The chemistry of Br species associated with sea salt ice and aerosols has been implicated in the episodes of ozone depletion reported at Arctic sunrise. However, Br{sup -} is only a minor component in sea salt, which has a Br{sup -}/Cl{sup -} molar ratio of {approx}0.0015. Sea salt is a complex mixture of many different species, with NaCl as the primary component. In recent years experimental and theoretical studies have reported enhancement of the large, more polarizable halide ion at the liquid/vapor interface of corresponding aqueous alkali halide solutions. The proposed enhancement is likely to influence the availability of sea salt Br{sup -} for heterogeneous reactions such as those involved in the ozone depletion episodes. We report here ambient pressure x-ray photoelectron spectroscopy studies and molecular dynamics simulations showing direct evidence of Br{sup -} enhancement at the interface of an aqueous NaCl solution doped with bromide. The experiments were carried out on samples with Br{sup -}/Cl{sup -} ratios in the range 0.1% to 10%, the latter being also the ratio for which simulations were carried out. This is the first direct measurement of interfacial enhancement of Br{sup -} in a multi-component solution with particular relevance to sea salt chemistry.

Plasma density gradients in a gas jet were used to control the wake phase velocity and trapping threshold in a laser wakefield accelerator, producing stable electron bunches with longitudinal and transverse momentum spreads more than ten times lower than in previous experiments (0.17 and 0.02 MeV/c FWHM, respectively) and with central momenta of 0.76 +- 0.02 MeV/c. Transition radiation measurements combined with simulations indicated that the bunches can be used as a wakefield accelerator injector to produce stable beams with 0.2 MeV/c-class momentum spread at high energies.

The non-equilibrium dynamics of mixing, oscillations and equilibration is studied in a field theory of flavored neutral mesons that effectively models two flavors of mixed neutrinos, in interaction with other mesons that represent a thermal bath of hadrons or quarks and charged leptons. This model describes the general features of neutrino mixing and relaxation via charged currents in a medium. The reduced density matrix and the non-equilibrium effective action that describes the propagation of neutrinos is obtained by integrating out the bath degrees of freedom. We obtain the dispersion relations, mixing angles and relaxation rates of ``neutrino'' quasiparticles. The dispersion relations and mixing angles are of the same form as those of neutrinos in the medium, and the relaxation rates are given by $\Gamma_1(k) = \Gamma_{ee}(k) \cos^2\theta_m(k)+\Gamma_{\mu\mu}(k)\sin^2\theta_m(k); \Gamma_2(k)= \Gamma_{\mu\mu}(k) \cos^2\theta_m(k)+\Gamma_{ee}(k)\sin^2\theta_m(k) $ where $\Gamma_{\alpha\alpha}(k)$ are the relaxation rates of the flavor fields in \emph{absence} of mixing, and $\theta_m(k)$ is the mixing angle in the medium. A Weisskopf-Wigner approximation that describes the asymptotic time evolution in terms of a non-hermitian Hamiltonian is derived. At long time $>>\Gamma^{-1}_{1,2}$ ``neutrinos'' equilibrate with the bath. The equilibrium density matrix is nearly diagonal in the basis of eigenstates of an \emph{effective Hamiltonian that includes self-energy corrections …

Detailed models for hydrogen storage systems provide essential design information about flow and temperature distributions, as well as, the utilization of a hydrogen storage media. However, before constructing a detailed model it is necessary to know the geometry and length scales of the system, along with its heat transfer requirements, which depend on the limiting reaction kinetics. More fundamentally, before committing significant time and resources to the development of a detailed model, it is necessary to know whether a conceptual storage system design is viable. For this reason, a hierarchical system of models progressing from scoping models to detailed analyses was developed. This paper, which discusses the scoping models, is the first in a two part series that presents a collection of hierarchical models for the design and evaluation of hydrogen storage systems.

There is significant interest in hydrogen storage systems that employ a media which either adsorbs, absorbs or reacts with hydrogen in a nearly reversible manner. In any media based storage system the rate of hydrogen uptake and the system capacity is governed by a number of complex, coupled physical processes. To design and evaluate such storage systems, a comprehensive methodology was developed, consisting of a hierarchical sequence of models that range from scoping calculations to numerical models that couple reaction kinetics with heat and mass transfer for both the hydrogen charging and discharging phases. The scoping models were presented in Part I [1] of this two part series of papers. This paper describes a detailed numerical model that integrates the phenomena occurring when hydrogen is charged and discharged. A specific application of the methodology is made to a system using NaAlH{sub 4} as the storage media.

