Reduction of the uranium metallocene,[eta5-1,2,4-(Me3C)3C5H2]2UCl2 (1), Cp'2UCl2, in the presence of2,2'-bipyridyl and sodium naphthalene gives the dark green metallocenecomplex, Cp'2U(bipy) (6), which reacts with p-tolylazide orpyridine-N-oxide to give Cp'2U=N(p-tolyl) (7) or Cp'2U(O)(py) (8),respectively. The Lewis acid, BPh3, precipitates Ph3B(py) and gives thebase-free oxo, Cp'2UO (10), which crystallizes from pentane. Theoxometallocene 10 behaves as a nucleophile with Me3SiX reagents but itdoes not exhibit cycloaddition behavior with acetylenes, suggesting thatthe polar resonance structure, Cp'2U+-O- dominates the double bondresonance structure Cp'2U=O.

We report the first detection of radio emission from any anomalous X-ray pulsar (AXP). Data from the Very Large Array (VLA) MAGPIS survey with angular resolution 6'' reveals a point-source of flux density 4.5 {+-} 0.5 mJy at 1.4 GHz at the precise location of the 5.54 s pulsar XTE J1810-197. This is greater than upper limits from all other AXPs and from quiescent states of soft gamma-ray repeaters (SGRs). The detection was made in 2004 January, 1 year after the discovery of XTE J1810-197 during its only known outburst. Additional VLA observations both before and after the outburst yield only upper limits that are comparable to or larger than the single detection, neither supporting nor ruling out a decaying radio afterglow related to the X-ray turn-on. Another hypothesis is that, unlike the other AXPs and SGRs, XTE J1810-197 may power a radio synchrotron nebula by the interaction of its particle wind with a moderately dense environment that was not evacuated by previous activity from this least luminous, in X-rays, of the known magnetars.

The Hanford External Dosimetry Technical Basis Manual PNL-MA-842 documents the design and implementation of the external dosimetry system used at Hanford. The manual describes the dosimeter design, processing protocols, dose calculation methodology, radiation fields encountered, dosimeter response characteristics, limitations of dosimeter design under field conditions, and makes recommendations for effective use of the dosimeters in the field. The manual describes the technical basis for the dosimetry system in a manner intended to help ensure defensibility of the dose of record at Hanford and to demonstrate compliance with 10 CFR 835, DOELAP, DOE-RL, ORP, PNSO, and Hanford contractor requirements. The dosimetry system is operated by PNNL’s Hanford External Dosimetry Program which provides dosimetry services to all Hanford contractors. The primary users of this manual are DOE and DOE contractors at Hanford using the dosimetry services of PNNL. Development and maintenance of this manual is funded directly by DOE and DOE contractors. Its contents have been reviewed and approved by DOE and DOE contractors at Hanford through the Hanford Personnel Dosimetry Advisory Committee which is chartered and chaired by DOE-RL and serves as means of coordinating dosimetry practices across contractors at Hanford. This manual was established in 1996. Since inception, it has …

We present here the PhIGs database, a phylogenomic resource for sequenced genomes. Although many methods exist for clustering gene families, very few attempt to create truly orthologous clusters sharing descent from a single ancestral gene across a range of evolutionary depths. Although these non-phylogenetic gene family clusters have been used broadly for gene annotation, errors are known to be introduced by the artifactual association of slowly evolving paralogs and lack of annotation for those more rapidly evolving. A full phylogenetic framework is necessary for accurate inference of function and for many studies that address pattern and mechanism of the evolution of the genome. The automated generation of evolutionary gene clusters, creation of gene trees, determination of orthology and paralogy relationships, and the correlation of this information with gene annotations, expression information, and genomic context is an important resource to the scientific community.

