A complete, isostructural series of lanthanide complexes (except Pm) with the ligand TREN-1,2-HOIQO has been synthesized and structurally characterized by means of single-crystal X-ray analysis. All complexes are 1D-polymeric species in the solid state, with the lanthanide being in an eight-coordinate, distorted trigonal-dodecahedral environment with a donor set of eight unique oxygen atoms. This series constitutes the first complete set of isostructural lanthanide complexes with a ligand of denticity greater than two. The geometric arrangement of the chelating moieties slightly deviates across the lanthanide series, as analyzed by a shape parameter metric based on the comparison of the dihedral angles along all edges of the coordination polyhedron. The apparent lanthanide contraction in the individual Ln-O bond lengths deviates considerably from the expected quadratic decrease that was found previously in a number of complexes with ligands of low denticity. The sum of all bond lengths around the trivalent metal cation, however, is more regular, showing an almost ideal quadratic behavior across the entire series. The quadratic nature of the lanthanide contraction is derived theoretically from Slater's model for the calculation of ionic radii. In addition, the sum of all distances along the edges of the coordination polyhedron show exactly the same …

A variety of laser-material interaction experiments have been conducted at Lawrence Livermore National Laboratory (LLNL) utilizing the solid-state heat capacity laser (SSHCL). For these series of experiments, laser output power is 25kW, on-target laser spot sizes of up to 16 cm by 16 cm square, with air speeds of approximately 100 meters per second flowing across the laser-target interaction surface as shown in Figure 1. The empirical results obtained are used to validate our simulation models.

Soft X-ray imager mirrors have been designed, calibrated and fabricated at Lawrence Livermore National Laboratory and characterized at the Advanced Light Source for their performance between 200 and 1300 eV. The mirrors are coated with a multilayer coating consisting of 70 bilayers of W/ SiC. The mirrors are to reflect at 22.5 deg from grazing angle at 1.50 nm wavelength and the width of the reflectivity peak should be at least 1.3%. Also, the mirrors should be non-reflective elsewhere. Our multilayer design was optimized to satisfy these requirements. The coating is very challenging since the individual layer thicknesses need to be less than 1 nm thick and reproducibility from layer to layer is crucial. To minimize the second harmonic peak we designed a multilayer with {Gamma} = 0.5 (W and SiC layer thicknesses are the same). This way we end up with a mirror that has only the 1st and 3rd harmonic peak as shown in Figure 1. To suppress reflectivity outside the first peak we used our novel approach, an antireflective coating. Modeling predicted substantial reduction in reflectivity, especially for lower energies as shown in Figure 1. The experimental results of the soft x-ray imager mirror as measured at …

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The general goal of this report is to diminish concentrations of metals/radionuclide in groundwaters of contaminated sites to below MCL values through reduction to lower solubility species.

We present a summary of the hadronic cross section measurements performed with BABAR at the PEP-II collider via radiative return. BABAR has performed measurements of exclusive final states containing 3, 4 and 6 hadrons via this complementary method, as well as a measurement of the proton form factor.

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Effective environmental management of DOE sites requires reliable prediction of reactive transport phenomena. A central issue in prediction of subsurface reactive transport is the impact of multiscale physical, chemical, and biological heterogeneity. Heterogeneity manifests itself through incomplete mixing of reactants at scales below those at which concentrations are explicitly defined (i.e., the numerical grid scale). This results in a mismatch between simulated reaction processes (formulated in terms of average concentrations) and actual processes (controlled by local concentrations). At the field scale, this results in apparent scale-dependence of model parameters and inability to utilize laboratory parameters in field models. Accordingly, most field modeling efforts are restricted to empirical estimation of model parameters by fitting to field observations, which renders extrapolation of model predictions beyond fitted conditions unreliable. The objective of this project is to develop a theoretical and computational framework for (1) connecting models of coupled reactive transport from pore-scale processes to field-scale bioremediation through a hierarchy of models that maintain crucial information from the smaller scales at the larger scales; and (2) quantifying the uncertainty that is introduced by both the upscaling process and uncertainty in physical parameters. One of the challenges of addressing scale-dependent effects of coupled processes in …

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Remediation and long-term stewardship of uranium-contaminated sediments and groundwaters are critical problems at a number of DOE facilities and mining sites. Some remediation strategies based on in-situ bioreduction of U are potentially effective in significantly decreasing U concentrations in groundwaters. However, a number of basic processes require understanding in order to identify conditions more conducive to success of reduction-based U stabilization. Our current research targets several of these issues including: (1) effects of organic carbon (OC) forms and supply rates on stability of bioreduced U, (2) the roles of Fe(III)- and Mn(III,IV)-oxides as potential U oxidants in sediments, and (3) microbial community changes in relation to U redox changes. These issues were identified in our previous study on U bioreduction and reoxidation (Wan et al., 2005). Most of our studies are being conducted on historically U-contaminated sediments from Area 2 of the Field Research Center, Oak Ridge National Laboratory, in flow-through columns simulating in-situ field remediation.

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We propose a model for 1/f flux noise in superconducting devices (f is frequency). The noise is generated by the magnetic moments of electrons in defect states which they occupy for a wide distribution of times before escaping. A trapped electron occupies one of the two Kramers-degenerate ground states, between which the transition rate is negligible at low temperature. As a result, the magnetic moment orientation is locked. Simulations of the noise produced by a plausible density of randomly oriented defects yield 1/f noise magnitudes in good agreement with experiments.

