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In Situ Real-Time Radiographic Study of Thin Film Formation Inside Rotating Hollow Spheres
Hollow spheres with uniform coatings on the inner surface have applications in optical devices, time- or site controlled drug release, heat storage devices, and target fabrication for inertial confinement fusion experiments. The fabrication of uniform coatings, which is often critical for the application performance, requires precise understanding and control over the coating process and its parameters. Here, we report on in-situ real-time radiography experiments that provide critical spatio-temporal information about the distribution of fluids inside hollow spheres during uniaxial rotation. Image analysis and computer fluid dynamics simulations were used to explore the effect of liquid viscosity and rotational velocity on the film uniformity. The data were then used to demonstrate the fabrication of uniform sol-gel chemistry derived porous polymer films inside 2mm inner diameter diamond shells.
Pulsed Sphere Time of Flight Neutron Spectrum Measurements: Blank Run and 1.8 Mean-Free-Path thick Polyethylene Moderating Sphere
From the late 1960s to 1985, Lawrence Livermore National Laboratory (LLNL) undertook a series of ‘pulsed sphere’ experiments for 32 materials involving 148 different experiments using 75 different spheres to measure the neutron leakage spectra for different materials from 14-MeV neutrons generated by 3 H(d, n) 4 He reactions induced by an incident D+ beam from the Insulated Core Transformer (ICT) accelerator at LLNL. This deuteron beam was focused to impinge on tritium loaded onto a titanium substrate within a low mass target assembly placed within the center of a spherical shell constructed from the material of interest. The neutron time of flight was measured at a detector outside a collimator. The program was intended to be comprehensive with numerous targets of various thicknesses spanning the periodic table from H to 239 Pu. Five different neutron detectors were utilized to avoid possible systematic errors due to differences in detector responses. Further, these measurements were designed with the aim that the simple geometry of the measurements could be easily simulated to validate Monte Carlo transport codes and nuclear data libraries. As a result, these benchmarks have been extensively used in the validation of ENDL, ENDF and other libraries. Two experiments selected as benchmark cases in this evaluation are: 1) target assembly without material sphere (blank run), and 2) target assembly with a hollow polyethylene sphere, 1.8 mean free path (mfp) or 16.56 cm thick.
Graphitized hollow carbon spheres and yolk-structured carbon spheres fabricated by metal-catalyst-free chemical vapor deposition
Hard-sphere-templating method has been widely used to synthesize hollow carbon spheres (HCSs), in which the spheres were firstly coated with a carbon precursor, followed by carbonization and core removal. The obtained HCSs are generally amorphous or weakly graphitized (with the help of graphitization catalysts). In this work, we report on the fabrication of graphitized HCSs and yolk–shell Au@HCS nanostructures using a modified templating method, in which smooth, uniform graphene layers were grown on SiO 2 spheres or Au@SiO 2 nanoparticles via metal-catalyst-free chemical vapor deposition (CVD) of methane. Furthermore, our work not only provides a new method to fabricate high-quality, graphitized HCSs but also demonstrates a reliable approach to grow quality graphene on oxide surfaces using CVD without the presence of metal catalysts.
Charge and force on a conductive sphere between two parallel electrodes: A Stokesian dynamics approach
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SPHERES Synchronized, Position, Hold, Engage, Reorient, Experimental Satellites: SPHERES Working Group (SWG) Quarterly Meeting
SPHERES Working Group (SWG) Quarterly meeting. Membership includes MIT, FIT, AFS, DARPA, CASIS, SJSU, and NASA (HQ, KSC, JSC, MSFC, and ARC). Face-to-Face, twice a year. Next Face-to-Face will be scheduled in Feb. 2017 at NASA Ames. Purpose: Information sharing across the SPHERES community. Program office shares National Lab Facility availability. Status of resources (batteries, CO2 tanks, etc.), Overall Calendar (scheduled Test Sessions, upmassreturn), and Updates on new PD, Investigations, and ISS infrastructure.Provide the SPHERES community (PD, investigators, etc.) with up-to-date information to determine opportunities to use the NL Facility. Discuss proposed changes updates to SPHERES Nat Lab which may be required to support a specific activity or research. Discuss specific support requests made to the ISS Office.
