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At least 73 records · Page 4

Oscillatory domain dynamics in GUVs immersed in hypotonic bath.

Time-lapse images of a bottom view of GUVs consisting of POPC:SM:Ch (1:1:1) labeled with 0.5% Rho-DPPE (pseudo-colored magenta) under a net osmotic differential. The GUVs encapsulate 1 M sucrose in their interior, and the external dispersion medium is MilliQ water. A striking temporal pattern of oscillatory phase separation revealing appearance, coalescence, and dispersion of optically resolved domains is evident (see manuscript for details).

59 BASIC BIOLOGICAL SCIENCES↗

Multiscale Analysis of Nonlinear Systems Using Computational Topology

Computational Homology in Fluids: M. Schatz, K. Mischaikow. This effort focused on characterizing both the structure and dynamics of complex spatio-temporal flows that arise in thermal convection. Microstructure Characterization: T. Wanner, K. Mischaikow. We extended our previous work on studying the time evolution of patterns associated with phase separation in conserved concentration fields. Probabilistic Homology Validation: W. Kalies, T. Wanner, K. Mischaikow. Our above mentioned work on microstructure characterization is based on numerically studying the homology of certain sublevel sets of a function, whose evolution is described by deterministic or stochastic evolution equations. Computational Homology and Dynamics: W. Kalies, T. Wanner, K. Mischaikow. Topological methods can be used to rigorously describe the dynamics of nonlinear systems. We are approaching this problem from several perspectives and through a variety of systems. Stress Networks in Polycrystals: T. Wanner. Together with E. Fuller (NIST) and D. Saylor (FDA) we have characterized stress networks in polycrystals. This part of the project is aimed at developing homological metrics which can aid in distinguishing not only microstructures, but also derived mechanical response fields. Microstructure-Controlled Drug Release: K. Mischaikow, T. Wanner. This part of the project is concerned with the development of topological metrics in the context of controlled drug delivery systems, such as drug-eluting stents. We are particularly interested in developing metrics which can be used to link the processing stage to the resulting microstructure, and ultimately to the achieved system response in terms of drug release profiles. Microstructure of Fuel Cells: W. Kalies, K. Mischaikow. In collaboration with P. Voorhees (Northwestern Univ.) and M. Gameiro (Rutgers) we have been using our computational homology software to analyze the topological structure of the void, metal and ceramic components of a Solid Oxide Fuel Cell.

97 MATHEMATICS AND COMPUTING↗

Electronic structures on swollen hydrogels

This document describes a conformable substrate that includes a hydrogel having adhesion-promoting moieties, said adhesion-promoting moieties comprising one or more catechol groups. The conformable substrate includes an array of microelectrodes bonded to the hydrogel by the adhesion-promoting moieties via the one or more catechol groups. This document also describes a method for transfer printing of an electronic structure to a hydrogel. The method includes the steps of coating a donor substrate with a film of polyacrylic acid, crosslinking the film of polyacrylic acid in a solution comprising divalent ions, patterning a microelectrode array onto the crosslinked film of polyacrylic acid, laminating an adhesive hydrogel substrate onto the donor substrate coated by the crosslinked film of polyacrylic acid comprising the patterned microelectrode array, and separating the crosslinked film of polyacrylic acid from the donor substrate in a monovalent solution.

Bettinger, Christopher J.↗

Criticality safety analysis of spent fuel storage or handling disposals using burnup credit - loading curve calculation - 14445

