The objectives of this report are: (1) Investigate the catalysis of water oxidation by cobalt and manganese hydrous oxides immobilized on titania or silica nanoparticles, and dinuclear metal complexes with quinonoid ligands in order to develop a better understanding of the critical water oxidation chemistry, and rationally search for improved catalysts. (2) Optimize the light-harvesting and charge-separation abilities of stable semiconductors including both a focused effort to improve the best existing materials by investigating their structural and electronic properties using a full suite of characterization tools, and a parallel effort to discover and characterize new materials. (3) Combine these elements to examine the function of oxidation catalysts on Band-Gap-Narrowed Semiconductor (BGNSC) surfaces and elucidate the core scientific challenges to the efficient coupling of the materials functions.

Density Functional Theory and small-core, relativistic pseudopotentials were used to look for symmetric and asymmetric transitions states of the gas-phase hydrolysis reaction of uranium hexafluoride, UF{sub 6}, with water. At the B3LYP/6-31G(d,p)/SDD level, an asymmetric transition state leading to the formation of a uranium hydroxyl fluoride, U(OH)F{sub 5}, and hydrogen fluoride was found with an energy barrier of +77.3 kJ/mol and an enthalpy of reaction of +63.0 kJ/mol (both including zero-point energy corrections). Addition of diffuse functions to all atoms except uranium led to only minor changes in the structure and relative energies of the reacting complex and transition state. However, a significant change in the product complex structure was found, significantly reducing the enthalpy of reaction to +31.9 kJ/mol. Similar structures and values were found for PBE0 and MP2 calculations with this larger basis set, supporting the B3LYP results. No symmetric transition state leading to the direct formation of uranium oxide tetrafluoride, UOF{sub 4}, was found, indicating that the reaction under ambient conditions likely includes several more steps than the mechanisms commonly mentioned. The transition state presented here appears to be the first published transition state for the important gas-phase reaction of UF{sub 6} with water.

The Hanford Site is a decommissioned nuclear productions complex located in south eastern Washington and is operated by the Department of Energy (DOE). From 1955 to 1973, carbon tetrachloride (CCl{sub 4}), used in mixtures with other organic compounds, was used to recover plutonium from aqueous streams at Z Plant located on the Hanford Site. The aqueous and organic liquid waste that remained at the end of this process was discharged to soil columns in waste cribs located near Z Plant. Included in this waste slurry along with CCl{sub 4} were tributyl phosphate, dibutyl butyl phosphate, and lard oil. (Truex et al., 2001). In the mid 1980's, CCl{sub 4} was found in the unconfined aquifer below the 200 West Area and subsequent ground water monitoring indicated that the plume was widespread and that the concentrations were increasing. It has been estimated that approximately 750,000 kg (826.7 tons) of CCl{sub 4} was discharged to the soil from 1955 to 1973. (Truex et al., 2001). With initial concentration readings of approximately 30,000 parts per million by volume (ppmv) in one well field alone, soil vapor extraction began in 1992 in an effort to remove the CCl{sub 4} from the soil. (Rohay, 1999). Since …

The objectives of this report are: (1) Investigate the catalysis of water oxidation by cobalt and manganese hydrous oxides immobilized on titania or silica nanoparticles, and dinuclear metal complexes with quinonoid ligands in order to develop a better understanding of the critical water oxidation chemistry, and rationally search for improved catalysts. (2) Optimize the light-harvesting and charge-separation abilities of stable semiconductors including both a focused effort to improve the best existing materials by investigating their structural and electronic properties using a full suite of characterization tools, and a parallel effort to discover and characterize new materials. (3) Combine these elements to examine the function of oxidation catalysts on Band-Gap-Narrowed Semiconductor (BGNSC) surfaces and elucidate the core scientific challenges to the efficient coupling of the materials functions.

For the users of the high-brightness radiation sources of free-electron lasers it is desirable to reduce the FEL pulse length to 10 fs and below for time-resolved pump and probe experiments. Although it can be achieved by conventional compression methods for the electron beam or the chirped FEL pulse, the technical realization is demanding. In this presentation we study the impact of longitudinal wakefields in the undulator and how their properties can be used to reduced the amplifying part of the bunch to the desired length. Methods of actively controlling the wakefields are presented.

