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At least 973 records · Page 54

All sources NASA NTRS DOE OSTI

DOE OSTI2014

Determination of reactive oxygen species from ZnO micro-nano structures with shape-dependent photocatalytic activity

Graphical abstract: ZnO micro/nano structures with shape dependent photocatalytic activity were prepared by hydrothermal reaction. The generations of hydroxyl radical, superoxide and singlet oxygen from irradiated ZnO were identified precisely by electron spin resonance spectroscopy. The type of reactive oxygen species was determined by band gap structure of ZnO. - Highlights: • ZnO micro/nano structures with different morphologies were prepared by solvothermal reaction. • Multi-pod like ZnO structures exhibited superior photocatalytic activity. • The generations of hydroxyl radical, superoxide and singlet oxygen from irradiated ZnO were characterized precisely by electron spin resonance spectroscopy. • The type of reactive oxygen species was determined by band gap structure of ZnO. - Abstract: ZnO micro/nano structures with different morphologies have been prepared by the changing solvents used during their synthesis by solvothermal reaction. Three typical shapes of ZnO structures including hexagonal, bell bottom like and multi-pod formed and were characterized by scanning electron microscopy and X-ray diffraction. Multi pod like ZnO structures exhibited the highest photocatalytic activity toward degradation of methyl orange. Using electron spin resonance spectroscopy coupled with spin trapping techniques, we demonstrate an effective way to identify precisely the generation of hydroxyl radicals, superoxide and singlet oxygen from the irradiated ZnO multi pod structures. The type of reactive oxygen species formed was predictable from the band gap structure of ZnO. These results indicate that the shape of micro-nano structures significantly affects the photocatalytic activity of ZnO, and demonstrate the value of electron spin resonance spectroscopy for characterizing the type of reactive oxygen species formed during photoexcitation of semiconductors.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Controlled preparation and structure characterization of BiFeO{sub 3} with macroscopic shapes

Graphical abstract: We firstly explored two facile and successful techniques for BiFeO{sub 3} immobilization on silica fiber, namely, a combined impregnation method with carbon nanofibers (CNFs) templates route, and a combined solvothermal method with CNFs templates route. It is expected that such materials with direct macroscopic shapes would hold promise as highly functionalized materials for potential practical applications, especially in photocatalysis. - Highlights: • BiFeO{sub 3} with macroscopic shape was successfully obtained. • The synthetic methods used here are facile, effective, and reproducible. • Phase composition was strongly affected by calcination temperatures. • The obtained materials are promising visible-light-driven photocatalysts. - Abstract: BiFeO{sub 3} was successfully immobilized on silica fiber via two synthetic techniques (a combined impregnation method with carbon nanofibers templates route; a combined solvothermal method with carbon nanofibers templates route). The phase structure, morphology and optical absorption property of the samples were characterized by X-ray diffraction, field emission scanning electron microscopy, and ultraviolet–visible diffuse reflectance spectroscopy. The results confirmed that carbon nanofibers can act as effective templates for BiFeO{sub 3} immobilization on silica fiber with the applied two methods. Compared with solvent thermal method, impregnation method tends to form a relatively uniform particle size distribution and highly-crystallized phase when the calcination temperature was kept at 773 K for 5 h. It turned out the phase composition of the samples is strongly affected by the calcination temperatures for both cases. Such materials with direct macroscopic shapes would hold promise as highly functionalized materials for potential practical applications, especially in photocatalysis.

36 MATERIALS SCIENCE↗

DOE OSTI2016

The effect of BaTiO{sub 3} particle shape on complex permittivity of 0.98MgTiO{sub 3}–0.02BaTiO{sub 3} composite powders at GHz frequencies

Highlights: • Elongated micrometre sized BaTiO{sub 3} particles had strong effect on permittivity. • Effect was significantly stronger compared to μm and nm sized spherical particles. • Properties could be tailored by varying the particle shapes of dielectric powders. • Could be utilized, e.g., in a production of electrical composites for RF applications. - Abstract: The effect of BaTiO{sub 3} particle shape on the properties of 0.98MgTiO{sub 3}–0.02BaTiO{sub 3} composite powders was characterized and analyzed using an indirectly coupled open-ended coaxial cavity resonator at gigahertz frequencies. Elongated micrometre sized BaTiO{sub 3} particles were found to have a significantly stronger effect on permittivity when compared to composite powders having micro and nano sized spherical BaTiO{sub 3} particles. Inclusion permittivities and dielectric loss tangents of composite powders increased from that of pure MgTiO{sub 3} powder, 13.3 and 4.6 × 10{sup −3}, up to 15.7 and 1.7 × 10{sup −2} with needle shaped BaTiO{sub 3} particles, respectively. The presented results give valuable information for tailoring the properties of dielectrics which can be utilized in the vast field of electronic component manufacturing.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Microwave-assisted synthesis of well-shaped UiO-66-NH2 with high CO2 adsorption capacity

