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At least 1,675 records · Page 93
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Hydride-Containing Eight-Electron Pt/Ag Superatoms: Structure, Bonding, and Multi-NMR Studies

Recent reports on hydride-doped noble metal nanoclusters strongly suggest that the encapsulated hydride is a part of the superatom core, but no accurate location of the hydride could be experimentally proved, so far. Here, we report herein a hydride-doped eight-electron platinum/silver alloy nanocluster in which the position of four-coordinated hydride was determined by neutron diffraction for the first time. X-ray structures of [PtHAg 19 (dtp/desp) 12 ] (dtp = S 2 P(O n Pr) 2 , 1; dsep = Se 2 P(O i Pr) 2 , 2) describe a central platinum hydride (PtH) unit encapsulated within a distorted Ag 12 icosahedron, the resulting (PtH)@Ag 12 core being stabilized by an outer sphere made up of 7 capping silver atoms and 12 dichalcogenolates. Solid-state structures of 1 and 2 differ somewhat in the spatial configuration of their outer spheres, resulting in overall different symmetries, C 1 and C 3 , respectively. Whereas the multi-NMR spectra of 2 in solution at 173 K reveal that the structure of C 3 symmetry is the predominant one, 1 H and 195 Pt NMR spectra of 1 at the same temperature disclose the presence of isomers of both C 1 and C 3 symmetry. DFT calculations found both isomers to be very close in energy, supporting the fact that they co-exist in solution. They also show that the [PtH@Ag 12 ] 5+ kernel can be viewed as a closed-shell superatomic core, the μ4-hydride electron contributing to its eight-electron count. On the other hand, the 1s(H) orbital contributes only moderately to the superatomic orbitals, being mainly involved in the building of a Pt–H bonding electron pair with the 5d z 2 (Pt) orbital.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Preparation and characterization of double layer thin films ZnO/ZnO:Ag for methylene blue photodegradation

Double layer (DL) thin films of zinc oxide and silver-doped zinc oxide (ZnO/ZnO:Ag) were deposited on glass substrate by sol-gel spray coating technique. The prepared thin films were subjected for optical and photocatalytic studies. UV-visible transmission spectra shows that the subtitution of Ag in ZnO leads to band gap reduction. The influence of Ag doping on the photocatalytic activity of ZnO for the degradation of methylene blue dye was studied under solar radiation. The light absorption over an extended visible region by Ag ion doping in ZnO film contributed equally to improve the photocatalytic activity up to 98.29%.

36 MATERIALS SCIENCE↗
DOE OSTI2016

A 10{sup 9} neutrons/pulse transportable pulsed D-D neutron source based on flexible head plasma focus unit

A 17 kJ transportable plasma focus (PF) device with flexible transmission lines is developed and is characterized. Six custom made capacitors are used for the capacitor bank (CB). The common high voltage plate of the CB is fixed to a centrally triggered spark gap switch. The output of the switch is coupled to the PF head through forty-eight 5 m long RG213 cables. The CB has a quarter time-period of 4 μs and an estimated current of 506 kA is delivered to the PF device at 17 kJ (60 μF, 24 kV) energy. The average neutron yield measured using silver activation detector in the radial direction is (7.1 ± 1.4) × 10{sup 8} neutrons/shot over 4π sr at 5 mbar optimum D{sub 2} pressure. The average neutron yield is more in the axial direction with an anisotropy factor of 1.33 ± 0.18. The average neutron energies estimated in the axial as well as in the radial directions are (2.90 ± 0.20) MeV and (2.58 ± 0.20) MeV, respectively. The flexibility of the PF head makes it useful for many applications where the source orientation and the location are important factors. The influence of electromagnetic interferences from the CB as well as from the spark gap on applications area can be avoided by putting a suitable barrier between the bank and the PF head.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Visible light broadband perfect absorbers

The visible light broadband perfect absorbers based on the silver (Ag) nano elliptical disks and holes array are studied using finite difference time domain simulations. The semiconducting indium silicon dioxide thin film is introduced as the space layer in this sandwiched structure. Utilizing the asymmetrical geometry of the structures, polarization sensitivity for transverse electric wave (TE)/transverse magnetic wave (TM) and left circular polarization wave (LCP)/right circular polarization wave (RCP) of the broadband absorption are gained. The absorbers with Ag nano disks and holes array show several peaks absorbance of 100% by numerical simulation. These simple and flexible perfect absorbers are particularly desirable for various potential applications including the solar energy absorber.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2016

Optical droplet vaporization of nanoparticle-loaded stimuli-responsive microbubbles