The signal in an NMR experiment is highly sensitive to fluctuations of the environment of the sample. If, for example, the static magnetic field B{sub 0}, the amplitude and phase of radio frequency (rf) pulses, or the resonant frequency of the detection circuit are not perfectly stable and reproducible, the magnetic moment of the spins is altered and becomes a noisy quantity itself. This kind of noise not only depends on the presence of a signal, it is in fact proportional to it. Since all the spins at a particular location in a sample experience the same environment at any given time, this noise primarily affects the reproducibility of an experiment, which is mainly of importance in the indirect dimensions of a multidimensional experiment, when intense lines are suppressed with a phase cycle, or for difference spectroscopy techniques. Equivalently, experiments which are known to be problematic with regard to their reproducibility, like flow experiments or experiments with a mobile target, tend to be affected stronger by multiplicative noise. In this article it is demonstrated how multiplicative noise can be identified and characterized using very simple, repetitive experiments. An error estimation approach is developed to give an intuitive, yet quantitative understanding …

Gravity waves arise in gravitationally stratified compressible flows at low Mach and Froude numbers. These waves can have a negligible influence on the overall dynamics of the fluid but, for numerical methods where the acoustic waves are treated implicitly, they impose a significant restriction on the time step. A way to alleviate this restriction is to filter out the modes corresponding to the fastest gravity waves so that a larger time step can be used. This paper presents a filtering strategy of the fully compressible equations based on normal mode analysis that is used throughout the simulation to compute the fast dynamics and that is able to damp only fast gravity modes.

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We report the density-dependent crossover of a resonantly photoexcited exciton gas from insulating to conducting phases. Broadband terahertz spectroscopy gives direct access to the exciton binding energy via intra-excitonic 1s-2p transitions. A strong shift, broadening, and ultimately the disappearance of this resonance occurs with decreasing inter-particle distance. Densities of excitons and unbound electron-hole pairs are followed quantitatively using a model of the composite free-carrier and exciton terahertz conductivity. Comparison with near-infrared absorption changes illustrates a significantly enhanced energy shift and broadening of the intra-excitonic resonance.

First-principles generalized pseudopotential theory (GPT) provides a fundamental basis for transferable multi-ion interatomic potentials in transition metals and alloys within density-functional quantum mechanics. In central bcc transition metals, where multi-ion angular forces are important to structural properties, simplified model GPT or MGPT potentials have been developed based on canonical d bands to allow analytic forms and large-scale atomistic simulations. Robust, advanced-generation MGPT potentials have now been obtained for Ta and Mo and successfully applied to a wide range of structural, thermodynamic, defect and mechanical properties at both ambient and extreme conditions. Selected applications to multiscale modeling discussed here include dislocation core structure and mobility, atomistically informed dislocation dynamics simulations of plasticity, and thermoelasticity and high-pressure strength modeling. Recent algorithm improvements have provided a more general matrix representation of MGPT beyond canonical bands, allowing improved accuracy and extension to f-electron actinide metals, an order of magnitude increase in computational speed for dynamic simulations, and the still-in-progress development of temperature-dependent potentials.

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The accuracy of a numerical method for solving the neutron transport equation is limited by the smallest mean free path in the problem. Since problems in the asymptotic diffusive regimes have vanishingly small mean free paths, it seems hopeless, given a limited amount of computer memory, that an accurate solution can be obtained for these problems. However we found that the accuracy of a numerical method improves as the scattering ratio increases with the total cross section and the grid spacing held fixed for problems that are in the asymptotic diffusive regime. This phenomenon is independent of the numerical method and can be explained on physical grounds. The numerical results by the Diamond Difference Method are given to show this phenomenon.

This issue of Science and Technology Review has the following articles: (1) Enhanced National Security through International Research Collaborations--Commentary by Stephen G. Cochran; (2) Building Networks of Trust through Collaborative Science--Livermore scientists are leading collaborative science and technology projects with colleagues from Central and South Asia and the Middle East; (3) Tracing the Steps in Nuclear Material Trafficking--The Laboratory.s nuclear science expertise is helping to thwart the illicit trafficking of nuclear material; (4) Looking at Earth in Action--Geophysicists at Livermore are using laboratory experiments to examine such issues as how best to store nuclear wastes and how to mitigate the effects of greenhouse gases; and (5) Gamma-Ray Bursts Shower the Universe with Metals--Computer models indicate that gamma-ray bursts from dying stars may be important sources of elements such as iron, zinc, titanium, and copper.

