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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

One-dimensional Hubbard-Holstein model with finite-range electron-phonon coupling

The Hubbard-Holstein model describes fermions on a discrete lattice, with on-site repulsion between fermions and a coupling to phonons that are localized on sites. Generally, at half-filling, increasing the coupling g to the phonons drives the system towards a Peierls charge density wave state, whereas increasing the electron-electron interaction U drives the fermions into a Mott antiferromagnet. At low g and U, or when doped, the system is metallic. In one dimension, using quantum Monte Carlo simulations, we study the case where fermions have a long-range coupling to phonons, with characteristic range ξ, interpolating between the Holstein and Fröhlich limits. Without electron-electron interaction, the fermions adopt a Peierls state when the coupling to the phonons is strong enough. This state is destabilized by a small coupling range ξ and leads to a collapse of the fermions, and, consequently, phase separation. Increasing interaction U will drive any of these three phases (metallic, Peierls, phase separation) into a Mott insulator phase. Furthermore, the phase separation region is once again present in the U ≠ 0 case, even for small values of the coupling range.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Anomalous nanoclusters, anisotropy, and electronic nematicity in the doped manganite L a 1 / 3 C a 2 / 3 Mn O 3

In doped manganites, a superlattice (SL) modulation associated with charge/orbital ordering is accepted as a key component in understanding many intriguing properties. It has been reported that the SL modulation always appears on the a axis of the crystals. Here in this study, by using multiple transmission electron microscopic techniques, we observe a type of anomalous nanocluster in which the SL modulation appears on the c axis of La 1/3 Ca 2/3 MnO 3 . By correlating the thermal evolution of the anomalous nanoclusters to other property measurements, we suggest that strain is responsible for the formation of the anomalous nanoclusters. The phase separation and phase transition scenario in La 1/3 Ca 2/3 MnO 3 are also described using electronic-liquid-crystal (ELC) phases. Lastly, an ELC phase diagram in La 1/3 Ca 2/3 MnO 3 is constructed as a function of temperature based on our observations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Nitroplasticizer-water phase diagram

Nitroplasticizer (NP) is used in conjunction with poly(ester urethane) block co-polymer as binder material for polymer bonded explosives (PBX). Water content contributes directly to the stability of NP, poly(ester urethane), and ultimately the PBX. Therefore a n NP-water miscibility phase diagram can be an important tool in understanding potential water content in NP and further PBX processes. To determine the NP-water miscibility phase diagram, a systematic series of experiments was conducted. NP samples were saturated with water and ramped through incremental temperature steps. Aliquots were taken at each step after equilibration. Water content in NP was determined by Coulmetric Karl Fischer (KF) titration at each incremental temperature step. The sample aliquots were then analyzed by Thermogravimetric analysis (TGA), Differential Scanning Calorimetry (DSC), and Transmission Fourier Transform Infrared Spectroscopy (Near-IR). The resultant data were analyzed and combined to construct a n NP-water phase diagram. The phase diagram, ranging from 500 ppm to 5800 ppm water concentration and –90°C to 130°C, contains six distinct phases separated by five distinct phase separations.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Thermodynamics of Deuterium Oxide Separations in Aqueous Two-Phase Systems

The thermodynamic behavior of aqueousorgame- toluene ternary systems where aqueous components are water (H 2 O) and deuterium oxide (D 2 O) and organic components are acetonitrile (MeCN), tetrahydrofuran (THF), and 1,4-dioxane (DIOX) have been recorded. Preliminary data has been taken for each ternary system to establish the concentration along the spinodal line where Gibbs energy is minimized. In pursuit of this goal, simple laboratory techniques using common equipment was used to benchmark thermodynamic measurements against values reported in the literature. The impact of deuterium on aqueous two-phase separations was determined for each combination of solvents.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Dynamic phases, clustering, and chain formation for driven disk systems in the presence of quenched disorder