A capillary co-flow focusing process is developed to generate stimuli-responsive microbubbles (SRMs) that comprise perfluorocarbon (PFC) suspension of silver nanoparticles (SNPs) in a lipid shell. Upon continuous laser irradiation at around their surface plasmon resonance band, the SNPs effectively absorb electromagnetic energy, induce heat accumulation in SRMs, trigger PFC vaporization, and eventually lead to thermal expansion and fragmentation of the SRMs. This optical droplet vaporization (ODV) process is further simulated by a theoretical model that combines heat generation of SNPs, phase change of PFC, and thermal expansion of SRMs. The model is validated by benchtop experiments, where the ODV process is monitored by microscopic imaging. The effects of primary process parameters on behaviors of ODV are predicted by the theoretical model, indicating the technical feasibility for process control and optimization in future drug delivery applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Validation of modelled imaging plates sensitivity to 1-100 keV x-rays and spatial resolution characterisation for diagnostics for the “PETawatt Aquitaine Laser”

Thanks to their high dynamic range and ability to withstand electromagnetic pulse, imaging plates (IPs) are commonly used as passive detectors in laser-plasma experiments. In the framework of the development of the diagnostics for the Petawatt Aquitaine Laser facility, we present an absolute calibration and spatial resolution study of five different available types of IP (namely, MS-SR-TR-MP-ND) performed by using laser-induced K-shell X-rays emitted by a solid silver target irradiated by the laser ECLIPSE at CEntre Lasers Intenses et Applications. In addition, IP sensitivity measurements were performed with a 160 kV X-ray generator at CEA DAM DIF, where the absolute response of IP SR and TR has been calibrated to X-rays in the energy range 8-75 keV with uncertainties of about 15%. Finally, the response functions have been modeled in Monte Carlo GEANT4 simulations in order to reproduce experimental data. Simulations enable extrapolation of the IP response functions to photon energies from 1 keV to 1 GeV, of interest, e.g., for laser-driven radiography.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Plasmon–phonon coupling in monolayer WS{sub 2}

The excitation of plasmon in metallic nanostructures produces intense and strongly localized near fields that enhance light-matter interaction. Here, we report plasmon–phonon coupling in monolayer WS{sub 2} deposited with gold and silver nanoparticles. The Raman spectra reveal phonon modes arising from the coupling between plasmon and WS{sub 2}. The localized surface plasmon resonance mediated excitation activates the Raman process without requiring defect for momentum conservation. Our results also reveal that the momentum induced by localized surface plasmon resonances losses to WS{sub 2} and the metal atoms adsorption modulated spin–orbit split are the two essential elements for the observed plasmon–phonon coupling. This work will open up exciting prospects for plasmon–phonon coupling in two dimensional systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Pristine carbon nanotubes based resistive temperature sensor

A good sensor must be highly sensitive, faster in response, of low cost cum easily producible, and highly reliable. Incorporation of nano-dimensional particles/ wires makes conventional sensors more effective in terms of fulfilling the above requirements. For example, Carbon Nanotubes (CNTs) are promising sensing element because of its large aspect ratio, unique electronic and thermal properties. In addition to their use for widely reported chemical sensing, it has also been explored for temperature sensing. This paper presents the fabrication of CNTs based temperature sensor, prepared on silicon substrate using low cost spray coating method, which is reliable and reproducible method to prepare uniform CNTs thin films on any substrate. Besides this, simple and inexpensive method of preparation of dispersion of single walled CNTs (SWNTs) in 1,2 dichlorobenzene by using probe type ultrasonicator for debundling the CNTs for improving sensor response were used. The electrical contacts over the dispersed SWNTs were taken using silver paste electrodes. Fabricated sensors clearly show immediate change in resistance as a response to change in temperature of SWNTs. The measured sensitivity (change in resistance with temperature) of the sensor was found ∼ 0.29%/°C in the 25°C to 60°C temperature range.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

MnFe{sub 2}O{sub 4} as a gas sensor towards SO{sub 2} and NO{sub 2} gases

The chemical co-precipitation method was used to synthesize MnFe{sub 2}O{sub 4} nanoparticles. Single cubic phase formation of nanoparticles was confirmed by X-ray diffraction technique. The average particle size of MnFe{sub 2}O{sub 4} nanoparticles was found to be 10.7 nm using Scherrer formula. The ultrafine powder of MnFe{sub 2}O{sub 4} nanoparticles was pressed to design pellet of 10 mm diameter and 1mm thickness. Copper electrodes have been deposited on the surface of pellet using silver paste in the form of capacitor. Fabricated gas sensing device of MnFe{sub 2}O{sub 4} nanoparticles was tested towards SO{sub 2} and NO{sub 2} gases. Cole-Cole plot of MnFe{sub 2}O{sub 4} was investigated with the help of electrochemical workstation. The performance of the sensors including sensitivity, response and recovery time was also determined. It was observed that the MnFe{sub 2}O{sub 4} nanoparticles are more sensible for NO{sub 2} gas as compared to SO{sub 2} gas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Structural, morphological, optical and photocatalytic investigation of Ag-doped TiO{sub 2}

