High-resolution spectroscopy of hot tokamak plasma seeded with argon ions and interacting with an energetic, short-pulse neutral hydrogen beam was used to obtain the first high-resolution K-shell x-ray spectrum formed solely by charge exchange. The observed K-shell emission of Ar{sup 16+} is dominated by the intercombination and forbidden lines, providing clear signatures of charge exchange. Results from an ab initio atomic cascade model provide excellent agreement, validating a semiclassical approach for calculating charge exchange cross sections.

A new version of the Community Climate System Model (CCSM) has been developed and released to the climate community. CCSM3 is a coupled climate model with components representing the atmosphere, ocean, sea ice, and land surface connected by a flux coupler. CCSM3 is designed to produce realistic simulations over a wide range of spatial resolutions, enabling inexpensive simulations lasting several millennia or detailed studies of continental-scale climate change. This paper will show results from the configuration used for climate-change simulations with a T85 grid for atmosphere and land and a 1-degree grid for ocean and sea-ice. The new system incorporates several significant improvements in the scientific formulation. The enhancements in the model physics are designed to reduce or eliminate several systematic biases in the mean climate produced by previous editions of CCSM. These include new treatments of cloud processes, aerosol radiative forcing, land-atmosphere fluxes, ocean mixed-layer processes, and sea-ice dynamics. There are significant improvements in the sea-ice thickness, polar radiation budgets, equatorial sea-surface temperatures, ocean currents, cloud radiative effects, and ENSO teleconnections. CCSM3 can produce stable climate simulations of millenial duration without ad hoc adjustments to the fluxes exchanged among the component models. Nonetheless, there are still systematic biases in …

Advanced Technology Systems, Inc. (ATS), with Desert Research Institute (DRI) and Ohio University as subcontractors, was contracted by the NETL in September 1998 to manage the Upper Ohio River Valley Project (UORVP), which included the establishment and operation of four ambient air monitoring sites located in the Upper Ohio River Valley (UORV). Two urban and two rural monitoring sites were included in the UORVP. The four sites selected for the UOVRP were collocated at existing local or state air quality monitoring stations. The goal of the UORVP was to characterize the nature and composition of PM{sub 2.5} and its precursor gases. In the process, the objectives of the UORVP were to examine the ambient air concentrations of PM{sub 2.5} as compared with the promulgated PM{sub 2.5} standards, the geographical, seasonal and temporal variations of ambient air concentrations of PM{sub 2.5}, the primary chemical constituents of PM{sub 2.5}, and the correlations between ambient air concentrations of PM{sub 2.5} and its precursor gases, other gaseous pollutants and meteorological parameters. A variety of meteorological and pollutant measurement devices, including several different PM{sub 2.5} samplers that provided either real-time or integrated concentration data, were deployed at the monitoring sites. The frequency of integrated sampling …

Safe disposal of the nation's nuclear waste in a geological repository involves unique scientific and engineering challenges owing to the very long-lived radioactivity of the waste. The repository must retain a variety of radionuclides that have vastly different chemical characters for several thousand years. Most of the radioactivity that will be housed in the proposed repository at Yucca Mountain will be associated with spent nuclear fuel, much of which is derived from commercial reactors. DOE is custodian of approximately 8000 tons of spent nuclear fuel that is also intended for eventual disposal in a geological repository. Unlike the spent fuel from commercial reactors, the DOE fuel is diverse in composition with more than 250 varieties. Safe disposal of spent fuel requires a detailed knowledge of its long-term behavior under repository conditions, as well as the fate of radionuclides released from the spent fuel as waste containers are breached.

This document describes soil sampling that will be performed by Pacific Northwest National Laboratory's Surface Environmental Surveillance Project on two units of the Hanford Reach National Monument: the McGee Ranch-Riverlands Unit (Riverlands Unit) and the North Slope made up of the Saddle Mountain Unit and the Wahluke Slope Unit. This sampling fulfills a U.S. Department of Energy requirement to evaluate the potential for residual radioactive contamination on this land and determine compliance with the requirements of DOE Order 5400.5 prior to radiological release of the property.

