Mixed Close-Packed Cobalt Molybdenum Nitrides as Non-noble Metal Electrocatalysts for the Hydrogen Evolution Reaction
Abstract not provided
Cao, Bingfei↗
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Genomes and gene expression across light and productivity gradients in eastern subtropical Pacific microbial communities
Here, transitions in community genomic features and biogeochemical processes were examined in surface and subsurface chlorophyll maximum (SCM) microbial communities across a trophic gradient from mesotrophic waters near San Diego, California to the oligotrophic Pacific. Transect end points contrasted in thermocline depth, rates of nitrogen and CO 2 uptake, new production and SCM light intensity. Relative to surface waters, bacterial SCM communities displayed greater genetic diversity and enrichment in putative sulfur oxidizers, multiple actinomycetes, low-light-adapted Prochlorococcus and cell-associated viruses. Metagenomic coverage was not correlated with transcriptional activity for several key taxa within Bacteria. Low-light-adapted Prochlorococcus, Synechococcus, and low abundance gamma-proteobacteria enriched in the>3.0-μm size fraction contributed disproportionally to global transcription. The abundance of these groups also correlated with community functions, such as primary production or nitrate uptake. In contrast, many of the most abundant bacterioplankton, including SAR11, SAR86, SAR112 and high-light-adapted Prochlorococcus , exhibited low levels of transcriptional activity and were uncorrelated with rate processes. Eukaryotes such as Haptophytes and non-photosynthetic Aveolates were prevalent in surface samples while Mamielles and Pelagophytes dominated the SCM. Metatranscriptomes generated with ribosomal RNA-depleted mRNA (total mRNA) coupled to in vitro polyadenylation compared with polyA-enriched mRNA revealed a trade-off in detection eukaryotic organelle and eukaryotic nuclear origin transcripts, respectively. Gene expression profiles of SCM eukaryote populations, highly similar in sequence identity to the model pelagophyte Pelagomonas sp. CCMP1756, suggest that pelagophytes are responsible for a majority of nitrate assimilation within the SCM.
54 ENVIRONMENTAL SCIENCES↗
Near-field examination of perovskite-based superlenses and superlens-enhanced probe-object coupling
A planar slab of negative-index material works as a superlens with sub-diffraction-limited resolution, as propagating waves are focused and, moreover, evanescent waves are reconstructed in the image plane. Here we demonstrate a superlens for electric evanescent fields with low losses using perovskites in the mid-infrared regime. The combination of nearfield microscopy with a tunable free-electron laser allows us to address precisely the polariton modes, which are critical for super-resolution imaging. We spectrally study the lateral and vertical distributions of evanescent waves around the image plane of such a lens, and achieve imaging resolution of λ/14 at the superlensing wavelength. Interestingly, at certain distances between the probe and sample surface, we observe a maximum of these evanescent fields. Comparisons with numerical simulations indicate that this maximum originates from an enhanced coupling between probe and object, which might be applicable for multifunctional circuits, infrared spectroscopy and thermal sensors.
36 MATERIALS SCIENCE↗
Manipulating the insulator–metal transition through tip-induced hydrogenation
Manipulating the insulator–metal transition in strongly correlated materials has attracted a broad range of research activity due to its promising applications in, for example, memories, electrochromic windows and optical modulators. Electric-field-controlled hydrogenation using ionic liquids and solid electrolytes is a useful strategy to obtain the insulator–metal transition with corresponding electron filling, but faces technical challenges for miniaturization due to the complicated device architecture. Here, in this work, we demonstrate reversible electric-field control of nanoscale hydrogenation into VO 2 with a tunable insulator–metal transition using a scanning probe. The Pt-coated probe serves as an efficient catalyst to split hydrogen molecules, while the positive-biased voltage accelerates hydrogen ions between the tip and sample surface to facilitate their incorporation, leading to non-volatile transformation from insulating VO 2 into conducting H x VO 2 . Remarkably, a negative-biased voltage triggers dehydrogenation to restore the insulating VO 2 . This work demonstrates a local and reversible electric-field-controlled insulator–metal transition through hydrogen evolution and presents a versatile pathway to exploit multiple functional devices at the nanoscale.
