The authors present the design and first results of a low-temperature, ultrahigh vacuum scanning probe microscope enabling atomic resolution imaging in both scanning tunneling microscopy (STM) and noncontact atomic force microscopy (NC-AFM) modes. A tuning-fork-based sensor provides flexibility in selecting probe tip materials, which can be either metallic or nonmetallic. When choosing a conducting tip and sample, simultaneous STM/NC-AFM data acquisition is possible. Noticeable characteristics that distinguish this setup from similar systems providing simultaneous STM/NC-AFM capabilities are its combination of relative compactness (on-top bath cryostat needs no pit), in situ exchange of tip and sample at low temperatures, short turnaround times, modest helium consumption, and unrestricted access from dedicated flanges. The latter permits not only the optical surveillance of the tip during approach but also the direct deposition of molecules or atoms on either tip or sample while they remain cold. Atomic corrugations as low as 1 pm could successfully be resolved. In addition, lateral drifts rates of below 15 pm/h allow long-term data acquisition series and the recording of site-specific spectroscopy maps. Results obtained on Cu(111) and graphite illustrate the microscope's performance.

The Savannah River Site (SRS) has 49 underground storage tanks used to store High Level Waste (HLW). The tank space in these tanks must be managed to support the continued operation of key facilities. The reduction of the tank volumes in these tanks are accomplished through the use of three atmospheric pressure HLW evaporators. For a decade, evaporation of highly alkaline HLW containing aluminum and silicates has produced sodium aluminosilicate scales causing both operation and criticality hazards in the 2H Evaporator System. Segregation of aluminum-rich wastes from silicate-rich wastes minimizes the amount of scale produced and reduces cleaning expenses, but does not eliminate the scaling nor increases operation flexibility in waste process. Similar issues have affected the aluminum refining industry for many decades. Over the past several years, successful commercial products have been identified to eliminate aluminosilicate fouling in the aluminum industry, but have not been utilized in a nuclear environment. Laboratory quantities of three proprietary aluminosilicate scale inhibitors have been produced and been shown to prevent formation of scales. SRNL has been actively testing these potential inhibitors to examine their radiation stability, radiolytic degradation behaviors, and downstream impacts to determine their viability within the HLW system. One of the …

It is shown that the transient expansion of plutonium-gallium alloys observed both in the lattice parameter as well as in the dimension of a sample held at ambient temperature can be explained by assuming incipient precipitation of Pu{sub 3}Ga. However, this ordered {zeta}-phase is also subject to radiation-induced disordering. As a result, the gallium-stabilized {delta}-phase, being metastable at ambient temperature, is driven towards thermodynamic equilibrium by radiation-enhanced diffusion of gallium and at the same time reverted back to its metastable state by radiation-induced disordering. A steady state is reached in which only a modest fraction of the gallium present is arranged in ordered {zeta}-phase regions.

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We found monochromatic electron photoemission from large-area self-assembled monolayers of a functionalized diamondoid, [121]tetramantane-6-thiol. Photoelectron spectra of the diamondoid monolayers exhibited a peak at the low-kinetic energy threshold; up to 68percent of all emitted electrons were emitted within this single energy peak. The intensity of the emission peak is indicative of diamondoids being negative electron affinity materials. With an energy distribution width of less than 0.5 electron volts, this source of monochromatic electrons may find application in technologies such as electron microscopy, electron beam lithography, and field-emission flatpanel displays.

An over-dense microwave driven ion source capable of producing deuterium (or hydrogen) beams at 100-200 mA/cm{sup 2} and with atomic fraction > 90% was designed and tested with an electrostatic low energy beam transport section (LEBT). This ion source was incorporated into the design of an Accelerator Driven Neutron Source (ADNS). The other key components in the ADNS include a 6 MeV RFQ accelerator, a beam bending and scanning system, and a deuterium gas target. In this design a 40 mA D{sup +} beam is produced from a 6 mm diameter aperture using a 60 kV extraction voltage. The LEBT section consists of 5 electrodes arranged to form 2 Einzel lenses that focus the beam into the RFQ entrance. To create the ECR condition, 2 induction coils are used to create {approx} 875 Gauss on axis inside the source chamber. To prevent HV breakdown in the LEBT a magnetic field clamp is necessary to minimize the field in this region. Matching of the microwave power from the waveguide to the plasma is done by an autotuner. They observed significant improvement of the beam quality after installing a boron nitride liner inside the ion source. The measured emittance data are compared …

Down the drain: Cryptophane cages in combination with selective radiofrequency spin labeling can be used as molecular 'transpletor' units for transferring depletion of spin polarization from a hyperpolarized 'source' spin ensemble to a 'drain' ensemble. The flow of nuclei through the gate is adjustable by the ambient temperature, thereby enabling controlled consumption of hyperpolarization.