In this paper, we numerically examine the dynamic phases and pattern formation of two-dimensional monodisperse repulsive disks driven over random quenched disorder. We show that there is a series of distinct dynamic regimes as a function of increasing drive, including a clogged or pile-up phase near depinning, a homogeneous disordered flow state, and a dynamically phase separated regime consisting of high-density crystalline regions surrounded by a low density of disordered disks. At the highest drives the disks arrange into one-dimensional moving chains. The phase separated regime has parallels with the phase separation observed in active matter systems, but arises from a distinct mechanism consisting of the combination of nonequilibrium fluctuations with density-dependent mobility. We discuss the pronounced differences between this system and previous studies of driven particles with longer-range repulsive interactions moving over random substrates, such as superconducting vortices or electron crystals, where dynamical phase separation and distinct one-dimensional moving chains are not observed. Finally, our results should be generic to a broad class of systems in which the particle-particle interactions are short ranged, such as sterically interacting colloids or Yukawa particles with strong screening driven over random pinning arrays, superconducting vortices in the limit of small penetration depths, or quasi-two-dimensional granular matter flowing over rough landscapes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Perspective: The Asakura Oosawa model: A colloid prototype for bulk and interfacial phase behavior

In many colloidal suspensions, the micrometer-sized particles behave like hard spheres, but when non-adsorbing polymers are added to the solution a depletion attraction (of entropic origin) is created. Since 60 years the Asakura-Oosawa model, which simply describes the polymers as ideal soft spheres, is an archetypical description for the statistical thermodynamics of such systems, accounting for many features of real colloid-polymer mixtures very well. While the fugacity of the polymers (which controls their concentration in the solution) plays a role like inverse temperature, the size ratio of polymer versus colloid radii acts as a control parameter to modify the phase diagram: when this ratio is large enough, a vapor-liquid like phase separation occurs at low enough colloid packing fractions, up to a triple point where a liquid-solid two-phase coexistence region takes over. For smaller size ratios, the critical point of the phase separation and the triple point merge, resulting in a single two-phase coexistence region between fluid and crystalline phases (of “inverted swan neck”-topology, with possibly a hidden metastable phase separation). Furthermore, liquid-crystalline ordering may be found if colloidal particles of non-spherical shape (e.g., rod like) are considered. Also interactions of the particles with solid surfaces should be tunable (e.g., walls coated by polymer brushes), and interfacial phenomena are particularly interesting experimentally, since fluctuations can be studied in the microscope on all length scales, down to the particle level. Due to its simplicity this model has become a workhorse for both analytical theory and computer simulation. Recently, generalizations addressing dynamic phenomena (phase separation, crystal nucleation, etc.) have become the focus of studies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Nonlinear transport, dynamic ordering, and clustering for driven skyrmions on random pinning

Using numerical simulations, we examine the nonlinear dynamics of skyrmions driven over random pinning. For weak pinning, the skyrmions depin elastically, retaining sixfold ordering; however, at the onset of motion there is a dip in the magnitude of the structure factor peaks due to a decrease in positional ordering, indicating that the depinning transition can be detected using the structure factor even within the elastic depinning regime. At higher drives, the moving skyrmion lattice regains full ordering. For increasing pinning strength, we find a transition from elastic to plastic depinning that is accompanied by a sharp increase in the depinning threshold due to the proliferation of topological defects, similar to the peak effect found at the elastic to plastic depinning transition in superconducting vortex systems. For strong pinning and strong Magnus force, the skyrmions in the moving phase can form a strongly clustered or phase-separated state with highly modulated skyrmion density, similar to that recently observed in continuum-based simulations for strong disorder. As the Magnus force is decreased, the density phase-separated state crosses over to a dynamically phase-separated state with uniform density but with flow localized in bands of motion, while in the strongly damped limit, both types of phase-separated states are lost. In the strong pinning limit, we find highly nonlinear velocity-force curves in the transverse and longitudinal directions, along with distinct regions of negative differential conductivity in the plastic flow regime. The negative differential conductivity is absent in the overdamped limit. In conclusion, the Magnus force is responsible for both the negative differential conductivity and the clustering effects since it causes faster moving skyrmions to partially rotate around slower moving or pinned skyrmions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Surface-Engineered Inorganic Nanoporous Membranes for Vapor and Pervaporative Separations of Water–Ethanol Mixtures