Highlights: • Well-shaped UiO-66-NH{sub 2} was prepared through microwave heating in a short time. • Addition of HAc improves crystallinity and CO{sub 2} adsorption capacity of the UiO-66-NH{sub 2}. • UiO-66-NH{sub 2} prepared by microwave heating shows a higher CO{sub 2}/N{sub 2} adsorption selectivity. - Abstract: In a detailed study, the influence of microwave irradiation, synthesis time and temperature, addition of acetic acid (HAc) as a modulator on the morphology, crystallinity and stability of UiO-66-NH{sub 2} is investigated to develop a reliable and reproducible strategy for the preparation of well-shaped UiO-66-NH{sub 2}. The UiO-66-NH{sub 2} were characterized by powder X-ray diffraction (PXRD), field emission scanning electron microscopy (FESEM), thermogravimetric analysis (TGA), and gas adsorption. It is found that well-shaped UiO-66-NH{sub 2} with a high CO{sub 2} adsorption capacity can be synthesized in a short time by microwave heating. The UiO-66-NH{sub 2} crystals synthesized by microwave heating are of high quality and show a superior CO{sub 2} adsorption capacity (5.8 mmol/g at 273k and 1 bar) due to the strong interactions between the −NH{sub 2} group and CO{sub 2}. The CO{sub 2}/N{sub 2} selectivity of the obtained UiO-66-NH{sub 2} at 298 K and 1 bar is 66, which is much higher than that of the pristine UiO-66 of 17.8.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2018

Digital pulse deconvolution with adaptive shaping for real-time high-resolution high-throughput gamma spectroscopy

A high-resolution high-throughput real-time adaptive digital pulse processing system is developed for high count rate gamma-ray spectroscopy applications. The adaptive digital pulse processing algorithms are implemented on a reconfigurable FPGA and include a pulse deconvolver, adaptive shaping filter, timing filter, baseline restorer, and pile-up rejecter. Digital pulse deconvolution is implemented to reconstruct the original detector signal from the preamplifier signal, which reduces the resolution deterioration due to pulse pile-up. The deconvoluted signal is shaped with a trapezoid filter and the shaping parameter is selected adaptively based on the time separation between successive input pulses. Experimental measurements are performed with a 137Cs source under varying count-rate conditions and using germanium detectors equipped with resistive feedback and transistor reset preamplifiers (TRP). The results herein demonstrate that when using a TRP, adaptive digital signal processing allows handling 106 counts/s. In addition, the implementation of a deconvolution approach limits resolution deterioration for throughput rates that are 4 to 10 times better than achievable in typical digital and analog gamma-ray spectroscopy systems.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Modification of charged-particle jets in event-shape engineered Pb–Pb collisions at $\sqrt{S_{NN}}$ = 5.02 TeV

Charged-particle jet yields have been measured in semicentral Pb–Pb collisions at center-of-mass energy per nucleon–nucleon collision $\sqrt{S_{NN}}$ = 5.02 TeV with the ALICE detector at the LHC. These yields are reported as a function of the jet transverse momentum, and further classified by their angle with respect to the event plane and the event shape, characterized by ellipticity, in an effort to study the path-length dependence of jet quenching. Jets were reconstructed at midrapidity from charged-particle tracks using the anti-k T algorithm with resolution parameters R = 0.2 and 0.4, with event-plane angle and event-shape values determined using information from forward scintillating detectors. The results presented in this letter show that, in semicentral Pb–Pb collisions, there is no significant difference between jet yields in predominantly isotropic and elliptical events. However, out-of-plane jets are observed to be more suppressed than in-plane jets. Further, this relative suppression is greater for low transverse momentum (< 50 GeV/c) R = 0.2 jets produced in elliptical events, with out-of-plane to in-plane jet-yield ratios varying up to 5.2σ between different event-shape classes. These results agree with previous studies indicating that jets experience azimuthally anisotropic suppression when traversing the QGP medium, and can provide additional constraints on the path-length dependence of jet energy loss.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2018

