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At least 649 records · Page 36

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DOE OSTI2014

A simple approach for the synthesis of Ag-coated Ni@TiO{sub 2} nanocomposites as recyclable photocatalysts and SERS substrate to monitor catalytic degradation of dye molecules

Graphical abstract: - Highlights: • A simple approach was used to synthesize Ag-coated Ni@TiO{sub 2} nanocomposites. • The nanocomposites can be the convenient and effective SERS substrate. • The nanocomposites can be a self-cleaning SERS substrate. • The nanocomposites can monitor the catalytic degradation of dye molecules. - Abstract: In this work, we demonstrate an extremely simple and speedy approach to synthesis Ag-coated Ni@TiO{sub 2} nanocomposites, which can be a convenient and effective substrate for surface enhanced Raman spectroscopy (SERS) observation. Due to possessing the excellent magnetic properties and stable catalytic properties at room temperature, the nanocomposites can clean themselves by photocatalytic degradation of dye molecules under irradiation with UV light into inorganic small molecules for the self-cleaning SERS detection. Furthermore, the nanocomposites can be used as the SERS substrate for monitoring the catalytic degradation of dye molecules.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Modulation of microstructure and optical properties of Mo-doped ZnO thin films by substrate temperature

Highlights: • Mo-doped ZnO films are obtained by sputtering at various substrate temperatures. • High-quality MZO thin films with good crystalline have been obtained at 200 °C. • Deposition temperature affects the amount of defects in the crystalline structure - Abstract: Mo-doped ZnO(MZO) films were deposited on Si (1 1 1) substrates by radio frequency sputtering at different substrate temperatures of 200, 300 and 400 °C. The effect of the substrate temperature on the structural and optical properties of the MZO films has been investigated. X-ray diffraction results reveal that all the films are polycrystalline with a hexagonal wurtzite structure with a preferential orientation according to the direction (0 0 2) plane. The crystallinity and surface morphologies of the films are strongly dependent on the growth temperature, which in turn exerts a great effect on microstructural and optical properties of the MZO films. The optical absorption measurements show high ultraviolet (UV) absorbance property of MZO with sharp and intense absorption band in this region and the optical band gap (E{sub g}) are 3.18, 3.22, 3.25 and 3.21 eV for the films deposited at room temperature, 200, 300 and 400 °C. The photoluminescence (PL) intensity of a strong broad violet–blue emission from MZO nanostructures with increasing deposited temperature was also observed. X-ray photoelectron spectroscopy (XPS) was employed to investigate the surface chemical composition of growth products.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Substrate bias induced synthesis of flowered-like bunched carbon nanotube directly on bulk nickel

Highlights: • Flowered-like bunched MWCNTs have been synthesized by MW PECVD technique. • Effect of substrate bias on the properties of MWCNT has been studied. • Minimum E{sub T} = 1.9 V/μm with β = 4770 has been obtained in the film deposited at −350 V. - Abstract: This paper reports the effect of substrate bias on the multiwalled carbon nanotube (MWCNT) deposited on nickel foil by microwave plasma enhanced chemical vapor deposition technique. The MWCNTs have been characterized by the scanning electron microscopy (SEM), high resolution transmission electron microscopy (HRTEM), Raman spectroscopy, field emission and current–voltage characteristic of the heterojunction diode. The SEM images exhibit unique hierarchical flowered-like bunched and conformally coated MWCNTs. Substrate bias induced ion bombardment helps in the enhancement of hydrocarbon dissociation and is responsible for flowered-like MWCNTs growth. The HRTEM micrographs show the base growth mechanism for MWCNTs. The value of turn on field for emission decreases from 5.5 to 1.9 V/μm and field enhancement factor increases from 927 to 4770, respectively, with the increase of substrate bias. The diode ideality factor of CNT/ n-Si heterojunction is evaluated as 2.4 and the on/off current ratio is found to be 7 at ±2 V, respectively.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Effect of Ar ion-beam-assistance and substrate temperature on physical properties of Al-doped ZnO thin films deposited by RF magnetron sputtering