MILLENNIUM and REEL SAS Companies have shared their own experience to develop a neutron and criticality calculations chain in order to perform isotopic composition predictions of spent fuel after irradiation in a reactor and criticality analysis of fuel storages taking into account burnup credit. The whole calculation sequence is divided into three steps, all calling SCALE 6.1.2 modules. The first two steps are dedicated to the evaluation of isotopic compositions of burnt fuel. As transport and depletion calculations in three dimensions appears to be way too long for the whole core (about several months), dealing with each fuel assembly one by one is the alternative solution MILLENNIUM and REEL SAS commonly chose to study. Therefore, the first step aims at determining the axial burnup profile of a given fuel assembly using a 3-D model with infinite reflections on lateral axes. The T6-depl sequence of TRITON module coupling KENO-VI and ORIGEN-S was used in this step. Sensitivity studies confirmed that addition of the 8 closest neighbors of the studied fuel assembly in the model has an insignificant impact on the axial burnup profile. However, fuel assemblies in the peripheral zone of the core must be treated separately with a model including the nearest fuel assemblies and the effect of peripheral water. Then, the second phase evaluates the isotopic compositions of each fuel assemblies at the center of the active height with a 2-D model under conservative core conditions. The T-depl sequence of the TRITON module coupling NEWT to ORIGEN-S is called in this step. Each fuel assembly must be studied separately to consider loading pattern changes occurring at each cycle. An infinite model with reflections on lateral axes is used and the closest neighbors of the fuel assembly are limited to 2 pins - which is around the size of the neutrons mean free path in the core. This is an innovative physical trick aiming at compensating for a limited computing power. Finally, isotopic compositions calculated are combined with the axial burnup profile of the first step to extrapolate the concentrations along the whole active length. Data can then be added in any criticality model, such as a spent fuel pit or any disposal handling fuel assemblies. Criticality analyses of burnt fissile material using burnup credit can be managed within a reasonable amount of time, on condition that sufficient proofs of code qualification for the studied range of parameters are provided, especially on fission products isotopic compositions calculation. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Dynamic phases, stratification, laning, and pattern formation for driven bidisperse disk systems in the presence of quenched disorder

Using numerical simulations, we examine the dynamics of driven two-dimensional bidisperse disks flowing over quenched disorder. The system exhibits a series of distinct dynamical phases as a function of applied driving force and packing fraction, including a phase-separated state as well as a smectic state with liquid-like or polycrystalline features. At low driving forces, we find a clogged phase with an isotropic density distribution, while at intermediate driving forces the disks separate into bands of high and low densities with either liquid-like or polycrystalline structure in the high-density bands. In addition to the density phase separation, we find that in some cases there is a fractionation of the disk species, particularly when the disk size ratio is large. The species phase-separated regimes form a variety of patterns such as large disks separated by chains of smaller disks. Here, our results show that the formation of laning states can be enhanced by tuning the ratio of disk radius of the two species, due to the clumping of small disks in the interstitial regions between the large disks. This system could be experimentally realized using sterically interacting colloidal particles suspended in a viscous fluid driven over random pinning arrays or granular matter suspended in fluid moving over a random landscape.

36 MATERIALS SCIENCE↗

Attribution of observed sea level pressure trends to greenhouse gas, aerosol, and ozone changes

Human influence on atmospheric sea level pressure (SLP) has previously been detected globally, but the contributions of greenhouse gas, aerosol, and ozone changes to the observed trends have not been separately identified. We use simulations from eight climate models to show that greenhouse gas, aerosol, and ozone changes each drive distinct seasonal and geographical patterns of trends, which are separately detectable in observed seasonal SLP trends over the 1951–2011 period. This detection is driven by significant low-latitude SLP responses to greenhouse gas, aerosol, and ozone changes, as well as the more frequently-studied high latitude responses. These results aid in understanding past atmospheric circulation changes, and have potential to improve projections of future circulation changes.

54 ENVIRONMENTAL SCIENCES↗

3D Printing at Los Alamos

At Los Alamos National Laboratory (LANL), their additive manufacturing division is seeking to answer the question whether it is possible to 3D print on a 5th axis. The end goal is to achieve true continuous fiber 3D printing. My goal on this project was to learn about additive manufacturing, and to learn how to operate the experimental 3D printer. Each print that was done demonstrated a different pattern that would change the strength and integrity of the print. Overall prints with minimal strand separation and featured weave-like patterns proved to have the best integrity.

42 ENGINEERING↗

First-order quantum phase transitions: Test ground for emergent chaoticity, regularity and persisting symmetries

We present a comprehensive analysis of the emerging order and chaos and enduring symmetries, accompanying a generic (high-barrier) first-order quantum phase transition (QPT). The interacting boson model Hamiltonian employed, describes a QPT between spherical and deformed shapes, associated with its U(5) and SU(3) dynamical symmetry limits. A classical analysis of the intrinsic dynamics reveals a rich but simply-divided phase space structure with a Hénon–Heiles type of chaotic dynamics ascribed to the spherical minimum and a robustly regular dynamics ascribed to the deformed minimum. The simple pattern of mixed but well-separated dynamics persists in the coexistence region and traces the crossing of the two minima in the Landau potential. A quantum analysis discloses a number of regular low-energy U(5)-like multiplets in the spherical region, and regular SU(3)-like rotational bands extending to high energies and angular momenta, in the deformed region. These two kinds of regular subsets of states retain their identity amidst a complicated environment of other states and both occur in the coexistence region. A symmetry analysis of their wave functions shows that they are associated with partial U(5) dynamical symmetry (PDS) and SU(3) quasi-dynamical symmetry (QDS), respectively. The pattern of mixed but well-separated dynamics and the PDS or QDS characterization of the remaining regularity, appear to be robust throughout the QPT. Effects of kinetic collective rotational terms, which may disrupt this simple pattern, are considered.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Carbon nanotube biconvex microcavities