Direct construction of optimized stellarator shapes. Part 1. Theory in cylindrical coordinates

The confinement of the guiding-centre trajectories in a stellarator is determined by the variation of the magnetic field strength $B$ in Boozer coordinates $(r,\unicode[STIX]{x1D703},\unicode[STIX]{x1D711})$ , but $B(r,\unicode[STIX]{x1D703},\unicode[STIX]{x1D711})$ depends on the flux surface shape in a complicated way. Here we derive equations relating $B(r,\unicode[STIX]{x1D703},\unicode[STIX]{x1D711})$ in Boozer coordinates and the rotational transform to the shape of flux surfaces in cylindrical coordinates, using an expansion in distance from the magnetic axis. A related expansion was done by Garren and Boozer ( Phys. Fluids B, vol. 3, 1991 a , 2805) based on the Frenet–Serret frame, which can be discontinuous anywhere the magnetic axis is straight, a situation that occurs in the interesting case of omnigenity with poloidally closed $B$ contours. Our calculation in contrast does not use the Frenet–Serret frame. The transformation between the Garren–Boozer approach and cylindrical coordinates is derived, and the two approaches are shown to be equivalent if the axis curvature does not vanish. The expressions derived here help enable optimized plasma shapes to be constructed that can be provided as input to VMEC and other stellarator codes, or to generate initial configurations for conventional stellarator optimization.

Physics↗

DOE OSTI2015

Mesophase stabilization in ionic liquid crystals through pairing equally shaped mesogenic cations and anions

The synthesis and properties of a set of novel ionic liquid crystals with congruently shaped cations and anions are reported to check whether pairing mesogenic cations with mesogenic anions leads to a stabilization of a liquid crystalline phase. To that avail 1-alkyl-3-methyl-triazolium cations with an alkyl chain length of 10, 12, and 14 carbon atoms have been combined with p-alkyloxy-benzenesulfonate anions with different alkyl chain lengths (n = 10, 12, and 14). The corresponding triazolium iodides have been synthesized as reference compounds where the cation and anion have strong size and shape mismatch. The mesomorphic behavior of all compounds is studied by differential scanning calorimetry and polarizing optical microscopy. All compounds except 1-methyl-3-decyltriazolium iodide, which qualifies as an ionic liquid, are thermotropic ionic liquid crystals. All other compounds adopt smectic A phases. As a result, a comparison of the thermal phase behavior of the 1-methyl-3-decyltriazolium bromides to the corresponding p-alkoxy-benzensulfonates reveals that definitely the mesophase is stabilized by pairing the rod-shaped 1-alkyl-3-methyltriazolium cation with a rod-like anion of similar size.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Precursor Identity and Surfactant Concentration Influence Shape of UO 2 Nanoparticles

A fundamental step toward studying the unique properties of actinide nanomaterials is control over the shape of actinide nanoparticles. Toward this goal, this work demonstrates the effects of precursor identity and surfactant concentration on the shape of uranium dioxide (UO 2 ) nanoparticles. UO 2 nanoparticles were synthesized by thermal decomposition of different precursors in the presence of oleylamine and oleic acid as surfactants. The size, shape, phase, and chemical composition of the nanoparticles was evaluated using transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDS), electron diffraction (ED), and U L 3 -edge X-ray absorption fine-structure (XAFS) spectroscopy. Anisotropic UO 2 nanocubes of ∼ 4 nm were obtained only with low surfactant concentrations, while increasing the surfactant concentration resulted in formation of nanoparticles with an isotropic, sphere morphology. The importance of precursor identity was also investigated by employing U(hfa) 4 , U(acac) 4 , UO 2 (acac) 2 , and UO 2 (hfa) 2 ·H 2 O (where hfa = hexafluoracetylacetone and acac = acetylacetone) as precursors. The nanocube morphology was only observed when U(hfa) 4 was used as a precursor. XAS allowed for comparison of the disorder in anisotropic vs isotropic UO 2 nanoparticles.