Highlights: • AZO and IAZO (303–473 K) films were grown by RF magnetron sputtering technique. • Ar ion-beam converts its kinetic energy as diffusion energy to the deposited atoms. • Structural evolution relies on diffusion energy imparted to the deposited atoms. • Surface texture densify under the aid of ion-beam and substrate temperature. - Abstract: In this study, pronounced effects of ion-beam-assistance and substrate temperature were revealed by exploring the physical properties of Al-doped ZnO thin films deposited by the RF magnetron sputtering technique. Herein, two measurable parameters, ion-beam discharge current (0.1 A) and substrate temperature (303–473 K) were adopted to regulate the structural changes in Al-doped ZnO films. Specifically, progressive structural changes were achieved based on the addition of Ar ion-beam during the film growth. From XRD analysis, we observed significant structural changes that provided an improvement in the film growth towards c-axis (002) plane. In addition, FESEM and AFM analyses demonstrated excellent surface features with the assisted Ar ion-beam. As a result of this process, we effectively modulated the binding energy of Zn 2p level. Finally, the structural investigation accurately demonstrated that the dependence of assisted ion-beam and substrate temperature linearly related to the superior visible transmittance and reduced band gap.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Microstructural evolution, defect mitigation, and precipitation behavior in AA6061 via laser powder bed fusion with high-temperature substrate heating

Defects, particularly solidification cracking, remain persistent challenges in the laser powder bed fusion (LPBF) processing of AA6061 aluminum alloy. This study systematically investigates defect mitigation, microstructural evolution, and mechanical properties associated with high-temperature substrate preheating at 500 °C. Comprehensive microstructural analyses, including characterization of defects, grain structures, and precipitation behavior, were performed on samples in both as-built and T6 heat-treated states. Elevated preheating substantially reduced solidification cracking across a wide processing window, while demonstrating decreased crack sensitivity to laser parameters. Columnar cracks along the build direction were observed despite substrate preheating. Lack-of-fusion and keyhole porosity were effectively eliminated, though gas-induced microporosity persisted at higher powers. In-depth characterization of two distinct laser power and speed conditions confirmed the formation of micron-sized, non-coherent Mg 2 Si precipitates under heated substrate conditions, alongside α-AlFeCrMnSi intermetallic phases indicative of in-situ thermal effects during fabrication. Subsequent T6 heat treatment revealed the formation of fine, coherent needle-shaped β″ strengthening precipitates. Despite substantial differences in processing parameters, comparable mechanical properties were measured in the as-built samples (∼52 MPa yield strength, ∼130 MPa tensile strength), primarily due to reduced strain hardening effects and consistent precipitation characteristics. Meanwhile, the T6 heat treatment led to significant improvement in properties, enhancing yield strength by over 400%, aligning closely with the performance of conventional wrought AA6061-T6. These findings underscore that high-temperature substrate preheating offers an effective means to suppress cracks, control precipitation, and enhance mechanical performance in LPBF-processed AA6061.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Chemical identity of carbon substrates drives differences in denitrification and N 2 O reduction within agricultural soils

Rates of nitrous oxide (N 2 O) production from agricultural soils are highly variable across space and time. Improving predictions of N 2 O emissions will require improving our understanding of the drivers of denitrification and the sources of variability in the rates of N 2 O production between soils and over time. While the amount of available carbon (C) is a known control on denitrification and N 2 O reduction, relatively little attention has been paid to the effect of the chemical identity of C substrates on rates of denitrification and N 2 O reduction. We investigated the effects of twelve different C-substrate additions on the production and reduction of N 2 O in five soils taken from two distinct agricultural locations in Michigan under multiple land uses. We provided additions of glucose, cellulose, N-acetyl-glucosamine, chitin, amino acids, protein, vanillyl alcohol, lignin, citrate, succinate, methanol, and water in laboratory denitrification potential assays to determine the effects of denitrifier C preference on denitrification rates. We found that amino acids, protein, and organic acids stimulated the greatest rates of denitrification potential across all land uses. Similarly, we found these same substrates caused the most N 2 O reduction, resulting in the lowest net concentrations of N 2 O. Soils from agricultural rotations without cover crops had overall lower rates of denitrifier activity, leading to less net N 2 O production compared to soils from other land uses. In general, C-utilization patterns were similar among all soils, and C-substrate identity had a much stronger effect than land use. Here, we demonstrate that the chemical identity of available C gives rise to wide variability in rates of denitrification and N 2 O reduction.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2023

