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At least 37 records · Page 2

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DOE OSTI2022

Diffusion characteristics of water molecules in a lamellar structure formed by triblock copolymers

The distribution and diffusion of water molecules are playing important roles in determining self-assembly and transport properties of polymeric systems. Small-angle neutron scattering (SANS) experiments and molecular dynamics (MD) simulation have been applied to understand the distribution of water molecules and their dynamics in the lamellar membrane formed by Pluronic L62 block copolymers. Penetration of water molecules into the polyethylene oxide (PEO) layers of the membranes has been estimated using scattering length density (SLD) profiles obtained from SANS measurements, which agree well with the molecular distribution observed from MD simulations. The water diffusion coefficient at different regions of the lamellar membrane was further investigated using MD simulation. The diffusion characteristic shows a transition from normal to anomalous diffusion as the position of the water molecule changes from the bulk to PEO and to the polypropylene oxide (PPO) layer. Here we find that water molecules within the PEO or PPO layers follow subdiffusive dynamics, which can be interpreted by the model of fractional Brownian motion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Densified vertically lamellar electrode architectures for compact energy storage

As one of the most compact electrochemical energy storage systems, lithium-ion batteries (LIBs) are playing an indispensable role in the process of vehicle electrification to accelerate the shift to sustainable mobility. Making battery electrodes thicker is a promising strategy for improving the energy density of LIBs which is essential for applications with weight or volume constraints, such as electric-powered transportation; however, their power densities are often significantly restricted due to elongated and tortuous charge traveling distances. Here, we propose an effective methodology that couples bidirectional freeze-casting and compression-induced densification to create densified vertically lamellar electrode architectures for compact energy storage. The vertically lamellar architectures not only overcome the critical thickness limit for conventional electrodes but also facilitate and redistribute the lithium-ion flux enabling both high rate capability and stable cyclability. Furthermore, this proposed methodology is universal as demonstrated in various electrochemical active material systems. This study offers a facile approach that realizes simultaneous high energy and high power in high-loading battery electrodes and provides useful rationales in designing electrode architectures for scalable energy storage systems.

42 ENGINEERING↗

DOE OSTI2024

Lamellar: A Rust-based Asynchronous Tasking and PGAS Runtime for High Performance Computing

Cybersecurity is one of the largest concerns in modern computing, impacting and dictating how governments, private corporations, and individuals interact with and live in an increasingly digital world. The NSA has recently released a memo [ 1] on “Software Memory Safety” where they highlight that both Microsoft and Google have stated around 70% of software vulnerabilities were due to memory safety issues. Although languages such as C and C++ provide freedom and flexibility with memory management, guaran- teeing safety falls mostly on the developer. The NSA recommends using “memory safe” languages whenever possible. In this paper we introduce Lamellar, an asynchronous tasking and PGAS HPC runtime written in Rust, one such "memory safe" language. We describe the entire Lamellar stack, from network interfaces to high- level abstractions such as distributed LamellarArrays and Active Messages. We conclude by showing comparable performance to legacy PGAS runtimes (e.g. OpenSHMEM) on a subset of the BALE kernel suite while maintaining strong memory safety principles.

HPC Software Systems, Rust Programming Language, P↗

NASA NTRS1981

A quantitative study of factors influencing lamellar eutectic morphology during solidification

The factors that influence the shape of the solid-liquid interface of a lamellar binary eutectic alloy are evaluated. Alloys of carbon tetrabromide and hexachloroethane which serve as a transparent analogue of lamellar metallic eutectics are used. The observed interface shapes are analyzed by computer-aided methods. The solid-liquid interfacial free energies of each of the individual phases comprising the eutectic system are measured as a function of composition using a 'grain boundary groove' technique. The solid-liquid interfacial free energy of the two phases are evaluated directly from the eutectic interface. The phase diagram for the system, the heat of fusion as a function of composition, and the density as a function of composition are measured. The shape of the eutectic interface is controlled mainly by the solid-liquid and solid-solid interfacial free energy relationships at the interface and by the temperature gradient present, rather than by interlamellar diffusion in the liquid at the interface, over the range of growth rates studied.

Kaukler, W. F. S.↗

NASA NTRS1985

The role of near-surface plastic deformation in the wear of lamellar solids

It is shown in this paper that the role of surface and near-surface plastic deformation is especially significant in both sliding and abrasive wear of lamellar composites. Lamellar structures were produced artificially from alternate layers of pure copper and pure tin or lead foils. The resulting composites were tested in three different wear tests: single-pass abrasion by a sharp, hard abrader; multiple-pass rubbing by a hard, rounded abrader; and pin-on-disk sliding. In each case the counterface was a hard alloy steel. Tests were run with the composite lamellae in two orientations: perpendicular and parallel to the sliding direction. It was found that the composites had much less wear resistance and greater abradability when oriented perpendicular to the rub direction. The mechanisms for wear particle removal and the role of plastic deformation in the process were studied by plasticity analysis and by microscopic (SEM and optical) observation.