Developing highly efficient microcavities with predictive narrow-band resonance frequencies using the least amount of material will allow the applications in nonlinear photonic devices. We have developed a microcavity array that comprised multi-walled carbon nanotubes (MWCNT) organized in a biconvex pattern. The finite element model allowed designing microcavity arrays with predictive transmission properties and assessing the effects of the microarray geometry. The microcavity array demonstrated negative index and produced high Q factors. 2–3 μm tall MWCNTs were patterned as biconvex microcavities, which were separated by 10 μm in an array. The microcavity was iridescent and had optical control over the diffracted elliptical patterns with a far-field pattern, whose properties were predicted by the model. It is anticipated that the MWCNT biconvex microcavities will have implications for the development of highly efficient lenses, metamaterial antennas, and photonic circuits.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Effective Electrostatic Interactions Between Two Overall Neutral Surfaces with Quenched Charge Heterogeneity Over Atomic Length Scale

Using Monte Carlo results as a reference, a classical density functional theory (CDFT) is shown to reliably predict the forces between two heterogeneously charged surfaces immersed in an electrolyte solution, whereas the Poisson–Boltzmann (PB) theory is demonstrated to deteriorate obviously for the same system even if the system parameters considered fall within the validity range of the PB theory in the homogeneously charged surfaces. By applying the tested CDFT, we study the effective electrostatic potential of mean force (EPMF) between two face–face planar and hard surfaces of zero net charge on which positive and negative charges are separated and considered to present as discontinuous spots on the inside edges of the two surfaces. Main conclusions are summarized as follows: (i) strength of the EPMF in the surface charge separation case is very sensitively and positively correlated with the surface charge separation level and valency of the salt ion. Particularly, the charge separation level and the salt ion valency have a synergistic effect, which makes high limit of the EPMF strength in the surface charge separation case significantly go beyond that of the ideal homogeneously charged surface counterpart at average surface charge density similar to the average surface positive or negative charge density in the charge separation case. (ii) The surface charge distribution patterns mainly influence sign of the EPMF: symmetrical and asymmetrical patterns induce repulsive and attractive (at small distances) EPMF, respectively; but with low valency salt ions and low charge separation level the opposite may be the case. With simultaneous presence of both higher valency cation and anion, the EPMF can be repulsive at intermediate distances for asymmetrical patterns. (iii) Salt ion size has a significant impact, which makes the EPMF tend to become more and more repulsive with the ion diameter regardless of the surface charge distribution patterns and the valency of the salt ion; whereas if the 1:1 type electrolyte and the symmetrical patterns are considered, then the opposite may be the case. All of these findings can be explained self-consistently from several perspectives: an excess adsorption of the salt ions (induced by the surface charge separation) serving to raise the osmotic pressure between the plates, configuration fine-tuning in the thinner ion adsorption layer driven by the energy decrease principle, direct Coulombic interactions operating between charged objects on the two face-to-face plates involved, and net charge strength in the ion adsorption layer responsible for the net electrostatic repulsion.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

A method for mapping submicron-scale crystallographic order/disorder applied to human tooth enamel

Tooth enamel, the outermost layer of human teeth, is a complex, hierarchically structured biocomposite. The details of this structure are important in multiple human health contexts, from understanding the progression of dental caries (tooth decay) to understanding the process of amelogenesis and related developmental defects. Enamel is composed primarily of long, nanoscale crystallites of hydroxyapatite that are bundled by the thousands to form micron-scale rods. Studies with transmission electron microscopy show the relationships between small groups of crystallites and X-ray diffraction characterize averages over many rods, but the direct measurement of variations in local crystallographic structure across and between enamel rods has been missing. Here, we describe a synchrotron X-ray-based experimental approach and a novel analysis method developed to address this gap in knowledge. A ~500-nm-wide beam of monochromatic X-rays in conjunction with a sample section only 1 μm in thickness enables 2D diffraction patterns to be collected from small well-separated volumes within the enamel microstructure but still probes enough crystallites (~300 per pattern) to extract population-level statistics on crystallographic features like lattice parameter, crystallite size, and orientation distributions. Furthermore, the development of a quantitative metric to characterize relative order and disorder based on the azimuthal autocorrelation of diffracted intensity enables these crystallographic measurements to be correlated with their location within the enamel microstructure (e.g., between rod and interrod regions). These methods represent a step forward in the characterization of human enamel and will elucidate the variation of the crystallographic structure across and between enamel rods for the first time.