Surface wettability-tailored porous ceramic/metallic membranes (in the tubular and planar disc form) were prepared and studied for both vapor-phase separation and liquid pervaporative separations of water-ethanol mixtures. Superhydrophobic nanoceramic membranes demonstrated more selective permeation of ethanol (relative to water) by cross-flow pervaporation of liquid ethanol–water mixture (10 wt % ethanol feed at 80 °C). In addition, both superhydrophilic and superhydrophobic membranes were tested for the vapor-phase separations of water–ethanol mixtures. Porous inorganic membranes having relatively large nanopores (up to 8-nm) demonstrated good separation selectivity with higher permeation flux through a non-molecular-sieving mechanism. Due to surface-enhanced separation selectivity, larger nanopore-sized membranes (~5–100 nm) can be employed for both pervaporation and vapor phase separations to obtain higher selectivity (e.g., permselectivity for ethanol of 13.9 during pervaporation and a vapor phase separation factor of 1.6), with higher flux due to larger nanopores than the traditional size-exclusion membranes (e.g., inorganic zeolite-based membranes having sub-nanometer pores). The prepared superhydrophobic porous inorganic membranes in this work showed good thermal stability (i.e., the large contact angle remains the same after 300 °C for 4 h) and chemical stability to ethanol, while the silica-textured superhydrophilic surfaced membranes can tolerate even higher temperatures. These surface-engineered metallic/ceramic nanoporous membranes should have better high-temperature tolerance for hot vapor processing than those reported for polymeric membranes.

09 BIOMASS FUELS↗
DOE OSTI2016

Local structure, composition, and crystallization mechanism of a model two-phase “composite nanoglass”

We report a detailed study of the local composition and structure of a model, bi-phasic nanoglass with nominal stoichiometry Cu{sub 55}Nb{sub 45}. Three dimensional atom probe data suggest a nanoscale-phase-separated glassy structure having well defined Cu-rich and Nb-rich regions with a characteristic length scale of ≈3 nm. However, extended x-ray absorption fine structure analysis indicates subtle differences in the local environments of Cu and Nb. While the Cu atoms displayed a strong tendency to cluster and negligible structural order beyond the first coordination shell, the Nb atoms had a larger fraction of unlike neighbors (higher chemical order) and a distinctly better-ordered structural environment (higher topological order). This provides the first experimental indication that metallic glass formation may occur due to frustration arising from the competition between chemical ordering and clustering. These observations are complemented by classical as well as ab initio molecular dynamics simulations. Our study indicates that these nanoscale phase-separated glasses are quite distinct from the single phase nanoglasses (studied by Gleiter and others) in the following three respects: (i) they contain at least two structurally and compositionally distinct, nanodispersed, glassy phases, (ii) these phases are separated by comparatively sharp inter-phase boundaries, and (iii) thermally induced crystallization occurs via a complex, multi-step mechanism. Such materials, therefore, appear to constitute a new class of disordered systems that may be called a composite nanoglass.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Use of Nucleating Agent NA11 in the Preparation of Polyvinylidene Fluoride Dual-Layer Hollow Fiber Membranes