Kennedy, F. E.↗

NASA NTRS1990

Effect of convection on the microstructure of a lamellar eutectic growing with a stepped interface

A two dimensional model developed to study the influence of convective flow on the concentration field ahead of a growing lamellar eutectic is described when one phase projects out into the melt creating a stepped interface. The two dimensional convective flow field, which is periodic in the horizontal direction, was computed numerically using the software FLUENT. The velocity field generated due to the flow of melt over the steps was then incorporated into a finite difference scheme employed to solve the concentration field. The average interfacial composition was calculated and converted to lamellar spacing using the Jackson and Hunt minimum supercooling criterion. It was found that a stepped interface is more sensitive to convection than a planar interface.

Seth, Jayshree↗

NASA NTRS1991

Sintering of two phase lamellar microstructures

The effect of an inert phase on neck growth rates during sintering of lamellar structures is described. Sintering diagrams are constructed for an aggregate of two-phase Cu spheres with lamellar microstructure containing an inert phase. It is shown that the regions corresponding to lattice diffusion domination shrink due to the inert phase presence. As the dispersion becomes finer, the alterations in the map become substantial.

Courtney, T. H.↗

NASA NTRS1991

Effect of convection on the microstructure of a lamellar eutectic growing with a stepped interface

Seth, Jayshree↗

NASA NTRS2001

Lamellar Spacing Selection in Al-Si Eutectic System: a Theoretical Investigation

It is well known that irregular eutectics such as Al-Si and Fe-C exhibit larger lamellar spacings and undercoolings compared to the predictions made by the Jackson and Hunt (JH) theory. In this paper, we reexamine the JH theory and relax some of the assumptions used in that treatment. The modified theoretical model has enhanced capabilities to predict the lamellar spacing in both regular and irregular eutectics. For the Al-Si system in particular we identified two different spacing selection mechanisms:a) for a particular growth rate, a nearly isothermal interface can be achieved at a unique minimum spacing lambda(sub I); b) the average spacing in the microstructure (lambda(sub av) greater than lambda(sub I)) is essentially dictated by the undercooling of the faceted phase. Based on the modified theoretical model a semi-empirical expression has been developed to account for the influence of the temperature gradient. Application of a Mullin and Sekerka type stability analysis for eutectics will also be presented and the results compared to the modified JH model. It will be shown that the both theoretical approaches are in good agreement with each other and also with the published experimental measurements.

Catalina, Adrian V.↗

DOE OSTI2022

Lamellar and Hexagonal Assemblies of PEG-Grafted Silver Nanoparticles: Implications for Plasmonics and Photonics

Assembly of silver nanoparticles (AgNPs) grafted with thiolated poly(ethylene glycol) (PEG-SH) with various molecular weights is reported. Synchrotron-based X-ray surface-sensitive diffraction methods are used to determine the nature of two-dimensional (2D) assemblies at liquid/vapor interfaces, and small-angle X-ray scattering (SAXS) is used to monitor the three-dimensional (3D) assemblies in bulk suspensions. We find that assembly can be induced either by the addition of K 2 CO 3 or polyacrylic acid (PAA) to the PEG-AgNP aqueous suspensions. The addition of K 2 CO 3 induces a 2D hexagonal structure at the liquid/vapor interface and a 3D hexagonal columnar structure in solutions, where the columns consist of tethered PEG-AgNP chains. On the other hand, the addition of PAA leads to the formation of a 2D lamella-like distorted hexagonal sheet at the liquid/vapor interface and a 3D lamellar superstructure formed by stacked 2D sheets in the PEG-AgNP suspension. Effects of the core type of nanoparticles on the assembly can be used to control structures for potential applications in plasmonics and photonics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Bioinspired Macrocyclic Molecule Supported Two‐Dimensional Lamellar Membrane with Robust Interlayer Structure for High‐Efficiency Nanofiltration

Abstract 2D lamellar membranes (2DLMs) are used for efficient desalination and nanofiltration. However, weak interactions between adjacent stacked nanosheets result in susceptibility to swelling that limits practical applicability. Inspired by the super adhesion of multi‐point suction cups on octopus tentacles, a 2DLM is constructed from Ti 3 C 2 T x MXene supported by the macrocyclic “multi‐point” molecule cucurbit[5]uril (CB5) and demonstrated for nanofiltration of methyl blue (MB) and enrichment of uranyl carbonate. Experimental results and density functional theory calculations indicate that CB5 rivets to the surface of the nanoflakes through strong stable interactions between its multiple binding sites and surface hydroxyl functional groups on MXene nanosheets. This novel 2DLM exhibits excellent nanofiltration performance (69 L m −2 h −1 bar −1 permeance with 93.6% rejection for MB) and can be recycled at least 30 times without significant degradation. The 2DLM exhibits excellent swelling resistance at high salinity, with a demonstration of selective enrichment of uranyl carbonate from artificial water and natural seawater. The results provide a new strategy for constructing highly stable 2DLMs with interlayer spacing controllable from sub‐nano to nanometer scales, for size‐selective sieving of molecules and ions, high‐efficiency nanofiltration, and other applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2024