The pure and Ag-doped TiO{sub 2} nanoparticles were prepared by using Titanium isoproxide (TTIP), silver nitrate sodium hydroxide and sodium hydroxide. The calcined nanoparticles at 400°C were characterized by means of X-ray diffraction (XRD). XRD analyses reveal that the nanoparticles of various doping concentration were having anatase phase. The particle size was calculated by Scherrer formula and was found 11.08 nm for pure TiO{sub 2} and 8.86 nm for 6 mol % Ag doped TiO{sub 2}. The morphology and nature of nanoparticles was analyzed by using scanning electron microscope (SEM), the optical absorption spectra of pure TiO{sub 2} and Ag-doped TiO{sub 2} nanoparticles showed that absorption edge increases towards longer wavelength from 390 nm (pure) to 450 nm (doped), also band gap energy calculated from Tauc’s plot decrease from 3.20eV to 2.92eV with increase in doing. The measurement of photocatalytic properties of pure TiO{sub 2} and Ag-doped TiO{sub 2} nanoparticles showed that Ag-doped TiO{sub 2} degrades MB dye more efficiently than pure TiO{sub 2}.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Note: Proof of principle of a new type of cluster beam source with potential for scale-up

We introduce a new type of cluster beam source based on the assembly of (metal) clusters within a condensed (rare gas) matrix. The “Matrix Assembly Cluster Source” employs an ion beam to enhance collisions between metal atoms in the matrix and to sputter out clusters to form a beam. We demonstrate the formation and deposition of gold and silver nanoclusters with mean size tunable from a few atoms to a few thousand atoms. The cluster flux is equivalent to a current nanoAmp regime but potentially scalable to milliAmps, which would open up a number of interesting experiments and applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

Investigation of ITO free transparent conducting polymer based electrode

The last few decades have seen a significant improvement in organic semiconductor technology related to solar cell, light emitting diode and display panels. The material and structure of the transparent electrode is one of the major concerns for superior performance of devices such as OPV, OLED, touch screen and LCD display. Commonly used ITO is now restricted due to scarcity of indium, its poor mechanical properties and rigidity, and mismatch of energy levels with the active layer. Nowadays DMD (dielectric-metal-dielectric) structure is one of the prominent candidates as alternatives to ITO based electrode. We have used solution based spin coated polymer layer as the dielectric layer with silver thin film embedded in between to make a polymer-metal-polymer (PMP) structure for TCE applications. The PMP structure shows low resistivity (2.3 x 10{sup −4}Ω-cm), high carrier concentration (2.9 x 10{sup 21} cm{sup −3}) and moderate transparency. The multilayer PMP structure is characterized with XRD, AFM and Hall measurement to prove its suitability for opto-electronic device applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Broad electrical tuning of plasmonic nanoantennas at visible frequencies

We report an experimental demonstration of electrical tuning of plasmon resonances of optical nanopatch antennas over a wide wavelength range. The antennas consist of silver nanocubes separated from a gold film by a thin 8 nm polyelectrolyte spacer layer. By using ionic liquid and indium tin oxide coated glass as a top electrode, we demonstrate dynamic and reversible tuning of the plasmon resonance over 100 nm in the visible wavelength range using low applied voltages between −3.0 V and 2.8 V. The electrical potential is applied across the nanoscale gap causing changes in the gap thickness and dielectric environment which, in turn, modifies the plasmon resonance. The observed tuning range is greater than the full-width-at-half-maximum of the plasmon resonance, resulting in a tuning figure of merit of 1.05 and a tuning contrast greater than 50%. Our results provide an avenue to create active and reconfigurable integrated nanophotonic components for applications in optoelectronics and sensing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Nanoscale current spreading analysis in solution-processed graphene oxide/silver nanowire transparent electrodes via conductive atomic force microscopy