36 MATERIALS SCIENCE↗
Fractal analysis of collision cascades in pulsed-ion-beam-irradiated solids [Collision cascade densities in ion pulsed ion irradiated solids { a fractal approach]
The buildup of radiation damage in ion-irradiated crystals often depends on the spatial distribution of atomic displacements within collision cascades. Although collision cascades have previously been described as fractals, the correlation of their fractal parameters with experimental observations of radiation damage buildup remains elusive. Here, we use a pulsed-ion-beam method to study defect interaction dynamics in 3C-SiC irradiated at 100 °C with ions of different masses. These data, together with results of previous studies of SiC and Si, are analyzed with a model of radiation damage formation which accounts for the fractal nature of collision cascades. Our emphasis is on the extraction of the effective defect diffusion length from pulsed beam measurements. Results show that, for both Si and SiC, collision cascades are mass fractals with fractal dimensions in the range of ~1–2, depending on ion mass, energy, and the depth from the sample surface. Within our fractal model, the effective defect diffusion length is ~10 nm for SiC and ~20 nm for Si, and it decreases with increasing cascade density. These results demonstrate a general method by which the fractal nature of collision cascades can be used to explain experimental observations and predict material’s response to radiation.
36 MATERIALS SCIENCE↗
Detection of antimicrobial resistance genes associated with the International Space Station environmental surfaces
Antimicrobial resistance (AMR) is a global health issue. In an effort to minimize this threat to astronauts, who may be immunocompromised and thus at a greater risk of infection from antimicrobial resistant pathogens, a comprehensive study of the ISS “resistome’ was conducted. Using whole genome sequencing (WGS) and disc diffusion antibiotic resistance assays, 9 biosafety level 2 organisms isolated from the ISS were assessed for their antibiotic resistance. Molecular analysis of AMR genes from 24 surface samples collected from the ISS during 3 different sampling events over a span of a year were analyzed with Ion AmpliSeq™ and metagenomics. Disc diffusion assays showed that Enterobacter bugandensis strains were resistant to all 9 antibiotics tested and Staphylococcus haemolyticus being resistant to none. Ion AmpliSeq™ revealed that 123 AMR genes were found, with those responsible for beta-lactam and trimethoprim resistance being the most abundant and widespread. Using a variety of methods, the genes involved in antimicrobial resistance have been examined for the first time from the ISS. Lastly, this information could lead to mitigation strategies to maintain astronaut health during long duration space missions when return to Earth for treatment is not possible.
59 BASIC BIOLOGICAL SCIENCES↗
Detection of hydrogen isotopes in Zircaloy-4 via femtosecond LIBS
Spatio-temporal mapping of species in a femtosecond laser induced Zircaloy-4 plasma identified conditions well-suited for the detection and analysis of deuterium across a wide range of concentrations.
Kautz, Elizabeth J.↗
Exploration of LIBS as a novel and rapid elemental mapping technique of nuclear fuels in the form of surrogate TRISO particles
Laser-induced breakdown spectroscopy (LIBS) was employed to characterize coatings on surrogate fuel particles. Tri-structural isotropic (TRISO) particles are a proposed nuclear fuel alternative for high temperature reactors. These particles are constructed of a ZrO 2 kernel (as a surrogate to uranium), surrounded by an inner pyrolytic carbon layer and are surrounded by an outer carbide layer (ZrC, presented here) to act as a barrier to fission products generated during nuclear reactions. These particles are embedded within a graphite compact and housed within the reactor core. Simply put, due to their robust nature, performing elemental analysis of these particles poses a challenge. Presented here, LIBS is explored as a method for characterizing elemental constituents of these particles, with the focus being on rapid elemental mapping and depth profiling. Different from traditional elemental analysis techniques (e.g., inductively coupled plasma – based methods), LIBS is advantageous because it can directly analyze the sample surface and can detect light elements such as C and O, making it a viable technique for the analysis of small, multilayered particles as spatial elemental information is warranted in the production of these particles. In the work presented here, LIBS was successfully used for discerning small layers (30–50 μm), detecting the location of carbon and oxygen layers, providing fast 2-D mapping (<5 min per particle) and rapid depth profiling (10 s per particle).