Dynamics of High Molecular Weight Cylindrical and Lamellar Block Copolymers with X‐ray Photon Correlation Spectroscopy

Here, the structure and dynamics of polystyrene (PS)-b-poly(ethylene oxide) block copolymers (BCPs) are studied. The BCPs exhibit microphase-separated cylindrical and lamellar morphologies. Structural dynamics are measured with X-ray photon correlation spectroscopy in the small-angle regime. Morphologies and domain sizes are evaluated using small-angle X-ray scattering (SAXS), scanning electron microscopy, and atomic force microscopy. Different solvent processing conditions are investigated. Grain sizes evaluated using SAXS are found to depend on processing only for the rubbery majority BCP. The structural relaxation times are examined as a function of PS volume fraction, temperature, morphology, and structural sizes. Well above the glass transition temperature (T g ) of PS, all samples exhibit stretched autocorrelation decays and diffusive dynamics. Near T g of PS, the dynamics of all samples are anomalous with compressed autocorrelation decays and hyperdiffusive dynamics. This transition occurs at 153 °C or 1.13 T g of PS. In the diffusive regime (at high temperature), structural relaxation times are dependent on the processing method. Near PS T g (at low temperature), structural relaxation times scale with the PS volume fraction. Structural relaxation times do not correlate with grain size, indicating that the out-of-equilibrium state of PS dominates the structural dynamics of these strongly phase-segregated BCPs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Soft-Shear-Aligned Vertically Oriented Lamellar Block Copolymers for Template-Free Sub-10 nm Patterning and Hybrid Nanostructures

The template-free unidirectional alignment of lamellar block copolymers (l-BCPs) for sub-10 nm high-resolution patterning and hybrid multicomponent nanostructures is important for technological applications. Here we demonstrate a modified soft-shear directed self-assembly (SDSA) approach for aligning pristine l-BCPs and l-BCPs with incorporated polymer grafted nanoparticles (PGNPs), as well as the l-BCPs conversion to aligned gold nanowires, and hybrid of metallic gold nanowire and dielectric silica nanoparticle in the form of line-dot nanostructures. The smallest patterns have a half-pitch as small as 9.8 nm. In all cases, soft-shear is achieved using a high molecular mass polymer topcoat layer, with support on a neutral bottom layer. We also show that the hybrid line-dot nanostructures have a red-shifted plasmonic response in comparison to the neat gold nanowires. These template-free aligned BCPs and nanowires have potential use in nanopatterning applications and the line-dot nanostructures should be useful in the plasmonic sensing of biomolecules and other molecular species based on the plasmonic response of the nanowires.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Pressure-Induced Multidimensional Assembly and Sintering of CuInS 2 Nanoparticles into Lamellar Nanosheets with Band Gap Narrowing

Two-dimensional (2D) nanomaterials have fascinating structural, electrical, and optical properties, especially strong excitonic effects due to decreased dielectric screening. However, constructing 2D ultrathin nanomaterials, with the exception of layered materials, remains a challenge. In this work, we successfully realize oriented attachment on guiding one-dimensional chalcopyrite CuInS 2 nanocrystal (NC) formation and 2D assembly into lamellar nanosheets by applying pressure-driven sintering of zero-dimensional CuInS2 nanoparticles (NPs). We discuss the atomic-level mechanism of such phenomena and illustrate a pressure-driven processing diagram that reveals the sintering process of NPs coordinated by pressure and structural transformation. Optical measurements exhibit that the band gap has a narrowing by 0.21 eV compared with the initial 2.03 eV upon decompression to ambient conditions. Our findings represent a significant step forward in gaining an in-depth understanding of the pressure-driven morphology engineering of nanomaterials and provide a promising strategy to prepare 2D NCs, thereby greatly increasing the choice of materials for various applications.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Effect of Molecular Weight and Layer Thickness on Dielectric Breakdown Strength of Neat and Homopolymer Swollen Lamellar Block Copolymer Films