The collapse of the Soviet Union sparked fears throughout the world that rogue nations and terrorist organizations would gain access to weapons of mass destruction (WMD). One specific concern has been 'WMD brain drain.' Russians with knowledge about nuclear, chemical, and biological weapons could now depart to any country of their choice, including rogue nations seeking to produce WMD. Meanwhile, Russian science fell into a protracted crisis, with plummeting salaries, little funding for research, and few new recruits to science. These developments increased both the incentives and the opportunities for scientists to sell their knowledge to governments and terrorist organizations with hostile intentions toward the United States. Recognizing the threat of WMD brain drain from Russia, the United States, and other governments implemented a host of programs designed to reduce the risk. Despite, or perhaps partly because of, massive assistance from the West to prevent scientists with WMD knowledge from emigrating, the threat of Russian WMD brain drain has recently faded from view. Yet we have seen no evidence that these programs are effective and little systematic assessment of the current threat of WMD migration. Our data from an unprecedented survey of 602 Russian physicists, biologists, and chemists suggest that …

The purpose of this cooperative research and development agreement (CRADA) between Sasol North America, Inc., and the oak Ridge National Laboratory (ORNL) was to improve the stability of alumina-based industrial catalysts through the combination of aberration-corrected scanning transmission electron microscopy (STEM) at ORNL and innovative sample preparation techniques at Sasol. Outstanding progress has been made in task 1, 'Atomistic processes of La stabilization'. STEM investigations provided structural information with single-atom precision, showing the lattice location of La dopant atoms, thus enabling first-principles calculations of binding energies, which were performed in collaboration with Vanderbilt University. The stabilization mechanism turns out to be entirely due to a particularly strong binding energy of the La tom to the {gamma}-alumina surface. The large size of the La atom precludes incorporation of La into the bulk alumina and also strains the surface, thus preventing any clustering of La atoms. Thus highly disperse distribution is achieved and confirmed by STEM images. la also affects relative stability of the exposed surfaces of {gamma}-alumina, making the 100 surface more stable for the doped case, unlike the 110 surface for pure {gamma}-alumina. From the first-principles calculations, they can estimate the increase in transition temperature for the 3% loading of …

Although the phylogenetic relationships of many organisms have been convincingly resolved by the comparisons of nucleotide or amino acid sequences, others have remained equivocal despite great effort. Now that large-scale genome sequencing projects are sampling many lineages, it is becoming feasible to compare large data sets of genome-level features and to develop this as a tool for phylogenetic reconstruction that has advantages over conventional sequence comparisons. Although it is unlikely that these will address a large number of evolutionary branch points across the broad tree of life due to the infeasibility of such sampling, they have great potential for convincingly resolving many critical, contested relationships for which no other data seems promising. However, it is important that we recognize potential pitfalls, establish reasonable standards for acceptance, and employ rigorous methodology to guard against a return to earlier days of scenario-driven evolutionary reconstructions.

Supramolecular chemistry represents a way to mimic enzyme reactivity by using specially designed container molecules. We have shown that a chiral self-assembled M{sub 4}L{sub 6} supramolecular tetrahedron can encapsulate a variety of cationic guests, with varying degrees of stereoselectivity. Reactive iridium guests can be encapsulated and the C-H bond activation of aldehydes occurs, with the host cavity controlling the ability of substrates to interact with the metal center based upon size and shape. In addition, the host container can act as a catalyst by itself. By restricting reaction space and preorganizing the substrates into reactive conformations, it accelerates the sigmatropic rearrangement of enammonium cations.

This report addresses the advancement of the ion beam thin film planarization process for the smoothing of substrate particles.

Solid state nuclear magnetic resonance techniques have been used to investigate aging mechanisms in a vinyl chloride:chlorotrifluoroethylene copolymer, FPC-461, due to exposure to {gamma}-radiation. Solid state {sup 1}H MAS NMR spectra revealed structural changes of the polymer upon irradiation under both air and nitrogen atmospheres. Considerable degradation is seen with {sup 1}H NMR in the vinyl chloride region of the polymer, particularly in the samples irradiated in air. {sup 19}F MAS NMR was used to investigate speciation in the chlorotrifluoroethylene blocks, though negligible changes were seen. {sup 1}H and {sup 19}F NMR at elevated temperature revealed increased segmental mobility and decreased structural heterogeneity within the polymer, yielding significant resolution enhancement over room temperature solid state detection. The effects of multi-site exchange are manifest in both the {sup 1}H and {sup 19}F NMR spectra as a line broadening and change in peak position as a function of temperature.