Nanocubes↗

DOE OSTI2025

Visualizing Stereodynamics in Cold Collisions through Shape Resonance Wavefunctions

Shape resonances in cold collisions are often strongly affected by stereodynamics. These resonances can sometimes be assigned by single-channel quantization along the scattering coordinate. However, sensitive steric control of collision implies strong anisotropy of the interaction potential energy surface, which usually leads to coupling among multiple scattering channels in the strongly interacting region. Hence, the resonances might be the result of quantization in a multidimensional space. Using the cold rotationally inelastic collision between para-H 2 (v 1 = 1, j 1 = 2) and HF (v 2 = 0, j 2 = 0) as an example, we analyze four low-lying shape resonances via diagonalization of the full-dimensional Hamiltonian with a stabilization method. While some resonances can indeed be assigned with a single partial wave, others apparently involve more than one scattering channel. Furthermore, a new model based on these resonance wavefunctions is developed to better understand the stereodynamics through shape resonances in cold collisions.

Collisions↗

DOE OSTI2015

Controlled Shape Memory Behavior of a Smectic Main-Chain Liquid Crystalline Elastomer

Here, we describe how a smectic main-chain liquid crystalline elastomer (LCE), with controlled shape memory behavior, is synthesized by polymerizing a biphenyl-based epoxy monomer with an aliphatic carboxylic acid curing agent. Microstructures of the LCEs, including their liquid crystallinity and cross-linking density, are modified by adjusting the stoichiometric ratio of the reactants to tailor the thermomechanical properties and shape memory behavior of the material. Thermal and liquid crystalline properties of the LCEs, characterized using differential scanning calorimetry and dynamic mechanical analysis, and structural analysis, performed using small-angle and wide-angle X-ray scattering, show that liquid crystallinity, cross-linking density, and network rigidity are strongly affected by the stoichiometry of the curing reaction. With appropriate structural modifications it is possible to tune the thermal, dynamic mechanical, and thermomechanical properties as well as the shape memory and thermal degradation behavior of LCEs.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Imaging Quantum Interference in Stadium-Shaped Monolayer and Bilayer Graphene Quantum Dots

Experimental realizations of graphene-based stadium-shaped quantum dots (QDs) have been few and have been incompatible with scanned probe microscopy. Yet, the direct visualization of electronic states within these QDs is crucial for determining the existence of quantum chaos in these systems. Here we report the fabrication and characterization of electrostatically defined stadium-shaped QDs in heterostructure devices composed of monolayer graphene (MLG) and bilayer graphene (BLG). To realize a stadium-shaped QD, we utilized the tip of a scanning tunneling microscope to charge defects in a supporting hexagonal boron nitride flake. The stadium states visualized are consistent with tight-binding-based simulations but lack clear quantum chaos signatures. The absence of quantum chaos features in MLG-based stadium QDs is attributed to the leaky nature of the confinement potential due to Klein tunneling. In contrast, for BLG-based stadium QDs (which have stronger confinement) quantum chaos is precluded by the smooth confinement potential which reduces interference and mixing between states.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Magnetic Solitons in Hierarchical 3D Magnetic Nanoarchitectures of Nanoflower Shape

Curvilinear magnetism emerged as a new route to tailor properties of magnetic solitons by the choice of geometry and topology of a magnetic architecture. Here, we develop an anodized aluminum oxide template-based approach to realize hierarchical 3D magnetic nanoarchitectures of nanoflower shape. The technique provides defect-free regular arrays of magnetic nanoflowers of tunable shape with a period of 400 nm over cm 2 areas. We combined advanced magnetic imaging methods with micromagnetic simulations to study complex magnetic states in nanoflowers originating due to magnetostatics-driven symmetry break in curvilinear nanomembranes. An interaction between surface and volume magnetostatic charges in 3D curved nanoflowers leads to the stabilization of asymmetric and shifted vortices as well as states with two Bloch lines. Ordered large area arrays of complex-shaped magnetic nanoarchitectures developed in this work are relevant for prospective research on 3D magnonics and spintronics.

3D nanoarchitectures↗

DOE OSTI2025

Volumetric Shaping of Nanoparticle-DNA Crystals by Light-Induced Milling

DNA-programmable self-assembly enables the formation of nanoparticle crystals with controlled lattice symmetry. While this approach offers the formation of complexly ordered nanostructures for optical, mechanical, and biological applications, a mesoscale control over such nanomaterials is limited. Directing the material formation process through the assembly pathway or external fields allows for modulating crystal morphology, but achieving arbitrary morphology remains challenging. Here, we present a photothermal method for shaping 3D DNA-programmable crystals of gold nanoparticles. Through local heating of nanoparticles due to plasmonic light absorption, we induce targeted volumetric dissolution of specifically defined crystal areas with micron-scale accuracy. This technique effectively prescribes crystal shaping and creates arbitrarily shaped voids within crystals. We further investigate both computationally and experimentally the key factors governing volumetric material subtraction. The developed automated light-milling platform enables the fabrication of nanomaterials exhibiting both DNA-programmable nanoscale order and custom-designed mesoscale architecture.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Shape-Specific Patterning of Polymer-Functionalized Nanoparticles