The background in the BaBar detector is especially high during injection, when most components are actually having reduced voltages. The situation is worse for the beam in High Energy Ring (HER) when the LER beam is present. It was found that the transverse feedback system plays an important role when stacking more charge on top of existing bunches. Lowering the feedback gain helped and it was realized later that the best scenario would be to gate off the feedback for only the one bunch, which got additional charge injected into it. The explanation is that the blown-up, but centered, original HER bunch plus the small injected off-axis bunch (each with half the charge) would stay in the ring if not touched, but the feedback system sees half the offset and wants to correct it, therefore disturbing and scraping the blown-up part.

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Experimental data that exhibits a continuous-wave, second-harmonic intensity threshold (15 kW/cm{sup 2}) that causes two-photon nonlinear absorption which leads to time-dependent photochromic damage in periodically poled KTiOPO{sub 4} is presented and verified through a thermal dephasing model.

Katzenstein and Apt investigate the important question of pollution emission reduction benefits from variable generation resources such as wind and solar. Their methodology, which couples an individual variable generator to a dedicated gas plant to produce a flat block of power is, however, inappropriate. For CO{sub 2}, the authors conclude that variable generators 'achieve {approx} 80% of the emission reductions expected if the power fluctuations caused no additional emissions.' They find even lower NO{sub x} emission reduction benefits with steam-injected gas turbines and a 2-4 times net increase in NO{sub x} emissions for systems with dry NO{sub x} control unless the ratio of energy from natural gas to variable plants is greater than 2:1. A more appropriate methodology, however, would find a significantly lower degradation of the emissions benefit than suggested by Katzenstein and Apt. As has been known for many years, models of large power system operations must take into account variable demand and the unit commitment and economic dispatch functions that are practiced every day by system operators. It is also well-known that every change in wind or solar power output does not need to be countered by an equal and opposite change in a dispatchable resource. The …

We give an effective field theory derivation, based on the running of Planck brane gauge correlators, of the large logarithms that arise in the predictions for low energy gauge couplings in compactified AdS}_5 backgrounds, including the one-loop effects of bulk scalars, fermions, and gauge bosons. In contrast to the case of charged scalars coupled to Abelian gauge fields that has been considered previously in the literature, the one-loop corrections are not dominated by a single 4D Kaluza-Klein mode. Nevertheless, in the case of gauge field loops, the amplitudes can be reorganized into a leading logarithmic contribution that is identical to the running in 4D non-Abelian gauge theory, and a term which is not logarithmically enhanced and is analogous to a two-loop effect in 4D. In a warped GUT model broken by the Higgs mechanism in the bulk,we show that the matching scale that appears in the large logarithms induced by the non-Abelian gauge fields is m_{XY}^2/k where m_{XY} is the bulk mass of the XY bosons and k is the AdS curvature. This is in contrast to the UV scale in the logarithmic contributions of scalars, which is simply the bulk mass m. Our results are summarized in a set …

Minimizing plutonium measurement uncertainty is essential to nuclear material control and international safeguards. In 2005, the International Organization for Standardization (ISO) published ISO 12183 'Controlled-potential coulometric assay of plutonium', 2nd edition. ISO 12183:2005 recommends a target of {+-}0.01% for the mass of original sample in the aliquot because it is a critical assay variable. Mass measurements in radiological containment were evaluated and uncertainties estimated. The uncertainty estimate for the mass measurement also includes uncertainty in correcting for buoyancy effects from air acting as a fluid and from decreased pressure of heated air from the specific heat of the plutonium isotopes.

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We have performed extensive numerical studies of quasi-phase-matched optical parametric amplification with the aim to improve its nondegenerate spectral bandwidth. Our multi-section fan-out design calculations indicate a 35-fold increase in spectral bandwidth.

This paper presents a combinatorial study on the problem ofconstructing a sparse basis forthe null-space of a sparse, underdetermined, full rank matrix, A. Such a null-space is suitable forsolving solving many saddle point problems. Our approach is to form acolumn space basis of A that has a sparse inverse, by selecting suitablecolumns of A. This basis is then used to form a sparse null-space basisin fundamental form. We investigate three different algorithms forcomputing the column space basis: Two greedy approaches that rely onmatching, and a third employing a divide and conquer strategy implementedwith hypergraph partitioning followed by the greedy approach. We alsodiscuss the complexity of selecting a column basis when it is known thata block diagonal basis exists with a small given block size.