Time-resolved PIV measurements in a low-aspect ratio facility of randomly packed spheres and flow analysis using modal decomposition
This work experimentally investigated the flow characteristics in a facility with randomly packed spheres at a low-aspect ratio of 4.4. Velocity fields in the near-wall region and in the pores between spheres were obtained by employing the matched-index-of-refraction (MIR) and time-resolved particle image velocimetry (TR-PIV) techniques for Reynolds numbers of 340, 520, and 720. From the obtained TR-PIV velocity vector fields, flow characteristics including first- and second-order statistics, such as mean velocity, root-mean-square fluctuating velocity, and Reynolds stress profiles, were computed. The effects of the wall enclosure and Reynolds numbers on the flow patterns were investigated by comparing the computed flow statistics and evaluating two-point cross correlations of the velocities measured adjacent to and far from the wall. Comparisons of the mean velocities, root-mean-square fluctuating velocities, and Reynolds stress component showed an increase in flow mixing and turbulent intensity in the gaps between spheres in the packed bed. The re-circulation-region sizes, however, were found to be independent from an increase in Reynolds numbers. Finally, flow modal decompositions, such as the proper orthogonal decomposition (POD) and dynamic mode decomposition (DMD), were applied to the vorticity fields extracted from sub-regions located near and far from the wall to reveal the most dominant POD and DMD flow structures.
Optimizing conditions for utilization of an H 2 oxidation catalyst with outer coordination sphere functionalities
[Ni(PCy2NArginine2)2]2+ ( CyArg ) or [Ni(PCy2NBenzyl2)2]2+ ( CyBn ) were evaluated for H 2 oxidation as a function of temperature, pressure, and solvent. 70 °C and 100 atm H 2 result in a TOF of 1.1 × 106 s -1 and an overpotential of 240 mV for CyArg in water. In methanol the rates were 280 s -1 for CyArg and 80 s -1 for CyBn , demonstrating the importance of water and the outer coordination sphere ( OCS ).
Plane shear flows of frictionless spheres: Kinetic theory and 3D soft-sphere discrete element method simulations
We use existing 3D Discrete Element simulations of simple shear flows of spheres to evaluate the radial distribution function at contact that enables kinetic theory to correctly predict the pressure and the shear stress, for different values of the collisional coefficient of restitution. Then, we perform 3D Discrete Element simulations of plane flows of frictionless, inelastic spheres, sheared between walls made bumpy by gluing particles in a regular array, at fixed average volume fraction and distance between the walls. The results of the numerical simulations are used to derive boundary conditions appropriated in the cases of large and small bumpiness. Those boundary conditions are, then, employed to numerically integrate the differential equations of Extended Kinetic Theory, where the breaking of the molecular chaos assumption at volume fraction larger than 0.49 is taken into account in the expression of the dissipation rate. We show that the Extended Kinetic Theory is in very good agreement with the numerical simulations, even for coefficients of restitution as low as 0.50. When the bumpiness is increased, we observe that some of the flowing particles are stuck in the gaps between the wall spheres. As a consequence, the walls are more dissipative than expected, and the flows resemble simple shear flows, i.e., flows of rather constant volume fraction and granular temperature.
Radiative energy and momentum transfer for various spherical shapes: A single sphere, a bubble, a spherical shell, and a coated sphere
We use fluctuational electrodynamics to determine spectral emissivity and van der Waals contribution to surface energy for various spherical shapes, such as a sphere, a bubble, a spherical shell, and a coated sphere, in a homogeneous and isotropic medium. The dyadic Green's function formalism of radiative energy and fluctuation-induced van der Waals stress for different spherical configurations has been developed. We show (1) emission spectra of micro- and nano-sized single and coated spheres display several emissivity sharp peaks as the size of object reduces and (2) surface energy becomes size dependent due to van der Waals phenomena when size of object is reduced to a nanoscopic length scale.
The Role of a Dipeptide Outer-Coordination Sphere on H2 -Production Catalysts: Influence on Catalytic Rates and Electron Transfer
The outer-coordination sphere of enzymes acts to fine-tune the active site reactivity and control catalytic rates, suggesting that incorporation of analogous structural elements into molecular catalysts may be necessary to achieve rates comparable to those observed in enzyme systems at low overpotentials. In this work, we evaluate the effect of an amino acid and dipeptide outer-coordination sphere on [Ni(PPh2NPh-R2)2]2+ hydrogen production catalysts. A series of 12 new complexes containing non-natural amino acids or dipeptides were prepared to test the effects of positioning, size, polarity and aromaticity on catalytic activity. The non-natural amino acid was either 3-(meta- or para-aminophenyl)propionic acid terminated as an acid, an ester or an amide. Dipeptides consisted of one of the non-natural amino acids coupled to one of four amino acid esters: alanine, serine, phenylalanine or tyrosine. All of the catalysts are active for hydrogen production, with rates averaging ~1000 s-1, 40% faster than the unmodified catalyst. Structure and polarity of the aliphatic or aromatic side chains of the C-terminal peptide do not strongly influence rates. However, the presence of an amide bond increases rates, suggesting a role for the amide in assisting catalysis. Overpotentials were lower with substituents at the N-phenyl meta position. This is consistent with slower electron transfer in the less compact, para-substituted complexes, as shown in digital simulations of catalyst cyclic voltammograms and computational modeling of the complexes. Combining the current results with insights from previous results, we propose a mechanism for the role of the amino acid and dipeptide based outer-coordination sphere in molecular hydrogen production catalysts.