We have previously described our methodology for quantification of risk and risk reduction, and the use of risk, quantified as a dollar value, in the Value Engineering and decision tradeoff process. In this work we extend our example theme of the safety of reactive materials during accidental impacts. We have begun to place the validation of our impact safety model into a systems engineering context. In that sense, we have made connections between the data and the trends in the data, our models of the impact safety process, and the implications regarding confidence levels and reliability based on given impact safety requirements. We have folded this information into a quantitative risk assessment, and shown the assessed risk reduction value of developing an even better model, with more model work or more experimental data or both. Since there is a cost incurred for either model improvement or testing, we have used a Benefit/Cost Ratio metric to quantify this, where Benefit is our quantification of assessed risk reduction, and cost is the cost of the new test data, code development, and model validation. This has left us with further questions posed for our evolving system engineering representation for impact safety and its …

Comparison of mutation spectra at the hypoxanthine-phosphoribosyl transferase (HPRT) gene of peripheral blood T lymphocytes may provide insight into the aetiology of somatic mutation contributing to carcinogenesis and other diseases. To increase knowledge of mutation spectra in healthy people, we have analyzed HPRT mutant T-cells of 50 healthy Russians originally recruited as controls for a study of Chernobyl clean-up workers (Jones et al. Radiation Res. 158, 2002, 424). Reverse transcriptase polymerase chain reactions and DNA sequencing identified 161 independent mutations among 176 thioguanine resistant mutants. Forty (40) mutations affected splicing mechanisms and 27 deletions or insertions of 1 to 60 nucleotides were identified. Ninety four (94) single base substitutions were identified, including 62 different mutations at 55 different nucleotide positions, of which 19 had not previously been reported in human T-cells. Comparison of this base substitution spectrum with mutation spectra in a USA (Burkhart-Schultz et al. Carcinogenesis 17, 1996, 1871) and two Swedish populations (Podlutsky et al, Carcinogenesis 19, 1998, 557, Podlutsky et al. Mutation Res. 431, 1999, 325) revealed similarity in the type, frequency and distribution of mutations in the four spectra, consistent with aetiologies inherent in human metabolism. There were 15-19 identical mutations in the three pair-wise comparisons …

Z-pinch dynamic hohlraum experiments on the Z-Machine at Sandia National Laboratories measured K-shell argon spectra using a focusing spectrometer with spatial resolution. The spectra are modeled using Hullac atomic data input, Cretin nonlocal thermodynamic equilibrium (nlte) atomic kinetics and radiative transfer calculations, and Dakota optimization capabilities. Hullac provides atomic structure and cross section data for Ar XIX, Ar XXVIII (n=1 (illegible) 5), Ar XXVII (n=1 (illegible) 10), and Ar XXVI (n=1 (illegible) 5), where n is the principal quantum number. Cretin calculates the area-integrated spectral intensity escaping an argon doped Dcapsule as a function of electron density, electron temperature, and capsule radius. Dakota optimizes the plasma properties for the best to the measured spectrum by minimizing an objective function comprise of argon spectral line ratios and full-width at half-maximums (fwhms). We highlight the framework of this general spectroscopic capability and discuss the extension to magnetized plasmas using Totalb spectral line shapes.

Tellurium doped AlGaAsSb epitaxial layers were grown lattice-matched on GaSb substrates and lattice-mismatched on semi-insulating GaAs substrates by organometallic vapor phase epitaxy. Secondary ion mass spectroscopy and Hall data showed that the ratio of carrier concentration to Te concentration decreases from 40% to 5% when the Te concentration increases from 4.8 x 10{sup 17} cm{sup -3} to 1.3 x 10{sup 19} cm{sup -3}. Transmission electron microscopy (TEM) showed that the material with heavily doped Te generates a high density (about 10{sup 8} cm{sup 2}) of planar defects. Most of the Te-related defects originate at the GaSb buffer layer/AlGaAsSb epilayer interface. In addition, discrete precipitates were observed in the heavily doped AlGaAsSb layer. TEM imaging revealed amorphous defects (likely residual native oxides) along the GaSb substrate/GaSb buffer interface. High resolution TEM imaging revealed high quality growth beyond the GaSb-buffer/GaSb-substrate interfacial defects. The microstructural impact of GaSb-buffer/GaSb-substrate interface defects on the crystalline quality of AlGaAsSb layers is insignificant.