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Product gas evolution above planar microstructured model catalysts--A combined scanning mass spectrometry, Monte Carlo, and Computational Fluid Dynamics study
The transport and distribution of reaction products above catalytically active Pt microstructures was studied by spatially resolved scanning mass spectrometry (SMS) in combination with Monte Carlo simulation and fluid dynamics calculations, using the oxidation of CO as test reaction. The spatial gas distribution above the Pt fields was measured via a thin quartz capillary connected to a mass spectrometer. Measurements were performed in two different pressure regimes, being characteristic for ballistic mass transfer and diffusion involving multiple collisions for the motion of CO{sub 2} product molecules between the sample and the capillary tip, and using differently sized and shaped Pt microstructures. The tip height dependent lateral resolution of the SMS measurements as well as contributions from shadowing effects, due to the mass transport limitations between capillary tip and sample surface at close separations, were evaluated and analyzed. The data allow to define measurement and reaction conditions where effects induced by the capillary tip can be neglected (''minimal invasive measurements'') and provide a basis for the evaluation of catalyst activities on microstructured model systems, e.g., for catalyst screening or studies of transport effects.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Analysis of indium zinc oxide thin films by laser-induced breakdown spectroscopy
We have performed spectroscopic analysis of the plasma generated by Nd:YAG ({lambda} = 266 nm) laser irradiation of thin indium zinc oxide films with variable In content deposited by combinatorial pulsed laser deposition on glass substrates. The samples were irradiated in 5 x 10{sup 4} Pa argon using laser pulses of 5 ns duration and 10 mJ energy. The plasma emission spectra were recorded with an Echelle spectrometer coupled to a gated detector with different delays with respect to the laser pulse. The relative concentrations of indium and zinc were evaluated by comparing the measured spectra to the spectral radiance computed for a plasma in local thermal equilibrium. Plasma temperature and electron density were deduced from the relative intensities and Stark broadening of spectral lines of atomic zinc. Analyses at different locations on the deposited thin films revealed that the In/(In + Zn) concentration ratio significantly varies over the sample surface, from 0.4 at the borders to about 0.5 in the center of the film. The results demonstrate that laser-induced breakdown spectroscopy allows for precise and fast characterization of thin films with variable composition.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Transforming graphite to nanoscale diamonds by a femtosecond laser pulse
Formation of cubic diamond from graphite following irradiation by a single, intense, ultra-short laser pulse has been observed. Highly oriented pyrolytic graphite (HOPG) samples were irradiated by a 100 fs pulse with a center wavelength of 800 nm. Following laser exposure, the HOPG samples were studied using Raman spectroscopy of the sample surface. In the laser-irradiated areas, nanoscale cubic diamond crystals have been formed. The exposed areas were also studied using grazing incidence x-ray powder diffraction showing a restacking of planes from hexagonal graphite to rhombohedral graphite.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Developing the model of laser ablation by considering the interplay between emission and expansion of aluminum plasma
In the present study, the ablation behavior of aluminum target and its plasma radiation in noble ambient gases by a laser pulse with wavelength of 266 nm and pulse duration of 10 ns are numerically studied. A thermal model of laser ablation considering heat conduction, Euler equations, Saha-Eggert equations, Knudsen layer, mass and energy balance relations and optical shielding effects are used for calculation of plasma parameters. Effects of excitation energy on plasma expansion and its emissivity are investigated. Time and spatial-resolved plasma emission including bremsstrahlung, recombination and spectral emission at early delay times after laser irradiation is obtained. Effects of two ambient gases (He and Ar) as well as different gas pressures of 100, 300, 500, and 760 Torr on plasma expansion and its spectrum are studied. Results illustrate that at initial delay times, especially at high noble gas pressures, ionic lines have the maximum intensities, while at later times neutral lines dominate. When the pressure of ambient gas increases, a confinement of the plasma plume is predicted and the intensity of neutral lines decreases. Continuous emission increases with wavelength in both ambient gases. Spatially resolved analysis shows that an intense continuous emission is predicted next to the sample surface decreasing with distance from the latter.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Lattice and grain-boundary diffusions of boron atoms in BaSi{sub 2} epitaxial films on Si(111)
A 180-nm-thick boron (B) layer was deposited on a 300-nm-thick a-axis-oriented BaSi{sub 2} epitaxial film grown by molecular beam epitaxy on Si(111) and was annealed at different temperatures in ultrahigh vacuum. The depth profiles of B were investigated using secondary ion mass spectrometry (SIMS) with O{sup 2+}, and the diffusion coefficients of B were evaluated. The B profiles were reproduced well by taking both the lattice and the grain boundary (GB) diffusions into consideration. The cross-sectional transmission electron microscopy (TEM) image revealed that the GBs of the BaSi{sub 2} film were very sharp and normal to the sample surface. The plan-view TEM image exhibited that the grain size of the BaSi{sub 2} film was approximately 0.6 {mu}m. The temperature dependence of lattice and GB diffusion coefficients was derived from the SIMS profiles, and their activation energies were found to be 4.6 eV and 4.4 eV, respectively.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
The effects of plasma exposure and vacuum ultraviolet irradiation on photopatternable low-k dielectric materials
The effects of plasma exposure and vacuum-ultraviolet (VUV) irradiation on photopatternable low-k (PPLK) dielectric materials are investigated. In order to examine these effects, current-voltage measurements were made on PPLK materials before and after exposure to a variety of inert plasma-exposure conditions. In order to examine the effects of photon irradiation alone, PPLK samples were also exposed to monochromatic synchrotron radiation with 10 eV photon energy. It was found that plasma exposure causes significant degradation in electrical characteristics, resulting in increased leakage-currents and decreased breakdown voltage. X-ray photoelectron spectroscopy measurements also show appreciable carbon loss near the sample surface after plasma exposure. Conversely, VUV exposure was found to increase breakdown voltage and reduce leakage-current magnitudes.
