The zone refining process was applied to Pu metal containing known amounts of impurities. Rod specimens of plutonium metal were melted into and contained in tantalum boats, each of which was passed horizontally through a three-turn, high-frequency coil in such a manner as to cause a narrow molten zone to pass through the Pu metal rod 10 times. The impurity elements Co, Cr, Fe, Ni, Np, U were found to move in the same direction as the molten zone as predicted by binary phase diagrams. The elements Al, Am, and Ga moved in the opposite direction of the molten zone as predicted by binary phase diagrams. As the impurity alloy was zone refined, {delta}-phase plutonium metal crystals were produced. The first few zone refining passes were more effective than each later pass because an oxide layer formed on the rod surface. There was no clear evidence of better impurity movement at the slower zone refining speed. Also, constant or variable coil power appeared to have no effect on impurity movement during a single run (10 passes). This experiment was the first step to developing a zone refining process for plutonium metal.

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Free radicals, elemental and van der Waals clusters and transition state species for bimolecular chemical reactions are investigated using anion photoelectron spectroscopy. Several low-lying electronic states of ozone have been identified via photoelectron spectroscopy of O{sub 3}{sup {minus}}. A characterization of these states is important to models for atmospheric ozone reaction kinetics. The fluoroformyloxyl radical, FCO{sub 2}, has been investigated, providing vibrational frequencies and energies for two electronic states. The technique has also been employed to make the first direct observation and characterization of the NNO{sub 2} molecule. Several electronic states are observed for this species which is believed to play a role as a reactive intermediate in the N + NO{sub 2} reaction. The experimental results for all three of these radicals are supplemented by ab initio investigations of their molecular properties. The clusters investigations include studies of elemental carbon clusters (C{sub 2}{sup {minus}} {minus} C{sub 11}{sup {minus}}), and van der Waals clusters (X{sup {minus}}(CO{sub 2}){sub n}, X = I, Br, Cl; n {le} 13 and I{sup {minus}} (N{sub 2}O){sub n=1--11}). Primarily linear clusters are observed for the smaller carbon clusters, while the spectra of the larger clusters contain contribution from cyclic anion photodetachment. Very interesting ion-solvent interactions are …

A discrete variable representation (DVR) suitable for treating the quantum scattering of a low energy electron from a hydrogen atom is presented. The benefits of DVR techniques (e.g. the removal of the requirement of calculating multidimensional potential energy matrix elements and the availability of iterative sparse matrix diagonalization/inversion algorithms) have for many years been applied successfully to studies of quantum molecular scattering. Unfortunately, the presence of a Coulomb singularity at the electrically unshielded center of a hydrogen atom requires high radial grid point densities in this region of the scattering coordinate, while the presence of finite kinetic energy in the asymptotic scattering electron also requires a sufficiently large radial grid point density at moderate distances from the nucleus. The constraints imposed by these two length scales have made application of current DVR methods to this scattering event difficult.

The isotopic production cross sections and momenta of all residues with nuclear charge (Z) greater than 39 from the reaction of 26, 40, and 50 MeV/nucleon {sup 129}Xe + Be, C, and Al were measured. The isotopic cross sections, the momentum distribution for each isotope, and the cross section as a function of nuclear charge and momentum are presented here. The new cross sections are consistent with previous measurements of the cross sections from similar reaction systems. The shape of the cross section distribution, when considered as a function of Z and velocity, was found to be qualitatively consistent with that expected from an incomplete fusion reaction mechanism. An incomplete fusion model coupled to a statistical decay model is able to reproduce many features of these reactions: the shapes of the elemental cross section distributions, the emission velocity distributions for the intermediate mass fragments, and the Z versus velocity distributions. This model gives a less satisfactory prediction of the momentum distribution for each isotope. A very different model based on the Boltzman-Nordheim-Vlasov equation and which was also coupled to a statistical decay model reproduces many features of these reactions: the shapes of the elemental cross section distributions, the intermediate mass …

The bonding and electronics of several small carbon and semiconductor clusters containing less than ten atoms are probed using negative ion threshold photodetachment (zero electron kinetic energy, or ZEKE) spectroscopy. ZEKE spectroscopy is a particularly advantageous technique for small cluster study, as it combines mass selection with good spectroscopic resolution. The ground and low-lying electronic states of small clusters in general can be accessed by detaching an electron from the ground anion state. The clusters studied using this technique and described in this work are C{sub 6}{sup {minus}}/C{sub 6}, Si{sub n}{sup {minus}}/Si{sub n} (n = 2, 3, 4), Ge{sub 2}{sup {minus}}/Ge{sub 2}, In{sub 2}P{sup {minus}}/In{sub 2}P,InP{sub 2}{sup {minus}}/InP{sup 2}, and Ga{sub 2}As{sup {minus}}. The total photodetachment cross sections of several other small carbon clusters and the ZEKE spectrum of the I{sup {minus}}{center_dot}CH{sub 3}I S{sub N}2 reaction complex are also presented to illustrate the versatility of the experimental apparatus. Clusters with so few atoms do not exhibit bulk properties. However, each specie exhibits bonding properties that relate to the type of bonding found in the bulk. C{sub 6}, as has been predicted, exhibits a linear cumulenic structure, where double bonds connect all six carbon atoms. This double bonding reflects how important …