The objective of this spent fuel burnup credit work was to study and describe a VVER-440 reactor spent fuel assembly (FA) initial state before irradiation, its operational irradiation history and the resulting radionuclide distribution in the fuel assembly after irradiation. This work includes the following stages: (1) to pick out and select a specific spent (irradiated) FA for examination; (2) to describe the FA initial state before irradiation; (3) to describe the irradiation history, including thermal calculations; (4) to examine the burnup distribution of select radionuclides along the FA height and cross-section; (5) to examine the radionuclide distributions; (6) to determine the Kr-85 release into the plenum; (7) to select and prepare FA rod specimens for destructive examinations; (8) to determine the radionuclide compositions, isotope masses and burnup in the rod specimens; and (9) to analyze, document and process the results. The specific workscope included the destructive assay (DA) of spent fuel assembly rod segments with an {approx}38.5 MWd/KgU burnup from a single VVER-440 fuel assembly from the Novovorenezh reactor in Russia. Based on irradiation history criteria, four rods from the fuel assembly were selected and removed from the assembly for examination. Next, 8 sections were cut from the four …

We study conditions for the existence of asymptotic observables in cosmology. With the exception of de Sitter space, the thermal properties of accelerating universes permit arbitrarily long observations, and guarantee the production of accessible states of arbitrarily large entropy. This suggests that some asymptotic observables may exist, despite the presence of an event horizon. Comparison with decelerating universes shows surprising similarities: Neither type suffers from the limitations encountered in de Sitter space, such as thermalization and boundedness of entropy. However, we argue that no realistic cosmology permits the global observations associated with an S-matrix.

Solid-state infrared spectroscopy, differential scanning calorimetry, and elemental analysis have been used to evaluate the reactivity of resorcinol formaldehyde resin with nitric acid and characterize the solid product. Two distinct reactions were identified within the temperature range 25-55 C. The first reaction is primarily associated with resin nitration, while the second involves bulk oxidation and degradation of the polymer network leading to dissolution and off-gassing. The threshold conditions promoting reaction have been identified. Reaction was confirmed with nitric acid concentrations as low as 3 M at 25 C applied temperature and 0.625 M at 66 C. Although a nitrated resin product can be isolated under appropriate experimental conditions, calorimetry testing indicates no significant hazard associated with handling the dry material.

We review the technical challenges associated with the production and use of various coal chars in a direct carbon conversion fuel cell. Existing chemical and physical deashing processes remove material below levels impacting performance at minimal cost. At equilibrium, sulfur entrained is rejected from the melt as COS in the offgas.

Thermal cook-off experiments were carried out using LX-04 explosive (85% HMX and 15% Viton by weight) with different levels of confinement to characterize the effect of confinement on the reaction violence. These experiments involved heating a porous LX-04 sample in a stainless steel container with varying container end plate thickness and assembly bolt diameter to control overall confinement. As expected, detonation did not occur and reducing the overall confinement lowered the reaction violence. This is consistent with modeling results that predict that a lower confinement will act to lower the cook-off pressure and thus the overall burn rate which lowers the overall violence. These results suggest that controlling the overall system confinement can modify the relative safety in a given scenario.

BAASS (Bayesian Approaches for Adaptive Spatial Sampling) is a set of computational routines developed to support the design and deployment of spatial sampling programs for delineating contamination footprints, such as those that might result from the accidental or intentional environmental release of radionuclides. BAASS presumes the existence of real-time measurement technologies that provide information quickly enough to affect the progress of data collection. This technical memorandum describes the application of BAASS to a simple example, compares the performance of a BAASS-based program with that of a traditional gridded program, and explores the significance of several of the underlying assumptions required by BAASS. These assumptions include the range of spatial autocorrelation present, the value of prior information, the confidence level required for decision making, and ''inside-out'' versus ''outside-in'' sampling strategies. In the context of the example, adaptive sampling combined with prior information significantly reduced the number of samples required to delineate the contamination footprint.