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Aerosol optical depth variation over short-term time intervals is determined from broadband observations of stars with a whole sky imager. The main difficulty in such measurements consists of accurately separating the star flux value from the non-stellar diffuse skylight. Using correction method to overcome this difficulty, the monochromatic extinction at the ground due to aerosols is extracted from heterochromatic measurements. A form of closure is achieved by comparison with simultaneous or temporally close measurements with other instruments, and the total error of the method, as a combination of random error of measurements and systematic error of calibration and model, is assessed as being between 2.6 and 3% rms.

The effect of aerosols on the clouds, or the so-called aerosol indirect effect (AIE), is highly uncertain (Penner et al. 2001). The estimation of the AIE can vary from 0.0 to -4.8 W/m2 in Global Climate Models (GCM). Therefore, it is very important to investigate these interactions and cloud-related physical processes further. The Aerosol Intensive Operation Period (AIOP) at the Southern Great Plains (SGP) site in May 2003 dedicated some effort towards the measurement of the Cloud Condensation Nucleus concentration (CCN) as a function of super-saturation and in relating CCN concentration to aerosol composition and size distribution. Furthermore, airborn measurement for the cloud droplet concentration was also available. Therefore this AIOP provides a good opportunity to examine the AIE. In this study, we use a Cloud Resolving Model (CRM), i.e., Active Tracer High-resolution Atmospheric Model (ATHAM), to discuss the effect of aerosol loadings on cloud droplet effective radius (Re) and concentration. The case we examine is a stratiform cloud that occurred on May 17, 2003.

The problem of the choice of the aerosol optical constants and, in particular, imaginary part of the refractive index of particles in visible and infrared (IR) wavelength ranges is very important for calculation of the global albedo of the atmosphere in climatic models. The available models of the aerosol optical constants obtained for the prescribed chemical composition of particles (see, for example, Ivlev et al. 1973; Ivlev 1982; Volz 1972), often are far from real aerosol. It is shown in (Krekov et al. 1982) that model estimates of the optical characteristics of the atmosphere depending on the correctness of real and imaginary parts of the aerosol complex refractive index can differ by some hundreds percent. It is known that the aerosol extinction coefficient {alpha}({lambda}) obtained from measurements on a long horizontal path can be represented as {alpha}({lambda})={sigma}({lambda})+{beta}({lambda}), where {sigma} is the directed light scattering coefficient, and {beta} is the aerosol absorption coefficient. The coefficient {sigma}({lambda}) is measured by means of a nephelometer. Seemingly, if measure the values {alpha}({lambda}) and {sigma}({lambda}), it is easy to determine the value {beta}({lambda}). However, in practice it is almost impossible for a number of reasons. Firstly, the real values {alpha}({lambda}) and {sigma}({lambda}) are very close …

Water vapor is well known to be a critical component in many aspects of atmospheric research, such as radiative transfer and cloud and aerosol processes. This requires both improved measurements of the columnar water vapor and its profiles in the atmosphere in a wide range of conditions, and adjustment of water vapor parameterizations in radiation codes including the perfection of spectroscopic parameters. In this paper we will present the results of comparison of our calculations and downward solar fluxes measured with Rotating Shadowband Spectroradiometer under conditions of horizontally homogeneous clouds. We also will discuss the sensitivity of atmospheric radiation characteristics to variations of water vapor in the band 940 nm: these results may be useful for development of new methods of retrieval of the total column water vapor content (WVC) in the atmosphere from data of radiation observations.