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We consider a charged porous material that is saturated bytwo fluid phases that are immiscible and continuous on the scale of arepresentative elementary volume. The wetting phase for the grains iswater and the nonwetting phase is assumed to be an electricallyinsulating viscous fluid. We use a volume-averaging approach to derivethe linear constitutive equations for the electrical current density aswell as the seepage velocities of the wetting and nonwetting phases onthe scale of a representative elementary volume. These macroscopicconstitutive equations are obtained by volume-averaging Ampere's lawtogether with the Nernst Planck equation and the Stokes equations. Thematerial properties entering the macroscopic constitutive equations areexplicitly described as functions of the saturation of the water phase,the electrical formation factor, and parameters that describe thecapillary pressure function, the relative permeability function, and thevariation of electrical conductivity with saturation. New equations arederived for the streaming potential and electro-osmosis couplingcoefficients. A primary drainage and imbibition experiment is simulatednumerically to demonstrate that the relative streaming potential couplingcoefficient depends not only on the water saturation, but also on thematerial properties of the sample, as well as the saturation history. Wealso compare the predicted streaming potential coupling coefficients withexperimental data from four dolomite core samples. Measurements on thesesamples include electrical …

We report on spectroscopic investigations of Nd{sup 3+}- and Tb{sup 3+}- doped low phonon energy, moisture-resistant host crystals, KPb{sub 2}Br{sub 5} and RbPb{sub 2}Br{sub 5}, and their potential to serve as new solid state laser materials at new wavelengths, especially in the long wavelength infrared region. This includes emission spectra, emission lifetime measurements, Raman scattering spectra as well as calculations of the multiphonon decay rate, radiative lifetimes and quantum efficiencies for relevant (laser) transitions in these crystals.

The tetrahedral [Ga{sub 4}L{sub 6}]{sup 12-} assembly (L = N,N-bis(2,3-dihydroxybenzoyl)-1,5-diaminonaphthalene) encapsulates a variety of cations, including propargyl enammonium cations capable of undergoing the aza Cope rearrangement. For propargyl enammonium substrates that are encapsulated in the [Ga{sub 4}L{sub 6}]{sup 12-} assembly, rate accelerations of up to 184 are observed when compared to the background reaction. After rearrangement, the product iminium ion is released into solution and hydrolyzed allowing for catalytic turnover. The activation parameters for the catalyzed and uncatalyzed reaction were determined, revealing that a lowered entropy of activation is responsible for the observed rate enhancements. The catalyzed reaction exhibits saturation kinetics; the rate data obey the Michaelis-Menten model of enzyme kinetics, and competitive inhibition using a non-reactive guest has been demonstrated.

We describe the development and applications of novel instrumentation for photoemission spectroscopy of solid or liquid surfaces in the presence of gases under ambient conditions or pressure and temperature. The new instrument overcomes the strong scattering of electrons in gases by the use of an aperture close to the surface followed by a differentially-pumped electrostatic lens system. In addition to the scattering problem, experiments in the presence of condensed water or other liquids require the development of special sample holders to provide localized cooling. We discuss the first two generations of Ambient Pressure PhotoEmission Spectroscopy (APPES) instruments developed at synchrotron light sources (ALS in Berkeley and BESSY in Berlin), with special focus on the Berkeley instruments. Applications to environmental science and catalytic chemical research are illustrated in two examples.

Historical seismic hazard characterizations did not include earthquake ground motion waveforms at frequencies below approximately 0.2 Hz (5 seconds period). This resulted from limitations in early strong motion instrumentation and signal processing techniques, a lack of measurements in the near-field of major earthquakes and therefore no observational awareness, and a delayed understanding in the engineering community of the potential significance of these types of motions. In recent years, there is a growing recognition of the relevance of near-fault, low frequency motions, particularly for long-period structures such as large bridges. This paper describes a computationally based study of the effects of low frequency (long-period) near-fault motions on long-span bridge response. The importance of inclusion of these types of motions for long span cable supported bridges is demonstrated using actual measured broad-band, near-fault motions from large earthquakes.

The urgent quest for new energy sources has led developed countries, representing over half of the world population, to collaborate on demonstrating the scientific and technological feasibility of magnetic fusion through the construction and operation of ITER. Data on high-Z ions will be important in this quest. Tungsten plasma facing components have the necessary low erosion rates and low tritium retention but the high radiative efficiency of tungsten ions leads to stringent restrictions on the concentration of tungsten ions in the burning plasma. The influx of tungsten to the burning plasma will need to be diagnosed, understood and stringently controlled. Expanded knowledge of the atomic physics of neutral and ionized tungsten will be important to monitor impurity influxes and derive tungsten concentrations. Also, inert gases such as argon and xenon will be used to dissipate the heat flux flowing to the divertor. This article will summarize the spectroscopic diagnostics planned for ITER and outline areas where additional data is needed.