crystallographic order/disorder↗

Understanding nanoscale structural distortions in Pb(Zr 0.2 Ti 0.8 )O 3 by utilizing X-ray nanodiffraction and clustering algorithm analysis

Hard X-ray nanodiffraction provides a unique nondestructive technique to quantify local strain and structural inhomogeneities at nanometer length scales. However, sample mosaicity and phase separation can result in a complex diffraction pattern that can make it challenging to quantify nanoscale structural distortions. In this work, a k-means clustering algorithm was utilized to identify local maxima of intensity by partitioning diffraction data in a three-dimensional feature space of detector coordinates and intensity. This technique has been applied to X-ray nanodiffraction measurements of a patterned ferroelectric PbZr 0.2 Ti 0.8 O 3 sample. The analysis reveals the presence of two phases in the sample with different lattice parameters. A highly heterogeneous distribution of lattice parameters with a variation of 0.02 Å was also observed within one ferroelectric domain. This approach provides a nanoscale survey of subtle structural distortions as well as phase separation in ferroelectric domains in a patterned sample.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Scalable Nanoimprint Manufacturing of Functional Multilayer Metasurface Devices

Optical metasurfaces, consisting of subwavelength-scale meta-atom arrays, hold great promise of overcoming the fundamental limitations of conventional optics. Due to their structural complexity, metasurfaces usually require high-resolution yet slow and expensive fabrication processes. Here, using a metasurface polarimetric imaging device as an example, the photonic structures and the Nanoimprint lithography (NIL) processes are designed, creating two separate NIL molds over a patterning area of > 20 mm2 with designed Moiré alignment markers by electron-beam writing, and further subsequently integrate silicon and aluminum metasurface structures on a chip. Uniquely, the silicon and aluminum metasurfaces are fabricated by using the nanolithography and 3D pattern-transfer capabilities of NIL, respectively, achieving nanometer-scale linewidth uniformity, sub-200 nm translational overlay accuracy, and <0.017 rotational alignment error while significantly reducing fabrication complexity and surface roughness. Here, the micro-sized multilayer metasurfaces have high circular polarization extinction ratios as large as ≈20 and ≈80 in blue and red wavelengths. Further, the metasurface chip-integrated CMOS imager demonstrates high accuracy in broad-band, full Stokes parameter analysis in the visible wavelength ranges and single-shot polarimetric imaging. This novel, NIL-based, multilayered nanomanufacturing approach is applicable to the scalable production of large-area functional structures for ultra-compact optic, electronic, and quantum devices.

36 MATERIALS SCIENCE↗

Maize yield under a changing climate: The hidden role of vapor pressure deficit

Temperatures over the next century are expected to rise to levels detrimental to crop growth and yield. As the atmosphere warms without additional water vapor input, vapor pressure deficit (VPD) increases as well. Increased temperatures and accompanied elevated VPD levels can both lead to negative impacts on crop yield. The independent importance of VPD, however, is often neglected or conflated with that from temperature due to a tight correlation between the two climate factors. We used a coupled process-based crop (MAIZSIM) and soil (2DSOIL) model to gain a mechanistic understanding of the independent roles temperature and VPD play in crop yield projections, as well as their interactions with rising CO 2 levels and changing precipitation patterns. We found that by separating out the VPD effect from rising temperatures, VPD increases had a greater negative impact on yield (12.9 ± 1.8%, increase in VPD associated with 2 °C warming) compared to that from warming (8.5 ± 1.4%, the direct effect of 2 °C warming). The negative impact of these two factors varied with precipitation levels and influenced yield through separate mechanisms. Warmer temperatures caused yield loss mainly through shortening the growing season, while elevated VPD increased water loss and triggered several water stress responses such as reduced photosynthetic rates, lowered leaf area development, and shortened growing season length. Elevated CO 2 concentrations partially alleviated yield loss under warming or increased VPD conditions through water savings, but the impact level varied with precipitation levels and was most pronounced under drier conditions. These results demonstrate the key role VPD plays in crop growth and yield, displaying a magnitude of impact comparative to temperature and CO 2 . A mechanistic understanding of the function of VPD and its relation with other climate factors and management practices is critical to improving crop yield projections under a changing climate.