Polyvinylidene fluoride (PVDF) dual-layer hollow fiber membranes were simultaneously fabricated by thermally induced phase separation (TIPS) and non-solvent induced phase separation (NIPS) methods using a triple orifice spinneret (TOS) for water treatment application. The support layer was prepared from a TIPS dope solution, which was composed of PVDF, gamma-butyrolactone (GBL), and N-methyl-2-pyrrolidone (NMP). The coating layer was prepared from a NIPS dope solution, which was composed of PVDF, N,N-dimethylacetamide (DMAc), and polyvinylpyrrolidone (PVP). In order to improve the mechanical strength of the dual-layer hollow fiber, a nucleating agent, sodium 2,2'-methylene bis-(4,6-di-tert-butylphenyl) phosphate (NA11), was added to the TIPS dope solution. The performance of the membrane was evaluated by surface and cross-sectional morphology, water flux, mechanical strength, and thermal property. Our results demonstrate that NA11 improved the mechanical strength of the PVDF dual-layer hollow fiber membranes by up to 42%. In addition, the thickness of the coating layer affected the porosity of the membrane and mechanical performance to have high durability in enduring harsh processing conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Influence of Annealing and Composition on the Crystal Structure of Mixed-Halide, Ruddlesden–Popper Perovskites

Mixed-halide two-dimensional (2D) hybrid organic–inorganic perovskites offer an important opportunity to control the band gap for applications in optoelectronic devices. In this study, we focus on phenethylammonium lead halide [(PEA) 2 Pb(I 1– x Br x ) 4 ] films, the pure iodide form of which is one of the most widely studied optically active 2D perovskite systems. Resonant infrared, matrix-assisted pulsed laser evaporation is used to grow films to explore the effects of post-growth annealing and mixed-halide composition. The composition, crystal structure, and optical properties are studied for as-grown and annealed films of (PEA) 2 Pb(I 1– x Br x ) 4 for x = 0, 0.25, 0.5, 0.75, and 1. First-principles calculations are used in conjunction with the experimental data to explain the mixed-halide behavior that does not trend monotonically with the bromide content. Important results of this work are as follows: (i) X-ray diffraction reveals evidence for halide phase separation around x = 0.25, consistent with first-principles calculations, whereas no phase separation is observed for x = 0.5 and above and (ii) a unique photoluminescence (PL) peak splitting is observed for x = 0.75, a composition for which no compositional phase separation is observed. The PL splitting is tentatively explained by the coexistence of two distinct types of halide short-range ordering at x = 0.75. Overall, this study demonstrates that mixed-halide n = 1 Ruddlesden–Popper perovskites are not simple random alloys but that instead, they display distinct sites and ordering preferences of the different halide anions. These preferences are critical to understand and rationally tune the properties of the materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Polyubiquitin ligand-induced phase transitions are optimized by spacing between ubiquitin units

Biomolecular condensates form via multivalent interactions among key macromolecules and are regulated through ligand binding and/or posttranslational modifications. One such modification is ubiquitination, the covalent addition of ubiquitin (Ub) or polyubiquitin chains to target macromolecules. Specific interactions between polyubiquitin chains and partner proteins, including hHR23B, NEMO, and UBQLN2, regulate condensate assembly or disassembly. Here, we used a library of designed polyubiquitin hubs and UBQLN2 as model systems for determining the driving forces of ligand-mediated phase transitions. Perturbations to either the UBQLN2-binding surface of Ub or the spacing between Ub units reduce the ability of hubs to modulate UBQLN2 phase behavior. By developing an analytical model based on polyphasic linkage principles that accurately described the effects of different hubs on UBQLN2 phase separation, we determined that introduction of Ub to UBQLN2 condensates incurs a significant inclusion energetic penalty. This penalty antagonizes the ability of polyUb hubs to scaffold multiple UBQLN2 molecules and cooperatively amplify phase separation. The extent to which polyubiquitin hubs promote UBQLN2 phase separation is encoded in the spacings between Ub units. This spacing is modulated by chains of different linkages and designed chains of different architectures, thus illustrating how the ubiquitin code regulates functionality via the emergent properties of the condensate. The spacing in naturally occurring linear polyubiquitin chains is already optimized to promote phase separation with UBQLN2. We expect our findings to extend to other condensates, emphasizing the importance of ligand properties, including concentration, valency, affinity, and spacing between binding sites in studies and designs of condensates.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2018

Triptycene as a Supramolecular Additive in PTB7:PCBM Blends and Its Influence on Photovoltaic Properties