The purpose of this analysis report is to evaluate and document the inclusion or exclusion of biosphere features, events, and processes (FEPs) with respect to modeling used to support the total system performance assessment (TSPA) for the license application (LA). A screening decision, either ''Included'' or ''Excluded'', is given for each FEP along with the corresponding technical basis for the excluded FEPs and the descriptions of how the included FEPs were incorporated in the biosphere model. This information is required by the U.S. Nuclear Regulatory Commission (NRC) regulations at 10 CFR 63.114 (d, e, and f) [DIRS 156605]. The FEPs addressed in this report concern characteristics of the reference biosphere, the receptor, and the environmental transport and receptor exposure pathways for the groundwater and volcanic ash exposure scenarios considered in biosphere modeling. This revision provides the summary of the implementation of included FEPs in TSPA-LA, (i.e., how the FEP is included); for excluded FEPs, this analysis provides the technical basis for exclusion from TSPA-LA (i.e., why the FEP is excluded). This report is one of the 10 documents constituting the biosphere model documentation suite. A graphical representation of the documentation hierarchy for the biosphere model is presented in Figure 1-1. …

Because fossil fuel fired power plants are among the largest and most concentrated producers of CO{sub 2} emissions, recovery and sequestration of CO{sub 2} from the flue gas of such plants has been identified as one of the primary means for reducing anthropogenic CO{sub 2} emissions. In this Phase II study, ALSTOM Power Inc. (ALSTOM) has investigated one promising near-term coal fired power plant configuration designed to capture CO{sub 2} from effluent gas streams for sequestration. Burning fossil fuels in mixtures of oxygen and recirculated flue gas (made principally of CO{sub 2}) essentially eliminates the presence of atmospheric nitrogen in the flue gas. The resulting flue gas is comprised primarily of CO{sub 2}, along with some moisture, nitrogen, oxygen, and trace gases like SO{sub 2} and NO{sub x}. Oxygen firing in utility scale Pulverized Coal (PC) fired boilers has been shown to be a more economical method for CO{sub 2} capture than amine scrubbing (Bozzuto, et al., 2001). Additionally, oxygen firing in Circulating Fluid Bed Boilers (CFB's) can be more economical than in PC or Stoker firing, because recirculated gas flow can be reduced significantly. Oxygen-fired PC and Stoker units require large quantities of recirculated flue gas to maintain acceptable …

The project aim was the improvement, evaluation, and application of one dimensional (1D) inversion and development and application of three dimensional (3D) inversion to processing of data collected at waste pits at the Idaho National Engineering and Environmental Laboratory. The inversion methods were intended mainly for the Very Early Time Electromagnetic (VETEM) system which was designed to improve the state-of-the-art of electromagnetic imaging of the shallow (0 to about 5m) subsurface through electrically conductive soils.

This project is directed at a fundamental understanding of hydrogen bonding, the primary reversible interaction leading to defined geometries, networks and supramolecular aggregates formed by organic molecules. Hydrogen bonding is still not sufficiently well understood that the geometry of such supramolecular aggregates can be predicted. In the approach taken existing quantum chemical methods capable of treating periodic solids have been applied to hydrogen bonded systems of known structure. The equilibrium geometry for the given space group and packing arrangement were computed and compared to that observed. The second derivatives and normal modes of vibration will then be computed and from this inelastic neutron scattering (INS) spectra were computed using the normal mode eigenvectors to compute spectral intensities. Appropriate inclusion of spectrometer line width and shape was made in the simulation and overtones, combinations and phonon wings were be included. These computed spectra were then compared with experimental results obtained for low-temperature polycrystalline samples at INS spectrometers at several facilities. This procedure validates the computational methodology for describing these systems including both static and dynamic aspects of the material. The resulting description can be used to evaluate the relative free energies of two or more proposed structures and so ultimately to …