Uranium-lead ratios (commonly represented as {sup 238}U/{sup 204}Pb = {mu}) calculated for the sources of martian basalts preserve a record of petrogenetic processes that operated during early planetary differentiation and formation of martian geochemical reservoirs. To better define the range of {mu} values represented by the source regions of martian basalts, we completed U-Pb elemental and isotopic analyses on whole rock, mineral and leachate fractions from the martian meteorite Queen Alexandra Range 94201 (QUE 94201). The whole rock and silicate mineral fractions have unradiogenic Pb isotopic compositions that define a narrow range ({sup 206}Pb/{sup 204}Pb = 11.16-11.61). In contrast, the Pb isotopic compositions of weak HCl leachates are more variable and radiogenic. The intersection of the QUE 94201 data array with terrestrial Pb in {sup 206}Pb/{sup 204}Pb-{sup 207}Pb/{sup 204}Pb-{sup 208}Pb/{sup 204}Pb compositional space is consistent with varying amounts of terrestrial contamination in these fractions. We calculate that only 1-7% contamination is present in the purified silicate mineral and whole rock fractions, whereas the HCl leachates contain up to 86% terrestrial contamination. Despite the contamination, we are able to use the U-Pb data to determine the initial {sup 206}Pb/{sup 204}Pb of QUE 94201 (11.086 {+-} 0.008) and calculate the {mu} value …

The performance of parallel Monte Carlo transport calculations which use both spatial and particle parallelism is increased by dynamically assigning processors to the most worked domains. Since the particle work load varies over the course of the simulation, this algorithm determines each cycle if dynamic load balancing would speed up the calculation. If load balancing is required, a small number of particle communications are initiated in order to achieve load balance. This method has decreased the parallel run time by more than a factor of three for certain criticality calculations.

Absolute line emission cross sections are presented for 1 keV/amu charge exchange collisions of multiply charged solar wind ions with H{sub 2}O, H, O, CO{sub 2}, and CO cometary targets. The present calculations are contrasted with available laboratory data. A parameter-free model is used to successfully predict the recently observed x-ray spectra of comet C/LINEAR 1999 S4. We show that the resulting spectrum is extremely sensitive to the time variations of the solar wind composition. Our results suggest that orbiting x-ray satellites may be a viable way to predict the solar wind intensities and composition on the Earth many hours before the ions reach the earth.

Ablative targets for the National Ignition Campaign (NIC) have been fabricated by sputter coating spherical mandrels made of glow discharge polymer (GDP) with graded copper doped beryllium (Be) layers. The inner mandrel must be completely removed to meet specific ignition design requirements. The process of removing the mandrel requires elevated temperature in the presence of oxygen. However, elevating the temperature in air also oxidizes the Be and can cause blistering on the inner surface of the Be shell. This paper will discuss a refined technique, which removes the GDP mandrel without compromising the integrity of the inner Be surface. The oxygen gradient that develops during the mandrel removal and the impact of its presence will also be discussed.

We report on recent developments with the Purgatorio code, a new implementation of Liberman's Inferno model. This fully relativistic average atom code uses phase shift tracking and an efficient refinement scheme to provide an accurate description of continuum states. The resulting equations of state accurately represent the atomic shell-related features which are absent in Thomas-Fermi-based approaches. We discuss various representations of the exchange potential and some of the ambiguities in the choice of the effective charge Z* in average atom models, both of which affect predictions of electrical conductivities and radiative properties.

Current fluctuations of cathodic arcs were recorded withhigh analog bandwidth (up to 1 GHz) and fast digital sampling (up to 5Gsamples/sec). The power spectral density of the arc current wasdetermined by fast Fourier transform clearly showing material dependent,non-linear features in the frequency domain. These features can beassociated with the non-linear impedance of the conducting channelbetween cathode and anode, driven by the explosive nature of electronemission and plasma formation. The characteristic times of less than 100ns can be associated with individual explosive processes, "ectons," andtherefore represent the short-time physical cutoff for the fractal modelof cathodic arcs.

Soft x-ray lasers in 10-30nm range are now routinely produced in hot plasmas generated either by a laser from a solid target or by an electrical discharge in a capillary. Such an x-ray laser is a convenient tool for future applications, such as probing dense plasmas of interest for fusion experiments. Their short wavelength enables plasma diagnosis beyond the capabilities of optical lasers, because the high critical plasma density ({approx}{lambda}{sup 2}) limits the optical beam propagation. In our paper, we present analytical and numerical ray tracing of an x-ray laser in dense amplifying plasmas. A general analytical formula for a beam propagation has been developed for a gradient plasma. The simplified analytical formulaes enable better understanding of processes involved. They also simplify optimization of the beam propagation and ''mapping'' the parameter space for further studies by numerical codes. We discuss implications for a transient x-ray laser that is produced from a slab target by a (sub-)picosecond laser pulse.