36 MATERIALS SCIENCE↗
Photoacoustic methods for in vitro study of kinetics progesterone release from the biodegradation of polyhydroxybutyrate/polycaprolactone used as intravaginal devices
Intravaginal devices composed of polyhydroxybutyrate/polycaprolactone blends incorporating progesterone were used over eight days in crossbred cow ovariectomized, and then analyzed with photoacoustic methods, measuring the absorption spectra, thermal diffusivity, and inspecting its degradation by means of scanning electron microscopy. The characteristic time found for progesterone release was TR ∼ 53 h, and the typical time found for biodegradation was TB ∼ 30 h. Morphological analysis complements the study showing that release of progesterone and biodegradation of the blend occurs on sample surface.
36 MATERIALS SCIENCE↗
Production of fullerene ions by combining of plasma sputtering with laser ablation
We have produced C{sub 60} ion beams by combining plasma sputtering and laser ablation. A C{sub 60} sample was placed in an electron cyclotron resonance type ion source, negatively biased and sputtered by argon plasma. The beam current of C{sub 60}{sup +} decreased rapidly, but it was transiently recovered by a single laser shot that ablates the thin sample surface on the sputtered area. Temporal variations in beam current are reported in response to laser shots repeated at intervals of a few minutes.
43 PARTICLE ACCELERATORS↗
Electrical characterization of defects introduced in n-Ge during electron beam deposition or exposure
Schottky barrier diodes prepared by electron beam deposition (EBD) on Sb-doped n-type Ge were characterized using deep level transient spectroscopy (DLTS). Pt EBD diodes manufactured with forming gas in the chamber had two defects, E{sub 0.28} and E{sub 0.31}, which were not previously observed after EBD. By shielding the samples mechanically during EBD, superior diodes were produced with no measureable deep levels, establishing that energetic ions created in the electron beam path were responsible for the majority of defects observed in the unshielded sample. Ge samples that were first exposed to the conditions of EBD, without metal deposition (called electron beam exposure herein), introduced a number of new defects not seen after EBD with only the E-center being common to both processes. Substantial differences were noted when these DLTS spectra were compared to those obtained using diodes irradiated by MeV electrons or alpha particles indicating that very different defect creation mechanisms are at play when too little energy is available to form Frenkel pairs. These observations suggest that when EBD ions and energetic particles collide with the sample surface, inducing intrinsic non-localised lattice excitations, they modify defects deeper in the semiconductor thus rendering them observable.
36 MATERIALS SCIENCE↗
Photoluminescence enhancement of the single InAs quantum dots through plasmonic Au island films
The approach of optical positioning the single InAs quantum dots (QDs) was used for investigating QD photoluminescence (PL) enhancement based on plasmonic effect of nanometer-sized Au island films. It is found that the maximum increase of QD PL intensity is about thirty-eight fold after 5-nm thick Au island films are evaporated on the QD sample surface. The enhanced localized excitation field and increased QD radiative decay rate are responsible for this PL enhancement. This provides an alternative way of preparing bright single photon sources based on the plasmonic effect.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