Reversal of Catalytic Material Substrate Selectivity through Partitioning of Polymers in Hierarchically Ordered Virus-like Particle Frameworks

Control over the selectivity of catalytic materials is a topic of growing interest. Virus-like particle (VLP) based materials such as protein macromolecular frameworks (PMFs) are promising for catalytic applications due to their ease of assembly, modular ability to encapsulate a variety of enzymes, and ease of separation from a reaction mixture. Here we demonstrate the reversal of the initially negative material charge through the titration of a positively charged polymer into the material, causing the reversal of guest molecule uptake and enzymatic activity of PMFs. The charge-inverse material partitions a charged enzyme substrate to concentrate the substrate near an enzyme incorporated within the material, generating up to 5.9-fold increases in enzyme activity toward the partitioned substrate over the excluded substrate. Here we also show that the polymer distributes heterogeneously through the material up to a point of saturation and the effects of guest macromolecules on the lattice parameters of PMFs.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Roughness of Ti Substrates for Control of the Preferred Orientation of TiO 2 Nanotube Arrays as a New Orientation Factor

We report the surface roughness of a Ti substrate as a critical factor for controlling the degree of the preferred orientation of anatase TiO2 nanotube arrays (NTAs) which are synthesized by anodization and a subsequent annealing process. The degree of the preferred orientation to the (004) plane of the anatase crystal structure has a strong dependency on the root-mean-square roughness (Sq) of the initial Ti substrate when the roughness-controlled substrates are anodized in an ethylene glycol-based electrolyte containing ~2 wt % of water. Highly preferred oriented NTAs were obtained from low-Sq (<10 nm) substrates, which were accompanied by uniform pore distribution and low concentration of hydroxyl ions in as-anodized amorphous NTAs. The mechanism of the preferred oriented crystallization of nanometer-scaled tube walls is explained considering the microscopic geometrical uniformity of the oxide barrier and nanopores at the early stage of anodization, which affected the local electric field and thus the insertion of the hydroxyl group into the amorphous TiO2 tube walls.

14 SOLAR ENERGY↗

DOE OSTI2012

A Conserved Surface Loop in Type I Dehydroquinate Dehydratases Positions an Active Site Arginine and Functions in Substrate Binding

Dehydroquinate dehydratase (DHQD) catalyzes the third step in the biosynthetic shikimate pathway. We present three crystal structures of the Salmonella enterica type I DHQD that address the functionality of a surface loop that is observed to close over the active site following substrate binding. Two wild-type structures with differing loop conformations and kinetic and structural studies of a mutant provide evidence of both direct and indirect mechanisms of involvement of the loop in substrate binding. In addition to allowing amino acid side chains to establish a direct interaction with the substrate, closure of the loop necessitates a conformational change of a key active site arginine, which in turn positions the substrate productively. The absence of DHQD in humans and its essentiality in many pathogenic bacteria make the enzyme a target for the development of nontoxic antimicrobials. The structures and ligand binding insights presented here may inform the design of novel type I DHQD inhibiting molecules.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2012

X-ray structures of LeuT in substrate-free outward-open and apo inward-open states

Neurotransmitter sodium symporters are integral membrane proteins that remove chemical transmitters from the synapse and terminate neurotransmission mediated by serotonin, dopamine, noradrenaline, glycine and GABA ({gamma}-aminobutyric acid). Crystal structures of the bacterial homologue, LeuT, in substrate-bound outward-occluded and competitive inhibitor-bound outward-facing states have advanced our mechanistic understanding of neurotransmitter sodium symporters but have left fundamental questions unanswered. Here we report crystal structures of LeuT mutants in complexes with conformation-specific antibody fragments in the outward-open and inward-open states. In the absence of substrate but in the presence of sodium the transporter is outward-open, illustrating how the binding of substrate closes the extracellular gate through local conformational changes: hinge-bending movements of the extracellular halves of transmembrane domains 1, 2 and 6, together with translation of extracellular loop 4. The inward-open conformation, by contrast, involves large-scale conformational changes, including a reorientation of transmembrane domains 1, 2, 5, 6 and 7, a marked hinge bending of transmembrane domain 1a and occlusion of the extracellular vestibule by extracellular loop 4. These changes close the extracellular gate, open an intracellular vestibule, and largely disrupt the two sodium sites, thus providing a mechanism by which ions and substrate are released to the cytoplasm. The new structures establish a structural framework for the mechanism of neurotransmitter sodium symporters and their modulation by therapeutic and illicit substances.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Insights from designing an artificial cascade catalysis system using principles from substrate channeling in enzymes