The Differential Microwave Radiometer (DMR) aboard the COBE satellite has detected anisotropies in the cosmic microwave background (CMB) radiation. A two-point correlation function analysis which helped lead to this discovery is presented in detail. The results of a correlation function analysis of the two year DMR data set is presented. The first and second year data sets are compared and found to be reasonably consistent. The positive correlation for separation angles less than {approximately}20{degree} is robust to Galactic latitude cuts and is very stable from year to year. The Galactic latitude cut independence of the correlation function is strong evidence that the signal is not Galactic in origin. The statistical significance of the structure seen in the correlation function of the first, second and two year maps is respectively > 9{sigma}, > 10{sigma} and > 18{sigma} above the noise. The noise in the DMR sky maps is correlated at a low level. The structure of the pixel temperature covariance matrix is given. The noise covariance matrix of a DMR sky map is diagonal to an accuracy of better than 1%. For a given sky pixel, the dominant noise covariance occurs with the ring of pixels at an angular separation of …

An integrated exposure and carcinogenic risk assessment model for organic contamination in soil, SoilRisk, was developed and used for evaluating the risk implications of both site-specific and uniform-concentration approaches to setting soil remediation goals at hazardous-waste-contaminated sites. SoilRisk was applied to evaluate the uncertainty in the risk estimate due to uncertainty in site conditions at a representative site. It was also used to evaluate the variability in risk across a region of sites that can occur due to differences in site characteristics that affect contaminant transport and fate when a uniform concentration approach is used. In evaluating regional variability, Ross County, Ohio and the State of Ohio were used as examples. All analyses performed considered four contaminants (benzene, trichloroethylene (TCE), chlordane, and benzo[a]pyrene (BAP)) and four exposure scenarios (commercial, recreational and on- and offsite residential). Regardless of whether uncertainty in risk at a single site or variability in risk across sites was evaluated, the exposure scenario specified and the properties of the target contaminant had more influence than variance in site parameters on the resulting variance and magnitude of the risk estimate. In general, variance in risk was found to be greater for the relatively less degradable and more mobile …

Many granular materials, including sedimentary rocks and soils, contain clay particles in the pores, grain contacts, or matrix. The amount and location of the clays and fluids can influence the mechanical and hydraulic properties of the granular material. This research investigated the mechanical effects of clay at grain-to-grain contacts in the presence of different fluids. Laboratory seismic wave propagation tests were conducted at ultrasonic frequencies using spherical glass beads coated with Montmorillonite clay (SWy-1) onto which different fluids were adsorbed. For all bead samples, seismic velocity increased and attenuation decreased as the contact stiffnesses increased with increasing stress demonstrating that grain contacts control seismic transmission in poorly consolidated and unconsolidated granular material. Coating the beads with clay added stiffness and introduced viscosity to the mechanical contact properties that increased the velocity and attenuation of the propagating seismic wave. Clay-fluid interactions were studied by allowing the clay coating to absorb water, ethyl alcohol, and hexadecane. Increasing water amounts initially increased seismic attenuation due to clay swelling at the contacts. Attenuation decreased for higher water amounts where the clay exceeded the plastic limit and was forced from the contact areas into the surrounding open pore space during sample consolidation. This work investigates …

Vitrification has been declared by the Environmental Protection Agency (USEPA) as the Best Demonstrated Available Technology (BDAT) for the permanent disposal of high-level radioactive waste. Savannah River Site currently uses a sodium tetraphenylborate (NaTPB) precipitation process to remove Cs-137 from a wastewater solution created from the processing of nuclear fuel. This process has several disadvantages such as the formation of a benzene waste stream. It has been proposed to replace the precipitation process with an ion exchange process using a new resorcinol-formaldehyde resin developed by Savannah River Technical Center (SRTC). Preliminary tests, however, showed that problems such as crust formation and a reduced final glass wasteform exist when the resin is placed in the melter environment. The newly developed stirred melter could be capable of overcoming these problems. This research explored the operational feasibility of using the stirred tank melter to vitrify an organic ion exchange resin. Preliminary tests included crucible studies to determine the reducing potential of the resin and the extent of oxygen consuming reactions and oxygen transfer tests to approximate the extent of oxygen transfer into the molten glass using an impeller and a combination of the impeller and an external oxygen transfer system. These preliminary studies …