Recent attention has focused on the effect of spherical convergence on the nonlinear phase of Rayleigh-Taylor growth. For instability growth on spherically converging interfaces, modifications to the predictions of the Layzer model for the secular growth of a single, nonlinear mode have been reported [D. S. Clark and M. Tabak, Phys. Rev. E 72, 0056308 (2005).]. However, this model is limited in assuming a self-similar background implosion history as well as only addressing growth from a perturbation of already nonlinearly large amplitude. Additionally, only the case of single-mode growth was considered and not the multimode growth of interest in applications. Here, these deficiencies are remedied. First, the connection of the recent nonlinear results including convergence to the well-known results for the linear regime of growth is demonstrated. Second, the applicability of the model to more general implosion histories (i.e., not self-similar) is shown. Finally, to address the case of multimode growth with convergence, the recent nonlinear single mode results are combined with the Haan model formulation for weakly nonlinear multimode growth. Remarkably, convergence in the nonlinear regime is found not to modify substantially the multimode predictions of Haan's original model.

Fluidized Bed Steam Reforming (FBSR) is being considered as an alternative technology for the immobilization of a wide variety of aqueous high sodium containing radioactive wastes at various DOE facilities in the United States. The addition of clay, charcoal, and a catalyst as co-reactants converts aqueous Low Activity Wastes (LAW) to a granular or ''mineralized'' waste form while converting organic components to CO{sub 2} and steam, and nitrate/nitrite components, if any, to N{sub 2}. The waste form produced is a multiphase mineral assemblage of Na-Al-Si (NAS) feldspathoid minerals with cage-like structures that atomically bond radionuclides like Tc-99 and anions such as SO{sub 4}, I, F, and Cl. The granular product has been shown to be as durable as LAW glass. Shallow land burial requires that the mineralized waste form be able to sustain the weight of soil overburden and potential intrusion by future generations. The strength requirement necessitates binding the granular product into a monolith. FBSR mineral products were formulated into a variety of monoliths including various cements, Ceramicrete, and hydroceramics. All but one of the nine monoliths tested met the <2g/m{sup 2} durability specification for Na and Re (simulant for Tc-99) when tested using the Product Consistency Test (PCT; …

We present the results of a series of experiments studying how visualization software scales to massive data sets. Although several paradigms exist for processing large data, we focus on pure parallelism, the dominant approach for production software. These experiments utilized multiple visualization algorithms and were run on multiple architectures. Two types of experiments were performed. For the first, we examined performance at massive scale: 16,000 or more cores and one trillion or more cells. For the second, we studied weak scaling performance. These experiments were performed on the largest data set sizes published to date in visualization literature, and the findings on scaling characteristics and bottlenecks contribute to understanding of how pure parallelism will perform at high levels of concurrency and with very large data sets.

The rate coefficient for the reaction of the ethynyl radical (C{sub 2}H) with 1-butyne (H-C{triple_bond}C-CH{sub 2}-CH{sub 3}) is measured in a pulsed Laval nozzle apparatus. Ethynyl radicals are formed by laser photolysis of acetylene (C{sub 2}H{sub 2}) at 193 nm and detected via chemiluminescence (C{sub 2}H + O{sub 2} {yields} CH (A{sup 2}{Delta}) + CO{sub 2}). The rate coefficients are measured over the temperature range of 74-295 K. The C{sub 2}H + 1-butyne reaction exhibits no barrier and occurs with rate constants close to the collision limit. The temperature dependent rate coefficients can be fit within experimental uncertainties by the expression k = (2.4 {+-} 0.5) x 10{sup -10} (T/295 K)-(0.04 {+-} 0.03) cm{sup 3} molecule{sup -1}s{sup -1}. Reaction products are detected at room temperature (295 K) and 533 Pa using a Multiplexed Photoionization Mass Spectrometer (MPIMS) coupled to the tunable VUV synchrotron radiation from the Advanced Light Source at the Lawrence Berkeley National Laboratory. Two product channels are identified for this reaction: m/z = 64 (C{sub 5}H{sub 4}) and m/z = 78 (C{sub 6}H{sub 6}) corresponding to the CH{sub 3}- and H-loss channels, respectively. Photoionization efficiency (PIE) curves are used to analyze the isomeric composition of both product channels. …

We built a bi-directional scatter diagnostics to measure and quantify losses due to scattering and absorption of harmonic conversion crystals (DKDP) for the National Ignition Facility (NIF). The main issues to be addressed are (1) amount of total energy reaching the target if the target hole was {+-}200 {micro}rad in size, (2) distribution of energy inside the target hole, (3) collateral damage of other optics by scattered light. The scatter diagnostics enables angle-resolved measurements at 351 nm, and is capable of both near specular transmission and large angle scatter measurements. In the near specular setup, the transmission can be measured within {+-}65 {micro}rad up to {+-}60 mrad acceptance angle. A silicon photo detector and a scientific-grade CCD camera provide total energy and energy distribution. A linear swing arm detection system enables large angle scatter measurements of 360{sup o}, in principal, with step sizes as small as 0.01{sup o} and different collection angle ranging between 1 and 20 mad. In this paper, scatter effects from laser damage and final finishing process of DKDP are discussed.