We present a method for computing a basis of localized orthonormal orbitals (both occupied and virtual), in whose representation the Fock matrix is extremely diagonal-dominant. The existence of these orbitals is shown empirically to be sufficient for achieving highly accurate MP@ energies, calculated according to Kapuy's method. This method (which we abbreviate KMP2), which involves a different partitioning of the n-electron Hamiltonian, scales at most quadratically with potential for linearity in the number of electrons. As such, we believe the KMP2 algorithm presented here could be the basis of a viable approach to local correlation calculations.

First, we review earlier studies reporting possible magnetic characteristics for radiation defects in Pu. We then report, for {alpha}-Pu, two studies of the excess magnetic susceptibility (EMS) due to radiation damage, as a function of time and temperature. We have observed several annealing stages associated with the EMS of the accumulated self-damage and we report that annealing begins at {approx}31K, while below that temperature the displacement damage from self-irradiation of the Pu alpha particle emission and the U recoil are immobile. A detailed investigation was made of this EMS well below the first annealing stage as a function of temperature (2K < T < 15K) and time in a magnetic field of 2T. A linear increase in magnetic susceptibility is seen as a function of time for all isotherms. The excess susceptibility per alpha decay, determined from a linear fit of the slope of the time dependent EMS, is reasonably described with a Curie-Weiss law exhibiting a small negative Weiss temperature. We conclude by describing some future experiments in light of the present results.

The A-01 wetland treatment system (WTS) was designed to remove metals from the effluent at the A-01 NPDES outfall at the Savannah River Site, Aiken, SC. Sequential extraction data was used to evaluate remobilization and retention of Cu, Pb, Zn, Mn, and Fe in the wetland sediment. Remobilization of metals was determined by the Potentially Mobile Fraction (PMF) and metal retention by the Recalcitrant Factor (RF). The PMF, which includes water soluble, exchangeable, and oxides fractions, is the contaminant fraction that has the potential to enter into the mobile aqueous phase under changeable environmental conditions. PMF values were low for Cu, Zn and Pb (about 20 percent) and high for Fe and Mn (about 60 to 70 percent). The RF, which includes crystalline oxides, sulfides or silicates and aluminosilicates, is the ratio of strongly bound fractions to the total concentration of elements in sediment. RF values were about 80 percent for Cu, Zn and Pb, indicating high retention in the sediment and 30 percent to above 40 percent for Fe and Mn indication low retention.

We present now a possible way to carry out soft-x-rayfluorescence spectroscopy of liquids. The liquid cell has a window toattain compatibility with UHV conditions of the spectrometer andbeamline, The synchrotron radiation enters the liquid cell through a 100nm-thick silicon nitride window and the emitted xrays exit through thesame window. This allows in particular liquid solid interfaces to bestudied. Such a liquid cell has been used to study the electronicstructure of a variety of systems ranging from water solutions ofinorganic salts and inertial drugs to nano materials and actinidecompounds in their wet conditions.

The purpose of the saturated zone (SZ) flow and transport model abstraction task is to provide radionuclide-transport simulation results for use in the total system performance assessment (TSPA) for license application (LA) calculations. This task includes assessment of uncertainty in parameters that pertain to both groundwater flow and radionuclide transport in the models used for this purpose. This model report documents the following: (1) The SZ transport abstraction model, which consists of a set of radionuclide breakthrough curves at the accessible environment for use in the TSPA-LA simulations of radionuclide releases into the biosphere. These radionuclide breakthrough curves contain information on radionuclide-transport times through the SZ. (2) The SZ one-dimensional (I-D) transport model, which is incorporated in the TSPA-LA model to simulate the transport, decay, and ingrowth of radionuclide decay chains in the SZ. (3) The analysis of uncertainty in groundwater-flow and radionuclide-transport input parameters for the SZ transport abstraction model and the SZ 1-D transport model. (4) The analysis of the background concentration of alpha-emitting species in the groundwater of the SZ.