Splitting of magnetic dipole modes in anisotropic TiO 2 micro-spheres: Splitting of magnetic dipole modes in anisotropic TiO 2 micro-spheres
Monocrystalline titanium dioxide (TiO 2 ) micro-spheres support two orthogonal magnetic dipole modes at terahertz (THz) frequencies due to strong dielectric anisotropy. For the first time, we experimentally detected the splitting of the first Mie mode in spheres of radii inline imagem through near-field time-domain THz spectroscopy. By fitting the Fano lineshape model to the experimentally obtained spectra of the electric field detected by the sub-wavelength aperture probe, we found that the magnetic dipole resonances in TiO 2 spheres have narrow linewidths of only tens of gigahertz. Lastly, anisotropic TiO 2 micro-resonators can be used to enhance the interplay of magnetic and electric dipole resonances in the emerging THz all-dielectric metamaterial technology.
Probing the evolution and morphology of hard carbon spheres
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A theory of interactions between polarizable dielectric spheres
Surface charging or polarization can strongly affect the nature of interactions between charged dielectric objects, particularly when sharp dielectric discontinuities are involved. The perturbative theory presented here efficiently accounts for this effect by introducing a generalized image method that enables the rapid evaluation of the electrostatic energies and forces that arise in many-body systems. The theory is validated by comparison to full numerical solutions. The importance of polarizability is then examined in the context of clusters of dielectric spheres, as well as a periodic crystal of charged dielectric spheres arranged into an NaCl-type lattice.
Evaluation of Attractive Interactions in the Second Coordination Sphere of Iron Complexes Containing Pendant Amines
The interactions between pendant amines in the second coordination sphere and ligands in the first coordination sphere are important for understanding the structures and reactivity of complexes containing PR2NR'2 ligands, which have been shown to be highly active H2 oxidation/production catalysts. A series of [Fe(PPh2NBn2)2(X)(Y)]n+ complexes have been prepared and structurally characterized. These complexes have two different ligands with which the pendant amines of the diphosphine ligand can interact. The solid state structure of cis-Fe(PPh2NBn2)2Cl2 reveals that the six-membered rings adjacent to the P atoms are in a boat confirmation, resulting in close N•••P distances that suggests the P atoms have a greater affinity for the lone pair of electrons on the N atom than chloride ligands. Similarly, boat conformations are observed for both rings adjacent to the hydride ligands of trans-[HFe(PPh2NBn2)2(CH3CN)]+ and trans-HFe(PPh2NBn2)2Cl, resulting in short N•••H distances. Spectroscopic and computational studies of trans-[HFe(PPh2NBn2)2(CO)]+, trans-[HFe(PPh2NBn2)(PPh2NBn2H)(CO)]2+, and trans-[HFe(PPh2NBn2)2(H2)]+ indicate the complexes are more stable when the pendant amines in boat conformations are adjacent to the hydride ligand. These data suggest an attractor ordering of H- > CO > H2 > PR3 > Cl- ~ CH3CN. This work was supported by the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory (PNNL) is operated by Battelle for the U.S. DOE. Computations were performed using the Cascade supercomputer at the Environmental Molecular Sciences Laboratory, a National Scientific User Facility sponsored by the DOE’s Office of Biological and Environmental Research and located at PNNL.
Flash Kα radiography of laser-driven solid sphere compression for fast ignition
Time-resolved compression of a laser-driven solid deuterated plastic sphere with a cone was measured with flash Kα x-ray radiography. A spherically converging shockwave launched by nanosecond GEKKO XII beams was used for compression while a flash of 4.51 keV Ti Kα x-ray backlighter was produced by a high-intensity, picosecond laser LFEX (Laser for Fast ignition EXperiment) near peak compression for radiography. Areal densities of the compressed core were inferred from two-dimensional backlit x-ray images recorded with a narrow-band spherical crystal imager. The maximum areal density in the experiment was estimated to be 87 ± 26 mg/cm{sup 2}. The temporal evolution of the experimental and simulated areal densities with a 2-D radiation-hydrodynamics code is in good agreement.
Sphere-by-Sphere Manufacturing of 3D Microscale Granular Materials
Two of the central challenges in the mechanical design of components in nuclear systems are the dissipation of energy from external shocks and the localization of energy in energetic materials. This research seeks to address these problems by developing a patterned granular microstructure that can be optimized to direct or impede the transfer of energy carried by stress waves. Such structures require the development of a manufacturing technique that can yield perfectly ordered lattices. Two branches of research are detailed here: the development of a sphere-by-sphere additive manufacturing technique, and the development of a framework for modeling the technique in order to guide future improvements. Proof of concept of the method is demonstrated, and recommendations for future work are made.