Using Chandra HETG data we present light curves for individual spectral lines of Mg XI and Mg XII for EX Hydrae, an intermediate-polar type cataclysmic variable. The Mg XI light curve, folded on the white dwarf spin period, shows two spikes that are not seen in the Mg XII or broad-band light curves. Occultation of the accretion column by the body of the white dwarf would produce such spikes for an angle between the rotation axis and the accretion columns of {alpha} = 18{sup o} and a height of the Mg XI emission above the white dwarf surface of {approx}< 0.0004 white dwarf radii or {approx}< 4 km. The absence of spikes in the Mg XII and broad-band light curves could then be explained if the bulk of its emission forms at much larger height, > 0.004 white dwarf radii or > 40 km, above the white dwarf surface. The technique described in this letter demonstrates that high signal-to-noise ratio and high spectral resolution X-ray spectra can be used to map the temperature and density structure of accretion flows in magnetic cataclysmic variables. The Mg XI and Mg XII light curves are not consistent with the temperature and density structure …

Two processes were chosen in the 1980's at the Savannah River Site (SRS) to decontaminate the soluble High Level Waste (HLW). The In Tank Precipitation (ITP) process (1,2) was developed at SRS for the removal of radioactive cesium and actinides from the soluble HLW. Sodium tetraphenylborate was added to the waste to precipitate cesium and monosodium titanate (MST) was added to adsorb actinides, primarily uranium and plutonium. Two products of this process were a low activity waste stream and a concentrated organic stream containing cesium tetraphenylborate and actinides adsorbed on monosodium titanate (MST). A copper catalyzed acid hydrolysis process was built to process (3, 4) the Tank 48H cesium tetraphenylborate waste in the SRS's Defense Waste Processing Facility (DWPF). Operation of the DWPF would have resulted in the production of benzene for incineration in SRS's Consolidated Incineration Facility. This process was abandoned together with the ITP process in 1998 due to high benzene in ITP caused by decomposition of excess sodium tetraphenylborate. Processing in ITP resulted in the production of approximately 1.0 million liters of HLW. SRS has chosen a solvent extraction process combined with adsorption of the actinides to decontaminate the soluble HLW stream (5). However, the waste in …

We have studied the spin relaxation in diluted spin ice Ho{sub 2-x} Y{sub x} Ti{sub 2}O{sub 7} by means of neutron spin echo spectroscopy. Remarkably, the geometrical frustration is not relieved by doping with non-magnetic Y, and the dynamics of the freezing is unaltered in the spin echo time window up to x {approx_equal} 1.6. At higher doping with non-magnetic Y (x {ge} 1.6) a new relaxation process at relatively high temperature (up to at least T {approx_equal} 55 K) appears which is more than 10 times faster than the thermally activated main relaxation process. We find evidence that over the whole range of composition all Ho spins participate in the dynamics. These results are compared to a.c. susceptibility measurements of the diluted Ho and Dy spin ice systems. X-ray absorption fine structure (EXAFS) spectra and x-ray diffraction show that the samples are structurally well ordered.

This paper outlines rock mechanics investigations associated with mechanical degradation of planned emplacement drifts at Yucca Mountain, which is the designated site for a US high-level nuclear waste repository. The factors leading to drift degradation include stresses from the overburden, stresses induced by the heat released from the emplaced waste, stresses due to seismically related ground motions, and time-dependent strength degradation. The welded tuff emplacement horizon consists of two groups of rock with distinct engineering properties: nonlithophysal units and lithophysal units, based on the relative proportion of lithophysal cavities. Part I of the paper concentrates on the generally hard, strong, and fractured nonlithophysal rock. The degradation behavior of the tunnels in the nonlithophysal rock is controlled by the occurrence of keyblocks. A statistically equivalent fracture model was generated based on extensive underground fracture mapping data from the Exploratory Studies Facility at Yucca Mountain. Three-dimensional distinct block analyses, generated with the fracture patterns randomly selected from the fracture model, were developed with the consideration of in situ, thermal, seismic loads. In this study, field data, laboratory data, and numerical analyses are well integrated to provide a solution for the unique problem of modeling drift degradation throughout the regulatory period for repository …

Denitrification can effectively mitigate the problem of high nitrate concentrations in groundwater under dairy operations by reducing nitrate to N{sub 2} gas, at sites where biogeochemical conditions are favorable. We present results from field studies at central California dairies that document the occurrence of saturated-zone denitrification in shallow groundwater using biomolecular indicators, stable isotope compositions of nitrate, and measurements of dissolved excess N{sub 2} gas. Excess N{sub 2} concentrations provide a measure of the extent to which nitrate in groundwater has been partially or completely denitrified. Abundant excess N{sub 2} and young {sup 3}H/{sup 3}He apparent groundwater ages indicate high denitrification rates near manure lagoons where multiple lines of evidence indicate seepage of lagoon water into the groundwater system. Natural tracers of lagoon water include high chloride and dissolved organic carbon concentrations, distinctive trace organic compounds, and high groundwater {delta}{sup 18}O values (relative to other recharge sources). Proximal to the lagoons, NH{sub 4}{sup +} may be present in groundwater, but is strongly adsorbed on to sediment particles. Bubble formation in the lagoons causes the exsolution of other gases (N{sub 2}, Ar, Ne, He, etc.), which partition into the gas phase and strip the lagoon water of its dissolved gas load, …