Generalizing the key requirements of highly-selective, multi-step chemical conversions involving spatially separated reaction centers remains one of the grand challenges of chemistry. Much work towards this effort has focused on decomposing multi-step conversions into their constituent reactions, whose intermediates are successively upgraded in a chemical cascade via diffusion from center to center. This approach for synthesizing more complex molecules takes its cues from biochemical networks, where near-unit conversion of even complex carbohydrates is achieved by upgrading chemical precursors via enzymatic cascades. In this computational study we examine a simple cascade involving coupled Ag and Cu catalysts that sequentially converts CO2 to CO and then CO2 and CO to reduced products, generically named CO2Product and COProduct. The system architecture is inspired by the phenomenon of biological substrate channeling, and components are examined to evaluate their effects on conversion efficiency in the cascade. Aside from a substrate channel linking two reaction centers, we find efficient cascades must also incorporate directional substrate diffusion, compartmentalization of the reaction centers, and proper timing of substrate arrival at the active center. We make explicit linkages between these requirements and chemical conversion in known biological systems, revealing additional control elements that could be incorporated.

CO 2 reduction↗

DOE OSTI2012

Role of the substrate in the electrical transport characteristics of focused ion beam fabricated nanogap electrode

Precise metallic nanogap structure is fabricated on a glass substrate by using a 30 keV focused Ga ion beam. While investigating the I-V behavior of the nanogap structure, tunneling through the substrate has been found to play a vital role in the electrical transportation process. Substrate breakdown occurs at a certain applied voltage and a metal vapor state is initiated through intense heat generation at the nanogap region. The experimental observation confirms the role of the substrate in the explosion process. Metallic spherical particles are formed during cooling/condensation of the metal vapors or splashing of the liquid droplets showing a wide distribution of size from few tens of nanometers to few microns.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2013

Impact of substrate temperature on the structural and optical properties of strain-balanced InAs/InAsSb type-II superlattices grown by molecular beam epitaxy

Molecular beam epitaxial growth of strain-balanced InAs/InAs{sub 1-x}Sb{sub x} type-II superlattices on GaSb substrates has been investigated for substrate temperatures from 400 Degree-Sign C to 450 Degree-Sign C. The Sb composition is found to vary linearly with substrate temperature at constant V/III ratios. For samples grown at the optimized substrate temperature (410 Degree-Sign C), superlattice zero-order peak full-width at half-maximums are routinely less than 25 arc sec using high-resolution X-ray diffraction. Cross-sectional transmission electron microscopy images show the absence of any visible defects. Strong photoluminescence covers a wavelength range from 5.5 to 13 {mu}m at 12 K. Photoluminescence linewidth simulations show satisfactory agreement with experiments.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Structural and optical properties of Ag-doped copper oxide thin films on polyethylene napthalate substrate prepared by low temperature microwave annealing

Silver doped cupric oxide thin films are prepared on polyethylene naphthalate (flexible polymer) substrates. Thin films Ag-doped CuO are deposited on the substrate by co-sputtering followed by microwave assisted oxidation of the metal films. The low temperature tolerance of the polymer substrates led to the search for innovative low temperature processing techniques. Cupric oxide is a p-type semiconductor with an indirect band gap and is used as selective absorption layer solar cells. X-ray diffraction identifies the CuO phases. Rutherford backscattering spectrometry measurements confirm the stoichiometry of each copper oxide formed. The surface morphology is determined by atomic force microscopy. The microstructural properties such as crystallite size and the microstrain for (-111) and (111) planes are calculated and discussed. Incorporation of Ag led to the lowering of band gap in CuO. Consequently, it is determined that Ag addition has a strong effect on the structural, morphological, surface, and optical properties of CuO grown on flexible substrates by microwave annealing. Tauc's plot is used to determine the optical band gap of CuO and Ag doped CuO films. The values of the indirect and direct band gap for CuO are found to be 2.02 eV and 3.19 eV, respectively.