There are currently twenty-four Multi-Filter Rotating Shadowband Radiometers (MFRSR) operating within Atmospheric Radiation Measurement (ARM). Eighteen are located within the Southern Great Plains (SGP) region, there is one at each of the North Slope of Alaska (NSA) and Tropical Western Pacific (TWP) sites, and one is part of the instrumentation of the ARM Mobile Facility. At this time there are four sites, all extended facilities within the SGP, that are equipped for a MFRSR but do not have one due to instrument failure and a lack of spare instruments. In addition to the MFRSRs, there are three other MFRSR derived instruments that ARM operates. They are the Multi-Filter Radiometer (MFR), the Normal Incidence Multi-Filter Radiometer (NIMFR) and the Narrow Field of View (NFOV) radiometer. All are essentially just the head of a MFRSR used in innovative ways. The MFR is mounted on a tower and pointed at the surface. At the SGP Central Facility there is one at ten meters and one at twenty-five meters. The NSA has a MFR at each station, both at the ten meter level. ARM operates three NIMFRs; one is at the SGP Central Facility and one at each of the NSA stations. There are …

Variations of dendrochronologic parameters, especially annual ring density, significantly reflect the physiological tree response to systematic variations of solar UV-B radiation, taking place on monthly and longer timescales during growing season. Such variations of UV-B radiation are totally governed by variations of total ozone (TO). Thus, in any dendrochronologic signal, especially for coniferous trees, there is also a recorded response to TO variations, characterizing variations of UV-B radiation. Because a monitoring of global TO distribution is regularly performed since 1979 using TOMS satellite instrumentation, there appears a possibility to reconstruct TO behavior in the past practically at any point of dendrochronologic monitoring network. The reconstruction is performed by the method of linear regression, based on significant correlation of annual ring density of coniferous trees and TO for coordinates of denrochronologic signal. The present report considers the Subarctic latitudes, which are characterized by considerable TO variations in the second half of twentieth century.

Our overall goal is identical to that of the Atmospheric Radiation Measurement (ARM) Program: the development of new and improved parameterizations of cloud-radiation effects and related processes, using ARM data at all three ARM sites, and the implementation and testing of these parameterizations in global and regional models. To test recently developed prognostic parameterizations based on detailed cloud microphysics, we have first compared single-column model (SCM) output with ARM observations at the Southern Great Plains (SGP), North Slope of Alaska (NSA) and Topical Western Pacific (TWP) sites. We focus on the predicted cloud amounts and on a suite of radiative quantities strongly dependent on clouds, such as downwelling surface shortwave radiation. Our results demonstrate the superiority of parameterizations based on comprehensive treatments of cloud microphysics and cloud-radiative interactions. At the SGP and NSA sites, the SCM results simulate the ARM measurements well and are demonstrably more realistic than typical parameterizations found in conventional operational forecasting models. At the TWP site, the model performance depends strongly on details of the scheme, and the results of our diagnostic tests suggest ways to develop improved parameterizations better suited to simulating cloud-radiation interactions in the tropics generally. These advances have made it possible to …

One of the Atmospheric Radiation Measurement (ARM) Program important goals is to develop and test radiation and cloud parameterizations of climate models using single column modeling (SCMs) (Randall et al. 1996). As forcing terms, SCMs need advection tendency of cloud condensates besides the tendencies of temperature, moisture and momentum. To compute the tendency terms of cloud condensates, 3D distribution of cloud condensates over a scale much larger than the climate model's grid scale is needed. Since they can cover a large area within a short time period, satellite measurements are useful utilities to provide advection tendency of cloud condensates for SCMs. However, so far, most satellite retrieval algorithms only retrieve vertically integrated quantities, for example, in the case of cloud ice, ice water path (IWP). To fulfill the requirement of 3D ice water content field for computing ice water advection, in this study, we develop an ice water content profile retrieval algorithm by combining the vertical distribution characteristics obtained from long-term surface radar observations and satellite high-frequency microwave observations that cover a large area. The algorithm is based on the Bayesian theorem using a priori database derived from analyzing cloud radar observations at the Southern Great Plains (SGP) site. The …

The methods of sun-photometry of the atmosphere based, for example, on interpretation of the angular distribution of radiation in the solar almucantar are widely used for retrieval of the aerosol optical characteristics. Preliminary analysis has shown that the near-horizon region also can be interesting for solving some applied problems. As is known, investigations of the structure of the daytime cloudless sky brightness at observation from the ground were carried out principally at zenith angles less than 80{sup o} in visible wavelength range. For further development of the methods it is necessary to obtain more complete data on the distribution of the cloudless sky brightness at great zenith angles of observation and wider wavelength range. The regularities of formation of the sky brightness field in the near-horizon region and just above the horizon line are considered in this paper.