We use conductive atomic force microscopy (CAFM) to study the origin of long-range conductivity in model transparent conductive electrodes composed of networks of reduced graphene oxide (rGO{sub X}) and silver nanowires (AgNWs), with nanoscale spatial resolution. Pristine networks of rGO{sub X} (1–3 monolayers-thick) and AgNWs exhibit sheet resistances of ∼100–1000 kΩ/□ and 100–900 Ω/□, respectively. When the materials are deposited sequentially to form bilayer rGO{sub X}/AgNW electrodes and thermally annealed at 200 °C, the sheet resistance reduces by up to 36% as compared to pristine AgNW networks. CAFM was used to analyze the current spreading in both systems in order to identify the nanoscale phenomena responsible for this effect. For rGO{sub X} networks, the low intra-flake conductivity and the inter-flake contact resistance is found to dominate the macroscopic sheet resistance, while for AgNW networks the latter is determined by the density of the inter-AgNW junctions and their associated resistance. In the case of the bilayer rGO{sub X}/AgNWs' networks, rGO{sub X} flakes are found to form conductive “bridges” between AgNWs. We show that these additional nanoscopic electrical connections are responsible for the enhanced macroscopic conductivity of the bilayer rGO{sub X}/AgNW electrodes. Finally, the critical role of thermal annealing on the formation of these nanoscopic connections is discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

A perfect wetting of Mg monolayer on Ag(111) under atomic scale investigation: First principles calculations, scanning tunneling microscopy, and Auger spectroscopy

First principles calculations, scanning tunneling microscopy, and Auger spectroscopy experiments of the adsorption of Mg on Ag(111) substrate are conducted. This detailed study reveals that an atomic scale controlled deposition of a metallic Mg monolayer perfectly wets the silver substrate without any alloy formation at the interface at room temperature. A liquid-like behavior of the Mg species on the Ag substrate is highlighted as no dot formation is observed when coverage increases. Finally a layer-by-layer growth mode of Mg on Ag(111) can be predicted, thanks to density functional theory calculations as observed experimentally.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

The confinement of phonon propagation in TiAlN/Ag multilayer coatings with anomalously low heat conductivity

TiAlN/Ag multilayer coatings with a different number of bilayers and thicknesses of individual layers were fabricated by DC magnetron co-sputtering. Thermal conductivity was measured in dependence of Ag layer thickness. It was found anomalous low thermal conductivity of silver comparing to TiAlN and Ag bulk standards and TiAlN/TiN multilayers. The physical nature of such thermal barrier properties of the multilayer coatings was explained on the basis of reflection electron energy loss spectroscopy. The analysis shows that nanostructuring of the coating decreases the density of states and velocity of acoustic phonons propagation. At the same time, multiphonon channels of heat propagation degenerate. These results demonstrate that metal-dielectric interfaces in TiAlN/Ag coatings are insurmountable obstacles for acoustic phonons propagation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Resonance coupling in plasmonic nanomatryoshka homo- and heterodimers

Here, we examine the electromagnetic (EM) energy coupling and hybridization of plasmon resonances between closely spaced concentric nanoshells known as “nanomatryoshka” (NM) units in symmetric and antisymmetric compositions using the Finite Difference Time Domain (FDTD) analysis. Utilizing plasmon hybridization model, we calculated the energy level diagrams and verified that, in the symmetric dimer (in-phase mode in a homodimer), plasmonic bonding modes are dominant and tunable within the considered bandwidth. In contrast, in the antisymmetric dimer (out-of-phase mode in a heterodimer), due to the lack of the geometrical symmetry, new antibonding modes appear in the extinction profile, and this condition gives rise to repeal of dipolar field coupling. We also studied the extinction spectra and positions of the antibonding and bonding modes excited due to the energy coupling between silver and gold NM units in a heterodimer structure. Our analysis suggest abnormal shifts in the higher energy modes. We propose a method to analyze the behavior of multilayer concentric nanoshell particles in an antisymmetric orientation employing full dielectric function calculations and the Drude model based on interband transitions in metallic components. This study provides a method to predict the behavior of the higher energy plasmon resonant modes in entirely antisymmetric structures such as compositional heterodimers.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2016

Rewritable three-dimensional holographic data storage via optical forces

The development of nanostructures that can be reversibly arranged and assembled into 3D patterns may enable optical tunability. However, current dynamic recording materials such as photorefractive polymers cannot be used to store information permanently while also retaining configurability. Here, we describe the synthesis and optimization of a silver nanoparticle doped poly(2-hydroxyethyl methacrylate-co-methacrylic acid) recording medium for reversibly recording 3D holograms. We theoretically and experimentally demonstrate organizing nanoparticles into 3D assemblies in the recording medium using optical forces produced by the gradients of standing waves. The nanoparticles in the recording medium are organized by multiple nanosecond laser pulses to produce reconfigurable slanted multilayer structures. We demonstrate the capability of producing rewritable optical elements such as multilayer Bragg diffraction gratings, 1D photonic crystals, and 3D multiplexed optical gratings. We also show that 3D virtual holograms can be reversibly recorded. This recording strategy may have applications in reconfigurable optical elements, data storage devices, and dynamic holographic displays.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