54 ENVIRONMENTAL SCIENCES↗

Designing Anion-Exchange Ionomers with Oriented Nanoscale Phase Separation at a Silver Interface

We report performance of polymer electrolyte-based energy systems is significantly impacted by transport within the electrode catalyst layer, where ionomer thin films coat catalyst particles. Proton exchange ionomer thin films have been thoroughly characterized, but few studies have critically examined anion-exchange ionomer (AEI) thin films. Further, none have reported nanoscale phase separation for hydrocarbon AEIs, which is critical to mitigate transport resistances. In this work, a set of hydrocarbon-based AEIs with nanoscale phase separation are developed from tunable block copolymer systems composed of polyisoprene (PIp) and polychloromethylstyrene (PCMS). The effect of the PIp/PCMS ratio, architecture, and thickness on the thin-film morphology of the neutral block copolymer precursors on silicon and silver substrates is investigated using grazing-incidence small-angle X-ray scattering (GISAXS) and atomic force microscopy (AFM). AEIs are prepared by quaternizing with trimethylamine or methylpiperidine and their cation-dependent morphology is characterized at 60 °C and 95% RH. A perpendicularly aligned morphology is observed on silver, while no phase separation is observed on silicon, indicating that silver-polymer interfacial interactions drive phase separation. After quaternization, dipole-dipole interactions induce some disorder, but nanoscale phase separation is still maintained. GISAXS patterns are modeled using a Unified Fit approach to understand water uptake and swelling, and recommendations for AEI design are presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Prospective life-cycle modeling of a carbon capture and storage system using metal-organic frameworks for CO2 capture

Metal-organic frameworks (MOFs) are promising new material media for carbon dioxide (CO2) capture. Their tunable adsorption patterns may allow relatively efficient separation of gases, e.g. from power plant exhaust. Here we conduct scenario-based prospective life-cycle system modeling to estimate the potentials and implications of large-scale MOF application for post-combustion carbon capture and storage (CCS), and estimate the source and magnitude of uncertainties. The methodological approach includes parametric system modeling to quantify relations between system components; scenario projections of plausible pathways for system scale-up; proxy data on analogous materials and processes; and uncertainty analysis of parameter significance. We estimate the system-wide material and energy flows and economic costs associated with projected large-scale CCS deployment. We compare the performance of a MOF-based system to currently more mature amine-based capture technology. We discuss balancing two critical factors that determine the success of CO2 capture media: thermodynamic efficiency of the capture/regeneration cycle, and life-cycle embodied energy and cost of the material and its ancillary systems.

Sathre, R↗

Higher fullerenes: Compositional analysis by EDXD and molecular dynamics

A carbon soot of higher fullerenes was studied by Energy Dispersive X-ray Diffraction (EDXD) aiming at defining the overall structure as accurately as possible to define the overall structure, without lengthy separation and purification procedures. EDXD pattern was compared with model curves obtained for single homogeneous fullerenes already crystallized and for the hypothesized C180. All fullerenes contribute to the overall experimental curve to different extents, with C96 giving the best agreement. The presence of even higher fullerenes is very likely, since the hypothesized C180 gives a very good match as well.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Multicontrast x-ray computed tomography imaging using Talbot-Lau interferometry without phase stepping

Purpose: The purpose of this work is to demonstrate that multicontrast computed tomography (CT) imaging can be performed using a Talbot-Lau interferometer without phase stepping, thus allowing for an acquisition scheme like that used for standard absorption CT. Methods: Rather than using phase stepping to extract refraction, small-angle scattering (SAS), and absorption signals, the two gratings of a Talbot-Lau interferometer were rotated slightly to generate a moire pattern on the detector. A Fourier analysis of the moire pattern was performed to obtain separate projection images of each of the three contrast signals, all from the same single-shot of x-ray exposure. After the signals were extracted from the detector data for all view angles, image reconstruction was performed to obtain absorption, refraction, and SAS CT images. A physical phantom was scanned to validate the proposed data acquisition method. The results were compared with a phantom scan using the standard phase stepping approach. Results: The reconstruction of each contrast mechanism produced the expected results. Signal levels and contrasts match those obtained using the phase stepping technique. Conclusions: Absorption, refraction, and SAS CT imaging can be achieved using the Talbot-Lau interferometer without the additional overhead of long scan time and phase stepping.

62 RADIOLOGY AND NUCLEAR MEDICINE↗