This report summarizes work performed for a larger multi-laboratory project named the Background Interferent Measurement and Standards project. While originally tasked to develop algorithms to optimize biological warfare agent detection using UV fluorescence LIDAR, the current uncertainties in the reported fluorescence profiles and cross sections the development of any meaningful models. It was decided that a better approach would be to model the wavelength-dependent elastic backscattering from a number of ambient background aerosol types, and compare this with that generated from representative sporulated and vegetative bacterial systems. Calculations in this report show that a 266, 355, 532 and 1064 nm elastic backscatter LIDAR experiment will allow an operator to immediately recognize when sulfate, VOC-based or road dust (silicate) aerosols are approaching, independent of humidity changes. It will be more difficult to distinguish soot aerosols from biological aerosols, or vegetative bacteria from sporulated bacteria. In these latter cases, the elastic scattering data will most likely have to be combined with UV fluorescence data to enable a more robust categorization.

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We have used experimental and computational analysis of R. sphaeroides photosynthesis and other gene expression networks (Kaplan, Gomelsky, Donohue) (3-9, 12, 13, 15-18, 20). We have identified many new candidate photosynthesis genes with expression patterns that varied as a function of light intensity. Results from these experiments suggest there are many more light-regulated aspects of the photosynthetic lifestyle of this bacterium than previously appreciated. Ongoing genetic analysis confirms that mutations in some of these newly-identified photosynthesis block the ability of cells to use solar energy in the laboratory. We also carried out transcriptome and computational analysis of individual R. sphaeroides regulons. This identified additional genes that are directly regulated by individual transcription factors and refined the consensus sequence for master regulators of photosystem development. We also showed that PpsR indirectly regulates genes that do not contain the PpsR-binding sites, e.g. puf and puhA operons. This suggests that PpsR plays a more global role as a regulator of photosystem development than what was assumed before. A similar computational and microarray analysis of PrrA target genes has identified many new candidate promoters that are controlled by this master regulator of photosynthesis. We have begun bioinformatic, genetic and biochemical experiments aimed at elucidating …

Environmental nanoparticles are often poorly-crystalline or metastable structures, whose kinetics of formation and growth are poorly understood. Further, the sorption or growth of nanoparticles on mineral surfaces may control the mineral surface's reactivity and modify its ability to influence contaminant transport. Due to the characteristic length scale, a holistic understanding of the nucleation mechanisms and kinetics of nanoparticle formation on mineral surfaces is difficult to achieve with traditional methodology. In this work, our intent is to determine the molecular nature of nucleation on surfaces, the kinetics of surface nucleation and growth, and the effect of crystal surface topology using new synchrotron-based techniques. We have approached these objectives by: (1) combining state-of-the-art crystal-truncation rod diffraction (CTR) and grazing incidence x-ray absorption fine structure spectroscopy (GIXAS) techniques to investigate the three-dimensional molecular-scale geometry of silicate monomer sorption on the r-plane of hematite; and (2) developing a new grazing-incidence small angle x-ray scattering (GISAXS) setup at SSRL (0.08 nm{sup -1} < q < 8 nm{sup -1}) to explore the initial development of environmental nanoparticles on various mineral surfaces. This study also includes complementary techniques such as atomic force microscopy (AFM), bulk SAXS, dynamic light scattering (DLS), XRD, and TEM.

We have performed experiments and modeling to evaluate a proposed merging beamlet approach for use in a compact high-brightness Heavy Ion Fusion injector. We used an RF plasma source to produce the initial beamlets. An extraction current density of 100 mA/cm{sup 2} was achieved, and the thermal temperature of the ions was below 1 eV. An array of converging beamlets was used to produce a beam with the envelope radius, convergence, and ellipticity matched to an electrostatic quadrupole channel. Experimental results were in good quantitative agreement with computer simulations and have demonstrated the feasibility of this concept. The size of a driver-scale injector system using this approach will be several times smaller than one designed using traditional single large-aperture beams. The success of this experiment has possible significant economical and technical impacts on the architecture of HIF drivers.

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New techniques for improving both the computational andimaging performance of the three dimensional (3D) electromagnetic inverseproblem are presented. A non-linear conjugate gradient algorithm is theframework of the inversion scheme. Full wave equation modelling forcontrolled sources is utilized for data simulation along with anefficient gradient computation approach for the model update. Improvingthe modelling efficiency of the 3D finite difference method involves theseparation of the potentially large modelling mesh, defining the set ofmodel parameters, from the computational finite difference meshes usedfor field simulation. Grid spacings and thus overall grid sizes can bereduced and optimized according to source frequencies and source-receiveroffsets of a given input data set. Further computational efficiency isobtained by combining different levels of parallelization. While theparallel scheme allows for an arbitrarily large number of parallel tasks,the relative amount of message passing is kept constant. Imageenhancement is achieved by model parameter transformation functions,which enforce bounded conductivity parameters and thus prevent parameterovershoots. Further, a remedy for treating distorted data within theinversion process is presented. Data distortions simulated here includepositioning errors and a highly conductive overburden, hiding the desiredtarget signal. The methods are demonstrated using both synthetic andfield data.