Designing next-generation lightweight pulsed power devices hinges on understanding the factors influencing the energy storage performance of dielectric materials. Polymer dielectric films have a quadratic dependence of energy storage on the voltage breakdown strength and strategies to enhance the breakdown strength are expected to yield a path toward high energy storage densities. Highly stratified lamellar block copolymer (L-BCP) films of model polystyrene-b-polymethylmethacrylate (PS-b-PMMA) exhibited as much as ~50% enhancement in breakdown voltage (E BD ), (225 % increase in stored energy density, U~ E BD 2 ), compared to unordered as-cast L-BCP films. Such an energy density using amorphous polymer is on par with industry-standard semi-crystalline biaxially oriented polypropylene (BOPP), and as such a notable development in the field. This work develops a deeper understanding of the molecular mechanisms of E BD enhancement in L-BCP films, due to combination of interface formation and spatial isolation of the chain ends into segregated zones. We further confirm the role of chain ends in the breakdown process blending a low M n L-BCP with matched M n homopolymers to attain same layer spacing as neat L-BCP of higher M n . E BD shows a significant decrease at low homopolymer fractions due to increased net chain end density within swollen ordered L-BCP domains in wet-brush regime, followed by increased E BD due to layer thickness increase via segregated “interphase layer” formation by excess homopolymers. Notably, E BD of homopolymer swollen L-BCPs is always lower than neat L-BCP of the same domain spacing, due to overall adverse chain ends contribution from homopolymers. These findings provide important selection rules for L-BCPs for designing next-generation flexible electronics with high energy density solid-state BCP film capacitors.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Phase Heterogeneity in Cholesterol-Containing Ternary Phospholipid Lamellar Phases

Pseudo-ternary mixtures of lamellar phase phospholipids (DPPC and brain sphingomyelin with cholesterol) were studied below T m while comparing the influence of cholesterol content, temperature, and the presence of small quantities of vitamin D binding protein (DBP) or vitamin D receptor (VDR). The measurements, conducted by X-ray diffraction (XRD) and nuclear magnetic resonance (NMR), cover a range of cholesterol concentrations (20% mol. wt to 40% mol. wt.) and physiologically relevant temperature range (294–314 K). In addition to rich intraphase behavior, data and modeling are used to approximate the lipids’ headgroup location variations under the abovementioned experimental conditions.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Strong, ductile, and hierarchical hetero-lamellar-structured alloys through microstructural inheritance and refinement

The strength−ductility trade-off exists ubiquitously, especially in brittle intermetallic-containing multiple principal element alloys (MPEAs), where the intermetallic phases often induce premature failure leading to severe ductility reduction. Hierarchical heterogeneities represent a promising microstructural solution to achieve simultaneous strength−ductility enhancement. However, it remains fundamentally challenging to tailor hierarchical heterostructures using conventional methods, which often rely on costly and time-consuming processing. Here, we report a multiscale microstructural inheritance and refinement strategy to process “structural hierarchy precursors” in as-cast heterogeneous Al 0.7 CoCrFeNi MPEAs, which lead directly to a hierarchical hetero-lamellar structure (HLS) after simple rolling and annealing. Interestingly, it takes only 10 min of annealing time, two orders of magnitude less than that required to render the state-of-the-art properties during conventional processing of Al 0.7 CoCrFeNi, for us to achieve record-high strength−ductility combinations via the hierarchical HLS design that sequentially stimulates multiple unusual deformation and reinforcement mechanisms. In particular, the HLS-enabled high hetero-deformation-induced (HDI) internal stress triggers profuse <111>-type dislocations on over five independent slip systems in the supposedly brittle intermetallic phase and activates extensive stacking faults (SFs) and nanotwinning in the adjoining soft phase with a rather high SF energy. These unexpected, dynamically reinforcing hetero-deformation mechanisms across multiple length scales facilitate high sustained HDI strain hardening, along with a salient microcrack-mediated extrinsic ductilization effect, suggesting that the proposed microstructural inheritance and refinement strategy provides an efficient, fast, and low-cost approach to overcome the strength−ductility trade-off in a broad range of structural materials.

Science & Technology - Other Topics↗

DOE OSTI2025

Fabrication and characterization of a full-size ultra-precise lamellar grating for the Cosmic beamline at ALS-U

We have developed a new process for the production of ultra-precise variable line spacing (VLS) lamellar diffraction gratings through nanofabrication. The process enables the fabrication of full-size X-ray gratings with sub-nanometre accuracy in groove depth, an optimal land-to-groove ratio, and uniform groove depth across the entire grating area. We also established a method for evaluating VLS groove density variation using stitched Fizeau interferometry. The measurements confirmed the exceptionally high accuracy of the VLS groove density in the fabricated gratings, which is well within the specification tolerances while the residual groove density errors are vanishingly small. The gold-coated grating demonstrated near-theoretical diffraction efficiency across the energy range of 100–1200 eV.

36 MATERIALS SCIENCE↗