Additives play an important role in modifying the morphology and phase separation of donor and acceptor molecules in bulk heterojunction (BHJ) solar cells. In this paper, we report triptycene (TPC) as a small-molecule additive for supramolecular control of phase separation and concomitant improvement of the power conversion efficiency (PCE) of PTB7 donor and fullerene acceptor-based BHJ polymer solar cells. An overall 60% improvement in PCE is observed for both PTB7:PC 61 BM and PTB7:PC 71 BM blends. The improved photovoltaic (PV) performance can be attributed to three factors: (a) TPC-induced supramolecular interactions with donor:acceptor components in the blends to realize a nanoscale phase-separated morphology; (b) an increase in the charge transfer state energy that lowers the driving force for electron transfer from donor to acceptor molecules; and (c) an increase in the charge carrier mobility. An improvement in efficiency using TPC as a supramolecular additive has also been demonstrated for other BHJ blends such as PBDB-T:PC 71 BM and P3HT:PCBM, implying the wide applicability of this new additive molecule. A comparison of the photostability of TPC as an additive for PTB7:PCBM solar cells to that of the widely used 1,8-diiodooctane additive shows ~30% higher retention of PV performance for the TPC-added solar cells after 34 h of AM 1.5G illumination. Finally, the results obtained suggest that the approach of using additives that can promote supramolecular interactions to modify the length scale of phase separation between donor and acceptor is very promising and can lead to the development of highly efficient and stable organic photovoltaics.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Regional-Scale Modeling Parameterizations for Secondary Organic Aerosol Formation from Isoprene Epoxydiols: Experimentally Based Evaluation and Optimization

Isoprene is an abundant volatile organic compound emitted from broadleaf forests. Under low nitric oxide concentrations, isoprene is photochemically oxidized to form gas-phase isoprene epoxydiols (IEPOX). In the presence of acidified sulfate aerosols, IEPOX enhances the secondary organic aerosol (SOA) formation. Predictions of IEPOX-SOA in regional-scale models, e.g., the Community Multiscale Air Quality Model (CMAQ), are uncertain due to homogeneous aerosol assumptions, underpredictions of water uptake (hygroscopicity), and aerosol surface area. Here, we used experimental measurements of IEPOX-SOA tracers, 2-methyltetrols (2-MT) and 2-methyltetrol sulfates (2-MTS), formed at initial IEPOX-to-inorganic sulfate ratios ranging from 1–10.5, at ∼50% relative humidity to constrain key IEPOX-SOA parameters: phase separation, organic shell diffusivity (D org ), acidity, hygroscopic growth, mass accommodation, and kinetics. The base CMAQ parametrization overpredicted experimental IEPOX-SOA with an average normalized mean bias (NMB average ) of 1.63. CMAQ with phase separation underpredicted IEPOX-SOA (NMB average = −0.71). Using the phase-separated model, CMAQ model performance was optimized (NMB average = 0.077) with an increased D org = 2 × 10 –16 m 2 s –1 and increased rate constants (k 2-MT = 1 × 10 –3 M 2 s –1 , k 2-MTS = 8.83 × 10 –3 M 2 s –1 ). The optimized model explicitly accounted for hygroscopic growth by utilizing experimentally derived growth rates, improving aerosol surface area predictions. Our model highlights the importance of the aerosol mixing state (homogeneous versus phase-separated), aerosol size dynamics, and hygroscopic growth in modeling heterogeneous reactive uptake of IEPOX.

