We report an evaporation-induced self-assembly procedure to prepare poly(bridged silsesquioxane) thin-film and particulate mesophases that incorporate organic moieties (1-3) into periodic, mesostructured frameworks as molecularly dispersed bridging ligands. Capacitance-voltage measurements along with a variety of structural characterization procedures were performed to begin to elucidate structure-property relationships of this new class of surfactant-templated mesophases. We observed a consistent trend of increasing modulus and hardness and decreasing dielectric constant with substitution of the bridged silsesquioxane (≡Si-(CH2)2-Si≡) for siloxane (≡Si-O-Si≡) in the framework. This preliminary evidence suggests that the introduction of integral organic groups into the frameworks of mesoporous materials can result in synergistic properties, promising an unprecedented ability to tune properties and function.
The need for a telerobotic vehicle with hazard sensing and integral manipulation capabilities has been identified for use in transportation accidents where nuclear weapons are involved. The Accident Response Mobile Manipulation System (ARMMS) platform has been developed to provide remote dexterous manipulation and hazard sensing for the Accident Response Group (ARG) at Sandia National Laboratories. The ARMMS' mobility platform is a military HMMWV [High Mobility Multipurpose Wheeled Vehicle] that is teleoperated over RF or Fiber Optic communication channels. ARMMS is equipped with two high strength Schilling Titan II manipulators and a suite of hazardous gas and radiation sensors. Recently, a modular telerobotic control architecture call SMART (Sandia Modular Architecture for Robotic and Teleoperation) has been applied to ARMMS. SMART enables input devices and many system behaviors to be rapidly configured in the field for specific mission needs. This paper summarizes current SMART developments applied to ARMMS.
A series of arylalcohols [H-OAr where OAr = OC{sub 6}H{sub 5} (OPh), OC{sub 6}H{sub 4}(2-Me) (oMP), OC{sub 6}H{sub 3}(2,6-Me){sub 2} (DMP), OC{sub 6}H{sub 4}(2-Pr{prime}) (oPP), OC{sub 6}H{sub 3}(2,6-Pr{prime}){sub 2} (DIP), OC{sub 6}H{sub 4}(2-Bu{prime}) (oBP), OC{sub 6}H{sub 3}(2,6-Bu{prime}){sub 2} (DBP) where Me = CH{sub 3}, Pr{prime} = CHMe{sub 2}, and Bu{prime} = CMe{sub 3}] were reacted with LiN(SiMe{sub 3}){sub 2} in pyridine (py) to generate the appropriate ``Li(OAr)(py){sub x}'' complex. The resultant products were characterized by single crystal X-ray diffraction as: [Li(OPh)(py){sub 2}]{sub 2} (1), [Li(oMP)(py){sub 2}]{sub 2} (2), [Li(DMP)(py){sub 2}]{sub 2} (3), [Li(oPP)(py){sub 2}]{sub 2} (4), [Li(DIP)(py){sub 2}]{sub 2} (5), [Li(oBP)(py){sub 2}]{sub 2} (6), and [Li(DBP)(py)]{sub 2} (7). Compounds 1--6 adopt a dinuclear, edge-shared tetrahedral complex. For 7, due to the steric crowding of the DBP ligand, only one py is coordinated yielding a dinuclear fused trigonal planar arrangement. Two additional structure types were also characterized for the DIP ligand as [Li(DIP)(H-DIP)(py)]{sub 2} (5b) and [Li{sub 2}(DIP){sub 2}(py){sub 3}] (5c). {sup 6,7}Li and {sup 13}C NMR solid state MAS spectroscopy indicated that the bulk powder was consistent with the crystalline material. Solution state NMR spectroscopy revealed a symmetric molecule existed in solution for 1--7.
Mechanical and hydrological properties of salt provide excellent bases for geological isolation of hazardous materials. Regulatory certification of the Waste Isolation Pilot Plant (WIPP) testifies to the nearly ideal characteristics of bedded salt deposits in southeast New Mexico. The WIPP history includes decades of testing and scientific investigations, which have resulted in a comprehensive understanding of salt's mechanical deformational and hydrological properties over an applicable range of stresses and temperatures. Comprehensive evaluation of salt's favorable characteristics helped demonstrate regulatory compliance and ensure isolation of radioactive waste placed in a salt geological setting.
Selectively oxidized vertical cavity lasers emitting at 1294 nm using InGaAsN quantum wells are reported for the first time which operate continuous wave at and above room temperature. The lasers employ two n-type Al{sub 0.94}Ga{sub 0.06}As/GaAs distributed Bragg reflectors each with a selectively oxidized current aperture adjacent to the optical cavity, and the top output mirror contains a tunnel junction to inject holes into the active region. Continuous wave single mode lasing is observed up to 55 C. These lasers exhibit the longest wavelength reported to date for vertical cavity surface emitting lasers grown on GaAs substrates.
The United States Department of Energy initiated the Nuclear Energy Research Initiative (NERI) to conduct research and development with the objectives of: (1) overcoming the principal technical obstacles to expanded nuclear energy use, (2) advancing the state of nuclear technology to maintain its competitive position in domestic and world markets, and (3) improving the performance, efficiency, reliability, and economics of nuclear energy. Fiscal Year 1999 program funding is $19 Million, with increased finding expected for subsequent years, emphasizing international cooperation. Among the programs selected for funding is the ``Smart Equipment and Systems to Improve Reliability and Safety in Future Nuclear Power Plant Operations''. This program is a 30 month collaborative effort bringing together the technical capabilities of ABB C-E Nuclear Power, Inc. (ABB CENP), Sandia National Laboratories, Duke Engineering and Services (DE and S), Massachusetts Institute of Technology (MIT) and Pennsylvania State University (PSU). The program's goal is to design, develop and evaluate an integrated set of smart equipment and predictive maintenance tools and methodologies that will significantly reduce nuclear plant construction, operation and maintenance costs. To accomplish this goal the Smart Equipment program will: (1) Identify and prioritize nuclear plant equipment that would most likely benefit from adding smart features; (2) Develop a methodology for systematically monitoring the health of individual pieces of equipment implemented with smart features (i.e. smart equipment); (3) Develop a methodology to provide plant operators with real-time information through smart equipment Man-Machine Interfaces (MMI) to support their decision making; (4) Demonstrate the methodology on a targeted component and/or system; (5) Expand the concept to system and plant levels that allow communication and integration of data among smart equipment. This paper will discuss (1) detailed subtask plans for the entire program, including expected achievements, (2) preliminary results from the early program phases and (3) the program's relationship to other NERI programs being conducted by the same team.
Backfills have been part of Sandia National Laboratories' [Sandia's] Waste Isolation Pilot Plant [WIPP] designs for over twenty years. Historically, backfill research at Sandia has depended heavily on the changing mission of the WIPP facility. Early testing considered heat producing, high level, wastes. Bentonite/sand/salt mixtures were evaluated and studies focused on developing materials that would retard brine ingress, sorb radionuclides, and withstand elevated temperatures. The present-day backfill consists of pure MgO [magnesium oxide] in a pelletized form and is directed at treating the relatively low contamination level, non-heat producing, wastes actually being disposed of in the WIPP. Its introduction was motivated by the need to scavenging CO{sub 2} [carbon dioxide] from decaying organic components in the waste. However, other benefits, such as a substantial desiccating capacity, are also being evaluated. The MgO backfill also fulfills a statutory requirement for assurance measures beyond those needed to demonstrate compliance with the US Environmental Protection Agency [EPA] regulatory release limits. However, even without a backfill, the WIPP repository design still operates within EPA regulatory release limits.