The RuC molecule has been a challenging species due to the open-shell nature of Ru resulting in a large number of low-lying electronic states. We have carried out state-of-the-art calculations using the complete active space multi-configuration self-consistent field (CASSCF) followed by multireference configuration interaction (MRCI) methods that included up 18 million configurations, in conjunction with relativistic effects. We have computed 29 low-lying electronic states of RuC with different spin multiplicities and spatial symmetries with energy separations less than 38 000 cm{sup -1}. We find two very closely low-lying electronic states for RuC, viz., {sup 1}{Sigma}{sup +} and {sup 3}{Delta} with the {sup 1}{Sigma}{sup +} being stabilized at higher levels of theory. Our computed spectroscopic constants and dipole moments are in good agreement with experiment although we have reported more electronic states than those that have been observed experimentally. Our computations reveal a strongly bound X{sup 1}{Sigma}{sup +} state with a large dipole moment and an energetically close {sup 3}{Delta} state with a smaller dipole moment. Overall our computed spectroscopic constants of the excited states with energy separations less than 18000 cm{sup -1} agree quite well with those of the corresponding observed states.

We present a study, based on simulations with SERDYCA, a spatially-explicit individual based model of rodent dynamics, on the connection between population persistence and the presence of inhomogeneities in the habitat. We are specifically interested on the effect that inhomogeneities that do not fragment the environment, have on population persistence. Our results suggest that a certain percentage of inhomogeneities can increase the average time to extinction of the population. Inhomogeneities decrease the population density and can increase the ratio of juveniles in the population thus providing a better chance for the population to restore itself after a severe period with critically low population density. We call this the ''inhomogeneity localization effect''.

We consider the full multinomial combinatorics of all irreducible representations of the octahedral (cubic) symmetry as a function of partitions for vertex, face and edge colorings. Full combinatorial tables for all irreducible representations and all multinomial partitions are constructed. These enumerations constitute multinomial expansions of character-based cycle index polynomials, and grow in combinatorial complexity as a function of edge or vertex coloring partitions.

We investigated chemical etching as a possible means to mitigate the growth of UV laser-induced surface damage on fused silica. The intent of this work is to examine the growth behavior of existing damage sites that have been processed to remove the UV absorbing, thermo-chemically modified material within the affected area. The study involved chemical etching of laser-induced surface damage sites on fused silica substrates, characterizing the etched sites using scanning electron microscopy (SEM) and laser fluorescence, and testing the growth behavior of the etched sites upon illumination with multiple pulses of 351nm laser light. The results show that damage sites that have been etched to depths greater than about 9 {micro}m have about a 40% chance for zero growth with 1000 shots at fluences of 6.8-9.4 J/cm{sup 2}. For the etched sites that grow, the growth rates are consistent with those for non-etched sites. There is a weak dependence of the total fluorescence emission with the etch depth of a site, but the total fluorescence intensity from an etched site is not well correlated with the propensity of the site to grow. Deep wet etching shows some promise for mitigating damage growth in fused silica, but fluorescence does not …

A new technique is described for the isochoric heating (i.e., heating at constant volume) of matter to high energy-density plasma states (>10{sup 5} J/g) on a picosecond timescale (10{sup -12} sec). An intense, collimated, ultrashort-pulse beam of protons--generated by a high-intensity laser pulse--is used to isochorically heat a solid density material to a temperature of several eV. The duration of heating is shorter than the timescale for significant hydrodynamic expansion to occur, hence the material is heated to a solid density warm dense plasma state. Using spherically-shaped laser targets a focused proton beam is produced and used to heat a smaller volume to over 20 eV. The technique described of ultrafast proton heating provides a unique method for creating isochorically heated high-energy density plasma states.

The character theory of relativistic double group spinor representations is developed in order to represent the total rovibronic states of non-rigid molecules. It is shown that the double groups can be represented in terms of wreath products and powerful matrix cycle type generators that are used to construct their character tables. It is shown that these tables are of use when spin-orbit coupling is included in the hamiltonian even for molecules containing lighter atoms. Applications to non-rigid molecules such as Tl{sub 2}H{sub 4} /Tl{sub 2}H{sub 4}{sup +} are considered. It is shown that the tunneling splittings and the nuclear spin statistical weights can be obtained for such species using the character tables thus constructed. The spinor double groups of several other molecules such as hexamethyl dilead and heavy weakly bound clusters such as (PoH{sub 2}){sub 4} are also considered.

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