36 MATERIALS SCIENCE↗

DOE OSTI2013

In situ study of the role of substrate temperature during atomic layer deposition of HfO{sub 2} on InP

The dependence of the “self cleaning” effect of the substrate oxides on substrate temperature during atomic layer deposition (ALD) of HfO{sub 2} on various chemically treated and native oxide InP (100) substrates is investigated using in situ X-ray photoelectron spectroscopy. The removal of In-oxide is found to be more efficient at higher ALD temperatures. The P oxidation states on native oxide and acid etched samples are seen to change, with the total P-oxide concentration remaining constant, after 10 cycles of ALD HfO{sub 2} at different temperatures. An (NH{sub 4}){sub 2} S treatment is seen to effectively remove native oxides and passivate the InP surfaces independent of substrate temperature studied (200 °C, 250 °C and 300 °C) before and after the ALD process. Density functional theory modeling provides insight into the mechanism of the changes in the P-oxide chemical states.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Growth mechanism and microstructure of low defect density InN (0001) In-face thin films on Si (111) substrates

Transmission electron microscopy has been employed to analyze the direct nucleation and growth, by plasma-assisted molecular beam epitaxy, of high quality InN (0001) In-face thin films on (111) Si substrates. Critical steps of the heteroepitaxial growth process are InN nucleation at low substrate temperature under excessively high N-flux conditions and subsequent growth of the main InN epilayer at the optimum conditions, namely, substrate temperature 400–450 °C and In/N flux ratio close to 1. InN nucleation occurs in the form of a very high density of three dimensional (3D) islands, which coalesce very fast into a low surface roughness InN film. The reduced reactivity of Si at low temperature and its fast coverage by InN limit the amount of unintentional Si nitridation by the excessively high nitrogen flux and good bonding/adhesion of the InN film directly on the Si substrate is achieved. The subsequent overgrowth of the main InN epilayer, in a layer-by-layer growth mode that enhances the lateral growth of InN, reduces significantly the crystal mosaicity and the density of threading dislocations is about an order of magnitude less compared to InN films grown using an AlN/GaN intermediate nucleation/buffer layer on Si. The InN films exhibit the In-face polarity and very smooth atomically stepped surfaces.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Controllable strain-induced uniaxial anisotropy of Fe{sub 81}Ga{sub 19} films deposited on flexible bowed-substrates

We propose a convenient method to induce a uniaxial anisotropy in magnetostrictive Fe{sub 81}Ga{sub 19} films grown on flexible polyethylene terephthalate (PET) substrates by bending the substrate prior to deposition. A tensile/compressive stress is induced in the Fe{sub 81}Ga{sub 19} films when PET substrates are shaped from concave/convex to flat after deposition. The stressed Fe{sub 81}Ga{sub 19} films exhibit a significant uniaxial magnetic anisotropy due to the internal stress arising from changes in shape of PET substrates. The easy axis is along the tensile stress direction and the coercive field along easy axis is increased with increasing the internal tensile stress. The remanence of hard axis is decreased with increasing the compressive stress, while the coercive field is almost unchanged. A modified Stoner-Wohlfarth model with considering the distribution of easy axes in polycrystalline films is used to account for the magnetic properties tuned by the strain-controlled magnetoelastic anisotropy in flexible Fe{sub 81}Ga{sub 19} films. Our investigations provide a convenient way to induce uniaxial magnetic anisotropy, which is particularly important for fabricating flexible magnetoelectronic devices.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Sharp semiconductor-to-metal transition of VO{sub 2} thin films on glass substrates

Outstanding phase transition properties of vanadium dioxide (VO{sub 2}) thin films on amorphous glass were achieved and compared with the ones grown on c-cut sapphire and Si (111) substrates, all by pulsed laser deposition. The films on glass substrate exhibit a sharp semiconductor-to-metal transition (∼4.3 °C) at a near bulk transition temperature of ∼68.4 °C with an electrical resistance change as high as 3.2 × 10{sup 3} times. The excellent phase transition properties of the films on glass substrate are correlated with the large grain size and low defects density achieved. The phase transition properties of VO{sub 2} films on c-cut sapphire and Si (111) substrates were found to be limited by the high defect density.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