aerosols↗
DOE OSTI2021

Controlling Polymer Morphology in Blade-Coated All-Polymer Solar Cells

In this report translating all-polymer solar cells from spin-coating to scalable roll-to-roll-compatible fabrication techniques is a critical step toward the application of organic photovoltaics at a scale. Techniques to control polymer crystallization and phase separation during solution printing are essential to obtain high-performance printed organic solar cells. Here, we demonstrate a novel solvent additive approach employing trace amounts of phthalates as additives to control polymer crystallinity and suppress unfavorable phase separation in a representative PTB7-Th/P(NDI2OD-2T) all-polymer solar cell. The best-performing additive increased the blade-coated device performance from 2.09 to 4.50% power conversion efficiency, an over twofold improvement, mitigating the loss in performance that is typically observed during process transfer from spin-coating to blade-coating. It is suggested that the improved device performance stems from a finer polymer phase-separation size and overall improved active layer morphology, evidenced by device characterization data and indirectly supported by grazing incidence wide-angle X-ray scattering analyses. Real-time X-ray diffraction measurements during blade-coating provide mechanistic insights and suggest that the dioctyl phthalate additive may act as a compatibilizer, reducing the demixing of the donor and acceptor polymer during film formation, enabling a smaller phase separation and improved performance. The structural diversity of the class of phthalate additives makes this simple yet effective concept promising for translating other all-polymer material systems to blade-coating and other scalable printing techniques.

14 SOLAR ENERGY↗
DOE OSTI2021

Tau and Membranes: Interactions That Promote Folding and Condensation

Tau misfolding and assembly is linked to a number of neurodegenerative diseases collectively described as tauopathies, including Alzheimer’s disease (AD) and Parkinson’s disease. Anionic cellular membranes, such as the cytosolic leaflet of the plasma membrane, are sites that concentrate and neutralize tau, primarily due to electrostatic interactions with tau’s microtubule binding repeat domain (RD). In addition to electrostatic interactions with lipids, tau also has interactions with membrane proteins, which are important for tau’s cellular functions. Tau also interacts with lipid tails to facilitate direct translocation across the membrane and can form stable protein-lipid complexes involved in cell-to-cell transport. Concentrated tau monomers at the membrane surface can form reversible condensates, change secondary structures, and induce oligomers, which may eventually undergo irreversible crosslinking and fibril formation. These β-sheet rich tau structures are capable of disrupting membrane organization and are toxic in cell-based assays. Given the evidence for relevant membrane-based tau assembly, we review the emerging hypothesis that polyanionic membranes may serve as a site for phase-separated tau condensation. Membrane-mediated phase separation may have important implications for regulating tau folding/misfolding, and may be a powerful mechanism to spatially direct tau for native membrane-mediated functions.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS1984

Space shuttle experiments on Al-In liquid phase miscibility gap (LPMG) alloys

Massive phase separation observed at low-g was studied during the phase separation process while cooling through the miscibility gap under a controlled thermal gradient was investigated. The molten drops which form during the phase separation process appear to move in a direction opposite to that predicted by the theory of thermocapillary droplet motion. A second experiment utilized a plunger arrangement designed to eliminate the surface tension driven convection currents originating at a free surface. This experiment suggests that the free surface does contribute to the coalescence process but that there are other mechanisms which are more important.

Gelles, S. H.↗
DOE OSTI2023

Magnetoresistance anomaly during the electrical triggering of a metal-insulator transition

Phase separation naturally occurs in a variety of magnetic materials and it often has a major impact on both electric and magnetotransport properties. In resistive switching systems, phase separation can be created on demand by inducing local switching, which provides an opportunity to tune the electronic and magnetic state of the device by applying voltage. Here we explore the magnetotransport properties in the ferromagnetic oxide La 0.7 ⁢Sr 0.3 ⁢MnO 3 (LSMO) during the electrical triggering of an intrinsic metal-insulator transition (MIT), which produces volatile resistive switching. This switching occurs in a characteristic spatial pattern, i.e., the formation of a high-resistance barrier perpendicular to the current flow, enabling an electrically actuated ferromagnetic-paramagnetic-ferromagnetic phase separation. At the threshold voltage of the MIT triggering, both anisotropic and colossal magnetoresistances exhibit anomalies including a large increase in magnitude and a sign flip. Computational analysis revealed that these anomalies originate from the coupling between the switching-induced phase separation state and the intrinsic magnetoresistance of LSMO. Furthermore, this work demonstrates that driving the MIT material into an out-of-equilibrium resistive switching state provides the means for electrical control of the magnetotransport phenomena.

Complex oxides↗