Chemically and topographically patterned nanoparticles (NPs) with dimensions on the order of tens of nanometers have a diverse range of applications and are a valuable system for fundamental research. Recently, thermodynamically controlled segregation of a smooth layer of polymer ligands into pinned micelles (patches) offered an approach to nanopatterning of polymer-functionalized NPs. Control of the patch number, size, and spatial distribution on the surface of spherical NPs has been achieved, however, the role of NP shape remained elusive. Here, we report the role of NP shape, namely, the effect of the local surface curvature, on polymer segregation into surface patches. For polymer-functionalized metal nanocubes, we show experimentally and theoretically that the patches form preferentially on the high-curvature regions such as vertices and edges. An in situ transformation of the nanocubes into nanospheres leads to the change in the number and distribution of patches; a process that is dominated by the balance between the surface energy and the stretching energy of the polymer ligands. The experimental and theoretical results presented in this work are applicable to surface patterning of polymer-capped NPs with different shapes, which then enables the exploration of patch-directed self-assembly, as colloidal surfactants, and as templates for the synthesis of hybrid nanomaterials.

36 MATERIALS SCIENCE↗

DOE OSTI2024

3D Printing ofThermally Responsive Shape Memory LiquidCrystalline Epoxy Networks

Abstract A two-component liquid crystalline epoxy network (LCEN) with shape memory behavior was developed and evaluated as a candidate material for 3D printing. The cure kinetics of the uncured material and the shape memory properties of the cured LCEN were investigated by using parallel plate rheology and dynamic mechanical analysis, respectively. A commercially available fumed silica additive was introduced to the neat, uncured material to improve the rheological properties for 3D printing. The addition of fumed silica was found to increase the yield stress, shear-thinning behavior, and toughness of the uncured epoxy ink. Polarized light microscopy, differential scanning calorimetry, and wide-angle X-ray scattering measurements between the neat and additive-modified LCEN suggested a reduction in liquid crystalline alignment in the modified LCEN, owing to interactions between crystalline domains and fumed silica, which in turn influenced the mechanical behavior. Overall, the additive was found to be successful in preserving the shape memory properties of LCEN while improving its printability.

Chemistry↗

DOE OSTI2021

Enabling the Application of Large Footprint Open-Bottom Permeameters through New Shape Factors

Open-bottom permeameters (OBP) are commonly used for estimating the hydraulic properties of sediment beds under water bodies and fluxes across the sediment-water interface. The specific shape factor for an OBP flow situation is necessary for data interpretation. It is determined by the ratio of the permeameter tube radius to the tube's penetration depth within the sediment. Previous permeameter designs favored small radii which allowed for deeper penetration and stability of the tube. The shape factor is provided here for large footprint OBPs that allows for shallow penetration and greater radius. Through a numerical and analytical modeling study of the OBP hydrodynamics, previous knowledge on the OBP shape factor is generalized to the entire range of radius-to-penetration ratios that might be practically applied. The results reveal the advantages of the large footprint design, including better sensitivity due to the ability to impose larger discharge over a shorter test duration.

42 ENGINEERING↗

DOE OSTI2015

Superlattices assembled through shape-induced directional binding

Organization of spherical particles into lattices is typically driven by packing considerations. Although the addition of directional binding can significantly broaden structural diversity, nanoscale implementation remains challenging. Here we investigate the assembly of clusters and lattices in which anisotropic polyhedral blocks coordinate isotropic spherical nanoparticles via shape-induced directional interactions facilitated by DNA recognition. We show that these polyhedral blocks—cubes and octahedrons—when mixed with spheres, promote the assembly of clusters with architecture determined by polyhedron symmetry. Moreover, three-dimensional binary superlattices are formed when DNA shells accommodate the shape disparity between nanoparticle interfaces. The crystallographic symmetry of assembled lattices is determined by the spatial symmetry of the block’s facets, while structural order depends on DNA-tuned interactions and particle size ratio. Lastly, the presented lattice assembly strategy, exploiting shape for defining the global structure and DNA-mediation locally, opens novel possibilities for by-design fabrication of binary lattices.

59 BASIC BIOLOGICAL SCIENCES↗