The development of a high-energy (10Mev) neutron imaging system at Lawrence Livermore National Laboratory (LLNL) depends on a precision engineered rotating aperture and vacuum system for generating neutrons that are used for imaging dense objects. This subsystem is part of a larger system which includes a linear accelerator that creates a deuteron beam, a scintillator detector, imaging optics and a high resolution CCD camera. The rotating aperture vacuum system has been successfully simulated and tested. Results show the feasibility of the design and point toward ways to improve the design by minimizing the rotating aperture gap.

The long-term program aimed at selection of a site for a deep repository was initiated in Finland in 1983. This program has come to end in 2001 and a new phase aimed at implementation of the geological disposal of spent fuel has been started. In this new phase the first milestone is the application for a construction license for the disposal facility around 2010. To fulfill the needs for detailed design of the disposal system, an underground rock characterization facility (URCF) will be constructed at the representative depth at Olkiluoto. The excavation of this facility will start the work for underground characterization, testing and demonstration, which is planned to be a continuous activity throughout the whole life cycle of the deep repository. The overall objectives for the underground site characterization are (1) verification of the present conclusions on site suitability, (2) definition and identification of suitable rock volumes for repository space and (3) characterization of planned host rock for detailed design, safety assessment and construction planning. The objective for verification aims at assessing that the Olkiluoto site meets the basic criteria for long-term safety and as well the basic requirements for construction and thus justifies the site selection. The two …

This paper describes the approaches used in the clearing, cleaning, decontamination and decommissioning of a very large suite of seven concrete shielded caves and other facilities used by UKAEA at Winfrith Technology Centre, England over a period of about 30 years for the postirradiation examination (PIE) of a wide range of nuclear fuels and other very active components. The basic construction of the facilities will first be described, setting the scene for the major challenges that 1970s' thinking posed for decommissioning engineers. The tendency then to use large and heavy items of equipment supported upon massive steel bench structures produced a series of major problems that had to be overcome. The means of solving these problems by utilization of relatively simple and inexpensive equipment will be described. Later, a further set of challenges was experienced to decontaminate the interior surfaces to allow man entries to be undertaken at acceptable dose rates. The paper will describe the types of tooling used and the range of complementary techniques that were employed to steadily reduce the dose rates down to acceptable levels. Some explanations will also be given for the creation of realistic dose budgets and the methods of recording and continuously assessing …

Four hand-held tools were tested for failed high-level waste melter decontamination and decommissioning (D&D). The forces felt by the tools during operation were measured using a tri-axial accelerometer since they will be operated by a remote manipulator. The efficiency of the tools was also recorded. Melter D&D consists of three parts: (1) glass fracturing: removing from the furnace the melted glass that can not be poured out through normal means, (2) glass cleaning: removing the thin layer of glass that has formed over the surface of the refractory material, and (3) K-3 refractory breakup: removing the K-3 refractory material. Surrogate glass, from a formula provided by the Savannah River Site, was melted in a furnace and poured into steel containers. K-3 refractory material, the same material used in the Defense Waste Processing Facility, was utilized for the demonstrations. Four K-3 blocks were heated at 1150 C for two weeks with a glass layer on top to simulate the hardened glass layer on the refractory surface in the melter. Tools chosen for the demonstrations were commonly used D&D tools, which have not been tested specifically for the different aspects of melter D&D. A jackhammer and a needle gun were tested for …

On February 22, 1999, the U.S. Nuclear Regulatory Commission (NRC) proposed licensing criteria in a new, separate part of its regulations, at 10 CFR Part 63 (hereafter referred to as Part 63), for disposal of high-level radioactive waste (HLW) in a potential geologic repository at Yucca Mountain, Nevada (1). After publication of the proposed Part 63, the staff provided members of the public and other stakeholders multiple opportunities to discuss the proposed requirements. On June 13, 2001, the U.S. Environmental Protection Agency (EPA) issued final environmental standards for a potential geologic repository at Yucca Mountain, Nevada at 40 CFR Part 197 (2), as mandated by the Energy Policy Act of 1992 (EnPA)(3). The NRC has prepared its final regulations based on careful review and consideration of the public comments received on its proposed rule and the statutory direction for NRC to adopt technical criteria consistent with final EPA standards.