A stabilized, nodally integrated linear tetrahedral is formulated and analyzed. It is well known that linear tetrahedral elements perform poorly in problems with plasticity, nearly incompressible materials, and acute bending. For a variety of reasons, linear tetrahedral elements are preferable to quadratic tetrahedral elements in most nonlinear problems. Whereas, mixed methods work well for linear hexahedral elements, they don't for linear tetrahedrals. On the other hand, automatic mesh generation is typically not feasible for building many 3D hexahedral meshes. A stabilized, nodally integrated linear tetrahedral is developed and shown to perform very well in problems with plasticity, nearly incompressible materials and acute bending. Furthermore, the formulation is analytically and numerically shown to be stable and optimally convergent. The element is demonstrated to perform well in several standard linear and nonlinear benchmarks.

Using first-order perturbation theory for maps, we extend the familiar formulae for space-charge tuneshift to encompass the case of a fully coupled lattice.

A multidimensional, mountain-scale, thermal-hydrologic (TH) numerical model is presented for investigating unsaturated flow behavior in response to decay heat from the radioactive waste repository in the Yucca Mountain unsaturated zone (UZ), Nevada. The model, consisting of both two-dimensional (2-D) and three-dimensional (3-D) representations of the UZ repository system, is based on the current repository design, drift layout, thermal loading scenario, and estimated current and future climate conditions. This mountain-scale TH model evaluates the coupled TH processes related to mountain-scale UZ flow. It also simulates the impact of radioactive waste heat release on the natural hydrogeological system, including heat-driven processes occurring near and far away from the emplacement tunnels or drifts. The model simulations predict thermally perturbed liquid saturation, gas- and liquid-phase fluxes, and water and rock temperature elevations, as well as the changes in water flux driven by evaporation/condensation processes and drainage between drifts. These simulations provide mountain-scale thermally perturbed flow fields for assessing the repository performance under thermal loading conditions.

The High Average Power Laser Program (HAPL) is a multi-institutional, synergistic effort to develop inertial fusion energy (IFE). This program is building a physics and technology base to complement the laser-fusion science being pursued by DOE Defense programs in support of Stockpile Stewardship. The primary institutions responsible for overseeing and coordinating the research activities are the Naval Research Laboratory (NRL) and Lawrence Livermore National Laboratory (LLNL). The current LLNL proposal is a companion document to the one submitted by NRL, for which the driver development element is focused on the krypton fluoride excimer laser option. The NRL and LLNL proposals also jointly pursue complementary activities with the associated rep-rated laser technologies relating to target fabrication, target injection, final optics, fusion chamber, target physics, materials and power plant economics. This proposal requests continued funding in FY03 to support LLNL in its program to build a 1 kW, 100 J, diode-pumped, crystalline laser, as well as research into high gain fusion target design, fusion chamber issues, and survivability of the final optic element. These technologies are crucial to the feasibility of inertial fusion energy power plants and also have relevance in rep-rated stewardship experiments. The HAPL Program pursues technologies needed for laser-driven …

Biological Aerosol Mass Spectrometry (BAMS) is an emerging technique for the detection of biological aerosols, which is being developed at Lawrence Livermore National Laboratory. The current system uses several orthogonal analytical methods to improve system selectivity, sensitivity and speed in order to maximize its utility as a biological aerosol detection system with extremely low probability of false alarm and high probability of detection. Our approach is to pre-select particles of interest by size and fluorescence prior to mass spectral analysis. The ability to distinguish biological aerosols from background and to discriminate bacterial spores, vegetative cells, viruses and toxins from one another will be shown. Data from particle standards of known chemical composition will be discussed. Analysis of ambient particles will also be presented.